June 1955 I N D U S T R I A L A N D E N G I N E E R I N G C H E M I S T R Y 1253

program of fundamental research sponsored both by industrial

contributions and by the U. S. Army, Corps of Engineers Research
and Development Laboratories. The authors gratefully acknowl-
edge the financial and technical assistance given by the many
sponsoring organizations, and the advice and criticism offered by
members of the staff of the Soil Stabilization Laboratory.
a H =
e =
K =
K* =
L =
jy =
u =
u* =
uom =
gn ==
Ap =
e =
NOMENCLATURE
activity of hydrogen ion, gram-mole per liter
activity of sodium ion, gram-mole per liter
streaming potential, stat-volts
void ratio, cc. of void per cc. of dry solid
permeability coefficient in presence of counterelectro-
permeability coefficient in absence of counterelectro-
thickness of porous bed, om.
actual length of flow path in porous bed, cm.
superficial linear flow velocity in presence of counter-
superficial linear flow velocity in the absence of counter-
linear electro-osmosis flow velocity in pores, cm. per
pressure drop across porous bed, gram/cm.( sec.)
dielectric constant
osmosis, sq. cm.
osmosis, sq. cm.
electro-osmosis, cm. per second
electro-osmosis, cm. per second
second
X
T =zeta potential, stat-volts
=specific conductance of liquid and surface of porous
medium, stat-mhos per cm.
=viscosity of liquid, gram/(cm.)(sec.)
LITERATURE CITED
(1) Booth, F. , Proc. Rou. Soc. (London), 203A, 533 (1950).
(2) Carman, P. C., Trans. Inst. Chem. Engrs. (London), 15, 150
(3) Cornel1 University, Final Report, Soil Solidification Research,
(4) Elton, G. A. H., Proc. Roy. SOC. (London), 194A, 259, 275
(5) Fuerstenau, D. W., So. D. thesis, Massachusetts Institute of
(6) Grace, H. P., Chem. Eng. Prop. , 49, 303, 367 (1953).
(7) Henniker, J . C., Reus. Mod. Phys. , 21, 322 (1949).
(8) Kruyt, H. R., Colloid Science, Vol. I, Elsevier Publishing Go.,
New York, 1952.
(9) Michaels, A. S., and Lin, C. S., ~ N D . ENG. CHEM., 46, 1239
(1954).
(10) Muskat, M., Flow of Homogeneous Fluids through Porous
fifedia, McGraw-Hill, New York, 1937.
(11) Prutton, C. F., and Maron, S. H., Fundamental Principles of
Physical Chemistry, p. 469, Macmillan, New York, 1950.
(12) Ruth, B. E., ~N D . ENG. CHEM., 38, 564 (1946).
R E C ~I V ~D for review J une 26, 1954.
(1937).
Vol. 11, 1951.
(1948); 197A, 568 (1949).
Technology, 1953.
ACCEPTED December 23, 1054.
Estimation of Diffusion Coefficients
for Gases and Vapors
c. R. WILKE AND C. Y. LEE
Division of Chemical Engineering, University of California, Berkeley, Calif.
S THE theory and engineering applications of diffusional
A operations are advanced, increasing need arises for dif-
fusion coefficients of gases and vapors. I n view of the scarcity of
reliable experimental data, methods of predicting such informa-
tion assume a useful role. The general objective of this paper is
to review critically the existing methods for estimation of diffu-
sivities. An effort has been made to establish therelativeaccuracy
of various procedures by comparison of calculated results with a
body of selected experimental data.
REVIEW OF PREVIOUS CORRELATIONS
Gilliland (7) developed an empirical formula based on the hard
sphere model of the classical kinetic theory (25). Collision di-
ameters were assumed proportional to the cube roots of the molar
volumes at the normal boiling point as in the earlier method of
Arnold. Examination of available data led to the relation:
As used in this paper, the diffusion coefficient is the proportion-
ality constant in the rate equation for mass transfer in absence
of convection or other modes of transfer, defined as follows for
unidirectional diffusion :
where Nt =rate of diffusion of component 1 of a binary mixture,
D12 =diffusion coefficient, sq. cm. per second
A =cross-sectional area perpendicular to direction of
pl
gram-moles per second
diffusion, sq. cm.
=partial pressure of component 1, atm.
