Theoretical Study on a Potential Oxygen Reduction Reaction Electrocatalyst: Single Fe Atoms Supported on Graphite Carbonitride.

In recent years, one of the research directions of proton-exchange membrane fuel cells (PEMFCs) was to exploit efficient electrocatalysts for oxygen reduction reaction (ORR) instead of precious metals. In this study, on the basis of the density-functional theory (DFT) calculations, we designed a new type of single-atom ORR electrocatalyst by doping single iron atoms into the N-coordination cavity of the substrate graphite carbonitride (Fe/g-C3N4). The adsorption site and the adsorption energy of all the intermediates, the reaction energy barriers, potential energy surface, and Mulliken charges have been analyzed. The feasible ORR reaction paths and the most favorable ORR reaction mechanism were performed. Our calculation results prove that Fe/g-C3N4 is a potential electrocatalyst toward ORR. This work proposes a novel notion for the development of cathode materials in PEMFCs.