Please use this identifier to cite or link to this item: http://hdl.handle.net/10773/20241
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dc.contributor.authorAmarante, Tatiana R.pt
dc.contributor.authorNeves, Patriciapt
dc.contributor.authorGomes, Ana C.pt
dc.contributor.authorNolasco, Mariela M.pt
dc.contributor.authorRibeiro-Claro, Paulopt
dc.contributor.authorCoelho, Ana C.pt
dc.contributor.authorValente, Anabela A.pt
dc.contributor.authorPaz, Filipe A. Almeidapt
dc.contributor.authorSmeets, Stefpt
dc.contributor.authorMcCusker, Lynne B.pt
dc.contributor.authorPillinger, Martynpt
dc.contributor.authorGoncalves, Isabel S.pt
dc.date.accessioned2017-12-07T19:40:12Z-
dc.date.issued2014pt
dc.identifier.issn0020-1669pt
dc.identifier.urihttp://hdl.handle.net/10773/20241-
dc.description.abstractThe reaction of [MoO2Cl2(pzpy)] (1) (pzpy = 2-[3(5)-pyrazolyl]pyridine) with water in an open reflux system (16 h), in a microwave synthesis system (120 degrees C, 2 h), or in a Teflon-lined stainless steel digestion bomb (100 degrees C, 19 h) gave the molybdenum oxide/pyrazolylpyridine polymeric hybrid material [Mo3O9(pzpy)](n) (2) as a microcrystalline powder in yields of 72-79%. Compound 2 can also be obtained by the hydrothermal reaction of MoO3, pzpy, and H2O at 160 degrees C for 3 d. Secondary products isolated from the reaction solutions included the salt (pzpyH)(2)(MoCl4) (3) (pzpyH = 2-[3(5)-pyrazolyl]pyridinium), containing a very rare example of the tetrahedral MoCl42- anion, and the tetranuclear compound [Mo4O12(pzpy)(4)] (4). Reaction of 2 with excess tert-butylhydroperoxide (TBHP) led to the isolation of the oxodiperoxo complex [MoO(O-2)(2)(pzpy)(4)] (5). Single-crystal X-ray structures of 3 and 5 are described. Fourier transform (FT)-IR and FT Raman spectra for 1, 4, and 5 were assigned based on density functional theory calculations. The structure of 2 was determined from synchrotron powder X-ray diffraction data in combination with other physicochemical information. In 2, a hybrid organic inorganic one-dimensional (1D) polymer, (1)(infinity)[Mo3O9(pzpy)], is formed by the connection of two very distinct components: a double ladder-type inorganic core reminiscent of the crystal structure of MoO3 and 1D chains of corner-sharing distorted {MoO4N2} octahedra. Compound 2 exhibits moderate activity and high selectivity when used as a (pre)catalyst for the epoxidation of cis-cyclooctene with TBHP. Under the reaction conditions used, 2 is poorly soluble and is gradually converted into 5, which is at least partly responsible for the catalytic reaction.pt
dc.language.isoengpt
dc.publisherAMER CHEMICAL SOCpt
dc.relationinfo:eu-repo/grantAgreement/FCT/5876-PPCDTI/121677/PTpt
dc.relationinfo:eu-repo/grantAgreement/FCT/COMPETE/132936/PTpt
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/EC/FP7/226716/EUpt
dc.rightsrestrictedAccesspor
dc.subjectPHOSPHINE OXIDE LIGANDSpt
dc.subjectCRYSTAL-STRUCTUREpt
dc.subjectHYDROTHERMAL SYNTHESISpt
dc.subjectDIOXOMOLYBDENUM(VI) COMPLEXESpt
dc.subjectMOLYBDENUM(VI) COMPLEXpt
dc.subjectMOLECULAR-STRUCTUREpt
dc.subjectPERFORMANCEpt
dc.subjectDERIVATIVESpt
dc.subjectDIOXOpt
dc.subjectDICHLORODIOXOMOLYBDENUM(VI)pt
dc.titleSynthesis, Structural Elucidation, and Catalytic Properties in Olefin Epoxidation of the Polymeric Hybrid Material [Mo3O9(2-[3(5)-Pyrazolyl]pyridine)](n)pt
dc.typearticlept
dc.peerreviewedyespt
ua.distributioninternationalpt
degois.publication.firstPage2652pt
degois.publication.issue5pt
degois.publication.lastPage2665pt
degois.publication.titleINORGANIC CHEMISTRYpt
degois.publication.volume53pt
dc.date.embargo10000-01-01-
dc.relation.publisherversion10.1021/ic403033jpt
dc.identifier.doi10.1021/ic403033jpt
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