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Time-resolved operando X-ray absorption study of CuO–CeO2/Al2O3 catalyst during total oxidation of propane

Paper ID Volume ID Publish Year Pages File Format Full-Text
47320 46467 2010 8 PDF Available
Title
Time-resolved operando X-ray absorption study of CuO–CeO2/Al2O3 catalyst during total oxidation of propane
Abstract

The local structure of the copper phase of a CuO–CeO2/Al2O3 catalyst and its activity for the total oxidation of propane have been studied under working conditions, using time-resolved X-ray absorption spectroscopy (XAS) in transmission mode at the Cu K edge coupled with on-line mass spectrometry (MS). In the temperature range of 573–723 K, the copper phase of the catalyst remains oxidized (i.e. Cu2+) during total oxidation reaction conditions (1%C3H8–5%O2/He), while three species are present (i.e. Cu2+, Cu1+ and Cu0) during reduction (2%C3H8/He) and re-oxidation (10%O2/He) treatments where a two-step mechanism is found. Catalyst reduction is fully reversible, as the Cu2+ nature of the catalyst is recovered after a reduction–oxidation cycle. Re-oxidation of the catalyst is two orders of magnitude faster than its reduction and has an apparent activation energy of 24 kJ/mol. On the other hand, catalyst reduction requires an apparent activation energy of 70 kJ/mol, which is equal to the apparent activation energy determined under total oxidation reaction conditions. These results give support to a Mars–van-Krevelen reaction scheme with the copper phase of the catalyst being close to a fully oxidized state.

Keywords
Structure–activity investigation; Supported metal oxides; Reduction and oxidation mechanism; Propane total oxidation; Volatile organic compounds
First Page Preview
Time-resolved operando X-ray absorption study of CuO–CeO2/Al2O3 catalyst during total oxidation of propane
Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis B: Environmental - Volume 97, Issues 3–4, 18 June 2010, Pages 381–388
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis