Hydrogen Bond-Regulated Rapid Prototyping and Performance Optimization of Polyvinyl Alcohol–Tannic Acid Hydrogels

Traditional hydrogel preparation methods typically require multiple steps and certain external stimuli. In this study, rapid and stable gelation of polyvinyl alcohol (PVA)-tannic acid (TA)-based hydrogels was achieved through the regulation of hydrogen bonds. The cross-linking between PVA and TA is triggered by the evaporation of ethanol. Rheological testing and analysis of the liquid-solid transformation process of the hydrogel were performed. The gelation onset time (GOT) could be tuned from 10 s to over 100 s by adjusting the ethanol content and temperature. The addition of polyhydroxyl components (e.g., glycerol) significantly enhances the hydrogel's water retention capacity (by 858%) and tensile strain rate (by 723%), while concurrently increasing the gelation time. Further studies have shown that the addition of alkaline substances (such as sodium hydroxide) promotes the entanglement of PVA molecular chains, increasing the tensile strength by 23% and the fracture strain by 41.8%. The experimental results indicate that the optimized PVA-TA hydrogels exhibit a high tensile strength (>2 MPa) and excellent tensile properties (~600%). Moreover, the addition of an excess of weakly alkaline substances (such as sodium acetate) reduces the degree of hydrolysis of PVA, enabling the system to form a hydrogel with extrudable characteristics before the ethanol has completely evaporated. This property allows for patterned printing and thus demonstrates the potential of the hydrogel in 3D printing. Overall, this study provides new insights for the application of PVA-TA based hydrogels in the fields of rapid prototyping and strength optimization.