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A lithium–tin fluoride anode enabled by ionic/electronic conductive paths for garnet-based solid-state lithium metal batteries

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Abstract

The high energy density and stability of solid-state lithium metal batteries (SSLMBs) have garnered great attention. Garnet-type oxides, especially Li6.4La3Zr1.4Ta0.6O12 (LLZTO), with high ionic conductivity, wide electrochemical window, and stability to Li metal anode, are promising solid-state electrolyte (SSEs) materials for SSLMBs. However, Li/LLZTO interface issues including high interface resistance, inhomogeneous Li deposition, and Li dendrite growth have hindered the practical application of SSLMBs. Herein, a multi-functional Li–SnF2 composite anode with Li, LiF, and Li-Sn alloy was specifically designed and prepared. The composite anode improves the wettability to LLZTO, constructing an intimate contact interface between it and LLZTO. Meanwhile, ionic/electronic conductive paths in situ formed at the interface can effectively uniform Li deposition and suppress Li dendrite. The solid-state symmetric cell exhibits low interface resistance (11 Ω·cm2) and high critical current density (1.3 mA·cm−2) at 25 °C. The full SSLMB based on LiFePO4 or LiNi0.5Co0.2Mn0.3O2 cathode also shows stable cycling performance and high rate capability. This work provides a new composite anode strategy for achieving high-energy density and high-safety SSLMBs.

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摘要

固态锂金属电池(SSLMBs) 因其高能量密度和稳定性引起了人们的兴趣。石榴石型氧化物特别是Li6.4La3Zr1.4Ta0.6O12(LLZTO) 因其高的离子电导率、宽的电化学窗口、和对锂金属负极的稳定性而成为SSLMBs有前途的固态电解质 (SSEs) 材料。然而, Li/LLZTO界面存在高的界面电阻、锂的不均匀沉积和锂枝晶生长等问题, 严重阻碍了SSLMBs的实际应用。本研究专门设计并制备了一种由Li、LiF、和Li − Sn合金共同构成的多功能Li − SnF2复合负极。一方面, 该复合负极改善了其对LLZTO的润湿能力, 从而使负极/LLZTO界面紧密接触。另一方面, 在界面处原位形成的离子/电子导电通道能够有效地均匀锂沉积和抑制锂枝晶。固态对称电池在室温下显示出低的界面电阻 (11 Ω·cm2) 和高的临界电流密度 (1.3 mA·cm−2) 。匹配LiFePO4或LiNi0.5Co0.2Mn0.3O2正极的全SSLMB同样表现出稳定的循环和倍率性能。因此, 这项工作为实现高能量密度和高安全性的SSLMB提供了一种新的复合负极策略。

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (Nos. 52177208, 52171202, 51971055 and 51871046) and the National Safety Academic Fund (Nos. U1930208, U2030206 and U1730136).

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Authors and Affiliations

  1. School of Materials Science and Engineering, Northeastern University, Shenyang, 110819, China

    Lei Zhang, Xiang-Ping Feng, Ming Shen, Run-Guo Zheng, Zhi-Yuan Wang & Yan-Guo Liu

  2. School of Resources and Materials, Northeastern University at Qinhuangdao, Qinhuangdao, 066004, China

    Lei Zhang, Xiang-Ping Feng, Ming Shen, Run-Guo Zheng, Zhi-Yuan Wang, Hong-Yu Sun & Yan-Guo Liu

  3. School of Materials and Physics, China University of Mining & Technology, Xuzhou, 221116, China

    Qian-Kun Meng, Yu-Qing Zhang & Quan-Chao Zhuang

  4. Institute of Electronic Engineering, China Academy of Engineering Physics, Mianyang, 621900, China

    Yan-Hua Cui

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Zhang, L., Meng, QK., Feng, XP. et al. A lithium–tin fluoride anode enabled by ionic/electronic conductive paths for garnet-based solid-state lithium metal batteries. Rare Met. 43, 575–587 (2024). https://doi.org/10.1007/s12598-023-02468-w

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