Fluid Phase Equilibria 180 (2001) 103113

A new modication of the UNIQUAC equation including

temperature dependent parameters
Barbara Wi sniewska-Gocowska, Stanisaw K. Malanowski

Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44, 01-224 Warszawa, Poland
Received 16 March 2000; accepted 28 November 2000
Abstract
The UNIQUAC equation was modied by introduction of a linear temperature dependence of the volume and
surface area parameters, r
i
and q
i
. The slope of r
i
and q
i
functions were found to be the same for hydrocarbons
and pyridine. The modied equation was used for prediction of vaporliquid equilibria (VLE) in binary mixtures
of hydrocarbons and pyridine with hydrocarbons as well as for the prediction of the excess enthalpy (H
E
) in
binary mixtures formed by pyridine with aliphatic alkanes. The results obtained were compared with predictions by
UNIFAC and further with UNIQUAC equation and its modication involving temperature dependant coordination
number z. The proposed temperature dependence of the r
i
and q
i
parameters enables prediction of the VLE at
various temperatures and leads to reasonable values of H
E
. The necessary input reduces to one set of isothermal
VLE data. One set of UNIQUAC interaction parameters u
ij
is sufcient for representation of VLE in a wide range
of temperature and to obtain a reasonable prediction of H
E
. 2001 Published by Elsevier Science B.V.
Keywords: Vaporliquid equilibria; Excess enthalpy; Activity coefcient; Correlation; Prediction
1. Introduction
Knowledge of the vaporliquid equilibriumdata (VLE) is necessary to design and optimize distillation,
which is one of the most frequently used separation methods. To minimize design cost, tedious and expen-
sive VLE measurements are avoided and prediction and correlation methods are used instead. The most
difcult problem is to obtain accurate information on the temperature dependence of activity coefcients.
Knowledge of this dependence is important for systems formed by pyridines with hydrocarbons. The
UNIQUAC equation [1] represents the activity coefcients as a function of concentration for systems
formed by pyridine with aliphatic alkanes very well.
The main aim of the present work was to modify the UNIQUAC equation in such a way that it would
be possible to predict, with high accuracy, the activity coefcients and VLE of these systems as function

Corresponding author. Tel.: +48-22-632-6713.

E-mail address: skm@ichf.edu.pl (S.K. Malanowski).
0378-3812/01/$20.00 2001 Published by Elsevier Science B.V.
PII: S0378- 3812( 00) 00514- 8
104 B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113
of temperature. Consequently, the excess enthalpy can also be predicted. As input data, measurements at
only one temperature are sufcient.
The UNIQUAC equation gives a good representation of vaporliquid equilibria (VLE) using only two
adjustable interaction parameters u
ij
which describe the energy of interaction between molecules i and j,
for each binary pair. These parameters are temperature independent. Therefore, the set of u
ij
parameters
calculated by tting the original UNIQUAC equation to isothermal VLE data should make it possible
to predict VLE in a wide range of temperatures. In practice, the accuracy of such a prediction is poor.
A more accurate prediction can be obtained by introduction of temperature dependent parameters into
the UNIQUAC model. Temperature dependent interaction parameters (u
ij
) and coordination number (z)
have been proposed by other authors [2,3].
In this work, the temperature dependence of the volume and the surface area parameters, r
i
and q
i
is
proposed. This modication is a physically better justied than earlier ones.
To test the proposed modication of the UNIQUAC model its comparison with experimental excess
enthalpies (H
E
), and excess enthalpies calculated from the original UNIQUAC and the proposed modi-
cation involving a temperature dependent z have been performed.
2. Temperature dependent volume and surface area parameters
The following assumptions are made to modify UNIQUAC equation:
The volume r
i
and the surface area q
i
parameters are linearly dependent on temperature while the
interaction parameters u
ij
remain constant.
Reference values of r

i
and q

i
at standard temperature T

are dependent on the molecule involved.