R
T =temperature, K.
x
=gas constant, cc.-atm./gram-mole-o K.
=distance in direction of diffusion
I n using Equation 1, values of V should be obtained in the same
way as were those used by Gilliland-namely, using Kopps law
of additive volumes, with the rules and values for each element
given by LeBas (18). Values of atomic volumes have been sum-
marized in several other sources ( 1 , b3,sO).
Arnold Method. Arnold ( 2 ) adopted the general equation
form proposed by Sutherland ( 25) containing an additional term
involving the Sutherland constant, Clz, to account for deviations
from the hard sphere model. Upon examination of available
data to determine the best numerical constant, Arnold recom-
mended the equation:
As outlined by Arnold, the Sutherland constant, C12, may be
calculated from the expression:
The constants, Cl and CZ, are to be obtained from the absolute
boiling temperature,
ci =1.47T~, (4)
From Equations 3 and 4 it can readily be seen that
ci2 =1.47F( TB,TB,)~ ( 5)
1254 I N D U S T R I A L A N D E N G I N E E R I N G C H E M I S T R Y Vol. 47, No. 6
Oo5 mm
004
LINES OF CONSTANT
0 03
VAL UES O F A F OR XI.O
A
002
001
0
001 002003 005 01 02 03 05 I O 20 30 50
MOL E C U L A R WE I GHT R AT I O, MI
M2
Figure 1, Values of A as mole fraction of one component
approaches zero
I n absence of experimental data V is obtained by using Kopp's
law of additive volumes, or calculated from viscosity data.
Hirschfelder, Bird, and Spotz Method. If the proper function
for potential energy of interaction between any two molecules is
known, the more rigorous kinetic theory as developed by Chap-
man and Cowling ( 6 ) may be employed to give improved expres-
sions for D and their temperature properties. Hirschfelder,
Bird, and Spotz (8-11) have carried out such calculations for
nonpolar gases which have an energy of attraction varying with
the inverse sixth power of the distance between centers of adja-
cent molecules and a repulsive energy varying with the inverse
twelfth power. For pairs of nonpolar gases the first approxi-
mation for the diffusion coefficient is expressed as follows
The numerical constant, B, is equal to 9.2916 X
theory.
felder, Bird, and Spotz as a function of k T/ .
values are listed in Table I.
according to
The collision integral, W(I)(I), has been calculated by Hirsch-
Representative
Table I. Collision Integrals for Viscosity and Diffusion
kT/ v/w(2)(2; k T/ r ) w'')(l; k T/ m)
0.3596
0.4432
0.5432
0.6301
0.7023
0.7613
0.8523
0.9172
0.9657
1.036
1.085
1.222
1.550
1.714
2.095
1.331
1.033
0.8335
0.7197
0.6479
0.6991
0.5373
0.4998
0.4745
0.4418
0.4211
0.3712
0.2878
0.2585
0.2085
For mixtures of two nonpolar gasee
and
12 =dZ ( 8 )
For collisions between a polar and a nonpolar molecule, modi-
fied forms of equations are suggested ( 14) . With these modifica-
tions Equation 6 applies to systems containing a polar and a non-
polar component. However, the energy of interaction among
polar molecules, valence-unsaturated molecules, and cigar-
shaped molecules is very different from that between nonpolar
molecules. Before Equation 6 may be considered strictly appli-
cable to systems containing such molecules, the collision integral
should be evaluated according to their respective potential func-
tions. The labor involved is formidable and as yet this has not
been accomplished.
The term A in Equation 6 is a correction factor, a small quan-
tity usually less than 0.03, which varies with gas composition.
Detailed equations for A have been given (8, 9). A is a com-
plicated function of mole fraction, molecular weights, viscosities,
the first approximation to the diffusion coefficient, and additional
functions of kT/ eI 2. However, these equations are so lengthy
that their use may not be justified for many engineering calcula-
tions, particularly when the force constants have been estimated.
As a first approximation to A for a given gas system it is suggested
that A values for mole fractions of each component equal to zero
be obtained and an average value calculated, assuming A to be
linear in mole fraction. Values of A at zero mole fraction are pre-
Rented in Figure 1. This procedure is not completely satis-
factory, as A may deviate considerably from a linear function, but
it should accomplish a major part of the correction. This pro-
cedure was adopted in subsequent applications of Equation 6.
