Methanol production from CO2: Via an integrated, formamide-assisted approach
- Autores
- Uranga, Jorge Gustavo; Gopakumar, Aswin; Pfister, Tim; Imanzade, Gunay; Lombardo, Loris; Gastelu, Gabriela; Züttel, Andreas; Dyson, Paul
- Año de publicación
- 2020
- Idioma
- inglés
- Tipo de recurso
- artículo
- Estado
- versión publicada
- Descripción
- The synthesis of fuels from CO2 has made tremendous progress in recent years, although practical applications remain limited. Herein, we describe a cyclic process that produces MeOH from CO2via formamide intermediates, which are initially reduced using NaBH4 to form methanol and concomitantly release the corresponding amine, from which the formamide is subsequently regenerated in the presence of CO2/NaBH4. By tuning the substituents on the formamide/amine, the selectivity of both steps can be controlled, allowing the process to proceed in high yields, either in two separate steps or in a single step process. The observed trends in reactivity were rationalized with a resonance model of the formamide, which supports the observed trends in reactivity, and further consolidated by spectroscopy and calculations.
Fil: Uranga, Jorge Gustavo. 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. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Gopakumar, Aswin. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Pfister, Tim. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Imanzade, Gunay. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Lombardo, Loris. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Gastelu, Gabriela. 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: Züttel, Andreas. École Polytechnique Fédérale de Lausanne; Suiza
Fil: Dyson, Paul. École Polytechnique Fédérale de Lausanne; Suiza - Materia
-
CO2
Utilización
Metanol
Sustentable - Nivel de accesibilidad
- acceso abierto
- Condiciones de uso
- https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
- Repositorio
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/144354
Ver los metadatos del registro completo
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Methanol production from CO2: Via an integrated, formamide-assisted approachUranga, Jorge GustavoGopakumar, AswinPfister, TimImanzade, GunayLombardo, LorisGastelu, GabrielaZüttel, AndreasDyson, PaulCO2UtilizaciónMetanolSustentablehttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The synthesis of fuels from CO2 has made tremendous progress in recent years, although practical applications remain limited. Herein, we describe a cyclic process that produces MeOH from CO2via formamide intermediates, which are initially reduced using NaBH4 to form methanol and concomitantly release the corresponding amine, from which the formamide is subsequently regenerated in the presence of CO2/NaBH4. By tuning the substituents on the formamide/amine, the selectivity of both steps can be controlled, allowing the process to proceed in high yields, either in two separate steps or in a single step process. The observed trends in reactivity were rationalized with a resonance model of the formamide, which supports the observed trends in reactivity, and further consolidated by spectroscopy and calculations.Fil: Uranga, Jorge Gustavo. 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. École Polytechnique Fédérale de Lausanne; SuizaFil: Gopakumar, Aswin. École Polytechnique Fédérale de Lausanne; SuizaFil: Pfister, Tim. École Polytechnique Fédérale de Lausanne; SuizaFil: Imanzade, Gunay. École Polytechnique Fédérale de Lausanne; SuizaFil: Lombardo, Loris. École Polytechnique Fédérale de Lausanne; SuizaFil: Gastelu, Gabriela. 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: Züttel, Andreas. École Polytechnique Fédérale de Lausanne; SuizaFil: Dyson, Paul. École Polytechnique Fédérale de Lausanne; SuizaRoyal Society of Chemistry2020-04info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/144354Uranga, Jorge Gustavo; Gopakumar, Aswin; Pfister, Tim; Imanzade, Gunay; Lombardo, Loris; et al.; Methanol production from CO2: Via an integrated, formamide-assisted approach; Royal Society of Chemistry; Sustainable Energy and Fuels; 4; 4; 4-2020; 1-72398-4902CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1039/C9SE01141Binfo:eu-repo/semantics/altIdentifier/url/https://pubs.rsc.org/en/content/articlelanding/2020/SE/C9SE01141Binfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:40:47Zoai:ri.conicet.gov.ar:11336/144354instacron: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 10:40:47.812CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse |
dc.title.none.fl_str_mv |
Methanol production from CO2: Via an integrated, formamide-assisted approach |
title |
Methanol production from CO2: Via an integrated, formamide-assisted approach |
spellingShingle |
Methanol production from CO2: Via an integrated, formamide-assisted approach Uranga, Jorge Gustavo CO2 Utilización Metanol Sustentable |
title_short |
Methanol production from CO2: Via an integrated, formamide-assisted approach |
title_full |
Methanol production from CO2: Via an integrated, formamide-assisted approach |
