A Versatile Zwitterionic Gelation Strategy Triggered by Phenol-Modified Biomacromolecules: Facile Synthesis of Bioactive and Customizable Hydrogels.

The functionalization and biological activity of hydrogel interfaces are significant for implantation and therapeutic applications. By introducing various monomers or additives during conventional gelation processes, facile functional modification and biological activity regulation of hydrogels can be achieved. However, these methods face challenges of potential toxicity and the preparation procedure. Here, we report a phenol-triggered universal gelation strategy involving solely phenol-modified biomacromolecules and zwitterionic monomers, which achieves superior biocompatibility. Significantly, this strategy exhibits universality for common biomass (e.g., polysaccharides and polypeptides), as well as for phenols, enabling substantial scope for functional diversification and application. The hydrogels are prepared by branching on the biomacromolecules, which imparts modular physicochemical and biomedical properties. Furthermore, simply by modulating substrate composition and performing rapid surface treatment, the hydrogel interfaces can regulate biological activities including cell adhesion and antifouling properties. This work presents a universal gelation strategy that offers an effective and promising approach for the design of biointerfaces.