Green-process preparation and characterizations of optically transparent, thermally stable and mechanically superior regenerated silk-hyaluronate composite films

High-performance regenerated silk-hyaluronate composite films prepared by an environment-friendly process were highly desirable for medical dressing base material. In this study, sericin was removed from silk by steam treatment without using any chemical reagent, and a low concentration solution of Na2CO3 was used as a green process to dissolve silk fibers. Then the obtained silk fibroin was physically blended with sodium hyaluronate to generate optically transparent, thermally stable and mechanically superior regenerated silk-hyaluronate films. The results of structural characterizations and property tests showed that the insoluble silk short fibers prepared by the dissolution of Na2CO3 were dominated by a β-sheet crystalline structure while the soluble silk fibroins by an amorphous structure. Moreover, both insoluble silk short fibers and soluble silk fibroins could form uniform composite films with a low coefficient of thermal expansion after being blended with sodium hyaluronate, which were named as insoluble silk film (ISH) and soluble silk film (SSH), respectively. The tensile strength of ISH could reach 138.8 MPa and SSH reached 153.9 MPa, which were 65.7 % and 30.5 % higher than that of the commercial control insoluble fibroin film (83.8 MPa) and commercial control soluble fibroin film (117.9 MPa), and 173.2 % and 203.0 % higher than that of pure hyaluronate film (50.8 MPa), respectively. Also, ISH and SSH had a modulus higher than 3 GPa. In this study, the low-concentration Na2CO3 method provides a simple and green technique for the preparation of high performance silk-hyaluronate composite materials.