Modeling for Heterogeneous Oxidative Aging of Polymers Using Coarse-Grained Molecular Dynamics

This study presents a coarse-grained molecular dynamics simulation model to investigate the process of oxidative aging in polymers. The chemical aging effect is attributed to the autoxidation mechanism, which is initiated by radicals, leading to the chain scission and cross-linking of polymer chains. In this study, we integrate a thermal oxidation kinetic model in the oxygen excess regime into the Kremer-Grest model, thereby enabling a reactive coarse-grained molecular dynamics simulation to capture the process of oxidative degradation. Our simulation reveals that when the time scale of the characteristic reaction step of oxidative degradation is shorter than the longest relaxation time of polymer chains, the scission sites exhibit spatial heterogeneity. This innovative simulation model possesses the potential to enhance our comprehension of polymer aging phenomena, thus making noteworthy contributions to the realm of polymer science and degradation chemistry.