ESTIMATION OF FORCE CONSTANTS FOR SIMILAR
MOLECULES
Both ~ / k and r , may be calculated from knowledge of gas vis-
cosity at two temperatures by solving the equation for viscosity
(9).
x 107 = (9)
where ?I =viscosity, grams per cm. second, and V/W2(2) =a
function of kT/ e which has been evaluated by Hirschfelder,
Bird, and Spotz. Representative values are given in Table I.
Equation 9 has been well substantiated by experimental evidence
and provides the most satisfactory basis for obtaining the force
constants.
I n absence of viscosity data Hirschfelder, Curtiss, and Bird ( I d )
recommend the following equations, which supersede those of the
earlier work (8).
el k =0.77TC (10)
=1.15Tb (11)
=1.92Tm (12)
Prior to publication of the above equations, in the course of the
present work examination of force constant data to check the
earlier suggestions of Hirschfelder, Bird, and Spotz (8) indicated
the following equations to be satisfactory:
/ I C =0.75Tc (13)
/ k =1.21Tb (14)
Because the collision integrals are relatively insensitive to small
errors in el k, Equations 10 and 11are considered to be equivalent
to 13 and 14 within the limits of precision of subsequent compari-
sons (Table I V). The relationships developed between T, and
Tb by Meissner (2%') indicate that the value 1.21 in Equation 14
should be preferable to the value 1.39 ( 8) , assuming that Equa-
tion 13 is valid, Unavailable critical and boiling data may be
estimated with the equations of Meissner.
The collision diameter may be calculated from a single value of
viscosity in Equation 6 using / k from Equations 13 and 14.
Alternatively Hirschfelder, Bird, and Spotz recommend:
yo =0.833V:'a (15)
where ro =A., and V, =critical volume, cc. per gram-mole
Bromley and Wilke ( 4) have tested the general form of equa-
tion proposed by Licht and Stechert ($0) and obtained a result
which in terms of y o becomes
June 1955 I N D U S T R I A L A N D E N G I N E E R I N G C H E M I S T R Y 1255
Table 11. Selected Diffusion Data for Test of Methods
System
Air-benzene
Air-ethyl alcohol
Air-ethyl ether
Air-diphenyl
Air-I2
Air-nitrobenzene
Air-n-heptadecane
Air-n-hexadecane
Air-n-octadecane
Air-n-octane
Air-mater
COz-ethyl alcohol
COa-ethyl ether
C0z-Hz
C 02- C H4
C02-Nz
COz-NZO
COz-CsHs
co2-I120
CO-CZHI
CO-Hi
CO-Nz
co-01
Freon 12-benzene
Freon 12-ethanol
Freon 12-mater
He-A
He-benzene
He-ethyl alcohol
He-Ne
He-nitrobenzene
He-Hz
He-HzO
H2-NHa
Hn-A
Hz-benzene
Ha-CClr
Hi-CzHa
Hz-ethyl alcohol
Hz-CZHI
Hg-ethyl ether
HI-HC1
H2-CHI
H2-h-i
Hz-h-20
Hz-02
Ha-CaHE
H2-SO2
HrHz0
h-2-NH1
Kz-CzHa
Nz-Hs
N2-I*
N2-NO
N2-02
NzO-CsHe
Os-NHz
Oz-CCh
02-C2H4
NHs-C1H4
A-Ne
CsHs-CzHe
CzHs-CHI
02-benzene
Exptl. Diffusion
Coefficient Sq
Cm./Sec. (at i
Temp., O K. Atm.)
