The theoretically proposed graphene/single-walled carbon nanotube (G/SWCNT) hybrids by placing SWCNTs among graphene planes through covalent C-C bonding are expected to have extraordinary physical properties and promising engineering applications. However, the G/CNT hybrids that have been fabricated differ greatly from the proposed G/SWCNT hybrids because either the covalent C-C bonding is not well constructed or only multiwalled CNTs/carbon nanofibers rather than SWCNTs are available in the hybrids. Herein, a novel G/SWCNT hybrid was successfully fabricated by a facile catalytic growth on layered double hydroxide (LDH) at a high temperature over 950 °C. The thermally stable Fe nanoparticles and the uniform structure of the calcined LDH flakes are essential for the simultaneously catalytic deposition of SWCNTs and graphene. The SWCNTs and the CVD-grown graphene, as well as the robust connection between the SWCNTs and graphene, facilitated the construction of a high electrical conductive pathway. The internal spaces between the two stacked graphene layers and among SWCNTs offer room for sulfur storage. Therefore, the as obtained G/SWCNT-S cathode exhibited excellent performance in Li-S batteries with a capacity as high as 650 mAh g(-1) after 100 cycles even at a high current rate of 5 C. Such a novel G/SWCNT hybrid can serve not only as a prototype to shed light on the chemical principle of G/CNT synthesis but also as a platform for their further applications in the area of nanocomposites, heterogeneous catalysis, drug delivery, electrochemical energy storage, and so on.

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Hollow nanostructures afford intriguing structural features ranging from large surface area and fully exposed active sites to kinetically favorable mass transportation and tunable surface permeability. The unique properties and potential applications of graphene nanoshells with well-defined small cavities and delicately designed graphene shells are strongly considered. Herein, a mesoscale approach to fabricate graphene nanoshells with a single or few graphene layers and quite small diameters through a catalytic self-limited assembly of nanographene on in situ formed nanoparticles was proposed. The graphene nanoshells with a diameter of ca. 10-30 nm and a pore volume of 1.98 cm(3) g(-1) were employed as hosts to accommodate the sulfur for high-rate lithium-sulfur batteries. A very high initial discharge capacity of 1520 mAh g(-1), corresponding to 91% sulfur utilization rate at 0.1 C, was achieved on a graphene nanoshell/sulfur composite with 62 wt % loading. A very high retention of 70% was maintained when the current density increased from 0.1 C to 2.0 C, and an ultraslow decay rate of 0.06% per cycle during 1000 cycles was detected.