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dc.contributor.authorKermagoret, Anthony
dc.contributor.authorKerber, Rachel Nathaniel
dc.contributor.authorConley, Matthew P.
dc.contributor.authorCallens, Emmanuel
dc.contributor.authorFlorian, Pierre
dc.contributor.authorMassiot, Dominique
dc.contributor.authorDelbecq, Françoise
dc.contributor.authorRozanska, Xavier
dc.contributor.authorCopéret, Christophe
dc.contributor.authorSautet, Philippe
dc.date.accessioned2016-02-25T12:56:31Z
dc.date.available2016-02-25T12:56:31Z
dc.date.issued2014-05
dc.identifier.citationKermagoret A, Kerber RN, Conley MP, Callens E, Florian P, et al. (2014) Chlorodiethylaluminum supported on silica: A dinuclear aluminum surface species with bridging μ2-Cl-ligand as a highly efficient co-catalyst for the Ni-catalyzed dimerization of ethene. Journal of Catalysis 313: 46–54. Available: http://dx.doi.org/10.1016/j.jcat.2014.02.006.
dc.identifier.issn0021-9517
dc.identifier.doi10.1016/j.jcat.2014.02.006
dc.identifier.urihttp://hdl.handle.net/10754/597776
dc.description.abstractSilica-supported chloro alkyl aluminum co-catalysts (DEAC@support) were prepared via Surface Organometallic Chemistry by contacting diethylaluminum chloride (DEAC) and high specific surface silica materials, i.e. SBA-15, MCM-41, and Aerosil SiO2. Such systems efficiently activate NiCl 2(PBu3)2 for catalytic ethene dimerization, with turnover frequency (TOF) reaching up to 498,000 molC2H4/ (molNi h) for DEAC@MCM-41. A detailed analysis of the DEAC@SBA-15 co-catalyst structure by solid-state aluminum-27 NMR at high-field (17.6 T and 20.0 T) and ultrafast spinning rates allows to detect six sites, characterized by a distribution of quadrupolar interaction principal values CQ and isotropic chemical shifts δiso. Identification of the corresponding Al-grafted structures was possible by comparison of the experimental NMR signatures with these calculated by DFT on a wide range of models for the aluminum species (mono- versus di-nuclear, mono- versus bis-grafted with bridging Cl or ethyl). Most of the sites were identified as dinuclear species with retention of the structure of DEAC, namely with the presence of μ2-Cl-ligands between two aluminum, and this probably explains the high catalytic performance of this silica-supported co-catalysts. © 2014 Elsevier Inc. All rights reserved.
dc.description.sponsorshipThis publication is based on work supported by Award No.UK-00017, made by King Abdullah University of Science and Technology (KAUST), and by the TGE RMN THC Fr3050. The authors thank the PSMN at ENS of Lyon for the attribution of CPU time.
dc.publisherElsevier BV
dc.subjectAluminum-27 solid state NMR
dc.subjectChloroalkylaluminum
dc.subjectCo-catalysts
dc.subjectDFT calculations
dc.subjectDimerization of ethene
dc.subjectHeterogeneous catalysts
dc.subjectNickel
dc.subjectOligomerization
dc.subjectSilica supported
dc.titleChlorodiethylaluminum supported on silica: A dinuclear aluminum surface species with bridging μ2-Cl-ligand as a highly efficient co-catalyst for the Ni-catalyzed dimerization of ethene
dc.typeArticle
dc.identifier.journalJournal of Catalysis
dc.contributor.institutionUniversite Claude Bernard Lyon 1, Villeurbanne, France
dc.contributor.institutionUniversite de Lyon, Lyon, France
dc.contributor.institutionEidgenossische Technische Hochschule Zurich, Zurich, Switzerland
dc.contributor.institutionUniversite d'Orleans, Orleans, France
kaust.grant.numberUK-00017


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