Enabling Uniform and Accurate Control of Cycling Pressure for All‐Solid‐State Batteries

Abstract All‐solid‐state batteries are emerging as potential successors in energy storage technologies due to their increased safety, stemming from replacing organic liquid electrolytes in conventional Li‐ion batteries with less flammable solid‐state electrolytes. However, all‐solid‐state batteries require precise control over cycling pressure to maintain effective interfacial contacts between materials. Traditional uniaxial cell holders, often used in battery research, face challenges in accommodating electrode volume changes, providing uniform pressure distribution, and maintaining consistent pressure over time. This study introduces isostatic pouch cell holders utilizing air as pressurizing media to achieve uniform and accurately regulated cycling pressure. LiNi _0.8 Co _0.1 Mn _0.1 O ₂ | Li ₆ PS ₅ Cl | Si pouch cells are fabricated and tested under 1 to 5 MPa pressures, revealing improved electrochemical performance with higher cycling pressures, with 2 MPa as the minimum for optimal operation. A bilayer pouch cell with a theoretical capacity of 100 mAh, cycled with an isostatic pouch cell holder, demonstrated a first‐cycle Coulombic efficiency of 76.9% and a discharge capacity of 173.6 mAh g ⁻¹ (88.1 mAh), maintaining 83.6% capacity after 100 cycles. These findings underscore the effectiveness of isostatic pouch cell holders in enhancing the performance and practical application of all‐solid‐state batteries.