Multiphase Porous Electrode Theory
© The Author(s) 2017. Porous electrode theory, pioneered by John Newman and collaborators, provides a macroscopic description of battery cycling behavior, rooted in microscopic physical models. Typically, the active materials are described as solid solution particles with transport and surface react...
| Main Authors: | , |
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| Format: | Article |
| Language: | English |
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The Electrochemical Society
2021
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| Online Access: | https://hdl.handle.net/1721.1/134525 |
| _version_ | 1811072118186573824 |
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| author | Smith, Raymond B Bazant, Martin Z |
| author_facet | Smith, Raymond B Bazant, Martin Z |
| author_sort | Smith, Raymond B |
| collection | MIT |
| description | © The Author(s) 2017. Porous electrode theory, pioneered by John Newman and collaborators, provides a macroscopic description of battery cycling behavior, rooted in microscopic physical models. Typically, the active materials are described as solid solution particles with transport and surface reactions driven by concentration fields, and the thermodynamics are incorporated through fitting of the open circuit potential. However, this approach does not apply to phase separating materials, for which the voltage is an emergent property of inhomogeneous concentration profiles, even in equilibrium. Here, we present a general framework, "multiphase porous electrode theory", based on nonequilibrium thermodynamics and implemented in an open-source software package called "MPET". Cahn-Hilliard-type phase field models are used to describe the active materials with suitably generalized models of interfacial reaction kinetics. Classical concentrated solution theory is implemented for the electrolyte phase, and Newman's porous electrode theory is recovered in the limit of solid solution active materials with Butler-Volmer kinetics. More general, quantum-mechanical models of faradaic reactions are also included, such as Marcus-Hush-Chidsey kinetics for electron transfer at electrodes, extended for concentrated solutions. The full model and implementation are described, and a variety of example calculations are presented to illustrate the novel features of the software compared to existing battery models. |
| first_indexed | 2024-09-23T09:01:10Z |
| format | Article |
| id | mit-1721.1/134525 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T09:01:10Z |
| publishDate | 2021 |
| publisher | The Electrochemical Society |
| record_format | dspace |
| spelling | mit-1721.1/1345252022-04-01T16:26:05Z Multiphase Porous Electrode Theory Smith, Raymond B Bazant, Martin Z © The Author(s) 2017. Porous electrode theory, pioneered by John Newman and collaborators, provides a macroscopic description of battery cycling behavior, rooted in microscopic physical models. Typically, the active materials are described as solid solution particles with transport and surface reactions driven by concentration fields, and the thermodynamics are incorporated through fitting of the open circuit potential. However, this approach does not apply to phase separating materials, for which the voltage is an emergent property of inhomogeneous concentration profiles, even in equilibrium. Here, we present a general framework, "multiphase porous electrode theory", based on nonequilibrium thermodynamics and implemented in an open-source software package called "MPET". Cahn-Hilliard-type phase field models are used to describe the active materials with suitably generalized models of interfacial reaction kinetics. Classical concentrated solution theory is implemented for the electrolyte phase, and Newman's porous electrode theory is recovered in the limit of solid solution active materials with Butler-Volmer kinetics. More general, quantum-mechanical models of faradaic reactions are also included, such as Marcus-Hush-Chidsey kinetics for electron transfer at electrodes, extended for concentrated solutions. The full model and implementation are described, and a variety of example calculations are presented to illustrate the novel features of the software compared to existing battery models. 2021-10-27T20:05:25Z 2021-10-27T20:05:25Z 2017 2019-08-13T17:34:00Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/134525 en 10.1149/2.0171711JES Journal of The Electrochemical Society Creative Commons Attribution 4.0 International license https://creativecommons.org/licenses/by/4.0/ application/pdf The Electrochemical Society Electrochemical Society (ECS) |
| spellingShingle | Smith, Raymond B Bazant, Martin Z Multiphase Porous Electrode Theory |
| title | Multiphase Porous Electrode Theory |
| title_full | Multiphase Porous Electrode Theory |
| title_fullStr | Multiphase Porous Electrode Theory |
| title_full_unstemmed | Multiphase Porous Electrode Theory |
| title_short | Multiphase Porous Electrode Theory |
| title_sort | multiphase porous electrode theory |
| url | https://hdl.handle.net/1721.1/134525 |
| work_keys_str_mv | AT smithraymondb multiphaseporouselectrodetheory AT bazantmartinz multiphaseporouselectrodetheory |