.flm‘vév.

‘.a:.

a. y‘. Vt

.k an. :a

~ 9 .3192.“
A}? x‘ ‘ , If

s ‘ . 9.1. “the
. L 5 ‘
. . as. . n."

in.

‘Mfw {yuan um...“

.- . w . [51.2.1- I

-.rm¥.fi_fia.fizm.m .
a ‘ 15.:

in»?
y s

. o.

5N. 5:44.“.th
if: ,

\‘W‘ Uri. it :v.
ur ’3‘an

. .3 g.
:1119 a.
2.]:

t .:
”inf.
. .. r

7‘

. L
y .. . £5
{:11 ,
,.\.l._.:

 

 

 

.l‘vlr.uv.¢llfit

3. I I ll. .

This is to certify that the
thesis entitled

SYNTHESIS AND STRUCTURAL CHARACTERIZATION OF
NEW MULTINARY GROUP 15 (BISMUTH AND ANTIMONY)
CHALCOGENIDES

presented by
SUMOHAN MISRA

has been accepted towards fulfillment
of the requirements for the

MASTER OF degree in CHEMISTRY

SCIENCE

Major Pr essor’ [Signature
€][/Z 0 /

Date

 

 

  

MSU is an Affinnative Action/Equal Opportunity Institution

LIBRARY
Michigan State
University

 

 

 

PLACE IN RETURN BOX to remove this checkout from your record.
To AVOID FINES return on or before date due.
MAY BE RECALLED with earlier due date if requested.

 

DATE DUE DATE DUE DATE DUE

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

6/01 c:/CIRC/DateDue.p65p.15

SYNTHESIS AND STRUCTURAL CHARACTERIZATION OF NEW
MULTINARY GROUP 15 (BISMUTH AND ANTIMONY)
CHALCOGENIDES

By

Sumohan Misra

A THESIS
Submitted to
Michigan State University
in partial fulfillment of the requirements
for the degree of
MASTER OF SCIENCE

Department of Chemistry

2004

(I:

“.371 E

m

V4.
. ALA-s
Tiff. CORPUS
VJ ' »o“..
u 'CI'SdnA\
IRJIHn “'9’

”Mk“ 5145;
w

' I .
h: ”503?; 4
bubkthuh

 

 

 

*Q1.
" ‘1'».
M'I ‘- ,
“ML

ABSTRACT

SYNTHESIS AND STRUCTURAL CHARACTERIZATION OF NEW MULTINARY
GROUP 15 (BISMUTH AND ANTIMONY) CHALCOGENIDES

By

Sumohan Misra

Multinary bismuth chalcogenides are an attractive class of compounds due to their
rich compositional and structural variety which makes them some of the most adaptable
and versatile systems. Together with this rich structural heterogeneity, their potential as
leading thermoelectric materials led us to the investigation of these multinary bismuth
chalcogenide.

Three new compounds KszBiSSIO, Kbe4-2xBi4+xSm-yTey, and NaxSr4-2xBi4+xSe10
all having KBI633S|o type structure and showing variation in either the metal or the
chalcogenide site were obtained. Physicochemical characterization of KszBissm is
reported. We also obtained two derivatives of the K2,sBig,5Se14 structure type: Rb1+be3-
2,.Bi7+,‘Sem.yTey and NaxBa5-2xBi6+xSe.4. Physicochemical characterization of NaxBas-
2xBi6+xSel4is reported. We also employed solvothennal synthetic conditions to study the
system Cszse/M/Se (M = Bi, Sb). C53Sb58e9 was obtained which is an ordered structural
variant than the one previously reported.

This thesis describes the synthesis and structural characterization of the above

mentioned compounds.

Iaould like
3; 5.73m and at

23:5 for their he?

 

ACKNOWLEDGEMENTS

Iwould like to thank my advisor, Professor Mercouri G. Kanatzidis for all his
help, support and advice. I would also like to thank all my past and present group

members for their help and support.

iii

ISTOFTABLEE
SYOFHGLRE
€3.71: 1. .Iluitm.
Fmoeiectn'r M.
lntrodu.
Bhflnna
Apphca
Malena

Referen

Cater 2. Sim/w:
.IJSHQBD. rSé’. U
A. Irim

B. Exp

Re;

5}:

 

 

C. PI

Table of Contents

LIST OF TABLES viii
LIST OF FIGURES x
Chapter 1.Multinary Bismuth Chalcogenides and Their Application as
Thermoelectric Materials 1
Introduction 1
Multinary Bismuth Chalcogenides 1
Application of Multinary Bismuth chalcogenides as Thermoelectric
Materials 5
References 8

Chapter 2. Synthesis and Structure of KszBi 5S ,0, Kbe4-2xBi4+xS 10.yTey, and

Na,Sr4-2xBi4+xSem belonging to the Cosalite structure type 10
A. Introduction 10
B. Experimental Section 11

Reagents 11
Synthesis 12
Bi28e3 12
PbTe 12
KzBigsl 3 12
KszBisslo 12
K,‘Pb4.2,,Bi4+xS10.),Tey 13
NaxSr4-2xBi4+xSem 13

C. Physical Measurements 14
Energy Dispersive Spectroscopy 14

iv

.I

Q9 "
1“.

Sim
Conclu

Refers

 

 

 

ii. PithBi .,5.
A. In

B. Ei.

R;

S;

 

Differential Thermal Analysis
Charge Transport Measurements
Powder X-ray diffraction
Single-Crystal X-ray Crystallography
KszBiSSm
Ko.93Pb3.043i4.34S9.60T€0.40

Nao.4755f2.7933i4.7133610

D. Results and discussion

Structure Description of KszBiSSlo

Thermal Analysis of KszBisslo

Charge Transport Measurement of KszBISSm
Structure Description of K,,Pb4.2,,Bi4+,,S10.),Tey

Structure Description of NaxSr4-2xBi4+xSelo

Conclusion

References

Chapter 3. Variation in the K 2, 531's. 5Se14 structure type: Synthesis and Structure of
Rbl+be3-2xBi7+,Sel4.yTey and NaxBa5-2xBi6+xSe,4
A. Introduction

B. Experimental Section

Reagents
Synthesis

Bi28e3

14

14

15

25

15

15

16

21

21

22

22

29

35

4O

41

43

43

fi

t

45

C. Ph)
Enc‘
Dif
C h:
For

Sin

D. Res
Stn

Sin

 

 

PbTe
szBIsSCl 3
Rb]+be3-2xBl7+xSCI4-yTey

NaxBa5-2xBi6+xSe14

C. Physical Measurements

Energy Dispersive Spectroscopy
Differential Thermal Analysis
Charge Transport Measurements
Powder X-ray diffraction
Single-Crystal X-ray Crystallography
Rbl.73Pbl .29Bi83613.42T60.59

NaiBaz.7oBi7.37S€i4

D. Results and discussion

Structure Description of Rb]+,(Pb3,.2,,Bi7+xSe14.yTey
Structure Description of NaxBa5-2xBi6+xSei4
Thermal Analysis of NaxBa5-2xBi6+xSe14

Charge Transport Measurement of NaxBa5-2xBi6+xSe14

Conclusion

References

Chapter 4. Solvothermal Synthesis of Ordered Structure of Cs 3Sb 5Seg
A. Introduction

B. Experimental Section

vi

45

45

45

46

46

46

46

47

47

48

48

48

54

54

61

62

62

7O

71

73

73

75

Sol

SW

C. Phj
En
Sir

D. Re

iDPExDICES

APPE

APPE

 

 

 

Reagents

Solvent

Synthesis

CS3Sb5$69

C. Physical Measurements

Energy Dispersive Spectroscopy

Single-Crystal X—ray Crystallography
D. Results and discussion

Structure Description of Cs3Sb58e9
Conclusion
References

APPENDICES

APPENDIX A. CIF FILE FOR KszBisslo
APPENDIX B. CIF FILE FOR Kbe4-2xBi4+xSlo-yTey
APPENDIX C. CIF FILE FOR NaxSr4-2xBi4+xSe10
APPENDIX D. CIF FILE FOR Rb.+,‘Pb3.2,,Bi7+,.Se14.yTey
APPENDIX E. CIF FILE FOR NaxBa5-2xBi6+xSel4

APPENDIX F. CIF FILE FOR CS3Sb58€9

vii

75

75

76

76

76

76

77

82

82

93

94

96

97

107

118

134

151

169

Table ll

'1 1 7
T331: ---'

Table 2

Table 2-7.

Table 2-8.

Table 3.3.

Iable 3.4_
T”able 3.5.

Table 36

 

 

Table 2-1.

Table 2-2.

Table 2-3.

Table 2-4.

Table 2-5.

Table 2-6.

Table 2-7.

Table 2-8.

Table 2-9.

Table 2-10.

Table 3-1.

Table 3-2.

Table 3-3.

Table 3-4.

Table 3-5.

Table 3-6.

Table 3-7.

LIST OF TABLES

Crystallographic Data for KszBisslo, Kbe4-2xBi4+xSm-yTey, and
Naxsr4-2xBi4+xsel 0

Atomic coordinates (x 104) and equivalent isotropic displacement
parameters (A2 x 103) for KszBisslo

Atomic coordinates (x 104) and equivalent isotropic displacement

parameters (A2 X 103) for K0.93Pb3.043i4.3439.60T€o.4o

Atomic coordinates (x 104) and equivalent isotropic displacement
parameters (A2 X 103) for Nao.4753f2.79sBi4.7i3Seio
Bond distances (A) for KszBisslo

Selected Angles (deg) for KszBi5810

Bond distances (A) for Kbe4-2xBi4+xSlo-yTey
Selected Angles (deg) for K,,Pb4_2,,Bi4.t,‘S10.,Tey
Bond distances (A) for NaxSr4-2xBi4+xSe10
Selected Angles (deg) for NaxSr4-2xBi4+xSe.o

Crystallographic Data for Rb;+,,Pb3,.;z,,Bi7+,,Se14.yTey and

NaxBa5-2xBi6+xSe14

Atomic coordinates ( x 104) and equivalent isotropic

displacement parameters (A2 x 103) for Rb],73Pb1,ngigSe.3,42Teo,59

Atomic coordinates (x 104) and equivalent isotropic
displacement parameters (A2 x 103) for NalBa2.7gBi7,378e14
Bond distances (A) for Rb1+be3-2xBi7+xSe14-yTey

Selected Angles (deg) for Rb1+,,Pb3.2,,Bi7+,,Se14.),Tey
Bond distances (A) for NaxBa5-2xBi6+xSe14

Selected Angles (deg) for NaxBa5-2xBi6+xSel4

viii

17

18

19

20

25

26

32

33

38

39

49

50

52

57

59

64

66

Table-H-

iale #2.

Table #3.

 

 

Table 4-1.

Table 4-2.

Table 4-3.

Table 4-4.

Table 4-5.

Physical constants for ethylene diamine

Crystallographic data for the ordered CS3Sb5$e9 and the structure
reported by Sheldrick and Hausler

Atomic coordinates (x 104) and equivalent isotropic displacement
parameters (A2 x 103) for CS3SbSSe9
Bond distances (A) for CS3Sb5869

Selected Angles (deg) for C53Sb58e9

ix

78

79

80

87

90

 

Figure 1-1.

 

Figure 1-1.

Figure 1-2.

Figure 2-1.

Figure 2-2.

Figure 2-3.

Figure 2-4.

Figure 2-5.

Figure 2-6.

Figure 2-7.

Figure 2-8.

Figure 3-1.

LIST OF FIGURES

Some of the different types of coordination environment that Bi
atoms adopt in various multinary bismuth chalcogenides: (a)
trigonal pyramidal in B-CsBiSz, (b) square pyramidal in
Rb23138613, (c) perfect octahedral in RbBiSz, (d) distorted
octahedral in B-KzBi38e13, (e) bicapped trigonal prismatic in
KBi6,33Sm, (t) monocapped trigonal prismatic in szLaxBig-xSI4
Different building blocks that are found in multinary bismuth
chalcogenides: (a) NaCl-type fragment, (b) BizTe3-type fragment,
(0) CdIz-type fragment, (d) SbZSe3-type fragment

Projection of the structure of KszBisslo down the b-axis

Polyhedral representation of KszBisslo down the b-axis showing
the connectivity of the M86 octahedra (M = Bi, Pb)

DTA diagram of KszBisslo showing the endothermic and
exothermic peaks. The heating and cooling rates were 10°C/min
Variable temperature thennopower for a polycrystalline oriented
ingot of KszBiSSm

Projection of the structure of Ko,93Pb3,o4Bi4,3489,60Te0,4o down the
b-axis

Polyhedral representation of Ko,93Pb3_04Bi4,3489,60Teo,4o down the
b-axis showing the connectivity of the M86 octahedra (M = Bi,
Pb, Bi/K)

Projection of the structure of Nao,4758r2,7ggBi4,7138e10 down the b-
axis

Polyhedral representation of Nao,4758r2,793Bi4,713Se10 down the b-
axis showing the connectivity of the M86 octahedra (M = Bi,
Bi/Sr)

Projection of the structure of Rbl,73Pb1.2gBi3$e13,42Te0,59 down the

b-axis

3

4

23

24

27

28

30

31

36

37

56

 

Table 3—1.

Table 4—1.
Table 4-2.

Table 4—3.

Table 4—4.

 

 

Table 3-2.

Table 3-3.

Table 3-4.

Table 4-1.

Table 4-2.

Table 4-3.

Table 4-4.

Projection of the structure of NalBa2,7gBi7,37Sel4 down the b-axis

DTA diagram of NaxBa5-2xBi6+xSe14 showing the endothermic and
exothermic peaks. The heating and cooling rates were 10°C/min
Variable temperature thennopower for a polycrystalline oriented
ingot of NaxBa5-2xBi6+xSe14

SEM image of the hexagonal rod type crystal of CS3Sb5$e9
Projection of the structure of CS3SbSSe9 down the c-axis

Different selenoantimonate units which act as

building-blocks

Projection of one of the layers in C53Sb5$e9 down the b-axis
showing the tunnels occupied by the alkali atoms. It also shows

the chains connected by the (SbZSe5)4' unit

xi

63

84

85

86

 

Mulllr

Introduction
The gen
a)l.)l'.Bi,Q,
ital}- is an it
ii'ersity and

iTITIOCIECIYII: a

Multinary Bisn

Bismuth
{as of compo
him some 0i ii

(Ely well exprc

 

Bmuih 310m:

 

 

hf “Walla!C

813315311] 310m

CHAPTER 1

Multinary Bismuth Chalcogenides and Their Application as

Thermoelectric Materials

Introduction

The general formula for multinary bismuth chalcogenide family can be expressed
as MwM'xBinz Where M & M' could be any metal and Q is a chalcogen (S, Se, Te). This
family is an interesting class of materials due to their compositional and structural
diversity and complexity and this makes them attractive for investigations for

thermoelectric applications.

Multinary Bismuth Chalcogenides

Bismuth chalcogenides from a solid state chemistry perspective are an attractive
class of compounds due to their rich compositional and structural variety which makes
them some of the most adaptable and versatile systems. In nature these characteristics are
very well expressed in the sulfosalts familyl where Bi compounds constitute 20% of them.
Bismuth atoms both in naturally occurring sulfosalts and in the synthetically derived
compounds show an amazing flexibility in bonding. This fact is an underlying reason for
the unparalleled diversity and complexity that bismuth chalcogenide compounds possess.

Bismuth atom adopt several different coordination environments ranging from trigonal

-l_
T I! I": ‘Ll

 

scandal. to SC
égfier coordln.
IOIleflIIOII en
53.11 This It
coordination gel
at d-Otbitals It
:ezter. Almost
fimhemieal l
755 ID probabl)
mime interes

30mg Of
domed in Van
lines; It
515’ch OCL'ihe
honxapped m!
35m“ to the

 

 

' “VI ,.
Anon»...

at“

l:
0%
.C‘dra I0 c

 
  
 

b‘h‘i' .
waking blOCk,

4n .
QmC 03563 S

pyramidal, to square pyramidal, to octahedral (usually distorted) to trigonal prismatic to
higher coordination number extending to nine. The cause of such a variety of
coordination environments can be pinned down to the 6s2 lone pair of electrons of
bismuth. This lone pair can be stereochemically expressed to locally distort the bismuth
coordination geometry or can be suppressed by hybridizing with energetically adjacent p-
and d-orbitals to form sp3d2 hybrid orbitals thereby producing a regular octahedral Bi”
center. Almost any intermediate stage in the continuum is observed between the full
stereochemical expression and complete suppression of the lone pair. This property gives
rise to probably the most malleable coordination geometry in the periodic table. It is
therefore interesting to observe the role of Bi3+ and its role in stabilizing various structure
types.

Some of the different types of coordination environment for Bi atoms that can be
observed in various multinary bismuth chalcogenides can range from trigonal pyramidal
in B—CsBiSz,2 to square p yramidal in szBigSe. 3,3 to p erfect o ctahedral in RbBiSz,4 to
distorted octahedral in [3-K2Bi38el3,5 to bicapped trigonal prismatic in I(Bi(,,33Sm,6 to
monocapped trigonal prismatic in szLa,.Big.,,Sl4.7 These are shown in Figure 1-1. With
reference to the figure, for (a) and (b) the lone pair is being completely expressed while
for (c) it is completely suppressed. For ((1) it is only partially expressed leading to short
bonds (solid lines) trans to longer bonds (dotted line).

Another interesting feature of these families of compounds is the ability of BiQ6
octahedra to combine with each other by sharing their edges thereby forming various
building blocks. NaCl-type, BizTeg-type and CdIz-type fragment is the most common and

in some cases Sb28e3-type fragment can also be seen (see figure 1-2.).

 

figurt l-l. Sort
: various mult.
care pnamida
3‘. 5-K;Bl;5613.

«It in Pb;l

 

C.
{C}
lei)
ff

h/

 

Figure 1-1. Some of the different types of coordination environment that Bi atoms adopt
in various multinary bismuth chalcogenides: (a) trigonal pyramidal in B-CsBiSz, (b)
square pyramidal in szBisSCn, (c) perfect octahedral in RbBiSz, (d) distorted octahedral
in B—KzBi38e13, (e) bicapped trigonal prismatic in KBi6,33810, (f) monocapped trigonal

prismatic in szLaxBi3.xSI4.

a

(a) (b)
(C) (d)
(e) (f)

 

 

figure 1'2.
.3: 33C 1'1}?

,.
"fix Iffiémfi

(I

it

 

 

Figure 1-2. Different building blocks that are found in multinary bismuth chalcogenides:
(a) NaCl-type fragment, (b) BizTeg-type fragment, (c) CdIz-type fragment, (d) Sb28e3-

type fragment.

(a)

(b)

 

(C) (d)

 

 

ruler system
“‘f .
randomness ini
as strongly 5c
- - .13
iOZldLiCIlI'lI}.
first of merit(
This n'c
:heir potential :

airman; bismt

Alimitation of.

“hen t

“011336 grad

 

an they Can b

«‘1. '
Ll 41653 are m .

 

The third characteristic property of bismuth atoms is its ability to display mixed
occupancy leading to structural disorder with a variety of similar sized ions like alkali
metals, 5'6 alkaline earth metals,8 Pb,8’ 9’ '0 Sns’ '0‘ H or rare earth metals.12 This mixed
occupancy ofien results in the formation of new structure types that do not exist in the
simpler systems. Also this kind of positional disorder in the structure generates
randomness in mass, size and charge of the atoms on a particular lattice position and this
can strongly scatter acoustic lattice phonons carrying heat and thus lower the thermal
conductivity.” The lowering of thermal conductivity is important in maximizing the
figure of merit (ZT) of thermoelectric materials (explained later in this chapter).

This rich structural heterogeneity that these compounds possess together with
their potential as leading thermoelectric materials led us to the investigation of these

multinary bismuth chalcogenide.

Application of Multinary Bismuth chalcogenides as Thermoelectric Materials

When two dissimilar conductors are in contact with each other then at the junction
a voltage gradient is generated automatically whose values depend on the type of
conductors used and the temperature. Also if a temperature gradient exists along a
conductor, a voltage difference is generated which again depends on the type of
conductor and the temperature gradient. These effects are known as thermoelectric effects
and they can be distinguished as Thomson, Peltier and Seebeck effects. The applications
of these are in thermocouples, refiigeration devices and in power generation.

The b est m aterials for thermoelectric c ooling applications c urrently u sed in the

industry are solid solutions of BizTe3 and Bi2.,,Sb,,Te3.ySey.l4 These materials possess high

 

, A 4",
isCCIFICal “Gnu“

resin-emit?" ll

stilt S is t}
wzjuctl‘IIV. K
.71" 1.0 at 30C
mare and

mmdently 1

Deleted that
perfonnmcels
sell is a Z T 2
Our 21;
:blcogenides
Ions. large un
mmsition the

simplex electr.

 

s .

“will cone.
tenductil'ltv u
“moeleclfic I

ll. 1
”53 rattler;

 

electrical conductivity and thermoelectric power (Seebeck coefficient) and low thermal
conductivity. These properties define the dimensionless figure of merit:
27 = (S20) T/ x

where S is the thermoelectric power or Seebeck coefficient, a is the electrical
conductivity, x is the thermal conductivity and T is the temperature. These alloys have a
ZT~ 1.0 at 300 K. The above properties are determined by the details of the electronic
structure and scattering of charge carriers (electrons and holes) and thus are not
independently controllable parameters. An increase in the electrical conductivity leads to
a simultaneous decrease in the thermoelectric power and a comparable increase in the
thermal conductivity. Hence it is not easy to improve the value of ZT. Moreover it is now
believed that the BizTe3 compounds may be nearing the limit of their potential
performance15 and the requirement for a thermoelectric material to be commercially
useful is a ZTZ 1.5.

Our approach in improving ZT is to identify new multinary bismuth
chalcogenides with higher compositional and structural complexity containing heavy
atoms, large unit cells and disorder in the crystal lattice. This rationale is based on the
proposition that materials with more complex compositions and structures may have
complex electronic structure which may give rise to high thermoelectric power and low
thermal conductivities.l6 Another concept which helps in lowering the thermal
conductivity was introduced by Slack as the limiting characteristic for a superior
thermoelectric.” In these materials a weakly bound atom or molecule ‘rattler’ is used.

These ‘rattlers’ create low-fi'equency vibration modes that scatter acoustic lattice phonons

.au

as
'I
- L nnfl-;:'1

 

rzip shows all
“rperties. This

In C hap
img these 5p
rill discuss Ill:

1”Lanziritimon

 

 

carrying heat thereby lowering the thermal conductivity of the solid without severely
affecting the electrical conduction, thus leading to improved thermoelectric efficiency.17

The compounds B-KzBIgSCj3,5 CsBi4Te6,18 KBi6,33S;o 6 reported earlier by our
group shows all the above mentioned characteristics and exhibit promising thermoelectric
properties. This has leaded us to investigate more complicated multinary systems.

In Chapters 2 and 3 we will describe the multinary bismuth chalcogenides found
during these synthetic investigations and their structural characterization. In Chapter 4 we
will discuss the ‘solvotherrnal’ synthesis technique and how it is used to synthesize a

ternary antimony chalcogenide.

References

1. (313134“
Miner. 19
160.369-2
E.Krist.1.".

g.)

McCarthj.
C. R.; K3

3. Iordanidi.
Chen, \K'.
Mater. 21.

 

P

Voroshi I.

- Chung,
Kanneu ;
1997, 9,

 

 

References

1.

(a) Makovicky, E. Eur. J. Mineral. 1993, 5, 545-591. (b) Makovicky, E. Fortschr.
Miner. 1981, 59,137-190. (c) Makovicky, E. Neues Jahrbuch Miner. Abh. 1989,
160, 269-297. ((1) Makovicky, E. Fortschr. Miner. 1985, 63,45-89. (e) Makovicky,
E. Kristallogr. 1985, 173, 1-23.

McCarthy, T. J.; Ngeyi, S. -P.; Liao, J. -H; DeGroot, D.; Hogan, T.; Kannewurf,
C. R.; Kanatzidis, M. G. Chem. Mater. 1993, 5, 331-340.

Iordanidis, L.; Brazis, P. W.; Kyratsi, T.; Ireland, J.; Lane, M. ;Kannewurf, C. R.;
Chen, W.; Dyck, J. S.; Uher, C.; Ghelani, N.; Hogan, T.; Kanatzidis, M. G. Chem.
Mater. 2001, 13, 622-633.

Voroshilov, Y. V.; Peresh, E . Y.; Golovei, M. I. Inorg. Mater. 1972, 8, 777-778.

Chung, D-. Y.; Choi, K. -S.; Iordanidis, L.; Schindler, J. L.; Brazis, P. W.;
Kannewurf, C. R.; Chen, 8.; Hu, 8.; Uher, C.; Kanatzidis, M. G. Chem. Mater.
1997, 9, 3060-3071.

Kanatzidis, M. G.; McCarthy, T. J.; Tanzer, T. A.; Chen, L.; Iordanidis, L.; Hogan,
T.; Kannewurf, C. R.; Uher, C.; Chen, B. Chem. Mater. 1996, 8, 1465-1474.

Iordanidis, L.; Kanatzidis, M. G. Inorg. Chem. 2001, 40, 1878-1887.

Wang, Y. C.; DiSalvo, F. J. Chem. Mater. 2000, 12, 1011-1017.

Chung, D-. Y.; Iordanidis, L.; Rangan, K. K.; Brazis, P. W.; Kannewurf, C. R.;
Kanatzidis, M. G. Chem. Mater. 1999, 11, 1352-1362.

10. Choi, K. -S.; Chung, D-. Y.; Mrotzek, A.; Brazis, P. W.; Kannewurf, C. R.; Uher,

C.; Chen, W.; Hogan, T.; Kanatzidis, M. G. Chem. Mater. 2001, 13, 756-764.

11. Mrotzek, A.; Chung, D-. Y.; Hogan, T.; Kanatzidis, M. G. J. Mater. Chem. 2000,

l 0( 7), 1667-1672.

 

12. IordzmlC

Chem. 1

13. (a) 5131‘
Coohng
Boca R
Ehrenre
p l.

14. la) Yim
W. M;
Przylusl

15. Goldsm

16. Mon, ,\'
Publicat

17. Sales, B

18- (a) Nola
73. 173-
C- J. Ap

 

12. Iordanidis, L.; Schindler, J. L.; Kannewurf, C. R.; Kanatzidis, M. G. J. Solid State
Chem. 1999, 143(2), 151-162.

13. (a) Slack, G. A. New Materials and Performance Limits for Thermoelectric
Cooling. In CRC Handbook of Thermoelectrics; Rowe, D. M., Ed,; CRC Press:
Boca Raton, F1, 1995; pp 407-440. (b) Slack, G. A. Solid State Physics;
Ehrenreich, H., Seitz, F., Tumbull, D., Eds.; Academic: New York, 1997; Vol. 34,

pl.

14. (a) Yim, W. M.; Fitzke, E. V. J. Electrochem. Soc. 1968, 115, 556-560. (b) Yim,
W. M.; Fitzke, E. V.; Rosi, F. D. J. Mater. Sci. 1996, 1, 52-65. (c) Borkowski, K.;
Przyluski, J. Mater. Res. Bull. 1987, 22, 381-387.

15. Goldsmid, H. J. Electronic Refrigeration, Pion: London, 1986.

16. Mott, N. R; Jones, H. The theory of the Properties of Metals and Alloys, Dover
Publications: New York, NY.

17. Sales, B. C.; Curr. Opin. Solid St.Mater. 1997, 2, 284-289.

18. (a) Nolas, G. S.; Cohn, J. L.; Slack, G. A.; Schujman, S. B. Appl. Phys. Lett. 1998,
73, 178-180. (b) Nolas, G. S.; Slack, G. A.; Morelli, D. T.; Tritt, T. M.; Ehrlich, A.
C. J. Appl. Phys. 1996, 79, 4002-4008.

 

Synthesis an

“fill-213i“

.tlntroducl

Bismutl
henoeleetrics
niitation in 1
suitinn bism
fie lo their co
b.1165: lone p
me which i
Times of th

A supe
iifibril coeffi.

Lime Ofmeri:

 

 

tinsel lat:

it. - .
“Minis.

CHAPTER 2

Synthesis and Structure of KszBiSSw, KbenszimSIMTey, and

Na,Sr4.2,Bi4+,Selo belonging to the Cosalite structure type.

A. Introduction

Bismuth chalcogenides have a wide range of applications including
thermoelectrics,1 and non-linear optical materials.2 From the point of view of their
application in thermoelectrics our approach has been to focus on new semiconducting
multinary bismuth chalcogenides. These materials are an interesting class of compounds
due to their compositional and structural complexity arising due to the presence of an
inert 6s2 lone pair of electrons on bismuth which may or may not be stereochemically
active which in turn affects the lattice structure, the electronic structure and thus the
properties of the resulting compounds.

A superior thermoelectric material has high electrical conductivity (0), high
seebeck coefficient (S) and low thermal conductivity (rc). These together define the TE
figure of merit ZT = (a 82/ x) T. Factors contributing to low thermal conductivity and thus
higher ZT are the presence of heavy atoms like Bi and Pb, large unit cells and disorder in
the crystal lattice. The rationale behind using lead is that in addition to being very heavy
it has similar electronic properties as Bi and has a well known tendency to disorder with
Bi or alkali metals, depending on the local environmentf"5 This kind of site occupancy

disorder in the structure generates randomness in mass, size and charge of the atoms on a

10

;afieular lattii
Enl- tl‘luS lone
tozd‘octiiity i:
channels or I.

1555 10115 m;

rend in the

133mg} Condu

Ripon
it: mClure
3:31ch I'Or I
new cOmpOu“

£31138;th

B'EXperim,

Reagen

(Cat. Milka).

 

 

particular lattice position that can strongly scatter acoustic lattice phonons carrying heat
and thus lower the thermal conductivity.6 Another approach in lowering the thermal
conductivity in these materials is to incorporate alkali or alkaline earth metals in the
channels or layers formed by these infinite anionic bismuth-chalcogen frameworks.
These ions make relatively weak ionic bonds with chalcogens due to which they rattle
around in their channels or in between the layers thereby creating low-frequency
vibration modes that scatter acoustic lattice phonons carrying heat, thus reducing the
thermal conductivity. 7

Reports previously from our group showed that KBi6,33Sw 8 which has a cosalite
like structure has thermal conductivity substantially lower than BIzTC3 making it
attractive for further investigations for thermoelectric applications. We report here three
new compounds KszBisslo, Kbe4-2xBi4+xSm-yTey, and NaxSr4-2xBi4+xSelo all having

KBi6,33Sm type structure showing variation in either the metal or the chalcogenide site.

B. Experimental Section

Reagents: Chemicals were used as obtained: (i) bismuth chunks, 99.999% purity,
Cerac, Milwaukee, WI, (ii) sulfur powder, sublimed, Spectrum Chemical Mfg. Corp.,
Gardena, CA, (iii) selenium shots (99.999% purity, Cerac, Milwaukee, WI), (iv)
tellurium chunks 99.999% purity, Cerac, Milwaukee, WI, (v) potassium metal, Aldrich,
Milwaukee, WI, (vi) lead metal, Cerac, Milwaukee, WI, (vii) strontium selenide powder
99.5% purity, -20 mesh, Cerac, Milwaukee, WI. Nazse was prepared by a stoichiometric

reaction of sodium metal and selenium shots in liquid ammonia.

11

 

spthfS
al'acuum Am
335 Vail-15d b?
{m 573312.110???
813593:
mum “35 I
i‘asuum (‘104
3o: 10 hours an
.‘taefions.
PbTe:
claim was I
sailed under V;
therefor 12 he

timer reactior

 

 

 

Synthesis: All manipulations were carried out under a dry nitrogen atmosphere in
a Vacuum Atmospheres Dri-Lab glovebox. The purity and homogeneity of the products
was verified by comparing the X-ray powder diffraction patterns to those calculated by
the crystallographically determined atomic coordinates.

Bizse3: A mixture of 6.383g (0.031 mol) of bismuth and 3.617g (0.046 mol) of
selenium was transferred into a 13mm quartz tube, which was then flame sealed under
vacuum (~10‘4 Torr). The tube was heated to 800°C in 10 hours, held at that temperature
for 10 hours and then cooled down to 50°C in 10 hours. The product was used for further
reactions.

PbTe: A mixture of 12.378g (0.060 mol) of lead and 7.622g (0.060 mol) of
tellurium was transferred into a 13mm carbon coated quartz tube, which was then flame
sealed under vacuum (~104 Torr). The tube was heated to 1100°C in 8 hours, isothenned
there for 12 hours and then cooled down to 50°C in 24 hours. The product was used for
further reactions.

KzBisSu: A mixture of 0.180g (4.60 mmol) of potassium, 3.858g (0.018 mol) of
bismuth and 0.962g (0.030 mol) of sulfur was transferred into 13mm quartz tube, which
was then flame sealed under vacuum (~104 Torr). The tube was heated to 150°C in 6
hours, and then firrther heated upto 850°C in 6 hours, isothermed there for 1 hour and
then cooled down to 50°C in 48 hours. The product was used for further reactions.

KszBisslo: A pure synthesis of KszBiSSlo was achieved with a mixture of
0.05g (1.280 mmol) of potassium, 0.265g (1.280 mmol) of lead, 0.668g (3.20 mmol) of
bismuth and 0.205g (6.40 mmol) of sulfur in the ratio 2:225:10 which were transferred

into a 13mm quartz tube and was flame sealed under vacuum (~10'4 Torr). The tube was

12

sealed to 850T
5511‘C in 30 he
2.:lle like cry
sag a Seannir
3153‘. gave an ;
le’bH
[553 mmol) of
tes- flme sea}
5d ISOIITCTmeg
t“31110 5135c
11113311131113 3:
Electron MICrc
WOleaze CC
NarSI'

XS’: and 047

 

 

heated to 850°C in 10 hours and isothermed there for 48 hours and then cooled slowly to
550°C in 30 hours and finally to 50°C in 3 hours. The product consisted of silvery-gray
needle like crystals. A quantitative analysis by Energy Dispersive Spectroscopy (EDS)
using a Scanning Electron Microscope (SEM) was performed on several of these crystals
which gave an approximate composition of “KPb3,30Bi3,3683.03”.

KbeasziflxquTey: A mixture of 0.4g (0.185 mmol) of KzBi8513 and 0.185g
(.553 mmol) of PbTe in the ratio 1:3 was transferred into a 9mm quartz tube, which was
then flame sealed under vacuum (~10“1 Torr). The tube was heated to 850°C in 10 hours
and isothenned there for 48 hours and then cooled slowly to 500°C in 96 hours and
finally to 50°C in 5 hours. The product consisted of silvery-gray needle like crystals. A
quantitative analysis by Energy Dispersive Spectroscopy (EDS) using 3 Scanning
Electron Microscope (SEM) was performed on several of these crystals which gave an
approximate composition of “KPb4_6zBi3,95S9_73Te0,27”.

NaxSrnsziflxSew: A mixture of 0.03g (0.24 mmol) of Na2Se, 0.2g (1.2 mmol) of
SrSe and 0.472g (7.2 mmol) of BiZSe3 in the ratio 1:5:3 were transferred into a graphite
tube which was placed in a 13mm quartz tube, which was then flame sealed under
vacuum (~104 Torr). The tube was heated to 800°C in 24 hours, held at that temperature
for 24 hours and then cooled to 50°C in 25 hours. The product consisted of silvery-gray
rod like crystals. Energy Dispersive Spectroscopy (EDS) on several of these crystals gave

an approximate composition of “NaSr1,9(,Bi4,6oSe9,6g”.

13

, ‘
c.1119“I ’

Energ.‘
sitimd “e:

$33611 “lit
1 ‘1

Differe

311371-ch “ll

‘ 1

gig}: CQSlalS
motile contai
he detector. T
11611 by co
if?! DTA, Ill:
ate was c

Charge

mmllllflll fro

   
 
  

7315mm (COT;

PM“. The ter:

heater which -

 

3535321 $139:
1‘13 11le 5.,

‘1‘" t. .
Q likafllrek

 

C. Physical Measurements

Energy Dispersive Spectroscopy: Quantitative microprobe analyses of the
compound were performed with a JEOL JSM-64OOV Scanning Electron Microscope
equipped with a Tracor Northern Energy Dispersive Spectroscopy (EDS) detector. Data
were acquired it sing an accelerating v oltage o f 20 k V and a 3 0 se conds accumulation
time.

Differential Thermal Analysis: Differential Thermal Analysis (DTA) was
performed with a computer-controlled Shimadzu DTA-50 thermal analyzer. Ground
single crystals (30-40 mg) were sealed in silica ampoules under vacuum. A silica
ampoule containing alumina of equal mass was sealed and placed on the reference side of
the detector. The samples were heated to 1000°C at 10°C/min, isothenned for 1 minute
followed by cooling at 10°C/min. The reported DTA temperature is the peak temperature.
After DTA, the samples were examined with powder X-ray diffiaction. Reproducibility
of results was checked with multiple heating / cooling cycles.

Charge Transport Measurements: Thermopower was measured using an
instrument fi'om MMR Technologies, Inc., Mountain View, CA. The sample and the
reference (constantan wire) were mounted on a Seebeck stage with conductive silver
paste. The temperature gradient across the sample was built up by a computer controlled
heater which is controlled by the MMR Programmable Seebeck Controller 88100. The
Seebeck stage was attached to the MMR stage, which provides a given stable temperature
for the measurement. The MR K20A Programmable Temperature Controller controls
this MMR stage. The voltage across the sample resulting from the temperature gradient

was measured.

14

 

Poudt‘
ifiaetion for
sing a CPS
position-semi
wraparlson 0f
theCERlL'S:

Single
K; 4%} {51.814
feet. The int
effectometei
513 sphere of
lheShLART
reéuction. Th
solution \k as c

KPb;I
Strands PCT

WP Puma .

 

 

 

Powder X-ray diffraction: The compounds were examined by X-ray powder
diffraction for identification and to assess phase purity. Powder patterns were obtained
using a CPS 120 INEL diffi'actometer using Cu-Ka radiation and equipped with a
position-sensitive detector. The purity and homogeneity of all phases was confirmed by
comparison of X-ray powder diffraction to those calculated from single-crystal data using
the CERIUS2 software.9

Single-Crystal X-ray Crystallography: Single crystals of KszBisslo,
Ko_93Pb3.o4Bi4,34S9_6oTeo,4o and Nao_475Sr2_793Bi4,-,.3Selo were mounted on the tip of a glass
fiber. The intensity data were collected at 293 K on a Bruker SMART Platform CCD
diffractometer using graphite monochromatized Mo K, (it = 0.71073 A) radiation over a
full sphere of reciprocal space. Individual frames were measured using O.3° steps in (o.
The SMART software was used for data acquisition and SAINT'0 for data extraction and
reduction. The absorption correction was done with SADABS'O, and the structure
solution was done with the SHELXTL'O package of crystallographic programs.

KszBissm: A full sphere of data was collected with an exposure time of 30
seconds per frame. Structure refinement was straightforward in orthorhombic space
group ana. After anisotropic refinement final R values, R1 = 2.75% and wR2 = 6.91%.
The fractional atomic coordinates and isotropic displacement parameters are shown in
Table 2-2.

Ko,93Pb3,uBi4.3489,wTeo,4o: A full sphere of data was collected with an exposure
time of 20 seconds per frame. Eighteen crystallographically independent positions (Bi 1-5,
Pb 1-4, K 1, S 1-9 and Te 10) were found to sit on a crystallographic mirror plane. Pb(3)

& Pb(4) and Bi(1) & K(1) were found to be disordered over a single site. After

15

 

 

zisotrOPiC ”
rte-mic 000le

520.4?
of 30 second:

to sit on a cry

iational ate

:4.

 

 

anisotropic refinement final R values, R1 = 2.96% and wR2 = 6.06%. The fractional
atomic coordinates and isotropic displacement parameters are shown in Table 2-3.
Nao,475Srz,mBi4,-,13Selo: A full sphere of date was collected with an exposure time
of 30 seconds per frame. Eighteen crystallographically independent positions were found
to sit on a crystallographic mirror plane. Bi(l) & Sr(1), Bi(3) & Sr(3), Bi(4) & Sr(4), Sr(5)
& Na(5), Sr(6) & Na(6) and Sr(7) & Na(7) were all found to be disordered over a single
site. After anisotropic refinement final R values, R1 = 7.00% and wR2 = 12.61%. The
fractional atomic coordinates and isotropic displacement parameters are shown in Table

2-4.

16

 

Irblc 21 C11

XéxSILZrBh°‘S

Unethical form

formula weigh
T. K

1.1
Cash} system

Space group

L1

L1

 

 

 

Table 2-1. Crystallographic Data for KszBiSSm, Kbe4-2xBi4+xS10-yTey, and

NaxSI'4.2XBI4+xSC| 0.

Chemical formula
Formula weight

T, K

A. A

Crystal system
Space group

a, A

b, A

c, A

0., deg

13. deg

7. deg

v, A3

Z

Pearce. g/cm3

it. mm]

Total reflections
Unique reflections
R(int)

No. of parameters
Goodness-of-fit on F2
Refinement method
R1ll

wR2b

KszBissm
487.33
293(2)
0.71073

ana
23.92700)
4.1 103(16)
19.315(8)
90

9O

90
1899.6(13)

14
5.964
64.327

21493
2674
0.0452
1 10
1.031

0.0275
0.0691

K0.93Pb3.043i4.3439.6oT60.4o Nao.4753f2.79sBi4.7135610

614.93
293(2)
0.71073
Orthorhombic
ana
24.11 1(12)
4.089(2)
19.371(9)
90
90
90
1909.8(16)

11
5.881
54.397

20504
2536
0.0577
114
0.911

8172.56
293(2)
0.71073

ana
24.512(15)
4.247(3)
20.205(13)
90

90

90

2104(2)

1
6.451
64.625

16913
2788
0.1820
117
1.013

Full-matrix least-squares on F2

0.0296
0.0606

0.0700
0.1261

‘ R1 = z IlFol-chll/ZIFOI- " wR2 = {z [W(Foz-Fc2)2]/ZIW(F02)ZI}”2-

17

Table 2-2. Ator

11:1 IN) for 1

311)
32:31
813)
Bil-‘1
31le5)
Full
or;
Kill
511)
3(2)

Sill
5(5)
16}
Si?)
18)
$19)
Sill)
\

 

 

Table 2—2. Atomic coordinates (x 104) and equivalent isotropic displacement parameters

(A2x 103) for KszBi5S10.

 

 

x y z U(eq)
Bi(l) 1507(1) 2500 161(1) 17(1)
Bi(2) 1716(1) -2500 -1897(1) 15(1)
Bi(3) 93(1) -2500 -961(1) 19(1)
Bi(4) 2020(1) -2500 4090(1) 14(1)
Bi(5) 688(1) -7500 4651(1) 18(1)
Pb(l) 428(1) 2500 -2751(1) 18(1)
Pb(2) 2865(1) -2500 1 157(1) 29(1)
K(1) 1301(1) -2500 2171(2) 18(1)
S(l) 885(1) 2500 -1367(2) 19(1)
8(2) 1402(1) -7500 3536(2) 17(1)
S(3) -272(1) -2500 -2252(2) 17(1)
8(4) 2219(1) -2500 -326(2) 20(1)
S(5) 1409(1) -12500 5211(2) 18(1)
S(6) 1235(1) -2500 -3094(2) 17(1)
S(7) -35(1) -7500 5893(2) 22(1)
3(8) -699(1) -7500 -564(2) 25(1)
8(9) 2376(1) -7500 -2312(2) 16(1)
S(lO) 2046(1) 2500 1321(2) 17(1)

 

U(eq) is defined as one third of the trace of the orthogonalized Uij tensor.

18

 

rmeJ.AH

113x103) 101

 

hill
n2)
as;
all

Bill 1
8:12)
EB)
Bit)
ho)
51.11
in
Rh
8.4}
13
8'6)

 

$8)
319)
16110)

islSdefi:

 

Table 2-3. Atomic coordinates (x 104) and equivalent isotropic displacement parameters

(AZX 103) for K0.93Pb3.04Bi4.34S9.60TCO.40~

 

 

x y z U(eq) Occ.
Pb(l) 4899(1) -2500 10957(1) 23(1)
Pb(2) 2143(1) -2500 8834(1) 32(1) 0.42601
Pb(3) 5681(1) -2500 14587(4) 19(1) 0.46327
Pb(4) 5701(1) -2500 14725(4) 22(1) 0.53673
K(1) 3706(2) -2500 7802(3) 25(1) 0.87487
Bi(l) 3708(3) -2500 8034(4) 36(2) 0.12513
Bi(2) 3490(1) 2500 9831(1) 20(1)
Bi(3) 3271(1) -2500 11889(1) 18(1)
Bi(4) 7015(1) -7500 14097(1) 17(1)
Bi(5) 4564(1) 2500 12726(1) 25(1)
S(l) 4110(1) 2500 11359(2) 21(1)
S(2) 6384(1) -2500 1352 1 (2) 17(1)
S(3) 5270(1) -2500 12243(2) 23(1)
S(4) 2769(2) -2500 10318(2) 24(1)
8(5) 2612(1) -7500 12304(2) 19(1)
S(6) 6409(2) -7500 15219(2) 23(1)
8(7) 3758(1) -2500 13073(2) 20(1)
S(8) 4283(2) -2500 9426(2) 25(1)
S(9) 2971(2) 2500 8670(2) 21(1)
Te(10) 4984(1) -2500 15908( 1) 27(1) 0.18924

 

U(eq) is defined as one third of the trace of the orthogonalized Uij tensor.

l9

 

Table 2-1

: 5 r ‘:
IA'X 1 A). i

Sal)
Sell)
56(3)
Soil)
Sail
56.5)
3‘17.)

5:9)
56110)

L'

E“1.115 deC.
1‘1

Table 2-4. Atomic coordinates (x 104) and equivalent isotropic displacement parameters

(AZX 103) for Nao.4753f2.79sBi4.7133610-

 

 

x y z U(eq) Occ.
Bi(l) 1513(1) 2500 9824(1) 14(1) 0.89828
Sr(l) 1513(1) 2500 9824(1) 14(1) 0.10172
Bi(2) 1719(1) -2500 11920(1) 16(1) 0.49244
Bi(3) 99(1) -2500 11006(1) 17(1) 0.89034
Sr(3) 99( 1) -2500 1 1006(1) 17(1) 0.10966
Bi(4) 2998(1) -7500 10934( 1) 17(1) 0.93817
Sr(4) 2998(1) -7500 10934(1) 17(1) 0.06183
Bi(5) 4358(1) -12500 10390(1) 23(1)
Sr(S) 3708(2) -7500 12897(2) 20(2) 0.79289
Na(5) 3708(2) -7500 12897(2) 20(2) 0.2071 1
Sr(6) 2968(1) -2500 8864(2) 15(1) 0.95836
Na(6) 2968( 1) -2500 8864(2) 15(1) 0.04164
Sr(7) 5423(2) -17500 12283(2) 21(2) 0.77261
Na(7) 5423(2) -17500 12283(2) 21(2) 0.22739
Se(l) 885(1) 2500 11308(2) 15(1)
Se(2) 2257(2) -2500 10313(2) 18(1)
Se(3) 3613(2) -7500 9789(2) 15(1)
Se(4) 2411(2) -7500 12301(2) 15(1)
Se(5) 5033(2) -17500 10874(2) 19(1)
Se(6) -346(2) -2500 12223(2) 18(1)
Se(7) 723(2) -2500 9438(2) 19(1)
Se(8) 2018(1) 2500 8628(2) 15(1)
Se(9) 3628(2) -12500 11563(2) 19(1)
Se(lO) 1244(2) -2500 13116(2) 16(1)

 

U(eq) is defined as one third of the trace of the orthogonalized Uij tensor.

20

 

D. Results

Structure Dt
This
£116?de mai
reels filled
cries are git
a: Figure 2-1
ocnhedral
chalcogenide:
51;". coordin
lb? same wa
3’833155331' 1
“ism 2.2
CLamels whj
313 Similar to
AIOm
while the M
234913) to
insult in a

bond P 5121

 

mad b1“ ei :~ l

 

D. Results and discussion

Structure Description of KszBissm

This compound is isostructural with KBi6.33Slo and has a three dimensional
structure made up of NaCl-type blocks and CdIz-type fragments that connect to form
tunnels filled with eight-coordinate K+ cations. The bond distances and selected bond
angles are given in Tables 2-7 and 2-8. The structural diagram down the b-axis is shown
in Figure 2-1. The existence of these types of NaCl- and CdIz-type fragments with Bi in
an octahedral coordination site is a very common structural motif found in most bismuth
chalcogenides. The two different fragments of NaCl-type and Cdlz-type are joined by
eight coordinated Pb atoms (i.e., Pb(2)) which are in a bicapped prismatic geometry, in
the same way as Bi is found in KBi6_33Slo 8 and various mineral sulfo salts.'1 The
[szBissiol' framework is made of edge-sharing MS6 (M = Bi, Pb) octahedra, as shown
in Figure 2.2. An interesting feature is the presence of small triangular shaped empty
channels which are lined by Bi(5)-S(7)-Pb(1)-S(6)-Pb(2)-S(5). These types of channels
are similar to the KBi6,33Slo structure.

Atoms Pb(l) and Bi(5) are present in a slightly distorted octahedral coordination
where the M-S (M = Bi, Pb) distances range from 2.820(2) to 2.897(2) A for Pb(l) and
2.749(3) to 2.957(4) A for Bi(5). On the other hand Bi(l), Bi(2), Bi(3) and Bi(4) are
present in a highly distorted octahedral coordination with a short bond trans to a long
bond. Pb(2) is present in a bicapped prismatic geometry where its coordination sphere is

filled by eight sulfur atoms and the bond length ranges fi'om 2.856(2) to 3.310(1) A.

21

..-I"

- 'u‘.l'h'-JA

 

l'lermal Ana
Ililerential th
eel: 'hermal l
decompositior
oéohermic

Im'sallizati

irritated no d

Charge Tran
Tiennoelectri
1.311111 b)‘ Br
mpemture tl

lkfiflmz

 

 

Thermal Analysis of KszBissm

Differential thermal analysis was performed on pure KszBiSSm samples to ascertain
their thermal behavior. At the end of two heating cycles the compound was checked for
decomposition by taking its powder X-ray diffraction pattern. KszBiSSm shows an
endothermic (melting) peak at 728°C and on cooling shows an exothermic
(recrystallization) peak at 703°C. The powder pattern of the compound after DTA

indicated no decomposition. (See Figure 2-3.)

Charge Transport Measurement of KszBiSSm

Thermoelectric power measurements were carried on polycrystalline oriented ingots
(grown by Bridgman technique) '2 of KszBiSSlo. It is a n-type conductor and at room
temperature the thennopower has a value of -1 33 uV/K. It shows a linear trend till 400 K.

(See Figure 2.4.)

22

figure 2-1. P

 

 

 

Figure 2-1. Projection of the structure of KszBisslo down the b-axis.

NaCl-type

,.

e / Q“ e..

Pooh'fibo of"
o 9', ‘

. f s-

It? '5“

- e“
9‘» e‘gRQ‘ - ‘o‘

    

 

 

23

Figure 2-2. Polyhedral representation of KszBisslo down the b-axis showing the

connectivity of the MS; octahedra (M = Bi, Pb).

 

24

 

IkaSBm

hnthOI
hdiRJle
Shihllxl
aural)

18186)
hfirh9lx2
hfllhl)x2
$0184)

 

lfilh3l
BfllSBJXI
Afiihl)xl
16118)

1U115)
Adlhzlx
huluilx
3115(9)

 

Rmihl)

Table 2-5. Bond distances (A) for KszBisslo.

Bi(l)-S(10)
Bi(1)-S(4) x 2
Bi(1)-S(8) x 2
Bi(1)-S(1)

Bi(2)-S(6)
Bi(2)-S(9) x 2
Bi(2)-8(1) x 2
Bi(2)-S(4)

Bi(3)-S(3)
Bi(3)-S(8) x 2
Bi(3)-S(1) x 2
Bi(3)-S(8)

Bi(4)-8(5)
Bi(4)-S(2) x 2
Bi(4)-S(4) x 2
Bi(4)-S(9)

Bi(5)-S(2)

2.586(3)
2.830(2)
2.927(3)
3.305(1)

2.583(3)
2.713(2)
3.038(3)
3.264(1)

2.643(3)
2.899(2)
2.903(2)
3.282(1)

2.612(3)
2.748(2)
2.969(2)
3.069(3)

2.749(3)

Bi(5)-S(7) x 2
Bi(5)-8(5) x 2
Bi(5)-S(7)

Pb(1)-S(3) x 2
Pb(1)-S(6) x 2
Pb(1)-S(7)
Pb(1)-S(l)

Pb(2)-S(10) x 2
Pb(2)-S(5) x 2
Pb(2)-S(6) x 2
Pb(2)-S(9)
Pb(2)-S(4)

K(1)-S(10) x 2
K(1)—S(3) x 2
K(1)-S(2) x 2
K(1)-S(9)
K(1)-S(8)

2.786(2)
2.894(2)
2.957(4)

2.820(2)
2.897(2)
2.844(3)
2.888(3)

2.856(2)
3.253(1)
3.310(1)
3.012(3)
3.254(1)

3.178(3)
3.211(3)
3.352(3)
3.319(4)
3.423(5)

 

liblc 2-6. Se?

38181115
$31811h5h
1141181115
Sl-IrBllll‘Sll
5441811150
SlIrBllll-Sll

1618131511.
StirBilZl-Sl‘j
Sill-Billl-Sl
19.181219
19181313“
5111812 )-S(

5131813 18
soloists.
SiirBlij3)-3(
513181013.
5181313”.
311131313

 

SISI'Bll-I)-S

 
 
   
  

SciBlh-s
Wists
51518114}:
113.1814};
314.1814“

 

Table 2-6. Selected Angles (deg) for KszBisslo.

S(10)-Bi(1)-S(4)

S(4)-Bi(1 )-S(4)

S(10)-Bi(1)-S(8)

S(4)-Bi(1)-S(8)
S(4)-Bi(1)-S(8)
S(8)-Bi(l)-S(8)

S(6)-Bi(2)-S(9)
S(9)-Bi(2)-S(9)
S(6)-Bi(2)-S(1)
S(9)-Bi(2)-S(1)
S(9)-Bi(2)-S(1)
S(1)-Bi(2)-S(1)

S(3)-Bi(3)-S(8)
S(8)-Bi(3)-S(8)
S(8)-Bi(3)-S(l)
S(3)-Bi(3)-S(1)
S(8)-Bi(3)-S(1)
S(1)-Bi(3)-S(l)

S(5)-Bi(4)-S(2)
S(2)-Bi(4)-S(2)
S(2)-Bi(4)-S(4)
S(5)-Bi(4)-S(4)
S(2)-Bi(4)-S(4)
S(4)-Bi(4)-S(4)

8924(9)
9313(10)
9568(9)
8863(7)

174.80(10)

89.21(10)

8969(8)
98.49(10)
9052(8)

173.33(7)

8818(7)
8515(9)

9193(9)
9029(10)
8978(7)
8772(8)

179.64(10)

90.14(10)

9124(8)
96.8000)

174.60(8)

9160(8)
87.72(7)
8761(9)

26

S(5)-Bi(4)-S(9)
S(2)-Bi(4)-S(9)
S(4)-Bi(4)-S(9)

S(2)-Bi(5)-S(7)
S(7)-Bi(5)-S(7)
S(7)-Bi(5)-S(5)
S(2)-Bi(5)-S(5)
S(7)-Bi(5)-S(5)
S(5)-Bi(5)-S(5)
S(2)-Bi(5)-S(7)
S(7)-Bi(5)-S(7)
S(5)-Bi(5)-S(7)

S(3)-Pb(1)-S(3)
S(3)-Pb(1)-S(7)
S(3)-Pb(1)-S(1)
S(7)-Pb(1)-S(1)
S(7)-Pb(1)-S(6)
S(3)-Pb(1)-S(6)
S(3)-Pb(1)-S(6)
S(1)-Pb(1)-S(6)
S(6)-Pb(1)-S(6)

S(10)-Pb(2)-S(10)
S(10)-Pb(2)-S(9)

174.06(9)
8482(8)
9268(8)

9307(9)
95.07(10)
177.39(8)
8551(8)
8720(7)
9050(9)
177.33(9)
8874(8)
9261(8)

93.57(10)
9481(8)
8474(8)
179.3400)
9283(8)
8762(7)
172.16(9)
8763(8)
9037(9)

92.02(10)
76.14(7)

Figure 2.3. D

1'26 heating a]

m

 

 

Figure 2.3. DTA diagram of KszBisslo showing the endothermic and exothermic peaks.

