Multi-doped borophene catalysts with engineered defects for CO reduction: A DFT study.

Carbon dioxide reduction reaction (CORR) to convert carbon dioxide (CO) into value-added products via the electrochemical method is a conducive way to tackle the hazard of high CO emissions. The present DFT study reports a novel dual chromium-anchored tri-vacancy borophene (Cr/TV-β) electrocatalyst, which showed high selectivity and stability for CORR. A tri-vacancy defect was introduced in β borophene to create an 11-membered ring borophene sheet (TV-β), and 28 different electrocatalysts were explored via doping various transition metals (Co, Cr, Cu, Fe, Mn, Ni, Zn). Density functional theory simulation results revealed that the Cr/TV-β electrocatalyst adsorbs and activates CO efficiently, which was validated by the partial density of states, charge density difference, Bader charge, and crystal orbital Hamilton population analyses. The limiting potential for CORR was evaluated to be -0.45 V, against hydrogen evolution reaction (HER) (0.57 V), with the main product being formaldehyde. The catalyst showed selectivity towards CO reduction and suppressed HER. The usual problem of carbon monoxide poisoning encountered in CO reduction was also assessed and a high resistance against the same was established. At the outset, the research revealed that dual atom-doped tri-vacancy β borophene has tremendous potential to be utilized as an efficient catalyst for CORR.