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Novel coordination polymers with (Pyrazolato)-based tectons: catalytic activity in the peroxidative oxidation of alcohols and cyclohexane

2015-05Journal article Restricted access
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dc.contributor.authorTimokhin, Ivan
dc.contributor.authorPettinari, Claudio
dc.contributor.authorMarchetti, Fabio
dc.contributor.authorPettinari, Riccardo
dc.contributor.authorCONDELLO, Francesca
dc.contributor.authorGALLI, SIMONA
dc.contributor.authorAlegria, Elisabete
dc.contributor.authorMartins, Luisa
dc.contributor.authorPombeiro, Armando
dc.date.accessioned2016-04-28T12:13:04Z
dc.date.available2016-04-28T12:13:04Z
dc.date.issued2015-05
dc.description.abstractCoupling five rigid or flexible bis(pyrazolato)based tectons with late transition metal ions allowed us to isolate 18 coordination polymers (CPs). As assessed by thermal analysis, all of them possess a remarkable thermal stability, their decomposition temperatures lying in the range of 340-500 degrees C. As demonstrated by N-2 adsorption measurements at 77 K, their Langmuir specific surface areas span the rather vast range of 135-1758 m(2)/g, in agreement with the porous or dense polymeric architectures retrieved by powder X-ray diffraction structure solution methods. Two representative families of CPs, built up with either rigid or flexible spacers, were tested as catalysts in (0 the microwave-assisted solvent-free peroxidative oxidation of alcohols by t-BuOOH, and (ii) the peroxidative oxidation of cydohexane to cydohexanol and cydohexanone by H2O2 in acetonitrile. Those CPs bearing the rigid spacer, concurrently possessing higher specific surface areas, are more active than the corresponding ones with the flexible spacer. Moreover, the two copper(I)-containing CPs investigated exhibit the highest efficiency in both reactions, leading selectively to a maximum product yield of 92% (and TON up to 1.5 x 10(3)) in the oxidation of 1-phenylethanol and of 11% in the oxidation of cydohexane, the latter value being higher than that granted by the current industrial process.pt_PT
dc.identifier.citationTIMOKHIN, Ivan; [et al] - Novel coordination polymers with (Pyrazolato)-based tectons: catalytic activity in the peroxidative oxidation of alcohols and cyclohexane. Crystal Growth & Design. ISSN 1528-7483. Vol. 15, N.º 5 (2015), pp. 2303-2317pt_PT
dc.identifier.doi10.1021/acs.cgd.5b00083pt_PT
dc.identifier.issn1528-7483
dc.identifier.issn1528-7505
dc.identifier.urihttp://hdl.handle.net/10400.21/6119
dc.language.isoengpt_PT
dc.peerreviewedyespt_PT
dc.publisherAmer Chemical Socpt_PT
dc.subjectMetal-organic frameworkspt_PT
dc.subjectInorganic hybrid polymerpt_PT
dc.subjectLate transition-metalspt_PT
dc.subjectAerobic oxidationpt_PT
dc.subjectBenzylic alcoholspt_PT
dc.subjectHighly efficientpt_PT
dc.subjectSelective oxidationpt_PT
dc.subjectPowder diffractionpt_PT
dc.subjectNitroxyl radicalspt_PT
dc.subjectCrystal-structurept_PT
dc.titleNovel coordination polymers with (Pyrazolato)-based tectons: catalytic activity in the peroxidative oxidation of alcohols and cyclohexanept_PT
dc.typejournal article
dspace.entity.typePublication
oaire.citation.endPage2317pt_PT
oaire.citation.issue5pt_PT
oaire.citation.startPage2303pt_PT
oaire.citation.titleCrystal Growth & Designpt_PT
oaire.citation.volume15pt_PT
person.familyNamePettinari
person.familyNamePettinari
person.familyNameCONDELLO
person.familyNameGALLI
person.familyNameAlegria
person.familyNameMartins
person.familyNamePombeiro
person.givenNameClaudio
person.givenNameRiccardo
person.givenNameFrancesca
person.givenNameSIMONA
person.givenNameElisabete
person.givenNameLuisa
person.givenNameArmando
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person.identifier637885
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person.identifier.orcid0000-0002-6313-4431
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person.identifier.orcid0000-0003-0335-5707
person.identifier.orcid0000-0003-4060-1057
person.identifier.orcid0000-0002-5403-9352
person.identifier.orcid0000-0001-8323-888X
person.identifier.ridE-9945-2012
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person.identifier.scopus-author-id7006581579
person.identifier.scopus-author-id6701344763
person.identifier.scopus-author-id7102963193
person.identifier.scopus-author-id8315848300
person.identifier.scopus-author-id8650947800
person.identifier.scopus-author-id7006067269
rcaap.rightsclosedAccesspt_PT
rcaap.typearticlept_PT
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