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Chronic diabetic wounds, caused by persistent infections, oxidative stress, and high blood sugar, still require dressings that can adapt in stages and adjust to the microenvironment. Here, we developed a self-adaptive glycopeptide hydrogel composite (MnS@ZGF hydrogel) reinforced with hybrid nanoenzymes, designed to coordinate glucose-consumption-driven ROS-H2S signaling cascades for multi-stage diabetic wound repair. The hybrid nanoenzyme (MnS@ZG) has a Co-coated MnS core with a dimethylimidazole/glucose oxidase shell, promoting synergistic glucose consumption, ROS-mediated antibacterial effects, and sustained H2S-driven anti-inflammatory and pro-angiogenic signaling. The MnS@ZGF hydrogel is embedded in a dynamic glycopeptide network formed spontaneously from oxidized sodium alginate (OSA), ε-poly-L-lysine (PL), and thermosensitive F127, showing excellent injectability, tissue adhesion, mechanical strength, and self-healing, allowing it to conform well to irregular wounds. Mechanistic simulations indicate that hydrogen bonding and metal coordination work together to stabilize the nanoenzyme-hydrogel interface. In vitro, the MnS@ZGF hydrogel demonstrates time-coded therapeutic features through glucose-responsive ROS-H2S cascade reactions, enabling early ROS-mediated infection control followed by H2S-driven immune modulation and fibroblast migration. In vivo, transcriptomic and histological analyses show it effectively remodels the wound immune microenvironment, accelerates wound closure, neovascularization, and collagen remodeling, while reducing scar formation and maintaining excellent biocompatibility. This study provides a promising strategy with significant clinical translation potential for time-planned, multi-stage repair of hard-to-heal diabetic wounds.
Summary
Diabetic wound infections, oxidative stress, and high blood sugar are all intertwined, and wound healing occurs in stages. So the authors introduced hybrid nanoenzymes into a glycopeptide hydrogel. MnS@ZG has an MnS core wrapped with a shell of Co²⁺/dimethylimidazole/glucose oxidase; it can consume glucose, produce ROS, and continuously release H₂S. Then, combined with oxidized sodium alginate, ε-polylysine, and F127 for self-crosslinking, they created an injectable, adhesive, self-healing MnS@ZGF gel. The key idea is to use glucose to drive a ROS-H₂S cascade, allowing the dressing to act in stages according to the wound microenvironment.
Simulations showed that hydrogen bonds and metal coordination together stabilize the interface between the nanoenzyme and the hydrogel. In vitro experiments showed that the gel first uses ROS to control infection, then uses H₂S to regulate immunity and promote fibroblast migration, showing a time-programmed effect. In vivo transcriptomics and histology indicated that it can reshape the wound immune microenvironment, speed up closure, angiogenesis, and collagen remodeling, reduce scarring, and maintain good biocompatibility. This approach combines glucose consumption, gas signaling, and adaptive dressings, offering a new idea for staged repair and clinical translation of hard-to-heal diabetic wounds.
Reference:
DOI: 10.1002/adfm.78900
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