Comparative chemical and structural analyses of two uranium dioxide fuel pellets

Tyler L. Spano; Antonio Simonetti; Loretta Corcoran; Philip A. Smith; Stefanie R. Lewis; Peter C. Burns

doi:10.1016/j.jnucmat.2019.02.038

Comparative chemical and structural analyses of two uranium dioxide fuel pellets

Tyler L. Spano, Antonio Simonetti, Loretta Corcoran, Philip A. Smith, Stefanie R. Lewis, Peter C. Burns

Materials & Chemistry Group

Research output: Contribution to journal › Article › peer-review

15 Scopus citations

Abstract

A comparative investigation of the trace element, U and Pb isotopic compositions, and structural attributes of two uranium dioxide fuel pellets was conducted for nuclear forensic applications. One fuel pellet consists of natural UO ₂ (0.71% ²³⁵ U), while the other contains enriched UO ₂ (3.98% ²³⁵ U). Numerous impurities, including transition metals, lanthanides, and main group elements were detected in both fuel pellets with total trace element contents that vary between 9.77 and 11.37 μg/g. The relative abundances of the transition metal impurities in the natural UO ₂ fuel pellet are linked to the source U ore and provide important insights into its provenance. X-ray fluorescence spectroscopy was utilized to investigate and compare the macro-(cm)-scale distribution of impurities within each of the fuel pellets. In addition, structural properties of the fuel pellets were examined using powder X-ray diffraction (PXRD) and Raman and infrared spectroscopy. Differences in the intensity of the T _2g U-O stretching vibrational mode were observed in the Raman spectra of the fuel pellets. Pb isotope ratios were investigated to potentially differentiate between the natural and enriched UO ₂ samples and are linked to the process history of these materials.

Original language	English
Pages (from-to)	149-161
Number of pages	13
Journal	Journal of Nuclear Materials
Volume	518
DOIs	https://doi.org/10.1016/j.jnucmat.2019.02.038
State	Published - May 2019

Funding

We thank Dr. Ginger E. Sigmon for making this work possible, and two anonymous reviewers for their helpful comments. This research was supported by the U.S. Department of Homeland Security grant DHS-14-DN-077-ARI , and the ND Energy Postdoctoral Fellowship Program. Analyses were conducted at the Midwest Isotopic and Trace Element Research Center (MITERAC), the Center for Environmental Science and Technology (CEST), the Actinide Center of Excellence (ACE), and the ND Energy Materials Characterization Facility (MCF) at the University of Notre Dame.

Keywords

Nuclear forensics
Pb isotopes
Transition metals
UO fuel
Uranium deposits

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10.1016/j.jnucmat.2019.02.038

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title = "Comparative chemical and structural analyses of two uranium dioxide fuel pellets",

abstract = " A comparative investigation of the trace element, U and Pb isotopic compositions, and structural attributes of two uranium dioxide fuel pellets was conducted for nuclear forensic applications. One fuel pellet consists of natural UO 2 (0.71% 235 U), while the other contains enriched UO 2 (3.98% 235 U). Numerous impurities, including transition metals, lanthanides, and main group elements were detected in both fuel pellets with total trace element contents that vary between 9.77 and 11.37 μg/g. The relative abundances of the transition metal impurities in the natural UO 2 fuel pellet are linked to the source U ore and provide important insights into its provenance. X-ray fluorescence spectroscopy was utilized to investigate and compare the macro-(cm)-scale distribution of impurities within each of the fuel pellets. In addition, structural properties of the fuel pellets were examined using powder X-ray diffraction (PXRD) and Raman and infrared spectroscopy. Differences in the intensity of the T 2g U-O stretching vibrational mode were observed in the Raman spectra of the fuel pellets. Pb isotope ratios were investigated to potentially differentiate between the natural and enriched UO 2 samples and are linked to the process history of these materials.",

keywords = "Nuclear forensics, Pb isotopes, Transition metals, UO fuel, Uranium deposits",

author = "Spano, {Tyler L.} and Antonio Simonetti and Loretta Corcoran and Smith, {Philip A.} and Lewis, {Stefanie R.} and Burns, {Peter C.}",

note = "Publisher Copyright: {\textcopyright} 2019",

year = "2019",

month = may,

doi = "10.1016/j.jnucmat.2019.02.038",

language = "English",

volume = "518",

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AU - Spano, Tyler L.

AU - Simonetti, Antonio

AU - Corcoran, Loretta

AU - Smith, Philip A.

AU - Lewis, Stefanie R.

AU - Burns, Peter C.

PY - 2019/5

Y1 - 2019/5

N2 - A comparative investigation of the trace element, U and Pb isotopic compositions, and structural attributes of two uranium dioxide fuel pellets was conducted for nuclear forensic applications. One fuel pellet consists of natural UO 2 (0.71% 235 U), while the other contains enriched UO 2 (3.98% 235 U). Numerous impurities, including transition metals, lanthanides, and main group elements were detected in both fuel pellets with total trace element contents that vary between 9.77 and 11.37 μg/g. The relative abundances of the transition metal impurities in the natural UO 2 fuel pellet are linked to the source U ore and provide important insights into its provenance. X-ray fluorescence spectroscopy was utilized to investigate and compare the macro-(cm)-scale distribution of impurities within each of the fuel pellets. In addition, structural properties of the fuel pellets were examined using powder X-ray diffraction (PXRD) and Raman and infrared spectroscopy. Differences in the intensity of the T 2g U-O stretching vibrational mode were observed in the Raman spectra of the fuel pellets. Pb isotope ratios were investigated to potentially differentiate between the natural and enriched UO 2 samples and are linked to the process history of these materials.

AB - A comparative investigation of the trace element, U and Pb isotopic compositions, and structural attributes of two uranium dioxide fuel pellets was conducted for nuclear forensic applications. One fuel pellet consists of natural UO 2 (0.71% 235 U), while the other contains enriched UO 2 (3.98% 235 U). Numerous impurities, including transition metals, lanthanides, and main group elements were detected in both fuel pellets with total trace element contents that vary between 9.77 and 11.37 μg/g. The relative abundances of the transition metal impurities in the natural UO 2 fuel pellet are linked to the source U ore and provide important insights into its provenance. X-ray fluorescence spectroscopy was utilized to investigate and compare the macro-(cm)-scale distribution of impurities within each of the fuel pellets. In addition, structural properties of the fuel pellets were examined using powder X-ray diffraction (PXRD) and Raman and infrared spectroscopy. Differences in the intensity of the T 2g U-O stretching vibrational mode were observed in the Raman spectra of the fuel pellets. Pb isotope ratios were investigated to potentially differentiate between the natural and enriched UO 2 samples and are linked to the process history of these materials.

KW - Nuclear forensics

KW - Pb isotopes

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KW - Uranium deposits

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ER -

Comparative chemical and structural analyses of two uranium dioxide fuel pellets

Abstract

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Keywords

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