The heating and cooling rates were 10°C/min.

20~

10'

“\ 9’“

200

703°C

 

400 600 800 1 000

Temperature (°C)

27

Figure 2.4.

-I3C

 

n4. :4. w
1 1 ‘II

o o I
AV_.\>.JV m LogohunvPEBCL.

455

160

 

 

Figure 2.4. Variable temperature thennopower for a polycrystalline oriented ingot of

KszBIsSlo.

-130 '
-135 l
'140 ' Q

445 . ’

Thennopower S (uVIK)

-150 . o
-155 '

-160 ' .- - ' ‘
300 320 340 360 380 400 420
Temperature (K)

28

C” "T'lfl

 

structure I
the
("3111311 51-;
(~35 herebj
metre 1*
nitrite 2
pp: and C
amels bu'
Kill. The
nicturalc
Att
site with 8
Iii-c Pb. l
33.1: 511110
2.3. Phil).
'1 tellunr
them in
Bill) and

tustoal

Structure Description of K,Pb4.z‘Bi4+,Slo.yTey

The idea of using tellurium here was to investigate whether it goes to a different
site than sulfur thereby creating a new structure or whether it goes to the same chalcogen
site thereby creating a known structure. In our research we ended up in getting a known
structure with a small uptake of tellurium in the sulfur site. The compound has a similar
structure as KszBisslo where we have a three dimensional network made up of NaCl-
type and Cdlz-type fragments. But here unlike KszBisSm these fragments do not form
tunnels but instead the K+ cations are disordered with one of the Bi3+ ions (i.e., Bi(l) &
K(l)). The bond distances and selected angles are given in Table 2.9 and 2.10. The
structural diagram down the b-axis is shown in Figure 2.6.

Atoms K(1) and Bi(l) are disordered in the highly coordinated bicapped prismatic
site with 87% K and 13% Bi. The other highly coordinated site is occupied by Pb(2) with
43% Pb. In these sites similar to KszBisSlo the metal coordination sphere is filled by
eight sulfur atoms. Here the CdIz-type fragments are made of disordered Pb atoms (Pb(3)
and Pb(4)) and Te atoms (Te(10)). The lead sites have 46% of Pb(3) and 54% Pb(4) and
the tellurium site is a partially filled site with 19% Te(10). Bi(5), Pb(3) and Pb(4) are
present in a slightly distorted octahedral coordination. On the other hand Pb(l), Bi(2),
Bi(3) and Bi(4) are present in a highly distorted octahedral coordination with a short bond

trans to a long bond.

29

 

- 1

JV..

Figure 2-5. Projection of the structure of Ko.93Pb3_o4Bi4.3489_6oTeo_4o down the b-axis.

co ‘0‘ 0" Ge ‘0‘ e‘
.' ... ‘b w. ... 1’
'O'Wv 03"?” >

'05? 2‘?
O . .Bi
0": 3:.

30

Figure 2-6. Polyhedral representation of K093Pb1043i434snge040 down the b-axis

showing the connectivity of the M86 octahedra (M = Bi, Pb, Bi/K).

 

31

 

 

Table 2-7. Bond distances (A) for Kbe4-2xBi4+xS(o-yTey.

Pb(1)«S(3)
Pb(l)-S(l) x 2
Pb(1)-S(8) x 2
Pb(l)-S(8)

Pb(2)-S(9) x 2
Pb(2)-S(6) x 2
Pb(2)-S(7) x 2
Pb(2)-8(5)
Pb(2)-S(4)

Pb(3)-S(2)
Pb(3)-Te(10) x 2
Pb(3)-S(6) x 2
Pb(3)-Te(10)

Pb(4)«S(6) x 2
Pb(4)-Te(10) x 2
Pb(4)—S(2)
Pb(4)-Te(10)

K(1).S(9) x 2
K(1)-S(3) x 2
K(1)-S(2) x 2
K(1)-S(5)
K(1)-S(8)

2.647(4)
2.899(3)
2.936(3)
3.316(1)

2.875(3)
3.267(1)
3.328(1)
3.022(4)
3.247(1)

2.671(7)
2.769(4)
2.960(5)
3.061(7)

2.831(4)
2.899(5)
2.855(7)
2.869(6)

3.186(5)
3.207(4)
3.287(5)
3.322(6)
3.439(7)

32

Bi(1)-S(9) x 2
Bi(1)-S(3) x 2
Bi(l)-S(2) x 2
Bi(1)-S(5)
Bi(l)-S(8)

Bi(2)-8(1)
Bi(2)-S(9)
Bi(2)-S(4) x 2
Bi(2)-S(8) x 2

Bi(3)-S(4)
Bi(3)-S(7)
Bi(3)-8(5) x 2
Bi(3)-8(1) x 2

Bi(4)-S(6)
Bi(4)—S(2) x 2
Bi(4)-S(4) x 2
Bi(4)-8(5)

Bi(5)-S(3) x 2
Bi(5)-Te(10)
Bi(5)-8(1)
Bi(5)-S(7) x 2

2.975(6)
3.248(1)
3.648(1)
3.483(1)
3.031(8)

3.316(1)
2.574(4)
2.844(3)
2.907(3)

3.274(1)
2.577(4)
2.712(2)
3.054(3)

2.620(4)
2.782(2)
2.962(3)
3.072(4)

2.820(3)
2.862(3)
2.865(4)
2.900(3)

 

hill

9'91

S391

NEILE

Table 2-8. Selected Angles (deg) for Kbe4-2xBi4+xSm-yTey.

S(3)—Pb(l)-S(l)
S(l)-Pb(1)-S(1)
S(3)-Pb(1)-S(8)
S(l)-Pb(1)-S(8)
S(l)-Pb(1)-S(8)
S(8)-Pb(l)-S(8)

S(9}Pb(2)-S(9)
S(9)-Pb(2)-S(5)

S(2)-Pb(3)-Te(10)
Te(lO)-Pb(3)-Te(10)

S(2)-Pb(3)-S(6)

Te(10)-Pb(3)-S(6)
Te(10)-Pb(3)-S(6)

S(6)-Pb(3)-S(6)

S(2)-Pb(3)-Te( 1 0)
Te( 1 O)-Pb(3 )-Te( 1 0)
S(6).Pb(3)-Te( l O)

S(6)-Pb(4)-S(6)
S(6)-Pb(4)-S(2)
S(5)-Bi(3)-S(1)
S(1)-Bi(3)-S(l)

S(6)-Bi(4)-S(2)
S(2)-Bi(4)—S(4)
S(4)-Bi(4)-S(4)
S(6)-Bi(4)-S(S)

88.18(9)
89.71(10)
9061(9)
91.01(8)
178.57(10)
88.26(11)

90.66(1 1)
75.89(8)

95.7(2)
95.2(2)
8675(10)

175.2(3)
88.65(7)
87.4(2)

173.9(3)
88.39(10)
88.9(2)

92.48(19)
85.88(10)

173.09(7)
8406(10)

9158(9)
88.97(8)
87.30(10)

174.05(10)

33

S(6)-Pb(4)-Te(lO)
S(2)-Pb(4)-Te(10)
S(6)-Pb(4)-Te(10)
S(2)-Pb(4)-Te(10)
Te(lO)-Pb(4)-Te(10)
S(6)-Pb(4)-Te(10)
Te(10)-Pb(4)-Te(10)
S(9)-Bi(l)-S(9)
S(9)-Bi(1)-S(8)

S(9)-Bi(2)—S(4)
S(4)-Bi(2)-S(4)
S(9)-Bi(2)-S(8)
S(4)-Bi(2)-S(8)
S(4)-Bi(2)-S(8)
S(8)-Bi(2)-S(8)

S(7)-Bi(3)-S(5)
S(5)-Bi(3)-S(5)
S(7)-Bi(3)-S(l)
S(5)-Bi(3)-S(l)

S(2)-Bi(4)-S(2)
S(6)-Bi(4)-S(4)
S(2)-Bi(4)-S(4)

S(2)-Bi(4)-S(5)
S(4)-Bi(4)-S(5)

95.4(2)
178.2(2)
8869(7)
89.0(2)
89.72(8)
174.6(3)
8968(18)
86.8(2)
84.53(19)

89.59(10)
91 .92(1 1)
94.80(10)
175.49(11)
89.18(8)
89.39(11)

90.16(9)
97.87(1 1)
89.87(9)
89.04(8)

94.60(l l)

91.44(10)
175.26(8)

84.40(8)
92.86(9)

 

 

Table 1

3.13131
313sz

15111

Table 2-8. (cont’d)

S(3)-Bi(5)-S(3)
S(3)-Bi(5)-Te(10)
S(3)-Bi(5)-S(1)
Te(10)-Bi(5)-S(1)

92.96(11)

94.43(8)

85.61(9)
179.94(9)

34

S(3)-Bi(5)-S(7)
Te(10)-Bi(S)-S(7)
S(l)-Bi(5)-S(7)
S(3)-Bi(5)-S(7)
S(7)-Bi(5)-S(7)

8830(8)
9235(8)
87.61(9)
172.99(10)
89.6400)

 

5mm

v
1.0-2‘

,'| .‘
.wb‘.

_ ~14;
"18211

Structure Description of N a,Sr4.2,Bi4+,Sem

The structure of this compound is very similar to the two previous one but
considering only ionic interactions between the alkali and alkaline earth metals with
chalcogenides the structure reduces to two dimensional structure having layers of NaCl-
type and Cdlz-type fragments joined together. The alkali and alkaline earth metals occupy
the sites in b etween these layers. The b 0nd distances and s elected angles are given in
Table 2-11 and 2-12. The structural diagram down the b-axis is shown in Figure 2-8.

All the three crystallographic sites between the layers are mixed occupied by the
alkali and alkaline earth metals. Sr(5) is mixed occupied with Na(S) with 79% Sr(5) and
21% Na(5), Sr(6) is mixed occupied with Na(6) with 96% Sr(6) and 4% Na(6) and Sr(7)
is mixed occupied with Na(7) with 77% Sr(7) and 23% Na(7). The BizTe3-type fragment
also has mixed occupation, by strontium and bismuth with one site containing only
bismuth (i.e., Bi(2)). Bi(l) is mixed occupied with Sr(l) with 90% Bi(l) and 10% Sr(1),
Bi(3) is mixed occupied with Sr(3) with 89% Bi(3) and 11% Sr(3) and Bi(4) is mixed
occupied with Sr(4) with 94% Bi(4) and 6% Sr(4).

Bi(5) is the only atom to be present in a slightly distorted octahedral coordination
where the Bi-Se distances range from 2.863(3) to 3.054(3). The remaining atoms
Bi(1)/Sr(1), Bi(2), Bi(3)/Sr(1) and Bi(4)/Sr(1) are all present in a highly distorted

octahedral coordination.

35

. .
' I

 

11

1"

Figure 2-7. Projection of the structure of Nao.4758r2,793Bi4_7.38e10 down the b-axis.

 

36

Figure 2-8. Polyhedral representation of Nao,475$r2.793Bi4.7l 38610 down the b-axis showing

the connectivity of the M86 octahedra (M = Bi, Bi/Sr).

 

37

 

la

Table 2-9. Bond distances (A) for NaxSr4-2xBi4+xSelo.

Bi(1)/Sr(1)-Se(8)
Bi(1)/Sr(1)-Se(1)
Bi(1)/Sr(1)-Se(2) x 2
Bi(1)/Sr(l)-Se(7) x 2

Bi(2)-Se(10)
Bi(2)-Se(2)
Bi(2)-Se(4) x 2
Bi(2)-Se(1) x 2

Bi(3)/Sr(3)-Se(6)
Bi(3)/Sr(3)-Se(7)
Bi(3)/Sr(3)-Se(1) x 2
Bi(3)/Sr(3)-Se(7) x 2

Bi(4)/Sr(4)-Se(3)
Bi(4)/Sr(4)-Se(4)
Bi(4)/Sr(4)-Se(9) x 2
Bi(4)/Sr(4)-Se(2) x 2

Bi(5)-Se(5)

2.715(4)
3.371(1)
2.968(3)
2.977(3)

2.682(4)
3.503(1)
2.825(3)
3.196(3)

2.691(4)
3.518(1)
2.931(3)
3.063(3)

2.761(4)
3.113(4)
2.918(3)
3.063(3)

2.958(5)

Bi(5)-Se(9)
Bi(5)-Se(5) x 2
Bi(5)-Se(3) x 2

Sr(5)/Na(5)-Se(8) x 2
Sr(5)/Na(S)-Se(6) x 2
Sr(5)/Na(5)-Se(9) x 2
Sr(5)/Na(5)-Se(4)
Sr(5)/Na(5)-Se(7)

Sr(6)/Na(6)-Se(8) x 2
Sr(6)/Na(6)-Se(3) x 2
Sr(6)/Na(6)-Se(10) x 2
Sr(6)/Na(6)-Se(4)
Sr(6)/Na(6)-Se(2)

Sr(7)/Na(7)-Se(5)
Sr(7)/Na(7)-Se(6) x 2
Sr(7)/Na(7)-Se(10) x 2
Sr(7)/Na(7)-Se(1)

2.971(4)
2.863(3)
3.054(3)

3.139(4)
3.153(4)
3.438(5)
3.400(6)
3.410(7)

3.187(4)
3.241(4)
3.245(4)
3.293(6)
3.408(6)

3.002(6)
3.010(4)
3.035(4)
3.065(6)

 

’1

Table 2-10. Selected Angles (deg) for NaxSr4-2xBi4+xSelo.

Se(8)-Bi(l)-Se(2)
Se(2)—Bi(l)-Se(2)
Se(2)-Bi(1)-Se(7)
Se(2)-Bi(l)-Se(7)
Se(8)-Bi(l)-Se(7)
Se(7)-Bi(1)-Se(7)

Se(lO)-Bi(2)-Se(4)

Se(4)-Bi(2)-Se(4)
Se(4)-Bi(2)-Se(1)

Se(lO)-Bi(2)-Se(1)

Se(4)-Bi(2)-Se(1)
Se(1)-Bi(2)-Se(1)

Se(6)-Bi(3)-Se(1)
Se(1)-Bi(3)-Se(l)
Se(6)-Bi(3)-Se(7)
Se(1)-Bi(3)-Se(7)
Se(1)~Bi(3)-Se(7)
Se(6)-Bi(3)-Se(7)

90.96(10)
91.36(12)

175.42(12)
8864(9)
93.62(1 1)
91.00(12)

90.88(10)
97.48(13)
8942(9)
94.06(10)
171.45(9)
83.27(10)

94.38(10)
92.86(12)
90.00(11)
174.85(12)
8949(9)
90.00(11)

39

Se(7)-Bi(3)-Se(7)
Se(3)-Bi(4)-Se(9)
Se(9)-Bi(4)-Se(9)
Se(3)-Bi(4)-Se(2)
Se(9)-Bi(4)-Se(2)
Se(9)-Bi(4)-Se(2)
Se(2)-Bi(4)-Se(2)
Se(3)-Bi(4)-Se(4)
Se(9)-Bi(4)-Se(4)
Se(2)-Bi(4)-Se(4)

Se(5)-Bi(5)-Se(5)
Se(5)-Bi(5)-Se(5)
Se(5)-Bi(5)-Se(9)
Se(5)-Bi(5)-Se(9)
Se(5)-Bi(5)-Se(3)
Se(5)-Bi(5)-Se(3)
Se(5)-Bi(5)-Se(3)
Se(9)-Bi(5)-Se(3)
Se(3)-Bi(5)-Se(3)

87.80(12)
94.35(11)
9342(13)
88.89(11)
8930(8)
175.59(11)
87.78(11)
174.43(11)
81.86(10)
95.11(10)

95.75(13)
90.21(11)
94.30(11)
173.26(12)
87.65(10)
8802(9)
175.68(10)
87.50(10)
88.13(12)

 

3.3T
ifiA

14,

El

E. Conclusion

The synthesis and structure of three new quaternary bismuth chalcogenides have
been presented. Variations in the cosalite structure type are observed whereby replacing
the softer Pb2+ with harder Sr2+ collapses the three dimensional character of the cosalite
structure to a layered type. The charge—transport properties of K,‘Pb4.2,‘Bi.1+,,Sl0.,Tey and
NaxSr¢2xBi4+xSem need to be investigated. Also it would be interesting to do some ion-

exchange reactions with NaxSr4-2xBi4+xSem.

4O

 

lel

References

1.

(a) Kaibe, H.; Tanaka, Y.; Sakata, M.; Nishida, I. J. Phys. Chem. Solids 1989, 50,
945-950. (b) Je on, H .-W.; H a, H .-P.; H yun, D .-B.; S him, J. -D. J. Phys. Chem.
Solids 1991, 4, 579-585.

(a) Feichtner, J. D.; Roland, G. W. Appl. Opt. 1972, 11, 993-998. (b) Balhnan, A.
A.; B yer, R. L.; E imerl, D .; Feigelson, R. S .; Feldman, B. J. ; Goldberg, L. S .;
Menyuk, N.; Tang, C. L. Appl. Opt. 1987, 26, 224-227.

Takagi, J.; Takeuchi, Y. Acta Crystallogr. 1972, 328, 649-651.

Takeuchi, Y.; Takagi, J. Proc. Jpn. Acad. 1974, 50, 76-79.

Skowron, A.; Boswell, F. W.; Corbett, J. M.; Taylor, N. J. J. Solid State Chem.
1974, 112, 307-311.

(a) Slack, G. A. New Materials and Performance Limits for Thermoelectric
Cooling. In CRC Handbook of Thermoelectrics; Rowe, D. M., Ed,; CRC Press:
Boca Raton, F1, 1995; pp 407-440. (b) Slack, G. A. Solid State Physics;
Ehrenreich, H., Seitz, F., Tumbull, D., Eds.; Academic: New York, 1997; Vol. 34,

pl.

Choi, K. -S.; Chung, D. -Y.; Mrotzek, A.; Brazis, P.; Kannewurf, C. R.; Uher, C.;
Chen, W.; Hogan, T.; Kanatzidis, M.G. Chem. Mater. 2001, 13, 756-764.

Kanatzidis, M.G.; McCarthy, T. J.; Tanzer, T. A.; Chen, L. H.; Iordanidis, L.
Chem. Mater. 1996, 8, 1465-1474.

CERIUSZ, Version 3.8., Molecular Simulations Inc., Cambridge, England, 1999.

10. SAINT v6.45, 1997-2003, SHELXTL v5.1, 1998, Bruker Analytical Xray

Systems Inc., Madison, WI 53719, USA.

41

11. (a) Makovicky, E. Eur. .1. Mineral. 1993, 5, 545-591. (b) Makovicky, E. Fortschr.
Miner. 1981, 59,137-190. (c) Makovicky, E. Neues Jahrbuch Miner. Abh. 1989,
160, 269-297.

12.Kyratsi, T.; Chung, D. -Y.; Choi, K. —-S.; Dyck, J. S.; Chen, W.; Uher, C.;
Kanatzidis, M. G. Mat. Res. Soc. Symp. Proc. 2000, 626, 28.8.1.

42

 

If—JON4I 5‘ t. I.» u ._ id .
we . . ..
A. r... v.

CHAPTER 3

Variation in the K2,5Bi8,58e14 structure type: Synthesis and Structure of

Rb.+,Pb3.szi7+,Se.4.yTey and N axBafixBimSeM.

A. Introduction

Bismuth compounds constitute a great part of the sulfosalt family.1 These
naturally occurring minerals present a remarkable structural diversity and complexity.
These characteristics are also found in the great number of ternaryz'8 and quatemarys’”
bismuth c halcogenides synthesized d uring the last d ecade. T he rich c ompositional and
structural variety makes them some of the most adaptable and versatile systems in solid
state chemistry. Bismuth atoms both in naturally occurring sulfosalts and in the above
mentioned compounds show an amazing flexibility in bonding. Although they usually
exhibit a distorted octahedral geometry, however they also adopt variety of other
coordination ranging from trigonal pyramidal in B-CsBiSz3, to square pyramidal in
szBigSen”, to trigonal prismatic in ALnlixBimSg (A = K, Rb; Ln = La, Ce, Pr, Nd)9
and sometimes the coordination number can range upto nine.2'12 These high-coordination
sites (> 6) serves to connect with each other the several NaCl-, BizTe3 and CdIz-type
blocks, formed by the BiQ6 (Q = chalcogen) octahedra when combined together by
sharing edges. These above mentioned blocks come in different sizes creating even more

structural possibilities. Another reason for the structural heterogeneity is the mixed

43

occupancy that bismuth atoms can display with a variety of similar sized ions such as
allitali‘la’l4 or alkaline earth metalss, Pb8’ ”’ '5, Sng' '2’ '5 , or lanthanides.9

Examples of the above mentioned structural diversity and complexity can be
found in compounds reported earlier from our group such as KBi385,3 KBi(5,3,3Sm,4a a—,B-
KzBissels, 2’ M K2.5Bi85S€14l4. KszBissw,l6 Kbe4-2xBi4+xslo-yTey516 I‘IaxSI'4-2xBi4+xS¢10l6
and many more. Our idea to move from ternary systems to quaternary system was that the
latter would give a much more complex structure thereby strongly scattering acoustic
lattice phonons carrying heat and thus lowering the thermal conductivity. This would lead
to better thermoelectric materials.

We report here the synthesis and structural characterization of Rb1+be3-

2,,Bi7+,,SeM.yTey and NaxBa5-2xBi6+xSe14 belonging to the K2,5Bi3,5Se14 structure type.

B. Experimental Section

Reagents: Chemicals were used as obtained: (i) bismuth chunks, 99.999% purity,
Cerac, Milwaukee, WI. (ii) selenium shots 99.999% purity, Cerac, Milwaukee, WI. (iii)
tellurium chunks 99.999% purity, Cerac, Milwaukee, WI. (iv) lead metal, Cerac,
Milwaukee, WI. (v) rubidium metal, 99.8% purity, Alfa Aesar, Ward Hill, MA. (vi)
sodium metal, Aldrich, Milwaukee, WI. (vii) barium selenide powder 99.5% purity, -20
mesh, Cerac, Milwaukee, WI. A2Se (A = Na, Rb) was prepared by a stoichiometric
reaction of alkali metal and selenium shots in liquid ammonia.

Synthesis: All manipulations were carried out under a dry nitrogen atmosphere in

3 Vacuum Atmospheres Dri-Lab glovebox. The purity and homogeneity of the products

was verified by comparing the X-ray powder diffraction patterns to those calculated by
the crystallographically determined atomic coordinates.

Bi;Se3: A mixture of 6.383g (0.045 mol) of bismuth and 3.617g (0.068 mol) of
selenium was transferred into a 13mm quartz tube, which was then flame sealed under
vacuum (~10‘4 Torr). The tube was heated to 800°C in 10 hours and isothenned there for
10 hours and then cooled down to 50°C in 10 hours. The product was used for further
reactions.

PbTe: A mixture of 12.378g (0.060 mol) of lead and 7.622g (0.060 mol) of
tellurium was transferred into a 13mm carbon coated quartz tube, which was then flame
sealed under vacuum (~10‘1 Torr). The tube was heated to 1100°C in 8 hours, held there
for 12 hours and then cooled down to 50°C in 24 hours. The product was used for further
reactions.

szBisSeu: A mixture of 0.871 g (3.50 mmol) of rubidium selenide and 9.129g
(0.140 mol) of bismuth selenide was transferred into a 13mm quartz tube, which was then
flame sealed under vacuum (~10'4 Torr). The tube was placed under the flame of a
natural gas-oxygen torch until the mixture melted, and then the tube was removed from
the flame and the molten mixture was allowed to solidify. The procedure was repeated
two more times to ensure homogeneity. The product was used for further reactions.

Rb1+,Pb3.2,Bi7+,,Se14-yTe,: A mixture of 0.4g (0.140 mmol) of Rb;BigSe13 and
0.047g (0.140 mmol) of lead telluride in the ratio 1:1 was transferred into a 9mm quartz
tube, which was then flame sealed under vacuum (~104 Torr). The tube was heated to

850°C in 10 hours and isothenned there for 48 hours and then cooled slowly to 350°C in

45

96 hours and finally to 50°C in 3 hours. The product consisted of silvery-gray needle like
crystals. A quantitative analysis by Energy Dispersive Spectroscopy (EDS) using 8
Scanning Electron Microscope (SEM) was performed on several of these crystals which
gave an approximate composition of “Rbl.67Pbl,43Bi7_39$e13,31Te0,70”.

Na,Ba5.2,,Bi6+,Se14: A mixture of 0.03g (0.240 mmol) of Nazse, 0.286g (1.32
mmol) of barium selenide and 0.472g (0.720 mmol) of bismuth selenide in the ratio
0.5:2.79:3.69 were transferred into a graphite tube which was placed in a 13mm quartz
tube, which was then flame sealed under vacuum (~104 Torr). The tube was heated to
800°C in 24 hours and isothenned there for 24 hours and then cooled 50°C in 25 hours.
The product consisted of silvery-gray needle like crystals. Energy Dispersive
Spectroscopy (EDS) on several of these crystals gave an approximate composition of

‘N3133553Bi7423615.47”.

C. Physical Measurements

Energy Dispersive Spectroscopy: Quantitative microprobe analyses of the
compound were performed with a JEOL JSM-6400V Scanning Electron Microscope
equipped with a Tracor Northern Energy Dispersive Spectroscopy (EDS) detector. Data
were acquired u sing an accelerating v oltage o f 20 k V and a 3 0 se conds accumulation
time.

Differential Thermal Analysis: Differential Thermal Analysis (DTA) was
performed with a computer-controlled Shimadzu DTA-50 thermal analyzer. Ground
single crystals (30-40 mg) were sealed in silica ampoules under vacuum. A silica

ampoule containing alumina of equal mass was sealed and placed on the reference side of

46

the detector. The samples were heated to 1000°C at 10°C/min, then isothenned for 1
minute followed by cooling at 10°C/minute. The reported DTA temperature is the peak
temperature. Afier DTA, the samples were examined with powder X-ray diffiaction.
Reproducibility of results was checked with multiple heating / cooling cycles.

Charge Transport Measurements: Thermopower was measured using an
instrument from MMR Technologies, Inc., Mountain View, CA. The sample and the
reference (constantan wire) were mounted on a Seebeck stage with conductive silver
paste. The temperature gradient across the sample was built up by a computer controlled
heater which is controlled by the MMR Programmable Seebeck Controller SBlOO. The
Seebeck stage was attached to the MMR stage, which provides a given stable temperature
for the measurement. The MR K20A Programmable Temperature Controller controls
this MMR stage. The voltage across the sample resulting from the temperature gradient
was measured.

Room temperature electrical conductivity was measured by a four probe
technique using a Keithley 236 Source Measure Unit. 0.003 inch copper wires were used
for the c urrent and v oltage electrodes. M easurements o f the p ellet c toss-sectional area
and voltage probe separation were made with a calibrated binocular microscope.

Powder X-ray diffraction: The compounds were examined by X-ray powder
diffraction for identification and to assess phase purity. Powder patterns were obtained
using a CPS 120 INEL diffractometer using Cu-Ka radiation and equipped with a
position-sensitive detector. The purity and homogeneity of all phases was confirmed by
comparison of X-ray powder diffraction to those calculated from single-crystal data using

the CERIUS2 software.17

47

Single-Crystal X-ray Crystallography: Intensity data were collected at 293 K
on a Bruker SMART Platform CCD diffractometer using graphite monochromatized Mo
Kg (2. = 0.71073A) radiation over a full sphere of reciprocal space. Individual frames
were measured using 0.3° steps in (o. The SMART software was used for data acquisition
and SAINT ‘8 for data extraction and reduction. The absorption correction was done with
SADABS'S, and the structure solution was done with the SHELXTL18 package of
crystallographic programs.

RbL-nPb1,298i38e13,42Te059: A full sphere of data was collected with an exposure
time of 45 seconds per frame. The crystallographic data is shown in Table 3-1. Twenty
five crystallographically independent positions were found to sit on a crystallographic
mirror plane. Pbl & Rb2, Pb2, Rb3 & Pb3, Te2 & Se2 and Te14 & Se14 were all found
to be disordered over a single site. Afier anisotropic refinement final R values, R1 =
5.17% and wR2 = 11.75%. The fractional coordinates and isotropic displacement
parameters along with occupancies for disordered atoms are shown in table 3-2.

NalBa2,7gBi-;37Se.4: A hemisphere of data was collected with an exposure time of
30 seconds per frame. The crystallographic data is shown in Table 3-1. Twenty seven
crystallographically independent positions were found to sit on a crystallographic mirror
plane. Bi6 & Na6, Bi7 &Na7, Bi8 & Na8 and 8e15, Se16 & Se17 were all found to be
disordered over a single site. After anisotropic refinement final R values, R1 = 5.29% and
wR2 = 10.78%. The fractional coordinates and isotropic displacement parameters along

with occupancies for disordered atoms are shown in table 3-3.

48

Table 3-1. Crystallographic Data for Rb]+be3-2xBi7+xSe14-yTey and NaxBa5-2xBi6+xSe14.

Chemical formula
Formula weight
T, K

L A

Crystal system
Space group

a, A

b, A

c, A

(1, deg

13. deg

7. deg

v, A3

Z

Pcalcd. g/cm3

H. mm“

Total reflections
Unique reflections
Rant)

No. of parameters
Goodness-of-fit on F2
Refinement method
R1a

wR2b

RbI .73Pb129Bi8Sel342T6059

798.10
293(2)
0.71073

P2(1)/m
17.610(11)

4.213(3)
21.398(13)
90

109.348(9)
90

1497.9(16)
8
7.078

73.827

16731
3890

0.0860
151

1.009

0.0517
0.1175

N8133279Bi7373614
3554.62

293(2)

0.71073

Monoclinic

P2(1)/m
17.407(6)

4.3165(15)
21.747(7)
90
98.768(6)
90

1614.9(10)
2

7.310

64.326

14160
4245

0.1181

171
1.294

F ull-matrix least-squares on F2

0.0529
0.1078

‘ R1 = z IlFol-chll/ZIFOI- " sz = {z 1w(F.2-F£)21/21w(F.2)21}”2.

49

Table 3-2. Atomic coordinates ( x 104) and equivalent isotropic displacement

parameters (Azx 103) for Rb1.73Pb1,29B138e1 3_42Te0,59

 

 

x y z U(eq) Occ
Rb(l) 4216(2) 2500 3546(2) 29(1)
Bi(l) 5215(1) 2500 913(1) 21(1)
Bi(2) 7203(1) -2500 632(1) 28(1)
Bi(3) 3367(1) -2500 1387(1) 24(1)
Bi(4) 8913(1) -12500 4290(1) 21(1)
Bi(5) 8756(1) -7500 6155(1) 21(1)
Bi(6) 9180(1) -7500 2701(1) 24(1)
Bi(7) 9083(1) -7500 135(1) 23(1)
Bi(8) 6659(1) -12500 4816(1) 21(1)
Pb(l) 6679(2) -l7500 3101(2) 33(1) 0.69871
Rb(2) 6617(7) -17500 2855(8) 13(2) 0.30129
Pb(2) 1663(5) -7500 2104(9) 34(2) 0.40436
Rb(3) 1375(7) -7500 1933(6) 12(2) 0.43145
Pb(3) 1645(9) -7500 1895(17) 31(5) 0.18427
Se(l) 8305(2) -7500 1262(2) 22(1)
Te(2) 4512(2) 2500 1958(2) 22(1) 0.08409
Se(2) 4512(2) 2500 1958(2) 22(1) 0.91591
Se(3) 7872(2) -7500 4486(2) 21(1)
Se(4) 9716(2) -7500 7457(2) 21(1)
Se(S) 10173(2) -12500 842(2) 22(1)
Se(6) 8124(2) -12500 2952(2) 21(1)
Se(7) 4210(2) -12500 4916(2) 19(1)
Se(8) 7811(2) -12500 6372(2) 22(1)
Se(9) 4010(2) -2500 150(2) 19(1)
Se(10) 10068(2) -17500 4147(2) 17(1)
Se(11) 7896(2) -2500 -595(2) 28(1)
Se(12) 2833(2) -2500 2435(2) 25(1)
Se(13) 5794(2) -12500 3480(2) 29(1)

50

Table 3-2. (cont’d)

 

 

x y z U(eq) Occ
Te(14) 6333(2) -2500 1600(2) 21(1) 0.20309
Se(14) 6333(2) ~2500 1600(2) 21(1) 0.79691

 

U(eq) is defined as one third of the trace of the orthogonalized Uij tensor.

 

51

Table 3-3. Atomic coordinates (x 104) and equivalent isotropic displacement parameters

(Azx 103) for NajBa2_79Bi7.378e.4.

 

 

x y z U(eq) ’ Occ.
Bi(l) 3225(1) 7500 4771(1) 12(1)
Bi(2) 4553(1) -2500 11723(1) 17(1)
Bi(3) 1894(1) 2500 6034(1) 16(1)
Bi(4) 696(1) -2500 14326(1) 20(1)
Bi(5) 3929(1) 2500 9695(1) 25(1)
Bi(6) 2483(1) 2500 1 11 17(1) 22(1) 0.68214
Na(6) 2483(1) 2500 11117(1) 22(1) 0.31786
Bi(7) -503(1) 2500 12842(1) 19( 1) 0.53889
Na(7) -503( 1) 2500 12842(1) 19(1) 0.46111
Bi(8) 1809(2) 7500 9440(1) 40(1) 0.70179
Na(8) 1809(2) 7500 9440(1) 40(1) 0.29821
Bi(9) 362(1) -2500 10936(1) 42(1)
Ba(l) 2159(1) 2500 12982(1) 14(1)
Ba(2) 3153(1) 7500 7776(1) 13(1)
38(3) 5043(1) 7500 6315(1) 14(1)
Se(l) 3262(2) -2500 10420(2) 18(1)
Se(2) 2962(2) 7500 6200(2) 15(1)
Se(3) 1884(2) 2500 4510(2) 15(1)
Se(4) 5360(2) -7 500 10983(2) 20(1)
Se(5) 3742(2) -7500 12192(2) 15(1)
Se(6) 2641(2) 2500 8826(2) 18(1)
Se(7) 1824(2) -2500 1 1 766(2) 26(1)
Se(8) 4274(2) 2500 51 12(2) 13(1)
Se(9) 1734(2) 2500 7265(2) 16(1)
Se(10) 3500(2) 7500 3572(2) 12(1)
Se(l l) 5663(2) -2500 12737(2) 11(1)
Se(12) 1075(2) 2500 10143(2) 21(1)
Se(13) 720(2) -2500 13069(2) 18(1)

52

Table 3-3. (cont’d.)

 

 

x Y Z U(eq) Occ
Se( 14) 531(2) -2500 5778(2) 14( 1)
Se(15) -399(l6) -7500 1 1481 (6) 47(6) 0.68043
Se(16) -606(18) -6200(110) 1 1513(13) 24(10) 0.24310
Se(l 7) -70(50) -7500 1 1540(20) 45(17) 0.16378

 

U(eq) is defined as one third of the trace of the orthogonalized Uij tensor.

53

D. Results and discussion

Structure Description of Rb.+,,Pb3.2,,Bi-;.,,Se.4.,Tey

The compound is isostructural to K25Bi358e14 ‘ and possesses a complex 3D
anionic framework which is very similar to that of B- K2Bi88e13l (see Figure 3-1.). The
main difference being the presence of only NaCl- and BizTe3-type fi‘agments in case of
Rbl4,.Pb3.2,.Bi7+,,Se14.y'l‘ey whereas the presence of additional CdIz-type fragments in case
of B- KzBlgsfil3. These different types of fragments are common in other multinary
bismuth chalcogenides such as Cs3Bi7Se1219 and KBi(,-,33810.4a The BizTe3-type fragments
in Rbp.,,Pb3.2,.Bi7+,.Se.4.yTey are arranged side by side to form layers. The NaCl-type
fiagments connect these layers which run p erpendicular to the c -axis, to b uild a three
dimensional framework with tunnels which are filled by the alkali (Rb+) cations. The
NaCl-type fragments in Rb]..,,Pb3.2,,Bi7+,,Se14.,Tey are three bismuth octahedra wide
whereas the BizTe3-type fragments are five bismuth octahedra wide. The latter is an
important structural difference with the B- KzBigseU structure where these fi'agments are
three Bi octahedra wide.

Among the Rb+ cations in Rb]+be3-2xBi7+xSe14-yTey, Rb( 1) is fully occupied by
Rb+ while Rb(2) is disordered with Pb( 1) and Rb(3) is disordered with Pb(2) and Pb(3)
(see figure 3-1). The Rb(2) site contains 70% Pb and 30% Rb while the Rb(3) site
contains 43% of Rb, 40% of Pb(2) and 18% of Pb(3). There are two eight coordinate sites.
One is occupied by Pb(l) and Rb(2) in a distorted bicapped trigonal prismatic
coordination by Se(6), Se(6)’, Se(13), Se(13)’, Te14/Se(14), Te(14)/Se(14)’, Se(3) and
Te(2)/Se(2) (the atoms primed outside parentheses are the symmetrically equivalent ones).

Pb(l) is disordered with Rb(2) at 0.499(1)A. The other site has Rb(3), Pb(2) and Pb(3)

54

atoms in a similar kind of coordination. The prism is defined by Se(4), Se(5), Se(12) and
their symmetry equivalent atoms while the capping atoms are Se(8) and Se(ll). Here
Rb(3) is disordered with Pb(2) and Pb(3) at a distance of 0.518(3) and 0.51(2)A
respectively. These high-coordinate sites serve to stitch together the layers formed by
BizTe3-type fi'agments.

Two of the chalcogenide sites in the BizTe3-type fragments close to Pb(1)/Rb(1)
disordered site has mixed occupancy. The Se(2) site contains 92% of Se(2) and 8% of
Te(2). The Se(14) site contains 80% of Se(14) and 20% of Te( 14). Apart from Bi(6) all
the bismuth atoms in both types of fragments are present in a highly distorted octahedral
coordination with a short bond trans to a long bond. In contrast Bi(6) is in a slightly
distorted octahedral coordination where the Bi-Se distances range fi'om 2.953(4) to
2.974(3) (see Table 3-4. & 3-5.). This site also serves as the second joining point for the

two types of fragments.

55

Figure 3-1. Projection of the structure of Rbmngl,29BigSe1342Te059 down the b-axis.

 

56

RR

R

Ft

5:

2h

EB

Table 3-4. Bond distances (A) for Rb],73Pb1,nglgsCI3,42T6059.

Rb(l )~Se(12)
Rb(1)-Se(13)
Rb(1)-Se(7)
Rb(l)-Te(2)/Se(2)
Rb(1)-Se(7)
Rb(1)-Se(8)

Rb(2)-Se(13)
Rb(2)-Te(14)/Se(14)
Rb(2)-Se(6)
Rb(2)-Se(3)
Rb(2)-Te(2)/Se(2)

Rb(3)-Pb(3)
Rb(3)-Pb(2)
Rb(3)-Se(12) x 2
Rb(3)-Se(5) x 2
Rb(3)-Se(4) x 2
Rb(3)-Se(8)
Rb(3)-Se(11)

Bi(1)-Te(14)/Se(14) x 2
Bi(1)-Se(9)x 2
Bi(1)-Te(2)/Se(2)
Bi(1)-Se(9)

Bi(2)-Se(1) x 2
Bi(2)-Se(9) x 2
Bi(2)-Te(14)/Se(14)

3.491(4)
3.527(4)
3.532(5)
3.603(5)
3.613(4)
3.632(5)

3.099(10)
3.319(13)

3.341(9)
3.457(16)
3.565(12)

0.51(2)

0.518(3)
3.219(10)
3.331(10)
3.390(10)
3.428(13)
3.505(13)

2.925(3)
3.051(3)
2.893(4)
3.016(4)

2.879(3)
3.071(3)
2.955(4)

Bi(2)-Se(1 1)

Bi(3)-Te(2)/Se(2) x 2
Bi(3)-Se(11) x 2
Bi(3)-Se(9)
Bi(3)-Se(12)

Bi(4)-Se(3) x 2
Bi(4)-Se(10) x 2
Bi(4)-Se(6)
Bi(4)-Se(10)

Bi(5)-Se(8) x 2
Bi(5)-Se(10) x 2
Bi(5)-Se(4)
Bi(5)-Se(3)

Bi(6)-Se(4) x 2
Bi(6)-Se(6) x 2
Bi(6)-Se(1)
Bi(6)-Se(10)

Bi(7)-Se(5) x 2
Bi(7)-Se(11) x 2
Bi(7)-36(1)
Bi(7)-Se(5)

Bi(8)-Se(7) x 2
Bi(8)-Se(3) x 2

57

3.241(5)

2.892(3)
3.124(3)
3.206(4)
2.702(4)

2.913(3)
3.013(3)
2.736(4)
3.231(4)

2.817(3)
3.167(3)
2.740(4)
3.389(1)

2.961(3)
2.974(3)
2.953(4)
2.968(4)

2.914(3)
3.013(3)
3.142(4)
2.811(4)

2.773(2)
3.240(3)

Table 3-4. (Cont’d)

Bi(8)-Se(13)
Bi(8)-Se(8)

Pb(1)-Se(13)x 2
Pb(1)-Se(6) x 2
Pb(1)s6(3)
Pb(1)-Rb(2)

2.759(4)
3.275(1)

2.892(3)
3.398(2)
3.012(5)
0.499(1)

Pb(2)-Se(12) x 2
Pb(2)-Se(8)

Pb(3)-Pb(2)

Pb(3)-Se(12) x 2
Pb(3)-Se(1 1)

58

2.867(6)
3.079(18)

0.439(1)
2.923(11)
314(4)

Table 3-5. SCIGCICd Angles (deg) fOI' Rb1_73Pb.,29Bi38e.3_42Te0,59.

Te(2)-Bi(1)-Te(14)
Te(14)-Bi(l)-Te(14)
Te(2)-Bi(1)-Se(9)
Te(14)-Bi(1)-Se(9)
Te(2)-Bi(1)-Se(9)
Te(14)-Bi(l)-Se(9)
Te(2)-Bi(1)-Se(9)
Te(14)-Bi(1)-Se(9)
Se(9)-Bi(l)—Se(9)
Se(9)-Bi(1)-Se(9)

Se(1)-Bi(2)-Se(1)
Se(1)-Bi(2)-Te(14)
Se(1)-Bi(2)—Se(9)
Se(1)-Bi(2)-Se(9)
Te(14)-Bi(2)-Se(9)
Se(9)-Bi(2)-Se(9)
Se(1)-Bi(2)-Se(1 1)
Te(14)-Bi(2)-Se(1 1)
Se(9)-Bi(2)-Se(1 1)

Se(12)-Bi(3)-Te(2)
Te(2)-Bi(3)-Se(2)
Se(12)-Bi(3)-Se(1 1)
Te(2)-Bi(3)-Se(1 1)
Te(2)-Bi(3)-Se(l 1)
Se(12)-Bi(3)-Se(1 1)
Se(l 1)«Bi(3)—Se(1 1)
Se(12)-Bi(3)-Se(9)

9008(9)
92.13(10)

178.57(10)
8893(9)
9078(9)
9027(7)
9078(9)

177.45(8)
9026(9)
87.32(10)

9405(12)
9560(9)
175.08(10)
8958(8)
8733(9)
86.61(10)
9015(9)
171.55(10)
8652(9)

92.02(10)
93.51(12)
93.98(10)

172.65(11)
9054(8)
93.98(10)
84.80(10)

179.68(11)

Te(2)-Bi(3)-Se(9)
Se(l 1)-Bi(3 )-Se(9)

Se(6)-Bi(4)-Se(3)
Se(3)-Bi(4)-Se(3)
Se(6)-Bi(4)-Se(10)
Se(3)-Bi(4)-Se(10)
Se(3)-Bi(4)-Se(10)
Se(10)-Bi(4)-Se(10)
Se(6)-Bi(4)-Se(10)
Se(3)-Bi(4)-Se(10)
Se( 1 0)-Bi(4)-Se( 10)

Se(4)-Bi(5)-Se(8)
Se(8)-Bi(5)-Se(8)
Se(4)-Bi(5)-Se(10)
Se(8)-Bi(5)-Se(10)
Se(8)-Bi(5)-Se(10)
Se(8)—Bi(5)-Se(10)
Se(10)-Bi(5)-Se(10)

Se(1)-Bi(6)-Se(4)
Se(4)-Bi(6)-Se(4)
Se(1)-Bi(6)-Se( 10)
Se(4)-Bi(6)-Se(10)
Se(1)-Bi(6)-Se(6)
Se(4)-Bi(6)-Se(6)
Se(4)-Bi(6)-Se(6)
Se(1)-Bi(6)-Se(6)

59

87.76(9)
8626(10)

9146(10)
92.63(1 1)
91.12(9)
176.76(10)
8927(8)
8871(10)
176.96(10)
9064(9)
8671(9)

91 .78(10)
96.79(1 1)
8898(9)
8991(8)
173.23(7)
173.23(7)
8837(9)

9091(9)
9070(1 1)
179.69(10)
8887(9)
9270(9)
176.39(12)
8943(8)
9270(9)

Table 3-5. (Cont’d)

Se(10)-Bi(6)-Se(6)
Se(6)-Bi(6)-Se(6)

Se(5)-Bi(7)-Se(5)
Se(5)-Bi(7)-Se(5)
Se(5)-Bi(7)-Se(1 1)
Se(5)-Bi(7)-Se(1 1)
Se(5)-Bi(7)-Se(1 1)
s60 1)-Bi(7)-Se(1 1)
Se(5)-Bi(7)-Se(1)
Se(5)-Bi(7)-Se(1)
Se(l 1)-Bi(7)-Se( 1)

Se(13)-Bi(8)-Se(7)
Se(7)-Bi(8)-Se(7)

8752(9)
9020(1 1)

89.82(10)
9259(12)
91.65(10)
177.58(9)
8933(8)
88.71(11)
178.16(11)
8890(9)
89.67(10)

93.5200)
98.86(11)

Se(13)-Bi(8)-Se(3)
Se(7)-Bi(8)-Se(3)
Se(7)-Bi(8)-Se(3)
Se(3)-Bi(8)-Se(3)

Se(13)-Pb(1)-Se(13)
Se(13)-Pb(1)-Se(3)
Rb(3)-Pb(2)-Se(12)
Se(12)-Pb(2)-Se(12)
Rb(3)-Pb(2)-Se(8)
Se(12)-Pb(2)-Se(8)

Se(12)-Pb(3)-Se(12)
Se(12)-Pb(3)-Se(l l)

60

87.21(10)
171.04(7)

9000(8)
81.1 1(9)

93.5004)
89.3503)

129.1(7)
946(3)

128.9(18)
784(4)

922(5)
894(7)

Structure Description of NaxBasszm,Se14

The structure of this compound is very similar to Rb,,Pb5.2,,Bi(,+,.Se14.,Tey structure.
In the previous compound lead replaces the bismuth atoms in the high-coordinate sites. In
NayBasquifixSeM moving from lead to barium the trend remains the same but the
bonding becomes more ionic. Barium too, replaces the high-coordinate bismuth sites but
due to its more ionic nature the resultant structure is different fi'om the previous one. Here
too, only NaCl- and BizTe3-type fragments exist and the former fi'agment is three bismuth
octahedra wide while the latter is five bismuth octahedra wide which is a point of
su'uctural difference with the B-KzBlgSCl 3 structure. The NaCl-type fragments connect the
layers formed by BizTeg-type fragments to generate a three dimensional fi'amework with
tunnels which are filled by the alkaline earth (Ba2+) cations.

Among the alkaline earth (Ba2+) cations, Ba(l) and Ba(2) occupy the bismuth
high-coordinate sites while Ba(3) occupies the tunnels (see figure 3-2). All these three
sites are fully occupied. Ba(1,2) is present in a bicapped trigonal prism like coordination
with eight Se atoms in the range between 3.293(3) —— 3.464(4)A for Ba(l) and between
3.295(3) — 3.443(5)A for Ba(2). The coordination environment of Ba(3) is a little
different and can be described as a distorted tricapped trigonal prism. The prism is
defined by Se(8), Se(10), Se(l 1) and their symmetry-equivalent atoms, while the capping
atoms are Se(2), Se(5) and Se(8). The alkali (Na+) cations have mixed occupancy over
three sites with Bi(6, 7, 8). The Bi(6) site contains 68% of Bi and 32% of Na, the Bi(7)
site contains 54% of Bi and 46% of Na and the Bi(8) site contains 70% of Bi and 30% of
Na. The Bi(7) mixed site is present in the NaCl fragment whereas the other two mixed

sites are present in the B12TC3 fragment. This disorder can be attributed to very similar

61

ionic sizes of Na+ and Bi3+ in octahedral coordination (n.1,,+ = 1.16A, r1313+ = 1.17A).20
Bi(1-5) are present in a highly distorted octahedral coordination with a short bond trans to
a long bond. The other interesting feature of this structure is the disordered selenium site
containing three selenium atoms, Se(15), Se(16) and Se(17) which also makes up the
coordination sphere for the mixed site of Bi(7)/Na(7) and Bi(8)/Na(8). For bond lengths

and selected angles see Table 3-6. & 3-7.

Thermal Analysis of NaxBaM,Bi6+,Se14

Differential thermal analysis was performed on pure NaxBa5-2xBi6+xSe14 to
ascertain its thermal behavior. At the end of two heating cycles the compound was
checked for decomposition by taking its powder X-ray diffraction pattern. NaxBa5-
2xBi6+xSe14 show an endothermic (melting) peak at 819°C and on cooling shows an
exothermic (recrystallization) peak at 788°C (see Figure 3-3.). The powder pattern of the

compound after DTA indicated no decomposition.

Charge Transport Measurement of NaxBayszififie”
Thermoelectric power measurements were carried on polycrystalline oriented ingots
(grown by Bridgman technique) 2' of NaxBa5-2xBi6+xSe14. It is a n-type conductor and at
room temperature the thennopower has a value of -24.22 uV/K. It shows a linear trend
till 400 K. (See Figure 34).

Electrical conductivity measurements were carried on polycrystalline oriented

ingots along the needle axis and at room temperature value of 183.61 S/cm was obtained.

62

Figure 3-2. Projection of the structure of NalBa2,7gBi7_37Sel4 down the b-axis.

 

63

Table 3.6. Bond distances (A) for NalBa2,79Bi7_37Se14.

Bi(1)-Se(10)
Bi(1)-Se(8) x 2
Bi(1)-Se(3) x 2
Bi(1)-Se(2)

Bi(2)-Se(l 1)
Bi(2)-Se(5) x 2
Bi(2)-Se(4) x 2
Bi(2)-86(1)

Bi(3)-Se(9)
Bi(3)-Se(2) x 2
Bi(3)-Se(14) x 2
Bi(3)-Se(3)

Bi(4)-Se(13)
Bi(4)-Se(3) x 2
Bi(4)-Se(14) x 2
Bi(4)-Se(14)

Bi(5)-Se(6)
Bi(5)-Se(4) x 2
Bi(5)-Se(1) x 2
Bi(5)-Se(4)

Bi(6)/Na(6)-Se(7) x 2
Bi(6)/Na(6)-Se(1) x 2
Bi(6)/Na(6)-Se(5)
Bi(6)/Na(6)-Se(12)

2.722(4)
2.851(3)
3.167(3)
3.208(4)

2.701(4)
2.851(2)
3.147(3)
3.337(1)

2.733(4)
2.836(3)
3.193(3)
3.313(1)

2.740(4)
2.974(3)
3.020(3)
3.215(4)

2.704(4)
2.987(3)
3.008(3)
3.453(1)

2.908(3)
3.070(3)
2.950(5)
2.984(5)

Bi(7)/Na(7)-Se(16) x 2
Bi(7)/Na(7)-Se(13) x 2
Bi(7)/Na(7)-Se(9) x 2
Bi(7)/Na(7)-Se(15)
Bi(7)/Na(7)-Se(14)
Bi(7)/Na(7)-Se(17)

Bi(8)/Na(8)-Se(16) x 2
Bi(8)/Na(8)-Se(15)
Bi(8)/Na(8)-Se(1 7)
Bi(8)/Na(8)-Se(6) x 2
Bi(8)/Na(8)-Se(12) x 2
Bi(8)/Na(8)-Se(l)

Bi(9)-Se(17) x 2
Bi(9)-Se(16) x 2
Bi(9)-Se(15) x 2
Bi(9)-Se(7)
Bi(9)-Se(12) x 2
Bi(9)-Se(12)

Ba(1)-Se(10) x 2
Ba(1)-Se(13) x 2
Ba(1)-Se(7) x 2
Ba(1)-Se(3)
Ba(1)-Se(5)

Ba(2)-Se(1 1) x 2
Ba(2)-Se(9) x 2

64

292(3)
3.019(3)
3.025(3)
2.992(12)
3.009(5)
305(4)

277(3)
292(2)
3.429(1 1)
3.022(3)
3.036(3)
3.049(5)

269(3)
276(3)
2.880(14)
2.887(5)
3.135(3)
3.159(5)

3.293(3)
3.334(3)
3.395(4)
3.427(4)
3.464(4)

3.295(3)
3.340(3)

Table 3-6. (cont’d)

Ba(2)-Se(6) x 2
Ba(2)-Se(2)
Ba(2)-Se(4)

Ba(3)-Se(10) x 2

3.359(3)
3.395(4)
3.443(5)

3.310(3)

Ba(3)-Se(11) x 2
Ba(3)-Se(8)
Ba(3)-Se(8) x 2
Ba(3)-Se(2)
Ba(3)-Se(5)

65

3.345(3)
3.488(4)
3.497(4)
3.593(4)
3.594(5)

Table 3-7. Selected Angles (deg) for NalBa2,79Bi7,37Se14.

