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    Stabilizing protic and aprotic liquid electrolytes at high-bandgap oxide interphases

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    Type
    Article
    Authors
    Tu, Zhengyuan
    Zachman, Michael J.
    Choudhury, Snehashis
    Khan, Kasim A.
    Zhao, Qing
    Kourkoutis, Lena F.
    Archer, Lynden A.
    KAUST Grant Number
    KUS-C1-018-02
    Date
    2018-07-25
    Online Publication Date
    2018-07-25
    Print Publication Date
    2018-08-28
    Permanent link to this record
    http://hdl.handle.net/10754/629783
    
    Metadata
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    Abstract
    Approaches for regulating electrochemical stability of liquid electrolytes in contact with solid-state electrodes are a requirement for efficient and reversible electrical energy storage in batteries. Such methods are particularly needed in electrochemical cells in which the working potentials of the electrodes lie well outside the thermodynamic stability limits of the liquid electrolyte. Here we study electrochemical stability of liquids at electrolyte/electrode interfaces protected by a nanometer-thick, high-electrical band gap ceramic phase. We report that well-designed ceramic interphases extend the oxi-dative stability limits for both protic and aprotic liquid electrolytes, in some cases by as much as 1.5V. It is shown further that such interphases facilitate stable electrodeposition of reactive metals such as lithium at high Coulombic efficiency and in electrochemical cells subject to extended galvanostatic cycling at a high current density of 3 mA cm-2 and at capacities as high as 3 mAh cm-2. High-resolution cryo-FIB-SEM characterization reveals that solid/compact Li electrodeposits anchored by the ceramic interphase are the source of the enhanced Li deposition stability. The results enable a proof-of-concept ‘an-ode-free’ Li metal rechargeable battery in which Li initially provided in the cathode is the only source of lithium in the cell.
    Citation
    Tu Z, Zachman MJ, Choudhury S, Khan KA, Zhao Q, et al. (2018) Stabilizing Protic and Aprotic Liquid Electrolytes at High-Bandgap Oxide Interphases. Chemistry of Materials 30: 5655–5662. Available: http://dx.doi.org/10.1021/acs.chemmater.8b01996.
    Sponsors
    This work was supported by the Department of Energy, Advanced Research Projects Agency - Energy (ARPA-E) through award #DE-AR0000750. M.J.Z. and L.F.K. acknowledge support by the NSF (DMR-1654596). The work made use of electrochemical characterization facilities in the KAUST-CU Center for Energy and Sustainability, supported by the King Abdullah University of Science and Technology (KAUST) through Award # KUS-C1-018-02. Electron microscopy facilities at the Cornell Center for Materials Research (CCMR), an NSF-supported MRSEC through Grant DMR-1120296, were also used for the study. Additional support for the FIB/SEM cryo-stage and transfer system was provided by the Kavli Institute at Cornell and the Energy Materials Center at Cornell, DOE EFRC BES (DE-SC0001086).
    Publisher
    American Chemical Society (ACS)
    Journal
    Chemistry of Materials
    DOI
    10.1021/acs.chemmater.8b01996
    ae974a485f413a2113503eed53cd6c53
    10.1021/acs.chemmater.8b01996
    Scopus Count
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