Pt/ZnxFe3-xOy for selectivity cascade amination:Dependent of interfacial electronic interaction and acid/base properties
The cascade amination of nitrobenzene with benzaldehyde represents an environmentally benign route for imine synthesis in fine chemistry. Nevertheless, challenges including harsh reaction conditions, inefficiency, and poor selectivity hinder its practical implementation. Herein, we report a Pt/Zn x Fe 3-x O y interfacial catalyst system that synergistically modulates both electronic states of Pt nanoparticles (NPs) and acid/base properties of the support to address these limitations. Controlling of chemical composition of Zn x Fe 3-x O y to can efficient regulate electronic state of Pt and acid/base sites of Pt/Zn x Fe 3-x O y . The catalytic performance was strongly dependent on the interfacial electronic interactions and acid-base properties at the Pt/Zn x Fe 3-x O 4 interface. Due to lower work function of ZnFe 2 O 4 , interfacial electrons transfer to Pt from ZnFe 2 O 4 support form rich-electronic Pt accelerated hydrogenation of nitrobenzene. Rich oxygen vacancies and hydroxyl groups as acid and base sites, optimize condensation efficiency and intermediate desorption. This dual regulation strategy achieves exceptional catalytic performance under mild conditions (30 °C, 1 MPa H 2 , 4 h), delivering 96.0 % conversion with 96.25 % imine selectivity. More than 20 different amines compounds and gram-scale of imines (1.495 g) were synthesized over Pt/ZnFe 2 O 4 . In-situ DRIFTS spectroscopy identifies aniline as the critical intermediate, confirming the proposed cascade mechanism. Our work establishes a materials design paradigm leveraging support composition to reconcile electronic and acid-base requirements in tandem catalysis.
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