DRYTNG OF PAPER PULP ON A HEATED SURFACE or the Degree of M. S. MlCHlGAN STATE COLLEGE Fhiroze Dhuniishaw Shmff 1949 Thefisf This is to certify that the thesis entitled TEIE DRYING CF PAPER. PULP CN A HEATED SURFACE presented by PHIROZE DEIUI‘IJISELZ'J SEIRC‘FF has been accepted towards fulfillment of the requirements for MA STERS degree in WEN GATE Edi N G WW Major professor SEPTEMBER 16 1 A- - -._ I _>g4 ' '. -_g,. ‘--.._-c. - , -a. DRYING OF PAPER PULP ON A HEATED SURFACE BY PHIROZE DHUNJISHAW SHROFF W A THESIS Submitted to the School of Graduate Studies of‘flichigen State College of Agriculture and Applied Science in partial fulfillment of the requirements for the degree of MASTER OF SCIENCE Department of Chemical Engineering 1949 THESlS ACKNOWLEDGMENTS The author is deeply indebted to Associate Professor Randall W. Ludt for his guidance, advice and assistance. Appreciation is also expressed to Mr. William B. Clippinger and.Miss Elizabeth F. Iledan for their valuable help. The pulp and some equipment for this investiga- tion were supplied hy the Watervliet Paper Company through.Mr. Louis Scheid. (en‘s'v 4' 0 ' -. m, ' Fish-.41 1' if} 5i, TABLE OF CONTENTS Introduction .................................. History ....................................... Experimental Procedure ... Discussion .................................... Conclusions ................................... Bibliography .................................. Appendix P__ag_e 1 3 9 26 32 3h INTRODUCTION Drying is one of the most important processes used in the production of paper. ‘It is important because the heat requirement is a major item in determining manufacturing costs and because low drier capacity may limit production. Machine apeed and production can frequently be increased by increasing the capacity of the drier section. The object of studies on the process is to obtain data upon which to base the design and Operation of equipment. DevelOpments in the theory and mechanism of drying can be expected to lead to economies both in oper- ating and capital costs. Generally these factors have been based on the results from previous installations or on established procedures. Very little scientific information is now available. Several different types of driers are used in the manufacture of paper, but they employ the same general principles. The web formed on the vet-end of the machine is passed over a wire mesh, then across suction boxes and finally through press rolls. In this way most of the water is removed, and the sheet now containing about 60 per cent moisture is dried on steam heated rolls. The drier section may consist of a series of steam heated drums, 48 inches in diameter. The paper passing over the rolls has alternately one Of’its faces and then the other, in contact with the drier surface. This Method of drying is known as drum drying. Another method commonly employed imakes use of a single large drum, 10-12 feet in diameter which is called aYankee drier. This is also a continuous process, the sheet is pressed 011 to the drum so that during the entire drying period only one of its ".90 Cl! I‘el u '- t" rL r; :3 H.- 55 1.5er «9;. .— 5... .... .. .fir‘h rub . - a II Vt faces is in continuous contact with the heated surface. Thus it is seen that air drying is not applicable to drier sections of paper machines while continuous drying on a heated surface applies specifically only to Yankee driers and not to a series of drum driers. Most of the experimental work on the drying of paper has been done with air drying. A small amount of work has been done with heated surfaces which correSponds to conditions on a Yankee drier. However, apparently only plant tests have been made on a series of drum driers. Some of the conditions found in air drying have been shown to exist when the material is dried on a hot surface. It is to be expected that the results obtained with heated surfaces can be corelated with the drying of paper on a series of drum driers. This work is being directed towards a better understanding of the mechanism existing on Yankee paper driers. HISTORY Many investigators have reported data on air drying processes, but few have investigated drying by a heated orifice. The important hypotheses on the air drying mechanism have been advanced by Lewis (12,15) and Sher- wood (29,30,51,53). Four possible mechanisms of drying have been postulated and their characteristics given. They are: (i) ‘§g§upated Surface Egyigg; The flow of water within the solid keeps the surface saturated so the equivalent of a film of water was pre- sented to the drying air. The mechanism of drying was similar to the evaporation of water from a free liquid surface as described by Badger & McCabe (6) and Walker et. al. (45). All factors remain constant so the rate of drying is constant. This was the mechanism of drying in the in- ternal of constant rate drying. (11) Unsaturated Surface m The flow of water in the solid was sufficient to keep the hollows in the surface saturated with water, the high points being dry. The rate of drying decreases in proportion to the decrease in saturated area. The over-all coefficient of heat transfer remained constant and equal to the value in the internal of constant rate drying which indicated that water was evaporating at the surface of the solid. 113g Factor: Water was evaporated at the surface of the solid as rapidly as it could diffuse to the surface from the interior. The rate of drying decreased as the rate of diffusion of liquid water decreased and the latter was a function of the thickness of the sample. (iv) Evapgration 5;; M212. is; the Interior 93 thg §p_l_i_t_i_: The zone of vaporization of water was in the interior of the solid and its location depended upon a balance of the rate of flow of water into and the water vapor out of it. The rate of drying and the over-all coefficient of heat transfer decreased and a layer of dried solid was formed beneath the sur- face, as the zone of vaporization retreated into the interior of the solid. Sherwood (29) has mentioned that mechanism (iii) applies to relatively non-porous materials and (iv) to porous materials but has not suggested at what porosity the mechanism changes. The mechanism of pulp drying has been showen to be of type 4. McCready (15) has pointed out that the formulation of the drying mechanism could be based on the rates of flow of heat and water vapor be- tween the air and the zone of vaporization or on the rate of transfer of liquid water through the solid. These are of little value as they did not include the rate of drying as a function of the water content of the solid. Lewis, McAdams, and.Adams (13) analyzed data on the drying of pulp and paper on drum driers. Sherwood (55) presented a means of calculating the influence of heat in flow through non-drying faces on the rate of drying. Stacey (40) and Sherwood and Cummings (58,59), have reported and discussed data on the drying of various materials in pans, a method which is similar to drying on heated surfaces. Diffusion equations analogous to those for unsteady heat conduction have been developed for application to the drying of solids (35). Sherwood (34) has discussed the application of theoretical diffusion equations to the drying of solids, which appeared to give reason- ably close agreement with experimental data. However since some of the 5 postulates were subject to criticism, Newman (21,22) suggested a new hypo- thesis. In support of it he obtained the liquid concentration-time—loca— tion relations in the interior of porous solids, together with equations develoPed for various shapes. The