金属团簇电催化合成含氮化合物: 设计与应用

doi:10.1016/S1872-2067(26)65185-6

催化学报 ›› 2026, Vol. 90: 82-116.DOI: 10.1016/S1872-2067(26)65185-6

金属团簇电催化合成含氮化合物: 设计与应用

伊尔沙德·艾哈迈德^a^,^b, 王莎莎^a^,^*(), 穆罕默德·卡西姆·阿尔法伊菲^c, 优素福·阿尔拉希德^d, 法哈德·阿尔巴基^d, 李杲^a^,^*()

^a 内蒙古师范大学化学与环境科学学院, 内蒙古呼和浩特 010022, 中国
^b 农业大学物理系, 费萨拉巴德, 巴基斯坦
^c 阿卜杜勒阿齐兹国王科技城氢技术研究所, 利雅得, 沙特阿拉伯
^d 阿卜杜勒阿齐兹国王科技城炼油技术与石化研究所, 利雅得, 沙特阿拉伯

收稿日期:2026-01-21 接受日期:2026-03-20 出版日期:2026-11-18 发布日期:2026-09-09
通讯作者: *电子信箱: li_gao82@yeah.net (李杲),
shasha@imnu.edu.cn (王莎莎).
基金资助:
国家自然科学基金(22065029)

Advancing metal cluster-based electrocatalysis for C-N synthesis: Fundamental, design strategies, and applications

Irshad Ahmad^a^,^b, Shasha Wang^a^,^*(), Mohammed Qasem Alfaifi^c, Yousef I. Alrashed^d, Fahad M. Albaqi^d, Gao Li^a^,^*()

^a College of Chemistry and Environmental Science, Inner Mongolia Normal University, Hohhot 010022, Inner Mongolia, China
^b Department of Physics, University of Agriculture, Faisalabad 38040, Pakistan
^c Hydrogen Technologies Institute, King Abdulaziz City for Science and Technology (KACST), Riyadh 11442, Saudi Arabia
^d Refining Technologies and Petrochemicals Institute (RTPI), King Abdulaziz City for Science and Technology (KACST), Riyadh 11442, Saudi Arabia

Received:2026-01-21 Accepted:2026-03-20 Online:2026-11-18 Published:2026-09-09
Contact: *E-mail:li_gao82@yeah.net(G. Li),shasha@imnu.edu.cn(S. Wang).
About author:Shasha Wang (Inner Mongolia Normal University) received his B.A. degree from Inner Mongolia University of Technology (China, 2011), Master from Dalian Maritime University (2013) and Ph.D. from Inner Mongolia University (China, 2018). And then she joined Inner Mongolia Normal University as a Associate Professor. Her current research interests include the controlled synthesis of nanomaterials (e.g. rare-earth upconversion luminescent materials) and their applications in energy catalysis. She has published > 10 peer-reviewed papers and granted 2 authorized patents.
Gao Li (Inner Mongolia Normal University) received his B.A. degree from Hunan Normal University (China) in 2004, and Ph.D. degree from Shanghai Jiaotong University (China) in 2011. He carried out postdoctoral research at Carnegie Mellon University (USA. 2011 to 2014). And then he worked for State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences from 2014 to 2025. After that he joined Inner Mongolia Normal University. His current research interests focused on the preparation and application of gold clusters. His research interests mainly focus on (i) Synthesis and application of metal nanoclusters: structure-composition-function correlations, and (ii) Functionalization of metal nanoclusters for emerging deployments: structure-activity correlation structure-performance relationship. He has published over 200 peer-reviewed papers.
Supported by:
National Natural Science Foundation of China(22065029)

摘要/Abstract

摘要：

全球可再生能源的迅猛扩张, 使得如何高效地存储、运输并将电能转化为具有高社会价值的化学能源, 已成为亟待解决的全球性挑战. 电化学合成作为一种强大而灵活的平台异军突起, 通过将电子直接转化为化学键, 在可再生能源与可持续化学制造之间架起了一座桥梁. 相较于通常伴随高能耗与高碳排放的传统热化学路线, 电化学过程能够在常温条件下运行, 并利用电极电位实现对反应路径与产物选择性的精准调控, 因而成为一种极具吸引力的替代方案. 其中碳-氮(C-N)键的电化学构建占据着举足轻重的战略地位. C-N偶联产物是肥料、燃料、聚合物、医药及精细化学品的物质基础, 构成了现代工业支柱. 电化学C-N偶联技术有望利用可再生能源, 直接驱动CO₂或CO等碳一化合物与NH₃, NO₃^-及N₂等含氮原料的偶联反应, 从而为高附加值含氮化合物的绿色合成开辟出一条新路径.

