Ind. Eng. Chem. Res.

2003, 42, 7037-7044 7037

The Second Virial Coefficient and the Redlich-Kwong Equation

Paul M. Mathias*
Aspen Technology, Inc., 10 Canal Park, Cambridge, Massachusetts 02141-2201

A two-parameter corresponding-states correlation, based upon the Redlich-Kwong equation, is

proposed for the second virial coefficient at relatively high temperature (reduced temperature
above 0.8). This remarkably simple correlation suggests an improvement to the venerable
Redlich-Kwong equation of state, gives guidance for the high-temperature extrapolation of
R-functions, and provides an independent tool to evaluate theoretical and empirical correlations
for the second virial coefficient.

Introduction RTc
b ) 0.08664035 (2)
Redlich and Kwong were concerned about the limiting Pc
behavior of their equation of state (EoS).1 They sought
an accurate gas-phase model at low density and high R2Tc2
ac ) 0.42748025 (3)
density and hence paid special attention to the second Pc
virial coefficient. This emphasis on the second virial
1
coefficient was distracted by the success of the proposal R(T) ) (4)
of Wilson2 and Soave,3 which recommended fitting the TeR
EoS directly to vapor pressures without attention to the
second virial coefficient, PVT properties, or other abso- R is the gas constant, Tc and Pc are the critical
lute thermodynamic properties. The focus on the second temperature and critical pressure of the fluid, respec-
virial coefficient was partially revived by the density- tively, and TR is the reduced temperature (TR ) T/Tc).
dependent EoS mixing rules of Mollerup4 and Whiting The R-function (eq 4) for the Redlich-Kwong equation
and Prausnitz,5 and the Wong-Sandler6 mixing rules; has been generalized by introducing the exponent e. In
these researchers developed EoS models that followed the original RK EoS, e ) 0.5, but in this work, we show
the theoretically correct quadratic mole fraction depen- that a better value for most substances is e ) 1.0.
dence of the second virial coefficient, but they paid little The virial equation is a power series for the com-
attention to the quantitative accuracy of the second pressibility factor in the reciprocal molar volume, 1/v.
virial coefficients.
In this work, we revisit the approach of Redlich and Pv B 2 B3
Kwong1 by seeking a simple model that provides an z) )1+ + 2 + ... (5)
RT v v
accurate description of the second virial coefficient in
the high-temperature region. It turns out that a two- z is the compressibility factor, B2 is the second virial
parameter corresponding-states model provides an ac- coefficient, and B3 is the third virial coefficient. Follow-
curate prediction of the second virial coefficients of ing Pitzer and Curl7 and Tsonopoulos,8 we develop a
nearly all substances, from nonpolar alkanes to polar correlation for the reduced second virial coefficient in
molecules to hydrogen-bonding substances such as terms of Tc and Pc, which, according to the RK EoS, is
water and methanol, as long as the range of the model as follows:
is limited to relatively high temperatures (reduced
temperatures above 0.8). This simple model suggests an B2Pc 0.42748025
improved Redlich-Kwong EoS, provides guidance for ) 0.08664035 - (6)
RTc T 1+e
the high-temperature extrapolation of R-functions, and R
provides an independent tool to evaluate experimental
data and theoretical and empirical correlations for the According to the RK EoS, the reduced second virial
second virial coefficient. coefficient at the critical temperature has a universal
value for all substances, which is equal to -0.34084.
The purpose of this paper is to report that eq 6
The Redlich-Kwong EoS and the Second Virial provides a surprisingly accurate correlation for B2 of
Coefficient most substances for reduced temperatures above about
The Redlich-Kwong EoS relates the pressure P of 0.8 if e is changed from the original RK value of 0.5 to
a fluid to its molar volume v and the absolute temper- the value of 1.0. As a historical note, we point out that
ature T. the model presented by Clausius9 used an equivalent
exponent of e ) 1.
Another historical note is that a correlation quanti-
RT acR(T) tatively equivalent to eq 6 was proposed over 100 years
P) - (1)
v - b v(v + b) ago by Berthelot.10

