Corrosion tests to determine temperature and pH dependencies of the dissolution rates of sodalite, binder glass, and ceramic waste form.

Jeong, S.-Y. ; Fanning, T. H. ; Morss, L. R. ; Ebert, W. L.

Argonne National Laboratory

关键词: Corrosion;    Flow Rate;    Specific Surface Area;    Binders;    Waste Forms;   

DOI  :  10.2172/808425
RP-ID  :  ANL-02/32
RP-ID  :  W-31-109-ENG-38
RP-ID  :  808425

美国|英语

来源: UNT Digital Library

【 摘 要 】

A glass bonded-sodalite ceramic waste form (CWF) has been developed to immobilize salt wastes from electrometallurgical treatment of sodium-bonded spent nuclear fuel. The CWF is a composite of salt-loaded sodalite and a binder glass formed at high temperature (850-950 C) by hot isostatic pressing (HIP) or pressureless-consolidation (PC) processes. A waste form degradation and radionuclide release model has been developed to support qualification of the CWF for disposal in the proposed repository at Yucca Mountain. Six series of tests were conducted in conjunction with the development of that model. (1) Static tests were conducted to measure the dissolution rate of sodalite, HIP binder glass, and HIP CWF at 40, 70, and 90 C in pH range 4.8-9.8 buffer solution. The parameter values in the degradation model were calculated from the dissolution rates measured by the static tests. (2) Static tests were conducted at 70 C in noncomplexing tertiary amine pH buffers to confirm that the dissolution rate measured with traditional buffers was not affected by the complexation of metal ions. The results showed that the difference between dissolution rate determined with noncomplexing buffer and that determined with traditional buffers was negligible. (3) Static tests were conducted in five buffer solutions in the pH range 4.8-9.8 at 20 C with HIP sodalite, HIP glass, and HIP CWF. The results showed that the model adequately predicts the dissolution rate of these materials at 20 C. (4) Static tests at 20 and 70 C with CWF made by the PC process indicated that the model parameters extracted from the results of tests with HIP CWF could be applied to PC CWF. (5) The dissolution rates of a modified glass made with a composition corresponding to 80 wt% glass and 20 wt% sodalite were measured at 70 C to evaluate the sensitivity of the rate to the composition of binder glass in the CWF. The dissolution rates of the modified binder glass were indistinguishable from the rates of the binder glass. (6) The dissolution rate of a simple five-component glass (CSG) was measured at 70 C using static tests and single-pass flow-through (SPFT) tests. Rates were similar for the two methods; however, the measured rates are about 10X higher than the rates measured previously at Lawrence Livermore National Laboratory (LLNL) for a glass having the same composition using an SPFT test method. Differences are attributed to effects of the solution flow rate on the glass dissolution rate and how the specific surface area of crushed glass is estimated. This comparison indicates the need to standardize the SPFT test procedure.