The intrinsic behavior of lithium fluoride in solid electrolyte interphases on lithium
© 2020 National Academy of Sciences. All rights reserved. Lithium is the most attractive anode material for high-energy density rechargeable batteries, but its cycling is plagued by morphological irreversibility and dendrite growth that arise in part from its heterogeneous “native” solid electrolyte...
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| Format: | Article |
| Language: | English |
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Proceedings of the National Academy of Sciences
2021
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| Online Access: | https://hdl.handle.net/1721.1/136636 |
| _version_ | 1826194364616933376 |
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| author | He, Mingfu Guo, Rui Hobold, Gustavo M Gao, Haining Gallant, Betar M |
| author2 | Massachusetts Institute of Technology. Department of Mechanical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Mechanical Engineering He, Mingfu Guo, Rui Hobold, Gustavo M Gao, Haining Gallant, Betar M |
| author_sort | He, Mingfu |
| collection | MIT |
| description | © 2020 National Academy of Sciences. All rights reserved. Lithium is the most attractive anode material for high-energy density rechargeable batteries, but its cycling is plagued by morphological irreversibility and dendrite growth that arise in part from its heterogeneous “native” solid electrolyte interphase (SEI). Enriching the SEI with lithium fluoride (LiF) has recently gained popularity to improve Li cyclability. However, the intrinsic function of LiF—whether chemical, mechanical, or kinetic in nature—remains unknown. Herein, we investigated the stability of LiF in model LiF-enriched SEIs that are either artificially preformed or derived from fluorinated electrolytes, and thus, the effect of the LiF source on Li electrode behavior. We discovered that the mechanical integrity of LiF is easily compromised during plating, making it intrinsically unable to protect Li. The ensuing in situ repair of the interface by electrolyte, either regenerating LiF or forming an extra elastomeric “outer layer,” is identified as the more critical determinant of Li electrode performance. Our findings present an updated and dynamic picture of the LiF-enriched SEI and demonstrate the need to carefully consider the combined role of ionic and electrolyte-derived layers in future design strategies. |
| first_indexed | 2024-09-23T09:54:32Z |
| format | Article |
| id | mit-1721.1/136636 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T09:54:32Z |
| publishDate | 2021 |
| publisher | Proceedings of the National Academy of Sciences |
| record_format | dspace |
| spelling | mit-1721.1/1366362023-02-28T20:43:12Z The intrinsic behavior of lithium fluoride in solid electrolyte interphases on lithium He, Mingfu Guo, Rui Hobold, Gustavo M Gao, Haining Gallant, Betar M Massachusetts Institute of Technology. Department of Mechanical Engineering Massachusetts Institute of Technology. Department of Materials Science and Engineering © 2020 National Academy of Sciences. All rights reserved. Lithium is the most attractive anode material for high-energy density rechargeable batteries, but its cycling is plagued by morphological irreversibility and dendrite growth that arise in part from its heterogeneous “native” solid electrolyte interphase (SEI). Enriching the SEI with lithium fluoride (LiF) has recently gained popularity to improve Li cyclability. However, the intrinsic function of LiF—whether chemical, mechanical, or kinetic in nature—remains unknown. Herein, we investigated the stability of LiF in model LiF-enriched SEIs that are either artificially preformed or derived from fluorinated electrolytes, and thus, the effect of the LiF source on Li electrode behavior. We discovered that the mechanical integrity of LiF is easily compromised during plating, making it intrinsically unable to protect Li. The ensuing in situ repair of the interface by electrolyte, either regenerating LiF or forming an extra elastomeric “outer layer,” is identified as the more critical determinant of Li electrode performance. Our findings present an updated and dynamic picture of the LiF-enriched SEI and demonstrate the need to carefully consider the combined role of ionic and electrolyte-derived layers in future design strategies. 2021-10-27T20:36:23Z 2021-10-27T20:36:23Z 2020 2020-07-09T16:49:45Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/136636 en 10.1073/PNAS.1911017116 Proceedings of the National Academy of Sciences of the United States of America 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 Proceedings of the National Academy of Sciences PNAS |
| spellingShingle | He, Mingfu Guo, Rui Hobold, Gustavo M Gao, Haining Gallant, Betar M The intrinsic behavior of lithium fluoride in solid electrolyte interphases on lithium |
| title | The intrinsic behavior of lithium fluoride in solid electrolyte interphases on lithium |
| title_full | The intrinsic behavior of lithium fluoride in solid electrolyte interphases on lithium |
| title_fullStr | The intrinsic behavior of lithium fluoride in solid electrolyte interphases on lithium |
| title_full_unstemmed | The intrinsic behavior of lithium fluoride in solid electrolyte interphases on lithium |
| title_short | The intrinsic behavior of lithium fluoride in solid electrolyte interphases on lithium |
| title_sort | intrinsic behavior of lithium fluoride in solid electrolyte interphases on lithium |
| url | https://hdl.handle.net/1721.1/136636 |
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