Optimizing the heterogeneous network structure to achieve polymer nanocomposites with excellent mechanical properties

Designing and optimizing the polymer network structure at the molecular level to manipulate its mechanical properties are of great scientific significance. Although heterogeneous multi-network structures have been extensively investigated, little effort has been devoted to investigating heterogeneous single-networks with a well-defined interface. Herein, through coarse-grained molecular dynamics simulation, we successfully fabricated a heterogeneous single-network, which was divided into several regions with different crosslink densities. Firstly, we found that there is an optimal crosslink density ratio between high and low crosslink density regions to obtain the best stress–strain behavior. Secondly, the effect of the regularity of the network topology (by changing the distribution of two-phase regions) on mechanical properties was also studied. It was clearly observed that the polymer network showed better elastic response and mechanical properties as the distribution of two-phase regions became uniform. Finally, we investigated the effect of the selective distribution of nanoparticles (NPs) on mechanical properties by introducing NPs into a pre-designed multiphase network. Results showed that the selective distribution of NPs in the high crosslink density region had a more significant effect on the mechanical reinforcement. Generally, our simulated results may provide some guidelines to design polymer network structures to achieve high-performance polymer nanocomposites with excellent mechanical properties.