Estimation of Carbon 14 Inventory in Hull and End-Piece Wastes From Japanese Commercial Reprocessing Operation

Abstract

Hull and end-piece wastes generated from reprocessing plant operations are expected to be disposed of in a deep underground repository as Group 2 TRU wastes under the Japanese classification system. The activated metals that compose the spent fuel assemblies such as Zircaloy claddings and stainless steel nozzles are mixed and compressed after fuel dissolution, and then stuffed into stainless steel canisters. Carbon 14 is a typical activated product in the hulls and end-pieces and is mainly generated by the 14N(n,p)14C reaction. In the previous safety assessment of the TRU waste in Japan, the radionuclides inventory was calculated by ORIGEN-2 code. Some conservative assumptions and preliminary estimates were used in this calculation. For example, total radionuclides generated from a single type of fuel assembly (45 GWd/tU for a PWR unit), and the thickness of the Zircaloy oxide film on the hulls (80 μm) were both overestimated. The second assumption in particular has a large effect on exposure dose evaluation. Therefore, it is essential to have a realistic source term evaluation regarding such items as the C-14 inventory and its distribution to waste parts. In the present study, a C-14 inventory of the hull and end-piece wastes from the operation of a commercial reprocessing plant in Japan corresponding to 32,000 tU (16,000 tU in each BWR and PWR) was calculated. Analysis using individual irradiation conditions and fuel characteristics was conducted on 6 types of fuel assemblies for BWRs and 12 types for PWRs (4 pile types × 3 burnup limits). The oxide film thickness data for each fuel type cladding were obtained from the published literature. Activation calculations were performed by using ORIGEN-2 code. For the amount of spent assembly and other waste characteristics, representative values were assumed based on the published literature. As a preliminary experiment, C-14 in irradiated BWR claddings was measured and found to be consistent with the calculated activation. The total C-14 inventory was estimated as 4.46×1014 Bq, consisting of 2.58×1014 Bq for BWRs and 1.87×1014 Bq for PWRs, and is consistent with the safety assessment of 4.4×1014 Bq. However, the distribution of the C-14 inventory to hull oxide, which was estimated under the assumption of instantaneous radionuclide release in the safety assessment, decreased from 5.72×1013 Bq (13% of the total) in the previous assessment to 1.30×1013 Bq (2.9% of the total; consisting of 1.48×1012 for BWRs and 1.15×1013 for PWRs). In other words, the exposure dose peak is reduced to approximate 25% of its previous value due to the use of detailed oxide film data that the BWR cladding has a thin oxide film. Other instantaneous release components for C-14 such as the fuel residual were negligible.

C-14 Release Behavior and Chemical Species from Irradiated Hull Waste under Geological Disposal Conditions

“…Regarding the C-14 inventory, Sakuragi et.al. have reported the total amount and concentration of C-14 in various kinds of metal waste [1]. Although it is assumed that the C-14 release behavior is related with metal corrosion, there are few studies that considered the relationship over a long period of time.…”