Fluorinating the Solid Electrolyte Interphase by Rational Molecular Design for Practical Lithium-Metal Batteries

The lifespan of practical lithium (Li)-metal batteries is severely hindered by the instability of Li-metal anodes. Fluorinated solid electrolyte interphase (SEI) emerges as a promising strategy to improve the stability of Li-metal anodes. The rational design of fluorinated molecules is pivotal to construct fluorinated SEI. Herein, design principles of fluorinated molecules are proposed. Fluoroalkyl (-CF2CF2-) is selected as an enriched F reservoir and the defluorination of the C-F bond is driven by leaving groups on beta-sites. An activated fluoroalkyl molecule (AFA), 2,2,3,3-tetrafluorobutane-1,4-diol dinitrate is unprecedentedly proposed to render fast and complete defluorination and generate uniform fluorinated SEI on Li-metal anodes. In Li-sulfur (Li-S) batteries under practical conditions, the fluorinated SEI constructed by AFA undergoes 183 cycles, which is three times the SEI formed by LiNO3. Furthermore, a Li-S pouch cell of 360 Wh kg(-1) delivers 25 cycles with AFA. This work demonstrates rational molecular design principles of fluorinated molecules to construct fluorinated SEI for practical Li-metal batteries.