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Effects of soluble organic complexants and their degradation products on the removal of selected radionuclides from high-level waste. Part II: Distributions of Sr, Cs, Tc, and Am onto 32 absorbers from four variations of Hanford tank 101-SY simulant solution

Description: Many of the radioactive waste storage tanks at U.S. Department of Energy facilities contain organic compounds that have been degraded by radiolysis and chemical reactions during decades of storage. In this second part of our three-part investigation of the effects of soluble organic complexants and their degradation products, we measured the sorption of strontium, cesium, technetium, and americium onto 32 absorbers that offer high sorption of these elements in the absence of organic complexants. The four solutions tested were (1) a simulant for a 3:1 dilution of Hanford Tank 101-SY contents that initially contained ethylenediaminetetraacetic acid (EDTA), (2) this simulant after gamma-irradiation to 34 Mrads, (3) the unirradiated simulant after treatment with a hydrothermal organic-destruction process, and (4) the irradiated simulant after hydrothermal processing. For each of 512 element/absorber/solution combinations, we measured distribution coefficients (Kds) twice for each period for dynamic contact periods of 30 min, 2 h, and 6 h to obtain information about sorption kinetics. On the basis of our 3,072 measured Kd values, the sorption of strontium and americium is significantly decreased by the organic components of the simulant solutions, whereas the sorption of cesium and technetium appears unaffected by the organic components of the simulant solutions.
Date: April 1, 1995
Creator: Marsh, S.F.; Svitra, Z.V. & Bowen, S.M.
Partner: UNT Libraries Government Documents Department

Effects of soluble organic complexants and their degradation products on the removal of selected radionuclides from high-level waste. Part 3, Distributions of Sr, Cs, Tc, Pu, and Am onto 33 absorbers from four variations of a 3:1 dilution of Hanford complexant concentrate (CC) simulant: Part 4, The effects of varying dilution ratios on the distributions of Sr, Cs, Tc, Pu, and Am onto 12 absorbers

Description: Many of the radioactive waste storage tanks at USDOE facilities contain organic compounds that have been degraded by radiolysis and chemical reactions during decades of storage. Objective of this study was to measure effects of soluble organic complexants and their degradation products on sorption of Sr, Cs, Tc, Pu and Am onto 33 absorbers that in the absence of these organic compounds offer high sorption of these elements. The elements were in a generic simulant for Hanford complexant concentrate supernate that initially contained six organic complexants: EDTA, HEDTA, NTA, citrate, gluconate, and iminodiacetate. This simulant was tested as prepared and after gamma-irradiation to approximately 34 Mrads. Two other variations consisted of the unirradiated and irradiated simulants after treatment at 450C and 15,000 psi in a hydrothermal organic-destruction process. These experiments were conducted with a 3:1 water-to-simulant dilution of each of the four simulant variations. To determine effects of varying dilution ratios on the sorption of these five elements from the unirradiated and gamma-irradiated simulants that were not treated with the hydrothermal process, we measured their distribution from a 1:1 dilution, using 1 M NaOH as the diluent, onto the 12 best-performing absorbers. We then measured the sorption of these five elements from solutions having diluent-simulant ratios of 0, 0.5, 2.0, and 3.0 onto the three absorbers that performed best for sorbing Sr, Pu and Am from the 1:1 dilution. For each of 900 element/absorber/solution combinations, we measured distribution coefficients (Kd values) twice for each period for dynamic contact periods of 30 min, 2 h, and 6 h to obtain information about absorber stability and sorption kinetics. The 5400 measured Kd values indicate that the sorption of Sr, Pu, and Am is significantly decreased by the organic complexants in these simulant solutions, whereas the sorption of Cs and Tc is much ...
Date: September 1, 1995
Creator: Marsh, S.F.; Svitra, Z.V. & Bowen, S.M.
Partner: UNT Libraries Government Documents Department

Stabilization of Rocky Flats combustible residues contaminated with plutonium metal and organic solvents

Description: This report describes tests on a proposed flowsheet designed to stabilize combustible residues that were generated at the Rocky Flats Environmental Technology Site (RFETS) during the machining of plutonium metal. Combustible residues are essentially laboratory trash contaminated with halogenated organic solvents and plutonium metal. The proposed flowsheet, designed by RFETS, follows a glovebox procedure that includes (1) the sorting and shredding of materials, (2) a low temperature thermal desorption of solvents from the combustible materials, (3) an oxidation of plutonium metal with steam, and (4) packaging of the stabilized residues. The role of Los Alamos National Laboratory (LANL) in this study was to determine parameters for the low temperature thermal desorption and steam oxidation steps. Thermal desorption of carbon tetrachloride (CCl{sub 4}) was examined using a heated air stream on a Rocky Flats combustible residue surrogate contaminated with CCl{sub 4}. Three types of plutonium metal were oxidized with steam in a LANL glovebox to determine the effectiveness of this procedure for residue stabilization. The results from these LANL experiments are used to recommend parameters for the proposed RFETS stabilization flowsheet.
Date: September 30, 1998
Creator: Bowen, S.M.; Cisneros, M.R.; Jacobson, L.L.; Schroeder, N.C. & Ames, R.L.
Partner: UNT Libraries Government Documents Department