Current-induced transition from particle-by-particle to concurrent intercalation in phase-separating battery electrodes
Many battery electrodes contain ensembles of nanoparticles that phase-separate on (de)intercalation. In such electrodes, the fraction of actively intercalating particles directly impacts cycle life: a vanishing population concentrates the current in a small number of particles, leading to current ho...
| Main Authors: | , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Article |
| Language: | en_US |
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Nature Publishing Group
2017
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| Online Access: | http://hdl.handle.net/1721.1/110915 https://orcid.org/0000-0003-2421-6781 |
| _version_ | 1811085977601441792 |
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| author | Li, Yiyang El Gabaly, Farid Bartelt, Norman C. Sugar, Joshua D. Fenton, Kyle R. Cogswell, Daniel A. Kilcoyne, A. L. David Tyliszczak, Tolek Chueh, William C. Ferguson, Todd Richard Smith, Raymond Barrett Bazant, Martin Z |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Li, Yiyang El Gabaly, Farid Bartelt, Norman C. Sugar, Joshua D. Fenton, Kyle R. Cogswell, Daniel A. Kilcoyne, A. L. David Tyliszczak, Tolek Chueh, William C. Ferguson, Todd Richard Smith, Raymond Barrett Bazant, Martin Z |
| author_sort | Li, Yiyang |
| collection | MIT |
| description | Many battery electrodes contain ensembles of nanoparticles that phase-separate on (de)intercalation. In such electrodes, the fraction of actively intercalating particles directly impacts cycle life: a vanishing population concentrates the current in a small number of particles, leading to current hotspots. Reports of the active particle population in the phase-separating electrode lithium iron phosphate (LiFePO4; LFP) vary widely, ranging from near 0% (particle-by-particle) to 100% (concurrent intercalation). Using synchrotron-based X-ray microscopy, we probed the individual state-of-charge for over 3,000 LFP particles. We observed that the active population depends strongly on the cycling current, exhibiting particle-by-particle-like behaviour at low rates and increasingly concurrent behaviour at high rates, consistent with our phase-field porous electrode simulations. Contrary to intuition, the current density, or current per active internal surface area, is nearly invariant with the global electrode cycling rate. Rather, the electrode accommodates higher current by increasing the active particle population. This behaviour results from thermodynamic transformation barriers in LFP, and such a phenomenon probably extends to other phase-separating battery materials. We propose that modifying the transformation barrier and exchange current density can increase the active population and thus the current homogeneity. This could introduce new paradigms to enhance the cycle life of phase-separating battery electrodes. |
| first_indexed | 2024-09-23T13:18:57Z |
| format | Article |
| id | mit-1721.1/110915 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T13:18:57Z |
| publishDate | 2017 |
| publisher | Nature Publishing Group |
| record_format | dspace |
| spelling | mit-1721.1/1109152022-10-01T14:28:20Z Current-induced transition from particle-by-particle to concurrent intercalation in phase-separating battery electrodes Li, Yiyang El Gabaly, Farid Bartelt, Norman C. Sugar, Joshua D. Fenton, Kyle R. Cogswell, Daniel A. Kilcoyne, A. L. David Tyliszczak, Tolek Chueh, William C. Ferguson, Todd Richard Smith, Raymond Barrett Bazant, Martin Z Massachusetts Institute of Technology. Department of Chemical Engineering Massachusetts Institute of Technology. Department of Mathematics Bazant, Martin Z. Ferguson, Todd Richard Smith, Raymond Barrett Bazant, Martin Z Many battery electrodes contain ensembles of nanoparticles that phase-separate on (de)intercalation. In such electrodes, the fraction of actively intercalating particles directly impacts cycle life: a vanishing population concentrates the current in a small number of particles, leading to current hotspots. Reports of the active particle population in the phase-separating electrode lithium iron phosphate (LiFePO4; LFP) vary widely, ranging from near 0% (particle-by-particle) to 100% (concurrent intercalation). Using synchrotron-based X-ray microscopy, we probed the individual state-of-charge for over 3,000 LFP particles. We observed that the active population depends strongly on the cycling current, exhibiting particle-by-particle-like behaviour at low rates and increasingly concurrent behaviour at high rates, consistent with our phase-field porous electrode simulations. Contrary to intuition, the current density, or current per active internal surface area, is nearly invariant with the global electrode cycling rate. Rather, the electrode accommodates higher current by increasing the active particle population. This behaviour results from thermodynamic transformation barriers in LFP, and such a phenomenon probably extends to other phase-separating battery materials. We propose that modifying the transformation barrier and exchange current density can increase the active population and thus the current homogeneity. This could introduce new paradigms to enhance the cycle life of phase-separating battery electrodes. 2017-08-03T13:59:55Z 2017-08-03T13:59:55Z 2014-09 2014-02 Article http://purl.org/eprint/type/JournalArticle 1476-1122 1476-4660 http://hdl.handle.net/1721.1/110915 Li, Yiyang; El Gabaly, Farid; Ferguson, Todd R. et al. “Current-Induced Transition from Particle-by-Particle to Concurrent Intercalation in Phase-Separating Battery Electrodes.” Nature Materials 13, 12 (September 2014): 1149–1156 © 2014 Macmillan Publishers Limited, part of Springer Nature https://orcid.org/0000-0003-2421-6781 en_US http://dx.doi.org/10.1038/nmat4084 Nature Materials Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf Nature Publishing Group Prof. Bazant via Erja Kajosalo |
| spellingShingle | Li, Yiyang El Gabaly, Farid Bartelt, Norman C. Sugar, Joshua D. Fenton, Kyle R. Cogswell, Daniel A. Kilcoyne, A. L. David Tyliszczak, Tolek Chueh, William C. Ferguson, Todd Richard Smith, Raymond Barrett Bazant, Martin Z Current-induced transition from particle-by-particle to concurrent intercalation in phase-separating battery electrodes |
| title | Current-induced transition from particle-by-particle to concurrent intercalation in phase-separating battery electrodes |
| title_full | Current-induced transition from particle-by-particle to concurrent intercalation in phase-separating battery electrodes |
| title_fullStr | Current-induced transition from particle-by-particle to concurrent intercalation in phase-separating battery electrodes |
| title_full_unstemmed | Current-induced transition from particle-by-particle to concurrent intercalation in phase-separating battery electrodes |
| title_short | Current-induced transition from particle-by-particle to concurrent intercalation in phase-separating battery electrodes |
| title_sort | current induced transition from particle by particle to concurrent intercalation in phase separating battery electrodes |
| url | http://hdl.handle.net/1721.1/110915 https://orcid.org/0000-0003-2421-6781 |
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