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Graphene oxide (GO) with outstanding mechanical properties is a satisfactory filler to reinforce artificial silk. To prepare tough regenerated silk fibroin/graphene oxide (RSF/GO) hybrid fibers, it is important to understand the structural evolution of the hybrid fibers with external deformation. The morphology and microstructural changes of the hybrid fibers at different tensile strains were investigated by SEM, Raman spectra and synchrotron radiation wide angle X-ray diffraction (SR-WAXD). Longer and deeper stripes were found on the surface of RSF/GO fibers with the increase of strain as revealed by SEM. SR-WAXD results revealed that the fraction and orientation of crystals and the mesophase had slight changes in the elastic deformation zone of the fiber. However, in the plastic deformation zone of the fiber with a strain from 5 to 18%, the fraction of crystals gradually increased while the fraction of the mesophase decreased. During this deformation, the orientation of crystals (fc) firstly increased significantly and then increased slightly, while the orientation of the mesophase (fm) increased steadily beyond the yield point. When the strain exceeded 18%, the fraction of crystals decreased while the fraction of mesophase increased. The fc had a rapid increase again at a strain above 18%. A model was proposed to explain how the tensile deformation affects the molecular orientation of the hybrid fibers.

Microstructural evolution of regenerated silk fibroin/graphene oxide hybrid fibers under tensile deformation