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20 along the reaction coordinate. The energy required to overcome the barrier (corresponding to the transition state) is the activation energyG# . The activation energy is connected to the equilibrium constant though the expression RTlnK G c The activation Gibbs free energy change can be written in terms of enthalpy (or internal energy) change and entropy change G# E# PV# TS#or G# H# TS# Since(G#/P)T Vwehave V# RTlnkX lnkC (1...) P P Gas-phase reaction (2.9) (2.10) T,x T,C When a chemical reaction takes place in the gas phase and considered ideal, the free energy barrier is completely determined by the interactions among the reactants. In that case, there is no pressure dependence on kinetic constant and always the activation volume value is zero in equation 2.10 Reaction in Solution When a reaction takes place in solution, however, the forces exerted by the solvent molecules also influenced the free energy barrier. For reactions in solution, it is usually assumed that the solute follows the same reaction path as it would if the same reaction were to occur in the gas phase, and that the transition state is taken to be located at some point along this path, most frequently at the free energy maximum. Additionally, the solute reaction path is nearly always identified as the reactive degree of freedom (Tucker and Truhlar, 1990) and then κTST is taken to be one. Note that this set of assumptions, known as the equilibrium solvation approximation, is equivalent to assuming that the solvent rapidly readjusts in response to changes in the solute,PDF Image | MOLECULAR SIMULATION STUDIES IN THE SUPERCRITICAL REGION
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