Abstract

Heterogeneous catalysis of alkenes to alkanes is of great importance in chemical industry, but more efficient and reusable heterogeneous catalysts are still demanded. Here, we report a metallically gradated composite of a silicon nanowire array and palladium nanoparticles which are reused for the hydrogenation of an alkene. The catalyst promotes the hydrogenation of stilbene with atmospheric hydrogen (0.1 MPa) to give diphenylethane quantitatively. The recovered catalyst can be reused, and mediates the reaction without loss of yield more than one hundred times, whereas the stability of Pd/C degrades rapidly over 10 cycles of reuse. The catalyst allows the hydrogenation of a variety of alkenes, including tetra-substituted olefins. Structural investigation reveals that palladium nanoparticles are metallically gradated onto the silicon nanowire array under mild conditions by agglomeration of palladium silicide, as confirmed by XAFS and XPS together with argon-ion sputtering. This means of metal agglomeration immobilization may be applicable to the preparation of a variety of metal nanoparticle catalysts.

Highlights

  • Heterogeneous catalysis of alkenes to alkanes is of great importance in chemical industry, but more efficient and reusable heterogeneous catalysts are still demanded

  • The other is the immobilization of metal species in solid matrices of polymers, dendrimers, and organic frameworks via coordinative interactions, where the metal species are stabilized through the steric bulk of the frameworks and/or the coordinative interactions with heteroatoms (e.g. N, O, P, and S) (Fig. 1b)[15,16,17,18,19,20,21,22,23,24,25]

  • We investigate the reusability of this system for the hydrogenation of olefins, where the catalyst can be readily reused more than one hundred times without loss of catalytic activity

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Summary

Introduction

Heterogeneous catalysis of alkenes to alkanes is of great importance in chemical industry, but more efficient and reusable heterogeneous catalysts are still demanded. We reported the development of a silicon nanowire array and palladium nanoparticle hybrid (SiNA-Pd) for catalytic organic transformations[33,34]. The recovered catalyst was reused without of loss of catalytic activity 150 times more in the same reaction and afforded 2a quantitatively in all conversions (Fig. 3).

Results
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