基于含氮杂环配体的金属有机框架材料在电催化CO2还原中的应用与前景展望★

doi:10.6023/A26020053

综述

基于含氮杂环配体的金属有机框架材料在电催化CO₂还原中的应用与前景展望^★

张亚^a,*, 周功兵^a, 孙为银^b,*

^a重庆师范大学化学与材料科学学院,绿色催化材料与技术重庆市重点实验室,重庆 401331;
^b南京大学化学学院,配位化学全国重点实验室,南京 210023

投稿日期:2026-02-10
作者简介:张亚,重庆师范大学化学与材料科学学院讲师,2024年于南京大学化学化工学院获博士学位,主要从事金属有机框架及其复合材料、过渡金属纳米材料的可控合成及其在电催化小分子（CO₂/H₂O/N₂）转化领域的应用。周功兵,重庆师范大学化学与材料科学学院教授,2009年于华南理工大学获学士学位（应用化学专业）,2014年于复旦大学获博士学位（物理化学专业)。目前研究方向为金属纳米催化剂的结构调控及其在生物质小分子催化转化、电催化水分解中的应用。孙为银,南京大学化学学院教授,1986年上海华东师范大学化学系本科毕业,1990年和1993年在日本大阪大学分别获得硕士和理学博士学位。近期的研究重点是利用金属有机框架及其衍生材料光/电催化CO₂还原。已发表超过400篇研究论文,担任J. Coord. Chem. 编委,CrystEngComm顾问编委,并自2014年起成为英国皇家化学学会会士（FRSC）。
基金资助:
项目受国家自然科学基金(Nos. 22231006和21703024),重庆市自然科学基金(CSTB2025NSCQ-GPX0259),重庆市教委科技项目(No. KJZDK202200514)和重庆师范大学基金项目(No. 24XLB028)资助

Recent Advance and Perspective of Metal-Organic Frameworks Based on Nitrogen-Containing Heterocyclic Ligands for Electrocatalytic CO₂ Reduction

Ya Zhang^a,*, Gongbing Zhou^a, Wei-Yin Sun^b,*

^aChongqing Key Laboratory of Green Catalysis Materials and Technology, College of Chemistry and Materials Science, Chongqing Normal University, Chongqing 401331, China;
^bState Key Laboratory of Coordination Chemistry, School of Chemistry, Nanjing University, Nanjing 210023, China

Received:2026-02-10
Contact: *E-mail: yazhang@cqnu.edu.cn; sunwy@nju.edu.cn
Supported by:
National Natural Science Foundation of China (Nos. 22231006 and 21703024), the Natural Science Foundation of Chongqing, China (CSTB2025NSCQ-GPX0259), the Science and Technology Research Program of Chongqing Municipal Education Commission of China (No. KJZDK202200514), and the Chongqing Normal University Foundation (No. 24XLB028).

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摘要/Abstract

降低大气中二氧化碳（CO₂）浓度以实现碳中和,已成为环境科学与可持续发展领域一项紧迫的全球性挑战。利用电催化CO₂还原反应（electrocatalytic CO₂ reduction reaction, ECRR）可制备高附加值化学品与燃料,为减少CO₂排放、将可再生电能转化为化学能提供了一种极具前景的方法。金属有机框架（metal-organic frameworks, MOFs）是一种具有潜力的ECRR催化剂,得益于其多孔、结构清晰且可调节的框架结构,这有利于CO₂富集,并有助于探索结构-性能之间关系和催化反应机理。基于含氮杂环配体MOFs材料因其独特的物理化学特性在ECRR研究中备受关注,这些特性包括灵活多样的框架、丰富的活性位点和高稳定性等。本综述系统评述了基于含氮杂环配体MOFs材料的相关性质和表征手段,并按含氮杂环结构类别,即咪唑基、吡唑基、三唑基、四唑基等,归纳了含氮杂环配体MOFs材料在ECRR领域的最新研究进展。最后,剖析了当前制约该类MOFs在ECRR实际应用方面的关键挑战,包括本征导电性不足、在长时间运行条件下结构和电化学稳定性问题、电解槽系统集成以及催化反应过程中动态结构演变导致的机理模糊等,并在此基础上对未来研究方向进行了展望。

关键词: 金属有机框架, 含氮杂环配体, CO₂还原反应, 电催化转化

Achieving carbon neutrality through reducing amounts of atmospheric carbon dioxide (CO₂) has emerged as an urgent global challenge in the fields of environmental science and sustainable development. Among the emerging mitigation strategies, electrocatalytic CO₂ reduction reaction (ECRR) stands out for its capacity to convert CO₂ into high-valued chemicals or energy-dense fuels, providing a promising approach for reducing CO₂ emissions and converting renewable electric energy into chemical energy. Metal-organic frameworks (MOFs) represent a promising class of catalysts for ECRR, owing to their intrinsic structural advantages—including well-defined porosity and atomic-level structural tunability—which collectively enhance CO₂ mass transport and adsorption, and enable systematic investigation of structure-activity relationship as well as reaction mechanism. In particular, MOFs constructed from nitrogen-containing heterocyclic ligands have garnered remarkable research interests, attributed to their superior features such as structural flexibility, abundant catalytic sites and suitable stability. This review outlines the fundamental physicochemical properties and advanced characterization techniques for the nitrogen-containing heterocyclic ligand-based MOFs. Then recent advances in the application of such MOFs to ECRR were summarized categorizing by the nitrogen-containing moieties, namely imidazolyl-, pyrazolyl-, triazolyl- and tetrazolyl-based ligands. Finally, this review analyzed the critical challenges impeding the practical application of nitrogen-containing heterocyclic ligand-based MOFs in ECRR, including intrinsic electronic conductivity limitations, structural and electrochemical stability under prolonged operational conditions, integration of electrolyze systems and mechanistic ambiguities arising from dynamic structural evolution during the ECRR. On this basis, prospects for future research directions are presented.

Key words: Metal-organic frameworks, nitrogen-containing heterocyclic ligands, CO₂ reduction reaction, electrocatalytic conversion

引用此文

张亚, 周功兵, 孙为银. 基于含氮杂环配体的金属有机框架材料在电催化CO₂还原中的应用与前景展望^★[J]. 化学学报, doi: 10.6023/A26020053.

Ya Zhang, Gongbing Zhou, Wei-Yin Sun. Recent Advance and Perspective of Metal-Organic Frameworks Based on Nitrogen-Containing Heterocyclic Ligands for Electrocatalytic CO₂ Reduction[J]. Acta Chimica Sinica, doi: 10.6023/A26020053.

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基于含氮杂环配体的金属有机框架材料在电催化CO₂还原中的应用与前景展望^★

Recent Advance and Perspective of Metal-Organic Frameworks Based on Nitrogen-Containing Heterocyclic Ligands for Electrocatalytic CO₂ Reduction

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