Fluid Phase Equilibria 226 (2004) 109–120

Correlations for second and third virial coefficients of pure fluids

Long Meng, Yuan-Yuan Duan∗ , Lei Li
Key Laboratory of Thermal Science and Power Engineering, Department of Thermal Engineering, Tsinghua University, Beijing 100084, PR China

Received 23 June 2004; received in revised form 17 September 2004; accepted 27 September 2004
Available online 6 November 2004

Abstract

A modified form of the well-known Tsonopoulos correlation for second virial coefficients was developed based on the corresponding-states
principle. Comparisons with the new, high-quality experimental data and existing models show that the present correlation is more accurate,
reliable and satisfactory for nonpolar compounds. The results also show that the present work is roughly equivalent to the Tsonopoulos and
Weber correlations for second virial coefficients of polar fluids.
The Weber correlation for the third virial coefficients was also improved since it did not well represent the experimental data of nonpolar
gases. The new correlation gives a satisfactory fit for nonpolar compounds as the Orbey and Vera correlation did and can also accurately
represent the literature data for the third virial coefficients of polar fluids, which was well represented by the Weber correlation. The two
correlations for the second and third virial coefficients need the same additional parameters, such as the critical temperature, critical pressure,
acentric factor and reduced dipole moment.
© 2004 Elsevier B.V. All rights reserved.

Keywords: Virial coefficients; PVT; Nonpolar fluids; Haloalkanes; Polar fluids

1. Introduction virial coefficients usually contribute little to the densities of

The thermodynamic properties of gases may be easily cal-
culated from a knowledge of the virial coefficients and their
dependence on temperature. The density explicit virial equa-
tion of state, truncated after the third virial coefficient, is a
useful expression for calculating the thermodynamic proper-
ties of gases for reduced densities less than 0.5. The virial
coefficients are basic thermodynamic properties that repre-
sent the nonideal behavior of real gases. The importance of
the virial coefficients lies in the fact that they are related
directly to the interactions between molecules. The second
virial coefficient represents the departure from ideality due to
interactions between pairs of molecules, the third virial coef-
ficient gives the effects of interactions of molecular triplets,
and so on. All of the equilibrium gas-phase thermodynamic
properties can be calculated from the virial coefficients com-
bined with the ideal gas heat capacity. The fourth and higher
∗ Corresponding author. Tel.: +86 10 6279 6318; fax: +86 10 6277 0209.
E-mail address: yyduan@mail.tsinghua.edu.cn (Y.-Y. Duan).
gases and have relatively large uncertainties; therefore, most
effort has been focused on obtaining the second and third
virial coefficients.
Virial coefficients are usually derived from experimen-
tal measurements such as (a) PVT measurements, (b) speed
of sound measurements, (c) Joule–Thomson measurements,
(d) refractive index and relative permittivity measurements
and (e) vapor pressure and enthalpy of vaporization mea-
surements. In recent years, many researches have noted that
most older PVT data, which historically have been the main
source of the virial coefficients, were not corrected for physi-
cal adsorption effects and, therefore, the results for the second
virial coefficients are too negative at subcritical temperatures
along with larger errors in the experimental data for the third
virial coefficients.
Many kinds of correlations have been developed to cal-
culate the second virial coefficients. However, most suffer
from adsorption effects; consequently, the correlations must
be modified using new, high-quality experimental data. The
new correlation was developed to solve these problems and

0378-3812/$ – see front matter © 2004 Elsevier B.V. All rights reserved.
doi:10.1016/j.fluid.2004.09.023
110 L. Meng et al. / Fluid Phase Equilibria 226 (2004) 109–120

