Publication date: 10th April 2024
The Li10GeP2S12 are promising candidates of solid electrolytes for all-solid-state batteries, because it shows the high lithium ionic conductivity of 12 mS cm-1 at room temperature. For practical use, Li10GeP2S12 should be synthesized by the liquid-phase method, which enables mass production. However, Li10GeP2S12 synthesized by this solution synthesis shows lower ionic conductivity than that of the mechanical milling [1]. In this study, Li10GeP2S12 were synthesized through the solution synthesis with the Ti boat at the heat treatment step as the improved version. In addition, their particle characteristics of the sample synthesized by the solution synthesis were analyzed by transmission electron microscopy, particle size analysis, the impedance measurements at low temperatures at 190 K, and X-ray photoelectron spectroscopy. The solution synthesis sample in this study exhibited an ionic conductivity of 5.5 mS cm-1, which is the highest ionic conductivity of previous studies of liquid phase synthesis. The solution synthesis sample exhibited the smaller particle size than that of the mechanical milling sample. This smaller particle size at the solution synthesis sample is correlate with the higher grain boundary resistance, which cause to show lower total ionic conductivity. Moreover, the surface layer from solvent was detected on the particle surface synthesized by the solution synthesis based on the XPS measurement. This surface layer contributes to show the higher stable interface of Li-In/Li10GeP2S12. We expect these findings to enable the effective harnessing of the particle states to develop sulfide solid electrolytes with higher ionic conductivity and fine particles.
This work was supported by JSPS KAKENHI (Grant Number JP 22H04614), and the SOLiD-EV project (JPNP18003) of the New Energy and Industrial Technology Development Organization (NEDO), Japan. The XPS experiments were conducted at BL7U at the Aichi Synchrotron Radiation Center, Aichi Science & Technology Foundation, Aichi, Japan (Proposal No. 202204118 and No. 202302109). We thank Ms. Ikuyo Kusaba for their assistance with the experiments.
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