Tuning the Coordination Environment of Carbon-Based Single-Atom Catalysts via Doping with Multiple Heteroatoms and Their Applications in Electrocatalysis

Carbon-based single-atom catalysts (SACs) are considered to be a perfect platform for studying the structure-activity relationship of different reactions due to the adjustability of their coordination environment. Multi-heteroatom doping has been demonstrated as an effective strategy for tuning the coordination environment of carbon-based SACs and enhancing catalytic performance in electrochemical reactions. Herein, recently developed strategies for multi-heteroatom doping, focusing on the regulation of single-atom active sites by heteroatoms in different coordination shells, are summarized. In addition, the correlation between the coordination environment and the catalytic activity of carbon-based SACs are investigated through representative experiments and theoretical calculations for various electrochemical reactions. Finally, concerning certain shortcomings of the current strategies of doping multi-heteroatoms, some suggestions are put forward to promote the development of carbon-based SACs in the field of electrocatalysis.

Automated summary

Carbon-based single-atom catalysts (SACs) are an ideal platform for studying the structure-activity relationship in different reactions, and doping with multiple heteroatoms is an effective strategy to enhance their catalytic performance. This article summarizes the recent strategies of multi-heteroatom doping, focusing on the regulation of single-atom active sites in different coordination shells. The correlation between the coordination environment and the catalytic activity of carbon-based SACs is investigated through experiments and theoretical calculations. Suggestions are also provided to promote the development of carbon-based SACs in electrocatalysis, addressing certain shortcomings of current doping strategies.