Modeling the kinetics of large sets of reactions on metal surfaces

Abstract

We are concerned with constructing and solving kinetic models for large-scale catalytic mechanisms involving hundreds of reactions. We need reliable estimates for hundreds of rate constants for each project we undertake. In order to obtain reliable estimates of activation barriers with co-adsorbate effects, we employ the UBI-QEP method whenever applicable. We also bring quantum mechanical electronic structure methods to bear when necessary. Herein we describe a new model for obtaining reasonable estimates for rate constants for reactions on metal surfaces that yields rate constants and rate constant parameters without large amounts of computer time. The model is based on a novel approach to surface-phase chemistry and a re-thinking regarding the phases from which surface adsorbates react. We will also discuss recent literature regarding trends in Arrhenius pre-exponential factors (prefactors).