Improving rechargeable magnesium batteries through dual cation co-intercalation strategy

Ananyo Roy, Mohsen Sotoudeh, Sirshendu Dinda, Yushu Tang, Christian Kübel, Axel Groß, Zhirong Zhao-Karger, Maximilian Fichtner and Zhenyou Li ()
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Ananyo Roy: Helmholtz Institute Ulm (HIU)
Mohsen Sotoudeh: Institute of Theoretical Chemistry, Universität Ulm
Sirshendu Dinda: Helmholtz Institute Ulm (HIU)
Yushu Tang: Institute of Nanotechnology (INT), Karlsruhe Institute of Technology (KIT)
Christian Kübel: Helmholtz Institute Ulm (HIU)
Axel Groß: Helmholtz Institute Ulm (HIU)
Zhirong Zhao-Karger: Helmholtz Institute Ulm (HIU)
Maximilian Fichtner: Helmholtz Institute Ulm (HIU)
Zhenyou Li: Helmholtz Institute Ulm (HIU)

Nature Communications, 2024, vol. 15, issue 1, 1-16

Abstract: Abstract The development of competitive rechargeable Mg batteries is hindered by the poor mobility of divalent Mg ions in cathode host materials. In this work, we explore the dual cation co-intercalation strategy to mitigate the sluggishness of Mg2+ in model TiS2 material. The strategy involves pairing Mg2+ with Li+ or Na+ in dual-salt electrolytes in order to exploit the faster mobility of the latter with the aim to reach better electrochemical performance. A combination of experiments and theoretical calculations details the charge storage and redox mechanism of co-intercalating cationic charge carriers. Comparative evaluation reveals that the redox activity of Mg2+ can be improved significantly with the help of the dual cation co-intercalation strategy, although the ionic radius of the accompanying monovalent ion plays a critical role on the viability of the strategy. More specifically, a significantly higher Mg2+ quantity intercalates with Li+ than with Na+ in TiS2. The reason being the absence of phase transition in the former case, which enables improved Mg2+ storage. Our results highlight dual cation co-intercalation strategy as an alternative approach to improve the electrochemical performance of rechargeable Mg batteries by opening the pathway to a rich playground of advanced cathode materials for multivalent battery applications.

Date: 2024
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DOI: 10.1038/s41467-023-44495-2

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