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Modeling Retrograde Vitrification in the Polystyrene-Toluene System.

Giuseppe Scherillo1, Valerio Loianno1, Davide Pierleoni2

  • 1Department of Chemical, Materials and Production Engineering (DICMAPI) , University of Naples Federico II , Naples , Italy.

The Journal of Physical Chemistry. B
|March 3, 2018
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Summary

Atactic polystyrene plasticization by toluene vapor causes retrograde vitrification, a rubber to glass transition upon heating at constant pressure. This study theoretically predicts this phenomenon using a lattice fluid model and the Gibbs-Di Marzio criterion.

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Area of Science:

  • Polymer Science
  • Thermodynamics
  • Materials Science

Background:

  • Atactic polystyrene exhibits a significant glass transition change upon exposure to toluene vapor due to plasticization.
  • This plasticization leads to retrograde vitrification, where the material transitions from rubbery to glassy states with increasing temperature at constant vapor pressure.

Purpose of the Study:

  • To theoretically predict the state (rubbery or glassy) of polymer-toluene mixtures.
  • To model the retrograde vitrification phenomenon as a function of toluene vapor pressure and temperature.
  • To validate theoretical predictions against experimental sorption data.

Main Methods:

  • Utilized a nonrandom lattice fluid thermodynamic model for the polymer-toluene mixture.
  • Applied the Gibbs-Di Marzio criterion, equating configurational entropy to zero, to locate the glass transition.
  • Coupled lattice fluid model equations with phase equilibrium and equations of state for polymer and vapor phases.

Main Results:

  • The theoretical approach successfully predicted the state of the polymer-toluene system across varying pressures and temperatures.
  • Theoretical predictions showed good qualitative and quantitative agreement with experimental dynamic sorption results.
  • The model accurately described the retrograde vitrification phenomenon and the glass transition temperature vs. pressure envelope.

Conclusions:

  • The nonrandom lattice fluid model provides a robust theoretical framework for understanding polymer-vapor interactions and phase transitions.
  • The study confirms the Gibbs-Di Marzio criterion's applicability in predicting glass transitions in polymer-penetrant systems.
  • The theoretical approach effectively explains the observed retrograde vitrification in atactic polystyrene-toluene mixtures.