Unveil Overcharge Performances of Activated Carbon Cathode in Various Li-Ion Electrolytes

Typically, the practical lithium-ion capacitor (LIC) is composed of a capacitive cathode (activated carbon, AC) and a battery-type anode (graphite, soft carbon, hard carbon). There is a risk of the LIC cell overcharging to an unsafe voltage under electrical abuse conditions. Since the anode potential is usually quite low during the charging process and can be controlled by adjusting the amount of anode materials, the overcharge performances of LIC full-cell mainly depend on the AC cathode. Thus, it is necessary to independently investigate the overcharge behaviors of the AC cathode in nonaqueous Li-ion electrolytes without the interference of the anode electrode. In this work, the stable upper potential limits of the AC electrode in three types of lithium-ion electrolytes were determined to be 4.0−4.1 V via the energy efficiency method. Then, the AC//Li half-cells were charged to 5.0 V and 10.0 V, respectively, to investigate the overcharge behaviors. For the half-cells with propylene carbonate (PC)-based electrolytes, the voltage increased sharply to 10.0 V with a vertical straight line at the end of the overcharging process, indicating that the deposits of electrolyte decomposition had separated the AC electrode surface from the electrolytes, forming a self-protective passivation film with a dielectric capacitor behavior. The dense and compact passivation film is significant in separating the AC electrode surface from the electrolytes and preventing LIC cells from volume expansion and explosion risks under electrical abuse and overcharging conditions.