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In Situ Raman Mapping of Si Island Electrodes and Stress Modeling as a Function of Lithiation and Size

  • Haotian Wang
    Haotian Wang
    Department of Materials Science and Engineering & Institute for Research in Electronics and Applied Physics, University of Maryland, College Park, Maryland 20740, United States
    More by Haotian Wang
  • Yueming Song
    Yueming Song
    Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, Maryland 20740, United States
    More by Yueming Song
  • Victoria Castagna Ferrari
    Victoria Castagna Ferrari
    Department of Materials Science and Engineering & Institute for Research in Electronics and Applied Physics, University of Maryland, College Park, Maryland 20740, United States
  • Nam Soo Kim
    Nam Soo Kim
    Department of Chemistry and Biochemistry, University of Maryland, College Park, Maryland 20740, United States
    More by Nam Soo Kim
  • Sang Bok Lee
    Sang Bok Lee
    Department of Chemistry and Biochemistry, University of Maryland, College Park, Maryland 20740, United States
    More by Sang Bok Lee
  • Paul Albertus
    Paul Albertus
    Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, Maryland 20740, United States
  • Gary Rubloff
    Gary Rubloff
    Department of Materials Science and Engineering & Institute for Research in Electronics and Applied Physics, University of Maryland, College Park, Maryland 20740, United States
    More by Gary Rubloff
  • , and 
  • David Murdock Stewart*
    David Murdock Stewart
    Department of Materials Science and Engineering & Institute for Research in Electronics and Applied Physics, University of Maryland, College Park, Maryland 20740, United States
    *Email: [email protected]
Cite this: ACS Appl. Mater. Interfaces 2023, 15, 34, 40409–40418
Publication Date (Web):August 16, 2023
https://doi.org/10.1021/acsami.3c06287
Copyright © 2023 American Chemical Society

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    Abstract

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    Si is known for cracking and delamination during electrochemical cycling of a battery due to the large volume change associated with Li insertion and extraction. However, it has been found experimentally that patterned Si island electrodes that are 200 nm thick and less than 7 μm wide can deform in a purely elastic manner. Inspired by this, we performed in situ Raman stress characterization of model poly-crystalline Si island electrodes using an electrochemical cell coupled with an immersion objective lens and designed for a short working distance. A 5 μm wide Si island electrode showed a parabolic stress profile during lithiation, while for a 15 μm Si island electrode, a stress plateau in the center of the electrode was observed. A continuum model with coupled electro-chemo-mechanical (ECM) physics was established to understand the stress measurement. A qualitative agreement was reached between modeling and experimental data, and the critical size effect could be explained by the Li diffusive flux as governed by competition between the Li concentration and hydrostatic stress gradients. Below the critical size, the stress gradient drives Li toward the edges, where the electrode volume is free to expand, while above the critical size, the stress plateau inhibits Li diffusion to the edge and forces destructive stress relief by cracking. This work represents a promising methodology for in situ characterization of ECM coupling in battery electrodes, with suggestions provided for further improvement.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.3c06287.

    • EDS elemental mapping of WO3 formation; development of finite element modeling using in this work and relevant material properties used; and derivation of the relationship between Raman shift and stress for these samples (PDF)

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