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Title: Computational Modeling of Heterogeneity of Stress, Charge, and Cyclic Damage in Composite Electrodes of Li-Ion Batteries

Abstract

Charge heterogeneity is a prevalent feature in many electrochemical systems. In a commercial cathode of Li-ion batteries, the composite is hierarchically structured across multiple length scales including the sub-micron single-crystal primary-particle domains up to the macroscopic particle ensembles. The redox kinetics of charge transfer and mass transport strongly couples with mechanical stresses. This interplay catalyzes substantial heterogeneity in the charge (re)distribution, stresses, and mechanical damage in the composite electrode during charging and discharging. We assess the heterogeneous electrochemistry and mechanics in a LiNixMnyCozO2 (NMC) cathode using a fully coupled electro-chemo-mechanics model at the cell level. A microstructure-resolved model is constructed based on the synchrotron X-ray tomography data. We calculate the stress field in the composite and then quantitatively evaluate the kinetics of surface charge transfer and Li transport biased by mechanical stresses. We further model the cyclic behavior of the cell. The repetitive deformation of the active particles and the weakening of the interfacial strength cause gradual increase of the interfacial debonding. The mechanical damage impedes electron transfer, incurs more charge heterogeneity, and results in the capacity degradation in batteries over cycles.

Authors:
 [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [2]
  1. Xi'an Jiaotong Univ., Shaanxi (China); Purdue Univ., West Lafayette, IN (United States)
  2. Purdue Univ., West Lafayette, IN (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1638245
Grant/Contract Number:  
AC02-76SF00515; CBET-1603866
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society (Online)
Additional Journal Information:
Journal Name: Journal of the Electrochemical Society (Online); Journal Volume: 167; Journal Issue: 4; Journal ID: ISSN 1945-7111
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Liu, Pengfei, Xu, Rong, Liu, Yijin, Lin, Feng, and Zhao, Kejie. Computational Modeling of Heterogeneity of Stress, Charge, and Cyclic Damage in Composite Electrodes of Li-Ion Batteries. United States: N. p., 2020. Web. https://doi.org/10.1149/1945-7111/ab78fa.
Liu, Pengfei, Xu, Rong, Liu, Yijin, Lin, Feng, & Zhao, Kejie. Computational Modeling of Heterogeneity of Stress, Charge, and Cyclic Damage in Composite Electrodes of Li-Ion Batteries. United States. https://doi.org/10.1149/1945-7111/ab78fa
Liu, Pengfei, Xu, Rong, Liu, Yijin, Lin, Feng, and Zhao, Kejie. Thu . "Computational Modeling of Heterogeneity of Stress, Charge, and Cyclic Damage in Composite Electrodes of Li-Ion Batteries". United States. https://doi.org/10.1149/1945-7111/ab78fa. https://www.osti.gov/servlets/purl/1638245.
@article{osti_1638245,
title = {Computational Modeling of Heterogeneity of Stress, Charge, and Cyclic Damage in Composite Electrodes of Li-Ion Batteries},
author = {Liu, Pengfei and Xu, Rong and Liu, Yijin and Lin, Feng and Zhao, Kejie},
abstractNote = {Charge heterogeneity is a prevalent feature in many electrochemical systems. In a commercial cathode of Li-ion batteries, the composite is hierarchically structured across multiple length scales including the sub-micron single-crystal primary-particle domains up to the macroscopic particle ensembles. The redox kinetics of charge transfer and mass transport strongly couples with mechanical stresses. This interplay catalyzes substantial heterogeneity in the charge (re)distribution, stresses, and mechanical damage in the composite electrode during charging and discharging. We assess the heterogeneous electrochemistry and mechanics in a LiNixMnyCozO2 (NMC) cathode using a fully coupled electro-chemo-mechanics model at the cell level. A microstructure-resolved model is constructed based on the synchrotron X-ray tomography data. We calculate the stress field in the composite and then quantitatively evaluate the kinetics of surface charge transfer and Li transport biased by mechanical stresses. We further model the cyclic behavior of the cell. The repetitive deformation of the active particles and the weakening of the interfacial strength cause gradual increase of the interfacial debonding. The mechanical damage impedes electron transfer, incurs more charge heterogeneity, and results in the capacity degradation in batteries over cycles.},
doi = {10.1149/1945-7111/ab78fa},
journal = {Journal of the Electrochemical Society (Online)},
number = 4,
volume = 167,
place = {United States},
year = {2020},
month = {3}
}

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Figures / Tables:

Figure 1 Figure 1: Overview of chemomechanical degradation in battery materials as a result of the interplay between mechanics, mass transport, and interfacial redox reactions. The electrochemical processes of Li diffusion and charge transfer modulate the deformation and damage of electrodes, likewise, the mechanical stress regulates the kinetics of diffusion and interfacialmore » reaction and impacts the polarization, voltage, capacity, and cyclic efficiency of the electrochemical system.« less

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Works referenced in this record:

The mechanics of large-volume-change transformations in high-capacity battery materials
journal, December 2016


