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Rechargeable magnesium metal batteries (RMMBs) are promising candidates for large-scale energy storage owing to the advantageous properties of magnesium metal negative electrodes. Recent advances, particularly in electrolyte chemistry, have accelerated progress toward practical RMMBs. Here, we combined two emerging concepts—weakly coordinating anion (WCA)-based Mg salts and alkoxyalkylamine solvents—in electrolyte design. Unexpectedly, the combination of a representative WCA-based Mg salt, Mg[Al(Ohfip)4]2, and a conventional alkoxyalkylamine, 2 methoxyethylamine (MOEA), resulted in inferior electrochemical performance, whereas MOEA favored strongly coordinating anion-based Mg salts such as Mg[TfO]2. Comprehensive electrochemical, spectroscopic, and computational analyses revealed distinct anion-dependent solvation structures and interfacial chemistries. In Mg[Al(Ohfip)4]2 systems, the anion and the solvent complexes are only minimally involved in initial Mg-interface formation. Yet, the higher trace water content of MOEA induces the formation of unstable oxygen-rich interfaces. In addition, the anion [Al(Ohfip)4]− undergoes MOEA-mediated partial hydroxylation. On the contrary, Mg2+, [TfO]⁻ and MOEA form associative ion-paired complexes that jointly contribute to the formation of fluorine- and nitrogen-rich hybrid interfaces that suppress parasitic reactions and enhance performance. Despite these benefits, the associative Mg[TfO]2–MOEA electrolyte still exhibits limitations for practical RMMB application. The complex dilemma in developing rational electrolyte materials for RMMB applications will also be discussed.

権利情報:

• Creative Commons BY Attribution 4.0 International
  

キーワード: Electrolyte, Magnesium battery, solvation, decomposition, interface

刊行年月日: 2026-07-29

出版者: Wiley

掲載誌:

• Advanced Science (ISSN: 21983844) vol. 13 issue. 59 e76897

研究助成金:

• Japan Science and Technology Agency JPMJPF2016
• Japan Society for the Promotion of Science JP26K01623

原稿種別: 出版者版 (Version of record)

MDR DOI:

公開URL: https://doi.org/10.1002/advs.76897

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更新時刻: 2026-10-24 14:05:30 +0900

MDRでの公開時刻: 2026-10-29 10:32:27 +0900