Concentration-induced spontaneous polymerization of protic ionic liquids for efficient in situ adhesion

Abstract The advancement of contemporary adhesives is often limited by the balancing act between cohesion and interfacial adhesion strength. This study explores an approach to overcome this trade-off by utilizing the spontaneous polymerization of a protic ionic liquid-based monomer obtained through the neutralization of 2-acrylamide-2-methyl propane sulfonic acid and hydroxylamine. The initiator-free polymerization process is carried out through a gradual increase in monomer concentration in aqueous solutions caused by solvent evaporation upon heating, which results in the in-situ formation of a tough and thin adhesive layer with a highly entangled polymeric network and an intimate interface contact between the adhesive and substrate. The abundance of internal and external non-covalent interactions also contributes to both cohesion and interfacial adhesion. Consequently, the produced protic poly(ionic liquid)s exhibit considerable adhesion strength on a variety of substrates. This method also allows for the creation of advanced adhesive composites with electrical conductivity or visualized sensing functionality by incorporating commercially available fillers into the ionic liquid adhesive. This study provides a strategy for creating high-performance ionic liquid-based adhesives and highlights the importance of in-situ polymerization for constructing adhesive composites.