A superior electrocatalyst toward the oxygen reduction reaction obtained by atomically dispersing copper on N, F co-doped graphene through atomic interface engineering†
Single-atom catalysts, featuring 100% metal atom utilization, strong metal–support interaction, low coordination environment, and high selectivity, have attracted great attention towards the enhancement of the oxygen reduction reaction (ORR). In the current work, we propose an atomic interface strategy for the construction of Cu single-atom catalysts dispersed on N, F co-doped graphene (Cu SA-NFG). The Cu SA-NFG catalyst exhibited excellent ORR activity in alkaline media. Both X-ray absorption fine structure and density functional theory results demonstrated that the Cu–N4 atomic interface is the active site for the ORR, and the electron-withdrawing F atoms can decrease the Gibbs free energy for the adsorption of intermediates. In addition, the Pt nanoparticle-decorated Cu SA-NFG catalyst displayed superior catalytic performance toward methanol oxidation. This work provides a new method for the rational design of advanced electrode materials and a new guide for the improvement of catalytic performance toward direct methanol fuel cells.