Impact of topology framework of microporous solids on methanol carbonylation: An operando DRIFTS-MS study

Methanol carbonylation was evaluated over heterogeneous catalysts based on Cu-exchanged zeolitic materials with different topology: Cu@MOR, Cu@FER, and Cu@ZSM-5. Despite the similar Si/Al ratios, it is crucial to acknowledge that the acid strength is influenced by the framework topology, as supporte...

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Autores: Luque-Álvarez, L. A., Serrano-Cruz, M., González Castaño, M., Bobadilla, Luis F., Odriozola, José Antonio
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2023
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/355437
Acceso en línea:http://hdl.handle.net/10261/355437
https://api.elsevier.com/content/abstract/scopus_id/85164722497
Access Level:acceso abierto
Palabra clave:Heterogeneous catalysts
Methanol carbonylation
Operando DRIFTS-MS
Zeolites topology
http://vocabularies.unesco.org/thesaurus/concept640
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spelling Impact of topology framework of microporous solids on methanol carbonylation: An operando DRIFTS-MS studyLuque-Álvarez, L. A.Serrano-Cruz, M.González Castaño, M.Bobadilla, Luis F.Odriozola, José AntonioHeterogeneous catalystsMethanol carbonylationOperando DRIFTS-MSZeolites topologyhttp://vocabularies.unesco.org/thesaurus/concept640Methanol carbonylation was evaluated over heterogeneous catalysts based on Cu-exchanged zeolitic materials with different topology: Cu@MOR, Cu@FER, and Cu@ZSM-5. Despite the similar Si/Al ratios, it is crucial to acknowledge that the acid strength is influenced by the framework topology, as supported by the NH3-TPD results. This, along with other characterization techniques allowed us to estimate the impact of pore size and pore distribution in these microporous materials on catalytic performance. The channel structure influenced catalytic parameters such as conversion and selectivity. The higher methanol conversion achieved on Cu@FER shows the importance of Brønsted acid sites and redox centres location regarding the topology of the material. Concerning the selectivity, the production of acetic acid was endorsed by the 12-MR (MOR) channels, methyl acetate's production by the 10-MR (FER) channels. Finally, the presence of 6-MR (ZSM-5) channels led to a complete selectivity towards DME production. The reaction mechanism was elucidated via operando DRIFTS-MS and results revealed a bifunctional mechanism in which methanol adsorbs and dehydrates on acidic Brønsted sites and CO is activated over Cu+ species.Financial support for this work has been obtained from the Spanish Ministerio de Ciencia e Innovación through the project SMART-FTS (PID2021-126876OB-I00). Miriam González Castaño acknowledges the University of Sevilla for her postdoctoral contract Maria Zambrano (MZAMBRANO-2021-198). Ligia A. Luque Álvarez thanks VI-PPITUS (University of Sevilla) for her current predoctoral contract. Moreover, Melania Serrano Cruz thanks the SECAT (Sociedad Española de Catálisis) for the grant of a scholarship to carry out the master's thesis.Peer reviewedElsevierUniversidad de SevillaMinisterio de Ciencia e Innovación (España)Agencia Estatal de Investigación (España)González Castaño, M.[0000-0003-2575-8398]Bobadilla, Luis F.[0000-0003-0085-9811]Odriozola, José Antonio[0000-0002-8283-0459]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202420242023info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionapplication/pdfhttp://hdl.handle.net/10261/355437https://api.elsevier.com/content/abstract/scopus_id/85164722497reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2021-126876OB-I00Microporous and Mesoporous Materialshttps://doi.org/10.1016/j.micromeso.2023.112725Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3554372026-05-22T06:33:51Z
dc.title.none.fl_str_mv Impact of topology framework of microporous solids on methanol carbonylation: An operando DRIFTS-MS study
title Impact of topology framework of microporous solids on methanol carbonylation: An operando DRIFTS-MS study
spellingShingle Impact of topology framework of microporous solids on methanol carbonylation: An operando DRIFTS-MS study
Luque-Álvarez, L. A.
Heterogeneous catalysts
Methanol carbonylation
Operando DRIFTS-MS
Zeolites topology
http://vocabularies.unesco.org/thesaurus/concept640
title_short Impact of topology framework of microporous solids on methanol carbonylation: An operando DRIFTS-MS study
title_full Impact of topology framework of microporous solids on methanol carbonylation: An operando DRIFTS-MS study
title_fullStr Impact of topology framework of microporous solids on methanol carbonylation: An operando DRIFTS-MS study
title_full_unstemmed Impact of topology framework of microporous solids on methanol carbonylation: An operando DRIFTS-MS study
title_sort Impact of topology framework of microporous solids on methanol carbonylation: An operando DRIFTS-MS study
dc.creator.none.fl_str_mv Luque-Álvarez, L. A.
Serrano-Cruz, M.
González Castaño, M.
Bobadilla, Luis F.
Odriozola, José Antonio
author Luque-Álvarez, L. A.
author_facet Luque-Álvarez, L. A.
Serrano-Cruz, M.
González Castaño, M.
Bobadilla, Luis F.
Odriozola, José Antonio
author_role author
author2 Serrano-Cruz, M.
González Castaño, M.
Bobadilla, Luis F.
Odriozola, José Antonio
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Universidad de Sevilla
Ministerio de Ciencia e Innovación (España)
Agencia Estatal de Investigación (España)
González Castaño, M.[0000-0003-2575-8398]
Bobadilla, Luis F.[0000-0003-0085-9811]
Odriozola, José Antonio[0000-0002-8283-0459]
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Heterogeneous catalysts
Methanol carbonylation
Operando DRIFTS-MS
Zeolites topology
http://vocabularies.unesco.org/thesaurus/concept640
topic Heterogeneous catalysts
Methanol carbonylation
Operando DRIFTS-MS
Zeolites topology
http://vocabularies.unesco.org/thesaurus/concept640
description Methanol carbonylation was evaluated over heterogeneous catalysts based on Cu-exchanged zeolitic materials with different topology: Cu@MOR, Cu@FER, and Cu@ZSM-5. Despite the similar Si/Al ratios, it is crucial to acknowledge that the acid strength is influenced by the framework topology, as supported by the NH3-TPD results. This, along with other characterization techniques allowed us to estimate the impact of pore size and pore distribution in these microporous materials on catalytic performance. The channel structure influenced catalytic parameters such as conversion and selectivity. The higher methanol conversion achieved on Cu@FER shows the importance of Brønsted acid sites and redox centres location regarding the topology of the material. Concerning the selectivity, the production of acetic acid was endorsed by the 12-MR (MOR) channels, methyl acetate's production by the 10-MR (FER) channels. Finally, the presence of 6-MR (ZSM-5) channels led to a complete selectivity towards DME production. The reaction mechanism was elucidated via operando DRIFTS-MS and results revealed a bifunctional mechanism in which methanol adsorbs and dehydrates on acidic Brønsted sites and CO is activated over Cu+ species.
publishDate 2023
dc.date.none.fl_str_mv 2023
2024
2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Postprint
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/355437
https://api.elsevier.com/content/abstract/scopus_id/85164722497
url http://hdl.handle.net/10261/355437
https://api.elsevier.com/content/abstract/scopus_id/85164722497
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/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2021-126876OB-I00
Microporous and Mesoporous Materials
https://doi.org/10.1016/j.micromeso.2023.112725
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
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
repository.name.fl_str_mv
repository.mail.fl_str_mv
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