I8

INDUSTRIAL A N D ENGINEERING CHEMISTR

An easily applied method for predicting binary gas-phase diffusivities is

based on the use of special diffusion volumes coupled with extensive
experiment and nonlinear least squares analysis of the data. Comparison

with eight other correlations demonstrates the relative reliability and simplicity of the new method.
EDWARD N. FULLER PAUL D. SCHETTLER J. CALVIN GlDDlNGS

A NEW METHOD FOR PREDICTION

OF BINARY GAS - PHASE DIFFUSION
COEFFICIENTS
T

he importance of gaseous diffusion in a wide variety

of chemical processes is well known. With growing
demands for the quantitative description of these
processes and with recent advances in m a s transport
theory, there has been an increasing need for accurate
gas-phase diffusion coefficients for reference purposes.
As a result of the scarcity of reliable experimental data,
methods for estimating diffusion coefficients must frequently be employed to meet the need. A number of
such methods have been reviewed elsewhere (77, 75,
44).
The present investigation develops a simple, reliable,
and widely applicable correlation equation for the estimation of gas-phase diffusion coefficients. This approach starts with the Stefan-Maxwell hard sphere model
and the principle of additive atomic volumes first employed in estimating diffusion coefficients by Arnold (5)
and Gilliland (78). Selected constants are allowed to

vary freely, with optimum values obtained from a nonlinear least squares analysis involving, in this case, 340
experimental diffusion coefficients obtained from the
literature.
A detailed comparison of the final equation has been
made with the methods of Arnold (5), Gilliland (78),
Himhfelder-Bird-Spotz (20-ZZ), b t h original and as
modified by Wilke and Lee (64), Andrussow (4,Slattery
Bird ( 5 4 ,C h e n - O t h e r ( I I ) , and Othmer-Chen (47) on
all 340 data points. The present correlation has proved
to be quite accurate, more so than all others for the 340
reference points. Despite the large sample, t h i s is not a
totally objective test since the parameters were obtained
from these particular data. This method shows the
added advantage of being simpler to apply than the
more rigorous techniques.
The large collection of diffusiondata asembled in this
report should prove useful to the many workers interested
in gas-phase diffusion.

AUTHORS J. Caluin Gzddings is Aofessw of Chishy at the

Theory

Uniucrsiry of Utah. Edward N . Fullcr and Paul D . Schcttlcr

are graduak and posldoctwol fcllows, respectiwly, at Utah.

The origin of most empirical diffusioncorrelations can

be traced back to the hard sphere model, given below in
VOL 5 8

NO. 5 M A Y 1 9 6 6

19

the Chapman-Enskog form ( 9 )

3
DAB

8kT
(ImA

= binary diffusion coefficient, sq. cm./sec.

12

uAB

total concentration of both species, molecules/cc.

temperature, O K.
the Boltzmann constant, ergs/ K.
molecular mass, grams
/z(u, uB),collision diameter, separation
between molecular centers of unlike pairs
upon collision, cni.

INDUSTRIAL A N D E N G I N E E R I N G CHEMISTRY

an arbitrary constant

fi

= pressure, atm.
M,,itlB = mol. wt., gram/mole

The parameters listed below are to be optimized by

least squares analysis :

This equation is sometimes used to predict gaseous

diffusion coefficients, but its use suffers from two serious
limitations. The first limitation is the
power temperature dependence; observed values usually lie in the
range 1.6 to 1.8 (29, 53). This difference between the
simple theory and experimental observations arises from
the fact that u slowly decreases with increasing temperature (molecular softness). The second limitation, although not a source of error, is that very few of the required u are available in the literature, and even these
are applicable only over narrow temperature ranges because of the temperature dependence of u.
In 1930 Arnold (5) made two contributions aimed at
overcoming the two main limitations on the hard sphere
model. First he introduced a Sutherland temperature
correction in his equation to obtain an improved temperature dependence. I n addition, he correlated u
with an easily measured property of the diffusing substance; in his method, c w-as estimated as the cube root
of the sum of Le Bas atomic volume parameters. Arnolds
second contribution solved the problem stemming from
the scarcity of experimental us, making it possible to
estimate diffusion coefficients for almost any binary gas
phase system.
The correlation of u with molar boiling point volumes
estimated from the Le Bas parameters was retained by
Gilliland (78) in his correlation of 1934, but he eliminated the Sutherland temperature correction. An apparent explanation for this step was increased simplicity.
Lack of data for diffusion coefficients as a function of
temperature with which to check the Arnold correction
made the latter doubtful in value.
Other workers have pursued different lines of attack.
I n 1950 another correlation based on the Le Bas parameters was introduced by Andrussow ( 4 ) with a 1.78
power temperature dependence. Some workers have
estimated u from the cube root of the critical volume,
and in 1962 Chen and Othmer ( 7 7) used the 0.4 power of
the critical volume. Correlations based on critical
volumes, however, are only partially able to overcome
the second limitation of the hard sphere model since
experimental critical volumes have been determined for
only a limited number of substances.
T o gain even more freedom from the physical and
mathematical restrictions of the hard sphere model,
the following generalized function was fitted to the
data in this investigation :
20

fi[(zAU;l

l/mB)]

DAB

T
=
=
k
mA, mB =

+ 1/MB)1l2
+ (ZBU,)P2]a3

Clb(l/MA
DAB =

112

o(1,

b = temperature power dependence

ut = special diffusion parameters to be summed
over atoms, groups, and structural
features of the diffusing species (dimensions determined by the cys)
a2, 0 1 3 = arbitrary exponents to the zAvcand
ZBV,

Later the uss will be converted to diffusion volumes,

but in this general form these are simply general parameters for which an additive relationship has been
assumed. The procedure for estimating u by means of
additive diffusion parameters is analogous to the procedure used in the earlier Arnold method using the Le Bas
volumes. However, the present approach of using
parameters obtained directly from experimental diffusion data probably has a higher accuracy than methods
using parameters obtained by independent means.
All parameters for use in the present correlation were
obtained from a nonlinear least squares analysis of 153
different binary systems (340 actual data points). The
resulting fit to these data gave an average difference
between oberved and predicted values of only 4.3%.
The Computational Problem

The least squares analysis involved minimizing the

expression :
N

(3)

suni of the squares of the relative differences

between observed and estimated values
N = number of data points
Y , = ith observed value of the dependent variable;
in this case the observed DAB
E, = ith estimated value corresponding to Y,; i n
this case DABestimated from Equation 2
=

The relative least squares approach was used because

the experimental values range over three orders of
magnitude while the fractional experimental error probably remains almost constant. In such cases an absolute least squares analysis becomes dominated by the
larger diffusion coefficients and their corresponding
larger absolute deviations.
An excellent general Fortran program by Marquardt
(39) [see also references (37, 3 8 ) ]was easily adapted to
the solution of this rather formidable problem of minimizing the 4 function simultaneously with respect to all
the parameters. When we started with initial guesses
for the volume parameters obtained from scaled critical

volumes and reasonable values for the others, the IBM

7040 computer met the convergence tests of the program by means of iteration over different values of each
parameter in roughly l / 2 hour of operation.
Results and Discussion

The final equation selected from the least squares

studies is given by

The high degree of correlation between a1, CYZ, a3, and

the v;s and the nearness of the as to the hard sphere
values led us to try the latter in Equation 2. Thus,
Equation 4 was obtained from Equation 2 by arbitrarily
using the values a1 = a2 = /a and a3 = 2. Consequently, the simple form, above, was retained. The
vs now have the dimensions of atomic volumes and
will be referred to as diffusion volumes.
The 1.75 temperature power dependence represents a
compromise value giving reasonable agreement for most
binary systems. The actual value of b obtained from
the least squares analysis was b = 1.749 f 0.013 (approximate 95% confidence limits). The value of b
was then rounded to 1.75 for the sake of simplicity;
inasmuch as Equation 2 is sensitive to small changes in
b, it was necessary to run the least squares program once
more for the purpose of adjusting the remaining parameters to minimize 4 with b constrained to this value
(+ at least squares minimum = 1.4707, at the constrained minimum = 1.4762). The resulting small
increase in + was taken to be insignificant.
The initial arbitrary constant, C, was chosen as
1.00 x
This value was picked so that the atomic
diffusion volumes would roughly correspond to Le Bas
volumes. With this constant, diffusion volumes are
usually about 10 to 15% smaller than the Le Bas volume.
The resulting optimized values of the special diffusion

TABLE 11.

System Type

Hz
He
N2
0 2

Ar
Air

Hz0
Organic substances
Overall yo error
8,

Per cent of calculated

values with more than
10% error

C
H
0
(NP

16.5
1.98
5.48
5.69

H2

7.07
6.70
2.88
17.9
16.6
20.1
5.59
16.1
22.8
37.9
18.9

D2
He
Nz
0 2

Air
Ne
Ar
Kr
(Xe)

co

a
b

(C1)

19.5
17.0

(S)
Aromatic or Heterocyclic rings

-20.2
26.9
35.9
14.9
12.7
114.8
69.7

GO2

NzO
a
320

(CClzFz)
(SFd
(Cld
(Brz)

37.7
67.2
41.1

(sod

b = 7.75.
( ) indicates that listed value is based on only a f e w data points.

