4.8 Article

Zero-oxidation state precursor assisted fabrication of highly dispersed and stable Pt catalyst for chemoselective hydrogenation of α,β-unsaturated aldehydes

期刊

NANO RESEARCH
卷 16, 期 5, 页码 6085-6093

出版社

TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-022-4822-4

关键词

platinum catalyst; zero-oxidation state; stability; chemoselective hydrogenation; alpha,beta-unsaturated aldehydes

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In this study, we developed an efficient method for depositing Pt particles on FeOx/SBA-15, using Pt-0-DVTMS precursor, and demonstrated its high performance and selectivity in the chemoselective hydrogenation of alpha,beta-unsaturated aldehydes. The research also showed the significant influence of metal support interactions on the selectivity and activity of the catalyst.
The chemoselective hydrogenation of alpha,beta-unsaturated aldehydes is a key strategy for the synthesis of fine chemicals. Herein, we developed an efficient method of depositing Pt particles on FeOx/SBA-15. This strategy is dependent on using a platinumdivinyltetramethyldisiloxane complex (Pt-0-DVTMS) as the precursor, which we demonstrate can be removed through a H-2-treatment under mild conditions. This, in turn, allowed for the synthesis of catalysts with well dispersed Pt particles. The presence of FeOx species also aided Pt dispersion; when coated onto SBA-15, FeOx strongly interacted with dissociated Pt species, inhibiting both Pt aggregation and metal leaching. Using cinnamaldehyde as a model alpha,beta-unsaturated aldehyde, it was demonstrated that this catalyst was highly selective towards the unsaturated alcohol and no obvious loss in activity was observed over five recycles. This catalyst was determined to be significantly more effective than an analogous catalyst prepared using chloroplatinic acid as a precursor, evidencing the importance of using the Pt-0-DVTMS precursor. We corroborate the excellent catalytic performance to highly dispersed Pt-species, whereby Pt-0 and Pt2+ play a critical role in activating H-2 and the C=O bond. This research demonstrates that the Pt precursor can have a significant impact on the physicochemical properties and thus, the performance of the final catalyst. It also evidences how metal support interactions can dramatically influence selectivity in such hydrogenation reactions. This novel catalyst preparation protocol, using a DVTMS ligand for Pt impregnation, offers a facile approach to the design of multi-component heterogeneous catalysts.

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