Enhancement of Mechanical Properties of Benign Polyvinyl Alcohol/Agar Hydrogel by Crosslinking Tannic Acid and Applying Multiple Freeze/Thaw Cycles

Hydrogels composed of natural and synthetic polymers have considerable potential for use in diverse areas such as biomedical applications and water purification. This is primarily because of their biocompatibility, biodegradability, and low toxicity. The widespread usage of composite hydrogels is hindered by a lack of simultaneous properties, such as high strength and low swelling rate. Herein, we report the preparation of novel hydrogels composed of polyvinyl alcohol (PVA)–intercalated agar polymer networks physically crosslinked with tannic acid. The hydrogel was subjected to multiple freeze/thaw (F/T) cycles (1, 3, and 5), and it was found to exhibit the highest strength after 5 F/T cycles. After 1 F/T cycle, the tensile strength of the composite hydrogel reached 1.56 MPa with a 1.0 wt% crosslinker, whereas after 5 F/T cycles, it increased to 3.77 MPa with a reduced amount (0.75 wt%) of the crosslinker. In addition, the swelling ability decreased upon increasing the crosslinker content and number of F/T cycles. Furthermore, the hydrogel demonstrated excellent water retention and a strong ability to adhere to different substrates. We have successfully implemented an innovative approach to improve the mechanical properties of PVA-based hydrogels by combining the use of tannic acid as a cross-linking agent and multiple F/T cycles. The developed hydrogels are expected to facilitate new developments in hydrogel technology, thus impacting diverse fields such as biomedical (wound dressing and artificial cartilage).