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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

Distributions of 15 elements on 58 absorbers from simulated Hanford Double-Shell Slurry Feed (DSSF)

Description: As part of the Hanford Tank Waste Remediation System program at Los Alamos, we evaluated 58 commercially available or experimental absorber materials for their ability to remove hazardous components from high-level waste. These absorbers included cation and anion exchange resins, inorganic exchangers, composite absorbers, pillared layered materials, and a series of liquid extractants sorbed on porous support-beads. We tested these absorbers with a solution that simulates Hanford double-shell slurry feed (DSSF) (pH 14.0). To this simulant solution we added the appropriate radionuclides and used gamma spectrometry to measure fission products (Ce, Cs, Sr, Tc, and Y), actinides (U and Am), and matrix elements (Cr, Co, Fe, Mn, Ni, V, Zn, and Zr). For each of 870 element/absorber combinations, we measured distribution coefficients for dynamic contact periods of 30 min, 2 h, and 6 h to obtain information about sorption kinetics. On the basis of these 2610 measured distribution coefficients, we determined that many of the tested absorbers may be suitable for processing DSSF solutions.
Date: November 1, 1994
Creator: Marsh, S. F.; Svitra, Z. V. & Bowen, S. M.
Partner: UNT Libraries Government Documents Department

Distributions of 14 elements into 10 liquid extractants from simulated acid-dissolved sludge and acidified supernate solutions of Hanford high-level waste

Description: The distributions of 14 elements into ten extractants were measured from simulant solutions that represent acidic dissolved sludge and acidified supernate from Hanford HLW Tank 102-SY. The extractants: LIX{sup TM}-26, LIX{sup TM}-54, LIX{sup TM}-84, LIX{sup TM}-1010, Cyanex{sup TM} 272, Cyanex{sup TM} 923, Aliquat{sup TM} 336, DHDECMP, DHDECMP-DIPB, and CMPO-DIPB, were sorbed on porous carbon beads to provide dry-appearing beads that would be suitable for column operations. The selected elements, which represent fission products: Ce, Cs, Sr, Tc, and Y; actinides: U, Pu, and Am; and matrix elements: Cr, Co, Fe, Mn, Zn, and Zr; were traced by radionuclides and measured by gamma spectrometry. Distribution coefficients for each of 280 element/absorber/solution combinations were measured for dynamic contact periods of 30 minutes, 2 hours, and 6 hours to provide sorption kinetics information for the selected elements from these complex media. The resulting 840 measured distribution coefficients are presented.
Date: February 1, 1994
Creator: Marsh, S. F.; Svitra, Z. V. & Bowen, S. M.
Partner: UNT Libraries Government Documents Department

Distributions of 14 elements on 60 selected absorbers from two simulant solutions (acid-dissolved sludge and alkaline supernate) for Hanford HLW Tank 102-SY

Description: Sixty commercially available or experimental absorber materials were evaluated for partitioning high-level radioactive waste. These absorbers included cation and anion exchange resins, inorganic exchangers, composite absorbers, and a series of liquid extractants sorbed on porous support-beads. The distributions of 14 elements onto each absorber were measured from simulated solutions that represent acid-dissolved sludge and alkaline supernate solutions from Hanford high-level waste (HLW) Tank 102-SY. The selected elements, which represent fission products (Ce, Cs, Sr, Tc, and Y); actinides (U, Pu, and Am); and matrix elements (Cr, Co, Fe, Mn, Zn, and Zr), were traced by radionuclides and assayed by gamma spectrometry. Distribution coefficients for each of the 1680 element/absorber/solution combinations were measured for dynamic contact periods of 30 min, 2 h, and 6 h to provide sorption kinetics information for the specified elements from these complex media. More than 5000 measured distribution coefficients are tabulated.
Date: October 1, 1993
Creator: Marsh, S. F.; Svitra, Z. V. & Bowen, S. M.
Partner: UNT Libraries Government Documents Department

Distributions of 12 elements on 64 absorbers from simulated Hanford Neutralized Current Acid Waste (NCAW)

Description: As part of the Hanford Tank Waste Remediation System program at Los Alamos, we evaluated 64 commercially available or experimental absorber materials for their ability to remove hazardous components from high-level waste. These absorbers included cation and anion exchange resins, inorganic exchangers, composite absorbers, and a series of liquid extractants sorbed on porous support-beads. We tested these absorbers with a solution that simulates Hanford neutralized current acid waste (NCAW) (pH 14.2). To this simulant solution we added the appropriate radionuclides and used gamma spectrometry to measure fission products (Cs, Sr, Tc, and Y) and matrix elements (Cr, Co, Fe, Mn, Ni, V, Zn, and Zr). For each of 768 element/absorber combinations, we measured distribution coefficients for dynamic contact periods of 30 min, 2 h, and 6 h to obtain information about sorption kinetics. On the basis of these 2304 measured distribution coefficients, we determined that many of the tested absorbers may be suitable for processing NCAW solutions.
Date: December 1, 1994
Creator: Svitra, Z. V.; Bowen, S. M. & Marsh, S. F.
Partner: UNT Libraries Government Documents Department

Effects of aqueous-soluble organic compounds on the removal of selected radionuclides from high-level waste part I: Distribution of Sr, Cs, and Tc onto 18 absorbers from an irradiated, organic-containing leachate simulant for Hanford Tank 101-SY

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. In this investigation, we measured the effect of some aqueous-soluble organic compounds on the sorption of strontium, cesium, and technetium onto 18 absorbers that offer high sorption of strontium from organic-free solutions. For our test solution we used a leachate from a simulated slurry for Hanford Tank 101-SY that initially contained ethylenediaminetetraacetic acid (EDTA) and then was gamma-irradiated to 34 Mrads. We measured distribution coefficients (Kds) for each element/absorber combination for dynamic contact periods of 30 min, 2 h, and 6 h to obtain information about sorption kinetics. To facilitate comparisons, we include Kd values for these same element/absorber combinations from three organic-free simulant solutions. The Kd values for strontium sorption from the simulant that contained the degraded organics usually decreased by large factors, whereas the Kd values for cesium and technetium sorption were relatively unaffected.
Date: January 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