Jump to main content
Jump to site search

Issue 27, 2007
Previous Article Next Article

Activation and isomerization of n-butane on sulfated zirconia model systems—an integrated study across the materials and pressure gaps

Author affiliations

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−1 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.

Graphical abstract: Activation and isomerization of n-butane on sulfated zirconia model systems—an integrated study across the materials and pressure gaps

Back to tab navigation

Article information


Submitted
06 Feb 2007
Accepted
11 May 2007
First published
01 Jun 2007

Phys. Chem. Chem. Phys., 2007,9, 3600-3618
Article type
Paper

Activation and isomerization of n-butane on sulfated zirconia model systems—an integrated study across the materials and pressure gaps

C. Breitkopf, H. Papp, X. Li, R. Olindo, J. A. Lercher, R. Lloyd, S. Wrabetz, F. C. Jentoft, K. Meinel, S. Förster, K.-M. Schindler, H. Neddermeyer, W. Widdra, A. Hofmann and J. Sauer, Phys. Chem. Chem. Phys., 2007, 9, 3600
DOI: 10.1039/B701854A

Social activity

Search articles by author

Spotlight

Advertisements