The temperature dependent parameters a and b (Eqs. (1) and (2)) are the same for each series of
homologues and isomers.
The assumptions are summarized in the following equations:
r
i
= r

i
+a(T T

) (1)
q
i
= q

i
+b(T T

) (2)
Reduction of literature data [4] available for two binary systems: pyridine +n-heptane and benzene +
cyclohexane leads to the following values:
a = 0.015 and b = 0.010
The reference values of r

i
and q

i
at temperature T

(used in Eqs. (1) and (2)) were computed by the

group contribution method proposed by Abrams and Prausnitz [1].
3. Calculations and results
The UNIQUAC equation with temperature dependent r
i
and q
i
parameters as given by Eqs. (1) and (2)
was used for the prediction of the VLE and excess enthalpies in binary systems based on data for only
one VLE isotherm. A set of u
ij
parameters was calculated by tting the original UNIQUAC equation to
the constant temperature VLE data. This temperature was set as reference (T

) for predictions in a wide

range of temperature.
B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113 105
Table 1
The average relative standard deviation of equilibrium pressures RMSD(P)
T (K) RMSD(P) Reference
Prediction (UNIQUAC) Correlation Prediction
r = f(T),
q = f(T)
z = f(T) r,q,z =
const.
UNIQUAC UNIFAC
Pyridine + n-heptane 298.15 3.978 5.557 8.970 1.000 10.099 [9]
303.15 3.466 4.773 7.956 0.950 9.092 [9]
313.15 2.144 3.204 6.276 0.277 7.432 [10]
313.15 2.777 3.675 6.297 0.843 7.432 [9]
323.15 2.148 2.742 4.727 0.861 5.856 [9]
333.15 1.735 2.118 3.411 0.680 4.514 [9]
340.95 0.538 0.908 2.043 0.361 3.410 [11]
348.15 2.841 2.978 3.301 1.287 4.336 [12]
353.15

0.254 1.197 [11]

Pyridine + n-octane 313.15 2.373 4.143 6.966 0.297 6.962 [10]
348.15 4.263 4.463 4.790 1.056 5.171 [12]
353.15

0.221 0.442 [11]

369.75 0.442 1.217 2.456 0.404 1.964 [11]
Pyridine + n-nonane 313.15 1.106 2.684 8.863 0.241 8.252 [10]
348.15 3.487 4.454 6.173 1.465 5.571 [12]
369.75

0.365 0.864 [11]

Pyridine + n-decane 353.15

0.592 1.827 [11]

373.55 1.929 2.757 4.443 1.640 4.690 [11]
Pyridine + cyclohexane 293.15 0.882 0.741 0.735 0.628 12.050 [13]
298.15

1.191 10.460 [14]

303.15 0.788 0.859 1.321 0.516 10.257 [13]
303.15 1.141 1.108 1.173 1.181 9.620 [14]
308.15 1.038 0.959 1.459 1.081 8.755 [14]
308.15 0.860 0.976 1.962 0.458 9.380 [13]
313.15 0.965 1.122 2.678 0.405 8.470 [13]
318.15 1.385 1.331 2.492 1.018 6.612 [15]
318.15 1.094 0.858 2.403 0.978 7.245 [14]
328.15 1.355 0.854 3.339 0.917 5.918 [14]
338.15 1.683 0.869 4.257 0.858 4.673 [14]
348.15 2.106 0.899 5.075 0.828 3.572 [14]
Pyridine + benzene 298.15 0.295 0.383 0.308 0.118 0.693 [16]
303.15 0.247 0.295 0.255 0.126 0.673 [16]
313.15 0.218 0.318 0.320 0.078 0.451 [16]
323.15

0.412 0.713 [16]

Pyridine + methylbenzene 293.15 0.578 0.889 0.704 0.548 1.610 [13]
298.15 0.660 0.537 0.493 0.492 1.696 [13]
303.15 0.539 0.639 0.587 0.504 1.372 [13]
308.15 0.527 0.477 0.475 0.464 1.490 [13]
313.15

0.363 1.368 [13]

323.15 0.413 0.708 0.727 0.173 1.402 [17]
333.15 0.284 0.840 0.930 0.134 1.321 [17]
373.15 0.609 1.061 1.702 0.019 1.118 [18]
106 B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113
Table 1 (Continued)
T (K) RMSD(P) Reference
Prediction (UNIQUAC) Correlation Prediction
r = f(T),
q = f(T)
z = f(T) r,q,z =
const.
UNIQUAC UNIFAC
Cyclohexane + n-octane 298.15

0.480 3.189 [19]

308.15 0.509 0.551 0.689 0.247 2.523 [19]
318.15 0.209 0.315 0.594 0.159 2.367 [19]
328.15 0.276 0.487 0.892 0.154 1.948 [19]
Benzene + n-hexane 298.15 2.486 2.438 2.697 0.383 3.703 [20]
298.15 0.294 0.256 0.547 0.106 1.778 [21]
303.15

