Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 3, Pages 4179-4185Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c21561
Keywords
lithium argyrodites; oxygen doping; stability; solid electrolyte; electrochemical performances
Funding
- National Natural Science Foundation of China [52177214, 51902116]
- China Postdoctoral Science Foundation [2019M652634]
- Department of Science and Technology of Guangdong Province [2017ZT07Z479]
- Presidential fund of Shenzhen Municipality
- Development and Reform Commission of Shenzhen Municipality
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This research successfully synthesized O-substituted Li5.5PS4.5-xOxCl1.5 solid electrolytes, among which Li5.5PS4.425O0.075Cl1.5 exhibits high ionic conductivity, improved moisture resistance, and enhanced electrochemical stability in higher voltage windows. Solid-state batteries using Li5.5PS4.425O0.075Cl1.5 show higher capacities and superior cyclability when operated at a high end-of-charge voltage, and exhibit outstanding performance in a wide temperature range.
Chlorine-rich argyrodite-type solid electrolyte Li5.5PS4.5Cl1.5 has been a promising choice for solid-state batteries (SSBs) because of its ultrafast Li-ion conduction. However, the poor air/moisture stability and low electrochemical stability with pristine high-voltage cathodes hinder their applications. Herein, O-substituted Li5.5PS4.5-xOxCl1.5 (x = 0, 0.075, 0.175, and 0.25) solid electrolytes are successfully synthesized. Among them, Li5.5PS4.425O0.075Cl1.5 delivers high ionic conductivity, improved moisture resistance, and enhanced electrochemical stability in higher voltage windows. SSBs using Li5.5PS4.425O0.075Cl1.5 show higher capacities and superior cyclability than those using Li5.5PS4.5Cl1.5 combined with a pristine LiNi0.8Mn0.1Co0.1O2 cathode when operated at a high end-of-charge voltage of 4.5 V (vs Li+/Li-0). Moreover, the batteries exhibit outstanding performance in a wide temperature range. This work provides a strategy to modify the inherent drawbacks of sulfide electrolytes, promoting their practical applications.
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