<p>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<sup>2+</sup> 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<sup>2+</sup> transport. Specifically, the spatial separator consists of hollow SiO<sub>2</sub> nanotubes (60–80&#xa0;nm in diameter) interconnected by radially aligned 2.6&#xa0;nm mesopores, i.e., a hierarchical mesopore@nanotube architecture. COMSOL simulations and in situ confocal laser scanning microscopy show that Zn<sup>2+</sup> ions preferentially migrate through the interconnected mesopore@nanotube spatial network, whereas SO<sub>4</sub><sup>2−</sup> anions and solvent can be selectively confined. This hierarchical ions segregation facilitates a Zn<sup>2+</sup>-rich microenvironment (<i>ca.</i>&#xa0;2.6&#xa0;M) and a localized electric field (<i>ca.</i>&#xa0;4&#xa0;mV), concomitantly accelerating uniform Zn<sup>0</sup> nucleation. As a proof of concept, we first demonstrate a 40&#xa0;cm-long flexible Zn//Br<sub>2</sub> fiber battery, enabling a high energy density of 49.9 Wh kg<sup>−1</sup> and stable operation over 600 cycles, with loading of <i>ca.</i>&#xa0;70&#xa0;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.</p>

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Mesoporous spatial separator rectified ion transport model for durable aqueous batteries

  • 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

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.