Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pH

Autores
Olaya, Astrid Johana; Riva, Jullieta Soledad; Baster, Dominika; Silva, Wanderson O.; Pichard, François; Girault, Hubert
Año de publicación
2021
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Sustainable water oxidation requires low-cost, stable, and efficient redox couples, photosensitizers, and catalysts. Here, we introduce the in situ self-assembly of metal-atom-free organic-based semiconductive structures on the surface of carbon supports. The resulting TTF/TTF•+@carbon junction (TTF = tetrathiafulvalene) acts as an all-in-one highly stable redox-shuttle/photosensitizer/molecular-catalyst triad for the visible-light-driven water oxidation reaction (WOR) at neutral pH, eliminating the need for metallic or organometallic catalysts and sacrificial electron acceptors. A water/butyronitrile emulsion was used to physically separate the photoproducts of the WOR, H+ and TTF, allowing the extraction and subsequent reduction of protons in water, and the in situ electrochemical oxidation of TTF to TTF•+ on carbon in butyronitrile by constant anode potential electrolysis. During 100 h, no decomposition of TTF was observed and O2 was generated from the emulsion while H2 was constantly produced in the aqueous phase. This work opens new perspectives for a new generation of metal-atom-free, low-cost, redox-driven water-splitting strategies.
Fil: Olaya, Astrid Johana. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Riva, Jullieta Soledad. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba; Argentina. Universidad Nacional de Córdoba. Facultad de Matemática, Astronomía y Física; Argentina. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Baster, Dominika. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Silva, Wanderson O.. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Pichard, François. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Girault, Hubert. École Polytechnique Fédérale de Lausanne; Suiza
Materia
WATER OXIDATION
HYDROGEN EVOLUTION
PHOTOCHEMISTRY SUSTAINABLE
REDOX SHUTTLES
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/164038
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/164038
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pHOlaya, Astrid JohanaRiva, Jullieta SoledadBaster, DominikaSilva, Wanderson O.Pichard, FrançoisGirault, HubertWATER OXIDATIONHYDROGEN EVOLUTIONPHOTOCHEMISTRY SUSTAINABLEREDOX SHUTTLEShttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Sustainable water oxidation requires low-cost, stable, and efficient redox couples, photosensitizers, and catalysts. Here, we introduce the in situ self-assembly of metal-atom-free organic-based semiconductive structures on the surface of carbon supports. The resulting TTF/TTF•+@carbon junction (TTF = tetrathiafulvalene) acts as an all-in-one highly stable redox-shuttle/photosensitizer/molecular-catalyst triad for the visible-light-driven water oxidation reaction (WOR) at neutral pH, eliminating the need for metallic or organometallic catalysts and sacrificial electron acceptors. A water/butyronitrile emulsion was used to physically separate the photoproducts of the WOR, H+ and TTF, allowing the extraction and subsequent reduction of protons in water, and the in situ electrochemical oxidation of TTF to TTF•+ on carbon in butyronitrile by constant anode potential electrolysis. During 100 h, no decomposition of TTF was observed and O2 was generated from the emulsion while H2 was constantly produced in the aqueous phase. This work opens new perspectives for a new generation of metal-atom-free, low-cost, redox-driven water-splitting strategies.Fil: Olaya, Astrid Johana. École Polytechnique Fédérale de Lausanne; SuizaFil: Riva, Jullieta Soledad. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba; Argentina. Universidad Nacional de Córdoba. Facultad de Matemática, Astronomía y Física; Argentina. École Polytechnique Fédérale de Lausanne; SuizaFil: Baster, Dominika. École Polytechnique Fédérale de Lausanne; SuizaFil: Silva, Wanderson O.. École Polytechnique Fédérale de Lausanne; SuizaFil: Pichard, François. École Polytechnique Fédérale de Lausanne; SuizaFil: Girault, Hubert. École Polytechnique Fédérale de Lausanne; SuizaAmerican Chemical Society2021-11info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/164038Olaya, Astrid Johana; Riva, Jullieta Soledad; Baster, Dominika; Silva, Wanderson O.; Pichard, François; et al.; Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pH; American Chemical Society; JACS Au; 1; 12; 11-2021; 2294-23022691-3704CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/jacsau.1c00408info:eu-repo/semantics/altIdentifier/doi/10.1021/jacsau.1c00408info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:21:22Zoai:ri.conicet.gov.ar:11336/164038instacron: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:34982025-10-22 11:21:22.826CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pH
title Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pH
spellingShingle Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pH
Olaya, Astrid Johana
WATER OXIDATION
HYDROGEN EVOLUTION
PHOTOCHEMISTRY SUSTAINABLE
REDOX SHUTTLES
title_short Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pH
title_full Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pH
title_fullStr Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pH
title_full_unstemmed Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pH
title_sort Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pH
dc.creator.none.fl_str_mv Olaya, Astrid Johana
Riva, Jullieta Soledad
Baster, Dominika
Silva, Wanderson O.
