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Low-temperature processing of Garnet-type ion conductive cubic Li7La3Zr2O12 powders for high performance all solid-type Li-ion batteries
Journal of the Taiwan Institute of Chemical Engineers ( IF 5.7 ) Pub Date : 2018-03-28 , DOI: 10.1016/j.jtice.2018.02.021
Jeevan Kumar Padarti , Taruna Teja Jupalli , Chie Hirayama , Mamoru Senna , Takahiko Kawaguchi , Naonori Sakamoto , Naoki Wakiya , Hisao Suzuki

Synthesis of lithium stuffed cubic Li7La3Zr2O12 (c-LLZO) garnet at low-processing temperatures is hampered by the lack of deep understanding on powder processing technology. The present article proposes a hybrid solid-state approach to accomplish controllable synthesis of Al doped LLZO cubic garnet oxide nanoparticles at low-processing temperatures. In this procedure, powders of ZrO2 and La(OH)3 in ethanol based suspension were mechanochemically (MC) treated along with 1 wt.% of AlOOH in a planetary ball mill with increasing milling time to increase the homogeneity of the precursor. Lithium acetate in the form of an ethanolic solution was subsequently added for the solid-state synthesis of single phase LLZO. Cubic LLZO phases were obtained at temperatures i.e. 700 °C within 3 h. The ease of lithium diffusion in these MC activated La-Zr precursor materials is attributed to the formation of single phase LLZO with the lowest Al3+ doping content. The sintered pellets (94% relative density at 1100°C for 3 h in air) of the newly obtained Li6.61La3Zr2Al0.13O11.98 deliver high bulk Li-ion conductivity of 1.35 × 104 Scm-1. The new low-temperature processing of typical garnet and the use of c-Li6.61La3Zr2Al0.13O11.98 nanoparticles could open pathways toward future solid electrolyte–electrode assembly options for all-solid state Li-ion batteries.



中文翻译:

用于高性能全固态锂离子电池的石榴石型离子导电立方Li 7 La 3 Zr 2 O 12粉末的低温加工

由于对粉末加工技术缺乏深入的了解,阻碍了锂填充立方晶Li 7 La 3 Zr 2 O 12c- LLZO)石榴石的合成。本文提出了一种混合固态方法,以在低处理温度下完成可控合成Al掺杂的LLZO立方石榴石氧化物纳米粒子。在此过程中,ZrO 2和La(OH)3的粉末在行星式球磨机中,以乙醇为基础的悬浮液中的乙醇与1 wt。%的AlOOH进行机械化学处理(MC),以增加研磨时间以增加前体的均质性。随后加入乙醇溶液形式的乙酸锂用于单相LLZO的固态合成。得到立方LLZO相在温度,即3小时内700℃。在这些MC活化的La-Zr前体材料中,锂易于扩散的原因是,形成了具有最低Al 3+掺杂含量的单相LLZO 。烧结的小球(1100时相对密度为94%℃下的新获得的锂在空气中3小时)6.61的La 3 Zr的2的Al 0.13 ö 11.98递送1.35×10的高堆积Li离子传导性- 4  SCM -1。典型的石榴石的新型低温处理工艺以及使用c- Li 6.61 La 3 Zr 2 Al 0.13 O 11.98纳米粒子的使用可能为通向未来的全固态锂离子电池固体电解质-电极装配选择开辟道路。

更新日期:2018-03-28
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