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

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62 Scopus citations

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

All Science Journal Classification (ASJC) codes

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

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    Islam, M. M., Ostadhossein, A., Borodin, O., Yeates, A. T., Tipton, W. W., Hennig, R. G., Kumar, N., & 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