Polymer Topology Reinforced Synergistic Interactions among Nanoscale Molecular Clusters for Impact Resistance with Facile Processability and Recoverability

Abstract The intrinsic conflicts between mechanical performances and processability are main challenges to develop cost‐effective impact‐resistant materials from polymers and their composites. Herein, polyhedral oligomeric silsesquioxanes (POSSs) are integrated as side chains to the polymer backbones. The one‐dimension (1D) rigid topology imposes strong space confinements to realize synergistic interactions among POSS units, reinforcing the correlations among polymer chains. The afforded composites demonstrate unprecedented mechanical properties with ultra‐stretchability, high rate‐dependent strength, superior impact‐resistant capacity as well as feasible processability/recoverability. The hierarchical structures of the hybrid polymers enable the co‐existence of multiple dynamic relaxations that are responsible for fast energy dissipation and high mechanical strengths. The effective synergistic correlation strategy paves a new pathway for the design of advanced cluster‐based materials.