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Reactivity and Evolution of Ionic Phases in the Lithium Solid–Electrolyte Interphase

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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Energy Lett. 2021, 6, 3, 877-885
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    Reactivity and Evolution of Ionic Phases in the Lithium Solid–Electrolyte Interphase
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    • Rui Guo
      Rui Guo
      Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States
      More by Rui Guo
      Orcidhttp://orcid.org/0000-0002-8826-2456
    • Dongniu Wang
      Dongniu Wang
      Canadian Light Source Inc., 44 Innovation Boulevard, Saskatoon, Saskatchewan S7N 2 V3, Canada
      More by Dongniu Wang
    • Lucia Zuin
      Lucia Zuin
      Canadian Light Source Inc., 44 Innovation Boulevard, Saskatoon, Saskatchewan S7N 2 V3, Canada
      More by Lucia Zuin
    • Betar M. Gallant*
      Betar M. Gallant
      Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States
      *E-mail: [email protected]
      More by Betar M. Gallant
      Orcidhttp://orcid.org/0000-0002-4586-2769
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    ACS Energy Letters

    Cite this: ACS Energy Lett. 2021, 6, 3, 877–885
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    https://doi.org/10.1021/acsenergylett.1c00117
    Published February 10, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    The unstable solid–electrolyte interphase (SEI) on Li anodes is the origin of major performance challenges in Li batteries, namely, insufficient Coulombic efficiency (CE) and cycle life. While it is known that the SEI participates in aging processes, pinpointing the chemical origins by tracing them to specific SEI phases has been experimentally challenging. Here, we formed single-phase, thin (<50 nm) interfaces of Li2O or LiF—the two most common ionic SEI phases—on Li and investigated their stability upon immersion in ether- or carbonate-based electrolytes. Contrary to some conventional wisdom that ionic phases are stable, we find by electrochemical impedance and X-ray spectroscopy that ionic SEI|electrolyte interfaces can undergo significant chemical evolution. While DOL/DME electrolytes impart minimal changes, organic/F-rich layers evolve at interfaces between Li2O or LiF and carbonate electrolyte containing LiPF6 salt, exacerbating subsequent plating overpotentials. The results suggest that electrolyte selection is important to improve transport in ionic-rich Li interfaces.

    Copyright © 2021 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.1c00117.

    • Experimental materials and methods; SEM images of Li2O SEI; Nyquist plot of EIS data; and XANES spectra of Li2O SEI (PDF)

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    ACS Energy Letters

    Cite this: ACS Energy Lett. 2021, 6, 3, 877–885
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsenergylett.1c00117
    Published February 10, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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