PREDICTION ACCURACY OF MULTICOMPONENT

VAPOR-LIQUID EQUILIBRIUM DATA FROM BINARY

PARAMETERS*

Isamu NAGATA
Department of Chemical Engineering, KanazawaUniversity,
Kanazawa,Japan
The prediction accuracy of the Wilson, NRTL,and Heil equations is shown on a wide
variety of multicomponent completely miscible systems including two quinary, seven
quaternary, sixty-nine ternary systems. Vapor
deration in all numerical calculations.
phase nonideality was taken into consi-
This assumption improves generally the
accuracy in the vapor composition and total pressure calculations for multicomponent
systems which were obtained under the assumption of an ideal vapor phase. The
Wilson equation seems to be the best of all the equations.

Introduction tion still experience

author's
remains partly unsolved, because the equilib-
in ternary vapor-liquid
present
rium calculations52'53'56'57) tends to suggest that
Calculations of vapor-liquid equilibria for a multi- the vapor phase nonideality should be taken into con-
component mixture from binary parameters have sideration. In this investigation the author carried out
drawn muchattention from a theoretical and practical predictions on two quinary, seven quaternary, and
standpoint. The applicability of the well-known Mar- sixty-nine ternary systems using the Wilson, NRTL,
gules and van Laar equations is widely understood. and Heil equations under the assumption of vapor
Several investigations have been carried out to evaluate phase nonideality in order to demonstrate the worka-
the merits of the recently published local composition bility of these equations and to compare the present
equations
TL), and
(the
Heil
Wilson, nonrandom two-liquid Most(NR
equations)22,25,36,58,60,64,69)#
results with those of Hudson and Van Winkle and
Nagata and Ohta.
of them dealt with the Wilson equation. Rather ex-
tensive studies on the capability of the Wilson equation Equilibrium Equation
are those of Homesand Van Winkle22) for twenty-
four ternary systems, Hudson and Van Winkle25) for An exact thermodynamic formula for vapor-liquid
one quinary, three quaternary, and twenty ternary equilibrium of a mixture is67)
systems, Nagata and Ohta58) for eleven ternary
systems, Renon and Prausnitz69) for tweleve ternary J>i<f>iPr-Vi(p
= TiXiPlfi
- p>) -]
exP
L RT J
systems, and Larson and Tassios36) for twenty-two (1)

ternary systems. Homesand Van Winkle, Hudson and
Van Winkle, and Nagata and Ohta assumed vapor
phase ideality. On the contrary, Renon and Prausnitz
and Larson and Tassios assumed vapor phase nonideal-
ity. Renonand Prausnitz also included results obtained
using the NRTL and Heil equations,
Tassios compared predicted ternary activity coefficient
with experimental data using the Wilson and NRTL
equations. The validity of vapor phase ideality assump-
where yi9 fii9 jiy xi9 P? and Vi are, respectively, the
vapor mole fraction, vapor phase fugacity coefficient,
liquid phase activity coefficient, liquid mole fraction,
vapor pressure of pure component i and partial molar
volume of comonent i. The partial molar liquid
Larson and
volume of component i was taken to be equal to the
molar liquid volume of pure component /. The vapor
fugacity coefficient is given by the virial equation
truncated after the second term.

In6i =
* Received onJune 21, 1972 l>lyjBij - in *
(2)
Paper presented at the 10th General Symposium (Nagoya, Nov.,
1971) of the Soc. ofGhem. Engrs., Japan The compressibility factor and the molar volume of the
18 (18) JOURNAL OF CHEMICAL ENGINEERING OF JAPAN
vapor mixture are related by Several methods have been suggested for obtaining
N N the binary parameters from experimental data. The
z= l +^ii=^ S Hytyfiu (3)
methods depend on the selected form of an objective
function. Homesand Van Winkle22) and Hudson and
Van Winkle25) used the following function.
The second virial coefficients, Bij:> are obtained from
the correlation of O'Gonnell and Prausnitz63). Liquid 2-j \Yiexptl T^-calcd)i 2-i Kf^exptl J'2calcd)%
molar volumes at three different temperatures were a =-k r-
fitted to a quadratic equation for interpolation. A six- k I
constant equation and the Antonie equation were (10)
used to represent the vapor pressure data of pure
components1'51'67). The critical constants, liquid molar Hudson and Van Winkle stated that their chosen
volumedata, vapor pressure data and other pertinent function yields the binary parameters which usually
physicochemical quantities are available67'68'84). give better multicomponent composition predictions
than the predictions resulting from the parameters ob-
Semitheoretieal Equations taining by minimizing the objective function suggested
by Orye and Prausnitz64) as follows.
The excess Gibbs free energy derived from the con-
cept of local composition for a multicomponent mixture t=iL * exptl _\i
is expressed by69)
However,better composition predictions are obtained
N
aE N N N . JLj^ji^ji^j
at the expense of poorer equilibrium temperature pre-
4= -&ln(SCW
RT <"* >-*
+©i^
^ ^Gktxk
(4) dictions. Nagata and Ohta58) used a regression method
fc=l which minimizes the deviations between the calculated
vapor compositions and experimental data. To fit the
where N is the number of components and tji and G^ experimental vapor compositions as well as the pressure
are defined as follows with the equation used, Renon and Prausnitz69) a-
rji = (gji - gu)lRT dopted as an objective function the sum of squares of
deviations in the vapor mole fraction plus the sum of
Gji = Pji
(6)
(5)
exP (- OCjitji squares of relative deviations in pressure. That is,
The Wilson, NRTL, and Heil equations are defined n
k
y(v v
k /
Y2_LV/.
p p
exptl rcalcd ^
\2
by giving the values given below top, q, p^ and aji- i=i i=i\ * exptl
Equation p q pjt a.ji*
Wilson 0 1 Vj/Vi 1
(12)
NRTL 1 0 1 aji In this work Eq.(12) was used to obtain each set of the
Heil 1 1 VjlVt 1 binary parameters. The detailed computation pro-
cedure is similar to the method suggested by Prausnitz
The activity coefficient is given by appropriate differ- et al.67). Table 1 indicates the numerical values of the
entiation of the excess Gibbs free energy expression. Wilson, NRTL, and Heil equations and the root-mean
square deviations of calculated values from experi-
\nTi=q\\ -\nT1xjGji- J:^JGil-~\
J]GkjXk å mental data. Several sets of equilibrium data for a
k=l binary system at a specified condition have been re-
ported by several investigators. The following items are
+P N ^^4-1
N
the criteria for selecting the proper binary parameters
Ti

HGkiXk
XlTljGlj åN
1=1

HGkiXjt J~1 TiGkjXk to be used for multicomponent prediction : 1. Equilibri-

k=i
umdata for a multicomponentsystem and its com-
(7) ponent binary systems should be taken from the same
This equation involves the liquid mole fractions and literature whenever possible. 2. Selected parameters
the binary parameters without any other parameters. should give a best fit for the binary data.
For a binary mixture Eq.(7) reduces to
^-{^C-^7-hh+"^']
Ihy^ ^21fill I ^12^12 I Prediction Accuracy of Multicomponent Vapor-
^ l (x1+x2G21)a + (x2+x1G12)2j Liquid Equilibrium Data
(8)
'" H-^tc XiG21 The binary parameters of the Wilson, NRTL, and
xx+x2G2 Heil equations listed in Table 1 were used to calculate
-ln(
^2+^12) multicomponent vapor-liquid equilibria. To indicate
+P4 how the respective assumptions ofa nonideal and ideal
T12G12
(x2+x1G12)2 (
(^+x2G2i)2 J
vapor phase affect predictions, the deviations in pre-
(9) dicted vapor mole fraction and system pressure of the
VOL6 NO.1 1973 (19) 19
ho
O Table 1 Parameters of Wilson, NRTL,and Heil equations and root-mean square deviations for binary dataD e v ia tio n s
P a ra m e ters [c a l/m o l]
N o .of R ela tiv e Vapo r mole
Bi n ar y Sy s te m (1 - 2) J em p . o r P re ssu re D a ta
d a ta W ilso n N R T L H e il p ressu re fr a ctio n
[m m H g ] so u rc e
p o i n t s [ x l O O O ] [ x lO O O]
(s 2 1 "S l l) (5 1 2-5 2 2 ) (5 2 1 -5 1 1) (5 1 2 -5 22 ) ｫ 12 (5 2 1 -5 1 1) (5 1 2-5 2 2 )
W a N b H e W N H W N H

