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Sample records for actinide removal characteristics

  1. Actinide removal from spent salts

    DOEpatents

    Hsu, Peter C.; von Holtz, Erica H.; Hipple, David L.; Summers, Leslie J.; Adamson, Martyn G.

    2002-01-01

    A method for removing actinide contaminants (uranium and thorium) from the spent salt of a molten salt oxidation (MSO) reactor is described. Spent salt is removed from the reactor and analyzed to determine the contaminants present and the carbonate concentration. The salt is dissolved in water, and one or more reagents are added to precipitate the thorium as thorium oxide and/or the uranium as either uranium oxide or as a diuranate salt. The precipitated materials are filtered, dried and packaged for disposal as radioactive waste. About 90% of the thorium and/or uranium present is removed by filtration. After filtration, salt solutions having a carbonate concentration >20% can be dried and returned to the reactor for re-use. Salt solutions containing a carbonate concentration <20% require further clean-up using an ion exchange column, which yields salt solutions that contain less than 0.1 ppm of thorium or uranium.

  2. Screening Evaluation of Sodium Nonatitanate for Strontium and Actinide Removal from Alkaline Salt Solution

    SciTech Connect

    Hobbs, D.T.

    2001-02-13

    This report describes results from screening tests evaluating strontium and actinide removal characteristics of a sodium titanate material developed by Clearfield and coworkers at Texas A and M University and offered commercially by Honeywell. Sodium nonatitanate may exhibit improved actinide removal kinetics and filtration characteristics compared to MST and thus merit testing.

  3. Actinide removal from nitric acid waste streams

    SciTech Connect

    Muscatello, A.C.; Navratil, J.D.

    1986-01-01

    Actinide separations research at the Rocky Flats Plant (RFP) has found ways to significantly improve plutonium secondary recovery and americium removal from nitric acid waste streams generated by plutonium purification operations. Capacity and breakthrough studies show anion exchange with Dowex 1x4 (50 to 100 mesh) to be superior for secondary recovery of plutonium. Extraction chromatography with TOPO(tri-n-octyl-phosphine oxide) on XAD-4 removes the final traces of plutonium, including hydrolytic polymer. Partial neutralization and solid supported liquid membrane transfer removes americium for sorption on discardable inorganic ion exchangers, potentially allowing for non-TRU waste disposal.

  4. In vitro removal of actinide (IV) ions

    DOEpatents

    Weitl, Frederick L.; Raymond, Kenneth N.

    1982-01-01

    A compound of the formula: ##STR1## wherein X is hydrogen or a conventional electron-withdrawing group, particularly --SO.sub.3 H or a salt thereof; n is 2, 3, or 4; m is 2, 3, or 4; and p is 2 or 3. The present compounds are useful as specific sequestering agents for actinide (IV) ions. Also described is a method for the 2,3-dihydroxybenzamidation of azaalkanes.

  5. Removal of actinides from nuclear reprocessing wastes: a pilot plant study using non-radioactive simulants

    SciTech Connect

    Maxey, H.R.; McIsaac, L.D.; Chamberlain, D.B.; McManus, G.J.

    1980-01-01

    Nuclear fuel reprocessing wastes generated at the ICPP contain small amounts of actinides, primarily Pu and Am. Removal of these actinides reduces the long term storage hazards of the waste. The development of a flowsheet to remove trivalent actinides is discussed in this paper. Pilot plant studies used actinide simulants. As a result of these studies, the Height of a Transfer Unit (HTU) was selected as the better measure of pulse column separation efficiency.

  6. Sequestering agents for the removal of actinides from waste streams

    SciTech Connect

    Raymond, K.N.; White, D.J.; Xu, Jide; Mohs, T.R.

    1997-10-01

    The goal of this project is to take a biomimetic approach toward developing new separation technologies for the removal of radioactive elements from contaminated DOE sites. To achieve this objective, the authors are investigating the fundamental chemistry of naturally occurring, highly specific metal ion sequestering agents and developing them into liquid/liquid and solid supported actinide extraction agents. Nature produces sideophores (e.g., Enterobactin and Desferrioxamine B) to selectivity sequester Lewis acidic metal ions, in particular Fe(III), from its surroundings. These chelating agents typically use multiple catechols or hydroxamic acids to form polydentate ligands that chelate the metal ion forming very stable complexes. The authors are investigating and developing analogous molecules into selective chelators targeting actinide(IV) ions, which display similar properties to Fe(III). By taking advantage of differences in charge, preferred coordination number, and pH stability range, the transition from nature to actinide sequestering agents has been applied to the development of new and highly selective actinide extraction technologies. Additionally, the authors have shown that these chelating ligands are versatile ligands for chelating U(VI). In particular, they have been studying their coordination chemistry and fundamental interactions with the uranyl ion [UO{sub 2}]{sup 2+}, the dominant form of uranium found in aqueous media. With an understanding of this chemistry, and results obtained from in vivo uranium sequestration studies, it should be possible to apply these actinide(IV) extraction technologies to the development of new extraction agents for the removal of uranium from waste streams.

  7. Actinide removal from wastewater applying waste minimization techniques

    SciTech Connect

    Covey, J.R.; Midkiff, W.S. ); Cadena, F. )

    1992-01-01

    A major concern at LANL is the large volume of low level radioactive sludge that is generated by the current treatment technology. The plant meets current discharge limits but annually produces 200 55-gallon drums of sludge (approximately 60 tons) during the process of removing only few grants of radioactive isotopes. Most of the sludge results from the coagulants, iron and lime, added at the plant at a concentration of 10,000 parts-per-million (ppm). If the principal actinides in the influent could be separated and reduced to pure metallic form, the annual volume of plutonium would be about the size of a marble and the americium would be about the size of a BB. Waste minimization will be a key design criteria for the new facility. Records of total suspended solids (TSS) in the influent average about 1000 Kg per year (approximately 1 ton). Therefore, the theoretical sludge volume reduction is near 98%. Research is underway to develop and evaluate technologies that achieve the desired removal efficiency with a minimum of produced waste volume.

  8. Actinide removal from wastewater applying waste minimization techniques

    SciTech Connect

    Covey, J.R.; Midkiff, W.S.; Cadena, F.

    1992-07-01

    A major concern at LANL is the large volume of low level radioactive sludge that is generated by the current treatment technology. The plant meets current discharge limits but annually produces 200 55-gallon drums of sludge (approximately 60 tons) during the process of removing only few grants of radioactive isotopes. Most of the sludge results from the coagulants, iron and lime, added at the plant at a concentration of 10,000 parts-per-million (ppm). If the principal actinides in the influent could be separated and reduced to pure metallic form, the annual volume of plutonium would be about the size of a marble and the americium would be about the size of a BB. Waste minimization will be a key design criteria for the new facility. Records of total suspended solids (TSS) in the influent average about 1000 Kg per year (approximately 1 ton). Therefore, the theoretical sludge volume reduction is near 98%. Research is underway to develop and evaluate technologies that achieve the desired removal efficiency with a minimum of produced waste volume.

  9. Process to remove actinides from soil using magnetic separation

    DOEpatents

    Avens, Larry R.; Hill, Dallas D.; Prenger, F. Coyne; Stewart, Walter F.; Tolt, Thomas L.; Worl, Laura A.

    1996-01-01

    A process of separating actinide-containing components from an admixture including forming a slurry including actinide-containing components within an admixture, said slurry including a dispersion-promoting surfactant, adjusting the pH of the slurry to within a desired range, and, passing said slurry through a pretreated matrix material, said matrix material adapted to generate high magnetic field gradients upon the application of a strong magnetic field exceeding about 0.1 Tesla whereupon a portion of said actinide-containing components are separated from said slurry and remain adhered upon said matrix material is provided.

  10. ACTINIDE REMOVAL PROCESS SAMPLE ANALYSIS, CHEMICAL MODELING, AND FILTRATION EVALUATION

    SciTech Connect

    Martino, C.; Herman, D.; Pike, J.; Peters, T.

    2014-06-05

    Filtration within the Actinide Removal Process (ARP) currently limits the throughput in interim salt processing at the Savannah River Site. In this process, batches of salt solution with Monosodium Titanate (MST) sorbent are concentrated by crossflow filtration. The filtrate is subsequently processed to remove cesium in the Modular Caustic Side Solvent Extraction Unit (MCU) followed by disposal in saltstone grout. The concentrated MST slurry is washed and sent to the Defense Waste Processing Facility (DWPF) for vitrification. During recent ARP processing, there has been a degradation of filter performance manifested as the inability to maintain high filtrate flux throughout a multi-batch cycle. The objectives of this effort were to characterize the feed streams, to determine if solids (in addition to MST) are precipitating and causing the degraded performance of the filters, and to assess the particle size and rheological data to address potential filtration impacts. Equilibrium modelling with OLI Analyzer{sup TM} and OLI ESP{sup TM} was performed to determine chemical components at risk of precipitation and to simulate the ARP process. The performance of ARP filtration was evaluated to review potential causes of the observed filter behavior. Task activities for this study included extensive physical and chemical analysis of samples from the Late Wash Pump Tank (LWPT) and the Late Wash Hold Tank (LWHT) within ARP as well as samples of the tank farm feed from Tank 49H. The samples from the LWPT and LWHT were obtained from several stages of processing of Salt Batch 6D, Cycle 6, Batch 16.

  11. Evaluation of different solvent extraction methods for removing actinides from high acid waste streams

    SciTech Connect

    Yarbro, S.L.; Schreiber, S.B.; Dunn, S.L. ); Rogers, J. )

    1991-01-01

    At the Los Alamos National Laboratory Plutonium Facility, anion exchange is used to recover plutonium from nitric acid solutions. Although this approach recovers >99%, trace amounts of plutonium and other actinides remain the effluent and require additional processing. Currently, a ferric hydroxide carrier precipitation is used to remove the trace actinides and the resulting sludge is cemented. Because it costs approximately $10,000 per drum for disposal, we are developing an additional polishing step so that the effluent actinide levels are reduced to below 100 nCi/g. This would allow the resulting waste sludge to disposed as low-level waste at approximately $200 per drum. We are investigating various solvent extraction techniques for removing actinides. The most promising are chelating resins and membrane-based liquid-liquid solvent extraction. This report details some of our preliminary results. 4 refs., 3 tabs.

  12. Sequestering agents for the removal of actinides from waste streams

    SciTech Connect

    Raymond, K.; White, D.; Whisenhunt, D.

    1996-10-01

    The ultimate goal of this project is to develop new separation technologies to remove radioactive metal ions from contaminated DOE sites. To this end we are studying both the fundamental chemistry and the extractant properties of some chelators that are either found in nature or are closely related to natural materials. The work is a collaboration betwen Lawrence Berkeley National Laboratory-University of California, Berkeley, and the Glenn T. Seaborg Institute for Transactinium Science at Lawrence Livermore National Laboratory.

  13. Removal of actinides from dissolved ORNL MVST sludge using the TRUEX process

    SciTech Connect

    Spencer, B.B.; Egan, B.Z.; Chase, C.W.

    1997-07-01

    Experiments were conducted to evaluate the transuranium extraction process for partitioning actinides from actual dissolved high-level radioactive waste sludge. All tests were performed at ambient temperature. Time and budget constraints permitted only two experimental campaigns. Samples of sludge from Melton Valley Storage Tank W-25 were rinsed with mild caustic (0.2 M NaOH) to reduce the concentrations of nitrates and fission products associated with the interstitial liquid. In one campaign, the rinsed sludge was dissolved in nitric acid to produce a solution containing total metal concentrations of ca. 1.8 M with a nitric acid concentration of ca. 2.9 M. About 50% of the dry mass of the sludge was dissolved. In the other campaign, the sludge was neutralized with nitric acid to destroy the carbonates, then leached with ca. 2.6 M NaOH for ca. 6 h before rinsing with the mild caustic. The sludge was then dissolved in nitric acid to produce a solution containing total metal concentrations of ca. 0.6 M with a nitric acid concentration of ca. 1.7 M. About 80% of the sludge dissolved. The dissolved sludge solution form the first campaign began gelling immediately, and a visible gel layer was observed after 8 days. In the second campaign, the solution became hazy after ca. 8 days, indicating gel formation, but did not display separated gel layers after aging for 20 days. Batch liquid-liquid equilibrium tests of both the extraction and stripping operations were conducted. Chemical analyses of both phases were used to evaluate the process. Evaluation was based on two metrics: the fraction of TRU elements removed from the dissolved sludge and comparison of the results with predictions made with the Generic TRUEX Model (GTM). The fractions of Eu, Pu, Cm, Th, and U species removed from aqueous solution in only one extraction stage were > 95% and were close to the values predicted by the GTM. Mercury was also found to be strongly extracted, with a one-stage removal of > 92%.

  14. Systematic calculation of the fission mode characteristics of the light actinides

    SciTech Connect

    Hambsch, F.-J.; Dematte, L.; Oberstedt, S.

    1998-10-26

    A systematic calculation of the fission mode characteristics of the light actinides in the frame of the multi-modal random neck-rupture model has been started. In particular the isotopes {sup 220,226,232}Th and {sup 220,226}Ac are under investigation. A clear competition between the outer barrier heights of the asymmetric standard and the symmetric superlong fission mode has been found. Their systematic variation with the compound nuclear mass might explain the drastic changes in the nuclear charge distributions recently observed at GSI. The current status will be reported and discussed in the light of the experimental results.

  15. Evaluation and testing of sequestering agents for the removal of actinides from waste streams

    SciTech Connect

    Hoffman, D.C.; Romanovski, V.V.; Veeck, A.C.

    1997-10-01

    The purpose of this project is to evaluate and test the complexing ability of a variety of promising new complexing agents synthesized by Professor Kenneth Raymond`s group at the University of California, Berkeley (ESP-CP TTP Number SF16C311). Some of these derivatives have already shown the potential for selectivity binding Pu(IV) in a wide range of solutions in the presence of other metals. Professor Raymond`s group uses molecular modeling to design and synthesize ligands based on modification of natural siderophores, or their analogs, for chelation of actinides. The ligands are then modified for use as liquid/liquid and solid/liquid extractants. The authors` group at the Glenn T. Seaborg Institute for Transactinium Science (ITS) at Lawrence Livermore National Laboratory determines the complex formation constants between the ligands and actinide ions, the capacity and time dependence for uptake on the resins, and the effect of other metal ions and pH.

  16. Actinide recovery process

    DOEpatents

    Muscatello, Anthony C.; Navratil, James D.; Saba, Mark T.

    1987-07-28

    Process for the removal of plutonium polymer and ionic actinides from aqueous solutions by absorption onto a solid extractant loaded on a solid inert support such as polystyrenedivinylbenzene. The absorbed actinides can then be recovered by incineration, by stripping with organic solvents, or by acid digestion. Preferred solid extractants are trioctylphosphine oxide and octylphenyl-N,N-diisobutylcarbamoylmethylphosphine oxide and the like.

  17. Actinide extraction methods

    DOEpatents

    Peterman, Dean R [Idaho Falls, ID; Klaehn, John R [Idaho Falls, ID; Harrup, Mason K [Idaho Falls, ID; Tillotson, Richard D [Moore, ID; Law, Jack D [Pocatello, ID

    2010-09-21

    Methods of separating actinides from lanthanides are disclosed. A regio-specific/stereo-specific dithiophosphinic acid having organic moieties is provided in an organic solvent that is then contacted with an acidic medium containing an actinide and a lanthanide. The method can extend to separating actinides from one another. Actinides are extracted as a complex with the dithiophosphinic acid. Separation compositions include an aqueous phase, an organic phase, dithiophosphinic acid, and at least one actinide. The compositions may include additional actinides and/or lanthanides. A method of producing a dithiophosphinic acid comprising at least two organic moieties selected from aromatics and alkyls, each moiety having at least one functional group is also disclosed. A source of sulfur is reacted with a halophosphine. An ammonium salt of the dithiophosphinic acid product is precipitated out of the reaction mixture. The precipitated salt is dissolved in ether. The ether is removed to yield the dithiophosphinic acid.

  18. A comparision of TRUEX and CMP solvent extraction processes for actinide removal from ICPP wastes

    SciTech Connect

    Herbst, R.S.; Brewer, K.N.; Garn, T.G.; Law, J.D.

    1996-04-01

    The Idaho Chemical Processing Plant (ICPP) is currently engaged in development efforts for the decontamination of high-level radioactive wastes generated from decades of nuclear fuel reprocessing. These wastes include several types of calcine, generated by high temperature solidification of reprocessing raffinates. In addition to calcine, there are smaller quantities of secondary wastes from decontamination and solvent wash activities which are typically referred to as sodium-bearing waste (SBW). Solvent extraction technologies based on octyl(phenyl)-N,N-diisobutyl-carbamoylmethylphosphine oxide (CMPO, the active extractant in the TRUEX process) and dihexyl-N,N-diethylcarbamoylmethylphosphonate (DHDECMP, the active extractant in the CMP process) are being evaluated for actinide partitioning from these waste streams. Calcines must first be dissolved in an appropriate acidic solution prior to treatment in solvent extraction based processes. The SBW is currently stored as an acidic solution and readily amenable to liquid extraction techniques. Development efforts to date have revolved around defining and refining baseline flowsheets with the TRUEX and CMP processes for each waste stream. Another objective of this work was to determine which of these technologies are best suited for the treatment of ICPP wastes. Laboratory batch contacts were performed to identify relevant chemistry and distribution coefficients. This information was then used to establish baseline flowsheet configuration with regard to chemistry. The laboratory data were used to model the behavior of the actinides and other constituents in the wastes in countercurrent, continuous processes based on centrifugal contactor technology. The laboratory data and modelling results form the basis for comparison of the two processes.

  19. FACILITY UPGRADES FOR RECEIPT FROM ACTINIDE REMOVAL AND MODULAR CAUSTIC SIDE SOLVENT EXTRACTION PROCESSES AT THE SAVANNAH RIVER SITE

    SciTech Connect

    Fellinger, T; Stephen Phillips, S; Benjamin Culbertson, B; Beverly02 Davis, B; Aaron Staub, A

    2007-02-13

    The Savannah River Site (SRS) is currently on an aggressive program to empty its High Level Waste (HLW) tanks and immobilize its radioactive waste into a durable borosilicate glass in the Defense Waste Processing Facility (DWPF). As a part of that program, two new processes will be brought on-line to assist in emptying the HLW tanks. These processes are in addition to the current sludge removal process and are called the Actinide Removal Process (ARP) and the Modular Caustic Side Solvent Extraction (MCU) Process. In order to accept and process the streams generated from these two new processes, several facility modifications are required and are broken down into several projects. These projects are handling the facility modifications required for the Tank Farm (241-96H), and DWPF vitrification facility (221-S), and DWPF ancillary facilities (511-S, and 512-S). Additional modifications to the 221-S building were required to address the flammability concern from the solvent carryover from the MCU process. This paper will describe a summary of the modifications impacting the 511-S, 512-S, and the 221-S facilities in order to receive the new streams from the ARP and MCU processes at the DWPF.

  20. Actinide recovery process

    DOEpatents

    Muscatello, A.C.; Navratil, J.D.; Saba, M.T.

    1985-06-13

    Process for the removal of plutonium polymer and ionic actinides from aqueous solutions by absorption onto a solid extractant loaded on a solid inert support such as polystyrene-divinylbenzene. The absorbed actinides can then be recovered by incineration, by stripping with organic solvents, or by acid digestion. Preferred solid extractants are trioctylphosphine oxide and octylphenyl-N,N-diisobutylcarbamoylmethylphosphine oxide and the like. 2 tabs.

  1. Evaluation of New Inorganic Sorbents for Strontium and Actinide Removal from High-Level Nuclear Waste Solutions

    SciTech Connect

    Hobbs, D.T.; Nyman, M.; Medvedev, D.G.; Tripathi, A.; Clearfield, A.

    2004-03-28

    Monosodium titanate (MST), a hydrous metal oxide sorbent, is the baseline material for the removal of 90Sr and alpha-emitting radionuclides (principally 238Pu, 239Pu, 240Pu and 237Np) from alkaline waste solutions generated during the processing of irradiated nuclear materials at the Savannah River Site. This material exhibits excellent performance characteristics for strontium removal. Plutonium removal is also good, but problematic at the estimated bonding concentration. We are currently developing new inorganic materials for improved sorption characteristics. These materials include sodium nonatitanates, pharmacosiderites and heteropolyniobates. We will present results evaluating the performance of these materials with simulated and actual high level nuclear waste solutions.

  2. Water-soluble chelating polymers for removal of actinides from wastewater

    SciTech Connect

    Jarvinen, G.D.

    1997-10-01

    Polymer filtration is a technology under development to selectively recover valuable or regulated metal ions from process or wastewaters. The technology uses water-soluble chelating polymers that are designed to selectively bind with metal ions in aqueous solutions. The polymers have a sufficiently large molecular weight that they can be separated and concentrated using available ultrafiltration (UF) technology. The UF range is generally considered to include molecular weights from about 3000 to several million daltons and particles sizes of about 2 to 1000 nm. Water and smaller unbound components of the solution pass freely through the UF membrane. The polymers can then be reused by changing the solution conditions to release the metal ions that are recovered in concentrated form for recycle or disposal. Some of the advantages of polymer filtration relative to technology now in use are rapid binding kinetics, high selectivity, low energy and capital costs, and a small equipment footprint. Some potential commercial applications include electroplating rinse waters, photographic processing, nuclear power plant cooling water; remediation of contaminated soils and groundwater; removal of mercury contamination; and textile, paint and dye production. The purpose of this project is to evaluate this technology to remove plutonium, americium, and other regulated metal ions from various process and waste streams found in nuclear facilities. The work involves preparation of the water-soluble chelating polymers; small-scale testing of the chelating polymer systems for the required solubility, UF properties, selectivity and binding constants; followed by an engineering assessment at a larger scale to allow comparison to competing separation technologies. This project focuses on metal-ion contaminants in waste streams at the Plutonium Facility and the Waste Treatment Facility at LANL. Potential applications at other DOE facilities are also apparent.

  3. Actinides-1981

    SciTech Connect

    Not Available

    1981-09-01

    Abstracts of 134 papers which were presented at the Actinides-1981 conference are presented. Approximately half of these papers deal with electronic structure of the actinides. Others deal with solid state chemistry, nuclear physic, thermodynamic properties, solution chemistry, and applied chemistry.

  4. Subsurface Biogeochemistry of Actinides

    SciTech Connect

    Kersting, Annie B.; Zavarin, Mavrik

    2016-06-29

    A major scientific challenge in environmental sciences is to identify the dominant processes controlling actinide transport in the environment. It is estimated that currently, over 2200 metric tons of plutonium (Pu) have been deposited in the subsurface worldwide, a number that increases yearly with additional spent nuclear fuel (Ewing et al., 2010). Plutonium has been shown to migrate on the scale of kilometers, giving way to a critical concern that the fundamental biogeochemical processes that control its behavior in the subsurface are not well understood (Kersting et al., 1999; Novikov et al., 2006; Santschi et al., 2002). Neptunium (Np) is less prevalent in the environment; however, it is predicted to be a significant long-term dose contributor in high-level nuclear waste. Our focus on Np chemistry in this Science Plan is intended to help formulate a better understanding of Pu redox transformations in the environment and clarify the differences between the two long-lived actinides. The research approach of our Science Plan combines (1) Fundamental Mechanistic Studies that identify and quantify biogeochemical processes that control actinide behavior in solution and on solids, (2) Field Integration Studies that investigate the transport characteristics of Pu and test our conceptual understanding of actinide transport, and (3) Actinide Research Capabilities that allow us to achieve the objectives of this Scientific Focus Area (SFA and provide new opportunities for advancing actinide environmental chemistry. These three Research Thrusts form the basis of our SFA Science Program (Figure 1).

  5. Analysis of large soil samples for actinides

    DOEpatents

    Maxwell, III; Sherrod L.

    2009-03-24

    A method of analyzing relatively large soil samples for actinides by employing a separation process that includes cerium fluoride precipitation for removing the soil matrix and precipitates plutonium, americium, and curium with cerium and hydrofluoric acid followed by separating these actinides using chromatography cartridges.

  6. Actinide Recovery Method for Large Soil Samples

    SciTech Connect

    Maxwell, S.L. III; Nichols, S.

    1998-11-01

    A new Actinide Recovery Method has been developed by the Savannah River Site Central Laboratory to preconcentrate actinides in very large soil samples. Diphonix Resin(r) is used eliminate soil matrix interferences and preconcentrate actinides after soil leaching or soil fusion. A rapid microwave digestion technique is used to remove the actinides from the Diphonix Resin(r). After the resin digestion, the actinides are recovered in a small volume of nitric acid which can be easily loaded onto small extraction-chromatography columns, such as TEVA Resin(r), U-TEVA Resin(r) or TRU Resin(r) (Eichrom Industries). This method enables the application of small, selective extraction-columns to recover actinides from very large soil samples with high selectivity, consistent tracer recoveries and minimal liquid waste.

  7. Actinide metal processing

    DOEpatents

    Sauer, N.N.; Watkin, J.G.

    1992-03-24

    A process for converting an actinide metal such as thorium, uranium, or plutonium to an actinide oxide material by admixing the actinide metal in an aqueous medium with a hypochlorite as an oxidizing agent for sufficient time to form the actinide oxide material and recovering the actinide oxide material is described together with a low temperature process for preparing an actinide oxide nitrate such as uranyl nitrate. Additionally, a composition of matter comprising the reaction product of uranium metal and sodium hypochlorite is provided, the reaction product being an essentially insoluble uranium oxide material suitable for disposal or long term storage.

  8. Actinide metal processing

    DOEpatents

    Sauer, Nancy N.; Watkin, John G.

    1992-01-01

    A process of converting an actinide metal such as thorium, uranium, or plnium to an actinide oxide material by admixing the actinide metal in an aqueous medium with a hypochlorite as an oxidizing agent for sufficient time to form the actinide oxide material and recovering the actinide oxide material is provided together with a low temperature process of preparing an actinide oxide nitrate such as uranyl nitrte. Additionally, a composition of matter comprising the reaction product of uranium metal and sodium hypochlorite is provided, the reaction product being an essentially insoluble uranium oxide material suitable for disposal or long term storage.

  9. SALTSTONE VAULT CLASSIFICATION SAMPLES MODULAR CAUSTIC SIDE SOLVENT EXTRACTION UNIT/ACTINIDE REMOVAL PROCESS WASTE STREAM APRIL 2011

    SciTech Connect

    Eibling, R.

    2011-09-28

    Savannah River National Laboratory (SRNL) was asked to prepare saltstone from samples of Tank 50H obtained by SRNL on April 5, 2011 (Tank 50H sampling occurred on April 4, 2011) during 2QCY11 to determine the non-hazardous nature of the grout and for additional vault classification analyses. The samples were cured and shipped to Babcock & Wilcox Technical Services Group-Radioisotope and Analytical Chemistry Laboratory (B&W TSG-RACL) to perform the Toxic Characteristic Leaching Procedure (TCLP) and subsequent extract analysis on saltstone samples for the analytes required for the quarterly analysis saltstone sample. In addition to the eight toxic metals - arsenic, barium, cadmium, chromium, mercury, lead, selenium and silver - analytes included the underlying hazardous constituents (UHC) antimony, beryllium, nickel, and thallium which could not be eliminated from analysis by process knowledge. Additional inorganic species determined by B&W TSG-RACL include aluminum, boron, chloride, cobalt, copper, fluoride, iron, lithium, manganese, molybdenum, nitrate/nitrite as Nitrogen, strontium, sulfate, uranium, and zinc and the following radionuclides: gross alpha, gross beta/gamma, 3H, 60Co, 90Sr, 99Tc, 106Ru, 106Rh, 125Sb, 137Cs, 137mBa, 154Eu, 238Pu, 239/240Pu, 241Pu, 241Am, 242Cm, and 243/244Cm. B&W TSG-RACL provided subsamples to GEL Laboratories, LLC for analysis for the VOCs benzene, toluene, and 1-butanol. GEL also determines phenol (total) and the following radionuclides: 147Pm, 226Ra and 228Ra. Preparation of the 2QCY11 saltstone samples for the quarterly analysis and for vault classification purposes and the subsequent TCLP analyses of these samples showed that: (1) The saltstone waste form disposed of in the Saltstone Disposal Facility in 2QCY11 was not characteristically hazardous for toxicity. (2) The concentrations of the eight RCRA metals and UHCs identified as possible in the saltstone waste form were present at levels below the UTS. (3) Most of the

  10. DWPF Flowsheet Studies with Simulants to Determine Modular Caustic Side Solvent Extraction Unit Solvent Partitioning and Verify Actinide Removal Process Incorporation Strategy

    SciTech Connect

    Herman, C

    2006-04-21

    The Actinide Removal Process (ARP) facility and the Modular Caustic Side Solvent Extraction Unit (MCU) are scheduled to begin processing salt waste in fiscal year 2007. A portion of the streams generated in the salt processing facilities will be transferred to the Defense Waste Processing Facility (DWPF) to be incorporated in the glass matrix. Before the streams are introduced, a combination of impact analyses and research and development studies must be performed to quantify the impacts on DWPF processing. The Process Science & Engineering (PS&E) section of the Savannah River National Laboratory (SRNL) was requested via Technical Task Request (TTR) HLW/DWPF/TTR-2004-0031 to evaluate the impacts on DWPF processing. Simulant Chemical Process Cell (CPC) flowsheet studies have been performed using previous composition and projected volume estimates for the ARP sludge/monosodium titanate (MST) stream. Due to changes in the flammability control strategy for DWPF for salt processing, the incorporation strategy for ARP has changed and additional ARP flowsheet tests were necessary to validate the new processing strategy. The last round of ARP testing included the incorporation of the MCU stream and identified potential processing issues with the MCU solvent. The identified issues included the potential carry-over and accumulation of the MCU solvent components in the CPC condensers and in the recycle stream to the Tank Farm. Therefore, DWPF requested SRNL to perform additional MCU flowsheet studies to better quantify the organic distribution in the CPC vessels. The previous MCU testing used a Sludge Batch 4 (SB4) simulant since it was anticipated that both of these facilities would begin salt processing during SB4 processing. The same sludge simulant recipe was used in this round of ARP and MCU testing to minimize the number of changes between the two phases of testing so a better comparison could be made. ARP and MCU stream simulants were made for this phase of testing

  11. Actinide-ion sensor

    DOEpatents

    Li, Shelly X; Jue, Jan-fong; Herbst, Ronald Scott; Herrmann, Steven Douglas

    2015-01-13

    An apparatus for the real-time, in-situ monitoring of actinide-ion concentrations. A working electrolyte is positioned within the interior of a container. The working electrolyte is separated from a reference electrolyte by a separator. A working electrode is at least partially in contact with the working electrolyte. A reference electrode is at least partially in contact with the reference electrolyte. A voltmeter is electrically connected to the working electrode and the reference electrode. The working electrolyte comprises an actinide-ion of interest. The separator is ionically conductive to the actinide-ion of interest. The separator comprises an actinide, Zr, and Nb. Preferably, the actinide of the separator is Am or Np, more preferably Pu. In one embodiment, the actinide of the separator is the actinide of interest. In another embodiment, the separator further comprises P and O.

  12. Actinide Spectroscopy Workshop

    SciTech Connect

    Tobin, J.G.; Shuh, D.K.

    2004-12-05

    Actinide materials present an extreme scientific challenge to the materials research community. The complex electronic structures of actinide materials result in many unusual and unique properties that have yet to be fully understood. The difficulties in handling, preparing, and characterizing actinide materials has frequently precluded investigations and has the limited the detailed understanding of these relevant, complex materials. However, modern experiments with actinide materials have the potential to provide key, fundamental information about many long-standing issues concerning actinide materials. This workshop focused on the scientific and technical challenges posed by actinide materials and the potential that synchrotron radiation approaches available at the ALS can contribute to improving the fundamental understanding of actinides materials. Fundamental experimental approaches and results, as well as theoretical modeling and computational simulations, were part of the workshop program.

  13. Removal characteristics of wipe devices under various conditions.

    PubMed

    Shoji, Miki; Kondo, Takashi; Kijima, Akihiro; Shibao, Yukinobu; Nakajima, Tomoko; Yamada, Koichi; Nemoto, Nobuo

    2010-08-01

    Understanding the removal factor for specific conditions is essential to estimate removable surface contamination levels by wiping. The removal characteristics of dry foamed polystyrene pads and filter paper applied to polyvinyl chloride flooring are investigated using C-thymidine under various conditions (i.e., weight of contaminants, wax coating, temperature and humidity). Eight wipes were performed per flooring piece with a uniformly deposited contaminant to estimate the total removable surface contamination. The wipe devices were pressed against the surface by 2 kg-force with fingertips. The first wipe ratio (the ratio of the activity removed by the first wipe to the activity removed by eight wipes) from flooring on which was deposited 500 microg mL of C-thymidine solution varies between 24% and 71% for polystyrene pads and between 33% and 83% for filter papers, depending on the atmospheric humidity and temperature. For deposition concentrations of 1 microg mL, the mean first wipe ratio using polystyrene pads, which are almost constant vs. humidity and temperature, are 68% and 24% for waxed and unwaxed surfaces, respectively. Under the same conditions, the mean first wipe ratio for filter paper varied with both the surface and the environmental conditions. The total recovery (the ratio of the total activity removed by eight wipes to the total deposited activity) for deposition concentrations of 500 microg mL tended to increase with humidity for both wiping devices. The total recovery for deposition concentrations of 1 microg mL is generally low. The first wipe ratio in the lowest case with foamed polystyrene pads in this study was 19%. In that case, the total removable activity is speculated to increase from the sum of eight wipes, if additional wipes are performed. Therefore, the theoretical value of 0.1 recommended by ISO for the removal factor is appropriate when wiping polyvinyl chloride flooring using foamed polystyrene pads.

  14. Bidentate organophosphorus solvent extraction process for actinide recovery and partition

    DOEpatents

    Schulz, Wallace W.

    1976-01-01

    A liquid-liquid extraction process for the recovery and partitioning of actinide values from acidic nuclear waste aqueous solutions, the actinide values including trivalent, tetravalent and hexavalent oxidation states is provided and includes the steps of contacting the aqueous solution with a bidentate organophosphorous extractant to extract essentially all of the actinide values into the organic phase. Thereafter the respective actinide fractions are selectively partitioned into separate aqueous solutions by contact with dilute nitric or nitric-hydrofluoric acid solutions. The hexavalent uranium is finally removed from the organic phase by contact with a dilute sodium carbonate solution.

  15. Research in actinide chemistry

    SciTech Connect

    Choppin, G.R.

    1993-01-01

    This research studies the behavior of the actinide elements in aqueous solution. The high radioactivity of the transuranium actinides limits the concentrations which can be studied and, consequently, limits the experimental techniques. However, oxidation state analogs (trivalent lanthanides, tetravalent thorium, and hexavalent uranium) do not suffer from these limitations. Behavior of actinides in the environment are a major USDOE concern, whether in connection with long-term releases from a repository, releases from stored defense wastes or accidental releases in reprocessing, etc. Principal goal of our research was expand the thermodynamic data base on complexation of actinides by natural ligands (e.g., OH[sup [minus

  16. Actinide recovery method -- Large soil samples

    SciTech Connect

    Maxwell , S.L. III

    2000-04-25

    There is a need to measure actinides in environmental samples with lower and lower detection limits, requiring larger sample sizes. This analysis is adversely affected by sample-matrix interferences, which make analyzing soil samples above five-grams very difficult. A new Actinide-Recovery Method has been developed by the Savannah River Site Central Laboratory to preconcentrate actinides from large-soil samples. Diphonix Resin (Eichrom Industries), a 1994 R and D 100 winner, is used to preconcentrate the actinides from large soil samples, which are bound powerfully to the resin's diphosphonic acid groups. A rapid microwave-digestion technique is used to remove the actinides from the Diphonix Resin, which effectively eliminates interfering matrix components from the soil matrix. The microwave-digestion technique is more effective and less tedious than catalyzed hydrogen peroxide digestions of the resin or digestion of diphosphonic stripping agents such as HEDPA. After resin digestion, the actinides are recovered in a small volume of nitric acid which can be loaded onto small extraction chromatography columns, such as TEVA Resin, U-TEVA Resin or TRU Resin (Eichrom Industries). Small, selective extraction columns do not generate large volumes of liquid waste and provide consistent tracer recoveries after soil matrix elimination.

  17. Separation of actinides from lanthanides utilizing molten salt electrorefining

    SciTech Connect

    Grimmett, D.L.; Fusselman, S.P.; Roy, J.J.; Gay, R.L.; Krueger, C.L.; Storvick, T.S.; Inoue, T.; Hijikata, T.; Takahashi, N.

    1996-10-01

    TRUMP-S (TRansUranic Management through Pyropartitioning Separation) is a pyrochemical process being developed to separate actinides form fission products in nuclear waste. A key process step involving molten salt electrorefining to separate actinides from lanthanides has been studied on a laboratory scale. Electrorefining of U, Np, Pu, Am, and lanthanide mixtures from molten cadmium at 450 C to a solid cathode utilizing a molten chloride electrolyte resulted in > 99% removal of actinides from the molten cadmium and salt phases. Removal of the last few percent of actinides is accompanied by lowered cathodic current efficiency and some lanthanide codeposition. Actinide/lanthanide separation ratios on the cathode are ordered U > Np > Pu > Am and are consistent with predictions based on equilibrium potentials.

  18. Thermodynamic Properties of Actinides and Actinide Compounds

    NASA Astrophysics Data System (ADS)

    Konings, Rudy J. M.; Morss, Lester R.; Fuger, Jean

    The necessity of obtaining accurate thermodynamic quantities for the actinide elements and their compounds was recognized at the outset of the Manhattan Project, when a dedicated team of scientists and engineers initiated the program to exploit nuclear energy for military purposes. Since the end of World War II, both fundamental and applied objectives have motivated a great deal of further study of actinide thermodynamics. This chapter brings together many research papers and critical reviews on this subject. It also seeks to assess, to systematize, and to predict important properties of the actinide elements, ions, and compounds, especially for species in which there is significant interest and for which there is an experimental basis for the prediction.

  19. Method for preparing actinide nitrides

    DOEpatents

    Bryan, G.H.; Cleveland, J.M.; Heiple, C.R.

    1975-12-01

    Actinide nitrides, and particularly plutonium and uranium nitrides, are prepared by reacting an ammonia solution of an actinide compound with an ammonia solution of a reactant or reductant metal, to form finely divided actinide nitride precipitate which may then be appropriately separated from the solution. The actinide nitride precipitate is particularly suitable for forming nuclear fuels.

  20. PREFACE: Actinides 2009

    NASA Astrophysics Data System (ADS)

    Rao, Linfeng; Tobin, James G.; Shuh, David K.

    2010-07-01

    This volume of IOP Conference Series: Materials Science and Engineering consists of 98 papers that were presented at Actinides 2009, the 8th International Conference on Actinide Science held on 12-17 July 2009 in San Francisco, California, USA. This conference was jointly organized by Lawrence Livermore National Laboratory and Lawrence Berkeley National Laboratory. The Actinides conference series started in Baden-Baden, Germany (1975) and this first conference was followed by meetings at Asilomar, CA, USA (1981), Aix-en-Provence, France (1985), Tashkent, USSR (1989), Santa Fe, NM, USA (1993), Baden-Baden, Germany (1997), Hayama, Japan (2001), and Manchester, UK (2005). The Actinides conference series provides a regular venue for the most recent research results on the chemistry, physics, and technology of the actinides and heaviest elements. Actinides 2009 provided a forum spanning a diverse range of scientific topics, including fundamental materials science, chemistry, physics, environmental science, and nuclear fuels. Of particular importance was a focus on the key roles that basic actinide chemistry and physics research play in advancing the worldwide renaissance of nuclear energy. Editors Linfeng Rao Lawrence Berkeley National Laboratory (lrao@lbl.gov) James G Tobin Lawrence Livermore National Laboratory (tobin1@llnl.gov) David K Shuh Lawrence Berkeley National Laboratory (dkshuh@lbl.gov)

  1. Elevated concentrations of actinides in Mono Lake

    SciTech Connect

    Anderson, R.F.; Bacon, M.P.; Brewer, P.G.

    1982-04-30

    Tetravalent thorium, pentavalent protactinium, hexavalent uranium, and plutonium (oxidation state uncertain) are present in much higher concentrations in Mono Lake, a saline, alkaline lake in eastern central California, than in seawater. Low ratios of actinium to protactinium and of americium to plutonium indicate that the concentrations of trivalent actinides are not similarly enhanced. The elevated concentrations of the ordinarily very insoluble actinides are maintained in solution by natural ligands, which inhibit their chemical removal from the water column, rather than by an unusually large rate of supply.

  2. Elevated concentrations of actinides in mono lake.

    PubMed

    Anderson, R F; Bacon, M P; Brewer, P G

    1982-04-30

    Tetravalent thorium, pentavalent protactinium, hexavalent uranium, and plutonium (oxidation state uncertain) are present in much higher concentrations in Mono Lake, a saline, alkaline lake in eastern central California, than in seawater. Low ratios of actinium to protactinium and of americium to plutonium indicate that the concentrations of trivalent actinides are not similarly enhanced. The elevated concentrations of the ordinarily very insoluble actinides are maintained in solution by natural ligands, which inhibit their chemical removal from the water column, rather than by an unusually large rate of supply.

  3. Systematization of actinides using cluster analysis

    SciTech Connect

    Kopyrin, A.A.; Terent`eva, T.N.; Khramov, N.N.

    1994-11-01

    A representation of the actinides in multidimensional property space is proposed for systematization of these elements using cluster analysis. Literature data for their atomic properties are used. Owing to the wide variation of published ionization potentials, medians are used to estimate them. Vertical dendograms are used for classification on the basis of distances between the actinides in atomic-property space. The properties of actinium and lawrencium are furthest removed from the main group. Thorium and mendelevium exhibit individualized properties. A cluster based on the einsteinium-fermium pair is joined by californium.

  4. Characteristics of Biological Nitrogen Removal in a Multiple Anoxic and Aerobic Biological Nutrient Removal Process

    PubMed Central

    Wang, Huoqing; Guan, Yuntao; Li, Li; Wu, Guangxue

    2015-01-01

    Two sequencing batch reactors, one with the conventional anoxic and aerobic (AO) process and the other with the multiple AO process, were operated to examine characteristics of biological nitrogen removal, especially of the multiple AO process. The long-term operation showed that the total nitrogen removal percentage of the multiple AO reactor was 38.7% higher than that of the AO reactor. In the multiple AO reactor, at the initial SBR cycle stage, due to the occurrence of simultaneous nitrification and denitrification, no nitrite and/or nitrate were accumulated. In the multiple AO reactor, activities of nitrite oxidizing bacteria were inhibited due to the multiple AO operating mode applied, resulting in the partial nitrification. Denitrifiers in the multiple AO reactor mainly utilized internal organic carbon for denitrification, and their activities were lower than those of denitrifiers in the AO reactor utilizing external organic carbon. PMID:26491676

  5. Phosphorus removal characteristics in hydroxyapatite crystallization using converter slag.

    PubMed

    Kim, Eung-Ho; Hwang, Hwan-Kook; Yim, Soo-Bin

    2006-01-01

    This study was performed to investigate the phosphorus removal characteristics in hydroxyapatite (HAP) crystallization using converter slag as a seed crystal and the usefulness of a slag column reactor system. The effects of alkalinity, and the isomorphic-substitutable presence of ionic magnesium, fluoride, and iron on HAP crystallization seeded with converter slag, were examined using a batch reactor system. The phosphorus removal efficiencies of the batch reactor system were found to increase with increases in the iron and fluoride ion concentrations, and to decrease with increases in the alkalinity and magnesium ion concentration. A column reactor system for HAP crystallization using converter slag was found to achieve high, stable levels of phosphorus elimination: the average PO4-P removal efficiency over 414 days of operation was 90.4%, in which the effluent phosphorus concentration was maintained at less than 0.5 mg/L under the appropriate phosphorus crystallization conditions. The X-ray diffraction (XRD) patterns and Fourier transform infrared (FTIR) spectra of the crystalline material deposited on the seed particles exhibited peaks consistent with HAP. Scanning electron micrograph (SEM) images showed that finely distributed crystalline material was formed on the surfaces of the seed particles. Energy dispersive X-ray spectroscopy (EDS) mapping analysis revealed that the molar Ca/P composition ratio of the crystalline material was 1.72.

  6. Hydraulic characteristics of a constructed wetland: Implications for pollutant removal

    NASA Astrophysics Data System (ADS)

    Wachniew, P.; Czuprynski, P.; Maloszewski, P.; Ozimek, T.

    2003-04-01

    Constructed wetlands are built in order to treat wastewaters of various origin with some degree of control over purification processes. Treatment wetlands improve water quality through removal of suspended solids, organics, nitrogen, phosphorus, pathogens (bacteria, parasites, viruses) and metals. Transformation and removal of pollutants from wastewaters occur via numerous interrelated physical, chemical and biological processes. The efficiency of soluble pollutants removal is related to the degree of contact between wastewaters and the reactive surfaces. Therefore knowledge of hydraulic phenomena is crucial in studies of wetland functioning. A subsurface flow wetland in Nowa Slupia, Poland was studied in order to find out relationships between hydraulic phenomena and wetland performance. The wetland consists of three parallel gravel beds overgrown by common reed with a total surface area of 6400 sq m, total active volume of around 900 cubic m and the average loading of around 4 l/s. Three tracer tests with bromide and tritium accompanied by observations of water quality, plant distribution and biomass were performed in summer and winter conditions. Tracer breakthrough curves obtained from tracer tests were used to identify sub-systems within the wetland and to infer their hydraulic properties (water residence times, active volumes, dispersive characteristics). Three reed beds receive different wastewater loadings and show different water residence times and dispersive characteristics. Wastewater flow occurs partly via surface overflow with apparent stagnant zones and preferential flow pathways. These flow patterns are reflected in complex structure of breakthrough curves. Inhomogenous wastewater distribution within the wetland is due to operation practices and clogging of the gravel beds with refractory organic matter. Observations of effluent water quality, plant distribution and biomass reflect these apparent inhomogenities in wastewater flow patterns. This work

  7. Research in actinide chemistry

    SciTech Connect

    Not Available

    1991-01-01

    This report contains research results on studies of inorganic and organic complexes of actinide and lanthanide elements. Special attention is given to complexes of humic acids and to spectroscopic studies.

  8. Health and environmental risk-related impacts of actinide burning on high-level waste disposal

    SciTech Connect

    Forsberg, C.W.

    1992-05-01

    The potential health and environmental risk-related impacts of actinide burning for high-level waste disposal were evaluated. Actinide burning, also called waste partitioning-transmutation, is an advanced method for radioactive waste management based on the idea of destroying the most toxic components in the waste. It consists of two steps: (1) selective removal of the most toxic radionuclides from high-level/spent fuel waste and (2) conversion of those radionuclides into less toxic radioactive materials and/or stable elements. Risk, as used in this report, is defined as the probability of a failure times its consequence. Actinide burning has two potential health and environmental impacts on waste management. Risks and the magnitude of high-consequence repository failure scenarios are decreased by inventory reduction of the long-term radioactivity in the repository. (What does not exist cannot create risk or uncertainty.) Risk may also be reduced by the changes in the waste characteristics, resulting from selection of waste forms after processing, that are superior to spent fuel and which lower the potential of transport of radionuclides from waste form to accessible environment. There are no negative health or environmental impacts to the repository from actinide burning; however, there may be such impacts elsewhere in the fuel cycle.

  9. PRODUCTION OF ACTINIDE METAL

    DOEpatents

    Knighton, J.B.

    1963-11-01

    A process of reducing actinide oxide to the metal with magnesium-zinc alloy in a flux of 5 mole% of magnesium fluoride and 95 mole% of magnesium chloride plus lithium, sodium, potassium, calcium, strontium, or barium chloride is presented. The flux contains at least 14 mole% of magnesium cation at 600-- 900 deg C in air. The formed magnesium-zinc-actinide alloy is separated from the magnesium-oxide-containing flux. (AEC)

  10. Thermochemistry of the actinides

    SciTech Connect

    Kleinschmidt, P.D.

    1993-10-01

    The measurement of equilibria by Knudsen effusion techniques and the enthalpy of formation of the actinide atoms is briefly discussed. Thermochemical data on the sublimation of the actinide fluorides is used to calculate the enthalpies of formation and entropies of the gaseous species. Estimates are made for enthalpies and entropies of the tetrafluorides and trifluorides for those systems where data is not available. The pressure of important species in the tetrafluoride sublimation processes is calculated based on this thermochemical data.

  11. Nonaqueous actinide hydride dissolution and production of actinide $beta$- diketonates

    DOEpatents

    Crisler, L.R.

    1975-11-11

    Actinide beta-diketonate complex molecular compounds are produced by reacting a beta-diketone compound with a hydride of the actinide material in a mixture of carbon tetrachloride and methanol. (auth)

  12. Positron Spectroscopy of Hydrothermally Grown Actinide Oxides

    DTIC Science & Technology

    2014-03-27

    In this method, the powdered material is placed in a solution which contains extremely powerful mineralizers, such as cesium fluoride for actinide...the isotope that acts as a positron source is sodium -22, which has a relatively short half-life (2.6 y) and emits a characteristic gamma photon (at

  13. Actinide Lanthanide Separation Process – ALSEP

    SciTech Connect

    Gelis, Artem V.; Lumetta, Gregg J.

    2014-01-29

    Separation of the minor actinides (Am, Cm) from the lanthanides at an industrial scale remains a significant technical challenge for closing the nuclear fuel cycle. To increase the safety of used nuclear fuel (UNF) reprocessing, as well as reduce associated costs, a novel solvent extraction process has been developed. The process allows for partitioning minor actinides, lanthanides and fission products following uranium/plutonium/neptunium removal; minimizing the number of separation steps, flowsheets, chemical consumption, and waste. This new process, Actinide Lanthanide SEParation (ALSEP), uses an organic solvent consisting of a neutral diglycolamide extractant, either N,N,N',N'-tetra(2 ethylhexyl)diglycolamide (T2EHDGA) or N,N,N',N'-tetraoctyldiglycolamide (TODGA), and an acidic extractant 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]), dissolved in an aliphatic diluent (e.g. n-dodecane). The An/Ln co-extraction is conducted from moderate-to-strong nitric acid, while the selective stripping of the minor actinides from the lanthanides is carried out using a polyaminocarboxylic acid/citrate buffered solution at pH anywhere between 3 and 4.5. The extraction and separation of the actinides from the fission products is very effective in a wide range of HNO3 concentrations and the minimum separation factors for lanthanide/Am exceed 30 for Nd/Am, reaching > 60 for Eu/Am under some conditions. The experimental results presented here demonstrate the great potential for a combined system, consisting of a neutral extractant such as T2EHDGA or TODGA, and an acidic extractant such as HEH[EHP], for separating the minor actinides from the lanthanides.

  14. Separation of actinides from spent nuclear fuel: A review.

    PubMed

    Veliscek-Carolan, Jessica

    2016-11-15

    This review summarises the methods currently available to extract radioactive actinide elements from solutions of spent nuclear fuel. This separation of actinides reduces the hazards associated with spent nuclear fuel, such as its radiotoxicity, volume and the amount of time required for its' radioactivity to return to naturally occurring levels. Separation of actinides from environmental water systems is also briefly discussed. The actinide elements typically found in spent nuclear fuel include uranium, plutonium and the minor actinides (americium, neptunium and curium). Separation methods for uranium and plutonium are reasonably well established. On the other hand separation of the minor actinides from lanthanide fission products also present in spent nuclear fuel is an ongoing challenge and an area of active research. Several separation methods for selective removal of these actinides from spent nuclear fuel will be described. These separation methods include solvent extraction, which is the most commonly used method for radiochemical separations, as well as the less developed but promising use of adsorption and ion-exchange materials.

  15. Trends in actinide processing at Hanford

    SciTech Connect

    Harmon, H.D.

    1993-09-01

    In 1989, the mission at the Hanford Site began a dramatic and sometimes painful transition. The days of production--as we used to know it--are over. Our mission officially has become waste management and environmental cleanup. This mission change didn`t eliminate many jobs--in fact, budgets have grown dramatically to support the new mission. Most all of the same skilled crafts, engineers, and scientists are still required for the new mission. This change has not eliminated the need for actinide processing, but it has certainly changed the focus that our actinide chemists and process engineers have. The focus used to be on such things as increasing capacity, improving separations efficiency, and product purity. Minimizing waste had become a more important theme in recent years and it is still a very important concept in the waste management and environmental cleanup arena. However, at Hanford, a new set of words dominates the actinide process scene as we work to deal with actinides that still reside in a variety of forms at the Hanford Site. These words are repackage, stabilize, remove, store and dispose. Some key activities in each of these areas are described in this report.

  16. Extraction of DBP and MBP from actinides: application to the recovery of actinides from TBP-sodium carbonate scrub solutions. [Aralex process

    SciTech Connect

    Horwitz, E.P.; Mason, G.W.; Bloomquist, C.A.A.; Leonard, R.A.; Bernstein, G.J.

    1980-01-01

    A flowsheet for the recovery of actinides from TBP-Na/sub 2/CO/sub 3/ scrub waste solutions has been developed, based on batch extraction data, and tested, using laboratory scale counter-current extraction techniques. The process, called the ARALEX process, utilizes 2-ethyl-1-hexanol (2-EHOH) to extract the TBP degradation products (HDBP and H/sub 2/MBP) from acidified Na/sub 2/CO/sub 3/ scrub waste leaving the actinides in the aqueous phase. Dibutyl and monobutyl phosphoric acids are attached to the 2-EHOH molecules through hydrogen bonds. These hydrogen bonds also diminish the ability of the HDBP and H/sub 2/MBP to complex actinides and thus all actinides remain in the aqueous raffinate. Dilute sodium hydroxide solutions can be used to back-extract the dibutyl and monobutyl phosphoric acid esters as their sodium salts. The 2-EHOH can then be recycled. After extraction of the acidified carbonate waste with 2-EHOH, the actinides may be readily extracted from the raffinate with DHDECMP or, in the case of tetra- and hexavalent actinides, with TBP. The ARALEX process is relatively simple and involves inexpensive and readily available chamicals. The ARALEX process can also be applied to other actinide waste streams which contain appreciable concentrations of polar organic compounds that interfere with conventional actinide ion exchange and liquid-liquid extraction procedures. One such application is the removal of detergents from laundry or clean-up solutions contaminated with actinides.

  17. Actinide halide complexes

    SciTech Connect

    Avens, L.R.; Zwick, B.D.; Sattelberger, A.P.; Clark, D.L.; Watkin, J.G.

    1991-02-07

    A compound of the formula MX{sub n}L{sub m} wherein M = Th, Pu, Np,or Am thorium, X = a halide atom, n = 3 or 4, L is a coordinating ligand selected from the group consisting of aprotic Lewis bases having an oxygen-, nitrogen-, sulfur-, or phosphorus-donor, and m is 3 or 4 for monodentate ligands or is 2 for bidentate ligands, where n + m = 7 or 8 for monodentate ligands or 5 or 6 for bidentate ligands, a compound of the formula MX{sub n} wherein M, X, and n are as previously defined, and a process of preparing such actinide metal compounds including admixing the actinide metal in an aprotic Lewis base as a coordinating solvent in the presence of a halogen-containing oxidant, are provided.

  18. Estimating organic micro-pollutant removal potential of activated carbons using UV absorption and carbon characteristics.

    PubMed

    Zietzschmann, Frederik; Altmann, Johannes; Ruhl, Aki Sebastian; Dünnbier, Uwe; Dommisch, Ingvild; Sperlich, Alexander; Meinel, Felix; Jekel, Martin

    2014-06-01

    Eight commercially available powdered activated carbons (PAC) were examined regarding organic micro-pollutant (OMP) removal efficiencies in wastewater treatment plant (WWTP) effluent. PAC characteristic numbers such as B.E.T. surface, iodine number and nitrobenzene number were checked for their potential to predict the OMP removal of the PAC products. Furthermore, the PAC-induced removal of UV254 nm absorption (UVA254) in WWTP effluent was determined and also correlated with OMP removal. None of the PAC characteristic numbers can satisfactorily describe OMP removal and accordingly, these characteristics have little informative value on the reduction of OMP concentrations in WWTP effluent. In contrast, UVA254 removal and OMP removal correlate well for carbamazepine, diclofenac, and several iodinated x-ray contrast media. Also, UVA254 removal can roughly describe the average OMP removal of all measured OMP, and can accordingly predict PAC performance in OMP removal. We therefore suggest UVA254 as a handy indicator for the approximation of OMP removal in practical applications where direct OMP concentration quantification is not always available. In continuous operation of large-scale plants, this approach allows for the efficient adjustment of PAC dosing to UVA254, in order to ensure reliable OMP removal whilst minimizing PAC consumption.

  19. PF-4 actinide disposition strategy

    SciTech Connect

    Margevicius, Robert W

    2010-05-28

    The dwindling amount of Security Category I processing and storage space across the DOE Complex has driven the need for more effective storage of nuclear materials at LANL's Plutonium Facility's (PF-4's) vault. An effort was begun in 2009 to create a strategy, a roadmap, to identify all accountable nuclear material and determine their disposition paths, the PF-4 Actinide Disposition Strategy (PADS). Approximately seventy bins of nuclear materials with similar characteristics - in terms of isotope, chemical form, impurities, disposition location, etc. - were established in a database. The ultimate disposition paths include the material to remain at LANL, disposition to other DOE sites, and disposition to waste. If all the actions described in the document were taken, over half of the containers currently in the PF-4 vault would been eliminated. The actual amount of projected vault space will depend on budget and competing mission requirements, however, clearly a significant portion of the current LANL inventory can be either dispositioned or consolidated.

  20. Environmental behavior of actinides

    NASA Astrophysics Data System (ADS)

    Choppin, G. R.

    2006-01-01

    Since the plutonium concentration in ocean waters is quite low, most of the plutonium deposited in marine waters has been sorbed onto plants and sediments. Actinides in natural waters usually are not in a state of thermodynamic equilibrium for long time periods as their solubility and migration behavior is strongly related to the form in which the nuclides are introduced initially into the aquatic system for long time periods. Their solubility depends on pH (hydrolysis), E H (oxidation state), reaction with complexants (e.g., carbonate, phosphate, humic acid, etc.), sorption to surfaces of minerals and/or colloids, etc. The primary variable is the oxidation state of the actinide cation. Actinides can be present in more than one oxidation state which complicates modeling actinide environmental behavior. Np(V)O 2 + and Pu(V)O 2 + are weakly complexing and resistant to hydrolysis and subsequent precipitation, but both can undergo reduction to the IV oxidation state. The solubility of NpO 2 + can be as high as 10-4M, while that of PuO 2 + is more limited as the very low solubility of Pu(OH)4 promotes reduction to Pu(IV). The solubility of hexavalent UO 2 2+ in sea water is limited by hydrolysis, but has a relatively high concentration due to carbonate complexation. Americium(III) hydroxocarbonate, Am(CO3)(OH), is the limiting species for the solubility of Am(III) in sea water. Thorium has a very low solubility due to the formation of Th(OH)4.

  1. Analysis of the Gas Core Actinide Transmutation Reactor (GCATR)

    NASA Technical Reports Server (NTRS)

    Clement, J. D.; Rust, J. H.

    1977-01-01

    Design power plant studies were carried out for two applications of the plasma core reactor: (1) As a breeder reactor, (2) As a reactor able to transmute actinides effectively. In addition to the above applications the reactor produced electrical power with a high efficiency. A reactor subsystem was designed for each of the two applications. For the breeder reactor, neutronics calculations were carried out for a U-233 plasma core with a molten salt breeding blanket. A reactor was designed with a low critical mass (less than a few hundred kilograms U-233) and a breeding ratio of 1.01. The plasma core actinide transmutation reactor was designed to transmute the nuclear waste from conventional LWR's. The spent fuel is reprocessed during which 100% of Np, Am, Cm, and higher actinides are separated from the other components. These actinides are then manufactured as oxides into zirconium clad fuel rods and charged as fuel assemblies in the reflector region of the plasma core actinide transmutation reactor. In the equilibrium cycle, about 7% of the actinides are directly fissioned away, while about 31% are removed by reprocessing.

  2. [Removal characteristics of DCM by biotrickling filter and biofilter].

    PubMed

    Pan, Wei-Long; Yu, Jian-Ming; Cheng, Zhuo-Wei; Cai, Wen-Ji

    2013-12-01

    A biofilter (BF) packed with nutrition slow-release material and a biotrickling filter (BTF) packed with ether-based polyurethane foam were set up to remove dichloromethane (DCM) from exhaust gas. Results showed that the biofilm formations in BTF and BF were completed by using the mixture of a special strain and a bacterial community, within 25d and 22d, respectively. Through the observation of the filter surface by SEM, the surface of packings in BF was loose with thin biofilm colonies, whereas the one in BTF was dense with thick biofilm. Under the condition of inlet DCM concentration of 100-1,500 mg x m(-3), EBRT of 25-85 s, the removal efficiency of DCM in BTF was better than that in BF, and the maximum removal load was 22.61 g x (m3 x h)(-1) and 29.05 g (m3 x h)(-1), respectively. The relationship between CO2 production and DCM removal was approximately linear, with the mineralization rate being 70.4% and 66.8% for BTF and BF, respectively. The dynamic behaviors of DCM in BTF and BF were described by the Michaelis-Menten model. Through the calculation, the unit volume maximum degradation rate r(max) was 22.7790 g x (m3 x h)(-1) and 28.5714 g x (m3 x h)(-1), while the gas phase saturation constant Ks was 0.1412 g x m(-3) and 0.1486 g x m(-3)

  3. PROCESS OF PRODUCING ACTINIDE METALS

    DOEpatents

    Magel, T.T.

    1959-07-14

    The preparation of actinide metals in workable, coherent form is described. In general, the objects of the invention are achieved by heating a mixture of an oxide and a halide of an actinide metal such as uranium with an alkali metal on alkaline earth metal reducing agent in the presence of iodine.

  4. Phytosiderophore effects on subsurface actinide contaminants: potential for phytostabilization and phytoextraction.

    SciTech Connect

    Ruggiero, C. E.; Twary, S. N.; Deladurantaye, E.

    2003-01-01

    In recognition of the need for a safe, effective technology for long term Pu/Th/Actinide stabilization or removal from soils, we have begun an investigation of the potential for phytoremediation (phytostabilization and/or phytoextraction) of Pu and other actinide soil contaminants at DOE sites using phytosiderophore producing plants, and are investigating the contribution of phytosiderophores to actinide mobility in the subsurface environment. Phytoremediation and Phytostabilization have been proven to be a cost-effective, safe, efficient, and publicly acceptable technology for clean up and/or stabilization of contaminant metals . However, no phyto-based technologies have been developed for stabilization or removal of plutonium from soils and groundwater, and very few have been investigated for other actinides . Current metal-phytostabilization and phytoremediation techniques, predominately based around lead, nickel, and other soft-metal phytoextraction, will almost certainly be inadequate for plutonium due its distinct chemical properties . Phytosiderophore-based phytoremediation may provide technically and financially practical methods for remediation and long-term stewardship of soils that have low to moderate, near surface actinide contamination . We plan to demonstrate potential benefits of phytosiderophore-producing plants for long-term actinide contaminant stabilization by the plant's prevention of soil erosion and actinide migration through hydraulic control and/or through actinide removal through phytoextraction . We may also show possible harm caused by these plants through increased presence of actinide chelators that could increase actinide mobilization and migration in the subsurface environment. This information can then be directly applied by either removal of harmful plants, or be used to develop plant-based soil stabilization/remediation technologies .

  5. Actinide halide complexes

    DOEpatents

    Avens, L.R.; Zwick, B.D.; Sattelberger, A.P.; Clark, D.L.; Watkin, J.G.

    1992-11-24

    A compound is described of the formula MX[sub n]L[sub m] wherein M is a metal atom selected from the group consisting of thorium, plutonium, neptunium or americium, X is a halide atom, n is an integer selected from the group of three or four, L is a coordinating ligand selected from the group consisting of aprotic Lewis bases having an oxygen-, nitrogen-, sulfur-, or phosphorus-donor, and m is an integer selected from the group of three or four for monodentate ligands or is the integer two for bidentate ligands, where the sum of n+m equals seven or eight for monodentate ligands or five or six for bidentate ligands. A compound of the formula MX[sub n] wherein M, X, and n are as previously defined, and a process of preparing such actinide metal compounds are described including admixing the actinide metal in an aprotic Lewis base as a coordinating solvent in the presence of a halogen-containing oxidant.

  6. Actinide halide complexes

    DOEpatents

    Avens, Larry R.; Zwick, Bill D.; Sattelberger, Alfred P.; Clark, David L.; Watkin, John G.

    1992-01-01

    A compound of the formula MX.sub.n L.sub.m wherein M is a metal atom selected from the group consisting of thorium, plutonium, neptunium or americium, X is a halide atom, n is an integer selected from the group of three or four, L is a coordinating ligand selected from the group consisting of aprotic Lewis bases having an oxygen-, nitrogen-, sulfur-, or phosphorus-donor, and m is an integer selected from the group of three or four for monodentate ligands or is the integer two for bidentate ligands, where the sum of n+m equals seven or eight for monodentate ligands or five or six for bidentate ligands, a compound of the formula MX.sub.n wherein M, X, and n are as previously defined, and a process of preparing such actinide metal compounds including admixing the actinide metal in an aprotic Lewis base as a coordinating solvent in the presence of a halogen-containing oxidant, are provided.

  7. Evaluation of actinide biosorption by microorganisms

    SciTech Connect

    Happel, A.M.

    1996-06-01

    Conventional methods for removing metals from aqueous solutions include chemical precipitation, chemical oxidation or reduction, ion exchange, reverse osmosis, electrochemical treatment and evaporation. The removal of radionuclides from aqueous waste streams has largely relied on ion exchange methods which can be prohibitively costly given increasingly stringent regulatory effluent limits. The use of microbial cells as biosorbants for heavy metals offers a potential alternative to existing methods for decontamination or recovery of heavy metals from a variety of industrial waste streams and contaminated ground waters. The toxicity and the extreme and variable conditions present in many radionuclide containing waste streams may preclude the use of living microorganisms and favor the use of non-living biomass for the removal of actinides from these waste streams. In the work presented here, we have examined the biosorption of uranium by non-living, non-metabolizing microbial biomass thus avoiding the problems associated with living systems. We are investigating biosorption with the long term goal of developing microbial technologies for the remediation of actinides.

  8. Thermally unstable complexants/phosphate mineralization of actinides

    SciTech Connect

    Nash, K.

    1996-10-01

    In situ immobilization is an approach to isolation of radionuclides from the hydrosphere that is receiving increasing attention. Rather than removing the actinides from contaminated soils, this approach transforms the actinides into intrinsically insoluble mineral phases resistant to leaching by groundwater. The principal advangates of this concept are the low cost and low risk of operator exposure and/or dispersion of the radionuclides to the wider environment. The challenge of this approach is toe accomplish the immobilization without causing collateral damage to the environment (the cure shouldn`t be worse than the disease) and verification of system performance.

  9. Managing Inventories of Heavy Actinides

    SciTech Connect

    Wham, Robert M; Patton, Bradley D

    2011-01-01

    The Department of Energy (DOE) has stored a limited inventory of heavy actinides contained in irradiated targets, some partially processed, at the Savannah River Site (SRS) and Oak Ridge National Laboratory (ORNL). The 'heavy actinides' of interest include plutonium, americium, and curium isotopes; specifically 242Pu and 244Pu, 243Am, and 244/246/248Cm. No alternate supplies of these heavy actinides and no other capabilities for producing them are currently available. Some of these heavy actinide materials are important for use as feedstock for producing heavy isotopes and elements needed for research and commercial application. The rare isotope 244Pu is valuable for research, environmental safeguards, and nuclear forensics. Because the production of these heavy actinides was made possible only by the enormous investment of time and money associated with defense production efforts, the remaining inventories of these rare nuclear materials are an important part of the legacy of the Nuclear Weapons Program. Significant unique heavy actinide inventories reside in irradiated Mark-18A and Mark-42 targets at SRS and ORNL, with no plans to separate and store the isotopes for future use. Although the costs of preserving these heavy actinide materials would be considerable, for all practical purposes they are irreplaceable. The effort required to reproduce these heavy actinides today would likely cost billions of dollars and encompass a series of irradiation and chemical separation cycles for at least 50 years; thus, reproduction is virtually impossible. DOE has a limited window of opportunity to recover and preserve these heavy actinides before they are disposed of as waste. A path forward is presented to recover and manage these irreplaceable National Asset materials for future use in research, nuclear forensics, and other potential applications.

  10. Nuclear waste forms for actinides.

    PubMed

    Ewing, R C

    1999-03-30

    The disposition of actinides, most recently 239Pu from dismantled nuclear weapons, requires effective containment of waste generated by the nuclear fuel cycle. Because actinides (e.g., 239Pu and 237Np) are long-lived, they have a major impact on risk assessments of geologic repositories. Thus, demonstrable, long-term chemical and mechanical durability are essential properties of waste forms for the immobilization of actinides. Mineralogic and geologic studies provide excellent candidate phases for immobilization and a unique database that cannot be duplicated by a purely materials science approach. The "mineralogic approach" is illustrated by a discussion of zircon as a phase for the immobilization of excess weapons plutonium.

  11. Actinide Burning in CANDU Reactors

    SciTech Connect

    Hyland, B.; Dyck, G.R.

