On the Way Toward Understanding Solution Chemistry of Lithium Polysulfides for High Energy Li-S Redox Flow Batteries

Lithium-sulfur (Li-S) redox flow battery (RFB) is a promising candidate for high energy large-scale energy storage application due to good solubility of long-chain polysulfide species and low cost of sulfur. Here, the fundamental understanding and control of lithium polysulfide chemistry are studied to enable the development of liquid phase Li-S redox flow prototype cells. These differ significantly from conventional static Li-S batteries targeting for vehicle electrification. A high solubility of the different lithium polysulfides generated at different depths of discharge and states of charge is required for a flow battery in order to take full advantage of the multiple electron transitions. A new dimethyl sulfoxide based electrolyte is proposed for Li-S RFBs, which not only enables the high solubility of lithium polysulfide species, especially for the short-chain species, but also results in excellent cycling with a high Coulombic efficiency. The challenges and opportunities for the Li-S redox flow concept have also been discussed in depth.