A Multifunctional Metallohydrogel with Injectability, Self‐Healing, and Multistimulus‐Responsiveness for Bioadhesives

Abstract

Multifunctional hydrogel bioadhesives have great prospects in biomedical applications, but their design still faces great challenges, such as multiple and tedious chemical modifications. However, it is difficult to integrate injectable, self‐healing, and stimulus‐responsive properties together. A facile approach based on dynamic metal‐ligand coordination chemistry between chondroitin sulfate (CS) and Fe3+ in the design and synthesis of novel multifunctional metallohydrogel bioadhesives is reported. This CS‐based hydrogel not only has strong tissue adhesion superior to that of commercial fibrin glue, but also exhibits an excellent self‐healing ability and injectability, which are beneficial in the field of bioadhesives. Moreover, the hydrogels undergo a rapid gel–sol transformation in response to multiple external stimuli, including pH, ions, neutral molecules, and chemical redox reactions enabling the rapid removal of the bioadhesive. In addition, metallohydrogels are rapidly formed within 10 s, quick enough to promptly seal the tissue. Importantly, the multifunctional CS‐based bioadhesives are shown to exhibit good biocompatibility, thus allowing the developed materials to meet key requirements for next‐generation tissue adhesives.

Stretchable, Injectable, and Self-Healing Conductive Hydrogel Enabled by Multiple Hydrogen Bonding toward Wearable Electronics

“…Moreover, when the strain returned to 1% after the failure of the hydrogel at 1000% strain, the reconstruction of the network occurred immediately demonstrated by an instant restoration of the mechanical strength. Both G ′ and G ″ were recovered to the initial values within 30 s. The spontaneous and reversible dissociation/association of the noncovalent cross-linkers formed by UPy dimerization and Fe 3+ coordination was responsible for the efficient energy dissipation upon elongation as well as the fast self-healing ability. , The effect of Fe 3+ concentration on the viscoelastic behavior and self-healing property of the hydrogels is displayed in Figure S8b,c. The repeatability of the self-healing behavior was further studied by applying continuous strain steps cycling between large and small amplitude (Figure c).…”

Adhesive hydrogels in osteoarthritis: from design to application

“…It has also been used as a dietary supplement for OA for decades to relieve pain and regenerate cartilage. Although CS has tissue adhesion because of its hydroxyl, carboxyl and amide groups, its intrinsic adhesion strength is relatively low [ 112 ]. Therefore, CS are chemically modified with tissue adhesive groups (such as thiol and aldehyde) to achieve higher tissue adhesiveness [ 66 ].…”

Evolution of nanostructured skin patches towards multifunctional wearable platforms for biomedical applications

“…176 Besides, chondroitin sulfate-based hydrogels were applied as multi-responsive adhesives to facilitate wound repair. 212 Furthermore, strategies for loading nucleic acids in composites have been recently evaluated to deliver RNAs, hence regulating the wound healing process. Specifically, miR-223 microRNAs (miRNAs) were incorporated in hyaluronic acid nanoparticles embedded in an adhesive gelatin methacryloyl hydrogel for reprogramming macrophages to anti-inflammatory phenotype (Fig.…”