    2007-07-01

    Actinide burning in CANDU reactors has been studied as a method of reducing the actinide content of spent nuclear fuel from light water reactors, and thereby decreasing the associated long term decay heat load. In this work simulations were performed of actinides mixed with natural uranium to form a mixed oxide (MOX) fuel, and also mixed with silicon carbide to form an inert matrix (IMF) fuel. Both of these fuels were taken to a higher burnup than has previously been studied. The total transuranic element destruction calculated was 40% for the MOX fuel and 71% for the IMF. (authors)

  12. Basic Characteristics of Bis(2-ethylhexyl)phosphate-impregnated Adsorbent Used for Separation of Minor Actinides from FBR-Spent Fuel

    NASA Astrophysics Data System (ADS)

    Oda, Ryohei; Arai, Tsuyoshi; Nagayama, Katsuhisa; Watanabe, Sou; Sano, Yuichi; Myouchin, Munetaka

    FBR-spent nuclear fuel includes a great deal of minor actinides (MA: Am and Cm), which become febrile. Radioactive wastes including MA require a large area of ground for dumping and result in high cost. In Fast Reactor Cycel System Technology Development Project (FaCT) in Japan, we have been investigating extraction chromatography for separation of long-lived MA and specific fission products (FP) from high-level liquid wastes (HLLW). This method is expected to allow us to reduce an organic solvent use and to realize compact equipment. In this work, we have studied the static and dynamic adsorption behavior of representative FP contained in HLLW, Mo(VI), Zr(IV), Nd(III) and EU(III), on a bis(2-ethylhexyl)phosphate (HDEHP)-impregnated adsorbent. Such fundamental data should facilitate the efficient design of efficient MA recovery processes. Column adsorption experiments with the HDEHP-impregnated adsorbent have revealed that an increase in a flow rate results in a short breakthrough time and reduces the adsorption capacity of the column for all the elements tested. These results strongly suggest that a lower flow rate is preferable to enhance the adsorption capacity of the adsorbent.

  13. Actinide biocolloid formation in brine by halophilic bacteria

    SciTech Connect

    Gillow, J.B.; Francis, A.J.; Dodge, C.J.; Harris, R.; Beveridge, T.J.; Brady, P.V.; Papenguth, H.W.

    1998-12-31

    The authors examined the ability of a halophilic bacterium (WIPP 1A) isolated from the Waste Isolation Pilot Plant (WIPP) site to accumulate uranium in order to determine the potential for biocolloid facilitated actinide transport. The bacterial cell surface functional groups involved in the complexation of the actinide were determined by titration. Uranium, added as uranyl nitrate, was removed from solution at pH 5 by cells but at pH 7 and 9 very little uranium was removed due to its limited solubility. Although present as soluble species, uranyl citrate at pH 5, 7, and 9, and uranyl carbonate at pH 9 were not removed by the bacterium because they were not bioavailable due to their neutral or negative charge. Addition of uranyl EDTA to brine at pH 5, 7, and 9 resulted in the immediate precipitation of U. Transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDS) analysis revealed that uranium was not only associated with the cell surface but also accumulated intracellularly as uranium-enriched granules. Extended X-ray absorption fine structure (EXAFS) analysis of the bacterial cells indicated the bulk sample contained more than one uranium phase. Nevertheless these results show the potential for the formation of actinide bearing bacterial biocolloids that are strictly regulated by the speciation and bioavailability of the actinide.

  14. Actinide Biocolloid Formation in Brine by Halophilic Bacteria

    SciTech Connect

    Gillow, J.B.; Francis, A.J.; Dodge, C.J.; Harris, R.; Beveridge, T.J.; Brady, P.V.; Papenguth, H.W.

    1999-07-28

    We examined the ability of a halophilic bacterium (WFP 1A) isolated from the Waste Isolation Pilot Plant (WIPP) site to accumulate uranium in order to determine the potential for biocolloid facilitated actinide transport. The bacterial cell Surface functional groups involved in the complexation of the actinide were determined by titration. Uranium, added as uranyl nitrate, was removed from solution at pH 5 by cells but at pH 7 and 9 very little uranium was removed due to its limited volubility. Although present as soluble species, uranyl citrate at pH 5, 7, and 9, and uranyl carbonate at pH 9 were not removed by the bacterium because they were not bioavailable due to their neutral or negative charge. Addition of uranyl EDTA to brine at pH 5, 7, and 9 resulted in the immediate precipitation of U. Transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDS) analysis revealed that uranium was not only associated with the cell surface but also accumulated intracellulary as uranium-enriched granules. Extended X-ray absorption fine structure (EXAFS) analysis, of the bacterial cells indicated the bulk sample contained more than one uranium phase. Nevertheless these results show the potential for the formation of actinide bearing bacterial biocolloids that are strictly regulated by the speciation and bioavailability of the actinide.

  15. ACTINIDE BIOCOLLOID FORMATION IN BRINE BY HALOPHILIC BACTERIA

    SciTech Connect

    GILLOW,J.B.; FRANCIS,A.J.; DODGE,C.J.; HARRIS,R.; BEVERIDGE,T.J.; BRADY,P.B.; PAPENGUTH,H.W.

    1998-11-09

    The authors examined the ability of a halophilic bacterium (WIPP 1A) isolated from the Waste Isolation Pilot Plant (WIPP) site to accumulate uranium in order to determine the potential for biocolloid facilitated actinide transport. The bacterial cell surface functional groups involved in the complexation of the actinide were determined by titration. Uranium, added as uranyl nitrate, was removed from solution at pH 5 by cells but at pH 7 and 9 very little uranium was removed due to its limited solubility. Although present as soluble species, uranyl citrate at pH 5, 7, and 9, and uranyl carbonate at pH 9 were not removed by the bacterium because they were not bioavailable due to their neutral or negative charge. Addition of uranyl EDTA to brine at pH 5, 7, and 9 resulted in the immediate precipitation of U. Transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDS) analysis revealed that uranium was not only associated with the cell surface but also accumulated intracellularly as uranium-enriched granules. Extended X-ray absorption fine structure (EXAFS) analysis of the bacterial cells indicated the bulk sample contained more than one uranium phase. Nevertheless these results show the potential for the formation of actinide bearing bacterial biocolloids that are strictly regulated by the speciation and bioavailability of the actinide.

  16. Environmental research on actinide elements

    SciTech Connect

    Pinder, J.E. III; Alberts, J.J.; McLeod, K.W.; Schreckhise, R.G.

    1987-08-01

    The papers synthesize the results of research sponsored by DOE's Office of Health and Environmental Research on the behavior of transuranic and actinide elements in the environment. Separate abstracts have been prepared for the 21 individual papers. (ACR)

  17. Actinide transmutation in nuclear reactors

    SciTech Connect

    Ganev, I.K.; Lopatkin, A.V.; Naumov, V.V.; Tocheny, L.V.

    1993-12-31

    Of some interest is the comparison between the actinide nuclide burning up (fission) rates such as americium 241, americium 242, curium 244, and neptunium 237, in the reactors with fast or thermal neutron spectra.

  18. Method for fluorination of actinide fluorides and oxyfluorides thereof using O[sub 2]F[sub 2

    DOEpatents

    Eller, P.G.; Malm, J.G.; Penneman, R.A.

    1988-11-08

    Method is described for fluorination of actinides and fluorides and oxyfluorides thereof using O[sub 2]F[sub 2] which generates actinide hexafluorides, and for removal of actinides and compounds thereof from surfaces upon which they appear as unwanted deposits. The fluorinating agent, O[sub 2]F[sub 2], has been observed to readily perform the above-described tasks at sufficiently low temperatures that there is virtually no damage to the containment vessels. Moreover, the resulting actinide hexafluorides are thereby not destroyed by high temperature reactions with the walls of the reaction vessel. Dioxygen difluoride is easily prepared, stored and transferred to the desired place of reaction.

  19. Method for fluorination of actinide fluorides and oxyfluorides thereof using O.sub.2 F.sub.2

    DOEpatents

    Eller, Phillip G.; Malm, John G.; Penneman, Robert A.

    1988-01-01

    Method for fluorination of actinides and fluorides and oxyfluorides thereof using O.sub.2 F.sub.2 which generates actinide hexafluorides, and for removal of actinides and compounds thereof from surfaces upon which they appear as unwanted deposits. The fluorinating agent, O.sub.2 F.sub.2, has been observed to readily perform the above-described tasks at sufficiently low temperatures that there is virtually no damage to the containment vessels. Moreover, the resulting actinide hexafluorides are thereby not destroyed by high temperature reactions with the walls of the reaction vessel. Dioxygen difluoride is easily prepared, stored and transferred to the desired place of reaction.

  20. Advanced Aqueous Separation Systems for Actinide Partitioning

    SciTech Connect

    Nash, Ken; Martin, Leigh; Lumetta, Gregg

    2015-04-02

    One of the most challenging aspects of advanced processing of used nuclear fuel is the separation of transplutonium actinides from fission product lanthanides. This separation is essential if actinide transmutation options are to be pursued in advanced fuel cycles, as lanthanides compete with actinides for neutrons in both thermal and fast reactors, thus limiting efficiency. The separation is difficult because the chemistry of Am3+ and Cm3+ is nearly identical to that of the trivalent lanthanides (Ln3+). The prior literature teaches that two approaches offer the greatest probability of devising a successful group separation process based on aqueous processes: 1) the application of complexing agents containing ligand donor atoms that are softer than oxygen (N, S, Cl-) or 2) changing the oxidation state of Am to the IV, V, or VI state to increase the essential differences between Am and lanthanide chemistry (an approach utilized in the PUREX process to selectively remove Pu4+ and UO22+ from fission products). The latter approach offers the additional benefit of enabling a separation of Am from Cm, as Cm(III) is resistant to oxidation and so can easily be made to follow the lanthanides. The fundamental limitations of these approaches are that 1) the soft(er) donor atoms that interact more strongly with actinide cations than lanthanides form substantially weaker bonds than oxygen atoms, thus necessitating modification of extraction conditions for adequate phase transfer efficiency, 2) soft donor reagents have been seen to suffer slow phase transfer kinetics and hydro-/radiolytic stability limitations and 3) the upper oxidation states of Am are all moderately strong oxidants, hence of only transient stability in media representative of conventional aqueous separations systems. There are examples in the literature of both approaches having been described. However, it is not clear at present that any extant process is sufficiently robust for application at the scale

  1. Removal characteristics of plasma chemical vaporization machining with a pipe electrode for optical fabrication

    SciTech Connect

    Takino, Hideo; Yamamura, Kazuya; Sano, Yasuhisa; Mori, Yuzo

    2010-08-10

    Plasma chemical vaporization machining (CVM) is a high-precision chemical shaping method using rf plasma generated in the proximity of an electrode in an atmospheric environment. The purpose of the present study is to clarify the removal characteristics of plasma CVM using a pipe electrode. Polished fused silica plates were processed by plasma CVM, polishing, and precision grinding under various conditions. The removal rate of plasma CVM was about 4 to 1100 times faster than that of polishing, and the maximum removal rate was almost equal to that of precision grinding. The roughness of the resultant surfaces was almost the same as that of the polished surfaces.

  2. RAPID SEPARATION OF ACTINIDES AND RADIOSTRONTIUM IN VEGETATION SAMPLES

    SciTech Connect

    Maxwell, S.

    2010-06-01

    A new rapid method for the determination of actinides and radiostrontium in vegetation samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used in emergency response situations or for routine analysis. The actinides in vegetation method utilizes a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step, and a streamlined column separation process with stacked TEVA, TRU and DGA Resin cartridges. Lanthanum was separated rapidly and effectively from Am and Cm on DGA Resin. Alpha emitters are prepared using rare earth microprecipitation for counting by alpha spectrometry. The purified {sup 90}Sr fractions are mounted directly on planchets and counted by gas flow proportional counting. The method showed high chemical recoveries and effective removal of interferences. The actinide and {sup 90}Sr in vegetation sample analysis can be performed in less than 8 h with excellent quality for emergency samples. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory actinide particles or vegetation residue after furnace heating is effectively digested.

  3. TAILORING INORGANIC SORBENTS FOR SRS STRONTIUM AND ACTINIDE SEPARATIONS: OPTIMIZED MONOSODIUM TITANATEPHASE II INTERIM REPORT FOR EXTERNAL RELEASE

    SciTech Connect

    Hobbs, D; Michael Poirier, M; Mark Barnes, M; Mary Thompson, M

    2006-08-31

    This document provides an interim summary report of Phase II testing activities for the development of a modified monosodium titanate (MST) that exhibits improved strontium and actinide removal characteristics compared to the baseline MST materials. The activities included determining the key synthesis conditions for preparation of the modified MST, preparation of the modified MST at a larger laboratory scale, demonstration of the strontium and actinide removal characteristics with actual tank waste supernate and characterization of the modified MST. Key findings and conclusions include the following: (1) Samples of the modified MST prepared by Method 2 and Method 3 exhibited the best combination of strontium and actinide removal. (2) We selected Method 3 to scale up and test performance with actual waste solution. (3) We successfully prepared three batches of the modified MST using the Method 3 procedure at a 25-gram scale. (4) Performance tests indicated successful scale-up to the 25-gram scale with excellent performance and reproducibility among each of the three batches. For example, the plutonium decontamination factors (6-hour contact time) for the modified MST samples averaged 13 times higher than that of the baseline MST sample at half the sorbent concentration (0.2 g L{sup -1} for modified MST versus 0.4 g L{sup -1} for baseline MST). (5) Performance tests with actual waste supernate demonstrated that the modified MST exhibited better strontium and plutonium removal performance than that of the baseline MST. For example, the decontamination factors for the modified MST measured 2.6 times higher for strontium and between 5.2 to 11 times higher for plutonium compared to the baseline MST sample. The modified MST did not exhibit improved neptunium removal performance over that of the baseline MST. (6) Two strikes of the modified MST provided increased removal of strontium and actinides from actual waste compared to a single strike. The improved performance

  4. Kinetics of actinide complexation reactions

    SciTech Connect

    Nash, K.L.; Sullivan, J.C.

    1997-09-01

    Though the literature records extensive compilations of the thermodynamics of actinide complexation reactions, the kinetics of complex formation and dissociation reactions of actinide ions in aqueous solutions have not been extensively investigated. In light of the central role played by such reactions in actinide process and environmental chemistry, this situation is somewhat surprising. The authors report herein a summary of what is known about actinide complexation kinetics. The systems include actinide ions in the four principal oxidation states (III, IV, V, and VI) and complex formation and dissociation rates with both simple and complex ligands. Most of the work reported was conducted in acidic media, but a few address reactions in neutral and alkaline solutions. Complex formation reactions tend in general to be rapid, accessible only to rapid-scan and equilibrium perturbation techniques. Complex dissociation reactions exhibit a wider range of rates and are generally more accessible using standard analytical methods. Literature results are described and correlated with the known properties of the individual ions.

  5. 33rd Actinide Separations Conference

    SciTech Connect

    McDonald, L M; Wilk, P A

    2009-05-04

    Welcome to the 33rd Actinide Separations Conference hosted this year by the Lawrence Livermore National Laboratory. This annual conference is centered on the idea of networking and communication with scientists from throughout the United States, Britain, France and Japan who have expertise in nuclear material processing. This conference forum provides an excellent opportunity for bringing together experts in the fields of chemistry, nuclear and chemical engineering, and actinide processing to present and discuss experiences, research results, testing and application of actinide separation processes. The exchange of information that will take place between you, and other subject matter experts from around the nation and across the international boundaries, is a critical tool to assist in solving both national and international problems associated with the processing of nuclear materials used for both defense and energy purposes, as well as for the safe disposition of excess nuclear material. Granlibakken is a dedicated conference facility and training campus that is set up to provide the venue that supports communication between scientists and engineers attending the 33rd Actinide Separations Conference. We believe that you will find that Granlibakken and the Lake Tahoe views provide an atmosphere that is stimulating for fruitful discussions between participants from both government and private industry. We thank the Lawrence Livermore National Laboratory and the United States Department of Energy for their support of this conference. We especially thank you, the participants and subject matter experts, for your involvement in the 33rd Actinide Separations Conference.

  6. Characteristics and transformations of dissolved organic nitrogen in municipal biological nitrogen removal wastewater treatment plants

    NASA Astrophysics Data System (ADS)

    Huo, Shouliang; Xi, Beidou; Yu, Honglei; Qin, Yanwen; Zan, Fengyu; Zhang, Jingtian

    2013-12-01

    Dissolved organic nitrogen (DON) represents most of the dissolved nitrogen in the effluent of biological nitrogen removal (BNR) wastewater treatment plants (WWTPs). The characteristics of wastewater-derived DON in two different WWTPs were investigated by several different methods. The major removals of DON and biodegradable dissolved organic nitrogen (BDON) along the treatment train were observed in the anaerobic process. Dissolved combined amino acids (DCAA) and dissolved free amino acids (DFAA) in the effluent accounted approximately for less than 4% and 1% of the effluent DON, respectively. Approximately half of wastewater-derived DON was capable of passing through a 1 kDa ultrafilter, and low MW DON cannot effectively be removed by BNR processes. More than 80% of effluent DON was composed of hydrophilic compounds, which stimulate algal growth. The study provided important information for future upgrading of WWTPs or the selection of DON removal systems to meet more demanding nitrogen discharge limits.

  7. Comparison of the biological NH3 removal characteristics among four inorganic packing materials.

    PubMed

    Hirai, M; Kamamoto, M; Yani, M; Shoda, M

    2001-01-01

    Four inorganic packing materials were evaluated in terms of their availability as a packing material of a packed tower deodorization apparatus (biofilter) from the viewpoints of biological NH3 removal characteristics and some physical properties. Porous ceramics (A), calcinated cristobalite (B), calcinated and formed obsidian (C), granulated and calculated soil (D) were used. The superiority of these packing materials determined based on the values of non-biological removal per unit weight or unit volume of packing material, complete removal capacity of NH3 per unit weight of packing material per day or unit volume of packing material per day and pressure drop of the packed bed was in the order of A approximately = C > B > or = D. Packing materials A and C with high porosity, maximum water content, and suitable mean pore diameter showed excellent removal capacity.

  8. Moisture removal characteristics of thin layer rough rice under sequenced infrared radiation heating and cooling

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Rice drying with infrared (IR) radiation has been investigated during recent years and showed promising potential with improved quality and energy efficiency. The objective of this study was to further investigate the moisture removal characteristics of thin layer rough rice heated by IR and cooled ...

  9. Nitrate removal and denitrification affected by soil characteristics in nitrate treatment wetlands.

    PubMed

    Lin, Ying-Feng; Jing, Shuh-Ren; Lee, Der-Yuan; Chang, Yih-Feng; Shih, Kai-Chung

    2007-03-01

    Several small-scale surface flow constructed wetlands unplanted and planted (monoculture) with various macrophytes (Phragmites australis, Typha orientalis, Pennisetum purpureum, Ipomoea aquatica, and Pistia stratiotes) were established to continuously receive nitrate-contaminated groundwater. Soil characteristics and their effects on nitrate removal and soil denitrification were investigated. The results showed that planted wetland cells exhibited significantly higher (P < 0.05) nitrate removal efficiencies (70-99%) and soil denitrification rates (3.78-15.02 microg N2O-N/g dry soil/h) than an unplanted covered wetland cell (1%, 0.11 microg N2O-N/g/h). However, the unplanted uncovered wetland cell showed a nitrate removal efficiency (55%) lower than but a soil denitrification rate (9.12 microg N2O-N/g/h) comparable to the planted cells. The nitrate removal rate correlated closely and positively with the soil denitrification rate for the planted cells, indicating that soil denitrification is an important process for removing nitrate in constructed wetlands. The results of nitrogen budget revealed that around 68.9-90.7% of the overall nitrogen removal could be attributed to the total denitrification. The soil denitrification rate was found to correlate significantly (P < 0.01) with the extractable organic carbon, organic matter, and in situ-measured redox potential of wetland soil, which accordingly were concluded as suitable indicators of soil denitrification rate and nitrate removal rate in nitrate treatment wetlands.

  10. [Characteristics of nitrogen and phosphorus removal and control of membrane fouling in MBR and SMBR].

    PubMed

    Guo, Xiao-Ma; Zhao, Yan; Wang, Kai-Yan; Zhao Yang-Guo

    2015-03-01

    To improve the efficiency and running stability of wastewater advanced treatment, a sequencing membrane bioreactor (SMBR) and a traditional membrane bioreactor (MBR) were used to investigate the characteristics of nitrogen and phosphorus removal, and the effect of anoxic time on treatment systems and membrane fouling. Simultaneously, molecular biology techniques were applied to analyze the composition of microbial community and the structure of suspended sludge. The results showed that SMBR had higher efficiency in removing TN than MBR, which indicated that intermittent aeration could enhance the ability of nitrogen removal. SMBR and MBR had a similar removal efficiency of NH4(+)-N, TP, COD, and turbidity with the removal rates of 94%, 78%, 80%, and 97%, respectively. Extension of SMBR anoxic time had no effect on COD, NH4(+) -N removal but decreased TN and TP removal rate, dropping from 61% and 74% to 46% and 52%, respectively. Intermittent aeration and powder activated carbon (PAC) could both mitigate membrane fouling. The analysis on microbial community indicated that there was no difference in the composition and structure of microbial community between SMBR and MBR. Nitrospira and Dechloromonas were both highly abundant functional groups, which provided the basis for highly efficient control of bioreactors.

  11. Experimental Investigation of Material Removal Characteristics in Silicon Chemical Mechanical Polishing

    NASA Astrophysics Data System (ADS)

    Park, Boumyoung; Jeong, Sukhoon; Lee, Hyunseop; Kim, Hyoungjae; Jeong, Haedo; Dornfeld, David A.

    2009-11-01

    The material removal characteristics of a silicon wafer were experimentally investigated with respect to the chemical dissolution and mechanical abrasion of the wafer during silicon chemical mechanical polishing (CMP) using an alkali-based slurry. The silicon surface without native oxide is rapidly dissolved by the slurry containing an amine agent, which effectively leads to the reduced hardness of the loaded silicon wafer due to Si-Si bond breaking during polishing. The abrasive particles in the slurry easily remove the reacted silicon surface, and the removal rate and wafer non-uniformity for abrasive concentrations of 1.5-3 wt % are better than those for other concentrations because of the low and steady coefficient of friction (COF) owing to the evenness of abrasive particles between the wafer and pad. Also, it was found that a high slurry flow rate of 700-1000 cm3/min improves wafer non-uniformity owing to the reduced temporal variation of temperature, because the slurry acts as a good cooling source during polishing. However, the removal rate remains almost constant upon varying the slurry flow rate because of the effective dissolution characteristic of the slurry with abundant amine as an accelerator, regardless of the reduction of average temperature with increasing slurry flow rate. In the break-in process used to stabilize the material removal, the viscoelastic behaviors of the pad and the ground wafer surface with native oxide and wheel marks cause a temporal change of the friction force during polishing, which is related to the removal rate and wafer non-uniformity. As a result, the stabilization of removal rate and wafer non-uniformity is achieved through a steady-state process with elevated temperature and reduced COF after a total polishing time of 60 min, based on the removal process of the wafer surface and the permanent deformation in the viscoelastic behavior of the pad.

  12. Nuclear waste forms for actinides

    PubMed Central

    Ewing, Rodney C.

    1999-01-01

    The disposition of actinides, most recently 239Pu from dismantled nuclear weapons, requires effective containment of waste generated by the nuclear fuel cycle. Because actinides (e.g., 239Pu and 237Np) are long-lived, they have a major impact on risk assessments of geologic repositories. Thus, demonstrable, long-term chemical and mechanical durability are essential properties of waste forms for the immobilization of actinides. Mineralogic and geologic studies provide excellent candidate phases for immobilization and a unique database that cannot be duplicated by a purely materials science approach. The “mineralogic approach” is illustrated by a discussion of zircon as a phase for the immobilization of excess weapons plutonium. PMID:10097054

  13. Actinides and Life's Origins

    NASA Astrophysics Data System (ADS)

    Adam, Zachary

    2007-12-01

    There are growing indications that life began in a radioactive beach environment. A geologic framework for the origin or support of life in a Hadean heavy mineral placer beach has been developed, based on the unique chemical properties of the lower-electronic actinides, which act as nuclear fissile and fertile fuels, radiolytic energy sources, oligomer catalysts, and coordinating ions (along with mineralogically associated lanthanides) for prototypical prebiotic homonuclear and dinuclear metalloenzymes. A four-factor nuclear reactor model was constructed to estimate how much uranium would have been required to initiate a sustainable fission reaction within a placer beach sand 4.3 billion years ago. It was calculated that about 1-8 weight percent of the sand would have to have been uraninite, depending on the weight percent, uranium enrichment, and quantity of neutron poisons present within the remaining placer minerals. Radiolysis experiments were conducted with various solvents with the use of uranium- and thorium-rich minerals (metatorbernite and monazite, respectively) as proxies for radioactive beach sand in contact with different carbon, hydrogen, oxygen, and nitrogen reactants. Radiation bombardment ranged in duration of exposure from 3 weeks to 6 months. Low levels of acetonitrile (estimated to be on the order of parts per billion in concentration) were conclusively identified in 2 setups and tentatively indicated in a 3rd by gas chromatography/mass spectrometry. These low levels have been interpreted within the context of a Hadean placer beach prebiotic framework to demonstrate the promise of investigating natural nuclear reactors as power production sites that might have assisted the origins of life on young rocky planets with a sufficiently differentiated crust/mantle structure. Future investigations are recommended to better quantify the complex relationships between energy release, radioactive grain size, fissionability, reactant phase, phosphorus

  14. Actinides and Life's Origins.

    PubMed

    Adam, Zachary

    2007-12-01

    There are growing indications that life began in a radioactive beach environment. A geologic framework for the origin or support of life in a Hadean heavy mineral placer beach has been developed, based on the unique chemical properties of the lower-electronic actinides, which act as nuclear fissile and fertile fuels, radiolytic energy sources, oligomer catalysts, and coordinating ions (along with mineralogically associated lanthanides) for prototypical prebiotic homonuclear and dinuclear metalloenzymes. A four-factor nuclear reactor model was constructed to estimate how much uranium would have been required to initiate a sustainable fission reaction within a placer beach sand 4.3 billion years ago. It was calculated that about 1-8 weight percent of the sand would have to have been uraninite, depending on the weight percent, uranium enrichment, and quantity of neutron poisons present within the remaining placer minerals. Radiolysis experiments were conducted with various solvents with the use of uraniumand thorium-rich minerals (metatorbernite and monazite, respectively) as proxies for radioactive beach sand in contact with different carbon, hydrogen, oxygen, and nitrogen reactants. Radiation bombardment ranged in duration of exposure from 3 weeks to 6 months. Low levels of acetonitrile (estimated to be on the order of parts per billion in concentration) were conclusively identified in 2 setups and tentatively indicated in a 3(rd) by gas chromatography/mass spectrometry. These low levels have been interpreted within the context of a Hadean placer beach prebiotic framework to demonstrate the promise of investigating natural nuclear reactors as power production sites that might have assisted the origins of life on young rocky planets with a sufficiently differentiated crust/mantle structure. Future investigations are recommended to better quantify the complex relationships between energy release, radioactive grain size, fissionability, reactant phase, phosphorus

  15. Removal characteristics of sulfuric acid aerosols from coal-fired power plants.

    PubMed

    Pan, Danping; Yang, Linjun; Wu, Hao; Huang, Rongting

    2017-03-01

    With increasing attention on sulfuric acid emission, investigations on the removal characteristics of sulfuric acid aerosols by the limestone gypsum wet flue gas desulfurization (WFGD) system and the wet electrostatic precipitator (WESP) were carried out in two coal-fired power plants, and the effects of the WFGD scrubber type and the flue gas characteristics were discussed. The results showed that it was necessary to install the WESP device after desulfurization, as the WFGD system was inefficient to remove sulfuric acid aerosols from the flue gas. The removal efficiency of sulfuric acid aerosols in the WFGD system with double scrubbers ranged from 50% to 65%, which was higher than that with a single scrubber, ranging from 30% to 40%. Furthermore, the removal efficiency of WESP on the sulfuric acid aerosols was from 47.9% to 52.4%. With increased concentrations of SO3 and particles in the flue gas, the removal efficiencies of the WFGD and the WESP on the sulfuric acid aerosols were increased.

  16. Preliminary considerations concerning actinide solubilities

    SciTech Connect

    Newton, T.W.; Bayhurst, B.P.; Daniels, W.R.; Erdal, B.R.; Ogard, A.E.

    1980-01-01

    Work at the Los Alamos Scientific Laboratory on the fundamental solution chemistry of the actinides has thus far been confined to preliminary considerations of the problems involved in developing an understanding of the precipitation and dissolution behavior of actinide compounds under environmental conditions. Attempts have been made to calculate solubility as a function of Eh and pH using the appropriate thermodynamic data; results have been presented in terms of contour maps showing lines of constant solubility as a function of Eh and pH. Possible methods of control of the redox potential of rock-groundwater systems by the use of Eh buffers (redox couples) is presented.

  17. Actinide chemistry in ionic liquids.

    PubMed

    Takao, Koichiro; Bell, Thomas James; Ikeda, Yasuhisa

    2013-04-01

    This Forum Article provides an overview of the reported studies on the actinide chemistry in ionic liquids (ILs) with a particular focus on several fundamental chemical aspects: (i) complex formation, (ii) electrochemistry, and (iii) extraction behavior. The majority of investigations have been dedicated to uranium, especially for the 6+ oxidation state (UO2(2+)), because the chemistry of uranium in ordinary solvents has been well investigated and uranium is the most abundant element in the actual nuclear fuel cycles. Other actinides such as thorium, neptunium, plutonium, americium, and curiumm, although less studied, are also of importance in fully understanding the nuclear fuel engineering process and the safe geological disposal of radioactive wastes.

  18. Actinide Thermodynamics at Elevated Temperatures

    SciTech Connect

    Friese, Judah I.; Rao, Linfeng; Xia, Yuanxian; Bachelor, Paula P.; Tian, Guoxin

    2007-11-16

    The postclosure chemical environment in the proposed Yucca Mountain repository is expected to experience elevated temperatures. Predicting migration of actinides is possible if sufficient, reliable thermodynamic data on hydrolysis and complexation are available for these temperatures. Data are scarce and scattered for 25 degrees C, and nonexistent for elevated temperatures. This collaborative project between LBNL and PNNL collects thermodynamic data at elevated temperatures on actinide complexes with inorganic ligands that may be present in Yucca Mountain. The ligands include hydroxide, fluoride, sulfate, phosphate and carbonate. Thermodynamic parameters of complexation, including stability constants, enthalpy, entropy and heat capacity of complexation, are measured with a variety of techniques including solvent extraction, potentiometry, spectrophotometry and calorimetry

  19. Fruit characteristics and factors affecting fruit removal in a Panamanian community of strangler figs.

    PubMed

    Korine, C; Kalko, E K V; Herre, E A

    2000-06-01

    We describe fruiting characteristics for 12 species in a community of strangler figs (Moraceae: Urostigma) studied in Panama. We quantify diurnal and nocturnal removal rates and proportions of fruits removed, and relate them to the activities of the main dispersers of the figs: bats and birds. These results combined with previous studies show that there are clear differences between fig species with fruit that ripen red and those with fruit that remain green(ish). In the red-fruited species, the fruit are small, ripen asynchronously over relatively long periods, produce little scent, and are mainly taken during the day by birds. In contrast, in the green(ish)-fruited species, the fruits are larger, span a range of sizes, ripen relatively synchronously, produce very distinctive aromas, and are mainly taken at night by bats. This dichotomy in fruiting characteristics suggests coadaptive links between groups of dispersers and different species within the genus Ficus. All fig species produce a range of fruit crop sizes (10-155 fuits/m(2) canopy area) of which a high proportion were removed by seed dispersers (>80%). Removal rates (fruit removed per day) were positively correlated with crop size, suggesting that trees with large crop size attract more frugivores. Removal rates of green-fruited figs were significantly lower and persistence and abortion of ripe fruit were significant higher around full moon, apparently due to the reduced activity of bats. We further estimate the number of bats that are sustained by a tree fruit crop and account for the observed fruit removal. We then discuss the evidence for coadaptation between different groups of figs and their seed dispersers, Finally, we consider the conservation implications for figs as keystone resources in tropical forests.

  20. Phytosiderophore Effects on Subsurface Actinide Contaminants: Potential for Phytostabilization and Phytoextraction

    SciTech Connect

    Ruggiero, Christy

    2005-06-01

    This project seeks to understand the influence of phytosiderophore-producing plants (grasses, including crops such as wheat and barley) on the biogeochemistry of actinide and other metal contaminants in the subsurface environment, and to determine the potential of phytosiderophore-producing plants for phytostabilization and phytoextraction of actinides and some metal soil contaminants. Phytosiderophores are secreted by graminaceous plants such as barley and wheat for the solubilization, mobilization and uptake of Fe and other essential nutrients from soils. The ability for these phytosiderophores to chelate and absorb actinides using the same uptake system as for Fe is being investigated though characterization of actinide-phytosiderophore complexes (independently of plants), and characterization of plant uptake of such complexes. We may also show possible harm caused by these plants through increased chelation of actinides that increase in actinide mobilization & migration in the subsurface environment. This information can then be directly applied by either removal of harmful plants, or can be used to develop plant-based soil stabilization/remediation technologies. Such technologies could be the low-cost, low risk solution to many DOE actinide contamination problems.

  1. Phytosiderophore Effects on Subsurface Actinide Contaminants: Potential for Phytostabilization and Phytoextraction

    SciTech Connect

    Ruggiero, Christy

    2004-06-01

    This project seeks to understand the influence of phytosiderophore-producing plants (grasses, including crops such as wheat and barley) on the biogeochemistry of actinide and other metal contaminants in the subsurface environment, and to determine the potential of phytosiderophoreproducing plants for phytostabilization and phytoextraction of actinides and some metal soil contaminants. Phytosiderophores are secreted by graminaceous plants such as barley and wheat for the solubilization, mobilization and uptake of Fe and other essential nutrients from soils. The ability for these phytosiderophores to chelate and absorb actinides using the same uptake system, as for Fe is being investigated though characterization of actinide-phytosiderophore complexes (independently of plants), and characterization of plant uptake of such complexes. We may also show possible harm caused by increased chelation of actinides, which may increase actinide mobilization & migration in the subsurface environment. This information can then be directly applied by either removal of harmful plants, or can be used to develop plant-based soil stabilization/remediation technologies. Such technologies could be the low-cost, low risk solution to many DOE actinide contamination problems.

  2. Combined effects of frequency and layer removal on background track characteristics of ECE polycarbonate detectors

    NASA Astrophysics Data System (ADS)

    Sohrabi, Mehdi; Soltani, Zahra; Hakimi, Amir

    2016-02-01

    Polycarbonate track detectors (PCTD) when electrochemically etched (ECE) provide excellent characteristics for registering relatively lower-LET charged particles (e.g. alphas, fast-neutron-induced recoils) for many health physics and ion detection applications.The layer removal method of PCTDs by ethylenediamine (EDA) developed in our laboratory reduces the background track (BGT) density significantly. The frequency of the applied electric field strongly affects the BGT density and diameter and thus affects the minimum detection limit (MDL). In order to study the combined effects of the frequency and layer removal on the BGT density and thus on the MDL, this research was conducted. The BGT density versus the layer thickness removed at frequencies up to 12 kHz decrease rapidly to about 10-20 μm above which they reach a minimum constant level, while the mean BGT diameter verses layer removed at all frequencies are constant with flat responses. On the other hand the BGT density and diameter versus frequency at different layers removed up to ~50 μm increase till 4 kHz above which they reach plateaus. The PCTDs with ~20 μm layer removal at frequencies up 1 to 2 kHz showed the lowest MDL. The results are presented and discussed.

  3. Separations of actinides, lanthanides and other metals

    DOEpatents

    Smith, Barbara F.; Jarvinen, Gordon D.; Ensor, Dale D.

    1995-01-01

    An organic extracting solution comprised of a bis(acylpyrazolone or a substituted bis(acylpyrazolone) and an extraction method useful for separating certain elements of the actinide series of the periodic table having a valence of four from one other, and also from one or more of the substances in a group consisting of hexavalent actinides, trivalent actinides, trivalent lanthanides, trivalent iron, trivalent aluminum, divalent metals, and monovalent metals and also from one or more of the substances in a group consisting of hexavalent actinides, trivalent actinides, trivalent lanthanides, trivalent iron, trivalent aluminum, divalent metals, and monovalent metals and also useful for separating hexavalent actinides from one or more of the substances in a group consisting of trivalent actinides, trivalent lanthanides, trivalent iron, trivalent aluminum, divalent metals, and monovalent metals.

  4. A literature review of actinide-carbonate mineral interactions

    SciTech Connect

    Stout, D.L.; Carroll, S.A.

    1993-10-01

    Chemical retardation of actinides in groundwater systems is a potentially important mechanism for assessing the performance of the Waste Isolation Pilot Plant (WIPP), a facility intended to demonstrate safe disposal of transuranic waste. Rigorous estimation of chemical retardation during transport through the Culebra Dolomite, a water-bearing unit overlying the WIPP, requires a mechanistic understanding of chemical reactions between dissolved elements and mineral surfaces. This report represents a first step toward this goal by examining the literature for pertinent experimental studies of actinide-carbonate interactions. A summary of existing models is given, along with the types of experiments on which these models are based. Articles pertaining to research into actinide interactions with carbonate minerals are summarized. Select articles involving trace element-carbonate mineral interactions are also reviewed and may serve as templates for future research. A bibliography of related articles is included. Americium(III), and its nonradioactive analog neodymium(III), partition strongly from aqueous solutions into carbonate minerals. Recent thermodynamic, kinetic, and surface studies show that Nd is preferentially removed from solution, forming a Nd-Ca carbonate solid solution. Neptunium(V) is rapidly removed from solution by carbonates. Plutonium incorporation into carbonates is complicated by multiple oxidation states. Little research has been done on the radium(H) and thorium(IV) carbonate systems. Removal of uranyl ion from solution by calcite is limited to monolayer surface coverage.

  5. Comparison of the biological H2S removal characteristics among four inorganic packing materials.

    PubMed

    Hirai, M; Kamamoto, M; Yani, M; Shoda, M

    2001-01-01

    Four inorganic packing materials were evaluated in terms of their availability as packing materials of a packed tower deodorization apparatus (biofilter) from the viewpoints of biological H2S removal characteristics and some physical properties. Among porous ceramics (A), calcinated cristobalite (B), calcinated and formed obsidian (C), granulated and calcinated soil (D), the superiority of these packing materials determined based on the values of non-biological removal per unit weight or unit volume of packing material, complete removal capacity of H2S per unit weight of packing material per day or unit volume of packing material per day and pressure drop of the packed bed was in the order of A approximately equal to C > D approximately equal to B, which is correlated with the maximum water content, porosity, and mean pore diameter.

  6. Molecular models for actinide speciation

    SciTech Connect

    Clark, D.L.; Watkin, J.G.; Morris, D.E.; Berg, J.M.

    1994-06-01

    Much effort has been devoted to the development of sensitive spectroscopic techniques for the study of actinide speciation based on the sensitivity of f-f electronic absorption bands to oxidation state and ligation of the actinide ions. These efforts assume that data obtained in such studies will be interpretable in terms of changes in complexation of the metal center. However, the current understanding of 5f electronic structure is based on data from solid state doped single crystals. In those studies, the local coordination geometry about the central actinide ion is maintained in an almost perfect high-symmetry environment and will have little relevance for species in solution where deviations from perfect high symmetry tend to be the rule rather than the exception. The authors have developed a vigorous research program in the systematic preparation and spectroscopic characterization of synthetic actinide complexes (Th, U, Np, and Pu) in which they can control nuclearity, oxidation state, and molecular structure. These complexes have been used to determine how observable electronic transitions are perturbed in response to structural changes in the complex in solution. From the spectra obtained for these model complexes, the authors have found that the f-f transitions naturally fall into obvious groupings by coordination number and symmetry by which they can now differentiate between monomeric, dimeric, and trimeric species in solution. The study of radionuclide speciation is fundamentally important to the determination of radionuclide solubility in the groundwater at Yucca Mountain.

  7. Development of Biodegradable Isosaccharinate-Containing Foams for Decontamination of Actinides

    SciTech Connect

    Rai, Dhanpat; Rao, Linfeng; Moore, R.C.; Hess, Nancy J.; Tucker, Mark D.

    2003-09-11

    The objective of this project is to develop fundamental information that will lead to the development of a new, more environmentally acceptable technology for decontaminating Pu and other actinides. The key component of this technology is isosaccharinate (ISA), a degradation product of cellulose materials that is biodegradable and binds strongly with tetravalent actinides. We are developing fundamental constants for (1) the effect of a wide range in pH and Ca concentrations on the speciation and thermodynamic reactions of ISA and (2) thermodynamic and kinetic reactions of ISA with tetravalent actinides and other competing ions such as Fe(III). We have successfully formulated and tested several ISA containing foams and gels for their effectiveness in removing tetravalent actinides from concrete and steel surfaces. These data along with a comprehensive thermodynamic mo del developed for Np(IV) and Ca(II) and applicable to a wide range in pH, ISA concentrations, and ionic strengths, will be presented.

  8. An Internet-based survey on characteristics of laser tattoo removal and associated side effects.

    PubMed

    Klein, Annette; Rittmann, Ines; Hiller, Karl-Anton; Landthaler, Michael; Bäumler, Wolfgang

    2014-03-01

    Tattoo removal by laser therapy is a frequently performed procedure in dermatological practices. Quality-switched ruby, alexandrite, or Nd:YAG lasers are the most suitable treatment devices. Although these techniques are regarded as safe, both temporary and permanent side effects might occur. Little has been published on the frequency of complications associated with laser tattoo removal. We performed an Internet survey in German-speaking countries on characteristics of laser tattoo removal and associated side effects. A total number of 157 questionnaires entered the final analysis. Motivations for laser tattoo removal were mainly considering the tattoo as youthful folly (29%), esthetic reasons (28%), and 6% indicated medical problems. One third of participants were unsatisfied with the result of laser tattoo removal, and a complete removal of the tattoo pigment was obtained in 38% only. Local transient side effects occurred in nearly all participants, but an important rate of slightly visible scars (24%) or even important scarring (8%) was reported. Every fourth participant described mild or intense tan when the laser treatment was performed, and the same number of people indicated UV exposure following laser therapy, which should normally be avoided in these circumstances. As reported in the literature, nearly half of the participants experienced hypopigmentation in the treated area. Our results show that from the patients' point of view there is an important rate of side effects occurring after laser tattoo removal. Appropriate pretreatment counseling with regard to realistic expectations, possible side effects, and the application of test spots is mandatory to ensure patient satisfaction. Laser treatment should be performed by appropriately trained personnel only.

  9. TAILORING INORGANIC SORBENTS FOR SRS STRONTIUM AND ACTINIDE SEPARATIONS: OPTIMIZED MONOSODIUM TITANATE PHASE II FINAL REPORT

    SciTech Connect

    Hobbs, D; Thomas Peters, T; Michael Poirier, M; Mark Barnes, M; Major Thompson, M; Samuel Fink, S

    2007-06-29

    This document provides a final report of Phase II testing activities for the development of a modified monosodium titanate (MST) that exhibits improved strontium and actinide removal characteristics compared to the baseline MST material. The activities included determining the key synthesis conditions for preparation of the modified MST, preparation of the modified MST at a larger scale by a commercial vendor, demonstration of the strontium and actinide removal characteristics with actual tank waste supernate and measurement of filtration characteristics. Key findings and conclusions include the following. Testing evaluated three synthetic methods and eleven process parameters for the optimum synthesis conditions for the preparation on an improved form of MST. We selected the post synthesis method (Method 3) for continued development based on overall sorbate removal performance. We successfully prepared three batches of the modified MST using Method 3 procedure at a 25-gram scale. The laboratory prepared modified MST exhibited increased sorption kinetics with simulated and actual waste solutions and similar filtration characteristics to the baseline MST. Characterization of the modified MST indicated that the post synthesis treatment did not significantly alter the particle size distribution, but did significantly increase the surface area and porosity compared to the original MST. Testing indicated that the modified MST exhibits reduced affinity for uranium compared to the baseline MST, reducing risk of fissile loading. Shelf-life testing indicated no change in strontium and actinide performance removal after storing the modified MST for 12-months at ambient laboratory temperature. The material releases oxygen during the synthesis and continues to offgas after the synthesis at a rapidly diminishing rate until below a measurable rate after 4 months. Optima Chemical Group LLC prepared a 15-kilogram batch of the modified MST using the post synthesis procedure (Method

  10. "Computational Modeling of Actinide Complexes"

    SciTech Connect

    Balasubramanian, K

    2007-03-07

    We will present our recent studies on computational actinide chemistry of complexes which are not only interesting from the standpoint of actinide coordination chemistry but also of relevance to environmental management of high-level nuclear wastes. We will be discussing our recent collaborative efforts with Professor Heino Nitsche of LBNL whose research group has been actively carrying out experimental studies on these species. Computations of actinide complexes are also quintessential to our understanding of the complexes found in geochemical, biochemical environments and actinide chemistry relevant to advanced nuclear systems. In particular we have been studying uranyl, plutonyl, and Cm(III) complexes are in aqueous solution. These studies are made with a variety of relativistic methods such as coupled cluster methods, DFT, and complete active space multi-configuration self-consistent-field (CASSCF) followed by large-scale CI computations and relativistic CI (RCI) computations up to 60 million configurations. Our computational studies on actinide complexes were motivated by ongoing EXAFS studies of speciated complexes in geo and biochemical environments carried out by Prof Heino Nitsche's group at Berkeley, Dr. David Clark at Los Alamos and Dr. Gibson's work on small actinide molecules at ORNL. The hydrolysis reactions of urnayl, neputyl and plutonyl complexes have received considerable attention due to their geochemical and biochemical importance but the results of free energies in solution and the mechanism of deprotonation have been topic of considerable uncertainty. We have computed deprotonating and migration of one water molecule from the first solvation shell to the second shell in UO{sub 2}(H{sub 2}O){sub 5}{sup 2+}, UO{sub 2}(H{sub 2}O){sub 5}{sup 2+}NpO{sub 2}(H{sub 2}O){sub 6}{sup +}, and PuO{sub 2}(H{sub 2}O){sub 5}{sup 2+} complexes. Our computed Gibbs free energy(7.27 kcal/m) in solution for the first time agrees with the experiment (7.1 kcal

  11. RAPID SEPARATION METHOD FOR ACTINIDES IN EMERGENCY SOIL SAMPLES

    SciTech Connect

    Maxwell, S.; Culligan, B.; Noyes, G.

    2009-11-09

    A new rapid method for the determination of actinides in soil and sediment samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used for samples up to 2 grams in emergency response situations. The actinides in soil method utilizes a rapid sodium hydroxide fusion method, a lanthanum fluoride soil matrix removal step, and a streamlined column separation process with stacked TEVA, TRU and DGA Resin cartridges. Lanthanum was separated rapidly and effectively from Am and Cm on DGA Resin. Vacuum box technology and rapid flow rates are used to reduce analytical time. Alpha sources are prepared using cerium fluoride microprecipitation for counting by alpha spectrometry. The method showed high chemical recoveries and effective removal of interferences. This new procedure was applied to emergency soil samples received in the NRIP Emergency Response exercise administered by the National Institute for Standards and Technology (NIST) in April, 2009. The actinides in soil results were reported within 4-5 hours with excellent quality.

  12. Actinide recovery techniques utilizing electromechanical processes

    SciTech Connect

    Westphal, B.R.; Benedict, R.W.

    1994-01-01

    Under certain conditions, the separation of actinides using electromechanical techniques may be an effective means of residue processing. The separation of granular mixtures of actinides and other materials discussed in this report is based on appreciable differences in the magnetic and electrical properties of the actinide elements. In addition, the high density of actinides, particularly uranium and plutonium, may render a simultaneous separation based on mutually complementary parameters. Both high intensity magnetic separation and electrostatic separation have been investigated for the concentration of an actinide waste stream. Waste stream constituents include an actinide metal alloy and broken quartz shards. The investigation of these techniques is in support of the Integral Fast Reactor (IFR) concept currently being developed at Argonne National Laboratory under the auspices of the Department of Energy.

  13. Selection of Actinide Chemical Analogues for WIPP Tests: Potential Nonradioactive Sorbing and Nonsorbing Tracers for Study of Ion Transport in the Environment

    SciTech Connect

    Dale Spall; Robert Villarreal

    1998-08-01

    Chemical characteristics of the actinides (Th, U, Np, Pu, Am) have been studied relative to nonradioactive chemical elements that have similar characteristics in an attempt to identify a group of actinide chemical analogues that are nonradioactive. In general, the chemistries of the actinides, especially U, Np, Pu, and Am, are very complex and attempts to identify a single chemical analogue for each oxidation state were not successful. However, the rationale for selecting a group of chemical analogues that would mimic the actinides as a group is provided. The categorization of possible chemical analogues (tracers) with similar chemical properties was based on the following criteria. Categorization was studied according.

  14. Superabsorbing gel for actinide, lanthanide, and fission product decontamination

    SciTech Connect

    Kaminski, Michael D.; Mertz, Carol J.

    2016-06-07

    The present invention provides an aqueous gel composition for removing actinide ions, lanthanide ions, fission product ions, or a combination thereof from a porous surface contaminated therewith. The composition comprises a polymer mixture comprising a gel forming cross-linked polymer and a linear polymer. The linear polymer is present at a concentration that is less than the concentration of the cross-linked polymer. The polymer mixture is at least about 95% hydrated with an aqueous solution comprising about 0.1 to about 3 percent by weight (wt %) of a multi-dentate organic acid chelating agent, and about 0.02 to about 0.6 molar (M) carbonate salt, to form a gel. When applied to a porous surface contaminated with actinide ions, lanthanide ions, and/or other fission product ions, the aqueous gel absorbs contaminating ions from the surface.

  15. Process for recovering actinide values

    DOEpatents

    Horwitz, E. Philip; Mason, George W.

    1980-01-01

    A process for rendering actinide values recoverable from sodium carbonate scrub waste solutions containing these and other values along with organic compounds resulting from the radiolytic and hydrolytic degradation of neutral organophosphorous extractants such as tri-n butyl phosphate (TBP) and dihexyl-N,N-diethyl carbamylmethylene phosphonate (DHDECAMP) which have been used in the reprocessing of irradiated nuclear reactor fuels. The scrub waste solution is preferably made acidic with mineral acid, to form a feed solution which is then contacted with a water-immiscible, highly polar organic extractant which selectively extracts the degradation products from the feed solution. The feed solution can then be processed to recover the actinides for storage or recycled back into the high-level waste process stream. The extractant is recycled after stripping the degradation products with a neutral sodium carbonate solution.

  16. Actinide abundances in ordinary chondrites

    NASA Technical Reports Server (NTRS)

    Hagee, B.; Bernatowicz, T. J.; Podosek, F. A.; Johnson, M. L.; Burnett, D. S.

    1990-01-01

    Measurements of actinide and light REE (LREE) abundances and of phosphate abundances in equilibrated ordinary chondrites were obtained and were used to define the Pu abundance in the solar system and to determine the degree of variation of actinide and LREE abundances. The results were also used to compare directly the Pu/U ratio with the earlier obtained ratio determined indirectly, as (Pu/Nd)x(Nd/U), assuming that Pu behaves chemically as a LREE. The data, combined with high-accuracy isotope-dilution data from the literature, show that the degree of gram-scale variability of the Th, U, and LREE abundances for equilibrated ordinary chondrites is a factor of 2-3 for absolute abundances and up to 50 percent for relative abundances. The observed variations are interpreted as reflecting the differences in the compositions and/or proportions of solar nebula components accreted to ordinary chondrite parent bodies.

  17. A study on removal characteristics of copper from aqueous solution by sewage sludge and pomace ashes.

    PubMed

    Bouzid, J; Elouear, Z; Ksibi, M; Feki, M; Montiel, A

    2008-04-01

    In the present work, the abilities of sewage sludge and pomace ashes to remove copper (Cu(2+)) ions from aqueous solutions are compared. Batch adsorption experiments were performed in order to evaluate the removal efficiency of these materials. Effect of contact time, solution pH, ash concentration and temperature on the removal of Cu(2+) was investigated. The results of batch equilibrium studies showed that the solution pH was the key factor affecting the adsorption characteristics. In general, the amount of Cu removed increased as the solid concentration and pH increased, and then it remained constant over a wide pH region. The adsorption test of applying sewage sludge and pomace ashes into synthetic wastewater revealed that the adsorption data of these materials for copper ions were better fitted to the Langmuir isotherm since the correlation coefficients for the Langmuir isotherm were higher than that for the Freundlich isotherm. The estimated maximum capacities of copper adsorbed by sewage sludge and pomace ashes were 5.71 and 6.98 mg g(-1), respectively. Experimental results indicated that the adsorption was favorable at higher pH and higher temperature. Values of DeltaG degrees ranging from -4.64 to -5.13 kcal mol(-1) for sewage sludge ash and from -4.97 to -5.53 kcal mol(-1) for pomace ash suggest that the adsorption reaction is a physical process enhanced by the electrostatic effect. The values of DeltaH degrees and DeltaS degrees are, respectively, 4.27 kcal mol(-1) and 30.6 cal K(-1)mol(-1) for sewage sludge ash and 4.33 kcal mol(-1) and 31.3 cal K(-1)mol(-1) for pomace ash. The mechanisms of copper removal by these materials included adsorption and precipitation. The sewage sludge and pomace ashes are shown to be effective adsorbents for this metal.

  18. CHARACTERIZATION OF ACTINIDES IN SIMULATED ALKALINE TANK WASTE SLUDGES AND LEACHATES

    SciTech Connect

    Nash, Kenneth L.

    2008-11-20

    In this project, both the fundamental chemistry of actinides in alkaline solutions (relevant to those present in Hanford-style waste storage tanks), and their dissolution from sludge simulants (and interactions with supernatants) have been investigated under representative sludge leaching procedures. The leaching protocols were designed to go beyond conventional alkaline sludge leaching limits, including the application of acidic leachants, oxidants and complexing agents. The simulant leaching studies confirm in most cases the basic premise that actinides will remain in the sludge during leaching with 2-3 M NaOH caustic leach solutions. However, they also confirm significant chances for increased mobility of actinides under oxidative leaching conditions. Thermodynamic data generated improves the general level of experiemental information available to predict actinide speciation in leach solutions. Additional information indicates that improved Al removal can be achieved with even dilute acid leaching and that acidic Al(NO3)3 solutions can be decontaminated of co-mobilized actinides using conventional separations methods. Both complexing agents and acidic leaching solutions have significant potential to improve the effectiveness of conventional alkaline leaching protocols. The prime objective of this program was to provide adequate insight into actinide behavior under these conditions to enable prudent decision making as tank waste treatment protocols develop.

  19. Mixed monofunctional extractants for trivalent actinide/lanthanide separations: TALSPEAK-MME

    DOE PAGES

    Johnson, Aaron T.; Nash, Kenneth L.

    2015-08-20

    The basic features of an f-element extraction process based on a solvent composed of equimolar mixtures of Cyanex-923 (a mixed trialkyl phosphine oxide) and 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) extractants in n-dodecane are investigated in this report. This system, which combines features of the TRPO and TALSPEAK processes, is based on co-extraction of trivalent lanthanides and actinides from 0.1 to 1.0 M HNO3 followed by application of a buffered aminopolycarboxylate solution strip to accomplish a Reverse TALSPEAK selective removal of actinides. This mixed-extractant medium could enable a simplified approach to selective trivalent f-element extraction and actinide partitioning in a singlemore » process. As compared with other combined process applications in development for more compact actinide partitioning processes (DIAMEX-SANEX, GANEX, TRUSPEAK, ALSEP), this combination features only monofunctional extractants with high solubility limits and comparatively low molar mass. Selective actinide stripping from the loaded extractant phase is done using a glycine-buffered solution containing N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA) or triethylenetetramine-N,N,N',N'',N''',N'''-hexaacetic acid (TTHA). Lastly, the results reported provide evidence for simplified interactions between the two extractants and demonstrate a pathway toward using mixed monofunctional extractants to separate trivalent actinides (An) from fission product lanthanides (Ln).« less

  20. Mixed monofunctional extractants for trivalent actinide/lanthanide separations: TALSPEAK-MME

    SciTech Connect

    Johnson, Aaron T.; Nash, Kenneth L.

    2015-08-20

    The basic features of an f-element extraction process based on a solvent composed of equimolar mixtures of Cyanex-923 (a mixed trialkyl phosphine oxide) and 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) extractants in n-dodecane are investigated in this report. This system, which combines features of the TRPO and TALSPEAK processes, is based on co-extraction of trivalent lanthanides and actinides from 0.1 to 1.0 M HNO3 followed by application of a buffered aminopolycarboxylate solution strip to accomplish a Reverse TALSPEAK selective removal of actinides. This mixed-extractant medium could enable a simplified approach to selective trivalent f-element extraction and actinide partitioning in a single process. As compared with other combined process applications in development for more compact actinide partitioning processes (DIAMEX-SANEX, GANEX, TRUSPEAK, ALSEP), this combination features only monofunctional extractants with high solubility limits and comparatively low molar mass. Selective actinide stripping from the loaded extractant phase is done using a glycine-buffered solution containing N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA) or triethylenetetramine-N,N,N',N'',N''',N'''-hexaacetic acid (TTHA). Lastly, the results reported provide evidence for simplified interactions between the two extractants and demonstrate a pathway toward using mixed monofunctional extractants to separate trivalent actinides (An) from fission product lanthanides (Ln).

  1. Pollutant removal characteristics of a two-influent-line BNR process performing denitrifying phosphorus removal: role of sludge recycling ratios.

    PubMed

    Liu, Hongbo; Leng, Feng; Chen, Piao; Kueppers, Stephan

    2016-11-01

    This paper studied denitrifying phosphorus removal of a novel two-line biological nutrient removal process treating low strength domestic wastewater under different sludge recycling ratios. Mass balance of intracellular compounds including polyhydroxyvalerate, polyhydroxybutyrate and glycogen was investigated together with total nitrogen (TN) and total phosphorus (TP). Results showed that sludge recycling ratios had a significant influence on the use of organics along bioreactors and 73.6% of the average removal efficiency was obtained when the influent chemical oxygen demand (COD) ranged from 175.9 mgL(-1) to 189.9 mgL(-1). The process performed better under a sludge recycling ratio of 100% compared to 25% and 50% in terms of ammonia and COD removal rates. Overall, TN removal efficiency for 50% and 100% sludge recycling ratios were 56.4% and 61.9%, respectively, unlike the big gap for carbon utilization and the TP removal rates, indicating that the effect of sludge recycling ratio on the anaerobic compartments had been counteracted by change in the efficiency of other compartments. The higher ratio of sludge recycling was conducive to the removal of TN, not in favor of TP, and less influence on COD. Thus, 25% was considered to be the optimal sludge recycling ratio.

  2. Patterns in the stability of the lower oxidation states of the actinides and lanthanides

    SciTech Connect

    Mikheev, N.B.; Auerman, L.N.; Ionova, G.V.; Korshunov, B.G.; Spitsyn, V.I.

    1986-09-01

    The authors compare the first half of the lanthanides and the second half of the actinides by considering the specifics of the electronic structure of the valence atoms of the f-, d-, and s-orbitals, consisting of he following: The lanthanides from praseodymium to europium and from dysprosium to ytterbium, as well as the actinides from californium to nobelium, have the same electronic configuration f /SUP n/ s/sub 2/ in the state of free neutral atoms, which corresponds to their divalent state. On the basis of a consideration of the energy characteristics of the valence orbitals of the elements of the lanthanide and actinide famililies and as a result of an experimental determination of the standard oxidation potential of these elements, the authors consider the profound similarity between the elements of the first half of the lanthanide family and the second half of the actinide family to be established.

  3. Kinetic characteristics and modelling of growth and substrate removal by Alcaligenes faecalis strain NR.

    PubMed

    Chen, Jie; Zhao, Bin; An, Qiang; Wang, Xia; Zhang, Yi Xin

    2016-04-01

    Alcaligenes faecalis strain NR has the capability of simultaneous ammonium and organic carbon removal under sole aerobic conditions. The growth and substrate removal characteristics of A. faecalis strain NR were studied and appropriate kinetic models were developed. The maximum substrate removal rate of NH4 (+)-N and TOC were determined as 2.27 mg NH4 (+)-N/L/h and 30.00 mg TOC/L/h, respectively with initial NH4 (+)-N = 80 mg/L and TOC = 800 mg/L. Single-substrate models and double-substrate models based on Monod, Contois, Moser and Teissier were employed to describe the bioprocess kinetic coefficients. As a result, two double-substrate models, Teissier-Contois and Contois-Contois, were considered to be appropriate to model growth kinetics with both NH4 (+)-N and TOC as limiting substrates. The kinetic constants of maximum growth rate (μ max) and half-saturation constant (K S and B S) were obtained by solving multiple equations with regression. This work can be used to further understand and predict the performance of heterotrophic nitrifiers, and thus provides specific guidance of these functional strains in practical wastewater treatment process.

  4. Uncertainties of stormwater characteristics and removal rates of stormwater treatment facilities: implications for stormwater handling.

    PubMed

    Langeveld, J G; Liefting, H J; Boogaard, F C

    2012-12-15

    Stormwater runoff is a major contributor to the pollution of receiving waters. This study focuses at characterising stormwater in order to be able to determine the impact of stormwater on receiving waters and to be able to select the most appropriate stormwater handling strategy. The stormwater characterisation is based on determining site mean concentrations (SMCs) and their uncertainties as well as the treatability of stormwater by monitoring specific pollutants concentration levels (TSS, COD, BOD, TKN, TP, Pb, Cu, Zn, E.coli) at three full scale stormwater treatment facilities in Arnhem, the Netherlands. This has resulted in 106 storm events being monitored at the lamella settler, 59 at the high rate sand filter and 132 at the soil filter during the 2 year monitoring period. The stormwater characteristics in Arnhem in terms of SMCs for main pollutants TSS and COD and settling velocities differ from international data. This implies that decisions for stormwater handling made on international literature data will very likely be wrong due to assuming too high concentrations of pollutants and misjudgement of the treatability of stormwater. The removal rates monitored at the full scale treatment facilities are within the expected range, with the soil filter and the sand filter having higher removal rates than the lamella settler. The full scale pilots revealed the importance of incorporating gross solids removal in the design of stormwater treatment facilities, as the gross solids determine operation and maintenance requirements.

  5. Effects of hemicellulose removal on cellulose fiber structure and recycling characteristics of eucalyptus pulp.

    PubMed

    Wan, JinQuan; Wang, Yan; Xiao, Qing

    2010-06-01

    Eucalyptus pulp fibers with large differences in cellulose and hemicellulose proportions but similar lignin contents were produced by partial removal of the hemicellulose and studied using Cross-Polarization Magic Angle Spinning Carbon-13 Nuclear Magnetic Resonance (CP/MAS (13)C NMR) in combination with spectral fitting, Atomic Force Microscopy (AFM), X-ray Diffraction (XRD) and Fourier Transform Infrared Spectroscopy (FTIR). There were remarkable differences in both cellulose fibril structure, pore structure and cellulose supermolecular structure between the samples. CP/MAS (13)C NMR combined with spectral fitting demonstrated an increase in average fibril aggregate size (17.9-22.2 nm) with decreasing hemicellulose content. AFM observations revealed that when the hemicellulose content decreased from 27.62% to 19.80%, the average diameters of pores decreased by 12.53%, but increased by 13.55% when the hemicellulose content decreased from 19.80% to 9.09%. XRD and FTIR analysis indicated that cellulose crystallinity increased with decreasing hemicellulose content. The low and high hemicellulose-containing pulps had very different recycling characteristics, which may be explained by the changes observed at cellulose fiber structure level. Fibrils appear to aggregate and form a more compact structure when the hemicellulose is removed, which was caused by a coalescence of the cellulose microfibrils. The removal of hemicellulose had disadvantageous influence on the accessibility of fibers and enhanced fiber flattening during drying, leading to increased sheet density and increased hornification.

  6. Atrazine adsorption removal with nylon6/polypyrrole core-shell nanofibers mat: possible mechanism and characteristics

    NASA Astrophysics Data System (ADS)

    Yang, Bi-Yi; Cao, Yang; Qi, Fei-Fei; Li, Xiao-Qing; Xu, Qian

    2015-05-01

    A functionalized nylon6/polypyrrole core-shell nanofibers mat (PA6/PPy NFM) was prepared via situ polymerization on nylon6 electrospun nanofibers mat (PA6 NFM) template and used as an adsorbent to remove atrazine from aqueous solutions. The core-shell structure of PA6/PPy NFM can be clearly proved under scanning electron microscope (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The effects of initial solution pH and ionic strength, as well as the comparison of the adsorption capacity of functionalized (PA6/PPy NFM) and non-functionalized (PA6 NFM) adsorbent, were examined to reveal the possible adsorption mechanism. The results indicated that π-π interaction and electrostatic interaction should play a key role in the adsorption process. The kinetics and thermodynamics studies also further elucidated the detailed adsorption characteristics of atrazine removal by PA6/PPy NFM. The adsorption of atrazine could be well described by the pseudo-second-order equation. The adsorption equilibrium data was well fitted with the Freundlich isotherm model with a maximum adsorption capacity value of 14.8 mg/g. In addition, the increase of adsorption rate caused by a temperature increase could be felicitously explained by the endothermic reaction. The desorption results showed that the adsorption capacity remained almost unchanged after six adsorption/desorption cycles. These results suggest that PA6/PPy NFM could be employed as an efficient adsorbent for removing atrazine from contaminated water sources.

  7. A high loading overland flow system: Impacts on soil characteristics, grass constituents, yields and nutrient removal.

    PubMed

    Wen, C G; Chen, T H; Hsu, F H; Lu, C H; Lin, J B; Chang, C H; Chang, S P; Lee, C S

    2007-04-01

    The objectives of this paper are to determine effects of different grass species and their harvests on pollutant removal, elucidate impacts on soil characteristics and grass constituents, observe grass yield and quantify nutrient uptake by vegetation in an overland flow system (OLFS). Polluted creek water was applied to eight channels in the OLFS, which were planted with Paragrass, Nilegrass, Cattail, and Vetiver, with each two channels being randomly planted with a given grass species. The grass in one channel was harvested while that in the other channel was not. At a high rate of 27.8 m d(-1) hydraulic loading, the removal efficiencies of conventional pollutants such as BOD, COD, suspended solids (SS), and total coliforms in wastewater are not affected by the type of the grasses species, but those of nitrogen and phosphorus are affected by different species. Overall average removal efficiencies of BOD, COD, SS, ammonia, total nitrogen, total phosphorus and total coliforms through the OLFS are 42%, 48%, 78%, 47%, 40%, 33% and 89%, respectively. The concentration of nitrate, however, increases due to nitrification. Soil characteristics in OLFS have been changed significantly; specific conductivity, organic matter, exchangeable magnesium, extractable copper and zinc in soils all increase with time while pHs decrease. During the winter season, there is a significant accumulation of nitrate in grass with the subsequent reduction during the active growing season (Spring). The contents of nitrate and phosphorus in grass tissue are higher than those of grass in general pastureland, probably due to nutrient luxury uptake by grass. The overall grass yield, growth rate and nutrient uptake are quantified and implication of such high rate OLFS discussed.

  8. REMOVAL OF RADIOACTIVE IONS FROM WATERS

    DOEpatents

    Silker, W.B.

    1962-04-10

    A process for removing neutron-reaction products, such as phosphorus, arsenic, manganese, copper, zinc, lanthanides, and actinides, from aqueous solutions by sorption on particles of aluminum metal is described. (AEC)

  9. Prompt fission neutron spectra of actinides

    DOE PAGES

    Capote, R.; Chen, Y. -J.; Hambsch, F. -J.; ...

    2016-01-06

    Here, the energy spectrum of prompt neutrons emitted in fission (PFNS) plays a very important role in nuclear science and technology. A Coordinated Research Project (CRP) "Evaluation of Prompt Fission Neutron Spectra of Actinides" was established by the IAEA Nuclear Data Section in 2009, with the major goal to produce new PFNS evaluations with uncertainties for actinide nuclei.

  10. Prompt fission neutron spectrum of actinides

    SciTech Connect

    Capote, R.; Chen, Y. -J.; Hambsch, F. J.; Jurado, B.; Lestone, J. P.; Litaize, O.; Morillon, B.; Neudecker, D.; Oberstedt, S.; Ohsawa, T.; Otuka, N.; Pronyaev, V. G.; Saxena, A.; Schmidt, K. H.; Shcherbakov, O. A.; Shu, N. -C.; Smith, D. L.; Talou, P.; Trkov, A.; Tudora, A. C.; Vogt, R.; Vorobyev, A. S.

    2016-01-06

    Here, the energy spectrum of prompt neutron emitted in fission (PFNS) plays a very important role in nuclear science and technology. A Coordinated Research Project (CRP) "Evaluation of Prompt Fission Neutron Spectra of Actinides" was established by the IAEA Nuclear Data Section in 2009, with the major goal to produce new PFNS evaluations with uncertainties for actinide nuclei.

  11. RAPID SEPARATION METHOD FOR ACTINIDES IN EMERGENCY AIR FILTER SAMPLES

    SciTech Connect

    Maxwell, S.; Noyes, G.; Culligan, B.

    2010-02-03

    A new rapid method for the determination of actinides and strontium in air filter samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used in emergency response situations. The actinides and strontium in air filter method utilizes a rapid acid digestion method and a streamlined column separation process with stacked TEVA, TRU and Sr Resin cartridges. Vacuum box technology and rapid flow rates are used to reduce analytical time. Alpha emitters are prepared using cerium fluoride microprecipitation for counting by alpha spectrometry. The purified {sup 90}Sr fractions are mounted directly on planchets and counted by gas flow proportional counting. The method showed high chemical recoveries and effective removal of interferences. This new procedure was applied to emergency air filter samples received in the NRIP Emergency Response exercise administered by the National Institute for Standards and Technology (NIST) in April, 2009. The actinide and {sup 90}Sr in air filter results were reported in {approx}4 hours with excellent quality.

  12. Minor Actinides Recycling in PWRs

    SciTech Connect

    Delpech, M.; Golfier, H.; Vasile, A.; Varaine, F.; Boucher, L.; Greneche, D.

