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, ri and qi . The slope of ri and qi 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 (HE ) 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 ri and qi parameters enables prediction of the VLE at various temperatures and leads to reasonable values of HE . The necessary input reduces to one set of isothermal VLE data. One set of UNIQUAC interaction parameters uij is sufcient for representation of VLE in a wide range of temperature and to obtain a reasonable prediction of HE . 2001 Published by Elsevier Science B.V.
Keywords: Vaporliquid equilibria; Excess enthalpy; Activity coefcient; Correlation; Prediction

1. Introduction Knowledge of the vaporliquid equilibrium data (VLE) is necessary to design and optimize distillation, which is one of the most frequently used separation methods. To minimize design cost, tedious and expensive 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: S 0 3 7 8 - 3 8 1 2 ( 0 0 ) 0 0 5 1 4 - 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 uij which describe the energy of interaction between molecules i and j, for each binary pair. These parameters are temperature independent. Therefore, the set of uij 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 (uij ) 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, ri and qi 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 (HE ), and excess enthalpies calculated from the original UNIQUAC and the proposed modication 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 ri and the surface area qi parameters are linearly dependent on temperature while the interaction parameters uij remain constant. Reference values of ri and qi 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: ri = ri + a(T T ) qi = qi + b(T T )

(1) (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 ri and qi 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 ri and qi 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 uij 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) Prediction (UNIQUAC) r = f(T), q = f(T) Pyridine + n-heptane 298.15 303.15 313.15 313.15 323.15 333.15 340.95 348.15 353.15 313.15 348.15 353.15 369.75 313.15 348.15 369.75 353.15 373.55 293.15 298.15 303.15 303.15 308.15 308.15 313.15 318.15 318.15 328.15 338.15 348.15 298.15 303.15 313.15 323.15 293.15 298.15 303.15 308.15 313.15 323.15 333.15 373.15 3.978 3.466 2.144 2.777 2.148 1.735 0.538 2.841 2.373 4.263 0.442 1.106 3.487 1.929 0.882 0.788 1.141 1.038 0.860 0.965 1.385 1.094 1.355 1.683 2.106 0.295 0.247 0.218 0.578 0.660 0.539 0.527 0.413 0.284 0.609 z = f(T) 5.557 4.773 3.204 3.675 2.742 2.118 0.908 2.978 4.143 4.463 1.217 2.684 4.454 2.757 0.741 0.859 1.108 0.959 0.976 1.122 1.331 0.858 0.854 0.869 0.899 0.383 0.295 0.318 0.889 0.537 0.639 0.477 0.708 0.840 1.061 r,q,z = const. 8.970 7.956 6.276 6.297 4.727 3.411 2.043 3.301 6.966 4.790 2.456 8.863 6.173 4.443 0.735 1.321 1.173 1.459 1.962 2.678 2.492 2.403 3.339 4.257 5.075 0.308 0.255 0.320 0.704 0.493 0.587 0.475 0.727 0.930 1.702 Correlation UNIQUAC 1.000 0.950 0.277 0.843 0.861 0.680 0.361 1.287 0.254 0.297 1.056 0.221 0.404 0.241 1.465 0.365 0.592 1.640 0.628 1.191 0.516 1.181 1.081 0.458 0.405 1.018 0.978 0.917 0.858 0.828 0.118 0.126 0.078 0.412 0.548 0.492 0.504 0.464 0.363 0.173 0.134 0.019 Prediction UNIFAC 10.099 9.092 7.432 7.432 5.856 4.514 3.410 4.336 1.197 6.962 5.171 0.442 1.964 8.252 5.571 0.864 1.827 4.690 12.050 10.460 10.257 9.620 8.755 9.380 8.470 6.612 7.245 5.918 4.673 3.572 0.693 0.673 0.451 0.713 1.610 1.696 1.372 1.490 1.368 1.402 1.321 1.118 [9] [9] [10] [9] [9] [9] [11] [12] [11] [10] [12] [11] [11] [10] [12] [11] [11] [11] [13] [14] [13] [14] [14] [13] [13] [15] [14] [14] [14] [14] [16] [16] [16] [16] [13] [13] [13] [13] [13] [17] [17] [18] Reference

