Critically, the central metal atoms along with their coordination environment play a significant role in the catalytic performance of single-atom catalysts (SACs). Herein, 12 single Fe, Mo, and Ru atoms supported on defective graphene are theoretically deigned for investigation of their structural and electronic properties and catalytic nitrogen reduction reaction (NRR) performance using first-principles calculations. Our results reveal that graphene with vacancies can be an ideal anchoring site for stabilizing isolated metal atoms owing to the strong metal-support interaction, forming stable TMC or TMN active centers ( = 3 or 4). Six SACs are screened as promising NRR catalyst candidates with excellent activity and selectivity during NRR, and RuN is identified as the optimal one with an overpotential of ≥0.10 V via the distal mechanism.
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