Protein-based biomaterials with innovative and controlled performance are being sought due to their unique characteristics for use in biomedical fields such as neural implants, drug delivery systems, cellbased therapies and soft tissue engineering. Here, we present a versatile approach for the synthesis of photo-crosslinkable fibroin silk biomaterial with highly tunable mechanical, chemical and biodegradation properties. Unlike the crystalline rich silk fibroin reported previously, the covalently crosslinked fibroin protein photoresist (FPP) via controlled light-induced radical grafting, allows generating a new amorphous biomaterial with tunable properties. It appears that the use of photoreactive acrylate groups to cross-link FPP induces plasticity that can be tuned by changing the photoinitiator concentration of the film. Tensile strength measurements revealed that elasticity was higher for FPP UV-cross-linked materials with higher concentration of photoinitiator. FTIR and relative humidity measurements showed that hydrophilicity was higher for UV-cross-linked FPP. These materials display stiffness between 0.01-1.5 GPa and tensile strains up to 60%, covering a significant portion of the properties of native soft biomaterials. Besides, in vitro proteolytic degradation of the photocrosslinked FPP films demonstrate a tunable degradation rate over a period ranging from hours to weeks. Those biomaterials have been successfully micropatterned by photolithography techniques across several orders of magnitude (μm to cm) and a systematic study of direct patterning of the fibroin protein to form high fidelity and high-resolution structures has been reported. It was also shown that the fabricated protein features are well suited to cell adhesion. The development of protein-based material with controlled and tunable elasticity that can be easily photopatterned into centimeter, micrometer and nanometer components will allow a wide range of applications in biomedical fields requesting a natural functional tissue.
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