NASA Astrophysics Data System (ADS)
Singh, Narayani P.; Zimmerman, Carol J.; Lewis, Laura L.; Wrenn, McDonald E.
1984-06-01
Solvent extraction and alpha-spectrometry have been emplyed in the quantitative simultaneous determination of uranium. thorium and plutonium. The bone specimens, spiked with 232U, 229Th and 242Pu tracers, are wet ashed with HNO 3 followed by alternate additions of a new drops of HNO 3 and H 2O 2. Uranium is reduced to the tetravalent state with 200 mg SnCl 2 and 25 ml HI. Uranium, thorium and plutonium are then coprecipitated with calcium as oxalate, heated to 550°C, dissolved in 50 ml HCl, and the acidity adjusted to 10 M. Uranium and plutonium are extracted into a 20% tri-lauryl amine (TLA) solution in xylene, leaving thorium in the aqueous phase. Plutonium is first back-extracted from the TLA phase by shaking with a 1:1.5 volume of 0.05 M NH 4I in 8 M HCl, which reduces Pu(IV) to Pu(III). Uranium is then back-extracted with an equal volume of 0.1 M HCl. Thorium, which was left in the aqueous phase, is evaporated to dryness, dissolved in 4 M HNO 3, and the acidity adjusted to 4 M. Thorium is then extracted into 20% TLA solution in xylene pre-equilibrated with 4 M HNO 3, and back-extracted with 10 M HCl. Uranium, thorium, and plutonium are then electrodeposited separately onto platinum discs and counted by an alpha-spectrometer with a multi-channel analyzer and surface barrier silicon diodes. The mean recoveries of uranium, thorium, and plutonium in bovine, dog, and human bones were over 70%.
PROCESS FOR SEGREGATING URANIUM FROM PLUTONIUM AND FISSION-PRODUCT CONTAMINATION
Ellison, C.V.; Runion, T.C.
1961-06-27
An aqueous nitric acid solution containing uranium, plutonium, and fission product values is contacted with an organic extractant comprised of a trialkyl phosphate and an organic diluent. The relative amounts of trialkyl phosphate and uranium values are controlled to achieve a concentration of uranium values in the organic extractant of at least 0.35 moles uranium per mole of trialkyl phosphate, thereby preferentially extracting uranium values into the organic extractant.
THE CHEMICAL ANALYSIS OF TERNARY ALLOYS OF PLUTONIUM WITH MOLYBDENUM AND URANIUM
DOE Office of Scientific and Technical Information (OSTI.GOV)
Phillips, G.; Woodhead, J.; Jenkins, E.N.
1958-09-01
It is shown that the absorptiometric determination of molybdenum as thiocyanate may be used in the presence of plutonium. Molybdenum interferes with previously published methods for determining uranium and plutonium but conditlons have been established for its complete removal by solvent extraction of the compound with alpha -benzoin oxime. The previous methods for uranium and plutonium are satisfactory when applied to the residual aqueous phase following this solvent extraction. (auth)
URANIUM DECONTAMINATION WITH RESPECT TO ZIRCONIUM
Vogler, S.; Beederman, M.
1961-05-01
A process is given for separating uranium values from a nitric acid aqueous solution containing uranyl values, zirconium values and tetravalent plutonium values. The process comprises contacting said solution with a substantially water-immiscible liquid organic solvent containing alkyl phosphate, separating an organic extract phase containing the uranium, zirconium, and tetravalent plutonium values from an aqueous raffinate, contacting said organic extract phase with an aqueous solution 2M to 7M in nitric acid and also containing an oxalate ion-containing substance, and separating a uranium- containing organic raffinate from aqueous zirconium- and plutonium-containing extract phase.
Evaluating ligands for use in polymer ligand film (PLF) for plutonium and uranium extraction
Rim, Jung H.; Peterson, Dominic S.; Armenta, Claudine E.; ...
2015-05-08
We describe a new analyte extraction technique using Polymer Ligand Film (PLF). PLFs were synthesized to perform direct sorption of analytes onto its surface for direct counting using alpha spectroscopy. The main focus of the new technique is to shorten and simplify the procedure for chemically isolating radionuclides for determination through a radiometric technique. 4'(5')-di-t-butylcyclohexano 18-crown-6 (DtBuCH 18C 6) and 2-ethylhexylphosphonic acid (HEH[EHP]) were examined for plutonium extraction. Di(2-ethyl hexyl) phosphoric acid (HDEHP) were examined for plutonium and uranium extraction. DtBuCH 18C 6 and HEH[EHP] were not effective in plutonium extraction. HDEHP PLFs were effective for plutonium but not formore » uranium.« less
SEPARATION OF URANIUM, PLUTONIUM, AND FISSION PRODUCTS
Spence, R.; Lister, M.W.
1958-12-16
Uranium and plutonium can be separated from neutron-lrradiated uranium by a process consisting of dissolvlng the lrradiated material in nitric acid, saturating the solution with a nitrate salt such as ammonium nitrate, rendering the solution substantially neutral with a base such as ammonia, adding a reducing agent such as hydroxylamine to change plutonium to the trivalent state, treating the solution with a substantially water immiscible organic solvent such as dibutoxy diethylether to selectively extract the uranium, maklng the residual aqueous solutlon acid with nitric acid, adding an oxidizing agent such as ammonlum bromate to oxidize the plutonium to the hexavalent state, and selectlvely extracting the plutonium by means of an immlscible solvent, such as dibutoxy dlethyletber.
PROCESSING OF NEUTRON-IRRADIATED URANIUM
Hopkins, H.H. Jr.
1960-09-01
An improved "Purex" process for separating uranium, plutonium, and fission products from nitric acid solutions of neutron-irradiated uranium is offered. Uranium is first extracted into tributyl phosphate (TBP) away from plutonium and fission products after adjustment of the acidity from 0.3 to 0.5 M and heating from 60 to 70 deg C. Coextracted plutonium, ruthenium, and fission products are fractionally removed from the TBP by three scrubbing steps with a 0.5 M nitric acid solution of ferrous sulfamate (FSA), from 3.5 to 5 M nitric acid, and water, respectively, and the purified uranium is finally recovered from the TBP by precipitation with an aqueous solution of oxalic acid. The plutonium in the 0.3 to 0.5 M acid solution is oxidized to the tetravalent state with sodium nitrite and extracted into TBP containing a small amount of dibutyl phosphate (DBP). Plutonium is then back-extracted from the TBP-DBP mixture with a nitric acid solution of FSA, reoxidized with sodium nitrite in the aqueous strip solution obtained, and once more extracted with TBP alone. Finally the plutonium is stripped from the TBP with dilute acid, and a portion of the strip solution thus obtained is recycled into the TBPDBP for further purification.
Rim, Jung H.; Armenta, Claudine E.; Gonzales, Edward R.; ...
2015-09-12
This paper describes a new analyte extraction medium called polymer ligand film (PLF) that was developed to rapidly extract radionuclides. PLF is a polymer medium with ligands incorporated in its matrix that selectively and quickly extracts analytes. The main focus of the new technique is to shorten and simplify the procedure for chemically isolating radionuclides for determination through alpha spectroscopy. The PLF system was effective for plutonium and uranium extraction. The PLF was capable of co-extracting or selectively extracting plutonium over uranium depending on the PLF composition. As a result, the PLF and electrodeposited samples had similar alpha spectra resolutions.
METHOD FOR SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS BY SOLVENT EXTRACTION
Seaborg, G.T.; Blaedel, W.J.; Walling, M.T. Jr.
1960-08-23
A process is given for separating from each other uranium, plutonium, and fission products in an aqueous nitric acid solution by the so-called Redox process. The plutonium is first oxidized to the hexavalent state, e.g., with a water-soluble dichromate or sodium bismuthate, preferably together with a holding oxidant such as potassium bromate. potassium permanganate, or an excess of the oxidizing agent. The solution is then contacted with a water-immiscible organic solvent, preferably hexone. whereby uranium and plutonium are extracted while the fission products remain in the aqueous solution. The separated organic phase is then contacted with an aqueous solution of a reducing agent, with or without a holding reductant (e.g., with a ferrous salt plus hydrazine or with ferrous sulfamate), whereby plutonium is reduced to the trivalent state and back- extracted into the aqueous solution. The uranium may finally be back-extracted from the organic solvent (e.g., with a 0.1 N nitric acid).
Bruce, F.R.
1962-07-24
A solvent extraction process was developed for separating actinide elements including plutonium and uranium from fission products. By this method the ion content of the acidic aqueous solution is adjusted so that it contains more equivalents of total metal ions than equivalents of nitrate ions. Under these conditions the extractability of fission products is greatly decreased. (AEC)
SEPARATION OF URANIUM, PLUTONIUM AND FISSION PRODUCTS
Nicholls, C.M.; Wells, I.; Spence, R.
1959-10-13
The separation of uranium and plutonium from neutronirradiated uranium is described. The neutron-irradiated uranium is dissolved in nitric acid to provide an aqueous solution 3N in nitric acid. The fission products of the solution are extruded by treating the solution with dibutyl carbitol substantially 1.8N in nitric acid. The organic solvent phase is separated and neutralized with ammonium hydroxide and the plutonium reduced with hydroxylamine base to the trivalent state. Treatment of the mixture with saturated ammonium nitrate extracts the reduced plutonium and leaves the uranium in the organic solvent.
SEPARATION OF PLUTONIUM FROM URANIUM
Feder, H.M.; Nuttall, R.L.
1959-12-15
A process is described for extracting plutonium from powdered neutron- irradiated urarium metal by contacting the latter, while maintaining it in the solid form, with molten magnesium which takes up the plutonium and separating the molten magnesium from the solid uranium.
Nelson, P.A.
1961-07-18
The liquid--liquid extraction of plutonium by magnesium from uranium or uranium--chromium alloy is described. Calcium is added to magnesium in about eutectic proportions, which results in a purer plutonium.
PLUTONIUM RECOVERY FROM NEUTRON-BOMBARDED URANIUM FUEL
Moore, R.H.
1962-04-10
A process of recovering plutonium from neutronbombarded uranium fuel by dissolving the fuel in equimolar aluminum chloride-potassium chloride; heating the mass to above 700 deg C for decomposition of plutonium tetrachloride to the trichloride; extracting the plutonium trichloride into a molten salt containing from 40 to 60 mole % of lithium chloride, from 15 to 40 mole % of sodium chloride, and from 0 to 40 mole % of potassium chloride or calcium chloride; and separating the layer of equimolar chlorides containing the uranium from the layer formed of the plutonium-containing salt is described. (AEC)
Seaborg, G.T.
1957-10-29
Methods for separating plutonium from the fission products present in masses of neutron irradiated uranium are reported. The neutron irradiated uranium is first dissolved in an aqueous solution of nitric acid. The plutonium in this solution is present as plutonous nitrate. The aqueous solution is then agitated with an organic solvent, which is not miscible with water, such as diethyl ether. The ether extracts 90% of the uraryl nitrate leaving, substantially all of the plutonium in the aqueous phase. The aqueous solution of plutonous nitrate is then oxidized to the hexavalent state, and agitated with diethyl ether again. In the ether phase there is then obtained 90% of plutonium as a solution of plutonyl nitrate. The ether solution of plutonyl nitrate is then agitated with water containing a reducing agent such as sulfur dioxide, and the plutonium dissolves in the water and is reduced to the plutonous state. The uranyl nitrate remains in the ether. The plutonous nitrate in the water may be recovered by precipitation.
Selective Extraction of Uranium from Liquid or Supercritical Carbon Dioxide
DOE Office of Scientific and Technical Information (OSTI.GOV)
Farawila, Anne F.; O'Hara, Matthew J.; Wai, Chien M.
2012-07-31
Current liquid-liquid extraction processes used in recycling irradiated nuclear fuel rely on (1) strong nitric acid to dissolve uranium oxide fuel, and (2) the use of aliphatic hydrocarbons as a diluent in formulating the solvent used to extract uranium. The nitric acid dissolution process is not selective. It dissolves virtually the entire fuel meat which complicates the uranium extraction process. In addition, a solvent washing process is used to remove TBP degradation products, which adds complexity to the recycling plant and increases the overall plant footprint and cost. A liquid or supercritical carbon dioxide (l/sc -CO2) system was designed tomore » mitigate these problems. Indeed, TBP nitric acid complexes are highly soluble in l/sc -CO2 and are capable of extracting uranium directly from UO2, UO3 and U3O8 powders. This eliminates the need for total acid dissolution of the irradiated fuel. Furthermore, since CO2 is easily recycled by evaporation at room temperature and pressure, it eliminates the complex solvent washing process. In this report, we demonstrate: (1) A reprocessing scheme starting with the selective extraction of uranium from solid uranium oxides into a TBP-HNO3 loaded Sc-CO2 phase, (2) Back extraction of uranium into an aqueous phase, and (3) Conversion of recovered purified uranium into uranium oxide. The purified uranium product from step 3 can be disposed of as low level waste, or mixed with enriched uranium for use in a reactor for another fuel cycle. After an introduction on the concept and properties of supercritical fluids, we first report the characterization of the different oxides used for this project. Our extraction system and our online monitoring capability using UV-Vis absorbance spectroscopy directly in sc-CO2 is then presented. Next, the uranium extraction efficiencies and kinetics is demonstrated for different oxides and under different physical and chemical conditions: l/sc -CO2 pressure and temperature, TBP/HNO3 complex used, reductant or complexant used for selectivity, and ionic liquids used as supportive media. To complete the extraction and recovery cycle, we then demonstrate uranium back extraction from the TBP loaded sc-CO2 phase into an aqueous phase and the characterization of the uranium complex formed at the end of this process. Another aspect of this project was to limit proliferation risks by either co-extracting uranium and plutonium, or by leaving plutonium behind by selectively extracting uranium. We report that the former is easily achieved, since plutonium is in the tetravalent or hexavalent oxidation state in the oxidizing environment created by the TBP-nitric acid complex, and is therefore co-extracted. The latter is more challenging, as a reductant or complexant to plutonium has to be used to selectively extract uranium. After undertaking experiments on different reducing or complexing systems (e.g., AcetoHydroxamic Acid (AHA), Fe(II), ascorbic acid), oxalic acid was chosen as it can complex tetravalent actinides (Pu, Np, Th) in the aqueous phase while allowing the extraction of hexavalent uranium in the sc-CO2 phase. Finally, we show results using an alternative media to commonly used aqueous phases: ionic liquids. We show the dissolution of uranium in ionic liquids and its extraction using sc-CO2 with and without the presence of AHA. The possible separation of trivalent actinides from uranium is also demonstrated in ionic liquids using neodymium as a surrogate and diglycolamides as the extractant.« less
Separation by solvent extraction
Holt, Jr., Charles H.
1976-04-06
17. A process for separating fission product values from uranium and plutonium values contained in an aqueous solution, comprising adding an oxidizing agent to said solution to secure uranium and plutonium in their hexavalent state; contacting said aqueous solution with a substantially water-immiscible organic solvent while agitating and maintaining the temperature at from -1.degree. to -2.degree. C. until the major part of the water present is frozen; continuously separating a solid ice phase as it is formed; separating a remaining aqueous liquid phase containing fission product values and a solvent phase containing plutonium and uranium values from each other; melting at least the last obtained part of said ice phase and adding it to said separated liquid phase; and treating the resulting liquid with a new supply of solvent whereby it is practically depleted of uranium and plutonium.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Sullivan, N.
1995-05-02
This document provides the Functional Design Criteria (FDC) for Project C-018H, the 242-A Evaporator and Plutonium-Uranium Extraction (PUREX) Plant Condensate Treatment Facility (Also referred to as the 200 Area Effluent Treatment Facility [ETF]). The project will provide the facilities to treat and dispose of the 242-A Evaporator process condensate (PC), the Plutonium-Uranium Extraction (PUREX) Plant process condensate (PDD), and the PUREX Plant ammonia scrubber distillate (ASD).
SEPARATION OF RUTHENIUM FROM AQUEOUS SOLUTIONS
Callis, C.F.; Moore, R.L.
1959-09-01
>The separation of ruthenium from aqueous solutions containing uranium plutonium, ruthenium, and fission products is described. The separation is accomplished by providing a nitric acid solution of plutonium, uranium, ruthenium, and fission products, oxidizing plutonium to the hexavalent state with sodium dichromate, contacting the solution with a water-immiscible organic solvent, such as hexone, to extract plutonyl, uranyl, ruthenium, and fission products, reducing with sodium ferrite the plutonyl in the solvent phase to trivalent plutonium, reextracting from the solvent phase the trivalent plutonium, ruthenium, and some fission products with an aqueous solution containing a salting out agent, introducing ozone into the aqueous acid solution to oxidize plutonium to the hexavalent state and ruthenium to ruthenium tetraoxide, and volatizing off the ruthenium tetraoxide.
McDowell, W J; Farrar, D T; Billings, M R
1974-12-01
A method for the determination of uranium and plutonium by a combined high-resolution liquid scintillation-solvent extraction method is presented. Assuming a sample count equal to background count to be the detection limit, the lower detection limit for these and other alpha-emitting nuclides is 1.0 dpm with a Pyrex sample tube, 0.3 dpm with a quartz sample tube using present detector shielding or 0.02 d.p.m. with pulse-shape discrimination. Alpha-counting efficiency is 100%. With the counting data presented as an alpha-energy spectrum, an energy resolution of 0.2-0.3 MeV peak half-width and an energy identification to +/-0.1 MeV are possible. Thus, within these limits, identification and quantitative determination of a specific alpha-emitter, independent of chemical separation, are possible. The separation procedure allows greater than 98% recovery of uranium and plutonium from solution containing large amounts of iron and other interfering substances. In most cases uranium, even when present in 10(8)-fold molar ratio, may be quantitatively separated from plutonium without loss of the plutonium. Potential applications of this general analytical concept to other alpha-counting problems are noted. Special problems associated with the determination of plutonium in soil and water samples are discussed. Results of tests to determine the pulse-height and energy-resolution characteristics of several scintillators are presented. Construction of the high-resolution liquid scintillation detector is described.
Ferric ion as a scavenging agent in a solvent extraction process
Bruns, Lester E.; Martin, Earl C.
1976-01-01
Ferric ions are added into the aqueous feed of a plutonium scrap recovery process that employs a tributyl phosphate extractant. Radiolytic degradation products of tributyl phosphate such as dibutyl phosphate form a solid precipitate with iron and are removed from the extraction stages via the waste stream. Consequently, the solvent extraction characteristics are improved, particularly in respect to minimizing the formation of nonstrippable plutonium complexes in the stripping stages. The method is expected to be also applicable to the partitioning of plutonium and uranium in a scrap recovery process.
CONTINUOUS CHELATION-EXTRACTION PROCESS FOR THE SEPARATION AND PURIFICATION OF METALS
Thomas, J.R.; Hicks, T.E.; Rubin, B.; Crandall, H.W.
1959-12-01
A continuous process is presented for separating metal values and groups of metal values from each other. A complex mixture. e.g., neutron-irradiated uranium, can be resolved into component parts. In the present process the values are dissolved in an acidic solution and adjusted to the proper oxidation state. Thenceforth the solution is contacted with an extractant phase comprising a fluorinated beta -diketone in an organic solvent under centain pH conditions whereupon plutonium and zirconium are extracted. Plutonium is extracted from the foregoing extract with reducing aqueous solutions or under specified acidic conditions and can be recovered from the aqueous solution. Zirconium is then removed with an oxalic acid aqueous phase. The uranium is recovered from the residual original solution using hexone and hexone-diketone extractants leaving residual fission products in the original solution. The uranium is extracted from the hexone solution with dilute nitric acid. Improved separations and purifications are achieved using recycled scrub solutions and the "self-salting" effect of uranyl ions.
PYROCHEMICAL DECONTAMINATION METHOD FOR REACTOR FUEL
Buyers, A.G.
1959-06-30
A pyro-chemical method is presented for decontaminating neutron irradiated uranium and separating plutonium therefrom by contact in the molten state with a metal chloride salt. Uranium trichloride and uranium tetrachloride either alone or in admixture with alkaline metal and alkaline eanth metal fluorides under specified temperature and specified phase ratio conditions extract substantially all of the uranium from the irradiated uranium fuel together with certain fission products. The phases are then separated leaving purified uranium metal. The uranium and plutonium in the salt phase can be reduced to forin a highly decontaminated uraniumplutonium alloy. The present method possesses advantages for economically decontaminating irradiated nuclear fuel elements since irradiated fuel may be proccessed immediately after withdrawal from the reactor and the uranium need not be dissolved and later reduced to the metallic form. Accordingly, the uranium may be economically refabricated and reinserted into the reactor.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Reilly, Sean Douglas; Smith, Paul Herrick; Jarvinen, Gordon D.
Understanding the water solubility of plutonium and uranium compounds and residues at TA-55 is necessary to provide a technical basis for appropriate criticality safety, safety basis and accountability controls. Individual compound solubility was determined using published solubility data and solution thermodynamic modeling. Residue solubility was estimated using a combination of published technical reports and process knowledge of constituent compounds. The scope of materials considered includes all compounds and residues at TA-55 as of March 2016 that contain Pu-239 or U-235 where any single item in the facility has more than 500 g of nuclear material. This analysis indicates that themore » following materials are not appreciably soluble in water: plutonium dioxide (IDC=C21), plutonium phosphate (IDC=C66), plutonium tetrafluoride (IDC=C80), plutonium filter residue (IDC=R26), plutonium hydroxide precipitate (IDC=R41), plutonium DOR salt (IDC=R42), plutonium incinerator ash (IDC=R47), uranium carbide (IDC=C13), uranium dioxide (IDC=C21), U 3O 8 (IDC=C88), and uranium filter residue (IDC=R26). This analysis also indicates that the following materials are soluble in water: plutonium chloride (IDC=C19) and uranium nitrate (IDC=C52). Equilibrium calculations suggest that PuOCl is water soluble under certain conditions, but some plutonium processing reports indicate that it is insoluble when present in electrorefining residues (R65). Plutonium molten salt extraction residues (IDC=R83) contain significant quantities of PuCl 3, and are expected to be soluble in water. The solubility of the following plutonium residues is indeterminate due to conflicting reports, insufficient process knowledge or process-dependent composition: calcium salt (IDC=R09), electrorefining salt (IDC=R65), salt (IDC=R71), silica (IDC=R73) and sweepings/screenings (IDC=R78). Solution thermodynamic modeling also indicates that fire suppression water buffered with a commercially-available phosphate buffer would significantly reduce the solubility of PuCl 3 by the precipitation of PuPO 4.« less
The behaviour of tributyl phosphate in an organic diluent
NASA Astrophysics Data System (ADS)
Leay, Laura; Tucker, Kate; Del Regno, Annalaura; Schroeder, Sven L. M.; Sharrad, Clint A.; Masters, Andrew J.
2014-09-01
Tributyl phosphate (TBP) is used as a complexing agent in the Plutonium Uranium Extraction (PUREX) liquid-liquid phase extraction process for recovering uranium and plutonium from spent nuclear reactor fuel. Here, we address the molecular and microstructure of the organic phases involved in the extraction process, using molecular dynamics to show that when TBP is mixed with a paraffinic diluent, the TBP self-assembles into a bi-continuous phase. The underlying self-association of TBP is driven by intermolecular interaction between its polar groups, resulting in butyl moieties radiating out into the organic solvent. Simulation predicts a TBP diffusion constant that is anomalously low compared to what might normally be expected for its size; experimental nuclear magnetic resonance (NMR) studies also indicate an extremely low diffusion constant, consistent with a molecular aggregation model. Simulation of TBP at an oil/water interface shows the formation of a bilayer system at low TBP concentrations. At higher concentrations, a bulk bi-continuous structure is observed linking to this surface bilayer. We suggest that this structure may be intimately connected with the surprisingly rapid kinetics of the interfacial mass transport of uranium and plutonium from the aqueous to the organic phase in the PUREX process.
Processing of irradiated, enriched uranium fuels at the Savannah River Plant
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hyder, M L; Perkins, W C; Thompson, M C
Uranium fuels containing /sup 235/U at enrichments from 1.1% to 94% are processed and recovered, along with neptunium and plutonium byproducts. The fuels to be processed are dissolved in nitric acid. Aluminum-clad fuels are disssolved using a mercury catalyst to give a solution rich in aluminum. Fuels clad in more resistant materials are dissolved in an electrolytic dissolver. The resulting solutions are subjected to head-end treatment, including clarification and adjustment of acid and uranium concentration before being fed to solvent extraction. Uranium, neptunium, and plutonium are separated from fission products and from one another by multistage countercurrent solvent extraction withmore » dilute tri-n-butyl phosphate in kerosene. Nitric acid is used as the salting agent in addition to aluminum or other metal nitrates present in the feed solution. Nuclear safety is maintained through conservative process design and the use of monitoring devices as secondary controls. The enriched uranium is recovered as a dilute solution and shipped off-site for further processing. Neptunium is concentrated and sent to HB-Line for recovery from solution. The relatively small quantities of plutonium present are normally discarded in aqueous waste, unless the content of /sup 238/Pu is high enough to make its recovery desirable. Most of the /sup 238/Pu can be recovered by batch extraction of the waste solution, purified by counter-current solvent extraction, and converted to oxide in HB-Line. By modifying the flowsheet, /sup 239/Pu can be recovered from low-enriched uranium in the extraction cycle; neptunium is then not recovered. The solvent is subjected to an alkaline wash before reuse to remove degraded solvent and fission products. The aqueous waste is concentrated and partially deacidified by evaporation before being neutralized and sent to the waste tanks; nitric acid from the overheads is recovered for reuse.« less
Plutonium recovery from spent reactor fuel by uranium displacement
Ackerman, John P.
1992-01-01
A process for separating uranium values and transuranic values from fission products containing rare earth values when the values are contained together in a molten chloride salt electrolyte. A molten chloride salt electrolyte with a first ratio of plutonium chloride to uranium chloride is contacted with both a solid cathode and an anode having values of uranium and fission products including plutonium. A voltage is applied across the anode and cathode electrolytically to transfer uranium and plutonium from the anode to the electrolyte while uranium values in the electrolyte electrolytically deposit as uranium metal on the solid cathode in an amount equal to the uranium and plutonium transferred from the anode causing the electrolyte to have a second ratio of plutonium chloride to uranium chloride. Then the solid cathode with the uranium metal deposited thereon is removed and molten cadmium having uranium dissolved therein is brought into contact with the electrolyte resulting in chemical transfer of plutonium values from the electrolyte to the molten cadmium and transfer of uranium values from the molten cadmium to the electrolyte until the first ratio of plutonium chloride to uranium chloride is reestablished.
Speciation of plutonium and other metals under UREX process conditIONS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Paulenova, Alena; Tkac, Peter; Matteson, Brent S.
2007-07-01
The extractability of various Pu and Np species into tri-n-butyl phosphate (TBP) was investigated. The concentration effects of aceto-hydroxamic acid, nitric acid and nitrate on the distribution ratio of U, Pu and Np were investigated. The considerable ability of AHA to form complexes with the studied elements even under strong acidic conditions was found. While the difference in the extraction of uranyl in the presence and absence of AHA is minimal, extraction yields of Pu and Np decrease significantly. The UV-Vis-NIR and FT-IR spectroscopic investigations of uranium, plutonium, and neptunium species in the presence and absence of AHA in bothmore » aqueous and organic extraction phase were also performed. Spectroscopic analysis showed that the organic phase can contain a substantial amount of metal-hydroxamate species. A solvated ternary complex of uranium UO{sub 2}.AHA.NO{sub 3}.2TBP was observed only after prolonged contact between the aqueous and organic phases, whereas the plutonium hydroxamate species, presumably Pu(AHA){sub x}(NO{sub 3}){sub 4-x}.2TBP, appeared in the organic phase after a four minute extraction. (authors)« less
Plutonium recovery from spent reactor fuel by uranium displacement
Ackerman, J.P.
1992-03-17
A process is described for separating uranium values and transuranic values from fission products containing rare earth values when the values are contained together in a molten chloride salt electrolyte. A molten chloride salt electrolyte with a first ratio of plutonium chloride to uranium chloride is contacted with both a solid cathode and an anode having values of uranium and fission products including plutonium. A voltage is applied across the anode and cathode electrolytically to transfer uranium and plutonium from the anode to the electrolyte while uranium values in the electrolyte electrolytically deposit as uranium metal on the solid cathode in an amount equal to the uranium and plutonium transferred from the anode causing the electrolyte to have a second ratio of plutonium chloride to uranium chloride. Then the solid cathode with the uranium metal deposited thereon is removed and molten cadmium having uranium dissolved therein is brought into contact with the electrolyte resulting in chemical transfer of plutonium values from the electrolyte to the molten cadmium and transfer of uranium values from the molten cadmium to the electrolyte until the first ratio of plutonium chloride to uranium chloride is reestablished.
Spent nuclear fuel recycling with plasma reduction and etching
Kim, Yong Ho
2012-06-05
A method of extracting uranium from spent nuclear fuel (SNF) particles is disclosed. Spent nuclear fuel (SNF) (containing oxides of uranium, oxides of fission products (FP) and oxides of transuranic (TRU) elements (including plutonium)) are subjected to a hydrogen plasma and a fluorine plasma. The hydrogen plasma reduces the uranium and plutonium oxides from their oxide state. The fluorine plasma etches the SNF metals to form UF6 and PuF4. During subjection of the SNF particles to the fluorine plasma, the temperature is maintained in the range of 1200-2000 deg K to: a) allow any PuF6 (gas) that is formed to decompose back to PuF4 (solid), and b) to maintain stability of the UF6. Uranium (in the form of gaseous UF6) is easily extracted and separated from the plutonium (in the form of solid PuF4). The use of plasmas instead of high temperature reactors or flames mitigates the high temperature corrosive atmosphere and the production of PuF6 (as a final product). Use of plasmas provide faster reaction rates, greater control over the individual electron and ion temperatures, and allow the use of CF4 or NF3 as the fluorine sources instead of F2 or HF.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lopez-Menchero, E.; Centeno, J.; Magni, G.
1962-03-01
The extraction of traces of Ru, Zr, Nb, Ce, and U at low concentrations (5 mg/l in aqueous solution) from nitric acid solutions using trilauryl amine (TLA) has been experimentally studied. TLA will eventually be used for final purification of plutonium. Room-temperature data on plutonium contaminant distribution between aqueous solutions of varying nitric acid concentrations and a Shellsol-T solution containing l0% TlA and 5% octyl alcohol are presented. Within the temperature and nitric acid concentration ranges tested, the extractability of uranium increased with increased acid concentrations, although acid concentration in the aqueous phase had no effect on the decontamination factorsmore » for the main fission products. (H.G.G.)« less
PROCESS FOR SEPARATING PLUTONIUM FROM IMPURITIES
Wahl, A.C.
1957-11-12
A method is described for separating plutonium from aqueous solutions containing uranium. It has been found that if the plutonium is reduced to its 3+ valence state, and the uranium present is left in its higher valence state, then the differences in solubility between certain salts (e.g., oxalates) of the trivalent plutonium and the hexavalent uranium can be used to separate the metals. This selective reduction of plutonium is accomplished by adding iodide ion to the solution, since iodide possesses an oxidation potential sufficient to reduce plutonium but not sufficient to reduce uranium.
Natural radionuclide and plutonium content in Black Sea bottom sediments
DOE Office of Scientific and Technical Information (OSTI.GOV)
Strezov, A.; Stoilova, T.; Yordanova, I.
1996-01-01
The content of uranium, thorium, radium, lead, polonium, and plutonium in bottom sediments and algae from two locations at the Bulgarian Black Sea coast have been determined. Some parent:progeny ratios for evaluation of the geochemical behavior of the nuclides have been estimated as well. The extractable and total uranium and thorium are determined by two separate radiochemical procedures to differentiate the more soluble chemical forms of the elements and to estimate the potential hazard for the biosphere and for humans. No distinct seasonal variation as well as no significant change in total and extractable uranium (also for {sup 226}Ra) contentmore » is observed. The same is valid for extractable thorium while the total thorium content in the first two seasons is slightly higher. Our data show that {sup 210}Po content is accumulated more in the sediments than {sup 210}Pb, and the evaluated disequilibria suggest that the two radionuclides belong to more recent sediment layers deposited in the slime samples compared to the silt ones for the different seasons. The obtained values for plutonium are in the lower limits of the data cited in literature, which is quite clear as there are no plutonium discharge facilities at the Bulgarian Black Sea coast. The obtained values for the activity ratio {sup 238}Pu: {sup 239+240}Pu are higher for Bjala sediments compared to those of Kaliakra. The ratio values are out of the variation range for the global contamination with weapon tests fallout plutonium which is probably due to Chernobyl accident contribution. The dependence of natural radionuclide content on the sediment type as well as the variation of nuclide accumulation for two types of algae in two sampling locations for five consecutive seasons is evaluated. No serious contamination with natural radionuclides in the algae is observed. 38 refs., 6 figs., 7 tabs.« less
Rapid Method for Sodium Hydroxide Fusion of Concrete and ...
Technical Fact Sheet Analysis Purpose: Qualitative analysis Technique: Alpha spectrometry Method Developed for: Americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in concrete and brick samples Method Selected for: SAM lists this method for qualitative analysis of americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in concrete or brick building materials. Summary of subject analytical method which will be posted to the SAM website to allow access to the method.
Multiple recycle of REMIX fuel at VVER-1000 operation in closed fuel cycle
NASA Astrophysics Data System (ADS)
Alekseev, P. N.; Bobrov, E. A.; Chibinyaev, A. V.; Teplov, P. S.; Dudnikov, A. A.
2015-12-01
The basic features of loading the VVER-1000 core with a new variant of REMIX fuel (REgenerated MIXture of U-Pu oxides) are considered during its multiple recycle in a closed nuclear fuel cycle. The fuel composition is produced on the basis of the uranium-plutonium regenerate extracted at processing the spent nuclear fuel (SNF) from a VVER-1000, depleted uranium, and the fissionable material: 235U as a part of highly enriched uranium (HEU) from warheads superfluous for defense purposes or 233U accumulated in thorium blankets of fusion (electronuclear) neutron sources or fast reactors. Production of such a fuel assumes no use of natural uranium in addition. When converting a part of the VVER-1000 reactors to the closed fuel cycle based on the REMIX technology, the consumption of natural uranium decreases considerably, and there is no substantial degradation of the isotopic composition of plutonium or change in the reactor-safety characteristics at the passage from recycle to recycle.
Volatile fluoride process for separating plutonium from other materials
Spedding, F. H.; Newton, A. S.
1959-04-14
The separation of plutonium from uranium and/or fission products by formation of the higher fluorides off uranium and/or plutonium is described. Neutronirradiated uranium metal is first converted to the hydride. This hydrided product is then treated with fluorine at about 315 deg C to form and volatilize UF/sub 6/ leaving plutonium behind. Thc plutonium may then be separated by reacting the residue with fluorine at about 5004DEC and collecting the volatile plutonium fluoride thus formed.
VOLATILE FLUORIDE PROCESS FOR SEPARATING PLUTONIUM FROM OTHER MATERIALS
Spedding, F.H.; Newton, A.S.
1959-04-14
The separation of plutonium from uranium and/or tission products by formation of the higher fluorides of uranium and/or plutonium is discussed. Neutronirradiated uranium metal is first convcrted to the hydride. This hydrided product is then treatced with fluorine at about 315 deg C to form and volatilize UF/sup 6/ leaving plutonium behind. The plutonium may then be separated by reacting the residue with fluorine at about 500 deg C and collecting the volatile plutonium fluoride thus formed.
METHOD OF SEPARATING URANIUM VALUES, PLUTONIUM VALUES AND FISSION PRODUCTS BY CHLORINATION
Brown, H.S.; Seaborg, G.T.
1959-02-24
The separation of plutonium and uranium from each other and from other substances is described. In general, the method comprises the steps of contacting the uranium with chlorine in the presence of a holdback material selected from the group consisting of lanthanum oxide and thorium oxide to form a uranium chloride higher than uranium tetrachloride, and thereafter heating the uranium chloride thus formed to a temperature at which the uranium chloride is volatilized off but below the volatilizalion temperature of plutonium chloride.
ADSORPTION-BISMUTH PHOSPHATE METHOD FOR SEPARATING PLUTONIUM
Russell, E.R.; Adamson, A.W.; Boyd, G.E.
1960-06-28
A process is given for separating plutonium from uranium and fission products. Plutonium and uranium are adsorbed by a cation exchange resin, plutonium is eluted from the adsorbent, and then, after oxidation to the hexavalent state, the plutonium is contacted with a bismuth phosphate carrier precipitate.
Combined transuranic-strontium extraction process
Horwitz, E.P.; Dietz, M.L.
1992-12-08
The transuranic (TRU) elements neptunium, plutonium and americium can be separated together with strontium from nitric acid waste solutions in a single process. An extractant solution of a crown ether and an alkyl(phenyl)-N,N-dialkylcarbanylmethylphosphine oxide in an appropriate diluent will extract the TRU's together with strontium, uranium and technetium. The TRU's and the strontium can then be selectively stripped from the extractant for disposal. 3 figs.
Combined transuranic-strontium extraction process
Horwitz, E. Philip; Dietz, Mark L.
1992-01-01
The transuranic (TRU) elements neptunium, plutonium and americium can be separated together with strontium from nitric acid waste solutions in a single process. An extractant solution of a crown ether and an alkyl(phenyl)-N,N-dialkylcarbanylmethylphosphine oxide in an appropriate diluent will extract the TRU's together with strontium, uranium and technetium. The TRU's and the strontium can then be selectively stripped from the extractant for disposal.
Evaluation of N,N-dialkylamides as promising process extractants
NASA Astrophysics Data System (ADS)
Pathak, P. N.; Prabhu, D. R.; Kanekar, A. S.; Manchanda, V. K.
2010-03-01
Studies carried out at BARC, India on the development of new extractants for reprocessing of spent fuel suggested that while straight chain N,N-dihexyloctanamide (DHOA) is promising alternative to TBP for the reprocessing of irradiated uranium based fuels, branched chain N,N-di(2-ethylhexyl)isobutyramide (D2EHIBA) is suitable for the selective recovery of 233U from irradiated Th. In advanced fuel cycle scenarios, the coprocessing of U/Pu stream appears attractive particularly with respect to development of proliferation resistant technologies. DHOA extracted Pu(IV) more efficiently than TBP, both at trace-level concentration as well as under uranium/plutonium loading conditions. Uranium extraction behavior of DHOA was however, similar to that of TBP during the extraction cycle. Stripping behavior of U and Pu (without any reductant) was better for DHOA than that of TBP. It was observed during batch studies that whereas 99% Pu is stripped in four stages in case of DHOA, only 89% Pu is stripped in case of TBP under identical experimental conditions. DHOA offered better fission product decontamination than that of TBP. GANEX (Group ActiNide EXtraction) and ARTIST (Amide-based Radio-resources Treatment with Interim Storage of Transuranics) processes proposed for actinide partitioning use branched chain amides for the selective extraction of uranium from spent fuel feed solutions. The branched-alkyl monoamide (BAMA) proposed to be used in ARTIST process is N,N-di-(2-ethylhexyl)butyramide (D2EHBA). In this context, the extraction behavior of U(VI) and Pu(IV) were compared using D2EHIBA, TBP, and D2EHBA under similar concentration of nitric acid (0.5 — 6M) and of uranium (0-50g/L). These studies suggested that D2EHIBA is a promising extractant for selective extraction of uranium over plutonium in process streams. Similarly, D2EHIBA offered distinctly better decontamination of 233U over Th and fission products under THOREX feed conditions. The possibility of simultaneous stripping and precipitation of thorium (as oxalate) from loaded organic phase was explored using 0.05M oxalic acid. Ammonium diuranate (ADU) precipitation was performed on the oxalate supernatant for the recovery of uranium. Quantitative recovery (>99.9%) of Th as well as of U was achieved. Radiolytic studies suggested that irradiated DHOA and D2EHIBA behaved better with respect to fission product decontamination as compared to that of TBP.
Code of Federal Regulations, 2010 CFR
2010-01-01
... reactors, flame tower reactors, liquid centrifuges, distillation columns and liquid-liquid extraction... to UF6 is performed by exothermic reaction with fluorine in a tower reactor. UF6 is condensed from..., flame tower reactors, liquid centrifuges, distillation columns and liquid-liquid extraction columns. Hot...
SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS
Boyd, G.E.; Adamson, A.W.; Schubert, J.; Russell, E.R.
1958-10-01
A chromatographic adsorption process is presented for the separation of plutonium from other fission products formed by the irradiation of uranium. The plutonium and the lighter element fission products are adsorbed on a sulfonated phenol-formaldehyde resin bed from a nitric acid solution containing the dissolved uranium. Successive washes of sulfuric, phosphoric, and nitric acids remove the bulk of the fission products, then an eluate of dilute phosphoric and nitric acids removes the remaining plutonium and fission products. The plutonium is selectively removed by passing this solution through zirconium phosphate, from which the plutonium is dissolved with nitric acid. This process provides a convenient and efficient means for isolating plutonium.
The Best Defense: Making Maximum Sense of Minimum Deterrence
2011-06-01
uranium fuel cycles and has unmatched experience in the thorium fuel cycle.25 Published sources claim India produces between 20 and 40kg of plutonium...nuclear energy was moderate at best. Pakistan‘s first reactor , which it received from the United States, did not become operational until 1965.4...In 1974 Pakistan signed an agreement with France to supply a reprocessing plant for extracting plutonium from spent fuel from power reactors
PROCESS FOR THE SEPARATION OF HEAVY METALS
Gofman, J.W.; Connick, R.E.; Wahl, A.C.
1959-01-27
A method is presented for thc separation of plutonium from uranium and the fission products with which it is associated. The method is based on the fact that hexavalent plutonium forms an insoluble complex precipitate with sodium acetate, as does the uranyl ion, while reduced plutonium is not precipitated by sodium acetate. Several embodiments are shown, e.g., a solution containing plutonium and uranium in the hexavalent state may be contacted with sodium acetate causing the formation of a sodium uranyl acetate precipitate which carries the plutonium values while the fission products remain in solution. If the original solution is treated with a reducing agent, so that the plutonium is reduced while the uranium remains in the hexavalent state, and sodium and acetate ions are added, the uranium will precipitutc while the plutonium remains in solution effecting separation of the Pu from urarium.
Multiple recycle of REMIX fuel at VVER-1000 operation in closed fuel cycle
DOE Office of Scientific and Technical Information (OSTI.GOV)
Alekseev, P. N.; Bobrov, E. A., E-mail: evgeniybobrov89@rambler.ru; Chibinyaev, A. V.
2015-12-15
The basic features of loading the VVER-1000 core with a new variant of REMIX fuel (REgenerated MIXture of U–Pu oxides) are considered during its multiple recycle in a closed nuclear fuel cycle. The fuel composition is produced on the basis of the uranium–plutonium regenerate extracted at processing the spent nuclear fuel (SNF) from a VVER-1000, depleted uranium, and the fissionable material: {sup 235}U as a part of highly enriched uranium (HEU) from warheads superfluous for defense purposes or {sup 233}U accumulated in thorium blankets of fusion (electronuclear) neutron sources or fast reactors. Production of such a fuel assumes no usemore » of natural uranium in addition. When converting a part of the VVER-1000 reactors to the closed fuel cycle based on the REMIX technology, the consumption of natural uranium decreases considerably, and there is no substantial degradation of the isotopic composition of plutonium or change in the reactor-safety characteristics at the passage from recycle to recycle.« less
Ackerman, John P.; Miller, William E.
1989-01-01
An electrorefining process and apparatus for the recovery of uranium and a mixture of uranium and plutonium from spent fuel using an electrolytic cell having a lower molten cadmium pool containing spent nuclear fuel, an intermediate electrolyte pool, an anode basket containing spent fuel, and two cathodes, the first cathode composed of either a solid alloy or molten cadmium and the second cathode composed of molten cadmium. Using this cell, additional amounts of uranium and plutonium from the anode basket are dissolved in the lower molten cadmium pool, and then substantially pure uranium is electrolytically transported and deposited on the first alloy or molten cadmium cathode. Subsequently, a mixture of uranium and plutonium is electrotransported and deposited on the second molten cadmium cathode.
Ackerman, J.P.; Miller, W.E.
1987-11-05
An electrorefining process and apparatus for the recovery of uranium and a mixture of uranium and plutonium from spent fuels is disclosed using an electrolytic cell having a lower molten cadmium pool containing spent nuclear fuel, an intermediate electrolyte pool, an anode basket containing spent fuels, two cathodes and electrical power means connected to the anode basket, cathodes and lower molten cadmium pool for providing electrical power to the cell. Using this cell, additional amounts of uranium and plutonium from the anode basket are dissolved in the lower molten cadmium pool, and then purified uranium is electrolytically transported and deposited on a first molten cadmium cathode. Subsequently, a mixture of uranium and plutonium is electrotransported and deposited on a second cathode. 3 figs.
Method for the recovery of actinide elements from nuclear reactor waste
Horwitz, E. Philip; Delphin, Walter H.; Mason, George W.
1979-01-01
A process for partitioning and recovering actinide values from acidic waste solutions resulting from reprocessing of irradiated nuclear fuels by adding hydroxylammonium nitrate and hydrazine to the waste solution to adjust the valence of the neptunium and plutonium values in the solution to the +4 oxidation state, thus forming a feed solution and contacting the feed solution with an extractant of dihexoxyethyl phosphoric acid in an organic diluent whereby the actinide values, most of the rare earth values and some fission product values are taken up by the extractant. Separation is achieved by contacting the loaded extractant with two aqueous strip solutions, a nitric acid solution to selectively strip the americium, curium and rare earth values and an oxalate solution of tetramethylammonium hydrogen oxalate and oxalic acid or trimethylammonium hydrogen oxalate to selectively strip the neptunium, plutonium and fission product values. Uranium values remain in the extractant and may be recovered with a phosphoric acid strip. The neptunium and plutonium values are recovered from the oxalate by adding sufficient nitric acid to destroy the complexing ability of the oxalate, forming a second feed, and contacting the second feed with a second extractant of tricaprylmethylammonium nitrate in an inert diluent whereby the neptunium and plutonium values are selectively extracted. The values are recovered from the extractant with formic acid.
SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Boyd, G.E.; Adamson, A.W.; Schubert, J.
A chromatographic adsorption process is presented for the separation of plutonium from other fission products formed by the irradiation of uranium. The plutonium and the lighter element fission products are adsorbed on a sulfonated phenol-formaldehyde resin bed from a nitric acid solution containing the dissolved uranium. Successive washes of sulfuric, phosphoric, and nitric acids remove the bulk of the fission products, then an eluate of dilute phosphoric and nitric acids removes the remaining plutonium and fission products. The plutonium is selectively removed by passing this solution through zirconium phosphate, from which the plutonium is dissolved with nitric acid. This processmore » provides a convenient and efficient means for isolating plutonium.« less
METHOD OF PREPARING URANIUM, THORIUM, OR PLUTONIUM OXIDES IN LIQUID BISMUTH
Davidson, J.K.; Robb, W.L.; Salmon, O.N.
1960-11-22
A method is given for forming compositions, as well as the compositions themselves, employing uranium hydride in a liquid bismuth composition to increase the solubility of uranium, plutonium and thorium oxides in the liquid bismuth. The finely divided oxide of uranium, plutonium. or thorium is mixed with the liquid bismuth and uranium hydride, the hydride being present in an amount equal to about 3 at. %, heated to about 5OO deg C, agitated and thereafter cooled and excess resultant hydrogen removed therefrom.
Steindler, M.J.
1962-07-24
A process was developed for separating uranium hexafluoride from plutonium hexafluoride by the selective reduction of the plutonium hexafluoride to the tetrafluoride with sulfur tetrafluoride at 50 to 120 deg C, cooling the mixture to --60 to -100 deg C, and volatilizing nonreacted sulfur tetrafluoride and sulfur hexafluoride formed at that temperature. The uranium hexafluoride is volatilized at room temperature away from the solid plutonium tetrafluoride. (AEC)
Code of Federal Regulations, 2011 CFR
2011-01-01
... reactors, flame tower reactors, liquid centrifuges, distillation columns and liquid-liquid extraction... UF4 to UF6 is performed by exothermic reaction with fluorine in a tower reactor. UF6 is condensed from..., flame tower reactors, liquid centrifuges, distillation columns and liquid-liquid extraction columns. Hot...
PROCESSES FOR SEPARATING AND RECOVERING CONSTITUENTS OF NEUTRON IRRADIATED URANIUM
Connick, R.E.; Gofman, J.W.; Pimentel, G.C.
1959-11-10
Processes are described for preparing plutonium, particularly processes of separating plutonium from uranium and fission products in neutron-irradiated uraniumcontaining matter. Specifically, plutonium solutions containing uranium, fission products and other impurities are contacted with reducing agents such as sulfur dioxide, uranous ion, hydroxyl ammonium chloride, hydrogen peroxide, and ferrous ion whereby the plutoninm is reduced to its fluoride-insoluble state. The reduced plutonium is then carried out of solution by precipitating niobic oxide therein. Uranium and certain fission products remain behind in the solution. Certain other fission products precipitate along with the plutonium. Subsequently, the plutonium and fission product precipitates are redissolved, and the solution is oxidized with oxidizing agents such as chlorine, peroxydisulfate ion in the presence of silver ion, permanganate ion, dichromate ion, ceric ion, and a bromate ion, whereby plutonium is oxidized to the fluoride-soluble state. The oxidized solution is once again treated with niobic oxide, thus precipitating the contamirant fission products along with the niobic oxide while the oxidized plutonium remains in solution. Plutonium is then recovered from the decontaminated solution.
PLUTONIUM-URANIUM-TITANIUM ALLOYS
Coffinberry, A.S.
1959-07-28
A plutonium-uranium alloy suitable for use as the fuel element in a fast breeder reactor is described. The alloy contains from 15 to 60 at.% titanium with the remainder uranium and plutonium in a specific ratio, thereby limiting the undesirable zeta phase and rendering the alloy relatively resistant to corrosion and giving it the essential characteristic of good mechanical workability.
PROCESS FOR SEPARATION OF HEAVY METALS
Duffield, R.B.
1958-04-29
A method is described for separating plutonium from aqueous acidic solutions of neutron-irradiated uranium and the impurities associated therewith. The separation is effected by adding, to the solution containing hexavalent uranium and plutonium, acetate ions and the ions of an alkali metal and those of a divalent metal and thus forming a complex plutonium acetate salt which is carried by the corresponding complex of uranium, such as sodium magnesium uranyl acetate. The plutonium may be separated from the precipitated salt by taking the same back into solution, reducing the plutonium to a lower valent state on reprecipitating the sodium magnesium uranyl salt, removing the latter, and then carrying the plutonium from ihe solution by means of lanthanum fluoride.
SEPARATION OF URANIUM, PLUTONIUM AND FISSION PRODUCTS FROM NEUTRON- BOMBARDED URANIUM
Martin, A.E.; Johnson, I.; Burris, L. Jr.; Winsch, I.O.; Feder, H.M.
1962-11-13
A process is given for removing plutonium and/or fission products from uranium fuel. The fuel is dissolved in molten zinc--magnesium (10 to 18% Mg) alloy, more magnesium is added to obtain eutectic composition whereby uranium precipitates, and the uranium are separated from the Plutoniumand fission-product- containing eutectic. (AEC)
Rapid extraction and assay of uranium from environmental surface samples
DOE Office of Scientific and Technical Information (OSTI.GOV)
Barrett, Christopher A.; Chouyyok, Wilaiwan; Speakman, Robert J.
Extraction methods enabling faster removal and concentration of uranium compounds for improved trace and low-level assay are demonstrated for standard surface sampling material in support of nuclear safeguards efforts, health monitoring, and other nuclear analysis applications. A key problem with the existing surface sampling swipes is the requirement for complete digestion of sample and sampling matrix. This is a time-consuming and labour-intensive process that limits laboratory throughput, elevates costs, and increases background levels. Various extraction methods are explored for their potential to quickly and efficiently remove different chemical forms of uranium from standard surface sampling material. A combination of carbonatemore » and peroxide solutions is shown to give the most rapid and complete form of uranyl compound extraction and dissolution. This rapid extraction process is demonstrated to be compatible with standard inductive coupled plasma mass spectrometry methods for uranium isotopic assay as well as screening techniques such as x-ray fluorescence. The general approach described has application beyond uranium to other analytes of nuclear forensic interest (e.g., rare earth elements and plutonium) as well as heavy metals for environmental and industrial hygiene monitoring.« less
NASA Astrophysics Data System (ADS)
Fisenko, Anatoliy I.; Lemberg, Vladimir F.
2016-09-01
The knowledge of thermal radiative and thermodynamic properties of uranium and plutonium carbides under extreme conditions is essential for designing a new metallic fuel materials for next generation of a nuclear reactor. The present work is devoted to the study of the thermal radiative and thermodynamic properties of liquid and solid uranium and plutonium carbides at their melting/freezing temperatures. The Stefan-Boltzmann law, total energy density, number density of photons, Helmholtz free energy density, internal energy density, enthalpy density, entropy density, heat capacity at constant volume, pressure, and normal total emissivity are calculated using experimental data for the frequency dependence of the normal spectral emissivity of liquid and solid uranium and plutonium carbides in the visible-near infrared range. It is shown that the thermal radiative and thermodynamic functions of uranium carbide have a slight difference during liquid-to-solid transition. Unlike UC, such a difference between these functions have not been established for plutonium carbide. The calculated values for the normal total emissivity of uranium and plutonium carbides at their melting temperatures is in good agreement with experimental data. The obtained results allow to calculate the thermal radiative and thermodynamic properties of liquid and solid uranium and plutonium carbides for any size of samples. Based on the model of Hagen-Rubens and the Wiedemann-Franz law, a new method to determine the thermal conductivity of metals and carbides at the melting points is proposed.
10 CFR 71.22 - General license: Fissile material.
Code of Federal Regulations, 2011 CFR
2011-01-01
... to obtain the value of X, then the values for the terms in the equation for uranium-233 and plutonium... if: (i) Uranium-233 is present in the package; (ii) The mass of plutonium exceeds 1 percent of the mass of uranium-235; (iii) The uranium is of unknown uranium-235 enrichment or greater than 24 weight...
10 CFR 71.22 - General license: Fissile material.
Code of Federal Regulations, 2012 CFR
2012-01-01
... to obtain the value of X, then the values for the terms in the equation for uranium-233 and plutonium... if: (i) Uranium-233 is present in the package; (ii) The mass of plutonium exceeds 1 percent of the mass of uranium-235; (iii) The uranium is of unknown uranium-235 enrichment or greater than 24 weight...
10 CFR 71.22 - General license: Fissile material.
Code of Federal Regulations, 2014 CFR
2014-01-01
... to obtain the value of X, then the values for the terms in the equation for uranium-233 and plutonium... if: (i) Uranium-233 is present in the package; (ii) The mass of plutonium exceeds 1 percent of the mass of uranium-235; (iii) The uranium is of unknown uranium-235 enrichment or greater than 24 weight...
10 CFR 71.22 - General license: Fissile material.
Code of Federal Regulations, 2010 CFR
2010-01-01
... to obtain the value of X, then the values for the terms in the equation for uranium-233 and plutonium... if: (i) Uranium-233 is present in the package; (ii) The mass of plutonium exceeds 1 percent of the mass of uranium-235; (iii) The uranium is of unknown uranium-235 enrichment or greater than 24 weight...
10 CFR 71.22 - General license: Fissile material.
Code of Federal Regulations, 2013 CFR
2013-01-01
... to obtain the value of X, then the values for the terms in the equation for uranium-233 and plutonium... if: (i) Uranium-233 is present in the package; (ii) The mass of plutonium exceeds 1 percent of the mass of uranium-235; (iii) The uranium is of unknown uranium-235 enrichment or greater than 24 weight...
DOE Office of Scientific and Technical Information (OSTI.GOV)
Fedorov, Y.S.; Bibichev, B.A.; Zilberman, B.Y.
2013-07-01
REMIX fuel consumption in WWER-1000 is considered. REMIX fuel is fabricated from non-separated mixture of uranium and plutonium obtained during NPP spent fuel reprocessing with further makeup by enriched natural uranium. It makes possible to recycle several times the total amount of uranium and plutonium obtained from spent fuel with 100% loading of the WWER-1000 core. The stored SNF could be also involved in REMIX fuel cycle by enrichment of regenerated uranium. The same approach could be applied to closing the fuel cycle of CANDU reactors. (authors)
Density functional theory study of defects in unalloyed δ-Pu
Hernandez, S. C.; Freibert, F. J.; Wills, J. M.
2017-03-19
Using density functional theory, we explore in this paper various classical point and complex defects within the face-centered cubic unalloyed δ-plutonium matrix that are potentially induced from self-irradiation. For plutonium only defects, the most energetically stable defect is a distorted split-interstitial. Gallium, the δ-phase stabilizer, is thermodynamically stable as a substitutional defect, but becomes unstable when participating in a complex defect configuration. Finally, complex uranium defects may thermodynamically exist as uranium substitutional with neighboring plutonium interstitial and stabilization of uranium within the lattice is shown via partial density of states and charge density difference plots to be 5f hybridization betweenmore » uranium and plutonium.« less
Density functional theory study of defects in unalloyed δ-Pu
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hernandez, S. C.; Freibert, F. J.; Wills, J. M.
Using density functional theory, we explore in this paper various classical point and complex defects within the face-centered cubic unalloyed δ-plutonium matrix that are potentially induced from self-irradiation. For plutonium only defects, the most energetically stable defect is a distorted split-interstitial. Gallium, the δ-phase stabilizer, is thermodynamically stable as a substitutional defect, but becomes unstable when participating in a complex defect configuration. Finally, complex uranium defects may thermodynamically exist as uranium substitutional with neighboring plutonium interstitial and stabilization of uranium within the lattice is shown via partial density of states and charge density difference plots to be 5f hybridization betweenmore » uranium and plutonium.« less
Supercritical Fluid Extraction and Separation of Uranium from Other Actinides
DOE Office of Scientific and Technical Information (OSTI.GOV)
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 uraniummore » 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.« less
Code of Federal Regulations, 2010 CFR
2010-01-01
.... Critical assembly means special nuclear devices designed and used to sustain nuclear reactions, which may... reaction becomes self-sustaining. Design features means the design features of a nuclear facility specified... reaction (e.g., uranium-233, uranium-235, plutonium-238, plutonium-239, plutonium-241, neptunium-237...
Rapid Method for Sodium Hydroxide Fusion of Asphalt ...
Technical Brief--Addendum to Selected Analytical Methods (SAM) 2012 The method will be used for qualitative analysis of americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in asphalt matrices samples.
10 CFR 150.14 - Commission regulatory authority for physical protection.
Code of Federal Regulations, 2012 CFR
2012-01-01
... significance in quantities greater than 15 grams of plutonium or uranium-233 or uranium-235 (enriched to 20 percent or more in the U-235 isotope) or any combination greater than 15 grams when computed by the equation grams=grams uranium-235+grams plutonium+grams uranium-233 shall meet the physical protection...