equations were integrated to give the average liquid concentration as a function of drying time. On the basis of his hypothesis he has derived diffusion and surface emission equations for the drying of porous solids. Sherwood (29) performed experiments on the drying of various solids and the case of drying by internal diffusion of the liquid to the surface with negligible resistance to the removal of vapor was discussed in detail. The Fourier equations of heat conduction in solids have been showen to apply to the drying of solid slabs by this mechanism,and a method was des- cribed by which the equation may be used in the analysis of drying data. In another paper, Sherwood (50) has described the effect of adjoining dry surfaces. Radiation from the surroundings and air velocity on the rate of drying of solids in the constant rate of drying period. He has derived a simple emperical equation to fit the data reasonably well in the falling ' rate period and to afford a simple basis of calculation in drier design. McCready (15) has summarized the effect of density on the mechanism of drying. Increasing the density or decreasing permeability of the solid for water vapor resulted in a change in the distribution of water vapor through the zone of vaporization. Two mechanisms of drying were found for the air drying of pulp and paper by McCready (15). Drying data on pulp slabs of varying permeability to water vapor have been presented as proof of the two mechanisms of drying, which also illustrated the effect of permeability on the water distribution in the solid. 6 Collins and Fisher (5) have showen that the over-all coefficient of heat flow remains constant druing the constant rate period but decreases rapidly after the critical moisture is reached; the decrease in the coef- ficient during the falling rate period correSponds to an increase in the over—all thermal resistance which must be due to the occurrence of the actual evaporation of water beneath the surface. Sherwood (56) also found that internal liquid diffusion was control- ling throughout the falling rate period for the case of thick pulp slabs, and evaporation has been shownto take place at points within the pulp structure. . . This information has been based on air drying of porous solids. It does not apply directly to drying on a heated surface. The mechanisms found, however, do show some corelation with those which are found dur- ing drying on heated surfaces. _ . ucCreedy (15,16) has reported data on the rate of drying of pulp slabs in contact with hot surfaces under experimental conditions similar to those in drum drying processes. However, his emperimental data are based on a hot plate temperature of 80 deg. C. which corresponds to a steam pressure of 6.9 psia. This pressure is below that commonly used in industrial driers of pulp and paper. The mechanism of drying of the slab ‘which described variations in the temperature and moisture content was ‘presented. Effects of the slab thickness and supplementary drying air ‘were investigated. .According to McCready, the slab dried at constant rate in the first .interval of the drying process and then the rate of drying decreased. Ending the constant-rate period local temperatures in the slab remained 7 constant until the indicated critical water concentration was approached and then the temperature decreased. The rate of drying decreased when the temperature decreased but the initial decrease in the rate was small. In the first period of the interval of falling rate drying, the rate of drying and consequently the rate of heat transfer from plate to slab decreased, temperature in the slab decreased, temperature difference be- tween plate and slab increased and temperature difference through the slab decreased. This indicated that thermal resistance between plate and slab increased due to drying out of the water film between slab and plate and that the thermal conductivity of the slab remained substantially constant and equal to the value of the wet slab in the interval of constant rate dry- ing. In the second period temperature difference across the first ply beneath the closed face increased, indicating that the ply was drying. The temperature difference across the remainder of the slab decreased, indicat— ing that, that part remained wet with substantially a constant thermal con- ductivity. In the third period the decrease in temperature difference between plate and slab indicated that thermal resistance between those points reached and remained at a constant value after the water had dried out. He also showed that thick slabs dried at a slower rate than the thin slabs. The rate of heat and water vapor transfer through the slabs decreased as the thickness of the slab increased. McCready (16) has shown that temperature of supplimentary air had very little effect on the rate. Increase in plate temperature increased greatly the rate of drying. Provided the difference between the hot surface and drying air temperatures was large, there was little effect or change of re- lative humidity of the air on the rate of drying. He suggested that thermal conductivity of the solid might be an important factor, since the heat absorbed by the dry surface must be conducted through the solid to the points where vaporization occurs. It is possible from the preceding statements to predict the effect of some variables on the drying process. However there is still a wide field for further research on this important subject with regard to de- termining the exact mechanism of the drying process in order to Operate on a more efficient basis in the inductrial drying of pulp and paper. The present work presents, in the form of rate curves, new data on the drying of pulp sheets. .All experiments were carried out in still air using a hot plate temperature of 240 deg. F. corresponding to a pres- sure of 25 pounds per sq. in. abs. which pressure correSponds closely to that which is used in the Yankee driers for pulp and paper. EXPERIMENTAL PROCEDURE The pulp used was of commercial can wrapper stock composed of sul- phite and waste pulp. The slurry used in making the sheets was obtained by macerating a known quantity of the raw stock in a ball mill for one hour, followed by treating it in a mixer after further dilution with water. It was observed that the ground pulp if kept in contact with water for any length of time, became hydrated, and as a result the sheets formed from it showed considerable shrinkage during the drying. In order to pre- vent this, freshly prepared pulp stock was used every time. A definite quantity, each time the same, of this stock pulp was used to form the Sheet. This ensured the sheet to be of uniform bone dry matter. The separate plies were first formed on a Buchner funnel and these pLys were assembled to make the sheet. A silmanite Buchner funnel #H, 186 mm. in diameter was used. The sheets formed had a diameter of 7.1875 inches. Copper constantan thermocouples, 32 gage, enameled wire were placed between the plies and the whole was pressed to form a compact sample of the sheet. It was then wetted slightly and placed on the Buchner funnel, Operated with a 26 inch vacuum to remove the water. This procedure was followed as clo- sely as possible in order to ensure uniformity of the initial moisture con- tant of the sheets. An electric hot plate was used as the source of heat. It was connected through several variable rheostats, so that the temperature could be con- trolled constant throughout the run. 41 type -Ta Industrial.Analyser was inserted in the circuit in order to keep an accurate check of the current supplied to the hot plate. 