Framework Integration for Adaptive Interfaces in Flexible Solid‐State Lithium–Oxygen Batteries

Lithium-oxygen batteries (LOBs), with their remarkable energy density, represent a pivotal advancement in energy storage technology. However, conventional Li-O₂ batteries face significant obstacles. This study introduces polyacrylonitrile (PAN)-based polymer membranes and self-supporting cathodes fabricated via electrospinning and thermal treatment. By incorporating poly(diallyldimethylammonium chloride) (PDDA)-functionalized cathodes through electrostatic adsorption, a polymeric electrolyte-functional integrated linkage structure was developed. This design facilitates adaptive interface modulation, creating a stable low-impedance interface between the electrolyte and cathode while enabling efficient ion and electron transport. The resulting solid-state LOBs (SSLOBs) demonstrate exceptional performance, achieving a specific capacity of 8600 mAh g^-1 and a cycling lifespan of 191 cycles. The adaptive interface provides abundant reaction sites, promoting uniform ring-like discharge product growth and reversible decomposition. Additionally, flexible batteries incorporating this structure exhibit outstanding resilience to bending deformation. These advancements highlight the transformative potential of Li-O₂ batteries, offering promising directions for future energy storage research.