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Concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide

Author

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  • Changmin Kim

    (University of New South Wales)

  • Sung O Park

    (Ulsan National Institute of Science and Technology (UNIST))

  • Sang Kyu Kwak

    (Ulsan National Institute of Science and Technology (UNIST)
    Korea University)

  • Zhenhai Xia

    (University of New South Wales)

  • Guntae Kim

    (Chinese Academy of Sciences)

  • Liming Dai

    (University of New South Wales)

Abstract

Electrosynthesis of hydrogen peroxide via selective two-electron transfer oxygen reduction or water oxidation reactions offers a cleaner, cost-effective alternative to anthraquinone processes. However, it remains a challenge to achieve high Faradaic efficiencies at elevated current densities. Herein, we report that oxygen-deficient Pr1.0Sr1.0Fe0.75Zn0.25O4-δ perovskite oxides rich of oxygen vacancies can favorably bind the reaction intermediates to facilitate selective and efficient two-electron transfer pathways. These oxides exhibited superior Faradic efficiencies (~99%) for oxygen reduction over a wide potential range (0.05 to 0.45 V versus reversible hydrogen electrode) and current densities surpassing 50 mA cm−2 under high ionic strengths. We further found that the oxides perform a high selectivity (~80%) for two-electron transfer water oxidation reaction at a low overpotential (0.39 V). Lastly, we devised a membrane-free electrolyser employing bifunctional electrocatalysts, achieving a record-high Faradaic efficiency of 163.0% at 2.10 V and 50 mA cm−2. This marks the first report of the concurrent oxygen reduction and water oxidation catalysed by efficient bifunctional oxides in a novel membrane-free electrolyser for scalable hydrogen peroxide electrosynthesis.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-41397-1
    DOI: 10.1038/s41467-023-41397-1
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    References listed on IDEAS

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    1. Qiaowan Chang & Pu Zhang & Amir Hassan Bagherzadeh Mostaghimi & Xueru Zhao & Steven R. Denny & Ji Hoon Lee & Hongpeng Gao & Ying Zhang & Huolin L. Xin & Samira Siahrostami & Jingguang G. Chen & Zheng , 2020. "Promoting H2O2 production via 2-electron oxygen reduction by coordinating partially oxidized Pd with defect carbon," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    2. Chang Hyuck Choi & Minho Kim & Han Chang Kwon & Sung June Cho & Seongho Yun & Hee-Tak Kim & Karl J. J. Mayrhofer & Hyungjun Kim & Minkee Choi, 2016. "Tuning selectivity of electrochemical reactions by atomically dispersed platinum catalyst," Nature Communications, Nature, vol. 7(1), pages 1-9, April.
    3. 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.
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    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. Hongni Chen & Chao Wang & Han Wu & Lili Li & Yali Xing & Chuanhui Zhang & Xiaojing Long, 2024. "Host-guest-induced electronic state triggers two-electron oxygen reduction electrocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-14, December.

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