Spatially resolved 3D aging model linking interdependent degradation mechanisms to knee and end-of-life prediction
Abstract
Forecasting battery lifetime and degradation is valuable but difficult because lithium-ion batteries age through complex, non-linear processes. Physics-based models are often preferred for their mechanistic insight into key aging modes. This work introduces a 3D+1D electro-thermal-aging model coupling multiple degradation phenomena to capture lithium inventory loss (LLI), loss of active material (LAM), and impedance increase at the cell level. The model integrates a DFNbased electrochemical component with a thermal model, alongside an aging component considering solid electrolyte interface (SEI) growth, lithium plating, and transition-metal dissolution, migration, and deposition as side reactions. We calibrated the model using data from an industrial graphite/LFP cell cycled under three CCCV protocols from 10 °C to 60 °C and C/3 to 6C. The spatially resolved 3D model predicts the nonlinear capacity "knee" and sudden-death behavior, linking them to interconnected knees of LLI and impedance increase caused by localized transport limitations, matching experimental degradation rates. Our findings indicate that knee point and sudden death result from gradual yet abrupt lithium loss due to continuous lithium plating and impedance rise restricting lithium availability. This study emphasizes the need to explore how aging processes influence the knee point, helping forecast and extend battery lifespan.
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BibTeX
@misc{yerumoh2026spatially,
title = {{Spatially resolved 3D aging model linking interdependent degradation mechanisms to knee and end-of-life prediction}},
author = {Emmanuel Yerumoh and Francisco Fernandez and Lalan-Kumar Singh and Mohamed Ati and Alejandro A. Franco},
howpublished = {ChemRxiv},
year = {2026},
month = sep,
doi = {10.26434/chemrxiv.15009214/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009214/v1},
note = {CC BY},
}
RIS
TY - UNPB
TI - Spatially resolved 3D aging model linking interdependent degradation mechanisms to knee and end-of-life prediction
AU - Emmanuel Yerumoh
AU - Francisco Fernandez
AU - Lalan-Kumar Singh
AU - Mohamed Ati
AU - Alejandro A. Franco
PY - 2026
DA - 2026/09/21
PB - ChemRxiv
DO - 10.26434/chemrxiv.15009214/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009214/v1
AB - Forecasting battery lifetime and degradation is valuable but difficult because lithium-ion batteries age through complex, non-linear processes. Physics-based models are often preferred for their mechanistic insight into key aging modes. This work introduces a 3D+1D electro-thermal-aging model coupling multiple degradation phenomena to capture lithium inventory loss (LLI), loss of active material (LAM), and impedance increase at the cell level. The model integrates a DFNbased electrochemical component with a thermal model, alongside an aging component considering solid electrolyte interface (SEI) growth, lithium plating, and transition-metal dissolution, migration, and deposition as side reactions. We calibrated the model using data from an industrial graphite/LFP cell cycled under three CCCV protocols from 10 °C to 60 °C and C/3 to 6C. The spatially resolved 3D model predicts the nonlinear capacity "knee" and sudden-death behavior, linking them to interconnected knees of LLI and impedance increase caused by localized transport limitations, matching experimental degradation rates. Our findings indicate that knee point and sudden death result from gradual yet abrupt lithium loss due to continuous lithium plating and impedance rise restricting lithium availability. This study emphasizes the need to explore how aging processes influence the knee point, helping forecast and extend battery lifespan.
ER -