Direct CO₂ dissociation into carbonyl (*CO) offers a simplified reaction route for CO₂-related synthesis. This study constructs a subnano MoO₃ layer on Mo₂N, creating a dynamic MoO₃/MoOₓ (x < 3) surface for CO₂ hydrogenation. Rich oxygen vacancies on the subnano MoOₓ surface directly cleave the C=O bond, forming CO at a high rate. H₂ removes the leached O atoms, regenerating active sites. The MoOₓ/Mo₂N catalyst shows excellent performance for CO₂ hydrogenation to CO, surpassing many supported metal catalysts.
