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Potential and electric double-layer effect in electrocatalytic urea synthesis

Author

Listed:
  • Qian Wu

    (Nanyang Technological University, 50 Nanyang Avenue)

  • Chencheng Dai

    (Nanyang Technological University, 50 Nanyang Avenue
    The Cambridge Centre for Advanced Research and Education in Singapore, 1 CREATE way)

  • Fanxu Meng

    (Nanyang Technological University, 50 Nanyang Avenue)

  • Yan Jiao

    (The University of Adelaide)

  • Zhichuan J. Xu

    (Nanyang Technological University, 50 Nanyang Avenue
    The Cambridge Centre for Advanced Research and Education in Singapore, 1 CREATE way
    Interdisciplinary Graduate School, Nanyang Technological University
    Nanyang Technological University, 50 Nanyang Avenue)

Abstract

Electrochemical synthesis is a promising way for sustainable urea production, yet the exact mechanism has not been fully revealed. Herein, we explore the mechanism of electrochemical coupling of nitrite and carbon dioxide on Cu surfaces towards urea synthesis on the basis of a constant-potential method combined with an implicit solvent model. The working electrode potential, which has normally overlooked, is found influential on both the reaction mechanism and activity. The further computational study on the reaction pathways reveals that *CO-NH and *NH-CO-NH as the key intermediates. In addition, through the analysis of turnover frequencies under various potentials, pressures, and temperatures within a microkinetic model, we demonstrate that the activity increases with temperature, and the Cu(100) shows the highest efficiency towards urea synthesis among all three Cu surfaces. The electric double-layer capacitance also plays a key role in urea synthesis. Based on these findings, we propose two essential strategies to promote the efficiency of urea synthesis on Cu electrodes: increasing Cu(100) surface ratio and elevating the reaction temperature.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-45522-6
    DOI: 10.1038/s41467-024-45522-6
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