Quantification of Carbon Nanotube Liquid Crystal Morphology via Neutron Scattering

Liquid phase assembly is among the most industrially attractive routes for scalable carbon nanotube (CNT) processing. Chlorosulfonic acid (CSA) is known to be an ideal solvent for CNTs, spontaneously dissolving them without compromising their properties. At typical processing concentrations, CNTs form liquid crystals in CSA; however, the morphology of these phases and their concentration dependence are only qualitatively understood. Here, we use small-angle neutron scattering (SANS), combined with polarized light microscopy and cryogenic transmission electron microscopy to study solution morphology over a range of concentrations and two different CNT lengths. Our results show that at the highest concentration studied the long CNTs form a highly ordered fully nematic phase, while short CNTs remain in a biphasic regime. Upon dilution, long CNTs undergo a 2D lattice expansion, whereas short CNTs seem to have an intermediate expansion between 2D and 3D probably due to the biphasic nature of the system. The average spacing between the CNTs scaled by the CNT diameter is the same in both systems, as expected for infinitely long aligned rods.