CONCENTRATION AND DECONTAMINATION OF SOLUTIONS CONTAINING PLUTONIUM VALUES BY BISMUTH PHOSPHATE CARRIER PRECIPITATION METHODS

DOEpatents

Seaborg, G.T.; Thompson, S.G.

1960-08-23

A process is given for isolating plutonium present in the tetravalent state in an aqueous solution together with fission products. First, the plutonium and fission products are coprecipitated on a bismuth phosphate carrier. The precipitate obtained is dissolved, and the plutonium in the solution is oxidized to the hexavalent state (with ceric nitrate, potassium dichromate, Pb/ sub 3/O/sub 4/, sodium bismuthate and/or potassium dichromate). Thereafter a carrier for fission products is added (bismuth phosphate, lanthanum fluoride, ceric phosphate, bismuth oxalate, thorium iodate, or thorium oxalate), and the fission-product precipitation can be repeated with one other of these carriers. After removal of the fission-product-containing precipitate or precipitates. the plutonium in the supernatant is reduced to the tetravalent state (with sulfur dioxide, hydrogen peroxide. or sodium nitrate), and a carrier for tetravalent plutonium is added (lanthanum fluoride, lanthanum hydroxide, lanthanum phosphate, ceric phosphate, thorium iodate, thorium oxalate, bismuth oxalate, or niobium pentoxide). The plutonium-containing precipitate is then dissolved in a relatively small volume of liquid so as to obtain a concentrated solution. Prior to dissolution, the bismuth phosphate precipitates first formed can be metathesized with a mixture of sodium hydroxide and potassium carbonate and plutonium-containing lanthanum fluorides with alkali-metal hydroxide. In the solutions formed from a plutonium-containing lanthanum fluoride carrier the plutonium can be selectively precipitated with a peroxide after the pH was adjusted preferably to a value of between 1 and 2. Various combinations of second, third, and fourth carriers are discussed.

SOLVENT EXTRACTION PROCESS FOR PLUTONIUM

DOEpatents

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.

Thromboelastograms of dogs with acute and subacute lesions due to inhalation of americium 241 and plutonium 239 nitrates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kalmykova, Z.I.

1978-01-01

The effects of inhalation of americium 241 and plutonium 231 on the clotting mechanism of dogs were investigated. Thromboelastograms of whole venous blood were used as the method for studying coagulation properties.

SEPARATION OF URANIUM, PLUTONIUM AND FISSION PRODUCTS

DOEpatents

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.

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

Evaluation of the Magnesium Hydroxide Treatment Process for Stabilizing PFP Plutonium/Nitric Acid Solutions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gerber, Mark A.; Schmidt, Andrew J.; Delegard, Calvin H.

2000-09-28

This document summarizes an evaluation of the magnesium hydroxide [Mg(OH)2] process to be used at the Hanford Plutonium Finishing Plant (PFP) for stabilizing plutonium/nitric acid solutions to meet the goal of stabilizing the plutonium in an oxide form suitable for storage under DOE-STD-3013-99. During the treatment process, nitric acid solutions bearing plutonium nitrate are neutralized with Mg(OH)2 in an air sparge reactor. The resulting slurry, containing plutonium hydroxide, is filtered and calcined. The process evaluation included a literature review and extensive laboratory- and bench-scale testing. The testing was conducted using cerium as a surrogate for plutonium to identify and quantifymore » the effects of key processing variables on processing time (primarily neutralization and filtration time) and calcined product properties.« less

Aqueous Nitrate Recovery Line at Los Alamos National Laboratory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Finstad, Casey Charles

2016-06-15

This powerpoint is part of the ADPSM Plutonium Engineering Lecture Series, which is an opportunity for new hires at LANL to get an overview of work done at TA55. It goes into detail about the aqueous nitrate recovery line at Los Alamos National Laboratory.

Method for dissolving delta-phase plutonium

DOEpatents

Karraker, David G.

1992-01-01

A process for dissolving plutonium, and in particular, delta-phase plutonium. The process includes heating a mixture of nitric acid, hydroxylammonium nitrate (HAN) and potassium fluoride to a temperature between 40.degree. and 70.degree. C., then immersing the metal in the mixture. Preferably, the nitric acid has a concentration of not more than 2M, the HAN approximately 0.66M, and the potassium fluoride 0.1M. Additionally, a small amount of sulfamic acid, such as 0.1M can be added to assure stability of the HAN in the presence of nitric acid. The oxide layer that forms on plutonium metal may be removed with a non-oxidizing acid as a pre-treatment step.

SOLVENT EXTRACTION PROCESS FOR SEPARATING URANIUM AND PLUTONIUM FROM AQUEOUS ACIDIC SOLUTIONS OF NEUTRON IRRADIATED URANIUM

DOEpatents

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)

10 CFR Appendix I to Part 110 - Illustrative List of Reprocessing Plant Components Under NRC Export Licensing Authority

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...

10 CFR Appendix I to Part 110 - Illustrative List of Reprocessing Plant Components Under NRC Export Licensing Authority

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...

10 CFR Appendix I to Part 110 - Illustrative List of Reprocessing Plant Components Under NRC Export Licensing Authority

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...

Uncertainty propagation for the coulometric measurement of the plutonium concentration in CRM126 solution provided by JAEA

DOE Office of Scientific and Technical Information (OSTI.GOV)

Morales-Arteaga, Maria

This GUM WorkbenchTM propagation of uncertainty is for the coulometric measurement of the plutonium concentration in a Pu standard material (C126) supplied as individual aliquots that were prepared by mass. The C126 solution had been prepared and as aliquoted as standard material. Samples are aliquoted into glass vials and heated to dryness for distribution as dried nitrate. The individual plutonium aliquots were not separated chemically or otherwise purified prior to measurement by coulometry in the F/H Laboratory. Hydrogen peroxide was used for valence adjustment.

Method for the recovery of actinide elements from nuclear reactor waste

DOEpatents

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.

Conceptual designs of NDA instruments for the NRTA system at the Rokkasho Reprocessing Plant

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, T.K.; Klosterbuer, S.F.; Menlove, H.O.

The authors are studying conceptual designs of selected nondestructive assay (NDA) instruments for the near-real-time accounting system at the rokkasho Reprocessing Plant (RRP) of Japan Nuclear Fuel Limited (JNFL). The JNFL RRP is a large-scale commercial reprocessing facility for spent fuel from boiling-water and pressurized-water reactors. The facility comprises two major components: the main process area to separate and produce purified plutonium nitrate and uranyl nitrate from irradiated reactor spent fuels, and the co-denitration process area to combine and convert the plutonium nitrate and uranyl nitrate into mixed oxide (MOX). The selected NDA instruments for conceptual design studies are themore » MOX-product canister counter, holdup measurement systems for calcination and reduction furnaces and for blenders in the co-denitration process, the isotope dilution gamma-ray spectrometer for the spent fuel dissolver solution, and unattended verification systems. For more effective and practical safeguards and material control and accounting at RRP, the authors are also studying the conceptual design for the UO{sub 3} large-barrel counter. This paper discusses the state-of-the-art NDA conceptual design and research and development activities for the above instruments.« less

Radiolysis of hexavalent plutonium in solutions of uranyl nitrate containing fission product simulants

NASA Astrophysics Data System (ADS)

Rance, Peter J. W.; Zilberman, B. Ya.; Akopov, G. A.

2000-07-01

The effect of the inherent radioactivity on the chemical state of plutonium ions in solution was recognized very shortly after the first macroscopic amounts of plutonium became available and early studies were conducted as part of the Manhattan Project. However, the behavior of plutonium ions, in nitric acid especially, has been found to be somewhat complex, so much so that a relatively modern summary paper included the comment that, "The vast amount of work carried out in nitric acid solutions can not be adequately summarized. Suffice it to say results in these solutions are plagued with irreproducibility and induction periods…" Needless to say, the presence of other ions in solution, as occurs when irradiated nuclear fuel is dissolved, further complicates matters. The purpose of the work described below was to add to the rather small amount of qualitative data available relating to the radiolytic behavior of plutonium in solutions of irradiated nuclear fuel.

Flowsheet Analysis of U-Pu Co-Crystallization Process as a New Reprocessing System

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shunji Homma; Jun-ichi Ishii; Jiro Koga

2006-07-01

A new fuel reprocessing system by U-Pu co-crystallization process is proposed and examined by flowsheet analysis. This reprocessing system is based on the fact that hexavalent plutonium in nitric acid solution is co-crystallized with uranyl nitrate, whereas it is not crystallized when uranyl nitrate does not exist in the solution. The system consists of five steps: dissolution of spent fuel, plutonium oxidation, U-Pu co-crystallization as a co-decontamination, re-dissolution of the crystals, and U re-crystallization as a U-Pu separation. The system requires a recycling of the mother liquor from the U-Pu co-crystallization step and the appropriate recycle ratio is determined bymore » flowsheet analysis such that the satisfactory decontamination is achieved. Further flowsheet study using four different compositions of LWR spent fuels demonstrates that the constant ratio of plutonium to uranium in mother liquor from the re-crystallization step is achieved for every composition by controlling the temperature. It is also demonstrated by comparing to the Purex process that the size of the plant based on the proposed system is significantly reduced. (authors)« less

Selected quality assurance data for water samples collected by the US Geological Survey, Idaho National Engineering Laboratory, Idaho, 1980 to 1988

USGS Publications Warehouse

Wegner, S.J.

1989-01-01

Multiple water samples from 115 wells and 3 surface water sites were collected between 1980 and 1988 for the ongoing quality assurance program at the Idaho National Engineering Laboratory. The reported results from the six laboratories involved were analyzed for agreement using descriptive statistics. The constituents and properties included: tritium, plutonium-238, plutonium-239, -240 (undivided), strontium-90, americium-241, cesium-137, total dissolved chromium, selected dissolved trace metals, sodium, chloride, nitrate, selected purgeable organic compounds, and specific conductance. Agreement could not be calculated for purgeable organic compounds, trace metals, some nitrates and blank sample analyses because analytical uncertainties were not consistently reported. However, differences between results for most of these data were calculated. The blank samples were not analyzed for differences. The laboratory results analyzed using descriptive statistics showed a median agreement between all useable data pairs of 95%. (USGS)

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.

Uncertainty propagation for the coulometric measurement of the plutonium concentration in MOX-PU4.

DOE Office of Scientific and Technical Information (OSTI.GOV)

None, None

This GUM WorkbenchTM propagation of uncertainty is for the coulometric measurement of the plutonium concentration in a Pu standard material (C126) supplied as individual aliquots that were prepared by mass. The C126 solution had been prepared and as aliquoted as standard material. Samples are aliquoted into glass vials and heated to dryness for distribution as dried nitrate. The individual plutonium aliquots were not separated chemically or otherwise purified prior to measurement by coulometry in the F/H Laboratory. Hydrogen peroxide was used for valence adjustment. The Pu assay measurement results were corrected for the interference from trace iron in the solutionmore » measured for assay. Aliquot mass measurements were corrected for air buoyancy. The relative atomic mass (atomic weight) of the plutonium from X126 certoficate was used. The isotopic composition was determined by thermal ionization mass spectrometry (TIMS) for comparison but not used in calculations.« less

DISSOLUTION OF ZIRCONIUM AND ALLOYS THEREFOR

DOEpatents

Swanson, J.L.

1961-07-11

The dissolution of zirconium cladding in a water solution of ammonium fluoride and ammonium nitrate is described. The method finds particular utility in processing spent fuel elements for nuclear reactors. The zirconium cladding is first dissolved in a water solution of ammonium fluoride and ammonium nitrate; insoluble uranium and plutonium fiuorides formed by attack of the solvent on the fuel materiai of the fuel element are then separated from the solution, and the fuel materiai is dissolved in another solution.

Coprocessed nuclear fuels containing (U, Pu) values as oxides, carbides or carbonitrides

DOEpatents

Lloyd, M.H.

1981-01-09

Method for direct coprocessing of nuclear fuels derived from a product stream of fuels reprocessing facility containing uranium, plutonium, and fission product values comprising nitrate stabilization of said stream vacuum concentration to remove water and nitrates, neutralization to form an acid deficient feed solution for the internal gelation mode of sol-gel technology, green spherule formation, recovery and treatment for loading into a fuel element by vibra packed or pellet formation technologies.

Coprocessed nuclear fuels containing (U, Pu) values as oxides, carbides or carbonitrides

DOEpatents

Lloyd, Milton H.

1983-01-01

Method for direct coprocessing of nuclear fuels derived from a product stream of a fuels reprocessing facility containing uranium, plutonium, and fission product values comprising nitrate stabilization of said stream vacuum concentration to remove water and nitrates, neutralization to form an acid deficient feed solution for the internal gelation mode of sol-gel technology, green spherule formation, recovery and treatment for loading into a fuel element by vibra packed or pellet formation technologies.

Microdistribution and Long-Term Retention of 239Pu (NO3)4 in the Respiratory Tracts of an Acutely Exposed Plutonium Worker and Experimental Beagle Dogs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nielsen, Christopher E.; Wilson, Dulaney A.; Brooks, Antone L.

The long-term retention of inhaled soluble forms of plutonium raises concerns as to the potential health effects in persons working in nuclear energy or the nuclear weapons program. The distributions of long-term retained inhaled plutonium-nitrate [239Pu (NO3)4] deposited in the lungs of an accidentally exposed nuclear worker (Human Case 0269) and in the lungs of experimentally exposed beagle dogs with varying initial lung depositions were determined via autoradiographs of selected histological lung, lymph node, trachea, and nasal turbinate tissue sections. These studies showed that both the human and dogs had a non-uniform distribution of plutonium throughout the lung tissue. Fibroticmore » scar tissue effectively encapsulated a portion of the plutonium and prevented its clearance from the body or translocation to other tissues and diminished dose to organ parenchyma. Alpha radiation activity from deposited plutonium in Human Case 0269 was observed primarily along the sub-pleural regions while no alpha activity was seen in the tracheobronchial lymph nodes of this individual. However, relatively high activity levels in the tracheobronchial lymph nodes of the beagles indicated the lymphatic system was effective in clearing deposited plutonium from the lung tissues. In both the human case and beagle dogs, the appearance of retained plutonium within the respiratory tract was inconsistent with current biokinetic models of clearance for soluble forms of plutonium. Bound plutonium can have a marked effect on the dose to the lungs and subsequent radiation exposure has the potential increase in cancer risk.« less

Adaptation of the ICRP publication 66 respiratory tract model to data on plutonium biokinetics for Mayak workers.

PubMed

Khokhryakov, V F; Suslova, K G; Vostrotin, V V; Romanov, S A; Eckerman, K F; Krahenbuhl, M P; Miller, S C

2005-02-01

The biokinetics of inhaled plutonium were analyzed using compartment models representing their behavior within the respiratory tract, the gastrointestinal tract, and in systemic tissues. The processes of aerosol deposition, particle transport, absorption, and formation of a fixed deposit in the respiratory tract were formulated in the framework of the Human Respiratory Tract Model described in ICRP Publication 66. The values of parameters governing absorption and formation of the fixed deposit were established by fitting the model to the observations in 530 autopsy cases. The influence of smoking on mechanical clearance of deposited plutonium activity was considered. The dependence of absorption on the aerosol transportability, as estimated by in vitro methods (dialysis), was demonstrated. The results of this study were compared to those obtained from an earlier model of plutonium behavior in the respiratory tract, which was based on the same set of autopsy data. That model did not address the early phases of respiratory clearance and hence underestimated the committed lung dose by about 25% for plutonium oxides. Little difference in lung dose was found for nitrate forms.

Ceramification: A plutonium immobilization process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rask, W.C.; Phillips, A.G.

1996-05-01

This paper describes a low temperature technique for stabilizing and immobilizing actinide compounds using a combination process/storage vessel of stainless steel, in which measured amounts of actinide nitrate solutions and actinide oxides (and/or residues) are systematically treated to yield a solid article. The chemical ceramic process is based on a coating technology that produces rare earth oxide coatings for defense applications involving plutonium. The final product of this application is a solid, coherent actinide oxide with process-generated encapsulation that has long-term environmental stability. Actinide compounds can be stabilized as pure materials for ease of re-use or as intimate mixtures withmore » additives such as rare earth oxides to increase their degree of proliferation resistance. Starting materials for the process can include nitrate solutions, powders, aggregates, sludges, incinerator ashes, and others. Agents such as cerium oxide or zirconium oxide may be added as powders or precursors to enhance the properties of the resulting solid product. Additives may be included to produce a final product suitable for use in nuclear fuel pellet production. The process is simple and reduces the time and expense for stabilizing plutonium compounds. It requires a very low equipment expenditure and can be readily implemented into existing gloveboxes. The process is easily conducted with less associated risk than proposed alternative technologies.« less

Electrolytic decontamination of conductive materials for hazardous waste management

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wedman, D.E.; Martinez, H.E.; Nelson, T.O.

1996-12-31

Electrolytic removal of plutonium and americium from stainless steel and uranium surfaces has been demonstrated. Preliminary experiments were performed on the electrochemically based decontamination of type 304L stainless steel in sodium nitrate solutions to better understand the metal removal effects of varying cur-rent density, pH, and nitrate concentration parameters. Material removal rates and changes in surface morphology under these varying conditions are reported. Experimental results indicate that an electropolishing step before contamination removes surface roughness, thereby simplifying later electrolytic decontamination. Sodium nitrate based electrolytic decontamination produced the most uniform stripping of material at low to intermediate pH and at sodiummore » nitrate concentrations of 200 g L{sup -1} and higher. Stirring was also observed to increase the uniformity of the stripping process.« less

Ultra-small plutonium oxide nanocrystals: an innovative material in plutonium science.

PubMed

Hudry, Damien; Apostolidis, Christos; Walter, Olaf; Janssen, Arne; Manara, Dario; Griveau, Jean-Christophe; Colineau, Eric; Vitova, Tonya; Prüssmann, Tim; Wang, Di; Kübel, Christian; Meyer, Daniel

2014-08-11

Apart from its technological importance, plutonium (Pu) is also one of the most intriguing elements because of its non-conventional physical properties and fascinating chemistry. Those fundamental aspects are particularly interesting when dealing with the challenging study of plutonium-based nanomaterials. Here we show that ultra-small (3.2±0.9 nm) and highly crystalline plutonium oxide (PuO2 ) nanocrystals (NCs) can be synthesized by the thermal decomposition of plutonyl nitrate ([PuO2 (NO3 )2 ]⋅3 H2 O) in a highly coordinating organic medium. This is the first example reporting on the preparation of significant quantities (several tens of milligrams) of PuO2 NCs, in a controllable and reproducible manner. The structure and magnetic properties of PuO2 NCs have been characterized by a wide variety of techniques (powder X-ray diffraction (PXRD), X-ray absorption fine structure (XAFS), X-ray absorption near edge structure (XANES), TEM, IR, Raman, UV/Vis spectroscopies, and superconducting quantum interference device (SQUID) magnetometry). The current PuO2 NCs constitute an innovative material for the study of challenging problems as diverse as the transport behavior of plutonium in the environment or size and shape effects on the physics of transuranium elements. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

4. VIEW OF ROOM 103 IN 1980. SIX OF THE ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

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

The efficacies of pure LICAM(C) and DTPA for enhancing the elimination of plutonium-238 and americium-241 from rats after their inhalation as nitrate.

PubMed

Stradling, G N; Stather, J W; Gray, S A; Moody, J C; Ellender, M; Hodgson, A

1989-01-01

After the inhalation of 238Pu and 241Am as nitrate, the repeated administration of DTPA is far superior to that of LICAM(C) for enhancing their elimination from the body. The therapeutic efficacies of these chelating agents are however similar after intravenous injection of 238Pu as citrate. It is concluded that DTPA should remain the agent of choice for treating persons contaminated internally with transportable forms of these actinides.

Actinide-contaminated Skin: Comparing Decontamination Efficacy of Water, Cleansing Gels, and DTPA Gels.

PubMed

Tazrart, A; Bolzinger, M A; Lamart, S; Coudert, S; Angulo, J F; Jandard, V; Briançon, S; Griffiths, N M

2018-07-01

Skin contamination by alpha-emitting actinides is a risk to workers during nuclear fuel production and reactor decommissioning. Also, the list of items for potential use in radiological dispersal devices includes plutonium and americium. The actinide chemical form is important and solvents such as tributyl phosphate, used to extract plutonium, can influence plutonium behavior. This study investigated skin fixation and efficacy of decontamination products for these actinide forms using viable pig skin in the Franz cell diffusion system. Commonly used or recommended decontamination products such as water, cleansing gel, diethylenetriamine pentaacetic acid, or octadentate hydroxypyridinone compound 3,4,3-LI(1,2-HOPO), as well as diethylenetriamine pentaacetic acid hydrogel formulations, were tested after a 2-h contact time with the contaminant. Analysis of skin samples demonstrated that more plutonium nitrate is bound to skin as compared to plutonium-tributyl phosphate, and fixation of americium to skin was also significant. The data show that for plutonium-tributyl phosphate all the products are effective ranging from 80 to 90% removal of this contaminant. This may be associated with damage to the skin by this complex and suggests a mechanical/wash-out action rather than chelation. For removal of americium and plutonium, both Trait Rouge cleansing gel and diethylenetriamine pentaacetic acid are better than water, and diethylenetriamine pentaacetic acid hydrogel is better than Osmogel. The different treatments, however, did not significantly affect the activity in deeper skin layers, which suggests a need for further improvement of decontamination procedures. The new diethylenetriamine pentaacetic acid hydrogel preparation was effective in removing americium, plutonium, and plutonium-tributyl phosphate from skin; such a formulation offers advantages and thus merits further assessment.

Comparative uptake of plutonium from soils by Brassica juncea and Helianthus annuus.

PubMed

Lee, J H; Hossner, L R; Attrep, M; Kung, K S

2002-01-01

Plutonium uptake by Brassica juncea (Indian mustard) and Helianthus annuus (sunflower) from soils with varying chemical composition and contaminated with Pu complexes (Pu-nitrate [239Pu(NO3)4], Pu-citrate [239Pu(C6H5O7)], and Pu-diethylenetriaminepentaacetic acid (Pu-DTPA [239Pu-C14H23O10N3]) was investigated. Sequential extraction of soils incubated with applied Pu was used to determine the distribution of Pu in the various soil fractions. The initial Pu activity levels in soils were 44.40-231.25 Bq g(-1) as Pu-nitrate Pu-citrate, or Pu-DTPA. A difference in Pu uptake between treatments of Pu-nitrate and Pu-citrate without chelating agent was observed only with Indian mustard in acidic Crowley soil. The uptake of Pu by plants was increased with increasing DTPA rates, however, the Pu concentration of plants was not proportionally increased with increasing application rate of Pu to soil. Plutonium uptake from Pu-DTPA was significantly higher from the acid Crowley soil than from the calcareous Weswood soil. The uptake of Pu from the soils was higher in Indian mustard than in sunflower. Sequential extraction of Pu showed that the ion-exchangeable Pu fraction in soils was dramatically increased with DTPA treatment and decreased with time of incubation. Extractability of Pu in all fractions was not different when Pu-nitrate and Pu-citrate were applied to the same soil. More Pu was associated with the residual Pu fraction without DTPA application. Consistent trends with time of incubation for other fractions were not apparent. The ion-exchangeable fraction, assumed as plant-available Pu, was significantly higher in acid soil compared with calcareous soil with or without DTPA treatment. When the calcareous soil was treated with DTPA, the ion-exchangeable Pu was comparatively less influenced. This fraction in the soil was more affected with time of incubation. The lowest extractable Pu was from a pH 6.55 Crockett soil that contained the highest clay compared to the other two soils. Extractable soil Pu was largely affected by soil pH and the amounts of clay, salt, metal oxide, and carbonate.

Literature review for oxalate oxidation processes and plutonium oxalate solubility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nash, C. A.

2015-10-01

A literature review of oxalate oxidation processes finds that manganese(II)-catalyzed nitric acid oxidation of oxalate in precipitate filtrate is a viable and well-documented process. The process has been operated on the large scale at Savannah River in the past, including oxidation of 20 tons of oxalic acid in F-Canyon. Research data under a variety of conditions show the process to be robust. This process is recommended for oxalate destruction in H-Canyon in the upcoming program to produce feed for the MOX facility. Prevention of plutonium oxalate precipitation in filtrate can be achieved by concentrated nitric acid/ferric nitrate sequestration of oxalate.more » Organic complexants do not appear practical to sequester plutonium. Testing is proposed to confirm the literature and calculation findings of this review at projected operating conditions for the upcoming campaign.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

MOSTELLER, RUSSELL D.

Previous studies have indicated that ENDF/B-VII preliminary releases {beta}-2 and {beta}-3, predecessors to the recent initial release of ENDF/B-VII.0, produce significantly better overall agreement with criticality benchmarks than does ENDF/B-VI. However, one of those studies also suggests that improvements still may be needed for thermal plutonium cross sections. The current study substantiates that concern by examining criticality benchmarks for unreflected spheres of plutonium-nitrate solutions and for slightly and heavily borated mixed-oxide (MOX) lattices. Results are presented for the JEFF-3.1 and JENDL-3.3 nuclear data libraries as well as ENDF/B-VII.0 and ENDF/B-VI. It is shown that ENDF/B-VII.0 tends to overpredict reactivity formore » thermal plutonium benchmarks over at least a portion of the thermal range. In addition, it is found that additional benchmark data are needed for the deep thermal range.« less

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

Actinide metal processing

DOEpatents

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

1992-03-24

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

ARRAYS OF BOTTLES OF PLUTONIUM NITRATE SOLUTION

DOE Office of Scientific and Technical Information (OSTI.GOV)

Margaret A. Marshall

2012-09-01

In October and November of 1981 thirteen approaches-to-critical were performed on a remote split table machine (RSTM) in the Critical Mass Laboratory of Pacific Northwest Laboratory (PNL) in Richland, Washington using planar arrays of polyethylene bottles filled with plutonium (Pu) nitrate solution. Arrays of up to sixteen bottles were used to measure the critical number of bottles and critical array spacing with a tight fitting Plexiglas® reflector on all sides of the arrays except the top. Some experiments used Plexiglas shells fitted around each bottles to determine the effect of moderation on criticality. Each bottle contained approximately 2.4 L ofmore » Pu(NO3)4 solution with a Pu content of 105 g Pu/L and a free acid molarity H+ of 5.1. The plutonium was of low 240Pu (2.9 wt.%) content. These experiments were sponsored by Rockwell Hanford Operations because of the lack of experimental data on the criticality of arrays of bottles of Pu solution such as might be found in storage and handling at the Purex Facility at Hanford. The results of these experiments were used “to provide benchmark data to validate calculational codes used in criticality safety assessments of [the] plant configurations” (Ref. 1). Data for this evaluation were collected from the published report (Ref. 1), the approach to critical logbook, the experimenter’s logbook, and communication with the primary experimenter, B. Michael Durst. Of the 13 experiments preformed 10 were evaluated. One of the experiments was not evaluated because it had been thrown out by the experimenter, one was not evaluated because it was a repeat of another experiment and the third was not evaluated because it reported the critical number of bottles as being greater than 25. Seven of the thirteen evaluated experiments were determined to be acceptable benchmark experiments. A similar experiment using uranyl nitrate was benchmarked as U233-SOL-THERM-014.« less

METHOD OF SEPARATION

DOEpatents

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.

The effect of x rays, DTPA, and aspirin on the absorption of plutonium from the gastrointestinal tract of rats

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sullivan, M.F.; Gorham, L.S.; Miller, B.M.

To measure the effect of radiation on plutonium transport, rats that were exposed to 250-kVp X rays were given /sup 238/Pu 3 days afterwards by either gavage or injection into a ligated segment of the duodenum. In a second group of experiments, rats were either injected intraduodenally with /sup 238/Pu-DTPA or administered the chelate intravenously and the /sup 238/Pu by gavage. In a third experiment, rats that had been gavaged with 200 or 400 mg/kg/day of aspirin for 2 days were injected intragastrically with /sup 238/Pu nitrate. Results of the first experiment showed a dose-dependent increase in /sup 238/Pu absorptionmore » between 800 and 1500 rad of lower-body X irradiation. Intravenous or intraduodenal injections of DTPA caused a marked increase in /sup 238/Pu absorption but resulted in decreased plutonium deposition in the skeleton and liver. Retention of /sup 238/Pu in the skeleton of rats given aspirin was double that of controls, but the effect on plutonium absorption was less marked than that of DTPA.« less

Uptake and translocation of plutonium in two plant species using hydroponics.

