Small Ionic‐Liquid‐Based Molecule Drives Strong Adhesives

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.