Issue 22, 2018

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

Abstract

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 19F NMR resonances at similar chemical shifts, their relative intensities strongly vary as a function of the spacer length.

Graphical abstract: 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

Supplementary files

Article information

Article type
Paper
Submitted
23 Mar 2018
Accepted
06 May 2018
First published
07 May 2018

Dalton Trans., 2018,47, 7498-7504

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

P. Lu, L. Gómez-Hortigüela and M. A. Camblor, Dalton Trans., 2018, 47, 7498 DOI: 10.1039/C8DT01127C

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