Synthesis of pure silica MFI zeolites using imidazolium-based long dications. A comparative study of structure-directing effects derived from a further spacer length increase

[EN] Length-dependent structure direction of linear methylimidazolium-based dications towards MFI zeolite, previously known only for the tetramethylene spacer, has also been found for octamethylene and decamethylene spacers. This works only under highly concentrated conditions, whereas dilution alwa...

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Detalles Bibliográficos
Autores: Lu, Peng, Gómez-Hortigüela Sainz, Luis, Camblor, Miguel Ángel
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2018
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/200457
Acceso en línea:http://hdl.handle.net/10261/200457
Access Level:acceso abierto
Palabra clave:Zeolites
Descripción
Sumario:[EN] Length-dependent structure direction of linear methylimidazolium-based dications towards MFI zeolite, previously known only for the tetramethylene spacer, has also been found for octamethylene and decamethylene spacers. This works only under highly concentrated conditions, whereas dilution always tends to favor TON, a default structure that is the only zeolite obtained with the other reported dications (with tri-, penta-, and hexamethylene spacers). The locations and conformations of the dications have been studied by molecular mechanics simulations. As longer dications introduce lower density of positive charges in the zeolite, the density of connectivity defects also decreases. Finally, these long dications cannot easily place each charged imidazolium ring in the two possible orientations (either parallel or perpendicular to 4MR close to F sites) found for the tetramethylene case. Hence, although the three MFI materials display two F NMR resonances at similar chemical shifts, their relative intensities strongly vary as a function of the spacer length.