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Transient Phase-Mediated Li+ Transportation in the Lithium Lanthanum Titanate Solid-State Electrolyte
Yuxin Qiu1, Yao Nian2, Yonghui Ma3
1Institute of Molecular Plus, Department of Chemistry, Tianjin University & Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300072, China.
ACS Applied Materials & Interfaces
|September 28, 2024
Summary
Lithium lanthanum titanium oxide (LLTO) solid electrolytes show promise for batteries. A transient (La, Ti)2O3 phase hinders lithium-ion diffusion, impacting conductivity.
Area of Science:
- Materials Science
- Solid-State Chemistry
- Electrochemistry
Background:
- Lithium lanthanum titanium oxide (LLTO) is a promising solid-state electrolyte for lithium batteries.
- Understanding lithium-ion diffusion mechanisms in LLTO is crucial for improving battery performance.
- Structural defects and impurity phases significantly impact LLTO's ionic conductivity.
Purpose of the Study:
- To investigate the atomic-scale lithium-ion diffusion mechanism in LLTO.
- To characterize the structural defects and transient phases present in LLTO ceramic pellets.
- To correlate the formation of these phases with the sintering process and their effect on Li-ion conductivity.
Main Methods:
- Aberration-corrected transmission electron microscopy (TEM) for detailed structural characterization.
- Crystallographic analysis to study phase transitions and orientations.
- Theoretical evaluation of atomistic mechanisms of lithium diffusion.
Main Results:
- A prevalent transient (La, Ti)2O3 phase was identified at antiphase boundaries within LLTO domains.
- This transient phase exhibits a gradual structural transition to a tetragonal LLTO structure.
- Lithium diffusion is retarded by the transient phase and correlated with excess lanthanum (La).
Conclusions:
- The transient (La, Ti)2O3 phase plays a significant role in LLTO's Li-ion conductivity.
- Controlling the formation of this phase during sintering is key to optimizing LLTO electrolytes.
- Excess La content exacerbates the diffusion hindrance caused by the transient phase.
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