Ultrafast ion transport at a cathode–electrolyte interface and its strong dependence on salt solvation
Bohua Wen,
Zhi Deng,
Ping-Chun Tsai,
Zachary W. Lebens-Higgins,
Louis F. J. Piper,
Shyue Ping Ong and
Yet-Ming Chiang ()
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Bohua Wen: Massachusetts Institute of Technology
Zhi Deng: University of California San Diego
Ping-Chun Tsai: Massachusetts Institute of Technology
Zachary W. Lebens-Higgins: Binghamton University
Louis F. J. Piper: Binghamton University
Shyue Ping Ong: University of California San Diego
Yet-Ming Chiang: Massachusetts Institute of Technology
Nature Energy, 2020, vol. 5, issue 8, 578-586
Abstract:
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.
Date: 2020
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natene:v:5:y:2020:i:8:d:10.1038_s41560-020-0647-0
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DOI: 10.1038/s41560-020-0647-0
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