Flexible Cages Enable Robust Supramolecular Elastomers.

Advances in modern industrial technology continue to place stricter demands on engineering polymeric materials, but simultaneously possessing superior strength and toughness remains a daunting challenge. Herein, we report a pioneering flexible cage-reinforced supramolecular elastomer (CSE) that exhibits superb robustness, tear resistance, anti-fatigue, and shape memory properties, achieved by innovatively introducing organic imide cages (OICs) into supramolecular networks. Intriguingly, extremely small amounts of OICs make the elastomer stronger, significantly improving mechanical strength (85.0 MPa; ∼10-fold increase) and toughness (418.4 MJ m -3 ; ∼7-fold increase). Significantly, we experimentally and theoretically demonstrate the cooperative effect of gradient hydrogen bonds and OICs as flexible nodes, enabling more robust supramolecular networks. In short, our proposed strengthening strategy of adding flexible cages effectively balances the inherent conflict between material strength and toughness, and the prepared CSEs are anticipated to be served in large-scale devices such as TBMs in the future. This article is protected by copyright. All rights reserved.