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., RodrÃguez, 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
- Stefan Vajda (first)
- Sungsik Lee (additional)
- Kristian Sell (additional)
- Ingo Barke (additional)
- Armin Kleibert (additional)
- Viola von Oeynhausen (additional)
- Karl-Heinz Meiwes-Broer (additional)
- Arantxa Fraile Rodríguez (additional)
- Jeffrey W. Elam (additional)
- Michael M. Pellin (additional)
- Byeongdu Lee (additional)
- Sönke Seifert (additional)
- Randall E. Winans (additional)
References
53
Referenced
40
10.1126/science.1104168
/ Science (2005)10.1021/ja039037k
/ J. Am. Chem. Soc. (2004)10.1063/1.1999627
/ J. Chem. Phys. (2005)10.1063/1.2035098
/ J. Chem. Phys. (2005){'first-page': '190', 'article-title': 'In situ GISAXS studies of the thermal stability and temperature induced growth of supported cluster-based platinum and gold nanoparticles', 'year': '2005', 'key': '2023073022125142900_c2c'}
/ In situ GISAXS studies of the thermal stability and temperature induced growth of supported cluster-based platinum and gold nanoparticles (2005)10.1038/415623a
/ Nature (London) (2002)10.1016/S0920-5861(96)00208-8
/ Catal. Today (1997)10.1126/science.281.5383.1647
/ Science (1998)10.1016/S0167-5729(98)00002-8
/ Surf. Sci. Rep. (1998)10.1016/S0039-6028(01)01543-6
/ Surf. Sci. (2002)10.1126/science.1083671
/ Science (2003)10.1021/jp055147x
/ J. Phys. Chem. B (2006)10.1016/0021-9517(88)90188-1
/ J. Catal. (1988)10.1007/s11244-006-0052-3
/ Top. Catal. (2006)10.1007/s11244-006-0050-5
/ Top. Catal. (2006)10.1063/1.2745330
/ J. Appl. Phys. (2007)10.1021/cm020607+
/ Chem. Mater. (2003)10.1126/science.1082146
/ Science (2003)10.1021/jp045549p
/ J. Phys. Chem. B (2004)10.1016/S0039-6028(00)00108-4
/ Surf. Sci. (2000){'volume-title': 'Small Angle Scattering of X-Rays', 'year': '1955', 'key': '2023073022125142900_c14'}
/ Small Angle Scattering of X-Rays (1955)10.1126/science.1069325
/ Science (2002)10.1002/anie.200462043
/ Angew. Chem., Int. Ed. (2005)10.1016/j.jcat.2008.06.020
/ J. Catal. (2008)10.1016/j.jcat.2009.04.023
/ J. Catal. (2009)10.1021/jp0503415
/ J. Phys. Chem. B (2005)10.1021/jp981070j
/ J. Phys. Chem. B (1998)10.1126/science.288.5468.1029
/ Science (2000)10.1016/S0039-6028(99)01089-4
/ Surf. Sci. (2000)10.1063/1.1421107
/ J. Chem. Phys. (2001)10.1063/1.1574798
/ J. Chem. Phys. (2003)10.1103/PhysRevB.66.205402
/ Phys. Rev. B (2002)10.1021/ja00341a008
/ J. Am. Chem. Soc. (1983)10.1016/S0039-6028(97)00184-2
/ Surf. Sci. (1997)10.1021/ie0513090
/ Ind. Eng. Chem. Res. (2006)10.1103/PhysRevB.63.081404
/ Phys. Rev. B (2001)10.1016/S1381-1169(00)00062-5
/ J. Mol. Catal. A: Chem. (2000)10.1023/A:1015484121891
/ Catal. Lett. (2002)10.1063/1.479488
/ J. Chem. Phys. (1999)10.1016/S0039-6028(03)00452-7
/ Surf. Sci. (2003)10.1016/j.jcat.2005.07.019
/ J. Catal. (2005)10.1016/j.jcat.2004.03.047
/ J. Catal. (2004)10.1006/jcat.1999.2427
/ J. Catal. (1999)10.1016/0039-6028(85)90634-X
/ Surf. Sci. (1985)10.1016/j.susc.2006.08.049
/ Surf. Sci. (2006)10.1103/PhysRevLett.96.146101
/ Phys. Rev. Lett. (2006)10.1103/PhysRevLett.96.146102
/ Phys. Rev. Lett. (2006)10.1016/j.susc.2006.12.008
/ Surf. Sci. (2007)10.1007/BF00806113
/ Catal. Lett. (1995)10.1002/anie.200800406
/ Angew. Chem., Int. Ed. (2008)10.1023/A:1022650723251
/ Catal. Lett. (2003)10.1016/j.molcata.2007.07.011
/ J. Mol. Catal. A: Chem. (2007)10.1021/ja075628p
/ J. Am. Chem. Soc. (2007)
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) |
@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 }