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Highly active and selective supported rhenium catalysts for aerobic oxidation of n-Hexane and n-Heptane

2018-03-15Journal article Open access
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dc.contributor.authorMishra, Gopal
dc.contributor.authorAlegria, Elisabete
dc.contributor.authorPombeiro, Armando
dc.contributor.authorMartins, Luisa
dc.date.accessioned2018-03-22T10:02:56Z
dc.date.available2018-03-22T10:02:56Z
dc.date.issued2018-03-15
dc.description.abstractA series of derivative C-scorpionate rhenium complexes, i.e., [ReCl2{NNC(O)C6H5} (Hpz)(PPh3)2] (A) (where Hpz is pyrazole), [ReCl2{NNC(O)C6H5}(Hpz)2(PPh3)] (B), [ReClF {NNC(O)C6H5}(Hpz)2(PPh3)] (C), and their precursor [ReOCl3(PPh3)2] (D), immobilized on 3-aminopropyl-functionalized silica have been prepared and used for neat O2 oxidation of n-hexane and n-heptane mainly to the corresponding alcohols and, in lower amounts, ketones. The supported catalyst C, with fluoro- and diazenido-ligands, exhibits the highest activity for both alkanes (overall turnover numbers (TONs) up to 3.8 _ 103 and 2.5 _ 103, for n-hexane and n-heptane, respectively) and can be reused in consecutive catalytic cycles. Improved conversion was observed after addition of hetero-carboxylate co-catalysts. A free-radical-based mechanism is proposed to explain the product formation.pt_PT
dc.description.versioninfo:eu-repo/semantics/publishedVersionpt_PT
dc.identifier.citationMISHRA, Gopal S.; ALEGRIA, Elisabete C. B. A.; POMBEIRO, Armando J. L.; MARTINS, Luísa M. D. R. S. – Highly active and selective supported rhenium catalysts for aerobic oxidation of n-Hexane and n-Heptane. ISSN 2073-4344. Vol. 8, N.º 3 (2018), pp. 1-16pt_PT
dc.identifier.doi10.3390/catal8030114pt_PT
dc.identifier.issn2073-4344
dc.identifier.urihttp://hdl.handle.net/10400.21/8278
dc.language.isoengpt_PT
dc.peerreviewedyespt_PT
dc.publisherMDPIpt_PT
dc.relationFCT - PTDC/QEQ-ERQ/1648/2014pt_PT
dc.relationFCT - PTDC/QEQ-QIN/3967/2014pt_PT
dc.relationFCT/9701/25/10/2013/S (Indian–Portuguese Cooperation Program 2013)pt_PT
dc.subjectRheniumpt_PT
dc.subjectScorpionate derivativept_PT
dc.subjectImmobilizationpt_PT
dc.subjectSupported catalysispt_PT
dc.subjectN-alkanept_PT
dc.subjectOxidationpt_PT
dc.subjectMolecular oxygenpt_PT
dc.subjectProduct selectivitypt_PT
dc.subjectRadical mechanismpt_PT
dc.titleHighly active and selective supported rhenium catalysts for aerobic oxidation of n-Hexane and n-Heptanept_PT
dc.typejournal article
dspace.entity.typePublication
oaire.awardURIinfo:eu-repo/grantAgreement/FCT/5876/UID%2FQUI%2F00100%2F2013/PT
oaire.citation.endPage16pt_PT
oaire.citation.issue3pt_PT
oaire.citation.startPage1pt_PT
oaire.citation.titleCatalystspt_PT
oaire.citation.volume8pt_PT
oaire.fundingStream5876
person.familyNameMishra
person.familyNameAlegria
person.familyNamePombeiro
person.familyNameMartins
person.givenNameGopal
person.givenNameElisabete
person.givenNameArmando
person.givenNameLuisa
person.identifier863202
person.identifier637885
person.identifier.ciencia-id4814-2CD6-F93E
person.identifier.ciencia-id8C1F-851A-9F1C
person.identifier.ciencia-id8311-38FA-CEFB
person.identifier.ciencia-idE218-E297-A4EA
person.identifier.orcid0000-0001-6566-7218
person.identifier.orcid0000-0003-4060-1057
person.identifier.orcid0000-0001-8323-888X
person.identifier.orcid0000-0002-5403-9352
person.identifier.ridE-9945-2012
person.identifier.ridI-5945-2012
person.identifier.ridG-6210-2011
person.identifier.scopus-author-id7102625692
person.identifier.scopus-author-id8315848300
person.identifier.scopus-author-id7006067269
person.identifier.scopus-author-id8650947800
project.funder.identifierhttp://doi.org/10.13039/501100001871
project.funder.nameFundação para a Ciência e a Tecnologia
rcaap.rightsopenAccesspt_PT
rcaap.typearticlept_PT
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relation.isAuthorOfPublication6d781c38-c45e-4159-b795-8c8675606160
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