10 CFR 150.14 - Commission regulatory authority for physical protection.
Code of Federal Regulations, 2010 CFR
2010-01-01
... significance in quantities greater than 15 grams of plutonium or uranium-233 or uranium-235 (enriched to 20 percent or more in the U-235 isotope) or any combination greater than 15 grams when computed by the equation grams=grams uranium-235+grams plutonium+grams uranium-233 shall meet the physical protection...
10 CFR 150.14 - Commission regulatory authority for physical protection.
Code of Federal Regulations, 2011 CFR
2011-01-01
... significance in quantities greater than 15 grams of plutonium or uranium-233 or uranium-235 (enriched to 20 percent or more in the U-235 isotope) or any combination greater than 15 grams when computed by the equation grams=grams uranium-235+grams plutonium+grams uranium-233 shall meet the physical protection...
10 CFR 150.14 - Commission regulatory authority for physical protection.
Code of Federal Regulations, 2013 CFR
2013-01-01
... significance in quantities greater than 15 grams of plutonium or uranium-233 or uranium-235 (enriched to 20 percent or more in the U-235 isotope) or any combination greater than 15 grams when computed by the equation grams=grams uranium-235+grams plutonium+grams uranium-233 shall meet the physical protection...
10 CFR 150.14 - Commission regulatory authority for physical protection.
Code of Federal Regulations, 2014 CFR
2014-01-01
... significance in quantities greater than 15 grams of plutonium or uranium-233 or uranium-235 (enriched to 20 percent or more in the U-235 isotope) or any combination greater than 15 grams when computed by the equation grams=grams uranium-235+grams plutonium+grams uranium-233 shall meet the physical protection...
BASIC PEROXIDE PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINANTS
Seaborg, G.T.; Perlman, I.
1959-02-10
A process is described for the separation from each other of uranyl values, tetravalent plutonium values and fission products contained in an aqueous acidic solution. First the pH of the solution is adjusted to between 2.5 and 8 and hydrogen peroxide is then added to the solution causing precipitation of uranium peroxide which carries any plutonium values present, while the fission products remain in solution. Separation of the uranium and plutonium values is then effected by dissolving the peroxide precipitate in an acidic solution and incorporating a second carrier precipitate, selective for plutonium. The plutonium values are thus carried from the solution while the uranium remains flissolved. The second carrier precipitate may be selected from among the group consisting of rare earth fluorides, and oxalates, zirconium phosphate, and bismuth lihosphate.
PROCESS OF SEPARATING PLUTONIUM FROM URANIUM
Brown, H.S.; Hill, O.F.
1958-09-01
A process is presented for recovering plutonium values from aqueous solutions. It comprises forming a uranous hydroxide precipitate in such a plutonium bearing solution, at a pH of at least 5. The plutonium values are precipitated with and carried by the uranium hydroxide. The carrier precipitate is then redissolved in acid solution and the pH is adjusted to about 2.5, causing precipitation of the uranous hydroxide but leaving the still soluble plutonium values in solution.
COLUMBIC OXIDE ADSORPTION PROCESS FOR SEPARATING URANIUM AND PLUTONIUM IONS
Beaton, R.H.
1959-07-14
A process is described for separating plutonium ions from a solution of neutron irradiated uranium in which columbic oxide is used as an adsorbert. According to the invention the plutonium ion is selectively adsorbed by Passing a solution containing the plutonium in a valence state not higher than 4 through a porous bed or column of granules of hydrated columbic oxide. The adsorbed plutonium is then desorbed by elution with 3 N nitric acid.
Maddock, A.G.; Smith, F.
1959-08-25
A method is described for separating plutonium from uranium and fission products by treating a nitrate solution of fission products, uranium, and hexavalent plutonium with a relatively water-insoluble fluoride to adsorb fission products on the fluoride, treating the residual solution with a reducing agent for plutonium to reduce its valence to four and less, treating the reduced plutonium solution with a relatively insoluble fluoride to adsorb the plutonium on the fluoride, removing the solution, and subsequently treating the fluoride with its adsorbed plutonium with a concentrated aqueous solution of at least one of a group consisting of aluminum nitrate, ferric nitrate, and manganous nitrate to remove the plutonium from the fluoride.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Delegard, Calvin H.; Schmitt, Bruce E.; Schmidt, Andrew J.
2006-08-01
This report establishes the technical bases for using a ''slow uptake'' instead of a ''moderate uptake'' transportability class for americium-241 (241Am) for the K Basin Sludge Treatment Project (STP) dose consequence analysis. Slow uptake classes are used for most uranium and plutonium oxides. A moderate uptake class has been used in prior STP analyses for 241Am based on the properties of separated 241Am and its associated oxide. However, when 241Am exists as an ingrown progeny (and as a small mass fraction) within plutonium mixtures, it is appropriate to assign transportability factors of the predominant plutonium mixtures (typically slow) to themore » Am241. It is argued that the transportability factor for 241Am in sludge likewise should be slow because it exists as a small mass fraction as the ingrown progeny within the uranium oxide in sludge. In this report, the transportability class assignment for 241Am is underpinned with radiochemical characterization data on K Basin sludge and with studies conducted with other irradiated fuel exposed to elevated temperatures and conditions similar to the STP. Key findings and conclusions from evaluation of the characterization data and published literature are summarized here. Plutonium and 241Am make up very small fractions of the uranium within the K Basin sludge matrix. Plutonium is present at about 1 atom per 500 atoms of uranium and 241Am at about 1 atom per 19000 of uranium. Plutonium and americium are found to remain with uranium in the solid phase in all of the {approx}60 samples taken and analyzed from various sources of K Basin sludge. The uranium-specific concentrations of plutonium and americium also remain approximately constant over a uranium concentration range (in the dry sludge solids) from 0.2 to 94 wt%, a factor of {approx}460. This invariability demonstrates that 241Am does not partition from the uranium or plutonium fraction for any characterized sludge matrix. Most of the K Basin sludge characterization data is derived spent nuclear fuel corroded within the K Basins at 10-15?C. The STP process will place water-laden sludges from the K Basin in process vessels at {approx}150-180 C. Therefore, published studies with other irradiated (uranium oxide) fuel were examined. From these studies, the affinity of plutonium and americium for uranium in irradiated UO2 also was demonstrated at hydrothermal conditions (150 C anoxic liquid water) approaching those proposed for the STP process and even for hydrothermal conditions outside of the STP operating envelope (e.g., 150 C oxic and 100 C oxic and anoxic liquid water). In summary, by demonstrating that the chemical and physical behavior of 241Am in the sludge matrix is similar to that of the predominant species (uranium and for the plutonium from which it originates), a technical basis is provided for using the slow uptake transportability factor for 241Am that is currently used for plutonium and uranium oxides. The change from moderate to slow uptake for 241Am could reduce the overall analyzed dose consequences for the STP by more than 30%.« less
IMPROVEMENTS IN OR RELATING TO THE PRODUCTION OF SINTERED URANIUM DIOXIDE
DOE Office of Scientific and Technical Information (OSTI.GOV)
Russell, L.E.; Harrison, J.D.L.; Brett, N.H.
A method is described for producing a dense sintered body of uranium dioxide or a mixture thereof with plutonium dioxide. Compacted uranium dioxide or a compacted uranium dioxide-plutonium dioxide mixture is heated to at least 1300 deg C in an atmosphere of carbon dioxide or carbon dioxide mixed with carbon monoxide. (R.J.S.)
SAM lists this method for the qualitative determination of Americium-241, Radium-226, Plutonium-238, Plutonium-239 and isotopic uranium in drinking water samples using alpha spectrometry and radiostrontium using beta counting.
FUSED SALT PROCESS FOR RECOVERY OF VALUES FROM USED NUCLEAR REACTOR FUELS
Moore, R.H.
1960-08-01
A process is given for recovering plutonium from a neutron-irradiated uranium mass (oxide or alloy) by dissolving the mass in an about equimolar alkali metalaluminum double chloride, adding aluminum metal to the mixture obtained at a temperature of between 260 and 860 deg C, and separating a uranium-containing metal phase and a plutonium-chloride- and fission-product chloridecontaining salt phase. Dissolution can be expedited by passing carbon tetrachloride vapors through the double salt. Separation without reduction of plutonium from neutron- bombarded uranium and that of cerium from uranium are also discussed.
Further evaluations of the toxicity of irradiated advanced heavy water reactor fuels.
Edwards, Geoffrey W R; Priest, Nicholas D
2014-11-01
The neutron economy and online refueling capability of heavy water moderated reactors enable them to use many different fuel types, such as low enriched uranium, plutonium mixed with uranium, or plutonium and/or U mixed with thorium, in addition to their traditional natural uranium fuel. However, the toxicity and radiological protection methods for fuels other than natural uranium are not well established. A previous paper by the current authors compared the composition and toxicity of irradiated natural uranium to that of three potential advanced heavy water fuels not containing plutonium, and this work uses the same method to compare irradiated natural uranium to three other fuels that do contain plutonium in their initial composition. All three of the new fuels are assumed to incorporate plutonium isotopes characteristic of those that would be recovered from light water reactor fuel via reprocessing. The first fuel investigated is a homogeneous thorium-plutonium fuel designed for a once-through fuel cycle without reprocessing. The second fuel is a heterogeneous thorium-plutonium-U bundle, with graded enrichments of U in different parts of a single fuel assembly. This fuel is assumed to be part of a recycling scenario in which U from previously irradiated fuel is recovered. The third fuel is one in which plutonium and Am are mixed with natural uranium. Each of these fuels, because of the presence of plutonium in the initial composition, is determined to be considerably more radiotoxic than is standard natural uranium. Canadian nuclear safety regulations require that techniques be available for the measurement of 1 mSv of committed effective dose after exposure to irradiated fuel. For natural uranium fuel, the isotope Pu is a significant contributor to the committed effective dose after exposure, and thermal ionization mass spectrometry is sensitive enough that the amount of Pu excreted in urine is sufficient to estimate internal doses, from all isotopes, as low as 1 mSv. In addition, if this method is extended so that Pu is also measured, then the combined amount of Pu and Pu is sufficiently high in the thorium-plutonium fuel that a committed effective dose of 1 mSv would be measurable. However, the fraction of Pu and Pu in the other two fuels is sufficiently low that a 1 mSv dose would remain below the detection limit using this technique. Thus new methods, such as fecal measurements of Pu (or other alpha emitters), will be required to measure exposure to these new fuels.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Liezers, Martin; Lehn, Scott A; Olsen, Khris B
2009-10-01
Electrochemically modulated separations (EMS) are shown to be a rapid and selective means of extracting and concentrating Pu from complex solutions prior to isotopic analysis by inductively coupled plasma mass spectrometry (ICP-MS). This separation is performed in a flow injection mode, on-line with the ICP-MS. A three-electrode, flow-by electrochemical cell is used to accumulate Pu at an anodized glassy carbon electrode by redox conversion of Pu(III) to Pu (IV&VI). The entire process takes place in 2% v/v (0.46M) HNO 3. No redox chemicals or acid concentration changes are required. Plutonium accumulation and release is redox dependent and controlled by themore » applied cell potential. Thus large transient volumetric concentration enhancements can be achieved. Based on more negative U(IV) potentials relative to Pu(IV), separation of Pu from uranium is efficient, thereby eliminating uranium hydride interferences. EMS-ICP-MS isotope ratio measurement performance will be presented for femtogram to attogram level plutonium concentrations.« less
NASA Astrophysics Data System (ADS)
Marshalkin, V. Ye.; Povyshev, V. M.
2017-12-01
It is shown for a closed thorium-uranium-plutonium fuel cycle that, upon processing of one metric ton of irradiated fuel after each four-year campaign, the radioactive wastes contain 54 kg of fission products, 0.8 kg of thorium, 0.10 kg of uranium isotopes, 0.005 kg of plutonium isotopes, 0.002 kg of neptunium, and "trace" amounts of americium and curium isotopes. This qualitatively simplifies the handling of high-level wastes in nuclear power engineering.
SEPARATION OF PLUTONIUM VALUES FROM URANIUM AND FISSION PRODUCT VALUES
Maddock, A.G.; Booth, A.H.
1960-09-13
Separation of plutonium present in small amounts from neutron irradiated uranium by making use of the phenomenon of chemisorption is described. Plutonium in the tetravalent state is chemically absorbed on a fluoride in solid form. The steps for the separation comprise dissolving the irradiated uranium in nitric acid, oxidizing the plutonium in the resulting solution to the hexavalent state, adding to the solution a soluble calcium salt which by the common ion effect inhibits dissolution of the fluoride by the solution, passing the solution through a bed or column of subdivided calcium fluoride which has been sintered to about 8OO deg C to remove the chemisorbable fission products, reducing the plutonium in the solution thus obtained to the tetravalent state, and again passing the solution through a similar bed or column of calcium fluoride to selectively absorb the plutonium, which may then be recovered by treating the calcium fluoride with a solution of ammonium oxalate.
JOWOG 22/2 - Actinide Chemical Technology (July 9-13, 2012)
DOE Office of Scientific and Technical Information (OSTI.GOV)
Jackson, Jay M.; Lopez, Jacquelyn C.; Wayne, David M.
2012-07-05
The Plutonium Science and Manufacturing Directorate provides world-class, safe, secure, and reliable special nuclear material research, process development, technology demonstration, and manufacturing capabilities that support the nation's defense, energy, and environmental needs. We safely and efficiently process plutonium, uranium, and other actinide materials to meet national program requirements, while expanding the scientific and engineering basis of nuclear weapons-based manufacturing, and while producing the next generation of nuclear engineers and scientists. Actinide Process Chemistry (NCO-2) safely and efficiently processes plutonium and other actinide compounds to meet the nation's nuclear defense program needs. All of our processing activities are done in amore » world class and highly regulated nuclear facility. NCO-2's plutonium processing activities consist of direct oxide reduction, metal chlorination, americium extraction, and electrorefining. In addition, NCO-2 uses hydrochloric and nitric acid dissolutions for both plutonium processing and reduction of hazardous components in the waste streams. Finally, NCO-2 is a key team member in the processing of plutonium oxide from disassembled pits and the subsequent stabilization of plutonium oxide for safe and stable long-term storage.« less
SEPARATION OF PLUTONIUM FROM FISSION PRODUCTS BY A COLLOID REMOVAL PROCESS
Schubert, J.
1960-05-24
A method is given for separating plutonium from uranium fission products. An acidic aqueous solution containing plutonium and uranium fission products is subjected to a process for separating ionic values from colloidal matter suspended therein while the pH of the solution is maintained between 0 and 4. Certain of the fission products, and in particular, zirconium, niobium, lanthanum, and barium are in a colloidal state within this pH range, while plutonium remains in an ionic form, Dialysis, ultracontrifugation, and ultrafiltration are suitable methods of separating plutonium ions from the colloids.
Impact of Reprocessed Uranium Management on the Homogeneous Recycling of Transuranics in PWRs
DOE Office of Scientific and Technical Information (OSTI.GOV)
Youinou, Gilles J.
This article presents the results of a neutronics analysis related to the homogeneous recycling of transuranics (TRU) in PWRs with a MOX fuel using enriched uranium instead of depleted uranium. It also addresses an often, if not always, overlooked aspect related to the recycling of TRU in PWRs, namely the use of reprocessed uranium. From a neutronics point of view, it is possible to multi-recycle the entirety of the plutonium with or without neptunium and americium in a PWR fleet using MOX-EU fuel in between one third and two thirds of the fleet. Recycling neptunium and americium with plutonium significantlymore » decreases the decay heat of the waste stream between 100 to 1,000 years compared to those of an open fuel cycle or when only plutonium is recycled. The uranium present in MOX-EU used fuel still contains a significant amount of 235uranium and recycling it makes a major difference on the natural uranium needs. For example, a PWR fleet recycling its plutonium, neptunium and americium in MOXEU needs 28 percent more natural uranium than a reference UO 2 open cycle fleet generating the same energy if the reprocessed uranium is not recycled and 19 percent less if the reprocessed uranium is recycled back in the reactors, i.e. a 47 percent difference.« less
Impact of Reprocessed Uranium Management on the Homogeneous Recycling of Transuranics in PWRs
Youinou, Gilles J.
2017-05-04
This article presents the results of a neutronics analysis related to the homogeneous recycling of transuranics (TRU) in PWRs with a MOX fuel using enriched uranium instead of depleted uranium. It also addresses an often, if not always, overlooked aspect related to the recycling of TRU in PWRs, namely the use of reprocessed uranium. From a neutronics point of view, it is possible to multi-recycle the entirety of the plutonium with or without neptunium and americium in a PWR fleet using MOX-EU fuel in between one third and two thirds of the fleet. Recycling neptunium and americium with plutonium significantlymore » decreases the decay heat of the waste stream between 100 to 1,000 years compared to those of an open fuel cycle or when only plutonium is recycled. The uranium present in MOX-EU used fuel still contains a significant amount of 235uranium and recycling it makes a major difference on the natural uranium needs. For example, a PWR fleet recycling its plutonium, neptunium and americium in MOXEU needs 28 percent more natural uranium than a reference UO 2 open cycle fleet generating the same energy if the reprocessed uranium is not recycled and 19 percent less if the reprocessed uranium is recycled back in the reactors, i.e. a 47 percent difference.« less
NASA Astrophysics Data System (ADS)
Manara, D.; De Bruycker, F.; Boboridis, K.; Tougait, O.; Eloirdi, R.; Malki, M.
2012-07-01
In this work, an experimental study of the radiance of liquid and solid uranium and plutonium carbides at wavelengths 550 nm ⩽ λ ⩽ 920 nm is reported. A fast multi-channel spectro-pyrometer has been employed for the radiance measurements of samples heated up to and beyond their melting point by laser irradiation. The melting temperature of uranium monocarbide, soundly established at 2780 K, has been taken as a radiance reference. Based on it, a wavelength-dependence has been obtained for the high-temperature spectral emissivity of some uranium carbides (1 ⩽ C/U ⩽ 2). Similarly, the peritectic temperature of plutonium monocarbide (1900 K) has been used as a reference for plutonium monocarbide and sesquicarbide. The present spectral emissivities of solid uranium and plutonium carbides are close to 0.5 at 650 nm, in agreement with previous literature values. However, their high temperature behaviour, values in the liquid, and carbon-content and wavelength dependencies in the visible-near infrared range have been determined here for the first time. Liquid uranium carbide seems to interact with electromagnetic radiation in a more metallic way than does the solid, whereas a similar effect has not been observed for plutonium carbides. The current emissivity values have also been used to convert the measured radiance spectra into real temperature, and thus perform a thermal analysis of the laser heated samples. Some high-temperature phase boundaries in the systems U-C and Pu-C are shortly discussed on the basis of the current results.
Rapid Method for Sodium Hydroxide Fusion of Asphalt ...
Technical Brief--Addendum to Selected Analytical Methods (SAM) 2012 Rapid method developed for analysis of Americium-241 (241Am), plutonium-238 (238Pu), plutonium-239 (239Pu), radium-226 (226Ra), strontium-90 (90Sr), uranium-234 (234U), uranium-235 (235U) and uranium-238 (238U) in asphalt roofing material samples
FISSION PRODUCT REMOVAL FROM ORGANIC SOLUTIONS
Moore, R.H.
1960-05-10
The decontamination of organic solvents from fission products and in particular the treatment of solvents that were used for the extraction of uranium and/or plutonium from aqueous acid solutions of neutron-irradiated uranium are treated. The process broadly comprises heating manganese carbonate in air to a temperature of between 300 and 500 deg C whereby manganese dioxide is formed; mixing the manganese dioxide with the fission product-containing organic solvent to be treated whereby the fission products are precipitated on the manganese dioxide; and separating the fission product-containing manganese dioxide from the solvent.
SULFIDE METHOD PLUTONIUM SEPARATION
Duffield, R.B.
1958-08-12
A process is described for the recovery of plutonium from neutron irradiated uranium solutions. Such a solution is first treated with a soluble sullide, causing precipitation of the plutoniunn and uraniunn values present, along with those impurities which form insoluble sulfides. The precipitate is then treated with a solution of carbonate ions, which will dissolve the uranium and plutonium present while the fission product sulfides remain unaffected. After separation from the residue, this solution may then be treated by any of the usual methods, such as formation of a lanthanum fluoride precipitate, to effect separation of plutoniunn from uranium.
METHOD FOR PREPARING URANIUM MONOCARBIDE-PLUTONIUM MONOCARBIDE SOLID SOLUTION
Ogard, A.E.; Leary, J.A.; Maraman, W.J.
1963-03-19
A method is given for preparing solid solutions of uranium monocarbide- plutonium monocarbide. In this method, the powder form of uranium dioxide, plutonium dioxide, and graphite are mixed in a ratio determined by the equation: xUO/sub 2/ + yPuO/sub 2/ + (2+z)C yields UxPu/sub y/C/sub z/ +2CO, where x + y equ al 1.0 and z is greater than 0.9 but less than 1.0. The resulting mixture is compacted and heated in a vacuum at a temperature of 1850 deg C. (AEC)
Real-time monitoring of plutonium content in uranium-plutonium alloys
Li, Shelly Xiaowei; Westphal, Brian Robert; Herrmann, Steven Douglas
2015-09-01
A method and device for the real-time, in-situ monitoring of Plutonium content in U--Pu Alloys comprising providing a crucible. The crucible has an interior non-reactive to a metallic U--Pu alloy within said interior of said crucible. The U--Pu alloy comprises metallic uranium and plutonium. The U--Pu alloy is heated to a liquid in an inert or reducing atmosphere. The heated U--Pu alloy is then cooled to a solid in an inert or reducing atmosphere. As the U--Pu alloy is cooled, the temperature of the U--Pu alloy is monitored. A solidification temperature signature is determined from the monitored temperature of the U--Pu alloy during the step of cooling. The amount of Uranium and the amount of Plutonium in the U--Pu alloy is then determined from the determined solidification temperature signature.
PLUTONIUM RECOVERY FROM NEUTRON-BOMBARDED URANIUM FUEL
Moore, R.H.
1964-03-24
A process of recovering plutonium from fuel by dissolution in molten KAlCl/sub 4/ double salt is described. Molten lithium chloride plus stannous chloride is added to reduce plutonium tetrachloride to the trichloride, which is dissolved in a lithium chloride phase while the uranium, as the tetrachloride, is dissolved in a double-salt phase. Separation of the two phases is discussed. (AEC)
SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS BY ADSORPTION
Seaborg, G.T.; Willard, J.E.
1958-01-01
A method is presented for the separation of plutonium from solutions containing that element in a valence state not higher than 41 together with uranium ions and fission products. This separation is accomplished by contacting the solutions with diatomaceous earth which preferentially adsorbs the plutonium present. Also mentioned as effective for this adsorbtive separation are silica gel, filler's earth and alumina.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Marsh, S.F.; Spall, W.D.; Abernathey, R.M.
1976-11-01
Relationships are provided to compute the decreasing plutonium content and changing isotopic distribution of plutonium materials for the radioactive decay of /sup 238/Pu, /sup 239/Pu, /sup 240/Pu and /sup 242/Pu to long-lived uranium daughters and of /sup 241/Pu to /sup 241/Am. This computation is important to the use of plutonium reference materials to calibrate destructive and nondestructive methods for assay and isotopic measurements, as well as to accountability inventory calculations.
Simulation of uranium and plutonium oxides compounds obtained in plasma
NASA Astrophysics Data System (ADS)
Novoselov, Ivan Yu.; Karengin, Alexander G.; Babaev, Renat G.
2018-03-01
The aim of this paper is to carry out thermodynamic simulation of mixed plutonium and uranium oxides compounds obtained after plasma treatment of plutonium and uranium nitrates and to determine optimal water-salt-organic mixture composition as well as conditions for their plasma treatment (temperature, air mass fraction). Authors conclude that it needs to complete the treatment of nitric solutions in form of water-salt-organic mixtures to guarantee energy saving obtainment of oxide compounds for mixed-oxide fuel and explain the choice of chemical composition of water-salt-organic mixture. It has been confirmed that temperature of 1200 °C is optimal to practice the process. Authors have demonstrated that condensed products after plasma treatment of water-salt-organic mixture contains targeted products (uranium and plutonium oxides) and gaseous products are environmental friendly. In conclusion basic operational modes for practicing the process are showed.
Code of Federal Regulations, 2014 CFR
2014-01-01
... dissolution, solvent extraction, and process liquor storage. There may also be equipment for thermal denitration of uranium nitrate, conversion of plutonium nitrate to oxide metal, and treatment of fission product waste liquor to a form suitable for long term storage or disposal. However, the specific type and...
Code of Federal Regulations, 2013 CFR
2013-01-01
... dissolution, solvent extraction, and process liquor storage. There may also be equipment for thermal denitration of uranium nitrate, conversion of plutonium nitrate to oxide metal, and treatment of fission product waste liquor to a form suitable for long term storage or disposal. However, the specific type and...
Code of Federal Regulations, 2012 CFR
2012-01-01
... dissolution, solvent extraction, and process liquor storage. There may also be equipment for thermal denitration of uranium nitrate, conversion of plutonium nitrate to oxide metal, and treatment of fission product waste liquor to a form suitable for long term storage or disposal. However, the specific type and...
Xu, Yihong; Qiao, Jixin; Hou, Xiaolin; Pan, Shaoming; Roos, Per
2014-02-01
This paper reports an analytical method for the determination of plutonium isotopes ((238)Pu, (239)Pu, (240)Pu, (241)Pu) in environmental samples using anion exchange chromatography in combination with extraction chromatography for chemical separation of Pu. Both radiometric methods (liquid scintillation counting and alpha spectrometry) and inductively coupled plasma mass spectrometry (ICP-MS) were applied for the measurement of plutonium isotopes. The decontamination factors for uranium were significantly improved up to 7.5 × 10(5) for 20 g soil compared to the level reported in the literature, this is critical for the measurement of plutonium isotopes using mass spectrometric technique. Although the chemical yield of Pu in the entire procedure is about 55%, the analytical results of IAEA soil 6 and IAEA-367 in this work are in a good agreement with the values reported in the literature or reference values, revealing that the developed method for plutonium determination in environmental samples is reliable. The measurement results of (239+240)Pu by alpha spectrometry agreed very well with the sum of (239)Pu and (240)Pu measured by ICP-MS. ICP-MS can not only measure (239)Pu and (240)Pu separately but also (241)Pu. However, it is impossible to measure (238)Pu using ICP-MS in environmental samples even a decontamination factor as high as 10(6) for uranium was obtained by chemical separation. © 2013 Elsevier B.V. All rights reserved.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Harold F. McFarlane; Terry Todd
2013-11-01
Reprocessing is essential to closing nuclear fuel cycle. Natural uranium contains only 0.7 percent 235U, the fissile (see glossary for technical terms) isotope that produces most of the fission energy in a nuclear power plant. Prior to being used in commercial nuclear fuel, uranium is typically enriched to 3–5% in 235U. If the enrichment process discards depleted uranium at 0.2 percent 235U, it takes more than seven tonnes of uranium feed to produce one tonne of 4%-enriched uranium. Nuclear fuel discharged at the end of its economic lifetime contains less one percent 235U, but still more than the natural ore.more » Less than one percent of the uranium that enters the fuel cycle is actually used in a single pass through the reactor. The other naturally occurring isotope, 238U, directly contributes in a minor way to power generation. However, its main role is to transmute into plutoniumby neutron capture and subsequent radioactive decay of unstable uraniumand neptuniumisotopes. 239Pu and 241Pu are fissile isotopes that produce more than 40% of the fission energy in commercially deployed reactors. It is recovery of the plutonium (and to a lesser extent the uranium) for use in recycled nuclear fuel that has been the primary focus of commercial reprocessing. Uraniumtargets irradiated in special purpose reactors are also reprocessed to obtain the fission product 99Mo, the parent isotope of technetium, which is widely used inmedical procedures. Among the fission products, recovery of such expensive metals as platinum and rhodium is technically achievable, but not economically viable in current market and regulatory conditions. During the past 60 years, many different techniques for reprocessing used nuclear fuel have been proposed and tested in the laboratory. However, commercial reprocessing has been implemented along a single line of aqueous solvent extraction technology called plutonium uranium reduction extraction process (PUREX). Similarly, hundreds of types of reactor fuels have been irradiated for different purposes, but the vast majority of commercial fuel is uranium oxide clad in zirconium alloy tubing. As a result, commercial reprocessing plants have relatively narrow technical requirements for used nuclear that is accepted for processing.« less
Some Thermodynamic Features of Uranium-Plutonium Nitride Fuel in the Course of Burnup
NASA Astrophysics Data System (ADS)
Rusinkevich, A. A.; Ivanov, A. S.; Belov, G. V.; Skupov, M. V.
2017-12-01
Calculation studies on the effect of carbon and oxygen impurities on the chemical and phase compositions of nitride uranium-plutonium fuel in the course of burnup are performed using the IVTANTHERMO code. It is shown that the number of moles of UN decreases with increasing burnup level, whereas UN1.466, UN1.54, and UN1.73 exhibit a considerable increase. The presence of oxygen and carbon impurities causes an increase in the content of the UN1.466, UN1.54 and UN1.73 phases in the initial fuel by several orders of magnitude, in particular, at a relatively low temperature. At the same time, the presence of impurities abruptly reduces the content of free uranium in unburned fuel. Plutonium in the considered system is contained in form of Pu, PuC, PuC2, Pu2C3, and PuN. Plutonium carbides, as well as uranium carbides, are formed in small amounts. Most of the plutonium remains in the form of nitride PuN, whereas unbound Pu is present only in the areas with a low burnup level and high temperatures.
TERNARY ALLOY-CONTAINING PLUTONIUM
Waber, J.T.
1960-02-23
Ternary alloys of uranium and plutonium containing as the third element either molybdenum or zirconium are reported. Such alloys are particularly useful as reactor fuels in fast breeder reactors. The alloy contains from 2 to 25 at.% of molybdenum or zirconium, the balance being a combination of uranium and plutonium in the ratio of from 1 to 9 atoms of uranlum for each atom of plutonium. These alloys are prepared by melting the constituent elements, treating them at an elevated temperature for homogenization, and cooling them to room temperature, the rate of cooling varying with the oomposition and the desired phase structure. The preferred embodiment contains 12 to 25 at.% of molybdenum and is treated by quenching to obtain a body centered cubic crystal structure. The most important advantage of these alloys over prior binary alloys of both plutonium and uranium is the lack of cracking during casting and their ready machinability.
Surugaya, Naoki; Hiyama, Toshiaki; Verbruggen, André; Wellum, Roger
2008-02-01
A stable solid spike for the measurement of uranium and plutonium content in nitric acid solutions of spent nuclear fuel by isotope dilution mass spectrometry has been prepared at the European Commission Institute for Reference Materials and Measurements in Belgium. The spike contains about 50 mg of uranium with a 19.838% (235)U enrichment and 2 mg of plutonium with a 97.766% (239)Pu abundance in each individual ampoule. The dried materials were covered with a thin film of cellulose acetate butyrate as a protective organic stabilizer to resist shocks encountered during transportation and to eliminate flaking-off during long-term storage. It was found that the cellulose acetate butyrate has good characteristics, maintaining a thin film for a long time, but readily dissolving on heating with nitric acid solution. The solid spike containing cellulose acetate butyrate was certified as a reference material with certified quantities: (235)U and (239)Pu amounts and uranium and plutonium amount ratios, and was validated by analyzing spent fuel dissolver solutions of the Tokai reprocessing plant in Japan. This paper describes the preparation, certification and validation of the solid spike coated with a cellulose derivative.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Swanson, Gerald C.
1975-10-01
The oxygen-to-metal atom ratio, or O/M, of solid solution uranium- plutonium oxide reactor fuel is a measure of the concentration of crystal defects in the oxide which affect many fuel properties, particularly, fuel oxygen potential. Fabrication of a high-temperature oxygen electrode, employing an electro-active tip of oxygen-deficient solid-state electrolyte, intended to confirm gaseous oxygen potentials is described. Uranium oxide and plutonium oxide O/M reference materials were prepared by in situ oxidation of high purity metals in the thermobalance. A solid solution uranium-plutonium oxide O/M reference material was prepared by alloying the uranium and plutonium metals in a yttrium oxide cruciblemore » at 1200°C and oxidizing with moist He at 250°C. The individual and solid solution oxides were isothermally equilibrated with controlled oxygen potentials between 800 and 1300°C and the equilibrated O/ M ratios calculated with corrections for impurities and buoyancy effects. Use of a reference oxygen potential of -100 kcal/mol to produce an O/M of 2.000 is confirmed by these results. However, because of the lengthy equilibration times required for all oxides, use of the O/M reference materials rather than a reference oxygen potential is recommended for O/M analysis methods calibrations.« less
Improving the Estimates of Waste from the Recycling of Used Nuclear Fuel - 13410
DOE Office of Scientific and Technical Information (OSTI.GOV)
Phillips, Chris; Willis, William; Carter, Robert
2013-07-01
Estimates are presented of wastes arising from the reprocessing of 50 GWD/tonne, 5 year and 50 year cooled used nuclear fuel (UNF) from Light Water Reactors (LWRs), using the 'NUEX' solvent extraction process. NUEX is a fourth generation aqueous based reprocessing system, comprising shearing and dissolution in nitric acid of the UNF, separation of uranium and mixed uranium-plutonium using solvent extraction in a development of the PUREX process using tri-n-butyl phosphate in a kerosene diluent, purification of the plutonium and uranium-plutonium products, and conversion of them to uranium trioxide and mixed uranium-plutonium dioxides respectively. These products are suitable for usemore » as new LWR uranium oxide and mixed oxide fuel, respectively. Each unit process is described and the wastes that it produces are identified and quantified. Quantification of the process wastes was achieved by use of a detailed process model developed using the Aspen Custom Modeler suite of software and based on both first principles equilibrium and rate data, plus practical experience and data from the industrial scale Thermal Oxide Reprocessing Plant (THORP) at the Sellafield nuclear site in the United Kingdom. By feeding this model with the known concentrations of all species in the incoming UNF, the species and their concentrations in all product and waste streams were produced as the output. By using these data, along with a defined set of assumptions, including regulatory requirements, it was possible to calculate the waste forms, their radioactivities, volumes and quantities. Quantification of secondary wastes, such as plant maintenance, housekeeping and clean-up wastes, was achieved by reviewing actual operating experience from THORP during its hot operation from 1994 to the present time. This work was carried out under a contract from the United States Department of Energy (DOE) and, so as to enable DOE to make valid comparisons with other similar work, a number of assumptions were agreed. These include an assumed reprocessing capacity of 800 tonnes per year, the requirement to remove as waste forms the volatile fission products carbon-14, iodine-129, krypton-85, tritium and ruthenium-106, the restriction of discharge of any water from the facility unless it meets US Environmental Protection Agency drinking water standards, no intentional blending of wastes to lower their classification, and the requirement for the recovered uranium to be sufficiently free from fission products and neutron-absorbing species to allow it to be re-enriched and recycled as nuclear fuel. The results from this work showed that over 99.9% of the radioactivity in the UNF can be concentrated via reprocessing into a fission-product-containing vitrified product, bottles of compressed krypton storage and a cement grout containing the tritium, that together have a volume of only about one eighth the volume of the original UNF. The other waste forms have larger volumes than the original UNF but contain only the remaining 0.1% of the radioactivity. (authors)« less
PROCESS OF MAKING A NEUTRONIC REACTOR FUEL ELEMENT COMPOSITION
Alter, H.W.; Davidson, J.K.; Miller, R.S.; Mewherter, J.L.
1959-01-13
A process is presented for making a ceramic-like material suitable for use as a nuclear fuel. The material consists of a solid solution of plutonium dioxide in uranium dioxide and is produced from a uranyl nitrate -plutonium nitrate solution containing uraniunm and plutonium in the desired ratio. The uranium and plutonium are first precipitated from the solution by addition of NH/ sub 4/OH and the dried precipitate is then calcined at 600 C in a hydrogen atmosphere to yield the desired solid solution of PuO/sub 2/ in UO/sub 2/.
METHOD OF SEPARATING URANIUM, PLUTONIUM AND FISSION PRODUCTS BY BROMINATION AND DISTILLATION
Jaffey, A.H.; Seaborg, G.T.
1958-12-23
The method for separation of plutonium from uranium and radioactive fission products obtained by neutron irradiation of uranlum consists of reacting the lrradiated material with either bromine, hydrogen bromide, alumlnum bromide, or sulfur and bromine at an elevated temperature to form the bromides of all the elements, then recovering substantlally pure plutonium bromide by dlstillatlon in combinatlon with selective condensatlon at prescribed temperature and pressure.
RECOVERY OF Pu VALUES BY FLUORINATION AND FRACTIONATION
Brown, H.S.; Webster, D.S.
1959-01-20
A method is presented for the concentration and recovery of plutonium by fluorination and fractionation. A metallic mass containing uranium and plutonium is heated to 250 C and contacted with a stream of elemental fluorine. After fluorination of the metallic mass, the rcaction products are withdrawn and subjected to a distillation treatment to separate the fluorination products of uranium and to obtain a residue containing the fluorination products of plutonium.
The measurement of U(VI) and Np(IV) mass transfer in a single stage centrifugal contactor
NASA Astrophysics Data System (ADS)
May, I.; Birkett, E. J.; Denniss, I. S.; Gaubert, E. T.; Jobson, M.
2000-07-01
BNFL currently operates two reprocessing plants for the conversion of spent nuclear fuel into uranium and plutonium products for fabrication into uranium oxide and mixed uranium and plutonium oxide (MOX) fuels. To safeguard the future commercial viability of this process, BNFL is developing novel single cycle flowsheets that can be operated in conjunction with intensified centrifugal contactors.
Xing, Shan; Zhang, Weichao; Qiao, Jixin; Hou, Xiaolin
2018-09-01
In order to measure trace plutonium and its isotopes ratio ( 240 Pu/ 239 Pu) in environmental samples with a high uranium, an analytical method was developed using radiochemical separation for separation of plutonium from matrix and interfering elements including most of uranium and ICP-MS for measurement of plutonium isotopes. A novel measurement method was established for extensively removing the isobaric interference from uranium ( 238 U 1 H and 238 UH 2 + ) and tailing of 238 U, but significantly improving the measurement sensitivity of plutonium isotopes by employing NH 3 /He as collision/reaction cell gases and MS/MS system in the triple quadrupole ICP-MS instrument. The results show that removal efficiency of uranium interference was improved by more than 15 times, and the sensitivity of plutonium isotopes was increased by a factor of more than 3 compared to the conventional ICP-MS. The mechanism on the effective suppress of 238 U interference for 239 Pu measurement using NH 3 -He reaction gases was explored to be the formation of UNH + and UNH 2 + in the reactions of UH + and U + with NH 3 , while no reaction between NH 3 and Pu + . The detection limits of this method were estimated to be 0.55 fg mL -1 for 239 Pu, 0.09 fg mL -1 for 240 Pu. The analytical precision and accuracy of the method for Pu isotopes concentration and 240 Pu/ 239 Pu atomic ratio were evaluated by analysis of sediment reference materials (IAEA-385 and IAEA-412) with different levels of plutonium and uranium. The developed method were successfully applied to determine 239 Pu and 240 Pu concentrations and 240 Pu/ 239 Pu atomic ratios in soil samples collected in coastal areas of eastern China. Copyright © 2018 Elsevier B.V. All rights reserved.
On the valence fluctuation in the early actinide metals
Soderlind, P.; Landa, A.; Tobin, J. G.; ...
2015-12-15
In this study, recent X-ray measurements suggest a degree of valence fluctuation in plutonium and uranium intermetallics. We are applying a novel scheme, in conjunction with density functional theory, to predict 5f configuration fractions of states with valence fluctuations for the early actinide metals. For this purpose we perform constrained integer f-occupation calculations for the α phases of uranium, neptunium, and plutonium metals. For plutonium we also investigate the δ phase. The model predicts uranium and neptunium to be dominated by the f 3 and f 4 configurations, respectively, with only minor contributions from other configurations. For plutonium (both αmore » and δ phase) the scenario is dramatically different. Here, the calculations predict a relatively even distribution between three valence configurations. The δ phase has a greater configuration fraction of f 6 compared to that of the α phase. The theory is consistent with the interpretations of modern X-ray experiments and we present resonant X-ray emission spectroscopy results for α-uranium.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Farmer, Orville T.; Olsen, Khris B.; Thomas, May-Lin P.
2008-05-01
A method for the separation and determination of total and isotopic uranium and plutonium by ICP-MS was developed for IAEA samples on cellulose-based media. Preparation of the IAEA samples involved a series of redox chemistries and separations using TRU® resin (Eichrom). The sample introduction system, an APEX nebulizer (Elemental Scientific, Inc), provided enhanced nebulization for a several-fold increase in sensitivity and reduction in background. Application of mass bias (ALPHA) correction factors greatly improved the precision of the data. By combining the enhancements of chemical separation, instrumentation and data processing, detection levels for uranium and plutonium approached high attogram levels.
This enclosure from a DOE letter to EPA regarding a waste container disposed at the WIPP from the Advanced Mixed Waste Treatment Project includes Table 5-2, Isotopic Compositions of Rocky Flats Plutonium and Uranium.
PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINATING ELEMENTS
Sutton, J.B.
1958-02-18
This patent relates to an improved method for the decontamination of plutonium. The process consists broadly in an improvement in a method for recovering plutonium from radioactive uranium fission products in aqueous solutions by decontamination steps including byproduct carrier precipitation comprising the step of introducing a preformed aqueous slurry of a hydroxide of a metal of group IV B into any aqueous acidic solution which contains the plutonium in the hexavalent state, radioactive uranium fission products contaminant and a by-product carrier precipitate and separating the metal hydroxide and by-product precipitate from the solution. The process of this invention is especially useful in the separation of plutonium from radioactive zirconium and columbium fission products.
A high converter concept for fuel management with blanket fuel assemblies in boiling water reactors
DOE Office of Scientific and Technical Information (OSTI.GOV)
Martinez-Frances, N.; Timm, W.; Rossbach, D.
2012-07-01
Studies on the natural Uranium saving and waste reduction potential of a multiple-plant BWR system were performed. The BWR High Converter system should enable a multiple recycling of MOX fuel in current BWR plants by introducing blanket fuel assemblies and burning Uranium and MOX fuel separately. The feasibility of Uranium cores with blankets and full-MOX cores with Plutonium qualities as low as 40% were studied. The power concentration due to blanket insertion is manageable with modern fuel and acceptable values for the thermal limits and reactivity coefficients were obtained. While challenges remain, full-MOX cores also complied with the main designmore » criteria. The combination of Uranium and Plutonium burners in appropriate proportions could enable obtaining as much as 40% more energy out of Uranium ore. Moreover, a proper adjustment of blanket average stay and Plutonium qualities could lead to a system with nearly no Plutonium left for final disposal. The achievement of such goals with current light water technology makes the BWR HC concept an attractive option to improve the fuel cycle until Gen-IV designs are mature. (authors)« less
NASA Astrophysics Data System (ADS)
Marshalkin, V. E.; Povyshev, V. M.
2015-12-01
A method for joint utilization of non-weapons-grade plutonium and highly enriched uranium in the thorium-uranium—plutonium oxide fuel of a water-moderated reactor with a varying water composition (D2O, H2O) is proposed. The method is characterized by efficient breeding of the 233U isotope and safe reactor operation and is comparatively simple to implement.
Johnson, B.M.
1963-08-20
A spray calcination reactor for calcining reprocessin- g waste solutions is described. Coaxial within the outer shell of the reactor is a shorter inner shell having heated walls and with open regions above and below. When the solution is sprayed into the irner shell droplets are entrained by a current of gas that moves downwardly within the inner shell and upwardly between it and the outer shell, and while thus being circulated the droplets are calcined to solids, whlch drop to the bottom without being deposited on the walls. (AEC) H03 H0233412 The average molecular weights of four diallyl phthalate polymer samples extruded from the experimental rheometer were redetermined using the vapor phase osmometer. An amine curing agent is required for obtaining suitable silver- filled epoxy-bonded conductive adhesives. When the curing agent was modified with a 47% polyurethane resin, its effectiveness was hampered. Neither silver nor nickel filler impart a high electrical conductivity to Adiprenebased adhesives. Silver filler was found to perform well in Dow-Corning A-4000 adhesive. Two cascaded hot-wire columns are being used to remove heavy gaseous impurities from methane. This purified gas is being enriched in the concentric tube unit to approximately 20% carbon-13. Studies to count low-level krypton-85 in xenon are continuing. The parameters of the counting technique are being determined. The bismuth isotopes produced in bismuth irradiated for polonium production are being determined. Preliminary data indicate the presence of bismuth207 and bismuth-210m. The light bismuth isotopes are probably produced by (n,xn) reactions bismuth-209. The separation of uranium-234 from plutonium-238 solutions was demonstrated. The bulk of the plutonium is removed by anion exchange, and the remainder is extracted from the uranium by solvent extraction techniques. About 99% of the plutonium can be removed in each thenoyltrifluoroacetone extraction. The viscosity, liquid density, and selfdiffusion coefficient for lanthanum, cerium, and praseodymium were determined. The investigation of phase relationships in the plutonium-cerium-copper ternary system was continued on samples containing a high concentration of copper. These analyses indicate that complete solid solution exists between the binary compounds CeCu/sub 2/ and PuCu/sub 2/, thus forming a quasi-binary system. The study of high temperature ceramic fuel materials has continued with the homogenization and microspheroidization of binary mixtures of plutonium dioxide and zirconium dioxide. Sintering a die-pressed pellet of the mixed powders for one hour at 1450 deg C was not sufficient to completely react the constituents. Complete homogenization was obtained when the pellet was melted in the plasma flame. In addition to the plutonium dioxide-zirconium dioxide microspheres, pure beryllium oxide microspheres were produced in the plasma torch. The electronic distribution functions for the 10% by weight PuO/sub 2/ dissolved in a silicate glass were determined. The plutonium-oxygen interaction at about 2.2A is less than the plutonium-oxygen distance for the 5% PuO/sub 2/. The decrease in the interionic distance is indicative of a stronger plutonium-oxygen association for the more concentrated composition. Potassium plutonium sulfate is being evaluated as a reagent to quantitatively separate plutonium from aqueous solutions. The compound containing two waters of hydration was prepared for thermogravimetric studies using analytically pure plutonium-239. Because of the stability of this compound, it is being evaluated as a calorimetric standard for plutonium-238. (auth)
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
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gao, Jun; Manard, Benjamin Thomas; Castro, Alonso
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
PLUTONIUM-CUPFERRON COMPLEX AND METHOD OF REMOVING PLUTONIUM FROM SOLUTION
Potratz, H.A.
1959-01-13
A method is presented for separating plutonium from fission products present in solutions of neutronirradiated uranium. The process consists in treating such acidic solutions with cupferron so that the cupferron reacts with the plutonium present to form an insoluble complex. This plutonium cupferride precipitates and may then be separated from the solution.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Marshalkin, V. E., E-mail: marshalkin@vniief.ru; Povyshev, V. M.
A method for joint utilization of non-weapons-grade plutonium and highly enriched uranium in the thorium–uranium—plutonium oxide fuel of a water-moderated reactor with a varying water composition (D{sub 2}O, H{sub 2}O) is proposed. The method is characterized by efficient breeding of the {sup 233}U isotope and safe reactor operation and is comparatively simple to implement.
A Graphical Examination of Uranium and Plutonium Fissility
ERIC Educational Resources Information Center
Reed, B. Cameron
2008-01-01
The issue of why only particular isotopes of uranium and plutonium are suitable for use in nuclear weapons is analyzed with the aid of graphs and semiquantitative discussions of parameters such as excitation energies, fission barriers, reaction cross-sections, and the role of processes such as [alpha]-decay and spontaneous fission. The goal is to…
O-Pu-U (Oxygen-Plutonium-Uranium)
NASA Astrophysics Data System (ADS)
Materials Science International Team MSIT
This document is part of Subvolume C4 'Non-Ferrous Metal Systems. Part 4: Selected Nuclear Materials and Engineering Systems' of Volume 11 'Ternary Alloy Systems - Phase Diagrams, Crystallographic and Thermodynamic Data critically evaluated by MSIT®' of Landolt-Börnstein - Group IV 'Physical Chemistry'. It provides data of the ternary system Oxygen-Plutonium-Uranium.
PEROXIDE PROCESS FOR SEPARATION OF RADIOACTIVE MATERIALS
Seaborg, G.T.; Perlman, I.
1958-09-16
reduced state, from hexavalent uranium. It consists in treating an aqueous solution containing such uranium and plutonium ions with sulfate ions in order to form a soluble uranium sulfate complex and then treating the solution with a soluble thorium compound and a soluble peroxide compound in order to ferm a thorium peroxide carrier precipitate which carries down with it the plutonium peroxide present. During this treatment the pH of the solution must be maintained between 2 and 3.
NASA Astrophysics Data System (ADS)
Sturm, Monika; Richter, Stephan; Aregbe, Yetunde; Wellum, Roger; Mayer, Klaus; Prohaska, Thomas
2014-05-01
Although the age determination of plutonium is and has been a pillar of nuclear forensic investigations for many years, additional research in the field of plutonium age dating is still needed and leads to new insights as the present work shows: Plutonium is commonly dated with the help of the 241Pu/241Am chronometer using gamma spectrometry; in fewer cases the 240Pu/236U chronometer has been used. The age dating results of the 239Pu/235U chronometer and the 238Pu/234U chronometer are scarcely applied in addition to the 240Pu/236U chronometer, although their results can be obtained simultaneously from the same mass spectrometric experiments as the age dating result of latter. The reliability of the result can be tested when the results of different chronometers are compared. The 242Pu/238U chronometer is normally not evaluated at all due to its sensitivity to contamination with natural uranium. This apparent 'weakness' that renders the age dating results of the 242Pu/238U chronometer almost useless for nuclear forensic investigations, however turns out to be an advantage looked at from another perspective: the 242Pu/238U chronometer can be utilized as an indicator for uranium contamination of plutonium samples and even help to identify the nature of this contamination. To illustrate this the age dating results of all four Pu/U clocks mentioned above are discussed for one plutonium sample (NBS 946) that shows no signs of uranium contamination and for three additional plutonium samples. In case the 242Pu/238U chronometer results in an older 'age' than the other Pu/U chronometers, contamination with either a small amount of enriched or with natural or depleted uranium is for example possible. If the age dating result of the 239Pu/235U chronometer is also influenced the nature of the contamination can be identified; enriched uranium is in this latter case a likely cause for the missmatch of the age dating results of the Pu/U chronometers.
Control of a laser inertial confinement fusion-fission power plant
Moses, Edward I.; Latkowski, Jeffery F.; Kramer, Kevin J.
2015-10-27
A laser inertial-confinement fusion-fission energy power plant is described. The fusion-fission hybrid system uses inertial confinement fusion to produce neutrons from a fusion reaction of deuterium and tritium. The fusion neutrons drive a sub-critical blanket of fissile or fertile fuel. A coolant circulated through the fuel extracts heat from the fuel that is used to generate electricity. The inertial confinement fusion reaction can be implemented using central hot spot or fast ignition fusion, and direct or indirect drive. The fusion neutrons result in ultra-deep burn-up of the fuel in the fission blanket, thus enabling the burning of nuclear waste. Fuels include depleted uranium, natural uranium, enriched uranium, spent nuclear fuel, thorium, and weapons grade plutonium. LIFE engines can meet worldwide electricity needs in a safe and sustainable manner, while drastically shrinking the highly undesirable stockpiles of depleted uranium, spent nuclear fuel and excess weapons materials.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hill, J.S., Westinghouse Hanford
1996-05-10
This report shows the methods used to test the stack gas outlet concentration and emission rate of Volatile Organic Compounds as Total Non-Methane Hydrocarbons in parts per million by volume,grams per dry standard cubic meter, and grams per minute from the PUREX ETF stream number G6 on the Hanford Site. Test results are shown in Appendix B.1.
On the equilibrium isotopic composition of the thorium-uranium-plutonium fuel cycle
NASA Astrophysics Data System (ADS)
Marshalkin, V. Ye.; Povyshev, V. M.
2016-12-01
The equilibrium isotopic compositions and the times to equilibrium in the process of thorium-uranium-plutonium oxide fuel recycling in VVER-type reactors using heavy water mixed with light water are estimated. It is demonstrated thEhfat such reactors have a capacity to operate with self-reproduction of active isotopes in the equilibrium mode.
Fluorination process using catalyst
Hochel, Robert C.; Saturday, Kathy A.
1985-01-01
A process for converting an actinide compound selected from the group consisting of uranium oxides, plutonium oxides, uranium tetrafluorides, plutonium tetrafluorides and mixtures of said oxides and tetrafluorides, to the corresponding volatile actinide hexafluoride by fluorination with a stoichiometric excess of fluorine gas. The improvement involves conducting the fluorination of the plutonium compounds in the presence of a fluoride catalyst selected from the group consisting of CoF.sub.3, AgF.sub.2 and NiF.sub.2, whereby the fluorination is significantly enhanced. The improvement also involves conducting the fluorination of one of the uranium compounds in the presence of a fluoride catalyst selected from the group consisting of CoF.sub.3 and AgF.sub.2, whereby the fluorination is significantly enhanced.
Fluorination process using catalysts
Hochel, R.C.; Saturday, K.A.
1983-08-25
A process is given for converting an actinide compound selected from the group consisting of uranium oxides, plutonium oxides, uranium tetrafluorides, plutonium tetrafluorides and mixtures of said oxides and tetrafluorides, to the corresponding volatile actinide hexafluoride by fluorination with a stoichiometric excess of fluorine gas. The improvement involves conducting the fluorination of the plutonium compounds in the presence of a fluoride catalyst selected from the group consisting of CoF/sub 3/, AgF/sub 2/ and NiF/sub 2/, whereby the fluorination is significantly enhanced. The improvement also involves conducting the fluorination of one of the uranium compounds in the presence of a fluoride catalyst selected from the group consisting of CoF/sub 3/ and AgF/sub 2/, whereby the fluorination is significantly enhanced.
Hyman, H.H.; Dreher, J.L.
1959-07-01
The recovery of uranium from the acidic aqueous metal waste solutions resulting from the bismuth phosphate carrier precipitation of plutonium from solutions of neutron irradiated uranium is described. The waste solutions consist of phosphoric acid, sulfuric acid, and uranium as a uranyl salt, together with salts of the fission products normally associated with neutron irradiated uranium. Generally, the process of the invention involves the partial neutralization of the waste solution with sodium hydroxide, followed by conversion of the solution to a pH 11 by mixing therewith sufficient sodium carbonate. The resultant carbonate-complexed waste is contacted with a titanated silica gel and the adsorbent separated from the aqueous medium. The aqueous solution is then mixed with sufficient acetic acid to bring the pH of the aqueous medium to between 4 and 5, whereby sodium uranyl acetate is precipitated. The precipitate is dissolved in nitric acid and the resulting solution preferably provided with salting out agents. Uranyl nitrate is recovered from the solution by extraction with an ether such as diethyl ether.
METHOD OF OPERATING NUCLEAR REACTORS
Untermyer, S.
1958-10-14
A method is presented for obtaining enhanced utilization of natural uranium in heavy water moderated nuclear reactors by charging the reactor with an equal number of fuel elements formed of natural uranium and of fuel elements formed of uranium depleted in U/sup 235/ to the extent that the combination will just support a chain reaction. The reactor is operated until the rate of burnup of plutonium equals its rate of production, the fuel elements are processed to recover plutonium, the depleted uranium is discarded, and the remaining uranium is formed into fuel elements. These fuel elements are charged into a reactor along with an equal number of fuel elements formed of uranium depleted in U/sup 235/ to the extent that the combination will just support a chain reaction, and reuse of the uranium is continued as aforesaid until it wlll no longer support a chain reaction when combined with an equal quantity of natural uranium.
Desideri, D; Meli, M A; Roselli, C; Testa, C; Boulyga, S F; Becker, J S
2002-11-01
It is well known that ammunition containing depleted uranium (DU) was used by NATO during the Balkan conflict. To evaluate the origin of DU (the enrichment of natural uranium or the reprocessing of spent nuclear fuel) it is necessary to directly detect the presence of activation products ((236)U, (239)Pu, (240)Pu, (241)Am, and (237)Np) in the ammunition. In this work the analysis of actinides by alpha-spectrometry was compared with that by inductively coupled plasma mass spectrometry (ICP-MS) after selective separation of ultratraces of transuranium elements from the uranium matrix. (242)Pu and (243)Am were added to calculate the chemical yield. Plutonium was separated from uranium by extraction chromatography, using tri- n-octylamine (TNOA), with a decontamination factor higher than 10(6); after elution plutonium was determined by ICP-MS ((239)Pu and (240)Pu) and alpha-spectrometry ((239+240)Pu) after electroplating. The concentration of Pu in two DU penetrator samples was 7 x 10(-12) g g(-1) and 2 x 10(-11) g g(-1). The (240)Pu/(239)Pu isotope ratio in one penetrator sample (0.12+/-0.04) was significantly lower than the (240)Pu/(239)Pu ratios found in two soil samples from Kosovo (0.35+/-0.10 and 0.27+/-0.07). (241)Am was separated by extraction chromatography, using di(2-ethylhexyl)phosphoric acid (HDEHP), with a decontamination factor as high as 10(7). The concentration of (241)Am in the penetrator samples was 2.7 x 10(-14) g g(-1) and <9.4 x 10(-15) g g(-1). In addition (237)Np was detected at ultratrace levels. In general, ICP-MS and alpha-spectrometry results were in good agreement. The presence of anthropogenic radionuclides ((236)U, (239)Pu,(240)Pu, (241)Am, and (237)Np) in the penetrators indicates that at least part of the uranium originated from the reprocessing of nuclear fuel. Because the concentrations of radionuclides are very low, their radiotoxicological effect is negligible.
Neace, J.C.
1984-03-13
A process is claimed for removing diluent degradation products from a solvent extraction solution, which has been used to recover uranium and plutonium from spent nuclear fuel. A wash solution and the solvent extraction solution are combined. The wash solution contains (a) water and (b) up to about, and including, 50 vol % of at least one-polar water-miscible organic solvent based on the total volume of the water and the highly-polar organic solvent. The wash solution also preferably contains at least one inorganic salt. The diluent degradation products dissolve in the highly-polar organic solvent and the organic solvent extraction solvent do not dissolve in the highly-polar organic solvent. The highly-polar organic solvent and the extraction solvent are separated.
Neace, James C.
1986-01-01
Process for removing diluent degradation products from a solvent extraction solution, which has been used to recover uranium and plutonium from spent nuclear fuel. A wash solution and the solvent extraction solution are combined. The wash solution contains (a) water and (b) up to about, and including, 50 volume percent of at least one-polar water-miscible organic solvent based on the total volume of the water and the highly-polar organic solvent. The wash solution also preferably contains at least one inorganic salt. The diluent degradation products dissolve in the highly-polar organic solvent and the organic solvent extraction solvent do not dissolve in the highly-polar organic solvent. The highly-polar organic solvent and the extraction solvent are separated.
