OH and O mediated interaction of CO2 with Ni(1 1 0) surface, and its implications on biomimetic CO2 hydration

Abstract Pre-coverage of a clean Ni(1 1 0) surface with OH and O plays an important role in activating CO2 molecules during a host of surface catalytic reactions involving CO2 and H2O. Appreciating this observation, the present work was designed to focus on providing detailed mechanistic insights into CO2 hydration reaction by Ni(1 1 0) surface, pre-covered by oxygenated surface species formed as a result of partial as well as complete dissociation of H2O. Density functional theory calculations were employed to investigate CO2 hydration with modified Ni(1 1 0) surfaces acting as biomimetic catalysts exhibiting carbonic anhydrase-like mechanism. Bader charge analysis was done to probe the charge distributions in different catalytic systems under study. Potential energy surfaces were developed for the formation of bicarbonate and carbonate. Our computational analysis conclusively demonstrates the feasibility of Ni(1 1 0) to act as biomimetic CO2 hydration catalyst, and the plausibility of carbonate formation to compete with biomimetic CO2 hydration.