ACS Applied Materials & Interfaces, 2018, vol 10, 3, pp. 2946-2956
Hydrophobically associated hydrogels (HA gels) are one of most extensively investigated high strength hydrogels. Semicrystalline HA gels, prepared by micellar copolymerization, show high strength and notable functionalities of self-healing and shape-memory. However, the hydrophobic comonomers in these semicrystalline HA gels are usually limited to the long alkyl length monomers (18-alkyl(meth)acrylates). In the present work, N-acryloyl 11-aminoundecanoic acid (A11AUA), consisting of 10 −CH2 groups and a −COOH group at the end of alkyl chain, was used as hydrophobic comonomer to prepare physical A11AUA-based HA gels in the presence of high concentration cetyltrimethylammonium bromide (CTAB) or sodium dodecyl sulfate. Differential scanning calorimetry, wide-angle X-ray scattering, and small-angle X-ray scattering experiments had identified that the A11AUA-based HA gels possessed crystalline domains and clusters of crystalline domains, while lauryl methacrylate (C12M)-based HA gels were amorphous. As a result, A11AUA-based HA gels displayed much better tensile properties than those of C12M-based HA gels. At the optimal condition, the A11AUA-CTAB HA gel demonstrated integrated high performances, including high stiffness (E of 1016 kPa), high strength (σf of 0.75 MPa), high toughness (T of 7540 J/m2), rapid self-recovery (94% recovery after heat treatment at 60 °C for 2 min), outstanding shape memory (fully recovered to the permanent shape only 2–14 s), and excellent self-healing properties (as healed at 60 °C for 2 h; stress and strain healing efficiency reached to 64% and 85%, respectively). We believe this work provides a new insight for HA gels, which is beneficial to design new hydrogels with integrated high performances, such as high strength, high toughness, large extensibility, and shape-memory and self-healing properties.