From the perspective of fundamental research on new LMB technologies, it is critical to meticulously develop suitable liquid electrolyte chemistry that works with promising anodes and cathodes.
They demonstrated a strategy for improving high-voltage compatibility of dilute (<3 M) ether-based lithium electrolytes by using the highly nonpolar ether solvent. The low concentration LiFSI-based electrolyte with nonfluorinated DPE solvent was shown to extend the high voltage (4.3 V) operation of LMBs with commercially viable battery configurations (high loading cathode, controlled anode, and electrolyte amount). Due to the weak coordination ability to Li+ and the ion aggregation enriched Li solvation behavior, DPE tunes the relative HOMO energy level of aggregated solvate species and rearranges the decomposition order of electrolyte components at cathode surface. The preferential degradation of ion aggregates circumvents the oxidation of free ether molecules and leads to a robust anion-derived CEI layer. The aggregated Li solvation structure displaces the ether molecules in the EDL, leading to solvent-deficient interfacial regime and synergistically enhances ion transfer process. Compared to the conventional electrolyte design strategies, stabilizing the positive electrode interface enables a CE of 99.90% by using the DPE electrolyte does not require diminishing the free ether molecules or improving the thermodynamic stability of the electrolyte. The Li||NCM811 coin cell retains 82% capacity after 220 cycles at 1 mA/cm2, and the practical pouch cell also demonstrates 150 stable cycles with 74.1% retention (0.33 and 1 mA/cm2 charge and discharge, respectively).