4.8 Article

Solvent selection criteria for temperature-resilient lithium-sulfur batteries

Publisher

NATL ACAD SCIENCES
DOI: 10.1073/pnas.2200392119

Keywords

lithium-sulfur batteries; temperature resilience; electrolytes; solvent selection; ion solvation

Funding

  1. NASA's Space Technology Research Grants Program [ECF 80NSSC18K1512]
  2. NSF through the University of California San Diego (UCSD) Materials Research Science and Engineering Center [DMR-2011924]
  3. Office of Vehicle Technologies of the U.S. Department of Energy through the Advanced Battery Materials Research Program (Battery500 Consortium) [DE-EE0007764]
  4. NSF [ECCS-1542148]

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This study demonstrates an electrolyte system using monodentate dibutyl ether as the solvent, which achieves the characteristics of avoiding dendrite growth and achieving high Coulombic efficiency at various temperatures. This research provides solvent-based design criteria for Li-sulfur pouch cells in a wide temperature range.
All-climate temperature operation capability and increased energy density have been recognized as two crucial targets, but they are rarely achieved together in rechargeable lithium (Li) batteries. Herein, we demonstrate an electrolyte system by using monodentate dibutyl ether with both low melting and high boiling points as the sole solvent. Its weak solvation endows an aggregate solvation structure and low solubility toward polysulfide species in a relatively low electrolyte concentration (2 mol L-1). These features were found to be vital in avoiding dendrite growth and enabling Li metal Coulombic efficiencies of 99.0%, 98.2%, and 98.7% at 23 degrees C, 240 degrees C, and 50 degrees C, respectively. Pouch cells employing thin Li metal (50 mu m) and high-loading sulfurized polyacrylonitrile (3.3 mAh cm(-2)) cathodes (negative-to-positive capacity ratio = 2) output 87.5% and 115.9% of their room temperature capacity at 240 degrees C and 50 degrees C, respectively. This work provides solvent-based design criteria for a wide temperature range Li-sulfur pouch cells.

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