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Ultrafast ion transport at a cathode–electrolyte interface and its strong dependence on salt solvation
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Wen, Bohua, Deng, Zhi, Tsai, Ping-Chun, Lebens-Higgins, Zachary W., Piper, Louis F. J., Ong, Shyue Ping and Chiang, Yet-Ming (2020) Ultrafast ion transport at a cathode–electrolyte interface and its strong dependence on salt solvation. Nature Energy, 5 (8). pp. 578-586. doi:10.1038/s41560-020-0647-0 ISSN 2058-7546.
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Official URL: http://dx.doi.org/10.1038/s41560-020-0647-0
Abstract
To access the full performance potential of advanced batteries, electrodes and electrolytes must be designed to facilitate ion transport at all applicable length scales. Here, we perform electrodynamic measurements on single electrode particles of ~6 nAh capacity, decouple bulk and interfacial transport from other pathways and show that Li intercalation into LiNi0.33Mn0.33Co0.33O2 (NMC333) is primarily impeded by interfacial kinetics when using a conventional LiPF6 salt. Electrolytes containing LiTFSI salt, with or without LiPF6, exhibit about 100-fold higher exchange current density under otherwise identical conditions. This anion group effect is explained using molecular dynamics simulations to identify preferred solvation structures, density functional theory calculations of their binding energies and Raman spectroscopy confirmation of solvation structure. We show that TFSI− preferentially solvates Li+ compared to PF6−, and yet its preferred solvation structures provide a lower Li+ binding energy, suggesting a lower desolvation energy consistent with ultrafast interfacial kinetics.
Item Type: | Journal Article | ||||||||
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Divisions: | Faculty of Science, Engineering and Medicine > Engineering > WMG (Formerly the Warwick Manufacturing Group) | ||||||||
Journal or Publication Title: | Nature Energy | ||||||||
Publisher: | Nature Publishing Group | ||||||||
ISSN: | 2058-7546 | ||||||||
Official Date: | August 2020 | ||||||||
Dates: |
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Volume: | 5 | ||||||||
Number: | 8 | ||||||||
Page Range: | pp. 578-586 | ||||||||
DOI: | 10.1038/s41560-020-0647-0 | ||||||||
Status: | Peer Reviewed | ||||||||
Publication Status: | Published | ||||||||
Access rights to Published version: | Restricted or Subscription Access |
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