Fluid Phase Equilibria 154 Ž1999.

99–108

Phase equilibria in the ternary system hexane q ethyl

1,1-dimethylethyl ether q heptane
a, )
Ricardo Reich , Marcela Cartes a , Jaime Wisniak b , Hugo Segura a

a
´ Quımica,
Departamento de Ingenierıa ´ ´ P.O.B. 53-C, Concepcion,
UniÕersidad de Concepcion, ´ Chile
b
Department of Chemical Engineering, Ben-Gurion UniÕersity of the NegeÕ, Beer-SheÕa, 84105, Israel
Received 9 March 1998; accepted 19 August 1998

Abstract

Consistent vapor–liquid equilibrium data at 94 kPa have been determined for the ternary system hexaneq
ethyl 1,1-dimethylethyl ether q heptane. The results indicate that the system deviates positively from ideality
and that no azeotrope is present. The ternary system were predicted with the composition by the Redlich–Kister,
Wilson, NRTL, UNIQUAC and UNIFAC models using only the parameters of the constituent binaries. Most of
the models allow a very good prediction of the phase equilibrium of the ternary system. In addition, the
Wisniak–Tamir relations were used for correlating bubble-point temperatures. q 1999 Elsevier Science B.V. All
rights reserved.

Keywords: Vapor–liquid equilibrium; Fuel oxygenating additives; Unleaded gasoline; Ethers; ETBE

1. Introduction

Amendments to the US Clean Air in 1990 has mandated that new gasoline formulations be sold in
highly polluted areas of the country, with oxygenated gasolines being supplied particularly during the
winter. Most of the oxygenates used in gasolines are alcohols or ethers that contain 1 to 6 carbons.
These regulations have caused oxygenates like methyl 1,1-dimethylethyl ether Ž MTBE. and ethanol to
play a significant role as octane improvers. MTBE has been used as a gasoline blending agent since
1979, although other oxygenates like ethyl 1,1-dimethylethyl ether Ž ETBE. and methyl 1,1-dimethyl-
propyl ether ŽTAME. are also being considered and used in lesser amounts. ETBE has some
important advantages over MTBE, for example, it is chemically more similar to hydrocarbons and has
a lower solubility in water. The higher boiling point of ETBE allows incorporation of more light
feedstocks in gasoline. In addition, ETBE has a Reid vapor pressure Ž Rvp. of 27.6 kPa, one half of

)
Corresponding author. E-mail: rreich@udec.cl

0378-3812r99r$ - see front matter q 1999 Elsevier Science B.V. All rights reserved.
PII: S 0 3 7 8 - 3 8 1 2 Ž 9 8 . 0 0 4 2 0 - 8
100 R. Reich et al.r Fluid Phase Equilibria 154 (1999) 99–108

that of MTBE, making it an attractive oxygenate for gasolines having a low vapor pressure. Phase
equilibrium data of oxygenated mixtures are important for predicting the vapor phase composition that
would be in equilibrium with hydrocarbon mixtures.
Vapor–liquid equilibrium data of ETBE in mixture with alkanes are scarce, limiting activity
coefficients g i` for ETBE with hexane at 333.15 K and for ETBE with heptane at 348.15 K have
been measured by Delcros et al. w1x, using the comparative ebulliometry technique. According to their
results, the systems under consideration deviate slightly from ideal behavior, when concentrated in
alkane, yielding g i` in the range 1.10–1.11. Delcros et al. showed that their results were in very good
agreement with those predicted by the DISQUAC w2,3x and the UNIFAC Dortmund group contribu-
tion methods w4x. Reich et al. w5x have recently measured the VLE of the systems hexaneq ETBE and
ETBEq heptane and concluded that the behavior of the liquid phase can be represented by a
symmetric or Porter model w6x. Isobaric vapor–liquid data for the system hexaneq heptane have been
reported in Ref. w7x at 12, 20, 31, 47, 70, 101, and 101.3 kPa and more recently by Wisniak et al. w8x
at 94 kPa. The later set will be used in the analysis of the ternary data reported in this work.
The present work was undertaken to measure vapor–liquid equilibrium ŽVLE. data for the title
system at 94 kPa, for which isobaric data are not available. It is part of our experimental program to
determine the phase equilibria of oxygenates and main gasoline components w8–11x.

