ACS Publications. Most Trusted. Most Cited. Most Read
Understanding the Surprising Ionic Conductivity Maximum in Zn(TFSI)2 Water/Acetonitrile Mixture Electrolytes

OR SEARCH CITATIONS

My Activity
Publications

Figure 1Loading Img
Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Phys. Chem. Lett. 2023, 14, 50, 11393-11399
    Physical Insights into Energy Science

    Understanding the Surprising Ionic Conductivity Maximum in Zn(TFSI)2 Water/Acetonitrile Mixture Electrolytes
    Click to copy article linkArticle link copied!

    • Yong Zhang*
      Yong Zhang
      Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana 46556, United States
      Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States
      *Email: [email protected]
      More by Yong Zhang
      Orcidhttps://orcid.org/0000-0003-3988-5961
    • Emily Carino
      Emily Carino
      Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States
      More by Emily Carino
      Orcidhttps://orcid.org/0000-0001-7779-8776
    • Nathan T. Hahn
      Nathan T. Hahn
      Material, Physical and Chemical Sciences Center, Sandia National Laboratories, Albuquerque, New Mexico 87123, United States
      Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States
      More by Nathan T. Hahn
      Orcidhttps://orcid.org/0000-0001-6187-4068
    • Nigel Becknell
      Nigel Becknell
      Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
      Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States
      More by Nigel Becknell
      Orcidhttps://orcid.org/0000-0001-7857-6841
    • Julian Mars
      Julian Mars
      Department of Chemical and Biological Engineering, University of Colorado Boulder, Boulder, Colorado 80309, United States
      Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States
      Materials Science and Engineering Program, University of Colorado Boulder, Boulder, Colorado 80309, United States
      More by Julian Mars
    • Kee Sung Han
      Kee Sung Han
      Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
      Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States
      More by Kee Sung Han
      Orcidhttps://orcid.org/0000-0002-3535-1818
    • Karl T. Mueller
      Karl T. Mueller
      Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
      Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States
      More by Karl T. Mueller
      Orcidhttps://orcid.org/0000-0001-9609-9516
    • Michael Toney
      Michael Toney
      Department of Chemical and Biological Engineering, University of Colorado Boulder, Boulder, Colorado 80309, United States
      Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States
      Materials Science and Engineering Program  and  Renewable and Sustainable Energy Institute, University of Colorado Boulder, Boulder, Colorado 80309, United States
      More by Michael Toney
      Orcidhttps://orcid.org/0000-0002-7513-1166
    • Edward J. Maginn*
      Edward J. Maginn
      Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana 46556, United States
      Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States
      *Email: [email protected]
      More by Edward J. Maginn
      Orcidhttps://orcid.org/0000-0002-6309-1347
    • Sanja Tepavcevic*
      Sanja Tepavcevic
      Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
      Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States
      *Email: [email protected]
      More by Sanja Tepavcevic
      Orcidhttps://orcid.org/0000-0003-0151-8832
    Other Access OptionsSupporting Information (1)

    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2023, 14, 50, 11393–11399
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.3c03048
    Published December 11, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

    Abstract

    Click to copy section linkSection link copied!
    Abstract Image

    Aqueous electrolytes composed of 0.1 M zinc bis(trifluoromethylsulfonyl)imide (Zn(TFSI)2) and acetonitrile (ACN) were studied using combined experimental and simulation techniques. The electrolyte was found to be electrochemically stable when the ACN V% is higher than 74.4. In addition, it was found that the ionic conductivity of the mixed solvent electrolytes changes as a function of ACN composition, and a maximum was observed at 91.7 V% of ACN although the salt concentration is the same. This behavior was qualitatively reproduced by molecular dynamics (MD) simulations. Detailed analyses based on experiments and MD simulations show that at high ACN composition the water network existing in the high water composition solutions breaks. As a result, the screening effect of the solvent weakens and the correlation among ions increases, which causes a decrease in ionic conductivity at high ACN V%. This study provides a fundamental understanding of this complex mixed solvent electrolyte system.

    Copyright © 2023 American Chemical Society

    Subjects

    what are subjects

    Read this article

    To access this article, please review the available access options below.

    Get instant access

    Purchase Access

    Read this article for 48 hours. Check out below using your ACS ID or as a guest.

    Recommended

    Access through Your Institution

    You may have access to this article through your institution.

    Your institution does not have access to this content. Add or change your institution or let them know you’d like them to include access.

    Supporting Information

    Click to copy section linkSection link copied!

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.3c03048.

    • Experimental and simulation methods; experimental Coulombic efficiency; calculated density and viscosity of water/ACN solvent and compared to available experimental results; calculated correlation functions; calculated and experimental X-ray S(q) of the electrolytes; further discussion on ionic conductivity (PDF)

    Terms & Conditions

    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    Click to copy section linkSection link copied!

    This article has not yet been cited by other publications.

    Download PDF
    Go to The Journal of Physical Chemistry Letters
    Get e-Alerts
    Get e-Alerts

    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2023, 14, 50, 11393–11399
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.3c03048
    Published December 11, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

    Article Views

    876

    Altmetric

    -

    Citations

    -
    Learn about these metrics

    Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.

    Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.

    The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.