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
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/127242
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oai:ri.conicet.gov.ar:11336/127242 |
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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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1844613305693372416 |
score |
13.070432 |