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<p>Direct ammoxidation of biomass-derived alcohols/aldehydes to nitriles faces challenges from N-species competitive adsorption, leading to low efficiency under harsh conditions. Herein, we report the rational design of a single-nitrogen-bridged Co-Ru dual-atom catalyst (CoRu-N-C) on nitrogen-doped carbon, enabling efficient ammoxidation at ambient conditions. At 35 °C and 1 bar air, CoRu-N-C achieved 98% yield of 2-furonitrile (FAN) with 73 mmol/g<sub>-metal</sub>/h productivity, representing a 3.5-fold enhancement compared to Co-N-C, and outperforming numerous reported noble/non-noble metal catalysts. Mechanistic studies reveal synergistic O<sub>2</sub> and imine adsorption on low-coordinated CoN<sub>3</sub> and RuN<sub>3</sub> sites, mitigating imine-induced oxygen activation inhibition. Specifically, the strong O₂ adsorption on CoN<sub>3</sub> forms superoxide radicals (O<sub>2</sub><sup>−•</sup>) via electron transfer, driving a relay mechanism with proximally adsorbed imine to accelerate overall reaction kinetics. This work provides valuable insights for the design of stable and highly efficient ammoxidation catalysts operating under mild conditions.</p>

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Low-coordinated Co-Ru dual-atom enables ambient ammoxidation via unlocking competitive adsorption limitations

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年10月22日

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  • Jialin Yang,
  • Zhecheng Fang,
  • Zhiwei Sun,
  • Wenhua Zhou,
  • Bing Nan,
  • Xiaolong Liu,
  • Zixu Ma,
  • Renfeng Nie,
  • Jie Fu

摘要

Direct ammoxidation of biomass-derived alcohols/aldehydes to nitriles faces challenges from N-species competitive adsorption, leading to low efficiency under harsh conditions. Herein, we report the rational design of a single-nitrogen-bridged Co-Ru dual-atom catalyst (CoRu-N-C) on nitrogen-doped carbon, enabling efficient ammoxidation at ambient conditions. At 35 °C and 1 bar air, CoRu-N-C achieved 98% yield of 2-furonitrile (FAN) with 73 mmol/g-metal/h productivity, representing a 3.5-fold enhancement compared to Co-N-C, and outperforming numerous reported noble/non-noble metal catalysts. Mechanistic studies reveal synergistic O2 and imine adsorption on low-coordinated CoN3 and RuN3 sites, mitigating imine-induced oxygen activation inhibition. Specifically, the strong O₂ adsorption on CoN3 forms superoxide radicals (O2−•) via electron transfer, driving a relay mechanism with proximally adsorbed imine to accelerate overall reaction kinetics. This work provides valuable insights for the design of stable and highly efficient ammoxidation catalysts operating under mild conditions.