enhance the prediction accuracy and reliability based on the lowing widely used expression:
corresponding-states form, which accounts for nonspherical BPc
effects and dipole moment effects, while neglecting chemical Br = = f (0) (Tr ) + ωf (1) (Tr ) + f (2) (Tr ) (1)
RTc
associations and quantum effects.
For the third virial coefficients, due to the relatively large where
uncertainties in the experimental measurements, reliable data 0.330 0.1385 0.0121 0.000607
is scarce. Theoretical calculations with potential energy func- f (0) = 0.1445 − − − −
Tr Tr2 Tr3 Tr8
tions used are tedious and, for accurate results, require cor- (2a)
rections to the assumption of pairwise additivity which are at
0.331 0.423 0.008
best known only approximately. In this work, we have col- f (1) = 0.0637 + − − (2b)
lected and examined the limited amount of experimental third Tr2 Tr3 Tr8
virial coefficients now available and correlated them as best a
as we can. f (2) = (3)
Tr6
In 1957, Pitzer and Curl [1] proposed a very successful cor-
relation for the second virial coefficients of nonpolar gases, In Eq. (1), Tr (=T/Tc ) is the reduced temperature, Pc
which was the basis for several later correlations. O’Connell and Tc are the critical pressure and critical temperature,
and Prausnitz [2], Tsonopoulos [3,4], Tarakad and Danner R = 8.314472 J mol−1 K−1 is the universal gas constant, and
[5], Orbey [6], Weber [7], and Hayden and O’Connell [8] ω is the acentric factor. f(0) was obtained by fitting data for
presented various modified Pitzer–Curl correlations which small spherical molecules (ω = 0), such as argon. Then f(1)
refitted the coefficients of the Pitzer–Curl correlation, added was obtained from data for larger, nonspherical, nonpolar
polar and hydrogen bonding terms, applied new parameters, molecules (ω = 0), such as butane and octane. f(2) was ob-
and so on. However, most inevitably suffered from adsorption tained from data for nonhydrogen bonding polar molecules.
effects. A large amount of second virial coefficient data have Initially, these functions gave good agreement with data for B
become available since 1980, some of which were corrected of nonpolar gases, especially at reduced temperatures below
for physical adsorption effects, as mentioned in Dymond et 0.75. But more recent, more accurate values from PVT and
al. [9]. This work presents a new correlation using the se- speed of sound measurements have indicated that the result-
lected data of Dymond’s compilation for nonpolar gases, po- ing B’s were too negative at subcritical temperatures [9]. Eq.
lar haloalkanes and other nonhydrogen bonding polar gases. (3) is very important at reduced temperatures less than unity
For the third virial coefficients, Rowlinson [10] calcu- for representing the behavior of polar fluids. The parameter
lated the third virial coefficients of polar molecules from a is proposed to be a function of the reduced dipole moment
the Stockmayer potential [11], assuming pairwise additivity. µr , defined as follows:
Hirschfelder et al. [12] showed that it is a strong function of µ2 Pc
the reduced dipole moment for polar gases. Chueh and Praus- µr = (4)
1.01325Tc2
nitz [13] proposed a corresponding-states correlation which
does not allow calculations in the absence of data. Santis and where µ is the dipole moment in Debye
Grande [14] proposed a modified correlation which requires (1D = 3.33564 × 10−30 C m), Tc is in kelvins and Pc is
additional dipole polarizability of a molecule and Bondi’s in pascals. The second virial coefficients of polar com-
molecular volume [15]. The correlation of Pope et al. [16] pounds are more negative than those of nonpolar compounds
can only be used for compounds with an acentric factor not (for the same Tr and ω). Thus, a should be negative.
exceeding 0.1. In 1983, Orbey and Vera [17] provided a par- However, a usually becomes slightly positive for µr < 100.
ticularly simple and effective correlation for nonpolar gases. This spurious behavior arises from the fact that the measured
Van Nhu et al. [18] gave a correlation which was linked to the acentric factor is also affected by the presence of the dipole
second virial coefficients with additional knowledge of the moment, causing an overcorrection when calculating B.
virial coefficients of hard convex body molecule. The Bosse To solve this problem, Weber [7] deleted the last term
and Reich [19] correlation and the Besher and Lielmezs [20] in Eq. (2b), which is assumed to cause the problem. For
correlation were not generalized and had limited applicabil- the halogenated methanes and ethanes of interest in the
ity. Weber [7] presented a successful correlation for polar refrigeration industry, Tsonopoulos [4] and Weber [7] gave
haloalkanes adapting the model of Van Nhu et al. [18] using the following expressions:
the critical volume, but the result does not well represent the
aTsonopoulos = −2.188 × 10−11 µ4r − 7.831 × 10−21 µ8r (5)
experimental data for nonpolar fluids.
aWeber = −9 × 10−7 µ2r (6)

2. Second virial coefficient Tsonopoulos [3] also gave

aTsonopoulos = −2.140 × 10−4 µr − 4.308 × 10−21 µ8r (7)
For the gaseous second virial coefficient data, Tsonopou-
los [3,4] modified the Pitzer–Curl equation to give the fol- for other nonhydrogen bonding polar compounds.
 L. Meng et al. / Fluid Phase Equilibria 226 (2004) 109–120 111

Eq. (1) is also used in this work. For nonpolar fluids, Eqs.
(2a) and (2b) are redefined here as
0.30252 0.15668
f (0) = 0.13356 − −
Tr Tr2
0.00724 0.00022
− − (8)
Tr3 Tr8

