Polyolefin‐Based Separator with Interfacial Chemistry Regulation for Robust Potassium Metal Batteries

Potassium metal batteries (KMBs) are ideal choices for high energy density storage system owing to the low electrochemical potential and low cost of K. However, the practical KMB applications suffer from intrinsically active K anode, which would bring serious safety concerns due to easier generation of dendrites. Herein, to explore a facile approach to tackle this issue, we propose to regulate K plating/stripping via interfacial chemistry engineering of commercial polyolefin-based separator using multiple functional units integrated in tailored metal organic framework. As a case study, the functional units of MIL-101(Cr) offer high elastic modulus, facilitate the dissociation of potassium salt, improve the K+ transfer number and homogenize the K+ flux at the electrode/electrolyte interface. Benefiting from these favorable features, uniform and stable K plating/stripping is realized with the regulated separator. Full battery assembled with the regulated separator showed ∼19.9 % higher discharge capacity than that with glass fiber separator at 20 mA g-1 and much better cycling stability at high rates. The generality of our approach is validated with KMBs using different cathodes and electrolytes. We envision that the strategy to suppress dendrite formation by commercial separator surface engineering using tailor-designed functional units can be extended to other metal/metal ion batteries.