298
298
293
49 1
298
298
298
298
298
298
298
273
273
273.2
273.2
288
298
298
297.7
273
273
288
273
298
298
298
273.2
298
298
293
298
293
298
293
293.2
273
296
273
340
293
293
294
273 2
293
273 2
273 2
300
273
293
293
300
288
273
293
273
298
293
296
298
293
293
293
293
293
0.0962
0.135
0.0896
0.160
0.0834
0.0868
0.423
0.0405
0.0397
0.0602
0.260
0.0693
0,0541
0,550
0.153
0.158
0.117
0.0863
0.164
0.151
0.622
0.211
0.185
0.0385
0,0475
0.105
0.641
0.384
0.494
1.23
0.372
1.64
0.908
0.849
0.770
0.317
0.345
0.439
0.578
0.483
0.354
0.795
0.626
1.205
0.535
0.697
0.450
0.483
0.850
0 241
0.187
0,743
0 070
0.232
0 181
0.086
0.253
0.0939
0.0731
0.182
0.177
0.329
0.085
0.163
Examination of data as in the case of e l k suggested an alter-
native method of estimation of ro based on molal volume at the
normal boiling point, which may be expressed as:
ro =1.18V1ia (17)
Equation 17 appears to be somewhat more satisfactory than
Equation 15 or 16. The '/3 power on Ve has been retained in
Equation 15, as it has a theoretical basis in the Lennard-J ones
and Devonshire theory of gases and liquids ( 8) , although the data
seem to correlate better us. V.O.sg. I n application of Equation
17 molal volumes may be estimated from Kopp's law and the
rules of LeBas as in the methods of Gilliland and Arnold.
COMPARISON OF EQUATIONS WITH EXPERIMENTAL
DIFFUSION DATA
To serve as a basis for comparison in determining the relative
accuracy of the foregoing methods, experimental diffusion data
were selected from reliable sources for 64 systems at atmospheric
pressure and near room temperature. (All methods of this paper
pertain to moderate pressure systems where ideal gas behavior
may be assumed-Le., where the product DP is independent of
Table 111. Force Constants and Collision Diameters for
Components of Selected Systems
TO, A. from Viscosity
Gas qp&f;"
Air
Ammonia
Argon
Benzene
COZ
co
CClr
CzHa
C2H30H
Diphenyl
Ethyl ether
CzHa
Freon 12
Helium
n-Heptadecane
H2
HC1
Iodine
CHI
Neon
Nitrobenzene
NO
N2
NzO
n-Octadecane
n-Octane
0 2
Propane
SO2
Water
97.0
315
124.0
440
190
110.3
327
230
391
600
350b
205
288 b
800
33.3
360
550
136.5
35.7
539 b
119
91.5
220
8200
320
113.2
254
252
363
356d
6. 03
3.617
2.624
3.418
5.270
3,996
3.590
5.881
4.418
4.455
6.223=
5,424'"
4.232
5,llOd
2.70
7.9235
2.968
3.305
4.982
3.882
2.80
4.931"
3.47
3.681
3.879
7.963a
7.451
3.433
5.061
4,290
2.655
2.649e
All values obtained from viscosity are taken from Hirschfelder, Bird, and
Spotz ( a) , unless otherwise noted. A mole complete table is presented by
Hirschfelder, Curtiss, and Bird (I S).
Values estimated from diffusion data.
b Values estimated from Tc .
C Values estimated from boiling temperature.
d (6). e ( 94) .
3 0
20
0
w
1.0
I
0
m
0 05
e 02
i o 1
; 03
l-
a
0
-I DEVIATION 200 %
4
0
005
003
003005 01 02 03 05 10 20 30
Figure 2. Comparison of experimental data
with results calculated by Gilliland equation
OBSERVED D, SQ CM/SEC
pressure.) These data are summarized in Table 11. I n view of
the uncertainty and lack of precision in many investigations re-
ported in the literature, use of this limited number of data from
selected sources covering a wide range of diffusion coefficients
and related properties was considered preferable to use of a larger
body of data selected at random. Also, for a large majority of the
systems force constants based on viscosity (see Table 111) were
known for the individual components.
Diffusivities calculated by Equations 1 and 2 and by Equation
6 with force constants from viscosity are presented in Figures 2, 3,
and 4. Comparison between calculated and observed results
from Table I1 are illustrated for these three methods. The
methods of Arnold and of Hirschfelder, Bird, and Spotz gave
nearly comparable results, with the latter somewhat better. The
method of Gilliland gives poor agreement for these systems. Var-
ious equations for estimating force constants were employed in
connection with Equation 6 to obtain additional comparisons of
1256 I N D U S T R I A L A N D E N G I N E E R I N G C H E M I S T R Y Vol. 47, No. 6
...v
2.0
v
cn 1.0
i
7 0.5
. 0.3
Q 0.2
5
g 0.1
W
\
0
rn
0
W
0
a
0.05
0.03
003 005 01 0.2 0.3 0.5 I O 20 3.0
OBSERVED D, SQ GM/SEC.
