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Steering from electrochemical denitrification to ammonia synthesis

Author

Listed:
  • Huan Li

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Jun Long

    (Chinese Academy of Sciences)

  • Huijuan Jing

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Jianping Xiao

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

Abstract

The removal of nitric oxide is an important environmental issue, as well as a necessary prerequisite for achieving high efficiency of CO2 electroreduction. To this end, the electrocatalytic denitrification is a sustainable route. Herein, we employ reaction phase diagram to analyze the evolution of reaction mechanisms over varying catalysts and study the potential/pH effects over Pd and Cu. We find the low N2 selectivity compared to N2O production, consistent with a set of experiments, is limited fundamentally by two factors. The N2OH* binding is relatively weak over transition metals, resulting in the low rate of as-produced N2O* protonation. The strong correlation of OH* and O* binding energies limits the route of N2O* dissociation. Although the experimental conditions of varying potential, pH and NO pressures can tune the selectivity slightly, which are insufficient to promote N2 selectivity beyond N2O and NH3. A possible solution is to design catalysts with exceptions to break the scaling characters of energies. Alternatively, we propose a reverse route with the target of decentralized ammonia synthesis.

Suggested Citation

  • Huan Li & Jun Long & Huijuan Jing & Jianping Xiao, 2023. "Steering from electrochemical denitrification to ammonia synthesis," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-35785-w
    DOI: 10.1038/s41467-023-35785-w
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    References listed on IDEAS

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    1. Byung Hee Ko & Bjorn Hasa & Haeun Shin & Emily Jeng & Sean Overa & Wilson Chen & Feng Jiao, 2020. "The impact of nitrogen oxides on electrochemical carbon dioxide reduction," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    2. Roy, Sounak & Hegde, M.S. & Madras, Giridhar, 2009. "Catalysis for NOx abatement," Applied Energy, Elsevier, vol. 86(11), pages 2283-2297, November.
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    Cited by:

    1. Qian Wu & Chencheng Dai & Fanxu Meng & Yan Jiao & Zhichuan J. Xu, 2024. "Potential and electric double-layer effect in electrocatalytic urea synthesis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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