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Electrosynthesis of formamide from methanol and ammonia under ambient conditions

Author

Listed:
  • Nannan Meng

    (Tianjin University)

  • Jiang Shao

    (Tianjin University)

  • Hongjiao Li

    (Sichuan University)

  • Yuting Wang

    (Tianjin University
    Haihe Laboratory of Sustainable Chemical Transformations)

  • Xiaoli Fu

    (Tianjin University)

  • Cuibo Liu

    (Tianjin University)

  • Yifu Yu

    (Tianjin University
    Haihe Laboratory of Sustainable Chemical Transformations)

  • Bin Zhang

    (Tianjin University
    Haihe Laboratory of Sustainable Chemical Transformations
    Tianjin University)

Abstract

Electrochemical conversion of abundant carbon- and nitrogen-containing small molecules into high-valued organonitrogen compounds is alluring to reducing current dependence on fossil energy. Here we report a single-cell electrochemical oxidation approach to transform methanol and ammonia into formamide under ambient conditions over Pt electrocatalyst that provides 74.26% selectivity from methanol to formamide and a Faradaic efficiency of 40.39% at 100 mA cm−2 current density, gaining an economic advantage over conventional manufacturing based on techno-economic analysis. A 46-h continuous test performed in the flow cell shows no performance decay. The combined results of in situ experiments and theoretical simulations unveil the C–N bond formation mechanism via nucleophilic attack of NH3 on an aldehyde-like intermediate derived from methanol electrooxidation. This work offers a way to synthesize formamide via C–N coupling and can be extended to substantially synthesize other value-added organonitrogen chemicals (e.g., acetamide, propenamide, formyl methylamine).

Suggested Citation

  • Nannan Meng & Jiang Shao & Hongjiao Li & Yuting Wang & Xiaoli Fu & Cuibo Liu & Yifu Yu & Bin Zhang, 2022. "Electrosynthesis of formamide from methanol and ammonia under ambient conditions," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33232-w
    DOI: 10.1038/s41467-022-33232-w
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    References listed on IDEAS

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    Cited by:

    1. Nannan Meng & Zhitan Wu & Yanmei Huang & Jie Zhang & Maoxin Chen & Haibin Ma & Hongjiao Li & Shibo Xi & Ming Lin & Wenya Wu & Shuhe Han & Yifu Yu & Quan-Hong Yang & Bin Zhang & Kian Ping Loh, 2024. "High yield electrosynthesis of oxygenates from CO using a relay Cu-Ag co-catalyst system," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Jiao Lan & Zengxi Wei & Ying-Rui Lu & DeChao Chen & Shuangliang Zhao & Ting-Shan Chan & Yongwen Tan, 2023. "Efficient electrosynthesis of formamide from carbon monoxide and nitrite on a Ru-dispersed Cu nanocluster catalyst," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. Qiqi Mao & Xu Mu & Wenxin Wang & Kai Deng & Hongjie Yu & Ziqiang Wang & You Xu & Liang Wang & Hongjing Wang, 2023. "Atomically dispersed Cu coordinated Rh metallene arrays for simultaneously electrochemical aniline synthesis and biomass upgrading," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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