    2006-07-01

    Recycling of minor actinides in current and near future PWR is considered as one of the options of the general waste management strategy. This paper presents the analysis of this option both from the core physics and fuel cycle point of view. A first indicator of the efficiency of different neutron spectra for transmutation purposes is the capture to fission cross sections ratio which is less favourable by a factor between 5 to 10 in PWRs compared to fast reactors. Another indicator presented is the production of high ranking isotopes like Curium, Berkelium or Californium in the thermal or epithermal spectrum conditions of PWR cores by successive neutron captures. The impact of the accumulation of this elements on the fabrication process of such PWR fuels strongly penalizes this option. The main constraint on minor actinides loadings in PWR (or fast reactors) fuels are related to their direct impact (or the impact of their transmutation products) on the reactivity coefficients, the reactivity control means and the core kinetics parameters. The main fuel cycle physical parameters like the neutron source, the alpha decay power, the gamma and neutrons dose rate and the criticality aspects are also affected. Recent neutronic calculations based on a reference core of the Evolutionary Pressurized Reactor (EPR), indicates typical maximum values of 1 % loadings. Different fuel design options for minor actinides transmutation purposes in PWRs are presented: UOX and MOX, homogeneous and heterogeneous assemblies. In this later case, Americium loading is concentrated in specific pins of a standard UOX assembly. Recycling of Neptunium in UOX and MOX fuels was also studied to improve the proliferation resistance of the fuel. The impact on the core physics and penalties on Uranium enrichment were underlined in this case. (authors)

  13. Actinide abundances in ordinary chondrites

    USGS Publications Warehouse

    Hagee, B.; Bernatowicz, T.J.; Podosek, F.A.; Johnson, M.L.; Burnett, D.S.; Tatsumoto, M.

    1990-01-01

    Measurements of 244Pu fission Xe, U, Th, and light REE (LREE) abundances, along with modal petrographic determinations of phosphate abundances, were carried out on equilibrated ordinary chondrites in order to define better the solar system Pu abundance and to determine the degree of variation of actinide and LREE abundances. Our data permit comparison of the directly measured Pu/ U ratio with that determined indirectly as (Pu/Nd) ?? (Nd/U) assuming that Pu behaves chemically as a LREE. Except for Guaren??a, and perhaps H chondrites in general, Pu concentrations are similar to that determined previously for St. Se??verin, although less precise because of higher trapped Xe contents. Trapped 130Xe 136Xe ratios appear to vary from meteorite to meteorite, but, relative to AVCC, all are similar in the sense of having less of the interstellar heavy Xe found in carbonaceous chondrite acid residues. The Pu/U and Pu/Nd ratios are consistent with previous data for St. Se??verin, but both tend to be slightly higher than those inferred from previous data on Angra dos Reis. Although significant variations exist, the distribution of our Th/U ratios, along with other precise isotope dilution data for ordinary chondrites, is rather symmetric about the CI chondrite value; however, actinide/(LREE) ratios are systematically lower than the CI value. Variations in actinide or LREE absolute and relative abundances are interpreted as reflecting differences in the proportions and/or compositions of more primitive components (chondrules and CAI materials?) incorporated into different regions of the ordinary chondrite parent bodies. The observed variations of Th/U, Nd/U, or Ce/U suggest that measurements of Pu/U on any single equilibrated ordinary chondrite specimen, such as St. Se??verin, should statistically be within ??20-30% of the average solar system value, although it is also clear that anomalous samples exist. ?? 1990.

  14. Interactions of microbial exopolymers with actinides

    NASA Astrophysics Data System (ADS)

    Johnson, Mitchell T.; Chitwood, Dawn J.; He, Lee; Neu, Mary P.

    2000-07-01

    The development of viable bioremediation strategies for radionuclide contaminated soils, sediments and ground waters at DOE sites is a formidable challenge. Ubiquitous microorganisms can absorb, oxidize, reduce and/or precipitate actinides and thereby affect the speciation, solubility, bioavailability, and migration of these toxic metals. Actinides can interact directly with microorganisms, i.e., via sorption to the cell wall, and indirectly via reaction with their byproducts, such as extracellular polymers. However, very little is known about the fundamental chemistry of any microbial-actinide interactions or their impact on environmental processes. Our goal is to fully characterize specific microbial-actinide interactions and determine how they may be exploited to effect environmental actinide mobility/immobility and remediation efforts.

  15. Actinide ion sensor for pyroprocess monitoring

    DOEpatents

    Jue, Jan-fong; Li, Shelly X.

    2014-06-03

    An apparatus for real-time, in-situ monitoring of actinide ion concentrations which comprises a working electrode, a reference electrode, a container, a working electrolyte, a separator, a reference electrolyte, and a voltmeter. The container holds the working electrolyte. The voltmeter is electrically connected to the working electrode and the reference electrode and measures the voltage between those electrodes. The working electrode contacts the working electrolyte. The working electrolyte comprises an actinide ion of interest. The reference electrode contacts the reference electrolyte. The reference electrolyte is separated from the working electrolyte by the separator. The separator contacts both the working electrolyte and the reference electrolyte. The separator is ionically conductive to the actinide ion of interest. The reference electrolyte comprises a known concentration of the actinide ion of interest. The separator comprises a beta double prime alumina exchanged with the actinide ion of interest.

  16. Exploring actinide materials through synchrotron radiation techniques.

    PubMed

    Shi, Wei-Qun; Yuan, Li-Yong; Wang, Cong-Zhi; Wang, Lin; Mei, Lei; Xiao, Cheng-Liang; Zhang, Li; Li, Zi-Jie; Zhao, Yu-Liang; Chai, Zhi-Fang

    2014-12-10

    Synchrotron radiation (SR) based techniques have been utilized with increasing frequency in the past decade to explore the brilliant and challenging sciences of actinide-based materials. This trend is partially driven by the basic needs for multi-scale actinide speciation and bonding information and also the realistic needs for nuclear energy research. In this review, recent research progresses on actinide related materials by means of various SR techniques were selectively highlighted and summarized, with the emphasis on X-ray absorption spectroscopy, X-ray diffraction and scattering spectroscopy, which are powerful tools to characterize actinide materials. In addition, advanced SR techniques for exploring future advanced nuclear fuel cycles dealing with actinides are illustrated as well.

  17. TAILORING INORGANIC SORBENTS FOR SRS STRONTIUM AND ACTINIDE SEPARATIONS: MODIFIED MONOSODIUM TITANATE PHASE III FINAL REPORT

    SciTech Connect

    Taylor-Pashow, K.; Hobbs, D.

    2010-09-01

    This document provides a final report of Phase III testing activities for the development of modified monosodium titanate (mMST), which exhibits improved strontium and actinide removal characteristics compared to the baseline MST material. The activities included characterization of the crystalline phases present at varying temperatures, solids settling characteristics, quantification of the peroxide content; evaluation of the post-synthesis gas release under different conditions; the extent of desorption of {sup 85}Sr, Np, and Pu under washing conditions; and the effects of age and radiation on the performance of the mMST. Key findings and conclusions include the following. The peroxide content of several mMST samples was determined using iodometric titration. The peroxide content was found to decrease with age or upon extended exposure to elevated temperature. A loss of peroxide was also measured after exposure of the material to an alkaline salt solution similar in composition to the simulated waste solution. To determine if the loss of peroxide with age affects the performance of the material, Sr and actinide removal tests were conducted with samples of varying age. The oldest sample (4 years and 8 months) did show lower Sr and Pu removal performance. When compared to the youngest sample tested (1 month), the oldest sample retained only 15% of the DF for Pu. Previous testing with this sample indicated no decrease in Pu removal performance up to an age of 30 months. No loss in Np removal performance was observed for any of the aged samples, and no uptake of uranium occurred at the typical sorbent loading of 0.2 g/L. Additional testing with a uranium only simulant and higher mMST loading (3.0 g/L) indicated a 10% increase of uranium uptake for a sample aged 3 years and 8 months when compared to the results of the same sample measured at an age of 1 year and 5 months. Performance testing with both baseline-MST and mMST that had been irradiated in a gamma source to

  18. Investigating Actinide Molecular Adducts From Absorption Edge Spectroscopy

    SciTech Connect

    Den Auwer, C.; Conradson, S.D.; Guilbaud, P.; Moisy, P.; Mustre de Leon, J.; Simoni, E.; /SLAC, SSRL

    2006-10-27

    Although Absorption Edge Spectroscopy has been widely applied to the speciation of actinide elements, specifically at the L{sub III} edge, understanding and interpretation of actinide edge spectra are not complete. In that sense, semi-quantitative analysis is scarce. In this paper, different aspects of edge simulation are presented, including semi-quantitative approaches. Comparison is made between various actinyl (U, Np) aquo or hydroxy compounds. An excursion into transition metal osmium chemistry allows us to compare the structurally related osmyl and uranyl hydroxides. The edge shape and characteristic features are discussed within the multiple scattering picture and the role of the first coordination sphere as well as contributions from the water solvent are described.

  19. Separation of actinides from lanthanides

    DOEpatents

    Smith, Barbara F.; Jarvinen, Gordon D.; Ryan, Robert R.

    1989-01-01

    An organic extracting solution and an extraction method useful for separating elements of the actinide series of the periodic table from elements of the lanthanide series, where both are in trivalent form. The extracting solution consists of a primary ligand and a secondary ligand, preferably in an organic solvent. The primary ligand is a substituted monothio-1,3-dicarbonyl, which includes a substituted 4-acyl-2-pyrazolin-5-thione, such as 4-benzoyl-2,4-dihydro-5-methyl-2-phenyl-3H-pyrazol-3-thione (BMPPT). The secondary ligand is a substituted phosphine oxide, such as trioctylphosphine oxide (TOPO).

  20. Rapid method to determine actinides and 89/90Sr in limestone and marble samples

    DOE PAGES

    Maxwell, Sherrod L.; Culligan, Brian; Hutchison, Jay B.; ...

    2016-04-12

    A new method for the determination of actinides and radiostrontium in limestone and marble samples has been developed that utilizes a rapid sodium hydroxide fusion to digest the sample. Following rapid pre-concentration steps to remove sample matrix interferences, the actinides and 89/90Sr are separated using extraction chromatographic resins and measured radiometrically. The advantages of sodium hydroxide fusion versus other fusion techniques will be discussed. Lastly, this approach has a sample preparation time for limestone and marble samples of <4 hours.

  1. Experimental studies of actinides in molten salts

    SciTech Connect

    Reavis, J.G.

    1985-06-01

    This review stresses techniques used in studies of molten salts containing multigram amounts of actinides exhibiting intense alpha activity but little or no penetrating gamma radiation. The preponderance of studies have used halides because oxygen-containing actinide compounds (other than oxides) are generally unstable at high temperatures. Topics discussed here include special enclosures, materials problems, preparation and purification of actinide elements and compounds, and measurements of various properties of the molten volts. Property measurements discussed are phase relationships, vapor pressure, density, viscosity, absorption spectra, electromotive force, and conductance. 188 refs., 17 figs., 6 tabs.

  2. Advanced Extraction Methods for Actinide/Lanthanide Separations

    SciTech Connect

    Scott, M.J.

    2005-12-01

    high level liquid wastes and a general actinide clean-up procedure. The selectivity of the standard extractant for tetravalent actinides, (N,N-diisobutylcarbamoylmethyl) octylphenylphosphineoxide (CMPO), was markedly improved by the attachment of three CMPO-like functions onto a triphenoxymethane platform, and a ligand that is both highly selective and effective for An(IV) ions was isolated. A 10 fold excess of ligand will remove virtually all of the 4+ actinides from the acidic layer without extracting appreciable quantities of An(III) and Ln(III) unlike simple CMPO ligands. Inspired by the success of the DIAMEX industrial process for extractions, three new tripodal chelates bearing three diglycolamide and thiodiglycolamide units precisely arranged on a triphenoxymethane platform have been synthesized for an highly efficient extraction of trivalent f-element cations from nitric acid media. A single equivalent of ligand will remove 80% of the Ln(III) ion from the acidic layer since the ligand is perfectly suited to accommodate the tricapped trigonal prismatic geometry preferred by the metal center. The ligand is perhaps the most efficient binder available for the heavier lanthanides and due to this unique attribute, the extraction event can be easily followed by 1H NMR spectroscopy confirming the formation of a TPP complex. The most lipophilic di-n-butyl tris-diglycolamide was found to be a significantly weaker extractant in comparison to the di-isopropyl analogs. The tris-thiodiglycolamide derivative proved to be an ineffective chelate for f-elements and demonstrated the importance of the etheric oxygens in the metal binding. The results presented herein clearly demonstrate a cooperative action of these three ligating groups within a single molecule, confirmed by composition and structure of the extracted complexes, and since actinides prefer to have high coordination numbers, the ligands should be particularly adept at binding with three arms. The use of such an

  3. Simultaneous removal and degradation characteristics of sulfonamide, tetracycline, and quinolone antibiotics by laccase-mediated oxidation coupled with soil adsorption.

    PubMed

    Ding, Huijun; Wu, Yixiao; Zou, Binchun; Lou, Qian; Zhang, Weihao; Zhong, Jiayou; Lu, Lei; Dai, Guofei

    2016-04-15

    The uses of laccase in the degradation and removal of antibiotics have recently been reported because of the high efficiency and environmental friendliness of laccase. However, these removal studies mostly refer to a limited number of antibiotics. In this study, soil adsorption was introduced into the laccase-oxidation system to assist the simultaneous removal of 14 kinds of sulfonamide, tetracycline, and quinolone antibiotics, which differed in structures and chemical properties. The complementary effects of laccase-mediated oxidation and soil adsorption enabled the simultaneous removal. Removal characteristics were determined by a comprehensive consideration of the separate optimum conditions for laccase oxidation and soil adsorption removal experiments. With concentrations of laccase, syringaldehyde (SA), and soil of 0.5mg/mL, 0.5mmol/L, and 50g/L, respectively, and at pH 6 and 25°C, the removal rates of each antibiotic exceeded 70% in 15min and were close to 100% in 180min. Sulfonamide antibiotics (SAs) were removed mainly by laccase oxidation and quinolone antibiotics (QUs) mainly by soil adsorption. Tetracycline antibiotics (TCs) were removed by both treatments in the coupled system, but laccase oxidation dominated. Electrostatic adsorption was speculated to be one of the adsorption mechanisms in soil adsorption with QUs and TCs.

  4. Strontium and Actinide Separations from High Level Nuclear Waste Solutions using Monosodium Titanate - Actual Waste Testing

    SciTech Connect

    Peters, T.B.; Barnes, M.J.; Hobbs,D.T.; Walker, D.D.; Fondeur, F.F.; Norato, M.A.; Pulmano, R.L.; Fink, S.D.

    2005-11-01

    Pretreatment processes at the Savannah River Site will separate {sup 90}Sr, alpha-emitting and radionuclides (i.e., actinides) and {sup 137}Cs prior to disposal of the high-level nuclear waste. Separation of {sup 90}Sr and alpha-emitting radionuclides occurs by ion exchange/adsorption using an inorganic material, monosodium titanate (MST). Previously reported testing with simulants indicates that the MST exhibits high selectivity for strontium and actinides in high ionic strength and strongly alkaline salt solutions. This paper provides a summary of data acquired to measure the performance of MST to remove strontium and actinides from actual waste solutions. These tests evaluated the effects of ionic strength, mixing, elevated alpha activities, and multiple contacts of the waste with MST. Tests also provided confirmation that MST performs well at much larger laboratory scales (300-700 times larger) and exhibits little affinity for desorption of strontium and plutonium during washing.

  5. Subsurface interactions of actinide species and microorganisms : implications for the bioremediation of actinide-organic mixtures.

    SciTech Connect

    Banaszak, J.E.; Reed, D.T.; Rittmann, B.E.

    1999-02-12

    By reviewing how microorganisms interact with actinides in subsurface environments, we assess how bioremediation controls the fate of actinides. Actinides often are co-contaminants with strong organic chelators, chlorinated solvents, and fuel hydrocarbons. Bioremediation can immobilize the actinides, biodegrade the co-contaminants, or both. Actinides at the IV oxidation state are the least soluble, and microorganisms accelerate precipitation by altering the actinide's oxidation state or its speciation. We describe how microorganisms directly oxidize or reduce actinides and how microbiological reactions that biodegrade strong organic chelators, alter the pH, and consume or produce precipitating anions strongly affect actinide speciation and, therefore, mobility. We explain why inhibition caused by chemical or radiolytic toxicities uniquely affects microbial reactions. Due to the complex interactions of the microbiological and chemical phenomena, mathematical modeling is an essential tool for research on and application of bioremediation involving co-contamination with actinides. We describe the development of mathematical models that link microbiological and geochemical reactions. Throughout, we identify the key research needs.

  6. Characteristics of the molar surface after removal of cervical enamel projections: comparison of three different rotating instruments

    PubMed Central

    2016-01-01

    Purpose The aim of this study was to evaluate and compare tooth surface characteristics in extracted human molars after cervical enamel projections (CEPs) were removed with the use of three rotating instruments. Methods We classified 60 extracted molars due to periodontal lesion with CEPs into grade I, II, or III, according to the Masters and Hoskins’ criteria. Each group contained 20 specimens. Three rotating instruments were used to remove the CEPs: a piezoelectric ultrasonic scaler, a periodontal bur, and a diamond bur. Tooth surface characteristics before and after removal of the projections were then evaluated with scanning electron microscopy (SEM). We analyzed the characteristics of the tooth surfaces with respect to roughness and whether the enamel projections had been completely removed. Results In SEM images, surfaces treated with the diamond bur were smoothest, but this instrument caused considerable harm to tooth structures near the CEPs. The piezoelectric ultrasonic scaler group produced the roughest surface but caused less harm to the tooth structure near the furcation. In general, the surfaces treated with the periodontal bur were smoother than those treated with the ultrasonic scaler, and the periodontal bur did not invade adjacent tooth structures. Conclusions For removal of grade II CEPs, the most effective instrument was the diamond bur. However, in removing grade III projections, the diamond bur can destroy both adjacent tooth structures and the periodontal apparatus. In such cases, careful use of the periodontal bur may be an appropriate substitute. PMID:27127691

  7. Advanced Aqueous Separation Systems for Actinide Partitioning

    SciTech Connect

    Nash, Kenneth L.; Clark, Sue; Meier, G Patrick; Alexandratos, Spiro; Paine, Robert; Hancock, Robert; Ensor, Dale

    2012-03-21

    One of the most challenging aspects of advanced processing of spent nuclear fuel is the need to isolate transuranium elements from fission product lanthanides. This project expanded the scope of earlier investigations of americium (Am) partitioning from the lanthanides with the synthesis of new separations materials and a centralized focus on radiochemical characterization of the separation systems that could be developed based on these new materials. The primary objective of this program was to explore alternative materials for actinide separations and to link the design of new reagents for actinide separations to characterizations based on actinide chemistry. In the predominant trivalent oxidation state, the chemistry of lanthanides overlaps substantially with that of the trivalent actinides and their mutual separation is quite challenging.

  8. BWR Assembly Optimization for Minor Actinide Recycling

    SciTech Connect

    G. Ivan Maldonado; John M. Christenson; J.P. Renier; T.F. Marcille; J. Casal

    2010-03-22

    The Primary objective of the proposed project is to apply and extend the latest advancements in LWR fuel management optimization to the design of advanced boiling water reactor (BWR) fuel assemblies specifically for the recycling of minor actinides (MAs).

  9. Overview of actinide chemistry in the WIPP

    SciTech Connect

    Borkowski, Marian; Lucchini, Jean - Francois; Richmann, Michael K; Reed, Donald T; Khaing, Hnin; Swanson, Juliet

    2009-01-01

    The year 2009 celebrates 10 years of safe operations at the Waste Isolation Pilot Plant (WIPP), the only nuclear waste repository designated to dispose defense-related transuranic (TRU) waste in the United States. Many elements contributed to the success of this one-of-the-kind facility. One of the most important of these is the chemistry of the actinides under WIPP repository conditions. A reliable understanding of the potential release of actinides from the site to the accessible environment is important to the WIPP performance assessment (PA). The environmental chemistry of the major actinides disposed at the WIPP continues to be investigated as part of the ongoing recertification efforts of the WIPP project. This presentation provides an overview of the actinide chemistry for the WIPP repository conditions. The WIPP is a salt-based repository; therefore, the inflow of brine into the repository is minimized, due to the natural tendency of excavated salt to re-seal. Reducing anoxic conditions are expected in WIPP because of microbial activity and metal corrosion processes that consume the oxygen initially present. Should brine be introduced through an intrusion scenario, these same processes will re-establish reducing conditions. In the case of an intrusion scenario involving brine, the solubilization of actinides in brine is considered as a potential source of release to the accessible environment. The following key factors establish the concentrations of dissolved actinides under subsurface conditions: (1) Redox chemistry - The solubility of reduced actinides (III and IV oxidation states) is known to be significantly lower than the oxidized forms (V and/or VI oxidation states). In this context, the reducing conditions in the WIPP and the strong coupling of the chemistry for reduced metals and microbiological processes with actinides are important. (2) Complexation - For the anoxic, reducing and mildly basic brine systems in the WIPP, the most important

  10. Joint Actinide Shock Physics Experimental Research - JASPER

    ScienceCinema

    None

    2016-07-12

    Commonly known as JASPER the Joint Actinide Shock Physics Experimental Research facility is a two stage light gas gun used to study the behavior of plutonium and other materials under high pressures, temperatures, and strain rates.

  11. Joint Actinide Shock Physics Experimental Research - JASPER

    SciTech Connect

    2014-10-31

    Commonly known as JASPER the Joint Actinide Shock Physics Experimental Research facility is a two stage light gas gun used to study the behavior of plutonium and other materials under high pressures, temperatures, and strain rates.

  12. Transmutation of actinides in power reactors.

    PubMed

    Bergelson, B R; Gerasimov, A S; Tikhomirov, G V

    2005-01-01

    Power reactors can be used for partial short-term transmutation of radwaste. This transmutation is beneficial in terms of subsequent storage conditions for spent fuel in long-term storage facilities. CANDU-type reactors can transmute the main minor actinides from two or three reactors of the VVER-1000 type. A VVER-1000-type reactor can operate in a self-service mode with transmutation of its own actinides.

  13. PREPARATION OF ACTINIDE-ALUMINUM ALLOYS

    DOEpatents

    Moore, R.H.

    1962-09-01

    BS>A process is given for preparing alloys of aluminum with plutonium, uranium, and/or thorium by chlorinating actinide oxide dissolved in molten alkali metal chloride with hydrochloric acid, chlorine, and/or phosgene, adding aluminum metal, and passing air and/or water vapor through the mass. Actinide metal is formed and alloyed with the aluminum. After cooling to solidification, the alloy is separated from the salt. (AEC)

  14. Predictive Modeling in Actinide Chemistry and Catalysis

    SciTech Connect

    Yang, Ping

    2016-05-16

    These are slides from a presentation on predictive modeling in actinide chemistry and catalysis. The following topics are covered in these slides: Structures, bonding, and reactivity (bonding can be quantified by optical probes and theory, and electronic structures and reaction mechanisms of actinide complexes); Magnetic resonance properties (transition metal catalysts with multi-nuclear centers, and NMR/EPR parameters); Moving to more complex systems (surface chemistry of nanomaterials, and interactions of ligands with nanoparticles); Path forward and conclusions.

  15. Recent progress in actinide borate chemistry.

    PubMed

    Wang, Shuao; Alekseev, Evgeny V; Depmeier, Wulf; Albrecht-Schmitt, Thomas E

    2011-10-21

    The use of molten boric acid as a reactive flux for synthesizing actinide borates has been developed in the past two years providing access to a remarkable array of exotic materials with both unusual structures and unprecedented properties. [ThB(5)O(6)(OH)(6)][BO(OH)(2)]·2.5H(2)O possesses a cationic supertetrahedral structure and displays remarkable anion exchange properties with high selectivity for TcO(4)(-). Uranyl borates form noncentrosymmetric structures with extraordinarily rich topological relationships. Neptunium borates are often mixed-valent and yield rare examples of compounds with one metal in three different oxidation states. Plutonium borates display new coordination chemistry for trivalent actinides. Finally, americium borates show a dramatic departure from plutonium borates, and there are scant examples of families of actinides compounds that extend past plutonium to examine the bonding of later actinides. There are several grand challenges that this work addresses. The foremost of these challenges is the development of structure-property relationships in transuranium materials. A deep understanding of the materials chemistry of actinides will likely lead to the development of advanced waste forms for radionuclides present in nuclear waste that prevent their transport in the environment. This work may have also uncovered the solubility-limiting phases of actinides in some repositories, and allows for measurements on the stability of these materials.

  16. Rapid determination of actinides in seawater samples

    DOE PAGES

    Maxwell, Sherrod L.; Culligan, Brian K.; Hutchison, Jay B.; ...

    2014-03-09

    A new rapid method for the determination of actinides in seawater samples has been developed at the Savannah River National Laboratory. The actinides can be measured by alpha spectrometry or inductively-coupled plasma mass spectrometry. The new method employs novel pre-concentration steps to collect the actinide isotopes quickly from 80 L or more of seawater. Actinides are co-precipitated using an iron hydroxide co-precipitation step enhanced with Ti+3 reductant, followed by lanthanum fluoride co-precipitation. Stacked TEVA Resin and TRU Resin cartridges are used to rapidly separate Pu, U, and Np isotopes from seawater samples. TEVA Resin and DGA Resin were used tomore » separate and measure Pu, Am and Cm isotopes in seawater volumes up to 80 L. This robust method is ideal for emergency seawater samples following a radiological incident. It can also be used, however, for the routine analysis of seawater samples for oceanographic studies to enhance efficiency and productivity. In contrast, many current methods to determine actinides in seawater can take 1–2 weeks and provide chemical yields of ~30–60 %. This new sample preparation method can be performed in 4–8 h with tracer yields of ~85–95 %. By employing a rapid, robust sample preparation method with high chemical yields, less seawater is needed to achieve lower or comparable detection limits for actinide isotopes with less time and effort.« less

  17. Actinide speciation in relation to biological processes.

    PubMed

    Ansoborlo, Eric; Prat, Odette; Moisy, Philippe; Den Auwer, Christophe; Guilbaud, Philippe; Carriere, M; Gouget, Barbara; Duffield, John; Doizi, Denis; Vercouter, Thomas; Moulin, Christophe; Moulin, Valérie

    2006-11-01

    In case of accidental release of radionuclides into the environment, actinides represent a severe health risk to human beings following internal contamination (inhalation, ingestion or wound). For a better understanding of the actinide behaviour in man (in term of metabolism, retention, excretion) and in specific biological systems (organs, cells or biochemical pathways), it is of prime importance to have a good knowledge of the relevant actinide solution chemistry and biochemistry, in particular of the thermodynamic constants needed for computing actinide speciation. To a large extent, speciation governs bioavailability and toxicity of elements and has a significant impact on the mechanisms by which toxics accumulate in cell compartments and organs and by which elements are transferred and transported from cell to cell. From another viewpoint, speciation is the prerequisite for the design and success of potential decorporation therapies. The purpose of this review is to present the state of the art of actinide knowledge within biological media. It is also to discuss how actinide speciation can be determined or predicted and to highlight the areas where information is lacking with the aim to encourage new research efforts.

  18. Recent progress in actinide borate chemistry

    SciTech Connect

    Wang, Shuao; Alekseev, Evgeny V.; Depmeier, Wulf; Albrecht-Schmitt, Thomas E.

    2011-01-01

    The use of molten boric acid as a reactive flux for synthesizing actinide borates has been developed in the past two years providing access to a remarkable array of exotic materials with both unusual structures and unprecedented properties. [ThB₅O₆(OH)₆][BO(OH)₂]·2.5H₂O possesses a cationic supertetrahedral structure and displays remarkable anion exchange properties with high selectivity for TcO4- Uranyl borates form noncentrosymmetric structures with extraordinarily rich topological relationships. Neptunium borates are often mixed-valent and yield rare examples of compounds with one metal in three different oxidation states. Plutonium borates display new coordination chemistry for trivalent actinides. Finally, americium borates show a dramatic departure from plutonium borates, and there are scant examples of families of actinides compounds that extend past plutonium to examine the bonding of later actinides. There are several grand challenges that this work addresses. The foremost of these challenges is the development of structure-property relationships in transuranium materials. A deep understanding of the materials chemistry of actinides will likely lead to the development of advanced waste forms for radionuclides present in nuclear waste that prevent their transport in the environment. This work may have also uncovered the solubility-limiting phases of actinides in some repositories, and allows for measurements on the stability of these materials.

  19. Minor actinide transmutation in thorium and uranium matrices in heavy water moderated reactors

    SciTech Connect

    Bhatti, Zaki; Hyland, B.; Edwards, G.W.R.

    2013-07-01

    The irradiation of Th{sup 232} breeds fewer of the problematic minor actinides (Np, Am, Cm) than the irradiation of U{sup 238}. This characteristic makes thorium an attractive potential matrix for the transmutation of these minor actinides, as these species can be transmuted without the creation of new actinides as is the case with a uranium fuel matrix. Minor actinides are the main contributors to long term decay heat and radiotoxicity of spent fuel, so reducing their concentration can greatly increase the capacity of a long term deep geological repository. Mixing minor actinides with thorium, three times more common in the Earth's crust than natural uranium, has the additional advantage of improving the sustainability of the fuel cycle. In this work, lattice cell calculations have been performed to determine the results of transmuting minor actinides from light water reactor spent fuel in a thorium matrix. 15-year-cooled group-extracted transuranic elements (Np, Pu, Am, Cm) from light water reactor (LWR) spent fuel were used as the fissile component in a thorium-based fuel in a heavy water moderated reactor (HWR). The minor actinide (MA) transmutation rates, spent fuel activity, decay heat and radiotoxicity, are compared with those obtained when the MA were mixed instead with natural uranium and taken to the same burnup. Each bundle contained a central pin containing a burnable neutron absorber whose initial concentration was adjusted to have the same reactivity response (in units of the delayed neutron fraction β) for coolant voiding as standard NU fuel. (authors)

  20. Development of Biodegradable Isosaccharinate-Containing Foams for Decontamination of Actinides: Thermodynamic and Kinetic Reactions between Isosaccharinate and Actinides on Metal and Concrete Surfaces

    SciTech Connect

    Rai, Dhanpat; Rao, Linfeng; Moore, Robert C.; Bontchev, Ranko; Holt, Kathleen

    2004-06-01

    Actinide contamination of steel and concrete surfaces is a major problem within the DOE complex. Almost all current decontamination technologies rely on removal of the contaminated surface layer by mechanical means or by chemical methods using harsh chemicals. Some of the technologies are ineffective. Others are expensive, labor intensive, and hazardous to workers. Still others create secondary mixed wastes that are not environmentally acceptable. This project seeks fundamental information that will lead to the development of a new and more environmentally acceptable technology for decontamination of actinides, especially Pu, on steel and concrete surfaces. The key component of this technology is isosaccharinate (ISA), a degradation product of cellulose materials that is biodegradable. Isosaccharinate will be incorporated into foams/gels for safe and easy use in decontamination of actinides from steel, concrete, and other surfaces. Thermodynamic data are being developed on ISA species as a function of pH and on ISA interactions with actinides and competing metals [e.g., Fe(III) and Ca(II)] under a wide range of conditions relevant to decontamination of steel and concrete. The efficiency of the ISA containing foams/gels/solutions for decontamination is also being tested. This project builds on capabilities at three different national laboratories, and represents a joint effort between PNNL, LBNL, and SNL.

  1. DEVELOPMENT OF BIODEGRADABLE ISOSACCHARINATE-CONTAINING FOAMS FOR DECONTAMINATION OF ACTINIDES: THERMODYNAMIC AND KINETIC REACTIONS BETWEEN ISOSACCHARINATE AND ACTINIDES ON METAL AND CONCRETE SURFACES

    SciTech Connect

    Rai, Dhanpat; Moore, Robert C.; Linfeng, Rao; Tucker, Mark D.

    2003-06-01

    Actinide contamination of steel and concrete surfaces is a major problem within the DOE complex. Almost all current decontamination technologies rely on removal of the contaminated surface layer by mechanical means or by chemical methods, using harsh chemicals. Some of the technologies are ineffective. Others are expensive, labor intensive, and hazardous to workers. Still others create secondary mixed wastes that are not environmentally acceptable. This project seeks fundamental information that will lead to the development of a new and more environmentally acceptable technology for decontamination of actinides, especially Pu, on steel and concrete surfaces. The key component of this technology is isosaccharinate (ISA), a degradation product of cellulose materials that is biodegradable. Isosaccharinate will be incorporated into foams/gels for safe and easy use in decontamination of actinides from steel, concrete, and other surfaces. Thermodynamic data are being developed on the interactions of ISA with actinides and competing metals [e.g., Fe(III) and Ca(II)] under a wide range of conditions relevant to decontamination of steel and concrete. The efficiency of the ISA containing foams/gels/solutions for decontamination is also being tested. This project builds on capabilities at three different national laboratories, and represents a joint effort between PNNL, LBNL, and SNL.

  2. Nitrogen Removal Characteristics of a Newly Isolated Indigenous Aerobic Denitrifier from Oligotrophic Drinking Water Reservoir, Zoogloea sp. N299.

    PubMed

    Huang, Ting-Lin; Zhou, Shi-Lei; Zhang, Hai-Han; Bai, Shi-Yuan; He, Xiu-Xiu; Yang, Xiao

    2015-05-04

    Nitrogen is considered to be one of the most widespread pollutants leading to eutrophication of freshwater ecosystems, especially in drinking water reservoirs. In this study, an oligotrophic aerobic denitrifier was isolated from drinking water reservoir sediment. Nitrogen removal performance was explored. The strain was identified by 16S rRNA gene sequence analysis as Zoogloea sp. N299. This species exhibits a periplasmic nitrate reductase gene (napA). Its specific growth rate was 0.22 h-1. Obvious denitrification and perfect nitrogen removal performances occurred when cultured in nitrate and nitrite mediums, at rates of 75.53%±1.69% and 58.65%±0.61%, respectively. The ammonia removal rate reached 44.12%±1.61% in ammonia medium. Zoogloea sp. N299 was inoculated into sterilized and unsterilized reservoir source waters with a dissolved oxygen level of 5-9 mg/L, pH 8-9, and C/N 1.14:1. The total nitrogen removal rate reached 46.41%±3.17% (sterilized) and 44.88%±4.31% (unsterilized). The cell optical density suggested the strain could survive in oligotrophic drinking water reservoir water conditions and perform nitrogen removal. Sodium acetate was the most favorable carbon source for nitrogen removal by strain N299 (p<0.05). High C/N was beneficial for nitrate reduction (p<0.05). The nitrate removal efficiencies showed no significant differences among the tested inoculums dosage (p>0.05). Furthermore, strain N299 could efficiently remove nitrate at neutral and slightly alkaline and low temperature conditions. These results, therefore, demonstrate that Zoogloea sp. N299 has high removal characteristics, and can be used as a nitrogen removal microbial inoculum with simultaneous aerobic nitrification and denitrification in a micro-polluted reservoir water ecosystem.

  3. Effect of surface characteristics on retention and removal of Escherichia coli O157:H7 on surfaces of spinach

    Technology Transfer Automated Retrieval System (TEKTRAN)

    The topography and the spatial heterogeneity of produce surfaces may impact the attachment of microbial cells onto produce surfaces and affect disinfection efficacy. In this study, the effects of produce surface characteristics on the removal of bacteria were studied. Fresh spinach leaves were sp...

  4. Rapid radiochemical method for determination of actinides in emergency concrete and brick samples.

    PubMed

    Maxwell, Sherrod L; Culligan, Brian K; Kelsey-Wall, Angel; Shaw, Patrick J

    2011-09-02

    A new rapid method for the determination of actinides in emergency concrete and brick samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used in emergency response situations or for routine analysis. If a radiological dispersive device (RDD), Improvised Nuclear Device (IND) or nuclear accident occurs, there will be a urgent need for rapid analyses of many different environmental matrices, including building materials such as concrete and brick, to support dose mitigation and environmental clean-up. The new method for actinides in concrete and brick method utilizes a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step, and a column separation process with stacked TEVA, TRU and DGA Resin cartridges. Alpha emitters are prepared using rare earth microprecipitation for counting by alpha spectrometry. The method showed high chemical recoveries and effective removal of interferences. The determination of actinides in concrete and brick sample analysis can be performed in less than 8h with excellent quality for emergency samples. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory actinide particles are effectively digested.

  5. MINOR ACTINIDE SEPARATIONS USING ION EXCHANGERS OR IONIC LIQUIDS

    SciTech Connect

    Hobbs, D.; Visser, A.; Bridges, N.

    2011-09-20

    This project seeks to determine if (1) inorganic-based ion exchange materials or (2) electrochemical methods in ionic liquids can be exploited to provide effective Am and Cm separations. Specifically, we seek to understand the fundamental structural and chemical factors responsible for the selectivity of inorganic-based ion-exchange materials for actinide and lanthanide ions. Furthermore, we seek to determine whether ionic liquids can serve as the electrolyte that would enable formation of higher oxidation states of Am and other actinides. Experiments indicated that pH, presence of complexants and Am oxidation state exhibit significant influence on the uptake of actinides and lanthanides by layered sodium titanate and hybrid zirconium and tin phosphonate ion exchangers. The affinity of the ion exchangers increased with increasing pH. Greater selectivity among Ln(III) ions with sodium titanate materials occurs at a pH close to the isoelectric potential of the ion exchanger. The addition of DTPA decreased uptake of Am and Ln, whereas the addition of TPEN generally increases uptake of Am and Ln ions by sodium titanate. Testing confirmed two different methods for producing Am(IV) by oxidation of Am(III) in ionic liquids (ILs). Experimental results suggest that the unique coordination environment of ionic liquids inhibits the direct electrochemical oxidation of Am(III). The non-coordinating environment increases the oxidation potential to a higher value, while making it difficult to remove the inner coordination of water. Both confirmed cases of Am(IV) were from the in-situ formation of strong chemical oxidizers.

  6. Experimental and calculational analyses of actinide samples irradiated in EBR-II

    SciTech Connect

    Gilai, D.; Williams, M.L.; Cooper, J.H.; Laing, W.R.; Walker, R.L.; Raman, S.; Stelson, P.H.

    1982-10-01

    Higher actinides influence the characteristics of spent and recycled fuel and dominate the long-term hazards of the reactor waste. Reactor irradiation experiments provide useful benchmarks for testing the evaluated nuclear data for these actinides. During 1967 to 1970, several actinide samples were irradiated in the Idaho EBR-II fast reactor. These samples have now been analyzed, employing mass and alpha spectrometry, to determine the heavy element products. A simple spherical model for the EBR-II core and a recent version of the ORIGEN code with ENDF/B-V data were employed to calculate the exposure products. A detailed comparison between the experimental and calculated results has been made. For samples irradiated at locations near the core center, agreement within 10% was obtained for the major isotopes and their first daughters, and within 20% for the nuclides up the chain. A sensitivity analysis showed that the assumed flux should be increased by 10%.

  7. Montmorillonite surface properties and sorption characteristics for heavy metal removal from aqueous solutions.

    PubMed

    Ijagbemi, Christianah Olakitan; Baek, Mi-Hwa; Kim, Dong-Su

    2009-07-15

    Surface properties of montmorillonite (MMT) and its adsorption characteristics for heavy metals have been investigated with nickel and copper as sorbate from aqueous solutions. Employing the potentiometric and mass titration techniques in batch experimental methods, the point of zero charge (PZC) and point of zero net proton charge (PZNPC) of MMT edges at different ionic strengths present pH(PZC) and pH(PZNPC) to be 3.4+/-0.2. A crossing point was observed for the proton adsorption vs. pH curves at different ionic strengths of KCl electrolyte and in investigating MMT remediation potentialities as sorbent for heavy metals polluted waters, the effects of heavy metal concentration, pH, MMT dosage, reaction time and temperature for Cu(2+) and Ni(2+) uptake were studied. The sorption of metal ions by MMT was pH dependent and the adsorption kinetics revealed sorption rate could be well fitted by the pseudo-second-order rate model. The data according to mass transfer and intraparticle diffusion models confirmed diffusion of solutes inside the clay particles as the rate-controlling step and more important for the adsorption rate than the external mass transfer. Adsorption isotherms showed that the uptake of Cu(2+) and Ni(2+) could be described by the Langmuir model and from calculations on thermodynamic parameters, the positive Delta G degrees values at different temperatures suggest that the sorption of both metal ions were non-spontaneous. Change in enthalpy (Delta H degrees) for Ni(2+) and Cu(2+) were 28.9 and 13.27 kJ/mol K respectively, hence an endothermic diffusion process, as ion uptake increased with increase in temperature. Values of DeltaS degrees indicate low randomness at the solid/solution interface during the uptake of both Cu(2+) and Ni(2+) by MMT. Montmorillonite has a considerable potential for the removal of heavy metal cationic species from aqueous solution and wastewater.

  8. [Study on characteristics of simultaneous removal of ammonium and phosphate from waste water by zeolitized fly ash].

    PubMed

    Zhao, Tong-gang; Wu, De-yi; Chen, Jian-gang; Kong, Hai-nan; Zhang, Bao-hua; Wang, Zao-sheng

    2006-04-01

    Characteristics of simultaneous removal of ammonium and phosphate from wastewater by zeolite synthesized from fly ash was investigated. The amount of ammonium and phosphate removed by zeolitized fly ash changed with time, and approached to a constant value after adsorption time of 24h was reached. The amount of ammonium and phosphate removed also increased with the rise in the amount of zeolite added, but slackened above the solid/liquid ratio of 8 g x L(-1). The removal rate of ammonium by zeolitized fly ash could rise to the maximum value of 60% when pH was between 7 and 9, and declined out of the pH range. For phosphate, minimum removal rate of about 85% was obtained within pH 7-9, and the removal rate increased to about 100% out of the pH range. The adsorption of ammonium on zeolitized fly ash was an exothermic reaction; the removal rate of ammonium could decrease with the rise in temperature. On the contrary, the adsorption of phosphate was an endothermic reaction, and the rise in temperature favored the removal of phosphate by zeolitized fly ash. The adsorptive ability of ammonium on zeolitized fly ash was: Al-Z > Mg-Z > Ca-Z > Na-Z > Fe-Z. The order for phosphate was: Al-Z > Fe-Z > Ca-Z > Mg-Z > Na-Z. It was proposed that the mechanism for the removal of ammonium from wastewater by zeolitized fly ash was cation exchange process, while the mechanism for phosphate was not only the precipitation reaction of phosphate with cation in solution, but also adsorption mechanism.

  9. Actinide consumption: Nuclear resource conservation without breeding

    SciTech Connect

    Hannum, W.H.; Battles, J.E.; Johnson, T.R.; McPheeters, C.C.

    1991-01-01

    A new approach to the nuclear power issue based on a metallic fast reactor fuel and pyrometallurgical processing of spent fuel is showing great potential and is approaching a critical demonstration phase. If successful, this approach will complement and validate the LWR reactor systems and the attendant infrastructure (including repository development) and will alleviate the dominant concerns over the acceptability of nuclear power. The Integral Fast Reactor (IFR) concept is a metal-fueled, sodium-cooled pool-type fast reactor supported by a pyrometallurgical reprocessing system. The concept of a sodium cooled fast reactor is broadly demonstrated by the EBR-II and FFTF in the US; DFR and PFR in the UK; Phenix and SuperPhenix in France; BOR-60, BN-350, BN-600 in the USSR; and JOYO in Japan. The metallic fuel is an evolution from early EBR-II fuels. This fuel, a ternary U-Pu-Zr alloy, has been demonstrated to be highly reliable and fault tolerant even at very high burnup (160-180,000 MWd/MT). The fuel, coupled with the pool type reactor configuration, has been shown to have outstanding safety characteristics: even with all active safety systems disabled, such a reactor can survive a loss of coolant flow, a loss of heat sink, or other major accidents. Design studies based on a small modular approach show not only its impressive safety characteristics, but are projected to be economically competitive. The program to explore the feasibility of actinide recovery from spent LWR fuel is in its initial phase, but it is expected that technical feasibility could be demonstrated by about 1995; DOE has not yet committed funds to achieve this objective. 27 refs.

  10. Nonaqueous method for dissolving lanthanide and actinide metals

    DOEpatents

    Crisler, L.R.

    1975-11-11

    Lanthanide and actinide beta-diketonate complex molecular compounds are produced by reacting a beta-diketone compound with a lanthanide or actinide element in the elemental metallic state in a mixture of carbon tetrachloride and methanol.

  11. Impact of virus surface characteristics on removal mechanisms within membrane bioreactors.

    PubMed

    Chaudhry, Rabia M; Holloway, Ryan W; Cath, Tzahi Y; Nelson, Kara L

    2015-11-01

    In this study we investigated the removal of viruses with similar size and shape but with different external surface capsid proteins by a bench-scale membrane bioreactor (MBR). The goal was to determine which virus removal mechanisms (retention by clean backwashed membrane, retention by cake layer, attachment to biomass, and inactivation) were most impacted by differences in the virus surface properties. Seven bench-scale MBR experiments were performed using mixed liquor wastewater sludge that was seeded with three lab-cultured bacteriophages with icosahedral capsids of ∼30 nm diameter (MS2, phiX174, and fr). The operating conditions were designed to simulate those at a reference, full-scale MBR facility. The virus removal mechanism most affected by virus type was attachment to biomass (removals of 0.2 log for MS2, 1.2 log for phiX174, and 3 log for fr). These differences in removal could not be explained by electrostatic interactions, as the three viruses had similar net negative charge when suspended in MBR permeate. Removals by the clean backwashed membrane (less than 1 log) and cake layer (∼0.6 log) were similar for the three viruses. A comparison between the clean membrane removals seen at the bench-scale using a virgin membrane (∼1 log), and the full-scale using 10-year old membranes (∼2-3 logs) suggests that irreversible fouling, accumulated on the membrane over years of operation that cannot be removed by cleaning, also contributes towards virus removal. This study enhances the current mechanistic understanding of virus removal in MBRs and will contribute to more reliable treatment for water reuse applications.

  12. TUCS/phosphate mineralization of actinides

    SciTech Connect

    Nash, K.L.

    1997-10-01

    This program has as its objective the development of a new technology that combines cation exchange and mineralization to reduce the concentration of heavy metals (in particular actinides) in groundwaters. The treatment regimen must be compatible with the groundwater and soil, potentially using groundwater/soil components to aid in the immobilization process. The delivery system (probably a water-soluble chelating agent) should first concentrate the radionuclides then release the precipitating anion, which forms thermodynamically stable mineral phases, either with the target metal ions alone or in combination with matrix cations. This approach should generate thermodynamically stable mineral phases resistant to weathering. The chelating agent should decompose spontaneously with time, release the mineralizing agent, and leave a residue that does not interfere with mineral formation. For the actinides, the ideal compound probably will release phosphate, as actinide phosphate mineral phases are among the least soluble species for these metals. The most promising means of delivering the precipitant would be to use a water-soluble, hydrolytically unstable complexant that functions in the initial stages as a cation exchanger to concentrate the metal ions. As it decomposes, the chelating agent releases phosphate to foster formation of crystalline mineral phases. Because it involves only the application of inexpensive reagents, the method of phosphate mineralization promises to be an economical alternative for in situ immobilization of radionuclides (actinides in particular). The method relies on the inherent (thermodynamic) stability of actinide mineral phases.

  13. Characteristics of nitrogen and phosphorus removal by a surface-flow constructed wetland for polluted river water treatment.

    PubMed

    Dzakpasu, Mawuli; Wang, Xiaochang; Zheng, Yucong; Ge, Yuan; Xiong, Jiaqing; Zhao, Yaqian

    2015-01-01

    The characteristics of nitrogen (N) and phosphorus (P) removal were studied during the 2-year operation of a free water surface flow wetland of 900 m² with hydraulic loading of 0.1 m/d to evaluate its potential to treat water from an urban stream polluted with municipal and industrial wastewater. Attention was focused on the removal of dissolved N and P by harvesting plants (local Phragmites australis and Typha orientalis) at the end of each growing season. According to findings, the removals of N and P increased from 47.1% and 17.6%, respectively, in the 1st year to 52.3% and 32.4%, respectively, in the 2nd year. Increments of N and P removal were largely attributable to plant biomass, which increased from an average dry weight of 1.77 kg/m² in the 1st year to 3.41 kg/m² in the 2nd year. The amount of nutrients assimilated by plants in the 2nd year was almost double that of the 1st year. Increasing biomass in the 2nd year also improved redox conditions in the substrate layer, which contributed to increasing the efficiency of N removal. Compared with T. orientalis, P. australis was more competitive and adapted to conditions in the wetland better; it regenerated more vigorously and contributed more to nutrient removal.

  14. Combined Extraction of Cesium, Strontium, and Actinides from Alkaline Media: An Extension of the Caustic-Side Solvent Extraction (CSSX) Process Technology

    SciTech Connect

    Kenneth Raymond

    2004-11-03

    The wastes present at DOE long-term storage sites are usually highly alkaline, and because of this, much of the actinides in these wastes are in the sludge phase. Enough actinide materials still remain in the supernatant liquid that they require separation followed by long-term storage in a geological repository. The removal of these metals from the liquid waste stream would permit their disposal as low-level waste and dramatically reduce the volume of high-level wastes.

  15. Ultratrace analysis of transuranic actinides by laser-induced fluorescence

    DOEpatents

    Miller, Steven M.

    1988-01-01

    Ultratrace quantities of transuranic actinides are detected indirectly by their effect on the fluorescent emissions of a preselected fluorescent species. Transuranic actinides in a sample are coprecipitated with a host lattice material containing at least one preselected fluorescent species. The actinide either quenches or enhances the laser-induced fluorescence of the preselected fluorescent species. The degree of enhancement or quenching is quantitatively related to the concentration of actinide in the sample.

  16. Ultratrace analysis of transuranic actinides by laser-induced fluorescence

    DOEpatents

    Miller, S.M.

    1983-10-31

    Ultratrace quantities of transuranic actinides are detected indirectly by their effect on the fluorescent emissions of a preselected fluorescent species. Transuranic actinides in a sample are coprecipitated with a host lattice material containing at least one preselected fluorescent species. The actinide either quenches or enhances the laser-induced fluorescence of the preselected fluorescent species. The degree of enhancement or quenching is quantitatively related to the concentration of actinide in the sample.

  17. Characteristics of HCN removal using CaO at high temperatures

    SciTech Connect

    Houzhang Tan; Xuebin Wang; Congling Wang; Tongmo Xu

    2009-03-15

    Experimental investigation on the removal of hydrogen cyanide (HCN) using calcium oxide (CaO) was carried out in a fixed bed reactor at temperature ranging from 300 to 1173 K, and the original HCN was produced during the pyrolysis of pyridine. Effects of temperature, volume space velocity, and initial HCN concentration on HCN removal were discussed. The results of temperature-programmed experiments show that temperature is the main factor affecting HCN removal. With the formation of CO, HCN starts to decrease from 473 K, and remains unchanged from 673 to 873 K. At 873 K, there is a further decrease in HCN without CO formation, and when temperature is higher than 1023 K, HCN is removed completely. In the isothermal experiments, CaCN{sub 2} was detected at 723 K, but at higher temperatures of 923 and 1123 K, there was no CaCN{sub 2} in the solid residues, and the nitrogen in the removed HCN was equal to that in the formed N{sub 2}. This indicates that at a lower temperature CaO is consumed to remove HCN, CaO + 2HCN {yields} CaCN{sub 2} + CO + H{sub 2}; but at a higher temperature, CaO acts as a catalyst for HCN removal, 2C{sub i}H{sub j} + 2HCN {yields} N{sub 2} + (j + 1 - k)H{sub 2} + 2C{sub I} + 1H{sub k}. The investigation on the removal efficiency shows that there is a critical temperature and a critical volume space velocity at which the HCN removal efficiency is able to reach up to 100%. 41 refs., 9 figs., 2 tabs.

  18. The Actinide-Lanthanide Separation Process

    SciTech Connect

    Lumetta, Gregg J.; Gelis, Artem V.; Carter, Jennifer C.; Niver, Cynthia M.; Smoot, Margaret R.

    2014-02-21

    The Actinide-Lanthanide SEParation (ALSEP) process is described. The process uses an extractant phase consisting of either N,N,N',N'-tetraoctyldiglycolamide (TODGA) or N,N,N',N'-tetra(2 ethylhexyl)diglycolamide (T2EHDGA) combined with 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]). The neutral TODGA or T2EHDGA serves to co-extract the trivalent actinide and lanthanide ions from nitric acid media. Switching the aqueous phase chemistry to a citrate buffered diethylenetriaminepentaacetic acid (DTPA) solution at pH 2.5 to 4 results in selective transfer of the actinides to the aqueous phase, thus resulting in separation of these two groups of elements.

  19. Characteristics of ammonium removal by heterotrophic nitrification-aerobic denitrification by Alcaligenes faecalis No. 4.

    PubMed

    Joo, Hung-Soo; Hirai, Mitsuyo; Shoda, Makoto

    2005-08-01

    Alcaligenes faecalis no. 4 has heterotrophic nitrification and aerobic denitrification abilities. By taking the nitrogen balance under different culture conditions, 40-50% of removed NH4+-N was denitrified and about one-half of removed NH4+-N was converted to intracellular nitrogen. The maximum ammonium removal rate of no. 4 (28.9 mg-N/l/h) and its denitrification rate at high-strength NH4+-N of about 1200 ppm in aerated batch experiments at a C/N ratio of 10 were 5-40 times higher than those of other bacteria with the same ability. Only a few percent of the removed ammonium was converted to nitrite, and the main denitrification process was speculated to be via hydroxylamine which was produced by ammonium oxidation.

  20. Optimization of performance assessment and design characteristics in constructed wetlands for the removal of organic matter.

    PubMed

    Hijosa-Valsero, María; Sidrach-Cardona, Ricardo; Martín-Villacorta, Javier; Bécares, Eloy

    2010-10-01

    Some of the most used constructed wetland (CW) configurations [conventional and modified free-water (FW) flow, surface flow, conventional horizontal subsurface flow (SSF) and soilless systems with floating macrophytes (FM)] were assessed in order to compare their efficiencies for the removal of organic pollutants [COD, filtered COD (FCOD), BOD and total suspended solids (TSS)] from urban sewage under the same climatic and wastewater conditions. The removal performance was calculated using three approaches: effluent concentrations, areal removed loads and mass removal. Results were very different depending on the approach, which indicates that the way to present CW efficiency should be considered carefully. All CW-configurations obtained BOD effluent concentrations below 25 mg L(-1) in summer, with a FW-CW with effluent leaving through the bottom of the tank being the only one maintaining low BOD effluent concentrations even in winter and under high organic loading conditions. In this kind of CW, the presence of plants favoured pollutant removal. SSF-CWs were the most efficient for the removal of COD. FM systems can be as efficient as some gravel bed CWs. Typhaangustifolia worked better than Phragmitesaustralis, at least when the systems were at the beginning of their operation period.

  1. ENHANCED CHEMICAL CLEANING OF SRS WASTE TANKS TO IMPROVE ACTINIDE SOLUBILITY

    SciTech Connect

    Rudisill, T.; Thompson, M.

    2011-09-20

    Processes for the removal of residual sludge from SRS waste tanks have historically used solutions containing up to 0.9 M oxalic acid to dissolve the remaining material following sludge removal. The selection of this process was based on a comparison of a number of studies performed to evaluate the dissolution of residual sludge. In contrast, the dissolution of the actinide mass, which represents a very small fraction of the waste, has not been extensively studied. The Pu, Np, and Am in the sludge is reported to be present as hydrated and crystalline oxides. To identify aqueous solutions which have the potential to increase the solubility of the actinides, the alkaline and mildly acidic test solutions shown below were selected as candidates for use in a series of solubility experiments. The efficiency of the solutions in solubilizing the actinides was evaluated using a simulated sludge prepared by neutralizing a HNO{sub 3} solution containing Pu, Np, and Am. The hydroxide concentration was adjusted to a 1.2 M excess and the solids were allowed to age for several weeks prior to starting the experiments. The sludge was washed with 0.01 M NaOH to prepare the solids for use. Following the addition of an equal portion of the solids to each test solution, the concentrations of Pu, Np, and Am were measured as a function of time over a 792 h (33 day) period to provide a direct comparison of the efficiency of each solution in solubilizing the actinide elements. Although the composition of the sludge was limited to the hydrated actinide oxides (and did not contain other components of demonstrated importance), the results of the study provides guidance for the selection of solutions which should be evaluated in subsequent tests with a more realistic surrogate sludge and actual tank waste.

  2. Strong correlations in actinide redox reactions

    NASA Astrophysics Data System (ADS)

    Horowitz, S. E.; Marston, J. B.

    2011-02-01

    Reduction-oxidation (redox) reactions of the redox couples An(VI)/An(V), An(V)/An(IV), and An(IV)/An(III), where An is an element in the family of early actinides (U, Np, and Pu), as well as Am(VI)/Am(V) and Am(V)/Am(III), are modeled by combining density functional theory with a generalized Anderson impurity model that accounts for the strong correlations between the 5f electrons. Diagonalization of the Anderson impurity model yields improved estimates for the redox potentials and the propensity of the actinide complexes to disproportionate.

  3. The gastrointestinal absorption of the actinide elements.

    PubMed

    Harrison, J D

    1991-03-01

    The greatest uncertainty in dose estimates for the ingestion of long-lived, alpha-emitting isotopes of the actinide elements is in the values used for their fractional absorption from the gastrointestinal tract (f1 values). Recent years have seen a large increase in the available data on actinide absorption. Human data are reviewed here, together with animal data, to illustrate the effect on absorption of chemical form, incorporation into food materials, fasting and other dietary factors, and age at ingestion. The f1 values recommended by the International Commission on Radiological Protection, by an Expert Group of the Nuclear Energy Agency and by the National Radiological Protection Board are discussed.

  4. Strong correlations in actinide redox reactions.

    PubMed

    Horowitz, S E; Marston, J B

    2011-02-14

    Reduction-oxidation (redox) reactions of the redox couples An(VI)/An(V), An(V)/An(IV), and An(IV)/An(III), where An is an element in the family of early actinides (U, Np, and Pu), as well as Am(VI)/Am(V) and Am(V)/Am(III), are modeled by combining density functional theory with a generalized Anderson impurity model that accounts for the strong correlations between the 5f electrons. Diagonalization of the Anderson impurity model yields improved estimates for the redox potentials and the propensity of the actinide complexes to disproportionate.

  5. Study on characteristics of biocometabolic removal of omethoate by the Aspergillus spp.

    PubMed

    Chun, Meng; Chngchun, S; Yanghao, Guo; Shi Xian'ai; Jianfeng, Cheng; Fen, Yan

    2004-03-01

    A strain Aspergillus spp. F1 which could effectively metabolized omethoate was screened out in this study. F1 tended to form granula with diameter 4-5mm after 5 days culture in shaker. The pH range from 4.5 to 6.5 was the suitable pH range for growth and metabolism of Aspergillus spp. F1. The maximum omethoate removal rate was about 3.0mg/(hL), and the removal fraction of omethoate reached 90% after 8 days culture when initial concentrations of omethoate were not more than 2000mg/L in medium. There was no obvious relativity between cell growth and cometabolism of omethoate. Starch was the best carbon source for omethoate removal and the result after 3 days reached 56.6% removal. F1 could use omethoate to metabolize as single nitrogen or phosphate source. The residual fragments in medium after treatment with the Aspergillus spp. F1 were determined by gas chromatography-mass spectrometry. The analysis results showed that only fragment o,o,s,-trimethyl phosphorothioate (TEP) containing phosphorus was available and the fragment containing nitrogen was consumed by F1 thoroughly in culture process. But no accumulations of TEP were observed in the omethoate bioremediation process. F1 could effectively remove omethoate in complex nutritional environment safely.

  6. Conversion characteristics and production evaluation of styrene/o-xylene mixtures removed by DBD pretreatment.

    PubMed

    Jiang, Liying; Zhu, Runye; Mao, Yubo; Chen, Jianmeng; Zhang, Liang

    2015-01-26

    The combination of chemical oxidation methods with biotechnology to removal recalcitrant VOCs is a promising technology. In this paper, the aim was to identify the role of key process parameters and biodegradability of the degradation products using a dielectric barrier discharge (DBD) reactor, which provided the fundamental data to evaluate the possibilities of the combined system. Effects of various technologic parameters like initial concentration of mixtures, residence time and relative humidity on the decomposition and the degradation products were examined and discussed. It was found that the removal efficiency of mixed VOCs decreased with increasing initial concentration. The removal efficiency reached the maximum value as relative humidity was approximately 40%-60%. Increasing the residence time resulted in increasing the removal efficiency and the order of destruction efficiency of VOCs followed the order styrene > o-xylene. Compared with the single compounds, the removal efficiency of styrene and o-xylene in the mixtures of VOCs decreased significantly and o-xylene decreased more rapidly. The degradation products were analyzed by gas chromatography and gas chromatography-mass spectrometry, and the main compounds detected were O3, COx and benzene ring derivatives. The biodegradability of mixed VOCs was improved and the products had positive effect on biomass during plasma application, and furthermore typical results indicated that the biodegradability and biotoxicity of gaseous pollutant were quite depending on the specific input energy (SIE).

  7. Conversion Characteristics and Production Evaluation of Styrene/o-Xylene Mixtures Removed by DBD Pretreatment

    PubMed Central

    Jiang, Liying; Zhu, Runye; Mao, Yubo; Chen, Jianmeng; Zhang, Liang

    2015-01-01

    The combination of chemical oxidation methods with biotechnology to removal recalcitrant VOCs is a promising technology. In this paper, the aim was to identify the role of key process parameters and biodegradability of the degradation products using a dielectric barrier discharge (DBD) reactor, which provided the fundamental data to evaluate the possibilities of the combined system. Effects of various technologic parameters like initial concentration of mixtures, residence time and relative humidity on the decomposition and the degradation products were examined and discussed. It was found that the removal efficiency of mixed VOCs decreased with increasing initial concentration. The removal efficiency reached the maximum value as relative humidity was approximately 40%–60%. Increasing the residence time resulted in increasing the removal efficiency and the order of destruction efficiency of VOCs followed the order styrene > o-xylene. Compared with the single compounds, the removal efficiency of styrene and o-xylene in the mixtures of VOCs decreased significantly and o-xylene decreased more rapidly. The degradation products were analyzed by gas chromatography and gas chromatography-mass spectrometry, and the main compounds detected were O3, COx and benzene ring derivatives. The biodegradability of mixed VOCs was improved and the products had positive effect on biomass during plasma application, and furthermore typical results indicated that the biodegradability and biotoxicity of gaseous pollutant were quite depending on the specific input energy (SIE). PMID:25629961

  8. NEW METHOD FOR DETERMINATION OF ACTINIDES AND STRONTIUM IN ANIMAL TISSUE

    SciTech Connect

    Maxwell, S; Jay Hutchison, J; Don Faison, D

    2007-05-07

    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.

  9. Adsorption Characteristics of Macroporous Resin for Oil Removal from Desulphurization Wastewater on Board

    NASA Astrophysics Data System (ADS)

    Li, Tie; Chen, Chen; Jin, Qi; Zhao, Jiao; Tang, Xiaojia; Zhu, Yimin

    2017-01-01

    According to our previous results on the magnesium-based exhaust gas cleaning system (Mg-EGCS), PAHs and total oil content were the main factors affecting the COD in the wastewater. In this work, three kinds of adsorption materials were investigated and macroporous resin was selected for oil removal. The effects of the dosage of macroporous resin, adsorption time and the flow rate were studied, and thermodynamics equation was used to characterize the adsorption process. The results showed that macroporous resin is a good candidate for oil removal from desulphurization wastewater on board, and the COD after treatment can meet the discharge criteria set by the International Maritime Organization (IMO).

  10. Material removal characteristics of orthogonal velocity polishing tool for efficient fabrication of CVD SiC mirror surfaces

    NASA Astrophysics Data System (ADS)

    Seo, Hyunju; Han, Jeong-Yeol; Kim, Sug-Whan; Seong, Sehyun; Yoon, Siyoung; Lee, Kyungmook; Lee, Haengbok

    2015-09-01

    Today, CVD SiC mirrors are readily available in the market. However, it is well known to the community that the key surface fabrication processes and, in particular, the material removal characteristics of the CVD SiC mirror surface varies sensitively depending on the shop floor polishing and figuring variables. We investigated the material removal characteristics of CVD SiC mirror surfaces using a new and patented polishing tool called orthogonal velocity tool (OVT) that employs two orthogonal velocity fields generated simultaneously during polishing and figuring machine runs. We built an in-house OVT machine and its operating principle allows for generation of pseudo Gaussian shapes of material removal from the target surface. The shapes are very similar to the tool influence functions (TIFs) of other polishing machine such as IRP series polishing machines from Zeeko. Using two CVD SiC mirrors of 150 mm in diameter and flat surface, we ran trial material removal experiments over the machine run parameter ranges from 12.901 to 25.867 psi in pressure, 0.086 m/sec to 0.147 m/sec in tool linear velocity, and 5 to 15 sec in dwell time. An in-house developed data analysis program was used to obtain a number of Gaussian shaped TIFs and the resulting material removal coefficient varies from 3.35 to 9.46 um/psi hour m/sec with the mean value to 5.90 ± 1.26(standard deviation). We report the technical details of the new OVT machine, of the data analysis program, of the experiments and the results together with the implications to the future development of the OVT machine and process for large CVD SiC mirror surfaces.

  11. DNAPL REMOVAL MECHANISMS AND MASS TRANSFER CHARACTERISTICS DURING COSOLVENT-AIR FLOODING

    EPA Science Inventory

    The concurrent injection of cosolvent and air, a cosolvent-air (CA) flood was recently suggested for a dense nonaqueous phase liquid (DNAPL) remediation technology. The objectives of this study were to elucidate the DNAPL removal mechanisms of the CA flood and to quantify mass t...

  12. Rapid method to determine actinides and 89/90Sr in limestone and marble samples

    SciTech Connect

    Maxwell, Sherrod L.; Culligan, Brian; Hutchison, Jay B.; Utsey, Robin C.; Sudowe, Ralf; McAlister, Daniel R.

    2016-04-12

    A new method for the determination of actinides and radiostrontium in limestone and marble samples has been developed that utilizes a rapid sodium hydroxide fusion to digest the sample. Following rapid pre-concentration steps to remove sample matrix interferences, the actinides and 89/90Sr are separated using extraction chromatographic resins and measured radiometrically. The advantages of sodium hydroxide fusion versus other fusion techniques will be discussed. Lastly, this approach has a sample preparation time for limestone and marble samples of <4 hours.

  13. Actinide measurements by AMS using fluoride matrices

    NASA Astrophysics Data System (ADS)

    Cornett, R. J.; Kazi, Z. H.; Zhao, X.-L.; Chartrand, M. G.; Charles, R. J.; Kieser, W. E.

    2015-10-01

    Actinides can be measured by alpha spectroscopy (AS), mass spectroscopy or accelerator mass spectrometry (AMS). We tested a simple method to separate Pu and Am isotopes from the sample matrix using a single extraction chromatography column. The actinides in the column eluent were then measured by AS or AMS using a fluoride target matrix. Pu and Am were coprecipitated with NdF3. The strongest AMS beams of Pu and Am were produced when there was a large excess of fluoride donor atoms in the target and the NdF3 precipitates were diluted about 6-8 fold with PbF2. The measured concentrations of 239,240Pu and 241Am agreed with the concentrations in standards of known activity and with two IAEA certified reference materials. Measurements of 239,240Pu and 241Am made at A.E. Lalonde AMS Laboratory agree, within their statistical uncertainty, with independent measurements made using the IsoTrace AMS system. This work demonstrated that fluoride targets can produce reliable beams of actinide anions and that the measurement of actinides using fluorides agree with published values in certified reference materials.

  14. Rapid determination of actinides in asphalt samples

    SciTech Connect

    Maxwell, Sherrod L.; Culligan, Brian K.; Hutchison, Jay B.

    2014-01-12

    A new rapid method for the determination of actinides in asphalt samples has been developed that can be used in emergency response situations or for routine analysis If a radiological dispersive device (RDD), Improvised Nuclear Device (IND) or a nuclear accident such as the accident at the Fukushima Nuclear Power Plant in March, 2011 occurs, there will be an urgent need for rapid analyses of many different environmental matrices, including asphalt materials, to support dose mitigation and environmental clean up. The new method for the determination of actinides in asphalt utilizes a rapid furnace step to destroy bitumen and organics present in the asphalt and sodium hydroxide fusion to digest the remaining sample. Sample preconcentration steps are used to collect the actinides and a new stacked TRU Resin + DGA Resin column method is employed to separate the actinide isotopes in the asphalt samples. The TRU Resin plus DGA Resin separation approach, which allows sequential separation of plutonium, uranium, americium and curium isotopes in asphalt samples, can be applied to soil samples as well.

  15. Rapid determination of actinides in asphalt samples

    DOE PAGES

    Maxwell, Sherrod L.; Culligan, Brian K.; Hutchison, Jay B.

