(237c) Single Metal Atom in N Doped Graphene for Electrocatalytic CO2 and Oxygen Reduction: Activation Energies and Catalytic Mechanisms

Single metal atom in N doped graphene (M-N-C) has shown promising performance for a variety of electrocatalytic reactions, such as CO2 and oxygen reduction, while the kinetic mechanisms (e.g. energy barriers) at the atomic-scale are not well understood. One of the major challenges is the lack of computational methods to effectively simulate the electrochemical kinetics at solid-water interface. Here we present a first-principles model, and use it to elucidate the atomistic mechanisms of M-N-C for CO2R and ORR. We show the unprecedented role of charge capacity of the site in determining its activity and selectivity in CO2R, and the kinetic origin of the ORR to H2O2 as well as the potential and pH dependence.