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Selective electrosynthesis of hydroxylamine from aqueous nitrate/nitrite by suppressing further reduction

Author

Listed:
  • Yirong Tang

    (Southern University of Science and Technology)

  • Zhan Jiang

    (Southern University of Science and Technology
    Ministry of Ecology and Environment)

  • Yubo Yuan

    (Southern University of Science and Technology)

  • Li Xu

    (State Environmental Protection Center for Coal-Fired Air Pollution Control)

  • Chuyao Jin

    (State Environmental Protection Center for Coal-Fired Air Pollution Control)

  • Bulin Chen

    (Southern University of Science and Technology)

  • Zhichao Lin

    (Southern University of Science and Technology)

  • Jie Zao

    (Southern University of Science and Technology)

  • Jianwei Du

    (Ministry of Ecology and Environment)

  • Xiao Zhang

    (State Environmental Protection Center for Coal-Fired Air Pollution Control)

  • Xiang Gao

    (State Environmental Protection Center for Coal-Fired Air Pollution Control)

  • Yongye Liang

    (Southern University of Science and Technology)

Abstract

The electrocatalytic reduction of nitrogenous waste offers a sustainable approach to producing nitrogen-containing chemicals. The selective synthesis of high-value hydroxylamine (NH2OH) is challenging due to the instability of NH2OH as an intermediate. Here, we present a rational electrocatalyst design strategy for promoting NH2OH electrosynthesis by suppressing the competing pathways of further reduction. We screen zinc phthalocyanines (ZnPc) with a high energy barrier for NH2OH reduction by regulating their intrinsic activity. Additionally, we discover that carbon nanotube substrates exhibit significant NH3-producing activity, which can be effectively inhibited by the high coverage of ZnPc molecules. In-situ characterizations reveal that NH2OH and HNO are generated as intermediates in nitrate reduction to NH3, and NH2OH can be enriched in the ZnPc electrode. In the H-cell, the optimized ZnPc catalyst demonstrates a Faradaic efficiency (FE) of 53 ± 1.7% for NH2OH with a partial current density exceeding 270 mA cm−2 and a turnover frequency of 7.5 ± 0.2 s−1. It also enables the rapid electrosynthesis of cyclohexanone oxime from nitrite with a FE of 64 ± 1.0%.

Suggested Citation

  • Yirong Tang & Zhan Jiang & Yubo Yuan & Li Xu & Chuyao Jin & Bulin Chen & Zhichao Lin & Jie Zao & Jianwei Du & Xiao Zhang & Xiang Gao & Yongye Liang, 2024. "Selective electrosynthesis of hydroxylamine from aqueous nitrate/nitrite by suppressing further reduction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-54204-2
    DOI: 10.1038/s41467-024-54204-2
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    References listed on IDEAS

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    1. Jia-Yi Fang & Qi-Zheng Zheng & Yao-Yin Lou & Kuang-Min Zhao & Sheng-Nan Hu & Guang Li & Ouardia Akdim & Xiao-Yang Huang & Shi-Gang Sun, 2022. "Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    2. Yueshen Wu & Zhan Jiang & Xu Lu & Yongye Liang & Hailiang Wang, 2019. "Domino electroreduction of CO2 to methanol on a molecular catalyst," Nature, Nature, vol. 575(7784), pages 639-642, November.
    3. Yueshen Wu & Zhan Jiang & Zhichao Lin & Yongye Liang & Hailiang Wang, 2021. "Direct electrosynthesis of methylamine from carbon dioxide and nitrate," Nature Sustainability, Nature, vol. 4(8), pages 725-730, August.
    4. Yongmeng Wu & Jinghui Zhao & Changhong Wang & Tieliang Li & Bo-Hang Zhao & Ziyang Song & Cuibo Liu & Bin Zhang, 2023. "Electrosynthesis of a nylon-6 precursor from cyclohexanone and nitrite under ambient conditions," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
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