Fluid Phase Equilibria 211 (2003) 3549

Second virial coefficients of polar haloalkanes2002

Constantine Tsonopoulos
18 Dorothy Drive, Morristown, NJ 07960, USA
Received 24 January 2003; accepted 25 March 2003

Abstract
The 1975 investigation of the second virial coefficients of polar haloalkanes [AIChE J. 21 (1975) 827] demonstrated an apparent difference between polar haloalkanes and non-hydrogen bonding fluids such as ketones and
ethers that had been examined earlier [AIChE J. 20 (1974) 263]. The difference was in the dependence of the polar
contribution to B (second virial coefficient) on r (reduced dipole moment). However, the 1975 observation was
based on data for only three polar haloalkanes. The large number of new measurements that have been made since
1990 on chlorofluoroalkanes and, especially, the environmentally-benign hydrofluoroalkanes has made it possible
to re-examine the B of polar haloalkanes. This re-examination has included the correlation of Weber [Int. J. Thermophys. 15 (1994) 461], which differs both in the non-polar terms and in the dependence of the polar contribution
to B on r .
A brief examination of three non-polar compounds (Ar, n-butane, n-octane) has helped clarify the strengths
and weaknesses of three non-polar correlations (PitzerCurl, Tsonopoulos, Weber). A definitive study of the polar
contribution to B may require an improvement of the non-polar B correlation. The two different approaches to the
B of polar haloalkanes (Tsonopoulos, Weber) were investigated primarily for haloalkanes with r > 100, and the
conclusion was that the two approaches are roughly equivalent, with Weber possibly having an advantage when
r < 50, but not for chloroalkanes. The 1975 recommendation for the dependence of the polar contribution to B
on r was confirmed by the new data. A more definitive conclusion on this dependence may be realized by using
molecular modeling techniques.
2003 Elsevier B.V. All rights reserved.
Keywords: Second virial coefficients; Non-polar compounds; Polar haloalkanes; Reduced dipole moment

1. Introduction
The 1975 investigation of haloalkanes [1] was hampered by the limited databaseboth in quantity
and quality. These limitations led to the erroneous conclusion that only monohaloalkanes (alkyl halides)

This paper was presented at the Halocarbon Workshop at the 17th IUPAC Conference on Chemical Thermodynamics (ICCT
2002), Rostock, Germany, 28 July2 August 2002.

Tel.: +1-973-540-9229.
E-mail address: ctsonop@ix.netcom.com (C. Tsonopoulos).
0378-3812/03/$ see front matter 2003 Elsevier B.V. All rights reserved.
doi:10.1016/S0378-3812(03)00112-2

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C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

required a polar contribution to their B (second virial coefficient). That was because the non-polar part of
the B correlation appeared to fit satisfactorily the B of the moderately polar dichloromethane (r = 57.6)
and the strongly polar 1,1-difluoroethane (r = 153). Thus, the polar contribution to B and its dependence
on r were based on just three compounds: chloromethane, fluoromethane, and chloroethane. But even
with these limited data it became clear that the dependence of the polar contribution on r was different
from that found earlier for non-hydrogen bonding CHO and CHN compounds [2]. For r < 200,
the polar contribution to the B of haloalkanes was much weaker than that for the organic compounds
containing O or N. However, for r > 200, the polar contribution appeared to approach the same limit
for all compounds.
This difference is generally attributed to the fact that at low r values the location and direction of the
dipole moment are important, but at much larger values (r > 200) the magnitude of the reduced dipole
moment overshadows the contributions of location and direction, and thus magnitude alone affects the
polar contribution to B.
The large number of new B data that have become available since around 1990, many of them mentioned in Dymonds 2000 review [3], can now be examined with the goal of testing and, if needed,
updating the 1975 correlation for polar haloalkanes; as well as comparing it with Webers 1994 correlation [4]. Most of the new B data are on chlorofluoroalkanes and, especially, hydrofluoroalkanes. The
environmentally-benign hydrofluoroalkanes have already started replacing the ozone-depleting chlorofluorocarbons that are currently being used as refrigerants.
2. Correlating equations for non-polar gases
The reduced second virial coefficient (BPc /RTc ) can be expressed as a sum of three functions of reduced
temperature, Tr (= T/Tc ):
BPc
= f (0) + f (1) + f (2)
RTc

