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

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    Type
    Article
    Authors
    Soignier, Sophie
    Saggio, Guillaume
    Taoufik, Mostafa
    Basset, Jean-Marie cc
    Thivolle-Cazat, Jean
    KAUST Department
    Chemical Science Program
    KAUST Catalysis Center (KCC)
    Physical Science and Engineering (PSE) Division
    Date
    2014
    Permanent link to this record
    http://hdl.handle.net/10754/563166
    
    Metadata
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    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.
    Citation
    Soignier, S., Saggio, G., Taoufik, M., Basset, J.-M., & Thivolle-Cazat, J. (2014). Dynamic behaviour of tantalum hydride supported on silica or MCM-41 in the metathesis of alkanes. Catal. Sci. Technol., 4(1), 233–244. doi:10.1039/c3cy00545c
    Publisher
    Royal Society of Chemistry (RSC)
    Journal
    Catal. Sci. Technol.
    DOI
    10.1039/c3cy00545c
    ae974a485f413a2113503eed53cd6c53
    10.1039/c3cy00545c
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

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