SUMMARY OF RESULTSa
Category II Methods

No. of
Exptl.
Points

FSG

Gilliland

Andrussow

Arnold

59
108
71
23
58
53
41
154
340

5.8
3.9
3.8
2.3
3.3
5.7
4.4
5.0
4.3

14.0
32.8
24.3
20.6
28.8
14.2
21.2
14.9
21.1

10.1
23.8
18.4
16.1
25.8
12.4
14.2
11.3
16.6

24.8
7.6
8.5
5.0
8.5
6.6
13.7
10.9
10.7

Category Z Methods

7.4

79.8

74.4

37.1

HBS

Mod. HBS,
Wilke-Lee

Chen,
Othmer

Slattery,
Bird

Othmer,
Chen

8.3
5.9
5.7
5.4
4.2
6.3
6.0
8.3
6.4
(5.4)b
( 8 . 9)d

8.7
6.3
6.8
2.6
5.7
8.0
7.2
8.1
6.8
( 5 . 6)b
(1O.l)d

6.8
14.1
7.0
1 1 .o
8.5
7.6

14.7
26.1
9.1
9.0
8.2
8.6
27.1
14.3
14.0
(6.2)

9.7
22.7
10.6
15.9
12.3
8.2
13.6
15.2
13.9

45.9

55.3

19.1

20.6

10.0

8.3
8.9

40.0

All entries are in average YOerror except as noted.

Average yo error excluding starred systems.
Average 70error excluding H Z and He systems.
The error from Hz and He estimates should not be charged to the Slattery-Bird method since the method does not apply to these systems.
Average yo error f o r
.starred system in Table III.
a

VOL. 5 8

NO. 5

MAY

1966

21

would be valuable in extending the range and accuracy

of the present method.
Certain structural features make contributions to the
diffusion volume. A value has been determined for
the aromatic ring (which has been grouped with heterocyclic rings) to be subtracted from the usual diffusion
volume to account for the bond shortening observed for
this type of molecular structure. With further refinements, branched chain, double bond, and triple
bond effects should also be taken into account; this
is not now worthwhile with the limited accuracy and
number of data points available. These effects are
apparently smaller than those of an aromatic ring, and
for the double and triple bonds are already partially
accounted for by adding in the smaller number of -H
volume increments.
Equation 4 together with the atomic diffusion volumes
listed in Table I provides a simple method for estimating
binary gaseous diffusion coefficients. No additional
data are required for its use and on the basis of the comparison which follows it is seen to be reliable for a wide
variety of systems. As additional experimental data
become available, other atomic diffusion volumes can be
determined and possibly minor adjustments made in the
ones already listed to improve the method.
Comparison of Methods

For the purpose of this report methods for estimating

DABwill be grouped into two broad categories. The
first category includes the present correlation and those
procedures like the Gilliland method which consist of
a n equation and a limited set of atomic and structural
parameters. These methods require no supplementary
data and are thus applicable to a wide range of substances. The second category includes methods such
as the Hirschfelder-Bird-Spotz equation which relate
diffusion to various molecular properties and thus require extensive data, such as knowledge of intermolecular forces or of critical properties covering every different substance for which the calculations are to be
made. The requirement for considerable supplemental
data seriously restricts the range of applicability of
category two methods since the required data are, in
most cases, available for only a limited number of common substances. Category one methods are usually
easier to apply and are applicable to a wider range of
compounds than category two methods, but lack of
rigor reduces the accuracy as will be seen shortly.
Before comparing the various methods, some comments about the experimental data are desirable. First
it should be pointed out that accurate experimental diffusion measurements are difficult to make and that most
observations are subject to a fair amount of experimental
uncertainty; this difficulty is greatest for high molecular
weight compounds. The typical amount of error is
probably of the order of 5%, as can be seen from the fact
that observations reported in the literature for identical
systems often differ by this amount or more. A second
limitation on the experimental side is that diffusion data,
in particular for organic vapors, are quite limited in
22

INDUSTRIAL A N D ENGINEERING CHEMISTRY

scope both as to types of systems and the range of temperatures. As a result, even considering all available
data, no completely adequate test of correlation methods
appears possible.
The list of experimental data in Table 111, although
extensive, is by no means complete. Several additional
sources might have been included but were either not
available or unknown to the authors during the period
in which the bulk of this study was carried out [see for
example references (8,33,36, 42,45,46, 55,58, 6 3 ) ] . No
doubt other sources have been overlooked. For the
purposes of this investigation, only recent determinations
(no data before 1930 being included) were considered;
since, as pointed out by Scott (52), much of the early
work requires critical evaluation.
Eight methods, in addition to the present one, are
compared by calculating values of the diffusion coefficient for all the experimental points used in fixing
parameters for the present correlation. The results of
these calculations are listed in Table 11. T o conserve
space, only per cent error has been given where

% error

Dcalcd.

Dohsd.

Dohsd.

100

(5)

If desired, any calculated DABvalue can be obtained

by use of the above equation.
For those methods based mainly on Le Bas molar
boiling point volumes-the
Arnold, Gilliland, and
Andrussow methods-the values of parameters listed in
Arnolds paper (5) were used in the calculations. For
the noble gases, experimental boiling point volumes,
V,, were used except for helium and neon which have
abnormally large V, values. Much better results were
obtained with these correlations using values (VbHe =
7.21; VbNe = 12.9) estimated from viscosity data according to an equation given by Arnold (5). Sutherland
constants for use in the Arnold method were taken from
reference (70) ; all others not listed there were estimated
by a relation used by Arnold:
C = 1.47 Tb
7; = boiling point temperature,

O K .

(6)

For methods employing collision integrals, the Hirschfelder-Bird-Spotz method (hereafter referred to as the
HBS method), and the Wilke-Lee modification of the HBS
method, the required force constants were taken from
the literature (22) and (23.) Svehla (59) has published
a more extended list with some values slightly different
from those in the literature (22) and (23). These parameters have been determined for most light gases and a
limited number of organic vapors.
All starred points in Table 111 indicate that these parameters were not available for one or both of the components and were estimated from critical properties.
I n calculations using these methods no corrections for
polarity were made nor were higher approximations
taken. Undoubtedly somewhat better agreement between estimated and observed results could have been

achieved using these refinements ; however, this would

have involved a substantial increase in labor.
All critical data for the correlations requiring them
were taken from reference (32) (except for V , of D Zwhich
was taken from reference (24) since the value quoted
in (32) is in error). I n some cases, critical data for
some of the organic vapors were not available-the required data were estimated using the methods due to
Lydersen (35) as quoted by Reid and Sherwood (43).

Data for the viscosity of air as a function of temperature, required for the Othmer-Chen reference substance method, were taken from a National Bureau of
Standards circular (40).
The results of the comparison are displayed in Table
I11 and have been summarized in Table 11. The Gilliland method is found to be the most erratic, showing an
overall 21.1% average error, with the closely related
Andrussow correlation performing slightly better. The

TABLE I l l PERCENTAGE ERROR INTRODUCED BY VARIOUS EQUATIONS

USED TO PREDICT EXPERIMENTAL DIFFUSION COEFFICIENTS.
SYSTEM
HZ-ME
H2-02
142-02
HZ-NZ
H2-N2
H2-N2
HZ-NZ
H2-NZ
H2-N2
H2-N2
H2-N2
H2-N2
H2-N2
H2-NZ
HZ-N2
H2-N2
H2-N2
H2-N2
H2-AR

REF.
17
19
27
47
48
47
47
6
52
17
48
47
52
52
49
52
52
52
57
57
57
27

HZ-AR
H2-AR
H2-CO
6
H2 -C 02
112-c 0 2
7
17
M2-CO2
H2-Y A T ER
50
HZ-YATER
50
H2-WATER
50
H2-NHj
52
HZ-NH 5
52
H2-NH3
27
H2-NH3
52
H2-NH3
52
HZ-NH~
52
H2-SfL
57
H2-SF6
57
HZ-SF6
57
M2-SF6
57
M2-HETHANE
7
HZ-E T HANE
7
H2-N-BUTANE
51
H2-N-BUTANE
57
H2-N-8UT AN
57
HZ-N-HEXANE
14
14
HZ-2.3-01HETHVL8UTANt*
H2-CYCLOHEXANE
14
H2-MET HVLCY CLOPENT AN*
14
H2-N-HEPT AN*
12
~ Z - 2 ~ 4 - O I M E l H V L P E N T A N E ~ 12
H2-N-OCTANE
12
M 2 ~ 2 ~ 2 ~ 4 ~ T R l M E T H Y L P E N T .1. 2
H2-N-OECANE*
14
H2-2.3v3-lRIMEIHYLHEPT.~
14
H2 -N-OOOECANE
14
H2-BENZENE
26
HZ-PYRIDINE*
26
26
H2-PIPERIOINE+
HZ-THIOPHENE*
26
~ 2 - rEl RAHVOROl H I OPHENE.
24
02-ME
27
02-N2
27
D2-AIR
21
02-AR
27
02-to
27
02-to2
27
02-NM3
2r
02-SF6
27
02-N-HEPT AN+
12
02-2~4-01NETHVLPENTANE~ 1 2
02-N-OCl ANE
12
02-212~4-1RIMETMYLPENT..
12
HE-NZ
59
H E I T R )-N2
60
HE-N2I T R )
60
HE-N2 I T R I
I?
HE (TRI-N2
17
HE-N2
60

TEMP.a
296.2
288.2
295.5
193.0
200.0
253.0
273.0
287.5
294.0
297.2
300.0
303.5
322.0
398.0
400.0
450.0
506.0
573.0
287.9
354.2
418.0
295.6
?89.2
298.0
298.2
307.3
328.6
352.?
273.0
293.0
296.8

333.0
413.0
533.0
286.2
506.9
370.8
418.0
298.0
298.0
287.9
354.2
430.0
288.7
288.8
288.5
288.5
303.2
303.3
303.2
303.2
364.1
363.9
399.6
311.3
317.9
314.7
302.2

318.4
295.1
296.0
296.8
296.8
295.7
295.7
296.8
295.7
303.2
303.2
303.2
303.2
293.0
298.0
2Y8.0
298.2
298.2

300.0

0BS.b
1.1320
1.2400
1.2500
0.3680
0.4010
0.6000
0.7080
0.7430
0.7630
0.7190
0.8000
0.8520
0.9030
1.2890
1.2700
1.5410
1.8830
2.4170
0.8280
1.1110
1.7140
0.7430
0.6190
0.6460

