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

YL Chen and ZW Li and SP Wen and QY Yang and LQ Zhang and CL Zhong and L Liu, JOURNAL OF CHEMICAL PHYSICS, 141, 104901 (2014).

DOI: 10.1063/1.4894502

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. (C) 2014 AIP Publishing LLC.

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