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Updated: May 26, 2025

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Synthesis of Ionic Liquid Based Electrolytes, Assembly of Li-ion Batteries, and Measurements of Performance at High Temperature
Published on: December 20, 2016
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Fluoride-rich Sulfide Solid Electrolyte With Ultrahigh Air Stability for All-Solid-State Batteries.
Seungwoo Lee1, Jeongheon Kim2, Chang Hun Park2
1Department of Energy Engineering, Hanyang University, Seoul, 04763, Republic of Korea.
Small (Weinheim an Der Bergstrasse, Germany)
|February 21, 2025
Summary
Researchers developed a new solid electrolyte (SE) with a fluoride-rich shell to enhance atmospheric stability. This innovation improves the performance of lithium-ion batteries by preventing degradation from moisture exposure.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Chemistry
Background:
- Sulfide-based solid electrolytes (SEs) show promise for solid-state batteries due to high ionic conductivity and ductility.
- Poor atmospheric stability of SEs, caused by reactions with moisture, generates toxic H2S gas and degrades performance, hindering commercialization.
- Argyrodite-type Li6PS5Cl (LPSCl) is a key material, but its air sensitivity remains a challenge.
Purpose of the Study:
- To improve the atmospheric stability of Li6PS5Cl (LPSCl) solid electrolytes.
- To investigate the protective effect of a fluoride-rich LPSCl shell against moisture.
- To evaluate the electrochemical performance and air stability of the modified SE in all-solid-state batteries.
Main Methods:
- Preparation of LPSCl solid electrolytes with a fluoride-rich LPSCl shell via fluorine treatment and annealing.
- Exposure of the modified SE to controlled humidity (20% RH at 25 °C) to assess air stability.
- Electrochemical characterization, including ionic conductivity, electronic conductivity, and cycling performance in full cells.
- First-principles density functional theory (DFT) modeling to understand the mechanism of enhanced air stability.
Main Results:
- A novel fluoride-rich LPSCl shell effectively protected the LPSCl core from moisture degradation.
- The modified SE maintained low electronic conductivity even after atmospheric exposure.
- Full cells using the air-exposed modified SE demonstrated improved initial discharge capacity (168.5 mAh g-1), excellent cycling stability (over 500 cycles at 0.3 C), and good rate capability.
- DFT models provided insights into the enhanced air stability mechanism.
Conclusions:
- The fluoride-rich LPSCl shell significantly enhances the atmospheric stability of argyrodite solid electrolytes.
- This surface modification effectively suppresses side reactions with moisture, preserving electrochemical properties.
- The developed material offers a promising pathway for the commercialization of stable and high-performance all-solid-state batteries.
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