Vauchy, Romain; Belin, Renaud C; Robisson, Anne-Charlotte; Lebreton, Florent; Aufore, Laurence; Scheinost, Andreas C; Martin, Philippe M
2016-03-07
Innovative americium-bearing uranium-plutonium mixed oxides U1-yPuyO2-x are envisioned as nuclear fuel for sodium-cooled fast neutron reactors (SFRs). The oxygen-to-metal (O/M) ratio, directly related to the oxidation state of cations, affects many of the fuel properties. Thus, a thorough knowledge of its variation with the sintering conditions is essential. The aim of this work is to follow the oxidation state of uranium, plutonium, and americium, and so the O/M ratio, in U0.750Pu0.246Am0.004O2-x samples sintered for 4 h at 2023 K in various Ar + 5% H2 + z vpm H2O (z = ∼ 15, ∼ 90, and ∼ 200) gas mixtures. The O/M ratios were determined by gravimetry, XAS, and XRD and evidenced a partial oxidation of the samples at room temperature. Finally, by comparing XANES and EXAFS results to that of a previous study, we demonstrate that the presence of uranium does not influence the interactions between americium and plutonium and that the differences in the O/M ratio between the investigated conditions is controlled by the reduction of plutonium. We also discuss the role of the homogeneity of cation distribution, as determined by EPMA, on the mechanisms involved in the reduction process.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kathren, R.L.
1992-09-01
This paper describes the history, organization, activities and recent scientific accomplishments of the United States Transuranium and Uranium Registries. Through voluntary donations of tissue obtained at autopsies, the Registries carry out studies of the concentration, distribution and biokinetics of plutonium in occupationally exposed persons. Findings from tissue analyses from more than 200 autopsies include the following: a greater proportion of the americium intake, as compared with plutonium, was found in the skeleton; the half-time of americium in liver is significantly shorter than that of plutonium; the concentration of actinide in the skeleton is inversely proportional to the calcium and ashmore » content of the bone; only a small percentage of the total skeletal deposition of plutonium is found in the marrow, implying a smaller risk from irradiation of the marrow relative to the bone surfaces; estimates of plutonium body burden made from urinalysis typically exceed those made from autopsy data; pathologists were unable to discriminate between a group of uranium workers and persons without known occupational exposure on the basis of evaluation of microscopic kidney slides; the skeleton is an important long term depot for uranium, and that the fractional uptake by both skeleton and kidney may be greater than indicated by current models. These and other findings and current studies are discussed in depth.« less
Baruzzini, Matthew L.; Hall, Howard L.; Spencer, Khalil J.; ...
2018-04-22
Investigations of the isotope fractionation behaviors of plutonium and uranium reference standards were conducted employing platinum and rhenium (Pt/Re) porous ion emitter (PIE) sources, a relatively new thermal ionization mass spectrometry (TIMS) ion source strategy. The suitability of commonly employed, empirically developed mass bias correction laws (i.e., the Linear, Power, and Russell's laws) for correcting such isotope ratio data was also determined. Corrected plutonium isotope ratio data, regardless of mass bias correction strategy, were statistically identical to that of the certificate, however, the process of isotope fractionation behavior of plutonium using the adopted experimental conditions was determined to be bestmore » described by the Power law. Finally, the fractionation behavior of uranium, using the analytical conditions described herein, is also most suitably modeled using the Power law, though Russell's and the Linear law for mass bias correction rendered results that were identical, within uncertainty, to the certificate value.« less
TRANSURANIC ELEMENT, COMPOSITION THEREOF, AND METHODS FOR PRODUCING SEPARATING AND PURIFYING SAME
Wahl, A.C.
1961-09-19
A process of separating plutonium from fission products contained in an aqueous solution is described. Plutonium, in the tri- or tetravalent state, and the fission products are coprecipitated on lanthanum fluoride, lanthanum oxalate, cerous fluoride, cerous phosphate, ceric iodate, zirconyl phosphate, thorium iodate, or thorium fluoride. The precipitate is dissolved in acid, and the plutonium is oxidized to the hexavalent state. The fission products are selectively precipitated on a carrier of the above group but different from that used for the coprecipitation. The plutonium in the solution, after removal of the fission product precipitate, is reduced to at least the tetravalent state and precipitated on lanthanum fluoride, lanthanum phosphate, lanthanum oxalate, lanthanum hydroxide, cerous fluoride, cerous phosphate, cerous oxalate, cerous hydroxide, ceric iodate, zirconyl phosphate, zirconyl iodate, zirconium hydroxide, thorium fluoride, thorium oxalate, thorium iodate, thorium peroxide, uranium iodate, uranium oxalate, or uranium peroxide, again using a different carrier than that used for the precipitation of the fission products.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Baruzzini, Matthew L.; Hall, Howard L.; Spencer, Khalil J.
Investigations of the isotope fractionation behaviors of plutonium and uranium reference standards were conducted employing platinum and rhenium (Pt/Re) porous ion emitter (PIE) sources, a relatively new thermal ionization mass spectrometry (TIMS) ion source strategy. The suitability of commonly employed, empirically developed mass bias correction laws (i.e., the Linear, Power, and Russell's laws) for correcting such isotope ratio data was also determined. Corrected plutonium isotope ratio data, regardless of mass bias correction strategy, were statistically identical to that of the certificate, however, the process of isotope fractionation behavior of plutonium using the adopted experimental conditions was determined to be bestmore » described by the Power law. Finally, the fractionation behavior of uranium, using the analytical conditions described herein, is also most suitably modeled using the Power law, though Russell's and the Linear law for mass bias correction rendered results that were identical, within uncertainty, to the certificate value.« less
Actinides in deer tissues at the rocky flats environmental technology site.
Todd, Andrew S; Sattelberg, R Mark
2005-11-01
Limited hunting of deer at the future Rocky Flats National Wildlife Refuge has been proposed in U.S. Fish and Wildlife planning documents as a compatible wildlife-dependent public use. Historically, Rocky Flats site activities resulted in the contamination of surface environmental media with actinides, including isotopes of americium, plutonium, and uranium. In this study, measurements of actinides [Americium-241 (241Am); Plutonium-238 (238Pu); Plutonium-239,240 (239,240Pu); uranium-233,244 (233,234U); uranium-235,236 (235,236U); and uranium-238 (238U)] were completed on select liver, muscle, lung, bone, and kidney tissue samples harvested from resident Rocky Flats deer (N = 26) and control deer (N = 1). In total, only 17 of the more than 450 individual isotopic analyses conducted on Rocky Flats deer tissue samples measured actinide concentrations above method detection limits. Of these 17 detects, only 2 analyses, with analytical uncertainty values added, exceeded threshold values calculated around a 1 x 10(-6) risk level (isotopic americium, 0.01 pCi/g; isotopic plutonium, 0.02 pCi/g; isotopic uranium, 0.2 pCi/g). Subsequent, conservative risk calculations suggest minimal human risk associated with ingestion of these edible deer tissues. The maximum calculated risk level in this study (4.73 x 10(-6)) is at the low end of the U.S. Environmental Protection Agency's acceptable risk range.
Michel, H; Levent, D; Barci, V; Barci-Funel, G; Hurel, C
2008-02-15
A new sequential method for the determination of both natural (U, Th) and anthropogenic (Sr, Cs, Pu, Am) radionuclides has been developed for application to soil and sediment samples. The procedure was optimised using a reference sediment (IAEA-368) and reference soils (IAEA-375 and IAEA-326). Reference materials were first digested using acids (leaching), 'total' acids on hot plate, and acids in microwave in order to compare the different digestion technique. Then, the separation and purification were made by anion exchange resin and selective extraction chromatography: transuranic (TRU) and strontium (SR) resins. Natural and anthropogenic alpha radionuclides were separated by uranium and tetravalent actinide (UTEVA) resin, considering different acid elution medium. Finally, alpha and gamma semiconductor spectrometer and liquid scintillation spectrometer were used to measure radionuclide activities. The results obtained for strontium-90, cesium-137, thorium-232, uranium-238, plutonium-239+240 and americium-241 isotopes by the proposed method for the reference materials provided excellent agreement with the recommended values and good chemical recoveries. Plutonium isotopes in alpha spectrometry planchet deposits could be also analysed by ICPMS.
PLUTONIUM PURIFICATION PROCESS EMPLOYING THORIUM PYROPHOSPHATE CARRIER
King, E.L.
1959-04-28
The separation and purification of plutonium from the radioactive elements of lower atomic weight is described. The process of this invention comprises forming a 0.5 to 2 M aqueous acidffc solution containing plutonium fons in the tetravalent state and elements with which it is normally contaminated in neutron irradiated uranium, treating the solution with a double thorium compound and a soluble pyrophosphate compound (Na/sub 4/P/sub 2/O/sub 7/) whereby a carrier precipitate of thorium A method is presented of reducing neptunium and - trite is advantageous since it destroys any hydrazine f so that they can be removed from solutions in which they are contained is described. In the carrier precipitation process for the separation of plutonium from uranium and fission products including zirconium and columbium, the precipitated blsmuth phosphate carries some zirconium, columbium, and uranium impurities. According to the invention such impurities can be complexed and removed by dissolving the contaminated carrier precipitate in 10M nitric acid, followed by addition of fluosilicic acid to about 1M, diluting the solution to about 1M in nitric acid, and then adding phosphoric acid to re-precipitate bismuth phosphate carrying plutonium.
METHOD OF SEPARATING PLUTONIUM
Heal, H.G.
1960-02-16
BS>A method of separating plutonium from aqueous nitrate solutions of plutonium, uranium. and high beta activity fission products is given. The pH of the aqueous solution is adjusted between 3.0 to 6.0 with ammonium acetate, ferric nitrate is added, and the solution is heated to 80 to 100 deg C to selectively form a basic ferric plutonium-carrying precipitate.
Seaborg, G.T.; Thompson, S.G.
1960-06-14
A process for concentrating plutonium is given in which plutonium is first precipitated with bismuth phosphate and then, after redissolution, precipitated with a different carrier such as lanthanum fluoride, uranium acetate, bismuth hydroxide, or niobic oxide.
Measurements of actinides in soil, sediments, water and vegetation in Northern New Mexico
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gallaher, B. M.; Efurd, D. W.
2002-01-01
This study was undertaken during 1991 - 1998 to identify the origin of plutonium uranium in northern New Mexico Rio Grande and tributary stream sediments. Isotopic fingerprinting techniques help distinguish radioactivity from Los Alamos National Laboratory (LANL) and from global fallout or natural sources. The geographic area covered by the study extended from the headwaters of the Rio Grande in southern Colorado to Elephant Butte Reservoir in southern New Mexico. Over 100 samples of stream channel and reservoir bottom sediments were analyzed for the atom ratios of plutonium and uranium isotopes using thermal ionization mass spectrometry (TIMS). Comparison of thesemore » ratios against those for fallout or natural sources allowed for quantification of the Laboratory impact. Of the seven major drainages crossing LANL, movement of LANL plutonium into the Rio Grande can only be traced via Los Alamos Canyon. The majority of sampled locations within and adjacent to LANL have little or no input of plutonium from the Laboratory. Samples collected upstream and distant to L A N show an average (+ s.d.) fallout 240Pu/239Pauto m ratio of 0.169 + 0.012, consistent with published worldwide global fallout values. These regional background ratios differ significantly from the 240Pu/239Pu atom ratio of 0.015 that is representative of LANL-derived plutonium entering the Rio Grande at Los Alamos Canyon. Mixing calculations of these sources indicate that the largest proportion (60% to 90%) of the plutonium in the Rio Grande sediments is from global atmospheric fallout, with an average of about 25% from the Laboratory. The LANL plutonium is identifiable intermittently along the 35-km reach of the Rio Grande to Cochiti Reservoir. The source of the LANL-derived plutonium in the Rio Grande was traced primarily to pre-1960 discharges of liquid effluents into a canyon bottom at a distance approximately 20 km upstream of the river. Plutonium levels decline exponentially with distance downstream after mixing with cleaner sediments, yet the LANL isotopic fingerprint remains distinct for at least 55 km from the effluent source. Plutonium isotopes in Rio Grande and Pajarito Plateau sediments are not at levels known to adversely affect public health. Activities of 239+240pwui thin this sample set ranged from 0.001- 0.046 pCUg in the Rio Grande to 3.7 pCi/g near the effluent discharge point. Levels in the Rio Grande are usually more than 1000 times. lower than prescribed cleanup standards. Uranium in stream and reservoir sediments is predominantly within natural concentration ranges and is of natural uranium isotopic composition. None of the sediments from the Rio Grande show identifiable Laboratory uranium, using the isotopic ratios. These results suggest that the mass of Laboratory-derived uranium entering the Rio Grande is small relative to the natural load carried with river sediments.« less
Atkinson, Will; Bérard, Philippe; Bingham, Derek; Birchall, Alan; Blanchardon, Eric; Bull, Richard; Guseva Canu, Irina; Challeton-de Vathaire, Cécile; Cockerill, Rupert; Do, Minh T.; Engels, Hilde; Figuerola, Jordi; Foster, Adrian; Holmstock, Luc; Hurtgen, Christian; Laurier, Dominique; Puncher, Matthew; Riddell, Anthony E.; Samson, Eric; Thierry-Chef, Isabelle; Tirmarche, Margot; Vrijheid, Martine; Cardis, Elisabeth
2017-01-01
Background: Carcinogenic risks of internal exposures to alpha-emitters (except radon) are poorly understood. Since exposure to alpha particles—particularly through inhalation—occurs in a range of settings, understanding consequent risks is a public health priority. We aimed to quantify dose–response relationships between lung dose from alpha-emitters and lung cancer in nuclear workers. Methods: We conducted a case–control study, nested within Belgian, French, and UK cohorts of uranium and plutonium workers. Cases were workers who died from lung cancer; one to three controls were matched to each. Lung doses from alpha-emitters were assessed using bioassay data. We estimated excess odds ratio (OR) of lung cancer per gray (Gy) of lung dose. Results: The study comprised 553 cases and 1,333 controls. Median positive total alpha lung dose was 2.42 mGy (mean: 8.13 mGy; maximum: 316 mGy); for plutonium the median was 1.27 mGy and for uranium 2.17 mGy. Excess OR/Gy (90% confidence interval)—adjusted for external radiation, socioeconomic status, and smoking—was 11 (2.6, 24) for total alpha dose, 50 (17, 106) for plutonium, and 5.3 (−1.9, 18) for uranium. Conclusions: We found strong evidence for associations between low doses from alpha-emitters and lung cancer risk. The excess OR/Gy was greater for plutonium than uranium, though confidence intervals overlap. Risk estimates were similar to those estimated previously in plutonium workers, and in uranium miners exposed to radon and its progeny. Expressed as risk/equivalent dose in sieverts (Sv), our estimates are somewhat larger than but consistent with those for atomic bomb survivors. See video abstract at, http://links.lww.com/EDE/B232. PMID:28520643
Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics
Booth, C.H.; Jiang, Yu; Wang, D.L.; Mitchell, J.N.; Tobash, P.H.; Bauer, E.D.; Wall, M.A.; Allen, P.G.; Sokaras, D.; Nordlund, D.; Weng, T.-C.; Torrez, M.A.; Sarrao, J.L.
2012-01-01
Uranium and plutonium’s 5f electrons are tenuously poised between strongly bonding with ligand spd-states and residing close to the nucleus. The unusual properties of these elements and their compounds (e.g., the six different allotropes of elemental plutonium) are widely believed to depend on the related attributes of f-orbital occupancy and delocalization for which a quantitative measure is lacking. By employing resonant X-ray emission spectroscopy (RXES) and X-ray absorption near-edge structure (XANES) spectroscopy and making comparisons to specific heat measurements, we demonstrate the presence of multiconfigurational f-orbital states in the actinide elements U and Pu and in a wide range of uranium and plutonium intermetallic compounds. These results provide a robust experimental basis for a new framework toward understanding the strongly-correlated behavior of actinide materials. PMID:22706643
Tags to Track Illicit Uranium and Plutonium
DOE Office of Scientific and Technical Information (OSTI.GOV)
Haire, M. Jonathan; Forsberg, Charles W.
2007-07-01
With the expansion of nuclear power, it is essential to avoid nuclear materials from falling into the hands of rogue nations, terrorists, and other opportunists. This paper examines the idea of detection and attribution tags for nuclear materials. For a detection tag, it is proposed to add small amounts [about one part per billion (ppb)] of {sup 232}U to enriched uranium to brighten its radioactive signature. Enriched uranium would then be as detectable as plutonium and thus increase the likelihood of intercepting illicit enriched uranium. The use of rare earth oxide elements is proposed as a new type of 'attribution'more » tag for uranium and thorium from mills, uranium and plutonium fuels, and other nuclear materials. Rare earth oxides are chosen because they are chemically compatible with the fuel cycle, can survive high-temperature processing operations in fuel fabrication, and can be chosen to have minimal neutronic impact within the nuclear reactor core. The mixture of rare earths and/or rare earth isotopes provides a unique 'bar code' for each tag. If illicit nuclear materials are recovered, the attribution tag can identify the source and lot of nuclear material, and thus help police reduce the possible number of suspects in the diversion of nuclear materials based on who had access. (authors)« less
Study on reduction and back extraction of Pu(IV) by urea derivatives in nitric acid conditions
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ye, G.A.; Xiao, S.T.; Yan, T.H.
2013-07-01
The reduction kinetics of Pu(IV) by hydroxyl-semicarbazide (HSC), hydroxyurea (HU) and di-hydroxyurea (DHU) in nitric acid solutions were investigated separately with adequate kinetic equations. In addition, counter-current cascade experiments were conducted for Pu split from U in nitric acid media using three kinds of reductant, respectively. The results show that urea derivatives as a kind of novel salt-free reductant can reduce Pu(IV) to Pu(III) rapidly in the nitric acid solutions. The stripping experimental results showed that Pu(IV) in the organic phase can be stripped rapidly to the aqueous phase by the urea derivatives, and the separation factors of plutonium /uraniummore » can reach more than 10{sup 4}. This indicates that urea derivatives is a kind of promising salt-free agent for uranium/plutonium separation. In addition, the complexing effect of HSC with Np(IV) was revealed, and Np(IV) can be back-extracted by HSC with a separation factor of about 20.« less
Donard, O F X; Bruneau, F; Moldovan, M; Garraud, H; Epov, V N; Boust, D
2007-03-28
Among the transuranic elements present in the environment, plutonium isotopes are mainly attached to particles, and therefore they present a great interest for the study and modelling of particle transport in the marine environment. Except in the close vicinity of industrial sources, plutonium concentration in marine sediments is very low (from 10(-4) ng kg(-1) for (241)Pu to 10 ng kg(-1) for (239)Pu), and therefore the measurement of (238)Pu, (239)Pu, (240)Pu, (241)Pu and (242)Pu in sediments at such concentration level requires the use of very sensitive techniques. Moreover, sediment matrix contains huge amounts of mineral species, uranium and organic substances that must be removed before the determination of plutonium isotopes. Hence, an efficient sample preparation step is necessary prior to analysis. Within this work, a chemical procedure for the extraction, purification and pre-concentration of plutonium from marine sediments prior to sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS) analysis has been optimized. The analytical method developed yields a pre-concentrated solution of plutonium from which (238)U and (241)Am have been removed, and which is suitable for the direct and simultaneous measurement of (239)Pu, (240)Pu, (241)Pu and (242)Pu by SF-ICP-MS.
Effect of cooling rate on achieving thermodynamic equilibrium in uranium-plutonium mixed oxides
NASA Astrophysics Data System (ADS)
Vauchy, Romain; Belin, Renaud C.; Robisson, Anne-Charlotte; Hodaj, Fiqiri
2016-02-01
In situ X-ray diffraction was used to study the structural changes occurring in uranium-plutonium mixed oxides U1-yPuyO2-x with y = 0.15; 0.28 and 0.45 during cooling from 1773 K to room-temperature under He + 5% H2 atmosphere. We compare the fastest and slowest cooling rates allowed by our apparatus i.e. 2 K s-1 and 0.005 K s-1, respectively. The promptly cooled samples evidenced a phase separation whereas samples cooled slowly did not due to their complete oxidation in contact with the atmosphere during cooling. Besides the composition of the annealing gas mixture, the cooling rate plays a major role on the control of the Oxygen/Metal ratio (O/M) and then on the crystallographic properties of the U1-yPuyO2-x uranium-plutonium mixed oxides.
Distillation of cadmium from uranium plutonium cadmium alloy
NASA Astrophysics Data System (ADS)
Kato, Tetsuya; Iizuka, Masatoshi; Inoue, Tadashi; Iwai, Takashi; Arai, Yasuo
2005-04-01
Uranium-plutonium alloy was prepared by distillation of cadmium from U-Pu-Cd ternary alloy. The initial ternary alloy contained 2.9 wt% U and 8.7 wt% Pu other than Cd, which were recovered by molten salt electrolysis with liquid Cd cathode. The distillation experiments were conducted in 10 g scale of the initial alloy using a small-scale distillation furnace equipped with an evaporator and a condenser in a vacuum vessel. After distillation at 1073 K, the weight of the residue was in good agreement with that of the loaded actinides, where the content of Cd decreased to less than 0.05 wt%. The uranium-plutonium alloy product was recovered without adhering to the yttria crucible. The cross section of the product was observed using electron probe micro-analyzer and it was found to consist of a dense material. Almost all of the evaporated Cd was recovered in the condenser and so enclosed well in the apparatus.
Inert matrix fuel in dispersion type fuel elements
NASA Astrophysics Data System (ADS)
Savchenko, A. M.; Vatulin, A. V.; Morozov, A. V.; Sirotin, V. L.; Dobrikova, I. V.; Kulakov, G. V.; Ershov, S. A.; Kostomarov, V. P.; Stelyuk, Y. I.
2006-06-01
The advantages of using inert matrix fuel (IMF) as a dispersion fuel in an aluminium alloy matrix are considered, in particular, low temperatures in the fuel centre, achievable high burn-ups, serviceability in transients and an environmentally friendly process of fuel rod fabrication. Two main versions of IMF are under development at A.A. Bochvar Institute, i.e. heterogeneous or isolated distribution of plutonium. The out-of-pile results on IMF loaded with uranium dioxide as plutonium simulator are presented. Fuel elements with uranium dioxide composition fabricated at A.A. Bochvar Institute are currently under MIR tests (RIAR, Dimitrovgrad). The fuel elements reached a burn-up of 88 MW d kg-1 (equivalent to the burn up of the standard uranium dioxide pelletized fuel) without loss of leak-tightness of the cladding. The feasibility of fabricating IMF of these particular types with plutonium dioxide is considered with a view to in-pile irradiation.
Baghdadi, S; Bouvier-Capely, C; Ritt, A; Peroux, A; Fevrier, L; Rebiere, F; Agarande, M; Cote, G
2015-11-01
Actinides determination in urine samples is part of the analyses performed to monitor internal contamination in case of an accident or a terrorist attack involving nuclear matter. Mineralisation is the first step of any of these analyses. It aims at reducing the sample volume and at destroying all organic compounds present. The mineralisation protocol is usually based on a wet ashing step, followed by actinides co-precipitation and a furnace ashing step, before redissolution and the quantification of the actinides by the appropriate techniques. Amongst the existing methods to perform the actinides co-precipitation, alkali-earth (typically calcium) precipitation is widely used. In the present work, the extraction of uranium(VI), plutonium(IV) and americium(III) from the redissolution solutions (called "mineralised urines") on calix[6]arene columns bearing hydroxamic groups was investigated as such an extraction is a necessary step before their determination by ICP-MS or alpha spectrometry. Difficulties were encountered in the transfer of uranium(VI) from raw to mineralised urines, with yield of transfer ranging between 0% and 85%, compared to about 90% for Pu and Am, depending on the starting raw urines. To understand the origin of such a difficulty, the speciation of uranium (VI) in mineralised urines was investigated by computer simulation using the MEDUSA software and the associated HYDRA database, compiled with recently published data. These calculations showed that the presence of phosphates in the "mineralised urines" leads to the formation of strong uranyl-phosphate complexes (such as UO2HPO4) which compete with the uranium (VI) extraction by the calix[6]arene bearing hydroxamic groups. The extraction constant of uranium (VI) by calix[6]arene bearing hydroxamic groups was determined in a 0.04 mol L(-1) sodium nitrate solution (logK=4.86±0.03) and implemented in an extraction model taking into account the speciation in the aqueous phase. This model allowed to simulate satisfactorily the experimental uranium extraction data and to support the preliminary conclusions about the role of the phosphates present in mineralised urines. These calculations also showed that the phosphate/calcium ratio is a key parameter as far as the efficiency of the uranium (VI) extraction by the calix[6]arene columns is concerned. It predicted that the addition of CaCl2 in mineralised urines would release uranium (VI) from phosphates by forming calcium (II)-phosphate complexes and thus facilitate the uranium (VI) extraction on calix[6]arene columns. These predictions were confirmed experimentally as the addition of 0.1 mol L(-1) CaCl2 to a mineralised urine containing naturally a high concentration of phosphate (typically 0.04 mol L(-1)) significantly increased the percentage of uranium (VI) extraction on the calix[6]arene columns. Copyright © 2015 Elsevier B.V. All rights reserved.
Measurement of dielectric constant of organic solvents by indigenously developed dielectric probe
NASA Astrophysics Data System (ADS)
Keshari, Ajay Kumar; Rao, J. Prabhakar; Rao, C. V. S. Brahmmananda; Ramakrishnan, R.; Ramanarayanan, R. R.
2018-04-01
The extraction, separation and purification of actinides (uranium and plutonium) from various matrices are an important step in nuclear fuel cycle. One of the separation process adopted in an industrial scale is the liquid-liquid extraction or solvent extraction. Liquid-liquid extraction uses a specific ligand/extractant in conjunction with suitable diluent. Solvent extraction or liquid-liquid extraction, involves the partitioning of the solute between two immiscible phases. In most cases, one of the phases is aqueous, and the other one is an organic solvent. The solvent used in solvent extraction should be selective for the metal of interest, it should have optimum distribution ratio, and the loaded metal from the organic phase should be easily stripped under suitable experimental conditions. Some of the important physical properties which are important for the solvent are density, viscosity, phase separation time, interfacial surface tension and the polarity of the extractant.
The North Korean nuclear dilemma.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hecker, Siegfried S.
2004-01-01
The current nuclear crisis, the second one in ten years, erupted when North Korea expelled international nuclear inspectors in December 2002, then withdrew from the Nuclear Nonproliferation Treaty (NPT), and claimed to be building more nuclear weapons with the plutonium extracted from the spent fuel rods heretofore stored under international inspection. These actions were triggered by a disagreement over U.S. assertions that North Korea had violated the Agreed Framework (which froze the plutonium path to nuclear weapons to end the first crisis in 1994) by clandestinely developing uranium enrichment capabilities providing an alternative path to nuclear weapons. With Stanford Universitymore » Professor John Lewis and three other Americans, I was allowed to visit the Yongbyon Nuclear Center on Jan. 8, 2004. We toured the 5 MWe reactor, the 50 MWe reactor construction site, the spent fuel pool storage building, and the radiochemical laboratory. We concluded that North Korea has restarted its 5 MWe reactor (which produces roughly 6 kg of plutonium annually), it removed the 8000 spent fuel rods that were previously stored under IAEA safeguards from the spent fuel pool, and that it most likely extracted the 25 to 30 kg of plutonium contained in these fuel rods. Although North Korean officials showed us what they claimed was their plutonium metal product from this reprocessing campaign, we were not able to conclude definitively that it was in fact plutonium metal and that it came from the most recent reprocessing campaign. Nevertheless, our North Korean hosts demonstrated that they had the capability, the facility and requisite capacity, and the technical expertise to produce plutonium metal. On the basis of our visit, we were not able to address the issue of whether or not North Korea had a 'deterrent' as claimed - that is, we were not able to conclude that North Korea can build a nuclear device and that it can integrate nuclear devices into suitable delivery systems. However, based on the capabilities we saw, we must assume that North Korea has the capability to produce a crude nuclear device. On the matter of uranium enrichment programs, our host categorically denied that North Korea has a uranium enrichment program - he said, 'we have no program, no equipment, and no technical expertise for uranium enrichment.' The denials were not convincing at the time and since then have proven to be quite hollow by the revelations of A.Q. Khan's nuclear black market activities. There is no easy solution to the nuclear crisis in North Korea. A military strike to eliminate the nuclear facilities was never very attractive and now has been overcome by events. The principal threat is posed by a stockpile of nuclear weapons and weapons-grade plutonium. We have no way of finding where either may be hidden. A diplomatic solution remains the only path forward, but it has proven elusive. All sides have proclaimed a nuclear weapons-free Korean Peninsula as the end goal. The U.S. Government has chosen to negotiate with North Korea by means of the six-party talks. It has very clearly outlined its position of insisting on complete, verifiable, irreversible dismantlement of all North Korean nuclear programs. North Korea has offered several versions of 're-freezing' its plutonium program while still denying a uranium enrichment program. It has insisted on simultaneous and reciprocal steps to a final solution. Regardless of which diplomatic path is chosen, the scientific challenges of eliminating the North Korean nuclear weapons programs (and its associated infrastructure) in a safe, secure, and verifiable manner are immense. The North Korean program is considerably more complex and developed than the fledgling Iraqi program of 1991 and Libyan program of 2004. It is more along the lines, but more complex than that of South Africa in the early 1990s. Actions taken or not taken by the North Koreans at their nuclear facilities during the course of the ongoing diplomatic discussions are key to whether or not the nuclear program can be eliminated safely and securely, and they will greatly influence the price tag for such operations. Moreover, they will determine whether or not one can verify complete elimination. Hence, cooperation of the North Koreans now and during the dismantlement and elimination stages is crucial. Technical discussions among specialists, perhaps within the framework of the working groups of the six-party talks, could be very productive in setting the stage for an effective, verifiable elimination of North Korea's nuclear weapons program.« less
Chemical Disposition of Plutonium in Hanford Site Tank Wastes
DOE Office of Scientific and Technical Information (OSTI.GOV)
Delegard, Calvin H.; Jones, Susan A.
2015-05-07
This report examines the chemical disposition of plutonium (Pu) in Hanford Site tank wastes, by itself and in its observed and potential interactions with the neutron absorbers aluminum (Al), cadmium (Cd), chromium (Cr), iron (Fe), manganese (Mn), nickel (Ni), and sodium (Na). Consideration also is given to the interactions of plutonium with uranium (U). No consideration of the disposition of uranium itself as an element with fissile isotopes is considered except tangentially with respect to its interaction as an absorber for plutonium. The report begins with a brief review of Hanford Site plutonium processes, examining the various means used tomore » recover plutonium from irradiated fuel and from scrap, and also examines the intermediate processing of plutonium to prepare useful chemical forms. The paper provides an overview of Hanford tank defined-waste–type compositions and some calculations of the ratios of plutonium to absorber elements in these waste types and in individual waste analyses. These assessments are based on Hanford tank waste inventory data derived from separately published, expert assessments of tank disposal records, process flowsheets, and chemical/radiochemical analyses. This work also investigates the distribution and expected speciation of plutonium in tank waste solution and solid phases. For the solid phases, both pure plutonium compounds and plutonium interactions with absorber elements are considered. These assessments of plutonium chemistry are based largely on analyses of idealized or simulated tank waste or strongly alkaline systems. The very limited information available on plutonium behavior, disposition, and speciation in genuine tank waste also is discussed. The assessments show that plutonium coprecipitates strongly with chromium, iron, manganese and uranium absorbers. Plutonium’s chemical interactions with aluminum, nickel, and sodium are minimal to non-existent. Credit for neutronic interaction of plutonium with these absorbers occurs only if they are physically proximal in solution or the plutonium present in the solid phase is intimately mixed with compounds or solutions of these absorbers. No information on the potential chemical interaction of plutonium with cadmium was found in the technical literature. Definitive evidence of sorption or adsorption of plutonium onto various solid phases from strongly alkaline media is less clear-cut, perhaps owing to fewer studies and to some well-attributed tests run under conditions exceeding the very low solubility of plutonium. The several studies that are well-founded show that only about half of the plutonium is adsorbed from waste solutions onto sludge solid phases. The organic complexants found in many Hanford tank waste solutions seem to decrease plutonium uptake onto solids. A number of studies show plutonium sorbs effectively onto sodium titanate. Finally, this report presents findings describing the behavior of plutonium vis-à-vis other elements during sludge dissolution in nitric acid based on Hanford tank waste experience gained by lab-scale tests, chemical and radiochemical sample characterization, and full-scale processing in preparation for strontium-90 recovery from PUREX sludges.« less
URANOUS IODATE AS A CARRIER FOR PLUTONIUM
Miller, D.R.; Seaborg, G.T.; Thompson, S.G.
1959-12-15
A process is described for precipitating plutonium on a uranous iodate carrier from an aqueous acid solution conA plutonium solution more concentrated than the original solution can then be obtained by oxidizing the uranium to the hexavalent state and dissolving the precipitate, after separating the latter from the original solution, by means of warm nitric acid.
Solvent extraction system for plutonium colloids and other oxide nano-particles
Soderholm, Lynda; Wilson, Richard E; Chiarizia, Renato; Skanthakumar, Suntharalingam
2014-06-03
The invention provides a method for extracting plutonium from spent nuclear fuel, the method comprising supplying plutonium in a first aqueous phase; contacting the plutonium aqueous phase with a mixture of a dielectric and a moiety having a first acidity so as to allow the plutonium to substantially extract into the mixture; and contacting the extracted plutonium with second a aqueous phase, wherein the second aqueous phase has a second acidity higher than the first acidity, so as to allow the extracted plutonium to extract into the second aqueous phase. The invented method facilitates isolation of plutonium polymer without the formation of crud or unwanted emulsions.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hay, M. S.
Savannah River National Laboratory analyzed samples from Tank 38H and Tank 43H to support Enrichment Control Program and Corrosion Control Program. The total uranium in the Tank 38H samples ranged from 20.5 to 34.0 mg/L while the Tank 43H samples ranged from 47.6 to 50.6 mg/L. The U-235 percentage ranged from 0.62% to 0.64% over the four samples. The total uranium and percent U-235 results appear consistent with previous Tank 38H and Tank 43H uranium measurements. The Tank 38H plutonium results show a large difference between the surface and sub-surface sample concentrations and a somewhat higher concentration than previous sub-surfacemore » samples. The two Tank 43H samples show similar plutonium concentrations and are within the range of values measured on previous samples. The plutonium results may be biased high due to the presence of plutonium contamination in the blank samples from the cell sample preparations. The four samples analyzed show silicon concentrations ranging from 47.9 to 105 mg/L.« less
ERIC Educational Resources Information Center
Finch, Warren I.
1978-01-01
The results of President Carter's policy on non-proliferation of nuclear weapons are expected to slow the growth rate in energy consumption, put the development of the breeder reactor in question, halt plans to reprocess and recycle uranium and plutonium, and expand facilities to supply enriched uranium. (Author/MA)
Plutonium Decontamination of Uranium using CO2 Cleaning
DOE Office of Scientific and Technical Information (OSTI.GOV)
Blau, M
A concern of the Department of Energy (DOE) Environmental Management (EM) and Defense Programs (DP), and of the Los Alamos National Laboratory (LANL) and the Lawrence Livermore National Laboratory (LLNL), is the disposition of thousands of legacy and recently generated plutonium (Pu)-contaminated, highly enriched uranium (HEU) parts. These parts take up needed vault space. This presents a serious problem for LLNL, as site limit could result in the stoppage of future weapons work. The Office of Fissile Materials Disposition (NN-60) will also face a similar problem as thousands of HEU parts will be created with the disassembly of site-return pitsmore » for plutonium recovery when the Pit Disassembly and Conversion Facility (PDCF) at the Savannah River Site (SRS) becomes operational. To send HEU to the Oak Ridge National Laboratory and the Y-12 Plant for disposition, the contamination for metal must be less than 20 disintegrations per minute (dpm) of swipable transuranic per 100 cm{sup 2} of surface area or the Pu bulk contamination for oxide must be less than 210 parts per billion (ppb). LANL has used the electrolytic process on Pu-contaminated HEU weapon parts with some success. However, this process requires that a different fixture be used for every configuration; each fixture cost approximately $10K. Moreover, electrolytic decontamination leaches the uranium metal substrate (no uranium or plutonium oxide) from the HEU part. The leaching rate at the uranium metal grain boundaries is higher than that of the grains and depends on the thickness of the uranium oxide layer. As the leaching liquid flows past the HEU part, it carries away plutonium oxide contamination and uranium oxide. The uneven uranium metal surface created by the leaching becomes a trap for plutonium oxide contamination. In addition, other DOE sites have used CO{sub 2} cleaning for Pu decontamination successfully. In the 1990's, the Idaho National Engineering Laboratory investigated this technology and showed that CO{sub 2} pellet blasting (or CO{sub 2} cleaning) reduced both fixed and smearable contamination on tools. In 1997, LLNL proved that even tritium contamination could be removed from a variety of different matrices using CO{sub 2}cleaning. CO{sub 2} cleaning is a non-toxic, nonconductive, nonabrasive decontamination process whose primary cleaning mechanisms are: (1) Impact of the CO{sub 2} pellets loosens the bond between the contaminant and the substrate. (2) CO{sub 2} pellets shatter and sublimate into a gaseous state with large expansion ({approx}800 times). The expanding CO{sub 2} gas forms a layer between the contaminant and the substrate that acts as a spatula and peels off the contaminant. (3) Cooling of the contaminant assists in breaking its bond with the substrate. Thus, LLNL conducted feasibility testing to determine if CO{sub 2} pellet blasting could remove Pu contamination (e.g., uranium oxide) from uranium metal without abrading the metal matrix. This report contains a summary of events and the results of this test.« less
Griffiths, N M; Van der Meeren, A; Fritsch, P; Abram, M-C; Bernaudin, J-F; Poncy, J L
2010-09-01
Accidental exposure by inhalation to alpha-emitting particles from mixed oxide (MOX: uranium and plutonium oxide) fuels is a potential long-term health risk to workers in nuclear fuel fabrication plants. For MOX fuels, the risk of lung cancer development may be different from that assigned to individual components (plutonium, uranium) given different physico-chemical characteristics. The objective of this study was to investigate late effects in rat lungs following inhalation of MOX aerosols of similar particle size containing 2.5 or 7.1% plutonium. Conscious rats were exposed to MOX aerosols and kept for their entire lifespan. Different initial lung burdens (ILBs) were obtained using different amounts of MOX. Lung total alpha activity was determined by external counting and at autopsy for total lung dose calculation. Fixed lung tissue was used for anatomopathological, autoradiographical, and immunohistochemical analyses. Inhalation of MOX at ILBs ranging from 1-20 kBq resulted in lung pathologies (90% of rats) including fibrosis (70%) and malignant lung tumors (45%). High ILBs (4-20 kBq) resulted in reduced survival time (N = 102; p < 0.05) frequently associated with lung fibrosis. Malignant tumor incidence increased linearly with dose (up to 60 Gy) with a risk of 1-1.6% Gy for MOX, similar to results for industrial plutonium oxide alone (1.9% Gy). Staining with antibodies against Surfactant Protein-C, Thyroid Transcription Factor-1, or Oct-4 showed differential labeling of tumor types. In conclusion, late effects following MOX inhalation result in similar risk for development of lung tumors as compared with industrial plutonium oxide.
Boyd, G.E.
1958-08-26
A process is presented fer separating uranium, plutonium, and fission products ions from uranyl nitrate solutions having a pH value between 1 and 3 obtained by dissolving neutron irradiated uranium. The method consists in passing such solutions through a bed of cation exchange resin, which may be a sulfonated phenol formaidehyde type. Following the adsorption step the resin is first treated with a solution of 0.2M to 0.3M sulfuric acid to desorb the uranium. Fission product ions are then desorbed by treating the resin in phosphoric acid and 1M in nitric acid. Lastly, the plutonium may be desorbed by treating the resin with a solution approximately 0.8M in phosphoric acid and 1M in nitric acid.
Recovery of fissile materials from nuclear wastes
Forsberg, Charles W.
1999-01-01
A process for recovering fissile materials such as uranium, and plutonium, and rare earth elements, from complex waste feed material, and converting the remaining wastes into a waste glass suitable for storage or disposal. The waste feed is mixed with a dissolution glass formed of lead oxide and boron oxide resulting in oxidation, dehalogenation, and dissolution of metal oxides. Carbon is added to remove lead oxide, and a boron oxide fusion melt is produced. The fusion melt is essentially devoid of organic materials and halogens, and is easily and rapidly dissolved in nitric acid. After dissolution, uranium, plutonium and rare earth elements are separated from the acid and recovered by processes such as PUREX or ion exchange. The remaining acid waste stream is vitrified to produce a waste glass suitable for storage or disposal. Potential waste feed materials include plutonium scrap and residue, miscellaneous spent nuclear fuel, and uranium fissile wastes. The initial feed materials may contain mixtures of metals, ceramics, amorphous solids, halides, organic material and other carbon-containing material.
NASA Astrophysics Data System (ADS)
Huda, Muhammad Nurul
Atomic and molecular adsorptions of oxygen and hydrogen on actinide surfaces have been studied within the generalized gradient approximations to density functional theory (GGA-DFT). The primary goal of this work is to understand the details of the adsorption processes, such as chemisorption sites, energies, adsorption configurations and activation energies for dissociation of molecules; and the signature role of the plutonium 5f electrons. The localization of the 5f electrons remains one of central questions in actinides and one objective here is to understand the extent to which localizations plays a role in adsorption on actinide surfaces. We also investigated the magnetism of the plutonium surfaces, given the fact that magnetism in bulk plutonium is a highly controversial issue, and the surface magnetism of it is not a well explored territory. Both the non-spin-polarized and spin-polarized calculations have been performed to arrive at our conclusions. We have studied both the atomic and molecular hydrogen and oxygen adsorptions on plutonium (100) and (111) surfaces. We have also investigated the oxygen molecule adsorptions on uranium (100) surface. Comparing the adsorption on uranium and plutonium (100) surfaces, we have seen that O2 chemisorption energy for the most favorable adsorption site on uranium surface has higher chemisorption energy, 9.492 eV, than the corresponding plutonium site, 8.787 eV. Also degree of localization of 5f electrons is less for uranium surface. In almost all of the cases, the most favorable adsorption sites are found where the coordination numbers are higher. For example, we found center sites are the most favorable sites for atomic adsorptions. In general oxygen reacts more strongly with plutonium surface than hydrogen. We found that atomic oxygen adsorption energy on (100) surface is 3.613 eV more than that of the hydrogen adsorptions, considering only the most favorable site. This is also true for molecular adsorptions, as the oxygen molecules on both (100) and (111) plutonium surfaces dissociate almost spontaneously, whereas hydrogen needs some activation energy to dissociate. From spin-polarized calculations we found both (100) and (111) surfaces have the layer by layer alternating spin-magnetic behavior. In general adsorption of H2 and O2 do not change this behavior.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Freeman-Pollard, J.R.
1994-03-02
This engineering study addresses 50 inactive underground radioactive waste tanks. The tanks were formerly used for the following functions associated with plutonium and uranium separations and waste management activities in the 200 East and 200 West Areas of the Hanford Site: settling solids prior to disposal of supernatant in cribs and a reverse well; neutralizing acidic process wastes prior to crib disposal; receipt and processing of single-shell tank (SST) waste for uranium recovery operations; catch tanks to collect water that intruded into diversion boxes and transfer pipeline encasements and any leakage that occurred during waste transfer operations; and waste handlingmore » and process experimentation. Most of these tanks have not been in use for many years. Several projects have, been planned and implemented since the 1970`s and through 1985 to remove waste and interim isolate or interim stabilize many of the tanks. Some tanks have been filled with grout within the past several years. Responsibility for final closure and/or remediation of these tanks is currently assigned to several programs including Tank Waste Remediation Systems (TWRS), Environmental Restoration and Remedial Action (ERRA), and Decommissioning and Resource Conservation and Recovery Act (RCRA) Closure (D&RCP). Some are under facility landlord responsibility for maintenance and surveillance (i.e. Plutonium Uranium Extraction [PUREX]). However, most of the tanks are not currently included in any active monitoring or surveillance program.« less
Rapid fusion method for the determination of refractory thorium and uranium isotopes in soil samples
Maxwell, Sherrod L.; Hutchison, Jay B.; McAlister, Daniel R.
2015-02-14
Recently, approximately 80% of participating laboratories failed to accurately determine uranium isotopes in soil samples in the U.S Department of Energy Mixed Analyte Performance Evaluation Program (MAPEP) Session 30, due to incomplete dissolution of refractory particles in the samples. Failing laboratories employed acid dissolution methods, including hydrofluoric acid, to recover uranium from the soil matrix. The failures illustrate the importance of rugged soil dissolution methods for the accurate measurement of analytes in the sample matrix. A new rapid fusion method has been developed by the Savannah River National Laboratory (SRNL) to prepare 1-2 g soil sample aliquots very quickly, withmore » total dissolution of refractory particles. Soil samples are fused with sodium hydroxide at 600 ºC in zirconium crucibles to enable complete dissolution of the sample. Uranium and thorium are separated on stacked TEVA and TRU extraction chromatographic resin cartridges, prior to isotopic measurements by alpha spectrometry on cerium fluoride microprecipitation sources. Plutonium can also be separated and measured using this method. Batches of 12 samples can be prepared for measurement in <5 hours.« less
Tc-99 Decontamination From Heat Treated Gaseous Diffusion Membrane -Phase I
DOE Office of Scientific and Technical Information (OSTI.GOV)
Oji, L.; Wilmarth, B.; Restivo, M.
2017-03-13
Uranium gaseous diffusion cascades represent a significant environmental challenge to dismantle, containerize and dispose as low-level radioactive waste. Baseline technologies rely on manual manipulations involving direct access to technetium-contaminated piping and materials. There is a potential to utilize novel thermal decontamination technologies to remove the technetium and allow for on-site disposal of the very large uranium converters. Technetium entered these gaseous diffusion cascades as a hexafluoride complex in the same fashion as uranium. Technetium, as the isotope Tc-99, is an impurity that follows uranium in the first cycle of the Plutonium and Uranium Extraction (PUREX) process. The technetium speciation ormore » exact form in the gas diffusion cascades is not well defined. Several forms of Tc-99 compounds, mostly the fluorinated technetium compounds with varying degrees of volatility have been speculated by the scientific community to be present in these cascades. Therefore, there may be a possibility of using thermal desorption, which is independent of the technetium oxidation states, to perform an in situ removal of the technetium as a volatile species and trap the radionuclide on sorbent traps which could be disposed as low-level waste.« less
Overview of reductants utilized in nuclear fuel reprocessing/recycling
DOE Office of Scientific and Technical Information (OSTI.GOV)
Paviet-Hartmann, P.; Riddle, C.; Campbell, K.
2013-07-01
The most widely used reductant to partition plutonium from uranium in the Purex process was ferrous sulfamate, other alternates were proposed such as hydrazine-stabilized ferrous nitrate or uranous nitrate, platinum catalyzed hydrogen, and hydrazine, hydroxylamine salts. New candidates to replace hydrazine or hydroxylamine nitrate (HAN) are pursued worldwide. They may improve the performance of the industrial Purex process towards different operations such as de-extraction of plutonium and reduction of the amount of hydrazine which will limit the formation of hydrazoic acid. When looking at future recycling technologies using hydroxamic ligands, neither acetohydroxamic acid (AHA) nor formohydroxamic acid (FHA) seem promisingmore » because they hydrolyze to give hydroxylamine and the parent carboxylic acid. Hydroxyethylhydrazine, HOC{sub 2}H{sub 4}N{sub 2}H{sub 3} (HEH) is a promising non-salt-forming reductant of Np and Pu ions because it is selective to neptunium and plutonium ions at room temperature and at relatively low acidity, it could serve as a replacement of HAN or AHA for the development of a novel used nuclear fuel recycling process.« less
METHOD OF RECOVERING TRANSURANIC ELEMENTS OF AN ATOMIC NUMBER BELOW 95
Seaborg, G.T.; James, R.A.
1959-12-15
The concentration of neptanium or plutonium by two carrier precipitation steps with identical carriers but using (after dissolution of the first carrier in nitric acid) a reduced quantity of carrier for the second precipitation is discussed. Carriers suitable are uranium(IV) hypophosphate, uranium(IV) pyrophosphate, uranium(IV) oxalate, thorium oxalate, thorium citrate, thorium tartrate, thorium sulfide, and uranium(IV) sulfide.
Fuel bundle design for enhanced usage of plutonium fuel
Reese, Anthony P.; Stachowski, Russell E.
1995-01-01
A nuclear fuel bundle includes a square array of fuel rods each having a concentration of enriched uranium and plutonium. Each rod of an interior array of the rods also has a concentration of gadolinium. The interior array of rods is surrounded by an exterior array of rods void of gadolinium. By this design, usage of plutonium in the nuclear reactor is enhanced.
Fuel bundle design for enhanced usage of plutonium fuel
Reese, A.P.; Stachowski, R.E.
1995-08-08
A nuclear fuel bundle includes a square array of fuel rods each having a concentration of enriched uranium and plutonium. Each rod of an interior array of the rods also has a concentration of gadolinium. The interior array of rods is surrounded by an exterior array of rods void of gadolinium. By this design, usage of plutonium in the nuclear reactor is enhanced. 10 figs.
DOUBLE TRACKS Test Site interim corrective action plan
DOE Office of Scientific and Technical Information (OSTI.GOV)
NONE
The DOUBLE TRACKS site is located on Range 71 north of the Nellis Air Force Range, northwest of the Nevada Test Site (NTS). DOUBLE TRACKS was the first of four experiments that constituted Operation ROLLER COASTER. On May 15, 1963, weapons-grade plutonium and depleted uranium were dispersed using 54 kilograms of trinitrotoluene (TNT) explosive. The explosion occurred in the open, 0.3 m above the steel plate. No fission yield was detected from the test, and the total amount of plutonium deposited on the ground surface was estimated to be between 980 and 1,600 grams. The test device was composed primarilymore » of uranium-238 and plutonium-239. The mass ratio of uranium to plutonium was 4.35. The objective of the corrective action is to reduce the potential risk to human health and the environment and to demonstrate technically viable and cost-effective excavation, transportation, and disposal. To achieve these objectives, Bechtel Nevada (BN) will remove soil with a total transuranic activity greater then 200 pCI/g, containerize the soil in ``supersacks,`` transport the filled ``supersacks`` to the NTS, and dispose of them in the Area 3 Radioactive Waste Management Site. During this interim corrective action, BN will also conduct a limited demonstration of an alternative method for excavation of radioactive near-surface soil contamination.« less
Bartholomay, Roy C.; L. Flint Hall,
2016-05-05
The upper limit of background concentrations for radiochemical constituents for eastern regional water was 5.43 ±0.574 pCi/L for tritium, 0.0002048 ±0.0000054 pCi/L for chlorine-36, 0.000000865 ±0.000000015 pCi/L for iodine-129, <0.0000054 pCi/L for technetium-99, 0 pCi/L for strontium-90, plutonium-238, plutonium-239, -240 (undivided), and americium-241, 1.32 ±0.77 pCi/L for uranium-234, 0.016 ±0.012 pCi/L for uranium-235, and 0.477 ±0.044 pCi/L for uranium-238.
CHEMICAL DIFFERENCES BETWEEN SLUDGE SOLIDS AT THE F AND H AREA TANK FARMS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Reboul, S.
2012-08-29
The primary source of waste solids received into the F Area Tank Farm (FTF) was from PUREX processing performed to recover uranium and plutonium from irradiated depleted uranium targets. In contrast, two primary sources of waste solids were received into the H Area Tank Farm (HTF): a) waste from PUREX processing; and b) waste from H-modified (HM) processing performed to recover uranium and neptunium from burned enriched uranium fuel. Due to the differences between the irradiated depleted uranium targets and the burned enriched uranium fuel, the average compositions of the F and H Area wastes are markedly different from onemore » another. Both F and H Area wastes contain significant amounts of iron and aluminum compounds. However, because the iron content of PUREX waste is higher than that of HM waste, and the aluminum content of PUREX waste is lower than that of HM waste, the iron to aluminum ratios of typical FTF waste solids are appreciably higher than those of typical HTF waste solids. Other constituents present at significantly higher concentrations in the typical FTF waste solids include uranium, nickel, ruthenium, zinc, silver, cobalt and copper. In contrast, constituents present at significantly higher concentrations in the typical HTF waste solids include mercury, thorium, oxalate, and radionuclides U-233, U-234, U-235, U-236, Pu-238, Pu-242, Cm-244, and Cm-245. Because of the higher concentrations of Pu-238 in HTF, the long-term concentrations of Th-230 and Ra-226 (from Pu-238 decay) will also be higher in HTF. The uranium and plutonium distributions of the average FTF waste were found to be consistent with depleted uranium and weapons grade plutonium, respectively (U-235 comprised 0.3 wt% of the FTF uranium, and Pu-240 comprised 6 wt% of the FTF plutonium). In contrast, at HTF, U-235 comprised 5 wt% of the uranium, and Pu-240 comprised 17 wt% of the plutonium, consistent with enriched uranium and high burn-up plutonium. X-ray diffraction analyses of various FTF and HTF samples indicated that the primary crystalline compounds of iron in sludge solids are Fe{sub 2}O{sub 3}, Fe{sub 3}O{sub 4}, and FeO(OH), and the primary crystalline compounds of aluminum are Al(OH){sub 3} and AlO(OH). Also identified were carbonate compounds of calcium, magnesium, and sodium; a nitrated sodium aluminosilicate; and various uranium compounds. Consistent with expectations, oxalate compounds were identified in solids associated with oxalic acid cleaning operations. The most likely oxidation states and chemical forms of technetium are assessed in the context of solubility, since technetium-99 is a key risk driver from an environmental fate and transport perspective. The primary oxidation state of technetium in SRS sludge solids is expected to be Tc(IV). In salt waste, the primary oxidation state is expected to be Tc(VII). The primary form of technetium in sludge is expected to be a hydrated technetium dioxide, TcO{sub 2} {center_dot} xH{sub 2}O, which is relatively insoluble and likely co-precipitated with iron. In salt waste solutions, the primary form of technetium is expected to be the very soluble pertechnetate anion, TcO{sub 4}{sup -}. The relative differences between the F and H Tank Farm waste provide a basis for anticipating differences that will occur as constituents of FTF and HTF waste residue enter the environment over the long-term future. If a constituent is significantly more dominant in one of the Tank Farms, its long-term environmental contribution will likely be commensurately higher, assuming the environmental transport conditions of the two Tank Farms share some commonality. It is in this vein that the information cited in this document is provided - for use during the generation, assessment, and validation of Performance Assessment modeling results.« less
A XAS study of the local environments of cations in (U, Ce)O 2
NASA Astrophysics Data System (ADS)
Martin, Philippe; Ripert, Michel; Petit, Thierry; Reich, Tobias; Hennig, Christoph; D'Acapito, Francesco; Hazemann, Jean Louis; Proux, Olivier
2003-01-01
Mixed oxide (MOX) fuel is usually considered as a solid solution formed by uranium and plutonium dioxides. Nevertheless, some physico-chemical properties of (U 1- y, Pu y)O 2 samples manufactured under industrial conditions showed anomalies in the domain of plutonium contents ranging between 3 and 15 at.%. Cerium is commonly used as an inactive analogue of plutonium in preliminary studies on MOX fuels. Extended X-ray Absorption Fine Structure (EXAFS) measurements performed at the European Synchrotron Radiation Facility (ESRF) at the cerium and uranium edges on (U 1- y, Ce y)O 2 samples are presented and discussed. They confirmed on an atomic scale the formation of an ideal solid solution for cerium concentrations ranging between 0 and 50 at.%.
A METHOD OF PREPARING URANIUM DIOXIDE
Scott, F.A.; Mudge, L.K.
1963-12-17
A process of purifying raw, in particular plutonium- and fission- products-containing, uranium dioxide is described. The uranium dioxide is dissolved in a molten chloride mixture containing potassium chloride plus sodium, lithium, magnesium, or lead chloride under anhydrous conditions; an electric current and a chlorinating gas are passed through the mixture whereby pure uranium dioxide is deposited on and at the same time partially redissolved from the cathode. (AEC)
15. VIEW OF LABORATORY EQUIPMENT IN THE BUILDING 771 ANALYTICAL ...
15. VIEW OF LABORATORY EQUIPMENT IN THE BUILDING 771 ANALYTICAL LABORATORY. THE LAB ANALYZED SAMPLES FOR PLUTONIUM, AMERICIUM, URANIUM, NEPTUNIUM, AND OTHER RADIOACTIVE ISOTOPES. (9/25/62) - Rocky Flats Plant, Plutonium Recovery & Fabrication Facility, North-central section of plant, Golden, Jefferson County, CO
Influence of point defects and impurities on the dynamical stability of δ-plutonium
NASA Astrophysics Data System (ADS)
Dorado, B.; Bieder, J.; Torrent, M.
2017-06-01
We use first-principles calculations to provide direct evidence of the effect of aluminum, gallium, iron and uranium on the dynamical stability of δ-plutonium. We first show that the δ phase is dynamically unstable at low temperature, as seen in experiments, and that this stability directly depends on the plutonium 5f orbital occupancies. Then, we demonstrate that both aluminum and gallium stabilize the δ phase, contrary to iron. As for uranium, which is created during self-irradiation and whose effect on plutonium has yet to be understood, we show that it leaves a few unstable vibrational modes and that higher concentrations lead to an almost complete stabilization. Finally, we provide an attempt at a consistent analysis of the experimental Pu-Ga phonon density of states. We show that the presence of gallium can reproduce only partially the experimental measurements, and we investigate how point defects, such as interstitials and vacancies, affect the calculated phonon density of states.
Influence of point defects and impurities on the dynamical stability of δ-plutonium.
Dorado, B; Bieder, J; Torrent, M
2017-06-21
We use first-principles calculations to provide direct evidence of the effect of aluminum, gallium, iron and uranium on the dynamical stability of δ-plutonium. We first show that the δ phase is dynamically unstable at low temperature, as seen in experiments, and that this stability directly depends on the plutonium 5f orbital occupancies. Then, we demonstrate that both aluminum and gallium stabilize the δ phase, contrary to iron. As for uranium, which is created during self-irradiation and whose effect on plutonium has yet to be understood, we show that it leaves a few unstable vibrational modes and that higher concentrations lead to an almost complete stabilization. Finally, we provide an attempt at a consistent analysis of the experimental Pu-Ga phonon density of states. We show that the presence of gallium can reproduce only partially the experimental measurements, and we investigate how point defects, such as interstitials and vacancies, affect the calculated phonon density of states.
METHOD OF SEPARATING PLUTONIUM
Brown, H.S.; Hill, O.F.