    2014-01-12

    A new rapid method for the determination of actinides in asphalt samples has been developed that can be used in emergency response situations or for routine analysis If a radiological dispersive device (RDD), Improvised Nuclear Device (IND) or a nuclear accident such as the accident at the Fukushima Nuclear Power Plant in March, 2011 occurs, there will be an urgent need for rapid analyses of many different environmental matrices, including asphalt materials, to support dose mitigation and environmental clean up. The new method for the determination of actinides in asphalt utilizes a rapid furnace step to destroy bitumen and organicsmore » present in the asphalt and sodium hydroxide fusion to digest the remaining sample. Sample preconcentration steps are used to collect the actinides and a new stacked TRU Resin + DGA Resin column method is employed to separate the actinide isotopes in the asphalt samples. The TRU Resin plus DGA Resin separation approach, which allows sequential separation of plutonium, uranium, americium and curium isotopes in asphalt samples, can be applied to soil samples as well.« less

  16. Semi-empirical models of actinide alloying

    NASA Astrophysics Data System (ADS)

    Gibson, John K.; Haire, Richard G.; Ogawa, Toru

    1999-07-01

    Alloys of Np have been studied less than those of the neighboring elements, U and Pu; the higher actinides have received even less attention. Recent interest in 237Np, 241Am and other actinide isotopes as significant, long-lived and highly radiotoxic nuclear waste components, and particularly the roles of metallic materials in new handling/separations and remediation technologies, demands that this paucity of information concerning alloy behaviors be addressed. An additional interest in these materials arises from the possibility of revealing fundamental properties and bonding interactions, which would further characterize the unique electronic structures (e.g., 5f electrons) of the actinide elements. The small empirical knowledge basis presently available for understanding and modeling the alloying behavior of Np is summarized here, with emphasis on our recent results for the Np-Am, Np-Zr and Np-Fe phase diagrams. In view of the limited experimental data base for neptunium and the transplutonium metals, the value of semi-empirical intermetallic bonding models for predicting actinide alloy thermodynamics is evaluated.

  17. Potential agents for removal of actinides from waste solutions

    SciTech Connect

    Romanovski, V.V.; Whisenhunt, D.W.; Veeck, A.C.; Andersen, W.A.; Hoffman, D.C.; Jide, X.; White, D.; Raymond, K.N.

    1996-07-01

    The uptake of Th(IV) from nitric acid and hydrochloric acid solutions by chelating ion exchange resins containing catechol, 1,2- hydroxypyridinone (1,2-HOPO) and 3,4-hydroxypyridinone (3,4-HOPO) functional groups, has been investigated. These polystyrene based materials show excellent kinetics for uptake of Th(IV) and have a high loading capacity. Liquid/liquid extractants have also been synthesized by addition of lipophilic side chains to the chelating groups (1,2-HOPO; 3,4-HOPO; 3,2-HOPO; catecholamide; terephthalamide). The initial evaluation of the extraction properties has been carried out.

  18. APPLICATION OF ABSORPTION SPECTROSCOPY TO ACTINIDE PROCESS ANALYSIS AND MONITORING

    SciTech Connect

    Lascola, R.; Sharma, V.

    2010-06-03

    The characteristic strong colors of aqueous actinide solutions form the basis of analytical techniques for actinides based on absorption spectroscopy. Colorimetric measurements of samples from processing activities have been used for at least half a century. This seemingly mature technology has been recently revitalized by developments in chemometric data analysis. Where reliable measurements could formerly only be obtained under well-defined conditions, modern methods are robust with respect to variations in acidity, concentration of complexants and spectral interferents, and temperature. This paper describes two examples of the use of process absorption spectroscopy for Pu analysis at the Savannah River Site, in Aiken, SC. In one example, custom optical filters allow accurate colorimetric measurements of Pu in a stream with rapid nitric acid variation. The second example demonstrates simultaneous measurement of Pu and U by chemometric treatment of absorption spectra. The paper concludes with a description of the use of these analyzers to supplement existing technologies in nuclear materials monitoring in processing, reprocessing, and storage facilities.

  19. Actinide nuclear data for reactor physics calculations

    SciTech Connect

    Brady, M.C.; Wright, R.Q. ); England, T.R. )

    1991-07-01

    Calculational methodologies and data sources used to predict and recommend fission-product yields and delayed neutron and prompt neutron data for a number of actinide nuclides are presented and discussed. This compilation of nuclear data is the result of a nearly three-year effort under the Japan/US Actinide Program (JUSAP) at Oak Ridge National Laboratory to provide nuclear data supporting the preliminary design of an actinide burner reactor. In this type of reactor, minor actinides are the major components of the fuel. Nuclear data for these minor actinides are, therefore, essential in the design of such reactors. Fission yield, delayed neutron, and prompt neutron data are presented in the report for the following nuclides: Neptumium-237, Plutonium-238, -240, and -242, Americium-241 and -243, and Curium-242, -243, -244, -246, and -248. Additionally, prompt neutron data are also presented for these nuclides (except Plutonium-240, -242 and Curium-242) and for Curium-245 and -247. As in all compilations of nuclear data, the information in this report is subject to change as newer data become available. Most of the data presented here are based on calculational methodologies and should be revised as experimental data become available. The release of Version 6 of the Evaluated Nuclear Data Files (ENDF/B-6) is expected to be completed in 1991 and should replace this evaluation in areas of overlap although no serious discrepancies are expected between this compilation and ENDF/B-6. Because of the large amount of data comprising this compilation and limitations in publishing such a voluminous report, a complete listing of the explicit data is not included in this report. The data are, however, available from the authors on 5 {1/2}-in. high-density (1.2-Mbyte) diskettes. The file contents and formats are described in the text, and examples are given in the appendices. 34 refs., 18 tabs.

  20. The use of Diphonix{sup {trademark}} ion exchange resin as a preconcentration step for the lanthanides and actinides in analytical applications

    SciTech Connect

    Rollins, A.N.; Thakkar, A.H.; Fern, M.J.

    1995-12-01

    Diphonix ion exchange resin is a chelating ion exchange resin containing sulfonic and gemdiphosphonic acid groups. This resin has a high specificity for the lanthanides and actinides, especially at acidities below pH = 3. Currently, we are investigating new ways to use Diphonix resin as a preconcentration step to separate the lanthanides and actinides from interfering elements present in a variety of environmental matrices. Once the lanthanides and actinides have been separated from the interfering matrix constituents, the elements are removed from the resin and passed through subsequent separation schemes. This presentation will outline the use of Diphonix resin with a variety of problem matrices, and demonstrate its usefulness for analysis of the lanthanides and actinides.

  1. Occurrence, removal and release characteristics of dissolved brominated flame retardants and their potential metabolites in various kinds of wastewater.

    PubMed

    Kim, Un-Jung; Lee, In-Seok; Oh, Jeong-Eun

    2016-11-01

    The dissolved phase compound and congener specific distribution characteristics of three widely used brominated flame retardants (BFRs) comprising 27 polybrominated diphenyl ethers (PBDEs), 12 hydroxylated and methoxylated metabolites (OH- and MeO-BDEs), 3 hexabromocyclododecanes (HBCDs) and tetrabromobisphenol A (TBBPA) were investigated in influents and effluents of various kinds of wastewater treatment plants (WWTPs), with varying source of wastewater and type of treatment, and nearby rivers in Korea. The concentration of total BFRs were the highest in industrial WWTPs nearby large industrial complexes specialized in heavy chemicals. The distribution of BFRs was differed according to composition of wastewater, with predominance of TBBPA in WWTPs with higher portion of inflowing industrial wastewater. Among HBCD diastereomers, γ-HBCD was dominant in industrial wastewater as consistent to the previous reports, however, similar contribution of α- and γ-HBCD was found in sewage and human wastewater. Through treatment process, PBDEs were the most effectively removed with a mean removal efficiency of 68.3%. HBCDs and TBBPA had removal efficiencies of 41.3% and 48.7%, respectively. The lowest removal efficiency (10.3%) was observed for PBDE metabolites and their concentration in effluent of human wastewater was even increased at maximum 1.9 fold compared with influent, implying the possibility of transformation during treatment. The estimated dissolved phase daily load of PBDEs was highest in sewage while that of TBBPA was highest in industrial wastewater.

  2. The removal characteristics of natural organic matter in the recycling of drinking water treatment sludge: Role of solubilized organics.

    PubMed

    Zhou, Zhiwei; Yang, Yanling; Li, Xing; Ji, Siyang; Zhang, Hao; Wang, Shuai; Zeng, Qingping; Han, Xinghang

    2016-01-01

    To clarify the role of solubilized organics derived from drinking water treatment sludge (DWTS) in the elimination of natural organic matter (NOM) in the DWTS recycling process, a probe sonoreactor at a frequency of 25 kHz was used to solubilize the organics at varied specific energies. The coagulation behavior related to NOM removal in recycling the sonicated DWTS with and without solubilized organics was evaluated, and the effect on organic fractionations in coagulated water was determined. The study results could provide useful implications in designing DWTS recycling processes that avoid the enrichment of organic matter. Our results indicate that DWTS was disrupted through a low release of soluble chemical oxygen demand (SCOD) and proteins, which could deteriorate the coagulated water quality under the specific energy of 37.87-1212.1 kW h/kg TS. The optimal coagulation behavior for NOM removal was achieved by recycling the sonicated DWTS without solubilized organics at 151.5 kW h/kg TS specific energy. Recycling the sonicated DWTS could increase the enrichment potential of weakly hydrophobic acid, hydrophilic matter, and <3 kDa fractions; the enrichment risks could be reduced by discharging the solubilized organics. Fluorescent characteristic analysis indicated that when recycling the sonicated DWTS without solubilized organics, the removal of humic-like substances was limited, whereas removal of protein-like substances was enhanced, lowering the enrichment potential of protein-like substances.

  3. [Removal Characteristics of Elemental Mercury by Mn-Ce/molecular Sieve].

    PubMed

    Tan, Zeng-qiang; Niu, Guo-ping; Chen, Xiao-wen; An, Zhen

    2015-06-01

    The impregnation method was used to support molecular sieve with active manganese and cerium components to obtain a composite molecular sieve catalyst. The mercury removal performance of the catalyst was studied with a bench-scale setup. XPS analysis was used to characterize the sample before and after the modification in order to study the changes in the active components of the catalyst prepared. The results showed that the catalyst carrying manganese and cerium components had higher oxidation ability of elemental mercury in the temperature range of 300 degrees C - 450 degrees C, especially at 450 degrees C, the oxidation efficiency of elemental mercury was kept above 80%. The catalyst had more functional groups that were conducive to the oxidation of elemental mercury, and the mercury removal mainly depended on the chemical adsorption. The SO2 and NO in flue gas could inhibit the oxidation of elemental mercury to certain extent.

  4. Tribology and Removal Rate Characteristics of Chemical Mechanical Planarization Pads Containing Water Soluble Particles

    NASA Astrophysics Data System (ADS)

    Charns, L.; Philipossian, A.

    2006-07-01

    Novel non-porous pads incorporating different amounts of embedded water soluble particles (WSP) have been characterized and compared to a conventional porous pad for interlayer dielectric (ILD) chemical mechanical planarization (CMP) applications. Removal rate results indicated that polishing with WSP pads was Prestonian in nature (similar to conventional porous pads). A decrease in removal rate at high combinations of pressure and velocity was observed during in-situ conditioning with WSP pads. This anomalous behavior was most likely due to the alternatively feeding and starving the wafer of slurry during in-situ conditioning since doubling the flow rate resolved the problem. The anomalous behavior, however, was not observed when conditioning was performed ex-situ. Frictional analysis indicated that polishing with WSP pads proceeded via boundary lubrication like the other porous pads with concentrically grooved surface geometries.

  5. Synthesis of Functionalized Superparamagnetic Iron Oxide Nanoparticles from a Common Precursor and their Application as Heavy Metal and Actinide Sorbents

    SciTech Connect

    Warner, Marvin G.; Warner, Cynthia L.; Addleman, Raymond S.; Droubay, Timothy C.; Engelhard, Mark H.; Davidson, Joseph D.; Cinson, Anthony D.; Nash, Michael A.; Yantasee, Wassana

    2009-10-12

    We describe the use of a simple and versatile technique to generate a series of ligand stabilized iron oxide nanoparticles containing different functionalities with specificities toward heavy metals and actinides at the periphery of the stabilizing ligand shell from a common, easy to synthesize precursor nanoparticle. The resulting nanoparticles are designed to contain affinity ligands that make them excellent sorbent materials for a variety of heavy metals from contaminated aqueous systems such as river water and ground water as well as actinides from clinical samples such as blood and urine. Functionalized superparamagnetic nanoparticles make ideal reagents for extraction of heavy metal and actinide contaminants from environmental and clinical samples since they are easily removed from the media once bound to the contaminant by simply applying a magnetic field. In addition, these engineered nanomaterials have an inherently high active surface area (often > 100 m2/g) making them ideal sorbent materials for these types of applications

  6. Adventures in Actinide Chemistry: A Year of Exploring Uranium and Thorium in Los Alamos

    SciTech Connect

    Pagano, Justin

    2016-01-08

    The first part of this collection of slides is concerned with considerations when working with actinides. The topics discussed in the document as a whole are the following: Actinide chemistry vs. transition metal chemistry--tools we can use; New synthetic methods to obtain actinide hydrides; Actinide metallacycles: synthesis, structure, and properties; and Reactivity of actinide metallacycles.

  7. Plutonium Futures -- The Science. Topical Conference on Plutonium and Actinides. AIP Conference Proceedings, No. 532 [APCPCS

    SciTech Connect

    Pillay, K.K.S.; Kim, K.C.

    2000-12-31

    Presentations at this conference covered the topics of materials science/nuclear fuels, condensed matter physics, actinides in the environment/separation and analysis, actinides/processing, actinides/TRU wastes, materials science, TRU waste forms, nuclear fuels/isotopes, separations and process chemistry, actinides in the environment, detection and analysis, Pu and Pu compounds, actinide compounds and complexes.

  8. Effects of removing Good Hope Mill Dam on selected physical, chemical, and biological characteristics of Conodoguinet Creek, Cumberland County, Pennsylvania

    USGS Publications Warehouse

    Chaplin, Jeffrey J.; Brightbill, Robin A.; Bilger, Michael D.

    2005-01-01

    The implications of dam removal on channel characteris-tics, water quality, benthic invertebrates, and fish are not well understood because of the small number of removals that have been studied. Comprehensive studies that document the effects of dam removal are just beginning to be published, but most research has focused on larger dams or on the response of a sin-gle variable (such as benthic invertebrates). This report, pre-pared in cooperation with the Conodoguinet Creek Watershed Association, provides an evaluation of how channel morphol-ogy, bed-particle-size distribution, water quality, benthic inver-tebrates, fish, and aquatic habitat responded after removal of Good Hope Mill Dam (a small 'run of the river' dam) from Conodoguinet Creek in Cumberland County, Pa. Good Hope Mill Dam was a 6-foot high, 220-foot wide concrete structure demolished and removed over a 3-day period beginning with the initial breach on November 2, 2001, at 10:00 a.m. eastern standard time. To isolate the effects of dam removal, data were collected before and after dam removal at five monitoring stations and over selected reaches upstream, within, and downstream of the impoundment. Stations 1, 2, and 5 were at free-flowing control locations 4.9 miles upstream, 2.5 miles upstream, and 5 miles downstream of the dam, respec-tively. Stations 3 and 4 were located where the largest responses were anticipated, 115 feet upstream and 126 feet downstream of the dam, respectively Good Hope Mill Dam was not an effective barrier to sedi-ment transport. Less than 3 inches of sediment in the silt/clay-size range (less than 0.062 millimeters) coated bedrock within the 7,160-foot (1.4-mile) impoundment. The bedrock within the impoundment was not incised during or after dam removal, and the limited sediment supply resulted in no measurable change in the thalweg elevation downstream of the dam. The cross-sec-tional areas at stations 3 and 4, measured 17 days and 23 months after dam removal, were within

  9. Linking the mobilization of dissolved organic matter in catchments and its removal in drinking water treatment to its molecular characteristics.

    PubMed

    Raeke, Julia; Lechtenfeld, Oliver J; Tittel, Jörg; Oosterwoud, Marieke R; Bornmann, Katrin; Reemtsma, Thorsten

    2017-04-15

    Drinking water reservoirs in the Northern Hemisphere are largely affected by the decadal-long increase in riverine dissolved organic carbon (DOC) concentrations. The removal of DOC in drinking water treatment is costly and predictions are needed to link DOC removal efficiency to its mobilization in catchments, both of which are determined by the molecular composition. To study the effect of hydrological events and land use on the molecular characteristics of dissolved organic matter (DOM), 36 samples from three different catchment areas in the German low mountain ranges, with DOC concentrations ranging from 3 to 32 mg L(-1), were examined. Additionally, nine pairs of samples from downstream drinking water reservoirs were analyzed before and after flocculation. The molecular composition and the age of DOM were analyzed using ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) and radiocarbon ((14)C) analysis. At elevated discharge in a forested catchment comparatively younger, more oxygenated and unsaturated molecules of higher molecular weight were preferentially mobilized, likely linked to the reductive mobilization of iron. DOM with highly similar molecular characteristics (O/C ratio > 0.5, m/z > 500) could also be efficiently removed through flocculation in drinking water treatment. The proportion of DOM removed through flocculation ranged between 43% and 73% of DOC and was highest at elevated discharge. In catchment areas with a higher percentage of grassland and agriculture a higher proportion of DOM molecules containing sulfur and nitrogen was detected, which in turn could be less efficiently flocculated. Altogether, it was shown that DOM that is released during large hydrological events can be efficiently flocculated again, suggesting a reversal of similar chemical mechanisms in both processes. Since the occurrence of heavy rainfall events is predicted to increase in the future, event-driven mobilization of DOC

  10. Synthesis of actinide nitrides, phosphides, sulfides and oxides

    DOEpatents

    Van Der Sluys, William G.; Burns, Carol J.; Smith, David C.

    1992-01-01

    A process of preparing an actinide compound of the formula An.sub.x Z.sub.y wherein An is an actinide metal atom selected from the group consisting of thorium, uranium, plutonium, neptunium, and americium, x is selected from the group consisting of one, two or three, Z is a main group element atom selected from the group consisting of nitrogen, phosphorus, oxygen and sulfur and y is selected from the group consisting of one, two, three or four, by admixing an actinide organometallic precursor wherein said actinide is selected from the group consisting of thorium, uranium, plutonium, neptunium, and americium, a suitable solvent and a protic Lewis base selected from the group consisting of ammonia, phosphine, hydrogen sulfide and water, at temperatures and for time sufficient to form an intermediate actinide complex, heating said intermediate actinide complex at temperatures and for time sufficient to form the actinide compound, and a process of depositing a thin film of such an actinide compound, e.g., uranium mononitride, by subliming an actinide organometallic precursor, e.g., a uranium amide precursor, in the presence of an effectgive amount of a protic Lewis base, e.g., ammonia, within a reactor at temperatures and for time sufficient to form a thin film of the actinide compound, are disclosed.

  11. [Coagulation characteristics of different Al species on humic acid removal from water].

    PubMed

    Wu, Zhen; Zhang, Pan-Yue; Zeng, Guang-Ming; Gao, Ying; Xiao, Hui-Huang; Zhou, Fan

    2008-07-01

    Polyaluminum chloride PAC-Al13 with high Al13 content and PAC-Al30 with high Al30 content were prepared. Coagulation behaviors of PAC-Al30, PAC-Al13 and AlCl3 for humic acid removal from water were compared by jar-test. The floc growth, the charge neutralization capacity, the effect of pH and coagulant dosage on coagulation efficiency were investigated, and the residual aluminium in the purified water was considered. The results show that the order of the floc formation capacity is PAC-Al30 > PAC-Al13 > AlCl3. PAC-Al30 and PAC-Al13 have a broader effective pH range of 5.0-8.0, compared with AlCl3. The difference of charge neutralization capacity between PAC-Al30 and PAC-Al13 is not significant, but PAC-Al30 performs a more effective coagulation at low coagulant dosages because of its stronger adsorption and bridging, and PAC-Al30 has a broader effective dosage range of 0.08-0.64 mmol/L, compared with AlCl3 and PAC-Al13. The humic acid removal reaches 98.5% at a pH of 7.0 and a PAC-Al30 dosage of 0.16 mmol/L for the sample water with a humic acid content of 10 mg/L; and the residual aluminum in the purified water is 0.066 mg/L. The results verify that Al30 is another highly efficient coagulation/flocculation species for humic acid removal.

  12. Electrorecovery of actinides at room temperature

    SciTech Connect

    Stoll, Michael E; Oldham, Warren J; Costa, David A

    2008-01-01

    There are a large number of purification and processing operations involving actinide species that rely on high-temperature molten salts as the solvent medium. One such application is the electrorefining of impure actinide metals to provide high purity material for subsequent applications. There are some drawbacks to the electrodeposition of actinides in molten salts including relatively low yields, lack of accurate potential control, maintaining efficiency in a highly corrosive environment, and failed runs. With these issues in mind we have been investigating the electrodeposition of actinide metals, mainly uranium, from room temperature ionic liquids (RTILs) and relatively high-boiling organic solvents. The RTILs we have focused on are comprised of 1,3-dialkylimidazolium or quaternary ammonium cations and mainly the {sup -}N(SO{sub 2}CF{sub 3}){sub 2} anion [bis(trif1uoromethylsulfonyl)imide {equivalent_to} {sup -}NTf{sub 2}]. These materials represent a class of solvents that possess great potential for use in applications employing electrochemical procedures. In order to ascertain the feasibility of using RTILs for bulk electrodeposition of actinide metals our research team has been exploring the electron transfer behavior of simple coordination complexes of uranium dissolved in the RTIL solutions. More recently we have begun some fundamental electrochemical studies on the behavior of uranium and plutonium complexes in the organic solvents N-methylpyrrolidone (NMP) and dimethylsulfoxide (DMSO). Our most recent results concerning electrodeposition will be presented in this account. The electrochemical behavior of U(IV) and U(III) species in RTILs and the relatively low vapor pressure solvents NMP and DMSO is described. These studies have been ongoing in our laboratory to uncover conditions that will lead to the successful bulk electrodeposition of actinide metals at a working electrode surface at room temperature or slightly elevated temperatures. The RTILs we

  13. Effect of silver and palladium on dye-removal characteristics of anatase-titania nanotubes.

    PubMed

    Harsha, N; Ranya, R; Shukla, S; Biju, S; Reddy, M L P; Warrier, K G K

    2011-03-01

    Anatase-titania nanotubes have been synthesized via hydrothermal and surface-modified by depositing silver and palladium via ultraviolet-reduction method. The pure and surface-modified anatase-titania nanotubes have been characterized using the transmission electron microscope, selected-area electron diffraction, X-ray diffraction, diffuse reflectance, photoluminescence, and Fourier transform infrared spectroscope to reveal their average size, structure, and surface-chemistry. The nanotubes have been utilized for the dye-removal application involving the surface-adsorption mechanism under the dark-condition and photocatalytic degradation mechanism under the ultraviolet-radiation exposure. The variation in the dye-concentration during the dye-adsorption and photocatalysis processes has been determined using the ultraviolet-visible absorption spectrophotometer with methylene blue as a model catalytic dye-agent. It has been shown that silver-deposited anatase-titania nanotubes are more effective in enhancing the kinetics of the dye-removal via surface-adsorption and photocatalytic degradation mechanisms relative to the palladium-deposited anatase-titania nanotubes, which has been attributed to the differences in the surface-chemistry of anatase-titania nanotubes induced by the respective metal-deposition.

  14. Enantioselective Characteristics and Montmorillonite-Mediated Removal Effects of α-Hexachlorocyclohexane in Laying Hens.

    PubMed

    Liu, Xueke; Shen, Zhigang; Wang, Peng; Liu, Chang; Yao, Guojun; Zhou, Zhiqiang; Liu, Donghui

    2016-06-07

    α-Hexachlorocyclohexane (α-HCH) is a chiral organochlorine pesticide that is often ubiquitously detected in various environmental matrices and may be absorbed by the human body via food consumption, with serious detriments to human health. In this study, enantioselective degradation kinetics and residues of α-HCH in laying hens were investigated after a single dose of exposure to the pesticide, whereas enantioselectivity and residues of α-HCH in eggs, droppings, and various tissues were investigated after long-term exposure. Meanwhile, montmorillonite (MMT), a feed additive with high capacity of adsorption, was investigated for its ability to remove α-HCH from laying hens. Most non-brain tissues enantioselectively accumulated (-)-α-HCH, while (+)-α-HCH was preferentially accumulated in the brain. The enantiomer fractions (EFs) in most tissues gradually decreased, implying continuous depletion of (+)-α-HCH in laying hens. After 30 days of exposure and 31 days of elimination, the concentration of α-HCH in eggs and tissues of laying hens with MMT-containing feed was lower than that with MMT-free feed, indicating the removal effects of MMT for α-HCH in laying hens. The findings presented herein suggest that modified MMT may potentially be useful in reducing the enrichment of α-HCH in laying hens and eggs, thus lowering the risk of human intake of α-HCH.

  15. Actinide Isotopes for the Synthesis of Superheavy Nuclei

    NASA Astrophysics Data System (ADS)

    Roberto, J. B.; Alexander, C. W.; Boll, R. A.; Dean, D. J.; Ezold, J. G.; Felker, L. K.; Rykaczewski, K. P.

    2014-09-01

    Recent research resulting in the synthesis of isotopes of new elements 113-118 has demonstrated the importance of actinide targets in superheavy element research. Oak Ridge National Laboratory (ORNL) has unique facilities for the production and processing of actinide target materials, including the High Flux Isotope Reactor (HFIR) and the Radiochemical Engineering Development Center (REDC). These facilities have provided actinide target materials that have been used for the synthesis of all superheavy (SHE) elements above Copernicium (element 112). In this paper, the use of actinide targets for SHE research and discovery is described, including recent results for element 117 using 249Bk target material from ORNL. ORNL actinide capabilities are reviewed, including production and separation/purification, availabilities of actinide materials, and future opportunities including novel target materials such as 251Cf.

  16. Collection of lanthanides and actinides from natural waters with conventional and nanoporous sorbents.

    PubMed

    Johnson, Bryce E; Santschi, Peter H; Chuang, Chia-Ying; Otosaka, Shigeyoshi; Addleman, Raymond Shane; Douglas, Matt; Rutledge, Ryan D; Chouyyok, Wilaiwan; Davidson, Joseph D; Fryxell, Glen E; Schwantes, Jon M

    2012-10-16

    Effective collection of trace-level lanthanides and actinides is advantageous for recovery and recycling of valuable resources, environmental remediation, chemical separations, and in situ monitoring. Using isotopic tracers, we have evaluated a number of conventional and nanoporous sorbent materials for their ability to capture and remove selected lanthanides (Ce and Eu) and actinides (Th, Pa, U, and Np) from fresh and salt water systems. In general, the nanostructured materials demonstrated a higher level of performance and consistency. Nanoporous silica surface modified with 3,4-hydroxypyridinone provided excellent collection and consistency in both river water and seawater. The MnO(2) materials, in particular the high surface area small particle material, also demonstrated good performance. Other conventional sorbents typically performed at levels below the nanostructured sorbents and demonstrate a larger variability and matrix dependency.

  17. Microbial Transformations of Actinides and Other Radionuclides

    SciTech Connect

    Francis,A.J.; Dodge, C. J.

    2009-01-07

    Microorganisms can affect the stability and mobility of the actinides and other radionuclides released from nuclear fuel cycle and from nuclear fuel reprocessing plants. Under appropriate conditions, microorganisms can alter the chemical speciation, solubility and sorption properties and thus could increase or decrease the concentrations of radionuclides in solution in the environment and the bioavailability. Dissolution or immobilization of radionuclides is brought about by direct enzymatic action or indirect non-enzymatic action of microorganisms. Although the physical, chemical, and geochemical processes affecting dissolution, precipitation, and mobilization of radionuclides have been extensively investigated, we have only limited information on the effects of microbial processes and biochemical mechanisms which affect the stability and mobility of radionuclides. The mechanisms of microbial transformations of the major and minor actinides U, Pu, Cm, Am, Np, the fission products and other radionuclides such as Ra, Tc, I, Cs, Sr, under aerobic and anaerobic conditions in the presence of electron donors and acceptors are reviewed.

  18. Chemistry of the actinide elements. Second edition

    SciTech Connect

    Katz, J.J.; Seaborg, G.T.; Morss, L.R.

    1987-01-01

    This is an exhaustive, updated discourse on the chemistry of Actinides, Volume 1 contains a systematic coverage of the elements Ac, Th, Pa, U, Np, and Pu, which constitutes Part 1 of the work. The characterization of each element is discussed in terms of its nuclear properties, occurrence, preparation, atomic and metallic properties, chemistry of specific compounds, and solution chemistry. The first part of Volume 2 follows the same format as Volume 1 but is confined to the elements Am, Cm, Bk, Cf, and Es, plus a more condensed coverage of the Transeinsteinium elements (Fm, Md, No, Lw, and 104-109). Part 2 of this volume is devoted to a discussion of the actinide elements in general, with a specific focus on electronic spectra, thermodynamic and magnetic properties, the metallic state, structural chemistry, solution kinetics, organometallic chemistry for /sigma/- and /pi/-bonded compounds, and some concluding remarks on the superheavy elements.

  19. Actinide phosphonate complexes in aqueous solutions

    SciTech Connect

    Nash, K.L.

    1993-10-01

    Complexes formed by actinides with carboxylic acids, polycarboxylic acids, and aminopolycarboxylic acids play a central role in both the basic and process chemistry of the actinides. Recent studies of f-element complexes with phosphonic acid ligands indicate that new ligands incorporating doubly ionizable phosphonate groups (-PO{sub 3}H{sub 2}) have many properties which are unique chemically, and promise more efficient separation processes for waste cleanup and environmental restoration. Simple diphosphonate ligands form much stronger complexes than isostructural carboxylates, often exhibiting higher solubility as well. In this manuscript recent studies of the thermodynamics and kinetics of f-element complexation by 1,1 and 1,2 diphosphonic acid ligands are described.

  20. VUV and soft x-ray spectroscopy of actinides

    SciTech Connect

    Olson, C. G.; Joyce, J. J.; Durakiewicz, T.; Guziewicz, E.

    2004-01-01

    Optical and photoelectron spectroscopies using VUV and Soft X-ray photons are powerful tools for studies of elemental and compound actinides. Large changes in the relative atomic cross sections of the 5f, 6d and sp electrons allow decomposition of the character of the valence bands using photoemission. Resonant enhancement of photoelectrons and Auger electrons at the 5d core threshold further aids the decomposition and gives a measure of elemental specificity. Angle-resolved photoemission can be used to map the momentum dependence of the electronic states. The large changes in relative cross section with photon energy yields further details when the mapping is done at equivalent points in multiple zones. Spectra for well understood rare earth materials will be presented to establish spectral characteristics for known atomic character initial states. These signatures will be applied to the case of USb to investigate f-d hybridization near the Fermi level.

  1. Surrogate Reactions in the Actinide Region

    SciTech Connect

    Burke, J T; Bernstein, L A; Scielzo, N D; Bleuel, D L; Lesher, S R; Escher, J; Ahle, L; Dietrich, F S; Hoffman, R D; Norman, E B; Sheets, S A; Phair, L; Fallon, P; Clark, R M; Gibelin, J; Jewett, C; Lee, I Y; Macchiavelli, A O; McMahan, M A; Moretto, L G; Rodriguez-Vieitez, E; Wiedeking, M; Lyles, B F; Beausang, C W; Allmond, J M; Ai, H; Cizewski, J A; Hatarik, R; O'Malley, P D; Swan, T

    2008-01-30

    Over the past three years we have studied various surrogate reactions (d,p), ({sup 3}He,t), ({alpha},{alpha}{prime}) on several uranium isotopes {sup 234}U, {sup 235}U, {sup 236}U, and {sup 238}U. An overview of the STARS/LIBERACE surrogate research program as it pertains to the actinides is discussed. A summary of results to date will be presented along with a discussion of experimental difficulties encountered in surrogate experiments and future research directions.

  2. Separation of Californium from other Actinides

    DOEpatents

    Mailen, J C; Ferris, L M

    1973-09-25

    A method is provided for separating californium from a fused fluoride composition containing californium and at least one element selected from the group consisting of plutonium, americium, curium, uranium, thorium, and protactinium which comprises contacting said fluoride composition with a liquid bismuth phase containing sufficient lithium or thorium to effect transfer of said actinides to the bismuth phase and then contacting the liquid bismuth phase with molten LiCl to effect selective transfer of californium to the chloride phase.

  3. Process to remove rare earth from IFR electrolyte

    DOEpatents

    Ackerman, J.P.; Johnson, T.R.

    1992-01-01

    The invention is a process for the removal of rare earths from molten chloride electrolyte salts used in the reprocessing of integrated fast reactor fuel (IFR). The process can be used either continuously during normal operation of the electrorefiner or as a batch process. The process consists of first separating the actinide values from the salt before purification by removal of the rare earths. After replacement of the actinides removed in the first step, the now-purified salt electrolyte has the same uranium and plutonium concentration and ratio as when the salt was removed from the electrorefiner.

  4. Process to remove rare earth from IFR electrolyte

    DOEpatents

    Ackerman, J.P.; Johnson, T.R.

    1994-08-09

    The invention is a process for the removal of rare earths from molten chloride electrolyte salts used in the reprocessing of integrated fast reactor fuel (IFR). The process can be used either continuously during normal operation of the electrorefiner or as a batch process. The process consists of first separating the actinide values from the salt before purification by removal of the rare earths. After replacement of the actinides removed in the first step, the now-purified salt electrolyte has the same uranium and plutonium concentration and ratio as when the salt was removed from the electrorefiner. 1 fig.

  5. Effects of Blood Coagulate Removal Method on Aedes albopictus (Diptera: Culicidae) Life Table Characteristics and Vector Competence for Dengue Virus.

    PubMed

    van Dodewaard, Caitlin A M; Richards, Stephanie L; Harris, Jonathan W

    2016-01-01

    Commercially available blood can be used as an alternative to live animals to maintain mosquito colonies and deliver infectious bloodmeals during research studies. We analyzed the extent to which two methods for blood coagulate removal (defibrination or addition of sodium citrate) affected life table characteristics (i.e., fecundity, fertility, hatch rate, and adult survival) and vector competence (infection, dissemination, and transmission) of Aedes albopictus (Skuse) for dengue virus (DENV). Two types of bovine blood were tested at two extrinsic incubation temperatures (27 or 30°C) for DENV-infected and uninfected mosquitoes. Fully engorged mosquitoes were transferred to individual cages containing an oviposition cup and a substrate. Eggs (fecundity) and hatched larvae (fertility) were counted. At 14 and 21 d post feeding on a DENV-infected bloodmeal, 15 mosquitoes were sampled from each group, and vector competence was analyzed (bodies [infection], legs [dissemination], and saliva [transmission]). Differences in life table characteristics and vector competence were analyzed for mosquitoes fed blood processed using different methods for removal of coagulates. The method for removal of coagulates significantly impacted fecundity, fertility, and hatch time in the uninfected group, but not DENV-infected group. Infected mosquitoes showed significantly higher fecundity and faster hatch time than uninfected mosquitoes. We show no significant differences in infection or dissemination rates between groups; however, horizontal transmission rate was significantly higher in mosquitoes fed DENV-infected citrated compared with defibrinated blood. We expect the findings of this study to inform research using artificial blood delivery methods to assess vector competence.

  6. Actinide behavior in a freshwater pond

    SciTech Connect

    Trabalka, J.R.; Bogle, M.A.; Scott, T.G.

    1983-01-01

    Long-term investigations of solution chemistry in an alkaline freshwater pond have revealed that actinide oxidation state behavior, particularly that of plutonium, is complex. The Pu(V,VI) fraction was predominant in solution, but it varied over the entire range reported from other natural aquatic environments, in this case, as a result of intrinsic biological and chemical cycles (redox and pH-dependent phenomena). A strong positive correlation between plutonium (Pu), but not uranium (U), and hydroxyl ion over the observation period, especially when both were known to be in higher oxidation states, was particularly notable. Coupled with other examples of divergent U and Pu behavior, this result suggests that Pu(V), or perhaps a mixture of Pu(V,VI), was the prevalent oxidation state in solution. Observations of trivalent actinide sorption behavior during an algal bloom, coupled with the association with a high-molecular weight (nominally 6000 to 10,000 mol wt) organic fraction in solution, indicate that solution-detritus cycling of organic carbon, in turn, may be the primary mechanism in amercium-curium (Am-Cm) cycling. Sorption by sedimentary materials appears to predominate over other factors controlling effective actinide solubility and may explain, at least partially, the absence of an expected strong positive correlation between carbonate and dissolved U. 49 references, 6 figures, 12 tables.

  7. Actinide and lanthanide separation process (ALSEP)

    DOEpatents

    Guelis, Artem V.

    2013-01-15

    The process of the invention is the separation of minor actinides from lanthanides in a fluid mixture comprising, fission products, lanthanides, minor actinides, rare earth elements, nitric acid and water by addition of an organic chelating aid to the fluid; extracting the fluid with a solvent comprising a first extractant, a second extractant and an organic diluent to form an organic extractant stream and an aqueous raffinate. Scrubbing the organic stream with a dicarboxylic acid and a chelating agent to form a scrubber discharge. The scrubber discharge is stripped with a simple buffering agent and a second chelating agent in the pH range of 2.5 to 6.1 to produce actinide and lanthanide streams and spent organic diluents. The first extractant is selected from bis(2-ethylhexyl)hydrogen phosphate (HDEHP) and mono(2-ethylhexyl)2-ethylhexyl phosphonate (HEH(EHP)) and the second extractant is selected from N,N,N,N-tetra-2-ethylhexyl diglycol amide (TEHDGA) and N,N,N',N'-tetraoctyl-3-oxapentanediamide (TODGA).

  8. Development of the Actinide-Lanthanide Separation (ALSEP) Process

    SciTech Connect

    Lumetta, Gregg J.; Carter, Jennifer C.; Niver, Cynthia M.; Gelis, Artem V.

    2014-09-30

    Separating the minor actinide elements (Am and Cm) from acidic high-level raffinates arising from the reprocessing of irradiated nuclear fuel is an important step in closing the nuclear fuel cycle. Most proposed approaches to this problem involve two solvent extraction steps: 1) co-extraction of the trivalent lanthanides and actinides, followed by 2) separation of the actinides from the lanthanides. The objective of our work is to develop a single solvent-extraction process for isolating the minor actinide elements. We report here a solvent containing N,N,N',N'-tetra(2 ethylhexyl)diglycolamide (T2EHDGA) combined with 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) that can be used to separate the minor actinides in a single solvent-extraction process. T2EHDGA serves to co-extract the trivalent actinide and lanthanide ions from nitric acid solution. Switching the aqueous phase chemistry to a citrate buffered solution of N-(2-hydroxyethyl)ethylenediamine-N,N',N'-triacetic acid at pH 2.5 to 4 results in selective transfer of the actinides to the aqueous phase, thus affecting separation of the actinides from the lanthanides. Separation factors between the lanthanides and actinides are approximately 20 in the pH range of 3 to 4, and the distribution ratios are not highly dependent on the pH in this system.

  9. DEVELOPMENT OF PROTOTYPE TITANATE ION EXCHANGE LOADED MEMBRANES FOR STRONTIUM, CESIUM AND ACTINIDE DECONTAMINATION FROM AQUEOUS MEDIA

    SciTech Connect

    Oji, L; Keisha Martin, K; David Hobbs, D

    2008-05-30

    We have successfully incorporated high surface area particles of titanate ion exchange materials (monosodium titanate and crystalline silicotitanate) with acceptable particle size distribution into porous and inert support membrane fibrils consisting of polytetrafluoroethylene (Teflon{reg_sign}), polyethylene and cellulose materials. The resulting membrane sheets, under laboratory conditions, were used to evaluate the removal of surrogate radioactive materials for cesium-137 and strontium-90 from high caustic nuclear waste simulants. These membrane supports met the nominal requirement for nonchemical interaction with the embedded ion exchange materials and were porous enough to allow sufficient liquid flow. Some of this 47-mm size stamped out prototype titanium impregnated ion exchange membrane discs was found to remove more than 96% of dissolved cesium-133 and strontium-88 from a caustic nuclear waste salt simulants. Since in traditional ion exchange based column technology monosodium titanate (MST) is known to have great affinity for the sorbing of other actinides like plutonium, neptunium and even uranium, we expect that the MST-based membranes developed here, although not directly evaluated for uptake of these three actinides because of costs associated with working with actinides which do not have 'true' experimental surrogates, would also show significant affinity for these actinides in aqueous media. It was also observed that crystalline silicotitanate impregnated polytetrafluoroethylene or polyethylene membranes became less selective and sorbed both cesium and strontium from the caustic aqueous salt simulants.

  10. Synthesis of some ferromagnetic composite resins and their metal removal characteristics in aqueous solutions.

    PubMed

    Sheha, R R; El-Zahhar, A A

    2008-02-11

    In this study, a procedure for synthesis of new organic-inorganic magnetic composite resins was established. The procedure was based upon immobilization of magnetite (Mag) as a ferromagnetic material within the polymer poly(acrylic acid acrylonitrile) P(AA-AN) and the ion exchange resin (Amberlite IR 120). The produced magnetic resins, IR 120-PAN-Mag (R1) and P(AA-AN)-Mag (R2) were assessed as sorbents for Cr(VI). Various factors influencing the sorption of Cr(VI), e.g., pH, equilibrium time, initial concentration and temperature were studied. The sorption process was very fast initially and maximum sorption was achieved within 3h and pH 5.1. The kinetic of the system has been evaluated with pseudo first order model, second order model, Elovich model, intra-particle diffusion model and liquid film diffusion model. Chromium interaction with composite particles followed second-order kinetics with a correlation coefficient extremely high and closer to unity and rate constant (k(s)) has the values 1.68 x 10(-4) and 1.9 x 10(-4)g(mg(-1)min(-1)) for R1 and R2, respectively. The values of equilibrium sorption capacity (q(e)) are consistent with the modeled data and attain the range 893-951 mg g(-1). Kinetically, both pore diffusion and film diffusion are participating in ruling the diffusion of Cr(VI) ions. The sorption data gave good fits with Temkin and Flory-Huggins isotherm models. The isotherm parameters related to the heat of sorption are in the range 8-16 kJ mol(-1) which is the range of bonding energy for ion exchange interactions and so suggest an ion exchange mechanism for removal of Cr(VI) by the composite sorbents. The adsorption process was exothermic with DeltaH in the range of -73 to -97 kJ mol(-1). The negative values of Gibbs free energy confirm the feasibility and the spontaneous nature of Cr(VI) removal with these novel composites.

  11. Occurrence and removal characteristics of phthalate esters from typical water sources in northeast china.

    PubMed

    Liu, Yu; Chen, Zhonglin; Shen, Jimin

    2013-01-01

    The presence of phthalate esters (PAEs) in the environment has gained a considerable attention due to their potential impacts on public health. This study reports the first data on the occurrence of 15 PAEs in the water near the Mopanshan Reservoir-the new and important water source of Harbin city in Northeast China. As drinking water is a major source for human exposure to PAEs, the fate of target PAEs in the two waterworks (Mopanshan Waterworks and Seven Waterworks) was also analyzed. The results demonstrated that the total concentrations of 15 PAEs in the water near the Mopanshan Reservoir were relatively moderate, ranging from 355.8 to 9226.5 ng/L, with the mean value of 2943.1 ng/L. DBP and DEHP dominated the PAE concentrations, which ranged from 52.5 to 4498.2 ng/L and 128.9 to 6570.9 ng/L, respectively. The occurrence and concentrations of these compounds were heavily spatially dependent. Meanwhile, the results on the waterworks samples suggested no significant differences in PAE levels with the input of the raw waters. Without effective and stable removal of PAEs after the conventional drinking water treatment in the waterworks (25.8% to 76.5%), the risks posed by PAEs through drinking water ingestion were still existing, which should be paid special attention to the source control in the Mopanshan Reservoir and some advanced treatment processes for drinking water supplies.

  12. Effects of initial air removal methods on microorganisms and characteristics of fermented plant beverages.

    PubMed

    Kantachote, Duangporn; Charernjiratrakul, Wilawan

    2008-01-15

    The effects of 3 different methods for removing the initial air on the properties of fermented plant beverages produced from phom-nang seaweed (Gracilaria fisheri) and wild forest noni (Morinda coreia Ham.) were investigated. Only method M which covered the space above the fermentation liquid with a water filled plastic bag produced no surface film of yeast, had the highest acidity and also antibacterial activity from both plants after 90 days of fermentation. However, the yeast count still exceeded the standard guidelines for plant beverages. The fermented beverage from wild forest noni showed more antibacterial activity against 3 of 4 pathogenic bacteria tested than that from the phomnang seaweed, probably for its higher levels of acidity and ethanol content. Lactic Acid Bacteria (LAB) isolated from the fermentation samples from days 1-5 using the method M from both fermented plant beverages were Leuconostoc mesenteroides supsp. mesenteroides and Leu. mesenteroides subsp. dextranicum while presence of Lactobacilus plantarum was only recorded at days 4-5 in the wild forest noni beverage. From days 6-14 the isolates were Lactobacillus plantarum, Lactobacillus fermentum and Lactobacillus brevis from wild forest noni beverage, whereas only L. brevis was not detected in the seaweed beverage. During days 21-45 both beverages had a similar LAB population of L. plantarum and L. brevis while L. coryniformis was only found in the wild forest noni beverage. Between days 60-90 in both plant beverages only L. plantarum and Lactobacillius sp. were detected.

  13. Adsorption characteristics and behaviors of graphene oxide for Zn(II) removal from aqueous solution

    NASA Astrophysics Data System (ADS)

    Wang, Hou; Yuan, Xingzhong; Wu, Yan; Huang, Huajun; Zeng, Guangming; Liu, Yan; Wang, Xueli; Lin, Ningbo; Qi, Yu

    2013-08-01

    In this study, graphene oxide (GO) was synthesized via modified Hummers’ method, and characterized by scanning electron microscopy (SEM), atomic force microscope (AFM), X-ray diffraction (XRD), and Fourier transform infrared spectrum (FT-IR), X-ray photoelectron spectroscopy (XPS). The adsorption of Zn(II) on GO as a function of pH, adsorbent dosage, foreign ions, contact time, and temperature was investigated using batch technique. Results showed that the suitable pH for Zn(II) removal was about 7.0, and the optimal dosage was 2 mg. The adsorption of Zn(II) onto GO increased sharply within 20 min and obtained equilibrium gradually. Meanwhile, foreign ion and temperature also affected the adsorption performance of GO. The adsorption process was found to be well described by the pseudo-second-order rate model. Equilibrium studies indicated that the data of Zn(II) adsorption followed the Langmuir model. The maximum adsorption capacity for Zn(II) was up to 246 mg/g with a Langmuir adsorption equilibrium constant of 5.7 L/g at 20 °C. The thermodynamic parameters calculated from temperature-dependent sorption isotherms suggested that Zn(II) sorption on GO was an exothermic and spontaneous process in nature. The possibility of Zn(II) recovery was investigated and the result revealed that the maximum Zn(II) recovery yield was achieved with hydrochloric acid.

  14. Characteristics and fate of organic nitrogen in municipal biological nutrient removal wastewater treatment plants.

    PubMed

    Czerwionka, K; Makinia, J; Pagilla, K R; Stensel, H D

    2012-05-01

    The aim of this study was to investigate the occurrence and fate of colloidal and dissolved organic nitrogen (CON and DON) across biological nutrient removal (BNR) activated sludge bioreactors. Primary and secondary effluent total nitrogen (TN) measurements and component fractionation, CON and DON concentration profiles across BNR bioreactors, and laboratory batch experiments with the process mixed liquor were carried out at several full-scale BNR plants in northern Poland. The organic nitrogen (ON) components were divided into high CON, low CON, and DON based on sequential filtration through 1.2, 0.45 and 0.1 μm pore-size filters. The average influent DON(0.1 μm) (<0.1 μm) concentrations ranged from 1.1 g N/m(3) to 3.9 g N/m(3) and accounted for only 4-13% of total organic nitrogen. In the effluents, however, this contribution increased to 12-45% (the DON(0.1 μm) concentrations varied in a narrow range of 0.5-1.3 g N/m(3)). Conversions of ON inside the bioreactors were investigated in more detail in two largest plants, i.e. Gdansk (565,000 PE) and Gdynia (516,000 PE). Inside the two studied bioreactors, the largest reductions of the colloidal fraction were found to occur in the anaerobic and anoxic compartments, whereas an increase of DON(0.1 μm) concentrations was observed under aerobic conditions in the last compartment. Batch experiments with the process mixed liquor confirmed that DON(0.1 μm) was explicitly produced in the aerobic phase and significant amounts of ON were converted in the anoxic phase of the experiments.

  15. Revealing the characteristics of a novel bioflocculant and its flocculation performance in Microcystis aeruginosa removal.

    PubMed

    Sun, Pengfei; Hui, Cai; Bai, Naling; Yang, Shengmao; Wan, Li; Zhang, Qichun; Zhao, YuHua

    2015-12-02

    In the present work, a novel bioflocculant, EPS-1, was prepared and used to flocculate the kaolin suspension and Microcystis aeruginosa. We focused on the characteristics and flocculation performance of EPS-1, especially with regard to its protein components. An important attribute of EPS-1 was its protein content, with 18 protein types identified that occupied a total content of 31.70% in the EPS-1. Moreover, the flocculating activity of these protein components was estimated to be no less than 33.93%. Additionally, polysaccharides that occupied 57.12% of the total EPS-1 content consisted of four monosaccharides: maltose, D-xylose, mannose, and D-fructose. In addition, carbonyl, amino, and hydroxyl groups were identified as the main functional groups. Three main elements, namely C1s, N1s, and O1s, were present in EPS-1 with relative atomic percentages of 62.63%, 24.91%, and 10.5%, respectively. Zeta potential analysis indicated that charge neutralization contributed to kaolin flocculation, but was not involved in M. aeruginosa flocculation. The flocculation conditions of EPS-1 were optimized, and the maximum flocculating efficiencies were 93.34% within 2 min for kaolin suspension and 87.98% within 10 min for M. aeruginosa. These results suggest that EPS-1 could be an alternative to chemical flocculants for treating wastewaters and cyanobacterium-polluted freshwater.

  16. Revealing the characteristics of a novel bioflocculant and its flocculation performance in Microcystis aeruginosa removal

    PubMed Central

    Sun, Pengfei; Hui, Cai; Bai, Naling; Yang, Shengmao; Wan, Li; Zhang, Qichun; Zhao, YuHua

    2015-01-01

    In the present work, a novel bioflocculant, EPS-1, was prepared and used to flocculate the kaolin suspension and Microcystis aeruginosa. We focused on the characteristics and flocculation performance of EPS-1, especially with regard to its protein components. An important attribute of EPS-1 was its protein content, with 18 protein types identified that occupied a total content of 31.70% in the EPS-1. Moreover, the flocculating activity of these protein components was estimated to be no less than 33.93%. Additionally, polysaccharides that occupied 57.12% of the total EPS-1 content consisted of four monosaccharides: maltose, D-xylose, mannose, and D-fructose. In addition, carbonyl, amino, and hydroxyl groups were identified as the main functional groups. Three main elements, namely C1s, N1s, and O1s, were present in EPS-1 with relative atomic percentages of 62.63%, 24.91%, and 10.5%, respectively. Zeta potential analysis indicated that charge neutralization contributed to kaolin flocculation, but was not involved in M. aeruginosa flocculation. The flocculation conditions of EPS-1 were optimized, and the maximum flocculating efficiencies were 93.34% within 2 min for kaolin suspension and 87.98% within 10 min for M. aeruginosa. These results suggest that EPS-1 could be an alternative to chemical flocculants for treating wastewaters and cyanobacterium-polluted freshwater. PMID:26626432

  17. Revealing the characteristics of a novel bioflocculant and its flocculation performance in Microcystis aeruginosa removal

    NASA Astrophysics Data System (ADS)

    Sun, Pengfei; Hui, Cai; Bai, Naling; Yang, Shengmao; Wan, Li; Zhang, Qichun; Zhao, Yuhua

    2015-12-01

    In the present work, a novel bioflocculant, EPS-1, was prepared and used to flocculate the kaolin suspension and Microcystis aeruginosa. We focused on the characteristics and flocculation performance of EPS-1, especially with regard to its protein components. An important attribute of EPS-1 was its protein content, with 18 protein types identified that occupied a total content of 31.70% in the EPS-1. Moreover, the flocculating activity of these protein components was estimated to be no less than 33.93%. Additionally, polysaccharides that occupied 57.12% of the total EPS-1 content consisted of four monosaccharides: maltose, D-xylose, mannose, and D-fructose. In addition, carbonyl, amino, and hydroxyl groups were identified as the main functional groups. Three main elements, namely C1s, N1s, and O1s, were present in EPS-1 with relative atomic percentages of 62.63%, 24.91%, and 10.5%, respectively. Zeta potential analysis indicated that charge neutralization contributed to kaolin flocculation, but was not involved in M. aeruginosa flocculation. The flocculation conditions of EPS-1 were optimized, and the maximum flocculating efficiencies were 93.34% within 2 min for kaolin suspension and 87.98% within 10 min for M. aeruginosa. These results suggest that EPS-1 could be an alternative to chemical flocculants for treating wastewaters and cyanobacterium-polluted freshwater.

  18. Removal characteristics of CO2 using aqueous MEA/AMP solutions in the absorption and regeneration process.

    PubMed

    Choi, Won-Joon; Seo, Jong-Beom; Jang, Sang-Yong; Jung, Jong-Hyeon; Oh, Kwang-Joong

    2009-01-01

    The carbon dioxide (CO2) removal efficiency, reaction rate, and CO2 loading into aqueous blended monoethanolamine (MEA) + 2-amino-2-methyl-1-propanol (AMP) solutions to enhance absorption characteristics of MEA and AMP were carried out by the absorption/regeneration process. As a result, compared to aqueous MEA and AMP solutions, aqueous blended MEA + AMP solutions have a higher CO2 loading than MEA and a higher reaction rate than AMP. The CO2 loading of rich amine of aqueous 18 wt.% MEA + 12 wt.% AMP solution was 0.62 mol CO2/mol amine, which is 51.2% more than 30 wt.% MEA (0.41 mol CO2/mol amine). Consequently, blending MEA and AMP could be an effective way to design considering economical efficiency and used to operate absorber for a long time.

  19. ENHANCING ADVANCED CANDU PROLIFERATION RESISTANCE FUEL WITH MINOR ACTINIDES

    SciTech Connect

    Gray S. Chang

    2010-05-01

    The advanced nuclear system will significantly advance the science and technology of nuclear energy systems and to enhance the spent fuel proliferation resistance. Minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. MAs can play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In this work, an Advanced CANDU Reactor (ACR) fuel unit lattice cell model with 43 UO2 fuel rods will be used to investigate the effectiveness of a Minor Actinide Reduction Approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance. The main MARA objective is to increase the 238Pu / Pu isotope ratio by using the transuranic nuclides (237Np and 241Am) in the high burnup fuel and thereby increase the proliferation resistance even for a very low fuel burnup. As a result, MARA is a very effective approach to enhance the proliferation resistance for the on power refueling ACR system nuclear fuel. The MA transmutation characteristics at different MA loadings were compared and their impact on neutronics criticality assessed. The concept of MARA, significantly increases the 238Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in atoms for peace and the intermediate term of nuclear energy reconnaissance.

  20. The influences of iron characteristics, operating conditions and solution chemistry on contaminants removal by zero-valent iron: A review.

    PubMed

    Sun, Yuankui; Li, Jinxiang; Huang, Tinglin; Guan, Xiaohong

    2016-09-01

    For successful application of a zero-valent iron (ZVI) system, of particular interest is the performance of ZVI under various conditions. The current review comprehensively summarizes the potential effects of the major influencing factors, such as iron intrinsic characteristics (e.g., surface area, iron impurities and oxide films), operating conditions (e.g., pH, dissolved oxygen, iron dosage, iron pretreatment, mixing conditions and temperature) and solution chemistry (e.g., anions, cations and natural organic matter) on the performance of ZVI reported in literature. It was demonstrated that all of the factors could exert significant effects on the ZVI performance toward contaminants removal, negatively or positively. Depending on the removal mechanisms of the respective contaminants and other environmental conditions, an individual variable may exhibit different effects. On the other hand, many of these influences have not been well understood or cannot be individually isolated in experimental or natural systems. Thus, more research is required in order to elucidate the exact roles and mechanisms of each factor in affecting the performance of ZVI. Furthermore, based on these understandings, future research may attempt to establish some feasible strategies to minimize the deteriorating effects and utilize the positive effects so as to improve the performance of ZVI.

  1. Study of actinide chemistry in saturated potassium fluoride solution

    NASA Technical Reports Server (NTRS)

    Cohen, D.; Thalmayer, C. E.

    1969-01-01

    Study concerning the chemistry of actinides in saturated KF solution included work with neptunium, uranium, and americium. Solubilities, absorption spectra, oxidation-reduction reactions, and solid compounds which can be produced in KF solution were examined. The information is used for preparation of various materials from salts of the actinides.

  2. Detailed calculations of minor actinide transmutation in a fast reactor

    SciTech Connect

    Takeda, Toshikazu

    2015-12-31

    The transmutation of minor actinides in a fast reactor is investigated by a new method to investigate the transmutation behavior of individual minor actinides. It is found that Np-237 and Am-241 mainly contributes to the transmutation rate though the transmutation behaviors are very different.

  3. POTENTIAL BENCHMARKS FOR ACTINIDE PRODUCTION IN HANFORD REACTORS

    SciTech Connect

    PUIGH RJ; TOFFER H

    2011-10-19

    A significant experimental program was conducted in the early Hanford reactors to understand the reactor production of actinides. These experiments were conducted with sufficient rigor, in some cases, to provide useful information that can be utilized today in development of benchmark experiments that may be used for the validation of present computer codes for the production of these actinides in low enriched uranium fuel.

  4. Improved method for extracting lanthanides and actinides from acid solutions

    DOEpatents

    Horwitz, E.P.; Kalina, D.G.; Kaplan, L.; Mason, G.W.

    1983-07-26

    A process for the recovery of actinide and lanthanide values from aqueous acidic solutions uses a new series of neutral bi-functional extractants, the alkyl(phenyl)-N,N-dialkylcarbamoylmethylphosphine oxides. The process is suitable for the separation of actinide and lanthanide values from fission product values found together in high-level nuclear reprocessing waste solutions.

  5. Process for making a ceramic composition for immobilization of actinides

    DOEpatents

    Ebbinghaus, Bartley B.; Van Konynenburg, Richard A.; Vance, Eric R.; Stewart, Martin W.; Walls, Philip A.; Brummond, William Allen; Armantrout, Guy A.; Herman, Connie Cicero; Hobson, Beverly F.; Herman, David Thomas; Curtis, Paul G.; Farmer, Joseph

    2001-01-01

    Disclosed is a process for making a ceramic composition for the immobilization of actinides, particularly uranium and plutonium. The ceramic is a titanate material comprising pyrochlore, brannerite and rutile. The process comprises oxidizing the actinides, milling the oxides to a powder, blending them with ceramic precursors, cold pressing the blend and sintering the pressed material.

  6. CHARACTERIZATION OF MODIFIED MONOSODIUM TITANATE - AN IMPROVED SORBENT FOR STRONTIUM AND ACTINIDE SEPARATIONS

    SciTech Connect

    Hobbs, D.; Taylor-Pashow, K.; Missimer, D.

    2010-12-21

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 134,137}Cs, {sup 90}Sr, and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. An inorganic sorbent, monosodium titanate (MST), is currently used to remove {sup 90}Sr and alpha-emitting radionuclides, while a caustic-side solvent extraction process is used for removing {sup 134,137}Cs. A new peroxotitanate material, modified MST, or mMST, has recently been developed and has shown increased removal kinetics and capacity for {sup 90}Sr and alpha-emitting radionuclides compared to the current baseline material, MST. This paper describes recent results focused on further characterization of this material.

  7. Actinide production in the reaction of heavy ions with curium-248

    SciTech Connect

    Moody, K.J.

    1983-01-01

    Chemical experiments were performed to examine the usefulness of heavy ion transfer reactions in producing new, neutron-rich actinide nuclides. A general quasi-elastic to deep-inelastic mechanism is proposed, and the utility of this method as opposed to other methods (e.g. complete fusion) is discussed. The relative merits of various techniques of actinide target synthesis are discussed. A description is given of a target system designed to remove the large amounts of heat generated by the passage of a heavy ion beam through matter, thereby maximizing the beam intensity which can be safely used in an experiment. Also described is a general separation scheme for the actinide elements from protactinium (Z = 91) to mendelevium (Z = 101), and fast specific procedures for plutonium, americium and berkelium. The cross sections for the production of several nuclides from the bombardment of /sup 248/Cm with /sup 18/Kr and /sup 86/O, /sup 136/Xe projectiles at several energies near and below the Coulomb barrier were determined. The results are compared with yields from /sup 48/Ca and /sup 238/U bombardments of /sup 248/Cm. A preliminary, unsuccessful attempt to isolate /sup 247/Pu is outlined. The absolute ..gamma.. ray intensities from /sup 251/Bk decay, necessary for calculating the /sup 251/Bk cross section, are also determined.

  8. Research in actinide chemistry. Progress report, 1990--1993

    SciTech Connect

    Choppin, G.R.

    1993-04-01

    This research studies the behavior of the actinide elements in aqueous solution. The high radioactivity of the transuranium actinides limits the concentrations which can be studied and, consequently, limits the experimental techniques. However, oxidation state analogs (trivalent lanthanides, tetravalent thorium, and hexavalent uranium) do not suffer from these limitations. Behavior of actinides in the environment are a major USDOE concern, whether in connection with long-term releases from a repository, releases from stored defense wastes or accidental releases in reprocessing, etc. Principal goal of our research was expand the thermodynamic data base on complexation of actinides by natural ligands (e.g., OH{sup {minus}}, CO{sub 3}{sup 2{minus}}, PO{sub 4}{sup 3{minus}}, humates). The research undertakes fundamental studies of actinide complexes which can increase understanding of the environmental behavior of these elements.

  9. Actinides and Rare Earths Topical Conference (Code AC)

    SciTech Connect

    Tobin, J G

    2009-11-24

    Actinide and the Rare Earth materials exhibit many unique and diverse physical, chemical and magnetic properties, in large part because of the complexity of their f electronic structure. This Topical Conference will focus upon the chemistry, physics and materials science in Lanthanide and Actinide materials, driven by 4f and 5f electronic structure. Particular emphasis will be placed upon 4f/5f magnetic structure, surface science and thin film properties. For the actinides, fundamental actinide science and its role in resolving technical challenges posed by actinide materials will be stressed. Both basic and applied experimental approaches, including synchrotron-radiation-based investigations, as well as theoretical modeling and computational simulations, are planned to be part of the Topical Conference. Of particular importance are the issues related to the potential renaissance in Nuclear Fuels, including synthesis, oxidation, corrosion, intermixing, stability in extreme environments, prediction of properties via benchmarked simulations, separation science, environmental impact and disposal of waste products.

  10. Oxyhydroxy Silicate Colloids: A New Type of Waterborne Actinide(IV) Colloids

    PubMed Central

    Weiss, Stephan; Hennig, Christoph; Brendler, Vinzenz; Ikeda‐Ohno, Atsushi

    2016-01-01

    Abstract At the near‐neutral and reducing aquatic conditions expected in undisturbed ore deposits or in closed nuclear waste repositories, the actinides Th, U, Np, and Pu are primarily tetravalent. These tetravalent actinides (AnIV) are sparingly soluble in aquatic systems and, hence, are often assumed to be immobile. However, AnIV could become mobile if they occur as colloids. This review focuses on a new type of AnIV colloids, oxyhydroxy silicate colloids. We herein discuss the chemical characteristics of these colloids and the potential implication for their environmental behavior. The binary oxyhydroxy silicate colloids of AnIV could be potentially more mobile as a waterborne species than the well‐known mono‐component oxyhydroxide colloids. PMID:27957406

  11. Design of an Actinide Burning, Lead-Bismuth Cooled Reactor That Produces Low Cost Electricity

    SciTech Connect

    C. Davis; S. Herring; P. MacDonald; K. McCarthy; V. Shah; K. Weaver; J. Buongiorno; R. Ballinger; K. Doyoung; M. Driscoll; P. Hejzler; M. Kazimi; N. Todreas

    1999-07-01

    The purpose of this project is to investigate the suitability of lead-bismuth cooled fast reactors for producing low-cost electricity as well as for actinide burning. The goal is to identify and analyze the key technical issues in core neutronics, materials, thermal-hydraulics, fuels, and economics associated with the development of this reactor concept. The choice of lead-bismuth for the reactor coolant is an actinide burning fast reactor offers enhanced safety and reliability. The advantages of lead-bismuth over sodium as a coolant are related to the following material characteristics: chemical inertness with air and water; higher atomic number; lower vapor pressure at operating temperatures; and higher boiling temperature. Given the status of the field, it was agreed that the focus of this investigation in the first two years will be on the assessment of approaches to optimize core and plant arrangements in order to provide maximum safety and economic potential in this type of reactor.

  12. Actinide management with commercial fast reactors

    SciTech Connect

    Ohki, Shigeo

    2015-12-31

    The capability of plutonium-breeding and minor-actinide (MA) transmutation in the Japanese commercial sodium-cooled fast reactor offers one of practical solutions for obtaining sustainable energy resources as well as reducing radioactive toxicity and inventory. The reference core design meets the requirement of flexible breeding ratio from 1.03 to 1.2. The MA transmutation amount has been evaluated as 50-100 kg/GW{sub e}y if the MA content in fresh fuel is 3-5 wt%, where about 30-40% of initial MA can be transmuted in the discharged fuel.

  13. Vapor pressure and thermodynamics of actinide metals

    SciTech Connect

    Ward, J.W.; Kleinschmidt, P.D.; Haire, R.G.; Brown, D.

    1980-01-01

    Precise vapor pressure measurements by target collection/mass spectrometric Knudsen effusion techniques were combined with crystal entropy estimates to produce self-consistent free-enrgy functions, permitting calculation of heats, entropies and free energies from 298/sup 0/K to the highest temperatures of measurement. The vapor pressures and thermodyamics of vaporization of americium, curium, berkelium, and californium are compared in terms of electronic structure and bonding trends in the trans-plutonium elements. These resuslts are contrasted with the behavior of the early actinides, with attention to energy states and possible effects of f-electron bonding. 9 figures, 4 tables.

  14. Status of nuclear data for actinides

    SciTech Connect

    Guzhovskii, B.Y.; Gorelov, V.P.; Grebennikov, A.N.

    1995-10-01

    Nuclear data required for transmutation problem include many actinide nuclei. In present paper the analysis of neutron fission, capture, (n,2n) and (n,3n) reaction cross sections at energy region from thermal point to 14 MeV was carried out for Th, Pa, U, Np, Pu, Am and Cm isotops using modern evaluated nuclear data libraries and handbooks of recommended nuclear data. Comparison of these data indicates on substantial discrepancies in different versions of files, that connect with quality and completeness of original experimental data.

  15. Actinide management with commercial fast reactors

    NASA Astrophysics Data System (ADS)

    Ohki, Shigeo

    2015-12-01

    The capability of plutonium-breeding and minor-actinide (MA) transmutation in the Japanese commercial sodium-cooled fast reactor offers one of practical solutions for obtaining sustainable energy resources as well as reducing radioactive toxicity and inventory. The reference core design meets the requirement of flexible breeding ratio from 1.03 to 1.2. The MA transmutation amount has been evaluated as 50-100 kg/GWey if the MA content in fresh fuel is 3-5 wt%, where about 30-40% of initial MA can be transmuted in the discharged fuel.

  16. Multicoordinate ligands for actinide/lanthanide separations.

    PubMed

    Dam, Henk H; Reinhoudt, David N; Verboom, Willem

    2007-02-01

    In nuclear waste treatment processes there is a need for improved ligands for the separation of actinides (An(III)) and lanthanides (Ln(III)). Several research groups are involved in the design and synthesis of new An(III) ligands and in the confinement of these and existing An(III) ligands onto molecular platforms giving multicoordinate ligands. The preorganization of ligands considerably improves the An(III) extraction properties, which are largely dependent on the solubility and rigidity of the platform. This tutorial review summarizes the most important An(III) ligands with emphasis on the preorganization strategy using (macrocyclic) platforms.

  17. Measurement and calculation of high-actinide burnup in the prototype fast reactor

    SciTech Connect

    Broadhead, B.L.; Raman, S.; Dickens, J.K. )

    1991-01-01

    An agreement was signed in May 1979 as a part of a long-term cooperative program between the United Kingdom and the US under the liquid-metal fast breeder reactor agreement of 1976. This agreement included an experiment to carry out irradiations of physics specimens of fissile and fertile actinides to improve our knowledge of basic nuclear physics phenomena. Three fuel pins were prepared by the US to contain the actinide physics samples; two of these pins were irradiated at the Dounreay prototype fast reactor (PFR) for a total irradiation of 63 full-power days. The third pin has only recently been removed from the PFT, following an irradiation of > 500 full-power days. Each pin houses 35 capsules containing milligram quantities of actinide oxides of {sup 231}Pa, {sup 230}Th, {sup 232}Th, {sup 233}U, {sup 234}U, {sup 235}U, {sup 236}U, {sup 238}U, {sup 237}Np, {sup 238}Pu, {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, {sup 242}Pu, {sup 244}Pu, {sup 241}Am, {sup 243}Am, {sup 243}Cm, {sup 244}Cm, {sup 246}Cm, and {sup 248}Cm. Following the return of the first fuel pin (FP-1) to the United States in May 1984, the actinide samples were prepared for studies of fission product yields, isotopics, and material concentrations. The measurements were repeated for the second fuel pin (FP-2) to remedy several problems encountered in the processing of the FP-1 pin. A brief description of the measured and calculated {sup 137}Cs yields for both FP-1 and FP-2 are included in this paper.

  18. Effects of salinity build-up on biomass characteristics and trace organic chemical removal: implications on the development of high retention membrane bioreactors.

