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the process, pressure-dependence studies reveal information on the volume profile of the process. 2.2 THEORETICAL BACKGROUND The theories available to chemists to explain and predict the effects of pressure on reactions, whether the objective of the investigation is a synthetic one or mechanistic one, are thermodynamics and applications of thermodynamics principles within the absolute reaction rate (Atkins, 1994; Moore and Pearson, 1982). We are interested in how the effect of pressure manifests itself on the equilibrium constant K and the free Gibbs energyG°, for the reaction (difference between products- reactants), or upon the kinetic constant k and the free Gibbs energy of activation ΔG (difference between transition state-reactants). If the effect of pressure is to increase the magnitude of K or reduce ΔG, the reaction will have a greater yield or a faster reaction rate respectively. Qualitatively it can be said that these effects can arise from the differing pressure effects on the chemical potentials of the reactants and products (equilibrium), or reactants and transition-state (kinetics). The approach favoured by many is one of considering the volume per mol of initial state, the transition-state and when appropriate, the product state. A reaction in which the transition-state has a smaller volume than the initial state is accelerated by application of pressure. Further, if the product has a different volume from the initial state, pressure will induce a change in product yield. To be more rigorous we must first remember that the volume of a chemical species in a solution is invariably different from that from the pure substance, where the volume per mole can readily be established from the density. The quantity we are interested in is the partial molar volume, which may be thought of as the effective volume per mole of a species when its intrinsic volume is modified by the influence 9PDF Image | MOLECULAR SIMULATION STUDIES IN THE SUPERCRITICAL REGION
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