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Title: Ion Diffusivity through the Solid Electrolyte Interphase in Lithium-Ion Batteries

Understanding the transport properties of the solid electrolyte interface (SEI) is a critical piece in the development of lithium ion batteries (LIB) with better performance. We studied the lithium ion diffusivity in the main components of the SEI found in LIB with silicon anodes and performed classical molecular dynamics (MD) simulations on lithium fluoride (LiF), lithium oxide (Li 2O) and lithium carbonate (Li 2CO 3) in order to provide insights and to calculate the diffusion coefficients of Li-ions at temperatures in the range of 250 K to 400 K, which is within the LIB operating temperature range. We find a slight increase in the diffusivity as the temperature increases and since diffusion is noticeable at high temperatures, Li-ion diffusion in the range of 130 to 1800 K was also studied and the diffusion mechanisms involved in each SEI compound were analyzed. We observed that the predominant mechanisms of Li-ion diffusion included vacancy assisted and knock-off diffusion in LiF, direct exchange in Li 2O, and vacancy and knock-off in Li 2CO 3. Moreover, we also evaluated the effect of applied electric fields in the diffusion of Li-ions at room temperature.
Authors:
 [1] ; ORCiD logo [2]
  1. Texas A & M Univ., College Station, TX (United States). Department of Chemical Engineering and Department of Electrical and Computer Engineering
  2. Texas A & M Univ., College Station, TX (United States). Department of Chemical Engineering, Department of Electrical and Computer Engineering, and Department of Materials Science and Engineering
Publication Date:
Grant/Contract Number:
EE0007766
Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 11; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Research Org:
Texas A&M Engineering Experiment Station, College Station, TX (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; diffusion; LAMMPS; Li-ion Battery; molecular dynamics; nanotechnology; SEI
OSTI Identifier:
1430652

Benitez, Laura, and Seminario, Jorge M. Ion Diffusivity through the Solid Electrolyte Interphase in Lithium-Ion Batteries. United States: N. p., Web. doi:10.1149/2.0181711jes.
Benitez, Laura, & Seminario, Jorge M. Ion Diffusivity through the Solid Electrolyte Interphase in Lithium-Ion Batteries. United States. doi:10.1149/2.0181711jes.
Benitez, Laura, and Seminario, Jorge M. 2017. "Ion Diffusivity through the Solid Electrolyte Interphase in Lithium-Ion Batteries". United States. doi:10.1149/2.0181711jes. https://www.osti.gov/servlets/purl/1430652.
@article{osti_1430652,
title = {Ion Diffusivity through the Solid Electrolyte Interphase in Lithium-Ion Batteries},
author = {Benitez, Laura and Seminario, Jorge M.},
abstractNote = {Understanding the transport properties of the solid electrolyte interface (SEI) is a critical piece in the development of lithium ion batteries (LIB) with better performance. We studied the lithium ion diffusivity in the main components of the SEI found in LIB with silicon anodes and performed classical molecular dynamics (MD) simulations on lithium fluoride (LiF), lithium oxide (Li2O) and lithium carbonate (Li2CO3) in order to provide insights and to calculate the diffusion coefficients of Li-ions at temperatures in the range of 250 K to 400 K, which is within the LIB operating temperature range. We find a slight increase in the diffusivity as the temperature increases and since diffusion is noticeable at high temperatures, Li-ion diffusion in the range of 130 to 1800 K was also studied and the diffusion mechanisms involved in each SEI compound were analyzed. We observed that the predominant mechanisms of Li-ion diffusion included vacancy assisted and knock-off diffusion in LiF, direct exchange in Li2O, and vacancy and knock-off in Li2CO3. Moreover, we also evaluated the effect of applied electric fields in the diffusion of Li-ions at room temperature.},
doi = {10.1149/2.0181711jes},
journal = {Journal of the Electrochemical Society},
number = 11,
volume = 164,
place = {United States},
year = {2017},
month = {5}
}

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