Modification of Nitrate Ion Enables Stable Solid Electrolyte Interphase in Lithium Metal Batteries

Angew Chem Int Ed Engl. 2022 May 9;61(20):e202201406. doi: 10.1002/anie.202201406. Epub 2022 Mar 16.

Abstract

The lifespan of high-energy-density lithium metal batteries (LMBs) is hindered by heterogeneous solid electrolyte interphase (SEI). The rational design of electrolytes is strongly considered to obtain uniform SEI in working batteries. Herein, a modification of nitrate ion (NO3 - ) is proposed and validated to improve the homogeneity of the SEI in practical LMBs. NO3 - is connected to an ether-based moiety to form isosorbide dinitrate (ISDN) to break the resonance structure of NO3 - and improve the reducibility. The decomposition of non-resonant -NO3 in ISDN enriches SEI with abundant LiNx Oy and induces uniform lithium deposition. Lithium-sulfur batteries with ISDN additives deliver a capacity retention of 83.7 % for 100 cycles compared with rapid decay with LiNO3 after 55 cycles. Moreover, lithium-sulfur pouch cells with ISDN additives provide a specific energy of 319 Wh kg-1 and undergo 20 cycles. This work provides a realistic reference in designing additives to modify the SEI for stabilizing LMBs.

Keywords: Isosorbide Dinitrate; Lithium Metal Anodes; Lithium-Sulfur Batteries; Molecular Modification; Solid Electrolyte Interphase.