A c eto n e-b en z en e 76 0 m m 12 626 - 270 712 - 322 0 .3 386 - 20 1 4 4 4

A c eto n e-c a rb o n tetra c h lo rid e 760m m 14 80 1 - 100 800 - 100 0 .3 46 1 - 120 8 8 8
A c eto n e -c h lo ro b en z en e 760m m ll 624 - 355 545 - 245 0 .3 369 - 230 11 11 11 10 10 10
A c e to n e -c h lo ro fo rm 760m m 3 3 3
- 20 - 386 60 - 460 0 .3 41 - 242
A c e to n e -c h lo ro fo rm 760m m ll - 4 12 10 7 - 499 0 .3 86 - 277 7 6 6
A c e to n e -c h lo ro fo rm 5 5 -C 75 - 480 80 - 500 0 .3 45 - 255 7 6 6
A c e to n e -c h lo ro fo rm 50 -C 29 71 - 4 77 17 5 - 569 0 .3 90 - 289 7 6 7
A c e to n e -c h lo ro fo rm 45 -C 9 8 8
A c e to n e -ch lo ro fo rm 35 -C 4 4 4
A c e to n e -cy c lo h ex a n e 760m m 355-4860 10 0 1 32 1 81881 61 - 563 00 027 0.3
0 .2 5 542 667 - 2 857 051 6 5 5
A c e to n e -c y c lo h e x a n e 5 5 -C 10 5 5 290 95 5 19 0 0 .2 555 50 9 10
A ce to n e -2 ,3 -d im eth y lb u ta n e 760m m ll 9 90 24 5 54 1 492 0 .2 501 42 10 12 12
A ce to n e -e th y l a lc o h o 1 760m m 13 2 05 2 00 54 0 - 12 0 0 .3 24 5 13 15 20 ll 10
A ce to n e -e th y l a lc o h o 1 5 5 -C 20 1 197 4 14 - 26 0 .3 114 84 9 9 9
Ac etone- w-hexa ne 760 mmAcet one-rc- hexane 55-G 11 8
13 11 12
A ce to n e-w -h ex a n e 4 5 -C 10
A ee to n e -72-h ex a n e 3 5 -C 9954245733704607 97 1 425 444 432 61 666 8613 7507 0..222 .
00. 454 808 772 1 1947 8508 16 16 15
A ce to n e-iso p ro p y l a lc o h o 1 760m m ll 340 10 0 12 5 295 0 .3 46 173 ll 12 8
A ce to n e-iso p ro p y l a lc o h o 1 5 5 -C 14 500 45 1 14 0 .3 245 - 5 11 10 10 9 7 8
A ce to n e-m eth y l a lc o h o 1 76 0 m m 10 - 14 7 545 265 120 0 .3 - 13 7 310 2 2 2
A ce to n e-m e th y l a lc o h o 1 760m m 12 25 390 4 18 - 31 0 .3 - 99 2 69 11 11 11 10
A ce to n e -m e th y l a lc o h o 1 7 6 0m m ll - 97 4 97 4 86 - 70 0 .3 - 12 9 30 0 4 5 4
A ce to n e-m e th y l a lc o h o 1 5 5 -C ll - 129 518 42 6 - 30 0 .3 - 16 5 3 30 4 4 10 11 10
A ce to n e-m e th y l a lc o h o 1 5 5 -C 28 - 126 54 6 44 3 - 16 0 .3 - 40 24 0 7 7 8 4 54 (3 9) 33 3 (3 9) 22 3 (17)
A ce to n e-m e th y l a lc o h o 1 5 0 -C 35 - 254 629 139 224 0 .3 - 19 0 350 14 14 14 4 4 4 (7 7 )
A ce to n e-m e th y l a c eta te 76 0 m m ll 195 - 128 - 140 2 10 0 .3 - 31 64 5 6 6
O
A ce to n e-m e th y l a c eta te 5 0 -C 4 4 4 4 54 (4 6) 3 43 (7 7 )7 7 7 (4)
A c eto n e-m e th y l e th y l k e to n e 760m m 23 -86 25 - 17
10 30 - - 137 05 220 0.
0 .33 -- 39 60 78 60 39 39 38
c
>
XJ
A c eto n e-m e th y l iso b u ty l k e to n e 760m m 17 5 - 70 342 - 240 0 .3 10 2 - 58 12 10 12 13 14 13 9 7 9 (2 7 )
z
I- A c eto n e-w a te r 760m m 8 9 9 4 19 18 (6 2 )
o B e n z en e -a n ilin e 7 0 -G 1 1 1 2 2 2 (2 3 )
B e n z e n e -ch lo ro b e n z e n e 760m m I l l 3 4 3 (16 )
B e n z e n e -cy c lo h ex a n e 760m m 10313710839491 12 14 9 - 1451372 452 146 02 069 - 2245 0874 0561 0.3
0 .3 - 3 47 487 - 72 096 264 5 24 23 2 2 2 2 2 2 (4 9 )
Tl
o
B e n z e n e -cy c lo h ex a n e 760m m 3 3 3 2 2 2 (7 0 )
I B e n z e n e -cy c lo h e x a n e 760m m 4 4 3
m B e n z e n e -cy c lo h e x a n e 300m m 9 9 1 1 12 2 2 (4 2 )(42)
o
B e n z e n e -cy c lo h ex a n e 7 0 -C 8 8 8 2 2 2 (8 2 )
> B e n z e n e -cy c lo h ex a n e 5 0 -C 11 11 11 2 2 2 (4 2 )
B e n z e n e -w-h e p ta n e 760m m 3 3 5
m B e n z e n e -w-h ep ta n e 4 00m m 6 4 4 223 2 1 1 ( 9 ) (59)
G) B e n z e n e -rc -h ep ta n e 180m m 6 3 4 1 1 1 (5 9 )
-z. B e n z e n e -rc -h ep ta n e 7 5 -C 4 6 4 3 7 5 (18 )
m B e n z e n e -rc -h ex a n e 760m m 4315ll1702-4836 24 28 1 2-1904 067 - - 235419256375
1 592317 - 5742212
194035982 0956737
10 0.3
0 .3 322119
149672
12 11660937
13 1 39510
13
- - 12 18
7390471 61 1 21 1 3 4 4 2 2 2 (70 )
m B e n z e n e -iso p ro p y l a lco h o 1 760m m 5 6 5 6 6 7 (4 6 )
B e n z e n e -iso p r o p y l a lco h o 1 760m m 12 12 14 4 3 6 (9 1 )
-z. B e n z e n e -iso p ro p y l a lco h o 1 5 5 -G ll 13 13 3 5 4 (4 0 )
a B e n z e n e -w-p ro p y l a lc o h o 1 7 5 -G 6 8 6
oTl B e n z e n e -to lu e n e 760m m 4 4 4 3 5 33 3 3 (1 8 )(29)
C a rb o n te tr ac h lo rid e -b e n ze n e 760m m 4 4 4 4 4 4 (1 5 )
> C a rb o n te tr a ch lo rid e-b e n ze n e 70 -C 3 3 3 2 2 2 (7 3 )
1-31190-365091325-10223050 104 045 060
12 - 23230
18541 2598 - 1 348916
107395722508 0.43 7
0.3
0. - - 110452315 090851 - 24561 4892175 501051 1 41 14 124 (c o n tin u ed )
a W = W ilso n . b N - N R T L . c H = H e il.
-z.
Data
Pressure
points
PreSS-
[nunHg]

'n
o
N3
B
mye)tr2say-n1Si(

Carbontetrachloride-benzene
Carbontetrachloride-cyclohexane
Carbontetrachloride-isopropylalcohol
Chloroform-benzene
Chloroform-benzene
Chloroform-ethylacetate
Chloroform-ethylalcohol
Chloroform-ethylalcohol
Chloroform-ethylalcohol
Chloroform-rc-hexane
Chloroform-rc-hexane
Chlorofornwz-hexane
Chloroform-rc-hexane
Chloroform-methylalcohol
Chloroform-methylalcohol
Chloroform-methylisobutylketone
Cyclohexane-aniline
Cyclohexane-/z-heptane
Cyclohexane-isopropylalcohol
Cyclohexane-toluene
Cyclohexane-toluene
2,3-Dimethylbutane-chloroform
2,3-Dirhethylnutane-methyl
1,4-Dioxane-H-hexane
1,4-Dioxane-l-hexene
Ethylalcohol-benzene
Ethylalcohol-benzene
Ethylalcohol-benzene
Ethylalcohol-benzene
Ethylalcohol-benzene
Ethylalcohol-cyclohexane
Ethylalcohol-cyclohexane
Ethylalcohol-cyclohexane
Ethylalcohol-cyclohexane
Ethylalcohols-heptane
Ethylalcohol-n-heptane
Ethylalcohol-rc-heptane
Ethylalcohol-isopropylalcohol
Ethylalcohol-methylcyclopentane
Ethylalcohol-toluene
Ethylalcohol-water
rc-Heptane-/z-butylalcohol
rc-Heptane-rc-butylalcohol
w-Heptane-rc-propylalcohol
w-Heptane-toluene
w-Hexane-benzene
n-Hexane-benzene
w-Hexane-cyclohexane
rc-Hexane-cyclohexane
rc-Hexane-cyclohexane
rc-Hexane-ethylalcohol
rc-Hexane-ethylalcohol
alcohol
TVá"á"
or

