Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionati...

Autores
Palopoli, Claudia Marcela; Bruzzo, Natalia; Hureau, Christelle; Ladeira, Sonia; Murgida, Daniel Horacio; Signorella, Sandra Rosanna
Año de publicación
2011
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
A new diMn III complex, Na[Mn 2(3-Me-5-SO 3-salpentO)(μ-MeO)(μ-AcO)(H 2O)]•4H 2O(1), where salpentOH = 1,5-bis(salicylidenamino) pentan-3-ol, was synthesized and structurally characterized. The complex possesses a bis(μ-alkoxo)(μ-acetato) triply bridged diMn III core, the structure of which is retained upon dissolution. Complex 1 is highly efficient to disproportionate H2O2 in an aqueous solution of pH ≥ 8.5 or in DMF, with only a slight decrease of activity. Electrospray ionization mass spectrometry, EPR, and UV-vis spectroscopy used to monitor the H2O2 disproportionation in buffered basic medium, suggest that the major active form of the catalyst during cycling occurs in the Mn III 2 oxidation state and that the starting complex retains the dinuclearity and composition during catalysis, with the acetate that moves from bridging to terminal ligand. UV-vis and Raman spectroscopy of H 2O 2 + 1 + Bu 4NOH mixtures in DMF suggest that the catalytic cycle involves Mn III 2/Mn IV 2 oxidation levels. At pH 10.6 in an Et 3N/Et 3NH + buffer, complex 1 catalyzes dismutation of H2O2 with saturation kinetics on the substrate, first order dependence on the catalyst, and k cat/K M = 16(1) ×10 2 s -1 M -1. During catalysis, the exogenous base contributes to retain the integrity of the bis(μ-alkoxo) doubly bridged diMn core and favors the formation of the catalyst-peroxide adduct (low value of K M), rendering 1 a highly efficient catalyst for H2O2 disproportionation.
Fil: Palopoli, Claudia Marcela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Química Rosario. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario; Argentina. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmaceuticas. Departamento de Química y Física; Argentina
Fil: Bruzzo, Natalia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Química Rosario. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario; Argentina. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmaceuticas. Departamento de Química y Física; Argentina
Fil: Hureau, Christelle. Centre National de la Recherche Scientifique; Francia. Université Paul Sabatier; Francia. Institut National Polytechnique de Toulouse; Francia
Fil: Ladeira, Sonia. Centre National de la Recherche Scientifique; Francia. Université Paul Sabatier; Francia. Institut de Chimie de Toulouse; Francia. Institut National Polytechnique de Toulouse; Francia
Fil: Murgida, Daniel Horacio. 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. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; Argentina
Fil: Signorella, Sandra Rosanna. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Química Rosario. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario; Argentina. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmaceuticas. Departamento de Química y Física; Argentina
Materia
Water soluble manganese complex
Schiff base ligand
Catalase-like activity
Mechanism
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:11336/127242

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network_name_str CONICET Digital (CONICET)
spelling Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionationPalopoli, Claudia MarcelaBruzzo, NataliaHureau, ChristelleLadeira, SoniaMurgida, Daniel HoracioSignorella, Sandra RosannaWater soluble manganese complexSchiff base ligandCatalase-like activityMechanismhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1A new diMn III complex, Na[Mn 2(3-Me-5-SO 3-salpentO)(μ-MeO)(μ-AcO)(H 2O)]•4H 2O(1), where salpentOH = 1,5-bis(salicylidenamino) pentan-3-ol, was synthesized and structurally characterized. The complex possesses a bis(μ-alkoxo)(μ-acetato) triply bridged diMn III core, the structure of which is retained upon dissolution. Complex 1 is highly efficient to disproportionate H2O2 in an aqueous solution of pH ≥ 8.5 or in DMF, with only a slight decrease of activity. Electrospray ionization mass spectrometry, EPR, and UV-vis spectroscopy used to monitor the H2O2 disproportionation in buffered basic medium, suggest that the major active form of the catalyst during cycling occurs in the Mn III 2 oxidation state and that the starting complex retains the dinuclearity and composition during catalysis, with the acetate that moves from bridging to terminal ligand. UV-vis and Raman spectroscopy of H 2O 2 + 1 + Bu 4NOH mixtures in DMF suggest that the catalytic cycle involves Mn III 2/Mn IV 2 oxidation levels. At pH 10.6 in an Et 3N/Et 3NH + buffer, complex 1 catalyzes dismutation of H2O2 with saturation kinetics on the substrate, first order dependence on the catalyst, and k cat/K M = 16(1) ×10 2 s -1 M -1. During catalysis, the exogenous base contributes to retain the integrity of the bis(μ-alkoxo) doubly bridged diMn core and favors the formation of the catalyst-peroxide adduct (low value of K M), rendering 1 a highly efficient catalyst for H2O2 disproportionation.Fil: Palopoli, Claudia Marcela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Química Rosario. