A Classical Molecular Dynamics Study on the Effect of Si/Al Ratio and Silanol Nest Defects on Water Diffusion in Zeolite HY

A. J. Porter, A. J. O' Malley

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The diffusion of water confined in zeolite HY has been studied using classical molecular dynamics at 300 K to probe the effects of water loading, Si/Al ratio, and silanol nest defect presence on the behavior of water confined in Brønsted acidic faujasite (FAU) zeolites. Water loading, ranging from 5 to 33 wt %, is shown to have a significant effect on diffusivity, showing an increase by a factor of ∼7 over the loading range, toward a maximum diffusivity. Upon probing the effect of Si/Al ratio (in a range of Si/Al = 5 to fully siliceous), water diffusivity tends to decrease with the concentration of Brønsted acid sites which show strong interactions with the water molecules and thus hinder molecular mobility. The average residence time of water adsorbed to each Brønsted acid site also decreased with both water loading and Si/Al ratio. Water diffusivity shows the highest dependency on Si/Al ratio at 18 wt % loading, as a lack of total mobility in the systems at the lowest loadings is observed (due to significant populations of water molecules being immobilized via interaction with the framework and Brønsted acid sites), and less of a dependence is observed at the highest loadings due to the prevalence of sorbate-sorbate interactions. Notably, silanol nest presence (at a concentration of 1 per unit cell) had no significant effect on the diffusivity of water in HY at any water loading or Si/Al ratio. Reasons considered for this lack of influence include silanol geometry and flexibility at ambient temperature and potentially a lower effective charge density of the defect site.

Original languageEnglish
Pages (from-to)11567-11579
Number of pages13
JournalJournal of Physical Chemistry C
Issue number21
Early online date19 May 2021
Publication statusPublished - 3 Jun 2021

Bibliographical note

Funding Information:
This work was supported by the UK Engineering and Physical Sciences Research Council (EPSRC) grant EP/R513155/1 for the University of Bath. This research made use of the Balena High Performance Computing (HPC) Service at the University of Bath. A.J.O.M. acknowledges Roger and Sue Whorrod for the funding of a Whorrod Fellowship. We also thank Professor Steve Parker, Dr. Carlos Hernandez Tamargo, and Sandra McHugh for their valuable discussion and insight.

Publisher Copyright:
© 2021 American Chemical Society.

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • General Energy
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films


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