<p>In situ construction of highly conductive and self-repairing electrode interface with porous materials remains a grand challenge for practical aqueous batteries. Herein, loose selective interface (LSI) is in situ constructed by self-assembly of porous organic cages (POCs) for practical Ah-level aqueous zinc metal batteries. The delicate balance between hydrogen-bonding interactions of POC-POC and coordination interactions of POC–anion/cation endows LSI with loose porous structure, selective Zn<sup>2+</sup>-conducting channels and dynamic self-repairing capability. LSI obtains the high Zn<sup>2+</sup> transfer number of 0.8, fast desolvation kinetics and homogeneous electric field distribution, which induces the dendrite-free Zn deposition along the Zn (002) plane. Meanwhile, LSI effectively confines the activity of interfacial water and enhances interfacial hydrophobicity, thus inhibiting the water-induced side reactions. Notably, Zn//Zn cells deliver the cycling life over 3200 cycles at 50&#xa0;mA&#xa0;cm<sup>−2</sup> and Zn//NVO full cells stably perform over 10,000 cycles at 10&#xa0;A&#xa0;g<sup>−1</sup>. Moreover, Ah-level pouch cell with high cathode areal capacity of 7.25&#xa0;mAh&#xa0;cm<sup>−2</sup> and limited<i> N</i>/<i>P</i> of 2.65 delivers the initial discharge capacity of 1&#xa0;Ah and cycling stability for over 237&#xa0;cycles. This study offers a novel methodology for constructing stable highly conductive interfaces with porous materials.</p>

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Engineering In Situ Loose Selective Interface with Conducting Channels for Practical Ah-Level Aqueous Zinc Metal Batteries

  • Dongdong Wang,
  • Shuo Dou,
  • Qiongying Huang,
  • Jiaying Li,
  • Mi Xu,
  • Jingshuai Li,
  • Zhendong Guo,
  • Siqi Qin,
  • Tieyan Wang,
  • Haipeng Yu,
  • Haozhen Dou,
  • Zhongwei Chen

摘要

In situ construction of highly conductive and self-repairing electrode interface with porous materials remains a grand challenge for practical aqueous batteries. Herein, loose selective interface (LSI) is in situ constructed by self-assembly of porous organic cages (POCs) for practical Ah-level aqueous zinc metal batteries. The delicate balance between hydrogen-bonding interactions of POC-POC and coordination interactions of POC–anion/cation endows LSI with loose porous structure, selective Zn2+-conducting channels and dynamic self-repairing capability. LSI obtains the high Zn2+ transfer number of 0.8, fast desolvation kinetics and homogeneous electric field distribution, which induces the dendrite-free Zn deposition along the Zn (002) plane. Meanwhile, LSI effectively confines the activity of interfacial water and enhances interfacial hydrophobicity, thus inhibiting the water-induced side reactions. Notably, Zn//Zn cells deliver the cycling life over 3200 cycles at 50 mA cm−2 and Zn//NVO full cells stably perform over 10,000 cycles at 10 A g−1. Moreover, Ah-level pouch cell with high cathode areal capacity of 7.25 mAh cm−2 and limited N/P of 2.65 delivers the initial discharge capacity of 1 Ah and cycling stability for over 237 cycles. This study offers a novel methodology for constructing stable highly conductive interfaces with porous materials.