TY  - JOUR
AU  - Liang, Ziteng
AU  - Xiang, Yuxuan
AU  - Wang, Kangjun
AU  - Zhu, Jianping
AU  - Jin, Yanting
AU  - Wang, Hongchun
AU  - Zheng, Bizhu
AU  - Chen, Zirong
AU  - Tao, Mingming
AU  - Liu, Xiangsi
AU  - Wu, Yuqi
AU  - Fu, Riqiang
AU  - Wang, Chunsheng
AU  - Winter, Martin
AU  - Yang, Yong
TI  - Understanding the failure process of sulfide-based all-solid-state lithium batteries via operando nuclear magnetic resonance spectroscopy
JO  - Nature Communications
VL  - 14
IS  - 1
SN  - 2041-1723
CY  - [London]
PB  - Nature Publishing Group UK
M1  - FZJ-2024-02609
SP  - 259
PY  - 2023
AB  - 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.
LB  - PUB:(DE-HGF)16
C6  - 36650152
UR  - <Go to ISI:>//WOS:001003645200035
DO  - DOI:10.1038/s41467-023-35920-7
UR  - https://juser.fz-juelich.de/record/1025015
ER  -