Mechanically Robust Supramolecular Plastics through Distinct Ionic Association Modes

Abstract Sustainable plastics require green-by-design, low-toxicity, and recyclable materials without sacrificing mechanical robustness. Here, we report a family of supramolecular plastics with distinct ionic association modes and investigate the relationships between these modes, supramolecular network architecture, and mechanical properties. The resulting supramolecular plastics exhibit varied mechanical performance, including high tensile strength and cyclic durability. The materials further exhibit tunable thermal stability and humidity-responsive sensing while allowing facile aqueous processing and recycling. This work highlights ionic association mode as a structural parameter for exploring supramolecular network organization and designing mechanically robust supramolecular plastics that combine integrated functionalities with recyclability.