Defense Waste Processing Facility Glass Research Articles

Measured63Ni contents in Savannah River Site high level waste and Defense Waste Processing Facility glass product by Ni-selective ion exchange purification and β-decay counting

We describe tests of EiChrom Industries' Ni-selective ion exchange resin for use in analysis of63Ni in Savannah River Site high level waste. We report measurement of63Ni content in two sets of Savannah River Site glass product from the Defense Waste Processing Facility. The63Ni β-decay activity was chemically separated in quintuplicate from fission product and plutonium α-β activities of up to 103 times the observed63Ni content. The separation used a Ni-dimethlyglyoxime precipitation followed by radiochemical purification using the Ni-selective extraction chromatography resin. Further removal of interfering activity was based on diagnosis of observed radioactivity in each successive product phase. We analyzed eleven plant glass product samples using seven spiked standard addition duplicates to measure63Ni recovery in the separations. Selected liquid scintillation β-decay spectra are shown to validate the method. Interpretation of accuracy is based upon three distinct comparisions to predicted63Ni content.

Dissolution Rates of DWPF Glasses from Long-Term PCT

ABSTRACTWe have characterized the corrosion behavior of several Defense Waste Processing Facility (DWPF) reference waste glasses by conducting static dissolution tests with crushed glasses. Glass dissolution rates were calculated from measured B concentrations in tests conducted for up to five years. The dissolution rates of all glasses increased significantly after certain alteration phases precipitated. Calculation of the dissolution rates was complicated by the decrease in the available surface area as the glass dissolves. We took the loss of surface area into account by modeling the particles to be spheres, then extracting from the short-term test results the dissolution rate corresponding to a linear decrease in the radius of spherical particles. The measured extent of dissolution in tests conducted for longer times was less than predicted with this linear dissolution model. This indicates that advanced stages of corrosion are affected by another process besides dissolution, which we believe to be associated with a decrease in the precipitation rate of the alteration phases. These results show that the dissolution rate measured soon after the formation of certain alteration phases provides an upper limit for the long-term dissolution rate, and can be used to determine a bounding value for the source term for radionuclide release from waste glasses. The long-term dissolution rates measured in tests at 20,000 m−1 at 90°C in tuff groundwater at pH values near 12 are about 0.2,0.07, and 0.04 g/(m2•d) for the Environmental Assessment glass and glasses made with SRL 131 and SRL 202 frits, respectively.

The Release of Technetium from Defense Waste Processing Facility Glasses

AbstractLaboratory tests are being conducted using two radionuclide-doped Defense Waste Processing Facility (DWPF) glasses (referred to as SRL 131A and SRL 202A) to characterize the effects of the glass surface area/solution volume (SN) ratio on the release and disposition of Tc and several actinide elements. Tests are being conducted at 90°C in a tuff ground water solution at S/V ratios of 10, 2000, and 20,000 m−1 and have been completed through 1822 days. The formation of certain alteration phases in tests at 2000 and 20,000 m−1 results in an increase in the dissolution rates of both glasses. The release of Tc parallels that of B and Na under most test conditions and its release increases when alteration phases form. However, in tests with SRL 202A glass at 20,000 m−1, the Tc concentration in solution decreases coincidentally with an increase in the nitrite/nitrate ratio that indicates a decrease in the solution Eh. This may have occurred due to radiolysis, glass dissolution, the formation of alteration phases, or vessel interactions. Technetium that was reduced from Tc(VII) to Tc(IV) may have precipitated, though the amount of Tc was too low to detect any Tc-bearing phases. These results show the importance of conducting long-term tests with radioactive glasses to characterize the behavior of radionuclides, rather than relying on the observed behavior of nonradioactive surrogates.

Long-Term Results from Unsaturated Durability Testing of Actinide-Doped DWPF and WVDP Waste Glasses

AbstractResults from durability drip tests designed to simulate the unsaturated conditions in the proposed Yucca Mountain Repository are reported for two actinide-doped glasses used as model waste forms. These tests are being conducted with reference glass compositions doped with neptunium, plutonium, and americium from the Defense Waste Processing Facility (DWPF) and the West Valley Demonstration Project (WVDP), and have been ongoing for over 8 years. Solution compositions, including transuranics, have been periodically determined, and selected analyses of colloid formation and composition, glass corrosion layers, and solid alteration phases have been obtained by scanning and analytical transmission electron microscopies. The importance of integrated testing has been demonstrated, as complex interactions among the glass, the groundwater, and the sensitized stainless steel have been observed. The cumulative releases of both glassforming and dopant elements are presented along with identification of reaction phases and their partitioning between solution and solid phases. Alteration phases, including smectite clay, iron silicates, uranium silicates, and calcium thorium phosphate, have been observed forming on the glass and stainless steel and have occasionally been found suspended in solution as colloids. Actinides, except neptunium, concentrate into alteration phases or sorb onto the stainless steel. The subsequent transport of the actinides is then controlled by these phases.