A Brief Review of Past INL Work Assessing Radionuclide Content in TMI-2 Melted Fuel Debris: The Use of 144 Ce as a Surrogate for Pu Accountancy
This report serves as a literature review of prior work performed at Idaho National Laboratory, and its predecessor organizations Idaho National Engineering Laboratory (INEL) and Idaho National Engineering and Environmental Laboratory (INEEL), studying radionuclide partitioning within the melted fuel debris of the reactor of the Three Mile Island 2 (TMI-2) nuclear power plant. The purpose of this review is to document prior published work that provides supporting evidence of the utility of using 144 Ce as a surrogate for plutonium within melted fuel debris. When the TMI-2 accident occurred no quantitative nondestructive analysis (NDA) techniques existed that could assay plutonium in the unconventional wastes from the reactor. However, unpublished work performed at INL by D. W. Akers in the late 1980s through the 1990s demonstrated that passive gamma-ray spectrometry of 144 Ce could potentially be used to develop a semi-quantitative correlation for estimating plutonium content in these materials. The fate and transport of radioisotopes in fuel from different regions of the core, including uranium, fission products, and actinides, appear to be well characterized based on the maximum temperature reached by fuel in different parts of the core and the melting point, boiling point, and volatility of those radioisotopes. Also, the chemical interactions between fuel, fuel cladding, control elements, and core structural components appears to have played a large role in determining when and how fuel relocation occurred in the core; perhaps the most important of these reaction appears to be related to the formation of mixed-material alloys, eutectics, in the fuel cladding. Because of its high melting point, low volatility, and similar chemical behavior to plutonium, the element cerium appears to have behaved similarly to plutonium during the evolution of the TMI-2 accident. Anecdotal evidence extrapolated from open-source literature strengthens this logical feasibility for using cerium, which is rather easy to analyze using passive nondestructive analysis gamma-ray spectrometry, as a surrogate for plutonium in the final analysis of TMI-2 melted fuel debris. The generation of this report is motivated by the need to perform nuclear material accountancy measurements on the melted fuel debris that will be excavated from the damaged nuclear reactors at the Fukushima Daiichi nuclear power plant in Japan, which were destroyed by the Tohoku earthquake and tsunami on March 11, 2011. Lessons may be taken from prior U.S. work related to the study of the TMI-2 core debris to support the development of new assay methods for use at Fukushima Daiichi. While significant differences exist between the two reactor systems (pressurized water reactor (TMI-2) versus boiling water reactor (FD), fresh water post-accident cooing (TMI-2) versus salt water (FD), maintained containment (TMI-2) versus loss of containment (FD)) there remain sufficient similarities to motivate these comparisons.