Graphene/single-walled carbon nanotube hybrids: One-step catalytic growth and applications for high-rate Li-S batteries

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.