Comprehensive Summary Supramolecular-polymeric hybrid hydrogels combining advantages of the assembled supramolecular networks and polymeric networks have attracted considerable attention recently. However, they are rarely used as multi-functional wound dressing materials. In this work, we report a supramolecular-polymeric hybrid hydrogel consisting of a co-assembled DBS-COOH/Naproxen network (DBS/NAP) and a polymeric gelatin (G)/quaternary ammonium group (Q) and phenylboronic acid groups (PBA)-grafted chitosan (QCS-PBA) network (G/QCS) for accelerating skin wound healing. The polymeric networks could obviously enhance the mechanical properties of the drug-derived supramolecular networks. Q groups endowed the hydrogel with enhanced antibacterial properties. Borate ester crosslinking between PBA groups and diol groups in DBS-COOH could effectively scavenge reactive radicals. The hybrid hydrogel exhibited tunable mechanical and adhesive properties due to the temperature-responsive gelatin networks. NAP could gradually release from hybrid hydrogel networks thus continuously relieving inflammation. Finally, the biocompatible, adhesive, antibacterial and antioxidant hybrid G/QCS-DBS/NAP gel could promote the in vivo healing stages in a full-thickness wounds with increased collagen deposition, upregulated CD31 expression and down-regulated TNF-α expression. Overall, this multi-functional supramolecular-polymeric hybrid hydrogel exhibited great potential for treating skin defects as promising wound dressing materials.
Hai-Yuan Zhang,Kun-Tang Wang,Yan Zhang,Yuan-Lu Cui,Qiangsong Wang
Skin trauma presents significant treatment challenges in clinical settings. Hydrogels made from naturally-derived polysaccharide have demonstrated great potential in wound healing. Here, a novel in-situ crosslinked self-healing hydrogel was prepared using oxidized Bletilla striata polysaccharide (BSP) and cationic gelatin via a Schiff-base reaction without the need for any chemical crosslinkers. Similar to the natural extracellular matrix, the BSP-gelatin hydrogel (BG-gel) exhibited typical viscoelastic characteristics. The rheological properties, mechanical behavior, porous structure, and degradation performance of BG-gel could be adjusted by changing the aldehyde group content of BSP. Importantly, the hydrogel showed superior hemostatic performance in rat tail amputation and liver incision models. It significantly facilitated wound healing by promoting hair follicles regeneration, blood vessels repair, collagen deposition, and inducing skin tissue remodeling via increased CD31 expression in a full-thickness skin wound rat model. This multifunctional hydrogel holds potential as a wound dressing for skin trauma, offering both hemostasis and expedited healing.
Traditional antibiotics are often ineffective against biofilm-associated infections, and biofilm-induced macrophage immune evasion directly halts the wound healing process. Disrupting biofilms and regulating macrophage immune functions are critical to improving wound healing. In this study, we synthesized g-C 3 N 4 with peroxidase (POD) enzyme activity via thermal polymerization and copper alginate microspheres (CAM) via gas cutting. These were co-encapsulated into GelMA hydrogels to form a functionalized wound repair system (GelMA/CAM@g-C 3 N 4 ) with both anti-biofilm and local immune microenvironment remodeling capabilities. In vitro, this system exhibited excellent biocompatibility and promoted endothelial cell migration, vascular formation, and CD31 expression. It also polarized macrophages toward the M1 phenotype, restoring their pro-inflammatory functions, upregulating inflammatory cytokines (IL-1, IL-6, TNF-α), and inhibiting Staphylococcus aureus and Escherichia coli . In vivo, the system suppressed S. aureus growth, promoted angiogenesis and collagen deposition, and reshaped the pathological microenvironment to achieve wound repair and regeneration. Conclusions: This system offers a new therapeutic strategy for chronic infectious wounds.
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