Comparative Study of Stability against Moisture for Solid Garnet Electrolytes with Different Dopants

Li Huang, Jian Gao, Zhijie Bi, Ning Zhao, Jipeng Wu, Qiu Fang, Xuefeng Wang, Yong Wan and Xiangxin Guo
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Li Huang: College of Physics, Qingdao University, Qingdao 266071, China
Jian Gao: Beijing Advanced Innovation Center for Soft Matter Science and Engineering, State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
Zhijie Bi: College of Physics, Qingdao University, Qingdao 266071, China
Ning Zhao: College of Physics, Qingdao University, Qingdao 266071, China
Jipeng Wu: Laboratory for Advanced Materials & Electron Microscopy, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
Qiu Fang: Laboratory for Advanced Materials & Electron Microscopy, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
Xuefeng Wang: Laboratory for Advanced Materials & Electron Microscopy, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
Yong Wan: College of Physics, Qingdao University, Qingdao 266071, China
Xiangxin Guo: College of Physics, Qingdao University, Qingdao 266071, China

Energies, 2022, vol. 15, issue 9, 1-9

Abstract: The cubic garnet Li 7 La 3 Zr 2 O 12 (c-LLZO) is one of the most promising solid electrolytes due to its high ionic conductivity and large electrochemical window. However, the critical issue of Li 2 CO 3 formation on the c-LLZO surface when exposed to air is problematic, which is detrimental to the ionic conductivity and storage. Herein, comparative studies were carried out on the air stability of Al-doped Li 7 La 3 Zr 2 O 12 (Al-LLZO), Al-Ta-doped Li 7 La 3 Zr 2 O 12 (Al-LLZTO), and Al-Nb-doped Li 7 La 3 Zr 2 O 12 (Al-LLZNO). It was found that Al-LLZTO and Al-LLZNO are less reactive with air than Al-LLZO. The morphology of Li 2 CO 3 on Al-LLZTO micro-sized powders after air exposure was island-like with ~1.5 ?m in thickness. The interfacial resistance of Li/Al-LLZTO was also a factor of ~3 smaller than that of Li/Al-LLZO, leading to the improved cycle stability of Li/Al-LLZTO/Li symmetric cells. The first-principles calculations based on density functional theory (DFT) verified that the decomposition energy of Al-LLZTO was larger than that of Al-LLZO, inhibiting the reaction product of Li 2 O and, thus, the next step product of Li 2 CO 3 following the reactions of Li 2 O + H 2 O ? LiOH and LiOH + CO 2 ? Li 2 CO 3 .

Keywords: solid garnet electrolytes; air stability; Li 2 CO 3; doped electrolytes (search for similar items in EconPapers)
JEL-codes: Q Q0 Q4 Q40 Q41 Q42 Q43 Q47 Q48 Q49 (search for similar items in EconPapers)
Date: 2022
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