Analysis of static and dynamic mechanical properties of carbon black/carbon nanotubes hybrid filled natural rubber nanocomposites using coarse‐grained molecular dynamics

Abstract Nanoparticle (NP)‐filled natural rubber (NR) has attracted much attention owing to their prominent mechanical strength, stiffness, and wear resistance. In this study, the static and dynamic mechanical properties of carbon black (CB)/carbon nanotubes (CNTs) hybrid filled NR nanocomposites are investigated using coarse‐grained molecular dynamics (CGMD) simulations. The non‐bonded coarse‐grained force fields for the CB/CNTs hybrid filled NR nanocomposites are constructed by combining several methods (i.e., effective force coarse‐graining, iterative Boltzmann inversion, and energy matching methods). The uniaxial tensile results indicate that the gradual replacement of CB by the same weight percentage of CNTs significantly improves the mechanical performances of the nanocomposites and increases the heterogeneity of the stress and strain distributions in the nanocomposites, which can be ascribed to the high mechanical strength of CNTs and the formation of the rigid interface networks between CNTs and the NR matrix due to the wrapping behavior of NR molecular chains on the surface of CNTs. Furthermore, the dynamic shear results demonstrate that the introduction of NPs significantly enhances the Payne effect of the nanocomposites, and the higher the CNT loading in hybrid NPs, the stronger the Payne effect. It is also found that the breakup of NP networks plays a dominant role for the Payne effect of filled rubber as compared to the interfacial separation between NPs and the rubber matrix. The present multiscale computational framework can be further extended to other polymer nanocomposites, and sheds new light on the design and exploration of polymer nanocomposites through bottom‐up prediction.