Self‐Healing Silk Fibroin‐Based Hydrogel for Bone Regeneration: Dynamic Metal‐Ligand Self‐Assembly Approach |
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Authors: | Liyang Shi Fanlu Wang Wei Zhu Zongpu Xu Sabine Fuchs Jöns Hilborn Liangjun Zhu Qi Ma Yingjie Wang Xisheng Weng Dmitri A Ossipov |
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Affiliation: | 1. Science for Life Laboratory, Division of Polymer Chemistry, Department of Chemistry‐?ngstr?m, Uppsala University, Uppsala, Sweden;2. Experimental Trauma Surgery, University Medical Center Schleswig Holstein UKSH, Kiel, Germany;3. Department of Big Surgery, Peking Union Medical College Hospital, Chinese Academy of Medical Sciences & Peking Union Medical College, Beijing, China;4. Institute of Applied Bioresources Research, College of Animal Science, Zhejiang University, Hangzhou, China;5. Department of Orthopedics, Peking Union Medical College Hospital, Chinese Academy of Medical Sciences & Peking Union Medical College, Beijing, China |
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Abstract: | Despite advances in the development of silk fibroin (SF)‐based hydrogels, current methods for SF gelation show significant limitations such as lack of reversible crosslinking, use of nonphysiological conditions, and difficulties in controlling gelation time. In the present study, a strategy based on dynamic metal‐ligand coordination chemistry is developed to assemble SF‐based hydrogel under physiological conditions between SF microfibers (mSF) and a polysaccharide binder. The presented SF‐based hydrogel exhibits shear‐thinning and autonomous self‐healing properties, thereby enabling the filling of irregularly shaped tissue defects without gel fragmentation. A biomineralization approach is used to generate calcium phosphate‐coated mSF, which is chelated by bisphosphonate ligands of the binder to form reversible crosslinkages. Robust dually crosslinked (DC) hydrogel is obtained through photopolymerization of acrylamide groups of the binder. DC SF‐based hydrogel supports stem cell proliferation in vitro and accelerates bone regeneration in cranial critical size defects without any additional morphogenes delivered. The developed self‐healing and photopolymerizable SF‐based hydrogel possesses significant potential for bone regeneration application with the advantages of injectability and fit‐to‐shape molding. |
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Keywords: | bone regeneration hydrogels self‐assembly self‐healing silk fibroin |
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