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| Hauptseite > Publikationsdatenbank > Investigation of Radiation Damage in the Monazite-Type Solid Solution La 1– x Ce x PO 4 |
| Hauptseite > Publikationsdatenbank > Investigation of Radiation Damage in the Monazite-Type Solid Solution La 1– x Ce x PO 4 |
| Journal Article | FZJ-2024-05510 |
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2024
American Chemical Society
Washington, DC
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Please use a persistent id in citations: doi:10.1021/acs.inorgchem.4c02041 doi:10.34734/FZJ-2024-05510
Abstract: Crystalline materials such as monazite have been considered for thestorage of radionuclides due to their favorable radiation stability. Understanding theirstructural chemical response to radiation damage as solid solutions is a key componentof determining their suitability for radionuclide immobilization. Herein, highresolutionstructural studies were performed on ceramics of the monazite solidsolution La1−xCexPO4 (x = 0.25, 0.5, 0.75, 1) in order to understand the role ofstructural chemistry on irradiation stability. Ceramic samples were irradiated with 14MeV Au ions with 1014 ions/cm2 and 1015 ions/cm2 to simulate the recoil of daughternuclei from the alpha decay of actinide radionuclides. The extent of radiation damagewas analyzed in detail using scanning electron microscopy (SEM), Ramanspectroscopy, grazing incidence X-ray diffraction (GI-XRD), and high-energy-resolution fluorescence detection extended X-rayabsorption fine structure (HERFD-EXAFS) spectroscopy. SEM and Raman spectroscopy revealed extensive structural damage aswell as the importance of grain boundary regions, which appear to impede the propagation of defects. Both radiation-inducedamorphization and recrystallization were studied by GI-XRD, highlighting the ability of monazite to remain crystalline at highfluences throughout the solid solution. Both, diffraction and HERFD-EXAFS experiments show that while atomic disorder isincreased in irradiated samples compared to pristine ceramics, the short-range order was found to be largely preserved, facilitatingrecrystallization. However, the extent of recrystallization was found to be dependent on the solid solution composition. Particularly,the samples with uneven ratios of solute cations, La0.75Ce0.25PO4 and La0.25Ce0.75PO4 were observed to exhibit the least apparentradiation damage resistance. The findings of this work are discussed in the context of the monazite solid solution chemistry and theirappropriateness for radionuclide immobilization.
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