Zhao Xin, He Daping, Xia Bao Yu, Sun Yujie, You Bo
School of Science, Wuhan University of Technology, Wuhan, Hubei, 430070, China.
Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074, China.
Adv Mater. 2023 Apr;35(14):e2210703. doi: 10.1002/adma.202210703. Epub 2023 Feb 17.
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.
由于具有极致的原子利用率、明确的活性位点构型和独特的电子性质，单原子位点催化剂（SASs）在通过水分解进行电催化绿色制氢以及后续通过氢氧燃料电池进行利用方面展现出诱人的性能，因此人们开发了大量针对基于单原子位点的催化剂（SASC）的合成策略。特别是，常压下的室温电合成提供了一种新颖、安全且有效的途径来制备单原子位点。在此，本文讨论了用于电催化可持续制氢及利用的单原子位点的环境电合成的最新进展以及未来机遇。本文首先对三种用于单原子位点的环境电化学合成路线进行了系统总结，包括电化学蚀刻（ECE）、直接电沉积（DED）和电化学浸出 - 再沉积（ELR），并介绍了相关的先进表征技术。接下来，综述了它们在氢能转换方面的电催化应用，包括析氢反应、析氧反应、全水分解和氧还原反应。最后，针对高性能且经济高效的单原子位点催化剂在许多其他电催化应用中的环境电合成的进一步发展所面临的未来挑战给出了简要结论和评论。