Pyridine + n-octane

Pyridine + n-nonane

Pyridine + n-decane Pyridine + cyclohexane

Pyridine + benzene

Pyridine + methylbenzene

106

B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113

Table 1 (Continued)
T (K) RMSD(P) Prediction (UNIQUAC) r = f(T), q = f(T) Cyclohexane + n-octane 298.15 308.15 318.15 328.15 298.15 298.15 303.15 307.91 312.94 313.15 323.15 328.25 333.15 343.15 293.15 318.15 333.15 348.15 353.15 283.15 311.65 313.15 328.15 333.15 343.15 343.15 343.15 351.95 403.15 413.15 423.15 313.15 333.15 353.15 313.15 333.15 353.15 373.15 298.15 373.15 298.15 308.15 318.15 328.15 0.509 0.209 0.276 2.486 0.294 0.125 0.131 0.213 0.191 0.750 0.270 0.927 1.394 0.607 0.492 0.269 0.819 0.259 0.272 0.626 0.203 0.223 1.064 0.393 0.551 0.815 1.196 0.474 0.577 1.032 1.185 0.856 0.236 0.444 0.476 0.320 z = f(T) 0.551 0.315 0.487 2.438 0.256 0.146 0.132 0.227 0.180 0.828 0.200 0.921 1.219 0.617 0.615 0.059 0.701 0.268 0.272 0.616 0.257 0.269 1.116 0.495 0.625 0.695 0.746 0.245 0.239 0.987 1.138 0.736 0.473 0.471 0.516 0.343 r,q,z = const. 0.689 0.594 0.892 2.697 0.547 0.234 0.550 0.505 0.976 0.680 1.536 2.709 3.269 1.292 1.090 0.689 2.467 0.889 0.908 0.505 0.570 0.565 1.419 0.946 2.167 2.359 2.511 0.618 0.815 1.257 1.656 1.717 0.599 1.108 0.934 0.488 Correlation UNIQUAC 0.480 0.247 0.159 0.154 0.383 0.106 0.245 0.114 0.113 0.216 0.179 0.266 0.166 0.218 0.492 0.382 0.123 0.418 0.058 0.220 0.201 0.171 0.308 0.082 0.023 0.140 0.445 0.026 0.130 0.083 0.086 0.417 0.140 0.101 0.866 0.782 0.809 0.048 0.787 0.072 0.349 0.218 0.292 0.117 Prediction UNIFAC 3.189 2.523 2.367 1.948 3.703 1.778 1.096 1.026 0.686 0.627 0.188 0.635 0.552 1.658 2.482 0.563 0.740 1.766 1.549 2.471 0.982 0.959 0.404 0.163 0.438 0.434 1.268 0.828 2.315 2.558 2.767 1.684 0.825 0.497 1.177 0.921 1.039 0.682 0.858 0.070 3.474 3.124 2.446 1.914 [19] [19] [19] [19] [20] [21] [22] [21] [21] [22] [22] [23] [22] [24] [25] [26] [27] [28] [29] [30] [31] [32] [31] [30] [33] [34] [24] [35] [36] [36] [36] [37] [37] [37] [37] [37] [37] [38] [39] [38] [40] [40] [40] [40] Reference

Benzene + n-hexane

Benzene + n-heptane

Benzene + cyclohexane

Isopropylbenzene + n-heptane

Ethylbenzene + methylcyclohexane

Ethylbenzene + methylbenzene Carbon tetrachloride + n-heptane

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 UNIQUAC equation: 1. 2. 3. 4. The proposed modication with temperature dependent ri and qi . The original equation with uij obtained in version 1. and ri and qi independent of temperature. The UNIQUAC equation with temperature dependent coordination number z. 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 1 RMSD(P ) = 100 N
exp. N i =1

Pi

exp.

Pi

Pical.
exp.

2 1/2

(3)

where Pi is the experimental vapor pressure, Pical. 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 ri and qi used in the UNIQUAC equation are shown in Table 2. The values of the interaction parameters uij 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 (HE ) 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 HE 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 Table 2 The values of volume ri and surface area qi parameters Substance Benzene Carbon tetrachloride Cyclohexane n-Decane Ethylbenzene n-Hexane n-Heptane iso-Propylbenzene Methylbenzene Methylcyclohexane n-Octane n-Nonane Pyridine ri 3.1878 3.3900 4.0464 7.1974 4.5972 4.4998 5.1742 5.2708 3.9228 4.7200 5.8486 6.5230 2.9993

