Supramolecular Adhesives with Extended Tolerance to Extreme Conditions via Water‐Modulated Noncovalent Interactions

Development of supramolecular adhesives with strong tolerance to extreme conditions has emerged as an important research area. In this study, by balancing supramolecular interactions such as hydrogen bonding interactions, electrostatic interactions, π-π stacking interactions, and cation-π interactions, we designed and prepared a series of two-component supramolecular adhesives derived from small organic molecules. Highly efficient interfacial adhesion with maximum adhesion strength of ≈10.0 MPa was realized on various surfaces in air, organic solvents, or liquid nitrogen. Owing to balanced supramolecular interactions, water participation prolonged and increased the tolerance of the adhesives in extreme environments. We demonstrate that the combination of imidazole-based ionic liquids and phenols can be applied for various interfacial adhesions, thereby aiding the development of next-generation adhesives capable of adapting to various extreme conditions in a controlled manner.