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Understanding the underlying processes associated with the viscoelasticity performance of ethylene-propylene-diene monomer (EPDM) during its service life is essential for assessing and predicting its waterproofing performance in underground infrastructure. The viscoelasticity of the polymer is closely related to its free volume, and both of these properties depend on multiple factors, such as temperature, stress magnitude, and strain level. To explore the fundamental viscoelastic behavior of EPDM using free volume as a proxy for viscoelasticity, this article investigates the influence of temperature, stress magnitude, and strain level, as well as their combined effect, on the free volume through molecular dynamics (MD) simulations. An EPDM cross-linked molecular model was built and verified by comparing the simulation values of glass transition temperature, mechanical properties, and gas diffusivity with the experimental results reported in the literature. Then, the dependence of EPDM's fractional free volume on temperature, strain, and their combined effect was investigated via MD simulations, on the basis of which the applicability of various superposition principles was also evaluated.

Understanding Free Volume Characteristics of Ethylene-Propylene-Diene Monomer (EPDM) through Molecular Dynamics Simulations