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Characterization of Group V Dubnium Homologs on DGA Extraction Chromatography Resin from Nitric and Hydrofluoric Acid Matrices

Description: Studies of the chemical properties of superheavy elements (SHE) pose interesting challenges due to their short half-lives and low production rates. Chemical systems must have extremely fast kinetics, fast enough kinetics to be able to examine the chemical properties of interest before the SHE decays to another nuclide. To achieve chemistry on such time scales, the chemical system must also be easily automated. Most importantly however, a chemical system must be developed which provides suitable separation and kinetics before an on-line study of a SHE can be performed. Relativistic effects make studying the chemical properties of SHEs interesting due to the impact these effects could have on the SHEs chemical properties. Relativistic effects arise when the velocity of the s orbital electrons approach the speed of light. As this velocity increases, the Bohr radius of the inner electron orbitals decreases and there is an increase in the particles mass. This contraction results in a destabilization of the energy of the outer d and f electron orbitals (5f and 6d in the case of SHE), which can cause these to expand due to their increased shielding from the nuclear charge. Another relativistic effect is the spin-orbit splitting for p, d, and f orbitals into j = 1 {+-} 1/2 states. This can lead most interestingly to a possible increased stability of element 114, which due to large spin-orbit splitting of the 7p orbital and the relativistically stabilized 7p{sub 1/2} and 7s orbital gives rise to a closed shell ground state of 7s{sup 2}7p{sub 1/2}{sup 2}. The homologs of element 105, dubnium (Db), Ta and Nb and the pseudo-homolog Pa, are well known to hydrolyze and form both neutral and non-neutral monoatomic and polyatomic species that may cause issues with extraction from a given chemical system. Early ion-exchange and solvent-extraction studies show ...
Date: February 21, 2012
Creator: Despotopulos, J D & Sudowe, R
Partner: UNT Libraries Government Documents Department

Calculation of Transactinide Homolog Isotope Production Reactions Possible with the Center for Accelerator Mass Spectrometry (CAMS) at Lawrence Livermore National Laboratory

Description: The LLNL heavy element group has been investigating the chemical properties of the heaviest elements over the past several years. The properties of the transactinides (elements with Z > 103) are often unknown due to their low production rates and short half-lives, which require lengthy cyclotron irradiations in order to make enough atoms for statistically significant evaluations of their chemistry. In addition, automated chemical methods are often required to perform consistent and rapid chemical separations on the order of minutes for the duration of the experiment, which can last from weeks to months. Separation methods can include extraction chromatography, liquid-liquid extraction, or gas-phase chromatography. Before a lengthy transactinide experiment can be performed at an accelerator, a large amount of preparatory work must be done both to ensure the successful application of the chosen chemical system to the transactinide chemistry problem being addressed, and to evaluate the behavior of the lighter elemental homologs in the same chemical system. Since transactinide chemistry is literally performed on one single atom, its chemical properties cannot be determined from bulk chemical matrices, but instead must be inferred from the behavior of the lighter elements that occur in its chemical group and in those of its neighboring elements. By first studying the lighter group homologs in a particular chemical system, when the same system is applied to the transactinide element under investigation, its decay properties can be directly compared to those of the homologues, thereby allowing an inference of its own chemistry. The Center for Accelerator Mass Spectrometry (CAMS) at Lawrence Livermore National Laboratory (LLNL) includes a 1 MV Tandem accelerator, capable of accelerating light ions such as protons to energies of roughly 15 MeV. By using the CAMS beamline, tracers of transactinide homolog elements can be produced both for development of chemical systems and for ...
Date: November 29, 2011
Creator: Moody, K J; Shaughnessy, D A & Gostic, J M
Partner: UNT Libraries Government Documents Department

Rapid Determination of 237 Np and Pu Isotopes in Water by Inductively Coupled Plasma Mass Spectrometry and Alpha Spectrometry

