电催化两电子水氧化制备过氧化氢的研究进展

引用本文: 林柳, 孙泽民, 陈华添, 赵莲, 孙明月, 杨逸涛, 廖振升, 吴鑫宇, 李欣欣, 唐城. 电催化两电子水氧化制备过氧化氢的研究进展[J]. 物理化学学报, 2024, 40(4): 230501. doi: 10.3866/PKU.WHXB202305019 shu

Citation: Liu Lin, Zemin Sun, Huatian Chen, Lian Zhao, Mingyue Sun, Yitao Yang, Zhensheng Liao, Xinyu Wu, Xinxin Li, Cheng Tang. Recent Advances in Electrocatalytic Two-Electron Water Oxidation for Green H₂O₂ Production[J]. Acta Physico-Chimica Sinica, 2024, 40(4): 230501. doi: 10.3866/PKU.WHXB202305019 shu

电催化两电子水氧化制备过氧化氢的研究进展

林柳 ^1, ,
孙泽民 ^{1,
,} ,
陈华添 ^1, ,
赵莲 ^1, ,
孙明月 ^1, ,
杨逸涛 ^1, ,
廖振升 ^1, ,
吴鑫宇 ^1, ,
李欣欣 ^2, ,
唐城 ^{2,
,}

1.
北京师范大学文理学院, 先进材料研究中心, 广东珠海 519087;
2.
清华大学化学工程系, 绿色反应工程与工艺北京市重点实验室, 北京 100084

通讯作者: 孙泽民,Email:zmsun@mail.bnu.edu.cn; 唐城,Email:cheng-net0@tsinghua.edu.cn

基金项目:
广东省自然科学基金(2023A1515010554)资助项目

摘要: 过氧化氢(H₂O₂)是一种环境友好的化学氧化剂，广泛应用于水处理、医疗消毒、化学合成等工业领域。电催化两电子水氧化反应(2e⁻ WOR)是一种可以在温和条件下直接从水中生产H₂O₂的方法。然而，受限于反应机理认识和催化材料设计的不足，2e⁻ WOR的催化选择性和活性仍然较低。本文综述了近年来通过2e⁻ WOR反应路径电合成H₂O₂的研究进展，首先介绍了2e⁻ WOR的催化机理和研究方法，强调了理论计算加速高选择性、高活性和高稳定性催化剂研究的作用，并讨论了电合成H₂O₂的不同定量方法和原位表征手段；然后详细总结了高性能2e⁻ WOR电催化剂的调控策略，包括缺陷、掺杂、晶面和界面工程，同时指出了反应器创新设计的重要性；最后展望了电合成H₂O₂的研究挑战和机遇。

关键词:

English

Recent Advances in Electrocatalytic Two-Electron Water Oxidation for Green H₂O₂ Production

Liu Lin ^1, ,
Zemin Sun ^{1,
,} ,
Huatian Chen ^1, ,
Lian Zhao ^1, ,
Mingyue Sun ^1, ,
Yitao Yang ^1, ,
Zhensheng Liao ^1, ,
Xinyu Wu ^1, ,
Xinxin Li ^2, ,
Cheng Tang ^{2,
,}

1.
Center for Advanced Materials Research, College of Arts and Sciences, Beijing Normal University, Zhuhai 519087, Guangdong Province, China;
2.
Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China

Corresponding author: Zemin Sun, ; Cheng Tang,

Received Date: 09 May 2023
Accepted Date: 07 June 2023
Revised Date: 05 June 2023
Available Online: 14 June 2023
Fund Project:
The project was supported by the Natural Science Foundation of Guangdong Province, China (2023A1515010554).

Abstract: Hydrogen peroxide (H₂O₂) is an environmentally friendly oxidant that has been widely used in water treatment, medical disinfection, chemical synthesis, and other industrial applications. However, traditional methods used to produce H₂O₂ consume significant amounts of energy and generate hazardous by-products, which limit their scope. On-site and on-demand electrocatalytic two-electron water oxidation chemistry is an attractive option for directly producing H₂O₂ from water; it also avoids the hazardous anthraquinone method, has fewer transportation costs and risks, and is integratable with renewable electricity. Despite these advantages, the two-electron water oxidation reaction (2e^– WOR) still suffers from poor selectivity and activity due to a lack of mechanistic, material-design, and reactor-engineering understanding. This study summarizes recent advances in H₂O₂ electrosynthesis technology using the 2e^– WOR. The catalytic 2e^– WOR mechanism is first introduced with a focus on selectivity, activity, and stability. This reaction involves the electrocatalytic oxidation of water to produce H₂O₂, which can be further oxidized to O₂. Selectivity is influenced by a variety of factors, including the electrocatalyst, pH, and electrolyte. Various quantitative H₂O₂ methods are discussed along with in situ characterization studies into the 2e^– WOR aimed at better understanding the reaction process. Such methods include in situ Fourier-transform infrared spectroscopy and in situ Raman spectroscopy. Researchers are able to identify reaction intermediates and understand reaction mechanisms better using these techniques, thereby providing guidance for the design of more efficient electrocatalysts. In turn, various strategies for preparing high-performance electrocatalysts are summarized, including defect, doping, facet, and interfacial engineering methods. Mechanism-guided multiscale materials engineering can improve the activities and selectivities of electrocatalysts, thereby increasing H₂O₂ yields. In addition, device-level engineering, especially in relation to reactor and system innovations, is emphasized, which is important for improving reaction efficiency and reducing the cost of the 2e^– WOR. Finally, current challenges and future opportunities in the 2e^– WOR H₂O₂ electrosynthesis field are discussed. More effort directed at improving reaction selectivity, activity, and durability is required, along with exploring suitable application scenarios. The 2e^– WOR is expected to become a more sustainable and efficient method for producing H₂O₂ facilitated by continuing progress in the materials science and electrochemical technology fields.

Key words:

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通讯作者: 孙泽民,Email:zmsun@mail.bnu.edu.cn; 唐城,Email:cheng-net0@tsinghua.edu.cn

English

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通讯作者: 陈斌, bchen63@163.com

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电催化两电子水氧化制备过氧化氢的研究进展

通讯作者: 孙泽民,Email:zmsun@mail.bnu.edu.cn; 唐城,Email:cheng-net0@tsinghua.edu.cn

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