Work

Spatially resolved 3D aging model linking interdependent degradation mechanisms to knee and end-of-life prediction

Year: 2026

Type: preprint

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.

Source: ChemRxiv

DOI: 10.26434/chemrxiv.15009214/v1

Authors: Emmanuel Yerumoh, Francisco Fernandez, Lalan-Kumar Singh, Mohamed Ati, Alejandro A. Franco

Institutions: Centre National de la Recherche Scientifique, Laboratoire de Réactivité et Chimie des Solides, Université de Picardie Jules Verne, Réseau sur le Stockage Electrochimique de l'énergie

Language: English

Topic: Battery Modeling and Management

Subfield: Automotive Engineering

Field: Engineering

Domain: Physical Sciences

SDG: Affordable and clean energy

Open Access status: green

Funders: Association Nationale de la Recherche et de la Technologie, Ministère de l'Education Nationale, de l'Enseignement Superieur et de la Recherche, Institut Universitaire de France, HORIZON EUROPE Framework Programme