Self-regenerated silk fibroin with controlled crystallinity for the reinforcement of silk

Hypothesis: Silk artifacts constitute a fundamental cultural and historical heritage, yet they are affected by degradation that alters the secondary structure of fibroin and weakens the mechanical properties of textiles, hindering their conservation. Feasible and compatible consolidants for silk are still widely needed. Experiments: Here, we propose a robust and reliable method to restore the mechanical properties of fragile, aged silk fibers, based on the adhesion of self-regenerated silk fibroin (SRSF) with controlled crystallinity, prepared from waste silk, to the aged fibers. By varying the concentration of fibroin dispersions, the content of crystalline and amorphous domains in SRSF films can be tuned, as demonstrated by 2D micro-Fourier transform infrared spectroscopy Imaging and thermal analysis. Findings: The presence of amorphous fibroin domains, distributed between the aged silk fibers, completely recovered their mechanical properties. Instead, the presence of domains with high content of ordered structures, distributed between the fibers, reduced their tensile strength and elongation length. The different mechanical behavior is likely due to the fact that adhesion of crystalline layers produces a brittle material, while amorphous layers with higher fibroin chain mobility increase ductility. The tunability of this treatment allows easy control of desired mechanical properties of degraded silk fibers, simply controlling the crystallinity Vs amorphousness of SRSF; these findings open up new perspectives in textile conservation, in the engineering of biomaterials and materials, and in the preparation of composite materials with enhanced properties.