Abstract
Development of sulfur cathodes with 100% coulombic efficiency (CE) and good cycle stability remains challenging due to the polysulfide dissolution in electrolytes. Here, it is demonstrated that electrochemical reduction of lithium bis(fluorosulfonyl)imide (LiFSI) based electrolytes at a potential close to the sulfur cathode operation forms in situ protective coating on both cathode and anode surfaces. Quantum chemistry studies suggest the coating formation is initiated by the FSI(‐F) anion radicals generated during electrolyte reduction. Such a reduction additionally results in the formation of LiF. Accelerated cycle stability tests at 60 °C in a very simple electrolyte (LiFSI in dimethoxyethane with no additives) show an average CE approaching 100.0% over 1000 cycles with a capacity decay less than 0.013% per cycle after stabilization. Such a remarkable performance suggests a great promise of both an in situ formation of protective solid electrolyte coatings to avoid unwanted side reactions and the use of a LiFSI salt for this purpose.
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Dates
Type | When |
---|---|
Created | 10 years, 8 months ago (Dec. 10, 2014, 2:30 a.m.) |
Deposited | 1 year, 10 months ago (Oct. 6, 2023, 10:23 a.m.) |
Indexed | 2 weeks, 2 days ago (Aug. 5, 2025, 8:31 a.m.) |
Issued | 10 years, 8 months ago (Dec. 10, 2014) |
Published | 10 years, 8 months ago (Dec. 10, 2014) |
Published Online | 10 years, 8 months ago (Dec. 10, 2014) |
Published Print | 10 years, 5 months ago (March 1, 2015) |
Funders
3
US Army Research Office
10.13039/100000183
Army Research OfficeRegion: Americas
gov (National government)
Labels
5
- U.S. Army Research Office
- United States Army Research Office
- U.S. Army Research Laboratory's Army Research Office
- ARL's Army Research Office
- ARO
Awards
1
- W911NF-12-1-0259
Korea government Ministry of Knowledge Economy
Awards
1
- 20118510010030
“Nanomaterials for future generation Lithium Sulphur batteries”
@article{Kim_2014, title={In Situ Formation of Protective Coatings on Sulfur Cathodes in Lithium Batteries with LiFSI‐Based Organic Electrolytes}, volume={5}, ISSN={1614-6840}, url={http://dx.doi.org/10.1002/aenm.201401792}, DOI={10.1002/aenm.201401792}, number={6}, journal={Advanced Energy Materials}, publisher={Wiley}, author={Kim, Hyea and Wu, Feixiang and Lee, Jung Tae and Nitta, Naoki and Lin, Huan‐Ting and Oschatz, Martin and Cho, Won Il and Kaskel, Stefan and Borodin, Oleg and Yushin, Gleb}, year={2014}, month=dec }