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 τcc, and two related structural scaling regimes.
- Authors:
-
[1];
[1];
- 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)
- 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. https://doi.org/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. https://doi.org/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}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 4 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Nanocomposites with Polymer Grafted Nanoparticles
journal, April 2013
- Kumar, Sanat K.; Jouault, Nicolas; Benicewicz, Brian
- Macromolecules, Vol. 46, Issue 9
Role of isostaticity and load-bearing microstructure in the elasticity of yielded colloidal gels
journal, September 2012
- Hsiao, L. C.; Newman, R. S.; Glotzer, S. C.
- Proceedings of the National Academy of Sciences, Vol. 109, Issue 40
Nonlinearity in the Dynamic Properties of Vulcanized Rubber Compounds
journal, March 1954
- Fletcher, W. P.; Gent, A. N.
- Rubber Chemistry and Technology, Vol. 27, Issue 1
The dynamic properties of carbon black-loaded natural rubber vulcanizates. Part I
journal, January 1962
- Payne, A. R.
- Journal of Applied Polymer Science, Vol. 6, Issue 19
Carbon Black Structure in Rubber
journal, March 1963
- Payne, A. R.; Watson, W. F.
- Rubber Chemistry and Technology, Vol. 36, Issue 1
Dynamic properties of heat-treated butyl vulcanizates
journal, May 1963
- Payne, A. R.
- Journal of Applied Polymer Science, Vol. 7, Issue 3
Low Strain Dynamic Properties of Filled Rubbers
journal, May 1971
- Payne, A. R.; Whittaker, R. E.
- Rubber Chemistry and Technology, Vol. 44, Issue 2
Energy Dissipation and the Fracture of Rubber Vulcanizates
journal, July 1991
- Hamed, Gary R.
- Rubber Chemistry and Technology, Vol. 64, Issue 3
Limiting Law of the Reinforcement of Rubber
journal, November 1944
- Smallwood, Hugh M.
- Journal of Applied Physics, Vol. 15, Issue 11
Theory of Filler Reinforcement
journal, January 1945
- Guth, Eugene
- Journal of Applied Physics, Vol. 16, Issue 1
Effective Degree of Immobilization of Rubber Occluded within Carbon Black Aggregates
journal, September 1972
- Medalia, A. I.
- Rubber Chemistry and Technology, Vol. 45, Issue 5
Filler—Elastomer Interactions. Part IV. The Effect of the Surface Energies of Fillers on Elastomer Reinforcement
journal, May 1992
- Wolff, Siegfried; Wang, Meng-Jiao
- Rubber Chemistry and Technology, Vol. 65, Issue 2
Effect of structural arrest on Poisson’s ratio in nanoreinforced elastomers
journal, May 2007
- Robertson, C. G.; Bogoslovov, R.; Roland, C. M.
- Physical Review E, Vol. 75, Issue 5
Morphology of aggregates
journal, January 1970
- Medalia, Avrom I.
- Journal of Colloid and Interface Science, Vol. 32, Issue 1
On the Mechanism of Hydrodynamic Reinforcement in Elastic Composites
journal, November 2002
- Huber, Gregor
- Macromolecules, Vol. 35, Issue 24
Nanoparticle self-assembly: from interactions in suspension to polymer nanocomposites
journal, January 2018
- Genix, Anne-Caroline; Oberdisse, Julian
- Soft Matter, Vol. 14, Issue 25
Macromolecular Diffusion in a Crowded Polymer Nanocomposite
journal, May 2011
- Gam, Sangah; Meth, Jeffrey S.; Zane, Steve G.
- Macromolecules, Vol. 44, Issue 9
Carbon Blacks for Highly Conductive Rubber
journal, March 1957
- Polley, M. H.; Boonstra, B. B. S. T.
- Rubber Chemistry and Technology, Vol. 30, Issue 1
Carbon Black Morphology in Rubber
journal, September 1977
- McDonald, G. C.; Hess, W. M.
- Rubber Chemistry and Technology, Vol. 50, Issue 4
Effect of Carbon Black and Silica Fillers in Elastomer Blends
journal, September 2001
- Zhang, Yimin; Ge, S.; Tang, B.
- Macromolecules, Vol. 34, Issue 20
Phase structure and adhesion in polymer blends: A criterion for rubber toughening
journal, November 1985
- Wu, Souheng
- Polymer, Vol. 26, Issue 12
Filler-Elastomer Interactions. Part VIII. The Role of the Distance between Filler Aggregates in the Dynamic Properties of Filled Vulcanizates
journal, May 1993
- Wang, Meng-Jiao; Wolff, Siegfried; Tan, Ewe-Hong
- Rubber Chemistry and Technology, Vol. 66, Issue 2
Electron tomography provides a direct link between the Payne effect and the inter-particle spacing of rubber composites
journal, December 2014
- Staniewicz, Lech; Vaudey, Thomas; Degrandcourt, Christophe
- Scientific Reports, Vol. 4, Issue 1
Solution of the tunneling-percolation problem in the nanocomposite regime
journal, April 2010
- Ambrosetti, G.; Grimaldi, C.; Balberg, I.
