Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activity

Autores
Ledesma, Gabriela Nanci; Anxolabéhère-Mallart, Elodie; Rivière, Eric; Mallet-Ladeira, Sonia; Hureau, Christelle; Signorella, Sandra Rosanna
Año de publicación
2014
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Two new tri-MnIII complexes of general formula [Mn 3L2(μ-OH)(OAc)]ClO4 (H3L = 1-[N-(2-pyridylmethyl),N-(2-hydroxybenzyl)amino]-3-[N′-(2-hydroxybenzyl), N′-(4-X-benzyl)amino]propan-2-ol; 1ClO4, X = Me; 2ClO 4, X = H) have been prepared and characterized. X-ray diffraction analysis of 1ClO4 reveals that the complex cation possesses a Mn 3(μ-alkoxo)2(μ-hydroxo)(μ-phenoxo)4+ core, with the three Mn atoms bound to two fully deprotonated N 3O3 chelating L3-, one exogenous acetato ligand, and one hydroxo bridge, the structure of which is retained upon dissolution in acetonitrile or methanol. The three Mn atoms occupy the vertices of a nearly isosceles triangle (Mn1···Mn3 = 3.6374(12) Å, Mn2···Mn3 3.5583(13) Å, and Mn1···Mn2 3.2400(12) Å), with one substitution-labile site on the apical Mn ion occupied by terminally bound monodentate acetate. Temperature-dependent magnetic susceptibility studies indicate the presence of predominant antiferromagnetic intramolecular interactions between Mn III ions in 1ClO4. Complexes 1ClO4 and 2ClO4 decompose H2O2 at comparable rates upon initial binding of peroxide through acetate substitution, with retention of core structure during catalysis. Kinetic and spectroscopic studies suggest that these complexes employ the [Mn-(μ-oxo/aquo)-Mn]4+ moiety to activate peroxide, with the additional (μ-alkoxo)(μ-phenoxo)Mn(μ- alkoxo) metallobridge carrying out a structural function.
Fil: Ledesma, Gabriela Nanci. 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
Fil: Anxolabéhère-Mallart, Elodie. Université Paris Diderot - Paris 7; Francia
Fil: Rivière, Eric. Université Paris Sud; Francia
Fil: Mallet-Ladeira, Sonia. Université Paul Sabatier; Francia
Fil: Hureau, Christelle. Université Paul Sabatier; Francia
Fil: Signorella, Sandra Rosanna. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas; Argentina. 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
Materia
MANGANESE
UNSYMMETRICAL LIGANDS
TRINUCLEAR COMPLEXES
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:11336/94401
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/94401
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activityLedesma, Gabriela NanciAnxolabéhère-Mallart, ElodieRivière, EricMallet-Ladeira, SoniaHureau, ChristelleSignorella, Sandra RosannaMANGANESEUNSYMMETRICAL LIGANDSTRINUCLEAR COMPLEXEShttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Two new tri-MnIII complexes of general formula [Mn 3L2(μ-OH)(OAc)]ClO4 (H3L = 1-[N-(2-pyridylmethyl),N-(2-hydroxybenzyl)amino]-3-[N′-(2-hydroxybenzyl), N′-(4-X-benzyl)amino]propan-2-ol; 1ClO4, X = Me; 2ClO 4, X = H) have been prepared and characterized. X-ray diffraction analysis of 1ClO4 reveals that the complex cation possesses a Mn 3(μ-alkoxo)2(μ-hydroxo)(μ-phenoxo)4+ core, with the three Mn atoms bound to two fully deprotonated N 3O3 chelating L3-, one exogenous acetato ligand, and one hydroxo bridge, the structure of which is retained upon dissolution in acetonitrile or methanol. The three Mn atoms occupy the vertices of a nearly isosceles triangle (Mn1···Mn3 = 3.6374(12) Å, Mn2···Mn3 3.5583(13) Å, and Mn1···Mn2 3.2400(12) Å), with one substitution-labile site on the apical Mn ion occupied by terminally bound monodentate acetate. Temperature-dependent magnetic susceptibility studies indicate the presence of predominant antiferromagnetic intramolecular interactions between Mn III ions in 1ClO4. Complexes 1ClO4 and 2ClO4 decompose H2O2 at comparable rates upon initial binding of peroxide through acetate substitution, with retention of core structure during catalysis. Kinetic and spectroscopic studies suggest that these complexes employ the [Mn-(μ-oxo/aquo)-Mn]4+ moiety to activate peroxide, with the additional (μ-alkoxo)(μ-phenoxo)Mn(μ- alkoxo) metallobridge carrying out a structural function.Fil: Ledesma, Gabriela Nanci. 