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario; Argentina. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmaceuticas. Departamento de Química y Física; ArgentinaFil: Bruzzo, Natalia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Química Rosario. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario; Argentina. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmaceuticas. Departamento de Química y Física; ArgentinaFil: Hureau, Christelle. Centre National de la Recherche Scientifique; Francia. Université Paul Sabatier; Francia. Institut National Polytechnique de Toulouse; FranciaFil: Ladeira, Sonia. Centre National de la Recherche Scientifique; Francia. Université Paul Sabatier; Francia. Institut de Chimie de Toulouse; Francia. Institut National Polytechnique de Toulouse; FranciaFil: Murgida, Daniel Horacio. 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. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; ArgentinaFil: Signorella, Sandra Rosanna. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Química Rosario. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario; Argentina. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmaceuticas. Departamento de Química y Física; ArgentinaAmerican Chemical Society2011-09info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/127242Palopoli, Claudia Marcela; Bruzzo, Natalia; Hureau, Christelle; Ladeira, Sonia; Murgida, Daniel Horacio; et al.; Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionation; American Chemical Society; Inorganic Chemistry; 50; 18; 9-2011; 8973-89830020-1669CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/pdf/10.1021/ic2011452info:eu-repo/semantics/altIdentifier/doi/10.1021/ic2011452info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:41:18Zoai:ri.conicet.gov.ar:11336/127242instacron: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:34982025-09-29 09:41:18.788CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionation
title Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionation
spellingShingle Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionation
Palopoli, Claudia Marcela
Water soluble manganese complex
Schiff base ligand
Catalase-like activity
Mechanism
title_short Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionation
title_full Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionation
title_fullStr Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionation
title_full_unstemmed Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionation
title_sort Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionation
dc.creator.none.fl_str_mv Palopoli, Claudia Marcela
Bruzzo, Natalia
Hureau, Christelle
Ladeira, Sonia
Murgida, Daniel Horacio
Signorella, Sandra Rosanna
author Palopoli, Claudia Marcela
author_facet Palopoli, Claudia Marcela
Bruzzo, Natalia
Hureau, Christelle
Ladeira, Sonia
Murgida, Daniel Horacio
Signorella, Sandra Rosanna
author_role author
author2 Bruzzo, Natalia
Hureau, Christelle
Ladeira, Sonia
Murgida, Daniel Horacio
Signorella, Sandra Rosanna
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Water soluble manganese complex
Schiff base ligand
Catalase-like activity
Mechanism
topic Water soluble manganese complex
Schiff base ligand
Catalase-like activity
Mechanism
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv A new diMn III complex, Na[Mn 2(3-Me-5-SO 3-salpentO)(μ-MeO)(μ-AcO)(H 2O)]•4H 2O(1), where salpentOH = 1,5-bis(salicylidenamino) pentan-3-ol, was synthesized and structurally characterized. The complex possesses a bis(μ-alkoxo)(μ-acetato) triply bridged diMn III core, the structure of which is retained upon dissolution. Complex 1 is highly efficient to disproportionate H2O2 in an aqueous solution of pH ≥ 8.5 or in DMF, with only a slight decrease of activity. Electrospray ionization mass spectrometry, EPR, and UV-vis spectroscopy used to monitor the H2O2 disproportionation in buffered basic medium, suggest that the major active form of the catalyst during cycling occurs in the Mn III 2 oxidation state and that the starting complex retains the dinuclearity and composition during catalysis, with the acetate that moves from bridging to terminal ligand. UV-vis and Raman spectroscopy of H 2O 2 + 1 + Bu 4NOH mixtures in DMF suggest that the catalytic cycle involves Mn III 2/Mn IV 2 oxidation levels. At pH 10.6 in an Et 3N/Et 3NH + buffer, complex 1 catalyzes dismutation of H2O2 with saturation kinetics on the substrate, first order dependence on the catalyst, and k cat/K M = 16(1) ×10 2 s -1 M -1. During catalysis, the exogenous base contributes to retain the integrity of the bis(μ-alkoxo) doubly bridged diMn core and favors the formation of the catalyst-peroxide adduct (low value of K M), rendering 1 a highly efficient catalyst for H2O2 disproportionation.