0.6650
1.0200
1,1210
1.2000
0.7454
0.8337
0.8560
1.0210
1.4350
2.1490
0.3960
0.4580
0.6070
0.8380
0.7260
0.5370
0.3610
0.5070
0.1630
0.2900

0.3010
0.3190
0.3180
0.2830
0.2970
0.2770
0.2920

0.3060
0.2700
0.3080
0.4036
0.4370
0.4030
0.4000
0.4120
1.2500
0.5420

0.5650
0.5750
0.5490
0.41kO
0.6300
0.3050
0.2180
0.2240
0.2080
0.2120
0.7050
0.7300

0.6880
0.6870
0.7170
0.7430

FSGC
46.16
-2.99
0.54
-3.72
-5.96

-5.16
-8.19
-4.22
-3.01
-3.18
-4.16
-8.17
-3.90
-2.46
-0.12
1-15
1.64
-1.56
-11.19
-4.87
-17.61
-1.53
-2.34
-1.36
-4.08
-9.19
-7.09
-1.76
-4.50
-3.37
-3.74
-1.29
2.37
6.82
-2.07
-4.32
-5.70
-10.21
-5.33
-3.33
-0.74
1.99

-4.85

3.08
-0.63
-4.94
-4.64
6.85
1.87
2.27
-2.98
14.16
29.26
21.74
-0.82
1.94
-?a67
6.46

-3.08
8.60
3.31
-5.48
-0.48

-0.79

-2.51
-0.90
-2.69
0.37

-2.32
-1.59
-3.44
-3.58
-4.08
1.77
2-04

-2.23
-4.65

ANDRd
12.18
-3.52
-0.64
-12.06
-14.86
-19.04
-23.10
-20.81
-20.25
-20.61
-21.60
-25.09
-22.77
-25.65
-23.97
-25.23
-27.04
-31.50
-27.05
-25.81
-38.35
-15.63
-8.59
-8-38
-10.91
-19.90
-19.41
-16.28
-20.50
-20.97
-21.53
-21-81
-23-16
-24.78
-3.56

-7-41
-12.95
-19.56
-10.44
-6.99
-2.26
-5.03
-15.59
1.41
-2.25
0.14
-0.94
3.95
-0.90
-0.42
-5.53
6.32
20.40
10.81
-2.03
-3.54
-1.24

-1.69
-4.05
-18.13
-16.53
-18.46
-20.12
-16.26
-10.51
-20.46
-6.02
-3.27
-5.86
-5.05
-6.84
-36.66
-31.26
-33.43
-33.26
-36.06
-31.73

HBSe
44.36
22.98
27.55
-15.83
-17.70
-16.42
-18.90
-15.26
-14.13
-14.26
-15.10
-18.62
-14.69
-12.86
-10.76
-9.30
-8.54
-11.09
-23.77
-17.84
-28.49
-3.02
-4.93
-3.91
-6.54
-9.65
-7.38
-1.86
-12.85
-11-63
-11.94
-3.38
-5.41
-0.55
-5.68
-7.65
-8.46
-12.53
1.12
0.02
-0.11
2.85
-3.48
1-66

-2.00
0.48
-0.60
4.92
0.04
-0.05
-5.18
11.35
26.07

15-34
0.77

-0.26
-4.69
-0.06
-1.25
1-01
-10.32
-12.59
-16.06

CH-OTf OT-CHg GlLLh

74.52

50.30
55.57
19.05
16.49
18-12

14.30
19.13
20.57
20.31
19.06
14.05
19.38
19.38
22.18
22.53
21.69
16-19
4.71
12.00
-3.63
27.53
25.99

%:::

-4.02
-0.96
5.54
-1.00
0.90
0.63
4.13
9.00
13.65
32.66
2Y.94
28.33
21.93
27.25
29.24
31.04
35.20
26.14
34.72
30.54
30.60

30.05
39.91
34.41
33.85
28.31
50.57
70.86
60.90
29.21
25.55
22.59
27.46
27.38
27.25
26.46
23.83

15.58

-10.13

26-59

-6.60
-11.54
-7.29
-2.45
-5.07
-4.77
-6.57
-32.20

24.14

-32.52
-28.40
-28.21
-31.21

-32.90

5-00

30.50
30.19
27-66
27.62
26.53
-5.14
-5.67
0.09
0.35
-3.84
-6.24

37.94
-5.67
-2.21
-2.16
-4.43
-3.96
-7.69
-3.48
-2.35
-2.58
-3.76
-7.72
-3.80
-3.52
-1.25
-0.84
-1.21
-5.00
-9.75
-4.16
-17.67
2.10
-3.06
-2.40
-4.84
-4.26
-1.66
3.97
9.09

10.84
10.54
13-36
17.79
22-02
-?.28
-4.30
-6.00
-10.87
-1.14
3.18
12.18
15.97
8.51
12.12
9.44
1.51
7.75
15.89
11.87
-3.74
7.11
25.12
41.68
33.99
6.41
0.17
2.11
4.89
5.03

-1.02
1.06
-1.98
-1.83
-0.03
-5.87
10.24
-34.00
6.53
4.98
-9.18
4.27
-3.52
-4.14
1.71
1.96
-2.31
-4.78

27.34
-12.93
-9.73
-6.20
-8.38
-7.93
-11.50
-7.47
-6.39
-6.61

-7.74
-11.53
-7.77
-7.51
-5.33
-4.94
-5.30
-8.93
-13.30
-7.93
-20.91
-2.12
-6.84
-6.20
-8.55
-8.56
-6.08
-0.69
4.13
5.81
5.51
8-20
12.44
16.47
-5.80
-7.75
-9.38
-14.08
-5.70
-1.04
7.92
11.57
4.40
7.98
5.40
-2.24
3.77
11.65
7-77
-7.24
3.21
20.61
36.58
29.19
2.46
-3.54
-1.66
1.01
1.16
-4.53
2.09
-0.94
-0.56
0.99
-4.60
10.75
-32.84
8.32
6.74
-7.62
6-05
-2.52
-3.16
2.75
3.01
-1.30
-3.80

VOL. 5 8

A R N l MOD-HB Si SL-BDk
54.66
-1.25
2.49
-2.44
-4.51
-2.33
-5.01
-0.60
0.79
0.68
-0.29
-4.39
0.41
3.22
5.72
7.83
9.12
6.47
-6.89
0.97
-11.67
2.32
3.77
4.57
1.71
-19.76
-17.57
-12.48
-14.36
-12.98
-13.24
-10.42
-5.89
-0.78
11.30
9.20
8.86
4.40
0.77
5.65
4.53
8.30
2.23
4.82
2.76
3.31
2.29
7.37
3.84
0.71
-1.61
13.10
28.05
19.39
2.10
-2.78
-2.05
2.39
1.81
13-69
6-64
3-19
3.85
2-34
2.67
-11.26
9.93
-0.19
-1.46
-4.13
-3.12
7.52
7.07
13.60
13.91
9.14
6.47

NO. 5

61.52

0.33
4.17

- 3.24

-5.24
-2.79
-5.36
-0.90
0.52
0.42
-0.53
-4.61
0.26
3.35
5.86
8.14
9.60
7.11
-8.95
-0.99
-13.21
2.58
-0.42
0.78
-1.98
33.40
41.93
56.41
-23.11
-21.79
-22.02
-19.36
-15.05
-9.69
17.33
15.22
15.14

10.60
0.29
6.46
14.36
18-81
12.43
20.84
18.67
15.94
15.84
26.74
23.71
22.15
19.78
40.84
59.46
53.26
11.54
9.50
9.82
3.56
9.12
18.91
6.82
2.82
1-91
3.07
-0.61
-20.00
16.95
19.37
18. 93
17.89
19.56
IO. 77
10.33
17.06
17.37
12.46
9.73

43.40
-14.14
-10.19
-22.02
-22.17
-11.26
-11.22
-5.48
-3.48
-3.27
-3.93
1.56
-1.33
5.97
8-62
12.44
14.79
12.37
-7.78
5.64
-4.93
-1.45
10.66
12.99
9.92
2.85
7.56
16.09
-3.23

0.64
0.73
7.32
17.43
27.08
10.36
10.59
15.28
12.70
2.34
7.20
5.05
14.98
12.05

3.33
1.44

5.30
3.28
-6.38
2.57
-1.25
-3.64
14.32
29.41
25.97
8.88
5.79
4.10
10.38
10.79
3.11
-2.09
-4.33
-0.91
-5.76
5.53
-1.07
4.55
-6.13
7.62
-10.82
-9.97
3.73
3.83
10.17
10.48

MAY 1966

5-86

3.46

23

SYSTEM

REF

TEMP. a

OBS. b

HE-N2
HE-N2
HE-N2
HE-N2
HE-Y2
HE-NZ
Ht-N2

53
53
53
53
53
53
53

323.2
353.2
383.2
413.2
443.2
473.2
498.2
600.0
YOO.0
1200.0
298.2
290.2
323.2
353.2
303.2
413.2
443.2
473.2
498.2
276.2
207.9
296.2
298.0
298.0
3 1 7.2
323.2
346.2
353.2
354.2
383.2
413.2
418.0
443.2
473.2
498.2
500.0
000.0
100.0
276.2
317.2
346.2
295.6
276.2
298.2
317.2
323.2
346.2
353.2
383.2
4 1 3.2
443.2
473.2
498.2
298.2
307.2
328.5
352.5
296.6
297.1
373.0
417.0
303.2
303.2
303.2
303.2
298.2
423.2
463.2
503.2
523.2
298.2
423.2
463.2
503.2
523.2
298.2
423.2
463.2
503.2
523.2
423.2
463.2
503.2
223.2
423.2
463-2
303.2
573.2
423.2
463.2
503.2
523.2
423.2
463.2
503.2
523.2
423.2
463.2

