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dc.contributor.authorWerghi, Baraa
dc.contributor.authorPump, Eva
dc.contributor.authorTretiakov, Mykyta
dc.contributor.authorAbou-Hamad, Edy
dc.contributor.authorGurinov, Andrei
dc.contributor.authorDoggali, Pradeep
dc.contributor.authorAnjum, Dalaver H.
dc.contributor.authorCavallo, Luigi
dc.contributor.authorBendjeriou-Sedjerari, Anissa
dc.contributor.authorBasset, Jean-Marie
dc.date.accessioned2018-04-16T11:27:42Z
dc.date.available2018-04-16T11:27:42Z
dc.date.issued2018
dc.identifier.citationWerghi B, Pump E, Tretiakov M, Abou-Hamad E, Gurinov A, et al. (2018) Exploiting the interactions between the ruthenium Hoveyda–Grubbs catalyst and Al-modified mesoporous silica: the case of SBA15 vs. KCC-1. Chemical Science 9: 3531–3537. Available: http://dx.doi.org/10.1039/c7sc05200f.
dc.identifier.issn2041-6520
dc.identifier.issn2041-6539
dc.identifier.doi10.1039/c7sc05200f
dc.identifier.urihttp://hdl.handle.net/10754/627503
dc.description.abstractImmobilization of the 2 generation Hoveyda-Grubbs catalyst HG-II onto well-ordered 2D hexagonal (SBA15) and 3D fibrous (KCC-1) mesostructured silica, which contained tetra-coordinated Al, has been investigated through the Surface Organometallic Chemistry (SOMC) methodology. The main interest of this study lies in the peculiarity of the silica supports, which display a well-defined tetrahedral aluminum hydride site displaying a strong Lewis acid character, [(Si-O-Si)(Si-O-)Al-H]. The resulting supported Hoveyda-Grubbs catalysts have been fully characterized by advanced solid state characterization techniques (FT-IR, H and C solid state NMR, DNP-SENS, EF-TEM...). Together with DFT calculations, the immobilization of HG-II does not occur through the formation of a covalent bond between the complex and the Al-modified mesoporous silica as expected, but through an Al⋯Cl-[Ru]-coordination. It is not surprising that in functionalized olefin metathesis of diethyldiallyl malonate, DEDAM (liquid phase), leaching of the catalyst is observed which is not the case in non-functionalized olefin metathesis of propene (gas phase). Besides, the results obtained in propene metathesis with HG-II immobilized either on SBA15 (d = 6 nm) or KCC-1 (d = 4 or 8 nm) highlight the importance of the accessibility of the catalytic site. Therefore, we demonstrate that KCC-1 is a promising and suitable 3D mesoporous support to overcome the diffusion of reactants into the porous network of heterogeneous catalysts.
dc.description.sponsorshipThe research reported in this publication was supported by funding from King Abdullah University of Science and Technology (KAUST). The authors are grateful to the KAUST Supercomputing Laboratory (KSL) for the resources provided.
dc.publisherRoyal Society of Chemistry (RSC)
dc.relation.urlhttp://pubs.rsc.org/en/Content/ArticleLanding/2018/SC/C7SC05200F#!divAbstract
dc.rightsThis article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
dc.rights.urihttp://creativecommons.org/licenses/by/3.0/
dc.titleExploiting the interactions between the ruthenium Hoveyda–Grubbs catalyst and Al-modified mesoporous silica: the case of SBA15 vs. KCC-1
dc.typeArticle
dc.contributor.departmentChemical Science Program
dc.contributor.departmentCore Labs
dc.contributor.departmentElectron Microscopy
dc.contributor.departmentImaging and Characterization Core Lab
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentNMR
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalChemical Science
dc.eprint.versionPublisher's Version/PDF
kaust.personWerghi, Baraa
kaust.personPump, Eva
kaust.personTretiakov, Mykyta
kaust.personAbou-Hamad, Edy
kaust.personGurinov, Andrei
kaust.personDoggali, Pradeep
kaust.personAnjum, Dalaver H.
kaust.personCavallo, Luigi
kaust.personBendjeriou-Sedjerari, Anissa
kaust.personBasset, Jean-Marie
refterms.dateFOA2018-06-14T04:19:17Z


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