Multiple Hydrogen Bonds–Reinforced Hydrogels with High Strength, Shape Memory, and Adsorption Anti‐Inflammatory Molecules

The research on multiple hydrogen bonds (H‐bonds) hydrogels have gradually aroused wide interest. In this paper, a multiple H‐bonds‐reinforced poly(acrylamide‐co‐2‐vinyl‐4,6‐diamino‐2‐vinyl‐1,3,5‐triazine)/tannic acid (P(Am‐co‐VDT)/TA) hydrogels are prepared. The results suggest that the prepared hydrogel has two types of H‐bonds crosslinking regions: A “soft” region of H‐bonds between the diaminotriazine (DAT) moieties on the polymer chains and the TA pyrogallol/catechol groups, and a “hard” region of H‐bonds forming by DAT moieties with itself. The hard crosslinking region exhibits significantly higher activation energy than the soft region. Such soft and hard dual physically crosslinked networks dramatically enhance the mechanical properties of P(Am‐co‐VDT)/TA hydrogels in a synergistic manner (tensile strength is 2.34 MPa, elongation at break is 410%). Due to the multiple hydrogen bonds, the hydrogel has good pH sensitivity and rapid response to shape memory within a few minutes. In addition, the hydrogels have the capacity of physical adsorption of the anti‐inflammatory drug diclofenac sodium and other molecules with a specific spatially arranged chemical composition. These hydrogels with high mechanical strength, excellent shape memory behavior, and capacity of adsorption of anti‐inflammatory drug could be attractive candidates for applications in the fields of biomedicine, tissue engineering, and medical materials. Diaminotriazine (DAT) moieties in the poly(acrylamide‐co‐2‐vinyl‐4,6‐diamino‐2‐vinyl‐1,3,5‐triazine)/tannic acid (P(Am‐co‐VDT)/TA) hydrogels create the “hard” region of H‐bonds and hence improve the hydrogels’ mechanical properties due to its synergetic interaction with the “soft” region of amide‐TA and DAT‐TA H‐bonds. The hydrogel exhibits fast response to shape memory and the ability to carry the anti‐inflammatory drug (diclofenac sodium) for biomedical treatment.