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Abstract
Gas-liquid mass transfer has been studied in a membrane module with non-wetted microporous fibres
in the laminar flow regime. This new type of gas/liquid contactor can be operated stabily over a large
range of gas and liquid flows because gas and liquid phase do not influence each other directly. Therefore
foam is not formed in the module, gas bubbles are not entrained in the liquid flowing out of the reactor
and the separation of both phases can be achieved very easily. These phenomena often limit the appli-
cability of conventional contactors, e.g. a bubble column which was also studied in the present work. The
large mass transfer area of a bundle of small fibres offers the possibility of creating a compact gas/liquid
mass exchanger. However, owing to the small channels in and around the fibres the flow of either gas or
liquid becomes laminar which reduces the mass transfer capacity of the module. Therefore the mass
transfer coefficients in the laminar flow regime were determined experimentally. For mass transfer de-
termined by the transport in the liquid phase it was found that the active mass transfer area is equal to
the total membrane area, regardlessthe porosity of the fibre. For processes with liquid flowing through
the fibres, the influence of fibre diameter, diffusivity in the liquid, liquid viscosity and liquid velocity on
mass transfer can be correlated extremely well with the Graetz-L&hue solution derived for the analo-
gous case of heat transfer. For liquid flowing around regularlypacked fibres mass transfer was described
satisfactory with a correlation derived from a numerical solution for the similar heat transfer problem
[ Miyatake and Iwashita, Int. J. Heat Mass Transf., 33 (1990) 4161. Correlating mass transfer in liquid
flowing around irregularly packed fibres was not possible because of the undefined dimensions of the
different channels between the fibres.
3. Literature
CrER =C,=mC,, OG.zGZ
A limited amount of papers concerning the
ac
- experimental verification of eqn. (4) is avail-
(ar> r=O
=o, o<z<z able. For heat transfer applications Sieder and
Tale [ 91 developed an expression similar toeqn.
For a fully developed laminar flow in a tube the (4a) for the Nusselt number form their exper-
velocity profile can be described by: imental results. In their empirically obtained
correlation, they also incorporated the influ-
01
2
branes water is not absorbed in the fibre wall. teraction of the different fibres must be taken
Therefore mass transfer in the free liquid can into account and therefore a three dimensional
be measured directly. Yang and Cussler [13] problem is obtained. A simple two dimensional
studied gas-liquid mass transfer. They deter- approximation of the fibre bundle is flow
mined the influence of velocity on the mass through an annulus.
transfer coefficient for laminar flow empiri- Lin et al. [ 171 used an electrochemical
cally by desorbing 0, from water. The results method for the determination of mass transfer
of experiments with liquid flowing through the coefficients in such a geometry. This method
fibres corresponded to eqn. (4a). cannot be used in real pipe flow because it needs
Qi and Cussler [ 141 measured mass transfer the use of two electrodes (Mixushina [ 181).
coefficients with the absorption of CO2 in a so- One being the tube wall while the other elec-
lution of sodium hydroxide. It might be ex- trode must be placed in the liquid stream, which
pected that the mass transfer process was in- disturbs the flow. Lin et al. translated their ex-
fluenced by the chemical reaction between perimental results with the use of the hydraulic
hydroxide and carbon dioxide (Kreulen [ 151) . diameter to give results which corresponded to
However, the dependency of the overall mass eqns. (4).
transfer coefficient on the liquid velocity was Yang and Cussler [13] also carried out ab-
found to be in accordance with eqn. (4a). sorption experiments with liquid flow around
When the porous fibres are used in absorp- the fibres. Like Lin et al. they also used the hy-
tion experiments the question arises which area draulic diameter for the translation of their ex-
of the porous membrane should be taken as the perimental results to the dimensionless corre-
exchanging area. Either the open pore area can lations. The mass transfer coefficients were
be chosen or the area of the total membrane found to depend almost linearly on the liquid
(i.e. pores +polymer ). In heat transfer and velocity. This is not in agreement with eqns.
mass transfer with soluble walls, the complete (4).
