Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling
The phase separation dynamics in graphitic anodes significantly affects lithium plating propensity, which is the major degradation mechanism that impairs the safety and fast charge capabilities of automotive lithium-ion batteries. In this study, we present comprehensive investigation employing opera...
| Main Authors: | , , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Article |
| Language: | English |
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Springer Science and Business Media LLC
2024
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| Online Access: | https://hdl.handle.net/1721.1/157522 |
| _version_ | 1824457925043683328 |
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| author | Lu, Xuekun Lagnoni, Marco Bertei, Antonio Das, Supratim Owen, Rhodri E Li, Qi O’Regan, Kieran Wade, Aaron Finegan, Donal P Kendrick, Emma Bazant, Martin Z Brett, Dan JL Shearing, Paul R |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Lu, Xuekun Lagnoni, Marco Bertei, Antonio Das, Supratim Owen, Rhodri E Li, Qi O’Regan, Kieran Wade, Aaron Finegan, Donal P Kendrick, Emma Bazant, Martin Z Brett, Dan JL Shearing, Paul R |
| author_sort | Lu, Xuekun |
| collection | MIT |
| description | The phase separation dynamics in graphitic anodes significantly affects lithium plating propensity, which is the major degradation mechanism that impairs the safety and fast charge capabilities of automotive lithium-ion batteries. In this study, we present comprehensive investigation employing operando high-resolution optical microscopy combined with non-equilibrium thermodynamics implemented in a multi-dimensional (1D+1D to 3D) phase-field modeling framework to reveal the rate-dependent spatial dynamics of phase separation and plating in graphite electrodes. Here we visualize and provide mechanistic understanding of the multistage phase separation, plating, inter/intra-particle lithium exchange and plated lithium back-intercalation phenomena. A strong dependence of intra-particle lithiation heterogeneity on the particle size, shape, orientation, surface condition and C-rate at the particle level is observed, which leads to early onset of plating spatially resolved by a 3D image-based phase-field model. Moreover, we highlight the distinct relaxation processes at different state-of-charges (SOCs), wherein thermodynamically unstable graphite particles undergo a drastic intra-particle lithium redistribution and inter-particle lithium exchange at intermediate SOCs, whereas the electrode equilibrates much slower at low and high SOCs. These physics-based insights into the distinct SOC-dependent relaxation efficiency provide new perspective towards developing advanced fast charge protocols to suppress plating and shorten the constant voltage regime. |
| first_indexed | 2025-02-19T04:17:44Z |
| format | Article |
| id | mit-1721.1/157522 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2025-02-19T04:17:44Z |
| publishDate | 2024 |
| publisher | Springer Science and Business Media LLC |
| record_format | dspace |
| spelling | mit-1721.1/1575222024-12-23T05:56:31Z Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling Lu, Xuekun Lagnoni, Marco Bertei, Antonio Das, Supratim Owen, Rhodri E Li, Qi O’Regan, Kieran Wade, Aaron Finegan, Donal P Kendrick, Emma Bazant, Martin Z Brett, Dan JL Shearing, Paul R Massachusetts Institute of Technology. Department of Chemical Engineering Massachusetts Institute of Technology. Department of Mathematics The phase separation dynamics in graphitic anodes significantly affects lithium plating propensity, which is the major degradation mechanism that impairs the safety and fast charge capabilities of automotive lithium-ion batteries. In this study, we present comprehensive investigation employing operando high-resolution optical microscopy combined with non-equilibrium thermodynamics implemented in a multi-dimensional (1D+1D to 3D) phase-field modeling framework to reveal the rate-dependent spatial dynamics of phase separation and plating in graphite electrodes. Here we visualize and provide mechanistic understanding of the multistage phase separation, plating, inter/intra-particle lithium exchange and plated lithium back-intercalation phenomena. A strong dependence of intra-particle lithiation heterogeneity on the particle size, shape, orientation, surface condition and C-rate at the particle level is observed, which leads to early onset of plating spatially resolved by a 3D image-based phase-field model. Moreover, we highlight the distinct relaxation processes at different state-of-charges (SOCs), wherein thermodynamically unstable graphite particles undergo a drastic intra-particle lithium redistribution and inter-particle lithium exchange at intermediate SOCs, whereas the electrode equilibrates much slower at low and high SOCs. These physics-based insights into the distinct SOC-dependent relaxation efficiency provide new perspective towards developing advanced fast charge protocols to suppress plating and shorten the constant voltage regime. 2024-11-08T20:31:44Z 2024-11-08T20:31:44Z 2023 2024-11-08T20:20:56Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/157522 Lu, X., Lagnoni, M., Bertei, A. et al. Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling. Nat Commun 14, 5127 (2023). en 10.1038/s41467-023-40574-6 Nature Communications 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 | Lu, Xuekun Lagnoni, Marco Bertei, Antonio Das, Supratim Owen, Rhodri E Li, Qi O’Regan, Kieran Wade, Aaron Finegan, Donal P Kendrick, Emma Bazant, Martin Z Brett, Dan JL Shearing, Paul R Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling |
| title | Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling |
| title_full | Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling |
| title_fullStr | Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling |
| title_full_unstemmed | Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling |
| title_short | Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling |
| title_sort | multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase field modelling |
| url | https://hdl.handle.net/1721.1/157522 |
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