109

qi 2.400 2.910 3.240 6.016 3.508 3.856 4.396 4.044 2.968 3.776 4.936 5.476 2.113

versions of UNIQUAC equation with experimental data [8] was made. The excess enthalpy was calculated by equation H E = RT2 (GE /T ) T (4)
p,x

The excess Gibbs energy (GE ) and the excess enthalpy HE were calculated using the UNIQUAC equation:
Table 3 The interaction parameters uij in original UNIQUAC equation and in UNIQUAC equation with temperature dependent coordination number z obtained by data reduction at temperature T System T (K) UNIQUAC u12 Pyridine + n-heptane Pyridine + n-octane Pyridine + n-nonane Pyridine + n-decane Pyridine + cyclohexane Pyridine + benzene Pyridine + methylbenzene Cyclohexane + n-octane Benzene + n-hexane Benzene + n-heptane Benzene + cyclohexane Isopropylbenzene + n-heptane Ethylbenzene + methylcyclohexane Ethylbenzene + methylbenzene Carbon tetrachloride + n-heptane 353.15 353.15 369.75 353.15 298.15 323.15 313.15 298.15 303.15 333.15 333.15 313.15 313.15 298.15 328.15 873.9553 969.6574 777.2268 1104.7529 509.7031 826.9825 1134.4036 134.1459 106.0332 105.5408 274.1619 17.6500 825.1420 285.7135 209.5097 u21 2531.1275 2626.7841 2244.7073 2822.1222 2417.1215 1225.0167 1987.1755 230.2397 573.4165 488.6144 724.2459 187.5485 524.7298 336.0915 27.1123 UNIQUAC with z = f(T) u12 104.9565 117.5503 96.8707 134.1502 52.7525 93.7916 124.3020 11.2007 10.8132 11.3499 31.9189 32.7202 92.1514 28.1192 25.3117 u21 324.2929 335.9785 304.1915 357.3889 249.7082 139.4815 218.1898 20.9408 60.5424 59.1902 86.1642 55.8501 58.9320 33.1345 3.8791

110

B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113

Fig. 5. Excess enthalpy, HE /(J mol1 ), for the binary mixture pyridine(1) + n-heptane(2) at 293.65 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).

Fig. 6. Excess enthalpy, HE (J mol1 ), 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, HE (J mol1 ), 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, HE (J mol1 ), 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, HE (J mol1 ), 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, HE (J mol1 ), for the binary mixture pyridine(1) + n-decane(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).

112

B. Wi sniewska-Gocowska, S.K. Malanowski / Fluid Phase Equilibria 180 (2001) 103113

Fig. 11. Excess enthalpy, HE (J mol1 ), for the binary mixture pyridine(1) + n-decane(2) at 298.15 K [44]; 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).

1. with temperature dependent ri and qi 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 ri and qi in the UNIQUAC equation enables the prediction of VLE and HE 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 HE 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 ri and qi 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 VLE data 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

