In Situ Raman Study of Voltage Tolerance Up to 2.2 V of Ionic Liquid Analogue Supercapacitor Electrolytes Immune to Water Adsorption Conferred by Amphoteric Imidazole Additives

Ionic liquid analogues (ILAs) are promising electrolytes for supercapacitors due to their low cost and considerable voltage (>2.0 V). However, the voltage is <1.1 V for wateradsorbed ILAs. Herein for the first time, an amphoteric imidazole (IMZ) additive is reported to address this concern by reconfiguring the solvent shell of ILAs. Addition of only 2 wt % IMZ increases the voltage from 1.1 to 2.2 V, with an increase in capacitance from 178 to 211 F g(-1) and an increase in energy density from 6.8 to 32.6 Wh kg(-1). In situ Raman reveals that the strong H-bonds formed by IMZ with completive ligands 1,3-propanediol and water induce a reversal of the polarity of the solvent shells, suppressing absorbed water electrochemical activity and thus increasing the voltage. This study solves the problem of low voltage for water-adsorbed ILAs and reduces the equipment cost of ILA-based supercapacitor assembly (e.g., assembly in air without a glovebox).