Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compounds

Autores
Bari, Sara Elizabeth; Amorebieta, Valentín Tomás; Gutierrez, Maria Marta; Olabe, José A.; Doctorovich, Fabio
Año de publicación
2010
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The reactions of hydroxylamine (HA) with several water-soluble iron(III) porphyrinate compounds, namely iron(III) meso-tetrakis-(N-ethylpyridinium-2yl)-porphyrinate ([FeIII(TEPyP)]5+), iron(III) meso-tetrakis-(4-sulphonatophenyl)-porphyrinate ([FeIII(TPPS)]3), and microperoxidase 11 ([FeIII(MP11)]) were studied for different [FeIII(Porph)]/[HA] ratios, under anaerobic conditions at neutral pH. Efficient catalytic processes leading to the disproportionation of HA by these iron(III) porphyrinates were evidenced for the first time. As a common feature, only N2 and N2O were found as gaseous, nitrogen-containing oxidation products, while NH3 was the unique reduced species detected. Different N2/N2O ratios obtained with these three porphyrinates strongly suggest distinctive mechanistic scenarios: while [FeIII(TEPyP)]5+ and [FeIII(MP11)] formed unknown steady-state porphyrinic intermediates in the presence of HA, [FeIII(TPPS)]3 led to the well characterized soluble intermediate, [FeII(TPPS)NO]4. Free-radical formation was only evidenced for [FeIII(TEPyP)]5+, as a consequence of a metal centered reduction. We discuss the catalytic pathways of HA disproportionation on the basis of the distribution of gaseous products, free radicals formation, the nature of porphyrinic intermediates, the FeII/FeIII redox potential, the coordinating capabilities of each complex, and the kinetic analysis. The absence of NO 2 revealed either that no HAO-like activity was operative under our reaction conditions, or that NO 2 , if formed, was consumed in the reaction milieu.
Fil: Bari, Sara Elizabeth. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Amorebieta, Valentín Tomás. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Gutierrez, Maria Marta. Universidad Nacional de Mar del Plata. Facultad de Ciencias Exactas y Naturales. Departamento de Química; Argentina
Fil: Olabe, José A.. Universidad Nacional de Mar del Plata. Facultad de Ciencias Exactas y Naturales. Departamento de Química; Argentina
Fil: Doctorovich, Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Materia
Hydroxylamine
Iron(III) porphyrinates
Catalysis
Nitrogen metabolism
Iron(III) microperoxidase 11
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/280558
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/280558
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compoundsBari, Sara ElizabethAmorebieta, Valentín TomásGutierrez, Maria MartaOlabe, José A.Doctorovich, FabioHydroxylamineIron(III) porphyrinatesCatalysisNitrogen metabolismIron(III) microperoxidase 11https://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The reactions of hydroxylamine (HA) with several water-soluble iron(III) porphyrinate compounds, namely iron(III) meso-tetrakis-(N-ethylpyridinium-2yl)-porphyrinate ([FeIII(TEPyP)]5+), iron(III) meso-tetrakis-(4-sulphonatophenyl)-porphyrinate ([FeIII(TPPS)]3), and microperoxidase 11 ([FeIII(MP11)]) were studied for different [FeIII(Porph)]/[HA] ratios, under anaerobic conditions at neutral pH. Efficient catalytic processes leading to the disproportionation of HA by these iron(III) porphyrinates were evidenced for the first time. As a common feature, only N2 and N2O were found as gaseous, nitrogen-containing oxidation products, while NH3 was the unique reduced species detected. Different N2/N2O ratios obtained with these three porphyrinates strongly suggest distinctive mechanistic scenarios: while [FeIII(TEPyP)]5+ and [FeIII(MP11)] formed unknown steady-state porphyrinic intermediates in the presence of HA, [FeIII(TPPS)]3 led to the well characterized soluble intermediate, [FeII(TPPS)NO]4. Free-radical formation was only evidenced for [FeIII(TEPyP)]5+, as a consequence of a metal centered reduction. We discuss the catalytic pathways of HA disproportionation on the basis of the distribution of gaseous products, free radicals formation, the nature of porphyrinic intermediates, the FeII/FeIII redox potential, the coordinating capabilities of each complex, and the kinetic analysis. The absence of NO 2 revealed either that no HAO-like activity was operative under our reaction conditions, or that NO 2 , if formed, was consumed in the reaction milieu.Fil: Bari, Sara Elizabeth. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaFil: Amorebieta, Valentín Tomás. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaFil: Gutierrez, Maria Marta. Universidad Nacional de Mar del Plata. Facultad de Ciencias Exactas y Naturales. Departamento de Química; ArgentinaFil: Olabe, José A.. Universidad Nacional de Mar del Plata. Facultad de Ciencias Exactas y Naturales. Departamento de Química; ArgentinaFil: Doctorovich, Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaElsevier Science Inc.2010-01info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/280558Bari, Sara Elizabeth; Amorebieta, Valentín Tomás; Gutierrez, Maria Marta; Olabe, José A.; Doctorovich, Fabio; Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compounds; Elsevier Science Inc.; Journal of Inorganic Biochemistry; 104; 1; 1-2010; 30-360162-0134CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/abs/pii/S0162013409002451info:eu-repo/semantics/altIdentifier/doi/10.1016/j.jinorgbio.2009.09.024info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2026-02-11T12:17:30Zoai:ri.conicet.gov.ar:11336/280558instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982026-02-11 12:17:30.835CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compounds
title Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compounds
spellingShingle Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compounds
Bari, Sara Elizabeth
Hydroxylamine
Iron(III) porphyrinates
Catalysis
Nitrogen metabolism
Iron(III) microperoxidase 11
title_short Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compounds
title_full Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compounds
title_fullStr Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compounds
title_full_unstemmed Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compounds
title_sort Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compounds
dc.creator.none.fl_str_mv Bari, Sara Elizabeth
Amorebieta, Valentín Tomás
Gutierrez, Maria Marta
Olabe, José A.
