Fluid Phase Equilibria 303 (2011) 157161

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Fluid Phase Equilibria

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Volumetric behavior of the binary systems benzenecyclohexane and

benzene2,2,4-trimethyl-pentane at temperatures 293.15323.15 K
Zdenka Kolsk, Denisa Dvorkov, Jan Mika, Toms Boublk
Department of Chemistry, J.E. Purkinje University, st nad Labem, Czech Republic

a r t i c l e

i n f o

Article history:
Received 13 September 2010
Received in revised form 12 January 2011
Accepted 13 January 2011
Available online 26 January 2011
Keywords:
Benzene
Cyclohexane
2,2,4-Trimethylpentane
Density
Vibrating-tube densimeter
Binary system
Excess molar volume
RedlichKister equation
PengRobinson equation
Mixing rules
Combining rules

a b s t r a c t
Densities of the binary system benzenecyclohexane at several temperatures (293.15323.15 K) and
at atmospheric pressure were measured using a vibrating-tube densimeter in a static mode. Excess
molar volumes were calculated from the densities and correlated using the second-order RedlichKister
equation. Present data were compared with those determined previously by pycnometric measurements; a fair agreement of the old and new data sets was found. Also comparison with previously
presented experimental data of other authors was proved with a good agreement. In order to test
ability of the cubic equations and the standard mixing and combining rules to correlate/predict the
concentration dependence of the excess volume, PengRobinson equation of state was successfully
applied to the present data. Close similarity of characteristic parameters of benzene and cyclohexane prevents to discern among mixing rules available in literature and those proposed within this paper. Thus,
another binary system, i.e. benzene2,2,4-trimethylpentane was investigated in the temperature range
293.15323.15 K. PengRobinson constants of the components of this system differ in their magnitude
and thus allow to study the effect of different combining rules. It was found that the considered two comE
bining rules with slightly different correction constants k12 yielded very similar Vm
dependencies on the
concentration.
2011 Elsevier B.V. All rights reserved.

1. Introduction
The excess molar volume belongs to four simple thermodynamic characteristics of the thermodynamic behavior of binary
and multi-component mixtures at ambient temperatures. With an
introduction of the vibrating-tube densimetry technique, the deterE , is relatively easy and quite
mination of the excess volume, Vm
accurate. Experimental data obtained via this experimental technique might thus serve to study the suitability of the semi-empirical
and exact expressions proposed to date, to correlate and predict
E from the equation of state for pure components and mixing
Vm
rules for their constants. In the latter case also different mixing
and combining rules have to be applied. Theoretical results on
E for binaries and ternaries might be tested against accurately
Vm
E data. System benzenecyclohexane
measured experimental Vm
[19] plays a special role among the binaries because of simple
structures of molecules of both the pure uids as well as small
electrostatic interactions. From the experimental point of view
these compounds might be relatively easily prepared and charac-

Corresponding author.
E-mail addresses: tomas.boublik@ujep.cz, boublik@sci.ujep.cz (T. Boublk).
0378-3812/$ see front matter 2011 Elsevier B.V. All rights reserved.
doi:10.1016/j.uid.2011.01.018

teristic properties (e.g. values of densities or refractive indices at

temperatures 293.15 or 298.15 K) are well known. In this paper
we measured the benzenecyclohexane system at temperatures
293.15, 303.15, 313.15 and 323.15 K and atmospheric pressure.
To check the absolute precision of the measurement we compare
our data obtained within modern technique with values from a
classic method (measured by one of the authors [10]), where density was determined in a SprengelOswald two-arm pycnometer
(with calibrated capillaries). The previously published data were
used for comparison [10]. After nding an excellent agreement
between both the data sets, measured with different techniques,
we correlated rstly the present experimental data, employing the
RedlichKister expression [11].
Next we developed and applied a simple and versatile proE on the basis of an
cedure/computer program to evaluate Vm
equation of state and compared the calculated/predicted valE with the experimental excess volume dependence on
ues of Vm
the composition. We considered three cubic equations of state
(van der Waals, RedlichKwong and PengRobinson) and mixing and combining rules recommended in literature [12]. We also
considered new harmonic mean rule found within our theoretical studies. Results and conclusions are given at the end of the
paper.