10 .1 circular steel plate one foot in diameter and 0.75 inches thick was placed on the hot plate. The upper surface of this steel plate was kept constantly polished. Six thermocouples, Leeds and Northrup, No. 20, copper— constantan, duplex wire, glass insulated, were inserted into the steel plate half way between the two faces of the slab, one thermocouple being at the center and the others at a distance of l, 2, 5, 4, and 5 inches reapectively away from the center. These thermocouples,as well as those between the plies in the sheet, were connected through single-pole, single-throw switches to a Leeds and Northrup potentiometer. In order to eliminate possible effects of shrinkage or curling at the edges of the sheet during drying, an annular ring was placed on the sheet. This ring was pressed down on the sheet by means of heavy lead weights placed around the rim of the annulus so as to allow free circulation of vapors. The ring 1.5 inches high had an internal diameter of 6.9575 inches and was made of number 14 B & S gage tin sheet. The area of the sheet covered by the annular ring was 0.00955 sq. ft. which was less than 5.5% of the total area of the sheet, and was therefore neglected in the calculations. At the end of the run the thickness was measured with a dial indicator on a.magnetio stand used with surface plate. The sample was then heated over night in an electric oven maintained at 100 deg. C. and the bone dry weight obtained. From a series of preliminary runs carried out on the variation of temperature in the hot plate above, it was observed that the temperature drop across the plate from the center to the outside edges was within 1 degree F. at all temperatures up to as high as 400 degrees F. As the 11 temperature across the plate was constant it was considered not necessary to take the temperatures at the various distances from the center to the outside to get an average temperature of the plate; only the temperature at the center of the plate was recorded as this represents the temperature of the plate. The drying samples for the first series of runs were prepared as des- cribed above and were built up of four plies. Three thermocouples were inserted between the plies, and the temperatures were all measured at intervals of one minute. In the first set of experiments of this series the sheets were kept intact at the end of the run. Determination of moisture content and thick- ness were carried out on the sheet as a whole. In the second set of this series the plies were separated at the end of the run and the thickness and moisture content of each ply separately determined. In the second series of experiments, the drying samples were prepared identically as before but were composed for two plies. One thermocouple was inserted between the two plies and the temperatures recorded at inter- 'wals of one minute. Moisture content and thickness of the sample were ob— tained for the sheet as a whole. The temperatures of the sample and of the hot plate were plotted :against time, (Graphs l, 2, 5, 14, 15, 16, and 25). The temperatures of the top and bottom of the sheet were obtained by extrapolating the lines Joining the local temperatures of the plies, Graphs (4, 5, 6, 7, l7, 18, 19, 20). Knowing the final and initial temperatures of the sheet, the final auui initial moisture contents, the amount of vaporization, and the quantity 12 of the bone dry material for various tests, the quantity of heat transferred by the hot plate which was picked up by the sheet together with that lost by radiation and convection from the surface were calculated for different intervals of time. For any particular interval of time and the corresponding temperature difference in the sheet in that interval, the quantity of heat (q. in B.t.u.'s) required to raise the temperature of the sheet from the average initial to the average final temperature is given by: ‘18 a 776' chp At where W1 Bone dry weight of sheet (1b.). Cp a Specific heat of pulp equals 0.32 B.t.u./(lb.)(°P). At = Temperature difference between the final (Av) and initial (Av) temperature of the sheet (01"). A0 =--— Time interval (minutes) The quantity of heat (q' in B.t.u.'s) required to raise the temper- ature of the total water in the sheet through the same temperature difference is given by: q' a: 60": A0 2P where '2 a Total water in the sample (lbs.). G1) a Specific heat of water equals 1.0 B.t.u./#°P. The latent heat contributed by the water evaporated is based on the mean temperature of the center of the sheet as measured by the middle thermo- couple, in that interval of time. Thus the heat given by the latent heat (91. in B.t.u.'s) is given by: 13 C11. : w3 L A 0 here W3 = Total grams of water evaporated in the interval, (1bs.). L = Latent heat (B.t.u./lb.). In order to estimate the quantity of heat lost by radiation and convec- tion from the top of the sheet, an over-all coefficient of heat transfer between the sheet and air was assumed, as h.0 B.t.u./(hr)(ft2)(°F). Then the quantity of heat lost (qR in B.t.u./hr) is given by: qR = 01 A, Atl := Over-all coefficient of heat transfer equals LO B.t.u./ (hr)(ft2)(°F)- A, = Area of sheet (ftz). where 01 At =- Temperature difference between the average temperature 1 of the tOp of the sheet in the interval of time 0 and the air temperature (TA), (01"). The total quantity of heat transferred (Q in B.t.u.'s/hr) by the plate is given by: 9:39... no Knowing the total heat transferred by the plate, the thickness of the (q3+q,+qL) +qr plate and the temperature of the plate half way between the two faces, the temperature of the tap of the plate is calculated as follows: KAs where S = 1/2 thickness of plate (ft). K = Thermal conductivity of steel equals 26.0 B.t.u./(hr)(ft2)(°F/ft) TP ..—= Temperature of plate (OF) Tor? =—. Temperature of the top of the plate (01"). Calculation for an estimate of the over-all coefficient of heat transfer between the sheet and plate is as follows: U A, A122 where A132 is the temperature difference between the top of the plate 0 and the bottom of the sheet: A t 2 '(TTP - TBS), ( F). The over-all coefficient U was plotted for the different intervals of time, and a smooth curve was drawn through the teps, so that the area between each top and the smooth curve was divided into segnents of equal size. The curve (Graph 12) gives the over-all coefficient of heat transfer between the sheet and plate at any time during the drying period. A curve (Graph 13) was then drawn of the over-all coefficient vs moisture content in the sample. The grams of water evaporated on the basis of bone dry pulp were plotted vs time and a curve drawn through the data points (Graphs 9 and 26). The instantaneous rate of drying of the sample at various times was readily calculated from the curve as shown below and the instantaneous rate vs average water concentration expressed as grams of water left per gram of bone dry material were plotted (Graphs 11 and 29). This is the drying rate curve. The instantaneous rate of drying at any time was obtained by the method of graphical differentiation as proposed by Mg (26). The grams of water evaporated for small intervals of time were obtained from the 15 graphs (9 and 26). evaporation divided by the product of time and area of the sheet gave the differential rates in lbs./(hr)(ft2) for the small intervals of time. The differential rates were then plotted for the 'various intervals and a smooth curve drawn through the tOps as before. This is the differential curve which gives the instantaneous rate at any time during the period covered (Graphs 10 and 28). The