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Issue 4, 2018
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Effect of composition on the structure of lithium- and manganese-rich transition metal oxides

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Abstract

The choice of chemical composition of lithium- and manganese-rich transition metal oxides used as cathode materials in lithium-ion batteries can significantly impact their long-term viability as storage solutions for clean energy automotive applications. Their structure has been widely debated: conflicting conclusions drawn from individual studies often considering different compositions have made it challenging to reach a consensus and inform future research. Here, complementary electron microscopy techniques over a wide range of length scales reveal the effect of lithium-to-transition metal-ratio on the surface and bulk structure of these materials. We found that decreasing the lithium-to-transition metal-ratio resulted in a significant change in terms of order and atomic-level local composition in the bulk of these cathode materials. However, throughout the composition range studied, the materials consisted solely of a monoclinic phase, with lower lithium content materials showing more chemical ordering defects. In contrast, the spinel-structured surface present on specific crystallographic facets exhibited no noticeable structural change when varying the ratio of lithium to transition metal. The structural observations from this study warrant a reexamination of commonly assumed models linking poor electrochemical performance with bulk and surface structure.

Graphical abstract: Effect of composition on the structure of lithium- and manganese-rich transition metal oxides

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Publication details

The article was received on 25 Aug 2017, accepted on 10 Jan 2018 and first published on 10 Jan 2018


Article type: Paper
DOI: 10.1039/C7EE02443F
Citation: Energy Environ. Sci., 2018,11, 830-840
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    Effect of composition on the structure of lithium- and manganese-rich transition metal oxides

    A. K. Shukla, Q. M. Ramasse, C. Ophus, D. M. Kepaptsoglou, F. S. Hage, C. Gammer, C. Bowling, P. A. H. Gallegos and S. Venkatachalam, Energy Environ. Sci., 2018, 11, 830
    DOI: 10.1039/C7EE02443F

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