In this Account we highlight the experimental evidence in favor of our view that carbon nanotubes should be considered as a new macromolecular form of carbon with unique properties and with great potential for practical applications. We show that carbon nanotubes may take on properties that are normally associated with molecular species, such as solubility in organic solvents, solutionbased chemical transformations, chromatography, and spectroscopy. It is already clear that the nascent field of nanotube chemistry will rival that of the fullerenes.

The addition of nitrophenyl groups to the surface of few-layer epitaxial graphene (EG) by the formation of covalent carbon-carbon bonds changed the electronic structure and transport properties of the EG from near-metallic to semiconducting.

Covalent derivatization of the acidic functional groups in oxidized graphite with octadecylamine renders graphite soluble in common organic solvents. Atomic force microscopic characterization of the soluble species supports the idea that the solutions consist of single and few layer graphene sheets, and we report the first solution properties of graphite.

Natural graphite was intercalated, thermally exfoliated, and dispersed in acetone to prepare graphite nanoplatelets (GNPs, G n ) of controlled aspect ratio. Thermal conductivity measurements indicate that few graphene layer G n , where n ∼ 4, with a thickness of ∼2 nm function as a very efficient filler for epoxy composites. When embedded in an epoxy matrix, the G4 GNPs provide a thermal conductivity enhancement of more than 3000% (loading of ∼25 vol %), and a thermal conductivity κ = 6.44 W/mK, which surpasses the performance of conventional fillers that require a loading of ∼70 vol % to achieve these values. We attribute the outstanding thermal properties of this material to a favorable combination of the high aspect ratio, two-dimensional geometry, stiffness, and low thermal interface resistance of the GNPs.