Degradation of All-Solid-State Lithium-Sulfur Batteries with PEO-Based Composite Electrolyte

Lithium-sulfur batteries (LSBs) have emerged as a promising alternative to lithium-ion batteries (LIBs) owing to their high energy density and economic viability. In addition, all-solid-state LSBs, which use solid-state electrolytes, have been proposed to overcome the polysulfide shuttle effect while improving safety. However, the high interfacial resistance and poor ionic conductivity exhibited by the electrode and solid-state electrolytes, respectively, are significant challenges in the development of these LSBs. Herein, we apply a poly (ethylene oxide) (PEO)-based composite solid-state electrolyte with oxide Li₇La₃Zr₂O₁₂ (LLZO) solid-state electrolyte in an all-solid-state LSB to overcome these challenges. We use an electrochemical method to evaluate the degradation of the all-solid-state LSB in accordance with the carbon content and loading weight within the cathode. The all-solid-state LSB, with sulfur-carbon content in a ratio of 3:3, exhibited a high initial discharge capacity (1386 mAh g^-1), poor C-rate performance, and capacity retention of less than 50%. The all-solid-state LSB with a high loading weight exhibited a poor overall electrochemical performance. The factors influencing the electrochemical performance degradation were revealed through systematic analysis.