2. Experimental section
2.1. Chemicals
Ethyl 1,1-dimethylethyl ether Ž 96.0 q mass%. was purchased from TCI ŽJapan. and was further
purified to 99.9 q mass% by distillation in a 1-m high = 30 mm diameter Normschliffgeratebau ¨
adiabatic column Žpacked with 3 = 3 mm SS spirals. working at a 1:100 reflux ratio. Hexane
Ž99.73 q mass%. and heptane Ž 99.57 mass%. were purchased from Aldrich and used without further
purification, after gas chromatography failed to show any significant impurities. The properties and
purity Ž as determined by GLC. of the pure components appear in Table 1. Appropriate precautions
were taken when handling ETBE in order to avoid peroxide formation.
Table 1
Mole % GLC purities Žmass %., refractive index n D at Na D line, and normal boiling points T of pure components
Components Žpurityrmass %. n D Ž298.15. T ŽK.
a
Hexane Ž99.73. 1.3730 341.84 a
1.37226 b 341.89 c
Ethyl 1,1-dimethylethyl ether Ž99.9q. 1.3730 a 345.85a
1.3729 d 345.86 e
Heptane Ž99.57. 1.3851a 371.54 a
1.38511f 371.57 g
a
Measured.
b
TRC Tables, fa-1010 w20x.
c
TRC Tables, k1440 w20x.
d
DIPPR w21x.
e
¨ ¨ and Gmehling w22x.
Krahenbuhl
f
TRC Tables, fa-1460 w20x.
g
TRC Tables, k1460 w20x.
 R. Reich et al.r Fluid Phase Equilibria 154 (1999) 99–108 101

2.2. Apparatus and procedure

An all glass Fischer LABODEST vapor–liquid-equilibrium apparatus, model 601 was used in the
equilibrium determinations. In this circulation method apparatus, the solution is heated to its boiling
point by a 250 W immersion heater ŽCottrell pump. . The vapor–liquid mixture flows through an
extended contact line which guarantees an intense phase exchange and then enters a separation
chamber whose construction prevents an entrainment of liquid particles into the vapor phase. The
separated gas and liquid phases are condensed and returned to a mixing chamber, where they are
stirred by a magnetic stirrer, and returned again to the immersion heater. The temperature in the VLE
still has been determined with a Systemteknik S1224 digital temperature meter and a Pt100 V probe
calibrated at the Swedish Statens Provningsanstalt with the IPTS-68 temperature scale. The accuracy
is estimated as "0.02 K. The total pressure of the system is controlled by a vacuum pump capable to
work under vacuum up to 0.25 kPa. The pressure is measured with a Fischer pressure transducer
calibrated against an absolute mercury-in-glass manometer Ž22 mm diameter precision tubing with
cathetometer reading. , the overall accuracy is estimated as "0.02 kPa. On the average the system
reached equilibrium conditions after 1–2 h operation. Samples, taken by syringing 1.0 ml over the
system had achieved equilibrium, were analyzed by gas chromatography on a Varian 3400 apparatus
provided with a thermal conductivity detector and a Tsp model SP4400 electronic integrator. The
column was 3 m long and 0.3 cm in diameter, packed with SE-30. Column, injector and detector
temperatures were 323.15, 353.15, 473.15 K, respectively. Very good separation was achieved under
these conditions, and calibration analyses using synthetic mixtures were carried out to convert the
peak ratio to the mass composition of the sample. The pertinent polynomial fits had a correlation
coefficient R 2 better than 0.99. At least three analyses were made of each composition. Concentration
measurements were accurate to better than "0.001 mole fraction.

