Liquid-Free Covalent Reinforcement of Carbon Nanotube Dry-Spun Yarns and Free-Standing Sheets

Carbon nanotubes (CNTs) possess exceptional mechanical properties, surpassing stiffness and strength metrics of common materials such as steel alloys by 100× at the nanoscale. However, when myriads of individual CNTs are bundled together into macroscopic ensembles like fibers or sheets, the result is a 100-fold drop in strength compared to its individual components. Here we present a general strategy aimed to close this gap in property scaling. By using vapor-phase polymerization of a cross-linkable polymer, we reinforced the weak interlinkages among individual CNTs within both yarns and sheets to promote a better transference of mechanical load across the structure. After the treatment, dry-spun, low-density 2.3 μm thin yarns increased their elastic moduli by at least 300%, and free-standing CNT sheets exhibited a 10× boost. In-situ synchrotron small-angle X-ray scattering revealed that polymer-reinforced yarns undergo limited CNT bundle rearrangement when subjected to tensile loads compared to pristine yarns. This evidence supports the hypothesis that the polymer hinders CNTs slippage, the root cause of the poor scaling of mechanical properties in these materials. While we demonstrated this reinforcement method for CNT structures, it is not specific to CNTs and could be used to reinforce a wide variety of hierarchical nanostructured ensembles.