Modulating the environment and metal choice doped in BC4N monolayer for carbon dioxide reduction: A computational study

Abstract

The utilization of the carbon dioxide reduction reaction (CO₂RR) through electrochemical means presents an effective approach for addressing the challenge posed by elevated carbon dioxide (CO₂) emissions, facilitating carbon dioxide conversion into valuable end products. In current DFT investigation, a new approach involving the singular metal doping of BC₄N electrocatalyst is highlighted. This catalyst demonstrates notable selectivity and durability in CO₂RR. The study involved the exploration of different electrocatalysts by incorporating diverse transition metals such as Cu, Co, Zn, and Mn. Simulation findings from density functional theory demonstrated that the Co-doped BC₄N electrocatalyst effectively adsorbs and triggers the activation of CO₂. This efficiency was confirmed through analyses including crystal orbital Hamilton population, Bader charge, charge density difference (CDD), and partial density of states (DOS) assessments. Assessment of the threshold potential for CO₂ reduction reaction has been determined to be −0.34 V, in contrast to hydrogen evolution reaction (HER) at 0.56 V, resulting primarily in production of formaldehyde. The catalyst exhibited a preference for CO₂ reduction while concurrently inhibiting HER. The research indicates that the altered BC₄N monolayer holds significant promise as a high-performance catalyst for CO₂RR and offers crucial theoretical insights for developing effective CO₂RR catalysts.