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Title: Strong Reduction in Amplitude of the Interfacial Segmental Dynamics in Polymer Nanocomposites

Abstract

Despite the wide use of polymer nanocomposites (PNCs) in various applications, our understanding of the microscopic parameters controlling their macroscopic properties remains limited. In this study, we examine the dielectric strength of segmental dynamics, ΔεIL(T) in the interfacial polymer layer surrounding the nanoparticles in PNCs. The presented analysis reveals a significant drop in ΔεIL(T) and its anomalous temperature dependence in the polymer layer adsorbed to nanoparticles. The drop in ΔεIL(T) was observed in all samples regardless of whether segmental relaxation time in the interfacial layer was slower or faster than in the bulk polymer, excluding interpretation of the “dead” layer. We ascribe the observed decrease in the dielectric strength to the restricted amplitude of segmental relaxation in the interfacial/adsorbed layer. Our results provide a new perspective on discussion of dynamics in the interfacial layer in PNCs and thin polymer films, demonstrating that not only segmental relaxation time but also its amplitude can be strongly affected by the interface.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1];  [3]; ORCiD logo [4];  [5];  [1]; ORCiD logo [6]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  2. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics
  3. Montpellier Univ. 2 (France)
  4. Michigan State Univ., East Lansing, MI (United States). Dept. of Chemical Engineering and Materials Science
  5. Kazan Federal Univ. (Russia)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1631231
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Macromolecules
Additional Journal Information:
Journal Volume: 53; Journal Issue: 10; Journal ID: ISSN 0024-9297
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Layers; Molecular dynamics; Nanocomposites; Insulators; Polymers

Citation Formats

Popov, Ivan, Carroll, Bobby, Bocharova, Vera, Genix, Anne-Caroline, Cheng, Shiwang, Khamzin, Airat, Kisliuk, Alexander, and Sokolov, Alexei P. Strong Reduction in Amplitude of the Interfacial Segmental Dynamics in Polymer Nanocomposites. United States: N. p., 2020. Web. https://doi.org/10.1021/acs.macromol.0c00496.
Popov, Ivan, Carroll, Bobby, Bocharova, Vera, Genix, Anne-Caroline, Cheng, Shiwang, Khamzin, Airat, Kisliuk, Alexander, & Sokolov, Alexei P. Strong Reduction in Amplitude of the Interfacial Segmental Dynamics in Polymer Nanocomposites. United States. https://doi.org/10.1021/acs.macromol.0c00496
Popov, Ivan, Carroll, Bobby, Bocharova, Vera, Genix, Anne-Caroline, Cheng, Shiwang, Khamzin, Airat, Kisliuk, Alexander, and Sokolov, Alexei P. Tue . "Strong Reduction in Amplitude of the Interfacial Segmental Dynamics in Polymer Nanocomposites". United States. https://doi.org/10.1021/acs.macromol.0c00496. https://www.osti.gov/servlets/purl/1631231.
@article{osti_1631231,
title = {Strong Reduction in Amplitude of the Interfacial Segmental Dynamics in Polymer Nanocomposites},
author = {Popov, Ivan and Carroll, Bobby and Bocharova, Vera and Genix, Anne-Caroline and Cheng, Shiwang and Khamzin, Airat and Kisliuk, Alexander and Sokolov, Alexei P.},
abstractNote = {Despite the wide use of polymer nanocomposites (PNCs) in various applications, our understanding of the microscopic parameters controlling their macroscopic properties remains limited. In this study, we examine the dielectric strength of segmental dynamics, ΔεIL(T) in the interfacial polymer layer surrounding the nanoparticles in PNCs. The presented analysis reveals a significant drop in ΔεIL(T) and its anomalous temperature dependence in the polymer layer adsorbed to nanoparticles. The drop in ΔεIL(T) was observed in all samples regardless of whether segmental relaxation time in the interfacial layer was slower or faster than in the bulk polymer, excluding interpretation of the “dead” layer. We ascribe the observed decrease in the dielectric strength to the restricted amplitude of segmental relaxation in the interfacial/adsorbed layer. Our results provide a new perspective on discussion of dynamics in the interfacial layer in PNCs and thin polymer films, demonstrating that not only segmental relaxation time but also its amplitude can be strongly affected by the interface.},
doi = {10.1021/acs.macromol.0c00496},
journal = {Macromolecules},
number = 10,
volume = 53,
place = {United States},
year = {2020},
month = {5}
}

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