water concentration on bone dry basis is obtained from graphs (8 and 27). In order to illustrate the extent of drying at different levels of thicknesses in the sheet, curves were drawn for each ply of the evaporation on the basis of bone dry pulp vs time (Graph 22). The per cent moisture content of each ply was corelated with the final moisture content expressed as lb. of water left per lb. of bone dry material, (Graph 21). Time (minutes) 2 Bone dry wt. (gms) ”tar Ming It. (8mg) 26.405 14.918 Total wet wt. (gms) 59.100 Initial moist. conp tent (gms) 24.182 Final moist. content (gms) 11.487 Moisture evap. (gms) 12.695 5 Initial moisture 61.846 % Final moisture 45.505 gms. 329 Evap/gm B.D. pup .850 Final moist. content/ gm. B.D. pulp .770 Initial moist. content/ gm. B.D. pulp 1.621 Total thickness (incheéo.188 .Approx. Thickness of each ply (inches) 0.047 TABLE 5 5 14.865 21.120 59.000 24.157 6.257 17.880 61.889 29.626 1.205 .421 1.624 0.196 0.049 4 15.257 18.741 59.950 24.715 5.504 21.210 61.860 18.696 1.592 .250 1.622 0.172 0.045 5 14.510 16.200 58.000 25.490 1.690 21.800 61.900 10.452 1.502 1.618 0.160 0.040 10 15.545 16.800 40.210 24.865 1.455 25.410 61.857 8.660 1.525 0.095 1.620 0.197 0.049 15 15.109 16.257 59.600 24.491 1.148 25.545 61.845 7.061 1.545 0.076 1.621 0.201 0.052 16 20 15.275 16.207 40.020 24.745 0.952 25.815 61.851 5.750 1.559 0.061 1.620 0.182 0.046 l7 TABLE 6 (overall coef. of Time Final Moist. Cont. Evaporation Rate h;::°t:nags;h::3reen (m) 1b. H20 left lbs H20 evap. lbs H20 evap. p B.t.u. lb B.D. pulp 1b B.D. pulp (lb B.D. pulpKhBCrt‘) Tn'rilrtZR—T‘OF 0.00 1.621 0.00 98.00 121.5 0.50 1.215 0.212 94.70 118.7 1.00 1.180 0.1.1.2 91.10 115.0 1.50 0.990 0061.2 87020 11005 2.00 0.770 0.850 82.20 101.0 2.25 0.655 0.959 78.80 95.0 2.50 0.560 1.01.5 73.10 79.0 2.75 0.2% 1.125 6h.30 59.5 30m 001.21 10203 55060 16508 3.25 0.360 1.260 1.7.00 38.4 3.50 0.310 1.310 1.0.00 33.5 3075 0.270 1.352 316000 2900 mo 0.230 1.392 29.10 22.5 6.25 0.190 1.1.30 26.60 20.5 #050 0.160 101060 23070 1700 4.75 0.135 1.1.85 18.00 13.2 5.00 0.116 1.502 10.00 10.0 6.00 0.108 1.510 1.00 2.0 8-00 0.101 1.518 0.90 1.1 10-00 0.095 1.525 0.90 2.2 13.00 0.083 1.536 0.85 t.5 15.00 0.076 1.51.5 0.85 6.0 $000 0.070 1.551 0.61. 7.9 .00 0.061 1.559 0.1.3 10.9 18 TABLE 11 (5 minutes) P7: P2 __Pi_5__ P B 8* Bone dry wt. (grams) 5.774 5.819 5.827 5.852 15.272 After drying wt. (grams) 4.500 4.500 4.200 4.200 17.200 Total wet wt. (grams) 9.956 10.001 10.009 10.054 40.000 Initial moist. content (grams) 6.182 6.182 6.182 6.182 24.728 Final moisture content (grams) 0.726 0.481 0.575 0.548 1.928 Moisture evaporated (grams) 5.456 5.701 5.809 5.854 22.800 5 Initial moisture 62.000 61.75 61.70 61.50 61.750 .iFMflmdflwe mam new 85% 82% new grams 520 Evep/grams B.D. pulp 1.449 1.495 1.510 1.515 1.496 Final moisture content/grams B.D. pulp 0.1925 0.126 0.0974 0.0905 .126 Initial moisture content/grams B.D. pulp 1.658 1.619 1.615 1.605 1.622 Total thickness (inches) 0.050 0.055 0.048 0.059 0.190 0000.000 tOP ply 2 assesses 2nd Ply from tOp P5 008.000. 5rd ply from top PB eeeeeese Bottom ply 3* assesses Sheet TABLE 12 (10 minutes) .31. Bone dry wt. (grams) 4.112 After drying wt. (grams) 4.700 Total wet wt. (grams) 10.800 Initial moisture content (grams) 6.688 Final moisture content (grams) 0.588 Moisture evaporated (grams) 6.100 5 Initial moisture 61.900 5 Final moistmre 12.500 gramsngO Evap/grams B.D.pulp 1.485 Final moisture content/grams B.D. pulp 0.145 Initial moisture content/grams B.D. pulp 1.626 Total thickness (inches) 0.050 000.000. top Ply oeeseeee 211d ply from top 5 cases... 5rd ply from top B 00...... BOttom ply seseeeee Sheet» P2 P5 . 4.159 4.156 4.600 4.570 10.827 10.844 6.688 6.688 0.461 0.214 6.227 6.474 61.600 61.550 10.040 4.900 1.504 1.557 0.111 0.052 1.615 1.609 0.440 0.046 P B 4.141 4.250 10.829 6.688 0.089 6.599 61.610 2.100 1.594 0.021 1.615 0.052 19 8* 16.548 17.900 45.500 26.752 1.552 25.400 61.550 7.550 1.554 0.082 1.616 0.192 TABLE 15 (15 minutes) .11... Bone dry wt. (grams) 5.790 After drying wt. (grams) .200 Total wet wt. (grams) 9.967 Initial moisture content (grams) 6.177 Final moisture content (grams) 0.410 Moistm'e evaporated (grams) 5.767 5 Initial moisture 61.974 5 Final moisture 9.761 grams 320 Evap/grams B.D. pulp 1.522 Final moisture content/grams B.D. pu1p0.108 Initial moisture content/grams B.D. pulp Total thickness (inches) T eeeseeee tOP Ply eeeeeoes 2nd Ply from top 5 0.000000 5rd ply from top B eeeseese BOttOm ply 5* 00...... Sheet 1.650 0.042 P 2 5.858 4.150 10.055 6.177 0.292 5.885 61.554 7.056 1.525 0.076 1.601 0.046 P5 ‘23 5* 5.809 5.854 15.291 5.920 5.890 16.160 9.986 10.012 40.000 6.177. 6.178 24.709 0.111 0.056 0.869 6.066 6.122 25.840 61.856 61.705 61.772 2.851 1.459 5.577 1.592 1.596 1.559 0.029 0.015 0.057 1.621 1.611 1.616 0.048 0.042 0.178 TABLE 14 (20 minutes) Bone dry wt. (grams) After drying wt. (grams) Total wet wt. (grams) Initial moisture content (grams) Final moisture content (grams) Moisture evaporated (grams) 5 Initial moisture % Final moisture grams 320 Evap/grams B.D. pulp Final moisture content/grams B.D. pulp Initial moisture content/grams B.D. pulp Total thickness (inches) PT ........ top ply 2 ssssssss 2nd ply from top 5 ssssssss 5rd ply from top B ssssssss BOttom ply 3* ........ Sheet PT Pg_‘ 5.796 5.842 4.151 4.051 10.004 10.050 6.208 6.208 0.555 0.189 5.855 6.019 62.055 61.771 8.552 4.688 1.542 1.567 0.095 0.049 1.655 1.616 0.042 0.044 P ...!L.. 5.856 5.922 10.064 6.208 0.066 6.142 61.685 1.682 1.595 0.017 1.610 0.042 PB 5.844 5.896 10.052 6.208 0.052 6.156 61.758 1.554 1.601 0.014 1.615 0.048 8* 15.558 16.000 40.170 24.852 0.662 24.170 61.817 4.157 1.576 0.045 1.619 0.176 (min) 10 15 10 15 10 15 10 15 °F 1L6.6 128.0 172.7 188.9 SECOND PLY FROM TOP 148.5 132.0 175.5 190.6 THIRD PLY FROM 50? 150.h 13h.3 178.8 192.2 152.0 138.0 182.1 193.7 TABLE 15 TOP PLY Temperature BOTTOM PLI Mbisture Content 1b. B.D. pU1p .1925 .1h30 .1080 .0930 .1260 .1110 .0760 .0h90 .0974 .0520 .0290 .0170 .0210 .0150 .01L0 22 23 TABLE 16 Thick Sheet Thin Sheet Rate Moisture Content Rate Moisture Content 1b. £120 evap. 1b. H20 1b. 1120 evap. 1b. P120 Tux-75's?) 1b. B.D. Pulp (ma-t2) 1b. B.D. Pulp 98.0 M80 1.621 108.0 775 1.624 91»? 11.30 1.1415 102.1 726 1.390 91.1 1376 1.180 97.0 690 1.160 87.2 1318 .990 91.9 65h 0.947 82.2 121.0 .770 86.8 616 0.710 78.8 1190 .655 8h.0 596 0.610 73.1 1105 .560 80.0 569 0.510 61.3 971 .490 73.0 519 0.120 55.6 81.0 .h21 62.8 M6 0.331. 1.7.0 710 .360 52.1 371 0.277 1.0.0 605 .310 1.3.1 306 0.225 3M0 511. .270 35-5 252 0.130 29.1. 11M .230 28.2 200 0.137 26.6 601 .190 21.5 153 0.112 23.7 358 .160 15.1 107 0.080 18.0 272 .135 9.0 61. 0.067 10.0 151 .116 3.0 21 0.052 0.90 13.6 .095 .972 6.9 0.031 0.85 12.9 .076 .723 5.1 0.016 0.113 6.5 .061 .310 2.1. 0.007 Time (minutes) 2 Bone dry wt. (gms) After drying wt (gms) 12.205 7.158 Total wet wt. (gms) 18.750 Initial moisture con- tent (gms) 11.592 Final moisture con» tent (gms) 5.067 Moisture evap. (gms) 6.525 % Initial moisture 61.890 5 Final moisture 41.52 gms Hap Evap/gm B.D. pulp 0.914 Final moist. cont./gm B.D. pulp 0.710 Initial moist. cont./ gm B.D. pulp 1.624 Total Thickness (inche8)0056 Approx; Thickness of each ply (inches) 0.018 TABLE 21 5 4 6.994 6.751 9.550 7.676 18.575 17.728 11.579 10.977 2.556 0.925 9.045 10.052 61.955 61.918 25.04 12.05 1.295 1.489 0.554 0.157 1.627 1.626 0.054 0.058 0.017 0.019 5 6.697 7.045 17.575 10.876 0.548 10.528 61.890 4.94 1.572 0.052 1.624 0.054 0.017 10 7.065 7.248 18.552 11.487 0.219 11.268 61.917 5.01 1.595 0.051 1.626 0.057 0.019 15 7.156 7.250 18.755 11.617 0.114 11.505 61.947 1.57 1.612 0.016 1.628 0.052 0.016 20 7.119 7.169 18.701 11.582 0.050 11.552 61.952 0.700 1.620 0.007 1.627 0.058 0.019 Time (min) 0.00 0.50 1.00 1.50 2.00 2.25 2.50 2.75 3.00 3.25 3.50 3.75 h.00 h.25 h.50 h.75 5.00 10.00 15.00 20.00 Final.Moist. Cont. lbs H20 left 1b B.D. pulp 1.624 1.390 1.150 0.9h0 0.710 0.610 0.510 0.h20 0.33h 0.277 0.225 0.180 0.137 0.112 0.080 0.067 0.052 0.031 0.016 0.007 TABLE 22 Evaporation lbs H20 evap. lb B.D. pulp 0.000 0.240 O.h80 0.690 0.91h 1.135 1.293 1.h12 1.h89 1.538 1.572 1.595 1.612 1.620 Rate Lbs H eva . 