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Effect of the Hydrofluoroether Cosolvent Structure in Acetonitrile-Based Solvate Electrolytes on the Li+ Solvation Structure and Li–S Battery Performance

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    Research Article

    Effect of the Hydrofluoroether Cosolvent Structure in Acetonitrile-Based Solvate Electrolytes on the Li+ Solvation Structure and Li–S Battery Performance
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    † Joint Center for Energy Storage Research, 9700 South Cass Avenue, Argonne, Illinois 60439, United States
    ‡ ‡Department of Chemistry and §Frederick Seitz Materials Research Laboratory, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States
    ∥ ∥Materials Science Division and ⊥Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
    *E-mail: [email protected]
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2017, 9, 45, 39357–39370
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    https://doi.org/10.1021/acsami.7b11566
    Published October 18, 2017
    Copyright © 2017 American Chemical Society
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    Abstract

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    We evaluate hydrofluoroether (HFE) cosolvents with varying degrees of fluorination in the acetonitrile-based solvate electrolyte to determine the effect of the HFE structure on the electrochemical performance of the Li–S battery. Solvates or sparingly solvating electrolytes are an interesting electrolyte choice for the Li–S battery due to their low polysulfide solubility. The solvate electrolyte with a stoichiometric ratio of LiTFSI salt in acetonitrile, (MeCN)2–LiTFSI, exhibits limited polysulfide solubility due to the high concentration of LiTFSI. We demonstrate that the addition of highly fluorinated HFEs to the solvate yields better capacity retention compared to that of less fluorinated HFE cosolvents. Raman and NMR spectroscopy coupled with ab initio molecular dynamics simulations show that HFEs exhibiting a higher degree of fluorination coordinate to Li+ at the expense of MeCN coordination, resulting in higher free MeCN content in solution. However, the polysulfide solubility remains low, and no crossover of polysulfides from the S cathode to the Li anode is observed.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsami.7b11566.

    • Electrochemical performance of Li–S cells cycled in solvate:HFE (1:1) electrolytes, physicochemical properties of solvate:HFE (1:1) electrolytes, assignments of Raman modes in (MeCN)2–LiTFSI/HFE electrolytes, low-wavenumber region Raman spectra of (MeCN)2–LiTFSI/HFE, high-wavenumber region Raman spectra of (MeCN)2–LiTFSI/HFE with Gaussian fits, 15N NMR spectra of neat MeCN and (MeCN)2–LiTFSI solutions, atomic partial charges of HFEs, voltage profiles of Li metal plating/stripping in symmetric Li–Li cells with (MeCN)2–LiTFSI:HFE (2:1) electrolytes, and UV–vis spectra of HFE-only solutions saturated with “Li2S8” (PDF)

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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2017, 9, 45, 39357–39370
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.7b11566
    Published October 18, 2017
    Copyright © 2017 American Chemical Society
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