Interface engineering enabling thin lithium metal electrodes down to 0.78 μm for garnet-type solid-state batteries

Weijie Ji, Bi Luo, Qi Wang, Guihui Yu, Zixun Zhang, Yi Tian, Zaowen Zhao, Ruirui Zhao, Shubin Wang, Xiaowei Wang (), Bao Zhang, Jiafeng Zhang (), Zhiyuan Sang and Ji Liang ()
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Weijie Ji: Central South University
Bi Luo: Central South University
Qi Wang: Central South University
Guihui Yu: Central South University
Zixun Zhang: Central South University
Yi Tian: Central South University
Zaowen Zhao: Hainan University
Ruirui Zhao: South China Normal University
Shubin Wang: Ministry of Ecology and Environment (MEE)
Xiaowei Wang: Central South University
Bao Zhang: Central South University
Jiafeng Zhang: Central South University
Zhiyuan Sang: Peking University
Ji Liang: Tianjin University

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract Controllable engineering of thin lithium (Li) metal is essential for increasing the energy density of solid-state batteries and clarifying the interfacial evolution mechanisms of a lithium metal negative electrode. However, fabricating a thin lithium electrode faces significant challenges due to the fragility and high viscosity of Li metal. Herein, through facile treatment of Ta-doped Li7La3Zr2O12 (LLZTO) with trifluoromethanesulfonic acid, its surface Li2CO3 species is converted into a lithiophilic layer with LiCF3SO3 and LiF components. It enables the thickness control of Li metal negative electrodes, ranging from 0.78 μm to 30 μm. Quasi-solid-state lithium-metal battery with an optimized 7.54 μm-thick lithium metal negative electrode, a commercial LiNi0.83Co0.11Mn0.06O2 positive electrode, and a negative/positive electrode capacity ratio of 1.1 shows a 500 cycles lifespan with a final discharge specific capacity of 99 mAh g−1 at 2.35 mA cm−2 and 25 °C. Through multi-scale characterizations of the thin lithium negative electrode, we clarify the multi-dimensional compositional evolution and failure mechanisms of lithium-deficient and -rich regions (0.78 μm and 7.54 μm), on its surface, inside it, or at the Li/LLZTO interface.

Date: 2024
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DOI: 10.1038/s41467-024-54234-w

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