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<p>All-solid-state batteries (ASSBs) with a garnet-type solid electrolyte have been considered promising alternatives to traditional batteries with a liquid organic electrolyte, due to their enhanced safety and ability to accommodate high energy density electrodes. In this study, we conducted a comprehensive investigation of the high-temperature chemical compatibility between the garnet-like Li<sub>6.4</sub>Ga<sub>0.2</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (Ga-LLZO) electrolyte and high-energy-density Li-rich layered Li<sub>1.2</sub>Ni<sub>0.2</sub>Mn<sub>0.6</sub>O<sub>2</sub> cathode (LNM). Our findings suggest that a high temperature reaction between the Li-rich cathode and Ga-LLZO occurs at 700-900<sup>o</sup>C depending on the form of reactants. This reaction results in the formation of La(Ni, Mn)O<sub>3</sub> and Li<sub>2</sub>ZrO<sub>3</sub> as the two main products, as confirmed by powder X-ray diffraction and transmission electron microscopy analysis. Li<sub>2</sub>ZrO<sub>3</sub> was discovered for the first time as a reaction product, and its formation in the case of Li-rich layered cathode material was rationalized with DFT + <i>U</i> calculations. The results were also compared with those obtained for a typical layered high-energy-density cathode material LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811).</p>

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Chemical compatibility at the interface of garnet-type Ga-LLZO solid electrolyte and high-energy Li-rich layered oxide cathode for all-solid-state batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年1月2日

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  • Natalia B. Timusheva,
  • Alexander A. Golubnichiy,
  • Anatolii V. Morozov,
  • Arseniy S. Burov,
  • Dmitry A. Aksyonov,
  • Aleksandra A. Savina,
  • Roman G. Markopolskii,
  • Artem M. Abakumov

摘要

All-solid-state batteries (ASSBs) with a garnet-type solid electrolyte have been considered promising alternatives to traditional batteries with a liquid organic electrolyte, due to their enhanced safety and ability to accommodate high energy density electrodes. In this study, we conducted a comprehensive investigation of the high-temperature chemical compatibility between the garnet-like Li6.4Ga0.2La3Zr2O12 (Ga-LLZO) electrolyte and high-energy-density Li-rich layered Li1.2Ni0.2Mn0.6O2 cathode (LNM). Our findings suggest that a high temperature reaction between the Li-rich cathode and Ga-LLZO occurs at 700-900oC depending on the form of reactants. This reaction results in the formation of La(Ni, Mn)O3 and Li2ZrO3 as the two main products, as confirmed by powder X-ray diffraction and transmission electron microscopy analysis. Li2ZrO3 was discovered for the first time as a reaction product, and its formation in the case of Li-rich layered cathode material was rationalized with DFT + U calculations. The results were also compared with those obtained for a typical layered high-energy-density cathode material LiNi0.8Mn0.1Co0.1O2 (NMC811).