Understanding the failure process of sulfide-based all-solid-state lithium batteries via operando nuclear magnetic resonance spectroscopy

Ziteng Liang, Yuxuan Xiang, Kangjun Wang, Jianping Zhu, Yanting Jin, Hongchun Wang, Bizhu Zheng, Zirong Chen, Mingming Tao, Xiangsi Liu, Yuqi Wu, Riqiang Fu, Chunsheng Wang, Martin Winter and Yong Yang ()
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Ziteng Liang: Xiamen University
Yuxuan Xiang: Xiamen University
Kangjun Wang: Xiamen University
Jianping Zhu: Xiamen University
Yanting Jin: Xiamen University
Hongchun Wang: Xiamen University
Bizhu Zheng: Xiamen University
Zirong Chen: Xiamen University
Mingming Tao: Xiamen University
Xiangsi Liu: Xiamen University
Yuqi Wu: Xiamen University
Riqiang Fu: National High Magnetic Field Laboratory
Chunsheng Wang: University of Maryland
Martin Winter: University of Münster
Yong Yang: Xiamen University

Nature Communications, 2023, vol. 14, issue 1, 1-15

Abstract: Abstract The performance of all-solid-state lithium metal batteries (SSLMBs) is affected by the presence of electrochemically inactive (i.e., electronically and/or ionically disconnected) lithium metal and solid electrolyte interphase (SEI), which are jointly termed inactive lithium. However, the differentiation and quantification of inactive lithium during cycling are challenging, and their lack limits the fundamental understanding of SSLMBs failure mechanisms. To shed some light on these crucial aspects, here, we propose operando nuclear magnetic resonance (NMR) spectroscopy measurements for real-time quantification and evolution-tracking of inactive lithium formed in SSLMBs. In particular, we examine four different sulfide-based solid electrolytes, namely, Li10GeP2S12, Li9.54Si1.74P1.44S11.7Cl0.3, Li6PS5Cl and Li7P3S11. We found that the chemistry of the solid electrolyte influences the activity of lithium. Furthermore, we demonstrate that electronically disconnected lithium metal is mainly found in the interior of solid electrolytes, and ionically disconnected lithium metal is found at the negative electrode surface. Moreover, by monitoring the Li NMR signal during cell calendar ageing, we prove the faster corrosion rate of mossy/dendritic lithium than flat/homogeneous lithium in SSLMBs.

Date: 2023
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DOI: 10.1038/s41467-023-35920-7

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