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Title: Impact of an Emergent Hierarchical Filler Network on Nanocomposite Dynamics

Abstract

Aggregated polymer fillers, such as carbon black and silica, at concentrations above the percolation threshold form an emergent structure, the hierarchical filler network, in immiscible systems where dispersion is driven by accumulated strain. It is proposed that the hierarchical filler network is composed of a primary nanoscale network that locally percolates at ~5 vol % of aggregates, associated with changes in the dynamic spectrum at low strain, and a secondary micrometer-scale network that globally percolates at ~20 vol % associated with the Payne effect and electrical conductivity. A model is proposed with an elastomer dominated dynamic response described by Einstein–Smallwood behavior at high frequencies and small sizes and a filler network dominated response at low frequencies and large sizes. The nanoscale mesh size correlates with this transition in low strain dynamic response. The micrometer-scale network displays a gel-like dynamic response at very low frequencies and a corresponding gel-like structural scaling regime at large sizes. In conclusion, the hierarchical filler network is described by two crossover frequencies and associated relaxation times, τ* and τ cc, and two related structural scaling regimes.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [1];  [1];  [1];  [3];  [4]
  1. Univ. of Cincinnati, Cincinnati, OH (United States)
  2. Univ. of Dayton Research Institute, Dayton, OH (United States)
  3. Bridgestone Americas Center for Research and Technology, Akron, OH (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE Office of Science (SC)
OSTI Identifier:
1484238
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Macromolecules
Additional Journal Information:
Journal Volume: 51; Journal Issue: 20; Journal ID: ISSN 0024-9297
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Rishi, Kabir, Beaucage, Gregory, Kuppa, Vikram, Mulderig, Andrew, Narayanan, Vishak, McGlasson, Alex, Rackaitis, Mindaugas, and Ilavsky, Jan. Impact of an Emergent Hierarchical Filler Network on Nanocomposite Dynamics. United States: N. p., 2018. Web. doi:10.1021/acs.macromol.8b01510.
Rishi, Kabir, Beaucage, Gregory, Kuppa, Vikram, Mulderig, Andrew, Narayanan, Vishak, McGlasson, Alex, Rackaitis, Mindaugas, & Ilavsky, Jan. Impact of an Emergent Hierarchical Filler Network on Nanocomposite Dynamics. United States. doi:10.1021/acs.macromol.8b01510.
Rishi, Kabir, Beaucage, Gregory, Kuppa, Vikram, Mulderig, Andrew, Narayanan, Vishak, McGlasson, Alex, Rackaitis, Mindaugas, and Ilavsky, Jan. Mon . "Impact of an Emergent Hierarchical Filler Network on Nanocomposite Dynamics". United States. doi:10.1021/acs.macromol.8b01510. https://www.osti.gov/servlets/purl/1484238.
@article{osti_1484238,
title = {Impact of an Emergent Hierarchical Filler Network on Nanocomposite Dynamics},
author = {Rishi, Kabir and Beaucage, Gregory and Kuppa, Vikram and Mulderig, Andrew and Narayanan, Vishak and McGlasson, Alex and Rackaitis, Mindaugas and Ilavsky, Jan},
abstractNote = {Aggregated polymer fillers, such as carbon black and silica, at concentrations above the percolation threshold form an emergent structure, the hierarchical filler network, in immiscible systems where dispersion is driven by accumulated strain. It is proposed that the hierarchical filler network is composed of a primary nanoscale network that locally percolates at ~5 vol % of aggregates, associated with changes in the dynamic spectrum at low strain, and a secondary micrometer-scale network that globally percolates at ~20 vol % associated with the Payne effect and electrical conductivity. A model is proposed with an elastomer dominated dynamic response described by Einstein–Smallwood behavior at high frequencies and small sizes and a filler network dominated response at low frequencies and large sizes. The nanoscale mesh size correlates with this transition in low strain dynamic response. The micrometer-scale network displays a gel-like dynamic response at very low frequencies and a corresponding gel-like structural scaling regime at large sizes. In conclusion, the hierarchical filler network is described by two crossover frequencies and associated relaxation times, τ* and τcc, and two related structural scaling regimes.},
doi = {10.1021/acs.macromol.8b01510},
journal = {Macromolecules},
number = 20,
volume = 51,
place = {United States},
year = {2018},
month = {10}
}

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