Se(10)-Bi(l)-Se(8)
Se(8)-Bi(1)-Se(8)
Se(10)-Bi(1)-Se(3)
Se(8)-Bi(1)-Se(3)
Se(8)-Bi(1)-Se(3)
Se(3)-Bi(l)-Se(3)
Se(10)-Bi(1)-Se(2)
Se(8)-Bi(1)-Se(2)
Se(3)-Bi(1)-Se(2)
Se(10)-Bi(1)-Ba(3)
Se(8)-Bi(1)-Ba(3)
Se(3)-Bi(1)-Ba(3)
Se(2)-Bi(1)-Ba(3)

Se(11)-Bi(2)-Se(5)
Se(5)-Bi(2)-Se(5)
Se(l 1)-Bi(2)-Se(4)
Se(5)-Bi(2)-Se(4)
Se(5)-Bi(2)-Se(4)
Se(4)-Bi(2)-Se(4)

Se(9)-Bi(3)-Se(2)
Se(2)-Bi(3)-Se(2)
Se(9)-Bi(3)-Se(14)
Se(2)-Bi(3)-Se(14)
Se(2)-Bi(3)-Se(14)
Se(14)-Bi(3)-Se(14)

Se(13)~Bi(4)-Se(3)
Se(3)-Bi(4)-Se(3)

9284(9)
9839(12)
9345(9)

171.16(9)
8750(7)
85.9300)

178.09(1 1)
8592(9)
8794(9)

122.58(9)
5485(7)

125.60(7)
5551(7)

9224(10)
9839(1 1)
95.64(10)

170.290 1)
8699(7)
86.60(10)

92.2000)
99.1002)
8925(9)

172.78(9)
8790(7)
85.05(10)

9104(10)
93.06(11)

Se(13)-Bi(4)-Se(14)
Se(3)-Bi(4)-Se(14)
Se(3)-Bi(4)-Se(14)
Se(14)-Bi(4)-Se(14)
Se(13)-Bi(4)-Se(14)
Se(3)-Bi(4)-Se(14)
Se(14)-Bi(4)-Se(14)

Se(6)-Bi(5)-Se(4)
Se(4)-Bi(5)-Se(4)
Se(6)-Bi(5)-Se(1)
Se(4)-Bi(S)-Se(1)
Se(4)-Bi(5)-Se(1)
Se(1)-Bi(5)-Se(1)

Se(7)-Bi(6)-Se(7)
Se(7)-Bi(6)-Se(5)
Se(7)-Bi(6)-Se(12)
Se(5)-Bi(6)-Se(12)
Se(7)-Bi(6)-Se(1)
Se(7)-Bi(6)-Se( 1)
Se(5)-Bi(6)-Se(1)
Se(12)-Bi(6)-Se(1)
Se(1)-Bi(6)-Se(1)

Se(16)-Bi(7)-Se(16)
Se(16)-Bi(7)-Se(15)
Se(16)-Bi(7)-Se(14)
Se(l 5)-Bi(7)-Se( 14)
Se(16)-Bi(7)-Se(13)

66

9249(10)

176.3702)
87.74(7)
9124(1 1)

175.7902)
9186(9)
8457(9)

9095(0)
9252(11)
9122(10)

177.7903)
8784(7)
91.7101)

9582(13)
85.20(12)
90.1402)
173.0303)
176.3900)
8740(8)
9345(10)
9151(11)
89.34(11)

22(2)

13.100)
168.1(10)
177.5(5)
103.6(10)

Table 3-7. (cont’d)

Se(16)-Bi(7)-Se(13)
Se(15)-Bi(7)-Se(13)
Se(14)-Bi(7)-Se(l3)
Se(16)-Bi(7)-Se(13)
Se(13)-Bi(7)-Se(13)
Se(16)-Bi(7)-Se(9)
Se(15)-Bi(7)-Se(9)
Se(14)-Bi(7)-Se(9)
Se(13)-Bi(7)-Se(9)
Se(13)-Bi(7)-Se(9)
Se(16)-Bi(7)—Se(9)
Se(9)-Bi(7)-Se(9)
Se(16)-Bi(7)-Se(17)
Se(15)-Bi(7)-Se(17)
Se(14)-Bi(7)-Se(17)
Se(13)-Bi(7)-Se(17)
Se(9)-Bi(7)-Se(l7)

Se(16)-Bi(8)-Se(16)
Se(16)-Bi(8)-Se(15)
Se(16)-Bi(8)-Se(6)
Se(16)-Bi(8)-Se(6)
Se(15)-Bi(8)-Se(6)
Se(6)-Bi(8)-Se(6)
Se(16)-Bi(8)-Se(12)
Se(16)-Bi(8)-Se(12)
Se(6)<Bi(8)-Se(12)
Se(6)-Bi(8)-Se(12)
Se(12)-Bi(8)-Se(12)
Se(16)-Bi(8)-Se(1)

87.7(7)
908(4)
87.42(11)
103.6(10)
91.28(13)
972(7)
942(4)
87.59(10)
175.0004)
8863(8)
81.4(10)
91.0302)
20.9(18)
10.9(14)
166.6(18)
83.2(12)
101.7(12)

23(2)
13.3(10)
100.0(7)
83.300)
96.1(3)
91.1602)
101.100)
84.5(7)
175.5005)
8894(8)
90.60(l3)
167.1(11)

Se(15)-Bi(8)-Se(1)
Se(6)-Bi(8)-Se(1)
Se(12)-Bi(8)-Se(1)

Se(17)-Bi(9)-Se(l 7)
Se(17)-Bi(9)-Se(16)
Se(17)-Bi(9)-Se(16)
Se(16)-Bi(9)-Se(16)
Se(17)-Bi(9)-Se(15)
Se(17)-Bi(9)-Se(15)
Se(16)-Bi(9)-Se(15)
Se(16)-Bi(9)-Se(15)
Se(15)-Bi(9)-Se(15)
Se(17)-Bi(9)-Se(7)

Se(16)-Bi(9)-Se(7)

Se(15)-Bi(9)-Se(7)

Se(17)-Bi(9)-Se(12)
Se(17)-Bi(9)-Se(12)
Se(16)-Bi(9)-Se(12)
Se(16)-Bi(9)-Se(12)
Se(15)-Bi(9)-Se(12)
Se(7)-Bi(9)-Se(12)

Se(15)-Bi(9)-Se(12)
Se(12)-Bi(9)-Se(12)
Se(17)-Bi(9)-Se(12)
Se(16)-Bi(9)-Se(12)
Se(15)-Bi(9)-Se(12)
Se(7)-Bi(9)-Se( 1 2)

Se(12)-Bi(9)-Se(12)

67

179.0(4)
84.62(1 1)
90.9101)

106.9(17)
23(2)
90.6(16)
71(2)

102.9(12)
1 1.2(16)
84.0(13)
136(9)
97.1(6)
88.8(19)

104.9(7)
99.2(5)
829(9)

169.4(13)
99.9(10)

165.8(9)

171.1(3)
87.61(10)
87.5(3)
87.02(11)
96.6(18)
824(6)
868(4)

170.9003)
85.80(10)

Figure 3-3. DTA diagram of NaxBas-2xBi6+xSe.4 showing the endothermic and

exothermic peaks. The heating and cooling rates were 10°C/min.

20-

‘\_ ‘ _ 788°C

 

 

 

-40

DTA (11V)

-60-

 

0 200 400 600 800 1000
Temperature (°C)

68

Figure 34. Variable temperature thennopower for a polycrystalline oriented ingot of

NaxBaS-ZxBi6+xsel4-

Thermopower (uVIK)

-22

-24

280

300 320 340 360 380 400
Temperature (K)

69

420

E. Conclusion

Two new quaternary bismuth chalcogenides that are derivatives of the
K2_5Big_5Se14 structure type have been prepared. In Rb]+,.Pb3.2,,Bi-,+,,Se14.yTey structure the
bigger Rb+ cations occupy the tunnels and are disordered with Bi atoms similar to the
parent structure. Pb atoms occupy the high-coordination sites. When we move to smaller
cations (Na) in NaxBa5-2xBi6+xSe14, they get disordered with Bi atoms and reside in the
NaCl- and BizTeg-type fiagments rather than the tunnels. The tunnels and the high-

coordination sites are occupied by the alkaline earth (Ba2+) cations.

70

References

l.

10.

11.

(a) Makovicky, E. Eur. J. Mineral. 1993, 5, 545-591. (b) Makovicky, E. Fortschr.
Miner. 1981, 59,137-190. (c) Makovicky, E. Neues Jahrbuch Miner. Abh. 1989,
160, 269-297.

McCarthy, T. J.; Ngeyi, S. -P.; Liao, J. -H; DeGroot, D.; Hogan, T.; Kannewurf,
C. R.; Kanatzidis, M. G. Chem. Mater. 1993, 5, 331-340.

McCarthy, T. J.; Tanzer, T. A.; Kanatzidis, M. G. J. Am. Chem. Soc. 1995, 117,
1294-1301.

(a) Kanatzidis, M. G.; McCarthy, T. J.; Tanzer, T. A.; Chen, L.; Iordanidis, L.;
Hogan, T.; Kannewurf, C. R.; Uher, C.; Chen, B. Chem. Mater. 1996, 8, 1465-
1474. (b) Chen, B.; Uher, C.; Iordanidis, L.; Kanatzidis, M. G. Chem. Mater.
1997, 9, 1655-1658.

Iordanidis, L.; Kanatzidis, M. G. Angew. Chem. Int. Ed. Engl. 2000, 39, 1927-
1930.

Chung, D-. Y.; Jobic, S.; Hogan, T.; Karmewurf, C. R.; Brec, R.; Rouxel, R.;
Kanatzidis, M. G. J. Am. Chem. Soc. 1997, 119, 2505-2515.

Chung, D-. Y.; Hogan, T.; Brazis, P. W.; Kannewurf, C. R.; Bastea, M.; Uher, C.;
Kanatzidis, M. G. Science, 2000, 287, 1024-1027.

Wang, Y. C.; DiSalvo, F. J. Chem. Mater. 2000, 12, 1011-1017.

Iordanidis, L.; Schindler, J. L.; Kannewurf, C. R.; Kanatzidis, M. G. J. Solid State
Chem. 1999, 143(2), 151-162.

Choi, K. -S.; Iordanidis, L.; Chondroudis, K.; Kanatzidis, M. G. Inorg. Chem.
1997, 36, 3804-3805.

Chung, D-. Y.; Iordanidis, L.; Rangan, K. K.; Brazis, P. W.; Kannewurf, C. R.;
Kanatzidis, M. G. Chem. Mater. 1999, 11, 1352-1362.

71

12.

13.

14.

15.

16.

17.

18.

19.

20.

21.

Mrotzek, A.; Chung, D-. Y.; Hogan, T.; Kanatzidis, M. G. J. Mater. Chem. 2000,
10(7), 1667-1672.

Iordanidis, L.; Brazis, P. W.; Kyratsi, T.; Ireland, J .; Lane, M.; Kannewurf, C. R.;
Chen, W.; Dyck, J. S.; Uher, C.; Ghelani, N. A.; Hogan, T.; Kanatzidis, M. G.
Chem. Mater. 2001, 13, 622-633.

Chung, D-. Y.; Choi, K. -S.; Iordanidis, L.; Schindler, J. L.; Brazis, P. W.;
Kannewurf, C. R.; Chen, 8.; Hu, 8.; Uher, C.; Kanatzidis, M. G. Chem. Mater.
1997, 9, 3060-3071.

Choi, K. -S.; Chung, D-. Y.; Mrotzek, A.; Brazis, P. W.; Kannewurf, C. R.; Uher,
C.; Chen, W.; Hogan, T.; Kanatzidis, M. G. Chem. Mater. 2001, 13, 756-764.

see Chapter 2.
CERIUSZ, Version 3.8., Molecular Simulations Inc., Cambridge, England, 1999.

SAM v6.45, 1997-2003, SHELXTL v5.1, 1998, Bruker Analytical Xray
Systems Inc., Madison, WI 53719, USA.

Cordier, G.; Schafer, H.; Schwidetzky, C. Rev. Chim. Miner. 1985, 22, 676-683.

Cotton, F. A.; Wilkinson, G.; Murillo, C. A.; Bochmann, M. Advanced Inorganic
Chemistry, John Wiley & Sons, Inc., 6‘h ed.; 1999, 1302-1303.

Kyratsi, T.; Chung, D. -Y.; Choi, K. —S.; Dyck, J. S.; Chen, W.; Uher, C.;
Kanatzidis, M. G. Mat. Res. Soc. Symp. Proc. 2000, 626, Z8.8.1.

72

CHAPTER 4

Solvothermal Synthesis of Ordered Structure of Cs3Sb5Se9

A. Introduction

Solid state reactions involve solid reactants and are characterized by slow
nucleation and diffusion processes. High temperatures are usually required so that the
reactants have enough mobility for sufficient diffusion to take place. This high-
temperature diffusion control leads to restrictions in the number and complexity of the
structural building blocks available for the construction of solid-state fi'ameworks. Thus
one has very little control in the rational design and prediction of the structures coming
out of this traditional solid-state reactions.1 Such experimental conditions lead almost
invariably to thermodynamically stable phases which have simple lattice structures of
high symmetry and high density.1 Usually these reactions occur at temperatures typically
above 600°C which allows adequate diffusion of ions and atoms to the site of product
formation.

In comparison to the results obtained fiom such high temperature synthetic
methods, alternative methods like chemical vapor deposition (CVD), molten salt flux
synthesis and hydrothermal synthesis have allowed the solid-state chemist to use lower
temperature regime where kinetically stable or metastable phases can be accessible.
These lower temperatures make possible the use of molecular assemblies as building

blocks, for incorporation in solid state structures.

73

Hydrothermal synthesis usually refers to heterogeneous reactions involving water
as a solvent at elevated temperatures and pressures in a closed system, often in the
vicinity o f i ts c ritical p oint.2 There are c ertain fundamental differences in the reaction
conditions involved in comparison to traditional solid-state reactions.l First, using a
suitable solvent removes diffusion control and allows the starting materials to mix
properly. Second, the reactions are restricted to one or more functional groups by the
employment of relatively low temperatures. This leaves the majority of the chemical
bonds intact.

‘Solvothermal’ is a more general term and it refers to similar reaction but in
which a different solvent, can be either inorganic or organic, is used. Certain properties of
the solvent under these conditions (hydro- or solvothermal), like viscosity, density and
diffusion coefficient changes appreciably and the solvent behaves much differently as
compared to what is expected at ambient conditions.3 As a result of this, the chemical
reactivity and the solubility of the reactants are greatly enhanced and this enables the
reaction to take place at a much lower temperature. This methodology is being applied
for the growth of various inorganic materials like metal carbonates, phosphates, oxides,
halides, quartz and zeolites.2‘ 4

A growing interest in solvotherrnal methods has been motivated by the fact that
these lead to materials containing regularly spaced pores and cavities, which have a
distinct technological potential.5 For example, these mild and soft conditions make it
possible to leave polychalcogen building-blocks intact while they reorganize themselves
to form various new structures, many of which might be promising for applications in

catalysis, electronic, magnetic, optical and thermalelectronic devices.6 Water and alcohol

74

so far have been solvents of choice and a number of alkali metal, alkaline-calth metal,
group 14-15 sulfides and selenides and other metal based chalcogenides have been
isolated both by our group7 and other groups.8 These reactions were canied out in the
temperature range 0 f l 10-220°C. Only recently ethylenediamine9 and ammonia10 h ave
been used as reaction medium to crystallize polychalcogenides at lower temperature
range of 160-170°C.

The structure of Cs3SbSSe9 which was reported by Sheldrick and Hiiuslerll shows
disorder in the Sb and chalcogen sites and this disorder extends to all the layers in the
structure. The structure of Cs3Sb5Se9 presented here has a more ordered structure in the

sense that the disorder in the metal and chalcogen site is extended only in alternate layers.

B. Experimental Section

Reagents: Chemicals were used as obtained: (i) antimony shots, 99.999% purity,
Cerac, Milwaukee, WI. (ii) selenium shots, 99.999% purity, Cerac, Milwaukee, WI. (iii)
cesium metal, 99.999% purity, Alfa Aesar, Ward Hill, MA. (iv) ethylenediamine,
Spectrum Chemical Mfg. Corp., Gardena, CA. Cs2Se was prepared by a stoichiometric
reaction of cesium metal and selenium shots in liquid ammonia.

Solvent: Ethylenediamine (HZNCHZCHzNHZ) is a very good solvent for
solvothermal synthesis of metal chalcogenides. Some of the physical constants of the
solvent are shown in Table 4-1.12 It has a relatively low critical pressure which makes it
possible to run these reactions in thick-walled pyrex tubes under mild temperature

conditions.

75

Synthesis: All manipulations were carried out under a dry nitrogen atmosphere in
a Vacuum Atmospheres Dri-Lab glovebox. All starting materials were ground to fine
powder and then loaded in thick walled pyrex tubes for efficient mixing with the solvent.

Cs3Sb58e9: A mixture of 0.09g (0.261 mol) of C52Se, 0.159g (1.31 mol) of
antimony and 0.206g (2.61 mol) of selenium in the ratio of 0.2:1:2 was transferred into a
9mm thick walled pyrex tube. 0.30ml (mol) of ethylene diamine was added to this and
the tube was cooled under liquid N2 until the solvent solidifies. This was then flame
sealed under vacuum (~10’4 Torr). The tube was then wrapped in aluminum foil and kept
in an oven maintained at a constant temperature of 154°C. The progress of the reaction
was monitored by checking for crystal grth inside the tube. The product consisted of
reddish brown hexagonal rods (see Figure 4-1.) and orange crystals. The rods were stable
in air whereas the orange crystals were sensitive to air as it lost its color when left outside.
These orange crystals were CS3SbSe4.l3 Energy Dispersive Spectroscopy (EDS) on
several of these hexagonal rod type crystals gave an approximate composition of

“CSSbl 53862.94”.

C. Physical Measurements

Energy Dispersive Spectroscopy: Quantitative microprobe analyses of the
compound were performed with a JEOL JSM-6400V Scanning Electron Microscope
equipped with a Tracor Northern Energy Dispersive Spectroscopy (EDS) detector. Data
were acquired u sing an accelerating v oltage o f 20 kV and a 3 0 se conds accumulation

time.

76

Single-Crystal X-ray Crystallography: Intensity data were collected at 293 K
on a Bruker SMART Platform CCD diffractometer using graphite monochromatized Mo
K, (A. = 0.71073A) radiation. Individual fiames were measured using 0.3° steps in 0)
using the SMART software. SAINTl4 was used for data extraction and reduction. The
absorption correction was done with SADABS”, and the structure solution was done
with the SHELXTLl4 package of crystallographic programs.

A hemisphere of data was collected with an exposure time of 30 seconds per
flame. The crystallographic data is shown in Table 4-2. The structure was first solved in
C2 space group. Then the TEXSAN15 package of crystallographic program was used to
find missing symmetry elements and an inversion center was found at (0.0001, 0.2845, -
0.0013) suggesting a higher centrosymmetric space group C2/m. The origin was shifted
to the inversion point and the coordinates of all the atoms were recalculated based on this
origin. 1/8th of this cell was chosen and refined in C2/m. Forty six crystallographically
independent positions were found out of which thirteen positions were found to sit on a
crystallographic mirror plane. The remaining sat on a general position. Sb(13) & Sb(14),
Se(18) & Se(l9), Se(20) & Se(21), Se(22) & Se(23) and Se(24) & Se(25) were all found
to be disordered over a single site. After anisotropic refinement final R values, R1 =
8.18% and wR2 = 22.68%. The fractional coordinates and isotropic displacement

parameters along with occupancies for disordered atoms are shown in Table 4-3.

77

Table 4-1. Physical constants for ethylene diamine.

Molecular formula CzHgNz
Formula weight (g.mol-') 60.10
Melting point (°C) 8.5
Boiling point (°C) 1 17.3
Flash point (°C) 43
Critical temp. (°C) 319.9
Critical pressure (atm) 62.1
Critical volume (cm3.mol'1) 206

Figure 4-1. SEM image of the hexagonal rod type crystal of CS3Sb5869.

 

 

78

Table 4-2. Crystallographic data for the ordered Cs3Sb5Se9 and the structure reported by

Sheldrick and Hitusler.ll

Empirical formula
Formula weight
T, K

1». A

Crystal System
Space group

a, A

b, A

c, A

0., deg

13. deg

1. deg

v, A3

Z

Pcalcd. g/ 01113

11. nun"

Total reflections
Unique reflections
RON)

No. of parameters
Goodness-of-fit on F2
Refinement method
Rl‘

wR2b

Cs3Sb5Se9
412.58
293(2)
0.71073

C2/m
19.156(4)
51.647(12)
1 1.615(3)
90
126.974(4)
90

9180(4)

70
5.224
25.789

38167
1 1209
0.0708
371
1.064

0.0818
0.2268

CS3Sb5Se9 (From ref. 11)

0.71073

Monoclinic

C2/m
9.587(4)
25.855(4)
9.638(1)
90
105.58(2)
90
2301(1)

4

4.96
24.57

1862
1582

99

F ull-matrix least-squares on F 2

0.064
0.061

“ R1 = z IlFol-chII/ZlFol. b wR2 = {z 1w(F.2-F.’)’1/Z[w(F.2/1}”2.

Table 4-3. Atomic coordinates (x 104) and equivalent isotropic displacement parameters

(A2x 103) for CS3Sb5Seg.

 

 

x y z U(eq) Occ.
CS(l) 2638(1) 1080(1) 7563(2) 20(1)
CS(2) 2353(1) 1076(1) 2328(2) 18(1)
CS(3) 0 408(1) 5000 24(1)
CS(4) 5000 41 1(1) 5000 25(1)
CS(S) 10102(1) 1425(1) 7574(2) 22(1)
CS(6) 7486(1) 2091(1) 4999(2) 33(1)
CS(7) 5155(1) 1419(1) 7618(2) 22(1)
Sb(l) 7493(1) 1886(1) 8394(2) 22(1)
Sb(2) 0 -2886(1) 5000 33(1)
Sb(3) 2417(1) 380(1) 4743(1) 8(1)
Sb(4) 2589(1) 380(1) -86(1) 7(1)
Sb(S) 1 168(1) 0 637(2) 7(1)
Sb(6) 3833(1) 0 8297(2) 8(1)
Sb(7) 4893(1) 615(1) 8283(2) 9(1)
Sb(8) -96(1) 611(1) 1510(2) 9(1)
Sb(9) 7501(1) 1888(1) 11612(2) 23(1)
Sb(10) 0 -2880(1) 0 36(1)
Sb(l l) 5000 -2879(1) 15000 33(1)
Sb(12) 5000 -2878(1) 10000 36(1)
Sb(13) 6334(3) -2497(1) 18311(4) 27(1) 0.51744
Sb(14) 6333(3) -2499(1) 1 93 50(4) 22(1) 0.48256
Se(l) 3801(2) O 1134(3) 11(1)
Se(2) 1217(2) O 3569(3) 11(1)
Se(3) 2290(1) 376(1) 1877(2) 8(1)
Se(4) 1 165(2) 0 -1620(3) 8(1)
Se(5) 3832(2) 0 6024(3) 8( 1)
86(6) 7518(2) 1533(1) 10030(2) 18(1)
Se(7) 1226(2) 773(1) 4001(2) 14(1)

80

Table 4-3. (cont’d)

 

 

x Y z U(eq) Occ.
Se(8) 3766(2) 771(1) 1546(3) 16(1)
Se(9) 0 965(1) 0 13(1)
8600) 1233(2) 823(1) -1620(3) 14(1)
Se(] 1) 3775(2) 836(1) 5939(2) 13(1)
Se(12) 8735(2) 1707(1) 8442(3) 26(1)
Se(13) 5000 967(1) 10000 15(1)
Se(14) 8717(2) 1700(1) 14034(3) 30(1)
Se(15) 6257(2) 1706(1) 11559(3) 26(1)
Se(16) 6276(2) 1692(1) 5991(3) 29(1)
Se(17) 2709(1) 377(1) 7297(2) 9(1)
Se(18) -191(4) -2881(1) 2719(6) 21(2) 0.48593
Se(l 9) -180(4) -2878(1) 1904(6) 25(2) 0.51407
Se(20) 4809(4) -2872(1) 12712(6) 22(2) 0.48630
Se(21) 4819(4) -2874(1) 1 1909(6) 25(2) 0.51370
Se(22) 6315(8) -2503(1) 161 10(50) 24(5) 0.66742
Se(23) 6279(1 1) -2489(5) 16510(50) 10(6) 0.33258
Se(24) 6334(9) -2497(4) 1 1620(50) 16(4) 0.43799
Se(25) 6313(7) -2500(2) 1 1 150(60) 20(6) 0.56201

 

U(eq) is defined as one third of the trace of the orthogonalized UiJ tensor.

81

D. Results and discussion

Structure Description of Cs3SbSSe9:

The structure of Cs3Sb58e9 consists of complex selenoantimonate layers and
builds up in the following manner: it has three kinds of building blocks which are
(8658,)“; (SbSe4)5‘ and (SbZSe5)4' (see Figure 43.). Each (SbZSe6)6' unit is bridged by
(SbSe4)5’ anion to another (Sb28e6)° unit to form chains which run along the c-direction.
The (SbSe4)5' bridging unit are positioned in an alternate fashion along this chain. These
linear chains are connected along the a-direction by two (Sb2Se5)4' anions to form layers
parallel to the ac-plane. Alternate layers in this structure h ave disordered S b- and S e-
sites.

The antimony atoms in the (Sb2Se6)6' unit are in a distorted octahedral
coordination with a long Sb-Se bond trans to a short Sb-Se bond. Sb-Se distances in this
unit ranges between 2.435(6)-3.189(1)A. In the (SbSe4)5' unit the antimony atoms are in
see-saw type coordination. Sb-Se distances in this unit ranges between 2.596(2)-
3.332(1)A. The (Sb28e5)4' unit is formed by the comer sharing of two trigonal pyramidal
SbSe3 units. Sb-Se distances in this unit ranges between 2.508 (3)-2.617(3)A. For bond
distances and selected bond angles see Table 4-3. and Table 4-4. respectively.

For the alkali (Cs+) atoms, Cs(3), CS(4) & CS(6) lies in the tunnels running along
the b-direction (see Figure 4-4.) which are within the layers and all the remaining alkali
atoms lie between the layers.

An interesting feature in this structure is the presence of disorder in the Sb- and
Se-sites. Specifically Sb is disordered in the (SbSe4)5' unit while Se is disordered in both

(Sb2Se6)6‘ and (SbSe4)5' u nits (see Figure 4 -3.). The S b-site in (SbSe4)5' unit h as 5 2%

82

Sb(13) and 48% Sb(14). Both the atoms are disordered at 1.207(1)A. In the Se-sites,

Se(18) (49% )is disordered with Se(19) (51%) and Se(20) (49%) is disordered with Se(21)
(51%). Se(18) is disordered with Se(19) at 0.959(1)A and Se(20) is disordered with Se(21)
at 0.945(1)A. In case of the (Sb2866)6' unit the disordered Se-sites are occupied by

Se(22)/Se(23) and Se(24)/Se(25). The Se(22) site contains 67% Se(22) and 33% Se(23)

whereas the Se(24) site has 44% Se(24) and 56% Se(25). Se(22) is disordered with Se(23)
at 0.512(1)A and Se(24) is disordered with Se(25) at 0.524(1)A.

Sheldrick and Hauslerll in their report on the structure of Cs3Sb5$e9 have noted
disorder in the Sb- and Se-site and this disorder is present in all the layers. They also
reported the disorder of Se-site to be present only in the (SbSe4)5' unit. In our structural
solution we observe the disorder in Sb- and Se-sites to be present in alternate layers and
this is probably a distinct structural difference with that reported earlier. Also the disorder
in the Se-sites is observed to be present in (Sb28e6)6' unit as well as in (SbSe4)5' unit.
Moving from disordered layers as reported earlier to ordered layers, probably explains

the doubling from 25.855(4)A to 51 .647(12)A in the b-parameter of the unit cell.

83

Figure 4-2. Projection of the structure of CS3Sb5Se9 down the c-axis.

 

 

 

 

 

84

 

.Cs
.Sb
OSe

Figure 4-3. Different selenoantimonate units which act as building-blocks.

 

88b
Se

 

‘ a) Linear chains composed

9.053%?” ..
- £117.)?

 

b) Similar chains showing
disorder in the Sb- and Se-
sites

 

(c) (Sb2Se5)4' unit, this
joins the two chains to
form a layer.

   

85

Figure 44. Projection of one of the layers in Cs3SbSSe9 down the b-axis showing the
tunnels occupied by the alkali atoms. It also shows the chains connected by the (Sb2Se5)4'

unit.

‘9§/"§‘ ‘%%,§
1 U as’

C
\_.. 3::

86

Table 4-4. Bond distances (A) for Cs3Sb5Se9.

Sb(1)-Se(12)
Sb(1)-Se(16)
Sb(1)-Se(6)

Sb(2)-Se(18) x 2
Sb(2)-Se(23)
Sb(2)-Se(22)
Sb(2)-Se(16) x 2

Sb(3)-Se(17)
Sb(3)-Se(2)
Sb(3)-Se(7)
Sb(3)-Se(5)
Sb(3)-Se(3)
Sb(3)-Se(] 1)

Sb(4)-Se(3)
Sb(4)-Se( 1 )
Sb(4)-Se(8)
Sb(4)-Se(4)
Sb(4)-Se(] 7)
Sb(4)-Se( 1 0)

Sb(5)-Se(3) x 2
Sb(5)-Se(4)

Sb(5)—Se(2)

Sb(6)-Se(l7) x 2
Sb(6)-Se(5)

2.521(3)
2.531(3)
2.614(3)

2.447(6)

2.765(19)
2.849(14)

2.948(4)

2.668(2)
2.687(3)
2.775(3)
2.926(3)
3.189(1)
3.149(4)

2.665(2)
2.700(3)
2.760(3)
2.936(3)
3.181(1)
3.097(5)

2.596(2)
2.617(3)
3.350(1)

2.601(2)
2.640(3)

87

Sb(6)-Se(1)

Sb(7)-Se(1 1)
Sb(7)-Se(8)
Sb(7)-Se(13)

Sb(8)-Se(10)
Sb(8)-Se(7)
Sb(8)-Se(9)

Sb(9)-Se(15)
Sb(9)-Se(14)
Sb(9)-Se(6)

Sb(10)-Se(19) x 2
Sb(10)-Se(25)
Sb(10)-Se(24)
Sb(10)-Se(15) x 2

Sb(11)-Se(20) x 2
Sb(l 1)-Se(22)
Sb(l 1)-Se(23)
Sb(11)-Se(14) x 2

Sb(12)-Se(21) x 2
Sb(12)-Se(25)
Sb(12)-Se(24)
Sb(12)-Se(12) x 2

3.332(1)

2.508(3)
2.583(3)
2.615(3)

2.509(3)
2.584(3)
2.617(3)

2.529(3)
2.530(3)
2.610(3)

2.435(6)
2.812(10)
2.843(12)
2.901(3)

2.455(6)
2.807(12)
282(2)

2.952(4)

2.441(6)
2.809(12)
286(2)

2.909(4)

Table 4-4. (cont’d)

Sb(13)-Sb(14)
Sb(13)-Se(23)
Sb(13)-Se(22)
Sb(13)-Se(20)
Sb(13)-Se(18)
Sb(13)-Se(19)
Sb(13)-Se(21)

Sb(14)-Se(25)
Sb(14)-Se(21)
Sb(14)-Se(19)
Sb(14)-Se(24)
Sb(14)-Se(20)
Sb(14)-Se(18)

Cs(1)-Se(10)
Cs(1)-Se(1 5)
Cs(1)-Se(17)
Cs(1)-Se(l 3)
Cs(1)-Se(7)
Cs(1)-Se(6)
Cs( 1 )-Se( 14)
Cs(1)-Se(l 1)
Cs(1)-Se(8)

Cs(2)-Se(1 1)
Cs(2)-Se(3)
Cs(2)-Se(9)
Cs(2)-Se(12)

1.207(5)
203(6)

253(6)

2.612(7)
2.623(7)
2.834(7)
2.836(7)

2.1 1(6)
2.623(7)
2.629(6)
264(6)
2.818(7)
2.841(6)

3.604(3)
3.654(3)
3.657(3)
3.6633(19)
3.673(3)
3.790(3)
3.824(3)
3.853(3)
4.073(3)

3.577(3)
3.645(3)
3.6458(19)
3.677(3)

88

Cs(2)-Se(8)
Cs(2)-Se(6)
Cs(2)-Se( 16)
Cs(2)-Se(10)
Cs(2)-Se(7)

Cs(3)-Se(7) x 2
Cs(3)-Se(4) x 2
Cs(3)-Se(10) x 2
Cs(3)-Se(2) x 2
Cs(3)-Se(17) x 2

CS(4)-Se(8) x 2
CS(4)-Se(5) x 2
CS(4)-Se(11) x 2
CS(4)-Se(3) x 2
CS(4)-Se(1)

Cs(5)-Se(10)
Cs(5)-Se(14)
Cs(5)-Se( 12)
Cs(5)-Se(20)
Cs(5)-Se(21)
Cs(5)-Se(6)

Cs(5)-Se(9)

Cs(5)-Se(7)

Cs(5)-Se( 14)
Cs(5)-Se( 12)

3.686(3)
3.735(3)
3.827(3)
3.937(3)
3.991(3)

3.701(3)
3.780(3)
3.800(3)
4.159(3)
4.173(2)

3.706(3)
3.758(3)
3.820(3)
4.182(2)
4.188(3)

3.577(3)
3.583(3)
3.629(3)
3.659(6)
3.660(6)
3.686(3)
3.779(3)
3.944(3)
3.964(4)
4.012(3)

 

Table 4.4. (cont’d)

CS(6)-Se(14)
CS(6)-Se(12)
CS(6)-Se( 15)
CS(6)-Se(16)
CS(6)-Se(24)
CS(6)-Se(22)
CS(6)-Se( 19)
CS(6)-Se( 1 8)

CS(7)-Se(16)

3.751(4)
3.759(3)
3.762(3)
3.764(4)
379(3)

384(4)

4.118(6)
4.124(6)

3.639(3)

89

CS(7)-Se(18)
CS(7)-Se(6)

CS(7)-Se(19)
CS(7)-Se(15)
CS(7)-Se(] 1)
CS(7)-Se(8)

CS(7)-Se(13)
CS(7)-Se(16)
CS(7)-Se(15)

3.644(5)
3.664(3)
3.670(5)
3.677(3)
3.694(3)
3.741(3)
3.764(3)
3.879(4)
3.996(3)

Table 4-5. Selected Angles (deg) for Cs3Sb5Se9.

Se(12)-Sb(1)-Se(16)
Se(12)-Sb(l)-Se(6)
Se(16)-Sb(1)-Se(6)

Se(18)-Sb(2)-Se(18)
Se(18)-Sb(2)-Se(23)
Se(18)-Sb(2)-Se(23)
Se(23)-Sb(2)-Se(23)
Se(18)-Sb(2)-Se(22)
Se(18)-Sb(2)-Se(22)
Se(18)-Sb(2)-Se(16)
Se(18)-Sb(2)-Se(16)
Se(23)-Sb(2)-Se(16

Se(23)-Sb(2)-Se(16)
Se(22)-Sb(2)-Se(16)
Se(22)-Sb(2)—Se(l6)
Se(16)-Sb(2)-Se(16)

Se(17)-Sb(3)-Se(2)
Se(17)-Sb(3)-Se(7)
Se(2)-Sb(3)-Se(7)
Se(17)-Sb(3)-Se(5)
Se(2)-Sb(3)-Se(5)
Se(7)-Sb(3)-Se(5)
Se(17)-Sb(3)-Cs(2)
Se(2)-Sb(3)-Cs(2)
Se(7)-Sb(3)-Cs(2)
Se(5)-Sb(3)-Cs(2)

9629(11)
97.1000)
97.26(10)

178.8(3)

78.8(13)

100.3(13)

91.3(10)
89.102)
90.0(12)
88.83(14)
92.06(15)

167.4(13)

935(3)
926(3)
176.2(5)
84.3304)

9593(9)
8616(7)
9485(8)
8543(8)
9095(8)

170.24(9)

127.21(7)

124.79(7)
6096(6)

121.34(6)

90

Se(3 )-Sb(4)-Se(1)
Se(3)-Sb(4)-Se(8)
Se(1)-Sb(4)-Se(8)
Se(3)-Sb(4)-Se(4)
Se(1)-Sb(4)-Se(4)
Se(8)-Sb(4)-Se(4)

Se(3)-Sb(5)-Se(3)
Se(3)-Sb(5)-Se(4)

Se(l 7)-Sb(6)-Se(17)
Se(17)-Sb(6)-Se(5)

Se(l 1)-Sb(7)-Se(8)
Se(l 1)-Sb(7)-Se(13)
Se(8)-Sb(7)-Se(13)

Se(10)-Sb(8)-Se(7)
Se(10)-Sb(8)-Se(9)
Se(7)-Sb(8)-Se(9)

Se(15)-Sb(9)-Se(14)
Se(15)-Sb(9)-Se(6)
Se(14)-Sb(9)-Se(6)

Se(19)-Sb(10)-Se(19)
Se(19)-Sb(10)-Se(25)
Se(19)-Sb(10)-Se(25)
Se(25)-Sb(10)-Se(25)

9599(9)
8572(8)
9474(8)
8507(8)
9138(8)

1 6942(9)

96.81(11)
9332(8)

9686(12)
9296(8)

9581(9)
9275(8)
9606(8)

9557(9)
9809(8)
9613(8)

96.17(11)
9755(10)
96.90(11)

179.5(3)

98.1(13)
81.6(13)
916(5)

Table 4-5. (cont’d)

Se(24)-Sb(10)-Se(24)
Se(19)-Sb(10)-Se(15)
Se(19)-Sb(10)-Se(15)
Se(25)-Sb(10)-Se(15)
Se(25)-Sb(10)-Se(15)
Se(24)-Sb(10)—Se(15)
Se(24)-Sb(10)-Se(15)
Se(15)-Sb(10)-Se(15)
Se(19)-Sb(10)-Se(24)
Se(19)-Sb(10)-Se(24)

Se(20)-Sb(] 1)-Se(20)
Se(20)-Sb(] l)-Se(22)
Se(20)-Sb(11)-Se(22)
Se(22)-Sb(11)-Se(22)
Se(20)-Sb(] l)-Se(23)
Se(20)-Sb(1 l)-Se(23)
Se(22)-Sb(] l)-Se(23)
Se(20)-Sb(] 1)-Se(23)
Se(23)-Sb(] 1)-Se(23)
Se(20)-Sb(11)-Se(14)
Se(20)-Sb(1 1)-Se(14)
Se(22)-Sb(] l)-Se(14)
Se(22)-Sb(1 1)-Se(14)
Se(23)-Sb(] 1)-Se(14)
Se(23)-Sb(] 1)-Se(14)
Se(20)-Sb(1 1)-Se(14)
Se(14)-Sb(11)-Se(14)

93.5(10)
93.0105)
87.39(14)

168.6(13)
928(2)

175.6(3)
908(5)
84.87(l4)
87.6(12)
92.1(12)

178.4(3)
89.0(12)
89.8(12)
923(6)
78.9(12)
99.9(12)
89.7(5)
99.9(12)
889(8)
88.26(15)
9294(15)

175.4(5)
914(3)

167.102)
944(6)
9294(15)
85.0704)

91

Se(21)-Sb(12)-Se(21)
Se(21)-Sb(12)-Se(25)
Se(21)-Sb(12)-Se(25)
Se(25)-Sb(12)-Se(25)
Se(21)-Sb(12)-Se(24)
Se(21)-Sb(12)-Se(24)
Se(25)-Sb(12)-Se(24)
Se(21)-Sb(12)-Se(24)
Se(24)-Sb(12)-Se(24)
Se(21)-Sb(12)-Se(12)
Se(21)-Sb(12)-Se(12)
Se(25)-Sb(12)-Se(l2)
Se(25)-Sb(] 2)-Se( 12)
Se(24)-Sb(12)-Se(12)
Se(24)-Sb(12)-Se(12)
Se(12)-Sb(12)-Se(12)

Sb(14)-Sb(l 3)-Se(23)
Sb(14)-Sb(13)-Se(22)
Sb(14)-Sb(13)-Se(20)
Se(23)-Sb(13)-Se(20)
Se(22)-Sb(13)-Se(20)
Sb(14)-Sb(13)-Se(18)
Se(23)-Sb(13)-Se(18)
Se(22)-Sb(13)-Se(18)
Se(20)-Sb(13)-Se(18)
Sb(14)-Sb(13)-Se(19)
Se(23)-Sb(13)-Se(19)
Se(22)-Sb(13)-Se(19)

178.9(3)

81.4(13)
97.9(13)
918(4)

87.4(11)
91 .9(1 1)
914(2)

87.4(11)
929(5)

9297(15)
87.82(15)

168.8(12)

925(4)

176.1(3)

910(2)
85.1504)

177.4(7)
178.8(4)

869(3)
921(6)
919(3)
876(3)
901(8)
927(3)
959(2)
678(3)

109.8(8)
1 124(3)

Table 4-5. (cont’d)

Se(20)-Sb(13)-Se(l 9)
Sb(14)-Sb(l3)-Se(21)
Se(23)-Sb(13)-Se(21)
Se(18)-Sb(13)-Se(21)
Se(19)-Sb(13)-Se(21)

Sb(13)-Sb(14)-Se(25)
Sb(13)-Sb(14)-Se(21)
Se(25)-Sb(14)-Se(21)
Sb(13)-Sb(14)-Se(19)

94.1(2)
675(3)
1 1 1.5(5)
945(2)
864(2)

179.2(5)
874(3)
923(3)
870(3)

92

Se(21)-Sb(14)-Se(l9)
Sb(13)-Sb(14)-Se(20)
Se(25)-Sb(14)-Se(20)
Se(21)-Sb(14)-Se(20)
Se(19)-Sb(14)-Se(20)
Se(24)-Sb(14)-Se(20)
Sb(13)-Sb(14)-Se(18)
Se(25)-Sb(14)-Se(18)
Se(21)-Sb(14)-Se(18)
Se(20)-Sb(14)-Se(18)

953(2)
67.8(3)
111.9(3)
19.58(15)
94.1(2)
112.6(4)
673(3)
112.0(4)
944(2)
868(2)

E. Conclusion

CS3Sb5Se9 was prepared by the solvothermal reaction of C8286, Sb and Se using ethylene
diamine as the solvent at a temperature of 154°C. It has a more ordered structure than
previously described and it consists of selenoantimonate layers parallel to the ac-plane.
The alkali atoms are present both in between these layers and also in the tunnels formed
within the layers. This type of low temperature reaction technique helps in retaining these
selenoantimonate building bocks, which may not survive under traditional high

temperature solid state reaction conditions.

93

References

1.

1. Sheldrick, W. S.; Wachhold, M. Angew. Chem. Int. Ed. Engl. 1997, 36, 206-
224.

Rabenau, A. Angew. Chem. Int. Ed. Engl. 1985, 24, 1026-1040.

Li, J.; Chen, Z.; Wang, R-. J .; Proserpio, D. M. Coord. Chem. Rev. 1999, I90-192,
707-735.

(a) Laudise, R. A. Progress in Inorganic Chemistry, vol. III, Interscience, New
York, 1962. (b) Barrer, R. M. Hydrothermal Chemistry of Zeolites, Academic
Press, London, 1982. (c) Laudise, R. A. C&EN News, 30, 1987. (d) Breck, D. W.
Zeolite Molecular Sieves, Structure, Chemistry and Use, Wiley, New York, 1974.
(e) Corbett, J. D. Chem. Rev. 1985, 85, 383. (f) Lii, K. H.; Haushalter, R. C. J.
Solid State Chem. 1987, 69, 320. (g) Haushalter, R. C.; Lai, F. W. ibid. 1988, 76,
218. (h) Haushalter, R. C.; Lai, F. W. Science, 1989, 246, 1289. (i) Mundi, L. A.;
Strohmaier, K. G.; Goshom, D. P.; Haushalter, R. C. J. Am. Chem. Soc. 1990,
112, 8182. (j) Haushalter, R. C.; Mundi, L. A. Inorg. Chem. 1990, 29, 157. (k)
Haushalter, R. C.; Mundi, L. A. Chem. Mater. 1992, 4, 31. (1) Meyer, L. M.;
Haushater, R. C. ibid. 1994, 6, 349.

(a) Stein, A.; Keller, S. W.; Mallouk, T. E. Science, 1993, 259, 1558-1564. (b)
Gopalakrishnan, J. Chem. Mater. 1995, 7, 1265-1275.

(a) Whittingharn, M. S.; Jacobson, A. J. Intercalation Chemistry, Academic Press,
New York, 1982. (b) Rouxel, J.; Brec, R. Ann. Rev. Mater. Sci. 1986, 16, 137. (c)
Bedard, R. L.; Wilson, S. T.; Vail, L. D.; Bennett, J. M.; Flanigen, E. M. The Next
Generations: Synthesis, Characterization and Structure of Metal—Sulfide-based
Microporous Solids, vol. 49, Elsevier, Amsterdam, 1989. (d) Bedard, R. L.; Vail,
L. D.; Wilson, S.T.; Flanigen, E. M. US Patent 4 880 068, 1989; 4 933 068, 1990.
(e) Parise, J. B.; K0, Y.; Rijssenbeck, J .; Nellis, D. M.; Tan, K.; Koch, S. J. Chem.
Soc. Chem. Commun. 1994, 527. (1) Tan, K.; K0, Y.; Parise, J. B.; Darovsky, A.
Chem. Mater. 1996, 8, 448. (g) Mahan, G. D.; Sofo, J. 0. Proc. Natl. Acad. Sci.
USA, 1996, 93, 7436. (h) Ramirez, A. P. Nature, 1997, 386, 156.

(a) Liao, J. -H.; Kanatzidis, M. G. J. Am. Chem. Soc., 1990, 112, 7400. (b) Liao, J.
-H.; Kanatzidis, M. G. Inorg. Chem. 1992, 31, 431. (c) Liao, J. -H.; Li, J.;
Kanatzidis, M. G. ibid. 1995, 34, 2658.(d) Kim, K. -W.; Kanatzidis, M. G.; J. Am.
Chem. Soc. 1992, 114, 4878. (e) Kim, K. -W.; Kanatzidis, M. G. Inorg. Chem.

94

1993, 32, 4161. (D Chou, J. -H.; Kanatzidis, M. G. Inorg. Chem. 1994, 33, 5372-
5373. (g) Chou, J. -H.; Kanatzidis, M. G. Chem. Mater. 1995, 7, 5. (h) Chou, J. -
H.; Kanatzidis, M. G. J. Solid State Chem. 1996, 123, 115. (i) Chou, J. -H.; Hanko,
J. A.; Kanatzidis, M. G. Inorg. Chem. 1996, 36, 4.

8. (a) Sheldrick, W. S.; Kraub, J. Z. Naturforsch. T eil B. 1985, 40, 1130. (b)
Sheldrick, W. S.; Kraub, J. ibid. 1986, 535, 179. (c) Sheldrick, W. S. Z. Anorg.
Allg. Chem. 1988, 56, 223. (d) Sheldrick, W. S.; Schaaf, B. Z. Anorg. Allg. Chem.
1994, 620, 1041. (e) Parise, J. B. J. Chem. Soc. Chem. Commun. 1990, 1553.

9. Li, J.; Rafferty, B. G.; Mulley, S.; Proserpio, D. M. Inorg. Chem. 1995, 34, 6417.

10. (a) Schimek, G. L.; Pennington, W. T.; Kolis, J. W. J. Solid State Chem. 1996,
123, 277. (b) Wood, P. T.; Schimek, G. L.; Kolis, J. W. Chem. Mater. 1996, 8,
721. (c) Young, D. M.; Schimek, G.; Kolis, J. W. Inorg. Chem. 1996, 35, 7620.

11. Sheldrick, W. S.; Hausler, H. -J. Z. Anorg. Allg. Chem. 1988, 561, 149-156.

12. Lange’s Handbook of Chemistry, p 1.199, 5.105, 6.139.

13. Sheldrick, W. S.; Wachhold, M. Zeitschrift fuer Naturforschung, T eil B.
Anorganische Chemie., Organische Chemie. 1996, 51, 32-36.

14. SAINT v6.45, 1997-2003, SHELXTL v5.1, 1998, Bruker Analytical Xray
Systems Inc., Madison, W153719, USA.

15. TEXSAN: Single Crystal Structure Analysis Software, Version 1.8, Molecular
Structure Corp., The Woodlands, TX 77381, October 22, 1996.

95

APPENDICES

96

4.. 5814.1548343148831444451

4.. 0451484838014Eem44a14axo1
240$ 4.814346530143881444451
8% 4.8141483614444346.-
.85308 8:. peanulb4mqov148mbol4444xol
$8.4 nae-4.4881381448-

4.. 36813480441483814444401

4.. 44481054814454.3143on

4.. uglofim148mbol4axo1

4.. 49441344481489.8139on

4.. 52814848481444on

4.. 84444584414848.4843on

4.. §1Soal4aoEoSmaoEI44ool

4.. EISofilfioEoSmeglzool

4.. v§1é0414ag058§14431
43mg o§fl§814ago§ma0814481

z N18§1a4e§eu4au
4444984: 8342, 448

8.8 «EEaNIo4w5144ool

8.3 $3Ho4w5H=ooH

8.8 44%. 94451448.

$424.84 615445414481

6:843 61.488414466-
844482 a ems. :8
.4448 64.4 .4443.-.

.N .4214- .4.

.4448- ..4 .4444.

.N- S. .44-.

444.8- .Ste 42+...

.4. .444; .3.-.

.444: .4- .383

.N S .x.

§4181me441>4=a01§§m1

14484
4.. 2-441083144444431 8814-3544541

4.. 34448144313244.4581

.v. 4.4 .o 4:5 wddé 844444.4- O :5 84445. 43348-545.
33.444 2.2.41 .5. mm.

.4... 4 . 4 .c 465 wedé 844444.4- 0 40> 844444-4- 430444458444.
34.4.46 4:3 w.e.m.v 84446-4- 0 40> 84.4.4.4. 4384444825.
vowfio 836 V4. .v4.

.44. 4 .4 .o 4.48 med-v 844494. U :5 8443.4. 484448585.
vm~4.o 3.2.44 .m. .m.

85813812518081
wglee4€o44m€14a81§183a1
4841=e4flonm€14u8lugb188a1
4.04444448044104518031

4§m1§188al

14484

2.44:. 4.4446319884148866-

1 .o4m M4444 v4 391

83 «44488.4 4848240

4.. 30484124881484.5461

4. .981w54ae14a6851

4.. non—4.481088148482401
ou§o4§m1§148482401

4884-44445 4.6568184551463-

emaanam 44044 54.4 440 a. 4444.24.44.43.

97

234-<4§~4:E<m<4/<~<o-.4448.o+446443492644. 4.. 4.4088442144813484444481

484amounxolaounvquxodfioqufil 4.. aou844eo18€1w§=44881

€488.45 48618465514412.4421 444284.? 84888146424824-8442.

6384.6. 4.6568184888191521 844 81.382.14.442.

448448 4co§aoblaowe€b41m4IoéBI when 43816448344134481

88w Eowoéxnleouasflm84.818031 No.3 4.4813051844219531

44944-4446 5486815484818:4814:3441 924 44341805134481.54461

48.4446 44.384444148445481846184431 mm an14144E441mq—4041FEB1
.m\4<~<6.4~+<~<oh4r.4 4.4- 35141486418448.5461

8243 4.4aRem-[2.4%8.82.424482444u; 648. n 46614148418442.5461
2.864.868.446312184481 n- 58134144518448.5443:

048 082481m5444w 4631441244421 4 m $144144E=Im44¢041§1

:8 63145818416548- .4. 88.441484184421844..-

vcmm 4361404onu1o§o§m1m410q¢81 mwmcd 44826151844214.8461

.Bw34 :03 044 4443 83 4-4< co 46844 flees-4-x mmvod $5444>4evoly41>a1m£421§1

4:8 .44 48 pee-44 8244 we emu—44 8 8434 Bone 444844343 84.4w 40448::1mé2145444441
2a <N<m no woman 398.4544 458244.48 8.4 804484.42 4.. $1>moup1mv§pasm1§1
.40 84240 244 9 448.642 8: 4.44 4:8 .20 4348984 4.. oEuIEESEImvSUQSmIgGI
54 4482848 .64 448 4.8.. 2 4.3488434 A (4..-4 4. 58143881882881.4861
.40 4843298 44424845 044-4. .<N<-.4 gamma: 3.4 Son 9 4.. 84482413846448.819561
48 m .4443 .44 no 484.344 03 .44 $88.34 4946445248 (~54 4.. 4.881482183188804614544441
no 48344 0.3 m 44.4 me $268» 4648 ~43 488,444 4434303 4.. 85081448883881.5461
044-4. .Eeuoocou -4-4< 483w.“ <~<n4 4e 48805-434 4.. 184>o4e145805w381§1
m4480p14a4oo44m10é21 844444an hegefioeaofilcegafilfimgl

4.. 3.48681844844442413459431 .6443 p048» mace-4-08.4. 35814404434481.5431

4.. moflnfiwl 84=oo4eEIwE4=44881 .5432 lacunae-414544441

.4484 96.5.4249 4844.44 53642518868158.

48-54-44.45. assume-65688453988.- 44484 83869664166481.4844.-
.884 84483144468514.4451

54654254 Sax-44,45. 84.281656336439681 4.. 84381884441438.4314?»-

4. concavBlsavIweuafiool 4.. 514.14.384.48143844441444451

98

laco—

N 8 :3: 358.8 3:883 833 3:833 Mew“
N _ as: 3:888 3928.? 833. 3:328}: mmam
_ was €388 3:88.? 833- #:8893mmwm
N _ 5: €288 3:882 833. 3:88.? mwm
N _ .aS 3:888 3:283. 833. 3:883. .mwm
N _ 5: 33:2: 3:852 832- 3:_8zd.mm3m
N _ a5 3323. 3:383? 83:18.88 mm.“
_ a“: 358.8 3:NN3NN.o- 833. 3:588..me
N _ 5: 355.8 3:833 833. 3:_8:8.mmNm
N _ 65 3:88... 5:828. 833 3:58.8. .mmm
N 8 as 3888 3:NEN.¢ 833. 2 3828.8. Wm
_ 5: 3:882: 3:5 3 88.8. 583de ammeM

. . m u N _ 5:
39 38.8 52 8N8. 88... 33383.8. .fi 38
3.5 3:353: 3838.8 88.8. 3:33538 mm.

85 3:333: 5882. 833. 3:883 a 3m

. . m u N
_ ES 3388.8 3888.8. 833- 35.83. 5 mm
. . m u N _ Ea:
3338.8 588; 833. 3:88;; a N5
Imv-
ES 3:».858 5388.8 833 3:82:28 5 2m
anonIBESEISfiIBSaI
bnfiommaluoougfiluzmlfiofil
mwaulfiuaoaaalozmlaaal
male—aolozmlfiofil
gum—aciulzbofifixmlfiulaoal
hugogloamlfiofil
ambigulogmlaofil
tacoluouamIDIBmmIEofil
nififilogmlfiofil
Alfiablammlfiofil
xlaowaluzmlfioaal
Enamloglofilfiofil
32.23.89“.
Inoc—
82: sfilaaamuxuoéau
sod .éuaaammamuéam
18.— I=alm 1353.38 £12621
:3 .8 a .8 30883.8 2&2
38.8 adsoaumzumfiuéa.
88.8 madsoaumsummoéan
2.8.8 &H.eénxum_-3uau
9.8.: 3 88am Mum—10621
o sgliaa 2 Sue
o: Egaafifiaauzmsuam
:3 $52 38:: .9.— once

99

N 333-3 3:8.N 8 :m

.8 . 3883 a :m

N 83 _ 3883 a :m

N . 3:833 88 :m

wan—palvaonlfigml

mlgufifixmlozmlvaonlfiooml

ougmfilwnonlfioomn

NI.oQEIozmIESaIEBIEoowI
_I~38_I281808I::318oowl

Inco—

8283 .m._ wfilgfi £88 @5888

8: com: a 3:8 :8 :o 82:80: 389:8: 885x888
2 .3088? .8930 3 35.8: o8 >2: can?
:8: 3:: 0.8 88258: :8 E 88 52.30: macaw—280
”mo—wan 8288 98 83:8 38:88: E 38 .3 8.59588
2: E 8:963:85 85888 85 :83 08 3:8 :8 2:.
#588 8.8538 :3 2: was: 8895.8 0.8 328—: 8..
92 5038: £88 862:: 2: E :8 2: E85: «:8 =<
m=SoUIEooamIEoowl

:::.:

2:288- 8.8 3:388 3888 3:888 88
:8:

2:288- 8.8 3:888 38888 3:288 8
:8:

3:888 8.8 3:888 3:888 3:88 8
:8:

3:88.? 8.8 3:888 3:888 3:888 Nm
:8:

23:39:. :8: $538.: $328.: 35:33.: em
:8:

2:288 8.8 3:288 3888 3:888 33

8.8

3:888 8.8 3:888 38888 3:888 em
8.8

3:288- 888 3:888 3:388 3:288 8
8.8

2:288- 8.8 3:888 3:888 3:888 8
8.8

3:888. 8.8 3:888 3:888 3:888 8
888

8::88. 8.8 3:288 3:888 3:388 s.
888 33388 888 3388 3888 3888 N8
8.8

3:888. 8.8 38:8 38:88 35.88 8,.
8.8

3:888 888 3888 3:888 3588 am
8.8

3:888 888 3888 3:888 3:888 am
88

3:3888 8.8 3:888 3888 3:888 mm
888

3:88.? 8.8 3:888 3:888 38388 NE
88

3:888 888 3888 3:888 3888 :m
SIDISEaI38I8o81

3 33185138489“.

