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We conducted comprehensive comparative studies on the representative WCA-based electrolytes incorporating tetrakis(hexafluoro-iso-propoxyl)borate ([B(HFIP)4]−) anions as a model system to understand the effect of valency of paired cation species on transport properties and electrochemical characteristics. As revealed by X-ray crystallography, the monovalent lithium and sodium salts were obtained as adducts, where the anion participated in cation coordination along with a single solvent molecule, whereas divalent magnesium, calcium, and zinc salts formed fully isolated solvates with the divalent cations being coordinated by solvents alone. Such valency-dependent differences in the dissociation states would affect the solution properties, as the divalent electrolytes exhibited greater conductivities than their monovalent counterparts, even though the same number of charged species were present in the respective solutions. The electrochemical metal deposition/dissolution studies combined with morphological and subsequent elemental analysis on the deposits suggested the specific favorable combination of magnesium cations and [B(HFIP)4]− anion in ethereal solutions. The modest surface reactivity of the deposited macrocrystalline magnesium, moderate reductive nature of the magnesium metal, and well-balanced mutual interactions among the components may have jointly contributed to such outstanding performance.

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  This document is the Accepted Manuscript version of a Published Work that appeared in final form in The 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.3c01160

Keyword: electrolyte, borate, divalent metal, monovalent metal, stability

Date published: 2023-05-04

Publisher: American Chemical Society (ACS)

Journal:

• The Journal of Physical Chemistry C (ISSN: 19327447) vol. 127 issue. 17 p. 7987-7997

Funding:

• JST JPMJPF2016 (先進蓄電池研究開発拠点)
• JSPS JP21K05263 (リチウムおよびナトリウム系電解質の電気化学安定性を支配する制御因子の究明)
• 電気化学会

Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.4431

First published URL: https://doi.org/10.1021/acs.jpcc.3c01160

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Updated at: 2024-04-21 08:30:12 +0900

Published on MDR: 2024-04-21 08:30:12 +0900