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Safety and performance implications of lithium plating induced by sub-zero temperature cycling of lithium-ion batteries

Kirchner-Burles, Charles; Fordham, Arthur; Reid, Hamish T; Johnson, Michael; Buckwell, Mark; Iacoviello, Francesco; Coke, Kofi; ... Robinson, James B; + view all (2025) Safety and performance implications of lithium plating induced by sub-zero temperature cycling of lithium-ion batteries. Journal of Power Sources , 660 , Article 238565. 10.1016/j.jpowsour.2025.238565. Green open access

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Abstract

The operation of lithium-ion cells at sub-zero temperatures can result in the deposition of metallic lithium onto the surface of the negative electrode. The resulting lithium deposits have substantial ramifications for the performance and safety of the cell, with rapid capacity fade and reduced thermal stability both exhibited in cells aged under these conditions. In this study, it is found that extending the cycling temperatures of these cells to sub-zero temperatures results in a change in plating behaviour, with cells cycled at −10 °C exhibiting reversible plating behaviour and cells cycled at −20 °C plating irreversibly instead. Additionally, the nature of the plating is observed to transition from reversible to irreversible with progressive ageing in the cells cycled at −10 °C. Using operando electrochemical analysis such as voltage relaxation and Coulombic efficiency (CE) measurement, characteristics of the degradation are revealed. Electrochemical impedance spectroscopy (EIS) is also employed between cycles to provide information on the changes in internal cell processes due to plating. Ex-situ investigations complement the analysis allowing images of electrode condition to be collected. In-situ X-ray computed tomography further highlights how lithium plating compromises the structural integrity of the internal cell architecture, leading to increased safety concerns. Testing the aged cells with accelerated rate calorimetry also shows that the presence of more strongly reductive metallic lithium within a cell results in lower onset temperatures for self-heating and thermal runaway, plus an increased potential for projectiles during failure.

Type: Article
Title: Safety and performance implications of lithium plating induced by sub-zero temperature cycling of lithium-ion batteries
Open access status: An open access version is available from UCL Discovery
DOI: 10.1016/j.jpowsour.2025.238565
Publisher version: https://doi.org/10.1016/j.jpowsour.2025.238565
Language: English
Additional information: This work is licensed under a Creative Commons License. The images or other third-party material in this article are included in the Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/10215263
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