Small Ionic Liquid‐based Molecule Drives Strong Adhesives

Abstract Nature has inspired scientists to fabricate adhesive materials for applications in many burgeoning areas. However, it is still a significant challenge to develop small‐molecule adhesives with high‐strength, low‐temperature and recyclable properties, although these merits are of great interest in various aspects. Herein, we report a series of strong adhesives based on low‐molecular‐weight molecular solids driven by the terminal modification of ionic liquids (ILs) and subsequent supramolecular self‐assembly. The emergence of high strength and liquid‐to‐solid transitions for these supramolecular aggregates relies on modifying IL with a high melting point motif and enriching the types of noncovalent interactions in the original ILs. Using this strategy, we demonstrate that our IL‐based molecular solids can efficiently obtain a high adhesion strength (up to 8.95 MPa). Importantly, we elucidate the mechanism underlying the reversible and strong adhesion enabled by monomer‐to‐polymer transitions. These fundamental findings provide guidance for the design of high‐performance supramolecular adhesive materials.