Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligand

Autores
Mecchia Ortiz, Juan Hugo; Vega, Nadia Celeste; Comedi, David Mario; Tirado, Monica Cecilia; Romero, Isabel; Fontrodona, Xavier; Parella, Teodor; Moran Vieyra, Faustino Eduardo; Borsarelli, Claudio Darío; Katz, Néstor Eduardo
Año de publicación
2013
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
We report in this work the synthesis and spectroscopic, electrochemical, spectroelectrochemical, and photophysical characterization of a novel series of ruthenium polypyridyl complexes with 4-methyl-2,2′-bipyridine-4′- carbonitrile (Mebpy-CN) as an auxiliary ligand of general formula [Ru(bpy) 3-x(Mebpy-CN)x](PF6)2 (x = 1-3) (with bpy = 2,2′-bipyridine). A significant increase in the lifetime and quantum yield of emission of the lowest 3MLCT excited state is disclosed when going from x = 1 to x = 3, evidencing an improvement of the photosensitizing properties with respect to [Ru(bpy)3](PF 6)2. Furthermore, quenching by molecular oxygen of 3MLCT excited states of the three complexes produced singlet molecular oxygen (1O2) with quantum yield values higher than that of [Ru(bpy)3]2+ in CH3CN. The structure of the complex with x = 1 has been determined by X-ray diffraction. The photoconductivity of ZnO nanowires covered with this same complex is increased by an order of magnitude, pointing to its feasibility as a component of a DSSC. A new dinuclear complex with Mebpy-CN as a bridging ligand has also been prepared and characterized by physicochemical techniques. The derived mixed-valent species of formula [(bpy)2RuII(Mebpy-CN) RuIII(NH3)5]5+ displays a considerable metal-metal electronic coupling due to the delocalization effect of a nitrile group in the 4′ position of the bpy ring. © 2013 American Chemical Society.
Fil: Mecchia Ortiz, Juan Hugo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Tucumán. Instituto de Química del Noroeste. Universidad Nacional de Tucumán. Facultad de Bioquímica, Química y Farmacia. Instituto de Química del Noroeste; Argentina
Fil: Vega, Nadia Celeste. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Tucumán. Facultad de Ciencias Exactas y Tecnología; Argentina
Fil: Comedi, David Mario. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Tucumán. Facultad de Ciencias Exactas y Tecnología; Argentina
Fil: Tirado, Monica Cecilia. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Tucumán. Facultad de Ciencias Exactas y Tecnología; Argentina
Fil: Romero, Isabel. Universidad de Girona; España
Fil: Fontrodona, Xavier. Universidad de Girona; España
Fil: Parella, Teodor. Universitat Autònoma de Barcelona; España
Fil: Moran Vieyra, Faustino Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro de Investigaciones y Transferencia de Santiago del Estero. Universidad Nacional de Santiago del Estero. Centro de Investigaciones y Transferencia de Santiago del Estero; Argentina
Fil: Borsarelli, Claudio Darío. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro de Investigaciones y Transferencia de Santiago del Estero. Universidad Nacional de Santiago del Estero. Centro de Investigaciones y Transferencia de Santiago del Estero; Argentina
Fil: Katz, Néstor Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Tucumán. Instituto de Química del Noroeste. Universidad Nacional de Tucumán. Facultad de Bioquímica, Química y Farmacia. Instituto de Química del Noroeste; Argentina
Materia
RUTHENIUM COMPLEXES
NANOWIRES
PHOTOSENSITIZATION
SINGLET OXYGEN
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:11336/78129

id CONICETDig_d3173cc3f04c349a2c25b554652b3549
oai_identifier_str oai:ri.conicet.gov.ar:11336/78129
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligandMecchia Ortiz, Juan HugoVega, Nadia CelesteComedi, David MarioTirado, Monica CeciliaRomero, IsabelFontrodona, XavierParella, TeodorMoran Vieyra, Faustino EduardoBorsarelli, Claudio DaríoKatz, Néstor EduardoRUTHENIUM COMPLEXESNANOWIRESPHOTOSENSITIZATIONSINGLET OXYGENhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1We report in this work the synthesis and spectroscopic, electrochemical, spectroelectrochemical, and photophysical characterization of a novel series of ruthenium polypyridyl complexes with 4-methyl-2,2′-bipyridine-4′- carbonitrile (Mebpy-CN) as an auxiliary ligand of general formula [Ru(bpy) 3-x(Mebpy-CN)x](PF6)2 (x = 1-3) (with bpy = 2,2′-bipyridine). A significant increase in the lifetime and quantum yield of emission of the lowest 3MLCT excited state is disclosed when going from x = 1 to x = 3, evidencing an improvement of the photosensitizing properties with respect to [Ru(bpy)3](PF 6)2. Furthermore, quenching by molecular oxygen of 3MLCT excited states of the three complexes produced singlet molecular oxygen (1O2) with quantum yield values higher than that of [Ru(bpy)3]2+ in CH3CN. The structure of the complex with x = 1 has been determined by X-ray diffraction. The photoconductivity of ZnO nanowires covered with this same complex is increased by an order of magnitude, pointing to its feasibility as a component of a DSSC. A new dinuclear complex with Mebpy-CN as a bridging ligand has also been prepared and characterized by physicochemical techniques. The derived mixed-valent species of formula [(bpy)2RuII(Mebpy-CN) RuIII(NH3)5]5+ displays a considerable metal-metal electronic coupling due to the delocalization effect of a nitrile group in the 4′ position of the bpy ring. © 2013 American Chemical Society.Fil: Mecchia Ortiz, Juan Hugo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Tucumán. Instituto de Química del Noroeste. Universidad Nacional de Tucumán. Facultad de Bioquímica, Química y Farmacia. Instituto de Química del Noroeste; ArgentinaFil: Vega, Nadia Celeste. