Superparamagnetic ferrogels with high swelling ability and potential applications as solvent absorbers and stimuli-responsive drug delivery devices were obtained by a non-toxic and environmentally friendly route based on dispersion of poly(acrylic acid)-coated iron oxide nanoparticles (PAA-coated NPs) in poly(vinyl alcohol) (PVA) solutions followed by freezing–thawing. Presence of carboxylate groups arising from the PAA coating allowed hydrogen bonding formation between NPs and PVA and enabled the synthesis of optically homogenous, superparamagnetic materials formed by a homogenous distribution of NPs diffuse clusters in the PVA matrix. The addition of PAA-coated NPs produced a remarkable increase in crystallinity degree, thermal degradation and swelling percentage respect to the neat matrix, which demonstrates that ferrogels with improved properties can be obtained by this procedure. Thereafter, combination of a cryogenic technique with the use of non-toxic components and magnetic NPs coated by a pH sensitive polymer makes these ferrogels very promising for applications in the biomedical field.

Self-assembly of natural polymers constitute a powerful route for the development of functional materials. In particular, layer-by-layer (LBL) assembly constitutes a versatile technique for the nanostructuration of biobased polymers into multilayer films. Gelatin has gained much attention for its abundance, biodegradability, and excellent gel-forming properties. However, gelatin gels melt at low temperature, thus limiting its practical application. With respect to the above considerations, here, we explored the potential application of gelatin gels as a matrix for protein delivery at physiological temperature. A model protein, bovine serum albumin (BSA), was encapsulated within gelatin gels and then coated with a different number of bilayers of alginate and chitosan (10, 25, 50) in order to modify the diffusion barrier. The coated gel samples were analyzed by means of Attenuated Total Reflectance-Fourier Transform Infrared (ATR-FTIR) and confocal Raman spectroscopy, and it was found that the multilayer coatings onto polymer film were interpenetrated to some extent within the gelatin. The obtained results inferred that the coating of gelatin gels with polysaccharide multilayer film increased the thermal stability of gelatin gels and modulated the BSA release. Finally, the influence of a number of bilayers onto the drug release mechanism was determined. The Ritger-Peppas model was found to be the most accurate to describe the diffusion mechanism.