    PubMed

    Luo, Wenhai; Hai, Faisal I; Kang, Jinguo; Price, William E; Guo, Wenshan; Ngo, Hao H; Yamamoto, Kazuo; Nghiem, Long D

    2015-02-01

    This study investigated the impact of salinity build-up on the performance of membrane bioreactor (MBR), specifically in terms of the removal and fate of trace organic chemicals (TrOCs), nutrient removal, and biomass characteristics. Stepwise increase of the influent salinity, simulating salinity build-up in high retention MBRs, adversely affected the metabolic activity in the bioreactor, thereby reducing organic and nutrient removal. The removal of hydrophilic TrOCs by MBR decreased due to salinity build-up. By contrast, with the exception of 17α-ethynylestradiol, the removal of all hydrophobic TrOCs was not affected at high salinity. Moreover, salinity build-up had negligible impact on the residual accumulation of TrOCs in the sludge phase except for a few hydrophilic compounds. Additionally, the response of the biomass to salinity stress also dramatically enhanced the release of both soluble microbial products (SMP) and extracellular polymeric substances (EPS), leading to severe membrane fouling.

  19. Actinide electronic structure and atomic forces

    NASA Astrophysics Data System (ADS)

    Albers, R. C.; Rudin, Sven P.; Trinkle, Dallas R.; Jones, M. D.

    2000-07-01

    We have developed a new method[1] of fitting tight-binding parameterizations based on functional forms developed at the Naval Research Laboratory.[2] We have applied these methods to actinide metals and report our success using them (see below). The fitting procedure uses first-principles local-density-approximation (LDA) linear augmented plane-wave (LAPW) band structure techniques[3] to first calculate an electronic-structure band structure and total energy for fcc, bcc, and simple cubic crystal structures for the actinide of interest. The tight-binding parameterization is then chosen to fit the detailed energy eigenvalues of the bands along symmetry directions, and the symmetry of the parameterization is constrained to agree with the correct symmetry of the LDA band structure at each eigenvalue and k-vector that is fit to. By fitting to a range of different volumes and the three different crystal structures, we find that the resulting parameterization is robust and appears to accurately calculate other crystal structures and properties of interest.

  20. Supercritical Carbon Dioxide Ligands for Extracting Actinide Metal Ions from Porous Solids

    SciTech Connect

    Albert W. Herlinger; Dr. Mark L. Dietz

    2003-03-06

    Numerous types of actinide-bearing waste materials are found throughout the DOE complex. Most of these wastes consist of large volumes of non-hazardous materials contaminated with relatively small quantities of actinide elements. Separation of these wastes into their inert and radioactive components would dramatically reduce the costs of stabilization and disposal. For example, the DOE is responsible for decontaminating concrete within 7000 surplus contaminated buildings. The best technology now available for removing surface contamination from concrete involves removing the surface layer by grit blasting, which produces a large volume of blasting residue containing a small amount of radioactive material. Disposal of this residue is expensive because of its large volume and fine particulate nature. Considerable cost savings would result from separation of the radioactive constituents and stabilization of the concrete dust. Similarly, gas diffusion plants for uranium enrichment contain valuable high-purity nickel in the form of diffusion barriers. Decontamination is complicated by the extremely fine pores in these barriers, which are not readily accessible by most cleaning techniques. A cost-effective method for the removal of radioactive contaminants would release this valuable material for salvage.

  1. Spectroscopic investigation of actinide speciation in concentrated chloride solution

    SciTech Connect

    Runde, W.; Neu, M.P.; Conradson, S.D.; Clark, D.L.; Palmer, P.D.; Reilly, S.D.; Scott, B.L.; Tait, C.D.

    1997-12-31

    The proposed disposal of nuclear waste in geological salt formations, e.g., the Waste Isolation Pilot Plant (USA) and the Gorleben site (Germany), raises a fundamental question: To what degree actinides will be solubilized and mobilized upon interaction with chloride ions? Actinide solubilities in highly concentrated chloride solutions are about one order of magnitude higher than in similar inert electrolyte (NaClO{sub 4}) solutions. This increased solubility is due to interactions between actinide and chloride ions. Contradictory results exist regarding the interaction mechanism between actinide and chloride ions. Specifically, both inner-sphere complex formation and ion pair association have been implicated in the interpretation of spectrophotometric and extraction data. To address this controversy, the authors investigated the interaction between actinide ions in the (III), (IV), (V) and (VI) oxidation states and chloride ions using a multi-method approach. Spectroscopic techniques (TRLFS, Raman, UV-Vis absorption, EXAFS) were used to distinguish between changes in the inner coordination sphere of the actinide ion and effects of ion pairing, X-ray absorption spectroscopy and single crystal X-ray diffraction were used to determine structural details of the actinide chloro complexes formed in solution and solid states.

  2. Thin extractive membrane for monitoring actinides in aqueous streams.

    PubMed

    Chavan, Vivek; Paul, Sumana; Pandey, Ashok K; Kalsi, P C; Goswami, A

    2013-09-15

    Alpha spectrometry and solid state nuclear track detectors (SSNTDs) are used for monitoring ultra-trace amount of alpha emitting actinides in different aqueous streams. However, these techniques have limitations i.e. alpha spectrometry requires a preconcentration step and SSNTDs are not chemically selective. Therefore, a thin polymer inclusion membrane (PIM) supported on silanized glass was developed for preconcentraion and determination of ultra-trace concentration of actinides by α-spectrometry and SSNTDs. PIMs were formed by spin coating on hydrophobic glass slide or solvent casting to form thin and self-supported membranes, respectively. Sorption experiments indicated that uptakes of actinides in the PIM were highly dependent on acidity of solution i.e. Am(III) sorbed up to 0.1 molL(-1) HNO₃, U(VI) up to 0.5 molL(-1) HNO₃ and Pu(IV) from HNO₃ concentration as high as 4 molL(-1). A scheme was developed for selective sorption of target actinide in the PIM by adjusting acidity and oxidation state of actinide. The actinides sorbed in PIMs were quantified by alpha spectrometry and SSNTDs. For SSNTDs, neutron induced fission-fragment tracks and α-particle tracks were registered in Garware polyester and CR-39 for quantifications of natural uranium and α-emitting actinides ((241)Am/(239)Pu/(233)U), respectively. Finally, the membranes were tested to quantify Pu in 4 molL(-1) HNO3 solutions and synthetic urine samples.

  3. Gas core reactors for actinide transmutation. [uranium hexafluoride

    NASA Technical Reports Server (NTRS)

    Clement, J. D.; Rust, J. H.; Wan, P. T.; Chow, S.

    1979-01-01

    The preliminary design of a uranium hexafluoride actinide transmutation reactor to convert long-lived actinide wastes to shorter-lived fission product wastes was analyzed. It is shown that externally moderated gas core reactors are ideal radiators. They provide an abundant supply of thermal neutrons and are insensitive to composition changes in the blanket. For the present reactor, an initial load of 6 metric tons of actinides is loaded. This is equivalent to the quantity produced by 300 LWR-years of operation. At the beginning, the core produces 2000 MWt while the blanket generates only 239 MWt. After four years of irradiation, the actinide mass is reduced to 3.9 metric tonnes. During this time, the blanket is becoming more fissile and its power rapidly approaches 1600 MWt. At the end of four years, continuous refueling of actinides is carried out and the actinide mass is held constant. Equilibrium is essentially achieved at the end of eight years. At equilibrium, the core is producing 1400 MWt and the blanket 1600 MWt. At this power level, the actinide destruction rate is equal to the production rate from 32 LWRs.

  4. Coastal and lower Elwha River, Washington, prior to dam removal--history, status, and defining characteristics: Chapter 1 in Coastal habitats of the Elwha River, Washington--biological and physical patterns and processes prior to dam removal

    USGS Publications Warehouse

    Duda, Jeffrey J.; Warrick, Jonathan A.; Magirl, Christopher S.; Duda, Jeffrey J.; Warrick, Jonathan A.; Magirl, Christopher S.

    2011-01-01

    Characterizing the physical and biological characteristics of the lower Elwha River, its estuary, and adjacent nearshore habitats prior to dam removal is essential to monitor changes to these areas during and following the historic dam-removal project set to begin in September 2011. Based on the size of the two hydroelectric projects and the amount of sediment that will be released, the Elwha River in Washington State will be home to the largest river restoration through dam removal attempted in the United States. Built in 1912 and 1927, respectively, the Elwha and Glines Canyon Dams have altered key physical and biological characteristics of the Elwha River. Once abundant salmon populations, consisting of all five species of Pacific salmon, are restricted to the lower 7.8 river kilometers downstream of Elwha Dam and are currently in low numbers. Dam removal will reopen access to more than 140 km of mainstem, flood plain, and tributary habitat, most of which is protected within Olympic National Park. The high capture rate of river-borne sediments by the two reservoirs has changed the geomorphology of the riverbed downstream of the dams. Mobilization and downstream transport of these accumulated reservoir sediments during and following dam removal will significantly change downstream river reaches, the estuary complex, and the nearshore environment. To introduce the more detailed studies that follow in this report, we summarize many of the key aspects of the Elwha River ecosystem including a regional and historical context for this unprecedented project.

  5. Actinide-specific complexing agents: their structural and solution chemistry

    SciTech Connect

    Raymond, K.N.; Freeman, G.E.; Kappel, M.J.

    1983-07-01

    The synthesis of a series of tetracatecholate ligands designed to be specific for Pu(IV) and other actinide(IV) ions has been achieved. Although these compounds are very effective as in vivo plutonium removal agents, potentiometric and voltammetric data indicate that at neutral pH full complexation of the Pu(IV) ion by all four catecholate groups does not occur. Spectroscopic results indicate that the tetracatecholates, 3,4,3-LICAMS and 3,4,3-LICAMC, complex Am(III). The Am(IV)/(III)-catecholate couple (where catecholate = 3,4,3-LICAMS or 3,4,3-LICAMC) is not observed, but may not be observable due to the large currents associated with ligand oxidation. However, within the potential range where ligand oxidation does not occur, these experiments indicate that the reduction potential of free Am(IV)/(III) is probably greater than or equal to + 2.6 V vs NHE or higher. Proof of the complexation of americium in the trivalent oxidation state by 3,4,3-LICAMS and 3,4,3-LICAMC elimates the possibility of tetracatholates stabilizing Am(IV) in vivo.

  6. Fundamental Thermodynamics of Actinide-Bearing Mineral Waste Forms - Final Report

    SciTech Connect

    Williamson, Mark A.; Ebbinghaus, Bartley B.; Navrotsky, Alexandra

    2001-03-01

    The end of the Cold War raised the need for the technical community to be concerned with the disposition of excess nuclear weapon material. The plutonium will either be converted into mixed-oxide fuel for use in nuclear reactors or immobilized in glass or ceramic waste forms and placed in a repository. The stability and behavior of plutonium in the ceramic materials as well as the phase behavior and stability of the ceramic material in the environment is not well established. In order to provide technically sound solutions to these issues, thermodynamic data are essential in developing an understanding of the chemistry and phase equilibria of the actinide-bearing mineral waste form materials proposed as immobilization matrices. Mineral materials of interest include zircon, zirconolite, and pyrochlore. High temperature solution calorimetry is one of the most powerful techniques, sometimes the only technique, for providing the fundamental thermodynamic data needed to establish optimum material fabrication parameters, and more importantly understand and predict the behavior of the mineral materials in the environment. The purpose of this project is to experimentally determine the enthalpy of formation of actinide orthosilicates, the enthalpies of formation of actinide substituted zirconolite and pyrochlore, and develop an understanding of the bonding characteristics and stabilities of these materials.

  7. Evaluation of radon adsorption characteristics of a coconut shell-based activated charcoal system for radon and thoron removal applications.

    PubMed

    Karunakara, N; Sudeep Kumara, K; Yashodhara, I; Sahoo, B K; Gaware, J J; Sapra, B K; Mayya, Y S

    2015-04-01

    Radon ((222)Rn), thoron ((220)Rn), and their decay products contribute a major fraction (more than 50%) of doses received from ionisation radiation in public domain indoor environments and occupation environments such as uranium mines, thorium plants, and underground facilities, and are recognised as important radiological hazardous materials, which need to be controlled. This paper presents studies on the removal of (222)Rn and (220)Rn from air using coconut shell-based granular activated charcoal cylindrical adsorber beds. Experiments were conducted to evaluate the (222)Rn and (220)Rn adsorption characteristics, and the mitigation efficiency of coconut-based activated charcoal available in India. The performance parameters evaluated include breakthrough time (τ) and adsorption coefficient (K), and degassing characteristics of the charcoal bed of varying dimensions at different flow rates. While the breakthrough for (222)Rn occurred depending on the dimension of the adsorber bed and flow rates, for (220)Rn, the breakthrough did not occur. The breakthrough curve exhibited a stretched S-shape response, instead of the theoretically predicted sharp step function. The experiments confirm that the breakthrough time individually satisfies the quadratic relationship with respect to the diameter of the bed, and the linear relationship with respect to the length, as predicted in the theory. The K value varied in the range of 2.3-4.12 m(3) kg(-1) with a mean value of 2.99 m(3) kg(-1). The K value was found to increase with the increase in flow rate. Heating the charcoal to ∼ 100 °C resulted in degassing of the adsorbed (222)Rn, and the K of the degassed charcoal and virgin charcoal were found to be similar with no deterioration in performance indicating the re-usability of the charcoal.

  8. Chemistry of tetravalent actinide phosphates-Part I

    SciTech Connect

    Brandel, V. . E-mail: vbrandel@neuf.fr; Dacheux, N. . E-mail: dacheux@ipno.in2p3.fr

    2004-12-01

    The chemistry and crystal structure of phosphates of tetravalent cations, including that of actinides was reviewed several times up to 1985. Later, new compounds were synthesized and characterized. In more recent studies, it was found that some of previously reported phases, especially those of thorium, uranium and neptunium, were wrongly identified. In the light of these new facts an update review and classification of the tetravalent actinide phosphates is proposed in the two parts of this paper. Their crystal structure and some chemical properties are also compared to non-actinide cation phosphates.

  9. Engineering-Scale Distillation of Cadmium for Actinide Recovery

    SciTech Connect

    J.C. Price; D. Vaden; R.W. Benedict

    2007-10-01

    During the recovery of actinide products from spent nuclear fuel, cadmium is separated from the actinide products by a distillation process. Distillation occurs in an induction-heated furnace called a cathode processor capable of processing kilogram quantities of cadmium. Operating parameters have been established for sufficient recovery of the cadmium based on mass balance and product purity. A cadmium distillation rate similar to previous investigators has also been determined. The development of cadmium distillation for spent fuel treatment enhances the capabilities for actinide recovery processes.

  10. An emergency bioassay method for actinides in urine.

    PubMed

    Dai, Xiongxin; Kramer-Tremblay, Sheila

    2011-08-01

    A rapid bioassay method has been developed for the sequential measurements of actinides in human urine samples. The method involves actinide separation from a urine matrix by co-precipitation with hydrous titanium oxide (HTiO), followed by anion exchange and extraction chromatography column purification, and final counting by alpha spectrometry after cerium fluoride micro-precipitation. The minimal detectable activities for the method were determined to be 20 mBq L(-1) or less for plutonium, uranium, americium and curium isotopes, with an 8-h sample turn-around time. Spike tests showed that this method would meet the requirements for actinide bioassay following a radiation emergency.

  11. Separating the Minor Actinides Through Advances in Selective Coordination Chemistry

    SciTech Connect

    Lumetta, Gregg J.; Braley, Jenifer C.; Sinkov, Sergey I.; Carter, Jennifer C.

    2012-08-22

    This report describes work conducted at the Pacific Northwest National Laboratory (PNNL) in Fiscal Year (FY) 2012 under the auspices of the Sigma Team for Minor Actinide Separation, funded by the U.S. Department of Energy Office of Nuclear Energy. Researchers at PNNL and Argonne National Laboratory (ANL) are investigating a simplified solvent extraction system for providing a single-step process to separate the minor actinide elements from acidic high-level liquid waste (HLW), including separating the minor actinides from the lanthanide fission products.

  12. Clinical evaluation of the air removal characteristics of an oxygenator with integrated arterial filter in a minimized extracorporeal circuit.

    PubMed

    Stehouwer, Marco C; Boers, Chris; de Vroege, Roel; C Kelder, Johannes; Yilmaz, Alaaddin; Bruins, Peter

    2011-04-01

    The use of minimized extracorporeal circuits (MECC) in cardiac surgery is an important measure to increase the biocompatibility of cardiopulmonary bypass during coronary artery bypass grafting (CABG). These circuits eliminate volume storage reservoirs and bubble traps to minimize the circuit. However, the reduction in volume may increase the risk of gaseous microemboli (GME). The MECC system as used by our group consists of a venous bubble trap, centrifugal pump, and an oxygenator. To further reduce the risk of introducing GME, an oxygenator with an integrated arterial filter was developed based on the concept of minimal volume and foreign surface. We studied the air removal characteristics of this oxygenator with and without integrated arterial filter. The quantity and volume of GME were measured with precision at both the inlet and outlet of the devices. Our results showed that integration of an arterial filter into this oxygenator increased GME reducing capacity from 69.2% to 92%. Moreover, we were able to obtain data on the impact of an arterial filter on the exact size-distribution of GME entering the arterial line. The present study demonstrates that an MECC system and oxygenator with integrated arterial filter significantly reduces the volume and size of GME. The use of an integrated arterial filter in an MECC system may protect the patient from the deleterious effects of CPB and may further improve patient safety.

  13. Characteristics and oil sorption effectiveness of kapok fibre, sugarcane bagasse and rice husks: oil removal suitability matrix.

    PubMed

    Ali, Norizan; El-Harbawi, Mohanad; Jabal, Ayman Abo; Yin, Chun-Yang

    2012-01-01

    The characteristics and water/oil sorption effectiveness ofkapok fibre, sugarcane bagasse and rice husks have been compared. The three biomass types were subjected to field emission scanning electron microscopy-energy dispersive X-ray spectroscopy and surface tension analyses for liquid-air and oil-water systems were conducted. Both kapok fibre and sugarcane bagasse exhibit excellent oil sorption capabilities for diesel, crude, new engine and used engine oils as their oil sorption capacities all exceed 10 g/g. The synthetic sorbent exhibits oil sorption capacities comparable with sugarcane bagasse, while rice husks exhibit the lowest oil sorption capacities among all the sorbents. Kapok fibre shows overwhelmingly high oil-to-water sorption (O/W) ratios ranging from 19.35 to 201.53 while sugarcane bagasse, rice husks and synthetic sorbent have significantly lower O/W ratios (0.76-2.69). This suggests that kapok fibre is a highly effective oil sorbent even in well-mixed oil-water media. An oil sorbent suitability matrix is proposed to aid stakeholders in evaluating customized oil removal usage of the natural sorbents.

  14. Separations and Actinide Science -- 2005 Roadmap

    SciTech Connect

    Not Available

    2005-09-01

    The Separations and Actinide Science Roadmap presents a vision to establish a separations and actinide science research (SASR) base composed of people, facilities, and collaborations and provides new and innovative nuclear fuel cycle solutions to nuclear technology issues that preclude nuclear proliferation. This enabling science base will play a key role in ensuring that Idaho National Laboratory (INL) achieves its long-term vision of revitalizing nuclear energy by providing needed technologies to ensure our nation's energy sustainability and security. To that end, this roadmap suggests a 10-year journey to build a strong SASR technical capability with a clear mission to support nuclear technology development. If nuclear technology is to be used to satisfy the expected growth in U.S. electrical energy demand, the once-through fuel cycle currently in use should be reconsidered. Although the once-through fuel cycle is cost-effective and uranium is inexpensive, a once-through fuel cycle requires long-term disposal to protect the environment and public from long-lived radioactive species. The lack of a current disposal option (i.e., a licensed repository) has resulted in accumulation of more than 50,000 metric tons of spent nuclear fuel. The process required to transition the current once-through fuel cycle to full-recycle will require considerable time and significant technical advancement. INL's extensive expertise in aqueous separations will be used to develop advanced separations processes. Computational chemistry will be expanded to support development of future processing options. In the intermediate stage of this transition, reprocessing options will be deployed, waste forms with higher loading densities and greater stability will be developed, and transmutation of long-lived fission products will be explored. SASR will support these activities using its actinide science and aqueous separations expertise. In the final stage, full recycle will be enabled by

  15. Production Pathways and Separation Procedures for High-Diagnostic-Value Activation Species, Fission Products, and Actinides Required for Preparation of Realistic Synthetic Post-Detonation Nuclear Debris: Status Report and FY16 Project Plan

    SciTech Connect

    Faye, S. A.; Shaughnessy, D. A.

    2015-08-19

    The objective of this project is to provide a comprehensive study on the production routes and chemical separation requirements for activation products, fission products, and actinides required for the creation of realistic post-detonation surrogate debris. Isotopes that have been prioritized by debris diagnosticians will be examined for their ability to be produced at existing irradiation sources, production rates, and availability of target materials, and chemical separation procedures required to rapidly remove the products from the bulk target matrix for subsequent addition into synthetic debris samples. The characteristics and implications of the irradiation facilities on the isotopes of interest will be addressed in addition to a summary of the isotopes that are already regularly produced. This is a planning document only.

  16. Complexation of actinides with derivatives of oxydiaceticacid

    SciTech Connect

    Rao, Linfeng; Tian, Guoxin

    2006-01-04

    Complexation of Np(V), U(VI) and Nd(III) with dimethyl-3-oxa-glutaramic acid (DMOGA) and tetramethyl-3-oxa-glutaramide (TMOGA) was studied in comparison with the complexation with oxydiacetic acid (ODA). Stability constants and enthalpy of complexation were determined by potentiometry, spectrophotometry and calorimetry. Thermodynamic parameters, in conjunction with structural information of solid compounds, indicate that DMOGA and TMOGA form tridentate complexes with the ether-oxygen participating in bonding with actinide/lanthanide ions. The trends in the stability constants, enthalpy and entropy of complexation are discussed in terms of the difference in the hydration of the amide groups and carboxylate groups and the difference in the charge density of the metal ions.

  17. Theoretical atomic volumes of the light actinides

    SciTech Connect

    Jones, M. D.; Boettger, J. C.; Albers, R. C.; Singh, D. J.

    2000-02-15

    The zero-pressure zero-temperature equilibrium volumes and bulk moduli are calculated for the light actinides Th through Pu using two independent all-electron, full-potential, electronic-structure methods: the full-potential linear augmented-plane-wave method and the linear combinations of Gaussian-type orbitals-fitting function method. The results produced by these two distinctly different electronic-structure techniques are in good agreement with each other, but differ significantly from previously published calculations using the full-potential linear muffin-tin-orbital (FP-LMTO) method. The theoretically calculated equilibrium volumes are in some cases nearly 10% larger than the previous FP-LMTO calculations, bringing them much closer to the experimentally observed volumes. We also discuss the anomalous upturn in equilibrium volume seen experimentally for {alpha}-Pu. (c) 2000 The American Physical Society.

  18. Actinides in HD 101065 (Przybylski's Star)

    NASA Astrophysics Data System (ADS)

    Cowley, C. R.; Hubrig, S.; Bord, D. J.

    2003-05-01

    There are many strange things about the abundances in Przybylski's star (HD 101065). The most recent study (MN, 217, 299, 2000) finds that among the elements through copper, the abundances scatter with no apparent pattern. The largest deviations from solar are found for magnesium, which may be deficient by somewhat more than 1 dex, and cobalt, which appears to be in excess by about the same amount. The heavier elements especially those beyond barium, and continuing through the actinides uranium and thorium, show a clear pattern and a remarkable coherence. We plot solar and stellar abundances on a logarithmic plot vs. atomic number Z, and displace the solar points upward by some 3 dex. While individual points do not overlap, there is a remarkable similarity in the overall trends from Z = 58-80, including the maxima caused in the solar case by the third r-process peak. Points for the displaced solar actinides fall near their stellar counterparts. The processes that produced the large enhancements of these heavy elements have not caused large fractionations of adjacent elements. We have new spectra from the ESO UVES spectrograph on UT2. Resolution is 80,000 (blue) and 110,000 (red), with S/N > 300. This material, and new oscillator strengths (AA 381, 1090,2002; AA 382, 368, 2002), allow a more complete analysis of U and Th. We find abundances near +2.5 for both elements (log(H) = 12), but uncertainties at the moment are surely +/- 0.3 dex. We are currently working to improve the accuracy. Current errors preclude the use of these observations for accurate cosmochronometry, even if the chemical differentiation were not relevant. If a U/Th ratio of unity could be taken at face value, it would imply an r-process event some 103 years ago. Thanks to B. Pfeiffer help and advice.

  19. Archetypes for actinide-specific chelating agents

    SciTech Connect

    Smith, W.L.

    1980-01-01

    The complexes of uranium and thorium with monomeric hydroxamic acids can serve as archetypes for an optimized macrochelate designed for tetravalent actinides. The eight-coordinate complexes, Th(i-PrN(O)C(O)R)/sub 4/, where R = tert-butyl or R = neopentyl, have been synthesized and their structures have been determined by x-ray diffraction. The bulky alkyl substituents impart remarkable volatility and hydrocarbon solubility to these complexes, and the steric interactions of these substituents largely determine the structures. When R = tert-butyl, the substituents occupy the corners of a tetrahedron and force the complex into a distorted cubic geometry with crystallographic S/sub 4/ symmetry. Insertion of a methylene group between the carbonyl carbon and the tert-butyl group relaxes the steric requirements, and the coordination polyhedron of the neopentyl derivative is close to the mmmm isomer of the trigonal-faced dodecahedron. Uranium tetrachloride was quantitatively oxidized via an oxygen transfer reaction with two equivalents of N-phenylbenzohydroxamic acid anion (PBHA) in tetrahydrofuran (THF) to form UO/sub 2/ Cl(PBHA)(THF)/sub 2/ and benzanilide. The structure of the uranyl complex has been determined from x-ray diffraction data; the linear uranyl ion is surrounded by a planar pentagonal array composed of two hydroxamate oxygen atoms, a chloride ion and two THF oxygens, such that the chloride ion is opposite the hydroxamate group. That the THF and phenyl rings are twisted from this equatorial plane limits the molecular geometry to that of the C/sub 1/ point group. Some aspects of the chemistry of hydroxamic acids and of their incorporation into molecules that may serve as precursors of tetravalent actinide specific sequestering agents have also been investigated.

  20. Separation of Minor Actinides from Lanthanides by Dithiophosphinic Acid Extractants

    SciTech Connect

    D. R. Peterman; M. R. Greenhalgh; R. D. Tillotson; J. R. Klaehn; M. K. Harrup; T. A. Luther; J. D. Law; L. M. Daniels

    2008-09-01

    The selective extraction of the minor actinides (Am(III) and Cm(III)) from the lanthanides is an important part of advanced reprocessing of spent nuclear fuel. This separation would allow the Am/Cm to be fabricated into targets and recycled to a reactor and the lanthanides to be dispositioned. This separation is difficult to accomplish due to the similarities in the chemical properties of the trivalent actinides and lanthanides. Research efforts at the Idaho National Laboratory have identified an innovative synthetic pathway yielding new regiospecific dithiophosphinic acid (DPAH) extractants. The synthesis provides DPAH derivatives that can address the issues concerning minor actinide separation and extractant stability. For this work, two new symmetric DPAH extractants have been prepared. The use of these extractants for the separation of minor actinides from lanthanides will be discussed.

  1. Actinide targets for the synthesis of super-heavy elements

    SciTech Connect

    Roberto, J.; Alexander, Charles W.; Boll, Rose Ann; Ezold, Julie G.; Felker, Leslie Kevin; Rykaczewski, Krzysztof Piotr; Hogle, Susan L.

    2015-06-18

    Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of 48Ca beams on actinide targets. These target materials, including 242Pu, 244Pu, 243Am, 245Cm, 248Cm, 249Cf, and 249Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing the production of rare actinides including 249Bk, 251Cf, and 254Es are described.

  2. Actinide targets for the synthesis of super-heavy elements

    DOE PAGES

    Roberto, J.; Alexander, Charles W.; Boll, Rose Ann; ...

    2015-06-18

    Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of 48Ca beams on actinide targets. These target materials, including 242Pu, 244Pu, 243Am, 245Cm, 248Cm, 249Cf, and 249Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing themore » production of rare actinides including 249Bk, 251Cf, and 254Es are described.« less

  3. Actinide targets for the synthesis of super-heavy elements

    NASA Astrophysics Data System (ADS)

    Roberto, J. B.; Alexander, C. W.; Boll, R. A.; Burns, J. D.; Ezold, J. G.; Felker, L. K.; Hogle, S. L.; Rykaczewski, K. P.

    2015-12-01

    Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of 48Ca beams on actinide targets. These target materials, including 242Pu, 244Pu, 243Am, 245Cm, 248Cm, 249Cf, and 249Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing the production of rare actinides including 249Bk, 251Cf, and 254Es are described.

  4. Unraveling characteristics of simultaneous nitrification, denitrification and phosphorus removal (SNDPR) in an aerobic granular sequencing batch reactor.

    PubMed

    He, Qiulai; Zhang, Shilu; Zou, Zhuocheng; Zheng, Li-An; Wang, Hongyu

    2016-11-01

    An aerobic granular sequencing batch reactor (SBR) on an aerobic/oxic/anoxic (AOA) mode was operated for 50days with acetate sodium as the sole carbon source for simultaneous carbon, nitrogen and phosphorus removal. Excellent removal efficiencies for chemical oxygen demand (COD) (94.46±3.59%), nitrogen (96.56±3.44% for ammonia nitrogen (NH4(+)-N) and 93.88±6.78% for total inorganic nitrogen (TIN)) and phosphorus (97.71±3.63%) were obtained over operation. Mechanisms for simultaneous nutrients removal were explored and the results indicated that simultaneous nitrification, denitrification and phosphorus removal (SNDPR) under aerobic conditions was mainly responsible for most of nitrogen and phosphorus removal. Identification and quantification of the granular AOA SBR revealed that higher rates of nutrients removal and more potentials were to be exploited by optimizing the operating conditions including time durations for AOA mode and the feeding compositions.

  5. Actinide Source Term Program, position paper. Revision 1

    SciTech Connect

    Novak, C.F.; Papenguth, H.W.; Crafts, C.C.; Dhooge, N.J.

    1994-11-15

    The Actinide Source Term represents the quantity of actinides that could be mobilized within WIPP brines and could migrate with the brines away from the disposal room vicinity. This document presents the various proposed methods for estimating this source term, with a particular focus on defining these methods and evaluating the defensibility of the models for mobile actinide concentrations. The conclusions reached in this document are: the 92 PA {open_quotes}expert panel{close_quotes} model for mobile actinide concentrations is not defensible; and, although it is extremely conservative, the {open_quotes}inventory limits{close_quotes} model is the only existing defensible model for the actinide source term. The model effort in progress, {open_quotes}chemical modeling of mobile actinide concentrations{close_quotes}, supported by a laboratory effort that is also in progress, is designed to provide a reasonable description of the system and be scientifically realistic and supplant the {open_quotes}Inventory limits{close_quotes} model.

  6. Enhancing BWR proliferation resistance fuel with minor actinides

    NASA Astrophysics Data System (ADS)

    Chang, Gray S.

    2009-03-01

    To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced light water reactor- LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides ( 237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of 238Pu/Pu. For future advanced nuclear systems, minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. As a result, MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In the study, a typical boiling water reactor (BWR) fuel unit lattice cell model with UO 2 fuel pins will be used to investigate the effectiveness of minor actinide reduction approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance in the intermediate-term goal for future nuclear energy systems. To account for the water coolant density variation from the bottom (0.76 g/cm 3) to the top (0.35 g/cm 3) of the core, the axial coolant channel and fuel pin were divided to 24 nodes. The MA transmutation characteristics at different elevations were compared and their impact on neutronics criticality discussed. The concept of MARA, which involves the use of transuranic nuclides ( 237Np and/or 241Am), significantly increases the 238Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in

  7. Proliferation Resistance Evaluation of ACR-1000 Fuel with Minor Actinides

    SciTech Connect

    Gray S. Chang

    2008-09-01

    The Global Nuclear Energy Partnership (GNEP) program is to significantly advance the science and technology of nuclear energy systems and to enhance the spent fuel proliferation resistance. It consists of both innovative nuclear reactors and innovative research in separation and transmutation. The merits of nuclear energy are high-density energy, with low environmental impacts (i.e. almost zero greenhouse gas emission). Planned efforts involve near-term and intermediate-term improvements in fuel utilization and recycling in current light water reactors (LWRs) as well as the longer-term development of new nuclear energy systems that offer much improved fuel utilization and proliferation resistance, along with continued advances in operational safety. For future advanced nuclear systems, minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. MAs can play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In this work, an Advanced CANDU Reactor (ACR) fuel unit lattice cell model with 43 UO2 fuel rods will be used to investigate the effectiveness of a Minor Actinide Reduction Approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance. The main MARA objective is to increase the 238Pu / Pu isotope ratio by using the transuranic nuclides (237Np and 241Am) in the high burnup fuel and thereby increase the proliferation resistance even for a very low fuel burnup. As a result, MARA is a very effective approach to enhance the proliferation resistance for the on power refueling ACR system nuclear fuel. The MA transmutation characteristics at different MA loadings were compared and their impact on neutronics

  8. Enhancing BWR Proliferation Resistance Fuel with Minor Actinides

    SciTech Connect

    Gray S. Chang

    2009-03-01

    To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced light water reactor- LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides (237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of 238Pu/Pu. For future advanced nuclear systems, minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. As a result, MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In the study, a typical boiling water reactor (BWR) fuel unit lattice cell model with UO2 fuel pins will be used to investigate the effectiveness of minor actinide reduction approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance in the intermediate-term goal for future nuclear energy systems. To account for the water coolant density variation from the bottom (0.76 g/cm3) to the top (0.35 g/cm3) of the core, the axial coolant channel and fuel pin were divided to 24 nodes. The MA transmutation characteristics at different elevations were compared and their impact on neutronics criticality discussed. The concept of MARA, which involves the use of transuranic nuclides (237Np and/or 241Am), significantly increases the 238Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in atoms

  9. Comparative studies of actinide and sub-actinide fission cross section calculation from MCNP6 and TALYS

    SciTech Connect

    Perkasa, Y. S.; Waris, A. Kurniadi, R. Su'ud, Z.

    2014-09-30

    Comparative studies of actinide and sub-actinide fission cross section calculation from MCNP6 and TALYS have been conducted. In this work, fission cross section resulted from MCNP6 prediction will be compared with result from TALYS calculation. MCNP6 with its event generator CEM03.03 and LAQGSM03.03 have been validated and verified for several intermediate and heavy nuclides fission reaction data and also has a good agreement with experimental data for fission reaction that induced by photons, pions, and nucleons at energy from several ten of MeV to about 1 TeV. The calculation that induced within TALYS will be focused mainly to several hundred MeV for actinide and sub-actinide nuclides and will be compared with MCNP6 code and several experimental data from other evaluator.

  10. Nuclear Dissipation via Peripheral Collisions with Relativistic Radioactive Actinides Beams

    SciTech Connect

    Schmitt, C.; Heinz, A.; Jurado, B.; Kelic, A.; Schmidt, K.-H.

    2007-05-22

    Peripheral collisions with radioactive actinide beams at relativistic energies are proposed as a relevant approach for the study of dissipation in nuclear matter. The characteristics of the systems resulting from the primary fragmentation of such beams are particularly well suited for probing the controversial existence of a sizeable delay in fission. Thanks to the radioactive beam facility at GSI an unusually large set of data involving about 60 secondary unstable projectiles between At and U has been collected under identical conditions. The properties of the set-up enabled the coincident measurement of the atomic number of both fission fragments, permitting a judicious classification of the data. The width of the fission-fragment charge distribution is shown to establish a thermometer at the saddle point which is directly related to the transient delay caused by the friction force. From a comparison with realistic model calculations, the dissipation strength at small deformation and the transient time are inferred. The present strategy is promoted as a complementary approach that avoids some complex problems inherent to conventional techniques. Combined to the paramount size of the data set, it sheds light on contradictory conclusions that have been published in the past. There is at this point no definite consensus on our understanding of the damping process in fission.

  11. Actinide/beryllium neutron sources with reduced dispersion characteristics

    DOEpatents

    Schulte, Louis D.

    2012-08-14

    Neutron source comprising a composite, said composite comprising crystals comprising BeO and AmBe.sub.13, and an excess of beryllium, wherein the crystals have an average size of less than 2 microns; the size distribution of the crystals is less than 2 microns; and the beryllium is present in a 7-fold to a 75-fold excess by weight of the amount of AmBe.sub.13; and methods of making thereof.

  12. Effects of effluent organic matter characteristics on the removal of bulk organic matter and selected pharmaceutically active compounds during managed aquifer recharge: Column study

    NASA Astrophysics Data System (ADS)

    Maeng, Sung Kyu; Sharma, Saroj K.; Abel, Chol D. T.; Magic-Knezev, Aleksandra; Song, Kyung-Guen; Amy, Gary L.

    2012-10-01

    Soil column experiments were conducted to investigate the effects of effluent organic matter (EfOM) characteristics on the removal of bulk organic matter (OM) and pharmaceutically active compounds (PhACs) during managed aquifer recharge (MAR) treatment processes. The fate of bulk OM and PhACs during an MAR is important to assess post-treatment requirements. Biodegradable OM from EfOM, originating from biological wastewater treatment, was effectively removed during soil passage. Based on a fluorescence excitation-emission matrix (F-EEM) analysis of wastewater effluent-dominated (WWE-dom) surface water (SW), protein-like substances, i.e., biopolymers, were removed more favorably than fluorescent humic-like substances under oxic compared to anoxic conditions. However, there was no preferential removal of biopolymers or humic substances, determined as dissolved organic carbon (DOC) observed via liquid chromatography with online organic carbon detection (LC-OCD) analysis. Most of the selected PhACs exhibited removal efficiencies of greater than 90% in both SW and WWE-dom SW. However, the removal efficiencies of bezafibrate, diclofenac and gemfibrozil were relatively low in WWE-dom SW, which contained more biodegradable OM than did SW (copiotrophic metabolism). Based on this study, low biodegradable fractions such as humic substances in MR may have enhanced the degradation of diclofenac, gemfibrozil and bezafibrate by inducing an oligotrophic microbial community via long term starvation. Both carbamazepine and clofibric acid showed persistent behaviors and were not influenced by EfOM.

  13. Effects of effluent organic matter characteristics on the removal of bulk organic matter and selected pharmaceutically active compounds during managed aquifer recharge: Column study.

    PubMed

    Maeng, Sung Kyu; Sharma, Saroj K; Abel, Chol D T; Magic-Knezev, Aleksandra; Song, Kyung-Guen; Amy, Gary L

    2012-10-01

    Soil column experiments were conducted to investigate the effects of effluent organic matter (EfOM) characteristics on the removal of bulk organic matter (OM) and pharmaceutically active compounds (PhACs) during managed aquifer recharge (MAR) treatment processes. The fate of bulk OM and PhACs during an MAR is important to assess post-treatment requirements. Biodegradable OM from EfOM, originating from biological wastewater treatment, was effectively removed during soil passage. Based on a fluorescence excitation-emission matrix (F-EEM) analysis of wastewater effluent-dominated (WWE-dom) surface water (SW), protein-like substances, i.e., biopolymers, were removed more favorably than fluorescent humic-like substances under oxic compared to anoxic conditions. However, there was no preferential removal of biopolymers or humic substances, determined as dissolved organic carbon (DOC) observed via liquid chromatography with online organic carbon detection (LC-OCD) analysis. Most of the selected PhACs exhibited removal efficiencies of greater than 90% in both SW and WWE-dom SW. However, the removal efficiencies of bezafibrate, diclofenac and gemfibrozil were relatively low in WWE-dom SW, which contained more biodegradable OM than did SW (copiotrophic metabolism). Based on this study, low biodegradable fractions such as humic substances in MR may have enhanced the degradation of diclofenac, gemfibrozil and bezafibrate by inducing an oligotrophic microbial community via long term starvation. Both carbamazepine and clofibric acid showed persistent behaviors and were not influenced by EfOM.

  14. The interaction of human serum albumin with selected lanthanide and actinide ions: Binding affinities, protein unfolding and conformational changes.

    PubMed

    Ali, Manjoor; Kumar, Amit; Kumar, Mukesh; Pandey, Badri N

    2016-04-01

    Human serum albumin (HSA), the most abundant soluble protein in blood plays critical roles in transportation of biomolecules and maintenance of osmotic pressure. In view of increasing applications of lanthanides- and actinides-based materials in nuclear energy, space, industries and medical applications, the risk of exposure with these metal ions is a growing concern for human health. In present study, binding interaction of actinides/lanthanides [thorium: Th(IV), uranium: U(VI), lanthanum: La(III), cerium: Ce(III) and (IV)] with HSA and its structural consequences have been investigated. Ultraviolet-visible, Fourier transform-infrared, Raman, Fluorescence and Circular dichroism spectroscopic techniques were applied to study the site of metal ions interaction, binding affinity determination and the effect of metal ions on protein unfolding and HSA conformation. Results showed that these metal ions interacted with carbonyl (CO..:)/amide(N..-H) groups and induced exposure of aromatic residues of HSA. The fluorescence analysis indicated that the actinide binding altered the microenvironment around Trp214 in the subdomain IIA. Binding affinity of U(VI) to HSA was slightly higher than that of Th(IV). Actinides and Ce(IV) altered the secondary conformation of HSA with a significant decrease of α-helix and an increase of β-sheet, turn and random coil structures, indicating a partial unfolding of HSA. A correlation was observed between metal ion's ability to alter HSA conformation and protein unfolding. Both cationic effects and coordination ability of metal ions seemed to determine the consequences of their interaction with HSA. Present study improves our understanding about the protein interaction of these heavy ions and their impact on its secondary structure. In addition, binding characteristics may have important implications for the development of rational antidote for the medical management of health effects of actinides and lanthanides.

  15. Synergistic extraction studies of trivalent actinides and lanthanides using crabs, crowns, and crypts

    SciTech Connect

    Ensor, D.D.; Shah, A.H.

    1984-01-01

    This report will describe the investigations of the synergistic characteristics of the novel neutral oxygen donors 1,13-bis-(quinolyl)-1,4,7,10,13-pentaoxotridecane (K-5), a crab; 4-tert-butylcyclohexo-15crown-5(15-C-5), a crown; and 5,6,14,15-dibenzo-4,7,13,16,21,24-hexaoxo-1,10-diazabicyclo(8,8,8)-hexacosane (222BB), a cryptate, for trivalent lanthanides and actinides in combination with HTTA. 3 references, 2 tables.

  16. A Heterogeneous Sodium Fast Reactor Designed to Transmute Minor Actinide Actinide Waste Isotopes into Plutonium Fuel

    SciTech Connect

    Samuel E. Bays

    2011-02-01

    An axial heterogeneous sodium fast reactor design is developed for converting minor actinide waste isotopes into plutonium fuel. The reactor design incorporates zirconium hydride moderating rods in an axial blanket above the active core. The blanket design traps the active core’s axial leakage for the purpose of transmuting Am-241 into Pu-238. This Pu-238 is then co-recycled with the spent driver fuel to make new driver fuel. Because Pu-238 is significantly more fissile than Am-241 in a fast neutron spectrum, the fissile worth of the initial minor actinide material is upgraded by its preconditioning via transmutation in the axial targets. Because, the Am-241 neutron capture worth is significantly stronger in a moderated epithermal spectrum than the fast spectrum, the axial targets serve as a neutron trap which recovers the axial leakage lost by the active core. The sodium fast reactor proposed by this work is designed as an overall transuranic burner. Therefore, a low transuranic conversion ratio is achieved by a degree of core flattening which increases axial leakage. Unlike a traditional “pancake” design, neutron leakage is recovered by the axial target/blanket system. This heterogeneous core design is constrained to have sodium void and Doppler reactivity worth similar to that of an equivalent homogeneous design. Because minor actinides are irradiated only once in the axial target region; elemental partitioning is not required. This fact enables the use of metal targets with electrochemical reprocessing. Therefore, the irradiation environment of both drivers and targets was constrained to ensure applicability of the established experience database for metal alloy sodium fast reactor fuels.

  17. Fusion Techniques for the Oxidation of Refractory Actinide Oxides

    SciTech Connect

    Rudisill, T.S.

    1999-04-15

    to the potential of achieving higher actinide recoveries from refractory materials. In this experiment, nominally 10 g of a graphite-containing residue generated during plutonium casting operations was initially calcined to remove the graphite. Removal of combustible material prior to a large-scale fusion with Na2O2 is needed due to the large amount of heat liberated during oxidation. Two successive fusions using the residue from the calcination and the residue generated from the initial dissolution allowed recovery of 98 percent of the plutonium. The fusion of the residue following the first dissolution was performed at a higher temperature (600 degrees Celsius versus 450 degrees Celsius during the first fusion). The ability to recover most of the remaining plutonium from the residue suggest the oxidation efficiency of the Na2O2 fusion improves with higher temperatures similar to results observed with NpO2 fusion.

  18. High-quality single crystal growth and strongly correlated electronic states in rare earth and actinide compounds

    NASA Astrophysics Data System (ADS)

    Ōnuki, Yoshichika; Honda, Fuminori; Hirose, Yusuke; Settai, Rikio; Takeuchi, Tetsuya

    2016-11-01

    We review the nature of strongly correlated electronic states in rare earth and actinide compounds, focusing on localized versus itinerant electronic states in CeRhIn5, quantum critical phenomena in YbIr2Zn20, residual resistivity in CeCu6, metamagnetism in heavy fermion compounds, and unconventional superconductivity in CeIrSi3 without inversion symmetry in the crystal structure, emphasizing that sample quality is essentially important to clarify the characteristic features for the heavy fermion compounds.

  19. Nitrogen Removal Characteristics of Pseudomonas putida Y-9 Capable of Heterotrophic Nitrification and Aerobic Denitrification at Low Temperature

    PubMed Central

    He, Tengxia; Ye, Qing; Chen, Yanli; Xie, Enyu; Zhang, Xue

    2017-01-01

    The cold-adapted bacterium Pseudomonas putida Y-9 was investigated and exhibited excellent capability for nitrogen removal at 15°C. The strain capable of heterotrophic nitrification and aerobic denitrification could efficiently remove ammonium, nitrate, and nitrite at an average removal rate of 2.85 mg, 1.60 mg, and 1.83 mg NL−1 h−1, respectively. Strain Y-9 performed nitrification in preference to denitrification when ammonium and nitrate or ammonium and nitrite coexisted in the solution. Meantime, the presence of nitrate had no effect on the ammonium removal rate of strain Y-9, and yet the presence of high concentration of nitrite would inhibit the cell growth and decrease the nitrification rate. The experimental results indicate that P. putida Y-9 has potential application for the treatment of wastewater containing high concentrations of ammonium along with its oxidation products at low temperature. PMID:28293626

  20. Actinide Sorption in Rainier Mesa Tunnel Waters from the Nevada Test Site

    SciTech Connect

    Zhao, P; Zavarin, M; Leif, R; Powell, B; Singleton, M; Lindvall, R; Kersting, A

    2007-12-17

    The sorption behavior of americium (Am), plutonium (Pu), neptunium (Np), and uranium (U) in perched Rainier Mesa tunnel water was investigated. Both volcanic zeolitized tuff samples and groundwater samples were collected from Rainier Mesa, Nevada Test Site, NV for a series of batch sorption experiments. Sorption in groundwater with and without the presence of dissolved organic matter (DOM) was investigated. Am(III) and Pu(IV) are more soluble in groundwater that has high concentrations of DOM. The sorption K{sub d} for Am(III) and Pu(IV) on volcanic zeolitized tuff was up to two orders of magnitude lower in samples with high DOM (15 to 19 mg C/L) compared to samples with DOM removed (< 0.4 mg C/L) or samples with naturally low DOM (0.2 mg C/L). In contrast, Np(V) and U(VI) sorption to zeolitized tuff was much less affected by the presence of DOM. The Np(V) and U(VI) sorption Kds were low under all conditions. Importantly, the DOM was not found to significantly sorb to the zeolitized tuff during these experiment. The concentration of DOM in groundwater affects the transport behavior of actinides in the subsurface. The mobility of Am(III) and Pu(IV) is significantly higher in groundwater with elevated levels of DOM resulting in potentially enhanced transport. To accurately model the transport behavior of actinides in groundwater at Rainier Mesa, the low actinide Kd values measured in groundwater with high DOM concentrations must be incorporated in predictive transport models.

  1. Actinide Production in the Reaction of Heavy Ions withCurium-248

    SciTech Connect

    Moody, K.J.

    1983-07-01

    Chemical experiments were performed to examine the usefulness of heavy ion transfer reactions in producing new, neutron-rich actinide nuclides. A general quasi-elastic to deep-inelastic mechanism is proposed, and the utility of this method as opposed to other methods (e.g. complete fusion) is discussed. The relative merits of various techniques of actinide target synthesis are discussed. A description is given of a target system designed to remove the large amounts of heat generated by the passage of a heavy ion beam through matter, thereby maximizing the beam intensity which can be safely used in an experiment. Also described is a general separation scheme for the actinide elements from protactinium (Z = 91) to mendelevium (Z = 101), and fast specific procedures for plutonium, americium and berkelium. The cross sections for the production of several nuclides from the bombardment of {sup 248}Cm with {sup 18}O, {sup 86}Kr and {sup 136}Xe projectiles at several energies near and below the Coulomb barrier were determined. The results are compared with yields from {sup 48}Ca and {sup 238}U bombardments of {sup 248}Cm. Simple extrapolation of the product yields into unknown regions of charge and mass indicates that the use of heavy ion transfer reactions to produce new, neutron-rich above-target species is limited. The substantial production of neutron-rich below-target species, however, indicates that with very heavy ions like {sup 136}Xe and {sup 238}U the new species {sup 248}Am, {sup 249}Am and {sup 247}Pu should be produced with large cross sections from a {sup 248}Cm target. A preliminary, unsuccessful attempt to isolate {sup 247}Pu is outlined. The failure is probably due to the half life of the decay, which is calculated to be less than 3 minutes. The absolute gamma ray intensities from {sup 251}Bk decay, necessary for calculating the {sup 251}Bk cross section, are also determined.

  2. [Rapid Start-up of Simultaneous Nitrification and Denitrification Coupled Phosphorus Removal Process and Its Performing Characteristics].

    PubMed

    Leng, Lu; Xin, Xin; Lu, Hang; Tang, Ya-nan; Wan, Li-hua; Guo, Jun-yuan; Cheng, Qing-feng

    2015-11-01

    In this study, simultaneous nitrification and denitrification (SND) coupled Phosphorus removal process through gradually decreasing DO concentration was investigated by treating wastewater with a low COD/TN ratio (C/N = 3 : 1-4: 1) in a sequencing batch reactor (SBR) inoculated with aerobic granular sludge (AGS). Successful SND coupled Phosphorus phenomenon occurred after 20d at the DO concentration of 0.50-1.0 mg x L(-1). In the following 40 days, the average removal rates of COD, NH4(+) -N, TN and TP were 84.84% , 93.51%, 77.06% and 85.69%, and the NO3(-) -N and NO2(-) -N average accumulations in the effluent were only 4.01 mg x L(-1) and 3.17 mg x L(-1), respectively. The AGS had complete forms and good settling performances, and the sludge volume index (SVI) was about 55.22 mL x g(-1) at the end of starting-up stage. The results of different nitrogen sources showed that the removal rate of TN was in the order of NH4(+) -N > NO2(-) -N > NO3(-) -N, and the removal rate of TP was in the order of NO3(-) -N > NO2(-) -N > NH4(+) -N. The nitrogen and phosphorus removal of wastewater were mainly realized by simultaneous nitrification and denitrification and denitrifying phosphorus removal, respectively.

  3. Correlation and relativistic effects in actinide ions

    SciTech Connect

    Safronova, U. I.; Safronova, M. S.

    2011-11-15

    Wavelengths, line strengths, and transition rates are calculated for the multipole (E1, M1, E2, M2, E3, and M3) transitions between the excited 6s{sup 2}6p{sup 5}nl and 6s6p{sup 6}nl states and the ground 6s{sup 2}6p{sup 6} state in Ac{sup 3+}, Th{sup 4+}, and U{sup 6+} Rn-like ions. Relativistic many-body perturbation theory (RMBPT), including the Breit interaction, is used to evaluate energies and transition rates for multipole transitions in these hole-particle systems. The RMBPT method agrees with multiconfigurational Dirac-Fock (MCDF) calculations in lowest order, includes all second-order correlation corrections, and includes corrections from negative-energy states. The calculations start from a [Xe]4f{sup 14}5d{sup 10}6s{sup 2}6p{sup 6} Dirac-Fock potential. First-order perturbation theory is used to obtain intermediate-coupling coefficients, and second-order RMBPT is used to determine the matrix elements. Evaluated multipole matrix elements for transitions from excited states to the ground states are used to determine the line strengths, transition rates, and multipole polarizabilities. This work provides a number of yet unmeasured properties of these actinide ions for various applications and for benchmark tests of theory and experiment.

  4. Synthesis of crystalline ceramics for actinide immobilisation

    SciTech Connect

    Burakov, B.; Gribova, V.; Kitsay, A.; Ojovan, M.; Hyatt, N.C.; Stennett, M.C.

    2007-07-01

    Methods for the synthesis of ceramic wasteforms for the immobilization of actinides are common to those for non-radioactive ceramics: hot uniaxial pressing (HUP); hot isostatic pressing (HIP); cold pressing followed by sintering; melting (for some specific ceramics, such as garnet/perovskite composites). Synthesis of ceramics doped with radionuclides is characterized with some important considerations: all the radionuclides should be incorporated into crystalline structure of durable host-phases in the form of solid solutions and no separate phases of radionuclides should be present in the matrix of final ceramic wasteform; all procedures of starting precursor preparation and ceramic synthesis should follow safety requirements of nuclear industry. Synthesis methods that avoid the use of very high temperatures and pressures and are easily accomplished within the environment of a glove-box or hot cell are preferable. Knowledge transfer between the V. G. Khlopin Radium Institute (KRI, Russia) and Immobilisation Science Laboratory (ISL, UK) was facilitated in the framework of a joint project supported by UK Royal Society. In order to introduce methods of precursor preparation and ceramic synthesis we selected well-known procedures readily deployable in radiochemical processing plants. We accounted that training should include main types of ceramic wasteforms which are currently discussed for industrial applications. (authors)

  5. Rapid determination of alpha emitters using Actinide resin.

    PubMed

    Navarro, N; Rodriguez, L; Alvarez, A; Sancho, C

    2004-01-01

    The European Commission has recently published the recommended radiological protection criteria for the clearance of building and building rubble from the dismantling of nuclear installations. Radionuclide specific clearance levels for actinides are very low (between 0.1 and 1 Bq g(-1)). The prevalence of natural radionuclides in rubble materials makes the verification of these levels by direct alpha counting impossible. The capability of Actinide resin (Eichrom Industries, Inc.) for extracting plutonium and americium from rubble samples has been tested in this work. Besides a strong affinity for actinides in the tri, tetra and hexavalent oxidation states, this extraction chromatographic resin presents an easy recovery of absorbed radionuclides. The retention capability was evaluated on rubble samples spiked with certified radionuclide standards (239Pu and 241Am). Samples were leached with nitric acid, passed through a chromatographic column containing the resin and the elution fraction was measured by LSC. Actinide retention varies from 60% to 80%. Based on these results, a rapid method for the verification of clearance levels for actinides in rubble samples is proposed.

  6. Recovery and chemical purification of actinides at JRC, Karlsruhe

    NASA Astrophysics Data System (ADS)

    Bokelund, H.; Apostolidis, C.; Glatz, J.-P.

    1989-07-01

    The application of actinide elements in research and in technology is many times subject to rather stringent purity requirements; often a nuclear grade quality is specified. The additional possible demand for a high isotopic purity is a special feature in the handling of these elements. The amount of actinide elements contained in or adhering to materials declared as waste should be low for safety reasons and out of economic considerations. The release of transuranium elements to the environment must be kept negligible. For these and for other reasons a keen interest in the separation of actinides from various materials exists, either for a re-use through recycling, or for their safe confinement in waste packages. This paper gives a short review of the separation methods used for recovery and purification of actinide elements over the past years in the European Institute for Transuranium Elements. The methods described here involve procedures based on precipitation, ion exchange or solvent extraction; often used in a combination. The extraction methods were preferably applied in a Chromatographie column mode. The actinide elements purified and/or separated from each other by the above methods include uranium, neptunium, plutonium, americium, curium, and californium. For the various elements the work was undertaken with different aims, ranging from reprocessing and fabrication of nuclear fuels on a kilogramme scale, over the procurement of alpha-free waste, to the preparation of neutron sources of milligramme size.

  7. Gas core reactors for actinide transmutation and breeder applications

    NASA Technical Reports Server (NTRS)

    Clement, J. D.; Rust, J. H.

    1978-01-01

    This work consists of design power plant studies for four types of reactor systems: uranium plasma core breeder, uranium plasma core actinide transmuter, UF6 breeder and UF6 actinide transmuter. The plasma core systems can be coupled to MHD generators to obtain high efficiency electrical power generation. A 1074 MWt UF6 breeder reactor was designed with a breeding ratio of 1.002 to guard against diversion of fuel. Using molten salt technology and a superheated steam cycle, an efficiency of 39.2% was obtained for the plant and the U233 inventory in the core and heat exchangers was limited to 105 Kg. It was found that the UF6 reactor can produce high fluxes (10 to the 14th power n/sq cm-sec) necessary for efficient burnup of actinide. However, the buildup of fissile isotopes posed severe heat transfer problems. Therefore, the flux in the actinide region must be decreased with time. Consequently, only beginning-of-life conditions were considered for the power plant design. A 577 MWt UF6 actinide transmutation reactor power plant was designed to operate with 39.3% efficiency and 102 Kg of U233 in the core and heat exchanger for beginning-of-life conditions.

  8. Theoretical investigation on multiple bonds in terminal actinide nitride complexes.

    PubMed

    Wu, Qun-Yan; Wang, Cong-Zhi; Lan, Jian-Hui; Xiao, Cheng-Liang; Wang, Xiang-Ke; Zhao, Yu-Liang; Chai, Zhi-Fang; Shi, Wei-Qun

    2014-09-15

    A series of actinide (An) species of L-An-N compounds [An = Pa-Pu, L = [N(CH2CH2NSiPr(i)3)3](3-), Pr(i) = CH(CH3)2] have been investigated using scalar relativistic density functional theory (DFT) without considering spin-orbit coupling effects. The ground state geometric and electronic structures and natural bond orbital (NBO) analysis of actinide compounds were studied systematically in neutral and anionic forms. It was found that with increasing actinide atomic number, the bond length of terminal multiple An-N1 bond decreases, in accordance with the actinide contraction. The Mayer bond order of An-N1 decreases gradually from An = Pa to Pu, which indicates a decrease in bond strength. The terminal multiple bond for L-An-N compounds contains one σ and two π molecular orbitals, and the contributions of the 6d orbital to covalency are larger in magnitude than the 5f orbital based on NBO analysis and topological analysis of electron density. This work may help in understanding of the bonding nature of An-N multiple bonds and elucidating the trends and electronic structure changes across the actinide series. It can also shed light on the construction of novel An-N multiple bonds.

  9. Siderocalin-mediated recognition, sensitization, and cellular uptake of actinides

    PubMed Central

    Allred, Benjamin E.; Rupert, Peter B.; Gauny, Stacey S.; An, Dahlia D.; Ralston, Corie Y.; Sturzbecher-Hoehne, Manuel; Strong, Roland K.; Abergel, Rebecca J.

    2015-01-01

    Synthetic radionuclides, such as the transuranic actinides plutonium, americium, and curium, present severe health threats as contaminants, and understanding the scope of the biochemical interactions involved in actinide transport is instrumental in managing human contamination. Here we show that siderocalin, a mammalian siderophore-binding protein from the lipocalin family, specifically binds lanthanide and actinide complexes through molecular recognition of the ligands chelating the metal ions. Using crystallography, we structurally characterized the resulting siderocalin–transuranic actinide complexes, providing unprecedented insights into the biological coordination of heavy radioelements. In controlled in vitro assays, we found that intracellular plutonium uptake can occur through siderocalin-mediated endocytosis. We also demonstrated that siderocalin can act as a synergistic antenna to sensitize the luminescence of trivalent lanthanide and actinide ions in ternary protein–ligand complexes, dramatically increasing the brightness and efficiency of intramolecular energy transfer processes that give rise to metal luminescence. Our results identify siderocalin as a potential player in the biological trafficking of f elements, but through a secondary ligand-based metal sequestration mechanism. Beyond elucidating contamination pathways, this work is a starting point for the design of two-stage biomimetic platforms for photoluminescence, separation, and transport applications. PMID:26240330

  10. Siderocalin-mediated recognition, sensitization, and cellular uptake of actinides.

    PubMed

    Allred, Benjamin E; Rupert, Peter B; Gauny, Stacey S; An, Dahlia D; Ralston, Corie Y; Sturzbecher-Hoehne, Manuel; Strong, Roland K; Abergel, Rebecca J

    2015-08-18

    Synthetic radionuclides, such as the transuranic actinides plutonium, americium, and curium, present severe health threats as contaminants, and understanding the scope of the biochemical interactions involved in actinide transport is instrumental in managing human contamination. Here we show that siderocalin, a mammalian siderophore-binding protein from the lipocalin family, specifically binds lanthanide and actinide complexes through molecular recognition of the ligands chelating the metal ions. Using crystallography, we structurally characterized the resulting siderocalin-transuranic actinide complexes, providing unprecedented insights into the biological coordination of heavy radioelements. In controlled in vitro assays, we found that intracellular plutonium uptake can occur through siderocalin-mediated endocytosis. We also demonstrated that siderocalin can act as a synergistic antenna to sensitize the luminescence of trivalent lanthanide and actinide ions in ternary protein-ligand complexes, dramatically increasing the brightness and efficiency of intramolecular energy transfer processes that give rise to metal luminescence. Our results identify siderocalin as a potential player in the biological trafficking of f elements, but through a secondary ligand-based metal sequestration mechanism. Beyond elucidating contamination pathways, this work is a starting point for the design of two-stage biomimetic platforms for photoluminescence, separation, and transport applications.

  11. Laboratory studies of actinide metal-silicate fractionation

    NASA Technical Reports Server (NTRS)

    Jones, J. H.; Burnett, D. S.

    1980-01-01

    Actinide and Sm partition coefficients between silicate melt and several metallic phases have been measured. Under reducing conditions Si, Th, U and Pu can be reduced to metals from silicate melts and alloyed with a platinum-gold alloy. U and Pu enter a molten Pt-Si alloy with roughly equal affinity but U strongly partitions into the solid Pt. Th behaves qualitatively the same as Pu but is much less readily reduced than U, and Sm appears to remain unreduced. Experiments with Fe metal have shown that the partition coefficients of the actinides between Fe and silicate liquid are extremely low, suggesting a very low actinide concentration in planetary cores. Experiments show that platinum metals can efficiently fractionate actinides and fractionate actinides from lanthanides and this process may be relevant to the condensation behavior of these elements from the solar nebula. Pt-metal grains in Allende Ca-Al-rich inclusions appear to be U-poor, although the sub-class of Zr-bearing Pt metals may have high U contents.

  12. Crystal growth methods dedicated to low solubility actinide oxalates

    NASA Astrophysics Data System (ADS)

    Tamain, C.; Arab-Chapelet, B.; Rivenet, M.; Grandjean, S.; Abraham, F.

    2016-04-01

    Two novel crystal growth syntheses dedicated to low solubility actinide-oxalate systems and adapted to glove box handling are described. These methods based on the use of precursors of either actinide metal or oxalic acid have been optimized on lanthanide systems (analogue of actinides(III)) and then assessed on real actinide systems. They allow the synthesis of several actinide oxalate single crystals, Am2(C2O4)3(H2O)3·xH2O, Th(C2O4)2·6H2O, M2+x[PuIV2-xPuIIIx(C2O4)5]·nH2O and M1-x[PuIII1-xPuIVx(C2O4)2·H2O]·nH2O. It is the first time that these well-known compounds are formed by crystal growth methods, thus enabling direct structural studies on transuranic element systems and acquisition of basic data beyond deductions from isomorphic (or not) lanthanide compounds. Characterizations by X-ray diffraction, UV-visible solid spectroscopy, demonstrate the potentialities of these two crystal growth methods to obtain oxalate compounds.

  13. A Summary of Actinide Enrichment Technologies and Capability Gaps

    SciTech Connect

    Patton, Bradley D.; Robinson, Sharon M.

    2017-01-01

    The evaluation performed in this study indicates that a new program is needed to efficiently provide a national actinide radioisotope enrichment capability to produce milligram-to-gram quantities of unique materials for user communities as summarized in Table 1. This program xiv should leverage past actinide enrichment, the recent advances in stable isotope enrichment, and assessments of the future requirements to cost effectively develop this capability while establishing an experience base for a new generation of researchers in this vital area. Preliminary evaluations indicate that an EMIS device would have the capability to meet the future needs of the user community for enriched actinides. The EMIS technology could be potentially coupled with other enrichment technologies, such as irradiation, as pre-enrichment and/or post-enrichment systems to increase the throughput, reduce losses of material, and/or reduce operational costs of the base EMIS system. Past actinide enrichment experience and advances in the EMIS technology applied in stable isotope separations should be leveraged with this new evaluation information to assist in the establishment of a domestic actinide radioisotope enrichment capability.

  14. Characteristics of a heterotrophic nitrogen removal bacterium and its potential application on treatment of ammonium-rich wastewater.

    PubMed

    Zhao, Bin; Tian, Meng; An, Qiang; Ye, Jun; Guo, Jin Song

    2017-02-01

    Nitrogen and organic carbon are major pollutants in wastewater causing environmental problems. Alcaligenes faecalis strain NR, isolated from activated sludge, exhibited the ability to remove ammonium and organic carbon from wastewater simultaneously under sole aerobic conditions in batch culture. Changes in carbon type, C/N ratio, oxygen concentration and inorganic ions significantly affected the treatment efficiency. Furthermore, a continuous bioreactor, solely inoculated with A. faecalis strain NR, was conducted to assess its feasibility for simultaneous nitrogen and organic matter removal in a single aerated reactor. Approximately 66.7-78.3% of NH4(+)-N and 85.8-92.2% of TOC were removed by using synthetic wastewater with 150-200mg/L of NH4(+)-N and 1350-2000mg/L of TOC. This research would be valuable to develop an innovative treatment method for ammonium-rich wastewater under aerobic conditions.

  15. Effects of floc aluminum on activated sludge characteristics and removal of 17-alpha-ethinylestradiol in wastewater systems.

    PubMed

    Park, Chul; Fang, Yuan; Murthy, Sudhir N; Novak, John T

    2010-03-01

    The effects of floc aluminum (Al) on activated sludge performance and 17-alpha-ethinylestradiol (EE2) removal were studied using bench-scale activated sludge systems. The results showed that higher Al-fed activated sludge led to better settling, dewatering, and effluent quality with better EE2 removal. EE2 concentrations in the effluent revealed correlations with effluent suspended solids and large particulate/colloidal effluent biopolymer (protein+polysaccharide). Furthermore, a significant correlation existed between effluent proteins and EE2 for all size fractions, indicating that hydrophobic proteinaceous colloids provide binding sites for EE2 and washout together into the effluent. These results suggest that aluminum plays a crucial role in bioflocculation of activated sludge and the efficacy of flocculation influences the removal of endocrine disrupting compounds (EDCs) from wastewater treatment systems.

  16. [Effect of internal recycle ratio on nitrogen and phosphorus removal characteristics in A2/O-BAF process].

    PubMed

    Chen, Yong-Zhi; Peng, Yong-Zhen; Wang, Jian-Hua; Zhang, Liang-Chang

    2011-01-01

    The behaviors of biological phosphorus (P) and nitrogen (N) removal in a lab-scaled anaerobic/anoxic/oxic-biological aerated filter (A2/O-BAF) combined system were investigated during the treatment of real domestic wastewater with the temperature at 15 degrees C, the C/N ratio of 4.9 and internal recycle ratio of 100%, 200%, 300% and 400%. Experimental results clearly showed that COD, N and P can be simultaneously deeply removed in this combined system. When the total HRT was 8.0 h, SRT was 15 d,sludge recycle ratio was 100% and MLSS was 4.0 mg x L(-1), the concentrations of COD, total phosphorus (TP) and ammonia nitrogen could be reached to less than 50.0, 0.5 and 1.0 mg x L(-1) in the effluent, respectively. The concentrations of total nitrogen (TN) could be reduced from 70.9, 72.1, 70.6 and 73.3 mg x L(-1) in the raw wastewater to that of 24.8, 16.5, 9.6 and 8.7 mg x L(-1) in the effluent, respectively. The removal efficiencies of TN were 65.0%, 77.1%, 86.4% and 88.1%, respectively. There was no distinct relationship between the internal recycle ratio and the removal efficiencies of COD, TP and ammonia nitrogen. However, the removal efficiencies of TN increased with the increasing of the internal recycle ratio, the rising rate was descending. Both the capacity of denitrifying and phosphorus removal in anoxic zone increased simultaneously with the increasing of the internal recycle ratio. Batch tests indicated that the population of denitrifying polyphosphate-accumulating organisms (DPAOs) was up to 40.5% of the total phosphate-accumulating organisms (PAOs).

  17. STRONTIUM AND ACTINIDE SORPTION BY MST AND MMST UNDER CONDITIONS REVELANT TO THE SMALL COLUMN ION-EXCHANGE PROCESS

    SciTech Connect

    Taylor-Pashow, K.; Hobbs, D.; Poirier, M.

