用于高效光催化水分解和原位水处理的氮杂环共价有机框架
Nitrogen heterocyclic covalent organic frameworks for efficient HO photosynthesis and in situ water treatment.
作者信息
Chen Zhong, Weng Hao, Chu Chengcheng, Yao Ducheng, Li Qiuju, Zhang Chen, Mao Shun
机构信息
College of Environmental Science and Engineering, State Key Laboratory of Water Pollution Control and Green Resource Recycling, Tongji University, Shanghai, China.
Shanghai Institute of Pollution Control and Ecological Security, Shanghai, China.
出版信息
Nat Commun. 2025 Jul 28;16(1):6943. doi: 10.1038/s41467-025-62371-z.
Nitrogen heterocyclic covalent organic frameworks offer great potential for HO production due to their unique optical and electrical properties. Herein, we design four photocatalysts with varying nitrogen atom configurations to tune their electronic and energy-band structures. Among them, the covalent organic frameworks with pyrimidine achieves an efficient HO production rate of 17014 μmol g h and a solar-to-chemical conversion efficiency of 1.84% in pure water without sacrificial agent or oxygen aeration. The theoretical calculation and experimental study confirm that it owns superior photoelectrochemical properties, oxygen reduction reaction activity, and the lowest reaction potential barrier, enabling dual channel HO production via 2e oxygen reduction reaction and 4e water oxidation reaction. To explore the application potential of the photocatalytic system, a panel reactor (20 × 20 cm) under natural sunlight demonstrates continuous HO generation for antibiotic degradation and long-lasting water disinfection. This work presents an advanced photocatalytic HO synthesis system with high efficiency and environmental remediation potential.
氮杂环共价有机框架由于其独特的光学和电学性质，在产过氧化氢方面具有巨大潜力。在此，我们设计了四种具有不同氮原子构型的光催化剂，以调节其电子和能带结构。其中，含嘧啶的共价有机框架在无牺牲剂或氧气曝气的纯水中实现了17014 μmol g⁻¹ h⁻¹的高效过氧化氢产率和1.84%的太阳能到化学能转换效率。理论计算和实验研究证实，它具有优异的光电化学性质、氧还原反应活性和最低的反应势垒，能够通过2e氧还原反应和4e水氧化反应实现双通道过氧化氢生成。为了探索光催化系统的应用潜力，一个20×20 cm的平板反应器在自然阳光下展示了用于抗生素降解的持续过氧化氢生成和持久的水消毒效果。这项工作提出了一种具有高效性和环境修复潜力的先进光催化过氧化氢合成系统。
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