An Injectable Self‐Crosslinked Wholly Supramolecular Polyzwitterionic Hydrogel for Regulating Microenvironment to Boost Infected Diabetic Wound Healing

Abstract

It is highly desirable yet significantly challenging to fabricate injectable, self‐crosslinked, self‐fused, and antifouling polyzwitterionic hydrogels, whose successful preparation will expand their application scope in biomedical fields. Herein, for the first time, a novel zwitterionic monomer, carboxybetaine urethane acrylate (CBUTA) is designed and synthesized with a urethane group and zwitterion on the same side chain. The strong inter‐urethane H‐bonds and zwitterionic dipole–dipole interactions of side chains contribute to self‐crosslinked wholly supramolecular polyzwitterionic hydrogel that is directly formed from photoinitiated polymerization of CBUTA aqueous solution without adding any chemical crosslinkers. After being swollen in water, the polyCBUTA (PCBUTA) hydrogel is squeezed into small particles and freeze‐dried to obtain hydrogel powder. The injectable and wholly zwitterionic supramolecular PCBUTA hydrogel can be easily reconstructed by mixing hydrogel powder with water due to the recombination of H‐bonds of urethane groups and zwitterionic dipole–dipole interactions. The re‐formed PCBUTA hydrogel exhibits an excellent self‐fused and antifouling ability, and this injectable PCBUTA hydrogel, endowed with a microenvironment‐regulated function, demonstrates excellent glucose consumption, antioxidation, antibacterial, and angiogenesis ability, thus accelerating the infected diabetic wound healing. Overall, this work provides a promising strategy to develop injectable and wholly zwitterionic hydrogels that will find broad biomedical applications.

Low hysteresis zwitterionic supramolecular polymer ion-conductive elastomers with anti-freezing properties, high stretchability, and self-adhesion for flexible electronic devices

“…To verify it, the as-prepared PCBUIA hydrogel cylinder samples were immersed in a 5 M urea aqueous solution or a precooled mixture solution of 7 wt% NaOH and 12 wt% urea, respectively, which are commonly used as hydrogen bond-breaking agents to verify the hydrogen interactions. 39 Immersed in the 5 M urea solution for 12 h, the PCBUIA hydrogel remained intact without the occurrence of dissolution. While in the precooled mixture solution of 7 wt% NaOH and 12 wt% urea for 12 h, a stronger H-bond dissociating agent, 40 the PCBUIA hydrogel almost disappeared and dissociated to the homogeneous aqueous solution (Fig.…”

Self‐assembly of PEG–PPS polymers and LL‐37 peptide nanomicelles improves the oxidative microenvironment and promotes angiogenesis to facilitate chronic wound healing

“…Angiogenesis plays a crucial role in diabetic wound healing. Neovascularization provides oxygen and nutrition to the wound, thereby accelerating wound healing 49 . Several studies have demonstrated that LL‐37 can promote vascular endothelial cell migration and angiogenesis.…”

Surface Wrinkled Microsphere Enhanced Irregular Wound Healing Through Synergistic Hygroscopicity, Reversible Wet‐Adhesion and Antibacterial Properties

“…Recently, researchers have reported in situ-formed wound dressings such as injectable hydrogels to circumvent the drawbacks of conventional dressings for irregular wounds. [20][21][22] Nonetheless, long gelation time, poor mechanical properties, and lack of an extracellular matrix-like (ECM) structure of these dressings have limited their potential for clinical application. [23][24][25] In addition, the gelation process of most of injectable hydrogels need to be accomplished under invasive external stimuli, such as pH, light, temperature or organic cross-linked agents.…”