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Chemical and elemental mapping of spent nuclear fuel sections by soft X-ray spectromicroscopy

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Chemical and elemental mapping of spent nuclear fuel sections by soft X-ray spectromicroscopy. / Ditter, Alex S.; Smiles, Danil E.; Lussier, Daniel et al.
In: Journal of Synchrotron Radiation, Vol. 29, No. 1, 31.01.2022, p. 67-79.

Research output: Contribution to Journal/MagazineJournal articlepeer-review

Harvard

Ditter, AS, Smiles, DE, Lussier, D, Altman, AB, Bachhav, M, He, L, Mara, MW, Degueldre, C, Minasian, SG & Shuh, DK 2022, 'Chemical and elemental mapping of spent nuclear fuel sections by soft X-ray spectromicroscopy', Journal of Synchrotron Radiation, vol. 29, no. 1, pp. 67-79. https://doi.org/10.1107/S1600577521012315

APA

Ditter, A. S., Smiles, D. E., Lussier, D., Altman, A. B., Bachhav, M., He, L., Mara, M. W., Degueldre, C., Minasian, S. G., & Shuh, D. K. (2022). Chemical and elemental mapping of spent nuclear fuel sections by soft X-ray spectromicroscopy. Journal of Synchrotron Radiation, 29(1), 67-79. https://doi.org/10.1107/S1600577521012315

Vancouver

Ditter AS, Smiles DE, Lussier D, Altman AB, Bachhav M, He L et al. Chemical and elemental mapping of spent nuclear fuel sections by soft X-ray spectromicroscopy. Journal of Synchrotron Radiation. 2022 Jan 31;29(1):67-79. doi: 10.1107/S1600577521012315

Author

Ditter, Alex S. ; Smiles, Danil E. ; Lussier, Daniel et al. / Chemical and elemental mapping of spent nuclear fuel sections by soft X-ray spectromicroscopy. In: Journal of Synchrotron Radiation. 2022 ; Vol. 29, No. 1. pp. 67-79.

Bibtex

@article{236ebc9f7c714a8fb9226e1db95732bd,
title = "Chemical and elemental mapping of spent nuclear fuel sections by soft X-ray spectromicroscopy",
abstract = "Soft X-ray spectromicroscopy at the O K-edge, U N4,5-edges and Ce M4,5-edges has been performed on focused ion beam sections of spent nuclear fuel for the first time, yielding chemical information on the sub-micrometer scale. To analyze these data, a modification to non-negative matrix factorization (NMF) was developed, in which the data are no longer required to be non-negative, but the non-negativity of the spectral components and fit coefficients is largely preserved. The modified NMF method was utilized at the O K-edge to distinguish between two components, one present in the bulk of the sample similar to UO2 and one present at the interface of the sample which is a hyperstoichiometric UO2+x species. The species maps are consistent with a model of a thin layer of UO2+x over the entire sample, which is likely explained by oxidation after focused ion beam (FIB) sectioning. In addition to the uranium oxide bulk of the sample, Ce measurements were also performed to investigate the oxidation state of that fission product, which is the subject of considerable interest. Analysis of the Ce spectra shows that Ce is in a predominantly trivalent state, with a possible contribution from tetravalent Ce. Atom probe analysis was performed to provide confirmation of the presence and localization of Ce in the spent fuel.",
author = "Ditter, {Alex S.} and Smiles, {Danil E.} and Daniel Lussier and Altman, {Alison B.} and Mukesh Bachhav and Lingfeng He and Mara, {Michael W.} and Claude Degueldre and Minasian, {Stefan G.} and Shuh, {David K.}",
year = "2022",
month = jan,
day = "31",
doi = "10.1107/S1600577521012315",
language = "English",
volume = "29",
pages = "67--79",
journal = "Journal of Synchrotron Radiation",
issn = "0909-0495",
publisher = "International Union of Crystallography",
number = "1",

}

RIS

TY - JOUR

T1 - Chemical and elemental mapping of spent nuclear fuel sections by soft X-ray spectromicroscopy

AU - Ditter, Alex S.

AU - Smiles, Danil E.

AU - Lussier, Daniel

AU - Altman, Alison B.

AU - Bachhav, Mukesh

AU - He, Lingfeng

AU - Mara, Michael W.

AU - Degueldre, Claude

AU - Minasian, Stefan G.

AU - Shuh, David K.

PY - 2022/1/31

Y1 - 2022/1/31

N2 - Soft X-ray spectromicroscopy at the O K-edge, U N4,5-edges and Ce M4,5-edges has been performed on focused ion beam sections of spent nuclear fuel for the first time, yielding chemical information on the sub-micrometer scale. To analyze these data, a modification to non-negative matrix factorization (NMF) was developed, in which the data are no longer required to be non-negative, but the non-negativity of the spectral components and fit coefficients is largely preserved. The modified NMF method was utilized at the O K-edge to distinguish between two components, one present in the bulk of the sample similar to UO2 and one present at the interface of the sample which is a hyperstoichiometric UO2+x species. The species maps are consistent with a model of a thin layer of UO2+x over the entire sample, which is likely explained by oxidation after focused ion beam (FIB) sectioning. In addition to the uranium oxide bulk of the sample, Ce measurements were also performed to investigate the oxidation state of that fission product, which is the subject of considerable interest. Analysis of the Ce spectra shows that Ce is in a predominantly trivalent state, with a possible contribution from tetravalent Ce. Atom probe analysis was performed to provide confirmation of the presence and localization of Ce in the spent fuel.

AB - Soft X-ray spectromicroscopy at the O K-edge, U N4,5-edges and Ce M4,5-edges has been performed on focused ion beam sections of spent nuclear fuel for the first time, yielding chemical information on the sub-micrometer scale. To analyze these data, a modification to non-negative matrix factorization (NMF) was developed, in which the data are no longer required to be non-negative, but the non-negativity of the spectral components and fit coefficients is largely preserved. The modified NMF method was utilized at the O K-edge to distinguish between two components, one present in the bulk of the sample similar to UO2 and one present at the interface of the sample which is a hyperstoichiometric UO2+x species. The species maps are consistent with a model of a thin layer of UO2+x over the entire sample, which is likely explained by oxidation after focused ion beam (FIB) sectioning. In addition to the uranium oxide bulk of the sample, Ce measurements were also performed to investigate the oxidation state of that fission product, which is the subject of considerable interest. Analysis of the Ce spectra shows that Ce is in a predominantly trivalent state, with a possible contribution from tetravalent Ce. Atom probe analysis was performed to provide confirmation of the presence and localization of Ce in the spent fuel.

U2 - 10.1107/S1600577521012315

DO - 10.1107/S1600577521012315

M3 - Journal article

VL - 29

SP - 67

EP - 79

JO - Journal of Synchrotron Radiation

JF - Journal of Synchrotron Radiation

SN - 0909-0495

IS - 1

ER -