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  Activation and Isomerization of n-Butane on Sulfated Zirconia Model Systems - An Integrated Study Across the Materials and Pressure Gaps

Breitkopf, C., Papp, H., Li, X., Olindo, R., Lercher, J. A., Lloyd, R., et al. (2007). Activation and Isomerization of n-Butane on Sulfated Zirconia Model Systems - An Integrated Study Across the Materials and Pressure Gaps. Physical Chemistry Chemical Physics, 9(27), 3600-3618. doi:10.1039/b701854a.

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 Creators:
Breitkopf, Cornelia1, Author
Papp, Helmut1, Author
Li, Xuebing2, Author
Olindo, Roberta2, Author
Lercher, Johannes A.2, Author
Lloyd, Rhys3, Author           
Wrabetz, Sabine3, Author           
Jentoft, Friederike C.3, Author           
Meinel, Klaus4, Author
Förster, Stefan4, Author
Schindler, Karl-Michael4, Author
Neddermeyer, Henning4, Author
Widdra, Wolf4, Author
Hofmann, Alexander5, Author
Sauer, Joachim5, Author
Affiliations:
1Universität Leipzig, Institut für Technische Chemie, Leipzig, Germany, ou_persistent22              
2Technische Universität München, Lehrstuhl für Technische Chemie II, Garching, Germany, ou_persistent22              
3Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
4Martin-Luther-University Halle-Wittenberg, Institute of Physics, Halle, Germany, ou_persistent22              
5Institut für Chemie, Humboldt-Universität zu Berlin, Berlin, Germany, ou_persistent22              

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Free keywords: Project 1: Acid-base & redox properties of promoted sulfated zirconia, Project 3: Zirconium oxide model systems
 Abstract: Butane activation has been studied using three types of sulfated zirconia materials, single-crystalline epitaxial films, nanocrystalline films, and powders. A surface phase diagram of zirconia in interaction with SO3 and water was established by DFT calculations which was verified by LEED investigations on single-crystalline films and by IR spectroscopy on powders. At high sulfate surface densities a pyrosulfate species is the prevailing structure in the dehydrated state; if such species are absent, the materials are inactive. Theory and experiment show that the pyrosulfate can react with butane to give butene, H2O and SO2, hence butane can be activated via oxidative dehydrogenation. This reaction occurred on all investigated materials; however, isomerization could only be proven for powders. Transient and equilibrium adsorption measurements in a wide pressure and temperature range (isobars measured via UPS on nanocrystalline films, microcalorimetry and temporal analysis of products measurements on powders) show weak and reversible interaction of butane with a majority of sites but reactive interaction with < 5 µmol/g sites. Consistently, the catalysts could be poisoned by adding sodium to the surface in a ratio S/Na=35. Future research will have to clarify what distinguishes these few sites.

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Language(s): eng - English
 Dates: 2007
 Publication Status: Issued
 Pages: 19
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: eDoc: 315346
DOI: 10.1039/b701854a
 Degree: -

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Title: Physical Chemistry Chemical Physics
  Abbreviation : Phys. Chem. Chem. Phys.
Source Genre: Journal
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Publ. Info: Cambridge, England : Royal Society of Chemistry
Pages: 19 Volume / Issue: 9 (27) Sequence Number: - Start / End Page: 3600 - 3618 Identifier: ISSN: 1463-9076
CoNE: https://pure.mpg.de/cone/journals/resource/954925272413_1