tube area is taking part in the transfer process. Recently, a numerical solution was pre-
This assumption is also used in the solution of sented for heat transfer in the shell side of a
eqn. (1). shell-tube heat exchanger by Miyatake and
Wakeham and Mason [ 161 developed a gen- Iwashita [ 191. From their numerical results di-
eral mathematical model to describe diffusion mensionless Nusselt correlations were derived
through perforated layers into a stagnant which can also be useful in the interpretation
boundary layer. One of their asymptotic solu- of experimental mass transfer data for hollow
tions may be applicable to the absorption pro- fibre modules (Appendix A). However, there is
cess with porous membranes. The main param- one very important difference between this type
eters which must be considered are the distance of heat exchanger and a commercially available
between two pores and the thickness of the membrane module. The tubes are welded in a
boundary layer. In the present work these pa- regular packing while the fibres are not posi-
rameters will be evaluated for two types of tioned regularly during the construction of the
membranes with different porosities to deter- modules. In the present work a module with
mine which area should be taken. regularly spaced fibres was used to compare its
The mass balance for absorption in the liq- performance with that of modules with irregu-
uid flowing around the fibres cannot be solved larly spaced fibres.
as easily as with liquid through the fibres which Due to differences in fibre diameter or in the
is in fact a two dimensional problem. The in- channel widths between the fibres, substantial
202 H. Kreukn et al./J. Membrane Sci. 76 (1993) 197-216
maldistributionof the liquid around the fibree calculatedfrom this degree of saturationmay
can occur. This can have a large influence on deviate substantially from the mass transfer
the efficiency of mass transfer as is shown in coefficient obtained from the degreeof satura-
the next section. tion in a bundle of fibres having exactly the
same diameter.
4. Effects of maldistribution of phases in To show this phenomenon,the absorptionin
hollow f’ibre modules modules with fibres which have a certain di-
ameter distribution, is mathematically anal-
In a lot of massexchangingequipmenta non- yses. Three distributionsare considered. The
idealdistributionof gasand liquidphasecaused first assumesa normalprobabilityfunction for
by the heterogeneityof the contactor resultsin the fibre diameters:
lower efficiency of the absorption which leads
to an incorrect interpretation of overall ab- (5)
sorption data. Schliinder [20] developed a
mathematicalmodel to estimate these effects The second distribution assumed an equal
in fixed beds, fluidisedbeds and bubble trays. probability for each diameter in the range of
In membrane modules maldistributioncan variation,f(d) = constant. In the third distri-
occur on both sides of the membrane; (1)the bution only two fibres are considered with di-
effect of the thickness of the membrane wall ameters equal to the boundary values for the
which effects the actual pore diameter in the fust and second distribution.It must be noted,
lumen,and (2) local variationsin the arrange- that this case is not encounteredfor the fibre
ment (pitch) of the membranefibres resulting modulesavailable,it is only used as an illustra-
in preferentialflow paths owingto differenthy- tive example.
drodynamicalresistances.The estimationof the The degreeof saturationin a f’ibrewith a fully
effect of the latter phenomenon on maldistri- developedvelocityprofileis calculatedwitheqn.
bution is very complicated and requires the (6).
availability of three-dimensional hydrodyn-
amical one-phase flow models in combination ?=1-exp(-E)=1-exp(-$?) (6)
with a mass transfer model. The estimationof
the first effect on the performanceof the mem-
The mass transfer coefficient k can be calcu-
brane module will be discussedin this study.
lated from a generalisednumericalsolution of
The fibres can introduce a similarheteroge-
the Graetz-L&que equation. Curve fitting
neitybecausethey do not haveexactlythe same
yields eqn. (7) which is also valid in the range
diameter. Moreover, the channels around the
of Gz numbers not covered by eqns. (4a) and
fibres do not have the same dimensions be-
cause the fibres are usually not installed regu- (4b).
larly in the modules. With the same pressure
differencebetween in- and outlet of the fibres Sh=;&.67”+ 1.623Gz (7)
or the channels,unequalflow ratesthroughthe
fibres or the channels are obtained This re- The velocity in the fibre is calculatedfrom the
sults in different degrees of saturation of the Hagen-Poiseuilleequation.
liquid at the outlet of the fibres. The flows of
the individual fibres combine to give a mean (6)
degreeof saturation.Mass transfercoefficients
H. Kreulen et al./J. Membrane Sci. 78 (1993) 197-216 203
0.88
0.0 0.1
(9) 0.2 0.3 0.4 0.5 0.6
2 Cm)
TABLE 1
Membrane specifications
TABLE 2
Module specifications
Code Fibre type d-w Length Nr. of fibres oLin oL0ti %bra
(lo-’ m) (m) (m-l) (m-l) (-)
polyurethane
potting
cz
-=-
hbs
(12)
/ \ G mQV
The determination of solubility and diffusivity
parameters of COP in the glycerol/water mix-
tures is reported in Appendix B.
