Applications of holdup data to

explain the effect of diffusivity on

the vaporization of liquids in packings and t o estimate effective interfacial areas for mass transfer have
been outlined.
ACKNOWLEDGMENT

The authors wish to acknowledge

support of this work ( P a r t s I, 11,
and 111) under Grant G-200 of t h e
National Science Foundation and
Contract No. AT(30-1)-1463 of t h e
Atomic Energy Commission.
NOTATION

a = effective interfacial area, sq.

f t .I cu.ft.

= constant in Equation (5)

G = superficial gas rate, 1b.I (hr.)

(sq.ft.)
h, = operating holdup, cu.ft./cu.ft.
li, = static holdup, cu.ft.1cu.ft.
ht = total holdup, cu.ft./cu.ft.
k, = gas-phase mass transfer coefficient, lb. moles/ (hr.) (sq.
ft.) (atm.)
k,a = gas-phase mass transfer coefficient, lb. moles/ (hr.) (cu.
ft.) (atrn.)
L = superficial liquid rate, 1b.l
(hr.) (sq.ft.)
m = constant in Equation (5)
M M = mean molecular weight of
gas, 1b.llb. mole
n = constant in Equation (5)
P,, = mean partial pressure of
inert gas in t h e gas phase,
atm.

D = diffusivity of solute in gas,

sq. ft./hr.
D, = diameter of sphere possessing
the same surface area a s a
piece of packing, f t .

Greek Letters
p

= liquid viscosity, centipoises

= gas viscosity, 1b.l (hr.) (ft.)

= liquid density, g./ml.

= gas density, 1b.lcu.ft.
o = surface tension, dyneslcm.
o = void fraction, cu. ft./cu.ft.
p

Subscripts

w = f o r water systems
abs = for absorption work without
a chemical reaction
vap = for vaporization work
LITERATURE CITED
1. Jesser, B. W., and J. C. Elgin,
Trans. Am. I n s t . Chem. Engrs.,
39, 277 (1943).
2. Leva, M., Tower Packings and
Packed Tower Design, 2nd ed.,

The United States Stoneware

Company, Akron, Ohio (1953).
3. Mehta, J. J., and R. H. Parekh,
S.M. thesis, Mass. Inst. Technol.
(1939).
4. Surosky, A. E., and B. F. Dodge,
Znd. Eng. Chem., 42, 1112 (1950).
Parts I and II presented at the A . I . Ch. E.
Sfiringfield mcetiny, Part III at the N e w Y-orn
?nPeting.

CORRELATION OF DIFFUSION
COEFFICIENTS IN DILUTE
SOLUTIONS
C. R. WILKE and PIN CHANG
University of California, Berkeley, California

The diffusion coefficient is normally defined and assumed in this

study to be the proportionality
constant in the rate equation written for undirectional mass transfer as follows :

Equation i 1) is strictly applicable

in ideal dilute solutions in which
convective transport due t o volume
changes on mixing is negligible,
and in which other possible modes
of mass transfer are not operative. This paper represents an attempi- to generalize the relation of
P to conveniently available proper-

Page 264

ties of dilute solutions so as to permit estimation of diffusion coefficients f o r engineering purposes.

general i t was assumed t h a t this

function extrapolated into the
Stokes-Einstein equation a t very
large solute molal volumes.

PREVIOUS COlRRELATION

I n the earlier paper by Wilke

(10) a method of correlating diffusion coefficients was proposed on
the basis of qualitative conclusions
of the Eyring theory(3) and t h e
Stokes-Einstein relation. It was
shown t h a t the group TID-q, designated as the diffusion factor F,
was essentially independent of temperature f o r available systems.
Furthermore F could be represented as a smooth function of
molal volume f o r diffusion of various solutes in a given solvent. I n

A.1.Ch.E. Journal

DEVELOPMENT OF NEW
CORRELATION
Sources of Data. A t the time of the
previous work so few data were
available for diffusion of single
solutes in a variety of solvents t h a t
the effect of solvent properties,
could not be brought into a general correlation. I n a special effort
t o obtain suitable data of this kind
a companion experimental study
( 2 ) was conducted involving the
diffusion of iodine and toluene i n
a wide variety of hydrocarbon

June, 1955

u ;d
v

polvents ranging from hexane

through tetradecane. Data were
also obtained f o r diffusion of organic acids in several solvents.
These new data were supplemented
by certain other data from the
literature, including all the data
reported in the previous paper ( l o ) ,
to provide a basis f o r the present
development. All data which supplement those presented in Tables
2 through 5 of referenceil0) are
presented in Table 1.