Fil: Palopoli, Claudia Marcela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Química Rosario. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario; Argentina. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmaceuticas. Departamento de Química y Física; Argentina
Fil: Bruzzo, Natalia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Química Rosario. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario; Argentina. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmaceuticas. Departamento de Química y Física; Argentina
Fil: Hureau, Christelle. Centre National de la Recherche Scientifique; Francia. Université Paul Sabatier; Francia. Institut National Polytechnique de Toulouse; Francia
Fil: Ladeira, Sonia. Centre National de la Recherche Scientifique; Francia. Université Paul Sabatier; Francia. Institut de Chimie de Toulouse; Francia. Institut National Polytechnique de Toulouse; Francia
Fil: Murgida, Daniel Horacio. 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. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; Argentina
Fil: Signorella, Sandra Rosanna. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Química Rosario. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario; Argentina. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmaceuticas. Departamento de Química y Física; Argentina
description A new diMn III complex, Na[Mn 2(3-Me-5-SO 3-salpentO)(μ-MeO)(μ-AcO)(H 2O)]•4H 2O(1), where salpentOH = 1,5-bis(salicylidenamino) pentan-3-ol, was synthesized and structurally characterized. The complex possesses a bis(μ-alkoxo)(μ-acetato) triply bridged diMn III core, the structure of which is retained upon dissolution. Complex 1 is highly efficient to disproportionate H2O2 in an aqueous solution of pH ≥ 8.5 or in DMF, with only a slight decrease of activity. Electrospray ionization mass spectrometry, EPR, and UV-vis spectroscopy used to monitor the H2O2 disproportionation in buffered basic medium, suggest that the major active form of the catalyst during cycling occurs in the Mn III 2 oxidation state and that the starting complex retains the dinuclearity and composition during catalysis, with the acetate that moves from bridging to terminal ligand. UV-vis and Raman spectroscopy of H 2O 2 + 1 + Bu 4NOH mixtures in DMF suggest that the catalytic cycle involves Mn III 2/Mn IV 2 oxidation levels. At pH 10.6 in an Et 3N/Et 3NH + buffer, complex 1 catalyzes dismutation of H2O2 with saturation kinetics on the substrate, first order dependence on the catalyst, and k cat/K M = 16(1) ×10 2 s -1 M -1. During catalysis, the exogenous base contributes to retain the integrity of the bis(μ-alkoxo) doubly bridged diMn core and favors the formation of the catalyst-peroxide adduct (low value of K M), rendering 1 a highly efficient catalyst for H2O2 disproportionation.
publishDate 2011
dc.date.none.fl_str_mv 2011-09
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/11336/127242
Palopoli, Claudia Marcela; Bruzzo, Natalia; Hureau, Christelle; Ladeira, Sonia; Murgida, Daniel Horacio; et al.; Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionation; American Chemical Society; Inorganic Chemistry; 50; 18; 9-2011; 8973-8983
0020-1669
CONICET Digital
CONICET
url http://hdl.handle.net/11336/127242
identifier_str_mv Palopoli, Claudia Marcela; Bruzzo, Natalia; Hureau, Christelle; Ladeira, Sonia; Murgida, Daniel Horacio; et al.; Synthesis, characterization and catalase activity of a water soluble diMnIII complex of a sulphonato-substituted Schiff base ligand: An efficient catalyst for H2O2 disproportionation; American Chemical Society; Inorganic Chemistry; 50; 18; 9-2011; 8973-8983
0020-1669
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/pdf/10.1021/ic2011452
info:eu-repo/semantics/altIdentifier/doi/10.1021/ic2011452
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
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
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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