Role of strontium cations in ZSM-5 zeolite in the methanol-to-hydrocarbons reaction

The selectivity of the methanol-to-hydrocarbons (MTH) reaction can be tuned by modifying zeolite catalysts with alkaline earth metals, which typically increase propylene selectivity and catalyst stability. Here we employed Sr2+ as its higher atomic number in comparison to the zeolite T atoms facilit...

Descripción completa

Detalles Bibliográficos
Autores: Liutkova, Anna, Drozhzhin, Victor, Heinrichs, Jason M. J. J., Jestl, Valentin, Evtushkova, Angelina, Mezari, Brahim, Mayoral, Álvaro, Kosinov, Nikolay, Hensen, Emiel J. M.
Tipo de recurso: artículo
Estado:Versión publicada
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:10261/344409
Acceso en línea:http://hdl.handle.net/10261/344409
Access Level:acceso abierto
Palabra clave:ddc:530
id ES_5f47f79dfe1f6bbfacaef5ab35ebcdea
oai_identifier_str oai:digital.csic.es:10261/344409
network_acronym_str ES
network_name_str España
repository_id_str
dc.title.none.fl_str_mv Role of strontium cations in ZSM-5 zeolite in the methanol-to-hydrocarbons reaction
title Role of strontium cations in ZSM-5 zeolite in the methanol-to-hydrocarbons reaction
spellingShingle Role of strontium cations in ZSM-5 zeolite in the methanol-to-hydrocarbons reaction
Liutkova, Anna
ddc:530
title_short Role of strontium cations in ZSM-5 zeolite in the methanol-to-hydrocarbons reaction
title_full Role of strontium cations in ZSM-5 zeolite in the methanol-to-hydrocarbons reaction
title_fullStr Role of strontium cations in ZSM-5 zeolite in the methanol-to-hydrocarbons reaction
title_full_unstemmed Role of strontium cations in ZSM-5 zeolite in the methanol-to-hydrocarbons reaction
title_sort Role of strontium cations in ZSM-5 zeolite in the methanol-to-hydrocarbons reaction
dc.creator.none.fl_str_mv Liutkova, Anna
Drozhzhin, Victor
Heinrichs, Jason M. J. J.
Jestl, Valentin
Evtushkova, Angelina
Mezari, Brahim
Mayoral, Álvaro
Kosinov, Nikolay
Hensen, Emiel J. M.
author Liutkova, Anna
author_facet Liutkova, Anna
Drozhzhin, Victor
Heinrichs, Jason M. J. J.
Jestl, Valentin
Evtushkova, Angelina
Mezari, Brahim
Mayoral, Álvaro
Kosinov, Nikolay
Hensen, Emiel J. M.
author_role author
author2 Drozhzhin, Victor
Heinrichs, Jason M. J. J.
Jestl, Valentin
Evtushkova, Angelina
Mezari, Brahim
Mayoral, Álvaro
Kosinov, Nikolay
Hensen, Emiel J. M.
author2_role author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Netherlands Organization for Scientific Research
Ministry of Education, Culture and Science (The Netherlands)
European Commission
Agencia Estatal de Investigación (España)
Ministerio de Ciencia, Innovación y Universidades (España)
Ministerio de Ciencia e Innovación (España)
Gobierno de Aragón
National Natural Science Foundation of China
Shanghai Synchrotron Radiation Facility
ShanghaiTech University
Diputación General de Aragón
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv ddc:530
topic ddc:530
description The selectivity of the methanol-to-hydrocarbons (MTH) reaction can be tuned by modifying zeolite catalysts with alkaline earth metals, which typically increase propylene selectivity and catalyst stability. Here we employed Sr2+ as its higher atomic number in comparison to the zeolite T atoms facilitates characterization by scanning transmission electron microscopy and operando X-ray absorption spectroscopy. Sr2+ dispersed in the ZSM-5 micropores coordinates water, methanol, and dimethyl ether during the MTH reaction. Complementary characterization with nuclear magnetic resonance spectroscopy, thermogravimetric analysis combined with mass spectrometry, operando infrared spectroscopy, and X-ray diffraction points to the retention of substantially more adsorbates during the MTH reaction in comparison to Sr-free zeolites. Our findings support the notion that alkaline earth metals modify the porous reaction environment such that the olefin cycle is favored over the aromatic cycle in the MTH, explaining the increased propylene yield and lower deactivation rate.
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