6
I

x v

FIG.1. DIFFUSIONIN WATEP..

D 10

20
4 0 GO 80100
200
400 600 1003 2000
SOLUTE MOL A L VOLUME, CU. Cm /qm m s l

6 4
03

0
-

__

Effect of Solute Molal Volume. Figure 1 shows the diffusion as a

function of molal volume f o r various solutes in water based on data
from Table 2 of reference 10. Molal
volumes used throughout this work
a r e values a t the normal boi!i?g
point estimated for complex molecules by the atomic contributions of
LeBas (I, 6) as summarized in
Table 2.
As indicated in Figure 1, F is a
smooth function of molal volume
having a log-log slope of about 0.7
at low molal volumes and apparently merging smoothly with t h e

1-

____

3---

---

0 BENZENE

BROMOBE NZ E NE

v CARBON TETRACHLORIDE]
IODINE
OTULUENE

I
40

I 20

60 80 100
200
V, c.c / g m m o l

6oo

400

c I . 2

1
,SLOPE

= 0.6

gv

vs
5:
0 ACETIC

BENZOIC
ClNNAMlC'0 F O R M I C
A

v..

20

40

v,

6 0 80 100
c.c./gm. mol

FIG. 3. DIFFUSION O F

ORGAPI'IC

2 00

400

20

ACIDSI N TOLUENE.

40

60 80 100
V, c.c./qm. mol

200

408

FIG.4. DIFFUSIONOF ORGANICACIDSI N

CARBONTETRACHLORIDE.

Vol. 1, No. 2

A.1.Ch.E. Journal

Page 263

TABLENAL DIFFUSION DATAFOR

VARIOUS

SYSTEMS

(Supplementary to Tables 2 to 5 of reference 10)

Solute
Acetic acid

Solvent
Acetone
Benzene
Carbon tetrachloride
Toluene

i-Amy1 alcohol
Aniliie
Benzene
Benzoic acid

Ethyl alcohol
Ethyl alcohol
Bromobenzene
Chloroform
n-Hexane
Acetone

MOLECULAR W E I G H T OF SOLVENTS

FIG. 5. EFFECTOF SOLVENT

MOLECULAR
WEIGHT.

Benzene
Carbon tetrachloride

Stokes-Einstein equation which requires a slope of 113 a t high molal

volumes. On the assumption t h a t
molecules a r e spherical with a
radius equal to (3V/4nN)1I3 t h e
Stokes-Einstein equation may be
written as follows:

-- = 1.004 X 10'
DS

d3 (2)

Equation (2) is shown as a dotted

line on Figure 1. The general behavior of the curve of Figure 1
relative to the Stokes-Einstein
equation constitutes reasonable evidence in favor of the proposed
method of correlation.
Over t h e middle range of molal
volumes the curve of Figure 1may
be satisfactorily represented by a
line of slope 0.6. Bearing in mind
the theoretical limitations of t h e
assumption i t is convenient t o assume t h a t the diffusion factor is
proportional to P6over the middle range. The proportionality of
Dy to V0.6 was used by Thakar and
Othmer (8) in their representation
of the correlation f o r diffusion of
substances in water.
To explore the mold volume effect in nonaqueous systems several
solvents were studied as shown in
Figures 2 through 4. The group
DqlT may be represented satisfactorily as proportional to VO.8.
It is therefore a f a i r generalization t h a t D y l T is proportional t o
Vo.6 in the medium molal volume

Page 266

Toluene
Benzo-trichloride
Bromobenzene

Toluene
Benzene
Cyclohexane
m-Cymene
Ethyl benzene
Ethl ether
n-Hexane
Mesitylene
Transdecalin
m-Xylene
Bromform
Acetone
Benzene
Ethyl alcohol
Bromonaphthalene Ethyl alcohol
a-BromoBenzene
naphthalene
Cyclohexane
Decalin
Dibenzyl ether
n-Hexane
a-Methyl naphthalene
Tetralin
Toluene
rn-Bromotoluene Toluene
Carbon
Benzene
tetrabromide
Carbn
Benzene
tetrachloride
Carbon tetrachloride
Cyclohexane
Decalin
Dioxane
n-Heptane
n-Hextane
Isooctane
Kerosene
Tetralin
Toluene
Cinnamic acid
Acetone
Benzene
Carbon tetrachloride
Toluene
Ethyl benzoate
Acetone
Benzo trichloride
Ethyl acetate
Nitrobenzene

