Reinforced cathode-garnet interface for high-capacity all-solid-state batteries

Chenxi Zheng; Shijun Tang; Fangmei Wen; Jinxue Peng; Wu Yang; Zhongwei Lv; Yongmin Wu; Weiping Tang; Zhengliang Gong; Yong Yang

doi:10.1088/2752-5724/aca110

Volume 1 Issue 4

December 2022

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Chenxi Zheng, Shijun Tang, Fangmei Wen, Jinxue Peng, Wu Yang, Zhongwei Lv, Yongmin Wu, Weiping Tang, Zhengliang Gong, Yong Yang. Reinforced cathode-garnet interface for high-capacity all-solid-state batteries[J]. Materials Futures, 2022, 1(4): 045103. doi: 10.1088/2752-5724/aca110

Citation:

Chenxi Zheng, Shijun Tang, Fangmei Wen, Jinxue Peng, Wu Yang, Zhongwei Lv, Yongmin Wu, Weiping Tang, Zhengliang Gong, Yong Yang. Reinforced cathode-garnet interface for high-capacity all-solid-state batteries[J]. Materials Futures, 2022, 1(4): 045103. doi: 10.1088/2752-5724/aca110

Citation:

Chenxi Zheng, Shijun Tang, Fangmei Wen, Jinxue Peng, Wu Yang, Zhongwei Lv, Yongmin Wu, Weiping Tang, Zhengliang Gong, Yong Yang. Reinforced cathode-garnet interface for high-capacity all-solid-state batteries[J]. Materials Futures, 2022, 1(4): 045103. doi: 10.1088/2752-5724/aca110

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Reinforced cathode-garnet interface for high-capacity all-solid-state batteries

Materials Futures, Volume 1, Number 4

Received Date: 2022-10-24
Accepted Date: 2022-11-08
Publish Date: 2022-12-09

Article information

doi: 10.1088/2752-5724/aca110

1 College of Energy, Xiamen University, Xiamen 361102, People’s Republic of China
2 State Key Laboratory of Space Power-Sources Technology, Shanghai Institute of Space Power-Sources, Shanghai 200245, People’s Republic of China
3 State Key Laboratory for Physical Chemistry of Solid Surface, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, People’s Republic of China

Funds:

This work was supported by the National Key R&D Program of China (Grant No. 2021YFB2401800), the National Natural Science Foundation of China (Grants Nos. 21875196, 22279108, 21935009 and 22021001) and the Fundamental Research Funds for Xiamen University (No. 20720202019).

Abstract

Abstract

Garnet-type solid-state electrolytes (SSEs) are particularly attractive in the construction of all-solid-state lithium (Li) batteries due to their high ionic conductivity, wide electrochemical window and remarkable (electro)chemical stability. However, the intractable issues of poor cathode/garnet interface and general low cathode loading hinder their practical application. Herein, we demonstrate the construction of a reinforced cathode/garnet interface by spark plasma sintering, via co-sintering Li_6.5La₃Zr_1.5Ta_0.5O₁₂ (LLZTO) electrolyte powder and LiCoO₂/LLZTO composite cathode powder directly into a dense dual-layer with 5 wt% Li₃BO₃ as sintering additive. The bulk composite cathode with LiCoO₂/LLZTO cross-linked structure is firmly welded to the LLZTO layer, which optimizes both Li-ion and electron transport. Therefore, the one-step integrated sintering process implements an ultra-low cathode/garnet interfacial resistance of 3.9 Ω cm² (100 °C) and a high cathode loading up to 2.02 mAh cm⁻². Moreover, the Li₃BO₃ reinforced LiCoO₂/LLZTO interface also effectively mitigates the strain/stress of LiCoO₂, which facilitates the achieving of superior cycling stability. The bulk-type Li|LLZTO|LiCoO₂-LLZTO full cell with areal capacity of 0.73 mAh cm⁻² delivers capacity retention of 81.7% after 50 cycles at 100 μA cm⁻². Furthermore, we reveal that non-uniform Li plating/stripping leads to the formation of gaps and finally results in the separation of Li and LLZTO electrolyte during long-term cycling, which becomes the dominant capacity decay mechanism in high-capacity full cells. This work provides insight into the degradation of Li/SSE interface and a strategy to radically improve the electrochemical performance of garnet-based all-solid-state Li batteries.
- garnet electrolyte,
- all-solid-state battery,
- high cathode loading,
- interface evolution,
- spark plasma sintering

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References(49)

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