Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates

Autores
Negre, Christian Francisco Andres; Young, Karin J.; Oviedo, María Belén; Allen, Laura J.; Sanchez, Cristian Gabriel; Jarzembska , Katarzyna N.; Benedict, Jason B.; Crabtree, Robert H.; Coppens, Philip; Brudvig, Gary W.; Batista, Víctor S.
Año de publicación
2014
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
We find that crystallographically resolved Ti17O24(OPri)20 nanoparticles, functionalized by covalent attachment of 4-nitrophenyl-acetylacetonate or coumarin 343 adsorbates, exhibit hole injection into surface states when photoexcited with visible light (λ = 400–680 nm). Our findings are supported by photoelectrochemical measurements, EPR spectroscopy, and quantum dynamics simulations of interfacial charge transfer. The underlying mechanism is consistent with measurements of photocathodic currents generated with visible light for thin layers of functionalized polyoxotitanate nanocrystals deposited on FTO working electrodes. The reported experimental and theoretical analysis demonstrates for the first time the feasibility of p-type sensitization of TiO2 solely based on covalent binding of organic adsorbates.
Fil: Negre, Christian Francisco Andres. University of Yale; Estados Unidos
Fil: Young, Karin J.. University of Yale; Estados Unidos
Fil: Oviedo, María Belén. Drexel University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Allen, Laura J.. University of Yale; Estados Unidos
Fil: Sanchez, Cristian Gabriel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Jarzembska , Katarzyna N.. State University of New York; Estados Unidos. University of Warsaw,. Varsovia; Polonia
Fil: Benedict, Jason B.. State University of New York; Estados Unidos
Fil: Crabtree, Robert H.. University of Yale; Estados Unidos
Fil: Coppens, Philip. State University of New York; Estados Unidos
Fil: Brudvig, Gary W.. University of Yale; Estados Unidos
Fil: Batista, Víctor S.. University of Yale; Estados Unidos
Materia
Photoinduced Electron Transfer
Dye Sensitized Solar Cells
Electron Paramagnetic Ressonance
Quantum Dynamics
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:11336/31537
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/31537
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbatesNegre, Christian Francisco AndresYoung, Karin J.Oviedo, María BelénAllen, Laura J.Sanchez, Cristian GabrielJarzembska , Katarzyna N.Benedict, Jason B.Crabtree, Robert H.Coppens, PhilipBrudvig, Gary W.Batista, Víctor S.Photoinduced Electron TransferDye Sensitized Solar CellsElectron Paramagnetic RessonanceQuantum Dynamicshttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1We find that crystallographically resolved Ti17O24(OPri)20 nanoparticles, functionalized by covalent attachment of 4-nitrophenyl-acetylacetonate or coumarin 343 adsorbates, exhibit hole injection into surface states when photoexcited with visible light (λ = 400–680 nm). Our findings are supported by photoelectrochemical measurements, EPR spectroscopy, and quantum dynamics simulations of interfacial charge transfer. The underlying mechanism is consistent with measurements of photocathodic currents generated with visible light for thin layers of functionalized polyoxotitanate nanocrystals deposited on FTO working electrodes. The reported experimental and theoretical analysis demonstrates for the first time the feasibility of p-type sensitization of TiO2 solely based on covalent binding of organic adsorbates.Fil: Negre, Christian Francisco Andres. University of Yale; Estados UnidosFil: Young, Karin J.. University of Yale; Estados UnidosFil: Oviedo, María Belén. Drexel University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Allen, Laura J.. University of Yale; Estados UnidosFil: Sanchez, Cristian Gabriel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; ArgentinaFil: Jarzembska , Katarzyna N.. State University of New York; Estados Unidos. University of Warsaw,. Varsovia; PoloniaFil: Benedict, Jason B.. State University of New York; Estados UnidosFil: Crabtree, Robert H.. University of Yale; Estados UnidosFil: Coppens, Philip. State University of New York; Estados UnidosFil: Brudvig, Gary W.. University of Yale; Estados UnidosFil: Batista, Víctor S.. University of Yale; Estados UnidosAmerican Chemical Society2014-11info: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/11336/31537Negre, Christian Francisco Andres; Young, Karin J.; Oviedo, María Belén; Allen, Laura J.; Sanchez, Cristian Gabriel; et al.; Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates; American Chemical Society; Journal of the American Chemical Society; 136; 46; 11-2014; 16420-164290002-7863CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1021/ja509270finfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/10.1021/ja509270finfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:50:36Zoai:ri.conicet.gov.ar:11336/31537instacron: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 09:50:36.452CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates
title Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates
spellingShingle Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates
Negre, Christian Francisco Andres
Photoinduced Electron Transfer
Dye Sensitized Solar Cells
Electron Paramagnetic Ressonance
Quantum Dynamics
title_short Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates
title_full Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates
title_fullStr Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates
title_full_unstemmed Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates
title_sort Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates
dc.creator.none.fl_str_mv Negre, Christian Francisco Andres
Young, Karin J.