Doctorovich, Fabio
author Bari, Sara Elizabeth
author_facet Bari, Sara Elizabeth
Amorebieta, Valentín Tomás
Gutierrez, Maria Marta
Olabe, José A.
Doctorovich, Fabio
author_role author
author2 Amorebieta, Valentín Tomás
Gutierrez, Maria Marta
Olabe, José A.
Doctorovich, Fabio
author2_role author
author
author
author
dc.subject.none.fl_str_mv Hydroxylamine
Iron(III) porphyrinates
Catalysis
Nitrogen metabolism
Iron(III) microperoxidase 11
topic Hydroxylamine
Iron(III) porphyrinates
Catalysis
Nitrogen metabolism
Iron(III) microperoxidase 11
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The reactions of hydroxylamine (HA) with several water-soluble iron(III) porphyrinate compounds, namely iron(III) meso-tetrakis-(N-ethylpyridinium-2yl)-porphyrinate ([FeIII(TEPyP)]5+), iron(III) meso-tetrakis-(4-sulphonatophenyl)-porphyrinate ([FeIII(TPPS)]3), and microperoxidase 11 ([FeIII(MP11)]) were studied for different [FeIII(Porph)]/[HA] ratios, under anaerobic conditions at neutral pH. Efficient catalytic processes leading to the disproportionation of HA by these iron(III) porphyrinates were evidenced for the first time. As a common feature, only N2 and N2O were found as gaseous, nitrogen-containing oxidation products, while NH3 was the unique reduced species detected. Different N2/N2O ratios obtained with these three porphyrinates strongly suggest distinctive mechanistic scenarios: while [FeIII(TEPyP)]5+ and [FeIII(MP11)] formed unknown steady-state porphyrinic intermediates in the presence of HA, [FeIII(TPPS)]3 led to the well characterized soluble intermediate, [FeII(TPPS)NO]4. Free-radical formation was only evidenced for [FeIII(TEPyP)]5+, as a consequence of a metal centered reduction. We discuss the catalytic pathways of HA disproportionation on the basis of the distribution of gaseous products, free radicals formation, the nature of porphyrinic intermediates, the FeII/FeIII redox potential, the coordinating capabilities of each complex, and the kinetic analysis. The absence of NO 2 revealed either that no HAO-like activity was operative under our reaction conditions, or that NO 2 , if formed, was consumed in the reaction milieu.
Fil: Bari, Sara Elizabeth. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Amorebieta, Valentín Tomás. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Gutierrez, Maria Marta. Universidad Nacional de Mar del Plata. Facultad de Ciencias Exactas y Naturales. Departamento de Química; Argentina
Fil: Olabe, José A.. Universidad Nacional de Mar del Plata. Facultad de Ciencias Exactas y Naturales. Departamento de Química; Argentina
Fil: Doctorovich, Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
description The reactions of hydroxylamine (HA) with several water-soluble iron(III) porphyrinate compounds, namely iron(III) meso-tetrakis-(N-ethylpyridinium-2yl)-porphyrinate ([FeIII(TEPyP)]5+), iron(III) meso-tetrakis-(4-sulphonatophenyl)-porphyrinate ([FeIII(TPPS)]3), and microperoxidase 11 ([FeIII(MP11)]) were studied for different [FeIII(Porph)]/[HA] ratios, under anaerobic conditions at neutral pH. Efficient catalytic processes leading to the disproportionation of HA by these iron(III) porphyrinates were evidenced for the first time. As a common feature, only N2 and N2O were found as gaseous, nitrogen-containing oxidation products, while NH3 was the unique reduced species detected. Different N2/N2O ratios obtained with these three porphyrinates strongly suggest distinctive mechanistic scenarios: while [FeIII(TEPyP)]5+ and [FeIII(MP11)] formed unknown steady-state porphyrinic intermediates in the presence of HA, [FeIII(TPPS)]3 led to the well characterized soluble intermediate, [FeII(TPPS)NO]4. Free-radical formation was only evidenced for [FeIII(TEPyP)]5+, as a consequence of a metal centered reduction. We discuss the catalytic pathways of HA disproportionation on the basis of the distribution of gaseous products, free radicals formation, the nature of porphyrinic intermediates, the FeII/FeIII redox potential, the coordinating capabilities of each complex, and the kinetic analysis. The absence of NO 2 revealed either that no HAO-like activity was operative under our reaction conditions, or that NO 2 , if formed, was consumed in the reaction milieu.
publishDate 2010
dc.date.none.fl_str_mv 2010-01
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/280558
Bari, Sara Elizabeth; Amorebieta, Valentín Tomás; Gutierrez, Maria Marta; Olabe, José A.; Doctorovich, Fabio; Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compounds; Elsevier Science Inc.; Journal of Inorganic Biochemistry; 104; 1; 1-2010; 30-36
0162-0134
CONICET Digital
CONICET
url http://hdl.handle.net/11336/280558
identifier_str_mv Bari, Sara Elizabeth; Amorebieta, Valentín Tomás; Gutierrez, Maria Marta; Olabe, José A.; Doctorovich, Fabio; Disproportionation of hydroxylamine by water-soluble iron(III) porphyrinate compounds; Elsevier Science Inc.; Journal of Inorganic Biochemistry; 104; 1; 1-2010; 30-36
0162-0134
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/abs/pii/S0162013409002451
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.jinorgbio.2009.09.024
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier Science Inc.
publisher.none.fl_str_mv Elsevier Science Inc.
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 12.930639

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