1b B.D. pulp hr ft ) 108.90 102.10 97.00 91.90 86.80 8h.00 80.00 73.00 62.80 52.10 h3.10 35.50 28.20 21.50 15.10 9.00 3.00 0.972 0.723 0.340 25 26 DISCUSSION Elmerimental work on the drying of sheets of the thickness of ordinary paper would be extremely difficult. In these experiments thicker sheets were used. The temperatures of the hot plate used corresponded to the steam pressure of commercial driers, and the drying itself was carried out in still air. The temperatures of the hot plate were measured within 1 deg. F. and it can be considered that the temperatures of the sheet were accurate to the same degree. The variation in temperatures across the plate were within 1 deg. F. The sheets were weighed immediately before the test and imediately after the end of the experiment. This introduced a certain amount of inac- curacy in the measurements, but these errors were believed to have been re- duced to a minimum. As the experimental procedures were difficult, the accur- acy of the data does not warrant a critical examination. Immediately on placing the sheet on the heated surface flash vaporiza- tion took place. The temperature of the sheet immediately rose to very near the atmospheric boiling point of water which the temperature of the plate dropped. The temperatures then continued to decrease until a minimum was reached, after which there was a continuous increase in both sheet and plate temperatures. The hot plate temperature continued to rise until it reached . its original value and then it remained constant. After the minimum, the temperature of the sheet increased continuously. The temperature in the slab at any time decreased from the plate to the Open face. The period during which the temperature decreases includes the normal falling rate period. Drying apparently begins in this period. Pulp of 60% 27 moisture, which is the normal moisture content of commercial driers, can always be expected to dry in this manner. The interval corresponding to the increasing temperatures includes the rest of the falling rate period. The latter part of the falling rate interval includes the period during which, apparently, internal diffusion controls the rate. This is an impor- tant part of paper drying because it indicates the difficulty in removing moisture from a thickesheet which contains less than 10% moisture. The data show that the temperature of thin sheets decreases to l63.lt deg. 1". while in the thick sheets the temperature decreases to 125 deg. F. Moreover, this minimum was reached in a shorter time in the former case. For the thick sheets, the interval after the minimum point is reached, during which the temperature of the sheet rises, corresponds to the period wherein internal diffusion is controlling. During this period the moisture content of the sheet is reduced from 0.101 to 0.061 pounds of water per pound of bone dry pulp. For the thin slabs, the minimum temperature of the sheet is reached when the falling rate period is only half completed. The period of temper- ature increase in the sheet corresponds to the latter half of the falling rate interval, during which time the moisture content of the sheet decreased from 0.331. pounds of water per pound of bone dry ply to 0.007 pounds of water per pound of bone dry pulp. The moisture content of the sheets decreased very rapidly during the initial drying period. Evaporation was practically complete for both sheets in five minutes. At a moisture content of approximately 10%, for the thick sheets, a critical rate change occurred tion was apparently due to a change in the mechanism of drying (Graph 8.). A similar critical rate was also 'M U- °'r~ ta.‘ 8’.- gm 28 observed for the thin sheets at a moisture content of about 5%, (Graph 27). The mechanism of drying after this lower critical point corresponded to that occurring when diffusion within the fibers is controlling. Thin sheets can be expected to dry down at a relatively high rate to 5% moisture, a concentration which is normally obtained in paper drying. 0n the other hand, the mechanism of drying of thick sheets changes to that in which diffusion is controlling before the paper has become dried to 5% moisture. When diffusion is controlling, the rate of drying is very slow. This condition would require the use of very extensive drying equipment. The lower critical point was reached at different moisture contexts and temperatures for the thick and thin sheets, but the time taken to reach than was approximately the same in both cases. During this five minute period of drying the amount of water vaporized from the thick sheet was almost twice as great as that from the thin sheets. This means that the overall rate was almost twice as great for the thick sheet as for the thin sheet, which indicates that a thick sheet with twice the quantity of water can be dried within the same period and on the same equipment, with twice the quantity of steam being used. It is to be noted that the amount evapor- ated per pound of bone dry material was less for the thick sheet as compared to that vaporized from the thinner material. Considering each ply as a single sheet, it was observed that at am given time during the drying period the amount of evaporation on bone dry basis was least at the top ply which is at the open face of the slab and the greatest was at the bottom ply, (Graphs 21, 22, 23). In five minutes of drying time the moisture content of the bottom sheet was 8% while the top sheet still had 16% moisture on dry basis. At the end of the next five 29 minute interval the bottom sheet had a moisture content of only 2.1%, while the top ply showed a moisture content of 12.5 5. This showed that the bottom ply was drying out much faster than the top ply. The ply innediately above the bottom one was also drying out much faster than the top most ply and the one below it. Since the two bottom plies were drying out faster, the thermal resistance must have increased and the thermal conductivity decreased in these plies with an increase in the drying time. As a result, as drying time continued less heat was supplied to the top two sheets and therefore the moisture content remained higher in them as compared to the bottom ones. This can more clearly be understood from Table 11, which gives the moisture analysis of the plies at the end of 20 minutes of drying time. It is seen that the percent moisture left in the top ply is 8.55 while at the same time the moisture left in the bottom two plies is 1.68 and 1.33 percent respectively. No corelation was found between the temperature of the plies and the moisture content. The data on the rate of drying as related to time and moisture content have been shown in (Graphs 10, ll, 28, and 29). Using the accepted mech- anism of drying, the rate versus time curve can be divided into three dis- tinct regions. They may be defined by the mechanisms controlling the drying: (a) Unsaturated surface drying (b) Internal liquid diffusion (c) Diffusion from the interior of the fibre. Heat must be transferred from the hot plate to the sheet. The amount of heat