Multi-doped borophene catalysts with engineered defects for CO2 reduction: A DFT study

Carbon dioxide reduction reaction (CO2RR) to convert carbon dioxide (CO2) into value-added products via the electrochemical method is a conducive way to tackle the hazard of high CO2 emissions. The present DFT study reports a novel dual chromium-anchored tri-vacancy borophene (Cr2/TV-β12) electrocatalyst, which showed high selectivity and stability for CO2RR. A tri-vacancy defect was introduced in β12 borophene to create an 11-membered ring borophene sheet (TV-β12), 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 Cr2/TV-β12 electrocatalyst adsorbs and activates CO2 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 CO2RR 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 CO2 reduction and suppressed HER. The usual problem of carbon monoxide poisoning encountered in CO2 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 β12 borophene has tremendous potential to be utilized as an efficient catalyst for CO2RR.