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Tris(pyrazolyl)methane molybdenum tricarbonyl complexes as catalyst precursors for olefin epoxidation

2013-04Journal article Restricted access
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dc.contributor.authorGomes, Ana C.
dc.contributor.authorNeves, Patrícia
dc.contributor.authorFigueiredo, Sónia
dc.contributor.authorFernandes, José A.
dc.contributor.authorValente, Anabela A.
dc.contributor.authorAlmeida Paz, Filipe A.
dc.contributor.authorPillinger, Martyn
dc.contributor.authorLopes, Andre D.
dc.contributor.authorGonçalves, Isabel S.
dc.date.accessioned2016-04-08T14:28:20Z
dc.date.available2016-04-08T14:28:20Z
dc.date.issued2013-04
dc.date.updated2016-03-08T15:48:05Z
dc.description.abstractThe molybdenum tricarbonyl complexes [Mo(CO)3(HC(3,5-Me2pz)3)] (1) and [Mo(CO)3(HC(pz)3)] (2)(HC(3,5-Me2pz)3 = tris(3,5-dimethyl-1-pyrazolyl)methane, HC(pz)3 = tris(1-pyrazolyl)methane) were obtained in good yields by the microwave-assisted reaction of Mo(CO)6 with the respective organic ligand. Complete oxidative decarbonylation of 1 and 2 was achieved by reaction with excess tert-butylhydroperoxide (TBHP) in 1,2-dichloroethane at 55 ◦C. For complex 1, the (2-oxo)bis[dioxomolybdenum(VI)] hexamolybdate of composition [{MoO2(HC(3,5-Me2pz)3)}2(2- O)][Mo6O19] (3) was obtained in good yield, and its structure was determined by single crystal X-ray diffraction. The compound (4) obtained by oxidative decarbonylation of 2 was not unambiguously identified, but may be chemically analogous to 3. Compounds 1–4 were examined for the first time as homogeneous (pre)catalysts for the epoxidation of olefins with TBHP, using different types of cosolvents at 55 ◦C. During the catalytic reactions 1 and 2 transform in situ into 3 and 4, respectively, and the latter two are fairly stable catalysts. Catalytic tests and characterization studies of the recovered catalysts were carried out in an attempt to understand the kinetic differences observed between the compounds prepared in situ during the catalytic reaction and those prepared prior to the catalytic reaction, from the same precursor complex.pt_PT
dc.identifier.citationGomes, A.C.; Neves, P.; Figueiredo, S.; Fernandes, J.A.; Valente, A.A.; Almeida Paz, F.A.; Pillinger, M.; Lopes, A.D.; Gonçalves, I.S.Tris(pyrazolyl)methane molybdenum tricarbonyl complexes as catalyst precursors for olefin epoxidation, Journal of Molecular Catalysis A: Chemical, 370, s/n, 64-76, 2013.pt_PT
dc.identifier.doihttp://dx.doi.org/10.1016/j.molcata.2012.12.010pt_PT
dc.identifier.issn1381-1169
dc.identifier.otherAUT: ADL01681;
dc.identifier.urihttp://hdl.handle.net/10400.1/7962
dc.language.isoengpt_PT
dc.peerreviewedyespt_PT
dc.publisherElsevierpt_PT
dc.relation.publisherversionhttp://www.sciencedirect.com/science/article/pii/S1381116912004165pt_PT
dc.subjectMolybdenumpt_PT
dc.subjectTris(pyrazolyl)methane ligandspt_PT
dc.subjectHomogeneous catalysispt_PT
dc.subjectOlefin epoxidationpt_PT
dc.subjectOxidative decarbonylationpt_PT
dc.titleTris(pyrazolyl)methane molybdenum tricarbonyl complexes as catalyst precursors for olefin epoxidationpt_PT
dc.typejournal article
dspace.entity.typePublication
oaire.awardURIinfo:eu-repo/grantAgreement/FCT/COMPETE/PEst-C%2FCTM%2FLA0011%2F2013/PT
oaire.citation.endPage74pt_PT
oaire.citation.startPage64pt_PT
oaire.citation.titleJournal of Molecular Catalysis A: Chemicalpt_PT
oaire.citation.volume370pt_PT
oaire.fundingStreamCOMPETE
person.familyNameD. Lopes
person.givenNameAndré
person.identifier2824636
person.identifier.ciencia-id351E-856A-0300
person.identifier.orcid0000-0002-9702-1216
person.identifier.ridE-2136-2012
person.identifier.scopus-author-id7201958625
project.funder.identifierhttp://doi.org/10.13039/501100001871
project.funder.nameFundação para a Ciência e a Tecnologia
rcaap.rightsrestrictedAccesspt_PT
rcaap.typearticlept_PT
relation.isAuthorOfPublicationf2f0fe56-e04d-4229-b37b-2b9f1789fe2d
relation.isAuthorOfPublication.latestForDiscoveryf2f0fe56-e04d-4229-b37b-2b9f1789fe2d
relation.isProjectOfPublicationd960b631-c7a8-4eb2-8a24-09e10fef0993
relation.isProjectOfPublication.latestForDiscoveryd960b631-c7a8-4eb2-8a24-09e10fef0993

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