3. Results and discussions

The temperature T and liquid-phase x i , and vapor-phase yi mole fraction measurements at P s 94

kPa are reported in Table 2, together with the activity coefficients g i which were calculated from the
following equation w12x:

Ž1.

where P is the total pressure, Pi0 is the pure component vapor pressure. The standard state for
calculation of activity coefficients is the pure component at the pressure and temperature of the
solution. The non-idealities of the vapor phase were not considered because the pressure is low and
vapor phase can be considered ideal. In addition, as pointed out by Reich et al. w5x, the estimation of
second virial coefficients of ETBE in mixtures with hydrocarbons is not reliable. The pure component
vapor pressure Pi0 were calculated according to the Antoine equation:
Bi
log Ž Pi0rkPa . s A i y Ž2.
Ž TrK . y Ci
102 R. Reich et al.r Fluid Phase Equilibria 154 (1999) 99–108

Table 2
Experimental vapor–liquid equilibria data for hexane Ž1.qethyl 1,1-dimethylethyl ether Ž2.qheptane Ž3. at 94 kPa
T ŽK. x1 x2 y1 y2 g1 g2 g3
340.76 0.894 0.048 0.922 0.053 0.991 1.205 1.089
342.05 0.682 0.203 0.753 0.201 1.019 1.036 0.965
342.30 0.591 0.294 0.641 0.311 0.993 1.098 0.998
342.64 0.483 0.399 0.549 0.400 1.030 1.030 1.021
342.92 0.391 0.494 0.453 0.495 1.041 1.020 1.058
343.26 0.144 0.795 0.178 0.793 1.099 1.004 1.099
343.30 0.287 0.602 0.341 0.608 1.055 1.015 1.060
343.71 0.198 0.693 0.242 0.707 1.071 1.012 1.064
344.02 0.707 0.093 0.806 0.101 0.990 1.067 1.046
344.31 0.589 0.194 0.688 0.217 1.005 1.089 0.975
344.36 0.104 0.786 0.132 0.814 1.090 1.007 1.091
344.42 0.494 0.296 0.575 0.334 0.998 1.095 0.961
344.42 0.081 0.818 0.102 0.848 1.080 1.006 1.098
345.00 0.384 0.394 0.469 0.429 1.029 1.037 0.999
345.20 0.297 0.489 0.369 0.530 1.040 1.026 1.019
345.51 0.195 0.597 0.248 0.651 1.054 1.022 1.037
345.65 0.668 0.057 0.795 0.073 0.983 1.195 1.020
345.80 0.111 0.694 0.144 0.759 1.066 1.016 1.051
346.43 0.589 0.106 0.731 0.119 1.000 1.023 1.017
346.71 0.481 0.205 0.603 0.247 1.002 1.088 0.978
346.78 0.402 0.290 0.497 0.355 0.986 1.103 0.982
346.89 0.476 0.208 0.605 0.236 1.010 1.019 1.024
347.28 0.207 0.496 0.274 0.575 1.040 1.028 1.021
347.39 0.293 0.389 0.385 0.455 1.029 1.034 1.007
347.78 0.110 0.588 0.150 0.695 1.055 1.032 1.013
348.86 0.520 0.087 0.656 0.129 0.945 1.253 1.041
349.23 0.307 0.289 0.418 0.370 1.009 1.069 0.986
349.52 0.386 0.202 0.518 0.254 0.986 1.041 1.029
349.74 0.115 0.490 0.164 0.620 1.041 1.041 1.010
349.90 0.202 0.380 0.287 0.484 1.032 1.042 1.006
350.82 0.478 0.056 0.646 0.085 0.955 1.208 1.028
350.84 0.476 0.060 0.641 0.089 0.951 1.180 1.035
351.63 0.430 0.089 0.568 0.138 0.911 1.204 1.059
352.12 0.210 0.280 0.316 0.386 1.024 1.055 0.996
352.33 0.280 0.196 0.417 0.271 1.007 1.051 1.008
354.51 0.319 0.094 0.468 0.148 0.931 1.122 1.030
354.82 0.120 0.281 0.193 0.421 1.011 1.058 1.004
355.05 0.197 0.201 0.304 0.296 0.964 1.033 1.028
356.25 0.287 0.060 0.452 0.107 0.951 1.207 1.005
357.48 0.217 0.107 0.347 0.164 0.932 1.001 1.034
357.94 0.103 0.191 0.180 0.316 1.006 1.066 1.006
360.86 0.111 0.102 0.202 0.178 0.965 1.035 1.012
362.47 0.098 0.070 0.182 0.128 0.942 1.036 1.013