A.1.Ch.E. Journal

DXlW
DX106
Tempera- sq. cm./sec. sq. cm./sec.
Ref.
ture, "C.
(obs.)
(calc.)
a

40.0
25.0
15.0
25.0
5.9
6.5
14.8
25.0
40.0
25.0
15.0
6.8
20.0
18.5
7.5
15.0
15.0
13.2
25.0
40.0
15.0
25.0
40.0
14.8
25.0
40.5
16.0
25.0
40.0
7.6
7.3
7.3
7.3
7.3
7.3
7.3
7.3
7.3
7.3
20.0
20.0
20.0
20.0

4.044
3.309
2.916
2.081
1.587
1.151
1.267
1.490
1.780
2.265
1.905
1.661
0.78
2.70
1.02
3.70
3.70
2.368
2.622
3.054
1.170
1.379
1.762
0.776
0.908
1.168
1.289
1.493
1.851
1.32
1.41
0.90
1.34
1.44
3.50
2.60
1.31
0.47
1.52
2.74
1.77
0.97
0.76

3.49
2.85
2.51
1.74
1.22
1.13
1.32
1.58
2.04
2.00
1.72
1.48
0.85
2.41

7.3
. .7.3
7.3
7.3
7.3
7.5
7.5
7.5
7.4

1.04
0.85
0.34
0.149
2.15
0.226
0.36
1.24
1.52

1.05
0.72
0.39
0.17
2.44
0.22
0.38
1.31
1.48

d
d
d
d
d
d

7.3

1.12

1.27

2.00
1.41
1.49
0.776
1.02
3.17
3.70
2.57
961
0.735
2.19
2.41
1.21
0.755

1.87
1.74
1.32
0.733
1.01
3.25
3.11
2.86
1.03
.735
2.22
2.51
0.99
0.91
1.14
2.29
0.58
2.01
0.51

g
j
g
g
g
g
g

25.0
25.0
25.0
25.0
25.0
25.0
25.0
25.0
25.0
25.0
25.0
25.0
25.0
25.0
25.0
20.0

20.0
20.0
20.0

1.18

2.47
0.52
1.85
0.60

1.20

2.54
3.85
1.66
1.89
2.19
0.95
1.13
1.44
0.87
1.04
1.36
1.16
1.34
1.65
1.29
1.29
0.91
1.18
1.55
3.80
3.02

