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Carbon electrodes for the electrocatalytic synthesis of hydrogen peroxide: A review

HUANG Xian-huai YANG Xin-ke GUI Ling LIU Shao-gen WANG Kun RONG Hong-wei WEI Wei

黄显怀, 杨鑫科, 桂玲, 刘绍根, 王坤, 荣宏伟, 韦伟. 用于电催化合成过氧化氢的碳电极综述. 新型炭材料(中英文), 2024, 39(2): 254-270. doi: 10.1016/S1872-5805(24)60846-2
引用本文: 黄显怀, 杨鑫科, 桂玲, 刘绍根, 王坤, 荣宏伟, 韦伟. 用于电催化合成过氧化氢的碳电极综述. 新型炭材料(中英文), 2024, 39(2): 254-270. doi: 10.1016/S1872-5805(24)60846-2
HUANG Xian-huai, YANG Xin-ke, GUI Ling, LIU Shao-gen, WANG Kun, RONG Hong-wei, WEI Wei. Carbon electrodes for the electrocatalytic synthesis of hydrogen peroxide: A review. New Carbon Mater., 2024, 39(2): 254-270. doi: 10.1016/S1872-5805(24)60846-2
Citation: HUANG Xian-huai, YANG Xin-ke, GUI Ling, LIU Shao-gen, WANG Kun, RONG Hong-wei, WEI Wei. Carbon electrodes for the electrocatalytic synthesis of hydrogen peroxide: A review. New Carbon Mater., 2024, 39(2): 254-270. doi: 10.1016/S1872-5805(24)60846-2

用于电催化合成过氧化氢的碳电极综述

doi: 10.1016/S1872-5805(24)60846-2
基金项目: 国家自然科学基金(52370001);安徽省重点研发开发项目(2023T07020011);珠江三角洲水质安全与保护教育部重点实验室开放基金资助项目(KLWQCPRD-202306);安徽省科技重大专项(202203a07020019)
详细信息
    通讯作者:

    韦 伟,博士,讲师. E-mail:weiw@ahjzu.edu.cn

  • 中图分类号: TQ127.1+1

Carbon electrodes for the electrocatalytic synthesis of hydrogen peroxide: A review

Funds: This work was funded by the National Natural Science Foundation of China (52370001), the Anhui Provincial Key Research and Development Project (2023t07020011), the Opening Fund of Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education (KLWQCPRD-202306), and the Science and Technology Major Project of Anhui Province (202203a07020019)
More Information
  • 摘要: 通过双电子(2e)途径的电催化氧还原方式能够即时合成过氧化氢(H2O2),远超传统的蒽醌工艺。近年来,碳电极因具有良好的催化效果和优越的稳定性在电催化合成H2O2方面受到越来越多的关注。本综述结合材料改性与润湿性调整,从三相界面的角度考虑与H2O2合成速率及使用寿命的关系。介绍了碳电极的结构与电催化合成H2O2的原理,包括单质炭材料、无金属催化剂、贵金属催化剂与非贵金属催化剂4种主流催化剂;金属阳极与电解液对于三相界面的影响;碳电极润湿性与三相界面的关系,指出侧重于提高2e途径选择性的改性方式也会对电极润湿性造成影响。此外,合理地设计电器原件与提升碳电极合成H2O2功效的关系。最后,讨论了当前碳电极电催化合成H2O2所面临的问题与未来的研究方向。
  • FIG. 3061.  FIG. 3061.

    FIG. 3061..  FIG. 3061.

    Figure  1.  Schematic structure of the carbon electrode in the electrochemical synthesis of hydrogen peroxide[15]. Reprinted with permission from Elsevier

    Figure  2.  ORR mechanism of oxygen at the air cathode surface in an acidic medium (ORR mechanism at the air cathode surface under alkaline conditions is shown in parentheses)[16]. Reprinted with permission from Elsevier

    Figure  3.  Volcano plot of oxygen reduction activity of different metals as a function of oxygen binding energy(ΔEO)[43]. Reprinted with permission from Elsevier

    Figure  4.  Concept for developing electrocatalysts with appropriate density of active sites: schematic representation of the different parameters controlling the catalytic performance of two-electron ORR catalysts[88]. Reprinted with permission from Elsevier

    Figure  5.  (a) Membrane-free electrolyser[115]. Reprinted with permission from The Royal Society of Chemistry. (b) Conventional polymer electrolyser[116]. Reprinted with permission from American Chemical Society. (c) Double-layer polymer electrolyser[117]. Reprinted with permission from The American Association for the Advancement of Science. (d) Phase transfer device[119]. Reprinted with permission from Elsevier

    Table  1.   Effect of catalyst engineering on the synthesis of H2O2 from carbon electrodes