FI
module
*2 Pump
102,
Sh Surfaceporosity
0 70%
l 3%
10’ :
- 100%. Eqs.4
100 I .-
10 ’ 10 * 10 3
GZ
Fig. 6. Absorption data of COz in water with two fibres with different surface porosities compared to the theoretical solutions,
eqns. (4).
TABLE 3
given together with the number of pores per area tioned in Appendix B. The data calculated from
at the interface. Thus a very small liquid layer the experiments are shown in Figs. 7 (a), (b)
adjacent to the fibre wall can be considered as and (c) for fibres I, II and III respectively. They
completely homogeneously saturated. From this are well described with eqn. (5a).
layer the diffusion process into the flowing liq-
uid takes place. In the further interpretation of
absorption data the total membrane area will
Modules with liquid through the fibres
be used as the interfacial area through which
In section 4 it was deduced that if only a mi-
the transport takes place. Keller and Stein [ 221,
nor spread of the diameter of the fibres in a
Malone and Anderson [23] and Lopez et al. bundle is present, no difference can be ob-
[ 241 have considered analogous phenomenon.
served between the absorption in liquid flowing
through the bundle or a single fibre of the mean
diameter. The absorption data measured with
Single fibres modules of type I and II fibres are shown in Fig.
In the absorption experiments with the dif- 8. Like with the single fibres the experimental
ferent viscous liquids mass transfer coef& data are in close agreement with the theoreti-
cienta were calcuIated according to eqn. (6) and cally derived solution (eqns. 4). It can be con-
translated into the dimensionless Sh and Gz cluded that the difference in fibre diameters is
numbers with the physical constants men- negligibly small.
208 H. Kreulen et al. jJ. Membrane Ski. 78 (1993) 197-216
w% glycerol
Sh
in water
0 0
l 50
o 80
10 ’
- Theory. Eqs. 4
10 O
I 4
GZ
A w% glycerol
in water
0
l
50
65
q 80
I 90
- Theory. Eqs. 4
102 -J
I
w% glycerol
Sh in water
0 50
l 65
- Theory, Eqs. 4
(cl
10’ ( I I
10 3 10 4 10 5
Gz
Fig. 7. Absorption data measured with a fibre of type I (Table 1) in different glycerol/water mixtures with a fibre of type
(Table l), (a) type I, (b) type II, (c) type III.
Modules with liquid around the fibres is plotted, modified for mass transfer outside
The results of the experiments are presented the fibres in a bundle (Appendix A). The ab-
in Figs. 9 (a) and (b). In these figures also the sorption in module A (Fig. 9a) with regularly
relation derived by Miyatake and Iwashita [ 191 placed fibres in a triangular pitch agrees well
H. Kreulen et al./J. Membrane Sci. 78 (1993) 197-216 209
10 2
w% glycerol
-. Module type
in water
Sh
1 0l 015
(Table 2)
2
q 50 A
n 65 A
10 ’ X 80 A
,/- + 90 A
1 A 50 B
- Theory. Eqs. 4
102
w % glycerol
Sh
in water
0 0
0 15
0 50
8 6.5
+ 80
X 90
102
Sh
ce
0
oo”
0
0
(b)
100 I - --.---., . . . . . . ..-
10 1 10 2 10 3 10 4
Gz --
Fig. 9. (a) Absorption data measured in a regularly packed hollow fibre module with different glycerol/water mixtures
flowing around the fibres. (b ) Absorption data measured in an irregular packed hollow fibre module with a 50 wt.% glycerol/
water mixture flowing around the fibres.
210 H. Kreukn et aL/J. Membrane Sci. 78 (1993) 197-216
w%glycerol
in waler
0 0
l 15
n 50
l 80
Fig. 10. Oxygen absorption measured in a bubble column with different glycerol water mixtures as a function of gas velocity.
with the theoretical solution of Miyatake and Mass transfer is also strongly dependent of
Iwashita.Small deviations must be attributed viscosity. At the lowest gas phase velocity izLu
to in- and outlet effects and the influenceof the differsa factor of 30 for the absorptionin water
wall of the module which are not incorporated and the 80% glycerol mixture, while at the
in the theoreticalequation. highestvelocitiesthis factor is about 125.
