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Proton-coupled electron transfer controls peroxide activation initiated by a solid-water interface

Author

Listed:
  • Jian-Hua Chen

    (Southwest University)

  • Wan-Ting Li

    (Southwest University
    Yibin Academy of Southwest University)

  • Kun-Yu Cai

    (Southwest University)

  • Hui-Jie Tu

    (Southwest University
    Yibin Academy of Southwest University)

  • Zi-Tong Long

    (Southwest University)

  • Shoaib Akhtar

    (Southwest University)

  • Lin-Dong Liu

    (Southwest University
    Yibin Academy of Southwest University)

Abstract

Decentralized water treatment technologies, designed to align with the specific characteristics of the water source and the requirements of the user, are gaining prominence due to their cost and energy-saving advantages over traditional centralized systems. The application of chemical water treatment via heterogeneous advanced oxidation processes using peroxide (O–O) represents a potentially attractive treatment option. These processes serve to initiate redox processes at the solid-water interface. Nevertheless, the oxidation mechanism exemplified by the typical Fenton-like persulfate-based heterogeneous oxidation, in which electron transfer dominates, is almost universally accepted. Here, we present experimental results that challenge this view. At the solid-liquid interface, it is demonstrated that protons are thermodynamically coupled to electrons. In situ quantitative titration provides direct experimental evidence that the coupling ratio of protons to transferred electrons is almost 1:1. Comprehensive thermodynamic analyses further demonstrate that a net proton-coupled electron transfer occurs, with both protons and electrons entering the redox cycle. These findings will inform future developments in O–O activation technologies, enabling more efficient redox activity via the tight coupling of protons and electrons.

Suggested Citation

  • Jian-Hua Chen & Wan-Ting Li & Kun-Yu Cai & Hui-Jie Tu & Zi-Tong Long & Shoaib Akhtar & Lin-Dong Liu, 2025. "Proton-coupled electron transfer controls peroxide activation initiated by a solid-water interface," Nature Communications, Nature, vol. 16(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-58917-w
    DOI: 10.1038/s41467-025-58917-w
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    1. Ying-Jie Zhang & Gui-Xiang Huang & Lea R. Winter & Jie-Jie Chen & Lili Tian & Shu-Chuan Mei & Ze Zhang & Fei Chen & Zhi-Yan Guo & Rong Ji & Ye-Zi You & Wen-Wei Li & Xian-Wei Liu & Han-Qing Yu & Menach, 2022. "Simultaneous nanocatalytic surface activation of pollutants and oxidants for highly efficient water decontamination," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    2. Meagan S. Mauter & Ines Zucker & François Perreault & Jay R. Werber & Jae-Hong Kim & Menachem Elimelech, 2018. "The role of nanotechnology in tackling global water challenges," Nature Sustainability, Nature, vol. 1(4), pages 166-175, April.
    3. Ziwei Yu & Xuming Jin & Yang Guo & Qian Liu & Wenyu Xiang & Shuai Zhou & Jiaying Wang & Dailin Yang & Hao Bin Wu & Juan Wang, 2024. "Decoupled oxidation process enabled by atomically dispersed copper electrodes for in-situ chemical water treatment," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    4. Xiang Gao & Zhichao Yang & Wen Zhang & Bingcai Pan, 2024. "Carbon redirection via tunable Fenton-like reactions under nanoconfinement toward sustainable water treatment," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    5. Dongpeng Zhang & Yanxiao Li & Pengfei Wang & Jinyong Qu & Yi Li & Sihui Zhan, 2023. "Dynamic active-site induced by host-guest interactions boost the Fenton-like reaction for organic wastewater treatment," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    6. Hong-Zhi Liu & Xiao-Xuan Shu & Mingjie Huang & Bing-Bing Wu & Jie-Jie Chen & Xi-Sheng Wang & Hui-Lin Li & Han-Qing Yu, 2024. "Tailoring d-band center of high-valent metal-oxo species for pollutant removal via complete polymerization," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
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