Description: A new method that allows rapid preconcentration and separation of plutonium and neptunium in water samples was developed for the measurement of {sup 237}Np and Pu isotopes by inductively-coupled plasma mass spectrometry (ICP-MS) and alpha spectrometry; a hybrid approach. {sup 238}U can interfere with {sup 239}Pu measurement by ICP-MS as {sup 238}UH{sup +} mass overlap and {sup 237}Np via peak tailing. The method provide enhanced removal of uranium by separating Pu and Np initially on TEVA Resin, then moving Pu to DGA resin for additional removal of uranium. The decontamination factor for uranium from Pu is almost 100,000 and the decontamination factor for U from Np is greater than 10,000. This method uses stacked extraction chromatography cartridges and vacuum box technology to facilitate rapid separations. Preconcentration is performed using a streamlined calcium phosphate precipitation method. Purified solutions are split between ICP-MS and alpha spectrometry so that long and short-lived Pu isotopes can be measured successfully. The method allows for simultaneous extraction of 20 samples (including QC samples) in 4 to 6 hours, and can also be used for emergency response. {sup 239}Pu, {sup 242}Pu and {sup 237}Np were measured by ICP-MS, while {sup 236}Pu, {sup 238}Pu, and {sup 239}Pu were measured by alpha spectrometry.
Date: June 23, 2010
Creator: Maxwell, S.; Jones, V.; Culligan, B.; Nichols, S. & Noyes, G.
Partner: UNT Libraries Government Documents Department

RAPID DETERMINATION OF ACTINIDES IN URINE BY INDUCTIVELY-COUPLED PLASMA MASS SPECTROMETRY AND ALPHA SPECTROMETRY: A HYBRID APPROACH

Description: A new rapid separation method that allows separation and preconcentration of actinides in urine samples was developed for the measurement of longer lived actinides by inductively coupled plasma mass spectrometry (ICP-MS) and short-lived actinides by alpha spectrometry; a hybrid approach. This method uses stacked extraction chromatography cartridges and vacuum box technology to facilitate rapid separations. Preconcentration, if required, is performed using a streamlined calcium phosphate precipitation. Similar technology has been applied to separate actinides prior to measurement by alpha spectrometry, but this new method has been developed with elution reagents now compatible with ICP-MS as well. Purified solutions are split between ICP-MS and alpha spectrometry so that long- and short-lived actinide isotopes can be measured successfully. The method allows for simultaneous extraction of 24 samples (including QC samples) in less than 3 h. Simultaneous sample preparation can offer significant time savings over sequential sample preparation. For example, sequential sample preparation of 24 samples taking just 15 min each requires 6 h to complete. The simplicity and speed of this new method makes it attractive for radiological emergency response. If preconcentration is applied, the method is applicable to larger sample aliquots for occupational exposures as well. The chemical recoveries are typically greater than 90%, in contrast to other reported methods using flow injection separation techniques for urine samples where plutonium yields were 70-80%. This method allows measurement of both long-lived and short-lived actinide isotopes. 239Pu, 242Pu, 237Np, 243Am, 234U, 235U and 238U were measured by ICP-MS, while 236Pu, 238Pu, 239Pu, 241Am, 243Am and 244Cm were measured by alpha spectrometry. The method can also be adapted so that the separation of uranium isotopes for assay is not required, if uranium assay by direct dilution of the urine sample is preferred instead. Multiple vacuum box locations may be set-up to supply several ICP-MS ...
Date: May 27, 2009
Creator: Maxwell, S. & Jones, V.
Partner: UNT Libraries Government Documents Department

