Voltage-Responsive Rapid Defluorination of Free Anions in the Inner Helmholtz Layer for High-Performance Lithium Metal Batteries.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41491969.
- Also identified by DOI 10.1021/acs.nanolett.5c05088.
- No licence information is recorded for this record.
- Because redistribution is not established, this page shows the abstract only. Follow the links below for the full text.
Abstract
The intrinsically low oxidative stability of ether solvents, together with the formation of unstable solid electrolyte interphases in ether-based electrolytes, imposes significant limitations on their development in high-voltage lithium metal batteries. To address these issues, this work utilizes the voltage-responsive advantages of free anions and the susceptibility to cleavage of the S-F bond in FSI<sup>-</sup> anions, promoting the accumulation of FSI<sup>-</sup> within the inner Helmholtz layer and facilitating rapid defluorination. The designed ether-based electrolyte with a solvent-separated ion pair-dominated solvation structure leads to an increased LiF content in the electrode-electrolyte interphases and achieves a high average Coulombic efficiency of 99.2% for lithium plating/stripping. Furthermore, the Cu@Li||NCM811 full cell exhibits a capacity retention of 92.2% over 450 cycles at a cutoff voltage of 4.3 V. This work provides new insights into the electrical double layer and electrode interphase design, expanding the application of ether-based electrolytes in high-voltage LMBs.