Lithium Ion Pathway within Li7La3Zr2O12-Polyethylene Oxide Composite Electrolytes

Polymer–ceramic composite electrolytes are emerging as a promising solution to deliver high ionic conductivity, optimal mechanical properties, and good safety for developing high‐performance all‐solid‐state rechargeable batteries. Composite electrolytes have been prepared with cubic‐phase Li7La3Zr2O...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2016-09, Vol.55 (40), p.12538-12542
Main Authors: Zheng, Jin, Tang, Mingxue, Hu, Yan-Yan
Format: Article
Language:English
Subjects:
6,7Li NMR
7Li NMR
Batteries
Battery cycles
Ceramics
Composite materials
Conductivity
Conductors
diffusion pathways
Electrodes
Electrolytes
Electrolytic cells
Energy harvesting
Energy storage
High resolution
Ion currents
Ions
isotope labeling
Labels
Lithium
Lithium batteries
lithium ion batteries
Lithium isotopes
Marking
Mechanical properties
Metals
Monitoring
NMR
Nuclear magnetic resonance
Optimization
Polyethylene
Polyethylene oxide
Polyethylenes
Rechargeable batteries
Safety
solid-state electrolytes
Symmetry
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Summary:Polymer–ceramic composite electrolytes are emerging as a promising solution to deliver high ionic conductivity, optimal mechanical properties, and good safety for developing high‐performance all‐solid‐state rechargeable batteries. Composite electrolytes have been prepared with cubic‐phase Li7La3Zr2O12 (LLZO) garnet and polyethylene oxide (PEO) and employed in symmetric lithium battery cells. By combining selective isotope labeling and high‐resolution solid‐state Li NMR, we are able to track Li ion pathways within LLZO‐PEO composite electrolytes by monitoring the replacement of 7Li in the composite electrolyte by 6Li from the 6Li metal electrodes during battery cycling. We have provided the first experimental evidence to show that Li ions favor the pathway through the LLZO ceramic phase instead of the PEO‐LLZO interface or PEO. This approach can be widely applied to study ion pathways in ionic conductors and to provide useful insights for developing composite materials for energy storage and harvesting. Where do they go? The first experimental evidence was obtained for lithium ions diffusing through composite ceramic electrolytes (LLZO and PEO) in an all‐solid‐state battery. Lithium ion diffusion was determined using 6,7Li NMR and isotope exchange, and indicated that Li ions mainly pass through the LLZO ceramic phase instead of the LLZO‐PEO interface or the PEO phase.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201607539