Self-recovering dual cross-linked hydrogels based on bioorthogonal click chemistry and ionic interactions

The biocompatible, injectable and high water-swollen nature of hydrogels makes them a popular candidate to imitate the extracellular matrix (ECM) for tissue engineering both in vitro and in vivo . However, commonly used covalently cross-linked hydrogels, despite their stability and tunability, are e...

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Bibliographic Details
Published in:Journal of materials chemistry. B, Materials for biology and medicine Materials for biology and medicine, 2020-07, Vol.8 (27), p.5912-592
Main Authors: Zhan, Henan, Jiang, Shanshan, Jonker, Anika M, Pijpers, Imke A. B, Löwik, Dennis W. P. M
Format: Article
Language:English
Subjects:
Alkynes
Alkynes - chemistry
Azides - chemistry
Biocompatibility
Biocompatible Materials - chemistry
Biocompatible Materials - metabolism
Calcium
Calcium - chemistry
Calcium ions
Cations, Divalent - chemistry
Cell culture
Cell Proliferation
Cells, Cultured
Chemical reactions
Chemical synthesis
Click Chemistry
Covalence
Cross-Linking Reagents - chemistry
Crosslinking
Cycloaddition
Cycloaddition Reaction
Extracellular matrix
Extracellular Matrix - metabolism
Gels
Humans
Hydrogels
Hydrogels - chemistry
Hydrogels - metabolism
Ionic interactions
Links
Mechanical Phenomena
Mechanical properties
Mesenchymal Stem Cells - cytology
Mesenchymal Stem Cells - metabolism
Mesenchyme
Oligopeptides - chemistry
Organophosphonates - chemistry
Phase separation
Phosphonates
Polyethylene glycol
Polyethylene Glycols - chemistry
Polyethylene Glycols - metabolism
Rheology
Scanning electron microscopy
Stem cells
Strain
Tissue Engineering
Tissue Scaffolds - chemistry
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Summary:The biocompatible, injectable and high water-swollen nature of hydrogels makes them a popular candidate to imitate the extracellular matrix (ECM) for tissue engineering both in vitro and in vivo . However, commonly used covalently cross-linked hydrogels, despite their stability and tunability, are elastic and deteriorate as bulk material degrades which would impair proper cell function. To improve these deficiencies, here, we present a self-recovering cross-linked hydrogel formed instantaneously with functionalized poly(ethylene glycol) as a basis. We combine covalent cross-links introduced via a strain-promoted azide-alkyne cycloaddition (SPAAC) click reaction and non-covalent links between phosphonate groups and calcium ions. By adjusting the ratios of non-covalent and covalent cross-links, we synthesized these dual cross-linked (DC) hydrogels that displayed storage moduli below ∼2000 Pa and relaxation times from seconds to minutes. The gels recovered to 41-96% of their initial mechanical properties after two subsequent strain failures. Cryo-scanning electron microscopy revealed that DC hydrogels containing approximately equal amounts of covalent and non-covalent cross-links displayed phase separation. Finally, we functionalized the DC hydrogels by incorporating an integrin binding motif, RGDS, to provide a biocompatible environment for human mesenchymal stem cells (HMSCs) by facilitating adhesion inside the gel network. Inside these DC gels HSMCs displayed a viability up to 73% after five days of cell culture. The biocompatible, injectable and high water-swollen nature of dual cross-linked hydrogels makes them a popular candidate to imitate the extracellular matrix (ECM) for tissue engineering both in vitro and in vivo .
ISSN:2050-750X
2050-7518
DOI:10.1039/d0tb01042a