Leaching Stability of Simulated Waste Forms for Immobilizing An^(3+) by Gd_2Zr_2O_7 with Nd^(3+)

In order to investigate the anti-leaching capability of pyrochlore Gd2Zr2O7 immobilized An3＋, trivalent neodymium was used as the simulacrums for radioactive wastes with trivalence, Gd2-xNdxZr2O7（0.0 ≤ x≤2.0） series samples were successfully synthesized by high temperature solid reaction and using Gd2O3, ZrO2 powders as starting materials. The experiments of long-term chemical stability were conducted in synthetic seawater at 40 and 70 ℃. The XRD diffractive data and extraction ratio of as-received samples were collected with the help of X-ray diffraction （XRD） instrument and inductively coupled plasma mass spectrometry （ICP- Mass）. The results indicate that the phases of as-received compounds keep the single phase of pyrochlore. The extraction ratio of Gd3＋, Zr4＋ and Nd3＋ in waste forms is increasing with the increase of immersion time in synthetic seawater. The extraction ratio of waste forms at 70 ℃ is higher than at 40 ℃. The highest extraction ratio of Gd3＋, Zr4＋ and Nd3＋ after 42 days is near 0.025 8, 0.003 8 and 0.045 2 μg.mL-1, respectively.

Chemical stability of simulated waste forms Zr1–xNdxSiO4–x/2： Influence of temperature, pH and their combined effects

The chemical stability of simulated waste forms Zr_（1–x）Nd_xSiO_（4–x/2） was investigated using the static leach test（MCC-1） with lixiviants of three pH values（pH=4, 6.7 and 10） at three temperature points（40, 90 and 150 oC） for periods ranging from 1 to 42 d, and the influence of temperature, pH, as well as their combined effects were explored in detail. The results showed that all the normalized release rate of Nd firstly decreased with leaching time and closed to equilibrium after 14 d. As the temperature increased, the normalized release rate of Nd also increased, but it was no more than 3×10^（–5） g/（m^2·d）. And, the normalized release rate of Nd reached the highest values（~5×10^（–5） g/（m^2·d）） when pH=4, whilst the normalized release rate of Nd remained the lowest value（~1×10^（–5） g/（m^2·d）） near neutral environment（pH=6.7）.

Self-propagating high-temperature synthesis of ZrO_2 incorporated Gd_2Ti_2O_7 pyrochlore

In this research, Zr-doped Gd_2Ti_2O_7 pyrochlores, with the composition of Gd_2(Ti_(1-x)Zr_x)_2O_7, were firstly synthesized by self-propagating high-temperature synthesis plus quick pressing(SHS/QP) using CuO as the oxidant and Ti as the reductant. To improve the radiation resistance of titanate–pyrochlore, up to 35 at% Zr was incorporated to substitute the Ti site of Gd_2Ti_2O_7 pyrochlore(Gd_2(Ti_(0.75)Zr_(0.35))_2O_7). XRD and SEM microstructural characterizations showed the formation of a composite ceramic with the major pyrochlore phase and the minor Cu phase. The generated temperature of samples decreased from 1702to 1011 ℃ with increasing Zr content. The effects of sintering temperature and pressure time on phase composition and microstructure were systematically studied. Besides, the influence of thermal transmission on the whole combustion process was also explored. The pyrochlore-based waste form possessed high bulk density of 6.25 g/cm^3 and Vickers hardness of 10.81 GPa. The MCC-1 leaching test showed the normalized elemental leaching rates(42d) of Cu, Gd, and Zr are 1.27×10^(-2), 1.33×10^(-3), and 8.44×10^(-7)g·m^(-2)·d^(-1), respectively.

Crystalline compounds for remediation of rare-earth fission products:A review

Rare earth(RE)-containing crystals have been investigated as media for the immobilization of RE fission products from nuclear waste streams.During reprocessing of spent nuclear fuel,fission products including REs,alkalis,and alkaline earths released from the fuel.One viable option to immobilize the RE fission products is to incorporate them into chemically durable crystalline phases in specific waste forms.This study summarizes the crystal structures and synthesis methods of six RE-containing compounds that have applications in remediation of RE fission products.These compounds include oxyapatite(AE_(2)RE_(8)(SiO_(4))_(6)O_(2)),oxychloride(REOCl),borosilicate(RE_(3)BSi_(2)O_(10)),pyrochlore(RE_(2)M_(2)O_(7)),monazite(REPO_(4)),and perovskite(REMO_(3))where AE denotes alkaline earth metals and M denotes transition metals.This review provides an overview of literature on the usage of these six compounds for immobilizing RE fission products and summarizes different synthesis methods for producing these compounds.Comparisons of structural parameters with different REs in each compound are also discussed.

Chemical stability of Ce-doped zircon ceramics:Influence of p H,temperature and their coupling effects

Zircon was employed to immobilize simulated tetravalentactinide nuclide（Ce^4＋）. Zr_（1–x）Ce_xSiO_4（0≤x≤0.10） ceramics were synthesized and their chemical durabilities were investigated systematically. The effects of p H and temperature on the chemical durability of the as-prepared compounds were investigated using the MCC-1 static leaching test, and their coupling effects were also explored. It was found that the normalized release rates of Ce in deionized water and alkaline solutions（pH=10） were smaller than those in acid solutions（p H=4）. At a certain p H value, the normalized release rate of Ce（LR Ce） increased with the temperature in the initial period. However, the leaching progress almost reached a balance after 14 days, and both of the p H and the temperature had slight impact on the leaching of Ce element. Moreover, the LR_（Ce） were below 10^（–5）g/m^2/d after 42 days, which was lower than those of other nuclear waste forms in all discussed leachates.