Designing Solvated Double‐Layer Polymer Electrolytes with Molecular Interactions Mediated Stable Interfaces for Sodium Ion Batteries

Unstable cathode-electrolyte and/or anode-electrolyte interface in polymer-based sodium-ion batteries (SIBs) will deteriorate their cycle performance. Herein, a unique solvated double-layer quasi-solid polymer electrolyte (SDL-QSPE) with high Na+ ion conductivity is designed to simultaneously improve stability on both cathode and anode sides. Different functional fillers are solvated with plasticizers to improve Na+ conductivity and thermal stability. The SDL-QSPE is laminated by cathode- and anode-facing polymer electrolyte to meet the independent interfacial requirements of the two electrodes. The interfacial evolution is elucidated by theoretical calculations and 3D X-ray microtomography analysis. The Na0.67Mn2/3Ni1/3O2|SDL-QSPE|Na batteries exhibit 80.4 mAh g-1 after 400 cycles at 1 C with the Coulombic efficiency close to 100%, which significantly outperforms those batteries using the monolayer-structured QSPE.