Dynamic Hydrogels with an Environmental Adaptive Self-Healing Ability and Dual Responsive Sol–Gel Transitions

Dynamic polymer hydrogels with an environmental adaptive self-healing ability and dual responsive sol-gel transitions were prepared by combining acylhydrazone and disulfide bonds together in the same system. The hydrogel can automatically repair damage to it under both acidic (pH 3 and 6) and basic (pH 9) conditions through acylhydrazone exchange or disulfide exchange reactions. However, the hydrogel is not self-healable at pH 7 because both bonds are kinetically locked, whereas the hydrogel gains self-healing ability by accelerating acylhydrazone exchange with the help of catalytic aniline. All of the self-healing processes are demonstrated to be effective without an external stimulus at room temperature in air. The hydrogel also displays unique reversible sol-gel transitions in response to both pH (HCl/triethylamine) and redox (DTT/H₂O₂) triggers.