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In Situ Formation of Protective Coatings on Sulfur Cathodes in Lithium Batteries with LiFSI‐Based Organic Electrolytes
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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Cited by
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Self-citationHigh rate and stable cycling of lithium metal anode
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Self-citationReview on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries
Wang, A., Kadam, S., Li, H., Shi, S., & Qi, Y. (2018) · npj Computational Materials · doi:10.1038/s41524-018-0064-0 · Cited by 1,639
Critical effects of electrolyte recipes for Li and Na metal batteries
Zheng, X., Huang, L., Ye, X., Zhang, J., Min, F., Luo, W., & Huang, Y. (2021) · Chem · doi:10.1016/j.chempr.2021.02.025 · Cited by 367
Interface engineering toward stable lithium–sulfur batteries
Guo, Y., Niu, Q., Pei, F., Wang, Q., Zhang, Y., Du, L., Zhang, Y., Zhang, Y., Zhang, Y., Fan, L., et al. (2024) · Energy & Environmental Science · doi:10.1039/d3ee04183b · Cited by 322
Metadata
- Authors
- Kim, H., Wu, F., Lee, J. T., Nitta, N., Lin, H., Oschatz, M., Cho, W. I., Kaskel, S., Borodin, O., & Yushin, G.
- Venue
- Advanced Energy Materials
- Publisher
- Wiley
- Published
- 2014-12-10
- Volume
- 5
- Issue
- 6
- ISSN
- 1614-6832 (ISSN-L)
- 1614-6840
- OpenAlex
- W2134363353
- Cited by
- 240
- References
- 0
- FWCI
- 11.14
- Type
- journal article
- Language
- en
- Open access
- closed
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- The paper
- Kim, H., Wu, F., Lee, J. T., Nitta, N., Lin, H., Oschatz, M., Cho, W. I., Kaskel, S., Borodin, O., & Yushin, G. (2015). In Situ Formation of Protective Coatings on Sulfur Cathodes in Lithium Batteries with LiFSI‐Based Organic Electrolytes. Advanced Energy Materials. https://doi.org/10.1002/aenm.201401792
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