1.54

0.48
1.69
3.22
1.88
0.96
0.72

d
d
d

d
d
d
d
d
d
d

i
b

d
d

g
g
g
g
U

a
U

h
h
h
h

June, 1955

Ethylene bromide Ethylene chloride

Formic acid
Acetone
Benzene
Carbon tetrachloride
Toluene

7.3

1.11

1.31

25.0
18.5
6.5
6.2
13.9
25.0
8.5
25.0
15.0
6.2
14.1
25.0

3.768
3.274
3.132
1.991
2.306
2.577
1.612
1.888
1.673
2.285
2.463
2.646

3.59
3.12
2.87
1.48
1.76
2.14
1.48
2.01
1.67
1.90
2.32
2.54

n-Heptyl bromide

Heptane

7.4

1.52

1.48

n-Hexyl bromide

Hexane

7.6

2.31

2.54

25.0
15.0
25.0
40.0
25.0
25.0
25.0
25.0
40.0
30.0
15.0
25.0

1.50
1.54
1.07
1.772
1.316
3.42
4.05
4.24
2.71
2.30
2.43
0.96

2.30
1.19
1.31
1.72
1.32
4.60
4.96
4.37
2.74
2.28
3.04
1.14

Iodine
Carbon tetrachloride
Cyclohexane
Dioxane
Ethyl alcohol

Iodine

Heptane
Hexane
n-Hexane
Methyl cyclohexane
n-Octane
n-Tetradecane

i
a

i
a

9i
a

Iodobenzene

Benzene

7.3

1.35

1.31

Methyl iodide

Toluene
Methylene chloride

7.4
7.5

2.23
2.06

2.40
2.54

d
d

20.0
20.0
20.0

2.94
0.73
2.25

2.83
0.66
2.48

h
h
h

7.5

1.46

1.42

20.0

1.12

1.00

7.6

1.24

1.03

7.6

1.34

1.12

2.09
1.35
4.33
3.72
2.95
4.21
1.02

1.77
1.19
4.08
3.35
2.56
4.13
0.86

a
a

Nitrobenzene

Acetone
Ethyl benzoate
Ethyl acetate

n-Octyl bromide

Octane

Pyridine

Ethyl alcohol

1, 2, 4, 5-Tetrachlorobenzene

Benzene

1, 2, 4-Trichlorotoluene

Benzene

Toluene

n-Decane
n-Dodecane
n-Heptane
n-Hexane
n-Tetradecane

25.0
25.0
40.0
25.0
6.9
25.0
25.0

a
a

a
a

brand (Sept. 21, 1954).

ILDurnmer, E., 2. akorg. u. a l l g e m Chem., 109, 49 (1919).
%tokes, R. H., P. J. Dunlop, and J . R. Hall., Trans. Faraday Soc., 49, 886
(1953).

jWatts, H.,B. J. Alder, and J. H. Hildebrand, J . Phys. Chem., 23, 659 (1955).

Vol. 1, No. 2

Effect of Solvent Properties. Study

of the effect of solvent properties
in addition to viscosity centered on
the behavior of the group D-qlT
for diffusion of single solutes in a
variety of solvents. A wide variety
of variables such as molal volume,
heat of vaporization, molecular
weight, etc., were examined. Of
these the solvent molecular weight

A.1.Ch.E. Journal

General Correlation for Unassociated

Liquids. From the results of the pre-

ceding section i t was concluded

that an equation of the frllowing
form would express the effects of
solute and solvent:

TM'/

= const. ___
r]

(3)

VoP6

Figure ti shows a log-log plot of

DIT vs. the group T V O . ~ / Mfor
~/a
~
wide variety of unassociated solvents embracing the data of Table
2 of this paper and Table 5 of
reference 10. The method of plotting was selected to spread the
data and best illustrate the scope
of the correlation. The line through
the data has slope -1 as required
in the assumptions of the correlation and may be expressed by the
equation

@hang, Pin, and C . R. Wilke, "Some Measurements of Diffusion in Liquids,"

J . Phys. Chem. (in press).
bznternational Critical Tables 5, 63-75 (1929).
CMuchin, G. E., and G. P. Faermann, 2. physik. Chem., 121, 180 (1926).
dHerzog, R. O., et al., 2. physik. Chem., ( A )167, 329 and 343 (1933).
C'e Monde, H., J . phys. radium, 7, 371-8 (1936).
fOholm, L. W., Medd. Nobelinst., 2, 23 (1913).
gHammofid, B. R., and R. H. Stokes, personal communication to J. H. Hilde-

range for both aqueous and nonaqueous solvents. However, it must

be recognized that special structural features of molecules and
other molecular interactions may
be important in certain cases and
that therefore the proposed relationship is a t best an oversimplification utilized to obtain a practical
result.

appeared to correlate the data most

successfully. Figure 5 shows the
group D-qlT as a function of molecular weight for diffusion of given
solutes in a number of solvents.
Although there is considerable
scatter of the points a line of slope
112 on the log-log plots correlates
each system moderately well. As in
the case of the molal-volume effect
there are obviously other factors
involved so that use of solvent
molecular weight is satisfactory
only a s a first approximation. The
data of Trevoy and Drickamer(9)
are for 0.50 mole fraction of phenol
in various hydrocarbons so that the
solvent molecular weight is used
primarily to show the trend.