0.15581 0.38183
f (1) = 0.17404 − +
Tr Tr2
0.44044 0.00541
− − (9)
Tr3 Tr8
Fig. 1. Br = f (0) (Tr ): (- - -) Tsonopoulos [3]; (· · ·) Pitzer–Curl [1]; (—)
Eqs. (8) and (9) were determined by fitting experimental data present work.
which mainly came from the compilation of Dymond et al.
[9]. The first term, f (0) , was determined by fitting the B data
for Ar, Kr and Xe, which have nearly zero acentric factors.
f (1) was determined by fitting the data for the C1 –C8 nor-
mal alkanes, oxygen, nitrogen, carbon dioxide and benzene.
Since the acentric factor of argon is not strictly equal to zero,
but is −0.0022, the final determination of f (0) was made by
iterative repetition. To reduce the adsorption effects, f (0) was
determined by heavily weighting the PVT data of Gilgen et
al. [21] and the speed of sound data of Estrada-Alexanders
and Trusler [22] for argon, since they are in excellent agree-
ment with each other. Comparison of our estimated results
with the recommended values for argon given by Dymond
et al. [9] shows that our correlation can represent B of argon Fig. 2. Deviations of measured second virial coefficient data for ar-
within the experimental uncertainties for 75 to 1000 K. Fur- gon (ω = −0.0022) from the present correlation: () Gilgen et al. [21];
thermore, our calculated results also are in excellent agree- ( ) Estrada-Alexanders and Trusler [22]; (- - -) Tsonopoulos [3]; (· · ·)
ment with those derived from the potential energy function Pitzer–Curl [1]; (-·-·-) Weber [7].
of Aziz and Slaman [23]. Hence, f (0) provides a more reli-
able basis for establishing f (1) and f (2) . The data of Gupta tainties, which led to their unreliable values. Fig. 2 shows that
and Eubank [24], which have been corrected for the physical the present results are in excellent agreement with the exper-
adsorption effects for butane, were weighted heavily to deter- imental data for argon over the entire range of temperatures,
mine f (1) . f (0) and f (1) decrease so steeply with decreasing while the other correlations are obviously too negative at
temperature for Tr < 0.75 that B could not be represented by subcritical temperatures. For example, the values calculated
cubic polynomials over the entire temperature range, so the
last terms in Eqs. (8) and (9) were added. In addition, a Tr−1
term was also added to f (1) . The three different correlations
for f (0) are compared in Fig. 1.
In Fig. 1, the values of B of our correlation are less neg-
ative than those of the Tsonopoulos correlation but lower
than those of the Pitzer–Curl correlation for Tr < 0.75, where
the adsorption effects are significant. The results show that
the present correlation effectively improves the Tsonopoulos
correlation with its too negative values at low temperatures.
The second virial coefficients for argon, methane, ethane,
butane and benzene, representative nonpolar compounds,
predicted by the present correlation are compared to experi-
mental data in Figs. 2–6. First, the selection of the literature
Fig. 3. Deviations of measured second virial coefficients for methane from
data was made taking account of the recommendation by
the present correlation: (
) Roe [25]; () Haendel et al. [26]; () Trusler
Dymond et al. [9]. Not all the data available in the litera- [27]; ( ) Michels et al. [28]; () Trappeniers et al. [29]; () Hou et al.
ture were shown in the figures, since some older data were [30]; (♦) Douslin et al. [31]; (䊉) Holleran [32]; (- - -) Tsonopoulos [3]; (· · ·)
suffered from physical adsorption effects or had large uncer- Pitzer–Curl [1]; (-·-·-) Weber [7].
112 L. Meng et al. / Fluid Phase Equilibria 226 (2004) 109–120
Fig. 4. Deviations of measured second virial coefficients for ethane from the
present correlation: (
) Estrada-Alexanders and Trusler [33]; ( ) Douslin
and Harrison [34]; (♦) Pompe and Spurling [35]; (䊉) Jaeschke [36]; (- - -)
Tsonopoulos [3]; (· · ·) Pitzer–Curl [1]; (-·-·-) Weber [7].
Fig. 5. Deviations of measured second virial coefficients for butane from
the present correlation: () Gupta and Eubank [24]; (- - -) Tsonopoulos [3];
(· · ·) Pitzer–Curl [1]; (-·-·-) Weber [7].
from the Tsonopoulos correlation are too negative below a
reduced temperature of 0.85, and this difference increases to
19 cm3 mol−1 at 81 K, where the uncertainty is expected to
be no more than 5 cm3 mol−1 . For methane (ω = 0.01142), a
nearly spherical molecule, the present work also gives very
Fig. 6. Deviations of measured second virial coefficients for benzene from
the present correlation: (
) Sherwood and Prausnitz [37]; ( ) Waelbroeck
[38]; () Bich et al. [39]; (♦) Bich et al. [40]; () Connolly and Kandalic
[41]; (- - -) Tsonopoulos [3]; (· · ·) Pitzer–Curl [1]; (-·-·-) Weber [7].
satisfactory results, while the other correlations have the same
problems as with argon: too negative for Tr < 1.6 and too posi-
tive for Tr < 1.6. The Tsonopoulos correlation gives a positive
deviation of 1.25 cm3 mol−1 at 673 K, where the experimen-
tal uncertainty is no more than 0.1 cm3 mol−1 . The data in
Fig. 3 also show that the present correlation for f (0) accu-
rately represents the B data for methane.
The comparison in Fig. 4 for ethane shows that the present
work appears to give the best results over the entire range,
except that it is slightly negative for Tr < 0.8, where the exper-
imental uncertainties are also large and only one set of data is
available. However, the Tsonopoulos correlation is too neg-
ative over the whole range, and the deviation increases con-
siderably as Tr decreases from 0.9 to 0.7. The Pitzer–Curl
correlation is also too negative at subcritical temperatures,
as is the Weber correlation at supercritical temperatures. The
data for butane in Fig. 5 also show that our correlation is in
excellent agreement with the experimental data of Gupta and
Eubank [24] which was successfully corrected for 90–95%
of the adsorption errors, while the errors of the Tsonopoulos
and Weber correlations increase at reduced temperatures less
than 0.75. A similar situation is found for benzene in Fig. 6
with the present correlation giving the best results, while the
other correlations have large deviations at low temperatures.
In addition, the four correlations for other kinds of nonpo-
lar fluids, such as Kr, CO2 , O2 , N2 , etc., were also compared
actually, just not shown with figures in this paper.
For polar fluids, the data analysis gave almost the same re-
lationship between f (2) and Tr as found earlier by Tsonopou-
los, so the form of Eq. (3) was used for f (2) . New B data were
used in the regression to obtain the optimum value for a of
polar haloalkanes, listed in Table 1, to establish the relation-
ship between a and µr . The second virial coefficient obtained
from the Stockmayer potential [11] for polar molecules is ex-
panded as
B(T ) = b{ϑ1 (T ) + ϑ2 (T )µ2r + ϑ3 (T )µ4r + ϑ4 (T )µ6r + · · ·}
(10)
Weber [7] indicated that the first two terms of Eq. (10) are not
sufficient to give the optimum value for a of strongly polar
fluids, therefore, µ4r and µ6r terms were added to correlate the
optimum value for a of both weakly and strongly polar fluids.
Since the 1990s, a large amount of new experimental data
have been reported for R22, R32, and R134a. Accordingly,
these three substances were heavily weighted in developing
a new fit for haloalkanes:
a = −1.1524 × 10−6 µ2r + 7.2238 × 10−11 µ4r
− 1.8701 × 10−15 µ6r (11)
In addition, since we took ketones, aldehyde, acetonitrile,
and ethers as nonhydrogen bonding compounds, the data for
propanone, acetonitrile, acetaldehyde, diethyl ether, etc. were
used to generate a different dependence of a as a function of
 L. Meng et al. / Fluid Phase Equilibria 226 (2004) 109–120 113