where the Antoine constants A i , Bi , and Ci are reported in Table 3. The ternary activity coefficients
reported in Table 2 are estimated accurate to within 3% and were found to be thermodynamically
consistent as tested by the McDermott–Ellis method w13x modified by Wisniak and Tamir w14x.
 R. Reich et al.r Fluid Phase Equilibria 154 (1999) 99–108 103

Table 3
Antoine coefficients, Eq. Ž2.
Compound Ai Bi Ci
a
Hexane 6.00091 1171.170 48.740
Ethyl 1,1-dimethylethyl ether b 5.96651 1151.728 55.062
Heptane c 6.02167 1264.900 56.610
a
TRC Tables, k1440 w20x.
b
Reich et al. w5x.
c
TRC Tables, k1460 w20x.

According to these references two experimental points a and b are considered thermodynamically
consistent if the following condition is fulfilled:

D - Dmax Ž3.
where the local deviation D is given by
N
Ds Ý Ž x i a q x i b .Žln g i a y ln g i b . Ž4.
is1

and N is the number of components. The maximum deviation Dmax is given by:
N 1 1 1 1 N DP
Dmax s Ý Ž xia q xib .
is1
ž xia
q
yi a
q
xib
q
yi b / Dxq Ý Ž xia q xib .
is1 P
N N
y2 y2
q 2 Ý ln g i b y ln g i a D x q Ý Ž x i a q x i b . Bj ½ Ž Ta q C j . q Ž Tb q C j . 5 DT Ž5.
is1 is1

The errors in the measurements D x, D P and DT were as previously indicated. The first term in
Eq. Ž 5. was the dominant one. For the experimental points reported here D never exceeded 0.021
while the smallest value of Dmax was 0.024.
The activity coefficients for the ternary system were correlated from the following Redlich–Kister
expansion w15x:

GE 2 2
s x 1 x 2 b 12 q c12 Ž x 1 y x 2 . q d12 Ž x 1 y x 2 . q x 1 x 3 b 13 q c13 Ž x 1 y x 3 . q d13 Ž x 1 y x 3 .
RT
2
q x 2 x 3 b 23 q c 23 Ž x 2 y x 3 . q d 23 Ž x 2 y x 3 . q x 1 x 2 x 3 Ž C q D 1 x 1 q D 2 x 2 . Ž6.
where bi j , c i j and d i j are the parameters of the pertinent ij binary, and C, D 1 , and D 2 are ternary
parameters. All the parameters in Eq. Ž6. are assumed to be independent of the temperature, and have
been obtained by fitting binary and ternary activity coefficient data. The parameters for the two
binaries hexane Ž 1. q ETBE Ž2. and ETBE Ž 2. q heptane Ž 3. , were calculated from the data in Ref.
w5x, and the corresponding parameters of the system hexane Ž1. q heptane Ž3. were calculated from
104 R. Reich et al.r Fluid Phase Equilibria 154 (1999) 99–108

Table 4
Constants for the Redlich-Kister model, Eq. Ž6.
A. BINARIES
System bi j =10 2 c i j =10 2 d i j =10 2 Fit of activity coefficients
rmsd a %dev b max %dev c
Hexane Ž1.qETBE Ž2. d 12.53 0.00 0.00 0.008 0.6 1.8
Hexane Ž1.qheptane Ž3. e 2.31 0.16 y0.41 0.005 1.7 3.1
ETBE Ž2.qheptane Ž3. a 13.43 0.00 0.00 0.010 0.8 2.3

