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CO2/carbonate-mediated electrochemical water oxidation to hydrogen peroxide

Author

Listed:
  • Lei Fan

    (Rice University
    College of Chemical and Biological Engineering, Zhejiang University)

  • Xiaowan Bai

    (The University of Texas at Austin)

  • Chuan Xia

    (Rice University
    Rice University)

  • Xiao Zhang

    (Rice University)

  • Xunhua Zhao

    (The University of Texas at Austin)

  • Yang Xia

    (Rice University)

  • Zhen-Yu Wu

    (Rice University)

  • Yingying Lu

    (College of Chemical and Biological Engineering, Zhejiang University)

  • Yuanyue Liu

    (The University of Texas at Austin)

  • Haotian Wang

    (Rice University
    Rice University
    Rice University)

Abstract

Electrochemical water oxidation reaction (WOR) to hydrogen peroxide (H2O2) via a 2e− pathway provides a sustainable H2O2 synthetic route, but is challenged by the traditional 4e− counterpart of oxygen evolution. Here we report a CO2/carbonate mediation approach to steering the WOR pathway from 4e− to 2e−. Using fluorine-doped tin oxide electrode in carbonate solutions, we achieved high H2O2 selectivity of up to 87%, and delivered unprecedented H2O2 partial currents of up to 1.3 A cm−2, which represents orders of magnitude improvement compared to literature. Molecular dynamics simulations, coupled with electron paramagnetic resonance and isotope labeling experiments, suggested that carbonate mediates the WOR pathway to H2O2 through the formation of carbonate radical and percarbonate intermediates. The high selectivity, industrial-relevant activity, and good durability open up practical opportunities for delocalized H2O2 production.

Suggested Citation

  • Lei Fan & Xiaowan Bai & Chuan Xia & Xiao Zhang & Xunhua Zhao & Yang Xia & Zhen-Yu Wu & Yingying Lu & Yuanyue Liu & Haotian Wang, 2022. "CO2/carbonate-mediated electrochemical water oxidation to hydrogen peroxide," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30251-5
    DOI: 10.1038/s41467-022-30251-5
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    References listed on IDEAS

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    1. Xinjian Shi & Samira Siahrostami & Guo-Ling Li & Yirui Zhang & Pongkarn Chakthranont & Felix Studt & Thomas F. Jaramillo & Xiaolin Zheng & Jens K. Nørskov, 2017. "Understanding activity trends in electrochemical water oxidation to form hydrogen peroxide," Nature Communications, Nature, vol. 8(1), pages 1-6, December.
    2. Artavazd Badalyan & Shannon S. Stahl, 2016. "Cooperative electrocatalytic alcohol oxidation with electron-proton-transfer mediators," Nature, Nature, vol. 535(7612), pages 406-410, July.
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    Cited by:

    1. Heng Zhu & Ximei Lv & Yuexu Wu & Wentao Wang & Yuping Wu & Shicheng Yan & Yuhui Chen, 2024. "Carbonate-carbonate coupling on platinum surface promotes electrochemical water oxidation to hydrogen peroxide," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Peike Cao & Xie Quan & Xiaowa Nie & Kun Zhao & Yanming Liu & Shuo Chen & Hongtao Yu & Jingguang G. Chen, 2023. "Metal single-site catalyst design for electrocatalytic production of hydrogen peroxide at industrial-relevant currents," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    3. Cong Liu & Bingbao Mei & Zhaoping Shi & Zheng Jiang & Junjie Ge & Wei Xing & Ping Song & Weilin Xu, 2024. "Operando formation of highly efficient electrocatalysts induced by heteroatom leaching," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    4. Jihyun Baek & Qiu Jin & Nathan Scott Johnson & Yue Jiang & Rui Ning & Apurva Mehta & Samira Siahrostami & Xiaolin Zheng, 2022. "Discovery of LaAlO3 as an efficient catalyst for two-electron water electrolysis towards hydrogen peroxide," Nature Communications, Nature, vol. 13(1), pages 1-10, December.

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