The integration of carbon nanotubes (CNT) and graphene with covalently bonded junctions is of great significance to inherit the outstanding properties of each component and obtain additional advantages afforded by the multiscale structures, but still in its infancy. Here we report the fabrication of covalently bonded graphene/CNT (G/CNT) structures by a facial thermal chemical vapor deposition method. Specifically, the defective carbon on the sidewall of CNTs can serve as nucleation sites for vertical growth of graphene to form a branch-leaf structure. This growth strategy can be used to grow graphene in CNT powders, films, sponges and arrays to obtain multiscale G/CNT hybrids. Due to the advantage of the covalently bonded structure, the as-synthesized G/CNT structure exhibit high electrical conductivity, large specific surface area and excellent anti-agglomeration properties. Naturally, G/CNT are expected as promising platform for electrocatalysis, in which electrons can be quickly transferred from the conductive network of CNTs to graphene through the covalently bonded junctions, and graphene increases the exposure of surface area for mass transport and charge transfer in electrolyte. As a proof of concept, G/CNT were applied as substrate to disperse iron species as oxygen electrocatalyst, which exhibited higher activity and durability than commercial noble-metal catalysts. These multiscale G/CNT hybrids are also highly promising for other energy and environmental applications.

Covalently bonded graphene-carbon nanotube hybrids

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