On the role of crack electrolyte wetting in the degradation and performance of battery active particles
File(s)
Published version
Author(s)
Luza-Vega, Sebastian
Zhao, Ying
Martínez-Pañeda, Emilio
Type
Journal Article
Abstract
Cathode particle fracture is widely recognised as a major degradation mechanism in lithium-ion batteries, yet cracking also permits electrolyte wetting of newly exposed internal surfaces, modifying interfacial reaction pathways. The mechanistic role of electrolyte wetting in redistributing reactions within cracked particles remains unclear. Here, we isolate this effect through a controlled comparison between (i) a fully coupled electro-chemo-mechanical model resolving lithium concentration, electrostatic potential, and stress fields in both the active material and the electrolyte inside and outside cracks, and (ii) a single-particle chemo-mechanical model employing the conventional uniform flux assumption. The coupled model predicts strong spatial heterogeneity in interfacial reaction rates, with flux amplification approximately 8×relative to the imposed uniform flux at the crack tip. Reaction redistribution, and thus lithium flux, is governed predominantly by local solid-state lithium concentration and stress variations, while electrolyte potential gradients inside cracks remain secondary under the conditions considered. Uniform flux models can underpredict delivered capacity by 25% at 1C-rate; this discrepancy increases at higher rates. They also underestimate tensile stresses throughout the delithiation process by 10%, directly affecting crack driving conditions. These results demonstrate that neglecting crack–electrolyte coupling leads to systematic underestimation of both utilisation limits and fatigue-relevant stress histories.
Date Issued
2026-08-01
Date Acceptance
2026-05-02
Citation
Journal of Power Sources, 2026, 682
ISSN
0378-7753
Publisher
Elsevier BV
Journal / Book Title
Journal of Power Sources
Volume
682
Copyright Statement
© 2026 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
License URL
Publication Status
Published
Article Number
240307
Date Publish Online
2026-05-10