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Localized high concentration electrolytes decomposition under electron-rich environments.

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Understanding electrolyte decomposition is key for stable solid-electrolyte interphase (SEI) layers in lithium-metal batteries. This study reveals lithium bis(fluorosulfonyl)imide and tris(2,2,2-trifluoroethyl)orthoformate decompose readily, while 1,2-dimethoxyethane remains stable.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Computational Chemistry

Background:

  • Stable solid-electrolyte interphase (SEI) formation is crucial for lithium-metal anode performance.
  • Limited understanding exists regarding electrolyte component decomposition mechanisms during SEI formation.

Purpose of the Study:

  • Investigate the reactivity and decomposition pathways of lithium bis(fluorosulfonyl)imide (LiFSI), 1,2-dimethoxyethane (DME), and tris(2,2,2-trifluoroethyl)orthoformate (TFEO) in mixed solvent electrolytes.
  • Characterize the energetics and activation barriers of key decomposition reactions.

Main Methods:

  • Computational simulations supplying excess electrons to electrolyte components.
  • Analysis of reaction mechanisms, including salt reduction, diluent decomposition, and anion-mediated reactions.
  • Thermodynamic and kinetic characterization of identified reaction pathways.

Main Results:

  • Lithium bis(fluorosulfonyl)imide (LiFSI) undergoes initial four-electron reduction.
  • Tris(2,2,2-trifluoroethyl)orthoformate (TFEO) decomposes via a six-electron pathway, with anion-attack mechanisms identified.
  • 1,2-dimethoxyethane (DME) demonstrates significant stability against electron reduction.
  • Most investigated decomposition reactions are thermodynamically favorable with low activation barriers.

Conclusions:

  • The study elucidates specific decomposition mechanisms for LiFSI and TFEO in Li-metal battery electrolytes.
  • DME exhibits superior electrochemical stability compared to LiFSI and TFEO under reducing conditions.
  • Findings provide insights into SEI formation and guide electrolyte design for improved battery performance.