Computational Modeling of Heterogeneity of Stress, Charge, and Cyclic Damage in Composite Electrodes of Li-Ion Batteries
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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 LiNi x Mn y Co z O 2 (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.
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Internal physical and chemical changes within lithium-ion batteries, such as stress variations, charge distribution imbalance, and cyclic damage in composite electrodes, impact SOC estimation by causing localized damage and uneven utilization of active material.
“Additionally, internal physical and chemical changes within LIBs, such as stress variations, charge distribution imbalance, and cyclic damage in composite electrodes, further impact SOC estimation by causing localized damage and uneven utilization of active material, as revealed by computational models[6]”
From Advancements in the estimation of the state of charge of lithium-ion battery: a comprehensive review of traditional and deep learning approaches (2025) · cites this paper as [6]
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Metal Release Mechanism and Electrochemical Properties of Lix(Ni1/3Mn1/3Co1/3)O2
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Concentration Distribution and Stresses in Porous Electrodes with Particle-Particle Contact
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Highly sensitive 2D X-ray absorption spectroscopy via physics informed machine learning
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Electro-Chemo-Mechanical Model for the Damage in Porous Electrodes of Lithium-Ion Batteries
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Differential pulse voltammetry analytics for lithium-ion battery degradation
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Kinetic Limitations in Single‐Crystal High‐Nickel Cathodes
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Manufacturing solid-state battery electrodes like an architect
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Analytical design of electrode particle debonding for battery applications
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- Authors
- Liu, P., Xu, R., Liu, Y., Lin, F., & Zhao, K.
- Affiliations
- Purdue University West Lafayette (US)
- SLAC National Accelerator Laboratory (US)
- Virginia Tech (US)
- Corresponding author
- Zhao, Kejie
- Venue
- Journal of The Electrochemical Society
- Publisher
- The Electrochemical Society
- Published
- 2020-01-03
- Volume
- 167
- Issue
- 4
- Pages
- 040527
- ISSN
- 0013-4651 (ISSN-L)
- 1945-7111
- OpenAlex
- W3009336421
- Cited by
- 74
- References
- 63
- Citations by year
- 2026: 6 · 2025: 8 · 2024: 13 · 2023: 14 · 2022: 16 · 2021: 14 · 2020: 3
- FWCI
- 4.04
- Type
- journal article
- Language
- en
- Open access
- hybrid
- doi.org
- Licence
- Locations
- Journal of The Electrochemical Society (publishedVersion, cc-by)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- VTechWorks (Virginia Tech) (submittedVersion, cc-by)
- Funders
- National Science Foundation (CBET-1603866)
- Topics
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advancements in Battery Materials
- Physical Sciences › Engineering › Automotive Engineering › Advanced Battery Technologies Research
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced Battery Materials and Technologies
- Keywords
- lithium-ion batteries, composite electrodes, charge heterogeneity, NCM cathode, stress heterogeneity, cyclic damage, debonding, synchrotron X-ray tomography, Li+ transport, capacity fade, redox kinetics, mass transfer
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