High performance and reversible ionic polypeptide hydrogel based on charge-driven assembly for biomedical applications

In the pursuit of new strategies for the design and synthesis of high performance, physically associated hydrogels, dynamic materials formed through electrostatic interactions can serve as a powerful model. Here, we introduce a convenient strategy to obtain biodegradable hydrogels from ABA triblock ionic polypeptides formed by mixing poly(l-glutamic acid)–block-poly(ethylene glycol)–block-poly(l-glutamic acid) (PGA–PEG–PGA) with poly(l-lysine)–block-poly(ethylene glycol)–block-poly(l-lysine) (PLL–PEG–PLL). The hydrogels showed tunable physical properties, high strength and reversible response. The reactive function groups in the ionic blocks can conjugate with oppositely charged drugs or proteins and allow for further modification. These ionic ABA triblock polyelectrolytes can also encapsulate intact cells without significantly compromising cell viability, suggesting that the hydrogels have excellent cytocompatibility. In vivo evaluation performed in rats with subcutaneous injection indicated that the gels were formed and degraded, and hematoxylin and eosin staining suggested good biocompatibility in vivo. In addition, these advantages, combined with the synthetic accessibility of the copolymer, make this cross-linking system a flexible and powerful new tool for the development of injectable hydrogels for biomedical applications.