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Z. Kolsk et al. / Fluid Phase Equilibria 303 (2011) 157161

Table 1
Values of PengRobinson constants a and b at 298.15 K.

2. Theory
E , similarly as the excess enthalpy, coinThe excess volume, Vm
cides with the mixing volume mix V,
E
Vm

= mix V = Vms

xi Vmi

(x1 M1 + x2 M2 )
M1
M2
=
x2
x1

1
2
(1)

where Vms and Vmi stand for the volume of one mol of the real
mixture and molar volume of component i, and xi is the corresponding mole fraction. With exception of the dilatometer proposed by
Pug and Benson [9], the molar volume has been determined indirectly from the measured density at the 
same temperature, 4t ,
and relative molecular mass, Mi , e.g. Vms =
xi Mi /4t . The simplest
semi-empirical expression used to correlate experimental data is
that proposed by Redlich and Kister [11]
E
Vm

= xi (1 xi )[A0 + A1 (1 2xi ) + A2 (1 2xi ) + ]

PVm
Vm
a
=

RT
RTVm
Vm b

(3)

Here the temperature- and density independent characteristic constants a, b were adjusted to the uid behavior, e.g. in the liquid
phase or in the critical point.
Due to the fact that the compressibility factor of liquids
possesses very low values, a pseudo-quadratic equation can be
obtained, by multiplying the above equation by Vm (Vm b); the
sought theoretical value of volume results from a few-step iteration.
Next, the more realistic EOS, proposed by Redlich and Kwong
[13] was considered, where
Vm
a
Z=


Vm b
RT 3/2 Vm (Vm + b )

(4)

Parameters of this EOS can be evaluated easily from the critical

constants, i.e.


a =

5/2
0.4275R2 Tc

Pc

0.08664RTc
b =
Pc


(5)

The equation of Peng and Robinson [14] is the most often used EOS
E [1]. It reads
to correlate and predict Vm
Z=

a
Vm

Vm b
Vm (Vm + b ) + b (Vm b )

a(Tc ) =

0.45724R2 Tc2
Pc

b =

b (dm3 mol1 )

Benzene
Cyclohexane
2,2,4-Trimethylpentane

2.8797
3.3239
5.3510

0.07522
0.06791
0.13701

Here Tr = T/Tc is the reduced temperature and Pitzers accentric

factor. Values of constants a and b for benzene, cyclohexane and
2,2,4-trimethylpentane at 298.15 K are listed in Table 1.
As a representant of the family of modern augmented van der
Waals EOSs the EOS by Chen and Kreglewski [15] might be mentioned
Z=

1 + (3 2)y + (32 3 + 1)y2 2 y3

(1 y)3



nDmn

 1  m  V 0 n
Tr

(9)

Vm

Tr = kT /u, u/k is the potential well, divided by Boltzmann constant

k and Dmn constants of the polynom; y b /Vm . It is obvious that
by multiplying numerator and denominator of the rst term by V,
denominator possesses the form (Vm b )(1 y)2 , where b = Vm V0 .
However, this equation is not used in the following sections.
2.1. Mixing and combining rules
In the case of mixtures the characteristic parameters of the used
EOSs are usually determined from the linear and quadratic rules
(related to the exact expression for the second virial coefcient of
a mixture). For constant a thus holds true
as =



xi xj aij

whereas for b
bs =

xi bi

or bs =

(10)



xi xj bij

(11)

In the case of quadratic expression, a combining rule is considered,

e.g.
aij = (1 kij )[aii ajj ]1/2
bij =

(1 lij )(bii + bjj )

2

(12)
1/3

or

bij =

(bii

1/3 3

+ bjj )
8

(13)

In this paper we considered for aij also the harmonic mean

2
1
1
=
+
aij
aii
ajj

(14)

found within the quantum mechanical study of intermolecular

interactions of simple molecules [16], eventually multiplied by
(1 kij ) like in (12). (A review of EOSs and mixing and combining
rules is given e.g. in Refs. [12,17].)

