A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation Reaction

Autores
Domínguez, Sofía Eugenia; Juárez, María Virginia; Pieslinger, German Eduardo; Baraldo Victorica, Luis Mario
Año de publicación
2021
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The catalytic activity towards water oxidation of a strongly coupled bimetallic ruthenium complex, trans-[Ru(tpy)(bpy)(μ-CN)Ru(py)4(OH2)]3+ (RuIIRuIIOH2), where tpy=2,2′:6′,2’’-terpyridine, bpy=2,2′-bipyridine and py=pyridine are presented. At pH 1 the first two oxidation reactions are centred at the aquo fragment and result in the RuIIRuIIIOH2 and RuIIRuIVO redox states as confirmed by its spectroscopy and DFT calculations. Oxidation by an additional electron is followed by an irreversible step and a catalytic wave associated with the water oxidation reaction. At pH 1 the reaction with an excess of Ce(IV) results in the generation of an stoichiometric amount of oxygen based on molar amounts of the added Ce(IV). The dominant species during the catalytic cycle is the three-electron oxidized product, RuIIIRuIVO. The reduction of the concentration of Ce(IV) monitored at 370 nm follow the rate equation, −d[Ce(IV)]/dt=kox[Ce(IV)][RuIIRuIIOH2] with a kox=82±3 M−1s−1 at T=298 K. The RuIIIRuIVO species is not stable and reacts to give RuIIRuIVO.
Fil: Domínguez, Sofía Eugenia. 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: Juárez, María Virginia. 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: Pieslinger, German Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Houssay. Instituto de Química y Físico-Química Biológicas "Prof. Alejandro C. Paladini". Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Instituto de Química y Físico-Química Biológicas; Argentina
Fil: Baraldo Victorica, Luis Mario. 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
CYANIDE BRIDGE
HOMOGENEOUS CATALYSIS
METAL METAL INTERACTION
RUTHENIUM
WATER OXIDATION
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:11336/173134
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/173134
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation ReactionDomínguez, Sofía EugeniaJuárez, María VirginiaPieslinger, German EduardoBaraldo Victorica, Luis MarioCYANIDE BRIDGEHOMOGENEOUS CATALYSISMETAL METAL INTERACTIONRUTHENIUMWATER OXIDATIONhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1https://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1https://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The catalytic activity towards water oxidation of a strongly coupled bimetallic ruthenium complex, trans-[Ru(tpy)(bpy)(μ-CN)Ru(py)4(OH2)]3+ (RuIIRuIIOH2), where tpy=2,2′:6′,2’’-terpyridine, bpy=2,2′-bipyridine and py=pyridine are presented. At pH 1 the first two oxidation reactions are centred at the aquo fragment and result in the RuIIRuIIIOH2 and RuIIRuIVO redox states as confirmed by its spectroscopy and DFT calculations. Oxidation by an additional electron is followed by an irreversible step and a catalytic wave associated with the water oxidation reaction. At pH 1 the reaction with an excess of Ce(IV) results in the generation of an stoichiometric amount of oxygen based on molar amounts of the added Ce(IV). The dominant species during the catalytic cycle is the three-electron oxidized product, RuIIIRuIVO. The reduction of the concentration of Ce(IV) monitored at 370 nm follow the rate equation, −d[Ce(IV)]/dt=kox[Ce(IV)][RuIIRuIIOH2] with a kox=82±3 M−1s−1 at T=298 K. The RuIIIRuIVO species is not stable and reacts to give RuIIRuIVO.Fil: Domínguez, Sofía Eugenia. 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: Juárez, María Virginia. 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: Pieslinger, German Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Houssay. Instituto de Química y Físico-Química Biológicas "Prof. Alejandro C. Paladini". Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Instituto de Química y Físico-Química Biológicas; ArgentinaFil: Baraldo Victorica, Luis Mario. 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; ArgentinaWiley VCH Verlag2021-12info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/173134Domínguez, Sofía Eugenia; Juárez, María Virginia; Pieslinger, German Eduardo; Baraldo Victorica, Luis Mario; A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation Reaction; Wiley VCH Verlag; European Journal of Inorganic Chemistry; 2022; 1; 12-2021; 1-121434-1948CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://onlinelibrary.wiley.com/doi/10.1002/ejic.202100843info:eu-repo/semantics/altIdentifier/doi/10.1002/ejic.202100843info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:47:55Zoai:ri.conicet.gov.ar:11336/173134instacron: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:34982025-09-03 09:47:56.188CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation Reaction
title A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation Reaction
spellingShingle A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation Reaction
