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Adiabatic and Nonadiabatic Charge Transport in Li–S Batteries

The insulating nature of the redox end members in Li–S batteries, α-S and Li2S, has the potential to limit the capacity and efficiency of this emerging energy storage system. Nevertheless, the mechanisms responsible for ionic and electronic transport in these materials remain a matter of debate. The present study clarifies these mechanisms—in both the adiabatic and nonadiabatic charge transfer regimes—by employing a combination of hybrid-functional-based and constrained density functional theory calculations. Charge transfer in Li2S is predicted to be adiabatic, and thus is well-described by conventional DFT methodologies. In sulfur, however, transitions between S8 rings are nonadiabatic. In this case, conventional DFT overestimates charge transfer rates by up to 2 orders of magnitude. Delocalized holes, and to a lesser extent, localized electron polarons, are predicted to be the most mobile electronic charge carriers in α-S; in Li2S, hole polarons dominate. Although all carriers exhibit extremely low equ...

Authors:   Haesun Park; Nitin Kumar; Marko Melander; Tejs Vegge; Juan Maria Garcia Lastra; Donald J. Siegel
Journal:   Chemistry of Materials
Year:   2018
DOI:   10.1021/acs.chemmater.7b04618
Publication date:   16-Jan-2018
Facts, background information, dossiers
  • matter
  • energy storage
  • density functional theory
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