The resultsobtainedwith moduleB (Fig. 9b) If it is assumedthat the diffusion coefficient
show a largedifferencewith the solution of Mi- of oxygen shows a similardecreasewith the in-
yatake and Iwashita.It can be concluded that crease of the glycerol content as the diffusion
the irregularpacking of the fibres does not al- coefficient of carbon dioxide in these liquids,
low the use of the approach of Miyatake and the diffusion coefficient lowers a factor 10 be-
Iwashita.The effects of the liquid distribution tween water and the 80 wt.% mixture.Calder-
(section 4) must be considered to explain the bank et al. [27] correlated IzLwith the square
absorptionbehaviourof moduleswith irregular root of the diffusioncoefficient,which meansa
packing of fibres. decrease of kL by a factor of about 3 between
water and the 80% glycerolmixture.Thus not
6.2. Bubble column only the lower diffusion coefficient is respon-
sible for the largedecreaseof kLu with increas-
Experimental K,a values obtained with ab- ing viscosity, but also the smaller interfacial
sorption in the bubble column, are plotted in area.
Fig. 10. The gas phase velocity could not be in-
creased above 1.5X 10m2m/set because foam 7. Discussion, bubble column versus
formation occurred in the water/glycerol membrane module
mixtures.
Mass transferis positively influencedby the To compare the performance of the hollow
gas velocity but this effect is less pronounced fibre membrane module with the bubble col-
in the more viscousliquids.Similareffects were umn, absorption processes under similar con-
measuredby Buchholz et al. [ 251 and Voigt et ditions in these co&actors must be studied.In
al. [ 261, who also studiedoxygen absorption in the presentwork the degreeof conversionthat
glycerol/water mixturesin bubble columns. can be realizedin the co&actors was used as a
H. Kreulen et al./J. Membrane Sci. 78 (1993) 197-216 211
TABLE 4
Comparison of hollow fibre membrane module (hfmm) with bubble column (bc )
tool for comparison. No allowance has been Although in Table 4 only the KLavalue for
made for additional aspects, e.g. pressure drop the most viscous glycerol/water mixture is
and the cost of investments. From the experi- higher for the hollow fibre membrane, the sat-
mental results it is concluded that mass trans- uration which is obtained in both absorbers is
fer in liquid flow through the fibres is described always higher with the hollow fibre module.
well with eqns. (4). In this section these rela- This effect is caused by the difference in the
tions are used to predict the absorption in a gas/liquid mixing in the absorbers. While the
hollow fibre membrane module which can be bubble column can be considered as a stirred
compared to data for the bubble column used tank, the contacting in the fibre module is bet-
in the experiments. Therefore a membrane ter described with plug flow.
module with fibres of type I (Table 1) is as-
sumed with the same liquid hold-up and liquid 8. Conclusions
height as the bubble column used in the exper-
iments. Such a module has a specific interfacial In the present study the applicability of hol-
area of 2000 m2/m3 with a fibre length of low fibre membrane modules in gas/liquid con-
1.8X10-l m. tacting processes was investigated. These mod-
From these data and eqns. (4) and (6), the ules offer the possibility of an increased
mass transfer coefficient, &,a and the degree of absorption capacity by applying small fibres in
saturation of oxygen in the water/glycerol mix- the modules which creates high interfacial
tures can be calculated for the hollow fibre areas. On the other hand, due to the small fibres
module. These results are compared with the and the narrow channels around the fibres, the
experimental data of the bubble column in Ta- phases on either side of the membrane are
ble 4. It is assumed that the diffusion coeffi- bound to flow laminarly, which may reduce the
cient of oxygen shows a similar decrease with absorption capacity again.
the increase of the glycerol content as the dif- In an absorption process carried out with a
fusion coefficient of carbon dioxide. microporous membrane module no special at-
When viscosity increase, kLa decreases for tention has to be paid to the separation of gas
both types of absorbers. However, while the in- and liquid phase. In the present work absorp-
terfacial area of the bubble column is also low- tion in viscous liquids was studied, because in
ered by viscosity (section 6.2), in the fibre this field the gas/liquid contact in the mem-
module this is not the case. Therefore, IzLaof brane module looks very attractive. Since gas
the module gets larger than kLuof the column. and liquid flow are separated by the membrane
212 H. Kreukn et al./J. Membrane Sci. 78 (1993) 197-216
no stagnant gas bubbles were formed in the liq- module and the bubble column are compared
uid nor was any foam formation observed. in terms of kLa, the module only shows a better
These two phenomena are known from indus- performance for more viscous liquids. This is
trial practice while they were also observed in caused by the fact that the mass transfer coef-
the application of the more viscous liquids in a ficient and the interfacial area in the bubble
lab scale bubble column. column are reduced while in the membrane
From the absorption experiments carried out module only the mass transfer coefficient is af-
in the membrane modules it was concluded that fected by an increasing viscosity.
