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@ARTICLE{Liang:1025015,
author = {Liang, Ziteng and Xiang, Yuxuan and Wang, Kangjun and Zhu,
Jianping and Jin, Yanting and Wang, Hongchun and Zheng,
Bizhu and Chen, Zirong and Tao, Mingming and Liu, Xiangsi
and Wu, Yuqi and Fu, Riqiang and Wang, Chunsheng and Winter,
Martin and Yang, Yong},
title = {{U}nderstanding the failure process of sulfide-based
all-solid-state lithium batteries via operando nuclear
magnetic resonance spectroscopy},
journal = {Nature Communications},
volume = {14},
number = {1},
issn = {2041-1723},
address = {[London]},
publisher = {Nature Publishing Group UK},
reportid = {FZJ-2024-02609},
pages = {259},
year = {2023},
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.},
cin = {IEK-12},
ddc = {500},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {1221 - Fundamentals and Materials (POF4-122)},
pid = {G:(DE-HGF)POF4-1221},
typ = {PUB:(DE-HGF)16},
pubmed = {36650152},
UT = {WOS:001003645200035},
doi = {10.1038/s41467-023-35920-7},
url = {https://juser.fz-juelich.de/record/1025015},
}