An ionic liquid- and PEO-based ternary polymer electrolyte for lithium metal batteries: an advanced processing solvent-free approach for solid electrolyte processing.

A processing solvent-free manufacturing process for cross-linked ternary solid polymer electrolytes (TSPEs) is presented. Ternary electrolytes (PEODA, Pyr14TFSI, LiTFSI) with high ionic conductivities of >1 mS cm-1 are obtained. It is shown that an increased LiTFSI content in the formulation (10 wt% to 30 wt%) decreases the risk of short-circuits by HSAL significantly. The practical areal capacity increases by more than a factor of 20 from 0.42 mA h cm-2 to 8.80 mA h cm-2 before a short-circuit occurs. With increasing Pyr14TFSI content, the temperature dependency of the ionic conductivity changes from Vogel-Fulcher-Tammann to Arrhenius behavior, leading to activation energies for the ion conduction of 0.23 eV. In addition, high Coulombic efficiencies of 93% in Cu‖Li cells and limiting current densities of 0.46 mA cm-2 in Li‖Li cells were obtained. Due to a temperature stability of >300 °C the electrolyte guarantees high safety in a broad window of conditions. In LFP‖Li cells, a high discharge capacity of 150 mA h g-1 after 100 cycles at 60 °C was achieved.