Nanoarchitectonics composite hydrogels with high toughness, mechanical strength, and self-healing capability for electrical actuators with programmable shape memory properties.

Hydrogel materials show promise in various fields, including flexible electronic devices, biological tissue engineering and wound dressing. Nevertheless, the inadequate mechanical properties, recovery performance, and self-healing speed still constrain the development of intelligent hydrogel materials. To tackle these challenges, we designed a composite hydrogel with high mechanical strength, rapid self-recovery and efficient self-healing ability based on multiple synergistic effects. With the synergistic effect of hydrogen bonds, metal coordination bonds and electrostatic interaction, the synthesized hydrogel could reach a maximum tensile strength of 6.2 MPa and a toughness of 50 MJ m. The interaction between the weak polyelectrolyte polyethyleneimine and polyacrylic acid aided in improving the elasticity of the hydrogel, thereby endowing it with prompt self-recovery attributes. The multiple reversible effects also endowed the hydrogel with excellent self-healing ability, and the fractured hydrogel could achieve 95% self-healing within 4 h at room temperature. By the addition of glycerol, the hydrogel could also cope with a variety of extreme environments in terms of moisture retention (12 h, maintaining 80% of its water content) and freeze protection (-36.8 °C) properties. In addition, the composite hydrogels applied in the field of shape memory possessed programmable and reversible shape transformation properties. The polymer chains were entangled at high temperatures to achieve shape fixation, and shape memory was eliminated at low temperatures, which allowed the hydrogels to be reprogrammed and achieve multiple shape transitions. In addition, we also assemble composite hydrogels as actuators and robotic arms for intelligent applications.