EPR detection of Fe(V)=O active species in nonheme iron-catalyzed oxidations

Very recently, in situ cryospray-assisted variable temperature mass spectrometry (VT-MS) has been used to obtain the first convincing evidence for a HO-Fe-V=O intermediate in the catalyst system [((Me2)PyTACN) Fe-II(OTf)(2)] (4)/H2O2 ((Me2)PyTACN = 1-(2'-pyridylmethyl)-4,7-dimethyl-1,4,7-triaza...

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Detalles Bibliográficos
Autores: Lyakin, Oleg Y., Prat Casellas, Irene, Bryliakov, Konstantin P., Costas Salgueiro, Miquel, Talsi, Evgenii P.
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2012
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:10256/10176
Acceso en línea:http://hdl.handle.net/10256/10176
Access Level:acceso embargado
Palabra clave:Química bioinorgànica
Bioinorganic chemistry
Aigua oxigenada
Hydrogen peroxide
Mecanismes de reacció (Química)
Reaction mechanisms (Chemistry)
Peròxids -- Oxidació
Peroxides -- Oxidation
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spelling EPR detection of Fe(V)=O active species in nonheme iron-catalyzed oxidationsLyakin, Oleg Y.Prat Casellas, IreneBryliakov, Konstantin P.Costas Salgueiro, MiquelTalsi, Evgenii P.Química bioinorgànicaBioinorganic chemistryAigua oxigenadaHydrogen peroxideMecanismes de reacció (Química)Reaction mechanisms (Chemistry)Peròxids -- OxidacióPeroxides -- OxidationVery recently, in situ cryospray-assisted variable temperature mass spectrometry (VT-MS) has been used to obtain the first convincing evidence for a HO-Fe-V=O intermediate in the catalyst system [((Me2)PyTACN) Fe-II(OTf)(2)] (4)/H2O2 ((Me2)PyTACN = 1-(2'-pyridylmethyl)-4,7-dimethyl-1,4,7-triazacyclononane, OTf = OSO2CF3). The herein presented EPR spectroscopic study of the same system witnesses the formation of S = 1/2 reactive iron species. Its EPR parameters, in combination with its reactivity pattern toward cyclohexene and with independently obtained VT-MS data, allow for its reasonable assignment to the reactive [((Me2)PyTACN)Fe-V=O(OH)](2+) (4c) speciesThe authors thank the Russian Foundation for Basic Research, grants 12-03-31709 and 12-03-00782, for financial support. M.C. thanks MCYT (CTQ-2009-08864, and Consolider Ingenio CSD-2010-00065), ERC-2009-StG-239910, ICREA Academia Awards and SGR-239910ElsevierMinisterio de Ciencia e Innovación (Espanya)Ministerio de Ciencia y Tecnología (Espanya)infoinfo2012info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionapplication/pdfhttp://hdl.handle.net/10256/10176http://hdl.handle.net/10256/10176© Catalysis Communications, 2012, vol. 29, p. 105-108Articles publicats (D-Q)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)Inglésinfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.catcom.2012.09.029info:eu-repo/semantics/altIdentifier/issn/1566-7367MICINN/PN 2010-2016/CSD2010-00065MICYT/CTQ2009-08864info:eu-repo/grantAgreement/EC/FP7/239910Tots els drets reservatsinfo:eu-repo/semantics/embargoedAccessoai:recercat.cat:10256/101762026-05-29T05:05:01Z
dc.title.none.fl_str_mv EPR detection of Fe(V)=O active species in nonheme iron-catalyzed oxidations
title EPR detection of Fe(V)=O active species in nonheme iron-catalyzed oxidations
spellingShingle EPR detection of Fe(V)=O active species in nonheme iron-catalyzed oxidations
Lyakin, Oleg Y.
Química bioinorgànica
Bioinorganic chemistry
Aigua oxigenada
Hydrogen peroxide
Mecanismes de reacció (Química)
Reaction mechanisms (Chemistry)
Peròxids -- Oxidació
Peroxides -- Oxidation
title_short EPR detection of Fe(V)=O active species in nonheme iron-catalyzed oxidations
title_full EPR detection of Fe(V)=O active species in nonheme iron-catalyzed oxidations
title_fullStr EPR detection of Fe(V)=O active species in nonheme iron-catalyzed oxidations
title_full_unstemmed EPR detection of Fe(V)=O active species in nonheme iron-catalyzed oxidations
title_sort EPR detection of Fe(V)=O active species in nonheme iron-catalyzed oxidations
dc.creator.none.fl_str_mv Lyakin, Oleg Y.
Prat Casellas, Irene
Bryliakov, Konstantin P.
Costas Salgueiro, Miquel
Talsi, Evgenii P.
author Lyakin, Oleg Y.
author_facet Lyakin, Oleg Y.
Prat Casellas, Irene
Bryliakov, Konstantin P.
Costas Salgueiro, Miquel
Talsi, Evgenii P.
author_role author
author2 Prat Casellas, Irene
Bryliakov, Konstantin P.
Costas Salgueiro, Miquel
Talsi, Evgenii P.
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Ministerio de Ciencia e Innovación (Espanya)
Ministerio de Ciencia y Tecnología (Espanya)
dc.subject.none.fl_str_mv Química bioinorgànica
Bioinorganic chemistry
Aigua oxigenada
Hydrogen peroxide
Mecanismes de reacció (Química)
Reaction mechanisms (Chemistry)
Peròxids -- Oxidació
Peroxides -- Oxidation
topic Química bioinorgànica
Bioinorganic chemistry
Aigua oxigenada
Hydrogen peroxide
Mecanismes de reacció (Química)
Reaction mechanisms (Chemistry)
Peròxids -- Oxidació
Peroxides -- Oxidation
description Very recently, in situ cryospray-assisted variable temperature mass spectrometry (VT-MS) has been used to obtain the first convincing evidence for a HO-Fe-V=O intermediate in the catalyst system [((Me2)PyTACN) Fe-II(OTf)(2)] (4)/H2O2 ((Me2)PyTACN = 1-(2'-pyridylmethyl)-4,7-dimethyl-1,4,7-triazacyclononane, OTf = OSO2CF3). The herein presented EPR spectroscopic study of the same system witnesses the formation of S = 1/2 reactive iron species. Its EPR parameters, in combination with its reactivity pattern toward cyclohexene and with independently obtained VT-MS data, allow for its reasonable assignment to the reactive [((Me2)PyTACN)Fe-V=O(OH)](2+) (4c) species
publishDate 2012
dc.date.none.fl_str_mv 2012
info
info
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10256/10176
http://hdl.handle.net/10256/10176
url http://hdl.handle.net/10256/10176
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1016/j.catcom.2012.09.029
info:eu-repo/semantics/altIdentifier/issn/1566-7367
MICINN/PN 2010-2016/CSD2010-00065
MICYT/CTQ2009-08864
info:eu-repo/grantAgreement/EC/FP7/239910
dc.rights.none.fl_str_mv Tots els drets reservats
info:eu-repo/semantics/embargoedAccess
rights_invalid_str_mv Tots els drets reservats
eu_rights_str_mv embargoedAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Elsevier
publisher.none.fl_str_mv Elsevier
dc.source.none.fl_str_mv © Catalysis Communications, 2012, vol. 29, p. 105-108
Articles publicats (D-Q)
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.811543

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