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Designing three-dimensional lithiophilic dual-skeletons-supported lithium metal anodes for long-life lithium metal batteries

长寿命锂电池用三维亲锂双骨架支撑锂金属负极的设计

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Abstract

Lithium metal is one of the most promising anode materials for use in the next generation of high-energy lithium batteries. However, uneven Li deposition and large volume changes severely restrict the practical use of lithium metal anodes. Here, a dendrite-free three-dimensional (3D) composite Li anode (Li-B-Sn) with dual-skeletons was produced by a simple melting method. The unique dual-skeleton structure was composed of LiB fiber phase and Li22Sn5 phase, which enabled even Li stripping and plating processes and reduced the volume variations to improve the performance of the Li-B-Sn anode. The Li-B-Sn anode exhibited a long lifespan of 1100 h during cycling operating under a large areal capacity of 10 mA h cm−2 in a symmetrical cell. In addition, full batteries assembled with the high mass loading LiFePO4 cathode (∼11 mg cm−2) and the Li-B-Sn composite anode showed superior electrochemical performance, with a high capacity retention of 92.5% at 2 C after 430 cycles. Li-S pouch cells based on the Li-B-Sn composite anode survived over 30 cycles, which constituted better cycling stability than that of the Li-B anode. This work describes new 3D skeletons for practical use in lithium metal batteries.

摘要

锂金属被认为是下一代高能锂电池最有前途的负极材料之一. 然而, 锂的不均匀沉积和巨大的体积变化严重限制了锂金属阳极的实际应用. 本文采用简单的熔融法制备了无枝晶的双骨架三维复合锂负极(Li-B-Sn). Li-B-Sn复合负极独特的双骨架结构由LiB纤维相和Li22Sn5 相组成, 有利于锂的均匀脱除和沉积, 减小了体积变化, 提高了Li-B-Sn负极的性能. 在对称电池中, Li-B-Sn负极在10 mA cm−2的大面积容量下实现了1100h的长循环寿命. 此外, 高负载的LiFePO4正极 (~11 mg cm−2)和Li-B-Sn复合负极组装的全电池表现出优异的电化学性能, 在2C循环430次后, 容量保持率高达92.5%. 基于Li-B-Sn复合负极的Li-S软包电池循环寿命超过30圈, 表现出比基于Li-B负极的Li-S软包电池更好的循环稳定性. 三维骨架设计为锂金属电池的实际应用带来了新思路.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (U1904216 and U22A20141), the Natural Science Foundation of Changsha City (kq2208258), and the Natural Science Foundation of Hunan Province (2022JJ20068). The authors thank the shiyanjia lab for the microcomputed tomography (https://www.shiyanjia.com).

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Authors and Affiliations

  1. State Key Laboratory of Powder Metallurgy, Central South University, Changsha, 410083, China

    Xinsheng Liu  (刘鑫胜), Kecheng Long  (龙科成), Piao Qing  (青飘), Shaozhen Huang  (黄绍祯), Pengfei Xiao  (肖鹏飞), Canhui Ling  (凌灿辉), Zhibin Wu  (吴志彬) & Libao Chen  (陈立宝)

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  1. Xinsheng Liu  (刘鑫胜)
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  2. Kecheng Long  (龙科成)
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  3. Piao Qing  (青飘)
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  4. Shaozhen Huang  (黄绍祯)
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  5. Pengfei Xiao  (肖鹏飞)
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  6. Canhui Ling  (凌灿辉)
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  7. Zhibin Wu  (吴志彬)
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  8. Libao Chen  (陈立宝)
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Contributions

Author contributions Liu X designed the experiments and wrote the manuscript. Long K, Qing P, and Huang S participated in the testing of the experiment. Xiao P and Ling C participated in the writing of the manuscript. Wu Z and Chen L guided the research and reviewed the manuscript. All authors participated in the discussion.

Corresponding authors

Correspondence to Zhibin Wu  (吴志彬) or Libao Chen  (陈立宝).

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Conflict of interest The authors declare that they have no conflict of interest.

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Supplementary information Supporting data are available in the online version of the paper.

Xinsheng Liu received the Bachelor of Engineering degree from the Central South University in 2021. At present, he is studying for a Master’s degree in the research group of Prof. Libao Chen at the Central South University, and his research interest mainly focuses on the application of lithium metal batteries.

Zhibin Wu is now a lecturer at the Central South University, China. He obtained his PhD degree in 2021 from the University of Wollongong, Australia. His current research interests mainly focus on lithium metal batteries, low-temperature lithium-ion batteries, and their electrochemical mechanism studies based on synchrotron-based X-ray techniques.

Libao Chen is a professor at the Institute of Powder Metallurgy, Central South University, China. He received his PhD degree in materials physics and chemistry from Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences in 2007. His research interests mainly focus on high-performance electrode materials and electrochemical energy storage systems, including lithium-ion batteries, lithium metal batteries, and Zn batteries.

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Liu, X., Long, K., Qing, P. et al. Designing three-dimensional lithiophilic dual-skeletons-supported lithium metal anodes for long-life lithium metal batteries. Sci. China Mater. 66, 4349–4356 (2023). https://doi.org/10.1007/s40843-023-2575-3

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