Li Intercalation into Graphite: Direct Optical Imaging and Cahn–Hilliard Reaction Dynamics
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Li Intercalation into Graphite with SI.pdf
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Author(s)
Guo, Yinsheng
Yu, Zhonghua
Efetov, Dmitri K.
Wang, Junpu
Kim, Philip
Brus, Louis E.
Smith, Raymond Barrett
Bazant, Martin Z
Date Issued
May 2016
Journal
The Journal of Physical Chemistry Letters
Publisher
American Chemical Society (ACS)
Citation
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
Version
Author's final manuscript
Abstract
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.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Mathematics
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DOI of Published Version
https://doi.org/10.1021/acs.jpclett.6b00625
