Novel effects of confinement and interfaces on the glass transition temperature and physical aging in polymer films and nanocomposites

John M Torkelson*, Rodney D. Priestley, Perla Rittigstein, Manish K. Mundra, Connie B. Roth

*Corresponding author for this work

Research output: Chapter in Book/Report/Conference proceedingConference contribution

11 Citations (Scopus)

Abstract

Recently, it has become evident that the magnitude of the glass transition (Tg)-confinement effect depends strongly on the polymer repeat unit and that the magnitude of the physical aging rate can be dramatically reduced relative to neat polymer when attractive polymer-nanofiller interactions are present in well-dispersed nanocomposites. However, in neither case has a quantitative, fundamental understanding been developed. By studying polymers with different chain backbone stiffness, e.g., polystyrene (PS) vs. polycarbonate (PC) vs. polysulfone (PSF) and that lack attractive interactions with the substrate interface, we show that the Tg-confinement effect is the weakest in the polymer with the least stiff backbone (PS) and strongest in the polymer with the most stiff backbone (PSF). These results are consisten with the notion that, other things being equal, a larger requirement by the polymer for the cooperativity of the segmental mobility that is associated with the glass transition will result in a greater reduction of Tg near the free surface of the film and thus the average Tg across the film. A quantitative understanding of the causes behind the effects of confinement on the glass transition and physical aging of nanocomposites with dispersed nanofiller is prevented by the complex nanoparticle distribution. Here, we have developed model silica nanocomposites with a single, quantifiable interlayer spacing equal to the film thickness separating two silica slides. Comparisons show that the model nanocomposites yield results consistent with the complex real nanocomposites. This provides the possibility to conduct studies that will allow for an understanding of how the separation distance between nanofiller interfaces impacts the glass transition and physical aging.

Original languageEnglish (US)
Title of host publicationComplex Systems - 5th International Workshop on Complex Systems
Pages192-195
Number of pages4
Volume982
DOIs
StatePublished - Mar 13 2008
Event5th International Workshop on Complex Systems - Sendai, Japan
Duration: Sep 25 2007Sep 28 2007

Other

Other5th International Workshop on Complex Systems
CountryJapan
CitySendai
Period9/25/079/28/07

Fingerprint

glass transition temperature
nanocomposites
polymers
glass
polystyrene
silicon dioxide
polycarbonates
chutes
interlayers
stiffness
film thickness
spacing
interactions
nanoparticles
requirements
causes

Keywords

  • Glass transition
  • Nanocomposites
  • Physical aging
  • Thin polymer films

ASJC Scopus subject areas

  • Physics and Astronomy(all)

Cite this

Torkelson, J. M., Priestley, R. D., Rittigstein, P., Mundra, M. K., & Roth, C. B. (2008). Novel effects of confinement and interfaces on the glass transition temperature and physical aging in polymer films and nanocomposites. In Complex Systems - 5th International Workshop on Complex Systems (Vol. 982, pp. 192-195) https://doi.org/10.1063/1.2897781
Torkelson, John M ; Priestley, Rodney D. ; Rittigstein, Perla ; Mundra, Manish K. ; Roth, Connie B. / Novel effects of confinement and interfaces on the glass transition temperature and physical aging in polymer films and nanocomposites. Complex Systems - 5th International Workshop on Complex Systems. Vol. 982 2008. pp. 192-195
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Torkelson, JM, Priestley, RD, Rittigstein, P, Mundra, MK & Roth, CB 2008, Novel effects of confinement and interfaces on the glass transition temperature and physical aging in polymer films and nanocomposites. in Complex Systems - 5th International Workshop on Complex Systems. vol. 982, pp. 192-195, 5th International Workshop on Complex Systems, Sendai, Japan, 9/25/07. https://doi.org/10.1063/1.2897781

Novel effects of confinement and interfaces on the glass transition temperature and physical aging in polymer films and nanocomposites. / Torkelson, John M; Priestley, Rodney D.; Rittigstein, Perla; Mundra, Manish K.; Roth, Connie B.

Complex Systems - 5th International Workshop on Complex Systems. Vol. 982 2008. p. 192-195.

Research output: Chapter in Book/Report/Conference proceedingConference contribution

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AU - Torkelson, John M

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AU - Roth, Connie B.

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N2 - Recently, it has become evident that the magnitude of the glass transition (Tg)-confinement effect depends strongly on the polymer repeat unit and that the magnitude of the physical aging rate can be dramatically reduced relative to neat polymer when attractive polymer-nanofiller interactions are present in well-dispersed nanocomposites. However, in neither case has a quantitative, fundamental understanding been developed. By studying polymers with different chain backbone stiffness, e.g., polystyrene (PS) vs. polycarbonate (PC) vs. polysulfone (PSF) and that lack attractive interactions with the substrate interface, we show that the Tg-confinement effect is the weakest in the polymer with the least stiff backbone (PS) and strongest in the polymer with the most stiff backbone (PSF). These results are consisten with the notion that, other things being equal, a larger requirement by the polymer for the cooperativity of the segmental mobility that is associated with the glass transition will result in a greater reduction of Tg near the free surface of the film and thus the average Tg across the film. A quantitative understanding of the causes behind the effects of confinement on the glass transition and physical aging of nanocomposites with dispersed nanofiller is prevented by the complex nanoparticle distribution. Here, we have developed model silica nanocomposites with a single, quantifiable interlayer spacing equal to the film thickness separating two silica slides. Comparisons show that the model nanocomposites yield results consistent with the complex real nanocomposites. This provides the possibility to conduct studies that will allow for an understanding of how the separation distance between nanofiller interfaces impacts the glass transition and physical aging.

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Torkelson JM, Priestley RD, Rittigstein P, Mundra MK, Roth CB. Novel effects of confinement and interfaces on the glass transition temperature and physical aging in polymer films and nanocomposites. In Complex Systems - 5th International Workshop on Complex Systems. Vol. 982. 2008. p. 192-195 https://doi.org/10.1063/1.2897781