Synthesis, Characterization, and Stability of Americium Phosphate, AmPO<sub>4</sub>

Popa, Karin; Vigier, Jean-François; Martel, Laura; Manara, D.; Colle, Jean‐Yves; Blanco, Oliver Dieste; Wiss, T.; Freis, Daniel; Konings, R.J.M.

doi:10.1021/acs.inorgchem.0c00697

Cited by 9 publications

(9 citation statements)

References 49 publications

(75 reference statements)

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“…Finally, we recorded the spectrum of La 0.96 Am 0.04 PO 4 (Figure 4a,b and Table S3) and determined a composition of La 0.957 Am 0.043 PO 4 (the uncertainty is 0.043 ± 0.008). Peak 8 corresponds to AmPO 4 29 with an amount of 2% in agreement with the XRD results. All of the experimental shifts are reported in Table 2.…”

Section: Methodssupporting

confidence: 88%

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Local Structure and Magnetism of La_1–xM_xPO₄ (M = Sm, ²³⁹Pu, ²⁴¹Am) Explained by Experimental and Computational Analyses

et al. 2021

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With their high chemical and self-irradiation stability, crystalline monazites are among the most promising materials for the encapsulation of nuclear wastes. Yet, the local and magnetic structures of the matrices doped with low-content actinide cation, depicted as most resistant, are still unclear. This limits the development of theoretical approaches predicting their behavior under extreme conditionsself-irradiation and long-term leaching. Here, we characterize the model matrices La 1−x M x PO 4 (0 ≤ x ≤ 0.10)with M = Sm, 239 Pu, 241 Amby X-ray diffraction and solid-state 31 P NMR. As an example, we confirm that La 0.96 241 Am 0.04 PO 4 has higher self-irradiation resistance compared to 241 AmPO 4 . Further, computational analyses show that magnetic properties of the Pu complex are strongly affected by the J-mixing and the paramagnetic NMR shifts are dominated by the Fermi contact contribution, arising from delocalization of the spin density of the cation toward the phosphorus through the bonds.

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Section: Methodssupporting

confidence: 88%

“…A different kind of variation can be expected when the material reaches higher doses and the well-described models 30 cannot be applied for these low doses. Overall, the V/ V 0 parameters of AmPO 4 29 are almost twice that of La 0.96 Am 0.04 PO 4 for the same dose (Figure 5a). The present sample is thus more resistant to radiation damage.…”

Section: Methodsmentioning

confidence: 88%

Local Structure and Magnetism of La_1–xM_xPO₄ (M = Sm, ²³⁹Pu, ²⁴¹Am) Explained by Experimental and Computational Analyses

et al. 2021

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“…The shifts of the modes in AmVO 4 compared to the Ln VO 4 series are very similar to AmPO 4 and Ln PO 4 . However, the strong broadening of the modes after aging that was observed for AmPO 4 did not occur.…”

Section: Resultssupporting

confidence: 87%

Synthesis, Characterization, and Stability of Two Americium Vanadates, AmVO₃ and AmVO₄

et al. 2023

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In search for chemically stable americium compounds with high power densities for radioisotope sources for space applications, AmVO3 and AmVO4 were prepared by a solid-state reaction. We present here their crystal structure at room temperature solved by powder X-ray diffraction combined with Rietveld refinement. Their thermal and self-irradiation stabilities have been studied. The oxidation states of americium were confirmed by the Am M5 edge high-resolution X-ray absorption near-edge structure (HR-XANES) technique. Such ceramics are investigated as potential power sources for space applications like radioisotope thermoelectric generators, and they have to endure extreme conditions including vacuum, high or low temperatures, and internal irradiation. Thus, their stability under self-irradiation and heat treatment in inert and oxidizing atmospheres was tested and discussed relative to other compounds with a high content of americium.

