In this study, a new strategy was adopted for obtaining polymer/protein hybrid hydrogels with shape stability and tunable mechanical or rheological characteristics by using non-toxic procedures. A chemical network was created using a poly(vinyl alcohol)(PVA)/bovine serum albumin (BSA) mixture in aqueous solution in the presence of genipin and reduced glutathione (GSH). Then, a second physical network was formed through PVA after applying freezing/thawing cycles. In addition, the protein macromolecules formed intermolecular disulfide bridges in the presence of GSH. In these conditions, multiple crosslinked networks were obtained, determining the strengthening and stiffening into relatively tough porous hydrogels with tunable viscoelasticity and a self-healing ability. A SEM analysis evidenced the formation of networks with interconnected pores of sizes between 20 μm and 50 μm. The mechanical or rheological investigations showed that the hydrogels' strength and response in different conditions of deformation were influenced by the composition and crosslinking procedure. Thus, the dynamics of the hybrid hydrogels can be adjusted to mimic the viscoelastic properties of the native tissues. The dynamic water vapor-sorption ability, swelling behavior in an aqueous environment, and bioadhesive properties were also investigated and are discussed in this paper. The hybrid hydrogels with tunable viscoelasticity can be designed on request, and they are promising candidates for tissue engineering, bioinks, and wound dressing applications.
Keywords: bioadhesivity; bovine serum albumin; elastic modulus; hybrid hydrogel; mechanical behavior; poly(vinyl alcohol); quasi-Fickian diffusion; self-healing ability; viscosity.