B2Pc 54/128
* Tel: (617) 949-1727. Fax: (617) 949-1030. E-mail: Paul. ) 9/128 - (7)
RTc T 2
Mathias@AspenTech.com. R

10.1021/ie0340037 CCC: $25.00 © 2003 American Chemical Society

Published on Web 11/12/2003
7038 Ind. Eng. Chem. Res., Vol. 42, No. 26, 2003

Figure 1. Comparison between DIPPR correlations12 for the reduced second virial coefficient of various substances and the predictions
of RK EoS (e ) 0.5), - - -; RK EoS (e ) 1.0), s; and PR EoS (e ) 1), - -. The error bars for the RK EoS (e ) 1.0) show (0.05 in the reduced
second virial coefficient.

Figure 2. Comparison between DIPPR correlations12 for the reduced second virial coefficient of n-alkanes and the predictions of RK EoS
(e ) 1.0), s; SRK (ω ) 0.0), - -; and SRK (ω ) 1.0), - - -.

The modified RK EoS (e ) 1.0) is a better choice than
the original model if the EoS is used as the vapor-phase
EoS together with activity-coefficient models. In addi-
tion, we demonstrate that the simple correlation pro-
vides guidance for the high-temperature extrapolation
of R-functions and is reliable enough to question or
analyze correlations that significantly disagree with it,
thus serving as an independent tool for theoretical and
correlation analysis.
In the remaining sections of this paper, the proposed
correlation is first evaluated broadly against data for
various classes of compounds, and is then compared in
detail with data for three classes of compounds: non-
polar, polar, and hydrogen-bonding polar. The experi-
mental data and empirical correlations for B2 have been
taken from the DIPPR 801 Project,11 and specifically,
the data and correlations of DIADEM Version 1.512 have
been used.
Optimum Value for e
Figure 1 presents comparisons between data for the
reduced second virial coefficients of a wide variety of
substances and two forms of the RK EoS, with e ) 0.5
(original proposal1) and e ) 1.0. The data points are the
evaluated DIPPR correlations presented in DIADEM
Version 1.5.12 Examination of Figure 1 shows that the
reduced second virial coefficient at the critical temper-
ature (TR ) 1) is, on average, equal to about -0.34,
which is the prediction of the RK EoS. In addition, while
the RK EoS with e ) 0.5 provides a reasonable predic-
tion of the reduced second virial coefficient over the
temperature range of interest, the RK EoS with e ) 1.0
provides an improved prediction for a broad range of
species.
The equation analogous to eq 6 for the Peng-
Robinson13 EoS is as follows:

Figure 3. Second virial coefficient of helium. Comparison of the
RK EoS (e ) 0.0), Soave (ω ) -0.-39003) and the DIPPR
correlation to experimental data. See Table 1 for details on data
references.
Figure 4. Second virial coefficient of hydrogen. Comparison of
the RK EoS (e ) 0.2), Soave (ω ) -0.-21599) and the DIPPR
correlation to experimental data. See Table 1 for details on data
references.
B2Pc 0.45724
) 0.07780 - (8)
RTc T 1+e R Wilson2 and Soave3 approach offers no guidance on how
While the PR EoS is usually not written in the form of
the original RK EoS, it is instructive to directly compare
these two popular models in this way. Evaluation of the
predictions of the PR EoS in Figure 1 suggests that it
is slightly worse than the RK EoS for the prediction of
the high-temperature second virial coefficient, and
according to this criterion, the RK EoS is the preferred
of these two popular models.
Lundgaard and Mollerup14 have demonstrated that
the RK EoS gives more accurate high-pressure gas-
phase fugacities than the PR EoS, and this is another
related reason that the RK EoS is the preferred of these
two popular models.
Figure 1 suggests that eq 4 should be used to guide
the extrapolation of R-functions for TR > 1. Previous
practice has been to simply use the subcritical model
Ind. Eng. Chem. Res., Vol. 42, No. 26, 2003 7039
Figure 5. Second virial coefficient of neon. Comparison of the
RK EoS (e ) 0.5), Soave (ω ) 0.0) and the DIPPR correlation to
experimental data. See Table 1 for details on data references.
beyond the critical temperature or to use an extrapola-
tion function that smoothly goes to zero at high reduced
temperatures.15 Past practices have ignored the useful
insight and guidance of the second virial coefficient.
Evaluation for Nonpolar Substances
Figure 2 evaluates the predictions of the RK EoS (e
) 1.0) against the DIPPR correlations (DIADEM 1.512)
for the reduced second virial coefficients of the n-alkanes
(methane to n-decane) as representative nonpolar com-
pounds. This figure also evaluates the Soave3 RK (SRK)
model with values of the acentric factor (ω) equal to 0.0
(slightly less than methane, ω ) 0.01155) and equal to
0.5 (slightly greater than n-decane, ω ) 0.49233). In the
formalism of eqs 1-3, the R-function of the SRK model
is as follows.
R(TR) ) [1 + m(1 - TR0.5)]2 (9)
m ) 0.480 + 1.57ω - 0.176ω2 (10)
Analysis of Figure 2 indicates that the RK EoS (e ) 1.0)
provides, on average, the best prediction of the high-
temperature second virial coefficient. More importantly,
it provides guidance for the optimum extrapolation of
the R-function to high reduced temperatures. The
to extrapolate the R-function to temperatures above the
critical temperature, and we see that the extrapolation
of the R-function for substances such as n-decane yields
a second virial coefficient that is too positive. We
recommend that RK EoS with e ) 1 should be used as
this guide. It is interesting that while the subcritical
R-function depends on additional parameters such as
the acentric factor, the high-temperature R-function
seems to be a universal function of the reduced tem-
perature alone.
Figures 3-5 (see also Table 1) compare predictions
of the RK EoS, the Soave R-function,3 and the DIPPR
correlation12 to experimental data for the quantum
fluids, helium, hydrogen, and neon. The acentric factors
used in the Soave R-function3 are those reported by
DIPPR.12 Chueh and Prausnitz16 proposed a special
correlation using effective critical constants to capture
7040 Ind. Eng. Chem. Res., Vol. 42, No. 26, 2003
Figure 6. Comparison between DIPPR correlations12 for the reduced second virial coefficient of polar compounds and the predictions of
RK EoS (e ) 1.0)
Figure 7. Second virial coefficient of ethyl ether. Comparison of
the RK EoS (e ) 1.0) and the DIPPR correlation to experimental
data. See Table 1 for details on data references.
the quantum effects of these low-molecular-weight
fluids. Figures 3-5 demonstrate that these quantum
fluids also follow the universal reduced second virial
coefficient at the critical temperature, and that the
quantum character is demonstrated by component-
specific values of the exponent e. Helium, with the
strongest quantum effects, is best described by e ) 0,
while the optimum exponents for hydrogen and neon
are 0.2 and 0.5, respectively. The model proposed in this
work provides an objective way to extrapolate the
R-functions of the quantum fluids to high reduced
temperatures. In the case of neon where the lowest
temperature data are at TR ) 1.13, the proposed method
provides a reliable way to extrapolate the data down to
about TR ) 0.8.
Evaluation for Polar Substances
Figure 6 presents comparisons between the predic-
tions of the RK EoS (e ) 1.0) and the DIPPR correlations
Figure 8. Second virial coefficient of acetonitrile. Comparison of
the RK EoS (e ) 1.0) and the DIPPR correlation to experimental
data. See Table 1 for details on data references.
(DIADEM 1.512) for the reduced second virial coefficients
of representative polar compounds. It is remarkable that
the accuracy of the RK EoS (e ) 1.0) is as good for polar
compounds as it is for nonpolar compounds (Figure 2).
The average reduced second virial coefficient at the
critical temperature remains about -0.34. There is a
tendency of the predicted second virial coefficient to be
biased high as the temperature is decreased, and this
is to be expected because the specific interactions of
polar compounds will become dominant at lower tem-
peratures.
Figure 7 provides an example (ethyl ether) where the
simple model proposed here (RK EoS with e ) 1)
provides an essentially quantitative prediction of the
data.
Figure 8 presents a counter example (acetonitrile)
where the simple model proposed here (RK EoS with e
) 1) does not capture the experimental data. The model
predictions for B2 are significantly higher than the data
from several sources, and the agreement among the data
sets is good. Prausnitz and Carter17 indicate that
 Ind. Eng. Chem. Res., Vol. 42, No. 26, 2003 7041

Figure 9. Comparison between DIPPR correlations12 for the reduced second virial coefficient of hydrogen-bonding polar compounds and
the predictions of RK EoS (e ) 1.0).