Data f o r 155 points among 123 different solute-solvent systems are

expressed by the correlation with
an average deviation of 12% between calculated and observed results.
Correlation of Associated Liquids. ASsociated liquids such as water and
other hydrogen-bonding solvents
might be expected t o show deviation from the correlation of Figure
6. Figure 7 shows the plot of DIT
vs. -qVO.6/M1/2 for diffusion in
water. The best line through the
data falls clearly above the dotted
line representing Figure ti. This
deviation is in the direction corresponding to association of the
solvent. By assigning a molecular
weightt to the solvent equal to 2.6
times the nominal molecular weight
of water one can bring the data of

Page 267

TABLE2-ATOhllC

VOLUMES FOR COMPLEX MOLECULES,

VOLUMES FOR SIMPLE SUBSTANCES

MOLECULAR

TABLE

27.0
14.8
24.6
3.7
37.0
15.6
10.5

12.0
Nitrogen, in secondary amines
Oxygen (except as noted below)
7.4
Oxygen, in methyl esters
9.1
Oxygen, in methyl ethers
9.9
Oxygen, in higher ethers and esters 11.0
Oxygen, in acids
12.0
Sulfur
25.6

For three-membered ring, as in ethylene oxide, deduct

For four-membered ring, as in cyclobutane, deduct
For five-membered ring, as in furan, thiophene, deduct
For pyridine, deduct
For benzene ring, deduct
For naphthalene ring, deduct
For anthracme ring, deduct

H,
0,

N,
Air

co
coz
so2

NO
D,O *

OF

ASSOCIA-

NUMBERSOF JACOBSEN

Atomic Volumes
Bromine
Carbon
Chlorine
Hydrogen
Iodine
Nitrogen, doub!e bonded.
Nitrogen, in primary amines

3-COMPARISON

TION PARAMETERS WITH ASSOClAlION

Molecular Volumes
14.3
N2 0
25.6
NH,
31.2
H,O
29.9
H&
3c1.7
cos
34.0
Clz
44.8
Br 2
23.6
12
20.0

0.6
8.5
11.5
15
15
30
47.5

36.4
25.8
18.9
32.9

*Estimated value.

Solvent

-4ssociation Association
parameter, x number *

Water
Methyl alcohol
Ethyl alcohol
Benzene
Ether
Heptane

60
3.5
2.7
1.0
1.02
1.0

2.6
1.9
1.5
1.o
1.o
1.0

*At 20C.

hol, illustrated in Figure 9, x is

found to be 1.5.
It is of interest to compare t h e
values of x with the association
numbers recommended by Jacobsen
( 4 ) from intermolecular freelength relationships as given in
Table 3. Although Jacobsens association numbers a r e larger than
the present association parameters
the agreement in order of t h e
solvents suggests t h a t the general
concept of t h e association effect
may be valid. The results further
suggest t h a t the methods of Jacobsen might be used to select an association parameter which normally would lie between t h e values of
2.6 for water and 1.0 f o r unassociated solvents.
By use of the given association
parameters the data or diffusion
in water a r e correlated by Equakion
(5) with a n average deviation of
about 6%. Data f o r methyl alcohol
a r e predicted within 11%.It should
be noted t h a t the experimental
data for methyl alcohol systems
a r e known to be of rather low precision in the original source.
DISCUSSION

7v0.6

M 12
FIG.6. DIFFUSIONI N

Figure 7 squarely onto t h e curve

of Figure 6.
Thus t h e correlation for diffusion
in water and also in nonassociated
solvents may be expressed by the
general equation

Page 268

UNASSOCIATED LIQUIDS.

The association parameter x is introduced to define the effective

molecular weight of t h e solvent
with respect t o t h e diffusion process. F o r nonassociated solvents
z = 1 and for water x = 2.6.
Diffusion in methyl alcohol is
shown similarly in Figure 8, indicating a n association parameter of
1.9, and f o r diffusion in ethyl alco-

A.1.Ch.E. Journal

General Comment. The correlation

represented by Equation (5) is
satisfactory for estimation of diffusion coefficients in dilute solutions with sufficient precision or
most engineering purposes, i.e.,
about 10% average error. It must
be emphasized that the diffusion
process is extremely complex and
that any rigorous treatment must
consider solute-solvent interaction
in a more detailed manner than
the present relation could possibly
imply.? Although the present functional relationship of diffusion coefficient to solute molal volume
rests upon some qualitative theo*For 285 points

among

251

solute-solvent

systems of this study.

?Diffusion of iodine in aromatic hydrocarbons,

for example, bas been excluded from t h e present
correlation because of known comples forrnat ion.