B. TERNARY SYSTEM
System C, D 1, D 2 Bubble-point pressures Dew-point pressures
f
D P r% D y 1g D y2 D Pr% D x1 D x2
Hexane Ž1.qETBE Ž2.qheptane Ž3. 0.00 0.93 0.007 0.006 0.58 0.007 0.006
a
Root mean square deviation,  SŽgexpt ygcalc . 2 r N 40.5.
b
Percent average deviation in activity coefficients.
c
Maximum percent deviation in activity coefficients.
d
Calculated from the data of Reich et al. w5x.
e
Calculated from the data of Wisniak et al. w8x.
f
Average percentual deviation in bubble pressure, D P s100rN S iN < Piexpt y Picalc <r Piexpt Ž N: number of data points..
g
Average absolute deviation in mole fraction D y s1r N SiN < yiexpt y yicalc <.

Table 5
Parameters and ternary system prediction statistics from binary parameters for different G E models
Model ij A i j rJ moly1 A ji rJ moly1 ai j System Bubble-point pressures Dew-point pressures
DPf D y 1g D y2 DP D x1 D x2
Ž%. =10 2 =10 2 Ž%. =10 2 =10 2
a
Wilson 1–2 d 33.11 371.25 1q2 0.28 0.2 0.2 0.29 0.2 0.2
1–3 e 45.79 23.01 1q3 0.43 0.3 – 0.67 0.3 –
2–3 d y594.04 1266.91 2q3 0.38 – 0.2 0.42 – 0.3
1q2q3 0.88 0.8 0.6 0.53 0.8 0.5
NRTL 1–2 d 275.14 79.86 0.3 1q2 0.12 0.2 0.2 0.12 0.2 0.2
1–3 e y8.53 66.71 0.3 1q3 0.43 0.3 – 0.66 0.3 –
2–3 d 776.74 y331.17 0.3 2q3 0.29 – 0.2 0.38 – 0.2
1q2q3 0.92 0.8 0.6 0.63 0.8 0.5
b
UNIQUAC 1–2 d y744.49 972.11 1q2 0.20 0.3 0.3 0.20 0.3 0.3
1–3 e y744.75 859.98 1q3 0.72 0.2 – 0.95 0.3 –
2–3 d 646.86 y489.27 2q3 0.25 – 0.3 0.40 – 0.4
1q2q3 0.68 0.8 0.7 0.37 0.8 0.6
c
UNIFAC 1q2q3 3.83 1.1 1.5 3.06 0.9 1.4
a
Liquid volumes have been estimated from the Rackett equation w23x.
b
Molecular parameters are those calculated from UNIFAC w16,17x
c
Calculations based on original UNIFAC w17x.
d
Data of Reich et al. w5x.
e
Data of Wisniak et al. w8x.
f
Average percent deviations in bubble pressure D P s100rN S iN < Piexpt y Picalc <r Piexpt Ž N: number of data points..
g
Average absolute deviation in mole fraction D y s1r N S iN < yiexpt y yicalc <.
 R. Reich et al.r Fluid Phase Equilibria 154 (1999) 99–108 105

Fig. 1. Isothermals for the ternary system hexane Ž1.qethyl 1,1-dimethylethyl ether Ž2.qheptane Ž3. at 94 kPa from 340 K
to 370 K, every 3 K. Coefficients from Eq. Ž8..

Ref. w8x. The coefficients C, D 1, and D 2 were obtained by correlating activity coefficients of the
present ternary system, and were found to be negligible and statistically not significant, suggesting
that the VLE ternary data can be predicted directly from the parameters of the binary systems as

Fig. 2. Three-dimensional graph T y x 1 y x 2 .

