Publication date: 10th April 2024
All-solid-state battery configurations using a solid electrolyte promise next-generation high-performance batteries. One of the main problems with all-solid-state lithium-ion batteries is their low cathode capacity, which requires the use of conductive carbon additives. The oxy-sulfide Li2FeSO with a cubic anti-perovskite structure has been investigated as a new cathode material due to its high theoretical capacity (455 mAhg-1). We constructed an all-solid-state battery with a Li2FeSO electrode that demonstrated a relatively high discharge capacity of approximately 270 mAh g-1 at a high electrode loading ratio (90 wt%) [1]. Hence, we demonstrated that Li2FeSO is suitable for all-solid-state batteries. However, the reason for its superior performance remains unclear. Therefore, In this study, Li2FeSO was synthesized through mechanical milling, and the charge compensation mechanism during the battery reaction and the cross-sectional microstructure were analyzed. According to the scanning electron microscopy image, a dense body was observed, even at a high Li2FeSO active material loading ratio (90 wt%). From an indentation test, the elastic modulus, Mayer hardness, and yield point were found to be 24.9, 0.46, and 0.82 GPa, respectively, which are similar to those of sulfide solid electrolyte all-solid-state batteries. The excellent low modulus and high formability due to the presence of sulfur contribute to superior battery performance. Finally, HAXPES measurements were conducted to analyze the charge compensation mechanism. Fe oxidation in the low-voltage region and S oxidation in the high-voltage region occurred during charging. In contrast, S reduction in the high-voltage region and Fe reduction in the low-voltage region occurred during discharge.
This work was supported by JSPS KAKENHI (Grant Number JP 21K14716), Tokai Foundation for Industrial Technology, and Hibi Science Foundation. The HAXPES experiments were conducted at BL6N1 at the Aichi Synchrotron Radiation Center, Aichi Science & Technology Foundation, Aichi, Japan (Proposal No. 202205052 and No. 202302108).
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