0.7660
0.8930
1.0770
1.2000
1.2890
1.5690
1.6500
2.4000
4. 7 6 0 0
7.7400
0.7370
0.7100
0.8090
0.9870
1.1200
1.2450
1.4200
1.5950
1.6830
0.6460
0.6970
0. 7 2 9 0
0.7250
0.7540
0.7968
0.8090
0.9244
0.9780
0.9790
1.1220
1.2370
I. 3980
1.4010
1.6120
1. 7 2 8 0
1.8600
6.2200
7.3800
0.6242
0.7652
0.9019
0.7020
0.5512
0.6120
0.6607
0.6780
0.7646
0.8000
0.8840
1.0400
1.1330
1.2790
1.4140
0.9080
0.9020
1.0110
1.1210
0.0310
0.8420
1.0050
0.5740
0.2650
0.2630
0.2480
0.2530
0.3840
0.6100
0. 71 5 0
0.8150
0.8610
0.3720
1.0320
1.2180
1.3890
1.4750
0.4940
0.8210
0.9250
1.0480
1.1730
0.6760
0.7610
0.8Y60
0.9590

HE-N~

HE-N2
HE-NZ
HE I1 R l -02
HE-021TRl
HE-02
HE-02
HE-02
HE-02
HE-02
HE-02
HE-02
HE-AK
HE-AR
HE-ARITR)
HE-ARI TR I
HE-AR
HE-AR
HE-AR
HE-AR
HE-AR
Hk-AR
HE-AR
HE-AR
HE-AR
HE-AR
HE-AR
HE-AK
HE-AR
HE-AR
HE-AR
HE-AIR
HE-A I R
HE-AIR

w-co

HE-CO2
HE-CO2
nt-co2
HE-CO2
Ht-CO2
HE-C02
HE-coz
HE-CO2
HE-CO2
HE-coz
HE-CO2
t i E-Y A T E R
HE-WAIER
HE-W A T E R
HE-WAT t K
HE-NH3
HE-NH3
HE-METHANE
HE-N-HEXANE
HE-N-HEPTANE.
HE-214,OiMETHYLPENTANE~
HE-N-OCT AN
HE-ZI~I~-TR~METHYLPENT..

HE-BENZENE
HE-8tNZENt
HE-BtNZENE
Ht-BENZENE
HE-BENZENE
H E - N l l R O 8 E N L EN*

HE-MET HANOL
HE-MtTHANOL
HE-MtTHAYOL
HE-METHANOL
HE-ETHANOL
HE-ETHANOL
~~E-E~HANoL
HE-EIHANOL
HE-tTHANOL
HE-PROPANOL.
HE-PROPANOL.
HE-PROPANOL
HE-PROPANOL
HE-2-PROPANOL.
tIE-2-PROPANOL
HE-2-PROPANOL.
HE-2-PROPANOL.
HE-BUTANOL.
HE-eur ANOLD
Ht-BUT ANCIL
Ht-BUTANOL.
HE-PENT ANOL
HE-PENTANOC.
H-P EN1 ANOL
HE-PENTANOL
HE-HEXANOL.
HE-HEXANOL

24

60

60
60
17
17
53
53
53
53
53
53
53
25
57
17
61
61

25
53
25
53
57
53
53
57
53
53
53
61
61
61
25
25
25
27
25
23
25
53
25
53
53
53
53
53
53
34
50
50
50
27
17
16
16
12

12
12
12
34
53
53
53
53
34
53
53

53
53
34
53
53
53
53
53
53
53
53
53
53
53

53
53
53
53
53
53
53
53
53
53
53

0.6170

0.7n40

v. n w o
0.9880
0.5870
0.6890
0.7Y2O
O.fl410
i). 5 0 7 0
0.5780
0.6660
0.7290
0.4690
0.5310

FSG c
5.36
5.57
0.95
3.38
8.80
0.24
4.31
-0.71
1.78
3.55
-2.52

0.06
2.24
-2.11
-0.51
2.12
1.22
1.06
4.81
-2.56
-2.89
-2.42
-0.83
-4.65
0.65
2.44
1.11
-1.03
-0.64
-0.50
2.98
-7.02
7.79
0.18
2.27
-4.39
-4.2Y
-4.24
-6.81

-3.15
-4.73
-3.95
-5.82
-6.53
-3.53
-2.86
-2.85
-3.84
0.37

-2.66
1.01
0.35
-0.67
-7.69
-2.11
-1.79
-5.33

-6.05
-7.00
-5.87
-17.50
-5.68
-4.96
-6.12
-7.98
-18.39
-5.20
-5.27
-3.93
-2.65
-22.65
-1.00
-1. 16
-0.42
0.40
-13.75
-4.23
-0.45
1.58
-2.84
-2.47
1.48
-0.37
-0.34
-2.61
-1.50
1.21
-3.27

-1.68
-1.90
-1.34
-0.53
1.24
5.04
5.38
3.07
1-01
4.49

INDUSTRIAL A N D ENGINEERING CHEMISTRY

ANDRd
-32.46
-33 02
-37.99
-37.68
-35.55
-41.59
-40.00
-45.48
-49.50
-52.18
-31.34
-29.52
-29.42
-33.91
-36.18
-33.70
-35.43
-36.58
-35.07
-35.76
-36.64
-36.78
-35.85
-38.32
-35.90
-35.07
-37.00
-38.64
-38.44
-39.56
-38.61
-44.74
-39.79
-42.27
-41.82
-45.66
-54.26
-55.31
-33.32
-33.06
-35.24
-34.13
-27.47
-29.37
-28.23
-28.07
-29.29

-30.35
-26.77
-32.21
-30.88
-32.45
-33.99
-35.53
-32.14
-33.06
-36.60
-39.37
-40.01
-31.81
-35.87
-20.09
-19.49
-20.04
-21.62
-30.29
-25.81
-27.52
-28.00
-27.75
-36.62
-30.60
-32.67
-33.15
-33.26
-31.27
-30.08
-28.94
-28.98
-32.73
-2Y.01
-27.80
-30.56
-31.22
-29.12
-29.91
-29.46
-33.24
-25.52
-27.34
-28.43
-28.54
-21.71
-21.37
-22.73
-25.16
-22.01
-21.13

HBSe
-25.69
-25.35
-20.43
-26.55
-22.53
-28.49
-25.47
-28.66
-25.90
-24.03
-26.76
-24.83
-23.00
-26.09
-24.69
-22.52
-23.05
-23.02
-20.04
-33.85
-33.99
-33.61
-32.52
-35.12

-31.38
-30.13
-30.89
-32.31
-37.04
-31.78
-29.24
-36.09
-2Y.22
-30.88
-21.33
-33.92
-32.47
-32.23
-77.95
-26.69
-27.52
-29.31
-25.73
-26.11
-23-61
-23-03
-22.86
-23.60
-20.07
-22.30
-1Y.20
-19-57
-20.27
-28.50
-24.12
-23.77
-30.49
-32.58
-33-26
-18.80
-28.82
-19.42
-18.80
-19.81
-21.39
-29.24
-16.93
-16.77
-15.38
-14.15
-36.92
-18.37
-18. I 7
-17.46
-16.68
-28.28
-19.53
-16.12
-14.20
-17.84
-19.48
-16.00
-17.32
-17.20
-19. 6 0

-18.46
-16.01

-19.63
-16.40
-16.35
-15.67
-14.88
-12.83
-10.20
-9.69
-11.57
-13.73
-10.51

C H - O T f OT-CHg

3.38
3.17
-1-79
0.04
4.70
-4.10
-0.70
-7.42
-10.43
-13.27
1.11
3.79
5.93
1-16
2.45
4.72
3.31
2.63
5.97
-9.75
-9.97
-9.49
-8.01
-11.55
-6.59
-4.93
-6.22

4-30
3.20
-2.26
-0.70
3.82
-4.82
-1.36
-6.90

-8.23

-0.98
-0.h3
-1.50
0.88
-9.07
-0.19
-3.35
-1.85
-8.27
-13.04
-13.64
0 a09
2.87
0 -46
-0.28
-3.69
-4 - 9 0
-2.28
-1.72
-2.20
-3.31
0.29
-3.35
-0.25
- 1 -89
-3.52
1.09
6 -96
6.92
2.76
12.39
11.20
-2.10
-2.22
13.07
15.22
-3.97
12.6C.
-3.87
9 -68
8-93
9.83
IO - 9 7
-16.07
7.35
5 -91

-7.87
-7.93
-5.00
-14.27
-5.51
-8.27
-6.70
-12.80
-1Y.53
-20.69
-1.26
2.29
0.77
-1.29
-2.53
-2.87
0.47
1.23
1.38
0.37
4.78
1.57
5.16

4.22
2.91
-24.82
-19.93
-18.93
-21.19
-23.29
-24.05
1.55

-6.41
6.38
8.02
6.30
5.39
-10.43
5.97
5.96
7.38
8.73
-21.51
-4.66
-5.09
-3.65
-2.84
-14.35
-2.51
1.57
3.70
-0.82
0.14
4.34
2.44
2.43
3-71
1.96
4.72
0.02
5.39
5.29
5.87
6.68
11.28
14.43
1+.75
12.16
11.26
15.18

-8.05
-8.93
0.42
3.08
4.64
-0.73
-0.19
1.51
-0.27
-1.06
2.04
-0.67
-1.27
-1.05
0.53
-3.33
1.57
3.23

1-30

6-83

7.37
-4.18
4.27
7.73
9.31
4.22
6.69
10.41
7.69
7 -46
7 -04
7.59
9.95
4.74
7.37
6.59
6.46
1-08
16-11

