Lowering the sintering temperature of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> electrolyte for co-fired all-solid-state batteries via partial Bi substitution and precise control of compositional deviation

DOI Web Site 40 References Open Access
  • Watanabe Ken
    Department of Advanced Materials Science and Engineering, Faculty of Engineering Sciences, Kyushu University
  • Tashiro Ayumu
    Department of Molecular and Material Science, Interdisciplinary Graduate School of Engineering Science, Kyushu University
  • Ichinose Yoshihiro
    Department of Molecular and Material Science, Interdisciplinary Graduate School of Engineering Science, Kyushu University
  • Takeno Shinichi
    Department of Molecular and Material Science, Interdisciplinary Graduate School of Engineering Science, Kyushu University
  • Suematsu Koichi
    Department of Advanced Materials Science and Engineering, Faculty of Engineering Sciences, Kyushu University
  • Mitsuishi Kazutaka
    Research Center for Advanced Measurement and Characterization, National Institute for Materials Science
  • Shimanoe Kengo
    Department of Advanced Materials Science and Engineering, Faculty of Engineering Sciences, Kyushu University

Description

<p>Li7La3Zr2O12 (LLZ) has great potential as a solid electrolyte for co-fired all-solid-state Li-ion secondary batteries. However, to realise a solid-state battery using LLZ, the sintering temperature of LLZ should be reduced to one that can suppress the formation of a high-resistance reaction layer at the interface between LLZ and the electrode. In this study, we demonstrate an effective method for reducing the sintering temperature of Li6La3ZrTaO12 by combining partial Bi-substitution for Ta and precise control of the compositional deviation. The intentional tuning of the La deficiency in Li6La3ZrTa0.8Bi0.2O12 (LLZTB0.2) promoted the formation of a liquid phase based on Li2O–Bi2O3 at the grain boundary, resulting in its densification at 775 °C. Furthermore, we fabricated a co-fired all-solid-state half-cell based on an LLZTB0.2 electrolyte attached to a LiCoO2 + LLZTB0.2 composite electrode and a half-cell operated at 60 °C. From these results, it was found that the proposed concept is effective in reducing the sintering temperature of LLZ and is applicable for co-firing an all-solid-state battery.</p>

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