transferred depends not only on the overall coefficient of heat transfer between sheet and ply but also upon the resistance to the flow of 30 heat within the sheet. Vapor forms in the region adjacent to the plate and passes up through the wet sheet to the outside air. As vaporization near the plate occurs the sheet is dried and becomes more resistant to the conduction of heat. It is not possible from these graphs (28, 29) to state the exact time or moisture content at which the critical water concentration would be reached because sufficient water was not present in the salnple. During the falling rate interval the decrease in rate was rapid. This continued for a little over two minutes when the moisture content of the samples were about 0.6 pounds of water per pound of bone dry pulp. The rate-time and the rate vs average water concentration curves were practic- ally straight lines. This corresponds to unsaturated surface drying. Be- tween 0.6 pounds 0f water per pound of bone dry pulp and less than 0.1 pounds of water per pound of bone dry pulp the rate decreased more rapidly. Internal diffusion between the fibres is assumed to be controlling. After this period there was another change in the mechanism of drying. In the interval from five minutes to twenty minutes of drying, the moisture content decreased from 0.52 pounds of water per pound of bone dry pulp for the thin sheets and from 0.95 pounds of water per pound of bone dry pulp for the thick sheets. It is believed that in this interval the mechanism of drying is suggestive of diffusion from the interior of the fibre control- ling the rate. Besides it must be noted that this latter interval extends over a period of fifteen minutes during which very small amounts of water were evaporated. The rate is very low but remains quite constant. This is significant from the point that it is extranely more difficult and time consuming to renove the water below this lower critical moisture content. 31 The overall heat transfer coefficient between the sheet and the plate was determined for the thick sheets only. It was found to decrease very rapidly with time from.122 B.t.u./(hr)(ft9(°F) to reach a.minimnm.of 0.9 B.t.u./(hr)(ft2)(°F). This minimum.was reached in seven minutes, at which point diffusion from.within the fibers appeared to have been controlling. Beyond this point the accuracy of the values are doubtful. They appear to increase but the apparent increase may be due to approximations made in the calculations. The corelation of the overall coefficient of heat transfer with mois- ture content indicates a gradual decrease in the overall coefficient as the evaporation continues during the period of unsaturated surface drying. The overall coefficient then falls sharply with further decrease in the moisture content to reach its minimum value. The drying curves in general agree with those obtained.bthcCreedy (15). The methods of experimentation as well as of conditions of drying which include the hot plate temperature, and the range of’moisture content of the samples, differ from that shown by McCreedy. In drying, the moisture content was such that no constant rate period was obtained; the whole of the drying period corresponded to the falling 'rate period. 32 CONCLUSIONS 1. 0n placing the sheet on the hot plate flash vaporization took place. This immediately increased the temperature of the sheet to about the atmospheric boiling point of water while the temperature of the hot plate decreased. The temperatures of the sheet decreased.to a.minimum and then increased. The temperature of a commercial Yankee drier may be expected to decrease in the same manner as the hot plate. 2. Evaporation was practically complete for both sheets in five minutes. At a moisture content of ten percent for the thick sheets and five per cent of the thin sheets, a critical rate change occurred. 3. No corelation was found between the temperatures of the plies and the moisture content. h. The entire period of drying corresponded to the falling rate interval. Three different mechanisms seem to prevail in this period. They are defined as follows: (a) unsaturated surface drying (b) internal diffusion (c) diffusion from the interior of the fibre. 5. The overall rate was almost twice as great for the thick sheets as for the thin sheets. 6. The specific rate on the basis of one pound of bone dry material was greater for the thin sheets than for the thick sheets. 7. The slow rate encountered during the period when drying is contri- buted by diffusion from within the fibers is not encountered in thin sheets, in drying down to five percent moisture; however this type of drying is 33 encountered in the case of drying of thick sheets to five percent. 8. The overall coefficient of heat transfer between the sheet and the plate, as calculated for the thick sheets, varied from 122 B.t.u./ (hr)(ft2)(°F) to 0.9 B.t.u./(hr)(ft2)(°F). 31+ BIBLIOGRAPHY 1. Adams, F. W. and Cooper, C. M., "The performance of Economizers in the Drying of Pulp and Paper', Trans. Am. Inst. Chem. Eng., _2_5_, 45, (1929). 2. Badger, W. L. and McCabe, W. L., "Elements of Chemical Engineering“, 2nd Edition, McGraw-Hill (1956). 5. Carrier, Ind. Eng. Chem., 15, 452, (1921). 4. Cowenz ”Smile Principles of Drying", Chem. Age (London), _5_9_, 410, 1958 . 5. Collins and Fisher, M.I.T. Undergraduate Thesis, (1927). 6. Doughty, R. 3., Tech. Assoc. Papers, Page 245, (1951). 7. Fisher, "Some Fundamental Principles of Drying“, J. Soc. Chem. Ind. , pg, 543—8T (1955). 8. Hinchley and Himus, Trans. Inst. Chem. Eng. (London), 3, 57, (1924). 9. Hinchley and Himus, Chem. & Ind., _4_§, 840, (1924). 10. Kirkbride, C. 0., ”Chemical Engineering Fundamentals“, lst Edition, McGraw—Hill Book 0o., Inc. (1947), page 45. 11. Lees and Charlton, Refrig. Eng., lg, 259, (1924). 12. Lewis, 17. K., Ind. Eng. Chem. 15, 427, (1921). 13. Lewis, McAdams, Adams, Pulp and Paper Mag. (Canada), _2_§, 122 (1927). 14. nartley, "Anals. of Applied Biology", _1_§_, 57, (1926). 15. McCready, D. 71., Am. Chem. Soc. (Abs.), 29, 7648-9, Nov.—Dec., (1955). 16. McCready, D. W., “Drying of Pulp and Paper', Paper Trade J., 101, No. 15, 65-66, 66-71, (1955). 17. McCready, D. W. and McCabe, W. L., 'The Adiabatic Air Drying of ?ygr0800pic Solids", Trans. Am. Inst. Chem. Eng. , 39, 151-60, 1955). 18. Minton, 'Driers in the Paper Industry", Paper Trade J ., _]_._(_)_6_, 50, (1958). 19. 20. 22. 25. 24. 25. 26. 27. 28. 29. 50. 51. 52. 55. 54. 55. 56. 57. 35 Molstad, et. 81., "Rate of Evaporation from a Free Water Surface”, Ind. Eng. Chem., 50, 1151, (1958). Montgpmerys ”Influence of Air on Drying“, Paper Trade J., 193, 50, 1957 . Newman, “Applying Diffusion Calculations to Drying Porous Solids“, Chem. & Met. Eng., 58, 710, (1951). Newman, “The Drying of Porous Solids; Diffusion Equations and Calcu- lations', Trans. Am. Inst. Chem. Eng.,.gz, 203, 510, (1951). Perry, “Chemical Engineers Handbook‘, McGrawhHill, (1941). Pukall, ”Drying of Ceramic Wear", Sprechsaal, £9, 567, (1926). Robson, 'Notes on Drying and Drier Operation“, J. Am. Cer. Soc., g4” 709, (1951). Running, T. R., "Graphical Calculations”, George Wehr, (1957), Ann Arbor, Michigan. Sanford, R., Worcester Polytechnic Inst., Undergraduate Thesis (1928). Seborg, C. 0. and Stamm, A. J., Ind. Eng. Chem.,.gé, 1271, (1951). Sherwood, T. K., "The Drying of Solids‘, Ind. Eng. Chem., 21, 12-16, 976-80, (1929). Sherwood, T. K., Paper Trade J., Feb. 2lst, (1929). Sherwood, T. K., “The Drying of Pulp and Paper", Trans. Am. Inst. Chem. huge a, 28, (1929)e Sherwood, T. K., Tech. Assoc. Papers, Page 12, (1929). Sherwood, T. K., "The Drying of Solids", Ind. Eng. Chem., 22, 152- 156, (1950). Sherwood, T. K.,!Applications of Theoretical Diffusion Equations", Trans. Am. Inst. Chem. Eng.,.gz, 190, (1951). SherWOOd, Ts Ks, Ind. Eng. Cheme, 23, 507, (1952)e Sherwood, T. K., ”The Air Drying of Solids", Trans. Am. Inst. Chem. Eng.,.