Please use this identifier to cite or link to this item: http://hdl.handle.net/10773/20772
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dc.contributor.authorAmarante, Tatiana R.pt
dc.contributor.authorNeves, Patriciapt
dc.contributor.authorValente, Anabela A.pt
dc.contributor.authorAlmeida Paz, Filipe A.pt
dc.contributor.authorFitch, Andrew N.pt
dc.contributor.authorPillinger, Martynpt
dc.contributor.authorGoncalves, Isabel S.pt
dc.date.accessioned2017-12-07T19:58:53Z-
dc.date.issued2013pt
dc.identifier.issn0020-1669pt
dc.identifier.urihttp://hdl.handle.net/10773/20772-
dc.description.abstractThe reaction of MoO3, 2,2'-bipyridine-5,5-dicarboxylic acid (H(2)bpdc), water, and dimethylformamide in the mole ratio 1:1:1730:130 at 150 degrees C for 3 days in a rotating Teflon-lined digestion bomb leads to the isolation of the molybdenum oxide/bipyridinedicarboxylate hybrid material (DMA)[MoO3(Hbpdc)]center dot nH(2)O (1) (DMA = dimethylammonium). Compound 1 was characterized by scanning electron microscopy, FT-IR and C-13{H-1} CP MAS NMR spectroscopies, and elemental and thermogravimetric analyses. The solid state structure of 1 was solved and refined through Rietveld analysis of high resolution synchrotron X-ray powder diffraction data in conjunction with information derived from the above techniques. The material, crystallizing in the noncentrosymmetric monoclinic space group Pc, is composed of an anionic one-dimensional organic-inorganic hybrid polymer, (1)(infinity)[MoO3(Hbpdc)](-), formed by corner-sharing distorted {MoO4N2} octahedra, which cocrystallizes with charge-balancing DMA(+) cations and one water molecule per metal center. In the crystal structure of 1, the close packing of individual anionic polymers, DMA(+) cations, and water molecules is mediated by a series of supramolecular contacts, namely strong (O-H center dot center dot center dot O, N+-H center dot center dot center dot O-) and weak (C-H center dot center dot center dot O) hydrogen bonding interactions, and pi-pi contacts involving adjacent coordinated Hbpdc(-) ligands. The catalytic potential of 1 was investigated in the epoxidation reactions of the bioderived olefins methyl oleate (Ole) and DL-limonene (Lim) using tert-butylhydroperoxide (TBHP) as the oxygen donor and 1,2-dichloroethane (DCE) or (trifluoromethyl)benzene (BTF) as cosolvent, at 55 or 75 degrees C. Under these conditions, 1 acts as a source of active soluble species, leading to epoxide yields of up to 98% for methyl 9,10-epoxystearate (BTF, 75 degrees C, 100% conversion of Ole) and 89% for 1,2-epoxy-p-menth-8-ene (DCE, 55 degrees C, 95% conversion of Lim). Catalytic systems employing the ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide as solvent could be effectively recycled.pt
dc.language.isoengpt
dc.publisherAMER CHEMICAL SOCpt
dc.relationinfo:eu-repo/grantAgreement/FCT/SFRH/SFRH%2FBPD%2F73540%2F2010/PTpt
dc.relationinfo:eu-repo/grantAgreement/FCT/SFRH/SFRH%2FBD%2F64224%2F2009/PTpt
dc.relationinfo:eu-repo/grantAgreement/FCT/COMPETE/132936/PTpt
dc.rightsrestrictedAccesspor
dc.subjectMETAL-ORGANIC FRAMEWORKpt
dc.subjectSTATE COORDINATION CHEMISTRYpt
dc.subjectTEMPERATURE IONIC LIQUIDSpt
dc.subjectOLEFIN EPOXIDATIONpt
dc.subjectDIOXOMOLYBDENUM(VI) COMPLEXESpt
dc.subjectPOLYOXOMOLYBDATE CLUSTERSpt
dc.subjectOCTAMOLYBDATE CLUSTERSpt
dc.subjectCARBON-DIOXIDEpt
dc.subjectMETHYL OLEATEpt
dc.subjectACTIVE-SITESpt
dc.titleHydrothermal Synthesis, Crystal Structure, and Catalytic Potential of a One-Dimensional Molybdenum Oxide/Bipyridinedicarboxylate Hybridpt
dc.typearticlept
dc.peerreviewedyespt
ua.distributioninternationalpt
degois.publication.firstPage4618pt
degois.publication.issue8pt
degois.publication.lastPage4628pt
degois.publication.titleINORGANIC CHEMISTRYpt
degois.publication.volume52pt
dc.date.embargo10000-01-01-
dc.relation.publisherversion10.1021/ic400248mpt
dc.identifier.doi10.1021/ic400248mpt
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