(1)

The first function, f (0) , gives the reduced B for compounds with (acentric factor) = 0, while f (1)
corrects the value of the reduced B for compounds with = 0 (that is, for deviations from spherical
symmetry). For polar compounds, that is, compounds that have a non-zero dipole moment, f (2) gives the
polar contribution to the reduced B (which will be examined in the following section).
Three correlations for non-polar compounds are considered. The first one and the best known was
proposed by Pitzer and Curl in 1957 [5]:
(0)
fPC
= 0.1445
(1)
fPC
= 0.073 +

0.33 0.1385 0.0121

Tr
Tr2
Tr3

0.46 0.5 0.097 0.0073

2

Tr
Tr
Tr3
Tr8

(2)
(3)

(0)
Pitzer and Curl determined the coefficients of fPC
by fitting the B data for Ar, Kr, and Xe, which have zero
acentric factor. In 1974, Tsonopoulos [2] examined data for Ar and Kr that were reported in 19671969
and found that Eq. (2) was unsatisfactory for Tr < 0.75; at Tr = 0.53, the error was 10%. This is illustrated
in Fig. 1 that was taken from [2]. Tsonopoulos proposed a slight modification of Eq. (2) that made it

C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

37

Fig. 1. Second virial coefficient of gases with 0 (from [2]).

possible to fit the data included in Fig. 1 to within 1%:

(0)
fT(0) = fPC

0.000607
Tr8

(4)

Tsonopoulos also modified Eq. (3) by fitting the 1969 recommendations of Dymond and Smith [6] for
n-butane ( = 0.200) and the experimental data of Connolly and Kandalic [7] and of McGlashan and
Potter [8] for n-octane ( = 0.398):
fT(1) = 0.0637 +

0.331 0.423 0.008

Tr2
Tr3
Tr8

(5)

Differences from Eq. (3) are relatively small, but persist up to high reduced temperatures (see example
for CO2 in Fig. 3 of [2]).
In 1994, Weber proposed a new correlation for polar haloalkanes [4]. In his introduction, Weber noted
that he used the modifications by Tsonopoulos, that is, Eqs. (4) and (5) for non-polar gases, but actually
he removed the Tr8 terms from both equations. Thus, Webers correlation can be summarized as
(0)
(0)
fW
= fPC
(1)
= fT(1) +
fW

(6)
0.008
Tr8

(7)

Eqs. (1)(7) will be compared with selected data for Ar, n-butane, n-octane, and a haloalkane that is
essentially non-polar.

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C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

2.1. Argon
In recent years it has been noted, for example by Dymond [3], that many of the older PvT data,
which historically have been the source of the B values in the literature, were not corrected for physical
adsorption effects, and therefore the resulting Bs are too negative. This is especially the problem at
subcritical temperatures. Although it is possible to correct for these effects, apparently this was not done
for the Ar and Kr data shown in Fig. 1, which today are generally considered to be too negative.
Eqs. (2) and (4) were examined against the 1994 data of Gilgen et al. [9] for Ar. (In an accompanying
paper [10], Gilgen et al. also measured the critical properties and the vapor pressure of Ar, which were
used to calculate the acentric factor: = 0.0022.)
The data extend from 110 (Tr = 0.73) to 340 K (Tr = 2.26), and the comparison of the deviations of
Eqs. (2) and (4) from the data in Fig. 2 clearly illustrates that these data from Wagners group do not
(0)
support the correction made to fPC
in 1974 (to fit the data for Ar and Kr that are plotted in Fig. 1). The
Bs from the PvT measurements of Gilgen et al. [9] are in excellent agreement with those derived from
the speed-of-sound measurements of Estrada-Alexanders and Trusler [11] at 110450 K; the maximum
difference is 0.56 cm3 mol1 (0.53%) at 135 K.
2.2. n-Butane and n-octane
These two compounds were used in 1974 to establish the new f (1) . The best data for n-butane are now
considered to be [12] the isochoric Burnett measurements of Gupta and Eubank [13] at 264.9450 K.

