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Electrochemical oxygen reduction to hydrogen peroxide at practical rates in strong acidic media

Author

Listed:
  • Xiao Zhang

    (Rice University)

  • Xunhua Zhao

    (The University of Texas at Austin)

  • Peng Zhu

    (Rice University)

  • Zachary Adler

    (Rice University)

  • Zhen-Yu Wu

    (Rice University)

  • Yuanyue Liu

    (The University of Texas at Austin)

  • Haotian Wang

    (Rice University
    Rice University
    Rice University)

Abstract

Electrochemical oxygen reduction to hydrogen peroxide (H2O2) in acidic media, especially in proton exchange membrane (PEM) electrode assembly reactors, suffers from low selectivity and the lack of low-cost catalysts. Here we present a cation-regulated interfacial engineering approach to promote the H2O2 selectivity (over 80%) under industrial-relevant generation rates (over 400 mA cm−2) in strong acidic media using just carbon black catalyst and a small number of alkali metal cations, representing a 25-fold improvement compared to that without cation additives. Our density functional theory simulation suggests a “shielding effect” of alkali metal cations which squeeze away the catalyst/electrolyte interfacial protons and thus prevent further reduction of generated H2O2 to water. A double-PEM solid electrolyte reactor was further developed to realize a continuous, selective (∼90%) and stable (over 500 hours) generation of H2O2 via implementing this cation effect for practical applications.

Suggested Citation

  • Xiao Zhang & Xunhua Zhao & Peng Zhu & Zachary Adler & Zhen-Yu Wu & Yuanyue Liu & Haotian Wang, 2022. "Electrochemical oxygen reduction to hydrogen peroxide at practical rates in strong acidic media," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30337-0
    DOI: 10.1038/s41467-022-30337-0
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    References listed on IDEAS

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    1. Gao-Feng Han & Feng Li & Wei Zou & Mohammadreza Karamad & Jong-Pil Jeon & Seong-Wook Kim & Seok-Jin Kim & Yunfei Bu & Zhengping Fu & Yalin Lu & Samira Siahrostami & Jong-Beom Baek, 2020. "Building and identifying highly active oxygenated groups in carbon materials for oxygen reduction to H2O2," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    2. Kun Jiang & Seoin Back & Austin J. Akey & Chuan Xia & Yongfeng Hu & Wentao Liang & Diane Schaak & Eli Stavitski & Jens K. Nørskov & Samira Siahrostami & Haotian Wang, 2019. "Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
    3. Hui Li & Peng Wen & Dominique S. Itanze & Zachary D. Hood & Shiba Adhikari & Chang Lu & Xiao Ma & Chaochao Dun & Lin Jiang & David L. Carroll & Yejun Qiu & Scott M. Geyer, 2020. "Scalable neutral H2O2 electrosynthesis by platinum diphosphide nanocrystals by regulating oxygen reduction reaction pathways," Nature Communications, Nature, vol. 11(1), pages 1-12, December.
    4. Chuan Xia & Peng Zhu & Qiu Jiang & Ying Pan & Wentao Liang & Eli Stavitski & Husam N. Alshareef & Haotian Wang, 2019. "Continuous production of pure liquid fuel solutions via electrocatalytic CO2 reduction using solid-electrolyte devices," Nature Energy, Nature, vol. 4(9), pages 776-785, September.
    5. Qingran Zhang & Xin Tan & Nicholas M. Bedford & Zhaojun Han & Lars Thomsen & Sean Smith & Rose Amal & Xunyu Lu, 2020. "Direct insights into the role of epoxy groups on cobalt sites for acidic H2O2 production," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    6. 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.
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    Cited by:

    1. 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.
    2. Jiannan Du & Guokang Han & Wei Zhang & Lingfeng Li & Yuqi Yan & Yaoxuan Shi & Xue Zhang & Lin Geng & Zhijiang Wang & Yueping Xiong & Geping Yin & Chunyu Du, 2023. "CoIn dual-atom catalyst for hydrogen peroxide production via oxygen reduction reaction in acid," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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