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Nanoscale Compositional Mapping of Commercial LiNi0.8Co0.15Al0.05O2 Cathodes Using Atom Probe Tomography

  • Pritesh Parikh
    Pritesh Parikh
    Department of NanoEngineering, University of California San Diego, 9500 Gilman Drive, La Jolla, California 92093, United States
  • Hyeseung Chung
    Hyeseung Chung
    Department of NanoEngineering, University of California San Diego, 9500 Gilman Drive, La Jolla, California 92093, United States
  • Ethan Vo
    Ethan Vo
    Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, Washington 99354, United States
    More by Ethan Vo
  • Abhik Banerjee
    Abhik Banerjee
    Department of NanoEngineering, University of California San Diego, 9500 Gilman Drive, La Jolla, California 92093, United States
    Research Institute for Sustainable Energy (RISE), TCG Centres for Research and Education in Science and Technology (TCG CREST), Salt Lake, Kolkata 700091, India
  • Ying Shirley Meng*
    Ying Shirley Meng
    Pritzker School of Molecular Engineering, University of Chicago, 5640 South Ellis Avenue, Chicago, Illinois 60637, United States
    Department of NanoEngineering, University of California San Diego, 9500 Gilman Drive, La Jolla, California 92093, United States
    *Email: [email protected]
  • , and 
  • Arun Devaraj*
    Arun Devaraj
    Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, Washington 99354, United States
    *Email: [email protected]
    More by Arun Devaraj
Cite this: J. Phys. Chem. C 2022, 126, 34, 14380–14388
Publication Date (Web):July 22, 2022
https://doi.org/10.1021/acs.jpcc.2c01217
Copyright © 2022 American Chemical Society

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    Abstract

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    Nickel-rich cathodes provide improved specific capacity, which leads to higher gravimetric energy density, which, in turn, is critical for electric vehicles. However, poor long-term capacity retention at elevated temperatures/high C rates (the rate of charge and discharge on a battery) stems from material issues: surface phase changes, corrosive side reactions with the electrolyte, ion dissolution, and propagation of cracks. Introducing dopants, developing nanoscale surface coatings, and graded core–shell structures all improved the electrochemical performance of nickel-rich cathodes. However, material-level understanding of the effect of Li composition and distribution in Ni-rich cathodes is limited due to a lack of characterization methods available that can directly image Li at the nanoscale. Hence, it is critical to establish methods such as atom probe tomography (APT) that have both nanometer-scale spatial resolution and high compositional sensitivity to quantitatively analyze battery cathodes. To fully realize its potential as a method for quantitative compositional analysis of commercial Li-ion batteries, we provide a comprehensive description of the challenges in sample preparation and analyze the dependency of the analysis parameters, specifically laser pulse energy on the measured stoichiometry of elements in a high-Ni-content cathode material LiNi0.8Co0.15Al0.05O2 (NCA). Our findings show that the stoichiometry variations cannot be explained by charge–state ratios or Ga implantation damage alone during FIB preparation, indicating that additional factors such as crystallographic orientation may need to be considered to achieve quantitative nanoscale compositional analysis of such battery cathodes using APT.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpcc.2c01217.

    • Table S1 contains numbers used to plot Figure 1, Table S2 contains composition numbers used for Figure 5, Figure S1 compares the effect of Ga on the composition analysis in the low-gradient and high-gradient regions, Figure S2 shows the Ga maps for each laser pulse energy, and Figure S3 shows the statistical analysis for Li uniformity (PDF)

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    Cited By

    This article is cited by 1 publications.

    1. Tong Li, Arun Devaraj, Norbert Kruse. Atomic-scale characterization of (electro-)catalysts and battery materials by atom probe tomography. Cell Reports Physical Science 2022, 3 (12) , 101188. https://doi.org/10.1016/j.xcrp.2022.101188

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