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

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 and S. Thevuthasan
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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
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

Nature Communications, 2015, vol. 6, issue 1, 1-8

Abstract: 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.

Date: 2015
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DOI: 10.1038/ncomms9014

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