A Polymerized-Ionic-Liquid-Based Polymer Electrolyte for >4 V Class Solid-State Lithium Metal Batteries

Wednesday, 12 October 2022: 12:00
Galleria 4 (The Hilton Atlanta)
C. Fu, G. Homann, R. Grissa, D. Rentsch, W. Zhao (Empa), T. Gouveia, A. Falgayrat, R. Lin, S. Fantini (Solvionic), and C. Battaglia (Empa)
Polymer solid electrolytes for solid-state batteries typically suffer from low ionic conductivity and low oxidative stability. We report a polymer electrolyte based on a polymerized ionic liquid and an ionic liquid plasticizer offering simultaneously a high room-temperature ionic conductivity of 0.8 mS cm-1 and a high oxidative stability > 5.0 V vs Li+/Li. The electrolyte is compatible with lithium metal, exhibits high thermal stability up to 300 °C, is non-flammable upon direct flame exposure, shows decent lithium-ion transference number of 0.44, and possesses a low gravimetric density of only 1.6 g cm-3, important when targeting batteries with high gravimetric energy density. In symmetric lithium metal cells, the electrolyte enables stable lithium plating and stripping at 0.1 mA cm−2 with a capacity of 1 mAh cm−2 per half cycle for over 1700 h at 25 °C. Cells with a lithium metal anode cycled against a state-of-the-art high-energy uncoated layered LiNi0.8Mn0.1Co0.1O2 cathode achieve an initial capacity of 162 mA h g-1 and a capacity retention of 72% after 600 cycles to an upper cut-off voltage of 4.4 V at 0.1 mA cm-2 and 25 °C. Cells with a high-voltage spinel LiMn1.5Ni0.5O4 cathode reach an initial capacity of 132 mAh g-1 and a capacity retention of 76% after 300 cycles to an upper cut-off voltage of 5 V at 0.1 mA cm-2 and 25 °C, confirming the high oxidative stability and technological potential of this electrolyte for high-voltage solid-state lithium metal batteries.