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ALD-Induced Changes in Lithium Dynamics throughout Garnet-Type Solid-State Electrolytes: Insights from 7Li NMR T1
Michael K Steinhoff1,2, Davis Thomas Daniel1, Shicheng Yu1
1Institute of Energy Technologies - Fundamental Electrochemistry (IET-1), Forschungszentrum Jülich, 52428 Jülich, Germany.
Atomic layer deposition (ALD) on solid-state battery materials like lithium lanthanum zirconium tantalum oxide (LLZTO) can alter lithium diffusion. Spectrally resolved NMR T1 relaxation effectively tracks these ALD-induced changes for battery optimization.
Area of Science:
- Solid-state chemistry
- Materials science
- Battery technology
Background:
- Garnet-type solid electrolytes, such as Li6.4La3Zr1.4Ta0.6O12 (LLZTO), are promising for solid-state batteries.
- Atomic layer deposition (ALD) is used for surface modification, but its impact on ion dynamics requires detailed study.
- Proton-lithium exchange reactions during ALD may influence lithium diffusion in LLZTO.
Purpose of the Study:
- To investigate the effect of Al2O3 ALD coating thickness on bulk lithium dynamics in LLZTO powder before sintering.
- To understand how ALD-induced diffusion phenomena influence lithium mobility within the LLZTO structure.
- To establish 7Li NMR T1 relaxation as a tool for monitoring ALD-induced changes in solid-state electrolyte materials.
Main Methods:
- Utilized 7Li Magic Angle Spinning (MAS) Nuclear Magnetic Resonance (NMR) spectroscopy.
- Analyzed T1 relaxation data to probe lithium dynamics.
- Investigated samples with varying Al2O3 ALD coating thicknesses on LLZTO powder.
Main Results:
- Observed considerable variation in 7Li NMR T1 relaxation characteristics across different ALD coating thicknesses.
- Traced these variations to diffusion phenomena occurring during the ALD process.
- Demonstrated that ALD surface modification significantly alters lithium mobility in the LLZTO host structure.
Conclusions:
- ALD surface modification can substantially impact the lithium ion dynamics of LLZTO.
- Monitoring material changes during ALD is crucial for understanding device-level properties.
- Spectrally resolved 7Li NMR T1 relaxation is a sensitive method for optimizing solid-state battery materials by tracking ALD-induced changes.
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