106 R. Reich et al.r Fluid Phase Equilibria 154 (1999) 99–108

shown in Table 4. The prediction of the ternary system from binary parameters was also confirmed
using other activity coefficient models, as shown by the statistics and the models with its respective
parameters given in Table 5. As it can be seen in the Table in question, equilibrium vapor pressures
and mole fractions of the ternary system were fairly predicted by the NRTL, Wilson and UNIQUAC
models Žwhose binary parameters were calculated from the data in Ref. w5,8x., both for bubble and
dew point-pressure calculations. In addition, Table 5 shows the results of the group contribution
UNIFAC model w16,17x, which yields somewhat less accurate predictions. It can be thus concluded
that the binary data allow a good prediction of the ternary system.
The boiling points of the systems were correlated by the equation proposed by Wisniak and Tamir
w18x:
n n m
k
TrK s
is1
0
Ý x iTi rK q Ý
i , js1
½ xi x j Ý Ck Ž x i y x j .
ks0
5
q x1 x 2 x 3 A q B Ž x1 y x 2 . q C Ž x1 y x 3 . q D Ž x 2 y x 3 . 4 Ž7.
In this equation n is the number of components Ž n s 2 or 3. , Ti0 is the boiling point of the pure
component i and m is the number of terms considered in the series expansion of Ž x i y x j .. Ck are the
binary constants where A, B, C, and D are ternary constants. The following equation, of the same

Table 6
Coefficients in correlation of boiling points, Eqs. Ž7. and Ž8., average deviation and root mean square deviations in
temperature, rmsd ŽT rK.
A B C D Max devrK a Avr devrK b Rmsd c
A. Eq. (7) (fit from binary constants)
20.900 57.790 y46.285 0.000 0.84 0.31 0.06

Binary constants
System C0 C1 C2 Max devrK a
Hexane Ž1.qETBE Ž2. d y3.8523 0.9660 y1.0502 0.05
Hexane Ž1.qheptane Ž3. y11.2715 2.9701 y10.7795 0.06
ETBE Ž2.qheptane Ž3. a y13.4115 5.7282 y2.9370 0.21

B. Eq. (8) (direct fit)

ij Ai j Bi j Ci j Max devrK a Avr devrK b rmsd c
1–2 y4.0439 0.6840 y0.2199
1–3 y9.1895 y0.5021 y0.7398 0.33 0.08 0.11
2–3 y14.4493 4.8621 0.2645
a
Maximum deviation.
b
Average deviation.
c
rmsd ŽT rK.: Root mean square deviation,  SŽTexpt yTcalc . 2 r N 40.5.
d
Calculated from the data of Reich et al. w5x.
e
Calculated from the data of Wisniak et al. w5x.
 R. Reich et al.r Fluid Phase Equilibria 154 (1999) 99–108 107

structure, has been suggested by Tamir w19x for the direct correlation of ternary data, without use of
binary data:
3
2
TrK s Ý x iTi0 q x 1 x 2 A12 q B12 Ž x 1 y x 2 . q C12 Ž x 1 y x 2 . q . . .
is1
2
q x 1 x 3 A13 q B13 Ž x 1 y x 3 . q C13 Ž x 1 y x 3 . q . . .
2
q x 2 x 3 A 23 q B23 Ž x 2 y x 3 . q C23 Ž x 2 y x 3 . q . . . Ž8.
In Eq. Ž8. coefficients A i j , Bi j , and Ci j are not binary constants, they are multicomponent
parameters determined directly from the data. Direct correlation of T Ž x . for ternary mixtures can be
very efficient as reflected by a lower % average deviation and root mean square deviation Žrmsd. and
a smaller number of parameters than those for Eq. Ž 7. . Both equations may require similar number of
constants for similar accuracy, but the direct correlation allows an easier calculation of boiling
isotherms ŽFigs. 1 and 2.. The various constants of Eqs. Ž 7. and Ž 8. are reported in Table 6, which
also contains information indicating the degree of goodness of the correlation. It is clear that for the
ternary system in question, a direct fit of the data gives a much better fit.

