Ultra-Strong and Highly-Robust Elastomers with Synergistic Multiple Weak Interactions

The increasing demand for high-performance elastomers has spurred research aimed at enhancing comprehensive properties. However, challenges such as complex molecular structures and poor understanding of structure-property relationship have hindered the development of advanced elastomers. To address these limitations, we propose a strategy that strengthens the intermolecular interactions via synergistic multiple weak interactions and leverages theoretical calculations. Adoption of symmetric hard segments effectively organizes π-π stacking, which have a positioning effect and lead to an increase in the spontaneous formation efficiency of multiple hydrogen bonds, resulting in ordered hard domains. Thereby, polyurethane elastomers with exceptional properties were successfully developed by using simple and efficient processes, achieving tensile strength of 104.7 MPa and toughness of 460.5 MJ/m³, which surpass substantial numbers of existing materials. These also exhibit superior resilience, thermal, and chemical resistance, as well as anti-relaxation behavior, making them ideal for extreme conditions. Additionally, we employed rigorous ab initio calculations to analyze the structure of specific segments, which convincingly demonstrate the immense impact of even slight changes of molecular structure and segment arrangement on material performance and provide excellent predictive power for material properties. Consequently, this work establishes a novel framework with vast potential for advancing innovation in high-performance materials.