PubMed

Lee, J H; Hossner, L R; Attrep, M; Kung, K S

2002-01-01

This study presents determinations of the uptake and translocation of Pu in Indian mustard (Brassica juncea) and sunflower (Helianthus annuus) from Pu contaminated solution media. The initial activity levels of Pu were 18.50 and 37.00 Bq ml(-1), for Pu-nitrate [239Pu(NO3)4] and for Pu-citrate [239Pu(C6H5O7)+] in nutrient solution. Plutonium-diethylenetriaminepentaacetic acid (DTPA: [239Pu-C14H23O10N3] solution was prepared by adding 0, 5, 10, and 50 microg of DTPA ml(-1) with 239Pu(NO3)4 in nutrient solution. Concentration ratios (CR, Pu concentration in dry plant material/Pu concentration in nutrient solution) and transport indices (Tl, Pu content in the shoot/Pu content in the whole plant) were calculated to evaluate Pu uptake and translocation. All experiments were conducted in hydroponic solution in an environmental growth chamber. Plutonium concentration in the plant tissue was increased with increased Pu contamination. Plant tissue Pu concentration for Pu-nitrate and Pu-citrate application was not correlated and may be dependent on plant species. For plants receiving Pu-DTPA, the Pu concentration was increased in the shoots but decreased in the roots resulting in a negative correlation between the Pu concentrations in the plant shoots and roots. The Pu concentration in shoots of Indian mustard was increased for application rates up to 10 microg DTPA ml(-1) and up to 5 microg DTPA ml(-1) for sunflower. Similar trends were observed for the CR of plants compared to the Pu concentration in the shoots and roots, whereas the Tl was increased with increasing DTPA concentration. Plutonium in shoots of Indian mustard was up to 10 times higher than that in shoots of sunflower. The Pu concentration in the apparent free space (AFS) of plant root tissue of sunflower was more affected by concentration of DTPA than that of Indian mustard.

Plutonium-239 and americium-241 uptake by plants from soil. Final report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brown, K.W.

1979-03-01

Alfalfa was grown in soil contaminated with plutonium-239 dioxide (239PuO2) at a concentration of 29.7 nanocuries per gram (nCi/g). In addition to alfalfa, radishes, wheat, rye, and tomatoes were grown in soils contaminated with americium-241 nitrate (241Am(NO3)3) at a concentration of 189 nCi/g. The length of exposure varied from 52 days for the radishes to 237 days for the alfalfa. The magnitude of plutonium incorporation by the alfalfa as indicated by the concentration ratio, 0.0000025, was similar to previously reported data using other chemical forms of plutonium. The results did indicate, however, that differences in the biological availability of plutoniummore » isotopes do exist. All of the species exposed to americium-241 assimilated and translocated this radioisotope to the stem, leaf, and fruiting structures. The magnitude of incorporation as signified by the concentration ratios varied from 0.00001 for the wheat grass to 0.0152 for the radishes. An increase in the uptake of americium also occurred as a function of time for four of the five plant species. Evidence indicates that the predominant factor in plutonium and americium uptake by plants may involve the chelation of these elements in soils by the action of compounds such as citric acid and/or other similar chelating agents released from plant roots.« less

LITERATURE REVIEW FOR OXALATE OXIDATION PROCESSES AND PLUTONIUM OXALATE SOLUBILITY

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nash, C.

2012-02-03

A literature review of oxalate oxidation processes finds that manganese(II)-catalyzed nitric acid oxidation of oxalate in precipitate filtrate is a viable and well-documented process. The process has been operated on the large scale at Savannah River in the past, including oxidation of 20 tons of oxalic acid in F-Canyon. Research data under a variety of conditions show the process to be robust. This process is recommended for oxalate destruction in H-Canyon in the upcoming program to produce feed for the MOX facility. Prevention of plutonium oxalate precipitation in filtrate can be achieved by concentrated nitric acid/ferric nitrate sequestration of oxalate.more » Organic complexants do not appear practical to sequester plutonium. Testing is proposed to confirm the literature and calculation findings of this review at projected operating conditions for the upcoming campaign. H Canyon plans to commence conversion of plutonium metal to low-fired plutonium oxide in 2012 for eventual use in the Mixed Oxide Fuel (MOX) Facility. The flowsheet includes sequential operations of metal dissolution, ion exchange, elution, oxalate precipitation, filtration, and calcination. All processes beyond dissolution will occur in HB-Line. The filtration step produces an aqueous filtrate that may have as much as 4 M nitric acid and 0.15 M oxalate. The oxalate needs to be removed from the stream to prevent possible downstream precipitation of residual plutonium when the solution is processed in H Canyon. In addition, sending the oxalate to the waste tank farm is undesirable. This report addresses the processing options for destroying the oxalate in existing H Canyon equipment.« less

Effects of surface applications of biosolids on soil, crops, ground water, and streambed sediment near Deer Trail, Colorado, 1999-2003

USGS Publications Warehouse

Yager, Tracy J.B.; Smith, David B.; Crock, James G.

2004-01-01

The U.S. Geological Survey, in cooperation with Metro Wastewater Reclamation District and North Kiowa Bijou Groundwater Management District, studied natural geochemical effects and the effects of biosolids applications to the Metro Wastewater Reclamation District properties near Deer Trail, Colorado, during 1999 through 2003 because of public concern about potential contamination of soil, crops, ground water, and surface water from biosolids applications. Parameters analyzed for each monitoring component included arsenic, cadmium, copper, lead, mercury, molybdenum, nickel, selenium, and zinc (the nine trace elements regulated by Colorado for biosolids), gross alpha and gross beta radioactivity, and plutonium, as well as other parameters. Concentrations of the nine regulated trace elements in biosolids were relatively uniform and did not exceed applicable regulatory standards. All plutonium concentrations in biosolids were below the minimum detectable level and were near zero. The most soluble elements in biosolids were arsenic, molybdenum, nickel, phosphorus, and selenium. Elevated concentrations of bismuth, mercury, phosphorus, and silver would be the most likely inorganic biosolids signature to indicate that soil or streambed sediment has been affected by biosolids. Molybdenum and tungsten, and to a lesser degree antimony, cadmium, cobalt, copper, mercury, nickel, phosphorus, and selenium, would be the most likely inorganic 'biosolids signature' to indicate ground water or surface water has been affected by biosolids. Soil data indicate that biosolids have had no measurable effect on the concentration of the constituents monitored. Arsenic concentrations in soil of both Arapahoe and Elbert County monitoring sites (like soil from all parts of Colorado) exceed the Colorado soil remediation objectives and soil cleanup standards, which were determined by back-calculating a soil concentration equivalent to a one-in-a-million cumulative cancer risk. Lead concentrations in soil slightly exceed the U.S. Environmental Protection Agency toxicity-derived ecological soil-screening levels for avian wildlife. Plutonium concentration in the soil was near zero. Wheat-grain data were insufficient to determine any measurable effects from biosolids. Comparison with similar data from other parts of North America where biosolids were not applied indicates similar concentrations. However, the Deer Trail study area had higher nickel concentrations in wheat from both the biosolids-applied fields and the control fields. Plutonium content of the wheat was near zero. Ground-water levels generally declined at most wells during 1999 through 2003. Ground-water quality did not correlate with ground-water levels. Vertical ground-water gradients during 1999 through 2003 indicate that bedrock ground-water resources downgradient from the biosolids-applied areas are not likely to be contaminated by biosolids applications unless the gradients change as a result of pumping. Ground-water quality throughout the study area varied over time at each site and from site to site at the same time, but plutonium concentrations in the ground water always were near zero. Inorganic concentrations at well D6 were relatively high compared to other ground-water sites studied. Ground-water pH and concentrations of fluoride, nitrite, aluminum, arsenic, barium, chromium, cobalt, copper, lead, mercury, nickel, silver, zinc, and plutonium in the ground water of the study area met Colorado standards. Concentrations of chloride, sulfate, nitrate, boron, iron, manganese, and selenium exceeded Colorado ground-water standards at one or more wells. Nitrate concentrations at well D6 significantly (alpha = 0.05) exceeded the Colorado regulatory standard. Concentrations of arsenic, cadmium, chromium, lead, mercury, nickel, and zinc in ground water had no significant (alpha = 0.05) upward trends. During 1999-2003, concentrations of nitrate, copper, molybdenum, and selenium

Using Nitrogen and Oxygen Isotope Compositions of Nitrate to Distinguish Contaminant Sources in Hanford Soil and Groundwater

DOE Office of Scientific and Technical Information (OSTI.GOV)

Conrad, Mark; Bill, Markus

2008-08-01

The nitrogen ({delta}{sup 15}N) and oxygen ({delta}{sup 18}O) isotopic compositions of nitrate in the environment are primarily a function of the source of the nitrate. The ranges of isotopic compositions for nitrate resulting from common sources are outlined in Figure 1 from Kendall (1998). As noted on Figure 1, processes such as microbial metabolism can modify the isotopic compositions of the nitrate, but the effects of these processes are generally predictable. At Hanford, nitrate and other nitrogenous compounds were significant components of most of the chemical processes used at the site. Most of the oxygen in nitrate chemicals (e.g., nitricmore » acid) is derived from atmospheric oxygen, giving it a significantly higher {delta}{sup 18}O value (+23.5{per_thousand}) than naturally occurring nitrate that obtains most of its oxygen from water (the {delta}{sup 18}O of Hanford groundwater ranges from -14{per_thousand} to -18{per_thousand}). This makes it possible to differentiate nitrate from Hanford site activities from background nitrate at the site (including most fertilizers that might have been used prior to the Department of Energy plutonium production activities at the site). In addition, the extreme thermal and chemical conditions that occurred during some of the waste processing procedures and subsequent waste storage in select single-shell tanks resulted in unique nitrate isotopic compositions that can be used to identify those waste streams in soil and groundwater at the site (Singleton et al., 2005; Christensen et al., 2007). This report presents nitrate isotope data for soil and groundwater samples from the Hanford 200 Areas and discusses the implications of that data for potential sources of groundwater contamination.« less

Safety analysis, 200 Area, Savannah River Plant: Separations area operations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Perkins, W.C.; Lee, R.; Allen, P.M.

1991-07-01

The nev HB-Line, located on the fifth and sixth levels of Building 221-H, is designed to replace the aging existing HB-Line production facility. The nev HB-Line consists of three separate facilities: the Scrap Recovery Facility, the Neptunium Oxide Facility, and the Plutonium Oxide Facility. There are three separate safety analyses for the nev HB-Line, one for each of the three facilities. These are issued as supplements to the 200-Area Safety Analysis (DPSTSA-200-10). These supplements are numbered as Sup 2A, Scrap Recovery Facility, Sup 2B, Neptunium Oxide Facility, Sup 2C, Plutonium Oxide Facility. The subject of this safety analysis, the, Plutoniummore » Oxide Facility, will convert nitrate solutions of {sup 238}Pu to plutonium oxide (PuO{sub 2}) powder. All these new facilities incorporate improvements in: (1) engineered barriers to contain contamination, (2) barriers to minimize personnel exposure to airborne contamination, (3) shielding and remote operations to decrease radiation exposure, and (4) equipment and ventilation design to provide flexibility and improved process performance.« less

Lung, liver and bone cancer mortality after plutonium exposure in beagle dogs and nuclear workers.

PubMed

Wilson, Dulaney A; Mohr, Lawrence C; Frey, G Donald; Lackland, Daniel; Hoel, David G

2010-01-01

The Mayak Production Association (MPA) worker registry has shown evidence of plutonium-induced health effects. Workers were potentially exposed to plutonium nitrate [(239)Pu(NO(3))(4)] and plutonium dioxide ((239)PuO(2)). Studies of plutonium-induced health effects in animal models can complement human studies by providing more specific data than is possible in human observational studies. Lung, liver, and bone cancer mortality rate ratios in the MPA worker cohort were compared to those seen in beagle dogs, and models of the excess relative risk of lung, liver, and bone cancer mortality from the MPA worker cohort were applied to data from life-span studies of beagle dogs. The lung cancer mortality rate ratios in beagle dogs are similar to those seen in the MPA worker cohort. At cumulative doses less than 3 Gy, the liver cancer mortality rate ratios in the MPA worker cohort are statistically similar to those in beagle dogs. Bone cancer mortality only occurred in MPA workers with doses over 10 Gy. In dogs given (239)Pu, the adjusted excess relative risk of lung cancer mortality per Gy was 1.32 (95% CI 0.56-3.22). The liver cancer mortality adjusted excess relative risk per Gy was 55.3 (95% CI 23.0-133.1). The adjusted excess relative risk of bone cancer mortality per Gy(2) was 1,482 (95% CI 566.0-5686). Models of lung cancer mortality based on MPA worker data with additional covariates adequately described the beagle dog data, while the liver and bone cancer models were less successful.

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

Development of an alternate pathway for materials destined for disposition to WIPP

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ayers, Georgette Y; Mckerley, Bill; Veazey, Gerald W

2010-01-01

The Los Alamos National Laboratory currently has an inventory of process residues that may be viable candidates for disposition to the Waste Isolation Pilot Project (WIPP) located at Carlsbad, New Mexico. A recent 'Attractiveness Level D' exemption allows for the discard of specified intractable materials regardless of the percent plutonium. However, the limits with respect to drum loadings must be met. Cementation is a key component of the aqueous nitrate flowsheet and serves as a 'bleed-off' stream for impurities separated from the plutonium during processing operations. The main 'feed' to the cementation operations are the 'bottoms' from the evaporation process.more » In the majority of cases, the cemented bottoms contain less than the allowed amount per drum for WIPP acceptance. This project would expand the route to WIPP for items that have no defined disposition path, are difficult to process, have been through multiple passes, have no current recovery operations available to recover the plutonium and that are amenable to cementation. This initial work will provide the foundation for a full scale disposition pathway of the candidate materials. Once the pathway has been expanded and a cementation matrix developed, routine discard activities will be initiated.« less

Accumulation, organ distribution, and excretion kinetics of ²⁴¹Am in Mayak Production Association workers.

PubMed

Suslova, Klara G; Sokolova, Alexandra B; Efimov, Alexander V; Miller, Scott C

2013-03-01

Americium-241 (²⁴¹Am) is the second most significant radiation hazard after ²³⁹Pu at some of the Mayak Production Association facilities. This study summarizes current data on the accumulation, distribution, and excretion of americium compared with plutonium in different organs from former Mayak PA workers. Americium and plutonium were measured in autopsy and bioassay samples and correlated with the presence or absence of chronic disease and with biological transportability of the aerosols encountered at different workplaces. The relative accumulation of ²⁴¹Am was found to be increasing in the workers over time. This is likely from ²⁴¹Pu that increases with time in reprocessed fuel and from the increased concentrations of ²⁴¹Am and ²⁴¹Pu in inhaled alpha-active aerosols. While differences were observed in lung retention with exposures to different industrial compounds with different transportabilities (i.e., dioxide and nitrates), there were no significant differences in lung retention between americium and plutonium within each transportability group. In the non-pulmonary organs, the highest ratios of ²⁴¹Am/²⁴¹Am + SPu were observed in the skeleton. The relative ratios of americium in the skeleton versus liver were significantly greater than for plutonium. The relative amounts of americium and plutonium found in the skeleton compared with the liver were even greater in workers with documented chronic liver diseases. Excretion rates of ²⁴¹Am in ‘‘healthy’’ workers were estimated using bioassay and autopsy data. The data suggest that impaired liver function leads to reduced hepatic ²⁴¹Am retention, leading to increased ²⁴¹Am excretion.

Carcinogenesis and Inflammatory Effects of Plutonium-Nitrate Retention in an Exposed Nuclear Worker and Beagle Dogs.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nielsen, Christopher E.; Wang, Xihai; Robinson, Robert J.

The genetic and inflammatory response pathways elicited following plutonium exposure in archival lung tissue of an occupationally exposed human and experimentally exposed beagle dogs were investigated. These pathways include: tissue injury, apoptosis and gene expression modifications related to carcinogenesis and inflammation. In order to determine which pathways are involved, multiple lung samples from a plutonium exposed worker (Case 0269), a human control (Case 0385), and plutonium exposed beagle dogs were examined using histological staining and immunohistochemistry. Examinations were performed to identify target tissues at risk of radiation-induced fibrosis, inflammation, and carcinogenesis. Case 0269 showed interstitial fibrosis in peripheral and subpleuralmore » regions of the lung, but no pulmonary tumors. In contrast, the dogs with similar and higher doses showed pulmonary tumors primarily in brochiolo-alveolar, peripheral and subpleural alveolar regions. The TUNEL assay showed slight elevation of apoptosis in tracheal mucosa, tumor cells, and nuclear debris was present in the inflammatory regions of alveoli and lymph nodes of both the human and the dogs. The expression of apoptosis and a number of chemokine/cytokine genes was slightly but not significantly elevated in protein or gene levels compared to that of the control samples. In the beagles, mucous production was increased in the airway epithelial goblet cells and glands of trachea, and a number of chemokine/cytokine genes showed positive immunoreactivity. This analysis of archival tissue from an accidentally exposed worker and in a large animal model provides valuable information on the effects of long-term retention of plutonium in the respiratory tract and the histological evaluation study may impact mechanistic studies of radiation carcinogenesis.« less

Solubility of Plutonium (IV) Oxalate During Americium/Curium Pretreatment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rudisill, T.S.

1999-08-11

Approximately 15,000 L of solution containing isotopes of americium and curium (Am/Cm) will undergo stabilization by vitrification at the Savannah River Site (SRS). Prior to vitrification, an in-tank pretreatment will be used to remove metal impurities from the solution using an oxalate precipitation process. Material balance calculations for this process, based on solubility data in pure nitric acid, predict approximately 80 percent of the plutonium in the solution will be lost to waste. Due to the uncertainty associated with the plutonium losses during processing, solubility experiments were performed to measure the recovery of plutonium during pretreatment and a subsequent precipitationmore » process to prepare a slurry feed for a batch melter. A good estimate of the plutonium content of the glass is required for planning the shipment of the vitrified Am/Cm product to Oak Ridge National Laboratory (ORNL).The plutonium solubility in the oxalate precipitation supernate during pretreatment was 10 mg/mL at 35 degrees C. In two subsequent washes with a 0.25M oxalic acid/0.5M nitric acid solution, the solubility dropped to less than 5 mg/mL. During the precipitation and washing steps, lanthanide fission products in the solution were mostly insoluble. Uranium, and alkali, alkaline earth, and transition metal impurities were soluble as expected. An elemental material balance for plutonium showed that greater than 94 percent of the plutonium was recovered in the dissolved precipitate. The recovery of the lanthanide elements was generally 94 percent or higher except for the more soluble lanthanum. The recovery of soluble metal impurities from the precipitate slurry ranged from 15 to 22 percent. Theoretically, 16 percent of the soluble oxalates should have been present in the dissolved slurry based on the dilution effects and volumes of supernate and wash solutions removed. A trace level material balance showed greater than 97 percent recovery of americium-241 (from the beta dec ay of plutonium-241) in the dissolved precipitate, a value consistent with the recovery of europium, the americium surrogate.In a subsequent experiment, the plutonium solubility following an oxalate precipitation to simulate the preparation of a slurry feed for a batch melter was 21 mg/mL at 35 degrees C. The increase in solubility compared to the value measured during the pretreatment experiment was attributed to the increased nitrate concentration and ensuing increase in plutonium complexation. The solubility of the plutonium following a precipitant wash with 0.1M oxalic acid was unchanged. The recovery of plutonium from the precipitate slurry was greater than 97 percent allowing an estimation that approximately 92 percent of the plutonium in Tank 17.1 will report to the glass. The behavior of the lanthanides and soluble metal impurities was consistent with the behavior seen during the pretreatment experiment. A trace level material balance showed that 99.9 percent of the americium w as recovered from the precipitate slurry. The overall recovery of americium from the pretreatment and feed preparation processes was greater than 97 percent, which was consistent with the measured recovery of the europium surrogate.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pool, Karl N.; Minette, Michael J.; Wahl, Jon H.

On September 28, 2015, debris collected from the PRF (236-Z) canyon floor, Pan J, was observed to exhibit chemical reaction. The material had been transferred from the floor pan to a collection tray inside the canyon the previous Friday. Work in the canyon was stopped to allow Industrial Hygiene to perform monitoring of the material reaction. Canyon floor debris that had been sealed out was sequestered at the facility, a recovery plan was developed, and drum inspections were initiated to verify no additional reactions had occurred. On October 13, in-process drums containing other Pan J material were inspected and showedmore » some indication of chemical reaction, limited to discoloration and degradation of inner plastic bags. All Pan J material was sealed back into the canyon and returned to collection trays. Based on the high airborne levels in the canyon during physical debris removal, ETGS (Encapsulation Technology Glycerin Solution) was used as a fogging/lock-down agent. On October 15, subject matter experts confirmed a reaction had occurred between nitrates (both Plutonium Nitrate and Aluminum Nitrate Nonahydrate (ANN) are present) in the Pan J material and the ETGS fixative used to lower airborne radioactivity levels during debris removal. Management stopped the use of fogging/lock-down agents containing glycerin on bulk materials, declared a Management Concern, and initiated the Potential Inadequacy in the Safety Analysis determination process. Additional drum inspections and laboratory analysis of both reacted and unreacted material are planned. This report compiles the results of many different sample analyses conducted by the Pacific Northwest National Laboratory on samples collected from the Plutonium Reclamation Facility (PRF) floor pans by the CH2MHill’s Plateau Remediation Company (CHPRC). Revision 1 added Appendix G that reports the results of the Gas Generation Rate and methodology. The scope of analyses requested by CHPRC includes the determination of common anions, gamma spectrometry, metals, corrosivity, organics and alpha spectrometry (note: alpha spectrometry was cancelled during the performance of this work with concurrence from CHPRC). Results may help elucidate the components that led to the unexpected reaction in the canyon as well as inform the radiological and hazardous characteristics. The specific anions, gamma emitters, organics and metals requested by CHPRC are provided in the analytical reports sections. The individual analyses were conducted under the Plutonium Finishing Plant (PFP) Floor Pan Evaluation Project Quality Assurance Project Plan (PFP Floor Pan Evaluation QAPP, Revision 0.) developed by PNNL specifically for this project. The final reports for each analysis set are included in this compilation of the results. Each package was reviewed under the PFP Floor Pan Evaluation Project Quality Assurance Project Plan so no additional reviews were conducted in this compilation task. The Gas Generation Rates in Appendix G were conducted under the PNNL “How Do I…” quality assurance program and were NOT conducted under the Plutonium Finishing Plant (PFP) Floor Pan Evaluation Project Quality Assurance Project Plan (PFP Floor Pan Evaluation QAPP, Revision 0.).« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dagle, G.E.; Weller, R.E.; Watson, C.R.

The life-span biological effects of inhaled soluble, alpha-emitting radionuclides deposited in the skeleton and liver were studied in 5 groups of 20 beagles exposed to initial lung depositions ranging from 0.48 to 518 Bq/g of lung. Average plutonium amounts in the lungs decreased to approximately 1% of the final body deposition in dogs surviving 5 years or more; more than 90% of the final depositions accumulated in the liver and skeleton. The liver-to-skeletal ratio of deposited plutonium was 0.83. The incidence of bone tumors, primarily osteogenic sarcomas causing early mortality, at final group average skeletal depositions of 15.8, 2.1, andmore » 0.5 Bq/g was, respectively, 85%, 50%, and 5%; there were no bone tumors in exposure groups with mean average depositions lower than 0.5 Bq/g. Elevated serum liver enzyme levels were observed in exposure groups down to 1.3 Bq/g. The incidence of liver tumors at final group average liver depositions of 6.9, 1.3, 0.2, and 0.1 Bq/g, was, respectively, 25%, 15%, 15%, and 15%; one hepatoma occurred among 40 control dogs. The risk of the liver cancer produced by inhaled plutonium nitrate was difficult to assess due to the competing risks of life shortening from lung and bone tumors.« less

The efficacies of pure LICAM(C) and DTPA on the retention of plutonium-238 and americium-241 in rats after their inhalation as nitrate and intravenous injection as citrate.

PubMed

Stradling, G N; Stather, J W; Gray, S A; Moody, J C; Ellender, M; Hodgson, A; Volf, V; Taylor, D M; Wirth, P; Gaskin, P W

1989-10-01

The pure carboxylated catechoyl amide LICAM(C) and the calcium and zinc salts of diethylenetriaminepenta-acetic acid (DTPA), were tested for efficacy for removing 238Pu and 241Am from rats after inhalation of the nitrate or intravenous injection of the citrate. The results were compared with the efficacy of methylated LICAM(C) used in previous experiments. It was shown that: (1) after inhalation of 238Pu nitrate, DTPA was far superior to pure LICAM(C); (2) after intravenous injection of 238Pu citrate, the infusion of DTPA plus LICAM(C) was only marginally more effective than DTPA alone; and (3) after inhalation or intravenous injection of 238Pu plus 241Am, the efficacy of pure LICAM(C) was only marginally more effective than the methylated form and neither form was effective for the decorporation of 241Am. It was concluded that DTPA, at present, remains the chelating agent of choice for treating persons accidentally contaminated with transportable forms of Pu and Am.

SEPARATION OF INORGANIC SALTS FROM ORGANIC SOLUTIONS

DOEpatents

Katzin, L.I.; Sullivan, J.C.

1958-06-24

A process is described for recovering the nitrates of uranium and plutonium from solution in oxygen-containing organic solvents such as ketones or ethers. The solution of such salts dissolved in an oxygen-containing organic compound is contacted with an ion exchange resin whereby sorption of the entire salt on the resin takes place and then the salt-depleted liquid and the resin are separated from each other. The reaction seems to be based on an anion formation of the entire salt by complexing with the anion of the resin. Strong base or quaternary ammonium type resins can be used successfully in this process.

Plutonium Extraction by the Formation of Insoluble Salts; EXTRACTION DU PLUTONIUM PAR FORMATION DE SELS INSOLUBLES

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ganivet, M.

1960-06-29

The aim of this work is to convert Pu IV nitrate in solution into an insoluble salt. Three methods have been studied: 1) the conventional oxalic acid method was improved; 2) precipitation with 8-hydroxyquinoline was tried; 3) the hydrogen peroxide method was adapted to the eluates of the ionic resins from Marcoule. The yield from the oxalic process has been increased (loss of Pu in the mother-liquor brought from 200 mg/l to 20 mg/l). The study of Pu IV precipitation by 8-hydroxyquinoline has shown that the yield is excellent (Pu concentration in the mother-liquor less than 5 mg/h), but decontaminationmore » from impurities is nil. Finally, experiments on the precipitation by hydrogen peroxide of Pu IV solutions at the concentrations normally obtained from the anionic resins at Marcoule have given us good yields (Pu concentration in the mother-liquor less than 7 mg/l), and the purification is better than that obtained by oxalic acid (1000 ppm total impurities after a precipitation). (author)« less

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

HB-LINE ANION EXCHANGE PURIFICATION OF AFS-2 PLUTONIUM FOR MOX

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kyser, E. A.; King, W. D.

2012-07-31

Non-radioactive cerium (Ce) and radioactive plutonium (Pu) anion exchange column experiments using scaled HB-Line designs were performed to investigate the feasibility of using either gadolinium nitrate (Gd) or boric acid (B as H{sub 3}BO{sub 3}) as a neutron poison in the H-Canyon dissolution process. Expected typical concentrations of probable impurities were tested and the removal of these impurities by a decontamination wash was measured. Impurity concentrations are compared to two specifications - designated as Column A or Column B (most restrictive) - proposed for plutonium oxide (PuO{sub 2}) product shipped to the Mixed Oxide (MOX) Fuel Fabrication Facility (MFFF). Usemore » of Gd as a neutron poison requires a larger volume of wash for the proposed Column A specification. Since boron (B) has a higher proposed specification and is more easily removed by washing, it appears to be the better candidate for use in the H-Canyon dissolution process. Some difficulty was observed in achieving the Column A specification due to the limited effectiveness that the wash step has in removing the residual B after ~4 BV's wash. However a combination of the experimental 10 BV's wash results and a calculated DF from the oxalate precipitation process yields an overall DF sufficient to meet the Column A specification. For those impurities (other than B) not removed by 10 BV's of wash, the impurity is either not expected to be present in the feedstock or process, or recommendations have been provided for improvement in the analytical detection/method or validation of calculated results. In summary, boron is recommended as the appropriate neutron poison for H-Canyon dissolution and impurities are expected to meet the Column A specification limits for oxide production in HB-Line.« less

HB-LINE ANION EXCHANGE PURIFICATION OF AFS-2 PLUTONIUM FOR MOX

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kyser, E.; King, W.

