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
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/144354
Acceder
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spelling 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 Técnicas2025-10-22T12:13:16Zoai: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:34982025-10-22 12:13:16.911CONICET 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
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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