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Tucumán. Facultad de Ciencias Exactas y Tecnología; ArgentinaFil: Comedi, David Mario. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Tucumán. Facultad de Ciencias Exactas y Tecnología; ArgentinaFil: Tirado, Monica Cecilia. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Tucumán. Facultad de Ciencias Exactas y Tecnología; ArgentinaFil: Romero, Isabel. Universidad de Girona; EspañaFil: Fontrodona, Xavier. Universidad de Girona; EspañaFil: Parella, Teodor. Universitat Autònoma de Barcelona; EspañaFil: Moran Vieyra, Faustino Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro de Investigaciones y Transferencia de Santiago del Estero. Universidad Nacional de Santiago del Estero. Centro de Investigaciones y Transferencia de Santiago del Estero; ArgentinaFil: Borsarelli, Claudio Darío. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro de Investigaciones y Transferencia de Santiago del Estero. Universidad Nacional de Santiago del Estero. Centro de Investigaciones y Transferencia de Santiago del Estero; ArgentinaFil: Katz, Néstor Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Tucumán. Instituto de Química del Noroeste. Universidad Nacional de Tucumán. Facultad de Bioquímica, Química y Farmacia. Instituto de Química del Noroeste; ArgentinaAmerican Chemical Society2013-05info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/78129Mecchia Ortiz, Juan Hugo; Vega, Nadia Celeste; Comedi, David Mario; Tirado, Monica Cecilia; Romero, Isabel; et al.; Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligand; American Chemical Society; Inorganic Chemistry; 52; 9; 5-2013; 4950-49620020-1669CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/ic302594binfo:eu-repo/semantics/altIdentifier/doi/10.1021/ic302594binfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:50:02Zoai:ri.conicet.gov.ar:11336/78129instacron: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 09:50:02.595CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligand
title Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligand
spellingShingle Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligand
Mecchia Ortiz, Juan Hugo
RUTHENIUM COMPLEXES
NANOWIRES
PHOTOSENSITIZATION
SINGLET OXYGEN
title_short Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligand
title_full Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligand
title_fullStr Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligand
title_full_unstemmed Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligand
title_sort Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligand
dc.creator.none.fl_str_mv Mecchia Ortiz, Juan Hugo
Vega, Nadia Celeste
Comedi, David Mario
Tirado, Monica Cecilia
Romero, Isabel
Fontrodona, Xavier
Parella, Teodor
Moran Vieyra, Faustino Eduardo
Borsarelli, Claudio Darío
Katz, Néstor Eduardo
author Mecchia Ortiz, Juan Hugo
author_facet Mecchia Ortiz, Juan Hugo
Vega, Nadia Celeste
Comedi, David Mario
Tirado, Monica Cecilia
Romero, Isabel
Fontrodona, Xavier
Parella, Teodor
Moran Vieyra, Faustino Eduardo
Borsarelli, Claudio Darío
Katz, Néstor Eduardo
author_role author
author2 Vega, Nadia Celeste
Comedi, David Mario
Tirado, Monica Cecilia
Romero, Isabel
Fontrodona, Xavier
Parella, Teodor
Moran Vieyra, Faustino Eduardo
Borsarelli, Claudio Darío
Katz, Néstor Eduardo
author2_role author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv RUTHENIUM COMPLEXES
NANOWIRES
PHOTOSENSITIZATION
SINGLET OXYGEN
topic RUTHENIUM COMPLEXES
NANOWIRES
PHOTOSENSITIZATION
SINGLET OXYGEN
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv We report in this work the synthesis and spectroscopic, electrochemical, spectroelectrochemical, and photophysical characterization of a novel series of ruthenium polypyridyl complexes with 4-methyl-2,2′-bipyridine-4′- carbonitrile (Mebpy-CN) as an auxiliary ligand of general formula [Ru(bpy) 3-x(Mebpy-CN)x](PF6)2 (x = 1-3) (with bpy = 2,2′-bipyridine). A significant increase in the lifetime and quantum yield of emission of the lowest 3MLCT excited state is disclosed when going from x = 1 to x = 3, evidencing an improvement of the photosensitizing properties with respect to [Ru(bpy)3](PF 6)2. Furthermore, quenching by molecular oxygen of 3MLCT excited states of the three complexes produced singlet molecular oxygen (1O2) with quantum yield values higher than that of [Ru(bpy)3]2+ in CH3CN. The structure of the complex with x = 1 has been determined by X-ray diffraction. The photoconductivity of ZnO nanowires covered with this same complex is increased by an order of magnitude, pointing to its feasibility as a component of a DSSC. A new dinuclear complex with Mebpy-CN as a bridging ligand has also been prepared and characterized by physicochemical techniques. The derived mixed-valent species of formula [(bpy)2RuII(Mebpy-CN) RuIII(NH3)5]5+ displays a considerable metal-metal electronic coupling due to the delocalization effect of a nitrile group in the 4′ position of the bpy ring. © 2013 American Chemical Society.
