Exchange-Mediated Transport in Battery Electrolytes: Ultrafast or Ultraslow?

Dereka, Bogdan; Lewis, Nicholas H C; Zhang, Yong; Hahn, Nathan T; Keim, Jonathan H; Snyder, Scott A; Maginn, Edward J; Tokmakoff, Andrei

doi:10.1021/jacs.2c00154

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Dereka, B., Lewis, N. H. C., Zhang, Y., Hahn, N. T., Keim, J. H., Snyder, S. A., Maginn, E. J., & Tokmakoff, A. (2022). Exchange-Mediated Transport in Battery Electrolytes: Ultrafast or Ultraslow? Journal of the American Chemical Society, 144(19), 8591–8604. https://doi.org/10.1021/jacs.2c00154

Abstract

Understanding the mechanisms of charge transport in batteries is important for the rational design of new electrolyte formulations. Persistent questions about ion transport mechanisms in battery electrolytes are often framed in terms of vehicular diffusion by persistent ion–solvent complexes versus structural diffusion through the breaking and reformation of ion–solvent contacts, i.e., solvent exchange events. Ultrafast two-dimensional (2D) IR spectroscopy can probe exchange processes directly via the evolution of the cross-peaks on p