Outstanding pristine properties of carbon nanotubes and graphene have limited the scope for real-life applications without precise controllability of the material structures and properties. This invited article to celebrate the 25th anniversary of Advanced Materials reviews the current research status in the chemical modification/doping of carbon nanotubes and graphene and their relevant applications with optimized structures and properties. A broad aspect of specific correlations between chemical modification/doping schemes of the graphitic carbons with their novel tunable material properties is summarized. An overview of the practical benefits from chemical modification/doping, including the controllability of electronic energy level, charge carrier density, surface energy and surface reactivity for diverse advanced applications is presented, namely flexible electronics/optoelectronics, energy conversion/storage, nanocomposites, and environmental remediation, with a particular emphasis on their optimized interfacial structures and properties. Future research direction is also proposed to surpass existing technological bottlenecks and realize idealized graphitic carbon applications.

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Graphene oxide (GO) is aqueous-dispersible oxygenated graphene, which shows colloidal discotic liquid crystallinity. Many properties of GO-based materials, including electrical conductivity and mechanical properties, are limited by the small flake size of GO. Unfortunately, typical sonochemical exfoliation of GO from graphite generally leads to a broad size and shape distribution. Here, we introduce a facile size selection of large-size GO exploiting liquid crystallinity and investigate the size-dependent N-doping and oxygen reduction catalysis. In the biphasic GO dispersion where both isotropic and liquid crystalline phases are equilibrated, large-size GO flakes (>20 μm) are spontaneously concentrated within the liquid crystalline phase. N-Doping and reduction of the size-selected GO exhibit that N-dopant type is highly dependent on GO flake size. Large-size GO demonstrates quaternary dominant N-doping and the lowest onset potential (-0.08 V) for oxygen reduction catalysis, signifying that quaternary N-dopants serve as principal catalytic sites in N-doped graphene.

N-doped sites at CNT and graphene trigger spontaneous encapsulation of Si particles by simple pH control at room temperature. Significantly, N-doped CNT encapsulated Si composite electrode materials show remarkable cycle life and rate performance in battery operations. Superior capacity retention of 79.4% is obtained after 200 cycles and excellent rate capability of 914 mA h g À1 is observed at a 10 C rate.