2012-04-25

Non-radioactive cerium (Ce) and radioactive plutonium (Pu) anion exchange column experiments using scaled HB-Line designs were performed to investigate the feasibility of using either gadolinium nitrate (Gd) or boric acid (B as H{sub 3}BO{sub 3}) as a neutron poison in the H-Canyon dissolution process. Expected typical concentrations of probable impurities were tested and the removal of these impurities by a decontamination wash was measured. Impurity concentrations are compared to two specifications - designated as Column A or Column B (most restrictive) - proposed for plutonium oxide (PuO{sub 2}) product shipped to the Mixed Oxide (MOX) Fuel Fabrication Facility (MFFF). Usemore » of Gd as a neutron poison requires a larger volume of wash for the proposed Column A specification. Since boron (B) has a higher proposed specification and is more easily removed by washing, it appears to be the better candidate for use in the H-Canyon dissolution process. Some difficulty was observed in achieving the Column A specification due to the limited effectiveness that the wash step has in removing the residual B after {approx}4 BV's wash. However a combination of the experimental 10 BV's wash results and a calculated DF from the oxalate precipitation process yields an overall DF sufficient to meet the Column A specification. For those impurities (other than B) not removed by 10 BV's of wash, the impurity is either not expected to be present in the feedstock or process, or recommendations have been provided for improvement in the analytical detection/method or validation of calculated results. In summary, boron is recommended as the appropriate neutron poison for H-Canyon dissolution and impurities are expected to meet the Column A specification limits for oxide production in HB-Line.« less

RECONDITIONING FUEL ELEMENTS

DOEpatents

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)

Use of boiled hexamethylenetetramine and urea to increase the porosity of cerium dioxide microspheres formed in the internal gelation process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hunt, R. D.; Collins, J. L.; Cowell, B. S.

Cerium dioxide (CeO 2) is a commonly used simulant for plutonium dioxide and for plutonium (Pu) in a mixed uranium (U) and Pu oxide [(U, Pu)O 2] in nuclear fuel development. This effort developed CeO 2 microspheres with different porosities and diameters for use in a crush-strength study. The internal gelation technique has produced CeO 2 microspheres with limited initial porosity. When an equal molar solution of urea and hexamethylenetetramine (HMTA) is gently boiling for 1 hr and used in the gelation process, the crystallite size and porosity of mixed U and thorium oxide microspheres and the (U, Pu)O 2more » microspheres increased significantly. In this study with cerium, the combination of ammonium cerium nitrate and 1-h boiled HMTA-urea failed to produce a stable feed broth. However, when the 1-h heated HMTA-urea was combined with unheated HMTA-urea in 1 to 3 volume ratio or the boiling time of the HMTA-urea was reduced to 15-20 min, a stable solution of HMTA, urea, and Ce was formed at 273 K. This new Ce solution produced CeO 2 microspheres with much higher initial porosities. Intermediate porosities were possible when the heated HMTA/urea was aged prior to use.« less

Use of boiled hexamethylenetetramine and urea to increase the porosity of cerium dioxide microspheres formed in the internal gelation process

DOE PAGES

Hunt, R. D.; Collins, J. L.; Cowell, B. S.

2017-05-13

Cerium dioxide (CeO 2) is a commonly used simulant for plutonium dioxide and for plutonium (Pu) in a mixed uranium (U) and Pu oxide [(U, Pu)O 2] in nuclear fuel development. This effort developed CeO 2 microspheres with different porosities and diameters for use in a crush-strength study. The internal gelation technique has produced CeO 2 microspheres with limited initial porosity. When an equal molar solution of urea and hexamethylenetetramine (HMTA) is gently boiling for 1 hr and used in the gelation process, the crystallite size and porosity of mixed U and thorium oxide microspheres and the (U, Pu)O 2more » microspheres increased significantly. In this study with cerium, the combination of ammonium cerium nitrate and 1-h boiled HMTA-urea failed to produce a stable feed broth. However, when the 1-h heated HMTA-urea was combined with unheated HMTA-urea in 1 to 3 volume ratio or the boiling time of the HMTA-urea was reduced to 15-20 min, a stable solution of HMTA, urea, and Ce was formed at 273 K. This new Ce solution produced CeO 2 microspheres with much higher initial porosities. Intermediate porosities were possible when the heated HMTA/urea was aged prior to use.« less

CONVERSION OF PLUTONIUM TRIFLUORIDE TO PLUTONIUM TETRAFLUORIDE

DOEpatents

Fried, S.; Davidson, N.R.

1957-09-10

A large proportion of the trifluoride of plutonium can be converted, in the absence of hydrogen fluoride, to the tetrafiuoride of plutonium. This is done by heating plutonium trifluoride with oxygen at temperatures between 250 and 900 deg C. The trifiuoride of plutonium reacts with oxygen to form plutonium tetrafluoride and plutonium oxide, in a ratio of about 3 to 1. In the presence of moisture, plutonium tetrafluoride tends to hydrolyze at elevated temperatures and therefore it is desirable to have the process take place under anhydrous conditions.

The nitrate to ammonia and ceramic (NAC) process for the denitration and immobilization of low-level radioactive liquid waste (LLW)

NASA Astrophysics Data System (ADS)

Muguercia, Ivan

Hazardous radioactive liquid waste is the legacy of more than 50 years of plutonium production associated with the United States' nuclear weapons program. It is estimated that more than 245,000 tons of nitrate wastes are stored at facilities such as the single-shell tanks (SST) at the Hanford Site in the state of Washington, and the Melton Valley storage tanks at Oak Ridge National Laboratory (ORNL) in Tennessee. In order to develop an innovative, new technology for the destruction and immobilization of nitrate-based radioactive liquid waste, the United State Department of Energy (DOE) initiated the research project which resulted in the technology known as the Nitrate to Ammonia and Ceramic (NAC) process. However, inasmuch as the nitrate anion is highly mobile and difficult to immobilize, especially in relatively porous cement-based grout which has been used to date as a method for the immobilization of liquid waste, it presents a major obstacle to environmental clean-up initiatives. Thus, in an effort to contribute to the existing body of knowledge and enhance the efficacy of the NAC process, this research involved the experimental measurement of the rheological and heat transfer behaviors of the NAC product slurry and the determination of the optimal operating parameters for the continuous NAC chemical reaction process. Test results indicate that the NAC product slurry exhibits a typical non-Newtonian flow behavior. Correlation equations for the slurry's rheological properties and heat transfer rate in a pipe flow have been developed; these should prove valuable in the design of a full-scale NAC processing plant. The 20-percent slurry exhibited a typical dilatant (shear thickening) behavior and was in the turbulent flow regime due to its lower viscosity. The 40-percent slurry exhibited a typical pseudoplastic (shear thinning) behavior and remained in the laminar flow regime throughout its experimental range. The reactions were found to be more efficient in the lower temperature range investigated. With respect to leachability, the experimental final NAC ceramic waste form is comparable to the final product of vitrification, the technology chosen by DOE to treat these wastes. As the NAC process has the potential of reducing the volume of nitrate-based radioactive liquid waste by as much as 70 percent, it not only promises to enhance environmental remediation efforts but also effect substantial cost savings.

Pyrochemical process for extracting plutonium from an electrolyte salt

DOEpatents

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

DOEpatents

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.

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-CERIUM-COBALT AND PLUTONIUM-CERIUM-NICKEL ALLOYS

DOEpatents

Coffinberry, A.S.

1959-08-25

>New plutonium-base teroary alloys useful as liquid reactor fuels are described. The alloys consist of 10 to 20 atomic percent cobalt with the remainder plutonium and cerium in any desired proportion, with the plutonium not in excess of 88 atomic percent; or, of from 10 to 25 atomic percent nickel (or mixture of nickel and cobalt) with the remainder plutonium and cerium in any desired proportion, with the plutonium not in excess of 86 atomic percent. The stated advantages of these alloys over unalloyed plutonium for reactor fuel use are a lower melting point and a wide range of permissible plutonium dilution.

Solvation of actinide salts in water using a polarizable continuum model.

PubMed

Kumar, Narendra; Seminario, Jorge M

2015-01-29

In order to determine how actinide atoms are dressed when solvated in water, density functional theory calculations have been carried out to study the equilibrium structure of uranium plutonium and thorium salts (UO2(2+), PuO2(2+), Pu(4+), and Th(4+)) both in vacuum as well as in solution represented by a conductor-like polarizable continuum model. This information is of paramount importance for the development of sensitive nanosensors. Both UO2(2+) and PuO2(2+) ions show coordination number of 4-5 with counterions replacing one or two water molecules from the first coordination shell. On the other hand, Pu(4+), has a coordination number of 8 both when completely solvated and also in the presence of chloride and nitrate ions with counterions replacing water molecules in the first shell. Nitrates were found to bind more strongly to Pu(IV) than chloride anions. In the case of the Th(IV) ion, the coordination number was found to be 9 or 10 in the presence of chlorides. Moreover, the Pu(IV) ion shows greater affinity for chlorides than the Th(IV) ion. Adding dispersion and ZPE corrections to the binding energy does not alter the trends in relative stability of several conformers because of error cancelations. All structures and energetics of these complexes are reported.

31. VIEW OF A WORKER HOLDING A PLUTONIUM 'BUTTON.' PLUTONIUM, ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

31. VIEW OF A WORKER HOLDING A PLUTONIUM 'BUTTON.' PLUTONIUM, A MAN-MADE SUBSTANCE, WAS RARE. SCRAPS RESULTING FROM PRODUCTION AND PLUTONIUM RECOVERED FROM RETIRED NUCLEAR WEAPONS WERE REPROCESSED INTO VALUABLE PURE-PLUTONIUM METAL (9/19/73). - Rocky Flats Plant, Bounded by Indiana Street & Routes 93, 128 & 72, Golden, Jefferson County, CO

Solvent extraction system for plutonium colloids and other oxide nano-particles

DOEpatents

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.

Effect of Americium-241 Content on Plutonium Radiation Source Terms

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rainisch, R.

1998-12-28

The management of excess plutonium by the US Department of Energy includes a number of storage and disposition alternatives. Savannah River Site (SRS) is supporting DOE with plutonium disposition efforts, including the immobilization of certain plutonium materials in a borosilicate glass matrix. Surplus plutonium inventories slated for vitrification include materials with elevated levels of Americium-241. The Am-241 content of plutonium materials generally reflects in-growth of the isotope due to decay of plutonium and is age-dependent. However, select plutonium inventories have Am-241 levels considerably above the age-based levels. Elevated levels of americium significantly impact radiation source terms of plutonium materials andmore » will make handling of the materials more difficult. Plutonium materials are normally handled in shielded glove boxes, and the work entails both extremity and whole body exposures. This paper reports results of an SRS analysis of plutonium materials source terms vs. the Americium-241 content of the materials. Data with respect to dependence and magnitude of source terms on/vs. Am-241 levels are presented and discussed. The investigation encompasses both vitrified and un-vitrified plutonium oxide (PuO2) batches.« less

Integrating the stabilization of nuclear materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dalton, H.F.

1996-05-01

In response to Recommendation 94-1 of the Defense Nuclear Facilities Safety Board, the Department of Energy committed to stabilizing specific nuclear materials within 3 and 8 years. These efforts are underway. The Department has already repackaged the plutonium at Rocky Flats and metal turnings at Savannah River that had been in contact with plastic. As this effort proceeds, we begin to look at activities beyond stabilization and prepare for the final disposition of these materials. To describe the plutonium materials being stabilize, Figure 1 illustrates the quantities of plutonium in various forms that will be stabilized. Plutonium as metal comprisesmore » 8.5 metric tons. Plutonium oxide contains 5.5 metric tons of plutonium. Plutonium residues and solutions, together, contain 7 metric tons of plutonium. Figure 2 shows the quantity of plutonium-bearing material in these four categories. In this depiction, 200 metric tons of plutonium residues and 400 metric tons of solutions containing plutonium constitute most of the material in the stabilization program. So, it is not surprising that much of the work in stabilization is directed toward the residues and solutions, even though they contain less of the plutonium.« less

A Piecewise Local Partial Least Squares (PLS) Method for the Quantitative Analysis of Plutonium Nitrate Solutions

DOE PAGES

Lascola, Robert; O'Rourke, Patrick E.; Kyser, Edward A.

2017-10-05

Here, we have developed a piecewise local (PL) partial least squares (PLS) analysis method for total plutonium measurements by absorption spectroscopy in nitric acid-based nuclear material processing streams. Instead of using a single PLS model that covers all expected solution conditions, the method selects one of several local models based on an assessment of solution absorbance, acidity, and Pu oxidation state distribution. The local models match the global model for accuracy against the calibration set, but were observed in several instances to be more robust to variations associated with measurements in the process. The improvements are attributed to the relativemore » parsimony of the local models. Not all of the sources of spectral variation are uniformly present at each part of the calibration range. Thus, the global model is locally overfitting and susceptible to increased variance when presented with new samples. A second set of models quantifies the relative concentrations of Pu(III), (IV), and (VI). Standards containing a mixture of these species were not at equilibrium due to a disproportionation reaction. Therefore, a separate principal component analysis is used to estimate of the concentrations of the individual oxidation states in these standards in the absence of independent confirmatory analysis. The PL analysis approach is generalizable to other systems where the analysis of chemically complicated systems can be aided by rational division of the overall range of solution conditions into simpler sub-regions.« less

A Piecewise Local Partial Least Squares (PLS) Method for the Quantitative Analysis of Plutonium Nitrate Solutions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lascola, Robert; O'Rourke, Patrick E.; Kyser, Edward A.

Here, we have developed a piecewise local (PL) partial least squares (PLS) analysis method for total plutonium measurements by absorption spectroscopy in nitric acid-based nuclear material processing streams. Instead of using a single PLS model that covers all expected solution conditions, the method selects one of several local models based on an assessment of solution absorbance, acidity, and Pu oxidation state distribution. The local models match the global model for accuracy against the calibration set, but were observed in several instances to be more robust to variations associated with measurements in the process. The improvements are attributed to the relativemore » parsimony of the local models. Not all of the sources of spectral variation are uniformly present at each part of the calibration range. Thus, the global model is locally overfitting and susceptible to increased variance when presented with new samples. A second set of models quantifies the relative concentrations of Pu(III), (IV), and (VI). Standards containing a mixture of these species were not at equilibrium due to a disproportionation reaction. Therefore, a separate principal component analysis is used to estimate of the concentrations of the individual oxidation states in these standards in the absence of independent confirmatory analysis. The PL analysis approach is generalizable to other systems where the analysis of chemically complicated systems can be aided by rational division of the overall range of solution conditions into simpler sub-regions.« less

Method for dissolving plutonium dioxide

DOEpatents

Tallent, Othar K.

1978-01-01

The fluoride-catalyzed, non-oxidative dissolution of plutonium dioxide in HNO.sub.3 is significantly enhanced in rate by oxidizing dissolved plutonium ions. It is believed that the oxidation of dissolved plutonium releases fluoride ions from a soluble plutonium-fluoride complex for further catalytic action.

METHOD FOR OBTAINING PLUTONIUM METAL AND ALLOYS OF PLUTONIUM FROM PLUTONIUM TRICHLORIDE

DOEpatents

Reavis, J.G.; Leary, J.A.; Maraman, W.J.

1962-11-13

A process is given for both reducing plutonium trichloride to plutonium metal using cerium as the reductant and simultaneously alloying such plutonium metal with an excess of cerium or cerium and cobalt sufficient to yield the desired nuclear reactor fuel composition. The process is conducted at a temperature from about 550 to 775 deg C, at atmospheric pressure, without the use of booster reactants, and a substantial decontamination is effected in the product alloy of any rare earths which may be associated with the source of the plutonium. (AEC)

METHOD OF SEPARATING PLUTONIUM

DOEpatents

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.

ADSORPTION-BISMUTH PHOSPHATE METHOD FOR SEPARATING PLUTONIUM

DOEpatents

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.

PLUTONIUM-HYDROGEN REACTION PRODUCT, METHOD OF PREPARING SAME AND PLUTONIUM POWDER THEREFROM

DOEpatents

Fried, S.; Baumbach, H.L.

1959-12-01

A process is described for forming plutonlum hydride powder by reacting hydrogen with massive plutonium metal at room temperature and the product obtained. The plutonium hydride powder can be converted to plutonium powder by heating to above 200 deg C.

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

Plutonium-related work and cause-specific mortality at the United States Department of Energy Hanford Site.

PubMed

Wing, Steve; Richardson, David; Wolf, Susanne; Mihlan, Gary

2004-02-01

Health effects of working with plutonium remain unclear. Plutonium workers at the United States Department of Energy (US-DOE) Hanford Site in Washington State, USA were evaluated for increased risks of cancer and non-cancer mortality. Periods of employment in jobs with routine or non-routine potential for plutonium exposure were identified for 26,389 workers hired between 1944 and 1978. Life table regression was used to examine associations of length of employment in plutonium jobs with confirmed plutonium deposition and with cause specific mortality through 1994. Incidence of confirmed internal plutonium deposition in all plutonium workers was 15.4 times greater than in other Hanford jobs. Plutonium workers had low death rates compared to other workers, particularly for cancer causes. Mortality for several causes was positively associated with length of employment in routine plutonium jobs, especially for employment at older ages. At ages 50 and above, death rates for non-external causes of death, all cancers, cancers of tissues where plutonium deposits, and lung cancer, increased 2.0 +/- 1.1%, 2.6 +/- 2.0%, 4.9 +/- 3.3%, and 7.1 +/- 3.4% (+/-SE) per year of employment in routine plutonium jobs, respectively. Workers employed in jobs with routine potential for plutonium exposure have low mortality rates compared to other Hanford workers even with adjustment for demographic, socioeconomic, and employment factors. This may be due, in part, to medical screening. Associations between duration of employment in jobs with routine potential for plutonium exposure and mortality may indicate occupational exposure effects. Copyright 2004 Wiley-Liss, Inc.

PRODUCTION OF PLUTONIUM METAL

DOEpatents

Lyon, W.L.; Moore, R.H.

1961-01-17

A process is given for producing plutonium metal by the reduction of plutonium chloride, dissolved in alkali metal chloride plus or minus aluminum chloride, with magnesium or a magnesium-aluminum alloy at between 700 and 800 deg C and separating the plutonium or plutonium-aluminum alloy formed from the salt.

PROCESS OF FORMING PLUOTONIUM SALTS FROM PLUTONIUM EXALATES

DOEpatents

Garner, C.S.

1959-02-24

A process is presented for converting plutonium oxalate to other plutonium compounds by a dry conversion method. According to the process, lower valence plutonium oxalate is heated in the presence of a vapor of a volatile non- oxygenated monobasic acid, such as HCl or HF. For example, in order to produce plutonium chloride, the pure plutonium oxalate is heated to about 700 deg C in a slow stream of hydrogen plus HCl. By the proper selection of an oxidizing or reducing atmosphere, the plutonium halide product can be obtained in either the plus 3 or plus 4 valence state.

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.

Development of Acetic Acid Removal Technology for the UREX+Process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Robert M. Counce; Jack S. Watson

2009-06-30

It is imperative that acetic acid is removed from a waste stream in the UREX+process so that nitric acid can be recycled and possible interference with downstreatm steps can be avoidec. Acetic acid arises from acetohydrozamic acid (AHA), and is used to suppress plutonium in the first step of the UREX+process. Later, it is hydrolyzed into hydroxyl amine nitrate and acetic acid. Many common separation technologies were examined, and solvent extraction was determined to be the best choice under process conditions. Solvents already used in the UREX+ process were then tested to determine if they would be sufficient for themore » removal of acetic acid. The tributyl phosphage (TBP)-dodecane diluent, used in both UREX and NPEX, was determined to be a solvent system that gave sufficient distribution coefficients for acetic acid in addition to a high separation factor from nitric acid.« less

STRIPPING PROCESS FOR PLUTONIUM

DOEpatents

Kolodney, M.

1959-10-01

A method for removing silver, nickel, cadmium, zinc, and indium coatings from plutonium objects while simultaneously rendering the plutonium object passive is described. The coated plutonium object is immersed as the anode in an electrolyte in which the plutonium is passive and the coating metal is not passive, using as a cathode a metal which does not dissolve rapidly in the electrolyte. and passing an electrical current through the electrolyte until the coating metal is removed from the plutonium body.

PLUTONIUM-CUPFERRON COMPLEX AND METHOD OF REMOVING PLUTONIUM FROM SOLUTION

DOEpatents

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.

Lithium metal reduction of plutonium oxide to produce plutonium metal

DOEpatents

Coops, Melvin S.

1992-01-01

A method is described for the chemical reduction of plutonium oxides to plutonium metal by the use of pure lithium metal. Lithium metal is used to reduce plutonium oxide to alpha plutonium metal (alpha-Pu). The lithium oxide by-product is reclaimed by sublimation and converted to the chloride salt, and after electrolysis, is removed as lithium metal. Zinc may be used as a solvent metal to improve thermodynamics of the reduction reaction at lower temperatures. Lithium metal reduction enables plutonium oxide reduction without the production of huge quantities of CaO--CaCl.sub.2 residues normally produced in conventional direct oxide reduction processes.

SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS

DOEpatents

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.

White Paper on Potential Hazards Associated with Contaminated Cheesecloth Exposed to Nitric Acid Solutions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hypes, Philip A.

This white paper addresses the potential hazards associated with waste cheesecloth that has been exposed to nitric acid solutions. This issue was highlighted by the cleanup of a 100 ml leak of aqueous nitric acid solution containing Heat Source (HS) plutonium on 21 June 2016. Nitration of cellulosic material is a well-understood process due to industrial/military applications of the resulting material. Within the Department of Energy complex, nitric acids have been used extensively, as have cellulosic wipes. If cellulosic materials are nitrated, the cellulosic material can become ignitable and in extreme cases, reactive. We have chemistry knowledge and operating experiencemore » to support the conclusion that all current wastes are safe and compliant. There are technical questions worthy of further experimental evaluation. An extent of condition evaluation has been conducted back to 2004. During this time period there have been interruptions in the authorization to use cellulosic wipes in PF-4. Limited use has been authorized since 2007 (for purposes other than spill cleanup), so our extent of condition includes the entire current span of use. Our evaluation shows that there is no indication that process spills involving high molarity nitric acid were cleaned up with cheesecloth since 2007. The materials generated in the 21 June leak will be managed in a safe manner compliant with all applicable requirements.« less

Volatile fluoride process for separating plutonium from other materials

DOEpatents

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

DOEpatents

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.

SEPARATION OF PLUTONIUM FROM LANTHANUM BY CHELATION-EXTRACTION

DOEpatents

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.

Air transport of plutonium metal: content expansion initiative for the plutonium air transportable (PAT01) packaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Caviness, Michael L; Mann, Paul T; Yoshimura, Richard H

2010-01-01

The National Nuclear Security Administration (NNSA) has submitted an application to the Nuclear Regulatory Commission (NRC) for the air shipment of plutonium metal within the Plutonium Air Transportable (PAT-1) packaging. The PAT-1 packaging is currently authorized for the air transport of plutonium oxide in solid form only. The INMM presentation will provide a limited overview of the scope of the plutonium metal initiative and provide a status of the NNSA application to the NRC.

The calculation of annual limits of intake for plutonium-239 in man using a bone model which allows for plutonium burial and recycling.

PubMed

Priest, N D; Hunt, B W

1979-05-01

Values of the annual limit of intake (ALI) for plutonium-239 in man have been calculated using committed dose equivalent limits as recommended by ICRP in Publication 26. The calculations were made using a multicompartment bone model which allows for plutonium burial and recycling in the skeleton. In one skeletal compartment, the growing surfaces of cortical bone, it is assumed that plutonium deposits are retained and are not subject to resorption or recycling. In the trabecular bone compartment plutonium is taken to be resorbed with either subsequent redeposition onto bone surfaces or retention in the bone marrow. ALIs for plutonium-239 have been calculated assuming a range of rates of bone accretion (0-32 micron yr-1), different amounts of plutonium retained in the marrow (0-60%) and a 20%, 45% or 70% deposition of plutonium in the skeleton from the blood. The calculations made using this bone model suggest that 750 Bq (20 nCi) is an appropriate ALI for the inhalation of class W and class Y plutonium compounds and that 830 kBq and 5 MBq (23 muCi and 136 muCi) are the appropriate ALIs for the ingestion of soluble and insoluble forms of plutonium respectively.

Radionuclide Basics: Plutonium

EPA Pesticide Factsheets

Plutonium (chemical symbol Pu) is a radioactive metal. Plutonium is considered a man-made element. Plutonium-239 is used to make nuclear weapons. Pu-239 and Pu-240 are byproducts of nuclear reactor operations and nuclear bomb explosions.

Plutonium inventories for stabilization and stabilized materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Williams, A.K.

1996-05-01

The objective of the breakout session was to identify characteristics of materials containing plutonium, the need to stabilize these materials for storage, and plans to accomplish the stabilization activities. All current stabilization activities are driven by the Defense Nuclear Facilities Safety Board Recommendation 94-1 (May 26, 1994) and by the recently completed Plutonium ES&H Vulnerability Assessment (DOE-EH-0415). The Implementation Plan for accomplishing stabilization of plutonium-bearing residues in response to the Recommendation and the Assessment was published by DOE on February 28, 1995. This Implementation Plan (IP) commits to stabilizing problem materials within 3 years, and stabilizing all other materials withinmore » 8 years. The IP identifies approximately 20 metric tons of plutonium requiring stabilization and/or repackaging. A further breakdown shows this material to consist of 8.5 metric tons of plutonium metal and alloys, 5.5 metric tons of plutonium as oxide, and 6 metric tons of plutonium as residues. Stabilization of the metal and oxide categories containing greater than 50 weight percent plutonium is covered by DOE Standard {open_quotes}Criteria for Safe Storage of Plutonium Metals and Oxides{close_quotes} December, 1994 (DOE-STD-3013-94). This standard establishes criteria for safe storage of stabilized plutonium metals and oxides for up to 50 years. Each of the DOE sites and contractors with large plutonium inventories has either started or is preparing to start stabilization activities to meet these criteria.« less

Search for Plutonium Salt Deposits in the Plutonium Extraction Batteries of the Marcoule Plant; RECHERCHE DE DEPOTS DE SELS DE PLUTONIUM DANS LES BATTERIES D'EXTRACTION DU PLUTONIUM DE L'USINE DE MARCOULE

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)

SEPARATION OF PLUTONIUM HYDROXIDE FROM BISMUTH HYDROXIDE

DOEpatents

Watt, G.W.

1958-08-19

An tmproved method is described for separating plutonium hydroxide from bismuth hydroxide. The end product of the bismuth phosphate processes for the separation amd concentration of plutonium is a inixture of bismuth hydroxide amd plutonium hydroxide. It has been found that these compounds can be advantageously separated by treatment with a reducing agent having a potential sufficient to reduce bismuth hydroxide to metalltc bisinuth but not sufficient to reduce the plutonium present. The resulting mixture of metallic bismuth and plutonium hydroxide can then be separated by treatment with a material which will dissolve plutonium hydroxide but not metallic bismuth. Sodiunn stannite is mentioned as a preferred reducing agent, and dilute nitric acid may be used as the separatory solvent.

An MS-DOS-based program for analyzing plutonium gamma-ray spectra

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ruhter, W.D.; Buckley, W.M.

1989-09-07

A plutonium gamma-ray analysis system that operates on MS-DOS-based computers has been developed for the International Atomic Energy Agency (IAEA) to perform in-field analysis of plutonium gamma-ray spectra for plutonium isotopics. The program titled IAEAPU consists of three separate applications: a data-transfer application for transferring spectral data from a CICERO multichannel analyzer to a binary data file, a data-analysis application to analyze plutonium gamma-ray spectra, for plutonium isotopic ratios and weight percents of total plutonium, and a data-quality assurance application to check spectral data for proper data-acquisition setup and performance. Volume 3 contains the software listings for these applications.

