The Preparation of Electrolyte Hydrogels with the Water Solubilization of Polybenzoxazine

Polybenzoxazine (PBZ) exhibits excellent heat resistance, and PBZ derivatives have been designed and synthesized to achieve high performance. However, the application range of PBZ is limited by the strong interactions between molecular chains and its low solubility in organic solvents, thereby limiting its processability. This study focused on the benzoxazine structure as the molecular backbone of new hydrogel materials that can be applied as electrolyte materials and prepared functional gel materials. Here, we prepared hydrogels by water-solubilizing PBZ derivatives, which typically exhibit low solubility in organic solvents. Although studies on the hydrophilization of PBZ and its complexation with hydrophilic polymers have been conducted, no studies have been performed on the hydrogelation of PBZ. First, the phenol in the organic solvent-insoluble PBZ thin film obtained after the thermal ring-opening polymerization of the monomer was transformed into sodium phenoxide by immersion in a NaOH aqueous solution to water-solubilize it and obtain a hydrogel thin film. Although the hydrogel thin film exhibited low mechanical strength, a free-standing hydrogel film with improved strength was obtained through the double network gelation method with an acrylamide monomer system. The physical properties of the polymer composite hydrogel thin film were evaluated. The ionic conductivity of the hydrogel thin films was in the order of 10^-4 S cm^-1, indicating the potential of PBZ as an electrolyte hydrogel material. However, improving its ionic conductivity will be undertaken in future studies.