4.7 Article

Liquid sintering of garnet electrolytes by lithium germanate: Properties and interfacial performance with lithium anode

Journal

APPLIED SURFACE SCIENCE
Volume 575, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apsusc.2021.151762

Keywords

Garnet electrolytes; Sintering temperature; Microstructure; Electrolyte/Li interface; Electrical performance

Funding

  1. National Natural Science Foundation of China (NSFC) [51805112, 51974101, 51975150]
  2. Natural Science Foundation of Heilongjiang Province, China [LH2020E037]
  3. China Postdoctoral Science Foundation [2019T120261, 2018M630349]

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By using a liquid sintering method with a specific additive, stable LLZTO ceramics with excellent conductivity and mechanical properties can be successfully prepared, suitable for electrolyte/Li interface design to enhance the performance of solid-state lithium batteries.
Garnet electrolytes have been approved widespread as one of the most competitive candidates in all solid state lithium batteries (ASSLBs). Herein, dense Li6.4La3Zr1.4Ta0.6O12 (LLZTO) ceramics were successfully produced via liquid sintering method by introducing 1 wt% 3Li(2)O-2GeO(2) additive at reduced sintering temperatures for a shortened process period compared to solid method in air atmosphere. Relationships among sintering temperature, microstructure, densities, mechanical properties and electrical performance of the ceramics were explored concretely. The ceramics can be well densified and modified microstructurally at the appropriate sintering temperature, making the ionic conductivity significantly promoted. Mechanical properties would be enhanced as well, resulted to a compact and tough ceramic surface. Hence, a good-contacted, homogeneous and electrochemically stable electrolyte/Li interface can be fabricated. The LLZTO-1 wt% (3Li(2)O-2GeO(2)) composite electrolyte sintered at 1160 degrees C for 3 h exhibits the best comprehensive properties, the ionic conductivity and critical current density (CCD) of which reach 6.27 x 10(-4) S.cm(-1) and 0.5 mA.cm(-2) at 25 degrees C. The improved interfacial performance enables the Li|LLZTO-1 wt% (3Li(2)O-2GeO(2))|Li symmetrical cells and the LiFePO4|LLZTO-1 wt% (3Li(2)O-2GeO(2))|Li cells a good cycling performance at different current densities.

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