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not affect the concentration yet it is found that at high pressures reaction rates are affected (‘kinetic pressure effect’)(Brennecke and Chateauneuf, 1999). The change in the rate is attributed to a change in the rate constant as a result change in pressure. Although pressure is inevitably the experimental controlled variable, sometimes the analysis of rate data can be facilitated by examining how the rate constant varies with the solvent density in that case lnkC lnkC lnkC (2.6) P P V 12 T,C T,C T,C T,C where V is the molar volume. 2.3 HISTORICAL DEVELOPMENTS AND MODERN KINETICS The transition state (TS) is the critical configuration of a reaction system situated at the highest point of the most favourable reaction path on the potential energy surface. It is regarded as critical in the sense that if it is attained the system will have a high probability of continuing reaction to completion. The concept of the transition state was first broached by M.Polanyi and M.G.Evans (Evans and Polanyi, 1935) and by H.Eyring (Eyring, 1935), both in 1935. Since that time, numerous pieces of work on chemical kinetics and dynamics, both experimental and theoretical, have been published in implicit or explicit reference to the concept. The theory of absolute reaction rates gained popularity under the name ‘transition-state theory’. Admittedly, however the theory has never been considered to be complete. A major reason for this is that little reliance could be place on the methods used to guess the characteristic properties (i.e. geometry, vibrational frequencies and activation energy) of the TS. Transition-state theory (TST) is a convenient and powerful formalism for explaining and interpreting the kinetics of elementary reactions. This theory views a chemicalPDF Image | MOLECULAR SIMULATION STUDIES IN THE SUPERCRITICAL REGION
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