Synthesis and Electrochemical Performance of Single-Atom Catalysts Derived from Metal-Organic Frameworks  

金属-有机骨架单原子催化剂的合成及其电化学性能

作　　者：Yu Zhang Xiaoxiao Su Xinmei Du Lan Wei Hao Zhang Ling Jiang 张钰;苏晓晓;杜欣媚;蔚蓝;张昊;江凌(信阳师范大学化学化工学院,信阳464000;信阳师范大学建筑与土木工程学院,信阳464000;美国麻省理工学院化学工程系,剑桥02139;中国科学院大连化学物理研究所分子反应动力学国家重点实验室,大连116023)

机构地区：[1]College of Chemistry and Chemical Engineering,Xinyang Normal University,Xinyang 464000,China [2]College of Architecture and Civil Engineering,Xinyang Normal University,Xinyang 464000,China [3]Department of Chemical Engineering,Massachusetts Institute of Technology,Cambridge MA 02139,USA [4]State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China

出　　处：《Chinese Journal of Chemical Physics》2025年第2期125-139,I0039,共16页化学物理学报(英文)

基　　金：supported by Henan Province Key Research and Development and Promotion of Science and Technology Project(No.25A150001);the National Natural Science Foundation of China(Nos.22409171,22125303,92361302,and 92061203).

摘　　要：Single-atom catalysts(SACs),as the rising stars in the field of catalytic science,are leading catalytic technology into an un-precedented new era.However,the synthe-sis of high-performance SACs with well-de-fined active sites and high loadings under precise control has become a hotly debated topic in scientific research.Metal-organic frameworks(MOFs),with their exceptional properties such as ultrahigh specific surface areas,precisely controllable structural de-signs,and highly flexible functional cus-tomization capabilities,are regarded as one of the ideal matrices for supporting and sta-bilizing SACs.This review provides an in-sightful overview of the diverse preparation strategies for MOFs-derived SACs.It comprehen-sively analyzes the unique advantages and challenges of each method in achieving efficient synthesis of SACs,emphasizing the crucial role of optimized processes in unlocking the antici-pated performance of SACs.Furthermore,this review delves into a series of advanced charac-terization techniques,including aberration-corrected scanning transmission electron mi-croscopy(AC-STEM),electron energy loss spectroscopy(EELS),X-ray absorption spec-troscopy(XAS),and infrared absorption spectroscopy(IRAS),offering valuable insights into the atomic-scale fine structures and properties of SACs,significantly advancing the under-standing of SAC mechanisms.Moreover,this review focuses on exploring the potential appli-cations of MOFs-derived SACs in electrocatalysis frontier fields.This comprehensive exami-nation lays a solid theoretical foundation and provides a directional guidance for the rational design and controllable synthesis of high-performance MOFs-derived SACs.单原子催化剂作为催化科学领域的璀璨新星,正引领催化技术步入一个前所未有的新时代.然而,如何在精确控制下合成具有明确活性位点和高负载量的高性能单原子催化剂已成为科研领域热议的话题.金属有机框架凭借其超高比表面积、精确可控的结构设计以及高度灵活的功能定制能力等卓越特性,被视为支撑和稳定单原子催化剂的理想载体之一.本文综述了金属有机框架衍生单原子催化剂的多种制备策略,全面分析了每种方法在高效合成单原子催化剂方面的独特优势与面临的挑战,并着重强调了优化工艺在发挥单原子催化剂预期性能中的关键作用.此外,文章还深入探讨了包括像差校正扫描透射电子显微镜、电子能量损失谱、X射线吸收光谱和红外吸收光谱在内的一系列先进表征技术,为揭示单原子催化剂的原子级精细结构和性质提供了宝贵见解,极大推进了对单原子催化剂机制的理解.同时,本文还探讨了金属有机框架衍生单原子催化剂在电催化前沿领域的潜在应用.本综述为高性能金属有机框架衍生单原子催化剂的合理设计与可控合成奠定了坚实的理论基础,并提供了方向性的指导.

关 键 词：Single-atom catalysts Metal-organic frameworks High-temperature pyrolysis Characterization methods Electrocatalysis applications 

分 类 号：O643.36[理学—物理化学]