Visualizing the failure of solid electrolyte under GPa-level interface stress induced by lithium eruption

Haowen Gao, Xin Ai, Hongchun Wang, Wangqin Li, Ping Wei, Yong Cheng, Siwei Gui, Hui Yang (), Yong Yang and Ming-Sheng Wang ()
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Haowen Gao: Xiamen University
Xin Ai: Huazhong University of Science and Technology
Hongchun Wang: Xiamen University
Wangqin Li: Xiamen University
Ping Wei: Xiamen University
Yong Cheng: Xiamen University
Siwei Gui: Huazhong University of Science and Technology
Hui Yang: Huazhong University of Science and Technology
Yong Yang: Xiamen University
Ming-Sheng Wang: Xiamen University

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract Solid electrolytes hold the promise for enabling high-performance lithium (Li) metal batteries, but suffer from Li-filament penetration issues. The mechanism of this rate-dependent failure, especially the impact of the electrochemo-mechanical attack from Li deposition, remains elusive. Herein, we reveal the Li deposition dynamics and associated failure mechanism of solid electrolyte by visualizing the Li|Li7La3Zr2O12 (LLZO) interface evolution via in situ transmission electron microscopy (TEM). Under a strong mechanical constraint and low charging rate, the Li-deposition-induced stress enables the single-crystal Li to laterally expand on LLZO. However, upon Li “eruption”, the rapidly built-up local stress, reaching at least GPa level, can even crack single-crystal LLZO particles without apparent defects. In comparison, Li vertical growth by weakening the mechanical constraint can boost the local current density up to A·cm−2 level without damaging LLZO. Our results demonstrate that the crack initiation at the Li|LLZO interface depends strongly on not only the local current density but also the way and efficiency of mass/stress release. Finally, potential strategies enabling fast Li transport and stress relaxation at the interface are proposed for promoting the rate capability of solid electrolytes.

Date: 2022
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DOI: 10.1038/s41467-022-32732-z

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