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

Graphene-like BC6N monolayers supported with TMN4 (TM = Sc similar to 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 C-1 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.

Automated summary

Graphene-like BC6N monolayers supported with TMN4 (TM = Sc to Zn) centers were studied as efficient CO2RR catalysts. High-throughput screening based on structural stability and reaction pathways identified the most promising catalyst candidates. Different charge coordination environments near the TMN4 centers were found to modulate the catalytic activity of the catalyst.