碳基非金属纳米材料用于二电子氧还原制备过氧化氢的研究进展

Research progress on carbon-based non-metallic nanomaterials as catalysts for the two-electron oxygen reduction for hydrogen peroxide production

  • 摘要: 电催化二电子氧还原反应(2e-ORR)制备过氧化氢(H2O2)凭借其高效、安全和绿色特点,逐步发展为一种可能替代工业蒽醌法的新途径。碳基纳米材料具有电子导电性高、结构稳定性好、纳米结构调控容易、成本低等优势,是一类具有良好前景的2e-ORR制备H2O2的催化剂。针对该类碳基电催化材料的发展现状及相应材料上的活性中心和反应机制进行详细论述有助于对本领域的最新进展实现全面、系统的认识。本文首先介绍了氧还原反应的四电子、二电子反应路径及相关机制;其次,综述了提高碳基纳米材料二电子氧还原活性和H2O2生成选择性的结构优化策略及其活性中心的设计思路,包括非金属单原子掺杂、双原子掺杂、结构缺陷和表面修饰等。最后,展望了电催化制备H2O2及相关催化材料的发展前景和面临的挑战。

     

    Abstract: The electrocatalytic two-electron oxygen reduction reaction (2e-ORR) is an effective, safe and green method to produce hydrogen peroxide (H2O2) as an alternative to the industrial anthraquinone process. Carbon-based nanomaterials with the advantages of high electrical conductivity, good structural stability, easy control of the nanostructure and low cost, are recognized as promising catalysts for H2O2 production by 2e-ORR. A detailed overview of the research progress on these carbon-based electrocatalysts, their intrinsic active centers and reaction mechanisms is helpful to obtain a comprehensive and systematic understanding of the latest progress in this field. Fundamental aspects and mechanisms of the two-electron and four-electron pathways for the ORR are introduced, followed by a comprehensive review of strategies to modify carbon-based nanomaterials such as single, dual or multiple heteroatom doping, defect design and surface modification, in order to obtain high activity and selectivity for H2O2 synthesis. Finally, the prospects and challenges in obtaining catalysts with high rate and yield are presented, which should shed light on future scientific research and their use for H2O2 synthesis.

     

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