Supported metal catalysts integrating advantages of catalytic hydrogenation and stoichiometric reduction are highly desirable for the green production of fine chemicals.Decoupling catalytic hydrogenation into H_(2)act...Supported metal catalysts integrating advantages of catalytic hydrogenation and stoichiometric reduction are highly desirable for the green production of fine chemicals.Decoupling catalytic hydrogenation into H_(2)activation and selective reduction taking place at different locations is expected to provide an effective strategy to fabricate such catalyst systems.Herein,we report a decoupled hydrogenation system by modifying Pt catalysts supported on reducible In2O3 with ethylenediamine(EDA).The system exhibits good catalytic performance in oximes production from nitroalkanes,an industrially important reaction,by employing H_(2).Systematic studies demonstrate that the surface coordination of EDA on Pt is crucial to passivate the Pt surface from nitro hydrogenation without inhibiting H_(2)activation.The activated H_(2)species can then transfer and reduce the In_(2)O_(3)support in situ to generate sustainable stoichiometric reducing agents for the chemoselective reduction of nitroalkanes.Based upon the mechanistic understanding,a sustainable strategy for the production of oximes has been successfully fabricated.展开更多
基金supported by the National Key R&D Program of China(grant no.2017YFA0207302)the National Natural Science Foundation of China(grant nos.21890752,21731005,21721001).
文摘Supported metal catalysts integrating advantages of catalytic hydrogenation and stoichiometric reduction are highly desirable for the green production of fine chemicals.Decoupling catalytic hydrogenation into H_(2)activation and selective reduction taking place at different locations is expected to provide an effective strategy to fabricate such catalyst systems.Herein,we report a decoupled hydrogenation system by modifying Pt catalysts supported on reducible In2O3 with ethylenediamine(EDA).The system exhibits good catalytic performance in oximes production from nitroalkanes,an industrially important reaction,by employing H_(2).Systematic studies demonstrate that the surface coordination of EDA on Pt is crucial to passivate the Pt surface from nitro hydrogenation without inhibiting H_(2)activation.The activated H_(2)species can then transfer and reduce the In_(2)O_(3)support in situ to generate sustainable stoichiometric reducing agents for the chemoselective reduction of nitroalkanes.Based upon the mechanistic understanding,a sustainable strategy for the production of oximes has been successfully fabricated.