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

PROCESS FOR SEPARATING PLUTONIUM FROM IMPURITIES

DOEpatents

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.

PRODUCTION OF PLUTONIUM FLUORIDE FROM BISMUTH PHOSPHATE PRECIPITATE CONTAINING PLUTONIUM VALUES

DOEpatents

Brown, H.S.; Bohlmann, E.G.

1961-05-01

A process is given for separating plutonium from fission products present on a bismuth phosphate carrier. The dried carrier is first treated with hydrogen fluoride at between 500 and 600 deg C whereby some fission product fluorides volatilize away from plutonium tetrafluoride, and nonvolatile fission product fluorides are formed then with anhydrous fluorine at between 400 and 500 deg C. Bismuth and plutonium distill in the form of volatile fluorides away from the nonvolatile fission product fluorides. The bismuth and plutonium fluorides are condensed at below 290 deg C.

PLUTONIUM COMPOUNDS AND PROCESS FOR THEIR PREPARATION

DOEpatents

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.

MCNP5 CALCULATIONS REPLICATING ARH-600 NITRATE DATA

DOE Office of Scientific and Technical Information (OSTI.GOV)

FINFROCK SH

This report serves to extend the previous document: 'MCNP Calculations Replicating ARH-600 Data' by replicating the nitrate curves found in ARH-600. This report includes the MCNP models used, the calculated critical dimension for each analyzed parameter set, and the resulting data libraries for use with the CritView code. As with the ARH-600 data, this report is not meant to replace the analysis of the fissile systems by qualified criticality personnel. The M CNP data is presented without accounting for the statistical uncertainty (although this is typically less than 0.001) or bias and, as such, the application of a reasonable safetymore » margin is required. The data that follows pertains to the uranyl nitrate and plutonium nitrate spheres, infinite cylinders, and infinite slabs of varying isotopic composition, reflector thickness, and molarity. Each of the cases was modeled in MCNP (version 5.1.40), using the ENDF/B-VI cross section set. Given a molarity, isotopic composition, and reflector thickness, the fissile concentration and diameter (or thicknesses in the case of the slab geometries) were varied. The diameter for which k-effective equals 1.00 for a given concentration could then be calculated and graphed. These graphs are included in this report. The pages that follow describe the regions modeled, formulas for calculating the various parameters, a list of cross-sections used in the calculations, a description of the automation routine and data, and finally the data output. The data of most interest are the critical dimensions of the various systems analyzed. This is presented graphically, and in table format, in Appendix B. Appendix C provides a text listing of the same data in a format that is compatible with the CritView code. Appendices D and E provide listing of example Template files and MCNP input files (these are discussed further in Section 4). Appendix F is a complete listing of all of the output data (i.e., all of the analyzed dimensions and the resulting k{sub eff} values).« less

Plutonium isotopic signatures in soils and their variation (2011-2014) in sediment transiting a coastal river in the Fukushima Prefecture, Japan.

PubMed

Jaegler, Hugo; Pointurier, Fabien; Onda, Yuichi; Hubert, Amélie; Laceby, J Patrick; Cirella, Maëva; Evrard, Olivier

2018-05-04

The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident resulted in a significant release of radionuclides that were deposited on soils in Northeastern Japan. Plutonium was detected at trace levels in soils and sediments collected around the FDNPP. However, little is known regarding the spatial-temporal variation of plutonium in sediment transiting rivers in the region. In this study, plutonium isotopic compositions were first measured in soils (n = 5) in order to investigate the initial plutonium deposition. Then, plutonium isotopic compositions were measured on flood sediment deposits (n = 12) collected after major typhoon events in 2011, 2013 and 2014. After a thorough radiochemical purification, isotopic ratios ( 240 Pu/ 239 Pu, 241 Pu/ 239 Pu and 242 Pu/ 239 Pu) were measured with a Multi-Collector Inductively Coupled Mass Spectrometer (MC ICP-MS), providing discrimination between plutonium derived from global fallout, from atmospheric nuclear weapon tests, and plutonium derived from the FDNPP accident. Results demonstrate that soils with the most Fukushima-derived plutonium were in the main radiocaesium plume and that there was a variable mixture of plutonium sources in the flood sediment samples. Plutonium concentrations and isotopic ratios generally decreased between 2011 and 2014, reflecting the progressive erosion and transport of contaminated sediment in this coastal river during flood events. Exceptions to this general trend were attributed to the occurrence of decontamination works or the remobilisation of contaminated material during typhoons. The different plutonium concentrations and isotopic ratios obtained on three aliquots of a single sample suggest that the Fukushima-derived plutonium was likely borne by discrete plutonium-containing particles. In the future, these particles should be isolated and further characterized in order to better understand the fate of this long-lived radionuclide in the environment. Copyright © 2018 Elsevier Ltd. All rights reserved.

Locating trace plutonium in contaminated soil using micro-XRF imaging

DOE PAGES

Worley, Christopher G.; Spencer, Khalil J.; Boukhalfa, Hakim; ...

2014-06-01

Micro-X-ray fluorescence (MXRF) was used to locate minute quantities of plutonium in contaminated soil. Because the specimen had previously been prepared for analysis by scanning electron microscopy, it was coated with gold to eliminate electron beam charging. However, this significantly hindered efforts to detect plutonium by MXRF. The gold L peak series present in all spectra increased background counts. Plutonium signal attenuation by the gold coating and severe peak overlap from potassium in the soil prevented detection of trace plutonium using the Pu Mα peak. However, the 14.3 keV Pu Lα peak sensitivity was not optimal due to poor transmissionmore » efficiency through the source polycapillary optic, and the instrument silicon drift detector sensitivity quickly declines for peaks with energies above ~10 keV. Instrumental parameters were optimized (eg. using appropriate source filters) in order to detect plutonium. An X-ray beam aperture was initially used to image a majority of the specimen with low spatial resolution. A small region that appeared to contain plutonium was then imaged at high spatial resolution using a polycapillary optic. Small areas containing plutonium were observed on a soil particle, and iron was co-located with the plutonium. Zinc and titanium also appeared to be correlated with the plutonium, and these elemental correlations provided useful plutonium chemical state information that helped to better understand its environmental transport properties.« less

Stabilizing stored PuO2 with addition of metal impurities

NASA Astrophysics Data System (ADS)

Moten, Shafaq; Huda, Muhammad

Plutonium oxides is of widespread significance due its application in nuclear fuels, space missions, as well as the long-termed storage of plutonium from spent fuel and nuclear weapons. The processes to refine and store plutonium bring many other elements in contact with the plutonium metal and thereby affect the chemistry of the plutonium. Pure plutonium metal corrodes to an oxide in air with the most stable form of this oxide is stoichiometric plutonium dioxide, PuO2. Defects such as impurities and vacancies can form in the plutonium dioxide before, during and after the refining processes as well as during storage. An impurity defect manifests itself at the bottom of the conduction band and affects the band gap of the unit cell. Studying the interaction between transition metals and plutonium dioxide is critical for better, more efficient storage plans as well as gaining insights to provide a better response to potential threats of exposure to the environment. Our study explores the interaction of a few metals within the plutonium dioxide structure which have a likelihood of being exposed to the plutonium dioxide powder. Using Density Functional Theory, we calculated a substituted metal impurity in PuO2 supercell. We repeated the calculations with an additional oxygen vacancy. Our results reveal interesting volume contraction of PuO2 supercell when one plutonium atom is substituted with a metal atom. The authors acknowledge the Texas Computing Center (TACC) at The University of Texas at Austin and High Performance Computing (HPC) at The University of Texas at Arlington.

PROCESSES FOR SEPARATING AND RECOVERING CONSTITUENTS OF NEUTRON IRRADIATED URANIUM

DOEpatents

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.

METHOD FOR RECOVERING PLUTONIUM VALUES FROM SOLUTION USING A BISMUTH HYDROXIDE CARRIER PRECIPITATE

DOEpatents

Faris, B.F.

1961-04-25

Carrier precipitation processes for separating plutonium values from aqueous solutions are described. In accordance with the invention a bismuth hydroxide precipitate is formed in the plutonium-containing solution, thereby carrying plutonium values from the solution.

Increased retention of americium in kidneys as compared with plutonium in an actinide wound contamination model in the rat.

PubMed

Griffiths, Nina M; Coudert, Sylvie; Molina, Thibaut; Wilk, Jean-Claude; Renault, Daniel; Berard, Philippe; Van der Meeren, Anne

2014-11-01

Americium-241 ((241)Am) presents a potential risk for nuclear industry workers associated with reactor decommissioning and aging combustible materials. The purpose of this study was to investigate Am renal retention after actinide contamination by wounding in the rat. Anesthetized rats were contaminated with Mixed Oxide (MOX) (7.1% Plutonium [Pu] by mass and containing 27% Am as % total alpha activity), Pu or Am nitrate following an incision wound of the hind leg. Times of euthanasia ranged from 2 hours to 5 months after contamination. Pu and Am levels were quantified following radiochemistry and alpha-spectrophotometry. Initial data show that over the experimental period the proportion of Am in kidneys as a fraction of total kidney alpha activity was elevated as compared to MOX powder indicating a specific retention in this organ. The percentage of Pu was similar to the powder. After MOX contamination, kidney to liver ratios appeared to increase more markedly for Am (from 0.2 at 7 days to 0.6 at 90 days) as compared with Pu (0.1 at 7 days to 0.2 at 90 days). In accordance with tissue actinide retention the dose from Am to the kidney increases with time. For comparison, the ratio of estimated equivalent doses due to Am to kidney is 1.5-fold greater than for Pu (around 90 versus 60 mSv). After actinide contamination of wounds, Am is concentrated in the kidneys as compared to Pu leading to potential exposure of renal tissue to both alpha particles and gamma radiation.

METHOD OF MAKING PLUTONIUM DIOXIDE

DOEpatents

Garner, C.S.

1959-01-13

A process is presented For converting both trivalent and tetravalent plutonium oxalate to substantially pure plutonium dioxide. The plutonium oxalate is carefully dried in the temperature range of 130 to300DEC by raising the temperature gnadually throughout this range. The temperature is then raised to 600 C in the period of about 0.3 of an hour and held at this level for about the same length of time to obtain the plutonium dioxide.

METHOD OF PRODUCING PLUTONIUM TETRAFLUORIDE

DOEpatents

Tolley, W.B.; Smith, R.C.

1959-12-15

A process is presented for preparing plutonium tetrafluoride from plutonium(IV) oxalate. The oxalate is dried and decomposed at about 300 deg C to the dioxide, mixed with ammonium bifluoride, and the mixture is heated to between 50 and 150 deg C whereby ammonium plutonium fluoride is formed. The ammonium plutonium fluoride is then heated to about 300 deg C for volatilization of ammonium fluoride. Both heating steps are preferably carried out in an inert atmosphere.

Lymph node clearance of plutonium from subcutaneous wounds in beagles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dagle, G.E.

1973-08-01

The lymph node clearance of /sup 239/Pu O/sub 2/ administered as insoluble particles from subcutaneous implants was studied in adult beagles to simulate accidental contamination of hand wounds. External scintillation data were collected from the popliteal lymph nodes of each dog after 9.2 to 39.4 mu Ci of plutonium oxide was subcutaneously implanted into the left or right hind paws. The left hind paw was armputated 4 weeks after implantation to prevent continued deposition of plutonium oxide particles in the left popliteal lymph node. Groups of 3 dogs were sacrificed 4, 8, 16, and 32 weeks after plutonium implantation formore » histopathologic, electron microscopic, and radiochemical analysis of regional lymph nodes. An additional group of dogs received treatment with the chelating agent diethyenetriaminepentaacetic acid (DTPA). Plutonium rapidly accumulated in the popliteal lymph nodes after subcutaneous injection into the hind paw, and 1 to 10% of the implant dose was present in the popliteal lymph nodes at the time of necropsy. Histopathologic changes in the popliteal lymph nodes with plutonium particles were characterized primarily by reticular cell hyperplasia, increased numbers of macrophages, necrosis, and fibroplasia. Eventually, the plutonium particles became sequestered by scar tissue that often replaced the entire architecture of the lymph node. Light microscopic autoradiographs of the popliteal lymph nodes showed a time-related increase in number of alpha tracks per plutonium source. Electron microscopy showed that the plutonium particles were aggregated in phagolysosomes of macrophages. There was slight clearance of plutonium from the popliteal lymph nodes of dogs monitored for 32 weeks. The clearance of plutonium particles from the popliteal lymph nodes was associated with necrosis of macrophages. The external iliac lymph nodes contained fewer plutonium particles than the popliteal lymph nodes and histopathologic changes were less severe. The superficial inguinal lymph nodes of one dog contained appreciable amounts of plutonium. Treatment with diethylenetriaminepentaacetic acid (DTPA) did not have a measurable effect on the clearance of plutonium from the popliteal lymph nodes. (60 references) (auth)« less

Plutonium in the arctic marine environment--a short review.

PubMed

Skipperud, Lindis

2004-06-18

Anthropogenic plutonium has been introduced into the environment over the past 50 years as the result of the detonation of nuclear weapons and operational releases from the nuclear industry. In the Arctic environment, the main source of plutonium is from atmospheric weapons testing, which has resulted in a relatively uniform, underlying global distribution of plutonium. Previous studies of plutonium in the Kara Sea have shown that, at certain sites, other releases have given rise to enhanced local concentrations. Since different plutonium sources are characterised by distinctive plutonium-isotope ratios, evidence of a localised influence can be supported by clear perturbations in the plutonium-isotope ratio fingerprints as compared to the known ratio in global fallout. In Kara Sea sites, such perturbations have been observed as a result of underwater weapons tests at Chernaya Bay, dumped radioactive waste in Novaya Zemlya, and terrestrial runoff from the Ob and Yenisey Rivers. Measurement of the plutonium-isotope ratios offers both a means of identifying the origin of radionuclide contamination and the influence of the various nuclear installations on inputs to the Arctic, as well as a potential method for following the movement of water and sediment loads in the rivers.

Tabulated Neutron Emission Rates for Plutonium Oxide

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shores, Erik Frederick

This work tabulates neutron emission rates for 80 plutonium oxide samples as reported in the literature. Plutonium-­238 and plutonium-­239 oxides are included and such emission rates are useful for scaling tallies from Monte Carlo simulations and estimating dose rates for health physics applications.

PROCESS OF SEPARATING PLUTONIUM FROM URANIUM

DOEpatents

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

DOEpatents

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.

PROCESS USING BISMUTH PHOSPHATE AS A CARRIER PRECIPITATE FOR FISSION PRODUCTS AND PLUTONIUM VALUES

DOEpatents

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.

PROCESS FOR THE SEPARATION OF HEAVY METALS

DOEpatents

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.

DISSOLUTION OF LANTHANUM FLUORIDE PRECIPITATES

DOEpatents

Fries, B.A.

1959-11-10

A plutonium separatory ore concentration procedure involving the use of a fluoride type of carrier is presented. An improvement is given in the derivation step in the process for plutonium recovery by carrier precipitation of plutonium values from solution with a lanthanum fluoride carrier precipitate and subsequent derivation from the resulting plutonium bearing carrier precipitate of an aqueous acidic plutonium-containing solution. The carrier precipitate is contacted with a concentrated aqueous solution of potassium carbonate to effect dissolution therein of at least a part of the precipitate, including the plutonium values. Any remaining precipitate is separated from the resulting solution and dissolves in an aqueous solution containing at least 20% by weight of potassium carbonate. The reacting solutions are combined, and an alkali metal hydroxide added to a concentration of at least 2N to precipitate lanthanum hydroxide concomitantly carrying plutonium values.

IDAHO CHEMICAL PROCESSING PLANT TECHNICAL PROGRESS REPORT FOR APRIL THROUGH JUNE 1958

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stevenson, C.E.

1958-11-01

Processing of uranium -aluminum alloy was continued with slight process modifications. Means for recovering rare gases from dissolver off-gas are described. Results of extensive decontamination procedures required to enable entrance to the continuous dissolver cell are also indicated. Pilot plant studies of dissolving aluminum continuously showed that rates of dissolution were decreased by factors of 2 to 4 as the concentration of nitric acid fed was increased from 5.4 to 11N. The rate of aluminum dissolution was found to be proportional to initial area exposed for pieces of different shape. It was found possible to produce a highly basic aluminummore » nitrate solution at a reasonable rate by dissolving to low concentration in dilute acid, followed by evaporation to the desired level. Uranium exchange rate measurements for the TBP extraction process are described. A canned rotor pump under test with graphite bearings operated 6000 hours with nominal wear. Difficulties were experienced in testing a nutating disc pump. Measurements of the potential of zirconium in hydrofluoric acid as a function of pH confirmed the predicted equation. In teflon vessels, zirconium dissolves a little more rapidly in nitric-hydrofluoric acid mixtures than in glass vessels, presumably due to reaction of fluoride with silica. Titunium alloy Types 55A and 75A were found to resist corrosion by certain boiling nitric-hydrochloric acid mixtures. Initial tests have commenced with a NaK-heated 100 liter/hour pilot plant aluminum nitrate calciner to continue process demonstration. In tests in the smaller pilot plant unit, increasing feed spray air ratio was found to increase particle loading in the cyclone effluent. Laboratory studies indicated that a venturi scrubber using dilute nitric acid at 80 C should remove ruthenium effectively from calciner off-gas. In a pilot plant test in which a significant fraction of ruthenium feed was retained by the alumina, substantial absorption of volatilized ruthenium was obtained. Thermal conductivity of alumina near 3000 F was about 0.26 Btu/hr)(ft)( F). In leaching studies, very little strontium or plutonium was removed by water from alumina calcined at 550 C. Dilute nitric acid, however, extracted strontium from this material to the same degree (~ 50 percent) as from material calcined at 400 C. Concentrated basic aluminum nitrate was produced from simulated aluminum nitrate waste by slow hydrolysis with urea followed by evaporation. Aluminum was efficiently extracted from buffered aluminum nitrate solution by acetylacetone and was stripped back into nitric acid. A filterable aluminum phosphate was precipituted from aluminum nitrate solution by urea hydrolysis; the phosphate effectively carried fission products, however. Spectrophotometric methods were developed for macro and micro quantities of uranium, in the presence of high concentrations of other ions, based on tetrapropylammonium nitrate extraction. (For preceding period see ID0-14443.) (auth)« less

NON-AQUEOUS DISSOLUTION OF MASSIVE PLUTONIUM

DOEpatents

Reavis, J.G.; Leary, J.A.; Walsh, K.A.

1959-05-12

A method is presented for obtaining non-aqueous solutions or plutonium from massive forms of the metal. In the present invention massive plutonium is added to a salt melt consisting of 10 to 40 weight per cent of sodium chloride and the balance zinc chloride. The plutonium reacts at about 800 deg C with the zinc chloride to form a salt bath of plutonium trichloride, sodium chloride, and metallic zinc. The zinc is separated from the salt melt by forcing the molten mixture through a Pyrex filter.

OXIDATIVE METHOD OF SEPARATING PLUTONIUM FROM NEPTUNIUM

DOEpatents

Beaufait, L.J. Jr.

1958-06-10

A method is described of separating neptunium from plutonium in an aqueous solution containing neptunium and plutonium in valence states not greater than +4. This may be accomplished by contacting the solution with dichromate ions, thus oxidizing the neptunium to a valence state greater than +4 without oxidizing any substantial amount of plutonium, and then forming a carrier precipitate which carries the plutonium from solution, leaving the neptunium behind. A preferred embodiment of this invention covers the use of lanthanum fluoride as the carrier precipitate.

PROCESS OF ELIMINATING HYDROGEN PEROXIDE IN SOLUTIONS CONTAINING PLUTONIUM VALUES

DOEpatents

Barrick, J.G.; Fries, B.A.

1960-09-27

A procedure is given for peroxide precipitation processes for separating and recovering plutonium values contained in an aqueous solution. When plutonium peroxide is precipitated from an aqueous solution, the supernatant contains appreciable quantities of plutonium and peroxide. It is desirable to process this solution further to recover plutonium contained therein, but the presence of the peroxide introduces difficulties; residual hydrogen peroxide contained in the supernatant solution is eliminated by adding a nitrite or a sulfite to this solution.

23. AERIAL VIEW LOOKING SOUTHEAST AT THE PLUTONIUM OPERATION BUILDINGS ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

23. AERIAL VIEW LOOKING SOUTHEAST AT THE PLUTONIUM OPERATION BUILDINGS 771, 776/777, AND 707. BUILDING 771, IN THE FOREGROUND, WAS BUILT IN 1952 TO HOUSE ALL PLUTONIUM OPERATIONS. BY 1956, BUILDING 771 WAS NO LONGER ADEQUATE FOR PRODUCTION DEMANDS. BUILDING 776/777, TO THE SOUTH OF BUILDING 771, WAS CONSTRUCTED TO HOUSE PLUTONIUM FABRICATION AND FOUNDRY OPERATIONS. PLUTONIUM RECOVERY REMAINED IN BUILDING 771. BY 1967, CONSTRUCTION ON BUILDING 707, TO THE SOUTH OF BUILDING 776/777, BEGAN AS PRODUCTION LEVELS CONTINUED TO EXPAND NECESSITATING THE NEED FOR ADDITIONAL PLUTONIUM FABRICATION SPACE (7/1/69). - Rocky Flats Plant, Bounded by Indiana Street & Routes 93, 128 & 72, Golden, Jefferson County, CO

PROCESS FOR SEPARATING PLUTONIUM BY REPEATED PRECIPITATION WITH AMPHOTERIC HYDROXIDE CARRIERS

DOEpatents

Faris, B.F.

1960-04-01

A multiple carrier precipitation method is described for separating and recovering plutonium from an aqueous solution. The hydroxide of an amphoteric metal is precipitated in an aqueous plutonium-containing solution. This precipitate, which carries plutonium, is then separated from the supernatant liquid and dissolved in an aqueous hydroxide solution, forming a second plutonium- containing solution. lons of an amphoteric metal which forms an insoluble hydroxide under the conditions existing in this second solution are added to the second solution. The precipitate which forms and which carries plutonium is separated from the supernatant liquid. Amphoteric metals which may be employed are aluminum, bibmuth, copper, cobalt, iron, lanthanum, nickel, and zirconium.

PROCESS FOR SEPARATION OF HEAVY METALS

DOEpatents

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.

PROCESS FOR THE RECOVERY OF PLUTONIUM

DOEpatents

Ritter, D.M.

1959-01-13

An improvement is presented in the process for recovery and decontamination of plutonium. The carrier precipitate containing plutonium is dissolved and treated with an oxidizing agent to place the plutonium in a hexavalent oxidation state. A lanthanum fluoride precipitate is then formed in and removed from the solution to carry undesired fission products. The fluoride ions in the reniaining solution are complexed by addition of a borate sueh as boric acid, sodium metaborate or the like. The plutonium is then reduced and carried from the solution by the formation of a bismuth phosphate precipitate. This process effects a better separation from unwanted flssion products along with conccntration of the plutonium by using a smaller amount of carrier.

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

PRECIPITATION OF PLUTONOUS PEROXIDE

DOEpatents

Barrick, J.G.; Manion, J.P.

1961-08-15

A precipitation process for recovering plutonium values contained in an aqueous solution is described. In the process for precipitating plutonium as plutonous peroxide, hydroxylamine or hydrazine is added to the plutoniumcontaining solution prior to the addition of peroxide to precipitate plutonium. The addition of hydroxylamine or hydrazine increases the amount of plutonium precipitated as plutonous peroxide. (AEC)

PROCESS USING POTASSIUM LANTHANUM SULFATE FOR FORMING A CARRIER PRECIPITATE FOR PLUTONIUM VALUES

DOEpatents

Angerman, A.A.

1958-10-21

A process is presented for recovering plutonium values in an oxidation state not greater than +4 from fluoride-soluble fission products. The process consists of adding to an aqueous acidic solution of such plutonium values a crystalline potassium lanthanum sulfate precipitate which carries the plutonium values from the solution.

PLUTONIUM-THORIUM ALLOYS

DOEpatents

Schonfeld, F.W.

1959-09-15

New plutonium-base binary alloys useful as liquid reactor fuel are described. The alloys consist of 50 to 98 at.% thorium with the remainder plutonium. The stated advantages of these alloys over unalloyed plutonium for reactor fuel use are easy fabrication, phase stability, and the accompanying advantuge of providing a means for converting Th/sup 232/ into U/sup 233/.

The Fireball integrated code package

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dobranich, D.; Powers, D.A.; Harper, F.T.

1997-07-01

Many deep-space satellites contain a plutonium heat source. An explosion, during launch, of a rocket carrying such a satellite offers the potential for the release of some of the plutonium. The fireball following such an explosion exposes any released plutonium to a high-temperature chemically-reactive environment. Vaporization, condensation, and agglomeration processes can alter the distribution of plutonium-bearing particles. The Fireball code package simulates the integrated response of the physical and chemical processes occurring in a fireball and the effect these processes have on the plutonium-bearing particle distribution. This integrated treatment of multiple phenomena represents a significant improvement in the state ofmore » the art for fireball simulations. Preliminary simulations of launch-second scenarios indicate: (1) most plutonium vaporization occurs within the first second of the fireball; (2) large non-aerosol-sized particles contribute very little to plutonium vapor production; (3) vaporization and both homogeneous and heterogeneous condensation occur simultaneously; (4) homogeneous condensation transports plutonium down to the smallest-particle sizes; (5) heterogeneous condensation precludes homogeneous condensation if sufficient condensation sites are available; and (6) agglomeration produces larger-sized particles but slows rapidly as the fireball grows.« less

Experimental and Numerical Investigations on Colloid-facilitated Plutonium Reactive Transport in Fractured Tuffaceous Rocks

NASA Astrophysics Data System (ADS)

Dai, Z.; Wolfsberg, A. V.; Zhu, L.; Reimus, P. W.

2017-12-01

Colloids have the potential to enhance mobility of strongly sorbing radionuclide contaminants in fractured rocks at underground nuclear test sites. This study presents an experimental and numerical investigation of colloid-facilitated plutonium reactive transport in fractured porous media for identifying plutonium sorption/filtration processes. The transport parameters for dispersion, diffusion, sorption, and filtration are estimated with inverse modeling for minimizing the least squares objective function of multicomponent concentration data from multiple transport experiments with the Shuffled Complex Evolution Metropolis (SCEM). Capitalizing on an unplanned experimental artifact that led to colloid formation and migration, we adopt a stepwise strategy to first interpret the data from each experiment separately and then to incorporate multiple experiments simultaneously to identify a suite of plutonium-colloid transport processes. Nonequilibrium or kinetic attachment and detachment of plutonium-colloid in fractures was clearly demonstrated and captured in the inverted modeling parameters along with estimates of the source plutonium fraction that formed plutonium-colloids. The results from this study provide valuable insights for understanding the transport mechanisms and environmental impacts of plutonium in fractured formations and groundwater aquifers.

Isotope ratio analysis of individual sub-micrometer plutonium particles with inductively coupled plasma mass spectrometry.

PubMed

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.

Plutonium recovery from spent reactor fuel by uranium displacement

DOEpatents

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.

Variations in the concentration of plutonium, strontium-90 and total alpha-emitters in human teeth collected within the British Isles.

PubMed

O'Donnell, R G; Mitchell, P I; Priest, N D; Strange, L; Fox, A; Henshaw, D L; Long, S C

1997-08-18

Concentrations of plutonium-239, plutonium-240, strontium-90 and total alpha-emitters have been measured in children's teeth collected throughout Great Britain and Ireland. The concentrations of plutonium and strontium-90 were measured in batched samples, each containing approximately 50 teeth, using low-background radiochemical methods. The concentrations of total alpha-emitters were determined in single teeth using alpha-sensitive plastic track detectors. The results showed that the average concentrations of total alpha-emitters and strontium-90 were approximately one to three orders of magnitude greater than the equivalent concentrations of plutonium-239,240. Regression analyses indicated that the concentrations of plutonium, but not strontium-90 or total alpha-emitters, decreased with increasing distance from the Sellafield nuclear fuel reprocessing plant-suggesting that this plant is a source of plutonium contamination in the wider population of the British Isles. Nevertheless, the measured absolute concentrations of plutonium (mean = 5 +/- 4 mBq kg-1 ash wt.) were so low that they are considered to present an insignificant radiological hazard.

