Low surface energy materials resist adhesion due to their chemical inertness and non-wetting properties. Herein, we report the creation of a transparent ionogel adhesive that uses ion−dipole interactions to achieve a higher bonding performance to polytetrafluoroethylene (PTFE) relative to most commercial glues. The ionogel adhesive is composed of a poly(hexafluorobutyl acrylate-co-methyl methacrylate) random copolymer and a hydrophobic ionic liquid. The prepared ionogel can adhere to various hydrophobic substrates, such as PTFE, polypropylene, and polyethylene, as well as hydrophilic glass, ceramics, and steel. The design strategy and adhesion behavior are well interpreted using the density functional theory calculations and molecular dynamics simulations. The straightforward ultravioletcuring method, high optical clarity, versatile adhesion ability, and reversible adhesion capabilities make this high-performance adhesive a promising product for commercialization.

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Poly­(ionic liquid)­s (PILs), combining the advantages of both polymers and ionic liquids, have attracted significant attention from the academia and industry. This study has developed a fluorinated PIL copolymer-based adhesive with versatile adhesion ability and high transparency. The adhesive was prepared by in situ UV-curing a precursor solution composed of commercially available monomers, that is, 2,2,3,4,4,4-hexafluorobutyl methacrylate and 1-vinyl-3-butylimidazolium bis­(trifluoromethylsulfonyl)­imide. The prepared adhesive showed a superior adhesion strength of 6.61 MPa toward glass substrates. Furthermore, minimal addition of a plasticizer in the bulk adhesive could significantly enhance the adhesion performance on fluorinated polymer substrates while maintaining the polar surface bonding strength and high transparency. The resulting PIL-based adhesive showed a strong adhesion on various adherends, such as glass, steel, ceramics, and low surface energy polymers. This work provides a methodology for using PILs as adhesives and is believed to have good potential for commercialization.

Adhesive materials have been widely used in almost every industrial domain. The art of the design principles of high‐performance adhesives lies in the regulation of adhesion and cohesion strengths. Compared with permanent covalent bonds, dynamic bonds, including dynamic covalent and noncovalent bonds, are vulnerable under mechanical stimuli but rebuildable, making them promising candidates to manipulate the internal and interfacial energy. In this review, we mainly discuss how dynamic bonds can be applied to adhesive materials to regulate adhesion and cohesion, simultaneously. Representative samples are rationally selected to elaborate on the engineering designs for improving the adhesive performance via incorporating dynamic bonds. We also offer a perspective on future research directions on the engineered construction of advanced adhesive materials.