    2011-05-06

    A series of tests were performed to examine the kinetics of Sr and actinide removal by monosodium titanate (MST) and modified monosodium titanate (mMST) under mixing conditions similar to what will be provided in the Small Column Ion Exchange (SCIX) Program. Similar removal kinetics were seen for two different mixing energies, indicating that under these conditions bulk solution transport is not the rate limiting step for Sr and actinide removal. Sr removal was found to be rapid for both MST and mMST, reaching steady-state conditions within six hours. In contrast, at least six weeks is necessary to reach steady-state conditions for Pu with MST. For mMST, steady-state conditions for Pu were achieved within two weeks. The actual contact time required for the SCIX process will depend on starting sorbate concentrations as well as the requirements for the decontaminated salt solution. During testing leaks occurred in both the MST and mMST tests and evidence of potential desorption was observed. The desorption likely occurred as a result of the change in solids to liquid phase ratio that occurred due to the loss of solution. Based on these results, Savannah River National Laboratory (SRNL) recommended additional testing to further study the effect of changing phase ratios on desorption. This testing is currently in progress and results will be documented in a separate report.

  18. Method and apparatus for providing negative ions of actinide-metal hexafluorides

    DOEpatents

    Compton, Robert N.; Reinhardt, Paul W.; Garrett, William R.

    1978-01-01

    This invention relates to a novel method and a novel generator, or source, for providing gaseous negative ions of selected metal hexafluorides. The method is summarized as follows: in an evacuated zone, reacting gaseous fluorine with an actinide-metal body selected from the group consisting of uranium, plutonium, neptunium, and americium to convert at least part of the metal to the hexafluoride state, thus producing gaseous negatively charged metal-hexafluoride ions in the evacuated zone, and applying an electric field to the zone to remove the ions therefrom. The ion source comprises a chamber defining a reaction zone; means for evacuating the zone; an actinide-metal body in the zone, the metal being uranium, plutonium, neptunium, or americium; means for contacting the body with gaseous fluorine to convert at least a part thereof to the hexafluoride state; and means for applying an electric field to the evacuated zone to extract gaseous, negatively charged metal-hexafluoride ions therefrom. The invention provides unique advantages over conventional surface-ionization techniques for producing such ions.

  19. Prompt Fission Neutron Spectra of Actinides

    SciTech Connect

    Capote, R; Chen, Y J; Hambsch, F J; Kornilov, N V; Lestone, J P; Litaize, O; Morillon, B; Neudecker, D; Oberstedt, S; Ohsawa, T; Smith, D. L.

    2016-01-01

    The energy spectrum of prompt neutrons emitted in fission (PFNS) plays a very important role in nuclear science and technology. A Coordinated Research Project (CRP) “Evaluation of Prompt Fission Neutron Spectra of Actinides”was established by the IAEA Nuclear Data Section in 2009, with the major goal to produce new PFNS evaluations with uncertainties for actinide nuclei. The following technical areas were addressed: (i) experiments and uncertainty quantification (UQ): New data for neutron-induced fission of 233U, 235U, 238U, and 239Pu have been measured, and older data have been compiled and reassessed. There is evidence from the experimental work of this CRP that a very small percentage of neutrons emitted in fission are actually scission neutrons; (ii) modeling: The Los Alamos model (LAM) continues to be the workhorse for PFNS evaluations. Monte Carlo models have been developed that describe the fission phenomena microscopically, but further development is needed to produce PFNS evaluations meeting the uncertainty targets; (iii) evaluation methodologies: PFNS evaluations rely on the use of the least-squares techniques for merging experimental and model data. Considerable insight was achieved on how to deal with the problem of too small uncertainties in PFNS evaluations. The importance of considering that all experimental PFNS data are “shape” data was stressed; (iv) PFNS evaluations: New evaluations, including covariance data, were generated for major actinides including 1) non-model GMA evaluations of the 235U(nth,f), 239Pu(nth,f), and 233U(nth,f) PFNS based exclusively on experimental data (0.02 ≤ E ≤ 10 MeV), which resulted in PFNS average energies E of 2.00±0.01, 2.073±0.010, and 2.030±0.013 MeV, respectively; 2) LAM evaluations of neutron-induced fission spectra on uranium and plutonium targets with improved UQ for incident energies from thermal up to 30 MeV; and 3) Point-by-Point calculations for 232Th, 234U and 237Np targets; and (v) data

  20. Determination of actinides at the radiological and environmental sciences laboratory

    NASA Astrophysics Data System (ADS)

    Williams, R. L.; Grothaus, G. E.

    1984-06-01

    This article briefly describes some of the techniques and procedures that have been developed at the Radiological and Environmental Sciences Laboratory (RESL) to determine the actinides in environmental and biological samples. Dried or ashed samples are totally decomposed in high temperature fusions or with an acid dissolution method. Actinides of interest are coprecipitated from the sample matrix with barium sulfate, cerium fluoride, or a combination of ferrous phosphate and calcium fluoride precipitations. The precipitates are dissolved in perchloric acid and extracted with bis(2-ethylhexyl)phosphoric acid (HDEHP) or dissolved in acidic aluminum nitrate and extracted with Aliquat-336. Actinides in the stripped fractions are coprecipitated with 50 μg of cerium as cerium fluoride, filtered onto membrane filters and counted by alpha spectrometry. The described procedures enable an experienced analyst to prepare sixteen 1 g soil or twelve 5 g faecal ash samples for alpha spectrometry in 14 to 16 working-hours.

  1. Actinide Dioxides in Water: Interactions at the Interface

    SciTech Connect

    Alexandrov, Vitaly; Shvareva, Tatiana Y.; Hayun, Shmuel; Asta, Mark; Navrotsky, Alexandra

    2011-12-15

    A comprehensive understanding of chemical interactions between water and actinide dioxide surfaces is critical for safe operation and storage of nuclear fuels. Despite substantial previous research, understanding the nature of these interactions remains incomplete. In this work, we combine accurate calorimetric measurements with first-principles computational studies to characterize surface energies and adsorption enthalpies of water on two fluorite-structured compounds, ThO₂ and CeO₂, that are relevant for understanding the behavior of water on actinide oxide surfaces more generally. We determine coverage-dependent adsorption enthalpies and demonstrate a mixed molecular and dissociative structure for the first hydration layer. The results show a correlation between the magnitude of the anhydrous surface energy and the water adsorption enthalpy. Further, they suggest a structural model featuring one adsorbed water molecule per one surface cation on the most stable facet that is expected to be a common structural signature of water adsorbed on actinide dioxide compounds.

  2. Actinide chemistry in Allende Ca-Al-rich inclusions

    NASA Technical Reports Server (NTRS)

    Murrell, M. T.; Burnett, D. S.

    1987-01-01

    Fission track radiography is used to investigate the U and Th microscale distribution in a set of Allende-meteorite Ca-Al-rich inclusions. In the Type B inclusions, the major phases melilite and fassaite are important actinide host phases, and on the rims of Type B inclusions and throughout all other inclusions studied, perovskite is the dominant actinide host phase. Results suggest that neither alteration nor loss or gain of an actinide-rich phase appears to have been an important Th/U fractionation mechanism, and that volatility differences may be the dominant factor. Th/U and rare earth element abundance patterns for the spinel and perovskite rim suggest rim formation by volatilization of interior material, and within the constraints of the brief time scale required for this heating, several mechanisms for spinel-perovskite rim formation are possible.

  3. Actinide chemistry in Allende Ca-Al-rich inclusions

    NASA Astrophysics Data System (ADS)

    Murrell, M. T.; Burnett, D. S.

    1987-04-01

    Fission track radiography is used to investigate the U and Th microscale distribution in a set of Allende-meteorite Ca-Al-rich inclusions. In the Type B inclusions, the major phases melilite and fassaite are important actinide host phases, and on the rims of Type B inclusions and throughout all other inclusions studied, perovskite is the dominant actinide host phase. Results suggest that neither alteration nor loss or gain of an actinide-rich phase appears to have been an important Th/U fractionation mechanism, and that volatility differences may be the dominant factor. Th/U and rare earth element abundance patterns for the spinel and perovskite rim suggest rim formation by volatilization of interior material, and within the constraints of the brief time scale required for this heating, several mechanisms for spinel-perovskite rim formation are possible.

  4. FY2010 Annual Report for the Actinide Isomer Detection Project

    SciTech Connect

    Warren, Glen A.; Francy, Christopher J.; Ressler, Jennifer J.; Erikson, Luke E.; Miller, Erin A.; Hatarik, R.

    2011-01-01

    This project seeks to identify a new signature for actinide element detection in active interrogation. This technique works by exciting and identifying long-lived nuclear excited states (isomers) in the actinide isotopes and/or primary fission products. Observation of isomers in the fission products will provide a signature for fissile material. For the actinide isomers, the decay time and energy of the isomeric state is unique to a particular isotope, providing an unambiguous signature for Special Nuclear Materials (SNM). Future work will include a follow-up measurement scheduled for December 2010 at LBNL. Lessons learned from the July 2010 measurements will be incorporated into these new measurements. Analysis of both the July and December experiments will be completed in a few months. A research paper to be submitted to a peer-reviewed journal will be drafted if the conclusions from the measurements warrant publication.

  5. A new opportunity: coincident spectroscopy in neutron-deficient actinides

    NASA Astrophysics Data System (ADS)

    Gothe, Oliver; Gates, J. M.; Gregorich, K. E.; Baartman, B.; Fallon, P.; Esker, N. E.; Kwarsick, J.; Machiavelli, A. O.; Mudder, P. R.; Olive, D. T.; Pang, G.; Rissanen, J.; Nitsche, H.

    2014-09-01

    Due to high γ-ray background rates heavy element production facilities are usually not sensitive to the electron capture decay of neutron deficient actinides. We have developed new capabilities at the Berkeley Gas Filled Separator (BGS) that allow us to study these isotopes. The highly selective and efficient separation of compound nucleus evaporation residue products using the BGS couple with a rapid delivery to a low-background detector facility, opens up many new possibilities for nuclear decay and structure studies in the neutron deficient actinides. The decay of these actinides produces vacancies in the K-shell resulting in x-rays uniquely identifying the Z of the decay products. We present the first results of this new methodology in studying the nuclear structure of fermium-254 by observing the gamma rays in coincidence with fermium x-rays. Coincident gamma-decay spectroscopy gives us a new tool to study the nuclear structure of previously inaccessible systems.

  6. Systematic view of optical absorption spectra in the actinide series

    SciTech Connect

    Carnall, W.T.

    1985-01-01

    In recent years sufficient new spectra of actinides in their numerous valence states have been measured to encourage a broader scale analysis effort than was attempted in the past. Theoretical modelling in terms of effective operators has also undergone development. Well established electronic structure parameters for the trivalent actinides are being used as a basis for estimating parameters in other valence states and relationships to atomic spectra are being extended. Recent contributions to our understanding of the spectra of 4+ actinides have been particularly revealing and supportive of a developing general effort to progress beyond a preoccupation with modelling structure to consideration of the much broader area of structure-bonding relationships. We summarize here both the developments in modelling electronic structure and the interpretation of apparent trends in bonding. 60 refs., 9 figs., 1 tab.

  7. Actinide science with soft x-ray synchrotron radiation

    NASA Astrophysics Data System (ADS)

    Shuh, David K.

    2000-07-01

    The primary methods for the experimental investigation of actinide materials in the VUV/soft x-ray region are the complementary photoelectron spectroscopies, near-edge x-ray absorption fine structure (NEXAFS), and x-ray emission spectroscopy (XES) techniques. Resonant photoemission techniques capable of resolving the 5f electron contributions to actinide bonding along with angle-resolving measurements for band structure and surface structure determinations, have clear and immediate applications. Venerable angle-integrating core and valence band photoelectron spectroscopy are valuable for characterization and analytical purposes. Combined with results from NEXAFS measurements, these techniques will provide the information needed to develop improved understandings of the electronic structure of actinide materials and their surface chemistries/physics.

  8. Advancing the scientific basis of trivalent actinide-lanthanide separations

    SciTech Connect

    Nash, K.L.

    2013-07-01

    For advanced fuel cycles designed to support transmutation of transplutonium actinides, several options have been demonstrated for process-scale aqueous separations for U, Np, Pu management and for partitioning of trivalent actinides and fission product lanthanides away from other fission products. The more difficult mutual separation of Am/Cm from La-Tb remains the subject of considerable fundamental and applied research. The chemical separations literature teaches that the most productive alternatives to pursue are those based on ligand donor atoms less electronegative than O, specifically N- and S-containing complexants and chloride ion (Cl{sup -}). These 'soft-donor' atoms have exhibited usable selectivity in their bonding interactions with trivalent actinides relative to lanthanides. In this report, selected features of soft donor reagent design, characterization and application development will be discussed. The roles of thiocyanate, aminopoly-carboxylic acids and lactate in separation processes are detailed. (authors)

  9. In pursuit of homoleptic actinide alkyl complexes.

    PubMed

    Seaman, Lani A; Walensky, Justin R; Wu, Guang; Hayton, Trevor W

    2013-04-01

    This Forum Article describes the pursuit of isolable homoleptic actinide alkyl complexes, starting with the pioneering work of Gilman during the Manhattan project. The initial reports in this area suggested that homoleptic uranium alkyls were too unstable to be isolated, but Wilkinson demonstrated that tractable uranium alkyls could be generated by purposeful "ate" complex formation, which serves to saturate the uranium coordination sphere and provide the complexes with greater kinetic stability. More recently, we reported the solid-state molecular structures of several homoleptic uranium alkyl complexes, including [Li(THF)4][U(CH2(t)Bu)5], [Li(TMEDA)]2[UMe6], [K(THF)]3[K(THF)2][U(CH2Ph)6]2, and [Li(THF)4][U(CH2SiMe3)6], by employing Wilkinson's strategy. Herein, we describe our attempts to extend this chemistry to thorium. The treatment of ThCl4(DME)2 with 5 equiv of LiCH2(t)Bu or LiCH2SiMe3 at -25 °C in THF affords [Th(CH2(t)Bu)5] (1) and [Li(DME)2][Th(CH2SiMe3)5 (2), respectively, in moderate yields. Similarly, the treatment of ThCl4(DME)2 with 6 equiv of K(CH2Ph) produces [K(THF)]2[Th(CH2Ph)6] (3), in good yield. Complexes 1-3 have been fully characterized, while the structures of 1 and 3 were confirmed by X-ray crystallography. Additionally, the electronic properties of 1 and 3 were explored by density functional theory.

  10. Modeling actinide chemistry with ASPEN PLUS

    SciTech Connect

    Grigsby, C.O.

    1995-12-31

    When chemical engineers think of chemical processing, they often do not include the US government or the national laboratories as significant participants. Compared to the scale of chemical processing in the chemical process, petrochemical and pharmaceutical industries, the government contribution to chemical processing is not large. However, for the past fifty years, the US government has been, heavily involved in chemical processing of some very specialized materials, in particular, uranium and plutonium for nuclear weapons. Individuals and corporations have paid taxes that, in part have been used to construct and to maintain a series of very expensive laboratories and production facilities throughout the country. Even ignoring the ongoing R & D costs, the price per pound of enriched uranium or of plutonium exceeds that of platinum by a wide margin. Now, with the end of the cold war, the government is decommissioning large numbers of nuclear weapons and cleaning up the legacy of radioactive wastes generated over the last fifty years. It is likely that the costs associated with the build-down and clean-up of the nuclear weapons complex will exceed the investment of the past fifty years of production. Los Alamos National Laboratory occupies a special place in the history of nuclear weapons. The first weapons were designed and assembled at Los Alamos using uranium produced in Oak Ridge, Tennessee or plutonium produced in Richland, Washington. Many of the thermophysical and metallurgical properties of actinide elements have been investigated at Los Alamos. The only plutonium processing facility currently operating in the US is in Los Alamos, and the Laboratory is striving to capture and maintain the uranium processing technology applicable to the post-cold war era. Laboratory researchers are actively involved in developing methods for cleaning up the wastes associated with production of nuclear weapons throughout the US.

  11. Impacts of the removal of shrubs on the physiological and biochemical characteristics of Syntrichia caninervis Mitt: in a temperate desert

    PubMed Central

    Yin, Ben-feng; Zhang, Yuan-ming; Lou, An-ru

    2017-01-01

    Moss crusts play important roles in biological soil crusts biomass and soil surface stabilization. However, because of increasingly intensive human activities, especially grazing, the growth and survival of shrubs are seriously threatened. This study aimed to test whether the presence of shrubs affects the physiological state of the bryophyte Syntrichia caninervis Mitt. in this desert ecosystem. We simulated animal-grazed shrubs at three levels in the Gurbantunggut Desert and compared these simulations to exposed areas, measuring the indicators of growth and stress tolerance exhibited by bryophytes. The results showed that the removal of shrubs significantly decreased chlorophyll fluorescence activity and soluble protein content in S. caninervis, especially under the total shrub removal treatment. The ratio between the total removal of shrubs and other treatments in antioxidative enzymes and in osmotic adjustment substances of S. caninervis exhibited two types of responses. With the exception of malonyldialdehyde (MDA) and superoxide dismutase (SOD), the variables examined fitted as downward parabolic then upward parabolic temporal dynamics. The removal of shrubs is harmful to the survival of S.caninervis. In resource-constrained conditions, SOD is an important antioxidant enzyme that of peroxidase (POD), catalase (CAT) and osmotic adjustment substances, for S. caninervis survival. PMID:28374741

  12. Structural and Functional Characteristics of Natural and Constructed Channels Draining a Reclaimed Mountaintop Removal and Valley Fill Coal Mine

    EPA Science Inventory

    Mountaintop removal and valley fill (MTR/VF) coal mining has altered the landscape of the Central Appalachian region in the USA. Among the changes are large-scale topographic recontouring, burial of headwater streams, and degradation of downstream water quality. The goals of our ...

  13. Structural and functional characteristics of natural and constructed channels draining a reclaimed mountaintop removal and valley fill coal mine

    EPA Science Inventory

    Mountaintop removal and valley fill (MTR/VF) coal mining has altered the landscape of the Central Appalachian region in the United States. The goals of this study were to 1) compare the structure and function of natural and constructed stream channels in forested and MTR/VF catch...

  14. Removal characteristics of As(III) and As(V) from acidic aqueous solution by steel making slag.

    PubMed

    Oh, Chamteut; Rhee, Sungsu; Oh, Myounghak; Park, Junboum

    2012-04-30

    This study focused on the environmental risk of steel making slag itself, arsenic removal mechanism and re-leaching possibility of arsenic to aqueous state after the adsorption. The purpose of the study is to promote the use of steel making slag as a low-cost adsorbent for arsenic in aqueous system. Calcium was easily dissolved out from the slag and become the dominant substance in the leachate. Some of the calcium could form amorphous calcium carbonate in alkaline condition, and arsenic in the aqueous solution would be removed by being co-precipitated with or adsorbed onto the amorphous calcium carbonate. Most of the amorphous calcium carbonate containing arsenic would be bound to amorphous iron oxide of the slag. When the slag was used as an adsorbent for arsenic removal, a little amount of toxic chemicals were leached from the slag itself under pH 0.8 to 13.6. Also, 70-80% of arsenic laden on the slag was bound to amorphous iron oxide which would not easily desorb unless given a reducing and complexing condition. Showing 95-100% removal efficiency near initial pH 2, the slag, therefore, could be used as an appropriate adsorbent for eliminating arsenic in acidic aqueous solution.

  15. Magnetic measurements of the transuranium elements and charge state characterization of actinides in monazite. Progress report

    SciTech Connect

    Huray, P. G.

    1980-01-01

    A micromagnetic susceptometer for the purpose of measuring extremely small sample quantities (on the microgram level) was designed, constructed, and calibrated in previous years. (The 1979 progress report gives details of its operation.) This device has operated without significant downtime in this funding period, and much progress has been made in the magnetic characterization of elements beyond Am in the periodic table. This program has roughly doubled man's knowledge of magnetism in Cm, Bk, and Cf, and includes the only Es magnetic measurements to date. The incorporation of an automatic data collection system in this period has made analysis much more accurate, and has allowed quicker turnaround of compounds and metals for study. Results obtained for the compounds and metals studied this year are summarized. The lanthanide orthophosphates are being investigated as an alternate means of primary containment for high-level actinide wastes. Researchers at the Oak Ridge National Laboratory are involved in preparation of actinide-doped compounds for all of the lanthanide transition series (La through Lu) for a study of leaching characteristics and E.S.R. classification. To aid this study the charge state of /sup 237/Np or /sup 57/Fe has been identified, either in the as-prepared compounds or following radioactive decay of /sup 241/Am via the Moessbauer Effect. The final charge state will be an influential variable in the immobilization characteristics of the waste products stored in this synthetic monazite form. 10 figures, 1 table. (RWR)

  16. Measurement of Actinides in Molybdenum-99 Solution Analytical Procedure

    SciTech Connect

    Soderquist, Chuck Z.; Weaver, Jamie L.

    2015-11-01

    This document is a companion report to a previous report, PNNL 24519, Measurement of Actinides in Molybdenum-99 Solution, A Brief Review of the Literature, August 2015. In this companion report, we report a fast, accurate, newly developed analytical method for measurement of trace alpha-emitting actinide elements in commercial high-activity molybdenum-99 solution. Molybdenum-99 is widely used to produce 99mTc for medical imaging. Because it is used as a radiopharmaceutical, its purity must be proven to be extremely high, particularly for the alpha emitting actinides. The sample of 99Mo solution is measured into a vessel (such as a polyethylene centrifuge tube) and acidified with dilute nitric acid. A gadolinium carrier is added (50 µg). Tracers and spikes are added as necessary. Then the solution is made strongly basic with ammonium hydroxide, which causes the gadolinium carrier to precipitate as hydrous Gd(OH)3. The precipitate of Gd(OH)3 carries all of the actinide elements. The suspension of gadolinium hydroxide is then passed through a membrane filter to make a counting mount suitable for direct alpha spectrometry. The high-activity 99Mo and 99mTc pass through the membrane filter and are separated from the alpha emitters. The gadolinium hydroxide, carrying any trace actinide elements that might be present in the sample, forms a thin, uniform cake on the surface of the membrane filter. The filter cake is first washed with dilute ammonium hydroxide to push the last traces of molybdate through, then with water. The filter is then mounted on a stainless steel counting disk. Finally, the alpha emitting actinide elements are measured by alpha spectrometry.

  17. Selection of actinide chemical analogues for WIPP tests

    SciTech Connect

    Villarreal, R.; Spall, D.

    1995-07-05

    The Department of Energy must demonstrate the effectiveness of the Waste Isolation Pilot Plant (WIPP) as a permanent repository for the disposal of transuranic (TRU) waste. Performance assessments of the WIPP require that estimates of the transportability and outcome of the radionuclides (actinides) be determined from disposal rooms that may become either partially or completely filled with brine. Federal regulations limit the amount of radioactivity that may be unintentionally released to the accessible environment by any mechanism during the post closure phase up to 10,000 years. Thermodynamic models have been developed to predict the concentrations of actinides in the WIPP disposal rooms under various situations and chemical conditions. These models are based on empirical and theoretical projections of the chemistry that might be present in and around the disposal room zone for both near and long-term periods. The actinides that are known to be present in the TRU wastes (and are included in the model) are Th, U, Np, Pu, and Am. Knowledge of the chemistry that might occur in the disposal rooms when the waste comes in contact with brine is important in understanding the range of oxidation states that might be present under different conditions. There is a need to establish the mechanisms and resultant rate of transport, migration, or effective retardation of actinides beyond the disposal rooms to the boundary of the accessible environment. The influence of the bulk salt rock, clay sediments and other geologic matrices on the transport behavior of actinides must be determined to establish the overall performance and capability of the WIPP in isolating waste from the environment. Tests to determine the capabilities of the WIPP geologic formations in retarding actinide species in several projected oxidation states would provide a means to demonstrate the effectiveness of the WIPP in retaining TRU wastes.

  18. Grouped actinide separation in advanced nuclear fuel cycles

    SciTech Connect

    Glatz, J.P.; Malmbeck, R.; Ougier, M.; Soucek, P.; Murakamin, T.; Tsukada, T.; Koyama, T.

    2013-07-01

    Aiming at cleaner waste streams (containing only the short-lived fission products) a partitioning and transmutation (P-T) scheme can significantly reduce the quantities of long-lived radionuclides consigned to waste. Many issues and options are being discussed and studied at present in view of selecting the optimal route. The choice is between individual treatment of the relevant elements and a grouped treatment of all actinides together. In the European Collaborative Project ACSEPT (Actinide recycling by Separation and Transmutation), grouped separation options derived from an aqueous extraction or from a dry pyroprocessing route were extensively investigated. Successful demonstration tests for both systems have been carried out in the frame of this project. The aqueous process called GANEX (Grouped Actinide Extraction) is composed of 2 cycles, a first one to recover the major part of U followed by a co-extraction of Np, Pu, Am, and Cm altogether. The pyro-reprocessing primarily applicable to metallic fuels such as the U-Pu-Zr alloy originally developed by the Argonne National Laboratory (US) in the mid 1980s, has also been applied to the METAPHIX fuels containing up to 5% of minor actinides and 5% of lanthanides (e.g. U{sub 60}Pu{sub 20}-Zr{sub 10}Am{sub 2}Nd{sub 3.5}Y{sub 0.5}Ce{sub 0.5}Gd{sub 0.5}). A grouped actinide separation has been successfully carried out by electrorefining on solid Al cathodes. At present the recovery of the actinides from the alloy formed with Al upon electrodeposition is under investigation, because an efficient P-T cycle requires multiple re-fabrication and re-irradiation. (authors)

  19. Actinide and metal toxicity to prospective bioremediation bacteria.

    PubMed

    Ruggiero, Christy E; Boukhalfa, Hakim; Forsythe, Jennifer H; Lack, Joseph G; Hersman, Larry E; Neu, Mary P

    2005-01-01

    Bacteria may be beneficial for alleviating actinide contaminant migration through processes such as bioaccumulation or metal reduction. However, sites with radioactive contamination often contain multiple additional contaminants, including metals and organic chelators. Bacteria-based bioremediation requires that the microorganism functions in the presence of the target contaminant, as well as other contaminants. Here, we evaluate the toxicity of actinides, metals and chelators to two different bacteria proposed for use in radionuclide bioremediation, Deinococcus radiodurans and Pseudomonas putida, and the toxicity of Pu(VI) to Shewanella putrefaciens. Growth of D. radiodurans was inhibited at metal concentrations ranging from 1.8 microM Cd(II) to 32 mM Fe(III). Growth of P. putida was inhibited at metal concentrations ranging from 50 microM Ni(II) to 240 mM Fe(III). Actinides inhibited growth at mM concentrations: chelated Pu(IV), U(VI) and Np(V) inhibit D. radiodurans growth at 5.2, 2.5 and 2.1 mM respectively. Chelated U(VI) inhibits P. putida growth at 1.7 mM, while 3.6 mM chelated Pu(IV) inhibits growth only slightly. Pu(VI) inhibits S. putrefaciens growth at 6 mM. These results indicate that actinide toxicity is primarily chemical (not radiological), and that radiation resistance does not ensure radionuclide tolerance. This study also shows that Pu is less toxic than U and that actinides are less toxic than other types of metals, which suggests that actinide toxicity will not impede bioremediation using naturally occurring bacteria.

  20. Magnetic exchange coupling in actinide-containing molecules.

    PubMed

    Rinehart, Jeffrey D; Harris, T David; Kozimor, Stosh A; Bartlett, Bart M; Long, Jeffrey R

    2009-04-20

    Recent progress in the assembly of actinide-containing coordination clusters has generated systems in which the first glimpses of magnetic exchange coupling can be recognized. Such systems are of interest owing to the prospects for involving 5f electrons in stronger magnetic exchange than has been observed for electrons in the more contracted 4f orbitals of the lanthanide elements. Here, we survey the actinide-containing molecules thought to exhibit magnetic exchange interactions, including multiuranium, uranium-lanthanide, uranium-transition metal, and uranium-radical species. Interpretation of the magnetic susceptibility data for compounds of this type is complicated by the combination of spin-orbit coupling and ligand-field effects arising for actinide ions. Nevertheless, for systems where analogues featuring diamagnetic replacement components for the non-actinide spin centers can be synthesized, a data subtraction approach can be utilized to probe the presence of exchange coupling. In addition, methods have been developed for employing the resulting data to estimate lower and upper bounds for the exchange constant. Emphasis is placed on evaluation of the linear clusters (cyclam)M[(mu-Cl)U(Me(2)Pz)(4)](2) (M = Co, Ni, Cu, Zn; cyclam = 1,4,8,11-tetraazacyclotetradecane; Me(2)Pz(-) = 3,5-dimethylpyrazolate), for which strong ferromagnetic exchange with 15 cm(-1) < or = J < or = 48 cm(-1) is observed for the Co(II)-containing species. Owing to the modular synthetic approach employed, this system in particular offers numerous opportunities for adjusting the strength of the magnetic exchange coupling and the total number of unpaired electrons. To this end, the prospects of such modularity are discussed through the lens of several new related clusters. Ultimately, it is hoped that this research will be of utility in the development of electronic structure models that successfully describe the magnetic behavior of actinide compounds and will perhaps even lead to new

  1. Analysis methodology and development of a statistical tool for biodistribution data from internal contamination with actinides.

    PubMed

    Lamart, Stephanie; Griffiths, Nina M; Tchitchek, Nicolas; Angulo, Jaime F; Van der Meeren, Anne

    2017-03-01

    The aim of this work was to develop a computational tool that integrates several statistical analysis features for biodistribution data from internal contamination experiments. These data represent actinide levels in biological compartments as a function of time and are derived from activity measurements in tissues and excreta. These experiments aim at assessing the influence of different contamination conditions (e.g. intake route or radioelement) on the biological behavior of the contaminant. The ever increasing number of datasets and diversity of experimental conditions make the handling and analysis of biodistribution data difficult. This work sought to facilitate the statistical analysis of a large number of datasets and the comparison of results from diverse experimental conditions. Functional modules were developed using the open-source programming language R to facilitate specific operations: descriptive statistics, visual comparison, curve fitting, and implementation of biokinetic models. In addition, the structure of the datasets was harmonized using the same table format. Analysis outputs can be written in text files and updated data can be written in the consistent table format. Hence, a data repository is built progressively, which is essential for the optimal use of animal data. Graphical representations can be automatically generated and saved as image files. The resulting computational tool was applied using data derived from wound contamination experiments conducted under different conditions. In facilitating biodistribution data handling and statistical analyses, this computational tool ensures faster analyses and a better reproducibility compared with the use of multiple office software applications. Furthermore, re-analysis of archival data and comparison of data from different sources is made much easier. Hence this tool will help to understand better the influence of contamination characteristics on actinide biokinetics. Our approach can aid

  2. Method for extracting lanthanides and actinides from acid solutions

    DOEpatents

    Horwitz, E. Philip; Kalina, Dale G.; Kaplan, Louis; Mason, George W.

    1985-01-01

    A process for the recovery of actinide and lanthanide values from aqueous acidic solutions with an organic extractant having the formula: ##STR1## where .phi. is phenyl, R.sup.1 is a straight or branched alkyl or alkoxyalkyl containing from 6 to 12 carbon atoms and R.sup.2 is an alkyl containing from 3 to 6 carbon atoms. The process is suitable for the separation of actinide and lanthanide values from fission product values found together in high level nuclear reprocessing waste solutions.

  3. New cubic structure compounds as actinide host phases

    NASA Astrophysics Data System (ADS)

    Stefanovsky, S. V.; Yudintsev, S. V.; Livshits, T. S.

    2010-03-01

    Various compounds with fluorite (cubic zirconia) and fluorite-derived (pyrochlore, zirconolite) structures are considered as promising actinide host phases at immobilization of actinide-bearing nuclear wastes. Recently some new cubic compounds — stannate and stannate-zirconate pyrochlores, murataite and related phases, and actinide-bearing garnet structure compounds were proposed as perspective matrices for complex actinide wastes. Zirconate pyrochlore (ideally Gd2Zr2O7) has excellent radiation resistance and high chemical durability but requires high temperatures (at least 1500 °C) to be produced by hot-pressing from sol-gel derived precursor. Partial Sn4+ substitution for Zr4+ reduces production temperature and the compounds REE2ZrSnO7 may be hot-pressed or cold pressed and sintered at ~1400 °C. Pyrochlore, A2B2O7-x (two-fold elementary fluorite unit cell), and murataite, A3B6C2O20-y (three-fold fluorite unit cell), are end-members of the polysomatic series consisting of the phases whose structures are built from alternating pyrochlore and murataite blocks (nano-sized modules) with seven- (2C/3C/2C), five- (2C/3C), eight- (3C/2C/3C) and three-fold (3C — murataite) fluorite unit cells. Actinide content in this series reduces in the row: 2C (pyrochlore) > 7C > 5C > 8C > 3C (murataite). Due to congruent melting murataite-based ceramics may be produced by melting and the firstly segregated phase at melt crystallization is that with the highest fraction of the pyrochlore modules in its structure. The melts containing up to 10 wt. % AnO2 (An = Th, U, Np, Pu) or REE/An fraction of HLW form at crystallization zoned grains composed sequentially of the 5C → 8C → 3C phases with the highest actinide concentration in the core and the lowest — in the rim of the grains. Radiation resistance of the "murataite" is comparable to titanate pyrochlores. One more promising actinide hosts are ferrites with garnet structure. The matrices containing sometime complex fluorite

  4. Analogue Study of Actinide Transport at Sites in Russia

    SciTech Connect

    Novikov, A P; Simmons, A M; Halsey, W G

    2003-02-12

    The U. S. Department of Energy (DOE) and the Russian Academy of Sciences (RAS) are engaged in a three-year cooperative study to observe the behavior of actinides in the natural environment at selected disposal sites and/or contamination sites in Russia. The purpose is to develop experimental data and models for actinide speciation, mobilization and transport processes in support of geologic repository design, safety and performance analyses. Currently at the mid-point of the study, the accomplishments to date include: evaluation of existing data and data needs, site screening and selection, initial data acquisition, and development of preliminary conceptual models.

  5. SOLVENT EXTRACTION PROCESS FOR SEPARATING ACTINIDE AND LANTHANIDE METAL VALUES

    DOEpatents

    Hildebrandt, R.A.; Hyman, H.H.; Vogler, S.

    1962-08-14

    A process of countercurrently extracting an aqueous mineral acid feed solution for the separation of actinides from lanthanides dissolved therern is described. The feed solution is made acid-defrcient with alkali metal hydroxide prior to.contact with acid extractant; during extraction, however, acid is transferred from organic to aqueous solution and the aqueous solution gradually becomes acid. The acid-deficient phase ' of the process promotes the extraction of the actinides, while the latter acid phase'' of the process improves retention of the lanthanides in the aqueous solution. This provides for an improved separation. (AEC)

  6. Physics studies of higher actinide consumption in an LMR

    SciTech Connect

    Hill, R.N.; Wade, D.C.; Fujita, E.K.; Khalil, H.S.

    1990-01-01

    The core physics aspects of the transuranic burning potential of the Integral Fast Reactor (IFR) are assessed. The actinide behavior in fissile self-sufficient IFR closed cycles of 1200 MWt size is characterized, and the transuranic isotopics and risk potential of the working inventory are compared to those from a once-through LWR. The core neutronic performance effects of rare-earth impurities present in the recycled fuel are addressed. Fuel cycle strategies for burning transuranics from an external source are discussed, and specialized actinide burner designs are described. 4 refs., 4 figs., 3 tabs.

  7. Actinide geochemistry: from the molecular level to the real system.

    PubMed

    Geckeis, Horst; Rabung, Thomas

    2008-12-12

    Geochemical processes leading to either mobilization or retention of radionuclides in an aquifer system are significantly influenced by their interaction with rock, sediment and colloid surfaces. Therefore, a sound safety assessment of nuclear waste disposal requires the elucidation and quantification of those processes. State-of-the-art analytical techniques as e.g. laser- and X-ray spectroscopy are increasingly applied to study solid-liquid interface reactions to obtain molecular level speciation insight. We have studied the sorption of trivalent lanthanides and actinides onto aluminium oxides, hydroxides and purified clay minerals by the time-resolved laser fluorescence spectroscopy and X-ray-absorption spectroscopy. Chemical constitution and structure of surface bound actinides are proposed based on spectroscopic information. Open questions still remain with regard to the exact nature of mineral surface ligands and the mineral/water interface. Similarities of spectroscopic data obtained for M(III) sorbed onto gamma-alumina, and clay minerals suggest the formation of very comparable inner-sphere surface complexes such as S-O-An(III)(OH)x(2-x)(H2O)5-x at pH > 5. Those speciation data are found consistent with those predicted by surface complexation modelling. The applicability of data obtained for pure mineral phases to actinide sorption onto heterogeneously composed natural clay rock is examined by experiments and by geochemical modelling. Good agreement of experiment and model calculations is found for U(VI) and trivalent actinide/lanthanide sorption to natural clay rock. The agreement of spectroscopy, geochemical modelling and batch experiments with natural rock samples and purified minerals increases the reliability in model predictions. The assessment of colloid borne actinide migration observed in various laboratory and field studies calls for detailed information on actinide-colloid interaction. Kinetic stabilization of colloid bound actinides can be due

  8. Role of fringing field on the electrical characteristics of metal-oxide-semiconductor capacitors with co-planar and edge-removed oxides

    NASA Astrophysics Data System (ADS)

    Yang, Chang-Feng; Hwu, Jenn-Gwo

    2016-12-01

    Due to the simplicity of the fabrication process, the ultra-thin oxide metal-oxide-semiconductor capacitors (MOSCAPs) can be a promising device for sensing, memory, and transconductance applications. The investigation of the fundamental electrical characteristics of ultra-thin oxide MOSCAPs is still of importance. In this work, the influence of the removal of the surrounded gate oxide was studied to know the role of fringing field. For edge-removed oxide, the tunneling saturation current shows no oxide thickness dependency and exhibits a low current level of 9.4×10-11 at 2V (dox=2.3 nm). Also, its deep depletion occurs earlier when biasing. In contrast, for the device without oxide removing, i.e., co-planar oxide, the saturation current is strongly related to the oxide thickness and exhibits a high current level of 3.5×10-6 at 2V (dox=2.3 nm) due to regular oxide voltage drop modulation effect on effective Schottky barrier height. For the thick oxide of 4.2 nm the inversion capacitances are frequency dependant for CP-OX but are independent for ER-OX MOSCAPs. These characteristics are mainly caused by the different fringing fields and the defect densities at device edge between two structures.

  9. Thermodynamic constants for actinide oxides and oxyhydroxides relevant to actinide volatility calculations for thermal oxidation processes

    SciTech Connect

    Ebbinghaus, B.B.; Krikorian, O.H.

    1993-10-27

    The purpose of this report is to provide input of thermodynamic data on actinide volatilities to EERC for use in their computer code for modeling of metal volatilities in incinerators. It is also anticipated that the data may be documented later in an EPA sponsored ``Metals Bible.`` It should be noted that only upper limits for the volatility of PuO{sub 2}(s) due to PuO{sub 3}(g) and PuO{sub 2}(OH){sub 2}(g) and the volatility of AmO{sub 2} in PuO{sub 2}(s) due to AmO{sub 3}(g) and AmO{sub 2}(OH){sub 2}(g) could be set. The data on the americium vapor species are intended for calculations where AmO{sub 2} is present as a solid solution in PuO{sub 2}(s).

  10. [Identification and Nitrogen Removal Characteristics of a Heterotrophic Nitrification-Aerobic Denitrification Strain Isolated from Marine Environment].

    PubMed

    Sun, Qing-hua; Yu, De-shuang; Zhang, Pei-yu; Lin, Xue-zheng; Li, Jin

    2016-02-15

    A heterotrophic nitrification-aerobic denitrification strain named y5 was isolated from marine environment by traditional microbial isolation method using seawater as medium. It was identified as Klebsiella sp. based on the morphological, physiological and 16S rRNA sequence analysis. The experiment results showed that the optimal carbon resource was sodium citrate; the optimal pH was 7.0; and the optimal C/N was 17. The strain could use NH4Cl, NaNO2 and KNO3 as sole nitrogen source, and the removal efficiencies were77.07%, 64.14% and 100% after 36 hours, respectively. The removal efficiency reached 100% after 36 hours in the coexistence of NH4Cl, NaNO2 and KNO3. The results showed that the strain y5 had independent and efficient heterotrophic nitrification and aerobic denitrification activities in high salt wastewater.

  11. Literature review of intrinsic actinide colloids related to spent fuel waste package release rates

    SciTech Connect

    Zhao, P.; Steward, S.A.

    1997-01-01

    Existence of actinide colloids provides an important mechanism in the migration of radionuclides and will be important in performance of a geologic repository for high-level nuclear waste. Actinide colloids have been formed during long-term unsaturated dissolution of spent fuel by groundwater. This article summarizes a literature search of actinide colloids. This report emphasizes the formation of intrinsic actinide colloids, because they would have the opportunity to form soon after groundwater contact with the spent fuel and before actinide-bearing groundwater reaches the surrounding geologic formations.

  12. High Precision Isotopic Analysis of Actinide Bearing Materials: Performance of a New Generation of Purpose Built Actinide Multi-Collector ICPMS Instruments

    SciTech Connect

    Eiden, Gregory C.; Duffin, Andrew M.; Liezers, Martin; Ward, Jesse D.; Robinson, John W.; Hart, Garret L.; Pratt, Sandra H.; Springer, Kellen WE; Carman, April J.; Duckworth, Douglas C.

    2014-11-14

    Recently, a new class of multi-collector inductively coupled plasma mass spectrometers (MC-ICPMS) has been introduced commercially that includes detector arrays purpose built for actinide measurements. These detector arrays significantly enhance the data quality possible for applications encountered in nuclear forensics. Two such instruments are described in this paper, the NeptunePlusTM, developed by Thermo-Fisher (Bremen, Germany), and the NuPlasma2, developed by Nu Instruments (Wrexham, UK). Research results are presented that have been obtained by the authors using the first commercial NeptunePlusTM. This paper also presents performance characteristics and results for traditional liquid introduction, including a means for ultra-trace detection via electrochemical separation prior to solution nebulization, as well as solid sample introduction with femtosecond-laser ablation. We also discuss the advantages and limitations of the current systems for detection of the transient signals associated with these two methods for introducing sample into the plasma.

  13. Nuclear energy waste-space transportation and removal

    NASA Technical Reports Server (NTRS)

    Burns, R. E.

    1975-01-01

    A method for utilizing the decay heat of actinide wastes to power an electric thrust vehicle is proposed. The vehicle, launched by shuttle to earth orbit and to earth escape by a tug, obtains electrical power from the actinide waste heat by thermionic converters. The heavy gamma ray and neutron shielding which is necessary as a safety feature is removed in orbit and returned to earth for reuse. The problems associated with safety are dealt with in depth. A method for eliminating fission wastes via chemical propulsion is briefly discussed.

  14. The effect of metal oxides on the characteristic and activation energy of sulfur removal reactivity of Ca(OH){sub 2}

    SciTech Connect

    Chen Yafei; Gao Xiang; Luo Zhongyang

    1997-07-01

    This study deals with the characteristic of sulfur removal reactivity of calcium hydroxide, Ca(OH){sub 2}, and the influence of metal oxides, e.g., ZnO, Fe{sub 2}O{sub 3}, MnO{sub 2}, V{sub 2}O{sub 5}, by examining the change in activation energy with different weight ratio of such additives in Ca(OH){sub 2}. Experimental results suggest that reaction rate decrease in exponential function, the addition of metal oxides may catalyze the sulfur removal reactivity of Ca(OH){sub 2}, and this catalytic effect becomes more pronounced with increasing metal oxides weight ratio. At the same time, ZnO and V{sub 2}O{sub 5} shows stronger catalytic effect compared with the other two kinds of metal oxides.

  15. Detection limits for actinides in a monochromatic, wavelength-dispersive x-ray fluorescence instrument

    SciTech Connect

    Collins, Michael L; Havrilla, George J

    2009-01-01

    Recent developments in x-ray optics have made it possible to examine the L x-rays of actinides using doubly-curved crystals in a bench-top device. A doubly-curved crystal (DCC) acts as a focusing monochromatic filter for polychromatic x-rays. A Monochromatic, Wavelength-Dispersive X-Ray Fluorescence (MWDXRF) instrument that uses DCCs to measure Cm and Pu in reprocessing plant liquors was proposed in 2007 by the authors at Los Alamos National Laboratory. A prototype design of this MWDXRF instrument was developed in collaboration with X-ray Optical Systems Inc. (XOS), of East Greenbush, New York. In the MWDXRF instrument, x-rays from a Rhodium-anode x-ray tube are passed through a primary DCC to produce a monochromatic beam of 20.2-keV photons. This beam is focused on a specimen that may contain actinides. The 20.2-keV interrogating beam is just above the L3 edge of Californium; each actinide (with Z = 90 to 98) present in the specimen emits characteristic L x-rays as the result of L3-shell vacancies. In the LANL-XOS prototype MWDXRf, these x-rays enter a secondary DCC optic that preferentially passes 14.961-keV photons, corresponding to the L-alpha-1 x-ray peak of Curium. In the present stage of experimentation, Curium-bearing specimens have not been analyzed with the prototype MWDXRF instrument. Surrogate materials for Curium include Rubidium, which has a K-beta-l x-ray at 14.961 keV, and Yttrium, which has a K-alpha-1 x-ray at 14.958 keV. In this paper, the lower limit of detection for Curium in the LANL-XOS prototype MWDXRF instrument is estimated. The basis for this estimate is described, including a description of computational models and benchmarking techniques used. Detection limits for other actinides are considered, as well as future safeguards applications for MWDXRF instrumentation.

  16. Enhancing BWR Proliferation Resistance Fuel with Minor Actinides

    SciTech Connect

    Gray S. Chang

    2008-07-01

    reactivity control of the systems into which they are incorporated. In the study, a typical boiling water reactor (BWR) fuel unit lattice cell model with UO2 fuel pins will be used to investigate the effectiveness of minor actinide reduction approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance in the intermediate term goal for future nuclear energy systems. To account for the water coolant density variation from the bottom (0.76 g/cm3) to the top (0.35 g/cm3) of the core, the axial coolant channel and fuel pin were divided to 24 nodes. The MA transmutation characteristics at different elevations were compared and their impact on neutronics criticality discussed. We concluded that the concept of MARA, which involves the use of transuranic nuclides (237Np and/or 241Am), significantly increases the 238Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in atoms for peace and the intermediate term of nuclear energy rennaissance.

  17. Method for recovery of actinides from actinide-bearing scrap and waste nuclear material using O/sub 2/F/sub 2/

    DOEpatents

    Asprey, L.B.; Eller, P.G.

    1984-09-12

    Method for recovery of actinides from nuclear waste material containing sintered and other oxides thereof and from scrap materials containing the metal actinides using O/sub 2/F/sub 2/ to generate the hexafluorides of the actinides present therein. The fluorinating agent, O/sub 2/F/sub 2/, has been observed to perform the above-described tasks at sufficiently low temperatures that there is virtually no damage to the containment vessels. Moreover, the resulting actinide hexafluorides are not detroyed by high temperature reactions with the walls of the reaction vessel. Dioxygen difluoride is readily prepared, stored and transferred to the place of reaction.

  18. Selective Separation of Trivalent Actinides from Lanthanides by Aqueous Processing with Introduction of Soft Donor Atoms

    SciTech Connect

    Kenneth L. Nash; Sue B. Clark; Gregg Lumetta

    2009-09-23

    With increased application of MOX fuels and longer burnup times for conventional fuels, higher concentrations of the transplutonium actinides Am and Cm (and even heavier species like Bk and Cf) will be produced. The half-lives of the Am isotopes are significantly longer than those of the most important long-lived, high specific activity lanthanides or the most common Cm, Bk and Cf isotopes, thus the greatest concern as regards long-term radiotoxicity. With the removal and transmutation of Am isotopes, radiation levels of high level wastes are reduced to near uranium mineral levels within less than 1000 years as opposed to the time-fram if they remain in the wastes.

  19. Long-term impact of anaerobic reaction time on the performance and granular characteristics of granular denitrifying biological phosphorus removal systems.

    PubMed

    Wang, Yayi; Guo, Gang; Wang, Hong; Stephenson, Tom; Guo, Jianhua; Ye, Liu

    2013-09-15

    Removal of nitrogen and phosphorus (P) from wastewater is successfully and widely practiced in systems employing both granular sludge technology and enhanced biological P removal (EBPR) processes; however, the key parameter, anaerobic reaction time (AnRT), has not been thoroughly investigated. Successful EBPR is highly dependent on an appropriate AnRT, which induces carbon and polyphosphate metabolism by phosphorus accumulating organisms (PAOs). Therefore, the long-term impact of AnRT on denitrifying P removal performance and granular characteristics was investigated in three identical granular sludge sequencing batch reactors with AnRTs of 90 (R1), 120 (R2) and 150 min (R3). The microbial community structures and anaerobic stoichiometric parameters related to various AnRTs were monitored over time. Free nitrite acid (FNA) accumulation (e.g., 0.0008-0.0016 mg HNO2-N/L) occurred frequently owing to incomplete denitrification in the adaptation period, especially in R3, which influenced the anaerobic/anoxic intracellular intermediate metabolites and activities of intracellular enzymes negatively, resulting in lower levels of poly-P and reduced activity of polyphosphate kinase. As a result, the Accumulibacter-PAOs population decreased from 51 ± 2.5% to 43 ± 2.1% when AnRT was extended from 90 to 150 min, leading to decreased denitrifying P removal performance. Additionally, frequent exposure of microorganisms to the FNA accumulation and anaerobic endogenous conditions in excess AnRT cases (e.g., 150 min) stimulated increased extracellular polymeric substances (EPS) production by microorganisms, resulting in enhanced granular formation and larger granules (size of 0.6-1.2 mm), but decreasing anaerobic PHA synthesis and glycogen hydrolysis. Phosphorus removal capacity was mediated to some extent by EPS adsorption in granular sludge systems that possessed more EPS, longer AnRT and relatively higher GAOs.

  20. REVIEW OF EXPERIMENTAL STUDIES INVESTIGATING THE RATE OF STRONTIUM AND ACTINIDE ADSORPTION BY MONOSODIUM TITANATE

    SciTech Connect

    Hobbs, D.

    2010-10-01

    A number of laboratory studies have been conducted to determine the influence of mixing and mixing intensity, solution ionic strength, initial sorbate concentrations, temperature, and monosodium titanate (MST) concentration on the rates of sorbate removal by MST in high-level nuclear waste solutions. Of these parameters, initial sorbate concentrations, ionic strength, and MST concentration have the greater impact on sorbate removal rates. The lack of a significant influence of mixing and mixing intensity on sorbate removal rates indicates that bulk solution transport is not the rate controlling step in the removal of strontium and actinides over the range of conditions and laboratory-scales investigated. However, bulk solution transport may be a significant parameter upon use of MST in a 1.3 million-gallon waste tank such as that planned for the Small Column Ion Exchange (SCIX) program. Thus, Savannah River National Laboratory (SRNL) recommends completing the experiments in progress to determine if mixing intensity influences sorption rates under conditions appropriate for this program. Adsorption models have been developed from these experimental studies that allow prediction of strontium (Sr), plutonium (Pu), neptunium (Np) and uranium (U) concentrations as a function of contact time with MST. Fairly good agreement has been observed between the predicted and measured sorbate concentrations in the laboratory-scale experiments.

  1. Chemistry of the heaviest actinides: fermium, mendelevium, nobelium, and lawrencium

    SciTech Connect

    Hulet, E.K.

    1980-01-01

    Conclusions regarding these shifts toward greater stabilization of 5f orbitals with increasing atomic number are mainly supported by the appearance of the divalent oxidation state well before the end of the actinide series and the predominance of the divalent state in the next to last element in the series. These conclusions and the underlying experimental evidence are the main subject of this review.

  2. Colloid-borne forms of tetravalent actinides: a brief review.

    PubMed

    Zänker, Harald; Hennig, Christoph

    2014-02-01

    Tetravalent actinides, An(IV), are usually assumed to be little mobile in near-neutral environmental waters because of their low solubility. However, there are certain geochemical scenarios during which mobilization of An(IV) in a colloid-borne (waterborne) form cannot be ruled out. A compilation of colloid-borne forms of tetravalent actinides described so far for laboratory experiments together with several examples of An(IV) colloids observed in field experiments and real-world scenarios are given. They are intended to be a knowledge base and a tool for those who have to interpret actinide behavior under environmental conditions. Synthetic colloids containing structural An(IV) and synthetic colloids carrying adsorbed An(IV) are considered. Their behavior is compared with the behavior of An(IV) colloids observed after the intentional or unintentional release of actinides into the environment. A list of knowledge gaps as to the behavior of An(IV) colloids is provided and items which need further research are highlighted.

  3. Experimental Evaluation of Actinide Transport in a Fractured Granodiorite

    SciTech Connect

    Dittrich, Timothy M.; Reimus, Paul W.

    2015-03-16

    The objective of this study was to demonstrate and evaluate new experimental methods for quantifying the potential for actinide transport in deep fractured crystalline rock formations. We selected a fractured granodiorite at the Grimsel Test Site (GTS) in Switzerland as a model system because field experiments have already been conducted with uranium and additional field experiments using other actinides are planned at the site. Thus, working on this system provides a unique opportunity to compare lab experiment results with fieldscale observations. Rock cores drilled from the GTS were shipped to Los Alamos National Laboratory, characterized by x-ray diffraction and microscopy, and used in batch sorption and column breakthrough experiments. Solutions with pH 6.8 and 8.8 were tested. Solutions were switched to radionuclide-free synthetic Grimsel groundwater after near-steady actinide/colloid breakthrough occurred in column experiments. We are currently evaluating actinide adsorption/desorption rates as a function of water chemistry (initial focus on pH), with future testing planned to evaluate the influence of carbonate concentrations, flow rates, and mineralogy in solutions and suspensions with bentonite colloids. (auth)

  4. Synthesis and characterization of a tetrathiafulvalene-salphen actinide complex.

    PubMed

    Bejger, Christopher; Tian, Yong-Hui; Barker, Beau J; Boland, Kevin S; Scott, Brian L; Batista, Enrique R; Kozimor, Stosh A; Sessler, Jonathan L

    2013-05-21

    A new tetrathiafulvalene-salphen uranyl complex has been prepared. The system was designed to study the electronic coupling between actinides and a redox active ligand framework. Theoretical and experimental methods--including DFT calculations, single crystal X-ray analysis, cyclic voltammetry, NMR and IR spectroscopies--were used to characterize this new uranyl complex.

  5. Removal characteristics of PCDD/Fs by the dual bag filter system of a fly ash treatment plant.

    PubMed

    Lin, Wen-Yinn; Wang, Lin-Chi; Wang, Ya-Fen; Li, Hsing-Wang; Chang-Chien, Guo-Ping

    2008-05-30

    In this study, a dual bag filter system was established to decrease the concentration of polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/Fs) in the stack flue gases of a fly ash treatment plant, which retained zinc from the fly ash of electric arc furnaces. Compared to the original single bag filter system with activated carbon injection (ACI) of 40 kg h(-1), the PCDD/F concentrations in the stack flue gas after the plant was equipped with the dual bag filter system dropped enormously from 3.38-7.73 ng I-TEQNm(-3) to 0.03 ng I-TEQNm(-3), and the total PCDD/F I-TEQ removal efficiency increased from 97.6% to 99.3% with ACI of 16 kg h(-1), that is, about 40% of the original AC usage. The AC utilization efficiency (0.560 mg I-TEQ absorbed kg ACI(-1)) of the dual bag filter system (AC: 16 kg h(-1)) was estimated about three times higher than that (0.192 mg I-TEQ absorbed kg ACI(-1)) of single bag filter system with ACI (40 kg h(-1)). The reason is that the particulate phase PCDD/Fs and some gas phase PCDD/Fs (captured by the recycled AC/ash mixture) were removed first by the first bag filter, and the rest of the gas phase PCDD/Fs were able to be adsorbed more completely by the AC/ash mixture due to a lower fly ash load, and then were removed by the second bag filter.

  6. [Research progress in microbiological characteristics in combined N2 removal process by partial nitrification and anaerobic ammonium oxidation].

    PubMed

    Zhao, Zhi-Rui; Hou, Yan-Lin

    2014-07-01

    Partial nitrification and anaerobic ammonium oxidation is a very significant biological nitrogen removal technology for saving energy and carbon sources. The development of this technology and the community ecology of ammonia-oxidizing bacterium (AOB) and anaerobic ammonium- oxidizing bacteria (ANAOB) using molecular biological methods have attracted growing attention. The paper reviewed the technological mechanism and the effects of key factors such as temperature, pH, dissolve oxygen and free ammonia on the distribution of AOB and ANAOB. It was also introduced that the populations of AOB and ANAOB species and their abundance in various environments. At the end, some suggestions were provided for the development of this technology in the future.

  7. FEASIBILITY OF RECYCLING PLUTONIUM AND MINOR ACTINIDES IN LIGHT WATER REACTORS USING HYDRIDE FUEL

    SciTech Connect

    Greenspan, Ehud; Todreas, Neil; Taiwo, Temitope

    2009-03-10

    The objective of this DOE NERI program sponsored project was to assess the feasibility of improving the plutonium (Pu) and minor actinide (MA) recycling capabilities of pressurized water reactors (PWRs) by using hydride instead of oxide fuels. There are four general parts to this assessment: 1) Identifying promising hydride fuel assembly designs for recycling Pu and MAs in PWRs 2) Performing a comprehensive systems analysis that compares the fuel cycle characteristics of Pu and MA recycling in PWRs using the promising hydride fuel assembly designs identified in Part 1 versus using oxide fuel assembly designs 3) Conducting a safety analysis to assess the likelihood of licensing hydride fuel assembly designs 4) Assessing the compatibility of hydride fuel with cladding materials and water under typical PWR operating conditions Hydride fuel was found to offer promising transmutation characteristics and is recommended for further examination as a possible preferred option for recycling plutonium in PWRs.

  8. Mechanical environmental transport of actinides and ¹³⁷Cs from an arid radioactive waste disposal site.

    PubMed

    Snow, Mathew S; Clark, Sue B; Morrison, Samuel S; Watrous, Matthew G; Olson, John E; Snyder, Darin C

    2015-10-01

    Aeolian and pluvial processes represent important mechanisms for the movement of actinides and fission products at the Earth's surface. Soil samples taken in the early 1970's near a Department of Energy radioactive waste disposal site (the Subsurface Disposal Area, SDA, located in southeastern Idaho) provide a case study for studying the mechanisms and characteristics of environmental actinide and (137)Cs transport in an arid environment. Multi-component mixing models suggest actinide contamination within 2.5 km of the SDA can be described by mixing between 2 distinct SDA end members and regional nuclear weapons fallout. The absence of chemical fractionation between (241)Am and (239+240)Pu with depth for samples beyond the northeastern corner and lack of (241)Am in-growth over time (due to (241)Pu decay) suggest mechanical transport and mixing of discrete contaminated particles under arid conditions. Occasional samples northeast of the SDA (the direction of the prevailing winds) contain anomalously high concentrations of Pu with (240)Pu/(239)Pu isotopic ratios statistically identical to those in the northeastern corner. Taken together, these data suggest flooding resulted in mechanical transport of contaminated particles into the area between the SDA and a flood containment dike in the northeastern corner, following which subsequent contamination spreading in the northeastern direction resulted from wind transport of discrete particles.

  9. Pumice Characteristics and Their Utilization on the Synthesis of Mesoporous Minerals and on the Removal of Heavy Metals

    PubMed Central

    Ismail, A. I. M.; El-Shafey, O. I.; Amr, M. H. A.; El-Maghraby, M. S.

    2014-01-01

    Wastewater treatment of some heavy metals was carried out by synthetic zeolite P1, which was prepared by alkaline hydrothermal treatment of the pumice. Both of the pumice raw materials and synthetic zeolite were investigated for their chemical phase composition, physical properties, and microstructure. The adsorption behavior of Na-zeolite P1 with respect to Co+2, Cu+2, Fe+2, and Cd+2 has been studied to be applied in the industrial wastewater treatment. Metal removal was investigated using synthetic solutions at different ions concentrations, time, and Na-P1 zeolite doses as well as constant temperature and pH. It is concluded that the optimum conditions for synthesis of highly active Na-P1 zeolite from natural pumice raw material are one molar NaOH concentration, temperature at 80°C, and one week as a crystallization time. In addition to the effect of time and zeolite dose as well as the ion concentration of the reaction efficiency for metals removals are recorded. PMID:27355006

  10. Pumice Characteristics and Their Utilization on the Synthesis of Mesoporous Minerals and on the Removal of Heavy Metals.

    PubMed

    Ismail, A I M; El-Shafey, O I; Amr, M H A; El-Maghraby, M S

    2014-01-01

    Wastewater treatment of some heavy metals was carried out by synthetic zeolite P1, which was prepared by alkaline hydrothermal treatment of the pumice. Both of the pumice raw materials and synthetic zeolite were investigated for their chemical phase composition, physical properties, and microstructure. The adsorption behavior of Na-zeolite P1 with respect to Co(+2), Cu(+2), Fe(+2), and Cd(+2) has been studied to be applied in the industrial wastewater treatment. Metal removal was investigated using synthetic solutions at different ions concentrations, time, and Na-P1 zeolite doses as well as constant temperature and pH. It is concluded that the optimum conditions for synthesis of highly active Na-P1 zeolite from natural pumice raw material are one molar NaOH concentration, temperature at 80°C, and one week as a crystallization time. In addition to the effect of time and zeolite dose as well as the ion concentration of the reaction efficiency for metals removals are recorded.

  11. Adsorption Characteristics of Different Adsorbents and Iron(III) Salt for Removing As(V) from Water

    PubMed Central

    Ćurko, Josip; Matošić, Marin; Crnek, Vlado; Stulić, Višnja

    2016-01-01

    Summary The aim of this study is to determine the adsorption performance of three types of adsorbents for removal of As(V) from water: Bayoxide® E33 (granular iron(III) oxide), Titansorb® (granular titanium oxide) and a suspension of precipitated iron(III) hydroxide. Results of As(V) adsorption stoichiometry of two commercial adsorbents and precipitated iron(III) hydroxide in tap and demineralized water were fitted to Freundlich and Langmuir adsorption isotherm equations, from which adsorption constants and adsorption capacity were calculated. The separation factor RL for the three adsorbents ranged from 0.04 to 0.61, indicating effective adsorption. Precipitated iron(III) hydroxide had the greatest, while Titansorb had the lowest capacity to adsorb As(V). Comparison of adsorption from tap or demineralized water showed that Bayoxide and precipitated iron(III) hydroxide had higher adsorption capacity in demineralized water, whereas Titansorb showed a slightly higher capacity in tap water. These results provide mechanistic insights into how commonly used adsorbents remove As(V) from water. PMID:27904416

  12. The INE-Beamline for actinide science at ANKA

    SciTech Connect

    Rothe, J.; Dardenne, K.; Denecke, M. A.; Kienzler, B.; Loeble, M.; Metz, V.; Steppert, M.; Vitova, T.; Geckeis, H.; Butorin, S.; Seibert, A.; Walther, C.

    2012-04-15

    Since its inauguration in 2005, the INE-Beamline for actinide research at the synchrotron source ANKA (KIT North Campus) provides dedicated instrumentation for x-ray spectroscopic characterization of actinide samples and other radioactive materials. R and D work at the beamline focuses on various aspects of nuclear waste disposal within INE's mission to provide the scientific basis for assessing long-term safety of a final nuclear waste repository. The INE-Beamline is accessible for the actinide and radiochemistry community through the ANKA proposal system and the European Union Integrated Infrastructure Initiative ACTINET-I3. Experiments with activities up to 1 x 10{sup +6} times the European exemption limit are feasible within a safe but flexible containment concept. Measurements with monochromatic radiation are performed at photon energies varying between {approx}2.1 keV (P K-edge) and {approx}25 keV (Pd K-edge), including the lanthanide L-edges and the actinide M- and L3-edges up to Cf. The close proximity of the INE-Beamline to INE controlled area labs offers infrastructure unique in Europe for the spectroscopic and microscopic characterization of actinide samples. The modular beamline design enables sufficient flexibility to adapt sample environments and detection systems to many scientific questions. The well-established bulk techniques x-ray absorption fine structure (XAFS) spectroscopy in transmission and fluorescence mode have been augmented by advanced methods using a microfocused beam, including (confocal) XAFS/x-ray fluorescence detection and a combination of (micro-)XAFS and (micro-)x-ray diffraction. Additional instrumentation for high energy-resolution x-ray emission spectroscopy has been successfully developed and tested.

  13. Lauriston S. Taylor Lecture: the quest for therapeutic actinide chelators.

    PubMed

    Durbin, Patricia W

    2008-11-01

    All of the actinides are radioactive. Taken into the body, they damage and induce cancer in bone and liver, and in the lungs if inhaled, and U(VI) is a chemical kidney poison. Containment of radionuclides is fundamental to radiation protection, but if it is breached accidentally or deliberately, decontamination of exposed persons is needed to reduce the consequences of radionuclide intake. The only known way to reduce the health risks of internally deposited actinides is to accelerate their excretion with chelating agents. Ethylendiaminetetraacetic acid (EDTA) and diethylenetriaminepentaacetic acid (DTPA) were introduced in the 1950's. DTPA is now clinically accepted, but its oral activity is low, it must be injected as a Ca(II) or Zn(II) chelate to avoid toxicity, and it is structurally unsuitable for chelating U(VI) or Np(V). Actinide penetration into the mammalian iron transport and storage systems suggested that actinide ions would form stable complexes with the Fe(III)-binding units found in potent selective natural iron chelators (siderophores). Testing of that biomimetic approach began in the late 1970's with the design, production, and assessment for in vivo Pu(IV) chelation of synthetic multidentate ligands based on the backbone structures and Fe(III)-binding groups of siderophores. New efficacious actinide chelators have emerged from that program, in particular, octadentate 3,4,3-LI(1,2-HOPO) and tetradentate 5-LIO(Me-3,2-HOPO) have potential for clinical acceptance. Both are much more effective than CaNa3-DTPA for decorporation of Pu(IV), Am(III), U(VI), and Np(IV,V), they are orally active, and toxicity is acceptably low at effective dosage.

  14. Photocatalytic activity of titanium dioxide nanoparticle coatings applied on autoclaved aerated concrete: effect of weathering on coating physical characteristics and gaseous toluene removal.

    PubMed

    Maury-Ramirez, Anibal; Demeestere, Kristof; De Belie, Nele

    2012-04-15

    Autoclaved aerated concrete has been coated by TiO(2) nanoparticles through a dip-coating (DC) and a novel vacuum saturation (VS) method to investigate the weathering resistance and gaseous toluene removal potential of both coating types. The effect of intensive weathering - corresponding to a period of about 25 years - on the coating characteristics was studied in terms of TiO(2) content, coating thickness and color changes. Toluene removal was investigated in a lab-scale flow-through photoreactor at 24°C and 52% relative humidity, and results obtained immediately after application of the coatings and after two weathering stages were compared. Weathering of the DC and VS coated samples resulted into a decrease of the coating layer thickness of more than 98%, confirmed by a decline in TiO(2) content by more than 99% and 93%, respectively. Surprisingly, toluene removal efficiencies before and after weathering kept constant at about 95% for both coating types, corresponding to an elimination rate of 60-70 mg/(m(2)h) at an initial toluene concentration of 15 ppm(v) and a gas residence time of 3 min. Increasing the toluene load by applying higher toluene inlet concentrations (up to 35 ppm(v)) and lower gas residence times (1 min) did decrease the toluene removal efficiency to 32-41%, but elimination rates increased up to 214 mg/(m(2)h), being a factor of 1.6-4.5 times higher than reported in recent work.

  15. Operational characteristics of efficient co-removal of H2S and NH3 in a horizontal biotrickling filter using exhausted carbon.

    PubMed

    Jiang, Xia; Tay, Joo Hwa

    2010-04-15

    Odorous H(2)S and NH(3) gases were effectively biodegraded in a horizontal biotrickling filter (HBTF) packed with H(2)S-exhausted carbon. During the process, the operational characteristics including the distribution of degradation products, biomass accumulation and biological activity, carbon surface characteristics and pressure drop were investigated. The results show that the content of biodegradation products on carbon was low, i.e. 0.9-2.8 wt% S and 0.3-1.0 wt% N. The low content benefited the stable operation of the HBTF, due to preventing a toxic concentration of degradation products on packing bed over a long-term operation. The biomass was distributed evenly along the HBTF . This avoided the problems of bed clogging and activity loss. On the other hand, the deteriorated performance was observed due to the biomass accumulation over a long-term operation. Carbon surface characteristics in the HBTF remained almost unchanged. pH values of carbon were neutral and micropore structure of carbon remained relatively stable. In addition, the pressure drop in the HBTF was very low. These operational characteristics of the HBTF system significantly contributed to efficient co-removal of H(2)S and NH(3) in the HBTF over a long-term operation.

  16. Laboratory actinide partitioning - Whitlockite/liquid and influence of actinide concentration levels

    NASA Technical Reports Server (NTRS)

    Benjamin, T. M.; Jones, J. H.; Heuser, W. R.; Burnett, D. S.

    1983-01-01

    The partition coefficients between synthetic whitlockite (beta Ca-phosphate) and coexisting silicate melts are determined for the actinide elements Th, U and Pu. Experiments were performed at 1 bar pressure and 1250 C at oxygen fugacities from 10 to the -8.5 to 10 to the -0.7 bars, and partitioning was determined from trace element radiography combined with conventional electron microprobe analysis. Results show Pu to be more readily incorporated into crystalline phases than U or Th under reducing conditions, which is attributed to the observation that Pu exists primarily in the trivalent state, while U and Th are tetravalent. Corrected partition coefficients for whitlockite of 3.6, less than or equal to 0.6, 1.2, 0.5 and less than or equal to 0.002 are estimated for Pu(+3), Pu(+4), Th(+4), U(+4) and U(+6), respectively. Experiments performed at trace levels and percent levels of UO2 indicate that Si is involved in U substitution in whitlockite, and show a reduced partition coefficient at higher concentrations of U that can be explained by effects on melt structure or the fraction of tetravalent U.

  17. A grit separation module for inorganic matter removal from activated sludge: investigation on characteristics of split sludge from the module.

