Atomic Insight into the Lithium Storage and Diffusion Mechanism of SiO2/Al2O3 Electrodes of Lithium Ion Batteries: ReaxFF Reactive Force Field Modeling

Alireza Ostadhossein, Sung Yup Kim, Ekin D. Cubuk, Yue Qi, Adri C T Van Duin

    Research output: Contribution to journalArticle

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    Abstract

    Atomically deposited layers of SiO2 and Al2O3 have been recognized as promising coating materials to buffer the volumetric expansion and capacity retention upon the chemo-mechanical cycling of the nanostructured silicon- (Si-) based electrodes. Furthermore, silica (SiO2) is known as a promising candidate for the anode of next-generation lithium ion batteries (LIBs) due to its superior specific charge capacity and low discharge potential similar to Si anodes. In order to describe Li-transport in mixed silica/alumina/silicon systems we developed a ReaxFF potential for Li-Si-O-Al interactions. Using this potential, a series of hybrid grand canonical Monte Carlo (GCMC) and molecular dynamic (MD) simulations were carried out to probe the lithiation behavior of silica structures. The Li transport through both crystalline and amorphous silica was evaluated using the newly optimized force field. The anisotropic diffusivity of Li in crystalline silica cases is demonstrated. The ReaxFF diffusion study also verifies the transferability of the new force field from crystalline to amorphous phases. Our simulation results indicates the capability of the developed force field to examine the energetics and kinetics of lithiation as well as Li transportation within the crystalline/amorphous silica and alumina phases and provide a fundamental understanding on the lithiation reactions involved in the Si electrodes covered by silica/alumina coating layers.

    Original languageEnglish (US)
    Pages (from-to)2114-2127
    Number of pages14
    JournalJournal of Physical Chemistry A
    Volume120
    Issue number13
    DOIs
    StatePublished - Apr 7 2016

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    silicon dioxide
    field theory (physics)
    Ergothioneine
    aluminum oxides
    lithium
    electrodes
    silicon
    Feline Sarcoma Viruses
    Arthrodesis
    Autoradiography
    electric batteries
    anodes
    coatings
    ions
    simulation
    Directed Tissue Donation
    Acetabularia
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    diffusivity
    buffers

    ASJC Scopus subject areas

    • Physical and Theoretical Chemistry

    Cite this

    Atomic Insight into the Lithium Storage and Diffusion Mechanism of SiO2/Al2O3 Electrodes of Lithium Ion Batteries : ReaxFF Reactive Force Field Modeling. / Ostadhossein, Alireza; Kim, Sung Yup; Cubuk, Ekin D.; Qi, Yue; Van Duin, Adri C T.

    In: Journal of Physical Chemistry A, Vol. 120, No. 13, 07.04.2016, p. 2114-2127.

    Research output: Contribution to journalArticle

    Ostadhossein, Alireza; Kim, Sung Yup; Cubuk, Ekin D.; Qi, Yue; Van Duin, Adri C T / Atomic Insight into the Lithium Storage and Diffusion Mechanism of SiO2/Al2O3 Electrodes of Lithium Ion Batteries : ReaxFF Reactive Force Field Modeling.

    In: Journal of Physical Chemistry A, Vol. 120, No. 13, 07.04.2016, p. 2114-2127.

    Research output: Contribution to journalArticle

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    abstract = "Atomically deposited layers of SiO2 and Al2O3 have been recognized as promising coating materials to buffer the volumetric expansion and capacity retention upon the chemo-mechanical cycling of the nanostructured silicon- (Si-) based electrodes. Furthermore, silica (SiO2) is known as a promising candidate for the anode of next-generation lithium ion batteries (LIBs) due to its superior specific charge capacity and low discharge potential similar to Si anodes. In order to describe Li-transport in mixed silica/alumina/silicon systems we developed a ReaxFF potential for Li-Si-O-Al interactions. Using this potential, a series of hybrid grand canonical Monte Carlo (GCMC) and molecular dynamic (MD) simulations were carried out to probe the lithiation behavior of silica structures. The Li transport through both crystalline and amorphous silica was evaluated using the newly optimized force field. The anisotropic diffusivity of Li in crystalline silica cases is demonstrated. The ReaxFF diffusion study also verifies the transferability of the new force field from crystalline to amorphous phases. Our simulation results indicates the capability of the developed force field to examine the energetics and kinetics of lithiation as well as Li transportation within the crystalline/amorphous silica and alumina phases and provide a fundamental understanding on the lithiation reactions involved in the Si electrodes covered by silica/alumina coating layers.",
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