40°C
760mm
760mm
760mm
50°C
760mm
55°G
45°C
35°C
760mm
55°C
45°C
35°C
760mm
50°C
760mm
70°C
760mm
760mm
760mm
50°C
760mm
760mm
760mm
760mm
760mm
400mm
300mm
180mm
50°G
760mm
300mm
50°C
50°C
750mm
400mm
180mm
760mm
760mm
50°C
760mm
760mm
50°C
75°C
760mm
760mm
70°C
760mm
760mm
70°C
760mm
760mm
No. °f
data

18
15
19
19
18
15
15
15

22
25
14
12
25
12
31

17
10
ll

10
10

18
18
17
10
13

19

15
22
12

32
16
16
9
8

9
9
9
9

5
9

5
5
5
5
5
5

8
8

7
(521-5ll)

-291

-75
-14
-428
-295
-295
-SCO

-3£0
-440
-248

-150

1485
1467
1710
1600
1651
1956
2501
2503
2185
2140
2220
2300
-60
2240
1427
442
150
215
245

320
-46
422
270
40
105

325
240
325
367

740
220
-64

125
545
710
520
46

70

127
310
310
Wilson

(512-522)

1720
1940
-182
1340
1500

-219
-148
292
435
246
2715
275
200

338
340
320
340
500

220
180
901
1350
1310
1485
180
100
344

-64
2205
2005
490

-50
-120
-34

13

70
173
105
150
128
319
365

20
70
1300

1445
1545
16C0
-15
120
45
6
-

320
-294

-758
-295
-2S0
-290
-£9
-73

-95
-205
-280
680
500
107

693
1505
307
501
1105
1125
1170
1160
1175
1401
1640
1605
1500
1420
1400
1220
-74
1620
956
1488
450
502
745
394
521
221
400
-110
273
950
920
Parameters

(521-5ll)

-341
37

21

ll
25

31

20
NRTL
[cal/mol]
~

(512-522)

-240

-215

-168

-300
-223
538

1020

-153

390
470
455
470
465
794
920
895
850
1000
1100
1380
-3
760
590

1050
1001

-145
945

1525
1340
66

186

350
1375
14C5
14C5
S96
381
326
325
1270
1535

955
-2
1150

-312
100
200

1865
601
193

68

150
«12

0.3
0.3
0.47
0.3
0.3
0.3
0.3
0.3
0.3
C.2
0.2
0.2
0.2
0.3
0.3
0.3
0.3
0.3
0.47
0.3
0.3
0.2
0.47
0.3
0.3
0.47
0.47
0.47
0.47
0.47
0.47
0.47
0.47
0.47
0.47
0.47
0.47
0.3
0.47
0.47
0.3
0.47
0.47
0.47
0.3
0.3
0.3
0.3
0.3
0.3
0.47
0.47
-
(521-5ll)

-175

-247
-1S9
-2C0
-2C0

-2£0
-347
-136
140

810
709
760
740
766
851
900
906
870
1120
940
820
-72
1031
720

-40

247
-36
125
107
-23
15
20

145

176
175
176
171

292
-46
100

265

400
256
25
25

40

77

70
21

20
5

5
Heil
-~^

(512-522)

270

-190
-195

-95

-29

-160
-40

-40
40
600

-4

8C0
973
-77
581
600

1020

-5
-13
-27
20
685
7C0
7C0
-33
-25

10

108

80
85
15

50
84

28
50
42
40

100

-41
71

460
705
660
660
99

178
-65
-59
36
920
870
1
25
Relative
pressure
[x
W N

19
24
19
27

17
lOOO]

10

17
22
26

10
15
ll

12

12

2
5
3
3
2
6

7
3
5

3
4
4

4
2
7 10
9 ll

5
2
3

6
13 23
5
7
2
9
3
6
3
5
2

37 34
43

18
6
27
31

18

10
14
18
28

20
14

21

13
21
7 12
2
15

26

2
2
4
2
3
6

7
4

5
7
3

5
8
8
3
7
6
8
6

3
3
5
9
3
5
5
1.8

6
6

1
H

26

63

44
50
38

21
12

18
23
27

15
13
ll

12

14
22
20
30

34
16
3
5

8
3

5
7
9

8
9
3
7
4
4
7
8
7

2
7
3
2
2
6
5
6
5

4
4

7
Deviations
Vapor mole
fraction

13
16

ll

10

12
14
[X 1000]

4
5
8
6
4
3
ll
13
15

24 26
25
40
10
13

14
10
23

14
15
9

3
5
7
3
3
5
5

4
2
6

8
4
2
4
5
9

9 19

9 10
4
5
6
4

7
16
18

27
21

15

17

24

18
16
N

10

10
12

ll
18

14

10

3
6
6
2
4
5
4
5

5
4

6
6
8

1
5

4
4
6

8
8

5
5
9
5

9
2
8

5
5

31
20
H

21

49
13

10
13
15

12
10
16

12

13
ll

12

18
20
16
41
45
37
10
17

16
10
28

2
4
5

8
4
3

4
4

1
5

4
4
9

7
6

8
8

3
5
7

3
5
4
3
W

10

19
15

14

14
18

12

13
3

2
3
3
2
4

5
p

8
3
2
9
4
0
2
9
5

4
3
2

5
1
2

8
5

1
3
8
2

3
6
5
4
3

3
3
8
7

1
1

1
1

1
N

16

20

17

20
14

14

ll

12

16
4

4
3
0
2

6
2
3
2

6
5

1
8

2
1
3
1
2
5

5
1

1
4

2
2
4

4
4
3
7
6

6
3
1

5
4
3
4
-
H

ll

20

48

33
20

16

10
17

13

26
12
5

2
5
2
2
1
5
4
2
7

6
9
6
3
1
1
3
2
3
3

1
1
4
9
4
2
3
6
6
5
3
3
3
2

8
4
2
1

(continued)
^

source

(73)
(71)
(50)
(47)
(56)
(48)
(72)
(72)
(72)
(32)
(32)
(32)
(32)
(48)
(77)
(27)
(23)
(45)
(54)
(44)
(92)
(88)
(88)
(81)
(81)
(42)
(59)
(42)
(59)
(42)
(42)
(42)
(42)
(92)
(28)
(28)
(28)
(31)
(78)
(92)
.(31)

(66)
(82)
(45)
(70)
(82
(73
(33
(3)
(3)
(18)
(21)
 BinarySystem(1-2)
Temp,or press.
No.of
points data
Parameters [cal/mol]
3N Wilson NRTL Heil
(g21-gll) (glit'g22) (g21-gll) (gl2~g22) «12 (g21-gll) (gl2'g22)

WN H WN H WN H
rc-Hexane-ethyl
n-Hexane-ethyl alcohol 55
45 °C 9 9 306
327 21441001
2300 945 1520 1381 0.475
0.4710 900
905
w-Hexane-ethyi
rc-Hexane- 1 -hexene alcohol 35°G 1
760mm 96 325 2380
320 10021567 0.47 21 894
rc-Hexane-methylcyclopentane
Isopropyl
Methyl alcohol-water
acetate-benzene 760mm
760mm
760mm 18
12 670 --200
29 7761222
425 255
-320
441
90
2010
387
- 640.3
- -
-
137
320
180
0.343 30
0.3180580
0.3242 --116
21 0
Methyl
Methyl
Methyl acetate-benzene
acetate-carbon
acetate-chloroform 50°G
tetrachloride
760mm 17
760mm
15 12126100-73
540
96-455 318
- 140430-50
397 - 0.3
690 0.3
0.3126-
327 95 - 13
126
-270
Methyl
Methyl
Methyl acetate-chloroform
acetate-isopropylalcoholacetate-cyclohexane
760mm1 7 207 301 1 12
Methylacetate-methyl alconol 760mm
50°G
760mm
14
16
14-63
127
1001 -503
731 88 412
231 652-387 724
402 2590.3
0.2
0.3
0.3 50122
147
-97 1 -302
-101
391 6
Methylalcohol-carbon tetrachloride
Methylalcohol-cyclohexane 35°G
55°G 9
10 2450
2700 155
600 1715
1805 800
1450 0.47
0.47 1203
1 107 -157
Methylalcohol-ethyl acetate 760mm 20 987 -246 447 250 0.3 577 -267 0

Methylethyl ketone-isopropyl alcohol 760mm 5 -289 692 -40 350 0.3 -200 400

Methyl acetate-methyl alcohol 50 °C 15 -89 800 338 331 0.3 - 138 450
Methyl acetate-methyl ethyl ketone 760mm 9 566 -42 1 555 -425 0.3 196 - 170
Methyl alcohol-benzene 760mm 18 1 740 100 1 126 668 0.47 92 1 - 147
Methyl alcohol-benzene 55 °G 9 1827 141 1242 690 0.47 940 - 120
Methyl alconol-benzene 35 °G 9 1822 181 1290 670 0.47 932 - 102
M ethyl alconol-carbon tetrachloride 55°G 6 2292 156 1559 770 0.47 1 152 - 174

