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T=308.38 K (Eckert et al., 1986), while the partial molar volume of ethane at infinite dilution in a mixture of ethane and supercritical carbon dioxide is +350 cm3 /mol at P=73.97 bar and T=305.65 K. According to the classification of Debenedetti and Mohamed the above mixtures (CO2/naphthalene and CO2/ethane) belong to different types of supercritical mixtures; CO2/naphthalene is an ‘attractive’ mixture and CO2/ethane is a ‘weakly attractive’ mixture. The research group of X.Zhang (Zhang et al., 2002a; Zhang et al., 2002b) reported new data of PMVs of solutes in dilute supercritical solution. In their study, the PMVs of two polar solutes (H2O and H2S) in supercritical CO2 are negative, and a minimum can be observed in each PMV versus pressure curve at the pressure where isothermal compressibility of the fluid is largest. On the opposite site the PMVs of two non-polar solutes (H2 and CH4) are positive. For a solute (u) in solvent (V), the partial molar volume is defined as Vu V (4.6) n upT,nV with nu and nV being the numbers of moles of the solute and solvent, respectively. At infinite dilution, V = lim n V(n =1,n ,T,P)-V(n =0,n ,T,P) , so V can be computed in the isothermal-isobaric ensemble (NPT) from Monte Carlo simulations (Iwai et al., 1997). The computational method is not limited to Monte Carlo simulations; molecular dynamics simulations are equally applicable. Partial molar volume studies have been reported with this method (Stubbs et al., 2005) for naphthalene carbon dioxide mixture near the critical point with reasonable accuracy. An alternative approach is to use the Kirkwood-Buff (KB) fluctuation theory (Kang and Smith, 2007). This theory and its extension have been applied to study dilute supercritical fluid mixtures (Akiya and Savage, 2000a; Akiya and Savage, unu0up,T,nV us us u 64PDF Image | MOLECULAR SIMULATION STUDIES IN THE SUPERCRITICAL REGION
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