Selective Aerobic Oxidation of Crotyl Alcohol Using AuPd Core-Shell Nanoparticles

Bimetallic nanoparticles containing Au and Pd were synthesized using poly(vinylpyrrolidone) (PVP) as the polymer stabilizer using both co-reduction and sequential reduction strategies. The nanoparticle structures and catalytic activities for the aerobic oxidation of crotyl alcohol to crotonaldehyde...

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Bibliographic Details
Published in:ACS catalysis 2011-05, Vol.1 (5), p.425-436
Main Authors: Balcha, Tesfalidet, Strobl, Jonathan R, Fowler, Candace, Dash, Priyabrat, Scott, Robert W. J
Format: Article
Language:English
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Summary:Bimetallic nanoparticles containing Au and Pd were synthesized using poly(vinylpyrrolidone) (PVP) as the polymer stabilizer using both co-reduction and sequential reduction strategies. The nanoparticle structures and catalytic activities for the aerobic oxidation of crotyl alcohol to crotonaldehyde at room temperature in the absence of base were investigated. The chemical, structural, and electronic properties of these nanoparticles were investigated using Pd-K-edge and Au-LIII-edge extended X-ray absorption fine structure (EXAFS) spectroscopy and Pd-LIII and Au-LIII edge X-ray absorption near edge structure (XANES) spectroscopy. EXAFS analysis for the sequentially reduced bimetallic systems indicates the presence of significantly Pd-enriched surfaces and Au cores. XANES spectra of the Pd-LIII edges indicated that the sequentially reduced particles showed significant d-charge depletion compared to pure monometallic Pd and co-reduced AuPd nanoparticles. The sequentially reduced nanoparticles with Pd rich surfaces were extremely active for crotyl alcohol oxidation at room temperature in the absence of base, and were quite selective for the formation of crotonaldehyde. A proposed mechanism for the reaction involving the oxidation and re-reduction of Pd on the surface of the particles is postulated based on catalytic activity measurements using sequentially reduced particles and control reactions with Pd2+ salts in the absence and presence of Au, Pd, and Pt nanoparticles.
ISSN:2155-5435
2155-5435
DOI:10.1021/cs200040a