Single Atom Catalysis for Hydrogen Evolution Reaction using Transition‐metal Atoms Doped g‐C3N3: A Density Functional Theory Study

Abstract

AbstractSingle transition‐metal atom coordinated graphite carbon nitride, including the metal atom doped g‐C3N4 system, displays catalytic activity comparable to that of the noble metal Pt catalyst with outstanding performance. Herein, we investigate the single atom catalytic performance of g‐C3N3 embedded by a single transition metal atom (M−C3N3; M=Mn, Fe, Co, Ni, Cu, Rh, Pd, Ag, and Pt) for hydrogen evolution reaction (HER) using density functional theory (DFT) calculations. The results indicate that all the M−C3N3 catalysts are thermally and dynamically stable systems. By comparing the Gibbs free energies, we found that the Rh−C3N3 catalyst exhibits the best HER electrocatalytic performance among the investigated systems. Subsequently, analysis of electronic structure indicates that the Rh−C3N3 system displays a metallic behavior, which is a beneficial feature for an adequate HER electrocatalyst. Finally, the charge density difference of the Rh−C3N3 structure further supports the rationality of our results. This study provides a new candidate of low‐cost, high‐performance, and highly active non‐noble metal electrocatalysts.