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; ArgentinaFil: Anxolabéhère-Mallart, Elodie. Université Paris Diderot - Paris 7; FranciaFil: Rivière, Eric. Université Paris Sud; FranciaFil: Mallet-Ladeira, Sonia. Université Paul Sabatier; FranciaFil: Hureau, Christelle. Université Paul Sabatier; FranciaFil: Signorella, Sandra Rosanna. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas; Argentina. 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; ArgentinaAmerican Chemical Society2014-03info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/94401Ledesma, Gabriela Nanci; Anxolabéhère-Mallart, Elodie; Rivière, Eric; Mallet-Ladeira, Sonia; Hureau, Christelle; et al.; Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activity; American Chemical Society; Inorganic Chemistry; 53; 5; 3-2014; 2545-25530020-1669CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1021/ic402843yinfo:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/ic402843yinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:08:01Zoai:ri.conicet.gov.ar:11336/94401instacron: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 10:08:01.801CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activity
title Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activity
spellingShingle Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activity
Ledesma, Gabriela Nanci
MANGANESE
UNSYMMETRICAL LIGANDS
TRINUCLEAR COMPLEXES
title_short Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activity
title_full Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activity
title_fullStr Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activity
title_full_unstemmed Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activity
title_sort Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activity
dc.creator.none.fl_str_mv Ledesma, Gabriela Nanci
Anxolabéhère-Mallart, Elodie
Rivière, Eric
Mallet-Ladeira, Sonia
Hureau, Christelle
Signorella, Sandra Rosanna
author Ledesma, Gabriela Nanci
author_facet Ledesma, Gabriela Nanci
Anxolabéhère-Mallart, Elodie
Rivière, Eric
Mallet-Ladeira, Sonia
Hureau, Christelle
Signorella, Sandra Rosanna
author_role author
author2 Anxolabéhère-Mallart, Elodie
Rivière, Eric
Mallet-Ladeira, Sonia
Hureau, Christelle
Signorella, Sandra Rosanna
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv MANGANESE
UNSYMMETRICAL LIGANDS
TRINUCLEAR COMPLEXES
topic MANGANESE
UNSYMMETRICAL LIGANDS
TRINUCLEAR COMPLEXES
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Two new tri-MnIII complexes of general formula [Mn 3L2(μ-OH)(OAc)]ClO4 (H3L = 1-[N-(2-pyridylmethyl),N-(2-hydroxybenzyl)amino]-3-[N′-(2-hydroxybenzyl), N′-(4-X-benzyl)amino]propan-2-ol; 1ClO4, X = Me; 2ClO 4, X = H) have been prepared and characterized. X-ray diffraction analysis of 1ClO4 reveals that the complex cation possesses a Mn 3(μ-alkoxo)2(μ-hydroxo)(μ-phenoxo)4+ core, with the three Mn atoms bound to two fully deprotonated N 3O3 chelating L3-, one exogenous acetato ligand, and one hydroxo bridge, the structure of which is retained upon dissolution in acetonitrile or methanol. The three Mn atoms occupy the vertices of a nearly isosceles triangle (Mn1···Mn3 = 3.6374(12) Å, Mn2···Mn3 3.5583(13) Å, and Mn1···Mn2 3.2400(12) Å), with one substitution-labile site on the apical Mn ion occupied by terminally bound monodentate acetate. Temperature-dependent magnetic susceptibility studies indicate the presence of predominant antiferromagnetic intramolecular interactions between Mn III ions in 1ClO4. Complexes 1ClO4 and 2ClO4 decompose H2O2 at comparable rates upon initial binding of peroxide through acetate substitution, with retention of core structure during catalysis. Kinetic and spectroscopic studies suggest that these complexes employ the [Mn-(μ-oxo/aquo)-Mn]4+ moiety to activate peroxide, with the additional (μ-alkoxo)(μ-phenoxo)Mn(μ- alkoxo) metallobridge carrying out a structural function.
