PVA-gelatin hydrogels formed using combined theta-gel and cryo-gel fabrication techniques

Poly(vinyl alcohol) (PVA) is a synthetic, biocompatible polymer that has been widely studied for use in bioengineered tissue scaffolds due to its relatively high strength, creep resistance, water retention, and porous structure. However, PVA hydrogels traditionally exhibit low percent elongation and energy dissipation. PVA material and mechanical properties can be fine-tuned by controlling the physical, non-covalent crosslinks during hydrogel formation through various techniques; PVA scaffolds were modified with gelatin, a natural collagen derivative also capable of forming reversible hydrogen bonds. Blending in gelatin and poly(ethylene glycol) (PEG) with PVA prior to solidification formed a highly organized hydrogel with improved toughness and dynamic elasticity. Theta-gels were formed from the solidification of warm solutions and the phase separation of high molecular weight gelatin and PVA from a low molecular PEG porogen upon cooling. While PVA-gelatin hydrogels can be synthesized in this manner, the hydrogels exhibited low toughness with increased elasticity. Thus, theta-gels were additionally processed using cryo-gel fabrication techniques, which involved freezing theta-gels, lyophilizing and re-hydrating. The result was a stronger, more resilient material. We hypothesized that the increased formation of physical hydrogen bonds between the PVA and gelatin allowed for the combination of a stiffer material with energy dissipation characteristics. Rheological data suggested significant changes in the storage moduli of the new PVA-gelatin theta-cryo-gels. Elastic modulus, strain to failure, hysteresis and resilience were studied through uniaxial tension and dynamic mechanical analysis in compression.