Evaluation of Tritium Content and Release from Pressurized Water Reactor Fuel Cladding (2015)

It is expected that tritium pretreatment will be required in future reprocessing plants to prevent the release of tritium to the environment (except for long-cooled fuels). To design and operate future reprocessing plants in a safe and environmentally compliant manner, the amount and form of tritium in the used nuclear fuel (UNF) must be understood and quantified. Tritium in light water reactor (LWR) fuel is dispersed between the fuel matrix and the fuel cladding, and some tritium may be in the plenum, probably as tritium labelled water (THO) or T2O. In a standard processing flowsheet, tritium management would be accomplished by treatment of liquid streams within the plant. Pretreating the fuel prior to dissolution to release the tritium into a single off-gas stream could simplify tritium management, so the removal of tritium in the liquid streams throughout the plant may not be required. The fraction of tritium remaining in the cladding may be reduced as a result of tritium pretreatment. Since Zircaloy® cladding makes up roughly 25% by mass of UNF in the United States, processes are being considered to reduce the volume of reprocessing waste for Zircaloy® clad fuel by recovering the zirconium from the cladding for reuse. These recycle processes could release the tritium in the cladding. For Zircaloy-clad fuels from light water reactors, the tritium produced from ternary fission and other sources is expected to be divided between the fuel, where it is generated, and the cladding. It has been previously documented that a fraction of the tritium produced in uranium oxide fuel from LWRs can migrate and become trapped in the cladding. Estimates of the percentage of tritium in the cladding typically range from 0–96%. There is relatively limited data on how the tritium content of the cladding varies with burnup and fuel history (temperature, power, etc.) and how pretreatment impacts its release. To gain a better understanding of how tritium in cladding will behave during processing, scoping tests are being performed to determine the tritium content in the cladding pre- and post-tritium pretreatment. Samples of Surry-2 and H.B. Robinson pressurized water reactor cladding were heated to 1100–1200°C to oxidize the zirconium and release all of the tritium in the cladding sample. Cladding samples were also heated within the temperature range of 480–600ºC expected for standard air tritium pretreatment systems, and to a slightly higher temperature (700ºC) to determine the impact of tritium pretreatment on tritium release from the cladding. The tritium content of the Surry-2 and H.B. Robinson cladding was measured to be ~234 and ~500 µCi/g, respectively. Heating the Surry-2 cladding at 500°C for 24 h removed ~0.2% of the tritium from the cladding, and heating at 700°C for 24 h removed ~9%. Heating the H.B. Robinson cladding at 700°C for 24 h removed ~11% of the tritium. When samples of the Surry-2 and H.B. Robinson claddings were heated at 700°C for 96 h, essentially all of the tritium in the cladding was removed. However, only ~3% of the tritium was removed when a sample of Surry-2 cladding was heated at 600°C for 96 h. These data indicate that the amount of tritium released from tritium pretreatment systems will be dependent on both the operating temperature and length of time in the system. Under certain conditions, a significant fraction of the tritium could remain bound in the cladding and would need to be considered in operations involving cladding recycle.