ON
Methyl alcohol-ethyl alcohol 760mm 12 - 175 280 242 -283 0.3 268 -298
Methyl alcohol-n-heptane 760mm 7 252 1 753 1 700 1 670 0.47 982 26
Methyl alcohol-isporopyl alcohol 760mm 8 467 -597 88 -2 15 0.3 10 - 10
Methyl alcohol-isopropyl alcohol 55 °G 20 48 11 107 - 100 0.3 7 32
Methyl alcohol-toluene 760mm 10 1910 140 1 160 825 0.47 896 - 11 7
Methyl alcohol-water 760mm 10 2 16 453 955 -299 0.3 151 197
o
Methylcyclohexane-aniline 1 00.02 °C 13 71 0 1 205 905 690 0.3 340 500
c
DI Methylcyclohexane-aniline 90 °G 16 76 1 1 254 940 700 0.3 323 542
:z Methylcyclohexane-aniline 80 °G 14 800 1 300 905 785 0.3 305 590
> Methylcyclohexane-toluene 1 00.02 °G 15 60 1 40 250 - 50 0.3 41 60
o Methylcyclohexane-toluene 90 °G 14 20 1 80 252 - 47 0.3 20 80
n~ Methylcyclohexnae-toluene 80 °C 12 85 1 36 260 40 0.3 6 99
O Methylcyclopentane-benzene 760mm 33 1 97 10 1 340 - 65 0.3 70 70
I Methylcylopentane-cyclohexane 760mm 3 472 - 322 262 - 220 0.3 425 - 2 70
Methylcylopentane-toluene 760mm 27 - 11 3 353 125 90 0.3 61 48
O Methyl ethyl ketone-benzene 760mm 10 492 -240 649 - 385 0.3 270 - 146
> Methyl ethyl ketone-benzene 760mm 5 422 -209 535 -32 1 0.3 318 - 179
Methyl ethyl ketone-benzene 55 °G 5 426 -201 487 -273 0.3 202 - 102
Methyl ethyl ketone-rc-butyl alcohol 760mm 6 - 95 535 - 98 501 0.3 - 64 275
o Methyl ethyl ketone-rc-butylalcohol 50 °C 7 572 - 94 655 - 190 0.3 298 - 66
Methyl ethyl ketone-cyclohexane 760mm 10 870 35 850 10 0.3 476 - 43
Methyl ethyl ketone-?2-heptane 760mm 8 1005 - 15 792 100 0.2 600 - 140
M
ethyl ethyl ketone-rc-heptane 50 °G 8 1032 - 9 866 45 0.2 550 - 90
DC
Methyl ethyl ketone-isopropyl alcohol 55 °G 5 -44 500 10 430 0.3 - 77 305
O Methyl ethyl ketone-toluene 760mm 23 51 5 -200 584 -244 0.3 331 - 166
Toluene-aniline 100.02 °C 12 1 10 520 200 400 0.3 26 277
> Toluene-aniline 90 °G 17 1 54 500 2 19 406 0.3 63 250
Toluene-aniline 80 °G 11 1 70 500 197 441 0.3 70 250
>
 Table 2 Comparison of multicomponent accuracy of Wilson, NRTLand Heil equations
H ud s on an d V a n W in k le Pr e se n t w or k
Te m p, o r - D at a^ st em pr es s. wi ls on W i l s o n N R T L H e i l W i l s o n N R T L H e i l so ur c e
A y [ x lO O O ] a A T [- C p o r A P [m m H g ] c Ay [ x lO O O ] A P [m m H g ]
Quina ry(HudsonandVanW i n k l e , 1 9 6 9 ) , 15datapoints 15datapoints (24)Ben zene 5 0.39-G 4 4 5 4 . 9 6.4 5.7

C h loro form
Met hyl al co hol 760 mm 12
M ethy l accetate
A ceton e
Quaternary(HudsonandV a n W i n k l e , 19 6 9 ) , 2 9 d a t a p o i n t s 29datapoints (24)Benzene 4 0.25-C 4 4 5 6 . 1 7 .4 6.0

Chlorofo rm 760 mm
Methylalcoho1 8 5 5 6M ethy lace tat e 4 5 5 4Qu ate rnar y(Si nor and Webe r, 1 960 ;Bel kna pand Webe r, 196 1;Ka esan dWe ber, 19 62), 40da tap oints (78)

3 8 da ta p oi n ts
E th yl a lc o ho 1 7 0 .6 3- C 8 ll 20 8. 4 1 3. 0 1 6. 4 Be n ze ne 7 60 m m 7 4 4 6

M eth ylcyclop entane 4 4 4 5r c-H ex ane 8 9 10 17

C hloroform
Ternary(Myers,1957), 25da ta poi nts 76 dat ap oin ts (4 3)c yc loh ex ane 10 0. 93 -G 4 4 4 5. 5. 6.2 5 .3r c- Hep tan e 76 0m m 7 2 2 2T olu en e 8 3 4 3

Ternary(Suryanarayanaan dV a n W in k l e ,1 9 6 6 ), 1 6 da t a p o in t s 16 d a ta p o i n ts ( 8 1) r c - He x a n e 6 0 . 87 - G 4 5 5 l l . 9 1 2.3 12.8

I- H e x e n e 760 mm 7 6 10
1,4 -D ioxan e 12 9 11
Ternary(Amer,Paxtonan dV a n W i n k l e , 1 9 5 6 ) , 2 5 d a t a p o i n t s 9 1 d a t a p o i n t s ( 2 3A c e t o n e 14 0.26-C 8 9 9 6 . 1 5.8 6.9

M e th y l c y c lo p e n t a n e 7 6 0 m m 4 3 3 3w.-Hexane 3 4 3 3

T e rn a ry ( Na g a ta , 19 6 2) , 25 d at a po i nt s 91 d at a po i n ts (4 7 )M e th y l ac e ta t e 8 0 . 21 - C 5 6 6 3 .3 3.2 4.4chloroform 760mm 4 3 2 5

B en z en e
X : -

Methyl a c e t a te 14 15 10 1 3

T e r n a r y( W i l l o c k an d V a n W i n kl e , 1 9 6 9 ), 2 5 d a t a po i n t s 2 7 d a t a po i n t s ( 8 8 )2 , 3 - D i m et h y l b u t an e 6 1 . 02 - C 8 l l 1 5 1 4 . 7 3 5 . 6 1 4 . 2M e t h y l a lc o h o 1 7 6 0mm 5 6 10 llAcetone 4 5 7 9

T e r n a r y ( N a g a t a , 1 9 6 4 ) , 1 5 d a t a p o i n t s 7 0 d a t a p o i n t s ( 4 6 ) B e n z e n e 3 0.62-C 4 4 6 4.4 4.7 6.7

C y c lo h e x a n e 7 6 0 m m 7 5 5 7 I s o p r o pylalcoho1 10 4 6 10

Ter nary(Nag ata,1962) , 25da tapoints 72da tapoints (48)Met hylalcoho 1 8 0. 27-C ll 1 2 12 15.2 18.7 16 .9Ethyla cetate 7 6 0 mm 7 8 8 8chloroform 8 9 ll ll

Acetone 8 8 9 12

Ternar y(HudsonandVanWinkle,1 969), 13datapoints 13d atapoints (24)Methylal coho1 6 0.27-C 3 5 6 7.3 10.6 9.3Methylacetate 760mm 5 7 6 8chloroform 6 7 7 8

( c o n t in u e d )
Jjy=J>calcd-JVexptl* b J T = jH c a lc d - 7 *e x p tl ｫ c J P = P e a le d - ^ e x ptl*

VOL.6 NO.1 1973 (23) 23

 H ud s on an d V an Wi n kl e P r es e nt w o rk
T emp , or - - -- - Dat ab ys tem pr ess . wi ls on W ils on NR TL He il W ils on N RTL H eil s our ce
Ay [xlOOO] AT¥-G] or AP [mmHg] Ay [xlOOO] AP [m mHgl
Terna ry (Wal do an d Webe r, 196 3), 7 data points 41 data points (86)
E thyl alcoh ol 6 0 .59 -C 6 7 11 4 .8 5.3 9 .1
Be nzene 760 m m
r c-H exan e 9 4 5 1 0
25 da ta p oin ts 5 7 da ta po in ts (2 6)
Ethylacohol90.25-C 8 12 2 1 6 .0 10 .4 18 .0
Methylcopenta 760 m m
rc-Hexane 7 9 10 16
Nagata a n d O h ta

