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group reported large positive partial molar volumes near the critical pressure, which is evidence that the system volume increases. While the partial molar volume is a macroscopic thermodynamic property, their measurements could be interpreted to show the cavitation of carbon dioxide molecules around methane molecule. A system, consisting of 999 carbon dioxide molecules and 1 molecule of methane, is used to represent the infinite dilution of methane in the supercritical carbon dioxide. As the addition of one methane molecule into 999 molecules gives a mixture 0,1% per volume, we assume that the critical point of the mixture remains the same. The correlation functions were determined by using the centre of each species, the carbon atom. We sampled the radial distribution function every 1000 configurations during MD simulations A sampling diagram from the radial distribution functions for Tr = 308.15 K over the densities ranging from 135.79 kg/m3 to 712.3 kg/m3 (critical density of CO2 is 468 kg/m3) for CO2-CH4 is shown in the Figure 9-1. The choppy appearance of the solute-solvent radial distribution function is common and has been observed in other infinite dilute solute mixtures simulations (Akiya and Savage, 2000b). The Figure 9-1 shows that the radial distributions functions exhibit a clear difference in appearance at subcritical and supercritical densities. The peak height decreases with increasing density from subcritical to supercritical ones and a second shell appears which is in agreement with theory (Clifford, 1999). Figure 9-2 shows the solute-solvent and solvent-solvent radial distribution functions for CO2-CH4 and CO2-CO2 pairs. Comparing the Figure 9-1 and Figure 8-4, we can see the trend of the RDF for carbon dioxide is strongly dependent on carbon dioxide bulk density compared to carbon dioxide-methane interaction. The height of the peaks and the contrasting 132PDF Image | MOLECULAR SIMULATION STUDIES IN THE SUPERCRITICAL REGION
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