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Pyrazole or tris(pyrazolyl)ethanol oxo-vanadium(IV) complexes as homogeneous or supported catalysts for oxidation of cyclohexane under mild conditions

2013-02Journal article Open access
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dc.contributor.authorSilva, Telma F. S.
dc.contributor.authorMac Leod, Tatiana C. O.
dc.contributor.authorMartins, Luisa
dc.contributor.authorGuedes Da Silva, M. Fátima C.
dc.contributor.authorSchiavon, Marco A.
dc.contributor.authorPombeiro, Armando
dc.date.accessioned2013-10-25T14:40:35Z
dc.date.available2013-10-25T14:40:35Z
dc.date.issued2013-02
dc.description.abstractThe oxovanadium(IV) complexes [VO(acac)(2)(Hpz)].HC(pz)(3) 1.HC(pz)(3) (acac= acetylacetonate, Hpz = pyrazole, pz = pyrazoly1) and [VOCl2{HOCH2C(pz)(3)}] 2 were obtained from reaction of [VO(acac)(2)] with hydrotris(1-pyrazolyl)methane or of VCl(3)with 2,2,2-tris(1-pyrazolyl)ethanol. The compounds were characterized by elemental analysis, IR, Far-IR and EPR spectroscopies, FAB or ESI mass-spectrometry and, for 1, by single crystal X-ray diffraction analysis. 1 and 2 exhibit catalytic activity for the oxidation of cyclohexane to the cyclohexanol and cyclohexanone mixture in homogeneous system (TONS up to 1100) under mild conditions (NCMe, 24h, room temperature) using benzoyl peroxide (BPO), tert-butyl hydroperoxide (TBHP), m-chloroperoxybenzoic acid (mCPBA), hydrogen peroxide or the urea-hydrogen peroxide adduct (UHP) as oxidants. 1 and 2 were also immobilized on a polydimethylsiloxane membrane (1-PDMS or 2-PDMS) and the systems acted as supported catalysts for the cyclohexane oxidation using the above oxidants (TONs up to 620). The best results were obtained with mCPBA or BP0 as oxidant. The effects of various parameters, such as the amount of catalyst, nitric acid, reaction time, type of oxidant and oxidant-to-catalyst molar ratio, were investigated, for both homogeneous and supported systems. (C) 2012 Elsevier B.V. All rights reserved.por
dc.identifier.citationSILVA, Telma F. S.; MAC LEOD, Tatiana C. O.; MARTINS, Luisa M. D. R. S.; SILVA, M. Fatima C. Guedes da; SCHIAVON, Marco A.; POMBEIRO, Armando J. L. - Pyrazole or tris(pyrazolyl)ethanol oxo-vanadium(IV) complexes as homogeneous or supported catalysts for oxidation of cyclohexane under mild conditions. Journal of Molecular Catalysis A-Chemical. ISSN 1381-1169. Vol. 367 (2013), p. 52-60.por
dc.identifier.issn1381-1169
dc.identifier.other10.1016/j.molcata.2012.10.024
dc.identifier.urihttp://hdl.handle.net/10400.21/2785
dc.language.isoengpor
dc.peerreviewedyespor
dc.publisherElsevier Science BVpor
dc.subjectCyclohexanepor
dc.subjectC-scorpionatespor
dc.subjectVanadiumpor
dc.subjectHomogeneous catalysispor
dc.subjectOxidationpor
dc.subjectCrystal structurepor
dc.subjectSupported catalysispor
dc.subjectO-2-H2O2-Vanadium Derivative-Pyrazine-2-Carboxylic Acidpor
dc.subjectModified Silica-Gelpor
dc.subjectHydrogen-Peroxidepor
dc.subjectVanadium Complexespor
dc.subjectMolecular-Oxygenpor
dc.subjectCarboxylic-Acidspor
dc.subjectHighly Efficientpor
dc.subjectAcetic-Acidpor
dc.subjectBis(Maltolato)Oxovanadium Complexespor
dc.subjectHydrocarbon Oxygenationspor
dc.titlePyrazole or tris(pyrazolyl)ethanol oxo-vanadium(IV) complexes as homogeneous or supported catalysts for oxidation of cyclohexane under mild conditionspor
dc.typejournal article
dspace.entity.typePublication
oaire.citation.conferencePlaceAmsterdampor
oaire.citation.endPage60por
oaire.citation.startPage52por
oaire.citation.titleJournal of Molecular Catalysis A-Chemicalpor
oaire.citation.volume367por
person.familyNameMartins
person.familyNameGuedes da Silva
person.familyNamePombeiro
person.givenNameLuisa
person.givenNameM. Fátima C.
person.givenNameArmando
person.identifier637885
person.identifier789079
person.identifier.ciencia-idE218-E297-A4EA
person.identifier.ciencia-id7619-8E8E-979A
person.identifier.ciencia-id8311-38FA-CEFB
person.identifier.orcid0000-0002-5403-9352
person.identifier.orcid0000-0003-4836-2409
person.identifier.orcid0000-0001-8323-888X
person.identifier.ridG-6210-2011
person.identifier.ridH-8274-2012
person.identifier.ridI-5945-2012
person.identifier.scopus-author-id8650947800
person.identifier.scopus-author-id6701761571
person.identifier.scopus-author-id7006067269
rcaap.rightsrestrictedAccesspor
rcaap.typearticlepor
relation.isAuthorOfPublication8ed70b09-b4d3-4a5d-9f75-12b13a332204
relation.isAuthorOfPublication18e14ad3-9937-46d0-83b2-36fab224c1c0
relation.isAuthorOfPublication6d18ff2e-5c33-4010-b1e7-964c72349813
relation.isAuthorOfPublication.latestForDiscovery6d18ff2e-5c33-4010-b1e7-964c72349813

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