Synergy of I-Cl co-occupation on halogen-rich argyrodites and resultant dual-layer interface for advanced all-solid-state Li metal batteries

doi:10.1016/j.jechem.2023.07.028

Abstract

Abstract: The (electro)chemical stability and Li dendrite suppression capability of sulfide solid electrolytes (SEs) need further improvement for developing all-solid-state Li batteries (ASSLBs). Here, we report advanced halogen-rich argyrodites via I and Cl co-occupation on the crystal lattice. Notably, a proper I content forms a single phase, whereas an excessive I causes precipitation of two argyrodite phases like a superlattice structure. The resultant synergistic effect of the optimized composition allows to gain high ionic conductivities at room temperature and -20 °C, and enhances the (electro)chemical stability against Li and Li dendrite suppression capability. The Li|argyrodite interface is very sensitive to the ratio of I and Cl. A LiCl- and LiI-rich double-layer interface is observed from the cell using the SE with optimized composition, whereas too high I content forms only a single interface layer with a mixture of LiI and LiCl. This double-layer interface is found to effectively mitigate the Li/SE reaction. The proper designed argyrodite enables ASSLBs to achieve good electrochemical properties at a broad temperature range regardless of the electrode materials. This co-occupation strategy provides a novel exploration for advanced halogen-rich argyrodite system.

Key words: Sulfide solid electrolytes, Argyrodites, Dual doping, Li metal anode, Solid-state batteries

Han Yan, Ruifeng Song, Ruonan Xu, Shulin Li, Qiaoquan Lin, Xinlin Yan, Zhenyu Wang, Chuang Yu, Long Zhang. Synergy of I-Cl co-occupation on halogen-rich argyrodites and resultant dual-layer interface for advanced all-solid-state Li metal batteries[J]. Journal of Energy Chemistry, 2023, 86(11): 499-509.

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URL: https://www.jenergychem.com/EN/10.1016/j.jechem.2023.07.028

https://www.jenergychem.com/EN/Y2023/V86/I11/499

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