Bilayer
hydrogel actuators are of great interest in mechanical
valves, soft robots, and bionic devices benefiting from their flexibility
and adaptability to actuate in different environments. They respond
rapidly to external stimuli through differential deformation of the
internal structure to achieve the actuation effect. However, the bilayer
hydrogel is prone to delamination due to the low interfacial toughness
of the two gel layers, thus they exhibit poor actuating performances.
In this work, a synchronous ultraviolet (UV) polymerization strategy
was proposed to enhance the interfacial toughness of bilayer hydrogel
actuators. Based on the synchronous UV polymerization strategy, a
gelatin/poly(N-hydroxyethyl acrylamide)–poly(N-isopropyl acrylamide-co-N-hydroxyethyl acrylamide) [gelatin/PHEAA–P(NIPAM-co-HEAA)] bilayer hydrogel actuator with gelatin/PHEAA functional layer
and P(NIPAM-co-HEAA) actuating layer was prepared.
The obtained bilayer hydrogel showed a maximum interfacial toughness
of 508.11 ± 45.62 J/m2, which was attributed to the
covalent bonding and topological entanglement of polymer chains at
the gel–gel interface induced by the permeation–polymerization
step. In addition, the copolymerization of NIPAM with the hydrophilic
monomer N-hydroxyethyl acrylamide (HEAA) increased
the lower critical solution temperature of the bilayer hydrogel actuator,
which allowed the actuator to exhibit stable actuating ability at
90 °C and to be used as a bionic gripper for high-temperature
pickup. Overall, a synchronous UV polymerization strategy was presented.
It simplified the fabrication of bilayer hydrogel actuators and enhanced
the interaction between bilayer hydrogels by forming strong covalent
bonding and local topological entanglement structure at the hydrogel
interface, which provided a new idea for preparing bilayer hydrogel
actuators with high interfacial toughness.