LAUSR

Thermo-responsive hydrogel actuators have attracted tremendous interest due to their promising applications in artificial muscles, soft robotics, and flexible electronics. However, most of these materials are based on polymers with lower critical solution temperature (LCST), while those from upper critical solution temperature (UCST) are rare. Herein, we report a multiple-responsive UCST hydrogel actuator based on the complex of poly(acrylic acid) (PAAc) and poly(acrylamide) (PAAm). By applying a heterogeneous photo-polymerization, a bilayer hydrogel was obtained, including a layer of interpenetrating network (IPN) of PAAm/PAAc and a layer of single network of PAAm. When cooled down below the UCST, the PAAm/PAAc layer contracted due to the hydrogen bonding of the two polymers while the PAAm layer stays in swelling state, driving the hydrogel to curl. By adjusting the composition of the two layers, the amplitude of actuation behavior could be regulated. By creating patterned IPN domains with photo-masks, the hydrogel could deform into complex 2D and 3D shapes. Active motion was realized in both water and oil bath, thanks to the internal water exchange between the two layers. Interestingly, the hydrogel actuator is also responsive to urea and salts (Na2SO4, NaCl, NaSCN), due to that the strength of the hydrogen bonds in the IPN changes with the additives. Overall, the current study realized an anisotropic UCST transition through introducing asymmetrically distributed polymer-polymer hydrogen-bonds, which would inspire new inventions of intelligent materials.