School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Key Laboratory of Electrical Insulation and Thermal Aging, Shanghai Jiao Tong University, Shanghai, 200240, P. R. China.
Adv Healthc Mater. 2022 Mar;11(6):e2101809. doi: 10.1002/adhm.202101809. Epub 2021 Dec 16.
Polymeric hydrogels have been increasingly studied for wound sealants, adhesives, hemostats, and dressings, however, multi-component gelation, adhesion-causing tissue damage, inefficient hemostasis, and skin scarring in wound healing hamper their advances. So it is urgent to develop multifunctional single-component polymeric hydrogels with benign tissue detachment, high performance hemostasis, and scarless wound healing attributes. Herein, a dopamine-modified poly(l-glutamate) hydrogel at an ultralow concentration of 0.1 wt% is serendipitously constructed by physical treatments, in which a gelation mechanism is disclosed via oxidative catechol-crosslinking and sequential dicatechol-carboxyl hydrogen-bonding interactions. The covalent/H-bonding co-crosslinked and highly negative-charged networks enable the polypeptide hydrogels thermo-, salt-, urea-resistant, self-healing, injectable, and adhesive yet detachable. In vitro and in vivo assays demonstrate they have superior biocompatibility with ≈0.5% hemolysis and negligible inflammation. The polypeptide/graphene oxide hybrid hydrogel performs fast and efficient hemostasis of 12 s and 1.4% blood loss, surpassing some hydrogels and commercial counterparts. Remarkably, the polypeptide hydrogels achieve scarless and full wound healing and regenerate thick dermis with some embedded hair follicles within 14 days, presenting superior full-thickness wound healing and skin scar-preventing capabilities. This work provides a simple and practicable method to construct multifunctional polypeptide hemostatic and healing hydrogels that overcome some above-mentioned hurdles.
高分子水凝胶在伤口密封剂、粘合剂、止血剂和敷料方面的研究越来越多，然而，多组分凝胶化、引起组织损伤的粘连、低效止血和伤口愈合中的皮肤瘢痕阻碍了它们的进展。因此，迫切需要开发具有良性组织分离、高性能止血和无瘢痕伤口愈合特性的多功能单组分高分子水凝胶。在此，通过物理处理意外构建了一种超低浓度（0.1wt%）的多巴胺修饰聚（谷氨酸）水凝胶，揭示了通过氧化儿茶酚交联和顺序二儿茶酚-羧基氢键相互作用的凝胶化机制。共价/H 键协同交联和高度带负电荷的网络使多肽水凝胶具有热稳定性、耐盐性、耐尿素性、自修复性、可注射性和可黏附性，但可分离。体外和体内试验表明，它们具有≈0.5%溶血和可忽略不计的炎症的优异生物相容性。多肽/氧化石墨烯杂化水凝胶的止血速度快，效率高，仅需 12s 即可止血，失血量仅为 1.4%，超过了一些水凝胶和商业产品。值得注意的是，多肽水凝胶可实现无瘢痕和完全伤口愈合，并在 14 天内再生带有一些嵌入毛囊的厚真皮，表现出优异的全层伤口愈合和皮肤瘢痕预防能力。这项工作提供了一种简单实用的方法来构建多功能多肽止血和愈合水凝胶，克服了上述一些障碍。
