Multi-Functional Supramolecular-Polymeric Hybrid Hydrogel for Promoting Cutaneous Wound Repair†

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.