Oviedo, María Belén
Allen, Laura J.
Sanchez, Cristian Gabriel
Jarzembska , Katarzyna N.
Benedict, Jason B.
Crabtree, Robert H.
Coppens, Philip
Brudvig, Gary W.
Batista, Víctor S.
author Negre, Christian Francisco Andres
author_facet Negre, Christian Francisco Andres
Young, Karin J.
Oviedo, María Belén
Allen, Laura J.
Sanchez, Cristian Gabriel
Jarzembska , Katarzyna N.
Benedict, Jason B.
Crabtree, Robert H.
Coppens, Philip
Brudvig, Gary W.
Batista, Víctor S.
author_role author
author2 Young, Karin J.
Oviedo, María Belén
Allen, Laura J.
Sanchez, Cristian Gabriel
Jarzembska , Katarzyna N.
Benedict, Jason B.
Crabtree, Robert H.
Coppens, Philip
Brudvig, Gary W.
Batista, Víctor S.
author2_role author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Photoinduced Electron Transfer
Dye Sensitized Solar Cells
Electron Paramagnetic Ressonance
Quantum Dynamics
topic Photoinduced Electron Transfer
Dye Sensitized Solar Cells
Electron Paramagnetic Ressonance
Quantum Dynamics
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 find that crystallographically resolved Ti17O24(OPri)20 nanoparticles, functionalized by covalent attachment of 4-nitrophenyl-acetylacetonate or coumarin 343 adsorbates, exhibit hole injection into surface states when photoexcited with visible light (λ = 400–680 nm). Our findings are supported by photoelectrochemical measurements, EPR spectroscopy, and quantum dynamics simulations of interfacial charge transfer. The underlying mechanism is consistent with measurements of photocathodic currents generated with visible light for thin layers of functionalized polyoxotitanate nanocrystals deposited on FTO working electrodes. The reported experimental and theoretical analysis demonstrates for the first time the feasibility of p-type sensitization of TiO2 solely based on covalent binding of organic adsorbates.
Fil: Negre, Christian Francisco Andres. University of Yale; Estados Unidos
Fil: Young, Karin J.. University of Yale; Estados Unidos
Fil: Oviedo, María Belén. Drexel University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Allen, Laura J.. University of Yale; Estados Unidos
Fil: Sanchez, Cristian Gabriel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Jarzembska , Katarzyna N.. State University of New York; Estados Unidos. University of Warsaw,. Varsovia; Polonia
Fil: Benedict, Jason B.. State University of New York; Estados Unidos
Fil: Crabtree, Robert H.. University of Yale; Estados Unidos
Fil: Coppens, Philip. State University of New York; Estados Unidos
Fil: Brudvig, Gary W.. University of Yale; Estados Unidos
Fil: Batista, Víctor S.. University of Yale; Estados Unidos
description We find that crystallographically resolved Ti17O24(OPri)20 nanoparticles, functionalized by covalent attachment of 4-nitrophenyl-acetylacetonate or coumarin 343 adsorbates, exhibit hole injection into surface states when photoexcited with visible light (λ = 400–680 nm). Our findings are supported by photoelectrochemical measurements, EPR spectroscopy, and quantum dynamics simulations of interfacial charge transfer. The underlying mechanism is consistent with measurements of photocathodic currents generated with visible light for thin layers of functionalized polyoxotitanate nanocrystals deposited on FTO working electrodes. The reported experimental and theoretical analysis demonstrates for the first time the feasibility of p-type sensitization of TiO2 solely based on covalent binding of organic adsorbates.
publishDate 2014
dc.date.none.fl_str_mv 2014-11
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/11336/31537
Negre, Christian Francisco Andres; Young, Karin J.; Oviedo, María Belén; Allen, Laura J.; Sanchez, Cristian Gabriel; et al.; Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates; American Chemical Society; Journal of the American Chemical Society; 136; 46; 11-2014; 16420-16429
0002-7863
CONICET Digital
CONICET
url http://hdl.handle.net/11336/31537
identifier_str_mv Negre, Christian Francisco Andres; Young, Karin J.; Oviedo, María Belén; Allen, Laura J.; Sanchez, Cristian Gabriel; et al.; Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates; American Chemical Society; Journal of the American Chemical Society; 136; 46; 11-2014; 16420-16429
0002-7863
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/ja509270f
info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/10.1021/ja509270f
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 12.885934

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