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“…Additionally, the low chemical reactivity, low solubility, and resistance to radiation damage also make xenotime a promising ceramic waste host candidate for permanent immobilization and disposal of actinides associated with nuclear wastes. − As xenotime is isostructural to other zircon structure-type phases, including coffinite (USiO 4 ), thorite (ThSiO 4 ), and stetindite (CeSiO 4 ), they share many similar thermochemical and thermophysical properties. Xenotime also has the ability to accommodate trivalent elements, the dominant valence state of the late actinides (Am–Es), − which were predicted to be thermodynamically unstable in orthosilicates. − All of the actinide orthophosphates (Pu–Es) synthesized in the air have been reported to adopt the monazite structure, ,,− yet there are also reports that Np and Pu were found to be stabilized in the xenotime structure (Y ( x ) An (1– x ) PO 4 , where An = Np or Pu) under reducing environments . This stabilization within the xenotime structure could most likely be attributed to the favorable energetics of mixing, similar to what is found with uranothorite (Th ( x ) U (1– x ) SiO 4 ). ,, …”

Section: Introductionmentioning

confidence: 99%

Crystal Chemistry and Thermodynamics of HREE (Er, Yb) Mixing in a Xenotime Solid Solution

Strzelecki

Reece

Zhao

et al. 2022

ACS Earth Space Chem.

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Rare earth elements (REEs), the 15 naturally occurring lanthanides plus yttrium and scandium, are ubiquitously used in modern life as they are critical components of many advanced devices and technologies. However, the demand for REEs is not equal, with the heavy rare earth elements (HREEs) having a higher demand. Xenotime (HREEPO4) is an important HREE ore mineral and globally is an economical source of HREE. Most of the crystallographic and thermodynamic properties of xenotime endmembers have been elucidated by calorimetric, solubility, and high-pressure studies. Yet, in natural systems, endmembers are rarely encountered, and instead, REE solid solutions are more commonly observed. In this work, we characterize the crystal chemistry, thermodynamics of HREE mixing, and high-temperature material behaviors and thermochemistry of a synthetic erbium (Er)–ytterbium (Yb) binary xenotime solid solution (Er(x)Yb(1–x)PO4) using a suite of experimental techniques, including X-ray fluorescence spectroscopy, synchrotron X-ray powder diffraction implemented with Rietveld analysis, Fourier transform infrared spectroscopy coupled with attenuated total reflectance, Raman spectroscopy, thermogravimetric analysis coupled with differential scanning calorimetry, and high-temperature oxide melt drop solution calorimetry. Our results shed light on the formation of natural xenotimes and lay the foundation for their industrial applications as thermal coating materials.

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Synthesis, Characterization, and Stability of Americium Phosphate, AmPO₄

Cited by 9 publications

References 49 publications

Local Structure and Magnetism of La_1–xM_xPO₄ (M = Sm, ²³⁹Pu, ²⁴¹Am) Explained by Experimental and Computational Analyses

Local Structure and Magnetism of La_1–xM_xPO₄ (M = Sm, ²³⁹Pu, ²⁴¹Am) Explained by Experimental and Computational Analyses

Synthesis, Characterization, and Stability of Two Americium Vanadates, AmVO₃ and AmVO₄

Crystal Chemistry and Thermodynamics of HREE (Er, Yb) Mixing in a Xenotime Solid Solution

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Synthesis, Characterization, and Stability of Americium Phosphate, AmPO4

Cited by 9 publications

References 49 publications

Local Structure and Magnetism of La1–xMxPO4 (M = Sm, 239Pu, 241Am) Explained by Experimental and Computational Analyses

Local Structure and Magnetism of La1–xMxPO4 (M = Sm, 239Pu, 241Am) Explained by Experimental and Computational Analyses

Synthesis, Characterization, and Stability of Two Americium Vanadates, AmVO3 and AmVO4

Crystal Chemistry and Thermodynamics of HREE (Er, Yb) Mixing in a Xenotime Solid Solution

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Product

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Synthesis, Characterization, and Stability of Americium Phosphate, AmPO₄

Local Structure and Magnetism of La_1–xM_xPO₄ (M = Sm, ²³⁹Pu, ²⁴¹Am) Explained by Experimental and Computational Analyses

Local Structure and Magnetism of La_1–xM_xPO₄ (M = Sm, ²³⁹Pu, ²⁴¹Am) Explained by Experimental and Computational Analyses

Synthesis, Characterization, and Stability of Two Americium Vanadates, AmVO₃ and AmVO₄