Please use this identifier to cite or link to this item: http://hdl.handle.net/10773/26360
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dc.contributor.authorNogueira, Lucie S.pt_PT
dc.contributor.authorAntunes, Margarida M.pt_PT
dc.contributor.authorGomes, Ana C.pt_PT
dc.contributor.authorCunha-Silva, Luíspt_PT
dc.contributor.authorPillinger, Martynpt_PT
dc.contributor.authorLopes, André D.pt_PT
dc.contributor.authorValente, Anabela A.pt_PT
dc.contributor.authorGonçalves, Isabel S.pt_PT
dc.date.accessioned2019-08-01T14:23:45Z-
dc.date.issued2019-07-11-
dc.identifier.issn1477-9226pt_PT
dc.identifier.urihttp://hdl.handle.net/10773/26360-
dc.description.abstractThe reaction of the macrocyclic cavitand cucurbit[6]uril (CB[6]) and the diaqua complex [MoO2Cl2(H2O)2] in hydrochloric acid solution gave a water insoluble supramolecular compound with the general composition 2[MoO2Cl2(H2O)2]·CB[6]·xH2O·yHCl·z(CH3COCH3) (2). Single crystal X-ray diffraction (XRD) analysis revealed the presence of barrel-shape supramolecular entities, {CB[6]·10(H2O)}, aligned in layers which are shifted relative to adjacent layers to form a brick-like pattern. The CB[6]/water hydrogen-bonded entities further engage in intermolecular interactions with water, HCl and [MoO2Cl2(H2O)2] molecules to form a three-dimensional (3D) framework. Compound 2 was characterised by thermogravimetric analysis (TGA), IR and Raman vibrational spectroscopy, and 13C{1H} CP MAS NMR. The reference complex [MoO2Cl2(H2O)2]·(diglyme)2 (1) and compound 2 were studied for the oxidative catalytic conversion of olefins (cis-cyclooctene, cyclohexene and styrene) with aqueous H2O2 as oxidant. Using alcohols as solvents, 2 was employed in a one-pot two-stage strategy for converting olefins to alkoxy products, which involves oxidation (with H2O2) and acid chemistry. Mechanistic studies were carried out using different intermediates as substrates, and the type of solvent and substrate scope were investigated. The results demonstrated the ability of the CB[6]/MoVI supramolecular adduct to function as an acid-oxidation multifunctional catalyst, and its recovery and reuse via relatively simple procedures.pt_PT
dc.description.sponsorshipWe acknowledge the support of CICECO – Aveiro Institute of Materials [FCT (Fundação para a Ciência e a Tecnologia) Ref. UID/CTM/50011/2019], REQUIMTE-LAQV (UID/QUI/50006/2019), Centre of Marine Sciences – CCMAR (UID/Multi/04326/2019), and the CENTRO 2020 Regional Operational Programme (Project CENTRO-01-0145-FEDER-028031; PTDC/QUI-QOR/28031/2017), co-financed by national funds through the FCT/MEC and the European Union (EU) through the European Regional Development Fund under the Portugal 2020 Partnership Agreement. The FCT and the EU are acknowledged for a Ph.D. grant to L. S. N. (PD/BD/109666/2015). The positions held by M. M. A. and A. C. G. were funded by national funds (OE), through FCT, I.P., in the scope of the framework contract foreseen in the numbers 4, 5 and 6 of article 23 of the Decree-Law 57/2016 of 29 August, changed by Law 57/2017 of 19 July.pt_PT
dc.language.isoengpt_PT
dc.publisherRoyal Society of Chemistrypt_PT
dc.relationUID/CTM/50011/2019pt_PT
dc.relationUID/QUI/50006/2019pt_PT
dc.relationUID/Multi/04326/2019pt_PT
dc.relationCENTRO-01-0145-FEDER-028031pt_PT
dc.relationPTDC/QUI-QOR/28031/2017pt_PT
dc.relationPD/BD/109666/2015pt_PT
dc.rightsembargoedAccesspt_PT
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/pt_PT
dc.titleA hydrogen-bonded assembly of cucurbit[6]uril and [MoO2Cl2(H2O)2] with catalytic efficacy for the one-pot conversion of olefins to alkoxy productspt_PT
dc.typearticlept_PT
dc.description.versionpublishedpt_PT
dc.peerreviewedyespt_PT
degois.publication.firstPage11508pt_PT
degois.publication.issue30pt_PT
degois.publication.lastPage11519pt_PT
degois.publication.titleDalton transactionspt_PT
degois.publication.volume48pt_PT
dc.date.embargo2020-07-12-
dc.relation.publisherversionhttps://pubs.rsc.org/en/content/articlehtml/2019/dt/c9dt02127bpt_PT
dc.identifier.doi10.1039/c9dt02127bpt_PT
dc.identifier.essn1477-9234pt_PT
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