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http://hdl.handle.net/10773/20772
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DC Field | Value | Language |
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dc.contributor.author | Amarante, Tatiana R. | pt |
dc.contributor.author | Neves, Patricia | pt |
dc.contributor.author | Valente, Anabela A. | pt |
dc.contributor.author | Almeida Paz, Filipe A. | pt |
dc.contributor.author | Fitch, Andrew N. | pt |
dc.contributor.author | Pillinger, Martyn | pt |
dc.contributor.author | Goncalves, Isabel S. | pt |
dc.date.accessioned | 2017-12-07T19:58:53Z | - |
dc.date.issued | 2013 | pt |
dc.identifier.issn | 0020-1669 | pt |
dc.identifier.uri | http://hdl.handle.net/10773/20772 | - |
dc.description.abstract | The 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.iso | eng | pt |
dc.publisher | AMER CHEMICAL SOC | 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/FCT/COMPETE/132936/PT | pt |
dc.rights | restrictedAccess | por |
dc.subject | METAL-ORGANIC FRAMEWORK | pt |
dc.subject | STATE COORDINATION CHEMISTRY | pt |
dc.subject | TEMPERATURE IONIC LIQUIDS | pt |
dc.subject | OLEFIN EPOXIDATION | pt |
dc.subject | DIOXOMOLYBDENUM(VI) COMPLEXES | pt |
dc.subject | POLYOXOMOLYBDATE CLUSTERS | pt |
dc.subject | OCTAMOLYBDATE CLUSTERS | pt |
dc.subject | CARBON-DIOXIDE | pt |
dc.subject | METHYL OLEATE | pt |
dc.subject | ACTIVE-SITES | pt |
dc.title | Hydrothermal Synthesis, Crystal Structure, and Catalytic Potential of a One-Dimensional Molybdenum Oxide/Bipyridinedicarboxylate Hybrid | pt |
dc.type | article | pt |
dc.peerreviewed | yes | pt |
ua.distribution | international | pt |
degois.publication.firstPage | 4618 | pt |
degois.publication.issue | 8 | pt |
degois.publication.lastPage | 4628 | pt |
degois.publication.title | INORGANIC CHEMISTRY | pt |
degois.publication.volume | 52 | pt |
dc.date.embargo | 10000-01-01 | - |
dc.relation.publisherversion | 10.1021/ic400248m | pt |
dc.identifier.doi | 10.1021/ic400248m | pt |
Appears in Collections: | CICECO - Artigos |
Files in This Item:
File | Description | Size | Format | |
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Hydrothermal Synthesis Crystal Structure and Catalytic Potential of a One-Dimensional Molybdenum OxideBipyridinedicarboxylate Hybrid_10.1021ic400248m.pdf | 3.77 MB | Adobe PDF |
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