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22 To see the relationship between V # and pressure, consider the case where the transition state volume is smaller than that of the reactantsV # . In this case an increase in pressure would shift the assumed equilibrium between the transition state and reactants toward the transition state, increasing the rate as given by equation (2.10) when V# 0. Although there is in principle nothing wrong with the activation volume approach, application of its traditional interpretation to the pressure dependence of reaction rates to SCFs can be misleading and our discussion of these effects is better to be given in terms of the pressure dependence of the activation barriers, G# (P) . The problem arises, as we can see from Figure 2-3, the traditional interpretation of the activation neglects the fact that other solvent properties, such as the dielectric constant, can be extremely pressure sensitive in compressible SCFs. Figure 2-3: Free energy sketches for reaction coordinates representing two different responses to density.(a) preferential solvation of the transition state as density increases, leading to a net decrease in ΔG# with increasing density. In (b) the reactants and products are preferentially solvated by increased density. Modified figure from Levert Sengers’ book (Levert Sengers, 1998). When these properties affect the solvation of the transition state and reactants differently, the activation energy will vary rapidly with pressure, causing large changes in the reaction rate, which are not representative of an actual volume effect.PDF Image | MOLECULAR SIMULATION STUDIES IN THE SUPERCRITICAL REGION
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