Scalable solid-phase synthesis of defect-rich graphene for oxygen reduction electrocatalysis

Defect-engineered carbon materials have been emerged as promising electrocatalysts for oxygen reduction reaction (ORR) in metal-air batteries. Developing a facile strategy for the preparation of highly active nanocarbon electrocatalysts remains challenging. Herein, a low-cost and simple route is developed to synthesize defective graphene by pyrolyzing the mixture of glucose and carbon nitride. Molecular dynamics simulations reveal that the graphene formation is ascribed to two-dimensional layered feature of carbon nitride, and high compatibility of carbon nitride/glucose systems. Structural measurements suggest that the graphene possesses rich edge and topological defects. The graphene catalyst exhibits higher power density than commercial Pt/C catalyst in a primary Zn-air battery. Combining experimental results and theoretical thermodynamic analysis, it is identified that graphitic nitrogen-modified topological defects at carbon framework edges are responsible for the decent ORR performance. The strategy presented in this work can be can be scaled up readily to fabricate defective carbon materials.