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Title: Unexpected molecular weight effect in polymer nanocomposites

Abstract

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.

Authors:
 [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)
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:
1265983
Alternate Identifier(s):
OSTI ID: 1235749
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 116; Journal Issue: 3; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Cheng, Shiwang, Holt, Adam P., Wang, Huiqun, Fan, Fei, Bocharova, Vera, Martin, Halie J., Etampawala, Thusitha N., White, Benjamin Tyler, Saito, Tomonori, Kang, Nam -Goo, Dadmun, Mark D., Mays, Jimmy W., and Sokolov, Alexei P. Unexpected molecular weight effect in polymer nanocomposites. United States: N. p., 2016. Web. doi:10.1103/PhysRevLett.116.038302.
Cheng, Shiwang, Holt, Adam P., Wang, Huiqun, Fan, Fei, Bocharova, Vera, Martin, Halie J., Etampawala, Thusitha N., White, Benjamin Tyler, Saito, Tomonori, Kang, Nam -Goo, Dadmun, Mark D., Mays, Jimmy W., & Sokolov, Alexei P. Unexpected molecular weight effect in polymer nanocomposites. United States. doi:10.1103/PhysRevLett.116.038302.
Cheng, Shiwang, Holt, Adam P., Wang, Huiqun, Fan, Fei, Bocharova, Vera, Martin, Halie J., Etampawala, Thusitha N., White, Benjamin Tyler, Saito, Tomonori, Kang, Nam -Goo, Dadmun, Mark D., Mays, Jimmy W., and Sokolov, Alexei P. Fri . "Unexpected molecular weight effect in polymer nanocomposites". United States. doi:10.1103/PhysRevLett.116.038302. https://www.osti.gov/servlets/purl/1265983.
@article{osti_1265983,
title = {Unexpected molecular weight effect in polymer nanocomposites},
author = {Cheng, Shiwang and Holt, Adam P. and Wang, Huiqun and Fan, Fei and Bocharova, Vera and Martin, Halie J. and Etampawala, Thusitha N. and White, Benjamin Tyler and Saito, Tomonori and Kang, Nam -Goo and Dadmun, Mark D. and Mays, Jimmy W. and Sokolov, Alexei P.},
abstractNote = {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.},
doi = {10.1103/PhysRevLett.116.038302},
journal = {Physical Review Letters},
issn = {0031-9007},
number = 3,
volume = 116,
place = {United States},
year = {2016},
month = {1}
}

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Cited by: 25 works
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