Plutonium from Above-Ground Nuclear Tests in Milk Teeth: Investigation of Placental Transfer in Children Born between 1951 and 1995 in Switzerland

PubMed Central

Froidevaux, Pascal; Haldimann, Max

2008-01-01

Background Occupational risks, the present nuclear threat, and the potential danger associated with nuclear power have raised concerns regarding the metabolism of plutonium in pregnant women. Objective We measured plutonium levels in the milk teeth of children born between 1951 and 1995 to assess the potential risk that plutonium incorporated by pregnant women might pose to the radiosensitive tissues of the fetus through placenta transfer. Methods We used milk teeth, whose enamel is formed during pregnancy, to investigate the transfer of plutonium from the mother’s blood plasma to the fetus. We measured plutonium using sensitive sector field inductively coupled plasma mass spectrometry techniques. We compared our results with those of a previous study on strontium-90 (90Sr) released into the atmosphere after nuclear bomb tests. Results Results show that plutonium activity peaks in the milk teeth of children born about 10 years before the highest recorded levels of plutonium fallout. By contrast, 90Sr, which is known to cross the placenta barrier, manifests differently in milk teeth, in accordance with 90Sr fallout deposition as a function of time. Conclusions These findings demonstrate that plutonium found in milk teeth is caused by fallout that was inhaled around the time the milk teeth were shed and not from any accumulation during pregnancy through placenta transfer. Thus, plutonium may not represent a radiologic risk for the radiosensitive tissues of the fetus. PMID:19079728

REMOVAL OF LEGACY PLUTONIUM MATERIALS FROM SWEDEN

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dunn, Kerry A.; Bellamy, J. Steve; Chandler, Greg T.

2013-08-18

U.S. Department of Energy’s National Nuclear Security Administration (NNSA) Office of Global Threat Reduction (GTRI) recently removed legacy plutonium materials from Sweden in collaboration with AB SVAFO, Sweden. This paper details the activities undertaken through the U.S. receiving site (Savannah River Site (SRS)) to support the characterization, stabilization, packaging and removal of legacy plutonium materials from Sweden in 2012. This effort was undertaken as part of GTRI’s Gap Materials Program and culminated with the successful removal of plutonium from Sweden as announced at the 2012 Nuclear Security Summit. The removal and shipment of plutonium materials to the United States wasmore » the first of its kind under NNSA’s Global Threat Reduction Initiative. The Environmental Assessment for the U.S. receipt of gap plutonium material was approved in May 2010. Since then, the multi-year process yielded many first time accomplishments associated with plutonium packaging and transport activities including the application of the of DOE-STD-3013 stabilization requirements to treat plutonium materials outside the U.S., the development of an acceptance criteria for receipt of plutonium from a foreign country, the development and application of a versatile process flow sheet for the packaging of legacy plutonium materials, the identification of a plutonium container configuration, the first international certificate validation of the 9975 shipping package and the first intercontinental shipment using the 9975 shipping package. This paper will detail the technical considerations in developing the packaging process flow sheet, defining the key elements of the flow sheet and its implementation, determining the criteria used in the selection of the transport package, developing the technical basis for the package certificate amendment and the reviews with multiple licensing authorities and most importantly integrating the technical activities with the Swedish partners.« less

Excess Weapons Plutonium Immobilization in Russia

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jardine, L.; Borisov, G.B.

2000-04-15

The joint goal of the Russian work is to establish a full-scale plutonium immobilization facility at a Russian industrial site by 2005. To achieve this requires that the necessary engineering and technical basis be developed in these Russian projects and the needed Russian approvals be obtained to conduct industrial-scale immobilization of plutonium-containing materials at a Russian industrial site by the 2005 date. This meeting and future work will provide the basis for joint decisions. Supporting R&D projects are being carried out at Russian Institutes that directly support the technical needs of Russian industrial sites to immobilize plutonium-containing materials. Special R&Dmore » on plutonium materials is also being carried out to support excess weapons disposition in Russia and the US, including nonproliferation studies of plutonium recovery from immobilization forms and accelerated radiation damage studies of the US-specified plutonium ceramic for immobilizing plutonium. This intriguing and extraordinary cooperation on certain aspects of the weapons plutonium problem is now progressing well and much work with plutonium has been completed in the past two years. Because much excellent and unique scientific and engineering technical work has now been completed in Russia in many aspects of plutonium immobilization, this meeting in St. Petersburg was both timely and necessary to summarize, review, and discuss these efforts among those who performed the actual work. The results of this meeting will help the US and Russia jointly define the future direction of the Russian plutonium immobilization program, and make it an even stronger and more integrated Russian program. The two objectives for the meeting were to: (1) Bring together the Russian organizations, experts, and managers performing the work into one place for four days to review and discuss their work with each other; and (2) Publish a meeting summary and a proceedings to compile reports of all the excellent Russian plutonium immobilization contract work. This proceedings document presents the wide extent of Russian immobilization activities, provides a reference for their work, and makes it available to others.« less

PLUTONIUM AND ITS METALLURGY. A STAGE IN ITS DEVELOPMENT: THE INTERNATIONAL CONFERENCE ON THE METALLURGY OF PLUTONIUM (GRENOBLE, APRIL 1960) (in French)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grison, E.

1961-01-01

A discussion is given on physical properties of plutonium, allotropic variations; kinetics of transformation; electrica; and magnetic properties; and electronic structure of the external layers of the atom. Plutonium can be used only as nuclear fuel; it is very expensive and toxic. (auth)

Siegfried S. Hecker, Plutonium, and Nonproliferation

Science.gov Websites

controversy involving the stability of certain structures (or phases) in plutonium alloys near equilibrium Cold War is Over. What Now?, DOE Technical Report, April, 1995 6th US-Russian Pu Science Workshop * Aging of Plutonium and Its Alloys * A Tale of Two Diagrams * Plutonium and Its Alloys-From Atoms to

SEPARATION OF PLUTONIUM FROM FISSION PRODUCTS BY A COLLOID REMOVAL PROCESS

DOEpatents

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.

PLUTONIUM RECOVERY FROM NEUTRON-BOMBARDED URANIUM FUEL

DOEpatents

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)

SEPARATION OF RUTHENIUM FROM AQUEOUS SOLUTIONS

DOEpatents

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.

Pyrochemical recovery of plutonium from calcium fluoride reduction slag

DOEpatents

Christensen, D.C.

A pyrochemical method of recovering finely dispersed plutonium metal from calcium fluoride reduction slag is claimed. The plutonium-bearing slag is crushed and melted in the presence of at least an equimolar amount of calcium chloride and a few percent metallic calcium. The calcium chloride reduces the melting point and thereby decreases the viscosity of the molten mixture. The calcium reduces any oxidized plutonium in the mixture and also causes the dispersed plutonium metal to coalesce and settle out as a separate metallic phase at the bottom of the reaction vessel. Upon cooling the mixture to room temperature, the solid plutonium can be cleanly separated from the overlying solid slag, with an average recovery yield on the order of 96 percent.

QUANTITATIVE PLUTONIUM MICRODISTRIBUTION IN BONE TISSUE OF VERTEBRA FROM A MAYAK WORKER

PubMed Central

Lyovkina, Yekaterina V.; Miller, Scott C.; Romanov, Sergey A.; Krahenbuhl, Melinda P.; Belosokhov, Maxim V.

2010-01-01

The purpose was to obtain quantitative data on plutonium microdistribution in different structural elements of human bone tissue for local dose assessment and dosimetric models validation. A sample of the thoracic vertebra was obtained from a former Mayak worker with a rather high plutonium burden. Additional information was obtained on occupational and exposure history, medical history, and measured plutonium content in organs. Plutonium was detected in bone sections from its fission tracks in polycarbonate film using neutron-induced autoradiography. Quantitative analysis of randomly selected microscopic fields on one of the autoradiographs was performed. Data included fission fragment tracks in different bone tissue and surface areas. Quantitative information on plutonium microdistribution in human bone tissue was obtained for the first time. From these data, quantitative relationship of plutonium decays in bone volume to decays on bone surface in cortical and trabecular fractions were defined as 2.0 and 0.4, correspondingly. The measured quantitative relationship of decays in bone volume to decays on bone surface does not coincide with recommended models for the cortical bone fraction by the International Commission on Radiological Protection. Biokinetic model parameters of extrapulmonary compartments might need to be adjusted after expansion of the data set on quantitative plutonium microdistribution in other bone types in human as well as other cases with different exposure patterns and types of plutonium. PMID:20838087

Analysis on Reactor Criticality Condition and Fuel Conversion Capability Based on Different Loaded Plutonium Composition in FBR Core

NASA Astrophysics Data System (ADS)

Permana, Sidik; Saputra, Geby; Suzuki, Mitsutoshi; Saito, Masaki

2017-01-01

Reactor criticality condition and fuel conversion capability are depending on the fuel arrangement schemes, reactor core geometry and fuel burnup process as well as the effect of different fuel cycle and fuel composition. Criticality condition of reactor core and breeding ratio capability have been investigated in this present study based on fast breeder reactor (FBR) type for different loaded fuel compositions of plutonium in the fuel core regions. Loaded fuel of Plutonium compositions are based on spent nuclear fuel (SNF) of light water reactor (LWR) for different fuel burnup process and cooling time conditions of the reactors. Obtained results show that different initial fuels of plutonium gives a significant chance in criticality conditions and fuel conversion capability. Loaded plutonium based on higher burnup process gives a reduction value of criticality condition or less excess reactivity. It also obtains more fuel breeding ratio capability or more breeding gain. Some loaded plutonium based on longer cooling time of LWR gives less excess reactivity and in the same time, it gives higher breeding ratio capability of the reactors. More composition of even mass plutonium isotopes gives more absorption neutron which affects to decresing criticality or less excess reactivity in the core. Similar condition that more absorption neutron by fertile material or even mass plutonium will produce more fissile material or odd mass plutonium isotopes to increase the breeding gain of the reactor.

PLUTONIUM-ZIRCONIUM ALLOYS

DOEpatents

Schonfeld, F.W.; Waber, J.T.

1960-08-30

A series of nuclear reactor fuel alloys consisting of from about 5 to about 50 at.% zirconium (or higher zirconium alloys such as Zircaloy), balance plutonium, and having the structural composition of a plutonium are described. Zirconium is a satisfactory diluent because it alloys readily with plutonium and has desirable nuclear properties. Additional advantages are corrosion resistance, excellent fabrication propenties, an isotropie structure, and initial softness.

Plutonium recovery from spent reactor fuel by uranium displacement

DOEpatents

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.

Characterization studies and indicated remediation methods for plutonium contaminated soils at the Nevada Test Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Murarik, T.M.; Wenstrand, T.K.; Rogers, L.A.

An initial soil characterization study was conducted to help identify possible remediation methods to remove plutonium from the Nevada Test Site and Tonapah Test Range surface soils. Results from soil samples collected across various isopleths at five sites indicate that the size-fraction distribution patterns of plutonium remain similar to findings from the Nevada Applied Ecology Group (NAEG) (1970's). The plutonium remains in the upper 10--15 cm of soils, as indicated in previous studies. Distribution of fine particles downwind'' of ground zero at each site is suggested. Whether this pattern was established immediately after each explosion or this resulted from post-shotmore » wind movement of deposited material is unclear. Several possible soil treatment scenarios are presented. Removal of plutonium from certain size fractions of the soils would alleviate the sites of much of the plutonium burden. However, the nature of association of plutonium with soil components will determine which remediation methods will most likely succeed.« less

Characterization studies and indicated remediation methods for plutonium contaminated soils at the Nevada Test Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Murarik, T.M.; Wenstrand, T.K.; Rogers, L.A.

An initial soil characterization study was conducted to help identify possible remediation methods to remove plutonium from the Nevada Test Site and Tonapah Test Range surface soils. Results from soil samples collected across various isopleths at five sites indicate that the size-fraction distribution patterns of plutonium remain similar to findings from the Nevada Applied Ecology Group (NAEG) (1970`s). The plutonium remains in the upper 10--15 cm of soils, as indicated in previous studies. Distribution of fine particles ``downwind`` of ground zero at each site is suggested. Whether this pattern was established immediately after each explosion or this resulted from post-shotmore » wind movement of deposited material is unclear. Several possible soil treatment scenarios are presented. Removal of plutonium from certain size fractions of the soils would alleviate the sites of much of the plutonium burden. However, the nature of association of plutonium with soil components will determine which remediation methods will most likely succeed.« less

Developing a physiologically based approach for modeling plutonium decorporation therapy with DTPA.

PubMed

Kastl, Manuel; Giussani, Augusto; Blanchardon, Eric; Breustedt, Bastian; Fritsch, Paul; Hoeschen, Christoph; Lopez, Maria Antonia

2014-11-01

To develop a physiologically based compartmental approach for modeling plutonium decorporation therapy with the chelating agent Diethylenetriaminepentaacetic acid (Ca-DTPA/Zn-DTPA). Model calculations were performed using the software package SAAM II (©The Epsilon Group, Charlottesville, Virginia, USA). The Luciani/Polig compartmental model with age-dependent description of the bone recycling processes was used for the biokinetics of plutonium. The Luciani/Polig model was slightly modified in order to account for the speciation of plutonium in blood and for the different affinities for DTPA of the present chemical species. The introduction of two separate blood compartments, describing low-molecular-weight complexes of plutonium (Pu-LW) and transferrin-bound plutonium (Pu-Tf), respectively, and one additional compartment describing plutonium in the interstitial fluids was performed successfully. The next step of the work is the modeling of the chelation process, coupling the physiologically modified structure with the biokinetic model for DTPA. RESULTS of animal studies performed under controlled conditions will enable to better understand the principles of the involved mechanisms.

URANIUM RECOVERY PROCESS

DOEpatents

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.

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

BASIC PEROXIDE PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINANTS

DOEpatents

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.

PREPARATION OF PLUTONIUM

DOEpatents

Kolodney, M.

1959-07-01

Methods are presented for the electro-deposition of plutonium from fused mixtures of plutonium halides and halides of the alkali metals and alkaline earth metals. Th salts, preferably chlorides and with the plutonium prefer ably in the trivalent state, are placed in a refractory crucible such as tantalum or molybdenam and heated in a non-oxidizing atmosphere to 600 to 850 deg C, the higher temperatatures being used to obtain massive plutonium and the lower for the powder form. Electrodes of graphite or non reactive refractory metals are used, the crucible serving the cathode in one apparatus described in the patent.

30. VIEW OF A GLOVEBOX LINE USED IN PLUTONIUM OPERATIONS. ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

30. VIEW OF A GLOVEBOX LINE USED IN PLUTONIUM OPERATIONS. SAFETY AND HEALTH CONCERNS WERE OF MAJOR IMPORTANCE AT THE PLANT, BECAUSE OF THE RADIOACTIVE NATURE OF THE MATERIALS USED. PLUTONIUM GIVES OFF ALPHA AND BETA PARTICLES, GAMMA PROTONS, NEUTRONS, AND IS ALSO PYROPHORIC. AS A RESULT, PLUTONIUM OPERATIONS ARE PERFORMED UNDER CONTROLLED CONDITIONS THAT INCLUDE CONTAINMENT, FILTERING, SHIELDING, AND CREATING AN INERT ATMOSPHERE. PLUTONIUM WAS HANDLED WITHIN GLOVEBOXES THAT WERE INTERCONNECTED AND RAN SEVERAL HUNDRED FEET IN LENGTH (5/5/70). - Rocky Flats Plant, Bounded by Indiana Street & Routes 93, 128 & 72, Golden, Jefferson County, CO

Rapid Method for Sodium Hydroxide/Sodium Peroxide Fusion ...

EPA Pesticide Factsheets

Technical Fact Sheet Analysis Purpose: Qualitative analysis Technique: Alpha spectrometry Method Developed for: Plutonium-238 and plutonium-239 in water and air filters Method Selected for: SAM lists this method as a pre-treatment technique supporting analysis of refractory radioisotopic forms of plutonium in drinking water and air filters using the following qualitative techniques: • Rapid methods for acid or fusion digestion • Rapid Radiochemical Method for Plutonium-238 and Plutonium 239/240 in Building Materials for Environmental Remediation Following Radiological Incidents. Summary of subject analytical method which will be posted to the SAM website to allow access to the method.

US Department of Energy Plutonium Stabilization and Immobilization Workshop, December 12-14, 1995: Final proceedings

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

1996-05-01

The purpose of the workshop was to foster communication within the technical community on issues surrounding stabilization and immobilization of the Department`s surplus plutonium and plutonium- contaminated wastes. The workshop`s objectives were to: build a common understanding of the performance, economics and maturity of stabilization and immobilization technologies; provide a system perspective on stabilization and immobilization technology options; and address the technical issues associated with technologies for stabilization and immobilization of surplus plutonium and plutonium- contaminated waste. The papers presented during this workshop have been indexed separately.

PROCESS OF REMOVING PLUTONIUM VALUES FROM SOLUTION WITH GROUP IVB METAL PHOSPHO-SILICATE COMPOSITIONS

DOEpatents

Russell, E.R.; Adamson, A.W.; Schubert, J.; Boyd, G.E.

1957-10-29

A process for separating plutonium values from aqueous solutions which contain the plutonium in minute concentrations is described. These values can be removed from an aqueous solution by taking an aqueous solution containing a salt of zirconium, titanium, hafnium or thorium, adding an aqueous solution of silicate and phosphoric acid anions to the metal salt solution, and separating, washing and drying the precipitate which forms when the two solutions are mixed. The aqueous plutonium containing solution is then acidified and passed over the above described precipi-tate causing the plutonium values to be adsorbed by the precipitate.

Plutonium controversy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Richmond, C.R.

1980-01-01

The toxicity of plutonium is discussed, particularly in relation to controversies surrounding the setting of radiation protection standards. The sources, amounts of, and exposure pathways of plutonium are given and the public risk estimated. (ACR)

PREPARATION OF PLUTONIUM TRIFLUORIDE

DOEpatents

Burger, L.L.; Roake, W.E.

1961-07-11

A process of producing plutonium trifluoride by reacting dry plutonium(IV) oxalate with chlorofluorinated methane or ethane at 400 to 450 deg C and cooling the product in the absence of oxygen is described.

MCNP Parametric Studies of Plutonium Metal and Various Interstitial Moderating Materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Glazener, Natasha; Kamm, Ryan James

2017-03-31

Nuclear Criticality Safety (NCS) has performed calculations evaluating the effect of different interstitial materials on 5.0-kg of plutonium metal. As with all non-fissionable interstitials, the results here illustrate that it requires significant quantities of oil to be intimately mixed with plutonium, reflected by a thick layer of full-density water, to achieve the same reactivity as that of solid plutonium metal.

Hydrologic conditions at the Idaho National Engineering Laboratory, 1982 to 1985

USGS Publications Warehouse

Pittman, J.R.; Fischer, P.R.; Jensen, R.G.

1988-01-01

Aqueous chemical and radioactive wastes discharged since 1952 to unlined ponds and wells at the INEL (Idaho National Engineering Laboratory) have affected water quality in perched groundwater zones and in the Snake River Plain Aquifer. Routine waste water disposal was changed from deep injection wells to ponds at the ICPP (Idaho Chemical Processing Plant) in 1984. During 1982-85, tritium concentrations increased in perched groundwater zones under disposal ponds, but cobalt-60 concentrations decreased. In 1985, perched groundwater under TRA disposal ponds contained up to 1,770 +or-30 pCi/mL (picocuries/milliliter) of tritium and 0.36+or-0.05 pCi/mL of cobalt-60. During 1982-85, tritium concentrations in water in the Snake River Plain aquifer decreased as much as 80 pCi/mL near the ICPP. In 1985, measurable tritium concentrations ranged from 0.9+or-0.3 to 93.4 +or-2.0 pCi/mL. Tritium was detected in groundwater near the southern boundary of the INEL, 9 miles south of the ICPP and TRA. Strontium-90 concentrations in groundwater, up to 63 +or-5 pCi/L (picocuries per liter) near the ICPP, generally were smaller than 1981 concentrations. Cesium-137 concentrations in groundwater near the ICPP ranged from 125 +or-14 to 237 +or-45 pCi/L. Maximum concentrations of plutonium-238 and plutonium-239 , -240 (undivided) were 1.31 +or-.0019 pCi/ml and 1.9 +or-0.00003 pCi/L. Sodium and chloride generally decreased during 1982-85. Nitrate concentrations increased near the TRA and NRF (Naval Reactors Facility) and decreased near the ICPP. (USGS)

SEPARATION OF PLUTONIUM IONS FROM SOLUTION BY ADSORPTION ON ZIRCONIUM PYROPHOSPHATE

DOEpatents

Stoughton, R.W.

1961-01-31

A method is given for separating plutonium in its reduced, phosphate- insoluble state from other substances. It involves contacting a solution containing the plutonium with granular zirconium pyrophosphate.

Tank 241-AZ-101 criticality assessment resulting from pump jet mixing: Sludge mixing simulation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Onishi, Y.; Recknagle, K.

Tank 241-AZ-101 (AZ-101) is one of 28 double-shell tanks located in the AZ farm in the Hanford Site`s 200 East Area. The tank contains a significant quantity of fissile materials, including an estimated 9.782 kg of plutonium. Before beginning jet pump mixing for mitigative purposes, the operations must be evaluated to demonstrate that they will be subcritical under both normal and credible abnormal conditions. The main objective of this study was to address a concern about whether two 300-hp pumps with four rotating 18.3-m/s (60-ft/s) jets can concentrate plutonium in their pump housings during mixer pump operation and cause amore » criticality. The three-dimensional simulation was performed with the time-varying TEMPEST code to determine how much the pump jet mixing of Tank AZ-101 will concentrate plutonium in the pump housing. The AZ-101 model predicted that the total amount of plutonium within the pump housing peaks at 75 g at 10 simulation seconds and decreases to less than 10 g at four minutes. The plutonium concentration in the entire pump housing peaks at 0.60 g/L at 10 simulation seconds and is reduced to below 0.1 g/L after four minutes. Since the minimum critical concentration of plutonium is 2.6 g/L, and the minimum critical plutonium mass under idealized plutonium-water conditions is 520 g, these predicted maximums in the pump housing are much lower than the minimum plutonium conditions needed to reach a criticality level. The initial plutonium maximum of 1.88 g/L still results in safety factor of 4.3 in the pump housing during the pump jet mixing operation.« less

Plutonium and americium separation from salts

DOEpatents

Hagan, Paul G.; Miner, Frend J.

1976-01-01

Salts or materials containing plutonium and americium are dissolved in hydrochloric acid, heated, and contacted with an alkali metal carbonate solution to precipitate plutonium and americium carbonates which are thereafter readily separable from the solution.

Plutonium storage criteria

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chung, D.; Ascanio, X.

1996-05-01

The Department of Energy has issued a technical standard for long-term (>50 years) storage and will soon issue a criteria document for interim (<20 years) storage of plutonium materials. The long-term technical standard, {open_quotes}Criteria for Safe Storage of Plutonium Metals and Oxides,{close_quotes} addresses the requirements for storing metals and oxides with greater than 50 wt % plutonium. It calls for a standardized package that meets both off-site transportation requirements, as well as remote handling requirements from future storage facilities. The interim criteria document, {open_quotes}Criteria for Interim Safe Storage of Plutonium-Bearing Solid Materials{close_quotes}, addresses requirements for storing materials with less thanmore » 50 wt% plutonium. The interim criteria document assumes the materials will be stored on existing sites, and existing facilities and equipment will be used for repackaging to improve the margin of safety.« less

PROCESS OF PRODUCING SHAPED PLUTONIUM

DOEpatents

Anicetti, R.J.

1959-08-11

A process is presented for producing and casting high purity plutonium metal in one step from plutonium tetrafluoride. The process comprises heating a mixture of the plutonium tetrafluoride with calcium while the mixture is in contact with and defined as to shape by a material obtained by firing a mixture consisting of calcium oxide and from 2 to 10% by its weight of calcium fluoride at from 1260 to 1370 deg C.

WET METHOD OF PREPARING PLUTONIUM TRIBROMIDE

DOEpatents

Davidson, N.R.; Hyde, E.K.

1958-11-11

S> The preparation of anhydrous plutonium tribromide from an aqueous acid solution of plutonium tetrabromide is described, consisting of adding a water-soluble volatile bromide to the tetrabromide to provide additional bromide ions sufficient to furnish an oxidation-reduction potential substantially more positive than --0.966 volt, evaporating the resultant plutonium tribromides to dryness in the presence of HBr, and dehydrating at an elevated temperature also in the presence of HBr.

Spectrophotometers for plutonium monitoring in HB-line

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lascola, R. J.; O'Rourke, P. E.; Kyser, E. A.

2016-02-12

This report describes the equipment, control software, calibrations for total plutonium and plutonium oxidation state, and qualification studies for the instrument. It also provides a detailed description of the uncertainty analysis, which includes source terms associated with plutonium calibration standards, instrument drift, and inter-instrument variability. Also included are work instructions for instrument, flow cell, and optical fiber setup, work instructions for routine maintenance, and drawings and schematic diagrams.

Plutonium radiation surrogate

DOEpatents

Frank, Michael I [Dublin, CA

2010-02-02

A self-contained source of gamma-ray and neutron radiation suitable for use as a radiation surrogate for weapons-grade plutonium is described. The source generates a radiation spectrum similar to that of weapons-grade plutonium at 5% energy resolution between 59 and 2614 keV, but contains no special nuclear material and emits little .alpha.-particle radiation. The weapons-grade plutonium radiation surrogate also emits neutrons having fluxes commensurate with the gamma-radiation intensities employed.

PLUTONIUM ALLOYS CONTAINING CONTROLLED AMOUNTS OF PLUTONIUM ALLOTROPES OBTAINED BY APPLICATION OF HIGH PRESSURES

DOEpatents

Elliott, R.O.; Gschneidner, K.A. Jr.

1962-07-10

A method of making stabilized plutonium alloys which are free of voids and cracks and have a controlled amount of plutonium allotropes is described. The steps include adding at least 4.5 at.% of hafnium, indium, or erbium to the melted plutonium metal, homogenizing the resulting alloy at a temperature of 450 deg C, cooling to room temperature, and subjecting the alloy to a pressure which produces a rapid increase in density with a negligible increase in pressure. The pressure required to cause this rapid change in density or transformation ranges from about 800 to 2400 atmospheres, and is dependent on the alloying element. (AEC)

PROCESS OF SECURING PLUTONIUM IN NITRIC ACID SOLUTIONS IN ITS TRIVALENT OXIDATION STATE

DOEpatents

Thomas, J.R.

1958-08-26

>Various processes for the recovery of plutonium require that the plutonium be obtalned and maintained in the reduced or trivalent state in solution. Ferrous ions are commonly used as the reducing agent for this purpose, but it is difficult to maintain the plutonium in a reduced state in nitric acid solutions due to the oxidizing effects of the acid. It has been found that the addition of a stabilizing or holding reductant to such solution prevents reoxidation of the plutonium. Sulfamate ions have been found to be ideally suitable as such a stabilizer even in the presence of nitric acid.

The effect of the composition of plutonium loaded on the reactivity change and the isotopic composition of fuel produced in a fast reactor

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.

METHOD OF SEPARATING TETRAVALENT PLUTONIUM VALUES FROM CERIUM SUB-GROUP RARE EARTH VALUES

DOEpatents

Duffield, R.B.; Stoughton, R.W.

1959-02-01

A method is presented for separating plutonium from the cerium sub-group of rare earths when both are present in an aqueous solution. The method consists in adding an excess of alkali metal carbonate to the solution, which causes the formation of a soluble plutonium carbonate precipitate and at the same time forms an insoluble cerium-group rare earth carbonate. The pH value must be adjusted to bctween 5.5 and 7.5, and prior to the precipitation step the plutonium must be reduced to the tetravalent state since only tetravalent plutonium will form the soluble carbonate complex.

CONCENTRATION OF Pu USING AN IODATE PRECIPITATE

DOEpatents

Fries, B.A.

1960-02-23

A method is given for separating plutonium from lanthanum in a lanthanum fluoride carrier precipitation process for the recovery of plutonium values from an aqueous solution. The carrier precipitation process includes the steps of forming a lanthanum fluoride precipi- . tate, thereby carrying plutonium out of solution, metathesizing the fluoride precipitate to a hydroxide precipitate, and then dissolving the hydroxide precipitate in nitric acid. In accordance with the invention, the nitric acid solution, which contains plutonium and lanthanum, is made 0.05 to 0.15 molar in potassium iodate. thereby precipitating plutonium as plutonous iodate and the plutonous iodate is separated from the lanthanum- containing supernatant solution.

