Ultra-Low Concentration Electrolyte Enabling LiF-Rich SEI and Dense Plating/Stripping Processes for Lithium Metal Batteries

Adv Sci (Weinh). 2022 Oct;9(28):e2203216. doi: 10.1002/advs.202203216. Epub 2022 Aug 17.

Abstract

The interface structure of the electrode is closely related to the electrochemical performance of lithium-metal batteries (LMBs). In particular, a high-quality solid electrode interface (SEI) and uniform, dense lithium plating/stripping processes play a key role in achieving stable LMBs. Herein, a LiF-rich SEI and a uniform and dense plating/stripping process of the electrolyte by reducing the electrolyte concentration without changing the solvation structure, thereby avoiding the high cost and poor wetting properties of high-concentration electrolytes are achieved. The ultra-low concentration electrolyte with an unchanged Li+ solvation structure can restrain the inhomogeneous diffusion flux of Li+ , thereby achieving more uniform lithium deposition and stripping processes while maintaining a LiF-rich SEI. The LiIICu battery with this electrolyte exhibits enhanced cycling stability for 1000 cycles with a coulombic efficiency of 99% at 1 mA cm-2 and 1 mAh cm-2 . For the LiIILiFePO4 pouch cell, the capacity retention values at 0.5 and 1 C are 98.6% and 91.4%, respectively. This study offers a new perspective for the commercial application of low-cost electrolytes with ultra-low concentrations and high concentration effects.

Keywords: dense plating/stripping process; electrolyte concentration; lithium metal batteries; pouch cell; solid electrolyte interphase.