Resolving Complex K-Pt-Sn Interactions in PtSn@K-MFI Catalysts for Alkane Dehydrogenation

[EN] K and Sn contents were rationalized during the synthesis of PtSn@K-MFI to maximize metal dispersion and stability along the MFI crystallites. Experimental results and theoretical calculations reveal a stoichiometry of similar to 1 K per unit cell of MFI, limiting then the final K incorporation...

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Authors: Martínez-Gómez-Aldaraví, Adrián|||0009-0007-1928-8277, Millán-Cabrera, Reisel|||0000-0002-4489-5411, Vidal Moya, José Alejandro, Martínez, Cristina|||0000-0002-4415-084X, Corma Canós, Avelino|||0000-0002-2232-3527, Boronat Zaragoza, Mercedes|||0000-0002-6211-5888, Serna Merino, Pedro Manuel, Moliner Marin, Manuel|||0000-0002-5440-716X, Millet Roig, Isabel, Alos Marti, Aroa, Meyer, Randall
Format: article
Publication Date:2025
Country:España
Institution:Universitat Politècnica de València (UPV)
Repository:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
Language:English
OAI Identifier:oai:dnet:riunet______::1b8dde5275cffb68acf8cf45571c489b
Online Access:https://riunet.upv.es/handle/10251/234894
Access Level:Open access
Keyword:Catalysts
Crystals
Deactivation
Platinum
Zeolites
07.- Asegurar el acceso a energías asequibles, fiables, sostenibles y modernas para todos
13.- Tomar medidas urgentes para combatir el cambio climático y sus efectos
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oai_identifier_str oai:dnet:riunet______::1b8dde5275cffb68acf8cf45571c489b
network_acronym_str ES
network_name_str España
repository_id_str
dc.title.none.fl_str_mv Resolving Complex K-Pt-Sn Interactions in PtSn@K-MFI Catalysts for Alkane Dehydrogenation
title Resolving Complex K-Pt-Sn Interactions in PtSn@K-MFI Catalysts for Alkane Dehydrogenation
spellingShingle Resolving Complex K-Pt-Sn Interactions in PtSn@K-MFI Catalysts for Alkane Dehydrogenation
Martínez-Gómez-Aldaraví, Adrián|||0009-0007-1928-8277
Catalysts
Crystals
Deactivation
Platinum
Zeolites
07.- Asegurar el acceso a energías asequibles, fiables, sostenibles y modernas para todos
13.- Tomar medidas urgentes para combatir el cambio climático y sus efectos
title_short Resolving Complex K-Pt-Sn Interactions in PtSn@K-MFI Catalysts for Alkane Dehydrogenation
title_full Resolving Complex K-Pt-Sn Interactions in PtSn@K-MFI Catalysts for Alkane Dehydrogenation
title_fullStr Resolving Complex K-Pt-Sn Interactions in PtSn@K-MFI Catalysts for Alkane Dehydrogenation
title_full_unstemmed Resolving Complex K-Pt-Sn Interactions in PtSn@K-MFI Catalysts for Alkane Dehydrogenation
title_sort Resolving Complex K-Pt-Sn Interactions in PtSn@K-MFI Catalysts for Alkane Dehydrogenation
dc.creator.none.fl_str_mv Martínez-Gómez-Aldaraví, Adrián|||0009-0007-1928-8277
Millán-Cabrera, Reisel|||0000-0002-4489-5411
Vidal Moya, José Alejandro
Martínez, Cristina|||0000-0002-4415-084X
Corma Canós, Avelino|||0000-0002-2232-3527
Boronat Zaragoza, Mercedes|||0000-0002-6211-5888
Serna Merino, Pedro Manuel
Moliner Marin, Manuel|||0000-0002-5440-716X
Millet Roig, Isabel
Alos Marti, Aroa
Meyer, Randall
author Martínez-Gómez-Aldaraví, Adrián|||0009-0007-1928-8277
author_facet Martínez-Gómez-Aldaraví, Adrián|||0009-0007-1928-8277
Millán-Cabrera, Reisel|||0000-0002-4489-5411
Vidal Moya, José Alejandro
Martínez, Cristina|||0000-0002-4415-084X
Corma Canós, Avelino|||0000-0002-2232-3527
Boronat Zaragoza, Mercedes|||0000-0002-6211-5888
Serna Merino, Pedro Manuel
Moliner Marin, Manuel|||0000-0002-5440-716X
Millet Roig, Isabel
Alos Marti, Aroa
Meyer, Randall
author_role author
author2 Millán-Cabrera, Reisel|||0000-0002-4489-5411
Vidal Moya, José Alejandro
Martínez, Cristina|||0000-0002-4415-084X
Corma Canós, Avelino|||0000-0002-2232-3527
Boronat Zaragoza, Mercedes|||0000-0002-6211-5888
Serna Merino, Pedro Manuel
Moliner Marin, Manuel|||0000-0002-5440-716X
Millet Roig, Isabel
Alos Marti, Aroa
Meyer, Randall
author2_role author
author
author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Instituto Universitario Mixto de Tecnología Química
Generalitat Valenciana
