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dc.contributor.authorWerghi, Baraa
dc.contributor.authorBendjeriou-Sedjerari, Anissa
dc.contributor.authorJedidi, Abdesslem
dc.contributor.authorMorlanes, Natalia Sanchez
dc.contributor.authorAbou-Hamad, Edy
dc.contributor.authorBhatte, Kushal Deepak
dc.contributor.authorGuan, Erjia
dc.contributor.authorMa, Tao
dc.contributor.authorAguilar-Tapia, Antonio
dc.contributor.authorOuld-Chikh, Samy
dc.contributor.authorCavallo, Luigi
dc.contributor.authorGates, Bruce C.
dc.contributor.authorBasset, Jean-Marie
dc.date.accessioned2019-03-14T14:12:21Z
dc.date.available2019-03-14T14:12:21Z
dc.date.issued2018-11-07
dc.identifier.citationWerghi B, Bendjeriou-Sedjerari A, Jedidi A, Morlanes N, Abou-Hamad E, et al. (2018) Tungsten Catalyst Incorporating a Well-Defined Tetracoordinated Aluminum Surface Ligand for Selective Metathesis of Propane, [(≡Si−O−Si≡)(≡Si−O−)2 Al−O−W(≡Ct Bu) (H)2 ]. ChemCatChem 11: 614–620. Available: http://dx.doi.org/10.1002/cctc.201801779.
dc.identifier.issn1867-3880
dc.identifier.doi10.1002/cctc.201801779
dc.identifier.urihttp://hdl.handle.net/10754/631591
dc.description.abstractA well-defined aluminium-bound hydroxyl group on the surface of mesoporous SBA-15, [(≡Si−O−Si≡) (≡Si−O) Al−OH], 3 was obtained by reacting di-isopropyl aluminium hydride with SBA-15 treated at 700 °C. The resulting surface [(≡Si−O−Si≡) (≡Si−O) Al (isobutyl) fragment undergoes β-H elimination at 400 °C leading to [(≡Si−O−Si≡)(≡Si−O−)Al−O) Al−H]. Further oxidation of this Al-hydride with NO leads to 3. This acidic support was used to create a well-defined surface organo-tungsten fragment [(≡Si−O−Si≡)(≡Si−O−)Al−O−W(≡CtBu)(CHtBu)] by reacting 3 with W(≡C-tBu)(CH-tBu). A further reaction with hydrogen under mild conditions afforded the tungsten carbyne bis-hydride [(≡Si−O−Si≡)(≡Si−O−)Al−O−W(H)(≡C-tBu)]. The performance of each of the W-supported catalysts was assessed for propane metathesis in a flow reactor at 150 °C. [(≡Si−O−Si≡)(≡Si−O−) Al−O−W(≡CtBu)(H)] was found to be a single-site catalyst, giving the highest turnover number (TON=800) and the highest reported selectivity for butane (45 %) vs. ethane (32 %) known for oxide-supported tungsten complex catalysts (with the supports being silica, silica-alumina, and alumina). The results demonstrate that modification of the oxide ligands on silica via the creation of Al Lewis acid center as an anchoring site for organometallic complexes opens up new catalytic properties, markedly enhancing the catalytic performance of supported organo-tungsten species.
dc.description.sponsorshipThe research was supported by the King Abdullah University of Science and Technology and by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Grant DE-FG02-04ER15513. We acknowledge the European Synchrotron Radiation Facility for providing synchrotron radiation facilities. L.C. and A. J. are grateful to the KAUST Supercomputing Laboratory for the resources. A. J. thank High-Performance Computing Center (AZIZ supercomputer) for the support.
dc.publisherWiley
dc.relation.urlhttps://onlinelibrary.wiley.com/doi/full/10.1002/cctc.201801779
dc.subjectLewis acidity
dc.subjectPropane metathesis
dc.subjectSBA-15
dc.subjectSurface organometallic chemistry (SOMC)
dc.subjecttetracoordinated aluminum
dc.titleTungsten Catalyst Incorporating a Well-Defined Tetracoordinated Aluminum Surface Ligand for Selective Metathesis of Propane, [(≡Si−O−Si≡)(≡Si−O−)2 Al−O−W(≡Ct Bu) (H)2 ]
dc.typeArticle
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Division
dc.contributor.departmentChemical Science Program
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentImaging and Characterization Core Lab
dc.contributor.departmentUniversity of Science and Technology 4700 King Abdullah; Thuwal 23955-6900 Kingdom of Saudi Arabia
dc.contributor.departmentKing Abdullah University of Science and Technology ( KAUST) Core Labs; Thuwal 23955-6900 Kingdom of Saudi Arabia
dc.identifier.journalChemCatChem
dc.contributor.institutionDepartment of Chemistry Faculty of Science; King Abdulaziz University (KAU); Jeddah 21589 Kingdom of Saudi Arabia
dc.contributor.institutionDepartment of Materials Science and Engineering; University of California; Davis CA 95616 USA
dc.contributor.institutionDepartment of Chemical Engineering; University of California; Davis CA 95616 USA
dc.contributor.institutionInstitut Néel UPR 2940 CNRS; Université Grenoble Alpes; Grenoble F-38000 France
kaust.personWerghi, Baraa
kaust.personBendjeriou-Sedjerari, Anissa
kaust.personMorlanes, Natalia Sanchez
kaust.personAbou-Hamad, Edy
kaust.personBhatte, Kushal Deepak
kaust.personOuld-Chikh, Samy
kaust.personCavallo, Luigi
kaust.personBasset, Jean-Marie


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