Abstract Introduction Second virial coefficient Third virial coefficient Discussion Conclusions Acknowledgements References

The new correlation Tsonopoulos to the second virial coefficient was developed based on the corresponding-states principle.

The present correlation is more accurate, reliable and satisfactory for nonpolar compounds.

The new correlation Weber can accurately represent the literature data for the third virial coefficients of polar fluids.

Both correlations for the second and third virial coefficient need additional parameters as the critical temperature, critical pressure, acentric factor and low dipole moment.

The virial coefficients are basic thermodynamic properties that represent the nonideal behavior of real gases.

The second virial coefficient represents the departure from ideality due to interactions between pairs of molecules.

The third virial coefficient gives the effects of interactions of molecular triplets.

The fourth virial coefficient usually contribute little to the densities of gases and have relatively large uncertainties.

Virial coefficients are usually derived from experimental measurements such as :

PVT measurements. Speed of sound measurements. JouleThomson measurements. Refractive index and relative permittivity measurements. Vapor pressure and enthalpy of vaporization measurements.

The new correlation was developed to enhance the prediction accuracy and reliability based on the corresponding-states form, which accounts for nonspherical effects and dipole moment effects, while neglecting chemical associations and quantum effects.

For the third virial coefficients reliable data is scarce and for accurate results, require corrections to the assumption of pairwise additivity.

In this work we have taken the limited amount of experimental third virial coefficients now available and correlated them as best as we can.

For the gaseous second virial coefficient data, Tsonopoulos modified the PitzerCurl equation to give the following widely used expression:

=
where,

= f (0)( ) + f (1)( ) + f (2)( )

(1)

f (0) = 0.1445 f (1) = 0.0637 + f

(2)

0.330 0.1385 0.121 0.000607 2 3 8 0.331 2

(2a)

0.423 3

0.008 8

(2b)

(3)

Eq. (3) is very important at reduced temperatures less than unity for representing the behavior of polar fluids.

The parameter a is proposed to be a function of the reduced dipole moment r defined as follows:

r =

2 2 1.01325

(4)

The second virial coefficients of polar compounds are more negative than those of nonpolar compounds (for the same Tr and ). Thus, a should be negative. However, a usually becomes slightly positive for r < 100.

For the halogenated methanes and ethanes of interest in the refrigeration industry, Tsonopoulos and Weber gave the following expressions: a Tsonopoulos = 2.188 1011 r4 7.831 1021 r8 a Weber = 9 107 r2

(5) (6)

Tsonopoulos also gave a Tsonopoulos = 2.140 104 r 4.308 1021 r8 for other nonhydrogen bonding polar compounds. (7)

Eq. (1) is also used in this work.

For nonpolar fluids, Eqs. (2a) and (2b) are redefined here as

f (0)

0.30252 0.15668 0.00724 0.00022 = 0.13356 2 3 8

(8)

0.15581 (1) f = 0.17404

0.38183 0.44044 0.00541 + 2 3 8

(9)

Fig. 1. Br = f (0)(Tr): (- - -) Tsonopoulos [3]; ( ) PitzerCurl [1]; ()present work.

Fig.2. Deviations of measured second virial coefficient data for argon ( =0.0022) from the present correlation: () Gilgen et al. [21]; (O) Estrada-Alexanders and Trusler [22]; (- - -) Tsonopoulos [3]; ( ) PitzerCurl [1]; (---) Weber [7].

Fig. 3. Deviations of measured second virial coefficients for methane from the present correlation: () Roe [25]; () Haendel et al. [26]; () Trusler [27]; () Michels et al. [28]; () Trappeniers et al. [29]; () Hou et al. [30]; () Douslin et al. [31]; () Holleran [32]; (- - -) Tsonopoulos [3]; ( ) PitzerCurl [1]; (---) Weber [7].

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]; () 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]; ( ) PitzerCurl [1]; (---) Weber [7].

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]; ( ) PitzerCurl [1]; (---) Weber [7].

Substance
R11 R12 R13 R22 R23 R32 R40 R41 R114 R115 R141b R142b R123 R124 R125 R134a R143a R152a R227ea R236ea Propanone 2-Butanone 2-Pentanone 3-Pentanone Dimethyl ether Diethyl ether Diisopropyl ether Ethanol Acetonitrile

r
3.97 7.16 10.92 76.76 144.77 180.95 136.80 198.08 7.93 6.68 77.50 109.29 31.84 49.36 75.82 121.17 169.91 152.76 43.58 25.90 149.03 111.29 84.42 92.84 55.98 21.80 14.26 191.44 249.48

