Deciphering the critical role of interstitial volume in glassy sulfide superionic conductors

Han Su, Yu Zhong (), Changhong Wang (), Yu Liu, Yang Hu, Jingru Li, Minkang Wang, Longan Jiao, Ningning Zhou, Bing Xiao, Xiuli Wang, Xueliang Sun () and Jiangping Tu ()
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Han Su: Zhejiang University
Yu Zhong: Zhejiang University
Changhong Wang: University of Western Ontario1151 Richmond St.
Yu Liu: Zhejiang University
Yang Hu: University of Western Ontario1151 Richmond St.
Jingru Li: Zhejiang University
Minkang Wang: Zhejiang University
Longan Jiao: Ltd.
Ningning Zhou: Ltd.
Bing Xiao: Ltd.
Xiuli Wang: Zhejiang University
Xueliang Sun: University of Western Ontario1151 Richmond St.
Jiangping Tu: Zhejiang University

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract Sulfide electrolytes represent a crucial category of superionic conductors for all-solid-state lithium metal batteries. Among sulfide electrolytes, glassy sulfide is highly promising due to its long-range disorder and grain-boundary-free nature. However, the lack of comprehension regarding glass formation chemistry has hindered their progress. Herein, we propose interstitial volume as the decisive factor influencing halogen dopant solubility within a glass matrix. We engineer a Li3PS4-Li4SiS4 complex structure within the sulfide glassy network to facilitate the release of interstitial volume. Consequently, we increase the dissolution capacity of LiI to 40 mol% in 75Li2S-25P2S5 glass. The synthesized glass exhibits one of the highest ionic conductivities among reported glass sulfides. Furthermore, we develop a glassy/crystalline composite electrolyte to mitigate the shortcomings of argyrodite-type sulfides by utilizing our synthesized glass as the filler. The composite electrolytes effectively mitigate Li intrusion. This work unveils a protocol for the dissolution of halogen dopants in glass electrolytes.

Date: 2024
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DOI: 10.1038/s41467-024-46798-4

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