18.64
18.30
15.37
15 0 9 4
19.25

GlLLh
5.37
4.26
-1.25
0.32
4.89
-3.85
-0.34
-5.94
-7.10
-7.99
1.57
4.26
5.83
0.40
0.95
2.67
0.87
0.06

3.20
0.61
0.01
0.23
1.84
-2.08
2.89
4.57
2.61
0.31
0.66
-0.23
2.19
-7.90
1.10
-2.10
-0.57
-7.08
-11.92
-12.52
1.14
3.95
1.52
0.75
-2.39
-3.61
-0.95
-0.39
-0.87
-2.00
1.64
-?.04
1.10
-0.56
-2.21
1.64
7.54
7.51
4.15
12.91
11.72
-1.72
-0.62
14.97
17.15
-2-33
14.61
-2.33
11.44
10.68
11.59
12.76
-14.61
8.57
7.12
8.04

ARN
18.18
19.04
14.40
17.68
24.38
15.04
20.08
15.58
21.40
25.67
8.91
11.79
14.78
10.48
12.84
16.35
15.81
16.08
20.75
9.00
8.90
9.62
11.44
7.15
13.53
15.68
14.65
12.36
12.82
13.52
18.01
6.63
18.29
15.75
1fl.52
10.83
15.66
16.39
10.09
15.37
14.h8
7.37
8.69
8.37
12.26
13.17
13.65
12.63
18.13
15.09
19.93
19.61
18.76
-13.66
-8.28
-7.61
-10.56

-9.73
-10.63
10.50
-1.18

9.67
12.11
7.36
8.41
-4.39
13.42
13.95
16.14
11.97
-17.83
3.21
2.98
4.90

H.60

6.01

-2.86
5.71
9.22
10.82
5.65
8. 30
12.08

-4.56
8.22
13.11
15.99
11.20
12.99
18.20
16.62
16.93
13.94
15.87
19.65
14.h2
14.02
14.39
15.hl
16.83
19.13
23.05
24-06
21-63
17.27
21.97

Y.31

9.08
n.65
9.22
11.61

6.32
9.08

R.28
8.16
8.78
1n.02
20.59
20.25
17.27
17.90
21.26

MOD-HBSI
21.91
22.94
18.27
21.78
2H.R3
19.26
24.56
20.19
26.91
31.86
12.21
15.18
18.38
14.07
16.63
20.38
19.93
20.31
25.24
9.87
9.83
10.59
12.44
8.11
14.64
16.83
15.90
13.62

14.09
14.90
19.57
8.05
19.97
17.49
20.3R
12.58
18.54
19.44
12.72
18.34
17.76
11.24
n. 1 4
7.94
11.90
12.83
13.41
12.42
18.04
15.11

20.06
19.85
19.07
132.88
151.27
162.15
163.33
-16.35
-17.19
14.04
19.75
3s. 59
39.87
36.53
38.34
8.87
29.75
3U. 5 0
33.15
35.32
-4.98
-2.64
-2.74
-0.82
0.28
-2.12
11.49
16.67
19.76
14.87
21.93
27.69
26.13
26.52
27.32
29. 6 2
34.00
28.43
35.49
36.10
37.69
39.21
41.30
46. 12
47.48
44.66
41. 70
47.55

SL-BD*
17.24
20.58
17.71
22-51
30.59
21.52
27.28
22.99
25.03
23.03
10.08
12.99
18.64
16-60
20.98
26.21
26. 70
21.76
33.37
7.22
8.60
10.29
12.33
8.01
16.48
19.27
20.18
18.29
18.85
21.40
27.69
15.55
29.09
27.08
30.58
22.13
21.81
20.51
s.21
15.01
16.79
4.29
15.28
17.81
24.19
25.82
28.45
27.85
36.22
34.28
41.13
41-60
41.08
11.14
1Y.10
22.13
18.62

6.16
5.15
20.03
5.82
8.69
10.75
5.72
6-15
0.87
26.83
30.69
33.97
36.32
-13.28
27.45
28.39
31.56

33. I8
5.10
28.30
35.40
39.65
34.12
30.27
37.59
36.55
37.15
30.45
33.94
39.11
33.50
28.48
30.15
32.31
3 4.94
31.63
37.29
39.22
36.73
28.09
34.51

SYSTEM

REF.

HE-HEXANOL*
HE-HEXANOLI
NZ-AR
N2-CO
NZ-CO
NZ-CO2
N2-CO2
n2-COZ
N2 I T R I -COZ
NZ-COZ I T R I
NZ-CO2 IT R I
NZ I T R I -C02
NZ-COZ
N2-co2
NZ-CO2
NZ-CO2
NZ-WATER
N2 -W AT ER
NZ-WATER
NZ-NH3
NZ-ET HVL t NE
NZ-ETHYL EN
NZ-ETHANE
NZ-N-BUTANE
N Z - I SOW T ANE
NZ-N-HEXANE
N2-2~3-OlMETHVL8UTANf.
N2 -CY C L OH EX ANE
NZ-MErHVLCVCLOPENTANE*
NZ-N-HE PT ANE 0
NZ-2 4 0 1 METHVL PENT AN*
NZ-N-OCT ANE
N2-2,2,4-TRIMETHVLPENT.*
NZ-N-UECANE.
N2-2,3~3-1RlMElHVLHEPT-*
NZ-N-OODECANE*
NZ-BENZENE
NZ-PYRIDINE*
NZ-PlPERlOINt*
NZ-1 H I OPHENEL
NZ-T ETRAHVOROT HlflPHENt*
02-WATER
02-HATER
02-W A T f R
02-N-HEXANE
02-2~3-OlMETHVL8UTAN*
02-CYCLOHEXANE
02-MET HVLCVCLOPENT AN*
02-N-OCT ANE
02-2~214-1RIMETHVLPENT~*
02-BENZENE
02-PVRIOINE*
02-PIPERIOlNE*
02-THIOPHENE*
02-TETRAHYOROTHIOPHENE.
NE-AR
NE-AR
NE-AR
NE-AR
NE-AR
NE-AR
Nt-AR
NE-AR
NE-AR
NE-KR
NE-KR
NE-KR
NE -K R
AH-KR
AR-KR
AR-KR
AR-KR
AI(-KR
AR-KR
AR-KR
AR-KR
AR-KR
AR-XE
AR-XE
AR-XE
AR-XE
AR-CO
AR-CO2
AR-COZ
AH-NH3
AR-N-HEXANE
AR-ZI~-O~HETHVL~UTANE*
AR-CYCLOHEXANE
AR-METHVLCVCLOPENTANE+
AR-N-HkPTANE*
AR-~I~-O~METHVLPENTANE+
AR-N-OCTANE
AR-2~2~4-1Rl~ETHVLPENT.*
to-CO2
CO-NH3
CO-SF6
C02-N20

53
53
59
6
27
6
59
7
60
60
17
17
60
60
60
60
50
50
50
27
31
7
7
7
7
14
14
14
14
12
12
12
12
14
14
14
26
26
26
26
26
50
50
50
14
14
14
14
14
14
26
26
26
26
26
49
49

49
56
56
56
56
49

49
56
56
56
56
49
49
56
56
56
56

49
49
49
2
2
2
2
27
25
25
27
14

14
14
14
12
12
12
12
27
27
27
1

TEMP. a
503.2
523.2
793.0
289.5
295.8
289.2
293.0
298.0
298.0
298.0
298.2
298.2

300.0
600.0
900.0
1200.0
307.6
328.6
352.2
295.1
291.2
298.0
298.0
298.0
298.0
288.6
288.7
288.6
288.6
303.2
303.1

303.1
303.3

363.6
363.8
399.4
311.3
317.9
514.9
302.1
318.5
308.1
?29.0
352.4
288.6
288.4
288.6
287.1
303.1
303.0
311.3
318.3
315.0
302.1
318.5
90.0
194.5
273.0
273.0
288.0

303.0
318.0
353.0
473.0
273.0
288.0

303.0
318.0
199.5
273.0
273.0
288.0
303.0
318.0
353.0
373.0
473.0
194.7
273.2
329.9
37R.O
295.1
276.2
31 7.2
295.1
288.6
288.9
288.7
287.1
303.2
303.2
303.2
303.2
296.1
295.1
296.8
194.0

OBS. b

0.631 0
0.6860
0.1940
0.2110
0.2120

0.1580
0.1630
0.1650
0.1670
0.1670
0.1630
0.1810
0.1730
0.6050
1.2170
1.9760
0.2560

0.3030
0.3590
0.2480
0.1630
0.1630
0.1480
0.0960
0.0905
0.0757
0.0751
0.0760
0.0760
0.0740
0.0744
0.0726
0.071 3
0.0841
0.0684

0.0813
0.1022
0.1068
0.0953
0.0992
0.0985
0.2820
0.3180
0.3520
0.0753
0.075?
0.0 I 4 4
0.0742
0.0705
0.0705
0.1011
0.1050
0.0953
0.0975
0.09 83
0.0360
0.1530
0.2710
0.2760
0.3000
0.3270
0.3570
0.4140
0.6710
0.2230
0.2400
0.2660
0.2840
0.0720
0.1260
0.1190
0.1280
0.1400
0.1530
0.1970
0.2160
0.3270
0.0508
O.OY62
0.1366
0.1 759

