Engineered magnetoactive collagen hydrogels with tunable and predictable mechanical response

In the present study, the synthesis of superparamagnetic collagen-based nanocomposite hydrogels with tunable swelling, mechanical and magnetic properties is reported. The fabrication strategy involved the preparation of pristine collagen type-I hydrogels followed by their immersion in highly stable aqueous solutions containing pre-formed double-layer oleic acid-coated hydrophilic magnetite nanoparticles (OA.OA.Fe3O4) at different concentrations, to interrogate nanoparticles' deposition within the 3D fibrous collagen matrix. Besides the investigation of the morphology, composition and magnetic properties of the produced materials, their mechanical properties were experimentally evaluated under confined compressive loading conditions while an exponential constitutive equation was employed to describe their mechanical response. Moreover, the deposition of the nanoparticles in the collagenous matrix was modeled mathematically with respect to the swelling of the gel and the effective stiffness of the matrix. The model recapitulated nanoparticle diffusion and deposition as well as hydrogel swelling, in terms of nanoparticles' size and concentration of OA.OA.Fe3O4 aqueous solution.