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    共价有机框架材料在光/电催化制备过氧化氢中的研究进展

    Research Progress of Covalent Organic Frameworks in Photocatalytic and Electrocatalytic Hydrogen Peroxide Production

    • 摘要: 光/电催化制备过氧化氢(H2O2)具有反应条件温和、原料来源广泛以及可利用太阳能或可再生电力等优势,为H2O2的绿色、分布式生产提供了新的技术途径。然而,H2O2合成过程中存在多种竞争反应,其催化活性和选择性高度依赖催化剂的结构、电子性质及活性位点。共价有机框架(COFs)作为一类结构可设计的晶态多孔材料,具有有序孔道、高比表面积和骨架易修饰等优点,可实现电子结构、活性位点和反应微环境的灵活调控,在光/电催化H2O2合成领域展现出良好的应用潜力。围绕近年来COFs光/电催化制备H2O2的研究进展,本文首先概述H2O2光/电催化合成的基本反应原理,随后分别总结COFs在光/电催化H2O2合成中的研究进展,重点从骨架与电子结构、活性位点与反应路径、载流子/电子传输以及反应微环境等方面归纳材料结构调控策略,并分析不同结构对H2O2生成速率性、选择性及稳定性的影响。在此基础上,总结当前COFs用于H2O2光/电催化合成面临的关键问题,并对高效催化剂设计、界面传质与电子传输优化以及器件化发展等方向进行展望,为COFs催化材料的理性设计及H2O2高效、可持续合成提供参考。

       

      Abstract: Photocatalytic and electrocatalytic production of hydrogen peroxide (H2O2) offers the advantages of mild reaction conditions, abundant raw materials, and the utilization of solar energy or renewable electricity, providing new routes for the green and distributed production of H2O2. However, multiple competing reactions occur during H2O2 synthesis, and the catalytic activity and selectivity are highly dependent on the structure, electronic properties, and active sites of the catalysts. Covalent organic frameworks (COFs), as a class of structurally designable crystalline porous materials, feature ordered channels, high specific surface areas, and readily modifiable frameworks, enabling flexible regulation of electronic structures, active sites, and reaction microenvironments, and thus showing great potential for photocatalytic and electrocatalytic H2O2 synthesis. Focusing on recent advances in COFs-based photocatalytic and electrocatalytic H2O2 production, this review first outlines the fundamental reaction principles of photocatalytic and electrocatalytic H2O2 production, and then summarizes recent advances in COF-based photocatalytic and electrocatalytic H2O2 synthesis, with emphasis on regulation strategies involving framework and electronic structures, active sites and reaction pathways, charge/electron transport, and reaction microenvironments. The relationships between structural features and H2O2 production activity, selectivity, and stability are further discussed. Finally, the key challenges and future directions of COFs-based photocatalytic and electrocatalytic H2O2 production are summarized and discussed, providing insights into the rational design of COFs-based catalysts and the efficient and sustainable production of H2O2.

       

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