Architectured Shape-Memory Hydrogels with Switching Segments Based on Oligo(Epsilon-caprolactone)


Shape-memory hydrogels (SMHs) are potential candidate materials for biomedical applications as they can mimic the elastic properties of soft tissue and exhibit shape transformations at body temperature. Here we explored, whether architectured SMHs can be designed by incorporating oligo(ε-caprolactone) (OCL, = 4500 g·mol-1, T m = 54 °C) side chains as switching segment into hydrophilic polymer networks based on N-vinylpyrrolidone as backbone forming component and oligo(ethylene glycol)divinylether (OEGDVE, = 250 g·mol-1) as crosslinker. By utilizing NaCl and NaHCO3 as porogene during thermal crosslinking architectured hydrogels having pore diameters between 30 and 500 µm and wall thicknesses ranging from 10 to 190 µm in the swollen state were synthesized. According to the porous microstructure, a macroscopic form stability was obtained when the polymer networks were swollen until equilibrium in water. Material properties were investigated as function of the OCL content, which was varied between 20 and 40 wt%. In compression experiments the architectured hydrogels exhibited strain fixity and strain recovery ratios above 80%. These architectured SMHs might enable biomaterial applications as smart implants with the recovery of bulky structures from compact shapes.
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