Separation of Lanthanide Ions with Kläui Ligand Resin

Description: Separation and pre-concentration of the desired analyte is often a critical step in many radioanalytical methods. Current procedures for separating and concentrating analytes for detection are complex, and can be both expensive and time consuming. Therefore, the purpose of this research is to develop an alternative method of separating lanthanide ions through the use of an extraction chromatography resin containing a Klaui ligand salt. This research is a continuation of a concerted effort to develop new methods of detecting small concentrations of radionuclides and lanthanides using Klaui ligands. The Klaui ligands, C5Me5Co(OP(OR)2)3- (R=Me, Et, n-Pr) (LOR-), have unique affinity for lanthanide and actinide ions in the presence of competing metal ions. The use of 1 wt% NaLOR (R=Et or n-Pr) adsorbed onto resin support has been shown to extract lanthanide ions from aqueous nitric acid solutions of different concentrations. In order to further evaluate the utility of these materials in radiochemical separation, the selectivity of the resins for the different lanthanide ions was examined by measuring the distribution coefficients (Kd) for a series of lanthanides over a range of solution conditions. Based on prior research with actinide ions, it was hypothesized that the lanthanide ions would bond strongly with the Klaui ligands. The success of this research is important, because it will assist in expanding and improving current automated radiochemical methods, which will decrease the cost of developing and implementing radiochemical methods. To date, Kd values have been determined for Eu+3, Nd+3 and Pr+3 under varying nitric acid (HNO3) concentration, using a resin consisting of 1.0 wt% NaLOPr on Amberlite XAD-7HP. The dependence of the Kd values for Eu+3 has also been examined as a function of the ligand-to-europium ratio and the nitrate concentration. Decreasing Kd values were obtained upon increasing the nitric acid concentration, indicating protonation of the ligand, ...
Date: July 1, 2007
Creator: Granger, Trinity D.; Henry, Victoria A. & Latesky, Stanley
Partner: UNT Libraries Government Documents Department

NEW METHOD FOR DETERMINATION OF ACTINIDES AND STRONTIUM IN ANIMAL TISSUE

Description: The analysis of actinides in animal tissue samples is very important for environmental monitoring. There is a need to measure actinide isotopes with very low detection limits in animal tissue samples, including fish, deer, hogs, beef and shellfish. A new, rapid actinide separation method has been developed and implemented that allows the measurement of plutonium, neptunium, uranium, americium, curium and strontium isotopes in large animal tissue samples (100-200 g) with high chemical recoveries and effective removal of matrix interferences. This method uses stacked TEVA Resin{reg_sign}, TRU Resin{reg_sign} and DGA-Resin{reg_sign} cartridges from Eichrom Technologies (Darien, IL, USA) that allows the rapid separation of plutonium (Pu), neptunium (Np), uranium (U), americium (Am), and curium (Cm) using a single multi-stage column combined with alpha spectrometry. Sr-90 is collected on Sr Resin{reg_sign} from Eichrom Technologies (Darien, IL, USA). After acid digestion and furnace heating of the animal tissue samples, the actinides and Sr-89/90 are separated using column extraction chromatography. This method has been shown to be effective over a wide range of animal tissue matrices. By using vacuum box cartridge technology with rapid flow rates, sample preparation time is minimized.
Date: May 7, 2007
Creator: Maxwell, S; Jay Hutchison, J & Don Faison, D
Partner: UNT Libraries Government Documents Department

RAPID METHOD FOR PLUTONIUM, AMERICIUM AND CURIUM IN VERY LARGE SOIL SAMPLES

Description: The analysis of actinides in environmental soil and sediment samples is very important for environmental monitoring. There is a need to measure actinide isotopes with very low detection limits. A new, rapid actinide separation method has been developed and implemented that allows the measurement of plutonium, americium and curium isotopes in very large soil samples (100-200 g) with high chemical recoveries and effective removal of matrix interferences. This method uses stacked TEVA Resin{reg_sign}, TRU Resin{reg_sign} and DGA-Resin{reg_sign} cartridges from Eichrom Technologies (Darien, IL, USA) that allows the rapid separation of plutonium (Pu), americium (Am), and curium (Cm) using a single multistage column combined with alpha spectrometry. The method combines an acid leach step and innovative matrix removal using cerium fluoride precipitation to remove the difficult soil matrix. This method is unique in that it provides high tracer recoveries and effective removal of interferences with small extraction chromatography columns instead of large ion exchange resin columns that generate large amounts of acid waste. By using vacuum box cartridge technology with rapid flow rates, sample preparation time is minimized.
Date: January 8, 2007
Creator: Maxwell, S
Partner: UNT Libraries Government Documents Department

