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Carbonate-carbonate coupling on platinum surface promotes electrochemical water oxidation to hydrogen peroxide

Author

Listed:
  • Heng Zhu

    (Nanjing Tech University
    Nanjing Tech University)

  • Ximei Lv

    (Nanjing Tech University)

  • Yuexu Wu

    (Nanjing Tech University)

  • Wentao Wang

    (Nanjing Tech University)

  • Yuping Wu

    (Southeast University)

  • Shicheng Yan

    (Nanjing University)

  • Yuhui Chen

    (Nanjing Tech University)

Abstract

Water electro-oxidation to form H2O2 is an important way to produce H2O2 which is widely applied in industry. However, its mechanism is under debate and HO(ads), hydroxyl group adsorbed onto the surface of the electrode, is regarded as an important intermediate. Herein, we study the mechanism of water oxidation to H2O2 at Pt electrode using in-situ Raman spectroscopy and differential electrochemical mass spectroscopy and find peroxide bond mainly originated from the coupling of two CO32- via a C2O62- intermediate. By quantifying the 18O isotope in the product, we find that 93% of H2O2 was formed via the CO32- coupling route and 7% of H2O2 is from OH(ads)-CO3•− route. The OH(ads)-OH(ads) coupling route has a negligible contribution. The comparison of various electrodes shows that the strong adsorption of CO3(ads) at the electrode surface is essential. Combining with a commercial cathode catalyst to produce H2O2 during oxygen reduction, we assemble a flow cell in which the cathode and anode simultaneously produce H2O2. It shows a Faradaic efficiency of 150% of H2O2 at 1 A cm−2 with a cell voltage of 2.3 V.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-53134-3
    DOI: 10.1038/s41467-024-53134-3
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    References listed on IDEAS

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    1. Yi-Fan Huang & Patricia J. Kooyman & Marc T. M. Koper, 2016. "Intermediate stages of electrochemical oxidation of single-crystalline platinum revealed by in situ Raman spectroscopy," Nature Communications, Nature, vol. 7(1), pages 1-7, November.
    2. Changmin Kim & Sung O Park & Sang Kyu Kwak & Zhenhai Xia & Guntae Kim & Liming Dai, 2023. "Concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    3. Ma, Jia & Choudhury, Nurul A. & Sahai, Yogeshwar, 2010. "A comprehensive review of direct borohydride fuel cells," Renewable and Sustainable Energy Reviews, Elsevier, vol. 14(1), pages 183-199, January.
    4. Lejing Li & Zhuofeng Hu & Yongqiang Kang & Shiyu Cao & Liangpang Xu & Luo Yu & Lizhi Zhang & Jimmy C. Yu, 2023. "Electrochemical generation of hydrogen peroxide from a zinc gallium oxide anode with dual active sites," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    5. 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.
    6. 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.
    7. Deqing Cao & Chuan Tan & Yuhui Chen, 2022. "Oxidative decomposition mechanisms of lithium carbonate on carbon substrates in lithium battery chemistries," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    8. Sadiq, Muhammad & Alshehhi, Reem J. & Urs, Rahul Rajeevkumar & Mayyas, Ahmad T., 2023. "Techno-economic analysis of Green-H2@Scale production," Renewable Energy, Elsevier, vol. 219(P1).
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