High-Sulfur Loading and Single Ion-Selective Membranes for High-Energy and Durable Decoupled Aqueous Batteries

The decoupled battery design is promising for breaking the energy density limit of traditional aqueous batteries. However, the complex battery configuration and low-selective separator membranes restrict their energy output and service time. Herein, a zinc–sulfur decoupled aqueous battery is achieved by designing a high-mass loading sulfur electrode and single ion-selective membrane (ISM). A vertically assembled nanosheet network constructed with the assistance of a magnetic field enables facile electron and ion conduction in thick sulfur electrodes, which is conducive to boosting the cell-level energy output. For the tailored ISM, the Na ions anchored on its skeleton effectively prevent the crossover of OH⁻ or Cu²⁺, facilitating the transport of Na⁺ and ensuring structural and mechanical stability. Consequently, the Zn–S aqueous battery achieves a reversible energy density of 3988 Wh kg_s⁻¹ (by sulfur mass), stable operation over 300 cycles, and an energy density of 53.2 mWh cm⁻². The sulfur-based decoupled system may be of immediate benefit toward safe, reliable, and affordable static energy storage.