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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. Creating renewable nitriles faces challenges like competitive adsorption and harsh conditions. Here a CoRu dual-atom catalyst enables efficient ammoxidation of aldehydes to nitriles under ambient conditions through synergistic adsorption.
Yang et al. (Wed,) studied this question.