Charge localization to optimize reactant adsorption on KCu7S4/CuO interfacial structure toward selective CO2 electroreduction

Abstract

Regulating electronic structure of electrocatalysts to optimize reactant adsorption on the catalyst surface is a crucial tactic to boost catalytic activity in electrocatalysis. Herein, a novel KCu7S4/CuO interfacial structure is well constructed to induce the formation of localized charge region to optimize the adsorption properties of active intermediates at the interface to promote CO2 electroreduction. The catalyst of interfacial catalyst delivered boosted CO2RR activity and selectivity toward formate with a Faraday efficiency (FE) of 71.0 % and a decent current density of 7.56 mA cm−2 at a moderate potential of -0.9 V (versus reversible hydrogen electrode) as well as a good durability. Theoretical calculations unveiled that the enhanced CO2RR activity and formate selectivity could be attributed to the strengthened CO2* adsorption in the initial step, the increased adsorption of the key intermediates OCHO*, and the weakened H* adsorption via the localized positive charge region induced by charge redistribution at interface.