原子级金属纳米团簇作为一类独特的前沿电催化材料, 凭借其离散的电子结构与可精细调控的配体环境, 为在原子水平上调控反应物吸附、活化及质子-电子转移动力学提供了可能, 从而为直接合成高附加值化学品开辟了新途径. 本文系统综述了金属团簇基电催化剂在电化学C-N偶联中的研究进展. 首先, 简要介绍了金属纳米团簇的基本特性、可控合成策略及其在电催化领域研究进展及优势. 其后, 通过重点介绍一些典型研究, 详细梳理了其在尿素、氨、胺、酰胺、肟及氨基酸等重要化学品合成中的设计原理和具体应用, 并重点探讨了团簇的组成、尺寸及局部配位环境与产物选择性、催化耐久性之间的构效关系和反应机理. 最后, 本文探讨了金属团簇基电催化剂在电催化研究方面所面临的挑战和未来的研究方向: (1)在理论研究方面, 通过精准设计质子穿梭体与导电载体, 协同调控团簇电催化剂的质子-电子传递路径, 建立电荷密度与选择性的定量关系, 并阐明配体特性对反应微环境及中间体的调控机制, 以实现C-N偶联过程的理性设计; (2)利用原子级精确的团簇模型, 结合不对称设计、同位素标记及原位光谱技术, 精准解析C-N键形成的位点与机理; 并通过脉冲电位和流动池等手段将活化与偶联步骤解耦, 构建氧化态依赖的定量反应图谱; (3)采用双锚定与多孔基质限域策略, 抑制团簇在真实工况下的迁移流失, 并结合标准化的长时工业级应力测试与原位结构监测, 建立兼顾活性与稳定性的评价体系, 为规模化应用加速准备; (4)于膜电极组件中评估团簇催化剂在百毫安级大电流下的性能, 并结合克级可扩展合成、技术经济分析及标准化基准测试(包括部分电流密度、法拉第效率、能量效率和长期稳定性), 以加速其在工业氮转化过程中的集成应用.

总之, 本综述剖析了团簇催化剂在稳定性、规模化制备及工业集成方面的瓶颈, 提出了下一代催化剂的理性设计原则, 旨在为电催化构建C-N键绘制清晰路线图, 推动绿色含氮化学品合成技术的发展.

关键词: 电催化剂, 金属团簇, C-N偶联, 合成方法, 法拉第效率

Abstract:

The escalating demand for sustainable nitrogen-containing chemicals calls for transformative electrocatalytic strategies that can precisely orchestrate C-N bond formation. Atomically defined metal nanoclusters have emerged as a frontier in electrocatalysis, enabling the direct synthesis of chemicals via C-N coupling. Their discrete electronic structures and tunable ligand environments permit atomic-level control over adsorption, activation, and proton-electron transfer dynamics, overcoming the intrinsic kinetic and thermodynamic challenges of multi-electron C-N coupling reactions. Here, we present a comprehensive overview of cluster-based electrocatalysts, encompassing cluster properties, synthetic routes, mechanistic insights, performance descriptors critical for evaluating catalytic efficiency, and their applications in the synthesis of urea, ammonia, amines, amides, oximes, and amino acids. We focus on the correlations between cluster composition, size, and local coordination in dictating product distribution and catalytic durability. Finally, we identify current bottlenecks in stability, scalability, and industrial integration, and propose rational design principles for engineering next-generation clusters to achieve sustainable, high-value nitrogen chemical production. This review frames a roadmap for exploiting atomic precision in electrocatalysis, charting a path toward transformative C-N bond-forming technologies.

Key words: Electrocatalyst, Metal clusters, C-N coupling, Synthesis methods, Faradic efficiency

伊尔沙德·艾哈迈德, 王莎莎, 穆罕默德·卡西姆·阿尔法伊菲, 优素福·阿尔拉希德, 法哈德·阿尔巴基, 李杲. 金属团簇电催化合成含氮化合物: 设计与应用[J]. 催化学报, 2026, 90: 82-116.

