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Solubility of Mixed Lanthanide Hydroxide and Oxide Solid Solutions
Moniruzzaman, Mohammad,Kobayashi, Taishi,Sasaki, Takayuki Korean Radioactive Waste Society 2021 방사성폐기물학회지 Vol.19 No.3
The solubilities of different multicomponent lanthanide oxide (Ln<sub>2</sub>O<sub>3</sub>) solid solutions including binary (Ln<sub>1</sub> and Ln<sub>2</sub> = La, Nd, Eu, or Tm), ternary (Ln<sub>1</sub>, Ln<sub>2</sub>, and Ln<sub>3</sub> = La, Nd, Eu, or Tm), and higher systems (Ln = La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu) were studied after aging for four weeks at 60℃. Our recent study revealed that the phase transformations in binary ((La, Nd) and (La, Eu)) and ternary (La, Nd, Eu) systems are responsible for the formation of (La, Nd)(OH)<sub>3</sub>, (La, Eu)(OH)<sub>3</sub>, and (La, Nd, Eu)(OH)<sub>3</sub> solid solutions, respectively. The variations in the mole fractions of La<sup>3+</sup>, Nd<sup>3+</sup>, and Eu<sup>3+</sup> in the sample solutions of these hydroxide solid solutions indicated that a thermodynamic equilibrium might account for the apparent La, Nd, and Eu solubilities. Conversely, the binary and ternary systems containing Tm<sub>2</sub>O<sub>3</sub> as the heavy lanthanide oxide retained the oxide-based solid solutions, and their solubility behaviors were dominated by their congruent dissolutions. In the higher multicomponent system, the X-ray diffraction patterns of the solid phases, before and after contact with the aqueous phase indicated the formation of a stable oxide solid solution and their solubility behavior was explained by its congruent dissolution.
Tonna Ryutaro,Sasaki Takayuki,Kodama Yuji,Kobayashi Taishi,Akiyama Daisuke,Kirishima Akira,Sato Nobuaki,Kumagai Yuta,Kusaka Ryoji,Watanabe Masayuki 한국원자력학회 2023 Nuclear Engineering and Technology Vol.55 No.4
Simulated debris was synthesized using UO2, Zr, and stainless steel and a heat treatment method under inert or oxidizing conditions. The primary U solid phase of the debris synthesized at 1473 K under inert conditions was UO2, whereas a (U, Zr)O2 solid solution formed at 1873 K. Under oxidizing conditions, a mixture of U3O8 and (Fe, Cr)UO4 phases formed at 1473 K, whereas a (U, Zr)O2+x solid solution formed at 1873 K. The leaching behavior of the fission products from the simulated debris was evaluated using two methods: the irradiation method, for which fission products were produced via neutron irradiation, and the doping method, for which trace amounts of non-radioactive elements were doped into the debris. The dissolution behavior of U depended on the properties of the debris and aqueous solution for immersion. Cs, Sr, and Ba leached out regardless of the primary solid phases. The leaching of high-valence Eu and Ru ions was suppressed, possibly owing to their solid-solution reaction with or incorporation into the uranium compounds of the simulated debris.