In situ atomic-scale imaging of electrochemical lithiation in silicon

Xiao Hua Liu, Jiang Wei Wang, Shan Huang, Feifei Fan, Xu Huang, Yang Liu, Sergiy Krylyuk, Jinkyoung Yoo, Shadi A. Dayeh, Albert V. Davydov, Scott X. Mao, S. Tom Picraux, Sulin Zhang, Ju Li, Ting Zhu, Jian Yu Huang

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Abstract

In lithium-ion batteries, the electrochemical reaction between the electrodes and lithium is a critical process that controls the capacity, cyclability and reliability of the battery. Despite intensive study, the atomistic mechanism of the electrochemical reactions occurring in these solid-state electrodes remains unclear. Here, we show that in situ transmission electron microscopy can be used to study the dynamic lithiation process of single-crystal silicon with atomic resolution. We observe a sharp interface (∼1 μnm thick) between the crystalline silicon and an amorphous Li x Si alloy. The lithiation kinetics are controlled by the migration of the interface, which occurs through a ledge mechanism involving the lateral movement of ledges on the close-packed {111} atomic planes. Such ledge flow processes produce the amorphous Li x Si alloy through layer-by-layer peeling of the {111} atomic facets, resulting in the orientation-dependent mobility of the interfaces.

Original languageEnglish (US)
Pages (from-to)749-756
Number of pages8
JournalNature nanotechnology
Volume7
Issue number11
DOIs
StatePublished - Nov 2012

All Science Journal Classification (ASJC) codes

  • Bioengineering
  • Atomic and Molecular Physics, and Optics
  • Biomedical Engineering
  • Materials Science(all)
  • Condensed Matter Physics
  • Electrical and Electronic Engineering

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  • Cite this

    Liu, X. H., Wang, J. W., Huang, S., Fan, F., Huang, X., Liu, Y., Krylyuk, S., Yoo, J., Dayeh, S. A., Davydov, A. V., Mao, S. X., Picraux, S. T., Zhang, S., Li, J., Zhu, T., & Huang, J. Y. (2012). In situ atomic-scale imaging of electrochemical lithiation in silicon. Nature nanotechnology, 7(11), 749-756. https://doi.org/10.1038/nnano.2012.170