Li Wenqi,Ding Xingeng,Meng Cheng,Ren Chunrong,Wu Huating,Yang Hui
Rare earth phosphates (REPO 4 ) are considered as promising materials to immobilize the high-level radioactive waste. In the paper, Gd 1− x Yb x PO 4 ( x = 0, 0.1, 0.2, 0.4, 0.6, 0.8 and 1.0) series were prepared via the solid-state reaction using Gd as the surrogate for minor actinide Am and Cm, and the structure, phase transformation and morphology were characterized by XRD, Raman, TEM and SEM. With the calcination temperature ranging from 1200 to 1500 °C, the coexisted phases of monazite- and xenotime-type structure are observed in Gd 0.9 Yb 0.1 PO 4 . The monophasic xenotime-type Gd 0.9 Yb 0.1 PO 4 is obtained at 1600 °C. The monazite → xenotime transformation of Gd 1− x Yb x PO 4 depends on the substitution of Gd 3+ by Yb 3+ ions. With the decrease in Gd 3+ content, the gradual changes of FWHM and the hypsochromic shift of P-O symmetrical stretching vibration (Vs) are observed in the Raman spectra, indicating that the distortion of PO 4 tetrahedra occurs during the phase transformation process. The chemical durability test is measured by the ASTM product consistency test leaching method, and the normalized mass loss (NL Gd ) of Gd and (NL Yb ) of Yb is extremely low and shown in the order of 10 −6 –10 −7 g/m 2 for all the ceramics.
Cheng Meng,Xingeng Ding,Junchuan Zhao,Wenqi Li,Chunrong Ren,Hui Yang
Monazites are of considerable interest for immobilization of minor actinides . In this work, the Gd 1-x Ce x PO 4 (0 ≤ x ≤ 1) series is synthesized via conventional solid–state reaction using Ce as the surrogate for minor actinide americium (Am), with microstructure/phase structure characterized by XRD , HRTEM, μ-Raman, and SEM as well. The optimized temperature for preparation of monazite-type Gd 0.4 Ce 0.6 PO 4 solid solution is more than 1300 °C. At 1400 °C, the GdPO 4 ceramic is essentially monazite with little metastable xenotime phase. The metastable xenotime (GdPO 4 ) to monazite transformation occurs during the immobilizing phase of Ce element. The formation of monazite-type Gd 1-x Ce x PO 4 solid solutions in the range 0.1 ≤ x ≤ 1 is confirmed by the Rietveld refinement and Raman spectra . The change of Ce content has no significant influence on the morphology of the monazite-type Gd 1-x Ce x PO 4 compounds.
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