Tailoring the mechanical properties of polymer nanocomposites via interfacial engineering

The improvement of mechanical properties of polymer nanocomposites (PNCs) has been studied for many years, with the main focus on the structure of the nanofillers. Much less effort has been devoted to unraveling the factors controlling the structure of the grafted chains. Herein, through coarse-grained molecular-dynamics simulations, we have successfully fabricated an ideal, mechanically-interlocked composite structure composed of end-functionalized chains grafted to the nanoparticle surface forming rings and making the matrix chains thread through these rings. Depending on the details of the grafting, the reinforcement effect can be remarkable, improving the tensile stress of the system significantly up to 700%. Meanwhile, anisotropy of the system's mechanical response is also observed. Furthermore, the influence of the grafted chain distribution on the mechanical properties of the system has been investigated as well. We observe that the mechanical properties of the system are closely related to the total number of the beads in the grafted chains or the synergistic effect between the length and density of the grafted chains leads to no significant difference in the performance of systems. At constant grafting density, the mechanical properties of the systems correlate negatively to the grafted chain length. In general, our study should help to design and fabricate high-performance PNCs with excellent mechanical properties.