Controllable bulk growth of few-layer graphene/single-walled carbon nanotube hybrids containing Fe@C nanoparticles in a fluidized bed reactor

A family of layered double hydroxides (LDHs) with varied Fe contents were employed as catalyst precursors for the controllable bulk growth of few-layer graphene/single-walled carbon nanotube (G/SWCNT) hybrids in a fluidized-bed reactor through chemical vapor deposition of methane at 950 °C. All the G/SWCNT hybrids exhibited the morphology of SWCNTs interlinked with graphene layers. The purity, thermal stability, graphitization degree, specific surface area, and total pore volume of the G/SWCNT hybrids decreased with the increasing Fe contents in the LDH precursors. A high yield of 0.97 gG/SWCNTs/gcat can be achieved by tuning the Fe content in the FeMgAl LDHs after a 15-min growth. After the removal of the as-calcined FeMgAl layered double oxide flakes, a high carbon purity of ca. 98.3% for G/SWCNT hybrids was achieved when the mole ratio of Fe–Al is 0.05:1. The size and density of Fe nanoparticles decorated in the as-obtained G/SWCNT hybrids depend largely on Fe content in the FeMgAl LDH precursors. Furthermore, the mass ratio of graphene materials to SWCNTs in the as-prepared G/SWCNT hybrids can be well controlled in a range of 0.4–15.1.