Property evolution of Al2O3 coated and uncoated Si electrodes: A first principles investigation

Sung Yup Kim, Yue Qi

    Research output: Contribution to journalArticle

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    Abstract

    In order to compare the difference between coated and uncoated Si electrode, the basic material properties of atomic layer deposition ALD-Al2O3 coating and native SiO2 layer on Si are investigated by using density functional theory calculations. These properties include: the open circuit voltage curve with respect to lithium metal, the elastic properties, and Li ion diffusion characteristics in SiO2 and Al2O3 and their lithiated compounds (such as Li4SiO4 and LiAlO2). Results show that lithiation occurs at the voltage above EC (Ethylene Carbonate) decomposition(~0.8V) causing initial irreversible capacity loss. Also, lithiation softens Al2O3 mechanically, while slightly stiffens SiO2. For the Li ion diffusion, SiO2 and Al2O3 have totally different behavior upon lithiation. For SiO2, Li diffuses very fast, but the energy barrier becomes higher as lithiation goes on. When SiO2 is lithiated to Li4SiO4, the diffusion energy barrier becomes lower again. For Al2O3, its intrinsic ionic conductivity is very low, but the Li diffusion energy barrier becomes lower (as low as Li2Si2O5) as lithiation proceeds and LiAlO2 is formed. Therefore, designing ALD coating should target the coating properties after lithiation.

    Original languageEnglish (US)
    Pages (from-to)F3137-F3143
    JournalJournal of the Electrochemical Society
    Volume161
    Issue number11
    DOIs
    StatePublished - 2014

    Profile

    Feline Sarcoma Viruses
    coatings
    energy
    Acetabularia
    African Swine Fever Virus
    Energy barriers
    Coatings
    electrodes
    ions
    Autoradiography
    Electrodes
    Ions
    atomic layer epitaxy
    open circuit voltage
    ion currents
    carbonates
    ethylene
    elastic properties
    lithium
    density functional theory

    ASJC Scopus subject areas

    • Electrochemistry
    • Electronic, Optical and Magnetic Materials
    • Materials Chemistry
    • Surfaces, Coatings and Films
    • Renewable Energy, Sustainability and the Environment
    • Condensed Matter Physics

    Cite this

    Property evolution of Al2O3 coated and uncoated Si electrodes : A first principles investigation. / Kim, Sung Yup; Qi, Yue.

    In: Journal of the Electrochemical Society, Vol. 161, No. 11, 2014, p. F3137-F3143.

    Research output: Contribution to journalArticle

    Kim, Sung Yup; Qi, Yue / Property evolution of Al2O3 coated and uncoated Si electrodes : A first principles investigation.

    In: Journal of the Electrochemical Society, Vol. 161, No. 11, 2014, p. F3137-F3143.

    Research output: Contribution to journalArticle

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    abstract = "In order to compare the difference between coated and uncoated Si electrode, the basic material properties of atomic layer deposition ALD-Al2O3 coating and native SiO2 layer on Si are investigated by using density functional theory calculations. These properties include: the open circuit voltage curve with respect to lithium metal, the elastic properties, and Li ion diffusion characteristics in SiO2 and Al2O3 and their lithiated compounds (such as Li4SiO4 and LiAlO2). Results show that lithiation occurs at the voltage above EC (Ethylene Carbonate) decomposition(~0.8V) causing initial irreversible capacity loss. Also, lithiation softens Al2O3 mechanically, while slightly stiffens SiO2. For the Li ion diffusion, SiO2 and Al2O3 have totally different behavior upon lithiation. For SiO2, Li diffuses very fast, but the energy barrier becomes higher as lithiation goes on. When SiO2 is lithiated to Li4SiO4, the diffusion energy barrier becomes lower again. For Al2O3, its intrinsic ionic conductivity is very low, but the Li diffusion energy barrier becomes lower (as low as Li2Si2O5) as lithiation proceeds and LiAlO2 is formed. Therefore, designing ALD coating should target the coating properties after lithiation.",
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