Identification of self-discharge mechanisms of ionic liquid electrolyte based supercapacitor under high-temperature operation

Ionic liquids (ILs) are promising electrolytes for supercapacitors (SCs) aimed for high-temperature applications, where increased ionic conductivity results in superior capacitive performance compared to room temperature (RT) performance. However, an increased temperature also accelerates the self-discharge rate that adversely affects energy retention and restricts the usage of SCs in standalone applications. In this study, a detailed electrochemical investigation on the self-discharge behaviour of carbon-based SCs containing an IL, 1-Ethyl-3-methylimidazolium acetate (EMIM Ac), has been carried out in the temperature range RT - 60 °C, and the underlying self-discharge mechanisms are identified. The results reveal that at a high voltage of 1.5 V, the self-discharge is characterized by a combination of charge redistribution and diffusion at both RT and 60 °C. At 60 °C, the diffusion-controlled mechanism dominates at lower voltages over the charge redistribution effect, while at RT both mechanisms contribute to a similar extent. The observed difference in the self-discharge mechanism between RT and 60 °C is explained in terms of a decreased RC time constant (τRC) at elevated temperature, and the same conclusions are potentially applicable to other IL-containing SCs as well.