Synergy between Two Metal Catalysts: A Highly Active Silica Supported Bimetallic W/Zr Catalyst for Metathesis of n-Decane

Handle URI:
http://hdl.handle.net/10754/613000
Title:
Synergy between Two Metal Catalysts: A Highly Active Silica Supported Bimetallic W/Zr Catalyst for Metathesis of n-Decane
Authors:
Samantaray, Manoja; Dey, Raju ( 0000-0001-6271-8518 ) ; Kavitake, Santosh Giridhar; Abou-Hamad, Edy; Bendjeriou-Sedjerari, Anissa; Hamieh, Ali Imad Ali ( 0000-0002-5218-3617 ) ; Basset, Jean-Marie ( 0000-0003-3166-8882 )
Abstract:
A well-defined, silica supported, bimetallic precatalyst [≡Si-O-W(Me)5 ≡Si-O-Zr(Np)3](4) has been synthesized for the first time via successively grafting two organometallic complexes [W(CH3)6 (1) followed by ZrNp4 (2)] on a single silica support. Surprisingly, multiple quantum NMR characterization demonstrates that W and Zr species are in close proximity to each other. Hydrogenation of this bimetallic catalyst at room temperature showed the easy formation of Zirconium hydride, probably facilitated by tungsten hydride which was formed at this temperature. This bimetallic W/Zr hydride precatalyst proved to be more efficient (TON: 1436) than the monometallic W hydride (TON: 650) in metathesis of n-decane at 150 0C. This synergy between Zr and W suggests that the slow step of alkane metathesis is the C-H bond activation which occurs on Zr. The produced olefin resulting from a ß–H elimination undergoes easy metathesis on W.
KAUST Department:
KAUST Catalysis Center (KCC)
Citation:
Synergy between Two Metal Catalysts: A Highly Active Silica Supported Bimetallic W/Zr Catalyst for Metathesis of n-Decane 2016 Journal of the American Chemical Society
Publisher:
American Chemical Society (ACS)
Journal:
Journal of the American Chemical Society
Issue Date:
1-Jun-2016
DOI:
10.1021/jacs.6b04307
Type:
Article
ISSN:
0002-7863; 1520-5126
Sponsors:
The authors acknowledge the KAUST Nuclear Magnetic Resonance Core Lab and analytical core lab (ACL) for the analysis of the sample. This publication is based upon work supported by the King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR).
Additional Links:
http://pubs.acs.org/doi/abs/10.1021/jacs.6b04307
Appears in Collections:
Articles

Full metadata record

DC FieldValue Language
dc.contributor.authorSamantaray, Manojaen
dc.contributor.authorDey, Rajuen
dc.contributor.authorKavitake, Santosh Giridharen
dc.contributor.authorAbou-Hamad, Edyen
dc.contributor.authorBendjeriou-Sedjerari, Anissaen
dc.contributor.authorHamieh, Ali Imad Alien
dc.contributor.authorBasset, Jean-Marieen
dc.date.accessioned2016-06-14T08:25:28Z-
dc.date.available2016-06-14T08:25:28Z-
dc.date.issued2016-06-01-
dc.identifier.citationSynergy between Two Metal Catalysts: A Highly Active Silica Supported Bimetallic W/Zr Catalyst for Metathesis of n-Decane 2016 Journal of the American Chemical Societyen
dc.identifier.issn0002-7863-
dc.identifier.issn1520-5126-
dc.identifier.doi10.1021/jacs.6b04307-
dc.identifier.urihttp://hdl.handle.net/10754/613000-
dc.description.abstractA well-defined, silica supported, bimetallic precatalyst [≡Si-O-W(Me)5 ≡Si-O-Zr(Np)3](4) has been synthesized for the first time via successively grafting two organometallic complexes [W(CH3)6 (1) followed by ZrNp4 (2)] on a single silica support. Surprisingly, multiple quantum NMR characterization demonstrates that W and Zr species are in close proximity to each other. Hydrogenation of this bimetallic catalyst at room temperature showed the easy formation of Zirconium hydride, probably facilitated by tungsten hydride which was formed at this temperature. This bimetallic W/Zr hydride precatalyst proved to be more efficient (TON: 1436) than the monometallic W hydride (TON: 650) in metathesis of n-decane at 150 0C. This synergy between Zr and W suggests that the slow step of alkane metathesis is the C-H bond activation which occurs on Zr. The produced olefin resulting from a ß–H elimination undergoes easy metathesis on W.en
dc.description.sponsorshipThe authors acknowledge the KAUST Nuclear Magnetic Resonance Core Lab and analytical core lab (ACL) for the analysis of the sample. This publication is based upon work supported by the King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR).en
dc.language.isoenen
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://pubs.acs.org/doi/abs/10.1021/jacs.6b04307en
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/jacs.6b04307.en
dc.titleSynergy between Two Metal Catalysts: A Highly Active Silica Supported Bimetallic W/Zr Catalyst for Metathesis of n-Decaneen
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.identifier.journalJournal of the American Chemical Societyen
dc.eprint.versionPost-printen
dc.contributor.affiliationKing Abdullah University of Science and Technology (KAUST)en
kaust.authorSamantaray, Manojaen
kaust.authorDey, Rajuen
kaust.authorKavitake, Santosh Giridharen
kaust.authorAbou-Hamad, Edyen
kaust.authorBendjeriou-Sedjerari, Anissaen
kaust.authorHamieh, Ali Imad Alien
kaust.authorBasset, Jean-Marieen
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