- Physical Review B, Vol. 81, Issue 15
Visualizing the Toughening Mechanism of Nanofiller with 3D X-ray Nano-CT: Stress-Induced Phase Separation of Silica Nanofiller and Silicone Polymer Double Networks
journal, September 2017
- Song, Lixian; Wang, Zhen; Tang, Xiaoliang
- Macromolecules, Vol. 50, Issue 18
Visualization of filler network in silicone rubber with confocal laser-scanning microscopy
journal, January 2017
- Liu, Min; Kang, Ming; Mou, Yongren
- RSC Advances, Vol. 7, Issue 84
A pseudo-thermodynamic description of dispersion for nanocomposites
journal, October 2017
- Jin, Yan; Beaucage, Gregory; Vogtt, Karsten
- Polymer, Vol. 129
Structural Emergence in Particle Dispersions
journal, November 2017
- Mulderig, Andrew; Beaucage, Gregory; Vogtt, Karsten
- Langmuir, Vol. 33, Issue 49
Structural studies of complex systems using small-angle scattering: a unified Guinier/power-law approach
journal, September 1994
- Beaucage, G.; Schaefer, D. W.
- Journal of Non-Crystalline Solids, Vol. 172-174
Approximations Leading to a Unified Exponential/Power-Law Approach to Small-Angle Scattering
journal, December 1995
- Beaucage, G.
- Journal of Applied Crystallography, Vol. 28, Issue 6
Small-Angle Scattering from Polymeric Mass Fractals of Arbitrary Mass-Fractal Dimension
journal, April 1996
- Beaucage, G.
- Journal of Applied Crystallography, Vol. 29, Issue 2
Analysis of structures of rubber-filler systems with combined scattering methods
journal, November 2012
- Takenaka, Mikihito
- Polymer Journal, Vol. 45, Issue 1
Determination of branch fraction and minimum dimension of mass-fractal aggregates
journal, September 2004
- Beaucage, G.
- Physical Review E, Vol. 70, Issue 3
Particle size distributions from small-angle scattering using global scattering functions
journal, July 2004
- Beaucage, G.; Kammler, H. K.; Pratsinis, S. E.
- Journal of Applied Crystallography, Vol. 37, Issue 4
Multiscale Filler Structure in Simplified Industrial Nanocomposite Silica/SBR Systems Studied by SAXS and TEM
journal, December 2012
- Baeza, Guilhem P.; Genix, Anne-Caroline; Degrandcourt, Christophe
- Macromolecules, Vol. 46, Issue 1
Thermodynamic stability of worm-like micelle solutions
journal, January 2017
- Vogtt, Karsten; Beaucage, Gregory; Weaver, Michael
- Soft Matter, Vol. 13, Issue 36
Elastic properties of nanoparticle chain aggregates of TiO2, Al2O3, and Fe2O3 generated by laser ablation
journal, January 2000
- Ogawa, K.; Vogt, T.; Ullmann, M.
- Journal of Applied Physics, Vol. 87, Issue 1
Viscoelasticity and Structure of Polystyrene/Fumed Silica Nanocomposites: Filler Network and Hydrodynamic Contributions
journal, February 2010
- Filippone, Giovanni; Romeo, Giovanni; Acierno, Domenico
- Langmuir, Vol. 26, Issue 4
Tuning Structure and Rheology of Silica–Latex Nanocomposites with the Molecular Weight of Matrix Chains: A Coupled SAXS–TEM–Simulation Approach
journal, April 2014
- Banc, Amélie; Genix, Anne-Caroline; Chirat, Mathieu
- Macromolecules, Vol. 47, Issue 9
Percolation Concept: Polymer-Filler Gel Formation, Electrical Conductivity and Dynamic Electrical Properties of Carbon-Black-Filled Rubbers
journal, February 1996
- Karásek, Ludek; Meissner, Bohumil; Asai, Shigeo
- Polymer Journal, Vol. 28, Issue 2
Structure and dynamics of carbon black-filled elastomers
journal, January 2000
- Yurekli, K.; Krishnamoorti, R.; Tse, M. F.