    PubMed

    Chen, You-Peng; Guo, Jin-Song; Wang, Jing; Yan, Peng; Ji, Fang-Ying; Fang, Fang; Dong, Yang

    2016-12-01

    A grit separation module was developed to prevent the accumulation of inorganic solids in activated sludge systems, and it achieved effective separation of organic matter and inorganic solids. To provide technical and theoretical support for further comprehensive utilization of split sludge (underflow and overflow sludge from the separation module), the characteristics of split sludge were investigated. The settling and dewatering properties of the underflow sludge were excellent, and it had high inorganic matter content, whereas the overflow sludge had higher organic matter content. The most abundant inorganic constituent was SiO2 (59.34%), and SiO2, Al2O3, and Fe2O3 together accounted for 79.53% of the inorganic matter in the underflow sludge. The mass ratio of Fe2O3, CaO, and MgO to SiO2 and Al2O3 was 0.245 in the inorganic component of the underflow sludge. The underflow sludge had the beneficial characteristics of simple treatment and disposal, and it was suitable for use as a base raw material for ceramsite production. The overflow sludge with higher organic matter content was constantly returned from the separation module to the wastewater treatment system, gradually improving the volatile suspended solid/total suspended solid ratio of the activated sludge in the wastewater treatment system.

  18. Chemistry of the heaviest actinides: fermium, mendelevium, nobelium, and lawrencium

    SciTech Connect

    Hulet, E.K.

    1980-01-01

    The chemical properties of the heavy actinides systematically deviate from those of their lanthanide counterparts. The differences between the later elements of the 4f and 5f series can be generally interpreted on the basis of subtle changes in electronic structure. The most important change is a lowering of the 5f energy levels with respect to the Fermi level and a wider separation between the 5f ground states and the first excited states in the 6d or 7p levels. It was concluded that these shifts toward greater stabilization of 5f orbitals with increasing atomic number are mainly supported by the appearance of the divalent oxidation state well before the end of the actinide series and the predominance of the divalent state in the next to last element in the series. The chemistry of fermium, mendelevium, nobelium, and lawrencium was discussed. 8 figures 4 tables. (DP)

  19. Actinide-specific sequestering agents and decontamination applications

    SciTech Connect

    Smith, William L.; Raymond, Kenneth N.

    1981-04-07

    With the commercial development of nuclear reactors, the actinides have become very important industrial elements. A major concern of the nuclear industry is the biological hazard associated with nuclear fuels and their wastes. The acute chemical toxicity of tetravalent actinides, as exemplified by Th(IV), is similar to Cr(III) or Al(III). However, the acute toxicity of 239Pu(IV) is similar to strychnine, which is much more toxic than any of the non-radioactive metals such as mercury. Although the more radioactive isotopes of the transuranium elements are more acutely toxic by weight than plutonium, the acute toxicities of 239Pu, 241Am, and 244Cm are nearly identical in radiation dose, ~100 μCi/kg in rodents. Finally and thus, the extreme acute toxicity of 239Pu is attributed to its high specific activity of alpha emission.

  20. Pulsed photothermal spectroscopy applied to lanthanide and actinide speciation

    SciTech Connect

    Berg, J.M.; Morris, D.E.; Clark, D.L.; Tait, C.D.; Woodruff, W.H. ); Ven Der Sluys, W.G. . Dept. of Chemistry)

    1991-01-01

    Several key elements important for the application of laser-based photothermal spectroscopies to the study of the complexation chemistry of lanthanides and actinides in solution have been demonstrated. The sensitivity of f-f electronic transition energies and band intensities to subtle changes in complexation was illustrated through comparison of visible and near infra-red absorption spectra of well-characterized U(IV) dimers with alkoxide ligands. Significant improvements in spectroscopic band resolution and energy measurement precision for solution species were shown to be achievable through work in frozen glasses at 77 K using a very simple cryogenic apparatus. A pulsed-laser photothermal spectroscopy apparatus was constructed and shown to be sensitive to optical density changes of 10{sup {minus}5} in an aqueous Nd{sup 3+} solution. In addition, the capability of obtaining photothermal lensing spectra of dilute actinide solutions in frozen glasses at 77 K was demonstrated. 6 refs., 5 figs.

  1. Development of a remote bushing for actinide vitrification

    SciTech Connect

    Schumacher, R.F.; Ramsey, W.G.; Johnson, F.M.

    1996-12-31

    The Savannah River Site (SRS) and the Savannah River Technology Center (SRTC) are combining their existing experience in handling highly radioactive, special nuclear materials with commercial glass fiberization technology in order to assemble a small vitrification system for radioactive actinide solutions. The vitrification system or {open_quotes}brushing{close_quotes}, is fabricated from platinum-rhodium alloy and is based on early marble remelt fiberization technology. Advantages of this unique system include its relatively small size, reliable operation, geometrical safety (nuclear criticality), and high temperature capability. The bushing design should be capable of vitrifying a number of the actinide nuclear materials, including solutions of americium/curium, neptunium, and possibly plutonium. State of the art, mathematical and oil model studies are being combined with basic engineering evaluations to verify and improve the thermal and mechanical design concepts.

  2. The pentavalent actinide solution chemistry in the environment.

    PubMed

    Topin, Sylvain; Aupiais, Jean

    2016-03-01

    With regard to environmental monitoring of certain nuclear facilities, pentavalent actinides, in particular neptunium and plutonium, play a key role, as the chief soluble, mobile forms of actinides. In the past five years, investigations carried out by hyphenating capillary electrophoresis to ICP-MS (CE-ICP-MS) have allowed a number of hitherto unknown thermodynamic data to be determined for Np(V) and Pu(V) interactions with the chief environmentally abundant anions. For the first time, data were provided for Pu(V) interactions with carbonate, sulfate, oxalate, chloride, and nitrate ions, allowing the Np(V)/Pu(V) analogy to be verified experimentally. Knowledge of Np(V) chemistry, especially in carbonate, and sulfate media, was also refined. These CE-ICP-MS studies, combined with some earlier findings, have brought about a renewal in the knowledge of An(V) chemistry in solution.

  3. Radioanalytical determination of actinides and fission products in Belarus soils.

    PubMed

    Michel, H; Gasparro, J; Barci-Funel, G; Dalmasso, J; Ardisson, G; Sharovarov, G

    1999-04-01

    Alpha emitting actinides such as plutonium, americium or curium were measured by alpha-spectrometry after radiochemical separation. The short range of alpha-particles within matter requires, after a pre-concentration process, a succession of isolation and purification steps based on the valence states modification of the researched elements. For counting, actinides were electrodeposited in view to obtain the mass-less source necessary to avoid self-absorption of the emitted radiations. Activity concentrations of gamma-emitting fission products were calculated after measurement with high purity germanium detectors (HPGe). These different methods were used to analyse soils sampled in the Republic of Belarus, not far from the Chernobyl nuclear plant.

  4. Comparative Study of f-Element Electronic Structure across a Series of Multimetallic Actinide, Lanthanide-Actinide and Lanthanum-Actinide Complexes Possessing Redox-Active Bridging Ligands

    SciTech Connect

    Schelter, Eric J.; Wu, Ruilian; Veauthier, Jacqueline M.; Bauer, Eric D.; Booth, Corwin H.; Thomson, Robert K.; Graves, Christopher R.; John, Kevin D.; Scott, Brian L.; Thompson, Joe D.; Morris, David E.; Kiplinger, Jaqueline L.

    2010-02-24

    A comparative examination of the electronic interactions across a series of trimetallic actinide and mixed lanthanide-actinide and lanthanum-actinide complexes is presented. Using reduced, radical terpyridyl ligands as conduits in a bridging framework to promote intramolecular metal-metal communication, studies containing structural, electrochemical, and X-ray absorption spectroscopy are presented for (C{sub 5}Me{sub 5}){sub 2}An[-N=C(Bn)(tpy-M{l_brace}C{sub 5}Me4R{r_brace}{sub 2})]{sub 2} (where An = Th{sup IV}, U{sup IV}; Bn = CH{sub 2}C{sub 6}H{sub 5}; M = La{sup III}, Sm{sup III}, Yb{sup III}, U{sup III}; R = H, Me, Et) to reveal effects dependent on the identities of the metal ions and R-groups. The electrochemical results show differences in redox energetics at the peripheral 'M' site between complexes and significant wave splitting of the metal- and ligand-based processes indicating substantial electronic interactions between multiple redox sites across the actinide-containing bridge. Most striking is the appearance of strong electronic coupling for the trimetallic Yb{sup III}-U{sup IV}-Yb{sup III}, Sm{sup III}-U{sup IV}-Sm{sup III}, and La{sup III}-U{sup IV}-La{sup III} complexes, [8]{sup -}, [9b]{sup -} and [10b]{sup -}, respectively, whose calculated comproportionation constant K{sub c} is slightly larger than that reported for the benchmark Creutz-Taube ion. X-ray absorption studies for monometallic metallocene complexes of U{sup III}, U{sup IV}, and U{sup V} reveal small but detectable energy differences in the 'white-line' feature of the uranium L{sub III}-edges consistent with these variations in nominal oxidation state. The sum of this data provides evidence of 5f/6d-orbital participation in bonding and electronic delocalization in these multimetallic f-element complexes. An improved, high-yielding synthesis of 4{prime}-cyano-2,2{prime}:6{prime},2{double_prime}-terpyridine is also reported.

  5. Role of Minor Actinides for Long-Life Reactor Cores

    SciTech Connect

    Saito, M.; Artisyuk, V.; Shmelev, A.; Nikitin, K.; Peryoga, Y

    2002-07-01

    The paper addresses the study on advanced fuel cycles for LWR oriented to high burnup values that exceed 100 GWd/tHM, thus giving the chance to establish the long-life reactor cores without fuel reloading on site. The key element of this approach is a broad involvement of Minor Actinides whose admixture to 20% enriched uranium fuel provides safe release of initial reactivity excess and improved proliferation resistance properties. (authors)

  6. Benefits of actinide-only burnup credit for shutdown PWRs

    SciTech Connect

    Lancaster, D.; Fuentes, E.; Kang, C.; Rivard, D.

    1998-02-01

    Owners of PWRs that are shutdown prior to resolution of interim storage or permanent disposal issues have to make difficult decisions on what to do with their spent fuel. Maine Yankee is currently evaluating multiple options for spent fuel storage. Their spent fuel pool has 1,434 assemblies. In order to evaluate the value to a utility of actinide-only burnup credit, analysis of the number of canisters required with and without burnup credit was made. In order to perform the analysis, loading curves were developed for the Holtec Hi-Star 100/MPC-32. The MPC-32 is hoped to be representative of future burnup credit designs from many vendors. The loading curves were generated using the actinide-only burnup credit currently under NRC review. The canister was analyzed for full loading (32 assemblies) and with partial loadings of 30 and 28 assemblies. If no burnup credit is used the maximum capacity was assumed to be 24 assemblies. this reduced capacity is due to the space required for flux traps which are needed to sufficiently reduce the canister reactivity for the fresh fuel assumption. Without burnup credit the 1,343 assemblies would require 60 canisters. If all the fuel could be loaded into the 32 assembly canisters only 45 canisters would be required. Although the actinide-only burnup credit approach is very conservative, the total number of canisters required is only 47 which is only two short of the minimum possible number of canisters. The utility is expected to buy the canister and the storage overpack. A reasonable cost estimate for the canister plus overpack is $500,000. Actinide-only burnup credit would save 13 canisters and overpacks which is a savings of about $6.5 million. This savings is somewhat reduced since burnup credit requires a verification measurement of burnup. The measurement costs for these assemblies can be estimated as about $1 million. The net savings would be $5.5 million.

  7. Determination of actinides in urine and fecal samples

    SciTech Connect

    McKibbin, T.T.

    1992-12-31

    A method of determining the radioactivity of specific actinides that are carried in urine or fecal sample material is disclosed. The samples are ashed in a muffle furnace, dissolved in an acid, and then treated in a series of steps of reduction, oxidation, dissolution, and precipitation, including a unique step of passing a solution through a chloride form anion exchange resin for separation of uranium and plutonium from americium.

  8. Future nuclear fuel cycles: Prospect and challenges for actinide recycling

    NASA Astrophysics Data System (ADS)

    Warin, Dominique

    2010-03-01

    The global energy context pleads in favour of a sustainable development of nuclear energy since the demand for energy will likely increase, whereas resources will tend to get scarcer and the prospect of global warming will drive down the consumption of fossil fuel. In this context, nuclear power has the worldwide potential to curtail the dependence on fossil fuels and thereby to reduce the amount of greenhouse gas emissions while promoting energy independence. How we deal with nuclear radioactive waste is crucial in this context. In France, the public's concern regarding the long-term waste management made the French Governments to prepare and pass the 1991 and 2006 Acts, requesting in particular the study of applicable solutions for still minimizing the quantity and the hazardousness of final waste. This necessitates High Active Long Life element (such as the Minor Actinides MA) recycling, since the results of fuel cycle R&D could significantly change the challenges for the storage of nuclear waste. HALL recycling can reduce the heat load and the half-life of most of the waste to be buried to a couple of hundred years, overcoming the concerns of the public related to the long-life of the waste and thus aiding the "burying approach" in securing a "broadly agreed political consensus" of waste disposal in a geological repository. This paper presents an overview of the recent R and D results obtained at the CEA Atalante facility on innovative actinide partitioning hydrometallurgical processes. For americium and curium partitioning, these results concern improvements and possible simplifications of the Diamex-Sanex process, whose technical feasibility was already demonstrated in 2005. Results on the first tests of the Ganex process (grouped actinide separation for homogeneous recycling) are also discussed. In the coming years, next steps will involve both better in-depth understanding of the basis of these actinide partitioning processes and, for the new promising

  9. Chemical properties of the heavier actinides and transactinides

    SciTech Connect

    Hulet, E.K.

    1981-01-01

    The chemical properties of each of the elements 99 (Es) through 105 are reviewed and their properties correlated with the electronic structure expected for 5f and 6d elements. A major feature of the heavier actinides, which differentiates them from the comparable lanthanides, is the increasing stability of the divalent oxidation state with increasing atomic number. The divalent oxidation state first becomes observable in the anhydrous halides of californium and increases in stability through the series to nobelium, where this valency becomes predominant in aqueous solution. In comparison with the analogous 4f electrons, the 5f electrons in the latter part of the series are more tightly bound. Thus, there is a lowering of the 5f energy levels with respect to the Fermi level as the atomic number increases. The metallic state of the heavier actinides has not been investigated except from the viewpoint of the relative volatility among members of the series. In aqueous solutions, ions of these elements behave as a normal trivalent actinides and lanthanides (except for nobelium). Their ionic radii decrease with increasing nuclear charge which is moderated because of increased screening of the outer 6p electrons by the 5f electrons. The actinide series of elements is completed with the element lawrencium (Lr) in which the electronic configuration is 5f/sup 14/7s/sup 2/7p. From Mendeleev's periodicity and Dirac-Fock calculations, the next group of elements is expected to be a d-transition series corresponding to the elements Hf through Hg. The chemical properties of elements 104 and 105 only have been studied and they indeed appear to show the properties expected of eka-Hf and eka-Ta. However, their nuclear lifetimes are so short and so few atoms can be produced that a rich variety of chemical information is probably unobtainable.

  10. Determination of actinides in urine and fecal samples

    DOEpatents

    McKibbin, T.T.

    1993-03-02

    A method of determining the radioactivity of specific actinides that are carried in urine or fecal sample material is disclosed. The samples are ashed in a muffle furnace, dissolved in an acid, and then treated in a series of steps of reduction, oxidation, dissolution, and precipitation, including a unique step of passing a solution through a chloride form anion exchange resin for separation of uranium and plutonium from americium.

  11. Determination of actinides in urine and fecal samples

    DOEpatents

    McKibbin, Terry T.

    1993-01-01

    A method of determining the radioactivity of specific actinides that are carried in urine or fecal sample material is disclosed. The samples are ashed in a muffle furnace, dissolved in an acid, and then treated in a series of steps of reduction, oxidation, dissolution, and precipitation, including a unique step of passing a solution through a chloride form anion exchange resin for separation of uranium and plutonium from americium.

  12. Relativistic effects on the thermal expansion of the actinide elements

    SciTech Connect

    Soederlind, P.; Nordstroem, L.; Lou Yongming; Johansson, B. )

    1990-09-01

    The room-temperature linear thermal-expansion coefficient is calculated for the light actinides thorium, protactinium, uranium, neptunium, and plutonium for the fcc crystal structure. The relativistic spin-orbit interaction is included in these calculations. We show that the spin-orbit splitting of the 5{ital f} band gives rise to a considerable increase of the thermal expansion and to a large extent explains the observed anomalously large thermal expansion for the neptunium and plutonium metals.

  13. Molecular Characterization of Actinide Oxocations from Protactinium to Plutonium

    SciTech Connect

    Den Auwer, C.; Guilbaud, P.; Guillaumont, D.; Moisy, P.; Hennig, C.; Scheinost, A.; Conradson, S. D.

    2007-02-02

    This presentation addresses the structural characterization by EXAFS of actinide cations at oxidation states (V) and (VI) as one walks across the periodic table from Z = 91 (protactinium) to Z = 94 (plutonium). A structural comparison between Pa, U, Np and Pu oxocations in aqueous solution at formal oxidation states (V) and (VI) is carried out. These results are corroborated by quantum chemical and molecular dynamics calculations.

  14. Chemical and Ceramic Methods Toward Safe Storage of Actinides

    SciTech Connect

    P.E.D. Morgan; R.M. Housley; J.B. Davis; M.L. DeHaan

    2005-08-19

    A very import, extremely-long-term, use for monazite as a radwaste encapsulant has been proposed. THe use of ceramic La-monazite for sequestering actinides (isolating them from the environment), especially plutonium and some other radioactive elements )e.g., fission-product rare earths), had been especially championed by Lynn Boatner of ORNL. Monazite may be used alone or, copying its compatibility with many other minerals in nature, may be used in diverse composite combinations.

  15. Method for the concentration and separation of actinides from biological and environmental samples

    DOEpatents

    Horwitz, E.P.; Dietz, M.L.

    1989-05-30

    A method and apparatus for the quantitative recover of actinide values from biological and environmental sample by passing appropriately prepared samples in a mineral acid solution through a separation column of a dialkyl(phenyl)-N,N-dialylcarbamoylmethylphosphine oxide dissolved in tri-n-butyl phosphate on an inert substrate which selectively extracts the actinide values. The actinide values can be eluted either as a group or individually and their presence quantitatively detected by alpha counting. 3 figs.

  16. Method for the concentration and separation of actinides from biological and environmental samples

    DOEpatents

    Horwitz, E. Philip; Dietz, Mark L.

    1989-01-01

    A method and apparatus for the quantitative recover of actinide values from biological and environmental sample by passing appropriately prepared samples in a mineral acid solution through a separation column of a dialkyl(phenyl)-N,N-dialylcarbamoylmethylphosphine oxide dissolved in tri-n-butyl phosphate on an inert substrate which selectively extracts the actinide values. The actinide values can be eluted either as a group or individually and their presence quantitatively detected by alpha counting.

  17. Design of unique pins for irradiation of higher actinides in a fast reactor

    SciTech Connect

    Basmajian, J.A.; Birney, K.R.; Weber, E.T.; Adair, H.L.; Quinby, T.C.; Raman, S.; Butler, J.K.; Bateman, B.C.; Swanson, K.M.

    1982-03-01

    The actinides produced by transmutation reactions in nuclear reactor fuels are a significant factor in nuclear fuel burnup, transportation and reprocessing. Irradiation testing is a primary source of data of this type. A segmented pin design was developed which provides for incorporation of multiple specimens of actinide oxides for irradiation in the UK's Prototype Fast Reactor (PFR) at Dounreay Scotland. Results from irradiation of these pins will extend the basic neutronic and material irradiation behavior data for key actinide isotopes.

  18. On-line Monitoring of Actinide Concentrations in Molten Salt Electrolyte

    SciTech Connect

    Curtis W. Johnson; Mary Lou Dunzik-Gougar; Shelly X. Li

    2006-11-01

    Pyroprocessing, a treatment method for spent nuclear fuel (SNF), is currently being studied at the Idaho National Laboratory. The key operation of pyroprocessing which takes place in an electrorefiner is the electrochemical separation of actinides from other constituents in spent fuel. Efficient operation of the electrorefiner requires online monitoring of actinide concentrations in the molten salt electrolyte. Square-wave voltammetry (SWV) and normal pulse voltammetry (NPV) are being investigated to assess their applicability to the measurement of actinide concentrations in the electrorefiner.

  19. Disposition of actinides released from high-level waste glass

    SciTech Connect

    Ebert, W.L.; Bates, J.K.; Buck, E.C.; Gong, M.; Wolf, S.F.

    1994-05-01

    A series of static leach tests was conducted using glasses developed for vitrifying tank wastes at the Savannah River Site to monitor the disposition of actinide elements upon corrosion of the glasses. In these tests, glasses produced from SRL 131 and SRL 202 frits were corroded at 90{degrees}C in a tuff groundwater. Tests were conducted using crushed glass at different glass surface area-to-solution volume (S/V) ratios to assess the effect of the S/V on the solution chemistry, the corrosion of the glass, and the disposition of actinide elements. Observations regarding the effects of the S/V on the solution chemistry and the corrosion of the glass matrix have been reported previously. This paper highlights the solution analyses performed to assess how the S/V used in a static leach test affects the disposition of actinide elements between fractions that are suspended or dissolved in the solution, and retained by the altered glass or other materials.

  20. Crystalline matrices for the immobilization of plutonium and actinides

    SciTech Connect

    Anderson, E.B.; Burakov, E.E.; Galkin, Ya.B.; Starchenko, V.A.; Vasiliev, V.G.

    1996-05-01

    The management of weapon plutonium, disengaged as a result of conversion, is considered together with the problem of the actinide fraction of long-lived high level radioactive wastes. It is proposed to use polymineral ceramics based on crystalline host-phases: zircon ZrSiO{sub 4} and zirconium dioxide ZrO{sub 2}, for various variants of the management of plutonium and actinides (including the purposes of long-term safe storage or final disposal from the human activity sphere). It is shown that plutonium and actinides are able to form with these phases on ZrSiO{sub 4} and ZrO{sub 2} was done on laboratory level by the hot pressing method, using the plasmochemical calcination technology. To incorporate simulators of plutonium into the structure of ZrSiO{sub 4} and ZrO{sub 2} in the course of synthesis, an original method developed by the authors as a result of studying the high-uranium zircon (Zr,U) SiO{sub 4} form Chernobyl {open_quotes}lavas{close_quotes} was used.

  1. Computational Modeling of Actinide Ions in Aqueous Solution

    NASA Astrophysics Data System (ADS)

    Atta-Fynn, Raymond

    2014-03-01

    Unraveling the chemical behavior of actinide species is difficult owing to the complex electronic structure of these species, the fact that many of these species can occur in multiple oxidation states, and the difficulties encountered in their experimental studies. First principles dynamical modeling, although computationally costly, allows us to gain rich insights into the behavior of actinide species. In this talk, we present results of the hydration shell structure and x-ray absorption spectra of aqueous actinides in different oxidation states including U(VI), U(V), U(IV), and Cm(III) using relativistic ab initiomolecular dynamics at 300 K. We also probed the thermodynamics of hydrolysis by calculating the first acidity constant for uranium in all three oxidation states (IV, V, and VI). We predicted, for the first time, that UO2+ is a weak acid in solution with a pKa value of 8.5. This result is particularly important since no thermodynamic data are available for hydrolyzed species of U(V). In our most recent work on concentrated Cm(III) solutions, we showed that counter-ions can strengthen or weaken the solvent structure itself rather than just the water coordination number. These new results are better explained in terms of the hydrogen bond lifetimes of the solvents.

  2. The EBR-II X501 Minor Actinide Burning Experiment

    SciTech Connect

    Jon Carmack; S. L. Hayes; M. K. Meyer; H. Tsai

    2008-06-01

    The X501 experiment was conducted in EBR-II as part of the IFR (Integral Fast Reactor) program to demonstrate minor actinide burning through the use of a homogeneous recycle scheme. The X501 subassembly contained two metallic fuel elements loaded with relatively small quantities of americium and neptunium. Interest in the behavior of minor actinides (MA) during fuel irradiation has prompted further examination of existing X501 data, and generation of new data where needed in support of the U.S. waste transmutation effort. The X501 experiment is one of the few minor actinide-bearing fuel irradiation tests conducted worldwide and knowledge can be gained by understanding the changes in fuel behavior due to addition of MA’s. Of primary interest are the affect of the MA’s on fuel-cladding-chemical-interaction, and the redistribution behavior of americium. The quantity of helium gas release from the fuel and any effects of helium on fuel performance are also of interest. It must be stressed that information presented at this time is based on the limited PIE conducted in 1995-1996, and currently represents a set of observations rather than a complete understanding of fuel behavior.

  3. Redox response of actinide materials to highly ionizing radiation

    NASA Astrophysics Data System (ADS)

    Tracy, Cameron L.; Lang, Maik; Pray, John M.; Zhang, Fuxiang; Popov, Dmitry; Park, Changyong; Trautmann, Christina; Bender, Markus; Severin, Daniel; Skuratov, Vladimir A.; Ewing, Rodney C.

    2015-01-01

    Energetic radiation can cause dramatic changes in the physical and chemical properties of actinide materials, degrading their performance in fission-based energy systems. As advanced nuclear fuels and wasteforms are developed, fundamental understanding of the processes controlling radiation damage accumulation is necessary. Here we report oxidation state reduction of actinide and analogue elements caused by high-energy, heavy ion irradiation and demonstrate coupling of this redox behaviour with structural modifications. ThO2, in which thorium is stable only in a tetravalent state, exhibits damage accumulation processes distinct from those of multivalent cation compounds CeO2 (Ce3+ and Ce4+) and UO3 (U4+, U5+ and U6+). The radiation tolerance of these materials depends on the efficiency of this redox reaction, such that damage can be inhibited by altering grain size and cation valence variability. Thus, the redox behaviour of actinide materials is important for the design of nuclear fuels and the prediction of their performance.

  4. Redox response of actinide materials to highly ionizing radiation.

    PubMed

    Tracy, Cameron L; Lang, Maik; Pray, John M; Zhang, Fuxiang; Popov, Dmitry; Park, Changyong; Trautmann, Christina; Bender, Markus; Severin, Daniel; Skuratov, Vladimir A; Ewing, Rodney C

    2015-01-27

    Energetic radiation can cause dramatic changes in the physical and chemical properties of actinide materials, degrading their performance in fission-based energy systems. As advanced nuclear fuels and wasteforms are developed, fundamental understanding of the processes controlling radiation damage accumulation is necessary. Here we report oxidation state reduction of actinide and analogue elements caused by high-energy, heavy ion irradiation and demonstrate coupling of this redox behaviour with structural modifications. ThO2, in which thorium is stable only in a tetravalent state, exhibits damage accumulation processes distinct from those of multivalent cation compounds CeO2 (Ce(3+) and Ce(4+)) and UO3 (U(4+), U(5+) and U(6+)). The radiation tolerance of these materials depends on the efficiency of this redox reaction, such that damage can be inhibited by altering grain size and cation valence variability. Thus, the redox behaviour of actinide materials is important for the design of nuclear fuels and the prediction of their performance.

  5. Supercritical Fluid Extraction and Separation of Uranium from Other Actinides

    SciTech Connect

    Donna L. Quach; Bruce J. Mincher; Chien M. Wai

    2014-06-01

    This paper investigates the feasibility of separating uranium from other actinides by using supercritical fluid carbon dioxide (sc-CO2) as a solvent modified with tri-n-butylphosphate (TBP) for the development of an extraction and counter current stripping technique, which would be a more efficient and environmentally benign technology for used nuclear fuel reprocessing compared to traditional solvent extraction. Several actinides (U(VI), Np(VI), Pu(IV), and Am(III)) were extracted in sc-CO2 modified with TBP over a range of nitric acid concentrations and then the actinides were exposed to reducing and complexing agents to suppress their extractability. According to this study, the separation of uranium from plutonium in sc-CO2 modified with TBP was successful at nitric acid concentrations of less than 3 M in the presence of acetohydroxamic acid or oxalic acid, and the separation of uranium from neptunium was successful at nitric acid concentrations of less than 1 M in the presence of acetohydroxamic acid, oxalic acid, or sodium nitrite.

  6. Multi-analytical assessment of iron and steel slag characteristics to estimate the removal of metalloids from contaminated water.

    PubMed

    Mercado-Borrayo, B M; Schouwenaars, R; González-Chávez, J L; Ramírez-Zamora, R M

    2013-01-01

    A multi-analytical approach was used to develop a mathematical regression model to calculate the residual concentration of borate ions in water present at high initial content, as a function of the main physicochemical, mineralogical and electrokinetic characteristics after adsorption on five different types of iron and steel slag. The analytical techniques applied and slag properties obtained in this work were: X-ray Fluorescence for the identification of the main chemical compounds, X-ray Diffraction to determine crystalline phases, physical adsorption of nitrogen for the quantification of textural properties and zeta-potential for electrokinetic measurements of slag particles. Adsorption tests were carried out using the bottle-point technique and a highly concentrated borate solution (700 mg B/L) at pH 10, with a slag dose of 10 g/L. An excellent correlation between the residual concentration of boron and three independent variables (content of magnesium oxide, zeta potential and specific surface area) was established for the five types of slag tested in this work. This shows that the methodology based on a multi-analytical approach is a very strong and useful tool to estimate the performance of iron and steel slag as adsorbent of metalloids.

  7. Survey on nitrogen removal and membrane filtration characteristics of Chlorella vulgaris Beij. on treating domestic type wastewaters.

    PubMed

    Wang, Yu-Hsuan; Wu, Chuen-Mei; Wu, Wan-Lin; Chu, Ching-Ping; Chung, Yu-Jen; Liao, Chien-Sen

    2013-01-01

    The main objective of this study is to evaluate the nitrogen assimilation and filtration characteristics of Chlorella vulgaris Beij. when treating domestic wastewaters. Chlorella could assimilate organic nitrogen, ammonia and nitrate in wastewater, and the mean cell residence time (MCRT) to achieve the maximum biomass content in a bioreactor was different for each individual nitrogen source used. The experimental results showed that using nitrate as the only nitrogen source was the most favorable for biomass growth. With ammonia and nitrate coexisting in the aquatic phase, Chlorella possibly utilized ammonia first, and this was unfavorable to subsequent biomass growth. Nitrifying bacteria in wastewaters significantly affected Chlorella growth as they possibly competed with Chlorella in assimilating ammonia and nitrate in domestic wastewater. In a submerged ultrafiltration (UF) membrane module, with an initial concentration of 850 mg/L of Chlorella, the optimized flux was 0.02 m(3)/(m(2)·h), and the filtration cycle was 30 min. A 'dual membrane bioreactor (MBR)' configuration using UF membranes for Chlorella incubation was proposed. MBR1 provides an environment with long MCRT for efficient nitrification. The converted nitrate is assimilated by Chlorella in MBR2 to sustain its growth. UF permeate from MBR1 is bacteria-free and does not affect the growth of Chlorella in MBR2. MCRT of Chlorella growth is controlled by the UF membrane of MBR2, providing the flexibility to adjust variations of nitrogen composition in the wastewater.

  8. Characteristics of adsorbents made from biological, chemical and hybrid sludges and their effect on organics removal in wastewater treatment.

    PubMed

    Pan, Zhi-hui; Tian, Jia-yu; Xu, Guo-ren; Li, Jun-jing; Li, Gui-bai

    2011-01-01

    Meso-macropore adsorbents were prepared from biological sludge, chemical sludge and hybrid sludge of biological and chemical sludges, by chemically activating with 18.0 M H(2)SO(4) in the mass ratio of 1:3, and then pyrolyzing at 550 °C for 1 h in anoxic atmosphere. The physical and chemical characteristics of the sludge-based adsorbents were examined in terms of surface physical morphology, specific surface area and pore size distribution, aluminum and iron contents, surface functional groups and crystal structure. Furthermore, the adsorption effect of these adsorbents on the organic substances in wastewater was also investigated. The results indicated that the adsorption capacities of the sludge-based adsorbents for UV(254) were lower than that of commercial activated carbon (AC), whereas the adsorption capacities of the adsorbents prepared from hybrid sludge (HA) and chemical sludge (CA) for soluble COD(Cr) (SCOD(Cr)) were comparable or even higher than that of the commercial AC. The reasons might be that the HA and CA possessed well-developed mesopore and macropore structure, as well as abundant acidic surface functional groups. However, the lowest adsorption efficiency was observed for the biological sludge-based adsorbent, which might be due to the lowest metal content and overabundance of surface acidic functional groups in this adsorbent.

  9. The study of organic removal efficiency and halophilic bacterial mixed liquor characteristics in a membrane bioreactor treating hypersaline produced water at varying organic loading rates.

    PubMed

    Sharghi, Elham Abdollahzadeh; Bonakdarpour, Babak

    2013-12-01

    In this study the organic pollutant removal performance and the mixed liquor characteristics of a membrane bioreactor (MBR), employing a halophilic bacterial consortium, for the treatment of hypersaline synthetic produced water - at varying organic loading rates (OLR) from 0.3 to 2.6 kg CODm(-3)d(-1) - were considered. The oil and grease (O&G) and COD removal efficiency were 95-99% and 83-93%, respectively with only transient O&G (mainly polycyclic aromatic hydrocarbons) and soluble microbial products accumulation being observed. With increasing OLR, in the range 0.9-2.6 kg COD m(-3)d(-1), as a result of change in both extracellular polymeric substances (EPS) and zeta potential, bioflocculating ability improved but the compressibility of the flocs decreased resulting in the occurrence of EPS bulking at the highest OLR studied. The latter resulted in a change in the rheology of the mixed liquor from Newtonian to non-Newtonian and the occurrence of significant membrane fouling.

  10. Separation of actinides using capillary extraction chromatography-inductively coupled plasma mass spectrometry.

    PubMed

    Peterson, Dominic S; Montoya, Velma M

    2009-08-01

    Trace levels of actinides have been separated on capillary extraction chromatography columns. Detection of the actinides was achieved using an inductively coupled plasma mass spectrometer, which was coupled with the extraction chromatography system. In this study, we compare 30-cm long, 4.6 mm i.d. columns to capillary columns (750 microm i.d.) with lengths from 30 cm up to 150 cm. The columns that were tested were packed with TRU resin. We were able to separate a mixture of five actinides ((232)Th, (238)U, (237)Np, (239)Pu, and (241)Am). This work has application to rapid bioassay as well as automated separations of actinide materials.

  11. Flowsheet report for baseline actinide blanket processing for accelerator transmutation of waste

    SciTech Connect

    Walker, R.B.

    1992-04-08

    We provide a flowsheet analysis of the chemical processing of actinide and fission product materials form the actinide blanket of an accelerator-based transmutation concept. An initial liquid ion exchange step is employed to recover unburned plutonium and neptunium, so that it can be returned quickly to the transmitter. The remaining materials, consisting of fission products and trivalent actinides (americium, curium), is processed after a cooling period. A reverse Talspeak process is employed to separate these trivalent actinides from lanthanides and other fission products.

  12. Fission fragment angular distributions in pre-actinide nuclei

    NASA Astrophysics Data System (ADS)

    Banerjee, Tathagata; Nath, S.; Jhingan, A.; Kaur, Gurpreet; Dubey, R.; Yadav, Abhishek; Laveen, P. V.; Shamlath, A.; Shareef, M.; Gehlot, J.; Saneesh, N.; Prasad, E.; Sugathan, P.; Pal, Santanu

    2016-10-01

    Background: Complete fusion of two nuclei leading to formation of a heavy compound nucleus (CN) is known to be hindered by various fission-like processes, in which the composite system reseparates after capture of the target and the projectile inside the potential barrier. As a consequence of these non-CN fission (NCNF) processes, fusion probability (PCN) starts deviating from unity. Despite substantial progress in understanding, the onset and the experimental signatures of NCNF and the degree of its influence on fusion have not yet been unambiguously identified. Purpose: This work aims to investigate the presence of NCNF, if any, in pre-actinide nuclei by systematic study of fission angular anisotropies and fission cross sections (σfis) in a number of nuclear reactions carried out at and above the Coulomb barrier (VB) . Method: Fission fragment angular distributions were measured for six 28Si-induced reactions involving isotopically enriched targets of 169Tm,176Yb,175Lu,180Hf,181Ta, and 182W leading to probable formation of CN in the pre-actinide region, at a laboratory energy (Elab) range of 129-146 MeV. Measurements were performed with large angular coverage (θlab=41∘ -170∘) in which fission fragments (FFs) were detected by nine hybrid telescope (E -Δ E ) detectors. Extracted fission angular anisotropies and σfis were compared with statistical model (SM) predictions. Results: Barring two reactions involving targets with large non-zero ground state spin (J ) , viz., 175Lu(7/2+) and 181Ta(7/2+) , experimental fission angular anisotropies were found to be higher in comparison with predictions of the statistical saddle point model (SSPM), at Ec .m . near VB. Comparison of present results with those from neighboring systems revealed that experimental anisotropies increasingly deviated from SSPM predictions as one moved from pre-actinide to actinide nuclei. For reactions involving targets with large nonzero J , this deviation was subdued. Comparison between

  13. Biomimetic Actinide Chelators: An Update on the Preclinical Development of the Orally Active Hydroxypyridonate Decorporation Agents 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO)

    PubMed Central

    Abergel, Rebecca J.; Durbin, Patricia W.; Kullgren, Birgitta; Ebbe, Shirley N.; Xu, Jide; Chang, Polly Y.; Bunin, Deborah I.; Blakely, Eleanor A.; Bjornstad, Kathleen A.; Rosen, Chris J.; Shuh, David K.; Raymond, Kenneth N.

    2010-01-01

    The threat of a dirty bomb or other major radiological contamination presents a danger of large-scale radiation exposure of the population. Because major components of such contamination are likely to be actinides, actinide decorporation treatments that will reduce radiation exposure must be a priority. Current therapies for the treatment of radionuclide contamination are limited and extensive efforts must be dedicated to the development of therapeutic, orally bioavailable, actinide chelators for emergency medical use. Using a biomimetic approach based on the similar biochemical properties of plutonium(IV) and iron(III), siderophore-inspired multidentate hydroxypyridonate ligands have been designed and are unrivaled in terms of actinide-affinity, selectivity and efficiency. A perspective on the preclinical development of two hydroxypyridonate actinide decorporation agents, 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO), is presented. The chemical syntheses of both candidate compounds have been optimized for scale-up. Baseline preparation and analytical methods suitable for manufacturing large amounts have been established. Both ligands show much higher actinide-removal efficacy than the currently approved agent, diethylenetriaminepentaacetic acid (DTPA), with different selectivity for the tested isotopes of plutonium, americium, uranium and neptunium. No toxicity is observed in cells derived from three different human tissue sources treated in vitro up to ligand concentrations of 1 mM, and both ligands were well tolerated in rats when orally administered daily at high doses (> 100 μmol kg−1 day−1) over 28 days under good laboratory practice (GLP) guidelines. Both compounds are on an accelerated development pathway towards clinical use. PMID:20699704

  14. Biomimetic actinide chelators: an update on the preclinical development of the orally active hydroxypyridonate decorporation agents 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO).

    PubMed

    Abergel, Rebecca J; Durbin, Patricia W; Kullgren, Birgitta; Ebbe, Shirley N; Xu, Jide; Chang, Polly Y; Bunin, Deborah I; Blakely, Eleanor A; Bjornstad, Kathleen A; Rosen, Chris J; Shuh, David K; Raymond, Kenneth N

    2010-09-01

    The threat of a dirty bomb or other major radiological contamination presents a danger of large-scale radiation exposure of the population. Because major components of such contamination are likely to be actinides, actinide decorporation treatments that will reduce radiation exposure must be a priority. Current therapies for the treatment of radionuclide contamination are limited and extensive efforts must be dedicated to the development of therapeutic, orally bioavailable, actinide chelators for emergency medical use. Using a biomimetic approach based on the similar biochemical properties of plutonium(IV) and iron(III), siderophore-inspired multidentate hydroxypyridonate ligands have been designed and are unrivaled in terms of actinide-affinity, selectivity, and efficiency. A perspective on the preclinical development of two hydroxypyridonate actinide decorporation agents, 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO), is presented. The chemical syntheses of both candidate compounds have been optimized for scale-up. Baseline preparation and analytical methods suitable for manufacturing large amounts have been established. Both ligands show much higher actinide-removal efficacy than the currently approved agent, diethylenetriaminepentaacetic acid (DTPA), with different selectivity for the tested isotopes of plutonium, americium, uranium and neptunium. No toxicity is observed in cells derived from three different human tissue sources treated in vitro up to ligand concentrations of 1 mM, and both ligands were well tolerated in rats when orally administered daily at high doses (>100 micromol kg d) over 28 d under good laboratory practice guidelines. Both compounds are on an accelerated development pathway towards clinical use.

  15. Biomimetic Actinide Chelators: An Update on the Preclinical Development of the Orally Active Hydroxypyridonate Decorporation Agents 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO)

    SciTech Connect

    Durbin, Patricia W.; Kullgren, Birgitta; Ebbe, Shirley N.; Xu, Jide; Chang, Polly Y.; Bunin, Deborah I.; Blakely, Eleanor A.; Bjornstad, Kathleen A.; Rosen, Chris J.; Shuh, David K.; Raymond, Kenneth N.

    2011-07-13

    The threat of a dirty bomb or other major radiological contamination presents a danger of large-scale radiation exposure of the population. Because major components of such contamination are likely to be actinides, actinide decorporation treatments that will reduce radiation exposure must be a priority. Current therapies for the treatment of radionuclide contamination are limited and extensive efforts must be dedicated to the development of therapeutic, orally bioavailable, actinide chelators for emergency medical use. Using a biomimetic approach based on the similar biochemical properties of plutonium(IV) and iron(III), siderophore-inspired multidentate hydroxypyridonate ligands have been designed and are unrivaled in terms of actinide-affinity, selectivity, and efficiency. A perspective on the preclinical development of two hydroxypyridonate actinide decorporation agents, 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO), is presented. The chemical syntheses of both candidate compounds have been optimized for scale-up. Baseline preparation and analytical methods suitable for manufacturing large amounts have been established. Both ligands show much higher actinide-removal efficacy than the currently approved agent, diethylenetriaminepentaacetic acid (DTPA), with different selectivity for the tested isotopes of plutonium, americium, uranium and neptunium. No toxicity is observed in cells derived from three different human tissue sources treated in vitro up to ligand concentrations of 1 mM, and both ligands were well tolerated in rats when orally administered daily at high doses (>100 micromol kg d) over 28 d under good laboratory practice guidelines. Both compounds are on an accelerated development pathway towards clinical use.

  16. Measuring and predicting the transport of actinides and fission product contaminants in unsaturated prairie soil

    NASA Astrophysics Data System (ADS)

    Sims, D. J.

    Soil samples have been taken in 2001 from the area of a 1951 release from an underground storage tank of 6.7 L of an aqueous solution of irradiated uranium (360 GBq). A simulation of the dispersion of the actinides and fission products was conducted in the laboratory using irradiated natural uranium, non-irradiated natural uranium and metal standards dissolved in acidic aqueous solutions and added to soil columns containing uncontaminated prairie soil. The lab soil columns were allowed 12 to 14 months for contaminant transport. Soil samples were analyzed using gamma-ray spectroscopy, neutron activation analysis (NAA) and liquid scintillation counting (LSC) to determine the elemental concentrations of U, Cs and Sr. Diffusion coefficients from the 50 year soil samples and the lab soil samples were determined. The measured diffusion coefficients from the field samples were 3.0 x 10-4 cm2 s-1 (Cs-137), 1.8 x 10-5 cm2 s-1 (U-238) and 2.6 x 10-3 cm2 s-1 (Sr-90) and the values determined from lab simulation were 5 x 10-6 cm 2 s-1 (Cs-137), 3 x 10-5 cm2 s-1 (U-238) and 1.9 x 10-5 cm 2 s-1 (Sr-90). The differences between the sets of diffusion coefficients can be attributed to differences in retardation effects, weather effects and changes in the soil characteristics when transporting, such as porosity. The analytical work showed that Cs-137 content of soil can be determined effectively using gamma-ray spectroscopy; U-238 content can be measured using NAA; and Sr-90 content can be measured using LSC. For non- and low-radioactive species, it was shown that both flame atomic absorption spectrometry (FAAS) and inductively-coupled plasma-mass spectrometry (ICP-MS) gave comparable results for Sr, Cs and Sm, with the average values ranging from 0.5 to 4.5 ppm of each other. The U-238 content results from NAA and from ICP-MS showed general agreement with an average difference of 81.3 ppm on samples having concentrations up to 988.2 ppm. The difference may have been due to matrix

  17. Comparison on the Surface Structure Properties along with Fe(II) and Mn(II) Removal Characteristics of Rice Husk Ash, Inactive Saccharomyces cerevisiae Powder, and Rice Husk.

    PubMed

    Jiang, Zhao; Cao, Bo; Su, Guangxia; Lu, Yan; Zhao, Jiaying; Shan, Dexin; Zhang, Xiuyuan; Wang, Ziyi; Zhang, Ying

    2016-01-01

    This study selected solid wastes, such as rice husk ash (RHA), inactive Saccharomyces cerevisiae powder (ISP), and rice husk (RH), as the potential adsorbents for the removal of Fe(II) and Mn(II) in aqueous solution. The structural characteristics, functional groups, and elemental compositions were determined by scanning electron microscope (SEM) and Fourier translation infrared spectrum (FT-IR) analyses, respectively. Then the influence on the Fe(II) and Mn(II) removing efficiency by the factors, such as pH, adsorbent dosage, initial Fe(II) and Mn(II) concentration, and contact time, was investigated by the static batch test. The adsorption isotherm study results show that Langmuir equation can better fit the Fe(II) and Mn(II) adsorption process by the three adsorbents. The maximum adsorption amounts for Fe(II) were 6.211 mg/g, 4.464 mg/g, and 4.049 mg/g by RHA, ISP, and RH and for Mn(II) were 3.016 mg/g, 2.229 mg/g, and 1.889 mg/g, respectively. The adsorption kinetics results show that the pseudo-second-order kinetic model can better fit the Fe(II) and Mn(II) adsorption process. D-R model and thermodynamic parameters hint that the adsorption processes of Fe(II) and Mn(II) on the three adsorbents took place physically and the processes were feasible, spontaneous, and exothermic.

  18. Comparison on the Surface Structure Properties along with Fe(II) and Mn(II) Removal Characteristics of Rice Husk Ash, Inactive Saccharomyces cerevisiae Powder, and Rice Husk

    PubMed Central

    Jiang, Zhao; Cao, Bo; Su, Guangxia; Lu, Yan; Zhao, Jiaying; Shan, Dexin; Zhang, Xiuyuan; Wang, Ziyi

    2016-01-01

    This study selected solid wastes, such as rice husk ash (RHA), inactive Saccharomyces cerevisiae powder (ISP), and rice husk (RH), as the potential adsorbents for the removal of Fe(II) and Mn(II) in aqueous solution. The structural characteristics, functional groups, and elemental compositions were determined by scanning electron microscope (SEM) and Fourier translation infrared spectrum (FT-IR) analyses, respectively. Then the influence on the Fe(II) and Mn(II) removing efficiency by the factors, such as pH, adsorbent dosage, initial Fe(II) and Mn(II) concentration, and contact time, was investigated by the static batch test. The adsorption isotherm study results show that Langmuir equation can better fit the Fe(II) and Mn(II) adsorption process by the three adsorbents. The maximum adsorption amounts for Fe(II) were 6.211 mg/g, 4.464 mg/g, and 4.049 mg/g by RHA, ISP, and RH and for Mn(II) were 3.016 mg/g, 2.229 mg/g, and 1.889 mg/g, respectively. The adsorption kinetics results show that the pseudo-second-order kinetic model can better fit the Fe(II) and Mn(II) adsorption process. D-R model and thermodynamic parameters hint that the adsorption processes of Fe(II) and Mn(II) on the three adsorbents took place physically and the processes were feasible, spontaneous, and exothermic. PMID:28042571

  19. Multi-podant diglycolamides and room temperature ionic liquid impregnated resins: An excellent combination for extraction chromatography of actinides.

    PubMed

    Gujar, R B; Ansari, S A; Verboom, W; Mohapatra, P K

    2016-05-27

    Extraction chromatography resins, prepared by impregnating two multi-podant diglycolamide ligands, viz. diglycolamide-functionalized calix[4]arene (C4DGA) and tripodal diglycolamide (T-DGA) dissolved in the room temperature ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)amide (RTIL: C4mimTf2N) on Chromosorb-W (an inert solid support), gave excellent results for the removal of trivalent actinides from acidic waste solutions. Distribution coefficient measurements on several metal ions showed selective sorption of Am(III) over hexavalent uranyl ions and other fission product elements such as strontium and cesium. The sorbed metal ions could be efficiently desorbed with a complexing solution containing guanidine carbonate and EDTA buffer. The sorption of Am(III) on both resins followed pseudo-second order rate kinetics with rate constants of 1.37×10(-6) and 6.88×10(-7)g/cpmmin for T-DGA and C4DGA resins, respectively. The metal sorption on both resins indicated the Langmuir monolayer chemisorption phenomenon with Eu(III) sorption capacities of 4.83±0.21 and 0.52±0.05mg per g of T-DGA and C4DGA resins, respectively. The results of column studies show that these resins are of interest for a possible application for the recovery of hazardous trivalent actinides from dilute aqueous solutions.

  20. Comparison of Processes of Transmutation of Long-Lived Actinides in Different Reactors

    SciTech Connect

    Bergelson, B.R.; Gerasimov, A.S.; Kiselev, G.V.; Tikhomirov, G.V.

    2002-07-01

    Efficiency of transmutation of actinides was compared for different types of reactors-transmuters: light water VVER-1000 type reactor, fast breeder BN-600 and Super-Phenix type reactors, as well as high-flux subcritical ADS-800 type facility. Feed with minor actinides extracted from the reactor of VVER-1000 type was supposed. (authors)

  1. Mathematical modeling of the effects of aerobic and anaerobic chelate bioegradation on actinide speciation.

    SciTech Connect

    Banaszak, J.E.; VanBriesen, J.; Rittmann, B.E.; Reed, D.T.

    1998-03-19

    Biodegradation of natural and anthropogenic chelating agents directly and indirectly affects the speciation, and, hence, the mobility of actinides in subsurface environments. We combined mathematical modeling with laboratory experimentation to investigate the effects of aerobic and anaerobic chelate biodegradation on actinide [Np(IV/V), Pu(IV)] speciation. Under aerobic conditions, nitrilotriacetic acid (NTA) biodegradation rates were strongly influenced by the actinide concentration. Actinide-chelate complexation reduced the relative abundance of available growth substrate in solution and actinide species present or released during chelate degradation were toxic to the organisms. Aerobic bio-utilization of the chelates as electron-donor substrates directly affected actinide speciation by releasing the radionuclides from complexed form into solution, where their fate was controlled by inorganic ligands in the system. Actinide speciation was also indirectly affected by pH changes caused by organic biodegradation. The two concurrent processes of organic biodegradation and actinide aqueous chemistry were accurately linked and described using CCBATCH, a computer model developed at Northwestern University to investigate the dynamics of coupled biological and chemical reactions in mixed waste subsurface environments. CCBATCH was then used to simulate the fate of Np during anaerobic citrate biodegradation. The modeling studies suggested that, under some conditions, chelate degradation can increase Np(IV) solubility due to carbonate complexation in closed aqueous systems.

  2. Actinide (An = Th-Pu) dimetallocenes: promising candidates for metal-metal multiple bonds.

    PubMed

    Wang, Cong-Zhi; Gibson, John K; Lan, Jian-Hui; Wu, Qun-Yan; Zhao, Yu-Liang; Li, Jun; Chai, Zhi-Fang; Shi, Wei-Qun

    2015-10-21

    Synthesis of complexes with direct actinide-actinide (An-An) bonding is an experimental 'holy grail' in actinide chemistry. In this work, a series of actinide dimetallocenes An2Cp (Cp(*) = C5(CH3)5, An = Th-Pu) with An-An multiple bonds have been systematically investigated using quantum chemical calculations. The coaxial Cp(*)-An-An-Cp(*) structures are found to be the most stable species for all the dimetallocenes. A Th-Th triple bond is predicted in the Th2Cp complex, and the calculated An-An bond orders decrease across the actinide series from Pa to Pu. The covalent character of the An-An bonds is analyzed by using natural bond orbitals (NBO), molecular orbitals (MO), the quantum theory of atoms in molecules (QTAIM), and electron density difference (EDD). While Th 6d orbitals dominate the Th-Th bonds in Th2Cp, the An 6d-orbital characters decrease and 5f-orbital characters increase for complexes from Pa2Cp to Pu2Cp. All these actinide dimetallocenes are stable in the gas phase relative to the AnCp(*) reference at room temperature. Based on the reactions of AnCp and An, Th2Cp, Pa2Cp and possibly also U2Cp should be accessible as isolated molecules under suitable synthetic conditions. Our results shed light on the molecular design of ligands for stabilizing actinide-actinide multiple bonds.

  3. Dose-dependent efficacy and safety toxicology of hydroxypyridinonate actinide decorporation agents in rodents: towards a safe and effective human dosing regimen.

    PubMed

    Bunin, Deborah I; Chang, Polly Y; Doppalapudi, Rupa S; Riccio, Edward S; An, Dahlia; Jarvis, Erin E; Kullgren, Birgitta; Abergel, Rebecca J

    2013-02-01

    Two hydroxypyridinone-containing actinide decorporation agents, 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO), are being developed for the treatment of internal actinide contamination by chelation therapy. Dose-response efficacy profiles in mice were established for the removal of intravenously injected (238)Pu and (241)Am after parenteral and oral treatment with these chelators. In both cases, presumed efficacious doses promoted substantially greater actinide elimination rates than the currently approved agent, diethylenetriamine-pentaacetic acid, considering two different interspecies scaling methods for the conversion of human doses to equivalent rodent dose levels. In addition, genotoxicity of both ligands was assessed using the Salmonella/ Escherichia coli /microsome plate incorporation test and the Chinese hamster ovary cell chromosome aberration assay, showing that neither ligand is genotoxic, in the presence and absence of metabolic activation. Finally, maximum tolerated dose studies were performed in rats for seven consecutive daily oral administrations with the chelators, confirming the safety of the presumed efficacious doses for 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO). The results of these studies add to the growing body of evidence that both decorporation agents have remarkable decorporation efficacy properties and promising safety toxicology profiles. These results are necessary components of the regulatory approval process and will help determine the optimal human dosing regimens for the treatment of internal radionuclide contamination.

  4. Dose-Dependent Efficacy and Safety Toxicology of Hydroxypyridinonate Actinide Decorporation Agents in Rodents: Towards a Safe and EffectiveHuman Dosing Regimen

    PubMed Central

    Bunin, Deborah I.; Chang, Polly Y.; Doppalapudi, Rupa S.; Riccio, Edward S.; An, Dahlia; Jarvis, Erin E.; Kullgren, Birgitta; Abergel, Rebecca J.

    2013-01-01

    Two hydroxypyridinone-containing actinide decorporation agents, 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO), are being developed for the treatment of internal actinide contamination by chelation therapy. Dose-response efficacy profiles in mice were established for the removal of intravenously injected 238Pu and 241Am after parenteral and oral treatment with these chelators. In both cases, presumed efficacious doses promoted substantially greater actinide elimination rates than the currently approved agent, diethylenetriamine-pentaacetic acid, considering two different interspecies scaling methods for the conversion of human doses to equivalent rodent dose levels. In addition, genotoxicity of both ligands was assessed using the Salmonella/Escherichia coli/microsome plate incorporation test and the Chinese hamster ovary cell chromosome aberration assay, showing that neither ligand is genotoxic, in the presence and absence of metabolic activation. Finally, maximum tolerated dose studies were performed in rats for seven consecutive daily oral administrations with the chelators, confirming the safety of the presumed efficacious doses for 3,4,3-LI(1,2-HOPO) and 5-LIO(Me-3,2-HOPO). The results of these studies add to the growing body of evidence that both decorporation agents have remarkable decorporation efficacy properties and promising safety toxicology profiles. These results are necessary components of the regulatory approval process and will help determine the optimal human dosing regimens for the treatment of internal radionuclide contamination. PMID:23289385

  5. Final Report on Actinide Glass Scintillators for Fast Neutron Detection

    SciTech Connect

    Bliss, Mary; Stave, Jean A.

    2012-10-01

    This is the final report of an experimental investigation of actinide glass scintillators for fast-neutron detection. It covers work performed during FY2012. This supplements a previous report, PNNL-20854 “Initial Characterization of Thorium-loaded Glasses for Fast Neutron Detection” (October 2011). The work in FY2012 was done with funding remaining from FY2011. As noted in PNNL-20854, the glasses tested prior to July 2011 were erroneously identified as scintillators. The decision was then made to start from “scratch” with a literature survey and some test melts with a non-radioactive glass composition that could later be fabricated with select actinides, most likely thorium. The normal stand-in for thorium in radioactive waste glasses is cerium in the same oxidation state. Since cerium in the 3+ state is used as the light emitter in many scintillating glasses, the next most common substitute was used: hafnium. Three hafnium glasses were melted. Two melts were colored amber and a third was clear. It barely scintillated when exposed to alpha particles. The uses and applications for a scintillating fast neutron detector are important enough that the search for such a material should not be totally abandoned. This current effort focused on actinides that have very high neutron capture energy releases but low neutron capture cross sections. This results in very long counting times and poor signal to noise when working with sealed sources. These materials are best for high flux applications and access to neutron generators or reactors would enable better test scenarios. The total energy of the neutron capture reaction is not the only factor to focus on in isotope selection. Many neutron capture reactions result in energetic gamma rays that require large volumes or high densities to detect. If the scintillator is to separate neutrons from gamma rays, the capture reactions should produce heavy particles and few gamma rays. This would improve the detection of a

  6. Detection of the actinides and cesium from environmental samples

    NASA Astrophysics Data System (ADS)

    Snow, Mathew Spencer

    Detection of the actinides and cesium in the environment is important for a variety of applications ranging from environmental remediation to safeguards and nuclear forensics. The utilization of multiple different elemental concentrations and isotopic ratios together can significantly improve the ability to attribute contamination to a unique source term and/or generation process; however, the utilization of multiple elemental "signatures" together from environmental samples requires knowledge of the impact of chemical fractionation for various elements under a variety of environmental conditions (including predominantly aqueous versus arid conditions). The research reported in this dissertation focuses on three major areas: 1. Improving the understanding of actinide-mineral interactions at ultra-low concentrations. Chapter 2 reports a batch sorption and modeling study of Np(V) sorption to the mineral goethite from attomolar to micromolar concentrations. 2. Improving the detection capabilities for Thermal Ionization Mass Spectrometry (TIMS) analyses of ultra-trace cesium from environmental samples. Chapter 4 reports a new method which significantly improves the chemical yields, purification, sample processing time, and ultimately, the detection limits for TIMS analyses of femtogram quantities of cesium from a variety of environmental sample matrices. 3. Demonstrating how actinide and cesium concentrations and isotopic ratios from environmental samples can be utilized together to determine a wealth of information including environmental transport mechanisms (e.g. aqueous versus arid transport) and information on the processes which generated the original material. Chapters1, 3 and 5 demonstrate these principles using Pu, Am, Np, and Cs concentrations and isotopic ratios from contaminated soils taken near the Subsurface Disposal Area (SDA) of Idaho National Laboratory (INL) (a low level radioactive waste disposal site in southeastern Idaho).

  7. Use of high gradient magnetic separation for actinide application

    SciTech Connect

    Avens, L.R.; Worl, L.A.; Padilla, D.D.

    1996-08-01

    Decontamination of materials such as soils or waste water that contain radioactive isotopes, heavy metals, or hazardous components is a subject of great interest. Magnetic separation is a physical separation process that segregates materials on the basis of magnetic susceptibility. Because the process relies on physical properties, separations can be achieved while producing a minimum of secondary waste. Most traditional physical separation processes effectively treat particles larger than 70 microns. In many situations, the radioactive contaminants are found concentrated in the fine particle size fraction of less than 20 microns. For effective decontamination of the fine particle size fraction most current operations resort to chemical dissolution methods for treatment. High gradient magnetic separation (HGMS) is able to effectively treat particles from 90 to {approximately}0.1 micron in diameter. The technology is currently used on the 60 ton per hour scale in the kaolin clay industry. When the field gradient is of sufficiently high intensity, paramagnetic particles can be physically captured and separated from extraneous nonmagnetic material. Because all actinide compounds are paramagnetic, magnetic separation of actinide containing mixtures is feasible. The advent of reliable superconducting magnets also makes magnetic separation of weakly paramagnetic species attractive. HGMS work at Los Alamos National Laboratory (LANL) is being developed for soil remediation, waste water treatment and treatment of actinide chemical processing residues. LANL and Lockheed Environmental Systems and Technologies Company (LESAT) have worked on a co-operative research and development agreement (CRADA) to develop HGMS for radioactive soil decontamination. The program is designed to transfer HGMS from the laboratory and other industries for the commercial treatment of radioactive contaminated materials. 9 refs., 2 figs., 2 tabs.

  8. Internal conversion in energy dispersive X-ray analysis of actinide-containing materials.

    PubMed

    Wiss, Thierry; Thiele, Hartmut; Cremer, Bert; Ray, Ian

    2007-06-01

    The use of X-ray elemental analysis tools like energy dispersive X-ray (EDS) is described in the context of the investigation of nuclear materials. These materials contain radioactive elements, particularly alpha-decaying actinides that affect the quantitative EDS measurement by producing interferences in the X-ray spectra. These interferences originating from X-ray emission are the result of internal conversion by the daughter atoms from the alpha-decaying actinides. The strong interferences affect primarily the L X-ray lines from the actinides (in the typical energy range used for EDS analysis) and would require the use of the M lines. However, it is typically at the energy of the actinide's M lines that the interferences are dominant. The artifacts produced in the X-ray analysis are described and illustrated by some typical examples of analysis of actinide-bearing material.

  9. Recovery of the actinides by electrochemical methods in molten chlorides using solid aluminium cathode

    SciTech Connect

    Malmbeck, R.; Mendes, E.; Serp, J.; Soucek, P.; Glatz, J.P.; Cassayre, L.

    2007-07-01

    An electrorefining process in molten chloride salts is being developed at ITU to reprocess the spent nuclear fuel. According to the thermochemical properties of the system, aluminium is the most promising electrode material for the separation of actinides (An) from lanthanides (Ln). The actinides are selectively reduced from the fission products and stabilized by the formation of solid and compact actinide-aluminium alloys with the reactive cathode material. In this work, the maximum loading of aluminium with actinides was investigated by potentiostatic and galvano-static electrorefining of U-Pu- Zr alloys. A very high aluminium capacity was achieved, as the average loading was 1.6 g of U and Pu into 1 g of aluminium and the maximum achieved loading was 2.3 g. For recovery of the actinides from aluminium, a process based on chlorination and a subsequent sublimation of AlCl{sub 3} is proposed. (authors)

  10. Actinide neutron-induced fission cross section measurements at LANSCE

    SciTech Connect

    Tovesson, Fredrik K; Laptev, Alexander B; Hill, Tony S

    2010-01-01

    Fission cross sections of a range of actinides have been measured at the Los Alamos Neutron Science Center (LANSCE) in support of nuclear energy applications in a wide energy range from sub-thermal energies up to 200 MeV. A parallel-plate ionization chamber are used to measure fission cross sections ratios relative to the {sup 235}U standard while incident neutron energies are determined using the time-of-flight method. Recent measurements include the {sup 233,238}U, {sup 239-242}Pu and {sup 243}Am neutron-induced fission cross sections. Obtained data are presented in comparison with ex isting evaluations and previous data.

  11. Vitrification of actinide solutions in SRS separations facilities

    SciTech Connect

    Minichan, R.L.; Ramsey, W.G.

    1995-09-01

    The actinide vitrification system being developed at SRS provides the capability to convert specialized or unique forms of nuclear material into a stable solid glass product that can be safely shipped, stored or reprocessed according to the DOE complex mission. This project is an application of technology developed through funds from the Office of Technology Development (OTD). This technology is ideally suited for vitrifying relatively small quantities of fissile or special nuclear material since it is designed to be critically safe. Successful demonstration of this system to safely vitrify radioactive material could open up numerous opportunities for transferring this technology to applications throughout the DOE complex.

  12. Status of the lanthanides and actinides in the periodic table

    SciTech Connect

    Holden, N.E.

    1985-01-01

    In extended discussions and correspondence with Ekkehard Fluck, the author was made aware of a problem with the Periodic Table, i.e., which element should be shown in the main table as the representative of the lanthanide series and the actinide series. In earlier discussion, he came to the conclusion that lanthanum and actinium are not the elements which should appear, but rather lutetium and lawrencium are more appropriate for inclusion in their place. This paper will attempt to justify the reasons for the above conclusions. 4 refs.

  13. Isotopic biases for actinide-only burnup credit

    SciTech Connect

    Rahimi, M.; Lancaster, D.; Hoeffer, B.; Nichols, M.

    1997-04-01

    The primary purpose of this paper is to present the new methodology for establishing bias and uncertainty associated with isotopic prediction in spent fuel assemblies for burnup credit analysis. The analysis applies to the design of criticality control systems for spent fuel casks. A total of 54 spent fuel samples were modeled and analyzed using the Shielding Analyses Sequence (SAS2H). Multiple regression analysis and a trending test were performed to develop isotopic correction factors for 10 actinide burnup credit isotopes. 5 refs., 1 tab.

  14. Detection of Actinides via Nuclear Isomer De-Excitation

    SciTech Connect

    Francy, Christopher J.

    2009-07-01

    This dissertation discusses a data collection experiment within the Actinide Isomer Identification project (AID). The AID project is the investigation of an active interrogation technique that utilizes nuclear isomer production, with the goal of assisting in the interdiction of illicit nuclear materials. In an attempt to find and characterize isomers belonging to 235U and its fission fragments, a 232Th target was bombarded with a monoenergetic 6Li ion beam, operating at 45 MeV.

  15. Plasma mass filtering for separation of actinides from lanthanides

    NASA Astrophysics Data System (ADS)

    Gueroult, R.; Fisch, N. J.

    2014-06-01

    Separating lanthanides from actinides is a key process in reprocessing nuclear spent fuel. Plasma mass filters, which operate on dissociated elements, offer conceptual advantages for such a task as compared with conventional chemical methods. The capabilities of a specific plasma mass filter concept, called the magnetic centrifugal mass filter, are analyzed within this particular context. Numerical simulations indicate separation of americium ions from a mixture of lanthanides ions for plasma densities of the order of 1012 cm-3, and ion temperatures of about 10 eV. In light of collision considerations, separating small fractions of heavy elements from a larger volume of lighter ones is shown to enhance the separation capabilities.

  16. Local structure in solid solutions of stabilised zirconia with actinide dioxides (UO{sub 2}, NpO{sub 2})

    SciTech Connect

    Walter, Marcus; Somers, Joseph; Bouexiere, Daniel; Rothe, Joerg

    2011-04-15

    The local structure of (Zr,Lu,U)O{sub 2-x} and (Zr,Y,Np)O{sub 2-x} solid solutions has been investigated by extended X-ray absorption fine structure (EXAFS). Samples were prepared by mixing reactive (Zr,Lu)O{sub 2-x} and (Zr,Y)O{sub 2-x} precursor materials with the actinide oxide powders, respectively. Sintering at 1600 {sup o}C in Ar/H{sub 2} yields a fluorite structure with U(IV) and Np(IV). As typical for stabilised zirconia the metal-oxygen and metal-metal distances are characteristic for the different metal ions. The bond lengths increase with actinide concentration, whereas highest adaptation to the bulk stabilised zirconia structure was observed for U---O and Np---O bonds. The Zr---O bond shows only a slight increase from 2.14 A at 6 mol% actinide to 2.18 A at infinite dilution in UO{sub 2} and NpO{sub 2}. The short interatomic distance between Zr and the surrounding oxygen and metal atoms indicate a low relaxation of Zr with respect to the bulk structure, i.e. a strong Pauling behaviour. -- Graphical abstract: Metal-oxygen bond distances in (Zr,Lu,U)O{sub 2-x} solid solutions with different oxygen vacancy concentrations (Lu/Zr=1 and Lu/Zr=0.5). Display Omitted Research Highlights: {yields} EXAFS indicates high U and Np adaption to the bulk structure of stabilised zirconia. {yields} Zr---O bond length is 2.18 A at infinite Zr dilution in UO{sub 2} and NpO{sub 2}. {yields} Low relaxation (strong Pauling behaviour) of Zr explains its low solubility in UO{sub 2}.

  17. Adenoid removal

    MedlinePlus

    ... This does not cause problems most of the time. Alternative Names Adenoidectomy; Removal of adenoid glands Images Adenoid removal - series References Wetmore RF. Tonsils and adenoids. In: Kliegman ...

  18. Thermal- and Fast-Spectrum Molten Salt Reactors for Actinide Burning and Fuel Production

    SciTech Connect

    Forsberg, Charles W

    2007-01-01

    In a molten salt reactor (MSR), the fuel is dissolved in a fluoride salt coolant. The technology was partly developed in the 1950s and 1960s. With changing goals for advanced reactors and new technologies, there is currently a renewed interest in MSRs. The new technologies include (1) Brayton power cycles (rather than steam cycles) that eliminate many of the historical challenges in building MSRs and (2) the conceptual development of several fast-spectrum MSRs that have large negative temperature and void coefficients, a unique safety characteristic not found in solid-fuel fast reactors. Earlier MSRs were thermal-neutron-spectrum reactors. Compared with solid-fueled reactors, MSR systems have lower fissile inventories, no radiation damage constraint on attainable fuel burnup, no spent nuclear fuel, no requirement to fabricate and handle solid fuel, and a single isotopic composition of fuel in the reactor. These and other characteristics may enable MSRs to have potentially unique capabilities and competitive economics for actinide burning and extending fuel resources. The status, unique characteristics, and recent worldwide advances in MSRs are described.

