Electronic Structure Regulated Carbon-Based Single-Atom Catalysts for Highly Efficient and Stable Electrocatalysis

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Single-atom catalysts (SACs) offer high atomic utilization and catalytic performance on carbon substrates.
• Precisely controlling the electronic structure of single-atom sites is key to optimizing electrocatalytic activity.
• Understanding the fundamental principles linking electronic structure to SACs' intrinsic activity remains a challenge.

Purpose of the Study:

• To summarize strategies for regulating the electronic structure of carbon-based SACs.
• To discuss the impact of electronic structure on reactive intermediate activation and key electrocatalytic reactions.
• To elucidate the electronic structure-performance relationships in SACs for electrochemical applications.

Main Methods:

• Summarizing strategies: nonmetal heteroatom doping, coordination number regulation, defect engineering, strain design, and dual-metal-site design.
• Discussing impacts on water splitting, oxygen reduction reaction, and CO2/N2 electroreduction reactions.
• Combining characterization techniques with density functional theory (DFT) calculations to understand structure-performance relationships.

Main Results:

• Various strategies effectively regulate the electronic structure of carbon-based SACs.
• Electronic structure significantly influences the activation of reactive intermediates and overall electrocatalytic activity.
• Clear electronic structure-performance relationships were established for key electrochemical reactions.

Conclusions:

• A comprehensive understanding of electronic structure-correlated electrocatalytic activity in SACs has been achieved.
• This review provides insights into challenges and future prospects for advancing SACs in electrochemistry.
• Optimizing electronic structure is a crucial pathway for developing high-performance SACs.