Ternay (K u d ry a v tse v a & S u sa re v , 19 6 3 ), 3 6 d a ta p o in ts 3 6 d a ta p o in ts (3 5 )

Ethyl a lco h o l 8 7 .8 m m 7 9 11 3 .8 4 .8 2 .9
Chloroform 3 5 -G 8 8 11 10
ra-Hexane 8 8 10 10
Ternary (K u d ry a v tsev a & S u sa re v , 19 6 3 ), 3 6 d a ta p o in ts 3 6 d a ta p o in ts (3 5 )
E t h y a llco h o l 6 8 .3 m m 7 7 1 1 3 .6 3 .9 3 .8
Chlorform 4 5 -G 13
rc-Hexane 12
Ternary (K u d ry a v tsev a & S u sa re v , 1 9 6 3 ), 36 d a ta p o in ts 3 6 d a ta p o in ts (3 5 )
E t h y allco h o l 7 1 1 .8 m m 11 13 17 8 .3 9 .2 5 .0
Chloroform 5 5 -C
rc-Hexane 4 8 8 12
Ternay (F r esh w a te r & P ik e , 19 6 7 ), 2 7 d a ta p o in ts 2 7 d a ta p o in t (1 7 )
Acetone 6 5. 3 m m 7 8 7 5. 8 3. 5 5. 0
Methyl a lc o h o l 5 5 -C 5 10 7 1 1
I so p ro p y l a lco h o l

T e r n a r y( M o r a c he v s k i i &Z h a r o v , 19 6 3 ) , 1 9 d a t a p oi n t s 1 9 d a t a po i n t s (4 2 ) E t h y la l c o h o 1 8 ll.Omm 10 12 13 5.6 5.5 4.8

B enzene 50 -C 11 1 1 11
Cyclohexane 7 11 12 13

Te rnary (Naga ta,19 70), 31dat apoin ts 31d atapo ints ( 52)Me thyla cetat e ll 0.6-G 4 4 4 7.4 5.7 6.3
Carbon tetra c h lo rid e 760 m m
B enzene

T e r n a r y (N a g a t a , 1 9 65 ) , 3 9 d a t a p o in t s 3 9 d a ta p o i n t s ( 50 ) c a r b o n te t r a c h l o r id e 4 0.4-G 3 3 4 ll.0 ll.8 13.5

Benzene 760 m m
Iso p ro p y l a lc o h o l 6 7 8 11

present work, and that of Hudson and Van Winkle, /2-hexane, and acetone-methyl alcohol-cyclohexane
and Nagata and Ohta, are compared on twenty-seven systems. Similar results were recently reported by
multicomponent systems as shown in Table 2. In the
Larson and Tassios36). All three equations give nearly
last two investigations only the Wilson equation was comparable and accurate results for systems with
used under the assumption of an ideal vapor phase. In strong hydrogen bonding compounds such as the
some cases, the predictions based on the vapor phase acetone-methyl alcohol-water, ethyl alcohol-isopropyl
ideality assumption are better than those based on the alcohol-water and acetone-methyl alcohol-isopropyl
vapor phase nonideality assumption. However, the pre- alcohol systems. The Wilson and NRTL equations do a
dictions, especially in pressure (equal to boiling point), considerably finejob for systems having more than four
are generally improved by using the vapor phase non- components, but the Heil equation gives the poorest
ideality assumption. Table 3 shows the deviations of predictions in three cases out of nine systems (two
predicted values from experimental data for two quina- quinary and seven quaternary systems). The Wilson
ry, seven quarternary and sixty-nine ternary systems. equation seems to be the best in overall performance on
For the ternary systems where, the deviations from ide- the basis of the systems studied.
ality are not too large, for example, the cyclohexane-ra-
heptane-toluene system and the methyl acetate-chloro-
Conclusion
form-benzene system, all equations give similar results.
However, for highly nonideal systems such as the 2, 3-
dimethylbutane-acetone-methyl alcohol system and the
The binary parameters of the Wilson, NRTL, and
Heil equations for 155 binary systems were determined
2, 3-dimethylbutane-methyl alcohol-chloroform system, using a nonlinear regression method. These parame-
the Wilson equation gives better predicted results than ters were used to predict vapor-liquid equilibria for
the other equations. For the mixtures of alcohol and 78 multicomponent systems. In all numerical calcu-
nonpolar liquids the Heil equation gives less accurate lations the vapor phase nonideality was taken into
predictions than the Wilson and NRTL equations. The consideration. It is found that the vapor phase nonide-
NRTL equation gives the poorest prediction in ality assumption usually improves multicomponent
pressure for three ternary systems consisting of alcohol, prediction accuracy compared with the ideal vapor
hydrocarbon, and acetone, namely, the 2,3-dimethyl-
phase assumption and the Wilson equation shows
butane-methyl alcohol-acetone, acetone-ethyl alcohol- better overall performance than the other equations.

24 (24) JOURNAL OF CHEMICAL ENGINEERING OF JAPAN

 Table 3 Deviations of predicted values from experimental data for multicomponent systems
Deviation in^vapor^mole fraction' Deviation in pressure

System Temp'or data° A-tVl t- Absolute Root-mean Relativeb Absolute^ ^at*

Arithmetlc Press* points arithmetic square [xlOOO] [mmHg] SOurce

Wd Ne Hf W N H W N H W N H W N H
yraniuQ (Weatherford & Van Winkle, 1970) (87)
w-Hexane -3 -4 -2 4 4 3 4 5 3 -19-14-21* -15-ll-16^
Methylcyclopentane 0 0-2 7 6 7 10 10 10 19 14 21* 15 ll 16^
Cyclohexane 760mm 10 1 1 -1 3 3 4 4 4 5 20 15 21* 15 ll 16*
Benzene -1 0 1 3 2 3 3 3 3
Toluene 3 3 4 4 3 4 4 4 5

Benzene -4 -4-5 4 4 7 6 6 7 2 6 -1 1 4 -1
Chloroform 3 4 2 4 6 3 5 7 3 6 9 7 5 6 6
Methylalcohol 760mm 15 8 8 8 8 9 10 10 10 10 8 ll 9 6 8 7
Methylacetate -3-2-2 5 4 6 6 5 6
Acetone -4-6 -3 4 6 5 6 7 5

2,3-Dimethylbutane 14 12 16 14 12 17 14 12 18 14 ll 28 ll 9 21
Methylalcohol 760mm 5 0-1 1 5 4 5 6 5 6 14 16 28 ll 12 21
Acetone -10-12-13 10 12 13 ll 13 15 16 17 29 12 13 22
Chloroform -4 1 -4 5 5 6 6 6 7

Cyclohexane -1-1-1 6 6 6 9 10 9 1-3 1 1-3 1

Benzene 760mm 58 -3 -2 -3 9 10 9 14 13 14 5 6 5 4 5 4
Isopropylalcohol 2 2 2 8 7 8 ll 10 ll 7 8 7 5 6 5
Methylethylketone 2 1 2 6 7 6 10 ll 10
Ethylalcohol 3 3 3 7 7 8 9 10 10 2-4-7 1-4-5
Chloroform 55°C 84 2 4 3 6 6 6 7 8 7 8 10 10 5 7 7
Acetone -4-6-4 8 9 9 ll 12 12 10 12 12 7 9 9
rc-Hexane -1 -1 -2 10 10 ll 13 12 13
Ethylalcohol 1 1 0 6 9 20 8 12 25 -10-8-22 -8-6-16
Benzene 760mm 20 1 0 2 4 4 7 6 5 9 10 ll 23 8 9 18
Methylcyclopentane 0 0 3 5 5 6 9 9 9 13 16 33 10 12 25
rc-Hexane -2 -1 -5 10 ll 18 18 19 26

Ethylalcohol 4 1-15 1.4 20 30 20 23 34 -3-5-34 -2-4-26

Benzene 760mm 10 -4-3 -1 4 4 4 5 5 4 14 18 35 10 14 26
Methylcyclopentane 0 1 4 2 2 4 3 3 5 17 21 41 13 16 31
rc-Hexane 0 1 12 12 14 24 17 19 28
Benzene _3_3-3 4 3 5 6 4 6 -2 6-5 -2 5-4
Chloroform 760mm 29 4 4 3 6 8 6 7 10 7 8 10 8 6 7 6
Methylalcohol 0 0 0 5 6 6 7 8 8 9 12 10 7 9 7
Methylacetate -1-1 0 5 5 4 6 6 6

Ethylalcohol 2 6 7 4 8 10 4 9 13 -9-4-3 -7-3-2

Benzene 760mm 10 -3-6-5 4 6 6 4 7 6 9 6 6 7 4 4
Methylcyclopentane 3 2 2 5 5 6 6 7 7 10 7 7 7 5 6
n-Hexane -2 -2 -4 3 4 8 5 6 9

