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Combined temperature-programmed reaction and in-situ x-ray scattering studies of size-selected silver clusters under realistic reaction conditions in the epoxidation of propene.

Journal Article · · J. Chem. Phys.
DOI:https://doi.org/10.1063/1.3237158· OSTI ID:966671
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The catalytic activity and dynamical shape changes in size-selected nanoclusters at work are studied under realistic reaction conditions by using a combination of simultaneous temperature-programmed reaction with in situ grazing-incidence small angle x-ray scattering. This approach allows drawing a direct correlation between nanocatalyst size, composition, shape, and its function under realistic reaction conditions for the first time. The approach is illustrated in a chemical industry highly relevant selective partial oxidation of propene on a monodisperse silver nanocatalyst. The shape of the catalyst undergoes rapid change already at room temperature upon the exposure to the reactants, followed by a complex evolution of shape with increasing temperature. Acrolein formation is observed around 50 C while the formation of the propylene oxide exhibits a sharp onset at 80 C and is leveling off at 150 C. At lower temperatures acrolein is produced preferentially to propylene oxide; at temperatures above 100 C propylene oxide is favored.
Research Organization:
Argonne National Laboratory (ANL)
Sponsoring Organization:
SC; Air Force Office fo Scientific Research; Deutsche Forschungsgemeinschaft; German Science Foundation
DOE Contract Number:
AC02-06CH11357
OSTI ID:
966671
Report Number(s):
ANL/CSE/JA-64094
Journal Information:
J. Chem. Phys., Journal Name: J. Chem. Phys. Journal Issue: Sep. 28, 2009 Vol. 131; ISSN JCPSA6; ISSN 0021-9606
Country of Publication:
United States
Language:
ENGLISH

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
ACROLEIN
CATALYSIS
CATALYSTS
CATALYTIC EFFECTS
EPOXIDES
MORPHOLOGICAL CHANGES
OXIDATION
PROPYLENE
SILVER