ION EXCHANGE ADSORPTION PROCESS FOR PLUTONIUM SEPARATION

DOEpatents

Boyd, G.E.; Russell, E.R.; Taylor, M.D.

1961-07-11

Ion exchange processes for the separation of plutonium from fission products are described. In accordance with these processes an aqueous solution containing plutonium and fission products is contacted with a cation exchange resin under conditions favoring adsorption of plutonium and fission products on the resin. A portion of the fission product is then eluted with a solution containing 0.05 to 1% by weight of a carboxylic acid. Plutonium is next eluted with a solution containing 2 to 8 per cent by weight of the same carboxylic acid, and the remaining fission products on the resin are eluted with an aqueous solution containing over 10 per cent by weight of sodium bisulfate.

IMPROVED PROCESS OF PLUTONIUM CARRIER PRECIPITATION

DOEpatents

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.

Advances in containment methods and plutonium recovery strategies that led to the structural characterization of plutonium(IV) tetrachloride tris-diphenylsulfoxide, PuCl 4(OSPh 2) 3

DOE PAGES

Schrell, Samantha K.; Boland, Kevin Sean; Cross, Justin Neil; ...

2017-01-18

In an attempt to further advance the understanding of plutonium coordination chemistry, we report a robust method for recycling and obtaining plutonium aqueous stock solutions that can be used as a convenient starting material in plutonium synthesis. This approach was used to prepare and characterize plutonium(IV) tetrachloride tris-diphenylsulfoxide, PuCl 4(OSPh 2) 3, by single crystal X-ray diffraction. The PuCl 4(OSPh 2) 3 compound represents a rare example of a 7-coordinate plutonium(IV) complex. Structural characterization of PuCl 4(OSPh 2) 3 by X-ray diffraction utilized a new containment method for radioactive crystals. The procedure makes use of epoxy, polyimide loops, and amore » polyester sheath to provide a robust method for safely containing and easily handling radioactive samples. Lastly, the described procedure is more user friendly than traditional containment methods that employ fragile quartz capillary tubes. Additionally, moving to polyester, instead of quartz, lowers the background scattering from the heavier silicon atoms.« less

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

PLUTONIUM-CERIUM ALLOY

DOEpatents

Coffinberry, A.S.

1959-01-01

An alloy is presented for use as a reactor fuel. The binary alloy consists essentially of from about 5 to 90 atomic per cent cerium and the balance being plutonium. A complete phase diagram for the cerium--plutonium system is given.

Plutonium recovery from organic materials

DOEpatents

Deaton, R.L.; Silver, G.L.

1973-12-11

A method is described for removing plutonium or the like from organic material wherein the organic material is leached with a solution containing a strong reducing agent such as titanium (III) (Ti/sup +3None)/, chromium (II) (Cr/ sup +2/), vanadium (II) (V/sup +2/) ions, or ferrous ethylenediaminetetraacetate (EDTA), the leaching yielding a plutonium-containing solution that is further processed to recover plutonium. The leach solution may also contain citrate or tartrate ion. (Official Gazette)

SEPARATION OF PLUTONIUM FROM AQUEOUS SOLUTIONS BY ION-EXCHANGE

DOEpatents

Schubert, J.

1958-06-01

A process is described for the separation of plutonium from an aqueous solution of a plutonium salt, which comprises adding to the solution an acid of the group consisting of sulfuric acid, phosphoric acid, and oxalic acid, and mixtures thereof to provide an acid concentration between 0.0001 and 1 M, contacting the resultant solution with a synthetic organic anion exchange resin, and separating the aqueous phase and the resin which contains the plutonium.

14. END VIEW OF THE PLUTONIUM STORAGE VAULT FROM THE ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

14. END VIEW OF THE PLUTONIUM STORAGE VAULT FROM THE REMOTE CONTROL STATION. THE STACKER-RETRIEVER, A REMOTELY-OPERATED, MECHANIZED TRANSPORT SYSTEM, RETRIEVES CONTAINERS OF PLUTONIUM FROM SAFE GEOMETRY PALLETS STORED ALONG THE LENGTH OF THE VAULT. THE STACKER-RETRIEVER RUNS ALONG THE AISLE BETWEEN THE PALLETS OF THE STORAGE CHAMBER. (3/2/86) - Rocky Flats Plant, Plutonium Recovery Facility, Northwest portion of Rocky Flats Plant, Golden, Jefferson County, CO

PROCESS OF TREATING URANIUM HEXAFLUORIDE AND PLUTONIUM HEXAFLUORIDE MIXTURES WITH SULFUR TETRAFLUORIDE TO SEPARATE SAME

DOEpatents

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)

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)

PROCESS OF SEPARATING PLUTONIUM VALUES BY ELECTRODEPOSITION

DOEpatents

Whal, A.C.

1958-04-15

A process is described of separating plutonium values from an aqueous solution by electrodeposition. The process consists of subjecting an aqueous 0.1 to 1.0 N nitric acid solution containing plutonium ions to electrolysis between inert metallic electrodes. A current density of one milliampere io one ampere per square centimeter of cathode surface and a temperature between 10 and 60 d C are maintained. Plutonium is electrodeposited on the cathode surface and recovered.

SEPARATION OF PLUTONIUM VALUES FROM URANIUM AND FISSION PRODUCT VALUES

DOEpatents

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.

Using Biomolecules to Separate Plutonium

NASA Astrophysics Data System (ADS)

Gogolski, Jarrod

Used nuclear fuel has traditionally been treated through chemical separations of the radionuclides for recycle or disposal. This research considers a biological approach to such separations based on a series of complex and interdependent interactions that occur naturally in the human body with plutonium. These biological interactions are mediated by the proteins serum transferrin and the transferrin receptor. Transferrin to plutonium in vivo and can deposit plutonium into cells after interacting with the transferrin receptor protein at the cell surface. Using cerium as a non-radioactive surrogate for plutonium, it was found that cerium(IV) required multiple synergistic anions to bind in the N-lobe of the bilobal transferrin protein, creating a conformation of the cerium-loaded protein that would be unable to interact with the transferrin receptor protein to achieve a separation. The behavior of cerium binding to transferrin has contributed to understanding how plutonium(IV)-transferrin interacts in vivo and in biological separations.

CARBONATE METHOD OF SEPARATION OF TETRAVALENT PLUTONIUM FROM FISSION PRODUCT VALUES

DOEpatents

Duffield, R.B.; Stoughton, R.W.

1959-02-01

It has been found that plutonium forms an insoluble precipitate with carbonate ion when the carbonate ion is present in stoichiometric proportions, while an excess of the carbonate ion complexes plutonium and renders it soluble. A method for separating tetravalent plutonium from lanthanum-group rare earths has been based on this discovery, since these rare earths form insoluble carbonates in approximately neutral solutions. According to the process the pH is adjusted to between 5 and 7, and approximately stoichiometric amounts of carbonate ion are added to the solution causing the formation of a precipitate of plutonium carbonate and the lanthanum-group rare earth carbonates. The precipitate is then separated from the solution and contacted with a carbonate solution of a concentration between 1 M and 3 M to complex and redissolve the plutonium precipitate, and thus separate it from the insoluble rare earth precipitate.

PROCESS FOR PRODUCTION OF PLUTONIUM FROM ITS OXIDES

DOEpatents

Weissman, S.I.; Perlman, M.L.; Lipkin, D.

1959-10-13

A method is described for obtaining a carbide of plutonium and two methods for obtaining plutonium metal from its oxides. One of the latter involves heating the oxide, in particular PuO/sub 2/, to a temperature of 1200 to 1500 deg C with the stoichiometrical amount of carbon to fornn CO in a hard vacuum (3 to 10 microns Hg), the reduced and vaporized plutonium being collected on a condensing surface above the reaction crucible. When an excess of carbon is used with the PuO/sub 2/, a carbide of plutonium is formed at a crucible temperature of 1400 to 1500 deg C. The process may be halted and the carbide removed, or the reaction temperature can be increased to 1900 to 2100 deg C at the same low pressure to dissociate the carbide, in which case the plutonium is distilled out and collected on the same condensing surface.

Excess Weapons Plutonium Disposition: Plutonium Packaging, Storage and Transportation and Waste Treatment, Storage and Disposal Activities

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jardine, L J; Borisov, G B

2004-07-21

A fifth annual Excess Weapons Plutonium Disposition meeting organized by Lawrence Livermore National Laboratory (LLNL) was held February 16-18, 2004, at the State Education Center (SEC), 4 Aerodromnya Drive, St. Petersburg, Russia. The meeting discussed Excess Weapons Plutonium Disposition topics for which LLNL has the US Technical Lead Organization responsibilities. The technical areas discussed included Radioactive Waste Treatment, Storage, and Disposal, Plutonium Oxide and Plutonium Metal Packaging, Storage and Transportation and Spent Fuel Packaging, Storage and Transportation. The meeting was conducted with a conference format using technical presentations of papers with simultaneous translation into English and Russian. There were 46more » Russian attendees from 14 different Russian organizations and six non-Russian attendees, four from the US and two from France. Forty technical presentations were made. The meeting agenda is given in Appendix B and the attendance list is in Appendix C.« less

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

Amarillo National Resource Center for Plutonium. Quarterly technical progress report, May 1, 1997--July 31, 1997

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

Progress summaries are provided from the Amarillo National Center for Plutonium. Programs include the plutonium information resource center, environment, public health, and safety, education and training, nuclear and other material studies.

SEPARATION OF PLUTONIUM FROM URANIUM

DOEpatents

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.

1. West facade of Plutonium Concentration Facility (Building 233S), ReductionOxidation ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

1. West facade of Plutonium Concentration Facility (Building 233-S), Reduction-Oxidation Building (REDOX-202-S) to the right. Looking east. - Reduction-Oxidation Complex, Plutonium Concentration Facility, 200 West Area, Richland, Benton County, WA

69. INTERIOR, BUILDING 272 (PLUTONIUM STORAGE BUILDING) LOOKING SOUTHWEST THROUGH ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

69. INTERIOR, BUILDING 272 (PLUTONIUM STORAGE BUILDING) LOOKING SOUTHWEST THROUGH DOOR-WAY INTO PLUTONIUM STORAGE AREA. - Loring Air Force Base, Weapons Storage Area, Northeastern corner of base at northern end of Maine Road, Limestone, Aroostook County, ME

Volatile Impurities in the Plutonium Immobilization Ceramic Wasteform

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cozzi, A.D.

1999-10-15

Approximately 18 of the 50 metric tons of plutonium identified for disposition contain significant quantities of impurities. A ceramic waste form is the chosen option for immobilization of the excess plutonium. The impurities associated with the stored plutonium have been identified (CaCl2, MgF2, Pb, etc.). For this study, only volatile species are investigated. The impurities are added individually. Cerium is used as the surrogate for plutonium. Three compositions, including the baseline composition, were used to verify the ability of the ceramic wasteform to accommodate impurities. The criteria for evaluation of the effect of the impurities were the apparent porosity andmore » phase assemblage of sintered pellets.« less

PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINATING ELEMENTS

DOEpatents

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.

Progress on plutonium stabilization

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hurt, D.

1996-05-01

The Defense Nuclear Facilities Safety Board has safety oversight responsibility for most of the facilities where unstable forms of plutonium are being processed and packaged for interim storage. The Board has issued recommendations on plutonium stabilization and has has a considerable influence on DOE`s stabilization schedules and priorities. The Board has not made any recommendations on long-term plutonium disposition, although it may get more involved in the future if DOE develops plans to use defense nuclear facilities for disposition activities.

NON-CORROSIVE PLUTONIUM FUEL SYSTEMS

DOEpatents

Coffinberry, A.S.; Waber, J.T.

1962-10-23

An improved plutonium reactor liquid fuel is described for utilization in a nuclear reactor having a tantalum fuel containment vessel. The fuel consists of plutonium and a diluent such as iron, cobalt, nickel, cerium, cerium-- iron, cerium--cobalt, cerium--nickel, and cerium--copper, and an additive of carbon and silicon. The carbon and silicon react with the tantalum container surface to form a coating that is self-healing and prevents the corrosive action of liquid plutonium on the said tantalum container. (AEC)

Plutonium in the atmosphere: A global perspective.

PubMed

Thakur, P; Khaing, H; Salminen-Paatero, S

2017-09-01

A number of potential source terms have contributed plutonium isotopes to the atmosphere. The atmospheric nuclear weapon tests conducted between 1945 and 1980 and the re-entry of the burned SNAP-9A satellite in 1964, respectively. It is generally believed that current levels of plutonium in the stratosphere are negligible and compared with the levels generally found at surface-level air. In this study, the time trend analysis and long-term behavior of plutonium isotopes ( 239+240 Pu and 238 Pu) in the atmosphere were assessed using historical data collected by various national and international monitoring networks since 1960s. An analysis of historical data indicates that 239+240 Pu concentration post-1984 is still frequently detectable, whereas 238 Pu is detected infrequently. Furthermore, the seasonal and time-trend variation of plutonium concentration in surface air followed the stratospheric trends until the early 1980s. After the last Chinese test of 1980, the plutonium concentrations in surface air dropped to the current levels, suggesting that the observed concentrations post-1984 have not been under stratospheric control, but rather reflect the environmental processes such as resuspension. Recent plutonium atmospheric air concentrations data show that besides resuspension, other environmental processes such as global dust storms and biomass burning/wildfire also play an important role in redistributing plutonium in the atmosphere. Copyright © 2017 Elsevier Ltd. All rights reserved.

Plutonium and americium in the foodchain lichen-reindeer-man

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jaakkola, T.; Hakanen, M.; Keinonen, M.

1977-01-01

The atmospheric nuclear tests have produced a worldwide fallout of transuranium elements. In addition to plutonium measurable concentrations of americium are to be found in terrestrial and aquatic environments. The metabolism of plutonium in reindeer was investigated by analyzing plutonium in liver, bone, and lung collected during 1963-1976. To determine the distribution of plutonium in reindeer all tissues of four animals of different ages were analyzed. To estimate the uptake of plutonium from the gastrointestinal tract in reindeer, the tissue samples of elk were also analyzed. Elk which is of the same genus as reindeer does not feed on lichenmore » but mainly on deciduous plants, buds, young twigs, and leaves of trees and bushes. The composition of its feed corresponds fairly well to that of reindeer during the summer. Studies on behaviour of americium along the foodchain lichen-reindeer-man were started by determining the Am-241 concentrations in lichen and reindeer liver. The Am-241 results were compared with those of Pu-239,240. The plutonium contents of the southern Finns, whose diet does not contain reindeer tissues, were determined by analyzing autopsy tissue samples (liver, lung, and bone). The southern Finns form a control group to the Lapps consuming reindeer tissues. Plutonium analyses of the placenta, blood, and tooth samples of the Lapps were performed.« less

METHOD OF REDUCING PLUTONIUM COMPOUNDS

DOEpatents

Johns, I.B.

1958-06-01

A method is described for reducing plutonium compounds in aqueous solution from a higher to a lower valence state. This reduction of valence is achieved by treating the aqueous solution of higher valence plutonium compounds with hydrogen in contact with an activated platinum catalyst.

71. INTERIOR, BUILDING 272 (PLUTONIUM STORAGE BUILDING) LOOKING NORTHEAST INTO ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

71. INTERIOR, BUILDING 272 (PLUTONIUM STORAGE BUILDING) LOOKING NORTHEAST INTO PLUTONIUM STORAGE ROOM SHOWING CUBICLES FOR STORAGE. - Loring Air Force Base, Weapons Storage Area, Northeastern corner of base at northern end of Maine Road, Limestone, Aroostook County, ME

Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA. A Long-Term Study

DOE PAGES

Armstrong, Christopher R.; Nuessle, Patterson R.; Brant, Heather A.; ...

2015-01-16

This work presents the findings of a long term plutonium study at Savannah River Site (SRS) conducted between 2003 and 2013. Terrestrial environmental samples were obtained at Savannah River National Laboratory (SRNL) in A-area. Plutonium content and isotopic abundances were measured over this time period by alpha spectrometry and three stage thermal ionization mass spectrometry (3STIMS). Here we detail the complete sample collection, radiochemical separation, and measurement procedure specifically targeted to trace plutonium in bulk environmental samples. Total plutonium activities were determined to be not significantly above atmospheric global fallout. However, the 238Pu/ 239+240Pu activity ratios attributed to SRS aremore » above atmospheric global fallout ranges. The 240Pu/ 239Pu atom ratios are reasonably consistent from year to year and are lower than fallout, while the 242Pu/ 239Pu atom ratios are higher than fallout values. Overall, the plutonium signatures obtained in this study reflect a mixture of weapons-grade, higher burn-up, and fallout material. This study provides a blue print for long term low level monitoring of plutonium in the environment.« less

Electronic structure, phase transitions and diffusive properties of elemental plutonium

NASA Astrophysics Data System (ADS)

Setty, Arun; Cooper, B. R.

2003-03-01

We present a SIC-LDA-LMTO based study of the electronic structure of the delta, alpha and gamma phases of plutonium, and also of the alpha and gamma phases of elemental cerium. We find excellent agreement with the experimental densities and magnetic properties [1]. Furthermore, detailed studies of the computational densities of states for delta plutonium, and comparison with the experimental photoemission spectrum [2], provide evidence for the existence of an unusual fluctuating valence state. Results regarding the vacancy formation and self-diffusion in delta plutonium will be presented. Furthermore, a study of interface diffusion between plutonium and steel (technologically relevant in the storage of spent fuel) or other technologically relevant alloys will be included. Preliminary results regarding gallium stabilization of delta plutonium, and of plutonium alloys will be presented. [1] M. Dormeval et al., private communication (2001). [2] A. J. Arko, J. J. Joyce, L. Morales, J. Wills, and J. Lashley et. al., Phys. Rev. B, 62, 1773 (2000). [3] B. R. Cooper et al, Phil. Mag. B 79, 683 (1999); B.R. Cooper, Los Alamos Science 26, 106 (2000)); B.R. Cooper, A.K. Setty and D.L.Price, to be published.

Radiation damage and annealing in plutonium tetrafluoride

NASA Astrophysics Data System (ADS)

McCoy, Kaylyn; Casella, Amanda; Sinkov, Sergey; Sweet, Lucas; McNamara, Bruce; Delegard, Calvin; Jevremovic, Tatjana

2017-12-01

A sample of plutonium tetrafluoride that was separated prior to 1966 at the Hanford Site in Washington State was analyzed at the Pacific Northwest National Laboratory (PNNL) in 2015 and 2016. The plutonium tetrafluoride, as received, was an unusual color and considering the age of the plutonium, there were questions about the condition of the material. These questions had to be answered in order to determine the suitability of the material for future use or long-term storage. Therefore, thermogravimetric/differential thermal analysis and X-ray diffraction evaluations were conducted to determine the plutonium's crystal structure, oxide content, and moisture content; these analyses reported that the plutonium was predominately amorphous and tetrafluoride, with an oxide content near ten percent. Freshly fluorinated plutonium tetrafluoride is known to be monoclinic. During the initial thermogravimetric/differential thermal analyses, it was discovered that an exothermic event occurred within the material near 414 °C. X-ray diffraction analyses were conducted on the annealed tetrafluoride. The X-ray diffraction analyses indicated that some degree of recrystallization occurred in conjunction with the 414 °C event. The following commentary describes the series of thermogravimetric/differential thermal and X-ray diffraction analyses that were conducted as part of this investigation at PNNL.

Determination of plutonium isotopes (238,239,240Pu) and strontium (90Sr) in seafood using alpha spectrometry and liquid scintillation spectrometry.

PubMed

Shin, Choonshik; Choi, Hoon; Kwon, Hye-Min; Jo, Hye-Jin; Kim, Hye-Jeong; Yoon, Hae-Jung; Kim, Dong-Sul; Kang, Gil-Jin

2017-10-01

The present study was carried out to survey the levels of plutonium isotopes ( 238 , 239 , 240 Pu) and strontium ( 90 Sr) in domestic seafood in Korea. In current, regulatory authorities have analyzed radionuclides, such as 134 Cs, 137 Cs and 131 I, in domestic and imported food. However, people are concerned about contamination of other radionuclides, such as plutonium and strontium, in food. Furthermore, people who live in Korea have much concern about safety of seafood. Accordingly, in this study, we have investigated the activity concentrations of plutonium and strontium in seafood. For the analysis of plutonium isotopes and strontium, a rapid and reliable method developed from previous study was used. Applicability of the test method was verified by examining recovery, minimum detectable activity (MDA), analytical time, etc. Total 40 seafood samples were analyzed in 2014-2015. As a result, plutonium isotopes ( 238 , 239 , 240 Pu) and strontium ( 90 Sr) were not detected or below detection limits in seafood. The detection limits of plutonium isotopes and strontium-90 were 0.01 and 1 Bq/kg, respectively. Copyright © 2017 Elsevier Ltd. All rights reserved.

Finding Balance Between Biological Groundwater Treatment and Treated Injection Water

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carlson, Mark A.; Nielsen, Kellin R.; Byrnes, Mark E.

2015-01-14

At the U.S. Department of Energy’s Hanford Site, CH2M HILL Plateau Remediation Company operates the 200 West Pump and Treat which was engineered to treat radiological and chemical contaminants in groundwater as a result of the site’s former plutonium production years. Fluidized bed bioreactors (FBRs) are used to remove nitrate, metals, and volatile organic compounds. Increasing nitrate concentrations in the treatment plant effluent and the presence of a slimy biomass (a typical microorganism response to stress) in the FBRs triggered an investigation of nutrient levels in the system. Little, if any, micronutrient feed was coming into the bioreactors. Additionally, carbonmore » substrate (used to promote biological growth) was passing through to the injection wells, causing biological fouling of the wells and reduced specific injectivity. Adjustments to the micronutrient feed improved microorganism health, but the micronutrients were being overfed (particularly manganese) plugging the injection wells further. Injection well rehabilitation to restore specific injectivity required repeated treatments to remove the biological fouling and precipitated metal oxides. A combination of sulfamic and citric acids worked well to dissolve metal oxides and sodium hypochlorite effectively removed the biological growth. Intensive surging and development techniques successfully removed clogging material from the injection wells. Ultimately, the investigation and nutrient adjustments took months to restore proper balance to the microbial system and over a year to stabilize injection well capacities. Carefully tracking and managing the FBRs and well performance monitoring are critical to balancing the needs of the treatment system while reducing fouling mechanisms in the injection wells.« less

EXTRACTION OF TETRAVALENT PLUTONIUM VALUES WITH METHYL ETHYL KETONE, METHYL ISOBUTYL KETONE ACETOPHENONE OR MENTHONE

DOEpatents

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)

10 CFR 830.3 - Definitions.

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...

3. AERIAL VIEW, LOOKING SOUTH, OF BUILDING 371 BASEMENT UNDER ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

3. AERIAL VIEW, LOOKING SOUTH, OF BUILDING 371 BASEMENT UNDER CONSTRUCTION. THE BASEMENT HOUSES HEATING, VENTILATION, AND AIR CONDITIONING EQUIPMENT AND MECHANICAL UTILITIES, THE UPPER PART OF THE PLUTONIUM STORAGE VAULT AND MAINTENANCE BAY, AND SMALL PLUTONIUM PROCESSING AREAS. THE BASEMENT LEVEL IS DIVIDED INTO NEARLY EQUAL NORTH AND SOUTH PARTS BY THE UPPER PORTION OF THE PLUTONIUM STORAGE VAULT. (10/7/74) - Rocky Flats Plant, Plutonium Recovery Facility, Northwest portion of Rocky Flats Plant, Golden, Jefferson County, CO

PLATINUM HEXAFLUORIDE AND METHOD OF FLUORINATING PLUTONIUM CONTAINING MIXTURES THERE-WITH

DOEpatents

Malm, J.G.; Weinstock, B.; Claassen, H.H.

1959-07-01

The preparation of platinum hexafluoride and its use as a fluorinating agent in a process for separating plutonium from fission products is presented. According to the invention, platinum is reacted with fluorine gas at from 900 to 1100 deg C to form platinum hexafluoride. The platinum hexafluoride is then contacted with the plutonium containing mixture at room temperature to form plutonium hexafluoride which is more volatile than the fission products fluorides and therefore can be isolated by distillation.

Uranium daughter growth must not be neglected when adjusting plutonium materials for assay and isotopic contents

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.

Sources of plutonium in the atmosphere and stratosphere-troposphere mixing

PubMed Central

Hirose, Katsumi; Povinec, Pavel P.

2015-01-01

Plutonium isotopes have primarily been injected to the stratosphere by the atmospheric nuclear weapon tests and the burn-up of the SNAP-9A satellite. Here we show by using published data that the stratospheric plutonium exponentially decreased with apparent residence time of 1.5 ± 0.5 years, and that the temporal variations of plutonium in surface air followed the stratospheric trends until the early 1980s. In the 2000s, plutonium and its isotope ratios in the atmosphere varied dynamically, and sporadic high concentrations of 239,240Pu reported for the lower stratospheric and upper tropospheric aerosols may be due to environmental events such as the global dust outbreaks and biomass burning. PMID:26508010

25. Plutonium Recovery From Contaminated Materials, Architectural Plans & Details, ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

25. Plutonium Recovery From Contaminated Materials, Architectural Plans & Details, Building 232-Z, U.S. Atomic Energy Commission, Hanford Atomic Products Operation, General Electric Company, Dwg. No. H-2-23105, 1959. - Plutonium Finishing Plant, Waste Incinerator Facility, 200 West Area, Richland, Benton County, WA

24. Plutonium Recovery From Contaminated Materials, Architectural Details, Building 232z, ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

24. Plutonium Recovery From Contaminated Materials, Architectural Details, Building 232-z, U.S. Atomic Energy Commission, Hanford Atomic Products Operation, General Electric Company, Dwg. No. H-2-23106, 1959. - Plutonium Finishing Plant, Waste Incinerator Facility, 200 West Area, Richland, Benton County, WA

26. Plutonium Recovery From Contaminated Materials, Architectural Elevations, Sections & ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

26. Plutonium Recovery From Contaminated Materials, Architectural Elevations, Sections & Dets., Building 232-Z, U.S. Atomic Energy Commission, Hanford Atomic Products Operation, General Electric Company, Dwg. No. H-2-23106, 1959. - Plutonium Finishing Plant, Waste Incinerator Facility, 200 West Area, Richland, Benton County, WA

13. VIEW OF THE MOLTEN SALT EXTRACTION LINE. THE MOLTEN ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

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

CONCENTRATION PROCESS FOR PLUTONIUM IONS, IN AN OXIDATION STATE NOT GREATER THAN +4, IN AQUEOUS ACID SOLUTION

DOEpatents

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.

Plutonium release from Fukushima Daiichi fosters the need for more detailed investigations

NASA Astrophysics Data System (ADS)

Schneider, Stephanie; Walther, Clemens; Bister, Stefan; Schauer, Viktoria; Christl, Marcus; Synal, Hans-Arno; Shozugawa, Katsumi; Steinhauser, Georg

2013-10-01

The contamination of Japan after the Fukushima accident has been investigated mainly for volatile fission products, but only sparsely for actinides such as plutonium. Only small releases of actinides were estimated in Fukushima. Plutonium is still omnipresent in the environment from previous atmospheric nuclear weapons tests. We investigated soil and plants sampled at different hot spots in Japan, searching for reactor-borne plutonium using its isotopic ratio 240Pu/239Pu. By using accelerator mass spectrometry, we clearly demonstrated the release of Pu from the Fukushima Daiichi power plant: While most samples contained only the radionuclide signature of fallout plutonium, there is at least one vegetation sample whose isotope ratio (0.381 +/- 0.046) evidences that the Pu originates from a nuclear reactor (239+240Pu activity concentration 0.49 Bq/kg). Plutonium content and isotope ratios differ considerably even for very close sampling locations, e.g. the soil and the plants growing on it. This strong localization indicates a particulate Pu release, which is of high radiological risk if incorporated.

Plutonium release from the 903 pad at Rocky Flats.

PubMed

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).

An analysis of the background and development of regulations for the air transport of plutonium in the USA

DOE Office of Scientific and Technical Information (OSTI.GOV)

McClure, J.D.; Luna, R.E.