0.1880
0.1326
0.1652
0.2320
0.0663
0.0657
0.0719
0.073 I
0.0658
0.0655
0.0587
0.0599
0.1520
0.2400
0.0887
0.0531

FSG 0

ANDR

1.64
0.09
-0.27
-7.69
-4.60
-1.50
-2.31
-0.59
-1.78
-1.78
0.74
-9.27
-4.07
-7.74
-6.75
-4.98
8.82
3.21
-1.65
1.01
-8.46
-4.68
-0.37
3.72
10.03
-0.50
0.36
0.79
0.79
2-06
1.46
-3.25
-1.38
1.88
25.39
12.69
-1 6 2
3.89
-1.94
5.61
0.89
-0.79
-1.31
0.55
-3.15
-3.27
-0.2 7
-0.91
-3.96
-4.01
-3.46
2.84
-4.94
4.31
-2. LO
7.90
-2.20
-0.06
-1.87
-0.87
-0.60
-0.92
2.57
5.61
-4.09
-2.14
-3.50
-1.64
-1.59
-2.64
3.09
5.24
5.16
4.72
-2.37
-1.94
-1.84
4.26
-0.40
-2.44
-3.06
2.66
1.16
3.45
5.43
2-40
3.53
-3.82
-6.31
2.84
3.32
6.75
4.61
4.91
2.44
7.39
2.89

-24.85
-26.71
-28.96
-31.15
-29.22
-20.71
-21.63
-20.59
-21.54
-2 1.54
-19.53
-27.53
-23.49
-38.12
-43.49
-46.42
-18.31
-23.80
-28.63
-20.29
-21.75
-18.99
-16.98
-11.31
-5.92
-13.09
-12.35
-6.76
-7.86
-11.52
-12.04
-15.79
-14.17
-14.72
4.94
-7.44
-14.76
-13.62
-13.42
-13.99
-12.31
-20.42
-22.12
-22.01
-11.32
-11.41

-3.08
-k.75
-12.60
-12.65
-11.97
-10.00
-11.79
-10.58
-10.*6
-4.74
-28.79
-33.14
-34.35
-34.56
-35.21
-36.20
-35.65
-38.42
-34.33
-33.89
-35.63
-35.17
-22.16
-28.79
-24.61
-24.05
-25.07
-26.28
-33.04

-33.66
-37.43
1.35
-11.04
-16.87
-20.82
-24.34

-18.08
-19.07
-25.73
-10.83
-9.87
-11.25
-14.46
-11.11
-10.70
-7.35
-9.21
-13.13
-24.56
-5.67
9.68

HBS

-12.73
-13.96
-27.53
-29.73
-26.81
-19.67
-20.30

-18.86
-19.83
-19.83
-11.76
-?5.94
-21 -68
-23.09
-21.32
-19.13
-13.57
-1 7.86
-21.57
-24.89
-19.44
-16.06
-14.16
-1 0.20
-4.74
-13.90
-13.16
-7.56
-8 - 6 5
-11 - 5 6
-12.08
-16.18
-1 4. 55
-11.27
P.20
-1.64
-13.47
-1 I. 83
-12.07
-13.63
-10.76
-16.19
-16.47
-14.72
-12.28
-12.38
-4.05
-5.84
-13.10
-1 3.15
-13.79
-8.75
-10.54
-10.34
-9.01
-29.69
-34.79
-32 + 68
-33.90

-33.11
-32.83
-32.95
-30.37
-27.60
-35.69
-34.27
-35.09
-33.74
-30.69
-30 78
-26.71
-25.06
-25.00
-25.21
-30.05
-29.63
-29.06
-11.48
-14.58
-15.84
-16.73
-22.63
-18.69
-16.51
-23.33
-12.03
-11.06
-12.38
-15.68
-11.46
-11.05
-8.05
-9.89
-11.40
-20.98
-7.35
-1.51

CH-OTf OT-CH
11.97
10.18
-6.76
-4.76
-1.49

-2.38
-3.04
-1.15
-2.34
-2.34
0.18
-9.78
-4.54
-5.91
-7.31
-8.51
-12.50
-15.96
-18.34
-18.53
-3.93
0.30
1.36
2.02
9.15
-4.34
-2.83
0.93
0.48
-1.48
-1.04
-6.95
-3.73
0.56
24-17
12.50
-5.42
-5.51
-4.32
-6.35
-2.15
-17.35
-16.65
-13.96
-3.48
-2.92
3.56
2.34
-4.26
-2.89
-3.74
-3.00
-3.78
-4.15
-1.46
-11.79
-8.20
-4.55
-6.27
-5.25
-4.99
-5.33
-2.22
-0.91
-6.92
-4.94
-6.23
-4.44
-19.97
-16.14
-11.21

15.33
13.24
-3.35
-8.52
-5.53
-9.04
-9.65
-8.01
-9.11
-9.11
-6.70
-15.98
-11.03
-13.81
-14.78
-14.97
3.73
-0.97
-4.86
3.91
-8.30
-4.16
-7.80
2.56

6.30
-5.22
-3.14
-4.47
-0.84
-2.98
-2.22
-18.16
-4 - 6 9
-3.12
19.22
9.92
-7.12
-9.72
-4.96
-8.17
-4.35
-4.47
-3.93
-1.40
-8.6R

-7.92
-6.20
-3.58
-19.72
-8.18
-9 - 3 3
-11.23
-8.34
-9.99
-7.74
-0.28
-2.29
-0.18
-1.98
-1.09
-1.02
-1.55
1.29
2.55
-1.73
0.35
-1.76
0.11
-11.06
-7.78
-2.35

-8.68

0.33

-8.16
-8.04
-13.38
-12.62
-11.53
-4.23
-1.35
-0.45

0.91
0.96
-5 e07
-4.28

-0.30
-0.42
-7.82
-3.69
-22.16
-9.28
-7.56
-11.39
-14.11
-8.36
-6.88
-5.25
-5.64
7.90
-14.31
13.52
-7.55

-3.33
-4.10
-2 - 7 8
-2.51
-2.74
1.38
-8.35
-4.86
7.19
-5.67
-3.40
-1 1.87
-10.51
-5.38
-3.59
-12.75
-2 3 4
-1.84
6.50
-0.73
-11.32

GlLLh
17.28
15.15
5.01
-1.11
2.12
-1.05
-1.72
0.06

-1.13
-1.13
1.49

-8.60
-3.23
-6.24
-7.30
-7.51
11.18
6.14
I .97
11.23
-0.87
3.61
5.19

11.88
15.96
3.71
5.98
4.51
8.48
6.25
7.08
-10.31
4.45
6.28
30.79
20.67
1.56
-1.28
3.99
0.47
4.68
2.58
3.16
5.87
0.17
1.01
2.88
5.75
-11.79
0.89
-0.61
-2.68
0.53
-1.28
1.23
7.64
5.47
7.76
5.80
6.77
6.84
6-27
9.34
0.69
6.74
8.99
6.70
8.73
2.09
1.52
1.50
0.45
1.09
1.15
4.50
5.37
6.43
5.86
7.33
7.62
7.36
10.16
0.26
4.08
15.25
3.86
6.36
-2.98
-1.48
4.29
6.27
-3.75
7.73
6.77
13.99
8.92
-2.87

VOL. 5 8

A R N I MOD-HBSJ SL-BD*
19.24
17.70
1.87
-7.00
-3.76
-0.56
-1.31
0.53
-0.68
-0.68
1.88
-8.25
-2.95
-2.70
0.77
4.46
-5.99
-10.49
-14.34
-11.15
-2.83
1.31
0.50
0.81
5.97
-7.24
-4.92
0.14
-1.08
-6.26
-5.52
-13.13
-8.88

-8.43
12.70
-0.08
-6.52
-7.94
-4.57
-5.43
-2.55
-13.66
-13.78
-11.79
-10.13
-8.76
-1.20
- 3 . LO
-14.33
-11.87
-8.48
-9.lU
-7.73
-6.78
-5.58
11.76
6.09
10.64

8.63
10.10
10.73
10.70
15.31
20.83
6.27
8.78
7.59
9.98
-1.48
-0.68
5-16
7.71
7.96
7.81
1.15
1.93
3.49
7.68
4.98
4.01
3.33
4.67
3.12
6.34
-6.06

-4.33
-1.67
-4.02
-7.72
-5.45
-3.67
-4.15
-3.31
5.69
-10.11
12.96
9.55

NO. 5

44.40
42.61
-2.36
-9.17
-5.98

32.27
30.79
-7.29
-17.23
-13.78
-6;68
-2.98
-7.36
-3.31
-5.62
-1.00
-6.75
-2.19
-ha75
-2.19
-4.35
0.35
-13.86
-9.63
-8.88
-4.24
-7.81
5.14
-4.03
5.39
-0.13
3.85
9.87
14.47
8.29
10.93
7.46
7.86
-21.68
-1.73
-7.38
-6.30
-3.40
-1.60
-0.62
-3.41
4.80
-7.06
11.91
-3.21
0.66
-17.82
3.42
-15.06
6.24
-R.28
5.81
-10.23
3.80
-16.75
5.63
-16.38
-1.48
-23.82
3.83
-20.19
6.19
-17.50
30.69
1.55
18.99
-9.92
-3.07
-10.34
-1.48
-9.94
1.29
-0.91
-8.95
-0.54
-0.88
-4.91
-4.70
9.17
-0.99
10.94
5.01
15.31
-0.44
-18.21
1.29
-16.89
6.80
-7.00
5.65
-9.78
-0.51
-22.95
2.78
-20.84
-3.47
-9.73
-1.04
-8.52
-0.27
-9.47
-8.83
-7.29
-2.31
-5.29
5.55
-56.65
1.20
-23.30
6-00
-6.88
4.08
-8.56
5.56
-5.66
6.24
-3.63
10.R6
6.27
16.60
3.66
6.19
5.10
7.50
-6.87
-5.73
-0.19
2.30
2-60
2-53
-3.68
-2.87
-1.07
3.28
1.14
0.45
-0.03

0.81
-4.63
-1.48
-18.65
4.35
7.46
2.10
-0.98
5.43
8-43
9.66
11-08
-0.36
-20.37
14.19
-1.52

-2.36
4.29
13.98
-10.34
-6.57
-6.14
-2.75
-22.80
-10.63
-5.38
-1.34
0.43
1.66
-2.21
-0.37
4.35
-16.19
-4.91
-0.36
1.91
-4.07
0.93
8.55
6.90
-14.59
-12.08
-11.34
-15.70
-15.53
-14.21
-15.56
-14.92
4.34
-0.15
0.82
-1.26

