Mesoporous spatial separator rectified ion transport model for durable aqueous batteries
摘要
Zinc-based aqueous batteries (ZABs) are inherently safe and offer high capacity, yet the separator penetration by dendrite protrusion still plagues their wide-scale application due to the inherent uncontrolled Zn2+ flux. Instead of conventional fibric separators with ion-surficial transport model, we introduce a spatial separator network via mono-micelle interface-confined assembly, featuring confined 3D nanofluidic channels that actively regulate Zn2+ transport. Specifically, the spatial separator consists of hollow SiO2 nanotubes (60–80 nm in diameter) interconnected by radially aligned 2.6 nm mesopores, i.e., a hierarchical mesopore@nanotube architecture. COMSOL simulations and in situ confocal laser scanning microscopy show that Zn2+ ions preferentially migrate through the interconnected mesopore@nanotube spatial network, whereas SO42− anions and solvent can be selectively confined. This hierarchical ions segregation facilitates a Zn2+-rich microenvironment (ca. 2.6 M) and a localized electric field (ca. 4 mV), concomitantly accelerating uniform Zn0 nucleation. As a proof of concept, we first demonstrate a 40 cm-long flexible Zn//Br2 fiber battery, enabling a high energy density of 49.9 Wh kg−1 and stable operation over 600 cycles, with loading of ca. 70 mg and capacity of 9 mAh. Our conceptual mesoporous spatial separator may accelerate the practical application of next-generation metal-based batteries by regulating ionic transport.