35.838882“.

mmIDIOmEquzmIEBaI

Nalbnaansmmuaozl

:-:.8§.sa.&§.

~3218€u|83|8¢8|

100

N 8Q 3883 mm 8
N SC 3383 :8 8
N 88-8 3883 am 8
N 88.8 3883 mm 8
N 33C 3833 :8 8
N 88; 3383 am 8
N 28.8 3383 3m 8
N 333.3 3:883 38 8
N 38 3 3:883 38 8
N 88: 3883 :m 8
NM 3: 33 U. 8

N 38. m 3: 33 E 8
N 38 ._ 3883 :8 8
N 38. 8 3838.3 8. 8
N 385 3883 :m 8
N 8C 388.3 38 8
N 88 8 3883 mm 8
N 83; 8:8. 3. U. 8.
N 88 £232 3 s. 3—
N 38:8 3883 8 8.
N 38 _ 3383 8 E
IN . 3383 8 Q

N 38 3 388.3 8 8.
NM. 3: 33 8 a.

N 88 m 3: 33 8 s.
M... . 38:3 88 8.

N 88 28:3 88 i
N . 38833 i 3.8

N 28.3 3383 8 3.8
N 88-— 3883 88 8..
N . 3883 88 88

N 8 3883.3 8. :8

m . 3:83 8 8..

N 83 _ 3:83 8 88
m . 3883 8 8.—

N 8C 338.3 8 88
N 88 _ 3883 8 88
N . 3883 8 88

N . 3:83 8 mm

m . 3383 8 mm

N 8C 338.3 8 nm
N 28.3 3883 8 an
N 88 m 3883 8 nm
N . 38:3 8 am

N . 3883 8. 38

N 883 388.3 8 38
N 88 3 38883 8 38
Nu3 38883 8 38

N 88 _ 38:3 8 38
m . 38:3 8 38

N 88 8 3383 8 38
m . 38883 8 38

N 88; 38883 8 mm
N 83 _ 38883 8 mm
N . 3883 8 an

.N . 38333 8 mm

N 88 _ 38883 8 38
N . 3883 8 38

IN . 38383 8 38

N 88 _ 3383 8 38
N . 38383 8 an

N 8 3:83 8 :m

101

N mxlN QWN €38 am :m %
Nun: N: N €38 am am cm

N m: N 2m _ €36» am am Nm
IN SPN . €ng Nm «5 Nm

N «X N 8m _ 52?: am 3m B
[N 9% .N N 635 a :m a

N m: N SC 553: % gm Nm
N m: m . ENNNN «m 3m Nm

N SNIN 8C 359; a «a 8
N N 8m _ ENNNN cm 3m Nm

N N . 353.: «m «E Nm

N N £3 $8.3 a 2m 3

Nnmom _ . 858.3 Nm 3m Nm

N 8m _ 83 3E: Nm 2m 8
N . Gm: $2.3 Nm 3m 8

N. Na w 832.8 5 mm a

N . Sm N ANVNNNN 8 mm 3.

N. Asia: 5 mm mm

. IN . . ANVNNNN 5 mm mm

N Na 2?. 12:5: 5 mm mm
N 3C . 83% a Na mm

N m: _ . @NNNN 5 mm 8

N Emu... . 832.8 mm mm mm

N Sn N . €33 Nm mm mm

m . . €38 mm mm mm

N new; .533 a NE a

.N 3C . Eng» 5 NE mm

N NE _ SC 3x2: 5 NE am
N 3 _ . $38 8 NE om

N .I. 52¢: a N5 am

N. Sm 29:3 5 NE am

m... . . $38 a N5 om

N . new _ 8&2; 3 NE a

m . . gag 3 NE 8

N 3C . 3:93 am NE om

N n 3 m 833% mm :m 3

N N @832 am am cm

N w New _ €83 mm :m cm

N m . €33 mm 2m em

I N 2m m . 53.3 mm :m cm
N 2n n 8C 858...: mm :m a
N 2% m . €33 mm 2m 2m

N. new 232.? cm 5. a

N. .533 to, an em

N 83 . NeeNNN E 2m 2w
wen—nalxwaulfioowl
mlgogmlogmlufiaalaoowl
~1§u88>mlozmlo_w§lfioowl
ofiqalfiooml
mn—can—loummlfioNan—wglfiouwl
~I_ecu—IoNNmIEoNan—waaIEoomu
_I_unm_no:w189alo_wqalfioowl
.82

N 2n... 5%; a. N;

N Sn CNVRNN Ni Sm

N 3%. N AVE? E am

N SnuN 6%? 3m om

N SalN 5N2; NE om

N a u_ SEN NE mm

N n3. n 82$. 5. mm

Nun ENNNN mm 3

N «3. n NNVNNNN 2m 3

102

N. abate: Nm NVN 8

N . «8 N 368$ Nm SN 8

N. .INNNNS8NN 8. SN 2m

N. SIN N $8.8 Nm UN 2m
NI?“ NI m $8me 3 NV. 8

N 9% N «cm W $8.92 8m 3. a
N NE N . $.38 3 SN 2m

N WRIN NEIN $3.8 3, SN 2m
N n 9.3. 8:82 8 SN 8.

IN N . $8.8 8 9 2m

N m a N 5:32 3 UN 2m

N mxIm .INNNNNNNNNN 8. UN 2m

N m: m 3 N $8.8 8 SN 2m
N. NE N 838.8 2m 3. 2m

N . NXIN $8.: UN NNNN 8

N. 33 $8.8 3N NNNNN 2m

I NH $53.. a. NNNNN 2m

N 2m N am N $2.3 8m NNNN 2m
N nWm N. $32 % NNNN 2m

N m: N .8388 2m NNNNN 2m

N m . 3832 SN 3N om

N n SNIN $83.2 NVN NNNNN om

N m . $2.8 5N NNNNN Nm

N n SnIN $2.8 NVN NNNNN 8

N m an N $3.8 5N NNNNN 3

N m. $3.3 NVN EN 8

N . 3“ N $8.8 em NNNNN em

NI. . $8.5 em 2: Nm

N . 3m N $8.8 em :5 B

N. 8n N$2.NNN om NNNN .8

N. . $8.8 om NNNNN 8

IN 8an . $8.8 om NNNNN Nm

N 8m N EnIN $8.8 om EN 5
N SnIN “Mn N $8.8 em NNNN .8
N SmIN .$2.NNN om SN 8

N. «on N I832: Nm EN 8

N . new N $2.5 Nm NNNNN mm

NI: $§$ Nm :5 8

N EmIN 8m N $5.8 Nm NNNN 8
N 3n N .$NNN.8 5 SN 8

N SmIN . 8:88 8 SN .8

NI. . $8.8 5. mm 8

N . SmIN $6.8 5 mm 8

N . 3mm $2.2 8 em 5

N . 08 m $3.8 8 am 8

N .I. $8.5 8 am 8

N . an N $8.8 mm mm 3

N . oenIm $82: 8 am 5

N . .5 m $8.8 8 am 8

I NI. . $3.3 mm mm Nm

N mom N 3m n $8.8 mm mm 5
N 8m N 98 m $82: mm mm B
N 8mm .$Nm.3 mm mm 8

N 2.3 98% 8:58 5 am 5
N 28% . $8.8 5 9m Nm

N 3“ In . $8.8 8 mm 8

N . 3m N $8.8 UN 3m a

N. n3 N $2.NNN U. <5 cm

N . m 82.5 NM gm em

N . an N $8.: UN in Nm

m . . $8.8 UN 3m 8

N. new N $822 SN «5 mm

103

N. 8.84 $2.8 NE 8 NE

N. 88 N 2:88: NE N8 mm

N . . $8.8 NE 8 mm

I N. $8.8 NE N8 NNNNN

N 88 N m8 N $8.8 NE N8 mm
N 88 NI. 2:88: NE 8 mm

N 8m N .888 NE N8 NNNNN

N 88 .m .3328 mm 8 an

N 88 N .$2.8 mm Nm :5

N. . $2.8 mm Nm NNNN

N . 88IN o8 NNNN Q E

N . 88 3.8 Ni ON UN

N .I. $8.8 NNNN SN «5

N. 2m 8 $8.8 N8 UN 8

N. 88 N $8.2: NNNNN SN 8

N .I. $8.8N NNNNN SN 8

N. 88 N $2.2~ N8 NM 8

N .Im $8.8N NNNN UN 8

N. 88 8 $8.8N N8 UN 8

NI. . $8.8 NNNNN SN 28

N. 88 N $8.8 NNNNN UN 28

N 88 N 88I N 32 5. UN 3N
NI88 NI. o8 a. UN 2m

N I88 N I88 8 88 UN UN 8

N 88 N 8mm N $2.8 UN UN 8
N 88L .$I8.NNN UN UN 8

N 88 IN 88 N o8 3N NVN 8

IN 88 IN 8 $NN.8 3N NM 8

N 88 N Sm 8 8882 SN 5 8
N 88L .858. SN NVN 28

N 88IN 88 N $832 UN UN 28

NI88INI. c8 E E :m

m 88 NI 8 8 88 UN UN 8

N 88 N 88IN $8NNN NVN SN 8
N am N .628 SN NVN 8

N 88I N 88 N o8 3N UN 8

N m8 N m $8.82 NVN UN 8

N 88 Nm8 2388 UN NM 8
N I88 NI. $8.9: UN UN 28

N 88 N am N $8.2. UN UN o8
N. 88 £288: E Q 8

N. 88 N $8.:. «5 UN 8

NI. . $8.; 3m NVN 8

N . 88 N $8.8 3m SN 8

N .Im. $2.82 3m NVN .8

N. 88 8 $2.2 3m SN 8

NI. . $3.82 :m E 28

N. 8 N $3.82 3m UN 28

N 888 QMIN $8.82 8 NVN 8
N 88 8 . $8.82 8 UN 8

N 88I8 88IIN $822 8 UN 8
NI 8 m8 $8.8 8 SN 8

N 88 8 8I8 8 $8.8 8 SN 8
N 88 .8. . $8.2. N8 NVN 28

N 88» 88IN $8.2. 8 NVN 28
m 88 w . $8.? 8 SN 8

N 88 N 88 N $NN.NN 8. UN 8
N 8m N 8 88.8 8 UN 8

N 88IN 88M NNNNNNSN 8 SN 8
I N am N ASN.8 8 UN 28

N 88 N 88 NNmNKBNNN 8 SN 28
N. 88 N $88 8 SN 8

104

w... . 3:88 SN 88 5

N . 88 N 3:88 N8 28 NNNN

m. . $8.2 N8 28 NE

N 88 N 38.2 NNN 28 5

N N8IN N.8IN $8.8 NVN 8 2m

N 8m N N.8I N $8.8 NVN 8 N8
N 8 N 8m N $8.82 UN 8 NE
I N N.8I N. $8.82 SN 8 NE

N 8 N 88 N MN :8.N2 3m 8 N8
N 38 N 88 N $8.8 2m 8 NE
IN N.8IN . $8.8 3m 8 NE

N 8 N 88IN $8.82 N8 8 NE
N N.8IIN . $8.82 N8 8 NE

N 88 w . 3:88 NE 8 N8

N 88 8 8 $8.8 SN 8 NE

N 888 8MI8 $8.8 SN 8 NE
W 88 m . $8.8 SN 8 mm

N 88 8 88 N $8.8 SN 8 NE

N 8 88 8 3:88 NE 8 NE

N 8 . $8.8 NE 8 «E

N 8 88IN 3:88: NE 8 mm

N M88 . 3:88: NE 8 mm

N 88 8 QMIN $8.8 2m 8 mm
N . 8m N 3:88 mm 8 mi

N . 88 NMN:8.NNN mm 8 :8

N . 88%. $8.8 am 8 am

IN . 8m 8 $8.8 mm 8 am

N 88IN 88% $882 N8 8 an
N e8IN 88M $NN..N.NN N8 8 am
N 88 8 88 8 3:88 am 8 mm
N 88IN .$8.8 SN 8 :8

N 88IN .388 N8 8 NE

NH $8.8 NNNNN 8 8m

N . 88IN $88 85 8 am

m . 88IN $8.8 mm 8 «E

N 88L 88IN $8.8 mm 8 3m

N N8IN 88IN $8.8 3m 8 «E

N 8 N m8 N $8.8 3m 8 NE

m 38 m . NN :88: am 8 NE

N 88 N 88 1288: 2m 8 NE
N 88 N. $8.88 vaN 8 NE

N 88IN... 3:28 NE 8 NE

N 8 88 8 3:88 UN 8 E

IN 8 . $8.8 UN 8 N8

N 8 88 N 3:882 UN 8 NNNN

wm . 3:8.N2 SN 8 mm

N 88 8 .INN:NN.8N SN 8 NNNNN

N 888 28 N $8.8 UN 8 N8

N 88Im . 3:8.N2 SN 8 mm

N. 88 N 3:88 N8 8. NNNNN

N . . $8.8 :8 8 mi

N 88INI.$NN.8 N8 8 mm

N. 88 N$88 UN 8 NVN

m . . $8.8N SN 8 nm

N. 88 N 8:88: SN 8 «E

IN . . $8.8 UN 8 2m

N I88 NI. $8.8N UN 8 am
N 88 N m8 N $8.8 SN 8 EN
N 88 N .INN:8.8N SN 8 :m
N . 88 N $8.8 2m 8 an
N . . $8.8 am 8. :m

N 88IN . 338.8 3m 8 am

105

$8.8 mambNaonNNeuoéem
N8.N- 58 88% 88 2&2
8N8 8888888888
88 NEIsuNNNINaNNoQIBsmsaIpeNNNI
8.8NI I NNaIawaNNIaNNenpeNNm
N88 .38 see 8888 85888 :88
N 8m8IN 8:88 UN 38 E
N 8I88 N .INN:8.88N NVN 38 N8
N 888 N 88 28:88.8 5N 3N8 N8
N 888 N 3:888 UN 38 an
N. 48:88.8 UN 38 N8
N . 888IN 8:882 SN 38 N8

106

Smém =5IE20530JE8ANI—Exol
NE osImIEmboIEfiI
.35me 8:. vofioEIb_m:ovI_SmbuI_aon
8mm geIQEQuIEmEIEEI

N. muglbmaouIEmEuI—Eon

m. EEIonmIEmbolzaon

m. vEIoEmIEmEuI—Exol

m. nguNmmIEmboI—Exol

N. So_oaI~SmEoI_~non

N. :ountomovlambqunqu

m. anISofilusfiouzmnuEI—Eol

M. :5ISofiIEoEuSmaoEI=8I

N. vomsIméEIEoEosmauEIzooI

ANVMQN _o_:BEo&:8I EoEoSfiuEI =ooI
NI 8.5:I £258 I=ooI

3%. 82 2:28 =8I
co co guMIoEfiEouI
8.8 sfimxmfimfiom
8.8 235 o_m§I=8I

8:82 #552203

5&3. Famine?
as. _ SN a 59.2 :8
.QE .3-» SE.-.

~51- .x.

.QE- s 53..

.N- S- .x-.

.SE- .SL- .5}

.N- .3; .f

.5: s- .St...

in x.

NOW 3 ImomIPSvoI Fogml
Inco—
a 2- : IogInonIouanmIaboEEhmI
a wgomI __ooIFoEEmI

.126 :5 m.o.N.v 835. U _o> 835. 3:32:85.
33.2 2.2.? .5. .5.

31.—.0 :5 wddé 85a... U :5 835. Egan—=85.
22.3 «and- hm. hm.

.v. _ . _ .o :5 w.c.~.v 835. U _o> 833. 35:585.
:3; womnd- .oh. .0?

.1: .c :5 w.o.~.v 833. U :5 853. 3:85:25.
vovwd 88d .v_. .M.

.v. _ . _ .e :5 wddé 339w 0 _o> 83: 3:38:85.
vmfi .o 32. o .m. .wI.

8593 “now Ionbl EOEI

wglgfiommmvl 30ml IESaI
_~8I:o_m:o%=vlfioml IEQaI
:ountomouI IEBaI

3ng :82“
Inco—

mo.3o “Aw—eBIaBEQI—aogonoI
.ov. cob co. am 3. MAE 3 CM 3 in.

:5... IEEEéI EEEEuI

N. buBEI flanmI _8._EofiI
N. H:_omlw:£oEI_mo::o;uI
N. :oEEoquEa:I_8::o:oI
oanoamwauEgIEoEozoI
8-53mi 85.55.32.463-

.fi.ém£.m§£.v_ mo: mam Bo .: 5:2me

107

528°... .Souaofiqufimmmoéem

Ecow Euwoéxnl 8558 I35 IESuI

@956 588% 5558 I35 IIEQa

Sub—u banglgusfimImoamIEofiI
.M\A<N<ULN+<N<OI.~VIIIA—

98:3 Ewaamdm+<~<aGmod¥A<~<omv<N<£>nB 28.
m~_So:Iw::5w_uBI 5 IoéouI

£8 oEonomImnuaw—oBI m_I gap—I

=5 unblewEI w. I052

gm”— moooluoaofllobzongflIoée

Fema— :o>o 3 EB 85. I5< :o comma 59055

:5 .m :o v3.3 805 mm owE mm 83: Sons 5855:...
Pa <N<n_ :o :33 392a-”— ..:oEu:c2 :8 3260:»:
go 8650 05 2 Ego—2 8: 2 :5 .80 C3588.“
a... 33:28 .8 38 Ba. m. A<~<m§=ma~ A <~<m
Me 5.83%». 2:585: 2F .<~<m gamma: .8 Son 2
.8 m 55 .m :o :83 98 M 95885 3:05—3:00 .<~<m
:o :33 8a m G we mmufivoow :5 M3 .8855 c8539:
2:. .mdouooco: I5< «magma <~<m mo 80:85qu
m=8uwl_a_oo%lo:woul

m. .uto§:l::t8=n:alw5§9:8

N. moEQaEIB_:oo_9:Iw5.:q=—8

.98. 12.238

3.5355. 80:85.52 IEBoPamegseugI
.82:

10:20am. 8-8355. =o..=_8I§...§mIma.=&=8I
5.. :ozustISavIwEEEOQI

m. EoEoEMBI =8 Iw5=EEooI

e 558:8 IflavleEEOoI

ACE—mu? :ommmoaonEcfiP—SIéEI
:8 5.35535
3.3 .Iso.I.IBE==IaaeI

5.2 fieI 52.. IE... IeeaI
of a... Is»... I3... IneaI
a .aaI _ IE... Isa... #85
a- aeI _ IE... I252 4:»va

m §EI._I.E£I§2I=E%I

m- EEIxI.§_Iau2I§%I

on xaaIgI.§_Imé2Ip:.GI

.m- =EI._I.E=I2:2I§%I
88... EningzIaceInaeI
in; 35335558:BIFEGI
32: 5955555.?
N isouImuaEsmIneeI
... oEuIatuiImuauasmIpaaI

... .58 was... $5.5. Eu...

m. ombIooSoUJSEoEmSEIgéI

85:8» 5.505888 £0568 Ina—cl

.33 :28... v.85- 0:? 358 I:o:a€EI IEEGI
3.32 ab! :oznmvfiI ShavI

mnoFd 5w:o_o>aBI :oaafifl IFEGI

Ema 2222.55 .555 IE5?

m=SucIEouamIzaon

N. 5_SouImmoooaI.BomnaI:aqu
N. xaEIHIaocunEooI.&oBaI_aqu
N. =.EIhIco:auteuI.Eo3aI_aon
N. 0:545:concuIESmnaI—Eon

108

. . m ..
N . .5... 68...... 3:28? 82.... 3.5:”... m B
. . m ..

N . .5: $28... 3:33? 83... 2:38.... m cm
. . m ..

N . .5: Emma... .2532. 83... 3.8.3... .9. mm
. . m ..

N . .5: .828... 3.5.8.. 82.... 3:808... m cm
. . m ..

N . .5... 83.2.... 8:5.NN. 82.... .5803... m mm
. . m ..

N . .55 5.2.... 5.29.2 82.... .2533... m Nm
. . m

.. N. .5:.:..N........:N%m...SmN....:.m......... m .m
. . m ..

N . .5: 3:32.... 5.88.. 82... 5.3.9.... .m m...
. . m .. N

. .55 3:22.... 528.... 8...... .N............ .m e...
. . m .. N

. .8: 8:32.... 58...... 82.... SEN... .m N...
. . m ..

N . .5: 2:38.... 529...... 82... 358%... .m N...
:mmnN

.33.... 8.: €08... $.36... 82.... .983... .m ..m
. . mm .. N :5...

8.: .. :GS... 58...... 82.... .5352... V. 3.
. . mm .. N .93...

8.: .8NNN..... .339... 82.... 8.8.5... A... 3..
. . mm .. N .33...

8... .838... .332... 82.... 8.88“... 9.. 2..

. . mm .. N .03....
.53 3:88.: Avvmvmwwd 83.... .3332. .5 N...—
. . m : N
_ .55 $303.8... A933...— oomNdI Amvmwmwvd a: 3.—
gothBEOmBIozmIESaI
.AEEommaIBESGISEIESaI
mwaclagoéalocmlfieal
male—aquzmIEoSI
b.o..&§::I>buEE>mIozmI8o.aI
xogaaooOISEIEofil
Elgaluzmlfienl
>.:3I8I8.IDI3....IEB~I
NISablongEQaI
zlfiablozmIEofiI
xluofiulo..mIEQaI
.35me Io..mIEo.aI
.3a_lo..mIEo§I
Inco—
oood :aofilsmEEmIm_Iu:uBI
.8... Ifiquaasmwamuéem
:od I:alm I:o::Emo. £Io:uo..l
.3... .2 2.. .o .833. 8......
coco... .mI.o.oa..I~—3Im_Io::2I
£8... .aI.o.8.I..3Im.IoéeI
88... .mI.o.8.I..I..I8..2I
3...... ....Iwo.o...I..Hm.H8..2H
c 3:358. 838:: m. 0:...2
:. §.§§..I.o..a==Im.I8..2I
an auaIfiasaInIauaI
2....-<.....N.=..\<m<..<N<£x.8.o+aubuiz...
:o.$8:on:cuo:uonm_Io:uBI

109

N. Sew swam mm :3

N. Scum swam 8 3..

8 m8 .683 a z:

N. . 583 a 38

N. . $23 mm 3.:

maul_n:nlvucnl800mu

Numbgmlammlvaonlfiooml

oogmmclvaonlfioowl

NI.cam—lozmlfiofilvaonIEooml
~438Io§|88~l€3|8oowl

I noo—

.mo§_a .3 9:395: 38 Magnum...

you com: a m3» :8 :0 30:58.5 Aufiobofiv 88855.?
n< .mboEEm .8900 3 35:0: 98 >05 son?
:8: Eco «.8 880888: :8 5 88 5233 gown—oboe
”mo—was H.289 can 835 $3586 3 8.8 .«o conga“.
2: 5 3.96363 2388 SE :83 8a mac :8 2E.
2.59: 85550 :3 05 main @3858 8a A853 .3
03. 52.33 035 .505: 05 E :8 05 E033 «Bu =<
mafia—uI—fiooamlaoomu

:86

8:38.? 88.8 5:388 6:888 $888.8 on;
:86

$328.: coed €338: $338.: 8:38.: am
:86 Am 338.: 8:6 Amvmmod 8:28.: 8338.: mm
08.:

2:28.? 8.8 5:888 5:888 6:888 8
8::

$3.88 83. 3:388 8::88 3:888 8
8a.:

3:888 88... 5:386 3:886 3:888 mm

8.8

3:888 88.8 5888 3:888 6:53 8

8.8

3:28.? 8.8 8:888 €888 3:888 mm

8.8

8:888 88.8 5:588 5:288 6:888 mm

8.8

3:88.? o8.o €888 5:888 6:388 a

88.8 5888 88.8 a: .988 €888 5888 mm

88.8

@8888 88.8 52.8.8 5:88 588.8 :m

8.8

8:38.? 88.8 $28.8 $58.8 588.8 mm

88.8 $288 88.8 585.8 5888 5:88 mm

88.8 528.8 88.8 $88.8 $28.8 $888 a:

888 $288 88.8 588.8 5.838 68%... Sum
N~ 3 Oman 3% 83a

m—IDISEanfiIESaI

muauaaausauasau

mmIDIOmEaIBmmIESaI

«Nuauaaausauasa.

_ _IDI8EuI8_mIEo8|

Esnsaausalasau

Inoc—

. . mm 8 N $83

was 538.8 588%; 82.? c :588 a. S»...

:m

u N _ as: 5:88 6:853 82.: GE End m 8

2m:

N _ as €888 €838 88.? @8888 m «m

110

N. 8ch 683 UN 8
N. E: n 688 UN 8
N. 8C 582 3m 8
N. 8Q 3888 mm 8
N. 8C 583 N8 8
N. 88 In 583 5. nm
N. new N 2888 8 am
N. . $888 8 am

. N. . $88 8 am

N. 88 n 583 Sub mm
N. . 5888 8 mm

N. 8m: $888 8 mm
N. 38 um 8:83. NVN «E
N. ”8'8 383 8 8
N. 88.8 583 8 3m
N. 88 e 582 8 «8
m . 582 8 3m

N. 88 N $82 8 :m
N. . $888. 8 3m

m . 588 8 mm

N. SC 3888 8 mm
N. Sm N 522 8 mm
N. . 522 8 «.8

N. . $52 8 mm

m . 583 8 mm

N. 8C 583 8 mm
N. 8“ N 53.8.” 8 «E
N. . £388 8 «E

N. . 3:2 8 «E

N. 83 5: 3. Na E.
N. 2.3 5: Na. UN NE

W . 3:88 8 E

N. m: N 652 8 NE

IN. . 65.2 8 E

N. 8m IN 5: N... NE SN

N. 8C 583. SN SN

N. «8. N 688+ 3N 5N

N. :8 8 6:83 2m 5N

.N... . €8.88 8 UN

N. 38% 3:82 8 UN

N. 8818 58?. 8 5.

N. Scum 588 8 E

N. Scum $83. 8 UN

N. Scum $88 8 UN

N. 88 N 582. 8 ON

I N. . 682 8 UN

N. 88.8 583 28. Ba
N. 88 n 583 88 I;
N. . 6:83 Bop as

N. . E83 8 Em

.N. . $52 8 Ba

N. 8n N 3188 8 a:

N. . €88 28. a:

m . 583 8 a:

N. «Mn N @888 8 m8

N. ”8.8 $82 28. Ba
N. 88 n 3828 Sue as
N. . 62.3 8 SN

Nu. €88. NVN Sm

N. New ~ 383 8 «8

N. . 583 8 Sn

N $3 583 8 8..

111

N M84 8:88 28 SN 8

N . 8818 8:88 28. N8 28.

N. . 88 8 8:88 28 SN 28

N . . €88: 28 N8 8

N. . m8 N 8:8 8 SN 8

N. . 88-8 52: 8 SN 8N8

N. . 88 8 $88 8 88 Sup

I m . . 8:88 8 SN 8

N 88; 88:8 688 8 SN 83
N. 88 N 88.8 6N8: 8 SN Sop
. N. 88 N 8:88 8 SN 8

N. 88 8 88w 88.8 28. 88 Sue
N. 8.8 . 8:8 28. N8 8

N. 88 m . 8:8 28. EN 8

N. . 3.8 N 8:88 SN N8 8

Nr: 888 UN N8 8

N. . 88 N 888 SN N8 8

8 3.81m . 8:88 8 N8 8

N. 3.8 N QM N 88.8 8 N8 8

m . 88; N N N88 8 N8 8

N. :8 m 88 m 2:88 8 N8 8
N Na. 8 m8 N 88.8 8 N8 8

N NE 8.. 8:88: 8 N8 8

n N. Sm n . 8:88 8 N8 8

N. 88 m 88 18:88: 8 SN 8
N. 88.8 . 8:88 8 N8 8

N 8.» m . 8:88 8 N8 8

N 88 w . 8::8 8 N8 8

N 88 N . 8:88 8 N8 8

N. . 8:88 8 SN 8
Mel—namioiualfiooml

mIF§8IBN8Ion§I88wI
NIEuEENAmIozmno—wnalfiooml
onaaIEoowl
mINBNNIoNleficNaIuNwfiIEoowI
~|_ona_IoN8|89alo_w§IEoowl
NINonuNIozmlaoNan—wnaIEOoml
Inoc—

N. 8on 583 EN 28.

N 8% 8 583 EN 28

N 881.8 583 am 8N8

N 88:8 582 N8 2.8

N 83 m €82 N8 209

N 88.. N 583. SN 8

N 88 N 8838 NE 8

N. 88w 85.3 N8 8

N 28.8 583 N8 8

N. 88 8 582 N8 8

N 88: 582 NE 8

N 2.9 8:83 am 8

N 88L 888N EN 8

N. 88 IN 8:8.N EN 8

N 88 N 888.8 E 8

N 88.8 $88.8 2m 8

N. 88.18388 N8 8

N. 88L NN:NNN.N mm 8

N. 88.8 8:83 am 8

N. 88.8 8:83 am 8

N. 88 ..N 5838 N8 8

N $8.8 €88 UN 8

N. 5. 8 $88 UN 8

N 88.; ENNNNNN 2m 8

112

N. 8M8-N . €8.88 SN SN 8

N. 8.8 N 28.8 8.8 3N 5N 3m
88 8.8.8 UN 5N8

N888 N.3N8 N888 SN 3. 8

N. 88 8 N88 M 8:82 UN UN 8
N. 8N8-N 28.8 5888 UN UN 8

N 88m N Sm 8 88.8 Q E 8

N. 88 8 N88 m 8582 SN UN 8
N 88 N 8N8 1:888 UN UN 8

N. 88.8 N . €8.82 3N SN 8

N N88 8 8:88: «8 SN 8

N 38.8 3.8-N 888.. ..Nm UN 8

N. 28.8 88 8 8:88 «8 UN 8

N. N88 8 2.8.8 8:88.. «8 UN 8

N 28.8 28.8 8:8.2: .8 UN 8
N. 5.8 8 888 8:852 in UN 8
N. 28.8 88m N 8:88.82 3m UN 8
N :8 8.. 8:88.82 .8 NVN 8

N. . 3.8 82882 8 UN 8

. 88-8 8:882 8 UN 8
. 2.8-8 88:2 8 SN 8
. $8-8 8:88 8 UN 8
. 88-8 8:88 8 UN 8
. 8.8 N 8:88 8 UN 8
- N... 8:88 8 UN 8
N. 3.8-N 88-8 8:28 8 UN 8
N 3m N Sm 8 8:888 8 UN 8
N. 3.8-N $8.8 8:28: 8 UN 8
N. 3.8 N 88 8 8:33 8 SN 8
N 3.8-N 8.8-N NN :NE8 8 UN 8
N 3.8-N . NN :NNS 8 SN 8

CM CM b- CM C‘-

N N8m.8 28.8 8988 8 SN 8
N. N88 .8. :8 m 8:88: 8 SN 8
N. N8 8 Rm 8 8:88 8 SN 8
N 88 8 88 .N. 8:83: 8 UN 8
-N 88.8 . 8:88 8 UN 8

N Sm 8 Sm 8 8888 8 SN 8
N. :8 8.88 8.8:8N8NN 8 UN 8
N. S8 8 m8 N 888 8 UN 8
N83 8.. 8:88.83 8 SN 8

N. :8 m 88 m 8:88 8 UN 8
N :8 8 88m N 88.8 8 NVN 8

N :8 m . 8:88: 8 SN 8

N. 88-8 8cm N 8:8: 8 UN 8

N. Rm 8 . 8:88 8 UN 8

N 88 N .8N88N 8 SN 8

N 88-8 888 8:88 2»... EN 208
N 888 8 . 8:88 8N8 EN Sop

N 88.8 . 888 20.8 IN 8

N... 88 m . 53.: 8N8 EN 8

N 88 8 m8 N 8888 8N8 EN 8
N 88 8 8:88 28. SN 2»...

N. 8m 8 . 8:88 28 EN 8

.N 88 m . €888 8N8 EN 8

N. 88 8 888 N 53.: 20.8 IN 8
N . . 88.8: 20.8 .8 8

N... 8:888 28 EN 8

N. . 888 N 88.88 298 EN 8

N... 8:88 8 EN 8

N . 888-N 8:88 8 SN 8

N . 888 N 888.8 8 EN 8

N . . 888 any 8.: 8

113

N 888.8 m8: 888 88 gm 8
N .888 8.. 8:88: 88 38 88

N 88 8 88.8. 8 8:88 8 3m 8
N .88 8.. 888.8: 8 3m 88

N 88 8 888 N 858 8 3m 88
N 88 .8. . 8:88 8 3m 88

-N 888.8 . 8:28.88 8 3m 88

N 888 8 88m N 8888: 8 38 88
N 888 @8818 8 am 88

N. 88 N NN :88 N8 8N8 88
81888.8 N8 88 88

N 888-N . 8:88.; 88 :m 88

N. 88 8 8:88 8 mm 8

N. 888 N 888.88 8 mm 88

N. 8:88.: 8 mm 88

- N . . 8:88 8 mm N8

N 88 N 888-N 8:88: N8 mm 88
N 88-N . 888.88 8 mm 88

N 88m: . 888.88 8 mm N8

N 888 w . NN :N8.NN 88 mm 88

N 888 N . 8:838 88 mm N8

.N . . 8:838 88 mm N8

N. 88m N NN :8888 88 mm 88

N. 888 N 8:882 88 mm 8

N . . 8:838 88 mm 8

- N ... 8:888 88 mm 88

N 888 N M88 N 88:88 88 mm 8
N 888 w . 2:88: 88 mm 8

N 888 N 8:888 88 NE 88

N 888-N .NN :88 8 «E 8

N 888-N . 8:88.88 8 mm 88

- NH 8:88.88 8 mm 88

N 888 N 88.8 N 8:8.N8N UN :8 UN

N .888 N.. 8:88.88 SN :8 88

N 888 N 8m N 8:N.88N UN :8 88

N 8 N . 888.88 UN NE 88

N .888 N.. 2:88.88 UN NE 88

N 88 N 8m 2888.88 UN NE 88

N 88 .N . 8:N.88N SN NNNN 88

N. 88 N 8:88.88 88 NE 88

N ... 8:88.88 88 NE 8

N 888. N .8888 88 NE 88

N 8m8-N 8.8.8 N 8:NN.8 NE SN NVN

N 888 .N 888 .N 8:88N NE SN UN
N 888 N 88.8 NN :8888 NE SN 3m
8 888 w . 8:88.88 :8 SN 88

N 888-N 3.8-8 8:88.; :8 N8 88
N 888 N N8m 82:88 NE UN 88
N 888HN 8.8 8:88.: :8 NVN 8
N 888 8 N88 M88882 NE SN 88
N 888 N Rm 8 8:88.88 NNNN SN 88
N 888-N 88 N 8:88.82 :8 N8 88
N .888-N..8:N8.8 NE UN 88

N 888 N 8.88 N €8.88 UN NVN SN

N 888 N 88.8 8.88 UN SN gm

8 888 w . 8.88 SN UN 88

N.888 N88 8 8.88 N8 SN 88

N. 8 N N8m 88:88.8 UN UN 88

N 888-N 88.8 $882 SN SN 88
N 888 8 N8 m 8882 SN UN 88
N 8 N N88 8 8:88.88 NVN SN 88

N 888 N 88-N 8:88.82 SN UN 88

114

£88 8 :888N SN 88 N88

N. N888 8- 8 :8888N UN 88 8E
NN8N8.8 -8 88. 88 SN 88 8E
N.88:88 88N UN 88 N88

8-8-N. NN :88. 88 88 88 8N8

N 8:88.88 85 88 NNNNN

- ... 8:88.88 86 88 N88

N. N88 8 N-N.8 8 8:88 SN 88 SN
N N88-8 . N8:N8.8NN UN 88 8.N

N N-88 8 .-8:NN.8N UN N8 38

N N88 8 .888 N N8:8N.88 UN N8 38
N N88-8 . N8:8N.8N UN 88 8.N

N N88 8wN8:N8.8NN UN 88 EN

- N New 8 . 88.88 N8 N8 38

N N88 8 88.8 N N8:NN.8N NVN 88 «E
N N88 8 . N8:8N.8N SN 88 8.N

- . 8:88.88 :8 88 gm

888 N 8:88.88 EN 88 gm

N . . 8:83 888 N8 8.N

N 88- N.NN:88 8 3m 88 am

.N. 8:3. 88 3m 88 8.N

N 888-N .N8N8N8 38 N8 888

N. 8 N 8:88 NE 8 mm

N 8.88 N ..8:88.8NN mm 8 NNNNN

N 888 N 88m N888 mm 8 N88
N 888 N .8888 85 N8 85

-N . . 888.88 mm 8 N88

N. 888 N 8:888: mm 8 N88
N. .8888 85 N8 88

N. 888-N 8:NN.88 N88 8 SN

N. 8:88.88 :5 N8 88

.N.. 888..N 8:88.88 :8 N8 88

N N88 8 8 N N8:88.8N UN 88 N8
N N88-8 . 8:88.82 NVN 85 N8

-N N88-8 . 8:888 SN 8N8 8

N N88 8 888 m 88.8 SN 85 23.
8 N88 m . 8888 UN 88 88

N N88 8 888 N 88.8 NVN 88 88
N 888-N . 8:88.88 N8 85 N8

- N 88m.N .888 N8 88 N8

N 888 N 88m 8 8:88.88 N8 88 888
N 8.88 N ..8:NN.NNN N8 8N8 88

N 888 N 888 N 8888 N8 88 88
-. .888 N8 88 8

N . 888 8 8:88.88 N8 88 88.8

-N . . 8:88.88 N8 8N8 88

N. 88m N 8:888: N8 88 88

N. 888 8 8888: N8 88 888

N . . 8888 N8 85 88

N. 888-N 8:88 N8 88 88

.N 888-m . 8:88 8N8 85 88

N 888 8 888 w 8:88 28 8E 88
N.. 888 .N NN :8888 88 8E 88

N N88 8 88m 8 8:88.88 UN 85 88
N N8H8 88.8 888.5 UN 88 8
N N88 8 888.8 8882 UN 3m 8
8 N88 .8. . 888.88 UN 28 88

N N88 8 m8 N 858 Nu 3m 88
N N88 8 6:88 SN 38 88

N 888 8 88 8 8:88.88 88 gm 8
N 888.8 888.8 888.88 88 gm 8
N 888.8 . 88.8 88 an 88

115

N ..888-N.. 8:288 NVN 88 NE

N 888-N 888-N N8NNN8.N SN 88 NE
N 888 N .8.88 N €88.88 UN 88 N88
N 888-N .N8NNNN88N SN 88 N88

N 888 N .N.8NNNN.8N UN N8 N5

N . .888 N $8.88 NE 88 NE

N. 888 N 8832 NE N8 N8N

N . . 8:88 5 88 NNNN

- N.. . NNNNNN.8 NNNN 88 NE

N 888 N 888 N NNNNNN888 NE 88 NNE
N 888 N. . NNNNo8.N8N NE 88 N8N

N 888. N . NNNNN N8 N5 88 Na

N 888-N .NN $88.8 N8N N8 N8N

N 888 N . €88.82 N88 88 NE

N. . 8888.82 N88 88 Na

8. .N8NN888 UN 88 NE

N. N88-8 NNNNNNNNN UN 88 :5

N . N88-8 8388.8 SN 88 NNNN

N . 888 N 8:88.88 3. 88 NE

N.. . 8:88.88 NVN 88 NE

N. N88-8 NNNN8N.8N NE 88 EN

N . N88-8 N8NN8N8N NE 88 NNNNN

N. 888 N 8:88.88 NE 88 NE

- N.. . 8:88.88 NE 88 an

N N88 8. N88 8. NNNNN8N88 EN 88 E
N N88 8 888 N 88828 NNNNN 88 NE
8 N88 8 . N83888: EN 88 NE

N N88 8 888 8 N8N8888NN NNN 88 NE
N N88... 8 . 88828 EN 88 NE

N 888 8 . 2:88.88 NE 88 NNNN

N. 888 N 8:88.88 8N8 N8 85

8 . . 8888.88 85 N8 an

N 888 N.. 8888.88 85 N8 mm

N. 888 N NN88.N8 888 88 88N

-N . . N8NNN.8 888 88 88N

N . 888 N 8:88.88 .25 88 888

8 . . N8NN8NN8 88N 88 85

N 8.88 N ..NNNN8NNNNN SN 88 88N

N 888 N 8.88 N N8NNN.8 SN 88 88N

N 888 .N .N8NN8NN8 as 88 85

N . 888 N NNNN88.NN 88N 88 EN

8. . 8:888 88N 88 8E

N.888 N.. N8NNNNN88 8.: 88 85

N 888-N 888-8 NNNN8N8N SN 88 8N8
N 888 N 888- N 8:88.88 SN 88 N8.N
8 888 8. N8NN888N SN 88 98

N 888 N 888 N N8NN888N UN 88 mm
N 888 8 888 N. NNNNNNN88N 8a 88 N8N
8 888 m . 888.8 85 88 mm

N 888 8 88.8 N N8N8N.8 8:8 88 mm
8 888 8 . €832 NNNN 88 mm

N 888 N 888-N €2.82 N88 88 mm
8 . 888-N N N NNN8.NN mm 88 mm

N 888 8 888.8 8:828 85 8 8E
- N 888 8. 8888.8 85 8 NE

N 888 8 888 N NNNN88.8NN 8a 8 Na
N 8.88 8 ..NNNN888NN 8B 8 NE

N 888 8 888 N 8888.8 85 8 NE
N.. 888 8 NNNNNNNN NE 8 NE

N N88 .8 N88 .8 NNNNNNNN UN 88 NVN
N N88 8 888 N $88.88 ON 88 85
N N88 8 . N8NN88.N8N SN 88 85

116

8N8.NN HumbNaonNNNNm-oéam
N88.N- .NN... £808 888 2.82

888.N 8§.bN888-8N8-uéoN.

N888 NNa.§NNN.Na§.8.8e-=§EH§N8H

No.8N. - NNa 8.N-28 888-£88-
N8N.o 88:. 528 8888 805888 E888

N . 888H8 N8888N8 88N 8N3. 88N

N . 888 8 N8888N8 88N cNuN 88N

- N. . N858 8.: 28. 88N

N. 888 .8. N8N888.8NN 88N SN; 85

N. 888 8 838.8 88N oNuN 88N

N. 888 8 NNNN8.NN EN 288 88N

N 888-8 888-8 8:88.88 IN 288. 88N

- N 888- 8 . N8N8NNNN 88N 2...; 88N

N 888 8 N88 8 N.8NN88.NNN 88N 28. 8N8

N 888 8 888 8 N8NN8.8 88N oNuN. 88N

N 888-8 888-8 NNNNN8.NN 88N 288 8.:

- N 8888 8 . N8N8N88 88N 8N3. 88N

N 888 8 888 8 N8NN88.NNN 88N 8:; 85

N 88.8 888-8-NNNNN8NN 88N NNNoN 88N

N 888-8 888 8 N8NN8.8 EN 2:. 88N

N . 888 8 .N8NNN88NN 888 28. 8N8

N . 888-8 882.88 888 8N“; 88N

- N . 888 8 €2.88 88N 288 88N

N 888-8 888-8 NNNN8N.NNN 85 288 88N

N 888 8 N88 8 N.8NN8N.NNN 85 2...; 88N

N 888 8 888 8. NNNN.8N 8.: 288 8.:

N. 888 N N8NN88.NN SN 88 UN

8. . NNNme UN N8 :8

N . 88.8. N 832.88 UN N8 :8

N . 888 N N8NNNNN88N NVN N8 NNNN

N . . €88.88 SN 88 N8.N

N. .NNNKNNNNNN SN 8 NE

117

I u.
.I. I ”..N
I... ; .I.. ... . .... ; tilt-«ti.-

N.. NNNEIHINNONNoobo01.908.88.39on
N.. unblaguoboulNBSna-NNNNon
38.88 =EINNNuNoEoOoINNNNo8NNNNINEon

vwmm

888.8-3888.885.

883838 8:. 352:.383848894898!

N888 £€IEN8NBN8INS8EINNNN§I
N.. 882=IbN8coclN88bolNExol

N..
N..
N..
N..
N..

§I8E8INS88N0INN98I
8::IoNN8-N38bolNfixol
NN88-088488834898.-

.NNNoN8IN88boINNNNon

:oNNNNNNo8oN8INS8boINNNNxo-

N.. xaEISofilNcofio§8moEINNool
N.. qNEISuNNNINcoEoB8aoNNN-NN8-
N.. 808sl8qaoNlNNNoEoB8auNNN-NN81
Adam oNBSoNNNNNoNINNNoNNNoNNN8moEINNoo-

N
NNN88NN
8.88
8.88
8.8
N8N888NNNN
NNNN8N8
N8NNNN8.8N

NI8NNNNNNI8NNNNNNN£INN8I
Snag-=8-
gum-uNwNNaINNooI
808-on5430-
EafilonaaINNool
oINNNmNNoNINNoo-
8.5882438.
alfiwaoNlNNool

.N\N-N .NNNN .N\N-8-.

.8 .N\N-N- ..N.

.N\N-N- ..N .N\N-x.

.N- .8- .8-.

.N\N+N- .N\N+N- .NNNtN.

 

 

.N. .N\N+N .8-.
.3: .N- .NNNt:
.n .8 .NN.
§xI8|8oaI>NNNNNoI8b§8I
132
N.. 2-:Iofiglqson-oonn818bog8l
N.. wfiao8l=oo|8bo§8l
.v. N . N .8 8:8 8.8.38 80388. U :5 82888. 358.8885.
888.2: N.8N.8.- .Nm. .5.
.v. N. N .8 8:8 8.8.2. 80588. U :5 88588. 12888588.
wovflm 388.7 .6. mm.
.8.. N . N .8 85 8.8.3. 82888. U :5 88388. 3888885.
mmumN aged. .om. .om.
.v.N.N.8 8:8 8.8.3. 82888. U :5 88388. 388anqu
983.8 N886 .82. .82.
8888-8888-0an888-
wNNNNNN-aoNfloNN8NN8INau8- 1888-
NaoNINNoNfioNN8NN8IN38I I828.
58308-331888-
NOE8I§I898I
Inoc—
88.NN N 8 3883-2358-5858“.-
.wahfiam Slow automz 2..ng-
ENN8 3:888 33826
N.. boNofilmNNNENomlNaoNNN—onol
N 388-8883848253-
N.. defiance-3438:080-
08.888888108348855-
NN-.NmeNN8 Bees-8888.883-

2883888882 808 BE Eu .0 885288.388

118

28:-<NN;NN=NNN<8<NN<N<8"NNN8.8+NN888-<28.
:oN88oNNNonNNoNNoNNNNon8NIoNNuBI

8:888 838-8855....Nda82-

538:8 Bean-888888.838».-

8oxNE NaogaoblaowoNNNbN-flloqwfll

Boom 80388315830818:8IEoNNNI

388:8 5888-8820818038.888..

88:8 8.55:1 8838-8038-898-
.8\N<N<8"NN+<N<oNNNuNN

22? NN88.8+<N<NN8888.8+N<N<ohNN<N<8NNNNu; oN88.
8NNSoN8IwNNNNNNwNoBI8NIoNEoNI

0N3 oanu8IwNNNNNNwNuBI8NIoéoNI

NN88 uglgglaloéal

8688 NooolNoNoéloNNNNoNE8l8NloquoN-

.NowNaN :26 RN :5 888 .N.—«N N8 8083 882884—

85 .NN no 80888 8805 88 093 8a 8.95 Sons 33088888
88 <N<..N N8 8083 8888.3N 8:080:83 No.8 8:280:08
.No 3380 85 8 896—8 8: 8N N85 .80 NNwKNoNoau
..N 8:82:28 5.. 88 N888 8N 8888838 A (Ni
.3 588295 208835 05. .<~<NN Sigma: New Son 9

8583:8430-3398:8-

N.
N.. ggoNNOoIEaNNIwNNNNNNNENooI
58538? :oN88oNNNon8NoNN8oNNNNI8NaoNI
888N NNHNoNNaaNHaNNaH
wmnm N88 388:: 8.53
8N8N 8888838889888-
N m . N £18805.anng-
8~ ngNINNENNIéBIFENvI
8N- 58- NINE-Baalgl
m quINNINNENNINNNNuoNIgNNuI
m- nNEINNINNENNIéoNIgNNVI
Nm quINNINNENNIéoNIHENNNI
mm- 58 NN NNENN 8:2 FEE

8N8; 888:88N8.>8.8é2-p§8-
8N8 N .8 88832888898882.8888-
8N88N Ease-882.58-

N .N.-N888-88N88858-8EN8-

N 858.335-3588.:88-

N Nfico-Natofiéauasflpea.

N Essa-883258-58-

119

808 ..N NE? .NN no 88888 88 .NN 8NoNoN8.N-~N 3.835250 (~58 N.. §IN8BI§INS§88I§I
no 80888 28 m E .No 882N800» 85 m3 Bfifium 828303 N.. gfloEINgaoamaoEIngl
23. 8.88882 .388 885.88 <~<NN .No 3083qu N.. I3308IE080§§EI§I
8NN888|NaNooNN8IoNN8NoNI SEN—8w NoNnfioEooaofilaoNNaNcfilgl

N.. 1538-5882827 wNNNNNNNNNNNooI .883 88.38 8:08.098. 0858-58888..ng-

N.. 8oNNNQEwIN8NNNooNoEIwNNNNNNNNNNNooI 332 gmaoNNaNNvEHgNNNH
.NNNNN 8.8.5288 NNNNNNNN 5882383 88858-5886-

NN-NmeNN8. saunas-858388888988. NNNNNN 85595 .8855 .888V
.NNNNNN 8883-3838-83-

N.. 8=8u818808NnINEO888|NEon
N.. Elk-aouooEOuINESNNaINNGNoI

885N388 88me88. 8828-2383....85838-
N.. 58382-83153881

. . 8 N. N

N N55 N88882:. N8NN888NN 882.. N8NNN N 83 8 8.8
. . 8 N. N

N N55 88888.8 N8NNNN8NNN. 88:8. N8NN8NN888 .8 88
. . 8 N.

N N Na: 88828.8 NNNNNNN: 883. N8NN888NNN. .8 N88
. . 8 N. N

N N55 N88882:. 8:822 882. 83888888 .8 N88
. . .8 N. N NNN.

N55 N8NNNNNN..N. NNNNNNNNN 88N.N- N8NN8NN888 82 N82
. . .8 N. N N8NNNNNN.

N5: N8NNNNNo.o NNNN8NNN 88N.N- N8NN8NN88.NN .8 N.8
. . N8 N. N 88.8

N5: NNNN88NNNNN N8NNN8888N. 883. 838N883 ..z 882
2.8 N. N 8:88.88

N95 8:88:88 N8NNN88888 882.. N8NN8N8NN.NN.8 8.8
. . N8 N. N NN.N.

N5: N8NNNNN88 NNNNN8NN 883. NNNNN8NNNNNN ..z 882
:8 N. N 8:82.

.5: N8NNNNN88 NNNNN8NN 88N? NNNNN8NNN8N. .8 8.8
. . 8 N.

N N N55 N8N8NNN..NN N88382: 88N.N- 888888 Na 85
:888N

88.8 NS: 58:88 8.883 882.. N8N8NNNNN. .8 8.8
. . .8 N. N 88888.8

N8: N888NN88 N8NN888N 888. N888NNNNN. .8 8E
:888N

NN.N. N55 N8NN8NNNNN N88888: 8828. 88888.8 .8 8.8
. . .8 N. N 8888.8

N55 3:886 vaonocNN 836. 33%.: mm mm

. . .8 N. N $888.8
N55 5888.8 NNNNNNNNNNN 88N? N8888NNNNN 5 NE
. . mm N. N
3.8 .883 8338ch $33ch 82.8 3522.8 Nm NNm
. . 8 N. N 88888.8
:33 535.8 98me8.8 83.8 GmeNmNd 5 NE
anonluovNaNUIoNNNNIEoNaI
83808881808586.881898-
8wa¢INNNoEoNNmNoNIoNN8IEoNaI
meloNaoloNulfioNaI
bNuNNNNNNNN§I90§8I3N8IEoNaI
gagging-898-
03-38-38-828-
>NNNN80INOIO8NIDI3N8I898I
ul8£I8N8IEoNaI
818381881888-
.NINoNNanNN8INNNoNNNI
N0E8I§I0NN8IEON8I
NonaNIoNN8I8oNal
I 902
88.8 898-388382888-
Nood .NSNNINN8ENNN8I8NI0NN82I
8:: NN.-8.8.538...8N.882.
NNNNN N..-.NN.No-.8..N.88..N-2.8..-
8: .N. .8N.988H83H8NH8..82H
mnmNd .NoN 888.8 M3 8N 9:82
88.8 awosamxmsuoéa.
vaN .o NNNN woNoau .NN-£1382-
8 8828.588 838:: 8N 382
N: gages-8.88...
$3 85.88 388:: 8N 2882

120

NINBnNIoNN8IEoNaIvaoN—IEooml

.82

.8283 .8._ wag—o2: 8:80 $858580

8.: N88: 8_ 8:80 :8 Mo 5258: 83288: oNNNENxENEa
5.. &ng8 38.88 .3 N.8N.8: 98 .35 8:3
:08: baa 28 8.80858: :3 5 8:80 c3382. 85:28.8
”8035 88.8 :5 80ng 88:88:. E 8:80 .No 338580
..N. ..N 38.2%.: .888 5.... 8.N.. o... .N.... =8 2:.
.8588 3:88.60 :3 on. was: 38.5.80 98 A828:— .8.—
025 503.3 298 .8623. 05 5 :80 2: 8388: 8:8... 5..
8=Sovl_a_uoa818ooMI

585

6:885 855 8:585 8:385 8:385 588
855 6N 8:85- 58.5 8885 8:585 8:885 508
585

6:285 585 8:85 8:885 8:885 88
585 6:88.? 855 8:85 8:385 8885 8.8
585

6:885 585 8:85 8:885 8:385 58
585 6:885- 855 8:85 8:885 8:85 8.8
585

5:85 585 8:85 8:885 8:885 88
585 8:885. 855 8:85 8:885 8:85 8.8
585

6:885. 855 8:855 8:8..85 8:8355 N08
585

8:885 585 8:85 8:885 8:285 N08
855 8:85- 855 8:85 8:85 8:85 :82
855 8:85. 585 8:85 8:85 8:85 :.8
585 6:855 585 8:85 8:885 8:85 582
855 8:855 585 8:85 8N 8885 8:85 8.8

855 8:85 855 8:85 8: 8.5 8:85 82

585 8:85 585 8:85 8: 85 8:85 8.8

585

8:855. 585 8:885 8:255 8:585 88

85.5 6:585 855 8:85 8:585 8:885 «.8

58.5 6:585 585 8:585 8:885 8:885 am

585 6:585 855 N2: 85.5 8:385 8:355 8.8

58.5 6:585 855 SN: NN55 8:255 8:255 mm

585 6:855 855 8:885 8:85 88885 NE

85.5 6:855 855 8:885 @885 8:355 :8

585 6:855 855 8:585 8: N .85 €83.55 NNmN
N~ 3 Oman“ 3% 89a

mNIDIo8EaIBN8IEoNaI

MNIDISEaIuNGIEoNaI

mmlDISEaISEIESaI

NNIDISEuIBN8IEoNaI

N NIDIO8Eanz8IEoNaI

Nona—I08NSI8N8IEQN8I

laco—

. . 8 N. N N

.55 8:885 8:58NN8.N 88.? 8:53.25 .8 588

. . 8 N.

N N N5: 8885 8:882 88N.N- 8:88.85 .8 8.8

. . 8 N. N

N NE: 8:385 8:85.85 88N5 6:8:5N5 .8 8.8

. . 8 N.

N N N55 8:885 8:885 885. 6:88:55 .8 8.8

. . 8 N.