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/344409
url http://hdl.handle.net/10261/344409
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/EC/H2020/801359
info:eu-repo/grantAgreement/EC/H2020/823717
info:eu-repo/grantAgreement/AEI//RYC2018-024561-I
https://doi.org/10.1021/acs.jpclett.3c01259
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 American Chemical Society
publisher.none.fl_str_mv American Chemical Society
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
_version_ 1869409194461888512
spelling Role of strontium cations in ZSM-5 zeolite in the methanol-to-hydrocarbons reactionLiutkova, AnnaDrozhzhin, VictorHeinrichs, Jason M. J. J.Jestl, ValentinEvtushkova, AngelinaMezari, BrahimMayoral, ÁlvaroKosinov, NikolayHensen, Emiel J. M.ddc:530The selectivity of the methanol-to-hydrocarbons (MTH) reaction can be tuned by modifying zeolite catalysts with alkaline earth metals, which typically increase propylene selectivity and catalyst stability. Here we employed Sr2+ as its higher atomic number in comparison to the zeolite T atoms facilitates characterization by scanning transmission electron microscopy and operando X-ray absorption spectroscopy. Sr2+ dispersed in the ZSM-5 micropores coordinates water, methanol, and dimethyl ether during the MTH reaction. Complementary characterization with nuclear magnetic resonance spectroscopy, thermogravimetric analysis combined with mass spectrometry, operando infrared spectroscopy, and X-ray diffraction points to the retention of substantially more adsorbates during the MTH reaction in comparison to Sr-free zeolites. Our findings support the notion that alkaline earth metals modify the porous reaction environment such that the olefin cycle is favored over the aromatic cycle in the MTH, explaining the increased propylene yield and lower deactivation rate.This work was supported by The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement no. 801359. We acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research were performed at Petra III, and we thank Dr. Edmund Welter for assistance in using P65 beamline. Beamtime was allocated for proposal I-20211187 EC XAS measurements. We acknowledge ALBA synchrotron for provision of synchrotron radiation facilities: to record the XAS data at BL22 CLÆSS under proposal no. AV-2021024881. We thank Dr. Vlad Martin-Diaconescu for assistance and support in using beamline BL22 CLÆSS, proposal no. AV-2021024881. We acknowledge the European Synchrotron Radiation Facility (ESRF) for provision of synchrotron radiation facilities: to record the XRD data under proposal no. CH6231 at ID31. We thank Dr. Marta Mirolo for assistance and support in using beamline ID31, proposal no. CH6231. This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 823717-ESTEEM3. A.M. acknowledges the Spanish Ministry of Science (RYC2018-024561-I), the regional government of Aragon (DGA E13_20R), the National Natural Science Foundation of China (NSFC-21835002), the Centre for High-resolution Electron Microscopy (ChEM, EM02161943), and Shanghai Key-Laboratory of HREM (21DZ2260400), ShanghaiTech University.Peer reviewedAmerican Chemical SocietyNetherlands Organization for Scientific ResearchMinistry of Education, Culture and Science (The Netherlands)European CommissionAgencia Estatal de Investigación (España)Ministerio de Ciencia, Innovación y Universidades (España)Ministerio de Ciencia e Innovación (España)Gobierno de AragónNational Natural Science Foundation of ChinaShanghai Synchrotron Radiation FacilityShanghaiTech UniversityDiputación General de AragónConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202420242023info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionapplication/pdfhttp://hdl.handle.net/10261/344409reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/EC/H2020/801359info:eu-repo/grantAgreement/EC/H2020/823717info:eu-repo/grantAgreement/AEI//RYC2018-024561-Ihttps://doi.org/10.1021/acs.jpclett.3c01259Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3444092026-05-22T06:33:51Z
score 15.811543

Similares en LA Referencia