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Nanomaterials (Basel). 2019 May 10;9(5). pii: E721. doi: 10.3390/nano9050721.

Dual Substitution and Spark Plasma Sintering to Improve Ionic Conductivity of Garnet Li7La3Zr2O12.

Dong Z1, Xu C2, Wu Y3, Tang W4, Song S5, Yao J6, Huang Z7, Wen Z8, Lu L9,10, Hu N11,12,13.

Author information

1
College of Aerospace Engineering, Chongqing University, Chongqing 400044, China. 20163113037@cqu.edu.cn.
2
College of Electrical Engineering, Chongqing University, Chongqing 400044, China. xuchao1995@cqu.edu.cn.
3
State Key Laboratory of Space Power-sources Technology, Shanghai Institute of Space Power-Sources, Shanghai 200245, China. wuym2014@126.com.
4
State Key Laboratory of Space Power-sources Technology, Shanghai Institute of Space Power-Sources, Shanghai 200245, China. tangwp@sina.cn.
5
College of Aerospace Engineering, Chongqing University, Chongqing 400044, China. sfsong@cqu.edu.cn.
6
College of Aerospace Engineering, Chongqing University, Chongqing 400044, China. yaojianyao@cqu.edu.cn.
7
College of Electrical Engineering, Chongqing University, Chongqing 400044, China. huangzhengyong@cqu.edu.cn.
8
CAS Key Laboratory of Materials for Energy Conversion, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China. zywen@mail.sic.ac.cn.
9
Department of Mechanical Engineering, National University of Singapore, Singapore 117575, Singapore. luli@nus.edu.sg.
10
National University of Singapore Suzhou Research Institute, Suzhou 215024, China. luli@nus.edu.sg.
11
College of Aerospace Engineering, Chongqing University, Chongqing 400044, China. ninghu@cqu.edu.cn.
12
School of Mechanical Engineering, Hebei University of Technology, Tianjin 300401, China. ninghu@cqu.edu.cn.
13
State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400044, China. ninghu@cqu.edu.cn.

Abstract

Garnet Li7La3Zr2O12 is one of the most promising solid electrolytes used for solid-state lithium batteries. However, low ionic conductivity impedes its application. Herein, we report Ta-doping garnets with compositions of Li7-xLa3Zr2-xTaxO12 (0.1 ≤ x ≤ 0.75) obtained by solid-state reaction and free sintering, which was facilitated by graphene oxide (GO). Furthermore, to optimize Li6.6La3Zr1.6Ta0.4O12, Mg2+ was select as a second dopant. The dual substitution of Ta5+ for Zr4+ and Mg2+ for Li+ with a composition of Li6.5Mg0.05La3Zr1.6Ta0.4O12 showed an enhanced total ionic conductivity of 6.1 × 10-4 S cm-1 at room temperature. Additionally, spark plasma sintering (SPS) was applied to further densify the garnets and enhance their ionic conductivities. Both SPS specimens present higher conductivities than those produced by the conventional free sintering. At room temperature, the highest ionic conductivity of Li6.5Mg0.05La3Zr1.6Ta0.4O12 sintered at 1000 °C is 8.8 × 10-4 S cm-1, and that of Li6.6La3Zr1.6Ta0.4O12 sintered at 1050 °C is 1.18 × 10-3 S cm-1.

KEYWORDS:

conductivity; dual substitution; garnet; spark plasma sintering

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