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 kgs-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. A single-membrane decoupled aqueous Zn-S battery is achieved by decoupling the S/Cu2S cathode and Zn/Zn(OH)42- anode, which presents an energy density of 3988 Wh kgs-1 (based on sulfur mass). The high areal energy density and long operational life originate from the high-sulfur loading cathode and newly designed single ion-selective membrane.image