Synthesis of a gallic acid-based self-healing waterborne polyurethane with a thermo-responsive dynamic phenol-carbamate network for enhanced mechanical strength, antimicrobial activity, and shape memory properties

To expedite the advancement of multifunctional next-generation smart materials, it is imperative to create polymers derived from renewable, green bio-based resources. This paper presents a direct synthesis of thermoresponsive aqueous polyurethanes by combining gallic acid (GA) with isocyanate groups to form a dynamic phenol-carbamate crosslinked network and the incorporation of the metal-organic framework Cu-MOF-2 for synergistic effects. The resulting GA-based polyurethane (MOF-GWPU) exhibits excellent thermal stability and mechanical properties, achieving an ideal balance between mechanical strength and self-healing efficiency. The MOF-GWPU film demonstrates strong antimicrobial efficacy against Escherichia coli and Staphylococcus aureus, highlighting its exceptional antibacterial performance. The thermo-responsive dynamic covalent bonds enable the MOF-GWPU film to rapidly revert from a temporary shape back to its original form. Post-processing experiments further indicate that the crosslinked GA-PU polymer can be efficiently recycled through solution casting and hot-pressing techniques. This design offers a novel approach and valuable insights for advancing the development of multifunctional smart polymers derived from bio-based resources.