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Characterization of vandenbrandeite: A potential alteration product of spent nuclear fuel

  • Victoria L. Frankland ORCID logo , Antoni E. Milodowski , Robert A. Lawrence , Marco Sacchi and David Read
Published/Copyright: March 30, 2023
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American Mineralogist
From the journal American Mineralogist Volume 108 Issue 4

Abstract

The use of copper canisters in the Swedish KBS-3 concept for spent nuclear fuel disposal could result in the formation of copper-bearing uranyl phases should a canister suffer from defects or if the containment were to fail before reducing conditions are established in the repository. Most uranyl species would be expected to display higher solubility than the original uranium(IV) dioxide fuel, leading to enhanced release, though this would depend on the phase and prevailing groundwater conditions. Secondary alteration products may also be poorly crystalline or even amorphous, making characterization difficult during the pre-closure period owing to the high radiation field close to the canister. Vandenbrandeite, [CuUO2(OH)4], is a rare mineral in nature but known to form by alteration of primary uraninite through interaction with oxidizing groundwater containing dissolved copper. Consequently, an attempt has been made to characterize two vandenbrandeite specimens of varying crystallinity by luminescence and multiple-laser Raman spectroscopy; techniques amenable to remote, robotic deployment and which have proved useful in discriminating other uranyl oxy-hydroxides, silicates, and phosphates. The first reported luminescence emission and excitation spectra for vandenbrandeite revealed near-negligible luminescence, with a slightly enhanced signal for the specimen displaying poorer crystallinity. This observation agrees well with density functional theory calculations. The simulated projected density of state and band structure show an unlikely transition from the U f-orbitals to Cu d-orbitals, or O states, would be required for luminescence to be detectable; this probably improves for poorly crystalline specimens as the spatial overlap between the orbitals increases. Furthermore, negligible differences in the number of peaks and peak positions were detected in the laser wavelength-dependent Raman spectra although again, variation in background noise and peak shape was observed based on the degree of crystallinity. Good agreement was obtained between experimental and simulated Raman spectra, particularly with the environmentally sensitive axial uranyl stretching modes, validating the crystal system derived in this study. The findings of this study suggest luminescence spectroscopy, when combined with Raman spectroscopy, may be able to both identify vandenbrandeite and distinguish between crystalline and amorphous forms based on their relative luminescence intensity.

Keywords: Raman spectroscopy; time-resolved laser fluorescence spectroscopy; density functional theory Raman simulation; projected density of states

Funding statement: This work was supported by funding from the Engineering & Physical Science Research Council projects EP/L014041/1 (DISTINCTIVE) and EP/S01019X/1 (TRANSCEND). The Raman and TRLFS apparatus were supported by capital grants from the Engineering & Physical Science Research Council (EP/M022749/1) and the Natural Environment Research Council (NERC/CC041), respectively.

Acknowledgments

The authors wish to thank Kay Green of the British Geological Survey and Tom Cotterell from the National Museum of Wales for the loan of the reference mineral samples. Acknowledgments are also given to John-William Brown, Sarah Heisig, Dave Jones, Dan Driscoll, and Carol Crean (University of Surrey) for advice and support.

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Received: 2021-08-25
Accepted: 2022-04-22
Published Online: 2023-03-30
Published in Print: 2023-04-25

© 2023 by Mineralogical Society of America

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  2. The iron spin transition of deep nitrogen-bearing mineral Fe3N1.2 at high pressure
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  6. Structural changes in shocked tektite and their implications to impact-induced glass formation
  7. Characterization of vandenbrandeite: A potential alteration product of spent nuclear fuel
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  17. Presentation of the Mineralogical Society of America Award for 2022 to Benjamin M. Tutolo
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  21. New Mineral Names
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https://doi.org/10.2138/am-2022-8272
Keywords for this article
Raman spectroscopy; time-resolved laser fluorescence spectroscopy; density functional theory Raman simulation; projected density of states

Articles in the same Issue

  1. Mineralogy and geochemistry of hot spring deposits at Námafjall, Iceland: Analog for sulfate soils at Gusev crater, Mars
  2. The iron spin transition of deep nitrogen-bearing mineral Fe3N1.2 at high pressure
  3. Hydrogen occupation and hydrogen-induced volume expansion in Fe0.9Ni0.1Dx at high P-T conditions
  4. Volumes and spin states of FeHx: Implication for the density and temperature of the Earth’s core
  5. Thermodynamic characterization of synthetic lead-arsenate apatites with different halogen substitutions
  6. Structural changes in shocked tektite and their implications to impact-induced glass formation
  7. Characterization of vandenbrandeite: A potential alteration product of spent nuclear fuel
  8. The NaCl-CaCO3 and NaCl-MgCO3 systems at 6 GPa: Link between saline and carbonatitic diamond forming melts
  9. Single-crystal elasticity of (Al,Fe)-bearing bridgmanite up to 82 GPa
  10. Single-crystal X-ray diffraction of fluorapatite to 61 GPa
  11. Iron and aluminum substitution mechanism in the perovskite phase in the system MgSiO3-FeAlO3-MgO
  12. Ultrasonic studies of alkali-rich hydrous silicate glasses: Elasticity, density, and implications for water dissolution mechanisms
  13. Gadolinium-dominant monazite and xenotime: Selective hydrothermal enrichment of middle REE during low-temperature alteration of uraninite, brannerite, and fluorapatite (the Zimná Voda REE-U-Au quartz vein, Western Carpathians, Slovakia)
  14. Nucleation of Th-rich cerianite on halloysite surface in a regolith-hosted rare earth elements deposit in South China
  15. Presentation of the Dana Medal of the Mineralogical Society of America for 2022 to Cin-Ty Lee
  16. Acceptance of the Dana Medal of the Mineralogical Society of America for 2022
  17. Presentation of the Mineralogical Society of America Award for 2022 to Benjamin M. Tutolo
  18. Acceptance of the Mineralogical Society of America Award for 2022
  19. Presentation of the 2022 Roebling Medal of the Mineralogical Society of America to John W. Valley
  20. Acceptance of the 2022 Roebling Medal of the Mineralogical Society of America
  21. New Mineral Names
  22. Book Review
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