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Comparison of liquid-phase olefin epoxidation catalysed by dichlorobis-(dimethylformamide)dioxomolybdenum(VI) in homogeneous phase and grafted onto MCM-41

2009Journal article Restricted access
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dc.contributor.authorMonteiro, Bernardo
dc.contributor.authorBalula, Salete S.
dc.contributor.authorGago, Sandra
dc.contributor.authorGrosso, Carla
dc.contributor.authorFigueiredo, Sónia
dc.contributor.authorLopes, Andre D.
dc.contributor.authorValente, Anabela A.
dc.contributor.authorPillinger, Martyn
dc.contributor.authorLourenço, J. P.
dc.contributor.authorGonçalves, Isabel S.
dc.date.accessioned2013-01-04T12:25:28Z
dc.date.available2013-01-04T12:25:28Z
dc.date.issued2009
dc.date.updated2013-01-03T10:38:02Z
dc.description.abstractA mesoporous silica-supported molybdenum oxide catalyst with a loading of 0.17Mo/nm2 was prepared by liquid phase deposition ofMoO2Cl2(dmf)2 (1) onto MCM-41 (dmf = dimethylformamide). Powder X-ray diffraction and N2 adsorption studies of Mo-MCM-41 indicate that the texture properties of the support were preserved during the grafting experiment. On the basis of evidence from FTIR spectroscopy, 13C and 29Si MAS NMR, and Mo K-edge EXAFS, the Mo atoms in this catalyst are mainly present as isolated {MoO2[(–O)3SiO]2(dmf)2} species, with a small contribution from oxo-bridged dimers. Catalysis tests show that complex 1 and Mo-MCM-41 are highly active oxidation catalysts for liquid-phase epoxidation of unfunctionalised olefins using tert-butylhydroperoxide as oxidant, from ambient to 55 ◦C. The high stability and recyclability of the heterogeneous Mo-MCM-41 catalyst is attributed to the strong metal oxide–support interaction. With cyclooctene, 1-octene, trans-2-octene and norbornene substrates, the corresponding epoxides were the only observed reaction products. The reactions of the other substrates gave by-products such as 8,9-p-menthen-1,2-diol from (R)-(+)-limonene, campholenic aldehyde from -pinene, and benzaldehyde from styrene. The addition of dichloromethane as a co-solvent had a beneficial effect on catalytic performance, and in the case of (R)-(+)-limonene allowed the epoxide to be formed as the only reaction product.por
dc.identifier.citationMonteiro, Bernardo; Balula, Salete S.; Gago, Sandra; Grosso, Carla; Figueiredo, Sónia; Lopes, André D.; Valente, Anabela A.; Pillinger, Martyn; Lourenço, João P.; Gonçalves, Isabel S. Comparison of liquid-phase olefin epoxidation catalysed by dichlorobis-(dimethylformamide)dioxomolybdenum(VI) in homogeneous phase and grafted onto MCM-41, Journal of Molecular Catalysis A: Chemical, 297, 2, 110-117, 2009.por
dc.identifier.issn1381-1169
dc.identifier.otherAUT: JLO01215; ADL01681;
dc.identifier.urihttp://hdl.handle.net/10400.1/2056
dc.language.isoengpor
dc.peerreviewedyespor
dc.publisherElsevierpor
dc.subjectMCM-41por
dc.subjectMesoporous materialspor
dc.subjectEXAFSpor
dc.subjectMolybdenumpor
dc.subjectOxidationpor
dc.subjectHeterogeneous catalysispor
dc.titleComparison of liquid-phase olefin epoxidation catalysed by dichlorobis-(dimethylformamide)dioxomolybdenum(VI) in homogeneous phase and grafted onto MCM-41por
dc.typejournal article
dspace.entity.typePublication
oaire.citation.endPage117por
oaire.citation.issue2por
oaire.citation.startPage110por
oaire.citation.titleJournal of Molecular Catalysis A: Chemicalpor
oaire.citation.volume297por
person.familyNameGrosso
person.familyNameD. Lopes
person.familyNameLourenço
person.givenNameCarla
person.givenNameAndré
person.givenNameJoão P.
person.identifier2824636
person.identifier634248
person.identifier.ciencia-idE01F-48D7-D37F
person.identifier.ciencia-id351E-856A-0300
person.identifier.ciencia-idF81F-A1F0-2A7C
person.identifier.orcid0000-0003-1999-3471
person.identifier.orcid0000-0002-9702-1216
person.identifier.orcid0000-0002-0501-6672
person.identifier.ridE-2136-2012
person.identifier.ridA-7758-2008
person.identifier.scopus-author-id25229731200
person.identifier.scopus-author-id7201958625
person.identifier.scopus-author-id57195730600
rcaap.rightsrestrictedAccesspor
rcaap.typearticlepor
relation.isAuthorOfPublication281e1cc5-59bc-47d4-96e1-ce923ad6be4c
relation.isAuthorOfPublicationf2f0fe56-e04d-4229-b37b-2b9f1789fe2d
relation.isAuthorOfPublicationf66ab886-d989-4c1d-9550-527507723c26
relation.isAuthorOfPublication.latestForDiscoveryf2f0fe56-e04d-4229-b37b-2b9f1789fe2d

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