U.S. Department of Energy
Agencia Estatal de Investigación
Ministerio de Ciencia e Innovación
Repositorio Institucional de la Universitat Politècnica de València Riunet
dc.subject.none.fl_str_mv Catalysts
Crystals
Deactivation
Platinum
Zeolites
07.- Asegurar el acceso a energías asequibles, fiables, sostenibles y modernas para todos
13.- Tomar medidas urgentes para combatir el cambio climático y sus efectos
topic Catalysts
Crystals
Deactivation
Platinum
Zeolites
07.- Asegurar el acceso a energías asequibles, fiables, sostenibles y modernas para todos
13.- Tomar medidas urgentes para combatir el cambio climático y sus efectos
description [EN] K and Sn contents were rationalized during the synthesis of PtSn@K-MFI to maximize metal dispersion and stability along the MFI crystallites. Experimental results and theoretical calculations reveal a stoichiometry of similar to 1 K per unit cell of MFI, limiting then the final K incorporation within siliceous MFI crystals at similar to 0.7 wt %. Above this stoichiometry, K is not incorporated into the final solids unless significant amounts of Sn are simultaneously present, leading to the formation of tin-silicate precipitates. The optimized PtSn@K-MFI catalysts improve the catalytic performance of well-established references, as PtSn/SiO2, for the propane dehydration (PDH) reaction. In particular, low Sn loadings (below 0.5 wt %) result in higher time-on-stream (TOS) deactivation catalytic profiles but excellent regenarability after consecutive PDH reaction, while higher Sn content (close to 1 wt %) minimizes TOS deactivation due to the maximization of Pt-Sn bonds but consecutive regenerations result in significant metal sintering. Increasing Sn contents within MFI crystallites facilitates Pt sintering and, thus, occurring catalyst deactivation upon regeneration cycles. As a result of complex interconnected nucleation/crystallization processes, fine-tuning rationalizations of one-pot synthesis approaches can substantially influence the final atomic and subnanometric metal interactions and, consequently, the catalytic and sintering-resistance properties when exposed to highly demanding industrial conditions.
publishDate 2025
dc.date.none.fl_str_mv 2025
2025-04-01
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://riunet.upv.es/handle/10251/234894
url https://riunet.upv.es/handle/10251/234894
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023 PID2021-122755OB-I00 CATALIZADORES MULTI-FUNCIONALES CON APLICACION EN PROCESOS DE INTERES MEDIOAMBIENTAL E INDUSTRIAL
U.S. Department of Energy https://doi.org/10.13039/100000015 DE-AC02-98CH10886
Generalitat Valenciana https://doi.org/10.13039/501100003359 CIPROM%2F2023%2F34
Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 TED2021-130739B-I00
Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 CEX2021-001230-S
Ministerio de Ciencia e Innovación http://dx.doi.org/10.13039/501100004837 PRE2019-088361
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Reconocimiento (by)
http://creativecommons.org/licenses/by/4.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Reconocimiento (by)
http://creativecommons.org/licenses/by/4.0/
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:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
instname:Universitat Politècnica de València (UPV)
instname_str Universitat Politècnica de València (UPV)
reponame_str RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
collection RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869417493891645440