4. List of symbols

P pressure wkPax
Pi0 vapor pressure of pure component i wkPax
T temperature wKx
Ti0 boiling point of pure component i wKx
x i , yi mole fraction of component i in the liquid and vapor phase respectively
gi activity coefficient of component i

Acknowledgements

This work was financed by FONDECYT, Chile, project No. 1960583. Graciela Galindo helped in
the experimental part.

References

w1x Delcros, J.-P.E. Grolier, V. Dohnal, D. Fenclov, Chem. Eng. Sci. 50 Ž1995. 2957–2962.
w2x H.V. Kehiaian, Fluid Phase Equilibria 13 Ž1983. 243–252.
w3x H.V. Kehiaian, Pure Appl. Chem. 57 Ž1985. 15–30.
w4x U. Weidlich, J. Gmehling, Ind. Eng. Chem. Res. 26 Ž1987. 1372–1381.
w5x R. Reich, M. Cartes, H. Segura, J. Wisniak, Phys. Chem. Liq., submitted, 1998.
w6x I. Prigogine, The Molecular Theory of Solutions. North-Holland, Amsterdam Pub., 1957.
w7x E.H. Leslie, A.R. Carr, Ind. Eng. Chem. 17 Ž1925. 810–818.
w8x J. Wisniak, E. Magen, M. Shachar, I. Zeroni, R. Reich, H. Segura, J. Chem. Eng. Data 42 Ž1997. 458–462.
108 R. Reich et al.r Fluid Phase Equilibria 154 (1999) 99–108

w9x J. Wisniak, G. Embon, R. Shafir, H. Segura, R. Reich, J. Chem. Eng. Data 42 Ž1997. 1191–1194.
w10x J. Wisniak, E. Magen, M. Shachar, I. Zeroni, R. Reich, H. Segura, J. Chem. Eng. Data 42 Ž1997. 243–247.
w11x R. Reich, M. Cartes, J. Wisniak, H. Segura, J. Chem. Eng. Data 43 Ž1998. 299–303.
w12x H.C. Van Ness, M.M. Abbott, Classical Thermodynamics of Nonelectrolyte Solutions, McGraw-Hill Book, New York,
1982.
w13x C. McDermott, S.R.M. Ellis, Chem. Eng. Sci. 20 Ž1965. 293–296.
w14x J. Wisniak, A. Tamir, J. Chem. Eng. Data 22 Ž1977. 253–260.
w15x O. Redlich, A.T. Kister, Ind. Eng. Chem. 40 Ž1948. 345–348.
w16x Aa. Fredenslund, J. Gmehling, P. Rasmussen, Vapor–Liquid Equilibria Using UNIFAC, Elsevier, Amsterdam, 1977.
w17x H.K. Hansen, P. Rasmussen, Aa. Fredenslund, M. Schiller, J. Gmehling, Ind. Eng. Chem. Res. 30 Ž1991. 2355–2358.
w18x J. Wisniak, A. Tamir, Chem. Eng. Sci. 31 Ž1976. 631–635.
w19x A. Tamir, Chem. Eng. Sci. 36 Ž1981. 1453–1465.
w20x TRC-Thermodynamic Tables—Hydrocarbons, fa-1010, 1994; fa-1460, 1991; k-1440, 1994; k-1460, 1991: Thermody-
namics Research Center, The Texas A&M University System, College Station, TX, extant 1996.
w21x T.E. Daubert, R.P. Danner, Physical and Thermodynamic Properties of Pure Chemicals, Data Compilation, Taylor and
Francis, Bristol, PA, 1989.
w22x ¨ ¨ J. Gmehling, J. Chem. Eng. Data. 39 Ž1994. 759–762.
M.A. Krahenbuhl,
w23x H.G. Rackett, J. Chem. Eng. Data 15 Ž1970. 514–517.