Acta Chimica Sinica ›› 2026, Vol. 84 ›› Issue (5): 775-804.DOI: 10.6023/A26010037 Previous Articles    

Review

基于金属有机框架的中性介质硝酸盐电催化还原制氨: 设计策略与机理研究

何乾龙, 胡洁颖, 钟礼匡*(), 何军*()   

  1. 广东工业大学 轻工化工学院 广州 510006 广东省 中国
  • 投稿日期:2026-01-31 发布日期:2026-04-03
  • 通讯作者: 钟礼匡, 何军
  • 作者简介:

    ★“框架材料化学”专辑

  • 基金资助:
    国家自然科学基金(22371054); 国家自然科学基金(22301045); 广东省基础与应用基础研究基金(2024A1515012801); 广东省基础与应用基础研究基金(2024B1515120009); 国家资助博士后研究人员计划(GZC20240311)

Metal-Organic Framework-Based Electrocatalysts for Neutral Nitrate-to-Ammonia Conversion: Design Strategies and Mechanistic Insights

Qianlong He, Jieying Hu, Lai-Hon Chung*(), Jun He*()   

  1. School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, Guangdong, China
  • Received:2026-01-31 Published:2026-04-03
  • Contact: Lai-Hon Chung, Jun He
  • About author:

    Qianlong He is now pursuing a master's study under the supervision of Prof. Jun He at Guangdong University of Technology. His research interests focus on MOF-based catalysts for electrocatalytic nitrate reduction.

    Jieying Hu received her PhD in Chemical Engineering and Technology from Guangdong University of Technology in 2023 under the supervision of Prof. Jun He. She is currently a Postdoctoral Researcher at Guangdong University of Technology, in ongoing collaboration with Prof. Jun He, working on the design and synthesis of sulfur- and alkyne-enriched porous organic frameworks and on their applications.

    Lai-Hon Chung is an Associate Professor at the School of Light Industry and Chemical Engineering, Guangdong University of Technology. He received his bachelor’s degree from City University of Hong Kong in 2010 and his PhD in 2015 under the supervision of Professor Chun-Yuen Wong. His early research focused on organometallic chemistry, particularly transition-metal-mediated alkyne cyclization and functionalization mechanisms, as well as exploration of metalated heterocycles. He joined Guangdong University of Technology in 2019 and was promoted to Associate Professor in 2025. He has published over 70 SCI-indexed papers and co-authored two book chapters. His current research interests focus on metallolinker-based crystalline frameworks for sustainable catalysis.

    Jun He is currently a Professor, PhD supervisor, and Vice Dean of the School of Light Industry and Chemical Engineering at Guangdong University of Technology. He has been selected as a Distinguished Professor under the Pearl River Scholars Program of Guangdong Province, a recipient of Guangdong Provincial Science Fund for Distinguished Young Scholars, and a Top Young Talent of the Guangdong Special Support Program (the “Hundred-Thousand-Ten Thousand” Young Talent Project). His research focuses on the design and synthesis of sulfur-enriched metal-organic frameworks (MOFs) and covalent organic frameworks (COFs), as well as their applications in energy catalysis and conversion. He has published nearly 150 SCI-indexed papers in leading journals, including JACS, Angew. Chem., Nat. Commun., CCS Chem., and holds over 20 granted invention patents. He has served as principal investigator for multiple projects funded by the National Natural Science Foundation of China (4 grants), Department of Science and Technology of Guangdong Province (15 grants) and industries (>10 grants).

    ★ For the VSI “Chemistry of Framework Materials”.

  • Supported by:
    National Natural Science Foundation of China(22371054); National Natural Science Foundation of China(22301045); Foundation of Basic and Applied Basic Research of Guangdong Province(2024A1515012801); Foundation of Basic and Applied Basic Research of Guangdong Province(2024B1515120009); Postdoctoral Fellowship Program of CPSF(GZC20240311)

With the continuous development of agriculture and industry, nitrate (NO3) pollution in water bodies worldwide remains a serious issue, characterized by decentralized distribution across multiple sites. The electrocatalytic nitrate reduction reaction (eNO3RR) technology enables the reduction of NO3 waste into ammonia (NH3)—a substance useful to humans—under ambient temperature and pressure. However, under near-neutral pH conditions that mimic actual aquatic environments, eNO3RR faces multiple bottlenecks, including limited proton supply, competition from hydrogen evolution side reactions, risks of nitrite (NO2) accumulation, and insufficient catalyst lifespan. Metal-organic framework (MOF) materials, which have attracted significant attention recently, hold tremendous potential. Their tunable porous structures and well-defined active sites are conducive to improving NO3 reduction efficiency and selectivity. Remarkable progress has been made in this field: advanced MOF-based materials have achieved an NH3 Faraday efficiency (FE) of nearly 99%, suppressed NO2 accumulation, and pushed the NH3 yield to >23000 μg•h−1•mgcat−1. By constructing conductive composite structures and employing derivatization strategies, MOF-based materials can maintain a FE of >90% and remain stable for over 10 h at industrial-level current densities (>950 mA•cm-2). This review focuses on MOF-based electrocatalysts and systematically analyzes the mechanism of neutral eNO3RR. Leveraging the atomic-level designability of MOFs, strategies such as single-atom/cluster regulation, multi-metal synergy, conductive composites, and derivatization can precisely overcome the bottlenecks of proton supply, hydrogen evolution competition, and stability in neutral eNO3RR, enabling efficient conversion of pollutants to NH3. Nevertheless, several challenges remain before this goal is fully achieved: the dynamic identification of active centers during catalysis is not sufficiently clear and accurate, long-term stability in real water bodies needs verification, and issues such as large-scale synthesis urgently require solutions.

Key words: metal-organic framework (MOF), MOF derivatives, electrocatalytic nitrate reduction reaction, ammonia synthesis, neutral conditions