References
[1] [2] [3] [4] [5] [6] [7] [8] [9] [10] [11] [12] [13] [14] [15] [16] [17] [18] [19] [20] [21] [22] [23] [24] [25] [26] [27] [28] [29] [30] [31] [32] [33] [34] [35] [36] [37] [38] [39] [40] [41] [42] [43] [44] D.S. Abrams, J.M. Prausnitz, AIChE J. 21 (1975) 116128. I. Nagata, T. Ohta, Chem. Eng. Sci. 33 (1978) 177182. S. Skjold-Jorgensen, P. Rasmussen, A. Fredenslund, Chem. Eng. Sci. 35 (1980) 23892403. A. M aczy nski, A. Skrzecz, Z. M aczy nska, Floppy Book on Binary VPE Thermodynamics Data Center, Warsaw, 2000. A. Fredenslund, J. Gmehling, P. Rasmussen, VapourLiquid Equilibria Using UNIFAC, Elsevier, Amsterdam, 1977. T. Magnussen, Report MAN 8101, Instituttet for Kemiteknik Danmarks Tekniske Hojskole DK 2800, Lyngby, Denmark. C. Tsonopoulos, AICHE J. 20 (1974) 263272. A. Skrzecz, A. M aczy nski, I. Tomaszkiewicz, Floppy Book on Heats of Mixing, Warsaw, 1995. M.A. Michou-Saucet, J. Jose, C. Michou-Saucet, Int. DATA Ser., Sel. Data Mixtures, Ser. A (2) (1986) 143. S.J. Warycha, Chem. Eng. Data 38 (1993) 274. Z. M aczy nska, K. Zi eborak, Bull. Acad. Polon. Sci., Ser. Sci. Chim. 11 (1963) 225229. T. Kasprzycka-Guttman, I. Chojnacka, J. Chem. Thermodyn. 21 (1989) 721725. E.G. Konakbaeva, Z.Kh. Anisimova, M.I. Shakhparonov, Vestn. Mosk. Univ., Khim. 15 (1) (1974) 3036. J. W ecawski, Fluid Phase Equilibr. 12 (1/2) (1983) 155174. D. Bares, M. Soulie, J. Metzger, J. Chim. Phys. Physicochim. Biol. 70 (1973) 15311539. J. Jose, C. Michou-Saucet, M.A. Michou-Saucet, Int. DATA Ser., Sel. Data Mixtures, Ser. A (1) (1988) 37. J. Jose, C. Michou-Saucet, M.A. Michou-Saucet, Int. DATA Ser., Sel. Data Mixtures, Ser. A (1) (1988) 40. M. Rogalski, A. Bylicki, J. Chem. Thermodyn. 17 (1985) 915919. D.V.S. Jain, O.P. Yadav, Indian J. Chem. 9 (1971) 342342. V.C. Smith, R.L. Robinson, J. Chem. Eng. Data 15 (3) (1970) 391395. D.V.S. Jain, V.K. Gupta, B.S. Lark, Indian J. Chem. 8 (1970) 815820. I.P.C. Li, Y.W. Wong, S.D. Chang, B.C.Y. Lu, J. Chem. Eng. Data 17 (4) (1972) 492498. J.C.K. Ho, B.C.Y. Lu, J. Chem. Eng. Data 8 (1963) 553558. M.P. Susarev, S.-T. Chen, Zh. Fiz. Khim. 37 (8) (1963) 17391744. G. Werner, H. Schuberth, J. Prakt. Chem. 31 (5/6) (1966) 225239. D.A. Palmer, B.D. Smith, J. Chem. Eng. Data 17 (1) (1972) 7176. D.O. Hanson, M. Van Winkle, J. Chem. Eng. Data 12 (1967) 319325. S.J. Fu, B.C.Y. Lu, J. Appl. Chem. 16 (1966) 324326. I. Brown, A.H. Ewald, Aus. J. Sci. Res. A4 (1951) 198212. T. Boublik, Coll. Czech. Chem. Commun. 28 (1963) 17711779. A.G. Morachevskii, E.G. Komarowa, Vestnik Leningrad. Univ. 12, No. 4, Ser. Fiz.iv Khim. 1 (1957) 118126. K.L. Young, R.A. Mentzer, R.A. Greenkorn, J. Chem. Thermodyn. 9 (1977) 979985. G. Scatchard, S.E. Wood, J.M. Mochel, J. Phys. Chem. 43 (1939) 119130. M. Diaz Pena, D. Rodriguez Cheda, Annu. Quim. 66 (1970) 721735. H.A. Beatty, G. Calingaret, Idn. Eng. Chem. 26 (1934) 504508. B. Wi sniewska, J. Gregorowicz, S. Malanowski, Fluid Phase Equilibr. 86 (1993) 173186. E.W. Funk, F.C. Chai, J.M. Prausnitz, J. Chem. Eng. Data 17 (1) (1972) 2427. B. Wi sniewska, J. Chem. Thermodyn. 19 (1987) 897901. H. Arm, F. Huegli, R. Signer, Helv. Chim. Acta 40 (1957) 12001205. D.V.S. Jain, V.K. Gupta, B.S. Lark, Indian J. Chem. 9 (5) (1971) 465468. M. Woycicka, Pure Appl. Chem. 2 (1961) 147153. R. Kechavarz, J.P. Dubes, H. Tachoire, Int. Data Ser., Sel. Data Mixtures, Ser. A 1 (1992) 12. R. Kechavarz, J.P. Dubes, H. Tachoire, Int. Data Ser., Sel. Data Mixtures, Ser. A 1 (1992) 13. R. Kechavarz, J.P. Dubes, H. Tachoire, Int. Data Ser., Sel. Data Mixtures, Ser. A 1 (1992) 14.