Metastable Decomposition Realizing Dendrite‐Free Solid‐State Li Metal Batteries

A stable interface and preventing dendrite‐growth are two crucial factors to realize long‐life all‐solid‐state Li batteries (ASSLBs) using sulfide‐based solid electrolytes (SEs) and Li metal anodes. But it remains a challenge to accomplish the two factors simultaneously. Here, an effective strategy...

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Bibliographic Details
Published in:Advanced energy materials 2023-03, Vol.13 (9), p.n/a
Main Authors: Song, Ruifeng, Yao, Jingming, Xu, Ruonan, Li, Zhixuan, Yan, Xinlin, Yu, Chuang, Huang, Zhigao, Zhang, Long
Format: Article
Language:English
Subjects:
Anodes
argyrodite solid electrolytes
Crystal growth
Decomposition
Decomposition reactions
Grain boundaries
interfaces
interphases
Lithium batteries
lithium dendrites
metastable decomposition
Molten salt electrolytes
Room temperature
Solid electrolytes
SSLMBs
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Summary:A stable interface and preventing dendrite‐growth are two crucial factors to realize long‐life all‐solid‐state Li batteries (ASSLBs) using sulfide‐based solid electrolytes (SEs) and Li metal anodes. But it remains a challenge to accomplish the two factors simultaneously. Here, an effective strategy is reported to realize this goal in Li‐argyrodites via self‐engineered metastable decomposition that is enabled by Si doping in Cl‐rich argyrodites. It is shown that Cl atoms in the lattice become metastable and are highly reactive with Li atoms. The locally deposited/grown Li crystal nuclei are thus depleted by the metastable Cl during electrochemical cycling, in situ generating electrically insulated LiCl shells concentrated at the argyrodite grain boundaries. The shells in turn prevent the autochthonous Li redeposition and act as self‐protective layers to restrain the continuous decomposition in the interior argyrodite, that is, self‐assembly of reactive‐cores‐stable‐shells to Li metal, thereby enabling an ultra‐long life ASSLB using Li metal anodes at room temperature under relatively high current densities. Si‐doping‐ignited metastable Cl atoms are highly reactive with deposited Li nuclei in Li‐argyrodite solid electrolytes during electrochemical cycling and form a special structure with reactive‐cores‐stable‐shells against Li metal, which effectively prevents local Li dendrite growth and maintains a stable Li/electrolyte interface simultaneously, leading to advanced solid‐state Li metal batteries.
ISSN:1614-6832
1614-6840
DOI:10.1002/aenm.202203631