Phase Transformation Dynamics in Porous Battery Electrodes
Porous electrodes composed of multiphase active materials are widely used in Li-ion batteries, but their dynamics are poorly understood. Two-phase models are largely empirical, and no models exist for three or more phases. Using a modified porous electrode theory based on non-equilibrium thermodynam...
| Main Authors: | , |
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| Other Authors: | |
| Format: | Article |
| Language: | en_US |
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Elsevier
2017
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| Online Access: | http://hdl.handle.net/1721.1/109043 |
| _version_ | 1826217120020561920 |
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| author | Ferguson, Todd Richard Bazant, Martin Z |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Ferguson, Todd Richard Bazant, Martin Z |
| author_sort | Ferguson, Todd Richard |
| collection | MIT |
| description | Porous electrodes composed of multiphase active materials are widely used in Li-ion batteries, but their dynamics are poorly understood. Two-phase models are largely empirical, and no models exist for three or more phases. Using a modified porous electrode theory based on non-equilibrium thermodynamics, we show that experimental phase behavior can be accurately predicted from free energy models, without artificially placing phase boundaries or fitting the open circuit voltage. First, we simulate lithium intercalation in porous iron phosphate, a popular two-phase cathode, and show that the zero-current voltage gap, sloping voltage plateau and under-estimated exchange currents all result from size-dependent nucleation and mosaic instability. Next, we simulate porous graphite, the standard anode with three stable phases, and reproduce experimentally observed fronts of color-changing phase transformations. These results provide a framework for physics-based design and control for electrochemical systems with complex thermodynamics. |
| first_indexed | 2024-09-23T16:58:19Z |
| format | Article |
| id | mit-1721.1/109043 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T16:58:19Z |
| publishDate | 2017 |
| publisher | Elsevier |
| record_format | dspace |
| spelling | mit-1721.1/1090432022-09-29T22:47:46Z Phase Transformation Dynamics in Porous Battery Electrodes Ferguson, Todd Richard Bazant, Martin Z Massachusetts Institute of Technology. Department of Chemical Engineering Massachusetts Institute of Technology. Department of Mathematics Ferguson, Todd Richard Bazant, Martin Z Porous electrodes composed of multiphase active materials are widely used in Li-ion batteries, but their dynamics are poorly understood. Two-phase models are largely empirical, and no models exist for three or more phases. Using a modified porous electrode theory based on non-equilibrium thermodynamics, we show that experimental phase behavior can be accurately predicted from free energy models, without artificially placing phase boundaries or fitting the open circuit voltage. First, we simulate lithium intercalation in porous iron phosphate, a popular two-phase cathode, and show that the zero-current voltage gap, sloping voltage plateau and under-estimated exchange currents all result from size-dependent nucleation and mosaic instability. Next, we simulate porous graphite, the standard anode with three stable phases, and reproduce experimentally observed fronts of color-changing phase transformations. These results provide a framework for physics-based design and control for electrochemical systems with complex thermodynamics. National Science Foundation (U.S.) (Contract DMS-0948071) Samsung-MIT Alliance 2017-05-12T15:29:12Z 2017-05-12T15:29:12Z 2014-09 2014-08 Article http://purl.org/eprint/type/JournalArticle 00134686 http://hdl.handle.net/1721.1/109043 Ferguson, Todd R., and Martin Z. Bazant. “Phase Transformation Dynamics in Porous Battery Electrodes.” Electrochimica Acta 146 (November 2014): 89–97. en_US http://dx.doi.org/10.1016/j.electacta.2014.08.083 Electrochimica Acta Creative Commons Attribution-NonCommercial-NoDerivs License http://creativecommons.org/licenses/by-nc-nd/4.0/ application/pdf Elsevier arXiv |
| spellingShingle | Ferguson, Todd Richard Bazant, Martin Z Phase Transformation Dynamics in Porous Battery Electrodes |
| title | Phase Transformation Dynamics in Porous Battery Electrodes |
| title_full | Phase Transformation Dynamics in Porous Battery Electrodes |
| title_fullStr | Phase Transformation Dynamics in Porous Battery Electrodes |
| title_full_unstemmed | Phase Transformation Dynamics in Porous Battery Electrodes |
| title_short | Phase Transformation Dynamics in Porous Battery Electrodes |
| title_sort | phase transformation dynamics in porous battery electrodes |
| url | http://hdl.handle.net/1721.1/109043 |
| work_keys_str_mv | AT fergusontoddrichard phasetransformationdynamicsinporousbatteryelectrodes AT bazantmartinz phasetransformationdynamicsinporousbatteryelectrodes |