Regenerated silk fibroin (SF) fiber is a multifaceted protein matrix suitable for engineering a wide variety of biological materials. Numerous artificial spinning systems have been developed to mimic the molecular structure and hierarchical properties found in native silks. Here, we show a bioinspired technique that can readily form nanofibers and induce both orientation and structure formation of crystalline β-sheet assemblies seen in natural silk. In this study, electrospun postdrawn SF nanofibers were fabricated using an automated track-drawing (TD) approach for the continuous production of highly aligned protein nanofibers. This one-step postdrawing process simulates the dominant pulling force seen in natural spinning. The mechanical performance of the postdrawn SF nanofibers with a draw ratio of 2 (DR2) via TD exhibited a 115% increase in Young's modulus and an 80% increase in ultimate tensile strength, compared with the undrawn SF fibers after water treatment. It was also determined that the intermolecular β-sheet content in DR2 nanofibers increased by 75%. This contribution led to higher glass-transition and degradation temperatures. These biomimetic fibers with structural hierarchy and mechanical properties may be used to build high-performance load-bearing and directionally propagating structures relevant in biomaterial and sustainable material applications.
Keywords: electrospinning; fibroin; nanofiber; postdrawing; silk; β-sheet.