Crystalline‐Amorphous Interfaces Engineering of CoO‐InOx for Highly Efficient CO2 Electroreduction to CO

Abstract

AbstractAs a fundamental product of CO2 conversion through two‐electron transfer, CO is used to produce numerous chemicals and fuels with high efficiency, which has broad application prospects. In this work, it has successfully optimized catalytic activity by fabricating an electrocatalyst featuring crystalline‐amorphous CoO‐InOx interfaces, thereby significantly expediting CO production. The 1.21%CoO‐InOx consists of randomly dispersed CoO crystalline particles among amorphous InOx nanoribbons. In contrast to the same‐phase structure, the unique CoO‐InOx heterostructure provides plentiful reactive crystalline‐amorphous interfacial sites. The Faradaic efficiency of CO (FECO) can reach up to 95.67% with a current density of 61.72 mA cm−2 in a typical H‐cell using MeCN containing 0.5 M 1‐Butyl‐3‐methylimidazolium hexafluorophosphate ([Bmim]PF6) as the electrolyte. Comprehensive experiments indicate that CoO‐InOx interfaces with optimization of charge transfer enhance the double‐layer capacitance and CO2 adsorption capacity. Theoretical calculations further reveal that the regulating of the electronic structure at interfacial sites not only optimizes the Gibbs free energy of *COOH intermediate formation but also inhibits HER, resulting in high selectivity toward CO.