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          Institute: Fritz-Haber-Institut     Collection: Inorganic Chemistry     Display Documents



  history
ID: 213989.0, Fritz-Haber-Institut / Inorganic Chemistry
Interaction between Sulfated Zirconia and Alkanes: Prerequisites for Active Sites – Formation and Stability of Reaction Intermediates
Authors:Li, Xuebing; Nagaoka, Katsutoshi; Simon, Laurent J.; Lercher, Johannes A.; Wrabetz, Sabine; Jentoft, Friederike C.; Breitkopf, Cornelia; Matysik, Silke; Papp, Helmut
Language:English
Research Context:Project 1: Acid-base & redox properties of promoted sulfated zirconia
Date of Publication (YYYY-MM-DD):2005
Title of Journal:Journal of Catalysis
Journal Abbrev.:J. Catal.
Volume:230
Start Page:214
End Page:225
Review Status:Peer-review
Audience:Experts Only
Abstract / Description:Two sulfated zirconia catalysts were prepared via sulfation and calcination at 873 K of zirconium hydroxide aged at room temperature for 1 h (SZ-1) or aged at 373 K for 24 h (SZ-2). SZ-1 was active for n-butane isomerisation at 373 K; SZ-2 reached similar performance only at 473 K. Both materials contained about 9 wt% sulfate and were tetragonal. Due to a BET lower surface area (105 m2/g vs. 148 m2/g) SZ-1 featured a higher sulfate density, and XRD and EXAFS analysis showed larger (ca. 10 nm) and more well ordered crystals than for SZ-2. n-Butane TPD on SZ-1 showed a butene desorption peak at low temperature, whereas, no obvious butene desorption was observed with SZ-2, suggesting that SZ-1 has a higher oxidizing power at low temperature than SZ-2. The number of sites capable of dehydrogenation are less than 5 µmol/g, because the differential heats of n-butane adsorption as measured by microcalorimetry were 45–60 kJ/mol for higher coverages, indicating weak and reversible interaction. TAP experiments describe the adsorption and desorption behavior of n-butane at different activity states and are the basis for a simple adsorption model. Reactant pulses and purge experiments show that the active species, presumably formed in an oxidative dehydrogenation step, are stable at the surface under reaction conditions.
External Publication Status:published
Document Type:Article
Communicated by:Robert Schlögl
Affiliations:Fritz-Haber-Institut/Inorganic Chemistry/Functional Characterization
External Affiliations:Technische Universität München, Department of Chemistry,
Lichtenbergstraße 4, 85747 Garching, Germany

Universität Leipzig, Institute of Technical Chemistry, Linnéstr. 3, 04103 Leipzig, Germany
Identifiers:URL:http://www.sciencedirect.com/science?_ob=MImg&_ima... [only for subscriber]
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li_jentoft_etal_jcatalfinal.pdf  [527,00 Kb]   
 
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