Fig. 2. B of argon: deviation from data of Gilgen et al. [9]; (- - -) PitzerCurl [5]; () Tsonopoulos [2].

C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

39

Fig. 3. B of n-butane: deviation from data of Gupta and Eubank [13]; (- - -) PitzerCurl [5]; () Tsonopoulos [2]; ( )
Weber [4].

All three correlations are compared in Fig. 3. The 1974 modification of the PitzerCurl correlation gives
the smallest deviation, except for Tr < 0.7, where the original PitzerCurl correlation is superior. On the
other hand, Webers correlation is everywhere too positive, and the deviation increases considerably as
Tr goes from 0.8 to 0.6.
The B values used for n-octane were those calculated at 375575 K with an equation determined by
Al-Bizreh and Wormald [14] from fitting the data used in the 1974 investigation [7,8] along with those

Fig. 4. B of n-octane: deviation from equation of Al-Bizreh and Wormald [14], which fits their data and those of Connolly and
Kandalic [7] and of McGlashan and Potter [8]; (- - -) PitzerCurl [5]; () Tsonopoulos [2]; ( ) Weber [4].

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C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

Fig. 5. B of CCl2 F2 : deviation from smoothed experimental data [1519]; (- - -) PitzerCurl [5]; () Tsonopoulos [2]; ( )
Weber [4].

they obtained from their JouleThomson measurements. As Fig. 4 demonstrates, at = 0.398 the overprediction of B with Webers correlation becomes much more pronounced, while the 1974 modification
appears to give the best results over the entire range. Thus, as increases, the removal of the Tr8 term
(1)
from fW
makes this correlation progressively worse, while the addition of the Tr8 term to fT(0) becomes
rapidly less of a factor.
2.3. Dichlorodifluoromethane
CCl2 F2 (R-12) is essentially non-polar ( = 0.51 D; r = 7.2), and so it is included in this section. Its
B was examined by Dymond, who found that Webers correlation was significantly better than the 1974
modification of the PitzerCurl correlation (see Fig. 5 in [3]). The same data are examined here, and the
deviation of the three non-polar correlations from the smoothed data [1519] is plotted in the new Fig. 5.
Table 1
RMSD of non-polar correlations from experimental B data
Compound (; r )

Ar (0.0022; 0)
n-Butane (0.200; 0)
n-Octane (0.398; 0)
CCl2 F2 (0.180; 7.2)a
a

and from [20].

RMSD (cm3 mol1 )

PitzerCurl

Tsonopoulos

Weber

0.7
8.6
32.1
15.7

1.1
10.8
6.1
17.2

0.7
29.2
87.2
8.6

C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

41

Although Webers correlation becomes too positive at Tr < 0.7, resulting from the elimination of the Tr8
term, overall it provides the best fit.
This is also shown in Table 1, which presents the RMSD (root-mean-square deviation) of the three
correlations from the smoothed experimental data for the four non-polar gases examined in this section.
It is perhaps surprising that Weber does better than PitzerCurl for CCl2 F2 ( = 0.180), even though it
is significantly worse for n-butane ( = 0.200). It may be that there is no exact correspondence between
alkanes and even weakly polar haloalkanes in the dependence of B on .

