AGR-3/4 Experiment Preliminary Mass Balance (2018)

AGR-3/4 was an experiment primarily aimed at studying fission product transport in graphite and graphitic materials. To accomplish this, 80 designed-to-fail (DTF) particles coated only with a thin pyrocarbon layer were incorporated among the roughly 7500 tristructural isotropic-coated driver fuel particles in each capsule. It was anticipated that intact DTF particles would behave like TRISO particles with SiC layer failures (releasing cesium and other metallic fission products to some extent, but retaining fission gases), and failed DTF particles would behave like TRISO particles with failed TRISO coatings (releasing both cesium and other metallic fission products and fission gases). The DTF particles provided a known source of fission products to migrate out into the fuel compact matrix and out into the surrounding concentric rings of graphite and graphitic matrix material for study. Post-irradiation examinations have focused on measuring the total releases of fission products from the fuel compacts (mass balance) and the spatial distribution of fission products in the rings. The total mass balance is an important parameter for comparison to fission product transport simulations of the AGR-3/4 experiment, and the spatial distribution within carbon rings is being used to derive fission product diffusion coefficients. To determine the fission product mass balance, each of the 12 irradiation capsules was disassembled, and their component parts analyzed via gamma counting and destructive leach or burn-leach methods. In “standard” capsules (Capsules 1, 3-5, 7-8, 10, and 12), inner rings, outer rings, sink rings, spacers, foils, felts, and through tubes were all analyzed for gamma-emitting fission products. Beta-emitting Sr-90 was measured as well, but because of the analysis program on the inner and outer rings, the Sr-90 inventory of the inner and outer rings is not yet available. “Fuel body” Capsules 2, 6, 9, and 11 were retained intact for future heating tests; thus, the inner and outer rings from these capsules were not measured. The most commonly detected radionuclide fission products were Ag-110m, Cs-134, Cs-137, Eu-154, Eu-155, and Sr-90. Sb-125 was also frequently detected in the sink rings and spacers; however, the zircaloy spacers used in Capsules 1 through 6 contained natural antimony that transmuted to Sb-125 and made it impossible to separate Sb-125 released from the fuel from that generated in the spacers. Summing the fission product inventory measured on each capsule component made it clear that the presence of 80 DTF particles in each capsule resulted in noticeably higher releases of cesium, europium, and strontium from AGR-3/4 fuel when compared to AGR-1 fuel which did not have DTF particles. Greater than 30 particles worth of Cs-134 was measured outside of the fuel compacts in Capsules 3-5, 7, 8, and 10. In Capsule 11 (an intact fuel body for which the inner and outer rings were not measured), 26 particle equivalents of Cs-134 was measured outside of the outer ring. Based on experience from AGR 1, it is very unlikely that any driver particles failed during the irradiation; therefore, this cesium is assumed to be overwhelmingly dominated by release from DTF particles.