OFFGAS GENERATION FROM THE DISPOSITION OF SCRAP PLUTONIUM BY VITRIFICATION SIMULANT TESTS
The Department of Energy Office of Environmental Management is supporting R&D for the conceptual design of the Plutonium Disposition Project at the Savannah River Site in Aiken, SC to reduce the attractiveness of plutonium scrap by fabricating a durable plutonium oxide glass form and immobilizing this form within the high-level waste glass prepared in the Defense Waste Processing Facility. A glass formulation was developed that is capable of incorporating large amounts of actinides as well as accommodating many impurities that may be associated with impure Pu feed streams. The basis for the glass formulation was derived from commercial glasses that had high lanthanide loadings. A development effort led to a Lanthanide BoroSilicate (LaBS) glass that accommodated significant quantities of actinides, tolerated impurities associated with the actinide feed streams and could be processed using established melter technologies. A Cylindrical Induction Melter (CIM) was used for vitrification of the Pu LaBS glass. Induction melting for the immobilization of americium and curium (Am/Cm) in a glass matrix was first demonstrated in 1997. The induction melting system was developed to vitrify a non-radioactive Am/Cm simulant combined with a glass frit. Most of the development of the melter itself was completed as part of that work. This same melter system used for Am/Cm was used for the current work. The CIM system used consisted of a 5 inch (12.7 cm) diameter inductively heated platinum-rhodium (Pt-Rh) containment vessel with a control system and offgas characterization. Scrap plutonium can contain numerous impurities including significant amounts of chlorides, fluorides, sodium, potassium, lead, gallium, chromium, and nickel. Smaller amounts of additional elements can also be present. The amount of chlorides present is unusually high for a melter feed. In commercial applications there is no reason to have chloride at such high concentrations. Because the melter operates at 1400-1475 C, many of the impurities present are extremely volatile. An alternative being considered is to pre-treat the impure PuO{sub 2} by water washing to remove the soluble salts, which would significantly reduce the melter emissions. The disadvantage of the washing alternative is the criticality concerns of using water with plutonium. In this paper, the testing that has been conducted at the Savannah River National Laboratory (SRNL) to demonstrate induction melting of impure plutonium simulants will be described. The work described concentrates on quantification of the gaseous and particulate emissions from the induction melter. The Pt-Rh melter vessel is a cylinder with a conical bottom and a tubular drain as shown in Figure 1. A 5-inch (12.7 cm) diameter CIM was used for all of the emissions tests. A 6-inch (15.24 cm) diameter CIM, which is the size of the full-scale melter, has since been constructed for further testing. The 5-inch CIM is heated by three induction coils: one for the 5 inch cylinder, one for the conical section, and one for the 1/4-inch (6.35 mm) drain tube. The 6-inch CIM is similar except the cylinder heater extends lower and also heats the cone. The induction heating system is manufactured by Ameritherm{trademark}. The heating system is controlled by a PC to maintain a specific heat up profile and then maintain a constant energy input that maintains a constant temperature. The CIM is operated in batch mode where the plutonium simulant and the glass-forming frit are first thoroughly mixed in an attrittor mill, then added to the melter. Hafnium oxide (HfO{sub 2}) is used as a simulant for the radioactive PuO{sub 2}. The melter is heated until the mixture begins to melt at about 1100 C, then completely melts at about 1400-1450 C. This temperature is maintained for about three hours. While the temperature is maintained at {approx} 1400 C, an air bubbler is normally used to promote mixing of the glass-forming frit and the waste simulant.
- Research Organization:
- Savannah River Site (SRS), Aiken, SC (United States)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- DE-AC09-96SR18500
- OSTI ID:
- 925848
- Report Number(s):
- WSRC-STI-2007-00503; TRN: US0802471
- Resource Relation:
- Conference: International Conference on Thermal Treatment Technologies
- Country of Publication:
- United States
- Language:
- English
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