Effects of heat treatment and formulation on the phase composition and chemical durability of the EBR-ll ceramic waste form.

Ebert, W. E. ; Dietz, N. L. ; Janney, D. E.

Argonne National Laboratory

关键词: Halite;    Zeolites;    X-Ray Diffraction;    Binders;    Process Control;   

DOI  :  10.2172/881576
RP-ID  :  ANL-05/32
RP-ID  :  W-31-109-ENG-38
RP-ID  :  881576

美国|其它

来源: UNT Digital Library

【 摘 要 】

High-level radioactive waste salts generated during the electrometallurgical treatment of spent sodium-bonded nuclear fuel from the Experimental Breeder Reactor-II will be immobilized in a ceramic waste form (CWF). Tests are being conducted to evaluate the suitability of the CWF for disposal in the planned federal high-level radioactive waste repository at Yucca Mountain. In this report, the results of laboratory tests and analyses conducted to address product consistency and thermal stability issues called out in waste acceptance requirements are presented. The tests measure the impacts of (1) variations in the amounts of salt and binder glass used to make the CWF and (2) heat treatments on the phase composition and chemical durability of the waste form. A series of CWF materials was made to span the ranges of salt and glass contents that could be used during processing: between 5.0 and 15 mass% salt loaded into the zeolite (the nominal salt loading is 10.7%, and the process control range is 10.6 to 11.2 mass%), and between 20 and 30 mass% binder glass mixed with the salt-loaded zeolite (the nominal glass content is 25% and the process control range is 20 to 30 mass%). In another series of tests, samples of two CWF products made with the nominal salt and glass contents were reheated to measure the impact on the phase composition and durability: long-term heat treatments were conducted at 400 and 500 C for durations of 1 week, 4 weeks, 3 months, 6 months, and 1 year; short-term heat treatments were conducted at 600, 700, 800, and 850 C for durations of 4, 28, 52, and 100 hours. All of the CWF products that were made with different amounts of salt, zeolite, and glass and all of the heat-treated CWF samples were analyzed with powder X-ray diffraction to measure changes in phase compositions and subjected to 7-day product consistency tests to measure changes in the chemical durability. The salt loading had the greatest impact on phase composition and durability. A relatively large amount of nepheline, Na{sub 4}(AlSiO{sub 4}){sub 4}, was formed in the material made with 5.0 mass% salt loading, which was also the least durable of the materials that were tested. Nepheline was not detected in materials made with salt-loaded zeolites containing 15 or 20 mass% salt. Conversely, halite was not detected with XRD in materials made with 5.0 or 7.5 mass% salt loading, but similar amounts of halite were measured in the other CWF materials. The sodalite contents of all materials were similar. The halite content in the CWF source material used in the short-term heat-treatment study, which had the nominal salt and binder glass loadings, was determined to be about 1.3 mass% by standard addition analysis. Heat treatment had only a small effect on the phase composition: the amount of halite increased to as much as 3.7 mass%, and trace amounts of nepheline were detected in samples treated at 800 and 850 C. The CWF samples treated at high temperatures had lower amounts of halite detected in the rapid water-soluble test. The releases of B, Na, and Si in the product consistency tests (PCTs) were not sensitive to the heat-treatment conditions. The PCT responses of all salt-loaded and heat-treated CWF materials were well below that of the Environmental Assessment (EA) glass.