Regulating Entanglement Networks of Fibrillatable Binders for Sub‐20‐µm Thick, Robust, Dry‐Processed Solid Electrolyte Membranes in All‐Solid‐State Batteries

Despite significant advancements in all-solid-state batteries (ASSBs), the reliance on thick solid electrolyte (SE) membranes hinders their commercial viability. Although the dry process using polytetrafluoroethylene (PTFE) binder is proposed for thin SE membranes, a comprehensive understanding of the correlation between PTFE fibrillation and SE membrane quality remains lacking. Here an important guidance is provided for producing durable SE membranes that can be reduced to sub-20-µm thickness by regulating the entanglement networks of PTFE. While establishing fabrication parameters; shear time and shear temperature, a dominant effect of the number-average molecular weight (M