Print Email Facebook Twitter Thermodynamics of multi-sublattice battery active materials Title Thermodynamics of multi-sublattice battery active materials: from an extended regular solution theory to a phase-field model of LiMnyFe1-yPO4 Author Ombrini, P. (TU Delft RST/Storage of Electrochemical Energy) Bazant, Martin Z. (Massachusetts Institute of Technology) Wagemaker, M. (TU Delft RST/Storage of Electrochemical Energy) Vasileiadis, A. (TU Delft RST/Storage of Electrochemical Energy) Date 2023 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. To reference this document use: http://resolver.tudelft.nl/uuid:01469449-f076-4c01-9873-88a2ae91e36c DOI https://doi.org/10.1038/s41524-023-01109-1 ISSN 2057-3960 Source npj Computational Materials, 9 (1) Part of collection Institutional Repository Document type journal article Rights © 2023 P. Ombrini, Martin Z. Bazant, M. Wagemaker, A. Vasileiadis Files PDF s41524_023_01109_1.pdf 2.07 MB Close viewer /islandora/object/uuid:01469449-f076-4c01-9873-88a2ae91e36c/datastream/OBJ/view