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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]
+ Show Author Affiliations
  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. doi:10.1149/1945-7111/ab78fa.
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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
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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.
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@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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https://doi.org/10.1149/1945-7111/ab78fa
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Cited by: 31 works
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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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