N N 85 88:85 8:83 88N5. N8N:5N.855. 08 88

. . 8 N.

N N .5: 8:85 8:85: 88:. 6:8885 08 8.8

121

8 . 6:58.... No8 8.8
... 3m N 6:8: 888 8.8
... 38IN 8:88 538 8.8
... N88 N $88.8 3.8 8.8
8 . 8:88 888 8.8
... 888 N 8:88 888 8.8
8 . 8:83 888 8.8
... 888. N 8:83 888 8.8
... 888IN 8:8... 882 8.8
... 888 N 8:8... 882 8.8
... 888-N 88:88 8.8 8.8
... 888...: 8:8... 8.8 8.8
... 888 N 6:888 888 8.8
... . 8:888 888 8.8
... 888118888 :88 8.8
... . 6:888 888 8.8
... 8888 8:83 888 8.8
... 888 8 6:28 888 8.8
.... N 8:888 888 8.8
N.. 8N8uN 8:28 888 8.8
... 888 N 8:52. 8.8 88
8. 8:85: 888 88
... 888 _ 8:858 888 88
8. . 8:88 888 88
... :N8 8 6:858 888 88
8 . 8:88N 8.8 88
... 888nN 8:88N 888 88
... 888IN 8:8... 8.8 :m
... 888 N 8:83 8.8 .8
N . 6:: N8 888 :m
N. . 8:858 N08 .8

... 8884 8:85: N88 88
8 . 8:88 888 :m

... 888 N 8:88 888 ..Nm
.... 8:82 888 88

N 888uN 8:82. 8.8 88
... 888|N 8:8... 8.8 mm
... 888.8 6:83 8.8 88
... 888.8 8:83. 8.8 88
... 888:8 8:858 :88 mm
... 28.8 88:85.: :88 88
N 888 N 8:8.N No8 mm
N. . 583 N88 88

N.. 6:888 888 mm

... 8818 8:38 8.8 Na
... 888 8 8:2... 8.8 Na
8. 8828 N8 N8

... 888 N 8883.8 N8 N8
8 . 8:88 888 N8

... 888 N 8:88 88 N8
36:83 288 N8

... 888IN 8:8... N8 N8
... 888uN 8:8... N8 N8
... 888 N 8:88 :88 N8
... . 8:88 :88 N8

8 . 8:82 N88 :8

... 888 N 8888 N8 NE

8 . 6:8.N 888 N8
maul—nznlvaonIEOoml

NIF§8I§8INEBIEBMI

o§83133183w|

NanaleNmuao..uN.aB.888.

122

N 88.185888 N02 208
N 888. 8 $888.8 :8 208
N 888 88388.8 N82 208
N 888. N 6888.8 88 N08
N 888 .N @8818 882 N08
N 8888 NNNNNNN «5 808
N 8%-N NNNNNNN :8 N08
N 888. N $22.8 88 808
N 888 .N €N8NN 802 808
N 888. N $32.8 8.8 808
N 888 ..N 382.8 802 808
N 38. N $32.8 8.8 808
N 3.8 N 382.8 802 808
N 33 €2.08 88 N08
N 381.2338 882 N08
N 38.8 588.8 mm N08
N $8.8 2:888 88 N08
N 28.8 688.8 mm N08
N 28.8 6888.8 88 N08
N 8888 NNNNNNN :8 N08
N $8IN NNNNNNN :8 N08
N 888. 8 $82.8 8.8 808
N 888185883 882 808
N 888 18:882.». 802 808
N 888.8 582.8 888 808
N 888. 8 $88.8 N8 808
N 888 :8 $28.8 N82 808
N 8N8: 8 388.8 N8 808
N 8N8 :8 $88.8 N02 808
N NN8I8 @883 am 808
N 8.08 N NNNN88.N 8a 808

N 888..N N8NNNN.N 8.8 «08
N 888 IN GNNNNN 882 .08
N 888 N NNN8N8N NE .08
N 888.: $5.8 8.8 808
N 83. nN NNVNNNNNN 802 808
N 888uN 5888.8 86 808
N 888 N 5888.8 38 N08
N 80 5888.8 :8 N08
N 8888 5882 :8 N08
N 888 N 5883 :8 N08
N 8884 @828 NE N08
N 8N8u8 @8888 N08 N08
N 83.8 @8888 N82 N08
N 888IN NNNNNNN mm N08
N 8884 NNNNNNN 88 N08
N 888:8 $82.8 N5 :8
N 8888 $83.8 NE :8
N 888.8 6883 88 N8
N 88.8 5883 mm N08
N 888.8 582... 88 8.8
N 888.8 5883. mm NN8
N 888 8 @8888 N08 NN8
N 888183888 208 2.8
N 888 m $88.8 208 :8
N 888183888 808 28
N 888 8 $28.8 808 N8
N . N8NN8.N 808 N8

N 888..N NNNNVNN. 802 88
N 888.-N 53... 88 8.8
N 888: N GEN... 88 8.8
N 888 N 63.3 882 88

123

N 888-88 NN NN88 N08 mm 808

N 3.8 8 888 N 53.88 N08 mm N08
N :8 m . 5888.8: N08 mm N08

N 28.8 . NN NN88 N08 85 808

N 888p .NNNN88NN N08 mm N08

N 888 N .8388: N08 mm 808

u N US$88.88 N08 mm 808

N 8N8 8 888. 8 N8N88.N8 N8 NE N8
8 8N8 m . @838 N8 N88 N08

N 8N8 8 8% N 58.8 N8 N5 N08
N 88818 . NN NNN8.NNN N8 N5 «08

N 8N8 8 8884 $2.88 N8 N5 «08
N 8N8 m . €88.88 :8 NE 208

8 888 m . 58.8 N8 N5 N08

N 888 8 888 N 5838 N8 N5 N08
I N 888 8 . €2.88 :8 N5 808

N 888 8 888m NN NNN8.N8N :8 NE 808
N 888 m . €88.88 N8 NE 208

N. 888 N SNNNNNNN N08 NNm N08

N ... €83: N08 NE 808

N. 888 N 85.88 N08 NE 808

N ... 8388.3 N08 NE 208

IN 8888 . €2.88 N08 NE 808

N 888 N £8 N 583: N08 NNm N008
N 888 N1. 8388.3 N08 NE 208

N . 888 N 8:838 N008 NE 808

8. . 8388.8 808 NE 208

N 888 N .ISNNNNNNN 808 NE 208

N 888; 8881283883 :8 NE N8
N 888 N 888..N €88.82 :8 NE N08
N 888 N 4838.3. :8 :8 N08

-N 20 .N8NNN.3. :8 :8 N08

N 888 N 888 N @8862 :8 :8 N08
1 N 88.8 N 8.8 :8 NE 808

N 888 N 888 N 638.3. :8 :8 N08
N 888; 4858.82 :8 NE N08

N 888 N.. €88.82 :8 NE N08

N 888: 888 N €3.30 :8 NE N08
N 888w .2382 :8 NE 808

N 888 N . NNNNSNN N08 :8 N08

N 888 N . NNNNNENN N08 NNm N08

N 888..N 8884 $88.88 N08 NNm N08
N 888 N .NN NNN8.NN N08 NE 808

-N . . €88.88 N08 NNm N08

N . 888 N NNNNNEN N08 :8 N08

N. . 23%.? N08 NE 808

N. 88 IN 3:88.; N08 :8 N08

N. . 8:88.88 N08 :8 808

N 888 N .NN 388.88 N08 NE 808
maul—nsnlonanEooml
mIFoEEz8IoNN8Ion§IEoowI
NIF§8ISN8Ion§IEo8wI
onnaIEooml
m..Ncan—ISBIESNNJESIEOowI
N..—ops—IoNN8IESanquaIEOomI
NINBNN—IoNfiIESan—maalfioomu
I noo—

N 888..N $83.8 88 208

N 888 N $3.8 802 208

N. a A¢va~d cum 20m

N..:N AEnvwd 082 Sum

N 8N8 8 $88.8 N08 208

124

NI. . NN 588.3 N08 85 808

N. 888 N NN 88.3 N08 85 808

8 NN8 m. NN NNNNNNN 808 85 808

N NN8 8 888IN NN NNNNNNN 808 85 808
N . 888 N NNNN8N8N 808 85 808

N 888IN 888IN @883 28 3m :8
N I888 N 8.88 :8 am 808

IN 888IN . 8: N88 :8 in N08

N 888 N 888 N 688.3 :8 3m N08
N I888 N .N8NNN88N :8 :m 808

N 888 N 888IN 88838 :8 am 808
N 888IN 8.8 $8 am 808

N 8.8 N 8.8 :8 am 808

N I888IN . €88.82 :8 38 N08

N 888 N 8884 N8: N88 38 N05 N08
N 888 N .N8NNN8N. :8 28 N08

N 8.08IN 888IN @NENN :8 :m 808
N 8.08 N 8.8 :8 :m 8.08

NI. . 8N: N88 808 «5 N08

N. 888 N 8N: N88 808 28 N08

NI. . 8:88.; 808 :m 808

N. 888 N 8:88.; 808 :m 808

N .I. NN NNNENN 808 vi 808

N . 888 N NN 38:8 N08 38 N08

N. .INNNNN88NN N08 am 808

N . 888 N €88.88 N08 38 N08

NI. . NN $88.88 N08 am 808

I N 888 N . €88.88 N08 «5 808

N 8N8 N 888 N 2:888: N08 «5 808
N 888I8 . NN 388.88 N08 am 808

N . 888 N 2:988 808 am 808

8. . 2 388.3 808 am 808

IN 888 IN . NN 388.3 808 «E 808

N 888 8 8N8 8 €88.88N 88 mm 88
N 888 8 888 m NN.:NNNNN 8.8 mm N08
N 888IN 8N8I8 $8.88 8.8 mm NN8

N 88.8. N N88 8 N829. 88 85 N08

N 888IN $8I8 358.82 8.8 mm N08
N 888 N 888IN 35.82 8.8 85 N08
N 888 N 48:88.. 88 mm N08

N 888 3268.8 8.8 mm 808

N 888..N 88m 8 €8.88 88 mm :8

N 8¢8IN 8N8I8 ENSNN 8.8 mm 2.8
N 8.08 8 N88 8 858.82 88 85 N08
N 888 N N88I8 €2.88 88 mm N08

N 8¢8IN 888 N 6:88.. 88 mm N08

N 888 N 4888.82 8.8 mm N08

N I888IN 8:58.88 88 mm 808

N 888 8 888 8 N8NN8.N8 :8 mm NN8

N 888 8888 8INN 9.8.82 N88 85 N08
N 888I8 Nv8I8 €88.88 t8 mm N08

N 888 8 8.08 N @885. :8 mm N08

N 888I8 . 52.3 NN8 mm N08

8 888 m . €88.88 t8 mm 808

N 888 8 N88 8 888.88 NN8 mm N08

N 8N8 8888 8INN $3.82 8.8 mm N08
N 8N8 8 888 N 52.3 NN8 mm N08

N 8N8I8 . 68:8 :8 mm N08

I N 8N8I8 . €88.88 NN8 mm 808

N N.8.8. 8 Sm 8 NNNNNNNNNN N08 85 N08
N N88 8 888 8 $388.8: N08 mm N08
N N88 8 . €88.88 N08 mm N08

125

N 8v8IIN 888IIN. 688.2. 882 888 808
N 888IN 888IN NNNNNNNNN 88 88 8.8

N 888 N 888 N 5838 8.8 888 808
8 888 8 . €8N8NN 888 808 808

N 888 N 888 N N838? 88 88 N08
I NI888 N . 8.88 88 88 808

N 888 8 888 8 688.3 8.8 88 808
N 888 N 88I8 8 $885. 88 88 808
IN 888 IN N681: 8.8 888 808

N 888IN 888IN EN8N8N 88 88 808
N 888 N 888IN €8N8NN 8.8 8.8 808
N 888 N .6838 88 8.8 808

N 8N8 N 8N8 N 8.88 88 88 N08

N 888INI. 588.88 88 88 808

N 888IN 8N8 8 688.: 8.8 8.8 808
N 888 N 88..8 8 €88.NNN 888 88 808
N 888 N 8 EN8.N8N 88 88 808

N 8.8 N 888 N 68:8 88 888 808
8 888 8 . $98.2 808 88 808

N 888 N 888 N 8888.5 808 88 N08
IN 888IN . AN :88? 808 8.8 808

N 888 8 888 m N83888: 808 888 808
N 888 N 88I8 8 AN $3.8 808 8.8 808
IN 888 IN N sNNN888 808 88 808

N 888 N 888 8 NNNNNSNNN 808 88 808
N . 888 N 688.5 N08 88 N08

NI: 29.8.2 808 888 808

N. 888 8 2:838 808 8.8 808

N . 888 8 3:888: N08 88 808

N . 8 NNNNNNNNNN N08 88 808

N. 888 N SNNNN88 808 8.8 808

N I888INI. 6:88.82 N08 88 N08

N 888IN 888I8 NNNxNN8N N08 88 808
N 888 N 88I8 8 NNNNNNN8N N08 88 808
NI888 NI N NNNNN88N N08 888 808

N 8.8 N 888 N 5:3: N08 88 808
N . 888I8 NNNNNNNNNN 808 888 808

N . 888 8 NNNNNNNNNN 808 88 808

N .IN 232.88 808 888 808

8 . 888IN NN 32.88 N08 88 808

N 888 8 8I88 8 $988.88 808 8.8 808
N 888 8 N INNNNNN88N 808 88 808

N 888 8 88.8 N €88.88 808 8.8 808
I N 888I 8 N $88.88 808 88 808

N 888 8 8N8 8 NNNNN8.88N 808 88 808
N N 888IN 8:388 808 8.8 808

8 8N8 8 . €88.88 :8 8a 808

N 888 N 888 N NNNNNNNN. :8 85 808
IN 888IN . 383.88 $8 86 808

N 8N8 N NN8I8 ENNNNN :8 85 808
I N 888 N 48888.88 :8 8a 808

N 8N8 N 888 IN 8:882 28 85 808
N. 888 N 55.88 808 85 808

NI: 8:828 808 85 808

N. NN8 8 6:88.; 808 8a 808

N . 88:88.8: 808 85 808

N. 888 N 58.88 808 8a 808

8 8.08 8 . 8388.5 808 85 808

N 888 N NN8I8 8388.3 808 8a 808
N 888 N 4.88.88 N08 85 808

N 888IN 888IN 8:888: 808 85 808
N . NN8I8 NNNN8N8NN 808 8a 808

126

N 888IN SMIN GNNNNN. 88 88 208
N 8.8 N N88 8 @582 8.8 8.8 28
IN 888IN . 6888.3 888 888 808

N 8N8 N 888 N €3.82 88 88 808
N I8N.8 NI. N8N8NN8N 8.8 88 808

N 888 N 888 NIGNNNNNN. 8.8 88 808

8 888 8 . 8.8 802 88 N08

IN 888IN 3.8 N 8.8 882 88 808

N 888 8 3.8 8 N858: 802 8.8 208
N 888 N 888 N 682.88 882 88 208
N I888 NI. 683.82 882 8.8 808

N 888 N 888 N €88.88 802 88 808
IN 888IN . N8NNN8NV 802 88 808

N 888 N 8v8I N @822 882 888 808
N . $.8IN NN.:NNNNN N08 888 808

N . $.8IN NNNN8.N.8N N08 88 208

N . 888 N 63.5 N08 88 208

NI. . NN NN8N.8N N08 888 808

N. 888 N NN NN8N.8N N08 88 808

NI. . 8:88.8N N08 888 808

IN. 888 N 8:88.? N08 88 808

N 3.8IN 3.8IN AN :3? 808 8.8 208
N 3.8 N N.88IN NN NNNNNN 808 8.8 208
8 3.8 8 . $88.82 808 8.8 808

N 38 N 888 N 588.82 808 8.8 808
8 3.8 8 . 8:88.88 808 88 808

N 888 N 88.8 N 8:88.88 N08 88 808
N 3.8 N 888IN 2:828 208 8.8 208
IN 3.8IN . 8:388 208 88 808

N 38 N 888 N $38.8: 208 8.8 808
N $8IN . N8NN8N8: 808 888 808

N 3.8IN 888IN €3.88 208 8.8 808
N 8.88 NI. $38.8: S08 88 808

N 888 N 888IN sNNNN.88 208 88 808
I N NN88 N . 53.88 208 88 808

N 888 N 888 N 88:82: 208 888 808
N. 888 N 88:88.; 808 88 808

N. .88NN88.N8N 808 88 808

N. 888 N 888.8 808 8.8 808

I N 888 N .8888 808 88 808

N 888 N 888 8 N8NN88.N8N 808 8.8 808
8.. 888 IN 5:888 808 888 808

N 888 N 8.8 N 58.83 882 8.8 882
N 888IN 888HN 588.8 802 88 88
N 888IN 888IN NNNNNNNNN 882 88 888
N 888IN 888 N 6838 802 8.8 808
8 888 8 . €8N8NN 882 88 808

N 888 N 8.8 N £68.88 802 88 N08
I NI888 N.8.88Nz888808

N 888 8 888 8 E83: 802 88 808
N 888 N 88.8 8 588.: 882 8.8 808
..N 888 IN N 68:8 802 88 808

N 888 NI 8N8 8€N8N8N 882 88 808
N 888IN 888IN NNdeNN 882 8.8 88
N 8N.I8 N 888 N 588.8 882 8.8 8.8
N 8% N 888 N €8N8NN 802 888 808
N 888IN . @838 882 88 808

N 8%IN 888 N 8.88 802 88 N08

N ..888 NI. 288.88 802 88 808

N 888 N 888 8 $88.: 802 8.8 808
N 888IN 888I8 588.3 802 888 808
N 888IN N €N8N8N 8.2 8.8 808

127

N 888I8 888I8 588.9. 88 :8 808

N 888 8 . IN N NN88.NNN 8.8 $8 808

N 888I8 888I8 3:38 mm $8 88

N 888I8 888I8 3:38 mm :8 mm

N 888 8 888 8 $8.88 mm 28 N08

N 888 8 888 8 8:88.88 mm N8 208
N 888 8I8N.8 8 88:88.82 mm $8 208
N 888 m 888 8 @8838 mm 28 808

N 888 8 888 8 $88.88 mm N88 808

N 888. 8 . 683.2 mm :8 808

N 88.8.. 8 888 8 58.8 88 28 mm

N 8.8 8 888 8 $8.88 88 N8 N08

N 83 m 888 w 8988.82 88 N8 208
N 888 8 .888 8 88:88.88 88 28 208
N 888 8 838 8 688.9. 88 N8 808

N 888 8 888 8 NNNNNNNN 88 $8 808

N 88.8 8 .INNNN8NNNNN 808 $8 808

N 888 8 888 8 £8.88 mm :8 N08

N 888 m 888 w 838.82 mm $8 208
N 888 8I8N.8 8 88:88.88 mm N88 208
N 888. 8 888 8 588.9. NE N8 808

N 888 8 888 8 $388.5 mm $8 808

8 888 m . NN 388.5 mm $8 808

N 888I8 888I8 €888.88 N08 N8 208
N 888 m 888 8 $388.88 N08 N8 208
N 888I8 888I8 €888.88 N08 :8 808

N 888 8 888 8 $388.88 N08 :8 808
IN 888I8 . 8:888: N08 28 808

N 888 8838 8 8832.88 208 $8 208
N 888I8 888I8 $8.82 208 N8 808

N 888 8 888 8 €8.88 208 $8 808

N I888I8I. $588.5 208 :8 808

N 888I8 888I8 8:888 208 28 808
N 888 8 888 8 58.8: 208 2.8 808
N I83 8I. $388.3 208 28 808

N 888 8 888IN 8 53.88 808 N8 808
N 888% . $588.88 808 $8 808
NI888 8I. $388.88 808 $8 808

N 888IN 888IN NNNNNNNNN 882 8.8 88
N 8N8I N 8N8I N $38.8 882 88 8.8
N 888 N 888 N 68.82 882 888 882
8 888 8 . 8.8 882 888 N08

8888 838 N 8.8 882 88 38

N 888 N am N $2.88 882 8.8 208
N 888IN 8.88 8 65.82 882 8.8 208
IN 888IN . 6888.9. 882 88 808

N 888 N 888 N €3.82 82 8.8 808
N I888 NI. 6852 882 8.8 808

N 888 IN 888 IN N8NNN.8N. 802 8.8 808
N 888I N 888I N NNNNNNNNN 88 8.8 888

N 888 N 888 N 8388.8 8.8 8.8 882
8 888 8. 8.88 8.8 8.8 N08

IN 888IN 3.8 N 8.88 88 8.8 808

N 888 8 38 8 3:882 88 88 208
N 888 N «88 N GNNNNN. 8.8 8.8 208
N I888 N... N8§NNNNN 88 8.8 808

N 888 N 888 N 6888.88 8.8 8.8 808
IN 888IN . GNNNNNN. 8.8 8.8 808

N 888 IN 888 IN @852 8.8 8.8 808
N 888 N 888 N NINNNNSN 88 8.8 802
8 888 8. 8.8 8.8 8.8 N08

N 888 N 3.8 3.8282838

128

N. 88:88.8: Em N08 :8

N. 888IN €2.88 38 N08 :5

NI. 888 8 85.8 :8 N08 :8

N 888 N 888 N 58.8 38 N08 :8

I N 888 N . 63.8 :8 N08 :8

N 888IN 888IN N83888: «5 N08 NE
N 888 N 888 8 N83888: Em N08 :8
I N 888 N .N8NNNNNN :8 N08 an

N 888IN 888IN N83888: :8 N08 :8
N 888 N 888 IN N83888: :8 N08 NN8
N. 888IN £388.; :8 N08 :8

N .I888 N 8388.; Na N08 NN8

N 888 N 88.8 N 58.8 :8 N08 :8

N. 888IN 83588 NE N08 NNm

N. 8N8I 8 NN NN8N.N8 NNm N08 NN8

N. 8N8I 8 NNNN8N.N8 NNm N08 N82

N. 888IN NN.:8N88N NNm N08 an

N. 888 N NN.:8NN8N 3 N08 88

I 8. . 65.8 NS N08 mm

N 888I N 8N8I 8 NN NN8N.N8 NNm N08 NN8
N 888 NI 8N8 8INN NN8N.N8 NNm N08 N02
N 888IN 888IN N8: N.NN NNm N08 8N8

N 888 N 888 N N8NNN.NN NNm N08 88

N 888 N .INEN8N88N NNm N08 mm

N 8N8I 8 8N8I 8 8:88 N88 N08 N82
N 8N8I8 888IN NN NNNNNN :8 N08 mm
N 8N8 8 888 N NNNNNNNNN t8 N08 88
IN 8N8 I8 . NNNNNNNN t8 N08 an

N 8N8I8 888IN NN NNNNNN N82 N08 mm
N 8N8 8 888 N NN NNNNNN N82 N08 88
N 8N8 8 . NNNNNNNNN N82 N08 mm

N 888IN 888IN £88 98 N08 88

N 888IN . NNNN88.NN 8N8 N08 mm

N I888 NI.NNNN88.N8 88 N08 mm

N 888I8 888I8 @828 NE N8 N5

N 888I8 888I8 €388 NE 28 8.8

N 8888 8 888 8 €3.88 NE :8 an

N 888I8 888I8 8:88.88 NE :8 8.8
N 888 8. 888 8 8388.3 NE $8 an
N 888 8 888 8 35.8.. NE N8 N08

N 888 8 88m 8 5838 NE N8 208
N 888I8 888I8 NNNxNNNN NE N8 208
N 888 m 888 8 3:88.82 Na :8 808
N 888 8 888 8 8:88.88 NE N8 808
N 888 8MNNNN§NNN NE N8 808

N 888I8 888I8 8:88.88 NE N8 88
N 888 m 888 8 8:88.28 NE 28 85
N 888I8 888I8 €2.88 NE $8 8.8

N 888I8 888IN. €3.88 NE N8 mi

N 888 8 888 8 $88.88 NE :8 N08

N 888 m 888 m NNNNNNNNN NE N8 208
N 888I8 888I8 @838 NE N8 208
N 888 8 888 8 8:88.88 NE N8 808
N 888 8 888 8 3:88.82 NE :8 808
N 888. 8 . N8NN8NNNN NE :8 808

N 8888 8 888 8 38.8 8.8 :8 mm

N 888I8 888I8 3:38 88 :8 8.8

N 888I8 888I8 N8NN8N8 88 :8 mm

N 888 8 888 8 $8.88 888 $8 N08

N 888 8 888 8 838.88 88 N8 208
N 888 8888 8 8838.82 88 N8 208
N 888 8 888 8 2:838 88 :8 808

129

N 888II8 8N8II8 3:88.82 82 808 $8
N 888 8 8N8I 8 8:88.82 82 808 N82
N 888 8 .INNNNNN.8NNN 882 808 mm

N 888I 8 888I 8 838.8 888 808 :8
N 888I 8 888I 8 898.88 8.8 808 N82
N 888I 8 8N8I 8 8:88.82 88 808 28
N 888 8 8N8I 8 3:88.82 8.8 808 N82
N 888 8 .IN8NNNN88N 8.8 808 mm

N 888.. 8 888I 8 NNNNSNN :8 808 :2

N 888I 8 8N8I 8 NNNN8N88 :8 808 N..8
N 888 8 8N8I 8 NNNN8NN8 N88 808 N82
8 888 I8 . NNNNN8.NN N8 808 an

N 888I 8 8N8I 8 NNNN8NN8 N82 808 $8
N 888 8 8N8I 8 E858 N82 808 N82
N 88I8 8 . N8NNN8.NN N82 808 mm

N 8N8 8I8N8 8 NNNNNNN :8 808 N82

N 8N8 8 . NNNNN8.NN :8 808 mm

N 8N8II8 . NNNNN8.NN N82 808 8.8

N . NN8 8 N8NNNN.N8N N8 808 85

.I. . NN NNN8.NNNN $8 808 85

N. 888IN NN NNN8.NNNN :8 808 85

8 NN8 m . NN 3838 85 808 85

N NN8 8 888IN NN 33.88 8.8 808 85
N. 888IN NNNN8N.8N 8N8 808 85

N 888I N 2:88.88 8.8 808 8.8

N . 888 N 88:88.88 8.8 808 882

N. .NNNN8N88 8.8 808 8a

NI. ..N8N8N NNN 88 808 NE

NI. 888888IN NN.8N8N NNN 8.8 808 NE

N 888N I N.NNNNNNNNNN8.8 808882

. . 8NN8NN88.88N 8.8 808 8a

8 888I8 . NNNNN8N.8N 8.8 808 NE

N 88.8N 8N 8:838 8.8 808 NE
88I8888 N..N8NN88 88N 882 808 8a

88 888 N.NNNNN8N. 88 882 808 NE

N 888 N8 N NNNNN8N 88 882 808 NE
N..NNNNN8NN. N8 8Nm 808 NE

N. 888I N NNNNN8NN N8 8.8 808 an

N. 888IIN N388. N8 N5 808 NE

N.. 888I N NNNN88.N8 8.8 808 8.8

N. 8I88 N N388 N8 88 808 882
N..IN8NNN8. N2 88 808 85

N. 888 N €858 8.8 808 85

I N . .INNNNN8.NNNN 8.8 808 8N8

N 888 N 888I N NN NN88 8.8 808 882
I N 888 N .NNN8N.NN 8.8 N08 85

N 888 N 888 N N8NNN8N8N 8.8 808 83
N 888 N .NNNNN8.NNNN 8.8 808 8N8

I N 888IN . 685.8 882 808 8N8

N 888 N 888 N N8NNN8.N8N 882 808 8N8
N 888 N .INNNNN8.NNNN 882 808 85

N. 888 N NNNNNN.88 8N8 808 85

8 . . 8:88.88 85 808 85

N 888 N . 8:88.88 85 808 8N8

NI. . NN NN8N.NN 8.8 N08 8N8

888IN NN NN8N.NN 8.8 N08 86

888 N NN NN8N.NN 8.8 N08 8.8

NI. . NN NN88.NN 88 N08 NNm

N. 888IN NNNN88.NN 88 N08 :8

N. 888IN NNNN88.NN8N8 N08 :8

N . 888IN NN 38:8 85 N08 85

N . 888 N NN 382.8 8NN. N08 8.8

130

N 888IN 888IIN N8NN8N.88 8.8 808 882
IN 888 IN. NNNNNNNN 8.8 808 28

N 888I N 888I N N8NN8N.88 882 808 8.8
N 888 N 888.. N N8NN8N.88 802 808 882
N I888 NI.NNNNNNNN 882 808 :8

N 888 N 88I8 N NNNNNNNNNN 8.8 808 882
N 888I N. NNNNNNNN 8.8 808 :8

N 88.8 N .INNNNNNNN 882 808 :8

N 88I8 N 88I8 N N888 88 N08 882

N 888IN N88I8 NN NNNNNNN 8.8 N08 mm
N 888IN N88I8 N N NNN NNNN 88 N08 8.8
N 888IN N88I8 NN NNN N88 88 N08 mm
N 888IN N88I8 NN NNN N88 8.8 N08 88
N 888IN 888 N NN 388.88 88 N08 :8
N 888 N 888IN NN 388.88 88 N08 :8
IN 888 IN . NN 388.88 88 N08 :8

N 888IN N88I8 NN NNN N88 882 N08 85
N 888IN N88 8 NN NNN N88 882 N08 8.8
N 888IN N88H8 NN NNN N88 882 N08 mm
N 888IN N88I8 NN NNN N88 882 N08 8.8
N 888IN 888IN NN 388.88 882 N08 5
N 888 N 88.8. N NN 388.88 882 N08 :8
N 888 N . NN $88.88 882 N08 :8

N N.8.8 8 N88I8 588 mm N08 8.8

N N88I8 N88I8 NNNNNN8N8 mm N08 mm
N N88 8 N88 8 NNNNNN8.N8 888 N08 8.8
N N88I8 888IN N8NN88.NNN mm N08 :8
N N88 8 888 8 N8NN88.NNN 85 N08 NN8
IN N88I8 . 6888.8 mm N08 :8

N N88I8 N88I8 NNNN88.N8 8.8 N08 mm
N N88 8 N88 8 NNNNNN8.N8 88 N08 8.8

N 888 888HN N8NN88.NNN 8.8 N08 :8
N N88 8 888 8 N8NN88.NNN 8.8 N08 :8
N IN88 8I. 688.8 8.8 N08 :8
N N88 8 N88 8 38.8 85 N08 8.8
N N88I8 888IN 688.8 mm N08 NNm
N N88 8 888 N 688.8 mm N08 :8
N NI88 8 .IN8NN88.NNN mm N08 :8
N N88I8 888IN 6888.8 8.8 N08 :8
N N88 8 888 N 888.88 8.8 N08 :8
N N8I8 8 . N83888: 8.8 N08 NNm
N 888 N 888 N N888 :8 N08 :8
N 888IN .NNNNNNNNNN NE N88 :8
N 888 N . NINNNNNNNNNN :8 N08 NNm
N 888 8 888 8 NNNNNNN 8.8 808 882
N 888II8 888II8 8:88.88 88 808 882
N 888 8 88m 8 8:88.88 8.8 808 8.8
N 888I 8 888I 8 3:88.82 8.8 808 N8
N 888 8 888 8INNNN8888N 8.8 808 2.2
N 888II8 8N8I 8 838.8 8.8 808 N8
N 888 8 8NI8 8 828.88 8.8 808 N82
8 888 m . NNNNNNNNNN 8.8 808 mm
N 888 I8 888 I8 8:88.88 82 808 882
N 888 8 88.8. 8 8:88.88 82 808 8.8
N 888II8 888I 8 8:88.82 82 808 N8
N 888 8I888 8INNNN8888N 882 808 N82
N 888I 8 8N8I 8NNNNNNN8.8 882 808 Cm
N 888 8 8N8 8 NNNNN8.
N 888.8 . N88NNNN .NNNNNNw 88”” 80m 882
N 888 8 888 8 NNNNNNN 82 W88 mm
N 888 8 888 8 NNNNNN8.NNN 802 808 8.8

N 888I8 888I8 8:38 802 808 NW.”

131

N NIN NN NN88 8.8 208 882

N N 8N8I 8 688.88 8.8 208 N8

N N 8N..8 8 €88.88 8N8 8N08 :2

N N 888I 8 NNNN88.N8N 8.8 208 $8

N N 888 8 NNNN88.N8N 8.8 208 N82

N NI. NNNN8N.NN 8.8 208 NE

N N 8N8I 8 €88.88 882 208 28

N N 8NI8 8 $88.88 882 28 N82

N N 888I 8 NNNN88.N8N 882 208 N8

N N 888 8 NNNN88.N8N 882 208 N82
IN N . N8NN8N.NN 882 208 NE

N 888 8 8IN8 8 NNNNNNN N8 208 N82

N 8N8. 8 888I 8 333.8 :8 208 N8
N 8N8 8 888I 8 N8NNNN.88 $8 208 N82
IN 8N8 I8 . N8NNN8.NN N8 208 N5

N 8N8I 8 888I 8 N8NNNN.88 N82 208 $8
N 8N8 8 888I 8 N8NNNN88 N82 208 2.2
N 88 8I.N8NNN8.NN N82 208 NE

N 888 8 88I8 8 NNNNoNNNN NN8 8N08 :2
N 888I 8 . N8NNN8.NN :8 208 NE

N 888 8I. N8NNN8N.NN N82 208 NNNN

N 888IN 888 N 8.8 8.8 808 882

N 888 N .N8NNN8.8N 8.8 808 8.8

N 888IN .NN NNNN.8NN 8.8 808 85

N 8I88 N .IN8NN8N.88N 8.8 N08 85

N 888IN 888IN 8888.88 8.8 N08 85

N 888 N 8I88 N $88.88 8.8 808 8.8

N 888 N .N8NNN88N 882 808 8.8

N 888IN .NN NNNN.8NN 882 808 85

N 8I88 N .IN8NN8N.88N 882 808 85

N 888 N 888 N $88.88 882 N08 8N8

N 888IN 888IN N8N88.88 882 808 8.8
N . . NN NNNN.8NN 8.8 808 85

IN . . €88.88 8.8 808 8N8

N. 888IN N8NN8N.88N 8.8 808 85

N . 888 N N8NN8N.88N 8.8 808 8.8

NI. . NN 38.88 85 N08 85

. 888IN NN N588 888 808 85
. 888IN NN 98.88 85 808 8.8
. 888 N NNNNN8.NN 8N8 N08 85
.I888ININNNNN888 8N8 808 8.8
N 888 N 88.8 N N388 85 808 8.8

N . 888I N NNNNN888 8.8 808 8.8

N . 888I N NNNNN888 8.8 808 802

N. 888I N N8NNNN.N8N 8.8 808 8.8

N . 888 N NI8NNNN.N8N 8.8 808 882

N . 888I N NNNNNNN 8.8 808 8.8

N. 888 N NNNNNNN 8.8 808 882

I N. .INNNNN8.NNNN 8.8 888 NE

N 888 IN 888 ..N 338.8 8.8 808 882

N 888.. N 888I N $88.8 8.8 808 8.8

N 88I8 N 88I8 N NNNNNNN 8.8 808 882

N 888I N 888I N N8NNNN88N 8.8 808 8.8
N 888 N 888I N N8NNNNN8N 8.8 808 882
N 888 N .INNNNN8.NNNN 8.8 808 :8

N 888I N 888I N NNNNNNN 882 808 8.8

N 88I8 N 88I8 N NNNNNNN 882 808 882

N 888I N 888.. N N8NNNN88N 882 808 8.8
N 888 N 888I N N8NNNN88N 882 808 802
N 8I88 N .INNNNN8.NNNN 882 808 NE

N 888I N 888I N NNNNSNN 8.8 808 802

N 888 N 888 N N8NN8N.88 8.8 808 8.8

c» c~~ c» c~~

132

N NN.N aEIbN808INNN8I0=80NI

888.8- ..NEINNNS08INNN8I0880NI

82.8 8§I8N8808I8N8I0882I

888.8 NEI80NNNI808088I8058808I£N8I

8N .8NI I NNaI880eI8NN0NHpEN8H
wwod use 805 85880888 00.58% FEM—u

N 888IN 888IN N N NN88 8.8 208 882

N 888I N N NNNN8N.N8 8.8 208 8.8

8 888 8 N NNNN8N.N8 8.8 208 882

N 888I N 8N8I 8 NNNN88.N8N 8.8 208 :8

N 888 N 8N8 8 NINNN88.N8N 8.8 208 N82

N 888I N 888I 8 $88.88 8.8 208 N..8

N 888 N 88I8 8 €88.88 8.8 208 N82

N 888 N . NNNN8N.NN 8.8 208 NE

N 888I N N NNNN8N.N8 882 208 8.8

8 888 8 N NNNN8N.N8 882 208 882

N 888I N 8N8I 8 NNNN88.N8N 882 208 N8

N 888 N 8N8 8 NINNN88.N8N 882 208 N82

N 888 N 888 8 $88.88 882 208 28

N 888IN 88I8I8 858.8... 882 208 2.2

N 888 N . NNNN8N88 882 208 NE

133

N.. 8NN80NNI88oooaINEo8NNaINNN8qu

N.. stNIHINNoNNooNNSINESNNNNINNNNon

N.. :NEIHINNONNoohcoINEoBaINEon

N.. emblaONNoobOolNEofialNaxol
NINwNmN. =EINNNoNoNI¢oOoINNNNo8NN8|NNNNon

ONoN

88IhNINsmb0INaN0I

88858888 8:. 36.881988848830489on
83.8 £€IEN85NNINS8E°INNNN§I
N.. 8auEIbN8NNoN81N8N§IN§SI

N..
N..
N..
N..
N..

:NNNNIoNN8INfl8boINN8NNNoI
NNNEIoNN8IN88boINEon
NNN.NEIQNN8INS8boINNNNon

BoNoolNflsolNNNNxol

couato8oN8IN58holNaxul

N.. anISoNNNINaoEoBNNaoNNNINNooI
N.. :NNNNISoNNNINNNoNNNoBSuNNNINNooI
N.. N888=I8NN8NoNINNNoEoB8aoEINN8I
vamam oaflogoNIEoEoSSoEINNool

8
N8NNN.NN8N
8.88
$888.82
8.8
NNNN888.NN
NNNNNNN.
NN 528.:

NIaasINNNEeINNaI
§No>INNooI
gawlonaalNNool
SonlonqalNNool
«NNNNNalonNNaINNooI
olfiwaoNINNool
NI.N.880NINN00I
alfiwNBNINNooI

.8 NNN-N- ....

.N- ..N- .88..

.Nl NN\—+NA 8XI.

.N ..N ..N.

Nxxl88|8oNNI>NNNNNoI8buEE>8I

lacoN
N.. EINNIoESInsonI 8381908588!
N.. quNNSINNooIAbuEE8I

.8. N . N .8 N8:8 @930 80388. U No> 80388. NESNNNNEoNaN.
comma: N.8N.8. .Nm. .Nm.

.8. N . N .8 N85 wddé 88388. U :5 80388. Ngouafiofir
N N 2.2 36.8.8”- .NNNN. .NNNN.

.8. N . N .8 88:8 8.8.38 80388. U :5 838,—. 3:39:35.
N85.N 38.de .08.. .88..

.8. N . N .8 v.88 8.8.2. 80388. U :5 80588. 3:35:85.
oncad .336. .98. .NNMN.

.v. N . N .8 N858 8.8.3. 8858.8 0 :5 80388. 3338885.
QWNN.N GNgAvI NOW. NOW.

8.384881 I888:
wglacN8N08N8NNNINN88I IESNNI
N8NI=oN8NoNNmNN8INuo8IoNSIESaI
couato8oN8I IESNNI

NOAE88I IEoNNNI

I852

282. anNoBI838808INaoNSoNNoI
686.88. 3.258223% aINNNNNN wNmr
8.8 83888 32823
N.. boNoEINNNNENNoNINSNEoNNuI
N.. NfionlwauNoEINaoNEoNNol
N.. nongcoIgINaoNEoNNul
ougoN8>8loEalN3NEoNNol
3-53.5.5 vofiofilaonaoblzgul

NoHN-8Nomx+NmeN-88NNNx+N8Nm ”No.8 mam EU .9 Nun—28mm:

134

N 330:3:I:088::I£I0:88I

NmN 0:0.0EEQI:088::I0NI0:80:I N. :080380:|808Iw:u:9:oou

comm soul:3§:ImNI0:80:I N. «:080:wBINN00Iw:NN:9:o0I

N. 8000::0805x0ImNI080W N. :O800=00I808Iw:u:&:ool

0:0: 8O£0EI::80:8§I£I0:¢0:I ANNnEmNmNA :onmBonlEQNmouflléel

80x8: “:0:ba0bl:0wo:8»:ImNI0:m0:l mmmm Engaglméfil

800w 80wo:8bNI:oN§N8ImozmIEoNul 3mm 39l:088::lm:c0:1

“Na—:38 §:oo0ml:oN§Nomlm0NNmIESal NN .wm §I805I8~N2IFEN8I

«00:8 Endouaalmozmlfieal OmN EIS0SI§2I£N8I
.:N<N<£~+<~<£I mm §:_s.§_.§2.§eu

223 $9.2$22.:So.8+N<~<o.8<~<m/Su3 28. R- aaufizaauaueuaeeu
m_.300.w€&.03.m_loéa- m gidfizuaaeng.

0N8 080nomlw§AwN0BIleoéal m- :EINIHNENNIENNBIgBI

:3 031503.815»... MN fie.:..§_.8:21§81

83m .NoooISNuleohzosmeleoéfil NN- :EIAINENIEHNBIQI

.592 :0>0 08 :85 8:8 ‘N.N< :o 8003 08808-1 Nwwod :0:\NS:wNmI>0Im:u£I:.EN8|

8:0 MN :0 8808 0.35 an own: 00 0085 «:30 33080880 888.8 8:203: IMNI>0I0:N.N£I:EN8I
08 <~<uN :o 8038 ESuééN 4:080:80: 8.N 838080: NQ.8N 3883188219881
.No 00680 05 9 8:906: No: 0N 8:0 .30 $308888 N. $I>0008Im888§01£N8|
.0 05:30.8 .8 :8 83... m. N<~E§0Nm~ A <3 ... gluteaueauasmfiesu
.No :23898 838025 2E. .<~<m 0.603: 8.N 800 9 N. N500IN030§I0838§01PEN8I
N8 hN 585 ."N :0 80008 03 .NN muouoai 83:85.68 .<~<nN N. 888::Im838:SmI:.EN83
:0 80008 0:: m 8.N .3 80:88» 8:0 MN? :SunuJN 802383 N. :gIN82I003I8808081PmNN8I
05. .8080080: .N.? 65%.: <~<,.N .No 8:080:80M N. 8:508IN:0E050008I:£N8I
mNNS08IN~N00nNmI0:80._I N. §I00$08IN§050008IFEN8|

N. 3538808002821 $559801 2390:» .NSanEoo:Q:I:oN§88I:.EN8I

N. moiaalgaoNglwgsgoul .088 80300. 3080:? 08:8I::80N881:.EN8I

Nae 105.258 332 008.88.823.88.

3:03:80. .goéofieaofimumésasfi £23 5088.,Suaofiaalpeen
.802 5:: 2330.12.55.58-

10:22.9 8-05:5. 8828.38513338- 3.88.3809:on

135

. . m a
N ~ END A3286 ABCthgd 82.6. 332.96 om vow

. . m u N

_ ea: €885 £:§35 83o. 8:253 om mom
. . mm c N N3

85 : :ESd 5:833 825 5235 um New
. . mm H. N $355

85 : :NNNod Evowmad 82: ENG}: up Nos
. . m u

N _ E: 3:23 3:283 82.5- 533... um 3m
:AmwN

ENS 85 5.86 9:3”; 835. 59.25 pm 2..
..mm c N 8:53

3.5 ENE: @225 8:6. €325 8. Ba
:mmuN

523 85 £3.85 @335 83:. 5963 a N9.
2% u N 8:83

85 5.23: @3de 83.7 €283 .2 N3.
2% o N €5.35

85 @285 A3258: 83.7 3:833 i :5
. . m c

N _ an: €886 685.3 82.7 sammoed 5 am
. . m a

N _ an: 5285 $0qu 82.? @383 5 am
. . m u

N _ as: 53ch 6223 839 @823 5 2m
. . m a

N _ ES 53ch €9.23 83.? 5356 5 am
. . m u

N _ 3.5 3:28.: ACbawNvd 83.7 AwUNawd 5 vi

. . m v
N _ EB €323 6526 825. @383 5 mm
. . m v
N _ END $358.: $328.: SnNd. 3&8th 5 NE
. . m
u N _ a5 5385 EN286 83o ENSNE a :m
. . m c
N _ an: 333° 8333 826 SEN}. 2 3a
anondoanEIozmIEcfil
baaommulbvuommvlozmIESal
mwaulfifluoéalogmlfiofil
mete—3183182“!
bmBEEN—Elabofifixmlozmlfiofil
353818618081
cabin—Valozmtfieal
>maaoI3I8mIDl3mmIEo§I
nluuflwlogmlfiofil
mlaofimlozmIESal
xlwogloxmlfiofil
Egalonblofilfiofil
~3£I§mlfi§al
Inco—
avod gofilamEEmIm—quuel
23 .fiwuaaammmuéau
coo; ..N m 33858 a 252
83 weuaugoaaéoomwfioéa.
m: 3 adeoenmzuauoéen
82 .c matueoalmamamoéem
:35 adosenananoéan
32 .c 3158. x 2 0&2

136

8888 8:888 888.8 €888 €88 €888 28

8:888 8888 €888 8:888 8:888 fiwm
8:888 8888 8:888 8:888 8:8N_8.88%wo.m
8:888 8888 8:888 8:288 8:8_8.%8%8.m
8:8:88 888.8 €888 8:388 8:8N_8.888%8m
8:888 888.8 €888 8:888 8:88.888Mm
8:888 8888 8:888 8:888 8:§8.%8%8w8
8:888 888.8 €888 8:288 8:88.888m88m
8:888 8888 €888 8:888 8:88.8888Mm
8:888 8888 €N88 8:888 8:N:88MMo.m

8:888 8888 8:888 8:888 8:888 .88
8888 €888 888.8 8588 8:888 @888 am
8888 88888 888.8 €888 €288 8588 cm
8888 888888 8888 €888 €388 €388 2m
8888 8:888 8888 8:888 €288 8588 um
8888 8:888 888.8 €888 €288 €888 3m
8888 8:888 8888 €888 €888 €888 mm
88.8 888888 8888 €888 €888 €888 NE
88.8 €888 8888 8:888 €888 €888 :m

88.8

8:888 8888 €N88 8:888 8:888 38

2128681281828.
25.88.38.828.
MNlblafialsmmIEofil
mmIDIOmEalozwIEofil
NNIDIOmEanngEoEI
~ ~IDI8§I88|ES~I
Baa—lemmdalozmlaeul

noo—

. . .8 8 N 888

85 8:888 8:888 8888. €8,888 88 Sum
. . .8 8 N 8:8N8

85 8:888 8:88: .8 8888. 8:8888 oh 388
. . m

8 N 8 8.5 €888 €8.88 88.: €388 um 28
. . m 8

N _ 85 8:888 8:888 8888. €888 88 N38
. . m 8

N _ 885 €888 €888- 8888- €888 um :88
. . m 8 N _

8a: €8.88 8:88:88 888.: 8:883 88 Sum
. . m 8 N

_ 8:5 €888 8:888 8888. 8:888 um 88
. . m 8 N

_ 8a: 88N88 8:888 888.: 8:N_ 888 88 wow
. . m 8 N

_ 8a: €888 8:82.888 88.: 8:858 08 5.
. . m 8

N _ 885 €_ 8.8 8:883 88.? €888 am 808
. . m 8

N _ 8.5 €888 8:588 88.? €888 um new

137

N. 888.». €83 88 gm
I... . €83 :8 2m

8 88-8 €83 28 am
8 88 m €83 Sow 2m
8 . €23 88 mm

... 88 _ €23 888 98
IN. . €883 :8 2m

8 8NN m €38 28 3m
8 . €288 838 :m

N. 88 _ €23 838 :m
m . €23 now am

... 88 _ €23 now am
. ... . €83 88 :m

8 8n 22:88.8 88 mm
... . 2:882. 88 88

I8 . €83 888 mm

... 88-8 €828 :88 mm
8 2.8 m €828 :88 mm
8 8C €83 N88 mm
8. 88 2 €83 Now mm
... . €83 Noe mm

8 . €83 28 mm

8 . €38 :88 NE

8 88.1.8 8:88 888 NE
8 88 8 8:88 888 NE
8 . €83 28,8 NE

W... . €888 :8 NE

8 8m _ €88N :8 NE
8 n8 2.8.88.8 88 zm
8 8n _ 8:88 808 :m
8 . 8:88 888 :m

8 88.8 €888 88 :m
m . €83 38.8 :m

N. 88-. €83 :88 :m
... 88 _ €83 :8 :m
I... . €83 No.8 5

8 8C €23. 38 Ex
8 88 .2 €2N... 38 Ba
... 888-8 €888 88 Ex
8 8C €288 88 38
8 88 _ €288 88 38
m . €888 Now 38

8 88m 8 €83. New 38
8 8C €83. 2cm :2
8 88-. €83 2.8 38
8 8n _ €83 N78 38

8 . €888 N38 28
wan—nan 9891803:

Nimbgmlozmlcaonlfiooml

nonsmmvlvaonlfioowl

NIELEIBEIEBaIvaonIEooml
_ I_ona_lo:mIEBaIv~—3I8ooml

moo—

.853 8.— wfizgfi £88 magma
3.. :8: a 38 :8 .3 88535 A2358: 88.585899
a< .Fgm .8980 3 won—wow 88 >05 3:3
888 >18 88 888883 :3 E 8.30 5953 «noun—oboe
”mo—wan 8289 v5 835 .88ng E 830 we aougmo
05 5 8:263:83 85588 85 :83 28 «v8 :3 2E.
.xEfl: 35550 :3 05 win: 888.588 93 A805:— .8.—
93 5953 298 .525. 05 E 30 05 8998: 830 =<

magi—8908:8380»:

138

8 8228..2 €888 2.2.2 808
8 8.8 2 €23 2.282 88

8 88 2. 282282288 8.22 808
8 888-2 €8.23 85 8..;
8 82.8. 2 €883 8282 208
8 8228-2 €38... 8.222 8.2.2
8 2.8 .2 €3.88 8.22 8.2.2
8 8% 8 €2.28 :08 8.2.2
28 2 22 :83 8228 8.2.2
8 ...22 :83 2.8 8.2.2

8 88-2 €28... 8.222 8.222
8 8288 2 €282. 8.222 8.222
8 8% m 22288.8 :28 8.222
8 22822-8 22282.8 888 8.222
8 222.22 8 82288.8 38 8.222
8 2282M... 82588.8 2.08 8.222
8 83.2 82:88.8 3 8.222
8 88m 2 8222888 88 8.222
8 82.8 2 8228288 8208 8.22
8 . 82288.8 208 8.222

- 8. €28.22 8.2.2 8.222

8 82.8 m 22888.2. 2.2 8.2.2
8 88-2 €88... 8.222 8.2.2

8 88m 2 €88... 8.222 8.2.2

8 8822.8 22288.8 8.28 8.2.2
8 82.8 2 2222888 2.8 8.2.2
8 . €888 8208 8.2.2

.8 . 282228.22 8.2.22 8.2.2

8 88.2 622228... 2282 8.222
8 888.2 22288.8 «.8 8.222
8 888 2 282282288 808 8.22

o.

8 88.8 22222888 8.8 8.222
8 88 2 €22.88 22.8 8.222

- 8. €22.88 2228 8.222

8 2.8.2 28228288 2.2.2.8 8.222
8 88.2 2228288 2.28 8.222
8 88.2 222288 2.2.; 8.222
8 888 2 2228288 :08 8.222
m . 82288.8 228 8.222

8 82.8 2 22222888 2.8 8.222
8 8228-2 €88... 8.222 2.2.2

8 82.8 .2 €88... 8.2 2.2.2

8 82.8 2 €888 8.28 2.2.2

8 . €8.23 28 2.2.2

8 82.8 m €8.23 28 2.2.2
8 22% .8 €288 2.222 8282

8 82.8 2 €388 8.8 8282

8 . €9.88 808 8282

8 888 €883 808 8282

8 88 8 €883 808 8282

.8 . €888 208 8282

8 8822 2 22288... 8.222 52
8. €8.28 28 8282

2... . €2.28 :8 8282

8 82.8 2 €2.28 :08 8282
m. €2.23 8.8 8282

8 8228-2 €2.23 808 E2

8 888.8 €2 23 8.8 8282

8 8228 2 €83 88 22282
-8 . €2.83 com 8282

8 8228 w €888 .2208 22282
8 2288 8 €83 2.08 222.2

139

8 82.8-8 88m.2 €828: 808 2.222 8288
-8 82.8-8 . €2.83 88 2.222 8208

8 88m 2 88m 2 22228888 2.28 2.222 2.28
8 888 2 888 12.228882208222228
8888 w . €88.88 8208 2.222 8208

8 88 2 M88 2 €88.88 28.8 2.222 8208
8 88 w . €288.82 288 2.222 8208

8 888 2 .22 2282.8 8208 2.222 8208
waalfialxwaalaooml
misogmlogmlo—wglfioowl
2I§o§8Io228Io2w§I8ooMI
o2w5-Eoom.
ml—BSISEIESan—waalfioowl
«Jens-88182221029222.83».
2Joan—IBGIEBa-xwaalfiooml
Inco—

8 8882 2228288 8.22 2.228

8 888 2. 28228288 8.222 2.208

8 82.8. 2 €83 2282 2.202.

8 82.8-2 €888 2.222 208

8 88m 2 €888 2.222 2.28

8 888 2.822888 8.222 208

8 888.2 €883 2.2.2 208

8 88m 2 €238 2.222 8208

8 888-2 8228288 8.222 8208

8 888 .2. 22 2283 8.2.2 2.8

8 88.8 2 €888 8.2.2 2.8

8 82.8 8 M22888 8.222 22.28

8 88m 8 €2.28 8.2.2 2208

8 888 8282828 8222 228

8 83-8 822.828 8222 228

8 888m €2.28 82m 2208
8 88.8 €288 2.282 22208
8 88-8 €82.28 8282 .2208
8 888-8 €828 8282 .2208
8 82.8-2 €888 2.2.22 2228.8
8 82.8 m €888 8282 222.8
8 888-8 €288 8222 8.28
8 82.8.8 €288 8282 888
8 82.8-2 €28.28 2282 808
8 888. 8 €82.28 2282 808
8 88m 8 2828888 2.222 8.28
8 888.8 22282.8 8.22 8.28
8 888 m 282288228 8.2.2 808
8 82.8. 2 €823 8282 8.8
8 82.8-2 €288 2.222 808
8 888-2 €288 2.222 808
8 82.8 .8 2828888 2.222 898
8 888-8 €883 8282 808
8 88. 8 €883 8282 808

8 888 .2 €22.88 8.222 808
8 88.8 2 €2.83 85 808
8 82.8.2 8222888 8.222 8.28
8 888 2. 8222888 8.222 808
8 82.8-2 €2.23 85 808

8 88.8 8 €223 82m 808

8 82.8-8 82288.8 8.222 2.08
8 88 8.822888 8.222 2.88
8 888-8 €283 8282 2.08

8 3.8 8 €283 82m $8

8 888 2 28228888 8.222 808

8 888-2 28238.8 8222 828

140

8 . 888.8 €8.88 88 2282 8.28

8 . . €88.88 808 2282 2.20.8

8. 888-2 282822.882 8.28 2282 2.2.2.8

8. 888 2 €82.82 .3 2282 2.208

-8 . . €88.22 808 2282 808

8 888 8 . €838 8.28 2222 2.20.2.

