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Electrolyte-Phobic Surface for the Next-Generation Nanostructured Battery Electrodes
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    Electrolyte-Phobic Surface for the Next-Generation Nanostructured Battery Electrodes
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    • Chenxi Qian
      Chenxi Qian
      Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States
      Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, Ontario M5S 3H6, Canada
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    • Jie Zhao
      Jie Zhao
      Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States
      More by Jie Zhao
    • Yongming Sun*
      Yongming Sun
      Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, 1037 Luoyu Road, Wuhan 430074, China
      *Email: [email protected]
      More by Yongming Sun
    • Hye Ryoung Lee
      Hye Ryoung Lee
      Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States
    • Langli Luo
      Langli Luo
      Institute of Molecular Plus, Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, Tianjin University, Tianjin 300072, China
      More by Langli Luo
    • Meysam Makaremi
      Meysam Makaremi
      Department of Materials Science and Engineering, University of Toronto, 184 College St., Toronto, Ontario M5S 3E4, Canada
    • Sankha Mukherjee
      Sankha Mukherjee
      Department of Materials Science and Engineering, University of Toronto, 184 College St., Toronto, Ontario M5S 3E4, Canada
    • Jiangyan Wang
      Jiangyan Wang
      Department of Materials 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
    • Chenxi Zu
      Chenxi Zu
      Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States
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    • Meikun Xia
      Meikun Xia
      Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, Ontario M5S 3H6, Canada
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    • Chongmin Wang
      Chongmin Wang
      Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, 902 Battelle Boulevard, Richland, Washington 99352, United States
    • Chandra Veer Singh*
      Chandra Veer Singh
      Department of Materials Science and Engineering, University of Toronto, 184 College St., Toronto, Ontario M5S 3E4, Canada
      *Email: [email protected]
    • Yi Cui*
      Yi Cui
      Department of Materials 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]
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    • Geoffrey A. Ozin*
      Geoffrey A. Ozin
      Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, Ontario M5S 3H6, Canada
      *Email: [email protected]
    Other Access OptionsSupporting Information (2)

    Nano Letters

    Cite this: Nano Lett. 2020, 20, 10, 7455–7462
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    https://doi.org/10.1021/acs.nanolett.0c02880
    Published October 5, 2020
    Copyright © 2020 American Chemical Society

    Abstract

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    Nanostructured electrodes are among the most important candidates for high-capacity battery chemistry. However, the high surface area they possess causes serious issues. First, it would decrease the Coulombic efficiencies. Second, they have significant intakes of liquid electrolytes, which reduce the energy density and increase the battery cost. Third, solid-electrolyte interphase growth is accelerated, affecting the cycling stability. Therefore, the interphase chemistry regarding electrolyte contact is crucial, which was rarely studied. Here, we present a completely new strategy of limiting effective surface area by introducing an “electrolyte-phobic surface”. Using this method, the electrolyte intake was limited. The initial Coulombic efficiencies were increased up to ∼88%, compared to ∼60% of the control. The electrolyte-phobic layer of Si particles is also compatible with the binder, stabilizing the electrode for long-term cycling. This study advances the understanding of interphase chemistry, and the introduction of the universal concept of electrolyte-phobicity benefits the next-generation battery designs.

    Copyright © 2020 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/acs.nanolett.0c02880.

    • Materials and methods, including synthesis of porous Si nanoparticles with perfluorinated-carbon electrolyte-phobic layer, battery fabrication, DFT simulations, and in situ TEM study (PDF)

    • In situ TEM observation of morphological evolution of pSi:PFD particle when negatively biasing the working electrode to make Li+ ions flow through the oxide layer and be reduced at the working electrode, where they alloy with Si (MP4)

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    Nano Letters

    Cite this: Nano Lett. 2020, 20, 10, 7455–7462
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.nanolett.0c02880
    Published October 5, 2020
    Copyright © 2020 American Chemical Society

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