The objective of the thesis was to analyze the ageing processes and the modifications of an Ir/CeO2catalyst for steam reforming of ethanol. Over a model Ir/CeO2 catalyst, the initial and fast deactivationwas ascribed to ceria surface restructuring and the build-up of intermediates monolayer (acetate,carbonate and hydroxyl groups). In parallel, a progressive and slow deactivation was found to come fromthe structural changes at the ceria/Ir interface linked to Ir sintering and ceria restructuring. Theencapsulating carbon, coming from C2 intermediates polymerization, did not seem too detrimental to theactivity in the investigated operating conditions. By doping ceria with PrOx, the oxygen storage capacityand thermal stability were greatly promoted, resulting in the enhanced activity and stability. The Ir/CeO2catalyst was then modified by changing the shape of ceria. It was found that the shape and therefore thestructure of ceria influenced the activity and stability significantly. A simplified modeling of theseprocesses has contributed to support the new proposals of this work.
| Identifer | oai:union.ndltd.org:CCSD/oai:tel.archives-ouvertes.fr:tel-00967128 |
| Date | 23 October 2012 |
| Creators | Wang, Fagen |
| Publisher | Université Claude Bernard - Lyon I |
| Source Sets | CCSD theses-EN-ligne, France |
| Language | English |
| Detected Language | English |
| Type | PhD thesis |
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