Photo-tunable hydrogel mechanical heterogeneity informed by predictive transport kinetics model

Understanding the three-dimensional (3D) mechanical and chemical properties of distinctly different, adjacent biological tissues is crucial to mimicking their complex properties with materials. 3D printing is a technique often employed to spatially control the distribution of the biomaterials, such as hydrogels, of interest, but it is difficult to print both mechanically robust (high modulus and toughness) and biocompatible (low modulus) hydrogels in a single structure. Moreover, due to the fast diffusion of mobile species during printing and nonequilibrium swelling conditions of low-solids-content hydrogels, it is challenging to form the high-fidelity structures required to mimic tissues. Here a predictive transport and swelling model is presented to model these effects and then is used to compensate for these effects during printing. This model is validated experimentally by photopatterning spatially distinct hydrogel elastic moduli using a single photo-tunable poly(ethylene glycol) (PEG) pre-polymer solution by sequentially patterning and in-diffusing fresh pre-polymer for further polymerization.