Multiscale Morphological and Electrical Characterization of Charge Transport Limitations to the Power Performance of Positive Electrode Blends for Lithium-Ion Batteries
journal, December 2016

  • Besnard, Nicolas; Etiemble, Aurélien; Douillard, Thierry
  • Advanced Energy Materials, Vol. 7, Issue 8
  • DOI: 10.1002/aenm.201602239

Isogeometric analysis of mechanically coupled Cahn–Hilliard phase segregation in hyperelastic electrodes of Li-ion batteries
journal, December 2015

  • Zhao, Ying; Stein, Peter; Xu, Bai-Xiang
  • Computer Methods in Applied Mechanics and Engineering, Vol. 297
  • DOI: 10.1016/j.cma.2015.09.008

Effects of surface tension and electrochemical reactions in Li-ion battery electrode nanoparticles
journal, November 2016


Grid indentation analysis of mechanical properties of composite electrodes in Li-ion batteries
journal, December 2016


Particle Size Polydispersity in Li-Ion Batteries
journal, December 2013

  • Chung, Ding-Wen; Shearing, Paul R.; Brandon, Nigel P.
  • Journal of The Electrochemical Society, Vol. 161, Issue 3
  • DOI: 10.1149/2.097403jes

Quantification of Heterogeneous Degradation in Li‐Ion Batteries
journal, May 2019


First-Principles Calculations of Lithium-Ion Migration at a Coherent Grain Boundary in a Cathode Material, LiCoO 2
journal, November 2012

  • Moriwake, Hiroki; Kuwabara, Akihide; Fisher, Craig A. J.
  • Advanced Materials, Vol. 25, Issue 4
  • DOI: 10.1002/adma.201202805

A nonlinear theory of thermochemical equilibrium of solids under stress
journal, January 1978


Modeling the impedance versus voltage characteristics of LiNi0.8Co0.15Al0.05O2
journal, January 2008


Mechanical and Structural Degradation of LiNi x Mn y Co z O 2 Cathode in Li-Ion Batteries: An Experimental Study
journal, January 2017

  • Xu, Rong; Sun, Hong; de Vasconcelos, Luize Scalco
  • Journal of The Electrochemical Society, Vol. 164, Issue 13
  • DOI: 10.1149/2.1751713jes

Three-Dimensional Finite Element Study on Li Diffusion Induced Stress in FIB-SEM Reconstructed LiCoO2 Half Cell
journal, December 2016


Mechanical interactions regulated kinetics and morphology of composite electrodes in Li-ion batteries
journal, September 2016


Trap effects on vacancy defect of C3N as anode material in Li-ion battery
journal, May 2019


Visualization and Quantification of Electrochemical and Mechanical Degradation in Li Ion Batteries
journal, October 2013


Understanding the role of mechanics in energy materials: A perspective
journal, December 2016


A linear theory of thermochemical equilibrium of solids under stress
journal, August 1973


3D Isogeometric Analysis of intercalation-induced stresses in Li-ion battery electrode particles
journal, January 2014


Persistent State-of-Charge Heterogeneity in Relaxed, Partially Charged Li 1− x Ni 1/3 Co 1/3 Mn 1/3 O 2 Secondary Particles
journal, May 2016

  • Gent, William E.; Li, Yiyang; Ahn, Sungjin
  • Advanced Materials, Vol. 28, Issue 31
  • DOI: 10.1002/adma.201601273

Electrochemomechanical degradation of high-capacity battery electrode materials
journal, August 2017


Deformation and stress in electrode materials for Li-ion batteries
journal, June 2014


The Impact of Elastic Deformation on Deposition Kinetics at Lithium/Polymer Interfaces
journal, January 2005

  • Monroe, Charles; Newman, John
  • Journal of The Electrochemical Society, Vol. 152, Issue 2
  • DOI: 10.1149/1.1850854

Stress fields in hollow core–shell spherical electrodes of lithium ion batteries
journal, December 2014

  • Liu, Yingjie; Lv, Pengyu; Ma, Jun
  • Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 470, Issue 2172
  • DOI: 10.1098/rspa.2014.0299

Solid-state diffusion limitations on pulse operation of a lithium ion cell for hybrid electric vehicles
journal, October 2006


High‐Voltage Charging‐Induced Strain, Heterogeneity, and Micro‐Cracks in Secondary Particles of a Nickel‐Rich Layered Cathode Material
journal, March 2019

  • Mao, Yuwei; Wang, Xuelong; Xia, Sihao
  • Advanced Functional Materials, Vol. 29, Issue 18
  • DOI: 10.1002/adfm.201900247

Effect of Misfit Dislocation on Li Diffusion and Stress in a Phase Transforming Spherical Electrode
journal, January 2015

  • Chen, Bingbing; Zhou, Jianqiu; Zhu, Jianwei
  • Journal of The Electrochemical Society, Vol. 162, Issue 8
  • DOI: 10.1149/2.0061508jes

Defects Mediated Corrosion in Graphene Coating Layer
journal, March 2017

  • Lei, Jincheng; Hu, Yaowu; Liu, Zishun
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 13
  • DOI: 10.1021/acsami.7b01539

