Properties of (μ-Oxo)di-iron complexes and catalytic activity toward cyclohexane oxidation

Detalhes bibliográficos
Autor(a) principal: Parrilha,Gabrieli L.
Data de Publicação: 2010
Outros Autores: Ferreira,Sarah S., Fernandes,Christiane, Silva,Giselle C., Carvalho,Nakédia M. F., Antunes,O. A. C., Drago,Valderes, Bortoluzzi,Adailton J., Horn Jr.,Adolfo
Tipo de documento: Artigo
Idioma: eng
Título da fonte: Journal of the Brazilian Chemical Society (Online)
Texto Completo: http://old.scielo.br/scielo.php?script=sci_arttext&pid=S0103-50532010000400004
Resumo: We report herein the synthesis and characterization of two dinuclear μ-oxo iron compounds obtained through the reactions of FeSO4•7H2 O and FeCl3•6H2 O with 1-(bis-pyridin-2-ylmethyl-amino)-3-chloropropan-2-ol (L5), which resulted in the compounds [(SO4)(L5)Fe(μ-O)Fe(L5)(SO4 )]•6H2O, 1, and [Cl(L5)Fe(μ-O)Fe(L5)Cl]Cl2• 2H2O, 2. The electronic spectra of both compounds show absorption bands only in the UV range. The electrochemical analysis showed that the dinuclear unit is more stable under reduction in compound 1 than in compound 2, while the Mössbauer spectroscopy revealed that the monodentate ligands (sulfate and chloride) have a significant influence on the Mössbauer parameters determined for 1 and 2, particularly on the quadrupole splitting values. Both compounds were studied as catalysts in reactions of cyclohexane oxidation, using H2O2 and t-BuOOH as oxidants, in a substrate:oxidant:catalyst ratio of 1000:1000:1. Cyclohexanol, cyclohexanone, cyclohexyl hydroperoxide, t-butyl cyclohexyl peroxide and adipic acid were formed during the process. The experiments revealed that compound 2 is, in general, more active than compound 1 in promoting cyclohexane oxidation.
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spelling Properties of (μ-Oxo)di-iron complexes and catalytic activity toward cyclohexane oxidationdi-iron complexbridgemethane monooxygenasecyclohexane oxidationWe report herein the synthesis and characterization of two dinuclear μ-oxo iron compounds obtained through the reactions of FeSO4•7H2 O and FeCl3•6H2 O with 1-(bis-pyridin-2-ylmethyl-amino)-3-chloropropan-2-ol (L5), which resulted in the compounds [(SO4)(L5)Fe(μ-O)Fe(L5)(SO4 )]•6H2O, 1, and [Cl(L5)Fe(μ-O)Fe(L5)Cl]Cl2• 2H2O, 2. The electronic spectra of both compounds show absorption bands only in the UV range. The electrochemical analysis showed that the dinuclear unit is more stable under reduction in compound 1 than in compound 2, while the Mössbauer spectroscopy revealed that the monodentate ligands (sulfate and chloride) have a significant influence on the Mössbauer parameters determined for 1 and 2, particularly on the quadrupole splitting values. Both compounds were studied as catalysts in reactions of cyclohexane oxidation, using H2O2 and t-BuOOH as oxidants, in a substrate:oxidant:catalyst ratio of 1000:1000:1. Cyclohexanol, cyclohexanone, cyclohexyl hydroperoxide, t-butyl cyclohexyl peroxide and adipic acid were formed during the process. The experiments revealed that compound 2 is, in general, more active than compound 1 in promoting cyclohexane oxidation.Sociedade Brasileira de Química2010-01-01info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersiontext/htmlhttp://old.scielo.br/scielo.php?script=sci_arttext&pid=S0103-50532010000400004Journal of the Brazilian Chemical Society v.21 n.4 2010reponame:Journal of the Brazilian Chemical Society (Online)instname:Sociedade Brasileira de Química (SBQ)instacron:SBQ10.1590/S0103-50532010000400004info:eu-repo/semantics/openAccessParrilha,Gabrieli L.Ferreira,Sarah S.Fernandes,ChristianeSilva,Giselle C.Carvalho,Nakédia M. F.Antunes,O. A. C.Drago,ValderesBortoluzzi,Adailton J.Horn Jr.,Adolfoeng2010-05-21T00:00:00Zoai:scielo:S0103-50532010000400004Revistahttp://jbcs.sbq.org.brONGhttps://old.scielo.br/oai/scielo-oai.php||office@jbcs.sbq.org.br1678-47900103-5053opendoar:2010-05-21T00:00Journal of the Brazilian Chemical Society (Online) - Sociedade Brasileira de Química (SBQ)false
dc.title.none.fl_str_mv Properties of (μ-Oxo)di-iron complexes and catalytic activity toward cyclohexane oxidation
title Properties of (μ-Oxo)di-iron complexes and catalytic activity toward cyclohexane oxidation
spellingShingle Properties of (μ-Oxo)di-iron complexes and catalytic activity toward cyclohexane oxidation
Parrilha,Gabrieli L.
