Capacitance properties of multi-walled carbon nanotubes modified by activation and ammoxidation

Catalytic multi-walled carbon nanotubes were modified by KOH activation at 800 °C and/or ammoxidation at 350 °C, and the effect of these treatments on the physicochemical and electrochemical properties was investigated. Whereas texture is moderately changed by ammoxidation, the chemical composition is significantly modified due to the formation of various nitrogen containing groups. The influence of nitrogenated functionality (pyridine, pyridone, NH) on charge accumulation is considered in full electrochemical capacitors, as well as in positive and negative electrodes separately, using acidic (4 mol L−1 H2SO4) and alkaline (7 mol L−1 KOH) electrolytes. The presence of nitrogen in the carbon network, especially in the form of pyridone/pyrrolic (N5) and/or pyridine (N6) groups, affects the electron density and enhances the charge affinity of the carbon material. It seems that the nitrogen groups improve particularly the capacitance performance of the negative electrode operating in alkaline medium. Besides the nitrogenated groups, the oxygenated functionality plays also an important role for the ammoxidized nanotubes. Generally, a few-fold increase of capacitance was observed in the N-enriched carbon nanotubular samples. Apart of this capacitance improvement, the presence of nitrogen in the carbon network limits significantly the leakage current and diminishes the self-discharge of supercapacitors.