8 888.8 888.2 €88.88 8.28 2282 2.2.22.
8 888 8 888 2 €838 8.28 2282 2.2.28
8 888.8 . 82288882 8.28 2222 8.28

8. 888-2 82282.88 2.28.8 282 2.20.8

8. 888 2 8222.88 2.2.28 2282 2.2.8

- 8 . . 282822.228 2.2.28 2282 8.2.8

8 888 2 888-2 28228.22 2.202. 22.22 2.208
8 888 2 282822.228 2.2.28 2282 8..;

8 888.8 . 282822.228 2.208 2222 8.28

8 888 2 8288 2 28.28.2282 2.222 2.222 2.222
8 888 2.82.22 8 22.228 2.222 2.222 8.28

8 888 8 888 8 €88.82 2.222 2.222 808
8 888 2 888 2 88228.28 2.222 2.222 888
8 888 2. . 22.228 2.222 2.222 8.22.

.8 888-2 82.8 8 8.228 2.222 2.222 88.8

8 888 8 888 8 28288.82 2.222 2.222 208
8 888-2 888-2 €88.88 2.222 2.222 2.28
8 888 2 888 2 €88.88 2.222 2.222 82.28
8 888 .2 . 2828-2882 2.222 2.222 828
8.82.8 2 82% 8 22.228 2.222 2.222 8.28

8 82.8 2 88.8. 2 €28.28 2.222 2.222 8.28
8 82.8 2 888 2 688.82 2.222 2.222 808
8 82.8 8 . 22.8 2.222 2.222 808

2.82.8 2.82.22 8 22.228 2.222 2.222 8.28

8 82.8 2 888 26288.88 2.222 2.222 8208

8 82.82 8882 28288.82 2.222 2.222 8208
8 82.8 2 888-2 28282.82 2.222 2.222 82.28
8 82.8 2 82838 2.222 2.222 82.28

8 82.8.8 888-2 €82.88 8.28 2.222 8.28

8 82.8 8 888 2 €82.88 808 2.222 808

8 82.8-8 . 222228.822 8.28 2.222 8.8

8 82.8-8 82.8-8 2228.8: 22.8 2.222 808
8 82.8-8 888-2 €888: 8.28 2.222 208
8 82.8-8 888-8 €88.82; 808 2.222 2.28
8 82.8.8 888 2 €8.88 88 2.222 82.28

8 82.8 8 . €8.88 8.28 2.222 82.28

8 888 2 88m 2 82288.28 808 2.222 808

8 .888 282822.88: 808 2.222 888

8 888 2 82.8 8 €822.88 8.28 2.222 8.28

8 888-2 888-2 €82.88 808 2.222 208

8 888-2 888 2 22288.82 808 2.222 2.28
8 888-2 888-8 282288.82 8.28 2.222 8208
8 888.2 . €88.92 8.28 2.222 8208

8 .888 282822.88: 8.28 2.222 808

8 M88 2 m3 8 €822.88 808 2.222 8.28

8 888 2 .888 2 822228.82 808 2.222 208
8 888-2 888-2 €22.22 3 2.222 8208

8 888 2 .888 2 28288.8 8.28 2.222 82.28

8 88 2.. 222228.82 8.28 2.222 8208

8 . 82.8.8 222222.82 80.8 2.222 808

8. 888-2 82282.88 80.8 2.222 208

8. 888-2 82282.88 82.8 2.222 208

8. 888 2 8222.288 80.8 2.222 8208

- 8H 8222.288 802. 2.222 8208

8 82.8 8 888 2 82228.88 88 2.222 2.28

8 82.2.8 888-2 282228.88 8.28 2.222 828

141

8 888m 8888 282288.88 8882 8282 2288
8 888.2 82.8-8 22.22.8888 8882 8282 2288
8 888-2 82.8-2 282288.882 8882 82m 888
8 888 2 82.8.2 282288.882 8882 8282 888
8 88m 2 . 282282.88 8882 8a 888

8 888 2 82228.82. 8822 8282 8288

8... . 282288.882 8822 8282 888

8 . 888.8 22.22.8888 8882 8282 :88
8.82.8 8 28228.88 8822 82m 2288

8 . 82.8-2 82282.88 882.22 8282 88.8

8 . 82.8 2 282282.88 882 8282 888

8 . . 282288.882 852 8282 888

8... 282228.82. 852 8282 8288

8. 888 8 82288.88 888 mm 2288

8 . 82.8-8.8228888 888 85 2288

8 . 82.8-2 8288.88 888 8282 888

8 . 82.8 2 8288.88 888 8282 888

8 . . 8288.88 888 8282 888

- 8.. . 2 2288.882 888 8282 8288

8 888-8 82.8-8 $2288.28 2288 8282 2288
8 888-8 82.8-2 2 2288.882 :88 8282 888
8 888 8 82.8 8 2 2288.882 :88 8282 888
8 888 8 . 28288.88 :88 8282 888

8 8.88 8 882288.88 2288 85 8288

8 82.8.8 82.8-2 2822.88 2288 85 88.8

8 82.8 8 82.8 2 28888.8 2288 8a 888

8 82.8.8 . 222288.882 2288 8282 888

8 82..8 8 . 282288888 2288 82m 8288

8 82.8 2 88.8 2 2:28.22 88.8 8282 888

8 82.8 2 . 282228.88 88.8 8282 888

2.. 3.8-— . 838.3 «08. mm Sum

8 82.8.2 . 282228.88 888 8222 888

8 82.8 2 .82288.88 888 8282 8288

8 88228.88 888 8282 8288

8 . 888-8 28288.88 :88 85 888

8. 82.8 8 28288.88 :88 8282 888

8. 282288.282 2288 8282 2.288

8.... 28282.8 288 8282 288

8. 888-2 8282.8 2288 8a 288

8 888-8 82.8 8 82228.88 888 8282 888
8 88m 8 . 28288.88 888 8282 2.288

8 8.88 8 882288.882 888 82m 288

8 888 8 888 2 2888.88 888 8282 288

8 82.8 m . 8288.88 888 8282 2.288

8 82.8 8 . 8288.88 888 8282 288

8 82.8-8 888 2 822822.882 888 8282 288
8.. . 28288.88 2.288 8282 288

8 . 888-2 28288.88 2.288 8228 288

-8 . 88.8 2 882288.88 288 8282 288

8 888 2 88m 2 822228.882 8.2.22 2282 888
8 888 8 . 282288.882 8882 2282 888

8 888 2 888-8 88282.88: 832 2282 888
8 888 8 . 8288.88 852 228. 2.288

8 888-2 888-2 28288.88 852 2282 2.28.8
8 888 2 88.8. 2 8288.88 852 2282 2.288
8 888 .2 . 282288.88 88.22 2282 888

8 ..888 2.8 82288.88 888 2282 888

8 888 2 888 8 28288.8 888 2282 888
8.888 2.. 28288.8: 888 2282 2.28.8

8 888-2 888-2 €88.88 888 2282 828.8
8 888 2 888 2 €88.88 888 2282 2.288

8 888.2 . 28288.8 888 2a 888

142

8 888-8 . 6288.282 852 8282 2288

8 888 2 82.8 8 882888.82 852 85 2288
8 888 8 . 28288.88 88.22 8282 888

8 88m 2 88.8. 2 2888.82. 88.22 8282 888

8 888 2 888 8 882288.88 8882 8282 888
8.. . 82288.88 288 8282 2288

8.82.8 2 82288.88 288 8282 2288

8.. . 8888.88 288 E 888

8 . 888 2 8828.88 288 8282 888

8 . 888 8 222282.882 288 8282 888
8.82.8 2 22228.88 2288 88m 2288

8 ... €88,882 :88 8B 888

8 . 888 2 88288.88 2288 8282 888

8. 888-882288.28 2288 8282 888

-8 82.8.2 . 88288.88 2288 8282 888

8 82.8.2 888-2 8288.882 :88 8282 888
8 82.8 2 888 8 82288.28 :88 8282 888
8 . 888-2 282288.88 888 8282 888

8. 888-8 82288.88 88 8a 888

8 888 2 888 8 82288.88 888 282 888
8 888 8 . 82 2288.88 888 8228 888

8 888 2 888 2 2388.88 888 8882 8288
8 888 2 .888 8 882288.882 888 8282 2.88
8 888 2 82.8 8 88282.88 888 8282 2.88

8 888-2 . 8288.88 888 8282 288

8 . 888 8 8288.88 888 8282 8288

8 . 888 8 88282.88 88 8282 2.88

8 . 82.8 8 882288.882 888 82m 2.88

- 8 . . 3288.88 888 8282 288

8 888-2 888-8 8288.88 8288 828. 2.88
8 888 2 82.8 8 8288.88 8288 88288 2.88

8 8.88-2 882288.882 8288 8282 288

8 888 8 82.8-8 82 2288.88 2.88 8228 888
8 888-8 . 28228.8 2.88 8288 288

- 8 82.8 8 . 88228.8 2.88 8282 288

8 888 8 888-8 $88.88 8288 88m 8288
-8 888.8 . 28228.88 8288 8a 888

8 888 8 888-2 688.882 8288 82m 888
8 888 8 . 8288.88 8288 8282 888

8 .888 8.. 688.882 8288 8:2 888

8 888 8 888 2 28228.88 8288 8282 888
8 888 8 . 8288.88 8288 85 2.88

8 . 888 2 82 2288.88 888 8288 888

8. . 82288.28 888 8882 2.88

8 888 2 282288.28 888 8282 2.88

8 888 8. 8228.88 8288 2.882 8288

8 888 8 888-2 8228.88 8288 2.282 8288
8 888 8 . 52.8.8 8288 2.282 888

8 888 8 888 2 52.8.8 288 2.2m 888
8 888 8 . 8:88.882 8288 8282 888

8. 888 2 $2228.88 8288 2.288 8288

8. 882288.882 8288 2.282 888

8 . 82.8 2 88288.88 8288 2.282 888

8. . 582.28 8288 2.282 888

- 8 888 2 . 28288.88 8288 2.282 888

8 888 2 82.8 8 $2288.82 8288 2.882 888
8 888 8. €82.28. 8288 2.282 888

8. 82.8 2 82 2288.88 888 282 888

8. . 82282.28 888 2.5 888

8 82.8- 2 .82282..28 888 2.282 888

8 888 2 42.28838 8.282 8.2m 2m

2.. 88m-— . 3:88.882 8.2.22 85 888

143

8 82.8.2 82.8.2 8828.88 888 852 888

- 8 888 2 8828.88 888 8.282 888

8 82.8.2 82.8.2 8888.882 888 852 2.288
8 82.8.2 82.8.2 8828.882 888 852 2.288
8 828.2 888.2 8828.882 888 8882 2.28.8
8 82.8 2 888-2 8828.882 888 852 :88
8 82.8 8 . 8828.88 888 8822 8288

8 888 2 82.8.2 8822.88 888 8882 8288

- 8 82.8 2 4828.88 88 8.2.22 888

8 82.8 2 82.8 2 $8.22 888 88.22 2.288
8 82.8.2 82.8.2 82.28.2222 888 82282 :88
8 82.8.2 888-2 882282.88 888 88.8 2.288
8 82.8 2 888-2 882282.88 888 88.22 2.288
-8 82.8-2 4828.282 888 8882 8288

8 82.8 282.8 2 882282.28 888 82282 8288
8 . 82.8H2 882288.88 888 8.282 2.288

8. 82.8 8 882282.88 888 8.282 :88

8. 888 2 82.28.2222 888 852 2.288

8 . 888-2 $8.22 888 8882 2.288

8 ... 882282.28 888 8.282 8288

-8 . 82.8 2 2828.282 888 852 8288

8 82.8 8 82.8 8 82 228.8 828.8 8.282 2.288
8 82.8 2 888-2 82.28.88 2.28.8 852 :88
8 82.8.2 888 2 $8.88 :88 88.82 2.28.8
8.82.8 2.. 882228.88 2.28.8 852 8288

8 82.8 8 82.8 8 82.28.32 2.288 852 8288
8 82.8-2 888-2 22.28.88 2.288 852 2.288
8 82.8 2 888 2 82.28.88 2.288 88.8 2.288
8 82.8 2.. 882228.88 2.288 8.282 8288

8 82.8-2 82.8 2 58.2.2.2 2.288 8.282 8288
8 888-2 888-2 82 228.8 2.288 822.8 2.288

-8 888H2 . 38.2.2.2 2.288 88.22 8288

8 888 2 82.8.2 282228.88 2.28.8 892 8288
-8 888-2 82.88.32 2.288 8.282 8288

8 888 2 82.8 2 882228.88 8288 8882 8288
8.. 82.8 .2 8828.88 8288 88.22 8288

8 888- 2 82.8- 2 38.882 852 2.2.2 88.22

8 888 2 888 2 82288.88 8.282 288 888
-8 888-2 . 882888.82. 852 288 8288

8 888 2.82.8 2 882288.882 832 2.2.2 8288
8 82.8 2 82.8 2 82288.88 8.282 2.28 888
8.82.8 2.. 882288.882 88282 2.28 8288

8 82.8 2 82.8 2 882288.82. 8882 288 8288
8 888-8 . 82288.88 88 28.2 8288

8 82.8 2 82.8 2 82288.88 88 2.2.2 8288
8 ..888-282.222.8828 8288 28.2 8288

8 82.8 8 82.8 2 E88882 252 8282 888
8.82.8 8.. 582.882 2.222 8282 888

8 82.8 8 888-8 €88.88 28.22 8282 888

8 82.8-8.888 8 €88.88 222.22 8282 888

8 82.8 8 822228.882 252 8282 8288

-8 82.8.2 .822 2.28 888 8282 888

8 82.8 8 888 8 8828.282 888 8282 888

8 82.8 2 888 8 8828.88 888 8282 888

8 82.8.2 82228.88 88 8282 8288

8 . 88m 8 8828.88 888 8282 888

8 .888 8 63.282 888 22288 888

- 8 ... 82228.88 88 8282 8288

8 888 8 888 8 82 2288.88 888 8282 888

8 888-8 . 82288.88 88 8282 8288

8 888 8 . 882288.88 888 5 828m

8 a: £33.88 8922 82m 288

144

- 8 8.82.-2 882882 888 8.22 8.2.2

8 882. 2 82.8-2 282288.28 88 8.2.22 828
8 882. 8 . 82.2382 888 8.222 8288

8 882. 2.. E22882 888 8.2.22 8.2.2

8 8.88 2 282882 888 8.2.22 8.2.2

8 82.8 .2 . 8828.28 8288 8.2.22 828

8 82.8 2 . 2828.82. 8288 8.222 8.22

8 82.8 2 88228.88 8288 8.222 8.2.2

8 . . 8828.82. 8288 8.2.22 8.2.2

8. 28228.88 8288 8.2.22 8.2.2

.. - 8. .8228 8.2.2 8.2.22 8.2.2

8 82.8-2 888-2 28228.88 2.2.22 8.2.2 8.222
8 82.8 2 82.8 2 88228.88 2.2.82 8.2.2 8.2.22
8 82.8 2 888 8 28228.88 2.222 8.2.2 888

8 82.8 2 82.8 2 22288.88 2.2.22 8.2.2 8288
8 82.8 .2 22288.88 2.2.22 8.2.2 8288
8.82.8 2.. 8228.882 2.2.22 8.2.2 8.2

8 888 2.82.8 2. 8828.882 8.2 8.2.2 8.2.22
8 88.8 2 888 8 2823.8 8.2.22 8.2.2 888

8 888 2 888 2 2828.882 8.222 8.2.2 8288
8 888 8 . 282288.82. 8.2.22 8.2.2 8288

8 888 2 . 88228.88 8.2 8.2.2 8.2.22

8 82.8 2 888 8 8822.88 8.2.22 8.2.2 888

8 82.8 2 82.8-2 282288.82. 8.2.22 8.2.2 8288
8 82.8.2 . 2828.82; 8.222 8.2.2 8288

8 888 2 88228.88 8.2..2 8.2.2 8.2.22

8 888 8 82.8 2 82.22.88 888 8.2.2 8288

8 88.8 8 . 82.22.88 888 8.2.2 8288

8 888 .8 . 88228882 888 8.2.2 8.2.22

8 82.8.2 8828.3 8288 8.2.2 8288

8 82.8 2 82.82.2282 8288 8.2.2 8.2

8. . 2822.882 8288 8.2.2 8.2

8 8882 888H2 282228.82. 2282 8.2.22 888
... 888 2 888 2 282228.82. 2282 8.222 888

8 888H2 82.8H2 22.28882 2282 8.222 888
8 888 2 82.8 2 2828.82 2282 8.222 888
8 888 8 . 2828.82 2282 8.2.22 888

8 888-2 82.8-2 2828.82. 2282 8.222 2.282.
8 888-2 82.8.2 8828.82. 2282 8.222 2.288
8 888-2 888-2 8828.82. 2282 8.2.22 2.28.8
8 888 2 888 2 2828.82. 2282 8.222 2.288
8 888-2 2828.82 2282 8.2.22 8288

8 888-2 82.8-2 2828.82 25 8.2.22 8288

8 888H2 888H2 82 228.8 88 8.2.22 888
8 888 2 82.8.2 22.28882 888 8.2.22 888
8 888-2 82.8 2 2822.82 888 8.2.22 888

8 888 8 . 52.2.82 888 8.222 888
8 888 2 888-2 2822.88 888 8.222 2.282.
8 8882 82.8.2 8822.88 888 8.282 2.288
8 888-2 888.2 822.88 888 8.222 8288
8 888 2 888 2 2822.88 888 8.2.22 2.288

8 888 8 . 2822.28 888 8.222 8288
8 888-2 82.8.2 8822.28 888 8.222 8288
8 888-2 82.8-2 22.28.2282 888 882.22 888
8 888 2 82.8 2 2822.282 888 8.222 888

8 888 8 . 2822.282 888 8.2.22 888
8 888-2 82.8-2 2828.88 882. 8.2.22 2.282.
8 888-2 888-2 2822.88 88.8 8.2.22 2.288
8 888-2 888.2 822.88 882. 8.222 2.28.8
8 888 2 888 2 822.88 88.8 8.2.22 2.288

8 888 2 8822828 888 8.2.22 828
8 888-2 888-2 2828.28 888 8.2.22 8288

145

- 8 82.8-.2 . 2822.88 8.2.22 8.2.2 8.222

8 82.8 8 82.8 2 2822.88 2288 8.2.2 8288

8 82.8 8. €2.88 2288 8.2.2 8288

8 888 8 . 22.2882 288 8.2.2 8.2.22

8 82.8 2. . 8828.88 8288 8.2.2 8288

8 82.8 2 . 282282 8288 8.2.2 8.222

- 8. . 882282 8288 8.2.2 8.2.22

8 888 2 82.8 2 8.828.882 8.2.22 8.2.22 8.2.22

8 888 8 82.8 8 22.88 8.2.22 8.2.8 2288

8 888 2. 888 8 8.88 8.222 8.222 888

8 888 2 82.8 8 82288.28 8.2.22 8.222 2.88
8 888 8 888 8 882282.882 8.2.22 8.222 888
8 888 2 888 2 22.228888 8.2.22 8.2.22 888
8 888 2 888 2 282288.882 8.2.22 8.2.22 888
8 888 2 82.8-2 882288.882 8.2.22 8.222 8288
8 888 8 . 282282.82. 8.222 8.222 8288

8 888-2 . 28288.88 8.2.22 8.2.22 8.2.2

8 888 2 828288.822 8.2.22 8.222 8.2.2

8 82.8 8 82.8 8 8.228 8.222 8.2.22 288

.8 82.8 -2 888 8 8.228 8.2.22 8.2.22 888

8 82.8 8 82.8 8 282282.882 8.2.22 8.2.22 2.88
8 82.8 2 88.8 8 82288.28 8.2.22 8.2.22 2.88
8 82.8 8 882. 8 882288.882 8.222 8.2.22 888
8 82.8 2 888 2 22.228888 8.222 8.222 888
8 82.8 2 88.8 2 82282.82. 8.222 8.222 8288
8 82.8 2... 882288.882 8.2.22 8.2.22 8288

8 82.8.2 . 282228.228 8.2.22 8.222 8.2.2

8.82.8 2. . 82.58.88 8.2.22 8.222 8.2.2

8 82.8.8 888-8 22.28882 2288 8.222 888
8 82.8-8 82.8-8 2828.882 :88 8.222 2.88
8 82.8 8 888 8 2828.882 :88 8.2.22 2.88

8 82.88 882m2 2828.88 2288 8.2.22 888
8 82.8 8 88.2. 2 8828.88 2288 8.222 888
8 82.8 8 82.8 2 2828.88 2288 8.2.22 828
8 888.8 . 2828.88 2288 8.222 8288

8 82.8 8 ..28228.88 2288 8.222 8.2.2

.8 82.8 .8 . 28282. 2288 8.222 8.2.2

8 888-8 82.8-8 2828.28 888 8.222 2.88

8 888 8 888 8 8828.28 888 8.2.22 2.88

8 888-8 882..2 2828.882 888 8.2.22 888
8 888-8 882.-2 8822.882 88 8.2.22 888
8 888 8 82.8 2 2828.88 888 8.2.22 828
8 888.8 . 2828.88 88 8.2.22 828

8 888 8 88228.3. 888 8.222 8.2.2

- 8 888. 8 . 28288 888 8.2.22 8.2.2

8 888 8 888 8 2828.88 2.88 8.222 2.88

8 82.8 8 882. 8 282288.28 2.88 8.222 888
8 82.8 8 888 2 2828.8: 2.88 8.222 888
8 82.8.8 88.8 2 22.22.32 2.88 8.2.22 828
8 82.8 8 . 282288.88 888 8.2.22 828

8 82.8-8 . 82.228882 2.88 8.2.22 8.2.2

8 82.8 8 . 282222.882 2.88 8.222 8.2.2

8 888-8 888-2 2828.22 2.88 8.2.22 888
8 888 8 888 2 282288.28 2.88 8.2.22 888
8 888 8 82.8-2 282288.88 2.88 8.222 8288
8 888.8 . 22.28.82 2.88 8.222 8288

8 888-8 . 22.228882 2.88 8.2.22 8.2.2

8 8.88 8 88228882 2.88 8.2.22 8.2.2

8 882. 2 882. 2 2828.88 888 8.222 888

8 882. 2 888 2 38.2.82 88 8.222 8288
8 888 2 . 28228.88 88 8.2.22 828

8 888-2 . 2828.882 888 8.222 8.2.2

146

8 82.8.8 . 22 2288.8 8282 888 8282

8 82.8 2 . 8288.88 8282 888 2.282

- 8... 28288.88 8282 888 2.282

8 888 2 88.8 2 8828.228 8.222 888 8.222
-8 82.8-2 . 2828.882 8.222 888 8282

8 888 8 82.8 8 22.228888 8.222 888 8282
8 82.8 2 888 8 2828.82 8.2.22 888 8282
8 .888 2.. 22288.88 8.2.22 888 8282

8 888-2 82.8-2 8828.882 8.222 888 8282
8 888 2 888. 8 2828.82 8.2.22 888 8282
8 . 82.8-2 282288.88 82m 888 8282

8 . 888-8 $2282.88 8282 888 8282

8 82.8 8 888 8 $2282.88 8282 888 8282
8 888. 8 888. 8 28222.88 8.222 2.88 8.2.22

8 82.8 8 888 8 2828.882 8.222 2.88 8282
8 82.8 8 82.8 8 22.222888 8.2.22 2.88 8282
- 8 82.8 8 . 2828.88 8.222 888 8282

8 888 8 888 .8. 22.222.82.22 8.2.2 2.88 8282
8 888 8 888-8 2828.882 8.2.22 2.88 8282
- 8 888. 8 . 2828.88 8.2.22 2.88 8282

8 888 8 82.8 8 82 2288.88 8282 2.88 8282
8 888-8 . $2228.88 8282 2.88 8282

.8 82.8 .8 . $2228.88 8282 2.88 8282

8 888 2 888 2 882282.88 8.222 888 8282
8 8888 2 882282.88 8.2.22 888 8282

8 888 2.888 2 8828.2. 8.2.22 888 2.2.2

8 888 8 . 882282.88 8.2.22 888 2.282

8 888 2 888 .2 282282.88 8.222 888 2.282
8 888 8 . 8222.28 8282 888 8282

8 888 2 8.88 2 222282.88 8282 888 2.2.2
8 888 2 . 8283.82 8282 888 :82

8 888-2 888H2 2822.22.88 8282 888 8282
8. 888 2 8282.88 8282 888 2.2.2

-8 . . 2822.22.88 8282 888 2.282

8 . 888.2 8223.882 8282 888 8282

8 888 8 . 82282.88 2.2.2 888 2.282

8 888 2 888.2 82282.88 2.2.2 888 2.282
8. 888 8 22 2288.822 2.282 888 2.282

8 . 888 2 2828.88 2.222 882. 8.2.22

8. 882228.282 2.2.22 888 2282

8 . 888 2 28288.88 2.222 882. 8282

8.. . 28288.88 2.2.22 88.8 8282

- 8 888 2 . 2822.88 8.2.22 888 2282

8 888 2 888 2 2823.882 8.2.22 888 8282
8 888 2. . 2823.882 8.2.22 88.8 8282

8. 888 2 $2228.88 2282 888 8282

8. . $2228.88 2282 888 8282

8 888 2 . 282228.88 8282 88.8 8282

8 . . 882288.882 8282 288 8222

8.. . $2288.88 8282 288 8282

8. 82.8 2 82288.88 2.282 288 8282

8... 52.8282 8282 288 8282

8. 82.8-2 822.8282 8282 288 8282

8. 82.8-2 282288.88 8282 288 8282

8 888 .2 82.8 .2 2828.882 8.2.22 8.2.2 8.2.22
8 888 2 888 8 22.28.28 8.2.22 8.2.2 2288
8 888 2 888 2 2822.282 8.222 8.2.2 8288
8 888 2 882288.82. 8.222 8.2.2 8288

.8 888 .2 2822.88 8.2.22 8.2.2 8.2.22

8 88.8 2 888 8 22.28.88 8.2.22 8.2.2 2288
8 82.8 2 82.8.2 82288.82. 8.222 8.2.2 8288
8 82.8 2 8822.282 8.2.22 8.2.2 8288

147

8 8.88-8 .82 2288.882 8282 2288 8282

8 888 8 888 2 2828.88 8282 2288 82m
- 8 82.8 8 . 822.888 8282 2288 82m

8 82.8 8 888 8 222288.882 8282 2288 8282
8.. 888 8 22228.88 8282 2288 8282

8 888-8 888-8 28288.28 2.282 8288 8282
8 888 8 888 8 28288.28 2.282 8288 8282
8 888 8 . 8288.88 8282 22288 8282

8 888 8 888 2 28288.88 2.282 22288 2.282
8 888 8.82.8 2 882282.882 2.222 8288 8282
8 888 8 888-8 28288.88 8282 8288 8222
8 8.88 8 882282.82 8282 8288 2.282

8 888-8 82.8-2 28288.88 8282 8288 2.282
8 888 8 82.8 2 8288.88 8282 8288 8222
- 8 888 8 . 28288.88 8282 8288 2.282

8 888 8 .82.8 2 882232.82 8282 8288 2.282
8 888 8 82.8 2 8288.88 8282 8288 8282
8. 82.8 8 82228.88 2.282 22288 2.282

8 . 82.8-2 88288.88 2.282 8288 8282

8 82.8 2 82.8 8 28888.88 2.282 8288 8282
8 . 888-8 28282.88 8282 888 8282

8 . 82.8-8 2828.82.22 82m 888 8282

8. 82.8 2 28288.88 85 888 2282

-8 . . 8288.88 8282 888 2282

8.. 888 8 882288.882 8282 888 2282

8 888 8 82.8 8 $2228.88 8282 888 8282
8 888 8 82.8 8 882288.882 8282 88m 2282
8 888 8 . 28288.88 8282 888 2282

8 888-8 888-8 8288.88 8282 .288 2222

8 888 8 82.8 2 2828.88 8282 888 2222

8 82.8 8 . 282288.882 8282 .288 2282

8 82.8.8 888.8 8288.88 8282 888 2282

8 .82.8 2.. $2288.88 2282 888 2282

8 82.8 2 888-8 8288.88 2282 888 2282
8. 888.8 822.888 2282 2888 2282

8 88.8 8 888 8 8828.28 2.2.22 888 8.2.2

8 82.8.8 888.8 282288.28 2.2.22 888 8.2.2
8 82.8 8 888 2 28288882 2.2.22 888 8282
8 8.8.8 8 . 2.8288882 2.2.22 888 8282

8 8888 8 8.88 8 2828.8 8.2.22 888 8.2.2

8 888 8 82.8 2 282282.88 8.2.22 888 8282
.8 888 .8 . 882282.88 8.222 888 8282

8 888 8 82.8 2 882228.82 8.2.2 888 8282
8 888 m . 282228.82 8.2.2 888 8282

.8 82.8-2 . 22 2288.88 8282 888 8282

8 828.2 888.2 82288.28 2.222 888 2.2.22
8 82.8 2.82.8 8. 8288.882 2.2.22 888 2.2.22
8 8.2.8 2 888 8 688.88 2.222 888 8282
8 82.8 .2 888 .8 882288.882 2.222 888 8282
8 888. 2 82.8. 8 222288.882 2.2.22 888 2.2.22
8 888 2 .888 8 882288.882 2.222 888 8282
8 888 2 888 8 28288.88 2.2.22 888 8282
8 82.8-8 888-8 82282.88 2.222 888 8282
8 888 .8 888 .8 82282.88 2.2.22 888 8282
8 888 8 888.8 82 2288.88 8282 888 8282
.8 888 .2 . 2828.88 8.2.22 888 8.2.22

8 888 2 888 2 2828.882 8.222 888 8282
8 888 8 . 82.228888 8.2.22 888 8282

8 888-2 . 8828.882 8.222 888 2.22.2

8 . 82.8 2 22.228888 8.2.22 888 8282

8 . . 2828.882 8.2.22 888 8282

8 . . 2828.82 8.2.22 888 2.282

148

8 .888-2 82828.88 8.222 8288 8.2.22

8 888 2 888 2 888.8 8.222 8288 2.2.2

8 88m 2 8822.228 8.222 8288 2.2.2

8 888 2.. 2828.882 8.222 8288 8282

8 . 888 2 8822.228. 8.222 8288 2.2.2

8 . . 2828.8 8.222 8288 2.2.2

-8 . . 8828.882 8.222 8288 82m

8 888.2 82.228888 2.2.2 8288 2.2.2

8 888 2 882288.88 2.2.2 8288 8282

.8 . . 882288.88 2.2.2 8288 8282

8 .82.8 2.. 22 32.8.2.8 2.222 8288 2.2.22

8 82.8 2 888 2 2828.882 2.222 8288 8.2.2
8 .82.8 2828228888 2.222 8288 8.222

8 82.8 2 888-2 8828.282 2.222 8288 8.2.2
-8 82.8-2 . 28282.22 2.222 8288 8.2.2

8 82.8 2 888-2 38.882 2.222 8288 8.2.2
8 8.2.8 2 . 2822.8... 2.2.22 8288 8.2.2

8 82.8 2.. 882288.882 2.222 8288 8282

8. 888 2 28288.88 2.222 8288 8.222

8 8828.882 2.222 8288 8.2.2

8 . 888 2 88282.8 2.222 8288 8.2.2

8 ... 2828.282 2.2.22 8288 8.2.2

8 . 888 2 2828.822 2.222 8288 8.2.2

8. . 22.28882 2.2.22 8288 8.2.2

8 . 88228.82 2.222 8288 8282

8 888 2 8828.28 8.222 8288 8.222

8 88 -2 888.2 8828.8 8.222 8288 8.2.2
-8 888-2 . 828.88 8.222 8288 8.2.2

8 888 2 888-2 28:82.8 8.222 8288 8.2.2
8 888 2 . 828.88 8.222 8288 8.2.2

8 888-2 . 2828.882 8.222 8288 8282

8. 888-2 2828.88 8.2.22 8288 8.2.2
8. . 828.8 8.222 8288 8.2.2

8. 888 2 2828.88 8.2.22 8288 8.2.2
8. 88222.28 8.222 8288 8.2.2

8.. . 2828.882 8.222 8288 8282

8 ..888 2.. 2828.88 8.2.2 8288 8.2.2
8 888 2 88.8 2 2288.8 8.2.2 8288 8.2.2
8 888-2 . 28892.8 8.2.2 8288 8.2.2

8 888 .2 8828.28 8.2.2 8288 8282
8 . 888 2 2823.8 8.2.2 8288 8.2.2

8 . . 2828.8 8.2.2 8288 8.2.2

8. . 58.2.8 8.2.2 8288 8282

8 888. 2 . 8828.; 8.2.2 8288 8.2.2

8 888 2 8822.882 8.2.2 8288 8282

8 . . 2822.82 8.22 8288 8222

8 8.2.8 8 8822.882 8.222 2288 8282

8 8.2.8 8 8.2.8 8 2828.8 8.222 2288 8.2.2

8 82.8 8 888.8 882228.88 8.2.22 2288 8282
8 82.8.8 82.8 8 282228.88 8.222 2288 82m
8 82.8 8 . 282288.88 8.2.22 :88 8282

8 82.8 8 888 2.2838888 8.222 2288 8282
8. 82.8. 8 828.882 8282 2288 8.2.2

8 . 888-8 $2288.88 8282 2288 8282

8 . 82.8 8 $2288.88 8282 2288 8222

8.8 . $2288.88 8282 2288 8282

8 ...888 2 882288.88 8282 2288 8282

8 82.8-8 888-8 2828.88 8.2.2 2288 8282

8 82.8 8 82.8 8 8828.88 8.2.2 2288 8282

8 82.8 8 . 2828.88 8.2.2 2288 8282

8 82.8 8 888 2 2828.88 8.2.2 2288 8282

8 888.8 82.8-8 8228.28 8282 2288 8282

149

888.8 5.32888-828-88882.

8822.2. 82.8-822.888.828.888.-

8888 888-822888.828-88882-

2.8.2.8 228-88e-8888m8-8888888Hpe22m

82 .88. - 2282 888.22 82282-928228-
vmad 88g 505 85305.8.“ $95.32: Fem—u

8 888-2 888-2 22.28.88 8.222 2.288 8.2.22

8 888-2.. 282282.882 8.2.22 8288 8282

-8 888-2 2822.882 8.2.22 2.288 2282

8 888 2 82.8 2 28228.28 8.2.22 2.288 2282

8 888.8 . 282282.882 8.2.22 2.288 8282

8 888 2 88228.28 8.222 2.28.8 2282

8 888-2 82.8-2 2822.882 8.222 2.288 2282

8... 8288.88 8282 2.288 2282

8 . 82.8 2 €88.88 8222 2.288 2282

.8 . 82.8- 2 $2282.88 2282 2.282. 2282

8 82.8-2 888-2 22288.88 2.222 8288 2.222

8 82.8 2 888-2 282288.88 2.282 8288 8.2.22

8 82.8 2. . 2828.882 2.2.22 8288 8.222

8 82.8 2888 28288.88 2.222 8288 2.2.2

8 82.8 2.. 282288.882 2.2.22 828 2.2.2

8- 82.8 2.. 282282.88 2.222 8288 8282

8 888 2 888 2 2828.882 2.222 8288 8.2.22

.8 888.2 882228.88 2.222 8288 8.222

8 888 2888 8282288882 2.2.2 8288 2.2.2

8 888 2 88288.28 2.2.22 8288 2.2.2

8 888-2 282282.88 2.222 8288 8282

150

282888 858.88.882.288282228.p22228.

88883848800288.228on

8.. figovlmmoooal 2&8n81_2axol

8.. xufilhlnouoobglxromnad2&8.

2.. 828222- 81220820022820.23038-2228220.

2.. unbiagoobglfismnalunxol
303 22222-282228.280123032218298-

mmam

888.2-238.228.22.288.

8882222822282 822. vofiofilbfigulfigolcaxul
82 8.8 FEE-328888.2sm828-22288.
8.. maofilbmmaovlgmbolzaxol

2..
8..
8..
8..
8..

§I0B81288bol~2qxot
caloummlgmbolznxol
anIufimlamboI—Exol

28228488820429on

nozntomoqumfiolzaxol

2.. xaEISofil2aoEo2amaoEI=ool
... glfiofilfiofiosmmoalfiol
8.. voglméo2l2aoEoB§oEI=ool
Amvmom 0238209220212=080888222I=8I

8

8228.382

8.88

282888.88

8.88
€828.28
282288288.
288882.82

8.338.283.5288.
2:33.:3-
888%.- 03:81:00-
Sonic—M22843”...
nan—alqual—Eol
alga—4622i
8.828.882.2288-
nuance—Izool

.8 .8828- ....

.N- ..8- .22-.
.8- .822.r8 J...
.N .8 .x.

8.828-881.8088. >822volmbu8888|

Inco—

8. 2-3Ioglgc2wlooamlzbofifizml

8..

wag-:oolmbofifixml

.28. _ . _ .0 88828 wddé 803228. U :5 80328.8. 3220822222285.

836— 8.8.3.81 mm. .5.

.8... 8 . _ .0 888228 wédé 80322.8. U :5 8038.8. 322082882285.

SwNN 38de- .28m. .89

.2... ~26 882228 w.c.m.v 80388. U 80> 8038.8. EnormEBS.

amNNd aged- .om. .om.

8.2.8.0 888228 wddé 8588. U _o> 80322.8. 3220822882285.

3.86 $86 .82. .82.
ouSSIESIoSIESaI

wglnomfiuammvifiomlonblfiofil
_32Iao_€o%fil2aomloablao2ul

8.6.8.888”

8..

3-158.585

2582888208028. .8922-
.ogml .8822-
I noo—
25.03.835.2848828230-
.v2omlaz 888.8% afimumv
8228 «222822.208 288222vo
bomglnufinouliogonol
25332222224888qu-
88222228108822.3282?-
0:8:02888-2828488235-
vofiofilacuaaudfinal

8.88..8282..-.882.8z 220.2 82.2222 .220 .82 582282.25.

151

2 822288.582I2on2222222I8—Io22wo2l

282 82828252825858.8862.

8888 2.22282 28.288.82.882-
28.2-82222282828\<8<22<8<82828.8+28822.88.82.
:088802onlaouoauxolm2lonuo2l

282888.22 2888-22822882288.82-8.22-282.

52.28.2228 Beau-8822882288-82da2282-

22228222 2268222822I22uwo28282~I82Io22uu2I

Boom aowgaalaowfiglmozmlfieal

8822822828 guacamlqouafimImozmIfiofiI

282:2 gfiaou928Imo228I8o2¢I
.8\2<8<828+<8<o22r.2

828.23 2288.2828<2.28888.82+2<8222288822.2.3 828.
822988-88828283-82-8.22282-

023 oEonumeuuanBIm—qucel

22222 8.282.588.2282??-

2222828 832I28088Io2222022me82122wo2I

288282 .2.-:8 8.2 2223 82822 2.2... .2.. 2.3.8.2 823882-22

8228 .28 28 2282822 82822222 88 0928— 88 3232 222222822 8228828228222
0222 <~<m 28 82822.2 829088-82 2220222222882 222.2 8223288802
.222 3222220 0222 8 222382.02 222 88 82228 .80 8&882288
..22 8.222.222.8288 2.22 8222.2 2288.2 82 2882282828 A 8.2
822 22388898 2225822222 0288. .<N<..8 22828922 20.2 Sou 8
208 ..8 22283 ...8 2222 82082222 028 .88 828088-8— 3223222268 .<~<..8
22o v83 028 m 282 8c fioqvoom 82228 MB 2888-x 8202238283
02E. 8282288892 .38. 282222892 <~<m .822 22292222qu
8838-3888-8882.

8.. 282202822ch228=222282Iw2222229228I

8.. 8oEaa2mI2a23o2oEIw22§29228I

.2882 828228282282

8.4838225. 2228:2888-8238:228Im222222222228.

.8882

828.522.2282 88882282828. 82228-85838.8.222...22228-
8.. nouosvo2Ia2~vafi2=quoI
2.. 22202222228822I=8Iw22822a2223I
8.. nowoozools22vlw22822a2228I
22288828? 828882.228.22222882.22-82282-
8888 222.288.223.882-

8888 282.22. 28.2.23... .3222-
8888 .28.- 828.22. 82282 #222222-
82.2 .228 Hmsoe 882282. .5222.
88 .322- -.2 .22822- 82282- .9828.
88- .228 .2 .22522 .8228. .5822.-
8 .aa- 22- 22.2.22 .....22282 .88-2222-

8- as. 2. 2222222 .8222 -..222222.

88 gun-...Emfitmfiuam
88- 222222 .2 228.222.882.522.-
8882 .8 222586828 >8 2.22282 .5222.-

2822 .o 822202232223 8. >22 banal gaw-
823 2222222222 Isal FEEI

8 .8 .8882. 822282222828 .8228-

8.. 022222 I222>2822222 #2252288 I§I

8 .58-28228282-8222888828-982222-
8 - 282.888.82.583m8222m
2.. 228222 2802 8222 29822822 282.582
2.. vofiofidgobaaofilggl
8.. IooFovIEoEBaaoEIEhva
8228288» 2388c3322922l22o2222€8I§I

.88... 2.82888 8:82.822. 82...... .822822282 .5222...
3.32 &bIco2282228I EEGI
88828.8 22222829283- 822222.22. E22222-

152

. . 8 22
8 2 22222: 2828822222 282228882 888.22. 282888.22 88 888
. . 8

22 8 2 22222: 2828822222 2822888822 888.22 282888222 88 888
. . 8

22 8 2 222282 2828822222 2822822822822 222288.22 282888822 88 888
. . 8 22

8 2 82: 28222822222 2822828222 222288.? 2828228822 88 288
. . 8 22 8

2 2228: 2828822222 22 228828822 888.22 282288822822 882 82222
. . 8 22 8

2 2225 282888.22 82282288822 888.22 28228882822 2222 82282
. . 8 22 8

2 2222222 282888.22 22 22888882 888.22 28228882822 8m 2822
..8888ono

222822 282222282222 282282288822 888.22 282288228222 222 82272
. . .28 22 8 628228.22

2222222 2222222282222 282282288822 888.22 282288228222 2m 8222
. . 8 22 8

2 2222222 282282222 822222882 888.22. 22 222228822 2m 8222
. . .28 22 8 88.22

222822 282288.22 2822828882 888.22 2822882282222. .22 8222
. . .28 22 8 282888.22

2222222 28228222222 2822828882 888.22 2822882282222. 2m 8222
. . .28 22 8 88.22

22225 2828282222 822882222 888.22 28228888822 .22 8222
. . .28 22 8 282888.22

222882 582822.22 822882 2 2.2 888.22 28228888822 282 22282
. . 8

22 8 2 22225 2828882222 28288822822 888.22 2222888822 282 8282

. . m 22
8 2 2228: 282882222 282888882 888.22. 282888822 2m 8222
. . m
22 8 2 2228: 2828822222 2822288222222 888.22 2828888222 222 8222
. . m 22
8 2 222882 282222222 282888822 888.22. 2828888822 222 8222
. . m
22 8 2 22282 28288288282828.8122 888.22 2828888822 282 2222
8222O2wl2o222o8222Io228IEo222I
2822280888I2o222o8222lo228l822o28I
8w2222l222022222co2Io228IEo28I
waclo2aolu228IEo28I
2822022222222E2I8bo§8lo228lfio2al
22022222288Iu228l228228l
o82>2I82228Io228IEo28I
>222220I2olo82IDIo228IEo222I
8I8£Io228IEo2aI
fi8£I828IEo222I
22.208.222Io228l222o28l
222222.28I I0228IEo222I
222222Io228I222o28I
I 2282
086 588I=88¢2228I82Io22uu2l
28.22 .2221.228>22222H22H8222282...
new: 228 m 220222922802 82 222.22
888.2 282.222.222.28222w822m22m8222282u
88222 .22 28H§8222w23w2w22228fl
mmn 2 .o .292 2322.2 MBI82Io22m28I
88822.22 28H2o2822.22.22.8222282.
32.22 22- 288.2 22 82 022228

153

222222.22 282288222222 222222.22 2822222222 282282222 282282282222 888
222222.22 2822822222222 222222.22 282222.22 2822222222 2228822222 888
222222.22 282288222222 222222.22 282822222 282822222 2228822222 888
222222.22

28288222222 222222.22 2822882222 2822222222 22228822222 8882
222222.22

2222228222222 222222.22 28228822222 282288222222 222222822222 82282
222222.22

282288222222 222222.22 28222282222 28228222222 222222222222 22282
222222.22

282222822222 222222.22 28228282222 28228882222 2228882222 882
222222.22

282222822222 222222.22 28228282222 28228882222 2228882222 8282
228.22

2222288222222 222222.22 28228882222 22228282222 222288822 2228
222222.22

222288222222 222222.22 2822282282222 22222822222 2822822222 8222
222222.22

222288222222 222222.22 2822282282222 2222222822222 2822822222 8222
222222.22

282288222222 222222.22 28228822222 28222882222 282222882222 8282
222222.22

222288222222 222222.22 28228822222 28222882222 282288822 8222
222222.22 282888.22 222222.22 2222 288822.22 2222288822 28282282222 8222
222222.22 28288222222 222222.22 2828822222 2828222222 2828882222 8222
222222.22 28288222222 222222.22 2828822222 2828822222 2822222222 8222
222222.22 282828.22 222222.22 22222822222 2828822222 2822822222 8222
222222.22 282888.22 222222.22 28282 222.22 2828822222 2222882222 2222
N2IDIo82228Io228I222822I

m2IDIo82228Io228IEo222I

MNIDIO8222¢I828IEO2¢I

mmIDIc822222Io228I8028I

NNIDIo82228Io228I8028I

2 2IDIo82228Io228I8o28I

222222Io82228I828I222o222I

I282

28888

28282.22 85 28228822 2828822 222288.22. 28288.22. 88 8288
:22 22 2 28282.22

228.5 222882222 282282822 2222228822. 2822822822.? 88 8288
. . 228 22 8 282822.22

85 2222882222 222228822 222288.22. 2822228822.? 88 8288
. . 8 22

8 2 2222282 2828822222 28222888822 222288.22. 2822882222 88 8288
. . 8 22

8 2 22222: 2222822222 2222288882 222288.22. 28222882222 88 8288
. . 8 22

8 2 22222: 282282282222 28228882222 222288.22 2828822222 88 8288
. . 8 22 8 2

2222222 28282 222.22 28222288882 222288.22. 282288828822 88 2288
. . 8 22 8

2 22225 2822822222 28228888822 222288.22 22222888822 88 22288
. . 8

22 8 2 2222222 2828822222 28222888822 222288.22 282888222 88 2288
. . 8 22 8

2 2222222 2828822222 28228222822 222288.22 28228888822 88 888
. . 8 22

8 2 2222282 222228882222 222222288282 222288.22. 282888222 88 2.88
. . 8

22 8 2 2225 22228822222 282222888822 222288.22 2822882822 88 2288
. . 8 22

8 2 2222222 2828822222 2822222282 222288.22. 282882.822 88 888

154

2.h . 28222828 22222 22222

2.. 8228 2 282228228 288 8222
2.. . 282228228 288 22222

2.... 2828888 8288 8222

2.. 8828 2 282228228 888 82222
8 . 282822228 888 22222

2.. 888 2 282822228 888 8222
8 . 282822228 288 8222

2.. 888 2 282822228 288 8222
2.. 888w. 28288228 888 8222
2.. 8822 8 28288228 888 8222
-2.. . 28282288 2288 8222

2.. 2288-2 2828288. 8288 82m
2.. 888 8 282228228 8288 8222
2.. 8888 282228228. 8288 8222
2.. 2288-2 28283.8 888 8222
2.. 888 2 28283.8 888 8222
m . 28222888 8288 82m

2.. 888 2 28282828 8288 8222
2.... 2828828 8288 8222

2.. 888 2 2828888 888 8222
2.. . 28222888 888 8222

m . 2828888 2888 8222

2.. 888 2 2828828 888 8222
2.. . 2828828 888 8222

m . 2822888 888 8222

2.. 888 2 2822888 888 8222
2.. . 28222288 2288 8222

2.. . 28222888 8.222 2222

2.. . 28282288 888 2222

2.. 888-2 2822.828 888 2222

2.. . 28282.8 888 2222

m . 2822888 888 2222

2.. 8228 2 2822888 888 2222

2.. . 2828888 22288 2222

waal2222222l22222222l222220wl

NIg§8I828IvnonIEoowl

00222228222I2222022I222220wl

NI2022222I0228I2222228I22222222I222220wl
2I2022222I0228I22222222I22222222I222220wl

#20222

80228222 .82 w222>222>222 82280 32282222280

222.2 220822 82 82280 2200 20 220222222022 202222222822 02.222222222222228
22< 5220222222228 2882820 2222 22052022 028 220222 220223

220822 2822222 028 8202022282822 2200 222 82280 22003202 8.222222222022220
28032222 22222822 22228 802w220 2800222228222 222 82280 .222 22222202222280
0222 222 82222222222222: 22222220022 222222 220228 0222 82280 2200 022.2.
2222222222 002282222220 2222.2 02.22 922822 2202222222280 028 2802222222 8.2
032 220032022 02w228 222222022222 0222 222 2280 0222 222002202 82280 22<
8228022I2u200228I222220wI

822.22 28 228822.22 coed 23225.22 23822.22 22222322222 282cm
222222.22 2822228222222 222222.22 282822222 282822222 282882222 8288
822.22

22.238226. coed 328222.22 2328.22 322228.822 ~20m
228.22

282288222222 222222.22 2822222222 22222222222 28228822222 2288
222222.22 2822222222222 222222.22 2822222222 282822222 2228822222 2228
222222.22 28222228.? 222222.22 28288.22 2822222222 2222222882222 2288
coed $2228.22 coed 288222.22 262 222.22 22222226 wow
228.22 28222.22 822.22 238 222.22 322286 $223.22 2.0m

222222.22 282 2828.22 222222.22 282822222 282822222 282882222 2288
222222.22 28222222222222 222222.22 282828.22 282822.22 2822882222 888

155

8 888.22 282228228 22.22 288

8 888. 2 282228228 8222 288

8 888 .2 28288228 882 288

8 8.88 2 282822228 8222 288

8 888-2 2822822288 8882 8822
8 888 2 282288288 82222 8822
8 888 8 2828888 888 8822

.22 . 2828888 888 82222

8 888 2 28282288 888 82222

.8 . 28288.8 888 8822

8 888 8 2828888 888 8.222

8 88828 2828888 2288 82222
8 888.8 2828888 2288 8822
8 88.8 28222288 22288 8822
8 8822 8 28222288 22288 8.222
8 8882 2822822288 8822 82222
8 888 2 282288288 82222 8822
8 8822 8 2828888 888 8822

8 . 2828888 888 8882

8 . 2828888 2288 82222

8 8228-2 2828888 888 8822

8 888 2 28222888 888 82222
-8 . 28222888 2288 8822

8 8882-8 2828888 2288 8822
8 2.8222 8 28282288 2288 8822
8 888-2 2822822288 2822 22222
8 888 2 282288288 22222 22222
8 888-2 2828888 888 2822

8 2288-2 2822.888 888 22222

8 82.28 2 28282288 2.88 2822

8 . 2828888 888 2822

8 8228-2 2828888 8288 22222
.8 . 2828888 8288 22222

8 888-2 28282288 22288 22222
8 888 2. 2828888 22288 2.222
8 8228 2 282228228 288 8222
m . 282228228 8288 8282

8 8228 2 282228228 8288 8222
m . 28288228 888 8222

8 8228-2 28288228 2288 82m
8 888-8 2828.8 8288 8222
8 888.8 28288.8 288 8222
8 88m 8 28288.8 288 8222
8 888-8 28222828 8288 8222
8 888 2 2828828 8288 22222
8 . 2828828 8288 8222

- 8 . 2828888 888 22222

8 888 2 282222888 8288 8282
8 . 282222888 8288 8222

8 . 28288.8 288 8222

8 8 28288.8 288 8222

m . 2828.8 8288 8282

8 8228-2 2822288 8288 82m
8 888-2 2828228 8288 8222
8 8228-8 28288228 2288 8222
8 888 8 28288228 888 8222
m . 28282228 8288 8222

8 8228-2 282222228 8288 8222
8 88m 8 282822228 8288 82m
8 8228 2 .28228888 8288 82m
8 8228 2 28288.8 288 8222
8 8 28288.8 288 8222

156

8 888.. 8 28288.8 8222 22288

8 88.8 8 28288.8 8.22 22288

8 888 8 22222822 82288 22288
- 8 . 22228.2 828 8288

8 888 .2 2822822228 882 8288
8 888 2 .282282888 8222 8288
8 888. 8 28288.8 8222 8288

8 88.8 8 28288.8 8.22 8288

8 888 2 282222888 22222 8288
8 888 8 282822.22 8288 8288
8 . 282822.22 22288 8288

8. 28288.22 :8 8288

8 888 2 2828288 8222 8288
8 888-2 2828828 8222 8288
8 8888 282228228 8222 8288
8 888-8 282228228 8282 8288
8 888 8 2822222228 8222 8288
8 8888 28288.8 82 8288
8 888 .2 2828888 2822 8288
8 888. 2 28282228 8222 8288
8 888 2 282222228 882 8288
8 888...8 28222828 8222 8288
8 8228-2 2828828 22222 8288
8 888. 2 28288228 8222 8288
8 888-2 282228228 8222 8288
8 888.8 2828888 8822 2288
8 8822.8 2828888 8822 2288
8 882-8 28282288 82222 2288
8 8228 8 2828888 8822 2288
8 888 28222288 8822 22288
8 2288 8 28222288 8822 22288

8 82282 2828888 2822 22288
8 888 2 28282288 22222 22288
8 888 .2 28222888 8822 2288
8 888. 8 28288228 8222 2288
8 2.88 .8 28288228 8222 888
8 888. 8 28288228 8222 2288
8 888.8 28288228 882 888
8 888-2 2828888 82222 888
8 228.8 2828888 82222 888
8 888.2 2822888 2222 888
8 888 .2 28282288 2822 2.88
8 888. 2 28282288 8222 888
8 888-2 282822228 82222 888
8 888 .2 2828888 82222 888
8 888. 2 28288228 8222 888
8 888-2 28288228 8872 2288
8 88.8 28282288 8822 888
8 888 2 2828888 22222 888
8 888..2 28222888 22222 888
8 888 .2 28222888 8222 888
8 888.2 2822888 8282 888
8 888 .8 2828888 82222 888
8 888-2 2828828 8222 888
8 8822-8 2828888 8222 888
8 8882. 8 2828888 8222 888
8 888 .2 2828888 2822 888
8 888-2 2822.28 2222 888
8 888-2 28288228 8222 888
8 888-2 28288.8 8222 888
8 8228-2 28222888 8222 888
8 888 2 282228228 22222 288

157

8 8.88-8 2.28-2 28288.88 8288 8222 888
8 888 8 88m 2 282288.882 8288 8222 888
8 8.88 8 ..222228888 8288 82m 8288

8 2288 2 8M8 2 22 22822.88 888 8282 888
8 888-2 2222282228 888 8222 8288

8 88m 2 22222822222 88 8282 8288

8 .888 2.. 2222282288 8288 82m 8288

8 888 2 888-2 28288.8: 8288 82m 888
8 888-2 . 282228.88 8288 8222 888

8 8228 2 . 222288.88 8288 8222 2288

8. 888 2 28222.88 8288 8222 888

8 . . 28288882 8288 8222 888

2... . . 222288.88 8288 8222 2288

8 888-2 . 282222288 888 8282 888

8 888 2 . 22222228822 88 8222 2288

m . . 22222228822 888 8222 2288

8 888 2 . 222228.88 888 8222 888

8 8.28.2 . .22 22882282 888 8222 888

8 8828 2 M88 2 28222.28 888 8222 888
8 8228 2 22222822822 888 8222 2288

-8 . . 282882.228 888 8222 888

8 . 888 2 22 22228.22: 888 8222 888

8 ... 2222282288 888 8222 2288

8. 888 222 2288.822 888 8222 888

m . . 2222288822 888 8282 2288

8 8228 2 222228888 888 8282 2288

.8 . . 2822888 8822 2222 888

8. 888 2 282228.882 8822 2222 888

8. 282228.882 82222 2222 888

8.. . 28288.88 8822 22m 888

8. 828 2 28288.88 8.222 2222 888

8 . . 282288.882 82222 2222 22288

8. 8228 2 282822.88 888 2222 888

8 . . 222288.88 888 2222 888

8.. . 222288.88 888 2222 888

8. 888 2 222288.88 888 2222 888

8 ... 22 222222.882 888 2222 22288

8 888-2 . 82288.88 88 2222 888
8.888 2.. 282222.282 888 2222 888
8 8828 2 8M8 2 282228.88 888 2222 888
8 888 2 . 222288.882 888 2222 22288
8 . . 282228.88 888 2222 888

8. 8228 2 222282.282 888 2222 888
8.. . 222288.882 888 2222 22288

8 . 888 2 282288.822 888 2222 888
8 . . 282288.88 888 2222 22288

8 8228-2 222288.88 888 2222 22288
w2222I22222221 02w228I222220mI
mlzbo22222228810228l02w2222l222220wI
2I28220222222288I0228I02w2281222220wl
02w228I222220wI
mI202282I0228I22222222I02w2222l222220ml
mI202282I0228I22222222I02w228I222220wI
2I202282I0228I2222228I02w228I222220mI
I2222222

8 8888 28288.8 8.22 8288

8 888 .2 2828228 882 8288

8 888-2 2828228 8282 8288

8 888 2 28288.8 22222 8288

8 888 8.2222282 2.2288 8288

8 888 .2 28288.8 8222 8288

8 888 2 28288.8 8222 22288

158

8 888.. 8 8 2828.88 888 8222 22288

- 8 88m 8 . 28288.88 888 8222 8288

8 888 m 888 2 28222222882 2.288 8222 8288
8 888 8 .888 8 2222222888 2288 82m 8288
8 888-8 888-2 2828.822 888 8222 8288

8 888 8 8.228 2 2828.88 888 8222 22288

8 888- 8 8 22222828 888 8222 8288
888-2 282288.222 8288 82m 8288
.888 8.22 2288.88 8288 82m 8288
8. 8m8 2 2828.228 8288 8222 8288
.888 2 2222288222 8288 8222 8288
- .8 . 8 22228.88 8288 8222 8288
8 8228 2 .888 8 222288.88 8288 82m 8288
8 8228 2 8228 2 2828.228 8288 82m 8288

8 888-2-888-2 2828.88 8288 8222 22288

8 M228 2 8 2222288222 8288 8222 8288

8 88.8. 8 888 2 2828.882 828 8222 8288
8 888 8 888-2 2222.882 8288 82m 8288
8 8.8.8-8 8 222222.882 8288 82m 2.2288

8 828 2 8.228 2 2822.82 8288 8222 22288

8 888 2 w 222222.82 8288 82m 8288

8 8828-2 8 28288 82288 8222 8288

8. 888 2 282822.882 2.222 2.2222 288

8. . 282822.882 2822 22222 288

8. . 62222.8: 22222 8222 8288

8 . 888 2 28288.88 2.222 8222 888

8.. . 28288.88 22222 8222 888

8 . 8228 2 282822.88 22222 22222 888

8 822m 2 .22 2288.88 288 22222 288

8.8228 2.. 222228.222 288 8222 8288

8 8828 2 888 2 2222288822 288 22222 888

on o.

