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Poor Stability of Li2 CO3 in the Solid Electrolyte Interphase of a Lithium-Metal Anode Revealed by Cryo-Electron Microscopy.

Bing HanZhen ZhangYucheng ZouKang XuGuiyin XuHong WangHong MengYonghong DengJu LiMeng Gu
Published in: Advanced materials (Deerfield Beach, Fla.) (2021)
The solid electrolyte interphase (SEI) dictates the cycling stability of lithium-metal batteries. Here, direct atomic imaging of the SEI's phase components and their spatial arrangement is achieved, using ultralow-dosage cryogenic transmission electron microscopy. The results show that, surprisingly, a lot of the deposited Li metal has amorphous atomic structure, likely due to carbon and oxygen impurities, and that crystalline lithium carbonate is not stable and readily decomposes when contacting the lithium metal. Lithium carbonate distributed in the outer SEI also continuously reacts with the electrolyte to produce gas, resulting in a dynamically evolving and porous SEI. Sulfur-containing additives cause the SEI to preferentially generate Li2 SO4 and overlithiated lithium sulfate and lithium oxide, which encapsulate lithium carbonate in the middle, limiting SEI thickening and enhancing battery life by a factor of ten. The spatial mapping of the SEI gradient amorphous (polymeric → inorganic → metallic) and crystalline phase components provides guidance for designing electrolyte additives.
Keyphrases
  • solid state
  • electron microscopy
  • ion batteries
  • high resolution
  • ionic liquid
  • room temperature
  • drug delivery
  • cancer therapy
  • mass spectrometry
  • metal organic framework