Self-recoverable semi-crystalline hydrogels with thermomechanics and shape memory performance

Stimuli-responsive hydrogels have become one of the most popular artificial soft materials due to their excellent adaption to complex environments. Thermoresponsive hydrogels triggered by temperature change can be efficiently utilized in many applications. However, these thermoresponsive hydrogels mostly cannot recover their mechanical states under large strain during the process. Herein, we utilize the heterogeneous comb-type polymer network with semicrystalline hydrophobic side chains to design self-recovery semi-crystalline hydrogels. Based on hydrophilic/hydrophobic cooperative complementary interaction and heterogeneous polymer network, hydrogels can be endowed with excellent thermosensitive properties and mechanical performance. The hydrogels exhibit high compressive strength (7.57 MPa) and compressive modulus (1.76 MPa) due to the semi-crystalline domains formed by association of the hydrophobic poly (epsilon-caprolactone) PCL. The melting-crystalline transition of PCL and elastic polymer network provide the hydrogels excellent thermomechanical performance and self-recovery property. Furthermore, the hydrogels exhibit shape memory behavior, which can be realized by simple process and smart surface patterning. With these excellent properties, our hydrogels can be applied in sensors, flexible devices and scaffolds for tissue engineering.