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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Detalles Bibliográficos
Autores: 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
Tipo de recurso: artículo
Fecha de publicación:2025
País:España
Institución:Universitat Politècnica de València (UPV)
Repositorio:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
Idioma:inglés
OAI Identifier:oai:dnet:riunet______::1b8dde5275cffb68acf8cf45571c489b
Acceso en línea:https://riunet.upv.es/handle/10251/234894
Access Level:acceso abierto
Palabra clave:Catalysts
Crystals
Deactivation
Platinum
Zeolites
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Descripción
Sumario:[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.