Domínguez, Sofía Eugenia
CYANIDE BRIDGE
HOMOGENEOUS CATALYSIS
METAL METAL INTERACTION
RUTHENIUM
WATER OXIDATION
title_short A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation Reaction
title_full A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation Reaction
title_fullStr A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation Reaction
title_full_unstemmed A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation Reaction
title_sort A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation Reaction
dc.creator.none.fl_str_mv Domínguez, Sofía Eugenia
Juárez, María Virginia
Pieslinger, German Eduardo
Baraldo Victorica, Luis Mario
author Domínguez, Sofía Eugenia
author_facet Domínguez, Sofía Eugenia
Juárez, María Virginia
Pieslinger, German Eduardo
Baraldo Victorica, Luis Mario
author_role author
author2 Juárez, María Virginia
Pieslinger, German Eduardo
Baraldo Victorica, Luis Mario
author2_role author
author
author
dc.subject.none.fl_str_mv CYANIDE BRIDGE
HOMOGENEOUS CATALYSIS
METAL METAL INTERACTION
RUTHENIUM
WATER OXIDATION
topic CYANIDE BRIDGE
HOMOGENEOUS CATALYSIS
METAL METAL INTERACTION
RUTHENIUM
WATER OXIDATION
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The catalytic activity towards water oxidation of a strongly coupled bimetallic ruthenium complex, trans-[Ru(tpy)(bpy)(μ-CN)Ru(py)4(OH2)]3+ (RuIIRuIIOH2), where tpy=2,2′:6′,2’’-terpyridine, bpy=2,2′-bipyridine and py=pyridine are presented. At pH 1 the first two oxidation reactions are centred at the aquo fragment and result in the RuIIRuIIIOH2 and RuIIRuIVO redox states as confirmed by its spectroscopy and DFT calculations. Oxidation by an additional electron is followed by an irreversible step and a catalytic wave associated with the water oxidation reaction. At pH 1 the reaction with an excess of Ce(IV) results in the generation of an stoichiometric amount of oxygen based on molar amounts of the added Ce(IV). The dominant species during the catalytic cycle is the three-electron oxidized product, RuIIIRuIVO. The reduction of the concentration of Ce(IV) monitored at 370 nm follow the rate equation, −d[Ce(IV)]/dt=kox[Ce(IV)][RuIIRuIIOH2] with a kox=82±3 M−1s−1 at T=298 K. The RuIIIRuIVO species is not stable and reacts to give RuIIRuIVO.
Fil: Domínguez, Sofía Eugenia. 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: Juárez, María Virginia. 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: Pieslinger, German Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Houssay. Instituto de Química y Físico-Química Biológicas "Prof. Alejandro C. Paladini". Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Instituto de Química y Físico-Química Biológicas; Argentina
Fil: Baraldo Victorica, Luis Mario. 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 catalytic activity towards water oxidation of a strongly coupled bimetallic ruthenium complex, trans-[Ru(tpy)(bpy)(μ-CN)Ru(py)4(OH2)]3+ (RuIIRuIIOH2), where tpy=2,2′:6′,2’’-terpyridine, bpy=2,2′-bipyridine and py=pyridine are presented. At pH 1 the first two oxidation reactions are centred at the aquo fragment and result in the RuIIRuIIIOH2 and RuIIRuIVO redox states as confirmed by its spectroscopy and DFT calculations. Oxidation by an additional electron is followed by an irreversible step and a catalytic wave associated with the water oxidation reaction. At pH 1 the reaction with an excess of Ce(IV) results in the generation of an stoichiometric amount of oxygen based on molar amounts of the added Ce(IV). The dominant species during the catalytic cycle is the three-electron oxidized product, RuIIIRuIVO. The reduction of the concentration of Ce(IV) monitored at 370 nm follow the rate equation, −d[Ce(IV)]/dt=kox[Ce(IV)][RuIIRuIIOH2] with a kox=82±3 M−1s−1 at T=298 K. The RuIIIRuIVO species is not stable and reacts to give RuIIRuIVO.
publishDate 2021
dc.date.none.fl_str_mv 2021-12
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/11336/173134
Domínguez, Sofía Eugenia; Juárez, María Virginia; Pieslinger, German Eduardo; Baraldo Victorica, Luis Mario; A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation Reaction; Wiley VCH Verlag; European Journal of Inorganic Chemistry; 2022; 1; 12-2021; 1-12
1434-1948
CONICET Digital
CONICET
url http://hdl.handle.net/11336/173134
identifier_str_mv Domínguez, Sofía Eugenia; Juárez, María Virginia; Pieslinger, German Eduardo; Baraldo Victorica, Luis Mario; A Strongly Coupled Biruthenium Complex as Catalyst for the Water Oxidation Reaction; Wiley VCH Verlag; European Journal of Inorganic Chemistry; 2022; 1; 12-2021; 1-12
1434-1948
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://onlinelibrary.wiley.com/doi/10.1002/ejic.202100843
info:eu-repo/semantics/altIdentifier/doi/10.1002/ejic.202100843
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 Wiley VCH Verlag
publisher.none.fl_str_mv Wiley VCH Verlag
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 13.13397

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