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Intercalation of a molybdenum eta3-allyl dicarbonyl complex in a layered double hydroxide and catalytic performance in olefin epoxidation.

2013Journal article Restricted access
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dc.contributor.authorGomes, A.
dc.contributor.authorBruno, S.
dc.contributor.authorGamelas ou Carla A. Gamelas, Carla
dc.contributor.authorValente, A.
dc.contributor.authorAbrantes, M.
dc.contributor.authorGonçalves, I.
dc.contributor.authorRomão, C.
dc.contributor.authorPillinger, M.
dc.date.accessioned2018-03-22T14:56:32Z
dc.date.available2018-03-22T14:56:32Z
dc.date.issued2013
dc.description.abstractA Zn–Al layered double hydroxide (LDH) intercalated by [Mo(η3-C3H5)Cl(CO)2(bpdc)]2− anions (bpdc = 2,2′-bipyridine-5,5′-dicarboxylate) has been prepared by coprecipitation from aqueous solution and characterised by various techniques. The one-pot method gives rise to a highly organised intercalate with an interlayer spacing of 18.3 Å and up to six (00l) basal reflections in the powder X-ray diffraction pattern. Spectroscopic studies (FT-IR, FT-Raman, 13C CP MAS NMR and UV-Vis) confirm the presence of structurally intact [Mo(η3-C3H5)Cl(CO)2(bpdc)]2− anions. The interlayer spacing of 18.3 Å indicates that the material contains a monolayer of guest anions positioned in such a way that the bpdc ligands are arranged with their longest dimension roughly perpendicular to the hydroxide layers of the host. Thermal properties were studied by thermogravimetric analysis and differential scanning calorimetry. The intracrystalline reactivity of intercalated dicarbonyl complexes was probed by using the hybrid nanocomposite as a precatalyst in the liquid phase epoxidation of cis-cyclooctene with tert-butylhydroperoxide as oxidant. Under the reaction conditions used, oxidative decarbonylation of the guest molecules takes place (with release of CO and CO2 as confirmed by on-line gas chromatography experiments) to give intercalated molybdenum oxide/bipyridine species that selectively catalyse the epoxidation reaction. The intracrystalline oxidative decarbonylation reaction is topotactic in nature.pt_PT
dc.description.versioninfo:eu-repo/semantics/publishedVersionpt_PT
dc.identifier.citationGomes, A., Bruno, S., Gamelas, C., Valente, A., Abrantes, M., Gonçalves, I., Romão, C. & Pillinger, M. (2013). Intercalation of a molybdenum eta3-allyl dicarbonyl complex in a layered double hydroxide and catalytic performance in olefin epoxidation. Dalton Transactions, 42, pp. 8231-8240. doi: 10.1039/C3DT50132A.pt_PT
dc.identifier.doi10.1039/C3DT50132Apt_PT
dc.identifier.urihttp://hdl.handle.net/10400.26/22037
dc.language.isoengpt_PT
dc.peerreviewedyespt_PT
dc.relation2013 - Strategic Project
dc.titleIntercalation of a molybdenum eta3-allyl dicarbonyl complex in a layered double hydroxide and catalytic performance in olefin epoxidation.pt_PT
dc.typejournal article
dspace.entity.typePublication
oaire.awardTitle2013 - Strategic Project
oaire.awardURIinfo:eu-repo/grantAgreement/FCT/6820 - DCRRNI ID/PEst-C%2FCTM%2FLA0011%2F2013/PT
oaire.citation.titleDalton Transactionspt_PT
oaire.fundingStream6820 - DCRRNI ID
person.familyNameGamelas Albuquerque Pinto Reis
person.givenNameCarla Alexandra
person.identifier.ciencia-id2219-54F2-BB9D
project.funder.identifierhttp://doi.org/10.13039/501100001871
project.funder.nameFundação para a Ciência e a Tecnologia
rcaap.rightsclosedAccesspt_PT
rcaap.typearticlept_PT
relation.isAuthorOfPublicationa02aa459-55c4-4506-b8f2-5189e5c13124
relation.isAuthorOfPublication.latestForDiscoverya02aa459-55c4-4506-b8f2-5189e5c13124
relation.isProjectOfPublication10470ba4-89bc-456b-9371-4bea8ad5c178
relation.isProjectOfPublication.latestForDiscovery10470ba4-89bc-456b-9371-4bea8ad5c178

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