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Identifying the Distribution of Al3+ in LiNi0.8Co0.15Al0.05O2

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Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, U.K.
Materials Department, University of California, Santa Barbara, Santa Barbara, California 93106, United States
§ Department of NanoEngineering, University of California, San Diego, La Jolla, California 92093, United States
X-ray Division, Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States
Institute for Materials Research, SUNY Binghamton, Binghamton, New York 13902-6000, United States
# Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
Cite this: Chem. Mater. 2016, 28, 22, 8170–8180
Publication Date (Web):October 7, 2016
https://doi.org/10.1021/acs.chemmater.6b02797
Copyright © 2016 American Chemical Society

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    Abstract

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    The doping of Al into layered Li transition metal (TM) oxide cathode materials, LiTMO2, is known to improve the structural and thermal stability, although the origin of the enhanced properties is not well understood. The effect of aluminum doping on layer stabilization has been investigated using a combination of techniques to measure the aluminum distribution in layered LiNi0.8Co0.15Al0.05O2 (NCA) over multiple length scales with 27Al and 7Li MAS NMR, local electrode atom probe (APT) tomography, X-ray and neutron diffraction, DFT, and SQUID magnetic susceptibility measurements. APT ion maps show a homogeneous distribution of Ni, Co, Al, and O2 throughout the structure at the single particle level in agreement with the high-temperature phase diagram. 7Li and 27Al NMR indicates that the Ni3+ ions undergo a dynamic Jahn–Teller (JT) distortion. 27Al NMR spectra indicate that the Al reduces the strain associated with the JT distortion, by preferential electronic ordering of the JT lengthened bonds directed toward the Al3+ ion. The ability to understand the complex atomic and orbital ordering around Al3+ demonstrated in the current method will be useful for studying the local environment of Al3+ in a range of transition metal oxide battery materials.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.chemmater.6b02797.

    • Additional details of the NCA phase diagram, structural and NMR shift calculations, atom probe tomography experimental details and additional maps, calculated NMR spectra, 2D 7Li pj-MATPASS spectra, full deconvolution of 27Al NMR spectra, and static 27Al NMR shifts (PDF)

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