Smart Hydrogels with Inhomogeneous Structures Assembled Using Nanoclay-Cross-Linked Hydrogel Subunits as Building Blocks

A novel and facile assembly strategy has been successfully developed to construct smart nanocomposite (NC) hydrogels with inhomogeneous structures using nanoclay-cross-linked stimuli-responsive hydrogel subunits as building blocks via rearranged hydrogen bonding between polymers and clay nanosheets. The assembled thermoresponsive poly(N-isopropylacrylamide-co-acrylamide) (poly(NIPAM-co-AM)) hydrogels with various inhomogeneous structures exhibit excellent mechanical properties due to plenty of new hydrogen bonding interactions created at the interface for locking the NC hydrogel subunits, which are strong enough to tolerate external forces such as high levels of elongations and multicycles of swelling/deswelling operations. The proposed approach is featured with flexibility and designability to build assembled hydrogels with diverse architectures for achieving various responsive deformations, which are highly promising for stimuli-responsive manipulation such as actuation, encapsulation, and cargo transportation. Our assembly strategy creates new opportunities for further developing mechanically strong hydrogel systems with complex architectures that composed of diverse internal structures, multistimuli-responsive properties, and controllable shape deformation behaviors in the soft robots and actuators fields.