Reduced Energy Barrier for Li+ Transport Across Grain Boundaries with Amorphous Domains in LLZO Thin Films

Yanlin ZHU; Shuai WU; Yilan PAN; Xiaokun ZHANG; Zongkai YAN; Yong XIANG

doi:10.1186/s11671-020-03378-x

Reduced Energy Barrier for Li⁺ Transport Across Grain Boundaries with Amorphous Domains in LLZO Thin Films

Yanlin ZHU, Shuai WU, Yilan PAN, Xiaokun ZHANG^*, Zongkai YAN^*, Yong XIANG^*

^*Corresponding author for this work

Research output: Journal Publications › Journal Article (refereed) › peer-review

39 Citations (Scopus)

Abstract

The high-resistive grain boundaries are the bottleneck for Li⁺ transport in Li₇La₃Zr₂O₁₂ (LLZO) solid electrolytes. Herein, high-conductive LLZO thin films with cubic phase and amorphous domains between crystalline grains are prepared, via annealing the repetitive LLZO/Li₂CO₃/Ga₂O₃ multi-nanolayers at 600 °C for 2 h. The amorphous domains may provide additional vacant sites for Li⁺, and thus relax the accumulation of Li⁺ at grain boundaries. The significantly improved ionic conductivity across grain boundaries demonstrates that the high energy barrier for Li⁺ migration caused by space charge layer is effectively reduced. Benefiting from the Li⁺ transport paths with low energy barriers, the presented LLZO thin film exhibits a cutting-edge value of ionic conductivity as high as 6.36 × 10⁻⁴ S/cm, which is promising for applications in thin film lithium batteries.

Original language	English
Article number	153
Number of pages	8
Journal	Nanoscale Research Letters
Volume	15
Issue number	1
Early online date	25 Jul 2020
DOIs	https://doi.org/10.1186/s11671-020-03378-x
Publication status	Published - Dec 2020
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2020, The Author(s).

Funding

This research work was financially supported by the National Science Funds of China (Grant No. 21905040), the Fundamental Research Funds for Central Universities (Contract No. ZYGX2019Z009), and the startup funds from the University of Electronic Science and Technology of China. Acknowledgements

Keywords

Energy barrier
Ionic conductivity
LLZO
Solid electrolytes
Thin film

Access to Document

10.1186/s11671-020-03378-xLicence: CC BY

Cite this

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title = "Reduced Energy Barrier for Li+ Transport Across Grain Boundaries with Amorphous Domains in LLZO Thin Films",

abstract = "The high-resistive grain boundaries are the bottleneck for Li+ transport in Li7La3Zr2O12 (LLZO) solid electrolytes. Herein, high-conductive LLZO thin films with cubic phase and amorphous domains between crystalline grains are prepared, via annealing the repetitive LLZO/Li2CO3/Ga2O3 multi-nanolayers at 600 °C for 2 h. The amorphous domains may provide additional vacant sites for Li+, and thus relax the accumulation of Li+ at grain boundaries. The significantly improved ionic conductivity across grain boundaries demonstrates that the high energy barrier for Li+ migration caused by space charge layer is effectively reduced. Benefiting from the Li+ transport paths with low energy barriers, the presented LLZO thin film exhibits a cutting-edge value of ionic conductivity as high as 6.36 × 10−4 S/cm, which is promising for applications in thin film lithium batteries.",

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AU - ZHU, Yanlin

AU - WU, Shuai

AU - PAN, Yilan

AU - ZHANG, Xiaokun

AU - YAN, Zongkai

AU - XIANG, Yong

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AB - The high-resistive grain boundaries are the bottleneck for Li+ transport in Li7La3Zr2O12 (LLZO) solid electrolytes. Herein, high-conductive LLZO thin films with cubic phase and amorphous domains between crystalline grains are prepared, via annealing the repetitive LLZO/Li2CO3/Ga2O3 multi-nanolayers at 600 °C for 2 h. The amorphous domains may provide additional vacant sites for Li+, and thus relax the accumulation of Li+ at grain boundaries. The significantly improved ionic conductivity across grain boundaries demonstrates that the high energy barrier for Li+ migration caused by space charge layer is effectively reduced. Benefiting from the Li+ transport paths with low energy barriers, the presented LLZO thin film exhibits a cutting-edge value of ionic conductivity as high as 6.36 × 10−4 S/cm, which is promising for applications in thin film lithium batteries.

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