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

Abstract

Electrochemical CO₂ reduction reaction (eCO₂ 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 eCO₂ RR due to their high utilization of metal atoms and flexible coordination structures. In this work, the recent progress in SACs for eCO₂ 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 eCO₂ RR. Three perspectives form the starting point: 1) Important factors of SACs for eCO₂ RR; 2) Typical SACs for eCO₂ RR; 3) eCO₂ 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 eCO₂ RR, the reaction mechanism and measures which can be taken to improve the selectivity of eCO₂ RR are discussed. Hopefully_, this work can provide a comprehensive understanding of SACs for eCO₂ RR and spark innovative design and modification ideas to develop highly efficient SACs for CO₂ conversion to various valuable fuels/chemicals.

Keywords: coordination environment; electrochemical CO2 reductions; electronic structures; product selectivity; single-atom catalysts; support effects.