:8.

8 8.88-2 2222288882 288 8222 888

8 8228 2 888 2 282228.88 288 8222 888

8 ... 22228.28 288 8222 8288

8 . 8228 2 222228888 288 8222 888

-8 . . 282228.88 288 8222 888

8 . 88.8. 2 222228282282 28 8222 888

8. 8228 2 2822822882 8288 8222 888

8.. . 282282.228 8288 8222 888

8 . 888-2 282282.228 8288 22222 888

8 888 2 . 282222888 888 22222 888

8 888.2 8882 282222888 888 8222 888
8 . 8228-2 282288.822 888 8222 888

8. 88m 2 222228.222 288 8222 288

8 . 8822 8 282288.882 288 8222 888

8 . 888-8 2828.88 288 8222 888

- 8 ... 222228828 288 8222 888

8 888 2 8M8 828288.88 288 8222 888

8 8228-2 88.2 8 282288.882 288 8222 888
.8 888.2 . 222228828 288 8222 2288

8 8822 8 88m 8 22 2288.88 888 8222 888
8 888-8 . 22 222222.228 888 8222 2288

8 888-8 . 22 2288.228 888 8222 888

8 8882 888-8 28288.88 8288 8282 8288
8 2288 2 888 m 28288.88 8288 8222 8288
8 2288-2 2288-2 28288.28 8288 8222 888
8 888 2 2288 2 28288.28 8288 8222 888
8 .888-2-. 282288.882 8288 8222 8288

8 888-8 888-8 22 2288.222 828 8222 8288
8 888 8 .2288 2 282288.882 8288 8222 888
8 888 8 888 2 28288.88 8288 8222 888
8 888-8 . 22222228822 8288 8282 8288

159

8 8888 8888 2228.82 8288 82m 8288
8 888 8 W88 8 2.2222882 8288 8222 8288
8 .888 8 .888 8 28288 8288 8222 22288

8 888 8 88m 2 2222222888 8288 22222 8288
8 888-8 . 2222222888 8288 8222 8288

8 8.88 8 28222282282 8288 22222 888

8 888 8 88m 2 2828.228 828 22222 8288
8 888-8 . 2828.88 8288 82m 8288

8 888- 8. 22228.88 8288 22222 22288

8 888 8 8 2828.88 8288 22222 8288

m 888-m . 282282222 8288 22222 8288

8 888 8 8M8 2 282222.228 8288 22222 8288
8 888 2 . 22 22822.88 8288 8222 8288

m 888 2 222222888 8288 28222 888

8 888 2 8882 2822.282 8288 22222 8288
8 88m 2 . 2828.88 8288 8222 8288

8 888-2 222228.288 8288 22222 8288

8 888 2.8 2828.82 8288 28222 8288

- 8 88m 2 . 28222.88 8288 8222 8288

8 888 2 8228 2 282288222 8288 22222 8288
8 ... 2222222288 8288 8222 888

8. 888 22828.88 8288 22222 8288

8. 2822.282 8288 82m 8288

8. 2828.82 8288 8222 22288

8 . 8 222228.228 8288 22222 8288

8. ..282288222 8288 22222 8288

8. 8228 2 222222.88 8288 82m 8288

8 . 8228 2 2828.88 888 22222 8288

8 . . 2828.228 888 8222 8288

8. 282228222 888 22222 22288

8. 8282228222 888 22222 82288

8... 2228.88 888 8222 8288

8. 888 2 2228.88 888 22222 8288

8 822m-2 2222.88 8288 8222 8288

8 8228 2 . 282222.88 8288 22222 8288

8 8228-2 8 2228.82 8288 8222 22288

8 888-2 282288222 8288 22222 8288

8 888-2 828-2 2228.22 8288 82222 8288
8. . 28222.82 8288 8222 22288

8 . 8 282222.88 8288 22222 8288

2... . . 28228.: 8288 22222 8288

8. 8828 2 282222.82: 8288 22282 8288

8. 828228 8288 822222288

- 8 . . 28288 22288 22222 8288

8 . 888 2 282222.228 8288 8222 8288

8 8. 2.8228228 82288 8222 8288

8 8.888 2 28288 8288 22222 8288

8.. 888 2 28228.82 8288 8222 8288

8 8228-2 8828-8 282282222 8288 82m 2288
8 8228 2 88m 8 282282222 8288 8222 2288
m 888 w . 28228.88 8288 8222 8288

8 822m 2 822m 2 28228.88 8288 8222 8288
8 8828 8 888 m 282288282 8288 8222 8288
8 888-2 888-2 282222.222 8288 8222 8288
8 8228 2 822-8 2 282222.228 8288 8222 8288
8 M88 2 .8 28228228 8288 82m 8288

8 888 8 888 8 282282228 2288 8222 2288
8 8.828 8 ..28222222882 2888 8222 8288

8 88m 8 88m 2 282822.88 2288 82m 8288
8 8228 8 .888 8 .2222222888 2288 8222 8288
8 888 8 822m 2 2828.882 888 8222 8288

8 8828-8 8228 2 2228.28 2888 8222 82288

160

8 888-2 2288-2 2828222282 22222 2822 22288
8. 88.8. 2 2822.88 8222 28m 888

8 . 888 w 222288.882 8222 2822 888

8 . 8228 2 28288.88 8222 2.222 888

-8 . . 222288.88 22222 22222 888

8. 888 2 282888222 8222 28m 8288

8.. . 282888222 82222 2822 8288

8 . 2288-2 282822.82 22222 22222 22288

8.. . 2288.2 282222222222 22222 22222 22288

8 828 2 .8288 2 222288.882 888 2822 888
8 8228 2 88m-2 282822.228 888 2822 888

- 8 88m 2 222288.228 888 2822 888

8 888 2 88m 2 2828.882 888 22222 8288
8 .888 2 282228.882 888 22222 8288

8 888-2 8882 28288.88 888 22222 22288
8 8828-2 2288-2 28288.88 88 2.222 22288
8 888 2 822m 2 222288.882 888 2.222 888
.8 8288 2 . 222288.882 888 2.222 888

8 888 2 88m 2 28288.88 888 2822 8288
.8 2288 2 . 28288.88 888 2822 8288

8 888-2 2288-2 222228.88 888 2822 22288
8 888 2 88m 2 222228.228 888 2822 22288
.8 888 w . 22 2288.88 888 2882 888

8 8228 2 M228 2 28288.8 888 2822 8288
m 888 2 . 282288.822 888 22222 8288

8 8228 2.888 2.2222228882 888 2822 22288
8 888 2 8M8 2 22228.88 888 22222 22288
8. 8228 2 282288.822 888 2.222 8288

8.“ . 222288.822 888 22222 8288

8 . 2288 2 282822.88 888 2822 22288

8 . 2288 2 222288.882 888 2.222 22288

8 8882 2222222228 8288 22222 8288

8 888-2 888 2 282288.882 8288 22222 22288
8 8228-2 2288-2 282228.822 8288 22222 22288

8 . 888-2 282228.822 8288 2822 22288

8 . 888 2 282288.882 8288 22222 22288

8 2288-2 2288-2 82228.28 22288 2822 22288
8 888-2 . 222228.228 288 8222 8288

8 8228-2 8228-2 222228.228 288 8222 8288

8 8228 2 . 22 22822.88 288 8222 2288

8 8228-2 888 2 22 22822.88 28 8222 2288

8 888-2 88m.8 28222882 288 8282 8288

8 82282 888.8 2:22.882 28 8222 8288

8 8228 2 88m 8 22222.82: 28 8222 8288
8. 8228 2 282222222222 8288 8222 8288

-8 . . 28288.88 8288 8282 8288

8. 8228 2 .2822228882 8288 8222 2288

8. 8M8 8 2828.88 8288 8222 8288
.888 8 2222222222 8288 8222 8288
8. 888-8 2828.88 8288 82m 8288
8 8.228 2 ..2822228882 8288 8222 888

8 888-2 888-2 28288.88 8288 82m 888
8 828-2 888-8 2828.88 8288 8222 8288
8 8m8 2 8M8 8 2828.88 8288 8222 22288
8 8228 2 888 8 .222222.2222 8288 8222 22288
8. 8228 2282222228888 8222 2288

8. 88m 8 2822.228 888 8222 8288

8. 888-828222.82 888 8222 8288

8.. 888 m 222228.88 888 8282 22288

8 8228 2 888 8 2822.822 228 8222 8288

8 888-2 8828-8 222228.88 888 8222 8288

8 8228-2 888-8 28222.82 2288 8222 22288

6.

161

8 8882 8882-8 22.228 8882 88m $8

8 82.8 m . 2258.25 8882 8882 808

-8 82.8-2 . 2888.228 88 8882 808

8 82.8-2 888-2 28288882 85 .8882 88
8 82.8 2 8828-2 288882282 8882 88m 808
-8 8228-2 . 28:882. 8882 8882 808

8 88m 2 88m 8 282822.82. 8882 88m 2208
8 888 w 88 m 22.28.2282 8882 8882 22am
8 8828 2 88m 8 222822.228 88m 8882 $8
8 888-2 . 2258.228 8882 8882 808

8 -888 2 . 282822.882 88m 888. com

8 888-2 888w 282822.228 88m 32 com
8 888 2 8m8 2 28888.82. 8882 8.882 888
-8 888-2 . 282828.882 8882 88m 808

8 888 w 888 m 22.28.2282 .8882 88m 2208
8 888 2 8% 8 2388.88 8882 88m 2208
8 888 8-. 2222288882 38 8882 808

-8 888 m . 228888.88 2.08 8882 88

8 88m 8 882m 2 2888.88 2.08 8882 88
8 888 8 88.8. 2 282882.882 $8 8882 8.08
-8 888 8 . 282882.882 2.08 8882 808

8 888-8 8888 2388.228 808 8882 2 208
8 888 8 88 8 28288228 2.08 88m 2208
8-. . 2818.882 New 8882 88

8 . 888 w 282288.882 808 88m 88

8. 888 2 2822.88 808 8882 808

-8 . . 2822.88 808 88 88.8

8 . 888-8 2882.88 808 8882 22am

8 . 888-8 2882.88 808 8882 22am

8 . 8828 2 222228888 88 82.82 com

8. 888-2 22225.8: 808 8.282 808

-8 . . 28288.88 88 8882 808

8. 8M8 8 68.88 com 88 22am

8. 8-8 8 2.8588882 88 8882 2208

8 8828 2 M828 2 28888.8 808 8882 808
-8 888-2 22222828822 88 8882 8cm

8 888 2 -888 8 882288.882 com 8882 22am
8 888 2 882m 8 €8.88 88 88 22am
- 8 882m 2 2222228228 808 8882 $8

8 88 2-888 P2228882: 808 8882 22am
8 888 2 88-8 2822.88 808 8882 2208
8 . 8882 8 2862.88 808 8882 22am

8-. 888-m 22 2288.2: 808 88 2208

8 8882- 8 8882- 8 28288.28 2208 88m 2208
8 88.8 2 82.8-2 2226222282 2882 2am 28m
8.. 888 m . 222228.228 2.82 2882 8282

8 888-2 888-2 222228.228 28m 2am 8cm
8 888 w 888 w 222228.228 28m 2882 8cm
8 888 2 8M8 228888.228 2am 28m 808
m 888 .2. . 282828882 2882 2am 8cm

8 888 2 8m8 2 28288818822882 8208
8 888 2 288882282 2882 28m 8208

8 888-8 888-.2. 282882282 2882 2am Sum
8 888 288.8. 2 282822.88 28m 2882 22208
8.. 82.8 m . 222228.288 2.82 2882 82m

8 82.8-2 888-2 222822.228 28m 28m 808
8 888-2 888-2 222228.228 2882 28m 808
8 82.8 2 888-2 2823.882 2am 2am 8am
- 8 88m 2 2388.228 2am 28m 808

8 888 2 8828 2 588.2282 2am 2882 822.8
8 8228-8 . 288882.82. 2am 28m 8208

8 888 2838 228882282. 2am 2.5 22208

162

8 88m: . @8828 88m 8am 808

8888 2-88 89888828882808

8 88m 2 88m 8 2388.82. 8882 8882 22am
8 82.8 888 M23832 8882 8882 2208
8 88m 2 8.8. 8 28828.82. 88m 8882 22208
8 82.8 2 888 8 282888.882 8am 8882 22208
8.. 888 .2. . 22.8 8822 88m 2282

8 888 2 88m 8 22.8 8882 88.82 808

- 8 8-88 2 . 28.8 8882 88m 808

8 888 2 88.8 2 28888.28 88m 88m 808

8 888-2 .28w2 2.882 8882 8882 808

-8 888-2 882 8 22.8 8882 8882 88.8

8 888 8888 M28283: 88m 88m 2208
8 88m 2 88m 8 28288.82. 88m 88m 2208
8 888 w 88 m 28882282 8882 8882 2228
8 888 2 888 -8 28228.82. 8882 8822 22208
8. 8882 8 28282882 2282 88m 808
8-. . €88.82. 2282 88m 808

8. 8828 2 282228.28 2282 88m 808
8-. . 28222.22‘ 25 8882 808

8 . ewe 8 28822.88 22m 8am 808
888-8 28228.82 :82 8882 2208
.88-8 2828.82 2282 88m 2208
.88-8 282822.282 2282 8882 2:08
Sm 8 2888.282 22m 88m 298
8 -888 8-. 225.2282 808 8882 808

8 888 8 882.8. 2 28888.2: 808 8882 808
-8 888-8 . 28888.2: 8am 8am 898

8 888 .8. Se m 222228.282 808 88m 808
8 888-8 888-8 28288.2 8am 8am 22am
8 888 8 88 8 28288.2. 8am 8am 2208

C‘- CM CM C‘-

8 8888 888 28: 2.8 808 8882 22208

8 888 8 888 m 28822.8 808 8882 2222.8
8. 888 2 2888.28 8am 88m 808

-8 . . 28888.28 808 8882 808

8 . 88 m 222288.822 808 8am 8cm

8 . 888-8 2888.88 808 88m 2228

8. Sm 8 2888.88 808 8882 22am

8 . 822-8 2388.882 808 8882 22208

8 . 888 m 2388.882 888 8882 22208

8... 888 w . 28228.88 808 8am 8cm

8 888 2 m8 8 2838.88 808 8am 8cm

8 8828-2-88 8 822223.882 808 8882 2208
8 8M8 2 8M8 8 28888.88 83 8882 22am

8 888 2 MS 8 “222288.282 808 8882 22208
8 888 2 2.8 M 288.28 808 8882 22298

8 . com 8 2858.88 808 8882 888

8. 8m. 8 28288.88 808 8882 22am

8. 88 8 822223.882 8am 88m 2208

8 . 9% 8 2888.28 808 8882 22208

8-. 888 .8. 282288.282 808 8882 2222.8

8 82828-8 888-8 2883.882 888 8882 22am
8 828 m 88 m 2883.882 2208 88m 2208
8 888-8 888-8 2888.88 8am 8882 2222.8

8 8m 8 88m 8 2888.88 808 8882 2:08

8 888-8 888-8 2388.228 :08 88m 2208
8 8M8 8 owe 8 2888.88 2208 8882 22208
8 888-8 8822-8 282282382 2 208 88 22208
8 88 8-88 P2825382 2208 8882 22208
8 888-8 888-8 2888.88 2208 88 222cm
8 88- 8 888- 8 28888.28 22208 88 222cm
8 8228 2 888 2 222282282 8.282 8882 88m

163

 

 

8 8288-2 8w8-2 238.22 8282 8cm 22

8 888 2 88m 2 222228888 8282 808 8282
-8 888 -2 . 22288.88 82m 808 8282

8 82.8 2 88m 2 8:88.88 8872 808 8282
8 82.8 -2 282288.88 8282 88.8 8282

8 888- 2 .22 2888.88 8282 808 8282

.28 8882 m . $2288.88 .8882 $8 8282

8 8822-8 82.8-2 222388.88 .8882 $8 8282
8 888-8 888-8 222222888. 8882 $8 8282
8 888 8 8% -8 82228.88 8.882 2.08 8282
8. 82.8 w 2228.88 8282 $8 8282

8. 8M8 8 2388.8 8282 $8 8222

m . 82.8-8 222258.882 8282 $8 8282

8 82.8 2 -888 8 822228.882 82m $8 8282
8 88m 2 88m 8 22.28288 8282 $8 8282
8 888 -8 82.8 -8 22 2288.88 8282 $8 8282
8 2.88 2 82m 2 28822.88 2.882 808 2282
-8 288-2 28822.88 28 808 2222

8 888-2 328-2 222388.88 2882 808 2.282
8 2.88 2 2.88- 2 22288.88 2.282 8.88 8.282
-8 82.8-2 222388.88 22m 808 2282

8 82.8 2-38 2 882288.882 22m 808 22282
8 82.8 2 288-2 2388.228 25 808 382
8. «m8 2 22.281228 2282 808 :82

8-. 888 w 282288.882 2282 88.8 2.282

8 38 2 888 2 22 228.88 2.282 808 2.282
8 . . 222238.88 88m New 8882

m . . 2832.88 8882 New 2282

8. 888 2 288.2282 88m 888 8282

8 . . 282282382 8882 898 8282

8. 282288.82 88m 898 2282

8 . 888-2 28882.88 88 808 82m

2". . 28882.88 88 898 8282

8. 888 2 22228.88 2282 808 8282

m. . 22228.88 25 8828 82m

8 888 8. 28252.88 85 808 8282

8. 82.8- 2 22:28.88 82m 208 8282

8 . 82.8 -2 22 $28.88 82m 208 882

8. 888- 2 222228888 82m 208 8282

8. 82.8- 2 22588.88 8.282 208 882

8. 888 2 282888.882 82m 208 8282

- 8 .-. $88.88 82282 208 8282

8 8..-8 2 8N8 2 28322.22 8.282 208 8282

8 82.8- 2 8228- 2 8:88.88 8282 208 8282
8 82.8 2-828 2-222288888 82m 208 882
8 888 2 M28 2 2388.88 8282 208 8282
8-888 2 282882382 8282 208 8282

8 82.8- 2 82.8-J 28:88.88 32 208 8282
8 82.8 2-888 2-8288888 22 298 882
8 82.8 2 8228 2 28888.88 82 208 8282
8 82w8-2 .2m2282..882 22 208 8282

8 82.8 2 82.8 2 28522.22 82m 208 882

8 82.8-2 88m-2 22 2228.88 8282 208 8282
-8 82.8 -2 222228.88 82m 208 8282

8 82.8 2 82M 2 222228.88 8.22 208 8282
8 8228 -2 22:28.88 82 208 8282

8 8.8.8 2 62:28.28 8282 2pm 8282

8 888 2 888 -2 22.2282 85 8882 8882

.8. 82.8 m . 22.8 8882 8882 22m

8 82.8 2 88m 8 22.8 8882 8am 8am

- 8-888 2 22.88.58.823

8 82.8 2 888 2 2882 2.882 8882 88m 808

164

8 . 888--8 2:83.32 8882 898 8282

8 . 888 8 22.282.28.32 85 8.98 892

- 8 .-. 28:88.88 8982 898 8282

8 888- 8 888- 8 22 288.22 8282 898 892
8 888- 8 888- 8 28:88.28 82m 898 8282
8 888 8 888- 8 28:88.28 8282 898 882
-8 888 -8 . 22 2828.88 8282 898 8282

8 888- 8 888- 8 28:88.28 82 898 8282
8 888 8 888- 8 28:88.28 82 898 892
8 888 8-. 22 2228.88 892 898 8282

8 888-8 888 8 22 288.22 8282 898 882
8 888--8 . 22 2228.88 8282 898 8282

8 888 -8 . 22 2228.88 892 898 8282

-8 8298-2 . 28228.88 88 898 8982

8 8298 2 88 8 2838.282 8982 898 8982
8 8-298-2 28:88.32 85 898 2282

8 888 2 8298-2 2388.88 8982 898 2282
8 . 888-8 282228.282 8982 898 8982

-8 . . 2888.88 8882 898 2282

8. 888 .2. 28:88.32 89m 898 2282

m 88 m . 28288.88 88m 898 2282

8 88 8 8298- 2 288829.88 8982 898 2282
8. 8298 2 282288.88 2282 898 2282

8 .8.v8-2 V22 2888.88 2982 898 2982

8 8298- 2 8298- 2 28288.88 28 898 8282
8 82.8 2 8-88 2 2888.88 2982 898 892
8 8298-2 . 28258.32 29m 898 8282

8 82.8 8 . 222882.282 2.82 898 8282

8. 82.8- 2 28258.32 25 898 8282

8 . 82.8 2 28258.32 2.282 898 892

8 . . 28288.88 2.982 898 8282

8 .-. 222288-2282 2982 898 8282

8 8298- 2 8298 2 22.8 8282 898 882

8 82.8-2 . 282288.88 8282 898 8282

8 82.8- 2 . 28:82.3 82m 898 8282

8 82.8-2 . 28:88.88 22 898 8282

8 82.8 2 28:82.28 82 898 8282

2.8. . 28:82.3 82m 898 8282

8 . 82.8 2 28:88.88 85 898 8882

-8 . . 288822.88 88m 898 8282

8 . 8298- 2 282888.882 8982 898 8282

8. 82.8 2 282888.882 88m 898 892

m. . 8:88.82 8982 898 8282

8 8.88 2 .-28:88.882 88 898 8282

8 82.8 2 82.8 2 288822.88 88m 898 8282
8 888-2 8-298-2 282822.88 8.98 898 882
8 82.8 28222288822: 8982 2298 82m

8. 8298- 2 28222.28 85 898 8282

8. 8298 2 22282.28 82m 898 882

- 8 . “.22 2888.88 8282 898 8282

8 82.8 2 8-298 2 2828.22 8282 898 892

8 82.8- 2 . 22 2888.88 8282 2298 82m

8.. 8298 -2 . 22 2288.88 892 898 8282

8 888 8 82.8- 2 222228888 8982 898 2982
8 888-..8 82.8- 2 282288.882 89m 898 82m
8 888 8 M28 2 6288.882 898. 898 8872
8 888 8 88m 2 2858.88 8882 898 8282
-8 888-8 . 2858.88 8882 898 8282

8 88.8- 2 82.8- 2 2222288228 2928 898 8282
8 8298 -2 8298 -2 28:88.88 25 898 892
8 82.8 2 88m 2 28882282 2982 898 8282
8 8298 2 . 2388.882 25 898 mm

165

8 888-4 82.8-J 28888.88 2.882 8298 82m
8 8298 2 8-298 2 28288.88 2.982 8298 892
8 888 2 . 22 28829.82 28 8298 2.282

-8 . . 28288.88 28 8298 82m

8 . 82.8- 2 282282.82 29m 8298 82m

8. 82.8 2 2:62.82 2882 8298 892
8.8258182 28m 8298 382

8 . 82.8- 2 28:88.28 85 8298 8282

8 . 8298 2 28:88.28 82m 8298 882

- 8. 22228.88 82m 8298 29282

8 82.8 2 8-88-2 2828.22 8282 8298 882

8 8298- 2 28:28.88 82m 8298 2.282

8 888 -2 28:28.88 892 8298 2.282

m 888 .8. . 222238.298 82m 8298 8.282

8 888-8 888-2 222258.298 8282 8298 82m
8 888- 8 82.8- 2 22 2888.88 8282 8298 8282
8 888 8 829m 2 22:88.88 82m 8298 892
8 88m 8 . 22 2888.88 8282 .8298 82m

8 888 8-. 282888.882 82m 8298 82m

8 . 888 w 22 22822.88 8282 8298 82m

8 . 82.8- 2 2822.28 8222 8298 8282

8. 888 2 2883.28 8282 8298 892

8. 282888.882 82m .8298 8282

- m . . 22 2288.88 8282 8298 82m

8 8828- 2 82.8- 2 282288.882 82m 8298 8282
8 888 2 82.8 2 282888.882 8282 8298 892
8 888-2 . 28:92.28 82m .8298 82m

8 888m . 22 £88.88 8222 8298 82m

8 8298- 2 82.8 2 22.22 8282 8298 892

8 82.8-2 28228.8 8282 8298 82m

8 888 2 . 22 258.88 8282 8298 82m

8 82982 . 28238.8 892 8298 82m

8 888 2 22288.88 882 8298 8282

- 8H 2228.88 8282 8298 82m

8 888-8 888-8 28888.8 825 2298 89m

8 8.8.8 8 8M8 8 28888.88 8.882 2298 88m

8 888 8 88- 8 2292888882 8982 2298 89m
-8 888 -8 . 2228.82 8982 2298 8282

8 888 8 -888 8 “292288.882 89m 2298 88m
8 88 8 8-8 8 28288.88 8.982 2298 89m

8 88 8 .-2o2§.82 88m 2298 82m

8 888-8 8m... 8 28288.28 8982 2298 89m

8 888-8 . 8:88.88. 8882 2298 8282

8-88 8-. 28:88.88 85 2298 82m

8 88 8 888 8 28288.28 8982 22298 8982

8 88-8-38-2-28223282 8982 22298 2882
8 88 8 2988 2 2828888 8982 2:98 2982

8 888-8 . 222222.82 8982 22298 2282

8 888-8 328-2 28288.88 8982 22298 2982

8 888-8 2988--2 282232.282 8982 22298 2982
8-888 8-. 222228.82 8.82 22298 2282

8 E8 2 2.88 -2 82228.28 2.882 22298 28
8 328-2 2823.88 2982 c298 2282

8 888-2 233.88 2982 22298 2282

-8 82.8 -2 22228.88 88 898 8982

8 82.8- 2 8828- 8 2:83.32 8982 898 8282
8 82.8 2 888 8 €23.32 8982 898 892
8 88.8 2 888- 8 2838.88 8982 898 8282

8 888-2 88-8 8 28298.88 85 898 892

8 82.8 2-. 222288.88 89m 898 8282

8 . 888- 8 28228.88 8.982 898 8282

8 . 888 8 23228.88. 8.982 898 892

166

8 82.8w. . 2828.8 8298 8298 8298

8 82.8 2. . 22.228 8298 8298 8298

- 8. 282228.88 8298 8298 8298

8 88m 2 82M 2 2828.22 892 8298 82m
8 82.8- 2 888- 8 2888.82 8.22 8298 82m
8 82.8 -2 888 -8 28282282 8872 8298 892
8 82.8 2 82.8 2 22.28.2282 892 8298 82m
8 m2.8-2 ...22.28.2282 8222 8298 8282

8 82.8 2 82M 2. 28288 8972 8298 8298
8 82.8-2 28288 882 8298 8298

-8 82.8-2 .2828 882 8298 8298

8 82.8- 2 888- 8 28282282 8282 8298 82m
8 82.8 2 888 8 28282282 8282 8298 8222
8 82.8-2 82.m-2 22.28.2282 8282 8298 8.282
8 .8.2.8 2 .-22.28.2282 8282 8298 82m

8 82.8 2 82m 2. 28288 8282 8298 8298

8 82.8-2 .28288 8282 8298 8298

-8 82.8-2 22.22222 8282 8298 8298

8 888 -8 888 -8 2828.22 8282 8298 882
8 888 8 82M 2 22.28.88. 8282 8298 8282
8-888 8.. 22.28.88 8282 8298 82m

8 888 8 82.m 2. 22.228 8282 8298 8298

8 88m 8 . 22.228 8282 8298 8298

8.888 m. 28282.2 828. 8298 8298

8 888 8 82M 2 22.28.88 892 8298 8282
8-888 8-. 22.28.88 892 8298 82m

8 888 8 88m 2. 22.228 8.22 8298 8298
8 88m 8 . 22.228 8.22 8298 8298

8 888 m . 28282.2 892 8298 8298

8- 82.8 2-. 2822.88 8282 8298 82m

8 82.8 2 82.8 2. 28288 8282 8298 8298

8 82.8-w . 282882 8282 8298 8298

8 82.8-2 282882 8282 8298 8298

8. 82.8 2. 282882 8282 8298 8298

8. 28288 8282 8298 8298

- 8. 28288 8282 8298 8298

8 82.8-2. . 282822 8298 8298 8298

8 82.8 v . 22.2282 298 8298 8298

- 8 .-. 22.2282 298 8298 8298

8 2.88 2 82.8 2 28288.88 2.282 2.298 8282
-8 2.88M . 28288.88 2.282 2.298 8282

8 288-2 888-8 28282.88 2.282 2.298 2.282
8 2.m8 2 82.8 8 28282.88 2.282 2.298 2.282
8 2.88 2 888--8 222288.882 2.282 2.298 8282
8 288-2 888 -8 282288.882 2.282 2.298 892
8 82.8-2 2222282288 8282 2.298 8282

8 82.8-2 888 8 222288.882 8222 2.298 2.222
8 82.8w 82.88 22.22828 8282 2.298 2.282
8 82.8- 2 888- 8 2822.88 8282 2.298 8282
8 82.8 2 888 -8 2822.88 8282 2.298 892
8.8.8.8 8 22.22828 8282 2.298 2.282

8 . 888 8 -22.2288.882 8282 2.298 2.282

8 . 888- 8 28282.88 85 2.298 8282

-8 . 888- 8 2382.88 8282 2.298 892

8 888 8 82.8 .8. 22 222.828 2.282 2.298 2.282
8 888--8 888- 8 28282.88 2.282 2.298 8282
8 888 -8 888 -8 28282.88 2.282 2.298 8.22
8 82.8- 8 888- 8 28288.88 2.282 2.298 8282
8 82.8 .8. 888 M23813 2.282 2.298 892
8 888 8 8.88 8 2828.22 8282 2.298 892

8 8N8 2 28288.88 2.282 8298 29m

8 82.8 2 22.228282 :5 8298 82m

167

828.22 mambfiemuawéam
22822.8- 222:2 8228929 82229 9222.292

88.8 .22-82289298223222.299-

88822 2E-s9e-a9229m22-2292-asampe22m

82.88- - 22a @9222 82299-228229-
hNad 2.38 805 85303.“ huh—mace £6

8 888-8 82.8-2 2828222 892 8298 882

8 88-8 8 82.-8 2 2828222 82272 8298 8282

8 888 8 82M 2 22222.88 892 8298 82m

8 888 8 .-282Voa8 892 8298 82m

8 888 8 82.8 8 22.282. 882 8298 8298

8 8888 . 22.282. 892 8298 8298

-8 888 -8 . 22.288 892 8298 8298

8 82M 2 82M 2 2828.22 892 8298 8282

8 82.8 2 82M 2 2822.882 882 8298 28282

8 M28 2 V2882..882 892 8298 8282

8 82.8 2 82M 2. 28288 892 8298 8298

8 82.8-2 28288 8.22 8298 8298

-8 82.8-2 . 28288 892 8298 8298

8 82.8 2 82M 2 2822.882 85 8298 8282

8 M28 2 V2822..882 8282 8298 8282

8 82.8 2 82.m 2. 28288 8282 8298 8298

8 82.8-2 . 28288 8282 8298 8298

8 88.8 2 . 28288 8282 8298 8298

8.. 82.8 m . 28228.82 282.82 8298 82m

8 82.8 2 82.8 -2. 28222.88 82m 8298 8298

8 82.8-2 2822.82 8282 8298 8298

8 82.8 2 2822.2 8282 8298 8298

8 . 82.8-2. 2822.82 8282 8298 8298

8. 28222.88 8282 8298 8298

8.. . . 2822.2 8282 8298 8298

8 82.8-2. . 28288 8298 8298 8298

8 82.8 2. . 22.288 8298 8298 8298

- 8H 22.288 8298 8298 8298

8 82M 2 88m 2 2828.22 882 8298 8282

8 82.8- 2 888- 8 2828.882 882 8298 82m
8 82.8 2 88..8 8 2828.882 882 8298 882
8.. 82.8 m . 22 228.882 892 8298 82m

8 82.8 2 82.8 2. 2228.88 892 8298 8298
8 82.82 28288 8222 8298 8298

8 82.8-2 . 28288 892 8298 8298

8 82.8-2 888 8 2828.882 8282 8298 82m
8 82.8-2 88-8-8 2828.882 8282 8298 882
8 82.8 m . 22 228.882 8282 8298 82m

8 82.8-2 82.8 2.-2o2x.88 82m 8298 8298
8 82.8-2 28288 8282 8298 8298

-8 82.8-2 28288 8282 8298 8298

8 888 8 88-8 8 2828.22 8282 8298 892
-8 888-8 . 2828.82 8282 8298 82m

8 888 8 82.8 -2. 22 228.88 8282 8298 8298
8 888 m . 22.222 8222 8298 8298

8 8M8 8 . 22.288 8282 8298 8298

-8 888-8 . 2828.82: 882 8298 82m

8 888 8 82.8 -2. 2228.88 892 8298 8298
8 888 .8. . 22.2822 882 8298 8298

8 8M8 8 . 22.288 892 8298 8298

8. 82.8 2. 222222.882 82m 8298 8298

8. 28288 8282 8298 8298

8. 2822.8 8282 8298 8298

168

2.. 82283-883881 22.222822284222on

2.. xglhlaonoobooJEoBaluqxol

2.. glhuqouoobooJEoBalznxol

2.. cab-22222282281282.582222-2222xon
$th 222.22-252022.208-22228228-222251
2.8-"24928829492289-
.3582: 2022. vofiglb283vl28§I=§ol
2.88.8 5229-8228929-258899-222289-

2.. 8aoEIb28aocl2S8bol2222xol
222282-2828I2S8Eol2282xol
2.2.22-98284388994922.29-
xglofi8l2~2§l22axol
528-288504282on
28222228829488.28122225-

822

2..
2..
2..
2..
2..

2.. glfiofllfiflaugmaofilaool
2.. Elana-22292295838423-
2.. 26822-822228I282oEo222822222-2231
ASSN 3382228822-2222222588922I223I

228
22.222828
8.8
22.22.88.882
8.228
2828 28.2 2
282282.828
22.288282

N18222222Ia222§81223|
328222312231
gum-03281228-
83Io2waal22uol
282222222Io2mdal22ool
8218223921228.-
8H5852-2299H

a 22.352 228

.8- 822+8 822....-.
.N- .8218- .8275.-.
.N- ..2 .22-.

.8.- ..2- .9.-.
.8 822.12- 822+...
.8 .822...2 822+...
.N S. .28.

.N S .22.

§xI3I8onl 32222018822828.28-

A282

2.. Silvana-22222236882818.5028

2..

mafia-2281.308528-

.2.. 2 . 2 6 2252 w.o.~.v 80222222. 0 2o> 80282282. 258222288222.

~a22.N owcmd- .80. .80.

.12 .2 .o 2292 deé 80222222. U :5 80222222. 238223.285.

23.02 8%.? .22—m. hm.

.2.. 2 . 2 .o 2288 wddé 8022282. D 20> 8022282. 22228223223222.

amNNd 22322.22. .om. .om.
§812a8lonb1588l

wglno2820228222l288lo8518o2al

2222-:028208282221238I I598.-
aauato8o2ul IESaI

2225.28- 1898.-

I382

88.8 2 2. 228293-8398-299289229-
bow mam M80.

2..
2..
2..

SAX-29.2w

82.8-22222502128225.2221
30282-8225828-2828220-
22223-83295-2822229229-
28888108348288.2220-
02282282281083.4830-
galaounaolufisal

2.0m882m880 M022 “824222 EU .82 aha—Zak:

169

8822 822222-2922258-82-922222-
22.:-<222.28222282<8<22<8<9.2..28.22+229.223898.
220288282xol22022o2222xol82Io22222I

282888822 289-8922982289-82-982292-

22382228 8582-8222239-82-982292-

22822222 2222222220bI2282w222222I82Io22uo2I

Scum gwo€>AI=Ou=2c8I8828I222°222I

829222229 5:088I220225208I8828I8822I

28.2222 2.2822281 22o22222o8l8o228I222o2¢I
.822<8<9.28+<8<o.22-.2

92922.: 2.2888882282822882 2.222+2<8<9.22<8<a22na 928.
8228022qu2222w2823|82Io22wo2I

028 022202208Iw222222w2o3I82Io22wo2I

22:2 92282-822285-82-9222292-

2229882 280I2o2o~2Io§o=b8I82Ioncfll

29982 2226 8222 2223 2222229 22¢. 28 2908822 822228.242

292222 .22 2229 22082222 2280222 822 99222 88 8232 222292222 8223228222228
928 <~<..2 220 22082222 820222.32 2222220222202 229.2 822292282202
.20 82292222 22222 9 2222222892222 2022 82 292222 .8... 2238,2982
.22 8822.22.292.29 .92 82.... 2.98.. 82 2,.8522828288 A .852
.229 228228888228 222292288222 022.2. («<82 222222922 282.2 29.208 3
208 82 22223 .22 2229 22082222 9222 .82 8288.2-m 28220222222228 .<~<..2
220 29082222 82.222 m E .222 888.50% 29228 ~23 238.242 220223203
2222.2. 82222228222 2.2 28222223 <N<82 .20 2228222282332
82282929-28299228-9222292-

2.. 282.288.22I22022822222222Im222222222228I

2.. 80.2222282wl2a2302922lw222222822228I

.2882 929.529.282

822.223.8228. 2892:9592-2829:228-8222299228-
.2882

19262928288828.282828. cones-92.229388822229228-

2.. 22o22022292I2222222Iw222222222228I

2.. 22222222022220.2I228Iw222222222228I

2.. 2229228228I222a29Iw222222222228I
222822282888 2.9288922289-29292289222-882292-
8888 28H2922§8H8222292H

8N: 2Ia2o2 2w222222222I 8222.292I

28.88 88222- -929.22- -8.22292 E22229-
882 222.22- -929.22- 8.22292- 2222-222.-

82 8.2.22- -2- -2222222 -.-.8.22292 82.2.2229-

82- .22...- 2 -22.2222 182292-5222.-

88 ..88- -.2.-. 22.2222 -8222292 422.2222.-
8. .22...- -.2- -22.2222 -8222292 48.82229-

88 .282..- -.2- -2222222- -8.22292 48222229-

88- 222.22- .2 -2222222- 8.22292 4.22222.-
28822. 22 8982222m28->8-8=222- 28.2.2229-

woB. 22 82220222222290 .22 >8 8222202I 22.5229.”
802mm 2222222222I 822228I 22.2222222I

8 .8-888H88538-822228-

8 9.2222 288292.22 -829292.2.928 -.22.2.222.-
8 222.59- 2.22.925 -82.282.2.828 4.2.2.2229-
8 29.28.... 829292.528 482.2222.-

2.. §I282I§I2o2uo2u22I222w2222I

22.. 2202220222I2220222022288222I§I

8.. uanou2>o22I2uoEoB8aoEI§I

8222228» 29822282282282I222922222298I§222I

.22... 2.92898 899.92-92.22. 9958-8988288-9e2u-
329: 92282892292298.4222?-

88222822 582.929.293-229228288-5229-

282888 23899892-2828288-922228-
82292929-28299a8-222289-

170

..8
2. 8 2 2228: 2828882222 22822.2 2828888822. 8228.22 .28 82228
..8

2. 8 2 2.28: 282888222. 2.88.2 28229888822. 2988.22 .28 22.28
..8

2. 8 2 28882 2828882222 88.22 282388822. 88.22 .28 222.28
2.2.2 22.29:

22.288882. 2822822822 28222888222 2832.22.88.22 .28 8.28
:2: 222.982

282288.22 2822828222 2828222822 282888822. .28 8.28
...2.2 2

2229: 282888.22 282222888822 282228282222 222288228822 .28 8.28
..8

2. 8 2 22.882 22.288822 282888822 88.22 282288888... .28 8.28
..8

2. 8 2 22...: 22.22.8822 282888.29 88.2. 28228882 2.22 .28 8.28
2.2.2 22228:

282888.22 22.382.88.22. 282222882222 2822.82.88.22 .28 2.228
...2.2 2

2228: 282888.22 232.282.82.22 28282288222. 28.282.22.822 .28 8.28
..8

2. 82 28822282888222. 8228.22 2828888829. 88.22 .28 8.28
...292 222.822

22.282832 28228888822 28222288222 28228882822 .28 2.28
2.2.2 22.2982

22.288832 28228828822 282822.222 22228882822 8o 880
...292 222.822

282888.22 28228288885 22.282.88.22 28228882822 80 880
2.2.2 2222.5

22.288832 28222888822 2982.82.22. 2222222222222 8o 880

. . 8 29 8 2 2.28: 28282.83. 888.22 22.282 22.22.22 8228.22 80 2.80
. . 8 2. 8 2 22.982 282888.22 2288.22 22.288832. 88.2. 8o 880

. . .29 2 2 22225

28288222... 28222288882. 2828882222 2222288888... 80 880
. . . 22 2 2 22282

233222.22 22.22.263.22 29382.22 8222.322 80 280
8222o2wI2o222o8222Io228I2229aI
.22QEo88aI2o222o8222Io228I222o222l
8w2222l222o222022ao2Io228I2223aI
wélo23Io228I22222222I
.2220222222222222I>bo222222288lu228I2229aI
>05308I828I222922I
oan82298I9228I222o222I
>2svoI2OIo82IDIo228I2229uI
8I2o29-22Io228I2229221
.2I2oa.2.,2I828I222292aI
xI2o£Io228IEo222I

2o22222228I I0228I222322I
222222Io228l222o222l

I2282

wood 22220222I2282¢2228I82Io22wo2I
82.8.2 -88.2.2-..82222.28H82H922..292-
2.8.2 228 m 2292228228822 82 one“:
2.8.2 22-28-29-889888-82-98222-
8888.22 28.292982-223-82-98229.-
22228.22 292-32982-223-82-9222292-
82822.22 2%....982-22-82-922222-
8222.2 .2. 228-wo2982-22H82H982292H
22 8222282802 2222222222 82 22228

288 8.929.225.2-2982888-82-9222292-

171

8 2-82-982228-9228-8929-

82-82-98299-9228-222928-

MNIDIo822222Io228IEo2nI

mmIDIo822222Io228IEo2aI

NNIDIo82228Io228IEo222I

2 2IDIo8222~Io228IEo2aI

2922222Io822222Io228IEo222I

A282

2.22. 2 282298.22

2228: 2922282229 22228222 282888.22- 282828922 98 8898
...22. 2 28223.22

2229: 22.22.222.22 28282.22 292882.822. 2822.883 98 2.898
2.229 2 282288.22

2.29: 28.22.222.22 2822892 282882.822. 2222228892. 98 8898
...2 29 2 282289.22

2.29: 2822.88.22 28:29.2 2922882288.? 282828922 98 8898
...22.222222.28.222229:

2822288222. 2222822822 2222288888.? 2828282922 98 2898
22229222229882.2229:

2822928222. 29282882 222228888822- 22.288282. 98 22898
...22.222222.28.222.29:

28222882222 292382.22 2228888822. 28222822222. 98 8298
...22.22222982..o2229:

282288.22 288288.22 2222282288822. 22.22.228.22. 98 8298
...2.2 2

2229: 282888.22 282888822 292898822 222288228822 98 8298
...2.2 2

2229: 2822.889... 282288822 22.282.292.22 28222988922 98 9298
...292 2

2.29: 2922982222 28288822 2922.82.82.29 28228988922 98 8298

. . .2. 2 2
222982 282889.22 2822.82.82 22.288.292.22 28228928822 98 2.298
. .8

2. 82 22.9: 282.22.222.22 88.2 282.898.222.882. 98 8298
. . .2. 2 2

222982 2822882222 282838.22 2922.82.82.22 28229288822 98 8298
. . .2. 2 2

298: 282888.22 282.28.28.22 22.22.988.22 28222888822 98 2298
. . .2. 2 2 222982

2829822222 2822289222- 292228882222 29228888222 98 22298
. . 8 2. 8 2 222922 2822.85.22 88... 2922282282222 88.22 98 898
. . .2. 2 2

2925 282298.22 2829.82.22 22.282882. 2922898822 98 898
. . .29 2 2

222982 282888.22 282282.22 28288882222 2922898822. 98 898
. . .2. 2 2

2229: 292888.22 28222882 2828888222 28228828822 98 998
. .8

29 8 2 2229: 292888.22 2822.88.22 88.22 282888822 98 898
. .8

2. 8 2 222.5 292888.29 2822288222. 88... 282892 2.22 98 2.98
. . .2. 2 2

2228: 22.22.8822 282888222 29288882222 22.228888... 98 898
. .8

29 8 2 2.2982 292822222 282.82.88.22 88.22 282828222 98 898
. .8

29 8 2 2228: 292829.22 2822.822. 88.22 2822228822 98 298
. . .2 2. 2 282882.22

2229: 28222882222 22.22.8882 292.28.228.22. 282888922 .28 2.2.28
...22. 2 282828.22

2.29: 282289822... 22.22 288.2 22.22.882.822. 2822.88.22. .28 82.28

172

282828.22 22 22888.22

282988.22 282282282222 222228.822 282222.822 22298
228.22

22.228.28.22 222922.22 292282.223 29228222222 282282.222 898
282988.22- 22 2282.28.22

2822.88.22- 282222.822... 22229822222 2822882222. 898

28282.82. 22222228822

282888.22- 2222822222. 222228829222. 2822228222 898
2828.28.22 282292222222

282298.22. 28222822222 22228822222 2822228222 998
822.22

282282.822 222222.22 22.222.88.22 29228822222 22.222.88.22 898
822.22

222282.822. 222222.22 282288.22 282282.222 22.228882. 2.98
282988.22.

2822.88.22 2822.88.22- 22222882222 2822.88.22 22 222283.22 898
228.22

282228822 228.22 22.222.98.22 282282.232 282288822 898
222222.22

282282.829 2.8.22 22.228882. 2822882222. 282228822 298
2832.28.29

2822229222... 28228982. 2828822... 282888.22 282822.22 2.2.28
282292822

- 282288222222 2822888.? 282288.22 282882.22 282888.22 82.28
222222.22

282282.822- 2.8.2. 28228882222 28228822222 282282.823 82.28
222222.22

292282.823 222222.22 2822.822 2822882222. 2822882222 22.28
222222.22

282282.829. 222222.22 2822888222. 2822822222... 222228882222 22228

2822.88.22
- 28282282222 282828.22- 28282282222 22228822222 22 222989.22 8.28
282822822
- 292828.22 2822.28.22. 282888.22 28222222922 282988.22 8.28
282898.22
282828.22 282882.22 292298.22 28282222922 292888.22 8.28
222222.22 282988.22. 222229.22 282298.22 282898.22 282828.22 9.28
222222.22 282988.22 222222.22 2822.28.22 22.22.288.22 2822 28.22 8.28

28288.22

- 292888.22 2822.88.22 2828.88.22 28282222222 28288.22 2.828
2822.98.22

- 2822.89.22. 2822.98.22- 28288.22 282888.22 282998.22 8.28
298.22

28229282222 822.22 28288.22 2822828222... 2822299822... 8228
2822.88.22

28282282229 288228.22 28292822... 28299222... 222282.832 2.28
2922.28.22

- 2828822222 292928.22 28298829... 28282.89 2828882222 880
2822222229.? 22222888222.

292828.22. 2228882922 22228882222 2822882222 9889
292888.22

28288222... 282888.22 2828982222 2828922922 2828282222 880
228.22

282282.822 222222.22 282222.822... 28228822222 22228982222 2.80
228.22

222228822922 228.22 222222822222 282222822222 282288822... 880
2828228...