ég, 150, (1956). Sherwood, T. K., "Air Drying of Solids", Chem. Eng. Cong. World Power Conf. (1956). 58. 59. 42. 45. 45. 46. 47. 36 Sherwood and Cummings, ”The Mechanism of Drying of Clays”, Trans. Am. Inst. Chem. Eng..g§, 118, (1952). Sherwood and Cummings, 'Mechanism of Drying of Clay", Ind. Eng. Chem., pg. 511-516,.E91.g§, (1955) Stacey, "Drying Rate Efficiency”, Trans. Am. Inst. Chem. Eng., 1§, 169-81, (1924). The Manufacture 9; Pulp and Pa er, Vol. 5, Page 51, McGrawaHill, (1925) . Troop and Wheeler, J. Cer. Soc. (Eng.),‘§Z, 505, (1927). Tuttle, J. Frank, Inst., £99, 609, (1925). Tu, C. M., M.I.T. Undergraduate Thesis (1928). walker, et. a1., "Principles of Chemical Engineering", McGrawbHill, 1957). Natson, "Some Remarks on Drying", Textile Col.,‘§;, 52—55, (1929). Witham, G. S., uModern Pulp and Paper Making”, P. 457, 2nd Edition, Reinhold.Publishing Corp., (1942). APPENDIX Time (min) HS 1'1. (graph) (egg) 185.5 178.5 165.5 155.4 141.0 71.2 187.5 181.5 169.1 156.9 142.5 TABLE 1. (GEE) 71.2 189.5 184.5 175.9 160.0 144.1 195.2 190.5 185.2 166.7 148.5 258.6 228.9 222.4 217.4 212.4 200.2 10 185.2 178.0 164.1 144.0 154.5 151.0 150.0 158.0 145.5 160.9 79.0 185.7 178.5 166.6 147.9 158.2 154.6 154.6 142.5 149.5 164.5 TABLE 2. Tu 12521 79.0 186.4 179.6 169.5 151.9 141.8 158.2 159.5 147.2 155.5 167.7 TB TBS (ggpl, (graph) 79.0 --— 186.8 187.4 181.4 185.6 172.8 176.4 158.0 165.0 145.0 148.2 141.8 145.4 145.6 147.7 152.0 156.6 161.4 167.4 169.5 171.5 TP 12521 259.0 226.7 221.4 222.3 215.4 211.6 214.0 217.0 224.8 250.4 255.4 Time (min) (Dmfl 10 15 14 15 T26 (Egaph) 184.0 178.0 175.4 147.2 151.0 128.4 124.0 125.5 128.0 155.0 158.0 144.0 152.5 160.5 168.7 12221 81.1 186.4 180.0 175.5 155.9 155.0 151.7 128.5 128.0 152.0 157.8 141.8 147.5 156.2 165.4 171.0 TB 81.1 191.0 186.0 185.0 167.0 141.4 158.6 156.4 155.7 158.2 145.0 149.0 154.0 165.5 171.0 177.4 TBS imam. 195.2 190.2 188.0 175.6 145.8 141.9 140.0 159.0 140.4 150.0 152.0 157.0 169.0 175.7 181.5 '1'? $252). 259.0 222.2 217.4 211.6 209.5 208.0 209.8 212.9 214.9 221.0 224.6 229.6 250.7 255.2 254.0 255.2 400340: 10 15 14 15 16 17 18 19 20 188.2 178.8 167.9 144.5 151.5 126.5 126.5 124.9 128.4 151.1 152.5 158.5 150.2 158.1 165.4 169.5 176.6 179.5 182.8 185.7 84.2 189.0 181.0 171.2 150.8 158.2 151.9 150.6 129.7 151.5 154.2 157.8 144.0 154.0 161.6 167.0 175.5 178.5 181.0 184.1 186.1 84.2 191.1 186.1 177.5 162.0 152.2 145.9 140.9 158.6 158.2 140.5 147.2 154.0 160.5 168.8 175.8 180.5 185.6 185.7 188.2 189.7 (graph) 192.7 188.8 180.7 166.4 159.1 154.2 148.0) 145.2 141.6 145.5 151.2 158.5 165.5 172.4 177.2 185.0 188.1 190.5 191.0 192.5 228.2 251.8 254.5 255.8 256.8 258.5 259.5 259.5 259.9 259.9 240.4 Time 14:41 NI-‘O TTS 1‘8. 181.2 169.5 155.5 148.5 145.7 TT 1.421 79.0 182.5 174.0 160.5 150.1 147.6 79.0 185.7 178.0 165.2 155.5 149.5 .12521 79.0 186.7 181.0 168.8 159.9 151.2 (graph) 189.0 185.5 171.7 165.8 152.7 12521 259.5 219.2 214.9 212.9 211.5 216.0 DIME-‘0 CDOI$ 10 174.2 175.4 167.0 155.6 141.5 155.5 127.9 124.5 120.2 125.9 (graph) 188.7 186.7 178.5 171.4 158.7 155.2 140.5 157.9 156.0 159.5 .12521 258.6 220.5 215.6 212.9 210.6 214.5 217.4 222.4 227.5 251.9 254.0 Time 0141 15 14 15 T16 TT LEEEEEL .12521 -—— 71.6 192.5 194.1 175.0 179.2 170.5 172.7 149.0 155.1 140.4 144.1 155.7 156.4 129.4 151.9 124.9 129.5 125.6 129.6 150.0 155.2 155.5 159.9 142.0 146.7 156.0 159.0 165.0 169.0 171.5 174.0 TABLE 9. 12921 71.6 185.4 181.4 175.5 157.5 147.9 159.5 154.6 152.6 154.2 156.9 142.5 151.9 161.1 171.5 176.9 71.6 187.5 185.7 177.4 162.0 152.4 144.7 140.0 157.5 159.6 144.1 150.1 157.5 165.7 174.9 180.5 BS (grag) 188.5 185.8 179.0 165.9 156.0 149.5 144.7 141.4 144.1 150.5 158.2 162.0 169.9 177.8 185.7 P 259.0 225.5 216.1 212.0 209.5 212.0 216.0 221.7 225.5 250.0 255.6 256.1 257.2 258.5 258.6 259.5 10 12 15 14 15 16 17 18 19 20 175.0 172.0 164.0 144.2 150.5 125.4 121.0 119.6 117.2 125.2 128.2 128.7 145.5 160.0 168.5 174.0 179.5 185.4 186.1 188.2 67.6 177.4 175.9 167.7 149.5 156.0 129.2 124.7 125.4 122.0 126.5 150.6 157.1 152.6 165.4 170.6 176.4 181.4 185.0 187.9 189.7 67.6 179.6 176.0 171.7 155.1 141.8 155.2 128.8 127.4 127.0 150.0 154.6 146.1 159.1 167.0 172.9 178.9 185.2 186.8 189.7 191.5 186.1 189.0 191.5 . 192.9 185.5 182.0 177.7 170.5 151.5 145.4 142.0 158.0 157.0 142.5 154.6 161.4 168.2 175.8 181.5 185.5 189.5 191.5 195.1 194.5 Time 1241 PO «30040) 10 15 14 15 16 17 18 19 20 T79 188.2 178.8 167.9 144.5 151.5 126.5 126.5 124.9 128.4 151.1 152.5 158.5 150.2 158.1 165.4 169.5 176.6 179.5 182.8 185.7 T7 84.2 189.0 181.0 171.2 150.8 158.2 151.9 150.6 129.7 151.5 154.2 157.8 144.0 154.0 161.6 167.0 175.5 178.5 181.0 184.1 186.1 185.2 174.6 157.6 145.4 157.1 155.0 154.2 154.6 157.5 145.2 149.5 157.6 165.2 170.6 177.8 180.1 182.5 185.4 187.2 T9 1252). 84.2 191.1 186.1 177.5 162.0 152.2 145.9 140.9 158.6 158.2 140.5 147.2 154.0 160.5 168.8 175.8 180.5 185.6 185.7 188.2 189.7 (graph) 192.7 188.8 180.7 166.4 159.1 154.2 148.0) 145.2 141.6 145.5 151.2 158.5 165.5 172.4 177.2 185.0 188.1 190.5 191.0 192.5 Time 1m). NI-‘O 01 T76 1‘8 181.2 169.5 155.5 148.5 145.7 12521 79.0 192.5 174.0 160.5 150.1 147.6 TABLE 7. 1421 79.0 185.7 178.0 165.2 155.5 149.5 TE 1252). 79.0 186.7 181.0 168.8 159.9 151.2 (graph) 189.0 185.5 171.7 165.8 152.7 (eXP) 259.5 219.2 214.9 212.9 211.5 216.0 Time (min) 0 1 (0QO 10 T75 (graph) 174.2 175.4 167.0 155.6 141.5 155.5 127.9 124.5 120.2 125.9 68.9 176.5 174.2 169.2 158.9 145.9 158.6 152.8 128.8 125.2 150.0 TABLE 8. TM 12.41 68.9 178.5 174.9 171.0 161.6 149.9 145.2 157.1 152.8 129.7 155.9 TB $.63). 68.9 185.2 180.5 174.2 165.5 154.0 148.0 158.9 155.1 152.8 156.5 (graph) 188.7 186.7 178.5 171.4 158.7 155.2 140.5 157.9 156.0 159.5 $2252). 258.6 220.5 215.6 212.9 210.6 214.5 217.4 222.4 227.5 251.8 254.0 Time 15 14 15 182.5 175.0 170.5 149.0 140.4 155.7 129.4 124.9 125.6 150.0 155.5 142.0 156.0 165.0 171.5 71.6 184.1 178.2 172.7 155.1 144.1 156.4 151.9 128.5 129.6 155.2 158.9 146.7 158.0 168.0 174.0 71.6 187.5 185.7 177.4 162.0 152.4 144.7 140.0 157.5 159.6 144.1 150.1 157.5 165.7 174.9 180.5 188.5 185.8 179.0 165.9 156.0 149.5 144.7 141.4 144.1 150.5 158.2 162.0 169.9 177.8 185.7 259.0 225.5 216.1 212.0 209.5 212.0 216.0 221.7 225.5 250.0 255.6 256.1 257.2 258.5 258.6 259.5 10 12 15 14 15 16 17 18 19 20 175.0 172.0 164.0 144.2 150.5 125.4 121.0 119.6 117.2 125.2 128.2 128.7 145.5 160.0 168.5 174.0 179.5 185.4 186.1 188.2 125.4 122.0 126.5 150.6 157.1 152.6 165.4 170.6 176.4 181.4 185.0 187.9 189.7 TABLE 10. TM 12521 67.6 179.6 176.0 171.7 155.1 141.9 155.2 129.9 127.4 127.0 150.0 154.6 146.1 159.1 167.0 172.9 179.9 195.2 196.9 199.7 191.5 TB 12521 67.6 191.4 179.9 174.6 162.5 146.5 159.9 155.0 152.5 151.7 155.7 145.2 155.5 165.4 170.2 177.1 192.1 196.1 199.0 191.5 , 192.9 TBS Tp (graph) ‘(ggpl —-- 255.8 185.5 220.6 182.0 215.2 177.7 212.9 170.5 215.8 151.5 214.9 145.4 218.5 142.0 220.6 158.0 222.8 157.0 224.6 142.5 227.1 154.6 250.7 161.4 255.6 168.2 256.5 175.8 257.2 181.5 258.5 185.5 258.0 189.5 259.0 191.5 259.0 195.1 259.0 194.5 259.0 TABLE 17 §2223 68.5 169.7 167.0 164.1 166.3 175.6 21919 257.6 251.8 219.6 215.6 217.4 219.6 #MNHO 0'! O) coooq 10 TABLE 18 .5222? 