Selective Media for Actinide Collection and Pre-Concentration: Results of FY 2006 Studies

Description: In this work, we have investigated new materials for potential use in automated radiochemical separations. The work can be divided into three primary tasks: (1) synthesis of new ligands with high affinity for actinide ions, (2) evaluation of new materials for actinide ion affinity, and (3) computational design of advanced ligand architectures for highly selective binding of actinide ions. Ligand Synthesis Work was conducted on synthesizing Kl?ui ligand derivatives containing functionalized pendant groups on the cyclopentadienyl ring. The functionalized pendent groups would allow these ligands to be attached to organic and inorganic solid supports. This work focused on synthesizing the compound Na[Cp?Co(PO(OC2H5)2)3], where Cp?= C5H4C(O)OCH3. Synthesizing this compound is feasible, but the method used in FY 2006 produced an impure material. A modified synthetic scheme has been developed and will be pursued in FY 2007. Work was also initiated on synthesizing bicyclic diamides functionalized for binding to polymeric resins or other surfaces. Researchers at the University of Oregon are collaborators in this work. To date, this effort has focused on synthesizing and characterizing a symmetrically substituted bicyclic diamide ligand with the ?COOH functionality. Again, this synthetic effort will continue into FY 2007. Separations Material Evaluation Work was conducted in FY 2006 to provide a more extensive set of data on the selectivity and affinity of extraction chromatography resins prepared by sorption of Kl?ui ligand onto an inert macroreticular polymeric support. Consistent with previous observations, it was found that these materials strongly bind tetravalent actinides. These materials also adsorb trivalent actinides at low nitric acid concentrations, but the affinity for the trivalent actinides decreases with increasing nitric acid concentration. These materials have relatively low affinity for U(VI), but they do sorb U(VI) to a greater extent than Am(III) at [HNO3] > 0.3 M. Preliminary results suggest that the Kl?ui resins can ...
Date: November 17, 2006
Creator: Lumetta, Gregg J.; Addleman, Raymond S.; Hay, Benjamin P.; Hubler, Timothy L.; Levitskaia, Tatiana G.; Sinkov, Sergey I. et al.
Partner: UNT Libraries Government Documents Department

Chemical Treatment of US Department of Energy High Level and Low Level Waste to Obtain a Pure Radiochemical Fraction for Determination of Californium Alpha-Decay Content

Description: We have developed a chemical separation technique that allows the radiochemical determination of the californium a-decay content in Department of Energy (DOE) high level wastes from the Hanford and Savannah River sites. The chemical separation technique uses a series of column extraction chromatography steps that use Eichrom Industries' lanthanide and actinide plus 3 oxidation state selective Ln-resin(R) and the transuranic selective plus 4 oxidation state TRU-resin(R) to obtain intermediate product phases in dilute nitric acid. The technique has been demonstrated on three types of authentic DOE high and low level waste samples. We obtain discrimination from Pu a-activity by a factor of over 200 and from Cm-244 a-activity by a factor approaching 1700. Californium recoveries are measured by addition of a Cf-249 spike and are in the range of 50 percent to 90 percent in the synthetic samples and are in the range of 1.4 percent to 48 percent for the authentic DOE waste samples.
Date: December 2, 2002
Creator: Dewberry, R.
Partner: UNT Libraries Government Documents Department

On-Line/At-Line Technetium Monitor Using Scintillating Ion Exchange Resins for the Savannah River Site

Description: The results of this study indicate that the combination of extraction chromatography and on-line flow-cell scintillation counting can exceed a 99Tc detection limit of 0.005 Ci/mL in the presence of 90Sr, 137Cs, and 239Pu in less than an 18 minute analysis time.
Date: August 30, 2000
Creator: Wach, S.T.
Partner: UNT Libraries Government Documents Department