Table 1
Optimum values and RMSD for some polar fluids
Substance µr Optimum a RMSD (cm3 mol−1 )
Present work Tsonopoulos Weber
R11 3.97 0.00614 33.4 35.3 28.2
R12 7.16 0.00171 10.2 16.9 8.9
R13 10.92 0.00856 4.7 6.0 4.2
R22 76.76 −0.00469 8.3 11.9 14.2
R23 144.77 −0.01469 4.9 3.7 3.6
R32 180.95 −0.02586 7.8 5.4 7.9
R40 136.80 −0.01053 10.7 10.2 13.0
R41 198.08 −0.05129 5.7 6.3 8.9
R114 7.93 0.00264 23.3 35.4 18.3
R115 6.68 0.01404 11.0 13.5 12.2
R141b 77.50 −0.00132 54.8 37.0 7.7
R142b 109.29 −0.00452 22.6 15.3 21.4
R123 31.84 −0.00091 6.5 22.8 76.2
R124 49.36 −0.00069 10.8 5.7 21.3
R125 75.82 0.00069 7.7 4.5 4.5
R134a 121.17 −0.00740 3.0 6.2 3.7
R143a 169.91 −0.01703 6.4 14.9 11.4
R152a 152.76 −0.01661 22.0 9.9 7.3
R227ea 43.58 0.00245 12.5 7.3 7.1
R236ea 25.90 −0.00078 21.6 25.7 28.1
Propanone 149.03 −0.03410 38.1 35.3
2-Butanone 111.29 −0.02313 65.5 74.1
2-Pentanone 84.42 −0.01803 163.6 142.8
3-Pentanone 92.84 −0.01308 65.9 76.9
Dimethyl ether 55.98 −0.01752 64.2 54.2
Diethyl ether 21.80 −0.00449 63.8 44.7
Diisopropyl ether 14.26 −0.00277 68.7 71.0
Ethanol 191.44 −0.04482 38.0 36.7
Acetonitrile 249.48 −0.12116 175.5 178.5