- Journal of Polymer Science Part B: Polymer Physics, Vol. 39, Issue 2
On the critical conductive filler loading in antistatic composites
journal, February 1975
- Janzen, Jay
- Journal of Applied Physics, Vol. 46, Issue 2
The effect of DBP of carbon black on the dynamic self-assembly in a polymer melt
journal, January 2016
- Li, Xiaoyu; Deng, Hua; Zhang, Qin
- RSC Advances, Vol. 6, Issue 30
Payne effect and shear elasticity of silica-filled polymers in concentrated solutions and in molten state
journal, April 2003
- Cassagnau, Philippe
- Polymer, Vol. 44, Issue 8
Scaling of the Viscoelasticity of Weakly Attractive Particles
journal, July 2000
- Trappe, V.; Weitz, D. A.
- Physical Review Letters, Vol. 85, Issue 2
Mechanical selfsimilarity of polymers during chemical gelation
journal, June 1988
- Vilgis, T. A.; Winter, H. H.
- Colloid & Polymer Science, Vol. 266, Issue 6
Topological properties of diffusion limited aggregation and cluster-cluster aggregation
journal, December 1984
- Meakin, P.; Majid, I.; Havlin, S.
- Journal of Physics A: Mathematical and General, Vol. 17, Issue 18
Density of states on fractals : « fractons »
journal, January 1982
- Alexander, S.; Orbach, R.
- Journal de Physique Lettres, Vol. 43, Issue 17
Ultra-small-angle X-ray scattering at the Advanced Photon Source
journal, April 2009
- Ilavsky, Jan; Jemian, Pete R.; Allen, Andrew J.
- Journal of Applied Crystallography, Vol. 42, Issue 3
Quantification of branching in fumed silica
journal, July 2017
- Mulderig, Andrew; Beaucage, Gregory; Vogtt, Karsten
- Journal of Aerosol Science, Vol. 109
New Insight into Hierarchical Structures of Carbon Black Dispersed in Polymer Matrices: A Combined Small-Angle Scattering Study
journal, December 2007
- Koga, Tadanori; Hashimoto, Takeji; Takenaka, Mikihito
- Macromolecules, Vol. 41, Issue 2
Multidimensional Nature of Fluidized Nanoparticle Agglomerates
journal, October 2014
- de Martín, Lilian; Bouwman, Wim G.; van Ommen, J. Ruud
- Langmuir, Vol. 30, Issue 42
Rheological Properties of Anionic Polystyrenes. II. Dynamic Viscoelasticity of Blends of Narrow-Distribution Polystyrenes
journal, March 1970
- Masuda, Toshiro; Kitagawa, Keishi; Inoue, Toshio
- Macromolecules, Vol. 3, Issue 2
A Unifying Approach for the Linear Viscoelasticity of Polymer Nanocomposites
journal, October 2012
- Filippone, Giovanni; Salzano de Luna, Martina
- Macromolecules, Vol. 45, Issue 21
Linear viscoelasticity of polymer melts filled with nano-sized fillers
journal, June 2010
- Song, Yihu; Zheng, Qiang
- Polymer, Vol. 51, Issue 14
Application of two phase model to linear viscoelasticity of reinforced rubbers
journal, February 2011
- Song, Yihu; Zheng, Qiang
- Polymer, Vol. 52, Issue 3
Nanotube Networks in Polymer Nanocomposites: Rheology and Electrical Conductivity
journal, November 2004
- Du, Fangming; Scogna, Robert C.; Zhou, Wei
- Macromolecules, Vol. 37, Issue 24
Nanoscale Particle Motion in Attractive Polymer Nanocomposites
journal, December 2017
- Senses, Erkan; Narayanan, Suresh; Mao, Yimin
- Physical Review Letters, Vol. 119, Issue 23
Modeling of dynamic-mechanical behavior of reinforced elastomers using a multiscale approach
journal, January 2016
- Ivaneiko, I.; Toshchevikov, V.; Saphiannikova, M.
- Polymer, Vol. 82
Superposition approach to the dynamic-mechanical behaviour of reinforced rubbers
journal, October 2017
- Ivaneiko, I.; Toshchevikov, V.; Stöckelhuber, K. W.
- Polymer, Vol. 127
Network dynamics in nanofilled polymers
journal, April 2016
- Baeza, Guilhem P.; Dessi, Claudia; Costanzo, Salvatore
- Nature Communications, Vol. 7, Issue 1
Influence of Carbon Nanotube Aspect Ratio on Normal Stress Differences in Isotactic Polypropylene Nanocomposite Melts
journal, February 2008
- Xu, Dong-Hua; Wang, Zhi-Gang; Douglas, Jack F.
- Macromolecules, Vol. 41, Issue 3
Works referencing / citing this record:
Structural identification of percolation of nanoparticles
journal, January 2020
- Musino, Dafne; Genix, Anne-Caroline; Chauveau, Edouard
- Nanoscale, Vol. 12, Issue 6