B atom dopant-manipulate electronic structure of CuIn nanoalloy delivering wide potential activity over electrochemical CO2RR

Abstract

The accuracy and efficiency tuning the local electronic structure of catalyst active sites are pre-requisites for achieving high selectivity CO2 reduction reaction on a wide potential window, whereas remain a great challenge. Here, a B-doped CuIn alloy catalyst with tunable electronic structure for the highly effective electrochemical conversion of CO2 to CO has been exploited. The obtained B-doped CuIn alloy performs an optimal CO Faraday efficiency of 99% at –0.6 V (vs. the reversible hydrogen electrode) and particularly keeps outstanding CO Faraday efficiency (> 90%) over a wide cathodic electrochemical window (400 mV). Density functional theory theoretical calculation manifests that the enhanced performance is primarily ascribed to the electron-capturing ability of high valence state B atom, which optimizes the local electronic structure of adjacent metal active sites and adjusts the binding energy between catalyst and intermediates. A foundation of designing advanced electrochemical CO2 reduction reaction catalysts can be served by the insights gained though this research.