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

Shiyun Li, Guangsheng Liu, Chuhao Liu, Yifan Fu, Yixuan Fu, Yifei Xu, Chengyu Li, Xueqiang Zhang (), Bingjun Xu (), Wan-Lu Li () and Mufan Li ()
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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
Mufan Li: Peking University, Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-65638-7

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