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초록

The pressing necessity to mitigate climate change and transition to a sustainable energy economy underscores the importance of developing highly efficient and selective catalysts for electrocatalytic CO2 reduction (CO2RR). This study explores nitrogen-doped graphyne (N-GY) as a promising substrate for anchoring 3d and 4d transition metal atoms (TMs), facilitating the creation of high-performance electrocatalysts. Through comprehensive computational analysis based on density functional theory (DFT), we provide a detailed understanding of the mechanisms involved in CO2 capture by these catalysts. Our results reveal a “donation-backdonation” mechanism during CO2 adsorption, characterized by significant charge transfer and orbital overlap, which enhance CO2 adsorption and activation. We identify ten catalysts exhibiting exceptional activity and selectivity, with V-S2@N-GY standing out for its ultra-low limiting potential of −0.279 V, which is particularly beneficial for carbon monoxide generation. The mechanistic analysis further underscores the critical role of the *COOH intermediate adsorption strength in dictating CO2RR activity. This study provides valuable theoretical insights for the design and optimization of efficient CO2RR catalysts. © 2025 Elsevier Inc.

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