Fil: Mecchia Ortiz, Juan Hugo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Tucumán. Instituto de Química del Noroeste. Universidad Nacional de Tucumán. Facultad de Bioquímica, Química y Farmacia. Instituto de Química del Noroeste; Argentina
Fil: Vega, Nadia Celeste. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Tucumán. Facultad de Ciencias Exactas y Tecnología; Argentina
Fil: Comedi, David Mario. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Tucumán. Facultad de Ciencias Exactas y Tecnología; Argentina
Fil: Tirado, Monica Cecilia. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Tucumán. Facultad de Ciencias Exactas y Tecnología; Argentina
Fil: Romero, Isabel. Universidad de Girona; España
Fil: Fontrodona, Xavier. Universidad de Girona; España
Fil: Parella, Teodor. Universitat Autònoma de Barcelona; España
Fil: Moran Vieyra, Faustino Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro de Investigaciones y Transferencia de Santiago del Estero. Universidad Nacional de Santiago del Estero. Centro de Investigaciones y Transferencia de Santiago del Estero; Argentina
Fil: Borsarelli, Claudio Darío. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro de Investigaciones y Transferencia de Santiago del Estero. Universidad Nacional de Santiago del Estero. Centro de Investigaciones y Transferencia de Santiago del Estero; Argentina
Fil: Katz, Néstor Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Tucumán. Instituto de Química del Noroeste. Universidad Nacional de Tucumán. Facultad de Bioquímica, Química y Farmacia. Instituto de Química del Noroeste; Argentina
description We report in this work the synthesis and spectroscopic, electrochemical, spectroelectrochemical, and photophysical characterization of a novel series of ruthenium polypyridyl complexes with 4-methyl-2,2′-bipyridine-4′- carbonitrile (Mebpy-CN) as an auxiliary ligand of general formula [Ru(bpy) 3-x(Mebpy-CN)x](PF6)2 (x = 1-3) (with bpy = 2,2′-bipyridine). A significant increase in the lifetime and quantum yield of emission of the lowest 3MLCT excited state is disclosed when going from x = 1 to x = 3, evidencing an improvement of the photosensitizing properties with respect to [Ru(bpy)3](PF 6)2. Furthermore, quenching by molecular oxygen of 3MLCT excited states of the three complexes produced singlet molecular oxygen (1O2) with quantum yield values higher than that of [Ru(bpy)3]2+ in CH3CN. The structure of the complex with x = 1 has been determined by X-ray diffraction. The photoconductivity of ZnO nanowires covered with this same complex is increased by an order of magnitude, pointing to its feasibility as a component of a DSSC. A new dinuclear complex with Mebpy-CN as a bridging ligand has also been prepared and characterized by physicochemical techniques. The derived mixed-valent species of formula [(bpy)2RuII(Mebpy-CN) RuIII(NH3)5]5+ displays a considerable metal-metal electronic coupling due to the delocalization effect of a nitrile group in the 4′ position of the bpy ring. © 2013 American Chemical Society.
publishDate 2013
dc.date.none.fl_str_mv 2013-05
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/11336/78129
Mecchia Ortiz, Juan Hugo; Vega, Nadia Celeste; Comedi, David Mario; Tirado, Monica Cecilia; Romero, Isabel; et al.; Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligand; American Chemical Society; Inorganic Chemistry; 52; 9; 5-2013; 4950-4962
0020-1669
CONICET Digital
CONICET
url http://hdl.handle.net/11336/78129
identifier_str_mv Mecchia Ortiz, Juan Hugo; Vega, Nadia Celeste; Comedi, David Mario; Tirado, Monica Cecilia; Romero, Isabel; et al.; Improving the photosensitizing properties of ruthenium polypyridyl complexes using 4-methyl-2,2′-bipyridine-4′-carbonitrile as an auxiliary ligand; American Chemical Society; Inorganic Chemistry; 52; 9; 5-2013; 4950-4962
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/abs/10.1021/ic302594b
info:eu-repo/semantics/altIdentifier/doi/10.1021/ic302594b
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
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
_version_ 1844613544701591552
score 13.070432