Benzene -"1 -1 -1 9 9 8 ll ll 10 -5-6-3 -3-4-2

rc-Hexane 70°C 21 -2-2-1 7 7 6 8 8 7 5 6 3 3 4 2
Cyclohexane 3 3 2 5 5 5 8 8 7 6 7 4 4 5 3

Methylcyclohexane 4-1 3 4 4 3 4 7 3 7 2 3 2 1 1
Aniline 80°C 7 0-1 0 0 1 0 0 1 1 7 6 3 2 2 1
Toluene _4 2-3 4 4 3 4 7 3 7 7 3 2 2 1
Ternary (Schneider, 1961) (76)
Methylcyclohexane 1-1 0 3 3 3 4 4 4 3-1-2 2- 0-1
Aniline 90°C 9 1 1 1 1 1 1 1 1 1 3 4 3 2 2 2
Toluene -2 0-1 3 3 3 4 4 3 4 5 4 2 2 2

Methylcyclohexane -1-2-3 2 2 3 3 3 4 5-1-1 3 1-1

Aniline 100.02°C 9 1 1 1 1 1 1 1 1 2 5 2 5 3 1 3
Toluene 0 1 2 2 1 3 3 2 3 6 2 6 3 1 3
Ternary (Podder, 1963) (65)
Cyclohexane 8 4 5 8 7 8 ll 8 10 8 0 5 3-1 1
Aniline 70°C 10 0 0 0 0 0 1 1 1 1 8 ll 12 3 5 5
Benzene -8-4-5 8 7 8 ll 8 9 18 16 18 5 6 6
Methylacetate 4 6 4 5 6 6 6 8 7 -3 3-5 -2 2-4
Chloroform 760mm 91 1 0 2 3 2 5 5 4 6 4 4 6 3 3 4
Benzene -5-6-6 5 6 6 6 8 7 5 5 7 4 4 5
^ffSe^^^'197^ 3 2 2 4 4 4 5 5 5 -1-6-7 -1-3-3 (M)
Chlorofonn 50»C 66 -2-1 -1 2 2 3 3 3 4 5 B * 2 3 4
(continued)
a 4)>Scaled->xplt. b iPrel^^calcd-PexplO/Pexplt. c JP^Pcalcd-^explt. d W=Wilson
e N^NRTL. f H=Heil. s Arithmetic. h Absolute arithmetic. i Root-mean square.

VOL6 NO.1 1973 (25) 25

Deviation irx
n vloo
apor
oi m ole fraction
Deviation in p ressure

No.ofsystem lemp.or d Absolute Root-meanpress- points Arlthmetlc aritbmrtic square R elative A bsolu te D ata
[ x lOOO] [m m H g]

W N H W N H W N H W N H W N H

Ternay(Ngat, 1970 ) (52 )

M eth yl aceta te _ 3 _ 1 9 - 3 - 1
Carbon tetrachloride 760 m m 31 - 2 - 2 - 2 10 8 8
B en zen e ll 9 10
Ternary(Nagata & O h ta , 197 1) (5 71
G ycloh exan e - 1 0 - 1 4 3 4 5 4 5 3 1 4 2 1 3
Carbon tetrachloride 760 m m 29 1 1 1 5 4 5 4 3 4
B enzen e 0 - 1 0 5 5 6 4 4 4
T ernary (N agata, 1962 )chloroform 00-1 9 ll ll ll 13 14 20 25 22 15 19 17 (48)

M eth yl alcoh o1 760 m m 72 2 2 4 ll 13 12 13 15 14 20 25 22 15 19 17

E thy l acetate - 2 - 2 - 3 8 8 8 ll ll ll 25 29 25 19 22 19
Ternay (N ag ata & H ayashida , 19 70) (56)
M eth yl acetate 1 4 1
Isopropyl alcoho l 760 m m 32 - 3 - 4 - 2 5 9 5 4 7 4
B en zen e - 2 - 3 6 10
Ternary (N agata & O hta, 19 711 (57)
M eth yl acetate _ 6 _ 9 - 4 - 5 - 1 - 3
M eth yl alcoh o1 760 m m 18 1 1 1 6 8
B en zen e - 2 - 3 - 3 7 10
T ern ary (N agata, 1965) (50 1
C arbo n tetrachloride - 1 - 1 - 1 3 3 4 4 5 10 9 10
Benzene 760 m m 39 - 2 - 2 - 2 15 16 18 ll 12 14
Isop ropy lalcoho1 3 3 3 7 8 ll 9 10 12 20 21 24 15 16 18
T ern ary (N ag ata , 19 62) (49)
M eth yl acetate 10 9 ll 15 10 13 19 ll 16 7 - 1 5 - 1 3
B en zen e 760 m m 60 _ 7 _ 6 - 7 ll 9 10 16 10 13 12 7 10
G y clohexan e - 3 - 3 - 4 9 5 8 12 7 10 20 12 15 15 9 12
T ern ary (N ag ata, 19 64) (46)
B en zen e - 3 - 3 - 2 4 4 6 2 - 6
G y clohexan e 760 m m 70 1 1 - 2 5 5 7 7 7 10 6 6 9 4 5 7
Isopropyl alcoh o1 2 2 4 4 6 10 6 7 13 8 8 13 6 10
Ternay (D on ald & R idgw ay , 1958) (13)
M ethy l ethy lk eton e 1 1 1 7 7 7 10 10 10 0 1 1 0 0
G y clohexan e 760 m m 86 - 2 - 2 - 2 7 .7 7 10 10 10 8 7 8 6 5 6
B en zen e 1 1 1 3 3 3 4 4 9 9 9 1 1 1
Ternary(Kudryavtseva & S usarev, 1963) (34)
A ceton e - 1 - 1 - 1 9 9 9 ll 12 12 10 13 15 8 10 ll
Chloroform 760 m m 37 - 1 - 2 - 2 ll 14 16 9 ll 12
ra -H exan e 14 17 19 ll 13 14
Ternay (K u dry avtseva & Su sarev, 19 63) (34 1
A ceton e - 3 - 5 - 5 ll 12 12 12 14 14 7 4 5 5 3 3
Chloroform 55 -G 37 0 0 1 10 8
/2-H exan e 12 ll ll
Ternay (K u dryavtseva & Su sarev , 19631 (34 )
A ceton e 0 - 2 - 1 12 14 14 13 15 16 19 18 22 9 10
C h loroform 4 5 -C 37 - 4 - 4 - 4 9 9 9 10 ll ll 21 20 24 10 9 ll
72-H exan e 4 6 5 9 ll ll ll 14 14 25 25 28 12 12 13
Ternary(Kudryavtseva & Su sarev, 1963) (34 )
A ceton e - 3 - 4 - 4 12 14 15 14 17 18 15 19 23
C hloroform 35 -C 37 - 5 - 6 - 5 8 10 9 10 12 12 16 19 23
rc -H exan e 8 10 9 12 15 15 15 18 19 20 24 28
T ernary (K u dry avtseva & Su sarev , 1963)Ethylalcoho1 79 1215 13 19 21 19 23 6 ll 0 (35 )

C hloroform 76 0 m m 36 0 - 2 - 1 7 8 8 10 10 ll 6 12
rc -H exane - 7 - 7 - ll 10 9 14 16 15 19 7 13 10 5 10
T ern ary (K ud ryav tseva & S usarev, 196 3)Ethylalcoho1 10 1214 ll 13 17 14 15 18 (35)
12 13 1 8 9 1
C hloroform 5 5 -G 36 - 3 - 5 - 3 7 9 8 9 ll 10 12 14 8 9
rc-H ex ane - 7 - 7 - ll 8 8 12 12 ll 15 13 15 10 9 10
Trneary (K ud ryav tseva & S usarev, 196 3) (35)
E thyl alcoh o1 3 6 9 7 7 11 10 8 12 0 12 1
C h lo roform 45 -C 36 - 5 - 4 - 3 8 9 8 10 10 10 13 8
rc-H ex ane 2 - 2 - 6 7 7 9 9 9 12 10 14 ll
T ern ary (K ud ryavtsev a & Su sarev, 1963)Ethylalcoho1 2 6 8 7 9 ll 8 ll 15 (35)
12 15 1
C h loroform 35 -G 36 - 2 - 5 - 3 8 ll 10 10 12 ll 12 16
rc-H exan e 0 - 1 - 5 8 10 10 10 13 15 14 18 12
T ern ary (M orach evskii & Z h arov , 19 63)Ethylalcoho1 610 1210 12 13 13 15 14 1 - 5 - 10 0 - 2 - 4 (42)

B enzene 50 -G 19 0 - 1 0 ll ll ll 20 20 22 13 13 ll
C ycloh ex ane - 6 - 9 - 12 ll 12 13 26 27 27 18 18 18
T ernary (M orachevskii & Z h arov, 196 3)Ethylalcoho1 4 7 9 10 ll ll 17 19 18 - 16 - 18 - 22 - 5 - 5 - 7 (42)