(6)
3. Experimental

where a and b are two characteristic constants, for which it
holds
a (T ) = a(Tc ),

a (dm6 MPa mol2 )

(2)

where parameters A0 , A1 , A2 , . . . are valid for a single temperature and pressure. However, to get more general information on
the molecular interactions of single components and their mixtures, the equations of state (EOS) have been considered. Up to
present time, different cubic equations of state have been applied
in majority of cases [1].
The cubic equations of state (by van der Waals, RedlichKwong
and PengRobinson) were considered also in this introductory
study, aimed in further steps at application of the modern noncubic EOSs (such as BACK and SAFT) to predict the mixture behavior,
too. We started with van der Waals equation as a prototype of the
cubic EOS the compressibility factor of which can be written as
Z=

Compound

0.07780RTc
Pc

(7)

and the temperature dependence of the attractive term is expressed

through the relation
= [1 + (0.37464 + 1.54226 0.269922 )(1 Tr0.5 )]

(8)

3.1. Chemicals
Benzene (Fluka Analytical, puris. p.a. ACS; purity 99.5 wt.%),
cyclohexane (SigmaAldrich, CHROMOSOLV, Plus, for HPLC, purity
99.9 wt.%) and 2,2,4-trimethylpentane (Riedel-de Haen., puris. p.a.
Reag. ACS, Reag. Ph, Eur. 99.5 wt.%) were used without further
purication. Their measured densities and refractive indices are
compared with the literature values [18] in Table 2.

Z. Kolsk et al. / Fluid Phase Equilibria 303 (2011) 157161

159

Table 2
Physical constants of pure compounds.
Substance

Constant

Benzene

420

Found
3

(g cm

n20
D
Cyclohexane

2,2,4-Trimethypentane

Ref. [18]

0.87898

0.8790

1.5010

1.5010

420 (g cm3 )

0.77854

0.7783

n20
D

1.4263

1.42623

425 (g cm3 )

0.68776

0.68774

n20
D

1.39145

1.39145

3.2. Apparatus and procedure

Refractive indices of pure compounds were measured by Refractometerr RM40, Mettler Toledo.
Vibrating tube densimetr (DMA 4500) supplied by Anton Paar,
Graz, Austria was used for density determination of pure uids and binary systems. The apparatus yields the direct density
values within density range 03 g cm3 , reproducibility of the density measurement 1.105 g cm3 and accuracy 5.105 g cm3 . The
temperature range of the apparatus was 273.15363.15 K, reproducibility of temperature was 0.01 K and its accuracy 0.03 K. Time
of measurement was 30 s for the sample of volume cca 1 cm5 .
Apparatus works with an automatic pressure compensation to
atmospheric pressure and with a viscosity correction for the whole
measurement range. For its calibration (at ambient temperature
and pressure), the redistilled water and air were used as standards; also the standard sample (liquid density standard Ultra pure
water by Anton Paar) was used for calibration. The samples for
the density measurements were prepared by weighing [by Mettler
Toledo balance XS205DU/M with a scale interval either 1.105 g (for
mass maximum of 81 g), or 1.104 g (for mass maximum of 210 g)].
The experimental uncertainty in composition (the mole fraction) is
less than 5.105 .
Results of the density measurement for the binary system
benzenecyclohexane are given in Table 3 and illustrated in Fig. 1.
In this gure we presented also the old data from pycnometric
measurement [10] at 283.15 and 333.15 K. The agreement with
the present smoothed data at 293.15 and 323.15 K is excellent and
gives evidence in favor of the accuracy of the modern densimetric
method.
From these density data the excess molar volumes were calculated, see [19] from relation (1). The data were also tted by the
E
second order RedlichKister type equation, see (2). Similarly, Vm
of the benzene2,2,4-trimethylpentane are summarized in Table 4.

