Recent advances in the theoretical studies on the electrocatalytic CO2 reduction based on single and double atoms

Abstract

Excess of carbon dioxide (CO2) in the atmosphere poses a significant threat to the global climate. Therefore, the electrocatalytic carbon dioxide reduction reaction (CO2RR) is important to reduce the burden on the environment and provide possibilities for developing new energy sources. However, highly active and selective catalysts are needed to effectively catalyze product synthesis with high adhesion value. Single-atom catalysts (SACs) and double-atom catalysts (DACs) have attracted much attention in the field of electrocatalysis due to their high activity, strong selectivity, and high atomic utilization. This review summarized the research progress of electrocatalytic CO2RR related to different types of SACs and DACs. The emphasis was laid on the catalytic reaction mechanism of SACs and DACs using the theoretical calculation method. Furthermore, the influences of solvation and electrode potential were studied to simulate the real electrochemical environment to bridge the gap between experiments and computations. Finally, the current challenges and future development prospects were summarized and prospected for CO2RR to lay the foundation for the theoretical research of SACs and DACs in other aspects.

A two-electron reducing reaction of CO2 to an oxalate anion: a theoretical study of delocalized (presolvated) electrons in Al(CH3)n(NH3)m, n = 0–2 and m = 1–6, clusters

“…A very large number of publications in 2023 testify to the high level of activity of researchers in this field. 57–62…”

Advances and challenges in the electrochemical reduction of carbon dioxide

“…It is a favorable weapon for reasonably analyzing the reaction mechanism and predicting the catalytic steps and has an indispensable inspiration and guidance for experimental preparation. 285 For ECO 2 RR, the intrinsic properties of CO 2 molecules are variable, the types of intermediates of CO 2 RR are multifarious, and the effects of solvation and ion on CO 2 RR at the solid–liquid interface are relatively complex. Theoretical calculations are increasingly being relied upon to reveal the mechanism of the tedious reaction steps and to screen for more optimized material compositions and structures.…”