The molten salt waste from the pyroprocess is one of the problematic wastes to directly apply a conventional process such as vitrification or ceramization. This study suggested a novel method using a reactive material for metal chlorides at a molten temperature of salt waste, and then converting them into manageable product at a high temperature. The inorganic composite, SAP (SiO2-Al2O3-P2O5), synthesized by a conventional sol-gel process has three or four distinctive domains that are bonded sequentially, Si-O-Si-O-A-O-P-O-P. The P-rich phase in the SAP composite is unstable for producing a series of reactive sites when in contact with a molten LiCl salt. After the reaction, metal aluminosilicate, metal aluminophosphate, metal phosphates and gaseous chlorines are generated. From this process, the volatile salt waste is stabilized and it is possible to apply a high temperature process. The reaction products were fabricated successfully by using a borosilicate glass with an arbitrary composition as a chemical binder. There was a low possibility for the valorization of radionuclides up to 1200 degrees C, based on the result of the thermo gravimetric analysis. The Cs and Sr leach rates by the PCT-A method were about 1 x 10(-3) g/(m2 day). For the final disposal of the problematic salt waste, this approach suggested the design concept of an effective stabilizer for metal chlorides and revealed the chemical route to the fabrication of monolithic wasteform by using a composite as an example. Using this method, we could obtain a higher disposal efficiency and lower waste volume, compared with the present immobilization methods.
The molten salt waste from a pyroprocess to recover uranium and transuranic elements is one of the problematic radioactive wastes to be solidified into a durable wasteform for its final disposal. By using a novel method, named as the GRSS (gel-route stabilization/solidification) method, a molten salt waste was treated to produce a unique wasteform. A borosilicate glass as a chemical binder dissolves the silicate compounds in the gel products to produce one amorphous phase while most of the phosphates are encapsulated by the vitrified phase. Also, Cs in the gel product is preferentially situated in the silicate phase, and it is vitrified into a glassy phase after a heat treatment. The Sr-containing phase is mainly phosphate compounds and encapsulated by the glassy phase. These phenomena could be identified by the static and dynamic leaching test that revealed a high leach resistance of radionuclides. The leach rates were about 10(-3) - 10(-2) g/m2 x day for Cs and 10(-4) - 10(-3) g/m2 x day for Sr, and the leached fractions of them were predicted to be 0.89% and 0.39% at 900 days, respectively. This paper describes the characteristics of a unique wasteform containing a molten salt waste and provides important information on a newly developed immobilization technology for salt wastes, the GRSS method.
The dehydration schemes of rare earth (La, Ce, Nd, Pr, Sm. Eu, Gd, Y) chloride hydrates was investigated by using a dehydration apparatus. To prevent the formation of the rare earth oxychlorides, the operation temperature was changed step by step (80 150 230 ) based on the TGA (thermo-gravimetric analysis) results of the rare earth chloride hydrates. A vacuum pump and preheated Ar gas were used to effectively remove the evaporated moisture and maintain an inert condition in the dehydration apparatus. The dehydration temperature of the rare earth chloride hydrate was increased when the atomic number of the rare earth nuclide was increased. The content of the moisture in the rare earth chloride hydrate was decreased below 10% in the dehydration apparatus.
For a treatment of molten salt wastes generated from a pyroprocessing of oxide spent fuel, we had suggested a stable chemical route, named GRSS (Gel-Route Stabilization & Solidification), and a subsequent consolidation method. By using this method, a series of monolithic wasteforms with different conditions were fabricated, and then their physicochemical properties were investigated. A simulated salt containing 90wt% LiCl, 6.8wt% CsCl, and 3.2wt% SrCl2 was treated with a gel-forming material system, Si/Al/P = 0.4/0.4/0.2 and 0.35/0.35/0.3, and the gel-products were treated at 1100C° after mixing with borosilicate glass powder, where the salt loadings were about 16∼20wt%. The solidified products had a density of 2.3∼2.35g/cm3, a micro-hardness of 4.69∼4.72GPa, a glass transition temperature of 528∼537C°, and a thermal expansion coefficient of 1.65×10−7∼3.38×10−5/C°. Leaching results by the PCT-A method revealed leached rates, 10−3∼10−2g/m2day and 10−4∼10−3g/m2day for Cs and Sr, respectively. From the long-term ISO leaching test, the 900day-leached fraction of Cs and Sr predicted by a semi-empirical model were 0.89% and 0.39%. The leaching behaviors indicated that Cs would be immobilized into a Si-rich phase while Sr would be in a P-rich phase. The experimental results revealed that the GRSS method could be an alternative method for a solidification of radioactive molten salt wastes.
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