High-Throughput Screening of Nitrogen-Coordinated Bimetal Catalysts for Multielectron Reduction of CO₂ to CH₄ with High Selectivity and Low Limiting Potential

Significant challenges remain for developing efficient catalysts in an electrochemical multielectron CO2 reduction reaction (CO2RR), which usually suffers from poor activity and selectivity. Motivated by the recent experimental progress fabricating dual-metal atom (DMACs) N-doped graphene materials (graphene-N6V4; N: nitrogen V: vacancy), we sampled eight types of homonuclear (N6V4-M2, M = Cr, Mn, Fe, Co, Ni, Cu, Pd, Ag) 28 heteronuclear (N6V4-M1M2) to study CO2RR via first-principles high-throughput screening. Using stability, activity, selectivity as indicators along with broken conventional scaling relationship, N6V4-AgCr was selected a promising candidate deep methane low overpotential 0.55 V after two screening rounds. Further analysis showed that frustrated Lewis pair, formed between metal para-N, owing difference electronic arrangement d orbitals various transition metals, caused spin polarization systems affected catalytic performance each DMAC. Our work not only provides solid strategy potential but also demonstrates their activities originate atomic structures DMACs.