SnS2(001)‐Reinforced Ion/Molecular Sieving Separator Enables High‐Performance Aqueous Zinc‐Organic Batteries

Abstract Challenges including dendrite growth on Zn anodes and organic cathode dissolution severely hinder the practical application of aqueous zinc‐organic batteries (AZOBs). Herein, a Janus separator engineered by anchoring SnS 2 (001) nanosheets onto glass fiber (SnS 2 (001)@GF) to tackle these issues is prsented. The (001) plane orientation of SnS 2 , compared to the (100) crystal plane, features reduced binding energy with Zn 2+ and lower work function, enhancing Zn 2+ ion diffusion, creating uniform electric field and ion concentration, and enabling preferential deposition of Zn 2+ along the (002) direction with rapid kinetics, while concurrently repelling SO 4 2− ions through electrostatic repulsion. Additionally, the hierarchical stacking properties of SnS 2 (001) mitigate the shuttling of organic cathodes. With this Janus separator, a robust SEI layer of ZnS, Zn 5 Sn 4 , and Zn 7 Sn 4 forms on the Zn surface, further inhibiting Zn dendrites and byproduct formation. The Zn//Zn cell exhibits stable cyclability exceeding 2100 h at 1 mA cm −2 and 1 mAh cm −2 . The Zn//bipolar organic molecular cathinone (IDT) full battery achieves stable electrochemical behavior over 2250 cycles at 10 A g −1 , with 100% capacity retention after 850 cycles at a mass loading of 17 mg cm −1 . Other full batteries utilizing dibenzo[b,i]thianthrene‐5,7,12,14–tetraone (DTT) and 5,7,12,14–pentacenetetrone (PT) respectively demonstrate significantly enhanced electrochemical performance.