di-iron complex
bridge
methane monooxygenase
cyclohexane oxidation
title_short Properties of (μ-Oxo)di-iron complexes and catalytic activity toward cyclohexane oxidation
title_full Properties of (μ-Oxo)di-iron complexes and catalytic activity toward cyclohexane oxidation
title_fullStr Properties of (μ-Oxo)di-iron complexes and catalytic activity toward cyclohexane oxidation
title_full_unstemmed Properties of (μ-Oxo)di-iron complexes and catalytic activity toward cyclohexane oxidation
title_sort Properties of (μ-Oxo)di-iron complexes and catalytic activity toward cyclohexane oxidation
author Parrilha,Gabrieli L.
author_facet Parrilha,Gabrieli L.
Ferreira,Sarah S.
Fernandes,Christiane
Silva,Giselle C.
Carvalho,Nakédia M. F.
Antunes,O. A. C.
Drago,Valderes
Bortoluzzi,Adailton J.
Horn Jr.,Adolfo
author_role author
author2 Ferreira,Sarah S.
Fernandes,Christiane
Silva,Giselle C.
Carvalho,Nakédia M. F.
Antunes,O. A. C.
Drago,Valderes
Bortoluzzi,Adailton J.
Horn Jr.,Adolfo
author2_role author
author
author
author
author
author
author
author
dc.contributor.author.fl_str_mv Parrilha,Gabrieli L.
Ferreira,Sarah S.
Fernandes,Christiane
Silva,Giselle C.
Carvalho,Nakédia M. F.
Antunes,O. A. C.
Drago,Valderes
Bortoluzzi,Adailton J.
Horn Jr.,Adolfo
dc.subject.por.fl_str_mv di-iron complex
bridge
methane monooxygenase
cyclohexane oxidation
topic di-iron complex
bridge
methane monooxygenase
cyclohexane oxidation
description We report herein the synthesis and characterization of two dinuclear μ-oxo iron compounds obtained through the reactions of FeSO4•7H2 O and FeCl3•6H2 O with 1-(bis-pyridin-2-ylmethyl-amino)-3-chloropropan-2-ol (L5), which resulted in the compounds [(SO4)(L5)Fe(μ-O)Fe(L5)(SO4 )]•6H2O, 1, and [Cl(L5)Fe(μ-O)Fe(L5)Cl]Cl2• 2H2O, 2. The electronic spectra of both compounds show absorption bands only in the UV range. The electrochemical analysis showed that the dinuclear unit is more stable under reduction in compound 1 than in compound 2, while the Mössbauer spectroscopy revealed that the monodentate ligands (sulfate and chloride) have a significant influence on the Mössbauer parameters determined for 1 and 2, particularly on the quadrupole splitting values. Both compounds were studied as catalysts in reactions of cyclohexane oxidation, using H2O2 and t-BuOOH as oxidants, in a substrate:oxidant:catalyst ratio of 1000:1000:1. Cyclohexanol, cyclohexanone, cyclohexyl hydroperoxide, t-butyl cyclohexyl peroxide and adipic acid were formed during the process. The experiments revealed that compound 2 is, in general, more active than compound 1 in promoting cyclohexane oxidation.
publishDate 2010
dc.date.none.fl_str_mv 2010-01-01
dc.type.driver.fl_str_mv info:eu-repo/semantics/article
dc.type.status.fl_str_mv info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.uri.fl_str_mv http://old.scielo.br/scielo.php?script=sci_arttext&pid=S0103-50532010000400004
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dc.language.iso.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv 10.1590/S0103-50532010000400004
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dc.publisher.none.fl_str_mv Sociedade Brasileira de Química
publisher.none.fl_str_mv Sociedade Brasileira de Química
dc.source.none.fl_str_mv Journal of the Brazilian Chemical Society v.21 n.4 2010
reponame:Journal of the Brazilian Chemical Society (Online)
instname:Sociedade Brasileira de Química (SBQ)
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reponame_str Journal of the Brazilian Chemical Society (Online)
collection Journal of the Brazilian Chemical Society (Online)
repository.name.fl_str_mv Journal of the Brazilian Chemical Society (Online) - Sociedade Brasileira de Química (SBQ)
repository.mail.fl_str_mv ||office@jbcs.sbq.org.br
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