E
Fig. 1. Comparison of experimental data of benzenecyclohexane, Vm
(cm3 mol1 )
vs. x1 , at 293.15 and 323.15 K (dashed and full lines) with the pycnometric results
at 283.15 and 333.15 K ( and ).

E
Fig. 2. Correlation of Vm
experimental data (cm3 mol1 ) of benzenecyclohexane,
at 293.15 K, from RedlichKwong (dashed) and PengRobinson (full line) equations
of state.

The parameters A0 A2 of the benzenecyclohexane system and that

of benzene2,2,4-trimethylpentane, A0 A2 and their standard
deviations are summarized in Table 5. for individual temperatures.
4. Results
Densities of the binary systems benzenecyclohexane and
benzene2,2,4-trimethylpentane at temperatures T = 293.15,
303.15, 313.15 and 323.15 K were measured. From these data the
excess volume dependence on concentration was calculated and
compared with the older data [10]. This comparison is shown
in Fig. 1. The present experimental data were correlated by the
RedlichKister (RK) equation. From the temperature dependence
E at x = 0.5 and at temof parameter A0 we found the values of Vm
1
E = 0.657 and 0.691 cm3 mol1 in
peratures 283.15 and 333.15 K Vm
comparison with RK values calculated from fragmentary results
in [10] 0.676 and 0.723 cm3 mol1 . Next, we present a prediction
of the excess volumes by means of the cubic equations of state.
E
The advantage of their application to predict (correlate) the Vm
dependence on the composition is twofold: (i) the temperature
E on x is mainly due to the temperature dependependence of Vm
i
dence of the constants (dependence of as on Tr ) of the used EOS;
only small changes of as is caused by the temperature dependence
of kij -corrections, (ii) the PV expressions might be used in the
general thermodynamic description of the mixture behavior. To
this end, we dealt with the correlation of the measured data of
benzenecyclohexane from three cubic equations of state, i.e. van
der Waals, RedlichKwong and PengRobinson. The rst EOS with
the recommended parameters yielded rather insufcient values of
the densities (volumes) of the pure uids and was withdrawn from
our further considerations. Application of the remaining two EOSs
is depicted in Fig. 2 for temperature T = 293.15 K. Because from
these two equations that of PengRobinson yielded better predicE we dealt in the
tion of values of the pure uid volumes and also Vm
remaining part only with the PengRobinson EOS. Its parameters,
calculated for temperature T = 298.15 K are given in Table 1. For
other temperatures the a-constant can be calculated from Eq. (8)
and the accentric parameter; for benzene = 0.2183, for cyclohexane = 0.2081 and = 0.3030 for 2,2,4-trimethylpentane. Results
of the correlation for temperatures T = 293.15 and 323.15 K are
presented in Fig. 3. A fair agreement (with  = 0.025 cm3 mol1 )
E and found experimental data for quite
of the predicted Vm
small values of kij = 0.0670.051 at T = 293.15 and 323.15 K are
obvious.

160

Z. Kolsk et al. / Fluid Phase Equilibria 303 (2011) 157161

Table 3
E
(cm3 mol1 ), calculated from Eq. (1) for binary system benzenecyclohexane at temperatures 293.15323.15 K.
Density, T (g cm3 ), and excess molar volume, Vm
x1

293

E
Vm,293

303

E
Vm,303

313

E
Vm,313

323

E
Vm,323

0.0000
0.1000
0.1805
0.2347
0.3029
0.3801
0.4453
0.5223
0.5814
0.6563
0.7135
0.7654
0.8191
0.8771
0.9161
1.0000

0.77854
0.78499
0.79071
0.79492
0.80047
0.80710
0.81309
0.82056
0.82662
0.83472
0.84121
0.84744
0.85416
0.86175
0.86703
0.87898

0.0000
0.2648
0.4273
0.5015
0.5755
0.6369
0.6597
0.6608
0.6411
0.5923
0.5395
0.4704
0.3836
0.2762
0.1969
0.0000

