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

摘要

Single 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.