Roles of inorganic surface layers on solid electrolyte interphase evolution at Li-metal anodes

The extreme reactivity of Li-metal with electrolytes leads to solid electrolyte interphase (SEI) layers that impede ion transport across interfaces. Using both experimental and computational methods, we studied the effects that nanometer-sized lithium compounds (the oxide, the hydroxide, and the carbonate) have on the chemistry, structure, and topography of the SEI that forms on bare Li-metal electrodes.

Scientific Achievement

We uncovered the effects of nanometer-sized lithium oxide, lithium hydroxide, and lithium carbonate as surface passivation layers on the interfacial reactivity of Li-metal anodes.

Significance and Impact

Our results are an important step towards predicting the chemical, structural, and topographical heterogeneity of solid electrolyte interphase layers arising from a multitude of interfacial constituents.

Research Details

  • Solution decomposition experiments were performed in pure solvent (dimethoxyethane) and then with the addition of 1 M of Li-bis(trifluoromethanesulfonyl)-imide.
  • When lithium oxide was the major component on the altered surface, lithium fluoride phases formed. The presence of a dominant hydroxide layer resulted in enhanced decomposition processes involving sulfur.
  • Our observations can be explained based on the calculated quantities of electronic charge transfer found for each of the passivating films.

DOI: 10.1021/acsami.9b07587

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