Coordination engineering of transition metal doped in B2CN3 electrocatalyst to enhance efficient carbon dioxide reduction reaction

One of the effective strategies adopted for mitigating the challenges posed by the elevated emission of CO₂ is its electrochemical reduction into valuable products. This work employs DFT to investigate a transition metal-doped B₂CN₃ electrocatalyst, which is one of the significantly selective and stable electrocatalysts for the carbon dioxide reduction reaction (CRR). Various transition metals, including cobalt, chromium, iron, and nickel, were utilized for doping to explore different electrocatalysts. The DFT indicated that the Fe–B₂CN₃ effectively adhered and activated CO₂, as confirmed by analyses of the crystal orbital Hamilton population, Bader charge, charge density differences and partial density of states. The limiting potential for CRR was −0.41 V, in contrast to the hydrogen evolution reaction (HER) at −0.244 V, with formaldehyde identified as the primary product. The B₂CN₃ exhibited a preference for CO₂ reduction while effectively suppressing the HER. This research highlights the promising application of the modified B₂CN₃ as a highly-efficient electrocatalyst for CRR and offers invaluable theoretical insights for designing efficient CRR electrocatalysts.