Electric Double Layer Modulation Synergizes Organic–Inorganic Hybrid Solid Electrolyte Interface Achieving Ultra‐High Reversible Zinc Anode

Abstract The lifetime of aqueous zinc ion batteries (AZIBs) is greatly hindered by irreversible plating/stripping and undesirable reactions at the interface. Here, fluorine‐terminated small molecules are selected as multifunctional additives for AZIBs, and dynamic electrical double layer () and organic–inorganic hybridized SEIs are proposed. The strong adsorption of the additive molecules on the surface of the Zn anode builds up a homogeneous and dynamic electric field. The dynamic EDLs and hybridized SEIs accelerate the interfacial kinetics in the electrolyte over a long period of time during the cycling to regulate the homogeneous deposition of Zn and inhibit the interfacial side‐reactions to provide a high degree of reversibility in plating/stripping. As a result, the Zn||Cu asymmetric cells with modified electrolytes has a cycle life of over 3100 cycles at an ultra‐high Coulombic efficiency of up to 99.87%. More importantly, the Zn||CVO full cell can still cycle stably without significant capacity degradation at N/P ratios as low as four. This work provides a new perspective for the construction of stable SEI for high Zn utilization AZIBs.