µr for other nonassociated polar compounds:
a = −3.0309 × 10−6 µ2r + 9.503 × 10−11 µ4r
− 1.2469 × 10−15 µ6r
Here we roughly ignored the associating effects of nonhy-
drogen bonding compounds. Both equations are plotted in
Fig. 7. The values of a for haloalkanes are mostly positive
for µr < 100 as already mentioned above. Although we have
developed the most reliable correlations for f (0) and f (1) ,
approaching the true values, Eq. (3) is perhaps not the best
polynomial form since f (2) is also expected to be effected by
(12) the dipole’s direction and location within the molecule which
are important at low µr values. The predicted second virial
coefficients of R22, R32, R134a and R123 are compared with
experimental data in Figs. 8–11. The results show how the

Fig. 7. Dependence of the polar parameter a on the reduced dipole moment
µr : (—) Eq. (11); (- - -) Eq. (12); ( ) optimum values for haloalkanes; (䊉)
optimum values for other nonhydrogen bonding polar fluids.
Fig. 8. Deviations of measured second virial coefficients for R22 from the
present correlation: (
) Zander [42]; ( ) Lisal et al. [43]; () Schramm and
Weber [44]; () Natour et al. [45]; (♦) Schramm et al. [46]; () Demiriz et
al. [47]; (䊉) Haendel et al. [48]; () Haworth and Sutton [49]; () Esper et
al. [50]; (- - -) Tsonopoulos [3]; (-·-·-) Weber [7].
114 L. Meng et al. / Fluid Phase Equilibria 226 (2004) 109–120
Fig. 9. Deviations of measured second virial coefficients for 32 from the
present correlation: (
) Qian et al. [51]; ( ) Sato et al. [52]; () Defibaugh et
al. [53]; (♦) Sun et al. [54]; () Weber and Goodwin [55]; (- - -) Tsonopoulos
[3]; (-·-·-) Weber [7].
Fig. 10. Deviations of measured second virial coefficients for R134a from
the present correlation: (♦) Schramm et al. [46]; (䊉) Tillner-Roth and Baehr
[56]; ( ) Qian et al. [57]; () Bignell and Dunlop [58]; () Goodwin and
Moldover [59]; () Beckermann and Kohler [60]; (
) Weber [61]; (- - -)
Tsonopoulos [3]; (-·-·-) Weber [7].
Fig. 11. Deviations of measured second virial coefficients for R123 from
the present correlation: () Schramm and Weber [44]; ( ) Goodwin and
Moldover [62]; (—) Weber’s equation [63]; (- - -) Tsonopoulos [3]; (-·-·-)
Weber [7].
present correlation is obviously better than the previous cor-
relations.
The present predicated results agree well with the experi-
mental data even at low temperatures for the polar molecules
in Figs. 8–11. The Tsonopoulos correlation has negative er-
rors while the Weber correlation has positive errors at low
temperatures, which are similar to the results for nonpolar
fluids. These errors are probably caused by the inaccuracy of
the nonpolar terms in their correlations.
The root mean square deviations (RMSD) for 28 kinds
of polar molecules, calculated using the data in Dymond et
al. [9], are listed in Table 1. These results show that in gen-
eral, all three correlations are roughly equivalent for polar
haloalkanes with most errors in line with the estimated exper-
imental uncertainties. The deviations are significantly greater
than the estimated uncertainties for only R11 and R141b, and
both this work and Tsonopoulos correlation have large errors
in calculating the data for other nonhydrogen bonding polar
molecules. So, these results suggest that although the current
correlation uses modified nonpolar terms, this work does not
give significantly improved predictions for the second virial
coefficients of polar fluids due to the weakness of Eq. (3).
3. Third virial coefficient
Since the experimental values of the third virial coeffi-
cients are often very much in error and scarce because of
inherent difficulties in avoiding systematic measurement and
evaluation errors, general correlations which directly fit the
data are not appropriate. The Van Nhu et al. [18] model is
often considered to be better than most for correlating the
experimental data for the third virial coefficients with the ad-
vantage that the uncertainty in the individual coefficients, B
and C, is offset to a large extent by their close association
when the truncated virial equation is used to represent the
PVT data. Weber [7] successfully simplified the model using
the critical volume as a parameter:
C = Ch + (B − Bh )2 δc ϑ(Tr ) (13)
where Bh = b, Ch = 0.625b2 , b = 0.36vc , δc is a function of
µr and ϑ(Tr ) is a strong functions of Tr , and vc is the criti-
cal volume. However, the additional critical volume param-
eter makes the use of the truncated virial equation awkward.
Different pieces of information are required depending on
whether the equation is truncated after the second or after the
third virial coefficient. To solve this problem, Bh and Ch are
substituted into Eq. (13) and then both sides of the equation
are multiplied by (Pc /RTc )2 . Eq. (13) is then transformed into
the corresponding-states form:
Cr = 0.081Zc2 + (Br − 0.36Zc )2 δc ϑ(Tr ) (14)
where Br = B(Pc /RTc ), Cr = C(Pc /RTc )2 and Zc = Pc vc /RTc .
Since the critical compressibility factors of most compounds
are in the range of 0.23–0.29, particularly 0.25–0.27 for
 L. Meng et al. / Fluid Phase Equilibria 226 (2004) 109–120 115