AMERICIUM SEPARATIONS FROM NITRIC ACID PROCESS EFFLUENT STREAMS

Description: The aging of the US nuclear stockpile presents a number of challenges, including the ever-increasing radioactivity of plutonium residues from {sup 241}Am. Minimization of this weak gamma-emitter in process and waste solutions is desirable to reduce both worker exposure and the effects of radiolysis on the final waste product. Removal of americium from plutonium nitric acid processing effluents, however, is complicated by the presence of large.quantities of competing metals, particularly Fe and Al, and-strongly oxidizing acidic solutions. The reprocessing operation offers several points at which americium removal maybe attempted, and we are evaluating two classes of materials targeted at different steps in the process. Extraction chromatography resin materials loaded with three different alkylcarbamoyl phosphinates and phosphine oxides were accessed for Am removal efficiency and Am/Fe selectivity from 1-7 molar nitric acid solutions. Commercial and experimental mono- and bifunctional anion-exchange resins were evaluated for total alpha-activity removal from post-evaporator solutions whose composition, relative to the original nitric acid effluent, is reduced in acid and greatly increased in total salt content. With both classes of materials, americium/total alpha emission removal is sufficient to meet regulatory requirements even under sub-optimal conditions. Batch distribution coefficients, column performance data, and the effects of Fe-masking agents will be presented.
Date: August 1, 2000
Creator: BARR, M.; JARVINEN, G. & AL, ET
Partner: UNT Libraries Government Documents Department

Rapid Column Extraction Methods for Urine

Description: A new fecal analysis method that dissolves plutonium oxide was developed at the Westinghouse Savannah River Site. Diphonix Resin (Eichrom Industries), is used to pre-concentrate the actinides from digested fecal samples. A rapid microwave digestion technique is used to remove the actinides from the Diphonix Resin, which effectively extracts plutonium and americium from acidic solutions containing hydrofluoric acid. After resin digestion, the plutonium and americium are recovered in a small volume of nitric acid that is loaded onto small extraction chromatography columns, TEVA Resin and TRU Resin (Eichrom Industries). The method enables complete dissolution of plutonium oxide and provides high recovery of plutonium and americium with good removal of thorium isotopes such as thorium-228.
Date: June 9, 2000
Creator: Maxwell, S.L. III
Partner: UNT Libraries Government Documents Department

Recent advances in the development of extraction chromatographic materials for the isolation of radionuclides from biological and environmental samples.

Description: The determination of low levels of radionuclides in environmental and biological samples is often hampered by the complex and variable nature of the samples. One approach to circumventing this problem is to incorporate into the analytical scheme a separation and preconcentration step by which the species of interest can be isolated from the major constituents of the sample. Extraction chromatography (EXC), a form of liquid chromatography in which the stationary phase comprises an extractant or a solution of an extractant in an appropriate diluent coated onto an inert support, provides a simple and efficient means of performing a wide variety of metal ion separations. Recent advances in extractant design, in particular the development of extractants capable of metal ion recognition or of strong complex formation even in acidic media, have substantially improved the utility of the method. For the preconcentration of actinides, for example, an EXC resin consisting of a liquid diphosphonic acid supported on a polymeric substrate has been shown to exhibit extraordinarily strong retention of these elements from acidic chloride media. This resin, together with other related materials, can provide the basis of a number of efficient and flexible schemes for the separation and preconcentration of radionuclides form a variety of samples for subsequent determination.
Date: November 30, 1998
Creator: Dietz, M. L.
Partner: UNT Libraries Government Documents Department

Simultaneous measurements of plutonium and uranium in spent-fuel dissolver solutions

