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Rationalizing Deactivation Behavior in Pyrochlore-Type CeO2-ZrO2 Oxygen Storage Catalysts Using Multimodal Nano X-Ray Fluorescence Computed Tomography, X-Ray Diffraction Computed Tomography, and Scanning Three-Dimensional X-ray Diffraction

Odarchenko, Yaroslav ; Vamvakeros, Antonis ; Price, Stephen W.T. ; Jones, Wilm ; Nagashima, Shinya ; Nguyen, Hai P. ; Wright, Jonathan ; Henningsson, Axel LU ; Hall, Stephen LU and Jacques, Simon D.M. , et al. (2025) In Chemistry-Methods 5(12).
Abstract

The authors report a combination of multimodal scanning three-dimensional X-ray diffraction (S3DXRD), X-ray diffraction computed tomography (XRD-CT), and X-ray fluorescence computed tomography (XRF-CT) used for the first time to provide multiscale (spanning the size regime 0.15–500 µm) insight into the aging of a CeO2-ZrO2 solid solution known to exhibit outstanding reversible oxygen storage capacity (OSC). The authors show that using nanobeams is necessary to map in detail the distribution of elements and crystalline phases. In particular, the latter information is derived from two imaging methodologies to capture the diffraction signal originating from single crystals and powder-averaged crystallites,... (More)

The authors report a combination of multimodal scanning three-dimensional X-ray diffraction (S3DXRD), X-ray diffraction computed tomography (XRD-CT), and X-ray fluorescence computed tomography (XRF-CT) used for the first time to provide multiscale (spanning the size regime 0.15–500 µm) insight into the aging of a CeO2-ZrO2 solid solution known to exhibit outstanding reversible oxygen storage capacity (OSC). The authors show that using nanobeams is necessary to map in detail the distribution of elements and crystalline phases. In particular, the latter information is derived from two imaging methodologies to capture the diffraction signal originating from single crystals and powder-averaged crystallites, respectively. Ultimately, a decrease in relative OSC by 25% in the aged material could be correlated with a transformation of the cation-ordered pyrochlore Ce2Zr2O7 phase to the cation-disordered CeO2-ZrO2 fluorite structure. This is manifested as a loss in homogeneity of Ce and Zr distribution of the cation-ordered pyrochlore seen by nanoXRF-CT. The diffraction signal in both the S3DXRD and XRD-CT provides evidence that the solid-state transformation between the phases preferentially takes place at the periphery of the catalyst particle, resulting in a pyrochlore-rich core and fluorite on the surface and accompanied by significant sintering.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
chemical imaging, diffraction, multimodal, oxygen storage capacity
in
Chemistry-Methods
volume
5
issue
12
article number
e202500074
publisher
Wiley-VCH Verlag
external identifiers
  • scopus:105017020103
DOI
10.1002/cmtd.202500074
language
English
LU publication?
yes
id
17ed832a-c3d8-416d-8e89-cd6b7957a5ec
date added to LUP
2025-12-09 08:27:52
date last changed
2025-12-09 08:28:26
@article{17ed832a-c3d8-416d-8e89-cd6b7957a5ec,
  abstract     = {{<p>The authors report a combination of multimodal scanning three-dimensional X-ray diffraction (S3DXRD), X-ray diffraction computed tomography (XRD-CT), and X-ray fluorescence computed tomography (XRF-CT) used for the first time to provide multiscale (spanning the size regime 0.15–500 µm) insight into the aging of a CeO<sub>2</sub>-ZrO<sub>2</sub> solid solution known to exhibit outstanding reversible oxygen storage capacity (OSC). The authors show that using nanobeams is necessary to map in detail the distribution of elements and crystalline phases. In particular, the latter information is derived from two imaging methodologies to capture the diffraction signal originating from single crystals and powder-averaged crystallites, respectively. Ultimately, a decrease in relative OSC by 25% in the aged material could be correlated with a transformation of the cation-ordered pyrochlore Ce<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> phase to the cation-disordered CeO<sub>2</sub>-ZrO<sub>2</sub> fluorite structure. This is manifested as a loss in homogeneity of Ce and Zr distribution of the cation-ordered pyrochlore seen by nanoXRF-CT. The diffraction signal in both the S3DXRD and XRD-CT provides evidence that the solid-state transformation between the phases preferentially takes place at the periphery of the catalyst particle, resulting in a pyrochlore-rich core and fluorite on the surface and accompanied by significant sintering.</p>}},
  author       = {{Odarchenko, Yaroslav and Vamvakeros, Antonis and Price, Stephen W.T. and Jones, Wilm and Nagashima, Shinya and Nguyen, Hai P. and Wright, Jonathan and Henningsson, Axel and Hall, Stephen and Jacques, Simon D.M. and Beale, Andrew M.}},
  keywords     = {{chemical imaging; diffraction; multimodal; oxygen storage capacity}},
  language     = {{eng}},
  number       = {{12}},
  publisher    = {{Wiley-VCH Verlag}},
  series       = {{Chemistry-Methods}},
  title        = {{Rationalizing Deactivation Behavior in Pyrochlore-Type CeO<sub>2</sub>-ZrO<sub>2</sub> Oxygen Storage Catalysts Using Multimodal Nano X-Ray Fluorescence Computed Tomography, X-Ray Diffraction Computed Tomography, and Scanning Three-Dimensional X-ray Diffraction}},
  url          = {{http://dx.doi.org/10.1002/cmtd.202500074}},
  doi          = {{10.1002/cmtd.202500074}},
  volume       = {{5}},
  year         = {{2025}},
}