(669h) Computational Study of Lithium Nucleation Tendency in Solid Electrolytes

The driving force for the metallic lithium formation in solid electrolytes is still puzzling, considering the large bandgap and the preference of Li being ionic in oxides. A method to evaluate and predict if the metallic lithium would form on the pore surfaces of solid electrolyte was suggested in our previous study, in which the Li nucleation tendency of Li₇La₃Zr₂O₁₂ (LLZO) was evaluated by Density Function Theory (DFT) and serves as a criterion for metallic Li forms on the surfaces. In this work, a comprehensive study based on this method, which analyzes the total and partial density of states and the difference in charge density before and after inserting additional electrons, is performed on the promising solid electrolytes, whose ionic conductivities are close to the liquid electrolyte, to evaluate their Li nucleation tendency. Li_0.33La_0.56TiO₃ (LLTO), Beta-Li₃PS₄ (LPS), Li₁₀GeP₂S₁₂ (LGPS), Li_1.3Al_0.3Ti_1.7 (PO₄)₃ (LATP), are investigated. Besides, some coating materials are also studies, such as LiAlO₂, and LiNbO₃, to check whether they can prevent the formation of metallic lithium. This work gives a guideline for choosing solid electrolytes and coating materials based on the formation of Li dendrites.