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Visualizing nanoscale 3D compositional fluctuation of lithium in advanced lithium-ion battery cathodes

Author

Listed:
  • A. Devaraj

    (Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory)

  • M. Gu

    (Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory)

  • R. Colby

    (Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory
    Present address: ExxonMobil Research and Engineering Company, Annandale, New Jersey 08801, USA)

  • P. Yan

    (Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory)

  • C. M. Wang

    (Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory)

  • J. M. Zheng

    (Energy and Environmental Directorate, Pacific Northwest National Laboratory)

  • J. Xiao

    (Energy and Environmental Directorate, Pacific Northwest National Laboratory)

  • A. Genc

    (FEI Company)

  • J. G. Zhang

    (Energy and Environmental Directorate, Pacific Northwest National Laboratory)

  • I. Belharouak

    (Qatar Environment and Energy Research Institute, Qatar Foundation)

  • D. Wang

    (Argonne National Laboratory)

  • K. Amine

    (Argonne National Laboratory)

  • S. Thevuthasan

    (Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory
    Qatar Environment and Energy Research Institute, Qatar Foundation)

Abstract

The distribution of cations in Li-ion battery cathodes as a function of cycling is a pivotal characteristic of battery performance. The transition metal cation distribution has been shown to affect cathode performance; however, Li is notoriously challenging to characterize with typical imaging techniques. Here laser-assisted atom probe tomography (APT) is used to map the three-dimensional distribution of Li at a sub-nanometre spatial resolution and correlate it with the distribution of the transition metal cations (M) and the oxygen. As-fabricated layered Li1.2Ni0.2Mn0.6O2 is shown to have Li-rich Li2MO3 phase regions and Li-depleted Li(Ni0.5Mn0.5)O2 regions. Cycled material has an overall loss of Li in addition to Ni-, Mn- and Li-rich regions. Spinel LiNi0.5Mn1.5O4 is shown to have a uniform distribution of all cations. APT results were compared to energy dispersive spectroscopy mapping with a scanning transmission electron microscope to confirm the transition metal cation distribution.

Suggested Citation

  • A. Devaraj & M. Gu & R. Colby & P. Yan & C. M. Wang & J. M. Zheng & J. Xiao & A. Genc & J. G. Zhang & I. Belharouak & D. Wang & K. Amine & S. Thevuthasan, 2015. "Visualizing nanoscale 3D compositional fluctuation of lithium in advanced lithium-ion battery cathodes," Nature Communications, Nature, vol. 6(1), pages 1-8, November.
    • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms9014
    DOI: 10.1038/ncomms9014
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