Table 1. References for Experimental Data in Figures 3-5, 7, 8, 10, and 11

substance DIPPR ref no. ref substance DIPPR ref no. ref
ethyl ether (Figure 7) 1 TRC21 acetonitrile (Figure 8) 1 TRC21

phenol (Figure 10)
2 TRC21
4 Lambert et al.22
5 Strein et al.23
6 Zaalishvili et al.24
7 Zaalishvili et al.24
9 Stryjek26
10 Knoebel and Edmister27
12 Olf et al.28
1 Kudchadker et al.30
ethanol (Figure 11)
2 TRC21
3 Lambert et al.22
4 Prausnitz and Carter17
6 Olf et al.28
7 Demiriz et al.25
1 TRC21
2 TRC21
3 Dymond and Smith29
4 Kretschmer and Wiebe31

2 Opel32 5 Knoebel and Edmister27

hydrogen (Figure 4) 1 TRC21 6 Wilson et al.33
4 Dymond and Smith29 7 Smith and Srivastava34
helium (Figure 3) 1 TRC21 Neon (Figure 5) 2 Dymond and Smith29

2 McCarty35 4 Dymond and Smith29

4 Kestin et al.36 5 Dymond and Smith29
6 Dymond and Smith29
7 Kestin et al.36

acetonitrile forms dimers in the vapor phase, and this
is probably the reason the proposed simple model fails.
One value of the proposed simple model is to identify
species where vapor-phase association is significant.
Evaluation of Hydrogen-Bonding Substances
Figure 9 presents comparisons between the predic-
tions of the RK EoS (e ) 1.0) and DIPPR correlations
(DIADEM 1.512) for the reduced second virial coefficients
of representative hydrogen-bonding polar compounds.
It is even more remarkable that the accuracy of the RK
EoS (e ) 1.0) is maintained for hydrogen-bonding polar
compounds as it is for nonpolar and polar compounds.
In this case, the average reduced second virial coefficient
at the critical temperature is slightly above -0.34, but
-0.34 is still a good estimate. Two substances show
significant differences from the proposed correlation,
and we discuss these below.
Figure 9 suggests that the model predictions for
phenol at high temperatures (TR > 1) are significantly
lower than the DIPPR correlation. In Figure 10, the
proposed correlation and the DIPPR correlation are
compared against experimental data. There are no data
above the critical temperature of phenol, so both cor-
relations are extrapolations, but the RK-based model
should be preferred since it has been validated by
agreement with a broad range of substances.
Figure 9 suggests that the model predictions for
ethanol are low in the region of the critical temperature
and high for reduced temperatures above 1.8. Figure
11 provides an assessment of this observation. The
DIPPR correlation for ethanol12 is based upon several
compilations among which there is some disagreement
above TR ) 0.9. There is at least one of these com-
pilations34 that agrees with the prediction of the RK EoS
(e ) 1.0), and examination of Figure 9 shows that
ethanol does not follow the pattern of the other normal
alcohols. We conclude that the DIPPR correlation for
the second virial coefficient of ethanol needs to be
reassessed.
Figures 10 and 11 clearly show that the two-param-
eter corresponding-states correlation presented here will
7042 Ind. Eng. Chem. Res., Vol. 42, No. 26, 2003
Figure 10. Second virial coefficient of phenol. Comparison of the
RK EoS (e ) 1.0) and the DIPPR correlation to experimental data.
See Table 1 for details on data references.
Figure 11. Second virial coefficient of ethanol. Comparison of the
RK EoS (e ) 1.0) and the DIPPR correlation to experimental data.
See Table 1 for details on data references.
be biased high as the temperature decreases. This bias
will remain significant at higher reduced temperatures
as the polarity and hydrogen-bonding nature of the
substance increase. But it is also true that essentially
all substances, including polar and hydrogen-bonding
molecules, follow the two-parameter corresponding-
states correlation at relatively high temperatures (TR
> 0.8), and this finding is useful for the advancement
of applied thermodynamics.
Evaluation of Predictive Methods
Figure 12 presents a comparison between the pro-
posed correlation and the DIPPR correlation,12 and the
predictions of the McCann18 group-contribution method
for butyronitrile. The DIPPR correlation agrees very
well with the McCann18 predictions because it was fit
on this basis; no experimental data are available for
butyronitrile. The McCann group-contribution method
predicts that the reduced second virial coefficient of
butyronitrile at its critical temperature is -0.68. This
is far more negative than the value found for most other
Figure 12. Second virial coefficient of butyronitrile. Comparison
of the RK EoS (e ) 1.0) and the DIPPR correlation to group-
contribution predictive method of McCann.18
Figure 13. Second virial coefficient of ethanol. Comparison of
the RK EoS (e ) 1.0), the DIPPR correlation, and the Twu
R-function20 to experimental data. See Table 1 for details on data
references.
substances and is thus subject to doubt. But we should
also point out that B2(Tc)Pc/(RTc) for acetonitrile and
propionitrile are -0.56 and -0.70, respectively. It would
be useful and interesting if new experimental measure-
ments were made on the nitrile family to determine if
their reduced second virial coefficients at the critical
temperature are indeed so strongly negative. If the
experimental studies confirm the existing data, theo-
retical studies to determine why the specific interactions
of this family persist up such high reduced temperatures
would also be useful.
Evaluation of High-Temperature r-Functions
Many researchers have proposed R-functions to im-
prove the correlation of vapor pressures.19 Perhaps the
most effective of these correlations is the one proposed
by Twu et al.,20 which is shown here.
R(TR) ) TN(M-1)
R exp{L(1 - TNM
R )} (11)

