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Proximity Matters: Interfacial Solvation Dictates Solid Electrolyte Interphase Composition

  • Solomon T. Oyakhire
    Solomon T. Oyakhire
    Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States
  • Sheng-Lun Liao
    Sheng-Lun Liao
    Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States
  • Sanzeeda Baig Shuchi
    Sanzeeda Baig Shuchi
    Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States
  • Mun Sek Kim
    Mun Sek Kim
    Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States
    Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States
    More by Mun Sek Kim
  • Sang Cheol Kim
    Sang Cheol Kim
    Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States
  • Zhiao Yu
    Zhiao Yu
    Department of Chemistry, Stanford University, Stanford, California 94305, United States
    More by Zhiao Yu
  • Rafael A. Vilá
    Rafael A. Vilá
    Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States
  • Paul E. Rudnicki
    Paul E. Rudnicki
    Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States
  • Yi Cui*
    Yi Cui
    Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States
    Department of Energy Science and Engineering, Stanford University, Stanford, California 94305, United States
    Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States
    *Email: [email protected]
    More by Yi Cui
  • , and 
  • Stacey F. Bent*
    Stacey F. Bent
    Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States
    Department of Energy Science and Engineering, Stanford University, Stanford, California 94305, United States
    *Email: [email protected]
Cite this: Nano Lett. 2023, 23, 16, 7524–7531
Publication Date (Web):August 11, 2023
https://doi.org/10.1021/acs.nanolett.3c02037
Copyright © 2023 American Chemical Society

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    Abstract

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    The composition of the solid electrolyte interphase (SEI) plays an important role in controlling Li–electrolyte reactions, but the underlying cause of SEI composition differences between electrolytes remains unclear. Many studies correlate SEI composition with the bulk solvation of Li ions in the electrolyte, but this correlation does not fully capture the interfacial phenomenon of SEI formation. Here, we provide a direct connection between SEI composition and Li-ion solvation by forming SEIs using polar substrates that modify interfacial solvation structures. We circumvent the deposition of Li metal by forming the SEI above Li+/Li redox potential. Using theory, we show that an increase in the probability density of anions near a polar substrate increases anion incorporation within the SEI, providing a direct correlation between interfacial solvation and SEI composition. Finally, we use this concept to form stable anion-rich SEIs, resulting in high performance lithium metal batteries.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.3c02037.

    • Description of all methods used in the paper, additional details on models for SEI growth, XPS spectra and atomic ratios for Al2O3 substrates and SEIs, additional voltage profiles, SEM images of lithium deposits (PDF)

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    Cited By

    This article is cited by 1 publications.

    1. Haodong Liu, Hongjian Zhang, Bing Ren, Yapeng Zheng, Wei Cao, Yufei Lu, Zhentao Nie, Feng Xu, Wei Huang, Jixin Zhu. Robust Ionics Reinforced Fiber As Implantable Sensor for Early Operando Monitoring Cell Thermal Safety of Commercial Lithium-Ion Batteries. Nano Letters 2024, 24 (7) , 2315-2321. https://doi.org/10.1021/acs.nanolett.3c04709

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