Promoting favorable interfacial properties in lithium-based batteries using chlorine-rich sulfide inorganic solid-state electrolytes

Dewu Zeng, Jingming Yao, Long Zhang (), Ruonan Xu, Shaojie Wang, Xinlin Yan, Chuang Yu and Lin Wang
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Dewu Zeng: Yanshan University
Jingming Yao: Yanshan University
Long Zhang: Yanshan University
Ruonan Xu: Yanshan University
Shaojie Wang: Yanshan University
Xinlin Yan: Vienna University of Technology
Chuang Yu: Huazhong University of Science and Technology
Lin Wang: Yanshan University

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

Abstract: Abstract The use of inorganic solid-state electrolytes is considered a viable strategy for developing high-energy Li-based metal batteries. However, suppression of parasitic interfacial reactions and growth of unfavorable Li metal depositions upon cycling are challenging aspects and not yet fully addressed. Here, to better understand these phenomena, we investigate various sulfide inorganic solid electrolytes (SEs), i.e., Li7−xPS6−xClx (x = 0.6, 1.0, 1.3, 1.45, and 1.6), via ex situ and in situ physicochemical and electrochemical measurements. We found that the Cl distribution and the cooling process applied during the SE synthesis strongly influence the evolution of the Li|SE interface in terms of microstructure, interphase composition, and morphology. Indeed, for a SE with a moderate chlorine content (i.e., x = 1.3) and obtained via a slow cooling process after sintering, the Cl atoms are located on the surface of the SE grains as interconnected LiCl nanoparticles that form an extended LiCl-based framework. This peculiar microstructure facilitates the migration of the Cl ions to the Li|SE interface during electrochemical cycling, thus, favouring the formation of a LiCl-rich interphase layer capable of improving the battery cycling performances.

Date: 2022
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DOI: 10.1038/s41467-022-29596-8

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