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Area of Science:

  • Materials Science
  • Polymer Science
  • Physical Chemistry

Background:

  • Diffusion of small molecules in polymer matrices is crucial for material properties.
  • Polymer nanocomposites often exhibit reduced diffusion coefficients compared to pure polymers.
  • Existing models primarily consider geometric tortuosity, potentially overlooking other factors.

Purpose of the Study:

  • To investigate the mechanisms behind reduced small molecule diffusion in polymer-nanoparticle composites.
  • To decouple the contributions of free volume changes and energetic interactions to diffusion.
  • To provide quantitative evidence for the role of diffusant-filler interactions.

Main Methods:

  • Utilized a model composite of silica nanoparticles in poly(methyl acrylate).
  • Conducted ethyl acetate sorption experiments near the polymer's glass transition temperature.
  • Applied the Vrentas-Duda free volume theory to separate energetic and free-volume effects.
  • Compared diffusion behavior of ethyl acetate (hydrogen bonding) and benzene (non-hydrogen bonding).

Main Results:

  • Nanoparticle addition did not significantly alter polymer segmental dynamics or free volume.
  • The energy barrier for ethyl acetate diffusion doubled with 40 vol% silica nanoparticles.
  • Hydrogen bonding interactions between silica and ethyl acetate were identified as a key factor.
  • Benzene diffusion coefficients were consistent with geometric tortuosity alone.

Conclusions:

  • Diffusant-filler energetic interactions, particularly hydrogen bonding, are critical in reducing diffusion in polymer nanocomposites.
  • Geometric blocking effects alone do not fully explain the observed diffusion reductions.
  • This study offers quantitative evidence that attractive interactions significantly impact diffusivity in such systems.