1958-02-01
Plutonium hexafluoride is a satisfactory fluorinating agent and may be reacted with various materials capable of forming fluorides, such as copper, iron, zinc, etc., with consequent formation of the metal fluoride and reduction of the plutonium to the form of a lower fluoride. In accordance with the present invention, it has been found that the reactivity of plutonium hexafluoride with other fluoridizable materials is so great that the process may be used as a method of separating plutonium from mixures containing plutonium hexafluoride and other vaporized fluorides even though the plutonium is present in but minute quantities. This process may be carried out by treating a mixture of fluoride vapors comprising plutonium hexafluoride and fluoride of uranium to selectively reduce the plutonium hexafluoride and convert it to a less volatile fluoride, and then recovering said less volatile fluoride from the vapor by condensation.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Essington, E.H.; Gilbert, R.O.; Wireman, D.L.
Blow-sand mounds or miniature sand dunes and mounds created by burrowing activities of animals were investigated by the Nevada Applied Ecology Group (NAEG) to determine the influence of mounds on plutonium, americium, and uranium distributions and inventories in areas of the Nevada Test Site and Tonopah Test Range. Those radioactive elements were added to the environment as a result of safety experiments of nuclear devices. Two studies were conducted. The first was to estimate the vertical distribution of americium in the blow-sand mounds and in the desert pavement surrounding the mounds. The second was to estimate the amount or concentrationmore » of the radioactive materials accumulated in the mound relative to the desert pavement. Five mound types were identified in which plutonium, americium, and uranium concentrations were measured: grass, shrub, complex, animal, and diffuse. The mount top (that portion above the surrounding land surface datum), the mound bottom (that portion below the mound to a depth of 5 cm below the surrounding land surface datum), and soil from the immediate area surrounding the mound were compared separately to determine if the radioactive elements had concentrated in the mounds. Results of the studies indicate that the mounds exhibit higher concentrations of plutonium, americium, and uranium than the immediate surrounding soil. The type of mound does not appear to have influenced the amount of the radioactive material found in the mound except for the animal mounds where the burrowing activities appear to have obliterated distribution patterns.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bouzigues, H.; Reneaud, J.-M.
1963-01-01
A method and a special apparatus are described which make it possible to detach the insoluble plutonium salt deposits in the extraction chain of an irradiated fuel treatment plant. The process chosen allows the detection, in the extraction batteries or in the highly active chemical engineering equipment, of plutonium quantities of a few grams. After four years operation it has been impossible to detect measurable quantities of plutonium in any part of the extraction chain. The results have been confirmed by visual examinations carried out with a specially constructed endoscope. (auth)
History of fast reactor fuel development
NASA Astrophysics Data System (ADS)
Kittel, J. H.; Frost, B. R. T.; Mustelier, J. P.; Bagley, K. Q.; Crittenden, G. C.; Van Dievoet, J.
1993-09-01
The first fast breeder reactors, constructed in the 1945-1960 time period, used metallic fuels composed of uranium, plutonium, or their alloys. They were chosen because most existing reactor operating experience had been obtained on metallic fuels and because they provided the highest breeding ratios. Difficulties in obtaining adequate dimensional stability in metallic fuel elements under conditions of high fuel burnup led in the 1960s to the virtual worldwide choice of ceramic fuels. Although ceramic fuels provide lower breeding performance, this objective is no longer an important consideration in most national programs. Mixed uranium and plutonium dioxide became the ceramic fuel that has received the widest use. The more advanced ceramic fuels, mixed uranium and plutonium carbides and nitrides, continue under development. More recently, metal fuel elements of improved design have joined ceramic fuels in achieving goal burnups of 15 to 20 percent. Low-swelling fuel cladding alloys have also been continuously developed to deal with the unexpected problem of void formation in stainless steels subjected to fast neutron irradiation, a phenomenon first observed in the 1960s.
Results of an inter-laboratory study of glass formulation for the immobilization of excess plutonium
DOE Office of Scientific and Technical Information (OSTI.GOV)
Peeler, D.K.
1999-12-08
The primary focus of the current study is to determine allowable loadings of feed streams containing different ratios of plutonium, uranium, and minor components into the LaBS glass and to evaluate thermal stability with respect to the DWPF pour.
A physical model for evaluating uranium nitride specific heat
NASA Astrophysics Data System (ADS)
Baranov, V. G.; Devyatko, Yu. N.; Tenishev, A. V.; Khlunov, A. V.; Khomyakov, O. V.
2013-03-01
Nitride fuel is one of perspective materials for the nuclear industry. But unlike the oxide and carbide uranium and mixed uranium-plutonium fuel, the nitride fuel is less studied. The present article is devoted to the development of a model for calculating UN specific heat on the basis of phonon spectrum data within the solid state theory.
METHOD OF SEPARATING PLUTONIUM FROM LANTHANUM FLUORIDE CARRIER
Watt, G.W.; Goeckermann, R.H.
1958-06-10
An improvement in oxidation-reduction type methods of separating plutoniunn from elements associated with it in a neutron-irradiated uranium solution is described. The method relates to the separating of plutonium from lanthanum ions in an aqueous 0.5 to 2.5 N nitric acid solution by 'treating the solution, at room temperature, with ammonium sulfite in an amount sufficient to reduce the hexavalent plutonium present to a lower valence state, and then treating the solution with H/sub 2/O/sub 2/ thereby forming a tetravalent plutonium peroxide precipitate.
77 FR 26149 - Access Authorization Fees
Federal Register 2010, 2011, 2012, 2013, 2014
2012-05-03
... Regulatory Affairs of OMB. List of Subjects 10 CFR Part 11 Hazardous materials--transportation... licensees for work performed under the Material Access Authorization Program (MAAP) and the Information... assigned duties which require access to special nuclear material (plutonium, uranium-233, and uranium...
Direct measurement of 235U in spent fuel rods with Gamma-ray mirrors
NASA Astrophysics Data System (ADS)
Ruz, J.; Brejnholt, N. F.; Alameda, J. B.; Decker, T. A.; Descalle, M. A.; Fernandez-Perea, M.; Hill, R. M.; Kisner, R. A.; Melin, A. M.; Patton, B. W.; Soufli, R.; Ziock, K.; Pivovaroff, M. J.
2015-03-01
Direct measurement of plutonium and uranium X-rays and gamma-rays is a highly desirable non-destructive analysis method for the use in reprocessing fuel environments. The high background and intense radiation from spent fuel make direct measurements difficult to implement since the relatively low activity of uranium and plutonium is masked by the high activity from fission products. To overcome this problem, we make use of a grazing incidence optic to selectively reflect Kα and Kβ fluorescence of Special Nuclear Materials (SNM) into a high-purity position-sensitive germanium detector and obtain their relative ratios.
NASA Astrophysics Data System (ADS)
Blandinskiy, V. Yu.
2014-12-01
This paper presents the results of a numerical investigation into burnup and breeding of nuclides in metallic fuel consisting of a mixture of plutonium and depleted uranium in a fast reactor with sodium coolant. The feasibility of using plutonium contained in spent nuclear fuel from domestic thermal reactors and weapons-grade plutonium is discussed. It is shown that the largest production of secondary fuel and the least change in the reactivity over the reactor lifetime can be achieved when employing plutonium contained in spent nuclear fuel from a reactor of the RBMK-1000 type.
IMPROVED PROCESS OF PLUTONIUM CARRIER PRECIPITATION
Faris, B.F.
1959-06-30
This patent relates to an improvement in the bismuth phosphate process for separating and recovering plutonium from neutron irradiated uranium, resulting in improved decontamination even without the use of scavenging precipitates in the by-product precipitation step and subsequently more complete recovery of the plutonium in the product precipitation step. This improvement is achieved by addition of fluomolybdic acid, or a water soluble fluomolybdate, such as the ammonium, sodium, or potassium salt thereof, to the aqueous nitric acid solution containing tetravalent plutonium ions and contaminating fission products, so as to establish a fluomolybdate ion concentration of about 0.05 M. The solution is then treated to form the bismuth phosphate plutonium carrying precipitate.
SEPARATION PROCESS USING COMPLEXING AND ADSORPTION
Spedding, J.H.; Ayers, J.A.
1958-06-01
An adsorption process is described for separating plutonium from a solution of neutron-irradiated uranium containing ions of a compound of plutonium and other cations. The method consists of forming a chelate complex compound with plutoniunn ions in the solution by adding a derivative of 8- hydroxyquinoline, which derivative contains a sulfonic acid group, and adsorbing the remaining cations from the solution on a cation exchange resin, while the complexed plutonium remains in the solution.
A CHEMICAL METHOD OF TREATING FISSIONABLE MATERIAL
Olson, C.M.
1959-09-01
One step of a process for separating plutonium from uranium and fission products is presented. A nitric acid solution containing these constituents is treated with formic acid to reduce simultaneously the plutonium to a valence state of not greater than +4 and destroy and eliminate the excess nitric acid.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Iseki, Tadahiro; Inaba, Makoto; Takahashi, Naoki
During the second and third steps of Active Test at Rokkasho Reprocessing Plant (RRP), the performances of the Separation Facility have been checked; (A) diluent washing efficiency, (B) plutonium stripping efficiency, (C) decontamination factor of fission products and (D) plutonium and uranium leakage into raffinate and spent solvent. Test results were equivalent to or better than expected. (authors)
Boulyga, S F; Becker, J S
2001-07-01
As a result of the accident at the Chernobyl nuclear power plant (NPP) the environment was contaminated with spent nuclear fuel. The 236U isotope was used in this study to monitor the spent uranium from nuclear fallout in soil samples collected in the vicinity of the Chernobyl NPP. Nuclear track radiography was applied for the identification and extraction of hot radioactive particles from soil samples. A rapid and sensitive analytical procedure was developed for uranium isotopic ratio measurement in environmental samples based on double-focusing inductively coupled plasma mass spectrometry (DF-ICP-MS) with a MicroMist nebulizer and a direct injection high-efficiency nebulizer (DIHEN). The performance of the DF-ICP-MS with a quartz DIHEN and plasma shielded torch was studied. Overall detection efficiencies of 4 x 10(-4) and 10(-3) counts per atom were achieved for 238U in DF-ICP-QMS with the MicroMist nebulizer and DIHEN, respectively. The rate of formation of uranium hydride ions UH+/U+ was 1.2 x 10(-4) and 1.4 x 10(-4), respectively. The precision of short-term measurements of uranium isotopic ratios (n = 5) in 1 microg L(-1) NBS U-020 standard solution was 0.11% (238U/235U) and 1.4% (236U/238U) using a MicroMist nebulizer and 0.25% (235U/238U) and 1.9% (236U/P38U) using a DIHEN. The isotopic composition of all investigated Chernobyl soil samples differed from those of natural uranium; i.e. in these samples the 236U/238U ratio ranged from 10(-5) to 10(-3). Results obtained with ICP-MS, alpha- and gamma-spectrometry showed differences in the migration properties of spent uranium, plutonium, and americium. The isotopic ratio of uranium was also measured in hot particles extracted from soil samples.
Significance of breeding in fast nuclear reactors
DOE Office of Scientific and Technical Information (OSTI.GOV)
Raza, S.M.; Abidi, S.B.M.
1983-12-01
Only breeder reactors--nuclear power plants that produce more fuel than they consume--are capable in principle of extracting the maximum amount of fission energy contained in uranium ore, thus offering a practical long-term solution to uranium supply problems. Uranium would then constitute a virtually inexhaustible fuel reserve for the world's future energy needs. The ultimate argument for breeding is to conserve the energy resources available to mankind. A long-term role for nuclear power with fast reactors is proven to be economically viable, environmentally acceptable and capable of wide scale exploitation in many countries. In this paper, various suggestions pertaining to themore » fuel fabrication route, fuel cycle economics, studies of the physics of fast nuclear reactors and of engineering design simplifications are presented. Fast reactors contain no moderator and inherently require enriched fuel. In general, the main aim is to suggest an improvement in the understanding of the safety and control characteristics of fast breeder power reactors. Development work is also being devoted to new carbide and nitride fuels, which are likely to exhibit breeding characteristics superior to those of the oxides of plutonium and uranium.« less
Assessment for advanced fuel cycle options in CANDU
DOE Office of Scientific and Technical Information (OSTI.GOV)
Morreale, A.C.; Luxat, J.C.; Friedlander, Y.
2013-07-01
The possible options for advanced fuel cycles in CANDU reactors including actinide burning options and thorium cycles were explored and are feasible options to increase the efficiency of uranium utilization and help close the fuel cycle. The actinide burning TRUMOX approach uses a mixed oxide fuel of reprocessed transuranic actinides from PWR spent fuel blended with natural uranium in the CANDU-900 reactor. This system reduced actinide content by 35% and decreased natural uranium consumption by 24% over a PWR once through cycle. The thorium cycles evaluated used two CANDU-900 units, a generator and a burner unit along with a drivermore » fuel feedstock. The driver fuels included plutonium reprocessed from PWR, from CANDU and low enriched uranium (LEU). All three cycles were effective options and reduced natural uranium consumption over a PWR once through cycle. The LEU driven system saw the largest reduction with a 94% savings while the plutonium driven cycles achieved 75% savings for PWR and 87% for CANDU. The high neutron economy, online fuelling and flexible compact fuel make the CANDU system an ideal reactor platform for many advanced fuel cycles.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Triay, I.R.; Cotter, C.R.; Kraus, S.M.
1996-08-01
We studied the retardation of actinides (neptunium, uranium, and plutonium) by sorption as a function of radionuclide concentration in water from Well J-13 and of tuffs from Yucca Mountain. Three major tuff types were examined: devitrified, vitric, and zeolitic. To identify the sorbing minerals in the tuffs, we conducted batch sorption experiments with pure mineral separates. These experiments were performed with water from Well J-13 (a sodium bicarbonate groundwater) under oxidizing conditions in the pH range from 7 to 8.5. The results indicate that all actinides studied sorb strongly to synthetic hematite and also that Np(V) and U(VI) do notmore » sorb appreciably to devitrified or vitric tuffs, albite, or quartz. The sorption of neptunium onto clinoptilolite-rich tuffs and pure clinoptilolite can be fitted with a sorption distribution coefficient in the concentration range from 1 X 10{sup -7} to 3 X 10{sup -5} M. The sorption of uranium onto clinoptilolite-rich tuffs and pure clinoptilolite is not linear in the concentration range from 8 X 10{sup -8} to 1 X 10{sup -4} M, and it can be fitted with nonlinear isotherm models (such as the Langmuir or the Freundlich Isotherms). The sorption of neptunium and uranium onto clinoptilolite in J-13 well water increases with decreasing pH in the range from 7 to 8.5. The sorption of plutonium (initially in the Pu(V) oxidation state) onto tuffs and pure mineral separates in J-13 well water at pH 7 is significant. Plutonium sorption decreases as a function of tuff type in the order: zeolitic > vitric > devitrified; and as a function of mineralogy in the order: hematite > clinoptilolite > albite > quartz.« less
LWR First Recycle of TRU with Thorium Oxide for Transmutation and Cross Sections
DOE Office of Scientific and Technical Information (OSTI.GOV)
Andrea Alfonsi; Gilles Youinou; Sonat Sen
2013-02-01
Thorium has been considered as an option to uranium-based fuel, based on considerations of resource utilization (thorium is approximately three times more plentiful than uranium) and as a result of concerns about proliferation and waste management (e.g. reduced production of plutonium, etc.). Since the average composition of natural Thorium is dominated (100%) by the fertile isotope Th-232, Thorium is only useful as a resource for breeding new fissile materials, in this case U-233. Consequently a certain amount of fissile material must be present at the start-up of the reactor in order to guarantee its operation. The thorium fuel can bemore » used in both once-through and recycle options, and in both fast and thermal spectrum systems. The present study has been aimed by the necessity of investigating the option of using reprocessed plutonium/TRU, from a once-through reference LEU scenario (50 GWd/ tIHM), mixed with natural thorium and the need of collect data (mass fractions, cross-sections etc.) for this particular fuel cycle scenario. As previously pointed out, the fissile plutonium is needed to guarantee the operation of the reactor. Four different scenarios have been considered: • Thorium – recycled Plutonium; • Thorium – recycled Plutonium/Neptunium; • Thorium – recycled Plutonium/Neptunium/Americium; • Thorium – recycled Transuranic. The calculations have been performed with SCALE6.1-TRITON.« less
LWR First Recycle of TRU with Thorium Oxide for Transmutation and Cross Sections
DOE Office of Scientific and Technical Information (OSTI.GOV)
Andrea Alfonsi; Gilles Youinou
2012-07-01
Thorium has been considered as an option to uranium-based fuel, based on considerations of resource utilization (thorium is approximately three times more plentiful than uranium) and as a result of concerns about proliferation and waste management (e.g. reduced production of plutonium, etc.). Since the average composition of natural Thorium is dominated (100%) by the fertile isotope Th-232, Thorium is only useful as a resource for breeding new fissile materials, in this case U-233. Consequently a certain amount of fissile material must be present at the start-up of the reactor in order to guarantee its operation. The thorium fuel can bemore » used in both once-through and recycle options, and in both fast and thermal spectrum systems. The present study has been aimed by the necessity of investigating the option of using reprocessed plutonium/TRU, from a once-through reference LEU scenario (50 GWd/ tIHM), mixed with natural thorium and the need of collect data (mass fractions, cross-sections etc.) for this particular fuel cycle scenario. As previously pointed out, the fissile plutonium is needed to guarantee the operation of the reactor. Four different scenarios have been considered: • Thorium – recycled Plutonium; • Thorium – recycled Plutonium/Neptunium; • Thorium – recycled Plutonium/Neptunium/Americium; • Thorium – recycled Transuranic. The calculations have been performed with SCALE6.1-TRITON.« less
Thompson, S.G.; Miller, D.R.; James, R.A.
1961-06-20
A process is described for precipitating Pu from an aqueous solution as the arsenate, either per se or on a bismuth arsenate carrier, whereby a separation from uranium and fission products, if present in solution, is accomplished.
On the use of thermal NF3 as the fluorination and oxidation agent in treatment of used nuclear fuels
NASA Astrophysics Data System (ADS)
Scheele, Randall; McNamara, Bruce; Casella, Andrew M.; Kozelisky, Anne
2012-05-01
This paper presents results of our investigation on the use of nitrogen trifluoride as a fluorination or fluorination/oxidation agent for separating valuable constituents from used nuclear fuels by exploiting the different volatilities of the constituent fission product and actinide fluorides. Our thermodynamic calculations show that nitrogen trifluoride has the potential to produce volatile fission product and actinide fluorides from oxides and metals that can form volatile fluorides. Simultaneous thermogravimetric and differential thermal analyses show that the oxides of lanthanum, cerium, rhodium, and plutonium are fluorinated but do not form volatile fluorides when treated with nitrogen trifluoride at temperatures up to 550 °C. However, depending on temperature, volatile fluorides or oxyfluorides can form from nitrogen trifluoride treatment of the oxides of niobium, molybdenum, ruthenium, tellurium, uranium, and neptunium. Thermoanalytical studies demonstrate near-quantitative separation of uranium from plutonium in a mixed 80% uranium and 20% plutonium oxide. Our studies of neat oxides and metals suggest that the reactivity of nitrogen trifluoride may be adjusted by temperature to selectively separate the major volatile fuel constituent uranium from minor volatile constituents, such as Mo, Tc, Ru and from the non-volatile fuel constituents based on differences in their reaction temperatures and kinetic behaviors. This reactivity is novel with respect to that reported for other fluorinating reagents F2, BrF5, ClF3.
METHODS OF PREPARATION OF ELEMENT 95
Seaborg, G.T.; James, R.A.
1962-07-17
A process of making americium by bombarding plutonium or uranium with neutrons or deuterons and aging the mass for decay of the plutonium formed to americium is described. The americium may then be separated by dissolving the mass in aqueous acid and carrier precipitation of the americium, especially on lanthanum or cerous fluoride. (AEC)
Beaufait, L.J. Jr.; Stevenson, F.R.; Rollefson, G.K.
1958-11-18
The recovery of plutonium ions from neutron irradiated uranium can be accomplished by bufferlng an aqueous solutlon of the irradiated materials containing tetravalent plutonium to a pH of 4 to 7, adding sufficient acetate to the solution to complex the uranyl present, adding ferric nitrate to form a colloid of ferric hydroxide, plutonlum, and associated fission products, removing and dissolving the colloid in aqueous nitric acid, oxldizlng the plutonium to the hexavalent state by adding permanganate or dichromate, treating the resultant solution with ferric nitrate to form a colloid of ferric hydroxide and associated fission products, and separating the colloid from the plutonlum left in solution.
Design and fabrication of 55-gallon drum shuffler standards
DOE Office of Scientific and Technical Information (OSTI.GOV)
Long, S.M.; Hsue, F.; Hoth, C.
1994-08-01
To analyze waste with varying levels of nuclear material, suitable standards are needed to calibrate analytical instrumentation. At the Los Alamos Plutonium Facility, the authors have designed and fabricated a single drum standard for a passive-active neutron counter (shuffler). The standard is modified simply by adding or subtracting plutonium of uranium cylinders to adapt to a range of nuclear material. The plutonium or uranium oxide was placed into small cylindrical containers (1-in. diameter by 5-in. long) and diluted with diatomaceous earth. The cylinders were welded closed and removed from the glove box environment without any external contamination. The containers weremore » leak tested and then placed on a segmented gamma scanner to assure homogeneous distribution of the nuclear material. The cylinders are now placed into the drum to achieve the needed ranges for calibration of the instruments.« less
PROCESS USING BISMUTH PHOSPHATE AS A CARRIER PRECIPITATE FOR FISSION PRODUCTS AND PLUTONIUM VALUES
Finzel, T.G.
1959-03-10
A process is described for separating plutonium from fission products carried therewith when plutonium in the reduced oxidation state is removed from a nitric acid solution of irradiated uranium by means of bismuth phosphate as a carrier precipitate. The bismuth phosphate carrier precipitate is dissolved by treatment with nitric acid and the plutonium therein is oxidized to the hexavalent oxidation state by means of potassium dichromate. Separation of the plutonium from the fission products is accomplished by again precipitating bismuth phosphate and removing the precipitate which now carries the fission products and a small percentage of the plutonium present. The amount of plutonium carried in this last step may be minimized by addition of sodium fluoride, so as to make the solution 0.03N in NaF, prior to the oxidation and prccipitation step.
NASA Astrophysics Data System (ADS)
Rim, Jung H.
Accurate and fast determination of the activity of radionuclides in a sample is critical for nuclear forensics and emergency response. Radioanalytical techniques are well established for radionuclides measurement, however, they are slow and labor intensive, requiring extensive radiochemical separations and purification prior to analysis. With these limitations of current methods, there is great interest for a new technique to rapidly process samples. This dissertation describes a new analyte extraction medium called Polymer Ligand Film (PLF) developed to rapidly extract radionuclides. Polymer Ligand Film is a polymer medium with ligands incorporated in its matrix that selectively and rapidly extract analytes from a solution. The main focus of the new technique is to shorten and simplify the procedure necessary to chemically isolate radionuclides for determination by alpha spectrometry or beta counting. Five different ligands were tested for plutonium extraction: bis(2-ethylhexyl) methanediphosphonic acid (H2DEH[MDP]), di(2-ethyl hexyl) phosphoric acid (HDEHP), trialkyl methylammonium chloride (Aliquat-336), 4,4'(5')-di-t-butylcyclohexano 18-crown-6 (DtBuCH18C6), and 2-ethylhexyl 2-ethylhexylphosphonic acid (HEH[EHP]). The ligands that were effective for plutonium extraction further studied for uranium extraction. The plutonium recovery by PLFs has shown dependency on nitric acid concentration and ligand to total mass ratio. H2DEH[MDP] PLFs performed best with 1:10 and 1:20 ratio PLFs. 50.44% and 47.61% of plutonium were extracted on the surface of PLFs with 1M nitric acid for 1:10 and 1:20 PLF, respectively. HDEHP PLF provided the best combination of alpha spectroscopy resolution and plutonium recovery with 1:5 PLF when used with 0.1M nitric acid. The overall analyte recovery was lower than electrodeposited samples, which typically has recovery above 80%. However, PLF is designed to be a rapid field deployable screening technique and consistency is more important than recovery. PLFs were also tested using blind quality control samples and the activities were accurately measured. It is important to point out that PLFs were consistently susceptible to analytes penetrating and depositing below the surface. The internal radiation within the body of PLF is mostly contained and did not cause excessive self-attenuation and peak broadening in alpha spectroscopy. The analyte penetration issue was beneficial in the destructive analysis. H2DEH[MDP] PLF was tested with environmental samples to fully understand the capabilities and limitations of the PLF in relevant environments. The extraction system was very effective in extracting plutonium from environmental water collected from Mortandad Canyon at Los Alamos National Laboratory with minimal sample processing. Soil samples were tougher to process than the water samples. Analytes were first leached from the soil matrixes using nitric acid before processing with PLF. This approach had a limitation in extracting plutonium using PLF. The soil samples from Mortandad Canyon, which are about 1% iron by weight, were effectively processed with the PLF system. Even with certain limitations of the PLF extraction system, this technique was able to considerably decrease the sample analysis time. The entire environmental sample was analyzed within one to two days. The decrease in time can be attributed to the fact that PLF is replacing column chromatography and electrodeposition with a single step for preparing alpha spectrometry samples. The two-step process of column chromatography and electrodeposition takes a couple days to a week to complete depending on the sample. The decrease in time and the simplified procedure make this technique a unique solution for application to nuclear forensics and emergency response. A large number of samples can be quickly analyzed and selective samples can be further analyzed with more sensitive techniques based on the initial data. The deployment of a PLF system as a screening method will greatly reduce a total analysis time required to gain meaningful isotopic data for the nuclear forensics application. (Abstract shortened by UMI.)
Tomczuk, Zygmunt; Miller, William E.; Wolson, Raymond D.; Gay, Eddie C.
1991-01-01
An electrochemical process and apparatus for the recovery of uranium and plutonium from spent metal clad fuel pins is disclosed. The process uses secondary reactions between U.sup.+4 cations and elemental uranium at the anode to increase reaction rates and improve anodic efficiency compared to prior art processes. In another embodiment of the process, secondary reactions between Cd.sup.+2 cations and elemental uranium to form uranium cations and elemental cadmium also assists in oxidizing the uranium at the anode.
Measurement of actinides and strontium-90 in high activity waste
DOE Office of Scientific and Technical Information (OSTI.GOV)
Maxwell, S.L. III; Nelson, M.R.
1994-08-01
The reliable measurement of trace radionuclides in high activity waste is important to support waste processing activities at SRS (F and H Area Waste Tanks, Extended Sludge Processing (ESP) and In-Tank precipitation (ITP) processing). Separation techniques are needed to remove high levels of gamma activity and alpha/beta interferences prior to analytical measurement. Using new extraction chromatographic resins from EiChrom Industries, Inc., the SRS Central Laboratory has developed new high speed separation methods that enable measurement of neptunium, thorium, uranium, plutonium, americium and strontium-90 in high activity waste solutions. Small particle size resin and applied vacuum are used to reduce analysismore » times and enhance column performance. Extraction chromatographic resins are easy to use and eliminate the generation of contaminated liquid organic waste.« less
2012-09-01
patrol vehicles. The Department’s Counter-Terror Operations Unit serves as the program coordinator and as the archetypical NIMS Type I Team. The...is defined by Title I of the Atomic Energy Act of 1954 as plutonium, uranium-233, or uranium enriched in the isotopes uranium-233 or uranium...end of World War II. Radioactive Materials—materials that contain radioactive atoms . Radioactive atoms are unstable; that is, they have too much
10 CFR 150.11 - Critical mass.
Code of Federal Regulations, 2013 CFR
2013-01-01
... uranium enriched in the isotope U-235 in quantities not exceeding 350 grams of contained U-235; uranium-233 in quantities not exceeding 200 grams; plutonium in quantities not exceeding 200 grams; or any... not exceed the limitation and are within the formula, as follows: (175 (grams contained U-235/350)+(50...
10 CFR 150.11 - Critical mass.
Code of Federal Regulations, 2011 CFR
2011-01-01
... uranium enriched in the isotope U-235 in quantities not exceeding 350 grams of contained U-235; uranium-233 in quantities not exceeding 200 grams; plutonium in quantities not exceeding 200 grams; or any... not exceed the limitation and are within the formula, as follows: (175 (grams contained U-235/350)+(50...
10 CFR 150.11 - Critical mass.
Code of Federal Regulations, 2010 CFR
2010-01-01
... uranium enriched in the isotope U-235 in quantities not exceeding 350 grams of contained U-235; uranium-233 in quantities not exceeding 200 grams; plutonium in quantities not exceeding 200 grams; or any... not exceed the limitation and are within the formula, as follows: (175 (grams contained U-235/350)+(50...
10 CFR 150.11 - Critical mass.
Code of Federal Regulations, 2014 CFR
2014-01-01
... uranium enriched in the isotope U-235 in quantities not exceeding 350 grams of contained U-235; uranium-233 in quantities not exceeding 200 grams; plutonium in quantities not exceeding 200 grams; or any... not exceed the limitation and are within the formula, as follows: (175 (grams contained U-235/350)+(50...
10 CFR 150.11 - Critical mass.
Code of Federal Regulations, 2012 CFR
2012-01-01
... uranium enriched in the isotope U-235 in quantities not exceeding 350 grams of contained U-235; uranium-233 in quantities not exceeding 200 grams; plutonium in quantities not exceeding 200 grams; or any... not exceed the limitation and are within the formula, as follows: (175 (grams contained U-235/350)+(50...
Extracting metals directly from metal oxides
Wai, Chien M.; Smart, Neil G.; Phelps, Cindy
1997-01-01
A method of extracting metals directly from metal oxides by exposing the oxide to a supercritical fluid solvent containing a chelating agent is described. Preferably, the metal is an actinide or a lanthanide. More preferably, the metal is uranium, thorium or plutonium. The chelating agent forms chelates that are soluble in the supercritical fluid, thereby allowing direct removal of the metal from the metal oxide. In preferred embodiments, the extraction solvent is supercritical carbon dioxide and the chelating agent is selected from the group consisting of .beta.-diketones, halogenated .beta.-diketones, phosphinic acids, halogenated phosphinic acids, carboxylic acids, halogenated carboxylic acids, and mixtures thereof. In especially preferred embodiments, at least one of the chelating agents is fluorinated. The method provides an environmentally benign process for removing metals from metal oxides without using acids or biologically harmful solvents. The chelate and supercritical fluid can be regenerated, and the metal recovered, to provide an economic, efficient process.
Extracting metals directly from metal oxides
Wai, C.M.; Smart, N.G.; Phelps, C.
1997-02-25
A method of extracting metals directly from metal oxides by exposing the oxide to a supercritical fluid solvent containing a chelating agent is described. Preferably, the metal is an actinide or a lanthanide. More preferably, the metal is uranium, thorium or plutonium. The chelating agent forms chelates that are soluble in the supercritical fluid, thereby allowing direct removal of the metal from the metal oxide. In preferred embodiments, the extraction solvent is supercritical carbon dioxide and the chelating agent is selected from the group consisting of {beta}-diketones, halogenated {beta}-diketones, phosphinic acids, halogenated phosphinic acids, carboxylic acids, halogenated carboxylic acids, and mixtures thereof. In especially preferred embodiments, at least one of the chelating agents is fluorinated. The method provides an environmentally benign process for removing metals from metal oxides without using acids or biologically harmful solvents. The chelate and supercritical fluid can be regenerated, and the metal recovered, to provide an economic, efficient process. 4 figs.
Zaitsev, Boris N.; Esimantovskiy, Vyacheslav M.; Lazarev, Leonard N.; Dzekun, Evgeniy G.; Romanovskiy, Valeriy N.; Todd, Terry A.; Brewer, Ken N.; Herbst, Ronald S.; Law, Jack D.
2001-01-01
Cesium and strontium are extracted from aqueous acidic radioactive waste containing rare earth elements, technetium and actinides, by contacting the waste with a composition of a complex organoboron compound and polyethylene glycol in an organofluorine diluent mixture. In a preferred embodiment the complex organoboron compound is chlorinated cobalt dicarbollide, the polyethylene glycol has the formula RC.sub.6 H.sub.4 (OCH.sub.2 CH.sub.2).sub.n OH, and the organofluorine diluent is a mixture of bis-tetrafluoropropyl ether of diethylene glycol with at least one of bis-tetrafluoropropyl ether of ethylene glycol and bis-tetrafluoropropyl formal. The rare earths, technetium and the actinides (especially uranium, plutonium and americium), are extracted from the aqueous phase using a phosphine oxide in a hydrocarbon diluent, and reextracted from the resulting organic phase into an aqueous phase by using a suitable strip reagent.
Solubility testing of actinides on breathing-zone and area air samples
NASA Astrophysics Data System (ADS)
Metzger, Robert Lawrence
The solubility of inhaled radionuclides in the human lung is an important characteristic of the compounds needed to perform internal dosimetry assessments for exposed workers. A solubility testing method for uranium and several common actinides has been developed with sufficient sensitivity to allow profiles to be determined from routine breathing zone and area air samples in the workplace. Air samples are covered with a clean filter to form a filter-sample-filter sandwich which is immersed in an extracellular lung serum simulant solution. The sample is moved to a fresh beaker of the lung fluid simulant each day for one week, and then weekly until the end of the 28 day test period. The soak solutions are wet ashed with nitric acid and hydrogen peroxide to destroy the organic components of the lung simulant solution prior to extraction of the nuclides of interest directly into an extractive scintillator for subsequent counting on a Photon-Electron Rejecting Alpha Liquid Scintillation (PERALSsp°ler ) spectrometer. Solvent extraction methods utilizing the extractive scintillators have been developed for the isotopes of uranium, plutonium, and curium. The procedures normally produce an isotopic recovery greater than 95% and have been used to develop solubility profiles from air samples with 40 pCi or less of Usb3Osb8. This makes it possible to characterize solubility profiles in every section of operating facilities where airborne nuclides are found using common breathing zone air samples. The new method was evaluated by analyzing uranium compounds from two uranium mills whose product had been previously analyzed by in vitro solubility testing in the laboratory and in vivo solubility testing in rodents. The new technique compared well with the in vivo rodent solubility profiles. The method was then used to evaluate the solubility profiles in all process sections of an operating in situ uranium plant using breathing zone and area air samples collected during routine plant operations. The solubility profiles developed from this work showed excellent agreement with the results of the worker urine bioassay program at the plant and identified a significant error in existing internal dose assessments at this facility.
Stabilization and immobilization of military plutonium: A non-proliferation perspective
DOE Office of Scientific and Technical Information (OSTI.GOV)
Leventhal, P.
1996-05-01
The Nuclear Control Institute welcomes this DOE-sponsored technical workshop on stabilization and immobilization of weapons plutonium (W Pu) because of the significant contribution it can make toward the ultimate non-proliferation objective of eliminating weapons-usable nuclear material, plutonium and highly enriched uranium (HEU), from world commerce. The risk of theft or diversion of these materials warrants concern, as only a few kilograms in the hands of terrorists or threshold states would give them the capability to build nuclear weapons. Military plutonium disposition questions cannot be addressed in isolation from civilian plutonium issues. The National Academy of Sciences has urged that {open_quotes}furthermore » steps should be taken to reduce the proliferation risks posed by all of the world`s plutonium stocks, military and civilian, separated and unseparated...{close_quotes}. This report discusses vitrification and a mixed oxide fuels option, and the effects of disposition choices on civilian plutonium fuel cycles.« less
METHOD OF RECOVERING PLUTONIUM VALUES FROM AQUEOUS SOLUTIONS BY CARRIER PRECIPITATION
James, R.A.; Thompson, S.G.
1959-11-01
A process is presented for pretreating aqueous nitric acid- plutonium solutions containing a small quantity of hydrazine that has formed as a decomposition product during the dissolution of neutron-bombarded uranium in nitric acid and that impairs the precipitation of plutonium on bismuth phosphate. The solution is digested with alkali metal dichromate or potassium permanganate at between 75 and 100 deg C; sulfuric acid at approximately 75 deg C and sodium nitrate, oxaiic acid plus manganous nitrate, or hydroxylamine are added to the solution to secure the plutonium in the tetravalent state and make it suitable for precipitation on BiPO/sub 4/.
Analysis of the 2H-evaporator scale samples (HTF-17-56, -57)
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hay, M.; Coleman, C.; Diprete, D.
Savannah River National Laboratory analyzed scale samples from both the wall and cone sections of the 242-16H Evaporator prior to chemical cleaning. The samples were analyzed for uranium and plutonium isotopes required for a Nuclear Criticality Safety Assessment of the scale removal process. The analysis of the scale samples found the material to contain crystalline nitrated cancrinite and clarkeite. Samples from both the wall and cone contain depleted uranium. Uranium concentrations of 16.8 wt% 4.76 wt% were measured in the wall and cone samples, respectively. The ratio of plutonium isotopes in both samples is ~85% Pu-239 and ~15% Pu-238 bymore » mass and shows approximately the same 3.5 times higher concentration in the wall sample versus the cone sample as observed in the uranium concentrations. The mercury concentrations measured in the scale samples were higher than previously reported values. The wall sample contains 19.4 wt% mercury and the cone scale sample 11.4 wt% mercury. The results from the current scales samples show reasonable agreement with previous 242-16H Evaporator scale sample analysis; however, the uranium concentration in the current wall sample is substantially higher than previous measurements.« less
Device for providing high-intensity ion or electron beam
McClanahan, Edwin D.; Moss, Ronald W.
1977-01-01
A thin film of a low-thermionic-work-function material is maintained on the cathode of a device for producing a high-current, low-pressure gas discharge by means of sputter deposition from an auxiliary electrode. The auxiliary electrode includes a surface with a low-work-function material, such as thorium, uranium, plutonium or one of the rare earth elements, facing the cathode but at a disposition and electrical potential so as to extract ions from the gas discharge and sputter the low-work-function material onto the cathode. By continuously replenishing the cathode film, high thermionic emissions and ion plasmas can be realized and maintained over extended operating periods.
Fabrication of thorium bearing carbide fuels
Gutierrez, Rueben L.; Herbst, Richard J.; Johnson, Karl W. R.
1981-01-01
Thorium-uranium carbide and thorium-plutonium carbide fuel pellets have been fabricated by the carbothermic reduction process. Temperatures of 1750.degree. C. and 2000.degree. C. were used during the reduction cycle. Sintering temperatures of 1800.degree. C. and 2000.degree. C. were used to prepare fuel pellet densities of 87% and >94% of theoretical, respectively. The process allows the fabrication of kilogram quantities of fuel with good reproducibility of chemicals and phase composition. Methods employing liquid techniques that form carbide microspheres or alloying-techniques which form alloys of thorium-uranium or thorium-plutonium suffer from limitation on the quantities processed of because of criticality concerns and lack of precise control of process conditions, respectively.
Seaborg, G.T.
1961-08-01
A process is described for extracting tetravalent plutonium from an aqueous acid solution with methyl ethyl ketone, methyl isobutyl ketone, or acetophenone and with the extraction of either tetravalent or hexavalent plutonium into menthone. (AEC)
SOLVENT EXTRACTION PROCESS FOR PLUTONIUM
Seaborg, G.T.
1959-04-14
The separation of plutonium from aqueous inorganic acid solutions by the use of a water immiscible organic extractant liquid is described. The plutonium must be in the oxidized state, and the solvents covered by the patent include nitromethane, nitroethane, nitropropane, and nitrobenzene. The use of a salting out agents such as ammonium nitrate in the case of an aqueous nitric acid solution is advantageous. After contacting the aqueous solution with the organic extractant, the resulting extract and raffinate phases are separated. The plutonium may be recovered by any suitable method.
THE ATTRACTIVENESS OF MATERIAS ASSOCIATED WITH THORIUM-BASED NUCLEAR FUEL CYCLES FOR PHWRS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Prichard, Andrew W.; Niehus, Mark T.; Collins, Brian A.
2011-07-17
This paper reports the continued evaluation of the attractiveness of materials mixtures containing special nuclear materials (SNM) associated with thorium based nuclear fuel cycles. Specifically, this paper examines a thorium fuel cycle in which a pressurized heavy water reactor (PHWR) is fueled with mixtures of natural uranium/233U/thorium. This paper uses a PHWR fueled with natural uranium as a base fuel cycle, and then compares material attractiveness of fuel cycles that use 233U/thorium salted with natural uranium. The results include the material attractiveness of fuel at beginning of life (BoL), end of life (EoL), and the number of fuel assemblies requiredmore » to collect a bare critical mass of plutonium or uranium. This study indicates what is required to render the uranium as having low utility for use in nuclear weapons; in addition, this study estimates the increased number of assemblies required to accumulate a bare critical mass of plutonium that has a higher utility for use in nuclear weapons. This approach identifies that some fuel cycles may be easier to implement the International Atomic Energy Agency (IAEA) safeguards approach and have a more effective safeguards by design outcome. For this study, approximately one year of fuel is required to be reprocessed to obtain one bare critical mass of plutonium. Nevertheless, the result of this paper suggests that all spent fuel needs to be rigorously safeguarded and provided with high levels of physical protection. This study was performed at the request of the United States Department of Energy /National Nuclear Security Administration (DOE/NNSA). The methodology and key findings will be presented.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Eller, P. G.; Stakebake, J. L.; Cooper, T. D.
2001-01-01
This paper evaluates potential analytical bias in application of the Loss on Ignition (LOI) technique for moisture measurement to relatively pure (plutonium assay of 80 wt.% or higher) oxides containing uranium that have been stabilized according to stabilization and storage standard DOE-STD-3013-2000 (STD-3013). An immediate application is to Rocky Flats (RF) materials derived from highgrade metal hydriding separations subsequently treated by multiple calcination cycles. Specifically evaluated are weight changes due to oxidatiodreduction of multivalent impurity oxides that could mask true moisture equivalent content measurement. Process knowledge and characterization of materials representing complex-wide materials to be stabilized and packaged according tomore » STD-3013, and particularly for the immediate RF target stream, indicate that oxides of uranium, iron and gallium are the only potential multivalent constituents expected to be present above 0.5 wt.%. The evaluation shows that of these constituents, with few exceptions, only uranium oxides can be present at a sufficient level to produce weight gain biases significant with respect to the LO1 stability test. In general, these formerly high-value, high-actinide content materials are reliably identifiable by process knowledge and measurement. Si&icant bias also requires that UO1 components remain largely unoxidized after calcination and are largely converted to U30s clsning LO1 testing at only slightly higher temperatures. Based on wellestablished literature, it is judged unlikely that this set of conditions will be realized in practice. We conclude that it is very likely that LO1 weight gain bias will be small for the immediate target RF oxide materials containing greater than 80 wt.% plutonium plus a much smaller uranium content. Recommended tests are in progress to confum these expectations and to provide a more authoritative basis for bounding LO1 oxidatiodreduction biases. LO1 bias evaluation is more difficult for lower purity materials and for fuel-type uranium-plutonium oxides. However, even in these cases testing may show that bias effects are manageable.« less
3. VIEW OF THE DEPRESSION PIT IN ROOM 103, IN ...
3. VIEW OF THE DEPRESSION PIT IN ROOM 103, IN 1965, WHEREIN FISSILE SOLUTION WAS STORED. THIS PHOTOGRAPH SHOWS THE URANIUM SOLUTION TANKS ON THE LEFT AND THE PLUTONIUM SYSTEM ON THE RIGHT. NO PLUTONIUM SOLUTION WAS EVER STORED IN BUILDING 886. - Rocky Flats Plant, Critical Mass Laboratory, Intersection of Central Avenue & 86 Drive, Golden, Jefferson County, CO
Coffinberry, A.S.; Schonfeld, F.W.
1959-09-01
Pu-U-Fe and Pu-U-Co alloys suitable for use as fuel elements tn fast breeder reactors are described. The advantages of these alloys are ease of fabrication without microcracks, good corrosion restatance, and good resistance to radiation damage. These advantages are secured by limitation of the zeta phase of plutonium in favor of a tetragonal crystal structure of the U/sub 6/Mn type.
10 CFR 20.2206 - Reports of individual monitoring.
Code of Federal Regulations, 2010 CFR
2010-01-01
... Energy NUCLEAR REGULATORY COMMISSION STANDARDS FOR PROTECTION AGAINST RADIATION Reports § 20.2206 Reports...) Operate a nuclear reactor designed to produce electrical or heat energy pursuant to § 50.21(b) or § 50.22... nuclear material in a quantity exceeding 5,000 grams of contained uranium-235, uranium-233, or plutonium...
10 CFR 20.2206 - Reports of individual monitoring.
Code of Federal Regulations, 2012 CFR
2012-01-01
... Energy NUCLEAR REGULATORY COMMISSION STANDARDS FOR PROTECTION AGAINST RADIATION Reports § 20.2206 Reports...) Operate a nuclear reactor designed to produce electrical or heat energy pursuant to § 50.21(b) or § 50.22... nuclear material in a quantity exceeding 5,000 grams of contained uranium-235, uranium-233, or plutonium...
10 CFR 20.2206 - Reports of individual monitoring.
Code of Federal Regulations, 2014 CFR
2014-01-01
... Energy NUCLEAR REGULATORY COMMISSION STANDARDS FOR PROTECTION AGAINST RADIATION Reports § 20.2206 Reports...) Operate a nuclear reactor designed to produce electrical or heat energy pursuant to § 50.21(b) or § 50.22... nuclear material in a quantity exceeding 5,000 grams of contained uranium-235, uranium-233, or plutonium...
13. VIEW OF THE MOLTEN SALT EXTRACTION LINE. THE MOLTEN ...
13. VIEW OF THE MOLTEN SALT EXTRACTION LINE. THE MOLTEN SALT EXTRACTION PROCESS WAS USED TO PURIFY PLUTONIUM BY REMOVING AMERICIUM, A DECAY BY-PRODUCT OF PLUTONIUM. (1/98) - Rocky Flats Plant, Plutonium Fabrication, Central section of Plant, Golden, Jefferson County, CO
1969-12-01
a five-year supply of enriched uranium for reactor fuel . Nevertheless, it seems clear that some foreign enrichment developments are approaching a...produc- tion of fissile material could powerfully influence the assessment of risks and benefits of a nuclear weapons development program . Since... program is likely to include the production of its own relatively pure fissile plutonium. This would involve more rapid cycling and reprocessing of fuel
Limiting Regret: Building the Army We Will Need
2015-08-18
Recently, U.S. and Chinese experts have estimated that the North Koreans may be able to produce enough fissionable plutonium and uranium to build up...long-range missiles, but their recently revealed ability to separate uranium could give them the ability to build gun-assembled fission weapons similar...weapons programs and living up to their international obligations.” 36North Korea has had a uranium enrichment capacity since at least November 2010
Thermal Stress in HFEF Hot Cell Windows Due to an In-Cell Metal Fire
Solbrig, Charles W.; Warmann, Stephen A.
2016-01-01
This work investigates an accident during the pyrochemical extraction of Uranium and Plutonium from PWR spent fuel in an argon atmosphere hot cell. In the accident, the heavy metals (U and Pu) being extracted are accidentally exposed to air from a leaky instrument penetration which goes through the cell walls. The extracted pin size pieces of U and Pu metal readily burn when exposed to air. Technicians perform the electrochemical extraction using manipulators through a 4 foot thick hot cell concrete wall which protects them from the radioactivity of the spent fuel. Four foot thick windows placed in the wallmore » allow the technicians to visually control the manipulators. These windows would be exposed to the heat of the metal fire. As a result, this analysis determines if the thermal stress caused by the fire would crack the windows and if the heat would degrade the window seals allowing radioactivity to escape from the cell.« less
Thermal Stress in HFEF Hot Cell Windows Due to an In-Cell Metal Fire
DOE Office of Scientific and Technical Information (OSTI.GOV)
Solbrig, Charles W.; Warmann, Stephen A.
This work investigates an accident during the pyrochemical extraction of Uranium and Plutonium from PWR spent fuel in an argon atmosphere hot cell. In the accident, the heavy metals (U and Pu) being extracted are accidentally exposed to air from a leaky instrument penetration which goes through the cell walls. The extracted pin size pieces of U and Pu metal readily burn when exposed to air. Technicians perform the electrochemical extraction using manipulators through a 4 foot thick hot cell concrete wall which protects them from the radioactivity of the spent fuel. Four foot thick windows placed in the wallmore » allow the technicians to visually control the manipulators. These windows would be exposed to the heat of the metal fire. As a result, this analysis determines if the thermal stress caused by the fire would crack the windows and if the heat would degrade the window seals allowing radioactivity to escape from the cell.« less
NASA Astrophysics Data System (ADS)
Degueldre, C.; Martin, M.; Kuri, G.; Grolimund, D.; Borca, C.
2011-09-01
Plutonium-uranium mixed oxide (MOX) fuels are currently used in nuclear reactors. The potential differences of metal redox state and microstructural developments of the matrix before and after irradiation are commonly analysed by electron probe microanalysis. In this work the structure and next-neighbor atomic environments of Pu and U oxide features within unirradiated homogeneous MOX and irradiated (60 MW d kg -1) MOX samples was analysed by micro-X-ray fluorescence (μ-XRF), micro-X-ray diffraction (μ-XRD) and micro-X-ray absorption fine structure (μ-XAFS) spectroscopy. The grain properties, chemical bonding, valences and stoichiometry of Pu and U are determined from the experimental data gained for the unirradiated as well as for irradiated fuel material examined in the center of the fuel as well as in its peripheral zone (rim). The formation of sub-grains is observed as well as their development from the center to the rim (polygonization). In the irradiated sample Pu remains tetravalent (>95%) and no (<5%) Pu(V) or Pu(VI) can be detected while the fuel could undergo slight oxidation in the rim zone. Any slight potential plutonium oxidation is buffered by the uranium dioxide matrix while locally fuel cladding interaction could also affect the redox of the fuel.
NASA Astrophysics Data System (ADS)
Clief Pattipawaej, Sandro; Su'ud, Zaki
2017-01-01
A preliminary design study of GFR with helium gas-cooled has been performed. In this study used natural uranium and plutonium results LWR waste as fuel. Fuel with a small percentage of plutonium are arranged on the inside of the core area, and the fuel with a greater percentage set on the outside of the core area. The configuration of such fuel is deliberately set to increase breeding in this part of the central core and reduce the leakage of neutrons on the outer side of the core, in order to get long-lived reactor with a small reactivity. Configuration of fuel as it is also useful to generate a peak power reactors with relatively low in both the direction of axial or radial. Optimization has been done to fuel fraction 45.0% was found that the reactor may be operating in more than 10 year time with excess reactivity less than 1%.
4. VIEW OF ROOM 103 IN 1980. SIX OF THE ...
4. VIEW OF ROOM 103 IN 1980. SIX OF THE NINE URANIUM NITRATE STORAGE TANKS ARE SHOWN. HIGHLY ENRICHED URANIUM WAS INTRODUCED INTO THE BUILDING IN THE SUMMER OF 1965 AND THE FIRST EXPERIMENTS WERE PERFORMED IN SEPTEMBER OF 1965. EXPERIMENTS WERE PERFORMED ON ENRICHED URANIUM METAL AND SOLUTION, PLUTONIUM METAL, LOW ENRICHED URANIUM OXIDE, AND SEVERAL SPECIAL APPLICATIONS. AFTER 1983, EXPERIMENTS WERE CONDUCTED PRIMARILY WITH URANYL NITRATE SOLUTIONS, AND DID NOT INVOLVE SOLID MATERIALS. - Rocky Flats Plant, Critical Mass Laboratory, Intersection of Central Avenue & 86 Drive, Golden, Jefferson County, CO
Method of Making Uranium Dioxide Bodies
Wilhelm, H. A.; McClusky, J. K.
1973-09-25
Sintered uranium dioxide bodies having controlled density are produced from U.sub.3 O.sub.8 and carbon by varying the mole ratio of carbon to U.sub.3 O.sub.8 in the mixture, which is compressed and sintered in a neutral or slightly oxidizing atmosphere to form dense slightly hyperstoichiometric uranium dioxide bodies. If the bodies are to be used as nuclear reactor fuel, they are subsequently heated in a hydrogen atmosphere to achieve stoichiometry. This method can also be used to produce fuel elements of uranium dioxide -- plutonium dioxide having controlled density.
Industrial safety and applied health physics. Annual report for 1980
DOE Office of Scientific and Technical Information (OSTI.GOV)
Not Available
1981-11-01
Information is reported in sections entitled: radiation monitoring; Environmental Management Program; radiation and safety surveys; industrial safety and special projects; Office of Operational Safety; and training, lectures, publications, and professional activities. There were no external or internal exposures to personnel which exceeded the standards for radiation protection as defined in DOE Manual Chapter 0524. Only 35 employees received whole body dose equivalents of 10 mSv (1 rem) or greater. There were no releases of gaseous waste from the Laboratory which were of a level that required an incident report to DOE. There were no releases of liquid radioactive waste frommore » the Laboratory which were of a level that required an incident report to DOE. The quantity of those radionuclides of primary concern in the Clinch River, based on the concentration measured at White Oak Dam and the dilution afforded by the Clinch River, averaged 0.16 percent of the concentration guide. The average background level at the Perimeter Air Monitoring (PAM) stations during 1980 was 9.0 ..mu..rad/h (0.090 ..mu..Gy/h). Soil samples were collected at all perimeter and remote monitoring stations and analyzed for eleven radionuclides including plutonium and uranium. Plutonium-239 content ranged from 0.37 Bq/kg (0.01 pCi/g) to 1.5 Bq/kg (0.04 pCi/g), and the uranium-235 content ranged from 0.7 Bq/kg (0.02 pCi/g) to 16 Bq/kg (0.43 pCi/g). Grass samples were collected at all perimeter and remote monitoring stations and analyzed for twelve radionuclides including plutonium and uranium. Plutonium-239 content ranged from 0.04 Bq/kg (0.001 pCi/g) to 0.07 Bq/kg (0.002 pCi/g), and the uranium-235 content ranged from 0.37 Bq/kg (0.01 pCi/g) to 12 Bq/kg (0.33 pCi/g).« less
EXAFS/XANES studies of plutonium-loaded sodalite/glass waste forms
NASA Astrophysics Data System (ADS)
Richmann, Michael K.; Reed, Donald T.; Kropf, A. Jeremy; Aase, Scott B.; Lewis, Michele A.
2001-09-01
A sodalite/glass ceramic waste form is being developed to immobilize highly radioactive nuclear wastes in chloride form, as part of an electrochemical cleanup process. Two types of simulated waste forms were studied: where the plutonium was alone in an LiCl/KCl matrix and where simulated fission-product elements were added representative of the electrometallurgical treatment process used to recover uranium from spent nuclear fuel also containing plutonium and a variety of fission products. Extended X-ray absorption fine structure spectroscopy (EXAFS) and X-ray absorption near-edge spectroscopy (XANES) studies were performed to determine the location, oxidation state, and particle size of the plutonium within these waste form samples. Plutonium was found to segregate as plutonium(IV) oxide with a crystallite size of at least 4.8 nm in the non-fission-element case and 1.3 nm with fission elements present. No plutonium was observed within the sodalite in the waste form made from the plutonium-loaded LiCl/KCl eutectic salt. Up to 35% of the plutonium in the waste form made from the plutonium-loaded simulated fission-product salt may be segregated with a heavy-element nearest neighbor other than plutonium or occluded internally within the sodalite lattice.
SEPARATION OF PLUTONIUM FROM LANTHANUM BY CHELATION-EXTRACTION
James, R.A.; Thompson, S.G.
1958-12-01
Plutonium can be separated from a mixture of plutonlum and lanthanum in which the lanthanum to plutonium molal ratio ls at least five by adding the ammonium salt of N-nitrosoarylhydroxylamine to an aqueous solution having a pH between about 3 and 0.2 and containing the plutonium in a valence state of at least +3, to form a plutonium chelate compound of N-nitrosoarylhydroxylamine. The plutonium chelate compound may be recovered from the solution by extracting with an immiscible organic solvent such as chloroform.
2015-06-01
Research Committee nm Nanometer Np Neptunium NPT Treaty of Non-proliferation of Nuclear Weapons ns Nanosecond ps Picosecond Pu Plutonium RIMS...discovery—credited also to Fritz Strassman— scientists realized these reactions also emitted secondary neutrons . These secondary neutrons could in...destructive capabilities of nuclear fission and atomic weapons . Figure 1. Uranium-235 Fission chain reaction, from [1
11. VIEW OF A SITE RETURN WEAPONS COMPONENT. SITE RETURNS ...
11. VIEW OF A SITE RETURN WEAPONS COMPONENT. SITE RETURNS WERE NUCLEAR WEAPONS SHIPPED TO THE ROCKY FLATS PLANT FROM THE NUCLEAR WEAPON STOCKPILE FOR RETIREMENT, TESTING, OR UPGRADING. FISSILE MATERIALS (PLUTONIUM, URANIUM, ETC.) AND RARE MATERIALS (BERYLLIUM) WERE RECOVERED FOR REUSE, AND THE REMAINDER WAS DISPOSED. (8/7/62) - Rocky Flats Plant, Plutonium Fabrication, Central section of Plant, Golden, Jefferson County, CO
Pyrochemical process for extracting plutonium from an electrolyte salt
Mullins, L.J.; Christensen, D.C.
1982-09-20
A pyrochemical process for extracting plutonium from a plutonium-bearing salt is disclosed. The process is particularly useful in the recovery of plutonium for electrolyte salts which are left over from the electrorefining of plutonium. In accordance with the process, the plutonium-bearing salt is melted and mixed with metallic calcium. The calcium reduces ionized plutonium in the salt to plutonium metal, and also causes metallic plutonium in the salt, which is typically present as finely dispersed metallic shot, to coalesce. The reduced and coalesced plutonium separates out on the bottom of the reaction vessel as a separate metallic phase which is readily separable from the overlying salt upon cooling of the mixture. Yields of plutonium are typically on the order of 95%. The stripped salt is virtually free of plutonium and may be discarded to low-level waste storage.
Pyrochemical process for extracting plutonium from an electrolyte salt
Mullins, Lawrence J.; Christensen, Dana C.
1984-01-01
A pyrochemical process for extracting plutonium from a plutonium-bearing salt is disclosed. The process is particularly useful in the recovery of plutonium from electrolyte salts which are left over from the electrorefining of plutonium. In accordance with the process, the plutonium-bearing salt is melted and mixed with metallic calcium. The calcium reduces ionized plutonium in the salt to plutonium metal, and also causes metallic plutonium in the salt, which is typically present as finely dispersed metallic shot, to coalesce. The reduced and coalesced plutonium separates out on the bottom of the reaction vessel as a separate metallic phase which is readily separable from the overlying salt upon cooling of the mixture. Yields of plutonium are typically on the order of 95%. The stripped salt is virtually free of plutonium and may be discarded to low-level waste storage.
Certified reference materials and reference methods for nuclear safeguards and security.
