Development of low-viscosity phosphonium-based ionic liquid electrolytes for lithium-ion batteries: Charge-discharge performance and ionic transport properties

Phosphonium cation-based ionic liquids (phosphonium ILs) have several advantages for electrochemical device applications compared with ammonium cation-based ionic liquids because of their unique features, such as higher ionic conductivity and a larger electrochemical potential window. In this study, we prepared various phosphonium ILs with different substituents (alkyl, alkyl ether, or allyl) on the cation, and bis(fluorosulfonyl)amide (FSA) or bis(trifluoromethanesulfonyl)amide (TFSA) as the anion. This study describes these phosphonium ILs used as electrolytes for lithium-ion batteries and investigates their performance as typical Li/LiCoO2 cells. We demonstrate that discharge capacity increases with increasing lithium-ion conductivity determined by electrochemical impedance and pulsed-field gradient nuclear magnetic resonance. A discharging rate test conducted in constant current (CC) mode also displays good high conductivity phosphonium IL electrolyte performance. Furthermore, the difference in cycle performance between FSA-based and TFSA-based phosphonium IL electrolytes is explained in terms of solid electrolyte interphase formation, similar to the performance of other cation-based ILs.