Complexation of Sulfonate-Containing Polyurethane and Polyacrylic Acid Enables Fabrication of Self-Healing Hydrogel Membranes with High Mechanical Strength and Excellent Elasticity

Artificial hydrogel membranes with good biocompatibility are strongly needed in biological fields. The preparation of biocompatible hydrogel membranes simultaneously possessing high mechanical strength, excellent elasticity, and satisfactory self-healing properties remains a challenge. Herein, we demonstrate the preparation of such hydrogel membranes by complexation of sulfonate-containing polyurethane (SPU) and poly(acrylic acid) (PAA) in the presence of Zn²⁺ ions followed by swelling in water (denoted as SPU-PAA/Zn). Originating from the synergy of the coordination and hydrogen-bonding interactions and the reinforcement effect of the in situ formed hydrophobic domains, the SPU-PAA/Zn hydrogel membrane exhibits a high tensile strength of ∼7.1 MPa and a toughness of ∼30.4 MJ m^-3. Moreover, the hydrogel membrane is highly elastic, which can restore to its initial state from an ∼500% strain within 40 min rest at room temperature without any external assistance. The dynamic noncovalent interactions and hydrophobic domains allow the fractured hydrogel membrane to heal and completely regain its original integrity and mechanical properties at room temperature. Both in vitro and in vivo tests confirm that the hydrogel membrane exhibits satisfactory biocompatibility and could be potentially used as a biological barrier membrane in surgical operations or artificial organs.