Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generation

Autores
Rodenas, Pau; Song, Taesup; Sudhagar, Pitchaimuthu; Marzari, Gabriela Lorena; Han, Hyungkyu; Badia Bou, Laura; Gimenez, Sixto; Fabregat-Santiago, Francisco; Mora Sero, Ivan; Bisquert, Juan; Paik, Ungyu; Kang, Yong Soo
Año de publicación
2013
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
TiO 2 hollow nanowires (HNWs) and nanoparticles (NPs) constitute prom- ising architectures for QDs sensitized photoanodes for H 2 generation. We sensitize these structures with CdS/CdSe quantum dots by two different methods (chemical bath deposition, CBD and succesive ionic layer adsorp- tion and reaction, SILAR) and evaluate the performance of these photoelec- trodes. Remarkable photocurrents of 4 mA · cm and 8 mA · cm − 2 and hydrogen generation rates of 40 ml · cm − 2 · day − 1 and 80 ml · cm − 2 · day − 1 have been obtained in a three electrode confi guration with sacrifi cial hole scavengers (Na 2 S and Na 2 SO 3 ), for HNWs and NPs respectively, which is confi rmed through gas analysis. More importantly, autonomous generation of H 2 (20 ml · cm − 2 · day − 1 corresponding to 2 mA · cm − 2 photocurrent) is obtained in a two electrode confi guration at short circuit under 100 mW · cm − 2 illumina- tion, clearly showing that these photoanodes can produce hydrogen without the assistance of any external bias. To the best of the authors? knowledge, this is the highest unbiased solar H 2 generation rate reported for these of QDs based heterostructures. Impedance spectroscopy measurements show similar electron density of trap states below the TiO 2 conduction band while the recombination resistance was higher for HNWs, consistently with the much lower surface area compared to NPs. However, the conductivity of both structures is similar, in spite of the one dimensional character of HNWs, which leaves some room for improvement of these nanowired structures. The effect of the QDs deposition method is also evaluated. Both structures show remarkable stability without any appreciable photocurrent loss after 0.5 hour of operation. The fi ndings of this study constitute a relevant step towards the feasibility of hydrogen generation with wide bandgap semiconductors/ quantum dots based heterostructures.
Fil: Rodenas, Pau. Hanyang University; Corea del Sur
Fil: Song, Taesup. Hanyang University; Corea del Sur
Fil: Sudhagar, Pitchaimuthu. Hanyang University; Corea del Sur
Fil: Marzari, Gabriela Lorena. Universitat Jaume I; España. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba; Argentina
Fil: Han, Hyungkyu. Hanyang University; Corea del Sur
Fil: Badia Bou, Laura. Hanyang University; Corea del Sur
Fil: Gimenez, Sixto. Universitat Jaume I; España
Fil: Fabregat-Santiago, Francisco. Universitat Jaume I; España
Fil: Mora Sero, Ivan. Universitat Jaume I; España
Fil: Bisquert, Juan. Universitat Jaume I; España
Fil: Paik, Ungyu. Hanyang University; Corea del Sur
Fil: Kang, Yong Soo. Hanyang University; Corea del Sur
Materia
TiO2 hollow nanowires
QDs sensitized photoanodes
H2 generation
CdS/CdSe quantum dots
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:11336/199134

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oai_identifier_str oai:ri.conicet.gov.ar:11336/199134
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generationRodenas, PauSong, TaesupSudhagar, PitchaimuthuMarzari, Gabriela LorenaHan, HyungkyuBadia Bou, LauraGimenez, SixtoFabregat-Santiago, FranciscoMora Sero, IvanBisquert, JuanPaik, UngyuKang, Yong SooTiO2 hollow nanowiresQDs sensitized photoanodesH2 generationCdS/CdSe quantum dotshttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1TiO 2 hollow nanowires (HNWs) and nanoparticles (NPs) constitute prom- ising architectures for QDs sensitized photoanodes for H 2 generation. We sensitize these structures with CdS/CdSe quantum dots by two different methods (chemical bath deposition, CBD and succesive ionic layer adsorp- tion and reaction, SILAR) and evaluate the performance of these photoelec- trodes. Remarkable photocurrents of 4 mA · cm and 8 mA · cm − 2 and hydrogen generation rates of 40 ml · cm − 2 · day − 1 and 80 ml · cm − 2 · day − 1 have been obtained in a three electrode confi guration with sacrifi cial hole scavengers (Na 2 S and Na 2 SO 3 ), for HNWs and NPs respectively, which is confi rmed through gas analysis. More importantly, autonomous generation of H 2 (20 ml · cm − 2 · day − 1 corresponding to 2 mA · cm − 2 photocurrent) is obtained in a two electrode confi guration at short circuit under 100 mW · cm − 2 illumina- tion, clearly showing that these photoanodes can produce hydrogen without the assistance of any external bias. To the best of the authors? knowledge, this is the highest unbiased solar H 2 generation rate reported for these of QDs based heterostructures. Impedance spectroscopy measurements show similar electron density of trap states below the TiO 2 conduction band while the recombination resistance was higher for HNWs, consistently with the much lower surface area compared to NPs. However, the conductivity of both structures is similar, in spite of the one dimensional character of HNWs, which leaves some room for improvement of these nanowired structures. The effect of the QDs deposition method is also evaluated. Both structures show remarkable stability without any appreciable photocurrent loss after 0.5 hour of operation. The fi ndings of this study constitute a relevant step towards the feasibility of hydrogen generation with wide bandgap semiconductors/ quantum dots based heterostructures.Fil: Rodenas, Pau. Hanyang University; Corea del SurFil: Song, Taesup. Hanyang University; Corea del SurFil: Sudhagar, Pitchaimuthu. Hanyang University; Corea del SurFil: Marzari, Gabriela Lorena. Universitat Jaume I; España. