Hydrolysis of Argyrodite Sulfide-Based Separator Sheets for Industrial All-Solid-State Battery Production

Researchers have been working for many years to find new material and cell systems that can be used as potential post-lithium-ion batteries. Among these, the all-solid-state battery is considered a promising candidate, with sulfide-based materials having essential advantages over other solid electrolyte materials, particularly in terms of their high ionic conductivity. A great challenge, however, is their high reactivity in contact with water, where harmful hydrogen sulfide (H2S) is formed. Since H2S formation has implications for both worker safety and material quality, it is important to quantify its impact. For this reason, this paper examines the relationship between the product properties and the H2S formation as well as influences resulting from the production environment. Exemplary material states along the process chain of a wet coating process route are analyzed for the steps of storage, mixing, coating, drying, and densifying with Li6PS5Cl (LPSCl) as a solid electrolyte material. By determining the H2S formation rate for sulfide-based separator sheets, it is shown that the water content in the surrounding atmosphere has the highest impact, while other investigated parameters are negligibly small in comparison. Among the product properties, the geometric surface and pore surface have a great influence. These results demonstrate the need for a controlled atmosphere in the production facilities at dew points of -40 to -50 °C. At those moisture levels, occupational safety and product quality are ensured for the investigated solid electrolyte sheets of LPSCl. This study is the first to provide quantitative data from the point of view of the production environment on the formation of H2S gas when using solid sulfide electrolytes and can therefore serve as a guideline for equipment, material, and cell manufacturers.