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Title: Molecular simulation study of role of polymer–particle interactions in the strain-dependent viscoelasticity of elastomers (Payne effect)

Abstract

The strain-amplitude dependence of viscoelastic behavior of model crosslinked elastomers containing various concentrations of spherical nanoparticles (NPs) was studied by non-equilibrium molecular dynamics simulation. All the filler NPs were in monodispersed state and the interactions between these particles were purely repulsive. The polymer–particle interactions were attractive and their interaction energies were tuned in a broad range. Through the computational study, many important features of the behavior of particle-reinforced elastomers observed in experiments, including the Payne effect, were successfully reproduced. It was shown that the magnitude of the Payne effect was found to depend on the polymer–particle interaction and the filler loading. By examining the microstructures of the simulation systems and their evolution during oscillatory shear, four different mechanisms for the role of the polymer–particle interactions in the Payne effect were revealed that consist of the debonding of polymer chains from NP surfaces, the breakage of polymer-shell-bridged NP network, the rearrangement of the NPs in the network into different layers and the shear-induced yielding of the rigid polymer shell in-between neighboring NPs.

Authors:
;  [1];  [2]; ;  [3];  [2]; ;  [4];  [2];  [1];  [2];  [2]
  1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029 (China)
  2. (China)
  3. Beijing Engineering Research Center of Advanced Elastomers, Beijing University of Chemical Technology, Beijing 100029 (China)
  4. State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029 (China)
Publication Date:
OSTI Identifier:
22308387
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 141; Journal Issue: 10; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; CROSS-LINKING; ELASTOMERS; MICROSTRUCTURE; MOLECULAR DYNAMICS METHOD; NANOPARTICLES; PARTICLE INTERACTIONS; SIMULATION; SURFACES

Citation Formats

Chen, Yulong, Li, Ziwei, Beijing Engineering Research Center of Advanced Elastomers, Beijing University of Chemical Technology, Beijing 100029, Wen, Shipeng, Zhang, Liqun, State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, Yang, Qingyuan, E-mail: qyyang@mail.buct.edu.cn, E-mail: LiuL@mail.buct.edu.cn, Zhong, Chongli, Laboratory of Advanced Nanostructural Materials, Beijing University of Chemical Technology, Beijing 100029, Liu, Li, E-mail: qyyang@mail.buct.edu.cn, E-mail: LiuL@mail.buct.edu.cn, Beijing Engineering Research Center of Advanced Elastomers, Beijing University of Chemical Technology, Beijing 100029, and Key Laboratory of Carbon Fiber and Functional Polymers, Ministry of Education, Beijing University of Chemical Technology, Beijing 100029. Molecular simulation study of role of polymer–particle interactions in the strain-dependent viscoelasticity of elastomers (Payne effect). United States: N. p., 2014. Web. doi:10.1063/1.4894502.
Chen, Yulong, Li, Ziwei, Beijing Engineering Research Center of Advanced Elastomers, Beijing University of Chemical Technology, Beijing 100029, Wen, Shipeng, Zhang, Liqun, State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, Yang, Qingyuan, E-mail: qyyang@mail.buct.edu.cn, E-mail: LiuL@mail.buct.edu.cn, Zhong, Chongli, Laboratory of Advanced Nanostructural Materials, Beijing University of Chemical Technology, Beijing 100029, Liu, Li, E-mail: qyyang@mail.buct.edu.cn, E-mail: LiuL@mail.buct.edu.cn, Beijing Engineering Research Center of Advanced Elastomers, Beijing University of Chemical Technology, Beijing 100029, & Key Laboratory of Carbon Fiber and Functional Polymers, Ministry of Education, Beijing University of Chemical Technology, Beijing 100029. Molecular simulation study of role of polymer–particle interactions in the strain-dependent viscoelasticity of elastomers (Payne effect). United States. doi:10.1063/1.4894502.
Chen, Yulong, Li, Ziwei, Beijing Engineering Research Center of Advanced Elastomers, Beijing University of Chemical Technology, Beijing 100029, Wen, Shipeng, Zhang, Liqun, State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, Yang, Qingyuan, E-mail: qyyang@mail.buct.edu.cn, E-mail: LiuL@mail.buct.edu.cn, Zhong, Chongli, Laboratory of Advanced Nanostructural Materials, Beijing University of Chemical Technology, Beijing 100029, Liu, Li, E-mail: qyyang@mail.buct.edu.cn, E-mail: LiuL@mail.buct.edu.cn, Beijing Engineering Research Center of Advanced Elastomers, Beijing University of Chemical Technology, Beijing 100029, and Key Laboratory of Carbon Fiber and Functional Polymers, Ministry of Education, Beijing University of Chemical Technology, Beijing 100029. Sun . "Molecular simulation study of role of polymer–particle interactions in the strain-dependent viscoelasticity of elastomers (Payne effect)". United States. doi:10.1063/1.4894502.
@article{osti_22308387,
title = {Molecular simulation study of role of polymer–particle interactions in the strain-dependent viscoelasticity of elastomers (Payne effect)},
author = {Chen, Yulong and Li, Ziwei and Beijing Engineering Research Center of Advanced Elastomers, Beijing University of Chemical Technology, Beijing 100029 and Wen, Shipeng and Zhang, Liqun and State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029 and Yang, Qingyuan, E-mail: qyyang@mail.buct.edu.cn, E-mail: LiuL@mail.buct.edu.cn and Zhong, Chongli and Laboratory of Advanced Nanostructural Materials, Beijing University of Chemical Technology, Beijing 100029 and Liu, Li, E-mail: qyyang@mail.buct.edu.cn, E-mail: LiuL@mail.buct.edu.cn and Beijing Engineering Research Center of Advanced Elastomers, Beijing University of Chemical Technology, Beijing 100029 and Key Laboratory of Carbon Fiber and Functional Polymers, Ministry of Education, Beijing University of Chemical Technology, Beijing 100029},
abstractNote = {The strain-amplitude dependence of viscoelastic behavior of model crosslinked elastomers containing various concentrations of spherical nanoparticles (NPs) was studied by non-equilibrium molecular dynamics simulation. All the filler NPs were in monodispersed state and the interactions between these particles were purely repulsive. The polymer–particle interactions were attractive and their interaction energies were tuned in a broad range. Through the computational study, many important features of the behavior of particle-reinforced elastomers observed in experiments, including the Payne effect, were successfully reproduced. It was shown that the magnitude of the Payne effect was found to depend on the polymer–particle interaction and the filler loading. By examining the microstructures of the simulation systems and their evolution during oscillatory shear, four different mechanisms for the role of the polymer–particle interactions in the Payne effect were revealed that consist of the debonding of polymer chains from NP surfaces, the breakage of polymer-shell-bridged NP network, the rearrangement of the NPs in the network into different layers and the shear-induced yielding of the rigid polymer shell in-between neighboring NPs.},
doi = {10.1063/1.4894502},
journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 10,
volume = 141,
place = {United States},
year = {2014},
month = {9}
}