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Non-Faradaic Li+ Migration and Chemical Coordination across Solid-State Battery Interfaces

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    Non-Faradaic Li+ Migration and Chemical Coordination across Solid-State Battery Interfaces
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    Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States
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    Nano Letters

    Cite this: Nano Lett. 2017, 17, 11, 6974–6982
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    https://doi.org/10.1021/acs.nanolett.7b03498
    Published October 23, 2017
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    Abstract

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    Efficient and reversible charge transfer is essential to realizing high-performance solid-state batteries. Efforts to enhance charge transfer at critical electrode–electrolyte interfaces have proven successful, yet interfacial chemistry and its impact on cell function remains poorly understood. Using X-ray photoelectron spectroscopy combined with electrochemical techniques, we elucidate chemical coordination near the LiCoO2–LIPON interface, providing experimental validation of space-charge separation. Space-charge layers, defined by local enrichment and depletion of charges, have previously been theorized and modeled, but the unique chemistry of solid-state battery interfaces is now revealed. Here we highlight the non-Faradaic migration of Li+ ions from the electrode to the electrolyte, which reduces reversible cathodic capacity by ∼15%. Inserting a thin, ion-conducting LiNbO3 interlayer between the electrode and electrolyte, however, can reduce space-charge separation, mitigate the loss of Li+ from LiCoO2, and return cathodic capacity to its theoretical value. This work illustrates the importance of interfacial chemistry in understanding and improving solid-state batteries.

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    Cite this: Nano Lett. 2017, 17, 11, 6974–6982
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.nanolett.7b03498
    Published October 23, 2017
    Copyright © 2017 American Chemical Society
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