Low-coordinated Co-Ru dual-atom enables ambient ammoxidation via unlocking competitive adsorption limitations.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41125592.
- Also identified by DOI 10.1038/s41467-025-64418-7 and PMC identifier 12546627.
- Licence recorded as CC BY-NC-ND.
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Abstract
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.