Dual Cross-Linked Hydrogels with Injectable, Self-Healing, and Antibacterial Properties Based on the Chemical and Physical Cross-Linking

Injectable hydrogels have become a promising material for biomedical engineering applications, but microbial infection remains a common challenge in their application. In this study, we presented an injectable antibacterial hydrogel with self-healing property based on a dual cross-linking network structure of dynamic benzoxaborole–sugar and quadruple hydrogen bonds of the 2-ureido-4-pyrimidone (UPy) moieties at physiological pH. Dynamic rheological experiments demonstrated the gelatinous behavior of the double cross-linking network (storage modulus G′ > loss modulus G″), and the modulus showed frequency-dependent behavior. The noncovalent interactions of UPy units in the polymer segment endowed the injectable hydrogels with good mechanical strength. By varying the solid contents, UPy units, as well as the pH, the mechanical properties of hydrogels could be controlled. Additionally, the hydrogels exhibited not only excellent self-healing and injectable properties but also pH and sugar dual-responsiveness. Moreover, the hydrogels could effectively inhibit the growth of both Escherichia coli and Staphylococcus aureus while exhibiting low toxicity. 3D cell encapsulation experiment results also demonstrated the potential use of these hydrogels as cell culture scaffolds. Taken together, the injectability, self-healing, and antimicrobial properties of the prepared hydrogels showed great promise for translational medicine, such as cell and tissue engineering applications.