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http://hdl.handle.net/10773/20241
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DC Field | Value | Language |
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dc.contributor.author | Amarante, Tatiana R. | pt |
dc.contributor.author | Neves, Patrícia | pt |
dc.contributor.author | Gomes, Ana C. | pt |
dc.contributor.author | Nolasco, Mariela M. | pt |
dc.contributor.author | Ribeiro-Claro, Paulo | pt |
dc.contributor.author | Coelho, Ana C. | pt |
dc.contributor.author | Valente, Anabela A. | pt |
dc.contributor.author | Almeida Paz, Filipe A. | pt |
dc.contributor.author | Smeets, Stef | pt |
dc.contributor.author | McCusker, Lynne B. | pt |
dc.contributor.author | Pillinger, Martyn | pt |
dc.contributor.author | Gonçalves, Isabel S. | pt |
dc.date.accessioned | 2017-12-07T19:40:12Z | - |
dc.date.issued | 2014 | pt |
dc.identifier.issn | 0020-1669 | pt |
dc.identifier.uri | http://hdl.handle.net/10773/20241 | - |
dc.description.abstract | The 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.iso | eng | pt |
dc.publisher | American Chemical Society | pt |
dc.relation | info:eu-repo/grantAgreement/FCT/5876-PPCDTI/121677/PT | pt |
dc.relation | info:eu-repo/grantAgreement/FCT/COMPETE/132936/PT | pt |
dc.relation | info:eu-repo/grantAgreement/FCT/SFRH/SFRH%2FBPD%2F73540%2F2010/PT | pt |
dc.relation | info:eu-repo/grantAgreement/FCT/SFRH/SFRH%2FBD%2F64224%2F2009/PT | pt |
dc.relation | info:eu-repo/grantAgreement/EC/FP7/226716/EU | pt |
dc.rights | restrictedAccess | por |
dc.subject | Phosphine oxide ligands | pt |
dc.subject | Crystal-structure | pt |
dc.subject | Hydrothermal synthesis | pt |
dc.subject | Dioxomolybdenum(VI) complexes | pt |
dc.subject | Molybdenum(VI) Complex | pt |
dc.subject | Molecular-structure | pt |
dc.subject | Performance | pt |
dc.subject | Derivatives | pt |
dc.subject | Dioxo | pt |
dc.subject | Dichlorodioxomolybdenum(VI) | pt |
dc.title | Synthesis, Structural Elucidation, and Catalytic Properties in Olefin Epoxidation of the Polymeric Hybrid Material [Mo3O9(2-[3(5)-Pyrazolyl]pyridine)](n) | pt |
dc.type | article | pt |
dc.peerreviewed | yes | pt |
ua.distribution | international | pt |
degois.publication.firstPage | 2652 | pt |
degois.publication.issue | 5 | pt |
degois.publication.lastPage | 2665 | pt |
degois.publication.title | Inorganic Chemistry | pt |
degois.publication.volume | 53 | pt |
dc.date.embargo | 10000-01-01 | - |
dc.relation.publisherversion | 10.1021/ic403033j | pt |
dc.identifier.doi | 10.1021/ic403033j | pt |
Appears in Collections: | CICECO - Artigos DQ - Artigos |
Files in This Item:
File | Description | Size | Format | |
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Synthesis Structural Elucidation and Catalytic Properties in Olefin Epoxidation of the Polymeric Hybrid Material [Mo 3O 9(2-[3(5)-Pyrazolyl]pyridine)] n_10.1021ic403033j.pdf | 1.96 MB | Adobe PDF |
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