Lithium concentration dependent elastic properties of battery electrode materials from first principles calculations

Yue Qi, Louis G. Hector, Christine James, Kwang Jin Kim

Research output: Contribution to journalArticle

  • 67 Citations

Abstract

This paper aims to help fill a gap in the literature on Li-ion battery electrode materials due to the absence of measured elastic constants needed for diffusion induced stress models. By examining results from new first principles density functional theory (DFT) calculations of LiCoO2, LiMn2O4, (and their delithiated hosts, CoO2 and MnO2), LixAl alloys, and data from the extant literature on LiFePO4 (and FePO4), LiTi2O4 (and Li2Ti2O4), LixSi, LixSn and lihtium graphite-interaction-compounds, a compelling picture emerges on the dependency of the elastic properties on Li concentration. Specifically, three distinct categories of behavior are found: (a) the averaged Young's moduli change very minimally upon lithiation of the spinel and olivine structures; (b) lithiation induced stiffening is observed only when new and stronger bonds between the Li ions and the hostmaterials are formed in layered compounds; and (c) for alloy-forming electrode materials, such as Si, β-Sn and Al, the averaged Young's moduli of lithiated compounds follow the linear rule of mixtures. The tendency of ductile or brittle behavior electrode materials is investigated with the Pugh criterion, and a ductile to brittle transition was found to occur during lithiation of Al and β-Sn, but not in Si.

LanguageEnglish (US)
PagesF3010-F3018
JournalJournal of the Electrochemical Society
Volume161
Issue number11
DOIs
StatePublished - 2014

Profile

electrode materials
Lithium
electric batteries
elastic properties
lithium
Electrodes
modulus of elasticity
Elastic moduli
Olivine
stiffening
Graphite
Elastic constants
olivine
spinel
Density functional theory
ions
tendencies
graphite
Ions
density functional theory

ASJC Scopus subject areas

  • Electrochemistry
  • Electronic, Optical and Magnetic Materials
  • Materials Chemistry
  • Surfaces, Coatings and Films
  • Renewable Energy, Sustainability and the Environment
  • Condensed Matter Physics

Cite this

Lithium concentration dependent elastic properties of battery electrode materials from first principles calculations. / Qi, Yue; Hector, Louis G.; James, Christine; Kim, Kwang Jin.

In: Journal of the Electrochemical Society, Vol. 161, No. 11, 2014, p. F3010-F3018.

Research output: Contribution to journalArticle

@article{19e72e9202ae4b62826987ec11b96906,
title = "Lithium concentration dependent elastic properties of battery electrode materials from first principles calculations",
abstract = "This paper aims to help fill a gap in the literature on Li-ion battery electrode materials due to the absence of measured elastic constants needed for diffusion induced stress models. By examining results from new first principles density functional theory (DFT) calculations of LiCoO2, LiMn2O4, (and their delithiated hosts, CoO2 and MnO2), LixAl alloys, and data from the extant literature on LiFePO4 (and FePO4), LiTi2O4 (and Li2Ti2O4), LixSi, LixSn and lihtium graphite-interaction-compounds, a compelling picture emerges on the dependency of the elastic properties on Li concentration. Specifically, three distinct categories of behavior are found: (a) the averaged Young's moduli change very minimally upon lithiation of the spinel and olivine structures; (b) lithiation induced stiffening is observed only when new and stronger bonds between the Li ions and the hostmaterials are formed in layered compounds; and (c) for alloy-forming electrode materials, such as Si, β-Sn and Al, the averaged Young's moduli of lithiated compounds follow the linear rule of mixtures. The tendency of ductile or brittle behavior electrode materials is investigated with the Pugh criterion, and a ductile to brittle transition was found to occur during lithiation of Al and β-Sn, but not in Si.",
author = "Yue Qi and Hector, {Louis G.} and Christine James and Kim, {Kwang Jin}",
year = "2014",
doi = "10.1149/2.0031411jes",
language = "English (US)",
volume = "161",
pages = "F3010--F3018",
journal = "Journal of the Electrochemical Society",
issn = "0013-4651",
publisher = "Electrochemical Society, Inc.",
number = "11",

}

TY - JOUR

T1 - Lithium concentration dependent elastic properties of battery electrode materials from first principles calculations

AU - Qi,Yue

AU - Hector,Louis G.

AU - James,Christine

AU - Kim,Kwang Jin

PY - 2014

Y1 - 2014

N2 - This paper aims to help fill a gap in the literature on Li-ion battery electrode materials due to the absence of measured elastic constants needed for diffusion induced stress models. By examining results from new first principles density functional theory (DFT) calculations of LiCoO2, LiMn2O4, (and their delithiated hosts, CoO2 and MnO2), LixAl alloys, and data from the extant literature on LiFePO4 (and FePO4), LiTi2O4 (and Li2Ti2O4), LixSi, LixSn and lihtium graphite-interaction-compounds, a compelling picture emerges on the dependency of the elastic properties on Li concentration. Specifically, three distinct categories of behavior are found: (a) the averaged Young's moduli change very minimally upon lithiation of the spinel and olivine structures; (b) lithiation induced stiffening is observed only when new and stronger bonds between the Li ions and the hostmaterials are formed in layered compounds; and (c) for alloy-forming electrode materials, such as Si, β-Sn and Al, the averaged Young's moduli of lithiated compounds follow the linear rule of mixtures. The tendency of ductile or brittle behavior electrode materials is investigated with the Pugh criterion, and a ductile to brittle transition was found to occur during lithiation of Al and β-Sn, but not in Si.

AB - This paper aims to help fill a gap in the literature on Li-ion battery electrode materials due to the absence of measured elastic constants needed for diffusion induced stress models. By examining results from new first principles density functional theory (DFT) calculations of LiCoO2, LiMn2O4, (and their delithiated hosts, CoO2 and MnO2), LixAl alloys, and data from the extant literature on LiFePO4 (and FePO4), LiTi2O4 (and Li2Ti2O4), LixSi, LixSn and lihtium graphite-interaction-compounds, a compelling picture emerges on the dependency of the elastic properties on Li concentration. Specifically, three distinct categories of behavior are found: (a) the averaged Young's moduli change very minimally upon lithiation of the spinel and olivine structures; (b) lithiation induced stiffening is observed only when new and stronger bonds between the Li ions and the hostmaterials are formed in layered compounds; and (c) for alloy-forming electrode materials, such as Si, β-Sn and Al, the averaged Young's moduli of lithiated compounds follow the linear rule of mixtures. The tendency of ductile or brittle behavior electrode materials is investigated with the Pugh criterion, and a ductile to brittle transition was found to occur during lithiation of Al and β-Sn, but not in Si.

UR - http://www.scopus.com/inward/record.url?scp=84923358335&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84923358335&partnerID=8YFLogxK

U2 - 10.1149/2.0031411jes

DO - 10.1149/2.0031411jes

M3 - Article

VL - 161

SP - F3010-F3018

JO - Journal of the Electrochemical Society

T2 - Journal of the Electrochemical Society

JF - Journal of the Electrochemical Society

SN - 0013-4651

IS - 11

ER -