haloalkanes, we simply let Zc = 0.26 in Eq. (14). Thus, the

critical volume parameter is not needed, and the character-
istic information required for calculating C is the same as
those required for calculating B. Therefore, the new corre-
lation representing the third virial coefficients for nonpolar
gases and haloalkanes is
Cr = c0 +(Br − c1 )2 [f0 (Tr ) + µ4r f1 (Tr )] (15)
where c0 = 5.476 × 10−3 , c1 = 0.0936;


3334.145 3389.848 1149.580
f0 (Tr ) = 1094.051− + −
Tr0.1 Tr0.2 Tr0.3
(16)
Fig. 12. Third virial coefficients of argon: (♦) Holborn and Otto [64]; ()

 Michels et al. [65]; () Whalley et al. [66]; () Kalfoglou and Miller [67];
0.85902 (䊉) Gilgen et al. [21]; ( ) Tanner and Masson [68]; () Onnes and Crom-
f1 (Tr ) = 2.0243 − × 10−10 (17)
Tr melin [9]; () Crain and Sonntag [69]; () Michels et al. [70]; (
) Estrada-
Alexanders and Trusler [71]; (—) Eq. (15); (- - -) Orbey and Vera [17]; (-·-·-)
The first term, f0 (Tr ), was determined by fitting the C data for Weber [7].
argon, carbon dioxide, methane, nitrogen and benzene, which
have zero reduced dipole moments. f1 (Tr ) was determined by
fitting the data for some haloalkanes, such as R134a, R143a,
R152a, R32 and R23. Noted that f0 (Tr ) is equal to 0.174 when
the reduced temperature is equal to unity, which is in agree-
ment with the calculated value at the critical temperature in
the Weber correlation. Weber suggested that the polar term
should be correlated using the cube of the reduced dipole
moment, however, we got better results with the quartic of
the reduced dipole moment which is similar to the case of
Van Nhu et al. [18]. Although f1 (Tr ) was somewhat arbitrary,
the results show that it accurately represents the experimen-
tal data of haloalkanes. Furthermore, as Weber also found,
the location of the maximum in C shifts to lower temper-
atures with increasing reduced dipole moment. In fact the
Fig. 13. Third virial coefficients of nitrogen: (♦) Roe [25]; () Zhang et al.
present correlation describes this phenomenon so well that
[72]; () Michels et al. [73]; () Holborn and Otto [64]; (䊉) Michels et al.
f1 (Tr ) need not be a function of µr as was necessary in the [74]; ( ) Canfield et al. [75]; () Onnes and Van Urk [9]; () Hoover et al.
Weber correlation. The calculated results for the third virial [76]; () Duschek et al. [77]; (
) Otto et al. [78]; (—) Eq. (15); (- - -) Orbey
coefficients for argon, carbon dioxide, nitrogen and methane, and Vera [17]; (-·-·-) Weber [7].
as classical nonpolar gases, are shown in Figs. 12–15.
Figs. 12–15 show that Eq. (15) agrees well with the Orbey
and Vera correlation in giving a satisfactory representation of
C for nonpolar fluids within the experimental uncertainties.
Since the equation of Weber was established to represent
small polar substances, it does not describe these nonpolar
substances well. For example, visible positive deviations can
be seen for Tr = 1.0–1.5 with obvious negative deviations for
Tr > 1.5.
The results obtained with the present correlation for R23,
R32, R134a, R143a, R152a, R125 are shown together with
the Weber correlation and the Orbey and Vera correlation
in Figs. 16–21. Figs. 16–21 show that Eq. (15) is in excel-
lent agreement with the Weber correlation which accurately
represents the data for polar haloalkanes within the experi-
Fig. 14. Third virial coefficients of carbon dioxide: (♦) Patel et al. [79]; ()
mental uncertainties. Since the Orbey and Vera correlation
Vukalovich and Masalov [80]; () Glowka [81]; () Pfefferle et al. [82];
is not for polar fluids, their results are not as good as those (䊉) Holste et al. [83]; ( ) Butcher and Dadson [84]; () Duschek et al.
of the present work. Thus, Eq. (15) incorporates the advan- [85]; () Katayama et al. [86]; () Michels and Michels [87]; (
) Holste et
tages of the other two correlations to represent the third virial al. [88]; (—) Eq. (15); (- - -) Orbey and Vera [17]; (-·-·-) Weber [7].
116 L. Meng et al. / Fluid Phase Equilibria 226 (2004) 109–120
Fig. 15. Third virial coefficients of methane: (♦) Kleinrahm et al. [89]; ()
Michels and Nederbragt [90]; () Trusler et al. [91]; () Dymond et al. [9];
(䊉) Haendel et al. [26]; ( ) Hoover et al. [92]; () Schamp et al. [93]; ()
Douslin et al. [31]; () Roe [25]; (
) Pope et al. [16]; ( ) Trappeniers et
al. [29]; ( ) Holleran [32]; (—) Eq. (15); (- - -) Orbey and Vera [17]; (-·-·-)
Weber [7].
Fig. 16. Third virial coefficients of R23: ( ) Timoshenko et al. [94]; ()
Rasskazov et al. [95]; (
) Lange and Stein [96]; (♦) Yokozeki et al. [97];
(—) Eq. (15); (- - -) Orbey and Vera [17]; (-·-·-) Weber [7].