title_fullStr |
Methanol production from CO2: Via an integrated, formamide-assisted approach |
title_full_unstemmed |
Methanol production from CO2: Via an integrated, formamide-assisted approach |
title_sort |
Methanol production from CO2: Via an integrated, formamide-assisted approach |
dc.creator.none.fl_str_mv |
Uranga, Jorge Gustavo Gopakumar, Aswin Pfister, Tim Imanzade, Gunay Lombardo, Loris Gastelu, Gabriela Züttel, Andreas Dyson, Paul |
author |
Uranga, Jorge Gustavo |
author_facet |
Uranga, Jorge Gustavo Gopakumar, Aswin Pfister, Tim Imanzade, Gunay Lombardo, Loris Gastelu, Gabriela Züttel, Andreas Dyson, Paul |
author_role |
author |
author2 |
Gopakumar, Aswin Pfister, Tim Imanzade, Gunay Lombardo, Loris Gastelu, Gabriela Züttel, Andreas Dyson, Paul |
author2_role |
author author author author author author author |
dc.subject.none.fl_str_mv |
CO2 Utilización Metanol Sustentable |
topic |
CO2 Utilización Metanol Sustentable |
purl_subject.fl_str_mv |
https://purl.org/becyt/ford/1.4 https://purl.org/becyt/ford/1 |
dc.description.none.fl_txt_mv |
The synthesis of fuels from CO2 has made tremendous progress in recent years, although practical applications remain limited. Herein, we describe a cyclic process that produces MeOH from CO2via formamide intermediates, which are initially reduced using NaBH4 to form methanol and concomitantly release the corresponding amine, from which the formamide is subsequently regenerated in the presence of CO2/NaBH4. By tuning the substituents on the formamide/amine, the selectivity of both steps can be controlled, allowing the process to proceed in high yields, either in two separate steps or in a single step process. The observed trends in reactivity were rationalized with a resonance model of the formamide, which supports the observed trends in reactivity, and further consolidated by spectroscopy and calculations. Fil: Uranga, Jorge Gustavo. 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. École Polytechnique Fédérale de Lausanne; Suiza Fil: Gopakumar, Aswin. École Polytechnique Fédérale de Lausanne; Suiza Fil: Pfister, Tim. École Polytechnique Fédérale de Lausanne; Suiza Fil: Imanzade, Gunay. École Polytechnique Fédérale de Lausanne; Suiza Fil: Lombardo, Loris. École Polytechnique Fédérale de Lausanne; Suiza Fil: Gastelu, Gabriela. 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: Züttel, Andreas. École Polytechnique Fédérale de Lausanne; Suiza Fil: Dyson, Paul. École Polytechnique Fédérale de Lausanne; Suiza |
description |
The synthesis of fuels from CO2 has made tremendous progress in recent years, although practical applications remain limited. Herein, we describe a cyclic process that produces MeOH from CO2via formamide intermediates, which are initially reduced using NaBH4 to form methanol and concomitantly release the corresponding amine, from which the formamide is subsequently regenerated in the presence of CO2/NaBH4. By tuning the substituents on the formamide/amine, the selectivity of both steps can be controlled, allowing the process to proceed in high yields, either in two separate steps or in a single step process. The observed trends in reactivity were rationalized with a resonance model of the formamide, which supports the observed trends in reactivity, and further consolidated by spectroscopy and calculations. |
publishDate |
2020 |
dc.date.none.fl_str_mv |
2020-04 |
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/11336/144354 Uranga, Jorge Gustavo; Gopakumar, Aswin; Pfister, Tim; Imanzade, Gunay; Lombardo, Loris; et al.; Methanol production from CO2: Via an integrated, formamide-assisted approach; Royal Society of Chemistry; Sustainable Energy and Fuels; 4; 4; 4-2020; 1-7 2398-4902 CONICET Digital CONICET |
url |
http://hdl.handle.net/11336/144354 |
identifier_str_mv |
Uranga, Jorge Gustavo; Gopakumar, Aswin; Pfister, Tim; Imanzade, Gunay; Lombardo, Loris; et al.; Methanol production from CO2: Via an integrated, formamide-assisted approach; Royal Society of Chemistry; Sustainable Energy and Fuels; 4; 4; 4-2020; 1-7 2398-4902 CONICET Digital CONICET |
dc.language.none.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
info:eu-repo/semantics/altIdentifier/doi/10.1039/C9SE01141B info:eu-repo/semantics/altIdentifier/url/https://pubs.rsc.org/en/content/articlelanding/2020/SE/C9SE01141B |
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 |
Royal Society of Chemistry |
publisher.none.fl_str_mv |
Royal Society of Chemistry |
dc.source.none.fl_str_mv |
reponame:CONICET Digital (CONICET) instname:Consejo Nacional de Investigaciones Científicas y Técnicas |
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CONICET Digital (CONICET) |
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CONICET Digital (CONICET) |
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Consejo Nacional de Investigaciones Científicas y Técnicas |
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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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13.070432 |