(169b) The Influence of Local Environment on Theoretical Calculations of Adsorption and Reaction for Catalyzed Reactions

Advances in algorithmic efficiency and computer speed have made it possible to carry out calculations of the thermodynamics and kinetics of elementary processes involved in reactions occurring on heterogeneous catalysts that now approach chemical accuracy. Work done in the last decade has revealed that the accuracy of computed results depends not only local interactions – bonding and non-bonding – but also the effects of the local environment. Examples of the latter effects include the influence of electrostatic and dispersive interactions of framework atoms in a zeolite that are distant from the active center and influence of solvation and direct effects of cations and anions with adsorbed species involved in electrochemical reactions. This talk will illustrate how such interactions of adsorbed species with the local environment affect the enthalpies and entropies of species adsorption and activation for elementary processes occurring in zeolites and at the surface of electrocatalysts.