Li Intercalation into Graphite: Direct Optical Imaging and Cahn–Hilliard Reaction Dynamics
Lithium intercalation into graphite is a critical process in energy storage technology. Studies of Li intercalation kinetics have proved challenging due to structural and phase complexity, and sample heterogeneity. Here we report direct time- and space-resolved, all-optical measurement of Li interca...
| Main Authors: | , , , , , , , |
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| Format: | Article |
| Language: | en_US |
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American Chemical Society (ACS)
2017
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| Online Access: | http://hdl.handle.net/1721.1/110917 https://orcid.org/0000-0003-2421-6781 |
| _version_ | 1826215141064048640 |
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| author | Guo, Yinsheng Yu, Zhonghua Efetov, Dmitri K. Wang, Junpu Kim, Philip Brus, Louis E. 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 Guo, Yinsheng Yu, Zhonghua Efetov, Dmitri K. Wang, Junpu Kim, Philip Brus, Louis E. Smith, Raymond Barrett Bazant, Martin Z |
| author_sort | Guo, Yinsheng |
| collection | MIT |
| description | Lithium intercalation into graphite is a critical process in energy storage technology. Studies of Li intercalation kinetics have proved challenging due to structural and phase complexity, and sample heterogeneity. Here we report direct time- and space-resolved, all-optical measurement of Li intercalation. We use a single crystal graphite electrode with lithographically defined disc geometry. All-optical, Raman and reflectance measurements distinguish the intrinsic intercalation process from side reactions, and provide new insight into the microscopic intercalation process. The recently proposed Cahn–Hilliard reaction (CHR) theory quantitatively captures the observed phase front spatial patterns and dynamics, using a two-layer free-energy model with novel, generalized Butler–Volmer kinetics. This approach unites Cahn–Hilliard and electrochemical kinetics, using a thermodynamically consistent description of the Li injection reaction at the crystal edge that involves a cooperative opening of graphene planes. The excellent agreement between experiment and theory presented here, with single-crystal resolution, provides strong support for the CHR theory of solid-state reactions. |
| first_indexed | 2024-09-23T16:17:13Z |
| format | Article |
| id | mit-1721.1/110917 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T16:17:13Z |
| publishDate | 2017 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1109172022-10-02T07:35:57Z Li Intercalation into Graphite: Direct Optical Imaging and Cahn–Hilliard Reaction Dynamics Guo, Yinsheng Yu, Zhonghua Efetov, Dmitri K. Wang, Junpu Kim, Philip Brus, Louis E. Smith, Raymond Barrett Bazant, Martin Z Massachusetts Institute of Technology. Department of Chemical Engineering Massachusetts Institute of Technology. Department of Mathematics Bazant, Martin Z. Smith, Raymond Barrett Bazant, Martin Z Lithium intercalation into graphite is a critical process in energy storage technology. Studies of Li intercalation kinetics have proved challenging due to structural and phase complexity, and sample heterogeneity. Here we report direct time- and space-resolved, all-optical measurement of Li intercalation. We use a single crystal graphite electrode with lithographically defined disc geometry. All-optical, Raman and reflectance measurements distinguish the intrinsic intercalation process from side reactions, and provide new insight into the microscopic intercalation process. The recently proposed Cahn–Hilliard reaction (CHR) theory quantitatively captures the observed phase front spatial patterns and dynamics, using a two-layer free-energy model with novel, generalized Butler–Volmer kinetics. This approach unites Cahn–Hilliard and electrochemical kinetics, using a thermodynamically consistent description of the Li injection reaction at the crystal edge that involves a cooperative opening of graphene planes. The excellent agreement between experiment and theory presented here, with single-crystal resolution, provides strong support for the CHR theory of solid-state reactions. United States. Dept. of Energy. Office of Basic Energy Sciences (DE-SC0001085) 2017-08-03T14:19:07Z 2017-08-03T14:19:07Z 2016-05 2016-03 Article http://purl.org/eprint/type/JournalArticle 1948-7185 http://hdl.handle.net/1721.1/110917 Guo, Yinsheng; Smith, Raymond B.; Yu, Zhonghua et al. “Li Intercalation into Graphite: Direct Optical Imaging and Cahn–Hilliard Reaction Dynamics.” The Journal of Physical Chemistry Letters 7, 11 (June 2016): 2151–2156 © 2016 American Chemical Society https://orcid.org/0000-0003-2421-6781 en_US http://dx.doi.org/10.1021/acs.jpclett.6b00625 The Journal of Physical Chemistry Letters 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 American Chemical Society (ACS) Prof. Bazant via Erja Kajosalo |
| spellingShingle | Guo, Yinsheng Yu, Zhonghua Efetov, Dmitri K. Wang, Junpu Kim, Philip Brus, Louis E. Smith, Raymond Barrett Bazant, Martin Z Li Intercalation into Graphite: Direct Optical Imaging and Cahn–Hilliard Reaction Dynamics |
| title | Li Intercalation into Graphite: Direct Optical Imaging and Cahn–Hilliard Reaction Dynamics |
| title_full | Li Intercalation into Graphite: Direct Optical Imaging and Cahn–Hilliard Reaction Dynamics |
| title_fullStr | Li Intercalation into Graphite: Direct Optical Imaging and Cahn–Hilliard Reaction Dynamics |
| title_full_unstemmed | Li Intercalation into Graphite: Direct Optical Imaging and Cahn–Hilliard Reaction Dynamics |
| title_short | Li Intercalation into Graphite: Direct Optical Imaging and Cahn–Hilliard Reaction Dynamics |
| title_sort | li intercalation into graphite direct optical imaging and cahn hilliard reaction dynamics |
| url | http://hdl.handle.net/1721.1/110917 https://orcid.org/0000-0003-2421-6781 |
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