Description: The authors have studied the isotope dilution gamma-ray spectrometry (IDGS) technique for simultaneous measurements of elemental concentrations and isotopic compositions for both plutonium and uranium in input spent-fuel dissolver solutions at a reprocessing plant. The technique under development includes both sample preparation and analysis methods. For simultaneous measurements of both plutonium and uranium, a critical issue is to develop a new method to keep both plutonium and uranium in the sample after they are separated from fission products. Furthermore, it is equally important to improve the analysis method so that the precision and accuracy of the plutonium analysis remain unaffected while uranium is retained in the sample. To keep both plutonium and uranium in the sample for simultaneous measurements, extraction chromatography is being studied and shows promise to achieve the goal of cosegregation of the plutonium and uranium. The technique uses U/TEVA{center_dot}Spec resin to separate fission products and recover both uranium and plutonium in the resin from dissolver solutions for subsequent measuring using high-resolution gamma-ray spectrometry. Owing to the fact that the U/Pu ratio is altered during the fission product separation phase, it is necessary to develop a method which could accurately correct for this effect. Such a method was developed using the unique decay properties of {sup 241}Pu to {sup 237}U and shows considerable promise in allowing for accurate determination of the {sup 235}U concentrations before the chemical extraction.
Date: November 1, 1997
Creator: Li, T.K.; Kuno, T.; Kitagawa, O.; Sato, S.; Kurosawa, A. & Kuno, Y.
Partner: UNT Libraries Government Documents Department

Extraction chromatography: Progress and opportunities

Description: Extraction chromatography provides a simple and effective method for the analytical and preparative-scale separation of a variety of metal ions. Recent advances in extractant design, particularly the development of extractants capable of metal ion recognition or of strong complex formation in highly acidic media, have significantly improved the utility of the technique. Advances in support design, most notably the introduction of functionalized supports to enhance metal ion retention, promise to yield further improvements. Column instability remains a significant obstacle, however, to the process-scale application of extraction chromatography. 79 refs.
Date: October 1, 1997
Creator: Dietz, M.L.; Horwitz, E.P. & Bond, A.H.
Partner: UNT Libraries Government Documents Department

Analytical support for characterization of americium-curium solution at SRS

Description: Americium-Curium (Am-Cm) solution in F-Canyon was produced during the Mk 40 and Mk 41 campaigns in the mid and late 1970`s. The Savannah River Site (SRS) Central Laboratory recently characterized this important solution of nuclear material to enable assessment by Westinghouse Savannah River Company and Department of Energy of disposition options. The tank had last been sampled and analyzed in 1986. A wide range of analyses were performed to determine the tank contents. New radiochemical column separation methods were developed to fully characterize the solution for actinides, metals, anions, and isotopics to support the disposition study in a timely manner. Current disposition is to perform a vitrification process on the Am/Cm solution at SRS to produce glass canisters for safe shipment and storage of this material. The SRS Am/Cm waste solution will be converted, in effect, to a product for an outside customer. Oak Ridge National Laboratory. To support the Am/Cm vitrification processing, process support analyses are required after completion of denitration, precipitation and redissolution steps. Full elemental chemistry characterization will be required on the final melter feed solution.
Date: October 1, 1996
Creator: Maxwell, S.L. III & Nelson, M.R.
Partner: UNT Libraries Government Documents Department

The removal of uranium from acidic media using ion exchange and/or extraction chromatography

Description: The separation and purification of uranium from either nitric acid or hydrochloric acid media can be accomplished by using either solvent extraction or ion-exchange. Over the past two years at Los Alamos, emerging programs are focused on recapturing the expertise required to do limited, small-quantity processing of enriched uranium. During this period of time, we have been investigating ion-addition, waste stream polishing is associated with this effort in order to achieve more complete removal of uranium prior to recycle of the acid. Extraction chromatography has been demonstrated to further polish the uranium from both nitric and hydrochloric acid media thus allowing for a more complete recovery of the actinide material and creation of less waste during the processing steps.
Date: June 1, 1996
Creator: FitzPatrick, J.R.; Schake, B.S.; Murphy, J.; Holmes, K & West, M.H.
Partner: UNT Libraries Government Documents Department

Application of extraction chromatography to actinide decontamination of hydrochloric acid effluent streams

