Thermodynamics of multi-sublattice battery active materials: from an extended regular solution theory to a phase-field model of LiMnyFe1-yPO4
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, performan...
| Main Authors: | , , , |
|---|---|
| Other Authors: | |
| Format: | Article |
| Language: | English |
| Published: |
Springer Science and Business Media LLC
2024
|
| Online Access: | https://hdl.handle.net/1721.1/157444 |
| _version_ | 1824458308974542848 |
|---|---|
| author | Ombrini, Pierfrancesco Bazant, Martin Z Wagemaker, Marnix Vasileiadis, Alexandros |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Ombrini, Pierfrancesco Bazant, Martin Z Wagemaker, Marnix Vasileiadis, Alexandros |
| author_sort | Ombrini, Pierfrancesco |
| collection | MIT |
| description | 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. |
| first_indexed | 2025-02-19T04:23:50Z |
| format | Article |
| id | mit-1721.1/157444 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2025-02-19T04:23:50Z |
| publishDate | 2024 |
| publisher | Springer Science and Business Media LLC |
| record_format | dspace |
| spelling | mit-1721.1/1574442025-01-03T04:31:34Z Thermodynamics of multi-sublattice battery active materials: from an extended regular solution theory to a phase-field model of LiMnyFe1-yPO4 Ombrini, Pierfrancesco Bazant, Martin Z Wagemaker, Marnix Vasileiadis, Alexandros Massachusetts Institute of Technology. Department of Chemical Engineering Massachusetts Institute of Technology. Department of Mathematics 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. 2024-10-30T16:19:56Z 2024-10-30T16:19:56Z 2023 2024-10-28T20:04:00Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/157444 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). en 10.1038/s41524-023-01109-1 npj Computational Materials Creative Commons Attribution https://creativecommons.org/licenses/by/4.0/ application/pdf Springer Science and Business Media LLC Springer Science and Business Media LLC |
| spellingShingle | Ombrini, Pierfrancesco Bazant, Martin Z Wagemaker, Marnix Vasileiadis, Alexandros Thermodynamics of multi-sublattice battery active materials: from an extended regular solution theory to a phase-field model of LiMnyFe1-yPO4 |
| title | Thermodynamics of multi-sublattice battery active materials: from an extended regular solution theory to a phase-field model of LiMnyFe1-yPO4 |
| title_full | Thermodynamics of multi-sublattice battery active materials: from an extended regular solution theory to a phase-field model of LiMnyFe1-yPO4 |
| title_fullStr | Thermodynamics of multi-sublattice battery active materials: from an extended regular solution theory to a phase-field model of LiMnyFe1-yPO4 |
| title_full_unstemmed | Thermodynamics of multi-sublattice battery active materials: from an extended regular solution theory to a phase-field model of LiMnyFe1-yPO4 |
| title_short | Thermodynamics of multi-sublattice battery active materials: from an extended regular solution theory to a phase-field model of LiMnyFe1-yPO4 |
| title_sort | thermodynamics of multi sublattice battery active materials from an extended regular solution theory to a phase field model of limnyfe1 ypo4 |
| url | https://hdl.handle.net/1721.1/157444 |
| work_keys_str_mv | AT ombrinipierfrancesco thermodynamicsofmultisublatticebatteryactivematerialsfromanextendedregularsolutiontheorytoaphasefieldmodeloflimnyfe1ypo4 AT bazantmartinz thermodynamicsofmultisublatticebatteryactivematerialsfromanextendedregularsolutiontheorytoaphasefieldmodeloflimnyfe1ypo4 AT wagemakermarnix thermodynamicsofmultisublatticebatteryactivematerialsfromanextendedregularsolutiontheorytoaphasefieldmodeloflimnyfe1ypo4 AT vasileiadisalexandros thermodynamicsofmultisublatticebatteryactivematerialsfromanextendedregularsolutiontheorytoaphasefieldmodeloflimnyfe1ypo4 |