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Formation mechanism of sol-gel synthesized Li7−3xAlxLa3Zr2O12 and the influence of abnormal grain growth on ionic conductivity
Solid State Ionics ( IF 3.0 ) Pub Date : 2020-07-17 , DOI: 10.1016/j.ssi.2020.115407
Ying Tian , Ying Zhou , Yang Liu , Chao Zhao , Wen Wang , Yu Zhou

The development of solid-state batteries requires the optimization of ceramic electrolyte such as garnet type cubic Li7La3Zr2O12(LLZO). Exploration of powders formation mechanism and the sintering behavior of ceramics are crucial to acquire high performance LLZO electrolytes. This study adopts quantitative analysis based on X-ray adiabatic principle to investigate the formation mechanism of Li73xAlxLa3Zr2O12 (x = 0, 0.1, 0.15, 0.2, 0.25, LALZO) powders synthesized by sol-gel method. The whole calcination procedure could be divided into three stages as follows, La2Zr2O7(LZO) formation (<750 °C), transformation from LZO to LLZO (750 °C–850 °C) and LLZO decomposition (>850 °C). The phase, morphology and conductivity of LALZO ceramics demonstrate abnormal grain growth (AGG) caused by over-sintering leads to random orientation and conductivity deterioration. The optimal sintering condition could not only make grains bound tightly but also avoid AGG. Ceramics consist of LALZO (x = 0.25) exhibit better total ionic conductivity of 3.08 × 10−4 S cm−1 (Ea = 0.27 eV) with density of 92.5% after sintering at 1100 °C for 15 h. This research provides guidance for quickly acquiring pure LLZO powders and excellent performance ceramics.



中文翻译:

溶胶-凝胶的形成机理合成锂7 - 3 X的Al X的La 3 Zr的2 ö 12和异常晶粒生长的上离子导电性的影响

固态电池的发展需要优化陶瓷电解质,例如石榴石型立方Li 7 La 3 Zr 2 O 12(LLZO)。探索粉末的形成机理和陶瓷的烧结行为对于获得高性能LLZO电解质至关重要。本研究中采用了基于透视绝热原理定量分析来调查Li的形成机制7 - 3 X的Al X的La 3 Zr的2 ø 12X = 0、0.1、0.15、0.2、0.25,LALZO)粉末通过溶胶-凝胶法合成。整个煅烧过程可分为以下三个阶段:La 2 Zr 2 O 7(LZO)形成(<750°C),从LZO转变为LLZO(750°C–850°C)和LLZO分解(> 850) °C)。LALZO陶瓷的相,形态和电导率显示出由于过度烧结导致晶粒随机取向和电导率下降而导致的异常晶粒生长(AGG)。最佳的烧结条件不仅可以使晶粒紧密结合,而且可以避免AGG。由LALZO(x  = 0.25)组成的陶瓷表现出更好的总离子传导率3.08×10 -4  S cm -1(E a 在1100°C烧结15小时后,密度为92.5%(= 0.27 eV)。这项研究为快速获取纯LLZO粉和性能优异的陶瓷提供了指导。

更新日期:2020-07-17
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