Fil: Ledesma, Gabriela Nanci. 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
Fil: Anxolabéhère-Mallart, Elodie. Université Paris Diderot - Paris 7; Francia
Fil: Rivière, Eric. Université Paris Sud; Francia
Fil: Mallet-Ladeira, Sonia. Université Paul Sabatier; Francia
Fil: Hureau, Christelle. Université Paul Sabatier; Francia
Fil: Signorella, Sandra Rosanna. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas; Argentina. 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
description Two new tri-MnIII complexes of general formula [Mn 3L2(μ-OH)(OAc)]ClO4 (H3L = 1-[N-(2-pyridylmethyl),N-(2-hydroxybenzyl)amino]-3-[N′-(2-hydroxybenzyl), N′-(4-X-benzyl)amino]propan-2-ol; 1ClO4, X = Me; 2ClO 4, X = H) have been prepared and characterized. X-ray diffraction analysis of 1ClO4 reveals that the complex cation possesses a Mn 3(μ-alkoxo)2(μ-hydroxo)(μ-phenoxo)4+ core, with the three Mn atoms bound to two fully deprotonated N 3O3 chelating L3-, one exogenous acetato ligand, and one hydroxo bridge, the structure of which is retained upon dissolution in acetonitrile or methanol. The three Mn atoms occupy the vertices of a nearly isosceles triangle (Mn1···Mn3 = 3.6374(12) Å, Mn2···Mn3 3.5583(13) Å, and Mn1···Mn2 3.2400(12) Å), with one substitution-labile site on the apical Mn ion occupied by terminally bound monodentate acetate. Temperature-dependent magnetic susceptibility studies indicate the presence of predominant antiferromagnetic intramolecular interactions between Mn III ions in 1ClO4. Complexes 1ClO4 and 2ClO4 decompose H2O2 at comparable rates upon initial binding of peroxide through acetate substitution, with retention of core structure during catalysis. Kinetic and spectroscopic studies suggest that these complexes employ the [Mn-(μ-oxo/aquo)-Mn]4+ moiety to activate peroxide, with the additional (μ-alkoxo)(μ-phenoxo)Mn(μ- alkoxo) metallobridge carrying out a structural function.
publishDate 2014
dc.date.none.fl_str_mv 2014-03
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/11336/94401
Ledesma, Gabriela Nanci; Anxolabéhère-Mallart, Elodie; Rivière, Eric; Mallet-Ladeira, Sonia; Hureau, Christelle; et al.; Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activity; American Chemical Society; Inorganic Chemistry; 53; 5; 3-2014; 2545-2553
0020-1669
CONICET Digital
CONICET
url http://hdl.handle.net/11336/94401
identifier_str_mv Ledesma, Gabriela Nanci; Anxolabéhère-Mallart, Elodie; Rivière, Eric; Mallet-Ladeira, Sonia; Hureau, Christelle; et al.; Trinuclear manganese complexes of unsymmetrical polypodal diamino N 3O3 ligands with an unusual [Mn3(μ-OR) 4]5+ triangular core: Synthesis, characterization, and catalase activity; American Chemical Society; Inorganic Chemistry; 53; 5; 3-2014; 2545-2553
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/doi/10.1021/ic402843y
info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/ic402843y
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
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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score 13.070432

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