ReaxFF molecular dynamics simulations on lithiated sulfur cathode materials

Md Mahbubul Islam, Alireza Ostadhossein, Oleg Borodin, A. Todd Yeates, William W. Tipton, Richard G. Hennig, Nitin Kumar, Adri C.T. Van Duin

Research output: Contribution to journalArticle

61 Citations (Scopus)

Abstract

Sulfur is a very promising cathode material for rechargeable energy storage devices. However, sulfur cathodes undergo a noticeable volume variation upon cycling, which induces mechanical stress. In spite of intensive investigation of the electrochemical behavior of the lithiated sulfur compounds, their mechanical properties are not very well understood. In order to fill this gap, we developed a ReaxFF interatomic potential to describe Li-S interactions and performed molecular dynamics (MD) simulations to study the structural, mechanical, and kinetic behavior of the amorphous lithiated sulfur (a-LixS) compounds. We examined the effect of lithiation on material properties such as ultimate strength, yield strength, and Young's modulus. Our results suggest that with increasing lithium content, the strength of lithiated sulfur compounds improves, although this increment is not linear with lithiation. The diffusion coefficients of both lithium and sulfur were computed for the a-LixS system at various stages of Li-loading. A grand canonical Monte Carlo (GCMC) scheme was used to calculate the open circuit voltage profile during cell discharge. The Li-S binary phase diagram was constructed using genetic algorithm based tools. Overall, these simulation results provide insight into the behavior of sulfur based cathode materials that are needed for developing lithium-sulfur batteries.

Original languageEnglish (US)
Pages (from-to)3383-3393
Number of pages11
JournalPhysical Chemistry Chemical Physics
Volume17
Issue number5
DOIs
StatePublished - Feb 7 2015

Fingerprint

Sulfur
Molecular dynamics
Cathodes
sulfur
cathodes
molecular dynamics
Computer simulation
Sulfur Compounds
sulfur compounds
Lithium
simulation
lithium
lithium sulfur batteries
Open circuit voltage
yield strength
energy storage
open circuit voltage
genetic algorithms
Energy storage
Phase diagrams

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Islam, M. M., Ostadhossein, A., Borodin, O., Yeates, A. T., Tipton, W. W., Hennig, R. G., ... Van Duin, A. C. T. (2015). ReaxFF molecular dynamics simulations on lithiated sulfur cathode materials. Physical Chemistry Chemical Physics, 17(5), 3383-3393. https://doi.org/10.1039/c4cp04532g
Islam, Md Mahbubul ; Ostadhossein, Alireza ; Borodin, Oleg ; Yeates, A. Todd ; Tipton, William W. ; Hennig, Richard G. ; Kumar, Nitin ; Van Duin, Adri C.T. / ReaxFF molecular dynamics simulations on lithiated sulfur cathode materials. In: Physical Chemistry Chemical Physics. 2015 ; Vol. 17, No. 5. pp. 3383-3393.
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Islam, MM, Ostadhossein, A, Borodin, O, Yeates, AT, Tipton, WW, Hennig, RG, Kumar, N & Van Duin, ACT 2015, 'ReaxFF molecular dynamics simulations on lithiated sulfur cathode materials', Physical Chemistry Chemical Physics, vol. 17, no. 5, pp. 3383-3393. https://doi.org/10.1039/c4cp04532g

ReaxFF molecular dynamics simulations on lithiated sulfur cathode materials. / Islam, Md Mahbubul; Ostadhossein, Alireza; Borodin, Oleg; Yeates, A. Todd; Tipton, William W.; Hennig, Richard G.; Kumar, Nitin; Van Duin, Adri C.T.

In: Physical Chemistry Chemical Physics, Vol. 17, No. 5, 07.02.2015, p. 3383-3393.

Research output: Contribution to journalArticle

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AU - Hennig, Richard G.

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AU - Van Duin, Adri C.T.

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Islam MM, Ostadhossein A, Borodin O, Yeates AT, Tipton WW, Hennig RG et al. ReaxFF molecular dynamics simulations on lithiated sulfur cathode materials. Physical Chemistry Chemical Physics. 2015 Feb 7;17(5):3383-3393. https://doi.org/10.1039/c4cp04532g