Density functional theory screening of gas-treatment strategies for stabilization of high energy-density lithium metal anodes

Stephan Koch, Benjamin Morgan, Stefano Passerini, Gilberto Teobaldi

Research output: Contribution to journalArticlepeer-review

30 Citations (Scopus)
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Abstract

To explore the potential of molecular gas treatment of freshly cut lithium foils in non-electrolyte-based passivation of high-energy-density Li anodes, density functional theory (DFT) has been used to study the decomposition of molecular gases on metallic lithium surfaces. By combining DFT geometry optimization and Molecular Dynamics, the effects of atmospheric (N2, O2, CO2) and hazardous (F2, SO2) gas decomposition on Li(bcc) (100), (110), and (111) surfaces on relative surface energies, work functions, and emerging electronic and elastic properties are investigated. The simulations suggest that exposure to different molecular gases can be used to induce and control reconstructions of the metal Li surface and substantial changes (up to over 1 eV) in the work function of the passivated system. Contrary to the other considered gases, which form metallic adlayers, SO2 treatment emerges as the most effective in creating an insulating passivation layer for dosages ≤1 monolayer. The substantial Li → adsorbate charge transfer and adlayer relaxation produce marked elastic stiffening of the interface, with the smallest change shown by nitrogen-treated adlayers.
Original languageEnglish
Pages (from-to)150-161
Number of pages12
JournalJournal of Power Sources
Volume296
Early online date24 Jul 2015
DOIs
Publication statusPublished - 20 Nov 2015

Keywords

  • density functional theory
  • lithium metal gas treatment
  • surface reconstruction
  • artificial solid electrolyte interphase
  • work function
  • elasticity

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