Preparation of Nitrogen-Doped Carbon Nanotubes with Different Morphologies from Melamine-Formaldehyde Resin

We report a facile method for the synthesis of nitrogen-doped carbon nanotubes (NCNTs) from melamine-formaldehyde (MR) resin using FeCl3 or supported FeCl3 as catalysts. The growth of NCNTs follows a decomposition-reconstruction mechanism, in which the polymer precursor would totally gasify during pyrolysis process and then transformed into carbon nanotubes. The morphology of the NCNTs could be adjusted via applying different catalyst supports and three kinds of carbon nanotubes with outer-diameter of 20-200 nm and morphologies of either bamboo-like or hollow interiors were obtained. Nitrogen atoms in the materials were mainly in the form of pyridinic and quaternary form while the formation of iron species strongly depended on the interaction between iron precursor and organic carbon/nitrogen sources. All MR resin derived NCNTs are efficient toward oxygen reduction reaction (ORR). NCNTs prepared using FeCl3 as catalyst showed the highest ORR activity with half-wave potentials of -0.17 V, which is comparable with commercial Pt/C. This is probably because of a close contact between MR resin and iron precursor could enhance the iron-ligand coordination strength and thus steadily improve the performance of the catalyst.