Structure and catalytic properties of Pt-modified hyper-cross-linked polystyrene exhibiting hierarchical porosity

被引:63
作者
Bronstein, LM [1 ]
Goerigk, G
Kostylev, M
Pink, M
Khotina, IA
Valetsky, PM
Matveeva, VG
Sulman, EM
Sulman, MG
Bykov, AV
Lakina, NV
Spontak, RJ
机构
[1] Indiana Univ, Dept Chem, Bloomington, IN 47405 USA
[2] Forsch Zentrum Julich, Forschungszentrum, D-52425 Julich, Germany
[3] AN Nesmeyanov Organoelement Cpds Inst, Moscow 117813, Russia
[4] Tver Tech Univ, Tver 170026, Russia
[5] N Carolina State Univ, Dept Chem Engn, Raleigh, NC 27695 USA
[6] N Carolina State Univ, Dept Mat Sci & Engn, Raleigh, NC 27695 USA
关键词
D O I
10.1021/jp046459n
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:18234 / 18242
页数:9
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