Spatial dynamics of lithiation and lithium plating during high-rate operation of graphite electrodes
© 2020 The Royal Society of Chemistry. The principal inhibitor of fast charging lithium ion cells is the graphite negative electrode, where favorable conditions for lithium plating occur at high charge rates, causing accelerated degradation and safety concerns. The local response of graphite, both a...
| Main Authors: | , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Royal Society of Chemistry (RSC)
2021
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| Online Access: | https://hdl.handle.net/1721.1/135404 |
| _version_ | 1826210557628252160 |
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| author | Finegan, Donal P Quinn, Alexander Wragg, David S Colclasure, Andrew M Lu, Xuekun Tan, Chun Heenan, Thomas MM Jervis, Rhodri Brett, Dan JL Das, Supratim Gao, Tao Cogswell, Daniel A Bazant, Martin Z Di Michiel, Marco Checchia, Stefano Shearing, Paul R Smith, Kandler |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Finegan, Donal P Quinn, Alexander Wragg, David S Colclasure, Andrew M Lu, Xuekun Tan, Chun Heenan, Thomas MM Jervis, Rhodri Brett, Dan JL Das, Supratim Gao, Tao Cogswell, Daniel A Bazant, Martin Z Di Michiel, Marco Checchia, Stefano Shearing, Paul R Smith, Kandler |
| author_sort | Finegan, Donal P |
| collection | MIT |
| description | © 2020 The Royal Society of Chemistry. The principal inhibitor of fast charging lithium ion cells is the graphite negative electrode, where favorable conditions for lithium plating occur at high charge rates, causing accelerated degradation and safety concerns. The local response of graphite, both at the electrode and particle level, when exposed to fast charging conditions of around 6C is not well understood. Consequently, the conditions that lead to the onset of lithium plating, as well as the local dynamics of lithium plating and stripping, have also remained elusive. Here, we use high-speed (100 Hz) pencil-beam X-ray diffraction to repeatedly raster along the depth of a 101 µm thick graphite electrode in 3 µm steps during fast (up to 6C) charge and discharge conditions. Consecutive depth profiles from separator to current collector were each captured in 0.5 seconds, giving an unprecedented spatial and temporal description of the state of the electrode and graphite's staging dynamics during high rate conditions. The electrode is preferentially activated near the separator, and the non-uniformity increases with rate and is influenced by free-energy barriers between graphite's lithiation stages. The onset of lithium plating and stripping was quantified, occurring only within the first 15 µm from the separator. The presence of lithium plating changed the behavior of the underlying graphite, such as causing co-existence of LiC6 and graphite in the fully discharged state. Finally, the staging behavior of graphite at different rates was quantified, revealing a high dependency on rate and drastic hysteresis between lithiation and delithiation. |
| first_indexed | 2024-09-23T14:51:51Z |
| format | Article |
| id | mit-1721.1/135404 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T14:51:51Z |
| publishDate | 2021 |
| publisher | Royal Society of Chemistry (RSC) |
| record_format | dspace |
| spelling | mit-1721.1/1354042023-09-19T18:24:52Z Spatial dynamics of lithiation and lithium plating during high-rate operation of graphite electrodes Finegan, Donal P Quinn, Alexander Wragg, David S Colclasure, Andrew M Lu, Xuekun Tan, Chun Heenan, Thomas MM Jervis, Rhodri Brett, Dan JL Das, Supratim Gao, Tao Cogswell, Daniel A Bazant, Martin Z Di Michiel, Marco Checchia, Stefano Shearing, Paul R Smith, Kandler Massachusetts Institute of Technology. Department of Chemical Engineering © 2020 The Royal Society of Chemistry. The principal inhibitor of fast charging lithium ion cells is the graphite negative electrode, where favorable conditions for lithium plating occur at high charge rates, causing accelerated degradation and safety concerns. The local response of graphite, both at the electrode and particle level, when exposed to fast charging conditions of around 6C is not well understood. Consequently, the conditions that lead to the onset of lithium plating, as well as the local dynamics of lithium plating and stripping, have also remained elusive. Here, we use high-speed (100 Hz) pencil-beam X-ray diffraction to repeatedly raster along the depth of a 101 µm thick graphite electrode in 3 µm steps during fast (up to 6C) charge and discharge conditions. Consecutive depth profiles from separator to current collector were each captured in 0.5 seconds, giving an unprecedented spatial and temporal description of the state of the electrode and graphite's staging dynamics during high rate conditions. The electrode is preferentially activated near the separator, and the non-uniformity increases with rate and is influenced by free-energy barriers between graphite's lithiation stages. The onset of lithium plating and stripping was quantified, occurring only within the first 15 µm from the separator. The presence of lithium plating changed the behavior of the underlying graphite, such as causing co-existence of LiC6 and graphite in the fully discharged state. Finally, the staging behavior of graphite at different rates was quantified, revealing a high dependency on rate and drastic hysteresis between lithiation and delithiation. 2021-10-27T20:23:19Z 2021-10-27T20:23:19Z 2020 2021-06-08T14:35:53Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/135404 en 10.1039/D0EE01191F Energy and Environmental Science Creative Commons Attribution 4.0 International license https://creativecommons.org/licenses/by/4.0/ application/pdf Royal Society of Chemistry (RSC) Royal Society of Chemistry (RSC) |
| spellingShingle | Finegan, Donal P Quinn, Alexander Wragg, David S Colclasure, Andrew M Lu, Xuekun Tan, Chun Heenan, Thomas MM Jervis, Rhodri Brett, Dan JL Das, Supratim Gao, Tao Cogswell, Daniel A Bazant, Martin Z Di Michiel, Marco Checchia, Stefano Shearing, Paul R Smith, Kandler Spatial dynamics of lithiation and lithium plating during high-rate operation of graphite electrodes |
| title | Spatial dynamics of lithiation and lithium plating during high-rate operation of graphite electrodes |
| title_full | Spatial dynamics of lithiation and lithium plating during high-rate operation of graphite electrodes |
| title_fullStr | Spatial dynamics of lithiation and lithium plating during high-rate operation of graphite electrodes |
| title_full_unstemmed | Spatial dynamics of lithiation and lithium plating during high-rate operation of graphite electrodes |
| title_short | Spatial dynamics of lithiation and lithium plating during high-rate operation of graphite electrodes |
| title_sort | spatial dynamics of lithiation and lithium plating during high rate operation of graphite electrodes |
| url | https://hdl.handle.net/1721.1/135404 |
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