Pichard, François
Girault, Hubert
author Olaya, Astrid Johana
author_facet Olaya, Astrid Johana
Riva, Jullieta Soledad
Baster, Dominika
Silva, Wanderson O.
Pichard, François
Girault, Hubert
author_role author
author2 Riva, Jullieta Soledad
Baster, Dominika
Silva, Wanderson O.
Pichard, François
Girault, Hubert
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv WATER OXIDATION
HYDROGEN EVOLUTION
PHOTOCHEMISTRY SUSTAINABLE
REDOX SHUTTLES
topic WATER OXIDATION
HYDROGEN EVOLUTION
PHOTOCHEMISTRY SUSTAINABLE
REDOX SHUTTLES
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Sustainable water oxidation requires low-cost, stable, and efficient redox couples, photosensitizers, and catalysts. Here, we introduce the in situ self-assembly of metal-atom-free organic-based semiconductive structures on the surface of carbon supports. The resulting TTF/TTF•+@carbon junction (TTF = tetrathiafulvalene) acts as an all-in-one highly stable redox-shuttle/photosensitizer/molecular-catalyst triad for the visible-light-driven water oxidation reaction (WOR) at neutral pH, eliminating the need for metallic or organometallic catalysts and sacrificial electron acceptors. A water/butyronitrile emulsion was used to physically separate the photoproducts of the WOR, H+ and TTF, allowing the extraction and subsequent reduction of protons in water, and the in situ electrochemical oxidation of TTF to TTF•+ on carbon in butyronitrile by constant anode potential electrolysis. During 100 h, no decomposition of TTF was observed and O2 was generated from the emulsion while H2 was constantly produced in the aqueous phase. This work opens new perspectives for a new generation of metal-atom-free, low-cost, redox-driven water-splitting strategies.
Fil: Olaya, Astrid Johana. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Riva, Jullieta Soledad. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba; Argentina. Universidad Nacional de Córdoba. Facultad de Matemática, Astronomía y Física; Argentina. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Baster, Dominika. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Silva, Wanderson O.. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Pichard, François. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Girault, Hubert. École Polytechnique Fédérale de Lausanne; Suiza
description Sustainable water oxidation requires low-cost, stable, and efficient redox couples, photosensitizers, and catalysts. Here, we introduce the in situ self-assembly of metal-atom-free organic-based semiconductive structures on the surface of carbon supports. The resulting TTF/TTF•+@carbon junction (TTF = tetrathiafulvalene) acts as an all-in-one highly stable redox-shuttle/photosensitizer/molecular-catalyst triad for the visible-light-driven water oxidation reaction (WOR) at neutral pH, eliminating the need for metallic or organometallic catalysts and sacrificial electron acceptors. A water/butyronitrile emulsion was used to physically separate the photoproducts of the WOR, H+ and TTF, allowing the extraction and subsequent reduction of protons in water, and the in situ electrochemical oxidation of TTF to TTF•+ on carbon in butyronitrile by constant anode potential electrolysis. During 100 h, no decomposition of TTF was observed and O2 was generated from the emulsion while H2 was constantly produced in the aqueous phase. This work opens new perspectives for a new generation of metal-atom-free, low-cost, redox-driven water-splitting strategies.
publishDate 2021
dc.date.none.fl_str_mv 2021-11
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/11336/164038
Olaya, Astrid Johana; Riva, Jullieta Soledad; Baster, Dominika; Silva, Wanderson O.; Pichard, François; et al.; Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pH; American Chemical Society; JACS Au; 1; 12; 11-2021; 2294-2302
2691-3704
CONICET Digital
CONICET
url http://hdl.handle.net/11336/164038
identifier_str_mv Olaya, Astrid Johana; Riva, Jullieta Soledad; Baster, Dominika; Silva, Wanderson O.; Pichard, François; et al.; Visible-Light-Driven Water Oxidation on Self-Assembled Metal-Free Organic@Carbon Junctions at Neutral pH; American Chemical Society; JACS Au; 1; 12; 11-2021; 2294-2302
2691-3704
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://pubs.acs.org/doi/10.1021/jacsau.1c00408
info:eu-repo/semantics/altIdentifier/doi/10.1021/jacsau.1c00408
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
dc.format.none.fl_str_mv 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 12.982451

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