spelling Resolving Complex K-Pt-Sn Interactions in PtSn@K-MFI Catalysts for Alkane DehydrogenationMartínez-Gómez-Aldaraví, Adrián|||0009-0007-1928-8277Millán-Cabrera, Reisel|||0000-0002-4489-5411Vidal Moya, José AlejandroMartínez, Cristina|||0000-0002-4415-084XCorma Canós, Avelino|||0000-0002-2232-3527Boronat Zaragoza, Mercedes|||0000-0002-6211-5888Serna Merino, Pedro ManuelMoliner Marin, Manuel|||0000-0002-5440-716XMillet Roig, IsabelAlos Marti, AroaMeyer, RandallCatalystsCrystalsDeactivationPlatinumZeolites07.- Asegurar el acceso a energías asequibles, fiables, sostenibles y modernas para todos13.- Tomar medidas urgentes para combatir el cambio climático y sus efectos[EN] K and Sn contents were rationalized during the synthesis of PtSn@K-MFI to maximize metal dispersion and stability along the MFI crystallites. Experimental results and theoretical calculations reveal a stoichiometry of similar to 1 K per unit cell of MFI, limiting then the final K incorporation within siliceous MFI crystals at similar to 0.7 wt %. Above this stoichiometry, K is not incorporated into the final solids unless significant amounts of Sn are simultaneously present, leading to the formation of tin-silicate precipitates. The optimized PtSn@K-MFI catalysts improve the catalytic performance of well-established references, as PtSn/SiO2, for the propane dehydration (PDH) reaction. In particular, low Sn loadings (below 0.5 wt %) result in higher time-on-stream (TOS) deactivation catalytic profiles but excellent regenarability after consecutive PDH reaction, while higher Sn content (close to 1 wt %) minimizes TOS deactivation due to the maximization of Pt-Sn bonds but consecutive regenerations result in significant metal sintering. Increasing Sn contents within MFI crystallites facilitates Pt sintering and, thus, occurring catalyst deactivation upon regeneration cycles. As a result of complex interconnected nucleation/crystallization processes, fine-tuning rationalizations of one-pot synthesis approaches can substantially influence the final atomic and subnanometric metal interactions and, consequently, the catalytic and sintering-resistance properties when exposed to highly demanding industrial conditions.The authors acknowledge financial support by ExxonMobil, by the Spanish Government through PID2021-122755OB-I00 (funded by MCIN/AEI/10.13039/501100011033) and TED2021-130739B-I00 (funded by MCIN/AEI/10.13039/501100011033/EU/PRTR), and by the Generalitat Valenciana through the Prometeo Program (CIPROM/2023/34). The authors are also thankful for the Severo Ochoa financial support by the Spanish Ministry of Science and Innovation (CEX2021-001230-S/funding by MCIN/AEI/10.13039/501100011033). AMGA acknowledges the Spanish Government for a Severo Ochoa FPI scholarship (PRE2019-088361). The Electron Microscopy Service of the UPV is also acknowledged for their help in sample characterization. The XAS results were collected under the PUP-309462 carried out at the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-AC02-98CH10886. RJM and PSM thank Eli Stavitski, Denis Leshchev, and Dominik Wierzbicki for their support at the ISS beamline at NSLS-II. RJM and PSM also thank Corey Kaminsky and Alyssa Love of ExxonMobil for their help with the collection of the XAS data.American Chemical SocietyInstituto Universitario Mixto de Tecnología QuímicaGeneralitat ValencianaU.S. Department of EnergyAgencia Estatal de InvestigaciónMinisterio de Ciencia e InnovaciónRepositorio Institucional de la Universitat Politècnica de València Riunet20252025-04-01journal articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://riunet.upv.es/handle/10251/234894reponame:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valénciainstname:Universitat Politècnica de València (UPV)InglésengAgencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023 PID2021-122755OB-I00 CATALIZADORES MULTI-FUNCIONALES CON APLICACION EN PROCESOS DE INTERES MEDIOAMBIENTAL E INDUSTRIALU.S. Department of Energy https://doi.org/10.13039/100000015 DE-AC02-98CH10886Generalitat Valenciana https://doi.org/10.13039/501100003359 CIPROM%2F2023%2F34Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 TED2021-130739B-I00Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 CEX2021-001230-SMinisterio de Ciencia e Innovación http://dx.doi.org/10.13039/501100004837 PRE2019-088361open accesshttp://purl.org/coar/access_right/c_abf2Reconocimiento (by)http://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:dnet:riunet______::1b8dde5275cffb68acf8cf45571c489b2026-06-13T07:49:27Z
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