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba; ArgentinaFil: Han, Hyungkyu. Hanyang University; Corea del SurFil: Badia Bou, Laura. Hanyang University; Corea del SurFil: Gimenez, Sixto. Universitat Jaume I; EspañaFil: Fabregat-Santiago, Francisco. Universitat Jaume I; EspañaFil: Mora Sero, Ivan. Universitat Jaume I; EspañaFil: Bisquert, Juan. Universitat Jaume I; EspañaFil: Paik, Ungyu. Hanyang University; Corea del SurFil: Kang, Yong Soo. Hanyang University; Corea del SurWiley-VCH2013-02info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/199134Rodenas, Pau; Song, Taesup; Sudhagar, Pitchaimuthu; Marzari, Gabriela Lorena; Han, Hyungkyu; et al.; Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generation; Wiley-VCH; advanced energy materials; 3; 2; 2-2013; 176-1821614-6840CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1002/aenm.201200255info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2026-03-31T15:04:51Zoai:ri.conicet.gov.ar:11336/199134instacron: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:34982026-03-31 15:04:51.682CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generation
title Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generation
spellingShingle Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generation
Rodenas, Pau
TiO2 hollow nanowires
QDs sensitized photoanodes
H2 generation
CdS/CdSe quantum dots
title_short Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generation
title_full Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generation
title_fullStr Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generation
title_full_unstemmed Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generation
title_sort Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generation
dc.creator.none.fl_str_mv Rodenas, Pau
Song, Taesup
Sudhagar, Pitchaimuthu
Marzari, Gabriela Lorena
Han, Hyungkyu
Badia Bou, Laura
Gimenez, Sixto
Fabregat-Santiago, Francisco
Mora Sero, Ivan
Bisquert, Juan
Paik, Ungyu
Kang, Yong Soo
author Rodenas, Pau
author_facet Rodenas, Pau
Song, Taesup
Sudhagar, Pitchaimuthu
Marzari, Gabriela Lorena
Han, Hyungkyu
Badia Bou, Laura
Gimenez, Sixto
Fabregat-Santiago, Francisco
Mora Sero, Ivan
Bisquert, Juan
Paik, Ungyu
Kang, Yong Soo
author_role author
author2 Song, Taesup
Sudhagar, Pitchaimuthu
Marzari, Gabriela Lorena
Han, Hyungkyu
Badia Bou, Laura
Gimenez, Sixto
Fabregat-Santiago, Francisco
Mora Sero, Ivan
Bisquert, Juan
Paik, Ungyu
Kang, Yong Soo
author2_role author
author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv TiO2 hollow nanowires
QDs sensitized photoanodes
H2 generation
CdS/CdSe quantum dots
topic TiO2 hollow nanowires
QDs sensitized photoanodes
H2 generation
CdS/CdSe quantum dots
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv TiO 2 hollow nanowires (HNWs) and nanoparticles (NPs) constitute prom- ising architectures for QDs sensitized photoanodes for H 2 generation. We sensitize these structures with CdS/CdSe quantum dots by two different methods (chemical bath deposition, CBD and succesive ionic layer adsorp- tion and reaction, SILAR) and evaluate the performance of these photoelec- trodes. Remarkable photocurrents of 4 mA · cm and 8 mA · cm − 2 and hydrogen generation rates of 40 ml · cm − 2 · day − 1 and 80 ml · cm − 2 · day − 1 have been obtained in a three electrode confi guration with sacrifi cial hole scavengers (Na 2 S and Na 2 SO 3 ), for HNWs and NPs respectively, which is confi rmed through gas analysis. More importantly, autonomous generation of H 2 (20 ml · cm − 2 · day − 1 corresponding to 2 mA · cm − 2 photocurrent) is obtained in a two electrode confi guration at short circuit under 100 mW · cm − 2 illumina- tion, clearly showing that these photoanodes can produce hydrogen without the assistance of any external bias. To the best of the authors? knowledge, this is the highest unbiased solar H 2 generation rate reported for these of QDs based heterostructures. Impedance spectroscopy measurements show similar electron density of trap states below the TiO 2 conduction band while the recombination resistance was higher for HNWs, consistently with the much lower surface area compared to NPs. However, the conductivity of both structures is similar, in spite of the one dimensional character of HNWs, which leaves some room for improvement of these nanowired structures. The effect of the QDs deposition method is also evaluated. Both structures show remarkable stability without any appreciable photocurrent loss after 0.5 hour of operation. The fi ndings of this study constitute a relevant step towards the feasibility of hydrogen generation with wide bandgap semiconductors/ quantum dots based heterostructures.
