Unravelling structural ambiguities in lithium- and manganese-rich transition metal oxides

Alpesh Khushalchand Shukla (), Quentin M. Ramasse, Colin Ophus, Hugues Duncan, Fredrik Hage and Guoying Chen
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Alpesh Khushalchand Shukla: Lawrence Berkeley National Laboratory
Quentin M. Ramasse: SuperSTEM Laboratory, SciTech Daresbury Campus
Colin Ophus: National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory
Hugues Duncan: Lawrence Berkeley National Laboratory
Fredrik Hage: SuperSTEM Laboratory, SciTech Daresbury Campus
Guoying Chen: Lawrence Berkeley National Laboratory

Nature Communications, 2015, vol. 6, issue 1, 1-9

Abstract: Abstract Although Li- and Mn-rich transition metal oxides have been extensively studied as high-capacity cathode materials for Li-ion batteries, the crystal structure of these materials in their pristine state is not yet fully understood. Here we apply complementary electron microscopy and spectroscopy techniques at multi-length scale on well-formed Li1.2(Ni0.13Mn0.54Co0.13)O2 crystals with two different morphologies as well as two commercially available materials with similar compositions, and unambiguously describe the structural make-up of these samples. Systematically observing the entire primary particles along multiple zone axes reveals that they are consistently made up of a single phase, save for rare localized defects and a thin surface layer on certain crystallographic facets. More specifically, we show the bulk of the oxides can be described as an aperiodic crystal consisting of randomly stacked domains that correspond to three variants of monoclinic structure, while the surface is composed of a Co- and/or Ni-rich spinel with antisite defects.

Date: 2015
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DOI: 10.1038/ncomms9711

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