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We revisited very different organic solvent-based electrolytes for RMB applications to clarify the possible molecular design toward anodically-stable ether-based electrolyte solutions. Through the comprehensive experimental and computational surveys, the intrinsic electrochemical/chemical stabilities against magnesium metal and the well-balanced solvating ability are found to be necessary to achieve the solvents with desired functionalities. Based on this knowledge, the glyme-analogues bearing trifluoroalkyl groups were designed and synthesized. By combining suitable fluorinated glyme-based solvents with appropriate supporting salts, the anodically-stable electrolytes those support electrochemical magnesium deposition/dissolution have been developed. These electrolytes showed the remarkable anodic limit of 4.4 V vs. Mg2+/Mg, highest ever reported to the best of our knowledges, and effectively suppressed undesired corrosion of Al current collectors. The application of such electrolytes to RMBs with high-voltage oxide-based cathodes however failed. The modest compatibility against magnesium metal anodes caused positive shift of the electrode potential of the magnesium metal anodes. Moreover, fragility against oxide-based cathodes caused undesired catalytic decomposition of the fluorinated solvents during charging. Based on the above findings and knowledges on RMBs, the basic concepts in designing feasible electrolyte materials and possible options toward constructing high-voltage magnesium batteries are proposed.

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• In Copyright
  

  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.3c01452.

Keyword: electrolyte, ether, anodic stability, fluorination, magnesium battery

Date published: 2023-06-08

Publisher: American Chemical Society (ACS)

Journal:

• The Journal of Physical Chemistry C (ISSN: 19327447) vol. 127 issue. 22 p. 10419-10433

Funding:

• Ministry of Education, Culture, Sports, Science and Technology JPMXP1020200301
• JST JPMJPF2016 (先進蓄電池研究開発拠点)
• Japan Society for the Promotion of Science 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)
• Japan Science and Technology Agency JPMJMI20G4
• Advanced Low Carbon Technology Research and Development Program JPMJAL1301

Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.4423

First published URL: https://doi.org/10.1021/acs.jpcc.3c01452

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Updated at: 2024-05-29 08:30:15 +0900

Published on MDR: 2024-05-29 08:30:15 +0900