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.

LanguageEnglish (US)
Pages2114-2127
Number of pages14
JournalJournal of Physical Chemistry A
Volume120
Issue number13
DOIs
StatePublished - Apr 7 2016

Profile

Lithium
Silicon Dioxide
field theory (physics)
electric batteries
lithium
silicon dioxide
Electrodes
electrodes
Aluminum Oxide
Silicon
ions
Crystalline materials
aluminum oxides
Anodes
silicon
anodes
coatings
Coatings
Lithium-ion batteries
diffusivity

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

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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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