Spatially Resolving Lithiation in Silicon-Graphite Composite Electrodes via in Situ High-Energy X-ray Diffraction Computed Tomography

Donal Finegan, Kandler Smith, Antonis Vamvakeros, Chun Tan, Thomas Heenan, Sohrab Daemi, Simon Jacques, Andrew Beale, Marco Michiel, Dan Brett, Paul Shearing, Chunmei Ban, Lei Cao

Research output: Contribution to journalArticlepeer-review

74 Scopus Citations

Abstract

Optimizing the chemical and morphological parameters of lithium-ion (Li-ion) electrodes is extremely challenging, due in part to the absence of techniques to construct spatial and temporal descriptions of chemical and morphological heterogeneities. We present the first demonstration of combined high-speed X-ray diffraction (XRD) and XRD computed tomography (XRD-CT) to probe, in 3D, crystallographic heterogeneities within Li-ion electrodes with a spatial resolution of 1 μm. The local charge-transfer mechanism within and between individual particles was investigated in a silicon(Si)-graphite composite electrode. High-speed XRD revealed charge balancing kinetics between the graphite and Si during the minutes following the transition from operation to open circuit. Subparticle lithiation heterogeneities in both Si and graphite were observed using XRD-CT, where the core and shell structures were segmented, and their respective diffraction patterns were characterized.

Original languageAmerican English
Pages (from-to)3811-3820
Number of pages10
JournalNano Letters
Volume19
Issue number6
DOIs
StatePublished - 12 Jun 2019

Bibliographical note

Publisher Copyright:
© 2019 American Chemical Society.

NREL Publication Number

  • NREL/JA-5400-73945

Keywords

  • Composite electrodes
  • high-speed XRD
  • lithitation heterogeneities
  • Si electrodes
  • X-ray diffraction computed tomography
  • XRD-CT

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