0.245 1.096 [22]

307.91 0.125 0.146 0.234 0.114 1.026 [21]
312.94 0.131 0.132 0.550 0.113 0.686 [21]
313.15 0.213 0.227 0.505 0.216 0.627 [22]
323.15 0.191 0.180 0.976 0.179 0.188 [22]
328.25 0.750 0.828 0.680 0.266 0.635 [23]
333.15 0.270 0.200 1.536 0.166 0.552 [22]
343.15 0.927 0.921 2.709 0.218 1.658 [24]
Benzene + n-heptane 293.15 1.394 1.219 3.269 0.492 2.482 [25]
318.15 0.607 0.617 1.292 0.382 0.563 [26]
333.15

0.123 0.740 [27]

348.15 0.492 0.615 1.090 0.418 1.766 [28]
353.15 0.269 0.059 0.689 0.058 1.549 [29]
Benzene + cyclohexane 283.15 0.819 0.701 2.467 0.220 2.471 [30]
311.65 0.259 0.268 0.889 0.201 0.982 [31]
313.15 0.272 0.272 0.908 0.171 0.959 [32]
328.15 0.626 0.616 0.505 0.308 0.404 [31]
333.15

0.082 0.163 [30]

343.15 0.203 0.257 0.570 0.023 0.438 [33]
343.15 0.223 0.269 0.565 0.140 0.434 [34]
343.15 1.064 1.116 1.419 0.445 1.268 [24]
351.95 0.393 0.495 0.946 0.026 0.828 [35]
403.15 0.551 0.625 2.167 0.130 2.315 [36]
413.15 0.815 0.695 2.359 0.083 2.558 [36]
423.15 1.196 0.746 2.511 0.086 2.767 [36]
Isopropylbenzene + n-heptane 313.15

0.417 1.684 [37]

333.15 0.474 0.245 0.618 0.140 0.825 [37]
353.15 0.577 0.239 0.815 0.101 0.497 [37]
Ethylbenzene + methylcyclohexane 313.15

0.866 1.177 [37]

333.15 1.032 0.987 1.257 0.782 0.921 [37]
353.15 1.185 1.138 1.656 0.809 1.039 [37]
373.15 0.856 0.736 1.717 0.048 0.682 [38]
Ethylbenzene + methylbenzene 298.15

0.787 0.858 [39]

373.15 0.236 0.473 0.599 0.072 0.070 [38]
Carbon tetrachloride + n-heptane 298.15 0.444 0.471 1.108 0.349 3.474 [40]
308.15 0.476 0.516 0.934 0.218 3.124 [40]
318.15 0.320 0.343 0.488 0.292 2.446 [40]
328.15

0.117 1.914 [40]

Denotes reference temperature.

B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113 107
To test the applicability of proposed equations, a comparison of computed equilibrium pressure with
experimental VLE data and earlier prediction methods was made for 86 binary systems.
The equilibrium pressure at various temperatures was calculated using the following versions of UNI-
QUAC equation:
1. The proposed modication with temperature dependent r
i
and q
i
.
2. The original equation with u
ij
obtained in version 1. and r
i
and q
i
independent of temperature.
3. The UNIQUAC equation with temperature dependent coordination number z.
4. An independent correlation of each set of isothermal data with the UNIQUAC equation and with
predictions with the UNIFAC [5,6] method.
The second virial coefcients used were estimated by the method of Tsonopoulos [7].
For each isotherm the average relative standard deviation of the equilibrium pressure was calculated
by the equation
RMSD(P) = 100

1
N
N

i=1

P
exp.
i
P
cal.
i
P
exp.
i

1/2
(3)
where P
exp.
i
is the experimental vapor pressure, P
cal.
i
the corresponding calculated vapor pressure, and N
the number of data points.
The average relative standard deviations of equilibrium pressures RMSD(P) for each investigated
isotherm are shown in Table 1. For binary mixtures formed by pyridine and aliphatic alkanes the average
relative standard deviation of equilibrium pressures RMSD(P) are also plotted in Figs. 14.
The values of r

i
and q

i
used in the UNIQUACequation are shown in Table 2. The values of the interac-
tion parameters u
ij
in the original UNIQUAC equation and in the UNIQUAC equation with temperature
dependent coordination number z (obtained by data reduction at the reference temperature T

