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dc.contributor.authorMerle, Nicolas
dc.contributor.authorMazoyer, Etienne
dc.contributor.authorSzeto, Kai C.
dc.contributor.authorRouge, Pascal
dc.contributor.authorde Mallmann, Aimery
dc.contributor.authorBerrier, Elise
dc.contributor.authorDelevoye, Laurent
dc.contributor.authorGauvin, Régis M.
dc.contributor.authorNicholas, Christopher P.
dc.contributor.authorBasset, Jean-Marie
dc.contributor.authorTaoufik, Mostafa
dc.date.accessioned2018-05-24T10:35:28Z
dc.date.available2018-05-24T10:35:28Z
dc.date.issued2018-05-22
dc.identifier.citationMerle N, Mazoyer E, Szeto KC, Rouge P, de Mallmann A, et al. (2018) Synthesis of an oxo trialkyl tungsten fluoride complex and its dual reactivity with silica dehydroxylated at high temperature. Journal of Organometallic Chemistry. Available: http://dx.doi.org/10.1016/j.jorganchem.2018.05.016.
dc.identifier.issn0022-328X
dc.identifier.doi10.1016/j.jorganchem.2018.05.016
dc.identifier.urihttp://hdl.handle.net/10754/627952
dc.description.abstractThe novel complex W (=O)Np3F has been prepared by fluorination of the corresponding chloride counterpart with AgBF4. The reactivity of this complex with silica dehydroxylated at 700 °C afforded a well-defined silica supported monopodal tungsten oxo trialkyl surface species (≡SiO)W (=O)Np3. The reaction proceeds both through silanolysis of the W-F bond and opening of a siloxane bridge, with formation of a Si-F fragment, thanks to the affinity of silicon for fluoride. The resulting surface species was characterized by elemental analysis, DRIFT, solid state NMR and EXAFS spectroscopy. This material presenting fluorine on its surface shows an enhanced catalytic activity in propylene self-metathesis compared to its monopodal counterpart (≡SiO)W (=O)Np3 (prepared from W (=O)Np3Cl) suggesting that the Si-F in a close vicinity to the W decreases the electron density of the W and thus increases its reactivity towards the olefinic substrate.
dc.description.sponsorshipE. Mazoyer thanks UOP for a graduate fellowship. This work was funded by the Agence Nationale de la Recherche (ANR-12-BS07-0021-01, OXOCAT). CNRS, We also thank Steven Fiddy, former scientist at the SRS of the CCLRC, in Daresbury, UK, for his help during the recording of the EXAFS data at SRS beam line 9.3 (project # AP 50049).
dc.publisherElsevier BV
dc.relation.urlhttp://www.sciencedirect.com/science/article/pii/S0022328X18303863
dc.rightsNOTICE: this is the author’s version of a work that was accepted for publication in Journal of Organometallic Chemistry. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Journal of Organometallic Chemistry, [(2018)] DOI: 10.1016/j.jorganchem.2018.05.016. © 2018. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/4.0/
dc.subjectOlefin metathesis
dc.subjectSurface chemistry
dc.subjectCatalysis
dc.subjectTungsten
dc.subjectOxo ligand
dc.subjectFluorine ligand
dc.titleSynthesis of an oxo trialkyl tungsten fluoride complex and its dual reactivity with silica dehydroxylated at high temperature
dc.typeArticle
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Division
dc.contributor.departmentChemical Science Program
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.identifier.journalJournal of Organometallic Chemistry
dc.eprint.versionPost-print
dc.contributor.institutionUniv. Lille, CNRS, Centrale Lille, ENSCL, Univ. Artois, UMR 8181 - UCCS - Unité de Catalyse et Chimie du Solide, F-59000, Lille, France
dc.contributor.institutionLaboratoire de Chimie, Catalyse, Polymères et Procédés, UMR 5265 CNRS/ESCPE-Lyon/UCBL, ESCPE Lyon, F-308, 43 Boulevard du 11 Novembre 1918, F-69616, Villeurbanne Cedex, France
dc.contributor.institutionExploratory Catalysis Research, UOP LLC, A Honeywell Company, 25 East Algonquin Road, Des Plaines, IL, 60017, USA
kaust.personBasset, Jean-Marie


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NOTICE: this is the author’s version of a work that was accepted for publication in Journal of Organometallic Chemistry. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Journal of Organometallic Chemistry, [(2018)] DOI: 10.1016/j.jorganchem.2018.05.016. © 2018. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/
Except where otherwise noted, this item's license is described as NOTICE: this is the author’s version of a work that was accepted for publication in Journal of Organometallic Chemistry. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Journal of Organometallic Chemistry, [(2018)] DOI: 10.1016/j.jorganchem.2018.05.016. © 2018. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/