  19. Thermal- and fast-spectrum molten salt reactors for actinide burning and fuel production

    SciTech Connect

    Forsberg, Charles W.

    2007-07-01

    In a molten salt reactor (MSR), the fuel is dissolved in a fluoride salt coolant. The technology was partly developed in the 1950's and 1960's. With changing goals for advanced reactors and new technologies, there is currently a renewed interest in MSRs. The new technologies include (1) Brayton power cycles (rather than steam cycles) that eliminate many of the historical challenges in building MSRs and (2) the conceptual development of several fast-spectrum MSRs that have large negative temperature and void coefficients, a unique safety characteristic not found in solid-fuel fast reactors. Earlier MSRs were thermal-neutron-spectrum reactors. Compared with solid-fueled reactors, MSR systems have lower fissile inventories, no radiation damage constraint on attainable fuel burnup, no spent nuclear fuel, no requirement to fabricate and handle solid fuel, and a single isotopic composition of fuel in the reactor. These and other characteristics may enable MSRs to have potentially unique capabilities and competitive economics for actinide burning and extending fuel resources. The status, unique characteristics, and recent worldwide advances in MSRs are described. (author)

  20. Biosorption characteristics of Aspergillus flavus biomass for removal of Pb(II) and Cu(II) ions from an aqueous solution.

    PubMed

    Akar, Tamer; Tunali, Sibel

    2006-10-01

    The Pb(II) and Cu(II) biosorption characteristics of Aspergillus flavus fungal biomass were examined as a function of initial pH, contact time and initial metal ion concentration. Heat inactivated (killed) biomass was used in the determination of optimum conditions before investigating the performance of pretreated biosorbent. The maximum biosorption values were found to be 13.46 +/- 0.99 mg/g for Pb(II) and 10.82 +/- 1.46 mg/g for Cu(II) at pH 5.0 +/- 0.1 with an equilibrium time of 2 h. Detergent, sodium hydroxide and dimethyl sulfoxide pretreatments enhanced the biosorption capacity of biomass in comparison with the heat inactivated biomass. The biosorption data obtained under the optimum conditions were well described by the Freundlich isotherm model. Competitive biosorption of Pb(II) and Cu(II) ions was also investigated to determine the selectivity of the biomass. The results indicated that A. flavus is a suitable biosorbent for the removal of Pb(II) and Cu(II) ions from aqueous solution.

  1. Unloading Characteristics of Sand-drift in Wind-shallow Areas along Railway and the Effect of Sand Removal by Force of Wind.

    PubMed

    Cheng, Jian-Jun; Xin, Guo-Wei; Zhi, Ling-Yan; Jiang, Fu-Qiang

    2017-01-25

    Wind-shield walls decrease the velocity of wind-drift sand flow in transit. This results in sand accumulating in the wind-shadow zone of both windshield wall and track line, causing severe sand sediment hazard. This study reveals the characteristics of sand accumulation and the laws of wind-blown sand removal in the wind-shadow areas of three different types of windshield walls, utilizing three-dimensional numerical simulations and wind tunnel experiments and on-site sand sediment tests. The results revealed the formation of apparent vortex and acceleration zones on the leeward side of solid windshield walls. For uniform openings, the vortex area moved back and narrowed. When bottom-opening windshield walls were adopted, the track-supporting layer at the step became a conflux acceleration zone, forming a low velocity vortex zone near the track line. At high wind speeds, windshield walls with bottom-openings achieved improved sand dredging. Considering hydrodynamic mechanisms, the flow field structure on the leeward side of different types of windshield structures is a result of convergence and diffusion of fluids caused by an obstacle. This convergence and diffusion effect of air fluid is more apparent at high wind velocities, but not obvious at low wind velocities.

  2. Unloading Characteristics of Sand-drift in Wind-shallow Areas along Railway and the Effect of Sand Removal by Force of Wind

    NASA Astrophysics Data System (ADS)

    Cheng, Jian-Jun; Xin, Guo-Wei; Zhi, Ling-Yan; Jiang, Fu-Qiang

    2017-01-01

    Wind-shield walls decrease the velocity of wind-drift sand flow in transit. This results in sand accumulating in the wind-shadow zone of both windshield wall and track line, causing severe sand sediment hazard. This study reveals the characteristics of sand accumulation and the laws of wind-blown sand removal in the wind-shadow areas of three different types of windshield walls, utilizing three-dimensional numerical simulations and wind tunnel experiments and on-site sand sediment tests. The results revealed the formation of apparent vortex and acceleration zones on the leeward side of solid windshield walls. For uniform openings, the vortex area moved back and narrowed. When bottom-opening windshield walls were adopted, the track-supporting layer at the step became a conflux acceleration zone, forming a low velocity vortex zone near the track line. At high wind speeds, windshield walls with bottom-openings achieved improved sand dredging. Considering hydrodynamic mechanisms, the flow field structure on the leeward side of different types of windshield structures is a result of convergence and diffusion of fluids caused by an obstacle. This convergence and diffusion effect of air fluid is more apparent at high wind velocities, but not obvious at low wind velocities.

  3. Zeolite formation from coal fly ash and heavy metal ion removal characteristics of thus-obtained Zeolite X in multi-metal systems.

    PubMed

    Jha, Vinay Kumar; Nagae, Masahiro; Matsuda, Motohide; Miyake, Michihiro

    2009-06-01

    Zeolitic materials have been prepared from coal fly ash as well as from a SiO(2)-Al(2)O(3) system upon NaOH fusion treatment, followed by subsequent hydrothermal processing at various NaOH concentrations and reaction times. During the preparation process, the starting material initially decomposed to an amorphous form, and the nucleation process of the zeolite began. The carbon content of the starting material influenced the formation of the zeolite by providing an active surface for nucleation. Zeolite A (Na-A) was transformed into zeolite X (Na-X) with increasing NaOH concentration and reaction time. The adsorption isotherms of the obtained Na-X based on the characteristics required to remove heavy ions such as Ni(2+), Cu(2+), Cd(2+) and Pb(2+) were examined in multi-metal systems. Thus obtained experimental data suggests that the Langmuir and Freundlich models are more accurate compared to the Dubinin-Kaganer-Radushkevich (DKR) model. However, the sorption energy obtained from the DKR model was helpful in elucidating the mechanism of the sorption process. Further, in going from a single- to multi-metal system, the degree of fitting for the Freundlich model compared with the Langmuir model was favored due to its basic assumption of a heterogeneity factor. The Extended-Langmuir model may be used in multi-metal systems, but gives a lower value for equilibrium sorption compared with the Langmuir model.

  4. Unloading Characteristics of Sand-drift in Wind-shallow Areas along Railway and the Effect of Sand Removal by Force of Wind

    PubMed Central

    Cheng, Jian-jun; Xin, Guo-Wei; Zhi, Ling-yan; Jiang, Fu-qiang

    2017-01-01

    Wind-shield walls decrease the velocity of wind-drift sand flow in transit. This results in sand accumulating in the wind-shadow zone of both windshield wall and track line, causing severe sand sediment hazard. This study reveals the characteristics of sand accumulation and the laws of wind-blown sand removal in the wind-shadow areas of three different types of windshield walls, utilizing three-dimensional numerical simulations and wind tunnel experiments and on-site sand sediment tests. The results revealed the formation of apparent vortex and acceleration zones on the leeward side of solid windshield walls. For uniform openings, the vortex area moved back and narrowed. When bottom-opening windshield walls were adopted, the track-supporting layer at the step became a conflux acceleration zone, forming a low velocity vortex zone near the track line. At high wind speeds, windshield walls with bottom-openings achieved improved sand dredging. Considering hydrodynamic mechanisms, the flow field structure on the leeward side of different types of windshield structures is a result of convergence and diffusion of fluids caused by an obstacle. This convergence and diffusion effect of air fluid is more apparent at high wind velocities, but not obvious at low wind velocities. PMID:28120915

  5. Actinide Partitioning and Radiation Effects in U(VI)-Solids: Thermodynamic & Mechanistic Study

    SciTech Connect

    Clark, Sue B.; Ewing, Rodney C.

    2010-05-20

    In most environmental systems, the mobility of a contaminant metal cation depends on its partitioning between the solid and solution phase. At the molecular level, partitioning to the solid phase is controlled by the coordination requirements of the contaminant cation. In this work, we developed linear free energy relationships (LFERs) to describe the partitioning of non-U actinide cations to U(VI) solid phases in a radiation environment; the LFERs are based on knowledge of the actinide coordination environment in or on the surface of the U(VI) solid, and the impact of ionizing radiation on the atomic interactions of the non-U actinide cations. LFERs were established for predicting (1) free energies of formation of pure U(VI) solids and solid solutions with non-U actinide cations, and (2) the adsorption of non-U actinide cations to pure U(VI) solids. We demonstrated the application of LFERs developed from knowledge of molecular structures of U(VI) solid phases to predict the predominance of U(VI) oxide hydrate and silicate solid phases as a function of geochemical conditions. We extended our efforts to define LFERs for U(VI) phosphate solids, and included the impact of actinide self-radiation on all LFERs for free energies of formation for U(VI) solids. We also defined LFERs for the formation of solid solutions between the U(VI) solids and non-U actinide cations such as Th, Np, Pu, Am, and Cm. We demonstrated the importance of nanocrystalline solids in the solid phase partitioning of these non-U actinide cations. For those solid solutions formed, we investigated the impact of ionizing radiation on the stability of those phases, and the release of the non-U actinide cations from the solids. Finally, developed LFERs to predict the adsorption of the non-U actinide cations to the surfaces of U(VI) oxide hydrates and U(VI) phosphates. We determined adsorption constants and coordination requirements for actinide adsorption to U(VI) solid phases. We determined

  6. Reflections on the criticality of special actinide elements

    SciTech Connect

    Clayton, E.D.

    1987-04-01

    During recent years, the list of nuclides known to be capable of supporting a chain reaction has substantially increased. Since the criticality aspects for some of these nuclides differ in important respects from those of the most common fissile nuclides, /sup 235//sub 92/U, and /sup 239//sub 94/Pu, a new term, ''fissible'' was recently proposed in nuclear engineering to help distinguish differences. Activation energies for fission have been calculated for 41 of the actinide isotopes which are grouped according to four types of nuclides, those with even-Z, even-N, odd-Z, odd-N, odd-Z, even-N, and even-Z, odd-N. With the possible exception of /sup 237//sub 92/U, all fissible isotopes listed have even N. The activation energy for fission is less in the case of the even-Z, even-N isotopes, but almost without eception it is the odd-N isotopes that undergo fission with thermal neutrons and which constitute the principal criticality problem. This paper reviews the criticality and fissionability aspects of the fissile and fissible actinide isotopes. The criticality of aqueous mixtures of fissile and fissible isotopes also is briefly discussed, including limits for criticality control.

  7. Heat capacities of lanthanide and actinide monazite-type ceramics

    NASA Astrophysics Data System (ADS)

    Kowalski, Piotr M.; Beridze, George; Vinograd, Victor L.; Bosbach, Dirk

    2015-09-01

    (Ln, An)xPO4 monazite-type ceramics are considered as potential matrices for the disposal of nuclear waste. In this study we computed the heat capacities and the standard entropies of these compounds using density functional perturbation theory. The calculations of lanthanide monazites agree well with the existing experimental data and provide information on the variation of the standard heat capacities and entropies along the lanthanide series. The results for AnPO4 monazites are similar to those obtained for the isoelectronic lanthanide compounds. This suggests that the missing thermodynamic data on actinide monazites could be similarly computed or assessed based on the properties of their lanthanide analogs. However, the computed heat capacity of PuPO4 appear to be significantly lower than the measured data. We argue that this discrepancy might indicate potential problems with the existing experimental data or with their interpretation. This shows a need for further experimental studies of the heat capacities of actinide-bearing, monazite-type ceramics.

  8. Effects of actinide burning on waste disposal at Yucca Mountain

    SciTech Connect

    Hirschfelder, J.

    1992-07-01

    Release rates of 15 radionuclides from waste packages expected to result from partitioning and transmutation of Light-Water Reactor (LWR) and Actinide-Burning Liquid-Metal Reactor (ALMR) spent fuel are calculated and compared to release rates from standard LWR spent fuel packages. The release rates are input to a model for radionuclide transport from the proposed geologic repository at Yucca Mountain to the water table. Discharge rates at the water table are calculated and used in a model for transport to the accessible environment, defined to be five kilometers from the repository edge. Concentrations and dose rates at the accessible environment from spent fuel and wastes from reprocessing, with partitioning and transmutation, are calculated. Partitioning and transmutation of LWR and ALMR spent fuel reduces the inventories of uranium, neptunium, plutonium, americium and curium in the high-level waste by factors of 40 to 500. However, because release rates of all of the actinides except curium are limited by solubility and are independent of package inventory, they are not reduced correspondingly. Only for curium is the repository release rate much lower for reprocessing wastes.

  9. Energy-Dependent Fission Q Values Generalized for All Actinides

    SciTech Connect

    Vogt, R

    2008-09-25

    We generalize Madland's parameterization of the energy release in fission to obtain the dependence of the fission Q values on incident neutron energy, E{sub n}, for all major and minor actinides. These Q(E{sub n}) parameterizations are included in the ENDL2008 release. This paper describes calculations of energy-dependent fission Q values based on parameterizations of the prompt energy release in fission [1], developed by Madland [1] to describe the prompt energy release in neutron-induced fission of {sup 235}U, {sup 238}U, and {sup 239}Pu. The energy release is then related to the energy deposited during fission so that experimentally measurable quantities can be used to obtain the Q values. A discussion of these specific parameterizations and their implementation in the processing code for Monte Carlo neutron transport, MCFGEN, [2] is described in Ref. [3]. We extend this model to describe Q(E) for all actinides, major and minor, in the Evaluated Nuclear Data Library (ENDL) 2008 release, ENDL2008.

  10. The EBR-II X501 Minor Actinide Burning Experiment

    SciTech Connect

    W. J. Carmack; M. K. Meyer; S. L. Hayes; H. Tsai

    2008-01-01

    The X501 experiment was conducted in EBR II as part of the Integral Fast Reactor program to demonstrate minor actinide burning through the use of a homogeneous recycle scheme. The X501 subassembly contained two metallic fuel elements loaded with relatively small quantities of americium and neptunium. Interest in the behavior of minor actinides (MA) during fuel irradiation has prompted further examination of existing X501 data and generation of new data where needed in support of the U.S. waste transmutation effort. The X501 experiment is one of the few MA bearing fuel irradiation tests conducted worldwide, and knowledge can be gained by understanding the changes in fuel behavior due to addition of MAs. Of primary interest are the effect of the MAs on fuel cladding chemical interaction and the redistribution behavior of americium. The quantity of helium gas release from the fuel and any effects of helium on fuel performance are also of interest. It must be stressed that information presented at this time is based on the limited PIE conducted in 1995–1996 and, currently, represents a set of observations rather than a complete understanding of fuel behavior. This report provides a summary of the X501 fabrication, characterization, irradiation, and post irradiation examination.

  11. Actinide Solubility and Speciation in the WIPP [PowerPoint

    SciTech Connect

    Reed, Donald T.

    2015-11-02

    The presentation begins with the role and need for nuclear repositories (overall concept, international updates (Sweden, Finland, France, China), US approach and current status), then moves on to the WIPP TRU repository concept (design, current status--safety incidents of February 5 and 14, 2014, path forward), and finally considers the WIPP safety case: dissolved actinide concentrations (overall approach, oxidation state distribution and redox control, solubility of actinides, colloidal contribution and microbial effects). The following conclusions are set forth: (1) International programs are moving forward, but at a very slow and somewhat sporadic pace. (2) In the United States, the Salt repository concept, from the perspective of the long-term safety case, remains a viable option for nuclear waste management despite the current operational issues/concerns. (3) Current model/PA prediction (WIPP example) are built on redundant conservatisms. These conservatisms are being addressed in the ongoing and future research to fill existing data gaps--redox control of plutonium by Fe(0, II), thorium (analog) solubility studies in simulated brine, contribution of intrinsic and biocolloids to the mobile concentration, and clarification of microbial ecology and effects.

  12. Supercritical fluid extraction and separation of uranium from other actinides.

    PubMed

    Quach, Donna L; Mincher, Bruce J; Wai, Chien M

    2014-06-15

    The feasibility of separating U from nitric acid solutions of mixed actinides using tri-n-butylphosphate (TBP)-modified supercritical fluid carbon dioxide (sc-CO2) was investigated. The actinides U, Np, Pu, and Am were extracted into sc-CO2 modified with TBP from a range of nitric acid concentrations, in the absence of, or in the presence of, a number of traditional reducing and/or complexing agents to demonstrate the separation of these metals from U under sc-CO2 conditions. The separation of U from Pu using sc-CO2 was successful at nitric acid concentrations of less than 3M in the presence of acetohydroxamic acid (AHA) or oxalic acid (OA) to mitigate Pu extraction, and the separation of U from Np was successful at nitric acid concentrations of less than 1M in the presence of AHA, OA, or sodium nitrite to mitigate Np extraction. Americium was not well extracted under any condition studied.

  13. Actinide production from xenon bombardments of curium-248

    SciTech Connect

    Welch, R.B.

    1985-01-01

    Production cross sections for many actinide nuclides formed in the reaction of /sup 129/Xe and /sup 132/Xe with /sup 248/Cm at bombarding energies slightly above the coulomb barrier were determined using radiochemical techniques to isolate these products. These results are compared with cross sections from a /sup 136/Xe + /sup 248/Cm reaction at a similar energy. When compared to the reaction with /sup 136/Xe, the maxima in the production cross section distributions from the more neutron deficient projectiles are shifted to smaller mass numbers, and the total cross section increases for the production of elements with atomic numbers greater than that of the target, and decreases for lighter elements. These results can be explained by use of a potential energy surface (PES) which illustrates the effect of the available energy on the transfer of nucleons and describes the evolution of the di-nuclear complex, an essential feature of deep-inelastic reactions (DIR), during the interaction. The other principal reaction mechanism is the quasi-elastic transfer (QE). Analysis of data from a similar set of reactions, /sup 129/Xe, /sup 132/Xe, and /sup 136/Xe with /sup 197/Au, aids in explaining the features of the Xe + Cm product distributions, which are additionally affected by the depletion of actinide product yields due to deexcitation by fission. The PES is shown to be a useful tool to predict the general features of product distributions from heavy ion reactions.

  14. Spectroscopy of Actinide Nuclei - Perspectives with Position Sensitive HPGe Detectors

    NASA Astrophysics Data System (ADS)

    Reiter, P.; Birkenbach, B.; Kotthaus, T.

    Recent advances in in-beam gamma-ray spectroscopy of actinide nuclei are based on highly efficient arrays of escape-suppressed spectrometers. The sensitivity of these detector arrays is greatly enhanced by the combination with powerful mass separators or particle detector systems. This technique is demonstrated by an experiment to investigate excited states in 234U after the one-neutron-transfer reaction 235U(d,t). In coincidence with the outgoing tritons, γ-rays were detected with the highly efficient MINIBALL spectrometer. In the near future an even enhanced sensitivity will be achieved by utilizing position sensitive HPGe detectors which will exploit the novel detection method of gamma-ray energy tracking in electrically segmented germanium detectors. An example for this novel approach is the investigation neutron-rich actinide Th and U nuclei after multi nucleon transfer reactions employing the AGATA demonstrator and PRISMA setup at LNL, Italy. A primary 136Xe beam hitting a 238U target was used to produce the nuclei of interest. Beam-like reaction products after neutron transfer were selected by the PRISMA spectrometer. Coincident γ-rays from excited states in beam and target like particles were measured with the position sensitive AGATA HPGe detectors. Improved Doppler correction and quality of the γ-spectra is based on the novel γ-ray tracking technique, which was successfully exploited in this region.

  15. IUPAC-NIST Solubility Data Series. 74. Actinide Carbon Compounds

    NASA Astrophysics Data System (ADS)

    Hála, Jiri; Hála, Jiri; Navratil, James D.

    2001-03-01

    This volume presents solubility data of the carbonates, salts of carboxylic acids, and other carbon containing compounds of actinides. Covered are compounds of thorium, uranium, neptunium, plutonium, americium, and one system for curium. No solubility data on carbonates or other carbon containing compounds have been found for other actinide elements. The literature has been covered up to the end of 1999, and there was a great effort to have the literature survey as complete as possible. Only those published results that report meaningful data were considered for the volume. Papers that reported qualitative results with statements like "sparingly soluble" or "insoluble," etc. were not considered. In addition to papers that published numerical data, some papers that presented data in graphical form only were considered as well. They were considered for the volume either if no other data were available for the system, if the data were published in difficult to obtain older literature, or if the data were considered to be of importance for other reasons. For many compounds it was not possible to provide the Chemical Abstracts Registry Numbers since these have not yet been assigned. For this reason, the Registry Number index is incomplete.

  16. Feasibility of actinide separation from UREX-like raffinates using a combination of sulfur- and oxygen-donor extractants

    SciTech Connect

    Zalupski, P.R.; Peterman, D.R.; Riddle, C.L.

    2013-07-01

    A synergistic combination of bis(o-trifluoromethylphenyl)dithios-phosphinic acid and trioctylphosphine oxide has been recently shown to selectively remove uranium, neptunium, plutonium and americium from aqueous environment containing up to 0.5 M nitric acid and 5.5 g/l fission products. Here the feasibility of performing this complete actinide recovery from aqueous mixtures is forecasted for a new organic formulation containing sulfur donor extractant of modified structure based on Am(III) and Eu(III) extraction data. A mixture of bis(bis-m,m-trifluoromethyl)phenyl)-dithios-phosphinic acid and TOPO in toluene enhances the extraction performance, accomplishing Am/Eu differentiation in aqueous mixtures up to 1 M nitric acid. The new organic recipe is also less susceptible to oxidative damage resulting from radiolysis. (authors)

  17. Feasibility of actinide separation from UREX-like raffinates using a combination of sulfur- and oxygen-donor extractants

    SciTech Connect

    Peter R. Zalupski; Dean R. Peterman; Catherine L. Riddle

    2013-09-01

    A synergistic combination of bis(o-trifluoromethylphenyl)dithiosphosphinic acid and trioctylphosphine oxide has been recently shown to selectively remove uranium, neptunium, plutonium and americium from aqueous environment containing up to 0.5 M nitric acid and 5.5 g/L fission products. Here the feasibility of performing this complete actinide recovery from aqueous mixtures is forecasted for a new organic formulation containing sulfur donor extractant of modified structure based on Am(III) and Eu(III) extraction data. A mixture of bis(bis-m,m-trifluoromethyl)phenyl)-dithiosphosphinic acid and TOPO in toluene enhances the extraction performance, accomplishing Am/Eu differentiation in aqueous mixtures up to 1 M nitric acid. The new organic recipe is also less susceptible to oxidative damage resulting from radiolysis.

  18. Loading Actinides in Multilayered Structures for Nuclear Waste Treatment: The First Case Study of Uranium Capture with Vanadium Carbide MXene.

    PubMed

    Wang, Lin; Yuan, Liyong; Chen, Ke; Zhang, Yujuan; Deng, Qihuang; Du, Shiyu; Huang, Qing; Zheng, Lirong; Zhang, Jing; Chai, Zhifang; Barsoum, Michel W; Wang, Xiangke; Shi, Weiqun

    2016-06-29

    Efficient nuclear waste treatment and environmental management are important hurdles that need to be overcome if nuclear energy is to become more widely used. Herein, we demonstrate the first case of using two-dimensional (2D) multilayered V2CTx nanosheets prepared by HF etching of V2AlC to remove actinides from aqueous solutions. The V2CTx material is found to be a highly efficient uranium (U(VI)) sorbent, evidenced by a high uptake capacity of 174 mg g(-1), fast sorption kinetics, and desirable selectivity. Fitting of the sorption isotherm indicated that the sorption followed a heterogeneous adsorption model, most probably due to the presence of heterogeneous adsorption sites. Density functional theory calculations, in combination with X-ray absorption fine structure characterizations, suggest that the uranyl ions prefer to coordinate with hydroxyl groups bonded to the V-sites of the nanosheets via forming bidentate inner-sphere complexes.

  19. The Dirac equation in electronic structure calculations: Accurate evaluation of DFT predictions for actinides

    SciTech Connect

    Wills, John M; Mattsson, Ann E

    2012-06-06

    Brooks, Johansson, and Skriver, using the LMTO-ASA method and considerable insight, were able to explain many of the ground state properties of the actinides. In the many years since this work was done, electronic structure calculations of increasing sophistication have been applied to actinide elements and compounds, attempting to quantify the applicability of DFT to actinides and actinide compounds and to try to incorporate other methodologies (i.e. DMFT) into DFT calculations. Through these calculations, the limits of both available density functionals and ad hoc methodologies are starting to become clear. However, it has also become clear that approximations used to incorporate relativity are not adequate to provide rigorous tests of the underlying equations of DFT, not to mention ad hoc additions. In this talk, we describe the result of full-potential LMTO calculations for the elemental actinides, comparing results obtained with a full Dirac basis with those obtained from scalar-relativistic bases, with and without variational spin-orbit. This comparison shows that the scalar relativistic treatment of actinides does not have sufficient accuracy to provide a rigorous test of theory and that variational spin-orbit introduces uncontrolled errors in the results of electronic structure calculations on actinide elements.

  20. Toward understanding the thermodynamics of TALSPEAK process. Medium effects on actinide complexation

    SciTech Connect

    Peter R Zalupski; Leigh R Martin; Ken Nash; Yoshinobu Nakamura; Masahiko Yamamoto

    2009-07-01

    The ingenious combination of lactate and diethylenetriamine-N,N,N’,N”,N”-pentaacetic acid (DTPA) as an aqueous actinide-complexing medium forms the basis of the successful separation of americium and curium from lanthanides known as the TALSPEAK process. While numerous reports in the prior literature have focused on the optimization of this solvent extraction system, considerably less attention has been devoted to the understanding of the basic thermodynamic features of the complex fluids responsible for the separation. The available thermochemical information of both lactate and DTPA protonation and metal complexation reactions are representative of the behavior of these ions under idealized conditions. Our previous studies of medium effects on lactate protonation suggest that significant departures from the speciation predicted based on reported thermodynamic values should be expected in the TALSPEAK aqueous environment. Thermodynamic parameters describing the separation chemistry of this process thus require further examination at conditions significantly removed from conventional ideal systems commonly employed in fundamental solution chemistry. Such thermodynamic characterization is the key to predictive modelling of TALSPEAK. Improved understanding will, in principle, allow process technologists to more efficiently respond to off-normal conditions during large scale process operation. In this report, the results of calorimetric and potentiometric investigations of the effects of aqueous electrolytes on the thermodynamic parameters for lactate protonation and lactate complexation of americium and neodymium will be presented. Studies on the lactate protonation equilibrium will clearly illustrate distinct thermodynamic variations between strong electrolyte aqueous systems and buffered lactate environment.

  1. Rapid Column Extraction Method for Actinides and Sr-89/90 in Water Samples

    SciTech Connect

    MAXWELL III, SHERROD L.

    2005-06-15

    The SRS Environmental Laboratory analyzes water samples for environmental monitoring, including river water and ground water samples. A new, faster actinide and strontium 89/90 separation method has been developed and implemented to improve productivity, reduce labor costs and add capacity to this laboratory. This method uses stacked TEVA Resin{reg_sign}, TRU Resin{reg_sign} and Sr-Resin{reg_sign} cartridges from Eichrom Technologies (Darien, IL, USA) that allows the rapid separation of plutonium (Pu), neptunium (Np), uranium (U), americium (Am), curium (Cm) and thorium (Th) using a single multi-stage column combined with alpha spectrometry. By using vacuum box cartridge technology with rapid flow rates, sample preparation time is minimized. The method can be used for routine analysis or as a rapid method for emergency preparedness. Thorium and curium are often analyzed separately due to the interference of the daughter of Th-229 tracer, actinium (Ac)-225, on curium isotopes when measured by alpha spectrometry. This new method also adds a separation step using DGA Resin{reg_sign}, (Diglycolamide Resin, Eichrom Technologies) to remove Ac-225 and allow the separation and analysis of thorium isotopes and curium isotopes at the same time.

  2. Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling

    DOE PAGES

    Burns, Jonathan D.; Moyer, Bruce A.

    2016-08-17

    Hexavalent Np, Pu, and Am individually, and as a group, have all been cocrystallized with UO2(NO3)2∙ 6H2O, constituting the first demonstration of an An(VI) group cocrystalliza- tion. The hexavalent dioxo cations of Np, Pu, and Am cocrystallize with UO2(NO3)2∙ 6H2O in near proportion with a simple reduction in temperature, while the lower valence states, An(III) and An(IV), are only slightly removed from solution. A separation of An(VI) species from An(III) ions by crystallization has been demonstrated, with an observed separation factor of 14. Separation of An(VI) species from key fission products, 95Zr, 95Nb, 137Cs, and 144Ce, has also been demonstratedmore » by crystallization, with separation factors ranging from 6.5 to 71 in the absence of Am(VI), while in the presence of Am(VI), the separation factors were reduced to 0.99 7.7. One interesting observation is that Am(VI) shows increased stability in the cocrystallized form, with no reduction observed after 13 days, as opposed to in solution, in which >50% is reduced after only 10 days. The ability to cocrystallize and stabilize hexavalent actinides from solution, especially Am(VI), introduces a new separations approach that can be applied to closing the nuclear fuel cycle.« less

  3. Microbial Transformation of TRU and Mixed Waste: Actinide Speciation and Waste Volume

    SciTech Connect

    Halada, Gary P

    2008-04-10

    In order to understand the susceptibility of transuranic and mixed waste to microbial degradation (as well as any mechanism which depends upon either complexation and/or redox of metal ions), it is essential to understand the association of metal ions with organic ligands present in mixed wastes. These ligands have been found in our previous EMSP study to limit electron transfer reactions and strongly affect transport and the eventual fate of radionuclides in the environment. As transuranic waste (and especially mixed waste) will be retained in burial sites and in legacy containment for (potentially) many years while awaiting treatment and removal (or remaining in place under stewardship agreements at government subsurface waste sites), it is also essential to understand the aging of mixed wastes and its implications for remediation and fate of radionuclides. Mixed waste containing actinides and organic materials are especially complex and require extensive study. The EMSP program described in this report is part of a joint program with the Environmental Sciences Department at Brookhaven National Laboratory. The Stony Brook University portion of this award has focused on the association of uranium (U(VI)) and transuranic analogs (Ce(III) and Eu(III)) with cellulosic materials and related compounds, with development of implications for microbial transformation of mixed wastes. The elucidation of the chemical nature of mixed waste is essential for the formulation of remediation and encapsulation technologies, for understanding the fate of contaminant exposed to the environment, and for development of meaningful models for contaminant storage and recovery.

  4. The role of transferrin in actinide(IV) uptake: comparison with iron(III).

    PubMed

    Jeanson, Aurélie; Ferrand, M; Funke, Harald; Hennig, Christoph; Moisy, Philippe; Solari, Pier Lorenzo; Vidaud, Claude; Den Auwer, Christophe

    2010-01-25

    The impact of actinides on living organisms has been the subject of numerous studies since the 1950s. From a general point of view, these studies show that actinides are chemical poisons as well as radiological hazards. Actinides in plasma are assumed to be mainly complexed to transferrin, the iron carrier protein. This paper casts light on the uptake of actinides(IV) (thorium, neptunium, plutonium) by transferrin, focusing on the pH dependence of the interaction and on a molecular description of the cation binding site in the protein. Their behavior is compared with that of iron(III), the endogenous transferrin cation, from a structural point of view. Complementary spectroscopic techniques (UV/Vis spectrophotometry, microfiltration coupled with gamma spectrometry, and X-ray absorption fine structure) have been combined in order to propose a structural model for the actinide-binding site in transferrin. Comparison of our results with data available on holotransferrin suggests some similarities between the behavior of Fe(III) and Np(IV)/Pu(IV)/ Np(IV) is not complexed at pH <7, whereas at pH approximately 7.4 complexation can be regarded as quantitative. This pH effect is consistent with the in vivo transferrin "cycle". Pu(IV) also appears to be quantitatively bound by apotransferrin at around pH approximately 7.5, whereas Th(IV) was never complexed under our experimental conditions. EXAFS data at the actinide edge have allowed a structural model of the actinide binding site to be elaborated: at least one tyrosine residue could participate in the actinide coordination sphere (two for iron), forming a mixed hydroxo-transferrin complex in which actinides are bound with transferrin both through An-tyrosine and through An--OH bonds. A description of interatomic distances is provided.

  5. MICROBIAL TRANSFORMATIONS OF PLUTONIUM AND OTHER ACTINIDES IN TRANSURANIC AND MIXED WASTES.

    SciTech Connect

    FRANCIS,A.J.

    2003-07-06

    The presence of the actinides Th, U, Np, Pu, and Am in transuranic (TRU) and mixed wastes is a major concern because of their potential for migration from the waste repositories and long-term contamination of the environment. The toxicity of the actinide elements and the long half-lives of their isotopes are the primary causes for concern. In addition to the radionuclides the TRU waste consists a variety of organic materials (cellulose, plastic, rubber, chelating agents) and inorganic compounds (nitrate and sulfate). Significant microbial activity is expected in the waste because of the presence of organic compounds and nitrate, which serve as carbon and nitrogen sources and in the absence of oxygen the microbes can use nitrate and sulfate as alternate electron acceptors. Biodegradation of the TRU waste can result in gas generation and pressurization of containment areas, and waste volume reduction and subsidence in the repository. Although the physical, chemical, and geochemical processes affecting dissolution, precipitation, and mobilization of actinides have been investigated, we have only limited information on the effects of microbial processes. Microbial activity could affect the chemical nature of the actinides by altering the speciation, solubility and sorption properties and thus could increase or decrease the concentrations of actinides in solution. Under appropriate conditions, dissolution or immobilization of actinides is brought about by direct enzymatic or indirect non-enzymatic actions of microorganisms. Dissolution of actinides by microorganisms is brought about by changes in the Eh and pH of the medium, by their production of organic acids, such as citric acid, siderophores and extracellular metabolites. Immobilization or precipitation of actinides is due to changes in the Eh of the environment, enzymatic reductive precipitation (reduction from higher to lower oxidation state), biosorption, bioaccumulation, biotransformation of actinides complexed

  6. Removal of dissolved actinides from alkaline solutions by the method of appearing reagents

    DOEpatents

    Krot, Nikolai N.; Charushnikova, Iraida A.

    1997-01-01

    A method of reducing the concentration of neptunium and plutonium from alkaline radwastes containing plutonium and neptunium values along with other transuranic values produced during the course of plutonium production. The OH.sup.- concentration of the alkaline radwaste is adjusted to between about 0.1M and about 4M. [UO.sub.2 (O.sub.2).sub.3 ].sup.4- ion is added to the radwastes in the presence of catalytic amounts of Cu.sup.+2, Co.sup.+2 or Fe.sup.+2 with heating to a temperature in excess of about 60.degree. C. or 85.degree. C., depending on the catalyst, to coprecipitate plutonium and neptunium from the radwaste. Thereafter, the coprecipitate is separated from the alkaline radwaste.

  7. Solid-phase extraction microfluidic devices for matrix removal in trace element assay of actinide materials.

    PubMed

    Gao, Jun; Manard, Benjamin T; Castro, Alonso; Montoya, Dennis P; Xu, Ning; Chamberlin, Rebecca M

    2017-05-15

    Advances in sample nebulization and injection technology have significantly reduced the volume of solution required for trace impurity analysis in plutonium and uranium materials. Correspondingly, we have designed and tested a novel chip-based microfluidic platform, containing a 100-µL or 20-µL solid-phase microextraction column, packed by centrifugation, which supports nuclear material mass and solution volume reductions of 90% or more compared to standard methods. Quantitative recovery of 28 trace elements in uranium was demonstrated using a UTEVA chromatographic resin column, and trace element recovery from thorium (a surrogate for plutonium) was similarly demonstrated using anion exchange resin AG MP-1. Of nine materials tested, compatibility of polyvinyl chloride (PVC), polypropylene (PP), and polytetrafluoroethylene (PTFE) chips with the strong nitric acid media was highest. The microcolumns can be incorporated into a variety of devices and systems, and can be loaded with other solid-phase resins for trace element assay in high-purity metals.

  8. Water-soluble chelating polymers for removal of actinides from watewater

    SciTech Connect

    Jarvinen, G.

    1996-10-01

    Polymer filtration is a technology being developed to recover valuable or regulated metal ions selectively from process or wastewaters. Water-soluble chelating polymers are specially designed to bind selectively with metal ions in aqueous solutions. The polymers molecular weight is large enough so they can be separated and concentrated using available ultrafiltration technology. Water and smaller unbound components of the solution pass freely through the ultrafiltration membrane. The polymers can then be reused by changing the solution conditions to release the metal ions, which are recovered in concentrated form, for recycle or disposal.

  9. Solid-phase extraction microfluidic devices for matrix removal in trace element assay of actinide materials

    DOE PAGES

    Gao, Jun; Manard, Benjamin Thomas; Castro, Alonso; ...

    2017-02-02

    Advances in sample nebulization and injection technology have significantly reduced the volume of solution required for trace impurity analysis in plutonium and uranium materials. Correspondingly, we have designed and tested a novel chip-based microfluidic platform, containing a 100-µL or 20-µL solid-phase microextraction column, packed by centrifugation, which supports nuclear material mass and solution volume reductions of 90% or more compared to standard methods. Quantitative recovery of 28 trace elements in uranium was demonstrated using a UTEVA chromatographic resin column, and trace element recovery from thorium (a surrogate for plutonium) was similarly demonstrated using anion exchange resin AG MP-1. Of ninemore » materials tested, compatibility of polyvinyl chloride (PVC), polypropylene (PP), and polytetrafluoroethylene (PTFE) chips with the strong nitric acid media was highest. Finally, the microcolumns can be incorporated into a variety of devices and systems, and can be loaded with other solid-phase resins for trace element assay in high-purity metals.« less

  10. Removal of dissolved actinides from alkaline solutions by the method of appearing reagents

    SciTech Connect

    Krot, N.N.; Charushnikova, I.A.

    1997-06-17

    A method is described for reducing the concentration of neptunium and plutonium from alkaline radwastes containing plutonium and neptunium values along with other transuranic values produced during the course of plutonium production. The OH{sup {minus}} concentration of the alkaline radwaste is adjusted to between about 0.1M and about 4M. [UO{sub 2}(O{sub 2}){sub 3}]{sup 4{minus}} ion is added to the radwastes in the presence of catalytic amounts of Cu{sup +2}, Co{sup +2} or Fe{sup +2} with heating to a temperature in excess of about 60 C or 85 C, depending on the catalyst, to coprecipitate plutonium and neptunium from the radwaste. Thereafter, the coprecipitate is separated from the alkaline radwaste. 2 figs.

  11. The separation of lanthanides and actinides in supercritical fluid carbon dioxide

    SciTech Connect

    Mincher, Bruce J.; Wai, Chien M.; Fox, Robert V.; Baek, Donna L.; Yen, Clive; Case, Mary E.

    2015-10-28

    Supercritical fluid carbon dioxide presents an attractive alternative to conventional solvents for recovery of the actinides and lanthanides. Carbon dioxide is a good solvent for fluorine and phosphate-containing ligands, including the traditional tributylphosphate ligand used in process-scale uranium separations. Actinide and lanthanide oxides may even be directly dissolved in carbon dioxide containing the complexes formed between these ligands and mineral acids, obviating the need for large volumes of acids for leaching and dissolution, and the corresponding organic liquid–liquid solvent extraction solutions. As a result, examples of the application of this novel technology for actinide and lanthanide separations are presented.

  12. Literature review of United States utilities computer codes for calculating actinide isotope content in irradiated fuel

    SciTech Connect

    Horak, W.C.; Lu, Ming-Shih

    1991-12-01

    This paper reviews the accuracy and precision of methods used by United States electric utilities to determine the actinide isotopic and element content of irradiated fuel. After an extensive literature search, three key code suites were selected for review. Two suites of computer codes, CASMO and ARMP, are used for reactor physics calculations; the ORIGEN code is used for spent fuel calculations. They are also the most widely used codes in the nuclear industry throughout the world. Although none of these codes calculate actinide isotopics as their primary variables intended for safeguards applications, accurate calculation of actinide isotopic content is necessary to fulfill their function.

  13. Chemical Speciation of Americium, Curium and Selected Tetravalent Actinides in High Level Waste

    SciTech Connect

    Felmy, Andrew R.

    2006-06-01

    Large volumes of high-level waste (HLW) currently stored in tanks at DOE sites contain both sludges and supernatants. The sludges are composed of insoluble precipitates of actinides, radioactive fission products, and nonradioactive components. The supernatants are alkaline carbonate solutions, which can contain soluble actinides, fission products, metal ions, and high concentrations of major electrolytes including sodium hydroxide, nitrate, nitrite, phosphate, carbonate, aluminate, sulfate, and organic complexants. The organic complexants include several compounds that can form strong aqueous complexes with actinide species and fission products including ethylenediaminetetraacetic acid (EDTA), N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA), nitrilotriacetic acid (NTA), iminodiacetic acid (IDA), citrate, glycolate, gluconate, and degradation products, formate and oxalate.

  14. Phytosiderophore Effects on Subsurface Actinide Contaminants: Potential for Phytostabilization and Phytoextraction

    SciTech Connect

    Ruggiero, Christy

    2003-06-01

    This project seeks to determine the potential of phytosiderophore-producing plants for phytostabilization and phytoextraction of actinides and some metal soil contaminants. Phytosiderophores are secreted by graminaceous plants such as barley and wheat for the solubilization, mobilization and uptake of Fe and other essential nutrients from soils. The ability for these phytosiderophores to chelate and absorb actinides using the same uptake system as for Fe is hereby investigated though characterization of actinide-phytosiderophore complexes (independently of plants), and characterization of plant uptake of such complexes.

  15. Thermodynamics of actinide complexation in solution at elevated temperatures: application of variable-temperature titration calorimetry.

    PubMed

    Rao, Linfeng

    2007-06-01

    Studies of actinide complexation in solution at elevated temperatures provide insight into the effect of solvation and the energetics of complexation, and help to predict the chemical behavior of actinides in nuclear waste processing and disposal where temperatures are high. This tutorial review summarizes the data on the complexation of actinides at elevated temperatures and describes the methodology for thermodynamic measurements, with the emphasis on variable-temperature titration calorimetry, a highly valuable technique to determine the enthalpy and, under appropriate conditions, the equilibrium constants of complexation as well.

  16. Fission-product data analysis from actinide samples exposed in the Dounreay Prototype Fast Reactor

    SciTech Connect

    Murphy, B.D.; Dickens, J.K.; Walker, R.L.; Newton, T.D.

    1994-12-31

    Since 1979 a cooperative agreement has been in effect between the United States and the United Kingdom to investigate the irradiation of various actinide species placed in the core of the Dounreay Prototype Fast Reactor (PFR). The irradiated species were isotopes of thorium, protactinium, uranium, neptunium, plutonium, americium, and curium. A set of actinide samples (mg quantities) was exposed to about 490 effective full power days (EFPD) of reactor operations. The fission-product results are reported here. The actinide results will be report elsewhere.

  17. Establishment of a room temperature molten salt capability to measure fundamental thermodynamic properties of actinide elements

    SciTech Connect

    Smith, W.H.; Costa, D.A.

    1998-12-31

    This is the final report of a six-month, Laboratory Directed Research and Development (LDRD) project at Los Alamos National Laboratory (LANL). The goal of this work was to establish a capability for the measurement of fundamental thermodynamic properties of actinide elements in room temperature molten salts. This capability will be used to study in detail the actinide chloro- and oxo-coordination chemistries that dominate in the chloride-based molten salt media. Uranium will be the first actinide element under investigation.

  18. Irradiaton of Metallic and Oxide Fuels for Actinide Transmutation in the ATR

    SciTech Connect

    Heather J. MacLean; Steven L. Hayes

    2007-09-01

    Metallic fuels containing minor actinides and rare earth additions have been fabricated and are prepared for irradiation in the ATR, scheduled to begin during the summer of 2007. Oxide fuels containing minor actinides are being fabricated and will be ready for irradiation in ATR, scheduled to begin during the summer of 2008. Fabrication and irradiation of these fuels will provide detailed studies of actinide transmutation in support of the Global Nuclear Energy Partnership. These fuel irradiations include new fuel compositions that have never before been tested. Results from these tests will provide fundamental data on fuel irradiation performance and will advance the state of knowledge for transmutation fuels.

  19. Conjugates of Actinide Chelator-Magnetic Nanoparticles for Used Fuel Separation Technology

    SciTech Connect

    Qiang, You; Paszczynski, Andrzej; Rao, Linfeng

    2011-10-30

    The actinide separation method using magnetic nanoparticles (MNPs) functionalized with actinide specific chelators utilizes the separation capability of ligand and the ease of magnetic separation. This separation method eliminated the need of large quantity organic solutions used in the liquid-liquid extraction process. The MNPs could also be recycled for repeated separation, thus this separation method greatly reduces the generation of secondary waste compared to traditional liquid extraction technology. The high diffusivity of MNPs and the large surface area also facilitate high efficiency of actinide sorption by the ligands. This method could help in solving the nuclear waste remediation problem.

  20. Chemical Speciation of Americium, Curium and Selected Tetravalent Actinides in High Level Waste

    SciTech Connect

    Felmy, Andrew R.

    2005-06-01

    Large volumes of high-level waste (HLW) currently stored in tanks at DOE sites contain both sludges and supernatants. The sludges are composed of insoluble precipitates of actinides, radioactive fission products, and nonradioactive components. The supernatants are alkaline carbonate solutions, which can contain soluble actinides, fission products, metal ions, and high concentrations of major electrolytes including sodium hydroxide, nitrate, nitrite, phosphate, carbonate, aluminate, sulfate, and organic complexants. The organic complexants include several compounds that can form strong aqueous complexes with actinide species and fission products including ethylenediaminetetraacetic acid (EDTA), N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA), nitrilotriacetic acid (NTA), iminodiacetic acid (IDA), citrate, glycolate, gluconate, and degradation products, formate and oxalate.

  1. FY2011 Annual Report for the Actinide Isomer Detection Project

    SciTech Connect

    Warren, Glen A.; Francy, Christopher J.; Ressler, Jennifer J.; Erikson, Luke E.; Tatishvili, Gocha; Hatarik, R.

    2011-10-01

    This project seeks to identify a new signature for actinide element detection in active interrogation. This technique works by exciting and identifying long-lived nuclear excited states (isomers) in the actinide isotopes and/or primary fission products. Observation of isomers in the fission products will provide a signature for fissile material. For the actinide isomers, the decay time and energy of the isomeric state is unique to a particular isotope, providing an unambiguous signature for SNM. This project entails isomer identification and characterization and neutron population studies. This document summarizes activities from its third year - completion of the isomer identification characterization experiments and initialization of the neutron population experiments. The population and decay of the isomeric state in 235U remain elusive, although a number of candidate gamma rays have been identified. In the course of the experiments, a number of fission fragment isomers were populated and measured [Ressler 2010]. The decays from these isomers may also provide a suitable signature for the presence of fissile material. Several measurements were conducted throughout this project. This report focuses on the results of an experiment conducted collaboratively by PNNL, LLNL and LBNL in December 2010 at LBNL. The measurement involved measuring the gamma-rays emitted from an HEU target when bombarded with 11 MeV neutrons. This report discussed the analysis and resulting conclusions from those measurements. There was one strong candidate, at 1204 keV, of an isomeric signature of 235U. The half-life of the state is estimated to be 9.3 {mu}s. The measured time dependence fits the decay time structure very well. Other possible explanations for the 1204-keV state were investigated, but they could not explain the gamma ray. Unfortunately, the relatively limited statistics of the measurement limit, and the lack of understanding of some of the systematic of the experiment, limit

  2. Start-up of a spiral periphyton bioreactor (SPR) for removal of COD and the characteristics of the associated microbial community.

    PubMed

    Shangguan, Haidong; Liu, Junzhuo; Zhu, Yan; Tong, Zhengong; Wu, Yonghong

    2015-10-01

    Periphyton-based bioreactors are widely accepted for removing various pollutants from wastewater; however, the slow start-up and low efficiency in widely fluctuating temperatures limit its application. A spiral periphyton bioreactor (SPR) was developed and its COD removal capability and the associated microbial communities were investigated. This SPR can be easily backwashed to stimulate periphyton growth and efficiently remove COD at temperatures ranging from 4 to 30 °C. The species richness and evenness of the periphyton community increased during domestication, while its functional diversity and organic carbon metabolic vitality were higher after 30 days domestication. Cyanobacteria were the main components of the SPR and produced an aerobic environment, while Alphaproteobacteria, Betaproteobacteria, Gammaproteobacteria and Sphingobacteria were the microorganisms responsible for COD removal. This study provides valuable insights into changes in pivotal microorganisms of the periphyton community during domestication, and indicates that SPR is simple to operate and efficient in COD removal.

  3. Actinide Sequestration Using Self-Assembled Monolayers on Mesoporous Supports

    SciTech Connect

    Fryxell, Glen E.; Lin, Yuehe; Fiskum, Sandra K.; Birnbaum, Jerome C.; Wu, Hong; Kemner, K. M.; Kelly, Shelley

    2005-03-01

    Surfactant templated synthesis of mesoporous ceramics provides a versatile foundation upon which to create high efficiency environmental sorbents. These nanoporous ceramic oxides condense a huge amount of surface area into a very small volume. The ceramic oxide interface is receptive to surface functionalization through molecular self-assembly. The marriage of mesoporous ceramics with self-assembled monolayer chemistry creates a powerful new class of environmental sorbent materials called self-assembled monolayers on mesoporous supports (SAMMS). These SAMMS materials are highly efficient sorbents, whose interfacial chemistry can be fine-tuned to selectively sequester a specific target species, such as heavy metals, tetrahedral oxometallate anions and radionuclides. Details addressing the design, synthesis and characterization of SAMMS materials specifically designed to sequester actinides, of central importance to the environmental clean-up necessary after 40 years of weapons grade plutonium production, as well as evaluation of their binding affinities and kinetics are presented.

  4. First ionization potential of the heaviest actinide lawrencium, element 103

    NASA Astrophysics Data System (ADS)

    Sato, Tetsuya K.; Asai, Masato; Borschevsky, Anastasia; Stora, Thierry; Sato, Nozomi; Kaneya, Yusuke; Tsukada, Kazuaki; Düllmann, Christoph E.; Eberhardt, Klaus; Eliav, Ephraim; Ichikawa, Shinichi; Kaldor, Uzi; Kratz, Jens V.; Miyashita, Sunao; Nagame, Yuichiro; Ooe, Kazuhiro; Osa, Akihiko; Renisch, Dennis; Runke, Jörg; Schädel, Matthias; Thörle-Pospiech, Petra; Toyoshima, Atsushi; Trautmann, Norbert

    2016-12-01

    The first ionization potential (IP1) of element 103, lawrencium (Lr), has been successfully determined for the first time by using a newly developed method based on a surface ionization process. The measured IP1 value is 4.963 eV. This value is the smallest among those of actinide elements and is in excellent agreement with the value of 4.963(15) eV predicted by state-of-the-art relativistic calculations also performed in this work. Our results strongly support that the Lr atom has an electronic configuration of [Rn]7s25f147p, which is influenced by strong relativistic effects. The present work provides a reliable benchmark for theoretical calculations and also opens the way for studies on atomic properties of heavy elements with atomic number Z > 100. Moreover, the present achievement has triggered a controversy on the position of lutetium (Lu) and Lr in the Periodic Table of Elements.

  5. Kinetics of dissociation of trivalent actinide chelates of TMDTA

    SciTech Connect

    Muscatello, A.C.; Choppin, G.R.; D'Olieslager, W. )

    1989-03-22

    Measurements by a radiotracer technique show that the dissociation of TMDTA (trimethylenediamine-N,N-tetraacetic acid) chelates with Am, Cm, Bk, Cf, and Eu proceeds through an acid-catalyzed pathway. The rates of dissociation of An(TMDTA){sup {minus}} are 2 orders of magnitude faster than those of the corresponding EDTA chelates, presumably due to the greater lability of the nitrogen atom in the six-membered nitrogen-metal-nitrogen ring of TMDTA chelates. The rate of dissociation also decreased with decreasing metal ion radius. A proton-catalyzed mechanism similar to that for dissociation of EDTA complexes of lanthanide and actinide cations is consistent with the rate data. 19 refs., 6 figs., 2 tabs.

  6. Magnetic structures of actinide materials by pulsed neutron diffraction

    SciTech Connect

    Lawson, A.C.; Goldstone, J.A.; Huber, J.G.; Giorgi, A.L.; Conant, J.W.; Severing, A.; Cort, B.; Robinson, R.A.

    1990-01-01

    We describe some attempts to observe magnetic structure in various actinide (5f-electron) materials. Our experimental technique is neutron powder diffraction as practiced at a spallation (pulsed) neutron source. We will discuss our investigations of {alpha}-Pu, {delta}-Pu, {alpha}-UD{sub 3} and {beta}-UD{sub 3}. {beta}-UD{sub 3} is a simple ferromagnet: surprisingly, the moments on the two non-equivalent uranium atoms are the same within experimental error. {alpha}-UD{sub 3}, {alpha}-Pu and {delta}-Pu are non-magnetic, within the limits of our observations. Our work with pulsed neutron diffraction shows that it is a useful technique for research on magnetic materials.

  7. Fission cross section measurements of actinides at LANSCE

    SciTech Connect

    Tovesson, Fredrik; Laptev, Alexander B; Hill, Tony S

    2010-01-01

    Fission cross sections of a range of actinides have been measured at the Los Alamos Neutron Science Center (LANSCE) in support of nuclear energy applications. By combining measurement at two LANSCE facilities, Lujan Center and the Weapons Neutron Research center (WNR), differential cross sections can be measured from sub-thermal energies up to 200 MeV. Incident neutron energies are determined using the time-of-flight method, and parallel-plate ionization chambers are used to measure fission cross sections relative to the {sup 235}U standard. Recent measurements include the {sup 233,238}U, {sup 239,242}Pu and {sup 243}Am neutron-induced fission cross sections. In this paper preliminary results for cross section data of {sup 243}Am and {sup 233}U will be presented.

  8. Specific sequestering agents for iron and the actinides

    SciTech Connect

    Raymond, K.N.

    1983-06-01

    The transuranium actinide ions represent one unique environmental hazard associated with the waste of the nuclear power industry. A major component associated with that waste and a potential hazard is plutonium. The synthesis of metal-ion-specific complexing agents for ions such as Pu(IV) potentially represents a powerful new approach to many of the problems posed by waste treatment. This document is a progress report of a rational approach to the synthesis of such chelating agents based on the similarities of Pu(IV) and Fe(III), the structures of naturally-occurring complexing agents which are highly specific for Fe(III), and the incorporation of the same kinds of ligating groups present in the iron complexes to make octadentate complexes highly specific for plutonium. Both thermodynamic and animal test results indicate that a relatively high degree of success has already been achieved in this aim.

  9. Theory in Evaluation of Actinide Fission and Capture Cross Sections

    SciTech Connect

    Lynn, J. Eric

    2005-05-24

    We discuss the possibilities and limitations of the use of theory as a tool in the evaluation of actinide fission and capture cross sections. We consider especially the target 235U as an example. We emphasize the roles of intermediate structure in the fission cross section and of level width fluctuations in both intermediate structure and fine structure, noting that these lead to a breakdown of Hauser-Feshbach theory at sub-barrier and near-barrier energies. At higher energies (where fluctuation-averaged Hauser-Feshbach theory is applicable) semi-quantitative and intuitive representations of transition state spectra and barrier level density functions have to be tested against experimental data wherever these are available. Adjustment of the fission cross section against inelastic scattering to the much better known levels of the residual nucleus should then lead to a fairly sound estimate of the capture cross section. We compare such estimates with evaluated and experimental data for 235U.

  10. Solid-state actinide acid phosphites from phosphorous acid melts

    SciTech Connect

    Oh, George N.; Burns, Peter C.

    2014-07-01

    The reaction of UO{sub 3} and H{sub 3}PO{sub 3} at 100 °C and subsequent reaction with dimethylformamide (DMF) produces crystals of the compound (NH{sub 2}(CH{sub 3}){sub 2})[UO{sub 2}(HPO{sub 2}OH)(HPO{sub 3})]. This compound crystallizes in space group P2{sub 1}/n and consists of layers of uranyl pentagonal bipyramids that share equatorial vertices with phosphite units, separated by dimethylammonium. In contrast, the reaction of phosphorous acid and actinide oxides at 210 °C produces a viscous syrup. Subsequent dilution in solvents and use of standard solution-state methods results in the crystallization of two polymorphs of the actinide acid phosphites An(HPO{sub 2}OH){sub 4} (An=U, Th) and of the mixed acid phosphite–phosphite U(HPO{sub 3})(HPO{sub 2}OH){sub 2}(H{sub 2}O)·2(H{sub 2}O). α- and β-An(HPO{sub 2}OH){sub 4} crystallize in space groups C2/c and P2{sub 1}/n, respectively, and comprise a three-dimensional network of An{sup 4+} cations in square antiprismatic coordination corner-sharing with protonated phosphite units, whereas U(HPO{sub 3})(HPO{sub 2}OH){sub 2}(H{sub 2}O){sub 2}·(H{sub 2}O) crystallizes in a layered structure in space group Pbca that is composed of An{sup 4+} cations in square antiprismatic coordination corner-sharing with protonated phosphites and water ligands. We discuss our findings in using solid inorganic reagents to produce a solution-workable precursor from which solid-state compounds can be crystallized. - Graphical abstract: Reaction of UO{sub 3} and H{sub 3}PO{sub 3} at 100 °C and subsequent reaction with DMF produces crystals of (NH{sub 2}(CH{sub 3}){sub 2})[UO{sub 2}(HPO{sub 2}OH)(HPO{sub 3})] with a layered structure. Reaction of phosphorous acid and actinide oxides at 210 °C produces a viscous syrup and further solution-state reactions result in the crystallization of the actinide acid phosphites An(HPO{sub 2}OH){sub 4} (An=U, Th), with a three-dimensional network structure, and the mixed acid phosphite

  11. Flammability Analysis For Actinide Oxides Packaged In 9975 Shipping Containers

    SciTech Connect

    Laurinat, James E.; Askew, Neal M.; Hensel, Steve J.

    2013-03-21

    Packaging options are evaluated for compliance with safety requirements for shipment of mixed actinide oxides packaged in a 9975 Primary Containment Vessel (PCV). Radiolytic gas generation rates, PCV internal gas pressures, and shipping windows (times to reach unacceptable gas compositions or pressures after closure of the PCV) are calculated for shipment of a 9975 PCV containing a plastic bottle filled with plutonium and uranium oxides with a selected isotopic composition. G-values for radiolytic hydrogen generation from adsorbed moisture are estimated from the results of gas generation tests for plutonium oxide and uranium oxide doped with curium-244. The radiolytic generation of hydrogen from the plastic bottle is calculated using a geometric model for alpha particle deposition in the bottle wall. The temperature of the PCV during shipment is estimated from the results of finite element heat transfer analyses.

  12. Actinide sequestration using self-assembled monolayers on mesoporous supports.

    PubMed

    Fryxell, Glen E; Lin, Yuehe; Fiskum, Sandy; Birnbaum, Jerome C; Wu, Hong; Kemner, Ken; Kelly, Shelley

    2005-03-01

    Surfactant templated synthesis of mesoporous ceramics provides a versatile foundation upon which to create high efficiency environmental sorbents. These nanoporous ceramic oxides condense a huge amount of surface area into a very small volume. The ceramic oxide interface is receptive to surface functionalization through molecular self-assembly. The marriage of mesoporous ceramics with self-assembled monolayer chemistry creates a powerful new class of environmental sorbent materials called self-assembled monolayers on mesoporous supports (SAMMS). These SAMMS materials are highly efficient sorbents whose interfacial chemistry can be fine-tuned to selectively sequester a specific target species, such as heavy metals, tetrahedral oxometalate anions, and radionuclides. Details addressing the design, synthesis, and characterization of SAMMS materials specifically designed to sequester actinides, of central importance to the environmental cleanup necessary after 40 years of weapons-grade plutonium production, as well as evaluation of their binding affinities and kinetics are presented.

  13. Laboratory studies of actinide partitioning relevant to 244Pu chronometry

    NASA Technical Reports Server (NTRS)

    Benjamin, T.; Heuser, W. R.; Burnett, D. S.

    1978-01-01

    Actinide partitioning and light lanthanide fractionation have been studied to gain an understanding of Pu chemistry under meteoritic and lunar conditions. The goal of the study was to identify conditions and samples from which chronological information can be retrieved. The laboratory investigations involved particle track radiography of the crystal/liquid partitioning of Th, U and Pu among diopsidic clinopyroxene, whitlockite and liquid. It is found that trivalent Pu plays an important role in partitioning for lunar and most meteoritic conditions. The use of Pu/Nd for relative age assessments is supported to some extent by the investigations; samples with unfractionated U, Th and Nd abundances (relative to average solar system values) may be suitable for Pu chronometry.

  14. Fission of actinide nuclei using multi-nucleon transfer reactions

    NASA Astrophysics Data System (ADS)

    Léguillon, Romain; Nishio, Katsuhisa; Hirose, Kentaro; Orlandi, Riccardo; Makii, Hiroyuki; Nishinaka, Ichiro; Ishii, Tetsuro; Tsukada, Kazuaki; Asai, Masato; Chiba, Satoshi; Ohtsuki, Tsutomu; Araki, Shohei; Watanabe, Yukinobu; Tatsuzawa, Ryotaro; Takaki, Naoyuki

    2014-09-01

    We are promoting a campaign to measure fission-fragment mass distributions for neutron-rich actinide nuclei populated by transfer reactions from their ground state up to an excitation energy of several tens MeV. We thus obtain the excitation energy dependence of the mass distribution. The experiment was carried out at the 20 MV JAEA tandem facility at Tokai. We report on the data obtained in the direct reaction 18 O + 232 Th . Transfer-channels and excitation energies of the fissioning nuclei were identified using silicon dE-E detectors located at forward angle. Two fission fragments were detected in coincidence using multi-wire proportional counters. Fission fragment masses were determined by kinematic consideration. We obtained the fission fragment mass distributions for 13 nuclei from actinium to uranium and some fission barrier heights. We are promoting a campaign to measure fission-fragment mass distributions for neutron-rich actinide nuclei populated by transfer reactions from their ground state up to an excitation energy of several tens MeV. We thus obtain the excitation energy dependence of the mass distribution. The experiment was carried out at the 20 MV JAEA tandem facility at Tokai. We report on the data obtained in the direct reaction 18 O + 232 Th . Transfer-channels and excitation energies of the fissioning nuclei were identified using silicon dE-E detectors located at forward angle. Two fission fragments were detected in coincidence using multi-wire proportional counters. Fission fragment masses were determined by kinematic consideration. We obtained the fission fragment mass distributions for 13 nuclei from actinium to uranium and some fission barrier heights. Present study is supported by the Ministry of Education, Culture, Sports, Science and Technology of Japan.

  15. Density functional theory calculations of the redox potentials of actinide(VI)/actinide(V) couple in water.

    PubMed

    Steele, Helen M; Guillaumont, Dominique; Moisy, Philippe

    2013-05-30

    The measured redox potential of an actinide at an electrode surface involves the transfer of a single electron from the electrode surface on to the actinide center. Before electron transfer takes place, the complexing ligands and molecules of solvation need to become structurally arranged such that the electron transfer is at its most favorable. Following the electron transfer, there is further rearrangement to obtain the minimum energy structure for the reduced state. As such, there are three parts to the total energy cycle required to take the complex from its ground state oxidized form to its ground state reduced form. The first part of the energy comes from the structural rearrangement and solvation energies of the actinide species before the electron transfer or charge transfer process; the second part, the energy of the electron transfer; the third part, the energy required to reorganize the ligands and molecules of solvation around the reduced species. The time resolution of electrochemical techniques such as cyclic voltammetry is inadequate to determine to what extent bond and solvation rearrangement occurs before or after electron transfer; only for a couple to be classed as reversible is it fast in terms of the experimental time. Consequently, the partitioning of the energy theoretically is of importance to obtain good experimental agreement. Here we investigate the magnitude of the instantaneous charge transfer through calculating the fast one electron reduction energies of AnO2(H2O)n(2+), where An = U, Np, and Pu, for n = 4-6, in solution without inclusion of the structural optimization energy of the reduced form. These calculations have been performed using a number of DFT functionals, including the recently developed functionals of Zhao and Truhlar. The results obtained for calculated electron affinities in the aqueous phase for the AnO2(H2O)5(2+/+) couples are within 0.04 V of accepted experimental redox potentials, nearly an order of magnitude

  16. Theoretical Studies of the Electronic Structure of the Compounds of the Actinide Elements

    SciTech Connect

    Kaltsoyannis, Nikolas; Hay, P. Jeffrey; Li, Jun; Blaudeau, Jean-Philippe; Bursten, Bruce E.

    2006-02-02

    In this chapter, we will present an overview of the theoretical and computational developments that have increased our understanding of the electronic structure of actinide-containing molecules and ions. The application of modern electronic structure methodologies to actinide systems remains one of the great challenges in quantum chemistry; indeed, as will be discussed below, there is no other portion of the periodic table that leads to the confluence of complexity with respect to the calculation of ground- and excited-state energies, bonding descriptions, and molecular properties. But there is also no place in the periodic table in which effective computational modeling of electronic structure can be more useful. The difficulties in creating, isolating, and handling many of the actinide elements provide an opportunity for computational chemistry to be an unusually important partner in developing the chemistry of these elements. The importance of actinide electronic structure begins with the earliest studies of uranium chemistry and predates the discovery of quantum mechanics. The fluorescence of uranyl compounds was observed as early as 1833 (Jørgensen and Reisfeld, 1983), a presage of the development of actinometry as a tool for measuring photochemical quantum yields. Interest in nuclear fuels has stimulated tremendous interest in understanding the properties, including electronic properties, of small actinide-containing molecules and ions, especially the oxides and halides of uranium and plutonium. The synthesis of uranocene in 1968 (Streitwieser and Mu¨ ller-Westerhoff, 1968) led to the flurry of activity in the organometallic chemistry of the actinides that continues today. Actinide organometallics (or organoactinides) are nearly always molecular systems and are often volatile, which makes them amenable to an arsenal of experimental probes of molecular and electronic structure (Marks and Fischer, 1979). Theoretical and computational studies of the electronic

  17. Partitioning of minor actinides from PUREX raffinate by the TODGA process

    SciTech Connect

    Magnusson, D.; Christiansen, B.; Glatz, J.P.; Malmbeck, R.; Serrano Purroy, D.; Modolo, G.; Sorel, C.

    2007-07-01

    A genuine High Active Raffinate (HAR) was produced from small scale PUREX reprocessing of a UO{sub 2} spent fuel solution as feed for a subsequent TODGA/TBP process. In this process, efficient recovery of the trivalent Minor Actinides (MA) actinides could be demonstrated using a hot cell set-up of 32 centrifugal contactor stages. The feed decontamination factors obtained for Am and Cm were in the range of 4 x 10{sup 4} which corresponds to a recovery of more than 99.99 % in the product fraction. Trivalent lanthanides and Y were co-extracted, otherwise only a small part of the Ru ended up in the product. The collected actinide/lanthanide fraction can be used as feed for a SANEX (separation actinides from lanthanides) with some modification of the acidity depending on the extracting molecule. (authors)

  18. Separation of actinides using capillary extraction chromatography-inductively coupled plasma mass spectrometry

    SciTech Connect

    Peterson, Dominic S

    2008-01-01

    Trace levels of actinides have been separated on extraction chromatography columns. Detection of the actinides was achieved using an inductively coupled plasma mass spectrometer (ICP-MS), which was coupled with the extraction chromatography system. In this study we compare 30 cm long, 4.6 mm ID columns to capillary columns (750 {micro}m ID) with lengths from 30 cm up to 150 cm. The columns that were tested were packed with TRU resin. We were able to separate a mixture of five actinides ({sup 232}Th, {sup 238}U, {sup 237}Np, {sup 239}pU, {sup 241}Am). This work has application to rapid bioassay as well as for automated separations of actinide materials.

  19. Organophosphorus reagents in actinide separations: Unique tools for production, cleanup and disposal

    SciTech Connect

    Nash, K. L.

    2000-01-12

    Interactions of actinide ions with phosphate and organophosphorus reagents have figured prominently in nuclear science and technology, particularly in the hydrometallurgical processing of irradiated nuclear fuel. Actinide interactions with phosphorus-containing species impact all aspects from the stability of naturally occurring actinides in phosphate mineral phases through the application of the bismuth phosphate and PUREX processes for large-scale production of transuranic elements to the development of analytical separation and environment restoration processes based on new organophosphorus reagents. In this report, an overview of the unique role of organophosphorus compounds in actinide production, disposal, and environment restoration is presented. The broad utility of these reagents and their unique chemical properties is emphasized.

  20. From carbon to actinides: A new universal 1MV accelerator mass spectrometer at ANSTO

    NASA Astrophysics Data System (ADS)

    Wilcken, K. M.; Hotchkis, M.; Levchenko, V.; Fink, D.; Hauser, T.; Kitchen, R.

    2015-10-01

    A new 1 MV NEC pelletron AMS system at ANSTO is presented. The spectrometer comprises large radius magnets for actinide measurements. A novel feature of the system is fast switching between isotopes both at low and high energy sections allowing measurements of up to 8 isotopes within a single sequence. Technical details and layout of the spectrometer is presented. Performance data for 14C, 10Be, 26Al and actinides demonstrate the system is ready for routine AMS measurements.