▎ 摘　　要

A systematic study on the catalytic performance of dual transition metal atoms (3d, 4d and 5d) embedded in three types of N-doped graphene (DV, TV, QV) for electrocatalytic nitrogen reduction reaction (NRR) was conducted by first-principles calculations, high-throughput screening and molecular dynamic simulations. Full reaction pathway search of the screened candidates shows Cr-2-TV, Mo-2-TV and Ir-2-TV to be the promising catalysts for NRR with onset potentials of -0.24, -0.39 and -0.38 V, respectively. In-deep analysis of the band structure, projected density of states, spin density, charge density difference, Bader charge population of N-2 molecule adsorbed on catalysts unveil that the charge transfer between the adsorbed N-2 molecules and the metal atoms in catalysts, good electronic conductivity, and significant orbital hybridization account for the high catalytic efficiency of NRR on Cr-2-TV, Mo-2-TV and Ir-2-TV. The evaluation of stability and selectivity of the three catalysts indicates that all three catalysts display high stabilities, and Cr-2-/Mo-2-TV shows good NRR selectivity compared to HER. Our present study sheds some insights on the design of novel dimetal anchored N-doped graphene as efficient electrocatalysts for NRR, promoting both experimental and theoretical investigations in this direction.