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Title: Predicting Calendar Aging in Lithium Metal Secondary Batteries: The Impacts of Solid Electrolyte Interphase Composition and Stability

Calendar aging of lithium metal batteries, in which cells’ components degrade internally due to chemical reactions while no current is being applied, is a relatively unstudied field. In this work, a model to predict calendar aging of lithium metal cells is developed using two sets of readily obtainable data: solid electrolyte interphase (SEI) layer composition (measured via X-ray photoelectron spectroscopy) and SEI stability (measured as a degradation rate using a simple constant current–constant voltage charging protocol). Electrolyte properties such as volume and salt concentration are varied in order to determine their effect on SEI stability and composition, with subsequent impacts to calendar aging. Lower salt concentrations produce a solvent-based, more soluble SEI, while the highest concentration produces a salt-based, less soluble SEI. Higher electrolyte volumes promote dissolution of the SEI and thus decrease its stability. The model predicts that lithium metal would be the limiting factor in calendar aging, depleting long before the electrolyte does. Furthermore, the relative composition of the electrolyte during aging is modeled and found to eventually converge to the same value independent of initial salt concentration.
Authors:
ORCiD logo [1] ;  [2] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ;  [2]
  1. Idaho National Lab. (INL), Idaho Falls, ID (United States)
  2. Univ. of California San Diego, La Jolla, CA (United States)
Publication Date:
Report Number(s):
INL/JOU-18-45118-Rev001
Journal ID: ISSN 1614-6832
Grant/Contract Number:
AC07-05ID14517
Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 26; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Research Org:
Idaho National Lab. (INL), Idaho Falls, ID (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; rechargeable lithium batteries; solid electrolyte interphase (SEI) layer stability; electrolyte salt concentration; electrolyte volume; lithium metal calendar life
OSTI Identifier:
1473703
Alternate Identifier(s):
OSTI ID: 1463193

Wood, Sean M., Fang, Chengcheng, Dufek, Eric J., Nagpure, Shrikant C., Sazhin, Sergiy V., Liaw, Boryann, and Meng, Y. Shirley. Predicting Calendar Aging in Lithium Metal Secondary Batteries: The Impacts of Solid Electrolyte Interphase Composition and Stability. United States: N. p., Web. doi:10.1002/aenm.201801427.
Wood, Sean M., Fang, Chengcheng, Dufek, Eric J., Nagpure, Shrikant C., Sazhin, Sergiy V., Liaw, Boryann, & Meng, Y. Shirley. Predicting Calendar Aging in Lithium Metal Secondary Batteries: The Impacts of Solid Electrolyte Interphase Composition and Stability. United States. doi:10.1002/aenm.201801427.
Wood, Sean M., Fang, Chengcheng, Dufek, Eric J., Nagpure, Shrikant C., Sazhin, Sergiy V., Liaw, Boryann, and Meng, Y. Shirley. 2018. "Predicting Calendar Aging in Lithium Metal Secondary Batteries: The Impacts of Solid Electrolyte Interphase Composition and Stability". United States. doi:10.1002/aenm.201801427.
@article{osti_1473703,
title = {Predicting Calendar Aging in Lithium Metal Secondary Batteries: The Impacts of Solid Electrolyte Interphase Composition and Stability},
author = {Wood, Sean M. and Fang, Chengcheng and Dufek, Eric J. and Nagpure, Shrikant C. and Sazhin, Sergiy V. and Liaw, Boryann and Meng, Y. Shirley},
abstractNote = {Calendar aging of lithium metal batteries, in which cells’ components degrade internally due to chemical reactions while no current is being applied, is a relatively unstudied field. In this work, a model to predict calendar aging of lithium metal cells is developed using two sets of readily obtainable data: solid electrolyte interphase (SEI) layer composition (measured via X-ray photoelectron spectroscopy) and SEI stability (measured as a degradation rate using a simple constant current–constant voltage charging protocol). Electrolyte properties such as volume and salt concentration are varied in order to determine their effect on SEI stability and composition, with subsequent impacts to calendar aging. Lower salt concentrations produce a solvent-based, more soluble SEI, while the highest concentration produces a salt-based, less soluble SEI. Higher electrolyte volumes promote dissolution of the SEI and thus decrease its stability. The model predicts that lithium metal would be the limiting factor in calendar aging, depleting long before the electrolyte does. Furthermore, the relative composition of the electrolyte during aging is modeled and found to eventually converge to the same value independent of initial salt concentration.},
doi = {10.1002/aenm.201801427},
journal = {Advanced Energy Materials},
number = 26,
volume = 8,
place = {United States},
year = {2018},
month = {8}
}