Understanding the Failure Process of Sulfide-Based All-Solid-State Lithium Batteries via Operando Nuclear Magnetic Resonance Spectroscopy
Primary author: Ziteng Liang (Xiamen University)
Co-Primary author: Yuxuan Xiang (Xiamen University)
Corresponding author: Yong Yang (Xiamen University)
Sulfide-based all-solid-state lithium batteries have attracted significant attention from the industry and academia due to their potential for high energy density and safety. However, in the case of lithium-negative electrode-type all-solid-state lithium batteries, non-active lithium is continuously generated during charge-discharge cycles, resulting in poor cycling performance and limiting their practical applications. Currently, non-active lithium consists of two parts: (1) non-active lithium metal (also known as "dead lithium"), which is caused by uneven lithium dissolution leading to the interruption of the electron-ion pathway, and (2) non-active lithium-containing compounds, which are formed due to interface (electro)chemical side reactions between the lithium metal negative electrode and the solid-state electrolyte. The presence of non-active lithium significantly affects the electrochemical performance of the battery. Therefore, accurately quantifying these two types of non-active lithium during the battery cycling process is crucial for understanding the failure process of all-solid-state lithium batteries.
Based on this, Yong Yang's team from Xiamen University, among others, for the first time utilized in-situ solid-state nuclear magnetic resonance (NMR) technology to analyze the failure mechanism of lithium metal negative electrodes in different sulfide-based all-solid-state lithium batteries. Through quantitative studies of non-active lithium in the system, the formation mechanisms of the two types of dead lithium in all-solid-state batteries were revealed. Additionally, the corrosion issue of the lithium metal negative electrode in all-solid-state lithium batteries was investigated for the first time, elucidating the relationship between the corrosion rate and the morphology of the lithium metal. This work deepens the understanding of the failure mechanism of all-solid-state lithium batteries and provides important guidance for further development. The research was published in the top international journal Nature Communications, with Ziteng Liang and Yuxuan Xiang as co-primary authors.
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