Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 7, Issue 11, Pages 2151-2156Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.6b00625
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Funding
- Center for Re-defining Photovoltaic Efficiency Through Molecular-Scale Control, an Energy Frontier Research Center (EFRC) - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001085]
- DMREF grant from National Science Foundation (NSF) [DMR-1435487]
- Samsung Advanced Institute of Technology
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1435487] Funding Source: National Science Foundation
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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.
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