Crossref journal-article
AIP Publishing
The Journal of Chemical Physics (317)
Abstract

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.

Bibliography

Vajda, S., Lee, S., Sell, K., Barke, I., Kleibert, A., von Oeynhausen, V., Meiwes-Broer, K.-H., Rodríguez, A. F., Elam, J. W., Pellin, M. M., Lee, B., Seifert, S., & Winans, R. E. (2009). 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. The Journal of Chemical Physics, 131(12).

Authors 13
  1. Stefan Vajda (first)
  2. Sungsik Lee (additional)
  3. Kristian Sell (additional)
  4. Ingo Barke (additional)
  5. Armin Kleibert (additional)
  6. Viola von Oeynhausen (additional)
  7. Karl-Heinz Meiwes-Broer (additional)
  8. Arantxa Fraile Rodríguez (additional)
  9. Jeffrey W. Elam (additional)
  10. Michael M. Pellin (additional)
  11. Byeongdu Lee (additional)
  12. Sönke Seifert (additional)
  13. Randall E. Winans (additional)
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Dates
Type When
Created 15 years, 10 months ago (Sept. 28, 2009, 3:43 p.m.)
Deposited 2 years ago (July 30, 2023, 6:12 p.m.)
Indexed 3 weeks, 2 days ago (July 30, 2025, 6:53 a.m.)
Issued 15 years, 10 months ago (Sept. 25, 2009)
Published 15 years, 10 months ago (Sept. 25, 2009)
Published Online 15 years, 10 months ago (Sept. 25, 2009)
Published Print 15 years, 10 months ago (Sept. 28, 2009)
Funders 0

None

@article{Vajda_2009, title={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}, volume={131}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.3237158}, DOI={10.1063/1.3237158}, number={12}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Vajda, Stefan and Lee, Sungsik and Sell, Kristian and Barke, Ingo and Kleibert, Armin and von Oeynhausen, Viola and Meiwes-Broer, Karl-Heinz and Rodríguez, Arantxa Fraile and Elam, Jeffrey W. and Pellin, Michael M. and Lee, Byeongdu and Seifert, Sönke and Winans, Randall E.}, year={2009}, month=sep }