Realigning the Chemistry and Parameterization of Lithium‐Sulfur Battery Models to Accommodate Emerging Experimental Evidence and Cell Configurations

This is the authors' abstract. We don't add key points for this paper.

Experimental insights into lithium‐sulfur (LiS) battery chemistry have resulted in practical improvements in cell coulombic efficiency, sulfur utilization, and cycle life. However, optimization of this complex battery chemistry requires experimentally aligned modeling tools. A porous electrode theory‐based model incorporating key electrolyte dissociation chemistry is developed for the LiS cell. The proposed chemistry produces a radical anion species that is widely observed spectroscopically in LiS electrolytes. We explore the implications of radical anion formation on the current‐voltage behavior within the context of a state‐of‐art high energy density LiS cell with low electrolyte:sulfur (E/S) ratio and ideally‐protected anode. Parameters describing the dissociation reaction equilibrium and kinetics are shown to alter the electrolyte speciation in ways that can be linked to observations from LiS electrolyte engineering experiments.