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<p>Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO)-based oxide solid-state electrolytes are recognized as one of the most promising electrolytes for solid-state batteries, yet the thermal stability of LLZO-based oxide solid electrolytes is lack of comprehensive understanding. Herein, we investigated the exothermic behaviors of LLZO-based oxide solid electrolytes and electrodes, revealing that both LiNi<sub>x</sub>Co<sub>y</sub>Mn<sub>1-x-y</sub>O<sub>2</sub> (NCM) and LiFePO<sub>4</sub> (LFP) cathodes have significant exothermic behavior during the heating process. The exothermic reactions of various LLZO/cathode mixture systems were also uncovered. Moreover, this study revealed the effects of doping element and grain size on the thermal stability of electrode/LLZO-based oxide solid-state electrolyte systems. The niobium (Nb) and tantalum (Ta) elements have both undermined the thermal stability of LLZO-based oxide solid electrolyte. The effect of grain size on thermal stability of LLZO/cathode systems follows the sequence of Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> (LLZTO) (LLZTO 300&#xa0;nm &lt; LLZTO 500&#xa0;nm &lt; LLZTO 5&#xa0;μm). These findings guide enhancement in the intrinsic thermal safety design and facilitate application for LLZO-based oxide solid electrolytes.</p>

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A comparative study on the thermal stability of Li7La3Zr2O12 (LLZO) solid-state electrolyte in composite electrode systems

  • 期刊论文

  • 发表日期：

    2026年7月25日

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  • Yixiu Gan,
  • Jiaying Wang,
  • Qianyu Ma,
  • Nan Ge,
  • Wei Gao

摘要

Li7La3Zr2O12 (LLZO)-based oxide solid-state electrolytes are recognized as one of the most promising electrolytes for solid-state batteries, yet the thermal stability of LLZO-based oxide solid electrolytes is lack of comprehensive understanding. Herein, we investigated the exothermic behaviors of LLZO-based oxide solid electrolytes and electrodes, revealing that both LiNixCoyMn1-x-yO2 (NCM) and LiFePO4 (LFP) cathodes have significant exothermic behavior during the heating process. The exothermic reactions of various LLZO/cathode mixture systems were also uncovered. Moreover, this study revealed the effects of doping element and grain size on the thermal stability of electrode/LLZO-based oxide solid-state electrolyte systems. The niobium (Nb) and tantalum (Ta) elements have both undermined the thermal stability of LLZO-based oxide solid electrolyte. The effect of grain size on thermal stability of LLZO/cathode systems follows the sequence of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) (LLZTO 300 nm < LLZTO 500 nm < LLZTO 5 μm). These findings guide enhancement in the intrinsic thermal safety design and facilitate application for LLZO-based oxide solid electrolytes.