Super tough bilayer actuators based on multi-responsive hydrogels crosslinked by functional triblock copolymer micelle macro-crosslinkers

Intelligent hydrogels responsive to external stimuli have been widely studied due to their great potentials for applications in artificial muscles, soft robotics, sensors and actuators. However, the weak mechanical properties, narrow response range, and slow response speed of many responsive hydrogels have hindered practical applications. In this paper, tough multi-responsive hydrogels were synthesized by using vinyl-functionalized triblock copolymer micelles as macro-crosslinkers and N -isopropyl acrylamide (NIPAM) and acrylamide (AAm) or 2-(dimethylamino)ethyl methacrylate (DMAEMA) and 2-acrylamido-2-methyl-1-propane-sulfonic acid (AMPS) as monomers. The P(NIPAM- co -AAm) hydrogels presented tensile strength of up to 1.6 MPa and compressive strength of up to 127 MPa and were tunable by changing their formulations. Moreover, the lower critical solution temperature (LCST) of the thermosensitive hydrogels was manipulated in a wide range by changing the molar ratio of NIPAM to AAm. Responsive hydrogel bilayers were fabricated through a two-step synthesis. A second layer of P(DMAEMA- co -AMPS) was synthesized on the first P(NIPAM- co -AAm) layer to obtain a bilayer hydrogel, which was responsive to temperature, pH and ionic strength changes to undergo fast and reversible shape transformation in a few minutes. This kind of strong and tough multi-responsive hydrogel device has broad prospects in soft actuators. Bilayer hydrogels crosslinked by vinylated Pluronic F127 micelles show independent thermo-, pH-, and salt-responsiveness, and outstanding toughness, which have great potentials for soft robotics, actuators, and artificial muscles.