Restraining Shuttle Effect in Rechargeable Batteries by Multifunctional Zeolite Coated Separator

Abstract The detrimental shuttle of soluble species from cathode to anode inside battery, is a critical thorn limiting stability and reversibility of rechargeable battery. Herein, an ordered pore‐window of zeolite molecular sieve is employed to effectively block shuttle of soluble matters, and prepared zeolite powder into thin zeolite layer (5 µm thick) coated on celgard separator (zeolite@celgard) with flexible and grid‐scale fabrication features. External pressure is applied to press zeolite@celgard to reduce existed interparticle gaps among zeolite particles. The separation function toward soluble species and attached H₂O scavenger role of zeolite@celgard are demonstrated via 1H/19F Nuclear Magnetic Resonance spectra, Inductive Coupled Plasma Emission Spectrometer and X‐Ray Photoelectron Spectroscopy results collected from Li/LiMn₂O₄ battery, time‐dependent in situ Raman tests in Li/S battery, and penetration experiments of redox mediator shuttle in Li/O₂ battery. Replacing typically‐used celgard/glassfiber separators, a series of side reactions (active material outflowing, low coulombic efficiency, and anode corrosion) induced via shuttle of soluble species are addressed, resulting in battery performance improvement of Li/LiMn₂O₄, Li/S, and Li/O₂ batteries. Both scientific hypothesis of utilizing pore‐size effect of zeolite for physically block soluble species, and cost‐effective, grid‐scale, and flexible zeolite‐based separators can be extended to other rechargeable battery systems based on flowing/soluble species.