coefficients for both nonpolar fluids and polar haloalkanes.
However, the predictions for weakly polar fluids are not as
good. The results for R124 as an example, for which the value
of µr is only 49.36, are shown in Fig. 22. The result shows
Fig. 17. Third virial coefficients of R32: (♦) Sato et al. [52]; (䊉) Kuznetsov
and Los [98]; ( ) Zhang et al. [99]; () Yokozeki et al. [97]; () Fu et al.
[100]; (
) Defibaugh et al. [53]; (—) Eq. (15); (- - -) Orbey and Vera [17];
(-·-·-) Weber [7].
Fig. 18. Third virial coefficients of R134a: ( ) Qian et al. [57]; ()
Yokozeki et al. [97]; (
) Goodwin and Moldover [59]; (—) Eq. (15); (- -
-) Orbey and Vera [17]; (-·-·-) Weber [7].
Fig. 19. Third virial coefficients of R143a: (♦) Yokozeki et al. [97]; ( )
Weber and Defibaugh [101]; () Nakamura et al. [102]; (
) Gillis [103];
(—) Eq. (15); (- - -) Orbey and Vera [17]; (-·-·-) Weber [7].
that none of the three correlations can accurately represent
the experimental data derived from the speed of sound mea-
surements of Gillis [103]. The errors are probably due to poor
representation of B for weakly polar fluids since the determi-
nation of C was related to B as expressed by Eq. (15). It is
Fig. 20. Third virial coefficients of R152a: () Yokozeki et al. [97]; ( )
Tamatsu et al. [104]; (
) Gillis [103]; (—) Eq. (15); (- - -) Orbey and Vera
[17]; (-·-·-) Weber [7].
 L. Meng et al. / Fluid Phase Equilibria 226 (2004) 109–120
Fig. 21. Third virial coefficients of R125: (♦) Yokozeki et al. [97]; ( ) Ye
et al. [105]; () Gillis [103]; (
) Boyes and Weber [106]; (䊉) Duarte-Garza
et al. [107]; (—) Eq. (15); (- - -) Orbey and Vera [17]; (-·-·-) Weber [7].
interesting to note that the predicted value is in good agree-
ment with the only data point of Boyes and Weber [108], with
only one other set of data available.
Eq. (15) has a positive minimum at Tr equal to about 5
for nonpolar molecules, which is certainly wrong for high
reduced temperatures. However, this error does not contribute
to a large numerical error in C here. The Weber correlation has
a similar problem, which we attribute to the assumption that
Bh (T) and Ch (T) are constants, and neglecting an important
term of the Van Nhu model for high temperatures. As Van
Nhu emphasized, his model is probably wrong for the limit
of Tr → ∞.
The correlation was also compared to data for strongly
polar and associating substances. The results for ammonia
(Br obtained using Eq. (10)) are shown in Fig. 23. Surpris-
ingly, although no experimental data for low temperatures are
available, Eq. (15) is in good agreement with the experimen-
tal data above 300 K. However, all three correlations cannot
give satisfactory predictions for water, which indicates that a
association term should be added to Eq. (15) to improve the
prediction.
Fig. 22. Third virial coefficients of R124: (
) Gillis [103]; (䊉) Boyes and
Weber [108]; (—) Eq. (15); (- - -) Orbey and Vera [17]; (-·-·-) Weber [7].
117
Fig. 23. Third virial coefficients of ammonia: ( ) Adam and Schramm
[109]; (
) Glowka [81]; (—) Eq. (15); (- - -) Orbey and Vera [17]; (-·-·-)
Weber [7].
4. Discussion
The importance of the virial coefficients lies in the fact
that they are very useful for representing the PVT behavior
of real gases at low densities. Although good-quality PVT
measurements in the gas phase have an experimental accu-
racy of about 0.1% in density, corresponding-states type cor-
relations, including the present one and Weber’s work, do not
normally achieve this accuracy. The virial equation of state,
truncated after the third virial coefficient, can provide a very
good fit to precise PVT data for densities up to about 0.5ρc
for nonpolar gases. For polar gases, this maximum density
decreases to about 0.25ρc or even lower.
The accuracies of the present correlation and the Weber
correlation for the nonpolar gases argon and nitrogen and
polar gas R134a are shown in Figs. 24–26. For these three
gases, the present correlation is better than Weber’s in rep-
resenting the gas-phase densities over the whole range. Esti-
mates for the density error for the nonpolar gases methane,
ethane, propane, butane, carbon dioxide and oxygen and the
polar gases R143a, R125a, R32 and R22 are shown in Table 2.
For most nonpolar fluids and polar haloalkanes, the present
Fig. 24. Density deviations of argon from EOS of Tegeler et al. [110]; present
work: () 105.15 K, (䊉) 181.15 K, () 303.15 K, ( ) 453.15 K; Weber [7]:
(
) 105.15 K, ( ) 181.15 K, () 303.15 K, ( ) 453.15 K.
118 L. Meng et al. / Fluid Phase Equilibria 226 (2004) 109–120

