Shape and Phase Controlled Synthesis of Mesostructured Carbon Single Crystals through Mesoscale Self-Assembly of Reactive Monomicelles and their Unprecedented Exfoliation into Single-Layered Carbon Nanoribbons

Abstract The formation of mesostructured polymer and carbon single-crystals is very difficult due to increased complexity of the energy hypersurface and the role of slowed-down kinetics. Here we reported the synthesis of ordered mesostructured phloroglucinol-formaldehyde single crystals through mesoscale self-assembly of reactive monomicelles under acidic conditions which were traditionally thought very difficult to control the morphology because of the rapid polymerization rate. Polymeric and carbon single crystals from unusual curved hexagonal rods and spindles with two-dimensional hexagonal mesostructures, to previously unreported lozenge single-crystal sheets with lamellar mesostructures were obtained. Contrary to the literature reports, the lamellar mesostructured lozenge single-crystal sheets were successfully transformed to graphene-like layered carbons after calcination under 800 °C, and they can be further exfoliated into unprecedented high-quality single-layered carbon nanoribbons. These results unambiguously expanded our understanding about mesocrystals, and opened up new avenues for the efficient production of single-layered carbon nanoribbons which possess promising applications in electrochemical devices.