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Soft thermoplastic polysiloxane-urea-elastomers (PSUs) were prepared for the application as a biomaterial to replace the human natural lens after cataract surgery. PSUs were synthesized from amino-terminated polydimethylsiloxanes (PDMS), 4,4′-Methylenebis(cyclohexylisocyanate) (H12MDI) and 1,3–Bis(3-aminopropyl)-1,1,3,3–tetramethyldisiloxane (APTMDS) by a two-step polyaddition route. Such a material has to be highly transparent and must exhibit a low Young’s Modulus and excellent dimensional stability. Polydimethylsiloxanes in the range of 3000–33,000 g·mol−1 were therefore prepared by ring-chain-equilibration of octamethylcyclotetrasiloxane (D4) and APTMDS in order to study the influence of the soft segment molecular weight on the mechanical properties and the transparency of the PSU-elastomers. 2,4,6,8-Tetramethyl-2,4,6,8-tetraphenylcyclotetrasiloxane (D4Me,Ph) was co-polymerized with D4 in order to adjust the refractive index of the polydimethyl-methyl-phenyl-siloxane-copolymers to a value equivalent to a young human natural lens. Very elastic PSUs with Elongation at Break values higher than 700% were prepared. PSU-elastomers, synthesized from PDMS of molecular weights up to 18,000 g·mol−1, showed transmittance values of over 90% within the visible spectrum range. The soft segment refractive index was increased through the incorporation of 14 mol % of methyl-phenyl-siloxane from 1.4011 to 1.4346 (37 °C). Young’s Moduli of PSU-elastomers were around 1 MPa and lower at PDMS molecular weights up to 15,000 g·mol−1. 10-cycle hysteresis measurements were applied to evaluate the mechanical stability of the PSUs at repeated stress. Hysteresis values at 100% strain decreased from 32 to 2% (10th cycle) with increasing PDMS molecular weight. Furthermore, hysteresis at 5% strain was only detected in PSU-elastomers with low PDMS molecular weights. Finally, preliminary results of in vitro cytotoxicity tests on a PSU-elastomer showed no toxic effects on HaCaT-cells.
Though bioprinting is a forward-looking approach in bone tissue engineering, the development of bioinks which are on the one hand processable with the chosen printing technique, and on the other hand possess the relevant mechanical as well as osteoconductive features remains a challenge. In the present study, polymer solutions based on methacrylated gelatin and methacrylated hyaluronic acid modified with hydroxyapatite (HAp) particles (5 wt%) were prepared. Encapsulation of primary human adipose derived stem cells in the HAp-containing gels and culture for 28 d resulted in a storage moduli significantly increased to 126% ± 9.6% compared to the value on day 1 by the sole influence of the HAp. Additional use of osteogenic media components resulted in an increase of storage module up to 199% ± 27.8%. Similarly, the loss moduli was increased to 370% ± 122.1% under the influence of osteogenic media components and HAp. Those changes in rheological material characteristics indicate a distinct change in elastic and viscous hydrogel properties, and are attributed to extensive matrix production in the hydrogels by the encapsulated cells, what could also be proven by staining of bone matrix components like collagen I, fibronectin, alkaline phosphatase and osteopontin. When using the cell-laden polymer solutions as bioinks to build up relevant geometries, the ink showed excellent printability and the printed grid structure's integrity remained intact over a culture time of 28 d. Again, an intense matrix formation as well as upregulation of osteogenic markers by the encapsulated cells could be shown. In conclusion, we demonstrated that our HAp-containing bioinks and hydrogels on basis of methacrylated gelatin and hyaluronic acid are on the one hand highly suitable for the build up of relevant three-dimensional geometries with microextrusion bioprinting, and on the other hand exhibit a significant positive effect on bone matrix development and remodeling in the hydrogels, as indicated by rheological measurements and staining of bone components. This makes the developed composite hydrogels an excellent material for bone bioprinting approaches.