Design of a Single‐Atom Indiumδ+–N4 Interface for Efficient Electroreduction of CO2 to Formate

Main‐group element indium (In) is a promising electrocatalyst which triggers CO2 reduction 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+–N4 atomic interface sites for CO2 electroreduction to formate with high efficiency. This catalyst exhibits an extremely large turnover frequency (TOF) up to 12500 h−1 at −0.95 V versus the reversible hydrogen electrode (RHE), with a FE for formate of 96 % and current density of 8.87 mA cm−2 at low potential of −0.65 V versus RHE. Our findings present a feasible strategy for the accurate regulation of main‐group indium catalysts for CO2 reduction at atomic scale. A new indium single‐atom catalyst with Inδ+–N4 atomic interface active sites is constructed for electroreduction of CO2 to formate. The system has a more negative potential and high Faradaic efficiency. This approach offers an effective strategy to develop superior main group metal CO2ER catalysts with not only high activity but also high selectivity.