Dynamic Recyclable High-Performance Epoxy Resins via Triazolinedione-Indole Click Reaction and Cation-π Interaction Synergistic Crosslinking.

Thermosetting plastics exhibit remarkable mechanical properties and high corrosion resistance, yet the permanent covalent crosslinked network renders these materials challenging for reshaping and recycling. In this study, a high-performance polymer film (EI-TAD-Mg) was synthesized by combining click chemistry and cation-π interactions. The internal network of the material was selectively constructed through flexible triazolinedione (TAD) and indole via a click reaction. Cation-π interactions were established between Mg and electron-rich indole units, leading to network contraction and reinforcement. Dynamic non-covalent interactions improved the covalent crosslinked network, and the reversible dissociation of cation-π interactions during loading provided effective energy dissipation. Finally, the epoxy resin exhibited excellent mechanical properties (tensile strength of 91.2 MPa) and latent dynamic behavior. Additionally, the thermal reversibility of the C-N click reaction and dynamic cation-π interaction endowed the material with processability and recyclability. This strategy holds potential value in the field of modifying covalent thermosetting materials.