Modulating the Structure and Composition of Single‐Atom Electrocatalysts for CO₂ reduction

Abstract

Electrochemical CO2 reduction reaction (eCO2RR) is a promising strategy to achieve carbon cycling by converting CO2 into value‐added products under mild reaction conditions. Recently, single‐atom catalysts (SACs) have shown enormous potential in eCO2RR due to their high utilization of metal atoms and flexible coordination structures. In this work, the recent progress in SACs for eCO2RR is outlined, with detailed discussions on the interaction between active sites and CO2, especially the adsorption/activation behavior of CO2 and the effects of the electronic structure of SACs on eCO2RR. Three perspectives form the starting point: 1) Important factors of SACs for eCO2RR; 2) Typical SACs for eCO2RR; 3) eCO2RR toward valuable products. First, how different modification strategies can change the electronic structure of SACs to improve catalytic performance is discussed; Second, SACs with diverse supports and how supports assist active sites to undergo catalytic reaction are introduced; Finally, according to various valuable products from eCO2RR, the reaction mechanism and measures which can be taken to improve the selectivity of eCO2RR are discussed. Hopefully, this work can provide a comprehensive understanding of SACs for eCO2RR and spark innovative design and modification ideas to develop highly efficient SACs for CO2 conversion to various valuable fuels/chemicals.