Predicting Local Lithium-Plating Onset with Upscaled Models

Abstract

Lithium plating is governed by microscale transport heterogeneity, yet conventional macroscale battery models resolve only spatially-averaged quantities. In this work, we extend the dual-continuum (DC) and Doyle-Fuller-Newman (DFN) frameworks to predict local lithium-plating onset within negative-electrode microstructures while retaining the computational efficiency of upscaled approaches. A closure problem for electrolyte transport is introduced to link averaged electrolyte variables to underlying geometric features, permitting reconstruction of local lithium-plating overpotential fields from an upscaled solution. Comparison with direct numerical simulations (DNS) demonstrates that the method accurately identifies regions of highest plating risk. Beyond pinpointing where lithium plating is most likely, the closure is further used to propose a correction to the DC and DFN models, improving predictions of when plating first becomes thermodynamically favourable. We envisage two primary applications for this framework: (i) in electrode design, to efficiently evaluate candidate microstructures without resorting to computationally intensive DNS; (ii) to improve upscaled models, by enhancing their estimation of when lithium plating becomes favourable. This framework is readily extendable to study other degradation mechanisms driven by microscale transport heterogeneity. Finally, the closure problem opens a pathway to understanding the geometrical features that drive lithium-plating risk.

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BibTeX RIS

BibTeX

@article{paten2026predicting,
  title = {{Predicting Local Lithium-Plating Onset with Upscaled Models}},
  author = {Isaac B Paten and Martin Petitfrére and Céline Merlet and Romain de Loubens and Michel Quintard and Yohan Davit},
  journal = {Journal of The Electrochemical Society},
  year = {2026},
  month = sep,
  doi = {10.1149/1945-7111/ae959c},
  url = {https://hal.science/hal-05757049v1},
  note = {CC BY 4.0},
}

RIS

TY  - JOUR
TI  - Predicting Local Lithium-Plating Onset with Upscaled Models
AU  - Isaac B Paten
AU  - Martin Petitfrére
AU  - Céline Merlet
AU  - Romain de Loubens
AU  - Michel Quintard
AU  - Yohan Davit
PY  - 2026
DA  - 2026/09/21
JO  - Journal of The Electrochemical Society
DO  - 10.1149/1945-7111/ae959c
UR  - https://hal.science/hal-05757049v1
AB  - Lithium plating is governed by microscale transport heterogeneity, yet conventional macroscale battery models resolve only spatially-averaged quantities. In this work, we extend the dual-continuum (DC) and Doyle-Fuller-Newman (DFN) frameworks to predict local lithium-plating onset within negative-electrode microstructures while retaining the computational efficiency of upscaled approaches. A closure problem for electrolyte transport is introduced to link averaged electrolyte variables to underlying geometric features, permitting reconstruction of local lithium-plating overpotential fields from an upscaled solution. Comparison with direct numerical simulations (DNS) demonstrates that the method accurately identifies regions of highest plating risk. Beyond pinpointing where lithium plating is most likely, the closure is further used to propose a correction to the DC and DFN models, improving predictions of when plating first becomes thermodynamically favourable. We envisage two primary applications for this framework: (i) in electrode design, to efficiently evaluate candidate microstructures without resorting to computationally intensive DNS; (ii) to improve upscaled models, by enhancing their estimation of when lithium plating becomes favourable. This framework is readily extendable to study other degradation mechanisms driven by microscale transport heterogeneity. Finally, the closure problem opens a pathway to understanding the geometrical features that drive lithium-plating risk.
SN  - 0013-4651
SN  - 1945-7111
ER  -

Abstract

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