Efficient DMF-assisted synthesis of formamides from amines using CO2 catalyzed by heterogeneous metal-free imidazolium-hypercrosslinked polymers

CO2 emissions are constantly increasing, so it is necessary to continue working to mitigate the excess of CO2 in the atmosphere and reduce the effects it has on the environment. In this regard, we have developed novel catalysts by synthesizing ionic liquids based on imidazolium chloride, supported o...

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Autores: Fuerte-Díez, Beatriz, Rangel-Rangel, Elizabeth, Iglesias, Marta, Maya, Eva M.
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2024
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/377487
Acceso en línea:http://hdl.handle.net/10261/377487
https://www.scopus.com/inward/record.uri?eid=2-s2.0-85182878030&doi=10.1016%2fj.jcou.2024.102679&partnerID=40&md5=c74d07dc93c2d86f41e5bd3432887d9e
Access Level:acceso abierto
Palabra clave:CO2
DMF
Hypercrosslinked polymers
Imidazolium
N-formylation
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spelling Efficient DMF-assisted synthesis of formamides from amines using CO2 catalyzed by heterogeneous metal-free imidazolium-hypercrosslinked polymersFuerte-Díez, BeatrizRangel-Rangel, ElizabethIglesias, MartaMaya, Eva M.CO2DMFHypercrosslinked polymersImidazoliumN-formylationCO2 emissions are constantly increasing, so it is necessary to continue working to mitigate the excess of CO2 in the atmosphere and reduce the effects it has on the environment. In this regard, we have developed novel catalysts by synthesizing ionic liquids based on imidazolium chloride, supported on hyper-crosslinked polymers (HCP-BzmimCl and HCP-Bis(BzmimCl)). These catalysts enable the highly selective N-formylation of secondary amines, utilizing CO2 as a carbon source, phenylsilane as a hydrogen donor, and DMF as a crucial polar additive. The reactions were carried out under mild conditions, with CO2 pressure at 5 bar and a temperature of 35ºC, yielding formamides in excellent yields. HCP-Bis(BzmimCl) has emerged as a particularly promising catalyst, boasting shorter reaction times, exceptional recyclability, and scalability for potential industrial applications. © 2024 The AuthorsThis work was supported by the project CATCO2NVERS funded by the European Union´s Horizon 2020 research and innovation program under grant agreement No 101000580.Peer reviewedElsevierEuropean CommissionConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202520252024info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionhttp://hdl.handle.net/10261/377487https://www.scopus.com/inward/record.uri?eid=2-s2.0-85182878030&doi=10.1016%2fj.jcou.2024.102679&partnerID=40&md5=c74d07dc93c2d86f41e5bd3432887d9ereponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/EC/H2020/101000580Journal of CO2 Utilizationhttps://doi.org/10.1016/j.jcou.2024.102679Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3774872026-05-22T06:33:51Z
dc.title.none.fl_str_mv Efficient DMF-assisted synthesis of formamides from amines using CO2 catalyzed by heterogeneous metal-free imidazolium-hypercrosslinked polymers
title Efficient DMF-assisted synthesis of formamides from amines using CO2 catalyzed by heterogeneous metal-free imidazolium-hypercrosslinked polymers
spellingShingle Efficient DMF-assisted synthesis of formamides from amines using CO2 catalyzed by heterogeneous metal-free imidazolium-hypercrosslinked polymers
Fuerte-Díez, Beatriz
CO2
DMF
Hypercrosslinked polymers
Imidazolium
N-formylation
title_short Efficient DMF-assisted synthesis of formamides from amines using CO2 catalyzed by heterogeneous metal-free imidazolium-hypercrosslinked polymers
title_full Efficient DMF-assisted synthesis of formamides from amines using CO2 catalyzed by heterogeneous metal-free imidazolium-hypercrosslinked polymers
title_fullStr Efficient DMF-assisted synthesis of formamides from amines using CO2 catalyzed by heterogeneous metal-free imidazolium-hypercrosslinked polymers
title_full_unstemmed Efficient DMF-assisted synthesis of formamides from amines using CO2 catalyzed by heterogeneous metal-free imidazolium-hypercrosslinked polymers
title_sort Efficient DMF-assisted synthesis of formamides from amines using CO2 catalyzed by heterogeneous metal-free imidazolium-hypercrosslinked polymers
dc.creator.none.fl_str_mv Fuerte-Díez, Beatriz
Rangel-Rangel, Elizabeth
Iglesias, Marta
Maya, Eva M.
author Fuerte-Díez, Beatriz
author_facet Fuerte-Díez, Beatriz
Rangel-Rangel, Elizabeth
Iglesias, Marta
Maya, Eva M.
author_role author
author2 Rangel-Rangel, Elizabeth
Iglesias, Marta
Maya, Eva M.
author2_role author
author
author
dc.contributor.none.fl_str_mv European Commission
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv CO2
DMF
Hypercrosslinked polymers
Imidazolium
N-formylation
topic CO2
DMF
Hypercrosslinked polymers
Imidazolium
N-formylation
description CO2 emissions are constantly increasing, so it is necessary to continue working to mitigate the excess of CO2 in the atmosphere and reduce the effects it has on the environment. In this regard, we have developed novel catalysts by synthesizing ionic liquids based on imidazolium chloride, supported on hyper-crosslinked polymers (HCP-BzmimCl and HCP-Bis(BzmimCl)). These catalysts enable the highly selective N-formylation of secondary amines, utilizing CO2 as a carbon source, phenylsilane as a hydrogen donor, and DMF as a crucial polar additive. The reactions were carried out under mild conditions, with CO2 pressure at 5 bar and a temperature of 35ºC, yielding formamides in excellent yields. HCP-Bis(BzmimCl) has emerged as a particularly promising catalyst, boasting shorter reaction times, exceptional recyclability, and scalability for potential industrial applications. © 2024 The Authors
publishDate 2024
dc.date.none.fl_str_mv 2024
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/377487
https://www.scopus.com/inward/record.uri?eid=2-s2.0-85182878030&doi=10.1016%2fj.jcou.2024.102679&partnerID=40&md5=c74d07dc93c2d86f41e5bd3432887d9e
url http://hdl.handle.net/10261/377487
https://www.scopus.com/inward/record.uri?eid=2-s2.0-85182878030&doi=10.1016%2fj.jcou.2024.102679&partnerID=40&md5=c74d07dc93c2d86f41e5bd3432887d9e
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/EC/H2020/101000580
Journal of CO2 Utilization
https://doi.org/10.1016/j.jcou.2024.102679

dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Elsevier
publisher.none.fl_str_mv Elsevier
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
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repository.mail.fl_str_mv
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