Metallically gradated silicon nanowire and palladium nanoparticle composites as robust hydrogenation catalysts

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.