3. Polar contribution to B
In Eq. (1), f (2) is the polar contribution to B. It was shown in 1974 [2] that for non-hydrogen bonding
polar fluids (such as ketones, ethers, as well as acetonitrile) f (2) can be given by a simple function of Tr :
a
f (2) = 6
(8)
Tr
where the parameter a can be correlated with the reduced dipole moment of the fluid.
r =

2 Pc
1.01325 Tc2

(9)

In Eq. (9), , the dipole moment of the compound (in the gas phase), is in Debyes (1 D = 3.33564
1030 C m), Pc is in pascals, and Tc is in kelvins. (The factor 1.01325 is used to make r numerically
identical to that used in [1,2], where it was defined as 105 2 Pc /Tc2 , but Pc was in atmospheres; 1 atm =
1.01325 105 Pa.) The relationship between a and r was determined to be
a = 2.140 104 r 4.308 1021 8r

(10)

In the 1975 investigation of the B of polar haloalkanes [1], it was observed that Eq. (10) worked well
only at high values of the reduced dipole moment (r > 200). However, for r < 200, the absolute value
of a decreased more steeply with decreasing r than Eq. (10) predicted. Thus, on the basis of the data
for chloromethane, fluoromethane, and chloroethane, a different dependence of a on r was proposed for
polar haloalkanes:
a = 2.188 1011 4r 7.831 1021 8r

(11)

(As noted in the introduction, it was erroneously concluded in 1975 that this correction would be required
only for monohaloalkanes.)
The difference between Eqs. (10) and (11) for r < 200 is clearly illustrated in Fig. 6. Thus, although
the polar parameter a depends very strongly on the reduced dipole moment, the functional dependence
is not universal, unless the reduced dipole moment is very large, say, r > 200. At lower values of r , as
noted earlier, the location and direction of the dipole moment apparently must be taken into account.
Weber also used Eq. (8) for the polar contribution to B, but found a different dependence of a on r
that is given by Eq. (12) which is plotted in Fig. 6.
a = 9 107 2r

(12)

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C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

Fig. 6. Dependence of polar parameter a on reduced dipole moment, r ; (- - -) CHO, CHN [2]; () haloalkanes [1]; ( )
Weber [4].
(2)
Weber, by removing the Tr8 terms from his f (0) and f (1) , increased the contribution of fW
to the B of
polar halolkanes for r < 200 so that it is non-negligible even for r < 50 (where the a parameter in the
1975 correlation can be neglected).
Webers correlation (Eqs. (1), (68) and (12)) is compared with the 1975 correlation for polar haloalkanes (Eqs. (1), (4), (5), (8) and (11)) in the following section. Although Eq. (11) is used to determine the
value of a for r < 100, for higher values the new B data are regressed to obtain the optimum value for
a in the 1975 correlation.

4. Polar haloalkanes
4.1. Halomethanes
Dymond noted in his recent review [3] that the most extensively investigated polar halomethanes in
the 1990s were CHClF2 (R-22) and the much more environmentally friendly CH2 F2 (R-32). The first
compound has a r < 100, and thus its parameter a was obtained from Eq. (11), but the data for the more
polar CH2 F2 were regressed to determine the optimum value for a. Figs. 7 and 8 show the deviation of
the two correlations from the smoothed experimental data. Both figures show the characteristic increase
in the deviation of Webers correlation as Tr decreases.
CHClF2 , CH2 F2 , and three other halomethanes with r > 100 are listed in Table 2 along with their
values for and r , the data sources, the optimum value for a in the 1975 correlation, and the RMSDs for
the two polar correlations. (Unless otherwise noted, Tc , Pc , , and were taken from the DIPPR data
compilation [20] .) Generally, the two correlations are equivalent, except for CH3 Cl, where the RMSD
with Webers correlation approaches 26 cm3 mol1 .

C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

43

Fig. 7. B of CHClF2 : deviation from smoothed experimental data [1619,2123]; () Tsonopoulos [2]; ( ) Weber [4].

4.2. Haloethanes
According to Dymond [3], two-thirds of the measurements on haloethanes were made in the 1990s,
and the majority of them were on hydrofluoroethanes with 5 (R-125), 4 (R-134a), 3 (R-143a), and 2
(R-152a) fluorine atoms. All four compounds were investigated, along with three other haloethanes with
r > 100, and the results are listed in Table 3. As in the case of the halomethanes, the two correlations
are roughly equivalent, even for C2 H5 Cl, where they show the largest deviations (2729 cm3 mol1 ).

Fig. 8. B of CH2 F2 : deviation from smoothed experimental data [2628]; () Tsonopoulos [2]; ( ) Weber [4].

