催化学报 ›› 2023, Vol. 47: 32-66.DOI: 10.1016/S1872-2067(23)64392-X

• 综述 • 上一篇    下一篇

单原子催化剂的合成及其在电化学能量转换中的应用

詹麒尼, 帅婷玉, 徐慧民, 黄陈金, 张志杰, 李高仁*()   

  1. 四川大学材料科学与工程学院, 四川成都610065
  • 收稿日期:2022-10-21 接受日期:2022-12-22 出版日期:2023-04-18 发布日期:2023-03-20
  • 通讯作者: *电子信箱: ligaoren@scu.edu.cn (李高仁).
  • 基金资助:
    国家基础研究计划(2016YFA0202603);国家自然科学基金(91645104);四川省自然科学基金(2023NSFSC0086);中央高校基本研究经费(YJ2021156)

Syntheses and applications of single-atom catalysts for electrochemical energy conversion reactions

Qi-Ni Zhan, Ting-Yu Shuai, Hui-Min Xu, Chen-Jin Huang, Zhi-Jie Zhang, Gao-Ren Li*()   

  1. College of Materials Science and Engineering, Sichuan University, Chengdu 610065, Sichuan, China
  • Received:2022-10-21 Accepted:2022-12-22 Online:2023-04-18 Published:2023-03-20
  • Contact: *E-mail: ligaoren@scu.edu.cn (G. Li).
  • About author:Prof. Gao-Ren Li (College of Materials Science and Engineering, Sichuan University) received his B.A. degree from East China University of Technology in 2000, and Ph.D. degree from Sun Yat-sen University in 2005. From September 2005 to September 2021, he worked in School of Chemistry, Sun Yat-sen Universtiy. Since October 2021, he has been working in College of Materials Science and Engineering, Sichuan University. His current research interests mainly focus on electrocatalysis, especially water splitting and electrochemical conversion of CO2.
  • Supported by:
    National Basic Research Program of China(2016YFA0202603);National Natural Science Foundation of China(91645104);Natural Science Foundation of Sichuan Province(2023NSFSC0086);Fundamental Research Funds for the Central Universities(YJ2021156)

摘要:

自2011年张涛院士等首次提出单原子催化剂(SACs)概念以来, 单原子催化迅速成为研究热点. SACs具有最大的原子利用率、独特的结构和性能, 因而在催化领域具有很好的应用前景, 备受关注.

本文首先介绍了基于自下而上和自上而下合成策略的各种SACs制备方法以及近年来相应的研究进展, 其中包括浸渍法、共沉淀法、原子层沉积法等较为传统的催化剂合成策略, 以及缺陷设计法、空间限域法和火焰喷雾热解法等新方法, 并详述了这些制备方法在实际应用中的优缺点. 对于电催化原理分析方面, 较详细地介绍了各电化学能源转换领域相关催化反应的理论计算结果以及各催化反应相应的原理与途径. 然后重点介绍了含贵金属(Pt, Pd, Ir等)和非贵金属(Fe, Cu, Co等)的SACs在析氧反应、析氢反应、氧还原反应、CO2还原反应和氮还原反应中的电催化应用. 最后讨论了SACs的应用前景和未来面临的挑战: (1) 深入进行SACs制备方法的研究, 提高合成策略的实际应用可行性以推进催化剂的工业化进程; (2) 提高SACs中金属负载量, 以提升其催化性能; (3) 结合理论计算, 增强对SACs配位环境、电子结构的精确控制, 进而优化催化剂的催化性能; (4) 由于高原子表面能, 单原子催化剂在催化应用中需解决活性金属单原子容易出现的团聚问题, 因此, 提高催化剂稳定性是SACs催化性能研究的重要方向; (5) 单原子催化剂的结构简单均一, 这非常有利于理论计算研究, 目前仍有很多单原子的催化机理尚未明确, 可基于理论模拟进一步加深对单原子催化机理的研究. 虽然SACs在未来的开发研究中仍面临着诸多亟待解决的问题, 但其未来应用潜力非常令人期待; 经过不断的发展创新, 高性能低成本的单原子催化剂将在工业化生产以及新能源发展中扮演着越来越重要的角色.

关键词: 单原子催化剂, 电催化, 析氧反应, 析氢反应, 氧还原反应, 二氧化碳还原反应, 氮还原反应

Abstract:

Singe-atom catalysts (SACs), as heterogeneous catalysts, have attracted increasing attention in recent years owing to their numerous advantages in the field of electrocatalysis, such as a high atom-utilization rate and unique structural characteristics. In this review, we introduce various preparation methods for obtaining SACs based on top-down and bottom-up synthesis strategies and the corresponding research progress made in recent years. We also focus on the electrocatalytic applications of SACs containing noble metals (Pt, Pd, Ir, etc.) and non-noble metals (Fe, Cu, Co, etc.) in the oxygen evolution reaction, hydrogen evolution reaction, oxygen reduction reaction, carbon dioxide reduction reaction, and nitrogen reduction reaction. Finally, the future challenges and prospects of monatomic catalysts are also discussed.

Key words: Single atom catalyst, Electrocatalysis, Oxygen evolution reaction, Hydrogen evolution reaction, Oxygen reduction reaction, CO2 reduction reaction, Nitrogen reduction reaction