Spatial Quantification of Dynamic Inter and Intra Particle Crystallographic Heterogeneities within Lithium Ion Electrodes

Donal Finegan, Kandler Smith, Natalie Seitzman, Antonis Vamvakeros, Chun Tan, Thomas Heenan, Sohrab Daemi, Marco Michiel, Simon Jacques, Andrew Beale, Dan Brett, Paul Shearing

Research output: Contribution to journalArticlepeer-review

65 Scopus Citations


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 LixMn2O4 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 LiMnO2 within the first cycle. Other particles contain monoclinic Li2MnO3 near the surface and almost pure spinel LixMn2O4 near the core. Following 150 cycles, concentrations of LiMnO2 and Li2MnO3 significantly increase and widely vary between particles.

Original languageAmerican English
Article numberArticle No. 631
Number of pages11
JournalNature Communications
Issue number1
StatePublished - 1 Dec 2020

Bibliographical note

Publisher Copyright:
© 2020, This is a U.S. government work and not under copyright protection in the U.S.; foreign copyright protection may apply.

NREL Publication Number

  • NREL/JA-5400-75809


  • computed tomography
  • crystallography
  • lithium ion batteries
  • x-ray diffraction


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