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.

We report a remarkably rapid method for assembling pristine graphene platelets into a large area transparent film at a liquid surface. Some 2-3 layer pristine graphene platelets temporally solvated with N-methyl-2-pyrrolidone (NMP) are assembled at the surface of a dilute aqueous suspension using an evaporation-driven Rayleigh-Taylor instability and then are driven together by Marangoni forces. The platelets are fixed through physical binding of their edges. Typically, 8-cm-diameter circular graphene films are generated within two minutes. Once formed, the films can be transferred onto various substrates with flat or textured topologies. This interfacial assembly protocol is generally applicable to other nanomaterials, including 0D fullerene and 1D carbon nanotubes, which commonly suffer from limited solution compatibility.

Flexible thin-film sensors have been developed for practical uses in invasive or noninvasive cost-effective healthcare devices, which requires high sensitivity, stretchability, biocompatibility, skin/organ-conformity, and often transparency. Graphene nanoplatelets can be spontaneously assembled into transparent and conductive ultrathin coatings on micropatterned surfaces or planar substrates via a convective Marangoni force in a highly controlled manner. Based on this versatile graphene assembled film preparation, a thin, stretchable and skin-conformal sensor array (144 pixels) is fabricated having microtopography-guided, graphene-based, conductive patterns embedded without any complicated processes. The electrically controlled sensor array for mapping spatial distributions (144 pixels) shows high sensitivity (maximum gauge factor ≈1697), skin-like stretchability (<48%), high cyclic stability or durability (over 10 cycles), and the signal amplification (≈5.25 times) via structure-assisted intimate-contacts between the device and rough skin. Furthermore, given the thin-film programmable architecture and mechanical deformability of the sensor, a human skin-conformal sensor is demonstrated with a wireless transmitter for expeditious diagnosis of cardiovascular and cardiac illnesses, which is capable of monitoring various amplified pulse-waveforms and evolved into a mechanical/thermal-sensitive electric rubber-balloon and an electronic blood-vessel. The microtopography-guided and self-assembled conductive patterns offer highly promising methodology and tool for next-generation biomedical devices and various flexible/stretchable (wearable) devices.

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