Mechanical Stabilization of Alginate Hydrogel Fiber and 3D Constructs by Mussel-Inspired Catechol Modification

Alginate is a representative biocompatible natural polymer with low cost for a variety of biomedical applications, such as wound dressing, drug delivery systems, tissue scaffolds, and 3D bioprinting. Particularly, the rapid and facile gelation of alginate via ionic interactions with divalent cations has been used for in situ 3D hydrogel fiber formation, which is potentially applicable to engineering cell alignment. However, challenges in enhancing the mechanical properties of alginate hydrogel fibers under physiological conditions are unresolved because of their fast dissociation by ion exchange. Herein, we report a stabilization strategy for alginate hydrogel fibers through mussel-inspired catechol chemistry, which involves inter-catechol crosslinking within a few minutes under basic conditions. The fabrication of catechol-tethered alginate hydrogel fibers through wet-spinning enabled the design of mechanically strong 3D constructs consisting of fibers. Catechol-to-quinone oxidation followed by covalent crosslinking enhanced the tensile strength of a single fiber. Additionally, the 'gluing' capability of the catechol stabilized the interface among the fibers, thus retaining the shape fidelity of the 3D constructs and encapsulating the cell density during culture. Our findings will be useful for designing bioink materials specialized in fibrous-type tissue scaffolds with mechanical stability.