although the gas is only in contact with the liq- Absorption capacity can also be compared in
uid at the pore mouths, which cover the area terms of the degree of saturation that can be
only partially, the total membrane area has to obtained in both absorbers. Because of the dif-
be used as the exchanging area for the deter- ference in the mixing pattern, ideal mixing for
mination of the mass transfer coefficient. Dif- the bubble column and plug flow for the mem-
fusion takes place effectively from the liquid brane module, a higher degree of saturation in
layer adjacent to the fibre wall which is homo- the membrane module is reached in a case with
geneously saturated, because the distances be- an equal mean residence time for the liquid.
tween the pores are extremely small compared
to the distance for diffusion to the centre of the Acknowledgements
fibre.
For predicting mass transfer in laminar flow These investigations were supported by TN0
through a single fibre, the Graetz-L&kque the Netherlands organization for applied sci-
equation can be used which was originally de- entific research. We also acknowledge G.
veloped for heat transfer. In a module, how- Schorthaar for the construction of the experi-
ever, due to small variations in fibre diameters, mental setup and E. Kippers for his part in the
differences in saturation per fibre can occur. experimental work.
With the aid of a mathematical model it was
demonstrated, that these differences were neg- List of symbols
ligible compared to the experimental accuracy
and thus the Graetz-L&%que equation can also A membrane area (m”)
be used in the case of a bundle of fibres in a C concentration ( mol/m3)
module. Mass transfer in a laminarly flowing d tibre diameter (m)
liquid around regularly packed fibres can be es- D diffusion coefficient (m2/sec)
timated satisfactory with the results of the nu- GZ Graetz number (- )
merical solution for the similar heat transfer GZ’ idem, defined in Appendix
problem obtained by Miyatake and Iwashita J absorption flux (mol/m2-set)
[ 191. Normally produced hollow fibre modules k mass transfer coefficient (m/set)
have irregular fibre packings and therefore a
wide variation of the dimensions of the chan-
nels occurs leading to substantial differences in
tu
P
distribution coefficient (- )
Nusselt number
pressure ( N/m2)
flow rates. Therefore the method of Miyatake 8" volumetric flow rate (m3/sec)
and Iwashita [ 191 cannot be used and it is very radial coordinate (m)
difficult to predict mass transfer in liquid flow- ii fibre radius (m)
ing around irregularly packed fibres. Re Reynolds number (-)
If the absorption capacity of the membrane S half pitch between fibres (- )
H. Kreulen et al./J. Membrane Sci. 78 (1993) 197-216 213
22 K.H. Keller and T.R. Stein, A two-dimensional anal- Triangular array, 1.0 <Z< 1.1:
ysis of porous membrane transport, Math. Biosci-
ences, 1 (1967) 421. Sh=9.26(1+0.0179Gz’1.46) 1’4
23 D.M. Malone and J.L. Anderson, Diffusional bound-
ary-layer resistance for membranes with low porosity, Square array, 1.0 GE< 1.2:
AIChE J., 23 (1977) 177.
24 J.L. Lopez, S.L. Matson, J. Marchese and J.A. Quinn, Sh=4.08(1+0.0349Gz’1.46)1’4
Diffusion through composite membranes. A two-di-
mension analysis, J. Membrane Sci., 27 (1986) 301.
Triangular array, 1.1<Z< 4.0 and square ar-
25 H. Buchholz, R. Buchholz, H. Niebeschlitz and K.
SchUgerl, Absorption of oxygen in highly viscous ray, 1.2 <Z< 4.0:
Newtonian and non-Newtonian fermentation model
media in bubble column bioreactors, Eur. J. Appl. Mi-
crobiol. Biotechnol., 6 (1978) 115.
