High-Performance Branched Polymer Elastomer Based on a Topological Network Structure and Dynamic Bonding

High performance has always been the research focus of elastomers. However, there are inherent conflicts among properties of elastomers, such as strength and toughness, strength and damping performance, strength and self-healing ability, etc. Herein, first, we synthesized a unique structure of the dangling chain containing proton donors and receptors. Then, we design and fabricate a kind of high-performance elastomer with a gradient distribution of a dangling chain and a dynamic bond structure. The dangling chains of different lengths intertwine with each other and self-assemble to form a “dense accumulation” structure driven by hydrogen bonds, and the elastomer exhibits special micro/nano scale aggregated states and microphase separation. The “dense accumulation” structure plays a vital role in the increase of mechanical properties. Meanwhile, under the joint action of a dangling chain and a dynamic bond, the damping performance and self-healing performance of the elastomer are greatly enhanced. High strength (27.5 MPa), toughness (121.9 MJ·m^–3), 94.8% healing efficiency and outstanding damping performance (tan δ ≥ 0.4, high damping temperature range up to 144 °C) are simultaneously achieved beyond the current state-of-the-art. This topoarchitected polymer with a gradient distribution of dangling chains successfully solves the defects of conventional branched polymers in deteriorating their mechanical properties. This material design provides a new strategy for the development of high-performance structural and functional integrated elastomers.