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Linear ether-based highly concentrated electrolytes for Li-sulfur batteries.

Toru Ishikawa1, Shohei Haga1, Keisuke Shigenobu2

  • 1Department of Chemistry and Life Science, Yokohama National University, 79-5 Tokiwadai, Hodogaya-ku, Yokohama, Kanagawa, 240-8501, Japan. ueno-kazuhide-rc@ynu.ac.jp.

Faraday Discussions
|July 19, 2024
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Sparsely solvating electrolytes with low donor numbers significantly reduce polysulfide solubility in lithium-sulfur (Li-S) batteries. Linear dialkyl ethers, particularly monomethyl ethers like BME, enhance Li-ion transport and enable high energy density Li-S cells.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Energy Storage

Background:

  • Lithium-sulfur (Li-S) batteries offer high theoretical capacity and cost-effectiveness for next-generation energy storage.
  • Sparingly solvating electrolytes are crucial for suppressing polysulfide shuttling, improving coulombic efficiency, and extending cycle life in Li-S batteries.

Purpose of the Study:

  • To investigate the solubility of lithium polysulfide (Li2S8) in various liquid electrolytes.
  • To correlate polysulfide solubility with electrolyte properties, specifically donor number (DNNMR).
  • To evaluate the performance of novel dialkyl ether-based electrolytes in Li-S cells.

Main Methods:

  • Measured Li2S8 solubility in organic electrolytes, highly concentrated electrolytes, and ionic liquids.
  • Estimated electrolyte donor numbers (DNNMR) using 23Na-NMR spectroscopy.
  • Fabricated and tested Li-S cells using electrolytes based on lithium bis(trifluoromethanesulfonyl)amide (LiTFSA) and linear chain dialkyl ethers (MPE, BME, EPE).

Main Results:

  • Li2S8 solubility correlated inversely with DNNMR, remaining below 100 mM (elemental sulfur) for DNNMR < 14.
  • Monomethyl ethers (e.g., BME) exhibited stronger Li-ion coordination and higher ionic conductivity compared to longer chain ethers (e.g., EPE).
  • Li-S cells with dialkyl ether electrolytes showed superior charge-discharge rate capabilities and achieved >300 W h kg-1 energy density with a pouch-type cell using [Li(BME)3][TFSA] under lean electrolyte conditions.

Conclusions:

  • Electrolytes with low donor numbers (<14) effectively minimize polysulfide dissolution in Li-S batteries.
  • Dialkyl ether-based electrolytes, particularly those with monomethyl ethers, offer excellent Li-ion transport properties for high-performance Li-S cells.
  • The developed [Li(BME)3][TFSA] electrolyte demonstrates significant potential for high energy density Li-S battery applications.