4.8 Article

Ion-Pairs in Aluminosilicate-Alkali Synthesis Liquids Determine the Aluminum Content and Topology of Crystallizing Zeolites

Journal

CHEMISTRY OF MATERIALS
Volume -, Issue -, Pages -

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.2c00773

Keywords

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Funding

  1. Flemish Government
  2. Flemish Science Foundation (FWO) [G083318N]
  3. European Research Council (ERC) [834134]
  4. Austrian Science Fund (FWF) [ZeoDirect I3680-N34]
  5. FWO [1.5.061.18N]
  6. Hercules Foundation [AKUL/13/21]
  7. Flemish Government [I001321N]
  8. department EWI via the Hermes Fund [AH.2016.134]
  9. FWO Vlaanderen [G083318N]
  10. FWF austria [G083318N]
  11. European Research Council (ERC) [834134] Funding Source: European Research Council (ERC)

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By using hydrated silicate ionic liquids, the phase selection and framework silicon-to-aluminum ratio during inorganic zeolite synthesis can be studied. The synthesis allows for control of crystallization parameters and evaluation of yield and sample homogeneity. The results show a correlation between batch stoichiometry and framework aluminum content, which is dependent on the type of alkali cation. The framework aluminum content also changes gradually with batch alkalinity and dilution.
Using hydrated silicate ionic liquids, phase selection and framework silicon-to-aluminum ratio during inorganic zeolite synthesis were studied as a function of batch composition. Consisting of homogeneous single phasic liquids, this synthesis concept allows careful control of crystallization parameters and evaluation of yield and sample homogeneity. Ternary phase diagrams were constructed for syntheses at 90 degrees C for I week. The results reveal a cation-dependent continuous relation between batch stoichiometry and framework aluminum content, valid across the phase boundaries of all different zeolites formed in the system. The framework aluminum content directly correlates to the type of alkali cation and gradually changes with batch alkalinity and dilution. This suggests that the observed zeolites form through a solution-mediated mechanism involving the concerted assembly of soluble cation-oligomer ion pairs. Phase selection is a consequence of the stability for a particular framework at the given aluminum content and alkali type.

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