In situ Re‐construction of Pt Nanoparticles Interface for Highly Selective Synthesis of Primary Amines

Abstract Regulation of the catalyst interface by adsorbates has been demonstrated as an efficacious methodology to enhance the catalytic selectivity. Herein, we demonstrated an in situ modifications induced by reactants to re‐construct the local interface of Pt nanoparticles anchored on the CoFe layered double hydroxides (CoFe‐LDH) supports for a highly selective synthesis of primary amines from reductive amination of aldehydes and ammonia. The strong metal‐support interaction between Pt metals and CoFe‐LDH supports results in the highly electron‐enriched surface of Pt and thereby makes the surface of Pt nanoparticles favor the enrichment of NH 4 + species and adsorption of NH 3 . Such a tailored interface can create an interfacial stereo‐hindrance effect and effectively slug the reaction kinetics of side‐reactions, further preventing the formation of side‐products. We anticipate that such an in situ re‐construction of metal interface by reactants and afterwards the constructed local environment of active sites may provide a new approach for the optimization of metal catalysts.