Description: Extraction chromatography is under development as a method to lower actinide activity levels in effluent steams. Successful application of this technique for radioactive liquid waste treatment would provide a low activity feed stream for HCl recycle, reduce the loss of radioactivity to the environment in aqueous effluents, and would lower the quantity and reduce the hazard of the associated solid waste. The extraction of Pu and Am from HCl solutions was examined for several commercial and laboratory-produced sorbed resin materials. Inert supports included silica and polymer beads of differing mesh sizes. The support material was coated with either n-octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (O-CMPO) or di-(4-t-butylphenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (D-CMPO) as an extractant, and using either tributyl phosphate (TBP) or diamyl amylphosphonate (DAAP) as a diluent. Solutions tested were effluent streams generated by ion exchange and solvent extraction recovery of Pu. A finer mesh silica support material demonstrated advantages in removal of trivalent Am in some tests, but also showed a tendency toward plugging and channeling as column sizes and flow rates were increased. Larger bead sizes showed better physical properties as the process was scaled up to removal of gram quantities of Am from large effluent volumes. The ratio of extractant to diluent also appeared to play a role in the retention of Am. In direct comparative studies, when loaded on identical supports and diluent conditions, D-CMPO demonstrated better Am retention than O-CMPO from HCl process effluents.
Date: May 1, 1996
Creator: Schulte, L.D.; McKee, S.D. & Salazar, R.R.
Partner: UNT Libraries Government Documents Department

Nineteenth annual actinide separations conference: Conference program and abstracts

Description: This report contains the abstracts from the conference presentations. Sessions were divided into the following topics: Waste treatment; Spent fuel treatment; Issues and responses to Defense Nuclear Facility Safety Board 94-1; Pyrochemical technologies; Disposition technologies; and Aqueous separation technologies.
Date: December 31, 1995
Creator: Bronson, M.
Partner: UNT Libraries Government Documents Department

Feasibility study of plutonium and uranium measurements in input dissolver solutions

Description: We are studying the isotope dilution gamma-ray spectrometry (IDGS) technique for the simultaneous measurements of concentrations and isotopic compositions for both plutonium and uranium in spent-fuel dissolver solutions at a reprocessing plant. Previous experiments have demonstrated that the IDGS technique can determine the elemental concentrations and isotopic compositions of plutonium in dissolver solutions. The chemical separation and recovery methods for just plutonium were ion-exchange techniques using anion exchange resin beads and filter papers. To keep both plutonium and uranium in the sample for simultaneous measurements, a new sample preparation method is being studied and developed: extraction chromatography. The technique uses U/TEVA{center_dot}Spec resin to separate fission products and recover both uranium and plutonium in the resin from dissolver solutions for measurements by high-resolution gamma-ray spectrometry.
Date: October 1, 1995
Creator: Li, T.K.; Kitagawa, O.; Kuno, Y. & Kurosawa, A.
Partner: UNT Libraries Government Documents Department

Arsenic speciation using high performance liquid chromatography-inductively coupled plasma-mass spectrometry

Description: A method has been developed by Argonne National Laboratory to identify and quantify As(III), As(V), and organoarsenic compounds in environmental samples. A arsenic species were separated by reversed-phase, ion-pairing, HPLC using a microbore Inertsil-ODS{trademark} column. Only 1 {micro}L of sample was injected on the column, and the mobile phase flow rates were typically on the order of 40 {micro}L/min. The HPLC mobile phase was a mixture of methanol and tetrabutylammonium hydroxide (TBAH), and the column effluent was introduced into an ICP-mass spectrometer using direct injection nebulization. Detection limits of less than 1 pg As (as injected on the column) were easily obtained for each arsenic species. The effect of changes in mobile phase composition and ICP-MS conditions will be described, as well as quality control measures, e.g., the use of surrogates, internal standards, and matrix spikes. Precision and accuracy information will be presented from the analysis of aqueous standards and soil extracts that were spiked with arsenic oxide [As(III)], sodium arsenate [As(V)], dimethylarsinic acid (DMAA), or chlorovinyl arsenious acid (CVAA). The authors believe that these data demonstrate the utility of this technique for the sensitive determination of arsenic species present in water or soil.
Date: August 1995
Creator: Bass, D. A.; Yaeger, J. S.; Crain, J. S.; Kiely, J. T.; Parish, K. J.; Gowdy, M. J. et al.
Partner: UNT Libraries Government Documents Department

