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

Electrochemical CO2 reduction reaction (eCO(2)RR) 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 eCO(2)RR due to their high utilization of metal atoms and flexible coordination structures. In this work, the recent progress in SACs for eCO(2)RR 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 eCO(2)RR. Three perspectives form the starting point: 1) Important factors of SACs for eCO(2)RR; 2) Typical SACs for eCO(2)RR; 3) eCO(2)RR 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 eCO(2)RR, the reaction mechanism and measures which can be taken to improve the selectivity of eCO(2)RR are discussed. Hopefully, this work can provide a comprehensive understanding of SACs for eCO(2)RR and spark innovative design and modification ideas to develop highly efficient SACs for CO(2 )conversion to various valuable fuels/chemicals.