0.76913
0.77547
0.78114
0.78530
0.79079
0.79733
0.80325
0.81063
0.81662
0.82462
0.83103
0.83718
0.84382
0.85131
0.85652
0.86830

0.0000
0.2720
0.4332
0.5078
0.5815
0.6444
0.6667
0.6674
0.6467
0.5970
0.5434
0.4736
0.3853
0.2771
0.1973
0.0000

0.75960
0.76587
0.77146
0.77557
0.78100
0.78747
0.79332
0.80062
0.80653
0.81444
0.82077
0.82683
0.83339
0.84079
0.84595
0.85757

0.0000
0.2745
0.4394
0.5149
0.5886
0.6511
0.6735
0.6730
0.6530
0.6020
0.5480
0.4792
0.3898
0.2801
0.1978
0.0000

0.74994
0.75614
0.76167
0.76573
0.77110
0.77750
0.78327
0.79048
0.79634
0.80414
0.81041
0.81641
0.82289
0.83019
0.83528
0.84676

0.0000
0.2776
0.4440
0.5207
0.5949
0.6575
0.6817
0.6817
0.6590
0.6095
0.5530
0.4821
0.3918
0.2823
0.2000
0.0000

Table 4
E
(cm3 mol1 ), calculated from Eq. (1) for binary system benzene2,2,4-trimethylpentane at temperatures 293.15323.15 K.
Density, T (g cm3 ), and excess molar volume, Vm
x1

293

E
Vm,293

303

E
Vm,303

313

E
Vm,313

323

E
Vm,323

0.0000
0.1248
0.1642
0.3682
0.4538
0.5020
0.5388
0.6023
0.6896
0.9443
1.0000

0.69188
0.70406
0.70826
0.73374
0.74653
0.75434
0.76070
0.77244
0.79037
0.85913
0.87898

0.0000
0.2569
0.3258
0.5266
0.5546
0.5629
0.5572
0.5362
0.4858
0.1490
0.0000

0.68364
0.69566
0.69980
0.72494
0.73757
0.74527
0.75154
0.76315
0.78086
0.84873
0.86830

0.0000
0.2629
0.3316
0.5367
0.5637
0.5736
0.5689
0.5438
0.4908
0.1488
0.0000

0.67530
0.68716
0.69124
0.71605
0.72851
0.73612
0.74233
0.75377
0.77125
0.83826
0.85757

0.0000
0.2652
0.3385
0.5471
0.5755
0.5836
0.5753
0.5531
0.4994
0.1500
0.0000

0.66684
0.67853
0.68255
0.70704
0.71933
0.72685
0.73296
0.74428
0.76154
0.82770
0.84676

0.0000
0.2727
0.3486
0.5593
0.5896
0.5961
0.5910
0.5636
0.5081
0.1519
0.0000

Table 5
Parameters of RedlichKister Eq. (2) (in cm3 mol1 ) for binary systems benzenecyclohexane (BCH) and benzene2,2,4-trimethylpentane (BTMP) at temperatures
293.15323.15 K.
Parameter

A0
A1
A2
A0
A1
A2

(BCH)
(BCH)
(BCH)
(BTMP)
(BTMP)
(BTMP)

T
293.15

STD

303.15

STD

313.15

STD

323.15

STD

2.657
0.184
0.164
2,233
0.048
0,377

0.008
0.015
0.034
0.013
0.041
0.080

2.682
0.206
0.173
2,273
0.021
0,349

0.009
0.017
0.039
0.013
0.042
0.082

2.708
0.216
0.186
2,313
0.012
0,338

0.009
0.017
0.039
0.013
0.042
0.083

2.739
0.225
0.174
2,366
0.012
0,336

0.009
0.017
0.040
0.013
0.043
0.085

E
Fig. 3. Correlation of Vm
experimental data (cm3 mol1 ) of benzenecyclohexane
at 293.15 and 323.15 K by PengRobinson equation of state.  and  experimental
data at 293.15 and 323.15 K.

