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Simple solvent-free preparation of dispersed composites and their application as catalysts in oxidation and hydrocarboxylation of cyclohexane

2017-09Journal article Restricted access
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dc.contributor.authorAlegria, Elisabete
dc.contributor.authorFontolan, Emmanuele
dc.contributor.authorDa Costa Ribeiro, Ana Paula
dc.contributor.authorKopylovich, Maximilian
dc.contributor.authorDomingos, Catarina
dc.contributor.authorFerraria, Ana Maria
dc.contributor.authorBertani, Roberta
dc.contributor.authorBotelho do Rego, Ana M.
dc.contributor.authorPombeiro, Armando
dc.date.accessioned2018-02-27T12:30:48Z
dc.date.available2018-02-27T12:30:48Z
dc.date.issued2017-09
dc.descriptionEste trabalho foi financiado pelo Concurso Anual para Projetos de Investigação, Desenvolvimento, Inovação e Criação Artística (IDI&CA) 2016 do Instituto Politécnico de Lisboa. Código de referência IPL/2016/MechSynCat_ISEL
dc.description.abstractA simple and clean mechanochemical synthesis at room temperature was employed to prepare CuO-Fe2O3-CoCl2 (100 nm scale), MoO3-V2O5, CuO-CoCl2, Fe2O3-CoCl2, CuO-V2O5, Cu(CH3COO)(2)-V2O5, Cu(CH3COO)(2)-MoO3 (1-100 mm scale) 3d metal based dispersed composites with different ratios of components using simple metal salts/oxides and multiwalled carbon nanotubes (CNT) or graphene oxide (GO) additives (CoCl2-CNT, CoCl2-GO). The thus prepared composite materials were characterized by Xray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), field emission gun scanning electron microscopy (FEGSEM), energy-dispersive X-ray spectroscopy (EDX) and transmission electron microscopy (TEM). XPS analysis revealed no metal redox change upon ball milling treatment, which however promotes metal hydroxylation. The catalytic activity of the prepared composites in the heterogeneous low power microwave-assisted oxidation of cyclohexane with aq. H2O2 at 30 degrees C was notorious with yields up to 31% and selectivity up to 94% towards cyclohexanol (upon treatment with PPh3) for the CuO-CoCl2-based material. The hydro-carboxylation of cyclohexane with CO, water and K2S2O8 to produce cyclohexanecarboxylic acid bearing one more carbon atom at 60 degrees C is achieved with yields up to 17% for the reaction performed in the presence of the CuO-CoCl2 catalyst. The clean CuO-CoCl2 (1:2) catalyst preparation and the catalytic reaction (oxidation of cyclohexane) can be achieved in one-pot at low temperature, without any added organic solvent, and by using exclusively the mechanochemical energy input, with a marked 23% yield at 30 degrees C.pt_PT
dc.description.versioninfo:eu-repo/semantics/publishedVersionpt_PT
dc.identifier.citationALEGRIA, Elisabete C. B. A.; [et al] – Simple solvent-free preparation of dispersed composites and their application as catalysts in oxidation and hydrocarboxylation of cyclohexane. Materials Today Chemistry. ISSN 2468-5194. Vol. 5, (2017), pp. 52-62pt_PT
dc.identifier.doi10.1016/j.mtchem.2017.07.002pt_PT
dc.identifier.issn2468-5194
dc.identifier.urihttp://hdl.handle.net/10400.21/8142
dc.language.isoengpt_PT
dc.peerreviewedyespt_PT
dc.publisherElsevierpt_PT
dc.relationFCT - SFRH/BPD/108338/2015pt_PT
dc.relationFCT - IF/01270/2013/CP1163/CT0007pt_PT
dc.relationFCT - PTDC/QEQ-QIN/3967/2014pt_PT
dc.relationProjeto financiado no âmbito do Concurso de Projetos de Investigação, Desenvolvimento, Inovação & Criação Artística (IDI&CA) financiados pelo Instituto Politécnico de Lisboa. IPL/2016/MechSynCat_ISELpt_PT
dc.relation.publisherversionhttps://ac.els-cdn.com/S2468519417301052/1-s2.0-S2468519417301052-main.pdf?_tid=spdf-6193c500-b4fb-44b0-a44a-0fecf46226b0&acdnat=1519733866_578c06aa4a5f1ff5e5098eee6bcefc9cpt_PT
dc.subjectMechanochemicalpt_PT
dc.subjectBall-millingpt_PT
dc.subjectCompositespt_PT
dc.subjectOne-pot oxidationpt_PT
dc.subjectHydrocarboxylationpt_PT
dc.subjectCyclohexanept_PT
dc.titleSimple solvent-free preparation of dispersed composites and their application as catalysts in oxidation and hydrocarboxylation of cyclohexanept_PT
dc.typejournal article
dspace.entity.typePublication
oaire.awardURIinfo:eu-repo/grantAgreement/FCT/SFRH/SFRH%2FBPD%2F90883%2F2012/PT
oaire.awardURIinfo:eu-repo/grantAgreement/FCT/5876/UID%2FQUI%2F00100%2F2013/PT
oaire.awardURIinfo:eu-repo/grantAgreement/FCT/5876/UID%2FNAN%2F50024%2F2013/PT
oaire.citation.endPage62pt_PT
oaire.citation.startPage52pt_PT
oaire.citation.titleMaterials Today Chemistrypt_PT
oaire.citation.volume5pt_PT
oaire.fundingStreamSFRH
oaire.fundingStream5876
oaire.fundingStream5876
person.familyNameAlegria
person.familyNameda Costa Ribeiro
person.familyNameKopylovich
person.familyNameDomingos
person.familyNameFerraria
person.familyNameBertani
person.familyNamePombeiro
person.givenNameElisabete
person.givenNameAna Paula
person.givenNameMaximilian
person.givenNameCatarina
person.givenNameAna Maria
person.givenNameRoberta
person.givenNameArmando
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person.identifier.scopus-author-id8315848300
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project.funder.identifierhttp://doi.org/10.13039/501100001871
project.funder.identifierhttp://doi.org/10.13039/501100001871
project.funder.identifierhttp://doi.org/10.13039/501100001871
project.funder.nameFundação para a Ciência e a Tecnologia
project.funder.nameFundação para a Ciência e a Tecnologia
project.funder.nameFundação para a Ciência e a Tecnologia
rcaap.rightsclosedAccesspt_PT
rcaap.typearticlept_PT
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