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

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 NH4+ species and adsorption of NH3. 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.

Automated summary

In this study, we demonstrated an in situ modification induced by reactants to reconstruct the local interface of Pt nanoparticles anchored on CoFe layered double hydroxides (CoFe-LDH) supports, resulting in a highly selective synthesis of primary amines. The strong metal-support interaction between Pt metals and CoFe-LDH supports led to a highly electron-enriched surface of Pt, favoring the enrichment of NH4+ species and adsorption of NH3. This tailored interface created an interfacial stereo-hindrance effect, effectively suppressing side-reactions and preventing the formation of side-products. We anticipate that this in situ reconstruction of metal interfaces and the subsequent construction of local active site environments may provide a new approach for optimizing metal catalysts.