Ammonium Additives to Dissolve Lithium Sulfide through Hydrogen Binding for High-Energy Lithium–Sulfur Batteries

In rechargeable Li–S batteries, the uncontrollable passivation of electrodes by highly insulating Li2S limits sulfur utilization, increases polarization, and decreases cycling stability. Dissolving Li2S in organic electrolyte is a facile solution to maintain the active reaction interface between electrolyte and sulfur cathode, and thus address the above issues. Herein, ammonium salts are demonstrated as effective additives to promote the dissolution of Li2S to 1.25 M in DMSO solvent at room temperature. NMR measurements show that the strong hydrogen binding effect of N–H groups plays a critical role in dissolving Li2S by forming complex ligands with S2– anions coupled with the solvent's solvating surrounding. Ammonium additives in electrolyte can also significantly improve the oxidation kinetics of Li2S, and therefore enable the direct use of Li2S as cathode material in Li–S battery system in the future. This provides a new approach to manage the solubility of lithium sulfides through cation coordination with sulfide anion.