Impact of an Emergent Hierarchical Filler Network on Nanocomposite Dynamics

Rishi, Kabir; Beaucage, Gregory; Kuppa, Vikram; Mulderig, Andrew; Narayanan, Vishak; McGlasson, Alex; Rackaitis, Mindaugas; Ilavsky, Jan

doi:10.1021/acs.macromol.8b01510

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

Journal Article · 01 October 2018 · Macromolecules

DOI: https://doi.org/10.1021/acs.macromol.8b01510 · OSTI ID:1484238

^[1];

^[1]; Kuppa, Vikram ^[2]; Mulderig, Andrew ^[1]; Narayanan, Vishak ^[1]; McGlasson, Alex ^[1]; Rackaitis, Mindaugas ^[3]; Ilavsky, Jan ^[4]

Univ. of Cincinnati, Cincinnati, OH (United States)
Univ. of Dayton Research Institute, Dayton, OH (United States)
Bridgestone Americas Center for Research and Technology, Akron, OH (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1484238

Journal Information:: Macromolecules, Vol. 51, Issue 20; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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