Table 2
Estimated density uncertainties of nonpolar and polar fluids
Temperature range Density uncertainty of nonpolar fluids (%) Density uncertainty of polar fluids (%)

Pr < 0.6 0.6 < Pr < 0.7 Pr > 0.7 Pr < 0.3 0.3 < Pr < 1.0
Tr = 0.6–0.9 0.2 – – 0.2 –
Tr = 0.9–1.2 0.2 0.3 2.0 0.5 2
Tr >1.2 0.1 0.2 1.0 0.5 2

and the nonpolar term f (1) very successfully represent the

Fig. 25. Density deviations of nitrogen from EOS of Span et al. [111]; present
work: () 78.15 K, (䊉) 128.15 K, () 253.15 K; Weber [7]: (
) 78.15 K,
( ) 128.15 K, () 253.15 K.
best available data within the experimental imprecision for
Tr = 0.5–6 or higher. The results give confidence that the
present forms for f (0) and f (1) are closer to the “final” form.
The representation of the polar term, f (2) , is not as good as
that of the nonpolar terms as evidenced by the spurious be-
havior (positive value of a) for weakly polar fluids. Further
work is needed to improve the model for f (2) without affect-
ing f (0) and f (1) , and extend the correlation to associated
substances.
For the third virial coefficients, Eq. (13) gives an implicit
dependence on ω through the second virial coefficient, so the
reasonable form of the empirical correlation should be
Cr = f (0) (Tr ) + ω2 f (1) (Tr ) + f (2) (Tr , µr ) (18)
where ω2 is used instead of ω. Eq. (18) accurately represents
nonpolar fluids; however it does not work well for polar fluids,
which was the same as the correlation for B. Perhaps B and C
both have the same unknown mechanism that requires further
work which should start with the second virial coefficient.
Additional work is also needed to provide improved mod-
els for mixtures. The extension of the correlation to mixtures
is feasible and would involve only one interaction coefficient
per binary system.

List of symbols
a parameter of polar contribution to B, f (2)
B, C second and third virial coefficients
f (0) , f (1) , f (2) dimensionless functions of Tr in B correla-
tions
Fig. 26. Density deviations of R134a from EOS of Tillner-Roth and P pressure
Baehr [112]; present work: () 228.15 K, (䊉) 298.15 K, () 338.15 K, R universal gas constant
( ) 373.15 K, () 449.15 K; Weber [7]: (
) 228.15 K, ( ) 298.15 K, () T temperature
338.15 K, ( ) 373.15 K; ( ) 449.15 K.

correlation is roughly equivalent to the Weber correlation in Greek letters

predicting the gas-phase nonideality. The Weber prediction µ dipole moment, in Debye
is often slightly better than this work near the critical temper- 1D = 3.33564 ×10−30 C m
ature and worse at supercritical temperatures. µr reduced dipole moment
ω acentric factor

5. Conclusions Subscripts
c critical property
A modified correlation was developed for the second and cal calculated result
third virial coefficients of nonpolar and polar fluids. For exp experimental result
the second virial coefficients, the simple spherical term f (0) r reduced property (not including µr )
 L. Meng et al. / Fluid Phase Equilibria 226 (2004) 109–120
Acknowledgements
This work was supported by the National Natural Science
Foundation of China (No. 50225622) and the Fok Ying Tung
Education Foundation (No. 81051).
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