Atomic Interface‐Exciting Catalysis on Cobalt Nitride‐Oxide for Accelerating Hydrogen Generation

Abstract The rational design of the interface structure between nitride and oxide using the same metallic element and correlating the interfacial active center with a determined catalytic mechanism remain challenging. Herein, a Co 4 N‐Co 3 O 4 interface structure is designed to determine the effect of interfacial active centers on hydrogen generation from ammonia borane. An unparalleled catalytic activity toward H 2 production with a turnover frequency up to 79 min −1 is achieved on Co 4 N‐Co 3 O 4 @C catalyst for ten recycles. Experimental analyses and theoretical simulation suggest that the atomic interface‐exciting effect (AieE) is responsible for the high catalytic activity. The Co 4 N‐Co 3 O 4 interface facilitates the targeted adsorption and activation of NH 3 BH 3 and H 2 O molecules to generate H * and H 2 . The two active centers of Co (N) * and Co (O) * at the Co 4 N‐Co 3 O 4 interface activate NH 3 BH 3 and H 2 O, respectively. This proof‐of‐concept research on AieE provides important insights regarding the design of heterogeneous catalysts and promotes the development of the nature and regulation of energy chemical conversion.