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Electro-assisted methane oxidation to formic acid via in-situ cathodically generated H2O2 under ambient conditions

Author

Listed:
  • Jiwon Kim

    (Yonsei University
    Korea Institute of Science and Technology)

  • Jae Hyung Kim

    (Korea Institute of Energy Research)

  • Cheoulwoo Oh

    (Yonsei University
    Korea Institute of Science and Technology)

  • Hyewon Yun

    (Seoul National University
    Institute for Basic Science (IBS))

  • Eunchong Lee

    (Seoul National University)

  • Hyung-Suk Oh

    (Korea Institute of Science and Technology
    Sungkyunkwan University (SKKU))

  • Jong Hyeok Park

    (Yonsei University)

  • Yun Jeong Hwang

    (Seoul National University
    Institute for Basic Science (IBS))

Abstract

Direct partial oxidation of methane to liquid oxygenates has been regarded as a potential route to valorize methane. However, CH4 activation usually requires a high temperature and pressure, which lowers the feasibility of the reaction. Here, we propose an electro-assisted approach for the partial oxidation of methane, using in-situ cathodically generated reactive oxygen species, at ambient temperature and pressure. Upon using acid-treated carbon as the electrocatalyst, the electro-assisted system enables the partial oxidation of methane in an acidic electrolyte to produce oxygenated liquid products. We also demonstrate a high production rate of oxygenates (18.9 μmol h−1) with selective HCOOH production. Mechanistic analysis reveals that reactive oxygen species such as ∙OH and ∙OOH radicals are produced and activate CH4 and CH3OH. In addition, unstable CH3OOH generated from methane partial oxidation can be additionally reduced to CH3OH on the cathode, and so-produced CH3OH is further oxidized to HCOOH, allowing selective methane partial oxidation.

Suggested Citation

  • Jiwon Kim & Jae Hyung Kim & Cheoulwoo Oh & Hyewon Yun & Eunchong Lee & Hyung-Suk Oh & Jong Hyeok Park & Yun Jeong Hwang, 2023. "Electro-assisted methane oxidation to formic acid via in-situ cathodically generated H2O2 under ambient conditions," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-40415-6
    DOI: 10.1038/s41467-023-40415-6
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    References listed on IDEAS

    as
    1. Yingying Fan & Wencai Zhou & Xueying Qiu & Hongdong Li & Yuheng Jiang & Zhonghui Sun & Dongxue Han & Li Niu & Zhiyong Tang, 2021. "Selective photocatalytic oxidation of methane by quantum-sized bismuth vanadate," Nature Sustainability, Nature, vol. 4(6), pages 509-515, June.
    2. Pengfei Xie & Jing Ding & Zihao Yao & Tiancheng Pu & Peng Zhang & Zhennan Huang & Canhui Wang & Junlei Zhang & Noah Zecher-Freeman & Han Zong & Dashui Yuan & Shengwei Deng & Reza Shahbazian-Yassar & C, 2022. "Oxo dicopper anchored on carbon nitride for selective oxidation of methane," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    3. Laihao Luo & Jie Luo & Hongliang Li & Fangning Ren & Yifei Zhang & Andong Liu & Wei-Xue Li & Jie Zeng, 2021. "Water enables mild oxidation of methane to methanol on gold single-atom catalysts," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    4. Shuxing Bai & Fangfang Liu & Bolong Huang & Fan Li & Haiping Lin & Tong Wu & Mingzi Sun & Jianbo Wu & Qi Shao & Yong Xu & Xiaoqing Huang, 2020. "High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    5. Lei Luo & Lei Fu & Huifen Liu & Youxun Xu & Jialiang Xing & Chun-Ran Chang & Dong-Yuan Yang & Junwang Tang, 2022. "Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
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