Jakopič, R; Sturm, M; Kraiem, M; Richter, S; Aregbe, Y
2013-11-01
Confidence in comparability and reliability of measurement results in nuclear material and environmental sample analysis are established via certified reference materials (CRMs), reference measurements, and inter-laboratory comparisons (ILCs). Increased needs for quality control tools in proliferation resistance, environmental sample analysis, development of measurement capabilities over the years and progress in modern analytical techniques are the main reasons for the development of new reference materials and reference methods for nuclear safeguards and security. The Institute for Reference Materials and Measurements (IRMM) prepares and certifices large quantities of the so-called "large-sized dried" (LSD) spikes for accurate measurement of the uranium and plutonium content in dissolved nuclear fuel solutions by isotope dilution mass spectrometry (IDMS) and also develops particle reference materials applied for the detection of nuclear signatures in environmental samples. IRMM is currently replacing some of its exhausted stocks of CRMs with new ones whose specifications are up-to-date and tailored for the demands of modern analytical techniques. Some of the existing materials will be re-measured to improve the uncertainties associated with their certified values, and to enable laboratories to reduce their combined measurement uncertainty. Safeguards involve the quantitative verification by independent measurements so that no nuclear material is diverted from its intended peaceful use. Safeguards authorities pay particular attention to plutonium and the uranium isotope (235)U, indicating the so-called 'enrichment', in nuclear material and in environmental samples. In addition to the verification of the major ratios, n((235)U)/n((238)U) and n((240)Pu)/n((239)Pu), the minor ratios of the less abundant uranium and plutonium isotopes contain valuable information about the origin and the 'history' of material used for commercial or possibly clandestine purposes, and have therefore reached high level of attention for safeguards authorities. Furthermore, IRMM initiated and coordinated the development of a Modified Total Evaporation (MTE) technique for accurate abundance ratio measurements of the "minor" isotope-amount ratios of uranium and plutonium in nuclear material and, in combination with a multi-dynamic measurement technique and filament carburization, in environmental samples. Currently IRMM is engaged in a study on the development of plutonium reference materials for "age dating", i.e. determination of the time elapsed since the last separation of plutonium from its daughter nuclides. The decay of a radioactive parent isotope and the build-up of a corresponding amount of daughter nuclide serve as chronometer to calculate the age of a nuclear material. There are no such certified reference materials available yet. Copyright © 2013 Elsevier Ltd. All rights reserved.
Critical review of analytical techniques for safeguarding the thorium-uranium fuel cycle
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hakkila, E.A.
1978-10-01
Conventional analytical methods applicable to the determination of thorium, uranium, and plutonium in feed, product, and waste streams from reprocessing thorium-based nuclear reactor fuels are reviewed. Separations methods of interest for these analyses are discussed. Recommendations concerning the applicability of various techniques to reprocessing samples are included. 15 tables, 218 references.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Holland, Michael K.; O'Rourke, Patrick E.
An SRNL H-Canyon Test Bed performance evaluation project was completed jointly by SRNL and LANL on a prototype monochromatic energy dispersive x-ray fluorescence instrument, the hiRX. A series of uncertainty propagations were generated based upon plutonium and uranium measurements performed using the alpha-prototype hiRX instrument. Data reduction and uncertainty modeling provided in this report were performed by the SRNL authors. Observations and lessons learned from this evaluation were also used to predict the expected uncertainties that should be achievable at multiple plutonium and uranium concentration levels provided instrument hardware and software upgrades being recommended by LANL and SRNL are performed.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hecker, Siegfried S.
Actions of the Government of the Democratic People's Republic of Korea have precipitated two nuclear crises in the past 10 years. The 1994 crisis was resolved through the 'Agreed Framework.' North Korea agreed to 'freeze' and eventually dismantle its nuclear program (with U.S. help to store spent fuel safely and under IAEA inspection). In return, the United States agreed (with the KEDO international consortium) to build two light-water reactors and supply North Korea with heavy-fuel oil until the reactors come on line. In addition, both sides agreed to move towards full normalization of relations, work for peace and security onmore » a nuclear-free Korean Peninsula, and work on strengthening the international nonproliferation regime. The second nuclear crisis erupted when North Korean Government officials allegedly admitted to having a clandestine uranium enrichment program when confronted with this accusation by U.S. officials in October 2002. The United States (through KEDO) suspended heavy-fuel oil shipments and North Korea responded by expelling the IAEA inspectors, withdrawing from the Nuclear Nonproliferation Treaty, and restarting its nuclear program in January 2003. The North Korean Government has invited Professor John Lewis of Stanford University, a China and North Korea scholar, for Track I1 discussions of nuclear and other key issues since 1987. In August 2003, Professor Lewis visited North Korea just before the first six-party talks, which were designed by the United States to solve the current nuclear crisis. Professor Lewis was invited back for the January 2004 visit. He asked Jack Pritchard, former U.S. special envoy for DRPK negotiations, and me to accompany him. Two Asian affairs staff specialists from the U.S. Senate Foreign Relations Committee also joined us. I will report on the visit to the Yongbyon Nuclear Scientific Research Center on January 8,2004. We toured the 5 MWe reactor, the 50 MWe reactor construction site, the spent fuel pool storage building, and the radiochemical laboratory. We concluded that North Korea has restarted its 5 MWe reactor (which produces roughly 6 kg of plutonium annually), it removed the 8000 spent fuel rods that were previously stored under IAEA safeguards from the spent fuel pool, and that it most likely extracted the 25 to 30 kg of plutonium contained in these fuel rods. Although North Korean officials showed us what they claimed was their plutonium metal product from this reprocessing campaign, we were not able to conclude definitively that it was in fact plutonium metal and that it came from the most recent reprocessing campaign. Nevertheless, our North Korean hosts demonstrated that they had the capability, the facility and requisite capacity, and the technical expertise to produce plutonium metal. We were not shown any facilities or had the opportunity to talk to technical or military experts who were able to address the issue of whether or not North Korea had a 'deterrent' as claimed - that is, we were not able to conclude that North Korea can build a nuclear device and that it can integrate nuclear devices into suitable delivery systems. On the matter of uranium enrichment programs, Vice Minister Kim Gye Gwan categorically denied that North Korea has a uranium enrichment program - he said, 'we have no program, no equipment, and no technical expertise for uranium enrichment.' Upon return to the United States, I shared my observations and analysis with U.S. Government officials in Washington, DC, including congressional testimony to the Senate Foreign Relations Committee and briefings to two House of Representative Committees.« less
Advanced electrorefiner design
Miller, W.E.; Gay, E.C.; Tomczuk, Z.
1996-07-02
A combination anode and cathode is described for an electrorefiner which includes a hollow cathode and an anode positioned inside the hollow cathode such that a portion of the anode is near the cathode. A retaining member is positioned at the bottom of the cathode. Mechanism is included for providing relative movement between the anode and the cathode during deposition of metal on the inside surface of the cathode during operation of the electrorefiner to refine spent nuclear fuel. A method is also disclosed which includes electrical power means selectively connectable to the anode and the hollow cathode for providing electrical power to the cell components, electrically transferring uranium values and plutonium values from the anode to the electrolyte, and electrolytically depositing substantially pure uranium on the hollow cathode. Uranium and plutonium are deposited at a liquid cathode together after the PuCl{sub 3} to UCl{sub 3} ratio is greater than 2:1. Slots in the hollow cathode provides close anode access for the liquid pool in the liquid cathode. 6 figs.
Advanced electrorefiner design
Miller, William E.; Gay, Eddie C.; Tomczuk, Zygmunt
1996-01-01
A combination anode and cathode for an electrorefiner which includes a hollow cathode and an anode positioned inside the hollow cathode such that a portion of the anode is near the cathode. A retaining member is positioned at the bottom of the cathode. Mechanism is included for providing relative movement between the anode and the cathode during deposition of metal on the inside surface of the cathode during operation of the electrorefiner to refine spent nuclear fuel. A method is also disclosed which includes electrical power means selectively connectable to the anode and the hollow cathode for providing electrical power to the cell components, electrically transferring uranium values and plutonium values from the anode to the electrolyte, and electrolytically depositing substantially pure uranium on the hollow cathode. Uranium and plutonium are deposited at a liquid cathode together after the PuCl.sub.3 to UCl.sub.3 ratio is greater than 2:1. Slots in the hollow cathode provides close anode access for the liquid pool in the liquid cathode.
PLUTONIUM COMPOUNDS AND PROCESS FOR THEIR PREPARATION
Wolter, F.J.; Diehl, H.C. Jr.
1958-01-01
This patent relates to certain new compounds of plutonium, and to the utilization of these compounds to effect purification or separation of the plutonium. The compounds are organic chelate compounds consisting of tetravalent plutonium together with a di(salicylal) alkylenediimine. These chelates are soluble in various organic solvents, but not in water. Use is made of this property in extracting the plutonium by contacting an aqueous solution thereof with an organic solution of the diimine. The plutonium is chelated, extracted and effectively separated from any impurities accompaying it in the aqueous phase.
Esaka, Fumitaka; Magara, Masaaki; Suzuki, Daisuke; Miyamoto, Yutaka; Lee, Chi-Gyu; Kimura, Takaumi
2010-12-15
Information on plutonium isotope ratios in individual particles is of great importance for nuclear safeguards, nuclear forensics and so on. Although secondary ion mass spectrometry (SIMS) is successfully utilized for the analysis of individual uranium particles, the isobaric interference of americium-241 to plutonium-241 makes difficult to obtain accurate isotope ratios in individual plutonium particles. In the present work, an analytical technique by a combination of chemical separation and inductively coupled plasma mass spectrometry (ICP-MS) is developed and applied to isotope ratio analysis of individual sub-micrometer plutonium particles. The ICP-MS results for individual plutonium particles prepared from a standard reference material (NBL SRM-947) indicate that the use of a desolvation system for sample introduction improves the precision of isotope ratios. In addition, the accuracy of the (241)Pu/(239)Pu isotope ratio is much improved, owing to the chemical separation of plutonium and americium. In conclusion, the performance of the proposed ICP-MS technique is sufficient for the analysis of individual plutonium particles. Copyright © 2010 Elsevier B.V. All rights reserved.
COUPLED FAST-THERMAL POWER BREEDER REACTOR
Avery, R.
1961-07-18
A nuclear reactor having a region operating predominantly on fast neutrons and another region operating predominantly on slow neutrons is described. The fast region is a plutonium core and the slow region is a natural uranium blanket around the core. Both of these regions are free of moderator. A moderating reflector surrounds the uranium blanket. The moderating material and thickness of the reflector are selected so that fissions in the uranium blanket make a substantial contribution to the reactivity of the reactor.
COST FUNCTION STUDIES FOR POWER REACTORS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Heestand, J.; Wos, L.T.
1961-11-01
A function to evaluate the cost of electricity produced by a nuclear power reactor was developed. The basic equation, revenue = capital charges + profit + operating expenses, was expanded in terms of various cost parameters to enable analysis of multiregion nuclear reactors with uranium and/or plutonium for fuel. A corresponding IBM 704 computer program, which will compute either the price of electricity or the value of plutonium, is presented in detail. (auth)
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dougherty, D.; Fainberg, A.; Sanborn, J.
On 27 September 1993, President Clinton proposed {open_quotes}... a multilateral convention prohibiting the production of highly enriched uranium or plutonium for nuclear explosives purposes or outside of international safeguards.{close_quotes} The UN General Assembly subsequently adopted a resolution recommending negotiation of a non-discriminatory, multilateral, and internationally and effectively verifiable treaty (hereinafter referred to as {open_quotes}the Cutoff Convention{close_quotes}) banning the production of fissile material for nuclear weapons. The matter is now on the agenda of the Conference on Disarmament, although not yet under negotiation. This accord would, in effect, place all fissile material (defined as highly enriched uranium and plutonium) produced aftermore » entry into force (EIF) of the accord under international safeguards. {open_quotes}Production{close_quotes} would mean separation of the material in question from radioactive fission products, as in spent fuel reprocessing, or enrichment of uranium above the 20% level, which defines highly enriched uranium (HEU). Facilities where such production could occur would be safeguarded to verify that either such production is not occurring or that all material produced at these facilities is maintained under safeguards.« less
Strength and fracture of uranium, plutonium and several their alloys under shock wave loading
NASA Astrophysics Data System (ADS)
Golubev, V. K.
2012-08-01
Results on studying the spall fracture of uranium, plutonium and several their alloys under shock wave loading are presented in the paper. The problems of influence of initial temperature in a range of - 196 - 800∘C and loading time on the spall strength and failure character of uranium and two its alloys with molybdenum and both molybdenum and zirconium were studied. The results for plutonium and its alloy with gallium were obtained at a normal temperature and in a temperature range of 40-315∘C, respectively. The majority of tests were conducted with the samples in the form of disks 4 mm in thickness. They were loaded by the impact of aluminum plates 4 mm thick through a copper screen 12 mm thick serving as the cover or bottom part of a special container. The character of spall failure of materials and the damage degree of samples were observed on the longitudinal metallographic sections of recovered samples. For a concrete test temperature, the impact velocity was sequentially changed and therefore the loading conditions corresponding to the consecutive transition from microdamage nucleation up to complete macroscopic spall fracture were determined. The conditions of shock wave loading were calculated using an elastic-plastic computer program. The comparison of obtained results with the data of other researchers on the spall fracture of examined materials was conducted.
Spall fracture and strength of uranium, plutonium and their alloys under shock wave loading
NASA Astrophysics Data System (ADS)
Golubev, Vladimir
2015-06-01
Numerous results on studying the spall fracture phenomenon of uranium, two its alloys with molybdenum and zirconium, plutonium and its alloy with gallium under shock wave loading are presented in the paper. The majority of tests were conducted with the samples in the form of disks 4mm in thickness. They were loaded by the impact of aluminum plates 4mm thick through a copper screen serving as the cover or bottom part of a special container. The initial temperature of samples was changed in the range of -196 - 800 C degree for uranium and 40 - 315 C degree for plutonium. The character of spall failure of materials and the degree of damage for all tested samples were observed on the longitudinal metallographic sections of recovered samples. For a concrete test temperature, the impact velocity was sequentially changed and therefore the loading conditions corresponding to the consecutive transition from microdamage nucleation up to complete macroscopic spall fracture were determined. Numerical calculations of the conditions of shock wave loading and spall fracture of samples were performed in the elastoplastic approach. Several two- and three-dimensional effects of loading were taken into account. Some results obtained under conditions of intensive impulse irradiation and intensive explosive loading are presented too. The rather complete analysis and comparison of obtained results with the data of other researchers on the spall fracture of examined materials were conducted.
Continuous process electrorefiner
Herceg, Joseph E [Naperville, IL; Saiveau, James G [Hickory Hills, IL; Krajtl, Lubomir [Woodridge, IL
2006-08-29
A new device is provided for the electrorefining of uranium in spent metallic nuclear fuels by the separation of unreacted zirconium, noble metal fission products, transuranic elements, and uranium from spent fuel rods. The process comprises an electrorefiner cell. The cell includes a drum-shaped cathode horizontally immersed about half-way into an electrolyte salt bath. A conveyor belt comprising segmented perforated metal plates transports spent fuel into the salt bath. The anode comprises the conveyor belt, the containment vessel, and the spent fuel. Uranium and transuranic elements such as plutonium (Pu) are oxidized at the anode, and, subsequently, the uranium is reduced to uranium metal at the cathode. A mechanical cutter above the surface of the salt bath removes the deposited uranium metal from the cathode.
NASA Astrophysics Data System (ADS)
Ault, Timothy M.
The environment, health, and safety properties of thorium-uranium-based (''thorium'') fuel cycles are estimated and compared to those of analogous uranium-plutonium-based (''uranium'') fuel cycle options. A structured assessment methodology for assessing and comparing fuel cycle is refined and applied to several reference fuel cycle options. Resource recovery as a measure of environmental sustainability for thorium is explored in depth in terms of resource availability, chemical processing requirements, and radiological impacts. A review of available experience and recent practices indicates that near-term thorium recovery will occur as a by-product of mining for other commodities, particularly titanium. The characterization of actively-mined global titanium, uranium, rare earth element, and iron deposits reveals that by-product thorium recovery would be sufficient to satisfy even the most intensive nuclear demand for thorium at least six times over. Chemical flowsheet analysis indicates that the consumption of strong acids and bases associated with thorium resource recovery is 3-4 times larger than for uranium recovery, with the comparison of other chemical types being less distinct. Radiologically, thorium recovery imparts about one order of magnitude larger of a collective occupational dose than uranium recovery. Moving to the entire fuel cycle, four fuel cycle options are compared: a limited-recycle (''modified-open'') uranium fuel cycle, a modified-open thorium fuel cycle, a full-recycle (''closed'') uranium fuel cycle, and a closed thorium fuel cycle. A combination of existing data and calculations using SCALE are used to develop material balances for the four fuel cycle options. The fuel cycle options are compared on the bases of resource sustainability, waste management (both low- and high-level waste, including used nuclear fuel), and occupational radiological impacts. At steady-state, occupational doses somewhat favor the closed thorium option while low-level waste volumes slightly favor the closed uranium option, although uncertainties are significant in both cases. The high-level waste properties (radioactivity, decay heat, and ingestion radiotoxicity) all significantly favor the closed fuel cycle options (especially the closed thorium option), but an alternative measure of key fission product inventories that drive risk in a repository slightly favors the uranium fuel cycles due to lower production of iodine-129. Resource requirements are much lower for the closed fuel cycle options and are relatively similar between thorium and uranium. In additional to the steady-state results, a variety of potential transition pathways are considered for both uranium and thorium fuel cycle end-states. For dose, low-level waste, and fission products contributing to repository risk, the differences among transition impacts largely reflected the steady-state differences. However, the HLW properties arrived at a distinctly opposite result in transition (strongly favoring uranium, whereas thorium was strongly favored at steady-state), because used present-day fuel is disposed without being recycled given that uranium-233, rather than plutonium, is the primarily fissile nuclide at the closed thorium fuel cycle's steady-state. Resource consumption was the only metric was strongly influenced by the specific transition pathway selected, favoring those pathways that more quickly arrived at steady-state through higher breeding ratio assumptions regardless of whether thorium or uranium was used.
Final Report on Two-Stage Fast Spectrum Fuel Cycle Options
DOE Office of Scientific and Technical Information (OSTI.GOV)
Yang, Won Sik; Lin, C. S.; Hader, J. S.
2016-01-30
This report presents the performance characteristics of two “two-stage” fast spectrum fuel cycle options proposed to enhance uranium resource utilization and to reduce nuclear waste generation. One is a two-stage fast spectrum fuel cycle option of continuous recycle of plutonium (Pu) in a fast reactor (FR) and subsequent burning of minor actinides (MAs) in an accelerator-driven system (ADS). The first stage is a sodium-cooled FR fuel cycle starting with low-enriched uranium (LEU) fuel; at the equilibrium cycle, the FR is operated using the recovered Pu and natural uranium without supporting LEU. Pu and uranium (U) are co-extracted from the dischargedmore » fuel and recycled in the first stage, and the recovered MAs are sent to the second stage. The second stage is a sodium-cooled ADS in which MAs are burned in an inert matrix fuel form. The discharged fuel of ADS is reprocessed, and all the recovered heavy metals (HMs) are recycled into the ADS. The other is a two-stage FR/ADS fuel cycle option with MA targets loaded in the FR. The recovered MAs are not directly sent to ADS, but partially incinerated in the FR in order to reduce the amount of MAs to be sent to the ADS. This is a heterogeneous recycling option of transuranic (TRU) elements« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Tandon, Lav; Kuhn, Kevin J; Drake, Lawrence R
Los Alamos National Laboratory's (LANL) Actinide Analytical Chemistry (AAC) group has been in existence since the Manhattan Project. It maintains a complete set of analytical capabilities for performing complete characterization (elemental assay, isotopic, metallic and non metallic trace impurities) of uranium and plutonium samples in different forms. For a majority of the customers there are strong quality assurance (QA) and quality control (QC) objectives including highest accuracy and precision with well defined uncertainties associated with the analytical results. Los Alamos participates in various international and national programs such as the Plutonium Metal Exchange Program, New Brunswick Laboratory's (NBL' s) Safeguardsmore » Measurement Evaluation Program (SME) and several other inter-laboratory round robin exercises to monitor and evaluate the data quality generated by AAC. These programs also provide independent verification of analytical measurement capabilities, and allow any technical problems with analytical measurements to be identified and corrected. This presentation will focus on key analytical capabilities for destructive analysis in AAC and also comparative data between LANL and peer groups for Pu assay and isotopic analysis.« less
Evaluation of phases in Pu-C-O and (U, Pu)-C-O systems by X-ray diffractometry and chemical analysis
NASA Astrophysics Data System (ADS)
Jain, G. C.; Ganguly, C.
1993-12-01
Preparation and characterisation of the carbides of uranium, plutonium and mixed uranium and plutonium form a part of advanced fuel development programs for fast breeder reactors. In the present study, the compositions of the phases of Pu-C-O and (U.Pu)-C-O systems have been determined by chemical analysis and lattice parameter measurement. The carbide samples have been prepared by vacuum carbothermic synthesis of tabletted oxide-graphite powder mixture. Dependence of stoichiometry of Pu 2C 3 phase on the oxygen content of Pu(C,O) phase in Pu(C,O) + Pu 2C 3 phase mixture has been evaluated. Stoichiometry and oxygen solubility of (U 0.3Pu 0.7)(C,O) phase in multiple phase mixture have been determined. Segregation of plutonium in (U,Pu) 2C 3 phase of (U,Pu)(C,O) + (U,Pu) 2C 3 phase mixture and its dependence on the oxygen content of (U,Pu)(C,O) phase have also been determined from the measurement of the lattice parameter of (U,Pu) 2C 3 phase.
Nuclear fuel requirements for the American economy - A model
NASA Astrophysics Data System (ADS)
Curtis, Thomas Dexter
A model is provided to determine the amounts of various fuel streams required to supply energy from planned and projected nuclear plant operations, including new builds. Flexible, user-defined scenarios can be constructed with respect to energy requirements, choices of reactors and choices of fuels. The model includes interactive effects and extends through 2099. Outputs include energy provided by reactors, the number of reactors, and masses of natural Uranium and other fuels used. Energy demand, including electricity and hydrogen, is obtained from US DOE historical data and projections, along with other studies of potential hydrogen demand. An option to include other energy demand to nuclear power is included. Reactor types modeled include (thermal reactors) PWRs, BWRs and MHRs and (fast reactors) GFRs and SFRs. The MHRs (VHTRs), GFRs and SFRs are similar to those described in the 2002 DOE "Roadmap for Generation IV Nuclear Energy Systems." Fuel source choices include natural Uranium, self-recycled spent fuel, Plutonium from breeder reactors and existing stockpiles of surplus HEU, military Plutonium, LWR spent fuel and depleted Uranium. Other reactors and fuel sources can be added to the model. Fidelity checks of the model's results indicate good agreement with historical Uranium use and number of reactors, and with DOE projections. The model supports conclusions that substantial use of natural Uranium will likely continue to the end of the 21st century, though legacy spent fuel and depleted uranium could easily supply all nuclear energy demand by shifting to predominant use of fast reactors.
Plutonium release from the 903 pad at Rocky Flats.
Mongan, T R; Ripple, S R; Winges, K D
1996-10-01
The Colorado Department of Public Health and Environment (CDH) sponsored a study to reconstruct contaminant doses to the public from operations at the Rocky Flats nuclear weapons plant. This analysis of the accidental release of plutonium from the area known as the 903 Pad is part of the CDH study. In the 1950's and 1960's, 55-gallon drums of waste oil contaminated with plutonium, and uranium were stored outdoors at the 903 Pad. The drums corroded, leaking contaminated oil onto soil subsequently carried off-site by the wind. The plutonium release is estimated using environmental data from the 1960's and 1970's and an atmospheric transport model for fugitive dust. The best estimate of total plutonium release to areas beyond plant-owned property is about 0.26 TBq (7 Ci). Off-site airborne concentrations and deposition of plutonium are estimated for dose calculation purposes. The best estimate of the highest predicted off-site effective dose is approximately 72 microSv (7.2 mrem).
The underwater coincidence counter (UWCC) for plutonium measurements in mixed oxide fuels
DOE Office of Scientific and Technical Information (OSTI.GOV)
Eccleston, G.W.; Menlove, H.O.; Abhold, M.
1998-12-31
The use of fresh uranium-plutonium mixed oxide (MOX) fuel in light-water reactors (LWR) is increasing in Europe and Japan and it is necessary to verify the plutonium content in the fuel for international safeguards purposes. The UWCC is a new instrument that has been designed to operate underwater and nondestructively measure the plutonium in unirradiated MOX fuel assemblies. The UWCC can be quickly configured to measure either boiling-water reactor (BWR) or pressurized-water reactor (PWR) fuel assemblies. The plutonium loading per unit length is measured using the UWCC to precisions of less than 1% in a measurement time of 2 tomore » 3 minutes. Initial calibrations of the UWCC were completed on measurements of MOX fuel in Mol, Belgium. The MCNP-REN Monte Carlo simulation code is being benchmarked to the calibration measurements to allow accurate simulations for extended calibrations of the UWCC.« less
Recent advances in the study of the UO2-PuO2 phase diagram at high temperatures
NASA Astrophysics Data System (ADS)
Böhler, R.; Welland, M. J.; Prieur, D.; Cakir, P.; Vitova, T.; Pruessmann, T.; Pidchenko, I.; Hennig, C.; Guéneau, C.; Konings, R. J. M.; Manara, D.
2014-05-01
Recently, novel container-less laser heating experimental data have been published on the melting behaviour of pure PuO2 and PuO2-rich compositions in the uranium dioxide-plutonium dioxide system. Such data showed that previous data obtained by more traditional furnace heating techniques were affected by extensive interaction between the sample and its containment. It is therefore paramount to check whether data so far used by nuclear engineers for the uranium-rich side of the pseudo-binary dioxide system can be confirmed or not. In the present work, new data are presented both in the UO2-rich part of the phase diagram, most interesting for the uranium-plutonium dioxide based nuclear fuel safety, and in the PuO2 side. The new results confirm earlier furnace heating data in the uranium-dioxide rich part of the phase diagram, and more recent laser-heating data in the plutonium-dioxide side of the system. As a consequence, it is also confirmed that a minimum melting point must exist in the UO2-PuO2 system, at a composition between x(PuO2) = 0.4 and x(PuO2) = 0.7 and 2900 K ⩽ T ⩽ 3000 K. Taking into account that, especially at high temperature, oxygen chemistry has an effect on the reported phase boundary uncertainties, the current results should be projected in the ternary U-Pu-O system. This aspect has been extensively studied here by X-ray diffraction and X-ray absorption spectroscopy. The current results suggest that uncertainty bands related to oxygen behaviour in the equilibria between condensed phases and gas should not significantly affect the qualitative trend of the current solid-liquid phase boundaries.
Deploying Nuclear Detection Systems: A Proposed Strategy for Combating Nuclear Terrorism
2007-07-01
lower cost than other gamma radiation detectors (if increased count rate is all one is looking for). Low cost makes plastic scintillation detectors...material, particularly enriched uranium and plutonium, the basic fuel for nuclear bombs. • Measures to strengthen international institutions to... uranium to specifications required for a nuclear weapon.1 This illicit shipment of centrifuges was part of an international nuclear materials
Organic Separation Test Results
DOE Office of Scientific and Technical Information (OSTI.GOV)
Russell, Renee L.; Rinehart, Donald E.; Peterson, Reid A.
2014-09-22
Separable organics have been defined as “those organic compounds of very limited solubility in the bulk waste and that can form a separate liquid phase or layer” (Smalley and Nguyen 2013), and result from three main solvent extraction processes: U Plant Uranium Recovery Process, B Plant Waste Fractionation Process, and Plutonium Uranium Extraction (PUREX) Process. The primary organic solvents associated with tank solids are TBP, D2EHPA, and NPH. There is concern that, while this organic material is bound to the sludge particles as it is stored in the tanks, waste feed delivery activities, specifically transfer pump and mixer pump operations,more » could cause the organics to form a separated layer in the tank farms feed tank. Therefore, Washington River Protection Solutions (WRPS) is experimentally evaluating the potential of organic solvents separating from the tank solids (sludge) during waste feed delivery activities, specifically the waste mixing and transfer processes. Given the Hanford Tank Waste Treatment and Immobilization Plant (WTP) waste acceptance criteria per the Waste Feed Acceptance Criteria document (24590-WTP-RPT-MGT-11-014) that there is to be “no visible layer” of separable organics in the waste feed, this would result in the batch being unacceptable to transfer to WTP. This study is of particular importance to WRPS because of these WTP requirements.« less
Determining the release of radionuclides from tank waste residual solids. FY2015 report
DOE Office of Scientific and Technical Information (OSTI.GOV)
King, William D.; Hobbs, David T.
Methodology development for pore water leaching studies has been continued to support Savannah River Site High Level Waste tank closure efforts. For FY2015, the primary goal of this testing was the achievement of target pH and Eh values for pore water solutions representative of local groundwater in the presence of grout or grout-representative (CaCO 3 or FeS) solids as well as waste surrogate solids representative of residual solids expected to be present in a closed tank. For oxidizing conditions representative of a closed tank after aging, a focus was placed on using solid phases believed to be controlling pH andmore » E h at equilibrium conditions. For three pore water conditions (shown below), the target pH values were achieved to within 0.5 pH units. Tank 18 residual surrogate solids leaching studies were conducted over an E h range of approximately 630 mV. Significantly higher Eh values were achieved for the oxidizing conditions (ORII and ORIII) than were previously observed. For the ORII condition, the target Eh value was nearly achieved (within 50 mV). However, E h values observed for the ORIII condition were approximately 160 mV less positive than the target. E h values observed for the RRII condition were approximately 370 mV less negative than the target. Achievement of more positive and more negative E h values is believed to require the addition of non-representative oxidants and reductants, respectively. Plutonium and uranium concentrations measured during Tank 18 residual surrogate solids leaching studies under these conditions (shown below) followed the general trends predicted for plutonium and uranium oxide phases, assuming equilibrium with dissolved oxygen. The highest plutonium and uranium concentrations were observed for the ORIII condition and the lowest concentrations were observed for the RRII condition. Based on these results, it is recommended that these test methodologies be used to conduct leaching studies with actual Tank 18 residual solids material. Actual waste testing will include leaching evaluations of technetium and neptunium, as well as plutonium and uranium.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Delegard, Calvin H.; Casella, Amanda J.
2016-09-30
This report summarizes the literature reviewed on crud formation at the liquid:liquid interface of solvent extraction processes. The review is focused both on classic PUREX extraction for industrial reprocessing, especially as practiced at the Hanford Site, and for those steps specific to plutonium purification that were used at the Plutonium Reclamation Facility (PRF) within the Plutonium Finishing Plant (PFP) at the Hanford Site.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Levy, Y.; Friedman, G. M.; Miller, D. S.
1978-12-31
Results of the analysis of uranium concentrations in the 8 coral heads sampled from the Bikini and Enewetak lagoons lead to the following conclusions: (1) no parallel increase in uranium concentration was found in the corals contaminated by Pu and Am; (2) in the noncontaminated corals, the fission track analysis shows wider ranges of uranium concentrations (1.8 to 3.1). Thus, in the corals not contaminated by Pu and Am, uranium concentrations similar to the uranium concentration in the contaminated corals were found; (3) uranium content in all corals analyzed was rather homogeneously distributed, i.e., no hot spots, stars, or areasmore » differing in concentration by more than a few percent were detected by the fission track analyses.« less
NASA Astrophysics Data System (ADS)
Degueldre, Claude; Cozzo, Cedric; Martin, Matthias; Grolimund, Daniel; Mieszczynski, Cyprian
2013-06-01
Plutonium uranium mixed oxide (MOX) fuels are currently used in nuclear reactors. The actinides in these fuels need to be analyzed after irradiation for assessing their behaviour with regard to their environment and the coolant. In this work the study of the atomic structure and next-neighbour environment of Am in the (Pu,U)O2 lattice in an irradiated (60 MW d kg-1) MOX sample was performed employing micro-X-ray fluorescence (µ-XRF) and micro-X-ray absorption fine structure (µ-XAFS) spectroscopy. The chemical bonds, valences and stoichiometry of Am (˜0.66 wt%) are determined from the experimental data gained for the irradiated fuel material examined in its peripheral zone (rim) of the fuel. In the irradiated sample Am builds up as Am3+ species within an [AmO8]13- coordination environment (e.g. >90%) and no (<10%) Am(IV) or (V) can be detected in the rim zone. The occurrence of americium dioxide is avoided by the redox buffering activity of the uranium dioxide matrix.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bi, G.; Liu, C.; Si, S.
This paper was focused on core design, neutronics evaluation and fuel cycle analysis for Thorium-Uranium Breeding Recycle in current PWRs, without any major change to the fuel lattice and the core internals, but substituting the UOX pellet with Thorium-based pellet. The fuel cycle analysis indicates that Thorium-Uranium Breeding Recycle is technically feasible in current PWRs. A 4-loop, 193-assembly PWR core utilizing 17 x 17 fuel assemblies (FAs) was taken as the model core. Two mixed cores were investigated respectively loaded with mixed reactor grade Plutonium-Thorium (PuThOX) FAs and mixed reactor grade {sup 233}U-Thorium (U{sub 3}ThOX) FAs on the basis ofmore » reference full Uranium oxide (UOX) equilibrium-cycle core. The UOX/PuThOX mixed core consists of 121 UOX FAs and 72 PuThOX FAs. The reactor grade {sup 233}U extracted from burnt PuThOX fuel was used to fabrication of U{sub 3}ThOX for starting Thorium-. Uranium breeding recycle. In UOX/U{sub 3}ThOX mixed core, the well designed U{sub 3}ThOX FAs with 1.94 w/o fissile uranium (mainly {sup 233}U) were located on the periphery of core as a blanket region. U{sub 3}ThOX FAs remained in-core for 6 cycles with the discharged burnup achieving 28 GWD/tHM. Compared with initially loading, the fissile material inventory in U{sub 3}ThOX fuel has increased by 7% via 1-year cooling after discharge. 157 UOX fuel assemblies were located in the inner of UOX/U{sub 3}ThOX mixed core refueling with 64 FAs at each cycle. The designed UOX/PuThOX and UOX/U{sub 3}ThOX mixed core satisfied related nuclear design criteria. The full core performance analyses have shown that mixed core with PuThOX loading has similar impacts as MOX on several neutronic characteristic parameters, such as reduced differential boron worth, higher critical boron concentration, more negative moderator temperature coefficient, reduced control rod worth, reduced shutdown margin, etc.; while mixed core with U{sub 3}ThOX loading on the periphery of core has no visible impacts on neutronic characteristics compared with reference full UOX core. The fuel cycle analysis has shown that {sup 233}U mono-recycling with U{sub 3}ThOX fuel could save 13% of natural uranium resource compared with UOX once through fuel cycle, slightly more than that of Plutonium single-recycling with MOX fuel. If {sup 233}U multi-recycling with U{sub 3}ThOX fuel is implemented, more natural uranium resource would be saved. (authors)« less
Natural chelates for radionuclide decorporation
Premuzic, E.T.
1983-08-25
This invention relates to the method and resulting chelates of desorbing a radionuclide selected from thorium, uranium, and plutonium containing cultures in a bioavailable form involving pseudomonas or other microorganisms. A preferred microorganism is Pseudomonas aeruginosa which forms multiple chelates with thorium in the range of molecular weight 1000 to 1000 and also forms chelates with uranium of molecular weight in the area of 100 to 1000 and 1000 to 2000.
JPRS Report, Science & Technology, Japan
1987-11-12
Change (4) Future Direction Anyway, it has become almost clear that the effect of power recovery cannot be expected from the insulation of...process spent fuels in greater safety and to recover the uranium or plutonium from spent fuels for effective reapplication. In 1974, the PNC began...constructed to serve as a pilot plant that could be used to establish reprocessing technology for the next practical stage. 32 As for enriched uranium
PUREX/UO{sub 3} deactivation project management plan
DOE Office of Scientific and Technical Information (OSTI.GOV)
Washenfelder, D.J.
1993-12-01
From 1955 through 1990, the Plutonium-Uranium Extraction Plant (PUREX) provided the United States Department of Energy Hanford Site with nuclear fuel reprocessing capability. It operated in sequence with the Uranium Trioxide (UO{sub 3}) Plant, which converted the PUREX liquid uranium nitrate product to solid UO{sub 3} powder. Final UO{sub 3} Plant operation ended in 1993. In December 1992, planning was initiated for the deactivation of PUREX and UO{sub 3} Plant. The objective of deactivation planning was to identify the activities needed to establish a passively safe, environmentally secure configuration at both plants, and ensure that the configuration could be retainedmore » during the post-deactivation period. The PUREX/UO{sub 3} Deactivation Project management plan represents completion of the planning efforts. It presents the deactivation approach to be used for the two plants, and the supporting technical, cost, and schedule baselines. Deactivation activities concentrate on removal, reduction, and stabilization of the radioactive and chemical materials remaining at the plants, and the shutdown of the utilities and effluents. When deactivation is completed, the two plants will be left unoccupied and locked, pending eventual decontamination and decommissioning. Deactivation is expected to cost $233.8 million, require 5 years to complete, and yield $36 million in annual surveillance and maintenance cost savings.« less
Synthesis of actinide nitrides, phosphides, sulfides and oxides
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hay, M.
2016-10-24
SRNL analyzed samples from Tank 38H and Tank 43H to support ECP and CCP. The total uranium in the Tank 38H surface sample was 57.6 mg/L, while the sub-surface sample was 106 mg/L. The Tank 43H samples ranged from 50.0 to 51.9 mg/L total uranium. The U-235 percentage was consistent for all four samples at 0.62%. The total uranium and percent U-235 results appear consistent with recent Tank 38H and Tank 43H uranium measurements. The Tank 38H plutonium results show a large difference between the surface and sub-surface sample concentrations and somewhat higher concentrations than previous samples. The Pu-238 concentrationmore » is more than forty times higher in the Tank 38H sub-surface sample than the surface sample. The surface and sub-surface Tank 43H samples contain similar plutonium concentrations and are within the range of values measured on previous samples. The four samples analyzed show silicon concentrations somewhat higher than the previous sample with values ranging from 104 to 213 mg/L.« less
Graphene-based filament material for thermal ionization
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hewitt, J.; Shick, C.; Siegfried, M.
The use of graphene oxide materials for thermal ionization mass spectrometry analysis of plutonium and uranium has been investigated. Filament made from graphene oxide slurries have been 3-D printed. A method for attaching these filaments to commercial thermal ionization post assemblies has been devised. Resistive heating of the graphene based filaments under high vacuum showed stable operation in excess of 4 hours. Plutonium ion production has been observed in an initial set of filaments spiked with the Pu 128 Certified Reference Material.
None
2017-12-09
In 1999, the National Nuclear Security Administration (NNSA) signed a contract with a consortium, now called Shaw AREVA MOX Services, LLC to design, build, and operate a Mixed Oxide (MOX) Fuel Fabrication Facility. This facility will be a major component in the United States program to dispose of surplus weapon-grade plutonium. The facility will take surplus weapon-grade plutonium, remove impurities, and mix it with uranium oxide to form MOX fuel pellets for reactor fuel assemblies. These assemblies will be irradiated in commercial nuclear power reactors.
DOE Office of Scientific and Technical Information (OSTI.GOV)
None
2010-05-21
In 1999, the National Nuclear Security Administration (NNSA) signed a contract with a consortium, now called Shaw AREVA MOX Services, LLC to design, build, and operate a Mixed Oxide (MOX) Fuel Fabrication Facility. This facility will be a major component in the United States program to dispose of surplus weapon-grade plutonium. The facility will take surplus weapon-grade plutonium, remove impurities, and mix it with uranium oxide to form MOX fuel pellets for reactor fuel assemblies. These assemblies will be irradiated in commercial nuclear power reactors.
DOE Office of Scientific and Technical Information (OSTI.GOV)
None
2009-07-29
In 1999, the Nuclear Nuclear Security Administration (NNSA) signed a contract with a consortium, now called Shaw AREVA MOX Services, LLC to design, build, and operate a Mixed Oxide (MOX) Fuel Fabrication Facility. This facility will be a major component in the United States program to dispose of surplus weapon-grade plutonium. The facility will take surplus weapon-grade plutonium, remove impurities, and mix it with uranium oxide to form MOX fuel pellets for reactor fuel assemblies. These assemblies will be irradiated in commercial nuclear power reactors.
None
2018-01-16
In 1999, the Nuclear Nuclear Security Administration (NNSA) signed a contract with a consortium, now called Shaw AREVA MOX Services, LLC to design, build, and operate a Mixed Oxide (MOX) Fuel Fabrication Facility. This facility will be a major component in the United States program to dispose of surplus weapon-grade plutonium. The facility will take surplus weapon-grade plutonium, remove impurities, and mix it with uranium oxide to form MOX fuel pellets for reactor fuel assemblies. These assemblies will be irradiated in commercial nuclear power reactors.
NASA Astrophysics Data System (ADS)
Reed, B. Cameron
2014-10-01
The Manhattan Project was the United States Army’s program to develop and deploy nuclear weapons during World War II. In these devices, which are known popularly as ‘atomic bombs’, energy is released not by a chemical explosion but by the much more violent process of fission of nuclei of heavy elements via a neutron-mediated chain-reaction. Three years after taking on this project in mid-1942, the Army’s Manhattan Engineer District produced three nuclear bombs of two different designs. Two of these devices were fueled with the 239 isotope of the synthetic element plutonium, while the third employed the rare 235 isotope of uranium. One of the plutonium devices, code-named Trinity, was detonated in a test in southern New Mexico on 16 July 1945; this was the world’s first nuclear explosion. Three weeks later, on 6 August, the uranium bomb, Little Boy, was dropped on the Japanese city of Hiroshima. On 9 August the second plutonium device, Fat Man, was dropped on Nagasaki. Together, the two bombings killed over 100 000 people and were at least partially responsible for the Japanese government’s 14 August decision to surrender. This article surveys, at an undergraduate level, the science and history of the Manhattan Project.
Detection Technology in the 21st Century: The Case of Nuclear Weapons of Mass Destruction
2008-03-26
Weapons of Mass Destruction FORMAT : Strategy Research Project DATE: 26 March 2008 WORD COUNT: 6,764 PAGES: 25 KEY TERMS: National Security, Deterrence...stocks remaining in Ukraine, Belarus, Uzbekistan, and other former Soviet and Eastern European states, and the unknown amounts of highly enriched uranium ...detect emissions from the decay of radioactive nuclides, which can occur naturally, such as uranium and thorium, or are manmade, such as plutonium
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.
Brandt, H.L.
1962-02-20
A process is given for decanning fuel elements that consist of a uranium core, an intermediate section either of bronze, silicon, Al-Si, and uranium silicide layers or of lead, Al-Si, and uranium silicide layers around said core, and an aluminum can bonded to said intermediate section. The aluminum can is dissolved in a solution of sodium hydroxide (9 to 20 wt%) and sodium nitrate (35 to 12 wt %), and the layers of the intermediate section are dissolved in a boiling sodium hydroxide solution of a minimum concentration of 50 wt%. (AEC) A method of selectively reducing plutonium oxides and the rare earth oxides but not uranium oxides is described which comprises placing the oxides in a molten solvent of zinc or cadmium and then adding metallic uranium as a reducing agent. (AEC)
DOE Office of Scientific and Technical Information (OSTI.GOV)
ITLV
1998-07-01
Corrective Action Unit 485, Corrective Action Site TA-39-001-TAGR, the Cactus Spring Ranch Soil Contamination Area, is located approximately six miles southwest of the Area 3 Compound at the eastern mouth of Sleeping Column Canyon in the Cactus Range on the Tonopah Test Range. This site was used in conjunction with animal studies involving the biological effects of radionuclides (specifically plutonium) associated with Operation Roller Coaster. According to field records, a hardened layer of livestock feces ranging from 2.54 centimeters (cm) (1 inch [in.]) to 10.2 cm (4 in.) thick is present in each of the main sheds. IT personnel conductedmore » a field visit on December 3, 1997, and noted that the only visible feces were located within the east shed, the previously fenced area near the east shed, and a small area southwest of the west shed. Other historical records indicate that other areas may still be covered with animal feces, but heavy vegetation now covers it. It is possible that radionuclides are present in this layer, given the history of operations in this area. Chemicals of concern may include plutonium and depleted uranium. Surface soil sampling was conducted on February 18, 1998. An evaluation of historical documentation indicated that plutonium should not be and depleted uranium could not be present at levels significantly above background as the result of test animals being penned at the site. The samples were analyzed for isotopic plutonium using method NAS-NS-3058. The results of the analysis indicated that plutonium levels of the feces and surface soil were not significantly elevated above background.« less
Why is weapons grade plutonium more hazardous to work with than highly enriched uranium?
Cournoyer, Michael E.; Costigan, Stephen A.; Schake, Bradley S.
2015-08-01
Highly Enriched Uranium and Weapons grade plutonium have assumed positions of dominant importance among the actinide elements because of their successful uses as explosive ingredients in nuclear weapons and the place they hold as key materials in the development of industrial use of nuclear power. While most chemists are familiar with the practical interest concerning HEU and WG Pu, fewer know the subtleties among their hazards. In this study, a primer is provided regarding the hazards associated with working with HEU and WG Pu metals and oxides. The care that must be taken to safely handle these materials is emphasizedmore » and the extent of the hazards is described. The controls needed to work with HEU and WG Pu metals and oxides are differentiated. Given the choice, one would rather work with HEU metal and oxides than WG Pu metal and oxides.« less
Why is weapons grade plutonium more hazardous to work with than highly enriched uranium?
DOE Office of Scientific and Technical Information (OSTI.GOV)
Cournoyer, Michael E.; Costigan, Stephen A.; Schake, Bradley S.
Highly Enriched Uranium and Weapons grade plutonium have assumed positions of dominant importance among the actinide elements because of their successful uses as explosive ingredients in nuclear weapons and the place they hold as key materials in the development of industrial use of nuclear power. While most chemists are familiar with the practical interest concerning HEU and WG Pu, fewer know the subtleties among their hazards. In this study, a primer is provided regarding the hazards associated with working with HEU and WG Pu metals and oxides. The care that must be taken to safely handle these materials is emphasizedmore » and the extent of the hazards is described. The controls needed to work with HEU and WG Pu metals and oxides are differentiated. Given the choice, one would rather work with HEU metal and oxides than WG Pu metal and oxides.« less
NASA Astrophysics Data System (ADS)
Chung, Brandon W.; Erler, Robert G.; Teslich, Nick E.
2016-05-01
Nuclear forensics requires accurate quantification of discriminating microstructural characteristics of the bulk nuclear material to identify its process history and provenance. Conventional metallographic preparation techniques for bulk plutonium (Pu) and uranium (U) metals are limited to providing information in two-dimension (2D) and do not allow for obtaining depth profile of the material. In this contribution, use of dual-beam focused ion-beam/scanning electron microscopy (FIB-SEM) to investigate the internal microstructure of bulk Pu and U metals is demonstrated. Our results demonstrate that the dual-beam methodology optimally elucidate microstructural features without preparation artifacts, and the three-dimensional (3D) characterization of inner microstructures can reveal salient microstructural features that cannot be observed from conventional metallographic techniques. Examples are shown to demonstrate the benefit of FIB-SEM in improving microstructural characterization of microscopic inclusions, particularly with respect to nuclear forensics.
Chung, Brandon W.; Erler, Robert G.; Teslich, Nick E.
2016-03-03
Nuclear forensics requires accurate quantification of discriminating microstructural characteristics of the bulk nuclear material to identify its process history and provenance. Conventional metallographic preparation techniques for bulk plutonium (Pu) and uranium (U) metals are limited to providing information in two-dimension (2D) and do not allow for obtaining depth profile of the material. In this contribution, use of dual-beam focused ion-beam/scanning electron microscopy (FIB-SEM) to investigate the internal microstructure of bulk Pu and U metals is demonstrated. Our results demonstrate that the dual-beam methodology optimally elucidate microstructural features without preparation artifacts, and the three-dimensional (3D) characterization of inner microstructures can revealmore » salient microstructural features that cannot be observed from conventional metallographic techniques. As a result, examples are shown to demonstrate the benefit of FIB-SEM in improving microstructural characterization of microscopic inclusions, particularly with respect to nuclear forensics.« less
Oxygen diffusion model of the mixed (U,Pu)O2 ± x: Assessment and application
NASA Astrophysics Data System (ADS)
Moore, Emily; Guéneau, Christine; Crocombette, Jean-Paul
2017-03-01
The uranium-plutonium (U,Pu)O2 ± x mixed oxide (MOX) is used as a nuclear fuel in some light water reactors and considered for future reactor generations. To gain insight into fuel restructuring, which occurs during the fuel lifetime as well as possible accident scenarios understanding of the thermodynamic and kinetic behavior is crucial. A comprehensive evaluation of thermo-kinetic properties is incorporated in a computational CALPHAD type model. The present DICTRA based model describes oxygen diffusion across the whole range of plutonium, uranium and oxygen compositions and temperatures by incorporating vacancy and interstitial migration pathways for oxygen. The self and chemical diffusion coefficients are assessed for the binary UO2 ± x and PuO2 - x systems and the description is extended to the ternary mixed oxide (U,Pu)O2 ± x by extrapolation. A simulation to validate the applicability of this model is considered.
Flammability Analysis For Actinide Oxides Packaged In 9975 Shipping Containers
DOE Office of Scientific and Technical Information (OSTI.GOV)
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 ofmore » 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.« less
Verification study of an emerging fire suppression system
Cournoyer, Michael E.; Waked, R. Ryan; Granzow, Howard N.; ...
2016-01-01
Self-contained fire extinguishers are a robust, reliable and minimally invasive means of fire suppression for gloveboxes. Moreover, plutonium gloveboxes present harsh environmental conditions for polymer materials; these include radiation damage and chemical exposure, both of which tend to degrade the lifetime of engineered polymer components. Several studies have been conducted to determine the robustness of selfcontained fire extinguishers in plutonium gloveboxes in a nuclear facility, verification tests must be performed. These tests include activation and mass loss calorimeter tests. In addition, compatibility issues with chemical components of the self-contained fire extinguishers need to be addressed. Our study presents activation andmore » mass loss calorimeter test results. After extensive studies, no critical areas of concern have been identified for the plutonium glovebox application of Fire Foe™, except for glovebox operations that use large quantities of bulk plutonium or uranium metal such as metal casting and pyro-chemistry operations.« less
PROCESS OF REDUCING PLUTONIUM TO TETRAVALENT TRIVALENT STATE
Mastick, D.F.
1960-05-10
The reduction of hexavalent and tetravalert plutonium ions to the trivalent state in strong nitric acid can be accomplished with hydrogen peroxide. The trivalent state may be stabilized as a precipitate by including oxalate or fluoride ions in the solution. The acid should be strong to encourage the reduction from the plutonyl to the trivalent state (and discourage the opposed oxidation reaction) and prevent the precipitation of plutonium peroxide, although the latter may be digested by increasing the acid concentration. Although excess hydrogen peroxide will oxidize plutonlum to the plutonyl state, complete reduction is insured by gently warming the solution to break down such excess H/ sub 2/O/sub 2/. The particular advantage of hydrogen peroxide as a reductant lies in the precipitation technique, where it introduces no contaminating ions. The process is adaptable to separate plutonium from uranium and impurities by proper adjustment of the sequence of insoluble anion additions and the hydrogen peroxide addition.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hurd, J.R.
The active-passive shuffler installed and certified a few years ago in Los Alamos National Laboratory`s plutonium facility has now been calibrated for different matrices to measure Waste Isolation Pilot Plant (WIPP)-destined transuranic (TRU)-waste. Little or no data presently exist for these types of measurements in plant environments where there may be sudden large changes in the neutron background radiation which causes distortions in the results. Measurements and analyses of twenty-two 55-gallon drums, consisting of mixtures of varying quantities of uranium and plutonium, have been recently completed at the plutonium facility. The calibration and measurement techniques, including the method used tomore » separate out the plutonium component, will be presented and discussed. Particular attention will be directed to those problems identified as arising from the plant environment. The results of studies to quantify the distortion effects in the data will be presented. Various solution scenarios will be indicated, along with those adopted here.« less
Verification study of an emerging fire suppression system
DOE Office of Scientific and Technical Information (OSTI.GOV)
Cournoyer, Michael E.; Waked, R. Ryan; Granzow, Howard N.
Self-contained fire extinguishers are a robust, reliable and minimally invasive means of fire suppression for gloveboxes. Moreover, plutonium gloveboxes present harsh environmental conditions for polymer materials; these include radiation damage and chemical exposure, both of which tend to degrade the lifetime of engineered polymer components. Several studies have been conducted to determine the robustness of selfcontained fire extinguishers in plutonium gloveboxes in a nuclear facility, verification tests must be performed. These tests include activation and mass loss calorimeter tests. In addition, compatibility issues with chemical components of the self-contained fire extinguishers need to be addressed. Our study presents activation andmore » mass loss calorimeter test results. After extensive studies, no critical areas of concern have been identified for the plutonium glovebox application of Fire Foe™, except for glovebox operations that use large quantities of bulk plutonium or uranium metal such as metal casting and pyro-chemistry operations.« less
METHOD OF SEPARATING Pu FROM METATHESIZED BiPO$sub 4$ CARRIER
Knox, W.J.; Thompson, S.G.
1960-05-31
A process is given for separating uranium, neptunium, and/or plutonium from a bismuth hydroxide carrier by selective dissolution of these actinides with nitric acid of a concentration of from 0.05 to 0.5N.
2007-08-01
Characterization (OHM 1998). From the plot, it is clear that the HEU dominates DU in the overall isotopic characteristic. Among the three uranium ... isotopes , 234U comprised about 90 % of the total activity, including naturally-occurring background sources. However, in comparison to the WGP, uranium ...listed for a few sampling locations that had isotopic plutonium analysis of wipe samples. Figure A-19 contains a scatterplot of the paired Table 4-13
Extraction of neptunium by trilaurylamine
DOE Office of Scientific and Technical Information (OSTI.GOV)
Patil, S.K.; Swarup, R.; Ramaniah, M.V.
1972-07-01
Trilaurylamine (TLA) is considered as useful solvent for the final purification of plutonium and neptunium. As TLA is considered as an alternate possible extractant for the final purification of plutonium and neptunium at Tarapur Reprocessing Plant under construction, it was considered necessary to study the optimum conditions for the extraction of neptunium using TLA.
The efficacy of denaturing actinide elements as a means of decreasing materials attractiveness
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hase, K.R.; Bathke, C.G.; Ebbinghaus, B.B.
2013-07-01
This study considers the concept of denaturing as applied to the actinide elements present in spent fuel as a means to reduce materials attractiveness. Highly attractive materials generally have low values of bare critical mass, heat content, and dose. To denature an attractive element, its spent-fuel isotopic composition (isotopic vector) is intentionally modified by introducing sufficient quantities of a significantly less attractive isotope to dilute the concentration of a highly attractive isotope so that the overall attractiveness of the element is reduced. The authors used FOM (Figure of Merit) formula as the material attractiveness metric for their parametric determination ofmore » the attractiveness of the Pu and U. Materials attractiveness needs to be considered in three distinct phases in the process to construct a nuclear explosive device (NED): the acquisition phase, processing phase, and utilization phase. The results show that denaturing uranium with {sup 238}U is actually an effective means of reducing the attractiveness. For uranium with a large minority of {sup 235}U, a mixture of 80% {sup 238}U to 20% {sup 235}U is required to reduce the attractiveness to low. For uranium with a large concentration of {sup 233}U, a mixture of 88% {sup 238}U to 12% {sup 233}U is required to reduce the attractiveness to low. The results also show that denaturing plutonium with {sup 238}Pu is less effective than denaturing uranium with {sup 238}U. Using {sup 238}Pu as the denaturing agent would require 80% or more by mass in order to reduce the attractiveness to low. No amount of {sup 240}Pu is enough to reduce the plutonium attractiveness below medium. The combination of {sup 238}Pu and {sup 240}Pu would require approximately 70% {sup 238}Pu and 25% {sup 240}Pu by mass to reduce the plutonium attractiveness to low.« less
Nuclear shape evolution based on microscopic level densities
Ward, D. E.; Carlsson, B. G.; Døssing, T.; ...
2017-02-27
Here, by combining microscopically calculated level densities with the Metropolis walk method, we develop a consistent framework for treating the energy and angular-momentum dependence of the nuclear shape evolution in the fission process. For each nucleus under consideration, the level density is calculated microscopically for each of more than five million shapes with a recently developed combinatorial method. The method employs the same single-particle levels as those used for the extraction of the pairing and shell contributions to the macroscopic-microscopic deformation-energy surface. Containing no new parameters, the treatment is suitable for elucidating the energy dependence of the dynamics of warmmore » nuclei on pairing and shell effects. It is illustrated for the fission fragment mass distribution for several uranium and plutonium isotopes of particular interest.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Liezers, Martin; Olsen, Khris B.; Mitroshkov, Alexandre V.
2010-08-11
The most time consuming process in uranium or plutonium isotopic analyses is performing the requisite chromatographic separation of the actinides. Filament preparation for thermal ionization (TIMS) adds further delays, but is generally accepted due to the unmatched performance in trace isotopic analyses. Advances in Multi-Collector Inductively Coupled Plasma Mass Spectrometry (MC-ICP-MS) are beginning to rival the performance of TIMS. Methods, such as Electrochemically Modulated Separations (EMS) can efficiently pre-concentrate U or Pu quite selectively from small solution volumes in a matrix of 0.5 M nitric acid. When performed in-line with ICP-MS, the rapid analyte release from the electrode is fast,more » and large transient analyte signal enhancements of >100 fold can be achieved as compared to more conventional continuous nebulization of the original starting solution. This makes the approach ideal for very low level isotope ratio measurements. In this paper, some aspects of EMS performance are described. These include low level Pu isotope ratio behavior versus concentration by MC-ICP-MS and uranium rejection characteristics that are also important for reliable low level Pu isotope ratio determinations.« less
Fusion of acid oxides for potentially radiation-resistant waste forms
DOE Office of Scientific and Technical Information (OSTI.GOV)
Herrick, C.C.; Penneman, R.A.
1983-02-01
Skull melting of groups VA and VB acid oxides with alkali metal oxides and urania leads to compounds with a good ability to retain radionuclides and establishes immunity to radiation damage. Substitution of neptunium and plutonium for uranium should not diminish these desirable properties. For hexavalent transplutonic elements, even at high oxygen fugacities and oxide activities, acid character losses and the reducing nature of radiation suggest the lower valences (III and IV) will be the stable states. Plutonium becomes the pivotal radionuclide when valence stability in a radiation field is considered.
METHOD OF MAKING ALLOYS OF BERYLLIUM WITH PLUTONIUM AND THE LIKE
Runnals, O.J.C.
1959-02-24
The production of alloys of beryllium with one or more of the metals uranium, plutonium, actinium, americium, curium, thorium, and cerium are described. A halide salt of the metal to be alloyed with the beryllium is heated at 1300 deg C in the presence of beryllium to reduce the halide to metal and cause the latter to alloy directly with the beryllium. Although the heavy metal halides are more stable, thermodynamically, than the beryllium halides, the reducing reaction proceeds to completion if the beryllium halide product is continuously removed by vacuum distillation.
