Physicochemically-informed continuum level model of a solid electrolyte interphase growth in Li-ion batteries

Zelič, Klemen (author), Esmaeilpour, Meysam (author), Jana, Saibal (author), Mele, Igor (author), Wenzel, Wolfgang (author), Katrašnik, Tomaž (author)

Despite extensive research, understanding the SEI’s formation mechanism, structure, and its impact on battery performance remains challenging due to its complexity. To enable model-based design studies and to enhance understanding and prediction of the macroscopically observable consequences of SEI layer on battery performance and safety, continuum models featuring high level of prediction capability are needed. This objective of this paper is to resolve this challenge through an innovative physicochemically-informed continuum level model derived using a scale-bridging methodology, which, for the first time, enables highly consistent transfer of detailed KMC level based governing equations and reactions rates to the physicochemically-informed continuum level model. This was made possible by the innovative methodology relying on identification of rate-limiting reactions, deriving dynamic equations, and implementing dimensionality reduction. The resulting continuum model accurately replicates KMC results and experimental results while significantly reducing computational complexity. Furthermore, it, for the first time, enables distinguishing between ‘bad’, ‘good’, and ‘inorganic’ SEI growth scenarios on the continuum scale, offering valuable insights into electrode/electrolyte interface design. Due to its computational efficiency and scalability the proposed model can be integrated into higher-scale battery models, making possible advanced virtual performance, degradation and safety assessments with higher level of prediction capability.

• Language: English
• Keywords: Li-ion batteries, solid electrolyte interphase, molecular dynamics, kinetic Monte Carlo, continuum model, scale-bridging
• Work type: Article
• Typology: 1.01 - Original Scientific Article
• Organization: FS - Faculty of Mechanical Engineering
• Publication status: Published
• Publication version: Version of Record
• Year: 2025
• Number of pages: 11 str.
• Numbering: Vol. 627, [art. no.] 235814
• PID: 20.500.12556/RUL-164982
• UDC: 621.3
• ISSN on article: 0378-7753
• DOI: 10.1016/j.jpowsour.2024.235814
• COBISS.SI-ID: 215623427
• Publication date in RUL: 19.11.2024

Record is a part of a journal

• Title: Journal of power sources
• Shortened title: J. power sources
• Publisher: Elsevier Sequoia
• ISSN: 0378-7753
• COBISS.SI-ID: 25782784

Licences

• License: CC BY-NC-ND 4.0, Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International
• Link: http://creativecommons.org/licenses/by-nc-nd/4.0/
• Description: The most restrictive Creative Commons license. This only allows people to download and share the work for no commercial gain and for no other purposes.

Secondary language

• Language: Slovenian
• Keywords: Litij ionske baterije, medfazni sloji, molekularna dinamika, kinetični Monte Karlo, kontinuumski model, prehod med skalam