Methods to Capture the Tritium Released by Recovery/Recycle of Zirconium from Used Fuel Cladding: A Review
After uranium, the second largest mass contained in most used nuclear fuel (UNF) is the zirconium-based Zircaloy{sup R} cladding in the fuel cladding which accounts for about 25% of the mass. In current practice, the cladding requires disposal in a geologic repository. Zirconium may be recovered from the Zircaloy cladding of UNF for recycle. Alternatively, it may be decontaminated to recategorize it as low-level waste. Either approach reduces the quantities of high-level waste destined for a geologic repository, thereby reducing the overall cost of recycling UNF. Process development studies are under way in the United States and Republic of Korea based on dry chlorination using a mixture of chlorine (Cl{sub 2}) and an inert carrier such as argon (Ar) to convert the zirconium in the alloy, which is greater than 98 wt% of the alloy mass, to zirconium tetrachloride (ZrCl{sub 4}). The ZrCl{sub 4} is volatile and is easily separated from the non-volatile components. The residues include non-volatile chlorides such as CrCl{sub 3}, oxychlorides and oxides. The product ZrCl{sub 4} is recovered as a solid salt by condensation when cooled to less than about 300 deg. C. Feasibility tests with actual UNF cladding have demonstrated that the recovered zirconium chloride salt is sufficiently separated from fuel and fission product radionuclides that it emanates no significant dose and can be handled without shielding. Several methods for capturing tritium released from cladding during the chlorination process have been identified. A detailed description of the methodologies, advantages, drawbacks, and conceptual flowsheets will be presented. (authors)