Boosting Energy Dissipation and Degradation Behaviors: Cation‐π Interactions as a Key to Stimuli Responsive Epoxy Adhesives

Abstract Epoxy resins, widely recognized for their stable cross‐linked structures and extensive use as adhesives, face a fundamental challenge in balancing high‐performance attributes with dynamic functionalities. To address this, a novel strategy leveraging synergistic effects is proposed to amplify dynamic bonds within the resin network. Specifically, an ionic monomer featuring imidazole cations and benzene rings is synthesized and combined with four‐arm thiol‐containing ester groups, forming a synergistic cross‐linked network through a dual curing process. This design endows the thermoset with multiple stimuli‐responsive functionalities. The ester groups are pivotal in enabling the resin's degradability and reprocessability, while the non‐covalent cation‐π interactions significantly enhance energy dissipation, resulting in superior mechanical properties. Notably, the imidazole cations not only lower the energy barrier of the epoxy thermal curing reaction but also accelerate the hydrolysis of ester groups via hydrogen bonding. This work demonstrates a tunable and responsive adhesive with cyclic features, offering a promising candidate for functional applications in energy devices and beyond. The innovative integration of dynamic bonds and synergistic effects provides a versatile platform for designing next‐generation epoxy resins with both high performance and full life‐cycle sustainability.