In Situ Crosslinked Biodegradable Hydrogels Based on Poly(Ethylene Glycol) and Poly(ε-Lysine) for Medical Application

Hydrogels have emerged as promising biomaterials due to their excellent performance; however, their biocompatibility, biodegradability, and absorbability still require improvement to support a broader range of medical applications. This paper presents a new biofunctionalized hydrogel based on in situ crosslinking between maleimide-terminated four-arm-poly(ethylene glycol) (4–arm–PEG–Mal) and poly(ε-lysine) (ε–PL). The PEG/ε–PL hydrogels, named LG–n, were rapidly formed via amine/maleimide reaction by mixing 4–arm–PEG–Mal and ε–PL under physiological conditions. The corresponding dry gels (DLG–n) were obtained through a freeze-drying technique. 1H NMR, FT–IR, and SEM were utilized to confirm the structures of 4–arm–PEG–Mal and LG–n (or DLG–n), and the effects of solid content on the physicochemical properties of the hydrogels were investigated. Although high solid content could increase the swelling ratio, all LG–n samples exhibited a low equilibrium swelling ratio of less than 30%. LG–7, which contained moderate solid content, exhibited optimal compression properties characterized by a compressive fracture strength of 45.2 kPa and a deformation of 69.5%. Compression cycle tests revealed that LG–n demonstrated good anti-fatigue performance. In vitro degradation studies confirmed the biodegradability of LG–n, with the degradation rate primarily governing the drug (ceftibuten) release efficiency, leading to a sustained release duration of four weeks. Cytotoxicity tests, cell survival morphology observation, live/dead assays, and hemolysis tests indicated that LG–n exhibited excellent cytocompatibility and low hemolysis rates (<5%). Furthermore, the broad-spectrum antibacterial activity of LG–n was verified by an inhibition zone method. In conclusion, the developed LG–n hydrogels hold promising applications in the medical field, particularly as drug sustained-release carriers and wound dressings.