An investigation of carbon nanotubes obtained from the decomposition of methane over reduced Mg1-xMxAl2O4 spinel catalysts

Carbon nanotubes produced by the treatment of Mg1-x,MxAl2O4 (M = Fe, Co, or Ni; r = 0.1, 0.2, 0.3, or 0.4) spinels with an H-2-CH4 mixture at 1070 degrees C have been investigated systematically. The grains of the oxide-metal composite particles are uniformly covered by a weblike network of carbon nanotube bundles, several tens of micrometers long, made up of single-wall nanotubes with a diameter close to 4 nm. Only the smallest metal particles (< 5 nm) are involved in the formation of the nanotubes. A macroscopic characterization method involving surface area measurements and chemical analysis has been developed in order to compare the different nanotube specimens. An increase in the transition metal content of the catalyst yields more carbon nanotubes (up to a metal content of 10.0 wt% or x = 0.3), but causes a decrease in carbon quality. The best compromise is to use 6.7 wt% of metal (r = 0.2) in the catalyst, Co gives superior results with respect to both the quantity and quality of the nanotubes. In the case of Fe, the quality is notably hampered by the formation of Fe3C particles.