Surface Coordination Decouples Hydrogenation Catalysis on Supported Metal Catalysts

Abstract

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 H2 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 H2. Systematic studies demonstrate that the surface coordination of EDA on Pt is crucial to passivate the Pt surface from nitro hydrogenation without inhibiting H2 activation. The activated H2 species can then transfer and reduce the In2O3 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.