Impedance as a Tool for Investigating Aging in Lithium-Ion Porous Electrodes
journal, January 2008

  • Brown, Shelley; Mellgren, Niklas; Vynnycky, Michael
  • Journal of The Electrochemical Society, Vol. 155, Issue 4
  • DOI: 10.1149/1.2832654

Ageing mechanisms in lithium-ion batteries
journal, September 2005


Defects and lithium migration in Li2CuO2
journal, April 2018

  • Kordatos, Apostolos; Kuganathan, Navaratnarajah; Kelaidis, Nikolaos
  • Scientific Reports, Vol. 8, Issue 1
  • DOI: 10.1038/s41598-018-25239-5

Modeling Lithium Intercalation of Single-Fiber Carbon Microelectrodes
journal, January 1996

  • Verbrugge, Mark W.
  • Journal of The Electrochemical Society, Vol. 143, Issue 2
  • DOI: 10.1149/1.1836486

Disintegration of Meatball Electrodes for LiNi x Mn y Co z O2 Cathode Materials
journal, May 2017


On the origin and application of the Bruggeman correlation for analysing transport phenomena in electrochemical systems
journal, May 2016

  • Tjaden, Bernhard; Cooper, Samuel J.; Brett, Daniel JL
  • Current Opinion in Chemical Engineering, Vol. 12
  • DOI: 10.1016/j.coche.2016.02.006

Inelastic shape changes of silicon particles and stress evolution at binder/particle interface in a composite electrode during lithiation/delithiation cycling
journal, December 2016


Heterogeneous damage in Li-ion batteries: Experimental analysis and theoretical modeling
journal, August 2019


Computational analysis of chemomechanical behaviors of composite electrodes in Li-ion batteries
journal, August 2016

  • Xu, Rong; Scalco de Vasconcelos, Luize; Zhao, Kejie
  • Journal of Materials Research, Vol. 31, Issue 18
  • DOI: 10.1557/jmr.2016.302

Transport Properties of LiPF[sub 6]-Based Li-Ion Battery Electrolytes
journal, January 2005

  • Valo̸en, Lars Ole; Reimers, Jan N.
  • Journal of The Electrochemical Society, Vol. 152, Issue 5
  • DOI: 10.1149/1.1872737

Mesoscale Battery Science: The Behavior of Electrode Particles Caught on a Multispectral X-ray Camera
journal, June 2018


Modeling of Galvanostatic Charge and Discharge of the Lithium/Polymer/Insertion Cell
journal, January 1993

  • Doyle, Marc
  • Journal of The Electrochemical Society, Vol. 140, Issue 6
  • DOI: 10.1149/1.2221597

Modeling, validation and analysis of mechanical stress generation and dimension changes of a pouch type high power Li-ion battery
journal, February 2013


GITT studies on oxide cathode LiNi1/3Co1/3Mn1/3O2 synthesized by citric acid assisted high-energy ball milling
journal, June 2013


Capacity fade study of lithium-ion batteries cycled at high discharge rates
journal, May 2003


Modeling Lithium Intercalation in a Porous Carbon Electrode
journal, January 2001

  • Botte, Gerardine G.; White, Ralph E.
  • Journal of The Electrochemical Society, Vol. 148, Issue 1
  • DOI: 10.1149/1.1344517

Microstructural Modeling and Design of Rechargeable Lithium-Ion Batteries
journal, January 2005

  • Garcı́a, R. Edwin; Chiang, Yet-Ming; Craig Carter, W.
  • Journal of The Electrochemical Society, Vol. 152, Issue 1
  • DOI: 10.1149/1.1836132

Materials Challenges Facing Electrical Energy Storage
journal, April 2008


Mechanical and Electrochemical Response of a LiCoO2 Cathode using Reconstructed Microstructures
journal, February 2016


Quantification and modeling of mechanical degradation in lithium-ion batteries based on nanoscale imaging
journal, June 2018


Stress generation and fracture in lithium insertion materials
journal, March 2006


Effect of Compressive Stress on Electrochemical Performance of Silicon Anodes
journal, November 2012

  • Piper, Daniela Molina; Yersak, Thomas A.; Lee, Se-Hee
  • Journal of The Electrochemical Society, Vol. 160, Issue 1
  • DOI: 10.1149/2.064301jes

Evolution of stress within a spherical insertion electrode particle under potentiostatic and galvanostatic operation
journal, May 2009


Phase-field study of electrochemical reactions at exterior and interior interfaces in Li-ion battery electrode particles
journal, December 2016

  • Zhao, Ying; Xu, Bai-Xiang; Stein, Peter
  • Computer Methods in Applied Mechanics and Engineering, Vol. 312
  • DOI: 10.1016/j.cma.2016.04.033

Theoretical Analysis of Stresses in a Lithium Ion Cell
journal, January 2010

  • Renganathan, Sindhuja; Sikha, Godfrey; Santhanagopalan, Shriram
  • Journal of The Electrochemical Society, Vol. 157, Issue 2
  • DOI: 10.1149/1.3261809

Generation and Distribution of Dislocations by Solute Diffusion
journal, October 1961