282898.22 292828.22 282288.22 282288.22 2822282222. 880
292828.22

- 28228222... 292888.22. 2828882.... 2822.88.22 2828822222 26

173

8 9892-. 2828888 9298 880

8 989 9 2828888 998 880

I8. . 2339.2” mom N80

2.. one 9 292.98” Sum N80

2.. . 82233.8. oom N80

8 . 2828998 898 8889

8-. 2828888 2298 8889

8 889 9 2828882. 880 280

I8. . £2802. Sm 28D

8 889-9 2828882. 8.28 280

2.. 9mm 2 28238.8. mom 280

I8. . 282823.89. 229m 280

8 889 .9. 2822.888 2.298 2889

2.. 2.89 9 2332.48. com 280

8 . 2828898 898 280

8. 2222288998 8298 26

.....2828898 8298 280

2.. 2.99% 232.898 929m 280

2.. 93 2 2339.8 29m 280

32248221 2922022I2228mI

~I§§8Io228IVQBIEoomI

3222228229I2222o22I2228wI

~I2982222Io228IEo222I2922022I222°oMI
2I2o2292lo228I222292aI29222x2I2228wI

I282

892222222 .82 w5>2o>222 8298 32292222289

229.2 299822 82 82980 223 .222 22222222222922 20222222229822 89222982822222
22< 9822922222228 288.829 .222 29052929 2229 220222 220223

290822 2222229 9222 8292922282222 223 222 82980 2283222 82229222220228
28932222 222928.202 292222 892w2222 .882238229 222 82989 .22. 22022222222280
9.22 .22 82239292992 .....898 92.22 2.9.2.2 92.. 82999 2299 9.2.2.

imbue 0052.825 :3 05 mama: 22035228 0.3 Amend—Q d.—
032 22332022 2mg 2822922229 222 222 2980 9222 2223262 82989 224.
8228929I22228828I222oom-

29229289

- 22.298... 2822.99.22- 282298.29 282829.22 282899.22 8898
28288.22 22.22.222.22 282899.22 282829.22 22.29299 22.282922 2.898
28298.9

22.29822 2929229.? 292288.22 282929.22 282899.22 8898
282289822

22.228822 28288.? 282889.29 2822.29.22 282829.22 8898
282899.22

2822.89.22 2822.99.29. 282989.22 282889.29 282889.22 2898
282298.22

282929.22 282288292222 282829.22 282829.22 2822.89.22 9898
282899.22 282889.22 282899.22 282889.22 282889.29 282989.22 8298

2822.99.22

282829.22 2922829822 282929.22 282289.22 282289.29 8298
28282.89

282888.22 282928.22 282888.22 22282.89 22 229829.22 8298
2832.28.22. 28228889

222282822 282299292. 282288322 2922992222. 9298
22 228899.22 282282.299

28228892222 28228282222 2832.28.22 22.228829... 8298
282282822. 282222.89

2822288.? 22.222882. 282282.322 22.222.829.22 2.298
98.9

282282299899 292222.299 2922922922 282292822... 8298
22 222.82.22.22. 2822882922

28228882.. 2822882222 2822888922 292282.299 8298
2822.98.29. 282888.22

€328.22 223822.22 222233.22 ANCwNEd 220w

174

8 . 2928888 9298 890

8-. 2829988 8298 89.0

8 989 9 28:98.8 898 89.0
-8 . 2829898. 2298 86

8 889-9 2828898 8298 890
8 988 8 2829898 8298 86
-8 . 2829998 998 880

8 988-8 2829998 8298 89.0
8 989 9 2828898 9298 86
8 8 2929829 8298 96

8 m 29282 2.9 8298 96

8 988 2 2828899 8.28 990
m . 2828899 298 990

8 889-8 28298.8 8898 99.0
8 988-8 29298.8 8898 980
8 889-8 28288.8 9898 990
8 988 8 28288.8 9898 96
-8 . 2929988 9298 96

8 988 2 2828988 8298 990
-8 . 2828888 8298 980

8 988 2 29:88.8 9298 990
8 989-2 2828989 86 890
8 98m 9 2829989 8228 86
8 888-9 28288.9 8298 86
8 888 m 2929988 9298 89.0
8 989-9 2829988 898 890
8 989-2 2828888 898 880
8 88m 9 2829898 998 890
8 889-8 29599.8 2898 89.0
8 889 8 2928898 9898 89.0
8 . 20889.8 8298 86

8 988H2 2828888 9298 86
8 989 8 2828888 9298 86
8 989 8 2828829 298 96
-8 . 29882.9 298 990

8 989 9 2828829 898 99.0
.. 8 . 2828822. 898 96

8 989 9 282288899 898 99.0
8 . 282288899 8.28 980

m . 2829888. 2298 2.90

8 989 m 2829888 2298 96
8 989 8 2828888 898 980
8 . 2828888 898 990

-8 . 2829988 898 990

8 989 9 2829988 898 990
m . 2828829 8298 890

8 988 9 2828829 8298 890
-8 . 2828829 898 86

8 988 8 2829829 898 880
9 . 282288899 898 890

8 988 9 282288899 8228 890
8-9 28288.8 298 890

8 988 2 28288.8 298 86
8 988 2 2829888 998 890
8 8 2829888 998 880

-8 . 28:98.8 898 880

8 988-9 28:98.8 898 890
8 989 2 2828989 890 86
-8 . 2829289 898 89.0

8 989 9 2828289 2.28 890
8 . 28228.8 898 880

8 . 2828898 9298 890

175

- 8. 28298.8 9898 82.28

8 889 9 28229988 8898 8298
8-. 28229988 8898 82.28

8 889 9 29:99.8 2898 82228
-8 . 29:99.8 2898 82.28

8 899-8 2928898 9298 22228
8 899 m 2928898 9298 22228
8 889 9 28288.8 8898 2:28

- 8. 28288.8 8.898 2298

8 889 9 28228988 8898 2298
8 . 28228988 8898 22.28

m . 2928898 9898 2 2228

8 889-9 2928898 9898 2 298
8 999 8 28:99.8 8298 92.28
8 99m-8 28:99.8 8298 92.28
8 998-8 28228988 9898 92228
8 999-9 28228988 9898 92228
8 998-8 29228288 8898 9298
8 999 9 29228288 8898 92228
8 9 2928898 9298 92228

8 .-292889.8 9298 92228

8 889-9 2828889 290 9228

8 988 2 2828899 980 9228

8 . 2829298 998 998

8 . 2829888 9298 9828

8-. 2829888 8298 9228

8 989 9 2829989 86 8.28

8 . 2828298 998 8228

8 . 2829888 898 8228

8 9 282888 9298 8.28

8 . 2828298 8298 8.28

8 989-9 2828888 898 8228
8. 2898988 2298 8228

8 . 2829998 898 9.28

8. 28:99.8 8298 9.28

8 8 28:99.8 8298 9.28

. 2828298 998 898
8 2829988 898 898
2829988 898 8.28
. 2829898 998 9228
. 2829988 898 9.28
. . 2829988 298 9.28
. . 2828998 898 9228
2829898 898 8228
. 2828888 898 8228
. 2828898 898 898
8. 2828998 8298 898

8 899...8 2928998 9298 8228
8 99.8. 8 2928998 9298 898
8 898-8 29229988 8898 8228
8 999-9 29229988 8898 8.28
8 898-8 29228988 8898 8228
8 999 9 29228988 8898 898
m . 2928998 8298 898

8 988 m 2928998 8298 8.28
8 989 9 2828289 86 2.28

8 . 2829298 998 298

8. 28:88.8 9298 2.28

8-. 28:88.8 8298 2.28

8 889 9 2828889 290 890

8 . 2828989 8.28 890

8. 28298.8 8298 890

c o- o- c~- c» en

en c» c» o

176

8 99m-8 28292.98 86 8298
8 898-8 29:98.8 9298 8298
8 898 8 2828898 8298 8298

8-. 2829899 9298 8298

8 989-9 2898888 880 9298

8 989 9 2829898 890 9298

8-8 2928998 898 9298

8 988-2 2828988 980 8298

8 889-9 2828898 890 8298

8 88m 9 2829898 290 8298
8 988 .8. 2822998 92828 8298

8 888-9 2929998. 880 9298

8 889-9 2829888 290 9298

8 988-2 29:88.8 96 9298

8 988 2 2828888 880 9298

8 m 2998898 22228 9298

8 8M9 9 2829988 880 8298

8 889 9 292288998 290 8298

8 889 9 2828298 8228 8298

8 8889 2828299 880 8298

8 989 9 2828898 890 8298

8 m 2929998 82.28 8298

8 988-2 2829988 890 9298

8 988-2 2829998 280 9298

8 989 2 2828888 880 9298

8 m 2829988 898 9298

8 989-2 2829888 880 998
8 989 9 2829888 880 998
8 9 292288998 890 998
8-9 2828298 8.28 998

8 988 2 2828899 290 898

8 9899 28:98.8 880 898

8 989-9 2828888 898 898

8 989-9 2822.998 86 898

8 889-9 2829988. 290 998

8 989-9 2828888 89.0 998

8 888-9 2829898 89.0 998

8 989 8 2828888 96 898
8-8 289898 8.28 898

8 988 2 2899888 890 998

8 8 20988.8 880 998

8-8 282988 928 998

8 988 8 2829829 890 898

8 8 2828898 898 898

8 989-8 2828829 990 298

- 8 8 2829988 998 298

8 898-8 29:98.8 8298 92228
8 889 M 288288 9898 92228
8 988 2 29299.8 9898 92228
8 898H8 2929898 9298 92.28
8 889 m 2828898 2898 92228
8 988 2 2922 2.8 8898 92.28
8 8899 2829888 2898 8298
8 898 8 2899888 9298 82228
8 8988 2828898 8298 82.28
8 889 9 2828298 9898 8298
8 . 29288.8 8898 82.28

8. 29289.8 8898 82.28

9. 2828982 92.28 82228

8 899-8 2929998 8298 82.28
8 899 .8. 2929998 8298 82.28
8 889 9 2898.8 9898 82.28

177

 

 

 

8-. . 28288.99 2298 26 8298
8 . 88m 9 28288.29 :98 26 8298

8 .-988 2 -29298.882 2298 26 9298

8 889 9 88m 9 29298.99 9298 26 998
8 8M9 9 . 28299.98 9298 29.0 898

8 889-9 . 28282882 9298 290 8298

8 -889 9-. 28289892 9298 280 8298

8 889-9 889-9 2822999 9298 290 8298
8 889 9 988-2 28298.89 9298 290 9298
8 889-9 . 28299992 998 280 898

8 889 9 . 29288.8... 998 26 8298

8 -889-9-. 299288.982 998 29.0 8298

8 889-9 889-9 29298.89 998 290 8298
8 889 9 988 2 29288.89 998 26 9298
8. 29282882 898 26 8298

8 . . 28289.99 898 290 8298

8 . 889-m 28298882 898 26 8298
8.988 2 28299.88 898 26 9298

8. 28288.98 8298 280 8298

8. 88m-92892828 8298 290 8298

8 . 988-2 29298982 8298 290 9298

8 .889 m 28299892 8298 26 8298

8 .988 2 2992.98 8298 2989 9298

8 889-9 988-2 28989982 8298 290 9298
mac-32287929284223»-

ml§o§8lo228I92w§I222oowl
2I>bo§>8lo228lo2w§|8°oml
93228-2228»-
812382-9228|Ec2alo2w2222lfiooml
ml2ona2|o228l222o28|o2w228|2228m|
2I2382Io228l222°28|o2m228|2228m|

-.282
8 9888 28282.9 990 8898

8 999 8 28282.9 990 8898

8 998 8 -2922828.8 92.28 8898
8 988 2 2922 2.8 92228 8898
8 899-8 28298.8 96 9898

8 M88 8 2888.8 96 9898

8 998 8 28228988 92228 9898
8 988 2 29299.8 9298 9898
8. 2-2 22988.9 8898 9898

8 899-8 29298.9 990 8898

8 9M8 8 29282.9 990 8898

8 898 8 29228988 8.28 8898
8 899-8 28298.8 990 8898

8 9M8 8 29298.8 990 8898

8 898 8 29229988 8228 8898
8 .-2222828.9 8898 8898

8 899 8 2999829 96 2898
8 899-8 2999998 86 2898
8 8899 2829888 82228 2898
8 889 m 2828898 9298 2898
8 899-8 2998929 990 9898
8 89m 8 2929898 86 9898
8 889-9 2828288 9228 9898
8 889 9 2828298 8298 9898
8-. 2928999 2898 9898

8 899-8 2982 2.9 990 9298
8 99m 8 2829898 880 9298
8 898-8 2829888 82228 9298
8 898 8 2929898 92.28 9298
8 899 8 2929829 96 8298

178

-8 9899 . 28288.89 9298 89.0 898

8 989 9 98m 9 28292.99 9298 86 8298
8 989-9 . 28228882 9298 890 998

8 989-9 . 28288892 9298 89.0 898

8 989 9-. 28298.88 9298 890 2298

-8 989-9 . 2989.88 998 89.0 898

8 989 9 989-9 29288.89 998 86 8298
8 98m 9 . 29228.89 998 880 998

8 98m 9 . 29292882 998 89.0 898

8 989 m . 28999882 998 89.0 2298

8 .989 9 28288882 898 8889 8298

8 . . 29299982 898 89.0 998

8 . . 29299.99 898 890 898

m . . 28298.98 898 89.0 2298

8 98m 9 . 28289.88 8298 890 998

8 98m 9 . 28988282 8298 890 898

8 989 9. 28988982 8298 880 2298

8 . . 28288.98 998 880 898

8. . 29289882 998 86 2298

8-. . 29298.98 898 890 2298

-8 889 m. 29299.98 8889 290 898

8 889-9 889-9 29288. 29 880 29.0 9.28
8 889 9 .9.88 2 29298.89 86 290 898
8 -889 9828299892 86 26 2298

8 889 m 889 m 2922 2.89 86 29.0 9298
8 889 9 8M9 9 28289.89 86 290 998
8 889-9 . 29299282 86 29.0 898

8 88m 9 . 29288.99 86 290 8298

8 -889 9-. 28988.8: 890 29.0 8298

8 889-9 889 9 28298.88 89.0 290 8298
8 889 9 988-2 29228.89 86 26 9298

8 . 889-m 28288982 898 290 9228
8 .988 2 28988.88 8.28 280 898

-8 . . 2998.88 8.28 290 2298

8 .889 m 28288892 898 29.0 9298
8. 889 9 29288882 8.28 26 998
8 . . 28928.88 8.28 290 898

8 . . 2989.98 898 290 8298

8-. . 29289.98 898 29.0 8298

8. 88m 9 29299.89 8228 290 8298
8-. 988 2 29282882 898 29.0 9298
8 889 9 9.8.8 2 28988992 998 26 898
8 -889 9-. 29288882 998 26 2298

8 889 m 889 w 2888.88 998 290 9298
8 889 9 8M9 9 28298.98 998 29.0 998

8 88m 9 . 29999982 9.28 290 898

8 889-9 . 29288292 9228 280 8298

8 -889 9.“ 29289282 9228 290 8298

8 889-9 889-9 29298.88 9.28 290 8298
8 889 9 9M8 2 29282.89 28 29.0 9298
m 988 2 . 29289.9: 898 26 2298

8 988 2 -889 9 28288882 898 290 9298
8 988 2 8M9 9 29282.89 898 26 998

8 988-2 29289882 898 290 898

8 988-2 28289.98 898 280 8298

-8 988-2 . 28299.28 898 26 8298

8 988 w 889 m 28299292 898 280 8298
8 988 2 9M8 2 29298.29 898 29.0 9298
8.889 m 28289.8: :98 280 9298
8.889 928288.282 2298 290 998

8. 29228.89 2298 290 898

8. 28988.29 :98 290 8298

179

8 988-9 288-9 29288.88 8.28 86 898
8 9 988 2 29298.2: 9298 880 9298

8 9 988 2 29289882 9298 89.0 998

8 9 8 29288.89 9298 890 998

8 m . 29298.99 9298 890 898

8-9 988-9 29298.88 9298 890 898

8 988 2 9-88 2 29288.89 9298 890 998
8 988 2-8 292828.882 9298 890 998

-8 988 2 . 29298.88 9298 89.0 898

8 988 2 98-8 9 2998.99 9298 880 898
8 988 -2 8 2888.8: 998 89.0 998

8 -988 2-. 29288282 998 880 898

8 988 2 988 9 28288.89 998 86 898
8 8 . 28988.89 998 89.0 898

8 8 9889 29288282 998 890 898

8. 98-8 9 29299.8: 898 890 898
8-989 2-. 29288882 890 86 8228

8 989 2 9M9 9 29299.89 86 89.0 298
8 989 2 28282892 880 890 898
2989-2 . 29289.99 86 86 9298

8 989 2 989 229299.89 890 86 9298
8 989 2 98m 9 28288.89 86 890 998
-8 989-2 . 29282.98 86 890 898

8 989 2 989-9 28298.88 89.0 890 8298
8 98.22 2 . 29288.98 86 890 998

8 982 2 . 282222.892 89.0 880 898

8 989 2-. 29288282 890 89.0 2298

8 . 989 9 28289982 828 890 2228

8. . 29299.88 8228 890 898

8-. . 28298992 8.28 880 9298

8.989 9 2992.982 898 890 9298

8 . 989-9 29228892 8228 89.0 998

-8 . . 28289.89 898 890 898

8.989 9 29289282 8228 880 8298

8 . . 28989.88 8228 86 998

8 . . 29289.99 898 880 898

-8 . . 29229.89 8.228 86 2298

8 989-9 . 28988982 2228 89.0 898

-8 989 m . 2888.89 2.28 880 9298

8 989 m 989 2 28229.88 2228 890 9298
8 989 9 9.8.9 9 28289.88 2.28 86 998
-8 989 m . 29298892 2.28 890 898

8 989 9 98m 9 2889.88 2.28 86 8298
8 989-9 . 29289292 2.28 86 998

8 98m 9 . 29282882 2.28 880 898

8 989 9 . 29289.8: 298 890 2298
8-. . 29292.2: 898 86 9298
8.989 9 28929.8: 898 890 9298
8 . 989-9 28299982 898 86 998
8-. . 29292982 898 890 898

8.989 9 28282.99 898 880 8298

8 . . 2889.99 898 86 998

8 . . 2898.88 898 86 898

-8 . . 29289.89 898 890 2298

. .989 9 28288982 9298 86 9298
8 . 989 9 29288.89 9298 86 998
-8 . . 29289.89 9298 880 898

. .989 9 28998992 9298 89.0 8298
8. 28288.29 9298 890 898

8 . . 28289.89 9298 890 898

8. 29299882 9298 86 2298

8 989-9 989 9 29229.29 9298 89.0 998

o

C‘

180

8-. . 29288.88 2 298 990 898

2 . 989-9 29288.99 :98 99.0 898

8 989 9 929 8 2988.99 2298 99.0 898
8 989 m . 29289882 2298 990 898

2 989 w . 29288.99 2298 990 898

8 989 9 98m 9 29288.88 :98 990 898
8 989 m . 28982.2 22 898 990 898

-8 989-8 . 28282.89 898 990 898

8 989 8 989 9 29298982 898 99,0 898
8 .-. 29298982 898 96 898

8 . 989 9 28282.89 898 990 898

8 . 929-9 29298.9: 898 990 898

8 .988 9 28289882 8298 880 8298

2 . . 28289.88 8298 890 898

8 .988 8 29288982 8298 890 898

8-. . 29299.98 8298 890 828

8 .988 9 2988.99 8298 86 828

8 . 2 28298922 8298 86 9298

8 .988 2 2889.99 8298 890 9298

8 . 988 2 28289.89 8298 890 998

8 . 8 29289.2: 8298 89.0 998

2 . . 28289.88 8298 880 898

8 . 98m 9 29288982 8298 890 898

8 -988 9-. 29288982 8298 890 898

8 988 9 98m 8 28289.88 8298 890 898
2 988 m . 29288.99 8298 890 828

8 988 9 9-88 9 29299.98 8298 86 828
-8 988 22 9 28289.99 8298 86 9298

8 988 m 988 2 28298.9: 8298 890 9298
8 988 9 988- 2 29289222 8298 890 998
8 988 9 8 28289.89 8298 890 998

8 -988-9-. 29288982 8298 89.0 898

8 988 9 988-9 28289.88 8298 890 898
8.988 8 28292.9: 898 890 898

2. . 29298.88 898 890 828

8 .988 9 28289892 898 89.0 828

8-. 9 28298.29 898 880 9298

8 .988 2 29288882 898 86 9298

8 . 988 2 29229.99 898 86 998

8 . 8 28289.98 898 86 998

2 . . 2988.29 898 890 898

8 . 98m 9 29298882 898 86 898

8 -988 8-. 28289892 898 890 828

8 988 8 -988 9 29298.88 898 89.0 828
8 .8288 8 2 29988882 898 86 9298

8 988 m 988 2 28298.28 898 86 9298
8 988 8 98-8 2 28289.98 898 890 998
8 988- 8 8 28229.98 898 890 998

8 -988 8-. 29298882 898 89.0 898

8 988 8 98-8 9 29288.29 898 89.0 898
8.988 9 28298982 828 890 828

8-. 9 29299.98 828 86 9298

8 .988 2 29289982 828 89.0 9298

8 .988 2 29992892 828 89.0 998

8. 8 29228.88 828 880 998

2 . . 29288.88 828 890 898

8 . 9-88 9 29289282 828 880 898

8 288 9 2 29289982 828 880 9298

8 988 m 988 2 29299.98 828 89.0 9298
8 988 9 9-88 2 29228.88 828 890 998
8 988 -9 8 29292892 828 86 998

8 988 9 . 29289282 828 880 898

181

8 8882-8 982-2 22 2299.98 2898 890 9298
8 889 8 989-2 282292.992 2898 89.0 9298
2 889 2 . 22 2289.88 9898 86 8298

8 88m 8 98m 2 292289.89 9898 8889 9298
8 889 8 989 2 282228.992 9898 890 9298
8 . 98m 2 2889.98 8298 880 9298

2 . 989-2 28299982 8298 89.0 9298

8 988 2 989 2 2828.882 9298 86 9298
8 2289 8-. 28299.9: 298 980 298

8 989 8 929 9 2829898 298 96 898

2 989 2 . 29292982 298 980 898

8 989 8 989-9 28289992 298 990 828

8 98m 8 . 29298.88 298 990 828

-8 989-8 . 28282.29 298 990 2298

8 989 8 -989 9 28298982 298 96 2298
8 989 8 98m 8 29288.99 298 96 898

8 98m 8 . 28299.98 298 980 898

8 -989 8-. 29298882 298 96 898

8 989 8 98m 9 29288.99 298 990 898
8.989 9 29292982 298 980 898

8-. . 28298.98 298 980 898

8 . 989 9 29298.88 298 990 828

8 . . 28289992 298 99.0 828

8 .-. 28298982 298 980 2298

8.989 228282.29 298 990 2298

8 . 989 8 28299.98 298 980 898

8 . . 29288.99 298 980 898

2 . . 29288.99 298 990 898

8 . 98m 9 29298882 298 96 898

8-989 9-. 28299882 898 99.0 898

8 989 9 989 9 29289.89 898 96 828

8 989-9 . 29298.98 898 980 828

8 2289-92 28289.8: 898 980 2298

8 989 m 989 2 28288.89 898 990 2298
8 989 9 929 8 29298.89 898 99.0 898
8 989-9 . 29289.2 22 898 980 898

8 -989 9-. 29928.882 898 980 898

8 989 9 989-9 28298.88 898 980 898
8.989 9 29298.98 898 980 828

8 . . 29289.89 898 96 828

2 . . 28288.89 898 990 2298

8.989 m 28289.8: 898 99.0 2298

8 . 989 8 29289.2 22 898 99.0 898

8. . 29298.89 898 99.0 898

2 . . 28298.88 898 980 898

8 . 9822 9 29228882 898 990 898

8 98m 9 . 28289982 828 980 828

8 -989 9-. 29288982 828 99.0 2298

8 989 w 989 2.. 29288.98 828 96 2298
8 989 9 929 8 29298.88 828 990 898
8 989 m . 29289992 828 96 898

-8 989-9 . 29299.88 828 990 898

8 989 9 989 9 29289282 828 99.89 898
2 . . 2988.98 828 980 2298

8 . 989 2 29288982 828 990 2298

8 . 989 8 29289992 828 980 898

8 . . 29298.88 828 990 898

8 .-. 29289282 828 96 898

8 . M89 9 29299.88 828 990 898
8.989 2 29288.82 :98 96 2298

8 . 989 8 29289882 2298 990 898

8 . . 29288.99 :98 980 898

182

8 . 982-2 29298.9: 9298 96 9298
8-988 2-. 28298.9: 8298 96 8298

8 988 2 988-2 28292.99 8298 990 9298
8 .-988 2 28288.88 8298 990 9298

8 98m 2 9882 9 28989.98 86 890 828

8 98m 2 882 9 28288.89 86 890 8298

8 989 2 -888 9 29289892 890 890 9298
8 989-2 989-9 28229.89 86 890 898

8 989-2 989-2 28288.89 880 89.0 998

8 M89 2 288 9 29289.99 89.0 8989 998

8 989-2 889-8 292289.892 8.90 89.0 2898
8 989 2 889 2 292288.922 86 890 9898
-8 989-2 . 29298.89 86 880 8298

8 989 2 988 2 28289282 890 890 9298
8 989-2 989-2 28299.88 86 89.0 9298

8 98m 9 882 9 29289.89 828 890 8298

8 989 9 -888 9 29298882 828 880 9298
8 989-9 989-9 29299.88 828 86 898

8 989-9 989-2 29298.98 828 890 998

8 289 9 288 9 29298.89 828 890 998

8 989-9 889-8 292289.882 828 86 2898
8 989 9 889-8 292298882 828 890 9898
2 989 m . 29298892 828 880 8298

8 989 m 988 2 28298882 828 89.0 9298
8 9M9 9 929 2 28228.88 828 890 9298

8 888 m 888 2 28998.82 8298 890 9298
8 888 m 989 m 282922.982 8298 890 898
8 888-9 989-2 2999.89 8298 89.0 998

8 828 9 828 9 29288.98 8298 890 998

8 888-9 889-8 292298.99 8298 890 2898
8 888 9 889 8 292288.88 8298 89.0 9898

-8 8889 . 28288.29 8298 86 8298

8 888-9 988-2 28299882 8298 890 9298
8 888 m 989 2 28289992 8298 890 9298
8 888-9 989-9 28229822 9298 890 898
8 888 m 989 2 29298282 9298 89.0 898
8 8M8 9 828 9 29288.99 9298 890 998

8 888-9 889 8 22 2282.88 9298 890 2898
8 888 9 882-8 22 2299.89 9298 89.0 9898
8 -888 9-. 28288982 9298 89.0 8298

8 888-9 988-2 29289.89 9298 880 9298
8 888 9 -989 2 28229.99 9298 89.0 9298
8 98m 9 98m 2 2889.99 898 89.0 8.98

8 929 9 828 9 28288882 898 890 998

8 989-9 889-8 22 2298.982 898 86 2898
8 989 9 889 2 22 2299.992 898 89.0 9898
2 989 .9. . 28298.89 898 880 8298

8 989-9 988-2 28288.88 898 890 9298

8 989 m 989 2 29289.98 898 880 9298

8 M89 2 288 9 28228.8 998 880 998

8 989-2 889-8 22 2289.282 998 890 2898
8 989 2 889 2 22 2298.882 998 890 9898
-8 989-2 . 29299.28 998 890 8298

8 989 2 988 2 28288992 998 880 9298
8 98.9. 2 98m 2 29299.89 998 890 9298

8 888-9 889-8 22 2229.98 998 89.0 2898
8 888 9 88m 8 22 2298.98 998 890 9898
2 888 m . 282289.982 998 890 8298

8 888 m 988 2 28292882 998 890 9298
8 828 9 929 2 29288.99 998 86 9298

8 889 8 88m 8 292298.92 2898 89.0 9898
8 889 8 . 22 2299.29 2898 890 8298

183

8 8 2 2998.82 8298 990 9298

8 8 988 2 29288.99 8298 96 928

8-8 . 2988.98 8298 990 228

8 8 889 2 2828.282 8298 99.0 8898

8 8 982 8 2898.98 8298 980 8898

8 8 889 2 2829.82 8298 990 9898

8 8 988 8 2928.89 8298 990 9898

8 2 . 29288.88 8298 990 9298

8 8 988 2 2989.99 8298 990 8298

8 2. 292298.922 8298 990 8298

8 8 988 2 222282.982 8298 96 9298
8 8 988 2 29298.88 9298 990 928

8-8 . 2988.89 9298 990 228

8 8 889 2 2898.2: 9298 99.0 8898

8 8 982 8 2829.99 9298 980 8898

8 8 889 2 2829.882 9298 990 9898

8 8 988 8 2922.88 9298 990 9898

8 2 . 2989.89 9298 980 9298

8 8 988 2 2988.88 9298 96 8298

8 2. 292289.882 9298 96 8298

8 8 988 2 292289.822 9298 990 9298
8 2.88 2.2892 2.982 928 980 228

8 982 2 882 8 2998.88 928 980 8898
8 988-2 988-8 2928.992 928 980 8898
8 988 2 889 2 2828.892 928 990 9898
8 988 2 2.88 8 2828.88 928 96 9898
8-988 2-. 28289282 928 96 9298

8 988 2 928 2 2898.88 928 990 8298
8-988 2-. 28288282 928 990 8298
8 988 2 988 2 28988.88 928 990 9298
8 . 889-8 2899.892 228 990 8898

8 . 9888 2999.88 228 990 8898

8 . 882 8 2829.98 228 96 9898

8 . 988 8 2829.992 228 980 9898

2 . . 2889.88 228 990 9298

8.988 2 28288282 228 99.0 8298

2. . 28288.88 228 980 8298

2 . 988-2 28298982 228 96 9298

8 889 2 988 2 2929.8: 8898 99.0 8898
8 889-8 889-8 2929.98 8898 990 9898
8 889 8 928 8 2828.98 8898 990 9898
8 889 8 . 2829.882 8898 990 9298

8 889-8 988-2 2929.89 8898 96 8298
8 889-8 . 2822.282 8898 96 8298

8 889-8 988-2 2928.89 8898 96 9298
8 988-8 8898 2928.98 8898 990 9898
8 988-8 982 8 2829.88 8898 99.0 9898
-8 988-8 . 2829.99 8898 980 9298

8 988 8 988-2 2822.882 8898 990 8298
-8 988-8 . 2928.89 8898 96 8298

8 988-8 988-2 288.882 8898 990 9298
8 889 8 988-8 2922.8: 9898 990 9898
8 889-8 . 2828.99 9898 96 9298

8 889-8 988-2 2828.882 9898 99.0 8298
8 889-8 . 2929.99 9898 980 8298

8 889-8 982 2 2829.282 9898 990 9298
8 -988 8-. 2928.882 9898 99.0 9298

8 988 8 928 2 2898.89 9898 990 8298
8 -988 8-. 2822.882 9898 96 8298

8 988 8 982 2 2829.89 9898 99.0 9298
8.988 2 2828.88 9298 96 8298

8. 28289.99 9298 990 8298

184

8 889-9 929-9 28299.98 26 890 898
2 889 2 . 28299.99 290 890 2298

8 829 9 829 9 29229.99 26 880 8298
8 889 9 988 8 292289.992 290 89.0 9298
- 8 829 9 . 28998.98 280 89.0 998

8 889 2 988 2 292288.922 29.0 86 8298
8 889 9 989 9 28282882 26 890 9298
8 . . 29289992 828 890 8298

8 . . 29288982 828 880 9298

8 .-. 2999.88 828 890 8298

8 . 989 9 28298.98 828 880 898

8-. . 29299.88 828 86 2298

8.829 9 2992.99 828 890 8298

8 .988 8 292288.982 828 880 9298
-8 . . 29299892 828 89.0 998

8 .988 2 222282.282 828 880 8298

8 . 989 9 28998.9: 828 890 9298

8. . 28289.9: 8298 890 9298

8-. . 29299.99 8298 880 8298

8 . 989 9 28288292 8298 880 898

8 .-. 28999882 8298 890 2298

8 . 882 9 2882.29 8298 86 8298

8 .988 8 292228.99 8298 890 9298
-8 . . 2989.99 8298 890 998

8 . 988-8 292229.98 8298 880 8298
8.989 9 28288882 8298 890 9298

8 . .-28229.882 9298 890 8298

8 . 989 9 2889.89 9298 890 898

8.2 . 28299.8: 9298 890 2298

8 . 889-9 28289882 9298 890 8298

8 .988 8 22 2298.88 9298 86 9298

-8 . . 29228.29 9298 890 998

8.988 2 22 2988.89 9298 890 8298

8 . 989 .9. 29289.89 9298 890 9298

8. 989 9 28299.89 8298 890 898

8-. . 2888.89 8298 890 2298

8.829 9 29288.98 8298 890 8298
8.988 8 22 2292.982 8298 880 9298

- 8 . . 2888.89 8298 890 998

8.988 2 222292.882 8298 890 8298

8 . 989 2 28289882 8298 89.0 9298

-8 989-9 . 29299.29 898 86 2298

8 982 9 882 9 28299882 898 880 8298
8 989 9 988 8 -22 2289.882 898 890 9298
- 8 989 9 . 28292.88 898 890 998

8 989 2 988-2 22 2298.982 898 890 8298
8 989 9 989-9 28299982 898 890 9298
8 . 829 9 2889.89 2298 880 8298
8.988 8 222288.892 2298 890 9298

-8 . 28292982 2298 89.0 998

8.988 8-22 2298.892 :98 890 8298

-8 . 982 9 28229.98 :98 890 9298

8 889 9 988-8 292298.99 8298 8989 9298
..8 889-9 . 28289982 8298 86 998

8 889 2 988 2 222282.88 8298 880 8298
8 889 9 982 9 28289.88 8298 89.0 9298
-8 988-8 . 292289.98 9298 880 998

8 988-8 988-8 292299.82 9298 89.0 8298
8 988 8 989 9 22 2289.88 9298 890 9298

8. 982-8 2 2: 2.8 3 82m 2298

. -8 982.9 28282882 998 829 9298
8 988 8 989 9 29298.89 8298 880 9298

185

8 . 8 282298.99 8298 928 8298

8. 8 2888.89 998 828 898

8. . 2888.89 998 828 898

8 8 . 22 2228.99 898 828 898

8 . . 29989992 998 928 898

8. . 2888.29 998 928 298

8 . . 2889.88 998 928 898

8 . . 2898.99 898 928 298

8 . . 2888.88 898 928 898

8. . 29299.89 298 928 898

8 . . 29298282 880 828 898

8. . 29299.99 86 828 898

8 . . 28298982 86 828 898

8. 28228882 890 828 8298

8 . . 29298982 898 828 898

8. . 2889.99 898 828 898

8 . . 2889.88 898 828 8298

8. . 2888.99 898 828 898

8. 28292.98 898 828 8298

- -8 . . 2989.89 898 828 8298

8 899 2 998 2 29288.98 9298 828 9298
8 899 2 898 2 288.982 9298 828 8898
8 829 8 929 9 2829.89 9298 828 8898

8 899 8 -898 8 28229892 9298 828 8898
8 899 8 299 9 2828.89 9298 828 8898

2 899 2. 29228.88 9298 828 8298

8 899 8-988 9-28229989 9298 828 8298
8 992 8 89.8.. 8 2829.89 9298 828 8898

8 998 2 999 2 288.982 9298 828 8898
8 9.9.8 8 828 8 2828.89 9298 828 8898

8 998 8 999 9 28229892 9298 828 8898

2 998-2 . 282299.89 9298 828 8298

8 998 8 .988 9 29288.88 9298 828 8298
8 898-8 999-9 2829.99 8898 828 8898

8 898-8 898-8 2828.92 8898 828 8898

8 898 8 929 9 2829.99 8898 828 8898

2 898 2. 28222.98 8898 828 8298

8 898 8 988 9 28229.99 8898 828 8298
2.

8

999-9 8988 2899.99 8898 828 8898
2.99 9 929 9 2828.92 8898 828 8898
2 2.99 2. 28299.99 8898 828 8298

8 999-9 988-9 28222.98 8898 828 8298
8 898 8 992 9 29228.29 8898 828 8898
-8 898-8 . 2828.88 8898 828 8298

8 898 8 982 9 29228992 8898 828 8298
8-999 9-. 28228992 8898 828 8298

8 999 9 988-9 2828.88 8898 828 8298
8 .988 2 288.882 8298 828 8298

8 989-9 . 28299.29 86 228 990

8 982 9 . 28298.98 86 228 998

8 989-9 . 28299.29 86 228 9298

8 989 9 . 28288.88 86 228 8298

8 . . 28288982 980 228 998

8. 28229.99 96 228 9298

8. . 28298.99 96 228 8298

8. 29298.89 998 228 9298

8. 292292.89 998228 8298

8. .-222298.99 9298228 8298

8 8822 9 . 28289.99 290 89.0 828

8 882 9 . 28288.89 26 86 8298

8 889 2 . 29228992 280 880 9298

8 889 9 . 28299.89 26 86 8298

186

8 999-8298-8-28229892 8298 9228 8898
8 999 82.2.9 9 2828.89 8298 9228 8898
8 2.99 -8 9 2829.89 8298 9228 9298

8 2299 8 .-292298.88 8298 9228 9298

8 992 8 992 8 2898.99 8298 9228 9898
8 998 2 999 2 2829.882 8298 9228 9898
8 928 8 928 8 2828.89 8298 9228 8898
8 998 8 99-9 9 28229892 8298 9228 8898
8 998 .8 9 292298.88 8298 9228 9298

8 -998 8-. 282229.89 8298 9228 9298

8 998 2 999 2 2928.89 9898 9228 9898
8 998-8 998-8 2829.92 9898 9228 8898
8 998 8 9.99 9 2829.29 9898 9228 8898
8 998 -8 9 28229.88 9898 9228 9298

8 -998 8-. 2822.89 9898 9228 9298

8 999-9 998-8 2829.29 9898 9228 8898
8 999 9 2299 9 2829.92 9898 9228 8898
8 2.99 -9 9 2822.89 9898 9228 9298
8-999 9-. 28229.88 9898 9228 9298

8 998 8 9-99 9 2829.29 8898 9228 8898
8 998 -8 9 28222.89 8898 9228 9298

8 998- 8 . 28229.28 8898 9228 9298

8 999 -9 9 28229.28 8898 9228 9298

8 999 9. 28222.89 8898 9228 9298

-8 9 . 2228.982 9298 9228 9298

8 889 9 98.8. 2 28288.98 26 928 96

8 882 9 . 28289.99 26 928 998

8 889-9 . 28299.29 26 928 9298

8 889-9 . 28298.88 26 928 8298

8 988-2 . 28282982 990 928 998

8 988 2 28299.99 99.0 928 9298

8 988-2 . 2888.99 990 928 8298
8. 222299.99 998 928 9298

8 . . 292288.89 998 928 8298

8. .-222282.99 9298 928 8298

8 989-9 . 28229.99 86 828 86
8 989-9 . 29288.98 86 828 998
8 98-9 9. 29289.89 86 828 898
8 989 9 9 29299.88 86 828 9298
8 . . 28289992 880 828 998

8. . 28998.89 86 828 898

8 . 9 28289.89 86 828 9298

8 . . 28282.99 998 828 898

8 . 9 28299.89 998 828 9298

8 . 9 29288.89 898 828 9298

8 . . 29299.98 26 828 890

8 . . 29299882 280 828 990

8-. . 28289.88 26 828 8298
8.989 9 28289982 280 828 898
8 . . 28989.88 28 828 2 298

8 . . 28298.99 86 828 980

8 .-. 29922.99 86 828 8298

8 . 989 9 29289.98 86 828 898
8 . . 29288.88 86 828 2298

8. .-28298.982 990 828 8298

8 . 989 9 29299.89 96 828 898
8-: 28289.89 99.0 828 2298

8 . 989 9 2899.99 8298 828 898
8-. . 2888.89 8298 828 2298

8 989 9 . 2928.89 898 828 2298
8 . . 28299.89 898 928 8298

8 . 8 2899.89 898 928 8298

187

8. . 2829.8 8898 8228 8898

8. 298.882 8898 8228 9228

- 2. . 2829.882 8898 8228 9228

8 899 2 899 2 29282.88 8298 8228 8298
8 899 8 889-9 2892.982 8298 8228 9898
- 8 892 8 . 2829.29 8298 8228 9898

8 899 8 889 2 28228892 8298 8228 8898
- 8 892 8 . 2928.89 8298 8228 8898

8 899 8 882 9 28:89.89 8298 8228 2898
8 8-99 8 28288.88 8298 82282898

8 899 8 829 9 2829.29 8298 8228 9898
8-899 8 . 2822.982 8298 8228 9898

8 899 8 289-9 2928.89 8298 8228 8898

2 899 2. 28228892 8298 8228 8898

8 899 8 882 9 28288.88 8298 8228 2898
8 899 8-. 282289.89 8298 8228 2898

2 889 2 . 2829.89 9898 8228 9898

8 889 9 88.9. 9 2829.92 9898 8228 8898
-8 889-9 . 2829.29 9898 8228 8898

8 889 9 882 9 2229.88 9898 8228 2898
8 889 9-. 2:29.29 9898 82282898

8. 889 9 2829.29 9898 8228 8898

2. . 2829.92 9898 8228 8898

8.889 9 22229.29 9898 8228 2898

8-. . 2:29.88 9898 8228 2898

-8 889-9 . 2998.29 8898 8228 8898

8 889 9 882 9 28229.89 8898 8228 2898
8 889 2 . 28229.28 8898 8228 2898
8.889 9 28229.28 8898 82282898

8. 28229.89 8898 82282898

8 889-9 . 2829.882 2898 8228 2898

8 8998 8998 292289.88 9298 2228 9298
8 899 8 889 2 28222892 9298 2228 8898
-8 899-8 . 2929.99 9298 2228 8898

8 899 8 889-9 2829.882 9298 2228 8898
8 829 8 . 2829.29 9298 2228 8898

2 899 2. 282998.88 9298 2228 9898

8 899 8 -889 9 282299.89 9298 2228 9898
8 899 8 289 9 2929.99 9298 2228 8898

8 8-99 8 282.892 9298 2228 8898

8 899 8 829 9 2829.29 9298 2228 8898

8 899 8. 2829.882 9298 2228 8898

8 899-8 . 282299.89 9298 2228 9898

8 899-8 889-2 282298.88 9298 2228 9898
2 889 9. 2829.88 8898 2228 8898

8 889 9 882-9 2829.92 8898 2228 8898

8 88.9. 9 . 2898.98 8898 2228 8898

8 889 9 . 28299.88 8898 2228 9898

8 889-9 889-2 28229.99 8898 2228 9898
8. 889 9 2828.98 8898 2228 8898

8 . . 2829.92 8898 2228 8898

8-.. 28229.99 8898 2228 9898

8 . 889-9 28229.88 8898 2228 9898

8 882 9 . 2928.89 8898 2228 8898

2 889 2 . 28229.98 8898 2228 9898

8 889 9 889 9 2828.98 8898 2228 9898
8-. . 2828.98 8898 2228 9898

8 . 889-9 28229.98 8898 2228 9898
8 . 882 9 2829882 9898 2228 9898
2 998 2 29228.98 8298 9228 8298
8 998 2 2829.882 8298 9228 9898
8 999-8 999 9 2828.99 8298 9228 9898

2.2839
2..

188

8 8 . 292289.982 8.90 998 928

8 8 . 28292882 890 998 828

8 8 . 292999.88 928 998 928

8 8. 2892.88 928 998 828

8. . 28992.8 928 998 828

8. . 29982.88 99.0 898 890

8 . . 29289.88 96 898 928

8 . . 28299982 990 898 828

8 . . 28298.99 86 898 928

8 . . 29989992 890 898 828

8-. . 28289.89 928 898 828

8 .988 8 28228.99 86 898 880

8. 8 292298.882 8.90 898 828

-8 . . 29299.98 89.0 898 828

8 98-8 8 8 29299.98 86 898 828

8 988 8 . 292298.882 880 898 828

8 2 . 282228.89 828 898 828

8 929 8 . 28299.99 96 298 980

8 989 8-. 292289.882 980 298 928

8 989 8 8 29289.98 96 298 928

8 . . 29289.98 96 298 928

8 . 8 292289.882 990 298 928

- 8-. 8 282298.89 928 298 928

8 892 8 882 9 2828.98 8298 9228 9898
8 892 8 982 2 2929.8: 8298 9228 9898
8 898 8 -898 8 292298.92 8298 9228 9298
8 892 8 882 9 2829.99 8298 9228 2898
8 898 8 988-2 2929.8: 8298 9228 8898
-8 898-8 . 2828.89 8298 9228 8228

8 889 2 988 2 2929.8: 9898 9228 9898
8 889 9 898 8 2822.99 9898 9228 9298

8 889-2 889-2 282288.92 9898 9228 2898
8 889 9 988-2 2829.2 22 9898 9228 8898
2 889 82 . 2828.89 9898 9228 8228

8 988-2 898-8 2928.89 9898 9228 9298
8 988 2 889 .9. 2922.89 9898 9228 2898
8 988 2 288 2 2829.9 9898 9228 8898

8 -988 222828.982 9898 9228 8228

8 898-8 889-9 2828.89 9298 9228 2898
8 898 8 982 2 2928.89 9298 9228 8898
2898 2. 2899.88 9298 9228 8228

8 889 9 982 2 2828.89 2898 9228 8898
8 882 9 . 2829.88 2898 9228 8228

8 -988 222828.982 8898 9228 8228

8 889-9 898-8 2829.98 2898 8228 9298
8 829 9 828 8 2828.99 2898 8228 8298
8 889 9 889-9 2929.92 2898 8228 9898
8 889 9. 2828.2: 2898 8228 8898

8 889-2 . 2828.2 22 2898 8228 8898

- 8 8882 9 . 2828.89 2898 8228 9228

8 898 8298 8 292298.92 9298 8228 8298
8 898 8 889 9 2822.99 9298 8228 9898
8 8988 . 2829.82 9298 8228 8898

8 898 2 . 288.992 9298 8228 8898

2 898 2. 2898.89 9298 8228 9228

8 898 8 882 9 2829.89 8298 8228 9898
8 898-8 . 2828.89 8298 8228 8898

8 898-8 . 2822.99 8298 8228 8898

8 898-8 . 2829.88 8298 8228 9228

8 889-9 . 2829.29 9898 8228 8898

8 889-9 . 2922.89 9898 8228 8898

8 889 9 . 2829.98 9898 8228 9228

189

8 . . 28298.99 89.0 998 828

- 8 9-. 282228.29 828 998 828

8 988 2 929 9 29282.88 26 898 890
8 988 2 . 28298992 29.89 898 96
8 988-2 . 28298.89 26 898 890

2 988 2. 28229.28 26 898 928

8 988 2 929 9 28299.29 26 898 828
8 989 .9. . 28289892 880 898 980
8 929 9 . 29298.88 88 898 880

8 9-89 9 .-292228.882 880 898 928
8 989 9 989 9 28288.88 86 898 828
8 . . 29298.29 96 898 880

8-. . 28298.89 96 898 928

8 . 989 9 28229.88 96 898 828
-8 . . 28999.89 86 898 928
8.989 2 292228.892 89.0 898 828
8.989 .9. 29288992 928 898 828
8.989 9 29289.98 86 898 880

8 . . 28298992 880 898 890

8 . . 28298.89 880 898 290

8. . 28299.28 86 898 828

-8 . . 28299.29 86 898 828

8 989 2 . 28282892 8989 898 86
8 982 9 . 29292.98 89.0 898 280

8 989 2 . 29288292 890 898 828
8 989 9 . 28229.98 86 898 828

8 . . 29298.89 89.0 898 26

8. . 28289.89 86 898 828

8 . . 28288.88 89.0 898 828

8 . . 28298.89 26 898 828

8. 292289.992 290 898 828

- 8-. . 28228992 828 898 828

8 889 2 989 2 28298892 290 998 880
8 889 9 882 9 29288.88 26 998 880
8 829 9 . 29288.28 26 998 89.0

8 889 9-. 292989.882 29.89 998 228

2 889 2 . 28298.88 26 998 928

8 989 9 882 9 29289.28 86 998 890
8 989-9 . 29298.98 86 998 89.0

8 929 9 . 28288.88 89.0 998 228

8 989 2 . 292299.982 89.0 998 928

8 888 2 . 29289892 89.0 998 880

8 888-9 . 28288.89 86 998 228

8 888 9 . 28228.99 86 998 928

8 . . 28288.99 86 998 228

8 . . 28298.99 86 998 928

8-. . 292299.29 228 998 928

8 982 8 . 28288.89 96 898 99.0

8 989 -8 . 29228982 980 898 828

8 989- 8 8 28298.99 96 898 828

8 989 8 . 28298882 980 898 928

8 . . 28298.99 96 898 828

8. 8 29228982 990 898 828

8 . . 28298882 9989 898 928

8 . 8 292292.98 828 898 828

8 . . 2898.88 828 898 928

2 8 . 2898.88 828 898 928
928 2 8 28989.89 86 998 89.0
8 2 2 292289.982 8.90 998 928
988 2 . 28229.99 86 998 928
8 988-2 . 28292882 86 998 828
8 8 8 28229.99 86 998 928

2..
2.292
2..

190

8 . 889.9 2828.88 880 8208 26

2. . 28288.98 86 8298 280

8 . 889 9 688.982 880 8298 8.28

- 8.. . 28988.88 86 8298 898

8 889 9 882 9 28288.98 86 8208 280
2 889 2. 2828.88 880 8298 26

8 889 9 829 9 28288.88 86 8208 8.28
8 889 9 . 282882282 880 8298 898

8 8.89.9 222299.292 280 8208 26

8 889 9 829 9 28988.28 26 8208 8.28
8 889 2 . 28282.22: 26 8208 898

8 .889 9 28282.22: 26 8208 8828

-8 . . 28288.28 26 8298 8828

8 889.9 . 28:88.28 8228 8208 8.28

8 .888 9.. 28282892 86 8208 980

8 888 9 929 9 29229.88 86 8298 88.0
8 888.. 9 . 28288.82 86 8208 86

8 888 9. 8 28289.88 86 8208 82228

8 888.9. 28298.28 86 8298 2.28

8 . 989 9 28289892 96 8298 88

8 . . 28282.28 96 8208 880

8 . 8 28298.28 96 8208 8298

2. 28282.88 96 8208 298

8.989 9. 28228.88 86 8228 86

8 989 9 8.22 2222.992 86 8208 8298
8 989 9 . 2823.98 880 8208 298

8. 828288.88 86 8208 8298

8. 282228.892 880 8208 2.28

8 8 . 22 2288.88 8298 8298 2.28

8. 28221892 26 2208 so

8. 29298.32 26 22cm 86

8 . . 2898.292 280 2208 86

8. 2828.88 280 2298 898

8. 28299.32 30 2298 86

8. 29228.28 3.0 2298 86

8. 28982.88 30 2208 8.28

8. 29228.88 88.0 2208 88

8. . 28998.88 86 2208 8228

8 ... 8:88.892 86 2228 828

8 . 2.88-2 282222.892 86 9208 86

8 . 2.88 2 28298.82: 88.0 9208 28.0

8. 982. 2 29988.8 880 9208 86

8 . 9 €92.88 86 9208 898

8 288.2 282.2 29988.28 86 Sum 26
8 888-2 2282. 2 28288.82 86 9208 86
8. 288.2. 9 $89.88 880 9208 8828

8 2.88 2 .982. 2 28298.88 26 9208 880
8 988 2 .9 8:89.892 26 9208 8.28

8. 2.8.. 2. 9 28298.88 86 9208 8228

8 2.8.. 2 989. 9 2822.892 880 808 880
8 2289 .2 9 28288.98 86 8.98 86

8 9822. 2 2828.28 880 808 86

8 2.89. 2 9 $88.88 880 808 8.28

8 .8.. .2 2823.982 86 898 898

8 989 .9 9 2828.28 86 898 86

8 98.9 9. 28288.98 86 898 86

8 989 9. 9 2893.982 880 898 8.28

8 989 9 . $88.88 86 808 8.28

8 9 . 2 2228.292 86 808 86

8 9 9 28288.88 86 808 8828

8 9 . 28999.88 86 898 898

8 . 9 28299.88 86 808 8.28

191

8 928.8 8288 2829.982 880 8298 222228
8 92.8 8 82.2 8 2829.882 880 8208 82.28
8 92.8 2. 28228.98 86 8298 8.28

- 8 928 8 . $38 880 8298 8288
8 888 8 82.8 2 282282.88 22.28 8208 82828
8 82.8.8 . 2828.822 2.298 8298 8828

8 888 2. $8.89 3828 8298 8298

8 82.2 8 . 28222.88 82228 8208 898

8 82.8 8 . 2829.88 8228 8298 8208

8. 2922.882 828 8298 8208

8. 29288.88 86 8298 280

8 . . 29288.98 86 8208 898

8. 28288882 880 8298 998

8. 28229.88 26 8298 8.28

8. 28288.9: 280 8298 998

8.. . 2889.88 898 8298 998

8 . 989 9 28289.88 86 9208 88

8. ..292288.992 8.20 9208 96

8 . 989 9 28229.88 86 9208 880

8 . 8 28228.88 86 9208 898

-8 . . 28222.28 86 9298 298

8 .989 9.. 28288.32 86 9298 980

8 989 9.989 9 28228.3 880 9208 86
8 989 9 2 222288.892 880 928.8 898

8 989 2 . 28298.88 86 9298 2228

8 . 989 9 28229.88 96 9208 86

8. 8 28229.88 96 9298 8.28

.8 . . 28288.88 96 9208 2828

8 989 9 8 28228.88 88.0 9208 898

8 989.9 . 282289.892 880 9208 298

8 8 . 222289.88 898 9298 :28

8 . 988H2 282822.992 880 8208 96

8 .889 2 28229.82 86 8208 86

8 . 882 9 2928.88 880 8208 26

8 .988 8 28289.88 86 8208 92228

- 8.. . 28288.8 880 8208 8828

8 982 2 882 9 28289.28 96 8208 880
8 988-2 889-9 28289.92: 96 8208 280
8 988 2 988-8 28288.28 96 8208 9298
2 988 2 . 28288.88 96 8208 8.28

8 882 9 882 9 2828.88 880 8298 26
8 889 9 928 8 28288.88 86 8208 22298
-8 889-9 . 282298.992 880 8208 898

8 889 9 988 8.22 2288.292 26 8208 222228
8 889 9 . 28288.98 26 8298 $8

8 988-8 222229.88 22:28 8298 898

8 828.9 829 9 28288.88 86 :08 28.0
8 888 9.988 2 292228.992 86 2.208 96
8 888 9 988 2 28288.88 88 2.208 86
8 888-9.8 28289.88 86 22298 2298

-8 888-9 . 28289.28 86 8208 8828

8 889 2 988 2 28228.82: 26 :08 980
8 889 2 988 2 28288.88 26 22208 880
8 889 9 8 .22 223.892 26 :08 22.28

8 889 2 . 28289.88 28 2.208 8228

8 988.2 9.88 2 28229.88 96 222cm 86
8 988 2. 8 2828.28 980 9208 2298

8 98.8 2 . 28288.88 96 9298 898

8 988. 2 8 28299.88 88 :08 2298

8 988 2 2828.892 86 :08 8228

8 8 . 22 2288.88 22.28 :08 898

8 . 889.9 2823.892 86 8208 86

192

8 899-8.. 2828.882 980 8808 8298
8.899 8. . 282992 90.0 8808 8808

8 988 8.898 8 2829.98 96 8808 8.28

8 988 2 . 28229992 96 8808 2298

8 988 8.. 2928.882 989 8808 82.28

8 988- 8. 282282 96 8808 8808

8 892 8 . 2828.88 898 8808 22228

8 898 8 ..2822988 898 8808 82.28

8 898 8 . 28288 898 8808 8808

8. 28299.98 22.28 8808 8298

8. . 29288 2298 8808 8808

- .8 . . 28292 8298 8808 8808

8 829 8 829 8 282289.98 90.89 2808 880
8 899 8.889 9282292882 96 2808 8298
8 899 8 829 9 2829.982 980 2808 9298
8 899 8229222899 980 2808 82.28

8 899.8 . 2828.98 980 2808 9808

8 8998 889-9 2828.982 86 2808 82.28
8 899 8 829 9 2828.882 880 2808 92.28
8 899 8228229289 8889 2808 8298

8 82.9 8 . 2828.88 86 2808 9808

8 889-9 889-9 282292.88 8298 2808 9298
8 889 2. 2829.9: 8298 2808 82.28

8 889-9 . 2828.99 82.28 2808 9808

8 889-9 . 2828.29 9298 2808 8298

8 889 9 . 2829.29 9298 2808 9808

- 8 ... 2929.982 8298 2808 9808

8 829 8 829 8 28228.98 96 9808 86
8 899 8 .889 9 292288.882 980 9808 92.28
8 899 8 829 9 2828.982 980 9808 8298
8 899 8 . 282289.88 9.89 9808 2298

-8 8998 . 2828.88 980 9808 2808

8 899-8 889-9 2829.282 880 9808 9298
8 899 8 829 9 2829.992 86 9808 8298
8 899 8.. 292288.89 8.20 9808 2298

- 8 829 8 . 2829.88 880 9808 2808

8 889 9 889.9 282288.88 9298 9808 8298
8 889 2. 2829.82 92.28 9808 2298

8 889-9 . 2828.89 9298 9808 2808

8 889-9 . 2829.89 8298 9808 2298

8 889 9 . 2828.89 82.28 9808 2808

8. 292.882 22228 98082808

8 899-8 9988 28222 2.98 9889 8208 880
8 899-8 898-8 2829.982 96 9208 8298
8 899.8 898 8 2828.982 90.0 9208 9298
8 899-8.. 292288.99 9.20 9208 92.28

-8 899-8 . 2828.88 96 8208 8208

8 998-8 898-8 2829.882 880 9208 82.28
8 998 8 82.8 8 2828.882 86 9208 92.28
8 998 8228228889 880 9208 9298

- 8 92.8 8 . 2929.98 880 9208 8208

8 898 8 898-8 282282.88 82228 9208 92.28
8 898 2. 2829.9: 8228 9208 92.28

8 898-8 . 2929.89 82.28 9208 8208

8 898-8 . 2828.29 92.28 9208 92.28

8 898 8 . 2828.89 9298 9208 8208

- 8 ... 2929.982 928 9208 8208

8 899-8 998-8 282 298.98 90.0 8208 8889
8 899 8 898-8 2828.982 96 8208 9298
8 899-8 898 8 2829.882 92.0 8208 82.28
8 899.2. 282282.98 90.0 8208 898

8 899 8 . 2829.88 96 8208 9208

193

929.9 mac-928909.2829-09902-

289.9 989-82282209623222.202-

8988 899-82289099223222.202-

8999 223.020.22.890828-200298808Hpe29m

28.88. - 2229 820222 82202-88229-
mead 988 505 88303 60.52.3228 any

8 982.8 892.8 2829.99 96 8808 989

8 988 8 298 8 2828.98 96 8808 9298

8.988 8.. 29228882 980 8808 82828

8 988 8 988 2.2828882 96 8808 92.28

- 8 9.88 8. 28288 90.0 8808 9808

8 899 8 998-8 28229882 980 8808 92828

2 899 228222.88 90.0 8808 82.28

8 899 8 988 2.2928882 96 8808 9298

8 8.99 8 . 28229 980 8808 9808

-8 998-8 . 2828.88 9298 8808 82.28

8 998 8 988 2.2922299 9298 8808 92.28

8 9228 8 . 28288 9298 8808 9808

8 .988 2 28228.99 8298 8808 9298

-8 . . 29299 8298 8808 9808

8 2.88 2 ..282882 9298 8808 9808

8 899 8 928 8 2829.89 980 9808 96

8 899 8 . 2922.89 980 9808 8298

8 8998 9988 28229992 980 9808 92.28
8 899 8 988 2.8228882 96 9808 92828
8 8.99 8 . 292982 980 9808 8808

8 .988 8.. 29222892 980 9808 82.28

8 988-8 998-8 22 228.89 980 9808 9298
8 988 8 988 .2 2929.882 980 9808 9298
8 988. 8. 282882 9889 9808 8808

8 . 992 8 2828.98 8298 9808 9298

8 . 988 2 29229.88 8298 9808 92.28

- - 8. 29298 8298 9808 8808

8 998 8 988 2.2922288 92228 9808 9298
8 998 2. 28228 9298 9808 8808

.8 988 .2 . 2829 9298 9808 8808

8 899 8 288 8 2828.98 980 8808 90.0

2 899 2 . 28228.88 96 8808 2298

8 899 8 89.8. 8 28228982 980 8808 898
8 899 8 ..2928882 980 8808 82.28
8.899 8 . 28288 90.0 8808 8808

8 98.8 8. 22228882 980 8808 2298

8 988 8.898 8 2828.88 920 8808 898

8 988 8 . 2.2229882 900 8808 8298

8 988. 8. 28299 980 8808 8808

8. 898 8 2829.98 2298 8808 8.28

8. 29228.99 22.28 8808 82.28

8.. . 29288 2298 8808 8808

8 898.8 . 28288 898 8808 82.28

8 898 8 . 28299 898 8808 8808

- 8 ...282892 82828 8808 8808

8 829 8 928 8 2929.99 980 8808 90.0

8 899 8 898-8 28228992 980 8808 898
8 899 8 . 2822.29 9889 8808 2298

194

.-...-......EEE....-.81..