FMDP reactor alternative summary report. Volume 1 - existing LWR alternative
DOE Office of Scientific and Technical Information (OSTI.GOV)
Greene, S.R.; Bevard, B.B.
1996-10-07
Significant quantities of weapons-usable fissile materials [primarily plutonium and highly enriched uranium (HEU)] are becoming surplus to national defense needs in both the United States and Russia. These stocks of fissile materials pose significant dangers to national and international security. The dangers exist not only in the potential proliferation of nuclear weapons but also in the potential for environmental, safety, and health (ES&H) consequences if surplus fissile materials are not properly managed. This document summarizes the results of analysis concerned with existing light water reactor plutonium disposition alternatives.
Nuclear Fuel Reprocessing: U.S. Policy Development
2006-11-29
to the chemical separation of fissionable uranium and plutonium from irradiated nuclear fuel. The World War II-era Manhattan Project developed...created the Atomic Energy Commission (AEC) and transferred production and control of fissionable materials from the Manhattan Project . As the exclusive
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bathke, C. G.; Ebbinghaus, Bartley B.; Collins, Brian A.
2012-08-29
We must anticipate that the day is approaching when details of nuclear weapons design and fabrication will become common knowledge. On that day we must be particularly certain that all special nuclear materials (SNM) are adequately accounted for and protected and that we have a clear understanding of the utility of nuclear materials to potential adversaries. To this end, this paper examines the attractiveness of materials mixtures containing SNM and alternate nuclear materials associated with the plutonium-uranium reduction extraction (Purex), uranium extraction (UREX), coextraction (COEX), thorium extraction (THOREX), and PYROX (an electrochemical refining method) reprocessing schemes. This paper provides amore » set of figures of merit for evaluating material attractiveness that covers a broad range of proliferant state and subnational group capabilities. The primary conclusion of this paper is that all fissile material must be rigorously safeguarded to detect diversion by a state and must be provided the highest levels of physical protection to prevent theft by subnational groups; no 'silver bullet' fuel cycle has been found that will permit the relaxation of current international safeguards or national physical security protection levels. The work reported herein has been performed at the request of the U.S. Department of Energy (DOE) and is based on the calculation of 'attractiveness levels' that are expressed in terms consistent with, but normally reserved for, the nuclear materials in DOE nuclear facilities. The methodology and findings are presented. Additionally, how these attractiveness levels relate to proliferation resistance and physical security is discussed.« less
Yiin, James H; Anderson, Jeri L; Bertke, Stephen J; Tollerud, David J
2018-05-09
To examine dose-response relationships between internal uranium exposures and select outcomes among a cohort of uranium enrichment workers. Cox regression was conducted to examine associations between selected health outcomes and cumulative internal uranium with consideration for external ionizing radiation, work-related medical X-rays and contaminant radionuclides technetium ( 99 Tc) and plutonium ( 239 Pu) as potential confounders. Elevated and monotonically increasing mortality risks were observed for kidney cancer, chronic renal diseases, and multiple myeloma, and the association with internal uranium absorbed organ dose was statistically significant for multiple myeloma. Adjustment for potential confounders had minimal impact on the risk estimates. Kidney cancer, chronic renal disease, and multiple myeloma mortality risks were elevated with increasing internal uranium absorbed organ dose. The findings add to evidence of an association between internal exposure to uranium and cancer. Future investigation includes a study of cancer incidence in this cohort. © 2018 Wiley Periodicals, Inc.
SOLVENT EXTRACTION PROCESS FOR URANIUM RECOVERY
Clark, H.M.; Duffey, D.
1958-06-17
A process is described for extracting uranium from uranium ore, wherein the uranium is substantially free from molybdenum contamination. In a solvent extraction process for recovering uranium, uranium and molybdenum ions are extracted from the ore with ether under high acidity conditions. The ether phase is then stripped with water at a lower controiled acidity, resaturated with salting materials such as sodium nitrate, and reextracted with the separation of the molybdenum from the uranium without interference from other metals that have been previously extracted.
NASA Astrophysics Data System (ADS)
Dacheux, N.; Podor, R.; Brandel, V.; Genet, M.
1998-02-01
In the framework of nuclear waste management aiming at the research of a storage matrix, the chemistry of thorium phosphates has been completely re-examined. In the ThO 2-P 2O 5 system a new compound thorium phosphate-diphosphate Th 4(PO 4) 4P 2O 7 has been synthesized. The replacement of Th 4+ by a smaller cation like U 4+ and Pu 4+ in the thorium phosphate-diphosphate (TPD) lattice has been achieved. Th 4- xU x(PO 4) 4P 2O 7 and Th 4- xPu x(PO 4) 4P 2O 7 solid solutions have been synthesized through wet and dry processes with 0< x<3.0 for uranium and 0< x<1.0 for plutonium. From the variation of the unit cell parameters, an upper x value equal to 1.67 has been estimated for the thorium-plutonium (IV) phosphate-diphosphate solid solutions. Two other tetravalent cations, Ce 4+ and Zr 4+, cannot be incorporated in the TPD lattice: cerium (IV) because of its reduction into Ce (III) at high temperature, and zirconium probably because of its too small radius compared to thorium.
20. AERIAL VIEW OF THE ROCKY FLATS PLANT LOOKING NORTHEAST. ...
20. AERIAL VIEW OF THE ROCKY FLATS PLANT LOOKING NORTHEAST. THE PLANT WAS COMPOSED OF FOUR WIDELY SEPARATED AREAS, EACH ONE PERFORMING A DIFFERENT TYPE OF WORK. PLANT A (44), SOUTHWEST, FABRICATED PARTS FROM DEPLETED URANIUM, PLANT B (81), SOUTH, WAS ENRICHED URANIUM OPERATIONS, PLANT C (71), NORTH, PLUTONIUM OPERATIONS, AND PLANT D (91), EAST, WAS FINAL ASSEMBLY, SHIPPING AND RECEIVING (2/6/66). - Rocky Flats Plant, Bounded by Indiana Street & Routes 93, 128 & 72, Golden, Jefferson County, CO
SEPARATION PROCESS FOR TRANSURANIC ELEMENT AND COMPOUNDS THEREOF
Calvin, M.
1958-10-14
S> A process is presented for the separation of pluto nium from uranium and fission products in an aqueous acidic solution by use of a chelating agent. The plutonium is maintained in the tetravalent state and the uranium in the hexavalent state, and the acidic concentration is adjusted to about 1 N bar. The aqueous solution is then contacted with a water-immiscible organic solvent solution and the chelating agent. The chelating agents covered by this invention comprise a group of compounds characterized as fluorinated beta-diketones.
Nuclear fuel element with axially aligned fuel pellets and fuel microspheres therein
Sease, J.D.; Harrington, F.E.
1973-12-11
Elongated single- and multi-region fuel elements are prepared by replacing within a cladding container a coarse fraction of fuel material which includes plutonium and uranium in the appropriate regions of the fuel element and then infiltrating with vibration a fine-sized fraction of uranium-containing microspheres throughout all interstices in the coarse material in a single loading. The fine, rigid material defines a thin annular layer between the coarse fraction and the cladding to reduce adverse mechanical and chemical interactions. (Official Gazette)
Crystalline matrices for the immobilization of plutonium and actinides
DOE Office of Scientific and Technical Information (OSTI.GOV)
Anderson, E.B.; Burakov, E.E.; Galkin, Ya.B.
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 pressingmore » 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.« less
NASA Astrophysics Data System (ADS)
Clark, David L.; Hecker, Siegfried S.; Jarvinen, Gordon D.; Neu, Mary P.
The element plutonium occupies a unique place in the history of chemistry, physics, technology, and international relations. After the initial discovery based on submicrogram amounts, it is now generated by transmutation of uranium in nuclear reactors on a large scale, and has been separated in ton quantities in large industrial facilities. The intense interest in plutonium resulted fromthe dual-use scenario of domestic power production and nuclear weapons - drawing energy from an atomic nucleus that can produce a factor of millions in energy output relative to chemical energy sources. Indeed, within 5 years of its original synthesis, the primary use of plutonium was for the release of nuclear energy in weapons of unprecedented power, and it seemed that the new element might lead the human race to the brink of self-annihilation. Instead, it has forced the human race to govern itself without resorting to nuclear war over the past 60 years. Plutonium evokes the entire gamut of human emotions, from good to evil, from hope to despair, from the salvation of humanity to its utter destruction. There is no other element in the periodic table that has had such a profound impact on the consciousness of mankind.
Aqueous Chloride Operations Overview: Plutonium and Americium Purification/Recovery
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gardner, Kyle Shelton; Kimball, David Bryan; Skidmore, Bradley Evan
These are a set of slides intended for an information session as part of recruiting activities at Brigham Young University. It gives an overview of aqueous chloride operations, specifically on plutonium and americium purification/recovery. This presentation details the steps taken perform these processes, from plutonium size reduction, dissolution, solvent extraction, oxalate precipitation, to calcination. For americium recovery, it details the CLEAR (chloride extraction and actinide recovery) Line, oxalate precipitation and calcination.
Neutron Based Non-Destructive Assay (NDA) Measurement Systems for Safeguard
DOE Office of Scientific and Technical Information (OSTI.GOV)
Swinhoe, Martyn Thomas
2017-09-21
The objectives of this project are to introduce the assay methods for plutonium measurements using the HLNC; introduce the assay method for bulk uranium measurements using the AWCC; and introduce the assay method for fuel assembly measurements using the UNCL.
Lemons, B; Khaing, H; Ward, A; Thakur, P
2018-06-01
A new sequential separation method for the determination of polonium and actinides (Pu, Am and U) in drinking water samples has been developed that can be used for emergency response or routine water analyses. For the first time, the application of TEVA chromatography column in the sequential separation of polonium and plutonium has been studied. This method utilizes a rapid Fe +3 co-precipitation step to remove matrix interferences, followed by plutonium oxidation state adjustment to Pu 4+ and an incubation period of ~ 1 h at 50-60 °C to allow Po 2+ to oxidize to Po 4+ . The polonium and plutonium were then separated on a TEVA column, while separation of americium from uranium was performed on a TRU column. After separation, polonium was micro-precipitated with copper sulfide (CuS), while actinides were micro co-precipitated using neodymium fluoride (NdF 3 ) for counting by the alpha spectrometry. The method is simple, robust and can be performed quickly with excellent removal of interferences, high chemical recovery and very good alpha peak resolution. The efficiency and reliability of the procedures were tested by using spiked samples. The effect of several transition metals (Cu 2+ , Pb 2+ , Fe 3+ , Fe 2+ , and Ni 2+ ) on the performance of this method were also assessed to evaluate the potential matrix effects. Studies indicate that presence of up to 25 mg of these cations in the samples had no adverse effect on the recovery or the resolution of polonium alpha peaks. Copyright © 2018 Elsevier Ltd. All rights reserved.
Mayer, S.W.
1962-11-13
This invention relates to a nuciear reactor fuel composition comprising (1) from about 0.01 to about 50 wt.% based on the total weight of said composition of at least one element selected from the class consisting of uranium, thorium, and plutonium, wherein said eiement is present in the form of at least one component selected from the class consisting of oxides, halides, and salts of oxygenated anions, with components comprising (2) at least one member selected from the class consisting of (a) sulfur, wherein the sulfur is in the form of at least one entity selected irom the class consisting of oxides of sulfur, metal sulfates, metal sulfites, metal halosulfonates, and acids of sulfur, (b) halogen, wherein said halogen is in the form of at least one compound selected from the class of metal halides, metal halosulfonates, and metal halophosphates, (c) phosphorus, wherein said phosphorus is in the form of at least one constituent selected from the class consisting of oxides of phosphorus, metal phosphates, metal phosphites, and metal halophosphates, (d) at least one oxide of a member selected from the class consisting of a metal and a metalloid wherein said oxide is free from an oxide of said element in (1); wherein the amount of at least one member selected from the class consisting of halogen and sulfur is at least about one at.% based on the amount of the sum of said sulfur, halogen, and phosphorus atom in said composition; and wherein the amount of said 2(a), 2(b) and 2(c) components in said composition which are free from said elements of uranium, thorium, arid plutonium, is at least about 60 wt.% based on the combined weight of the components of said composition which are free from said elements of uranium, thorium, and plutonium. (AEC)
DOE Office of Scientific and Technical Information (OSTI.GOV)
Reed, Donald Timothy; Borkowski, Marian; Lucchini, Jean - Francois
2010-12-10
The fate and potential mobility of multivalent actinides in the subsurface is receiving increased attention as the DOE looks to cleanup the many legacy nuclear waste sites and associated subsurface contamination. Plutonium, uranium and neptunium are the near-surface multivalent contaminants of concern and are also key contaminants for the deep geologic disposal of nuclear waste. Their mobility is highly dependent on their redox distribution at their contamination source as well as along their potential migration pathways. This redox distribution is often controlled, especially in the near-surface where organic/inorganic contaminants often coexist, by the direct and indirect effects of microbial activity.more » Under anoxic conditions, indirect and direct bioreduction mechanisms exist that promote the prevalence of lower-valent species for multivalent actinides. Oxidation-state-specific biosorption is also an important consideration for long-term migration and can influence oxidation state distribution. Results of ongoing studies to explore and establish the oxidation-state specific interactions of soil bacteria (metal reducers and sulfate reducers) as well as halo-tolerant bacteria and Archaea for uranium, neptunium and plutonium will be presented. Enzymatic reduction is a key process in the bioreduction of plutonium and uranium, but co-enzymatic processes predominate in neptunium systems. Strong sorptive interactions can occur for most actinide oxidation states but are likely a factor in the stabilization of lower-valent species when more than one oxidation state can persist under anaerobic microbiologically-active conditions. These results for microbiologically active systems are interpreted in the context of their overall importance in defining the potential migration of multivalent actinides in the subsurface.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hay, M.; Coleman, C.; Diprete, D.
SRNL analyzed samples from Tank 38H and Tank 43H to support ECP and CCP. The total uranium in the Tank 38H surface sample was 41.3 mg/L while the sub-surface sample was 43.5 mg/L. The Tank 43H samples contained total uranium concentrations of 28.5 mg/L in the surface sample and 28.1 mg/L in the sub-surface sample. The U-235 percentage ranged from 0.62% to 0.63% for the Tank 38H samples and Tank 43H samples. The total uranium and percent U-235 results in the table appear slightly lower than recent Tank 38H and Tank 43H uranium measurements. The plutonium results in the tablemore » show a large difference between the surface and sub-surface sample concentrations for Tank 38H. The Tank 43H plutonium results closely match the range of values measured on previous samples. The Cs-137 results for the Tank 38H surface and sub-surface samples show similar concentrations slightly higher than the concentrations measured in recent samples. The Cs-137 results for the two Tank 43H samples also show similar concentrations within the range of values measured on previous samples. The four samples show silicon concentrations somewhat lower than the previous samples with values ranging from 124 to 168 mg/L.« less
The Manhattan Project; A very brief introduction to the physics of nuclear weapons
NASA Astrophysics Data System (ADS)
Reed, B. Cameron
2017-05-01
The development of nuclear weapons by the Manhattan Project during World War II was one of the most dramatic scientific/technological episodes in human history. This book, prepared by a recognized expert on the Manhattan Project, offers a concise survey of the essential physics concepts underlying fission weapons. The text describes the energetics and timescales of fast-neutron chain reactions, why only certain isotopes of uranium and plutonium are suitable for use in fission weapons, how critical mass and bomb yield can be estimated, how the efficiency of nuclear weapons can be enhanced, how the fissile forms of uranium and plutonium were obtained, some of the design details of the 'Little Boy' and 'Fat Man' bombs, and some of the thermal, shock, and radiation effects of nuclear weapons. Calculation exercises are provided, and a Bibliography lists authoritative print and online sources of information for readers who wish to pursue more detailed study of this fascinating topic.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Nelson, A. J.; Percher, C. M.; Zywiec, W. J.
This report presents the final design (CED-2) for IER-297, and focuses on 15 critical configurations using highly enriched uranium (HEU) Jemima plates moderated by polyethylene with and without hafnium diluent. The goal of the U.S. Nuclear Criticality Safety Program’s Thermal/Epithermal eXperiments (TEX) is to design and conduct new critical experiments to address high priority nuclear data needs from the nuclear criticality safety and nuclear data communities, with special emphasis on intermediate energy (0.625 eV – 100 keV) assemblies that can be easily modified to include various high priority diluent materials. The TEX (IER 184) CED-1 Report [1], completed in 2012,more » demonstrated the feasibility of meeting the TEX goals with two existing NCSP fissile assets, plutonium Zero Power Physics Reactor (ZPPR) plates and highly enriched uranium (HEU) Jemima plates. The first set of TEX experiments will focus on using the plutonium ZPPR plates with polyethylene moderator and tantalum diluents.« less
Leo Szilard Lectureship Award Talk: Controlling and eliminating nuclear-weapon materials
NASA Astrophysics Data System (ADS)
von Hippel, Frank
2010-02-01
Fissile material -- in practice plutonium and highly enriched uranium (HEU) -- is the essential ingredient in nuclear weapons. Controlling and eliminating fissile material and the means of its production is therefore the common denominator for nuclear disarmament, nuclear non-proliferation and the prevention of nuclear terrorism. From a fundamentalist anti-nuclear-weapon perspective, the less fissile material there is and the fewer locations where it can be found, the safer a world we will have. A comprehensive fissile-material policy therefore would have the following elements: *Consolidation of all nuclear-weapon-usable materials at a minimum number of high-security sites; *A verified ban on the production of HEU and plutonium for weapons; *Minimization of non-weapon uses of HEU and plutonium; and *Elimination of all excess stocks of plutonium and HEU. There is activity on all these fronts but it is not comprehensive and not all aspects are being pursued vigorously or competently. It is therefore worthwhile to review the situation. )
DOE Office of Scientific and Technical Information (OSTI.GOV)
Mechelynck, Ph.
1958-07-15
After an examination of the different processes for the treatment of uranium minerals, it is concluded that the extraction of uranium by ion exchange is not applicable to hydrochloric acid solutions of phosphates. A sulfuric or phosphoric solution can be used. For solvent extraction of uranium, sulfuric or phosphoric solutions are the best, but hydrochloric solutions can be used. The cost of the solvents used would determine the cost of the operation. It is necessary, in the case of liquid-liquid extraction, to filter or decant the solution before extraction. (tr-auth)
U.S. program assessing nuclear waste disposal in space - A status report
NASA Technical Reports Server (NTRS)
Rice, E. E.; Priest, C. C.; Friedlander, A. L.
1980-01-01
Various concepts for the space disposal of nuclear waste are discussed, with attention given to the destinations now being considered (high earth orbit, lunar orbit, lunar surface, solar orbit, solar system escape, sun). Waste mixes are considered in the context of the 'Purex' (Plutonium and Uranium extraction) process and the potential forms for nuclear waste disposal (ORNL cermet, Boro-silicate glass, Metal matrix, Hot-pressed supercalcine) are described. Preliminary estimates of the energy required and the cost surcharge needed to support the space disposal of nuclear waste are presented (8 metric tons/year, requiring three Shuttle launches). When Purex is employed, the generated electrical energy needed to support the Shuttle launches is shown to be less than 1%, and the projected surcharge to electrical users is shown to be slightly more than two mills/kW-hour.
SOLVENT EXTRACTION PROCESS FOR URANIUM FROM CHLORIDE SOLUTIONS
Blake, C.A. Jr.; Brown, K.B.; Horner, D.E.
1960-05-24
An improvement was made in a uranium extraction process wherein the organic extractant is a phosphine oxide. An aqueous solution containing phosphate ions or sulfate ions together with uranium is provided with a source of chloride ions during the extraction step. The presence of the chloride ions enables a phosphine oxide to extract uranium in the presence of strong uranium- complexing ions such as phosphate or sulfate ions.
Method of making alloys of beryllium with plutonium and the like
Runnals, O J.C.
1959-02-24
The production or alloys of beryllium with one or more of the metals uranium, plutonium, actinium, americium, curium, thorium, and cerium is described. A halide salt or the metal to be alloyed with the beryllium is heated at l3O0 deg C in the presence of beryllium to reduce the halide to metal and cause the latter to alloy directly with the beryllium. Although the heavy metal halides are more stable, thermodynamically, than the beryllium halides, the reducing reaction proceeds to completion if the beryllium halide product is continuously removed by vacuum distillation.
CONCENTRATION OF Pu USING OXALATE TYPE CARRIER
Ritter, D.M.; Black, R.P.S.
1960-04-19
A method is given for dissolving and reprecipitating an oxalate carrier precipitate in a carrier precipitation process for separating and recovering plutonium from an aqueous solution. Uranous oxalate, together with plutonium being carried thereby, is dissolved in an aqueous alkaline solution. Suitable alkaline reagents are the carbonates and oxulates of the alkali metals and ammonium. An oxidizing agent selected from hydroxylamine and hydrogen peroxide is then added to the alkaline solution, thereby oxidizing uranium to the hexavalent state. The resulting solution is then acidified and a source of uranous ions provided in the acidified solution, thereby forming a second plutoniumcarrying uranous oxalate precipitate.
Measurements of plutonium, 237Np, and 137Cs in the BCR 482 lichen reference material
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lavelle, Kevin B.; Miller, Jeffrey L.; Hanson, Susan K.
Select anthropogenic radionuclides were measured in lichen reference material, BCR 482. This material was originally collected in Axalp, Switzerland in 1991 and is composed of the epiphytic lichen Pseudevernia furfuracea. Samples from three separate bottles of BCR 482 were analyzed for uranium, neptunium, and plutonium isotopes by inductively coupled plasma mass spectrometry (ICP-MS) and analyzed for cesium-137 by gamma-ray spectrometry. The isotopic composition of the radionuclides measured in BCR 482 suggests contributions from both global fallout resulting from historical nuclear weapons testing and more volatile materials released following the Chernobyl accident.
Measurements of plutonium, 237Np, and 137Cs in the BCR 482 lichen reference material
Lavelle, Kevin B.; Miller, Jeffrey L.; Hanson, Susan K.; ...
2015-10-01
Select anthropogenic radionuclides were measured in lichen reference material, BCR 482. This material was originally collected in Axalp, Switzerland in 1991 and is composed of the epiphytic lichen Pseudevernia furfuracea. Samples from three separate bottles of BCR 482 were analyzed for uranium, neptunium, and plutonium isotopes by inductively coupled plasma mass spectrometry (ICP-MS) and analyzed for cesium-137 by gamma-ray spectrometry. The isotopic composition of the radionuclides measured in BCR 482 suggests contributions from both global fallout resulting from historical nuclear weapons testing and more volatile materials released following the Chernobyl accident.
Remediation of uranium contaminated soils with bicarbonate extraction and microbial U(VI) reduction
Philips , Elizabeth J.P.; Landa, Edward R.; Lovely, Derek R.
1995-01-01
A process for concentrating uranium from contaminated soils in which the uranium is first extracted with bicarbonate and then the extracted uranium is precipitated with U(VI)-reducing microorganisms was evaluated for a variety of uranuum-contaminated soils. Bicarbonate (100 mM) extracted 20–94% of the uranium that was extracted with nitric acid. The U(VI)-reducing microorganism,Desulfovibrio desulfuricans reduced the U(VI) to U(IV) in the bicarbonate extracts. In some instances unidentified dissolved extracted components, presumably organics, gave the extract a yellow color and inhibited U(VI) reduction and/or the precipitation of U(IV). Removal of the dissolved yellow material with the addition of hydrogen peroxide alleviated this inhibition. These results demonstrate that bicarbonate extraction of uranium from soil followed by microbial U(VI) reduction might be an effective mechanism for concentrating uranium from some contaminated soils.
NASA Astrophysics Data System (ADS)
Goddard, Braden
The ability of inspection agencies and facility operators to measure powders containing several actinides is increasingly necessary as new reprocessing techniques and fuel forms are being developed. These powders are difficult to measure with nondestructive assay (NDA) techniques because neutrons emitted from induced and spontaneous fission of different nuclides are very similar. A neutron multiplicity technique based on first principle methods was developed to measure these powders by exploiting isotope-specific nuclear properties, such as the energy-dependent fission cross sections and the neutron induced fission neutron multiplicity. This technique was tested through extensive simulations using the Monte Carlo N-Particle eXtended (MCNPX) code and by one measurement campaign using the Active Well Coincidence Counter (AWCC) and two measurement campaigns using the Epithermal Neutron Multiplicity Counter (ENMC) with various (alpha,n) sources and actinide materials. Four potential applications of this first principle technique have been identified: (1) quantitative measurement of uranium, neptunium, plutonium, and americium materials; (2) quantitative measurement of mixed oxide (MOX) materials; (3) quantitative measurement of uranium materials; and (4) weapons verification in arms control agreements. This technique still has several challenges which need to be overcome, the largest of these being the challenge of having high-precision active and passive measurements to produce results with acceptably small uncertainties.
Critical Need for Plutonium and Uranium Isotopic Standards with Lower Uncertainties
Mathew, Kattathu Joseph; Stanley, Floyd E.; Thomas, Mariam R.; ...
2016-09-23
Certified reference materials (CRMs) traceable to national and international safeguards database are a critical prerequisite for ensuring that nuclear measurement systems are free of systematic biases. CRMs are used to validate measurement processes associated with nuclear analytical laboratories. Diverse areas related to nuclear safeguards are impacted by the quality of the CRM standards available to analytical laboratories. These include: nuclear forensics, radio-chronometry, national and international safeguards, stockpile stewardship, nuclear weapons infrastructure and nonproliferation, fuel fabrication, waste processing, radiation protection, and environmental monitoring. For the past three decades the nuclear community is confronted with the strange situation that improvements in measurementmore » data quality resulting from the improved accuracy and precision achievable with modern multi-collector mass spectrometers could not be fully exploited due to large uncertainties associated with CRMs available from New Brunswick Laboratory (NBL) that are used for instrument calibration and measurement control. Similar conditions prevail for both plutonium and uranium isotopic standards and for impurity element standards in uranium matrices. Herein, the current status of U and Pu isotopic standards available from NBL is reviewed. Critical areas requiring improvement in the quality of the nuclear standards to enable the U. S. and international safeguards community to utilize the full potential of modern multi-collector mass spectrometer instruments are highlighted.« less
Mechanistic approach for nitride fuel evolution and fission product release under irradiation
NASA Astrophysics Data System (ADS)
Dolgodvorov, A. P.; Ozrin, V. D.
2017-01-01
A model for describing uranium-plutonium mixed nitride fuel pellet burning was developed. Except fission products generating, the model includes impurities of oxygen and carbon. Nitrogen behaviour in nitride fuel was analysed and the nitrogen chemical potential in solid solution with uranium-plutonium nitride was constructed. The chemical program module was tested with the help of thermodynamic equilibrium phase distribution calculation. Results were compared with analogous data in literature, quite good agreement was achieved, especially for uranium sesquinitride, metallic species and some oxides. Calculation of a process of nitride fuel burning was also conducted. Used mechanistic approaches for fission product evolution give the opportunity to find fission gas release fractions and also volumes of intergranular secondary phases. Calculations present that the most massive secondary phases are the oxide and metallic phases. Oxide phase contain approximately 1 % wt of substance over all time of burning with slightly increasing of content. Metallic phase has considerable rising of mass and by the last stage of burning it contains about 0.6 % wt of substance. Intermetallic phase has less increasing rate than metallic phase and include from 0.1 to 0.2 % wt over all time of burning. The highest element fractions of released gaseous fission products correspond to caesium and iodide.
Critical Need for Plutonium and Uranium Isotopic Standards with Lower Uncertainties
DOE Office of Scientific and Technical Information (OSTI.GOV)
Mathew, Kattathu Joseph; Stanley, Floyd E.; Thomas, Mariam R.
Certified reference materials (CRMs) traceable to national and international safeguards database are a critical prerequisite for ensuring that nuclear measurement systems are free of systematic biases. CRMs are used to validate measurement processes associated with nuclear analytical laboratories. Diverse areas related to nuclear safeguards are impacted by the quality of the CRM standards available to analytical laboratories. These include: nuclear forensics, radio-chronometry, national and international safeguards, stockpile stewardship, nuclear weapons infrastructure and nonproliferation, fuel fabrication, waste processing, radiation protection, and environmental monitoring. For the past three decades the nuclear community is confronted with the strange situation that improvements in measurementmore » data quality resulting from the improved accuracy and precision achievable with modern multi-collector mass spectrometers could not be fully exploited due to large uncertainties associated with CRMs available from New Brunswick Laboratory (NBL) that are used for instrument calibration and measurement control. Similar conditions prevail for both plutonium and uranium isotopic standards and for impurity element standards in uranium matrices. Herein, the current status of U and Pu isotopic standards available from NBL is reviewed. Critical areas requiring improvement in the quality of the nuclear standards to enable the U. S. and international safeguards community to utilize the full potential of modern multi-collector mass spectrometer instruments are highlighted.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kathren, R.L.; Harwick, L.A.; Toohey, R.E.
The Registries originated in 1968 as the National Plutonium Registry with the name changed to the United States Transuranium Registry the following year to reflect a broader concern with the heavier actinides as well. Initially, the scientific effort of the USTR was directed towards study of the distribution and dose of plutonium and americium in occupationally exposed persons, and to assessment of the effects of exposure to the transuranium elements on health. This latter role was reassessed during the 1970`s when it was recognized that the biased cohort of the USTR was inappropriate for epidemiologic analysis. In 1978, the administrativelymore » separate but parallel United States Uranium Registry was created to carry out similar work among persons exposed to uranium and its decay products. A seven member scientific advisory committee provided guidance and scientific oversight. In 1992, the two Registries were administratively combined and transferred from the purview of a Department of Energy contractor to Washington State University under the provisions of a grant. Scientific results for the first twenty-five years of the Registries are summarized, including the 1985 publication of the analysis of the first whole body donor. Current scientific work in progress is summarized along with administrative activities for the period.« less
On the Use of Thermal NF3 as the Fluorination and Oxidation Agent in Treatment of Used Nuclear Fuels
DOE Office of Scientific and Technical Information (OSTI.GOV)
Scheele, Randall D.; McNamara, Bruce K.; Casella, Andrew M.
2012-05-01
This paper presents results of our investigation on the use of nitrogen trifluoride as the fluorination or fluorination/oxidation agent for use in a process for separating valuable constituents from used nuclear fuels by employing the volatility of many transition metal and actinide fluorides. Nitrogen trifluoride is less chemically and reactively hazardous than the hazardous and aggressive fluorinating agents used to prepare uranium hexafluoride and considered for fluoride volatility based nuclear fuels reprocessing. In addition, nitrogen trifluoride’s less aggressive character may be used to separate the volatile fluorides from used fuel and from themselves based on the fluorination reaction’s temperature sensitivitymore » (thermal tunability) rather than relying on differences in sublimation/boiling temperature and sorbents. Our thermodynamic calculations found that nitrogen trifluoride has the potential to produce volatile fission product and actinide fluorides from candidate oxides and metals. Our simultaneous thermogravimetric and differential thermal analyses found that the oxides of lanthanum, cerium, rhodium, and plutonium fluorinated but did not form volatile fluorides and that depending on temperature volatile fluorides formed from the oxides of niobium, molybdenum, ruthenium, tellurium, uranium, and neptunium. We also demonstrated near-quantitative removal of uranium from plutonium in a mixed oxide.« less
Uranium in bone: metabolic and autoradiographic studies in the rat.
Priest, N D; Howells, G R; Green, D; Haines, J W
1982-03-01
The distribution and retention of intravenously injected hexavalent uranium-233 in the skeleton of the female rat has been investigated using a variety of autoradiographic and radiochemical techniques. These showed that approximately one third of the injected uranium is deposited in the skeleton where it is retained with an initial biological half-time of approximately 40 days. The studies also showed that: 1 Uranium is initially deposited onto all types of bone surface, but preferentially onto those that are accreting. 2 Uranium is deposited in the calcifying zones of skeletal cartilage. 3 Bone accretion results in the burial of surface deposits of uranium. 4 Bone resorption causes the removal of uranium from surfaces. 5 Resorbed uranium is not retained by osteoclasts and macrophages in the bone marrow. 6 Uranium removed from bone surfaces enters the bloodstream where most is either redeposited in bone or excreted via the kidneys. 7 The recycling of resorbed uranium within the skeleton tends to produce a uniform level of uranium contamination throughout mineralized bone. These results are taken to indicate that uranium deposition in bone shares characteristics in common with both the 'volume-seeking radionuclides' typified by the alkaline earth elements and with the 'bone surface-seeking radionuclides' typified by plutonium.
Micro-Raman Technology to Interrogate Two-Phase Extraction on a Microfluidic Device.
Nelson, Gilbert L; Asmussen, Susan E; Lines, Amanda M; Casella, Amanda J; Bottenus, Danny R; Clark, Sue B; Bryan, Samuel A
2018-05-21
Microfluidic devices provide ideal environments to study solvent extraction. When droplets form and generate plug flow down the microfluidic channel, the device acts as a microreactor in which the kinetics of chemical reactions and interfacial transfer can be examined. Here, we present a methodology that combines chemometric analysis with online micro-Raman spectroscopy to monitor biphasic extractions within a microfluidic device. Among the many benefits of microreactors is the ability to maintain small sample volumes, which is especially important when studying solvent extraction in harsh environments, such as in separations related to the nuclear fuel cycle. In solvent extraction, the efficiency of the process depends on complex formation and rates of transfer in biphasic systems. Thus, it is important to understand the kinetic parameters in an extraction system to maintain a high efficiency and effectivity of the process. This monitoring provided concentration measurements in both organic and aqueous plugs as they were pumped through the microfluidic channel. The biphasic system studied was comprised of HNO 3 as the aqueous phase and 30% (v/v) tributyl phosphate in n-dodecane comprised the organic phase, which simulated the plutonium uranium reduction extraction (PUREX) process. Using pre-equilibrated solutions (post extraction), the validity of the technique and methodology is illustrated. Following this validation, solutions that were not equilibrated were examined and the kinetics of interfacial mass transfer within the biphasic system were established. Kinetic results of extraction were compared to kinetics already determined on a macro scale to prove the efficacy of the technique.
A simple model for the critical mass of a nuclear weapon
NASA Astrophysics Data System (ADS)
Reed, B. Cameron
2018-07-01
A probability-based model for estimating the critical mass of a fissile isotope is developed. The model requires introducing some concepts from nuclear physics and incorporating some approximations, but gives results correct to about a factor of two for uranium-235 and plutonium-239.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Zalupski, Peter R.; Klaehn, John R.; Peterman, Dean R.
The feasibility of simultaneous separation of uranium, neptunium, plutonium, americium, and curium from a simulated dissolved used fuel simulant adjusted to 1.0 M nitric acid is investigated using a mixture of the soft donor bis(bis-3,5-trifluoromethyl)phenyl) dithiophosphinic acid (“0”) and the hard donor synergist trioctylphosphine oxide (TOPO) dissolved in toluene. The results reported in this work are compared to our recent demonstration of a complete actinide recovery from a simulated dissolved fuel solution using a synergistic combination of bis(o-trifluoromethylphenyl)dithiophosphinic acid (“1”) and TOPO dissolved in either toluene or trifluoromethylphenyl sulfone. While the extraction efficiency of americium was enhanced for the liquid-liquidmore » system containing “0”, enabling to accomplish a trivalent An/Ln separation at 1.0 M HNO3, the extraction of neptunium was drastically diminished, relative to “1”. The partitioning behavior of curium was also negatively impacted, introducing an effective opportunity for americium/curium separation. Radiometric and spectrophotometric studies demonstrate that the complete actinide recovery using the solvent based upon “0” and TOPO is not feasible. Additionally, the importance of radiolytic degradation processes is discussed through the comparisons of extraction properties of liquid-liquid systems based on both soft donor reagents.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Vo, Quynh N.; Dang, Liem X.; Nilsson, Mikael
2016-07-21
Tri-n-butyl phosphate (TBP), a representative of neutral organophosphorous ligands, is an important extractant used in solvent extraction process for the recovery of uranium and plutonium from spent nuclear fuel. Microscopic pictures of TBP isomerism and its behavior in n-dodecane diluent were investigated utilizing MD simulations with previously optimized force field parameters for TBP and n-dodecane. Potential Mean Force (PMF) calculations on a single TBP molecule show seven probable TBP isomers. Radial Distribution Functions (RDF) of TBP suggests the existence of TBP trimers at high TBP concentrations in addition to dimers. 2D PMF calculations were performed to determine the angle andmore » distance criteria for TBP trimers. The dimerization and trimerization constants of TBP in n-dodecane were obtained and match our own experimental values using FTIR technique. The new insights into the conformational behaviors of TBP molecule as a monomer and as part of an aggregate could greatly aid the understanding of the complexation between TBP and metal ions in solvent extraction system. The U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences funded the work performed by LXD.« less
Sheppard, J.C.
1962-07-31
A process of selectively extracting plutonium nitrate and neptunium nitrate with an organic solution of a tertiary amine, away from uranyl nitrate present in an aqueous solution in a maximum concentration of 1M is described. The nitric acid concentration is adjusted to about 4M and nitrous acid is added prior to extraction. (AEC)
Thermodynamic calculations of oxygen self-diffusion in mixed-oxide nuclear fuels
Parfitt, David C.; Cooper, Michael William; Rushton, Michael J.D.; ...
2016-07-29
Mixed-oxide fuels containing uranium with thorium and/or plutonium may play an important part in future nuclear fuel cycles. There are, however, significantly less data available for these materials than conventional uranium dioxide fuel. In the present study, we employ molecular dynamics calculations to simulate the elastic properties and thermal expansivity of a range of mixed oxide compositions. These are then used to support equations of state and oxygen self-diffusion models to provide a self-consistent prediction of the behaviour of these mixed oxide fuels at arbitrary compositions.
NASA Astrophysics Data System (ADS)
Runde, Wolfgang; Neu, Mary P.
Since the 1950s actinides have been used to benefit industry, science, health, and national security. The largest industrial application, electricity generation from uranium and thorium fuels, is growing worldwide. Thus, more actinides are being mined, produced, used and processed than ever before. The future of nuclear energy hinges on how these increasing amounts of actinides are contained in each stage of the fuel cycle, including disposition. In addition, uranium and plutonium were built up during the Cold War between the United States and the Former Soviet Union for defense purposes and nuclear energy.
Modeling of point defects and rare gas incorporation in uranium mono-carbide
NASA Astrophysics Data System (ADS)
Chartier, A.; Van Brutzel, L.
2007-02-01
An embedded atom method (EAM) potential has been established for uranium mono-carbide. This EAM potential was fitted on structural properties of metallic uranium and uranium mono-carbide. The formation energies of point defects, as well as activation energies for self migration, have been evaluated in order to cross-check the suitability of the potential. Assuming that the carbon vacancies are the main defects in uranium mono-carbide compounds, the migration paths and energies are consistent with experimental data selected by Catlow[C.R.A. Catlow, J. Nucl. Mater. 60 (1976) 151]. The insertion and migration energies for He, Kr and Xe have also been evaluated with available inter-atomic potentials [H.H. Andersen, P. Sigmund, Nucl. Instr. and Meth. B 38 (1965) 238]. Results show that the most stable defect configuration for rare gases is within uranium vacancies. The migration energy of an interstitial Xe is 0.5 eV, in agreement with the experimental value of 0.5 eV [Hj. Matzke, Science of advanced LMFBR fuels, Solid State Physics, Chemistry and Technology of Carbides, Nitrides and Carbonitrides of Uranium and Plutonium, North-Holland, 1986].
METHOD OF SEPARATION OF PLUTONIUM FROM CARRIER PRECIPITATES
Dawson, I.R.
1959-09-22
The recovery of plutonium from fluoride carrier precipitates is described. The precipitate is dissolved in zirconyl nitrate, ferric nitrate, aluminum nitrate, or a mixture of these complexing agents, and the plutonium is then extracted from the aqueous solution formed with a water-immiscible organic solvent.
TRANSURANIC STUDIES STATUS AND PROBLEM STATEMENT
DOE Office of Scientific and Technical Information (OSTI.GOV)
Leuze, R E
1959-04-29
The purpose of the Transuranics Program is to develop separation processes for the transuranic elements, primarily those produced by long-term neutron irradiation of Pu/sup 239/. The program includes laboratory process development, pilot-plant process testing, processing of 10 kg of Pu/sup 239/ irradiated to greater than 99% burn-up for plutonium and americium-curium recovery, and processing the reirradiated plutonium and americium-curium fractions. The proposed method for processing highly irradiated plutonium is: (1) plutonium-aluminum alloy dissolution in HNO/sub 3/; (2) plutonium recovery by TBP extraction; (3) americium, curium, and rare-earth extraction by TBP from neutral nitrate solution; (4) partial rare-earth removal (primarily lanthanum)more » by americium-curium extraction into 100% TBP from 15M HNO/sub 3/; (5) additional rare-earth removal by extraction in 0.48M mono-2-ethylhexylphosphoric acid from 12M HCl; and (6) americium-curium purification by chloride anion exchange. Processing through the 100% TBP, 15M HNO/sub 3/ cycle can be carried out in the Power Reactor Fuel Reprocessing Pilot Plant. New facilities are proposed 15M HNO/ sub 3/ cycle can be carried out in the Power Reactor Fuel Reprocessing Pilot Plant. New facilities are proposed for laboratory process development studies and the final processing of the transplutonic elements. (auth)« less
241Am Ingrowth and Its Effect on Internal Dose
Konzen, Kevin
2016-07-01
Generally, plutonium has been manufactured to support commercial and military applications involving heat sources, weapons and reactor fuel. This work focuses on three typical plutonium mixtures, while observing the potential of 241Am ingrowth and its effect on internal dose. The term “ingrowth” is used to describe 241Am production due solely from the decay of 241Pu as part of a plutonium mixture, where it is initially absent or present in a smaller quantity. Dose calculation models do not account for 241Am ingrowth unless the 241Pu quantity is specified. This work suggested that 241Am ingrowth be considered in bioassay analysis when theremore » is a potential of a 10% increase to the individual’s committed effective dose. It was determined that plutonium fuel mixtures, initially absent of 241Am, would likely exceed 10% for typical reactor grade fuel aged less than 30 years; however, heat source grade and aged weapons grade fuel would normally fall below this threshold. In conclusion, although this work addresses typical plutonium mixtures following separation, it may be extended to irradiated commercial uranium fuel and is expected to be a concern in the recycling of spent fuel.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Konzen, Kevin
Generally, plutonium has been manufactured to support commercial and military applications involving heat sources, weapons and reactor fuel. This work focuses on three typical plutonium mixtures, while observing the potential of 241Am ingrowth and its effect on internal dose. The term “ingrowth” is used to describe 241Am production due solely from the decay of 241Pu as part of a plutonium mixture, where it is initially absent or present in a smaller quantity. Dose calculation models do not account for 241Am ingrowth unless the 241Pu quantity is specified. This work suggested that 241Am ingrowth be considered in bioassay analysis when theremore » is a potential of a 10% increase to the individual’s committed effective dose. It was determined that plutonium fuel mixtures, initially absent of 241Am, would likely exceed 10% for typical reactor grade fuel aged less than 30 years; however, heat source grade and aged weapons grade fuel would normally fall below this threshold. In conclusion, although this work addresses typical plutonium mixtures following separation, it may be extended to irradiated commercial uranium fuel and is expected to be a concern in the recycling of spent fuel.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ryerson, F J; Ebbinghaus, B
2000-05-25
Three compositions representing plutonium-free analogs of a proposed Ca-Ti-Gd-Hf-U-PU oxide ceramic for the immobilization of plutonium were equilibrated at 1 atm, 1350 C over a range of oxygen fugacities between air and that equivalent to the iron-wuestite buffer. The cerium analog replaces Pu on a mole-per-mole basic with Ce; the thorium analog replaces Pu with Th. A third material has 10 wt% Al{sub 2}O{sub 3} added to the cerium analog to encourage the formation of a Hf-analog of, CaHfTi{sub 2}O{sub 7}, zirconolite, which is referred to as hafnolite. The predominant phase produced in each formulation under all conditions is pyrochlore,more » A{sub 2}T{sub 2}O{sub 7}, where the T site is filled by Ti, and Ca, the lanthanides, Hf, U and Pu are accommodated on the A-site. Other lanthanide and uranium-bearing phases encountered include brannerite (UTi{sub 2}O{sub 6}), hafnolite (CaHfTi{sub 2}O{sub 7}), perovskite (CaTiO{sub 3}) and a calcium-lanthanide aluminotitanate with nominal stoichiometry (Ca,Ln)Ti{sub 2}Al{sub 9}O{sub 19}, where Ln is a lanthanide. The phase compositions show progressive shifts with decreasing oxygen fugacity. All of the phases observed have previously been identified in titanate-based high-level radioactive waste ceramics and demonstrate the flexibility of these ceramics to variations in processing parameters. The main variation is an increase in the uranium concentrations of pyrochlore and brannerite which must be accommodated by variations in modal abundance. Pyrochlore compositions are consistent with existing spectroscopic data suggesting that uranium is predominantly pentavalent in samples synthesized in air. A simple model based on ideal stoichiometry suggests the U{sup +4}/{Sigma}U varies linearly with log fO{sub 2} and that all of the uranium is quadravalent at the iron-wuestite buffer.« less
Evaluation of isotopic composition of fast reactor core in closed nuclear fuel cycle
NASA Astrophysics Data System (ADS)
Tikhomirov, Georgy; Ternovykh, Mikhail; Saldikov, Ivan; Fomichenko, Peter; Gerasimov, Alexander
2017-09-01
The strategy of the development of nuclear power in Russia provides for use of fast power reactors in closed nuclear fuel cycle. The PRORYV (i.e. «Breakthrough» in Russian) project is currently under development. Within the framework of this project, fast reactors BN-1200 and BREST-OD-300 should be built to, inter alia, demonstrate possibility of the closed nuclear fuel cycle technologies with plutonium as a main source of energy. Russia has a large inventory of plutonium which was accumulated in the result of reprocessing of spent fuel of thermal power reactors and conversion of nuclear weapons. This kind of plutonium will be used for development of initial fuel assemblies for fast reactors. The closed nuclear fuel cycle concept of the PRORYV assumes self-supplied mode of operation with fuel regeneration by neutron capture reaction in non-enriched uranium, which is used as a raw material. Operating modes of reactors and its characteristics should be chosen so as to provide the self-sufficient mode by using of fissile isotopes while refueling by depleted uranium and to support this state during the entire period of reactor operation. Thus, the actual issue is modeling fuel handling processes. To solve these problems, the code REPRORYV (Recycle for PRORYV) has been developed. It simulates nuclide streams in non-reactor stages of the closed fuel cycle. At the same time various verified codes can be used to evaluate in-core characteristics of a reactor. By using this approach various options for nuclide streams and assess the impact of different plutonium content in the fuel, fuel processing conditions, losses during fuel processing, as well as the impact of initial uncertainties on neutron-physical characteristics of reactor are considered in this study.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Farmer, J C; Diaz de la Rubia, T; Moses, E
2008-12-23
The National Ignition Facility (NIF) project, a laser-based Inertial Confinement Fusion (ICF) experiment designed to achieve thermonuclear fusion ignition and burn in the laboratory, is under construction at the Lawrence Livermore National Laboratory (LLNL) and will be completed in April of 2009. Experiments designed to accomplish the NIF's goal will commence in late FY2010 utilizing laser energies of 1 to 1.3 MJ. Fusion yields of the order of 10 to 20 MJ are expected soon thereafter. Laser initiated fusion-fission (LIFE) engines have now been designed to produce nuclear power from natural or depleted uranium without isotopic enrichment, and from spentmore » nuclear fuel from light water reactors without chemical separation into weapons-attractive actinide streams. A point-source of high-energy neutrons produced by laser-generated, thermonuclear fusion within a target is used to achieve ultra-deep burn-up of the fertile or fissile fuel in a sub-critical fission blanket. Fertile fuels including depleted uranium (DU), natural uranium (NatU), spent nuclear fuel (SNF), and thorium (Th) can be used. Fissile fuels such as low-enrichment uranium (LEU), excess weapons plutonium (WG-Pu), and excess highly-enriched uranium (HEU) may be used as well. Based upon preliminary analyses, it is believed that LIFE could help meet worldwide electricity needs in a safe and sustainable manner, while drastically shrinking the nation's and world's stockpile of spent nuclear fuel and excess weapons materials. LIFE takes advantage of the significant advances in laser-based inertial confinement fusion that are taking place at the NIF at LLNL where it is expected that thermonuclear ignition will be achieved in the 2010-2011 timeframe. Starting from as little as 300 to 500 MW of fusion power, a single LIFE engine will be able to generate 2000 to 3000 MWt in steady state for periods of years to decades, depending on the nuclear fuel and engine configuration. Because the fission blanket in a fusion-fission hybrid system is subcritical, a LIFE engine can burn any fertile or fissile nuclear material, including unenriched natural or depleted U and SNF, and can extract a very high percentage of the energy content of its fuel resulting in greatly enhanced energy generation per metric ton of nuclear fuel, as well as nuclear waste forms with vastly reduced concentrations of long-lived actinides. LIFE engines could thus provide the ability to generate vast amounts of electricity while greatly reducing the actinide content of any existing or future nuclear waste and extending the availability of low cost nuclear fuels for several thousand years. LIFE also provides an attractive pathway for burning excess weapons Pu to over 99% FIMA (fission of initial metal atoms) without the need for fabricating or reprocessing mixed oxide fuels (MOX). Because of all of these advantages, LIFE engines offer a pathway toward sustainable and safe nuclear power that significantly mitigates nuclear proliferation concerns and minimizes nuclear waste. An important aspect of a LIFE engine is the fact that there is no need to extract the fission fuel from the fission blanket before it is burned to the desired final level. Except for fuel inspection and maintenance process times, the nuclear fuel is always within the core of the reactor and no weapons-attractive materials are available outside at any point in time. However, an important consideration when discussing proliferation concerns associated with any nuclear fuel cycle is the ease with which reactor fuel can be converted to weapons usable materials, not just when it is extracted as waste, but at any point in the fuel cycle. Although the nuclear fuel remains in the core of the engine until ultra deep actinide burn up is achieved, soon after start up of the engine, once the system breeds up to full power, several tons of fissile material is present in the fission blanket. However, this fissile material is widely dispersed in millions of fuel pebbles, which can be tagged as individual accountable items, and thus made difficult to divert in large quantities. This report discusses the application of the LIFE concept to nonproliferation issues, initially looking at the LIFE (Laser Inertial Fusion-Fission Energy) engine as a means of completely burning WG Pu and HEU. By combining a neutron-rich inertial fusion point source with energy-rich fission, the once-through closed fuel-cycle LIFE concept has the following characteristics: it is capable of efficiently burning excess weapons or separated civilian plutonium and highly enriched uranium; the fission blanket is sub-critical at all times (keff < 0.95); because LIFE can operate well beyond the point at which light water reactors (LWRs) need to be refueled due to burn-up of fissile material and the resulting drop in system reactivity, fuel burn-up of 99% or more appears feasible. The objective of this work is to develop LIFE technology for burning of WG-Pu and HEU.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wang, Taiping; Khangaonkar, Tarang; Long, Wen
2014-02-07
In recent years, with the rapid growth of global energy demand, the interest in extracting uranium from seawater for nuclear energy has been renewed. While extracting seawater uranium is not yet commercially viable, it serves as a “backstop” to the conventional uranium resources and provides an essentially unlimited supply of uranium resource. With recent advances in seawater uranium extraction technology, extracting uranium from seawater could be economically feasible when the extraction devices are deployed at a large scale (e.g., several hundred km2). There is concern however that the large scale deployment of adsorbent farms could result in potential impacts tomore » the hydrodynamic flow field in an oceanic setting. In this study, a kelp-type structure module was incorporated into a coastal ocean model to simulate the blockage effect of uranium extraction devices on the flow field. The module was quantitatively validated against laboratory flume experiments for both velocity and turbulence profiles. The model-data comparison showed an overall good agreement and validated the approach of applying the model to assess the potential hydrodynamic impact of uranium extraction devices or other underwater structures in coastal oceans.« less
NASA Astrophysics Data System (ADS)
Pistner, C.; Liebert, W.; Fujara, F.
2006-06-01
Inert matrix fuels (IMF) with plutonium may play a significant role to dispose of stockpiles of separated plutonium from military or civilian origin. For reasons of reactivity control of such fuels, burnable poisons (BP) will have to be used. The impact of different possible BP candidates (B, Eu, Er and Gd) on the achievable burnup as well as on safety and non-proliferation aspects of IMF are analyzed. To this end, cell burnup calculations have been performed and burnup dependent reactivity coefficients (boron worth, fuel temperature and moderator void coefficient) were calculated. All BP candidates were analyzed for one initial BP concentration and a range of different initial plutonium-concentrations (0.4-1.0 g cm-3) for reactor-grade plutonium isotopic composition as well as for weapon-grade plutonium. For the two most promising BP candidates (Er and Gd), a range of different BP concentrations was investigated to study the impact of BP concentration on fuel burnup. A set of reference fuels was identified to compare the performance of uranium-fuels, MOX and IMF with respect to (1) the fraction of initial plutonium being burned, (2) the remaining absolute plutonium concentration in the spent fuel and (3) the shift in the isotopic composition of the remaining plutonium leading to differences in the heat and neutron rate produced. In the case of IMF, the remaining Pu in spent fuel is unattractive for a would be proliferator. This underlines the attractiveness of an IMF approach for disposal of Pu from a non-proliferation perspective.
PROCESS FOR UTILIZING ORGANIC ORTHOPHOSPHATE EXTRACTANTS
Grinstead, R.R.
1958-11-11
A process is presented for recovering uranium from its ores, the steps comprising producing the uranium in solution in the trivalent state, extracting the uranium from solution in an lmmiscible organic solvent extract phase which lncludes mono and dialkyl orthophosphorlc acid esters having a varying number of carbon atoms on the alkyl substituent, amd recovering the uranium from tbe extract phase.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Reese, A.P.; Crowther, R.L. Jr.
1992-02-18
This patent describes improvement in a boiling water reactor core having a plurality of vertically upstanding fuel bundles; each fuel bundle containing longitudinally extending sealed rods with fissile material therein; the improvement comprises the fissile material including a mixture of uranium and recovered plutonium in rods of the fuel bundle at locations other than the corners of the fuel bundle; and, neutron absorbing material being located in rods of the fuel bundle at rod locations adjacent the corners of the fuel bundles whereby the neutron absorbing material has decreased shielding from the plutonium and maximum exposure to thermal neutrons formore » shaping the cold reactivity shutdown zone in the fuel bundle.« less
Plutonium-fission xenon found in Earth's mantle
Kunz; Staudacher; Allegre
1998-05-08
Data from mid-ocean ridge basalt glasses indicate that the short-lived radionuclide plutonium-244 that was present during an early stage of the development of the solar system is responsible for roughly 30 percent of the fissiogenic xenon excesses in the interior of Earth today. The rest of the fissiogenic xenon can be ascribed to the spontaneous fission of still live uranium-238. This result, in combination with the refined determination of xenon-129 excesses from extinct iodine-129, implies that the accretion of Earth was finished roughly 50 million to 70 million years after solar system formation and that the atmosphere was formed by mantle degassing.
NASA Astrophysics Data System (ADS)
Tajima, Naoki; Yusa, Noritaka; Hashizume, Hidetoshi
2018-04-01
This paper discusses the applicability of simple low-frequency eddy current testing to the detection of deeply embedded flaws. The study specifically considered a double tank in a reprocessing plant for extracting plutonium-uranium from spent nuclear fuels. The tank was modelled by two type 304 austenitic stainless steel plates situated with an air gap of 80 mm, and the change in the thickness of one of the plates was detected through the other plate and the air gap. Axisymmetric two-dimensional finite element simulations were conducted and found that a simple circular coil with a large diameter enabled to detect the thickness based on the magnetic flux density at the centre of the coil although the plates were as thick as 30 mm. The results of the numerical simulations were validated by experiments.
Investigation of Tank 241-AN-101 Floating Solids
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kraft, Douglas P.; Meznarich, H. K.
Tank 241-AN-101 is the receiver tank for retrieval of several C-Farms waste tanks, including Tanks 241-C-102 and 241-C-111. Tank 241 C 111 received first-cycle decontamination waste from the bismuth phosphate process and Plutonium and Uranium Extraction cladding waste, as well as hydraulic fluid. Three grab samples, 1AN-16-01, 1AN-16-01A, and 1AN-16-01B, were collected at the surface of Tank 241-AN-101 on April 25, 2016, after Tank 241-C-111 retrieval was completed. Floating solids were observed in the three grab samples in the 11A hot cell after the samples were received at the 222-S Laboratory. Routine chemical analyses, solid phase characterization on the floatingmore » and settled solids, semivolatile organic analysis mainly on the aqueous phase for identification of degradation products of hydraulic fluids were performed. Investigation of the floating solids is reported.« less
Facility effluent monitoring plan for the plutonium uranium extraction facility
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wiegand, D.L.
A facility effluent monitoring plan is required by the US Department of Energy in DOE Order 5400.1 for any operations that involve hazardous materials and radioactive substances that could impact employee or public safety or the environment. This document is prepared using the specific guidelines identified in A Guide for Preparing Hanford Site Facility Effluent Monitoring Plans, WHC-EP-0438-01. This facility effluent monitoring plan assesses effluent monitoring systems and evaluates whether they are adequate to ensure the public health and safety as specified in applicable federal, state, and local requirements. This facility effluent monitoring plan shall ensure long-range integrity of themore » effluent monitoring systems by requiring an update whenever a new process or operation introduces new hazardous materials or significant radioactive materials. This document must be reviewed annually even if there are no operational changes, and it must be updated at a minimum of every three years.« less
Tracking of Nuclear Production using Indigenous Species: Final LDRD Report
DOE Office of Scientific and Technical Information (OSTI.GOV)
Alam, Todd Michael; Alam, Mary Kathleen; McIntyre, Sarah K.
Our LDRD research project sought to develop an analytical method for detection of chemicals used in nuclear materials processing. Our approach is distinctly different than current research involving hardware-based sensors. By utilizing the response of indigenous species of plants and/or animals surrounding (or within) a nuclear processing facility, we propose tracking 'suspicious molecules' relevant to nuclear materials processing. As proof of concept, we have examined TBP, tributylphosphate, used in uranium enrichment as well as plutonium extraction from spent nuclear fuels. We will compare TBP to the TPP (triphenylphosphate) analog to determine the uniqueness of the metabonomic response. We show thatmore » there is a unique metabonomic response within our animal model to TBP. The TBP signature can further be delineated from that of TPP. We have also developed unique methods of instrumental transfer for metabonomic data sets.« less
Second NBL measurement evaluation program meeting: A summary
DOE Office of Scientific and Technical Information (OSTI.GOV)
Spaletto, M.I.; Clapper, M.; Tolbert, M.E.M.
