Design of a Single‐Atom Indiumδ+–N4Interface for Efficient Electroreduction of CO2to Formate

Abstract Main‐group element indium (In) is a promising electrocatalyst which triggers CO2reduction to formate, while the high overpotential and low Faradaic efficiency (FE) hinder its practical application. Herein, we rationally design a new In single‐atom catalyst containing exclusive isolated Inδ+–N4atomic interface sites for CO2electroreduction to formate with high efficiency. This catalyst exhibits an extremely large turnover frequency (TOF) up to 12500 h−1at −0.95 V versus the reversible hydrogen electrode (RHE), with a FE for formate of 96 % and current density of 8.87 mA cm−2at low potential of −0.65 V versus RHE. Our findings present a feasible strategy for the accurate regulation of main‐group indium catalysts for CO2reduction at atomic scale.