A time-dependent understanding of swelling characteristics and external stimuli behavior is crucial for the development and understanding of functional hydrogels. Magnetic resonance imaging (MRI) offers the opportunity to study three-dimensional (3D) soft materials nondestructively. This technique is already widely used as an image-based medical diagnostic tool and is applied here to evaluate complex structures of a hydrogel-a double network of chemically crosslinked casein enhanced with alginate-fabricated by 3D printing. When hydrogel disks immersed in four different liquid systems were analyzed, the material exhibited distinct system-dependent behavior characterized by rheological and mechanical measurements. Further material functionalization was achieved by macroscopic structuring of the hydrogel as an auxetic material based on a re-entrant honeycomb structure. MRI offers the advantage of monitoring overall changes in the area of the analyzed specimen and internal structural changes simultaneously. To assess the behavior of this complex structure, a series of short MRI measurements, each lasting 1.7 min, captured liquid diffusion and thus structural swelling behavior. A clear dependence of external and internal structural changes as a function of liquid properties causing these changes was observed. In conclusion, this approach might pave the way for prospective applications to monitor liquid diffusion into (e.g., vascularization) and swelling behavior of functional hydrogels.
Keywords: 3D printing; auxetics; localized anisotropic swelling; magnetic resonance imaging; protein-based hydrogels; stimuli-responsive material.