New Brunswick Laboratory (NBL), the US government`s nuclear materials measurements and reference materials laboratory, administers interlaboratory measurement evaluation programs to evaluate the quality and adequacy of safeguards measurements. The NBL Measurement Evaluation Program covers several types of safeguards analytical measurements. The Safeguards Measurement Evaluation (SME) program distributes test materials destructive measurements of uranium for both elemental concentration and isotopic abundances, and of plutonium for isotopic abundances. The Calorimetry Exchange (CalEx) Program tests the quality of nondestructive measurements of plutonium isotopic abundances by gamma spectroscopy and plutonium concentration by calorimetry. In May 1997, more than 30 representatives from the Department ofmore » Energy (DOE), its contractor laboratories, and Nuclear Regulatory Commission licensees met at NBL in Argonne, Illinois, for the annual meeting of the Measurement Evaluation Program. The summary which follows details key points that were discussed or presented at the meeting.« less
SLURRY SOLVENT EXTRACTION PROCESS FOR THE RECOVERY OF METALS FROM SOLID MATERIALS
Grinstead, R.R.
1959-01-20
A solvent extraction process is described for recovering uranium from low grade uranium bearing minerals such as carnotit or shale. The finely communited ore is made up as an aqueous slurry containing the necessary amount of acid to solubilize the uranium and simultaneously or subsequently contacted with an organic solvent extractant such as the alkyl ortho-, or pyro phosphoric acids, alkyl phosphites or alkyl phosphonates in combination with a diluent such as kerosene or carbon tetrachlorids. The extractant phase is separated from the slurry and treated by any suitable process to recover the uranium therefrom. One method for recovering the uranium comprises treating the extract with aqueous HF containing a reducing agent such as ferrous sulfate, which reduces the uranium and causes it to be precipitated as uranium tetrafluoride.
Introduction to Pits and Weapons Systems (U)
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kautz, D.
2012-07-02
A Nuclear Explosive Package includes the Primary, Secondary, Radiation Case and related components. This is the part of the weapon that produces nuclear yield and it converts mechanical energy into nuclear energy. The pit is composed of materials that allow mechanical energy to be converted to electromagnetic energy. Fabrication processes used are typical of any metal fabrication facility: casting, forming, machining and welding. Some of the materials used in pits include: Plutonium, Uranium, Stainless Steel, Beryllium, Titanium, and Aluminum. Gloveboxes are used for three reasons: (1) Protect workers and public from easily transported, finely divided plutonium oxides - (a) Plutoniummore » is very reactive and produces very fine particulate oxides, (b) While not the 'Most dangerous material in the world' of Manhattan Project lore, plutonium is hazardous to health of workers if not properly controlled; (2) Protect plutonium from reactive materials - (a) Plutonium is extremely reactive at ambient conditions with several components found in air: oxygen, water, hydrogen, (b) As with most reactive metals, reactions with these materials may be violent and difficult to control, (c) As with most fabricated metal products, corrosion may significantly affect the mechanical, chemical, and physical properties of the product; and (3) Provide shielding from radioactive decay products: {alpha}, {gamma}, and {eta} are commonly associated with plutonium decay, as well as highly radioactive materials such as {sup 241}Am and {sup 238}Pu.« less
TC-99 Decontaminant from heat treated gaseous diffusion membrane -Phase I, Part B
DOE Office of Scientific and Technical Information (OSTI.GOV)
Oji, L.; Restivo, M.; Duignan, M.
2017-11-01
Uranium gaseous diffusion cascades represent a significant environmental challenge to dismantle, containerize and dispose as low-level radioactive waste. Baseline technologies rely on manual manipulations involving direct access to technetium-contaminated piping and materials. There is a potential to utilize novel decontamination technologies to remove the technetium and allow for on-site disposal of the very large uranium converters. Technetium entered these gaseous diffusion cascades as a hexafluoride complex in the same fashion as uranium. Technetium, as the isotope Tc-99, is an impurity that follows uranium in the first cycle of the Plutonium and Uranium Extraction (PUREX) process. The technetium speciation or exactmore » form in the gaseous diffusion cascades is not well defined. Several forms of Tc-99 compounds, mostly the fluorinated technetium compounds with varying degrees of volatility have been speculated by the scientific community to be present in these cascades. Therefore, there may be a possibility of using thermal or leaching desorption, which is independent of the technetium oxidation states, to perform an insitu removal of the technetium as a volatile species and trap the radionuclide on sorbent traps which could be disposed as low-level waste. Based on the positive results of the first part of this work1 the use of steam as a thermal decontamination agent was further explored with a second piece of used barrier material from a different location. This new series of tests included exposing more of the material surface to the flow of high temperature steam through the change in the reactor design, subjecting it to alternating periods of stream and vacuum, as well as determining if a lower temperature steam, i.e., 121°C (250°F) would be effective, too. Along with these methods, one other simpler method involving the leaching of the Tc-99 contaminated barrier material with a 1.0 M aqueous solution of ammonium carbonate, with and without sonication, was evaluated.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Meade, Roger Allen
In the summer of 1944, J. Robert Oppenheimer and Los Alamos faced a crisis. An isotopic impurity in Plutonium rendered the metal unusable in a gun-assembled atomic bomb (i.e., Little Boy). Making this situation worse was a shortage of Uranium. The combination of these two problems threatened the entire wartime project. The answer to this dilemma, in part, was to develop a novel assembly method for Plutonium using the supersonic shock waves created by several tons of high explosives to compress a ball of Plutonium into a supercritical state. Since this method, implosion, was not much more than a theoreticalmore » construct, the Trinity test was devised to proof test the process. Given the speculative nature of implosion, Trinity was a gamble of sorts. If the test failed (i.e., little or no nuclear yield), the blast of the high explosives would scatter the scarce and expensive Plutonium over the surrounding desert. Since the probability of failure remained high into the early summer of 1945, some method of containing a failed nuclear explosion was needed. Jumbo was the answer.« less
Lecompte, Yannick; Bohand, Sandra; Laroche, Pierre; Cazoulat, Alain
2013-01-01
After a review of radiometric reference methods used in radiotoxicology, analytical performance of inductively coupled plasma mass spectrometry (ICP-MS) for the workplace urinary diagnosis of internal contamination by radionuclides are evaluated. A literature review (covering the period from 2000 to 2012) is performed to identify the different applications of ICP-MS in radiotoxicology for urine analysis. The limits of detection are compared to the recommendations of the International commission on radiological protection (ICRP 78: "Individual monitoring for internal exposure of workers"). Except one publication describing the determination of strontium-90 (β emitter), all methods using ICP-MS reported in the literature concern actinides (α emitters). For radionuclides with a radioactive period higher than 10(4) years, limits of detection are most often in compliance with ICRP publication 78 and frequently lower than radiometric methods. ICP-MS allows the specific determination of plutonium-239 + 240 isotopes which cannot be discriminated by α spectrometry. High resolution ICP-MS can also measure uranium isotopic ratios in urine for total uranium concentrations lower than 20 ng/L. The interest of ICP-MS in radiotoxicology concerns essentially the urinary measurement of long radioactive period actinides, particularly for uranium isotope ratio determination and 239 and 240 plutonium isotopes discrimination. Radiometric methods remain the most efficient for the majority of other radionuclides.
AMINE EXTRACTION OF PLUTONIUM FROM NITRIC ACID SOLUTIONS LOADING AND STRIPPING EXPERIMENTS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wilson, A.S.
1961-01-19
Information is presented on a suitable amine processing system for plutonium nitrate. Experiments with concentrated plutonium nitrate solutions show that trilaurylamine (TLA) - xylene solvent systems did not form a second organic phase. Experiments are also reported with tri-noctylamine (TnOA)-xylene and TLA-Amsco - octyl alcohol. Two organic phases appear in both these systems at high plutonium nitrate concentrations. Data are tabulated from loading and stripping experiments. (J.R.D.)
plutonium from uranium and fission products in an aqueous acidic solution by use of a chelating agent. The concentration is adjusted to about 1 N bar. The aqueous solution is then contacted with a water-immiscible organic solvent solution and the chelating agent. The chelating agents covered by this invention comprise
Method for preparing actinide nitrides
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.
10 CFR 140.91 - Appendix A-Form of nuclear energy liability policy for facilities.
Code of Federal Regulations, 2010 CFR
2010-01-01
... designed or used for (a) separating the isotopes of uranium or plutonium, (b) processing or utilizing spent... processing, fabricating or alloying of special nuclear material if at any time the total amount of such... operations conducted thereat; Nuclear reactor means any apparatus designed or used to sustain nuclear fission...
10 CFR 140.91 - Appendix A-Form of nuclear energy liability policy for facilities.
Code of Federal Regulations, 2013 CFR
2013-01-01
... designed or used for (a) separating the isotopes of uranium or plutonium, (b) processing or utilizing spent... processing, fabricating or alloying of special nuclear material if at any time the total amount of such... operations conducted thereat; Nuclear reactor means any apparatus designed or used to sustain nuclear fission...
10 CFR 140.91 - Appendix A-Form of nuclear energy liability policy for facilities.
Code of Federal Regulations, 2014 CFR
2014-01-01
... designed or used for (a) separating the isotopes of uranium or plutonium, (b) processing or utilizing spent... processing, fabricating or alloying of special nuclear material if at any time the total amount of such... operations conducted thereat; Nuclear reactor means any apparatus designed or used to sustain nuclear fission...
10 CFR 140.91 - Appendix A-Form of nuclear energy liability policy for facilities.
Code of Federal Regulations, 2012 CFR
2012-01-01
... designed or used for (a) separating the isotopes of uranium or plutonium, (b) processing or utilizing spent... processing, fabricating or alloying of special nuclear material if at any time the total amount of such... operations conducted thereat; Nuclear reactor means any apparatus designed or used to sustain nuclear fission...
10 CFR 140.91 - Appendix A-Form of nuclear energy liability policy for facilities.
Code of Federal Regulations, 2011 CFR
2011-01-01
... designed or used for (a) separating the isotopes of uranium or plutonium, (b) processing or utilizing spent... processing, fabricating or alloying of special nuclear material if at any time the total amount of such... operations conducted thereat; Nuclear reactor means any apparatus designed or used to sustain nuclear fission...
The thermodynamics of pyrochemical processes for liquid metal reactor fuel cycles
DOE Office of Scientific and Technical Information (OSTI.GOV)
Johnson, I.
1987-01-01
The thermodynamic basis for pyrochemical processes for the recovery and purification of fuel for the liquid metal reactor fuel cycle is described. These processes involve the transport of the uranium and plutonium from one liquid alloy to another through a molten salt. The processes discussed use liquid alloys of cadmium, zinc, and magnesium and molten chloride salts. The oxidation-reduction steps are done either chemically by the use of an auxiliary redox couple or electrochemically by the use of an external electrical supply. The same basic thermodynamics apply to both the salt transport and the electrotransport processes. Large deviations from idealmore » solution behavior of the actinides and lanthanides in the liquid alloys have a major influence on the solubilities and the performance of both the salt transport and electrotransport processes. Separation of plutonium and uranium from each other and decontamination from the more noble fission product elements can be achieved using both transport processes. The thermodynamic analysis is used to make process design computations for different process conditions.« less
The role of the 5f valence orbitals of early actinides in chemical bonding
Vitova, T.; Pidchenko, I.; Fellhauer, D.; Bagus, P. S.; Joly, Y.; Pruessmann, T.; Bahl, S.; Gonzalez-Robles, E.; Rothe, J.; Altmaier, M.; Denecke, M. A.; Geckeis, H.
2017-01-01
One of the long standing debates in actinide chemistry is the level of localization and participation of the actinide 5f valence orbitals in covalent bonds across the actinide series. Here we illuminate the role of the 5f valence orbitals of uranium, neptunium and plutonium in chemical bonding using advanced spectroscopies: actinide M4,5 HR-XANES and 3d4f RIXS. Results reveal that the 5f orbitals are active in the chemical bonding for uranium and neptunium, shown by significant variations in the level of their localization evidenced in the spectra. In contrast, the 5f orbitals of plutonium appear localized and surprisingly insensitive to different bonding environments. We envisage that this report of using relative energy differences between the 5fδ/ϕ and 5fπ*/5fσ* orbitals as a qualitative measure of overlap-driven actinyl bond covalency will spark activity, and extend to numerous applications of RIXS and HR-XANES to gain new insights into the electronic structures of the actinide elements. PMID:28681848
The role of the 5f valence orbitals of early actinides in chemical bonding
NASA Astrophysics Data System (ADS)
Vitova, T.; Pidchenko, I.; Fellhauer, D.; Bagus, P. S.; Joly, Y.; Pruessmann, T.; Bahl, S.; Gonzalez-Robles, E.; Rothe, J.; Altmaier, M.; Denecke, M. A.; Geckeis, H.
2017-07-01
One of the long standing debates in actinide chemistry is the level of localization and participation of the actinide 5f valence orbitals in covalent bonds across the actinide series. Here we illuminate the role of the 5f valence orbitals of uranium, neptunium and plutonium in chemical bonding using advanced spectroscopies: actinide M4,5 HR-XANES and 3d4f RIXS. Results reveal that the 5f orbitals are active in the chemical bonding for uranium and neptunium, shown by significant variations in the level of their localization evidenced in the spectra. In contrast, the 5f orbitals of plutonium appear localized and surprisingly insensitive to different bonding environments. We envisage that this report of using relative energy differences between the 5fδ/φ and 5fπ*/5fσ* orbitals as a qualitative measure of overlap-driven actinyl bond covalency will spark activity, and extend to numerous applications of RIXS and HR-XANES to gain new insights into the electronic structures of the actinide elements.
Apparatus and process for the electrolytic reduction of uranium and plutonium oxides
Poa, David S.; Burris, Leslie; Steunenberg, Robert K.; Tomczuk, Zygmunt
1991-01-01
An apparatus and process for reducing uranium and/or plutonium oxides to produce a solid, high-purity metal. The apparatus is an electrolyte cell consisting of a first container, and a smaller second container within the first container. An electrolyte fills both containers, the level of the electrolyte in the first container being above the top of the second container so that the electrolyte can be circulated between the containers. The anode is positioned in the first container while the cathode is located in the second container. Means are provided for passing an inert gas into the electrolyte near the lower end of the anode to sparge the electrolyte and to remove gases which form on the anode during the reduction operation. Means are also provided for mixing and stirring the electrolyte in the first container to solubilize the metal oxide in the electrolyte and to transport the electrolyte containing dissolved oxide into contact with the cathode in the second container. The cell is operated at a temperature below the melting temperature of the metal product so that the metal forms as a solid on the cathode.
Actinides in metallic waste from electrometallurgical treatment of spent nuclear fuel
NASA Astrophysics Data System (ADS)
Janney, D. E.; Keiser, D. D.
2003-09-01
Argonne National Laboratory has developed a pyroprocessing-based technique for conditioning spent sodium-bonded nuclear-reactor fuel in preparation for long-term disposal. The technique produces a metallic waste form whose nominal composition is stainless steel with 15 wt.% Zr (SS-15Zr), up to ˜ 11 wt.% actinide elements (primarily uranium), and a few percent metallic fission products. Actual and simulated waste forms show similar eutectic microstructures with approximately equal proportions of iron solid solution phases and Fe-Zr intermetallics. This article reports on an analysis of simulated waste forms containing uranium, neptunium, and plutonium.
STRIPPING OF URANIUM FROM ORGANIC EXTRACTANTS
Crouse, D.J. Jr.
1962-09-01
A liquid-liquid extraction method is given for recovering uranium values from uranium-containing solutions. Uranium is removed from a uranium-containing organic solution by contacting said organic solution with an aqueous ammonium carbonate solution substantially saturated in uranium values. A uranium- containing precipitate is thereby formed which is separated from the organic and aqueous phases. Uranium values are recovered from this separated precipitate. (AE C)
RECOVERY OF URANIUM FROM PITCHBLENDE
Ruehle, A.E.
1958-06-24
The decontamination of uranium from molybdenum is described. When acid solutions containing uranyl nitrate are contacted with ether for the purpose of extracting the uranium values, complex molybdenum compounds are coextracted with the uranium and also again back-extracted from the ether with the uranium. This invention provides a process for extracting uranium in which coextraction of molybdenum is avoided. It has been found that polyhydric alcohols form complexes with molybdenum which are preferentially water-soluble are taken up by the ether extractant to only a very minor degree. The preferred embodiment of the process uses mannitol, sorbitol or a mixture of the two as the complexing agent.
Rainey, R.H.; Moore, J.G.
1962-08-14
A liquid-liquid extraction process was developed for recovering thorium and uranium values from a neutron irradiated thorium composition. They are separated from a solvent extraction system comprising a first end extraction stage for introducing an aqueous feed containing thorium and uranium into the system consisting of a plurality of intermediate extractiorr stages and a second end extractron stage for introducing an aqueous immiscible selective organic solvent for thorium and uranium in countercurrent contact therein with the aqueous feed. A nitrate iondeficient aqueous feed solution containing thorium and uranium was introduced into the first end extraction stage in countercurrent contact with the organic solvent entering the system from the second end extraction stage while intro ducing an aqueous solution of salting nitric acid into any one of the intermediate extraction stages of the system. The resultant thorium and uranium-laden organic solvent was removed at a point preceding the first end extraction stage of the system. (AEC)
DOE Office of Scientific and Technical Information (OSTI.GOV)
Amber Wright; Edward Mausolf; Keri Campbell
2010-05-01
Acetohydroxamic acid (AHA) is an organic ligand planned for use in the Uranium Extraction (UREX) process. It reduces neptunium and plutonium, and the resultant hydrophilic complexes are separated from uranium by extraction with tributyl phosphate (TBP) in a hydrocarbon diluent. AHA undergoes hydrolysis to acetic acid which will impede the recycling of nitric acid. During recent discussions of the UREX process, it has been proposed to replace AHA by formohydroxamic acid (FHA). FHA will undergo hydrolysis to formic acid which is volatile, thus allowing the recycling of nitric acid. The reported reduction potentials of AHA and pertechnetate (TcO{sub 4}{sup -})more » indicated that it may be possible for AHA to reduce technetium, altering its fate in the fuel cycle. At UNLV, it has been demonstrated that TcO{sub 4}{sup -} undergoes reductive nitrosylation by AHA under a variety of conditions. The resulting divalent technetium is complexed by AHA to form the pseudo-octahedral trans-aquonitrosyl (diacetohydroxamic)-technetium(II) complex ([Tc{sup II}(NO)(AHA){sub 2}H{sub 2}O]{sup +}). In this paper, we are reporting the synthesis of FHA and its complex formation with technetium along with the characterization of FHA crystals achieved by NMR and IR spectroscopy. Two experiments were conducted to investigate the complexation of FHA with Tc and the results were compared with previous data on AHA. The first experiment involved the elution of Tc from a Reillex HP anion exchange resin, and the second one monitored the complexation of technetium with FHA by UV-visible spectrophotometry.« less
Plant-uptake of uranium: Hydroponic and soil system studies
Ramaswami, A.; Carr, P.; Burkhardt, M.
2001-01-01
Limited information is available on screening and selection of terrestrial plants for uptake and translocation of uranium from soil. This article evaluates the removal of uranium from water and soil by selected plants, comparing plant performance in hydroponic systems with that in two soil systems (a sandy-loam soil and an organic-rich soil). Plants selected for this study were Sunflower (Helianthus giganteus), Spring Vetch (Vicia sativa), Hairy Vetch (Vicia villosa), Juniper (Juniperus monosperma), Indian Mustard (Brassica juncea), and Bush Bean (Phaseolus nanus). Plant performance was evaluated both in terms of the percent uranium extracted from the three systems, as well as the biological absorption coefficient (BAC) that normalized uranium uptake to plant biomass. Study results indicate that uranium extraction efficiency decreased sharply across hydroponic, sandy and organic soil systems, indicating that soil organic matter sequestered uranium, rendering it largely unavailable for plant uptake. These results indicate that site-specific soils must be used to screen plants for uranium extraction capability; plant behavior in hydroponic systems does not correlate well with that in soil systems. One plant species, Juniper, exhibited consistent uranium extraction efficiencies and BACs in both sandy and organic soils, suggesting unique uranium extraction capabilities.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hay, M. S.; Coleman, C. J.; Diprete, D. P.
SRNL analyzed samples from Tank 38H and Tank 43H to support ECP and CCP. The total uranium in the Tank 38H samples ranged from 53.7 mg/L for the surface sample to 57.0 mg/L in the sub-surface sample. The Tank 43H samples showed uranium concentrations of 46.2 mg/L for the surface sample and 45.7 mg/L in the sub-surface sample. The U-235 percentage was 0.63% in the Tank 38H samples and 0.62% in the Tank 43H samples. The total uranium and percent U-235 results appear consistent with recent Tank 38H and Tank 43H uranium measurements. The plutonium results for the Tank 38Hmore » surface sample are slightly higher than recent sample results, while the Tank 43H plutonium results are within the range of values measured on previous samples. The Cs-137 results for the Tank 38H surface and subsurface samples are slightly higher than the concentrations measured in recent samples. The Cs-137 results for the two Tank 43H samples are within the range of values measured on previous samples. The comparison of the sum of the cations in each sample versus the sum of the anions shows a difference of 23% for the Tank 38H surface sample and 18% for the Tank 43H surface sample. The four samples show silicon concentrations somewhat lower than the previous samples with values ranging from 80.2 to 105 mg/L.« less
Comparison of actinide production in traveling wave and pressurized water reactors
DOE Office of Scientific and Technical Information (OSTI.GOV)
Osborne, A.G.; Smith, T.A.; Deinert, M.R.
The geopolitical problems associated with civilian nuclear energy production arise in part from the accumulation of transuranics in spent nuclear fuel. A traveling wave reactor is a type of breed-burn reactor that could, if feasible, reduce the overall production of transuranics. In one possible configuration, a cylinder of natural or depleted uranium would be subjected to a fast neutron flux at one end. The neutrons would transmute the uranium, producing plutonium and higher actinides. Under the right conditions, the reactor could become critical, at which point a self-stabilizing fission wave would form and propagate down the length of the reactormore » cylinder. The neutrons from the fission wave would burn the fissile nuclides and transmute uranium ahead of the wave to produce additional fuel. Fission waves in uranium are driven largely by the production and fission of {sup 239}Pu. Simulations have shown that the fuel burnup can reach values greater than 400 MWd/kgIHM, before fission products poison the reaction. In this work we compare the production of plutonium and minor actinides produced in a fission wave to that of a UOX fueled light water reactor, both on an energy normalized basis. The nuclide concentrations in the spent traveling wave reactor fuel are computed using a one-group diffusion model and are verified using Monte Carlo simulations. In the case of the pressurized water reactor, a multi-group collision probability model is used to generate the nuclide quantities. We find that the traveling wave reactor produces about 0.187 g/MWd/kgIHM of transuranics compared to 0.413 g/MWd/kgIHM for a pressurized water reactor running fuel enriched to 4.95 % and burned to 50 MWd/kgIHM. (authors)« less
Balanced program plan. Analysis for biomedical and environmental research
DOE Office of Scientific and Technical Information (OSTI.GOV)
Not Available
1976-06-01
Major issues associated with the use of nuclear power are health hazards of exposure to radioactive materials; sources of radiation exposure; reactor accidents; sabotage of nuclear facilities; diversion of fissile material and its use for extortion; and the presence of plutonium in the environment. Fission fuel cycle technology is discussed with regard to milling, UF/sub 6/ production, uranium enrichment, plutonium fuel fabrication, power production, fuel processing, waste management, and fuel and waste transportation. The following problem areas of fuel cycle technology are briefly discussed: characterization, measurement, and monitoring; transport processes; health effects; ecological processes and effects; and integrated assessment. Estimatedmore » program unit costs are summarized by King-Muir Category. (HLW)« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Jaffke, Patrick John
This acts as a short note on the effects of varying the value of the endpoints of the thermal, epithermal, and fast flux groups. As expected, varying these endpoints can alter the value of the cross-section for a given nuclide. This effect is quantified in this note for an important nuclide in reactor simulations, 238U. Uranium-238 is responsible for the production of Plutonium in most reactors, making it critical to understand all of the 238U capture modes leading to Plutonium. We explicitly quantify the reaction rates for 238U that are altered when we use a given research reactor fluxmore » and vary the endpoint definitions of said flux as well as the reactor position.« less
Corrosion Testing of 304L SS 3013 Inner Container and Teardrop Samples
DOE Office of Scientific and Technical Information (OSTI.GOV)
Tokash, Justin Charles; Hill, Mary Ann; Lillard, Scott
The Department of Energy (DOE) 3013 Standard specifies a minimum of two containers to be used for the storage of plutonium-bearing materials containing at least 30 wt.% plutonium and uranium. Three nested containers are typically used, the outer, inner, and convenience containers, shown in Figure 1. Both the outer and inner containers are sealed with a weld while the innermost convenience container must not be sealed. Lifetime of the containers is expected to be fifty years. The containers are fabricated of austenitic stainless steels (SS) due to their high corrosion resistance. Potential failure mechanisms of the storage containers have beenmore » examined by Kolman and Lillard et al.« less
New Organic Scintillators for Neutron Detection
2016-03-01
highly enriched uranium and weapons grade plutonium. Neutrons and gamma rays are two signatures of these materials. Gamma ray detection techniques are...New Organic Scintillators for Neutron Detection Distribution Statement A. Approved for public release; distribution is unlimited. March...Title: New Organic Scintillators for Neutron Detection I. Abstract In this project, Radiation Monitoring Devices (RMD) proposes to develop novel
SEPARATION OF URANIUM AND PLUTONIUM OXIDES
Benedict, G.E.; Lyon, W.L.
1961-12-01
ABS>A method of separating a mixture of UO/sub 2/ and PuO/sub 2/ is given which comprises immersing the mixture in a fused NaCl-KCl bath, chlorinating with chlorine or phosgene, and preferentially electrolytically or chemically reducing the UO/sub 2/Cl/sub 2/ so produced to UO/sub 2/ and filtering it out. (AEC)
Process for making a ceramic composition for immobilization of actinides
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
TODOSOW,M.; KAZIMI,M.
2004-08-01
Issues affecting the implementation, public perception and acceptance of nuclear power include: proliferation, radioactive waste, safety, and economics. The thorium cycle directly addresses the proliferation and waste issues, but optimization studies of core design and fuel management are needed to ensure that it fits within acceptable safety and economic margins. Typical pressurized water reactors, although loaded with uranium fuel, produce 225 to 275 kg of plutonium per gigawatt-year of operation. Although the spent fuel is highly radioactive, it nevertheless offers a potential proliferation pathway because the plutonium is relatively easy to separate, amounts to many critical masses, and does notmore » present any significant intrinsic barrier to weapon assembly. Uranium 233, on the other hand, produced by the irradiation of thorium, although it too can be used in weapons, may be ''denatured'' by the addition of natural, depleted or low enriched uranium. Furthermore, it appears that the chemical behavior of thoria or thoria-urania fuel makes it a more stable medium for the geological disposal of the spent fuel. It is therefore particularly well suited for a once-through fuel cycle. The use of thorium as a fertile material in nuclear fuel has been of interest since the dawn of nuclear power technology due to its abundance and to potential neutronic advantages. Early projects include homogeneous mixtures of thorium and uranium oxides in the BORAX-IV, Indian Point I, and Elk River reactors, as well as heterogeneous mixtures in the Shippingport seed-blanket reactor. However these projects were developed under considerably different circumstances than those which prevail at present. The earlier applications preceded the current proscription, for non-proliferation purposes, of the use of uranium enriched to more than 20 w/o in {sup 235}U, and has in practice generally prohibited the use of uranium highly enriched in {sup 235}U. They were designed when the expected burnup of light water fuel was on the order of 25 MWD/kgU--about half the present day value--and when it was expected that the spent fuel would be recycled to recover its fissile content.« less
León Vintró, L; Mitchell, P I; Omarova, A; Burkitbayev, M; Jiménez Nápoles, H; Priest, N D
2009-04-01
New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel'kem 1 and Tel'kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that (241)Am, (239,240)Pu and (238)U concentrations in well waters within the study area are in the range 0.04-87mBq dm(-3), 0.7-99mBq dm(-3), and 74-213mBq dm(-3), respectively, and for (241)Am and (239,240)Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01mBq dm(-3), 0.08mBq dm(-3) and 0.32mBq dm(-3) for (241)Am, (239,240)Pu and (238)U, respectively. The (235)U/(238)U isotopic ratio in almost all well and stream waters is slightly elevated above the 'best estimate' value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53-85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11-42microSv (mean 21microSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel'kem explosions.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Simmons, Mary Ann; Poston, Ted M.; Fritz, Brad G.
2011-07-29
Environmental monitoring is conducted on the U.S. Department of Energy (DOE) Hanford Site to comply with DOE Orders and federal and state regulations. Major objectives of the monitoring are to characterize contaminant levels in the environment and to determine site contributions to the contaminant inventory. This report focuses on surface soil and perennial vegetation samples collected between 1971 and 2008 as part of the Pacific Northwest National Laboratory Surface Environmental Surveillance Project performed under contract to DOE. Areas sampled under this program are located on the Hanford Site but outside facility boundaries and on public lands surrounding the Hanford Site.more » Additional samples were collected during the past 8 years under DOE projects that evaluated parcels of land for radiological release. These data were included because the same sampling methodology and analytical laboratory were used for the projects. The spatial and temporal trends of six radionuclides collected over a 38-year period were evaluated. The radionuclides----cobalt-60, cesium-137, strontium-90, plutonium-238, plutonium-239/240, and uranium (reported either as uranium-238 or total uranium)----were selected because they persist in the environment and are still being monitored routinely and reported in Hanford Site environmental reports. All these radionuclides were associated with plutonium production and waste management of activities occurring on the site. Other sources include fallout from atmospheric testing of nuclear weapons, which ended in 1980, and the Chernobyl explosion in 1986. Uranium is also a natural component of the soil. This assessment of soil and vegetation data provides important information on the distribution of radionuclides in areas adjacent to industrial areas, established perimeter locations and buffer areas, and more offsite nearby and distant locations. The concentrations reflect a tendency for detection of some radionuclides close to where they were utilized onsite, but as one moves to unindustrialized areas on the site, surrounding buffer areas and perimeter location into the more distant sites, concentrations of these radionuclides approach background and cannot be distinguished from fallout activity. More importantly, concentrations in soil and vegetation samples did not exceed environmental benchmark concentrations, and associated exposure to human and ecological receptors were well below levels that are demonstratively hazardous to human health and the environment.« less
Cola soft drinks for evaluating the bioaccessibility of uranium in contaminated mine soils.
Lottermoser, Bernd G; Schnug, Ewald; Haneklaus, Silvia
2011-08-15
There is a rising need for scientifically sound and quantitative as well as simple, rapid, cheap and readily available soil testing procedures. The purpose of this study was to explore selected soft drinks (Coca-Cola Classic®, Diet Coke®, Coke Zero®) as indicators of bioaccessible uranium and other trace elements (As, Ce, Cu, La, Mn, Ni, Pb, Th, Y, Zn) in contaminated soils of the Mary Kathleen uranium mine site, Australia. Data of single extraction tests using Coca-Cola Classic®, Diet Coke® and Coke Zero® demonstrate that extractable arsenic, copper, lanthanum, manganese, nickel, yttrium and zinc concentrations correlate significantly with DTPA- and CaCl₂-extractable metals. Moreover, the correlation between DTPA-extractable uranium and that extracted using Coca-Cola Classic® is close to unity (+0.98), with reduced correlations for Diet Coke® (+0.66) and Coke Zero® (+0.55). Also, Coca-Cola Classic® extracts uranium concentrations near identical to DTPA, whereas distinctly higher uranium fractions were extracted using Diet Coke® and Coke Zero®. Results of this study demonstrate that the use of Coca-Cola Classic® in single extraction tests provided an excellent indication of bioaccessible uranium in the analysed soils and of uranium uptake into leaves and stems of the Sodom apple (Calotropis procera). Moreover, the unconventional reagent is superior in terms of availability, costs, preparation and disposal compared to traditional chemicals. Contaminated site assessments and rehabilitation of uranium mine sites require a solid understanding of the chemical speciation of environmentally significant elements for estimating their translocation in soils and plant uptake. Therefore, Cola soft drinks have potential applications in single extraction tests of uranium contaminated soils and may be used for environmental impact assessments of uranium mine sites, nuclear fuel processing plants and waste storage and disposal facilities. Copyright © 2011 Elsevier B.V. All rights reserved.
11. AERIAL VIEW LOOKING NORTH AT THE BUILDING 800 ...
11. AERIAL VIEW LOOKING NORTH AT THE BUILDING 800 - AREA COMPLEX. ENRICHED URANIUM COMPONENTS WERE MANUFACTURED IN THIS AREA OF THE SITE. BUILDING 881, IN THE RIGHT FOREGROUND OF THE PHOTOGRAPH, WAS THE ORIGINAL PLANT B. BUILDING 883, USED FOR ROLLING AND FORMING URANIUM COMPONENTS, IS DIRECTLY TO THE NORTH OF BUILDING 881. TO THE EAST OF BUILDING 883 IS BUILDING 885, A RESEARCH AND DEVELOPMENT FACILITY FOR ALLOYS AND NON-PLUTONIUM METALS. IN THE FOREGROUND TO THE WEST OF BUILDING 881 IS AN OFFICE BUILDING, 850 (6/7/90). - Rocky Flats Plant, Bounded by Indiana Street & Routes 93, 128 & 72, Golden, Jefferson County, CO
Hydrothermal Synthesis and Crystal Structures of Actinide Compounds
NASA Astrophysics Data System (ADS)
Runde, Wolfgang; Neu, Mary P.
Since the 1950s actinides have been used to benefit industry, science, health, and national security. The largest industrial application, electricity generation from uranium and thorium fuels, is growing worldwide. Thus, more actinides are being mined, produced, used and processed than ever before. The future of nuclear energy hinges on how these increasing amounts of actinides are contained in each stage of the fuel cycle, including disposition. In addition, uranium and plutonium were built up during the Cold War between the United States and the Former Soviet Union for defense purposes and nuclear energy. These stockpiles have been significantly reduced in the last decade.
METHOD FOR DISSOLVING ZIRCONIUM-URANIUM COMPOSITIONS
Gens, T.A.
1961-07-18
A method is descrioed for treating a zirconium-- uranium composition to form a stable solution from which uranium and other values may be extracted by contacting the composition with at least a 4 molar aqueous solution of ammonium fluoride at a temperature of about 100 deg C, adding a peroxide, in incremental amounts, to the heated solution throughout the period of dissolution until all of the uranium is converted to soluble uranyl salt, adding nitric acid to the resultant solution to form a solvent extraction feed solution to convert the uranyl salt to a solvent extractable state, and thereafter recovering the uranium and other desired values from the feed solution by solvent extraction.
SOLVENT EXTRACTION OF URANIUM VALUES
Feder, H.M.; Ader, M.; Ross, L.E.
1959-02-01
A process is presented for extracting uranium salt from aqueous acidic solutions by organic solvent extraction. It consists in contacting the uranium bearing solution with a water immiscible dialkylacetamide having at least 8 carbon atoms in the molecule. Mentioned as a preferred extractant is dibutylacetamide. The organic solvent is usually used with a diluent such as kerosene or CCl/sub 4/.
Zinn, W.H.
1958-07-01
A fast nuclear reactor system ls described for producing power and radioactive isotopes. The reactor core is of the heterogeneous, fluid sealed type comprised of vertically arranged elongated tubular fuel elements having vertical coolant passages. The active portion is surrounded by a neutron reflector and a shield. The system includes pumps and heat exchangers for the primary and secondary coolant circuits. The core, primary coolant pump and primary heat exchanger are disposed within an irapenforate tank which is filled with the primary coolant, in this case a liquid metal such as Na or NaK, to completely submerge these elements. The tank is completely surrounded by a thick walled concrete shield. This reactor system utilizes enriched uranium or plutonium as the fissionable material, uranium or thorium as a diluent and thorium or uranium containing less than 0 7% of the U/sup 235/ isotope as a fertile material.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bruce J. Mincher; Guiseppe Modolo; Strephen P. Mezyk
2009-01-01
Solvent extraction is the most commonly used process scale separation technique for nuclear applications and it benefits from more than 60 years of research and development and proven experience at the industrial scale. Advanced solvent extraction processes for the separation of actinides and fission products from dissolved nuclear fuel are now being investigated worldwide by numerous groups (US, Europe, Russia, Japan etc.) in order to decrease the radiotoxic inventories of nuclear waste. While none of the advanced processes have yet been implemented at the industrial scale their development studies have sometimes reached demonstration tests at the laboratory scale. Most ofmore » the partitioning strategies rely on the following four separations: 1. Partitioning of uranium and/or plutonium from spent fuel dissolution liquors. 2. Separation of the heat generating fission products such as strontium and cesium. 3. Coextraction of the trivalent actinides and lanthanides. 4. Separation of the trivalent actinides from the trivalent lanthanides. Tributylphosphate (TBP) in the first separation is the basis of the PUREX, UREX and COEX processes, developed in Europe and the US, whereas monoamides as alternatives for TBP are being developed in Japan and India. For the second separation, many processes were developed worldwide, including the use of crown-ether extractants, like the FPEX process developed in the USA, and the CCD-PEG process jointly developed in the USA and Russia for the partitioning of cesium and strontium. In the third separation, phosphine oxides (CMPOs), malonamides, and diglycolamides are used in the TRUEX, DIAMEX and the ARTIST processes, respectively developed in US, Europe and Japan. Trialkylphosphine oxide(TRPO) developed in China, or UNEX (a mixture of several extractants) jointly developed in Russia and the USA allow all actinides to be co-extracted from acidic radioactive liquid waste. For the final separation, soft donor atom-containing ligands such as the bistriazinylbipyridines (BTBPs) or dithiophosphinic acids have been developed in Europe and China to selectively extract the trivalent actinides. However, in the TALSPEAK process developed in the USA, the separation is based on the relatively high affinity of aminopolycarboxylic acid complexants such as DTPA for trivalent actinides over lanthanides. In the DIDPA, SETFICS and the GANEX processes, developed in Japan and France, the group separation is accomplished in a reverse TALSPEAK process. A typical scenario is shown in Figure 1 for the UREX1a (Uranium Extraction version 1a) process. The initial step is the TBP extraction for the separation of recyclable uranium. The second step partitions the short-lived, highly radioactive cesium and strontium to minimize heat loading in the high-level waste repository. The third step is a group separation of the trivalent actinides and lanthanides with the last step being partitioning of the trivalent lanthanides from the actinides.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Trellue, Holly Renee; Fugate, Michael Lynn; Tobin, Stephen Joesph
The Next Generation Safeguards Initiative (NGSI), Office of Nonproliferation and Arms Control (NPAC), National Nuclear Security Administration (NNSA) of the U.S. Department of Energy (DOE) has sponsored a multi-laboratory, university, international partner collaboration to (1) detect replaced or missing pins from spent fuel assemblies (SFA) to confirm item integrity and deter diversion, (2) determine plutonium mass and related plutonium and uranium fissile mass parameters in SFAs, and (3) verify initial enrichment (IE), burnup (BU), and cooling time (CT) of facility declaration for SFAs. A wide variety of nondestructive assay (NDA) techniques were researched to achieve these goals [Veal, 2010 andmore » Humphrey, 2012]. In addition, the project includes two related activities with facility-specific benefits: (1) determination of heat content and (2) determination of reactivity (multiplication). In this research, a subset of 11 integrated NDA techniques was researched using data mining solutions at Los Alamos National Laboratory (LANL) for their ability to achieve the above goals.« less
Preparation of plutonium-bearing ceramics via mechanically activated precursor
NASA Astrophysics Data System (ADS)
Chizhevskaya, S. V.; Stefanovsky, S. V.
2000-07-01
The problem of excess weapons plutonium disposition is suggested to be solved by means of its incorporation in stable ceramics with high chemical durability and radiation resistivity. The most promising host phases for plutonium as well as uranium and neutron poisons (gadolinium, hafnium) are zirconolite, pyrochlore, zircon, zirconia [1,2], and murataite [3]. Their production requires high temperatures and a fine-grained homogeneous precursor to reach final waste form with high quality and low leachability. Currently various routes to homogeneous products preparation such as sol-gel technology, wet-milling, and grinding in a ball or planetary mill are used. The best result demonstrates sol-gel technology but this route is very complicated. An alternative technology for preparation of ceramic precursors is the treatment of the oxide batch with high mechanical energy [4]. Such a treatment produces combination of mechanical (fine milling with formation of various defects, homogenization) and chemical (split bonds with formation of active centers—free radicals, ion-radicals, etc.) effects resulting in higher reactivity of the activated batch.
Method of separating short half-life radionuclides from a mixture of radionuclides
Bray, Lane A.; Ryan, Jack L.
1999-01-01
The present invention is a method of removing an impurity of plutonium, lead or a combination thereof from a mixture of radionuclides that contains the impurity and at least one parent radionuclide. The method has the steps of (a) insuring that the mixture is a hydrochloric acid mixture; (b) oxidizing the acidic mixture and specifically oxidizing the impurity to its highest oxidation state; and (c) passing the oxidized mixture through a chloride form anion exchange column whereupon the oxidized impurity absorbs to the chloride form anion exchange column and the 22.sup.9 Th or 2.sup.27 Ac "cow" radionuclide passes through the chloride form anion exchange column. The plutonium is removed for the purpose of obtaining other alpha emitting radionuclides in a highly purified form suitable for medical therapy. In addition to plutonium; lead, iron, cobalt, copper, uranium, and other metallic cations that form chloride anionic complexes that may be present in the mixture; are removed from the mixture on the chloride form anion exchange column.
Method of separating short half-life radionuclides from a mixture of radionuclides
Bray, L.A.; Ryan, J.L.
1999-03-23
The present invention is a method of removing an impurity of plutonium, lead or a combination thereof from a mixture of radionuclides that contains the impurity and at least one parent radionuclide. The method has the steps of (a) insuring that the mixture is a hydrochloric acid mixture; (b) oxidizing the acidic mixture and specifically oxidizing the impurity to its highest oxidation state; and (c) passing the oxidized mixture through a chloride form anion exchange column whereupon the oxidized impurity absorbs to the chloride form anion exchange column and the {sup 229}Th or {sup 227}Ac ``cow`` radionuclide passes through the chloride form anion exchange column. The plutonium is removed for the purpose of obtaining other alpha emitting radionuclides in a highly purified form suitable for medical therapy. In addition to plutonium, lead, iron, cobalt, copper, uranium, and other metallic cations that form chloride anionic complexes that may be present in the mixture are removed from the mixture on the chloride form anion exchange column. 8 figs.
Environmental aspects of the transuranics. A selected, annotated bibliography. Volume 9
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ensminger, J.T.; Fore, C.S.; Dailey, N.S.
This ninth published bibliography of 589 references is compiled from the Nevada Applied Ecology Information Center`s Data Base on the Environmental Aspects of the Transuranics. The data base was built to provide information support to the Nevada Applied Ecology Group (NAEG) of DOE`s Nevada Operations Office. The general scope covers environmental aspects of uranium and the transuranic elements, with emphasis on plutonium. This annotated bibliography highlights literature on plutonium 238 and 239 and americium 241 in the critical organs of man and animals. Studies on the migration of plutonium and the transplutonics through the environment are also emphasized. Supporting informationmore » on ecology of the Nevada Test Site and reviews and summarizing literature on other radionuclides have been included at the request of the NAEG. The references are arranged by subject category with leading authors appearing alphabetically within each category. Indexes are provided for author(s), geographic location, keywords, taxonomic name, title, and publication description.« less
The current document represents the third volume of a set of three volumes that address the technical basis and requirements for assessing the potential applicability of MNA as part of a ground-water remedy for plumes with nonradionuclide and/or radionuclide inorganic contamina...
Code of Federal Regulations, 2011 CFR
2011-01-01
..., holding or storage vessels for plutonium solutions are designed to avoid criticality problems resulting... windings on a laminated low loss iron core comprised of thin layers typically 2.0 mm (0.08 in) thick or..., and columns with internal turbine mixers), specially designed or prepared for uranium enrichment using...
Code of Federal Regulations, 2012 CFR
2012-01-01
..., holding or storage vessels for plutonium solutions are designed to avoid criticality problems resulting... windings on a laminated low loss iron core comprised of thin layers typically 2.0 mm (0.08 in) thick or..., and columns with internal turbine mixers), specially designed or prepared for uranium enrichment using...
Code of Federal Regulations, 2010 CFR
2010-01-01
..., holding or storage vessels for plutonium solutions are designed to avoid criticality problems resulting... windings on a laminated low loss iron core comprised of thin layers typically 2.0 mm (0.08 in) thick or..., and columns with internal turbine mixers), specially designed or prepared for uranium enrichment using...
Code of Federal Regulations, 2013 CFR
2013-01-01
..., holding or storage vessels for plutonium solutions are designed to avoid criticality problems resulting... windings on a laminated low loss iron core comprised of thin layers typically 2.0 mm (0.08 in) thick or..., and columns with internal turbine mixers), specially designed or prepared for uranium enrichment using...
Code of Federal Regulations, 2014 CFR
2014-01-01
..., holding or storage vessels for plutonium solutions are designed to avoid criticality problems resulting... windings on a laminated low loss iron core comprised of thin layers typically 2.0 mm (0.08 in) thick or..., and columns with internal turbine mixers), specially designed or prepared for uranium enrichment using...
2. VIEW OF THE EXPERIMENT CONTROL PANEL IN 1970. THE ...
2. VIEW OF THE EXPERIMENT CONTROL PANEL IN 1970. THE NUCLEAR SAFETY GROUP CONDUCTED ABOUT 1,700 CRITICAL MASS EXPERIMENTS USING URANIUM AND PLUTONIUM IN SOLUTIONS (900 TESTS), COMPACTED POWDER (300), AND METALLIC FORMS (500). ALL 1,700 CRITICALITY ASSEMBLIES WERE CONTROLLED FROM THIS PANEL. - Rocky Flats Plant, Critical Mass Laboratory, Intersection of Central Avenue & 86 Drive, Golden, Jefferson County, CO
f-Elements in ionic liquids: A synthetic, spectroscopic and electrochemical study
NASA Astrophysics Data System (ADS)
Bhatt, Anand Indravadan
This thesis reports on chemical research directed towards the utilisation of low temperature ionic liquids (LTILs) for the electrorefming of uranium and plutonium from spent nuclear fuel. Initial studies focus on evaluating the relevant physical and electrochemical properties of LTILs. One room temperature ionic liquid, [(CH[3])[3]N(n-C[4]H[9])][N(SO[2]CF[3])[2
Rapid separation and purification of uranium and plutonium from dilute-matrix samples
Armstrong, Christopher R.; Ticknor, Brian W.; Hall, Gregory; ...
2014-03-11
This work presents a streamlined separation and purification approach for trace uranium and plutonium from dilute (carrier-free) matrices. The method, effective for nanogram quantities of U and femtogram to picogram quantities of Pu, is ideally suited for environmental swipe samples that contain a small amount of collected bulk material. As such, it may be applicable for processing swipe samples such as those collected in IAEA inspection activities as well as swipes that are loaded with unknown analytes, such as those implemented in interlaboratory round-robin or proficiency tests. Additionally, the simplified actinide separation could find use in internal laboratory monitoring ofmore » clean room conditions prior to or following more extensive chemical processing. We describe key modifications to conventional techniques that result in a relatively rapid, cost-effective, and efficient U and Pu separation process. We demonstrate the efficacy of implementing anion exchange chromatography in a single column approach. We also show that hydrobromic acid is an effective substitute in lieu of hydroiodoic acid for eluting Pu. Lastly, we show that nitric acid is an effective digestion agent in lieu of perchloric acid and/or hydrofluoric acid. A step by step procedure of this process is detailed.« less
Electrochemical Nucleation and Growth of Uranium and Plutonium from Molten Salts
Tylka, M. M.; Willit, J. L.; Williamson, M. A.
2017-07-18
This work examines the nucleation and growth behavior of uranium and plutonium from molten LiCl-KCl eutectic on inert electrodes using electrochemical techniques. Current-time transients obtained from chronoamperometric experiments were compared with theoretical models to characterize the type of nucleation (progressive or instantaneous) for deposition of U and Pu, and co-deposition of U-Pu, from molten LiCl-KCl at inert electrodes. It was established that the nucleation mode of actinides present as chlorides in molten chloride salts changes from progressive to instantaneous with an increasing concentration of the trivalent actinide ions in the salt. The effect of the material of the working electrodemore » was investigated, and it was found that changing the material from tungsten to silver improves resolvability of the nucleation peaks and allows more accurate analysis of the experimental measurements. Using the nucleation data, diffusion coefficients were obtained for U 3+ and Pu 3+, and were found to be in very good agreement with the values obtained from other studies. Furthermore, the density of nuclei produced during instantaneous nucleation, the rate of nucleation for progressive nucleation, and the radius of the deposited nuclei were evaluated and examined at different overpotentials.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Carmack, Jon; Hayes, Steven; Walters, L. C.
This document explores startup fuel options for a proposed test/demonstration fast reactor. The fuel options considered are the metallic fuels U-Zr and U-Pu-Zr and the ceramic fuels UO 2 and UO 2-PuO 2 (MOX). Attributes of the candidate fuel choices considered were feedstock availability, fabrication feasibility, rough order of magnitude cost and schedule, and the existing irradiation performance database. The reactor-grade plutonium bearing fuels (U-Pu-Zr and MOX) were eliminated from consideration as the initial startup fuels because the availability and isotopics of domestic plutonium feedstock is uncertain. There are international sources of reactor grade plutonium feedstock but isotopics and availabilitymore » are also uncertain. Weapons grade plutonium is the only possible source of Pu feedstock in sufficient quantities needed to fuel a startup core. Currently, the available U.S. source of (excess) weapons-grade plutonium is designated for irradiation in commercial light water reactors (LWR) to a level that would preclude diversion. Weapons-grade plutonium also contains a significant concentration of gallium. Gallium presents a potential issue for both the fabrication of MOX fuel as well as possible performance issues for metallic fuel. Also, the construction of a fuel fabrication line for plutonium fuels, with or without a line to remove gallium, is expected to be considerably more expensive than for uranium fuels. In the case of U-Pu-Zr, a relatively small number of fuel pins have been irradiated to high burnup, and in no case has a full assembly been irradiated to high burnup without disassembly and re-constitution. For MOX fuel, the irradiation database from the Fast Flux Test Facility (FFTF) is extensive. If a significant source of either weapons-grade or reactor-grade Pu became available (i.e., from an international source), a startup core based on Pu could be reconsidered.« less
Processes for metal extraction
NASA Technical Reports Server (NTRS)
Bowersox, David F.
1992-01-01
This report describes the processing of plutonium at Los Alamos National Laboratory (LANL), and operation illustrating concepts that may be applicable to the processing of lunar materials. The toxic nature of plutonium requires a highly closed system for processing lunar surface materials.
SHIPMENT OF TWO DOE-STD-3013 CONTAINERS IN A 9977 TYPE B PACKAGE
DOE Office of Scientific and Technical Information (OSTI.GOV)
Abramczyk, G.; Bellamy, S.; Loftin, B.
2011-06-06
The 9977 is a certified Type B Packaging authorized to ship uranium and plutonium in metal and oxide forms. Historically, the standard container for these materials has been the DOE-STD-3013 which was specifically designed for the long term storage of plutonium bearing materials. The Department of Energy has used the 9975 Packaging containing a single 3013 container for the transportation and storage of these materials. In order to reduce container, shipping, and storage costs, the 9977 Packaging is being certified for transportation and storage of two 3013 containers. The challenges and risks of this content and the 9977s ability tomore » meet the Code of Federal Regulations for the transport of these materials are presented.« less
Preparation of alpha-emitting nuclides by electrodeposition
NASA Astrophysics Data System (ADS)
Lee, M. H.; Lee, C. W.
2000-06-01
A method is described for electrodepositing the alpha-emitting nuclides. To determine the optimum conditions for plating plutonium, the effects of electrolyte concentration, chelating reagent, current, pH of electrolyte and the time of plating on the electrodeposition were investigated on the base of the ammonium oxalate-ammonium sulfate electrolyte containing diethyl triamino pentaacetic acid. An optimized electrodeposition procedure for the determination of plutonium was validated by application to environmental samples. The chemical yield of the optimized method of electrodeposition step in the environmental sample was a little higher than that of Talvitie's method. The developed electrodeposition procedure in this study was applied to determine the radionuclides such as thorium, uranium and americium that the electrodeposition yields were a little higher than those of the conventional method.
Special Nuclear Material Gamma-Ray Signatures for Reachback Analysts
DOE Office of Scientific and Technical Information (OSTI.GOV)
Karpius, Peter Joseph; Myers, Steven Charles
2016-08-29
These are slides on special nuclear material gamma-ray signatures for reachback analysts for an LSS Spectroscopy course. The closing thoughts for this presentation are the following: SNM materials have definite spectral signatures that should be readily recognizable to analysts in both bare and shielded configurations. One can estimate burnup of plutonium using certain pairs of peaks that are a few keV apart. In most cases, one cannot reliably estimate uranium enrichment in an analogous way to the estimation of plutonium burnup. The origin of the most intense peaks from some SNM items may be indirect and from ‘associated nuclides.' Indirectmore » SNM signatures sometimes have commonalities with the natural gamma-ray background.« less
Application of Compton-suppressed self-induced XRF to spent nuclear fuel measurement
NASA Astrophysics Data System (ADS)
Park, Se-Hwan; Jo, Kwang Ho; Lee, Seung Kyu; Seo, Hee; Lee, Chaehun; Won, Byung-Hee; Ahn, Seong-Kyu; Ku, Jeong-Hoe
2017-11-01
Self-induced X-ray fluorescence (XRF) is a technique by which plutonium (Pu) content in spent nuclear fuel can be directly quantified. In the present work, this method successfully measured the plutonium/uranium (Pu/U) peak ratio of a pressurized water reactor (PWR)'s spent nuclear fuel at the Korea atomic energy research institute (KAERI)'s post irradiation examination facility (PIEF). In order to reduce the Compton background in the low-energy X-ray region, the Compton suppression system additionally was implemented. By use of this system, the spectrum's background level was reduced by a factor of approximately 2. This work shows that Compton-suppressed selfinduced XRF can be effectively applied to Pu accounting in spent nuclear fuel.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hopkins, A.; Sutter, C.; Klos, D.B.
2008-07-01
The Department of Energy, Richland Operations Office is preparing to conduct a Comprehensive Environmental Response, Compensation, and Liability Act (CERCLA) removal action for the decontamination and demolition of the above-grade mining structures and equipment at the 216-Z-9 Crib. An investigation of the condition of the mining complex was initiated to determine constraints necessary for safely conducting the removal of the buildings. While crib headspace chemical analysis and nondestructive analysis of the interior of the buildings was completed to address radiological contamination concerns, the primary concern regarding the removal of the above-grade structures located on the crib cover involves determining themore » loading capacity and structural integrity of the crib cover slab. Additional concerns included headspace gases and radionuclide contamination. Until the structural analysis was completed, loading limits on the crib cover had been restricted. Photographic documentation revealed the loss of protective tiles and acid resistant coating from the underside of the cover raising a question of concrete stability. The investigation relied heavily on the use of high resolution photography with high intensity lighting for photographic documentation of the underside of the crib cover, followed by structural analysis of the documentation by a team of qualified engineers. Deployment of a robot crawler with attached camera and positioning of a fixed camera were integral to this structural characterization effort. Results of the photographic documentation were of sufficient quality to allow for bounding decisions to be made regarding the loading of the crib cover while performing the demolition of the mining structures (glovebox, excavator, bucket) and the associated buildings. The 216-Z-9 Crib, also known as the 216 Z-9 Recuplex CAW (CA column waste) Waste Disposal Cavern, the Z-9 Trench and the Z-9 Crib was constructed as an engineered trench with an open area beneath a concrete slab. The crib is located near the Plutonium Finishing Plant (PFP) facility, at the Hanford Nuclear Reservation in Eastern Washington State. The crib was used as a disposal site for effluent chemical and radiological wastes from the recovery of uranium and plutonium through extraction or RECUPLEX process, a method that recovered uranium and plutonium from liquid and solid wastes and scraps from other PFP processes. During its operating life, from 1955 through 1962, the Z-9 Crib received liquid wastes totaling approximately four million liters, or one million gallons. Analyses of the crib soil in seven locations to a depth of up to two meters (six feet) beneath the crib floor indicated that the plutonium content of the crib soil ranged from 50 to 150 kg (the highest concentration measured was 34.5 g/L of soil). While performing the structural evaluation of the crib cover, additional characterization information was obtained on the radiological and chemical conditions of the crib and structures. (authors)« less
Szabo, Zoltan; Zapecza, Otto S.; Oden, Jeannette H.; Rice, Donald E.
2005-01-01
A field sampling experiment was designed using low-flow purging with a portable pump and sample-collection equipment for the collection of water and sediment samples from observation wells screened in the Kirkwood-Cohansey aquifer system to determine radionuclide or trace-element concentrations for various size fractions. Selected chemical and physical characteristics were determined for water samples from observation wells that had not been purged for years. The sampling was designed to define any particulate, colloidal, and solution-phase associations of radionuclides or trace elements in ground water by means of filtration and ultrafiltration techniques. Turbidity was monitored and allowed to stabilize before samples were collected by means of the low-flow purging technique rather than by the traditional method of purging a fixed volume of water at high-flow rates from the observation well. A minimum of four water samples was collected from each observation well. The samples of water from each well were collected in the following sequence. (1) A raw unfiltered sample was collected within the first minutes of pumping. (2) A raw unfiltered sample was collected after at least three casing volumes of water were removed and turbidity stabilized. (3) A sample was collected after the water was filtered with a 0.45-micron filter. (4) A sample was collected after the water passed through a 0.45-micron filter and a 0.003-micron tangential-flow ultrafilter in sequence. In some cases, a fifth sample was collected after the water passed through a 0.45-micron filter and a 0.05-micron filter in sequence to test for colloids of 0.003 microns to 0.05 microns in size. The samples were analyzed for the concentration of manmade radionuclides plutonium-238 and -239 plus -240, and americium-241. The samples also were analyzed for concentrations of uranium-234, -235, and -238 to determine whether uranium-234 isotope enrichment (resulting from industrial processing) is present. A subset of samples was analyzed for concentrations of thorium-232, -230, and -228 to determine if thorium-228 isotope enrichment, also likely to result from industrial processing, is present. Concentrations of plutonium isotopes and americium-241 in the water samples were less than 0.1 picocurie per liter, the laboratory reporting level for these manmade radionuclides, with the exception of one americium-241 concentration from a filtered sample. A sequential split sample from the same well did not contain a detectable concentration of americium-241, however. Other filtered and unfiltered samples of water from the same well did not contain quantities of americium-241 nearly as high as 0.1 pCi/L. Therefore, the presence of americium-241 in a quantifiable concentration in water samples from this well could not be confirmed. Neither plutonium nor americium was detected in samples of settled sediment collected from the bottom of the wells. Concentrations of uranium isotopes (maximum of 0.05 and 0.08 picocuries per liter of uranium-238 and uranium-234, respectively) were measurable in unfiltered samples of turbid water from one well and in the settled bottom sediment from 6 wells (maximum concentrations of 0.25 and 0.20 picocuries per gram of uranium-238 and uranium-234, respectively). The uranium-234/uranium-238 isotopic ratio was near 1:1, which indicates natural uranium. The analytical results, therefore, indicate that no manmade radionuclide contamination is present in any of the well-bottom sediments, or unfiltered or filtered water samples from any of the sampled wells. No evidence of manmade radionuclide contamination was observed in the aquifer as settled or suspended particulates, colloids, or in the dissolved phase.
