First Principles Computations of the Oxygen Reduction Reaction on Solid Metal Clusters

An improvement in the catalytic process of oxygen reduction reactions is of prime importance for further progress in low temperature fuel cell performance. This paper intends to investigate this problem from a fundamental quantum mechanics viewpoint. For this purpose, a hybrid density functional theory is employed to analyze the catalytic mechanism of the oxygen reduction at the fuel cell cathode. Major steps in the oxygen reduction that include the oxygen adsorption on solid metal clusters (e.g. Cu and Pt) and complete four proton transfer steps are simulated. Proton transfer processes from hydroniums to the adsorbed oxygen molecules to produce water are observed to be mainly influenced by the electronic cloud at the catalyst. The first principles computation results reveal a difficulty in choosing the catalyst material and how the catalytic mechanism limits the performance of current low temperature fuel cells.