Viscoelasticity of Nanosheet-Filled Polymer Composites: Three Regimes in the Enhancement of Moduli

We employed nonequilibrium molecular dynamics simulations to elucidate the viscoelastic properties of nanosheet (NS)-filled polymer composites. The effects of NS loadings and NS-polymer interaction on viscoelasticity were examined. The simulation results show that the NS-filled polymer composites exhibit an enhanced storage modulus and loss modulus as the NSs are loaded. There are three regimes of the enhanced process based on the NS loadings. At lower NS loadings, the motion of polymers slows down owing to the interaction between NSs and polymers, and the polymer chains generally follow the Rouse dynamics. As the NS loadings increase, the polymer chains are confined between NSs, leading to a substantial increment in dynamic moduli. At higher NS loadings, a transient network is formed, which strengthens the dynamic moduli further. In addition, the attractive NS-polymer interaction can improve the dispersion of NSs and increase the storage and loss moduli. The present work could provide essential information for designing high-performance hybrid polymeric materials.