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

Ge Zhang; Hong Jie Peng; Chen Zi Zhao; Xiang Chen; Li Da Zhao; Peng Li; Jia Qi Huang; Qiang Zhang

doi:10.1002/anie.201810132

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

Ge Zhang, Hong Jie Peng, Chen Zi Zhao, Xiang Chen, Li Da Zhao, Peng Li, Jia Qi Huang, Qiang Zhang^*

^*Corresponding author for this work

Advanced Research Institute of Multidisciplinary Science

Tsinghua University

Research output: Contribution to journal › Article › peer-review

193 Citations (Scopus)

Abstract

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 S₃ ^.− 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.

Original language	English
Pages (from-to)	16732-16736
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	57
Issue number	51
DOIs	https://doi.org/10.1002/anie.201810132
Publication status	Published - 17 Dec 2018

Keywords

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

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Zhang, G., Peng, H. J., Zhao, C. Z., Chen, X., Zhao, L. D., Li, P., Huang, J. Q., & Zhang, Q. (2018). The Radical Pathway Based on a Lithium-Metal-Compatible High-Dielectric Electrolyte for Lithium–Sulfur Batteries. Angewandte Chemie - International Edition, 57(51), 16732-16736. https://doi.org/10.1002/anie.201810132

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abstract = "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 S3 .− 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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author = "Ge Zhang and Peng, {Hong Jie} and Zhao, {Chen Zi} and Xiang Chen and Zhao, {Li Da} and Peng Li and Huang, {Jia Qi} and Qiang Zhang",

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AU - Zhang, Ge

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AU - Chen, Xiang

AU - Zhao, Li Da

AU - Li, Peng

AU - Huang, Jia Qi

AU - Zhang, Qiang

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AB - 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 S3 .− 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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KW - reaction mechanisms

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

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