Figure 3. Comparison of experimental data
with results calculated by Arnold equation
2,0c
H.B.S. METHOD
DEVIATION =7.0 %
0.03 0.05 0.1 0.2 0.3 0.5 1.0 2.0 3.0
OBSERVED 0, SQ. CM. / SEC.
Figure 4. Comparison of experimental data
with results calculated by Hirschfelder,
Bird, and Spotz equation
e/ k and r o from viscosity
Table IV. Deviations Between Experimental Data and
Calculated Values for 64 Systems
Ay. % Max. ,%
Deviation Deviation
Item Method
1 Gilliland
2 Arnold
3 Hirschfelder, Bird and Spotz,
4 T O from Tc/ p?, (Eq. le), e l k
5 TO from V (Ea. 17), r / k from
e / k and r o from viscosity
from viscosity
6 ro
7 TO
8 M
9 ro
10 T O
11 ro
12 T O
13 TO
14 TO
15 TO
viscosity
from V. (Eq. 151, a/k from
viscosity
from V (Eq. 17), e / k =1.21
Tb (Eq. 14)
[odified Hirschfelder Bird,
Spotz, ,Eq., 18, e l k 'and ro
from viscosity
from Tc / pc (Eq. 16), c / k
from viscosity
from V (Eq. 17), a/k from
viscosity
from Ve (Eq. 15), r / k from
viscosity
from viscosity, c / k =0.75
Tc (Eq. 13)
from viscosity, r / k =1.39
Tb (9)
from viscosity, a/ k =1.21
from V (Eq. 17), e / k =
1.21Tb (Eq. 14)
Ta (Eq. 14)
Equation
1
2
18
18
18
18
1.8
18
18
18
20.0
8.4
7.0
10.1
10.3
11.8
12.0
3.9
9.4
7.0
1o.a
5.4
7.2
5.1
7.7
46.8
20.5
21.4
31.3
24.9
32.7
31.0
16.0
32.7
21.9
37.6
26.0
24.9
20.5
24.5
0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 09
Figure 5. Variation of constant in Hirschfelder, Bird,
and Spotz equation
calculations with observed data. Average and maximum devia-
tions between calculation and experiment are summarized in
Table I V for all methods.
It is of interest to compare the three methods with respect to
the effect of temperature on the diffusion coefficient. The equa-
tion of Gilliland is theoretically at variance with the Arnold and
the Hirschfelder, Bird, and Spotz equations. The two latter
methods consider possible molecular interaction upon collision
and therefore in principle should give more satisfactory results.
This conclusion is borne out by the relatively meager experimen-
tal evidence available. Table V shows the temperature behavior
of the carbon dioxide-air system over a range of 293 O to 1500' K.,
as observed by Kilbanova, Pomerantsev, and Frank-Kamenetskil
(16). Results calculated by each method, assuming the value at
293' K. to be correct, are also given. The Arnold and the
Hirschfelder, Bird, and Spotz methods agree closely, probably
within the limits of experimental error, while the Gilliland equa-
tion gives low values at higher temperatures.
POSSIBLE MODIFICATION OF HIRSCHFELDER,
BIRD, AND SPOTZ EQUATION
As a means of studying deviations of Equation 6 from experi-
mental results, values of the constant B were computed for each
system given in Table I11 which would make the equation agree
with experiment. Force constants were based on viscosity.
Various attempts were made to relate these values of B to prop-
erties of the systems. As shown in Figure 5, there appears to be
some correlation of the constant with the molecular weight group
[Mhky2] '". Assuming a linear relationship, the data of
Figure 5 may be approximated by the equation:
B =10.7 - 2.46 [ ML;Mfz] l I 2
Results obtained employing Equation 18 in connection with
Equation 6 for the systems are shown in Figure 5 and Table I V.
The average and maximum deviations between calculated and
experimental values are significantly lese than those obtained with
Equation 6, using the theoretical value of 9.2916 X lod4 for B.
Table V. Variation of D with Temperature for Carbon
Diffusion Coefficient, 9s. Cm./Sec.
