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dc.contributor.authorLe Quéméner, Frédéric
dc.contributor.authorBasset, Jean-Marie
dc.contributor.authorBarman, Samir
dc.contributor.authorMerle, Nicolas
dc.contributor.authorAljuhani, Maha A.
dc.contributor.authorSamantaray, Manoja
dc.contributor.authorSaih, Youssef
dc.contributor.authorSzeto, Kai C.
dc.contributor.authorde Mallmann, Aimery
dc.contributor.authorMinenkov, Yury
dc.contributor.authorHuang, Kuo-Wei
dc.contributor.authorCavallo, Luigi
dc.contributor.authorTaoufik, Mostafa
dc.date.accessioned2018-12-31T14:05:52Z
dc.date.available2018-12-31T14:05:52Z
dc.date.issued2018-07-10
dc.identifier.citationLe Quéméner F, Barman S, Merle N, Aljuhani MA, Samantaray MK, et al. (2018) Metathetic Oxidation of 2-Butenes to Acetaldehyde by Molecular Oxygen Using the Single-Site Olefin Metathesis Catalyst (≡SiO)2Mo(═O)2. ACS Catalysis 8: 7549–7555. Available: http://dx.doi.org/10.1021/acscatal.8b01767.
dc.identifier.issn2155-5435
dc.identifier.issn2155-5435
dc.identifier.doi10.1021/acscatal.8b01767
dc.identifier.urihttp://hdl.handle.net/10754/630669
dc.description.abstractThe catalytic oxidation of cis-2-butene and propylene with molecular oxygen in the presence of a well-defined surface coordination compound, (≡SiO)2Mo(═O)2, affords acetaldehyde. Using a cis-2-butene/O2 feed at 350–400 °C, the reaction yields a conversion of approximately 10% and an acetaldehyde selectivity of approximately 70%. This performance is maintained up to an experimental time of 20 h in a continuous flow reactor. The Mo(bis-oxo) surface compound was fully characterized by multiple spectroscopic techniques as well as surface microanalysis. The results from quantum mechanics calculations indicate that the reaction proceeds via [2 + 2] cycloaddition/cycloelimination steps with the formation of metalla-oxacyclobutane intermediates, analogous to the Chauvin mechanism in olefin metathesis.
dc.description.sponsorshipThe Competitive Research Grant Program, supported by the KAUST Research Fund (project # 2174 CGR3) is gratefully acknowledged for financial support. We wish to thank Olivier Mathon for his help during the recording of the XAS spectra on BM23 beamline at ESRF (experiment code IN-986). For computer time, this study employed the resources of the KAUST Supercomputing Laboratory (KSL).
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttps://pubs.acs.org/doi/10.1021/acscatal.8b01767
dc.subjectacetaldehyde
dc.subjectDFT calculations
dc.subjectmetathetic oxidation
dc.subjectmolybdenum catalyst
dc.subjectsilica-supported catalyst
dc.subjectsurface organometallic chemistry
dc.titleMetathetic oxidation of 2-butenes to acetaldehyde by molecular oxygen using the single-site olefin metathesis catalyst (≡SiO)2Mo(=O)2
dc.typeArticle
dc.contributor.departmentChemical Science Program
dc.contributor.departmentHomogeneous Catalysis Laboratory (HCL)
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalACS Catalysis
dc.contributor.institutionLaboratoire de Chimie, Catalyse, Polymères et Procédés, UMR 5265 CNRS/ESCPE-Lyon/UCBL, ESCPE Lyon, F-308-43, Boulevard du 11 Novembre 1918, F-69616 Villeurbanne Cedex, France
dc.contributor.institutionUniversity of Lille, CNRS, Centrale Lille, ENSCL, Univ. Artois, UMR 8181, UCCS − Unité de Catalyse et Chimie du Solide, F-59000 Lille, France
dc.contributor.institutionMoscow Institute of Physics and Technology, Institutskiy Pereulok 9, Dolgoprudny, Moscow Region 141700, Russia
kaust.personBasset, Jean-Marie
kaust.personBarman, Samir
kaust.personAljuhani, Maha A.
kaust.personSamantaray, Manoja
kaust.personSaih, Youssef
kaust.personMinenkov, Yury
kaust.personHuang, Kuo-Wei
kaust.personCavallo, Luigi
kaust.grant.number2174 CGR3
dc.date.published-online2018-07-10
dc.date.published-print2018-08-03


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