1989-01-01

Several aspects of special packagings of plutonium for air transport should be recognized. The accident cases cited by Congressman Scheuer were incidents of local plutonium contamination in military aircraft accidents that had nuclear weapons on board. There is no disputing the occurrence of these military accidents but military weapon shipments were exempted from the provisions of the Scheuer amendment. There have been no recorded civilian aircraft crashes involving plutonium dispersal although there have been civilian aircraft crashes that were severe. Shortly after the introduction of the amendment by Mr. Scheuer on June 20, 1975, there was a serious aircraft crashmore » at JFK International. In his remarks to the House on July 24, 1975 Mr. Scheuer called attention to this event. The NRC originally opposed the provisions of the Scheuer amendment but with the passing of the amendment NRC compiled with its provisions. This led to the development of the plutonium air transport package PAT-1 in the US. The introduction of special rules for the air transport of plutonium into the US packaging regulations has been made them more severe than the provision of the international regulations, IAEA Safety Series 6. The IAEA is now discussing proposed regulations related to the air transport of plutonium. An additional legislative action was introduced the US in December 1987 which would require actual crash tests of packages intended for the air transport of plutonium, the Murkowski amendment. 13 refs.« less

Effects of Aging on PuO2∙xH2O Particle Size in Alkaline Solution

DOE Office of Scientific and Technical Information (OSTI.GOV)

Delegard, Calvin H.

Between 1944 and 1989, 54.5 metric tons of the United States’ weapons-grade plutonium and an additional 12.9 metric tons of fuel-grade plutonium were produced and separated from irradiated fuel at the Hanford Site. Acidic high-activity wastes containing around 600 kg of plutonium were made alkaline and discharged to underground storage tanks from separations, isolation, and recycle processes to yield average plutonium concentration of about 0.003 grams per liter (or ~0.0002 wt%) in the ~200 million liter tank waste volume. The plutonium is largely associated with low-solubility metal hydroxide/oxide sludges where its low concentration and intimate mixture with neutron-absorbing elements (e.g.,more » iron) are credited in nuclear criticality safety. However, concerns have been expressed that plutonium, in the form of plutonium hydrous oxide, PuO2∙xH2O, could undergo sufficient crystal growth through dissolution and reprecipitation in the alkaline tank waste to potentially become separable from neutron absorbing constituents by settling or sedimentation. Thermodynamic considerations and laboratory studies of systems chemically analogous to tank waste show that the plutonium formed in the alkaline tank waste by precipitation through neutralization from acid solution probably entered as 2–4-nm PuO2∙xH2O crystallite particles that, because of their low solubility and opposition from radiolytic processes, grow from that point at exceedingly slow rates, thus posing no risk of physical segregation.« less

Radioecology of natural systems. Fifteenth annual progress report, August 1, 1976--July 31, 1977. [Plutonium transport in terrestrial ecosystems at Rocky Flats Plant with emphasis on biological effects on mule deer and coyotes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Whicker, F.W.

1977-08-01

This report summarizes project activities during the period August 1, 1976 through July 31, 1977. Four major areas of effort are reported, namely plutonium behavior in a terrestrial ecosystem at Rocky Flats, mule deer and coyote studies at Rocky Flats, ecological consequences of transuranics in the terrestrial environment, and lead geochemistry of an alpine lake ecosystem. Much of the first area of effort involved the synthesis of data and preparation of manuscripts, although some new data are reported on plutonium levels in small mammals, plant uptake of plutonium from contaminated soil, and plutonium deposition rates on macroplot 1. The mulemore » deer studies generated a substantial body of new information which will permit quantitative assessment of plutonium dispersion by deer that utilize contaminated areas. These studies involve population dynamics, movement and use patterns, food habits, ingestion rates of contaminated soil and vegetation and plutonium burdens of deer tissues. A related study of coyote food habits in summer at Rocky Flats is reported. A manuscript dealing with the question of ecological effects of transuranics was prepared. This manuscript incorporates data from Rocky Flats on characteristics of natural populations which occupy ecologically similar areas having differing levels of plutonium contamination. The lead geochemistry studies continued to generate new data but the data are not yet reported.« less

COMPLEX FLUORIDES OF PLUTONIUM AND AN ALKALI METAL

DOEpatents

Seaborg, G.T.

1960-08-01

A method is given for precipitating alkali metal plutonium fluorides. such as KPuF/sub 5/, KPu/sub 2/F/sub 9/, NaPuF/sub 5/, and RbPuF/sub 5/, from an aqueous plutonium(IV) solution by adding hydrogen fluoride and alkali-metal- fluoride.

DELTA PHASE PLUTONIUM ALLOYS

DOEpatents

Cramer, E.M.; Ellinger, F.H.; Land. C.C.

1960-03-22

Delta-phase plutonium alloys were developed suitable for use as reactor fuels. The alloys consist of from 1 to 4 at.% zinc and the balance plutonium. The alloys have good neutronic, corrosion, and fabrication characteristics snd possess good dimensional characteristics throughout an operating temperature range from 300 to 490 deg C.

RECOVERY OF PLUTONIUM BY CARRIER PRECIPITATION

DOEpatents

Goeckermann, R.H.

1961-04-01

A process is given for recovering plutonium from an aqueous nitric acid zirconium-containing solution of an acidity between 0.2 and 1 N by adding fluoride anions (1.5 to 5 mg/l) and precipitating the plutonium with an excess of hydrogen peroxide at from 53 to 65 deg C.

EPA Method: Rapid Radiochemical Method for Americium-241, Radium-226, Plutonium-238/-239, Radiostronium, and Isotopic Uranium in Water for Environmental Restoration Following Homeland Security Events

EPA Pesticide Factsheets

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.

METHOD FOR OBTAINING PLUTONIUM METAL FROM ITS TRICHLORIDE

DOEpatents

Reavis, J.G.; Leary, J.A.; Maraman, W.J.

1962-08-14

A method was developed for obtaining plutonium metal by direct reduction of plutonium chloride, without the use of a booster, using calcium and lanthamum as a reductant, the said reduction being carried out at temperature in the range of 700 to 850 deg C and at about atmospheric pressure. (AEC)

MOLTEN PLUTONIUM FUELED FAST BREEDER REACTOR

DOEpatents

Kiehn, R.M.; King, L.D.P.; Peterson, R.E.; Swickard, E.O. Jr.

1962-06-26

A description is given of a nuclear fast reactor fueled with molten plutonium containing about 20 kg of plutonium in a tantalum container, cooled by circulating liquid sodium at about 600 to 650 deg C, having a large negative temperature coefficient of reactivity, and control rods and movable reflector for criticality control. (AEC)

ELECTRODEPOSITION OF PLUTONIUM

DOEpatents

Wolter, F.J.

1957-09-10

A process of electrolytically recovering plutonium from dilute aqueous solutions containing plutonium ions comprises electrolyzing the solution at a current density of about 0.44 ampere per square centimeter in the presence of an acetate-sulfate buffer while maintaining the pH of the solution at substantially 5 and using a stirred mercury cathode.

Removal of plutonium from hepatic tissue

DOEpatents

Lindenbaum, Arthur; Rosenthal, Marcia W.

1979-01-01

A method is provided for removing plutonium from hepatic tissues by introducing into the body and blood stream a solution of the complexing agent DTPA and an adjunct thereto. The adjunct material induces aberrations in the hepatic tissue cells and removes intracellularly deposited plutonium which is normally unavailable for complexation with the DTPA. Once the intracellularly deposited plutonium has been removed from the cell by action of the adjunct material, it can be complexed with the DTPA present in the blood stream and subsequently removed from the body by normal excretory processes.

Rapid Method for Sodium Hydroxide Fusion of Concrete and ...

EPA Pesticide Factsheets

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.

METHOD OF SEPARATING PLUTONIUM FROM LANTHANUM FLUORIDE CARRIER

DOEpatents

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.

PROCESS OF TREATING OR FORMING AN INSOLUBLE PLUTONIUM PRECIPITATE IN THE PRESENCE OF AN ORGANIC ACTIVE AGENT

DOEpatents

Balthis, J.H.

1961-07-18

Carrier precipitation processes for the separation of plutonium from fission products are described. In a process in which an insoluble precipitate is formed in a solution containing plutonium and fission products under conditions whereby plutonium is carried by the precipitate, and the precipitate is then separated from the remaining solution, an organic surface active agent is added to the mixture of precipitate and solution prior to separation of the precipitate from the supernatant solution, thereby improving the degree of separation of the precipitate from the solution.

1. VIEW OF THE CONTROL ROOM FOR THE XY RETRIEVER. ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

1. VIEW OF THE CONTROL ROOM FOR THE X-Y RETRIEVER. USING THE X-Y RETRIEVER, OPERATORS RETRIEVED PLUTONIUM METAL FROM THE PLUTONIUM STORAGE VAULTS (IN MODULE K) AND CONVEYED IT TO THE X-Y SHUTTLE AREA WHERE IT WAS CUT AND WEIGHED. FROM THE SHUTTLE AREA THE PLUTONIUM WAS CONVEYED TO MODULES A, J OR K FOR CASTING, OR MODULE B FOR ROLLING AND FORMING. (5/17/71) - Rocky Flats Plant, Plutonium Manufacturing Facility, North-central section of Plant, just south of Building 776/777, Golden, Jefferson County, CO

Radiation from plutonium 238 used in space applications

NASA Technical Reports Server (NTRS)

Keenan, T. K.; Vallee, R. E.; Powers, J. A.

1972-01-01

The principal mode of the nuclear decay of plutonium 238 is by alpha particle emission at a rate of 17 curies per gram. Gamma radiation also present in nuclear fuels arises primarily from the nuclear de-excitation of daughter nuclei as a result of the alpha decay of plutonium 238 and reactor-produced impurities. Plutonium 238 has a spontaneous fission half life of 4.8 x 10 to the 10th power years. Neutrons associated with this spontaneous fission are emitted at a rate of 28,000 neutrons per second per gram. Since the space fuel form of plutonium 238 is the oxide pressed into a cermet with molybdenum, a contribution to the neutron emission rate arises from (alpha, n) reactions with 0-17 and 0-18 which occur in natural oxygen.

Evaluating ligands for use in polymer ligand film (PLF) for plutonium and uranium extraction

DOE PAGES

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

METHOD OF FORMING PLUTONIUM-BEARING CARRIER PRECIPITATES AND WASHING SAME

DOEpatents

Faris, B.F.

1959-02-24

An improvement of the lanthanum fluoride carrier precipitation process for the recovery of plutonium is presented. In this process the plutonium is first segregated in the LaF/su precipitate and this precipitate is later dissolved and the plutonium reprecipitated as the peroxide. It has been found that the loss of plutonium by its remaining in the supernatant liquid associated with the peroxide precipitate is greatly reduced if, before dissolution, the LaF/ sub 3/ precipitate is subjected to a novel washing step which constitutes the improvement of this patent. The step consists in intimately contactifng the LaF/ sub 3/ precipitate with a 4 to 10 percent solution of sodium hydrogen sulfate at a temperature between 10 and 95 deg C for 1/2 to 3 hours.

Plutonium dissolution process

DOEpatents

Vest, Michael A.; Fink, Samuel D.; Karraker, David G.; Moore, Edwin N.; Holcomb, H. Perry

1996-01-01

A two-step process for dissolving plutonium metal, which two steps can be carried out sequentially or simultaneously. Plutonium metal is exposed to a first mixture containing approximately 1.0M-1.67M sulfamic acid and 0.0025M-0.1M fluoride, the mixture having been heated to a temperature between 45.degree. C. and 70.degree. C. The mixture will dissolve a first portion of the plutonium metal but leave a portion of the plutonium in an oxide residue. Then, a mineral acid and additional fluoride are added to dissolve the residue. Alteratively, nitric acid in a concentration between approximately 0.05M and 0.067M is added to the first mixture to dissolve the residue as it is produced. Hydrogen released during the dissolution process is diluted with nitrogen.

Structures of plutonium coordination compounds: A review of past work, recent single crystal x-ray diffraction results, and what we're learning about plutonium coordination chemistry

NASA Astrophysics Data System (ADS)

Neu, M. P.; Matonic, J. H.; Smith, D. M.; Scott, B. L.

2000-07-01

The compounds we have isolated and characterized include plutonium(III) and plutonium(IV) bound by ligands with a range of donor types and denticity (halide, phosphine oxide, hydroxamate, amine, sulfide) in a variety of coordination geometries. For example, we have obtained the first X-ray structure of Pu(III) complexed by a soft donor ligand. Using a "one pot" synthesis beginning with Pu metal strips and iodine in acetonitrile and adding trithiacyclononane we isolated the complex, PuI3(9S3)(MeCN)2 (Figure 1). On the other end of the coordination chemistry spectrum, we have obtained the first single crystal structure of the Pu(IV) hexachloro anion (Figure 2). Although this species has been used in plutonium purification via anion exchange chromatography for decades, the bond distances and exact structure were not known. We have also characterized the first plutonium-biomolecule complex, Pu(IV) bound by the siderophore desferrioxamine E.In this presentation we will review the preparation, structures, and importance of previously known coordination compounds and of those we have recently isolated. We will show the coordination chemistry of plutonium is rich and varied, well worth additional exploration.

Radiation damage and annealing in plutonium tetrafluoride

DOE PAGES

McCoy, Kaylyn; Casella, Amanda; Sinkov, Sergey; ...

2017-08-03

A sample of plutonium tetrafluoride that was separated prior to 1966 at the Hanford Site in Washington State was analyzed at the Pacific Northwest National Laboratory (PNNL) in 2015 and 2016. The plutonium tetrafluoride, as received, was an unusual color and considering the age of the plutonium, there were questions about the condition of the material. These questions had to be answered in order to determine the suitability of the material for future use or long-term storage. Therefore, thermogravimetric/differential thermal analysis and X-ray diffraction evaluations were conducted to determine the plutonium's crystal structure, oxide content, and moisture content; these analysesmore » reported that the plutonium was predominately amorphous and tetrafluoride, with an oxide content near ten percent. Freshly fluorinated plutonium tetrafluoride is known to be monoclinic. And during the initial thermogravimetric/differential thermal analyses, it was discovered that an exothermic event occurred within the material near 414 °C. X-ray diffraction analyses were conducted on the annealed tetrafluoride. The X-ray diffraction analyses indicated that some degree of recrystallization occurred in conjunction with the 414 °C event. This commentary describes the series of thermogravimetric/differential thermal and X-ray diffraction analyses that were conducted as part of this investigation at PNNL.« less

Radiological analysis of plutonium glass batches with natural/enriched boron

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rainisch, R.

2000-06-22

The disposition of surplus plutonium inventories by the US Department of Energy (DOE) includes the immobilization of certain plutonium materials in a borosilicate glass matrix, also referred to as vitrification. This paper addresses source terms of plutonium masses immobilized in a borosilicate glass matrix where the glass components include both natural boron and enriched boron. The calculated source terms pertain to neutron and gamma source strength (particles per second), and source spectrum changes. The calculated source terms corresponding to natural boron and enriched boron are compared to determine the benefits (decrease in radiation source terms) for to the use ofmore » enriched boron. The analysis of plutonium glass source terms shows that a large component of the neutron source terms is due to (a, n) reactions. The Americium-241 and plutonium present in the glass emit alpha particles (a). These alpha particles interact with low-Z nuclides like B-11, B-10, and O-17 in the glass to produce neutrons. The low-Z nuclides are referred to as target particles. The reference glass contains 9.4 wt percent B{sub 2}O{sub 3}. Boron-11 was found to strongly support the (a, n) reactions in the glass matrix. B-11 has a natural abundance of over 80 percent. The (a, n) reaction rates for B-10 are lower than for B-11 and the analysis shows that the plutonium glass neutron source terms can be reduced by artificially enriching natural boron with B-10. The natural abundance of B-10 is 19.9 percent. Boron enriched to 96-wt percent B-10 or above can be obtained commercially. Since lower source terms imply lower dose rates to radiation workers handling the plutonium glass materials, it is important to know the achievable decrease in source terms as a result of boron enrichment. Plutonium materials are normally handled in glove boxes with shielded glass windows and the work entails both extremity and whole-body exposures. Lowering the source terms of the plutonium batches will make the handling of these materials less difficult and will reduce radiation exposure to operating workers.« less

Neutronics calculations on the impact of burnable poisons to safety and non-proliferation aspects of inert matrix fuel

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.

Comparisons of the skeletal locations of putative plutonium-induced osteosarcomas in humans with those in beagle dogs and with naturally occurring tumors in both species.

PubMed

Miller, Scott C; Lloyd, Ray D; Bruenger, Fred W; Krahenbuhl, Melinda P; Polig, Erich; Romanov, Sergey A

2003-11-01

Osteosarcomas occur from exposures to bone-seeking, alpha-particle-emitting isotopes, particularly plutonium. The skeletal distribution of putative 239Pu-induced osteosarcomas reported in Mayak Metallurgical and Radiochemical Plutonium Plant workers is compared with those observed in canine studies, and these are compared with distributions of naturally occurring osteosarcomas in both species. In the Mayak workers, 29% and 71% of the osteosarcomas were in the peripheral and central skeleton, respectively, with the spine having the most tumors (36%). An almost identical distribution of plutonium-induced osteosarcomas was reported for dogs injected with 239Pu as young adults. This distribution of osteosarcomas is quite different from the distributions of naturally occurring osteosarcomas for both species. In the Cooperative Osteosarcoma Study Group in humans (1,736 osteosarcomas from all ages), over 91% of the tumors occurred in the peripheral skeleton. In the Mayo Clinic group of older individuals (>40 years old), over 60% of the osteosarcomas appeared in the peripheral skeleton. The distribution of naturally occurring osteosarcomas in the canine is similar to that in the adult human. The similarities of the distributions of plutonium-associated osteosarcomas in the Mayak workers with those found in experimental studies suggest that many of the reported osteosarcomas may have been associated with plutonium exposures. These results also support the experimental paradigm that plutonium osteosarcomas have a preference for well vascularized cancellous bone sites. These sites have a greater initial deposition of plutonium, but also greater turnover due to elevated bone remodeling rates.

Study on Characteristic of Temperature Coefficient of Reactivity for Plutonium Core of Pebbled Bed Reactor

NASA Astrophysics Data System (ADS)

Zuhair; Suwoto; Setiadipura, T.; Bakhri, S.; Sunaryo, G. R.

2018-02-01

As a part of the solution searching for possibility to control the plutonium, a current effort is focused on mechanisms to maximize consumption of plutonium. Plutonium core solution is a unique case in the high temperature reactor which is intended to reduce the accumulation of plutonium. However, the safety performance of the plutonium core which tends to produce a positive temperature coefficient of reactivity should be examined. The pebble bed inherent safety features which are characterized by a negative temperature coefficient of reactivity must be maintained under any circumstances. The purpose of this study is to investigate the characteristic of temperature coefficient of reactivity for plutonium core of pebble bed reactor. A series of calculations with plutonium loading varied from 0.5 g to 1.5 g per fuel pebble were performed by the MCNPX code and ENDF/B-VII library. The calculation results show that the k eff curve of 0.5 g Pu/pebble declines sharply with the increase in fuel burnup while the greater Pu loading per pebble yields k eff curve declines slighter. The fuel with high Pu content per pebble may reach long burnup cycle. From the temperature coefficient point of view, it is concluded that the reactor containing 0.5 g-1.25 g Pu/pebble at high burnup has less favorable safety features if it is operated at high temperature. The use of fuel with Pu content of 1.5 g/pebble at high burnup should be considered carefully from core safety aspect because it could affect transient behavior into a fatal accident situation.

PLUTONIUM-CERIUM-COPPER ALLOYS

DOEpatents

Coffinberry, A.S.

1959-05-12

A low melting point plutonium alloy useful as fuel is a homogeneous liquid metal fueled nuclear reactor is described. Vessels of tungsten or tantalum are useful to contain the alloy which consists essentially of from 10 to 30 atomic per cent copper and the balance plutonium and cerium. with the plutontum not in excess of 50 atomic per cent.

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2012 CFR

2012-01-01

... 10 Energy 2 2012-01-01 2012-01-01 false Air transport of plutonium. 71.88 Section 71.88 Energy... Controls and Procedures § 71.88 Air transport of plutonium. (a) Notwithstanding the provisions of any..., whether for import, export, or domestic shipment, is not transported by air or delivered to a carrier for...

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2014 CFR

2014-01-01

... 10 Energy 2 2014-01-01 2014-01-01 false Air transport of plutonium. 71.88 Section 71.88 Energy... Controls and Procedures § 71.88 Air transport of plutonium. (a) Notwithstanding the provisions of any..., whether for import, export, or domestic shipment, is not transported by air or delivered to a carrier for...

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2013 CFR

2013-01-01

... 10 Energy 2 2013-01-01 2013-01-01 false Air transport of plutonium. 71.88 Section 71.88 Energy... Controls and Procedures § 71.88 Air transport of plutonium. (a) Notwithstanding the provisions of any..., whether for import, export, or domestic shipment, is not transported by air or delivered to a carrier for...

11. SIDE VIEW OF INSTALLATION OF A CONTINUOUS ROTARYTUBE HYDROFLUORINATOR ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

11. SIDE VIEW OF INSTALLATION OF A CONTINUOUS ROTARY-TUBE HYDROFLUORINATOR LOCATED IN ROOM 146. THE HYDROFLUORINATOR IS BEING INSTALLED INSIDE A GLOVE BOX. HYDROFLUORINATION CONVERTED PLUTONIUM OXIDE TO PLUTONIUM TETRAFLUORIDE. (1/11/62) - Rocky Flats Plant, Plutonium Recovery & Fabrication Facility, North-central section of plant, Golden, Jefferson County, CO

10. VIEW OF CALCINER IN ROOM 146148. THE CALCINER HEATED ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

10. VIEW OF CALCINER IN ROOM 146-148. THE CALCINER HEATED PLUTONIUM PEROXIDE TO CONVERT IT TO PLUTONIUM OXIDE. THE PROCESS REMOVED RESIDUAL WATER AND NITRIC ACID LEAVING A DRY, POWDERED PRODUCT. (4/29/65) - Rocky Flats Plant, Plutonium Recovery & Fabrication Facility, North-central section of plant, Golden, Jefferson County, CO

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2010 CFR

2010-01-01

... 10 Energy 2 2010-01-01 2010-01-01 false Air transport of plutonium. 71.88 Section 71.88 Energy... Controls and Procedures § 71.88 Air transport of plutonium. (a) Notwithstanding the provisions of any..., whether for import, export, or domestic shipment, is not transported by air or delivered to a carrier for...

Removal of plutonium and americium from alkaline waste solutions

DOEpatents

Schulz, Wallace W.

1979-01-01

High salt content, alkaline waste solutions containing plutonium and americium are contacted with a sodium titanate compound to effect removal of the plutonium and americium from the alkaline waste solution onto the sodium titanate and provide an effluent having a radiation level of less than 10 nCi per gram alpha emitters.

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2011 CFR

2011-01-01

... 10 Energy 2 2011-01-01 2011-01-01 false Air transport of plutonium. 71.88 Section 71.88 Energy... Controls and Procedures § 71.88 Air transport of plutonium. (a) Notwithstanding the provisions of any..., whether for import, export, or domestic shipment, is not transported by air or delivered to a carrier for...

SEPARATION OF FISSION PRODUCT VALUES FROM THE HEXAVALENT PLUTONIUM BY CARRIER PRECIPITATION

DOEpatents

Davies, T.H.

1959-12-15

An improved precipitation of fission products on bismuth phosphate from an aqueous mineral acid solution also containing hexavalent plutonium by incorporating, prior to bismuth phosphate precipitation, from 0.05 to 2.5 grams/ liter of zirconium phosphate, niobium oxide. and/or lanthanum fluoride is described. The plutonium remains in solution.

Enhanced ionization efficiency in TIMS analyses of plutonium and americium using porous ion emitters

DOE PAGES

Baruzzini, Matthew L.; Hall, Howard L.; Watrous, Matthew G.; ...

2016-12-05

Investigations of enhanced sample utilization in thermal ionization mass spectrometry (TIMS) using porous ion emitter (PIE) techniques for the analyses of trace quantities of americium and plutonium were performed. Repeat ionization efficiency (i.e., the ratio of ions detected to atoms loaded on the filament) measurements were conducted on sample sizes ranging from 10–100 pg for americium and 1–100 pg for plutonium using PIE and traditional (i.e., a single, zone-refined rhenium, flat filament ribbon with a carbon ionization enhancer) TIMS filament sources. When compared to traditional filaments, PIEs exhibited an average boost in ionization efficiency of ~550% for plutonium and ~1100%more » for americium. A maximum average efficiency of 1.09% was observed at a 1 pg plutonium sample loading using PIEs. Supplementary trials were conducted using newly developed platinum PIEs to analyze 10 pg mass loadings of plutonium. As a result, platinum PIEs exhibited an additional ~134% boost in ion yield over standard PIEs and ~736% over traditional filaments at the same sample loading level.« less

Design, installation, and performance of a multi-layered permeable reactive barrier, Los Alamos National Laboratory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kaszuba, J. P.; Longmire, P. A.; Strietelmeier, E. A.

2004-01-01

A multi-layered permeable reactive barrier (PRB) has been installed in Mortandad Canyon, on the Pajarito Plateau in the north-central part of LANL, to demonstrate in-situ treatment of a suite of contaminants with dissimilar geochemical properties. The PRB will also mitigate possible vulnerabilities from downgradient contaminant movement within alluvial and deeper perched groundwater. Mortandad Canyon was selected as the location for this demonstration project because the flow of alluvial groundwater is constrained by the geology of the canyon, a large network of monitoring wells already were installed along the canyon reach, and the hydrochemistry and contaminant history of the canyon ismore » well-documented. The PRB uses a funnel-and-gate system with a series of four reactive media cells to immobilize or destroy contaminants present in alluvial groundwater, including strontium-90, plutonium-238,239,240, americium-241, perchlorate, and nitrate. The four cells, ordered by sequence of contact with the groundwater, consist of gravel-sized scoria (for colloid removal); phosphate rock containing apatite (for metals and radionuclides); pecan shells and cotton seed admixed with gravel (bio-barrier, to deplete dissolved oxygen and destroy potential RCRA organic compounds, nitrate and perchlorate); and limestone (pH buffering and anion adsorption). Design elements of the PRB are based on laboratory-scale treatability studies and on a field investigation of hydrologic, geochemical, and geotechnical parameters. The PRB was designed with the following criteria: 1-day residence time within the biobarrier, 10-year lifetime, minimization of surface water infiltration and erosion, optimization of hydraulic capture, and minimization of excavated material requiring disposal. Each layer has been equipped with monitoring wells or ports to allow sampling of groundwater and reactive media, and monitor wells are located immediately adjacent to the up- and down-gradient perimeter of the engineered structure. Groundwater sampling upgradient, within, and downgradient of the PRB took place from May through August 2003. Concentrations of strontium-90 have diminished by 80% and 40% within the central portion of the phosphate rock (apatite) and bio-barrier cells, respectively. Higher concentrations of this radionuclide occur in groundwater near the north and south perimeters of the two cells. The non-uniform distribution of strontium-90 may result from varying residence time and saturated thickness of pore water. Initial concentrations of nitrate (8-12 parts per million or ppm as nitrate) and perchlorate (0.035 ppm) have been reduced in the phosphate rock and bio-barrier cells to concentrations that are less than method detection limits (0.01 and 0.002 ppm, respectively). Initial microbial analyses suggest the presence of both dissimilatory perchlorate- and nitrate-reducing bacterial populations, along with production of acetate and propionate, and decreasing dissolved oxygen and pH. The dominant group of perchlorate reducers consists of members of the previously described Dechloromonas genus, in the beta subclass of the Proteobacteria, which together with the Dechlorosoma genus are considered to be the dominant genera in circum-neutral mesophilic environments. Groundwater flow through the multiple PRB is taking place at a very slow rate based on similar concentrations of nitrate, perchlorate, chlorate, and chlorite in the upgradient well MCO-4B and downgradient well MCO-5. Concentrations of these constituents also increase within the limestone cell. Decreased precipitation due to extreme drought is probably responsible for decreasing saturated thickness within both the alluvium and PRB, resulting in stagnant conditions. Varying distributions of ammonium, nitrate, sulfate, iron, and manganese within the phosphate rock, bio-barrier, and limestone cells also support this hypothesis.« less

Mortality among workers with chronic radiation sickness

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shilnikova, N.S.; Koshurnikova, N.A.; Bolotnikova, M.G.