Benzene 300 m m 19 3 0 0 17 18 22
C ycloh ex ane - 7 - 7 - 9 7 8 10 14 15 15 19 20 24
(con tin ued )

26 (26) JOURNAL OF CHEMICAL ENGINEERING OF JAPAN

 D ev iation in v ap or m ole fraction
D e v i a t i o in
n p ressure

[xlOOO]No.of _ _system ^ data Arithmetic Absolute Root-meanr- points arithmetic square R elativ e A b solu te D ata
[x lO OO] [m m H g]

W N H W N H W N H W N H W N H
Ternary (M orachevskii & Z h arov, 1963) (42)
E th yl alcoh o1 5 7 7 12 14 14 18 19 18 0 2 - 1
Benzene 760 m m 19 - 3 - 4 - 2 9 9 8 7 7 6
G ycloh ex ane - 2 - 3 - 5 ll 12 14 17 18 18 13 13 ll 10 10 8
Ternary (D eshp an de & L u , 196 5) - 12 - 12 - 18 - 9 - 9 - 14 (10)
E th yl alcoho 1 4 4 3 15 17 19 22 24 27
B en zen e 760 m m 57 - 2 - 1 0 10 ll ll 18 19 19 17 17 20 13 13 15
C ycloh exan e - 2 - 3 - 3 10 10 13 15 16 19 24 26 31 19 20 23
Ternary (S catchard & T ick nor, 19 52) 19 12 40 4 12 (75)
M eth yl alcoh o1 5 2 5 5 6 21 6 7 23
Carbontetrachloride 34.68 -C 6 - 1 0 - 2 3 4 9 3 4 10 19 12 40 4 12
B en zen e - 4 - 2 - 3 4 5 13 5 5 15 19 14 46 4 14
Ternary (S catch ard & T ickn or, 1952 ) (75 )
M ethyl alcoho1 6 7 7 6 8 17 7 10 18 ll 8 11
C arbon tetrach lorid e 55 -C 8 - 6 - 8 - 5 6 9 9 12 13 10 ll 8 25 6 17
B en zen e 0 1 - 2 ll 13 10 ll ll 28 8 19
Ternary (W illock & V an W in kle, 1970) 15 20 17 ll 15 13 (88)
M ethyl alcoh o1 6 6 9 6 7 9 8 9 10
Acetone 760 m m 5 - 7 - 7 - ｣ 15 20 17 ll 15 13
Chloroform 1 1 - 1 15 20 18 12 15 14
Ternary (W illock & V an W in kle, 1970) (8 8)
2,3-D im ethylbu tane 7 3 6 8 ll 15 10 13 19 - 19 - 47 - 12 - 14 - 36
M eth yl alcoh o1 760 m m 27 - 4 - 4 - 1 .6 10 ll 7 ll 15 19 47 19 15 36 14
A cetone - 3 1 - 5 5 7 9 5 9 ll 2 1 50 22 16 38 16
Ternary (K irby & V an W ink le, 1970) (30)
2,3-D im ethy lbu tan e 1 0 3 4 9 19 5 ll 29 14 22 17 ll 17 13
M eth yl alcoh o1 760 m m 21 - 1 1 - 2 6 9 24 8 ll 34 14 24 37 ll 18 28
C hlorofo rm 0 - 1 - 1 7 9 12 10 ll 14 15 27 45 12 , 20 35
Ternary (H ud son & V an W ink le, 1969) (24 )
C hloroform 6 ll 4 8
M eth yl alcoho 1 760 m m 13 0 - 2 1 10 14 12 7 ll
M eth yl acetate - 3 - 2 - 4 ll 16 14 8 13 10
Ternary (G arrett & V an W in kle, 1969 1 (20)
A ceto ne 3 3 3 8 9 12 9 ll 14 14 18 24 ll 14 18
Chloroform 760 m m 19 - 1 14 18 24 ll 14 18
2 ,3-D im eth ylbu tan e - 2 - 1 - 2 7 8 14 8 10 17 16 21 27 12 16 21
Ternary (Fu & L u , 19 68) (19)
B en zene 4 3 1 14 15 14 22 22 22 - 13 - 17 - 18 - 8 - 10 - 12
^-H ep tane 75 -C 78 - 6 - 5 - 7 12 12 14 22 22 24 15 18 20 9 l l 13
rc -P ropy lalcoh o1 2 2 - 6 14 14 15 22 22 23 18 2 1 22 ll 13 14
Ternay (W agn er & W eb er, 19581 (851
E th yl alcoho l - ll- 10 - 16 14 13 22 19 18 27 - 2 - 1- 12 - 2 - 1 .- 9
B enzene 76 0 m m 47 4 3 8 9 3 ll 13 12 15 8 10 17 7 13
rc -H eptan e 7 7 8 9 8 14 13 12 19 12 14 2 2 9 ll 17
Ternay (N ielsen & W eb er, 19 59) (59 )
E thy l alcohol - 6 - 5 - 14 ll 14 24 . 21 26 40 7 10 - 13 4 - 5
B enzen e 400 m m 50 3 3 9 8 9 14 12 13 20 17 23 25 9 10
^-H eptan e 3 2 5 7 9 13 14 18 25 26 32 4 2 10 13 17
Ternary (O akeson & W eb er, 1960) (6 1)
E thy lalcoho1 2 4 3 8 17 22 17 27 35 5 - 3 - ll 1 ^ 1 - 2
Benzene 180 m m 55 - 2 - 1 0 7 10 ll 10 14 17 ll 16 2 1
rc-H ep tan e 0 - 3 - 3 7 12 13 14 20 22 15 27 38
Ternary (Su ry anaray ana & V an W ink le, 1966) .(8 1)
rc-H ex an e 0 0 0 _ 10 - 4 - ll - 7 - 3 - 9
1-H exen e 760 m m 16 5 5 4 6 10 6 8 ll 8 16 16 17 12 12 13
1,4-D iox ane _ 5 - 5 - 4 9 ll 9 10 13 ll 19 22 2 1 15 17 16
Ternay (V inich en ko & S usarev, 196 6) (90)
A ceto ne 9 7 7 10 13 13 14 17 16 - 17- 36 - 32 - 13- 27 - 24
E thyl alcoh o1 760 m m 20 - 10 - 9 - 8 ll 13 12 15 17 17 19 36 32 14 27 24
rc-H exan e 1 2 1 5 8 7 7 10 20 37 34 16 28 26
Ternay (V in ich en ko & S usarev, 196 6) (90)
A ceton e 1 1 1 8 12 ll ll 14 14 - 16 - 2 7 - 23 - 13 - 22 - 18
E th yl alcoh o1 55 -G 21 - 4 - 3 - 4 6 8 7 8 10 16 2 7 23 13 2 2 18
w.-Hexane 3 2 3 6 8 9 8 10 ll 17 28 24 14 2 2 19
Ternary (Z h arov et al.9 1968) (92)
T olu ene 1 0 0 4 12 4 7 16 - 10 - 52 - 14 - 3 - 16 - 5
C ycloh ex ane 50 -G 19 1 29 - 7 6 30 9 8 32 12 13 53 18 4 16
E th yl alcoho l - 2 - 29 7 8 3.1 ll ll 37 15 16 62 23 5 18
Ternary (K aes & W eber, 1962) (2 6)
E th yl alcoho l - 1 - 1 - 1 8 12 21 12 16 27 4 3
M eth ylcyclop en tane 760 m m 57 1 0 1 5 6 9 8 9 12 8 14 23 6 10 18
rc -H ex ane 0 1 0 9 10 16 ll 14 22 ll 17 30 9 13 23
Ternay (O ch i & K qjim a, 197 1) (62 )
A ceton e 1 1 - 2 9 9 9 ll 12 12 1 - 3
M ethy l alcoho1 760 m m 109 4 4 5 9 9 9 12 12 13 9 10 10
W ater - 5 - 5 - 3 12 12 12
(continu ed )

VOL..6 NO.1 1973 (27) 27

 Deviation m vapor mole fraction Deviation in pressure

System Temp'or data° A.., ,. Absolute Root-mean Relative Absolute ^f**

Arithmetlc
Source ress' points arithmetic square [xlOOO] [mmHg]

