Curvature effect on graphene-based Co/Ni single-atom catalysts

Graphene has been widely utilized as a substrate for metal-based catalysts due to its unique structural and material properties. Despite the numerous strategies proposed for designing graphene-based catalysts, the effect of curvature on their performance has received relatively little attention. In this work, we construct novel curved graphene models by compressing lattice constant and curving C–C bonds. Curved graphene-based single-atom catalysts (SACs) are obtained by doping Co, Ni, or CoNi atoms with pyridine nitrogen coordination on the curved graphene. Through first-principles calculations, we investigate the effect of curvature on both graphene and graphene-based SACs in terms of their structure and catalytic performance for the hydrogen evolution reaction, the oxygen evolution reaction, and the oxygen reduction reaction. Our results show that tuning the curvature of graphene can effectively modulate the catalytic performance and stability of graphene-based SACs, providing novel design guidance for these materials.