Role of Dynamic Crosslinks on the Phase Behaviour and Stability of Polymer Nanocomposites

Polymer nanocomposites are well-known for their tunable mechanical, electrical, and rheological properties which are attributed to their rich phase behaviours. However, the phase change during critical operations reduces their efficiency in a given application. Here we study how dynamic crosslinking of polymers can enhance the stability of phases in a nanocomposite. We perform large-scale coarse-grained molecular dynamics (MD) – Monte Carlo (MC) hybrid simulations of a phenomenological model nanorod-polymer system. Our simulations suggest the formation of a percolating network-like distribution of nanorods with the increment of their concentration for a given nanorod-polymer size ratio. The crosslink is found to retain the network structure during multiple thermal treatment cycles. We establish correlations between nanorod concentration, crosslink concentration, and the stability of phases. The work provides important design rules for highly stable and re-processable polymer nanocomposites.