Catalytic Kinetics Regulation for Enhanced Electrochemical Nitrogen Oxidation by Ru‐Nanoclusters‐Coupled Mn₃O₄ Catalysts Decorated with Atomically Dispersed Ru Atoms

Abstract Electrochemical N₂ oxidation reaction (NOR), using water and N₂ in the atmosphere, represents a sustainable approach for nitric production to replace the conventional industrial synthesis with high energy consumption and greenhouse gas emission. Meanwhile, owing to chemical inertness of N₂ and sluggish kinetics for 10‐electron transfer, emerging electrocatalysts remain largely underexplored. Herein, Ru‐nanoclusters‐coupled Mn₃O₄ catalysts decorated with atomically dispersed Ru atoms (Ru–Mn₃O₄) are designed and explored as an advanced electrocatalyst for ambient N₂ oxidation, with an excellent Faraday efficiency (28.87%) and a remarkable NO₃^‐ yield (35.34 µg h^‐1 mg^‐1_cat.), respectively. Experiments and density functional theory calculations reveal that the outstanding activity is ascribed to the coexistence of Ru clusters and single‐atom Ru. The synergistic effect between the Ru clusters and Mn₃O₄ can effectively activate the chemically inert N₂, lowering the kinetic barrier for the vital breakage of N≡N. The intensive *OH supply and enhanced conductivity are used to regulate the catalytic kinetics for optimized performance. This work provides brand‐new ideas for the rational design of electrocatalysts in complicated electrocatalytic reactions with multiple dynamics‐different steps.