Dynamic behaviour of tantalum hydride supported on silica or MCM-41 in the metathesis of alkanes

Handle URI:
http://hdl.handle.net/10754/563166
Title:
Dynamic behaviour of tantalum hydride supported on silica or MCM-41 in the metathesis of alkanes
Authors:
Soignier, Sophie; Saggio, Guillaume; Taoufik, Mostafa; Basset, Jean-Marie ( 0000-0003-3166-8882 ) ; Thivolle-Cazat, Jean
Abstract:
The metathesis of ethane and propane catalysed by tantalum hydride supported on silica or MCM-41 was studied under static and dynamic conditions. During the reaction, the rate decreased over time, indicating deactivation of the catalyst. The evolution of the catalytic system and surface species over time was monitored by various physico-chemical methods: FTIR, 13C NMR spectroscopy, elemental analysis and chemical reactivity. A carbonaceous deposit composed of unsaturated hydrocarbyl species was observed by 13C NMR. This deposit was responsible for poisoning of the catalyst. The deactivation of the catalyst proved more severe at higher temperatures and under static rather than dynamic conditions. A partial regeneration of the catalyst could be achieved during a series of repeated runs. Mechanistically, the deconvolution of the products' distribution over time indicated the occurrence of hydrogenolysis in the early stages of the reaction, while pure metathesis dominated later on. The hydrogen was supplied by the dehydrogenation of hydrocarbyl surface species involved in the deactivation process. © 2014 The Royal Society of Chemistry.
KAUST Department:
KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division; Chemical Science Program
Publisher:
Royal Society of Chemistry (RSC)
Journal:
Catal. Sci. Technol.
Issue Date:
2014
DOI:
10.1039/c3cy00545c
Type:
Article
ISSN:
20444753
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorSoignier, Sophieen
dc.contributor.authorSaggio, Guillaumeen
dc.contributor.authorTaoufik, Mostafaen
dc.contributor.authorBasset, Jean-Marieen
dc.contributor.authorThivolle-Cazat, Jeanen
dc.date.accessioned2015-08-03T11:37:18Zen
dc.date.available2015-08-03T11:37:18Zen
dc.date.issued2014en
dc.identifier.issn20444753en
dc.identifier.doi10.1039/c3cy00545cen
dc.identifier.urihttp://hdl.handle.net/10754/563166en
dc.description.abstractThe metathesis of ethane and propane catalysed by tantalum hydride supported on silica or MCM-41 was studied under static and dynamic conditions. During the reaction, the rate decreased over time, indicating deactivation of the catalyst. The evolution of the catalytic system and surface species over time was monitored by various physico-chemical methods: FTIR, 13C NMR spectroscopy, elemental analysis and chemical reactivity. A carbonaceous deposit composed of unsaturated hydrocarbyl species was observed by 13C NMR. This deposit was responsible for poisoning of the catalyst. The deactivation of the catalyst proved more severe at higher temperatures and under static rather than dynamic conditions. A partial regeneration of the catalyst could be achieved during a series of repeated runs. Mechanistically, the deconvolution of the products' distribution over time indicated the occurrence of hydrogenolysis in the early stages of the reaction, while pure metathesis dominated later on. The hydrogen was supplied by the dehydrogenation of hydrocarbyl surface species involved in the deactivation process. © 2014 The Royal Society of Chemistry.en
dc.publisherRoyal Society of Chemistry (RSC)en
dc.titleDynamic behaviour of tantalum hydride supported on silica or MCM-41 in the metathesis of alkanesen
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.identifier.journalCatal. Sci. Technol.en
dc.contributor.institutionUniversité de Lyon, C2P2 UMR 5265, CNRS-CPE-Université Lyon 1, 43 Boulevard du 11 Novembre 1918, F-69616, Villeurbanne, Franceen
kaust.authorBasset, Jean-Marieen
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