MAY 1966

25

SYSTEM

REF

C02-N20
COZ-NZO
COZ-NZO
C02-N2O
COZ -NZ 0
COZ-WATEH
COZ-WATER
COZ-WATEI(
COZ-PROPANE
COZ-ETHYLENEflXIOE*
N2 0-PROP ANE
N Z O - t T H Y L ENEOX I OE
NH3-SF6
METHANE-Y ATEK
METHANE-WATER
HTHANE-M ATEK
kTHYLENt-WATCW
LlHYLENE-WATtR
ETHYLENE-WAT E R
FREON1 2 *-WATER
FREON12*-8ENL E N
FRtONl2*-tTHANUL
AIH-CL2
A IK-8H2
A I R-CO2
A IR-CO2
AIR-CO2
A I R-SO2
A IR-WAT E R
A IR-WAT ER
A I H-MAT EH
A I R-WATER
A IR-NH3
AIR-METHAVE
A I R-MtT HANE
AIR-BENZENE
A I R- 8 t NZ ENE
AIR-TOLUENE
A IR-T OLUENE
AIR-1OLUtNE
A I H - C H L O H O ~ E N ZEN.
AIH-CHLOKO8ENLEY6.
AIR-CHLOROBENZENE.
AIR-ANILINE.
AIR-ANILINE*
A I R-AN IL 1 YE.
AIR-NITRORENZENE.
A I R - 0 1 PHk NY L
A IR-ETHANOL
A I R-2-PROPANOL
AIR-2-PROPANOL.
A I R-2-PROPANOL
A I R-OUT ANOLe
A I H-8JT ANDL
A I R-BU T ANOL
A IR-2-BUT ANOL
AIR-2-RUTANOL.
AIR-2-8UTANOL*
A I H-2-PtNTANOL
AIR-2-PENTANOL.
AIR-2-PENTANOL
A I R-ET HVL ACET ATE
A 1 R - t l HYLACE I A T E
A I K - E T H Y L ACE 1 A T E
AIK-HCYc
AIR-CY ANOGtNCHLOR 1DF.
A IR-PHOSGENE
AIR-CHLOHnPICR IN.

AVC.EKROK

1
6

62

1
1
50
50
50
62
62
62
62

27
20
50
50
50
50
50
34
34
34
3
3
25
3
25
3
34
18
18

in

27
$3
13
34
2R
18
18
18
18

lfl
18
18
LR
18
34
18
34
18
18
18
18
18
I H

18

1A
18
18
18

18
I8
18
18
30
30
30
30

I P t R CENT1

STANOARO U f V l A l I f l N ( P k K CENT1

TEMP.*
273.2
287.3
298.0
312.8
362.8
307.5
328.6
352.4
298.0
L98.0
298.0
298.0
296.6
30 7.7
328.8
352.3
307.8
32H.5
352.3
238.2
298.2
298.2
293.0
293.0
276.2
293.0
3 1 7.2
293.3
298.2
299.1
312.6
333.2
295.1
LR9.0
294.6
298.2
308.0
29Y. I
312.6
333.2
299. 1
317.6
333.2
299.1
312.6
333.2
298.2
490.3
298.2
299.1
312.6
333.2
299.1
312.6
333.2
299.1
312.6
333.2
299.1
312.6
333.2
299.1
312.6
333.2
273.3
277.0
273.3
298.0

OBS.~
0.0989
0.1070
0.1170
0.1280
0.1683
0.2020
0.2110
0.2450
0.0863
0.0918
0.0860
0.0914
0. 1090
0.2920
0.3310
0. 3 5 6 0
0.2040
0.7330
0.24 70
0. I O 5 0

0.0385
0.0415
0. 1 2 4 0
0.0910
0.1420
0.1650
0.1772
0.1220
0.2600
0.2580
0.2770
0.3050
0.2470
0.2190
0.2240
0. 0 9 h 2
0.1021
0.0860
0.0920
0.1040
0.0740
0.0700
0.0900
0.0740
0.0790
0.0900

0.0655
0. 1600
0.1350
0.0990
0.1070
0.1210
0.0870
0.0920
0.1040
0.0890
0.0960
0.1080
0.0710
0. 0 7 6 0
0.0860
0.0870
0.0940
0. l U b 0
0.1730
0.1110
0.0950
0. OHHO

FSGc
-0.15
0.79
-1.74
-2.23
-3.61
10.08
18.36
15.21
6.96
15.09
-1.35
4.91
15.15
-3.00
-3.90
0.83

0.23

-1.65
4.85

-2.20
-2.51
-5.82
-7.42
-12.05
-7.13
-1.79
-6.06
-1.28
17.53
-2.58
15.84
-2.05
-16.99
-19.11
-16.59
-10.05
-13.17
-9.03
13.26
7.91
22.57
-16.11
1.20
-17.17
-22.12
-1M.31

-0.53
-I.76
6-62
0.08
0.03
-3.48
-7.89
-1.45
0.03
-10.88
-3.25
-22.36
-1.98
-21.40
-1.37
-21.78
0.16
-21.83
-3.18
-27.24
-8.8h
-21.6.5
-7.85
-21.16
-6.96
-15.01
-7.23
-15.95
-5.95
-15.09
-5.02
-15.20
-6.06
-17.45
8.13
-0.81
9.42
-0.73
7.39
-4.11
14.94
1.37
16.32
1.41
14.17
-2.05
-6.68
-17.91
-1.10
-23.62
-8.58
-20.50
4.55
-7.96
4.51
-9.01
3 . 3 3 -11.46
3.89
-7.77
-6.01
6.13
4.98
-9.28
1.56
-9.84
1.71
-10.69
1.09
-12.64
14.77
2.07
1-88
15.33
13.96
-0.92
0.R5
-11.54
0.H4
-12.53
-0.01
-14.64
- Y e 9 6 -21.22
-12.36
-2.75
-7.94
-15.06
-6.32
-11.59

HBSe
-3.45

-2.40
-4.74
-5.08
-6.00
-3.49
3-98
1.42
-0.15
18-87
-1.46
17.17
-3.58
-10.32
-10.98
-5.41
-4.H1
-6.42
-9.07
12.33
5-64
20-73
-16.04

CH-OT' OT-CHg
-1.54
0.53
-1.22
-0.73
0.53
-16.34
-8.36
-9.16
-0.62
11-07
-5.06
5.09
-8.98
-21.62
-21.01
-19.15
-19.05
-19.12
-12.17
-1.15
-14.17
-2.39
-1.04
9.84

-7.21
-5.40
-7.33
-7.06
-7.42

GlLLh A R N '
1.64

3.67
1.51

1.80

1.40
1.67
11.11
9.33
0.60
4.36
0.55
4.13
9.86
-3.41
-3.06
-8.62
-9.27
7.62
-7.21
-0.55
-7.56
-0.32
-0.02
fa16
4.13
12.97
-14.13
-4.39
1.23
11.95
-6.50
7.23
-1.23
4.50
14.78
-17.21
3.88
-7.32
0.88
-20.85
-3.06
-10.93
-3.06
-15.12
4.56
-4.30
4.17
-13.52
-0.11
-0.35
8.86
-18.66
-17.46
-3.61
3.36
-17.59
-lh-33
-7.17
4.90
-16.97
-15.07
-1.03
h.13
-15.52
-12.73
1.30
8.63
-23.89
-16.79
4.62
lZ.04
-18.41
0.32
-h.19
0.31
-17.46
1-61
-4.93
1.66
-14.80
-6.59
-10.11
-1.h5
-14.96
-6-32
-Y.76
-1.27
-15.25
-7.21
-11.43
-2.98
-14.30
-5.53
-9.R5
-1.26
-15.07
-5.54
-10.15
-1.58
-1.61
6.74
7.00
11.85
-0.31
Ha94
3.97
13.96
-1.96
8.15
3.01
12.96
17.08
1-10
6.06
6.88
2.44
8.31
9.03
19.44
3.74
7.63
8.19
18.51
-18.87 -14.96
-18.H4
-10.95
-13.82
-7.70
-h.2R
2.92
-18.93 -13.95
-13.16
-5.43
-6.86
1.78
-0.H9
H.22
-6.78
2.52
-0.26
8.91
-7.65
2.44
-0.47
8.hR
-7.30
-3.40
-2.22
6.94
-5.17
2.61
0.45
9.67
0.64
-6.02
2.65
0.24
-9.38
-1-62
-3.86
5.15
-9.12
-0.67
-3.08
6.01
-9.50
-0.19
-2.72
6.40
2.02
11.18
9.17
lV.4Y
3.10
13.12
11.04
21.59
2.07
13-01
10.70
21.22
-11.58
-1.95
-2.Y5
6.28
-11.48
-1.70
-2.17
7.13
7.40
-12.06
-1.02
-1.92
-)0.35-15.77
-31.65
-76.11
-H.56
-13.hL
-5.05
-16.27
-17.54
-6.88
-1?.hR
-4.31
-19.26-10-74
-15.86
-7.57
-5.66

