Lipeng Wang, Yi Yang, Fengliang Liu, Xinran Li, Xia Wang, Hongpeng Li, Pengzhou Li, Zaiwang Zhao, Wanhai Zhou, Fanxing Bu, Wei Li, Yagang Yao, Bingjie Wang, Dongyuan Zhao, Dongliang Chao
Abstract 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 Zn 2+ 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 Zn 2+ transport. Specifically, the spatial separator consists of hollow SiO 2 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 Zn 2+ ions preferentially migrate through the interconnected mesopore@nanotube spatial network, whereas SO 4 2− anions and solvent can be selectively confined. This hierarchical ions segregation facilitates a Zn 2+ -rich microenvironment ( ca. 2.6 M) and a localized electric field ( ca. 4 mV), concomitantly accelerating uniform Zn 0 nucleation. As a proof of concept, we first demonstrate a 40 cm-long flexible Zn//Br 2 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.