Determination of total and isotopic uranium by inductively coupled plasma-mass spectrometry at the Fernald Environmental Management Project

Description: At the Fernald Environmental Management Project (FEMP) in southwestern Ohio, ICP-mass spectrometry (ICP-MS), with sample introduction by peristaltic pumping, is used to determine total and isotopic uranium (U-234, U-235, U-236 and U-238) in soil samples. These analyses are conducted in support of the environmental cleanup of the FEMP site. Various aspects of the sample preparation and instrumental analysis will be discussed. Initial sample preparation consists of oven drying to determine moisture content, and grinding and rolling to homogenize the sample. This is followed by a nitric/hydrofluoric acid digestion to bring the uranium in the sample into solution. Bismuth is added to the sample prior to digestion to monitor for losses. The total uranium (U-238) content of this solution and the U{sup 235}/U{sup 238} ratio are measured on the first pass through the ICP-MS. To determine the concentration of the less abundant U{sup 234} and U{sup 236} isotopes, the digestate is further concentrated by using Eichrom TRU-Spec extraction columns before the second pass through the ICP-MS. Quality controls for both the sample preparation and instrumental protocols will also be discussed. Finally, an explanation of the calculations used to report the data in either weight percent or activity units will be given.
Date: April 1, 1995
Creator: Miller, F.L.; Bolin, R.N.; Feller, M.T. & Danahy, R.J.
Partner: UNT Libraries Government Documents Department

Removal of plutonium and Americium from hydrochloric acid waste streams using extraction chromatography

Description: Extraction chromatography is under development as a method to lower actinide activity levels in hydrochloric acid (HCl) effluent streams. Successful application of this technique for radioactive liquid waste treatment would provide a low activity feedstream for HCl recycle, reduce the loss of radioactivity to the environment in aqueous effluents, and lower the quantity and improve the form of solid waste generated. The extraction of plutonium and americium from HCl solutions was examined for several commercial and laboratory-produced sorbed resin materials. Polymer beads were coated with n-octyl(phenyl)-N,N-diisobutylcarbamoyl- methylphosphine oxide (CMPO) and either tributyl phosphate (TBP), or diamyl amylphosphonate (DAAP). Distribution coefficients for Pu and Am were measured by contact studies in 1-10 M HCl, while varying REDOX conditions, actinide loading levels, and resin formulations. Flow experiments were run to evaluate actinide loading and elution under varied conditions. Significant differences in the actinide distribution coefficients in contact experiments, and in actinide retention in flow experiments were observed as a function of resin formulation.
Date: January 1, 1995
Creator: Schulte, L. D.; FitzPatrick, J. R.; Salazar, R. R.; Schake, B. S. & Martinez, B. T.
Partner: UNT Libraries Government Documents Department

Improved separation techniques for the characterization of radioactive waste samples

Description: Analysts have routinely used organic solvent extractions and precipitation techniques to remove matrix constituents which interfere with the characterization of radioactive waste samples. Problems with these traditional techniques involve the production of organic waste and time consuming steps. Extraction chromatography using recently developed resins manufactured by Eichrom Industries provides accuracy comparable to traditional techniques while reducing waste and time. Three types of Eichrom resins were evaluated on samples from radioactive waste tanks at the Department of Energy`s (DOE) Oak Ridge National Laboratory (ORNL) for the analysis of the inorganic EPA target analyte elements, radioactive strontium, and radioactive technetium. Results show that extraction chromatography may be successfully applied to the characterization of DOE radioactive waste samples similar to those at ORNL, providing high efficiency, reduced waste production, and safety benefits.
Date: 1994
Creator: Meeks, A. M.; Keller, J. M.; Giaquinto, J. M. & Ross, T.
Partner: UNT Libraries Government Documents Department