WMe6 tamed by silica: Si-O-WMe5 as an efficient, well-defined species for alkane metathesis, leading to the observation of a supported W-methyl/methylidyne species

Handle URI:
http://hdl.handle.net/10754/563348
Title:
WMe6 tamed by silica: Si-O-WMe5 as an efficient, well-defined species for alkane metathesis, leading to the observation of a supported W-methyl/methylidyne species
Authors:
Samantaray, Manoja; Callens, Emmanuel; Abou-Hamad, Edy; Rossini, Aaron J.; Widdifield, Cory M.; Dey, Raju ( 0000-0001-6271-8518 ) ; Emsley, Lyndon; Basset, Jean-Marie ( 0000-0003-3166-8882 )
Abstract:
The synthesis and full characterization of a well-defined silica-supported ≡Si-O-W(Me)5 species is reported. Under an inert atmosphere, it is a stable material at moderate temperature, whereas the homoleptic parent complex decomposes above -20 °C, demonstrating the stabilizing effect of immobilization of the molecular complex. Above 70 °C the grafted complex converts into the two methylidyne surface complexes [(≡SiO-)W(≡CH) Me2] and [(≡SiO-)2W(≡CH)Me]. All of these silica-supported complexes are active precursors for propane metathesis reactions. © 2013 American Chemical Society.
KAUST Department:
KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division; Chemical Science Program
Publisher:
American Chemical Society (ACS)
Journal:
Journal of the American Chemical Society
Issue Date:
22-Jan-2014
DOI:
10.1021/ja410747g
Type:
Article
ISSN:
00027863
Sponsors:
The authors acknowledge the KAUST Nuclear Magnetic Resonance Core Lab and technical assistance of Dr. Kazuo Yamauchi. The authors also thank Dr. Nassima Riache for her fruitful discussions. Mr. Benoit Vincenti is thanked for inert-atmosphere sample preparation prior to solid-state NMR experiments upon 2. A.J.R. acknowledges support from an EU Marie-Curie IIF fellowship (PIIF-GA-2010-274574). C.M.W. acknowledges the Natural Sciences and Engineering Council of Canada (NSERC) for a postdoctoral fellowship. Computational resources for DFT calculations were provided by the Pole Scientifique de Modelisation Numerique (PSMN). This work was supported by funds from King Abdullah University of Science and Technology.
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.authorSamantaray, Manojaen
dc.contributor.authorCallens, Emmanuelen
dc.contributor.authorAbou-Hamad, Edyen
dc.contributor.authorRossini, Aaron J.en
dc.contributor.authorWiddifield, Cory M.en
dc.contributor.authorDey, Rajuen
dc.contributor.authorEmsley, Lyndonen
dc.contributor.authorBasset, Jean-Marieen
dc.date.accessioned2015-08-03T11:46:20Zen
dc.date.available2015-08-03T11:46:20Zen
dc.date.issued2014-01-22en
dc.identifier.issn00027863en
dc.identifier.doi10.1021/ja410747gen
dc.identifier.urihttp://hdl.handle.net/10754/563348en
dc.description.abstractThe synthesis and full characterization of a well-defined silica-supported ≡Si-O-W(Me)5 species is reported. Under an inert atmosphere, it is a stable material at moderate temperature, whereas the homoleptic parent complex decomposes above -20 °C, demonstrating the stabilizing effect of immobilization of the molecular complex. Above 70 °C the grafted complex converts into the two methylidyne surface complexes [(≡SiO-)W(≡CH) Me2] and [(≡SiO-)2W(≡CH)Me]. All of these silica-supported complexes are active precursors for propane metathesis reactions. © 2013 American Chemical Society.en
dc.description.sponsorshipThe authors acknowledge the KAUST Nuclear Magnetic Resonance Core Lab and technical assistance of Dr. Kazuo Yamauchi. The authors also thank Dr. Nassima Riache for her fruitful discussions. Mr. Benoit Vincenti is thanked for inert-atmosphere sample preparation prior to solid-state NMR experiments upon 2. A.J.R. acknowledges support from an EU Marie-Curie IIF fellowship (PIIF-GA-2010-274574). C.M.W. acknowledges the Natural Sciences and Engineering Council of Canada (NSERC) for a postdoctoral fellowship. Computational resources for DFT calculations were provided by the Pole Scientifique de Modelisation Numerique (PSMN). This work was supported by funds from King Abdullah University of Science and Technology.en
dc.publisherAmerican Chemical Society (ACS)en
dc.titleWMe6 tamed by silica: Si-O-WMe5 as an efficient, well-defined species for alkane metathesis, leading to the observation of a supported W-methyl/methylidyne speciesen
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.identifier.journalJournal of the American Chemical Societyen
dc.contributor.institutionInstitut de Sciences Analytiques (CNRS, ENS-Lyon, UCB Lyon 1), Université de Lyon, Centre de RMN À Très Hauts Champs, 5 rue de la Doua, 69100 Villeurbanne, Franceen
kaust.authorSamantaray, Manojaen
kaust.authorCallens, Emmanuelen
kaust.authorAbou-Hamad, Edyen
kaust.authorDey, Rajuen
kaust.authorBasset, Jean-Marieen
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