Abstract
This research investigates challenges associated with gelation in Li6.4La3Zr1.4Ta0.6O12 (LLZTO) slurry preparation for solid-state Li-ion batteries. Gelation arises from a cross-linking reaction between the sintering aid, boron oxide (B2O3), and the poly(vinyl butyral) (PVB) binder. With increasing B2O3 content, LLZTO slurry viscosity dramatically rises, resulting in unsuitable solid-like behavior for tape casting. The alkaline nature of LLZTO powder intensifies cross-linking, a phenomenon confirmed through boron-11 nuclear magnetic resonance spectroscopy. To mitigate gelation, diol compounds, such as ethylene glycol, are introduced to deactivate B2O3-PVB cross-linking, with selection guided by support from density functional theory-based simulations.
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