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Garnet-type oxide is one of the most promising solid-state electrolytes (SSEs) for solid-state lithium-metal batteries (SSLMBs). However, the Li dendrite formation in garnet oxides obstructs the further development of the SSLMBs seriously. Here, we report a high-performance garnet oxide by using AlN as a sintering additive and Li as an anode interface layer. AlN with high thermal conductivity can promote the sintering activity of the garnet oxides, resulting in larger particle size and higher relative density. Moreover, Li3N with high ionic conductivity formed at grain boundaries and interface can also improve Li-ion transport kinetics. As a result, the garnet oxide electrolytes with AlN show enhanced thermal conductivity, improved ionic conductivity, reduced electronic conductivity, and increased critical current density (CCD), compared with the counterpart using Al2O3 sintering aid. In addition, Li symmetric cells and Li|LiFePO4 (Li|LFP) half cells using the garnet electrolyte with the AlN additive exhibit good electrochemical performances. This work provides a simple and effective strategy for high-performance SSEs.


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High-performance Ta-doped Li7La3Zr2O12 garnet oxides with AlN additive

Show Author's information Chang ZHANGa,bXiangchen HUaZhiwei NIEaCong WUaNan ZHENGaShaojie CHENaYihang YANGaRan WEIaJiameng YUaNan YANGaYi YUa,bWei LIUa,b( )
School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China
Shanghai Key Laboratory of High-resolution Electron Microscopy, ShanghaiTech University, Shanghai 201210, China

Abstract

Garnet-type oxide is one of the most promising solid-state electrolytes (SSEs) for solid-state lithium-metal batteries (SSLMBs). However, the Li dendrite formation in garnet oxides obstructs the further development of the SSLMBs seriously. Here, we report a high-performance garnet oxide by using AlN as a sintering additive and Li as an anode interface layer. AlN with high thermal conductivity can promote the sintering activity of the garnet oxides, resulting in larger particle size and higher relative density. Moreover, Li3N with high ionic conductivity formed at grain boundaries and interface can also improve Li-ion transport kinetics. As a result, the garnet oxide electrolytes with AlN show enhanced thermal conductivity, improved ionic conductivity, reduced electronic conductivity, and increased critical current density (CCD), compared with the counterpart using Al2O3 sintering aid. In addition, Li symmetric cells and Li|LiFePO4 (Li|LFP) half cells using the garnet electrolyte with the AlN additive exhibit good electrochemical performances. This work provides a simple and effective strategy for high-performance SSEs.

Keywords: thermal conductivity, electronic conductivity, solid-state lithium-metal battery (SSLMB), garnet oxide, critical current density (CCD)

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Publication history

Received: 09 March 2022
Revised: 21 June 2022
Accepted: 21 June 2022
Published: 24 August 2022
Issue date: October 2022

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© The Author(s) 2022.

Acknowledgements

The authors gratefully acknowledge financial support from the National Key R&D Program of China (No. 2019YFA0210600), the National Natural Science Foundation of China (No. 21805185), Shanghai Science and Technology Plan (No. 21DZ2260400), and Shanghai Rising-Star Program (No. 20QA1406600). We also acknowledge Center for High-resolution Electron Microscopy, SPST of ShanghaiTech University (No. EM02161943) for support.

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