67.1 168.8 165.6 165.4 165.2 175.8 178.9 181.0 182.8 188.0 184.4 Q0301 00 10 12 15 14 15 TABLE 19 $193.12 67.1 167.7 165.9 165.8 167.0 172.4 181.0 184.1 186.8 187.2 188.6 189.7 190.8 191.8 192.6 195.1 £19132 259.5 226.9 217.4 214.5 215.6 217.0 219.2 225.9 229.6 252.2 254.5 256.1 257.2 257.9 259.6 259.0 (nah-«NFC coon-70: 10 I: 13 14 15 16 17 18 19 20 ZIBLE 20 .2921 67.6 171.0 168.4 165.2 170.2 176.5 179.6 181.9 184.3 186.4 187.9 188.6 189.3 191.1 192.6 194.0 194.7 195.4 195.8 196.3 196.5 Plate 239.0 229.3 221.7 216.3 217.0 218.3 221.7 225.5 228.9 231.4 233.2 235.4 236.8 237.9 238.6 239.5 239.5 240.4 240.8 240.8 240.8 'H-IICK SHEETS .1.. 1..-1.- 1 1-1.1-1111 .4 1 . 111.1111- 1 . 1 1 1. 1 . .1 1.7.1.1. -111- 1 _. . . 1 _ -..-1.11.1 . 1 w 91.1w 1 1.1 1 . u 1 1 11.11 p 1. 1 . 1 .1 11'1- 1. 1 1 11 111 1.1 ...-1.- .. 1 . ... - . . 1, 1 .1..- --1-. -- 1. - . --.1 1 1 1 1 -.-1-.. 1. _ . --.-11......- -.1 1 7* 1.. 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H . . .. . d . . . _V a .00 . 0. . 0 0 0. 1 a ) 3.00-0.)). )1 ..0) .)0L.).) 4.0) 7- .. .._ .. w _ _ a . _ . . _ .0 . ‘ h , U . . . . _ . . . . . . . _ . . . .- . .. . . V _ . . .. .. . .. Tril0 Qizl4litr|j )lh ) $— 0.000 )-0 1..-‘00 H9. L.r ~ )) V “F >0 0 1) .. [M h _ V 1%..) . H _ . .. . . _ - 0. . r . . . . 0 ...q 0. “...-mafia) . .. V. . 00.00)- )0.- _ . . u. . . _ . 000....) lui _ * a * . K _ :..“) M .h- ..H .. . V . u . . _. _ «- .0.... . . .uv t . . . . . . p . M . w . . . . w - . _ . .. .0000 ..0l 0 0 - )0 . 0.0.0 0 00.0 f-0. . t . .. 00 )) 0000.0) 001 0 0) .0 .00 .. ))0 b. .0 0 . . . . . . .. . . .. . . . . l 0.. . . . . 0. --. .- -- :0: -1--0.--. 0-0.171)- ...- :0: . F . fl 4 .1 0 0+ ...-J»): .. . N 0* fl $ _ . fl ., ... .. .. a) n . 01) . . .. . A “a ‘0. . . ¢ . .. . . * . M . n . . H . . . 0. ._-: 0. _I )| +0 \- ) I 40000. 0 00 Q +0.) L . . 7 0- :... -0 00. "J . . . - . V * . . . . .. . .. - V . ...sL . d . fl _ _ ._ . .. ~ V _ 0.0.. ....hv)0o. 00..0 0. 0000. I. at . 0 .10 . . . . a. . . .“ V. .. .. .. .. ....‘ . . H , .. a _ . H . . .. . . . _._0 4.. 0:.- .. .0; -00..0+.. .01.)- ..0 0.1). H .. .. .-. .10: L . _ . _ . . ‘ q _ . H . . . * ~ .. . . . . ._ . a .. H . .. . V . .. .~ . . ...» r)) )0) )))0) . )0)0) 0.). 00 r H .. . . V. . ... V . .. . . . V. )0----a)00 )0. r -00.)». p ..I - . 1 0.)” )._ ..L L., . h . THIN SHEETS .— a IIII.I.I 1 A I I I IIII1 ,IIIIIIIIIIIIIII IIIIII ,I‘ II‘II _,_;.- I 4p.-.—..I.---. I .4»- -..—..I_L..V-- n . 5M ~.—A>._pv~a—a—.— .... ~ _ I I . ---.L..-_.. ...”...h. , , T ' I I.--—_+...<-._.I . . . I I , . v -I.. I TIIHII-I+ o .m .. H .g . I. .I D --II- I 5 i I o I II.-. .. fl __ I I I I I I v v I .....H 4,. “‘P" -->-~I‘ -_ -. . _ . Vwo—fi »'»-—q—. . ”91.4..-“ ---. I--; .--... . _ . .V _ III. I? I I III .aIIIIII. + v IIII It .IA III IIII4 .IQ II p . , I. I . A. Q . . +I . . _. . , . H » II 4 u r I I _ . I . I , . I . < -_ I ..-..‘p-.. _._. i I .— ._.+._..-_._1 ;-.“. I..-_._..—J I I A I If I- I I l ,. . . H .., V m . ~ I Iu.I..Iw , I VIII.» I H .... .L V . N d . w u m. .V... H n . _ . VIII c I .II ‘.!.IIIOII‘IOI‘I o I.I . II II _ III! .I \I. ,l I JI I .4 IIA I I4 . _ V . . I . ‘ .. I m , _ m V _ .. . V II.IlIIlI II M - . . . .. _ , . c w m . . _ . . _ a , , . _ I-.. III .I.IHIIII¢.III+.LI I.I-I..II.II. . ._ ._ I ‘I I . , ’ . w v _ . A. ‘ aIlII II » III III; . .. .h . .. _ . . . I —< . - IIITI IILYIO I II I I » I -—o 4- ...-L- -.1 ' I ' .o—- ....4 “...“... _I... ”_,.Ip. I I .V.— ...» . I....w- . - -4--....- I I I t I ~—II~¢ v. _ v - -++——.— ...- ..- {pg-fa... I I I fimm'7*" I I i I~ I km” I I . . . . IAIWI. > .IfiI.I.¢ 1 H I .o I" . . V Q . a I | I I. I.IIIII III+IIII IL I I I4 I. k . _ V . _ J . _ I , D. . n w # n . Q1 . I II. III II II 0, .V . V . VI . . . . . _ . .. . . .. Ia . I II I .II4.I.: IA? III1I. III TIIIIHII I I4 . u- N . . o. W . . , .I I. I. . T rIIQII.II4 . ~ 1' . . > _ I . H I m . .. fl . _ III I. III III. IIII I II III. III I IIIbIIII I a v .V — V .. I._ . . ... . _ . l 0 p Q , IIII , IrlII AYI IIIII . « I“ ' o . V _ l . . J — .. I V' T . 4 I ..- -~...1.-_I - ...; - ,........4L...._-_l‘ .... -., _ I -- -I-“--LW I . ' I V .4— I ; - I I I I I I I I L I I f‘ I I I --—I I T7 ‘I .‘- I *I‘ I . ...!" L 1' 2 . ..YA-— -- ba—J ._ ‘IL‘"“*' - "AL... -, I I ---'+ I I I I --- - ----1" - I ' .4 I I I".' V4,-.- I I ~’*.r**“ff' I I "I I I I I I "1 “”"' “17’" I I J! .- .4-..” 4“,. . I I I I I I I I . §~o a- M w» - -——~—--—- I .I;.. MI. .-.. ; ' “_-‘oMo- d—w—Q -— v u . I I I I I ;;-...' IW . . TI! IH IIIIO TV-” _ . I. . _ L.....;_.._._ .. ..I I --< ,..-. 7 4-... fl- I I ,I I -I I I T I _ I IIIIL IIII _ . .-. I I IIIIA, III I .....— .-.—...- I I.IIL III II II. AYI. IIIMIII IA -—_H.-. -,.- -7 ”WV.— . I ' I ’ I I I I I ‘-—- >-~ r. I {I}L_ ___ ...." I I - I». "’I"_"". .4. f I . I-~ - :. ~0“—‘— - I .., : . I I . «\6 u . v . .I _I I I D . V. . . _ o ”— O . . _ . _ M .. _, III. piqllzl ... .0 IIIA III 0 Q 0‘!!! VI A . . . . . II «III; # _ _ _ . . g . . .— . . , . o . — . . . . ‘o H V F .I. .h « I I”n.fl\l..‘i.fl«.r1"lluu. ' I I'IIIIIIIIIIIIIIIIHIIIQI «IIIII. _ I IIHHI'I'IIIV H 4 uliIIIIIIII III‘I‘II'III II IIIIIIIIIIIIIIIIIl—I'I'IIIII‘.IIII.IIII-» IIII‘I! III-III" Illl IIIHI J: IIIIIIIIIIIH H H U H H HI H H . . . I H . H . H u H p H m . U H u H — » H H “ . . . _ _ . w n w — . H _. - I- I; ....H....... _.HI IIH - I HI. .LIH . I- H.. I- I; .H .I. L: - - I-ILIH III I _ H H H H I H H _. . H I H I H H I H H . _ I H H .I H I H H H H . H I I H H H H . H H I._ . H H . H I . H I. H T .I.. I”! I r I I I I.I I H H I -III _III -IIIIIIIII. III II IIIIIII I-IIIrI-IIIIIILIII IIIIIII- IIITII+ III. III I .III H H I H H I. H H H H I H . J H H. _ H .H HI I H H I I. H H H . I ... H H H H. H H H. H. H . H H. H._ II H H H H H . I H H H H w H . _ H — .I. — . I . . I . .. I . c . H H . u ..H H H I. M .I. 4 I “III; I.IWII I I IIm I IIfl I.IIIT II .I III.II.I II I L . I IIII“ . . :IIIWI I if . I 4I.III. LII: II III “ I Il.v . I I ”III? III HI . II? I.Il .W.II.I4 II + ;II I II I. _m III III .II+ . I) .. II I? I .II a II IA ¢ III. I.I. I _ .-H _ H H H H .H . . .H I. III. . H .I. H ... H H H :H m H H H H H .I _ H H H H H H .H H .H . H H H H H H H I , III H . H H a H . . g. H ~ H. I 4 < H .H_ . . . . . . _.II I HH‘II H IWI.I I” w “ Ir“ I — R1 w H T 4‘ HIIIIHPI . H P H II I” . IOIIIIIJIIIITIII‘IJIIIII I‘I+.IIIII.II.I*IIIIIIIIHIIIIIQ|0. III-’IL H . H _I .I I H HI H H . H u I H H H Im ” I. I U m . w I H. I . H a . H . .H .* w I . . — H . H . . . m . w w h.. H . n H H _ . I. a m _ . I. H. I “-I.-.- .,I II I-IIHIIIII- I I. I-./1H -III -I-, II .I. II . :1 HI I II HIII I I--- I.I.-IH I. -I .I. II I .I.... I.I.IIIIIHI...IM.I. ;--: I.I-Ifi- I.I.III I- I III. IIHI- ILII IH . II* I A... . Y 1* H Iw W I” .I. H b . H . 1 M 4. w . . I _ . _ _ H v H ‘v H . H _ H H _ H I I . HHI I HH ‘. H H; HIIH H H HIHI H “..H . H H H H I. H H _ H H H. H. .I L H .H H I, . .H H H I..... II I 1 I . II > . III-I. Jr >1 I I0 I I H . H H II. III I _ II I. III. I I- I; r I. I I fl I _ . . H . ¢ 1: H v N I, . . . w .. .I I m I.I—1| I‘l'. . “I H I 1.."! H H c I. . _ H H . H H H . I I . . . . H H H . H H H H H H H H H .. H H. H H_:_ H . H H H .H H H H . I H H I . I I 4 I III III IIJII I 4 III IHT III-I II WII IW I I V I. IOIII I 4 II ILTIIII 4 HI OI+IIII III I IIIII 0 II IIYIIIIII+II II; IIIIIIVIIOII .III I ..IIII... III II OIII IIAfi. III I. ‘1 _ I IIJI III I r» I.III I .I. ~ I I H. II II . IWII III. 0 I.IH I I I IL . H . H H H A I I I I I H H . . . I » o I. . . c . I" . . I . H I . - . . _ H o . — “o H m H m. W . I.I . . H W ..H HH a .I.. . ~ H: H . I w . . v . . . + o H .I . . a o _ H . . . H. H H H . H v . I H u *I . “I. II I W H Jur AI I I. 1 p F H # w “I . F“ a > IL— PI .II I‘ll. L— I.I: .IIIiIIIII'II. TYI‘IIII LII'II. «IA H . .. H . I H I . _ . H I H H H. .H ... .H. H H H H. .. H ..H H .H I. _ ”.ITH .H H H H .H. H H .HI _ . I . I» H H H .H. . .. . fix .I H I v . 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