) are shown
in Table 3.
A computation of the excess enthalpy (H
E
) is the most sensitive method to check the reliability of
equations representing the temperature dependence of phase equilibrium parameters for mixtures. For
binary systems formed by pyridine and aliphatic alkanes a comparison of H
E
computed from various
Fig. 1. The average relative standard deviation of equilibrium pressures, RMSD(P), for each isotherm T for the binary mixture
pyridine + n-heptane: () prediction using UNIQUAC with r, q = f (T T

); () prediction using UNIQUAC with

z = f (T ); () prediction using original UNIQUAC; () correlation using UNIQUAC; () prediction using UNIFAC.
108 B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113
Fig. 2. The average relative standard deviation of equilibrium pressures, RMSD(P), for each isotherm T for the binary mixture
pyridine + n-octane: () prediction using UNIQUAC with r, q = f (T T

); () prediction using UNIQUAC with

z = f (T ); () prediction using original UNIQUAC; () correlation using UNIQUAC; () prediction using UNIFAC.
Fig. 3. The average relative standard deviation of equilibrium pressures, RMSD(P), for each isotherm T for the binary mixture
pyridine + n-nonane; () prediction using UNIQUAC with r, q = f (T T

); () prediction using UNIQUAC with

z = f (T ); () prediction using original UNIQUAC; () correlation using UNIQUAC; () prediction using UNIFAC.
Fig. 4. The average relative standard deviation of equilibrium pressures, RMSD(P), for each isotherm T for the binary mixture
pyridine + n-decane: () prediction using UNIQUAC with r, q = f (T T

); () prediction using UNIQUAC with

z = f (T ); () prediction using original UNIQUAC; () correlation using UNIQUAC; () prediction using UNIFAC.
B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113 109
Table 2
The values of volume r

i
and surface area q

i
parameters
Substance r

i
q

i
Benzene 3.1878 2.400
Carbon tetrachloride 3.3900 2.910
Cyclohexane 4.0464 3.240
n-Decane 7.1974 6.016
Ethylbenzene 4.5972 3.508
n-Hexane 4.4998 3.856
n-Heptane 5.1742 4.396
iso-Propylbenzene 5.2708 4.044
Methylbenzene 3.9228 2.968
Methylcyclohexane 4.7200 3.776
n-Octane 5.8486 4.936
n-Nonane 6.5230 5.476
Pyridine 2.9993 2.113
versions of UNIQUACequation with experimental data [8] was made. The excess enthalpy was calculated
by equation
H
E
= RT
2

(G
E
/T )
T

p,x
(4)
The excess Gibbs energy (G
E
) and the excess enthalpy H
E
were calculated using the UNIQUAC equa-
tion:
Table 3
The interaction parameters u
ij
in original UNIQUAC equation and in UNIQUAC equation with temperature dependent coordi-
nation number z obtained by data reduction at temperature T

System T

(K) UNIQUAC UNIQUAC with z = f(T)

u
12
u
21
u
12
u
21
Pyridine + n-heptane 353.15 873.9553 2531.1275 104.9565 324.2929
Pyridine + n-octane 353.15 969.6574 2626.7841 117.5503 335.9785
Pyridine + n-nonane 369.75 777.2268 2244.7073 96.8707 304.1915
Pyridine + n-decane 353.15 1104.7529 2822.1222 134.1502 357.3889
Pyridine + cyclohexane 298.15 509.7031 2417.1215 52.7525 249.7082
Pyridine + benzene 323.15 826.9825 1225.0167 93.7916 139.4815
Pyridine + methylbenzene 313.15 1134.4036 1987.1755 124.3020 218.1898
Cyclohexane + n-octane 298.15 134.1459 230.2397 11.2007 20.9408
Benzene + n-hexane 303.15 106.0332 573.4165 10.8132 60.5424
Benzene + n-heptane 333.15 105.5408 488.6144 11.3499 59.1902
Benzene + cyclohexane 333.15 274.1619 724.2459 31.9189 86.1642
Isopropylbenzene + n-heptane 313.15 17.6500 187.5485 32.7202 55.8501
Ethylbenzene + methylcyclohexane 313.15 825.1420 524.7298 92.1514 58.9320
Ethylbenzene + methylbenzene 298.15 285.7135 336.0915 28.1192 33.1345
Carbon tetrachloride + n-heptane 328.15 209.5097 27.1123 25.3117 3.8791
110 B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113
Fig. 5. Excess enthalpy, H
E
/(J mol
1
), for the binary mixture pyridine(1) + n-heptane(2) at 293.65 K [41]: experimental data
(); predicted fromVLE data at 353.15 Kusing: UNIQUACwith r, q = f (T T

