High-Voltage Superionic Halide Solid Electrolytes for All-Solid-State Li-Ion Batteries,ACS Energy Letters

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High-Voltage Superionic Halide Solid Electrolytes for All-Solid-State Li-Ion Batteries
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-01-21 , DOI: 10.1021/acsenergylett.9b02599
Kern-Ho Park ₁ , Kavish Kaup ₁ , Abdeljalil Assoud ₁ , Qiang Zhang ₂ , Xiaohan Wu ₃ , Linda F. Nazar ₁

Affiliation

All-solid-state Li-ion batteries (ASSBs), considered to be potential next-generation energy storage devices, require solid electrolytes (SEs). Thiophosphate-based materials are popular, but these sulfides exhibit poor anodic stability and require specialty coatings on lithium metal oxide cathodes. Moreover, electrode designs aimed at high energy density are limited by their narrow electrochemical stability window. Here, we report new mixed-metal halide Li_3–xM_1–xZr_xCl₆ (M = Y, Er) SEs with high ionic conductivity—up to 1.4 mS cm^–1 at 25 °C—that are stable to high voltage. Substitution of M (M = Y, Er) by Zr is accompanied by a trigonal-to-orthorhombic phase transition, and structure solution using combined neutron and single-crystal X-ray diffraction methods reveal a new framework. The employment of >4 V-class cathode materials without any protective coating is enabled by the high electrochemical oxidation stability of these halides. An ASSB showcasing their electrolyte properties exhibits very promising cycling stability up to 4.5 V at room temperature.

中文翻译：

用于全固态锂离子电池的高压超离子卤化物固体电解质

全固态锂离子电池（ASSB）被认为是潜在的下一代能量存储设备，需要固态电解质（SE）。硫代磷酸盐基材料很受欢迎，但是这些硫化物的阳极稳定性差，并且需要在锂金属氧化物阴极上进行特殊涂层。此外，针对高能量密度的电极设计受到其狭窄的电化学稳定性窗口的限制。在这里，我们报告了新的混合金属卤化物Li ₃ – _x M _{1– x} Zr _x Cl ₆（M = Y，Er）SE，具有高离子电导率-高达1.4 mS cm ^–1在25°C的温度下对高压稳定。Zr取代M（M = Y，Er）伴随着从三角形到斜方晶的相变，并且使用中子和单晶X射线衍射方法相结合的结构求解揭示了一个新的框架。这些卤化物具有很高的电化学氧化稳定性，因此可以采用> 4 V级阴极材料而没有任何保护性涂层。展示其电解质特性的ASSB在室温下显示出非常有希望的高达4.5 V的循环稳定性。

更新日期：2020-01-22

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