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Insights into the activity of nickel boride/nickel heterostructures for efficient methanol electrooxidation

Author

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  • Yanbin Qi

    (East China University of Science and Technology
    East China University of Science and Technology)

  • Yue Zhang

    (Anhui University)

  • Li Yang

    (Anhui University)

  • Yuhan Zhao

    (East China University of Science and Technology)

  • Yihua Zhu

    (East China University of Science and Technology)

  • Hongliang Jiang

    (East China University of Science and Technology)

  • Chunzhong Li

    (East China University of Science and Technology
    East China University of Science and Technology)

Abstract

Designing efficient catalysts and understanding the underlying mechanisms for anodic nucleophile electrooxidation are central to the advancement of electrochemically-driven technologies. Here, a heterostructure of nickel boride/nickel catalyst is developed to enable methanol electrooxidation into formate with a Faradaic efficiency of nearly 100%. Operando electrochemical impedance spectroscopy and in situ Raman spectroscopy are applied to understand the influence of methanol concentration in the methanol oxidation reaction. High concentrations of methanol inhibit the phase transition of the electrocatalyst to high-valent electro-oxidation products, and electrophilic oxygen species (O* or OH*) formed on the electrocatalyst are considered to be the catalytically active species. Additional mechanistic investigation with density functional theory calculations reveals that the potential-determining step, the formation of *CH2O, occurs most favorably on the nickel boride/nickel heterostructure rather than on nickel boride and nickel. These results are highly instructive for the study of other nucleophile-based approaches to electrooxidation reactions and organic electrosynthesis.

Suggested Citation

  • Yanbin Qi & Yue Zhang & Li Yang & Yuhan Zhao & Yihua Zhu & Hongliang Jiang & Chunzhong Li, 2022. "Insights into the activity of nickel boride/nickel heterostructures for efficient methanol electrooxidation," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-32443-5
    DOI: 10.1038/s41467-022-32443-5
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    Cited by:

    1. Sixie Zhang & Yunan Wang & Shuyu Li & Zhongfeng Wang & Haocheng Chen & Li Yi & Xu Chen & Qihao Yang & Wenwen Xu & Aiying Wang & Zhiyi Lu, 2023. "Concerning the stability of seawater electrolysis: a corrosion mechanism study of halide on Ni-based anode," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Jun Qi & Yadong Du & Qi Yang & Na Jiang & Jiachun Li & Yi Ma & Yangjun Ma & Xin Zhao & Jieshan Qiu, 2023. "Energy-saving and product-oriented hydrogen peroxide electrosynthesis enabled by electrochemistry pairing and product engineering," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    3. Zheng-Jie Chen & Jiuyi Dong & Jiajing Wu & Qiting Shao & Na Luo & Minwei Xu & Yuanmiao Sun & Yongbing Tang & Jing Peng & Hui-Ming Cheng, 2023. "Acidic enol electrooxidation-coupled hydrogen production with ampere-level current density," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    4. Botao Zhu & Bo Dong & Feng Wang & Qifeng Yang & Yunpeng He & Cunjin Zhang & Peng Jin & Lai Feng, 2023. "Unraveling a bifunctional mechanism for methanol-to-formate electro-oxidation on nickel-based hydroxides," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    5. Xintong Gao & Xiaowan Bai & Pengtang Wang & Yan Jiao & Kenneth Davey & Yao Zheng & Shi-Zhang Qiao, 2023. "Boosting urea electrooxidation on oxyanion-engineered nickel sites via inhibited water oxidation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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