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
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/164038
Ver los metadatos del registro completo
id |
CONICETDig_06e022e5d6eb4253a54b21d6977f4022 |
---|---|
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 Técnicas2025-09-29T09:51:58Zoai: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:34982025-09-29 09:51:58.415CONICET 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 |
_version_ |
1844613595742076928 |
score |
13.070432 |