Computational screening of TMN₄ based graphene-like BC₆N for CO₂ electroreduction to C₁ hydrocarbon products

Graphene-like BC₆N monolayers supported with TMN₄ (TM = Sc ∼ Zn) (TMN₄@BC₆N) centers, which can provide various coordination environment, was studied to explore its performance as efficient CO₂RR catalysts through density functional theory (DFT). High-throughput screening based on structural stability and reaction pathways identified the most promising catalyst candidates. According to the optimal path and overpotential analysis, five TMN₄@BC₆N (TM = Cr, Mn, Fe, Co and Zn) systems with low limiting potentials exhibit high CO₂RR activity towards C1 products. The potential origin of electrocatalytic performance shows the descriptors of E_b (*CO) and E_b (*OH) act as performance indicators. It is revealed that coordination environment with different charge near the TMN₄ active center can modulate the catalytic activity of the catalyst. Overall, this work suggests the novel TMN₄@BC₆N SAC has potential application prospects in CO₂RR and sheds light on designing of new two-dimensional materials with high stability and superior CO₂RR activity.