Liang, Z.; et al. Understanding the failure process of sulfide-based all-solid-state lithium batteries via operando nuclear magnetic resonance spectroscopy. Nature Communications. 2023, 14(1): 259.
Introduction
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, the authors propose operando nuclear magnetic resonance (NMR) spectroscopy measurements for real-time quantification and evolution-tracking of inactive lithium formed in SSLMBs. The authors studied four different sulfide-based solid electrolytes, namely, Li10GeP2S12, Li9.54Si1.74P1.44S11.7Cl0.3, Li6PS5Cl and Li7P3S11. By monitoring the Li NMR signal during cell calendar ageing, the authors prove the faster corrosion rate of mossy/dendritic lithium than flat/homogeneous lithium in SSLMBs.