Abstract
Lithium metal penetration through garnet based LLZO solid electrolytes (SEs) have been identified as a critical failure process. At critical current density (CCD), LLZO SE has been known to short-circuiting, and can even result in fracturing of the SE. The combined chemo-mechanical phenomena- which can significantly affect the performance in all solid-state batteries, requires detailed investigation of several related phenomena. Characterizing the dynamical mechanical evolution that occurs in the electrode-SE is challenging. Investigation of the mechanical driving forces of lithium metal penetration through the SE is a particularly important challenge. To probe the chemo-mechanical phenomena that occur during lithium plating, this study reports in-situ curvature measurements that were designed to evaluate the stresses that evolve in LLZO during lithium plating. The experimental configuration created for this work provides data which was analyzed with a detailed Finite Element Model (FEM) to quantitatively evaluate stress evolution in the solid electrolyte. The results show that Li metal plating within a surface flaw can produce stress build-up prior to short-circuiting. The combined results from both the experiments and the FEM suggest that it is critical to minimize surface defects and flaws during manufacturing processes.
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