Optimization of the Form Factors of Advanced Li‐S Pouch Cells

Abstract Lithium‐sulfur (Li‐S) batteries hold immense promise as next‐generation energy storage due to their high theoretical energy density (2600 Wh kg⁻¹), low cost, and non‐toxic nature. However, practical implementation faces challenges, primarily from Li polysulfide (LiPS) shuttling within the cathode and Li dendrite growth at the anode. Optimized electrodes/electrolytes design effectively confines LiPS to the cathode, boosting cycling performance in coin cells to up to hundreds of cycles. Scaling up to larger pouch cells presents new obstacles, requiring further research for long‐term stability. A 1.45 Ah pouch cell, with optimized sulfur loading and electrolyte/sulfur ratio is developed, which delivers an energy density of 151 Wh kg −1 with 70% capacity retention up to 100 cycles. Targeting higher energy density (180 Wh kg −1 ), the developed 1Ah pouch cell exhibits 68% capacity retention after 50 cycles. Morphological analysis reveals that pouch cell failure is primarily from Li metal powdering and resulting polarization, rather than LiPS shuttling. This occurs for continuous Li ion stripping/plating during cycling, leading to dendrite growth and formation of non‐reactive Li powder, especially under high currents. These issues increase ion diffusion resistance and reduce coulombic efficiency over time. Therefore, the study highlights the importance of a protected Li metal anode for achieving high‐energy‐dense batteries.