ACTUAL WASTE TESTING OF GYCOLATE IMPACTS ON THE SRS TANK FARM
DOE Office of Scientific and Technical Information (OSTI.GOV)
Martino, C.
2014-05-28
Glycolic acid is being studied as a replacement for formic acid in the Defense Waste Processing Facility (DWPF) feed preparation process. After implementation, the recycle stream from DWPF back to the high-level waste Tank Farm will contain soluble sodium glycolate. Most of the potential impacts of glycolate in the Tank Farm were addressed via a literature review and simulant testing, but several outstanding issues remained. This report documents the actual-waste tests to determine the impacts of glycolate on storage and evaporation of Savannah River Site high-level waste. The objectives of this study are to address the following: Determine the extentmore » to which sludge constituents (Pu, U, Fe, etc.) dissolve (the solubility of sludge constituents) in the glycolate-containing 2H-evaporator feed. Determine the impact of glycolate on the sorption of fissile (Pu, U, etc.) components onto sodium aluminosilicate solids. The first objective was accomplished through actual-waste testing using Tank 43H and 38H supernatant and Tank 51H sludge at Tank Farm storage conditions. The second objective was accomplished by contacting actual 2H-evaporator scale with the products from the testing for the first objective. There is no anticipated impact of up to 10 g/L of glycolate in DWPF recycle to the Tank Farm on tank waste component solubilities as investigated in this test. Most components were not influenced by glycolate during solubility tests, including major components such as aluminum, sodium, and most salt anions. There was potentially a slight increase in soluble iron with added glycolate, but the soluble iron concentration remained so low (on the order of 10 mg/L) as to not impact the iron to fissile ratio in sludge. Uranium and plutonium appear to have been supersaturated in 2H-evaporator feed solution mixture used for this testing. As a result, there was a reduction of soluble uranium and plutonium as a function of time. The change in soluble uranium concentration was independent of added glycolate concentration. The change in soluble plutonium content was dependent on the added glycolate concentration, with higher levels of glycolate (5 g/L and 10 g/L) appearing to suppress the plutonium solubility. The inclusion of glycolate did not change the dissolution of or sorption onto actual-waste 2H-evaporator pot scale to an extent that will impact Tank Farm storage and concentration. The effects that were noted involved dissolution of components from evaporator scale and precipitation of components onto evaporator scale that were independent of the level of added glycolate.« less
Hydrolysis of aceto-hydroxamic acid under UREX+ conditions
DOE Office of Scientific and Technical Information (OSTI.GOV)
Alyapyshev, M.; Paulenova, A.; Tkac, P.
2007-07-01
Aceto-hydroxamic acid (AHA) is used as a stripping agent In the UREX process. While extraction yields of uranium remain high upon addition of AHA, hexavalent plutonium and neptunium are rapidly reduced to the pentavalent state while the tetravalent species and removed from the product stream. However, under acidic conditions, aceto-hydroxamic acid undergoes hydrolytic degradation. In this study, the kinetics of the hydrolysis of aceto-hydroxamic acid in nitric and perchloric acid media was investigated at several temperatures. The decrease of the concentration of AHA was determined via its ferric complex using UV-Vis spectroscopy. The data obtained were analyzed using the methodmore » of initial rates. The data follow the pseudo-first order reaction model. Gamma irradiation of AHA/HNO{sub 3} solutions with 33 kGy/s caused two-fold faster degradation of AHA. The rate equation and thermodynamic data will be presented for the hydrolysis reaction with respect to the concentrations of aceto-hydroxamic acid, nitrate and hydronium ions, and radiation dose. (authors)« less
SEPARATION OF THORIUM FROM URANIUM BY EXTRACTION
Bohlmann, E.G.
1959-07-28
A method is presented for the recovery and separation of uranium and thorium values contained in an aqueous nitric acid solution which is more than 3 M in nitric acid. The uranium and thorium containing solution preferable about 7 M in nitric acid is contacted with tributyl phosphatekerosene mixture. Both U and Th are extracted by the immiscible organic. After phase separation the Th is selectively back extracted by contacting with an aqueous nitric acid solution preferably between 0.1 to 1.5 M in nitric acid. The uranium which is still in the organic extractant phase may be recovered by contacting with water.
The role of chemical reactions in the Chernobyl accident
DOE Office of Scientific and Technical Information (OSTI.GOV)
Grishanin, E. I., E-mail: egrishanin@orexovo.net
2010-12-15
It is shown that chemical reactions played an essential role in the Chernobyl accident at all of its stages. It is important that the reactor before the explosion was at maximal xenon poisoning, and its reactivity, apparently, was not destroyed by the explosion. The reactivity release due to decay of Xe-235 on the second day after the explosion led to a reactor power of 80-110 MW. Owing to this power, the chemical reactions of reduction of uranium, plutonium, and other metals at a temperature of about 2000 Degree-Sign C occurred in the core. The yield of fission products thus sharplymore » increased. Uranium and other metals flew down in the bottom water communications and rooms. After reduction of the uranium and its separation from the graphite, the chain reaction stopped, the temperature of the core decreased, and the activity yield stopped.« less
NASA Astrophysics Data System (ADS)
Reed, B. Cameron
2014-12-01
The feed materials program of the Manhattan Project was responsible for procuring uranium-bearing ores and materials and processing them into forms suitable for use as source materials for the Project's uranium-enrichment factories and plutonium-producing reactors. This aspect of the Manhattan Project has tended to be overlooked in comparison with the Project's more dramatic accomplishments, but was absolutely vital to the success of those endeavors: without appropriate raw materials and the means to process them, nuclear weapons and much of the subsequent cold war would never have come to pass. Drawing from information available in Manhattan Engineer District Documents, this paper examines the sources and processing of uranium-bearing materials used in making the first nuclear weapons and how the feed materials program became a central foundational component of the postwar nuclear weapons complex.
Simulation on reactor TRIGA Puspati core kinetics fueled with thorium (Th) based fuel element
NASA Astrophysics Data System (ADS)
Mohammed, Abdul Aziz; Pauzi, Anas Muhamad; Rahman, Shaik Mohmmed Haikhal Abdul; Zin, Muhamad Rawi Muhammad; Jamro, Rafhayudi; Idris, Faridah Mohamad
2016-01-01
In confronting global energy requirement and the search for better technologies, there is a real case for widening the range of potential variations in the design of nuclear power plants. Smaller and simpler reactors are attractive, provided they can meet safety and security standards and non-proliferation issues. On fuel cycle aspect, thorium fuel cycles produce much less plutonium and other radioactive transuranic elements than uranium fuel cycles. Although not fissile itself, Th-232 will absorb slow neutrons to produce uranium-233 (233U), which is fissile. By introducing Thorium, the numbers of highly enriched uranium fuel element can be reduced while maintaining the core neutronic performance. This paper describes the core kinetic of a small research reactor core like TRIGA fueled with a Th filled fuel element matrix using a general purpose Monte Carlo N-Particle (MCNP) code.
Simulation on reactor TRIGA Puspati core kinetics fueled with thorium (Th) based fuel element
DOE Office of Scientific and Technical Information (OSTI.GOV)
Mohammed, Abdul Aziz, E-mail: azizM@uniten.edu.my; Rahman, Shaik Mohmmed Haikhal Abdul; Pauzi, Anas Muhamad, E-mail: anas@uniten.edu.my
2016-01-22
In confronting global energy requirement and the search for better technologies, there is a real case for widening the range of potential variations in the design of nuclear power plants. Smaller and simpler reactors are attractive, provided they can meet safety and security standards and non-proliferation issues. On fuel cycle aspect, thorium fuel cycles produce much less plutonium and other radioactive transuranic elements than uranium fuel cycles. Although not fissile itself, Th-232 will absorb slow neutrons to produce uranium-233 ({sup 233}U), which is fissile. By introducing Thorium, the numbers of highly enriched uranium fuel element can be reduced while maintainingmore » the core neutronic performance. This paper describes the core kinetic of a small research reactor core like TRIGA fueled with a Th filled fuel element matrix using a general purpose Monte Carlo N-Particle (MCNP) code.« less
Method for cleaning solution used in nuclear fuel reprocessing
Tallent, O.K.; Crouse, D.J.; Mailen, J.C.
1980-12-17
Nuclear fuel processing solution consisting of tri-n-butyl phosphate and dodecane, with a complex of uranium, plutonium, or zirconium and with a solvent degradation product such as di-n-butyl phosphate therein, is contacted with an aqueous solution of a salt formed from hydrazine and either a dicarboxylic acid or a hydroxycarboxylic acid, thereby removing the aforesaid complex from the processing solution.
PREPARATION OF ACTINIDE-ALUMINUM ALLOYS
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)
1. VIEW IN ROOM 125, BIOASSAY LABORATORY, SHOWN IS THE ...
1. VIEW IN ROOM 125, BIOASSAY LABORATORY, SHOWN IS THE FIRST STEP IN A SIX-STEP PROCESS TO ANALYZE URINE SAMPLES FOR PLUTONIUM AND URANIUM CONTAMINATION. IN THIS STEP, NITRIC ACID IS ADDED TO SAMPLE, AND THE SAMPLE IS BOILED DOWN TO A WHITE POWDER. - Rocky Flats Plant, Health Physics Laboratory, On Central Avenue between Third & Fourth Streets, Golden, Jefferson County, CO
Method for cleaning solution used in nuclear fuel reprocessing
Tallent, Othar K.; Crouse, David J.; Mailen, James C.
1982-01-01
Nuclear fuel processing solution consisting of tri-n-butyl phosphate and dodecane, with a complex of uranium, plutonium, or zirconium and with a solvent degradation product such as di-n-butyl phosphate therein, is contacted with an aqueous solution of a salt formed from hydrazine and either a dicarboxylic acid or a hydroxycarboxylic acid, thereby removing the aforesaid complex from the processing solution.
PREPARATION OF ANHYDROUS CERIUM CHLORIDE, URANIUM BROMIDE OR PLUTONIUM FLUORIDE
Marmon, K.M.; Wichers, E.
1961-05-01
A process is given for preparing anhydrous metal halides and converting metal oxalates to anhydrous metal halides which are free from oxyhalides. In accordance with one embodiment of the invention, cerous chloride is prepared by passing hydrogen chloride gas over hydrated cerous oxalate below lOO deg C until no more gas is absorbed and then continuing the treatmert at higher temperatures.
Fuel element design for the enhanced destruction of plutonium in a nuclear reactor
Crawford, Douglas C.; Porter, Douglas L.; Hayes, Steven L.; Hill, Robert N.
1999-01-01
A uranium-free fuel for a fast nuclear reactor comprising an alloy of Pu, Zr and Hf, wherein Hf is present in an amount less than about 10% by weight of the alloy. The fuel may be in the form of a Pu alloy surrounded by a Zr--Hf alloy or an alloy of Pu--Zr--Hf or a combination of both.
NASA Astrophysics Data System (ADS)
Vislov, I. S.; Pischulin, V. P.; Kladiev, S. N.; Slobodyan, S. M.
2016-08-01
The state and trends in the development of nuclear fuel cycles in nuclear engineering, taking into account the ecological aspects of using nuclear power plants, are considered. An analysis of advantages and disadvantages of nuclear engineering, compared with thermal engineering based on organic fuel types, was carried out. Spent nuclear fuel (SNF) reprocessing is an important task in the nuclear industry, since fuel unloaded from modern reactors of any type contains a large amount of radioactive elements that are harmful to the environment. On the other hand, the newly generated isotopes of uranium and plutonium should be reused to fabricate new nuclear fuel. The spent nuclear fuel also includes other types of fission products. Conditions for SNF handling are determined by ecological and economic factors. When choosing a certain handling method, one should assess these factors at all stages of its implementation. There are two main methods of SNF handling: open nuclear fuel cycle, with spent nuclear fuel assemblies (NFAs) that are held in storage facilities with their consequent disposal, and closed nuclear fuel cycle, with separation of uranium and plutonium, their purification from fission products, and use for producing new fuel batches. The development of effective closed fuel cycles using mixed uranium-plutonium fuel can provide a successful development of the nuclear industry only under the conditions of implementation of novel effective technological treatment processes that meet strict requirements of environmental safety and reliability of process equipment being applied. The diversity of technological processes is determined by different types of NFA devices and construction materials being used, as well as by the composition that depends on nuclear fuel components and operational conditions for assemblies in the nuclear power reactor. This work provides an overview of technological processes of SNF treatment and methods of handling of nuclear fuel assemblies. Based on analysis of modern engineering solutions on SNF regeneration, it has been concluded that new reprocessing technologies should meet the ecological safety requirements, provide a more extensive use of the resource base of nuclear engineering, allow the production of valuable and trace elements on an industrial scale, and decrease radioactive waste release.
United States Transuranium and Uranium Registries
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kathren, R.L.; Filipy, R.E.; Dietert, S.E.
1991-06-01
This report summarizes the primary scientific activities of the United States Transuranium and Uranium Registries for the period October 1, 1989 through September 30, 1990. The Registries are parallel human tissue research programs devoted to the study of the actinide elements in humans. To date there have been 261 autopsy or surgical specimen donations, which include 11 whole bodies. The emphasis of the Registry was directed towards quality improvement and the development of a fully computerized data base that would incorporate not only the results of postmortem radiochemical analysis, but also medical and monitoring information obtained during life. Human subjectsmore » reviews were also completed. A three compartment biokinetic model for plutonium distribution is proposed. 2 tabs.« less
Development of Novel Sorbents for Uranium Extraction from Seawater
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lin, Wenbin; Taylor-Pashow, Kathryn
2014-01-08
As the uranium resource in terrestrial ores is limited, it is difficult to ensure a long-term sustainable nuclear energy technology. The oceans contain approximately 4.5 billion tons of uranium, which is one thousand times the amount of uranium in terrestrial ores. Development of technologies to recover the uranium from seawater would greatly improve the uranium resource availability, sustaining the fuel supply for nuclear energy. Several methods have been previously evaluated including solvent extraction, ion exchange, flotation, biomass collection, and adsorption; however, none have been found to be suitable for reasons such as cost effectiveness, long term stability, and selectivity. Recentmore » research has focused on the amidoxime functional group as a promising candidate for uranium sorption. Polymer beads and fibers have been functionalized with amidoxime functional groups, and uranium adsorption capacities as high as 1.5 g U/kg adsorbent have recently been reported with these types of materials. As uranium concentration in seawater is only ~3 ppb, great improvements to uranium collection systems must be made in order to make uranium extraction from seawater economically feasible. This proposed research intends to develop transformative technologies for economic uranium extraction from seawater. The Lin group will design advanced porous supports by taking advantage of recent breakthroughs in nanoscience and nanotechnology and incorporate high densities of well-designed chelators into such nanoporous supports to allow selective and efficient binding of uranyl ions from seawater. Several classes of nanoporous materials, including mesoporous silica nanoparticles (MSNs), mesoporous carbon nanoparticles (MCNs), meta-organic frameworks (MOFs), and covalent-organic frameworks (COFs), will be synthesized. Selective uranium-binding liagnds such as amidoxime will be incorporated into the nanoporous materials to afford a new generation of sorbent materials that will be evaluated for their uranium extraction efficiency. The initial testing of these materials for uranium binding will be carried out in the Lin group, but more detailed sorption studies will be carried out by Dr. Taylor-Pashow of Savannah River National Laboratory in order to obtain quantitative uranyl sorption selectivity and kinetics data for the proposed materials. The proposed nanostructured sorbent materials are expected to have higher binding capacities, enhanced extraction kinetics, optimal stripping efficiency for uranyl ions, and enhanced mechanical and chemical stabilities. This transformative research will significantly impact uranium extraction from seawater as well as benefit DOE’s efforts on environmental remediation by developing new materials and providing knowledge for enriching and sequestering ultralow concentrations of other metals.« less
NASA Astrophysics Data System (ADS)
Streicher, Michael; Brown, Steven; Zhu, Yuefeng; Goodman, David; He, Zhong
2016-10-01
To accurately characterize shielded special nuclear materials (SNM) using passive gamma-ray spectroscopy measurement techniques, the effective atomic number and the thickness of shielding materials must be measured. Intervening materials between the source and detector may affect the estimated source isotopics (uranium enrichment and plutonium grade) for techniques which rely on raw count rates or photopeak ratios of gamma-ray lines separated in energy. Furthermore, knowledge of the surrounding materials can provide insight regarding the configuration of a device containing SNM. The described method was developed using spectra recorded using high energy resolution CdZnTe detectors, but can be expanded to any gamma-ray spectrometers with energy resolution of better than 1% FWHM at 662 keV. The effective atomic number, Z, and mass thickness of the intervening shielding material are identified by comparing the relative attenuation of different gamma-ray lines and estimating the proportion of Compton scattering interactions to photoelectric absorptions within the shield. While characteristic Kα x-rays can be used to identify shielding materials made of high Z elements, this method can be applied to all shielding materials. This algorithm has adequately estimated the effective atomic number for shields made of iron, aluminum, and polyethylene surrounding uranium samples using experimental data. The mass thicknesses of shielding materials have been estimated with a standard error of less than 1.3 g/cm2 for iron shields up to 2.5 cm thick. The effective atomic number was accurately estimated to 26 ± 5 for all iron thicknesses.
Colloids from the aqueous corrosion of uranium nuclear fuel
NASA Astrophysics Data System (ADS)
Kaminski, M. D.; Dimitrijevic, N. M.; Mertz, C. J.; Goldberg, M. M.
2005-12-01
Colloids may enhance the subsurface transport of radionuclides and potentially compromise the long-term safe operation of the proposed radioactive waste repository at Yucca Mountain. Little data is available on colloid formation for the many different waste forms expected to be buried in the repository. This work expands the sparse database on colloids formed during the corrosion of metallic uranium nuclear fuel. We characterized spherical UO 2 and nickel-rich montmorilonite smectite-clay colloids formed during the corrosion of uranium metal fuel under bathtub conditions at 90 °C. Iron and chromium oxides and calcium carbonate colloids were present but were a minor population. The estimated upper concentration of the UO 2 and clays was 4 × 10 11 and 7 × 10 11-3 × 10 12 particles/L, respectively. However, oxygen eventually oxidized the UO 2 colloids, forming long filaments of weeksite K 2(UO 2) 2Si 6O 15 · 4H 2O that settled from solution, reducing the UO 2 colloid population and leaving predominantly clay colloids. The smectite colloids were not affected by oxygen. Plutonium was not directly observed within the UO 2 colloids but partitioned completely to the colloid size fraction. The plutonium concentration in the colloidal fraction was slightly higher than the value used in the viability assessment model, and does not change in concentration with exposure to oxygen. This paper provides conclusive evidence for single-phase radioactive colloids composed of UO 2. However, its impact on repository safety is probably small since oxygen and silica availability will oxidize and effectively precipitate the UO 2 colloids from concentrated solutions.
Boulyga, Sergei F; Tibi, Markus; Heumann, Klaus G
2004-01-01
The methods available for determination of environmental contamination by plutonium at ultra-trace levels require labor-consuming sample preparation including matrix removal and plutonium extraction in both nuclear spectroscopy and mass spectrometry. In this work, laser-ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) was applied for direct analysis of Pu in soil and sediment samples. Application of a LINA-Spark-Atomizer system (a modified laser ablation system providing high ablation rates) coupled with a sector-field ICP-MS resulted in detection limits as low as 3x10(-13) g g(-1) for Pu isotopes in soil samples containing uranium at a concentration of a few microg g(-1). The isotope dilution (ID) technique was used for quantification, which compensated for matrix effects in LA-ICP-MS. Interferences by UH+ and PbO2+ ions and by the peak tail of 238U+ ions were reduced or separated by use of dry plasma conditions and a mass resolution of 4000, respectively. No other effects affecting measurement accuracy, except sample inhomogeneity, were revealed. Comparison of results obtained for three contaminated soil samples by use of alpha-spectrometry, ICP-MS with sample decomposition, and LA-ICP-IDMS showed, in general, satisfactory agreement of the different methods. The specific activity of (239+240)Pu (9.8 +/- 3.0 mBq g(-1)) calculated from LA-ICP-IDMS analysis of SRM NIST 4357 coincided well with the certified value of 10.4 +/- 0.2 mBq g(-1). However, the precision of LA-ICP-MS for determination of plutonium in inhomogeneous samples, i.e. if "hot" particles are present, is limited. As far as we are aware this paper reports the lowest detection limits and element concentrations yet measured in direct LA-ICP-MS analysis of environmental samples.
Zalupski, Peter R.; Klaehn, John R.; Peterman, Dean R.
2015-07-30
The feasibility of simultaneous separation of uranium, neptunium, plutonium, americium, and curium from a simulated dissolved used fuel simulant adjusted to 1.0 M nitric acid is investigated using a mixture of the soft donor bis(bis-3,5-trifluoromethyl)phenyl) dithiophosphinic acid (“0”) and the hard donor synergist trioctylphosphine oxide (TOPO) dissolved in toluene. The results reported in this work are compared to our recent demonstration of a complete actinide recovery from a simulated dissolved fuel solution using a synergistic combination of bis(o-trifluoromethylphenyl)dithiophosphinic acid (“1”) and TOPO dissolved in either toluene or trifluoromethylphenyl sulfone. While the extraction efficiency of americium was enhanced for the liquid-liquidmore » system containing “0”, enabling to accomplish a trivalent An/Ln separation at 1.0 M HNO3, the extraction of neptunium was drastically diminished, relative to “1”. The partitioning behavior of curium was also negatively impacted, introducing an effective opportunity for americium/curium separation. Radiometric and spectrophotometric studies demonstrate that the complete actinide recovery using the solvent based upon “0” and TOPO is not feasible. Additionally, the importance of radiolytic degradation processes is discussed through the comparisons of extraction properties of liquid-liquid systems based on both soft donor reagents.« less
Esaka, Fumitaka; Yasuda, Kenichiro; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki
2017-04-01
Isotope ratio analysis of individual uranium-plutonium (U-Pu) mixed oxide particles contained within environmental samples taken from nuclear facilities is proving to be increasingly important in the field of nuclear safeguards. However, isobaric interferences, such as 238 U with 238 Pu and 241 Am with 241 Pu, make it difficult to determine plutonium isotope ratios in mass spectrometric measurements. In the present study, the isotope ratios of 238 Pu/ 239 Pu, 240 Pu/ 239 Pu, 241 Pu/ 239 Pu, and 242 Pu/ 239 Pu were measured for individual Pu and U-Pu mixed oxide particles by a combination of alpha spectrometry and inductively coupled plasma mass spectrometry (ICP-MS). As a consequence, we were able to determine the 240 Pu/ 239 Pu, 241 Pu/ 239 Pu, and 242 Pu/ 239 Pu isotope ratios with ICP-MS after particle dissolution and chemical separation of plutonium with UTEVA resins. Furthermore, 238 Pu/ 239 Pu isotope ratios were able to be calculated by using both the 238 Pu/( 239 Pu+ 240 Pu) activity ratios that had been measured through alpha spectrometry and the 240 Pu/ 239 Pu isotope ratios determined through ICP-MS. Therefore, the combined use of alpha spectrometry and ICP-MS is useful in determining plutonium isotope ratios, including 238 Pu/ 239 Pu, in individual U-Pu mixed oxide particles. Copyright © 2016 Elsevier B.V. All rights reserved.
SEPARATION OF PLUTONIUM FROM ELEMENTS HAVING AN ATOMIC NUMBER NOT LESS THAN 92
Fitch, F.T.; Russell, D.S.
1958-09-16
other elements having atomic numbers nnt less than 92, It has been proposed in the past to so separate plutonium by solvent extraction iato an organic solvent using triglycoldichlcride as the organic solvent. The improvement lies in the discovery that triglycoldichloride performs far more efflciently as an extractant, wher certain second organie compounds are added to it. Mentioned as satisfactory additive compounds are benzaldehyde, saturated aliphatic aldehydes containtng at least twc carbon atoms, and certain polyhydric phenols.
Uranium extraction by complexation with siderophores
NASA Astrophysics Data System (ADS)
Bahamonde Castro, Cristina
One of the major concerns of energy production is the environmental impact associated with the extraction of natural resources. Nuclear energy fuel is obtained from uranium, an abundant and naturally occurring element in the environment, but the currently used techniques for uranium extraction leave either a significant fingerprint (open pit mines) or a chemical residue that alters the pH of the environment (acid or alkali leaching). It is therefore clear that a new and greener approach to uranium extraction is needed. Bioleaching is one potential alternative. In bioleaching, complexants naturally produced from fungi or bacteria may be used to extract the uranium. In the following research, the siderophore enterobactin, which is naturally produced by bacteria to extract and solubilize iron from the environment, is evaluated to determine its potential for complexing with uranium. To determine whether enterobactin could be used for uranium extraction, its acid dissociation and its binding strength with the metal of interest must be determined. Due to the complexity of working with radioactive materials, lanthanides were used as analogs for uranium. In addition, polyprotic acids were used as structural and chemical analogs for the siderophore during method development. To evaluate the acid dissociation of enterobactin and the subsequent binding constants with lanthanides, three different analytical techniques were studied including: potentiometric titration, UltraViolet Visible (UV-Vis) spectrophotometry and Isothermal Titration Calorimetry (ITC). After evaluation of three techniques, a combination of ITC and potentiometric titrations was deemed to be the most viable way for studying the siderophore of interest. The results obtained from these studies corroborate the ideal pH range for enterobactin complexation to the lanthanide of interest and pave the way for determining the strength of complexation relative to other naturally occurring metals. Ultimately, this fundamental research enhances our current understanding of heavy metal complexation to naturally occurring complexants, which may enhance the metals mobility in the environment or potentially be used as a greener alternative in uranium extraction or remediation.
Performance evaluation of two-stage fuel cycle from SFR to PWR
DOE Office of Scientific and Technical Information (OSTI.GOV)
Fei, T.; Hoffman, E.A.; Kim, T.K.
2013-07-01
One potential fuel cycle option being considered is a two-stage fuel cycle system involving the continuous recycle of transuranics in a fast reactor and the use of bred plutonium in a thermal reactor. The first stage is a Sodium-cooled Fast Reactor (SFR) fuel cycle with metallic U-TRU-Zr fuel. The SFRs need to have a breeding ratio greater than 1.0 in order to produce fissile material for use in the second stage. The second stage is a PWR fuel cycle with uranium and plutonium mixed oxide fuel based on the design and performance of the current state-of-the-art commercial PWRs with anmore » average discharge burnup of 50 MWd/kgHM. This paper evaluates the possibility of this fuel cycle option and discusses its fuel cycle performance characteristics. The study focuses on an equilibrium stage of the fuel cycle. Results indicate that, in order to avoid a positive coolant void reactivity feedback in the stage-2 PWR, the reactor requires high quality of plutonium from the first stage and minor actinides in the discharge fuel of the PWR needs to be separated and sent back to the stage-1 SFR. The electricity-sharing ratio between the 2 stages is 87.0% (SFR) to 13.0% (PWR) for a TRU inventory ratio (the mass of TRU in the discharge fuel divided by the mass of TRU in the fresh fuel) of 1.06. A sensitivity study indicated that by increasing the TRU inventory ratio to 1.13, The electricity generation fraction of stage-2 PWR is increased to 28.9%. The two-stage fuel cycle system considered in this study was found to provide a high uranium utilization (>80%). (authors)« less
Assessment of a French scenario with the INPRO methodology
DOE Office of Scientific and Technical Information (OSTI.GOV)
Vasile, A.; Fiorini, G.L.; Cazalet, J.
2006-07-01
This paper presents the French contribution to the Joint Study of the IAEA International Project on Innovative Nuclear Reactors and Fuel Cycles (INPRO). It concerns the application of the INPRO methodology to a French scenario, on the transition from present LWRs to EPRs in a first phase and to 4. generation fast reactors in a second phase during the 21. century. The scenario also considers the renewal of the present fuel cycle facilities by the third and the fourth generation ones. Present practice of plutonium recycling in PWR is replaced by the middle of the century by a global recyclingmore » of actinides, uranium, plutonium and minor actinides in fast reactors. The status and the evolution of the INPRO criteria and the corresponding indicators during the studied period are analyzed for each of the six considered areas: economics, safety, environment, waste management, proliferation resistance and infrastructure. Improvements on economic and safety are expected for both the EPR and the 4. generation systems having these improvements among their basic goals. The use of fast reactors and global recycling of actinides leads to a significant improvement on environment indicators and in particular on the natural resources utilization. The envisaged waste management policy results in significant reductions on mass, thermal loads and radiotoxicity of the final waste which only contains fission products. The use of fuels that do not relay on enriched uranium and separated plutonium increases the proliferation resistance characteristics of the future fuel cycle. The paper summarizes also some recommendations on the data, codes and methods used to support the continuous improvement of the INPRO methodology and help future assessors. (authors)« less
Yeager, J.H.
1958-08-12
In the prior art processing of uranium ores, the ore is flrst digested with nitric acid and filtered, and the uranium values are then extracted tom the filtrate by contacting with an organic solvent. The insoluble residue has been processed separately in order to recover any uranium which it might contain. The improvement consists in contacting a slurry, composed of both solution and residue, with the organic solvent prior to filtration. Tbe result is that uranium values contained in the residue are extracted along with the uranium values contained th the solution in one step.
Determination of actinides in urine and fecal samples
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.
U.S. and South Korean Cooperation in the World Nuclear Energy Market: Major Policy Considerations
2010-01-21
a laboratory-scale research program on reprocessing spent fuel with an advanced pyroprocessing technique. However, the level of consensus over the... pyroprocessing option among government agencies, Korean electric utilities, and the public remains uncertain. The current U.S.-Korea 123 agreement...permission. KAERI’s pyroprocessing technology would partially separate plutonium and uranium from spent fuel, but the United States has not allowed the
Determination of actinides in urine and fecal samples
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.
Fuel element design for the enhanced destruction of plutonium in a nuclear reactor
Crawford, D.C.; Porter, D.L.; Hayes, S.L.; Hill, R.N.
1999-03-23
A uranium-free fuel for a fast nuclear reactor comprising an alloy of Pu, Zr and Hf, wherein Hf is present in an amount less than about 10% by weight of the alloy. The fuel may be in the form of a Pu alloy surrounded by a Zr--Hf alloy or an alloy of Pu--Zr--Hf or a combination of both. 7 figs.
Hazardous Waste Surveys of Two Army Installations and an Army Hospital.
1980-08-01
232 Nickel-63 Uranium-238 Plutonium-239 Polonium - 210 6 Army Medical Treatment Facilities: General Administration Army Regulation (AR) 40-2, 42A peren...Categories 10 2 Waste Matrix 14 3 Search Format 16 4 Field Sanitation Unit Personal Health Supplies 19 5 Company Vehicle Maintenance Supplies...increasing industrialization of society, coupled with an equally increasing environmental and health safety awareness, has created a long list of wastes
Recovery of Uranium from Wet Phosphoric Acid by Solvent Extraction Processes
Beltrami, Denis; Cote, Gérard; Mokhtari, Hamid; ...
2014-11-17
Between 1951 and 1991, we developed about 17 processes to recover uranium from wet phosphoric acid (WPA), but the viability of these processes was subject to the variation of the uranium price market. Nowadays, uranium from WPA appears to be attractive due to the increase of the global uranium demand resulting from the emergence of developing countries. Moreover, the increasing demand provides impetus for a new look at the applicable technology with a view to improvements as well as altogether new approaches. This paper gives an overview on extraction processes developed in the past to recover uranium from wet phosphoricmore » acid (WPA) as well as the physicochemistry involved in these processes. Recent advances concerning the development of new extraction systems are also reported and discussed.« less
NASA Astrophysics Data System (ADS)
Roycroft, S. J.; Noel, V.; Boye, K.; Besancon, C.; Weaver, K. L.; Johnson, R. H.; Dam, W. L.; Fendorf, S. E.; Bargar, J.
2016-12-01
Uranium contaminated groundwater in Riverton, Wyoming persists despite anticipated natural attenuation outside of a former uranium ore processing facility. The inability of natural flushing to dilute the uranium below the regulatory threshold indicates that sediments act as secondary sources likely (re)supplying uranium to groundwater. Throughout the contaminated floodplain, uranium rich-evaporites are readily abundant in the upper 2 m of sediments and are spatially coincident with the location of the plume, which suggests a likely link between evaporites and increased uranium levels. Knowledge of where and how uranium is stored within evaporite-associated sediments is required to understand processes controlling the mobility of uranium. We expect that flooding and seasonal changes in hydrologic conditions will affect U phase partitioning, and thus largely control U mobility. The primary questions we are addressing in this project are: What is the relative abundance of uranium incorporated in various mineral complexes throughout the evaporite sediments? How do the factors of depth, location, and seasonality influence the relative incorporation, mobility and speciation of uranium?We have systematically sampled from two soil columns over three dates in Riverton. The sampling dates span before and after a significant flooding event, providing insight into the flood's impact on local uranium mobility. Sequential chemical extractions are used to decipher the reactivity of uranium and approximate U operationally defined within reactants targeting carbonate, silicate, organic, and metal oxide bound or water and exchangeable phases. Extractions throughout the entirety of the sediment cores provide a high-resolution vertical profile of the distribution of uranium in various extracted phases. Throughout the profile, the majority (50-60%) of uranium is bound within carbonate-targeted extracts, a direct effect of the carbonate-rich evaporite sediments. The sum of our analyses provide a dynamic model of uranium incorporation within evaporite sediments holding implications for the fate of uranium throughout contaminated sites across the Colorado River Basin.
Extractive separation of uranium and zirconium sulfates by amines
DOE Office of Scientific and Technical Information (OSTI.GOV)
Schroetterova, D.; Nekovar, P.; Mrnka, M.
1992-04-01
This paper describes an amine extraction process for zirconium and uranium separation. The behaviour of an extraction system containing uranium (VI) sulfate, zirconium (IV) sulfate, 0.2 and 0.5 M sulfuric acid (as the original aqueous phase), tertiary amine tri-n-lauryl- amine or primary amine Primene JMT in benzene (as the original organic phase) is discussed on the basis of equilibrium data. The measured dependences show that the degree of extraction of zirconium at the sulfuric acid concentration of 0.5 M and above is only slightly affected by a presence of uranium in solution. From this surprising behaviour it follows that zirconiummore » may be employed for the displacement of uranium from the organic phase. This effect is more pronounced with the primary amine Primene JMT than with TLA. 29 refs., 4 figs., 1 tab.« less
Uranium extraction: Fuel from seawater
Tsouris, Costas; Oak Ridge National Lab.
2017-02-17
Over four billion tonnes of uranium are currently in the oceans that could be harvested for nuclear fuel, but current capture methods have limited performance and reusability. Now, an electrochemical method using modified carbon electrodes is shown to be promising for the extraction of uranium from seawater.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Baruzzini, Matthew Louis
The precise and accurate determination of isotopic composition in nuclear forensic samples is vital for assessing origin, intended use and process history. Thermal ionization mass spectrometry (TIMS) is widely accepted as the gold standard for high performance isotopic measurements and has long served as the workhorse in the isotopic ratio determination of nuclear materials. Nuclear forensic and safeguard specialists have relied heavily on such methods for both routine and atypical e orts. Despite widespread use, TIMS methods for the assay of actinide systems continue to be hindered by poor ionization e ciency, often less than tenths of a percent; themore » majority of a sample is not measured. This represents a growing challenge in addressing nextgeneration nuclear detection needs by limiting the ability to analyze ultratrace quantities of high priority elements that could potentially provide critical nuclear forensic signatures. Porous ion emitter (PIE) thermal ion sources were developed in response to the growing need for new TIMS ion source strategies for improved ionization e ciency, PIEs have proven to be simple to implement, straightforward approach to boosting ion yield. This work serves to expand the use of PIE techniques for the analysis of trace quantities of plutonium and americium. PIEs exhibited superior plutonium and americium ion yields when compared to direct lament loading and the resin bead technique, one of the most e cient methods for actinide analysis, at similar mass loading levels. Initial attempts at altering PIE composition for the analysis of plutonium proved to enhance sample utilization even further. Preliminary investigations of the instrumental fractionation behavior of plutonium and uranium analyzed via PIE methods were conducted. Data collected during these initial trial indicate that PIEs fractionate in a consistent, reproducible manner; a necessity for high precision isotope ratio measurements. Ultimately, PIEs methods were applied for the age determination of various uranium isotopic standards. PIEs did not exhibit signi cant advantages for the determination of model ages when compared to traditional laments; however, this trial was able to provide valuable insight for guiding future investigations.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Moir, R.W.
1982-02-22
The fusion breeder is a fusion reactor designed with special blankets to maximize the transmutation by 14 MeV neutrons of uranium-238 to plutonium or thorium to uranium-233 for use as a fuel for fission reactors. Breeding fissile fuels has not been a goal of the US fusion energy program. This paper suggests it is time for a policy change to make the fusion breeder a goal of the US fusion program and the US nuclear energy program. The purpose of this paper is to suggest this policy change be made and tell why it should be made, and to outlinemore » specific research and development goals so that the fusion breeder will be developed in time to meet fissile fuel needs.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Moir, R.W.
1982-04-20
The fusion breeder is a fusion reactor designed with special blankets to maximize the transmutation by 14 MeV neutrons of uranium-238 to plutonium or thorium to uranium-233 for use as a fuel for fission reactors. Breeding fissile fuels has not been a goal of the US fusion energy program. This paper suggests it is time for a policy change to make the fusion breeder a goal of the US fusion program and the US nuclear energy program. The purpose of this paper is to suggest this policy change be made and tell why it should be made, and to outlinemore » specific research and development goals so that the fusion breeder will be developed in time to meet fissile fuel needs.« less
Report on {open_quotes}audit of internal controls over special nuclear materials{close_quotes}
DOE Office of Scientific and Technical Information (OSTI.GOV)
NONE
1996-04-01
The Department of Energy (Department) is responsible for safeguarding a significant amount of plutonium, uranium-233 and enriched uranium - collectively referred to as special nuclear materials - stored in the United States. The Department`s office of Nonproliferation and National Security has overall management cognizance for developing policies for safeguarding these materials, while other Headquarters program offices have {open_quotes}landlord{close_quotes} responsibilities for the sites where the materials are stored, and the Department`s operations and field offices provide onsite management of contractor operations. The Department`s management and operating contractors, under the direction of the Department, safeguard and account for the special nuclear materialmore » stored at Department sites.« less
Hyde, E.K.; Katzin, L.I.; Wolf, M.J.
1959-07-14
The separation of uranium from a mixture of uranium and thorium by organic solvent extraction from an aqueous solution is described. The uranium is separrted from an aqueous mixture of uranium and thorium nitrates 3 N in nitric acid and containing salting out agents such as ammonium nitrate, so as to bring ihe total nitrate ion concentration to a maximum of about 8 N by contacting the mixture with an immiscible aliphatic oxygen containing organic solvent such as diethyl carbinol, hexone, n-amyl acetate and the like. The uranium values may be recovered from the organic phase by back extraction with water.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Singh, D.K.; Yadav, K.K.; Varshney, L.
The present study deals with the preparation and evaluation of the poly-ethersulfone (PES) based composite beads encapsulating synergistic mixture of D2EHPA and Cyanex 923 (at 4:1 mole ratio) for the separation of uranium from phosphoric acid medium. SEM was used for the characterization of the composite materials. Addition of 1% PVA (polyvinyl alcohol) improved the internal morphology and porosity of the beads. Additionally, microscopic examination of the composite bead confirmed central coconut type cavity surrounded by porous polymer layer of the beads through which exchange of metal ions take place. Effect of various experimental variables including aqueous acidity, metal ionmore » concentration in aqueous feed, concentration of organic extractant inside the beads, extractant to polymer ratio, liquid to solid (L/S) ratio and temperature on the extraction of uranium was studied. Increase in acidity (1-6 M), L/S ratio (1- 10), metal ion concentration (0.2-3 g/L U{sub 3}O{sub 8}) and polymer to extractant ratio (1:4 -1:10) led to decrease in extraction of uranium. At 5.5 M (comparable to wet process phosphoric acid concentration) the extraction of uranium was about 85% at L/S ratio 5. Increase in extractant concentration inside the bead resulted in enhanced extraction of metal ion. Increase in temperature in the range of 30 to 50 Celsius degrees increased the extraction, whereas further increase to 70 C degrees led to the decrease in extraction of uranium. Amongst various reagents tested, stripping of uranium was quantitative by 12% Na{sub 2}CO{sub 3} solution. Polymeric beads were found to be stable and reusable up-to 10 cycles of extraction/stripping. (authors)« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Judge, Elizabeth J.; Berg, John M.; Le, Loan A.
2012-06-18
Laser-induced breakdown spectroscopy (LIBS) was used to analyze a mixed actinide fuel pellet containing 75% UO{sub 2}/20% PuO{sub 2}/3% AmO{sub 2}/2% NpO{sub 2}. The preliminary data shown here is the first report of LIBS analysis of a mixed actinide fuel pellet, to the authors knowledge. The LIBS spectral data was acquired in a plutonium facility at Los Alamos National Laboratory where the sample was contained within a glove box. The initial installation of the glove box was not intended for complete ultraviolet (UV), visible (VIS) and near infrared (NIR) transmission, therefore the LIBS spectrum is truncated in the UV andmore » NIR regions due to the optical transmission of the window port and filters that were installed. The optical collection of the emission from the LIBS plasma will be optimized in the future. However, the preliminary LIBS data acquired is worth reporting due to the uniqueness of the sample and spectral data. The analysis of several actinides in the presence of each other is an important feature of this analysis since traditional methods must chemically separate uranium, plutonium, neptunium, and americium prior to analysis. Due to the historic nature of the sample fuel pellet analyzed, the provided sample composition of 75% UO{sub 2}/20% PuO{sub 2}/3% AmO{sub 2}/2% NpO{sub 2} cannot be confirm without further analytical processing. Uranium, plutonium, and americium emission lines were abundant and easily assigned while neptunium was more difficult to identify. There may be several reasons for this observation, other than knowing the exact sample composition of the fuel pellet. First, the atomic emission wavelength resources for neptunium are limited and such techniques as hollow cathode discharge lamp have different dynamics than the plasma used in LIBS which results in different emission spectra. Secondly, due to the complex sample of four actinide elements, which all have very dense electronic energy levels, there may be reactions and interactions occurring within the plasma, such as collisional energy transfer, that might be a factor in the reduction in neptunium emission lines. Neptunium has to be analyzed alone using LIBS to further understand the dynamics that may be occurring in the plasma of the mixed actinide fuel pellet sample. The LIBS data suggests that the emission spectrum for the mixed actinide fuel pellet is not simply the sum of the emission spectra of the pure samples but is dependent on the species present in the plasma and the interactions and reactions that occur within the plasma. Finally, many of the neptunium lines are in the near infrared region which is drastically reduced in intensity by the current optical setup and possibly the sensitivity of the emission detector in the spectral region. Once the optics are replaced and the optical collection system is modified and optimized, the probability of observing emission lines for neptunium might be increased significantly. The mixed actinide fuel pellet was analyzed under the experimental conditions listed in Table 1. The LIBS spectra of the fuel pellet are shown in Figures 1-49. The spectra are labeled with the observed wavelength and atomic species (both neutral (I) and ionic (II)). Table 2 is a complete list of the observed and literature based emission wavelengths. The literature wavelengths have references including NIST Atomic Spectra Database (NIST), B.A. Palmer et al. 'An Atlas of Uranium Emission Intensities in a Hollow Cathode Discharge' taken at the Kitt Peak National Observatory (KPNO), R.L. Kurucz 1995 Atomic Line Data from the Smithsonian Astrophysical Observatory (SAO), J. Blaise et al. 'The Atomic Spectrum of Plutonium' from Argonne National Laboratory (BFG), and M. Fred and F.S. Tomkins, 'Preliminary Term Analysis of Am I and Am II Spectra' (FT). The dash (-) shown under Ionic State indicates that the ionic state of the transition was not available. In the spectra, the dash (-) is replaced with a question mark (?). Peaks that are not assigned are most likely real features and not noise but cannot be confidently assigned to a transition without further investigation. Several peaks have multiple assignments due to limited resolution of the spectrometer used (20,000, {lambda}/{Delta}{lambda}) and without the availability, at this point in time, of pure PuO{sub 2}, AmO{sub 2}, and NpO{sub 2} to confirm the identity of the peaks. A different spectrometer was used in the plutonium facility to collect the mixed actinide fuel pellet data (Echelle 3000) than the DUO{sub 2}, ThO{sub 2} and uranium ore previously reported [6-8] (Echelle 4000) which accounts for the slight shift in the observed wavelength of the uranium emission lines.« less
NASA Astrophysics Data System (ADS)
Ye, Fa-wang; Liu, De-chang
2008-12-01
Practices of sandstone-type uranium exploration in recent years in China indicate that the uranium mineralization alteration information is of great importance for selecting a new uranium target or prospecting in outer area of the known uranium ore district. Taking a case study of BASHIBULAKE uranium ore district, this paper mainly presents the technical minds and methods of extracting the reduced alteration information by oil and gas in BASHIBULAKE ore district using ASTER data. First, the regional geological setting and study status in BASHIBULAKE uranium ore district are introduced in brief. Then, the spectral characteristics of altered sandstone and un-altered sandstone in BASHIBULAKE ore district are analyzed deeply. Based on the spectral analysis, two technical minds to extract the remote sensing reduced alteration information are proposed, and the un-mixing method is introduced to process ASTER data to extract the reduced alteration information in BASHIBULAKE ore district. From the enhanced images, three remote sensing anomaly zones are discovered, and their geological and prospecting significances are further made sure by taking the advantages of multi-bands in SWIR of ASTER data. Finally, the distribution and intensity of the reduced alteration information in Cretaceous system and its relationship with the genesis of uranium deposit are discussed, the specific suggestions for uranium prospecting orientation in outer of BASHIBULAKE ore district are also proposed.
Enhancement of Extraction of Uranium from Seawater
DOE Office of Scientific and Technical Information (OSTI.GOV)
Al-Sheikhly, Mohamad; Dietz, Travis; Tsinas, Zois
2016-04-01
Even at a concentration of 3 μg/L, the world’s oceans contain a thousand times more uranium than currently know terrestrial sources. In order to take advantage of this stockpile, methods and materials must be developed to extract it efficiently, a difficult task considering the very low concentration of the element and the competition for extraction by other atoms in seawater such as sodium, calcium, and vanadium. The majority of current research on methods to extract uranium from seawater are vertical explorations of the grafting of amidoxime ligand, which was originally discovered and promoted by Japanese studies in the late 1980s.more » Our study expands on this research horizontally by exploring the effectiveness of novel uranium extraction ligands grafted to the surface of polymer substrates using radiation. Through this expansion, a greater understanding of uranium binding chemistry and radiation grafting effects on polymers has been obtained. While amidoxime-functionalized fabrics have been shown to have the greatest extraction efficiency so far, they suffer from an extensive chemical processing step which involves treatment with powerful basic solutions. Not only does this add to the chemical waste produced in the extraction process and add to the method’s complexity, but it also significantly impacts the regenerability of the amidoxime fabric. The approach of this project has been to utilize alternative, commercially available monomers capable of extracting uranium and containing a carbon-carbon double bond to allow it to be grafted using radiation, specifically phosphate, oxalate, and azo monomers. The use of commercially available monomers and radiation grafting with electron beam or gamma irradiation will allow for an easily scalable fabrication process once the technology has been optimized. The need to develop a cheap and reliable method for extracting uranium from seawater is extremely valuable to energy independence and will extend the quantity of uranium available to the nuclear power industry far into the future. The development of this technology will also promote science in relation to the extraction of other elements from seawater which could expand the known stockpiles of other highly desirable materials.« less
Enhancement of Extraction of Uranium from Seawater – Final Report
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dietz, Travis Cameron; Tsinas, Zois; Tomaszewski, Claire
2016-05-16
Even at a concentration of 3 μg/L, the world’s oceans contain a thousand times more uranium than currently know terrestrial sources. In order to take advantage of this stockpile, methods and materials must be developed to extract it efficiently, a difficult task considering the very low concentration of the element and the competition for extraction by other atoms in seawater such as sodium, calcium, and vanadium. The majority of current research on methods to extract uranium from seawater are vertical explorations of the grafting of amidoxime ligand, which was originally discovered and promoted by Japanese studies in the late 1980s.more » Our study expands on this research horizontally by exploring the effectiveness of novel uranium extraction ligands grafted to the surface of polymer substrates using radiation. Through this expansion, a greater understanding of uranium binding chemistry and radiation grafting effects on polymers has been obtained. While amidoxime-functionalized fabrics have been shown to have the greatest extraction efficiency so far, they suffer from an extensive chemical processing step which involves treatment with powerful basic solutions. Not only does this add to the chemical waste produced in the extraction process and add to the method’s complexity, but it also significantly impacts the regenerability of the amidoxime fabric. The approach of this project has been to utilize alternative, commercially available monomers capable of extracting uranium and containing a carbon-carbon double bond to allow it to be grafted using radiation, specifically phosphate, oxalate, and azo monomers. The use of commercially available monomers and radiation grafting with electron beam or gamma irradiation will allow for an easily scalable fabrication process once the technology has been optimized. The need to develop a cheap and reliable method for extracting uranium from seawater is extremely valuable to energy independence, and will extend the quantity of uranium available to the nuclear power industry far into the future. The development of this technology will also promote science in relation to the extraction of other elements from seawater, which could expand the known stockpiles of other highly desirable materials.« less
Duquène, L; Vandenhove, H; Tack, F; Van Hees, M; Wannijn, J
2010-02-01
The usefulness of uranium concentration in soil solution or recovered by selective extraction as unequivocal bioavailability indices for uranium uptake by plants is still unclear. The aim of the present study was to test if the uranium concentration measured by the diffusive gradient in thin films (DGT) technique is a relevant substitute for plant uranium availability in comparison to uranium concentration in the soil solution or uranium recovered by ammonium acetate. Ryegrass (Lolium perenne L. var. Melvina) is grown in greenhouse on a range of uranium spiked soils. The DGT-recovered uranium concentration (C(DGT)) was correlated with uranium concentration in the soil solution or with uranium recovered by ammonium acetate extraction. Plant uptake was better predicted by the summed soil solution concentrations of UO(2)(2+), uranyl carbonate complexes and UO(2)PO(4)(-). The DGT technique did not provide significant advantages over conventional methods to predict uranium uptake by plants. Copyright 2009 Elsevier Ltd. All rights reserved.
New developments and prospects on COSI, the simulation software for fuel cycle analysis
DOE Office of Scientific and Technical Information (OSTI.GOV)
Eschbach, R.; Meyer, M.; Coquelet-Pascal, C.
2013-07-01
COSI, software developed by the Nuclear Energy Direction of the CEA, is a code simulating a pool of nuclear power plants with its associated fuel cycle facilities. This code has been designed to study various short, medium and long term options for the introduction of various types of nuclear reactors and for the use of associated nuclear materials. In the frame of the French Act for waste management, scenario studies are carried out with COSI, to compare different options of evolution of the French reactor fleet and options of partitioning and transmutation of plutonium and minor actinides. Those studies aimmore » in particular at evaluating the sustainability of Sodium cooled Fast Reactors (SFR) deployment and the possibility to transmute minor actinides. The COSI6 version is a completely renewed software released in 2006. COSI6 is now coupled with the last version of CESAR (CESAR5.3 based on JEFF3.1.1 nuclear data) allowing the calculations on irradiated fuel with 200 fission products and 100 heavy nuclides. A new release is planned in 2013, including in particular the coupling with a recommended database of reactors. An exercise of validation of COSI6, carried out on the French PWR historic nuclear fleet, has been performed. During this exercise quantities like cumulative natural uranium consumption, or cumulative depleted uranium, or UOX/MOX spent fuel storage, or stocks of reprocessed uranium, or plutonium content in fresh MOX fuel, or the annual production of high level waste, have been computed by COSI6 and compared to industrial data. The results have allowed us to validate the essential phases of the fuel cycle computation, and reinforces the credibility of the results provided by the code.« less
NASA Astrophysics Data System (ADS)
Shi, Xue-Ming; Peng, Xian-Jue
2016-09-01
Fusion science and technology has made progress in the last decades. However, commercialization of fusion reactors still faces challenges relating to higher fusion energy gain, irradiation-resistant material, and tritium self-sufficiency. Fusion Fission Hybrid Reactors (FFHR) can be introduced to accelerate the early application of fusion energy. Traditionally, FFHRs have been classified as either breeders or transmuters. Both need partition of plutonium from spent fuel, which will pose nuclear proliferation risks. A conceptual design of a Fusion Fission Hybrid Reactor for Energy (FFHR-E), which can make full use of natural uranium with lower nuclear proliferation risk, is presented. The fusion core parameters are similar to those of the International Thermonuclear Experimental Reactor. An alloy of natural uranium and zirconium is adopted in the fission blanket, which is cooled by light water. In order to model blanket burnup problems, a linkage code MCORGS, which couples MCNP4B and ORIGEN-S, is developed and validated through several typical benchmarks. The average blanket energy Multiplication and Tritium Breeding Ratio can be maintained at 10 and 1.15 respectively over tens of years of continuous irradiation. If simple reprocessing without separation of plutonium from uranium is adopted every few years, FFHR-E can achieve better neutronic performance. MCORGS has also been used to analyze the ultra-deep burnup model of Laser Inertial Confinement Fusion Fission Energy (LIFE) from LLNL, and a new blanket design that uses Pb instead of Be as the neutron multiplier is proposed. In addition, MCORGS has been used to simulate the fluid transmuter model of the In-Zinerater from Sandia. A brief comparison of LIFE, In-Zinerater, and FFHR-E will be given.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Thompson, G H; Thompson, M C
Solvent extraction of /sup 237/Np and /sup 238/Pu from irradiated neptunium is being investigated as a possible replacement for the currently used anion exchange process at the Savannah River Plant. Solvent extraction would reduce separations costs and waste volume and increase the production rate. The major difficulty in solvent extraction processing is maintaining neptunium and plutonium in the extractable IV or VI valence states during initial extraction. This study investigated the stability of these states. Results show that: The extractable M(IV) valence states of neptunium and plutonium are mutually unstable in plant dissolver solution (2 g/l /sup 237/Np, 0.4 g/lmore » /sup 238/Pu, 1.2M Al/sup 3 +/, 4.6M NO/sub 3//sup -/, and 1M H/sup +/). The reaction rates producing inextractable species from extractable M(IV) or M(VI) are fast enough that greater than or equal to 99.9 percent extractable species in /sup 237/Np--/sup 238/Pu mixtures cannot be maintained for a practicable processing period (24 hours).« less
Detection of Nuclear Weapons and Materials: Science, Technologies, Observations
2010-06-04
extensive use of photons, packets of energy with no rest mass and no electrical charge. Electromagnetic radiation consists of photons, and may be measured...bulk property, expressed as mass per unit volume. In general, the densest materials are those of high Z. These properties may be used to detect...SNM by detecting the time pattern of neutron generation. A subcritical mass of highly enriched uranium or weapons-grade plutonium can support a
Code of Federal Regulations, 2013 CFR
2013-01-01
... cracked ammonia gas or hydrogen. (4) Especially Designed or Prepared Systems for the conversion of UO2 to UF4. Conversion of UO2 to UF4 can be performed by reacting UO2 with hydrogen fluoride gas (HF) at 300... hydrolyzed to UO2 using hydrogen and steam. In the second, UF6 is hydrolyzed by solution in water, ammonia is...
Code of Federal Regulations, 2012 CFR
2012-01-01
... cracked ammonia gas or hydrogen. (4) Especially Designed or Prepared Systems for the conversion of UO2 to UF4. Conversion of UO2 to UF4 can be performed by reacting UO2 with hydrogen fluoride gas (HF) at 300... UO2 using hydrogen and steam. In the second, UF6 is hydrolyzed by solution in water, ammonia is added...
Code of Federal Regulations, 2014 CFR
2014-01-01
... cracked ammonia gas or hydrogen. (4) Especially Designed or Prepared Systems for the conversion of UO2 to UF4. Conversion of UO2 to UF4 can be performed by reacting UO2 with hydrogen fluoride gas (HF) at 300... hydrolyzed to UO2 using hydrogen and steam. In the second, UF6 is hydrolyzed by solution in water, ammonia is...
A small, 1400 K, reactor for Brayton space power systems.
NASA Technical Reports Server (NTRS)
Lantz, E.; Mayo, W.
1972-01-01
An investigation was conducted to determine minimum dimensions and minimum weight obtainable in a design for a reactor using uranium-233 nitride or plutonium-239 nitride as fuel. Such a reactor had been considered by Krasner et al. (1971). Present space power status is discussed, together with questions of reactor design and power distribution in the reactor. The characteristics of various reactor types are compared, giving attention also to a zirconium hydride reactor.
JPRS Report, Soviet Union, International Affairs
1990-05-17
was built to produce enriched uranium , and work has been completed on a plant to refine plutonium received from the nuclear electric power plant in... oil . "Have a look," Mikhail Aleksandrovich couldn’t resist saying, summoning his visitor to the window. The latter approached the window slowly...would like to exchange 1,200 metric tons of processed sunflower-seed oil for imports of common consumer goods. But without the permission of the
Nondestructive Assay Data Integration with the SKB-50 Assemblies - FY16 Update
DOE Office of Scientific and Technical Information (OSTI.GOV)
Tobin, Stephen Joseph; Fugate, Michael Lynn; Trellue, Holly Renee
2016-10-28
A project to research the application of non-destructive assay (NDA) techniques for spent fuel assemblies is underway at the Central Interim Storage Facility for Spent Nuclear Fuel (for which the Swedish acronym is Clab) in Oskarshamn, Sweden. The research goals of this project contain both safeguards and non-safeguards interests. These nondestructive assay (NDA) technologies are designed to strengthen the technical toolkit of safeguard inspectors and others to determine the following technical goals more accurately; Verify initial enrichment, burnup, and cooling time of facility declaration for spent fuel assemblies; Detect replaced or missing pins from a given spent fuel assembly tomore » confirm its integrity; and Estimate plutonium mass and related plutonium and uranium fissile mass parameters in spent fuel assemblies. Estimate heat content, and measure reactivity (multiplication).« less