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.

Document Details

Document Type
Pub Defense Publication
Publication Date
Dec 10, 2014
Source ID
10.1002/aenm.201401792

Entities

People

  • Feixiang Wu
  • Gleb Yushin
  • Huan‐ting Lin
  • Hyea Kim
  • Jung Tae Lee
  • Martin Oschatz
  • Naoki Nitta
  • Oleg Borodin
  • Stefan Kaskel
  • Won Il Cho

Organizations

  • Army Research Office
  • Central South University
  • Georgia Tech
  • Technische Universität Dresden
  • United States Army Research Laboratory

Tags

Fields of Study

  • Materials science

Readers

  • Electrochemical Engineering/ Fuel Cell Technologies
  • Surface Coatings Technology.

Technology Areas

  • Quantum Computing