Fil: Rodenas, Pau. Hanyang University; Corea del Sur
Fil: Song, Taesup. Hanyang University; Corea del Sur
Fil: Sudhagar, Pitchaimuthu. Hanyang University; Corea del Sur
Fil: Marzari, Gabriela Lorena. Universitat Jaume I; España. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba; Argentina
Fil: Han, Hyungkyu. Hanyang University; Corea del Sur
Fil: Badia Bou, Laura. Hanyang University; Corea del Sur
Fil: Gimenez, Sixto. Universitat Jaume I; España
Fil: Fabregat-Santiago, Francisco. Universitat Jaume I; España
Fil: Mora Sero, Ivan. Universitat Jaume I; España
Fil: Bisquert, Juan. Universitat Jaume I; España
Fil: Paik, Ungyu. Hanyang University; Corea del Sur
Fil: Kang, Yong Soo. Hanyang University; Corea del Sur
description TiO 2 hollow nanowires (HNWs) and nanoparticles (NPs) constitute prom- ising architectures for QDs sensitized photoanodes for H 2 generation. We sensitize these structures with CdS/CdSe quantum dots by two different methods (chemical bath deposition, CBD and succesive ionic layer adsorp- tion and reaction, SILAR) and evaluate the performance of these photoelec- trodes. Remarkable photocurrents of 4 mA · cm and 8 mA · cm − 2 and hydrogen generation rates of 40 ml · cm − 2 · day − 1 and 80 ml · cm − 2 · day − 1 have been obtained in a three electrode confi guration with sacrifi cial hole scavengers (Na 2 S and Na 2 SO 3 ), for HNWs and NPs respectively, which is confi rmed through gas analysis. More importantly, autonomous generation of H 2 (20 ml · cm − 2 · day − 1 corresponding to 2 mA · cm − 2 photocurrent) is obtained in a two electrode confi guration at short circuit under 100 mW · cm − 2 illumina- tion, clearly showing that these photoanodes can produce hydrogen without the assistance of any external bias. To the best of the authors? knowledge, this is the highest unbiased solar H 2 generation rate reported for these of QDs based heterostructures. Impedance spectroscopy measurements show similar electron density of trap states below the TiO 2 conduction band while the recombination resistance was higher for HNWs, consistently with the much lower surface area compared to NPs. However, the conductivity of both structures is similar, in spite of the one dimensional character of HNWs, which leaves some room for improvement of these nanowired structures. The effect of the QDs deposition method is also evaluated. Both structures show remarkable stability without any appreciable photocurrent loss after 0.5 hour of operation. The fi ndings of this study constitute a relevant step towards the feasibility of hydrogen generation with wide bandgap semiconductors/ quantum dots based heterostructures.
publishDate 2013
dc.date.none.fl_str_mv 2013-02
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/11336/199134
Rodenas, Pau; Song, Taesup; Sudhagar, Pitchaimuthu; Marzari, Gabriela Lorena; Han, Hyungkyu; et al.; Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generation; Wiley-VCH; advanced energy materials; 3; 2; 2-2013; 176-182
1614-6840
CONICET Digital
CONICET
url http://hdl.handle.net/11336/199134
identifier_str_mv Rodenas, Pau; Song, Taesup; Sudhagar, Pitchaimuthu; Marzari, Gabriela Lorena; Han, Hyungkyu; et al.; Quantum dot based heterostructures for unassisted photoelectrochemical hydrogen generation; Wiley-VCH; advanced energy materials; 3; 2; 2-2013; 176-182
1614-6840
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1002/aenm.201200255
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
publisher.none.fl_str_mv Wiley-VCH
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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