物理化学学报

所属专题: 多物理场能源催化转化

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电化学二电子氧还原制备过氧化氢研究进展

文兆宇1, 韩娜1, 李彦光1,2   

  1. 1 苏州大学功能纳米与软物质研究院, 江苏苏州 215123;
    2 澳门科技大学材料科学与工程研究院, 澳门氹仔岛 999078
  • 收稿日期:2023-04-03 修回日期:2023-05-16 录用日期:2023-05-17 发布日期:2023-05-29
  • 通讯作者: 韩娜, 李彦光 E-mail:hanna@suda.edu.cn;yanguang@suda.edu.cn
  • 基金资助:
    国家自然科学基金(U2002213,52161160331,2227090515)资助项目

Recent Progress towards the Production of H2O2 by Electrochemical Two-Electron Oxygen Reduction Reaction

Zhaoyu Wen1, Na Han1, Yanguang Li1,2   

  1. 1 Institute of Functional Nano&Soft Materials(FUNSOM), Soochow University, Suzhou 215123, Jiangsu Province, China;
    2 Macao Institute of Materials Science and Engineering, Macau University of Science and Technology, Taipa 999078, Macau SAR, China
  • Received:2023-04-03 Revised:2023-05-16 Accepted:2023-05-17 Published:2023-05-29
  • Contact: Na Han, Yanguang Li E-mail:hanna@suda.edu.cn;yanguang@suda.edu.cn
  • Supported by:
    The project was supported by the National Natural Science Foundation of China (U2002213, 52161160331, 2227090515).

摘要: 利用电化学二电子氧还原(2e Oxygen Reduction Reaction,2e ORR)方法实现过氧化氢(H2O2)的分散式制备,被认为是具有广阔发展前景的技术之一。为实现高的氧还原活性和理想的H2O2选择性,设计高性能2eORR电催化剂是该技术的核心关键。尽管现阶段发展的2e ORR催化剂已经取得了显著进展,但距离规模化应用仍存在很大的差距。基于此,本文综述了电化学二电子氧还原制备H2O2的最新研究进展,首先简要介绍了反应机理和评价方法,并根据机理分析了影响电催化性能的关键因素。随后围绕贵金属催化剂、碳基催化剂、单原子及分子催化剂的最新研究进展,阐述了提升催化剂活性与H2O2选择性的主要策略。最后,针对电化学二电子氧还原制备H2O2体系面临的关键问题和挑战,对该领域未来的发展趋势进行了展望。

关键词: 电化学, 二电子氧还原反应, 过氧化氢, 催化剂, 选择性

Abstract: Hydrogen peroxide (H2O2) is an important chemical and has been extensively used in various industrial and manufacturing applications, such as wastewater treatment, sterilization, energy storage, and oxidation of small molecules. With increasing demand in various fields, the global hydrogen peroxide market is expected to grow to $8.9 billion by 2031. Currently, over 90% of H2O2 is industrially synthesized by the anthraquinone process, which requires complex infrastructure and expensive catalysts. Additionally, the anthraquinone process is energy intensive and leads to increased levels of environmental pollution. Although the direct synthetic process, which involves mixing hydrogen and oxygen, can achieve high atomic utilization, its development is limited due to explosion risk and high cost. Thus, there is a pressing need for a safe, cost-effective, and efficient industrial method for the production of H2O2. The electrochemical synthesis of H2O2 via a two-electron oxygen reduction reaction (2e ORR) has emerged as an attractive method for the decentralized production of H2O2, which could effectively address the issues associated with the indirect anthraquinone and direct synthetic processes. However, sluggish reaction kinetics and poor selectivity decrease the energy efficiency of electrochemical H2O2 synthesis. In this regard, developing electrocatalysts with high 2e ORR selectivity is vital for the efficient production of H2O2. In the past decades, extensive efforts have been devoted to developing effective 2e ORR electrocatalysts such as noble metals/alloys, carbon-based materials, single-atom catalysts, and molecular complexes. However, the reported catalysts still have unsatisfactory catalytic performances. Therefore, there is still a long way to realize the large−scale production of H2O2 via electrochemical 2e ORR pathway. In this perspective, we systematically summarize recent developments regarding the direct production of H2O2 through electrochemical two-electron oxygen reaction. First, the fundamental aspects of electrochemical 2e ORR are discussed, including their reaction mechanisms, possible reaction pathways, testing techniques and performance figures of merit. This introduction is followed by detailed discussions on the different types of 2e ORR electrocatalysts, with an emphasis on the underlying material design principles used to promote reaction activity, selectivity, and stability. Subsequently, the applications of electrosynthetic hydrogen peroxide in various fields are briefly described, including pollutant degradation, water sterilization, energy storage, and small-molecule synthesis. Finally, potential future directions and prospects in 2e ORR catalysts for electrochemically producing H2O2 are examined.

Key words: Electrochemical, 2e oxygen reduction reaction, Hydrogen peroxide, Catalyst, Selectivity