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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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Hopping Rate and Migration Entropy as the Origin of Superionic Conduction within Solid-State Electrolytes
Xiaona Li1, Honggang Liu2,3, Changtai Zhao4
1Department of Mechanical and Materials Engineering, University of Western Ontario, 1151 Richmond St, London, Ontario N6A 3K7, Canada.
Journal of the American Chemical Society
|May 17, 2023
Summary
Understanding fast ion conduction in solid-state electrolytes (SSEs) is key for advanced batteries. This study reveals that ion hopping rate, not just carrier concentration, significantly impacts conductivity in SSEs.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Chemistry
Background:
- Inorganic solid-state electrolytes (SSEs) are crucial for developing high-energy solid-state batteries.
- A deep understanding of the mechanisms governing fast ion conduction in SSEs is currently lacking.
Purpose of the Study:
- To clarify the critical parameters influencing ion conductivity in SSEs.
- To elucidate the relationship between mobile carrier concentration, hopping rate, and overall ionic conductivity.
Main Methods:
- Combined analysis of conductivity spectra from representative SSEs (Li3YCl6, Li3HoCl6, Li6PS5Cl) and the xLiCl-InCl3 system.
- Scaling analysis to decouple the effects of carrier concentration and hopping rate on ionic conductivity.
Main Results:
- Mobile carrier concentration changes with temperature but is not the sole driver of conductivity variations.
- Ionic conductivity and ion hopping rate exhibit similar temperature dependencies.
- Migration entropy, linked to lattice vibrations during ion jumps, significantly influences fast Li+ migration.
Conclusions:
- Fast ion conduction in SSEs is governed by multiple interdependent variables, including Li+ hopping frequency and migration energy.
- The hopping rate is a more critical factor than carrier concentration for achieving high ionic conductivity in SSEs.
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