Spatiotemporally adjustable hybrid hydrogels interconnected by 2D MXene for combinatorial therapy of infected diabetic wounds

초록

Spatiotemporally adjustable and multifunctional bioresponsive dual-crosslinked hydrogels (MultiBioGel) were developed by integrating two-dimensional (2D) MXene nanosheets into a peptide-annealed terpolymer matrix via response surface methodology-optimized fabrication. This 2D nanostructure-entangled hydrogel system harnesses the combinatorial contributions of MXene's reactive oxygen species (ROS)-scavenging and photothermal properties, the mechanical durability and pH-responsive nature of the poly(acrylic acid-co-3-acrylamidopropanoic acid-co-acrylamide) network, and daptomycin (DPT)'s antimicrobial activity. Our MultiBioGel hydrogel integrates (i) a mechanically robust dual-crosslinked terpolymer matrix, (ii) MXene, which provides redox-mediated ROS/reactive nitrogen species scavenging and photothermal antibacterial activity, and (iii) DPT, a potent gram-positive membrane-disruptive antibiotic. This design enables rapid gelation, injectability, shape adaptability, sustained drug release, and combinatorial antibacterial performances under near-infrared light irradiation-features that are often absent or underdeveloped in traditional natural polymer-based hydrogels. In addition, the hydrogel promotes tissue regeneration through epidermal renewal, angiogenesis, and macrophage polarization. This hybrid hydrogel platform demonstrated potent therapeutic efficacy in both non-infected and bacteria-infected diabetic wound models, offering a promising solution for advanced combinatorial wound healing therapy.

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