Ambient Electrosynthesis toward Single-Atom Sites for Electrocatalytic Green Hydrogen Cycling

With the ultimate atomic utilization, well-defined configuration of active sites and unique electronic properties, catalysts with single-atom sites (SASs) exhibit appealing performance for electrocatalytic green hydrogen generation from water splitting and further utilization via hydrogen-oxygen fuel cells, such that a vast majority of synthetic strategies toward SAS-based catalysts (SASCs) are exploited. In particular, room-temperature electrosynthesis under atmospheric pressure offers a novel, safe, and effective route to access SASs. Herein, the recent progress in ambient electrosynthesis toward SASs for electrocatalytic sustainable hydrogen generation and utilization, and future opportunities are discussed. A systematic summary is started on three kinds of ambient electrochemically synthetic routes for SASs, including electrochemical etching (ECE), direct electrodeposition (DED), and electrochemical leaching-redeposition (ELR), associated with advanced characterization techniques. Next, their electrocatalytic applications for hydrogen energy conversion including hydrogen evolution reaction, oxygen evolution reaction, overall water splitting, and oxygen reduction reaction are reviewed. Finally, a brief conclusion and remarks on future challenges regarding further development of ambient electrosynthesis of high-performance and cost-effective SASCs for many other electrocatalytic applications are presented.

Automated summary

This article discusses the methods and applications of ambient electrosynthesis for the synthesis of single-atom site catalysts (SASCs). A systematic summary is provided for three synthetic routes of SASCs, along with advanced characterization techniques. The applications of these synthesis methods in hydrogen energy conversion are reviewed. Finally, challenges for further development of high-performance and cost-effective SASCs are presented.