Journal
JOURNAL OF PHYSICAL CHEMISTRY B
Volume 108, Issue 47, Pages 18234-18242Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp046459n
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The structural transformation and catalytic properties of metal/polymer nanocomposites derived from hypercross-linked polystyrene (HPS) exhibiting both microporosity and macroporosity, and filled with Pt nanoparticles, are investigated in the direct oxidation Of L-sorbose to 2-keto-L-gulonic acid. Transmission electron microscopy, X-ray photoelectron spectroscopy, X-ray diffraction, anomalous small-angle X-ray scattering, and catalytic studies suggest that the catalytically active species, nanoparticles of mixed composition with a mean diameter of 1.6 nm, develop after the initial induction period. At the highest selectivity (96.8%) at 100% L-sorbose conversion, the catalytic activity is measured to be 2.5 x 10(-3) mol/mol Pt-s, which corresponds to a 4.6-fold increase in activity relative to the Pt-modified microporous HPS previously reported. This substantial increase in catalytic activity is attributed to the presence of macropores, which facilitate mass transport and, consequently, accessibility of the nanoparticle surface for reactants.
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