<p>The development of multifunctional, biocompatible hydrogels is crucial for advancing regenerative medicine, rehabilitation, and 3D bioprinting. In this study, we report the synthesis and characterization of methacrylated chitosan (MACS) hydrogels functionalized with choline-based bio-ionic liquids (Bio-ILs) as a novel class of photocurable bioinks for bone-oriented biofabrication. Methacrylation of chitosan was confirmed by 1H NMR and FTIR spectroscopy, verifying successful functional group integration. Incorporation of methacrylated choline-based ionic liquids enabled efficient UV crosslinking and introduced an anion-dependent design parameter, allowing tunable porosity and viscoelastic behavior beyond conventional photocurable chitosan bioinks. These hybrid formulations were crosslinked using lithium phenyl-2,4,6-trimethylbenzoylphosphinate (LAP) and successfully 3D printed to yield structurally stable scaffolds. Scanning electron microscopy revealed controlled pore architectures (23.6–71.9&#xa0;μm), adjustable through Bio-IL anion chemistry, supporting cell infiltration. Swelling studies demonstrated high water uptake conducive to nutrient diffusion, while rheological analysis confirmed predominantly elastic gel behavior. Cytocompatibility was demonstrated using human mesenchymal stem cells (hMSCs), which maintained high viability and favorable adhesion over short-term culture. Overall, MACS/Bio-IL hydrogels represent customizable, cytocompatible scaffolds for bone-oriented biofabrication and additive biomanufacturing, providing a promising materials platform for future biomedical and rehabilitative applications.</p> Graphical Abstract <p></p>

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Development of Methacrylated Chitosan–Bio-Ionic Liquid Hybrid Bioinks: Photoreactive and Biocompatible Scaffolds for Additive Biomanufacturing in Bone Regeneration

  • Syeda Bushra Rahat,
  • Faiza Lughmani,
  • Rabid Ullah,
  • Vineetha Jayawarna,
  • Manuel Salmeron Sanchez,
  • Mudassir Iqbal

摘要

The development of multifunctional, biocompatible hydrogels is crucial for advancing regenerative medicine, rehabilitation, and 3D bioprinting. In this study, we report the synthesis and characterization of methacrylated chitosan (MACS) hydrogels functionalized with choline-based bio-ionic liquids (Bio-ILs) as a novel class of photocurable bioinks for bone-oriented biofabrication. Methacrylation of chitosan was confirmed by 1H NMR and FTIR spectroscopy, verifying successful functional group integration. Incorporation of methacrylated choline-based ionic liquids enabled efficient UV crosslinking and introduced an anion-dependent design parameter, allowing tunable porosity and viscoelastic behavior beyond conventional photocurable chitosan bioinks. These hybrid formulations were crosslinked using lithium phenyl-2,4,6-trimethylbenzoylphosphinate (LAP) and successfully 3D printed to yield structurally stable scaffolds. Scanning electron microscopy revealed controlled pore architectures (23.6–71.9 μm), adjustable through Bio-IL anion chemistry, supporting cell infiltration. Swelling studies demonstrated high water uptake conducive to nutrient diffusion, while rheological analysis confirmed predominantly elastic gel behavior. Cytocompatibility was demonstrated using human mesenchymal stem cells (hMSCs), which maintained high viability and favorable adhesion over short-term culture. Overall, MACS/Bio-IL hydrogels represent customizable, cytocompatible scaffolds for bone-oriented biofabrication and additive biomanufacturing, providing a promising materials platform for future biomedical and rehabilitative applications.

Graphical Abstract