Optimum a
0.00614 0.00171 0.00856 0.00469 0.01469 0.02586 0.01053 0.05129 0.00264 0.01404 0.00132 0.00452 0.00091 0.00069 0.00069 0.00740 0.01703 0.01661 0.00245 0.00078 0.03410 0.02313 0.01803 0.01308 0.01752 0.00449 0.00277 0.04482 0.12116

RMSD (cm3 mol-1)

Present work
33.4 10.2 4 .7 8 .3 4 .9 7 .8 10.7 5 .7 23.3 11.0 54.8 22.6 6 .5 10.8 7 .7 3 .0 6 .4 22.0 12.5 21.6 38.1 65.5 163.6 65.9 64.2 63.8 68.7 38.0 175.5

Tsonopoulos
35.3 16.9 6.0 11.9 3.7 5.4 10.2 6.3 35.4 13.5 37.0 15.3 22.8 5.7 4.5 6.2 14.9 9.9 7.3 25.7 35.3 74.1 142.8 76.9 54.2 44.7 71.0 36.7 178.5

Weber
28.2 8.9 4.2 14.2 3.6 7.9 13.0 8.9 18.3 12.2 7.7 21.4 76.2 21.3 4.5 3.7 11.4 7.3 7.1 28.1

Fig. 7. Dependence of the polar parameter a on the reduced dipole moment r: () Eq. (11); (- - -) Eq. (12); () optimum values for haloalkanes; () 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]; () Haendel et al. [48]; () Haworth and Sutton [49]; () Esper et al. [50]; (- -) Tsonopoulos [3]; (---) Weber [7].

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]; () 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].

The results for 28 kinds of polar molecules listed in Table 1 show that in general, all three correlations are roughly equivalent for polar haloalkanes. And both this work and Tsonopoulos correlation have large errors in calculating the data for other nonhydrogen bonding polar molecules. So, this work does not give significantly improved predictions for the second virial coefficients of polar fluids due to the weakness of Eq. (3).

Fig. 11. Deviations of measured second virial coefficients for R123 from the present correlation: () Schramm and Weber [44]; () Goodwin and Moldover [62]; () Webers equation [63]; (- - -) Tsonopoulos [3]; (---) Weber [7].

The Van Nhu model is often considered to be better than most for correlating the experimental data for the third virial coefficients.

Weber successfully simplified the model using the critical volume as a parameter:

C = + ( )2 ( )

(13)

where = b, = 0.625 2 , b = 0.36 , is a function of and ( ) is a strong functions of , and is the critical volume.

As virial equation may be truncated after the second or after the third virial coefficient, and are substituted into Eq. (13) and both sides of the equation are multiplied by ( )2 , so:

= 0.081 2 + ( 0.36 )2 ( ) where, = B ( / ) = C ( )2 = /R

(14)

In Eq. (14), = 0.26. Thus, the critical volume parameter is not needed.

Therefore, the new correlation representing the third virial coefficients for nonpolar gases and haloalkanes is
4 Cr = c0 + (Br c1)2 [f0 (Tr) + r f1 (Tr)]

(15)

where c0 = 5.476 103, c1 = 0.0936 ;

3334.145 3389.848 1149.580 f0 (Tr) = 1094.051 T0.1 + T0.2 T0.3 r r r

(16)

f1 (Tr) = ( 2.0243

0.85902 ) Tr

1010

(17)

The first term, f0 (Tr), was determined by fitting the C data for argon, carbon dioxide, methane, nitrogen and benzene, which have zero reduced dipole moments.

Noted that f0 (Tr) is equal to 0.174 when the reduced temperature is equal to unity.

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.

f1 (Tr) was determined by fitting

the data for some haloalkanes, such as R134a, R143a, R152a, R32 and R23.

Although f1 (Tr) was somewhat arbitrary, the results show that it accurately represents the experimental data of haloalkanes.

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.

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 0.5 c for nonpolar gases.For polar gases, this maximum density decreases to about 0.25 c 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. 2426.

For argon, nitrogen and R134a the present correlation is better than Webers in representing the gas-phase densities over the whole range. Estimates 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 correlation is roughly equivalent to the Weber correlation in predicting the gas-phase nonideality.

The Weber prediction is often slightly better than this work near the critical temperature and worse at supercritical temperatures.

A modified correlation was developed for the second and third virial coefficients of nonpolar and polar fluids. For the second virial coefficients, the simple spherical term f (0) and the nonpolar term f (1) very successfully represent the best available data within the experimental imprecision for Tr = 0.56 or higher. For the third virial coefficients, Eq. (13) gives an implicit dependence on through the second virial coefficient, so the reasonable form of the empirical correlation should be = f (0)(Tr ) + 2 f (1) (Tr) + f (2) (Tr , r ) (18)

Eq. (18) accurately represents nonpolar fluids; however it does notwork well for polar fluids, which was the same as the correlation for B.

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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