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Mechanism of Zn Insertion into Nanostructured δ-MnO2: A Nonaqueous Rechargeable Zn Metal Battery

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Download Hi-Res ImageDownload to MS-PowerPointCite This:Chem. Mater. 2017, 29, 11, 4874-4884
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    Mechanism of Zn Insertion into Nanostructured δ-MnO2: A Nonaqueous Rechargeable Zn Metal Battery
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    † ‡ †Joint Center for Energy Storage Research (JCESR), ‡Chemical Sciences and Engineering Division, and §Material Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
    # Department of Physics, Central Michigan University, Mt. Pleasant, Michigan 48859, United States
    ∥ ∥Department of Chemistry and ⊥Department of Physics, University of Illinois at Chicago, Chicago, Illinois 60607, United States
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    *E-mail: [email protected]
    *E-mail: [email protected]
    *E-mail: [email protected]
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    Chemistry of Materials

    Cite this: Chem. Mater. 2017, 29, 11, 4874–4884
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    https://doi.org/10.1021/acs.chemmater.7b00852
    Published May 8, 2017
    Copyright © 2017 American Chemical Society
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    Unlike the more established lithium-ion based energy storage chemistries, the complex intercalation chemistry of multivalent cations in a host lattice is not well understood, especially the relationship between the intercalating species solution chemistry and the prevalence and type of side reactions. Among multivalent metals, a promising model system can be based on nonaqueous Zn2+ ion chemistry. Several examples of these systems support the use of a Zn metal anode, and reversible intercalation cathodes have been reported. This study utilizes a combination of analytical tools to probe the chemistry of a nanostructured δ-MnO2 cathode in association with a nonaqueous acetonitrile–Zn(TFSI)2 electrolyte and a Zn metal anode. As many of the issues related to understanding a multivalent battery relate to the electrolyte–electrode interface, the high surface area of a nanostructured cathode provides a significant interface between the electrolyte and cathode host that maximizes the spectroscopic signal of any side reactions or minor mechanistic pathways. Numerous factors affecting capacity fade and issues associated with the second phase formation including Mn dissolution in heavily cycled Zn/δ-MnO2 cells are presented including dramatic mechanistic differences in the storage mechanism of this couple when compared to similar aqueous electrolytes are noted.

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    Cite this: Chem. Mater. 2017, 29, 11, 4874–4884
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