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Recycling of garnet solid electrolytes with lithium-dendrite penetration by thermal healing

通过热愈合方法回收被锂枝晶刺穿的石榴石型固态电解质

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Abstract

Solid-state lithium metal batteries (SSLMBs) have attracted a lot of interest owing to their high safety and high energy density potential. However, the growth of lithium dendrite in solid electrolytes still hinders practical applications of SSLMBs. In this study, we develop a simple heat treatment method for reviving and recycling garnet oxide electrolytes with Li dendrite penetration. Interestingly, the recovered garnet electrolyte exhibits higher relative density, enhanced ionic conductivity and improved critical current density compared with the pristine one. The thermal healing is due to the products of the reaction between dendritic Li metal and air that contribute to the further densification of garnet electrolytes during heat treatment. This work demonstrates a new way to recycle garnet electrolytes, which may further extend to other various solid electrolytes.

摘要

固态锂金属电池(SSLMBs)因其高安全性和潜在的高能量密度引起了广泛的兴趣. 然而, 锂枝晶在固态电解质中的生长严重阻碍了SSLMBs的实际应用. 在本文中, 我们开发了一种简单的方法, 通过热处理修复和回收被锂枝晶刺穿的石榴石氧化物电解质. 与初始对照样相比, 回收后的石榴石电解质表现出更高的相对密度、离子电导率和临界电流密度. 热愈合是基于树突状锂枝晶和空气间的反应产物, 其有助于在热处理过程中石榴石电解质的进一步致密化. 这项工作为石榴石型固态电解质的回收利用开辟了一条新的途径.

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Acknowledgements

This work was partially supported by Shanghai Rising-Star Program (20QA1406600). We also acknowledge the Centre for High-resolution Electron Microscopy (CℏEM), School of Physical Science and Technology, ShanghaiTech University (EM02161943), Shanghai Science and Technology Plan (21DZ2260400) and Double-Class Initiative Fund of ShanghaiTech University for support.

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Authors and Affiliations

Authors

Contributions

Chen S and Hu X contributed to the experiments and editing; Nie L contributed to the discussion; Yu Y and Liu W were in charge of the scientific research project. All authors contributed to the general discussion.

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Correspondence to Wei Liu  (刘巍).

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The authors declare that they have no conflict of interest.

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

Shaojie Chen received his BS degree in materials science and engineering from Zhejiang Sci-Tech University in 2018. He then joined the School of Physical Science and Technology at ShanghaiTech University under the supervision of Prof. Wei Liu. His research interests focus on solid-state lithium metal batteries and lithium-sulfur batteries.

Xiangchen Hu received his BE degree in materials science and engineering from Shanghaitech University in 2018. He then joined the School of Physical Science and Technology at Shanghaitech University under the supervision of Prof. Yi Yu. His research focuses on the aberration-corrected TEM characterization on beam-sensitive materials (halide perovskite and lithium batteries).

Wei Liu received her BS degree in materials physics from Beijing Normal University in 2008 and her PhD degree in materials science and engineering from Tsinghua University in 2013. She visited the University of Tokyo during 2010–2011. From 2013 to 2017, she was a postdoctoral scholar at Stanford University. She joined ShanghaiTech University as an assistant professor in 2017. Her research interests cover the area of solid-state ionics and nanotechnology, with a focus on the studies of lithium batteries.

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Chen, S., Hu, X., Nie, L. et al. Recycling of garnet solid electrolytes with lithium-dendrite penetration by thermal healing. Sci. China Mater. 66, 2192–2198 (2023). https://doi.org/10.1007/s40843-022-2371-9

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