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Modified Li7P3S11 Glass-Ceramic Electrolyte and Its Characterization.
Kazuki Uchida1, Takahiro Ohkubo1, Futoshi Utsuno2
1Graduate School of Engineering, Chiba University, 1-33 Yayoi-cho Inage-ku, Chiba 263-8522, Japan.
ACS Applied Materials & Interfaces
|August 2, 2021
Summary
Modified Li7P3S11 glass ceramics show enhanced conductivity for solid-state lithium-ion batteries. A novel synthetic route reveals a unique structural modification, improving ion transport in these metastable electrolytes.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Chemistry
Background:
- Li7P3S11 glass ceramics are promising solid-state electrolytes for lithium-ion batteries due to high ionic conductivity.
- The metastable nature and structural intricacies of Li7P3S11 hinder a full understanding of its performance.
Purpose of the Study:
- To investigate the metastable nature and enhance the performance of Li7P3S11 glass ceramics.
- To develop a novel synthetic route for improved solid-state electrolytes.
Main Methods:
- Preparation of modified Li7P3S11 glass ceramics (70Li2S-30P2S5) via two-step mechanical milling and thermal annealing.
- Characterization using 31P solid-state nuclear magnetic resonance (NMR) spectroscopy, including 2D double-quantum NMR.
- Analysis of Li+ ion dynamics using 7Li spin-lattice relaxation time measurements.
Main Results:
- A modified Li7P3S11 phase with enhanced conductivity (1.7x increase) was synthesized.
- 31P NMR revealed an additional PS43- unit within the Li7P3S11 structure, adjacent to P2S74- units.
- Li+ flip motion was linked to conduction pathways between PS43- units, with independent activation energy.
Conclusions:
- A novel synthetic approach yields metastable Li7P3S11 glass ceramics with superior ionic conductivity.
- Structural insights from NMR spectroscopy elucidate the role of PS43- units in facilitating ion transport.
- This study provides a pathway for developing advanced metastable solid-state electrolytes for next-generation batteries.