) (continous line); UNIQUACwith z = f (T )

(dashed line); original UNIQUAC (dotted line).
Fig. 6. Excess enthalpy, H
E
(J mol
1
), for the binary mixture pyridine(1)+n-heptane(2) at 298.15 K[42]; experimental data ();
predicted from VLE data at 353.15 K using: UNIQUAC with r, q = f (T T

) (continous line); UNIQUAC with z = f (T )

(dashed line); original UNIQUAC (dotted line).
Fig. 7. Excess enthalpy, H
E
(J mol
1
), for the binary mixture pyridine(1) +n-octane(2) at 293.50 K [41]; experimental data ();
predicted from VLE data at 353.15 K using: UNIQUAC with r, q = f (T T

) (continous line); UNIQUAC with z = f (T )

(dashed line); original UNIQUAC (dotted line).
B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113 111
Fig. 8. Excess enthalpy, H
E
(J mol
1
), for the binary mixture pyridine(1) +n-octane(2) at 298.15 K [43]; experimental data ();
predicted from VLE data at 353.15 K using: UNIQUAC with r, q = f (T T

) (continous line); UNIQUAC with z = f (T )

(dashed line); original UNIQUAC (dotted line).
Fig. 9. Excess enthalpy, H
E
(J mol
1
), for the binary mixture pyridine(1) +n-nonane(2) at 293.50 K [41]; experimental data ();
predicted from VlE data at 369.75 K using: UNIQUAC with r, q = f (T T

) (continous line); UNIQUAC with z = f (T )

(dashed line); original UNIQUAC (dotted line).
Fig. 10. Excess enthalpy, H
E
(J mol
1
), for the binary mixture pyridine(1) + n-decane(2) at 293.50 K [41]; experimental data
(); predicted fromVLE data at 353.15 Kusing: UNIQUACwith r, q = f (T T

) (continous line); UNIQUACwith z = f (T )

(dashed line); original UNIQUAC (dotted line).
112 B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113
Fig. 11. Excess enthalpy, H
E
(J mol
1
), for the binary mixture pyridine(1) + n-decane(2) at 298.15 K [44]; experimental data
(); predicted fromVLE data at 353.15 Kusing: UNIQUACwith r, q = f (T T

) (continous line); UNIQUACwith z = f (T )

(dashed line); original UNIQUAC (dotted line).
1. with temperature dependent r
i
and q
i
parameters;
2. in the original version;
3. with temperature dependent coordination number z.
The results obtained are plotted in Figs. 511.
4. Conclusions
The calculations show that for binary mixtures formed by pyridine and aliphatic alkanes the proposed
temperature dependence of r
i
and q
i
in the UNIQUAC equation enables the prediction of VLE and H
E
at various temperatures based on data for one isotherm only. The accuracy of prediction of the VLE is
much higher than that obtained using the UNIFAC method or using the original UNIQUAC equation or
the UNIQUAC equation with the temperature dependant coordination number z and comparable with
those achieved by correlation of one particular isotherm using the UNIQUAC equation. The accuracy of
the prediction of the H
E
is acceptable. It is much higher than that obtained using the original UNIQUAC
equation or the UNIQUAC equation with the temperature dependant coordination number z.
For binary mixtures formed by pyridine and other hydrocarbons or formed by two hydrocarbons the
proposed temperature dependence of r
i
and q
i
in the UNIQUAC equation enables the prediction of VLE
at various temperatures based on experimental data for one isotherm only. Once more the accuracy is
much better than that obtained using other methods based on UNIQUAC equation.
The results of computation suggest, that values of a and b parameters can be the same for other, not
mentioned in this paper non-associating molecules. Example of the carbon tetrachloride + n-heptane
system conrms this conclusion. It is hard to proof for other molecules due to lack of temperature
dependent VLEdata for appropriate systems. The case of associating molecules situation is more complex,
crucial is the temperature dependence of association constant.
It can be concluded that the proposed method is superior to other methods if there is at least one
experimental isotherm for a binary mixture formed by pyridine and hydrocarbon or formed by two
hydrocarbons available.
B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113 113
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