Lithium–sulfur batteries are attractive alternatives to lithium-ion batteries because of their high theoretical specific energy and natural abundance of sulfur. However, the polysulfides shuttle and the Li metal dendrite and corrosion significantly limit their cycle life. Moreover, the poor electronic conductivity of sulfur results in low areal sulfur loading and poor utilization, leading to low overall specific energy.
In the past years, we have developed several new strategies to mitigate these probelms, including: (1) Se doing because of much higher electronic conductivity of Se than Sulfur;[ref 1] (2) new electrolytes to directly bypass polysulfides formation and enable reversible Li stripping/plating;[ref 2 and 3]; (3) rational cathode design to boost sulfur reaction kinetics and suppress polysulfides shuttle and Li corrosion (ref 4-6); (4) Advanced Interlayer to minimize the shuttling effect and boost the cell capacity (ref 7.). Through these approaches, we have significantly improve the cycle life and specific energ of Li-S batteries in both coin-cells and pouch-cells.

1] Xu, G. L.; et al.; Nano Lett., 2016, 16, 2663-2673.
[2] Xu, G. L.; et al.; Solid-State Lithium/Selenium-Sulfur Chemistry Enabled via a Robust Solid-Electrolyte Interphase. Adv. Energy Mater., 2018, 1802235.
[3] Xu, G. L.; et al.; Regulating the Hidden Solvation-Ion-Exchange in Concentrated Electrolytes for Stable and Safe Lithium Metal Batteries. Adv. Energy Mater., 2020, 2000901.
[4] Zhao, C.; Xu, G. L.(*); et al.; Beyond Polysulfides Shuttle and Li Dendrite Formation: Addressing the Sluggish S Redox Kinetics for Practical High Energy Li-S batteries. Angew. Chem. Int. Ed. 2020, 17634-17640.
[5] Zhao, C.; Xu, G. L.(*); et al.; A high-energy and long-cycling lithium-sulfur pouch cell via a macroporous catalytic cathode with double-end binding sites. Nature Nanotechnology, 2021, 16, 166-173.
[6] Zhao, C.; Xu, G. L.(*); et al.; Pushing lithium-sulfur batteries towards practical working conditions through cathode-electrolyte synergy. Angew. Chem. Int. Ed. 2022, e202203466.
[7] Lee, B. J.; Zhao C.; Yu, J. H.; Kang, T. H.; Park, H. Y.; Kang, J.; Jung, Y.; Liu, X.; Li, T.; Xu, W.; Zuo, X.; Xu, G. L.(*); Amine, K.(*); Yu, J. S(*). Development of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy. Nature Commun. 2022, 13, 4629.

Gui-Liang Xu

Argonne National Laboratory

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