Molecular Insights into Carbon Nanotube Supercapacitors: Capacitance Independent of Voltage and Temperature

Molecular dynamics (MD) simulations of supercapacitors with single-walled carbon nanotube (SWCNT) electrodes in room-temperature ionic liquids were performed to investigate the influences of the applied electrical potential, the radius/curvature of SWCNTs, and temperature on their capacitive behavior. It is found that (1) SWCNTs-based supercapacitors exhibit a near-flat capacitance-potential curve, (2) the capacitance increases as the tube radius decreases, and (3) the capacitance depends little on the temperature. We report the first MD study showing the influence of the electrode curvature on the capacitance-potential curve and negligible dependence of temperature on capacitance of tubular electrode. The latter is in good agreement with recent experimental findings and is attributed to the similarity of the electrical double layer (EDL) microstructure with temperature varying from 260 to 400 K. The electrode curvature effect is explained by the dominance of charge overscreening and increased ion density per unit area of electrode surface.