June, 1955

retical foundation, the relationship t o solvent molecular weight

is strictly empirical. Some theoretical basis f o r the latter rela-

tionship or some improved correlation would be highly desirable,

Only a tenfold range of viscosity
is covered by t h e solvents present-

ed here. Study of the correlation

and deviations from constancy of
t h e group DTIT over more extensive temperature and viscosity
ranges is especially needed. Although deviations in constany of
DTIT have been observed and
might well be expected f o r strongly
interacting solute-solvent systems
such as iodine in aromatic solvents
and acetic acid in ethylene glycol,
use of the group seems justified
for prediction of t h e effect of temperature on D in absence of experimental data.
Comparison with Other Correlations.

0.4 0.6

8 I0

20

3 V 0.6
M "2

FIG.7. DIFFUSION
IN

WATER.

a
l
0
X

all-

0.4 0.6

6 8 10

20

9 vo.6
M '4
FIG.8. DIFFUSION
IN METHYLALCOHOL.

Vol. 1, No. 2

A.1.Ch.E. Journal

Olson and Walton ( 5 ) have proposed a general form of correlation of diffusion coefficients based
on surface-tension lowering of the
solvent by hhe solute. In view of
the special data required no attempt will be made to compare
their method quantitatively with
the present correlation.
Scheibel(7) has fitted the correlation of Wilke to a general equation involving t h e molal volumes
of solute and solvent based on the
curves f o r water, methyl alcohol,
and benzene. I n view of t h e special
distinction developed above between water and methyl alcohol as
associated solvents and benzene as
an unassociated solvent t h e basic
assumptions used by Scheibel are
believed to be in error.
Thakar and Othmer (8) have proposed t h e following general equation developed through the reference substance method :

For diffusion in water only i t was

assumed t h a t the group D-ql.1 fitted
the temperature behavior better
than did the Stokes-Einstein group
DqlT. However since t h e ratio
[-ql.ll / [-q/ TI changes only 10% for
water between 0" and 80C. it is
difficult to justify a choice between
the two ways of representing the
temperature dependence on t h e
basis of the relatively limited data
presently available.
Contrary to conclusions of t h e
present study, for diffusion of a
single solute in various solvents at
20C. Equation ( 6 ) does not permit variation of Dq,O with solvent
molecular weight. Application of
Equation (6) to thirty-six representative systems involving diffusion of various solutes among
twenty-one unassociated solvents
gave rather unsatisfactory results,
with an average deviation of over
30 % between calculated and experimental diffusion coefficients.

Page 269

caution of course should be observed in extending the method f a r

beyond the range of variables and
types of systems included i n the
present development. To facilitate

CONCLUSION

It is believed that Equation ( 5 )

represents an improvement over
previous correlations of diffusion
coefficients in dilute solutions. Due

use of t h e method a revised diffusion-faotor chart is given in Figure 10 t o include the association
parameter and molecular weight of
the solvent.
ACKNOWLEDGMENT

Assistance of Research Corporation through a grant-in-aid is

gratefully acknowledged.
N W A T I ON

Q)

0
X

4-

0.4 0.6

6 8 10

20

1VO.6

M /2

FIG.9. DIFFUSIONIN ETHYLALCOHOL.

C = concentration, g. moles/cc.
D = diffusion coefficient, sq.cm./
see.
F = diffusion factor, TJDq,
(OK.) (see.)
(sqxm.) (centipoise)
L, = latent heat of vaporization of
solvent
L, = latent heat of vaporization of
water
M = molecular weight of solvent
N = Avogadros number, molecules per mole
N A = diffusion rate of component
A , g. moles/ (see.) (sqxm.)
V = molal volume of solute a t normal boiling point, cc.lg. mole
t =temperature, C .
T = temperature, OK.
x = association parameter, multiple of nominal molecular
weight of solvent to give effective value
Z = distance in direction of diffusion
q = viscosity of solution, centipoise
qw = viscosity of water, centipoise
q S o = viscosity of solvent at 20C.,
centipoise

LITERATURE
CITED

4
u
d
0)
v)

I u
Y
0

s:

SOLUTE M O L A L VOLUME, CU. cm./gm. mol.

FIG.10. GENERALIZED
DIFFUSION-FACTOR CHART.
Page 270

A.1.Ch.E. Journal

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Presented at A . I. Ch. E . brew York meetinp.

June, 1955