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 Co4 N-Co3 O4 interface structure is designed to determine the effect of interfacial active centers on hydrogen generation from ammonia borane. An unparalleled catalytic activity toward H2 production with a turnover frequency up to 79 min-1 is achieved on Co4 N-Co3 O4 @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 Co4 N-Co3 O4 interface facilitates the targeted adsorption and activation of NH3 BH3 and H2 O molecules to generate H* and H2 . The two active centers of Co(N)* and Co(O)* at the Co4 N-Co3 O4 interface activate NH3 BH3 and H2 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.
Keywords: Co 4N-Co 3O 4@C; active centers; atomic interface-exciting effect; hydrogen generation; hydrolysis.
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