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Issue 2, 2019
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Quantifying lithium concentration gradients in the graphite electrode of Li-ion cells using operando energy dispersive X-ray diffraction

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Abstract

Safe, fast, and energy efficient cycling of lithium ion batteries is desired in many practical applications. However, modeling studies predict steep Li+ ion gradients in the electrodes during cycling at the higher currents. Such gradients introduce heterogeneities in the electrodes, which make it difficult to predict cell lifetimes as different portions of the cell age at different rates. There is a dearth of experimental methods to probe these concentration gradients across the depth of the electrode. Here we use spatially resolved energy dispersive X-ray diffraction to obtain a “movie” of lithiation and delithiation in different sections of the cell and quantify lithium gradients that develop in a porous graphite electrode during cycling at a 1C rate. Inhomogeneity in the total Li content, and in the individual ordered LixC6 phases formed during lithium insertion into (and extraction from) the graphite, has been observed in an operando fashion. The complex dynamics of lithium-staging in graphite with the distinct front propagation of phase changes have been characterized and new features of these dynamics are highlighted here. As large Li+ ion gradients contribute to cell polarization, our results suggest that Li plating conditions can be met near the graphite electrode surface, even when the cell is charged at a moderate (1C) rate.

Graphical abstract: Quantifying lithium concentration gradients in the graphite electrode of Li-ion cells using operando energy dispersive X-ray diffraction

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Publication details

The article was received on 14 Aug 2018, accepted on 15 Nov 2018 and first published on 09 Jan 2019


Article type: Paper
DOI: 10.1039/C8EE02373E
Energy Environ. Sci., 2019,12, 656-665
  • Open access: Creative Commons BY license
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    Quantifying lithium concentration gradients in the graphite electrode of Li-ion cells using operando energy dispersive X-ray diffraction

    K. P. C. Yao, J. S. Okasinski, K. Kalaga, I. A. Shkrob and D. P. Abraham, Energy Environ. Sci., 2019, 12, 656
    DOI: 10.1039/C8EE02373E

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