Technetium Incorporation in Glass for the Hanford Tank Waste Treatment and Immobilization Plant
A priority of the United States Department of Energy (U.S. DOE) is to dispose of nuclear wastes accumulated in 177 underground tanks at the Hanford Nuclear Reservation in eastern Washington State. These nuclear wastes date from the Manhattan Project of World War II and from plutonium production during the Cold War. The DOE plans to separate high-level radioactive wastes from low activity wastes and to treat each of the waste streams by vitrification (immobilization of the nuclides in glass) for disposal. The immobilized low-activity waste will be disposed of here at Hanford and the immobilized high-level waste at the national geologic repository. Included in the inventory of highly radioactive wastes is large volumes of 99Tc (~9 × 10E2 TBq or ~2.5 × 104 Ci or ~1500 kg). A problem facing safe disposal of Tc-bearing wastes is the processing of waste feed into in a chemically durable waste form. Technetium incorporates poorly into silicate glass in traditional glass melting. It readily evaporates during melting of glass feeds and out of the molten glass, leading to a spectrum of high-to-low retention (ca. 20 to 80%) in the cooled glass product. DOE-ORP currently has a program at Pacific Northwest National Laboratory (PNNL), in the Department of Materials Science and Engineering at Rutgers University and in the School of Mechanical and Materials Engineering at Washington State University that seeks to understand aspects of Tc retention by means of studying Tc partitioning, molten salt formation, volatilization pathways, and cold cap chemistry. Another problem involves the stability of Tc in glass in both the national geologic repository and on-site disposal after it has been immobilized. The major environmental concern with 99Tc is its high mobility in addition to a long half-life (2.1×105 yrs). The pertechnetate ion (TcO4-) is highly soluble in water and does not adsorb well onto the surface of minerals and so migrates nearly at the same velocity as groundwater. Long-term corrosion of glass waste forms is an area of current interest to the DOE, but attention to the release of Tc from glass has been little explored. It is expected that the release of Tc from glass should be highly dependent on the local glass structure as well as the chemistry of the surrounding environment, including groundwater pH. Though the speciation of Tc in glass has been previously studied, and the Tc species present in waste glass have been previously reported, environmental Tc release mechanisms are poorly understood. The recent advances in Tc chemistry that have given rise to an understanding of incorporation in the glass giving rise to significantly higher single-pass retention during vitrification are presented. Additionally, possible changes to the baseline flowsheet that allow for relatively minor volumes of Tc reporting to secondary waste treatment will be discussed.
- Research Organization:
- Hanford Site (HNF), Richland, WA (United States)
- Sponsoring Organization:
- USDOE Office of Environmental Management (EM)
- Contributing Organization:
- Department of Energy - Office of River Protection, Pacific Northwest National Laboratory
- DOE Contract Number:
- DE-AC27-08RV14800
- OSTI ID:
- 1167469
- Report Number(s):
- ORP-58131-FP Rev 0
- Resource Relation:
- Conference: WM2015 Waste Management Symposia 03/15/2015 - 03/19/2015 Phoenix, AZ
- Country of Publication:
- United States
- Language:
- English
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