4.8 Article

The Radical Pathway Based on a Lithium-Metal-Compatible High-Dielectric Electrolyte for Lithium-Sulfur Batteries

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 51, Pages 16732-16736

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201810132

Keywords

electrolytes; high-dielectric systems; lithium-sulfur batteries; radicals; reaction mechanisms

Funding

  1. National Key Research and Development Program [2016YFA0202500, 2016YFA0200102, 2015CB932500]
  2. National Natural Scientific Foundation of China [21676160, 21825501, 21776019]
  3. Tsinghua University Initiative Scientific Research Program

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High-dielectric solvents were explored for enhancing the sulfur utilization in lithium-sulfur (Li-S) batteries, but their applications have been impeded by low stability at the lithium metal anode. Now a radical-directed, lithium-compatible, and strongly polysulfide-solvating high-dielectric electrolyte based on tetramethylurea is presented. Over 200 hours of cycling was realized in Li\Li symmetric cells, showing good compatibility of the tetramethylurea-based electrolyte with lithium metal. The high solubility of short-chain polysulfides, as well as the presence of active S-3(center dot-) radicals, enabled pouch cells to deliver a discharge capacity of 1524 mAh g(-1) and an energy density of 324 Wh kg(-1). This finding suggests an alternative recipe to ether-based electrolytes for Li-S batteries.

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