Hopping Rate and Migration Entropy as the Origin of Superionic Conduction within Solid-State Electrolytes

Xiaona Li, Honggang Liu, Changtai Zhao, Jung Tae Kim, Jiamin Fu, Xiaoge Hao, Weihan Li, Ruying Li, Ning Chen, Duanyun Cao, Zhenwei Wu, Yuefeng Su*, Jianwen Liang*, Xueliang Sun*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

13 Citations (Scopus)

Abstract

Inorganic solid-state electrolytes (SSEs) have gained significant attention for their potential use in high-energy solid-state batteries. However, there is a lack of understanding of the underlying mechanisms of fast ion conduction in SSEs. Here, we clarify the critical parameters that influence ion conductivity in SSEs through a combined analysis approach that examines several representative SSEs (Li3YCl6, Li3HoCl6, and Li6PS5Cl), which are further verified in the xLiCl-InCl3system. The scaling analysis on conductivity spectra allowed the decoupled influences of mobile carrier concentration and hopping rate on ionic conductivity. Although the carrier concentration varied with temperature, the change alone cannot lead to the several orders of magnitude difference in conductivity. Instead, the hopping rate and the ionic conductivity present the same trend with the temperature change. Migration entropy, which arises from lattice vibrations of the jumping atoms from the initial sites to the saddle sites, is also proven to play a significant role in fast Li+migration. The findings suggest that the multiple dependent variables such as the Li+hopping frequency and migration energy are also responsible for the ionic conduction behavior within SSEs.

Original languageEnglish
Pages (from-to)11701-11709
Number of pages9
JournalJournal of the American Chemical Society
Volume145
Issue number21
DOIs
Publication statusPublished - 31 May 2023

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