    TechniqueSubtrateElectrolytes/pHWettabilityH2O2 yieldSelectivenessDurabilityRef.
    Monolithic carbon
    material
    1000 °C
    1% O2
    Porous carbon0.5 mol·L−1 Na2SO489.9°→0°7.9→24.9 mg·L−1/20 h[61]
    600 °C calcination in airCarbon black0.1 mol·L−1 Na2SO4100°→79°65.3→517.7 mg·L−147.1%→56.1%/[62]
    Coated by electrochemically exfoliated grapheneCarbon cloth0.05 mol·L−1 K2SO4138.4°→73.2°251.4→450.8 mg·L−1//[63]
    Metal-free
    carbon-based catalysts
    Heteroatom dopingP-CNTs0.1 mol·L−1 Na2SO4/419.5–1291.3 mg·L−1·h−188.5%/[64]
    N-Graphite
    (N 60.7%)
    0.1 mol·L−1 KOH/1286.9 mmol·g−1·h−1~75%/[52]
    N-CMK3-IL0.1 mol·L−1 KOH//86%/[65]
    F-mrGO0.1 mol·L−1 KOH/430.8 mmol·g−1·h−1~100%/[66]
    Introducing oxygen-containing functional groupsCarbon black0.1 mol·L−1 Na2SO457°→45°83→120 mg·L−150% increase[67]
    O-CNTs0.1 mol·L−1 KOH~3950 mg·L−1·h−1~90%[68]
    rGO-KOH0.1 mol·L−1 KOH/~100%[69]
    Precious metal
    catalysts
    Pt-Hg0.1 mol·L−1 HClO4//~90%[70]
    Au-Pd0.1 mol·L−1 HClO4//~95%[71]
    Au-Pd-Ni0.1 mol·L−1 KOH/0.0591 mmol·g−1·h−1/[72]
    h-Pt1-CuSx0.1 mol·L−1 HClO4/~546 mmo·g−1·h−192%–96%/[73]
    Non-precious
    metal catalysts
    Co-N-C0.1 mol·L−1 HClO4/80–275 mmol·g−1·h−1~90%/[74]
    Ni-N2O2/C0.1 mol·L−1 KOH/5.9 mmol·g−1·h−196%/[75]
    Ni-O-C0.1 mol·L−1 KOH/59.3 mg·L−182%200 h[76]
    Co1-NG(O)0.1 mol·L−1 KOH/~418 mmol·g−1·h−190%/[58]
    下载: 导出CSV

    Table  2.   Improvement of H2O2 production by wettability modification of carbon electrode

    ObjectiveTechniqueSubstrateDetailWetting angleH2O2 yieldRef.
    Hydrophilic improvementFunctionalizationPorous carbonFabricate honeycomb carbon
    nanofibers with abundent OFGs
    37.7°→ 0°6 mmol L−1[106]
    Physical
    method
    Graphite sheetAlternating current glow discharge/35 → 119 µmol L−1[63]
    Chemical modificationGraphite feltH2SO4, NaNO3, KMnO4 solution treatment followed by 900 °C NH3 activation120.3° → 61.5°277 → 479 mg·L−1[107]
    Graphite felt0.5 mol L−1 NaOH treatment followed by NaOH activated at 400 °C127.3° → 0°50 → 100 mg·L−1[108]
    Electrochemical techniquesGraphite felt0–2 V (vs SCE) cyclical polarization/85 → 235 mg·L−1[109]
    Reticulated vitreous carbon0–2 V (vs. Ag/AgCl) cyclical/18 → 64 mg·L−1[110]
    Hydrophobic improvementUsing hydrophobic auxiliary materials or treatmentsGraphite feltLoaded with NPC carbonized by ZIF-8 nanocrystals as precursor112.0° → 125.0°11 → 113 mg·L−1[111]
    CB + graphite + PTFEDecrease PTFE content in CL107.1° → 141.1°2131 → 3005 mg·L−1[112]
    Graphite feltModified by CB + PTFE followed by 360 °C calcination68.4° → 141.0°25 →
    31 mg·cm−2 h−1
    [93]
    Constructing amphiphilic interfaceConstrcting hydrophobic GSL and hydrophilic CLGraphite feltCB + PVDF facilitate hydrophilic; PTFE + 350 °C calcination facilitate hydrophobicCL: 81.2° → 74.4°
    GSL: 81.2° → 137.7°
    3 → 62 mg·L−1[113]
    Fabricating Janus electrodeGraphite feltPTFE immersion to realize Hydrophobic; galvanostatic anodization to realize hydrophilicCA increased after hydrophobic treatment and decreased after hydrophilic treatment7 → 50 mg·L−1[114]
    下载: 导出CSV
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  • 收稿日期:  2023-11-10
  • 录用日期:  2024-02-27
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  • 网络出版日期:  2024-02-28
  • 刊出日期:  2024-04-20

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