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C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

Table 2
RMSD of polar correlations from experimental B data for halomethanes
Compound (; r )a

CHClF2 (0.219; 76.5)b

CHF3 (0.264; 144.6)
CH2 F2 (0.277; 181.0)b
CH3 Cl (0.153; 133.1)
CH3 F (0.198; 197.2)

Data sources

[1619,2123]
[16,2426]
[2628]
[2931]d
[23,26,29]

Optimum a for 1975 correlations

(0.00076)c
0.0152
0.0236
0.00489
0.0451

RMSD (cm3 mol1 )

Tsonopoulos

Weber

8.5
5.4
5.0
11.9
3.3

11.9
5.0
10.2
25.9
7.0

and from [20], unless otherwise noted.

from [32].
c
a obtained from Eq. (11).
d
Did not use recommended values in [29] at 500600 K.
a

Two examples are given. Fig. 9 shows the deviations from the smoothed data for 1,1,1,2-tetrafluoroethane
(R-134a). Once again we see the large increase in the deviation with Webers correlation as Tr goes below
0.7. But in the case of 1,1-difluoroethane (R-152a) in Fig. 10, there is no such increase, even at Tr = 0.6,
and as a result Webers correlation is slightly better than the 1975 correlation with an optimum value
for a.
4.3. Dependence of a on r
The data analysis summarized in Sections 4.1 and 4.2 led to 10 optimum values for the a parameter
in the 1975 correlation. These values were expected to give a more definitive relationship between a and
r for haloalkanes that would improve upon Eq. (11)which had been based on relatively limited data
available in 1975 for just three monohalolkanes: CH3 Cl, CH3 F, and C2 H5 Cl.

Table 3
RMSD of polar correlations from experimental B data for haloethanes
Compound (; r )a

CHF2 CF3 (0.305; 75.9)b

CH2 FCF3 (0.327; 121.1)b
CH3 CClF2 (0.231; 108.5)
CH3 CF3 (0.261; 170.0)b
CH3 CHF2 (0.275; 152.8)b
CH3 CH2 Cl (0.190; 103.1)
CH3 CH2 F (0.220; 132.6)

Data sources

[3335]
[18,33,3638]
[18,22]
[33,39]
[18,22,33,38]
[16,31,40,41]
[33]

and from [20], unless otherwise noted.

from [42].
c
a obtained from Eq. (11).
a

Optimum a for 1975 correlations

(0.00073)c
0.00667
0.00244
0.0191
0.0143
0.00323
0.00476

RMSD (cm3 mol1 )

Tsonopoulos

Weber

4.2
3.8
8.6
4.5
8.6
27.4
0.7

4.3
6.1
19.1
5.9
7.0
29.3
17.9

C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

45

Fig. 9. B of CH2 FCF3 : deviation from smoothed experimental data [18,33,3638]; ()Tsonopoulos [2]; ( ) Weber [4].

The result was somewhat surprising. When the optimum a values for the 10 haloalkanes were plotted
versus r in Fig. 11, the 1975 relationship, Eq. (11), turned out to give a most satisfactory representation
of the 2002 results. Thus, although a slight improvement in the fit of the 2002 optimum a values is possible
with some adjustment in the coefficients of Eq. (11), it was decided to retain the original Eq. (11) for
representing the dependence of a on r for polar haloalkanes.

Fig. 10. B of CH3 CHF2 : deviation from smoothed experimental data [18,22,33,38]; () Tsonopoulos [2]; ( ) Weber [4].

46

C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

Fig. 11. Dependence of 2002 results for polar parameter a on r : () 1975 correlation [1]; () 2002 optimum values.

