3D Asymmetric Bilayer Garnet-Hybridized High-Energy-Density Lithium–Sulfur Batteries

• DOI: 10.1021/acsami.2c14087
• Publication Date: 2022-12-29T16:58:06Z
• Authors: Changmin Shi; Tanner Hamann; Saya Takeuchi; George V. Alexander; Adelaide M. Nolan; Matthew Limpert; Zhezhen Fu; Jonathan O’Neill; Griffin Godbey; Joseph A. Dura; Eric D. Wachsman
• Keywords: Lanthanum; Polysulfide; Lanthanum oxide

Lithium garnet Li7La3Zr2O12 (LLZO), with high ionic conductivity and chemical stability against a Li metal anode, is considered one of the most promising solid electrolytes for lithium-sulfur batteries. However, an infinite charge time resulting in low capacity has been observed Li-S cells using Ta-doped LLZO (Ta-LLZO) as electrolyte. It was that this cell failure correlated lanthanum segregation to surface Ta-LLZO reacts sulfur cathode. We demonstrated correlation by excess deficient electrolyte cells. To resolve challenge, we physically separated cathode poly(ethylene oxide) (PEO)-based buffer interlayer. With thin bilayer stabilized cathode/LLZO interface, hybridized batteries achieved initial discharge 1307 mA h/g corresponding energy density 639 W h/L 134 h/kg under current 0.2 mA/cm2 at room temperature without any indication polysulfide shuttle. By simply reducing dense layer thickness 10 μm have before, significantly higher 1308 257 achievable. X-ray diffraction photoelectron spectroscopy indicate PEO-based interlayer, which separates LLZO, both chemically electrochemically stable LLZO. In addition, interlayer can adapt stress/strain associated volume expansion during lithiation.