Controlled Structural Relaxation of Aramid Nanofibers for Superstretchable Polymer Fibers with High Toughness and Heat Resistance

Polymer fibers that combine high toughness and heat resistance are hard to achieve, which, however, hold tremendous promise in demanding applications such as aerospace and military. This prohibitive design task exists due to the opposing property dependencies on chain dynamics because traditional heat-resistant materials with rigid molecular structures typically lack the mechanism of energy dissipation. Aramid nanofibers have received great attention as high-performance nanoscale building units due to their intriguing mechanical and thermal properties, but their distinct structural features are yet to be fully captured. We show that aramid nanofibers form nanoscale crimps during the removal of water, which primarily resides at the defect planes of pleated sheets, where the folding can occur. The precise control of such a structural relaxation can be realized by exerting axial loadings on hydrogel fibers, which allows the emergence of aramid fibers with varying angles of crimps. These crimped fibers integrate high toughness with heat resistance, thanks to the extensible nature of nanoscale crimps with rigid molecular structures of poly(