Zn@TA assisted dual cross-linked 3D printable glycol grafted chitosan hydrogels for robust antibiofilm and wound healing

• Published in: Carbohydrate polymers 2024-11, Vol.344, p.122522, Article 122522
• Main Authors: Patil, Tejal V., Jin, Hexiu, Dutta, Sayan Deb, Aacharya, Rumi, Chen, Kehan, Ganguly, Keya, Randhawa, Aayushi, Lim, Ki-Taek
• Format: Article
• Language: English
• Subjects: 3D printing; Animals; Anti-Bacterial Agents - chemistry; Anti-Bacterial Agents - pharmacology; Antibacterial; Bacillus subtilis - drug effects; Biocompatible Materials - chemistry; Biocompatible Materials - pharmacology; Biofilms - drug effects; Chitosan; Chitosan - chemistry; Chitosan - pharmacology; Cross-Linking Reagents - chemistry; Escherichia coli - drug effects; Fibroblasts - drug effects; Humans; Hydrogels - chemistry; Hydrogels - pharmacology; Macrophages - drug effects; Male; Mice; Multifunctional hydrogel; Printing, Three-Dimensional; Rats; Rats, Sprague-Dawley; RAW 264.7 Cells; Wound healing; Wound Healing - drug effects; Zinc - chemistry; Zinc - pharmacology; Zinc-tannic acid
• ISSN: 0144-8617; 1879-1344; 1879-1344
• DOI: 10.1016/j.carbpol.2024.122522

Rapid regeneration of the injured tissue or organs is necessary to achieve the usual functionalities of the damaged parts. However, bacterial infections delay the regeneration process, a severe challenge in the personalized healthcare sector. To overcome these challenges, 3D-printable multifunctional hydrogels of Zn/tannic acid-reinforced glycol functionalized chitosan for rapid wound healing were developed. Polyphenol strengthened intermolecular connections, while glutaraldehyde stabilized 3D-printed structures. The hydrogel exhibited enhanced viscoelasticity (G′; 1.96 × 104 Pa) and adhesiveness (210 kPa). The dual-crosslinked scaffolds showed remarkable antibacterial activity against Bacillus subtilis (∼81 %) and Escherichia coli (92.75 %). The hydrogels showed no adverse effects on human dermal fibroblasts (HDFs) and macrophages (RAW 264.7), indicating their superior biocompatibility. The Zn/TA-reinforced hydrogels accelerate M2 polarization of macrophages through the activation of anti-inflammatory transcription factors (Arg-1, VEGF, CD163, and IL-10), suggesting better immunomodulatory effects, which is favorable for rapid wound regeneration. Higher collagen deposition and rapid re-epithelialization occurred in scaffold-treated rat groups vis-à-vis controls, demonstrating superior wound healing. Taken together, the developed multifunctional hydrogels have great potential for rapidly regenerating bacteria-infected wounds in the personalized healthcare sector. [Display omitted] •Zn@TA-assisted multifunctional glycol-functionalized chitosan hydrogels were fabricated.•The hydrogels demonstrated superior printability and adhesiveness (210 kPa).•Remarkable antibacterial and antibiofilm activity against B. subtilis and E. coli.•Hydrogels accelerated M2 polarization and expression of wound healing gene markers.•Higher collagen deposition and rapid re-epithelialization in 3D printed scaffold-treated rat groups.