Figure 13 compares the R-function of eq 6 and that
of the Twu correlation to experimental data for the
second virial coefficient of ethanol. Figure 13 indi-
cates that there is very little observable difference
between eqs 6 and 11 for the subcritical R-function (of
course, vapor pressure is extremely sensitive to the
R-function, so small differences are significant), but
the extrapolation from the R-function model of Twu
et al.20 gives a poor second virial coefficient at super-
critical temperatures. The conclusion of this work is that
new R-functions, which will provide both good vapor-
pressure predictions and accurate correlations for the
supercritical second virial coefficients, need to be in-
vented.
On the basis of the analysis in this paper, we propose
a new model for EoS R-functions
1 a1 b1 c1
R(TR) ) + + + (12)
TR a2 + TR b2 + TR c2 + T4R
N 2 3 (15) Boston, J. F.; Mathias, P. M. Proceedings of the 2nd
where N equals 1 for most fluids, and will be less than
for quantum fluids; a2, b2, and c2 are positive adjust-
able constants smaller than unity; and a1, b1, and c1
are adjustable constants subject to the constraint that
R(TR) ) 1 when TR ) 1. Limited investigation of eq 12
indicates that it provides an accurate prediction of pure-
component vapor pressures and an accurate description
of the supercritical second virial coefficient.
Conclusion
This work presents a two-parameter corresponding-
states correlation for the second virial coefficient that
has the following benefits for applied thermodynamics:
(i) It suggests an improved R-function for the Redlich-
Kwong EoS, which will be useful when this EoS is used
as the vapor-phase EoS together with activity-coefficient
models. (ii) The reduced second virial coefficient pre-
dicted by the Redlich-Kwong EoS at the critical tem-
perature (-0.341) agrees with data for most substances.
This suggests that the RK EoS should be preferred over
other popular cubic EoSs such as the Peng-Robinson13
model. (iii) It offers guidance for the high-temperature
extrapolation of R-functions based upon the Wilson2 and
Soave3 proposal. (iv) It offers a useful independent tool
to evaluate and interpret data and models for the second
virial coefficient.
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Received for review July 15, 2003
Revised manuscript received October 6, 2003
Accepted October 10, 2003
IE0340037