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

College of Aerospace Engineering, Chongqing University, Chongqing 400044, China
College of Electrical Engineering, Chongqing University, Chongqing 400044, China
State Key Laboratory of Space Power-sources Technology, Shanghai Institute of Space Power-Sources, Shanghai 200245, China
CAS Key Laboratory of Materials for Energy Conversion, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China
Department of Mechanical Engineering, National University of Singapore, Singapore 117575, Singapore
National University of Singapore Suzhou Research Institute, Suzhou 215024, China
School of Mechanical Engineering, Hebei University of Technology, Tianjin 300401, China
State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400044, China
Authors to whom correspondence should be addressed.
These authors contributed equally to this work.
Nanomaterials 2019, 9(5), 721;
Received: 18 March 2019 / Revised: 28 April 2019 / Accepted: 8 May 2019 / Published: 10 May 2019
PDF [3101 KB, uploaded 10 May 2019]


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. View Full-Text
Keywords: garnet; dual substitution; spark plasma sintering; conductivity garnet; dual substitution; spark plasma sintering; conductivity

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Dong, Z.; Xu, C.; Wu, Y.; Tang, W.; Song, S.; Yao, J.; Huang, Z.; Wen, Z.; Lu, L.; Hu, N. Dual Substitution and Spark Plasma Sintering to Improve Ionic Conductivity of Garnet Li7La3Zr2O12. Nanomaterials 2019, 9, 721.

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