Repository logo
 
Publication

Cyclohexane oxidation with dioxygen catalyzed by supported pyrazole rhenium complexes

2008-04-18Journal article Restricted access
Simple item page
dc.contributor.authorMishra, Gopal S.
dc.contributor.authorAlegria, Elisabete
dc.contributor.authorMartins, Luisa
dc.contributor.authorFraústo Da Silva, João
dc.contributor.authorPombeiro, Armando
dc.date.accessioned2020-07-21T13:49:33Z
dc.date.available2020-07-21T13:49:33Z
dc.date.issued2008-04-18
dc.description.abstractThe pyrazole complexes [ReCl2{N2C(O)Ph}(Hpz)(PPh3)2] 2 (Hpz = pyrazole), [ReCl2{N2C(O)Ph}(Hpz)2(PPh3)] 3 and [ReClF{N2C(O)Ph}(Hpz)2(PPh3)] 4, and their precursor [ReOCl3(PPh3)2] 1, immobilized on 3-aminopropyl functionalized silica, catalyze the cyclohexane oxidation with dioxygen, to cyclohexanol and cyclohexanone (the main product), in the absence of solvent and additives and under relatively mild conditions. Complex 4, whose synthesis and characterization are reported herein for the first time, provides the best activity (ca. 16% overall conversion towards the ketone and alcohol, at the O2 pressure of 19 atm, at 150 °C, 8 h reaction time). The reaction is further promoted by pyrazinecarboxylic acid. TGA analysis shows that the supported complexes are stable up to ca. 200 °C. The use of radical traps supports the involvement of a free-radical mechanism via carbon- and oxygen-centred radicals. The effects of various factors were studied towards the optimization of the processes. Complex 4 also catalyzes the oxidation of other cycloalkanes to the corresponding cycloalkanols and cycloalkanones.pt_PT
dc.description.versioninfo:eu-repo/semantics/publishedVersionpt_PT
dc.identifier.citationMISHRA, Gopal S.; [et al] – Cyclohexane oxidation with dioxygen catalyzed by supported pyrazole rhenium complexes. Journal of Molecular Catalysis A: Chemical. ISSN 1381-1169. Vol. 285, N.º 1-2 (2008), pp. 92-100pt_PT
dc.identifier.doi10.1016/j.molcata.2008.01.022pt_PT
dc.identifier.issn1381-1169
dc.identifier.urihttp://hdl.handle.net/10400.21/12072
dc.language.isoengpt_PT
dc.peerreviewedyespt_PT
dc.publisherElsevierpt_PT
dc.relation.publisherversionhttps://pdf.sciencedirectassets.com/271358/1-s2.0-S1381116908X00044/1-s2.0-S1381116908000514/main.pdf?X-Amz-Date=20200721T133452Z&X-Amz-Algorithm=AWS4-HMAC-SHA256&X-Amz-Signature=09f2a0f3872cddd1acb8f0f90e2b345ad29840dac595347c47142a54fdadc096&X-Amz-Credential=ASIAQ3PHCVTYYIAB4RNC%2F20200721%2Fus-east-1%2Fs3%2Faws4_request&type=client&tid=prr-394ced51-a1e7-4009-a4ee-e9c8e3e58291&sid=8a88f6178de3764c2498ecf27a50dd60f553gxrqb&pii=S1381116908000514&X-Amz-SignedHeaders=host&X-Amz-Security-Token=IQoJb3JpZ2luX2VjEI3%2F%2F%2F%2F%2F%2F%2F%2F%2F%2FwEaCXVzLWVhc3QtMSJHMEUCIQCBe70oQB3OkDWrZ%2BlTgYEGuIWBW0PJwjb6xKgt4RIDcAIgfpZi5%2B%2FNMRgd9LAH8v6abUCHgHFBCCdv6dnkMNKAptQqtAMIRhADGgwwNTkwMDM1NDY4NjUiDIJTrJMqR2jWjRLYciqRA4Oj9M7niGvuEZCClvLY3VktFh%2BQqHnDqtI99GNs2xxOkqoEGbrNT26QhBmhIk0JJmhWhWGlRuJbrjQkq83I6m61%2B6L0ggGTWHxEc3WpNhMn69uT9tTinvteecwf7yIjTJ3g2pxlEnmGYobwF0CcImlqjISc2210BgAp90l4Q%2Bm08Ur0Vaxcf%2FPJuB7h1cBT0LHklPtCrLzKB5AMMFqG4hZZii%2BW1zOkd9igS3VszF1bla%2BQvYcwCQdjhJQF922JmRVyPhC12Ub0I1oRc0xYSfD%2FAG%2BYWRWL%2FD57yUkYQRGhRM5b3kdb4T1I%2FAfcRhohVDctzFKF2UHjMBatHbIdGSmt%2BpX7xzjX1hEeIWiVwznRblklgepHOTL3%2FNB%2FqJ1yEsfOfWVKYq0jFV2P5Wrd%2BrmUGz939JotNCVg9S%2B6a6gD%2F6zoDDMa9TSPMXcBX5uDitbsY%2FA8vi1B1RIcqFf%2BE%2Bc7itSpiVXOL73RGT6JT7E1YLcDiOHLliniOIRHXB1QhQ2bwsNAqrOBPzlPq0q7aGEcMLy82%2FgFOusBfzgFXHoIFiGh7r1RG7wxToy7w4gWJ8qLd9gkTu706DuIuBLQ2rDhKeXDvV8CPkeVWxtCFFrel0KzpqWMhW2h7QwKr5Jdk9zZMjvT1dO3Lshd%2BUbV2KCeKR3hQJbb6L75oG4pmdvU06VKw2gwYfvSwVfIfO0rODalO0rhGKjvX4mORNR7JnDHgP6Oip7gRmmDQhhEHVQF%2Fv71%2Fr7lvxBC%2B2rvupXwnDbvf9dc5VhvZCCBqTdlUMOqkjljb9ccFwE6sbPFnyngrkSWSddURhXLTiPUR4VqDXwpNcyHGtJ7AZMKFxXn0y1qX9wd6w%3D%3D&host=68042c943591013ac2b2430a89b270f6af2c76d8dfd086a07176afe7c76c2c61&X-Amz-Expires=300&hash=00866b52183977dc776aead738a561efff45dc7869329386f6287b3782b2d6abpt_PT
dc.subjectRheniumpt_PT
dc.subjectCyclohexanept_PT
dc.subjectDioxygenpt_PT
dc.subjectCarboxylic acidspt_PT
dc.subjectRadical mechanismpt_PT
dc.subjectCyclohexanolpt_PT
dc.subjectCyclohexanonept_PT
dc.titleCyclohexane oxidation with dioxygen catalyzed by supported pyrazole rhenium complexespt_PT
dc.typejournal article
dspace.entity.typePublication
oaire.citation.endPage100pt_PT
oaire.citation.issue1-2pt_PT
oaire.citation.startPage92pt_PT
oaire.citation.titleJournal of Molecular Catalysis A: Chemicalpt_PT
oaire.citation.volume285pt_PT
person.familyNameMishra
person.familyNameAlegria
person.familyNameMartins
person.familyNameFraústo da Silva
person.familyNamePombeiro
person.givenNameGopal
person.givenNameElisabete
person.givenNameLuisa
person.givenNameJoão
person.givenNameArmando
person.identifier863202
person.identifier637885
person.identifier.ciencia-id4814-2CD6-F93E
person.identifier.ciencia-id8C1F-851A-9F1C
person.identifier.ciencia-idE218-E297-A4EA
person.identifier.ciencia-id8311-38FA-CEFB
person.identifier.orcid0000-0001-6566-7218
person.identifier.orcid0000-0003-4060-1057
person.identifier.orcid0000-0002-5403-9352
person.identifier.orcid0000-0001-8367-7276
person.identifier.orcid0000-0001-8323-888X
person.identifier.ridE-9945-2012
person.identifier.ridG-6210-2011
person.identifier.ridF-8346-2014
person.identifier.ridI-5945-2012
person.identifier.scopus-author-id7102625692
person.identifier.scopus-author-id8315848300
person.identifier.scopus-author-id8650947800
person.identifier.scopus-author-id6701716473
person.identifier.scopus-author-id7006067269
rcaap.rightsclosedAccesspt_PT
rcaap.typearticlept_PT
relation.isAuthorOfPublication4199db96-cf5b-48ba-9176-8adba9e3f452
relation.isAuthorOfPublication6d781c38-c45e-4159-b795-8c8675606160
relation.isAuthorOfPublication8ed70b09-b4d3-4a5d-9f75-12b13a332204
relation.isAuthorOfPublication60210cdc-b56f-472f-af65-a69c515e19e3
relation.isAuthorOfPublication6d18ff2e-5c33-4010-b1e7-964c72349813
relation.isAuthorOfPublication.latestForDiscovery6d18ff2e-5c33-4010-b1e7-964c72349813

Files

Original bundle
Now showing 1 - 1 of 1
No Thumbnail Available
Name:
Cyclohexane_ECBAAlegria.pdf
Size:
639.47 KB
Format:
Adobe Portable Document Format
Download

Collections

ISEL - Eng. Quim. Biol. - Artigos