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

Huang, Li; Gao, Jian; Bi, Zhijie; Zhao, Ning; Wu, Jipeng; Fang, Qiu; Wang, Xuefeng; Wan, Yong; Guo, Xiangxin

doi:10.3390/en15093206

Open AccessArticle

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

by

Li Huang

¹,

Jian Gao

²,

Zhijie Bi

^1,*,

Ning Zhao

¹

,

Jipeng Wu

^3,4,

Qiu Fang

^3,4,

Xuefeng Wang

^3,4,

Yong Wan

^1,* and

Xiangxin Guo

^1,*

¹

College of Physics, Qingdao University, Qingdao 266071, China

²

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

³

Laboratory for Advanced Materials & Electron Microscopy, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

⁴

College of Materials Science and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100049, China

^*

Authors to whom correspondence should be addressed.

Energies 2022, 15(9), 3206; https://doi.org/10.3390/en15093206

Submission received: 27 March 2022 / Revised: 17 April 2022 / Accepted: 25 April 2022 / Published: 27 April 2022

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Abstract

The cubic garnet Li₇La₃Zr₂O₁₂ (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 Li₂CO₃ 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 Li₇La₃Zr₂O₁₂ (Al-LLZO), Al-Ta-doped Li₇La₃Zr₂O₁₂ (Al-LLZTO), and Al-Nb-doped Li₇La₃Zr₂O₁₂ (Al-LLZNO). It was found that Al-LLZTO and Al-LLZNO are less reactive with air than Al-LLZO. The morphology of Li₂CO₃ on Al-LLZTO micro-sized powders after air exposure was island-like with ~1.5 μm 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 Li₂O and, thus, the next step product of Li₂CO₃ following the reactions of Li₂O + H₂O → LiOH and LiOH + CO₂ → Li₂CO₃.

Keywords: solid garnet electrolytes; air stability; Li₂CO₃; doped electrolytes

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MDPI and ACS Style

Huang, L.; Gao, J.; Bi, Z.; Zhao, N.; Wu, J.; Fang, Q.; Wang, X.; Wan, Y.; Guo, X. Comparative Study of Stability against Moisture for Solid Garnet Electrolytes with Different Dopants. Energies 2022, 15, 3206. https://doi.org/10.3390/en15093206

AMA Style

Huang L, Gao J, Bi Z, Zhao N, Wu J, Fang Q, Wang X, Wan Y, Guo X. Comparative Study of Stability against Moisture for Solid Garnet Electrolytes with Different Dopants. Energies. 2022; 15(9):3206. https://doi.org/10.3390/en15093206

Chicago/Turabian Style

Huang, Li, Jian Gao, Zhijie Bi, Ning Zhao, Jipeng Wu, Qiu Fang, Xuefeng Wang, Yong Wan, and Xiangxin Guo. 2022. "Comparative Study of Stability against Moisture for Solid Garnet Electrolytes with Different Dopants" Energies 15, no. 9: 3206. https://doi.org/10.3390/en15093206

APA Style

Huang, L., Gao, J., Bi, Z., Zhao, N., Wu, J., Fang, Q., Wang, X., Wan, Y., & Guo, X. (2022). Comparative Study of Stability against Moisture for Solid Garnet Electrolytes with Different Dopants. Energies, 15(9), 3206. https://doi.org/10.3390/en15093206

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

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