It has been a challenge to achieve strong adhesion strength for gel adhesives in water. In this study, a novel eutectogel adhesive is synthesized via one-step photoinitiated polymerization of N-vinylpyrrolidone (NVP) in deep eutectic solvent (DES). The abundant hydrogen bonding interactions and the hydrophilic polyvinylpyrrolidone network structure endow the eutectogel with excellent adhesion to both hydrophilic and hydrophobic surfaces in air and underwater. Moreover, for hydrophilic substrates, the underwater adhesion strength of the eutectogel adhesives is 1.3 times larger than that in air, demonstrating an underwater-enhanced adhesion effect. In contrast, for hydrophobic substrates, the underwater adhesion strength is lower than in air. Furthermore, strong adhesion performance is maintained even in boiling water, strong acidic medium, strong basic medium, and organic solvents. The experimental and simulation results have unveiled the underwater adhesion enhancement mechanism of the eutectogel. It is believed that the designed eutectogel will show great promise in the development of the next-generation of gel adhesives with underwater adhesion capabilities and high environmental adaptability.
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