Originally, we intended to study the effect of the use of harmonic mean (hm) (14) instead of geometric mean (gm) for constant
aij in (12). However, values of aii -parameters of benzene and cyclohexane are so closed, that the resulting values of aij differed only
negligibly, i.e. ahm = 3.086 in comparison with agm = 3.093; no effect
E vs. x was
on the course of the theoretical dependence of Vm
i
observed.
In order to study different combining rules we
measured another binary system, i.e. system benzene2,2,4trimethylpentane (formerly considered e.g. in Refs. [1924]).
PengRobinson characteristic constants of its pure components
differ substantially and thus allow to discern between relations
E (of
(12) and (14). To this end we plotted experimental data of Vm
the latter system at 293.15 K) together with calculated dependence for the combining rule (12) with k12 = 0.0 and compared the
E (dashed line) with experimental data in
predicted course of Vm
Fig. 4. A fair agreement was found. Next, we considered combining
rule (14) and k12 = 0.0, and got a curve with signicantly higher
E than experimental ones for the single concentrations.
values of Vm
However, when we multiplied calculated value of a12 by the
correction with k12 = 0.05, we obtained practically indistinguish-

Z. Kolsk et al. / Fluid Phase Equilibria 303 (2011) 157161

161

As the use of the harmonic combining rule is concerned, no

denitive conclusion can be drawn because of the negative sign
of the correction parameter kij .

E
experimental data (cm3 mol1 ) of benzene2,2,4Fig. 4. Correlation of Vm
trimethylpentane at 293.15 by PengRobinson equation of state.  experimental
data; dashed line, calculated employing the geometric mean; full line, from harmonic mean.

able dependence (see full line in Fig. 4). In both the cases  was
0.016 cm3 mol1 . However, because positive values of k12 are
generally assumed to be the correct ones, we can conclude that
for the latter binary system the usual combining rule is preferable
for temperature T = 293.15 K. [For the highest measured temperature T = 323.15 K a fair agreement can be obtained for both the
combining rules, however, in both the cases with negative values
of k12 (for the geometric mean k12gm = 0.009 in comparison with
k12hm = 0.057).]
5. Conclusion
In this contribution we measured densities and calculated
the excess volume dependence on concentration at temperatures
T 293.15, 303.15, 313.15 and 323.15 K for the binary systems benzenecyclohexane and benzene2,2,4-trimethylpentane.
E for the former system at the lowest and
Experimental results of Vm
highest temperatures were compared with the older data and indicate a fair mutual agreement. These data were correlated by RK
equation; from the temperature dependence of its parameter A0
E at x = 0.5 and at temperatures 283.15 and
we found values of Vm
1
E
333.15 K to be Vm = 0.657 and 0.691 cm3 mol1 in comparison with
RK values 0.676 and 0.723 cm3 mol1 . Taking into account the error
estimates of the old pycnometric- and the modern experimental
techniques a fair agreement was found.
The use of the newer equations of state instead of the semiempirical RedlichKister expression for the correlation of the
excess volume brings with itself an inclusion of the temperature
E . Values of terms PV E might be thus correctly
dependence of Vm
m
used in different thermodynamic expressions. The best results for
the considered binaries were obtained by PengRobinson equation
of state.

List of symbols
Ai
constants of RedlichKister equations
a,b
constants of semi-empirical equations
constant of PengRobinson equation (dm6 MPa mol2 )
a
b
constant of PengRobinson equation (dm3 mol1 )
Dmn
constants of a polynom
M
molecular mass
P
pressure (Pa)
Pc
critical pressure (Pa)
R
gas constant (J K1 mol1 )
T
temperature (K)
Tc
critical temperature (K)
Tr
reduced temperature
V
volume (m3 )
molar volume (m3 mol1 )
Vm
E
Vm
excess (molar) volume (cm3 mol1 )
xi
molar fraction
y
packing fraction
Z
compressibility factor

non-sphericity factor

density (kg m3 , g cm3 )
E (cm3 mol1 )

standard deviation in Vm

accentric factor
Acknowledgement
This work was carried out within the Grant Agency of Academy
of Science of Czech Republic project no. IAA 400720710.
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