A Polymer-in-Salt Electrolyte with Enhanced Oxidative Stability for Lithium Metal Polymer Batteries

The lithium (Li) metal polymer battery (LMPB) is a promising candidate for solid-state batteries with high safety. However, high voltage stability of such a battery has been hindered by the use of polyethylene oxide (PEO), which oxidizes at a potential lower than 4 V versus Li. Herein, we adopt the polymerin-salt electrolyte (PISE) strategy to circumvent the disadvantage of the PEO-lithium bis(fluorosulfonyl)imide (LiFSI) system with EO/Li <= 8 through a dry ball-milling process to avoid the contamination of the residual solvent. The obtained solid-state PISEs exhibit distinctly different morphologies and coordination structures which lead to significant improvement in oxidative stability. P(EO)(1)LiFSI has a low melting temperature, a high ionic conductivity at 60 degrees C, and an oxidative stability of similar to 4.5 V versus Li/Li+. With an effective interphase rich in inorganic species and a good stability of the hybrid polymer electrolyte toward Li metal, the LMPB constructed with Li parallel to LiNi1/3Co1/3Mn1/3O2 can retain 74.4% of capacity after 186 cycles at 60 degrees C under the cutoff charge voltage of 4.3 V. The findings offer a promising pathway toward high-voltage stable polymer electrolytes for high-energy-density and safe LMPBs.

Automated summary

The newly developed polymer-in-salt electrolyte (PISE) provides a method to improve the oxidative stability of lithium metal polymer batteries (LMPBs) while maintaining high charge capacity. The solid-state PISEs prepared with a special process exhibit excellent performance, offering a promising pathway towards high-voltage stable LMPBs.