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Cited by 304

The DOI matches its Crossref record; 39 of the 39 references it cites were found in a registry or an index.

Direct Evidence for Li Ion Hopping Conduction in Highly Concentrated Sulfolane-Based Liquid Electrolytes

Open access
Dokko, Kaoru, Watanabe, Daiki, Ugata, Yosuke, Thomas, Morgan L., Tsuzuki, Seiji, Shinoda, Wataru, Hashimoto, Kei, Ueno, Kazuhide, Umebayashi, Yasuhiro, Watanabe, Masayoshi·2018·The Journal of Physical Chemistry B
DOI 10.1021/acs.jpcb.8b09439
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Abstract

Abstract We demonstrate that Li+ hopping conduction, which cannot be explained by conventional models i.e., Onsager’s theory and Stokes’ law, emerges in highly concentrated liquid electrolytes composed of LiBF4 and sulfolane (SL). Self-diffusion coefficients of Li+ (DLi), BF4– (DBF4), and SL (DSL) were measured with pulsed-field gradient NMR. In the concentrated electrolytes with molar ratios of SL/LiBF4 ≤ 3, the ratios DSL/DLi and DBF4/DLi become lower than 1, suggesting faster diffusion of Li+ than SL and BF4–, and thus the evolution of Li+ hopping conduction. X-ray crystallographic analysis of the LiBF4/SL (1:1) solvate revealed that the two oxygen atoms of the sulfone group are involved in the bridging coordination of two different Li+ ions. In addition, the BF4– anion also participates in the bridging coordination of Li+. The Raman spectra of the highly concentrated LiBF4–SL solution suggested that Li+ ions are bridged by SL and BF4– even in the liquid state. Moreover, detailed investigation along with molecular dynamics simulations suggests that Li+ exchanges ligands (SL and BF4–) dynamically in the highly concentrated electrolytes, and Li+ hops from one coordination site to another. The spatial proximity of coordination sites, along with the possible domain structure, is assumed to enable Li+ hopping conduction. Finally, we demonstrate that Li+ hopping suppresses concentration polarization in Li batteries, leading to increased limiting current density and improved rate capability compared to the conventional concentration electrolyte. Identification and rationalization of Li+ ion hopping in concentrated SL electrolytes is expected to trigger a new paradigm of understanding for such unconventional electrolyte systems.

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Metadata

Authors
Dokko, K., Watanabe, D., Ugata, Y., Thomas, M. L., Tsuzuki, S., Shinoda, W., Hashimoto, K., Ueno, K., Umebayashi, Y., & Watanabe, M.
Venue
The Journal of Physical Chemistry B
Publisher
American Chemical Society (ACS)
Published
2018-11-07
Volume
122
Issue
47
Pages
10736-10745
ISSN
  • 1520-5207 (ISSN-L)
  • 1520-6106
DOI
10.1021/acs.jpcb.8b09439
OpenAlex
W2899927586
Cited by
304
References
39
FWCI
7.24
Type
journal article
Language
en
Open access
hybrid

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