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Title: Unexpected molecular weight effect in polymer nanocomposites

Journal Article · · Physical Review Letters
 [1];  [2];  [2];  [2];  [1];  [2];  [2];  [1];  [1];  [2];  [2];  [2];  [3]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Here, the properties of the interfacial layer between the polymer matrix and nanoparticles largely determine the macroscopic properties of polymer nanocomposites (PNCs). Although the static thickness of the interfacial layer was found to increase with the molecular weight (MW), the influence of MW on segmental relaxation and the glass transition in this layer remains to be explored. In this Letter, we show an unexpected MW dependence of the interfacial properties in PNC with attractive polymer-nanoparticle interactions: the thickness of the interfacial layer with hindered segmental relaxation decreases as MW increases, in sharp constrast to theoretical predictions. Further analyses reveal a reduction in mass density of the interfacial layer with increasing MW, which can explain these unexpected dynamic effects. Our observations call for a significant revision of the current understandings of PNCs and suggest interesting ways to tailor their properties.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1265983
Alternate ID(s):
OSTI ID: 1235749
Journal Information:
Physical Review Letters, Vol. 116, Issue 3; ISSN 0031-9007
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 111 works
Citation information provided by
Web of Science

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Cited By (13)

Rheological behavior of fumed silica filled polyethylene oxide journal February 2019
Unexpected Molecular Weight Dependence to the Physical Aging of Thin Polystyrene Films Present at Ultra‐High Molecular Weights journal February 2019
Conformational changes underlying variation in the structural dynamics of materials confined at the nanometric scale journal January 2018
Influence of molecular weight on molecular dynamics and dynamic rheology of polypropylene glycol filled with silica journal January 2018
Segmental and secondary dynamics of nanoparticle-grafted oligomers journal January 2018
Focus: Structure and dynamics of the interfacial layer in polymer nanocomposites with attractive interactions journal May 2017
Influence of knot complexity on glass-formation in low molecular mass ring polymer melts journal March 2019
Heterogeneous dynamics of unentangled chains in polymer nanocomposites journal May 2019
The interfacial zone in thin polymer films and around nanoparticles in polymer nanocomposites journal September 2019
Glass transition of polymers in bulk, confined geometries, and near interfaces journal January 2017
Effect of Local Chain Conformation in Adsorbed Nanolayers on Confined Polymer Molecular Mobility journal May 2019
Initial Solvent-Driven Nonequilibrium Effect on Structure, Properties, and Dynamics of Polymer Nanocomposites journal October 2019
Interfacial Properties and Hopping Diffusion of Small Nanoparticle in Polymer/Nanoparticle Composite with Attractive Interaction on Side Group journal May 2018

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