The presence of organic dyes in wastewater is a problem of growing interest due to its effect on the environment and human health. The aim of this work was to obtain magnetic hydrogels of methacrylated gelatin-g-polyelectrolyte to be used for the removal of methylene blue (MB) used as a model contaminant dye. Grafted gelatins with two degrees of functionalization (48% and 76%) were obtained and subsequently crosslinked using 2-acrylamido-2-methyl-1-propansulfonic acid (AMPS) and sodium 4-vinylbenzenesulfonate (SSNa) monomers. Magnetic nanoparticles were formed by an in situ precipitation method to easily remove the hydrogel from the adsorption medium. Our data show that the hydrogel with a low degree of methacrylation displayed a high degree of swelling and decreased stiffness due to its less connected polymer network. MB adsorption experiments showed that neither the low degree of methacrylation nor the presence of the aromatic group in the PSSNa polyelectrolyte generated an increase in the adsorption capacity of the hydrogel. However, a significant increase in the adsorption capacity was observed when dry hydrogels were combined compared to that of previously swollen hydrogel. The experimental data were non-linearly fitted to the pseudo-first and pseudo-second order models and in both cases, the highest q_e values were obtained for the GelMA-HF/PAMPS and GelMA-LF/PAMPS hydrogels. The Freundlich isotherm model was the one with the best correlation with the data (r² > 0.9700). Higher k_f values were obtained for the GelMA-HF/PAMPS and GelMA-LF/PAMPS hydrogels at 20 °C. The results obtained from this study demonstrated that magnetic polyelectrolyte-grafted gelatins are an efficient option for the removal of contaminant dyes from aqueous solutions.

Incorporating nanoparticles into injectable hydrogels is a well-known technique for improving the mechanical properties of these materials. However, significant differences in the mechanical properties of the polymer matrix and the nanoparticles can result in localized stress concentrations at the polymer–nanoparticle interface. This situation can lead to problems such as particle–matrix debonding, void formation, and material failure. This work introduces boronic acid/boronate ester dynamic covalent bonds (DCBs) as energy dissipation sites to mitigate stress concentrations at the polymer–nanoparticle interface. Once boronic acid groups were immobilized on the surface of SiO₂ nanoparticles (SiO₂-BA) and incorporated into an alginate matrix, the nanocomposite hydrogels exhibited enhanced viscoelastic properties. Compared to unmodified SiO₂ nanoparticles, introducing SiO₂ nanoparticles with boronic acid on their surface improved the structural integrity and stability of the hydrogel. In addition, nanoparticle-reinforced hydrogels showed increased stiffness and deformation resistance compared to controls. These properties were dependent on nanoparticle concentration. Injectability tests showed shear-thinning behavior for the modified hydrogels with injection force within clinically acceptable ranges and superior recovery.