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9.1 INTRODUCTION The role of local density in influencing chemistry in supercritical fluids is a key element to our understanding of reaction dynamics. At temperatures appreciably higher than the critical temperature T>Tc, the solvent fluid itself is rather uniform and homogeneous and the isothermal compressibility of the fluid is not large. However, when for example a solute with large attractive solute-solvent interactions is placed in the fluid, the solvent molecules form a cluster surrounding the solute molecule. The number of solvent molecules participating in the cluster under such conditions is rather small and they form only the first solvation shells, in contrast to large clusters near the critical point In traditional solution thermodynamics, the process of solvation can be thought of two steps, finding space and occupying it. In previous chapter, we have seen the random movements of the molecules cause cavities (void spaces in the fluid) to form. The likelihood of a cavity being available to a solute particle is proportional to the density of the fluid; dense systems have few large cavities. According to conventional theories of solution, somebody expects the cavity must be sufficiently sized and shaped to allow a solute particle to move into the cavity during solvation process. The size of cavities is maximized close to the critical point. One expects that the size of cavitations should pass through a maximum with increasing pressure on a critical isotherm. 9.2 INFINITE DILUTION OF METHANE IN SUPERCRITICAL CARBON DIOXIDE Experimental observations (Zhang et al., 2002a) found that the addition of methane into supercritical carbon dioxide increases the volume of solution. Their 131PDF Image | MOLECULAR SIMULATION STUDIES IN THE SUPERCRITICAL REGION
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