5. Where are we?

For non-polar gases, fT(0) appears to be too negative at subcritical temperatures (Fig. 2), but this
deficiency becomes smaller as increases, because fT(1) becomes progressively more important. On the
(1)
other hand, the removal of the Tr8 term from fW
makes Webers correlation too positive at low Tr , and
this deficiency increases as increases to 0.2 (Fig. 3) and 0.398 (Fig. 4). However, Webers correlation
is surprisingly good for CCl2 F2 , = 0.18 (Fig. 5).
For polar haloalkanes, the Tsonopoulos [1] and Weber [4] correlations are roughly equivalent, especially
considering that the results with Webers correlation can be improved by using component-specific
parameters in place of Eq. (12). In the case of the Tsonopoulos correlation, results with Eq. (11) are
significantly worse than with the optimum a value only for CH2 F2 . This is also the only case where a
direct fit of the new a values (Tables 2 and 3) would be a significant improvement over Eq. (11); otherwise,
the 2002 investigation supports the 1975 results for the dependence of a on r but not the erroneous
1975 conclusion that only monohaloalkanes require a polar correction to their B.
(1)
The elimination of the Tr8 term from fW
improves the predictions with Webers correlation for mildly
polar haloalkanes (r < 50), but not for chloroalkanes (with or without fluorine). Although there is no
longer much interest in chloroalkanes, at least as refrigerants, it would be of interest to measure their B
at low Tr , because some recent data may be too positive. More experimental data may also be needed for
C2 H5 F, for which only three B values have been determined [33].
6. What more do we need for haloalkanes?
If there is an interest in improving the generalized correlations for polar haloalkanes, it may be
necessary, as Dymond recommended in his review [3], to go back to the non-polar correlation and

C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

47

improve both f (0) and f (1) over a wide Tr range. There are limitations both at Tr < 0.7 and
Tr > 2.
Once f (0) and f (1) are improved, f (2) and the relationship between a and r can be tested and put
in some final form. Molecular modeling techniques should be very helpful in establishing the proper
dependence of the polar contribution to B on r , at both low and high values. Such techniques should make
possible the quantification of dipole location and direction effects, which presumably are important at
low r values (<100?), and whether at high values (r > 200) only the magnitude of the dipole moment
matters. If that turns out to be true, as suspected at present, then all strongly polar, but non-hydrogen
bonding, gases would have the same dependence of a on r .
Nothing has been said here about mixtures of haloalkanes. The data available in 1975 were examined
in [1], and a similar approach can be taken in analyzing the new data. On the basis of what has been
found for other classes of compounds, when the two components of a binary are very dissimilar in
size or chemical nature (or both), then a binary interaction constant may be needed to correct for the
deviation of the characteristic temperature, Tcij , from the geometric mean of the two critical temperatures
[1,2]:
Tcij = (Tci Tcj )0.5 (1 kij )

(13)

Finally, what about calculations at high densities, where B alone will not suffice? The traditional
approach is to use the virial equation of state with the less well-known third virial coefficients and, at
still higher densities, the virtually unknown fourth virial coefficients. Or an alternative, simpler approach
can be taken that may work just as well: use the VirialRedlichKwong equation of state [43], which
combines the B correlation with the original RedlichKwong equation of state.
List of symbols
a
B
f (0) , f (1) , f (2)
kij
P
Psat
R
T
Tcij
v

parameter of polar contribution to B, f (2)

second virial coefficient
dimensionless functions of Tr in B correlations
characteristic binary constant; see Eq. (13)
pressure
vapor pressure
gas constant
absolute temperature (in kelvins)
characteristic temperature used in B correlation for mixtures; see Eq. (13)
molar volume

Greek letters

dipole moment, in Debyes (1 D = 3.33564 1030 C m)

reduced dipole moment {r = 2 Pc /(1.01325 Tc2 ); where Pc is in Pa}
acentric factor { = log10 (Prsat ) 1}

Subscripts
c
i, j
PC

critical property
property of component i, j
functions in PitzerCurl correlation

48

C. Tsonopoulos / Fluid Phase Equilibria 211 (2003) 3549

r
T
W

reduced property (Mr = M/Mc , for M = P or T, but not )

functions in Tsonopoulos correlation
functions in Weber correlation

Acknowledgements
The author is grateful to Alexi Tsonopoulos, for assistance in preparation of Figs. 211.
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