26 J. Voigt, V. Hecht and K. Schiigerl, Absorption of ox-
ygen in countercurrent multistage bubble columns. II, Triangular array:
Aqueous solutions with high viscosity, Chem. Eng. Sci.,
35 (1980) 1317. 8.92(1+2.2&P)
27 P.H. CaIderbank, D.S.L. Johnson and J. Loudon, f=
Mechanisms and mass transfer of single bubbles in l+6.86@5’3
free rise through Newtonian and non-Newtonian liq-
2.34(1+24@)
uids, Chem. Eng. Sci., 25 (1970) 235.
28 P.H. Caiderbank, Mass transfer coefficients in gas- g= (1+36.5@5’4)(2fiZ2-x)1’3
liquid contacting with and without mechanical agi-
tation, Trans. Inst. Chem. Eng., 37 (1959) 173. Square array:
29 R.A.T.O. Nijsing, R.H. Hendriksz and H. Kramers,
Absorption of CO, in jets and falling films of electro- _ 4.00(1+0.509@)
lyte solutions, with and without chemical reaction,
I-- l+0.765@5’3
Chem. Eng. Sci., 10 (1959) 88.
30 R.B. Bird, W.E. Stewart and E.N. Lightfoot, Trans- 1.69(1+9.1@)
port Phenomena, Wiley & Sons, New York, NY, 1960.
31 G.F. Versteeg and W.P.M. Van Swaaij, Diffusivity and
g= (1+10.8@5’4) (~cJ~-Ic)~‘~
aolubility of acid gases in aqueous amine solutions. J.
@=X-l
Chem. Eng. Data, 33 (1988) 29.
Appendix B
Appendix A
Heat transfer correlations of Miyatake and Solubility and diffusivity of CO, in glycerol-
Iwashita [19] modified for muss transfer water mixtures at 298 K
In this appendix the heat transfer correla- In deriving the Sherwood relations for mass
tions derived by Miyatake and Iwashita [19] transfer in hollow fibre modules which were op-
are given, modified for mass transfer. Different erated at 25 oC, the diffusion coefficient of CO,
equations were obtained for triangular and in the glycerol/water mixtures is needed. Val-
square arrangement of the cylinders and differ- ues in mixtures with a glycerol content between
ent ranges of the relative distance between the 0 and 70% have been reported by Calderbank
cylinders, Z. The fibres in the regularly packed [28], who derived the data from experiments
module used in the present study were ar- in a liquid-jet. In the present study diffusion
ranged in a triangular array. coefficients for mixtures with higher glycerol
H. Kreulen et al./J. Membrane Sci. 76 (1993) 197-216 215
TABLE B-l
TABLE B-2
contents are reported These were determined mixtures was determined in a stirred cell as de-
in experiments with a laminar film reactor. scribed by Versteeg and Van Swaaij [ 311.
For the determination of diffusion coeffi- The results of the solubility experiments are
cients from absorption experiments the lami- reported in Table B-l. The solubility is ex-
nar flm reactor is widely used as a model re- pressed as the distribution coefficient, the ratio
actor because the interfacial area and the of concentration in liquid and gas phase at
hydrodynamics of the liquid phase are known, equilibrium. Viscosity and density of the glyc-
see e.g. Nijsing et al. [ 291 and Bird et al. [ 301. erol/water system are also reported in Table B-
From the experiments the product of solubility 1. Viscosity was determined using Ubbelohde
and the square root of the diffusion coefficient viscosimeters and density was measured in
can be derived. Therefore the solubility must pycnometers. Both apparatus were submerged
be measured separately in order to be able to in a thermostatted water bath, which was op-
calculate the diffusion coefficients. In the pres- erated at 25’ C. The mixtures used, were taken
ent study the solubility of CO, in glycerol/water from the mass transfer experiments. For the
216 H. Kreulen et al./J. Membrane Sci. 78 (1993) 197-216
0 Calderbank ( 1959)
0 Present work
lo-” I
1 10 100
p (10-3Pas)
experiments in the laminar film reactor fresh Both sets of data are presented in Fig. B-l. A
glycerol/water mixtures were prepared. modified Stokes-Einstein correlation deter-
The diffusion coefficients determined in the mined from the data of Calderbank also holds
present study are given in Table B-2 with the for the diffusion coefficient at higher viscosi-
viscosity of the mixture. This table also in- ties (Dq “=constant, with a=0.74).
eludes the data determined by Calderbank [ 281.