<br>Li2ZrCl6 电解质在潮湿空气中的降解演化以及通过有效的铟替代增强空气稳定性,Small

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Li2ZrCl6 电解质在潮湿空气中的降解演化以及通过有效的铟替代增强空气稳定性
Small ( IF 13.0 ) Pub Date : 2023-10-25 , DOI: 10.1002/smll.202306736
Xuming Luo ₁ , Xiaoyu Hu ₁ , Yu Zhong ₁ , Xiuli Wang ₁ , Jiangping Tu ₁

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超离子卤化物引起了Li ₂ ZrCl ₆等固体电解质领域的兴趣。然而，他们仍然面临着空中稳定性差等挑战，缺乏深入的调查。在此，证明了Li ₂ ZrCl ₆的水分不稳定性，并清楚地揭示了空气中的分解机制。当暴露于湿气时，Li ₂ ZrCl ₆在初始阶段作为卤化物分解成Li ₂ ZrO ₃ 、ZrOCl ₂ · x H ₂ O和LiCl。随后，经过较长时间的暴露，这些副产物演变为LiCl(H ₂ O)和Li ₆ Zr ₂ O ₇ 。更重要的是，被破坏的卤化物结构在后加热后无法恢复。随后，将铟掺杂到Li ₂ ZrCl ₆ (9.7 × 10 ^-5 S cm ^-1 )中以探讨其对结构和性能的影响。随着In含量的增加，球磨In掺杂Li ₂ ZrCl ₆电解质的晶体结构从Li ₃ YCl ₆类转变为Li ₃ InCl ₆类，离子电导率也得到增强 (0.768–1.13) × 10 ^{− 3} S cm ^-1 )。更重要的是，最佳Li _2.8 Zr _0.2 In _0.8 Cl ₆具有良好的空气稳定性，因为暴露在空气中后形成卤化物水合物而不是完全分解，并且水合物在后加热后可以恢复为Li _2.8 Zr _0.2 In _0.8 Cl ₆ 。此外，重新加热Li _2。暴露空气后的8 Zr _0.2 In _0.8 Cl ₆成功应用于固态LiNi _0.8 Co _0.1 Mn _0.1 O ₂ /卤化物/Li ₆ PS ₅ Cl/Li–In电池。这项工作的结果可以为Li ₂ ZrCl ₆的空气不稳定性提供深入的见解，并为调节卤化物的空气稳定性提供有效的策略。

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Degradation Evolution for Li2ZrCl6 Electrolytes in Humid Air and Enhanced Air Stability via Effective Indium Substitution

Superionic halides have aroused interests in field of solid electrolytes such as Li₂ZrCl₆. However, they are still facing challenges including poor air stability which lacks in-depth investigation. Here, moisture instability of Li₂ZrCl₆ is demonstrated and decomposition mechanism in air is clearly revealed. Li₂ZrCl₆ decomposes into Li₂ZrO₃, ZrOCl₂·xH₂O and LiCl during initial stage as halides upon moisture exposure. Later, these side products evolve into LiCl(H₂O) and Li₆Zr₂O₇ after longer time exposure. More importantly, structure of destroyed halides cannot be recovered after postheating. Later, Indium is doped into Li₂ZrCl₆ (9.7 × 10⁻⁵ S cm⁻¹) to explore its effect on structure and properties. Crystal structure of ball-milled In-doped Li₂ZrCl₆ electrolytes is converted from the Li₃YCl₆-like to Li₃InCl₆-like with increasing In content and ionic conductivity can also be enhanced (0.768–1.13) × 10⁻³ S cm⁻¹). More importantly, good air stability of optimal Li_2.8Zr_0.2In_0.8Cl₆ is achieved since halide hydrates are formed after air exposure instead of total decomposition and the hydrates can be restored to Li_2.8Zr_0.2In_0.8Cl₆ after postheating. Moreover, reheated Li_2.8Zr_0.2In_0.8Cl₆ after air exposure is successfully applied in solid-state LiNi_0.8Co_0.1Mn_0.1O₂/halides/Li₆PS₅Cl/Li–In battery. The results in this work can provide insights into air instability of Li₂ZrCl₆ and effective strategy to regulate air stability of halides.

更新日期：2023-10-25

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