Tunable mechanical properties and phase transitions in nanoconfined polyzwitterionic UCST hydrogels

Stimuli-responsive hydrogels with thermal phase transitions serve as pivotal components in advancing biomedical and soft robotics applications. In contrast to widely studied LCST-type thermo-responsive hydrogels, UCST-type hydrogels provide reverse thermo-responses. However, conventional UCST-type hydrogels suffer from weak mechanical properties and fixed phase transition kinetics. Here, we present polyzwitterionic UCST-type hydrogels under coplanar nanoconfinement by large aspect ratio hectorite nanosheets. The nanoconfinement significantly enhances the strength and stiffness of the hydrogels. In addition, the nanosheets serve as kinetic barriers for water diffusion. This regulates the swelling and shrinking kinetics of the polyzwitterionic hydrogels and thus allows for tunable phase transitions dependent on the thermal history of the hydrogels. Furthermore, we demonstrate that the incorporation of gold nanoparticles allows precise control of the optical properties of the hydrogel through photothermal means. These findings pave the way for engineering both the mechanical and thermoresponsive properties in polyzwitterionic hydrogels, thus broadening their applications in smart soft materials.