Dual Cross-Linked Polymethacrylic Acid Hydrogels with Tunable Mechanical Properties and Shape Memory Behavior

Abstract

Herein, a series of poly(methacrylic acid) hydrogels are prepared via bulk polymerization of methacrylic acid (MAAc) and grafting of Triton X-100 (TX-100). One-pot and extremely simple chemistry consist of only mixing and subsequently heating of commercially available monomer and surfactant. The polymer chains are interconnected through dual physical cross-link points formed by the hydrophobic associations in the center of TX-100 micelles and hydrogen bonds stabilized by hydrophobic alpha-methyl groups of MAAc. The hydrogels exhibit tunable mechanical properties ranging between softness and stiffness by adjusting the surfactant/monomer molar ratio, such as Young modulus of 0.6-22 MPa, elongation at break of 750-1700%, tensile strength of 0.21-3.6 MPa, and compressive strength of 41-93 MPa. The synergistic effect of high-density hydrogen bonds with hydrophobic associations endows a plastic-like hydrogel with high strength and shape memory (SM) behavior, while a high concentration of micelles with low-density hydrogen bonds endows a stretchable elastic hydrogel. The combination of temperature-induced SM property and wide-ranging mechanical performance will make such hydrogels useful in diverse applications.