Irshad Ahmad, Shasha Wang, Mohammed Qasem Alfaifi, Yousef I. Alrashed, Fahad M. Albaqi, Gao Li. Advancing metal cluster-based electrocatalysis for C-N synthesis: Fundamental, design strategies, and applications[J]. Chinese Journal of Catalysis, 2026, 90: 82-116.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65185-6

https://www.cjcatal.com/CN/Y2026/V90/I11/82

图/表 14

Fig. 1. Schematic illustration of this review.

Fig. 2. Timeline of cluster-based electrocatalysts for CO2RR, HER, NH3 synthesis, OER, amino acid, oxime, and amine synthesis reactions is outlined.

Fig. 3. Properties of nanoclusters for electrocatalytic C-N coupling reactions.

Fig. 4. Schematic illustration of significant evaluation indices for electrocatalytic performance.

Fig. 5. Schematic illustration of urea synthesis via electroreduction vs. electrocatalytic C-N coupling under ambient conditions.

Fig. 6. The advantages and disadvantages of different synthesis methods for cluster-based electrocatalysts.

Fig. 7. (a,b) FEs comparison of Pd4Cu1-Ni(OH)2 and Pd4Cu1-FeNi(OH)2 for electrosynthesis of urea. Reprinted with permission from Ref. [11]. Copyright 2024, John Wiley and Sons. (c) In-situ FTIR spectroscopy analysis under applied bias for Cu1-CeO2 during electrocatalytic CO2-NO3-electroreduction. Reprinted with permission from Ref. [13]. Copyright 2023, John Wiley and Sons. (d) Various intermediates’ free energy and reaction routes on POP in the electroreduction of nitrogen and carbon dioxide. Reprinted with permission from Ref. [12]. Copyright 2024, Elsevier B.V.

Fig. 8. STEM image (a), Fe 2p (b), and N 1s (c) XPS spectra, and potential dependent urea synthesis performance (d) of FeNC-Fe1N4. Reprinted with permission from Ref. [16]. Copyright 2024, John Wiley and Sons. TGA analysis (e) and UV-vis spectra (f) verifying the light resistance of Au13Ag12:BMIm. Reprinted with permission from Ref. [17]. Copyright 2025, John Wiley and Sons.

Fig. 9. (a) Synthesis scheme of Ni6@CuFe-LDH. (b) Mechanistic pathway of CuFe-LDH and Ni6@CuFe-LDH. Reprinted with permission from Ref. [18]. Copyright 2025, American Chemical Society. Synthesis (c) and electroreduction NO3- to NH3 (d) over clusters (Fe2M-MOF, M = Fe, Co, Ni, Zn). Reprinted with permission from Ref. [41]. Copyright 2022, John Wiley and Sons.

Fig. 10. (a) Synthesis scheme of Ru1Cu SAA. Reprinted with permission from Ref. [46]. Copyright 2023, Springer Nature. Catalytic performance (b) and durability (c) of Cu12Ag17, Cu12Ag16Au1 and Ag28Au1 for the formylation of CO2 with secondary amines. Reprinted with permission from Ref. [48]. Copyright 2023, American Chemical Society.

Fig. 11. (a) Synthesis scheme. (b) ATR-SEIRAS measurements of Ag16Cu18(C≡C-C6H11)24 nanocluster. Reprinted with permission from Ref. [119]. Copyright 2023, John Wiley and Sons. (c) DFT and (d) electroreduction route of NO3− to NH2OH over Ag4Pd2-S-Ti4. Reprinted with permission from Ref. [50]. Copyright 2025, John Wiley and Sons.

Fig. 12. Cu k-edge XANES (a) and k3-weighted FT-EXAFS (b) spectra of Cu-SAs-CBC and Cu-SAs/ACs-CBC. Reprinted with permission from Ref. [64]. Copyright 2023, John Wiley and Sons. Synthesis scheme (c) and FE (d) of cyclohexanone oxime. Reprinted with permission from Ref. [65]. Copyright 2024, John Wiley and Sons.

Fig. 13. Synthesis scheme (a) and EXFAS spectra (b) of AD-Fe/NC. Synthesis scheme (c) and trinuclear copper sites (d) for F-Cu3-OFobtained from XANES analysis. Reprinted with permission from Refs. [66] and [67]. Copyright 2024, American Chemical Society and Elsevier B.V.

Fig. 14. Schematic illustration of unaddressed current gaps, research targets, and future avenues for cluster-based electrocatalysts for C-N coupling reactions [165-168].

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金属团簇电催化合成含氮化合物: 设计与应用

Advancing metal cluster-based electrocatalysis for C-N synthesis: Fundamental, design strategies, and applications

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