Multiscale modeling of the effects of unlimited four-membered ring formation on sol-gel silica film molecular structure

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1 Scopus citations

Abstract

A modified multiscale model of a sol-gel silica drying process is presented that treats first-shell substitution effects and unlimited four-membered ring cyclization. The inclusion of four-membered (8-atom) rings allows the model to simulate the formation of the tetrasiloxane rings and cubic silsesquioxane cages known to be prevalent components of sol-gel silica systems, as well as a full range of other ring-containing structures. The polymerization process is treated using a dynamic Monte Carlo method where a discrete population of one million monomers evolves according to kinetic rules, including unimolecular-like closure of three-bond blocks. Compared with prior simulations with extensive cyclization that allowed only three-membered rings, the molecular structures formed with unlimited four-membered ring are more complex, and the occurrence of "skinning" (the rapid formation of a gel only at the surface of the film) is more pronounced and leads to more severe structure gradients.

Original languageEnglish
Pages (from-to)707-718
Number of pages12
JournalAICHE Journal
Volume59
Issue number3
DOIs
StatePublished - Mar 2013

Keywords

  • Dynamic Monte Carlo
  • Film
  • Four-membered rings
  • Multiscale modeling
  • Polycondensation
  • Sol-gel silica

ASJC Scopus subject areas

  • Biotechnology
  • Environmental Engineering
  • General Chemical Engineering

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