The role of interface on the toughening and failure mechanisms of thermoplastic nanocomposites reinforced with nanofibrillated rubber

The interface plays a crucial role in the physical and functional properties of polymer nanocomposites, yet its effects have not been fully recognized in the setting of classical continuum-based modeling. In the present study, we investigate the roles of interface and interfiber interactions on the toughening effects of rubber nanofibers embodied in thermoplastic-based materials. Emphasis is placed on establishing comprehensive theoretical and atomistic descriptions of the nanocomposite systems subjected to pull-out and uniaxial extension in the longitudinal and transverse directions. Using the framework of molecular dynamics, the annealed melt-drawn nanofibers were spontaneously formed via the proposed four-step methodology. The generated nanofibers were then crosslinked using the proposed robust topology-matching algorithm, through which the chemical reactions arising in the crosslinking were closely assimilated. The interfiber interactions were also examined with respect to separation distances and nanofiber radius via a nanofiber-pair atomistic scheme, and the obtained results were subsequently incorporated into the pull-out and uniaxial test simulations. The results indicate that the compatibilizer grafting results in enhanced interfacial shear strength by introducing extra chemical interactions at the interface. In particular, it was found that the compatibilizer restricts the formation and coalescence of nanovoids, resulting in enhanced toughening effects. Together, we have shown that the presence of a small amount of well-dispersed rubber nanofibrillar network whose surfaces are grafted with maleic anhydride compatibilizer can dramatically increase the toughness and alter the failure mechanisms of the nanocomposites without any deterioration in the stiffness, which is also consistent with the recent experimental observations in our lab. The interfacial failure mechanism was also investigated by monitoring the changes in the atomic concentration profiles, mean square displacement and fractional free volume. The results obtained may serve as a promising alternative for the continuum-based modeling and analysis of interfaces. The interface plays a crucial role in the physical and functional properties of polymer nanocomposites, yet its effects have not been fully recognized in the setting of classical continuum-based modeling.