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Co-intercalation of Mg2+ and Na+ in Na0.69Fe2(CN)6 as a High-Voltage Cathode for Magnesium Batteries

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    Research Article

    Co-intercalation of Mg2+ and Na+ in Na0.69Fe2(CN)6 as a High-Voltage Cathode for Magnesium Batteries
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    † School of Chemical and Biological Engineering, Institute of Chemical Processes, Seoul National University, 1, Gwanak-ro, Gwanak-gu, Seoul 08826, South Korea
    ‡ School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50, UNIST-gil, Eonyang-eup, Ulju-gun, Ulsan 44919, South Korea
    § Advanced Batteries Research Center, Korea Electronics Technology Institute (KETI), 25, Saenari-ro, Bundang-gu, Seongnam-si, Gyeonggi-do 13509, South Korea
    *E-mail: [email protected]
    *E-mail: [email protected]
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2016, 8, 13, 8554–8560
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    https://doi.org/10.1021/acsami.6b01352
    Published March 11, 2016
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    Thanks to the advantages of low cost and good safety, magnesium metal batteries get the limelight as substituent for lithium ion batteries. However, the energy density of state-of-the-art magnesium batteries is not high enough because of their low operating potential; thus, it is necessary to improve the energy density by developing new high-voltage cathode materials. In this study, nanosized Berlin green Fe2(CN)6 and Prussian blue Na0.69Fe2(CN)6 are compared as high-voltage cathode materials for magnesium batteries. Interestingly, while Mg2+ ions cannot be intercalated in Fe2(CN)6, Na0.69Fe2(CN)6 shows reversible intercalation and deintercalation of Mg2+ ions, although they have the same crystal structure except for the presence of Na+ ions. This phenomenon is attributed to the fact that Mg2+ ions are more stable in Na+-containing Na0.69Fe2(CN)6 than in Na+-free Fe2(CN)6, indicating Na+ ions in Na0.69Fe2(CN)6 plays a crucial role in stabilizing Mg2+ ions. Na0.69Fe2(CN)6 delivers reversible capacity of approximately 70 mA h g–1 at 3.0 V vs Mg/Mg2+ and shows stable cycle performance over 35 cycles. Therefore, Prussian blue analogues are promising structures for high-voltage cathode materials in Mg batteries. Furthermore, this co-intercalation effect suggests new avenues for the development of cathode materials in hybrid magnesium batteries that use both Mg2+ and Na+ ions as charge carriers.

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    Cite this: ACS Appl. Mater. Interfaces 2016, 8, 13, 8554–8560
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.6b01352
    Published March 11, 2016
    Copyright © 2016 American Chemical Society
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