P W N H W N H W N H W N H W N H
Ternary (Severns et al., 1955) (77)
Acetone -5 -6 -6 9 10 9 12 13 13 14 16 14 7 8 8
Chloroform 50°C 30 -3 -2 -2 9 9 9 12 ll ll 17 18 18 9 10 10
Methylalcohol 8 8 8 10 9 9 12 ll ll 21 22 22 ll 12 12
Ternary (Severns et al., 1955) (77)
Acetone -4 -4 -4 1 1 1 ll ll ll 7 8 5 4 5 3
Methylalcohol 50°C 35 1 1 2 13 13 13 20 20 20 8 9 7 5 6 5
Methylacetate 3 3 2 9 9 9 15 15 15 ll 12 10 1 1 1
Ternary (Waldo & Weber, 1963) (86)
Ethylalcohol 5 6 5 6 7 ll 8 10 15 -2-1 -6 -1 -1 -5
Benzene 760mm 41 -5 -7 -3 6 7 7 8 9 8 6 7 12 5 5 9
rc-Hexane 0 1 -2 4 5 10 6 7 13 9 10 20 7 8 15
Ternary (Belknap & Weber, 1961) (7)
Benzene -3 -4 -3 4 4 4 4 6 5 -8 -4 -5 -6 -3 -4
Methylcyclopentane 760mm 54 2 2 2 3 3 3 4 5 4 8 4 5 6 3 4
n-Hexane 1 2 1 4 3 3 5 4 5 9 5 6 7 4 5
Ternary (Kojima et al., 1968) (31)
Ethylalcohol -1 -2 -1 12 12 12 14 15 14 5-13 -6 0-10 -4
Isopropylalcohol 760mm 53 6 3 4 12 ll 10 15 14 13 9 15 9 7 ll 7
Water -5 -2 -2 8 10 8 10 12 10 12 18 12 9 13 9
Ternary (Amer et al., 1956) (2)
Acetone 3 5 5 8 9 9 10 ll ll -1 1 1 -1 1 1
Methylalcohol 760mm 91 -7-7-8 12 ll 12 15 14 15 8 8 9 6 6 7
Ethylalcohol 4 2 3 6 6 6 8 8 8 10 9 ll 8 7 8
Ternary (Karr et al., 1951) (27)
Acetone 2 2 2 6 10 6 9 13 9 -16-15-15 -12-12-12
Chloroform 760mm 46 2 3 2 4 6 4 5 8 5 21 20 20 16 16 16
MethylisobutylKetone -4-5 -4 6 7 6 9 10 10 28 28 28 22 21 21
Ternary (Babich et al., 1969) (4)
Acetone -3 -4 -4 8 7 8 10 8 9 -6 1 -3 -5 0 -3
Methylacetate 760mm 16 9 9 10 10 10 10 13 12 13 12 8 10 9 6 7
Methylethylketone -6-5-6 8 6 7 9 7 8 15 10 12 ll 7 9
Ternary (Freshwater & Pike, 1967) (17)
Acetone -2 -5 -1 7 8 7 8 9 8 -7 6 -6 -3 3 -2
Methylalcohol 55°C 27 -5-1 -6 10 7 ll 13 9 14 12 7 ll 6 4 5
Isopropylalcohol 7 6 7 9 7 9 ll 9 ll 14 9 13 7 4 6
Ternary (Ridgway & Butler, 1967) (70)
Benzene -1 -2 -2 4 4 4 6 6 6 4 4 2 3 3 1
Cyclohexane 760mm 108 2 2 2 6 5 6 1 1 1 5 4 3 3 3 2
w-Hexane -1 0 0 5 5 5 1 1 1 5 5 4 4 4 3
Ternary (Freshwater & Pike, 1967) , (17)
Acetone 1 -1 1 1 1 1 8 9 8 -14-15-15 -ll-ll-ll
Methylalcohol 760mm 21 -ll -9-12 13 ll 13 16 14 16 15 16 17 ll 12 13
Isopropylalcohol 10 10 ll 10 10 ll 14 15 15 17 19 21 13 14 16
Ternary (Sinor & Weber, 1960) (78)
Ethylalcohol -1 0-1 6 9 13 10 12 16 -ll -7-2 -9-6-1
Benzene 760mm 47 -2 -4 -4 3 4 5 4 5 6 12 ll 10 9 8 8
Methylcyclopentane 3 4 5 5 7 ll 9 ll 15 15 14 14 ll ll ll
Ternary (Myers, 1957) (43)
Cyclohexane -2 -2 -1 4 4 4 5 5 5 -5-7-5 -4-5-4
w-Heptane 760mm 76 1 0 0 2 2 2 3 2 2 7 8 7 6 6 5
Toluene 1 2 1 3 4 3 4 5 4 9 9 8 7 7 6
Ternary (Free & Hutchison, 1959) . (16)
Acetone 0 2 2 5 4 4 6 5 6 -13 -7 -9 -10 -5 -6
Benzene 760 mm 54 5 3 3 6 4 4 7 5 6 14 8 9 10 6 7
Chlorobenzene -5 -5 -5 5 5 5 5 6 6 16 10 ll 12 8 9
Ternary (Subba Rao & Venkata Rao, 1966) (80)
Acetone 4 3 4 7 7 7 9 9 9 -2 -3 -1 -2 -2 -1
Carbontetrachloride 760mm 57 -3 -2 -3 1 1 1 8 8 8 16 15 15 12 ll ll
Benzene -1 -1 -1 4 4 4 6 6 6 21 21 20 16 16 15
Ternary (Steinhauser & White, 1949) (79)
Methylethylketone -6-6-7 7 7 8 8 9 10 -1 -4-5 -1 -3-3
w-Heptane 760mm 37 3 3 4 5 6 6 6 7 8 4 5 6 3 4 4
Toluene 3 3 3 3 4 4 4 4 4 5 6 7 3 5 5
Ternary (Benedict et al., 1945) (8)
Methylalcohol -1 2 -2 7 7 ll 8 9 13 -5-12-4 -4-9-3
rc-Heptane 760mm 8 1 -2 2 4 3 8 4 5 9 6 12 14 5 9 10
.6 Toluene 0 0 0 3 3 5 4 5 13 17 16 10 13 12
Ternary (Marinichev & Susarev, 1965) (40)
Methylethylketone -10-8-9 14 12 14 17 16 18 2 -4 4 1 -1 1
Benzene 55°C 19 2 -3 -3 6 4 8 7 5 9 6. 6 8 2 2 2
Isopropylalcohol 12 ll 12 13 12 13 16 15 16 7 8 9 2 3 3
Ternary (Zharov et al., 1965) (91)
Methylethylketone -8 -9 -8 12 12 12 15 15 15 1 -2 -5 1 -2 -4
Benzene 760 mm 19 3 3 2 5 4 4 6 4 5 5 3 6 4 2 5
Isopropylalcohol 5 7 6 10 12 ll 13 15 13 7 5 8 6 4 6
(continued)

28 (28) JOURNAL OF CHEMICAL ENGINEERING OF JAPAN

 Daviton in
[x vap
lO OO]
or m ole fraction
Deviation in p ressu re
Fj^ poi
m p nts
.or arithmetic
dN o . ofssquare
ysteAm rith m etic A b so lu te R o ot-m ean
R elative A bsolute D ata
[x lOOO] [m m H g] sou rce

W N H W N H W N H W N H W N H

T ern ary (S usarev etaL , 1965)Acetone ^8 -8 -9 9 9 10 10 10 ll (83)

10 6 0 4 0
Chloroform 760 m m 36 - 2 - 2 - 3 10 8
E th yl alcoho1 10 10 12 10 10 13 ll ll 15 14 ll 12 ll 8
T ernary (M arin ich ev & Su sarev, 19 65)Acetone -4 -1 -5 9 14 ll 12 18 13 (40)
- 25 - 65 - 3 1 - 22 - 55 - 26
M eth yl alcoh o1 5 5 -G 21 6 5 4 9 22 10 13 26 13 25 65 3 1 22 55 26
C ycloh ex ane - 2 - 4 1 ll 24 14 12 27 16 26 66 33 22 56 28
Ternay (M arin ich ev & Su sarev, 19 65) (40)
A ceton e - 7 - 4 - 18 10 15 19 13 17 22 - 16 - 53 8 - 12 - 40
M ethyl alcoh o1 760 m m 21 ll 10 22 ll 19 22 14 24 26 16 53 17 12 40 13
C ycloh ex ane - 4 - 6 - 4 10 22 10 12 25 12 17 54 22 13 4 1 17
T ernary (A ristovich et al., 1965 )Methylethylketone 33 312 13 12 14 16 16 (3)
15 8 8 12
cr -H ep tan e 760 m m 14 15 15 15 18 19 19 26 27 27 25 22 22 19 17 17
w-Bu tyl alcoh ol - 18 - 18 - 18 19 18 18 23 22 22 29 26 27 22 20 21
Ternary (A ristovich et al., 1965 ) (3)
M ethy lethyl keton e 15 16 17 21 22 22 24 24 25 - 7 - 20 - 9 - 2 - 4 - 2
n-H ep tan e 50 -C 14 5 4 3 19 21 20 24 25 25 24 30 25
B-B utyl alcoh ol - 20 - 20 - 20 22 22 22 28 27 28 3 1 37 32

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