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<p>Direct co-conversion of earth-abundant N<sub>2</sub> and CH<sub>4</sub> to high-value C–N–O compounds is a promising synthetic method but remains challenging, as the activation of N<sub>2</sub> and CH<sub>4</sub> typically requires high-energy conditions that can cause product decomposition. Here we report a plasma-cascade process for synthesizing cyclohexanone cyanohydrin (Cy(OH)CN) via direct coupling of N<sub>2</sub> and CH<sub>4</sub> plasma with cyclohexanone. This catalyst-free process achieves a Cy(OH)CN formation rate of 0.60 mmol h<sup>−1</sup> with a high selectivity of 95.8% towards the cyclohexanone-derived products under mild conditions, concurrently generating ammonia as a valuable coproduct. Comprehensive mechanistic studies reveal that plasma-generated ·CH<sub><i>x</i></sub> and hydrogen radicals enable direct α-carbonyl functionalization of cyclohexanone to α-CH<sub><i>x</i></sub> cyclohexanol intermediates, which then coupled mainly with excited-state N<sub>2</sub> and are further activated by hydrogen radicals to generate Cy(OH)CN. This plasma-cascade strategy decouples the activation of inert molecules from the formation of relatively unstable C–N–O compounds, enabling selective cyanohydrin synthesis that avoids using high-cost NH<sub>3</sub> and toxic HCN.</p><p></p>

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Direct plasma synthesis of a high-value C–N–O compound with inert N2 and CH4

  • 期刊论文

  • 发表日期：

    2026年4月21日

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  • Hao Zhang,
  • Ziming Liu,
  • Di Li,
  • Chenxin Wu,
  • Lei Hua,
  • Haiyang Li,
  • Yanhui Yi,
  • Rui Huang,
  • Liang Yu,
  • Dehui Deng

摘要

Direct co-conversion of earth-abundant N2 and CH4 to high-value C–N–O compounds is a promising synthetic method but remains challenging, as the activation of N2 and CH4 typically requires high-energy conditions that can cause product decomposition. Here we report a plasma-cascade process for synthesizing cyclohexanone cyanohydrin (Cy(OH)CN) via direct coupling of N2 and CH4 plasma with cyclohexanone. This catalyst-free process achieves a Cy(OH)CN formation rate of 0.60 mmol h−1 with a high selectivity of 95.8% towards the cyclohexanone-derived products under mild conditions, concurrently generating ammonia as a valuable coproduct. Comprehensive mechanistic studies reveal that plasma-generated ·CHx and hydrogen radicals enable direct α-carbonyl functionalization of cyclohexanone to α-CHx cyclohexanol intermediates, which then coupled mainly with excited-state N2 and are further activated by hydrogen radicals to generate Cy(OH)CN. This plasma-cascade strategy decouples the activation of inert molecules from the formation of relatively unstable C–N–O compounds, enabling selective cyanohydrin synthesis that avoids using high-cost NH3 and toxic HCN.