Hydrophobically Associating Hydrogels with Microphase-Separated Morphologies

Hydrophobically associating hydrogels based on copolymers of a water-soluble monomer with a fluoroacrylate or fluoromethacrylate possess microphase-separated morphologies that provide unique properties. Physical crosslinks in these hydrogels involve hydrophobic bonds between fluoro(meth)acrylate groups that associate into 2–6-nm-diameter core–shell nanodomains that represent multifunctional crosslinks. These hydrogels exhibit exceptional mechanical properties and fracture toughness values approaching 104 J/m2, are extrudable, and show self-healing behavior of the microstructure. This chapter reviews the characteristics of these microphase-separated, hydrophobically associating hydrogels and discusses potential applications of these materials as injectable in situ forming hydrogels, electrospun fiber mats suitable for tissue scaffolds, controlled drug release, antifreeze materials, and shape memory hydrogels.