First Principles Study of Morphology, Doping Level, and Water Solvation Effects on the Catalytic Mechanism of Nitrogen-Doped Graphene in the Oxygen Reduction Reaction

摘要: By using first principles DFT calculations, we reveal oxygen reduction reaction mechanisms in N-doped graphene (N-Gr). Considering both the morphology and concentration of dopant N atoms bulk edge N-Gr forms, calculate energies a large number model systems to cover wide range possible structures determine most stable forms. In agreement with experiments, our calculations suggest that doping levels forms are limited less than approximately 30 at. % N, above which hexagonal framework is broken. The ground state found differ depending on level poisoning bonds. Oxygen evaluated by Gibbs free-energy diagrams without water solvation. Our results indicate significantly alters catalytic properties pure dilutely doped active.