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<p>Cyclohexanone oxime (CHO) electrosynthesis from NO and cyclohexanone with high Faradaic efficiency at ampere-level current density is desirable but challenging. Here theoretical calculations reveal that NO coverage on silver catalysts plays a critical role in CHO electrosynthesis. We then experimentally adjust the NO coverage by tuning the bulk NO concentration and reaction rate. We find that low NO coverage benefits NH<sub>3</sub> formation, whereas high coverage delivers CHO and N<sub>2</sub>. Mechanistic studies indicate that with increasing NO coverage, active sites transfer from bridge step to hollow terrace sites at which NH<sub>2</sub>OH* can stably exist, rather than its decomposition into NH<sub>3</sub>. However, N‒N coupling also readily occurs at high NO coverage. This understanding inspires us to develop a doping strategy to inhibit NO–NO coupling at high NO coverage. A ruthenium-doped silver catalyst is therefore developed, realizing 86% CHO Faradaic efficiency at 1.0 A cm<sup>−2</sup>, far exceeding previously reported performance.</p><p></p>

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Ampere-level electrosynthesis of a nylon-6 precursor by local NO coverage tuning

  • 期刊论文

  • 发表日期：

    2025年8月7日

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  • Yongmeng Wu,
  • Xinyu Liu,
  • Rong Yang,
  • Chuanqi Cheng,
  • Ziyang Song,
  • Bin Zhang

摘要

Cyclohexanone oxime (CHO) electrosynthesis from NO and cyclohexanone with high Faradaic efficiency at ampere-level current density is desirable but challenging. Here theoretical calculations reveal that NO coverage on silver catalysts plays a critical role in CHO electrosynthesis. We then experimentally adjust the NO coverage by tuning the bulk NO concentration and reaction rate. We find that low NO coverage benefits NH3 formation, whereas high coverage delivers CHO and N2. Mechanistic studies indicate that with increasing NO coverage, active sites transfer from bridge step to hollow terrace sites at which NH2OH* can stably exist, rather than its decomposition into NH3. However, N‒N coupling also readily occurs at high NO coverage. This understanding inspires us to develop a doping strategy to inhibit NO–NO coupling at high NO coverage. A ruthenium-doped silver catalyst is therefore developed, realizing 86% CHO Faradaic efficiency at 1.0 A cm−2, far exceeding previously reported performance.