4.7 Article

Thiol-Rich Multifunctional Macromolecular Crosslinker for Gelatin-Norbornene-Based Bioprinting

期刊

BIOMACROMOLECULES
卷 22, 期 6, 页码 2729-2739

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.biomac.1c00421

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资金

  1. National Key R&D Program of China [2018YFC1106001]
  2. National Natural Science Foundation of China [51903255]
  3. Science and Technology Program of Guangzhou City [201904010364]
  4. Key Areas Research and Development Program of Guangdong [2020B1111150003]

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Extrusion-based bioprinting using GelNB hydrogels has shown to be promising for cell encapsulation and protection, with the inclusion of a thiolated heparin crosslinker (HepSH) allowing for customization of mechanical properties and providing benefits for cell viability and potential neovascularization. The GelNB/HepSH bioink demonstrates good printability and potential applications in regenerative medicine.
Extrusion-based bioprinting is an emerging and most frequently used technique for the fabrication of cell-laden constructs. A suitable hydrogel-based bioink for cell encapsulation and protection is critical for printability, structural stability, and post-printing cell viability. The thiol-ene chemistry-based gelatin-norbomene (GelNB) hydrogels have drawn much attention as a promising substitution of gelatin methacryloyl (GelMA), owing to the fast and controllable step-growth polymerization mechanism, as well as a significant reduction in reactive oxygen species (ROS) accumulation. Herein, thiolated heparin (HepSH) was synthesized and used as a macromolecular crosslinker for GelNB-based bioprinting, so that GelNB gelation became less sensitive to the thiol/ene ratio. The mechanical stability and moduli of GelNB/HepSH hydrogels were easily manipulated by the concentration and/or degree of thiol substitution. The GelNB/HepSH hydrogel allowed little intracellular ROS for encapsulated cells but provided vascular endothelial growth factor binding affinity for potential facilitation of neovascularization. Finally, the GelNB/HepSH bioink enabled a convenient printing process for both complex-structured bioscaffolds and cell-laden constructs, and resulted in good printability and high post-crosslinldng cell viability. The crosslinker HepSH may serve as a multifunctional macromolecule that enables GelNB-based bioprinting in broad applications in regenerative medicine.

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