A Generalized Approach for Predicting Coverage-Dependent Reaction Parameters of Complex Surface Reactions: Application to H2 Oxidation over Platinum

Abstract

A new methodology is presented for calculating parameters of complex surface reaction mechanisms. This approach takes into consideration adsorbate−adsorbate interactions along with their influence on the activation energies of surface reactions as a function of operating conditions. It combines an extension of the unity bond index−quadratic exponential potential theory, reactor scale modeling, important feature identification, and model validation. The H2 oxidation over platinum has been chosen as a model system to test this methodology. Comparison with a variety of available experimental data in the literature, such as catalytic ignition temperature, laser-induced fluorescence OH desorption measurements, catalytic autotherms, and species profiles, shows that the proposed surface mechanism is capable of quantitatively capturing all the important features of the published experiments. Our approach offers the potential of quantitative modeling of catalytic reactors exhibiting complex surface reaction processes under realistic operating conditions.