ID | 65697 |
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Author |
Ikeda, Shuhei
Department of Materials Chemistry, Nagoya University
Tsuzuki, Seiji
Advanced Chemical Energy Research Centre (ACERC), Institute of Advanced Sciences, Yokohama National University
Sudoh, Taku
Department of Chemistry and Life Science, Yokohama National University
Shigenobu, Keisuke
Research Institute for Interdisciplinary Science, Okayama University
Ueno, Kazuhide
Advanced Chemical Energy Research Centre (ACERC), Institute of Advanced Sciences, Yokohama National University
Dokko, Kaoru
Advanced Chemical Energy Research Centre (ACERC), Institute of Advanced Sciences, Yokohama National University
Watanabe, Masayoshi
Advanced Chemical Energy Research Centre (ACERC), Institute of Advanced Sciences, Yokohama National University
Shinoda, Wataru
Research Institute for Interdisciplinary Science, Okayama University,
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Abstract | Here, we report the use of molecular dynamics simulations with a polarizable force field to investigate Li-ion dynamics in sulfolane (SL)-based electrolytes. In SL-based highly concentrated electrolytes (HCEs) (e.g., SL/Li = 2:1), Li displays faster translational motion than other components, which should be related to the structural and dynamical properties of SL. In HCEs, a transient conduction network that penetrated the simulation system was always observed. Rapid (<1 ns) Li-ion hopping between adjacent coordination sites was observed throughout the network. Additionally, SLs rotated in the same timeframe without disrupting the conduction network. This rotation is believed to promote the hopping diffusion in the network. This was followed by a rotational relaxation of the SL dipole axis around the non-polar cyclohydrocarbon segment of SL (∼3.3 ns), which involves a reorganization of the network structure and an enhancement of the translational motion of the coordinating Li ions. The observed lifetime of Li–SL coordination was longer (>11 ns). Hence, it was concluded that the faster Li translational motion was obtained due to the faster rotational relaxation time of SL rather than the lifetime of Li–SL binding. The faster rotation of SL is related to its amphiphilic molecular structure with compact non-polar segments. Transport properties, such as the Onsager transport coefficients, ionic conductivity, and transference number under anion-blocking conditions, were also analyzed to characterize the features of the SL-based electrolyte.
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Note | This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry C, copyright © 2023 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpcc.3c02155
This fulltext file will be available in Jul. 2024.
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Published Date | 2023-07-07
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Publication Title |
Journal of Physical Chemistry C
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Volume | volume127
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Issue | issue28
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Publisher | American Chemical Society (ACS)
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Start Page | 13837
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End Page | 13845
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ISSN | 1932-7447
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NCID | AA1217589X
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Content Type |
Journal Article
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language |
English
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OAI-PMH Set |
岡山大学
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Copyright Holders | © 2023 American Chemical Society
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File Version | author
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DOI | |
Web of Science KeyUT | |
Related Url | isVersionOf https://doi.org/10.1021/acs.jpcc.3c02155
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Funder Name |
Japan Science and Technology Agency
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助成番号 | JPMJAL1301
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