All-solid-state batteries utilizing sulfide solid electrolytes are considered to be a promising alternative to traditional Li-ion batteries due to their high lithium-ion conductivity and chemical compatibility with lithium metal anodes. These characteristics are anticipated to inhibit lithium penetration in the electrolyte and prevent cell short-circuiting. However, lithium penetration is still reported to occur within the solid electrolytes during battery operations, leading to premature failures. Various mechanisms have been proposed to explain this complex electro-chemo-mechanical phenomenon. A thorough understanding of the mechanical properties of these electrolytes is crucial for enhancing the performance and reliability of all-solid-state lithium batteries. This study focuses on understanding the influence of chemical reactions on the mechanical degradation of a sulfide-based solid electrolyte, and first-principles atomistic simulations were employed to elucidate the relationship between lithium concentration within the solid electrolyte and its consequential changes in the mechanical properties. Li6PS5Cl is selected as a prototypical solid electrolyte and evaluated, and a critical linkage between lithium concentration and mechanical property degradation was identified. Reduction in the mechanical strength and modulus was observed at off-stoichiometric lithium concentrations, which can contribute to the mechanical weakening of the solid electrolyte accelerating the lithium penetration during the charge/discharge processes. The results obtained in this work provide significant insights into the mechanical integrity of solid electrolytes under operational conditions, laying a foundation for enhancing the durability and safety of all-solid-state batteries.
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