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Published on: November 11, 2013
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.
None:
Al2O3 atomic layer deposition (ALD) on garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZTO) powder has been shown to induce extensive lithium diffusion during layer formation, likely driven by proton-lithium exchange reactions. Here, we use 7Li MAS NMR and T1 relaxation data to study the influence on bulk lithium dynamics in LLZTO with respect to ALD coating thickness before high-temperature sintering. Considerable variation in relaxation characteristics was observed for the samples investigated, which could be traced back to diffusion phenomena occurring throughout the ALD process. These results suggest that surface modifications via ALD can significantly alter the lithium mobility of its host structure, underlining the necessity of material monitoring at different stages of cell production for a mechanistic understanding of various properties at device level. This work establishes spectrally resolved 7Li NMR T1 relaxation as sensitive tool for tracking ALD-induced changes in Li environments and ion dynamics relevant for systematic optimization of solid-state battery materials.
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