Well-aligned macroscopic fibers composed solely of single-walled carbon nanotubes (SWNTs) were produced by conventional spinning. Fuming sulfuric acid charges SWNTs and promotes their ordering into an aligned phase of individual mobile SWNTs surrounded by acid anions. This ordered dispersion was extruded via solution spinning into continuous lengths of macroscopic neat SWNT fibers. Such fibers possess interesting structural composition and physical properties.

Translating the unique characteristics of individual single-walled carbon nanotubes into macroscopic materials such as fibres and sheets has been hindered by ineffective assembly. Fluid-phase assembly is particularly attractive, but the ability to dissolve nanotubes in solvents has eluded researchers for over a decade. Here, we show that single-walled nanotubes form true thermodynamic solutions in superacids, and report the full phase diagram, allowing the rational design of fluid-phase assembly processes. Single-walled nanotubes dissolve spontaneously in chlorosulphonic acid at weight concentrations of up to 0.5 wt%, 1,000 times higher than previously reported in other acids. At higher concentrations, they form liquid-crystal phases that can be readily processed into fibres and sheets of controlled morphology. These results lay the foundation for bottom-up assembly of nanotubes and nanorods into functional materials.

Graphene combines unique electronic properties and surprising quantum effects with outstanding thermal and mechanical properties. Many potential applications, including electronics and nanocomposites, require that graphene be dispersed and processed in a fluid phase. Here, we show that graphite spontaneously exfoliates into single-layer graphene in chlorosulphonic acid, and dissolves at isotropic concentrations as high as approximately 2 mg ml(-1), which is an order of magnitude higher than previously reported values. This occurs without the need for covalent functionalization, surfactant stabilization, or sonication, which can compromise the properties of graphene or reduce flake size. We also report spontaneous formation of liquid-crystalline phases at high concentrations ( approximately 20-30 mg ml(-1)). Transparent, conducting films are produced from these dispersions at 1,000 Omega square(-1) and approximately 80% transparency. High-concentration solutions, both isotropic and liquid crystalline, could be particularly useful for making flexible electronics as well as multifunctional fibres.

Single-walled carbon nanotubes (SWNTs) can be dispersed at high concentration in superacids; the protonation of SWNTs sidewalls eliminates wall-wall van der Waals interactions and promotes the dispersion process. At very low concentration, SWNTs in superacids dissolve as individual tubes which behave as Brownian rods. At higher concentration, SWNTs form a highly unusual nematic phase consisting of spaghetti-like self-assembled supermolecular strands of mobile, solvated tubes in equilibrium with a dilute isotropic phase. At even higher concentration, the spaghetti strands self-assemble into a polydomain nematic liquid crystal. Upon the introduction of small amounts of water, the liquid crystal phase separates into needle-shaped strands (∼20 µm long) of highly aligned SWNTs, termed alewives. Under anhydrous condition, the liquid crystalline phase can be processed into highly aligned fibers of pure SWNT without the aid of any surfactants or polymers.