TY - JOUR
T1 - 3D Asymmetric Bilayer Garnet-Hybridized High-Energy-Density Lithium−Sulfur Batteries
AU - Shi, Changmin
AU - Hamann, Tanner
AU - Takeuchi, Saya
AU - Alexander, George V.
AU - Nolan, Adelaide M.
AU - Limpert, Matthew
AU - Fu, Zhezhen
AU - O’Neill, Jonathan
AU - Godbey, Griffin
AU - Dura, Joseph A.
AU - Wachsman, Eric D.
N1 - Publisher Copyright:
© 2022 American Chemical Society.
PY - 2023/1/11
Y1 - 2023/1/11
N2 - 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 in Li−S cells using Ta-doped LLZO (Ta-LLZO) as a solid electrolyte. It was observed that this cell failure is correlated with lanthanum segregation to the surface of Ta-LLZO that reacts with a sulfur cathode. We demonstrated this correlation by using lanthanum excess and lanthanum deficient Ta-LLZO as the solid electrolyte in Li−S cells. To resolve this challenge, we physically separated the sulfur cathode and LLZO using a poly(ethylene oxide) (PEO)-based buffer interlayer. With a thin bilayer of LLZO and the stabilized sulfur cathode/LLZO interface, the hybridized Li−S batteries achieved a high initial discharge capacity of 1307 mA h/g corresponding to an energy density of 639 W h/L and 134 W h/kg under a high current density of 0.2 mA/cm2 at room temperature without any indication of a polysulfide shuttle. By simply reducing the LLZO dense layer thickness to 10 μm as we have demonstrated before, a significantly higher energy density of 1308 W h/L and 257 W h/kg is achievable. X-ray diffraction and X-ray photoelectron spectroscopy indicate that the PEO-based interlayer, which physically separates the sulfur cathode and LLZO, is both chemically and electrochemically stable with LLZO. In addition, the PEO-based interlayer can adapt to the stress/strain associated with sulfur volume expansion during lithiation.
AB - 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 in Li−S cells using Ta-doped LLZO (Ta-LLZO) as a solid electrolyte. It was observed that this cell failure is correlated with lanthanum segregation to the surface of Ta-LLZO that reacts with a sulfur cathode. We demonstrated this correlation by using lanthanum excess and lanthanum deficient Ta-LLZO as the solid electrolyte in Li−S cells. To resolve this challenge, we physically separated the sulfur cathode and LLZO using a poly(ethylene oxide) (PEO)-based buffer interlayer. With a thin bilayer of LLZO and the stabilized sulfur cathode/LLZO interface, the hybridized Li−S batteries achieved a high initial discharge capacity of 1307 mA h/g corresponding to an energy density of 639 W h/L and 134 W h/kg under a high current density of 0.2 mA/cm2 at room temperature without any indication of a polysulfide shuttle. By simply reducing the LLZO dense layer thickness to 10 μm as we have demonstrated before, a significantly higher energy density of 1308 W h/L and 257 W h/kg is achievable. X-ray diffraction and X-ray photoelectron spectroscopy indicate that the PEO-based interlayer, which physically separates the sulfur cathode and LLZO, is both chemically and electrochemically stable with LLZO. In addition, the PEO-based interlayer can adapt to the stress/strain associated with sulfur volume expansion during lithiation.
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U2 - 10.1021/acsami.2c14087
DO - 10.1021/acsami.2c14087
M3 - Article
C2 - 36580372
AN - SCOPUS:85145473662
SN - 1944-8244
VL - 15
SP - 751
EP - 760
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
IS - 1
ER -