LAUSR

Identifying and generating more active sites with high activity on N‐doped graphene for oxygen evolution reaction (OER) are challenging in the renewable energy conversion and storage technologies. However, the local electronic/chemical environment on graphene surface is significantly influenced and can be controlled by doping with foreign atoms, which will contribute to its improved catalytic performance. Henceforth, different N‐doping formats, diverse N distributions and concentrations, as well as the edge effect are investigated on the basis of density functional theory, to discover the ideal N‐doping condition for high OER behavior. By analyzing the free‐energy‐change diagrams, adsorbed interactions of reactant intermediates, electrostatic potential surfaces, and other obtained data, it is suggested that graphitic N with low doping concentration and N atoms distributed near edge sites is the ideal candidate for high OER activity, which is efficient as a carbon‐based electrocatalyst for water splitting and metal–air batteries applications.