A Silica-Supported Monoalkylated Tungsten Dioxo Complex Catalyst for Olefin Metathesis

Handle URI:
http://hdl.handle.net/10754/627619
Title:
A Silica-Supported Monoalkylated Tungsten Dioxo Complex Catalyst for Olefin Metathesis
Authors:
Maity, Niladri ( 0000-0002-0588-7849 ) ; Barman, Samir; Minenkov, Yury; Ould-Chikh, Samy ( 0000-0002-3486-0944 ) ; Abou-Hamad, Edy; Ma, Tao; Qureshi, Ziyauddin ( 0000-0002-1246-0827 ) ; Cavallo, Luigi ( 0000-0002-1398-338X ) ; D'Elia, Valerio; Gates, Bruce C.; Basset, Jean-Marie ( 0000-0003-3166-8882 )
Abstract:
A well-defined silica-supported monoalkylated tungsten dioxo complex [(Si-O-)W(=O)(CH-Bu)] was prepared by treatment of highly dehydroxylated silica (SiO: silica treated at 700 °C under high vacuum) with an ionic precursor complex [NEt][W(=O)(CH-Bu)]. The identity of the resulting neutral monoalkylated tungsten dioxo surface complex was established by means of elemental microanalysis and spectroscopic studies (IR, solid-state NMR, Raman, and X-ray absorption spectroscopies). The supported tungsten complex was found to act as a precatalyst for the self-metathesis of 1-octene in a batch reactor. The mechanistic implications of this reaction are discussed with the support of DFT calculations highlighting the potential occurrence of thus-far unexplored mechanistic pathways.
KAUST Department:
KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division; Imaging and Characterization Core Lab; Chemical Science Program
Citation:
Maity N, Barman S, Minenkov Y, Ould-Chikh S, Abou-Hamad E, et al. (2018) A Silica-Supported Monoalkylated Tungsten Dioxo Complex Catalyst for Olefin Metathesis. ACS Catalysis 8: 2715–2729. Available: http://dx.doi.org/10.1021/acscatal.7b04304.
Publisher:
American Chemical Society (ACS)
Journal:
ACS Catalysis
Issue Date:
15-Feb-2018
DOI:
10.1021/acscatal.7b04304
Type:
Article
ISSN:
2155-5435; 2155-5435
Sponsors:
The research was supported by the King Abdullah University of Science and Technology (KAUST). The authors acknowledge Dr. Christian G. Canlas and Erjia Guan for their assistance. The work at the University of California was supported by the U.S. Department of Energy (DOE, Basic Energy Sciences DE-FG02-04ER15513). We acknowledge the European Synchrotron Radiation Facility for provision of synchrotron radiation facilities, and we would like to thank Antonio Aguilar for assistance in using beamline BM30 B.
Additional Links:
https://pubs.acs.org/doi/full/10.1021/acscatal.7b04304
Appears in Collections:
Articles; Advanced Nanofabrication, Imaging and Characterization Core Lab; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorMaity, Niladrien
dc.contributor.authorBarman, Samiren
dc.contributor.authorMinenkov, Yuryen
dc.contributor.authorOuld-Chikh, Samyen
dc.contributor.authorAbou-Hamad, Edyen
dc.contributor.authorMa, Taoen
dc.contributor.authorQureshi, Ziyauddinen
dc.contributor.authorCavallo, Luigien
dc.contributor.authorD'Elia, Valerioen
dc.contributor.authorGates, Bruce C.en
dc.contributor.authorBasset, Jean-Marieen
dc.date.accessioned2018-04-24T07:48:27Z-
dc.date.available2018-04-24T07:48:27Z-
dc.date.issued2018-02-15en
dc.identifier.citationMaity N, Barman S, Minenkov Y, Ould-Chikh S, Abou-Hamad E, et al. (2018) A Silica-Supported Monoalkylated Tungsten Dioxo Complex Catalyst for Olefin Metathesis. ACS Catalysis 8: 2715–2729. Available: http://dx.doi.org/10.1021/acscatal.7b04304.en
dc.identifier.issn2155-5435en
dc.identifier.issn2155-5435en
dc.identifier.doi10.1021/acscatal.7b04304en
dc.identifier.urihttp://hdl.handle.net/10754/627619-
dc.description.abstractA well-defined silica-supported monoalkylated tungsten dioxo complex [(Si-O-)W(=O)(CH-Bu)] was prepared by treatment of highly dehydroxylated silica (SiO: silica treated at 700 °C under high vacuum) with an ionic precursor complex [NEt][W(=O)(CH-Bu)]. The identity of the resulting neutral monoalkylated tungsten dioxo surface complex was established by means of elemental microanalysis and spectroscopic studies (IR, solid-state NMR, Raman, and X-ray absorption spectroscopies). The supported tungsten complex was found to act as a precatalyst for the self-metathesis of 1-octene in a batch reactor. The mechanistic implications of this reaction are discussed with the support of DFT calculations highlighting the potential occurrence of thus-far unexplored mechanistic pathways.en
dc.description.sponsorshipThe research was supported by the King Abdullah University of Science and Technology (KAUST). The authors acknowledge Dr. Christian G. Canlas and Erjia Guan for their assistance. The work at the University of California was supported by the U.S. Department of Energy (DOE, Basic Energy Sciences DE-FG02-04ER15513). We acknowledge the European Synchrotron Radiation Facility for provision of synchrotron radiation facilities, and we would like to thank Antonio Aguilar for assistance in using beamline BM30 B.en
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttps://pubs.acs.org/doi/full/10.1021/acscatal.7b04304en
dc.subjectmechanistic studyen
dc.subjectmetallacyclobutane intermediateen
dc.subjectOlefin metathesisen
dc.subjecttungsten alkylideneen
dc.subjecttungsten dioxo complexen
dc.titleA Silica-Supported Monoalkylated Tungsten Dioxo Complex Catalyst for Olefin Metathesisen
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentImaging and Characterization Core Laben
dc.contributor.departmentChemical Science Programen
dc.identifier.journalACS Catalysisen
dc.contributor.institutionDepartment of Chemical Engineering, University of California at Davis, Davis, CA, 95616, , United Statesen
dc.contributor.institutionCenter of Research Excellence in Petroleum Refining and Petrochemicals, King Fahd University of Petroleum and Minerals, Dhahran, 31261, , Saudi Arabiaen
dc.contributor.institutionDepartment of Materials Science and Engineering, School of Molecular Science and Engineering, Vidyasirimedhi Institute of Science and Technology (VISTEC), Payupnai, WangChan Rayong, 21210, , Thailanden
kaust.authorMaity, Niladrien
kaust.authorBarman, Samiren
kaust.authorMinenkov, Yuryen
kaust.authorOuld-Chikh, Samyen
kaust.authorAbou-Hamad, Edyen
kaust.authorQureshi, Ziyauddinen
kaust.authorCavallo, Luigien
kaust.authorD'Elia, Valerioen
kaust.authorBasset, Jean-Marieen
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