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<p>The manufacture of nitriles is critical to various industrial applications, but poor selectivity results in the significant release of pollutive byproducts such as CO<sub>2</sub>, NO<sub><i>x</i></sub> and toxic cyanide. Here, we report the electrochemical conversion of benzaldehyde to benzonitrile at near-unity selectivity, during which Co<sub>3</sub>O<sub>4</sub> clusters-decorated Cu<sub><i>x</i></sub>O electrocatalyst activates the C−N bond of an unstable intermediate species. Operando spectroelectrochemical studies and theoretical calculations reveal that benzaldehyde couples with NH<sub>3</sub> to form the phenylmethanimine intermediate bound atop Cu<sup>2+</sup> active sites, which facilitates hydrogen transfer from the imine group to nearby surface oxygen. Our electrochemical system can convert aromatic and aliphatic aldehydes to the corresponding nitriles at Faradaic efficiencies of 78–97%. This can be paired with cathodic NO<sub><i>x</i></sub> reduction, which produces a commensurable amount of NH<sub>3</sub> to that consumed even at a current density of 200 mA cm<sup>−2</sup>. Our work offers a clean synthetic route to otherwise-pollutive chemicals, and also expands the repertoire of organonitrogen compounds that can be accessed by electrocatalysis.</p>

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A cyanide-free route towards the electrosynthesis of nitriles

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月17日

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  • Jiahui Xian,
  • Lulu Wang,
  • Ziyu Mi,
  • Meng Wang,
  • Sze Xing Tan,
  • Xun Cao,
  • Mingsheng Zhang,
  • Shibo Xi,
  • Jiajian Gao,
  • Yanwei Lum,
  • Pengfei Ou,
  • Wan Ru Leow

摘要

The manufacture of nitriles is critical to various industrial applications, but poor selectivity results in the significant release of pollutive byproducts such as CO2, NOx and toxic cyanide. Here, we report the electrochemical conversion of benzaldehyde to benzonitrile at near-unity selectivity, during which Co3O4 clusters-decorated CuxO electrocatalyst activates the C−N bond of an unstable intermediate species. Operando spectroelectrochemical studies and theoretical calculations reveal that benzaldehyde couples with NH3 to form the phenylmethanimine intermediate bound atop Cu2+ active sites, which facilitates hydrogen transfer from the imine group to nearby surface oxygen. Our electrochemical system can convert aromatic and aliphatic aldehydes to the corresponding nitriles at Faradaic efficiencies of 78–97%. This can be paired with cathodic NOx reduction, which produces a commensurable amount of NH3 to that consumed even at a current density of 200 mA cm−2. Our work offers a clean synthetic route to otherwise-pollutive chemicals, and also expands the repertoire of organonitrogen compounds that can be accessed by electrocatalysis.