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Effect of Li₆.₄La₃Zr₁.₄Ta₀.₆O₁₂ Fillers on the Interfacial Properties between Composite PEO-LiTFSI Electrolytes with Li Metal during Cycling.

Zhang, Lun; Feng, Junrun; Zhu, Guanghan; Yan, Jay; Bartlett, Stuart; Wang, Zhipeng; Hao, Zhangxiang; ... Wang, Ryan; + view all (2024) Effect of Li₆.₄La₃Zr₁.₄Ta₀.₆O₁₂ Fillers on the Interfacial Properties between Composite PEO-LiTFSI Electrolytes with Li Metal during Cycling. ACS Applied Materials and Interfaces , 16 (11) pp. 13786-13794. 10.1021/acsami.3c19519.

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Abstract

PEO-LiX solid polymer electrolyte (SPE) with the addition of Li₆.₄La₃Zr₁.₄Ta₀.₆O₁₂ (LLZTO) fillers is considered as a promising solid-state electrolyte for solid-state Li-ion batteries. However, the developments of the SPE have caused additional challenges, such as poor contact interface and SPE/Li interface stability during cycling, which always lead to potentially catastrophic battery failure. The main problem is that the real impact of LLZTO fillers on the interfacial properties between SPE and Li metal is still unclear. Herein, we combined the electrochemical measurement and in situ synchrotron-based X-ray absorption near-edge structure (XANES) imaging technology to study the role of LLZTO fillers in directing SPE/Li interface electrochemical performance. In situ XRF-XANES mapping during cycling showed that addition of an appropriate amount of LLZTO fillers (50 wt %) can improve the interfacial contact and stability between SPE and Li metal without reacting with the PEO and Li salts. Additionally, it also demonstrated the beneficial effect of LLZTO particles for suppressing the interface reactions between the Li metal and PEO-LiTFSI SPE and further inhibiting Li-metal dendrite growth. The Li|LiFePO₄ batteries deliver long cycling for over 700 cycles with a low-capacity fade rate of 0.08% per cycle at a rate of 0.3C, revealing tremendous potential in promoting the large-scale application of future solid-state Li-ion batteries.

Type: Article
Title: Effect of Li₆.₄La₃Zr₁.₄Ta₀.₆O₁₂ Fillers on the Interfacial Properties between Composite PEO-LiTFSI Electrolytes with Li Metal during Cycling.
Location: United States
DOI: 10.1021/acsami.3c19519
Publisher version: https://doi.org/10.1021/acsami.3c19519
Language: English
Additional information: This version is the author-accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: solid polymer electrolytes all-solid-state lithium-ion battery Li₆.₄La₃Zr₁.₄Ta₀.₆O₁₂
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/10190731
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