The electrochemical CO2 reduction reaction can effectively convert CO2 into promising fuels and chemicals, which is helpful in establishing a low-carbon emission economy. Compared with other types of electrocatalysts, single-atom catalysts (SACs) immobilized on carbon substrates are considered to be promising candidate catalysts. Atomically dispersed SACs exhibit excellent catalytic performance in CO2RR due to their maximum atomic utilization, unique electronic structure, and coordination environment. In this paper, we first briefly introduce the synthetic strategies and characterization techniques of SACs. Then, we focus on the optimization strategies of the atomic structure of carbon-based SACs, including adjusting the coordination atoms and coordination numbers, constructing the axial chemical environment, and regulating the carbon substrate, focusing on exploring the structure–performance relationship of SACs in the CO2RR process. In addition, this paper also briefly introduces the diatomic catalysts (DACs) as an extension of SACs. At the end of the paper, we summarize the article with an exciting outlook discussing the current challenges and prospects for research on the application of SACs in CO2RR.
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