Synergism of highly graphitic N-doped graphene-like carbon and Pt@PtCo core-shell structure for efficient oxygen reduction reaction

It is crucial to develop efficient, highly durable platinum-based oxygen reduction reaction (ORR) catalysts to advance fuel cell development. In this study, a series of N-doped graphene-like carbon (NGC) materials was synthesized by pyrolyzing a mixture of glucose and graphitic carbon nitride (g-C 3 N 4 ), with g-C 3 N 4 acting as both a structural template and a nitrogen source. An NGC material containing approximately 6.9% N was obtained at a mass ratio of 4:1 for g-C 3 N 4 to glucose and a pyrolysis temperature of 900 °C. PtCo alloy nanoparticles were homogeneously anchored onto NGC via an impregnation-ethylene glycol reduction method. A core-shell structured catalyst consisting of a Pt shell surrounding a PtCo alloy core was subsequently fabricated by annealing the PtCo/NGC composite at 700 °C. The resulting Pt@PtCo/NGC catalyst exhibits superior ORR activity, with mass activity 3.22 and 3.25 times higher than that of a commercial Pt/C catalyst under acidic and alkaline conditions, respectively. Furthermore, the ORR mechanism was systematically investigated through combined material characterization, electrochemical analysis, and DFT calculations, providing deeper insight into the electrocatalytic structure-activity relationship.