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Reduction and re-oxidation of Cu/Al2O3 catalysts investigated with quick-scanning XANES and EXAFS

J Stötzel1,5, D Lützenkirchen-Hecht1, R Frahm1, B Kimmerle2, A Baiker2, M Nachtegaal3, M J Beier4 and J-D Grunwaldt4,5

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In the present study the structure of copper catalysts on alumina support were investigated in situ and time resolved during reduction and re-oxidation at different temperatures with the quick-scanning EXAFS (QEXAFS) technique. Different impregnation times (2 min and 90 min) were chosen for the preparation which resulted in different copper species that show a strong variation in the reduction/re-oxidation behaviour. These dynamic changes as well as possible intermediate phases during the gas atmospheres changes were followed with up to 20 EXAFS spectra per second at the copper K-edge covering an energy range of 450 eV. The high time resolution provided new insights into the dynamics of the catalysts e.g. revealing Cu(I) as intermediate state during re-oxidation. Latest advances in the data acquisition hardware are leading to an improved data quality of spectra collected at the SuperXAS beamline. Thus, not only accurate analysis of the catalysts via XANES but also by EXAFS was possible. This is also due to the recent upgrade to monitor the Bragg angle directly with an encoder during the experiments.


PACS

78.70.Dm X-ray absorption spectra

64.70.K- Solid–solid transitions

82.30.-b Specific chemical reactions; reaction mechanisms

82.65.+r Surface and interface chemistry; heterogeneous catalysis at surfaces

Subjects

Condensed matter: electrical, magnetic and optical

Surfaces, interfaces and thin films

Condensed matter: structural, mechanical & thermal

Chemical physics and physical chemistry

Dates

Issue 1 (2009)



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