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.

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.

Strong tube-tube van der Waal attractions that hinder the dissolution of single walled carbon nanotubes (SWNTs) as individuals have been overcome by the direct protonation of the tubes by superacids. The pristine nanotubes disperse as individuals in 100% H 2 SO 4 , oleum, trifluromethanesulfonic acid, and chlorosulfonic acid to varying solubility levels. Optically homogeneous solutions with concentration as high as 45 g/L (2.5 wt %) at room temperature have been observed in the case of chlorosulfonic acid, the strongest among the series of superacids investigated. A dissolution model is proposed wherein the solubilized tubes exist as protonated polycarbocations, charge balanced by corresponding conjugate base anions. The removal of electrons from the SWNT, leading to a fractional positive charge on the carbons in the protonated state, is reversible upon deprotonation. With increasing concentration of the solubilized nanotubes, anion-mediated attractions at lower concentrations and spatial constraints at high concentrations guide the transformation of the SWNTacid system into a nematic mesophase. Highly anisotropic, nematic mesophases formed in the dissolution process are promising precursors for the fabrication of macroscopic forms of SWNTs with high alignment of the carbon nanotubes.