<p>Dynamic hydrogels serve as promising wound dressings by mimicking extracellular matrix (ECM) structures to regulate tissue hydration and oxygen permeability. In this study, a dynamic OG-ACMC hydrogel was synthesized via a Schiff base reaction between periodate-oxidized gellan gum (OG) and ethylenediamine-modified carboxymethyl chitosan (ACMC). Structural changes in oxidation, amination, and crosslinking processes were characterized, and the effects of designed OG/ACMC volume ratios (0.5:1–2:1) on morphologies and physicochemical and biological properties were investigated. Results demonstrated that C = N was successfully formed for achieving dynamic crosslinking, and the hydrogels exhibited a three-dimensional architecture with interconnected pores formed by stacked polymer lamellae. The morphological evolution of the lyophilized scaffolds, from fragile to stable porous architectures, was quantitatively correlated with a significant increase in crosslinking density. Increasing the OG/ACMC ratio densified the network, prolonged gelation time from 75.5 ± 3.2 s to over 300 s, and reduced the equilibrium swelling ratio at the 2:1 formulation while maintaining high and stable water vapor transmission rates. All hydrogels exhibited selective antibacterial activity, achieving up to 83.4% bactericidal rates against <i>S. aureus</i> but none against <i>E. coli</i>; L929 fibroblasts maintained 90.7–99.3% viability, confirming non-cytotoxicity of these hydrogels. After 72&#xa0;h, they promoted cell proliferation with viabilities of 101.95–103.98% and healthy spindle morphology. Notably, the 1:1 OG/ACMC ratio hydrogel additionally exhibited good injectability, shape adaptability, and self-healing capability. It also demonstrated elastic-dominated rheological behavior (G’ &gt; G’’), as well as stimuli-responsive degradation accelerated by vibration and delayed by Ca²⁺ chelation. These combined properties established the OG-ACMC dynamic hydrogel as a promising multifunctional wound dressing, with the 1:1 ratio demonstrating superior performance.</p>

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Fabrication of a schiff-base crosslinked hydrogel with tunable dynamic properties and cytocompatibility based on oxidized gellan gum and aminated carboxymethyl chitosan for wound dressing

  • Dong Liu,
  • Ling Zhang,
  • Zebin Shao,
  • Chenyang Liu,
  • Tianxiang Gao,
  • Jinkun Liu,
  • Yan Zhu,
  • Toshiki Miyazaki

摘要

Dynamic hydrogels serve as promising wound dressings by mimicking extracellular matrix (ECM) structures to regulate tissue hydration and oxygen permeability. In this study, a dynamic OG-ACMC hydrogel was synthesized via a Schiff base reaction between periodate-oxidized gellan gum (OG) and ethylenediamine-modified carboxymethyl chitosan (ACMC). Structural changes in oxidation, amination, and crosslinking processes were characterized, and the effects of designed OG/ACMC volume ratios (0.5:1–2:1) on morphologies and physicochemical and biological properties were investigated. Results demonstrated that C = N was successfully formed for achieving dynamic crosslinking, and the hydrogels exhibited a three-dimensional architecture with interconnected pores formed by stacked polymer lamellae. The morphological evolution of the lyophilized scaffolds, from fragile to stable porous architectures, was quantitatively correlated with a significant increase in crosslinking density. Increasing the OG/ACMC ratio densified the network, prolonged gelation time from 75.5 ± 3.2 s to over 300 s, and reduced the equilibrium swelling ratio at the 2:1 formulation while maintaining high and stable water vapor transmission rates. All hydrogels exhibited selective antibacterial activity, achieving up to 83.4% bactericidal rates against S. aureus but none against E. coli; L929 fibroblasts maintained 90.7–99.3% viability, confirming non-cytotoxicity of these hydrogels. After 72 h, they promoted cell proliferation with viabilities of 101.95–103.98% and healthy spindle morphology. Notably, the 1:1 OG/ACMC ratio hydrogel additionally exhibited good injectability, shape adaptability, and self-healing capability. It also demonstrated elastic-dominated rheological behavior (G’ > G’’), as well as stimuli-responsive degradation accelerated by vibration and delayed by Ca²⁺ chelation. These combined properties established the OG-ACMC dynamic hydrogel as a promising multifunctional wound dressing, with the 1:1 ratio demonstrating superior performance.