Transparent, High‐Strength, and Shape Memory Hydrogels from Thermo‐Responsive Amino Acid–Derived Vinyl Polymer Networks

Abstract Herein, the formation of unique shape‐memory hydrogels that are composed of thermo‐responsive amino‐acid‐derived vinyl polymer networks is reported; these are readily prepared by radical copolymerization of N ‐acryloyl glycinamide with commercially available cross‐linkers, namely, methylenebis(acrylamide) and poly(ethylene glycol) diacrylate. These hydrogels are transparent (>90% transmittance at 600 nm) and are comprised of 97–70 wt% water. Furthermore, these contain both chemical and physical cross‐linkages that are based on the multiple hydrogen bonds attained via amino acid units; this composition is aimed at generating opposing stimuli‐responsive characters, namely, chemically stable and thermo‐sensitive properties. A cooperative interplay of these two networks enables the hydrogels to exhibit a decent mechanical toughness (breaking strength ≈0.3 MPa and breaking elongation >600%) and a shape fix/memory capability. The temporary shape is easily fixed by cooling at 4 °C after deformation at high temperature, and it instantly recovers its original shape through reheating. Furthermore, a multi‐shape memory effect is achieved by incorporating the pH‐responsive N ‐acryloyl alanine unit into the hydrogel system as a comonomer; in this system, three distinct shapes can be fixed through temperature and pH manipulations. This facilely attainable shape memory hydrogel has significant potential in various fields, such as soft actuators, sensors, and biomedical materials.