Thermodynamics of multi-sublattice battery active materials: from an extended regular solution theory to a phase-field model of LiMnyFe1-yPO4
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s41524-023-01109-1.pdf
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Published version
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1.97 MB
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Author(s)
Ombrini, Pierfrancesco
Bazant, Martin Z
Wagemaker, Marnix
Vasileiadis, Alexandros
Date Issued
2023
Journal
npj Computational Materials
Publisher
Springer Science and Business Media LLC
Citation
Ombrini, P., Bazant, M.Z., Wagemaker, M. et al. Thermodynamics of multi-sublattice battery active materials: from an extended regular solution theory to a phase-field model of LiMnyFe1-yPO4. npj Comput Mater 9, 148 (2023).
Version
Final published version
Abstract
Phase separation during the lithiation of redox-active materials is a critical factor affecting battery performance, including energy density, charging rates, and cycle life. Accurate physical descriptions of these materials are necessary for understanding underlying lithiation mechanisms, performance limitations, and optimizing energy storage devices. This work presents an extended regular solution model that captures mutual interactions between sublattices of multi-sublattice battery materials, typically synthesized by metal substitution. We apply the model to phospho-olivine materials and demonstrate its quantitative accuracy in predicting the composition-dependent redox shift of the plateaus of LiMnyFe1-yPO4 (LFMP), LiCoyFe1-yPO4 (LFCP), LiCoxMnyFe1-x-yPO4 (LFMCP), as well as their phase separation behavior. Furthermore, we develop a phase-field model of LFMP that consistently matches experimental data and identifies LiMn0.4Fe0.6PO4 as a superior composition that favors a solid solution phase transition, making it ideal for high-power applications.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Mathematics
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DOI of Published Version
https://doi.org/10.1038/s41524-023-01109-1
