Self-discharge of supercapacitors based on carbon nanotubes with different diameters

The self-discharge of supercapacitors was investigated using electrodes composed of multiwalled carbon nanotubes (MWCNTs) of three different diameters: 20, 30, and 50 nm, respectively. A combined self-discharge mechanism including both ohmic leakage and diffusion-controlled faradaic reaction was employed to fit the open circuit voltage (OCV) decays of the supercapacitors. The existence of both large inter-bundle pores and small intra-bundle pores in the MWCNT electrodes led to a two-stage diffusion-controlled faradaic reaction process - while the first stage can be described as a divided diffusion-controlled (DDC) process due to the diffusion of ions from both inter- and intra-bundle pores, and the second stage corresponds to a single diffusion-controlled (SDC) process mainly due to the diffusion of ions from the intra-bundle pores. The diffusion parameters obtained based on this model were consistent with the measured self-discharge rates which increased with the size of the MWCNTs. The results of this work demonstrate that electrode materials with wide pore size distributions may be associated with more complex self-discharge processes.