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Title: Interphase Structures and Dynamics near Nanofiller Surfaces in Polymer Solutions

Abstract

Here, we report the in situ structures and dynamics of hydrogenated polybutadiene (PB) chains bound to carbon black nanoparticle surfaces in polymer solutions composed of deuterated PB and deuterated toluene using small-angle neutron scattering and neutron spin-echo techniques together with molecular dynamics (MD) simulations. The experimental results showed that the swollen bound polymer chains exhibit the collective dynamics (the so-called breathing mode) at polymer concentrations ( c) below and above the overlap polymer concentration ( c*) (i.e., 0.61 < c/c* < 1.83), where the concentration profiles of the bound polymer remained unchanged with the different c values. Interestingly, the collective dynamics slowed down by a factor of 2 compared to that in pure d-toluene when the chain lengths of the bound polymer and matrix polymer were equal. However, when the free polymer chains were longer than the bound polymer chains, the decrease in collective dynamics was not as significant. MD simulations were performed to explore the interfacial event as a whole. As a result, we found that the matrix polymer chains, whose length is equal to that of the bound polymer, can be accommodated in the bound polymer layer effectively and are “strangulated” by the bound polymer chains, while themore » longer matrix polymer chains only partly penetrate into the bound chains and the diffusion behavior was hardly affected compared to that in bulk.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [4];  [5];  [5];  [6]; ORCiD logo [1];  [1]
  1. Stony Brook Univ., Stony Brook, NY (United States)
  2. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Indiana Univ., Bloomington, IN (United States)
  3. Kyoto Univ., Kyoto (Japan)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Sumitomo Rubber Industries Ltd., Kobe (Japan)
  6. Cornell Univ., Ithaca, NY (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) (SC-22)
OSTI Identifier:
1483174
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Macromolecules
Additional Journal Information:
Journal Name: Macromolecules; Journal ID: ISSN 0024-9297
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Koga, Tadanori, Barkley, Deborah, Nagao, Michihiro, Taniguchi, Takashi, Carrillo, Jan-Michael Y., Sumpter, Bobby G., Masui, Tomomi, Kishimoto, Hiroyuki, Koga, Maho, Rudick, Jonathan G., and Endoh, Maya K. Interphase Structures and Dynamics near Nanofiller Surfaces in Polymer Solutions. United States: N. p., 2018. Web. doi:10.1021/acs.macromol.8b01615.
Koga, Tadanori, Barkley, Deborah, Nagao, Michihiro, Taniguchi, Takashi, Carrillo, Jan-Michael Y., Sumpter, Bobby G., Masui, Tomomi, Kishimoto, Hiroyuki, Koga, Maho, Rudick, Jonathan G., & Endoh, Maya K. Interphase Structures and Dynamics near Nanofiller Surfaces in Polymer Solutions. United States. doi:10.1021/acs.macromol.8b01615.
Koga, Tadanori, Barkley, Deborah, Nagao, Michihiro, Taniguchi, Takashi, Carrillo, Jan-Michael Y., Sumpter, Bobby G., Masui, Tomomi, Kishimoto, Hiroyuki, Koga, Maho, Rudick, Jonathan G., and Endoh, Maya K. Fri . "Interphase Structures and Dynamics near Nanofiller Surfaces in Polymer Solutions". United States. doi:10.1021/acs.macromol.8b01615.
@article{osti_1483174,
title = {Interphase Structures and Dynamics near Nanofiller Surfaces in Polymer Solutions},
author = {Koga, Tadanori and Barkley, Deborah and Nagao, Michihiro and Taniguchi, Takashi and Carrillo, Jan-Michael Y. and Sumpter, Bobby G. and Masui, Tomomi and Kishimoto, Hiroyuki and Koga, Maho and Rudick, Jonathan G. and Endoh, Maya K.},
abstractNote = {Here, we report the in situ structures and dynamics of hydrogenated polybutadiene (PB) chains bound to carbon black nanoparticle surfaces in polymer solutions composed of deuterated PB and deuterated toluene using small-angle neutron scattering and neutron spin-echo techniques together with molecular dynamics (MD) simulations. The experimental results showed that the swollen bound polymer chains exhibit the collective dynamics (the so-called breathing mode) at polymer concentrations (c) below and above the overlap polymer concentration (c*) (i.e., 0.61 < c/c* < 1.83), where the concentration profiles of the bound polymer remained unchanged with the different c values. Interestingly, the collective dynamics slowed down by a factor of 2 compared to that in pure d-toluene when the chain lengths of the bound polymer and matrix polymer were equal. However, when the free polymer chains were longer than the bound polymer chains, the decrease in collective dynamics was not as significant. MD simulations were performed to explore the interfacial event as a whole. As a result, we found that the matrix polymer chains, whose length is equal to that of the bound polymer, can be accommodated in the bound polymer layer effectively and are “strangulated” by the bound polymer chains, while the longer matrix polymer chains only partly penetrate into the bound chains and the diffusion behavior was hardly affected compared to that in bulk.},
doi = {10.1021/acs.macromol.8b01615},
journal = {Macromolecules},
number = ,
volume = ,
place = {United States},
year = {Fri Nov 16 00:00:00 EST 2018},
month = {Fri Nov 16 00:00:00 EST 2018}
}

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