Dioxide-Air System
Exptl. data Arnold H.B.S. Gilliland
T, K. (smoothed) method method method
293
400
600
800
1000
1300
1500
0.151
0.273
0.555
0.915
1.32
1.97
2.45
0 : 267
0.543
0.905
1.28
1.97
2.49
0 : 266
0.523
0.883
1.97
2.52
1.28
0:iiz
0.448
0.690
0.970
1.42
1.77
...
June 1955 I N D U S T R I A L A N D E N G I N E E R I N G C H E M I S T R Y 1251
3 .O
2.0
MODIFIED H.B.S. METHOD
OBSERVED D, SQ. GM. / SEC
Figure 6. Comparison of experimental data
with results calculated by modified Hirsch-
felder, Bird, and Spotz equation
3.0
2.0
Y
: 1.0
i
c; 0.5
V
v)
o- 0.3
0 0.2
W
-I
5i
Y
3 0.1
a
V
0.0 5
0.03
0.03 0.05 0.1 0.2 0.3 0.5 1.0 20 3.0
OBSERVED D, SQ. CM./SEC
Figure 7. Results of modified Hirschfelder,
Bird, and Spotz equation using estimated
force constants
Further results using estimated force constants are summarized
in Table I V, items 9 to 15. Figure 7 shows results obtained with
Equation 18 using force constants estimated from boiling point
and molar volume. This procedure seems comparable in ac-
curacy to the Arnold method for these systems.
W()(I) =collision integral for diffusion, function of kT/e
A =small correction term seldom exceeding 0.03
E =maximum energy of attraction
7 =viscosity, gram/cm.-sec.
Subscripts 1 and 2 denote components 1 and 2, respectively.
DISCUSSION
One of the reasons for using Equation 18 was to obtain a best
possible correlation of the data using force constants based on
viscosity, and then to use this relation as a basis for comparing
the various procedures for estimating the force constants.
Methods of obtaining r o are compared in Table IV, items 8 to 11.
Estimation of r o from molar volume (Equation 17) appears most
satisfactory. Use of TJP, yields slightly better results than use
of critical volume. However, experimental uncertainty in meas-
urement of critical properties may contribute to the apparent in-
accuracy. Methods of estimating ~ / k are compared in Table
IV, items 12 to 14. Equation 13 ( / I C =0.755 T, ) and Equation
14 ( e l k =1.21 Ti ) show essentially equivalent behavior. As
noted reviously, Equations 10 and 11 should be essentially
equivagnt to 13 and 14.
It is recognized that Equation 18 is highly empirical and that its
use can be justified only on the basis of the improved corre-
lation obtained for the present systems. It is believed that the
deviations of B from the theoretical value as shown in Figure 5
represent some failure in the theory, which should ultimately be
improved by a more fundamental approach. To seek modified
relations for obtaining the force constants for dissimilar molecules
from the values for the pure components would seem more
romising ultimately than the more simple expedient of modi-
rying the numerical constant in the diffusion equation.
NOMENCLATURE
B =numerical constant equal to 9.2916 X according
C =Sutherlands constant for diffusion, O K.
D =diffusion coefficient, sq. cm. per second
k =gas constant/molecule, Boltzmanns constant
M =molecular weight
P =total pressure, atm.
r =molecular diameter
r12 or ro =collision diameter, A.
7 =absolute temperature, O K.
Ta =normal boiling point, O K.
T, =critical temperature, O K.
T, =melting point, O K.
=function of AT/
V =molar volume at normal boiling point, cc. per gram-
Vc =critical volume, cc. per gram-mole
to theory
W2(2)
mole (total molar volume of each component)
REFERENCES
(1) Arnold, J . H., IND. ENQ. CHEM., 22, 1091 (1930).
(2) Boardman, L. E., and Wild, N.E., Proc. Roy. SOC. (London),
(3) Bradley, R. S., and Shellard, A. D., Ibid. , A198, 239 (1949).
(4) Bromley, L. A, , and Wilke, C. R., IND. ENQ. CHEM., 43, 1641
(5) Buddenberg, J . W., and Wilke, C. R., I bi d. , 41, 1345 (1949).
(6) Chapman, Sydney, and Cowling, T. G., Mathematical Theory
of NonuniformGases, Cambridge University Press, Ted-
A162, 511 (1937).
(1951).
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\ - - - ,
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RECEIVED for review June 1, 1954. ACCEPTED December 4, 1954.