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Spatial quantification of dynamic inter and intra particle crystallographic heterogeneities within lithium ion electrodes

Finegan, DP; Vamvakeros, A; Tan, C; Heenan, TMM; Daemi, SR; Seitzman, N; Di Michiel, M; ... Smith, K; + view all (2020) Spatial quantification of dynamic inter and intra particle crystallographic heterogeneities within lithium ion electrodes. Nature Communications , 11 (1) , Article 631. 10.1038/s41467-020-14467-x. Green open access

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Abstract

The performance of lithium ion electrodes is hindered by unfavorable chemical heterogeneities that pre-exist or develop during operation. Time-resolved spatial descriptions are needed to understand the link between such heterogeneities and a cell’s performance. Here, operando high-resolution X-ray diffraction-computed tomography is used to spatially and temporally quantify crystallographic heterogeneities within and between particles throughout both fresh and degraded Li_{x}Mn_{2)O_{4} electrodes. This imaging technique facilitates identification of stoichiometric differences between particles and stoichiometric gradients and phase heterogeneities within particles. Through radial quantification of phase fractions, the response of distinct particles to lithiation is found to vary; most particles contain localized regions that transition to rock salt LiMnO_{2} within the first cycle. Other particles contain monoclinic Li_{2}MnO_{3}near the surface and almost pure spinel Li_{x}Mn_{2}O_{4} near the core. Following 150 cycles, concentrations of LiMnO_{2} and Li_{2}MnO_{3} significantly increase and widely vary between particles.

Type: Article
Title: Spatial quantification of dynamic inter and intra particle crystallographic heterogeneities within lithium ion electrodes
Location: England
Open access status: An open access version is available from UCL Discovery
DOI: 10.1038/s41467-020-14467-x
Publisher version: https://doi.org/10.1038/s41467-020-14467-x
Language: English
Additional information: © The Authors. This article is licensed under a Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/).
Keywords: Batteries, Chemical engineering
UCL classification: UCL
UCL > Provost and Vice Provost Offices
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10092782
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