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Carbon defects enhanced TEMPO redox cycles for high-efficiency urotropine electrosynthesis

Author

Listed:
  • Shiyun Li

    (Peking University, Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering)

  • Guangsheng Liu

    (University of California San Diego, Program of Materials Science and Engineering)

  • Chuhao Liu

    (Fuzhou University, Institute of Molecular Engineering Plus, College of Chemistry)

  • Yifan Fu

    (Peking University, Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering)

  • Yixuan Fu

    (Peking University, Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering)

  • Yifei Xu

    (Peking University, Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering)

  • Chengyu Li

    (Peking University, Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering)

  • Xueqiang Zhang

    (Beijing Institute of Technology, Laser Micro/Nano-Fabrication Laboratory, School of Mechanical Engineering)

  • Bingjun Xu

    (Peking University, Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering)

  • Wan-Lu Li

    (University of California San Diego, Program of Materials Science and Engineering
    University of California San Diego, Aiiso Yufeng Li Family Department of Chemical and Nano Engineering)

  • Mufan Li

    (Peking University, Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering)

Abstract

Electrocatalysis provides a sustainable alternative route to produce nitrogen-containing molecules. However, poor carbon-nitrogen (C-N) coupling selectivity and limited current density pose challenges to its widespread adoption. Herein, we introduce a carbon-defect enhanced 2,2,6,6-tetramethylpiperidine N-oxyl (TEMPO) mediated tandem process to tackle both problems. Our hetero-homogeneous system achieves a Faraday efficiency of ~99% with industrial-level current density of ~0.6 A·cm−2 for urotropine electrosynthesis. In situ near ambient pressure X-ray photoelectron spectroscopy and quasi in situ electron paramagnetic resonance reveal that the boosted activity originated from the oxidation of TEMPOH on the carbon defective sites, which accelerates the redox cycling of the molecular mediator for urotropine formation. This work highlights the catalytic effect of carbon defects on the redox cycling of TEMPO, improves both the selectivity and the rate of the electrocatalytic C-N coupling reaction, and offers insights for designing efficient electrochemical mediated oxidation processes and C-N coupling reactions.

Suggested Citation

  • Shiyun Li & Guangsheng Liu & Chuhao Liu & Yifan Fu & Yixuan Fu & Yifei Xu & Chengyu Li & Xueqiang Zhang & Bingjun Xu & Wan-Lu Li & Mufan Li, 2025. "Carbon defects enhanced TEMPO redox cycles for high-efficiency urotropine electrosynthesis," Nature Communications, Nature, vol. 16(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-65638-7
    DOI: 10.1038/s41467-025-65638-7
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