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

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Abstract

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.

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

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Supplementary files

Article information


Submitted
21 Apr 2020
Accepted
08 Jun 2020
First published
09 Jun 2020

This article is Open Access

J. Mater. Chem. B, 2020, Advance Article
Article type
Paper

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

H. Zhan, S. Jiang, A. M. Jonker, I. A. B. Pijpers and D. W. P. M. Löwik, J. Mater. Chem. B, 2020, Advance Article , DOI: 10.1039/D0TB01042A

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