3.10
1.45
-8.16
-4.72
-8.20
-4.93
1.35
-8.95

8.49
9.84
7.32
7.10
6.53
-4.34
3.27
0.94

MOD-HBSJ SL-Bbk
-2.04
-0.76
-2.9R
-3.13
-3.46
-13.69
-3.53
-2.19
0.74
0.45
-0.36
-0.56
-1.96
-10.76

3.52
11-10
2.76
10.31
5.88
-15.25
-15.70
-H.IO
-11.19
0.39
-6.68
-13.78
-10.05
-r2.12
-3-70
-2.41
2.07
-4.53
-5.13
-4.53
5.00
10.56
1.80
-3.07
13.54
12.H9
-4.97
1.72
-2.59
-8.92
4.72
-1.99
5.72
-0.87
-17.10
-0.64
-10.93
0.84
-10.14
4.11
9.74
-0.40
-10-44
-21.42
-6.15
-2.67
-1.48
-4.98
-8.70
-5.49
-5.54
-8.80
-9.95
-3.79
-7.S2
-8.82
-9.47
-3.13
8.51
3.42
4.93
10.16
3.38
8.63
10.34
11.22
11.95
12.91
11.34
10.30
-13.84
-11.42
0.48
-11.75
-16.46
-11.64
2.14
3.H7
2-37
4.16
1.61
3.47
-1.02
6.28
1.39
8.93
0.68
0.25
-2.h7
6.07
6.58
-2.26
6-42
-2.4M
8.82
1H.22
13-70
10.11
18.83
9.22
-1.30
-3.60
-1.08
-3.36
-3.H1
-1.45
-26.84
-37.15
-1l.hB
-13.69
-8.65
-7.88
-15.19
-9.00

13.78
17.15
15.77
17.15
20.69
28.92
41.66
40.72
6.49
22.70
5.17
21.88
18.38
11.52
12.90
20.86
20.47
20.74
31.37
25.57
-11.06
11.01
0.39
13.33
-1.51
3.84
5.76
4.Rb
7.00
8.51
10.81
14.90
-0.09
-5.26

-3.5?
-12.95
-12.21
-15.53
-13.69
-12.88
-2.55
0. I 3
0.30
1.37
10.33
10.51
-21.88
-17.94
-10.94
-1.17
0.31
1.27
-h.12
-2.62
-1.70
-8.23
-6.67
-5.34

0.12
2.61
3.47
-10.22
-8.85
- 7 . 76
-26.71
-16.29
-15.58
-21.65

4.32

21.11

16-57

10.67

6-38

6.76

5-86

14.02

13.89

6.71

24-34

19.24

15-61

0.77

8.91

10.95

23.73

11.67

Temperature (OK)
OBS = Experimentally observed diffusion coefficient reduced to 1 atm.
pressure
(cm.z/sec.)
FSG = Value obtained in this work
d ANDR = Value obtained from Andrussow ( 4 )
e HBS = Value obtained from Hirschfelder-Bird-Spotz (20.22)
t CH-OT = Value obtained from Chen-Othmer (77)
a

26

ANDRd

INDUSTRIAL A N D ENGINEERING CHEMISTRY

OT-CH = Value obtained from Othmer-Chen (47)

GILL = Value obtained from Gilliland (78)
1 ARN = Value obtained from Arnold (5)
'I MOD-HBS = Values obtained from the Wilke-Lee modification of HBS (64)
k SL-BD = Value obtained from Slattery-Bird f54J
* Indicates that, in the HBS and MOD-HBS calculations, force constants for the
starred components were estimated from critical properties.
g

Arnold method is seen to perform substantially better

than the other methods based mainly on the Le Bas
parameters. The well known HBS method is seen to be
quite reliable with an average error of only 6.4%,. Wilke
and Lees modification of the HBS method is seen to
improve results in some cases, but the average overall
error is increased by its use.
The Slattery-Bird method is seen to give good agreement on NPsystems, but in the case of He systems and to
a somewhat lesser extent for HBsystems, its use can lead
to rather large errors. This is expected since the authors
state that their correlation is not applicable to He and
Hz systems. Thus the error for systems with these gases
should not be charged against this method.
The Chen-Othmer correlation gives good results close
to room temperature, but for some systems the 1.81
temperature dependence of this method appears too
high. The Othmer-Chen reference substance method
shows poorer agreement than expected, with an average
error of 13.9%. The present diffusion volume correlation with an average error of 4.3% shows the best
agreement between calculated and observed values
in each of the categories of Table 11. Furthermore, if
the maximum permissible per cent error is taken arbitrarily to be lo%, the correlation developed here has
far fewer points in error greater than this amount than
any of the other methods.
Conclusion

From the above comparison it is seen that the diffusion volume correlation gives the best fit to the data
used in this report. If force constants from viscosity
data are available for use with the HBS method, comparable results are obtained. Average error using
estimated force constants, starred points in Table 111,
was 8.9y0; excluding starred points 5.4%. I t is apparent
that the HBS method rests on firm theoretical grounds
while the present method can be no more reliable than
the diffusion data used in its development. Any systematic errors in the data would be reflected in the atomic
diffusion volumes and would lead to error through their
use.
The present method has the advantage of being able
to overcome the general lack of accuracy associated with
other category one methods, and it is still simple to use.
The additional advantage of wide applicability is a
major one, I t should be noted that supplementary
data needed for category two methods, although limited
to common substances, can be estimated using procedures described in the literature, but this adds considerably to the labor of calculation and adds an additional
element of uncertainty. The diffusion volume correlation should prove useful in such cases.
Use of the diffusion volume correlation or alternatively the HBS method according to the preceding
recommendations should be a valuable aid in the estimation of binary gas-phase diffusion coefficients in the
absence of experimental data. Some caution is still
necessary when estimating DABfor systems not included
in this study since in extreme cases the error of estima-

tion from either method may apparently exceed the

average by a wide margin. I n general, satisfactory
results will be obtained since the average error of both
methods is probably close to the average experimental
error.
B I BL IOG RAPHY
(1) Amdur, I., Irvine, J. W., Jr., Mason, E. A., Ross, J., J . Chcm. Phys. 20, 436
(1952).
( 2 ) Amdur, I., Schatzki, T. F., Ibid., 27, 1049 (1957).
(3) Andrew, S . P. S.,Chem. Eng. S&.4, 269 (1955).
(4) Andrussow, L., Z. Elektrochem. 54, 566 (1950).
(5) Arnold, J. H., IND.END.CHEM.22, 1091 (1930).
(6) Boardman, L. E., Wild, N. E., Proc. Roy. Soc. (London) A 162, 511 (1937).
(7) Boyd C. A., Stein, N., Steingrimsson, V., Rumpel, W. F., J . Chem. Phys. 19,
548 (1451).
(8) Bunde, R. E. University of Wisconsin Naval Research Laboratory Report
C M 850 (19551.
(9) Chapman, S., Cowling T G The Mathematical Theory of Nonuniform
Gases, 2nd ed., p. 245, 6ambriJge Univ. Press, London, 1952.
(10) Ibid., p. 225.
(11) Chen, N. H., Othmer, D. F., J. Chem. Eng.Data 7 , 3 7 (1962).
(12) Clarke, J. K., Ubbelohde, A. R., J. Chem. SOC.(London) 1957, p. 2050.
(13) Coward, H. F., Georgeson, E. H. M., Ibid., 1937, p. 1085.
(14) Cummings, G.A. McD., Ubbelohde, A. R.,Ibid., 1953, p.3751.
(15) Fuller, E. N., Giddings, J. C., J. Gas Chrom. 3 (7), 222 (1965).
(16) Fuller, E. N., Giddings, J. C., unpublished results.
(17) Giddings, J. C., Seager, S . L., IND.END.CHEM.FUNDAMENTALS
1,277 (1962).
(18) Gilliland, E. R., IND.ENO.CHEM.26,681 (1934).
(19) Heath, H. R., Ibbs, T. L., Wild, N. E., Proc. Roy. SOC.(London) A178, 380
(1941).
(20) Hirschfelder, J. O., Bird, R. B., Spotz, E. L., J . Chem. Phys. 16,968 (1948).
(21) Hirschfelder, J. O . , Bird, R. B., Spotz, E. L., Chem. Reu. 44,205 (1949).
(22) Hirschfelder, J. O., Bird, R. B., Spotz, E. L., Tmns. Am. SOC.Meck. Eng. 71,
921 (1949).
(23) Hirschfelder, J. O., Curtis, C. F., Bird, R. B., Molecular Theory of Gases
and Liquids, Wiley, New York (1964).
(24) Hoge, H. J., Lassiter, J. W., J. Res. Not. Bur. Sld. 47, 75 (1951).
(25) Holsen, J. N., Strunk, M. R., IND.ENG.CHEM.FUNDAMENTALS
3 , 1 4 3 (1964).
(26) Hudson G. H., McCoubrey, J. C., Ubbelohde, A. R., Trans. Faraday SOC.56,
1144 (1960).
(27) Ivakin, B. A., Suetin, P. E., Souiet Phys.-Tech. Phys. (English Trawl.) 8, 748
(1964).
(28) Jorgensen, F., Watts, H., Chem. Ind. 1961, 1441.
(29) Kennard, E. R., Kinetic Theory of Gases, p. 201, McGraw-Hill, New York,
1938.
(30) Klotz, I. M., Miller,D. K., J . Am. Chem. SOC.69,2557 (1947).
(31) Knox, J. H., McLaren, L., A n d . Chem. 8,1477 (1964).
(32) Kobe, K. A., Lynn, R. E., Jr., Chem. Reu. 52, 117 (1952).
(33) Kohn, J. P., Romero, N., J . Chem. Eng. Datu IO, 125 (1965).
(34) Lee, C. Y.,Wilke, C. R., IND.END.CHEM.46, 2381 (1954).
(35) Lydersen A. L. Estimation of Critical Properties of Organic Compounds,
Univ. Wiscdnsin, dng. Expt. Sta. Rept. 3, Madison, Wis. (April 1955).
(36) Malinauskas, A. P., J . Chem. Phys. 42, 156 (1965).
(37) Marquardt, D. W., Chem. Eng. Prog. 55 (6), 65 (1959).
(38) Marquardt, D. W., J. SOC.Ind. A p j l . M a t h . 11, 431 (1963).
. Least-Squares Estimation of Nonlinear Parameters,
(39) Marquardt, D. W
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