Potassium Hexafluorophosphate Additive Enables Stable Lithium-Sulfur Batteries

ACS Appl Mater Interfaces. 2020 Dec 16;12(50):56017-56026. doi: 10.1021/acsami.0c17406. Epub 2020 Dec 3.

Abstract

Uncontrollable dendrite growth and low Coulombic efficiency are the two main obstacles that hinder the application of rechargeable Li metal batteries. Here, an optimized amount of potassium hexafluorophosphate (KPF6, 0.01 M) has been added into the 2 M LiTFSI/ether-based electrolyte to improve the cycling stability of lithium-sulfur (Li-S) batteries. Due to the synergistic effect of self-healing electrostatic shield effect from K+ cations and the LiF-rich solid electrolyte interphases derived from PF6- anions, the KPF6 additive enables a high Li Coulombic efficiency of 98.8% (1 mA cm-2 of 1 mAh cm-2). The symmetrical Li cell can achieve a stable cycling performance for over 200 cycles under a high Li utilization up to 33.3%. Meanwhile, the polysulfide shuttle has been restrained due to the higher concentration of the LiTFSI in the electrolyte. As a result, the assembled Li-S full cell displays excellent capacity retention with only 0.25% decay per cycle in the final electrolyte. Our work offers a smart approach to improve both the anode and cathode performance by the electrolyte modification of rechargeable Li-S batteries.

Keywords: Li metal anode; LiF-rich interphase; Li−S battery; dendrite suppression; self-healing electrostatic shield.