1996-07-01

This study is based on a registry containing medical and dosimetric data of the employees who began working at different plants of the Mayak nuclear complex between 1948 and 1958 who developed chronic radiation sickness. Mayak is the first nuclear weapons plutonium production enterprise built in Russia and includes nuclear reactors, a radiochemical plant for plutonium separation, and a plutonium production enterprise built in Russia and includes nuclear reactors, a radiochemical plant for plutonium separation, and a plutonium production plant.Workers whose employment began between 1948 and 1958 exhibited a 6-28% incidence of chronic radiation sickness at the different facilities. Theremore » were no cases of chronic radiation sickness among those who began working after 1958. Data on doses of external whole-body gamma-irradiation and mortality in workers with chronic radiation sickness are presented. 6 refs., 5 tabs.« less

Real-time monitoring of plutonium content in uranium-plutonium alloys

DOEpatents

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 segregation in glassy aerodynamic fallout from a nuclear weapon test

DOE PAGES

Holliday, K. S.; Dierken, J. M.; Monroe, M. L.; ...

2017-01-11

Our study combines electron microscopy equipped with energy dispersive spectroscopy to probe major element composition and autoradiography to map plutonium in order to examine the spatial relationships between plutonium and fallout composition in aerodynamic glassy fallout from a nuclear weapon test. We interrogated a sample set of 48 individual fallout specimens in order to reveal that the significant chemical heterogeneity of this sample set could be described compositionally with a relatively small number of compositional endmembers. Furthermore, high concentrations of plutonium were never associated with several endmember compositions and concentrated with the so-called mafic glass endmember. Our result suggests thatmore » it is the physical characteristics of the compositional endmembers and not the chemical characteristics of the individual component elements that govern the un-burnt plutonium distribution with respect to major element composition in fallout.« less

Assessment of plutonium in the Savannah River Site environment. Revision 1

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carlton, W.H.; Evans, A.G.; Geary, L.A.

1992-12-31

Plutonium in the Savannah River Site Environment is published as a part of the Radiological Assessment Program (RAP). It is the fifth in a series of eight documents on individual radioisotopes released to the environment as a result of Savannah River Site (SRS) operations. These are living documents, each to be revised and updated on a two-year schedule. This document describes the sources of plutonium in the environment, its release from SRS, environmental transport and ecological concentration of plutonium, and the radiological impact of SRS releases to the environment. Plutonium exists in the environment as a result of above-ground nuclearmore » weapons tests, the Chernobyl accident, the destruction of satellite SNAP 9-A, plane crashes involving nuclear weapons, and small releases from reactors and reprocessing plants. Plutonium has been produced at SRS during the operation of five production reactors and released in small quantities during the processing of fuel and targets in chemical separations facilities. Approximately 0.6 Ci of plutonium was released into streams and about 12 Ci was released to seepage basins, where it was tightly bound by clay in the soil. A smaller quantity, about 3.8 Ci, was released to the atmosphere. Virtually all releases have occurred in F- and H-Area separation facilities. Plutonium concentration and transport mechanisms for the atmosphere, surface water, and ground water releases have been extensively studied by Savannah River Technology Center (SRTC) and ecological mechanisms have been studied by Savannah River Ecology Laboratory (SREL). The overall radiological impact of SRS releases to the offsite maximum individual can be characterized by a total dose of 15 mrem (atmospheric) and 0.18 mrem (liquid), compared with the dose of 12,960 mrem from non-SRS sources during the same period of time (1954--1989). Plutonium releases from SRS facilities have resulted in a negligible impact to the environment and the population it supports.« less

Plutonium Oxidation State Distribution under Aerobic and Anaerobic Subsurface Conditions for Metal-Reducing Bacteria

NASA Astrophysics Data System (ADS)

Reed, D. T.; Swanson, J.; Khaing, H.; Deo, R.; Rittmann, B.

2009-12-01

The fate and potential mobility of plutonium in the subsurface is receiving increased attention as the DOE looks to cleanup the many legacy nuclear waste sites and associated subsurface contamination. Plutonium is the near-surface contaminant of concern at several DOE sites and continues to be the contaminant of concern for the permanent disposal of nuclear waste. The mobility of plutonium is highly dependent on its redox distribution at its contamination source and along its 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. The redox distribution of plutonium in the presence of facultative metal reducing bacteria (specifically Shewanella and Geobacter species) was established in a concurrent experimental and modeling study under aerobic and anaerobic conditions. Pu(VI), although relatively soluble under oxidizing conditions at near-neutral pH, does not persist under a wide range of the oxic and anoxic conditions investigated in microbiologically active systems. Pu(V) complexes, which exhibit high chemical toxicity towards microorganisms, are relatively stable under oxic conditions but are reduced by metal reducing bacteria under anaerobic conditions. These facultative metal-reducing bacteria led to the rapid reduction of higher valent plutonium to form Pu(III/IV) species depending on nature of the starting plutonium species and chelating agents present in solution. Redox cycling of these lower oxidation states is likely a critical step in the formation of pseudo colloids that may lead to long-range subsurface transport. The CCBATCH biogeochemical model is used to explain the redox mechanisms and final speciation of the plutonium oxidation state distributions observed. These results for microbiologically active systems are interpreted in the context of their importance in defining the overall migration of plutonium in the subsurface.

Estimation of Plutonium-240 Mass in Waste Tanks Using Ultra-Sensitive Detection of Radioactive Xenon Isotopes from Spontaneous Fission

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bowyer, Theodore W.; Gesh, Christopher J.; Haas, Daniel A.

This report details efforts to develop a technique which is able to detect and quantify the mass of 240Pu in waste storage tanks and other enclosed spaces. If the isotopic ratios of the plutonium contained in the enclosed space is also known, then this technique is capable of estimating the total mass of the plutonium without physical sample retrieval and radiochemical analysis of hazardous material. Results utilizing this technique are reported for a Hanford Site waste tank (TX-118) and a well-characterized plutonium sample in a laboratory environment.

PLUTONIUM ELECTROREFINING CELLS

DOEpatents

Mullins, L.J. Jr.; Leary, J.A.; Bjorklund, C.W.; Maraman, W.J.

1963-07-16

Electrorefining cells for obtaining 99.98% plutonium are described. The cells consist of an impure liquid plutonium anode, a molten PuCl/sub 3/-- alkali or alkaline earth metal chloanode, a molten PuCl/sub 3/-alkali or alkaline earth metal chloride electrolyte, and a nonreactive cathode, all being contained in nonreactive ceramic containers which separate anode from cathode by a short distance and define a gap for the collection of the purified liquid plutonium deposited on the cathode. Important features of these cells are the addition of stirrer blades on the anode lead and a large cathode surface to insure a low current density. (AEC)

Development of first ever scanning probe microscopy capabilities for plutonium

NASA Astrophysics Data System (ADS)

Beaux, Miles F.; Cordoba, Miguel Santiago; Zocco, Adam T.; Vodnik, Douglas R.; Ramos, Michael; Richmond, Scott; Moore, David P.; Venhaus, Thomas J.; Joyce, Stephen A.; Usov, Igor O.

2017-04-01

Scanning probe microscopy capabilities have been developed for plutonium and its derivative compounds. Specifically, a scanning tunneling microscope and an atomic force microscope housed in an ultra-high vacuum system and an inert atmosphere glove box, respectively, were prepared for the introduction of small non-dispersible δ-Pu coupons. Experimental details, procedures, and preliminary imaging of δ-Pu coupons are presented to demonstrate the functionality of these new capabilities. These first of a kind capabilities for plutonium represent a significant step forward in the ability to characterize and understand plutonium surfaces with high spatial resolution.

Development of first ever scanning probe microscopy capabilities for plutonium

DOE PAGES

Beaux, Miles F.; Cordoba, Miguel Santiago; Zocco, Adam T.; ...

2017-04-01

Scanning probe microscopy capabilities have been developed for plutonium and its derivative compounds. Specifically, a scanning tunneling microscope and an atomic force microscope housed in an ultra-high vacuum system and an inert atmosphere glove box, respectively, were prepared for the introduction of small non-dispersible δ-Pu coupons. Experimental details, procedures, and preliminary imaging of δ-Pu coupons are presented to demonstrate the functionality of these new capabilities. In conclusion, these first of a kind capabilities for plutonium represent a significant step forward in the ability to characterize and understand plutonium surfaces with high spatial resolution.

Ecotoxicity literature review of selected Hanford Site contaminants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Driver, C.J.

1994-03-01

Available information on the toxicity, food chain transport, and bioconcentration of several Hanford Site contaminants were reviewed. The contaminants included cesium-137, cobalt-60, europium, nitrate, plutonium, strontium-90, technetium, tritium, uranium, and chromium (III and VI). Toxicity and mobility in both aquatic and terrestrial systems were considered. For aquatic systems, considerable information was available on the chemical and/or radiological toxicity of most of the contaminants in invertebrate animals and fish. Little information was available on aquatic macrophyte response to the contaminants. Terrestrial animals such as waterfowl and amphibians that have high exposure potential in aquatic systems were also largely unrepresented in themore » toxicity literature. The preponderance of toxicity data for terrestrial biota was for laboratory mammals. Bioconcentration factors and transfer coefficients were obtained for primary producers and consumers in representative aquatic and terrestrial systems; however, little data were available for upper trophic level transfer, particularly for terrestrial predators. Food chain transport and toxicity information for the contaminants were generally lacking for desert or sage brush-steppe organisms, particularly plants and reptiles« less

URANOUS IODATE AS A CARRIER FOR PLUTONIUM

DOEpatents

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.

PLUTONIUM-URANIUM-TITANIUM ALLOYS

DOEpatents

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.

Radioisotope contaminations from releases of the Tomsk-Seversk nuclear facility (Siberia, Russia).

PubMed

Gauthier-Lafaye, F; Pourcelot, L; Eikenberg, J; Beer, H; Le Roux, G; Rhikvanov, L P; Stille, P; Renaud, Ph; Mezhibor, A

2008-04-01

Soils have been sampled in the vicinity of the Tomsk-Seversk facility (Siberia, Russia) that allows us to measure radioactive contaminations due to atmospheric and aquatic releases. Indeed soils exhibit large inventories of man-made fission products including 137Cs (ranging from 33,000 to 68,500 Bq m(-2)) and actinides such as plutonium (i.e. 239+240Pu from 420 to 5900 Bq m(-2)) or 241Am (160-1220 Bq m(-2)). Among all sampling sites, the bank of the Romashka channel exhibits the highest radioisotope concentrations. At this site, some short half-life gamma emitters were detected as well indicating recent aquatic discharge in the channel. In comparison, soils that underwent atmospheric depositions like peat and forest soils exhibit lower activities of actinides and 137Cs. Soil activities are too high to be related solely to global fallout and thus the source of plutonium must be discharges from the Siberian Chemical Combine (SCC) plant. This is confirmed by plutonium isotopic ratios measured by ICP-MS; the low 241Pu/239Pu and 240Pu/239Pu atomic ratios with respect to global fallout ratio or civil nuclear fuel are consistent with weapons grade signatures. Up to now, the influence of Tomsk-Seversk plutonium discharges was speculated in the Ob River and its estuary. Isotopic data from the present study show that plutonium measured in SCC probably constitutes a significant source of plutonium in the aquatic environment, together with plutonium from global fallout and other contaminated sites including Tomsk, Mayak (Russia) and Semipalatinsk (Republic of Kazakhstan). It is estimated that the proportion of plutonium from SCC source can reach 45% for 239Pu and 60% for 241Pu in the sediments.

High-Temperature Oxidation of Plutonium Surrogate Metals and Alloys

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sparks, Joshua C.; Krantz, Kelsie E.; Christian, Jonathan H.

The Plutonium Management and Disposition Agreement (PMDA) is a nuclear non-proliferation agreement designed to remove 34 tons of weapons-grade plutonium from Russia and the United States. While several removal options have been proposed since the agreement was first signed in 2000, processing the weapons-grade plutonium to mixed-oxide (MOX) fuel has remained the leading candidate for achieving the goals of the PMDA. However, the MOX program has received its share of criticisms, which causes its future to be uncertain. One alternative pathway for plutonium disposition would involve oxidizing the metal followed by impurity down blending and burial in the Waste Isolationmore » Pilot Plant (WIPP) in Carlsbad, New Mexico. This pathway was investigated by use of a hybrid microwave and a muffle furnace with Fe and Al as surrogate materials. Oxidation occurred similarly in the microwave and muffle furnace; however, the microwave process time was significantly faster.« less

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

TERNARY ALLOY-CONTAINING PLUTONIUM

DOEpatents

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.

Microprobe Analysis of Pu-Ga Standards

DOE PAGES

Wall, Angélique D.; Romero, Joseph P.; Schwartz, Daniel

2017-08-04

In order to obtain quantitative analysis using an Electron Scanning Microprobe it is essential to have a standard of known composition. Most elemental and multi-elemental standards can be easily obtained from places like Elemental Scientific or other standards organizations that are NIST (National Institute of Standards and Technology) traceable. It is, however, more challenging to find standards for plutonium. Past work performed in our group has typically involved using the plutonium sample to be analysed as its own standard as long as all other known components of the sample have standards to be compared to [1,2,3]. Finally, this method worksmore » well enough, but this experiment was performed in order to develop a more reliable standard for plutonium using five samples of known chemistry of a plutonium gallium mix that could then be used as the main plutonium and gallium standards for future experiments.« less

Microprobe Analysis of Pu-Ga Standards

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wall, Angélique D.; Romero, Joseph P.; Schwartz, Daniel

In order to obtain quantitative analysis using an Electron Scanning Microprobe it is essential to have a standard of known composition. Most elemental and multi-elemental standards can be easily obtained from places like Elemental Scientific or other standards organizations that are NIST (National Institute of Standards and Technology) traceable. It is, however, more challenging to find standards for plutonium. Past work performed in our group has typically involved using the plutonium sample to be analysed as its own standard as long as all other known components of the sample have standards to be compared to [1,2,3]. Finally, this method worksmore » well enough, but this experiment was performed in order to develop a more reliable standard for plutonium using five samples of known chemistry of a plutonium gallium mix that could then be used as the main plutonium and gallium standards for future experiments.« less

GEOPHYSICS AND SITE CHARACTERIZATION AT THE HANFORD SITE THE SUCCESSFUL USE OF ELECTRICAL RESISTIVITY TO POSITION BOREHOLES TO DEFINE DEEP VADOSE ZONE CONTAMINATION - 11509

DOE Office of Scientific and Technical Information (OSTI.GOV)

GANDER MJ; LEARY KD; LEVITT MT

2011-01-14

Historic boreholes confirmed the presence of nitrate and radionuclide contaminants at various intervals throughout a more than 60 m (200 ft) thick vadose zone, and a 2010 electrical resistivity survey mapped the known contamination and indicated areas of similar contaminants, both laterally and at depth; therefore, electrical resistivity mapping can be used to more accurately locate characterization boreholes. At the Hanford Nuclear Reservation in eastern Washington, production of uranium and plutonium resulted in the planned release of large quantities of contaminated wastewater to unlined excavations (cribs). From 1952 until 1960, the 216-U-8 Crib received approximately 379,000,000 L (100,000,000 gal) ofmore » wastewater containing 25,500 kg (56,218 lb) uranium; 1,029,000 kg (1,013 tons) of nitrate; 2.7 Ci of technetium-99; and other fission products including strontium-90 and cesium-137. The 216-U-8 Crib reportedly holds the largest inventory of waste uranium of any crib on the Hanford Site. Electrical resistivity is a geophysical technique capable of identifying contrasting physical properties; specifically, electrically conductive material, relative to resistive native soil, can be mapped in the subsurface. At the 216-U-8 Crib, high nitrate concentrations (from the release of nitric acid [HNO{sub 3}] and associated uranium and other fission products) were detected in 1994 and 2004 boreholes at various depths, such as at the base of the Crib at 9 m (30 ft) below ground surface (bgs) and sporadically to depths in excess of 60 m (200 ft) bgs. These contaminant concentrations were directly correlative with the presence of observed low electrical resistivity responses delineated during the summer 2010 geophysical survey. Based on this correlation and the recently completed mapping of the electrically conductive material, additional boreholes are planned for early 2011 to identify nitrate and radionuclide contamination: (a) throughout the entire vertical length of the vadose zone (i.e., 79 m [260 ft] bgs) within the footprint of the Crib, and (b) 15 to 30 m (50 to 100 ft) east of the Crib footprint, where contaminants are inferred to have migrated through relatively permeable soils. Confirmation of the presence of contamination in historic boreholes correlates well with mapping from the 2010 survey, and serves as a basis to site future characterization boreholes that will likely intersect contamination both laterally and at depth.« less

PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINATING ELEMENTS

DOEpatents

Duffield, R.B.

1959-02-24

S>A method is described for separating plutonium, in a valence state of less than five, from an aqueous solution in which it is dissolved. The niethod consists in adding potassium and sulfate ions to such a solution while maintaining the solution at a pH of less than 7.1, and isolating the precipitate of potassium plutonium sulfate thus formed.

Density of Plutonium Turnings Generated from Machining Activities

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gonzales, John Robert; Vigil, Duane M.; Jachimowski, Thomas A.

The purpose of this project was to determine the density of plutonium (Pu) turnings generated from the range of machining activities, using both surrogate material and machined Pu turnings. Verify that 500 grams (g) of plutonium will fit in a one quart container using a surrogate equivalent volume and that 100 grams of Pu will fit in a one quart Savy container.

Airborne plutonium-239 and americium-241 concentrations measured from the 125-meter Hanford Meteorological Tower

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sehmel, G.A.

1978-01-01

Airborne plutonium-239 and americium-241 concentrations and fluxes were measured at six heights from 1.9 to 122 m on the Hanford meteorological tower. The data show that plutonium-239 was transported on nonrespirable and small particles at all heights. Airborne americium-241 concentrations on small particles were maximum at the 91 m height.

PLUTONIUM RECOVERY FROM NEUTRON-BOMBARDED URANIUM FUEL

DOEpatents

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

DOEpatents

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.

Integrated approaches for reducing sample size for measurements of trace elemental impurities in plutonium by ICP-OES and ICP-MS

DOE PAGES

Xu, Ning; Chamberlin, Rebecca M.; Thompson, Pam; ...

2017-10-07

This study has demonstrated that bulk plutonium chemical analysis can be performed at small scales (\\50 mg material) through three case studies. Analytical methods were developed for ICP-OES and ICP-MS instruments to measure trace impurities and gallium content in plutonium metals with comparable or improved detection limits, measurement accuracy and precision. In two case studies, the sample size has been reduced by 109, and in the third case study, by as much as 50009, so that the plutonium chemical analysis can be performed in a facility rated for lower-hazard and lower-security operations.

METHOD AND MEANS FOR ELECTROLYTIC PURIFICATION OF PLUTONIUM

DOEpatents

Bjorklund, C.W.; Benz, R.; Maraman, W.J.; Leary, J.A.; Walsh, K.A.

1960-02-01

The technique of electrodepositing pure plutonium from a fused salt electrolyte of PuCl/sub 3/ and aixati metal halides is described. When an iron cathode is used, the plutonium deposit alloys therewith in the liquid state at the 400 to 600 deg C operating temperature, such liquid being allowed to drip through holes in the cathode and collect in a massive state in a tantallum cup. The process is adaptable to continuous processing by the use of depleted plutonium fuel as the anode: good to excellent separation from fission products is obtained with a Pu--Fe "fission" anode containing representative fractions of Ce, Ru, Zr, La, Mo, and Nb.

Integrated approaches for reducing sample size for measurements of trace elemental impurities in plutonium by ICP-OES and ICP-MS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, Ning; Chamberlin, Rebecca M.; Thompson, Pam

This study has demonstrated that bulk plutonium chemical analysis can be performed at small scales (\\50 mg material) through three case studies. Analytical methods were developed for ICP-OES and ICP-MS instruments to measure trace impurities and gallium content in plutonium metals with comparable or improved detection limits, measurement accuracy and precision. In two case studies, the sample size has been reduced by 109, and in the third case study, by as much as 50009, so that the plutonium chemical analysis can be performed in a facility rated for lower-hazard and lower-security operations.

PROCESSING OF NEUTRON-IRRADIATED URANIUM

DOEpatents

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.

Selecting a plutonium vitrification process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jouan, A.

1996-05-01

Vitrification of plutonium is one means of mitigating its potential danger. This option is technically feasible, even if it is not the solution advocated in France. Two situations are possible, depending on whether or not the glass matrix also contains fission products; concentrations of up to 15% should be achievable for plutonium alone, whereas the upper limit is 3% in the presence of fission products. The French continuous vitrification process appears to be particularly suitable for plutonium vitrification: its capacity is compatible with the required throughout, and the compact dimensions of the process equipment prevent a criticality hazard. Preprocessing ofmore » plutonium metal, to convert it to PuO{sub 2} or to a nitric acid solution, may prove advantageous or even necessary depending on whether a dry or wet process is adopted. The process may involve a single step (vitrification of Pu or PuO{sub 2} mixed with glass frit) or may include a prior calcination step - notably if the plutonium is to be incorporated into a fission product glass. It is important to weigh the advantages and drawbacks of all the possible options in terms of feasibility, safety and cost-effectiveness.« less

Preserving Plutonium-244 as a National Asset

DOE Office of Scientific and Technical Information (OSTI.GOV)

Patton, Bradley D; Alexander, Charles W; Benker, Dennis

Plutonium-244 (244 Pu) is an extremely rare and long-lived isotope of plutonium with a half-life of 80 million years. Measureable amounts of 244 Pu are found in neither reactor-grade nor weapons-grade plutonium. Production of this isotope requires a very high thermal flux to permit the two successive neutron captures that convert 242 Pu to 243 Pu to 244 Pu, particularly given the short (about 5 hour) half-life of 243 Pu. Such conditions simply do not exist in plutonium production processes. Therefore, 244 Pu is ideal for precise radiochemical analyses measuring plutonium material properties and isotopic concentrations in items containing plutonium.more » Isotope dilution mass spectrometry is about ten times more sensitive when using 244 Pu rather than 242 Pu for determining plutonium isotopic content. The isotope can also be irradiated in small quantities to produce superheavy elements. The majority of the existing global inventory of 244 Pu is contained in the outer housing of Mark-18A targets at the Savannah River Site (SRS). The total inventory is about 20 grams of 244 Pu in about 400 grams of plutonium distributed among the 65 targets. Currently, there are no specific plans to preserve these targets. Although the cost of separating and preserving this material would be considerable, it is trivial in comparison to new production costs. For all practical purposes, the material is irreplaceable, because new production would cost billions of dollars and require a series of irradiation and chemical separation cycles spanning up to 50 years. This paper will discuss a set of options for overcoming the significant challenges to preserve the 244 Pu as a National Asset: (1) the need to relocate the material from SRS in a timely manner, (2) the need to reduce the volume of material to the extent possible for storage, and (3) the need to establish an operational capability to enrich the 244 Pu in significant quantities. This paper suggests that if all the Mark-18A plutonium is separated, it would occupy a small volume and would be inexpensive to store while an enrichment capability is developed. Very small quantities could be enriched in existing mass separators to support critical needs.« less

Photoemission Spectroscopy of Delta- Plutonium: Experimental Review

NASA Astrophysics Data System (ADS)

Tobin, J. G.

2002-03-01

The electronic structure of Plutonium, particularly delta- Plutonium, remains ill defined and without direct experimental verification. Recently, we have embarked upon a program of study of alpha- and delta- Plutonium, using synchrotron radiation from the Advanced Light Source in Berkeley, CA, USA [1]. This work is set within the context of Plutonium Aging [2] and the complexities of Plutonium Science [3]. The resonant photoemission of delta-plutonium is in partial agreement with an atomic, localized model of resonant photoemission, which would be consistent with a correlated electronic structure. The results of our synchrotron- based studies will be compared with those of recent laboratory- based works [4,5,6]. The talk will conclude with a brief discussion of our plans for the future, such as the performance of spin-resolving and dichroic photoemission measurements of Plutonium [7] and the development of single crystal ultrathin films of Plutonium. This work was performed under the auspices of the U.S. Department of Energy by the University of California, Lawrence Livermore National Laboratory under Contract No. W-7405-Eng-48. 1. J. Terry, R.K. Schulze, J.D. Farr, T. Zocco, K. Heinzelman, E. Rotenberg, D.K. Shuh, G. van der Laan, D.A. Arena, and J.G. Tobin, “5f Resonant Photoemission from Plutonium”, UCRL-JC-140782, Surf. Sci. Lett., accepted October 2001. 2. B.D. Wirth, A.J. Schwartz, M.J. Fluss, M.J. Caturla, M.A. Wall, and W.G. Wolfer, MRS Bulletin 26, 679 (2001). 3. S.S. Hecker, MRS Bulletin 26, 667 (2001). 4. T. Gouder, L. Havela, F. Wastin, and J. Rebizant, Europhys. Lett. 55, 705 (2001); MRS Bulletin 26, 684 (2001); Phys. Rev. Lett. 84, 3378 (2000). 5. A.J. Arko, J.J. Joyce, L. Morales, J. Wills, J. Lashley, F. Wastin, and J. Rebizant, Phys. Rev. B 62, 1773 (2000). 6. L.E. Cox, O. Eriksson, and B.R. Cooper, Phys. Rev. B 46, 13571 (1992). 7. J. Tobin, D.A. Arena, B. Chung, P. Roussel, J. Terry, R.K. Schulze, J.D. Farr, T. Zocco, K. Heinzelman, E. Rotenberg, and D.K. Shuh, “Photoelectron Spectroscopy of Plutonium at the Advanced Light Source”, UCRL-JC-145703, J. Nucl. Sci. Tech./ Proc. of Actinides 2001, submitted November 2001.

Experimental investigation of the ionization mechanisms of uranium in thermal ionization mass spectrometry in the presence of carbon

NASA Astrophysics Data System (ADS)

Kraiem, M.; Mayer, K.; Gouder, T.; Seibert, A.; Wiss, T.; Thiele, H.; Hiernaut, J.-P.

2010-01-01

Thermal ionization mass spectrometry (TIMS) is a well established instrumental technique for providing accurate and precise isotope ratio measurements of elements with reasonably low first ionization potential. In nuclear safeguards and in environmental research, it is often required to measure the isotope ratios in small samples of uranium. Empirical studies had shown that the ionization yield of uranium and plutonium in a TIMS ion source can be significantly increased in the presence of a carbon source. But, even though carbon appeared crucial in providing high ionization yields, processes taking place on the ionization surface were still not well understood. This paper describes the experimental results obtained from an extended study on the evaporation and ionization mechanisms of uranium occurring on a rhenium mass spectrometry filament in the presence of carbon. Solid state reactions were investigated using X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM). Additionally, vaporization measurements were performed with a modified-Knudsen cell mass spectrometer for providing information on the neutral uranium species in the vapor phase. Upon heating, under vacuum, the uranyl nitrate sample was found to turn into a uranium carbide compound, independent of the type of carbon used as ionization enhancer. With further heating, uranium carbide leads to formation of single charged uranium metal ions and a small amount of uranium carbide ions. The results are relevant for a thorough understanding of the ion source chemistry of a uranyl nitrate sample under reducing conditions. The significant increase in ionization yield described by many authors on the basis of empirical results can be now fully explained and understood.

DOE Office of Scientific and Technical Information (OSTI.GOV)

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

A new rapid fusion method for the determination of plutonium in large rice samples has been developed at the Savannah River National Laboratory (Aiken, SC, USA) that can be used to determine very low levels of plutonium isotopes in rice. The recent accident at Fukushima Nuclear Power Plant in March, 2011 reinforces the need to have rapid, reliable radiochemical analyses for radionuclides in environmental and food samples. Public concern regarding foods, particularly foods such as rice in Japan, highlights the need for analytical techniques that will allow very large sample aliquots of rice to be used for analysis so thatmore » very low levels of plutonium isotopes may be detected. The new method to determine plutonium isotopes in large rice samples utilizes a furnace ashing step, a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step, and a column separation process with TEVA Resin cartridges. The method can be applied to rice sample aliquots as large as 5 kg. Plutonium isotopes can be determined using alpha spectrometry or inductively-coupled plasma mass spectrometry (ICP-MS). The method showed high chemical recoveries and effective removal of interferences. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory plutonium particles are effectively digested. The MDA for a 5 kg rice sample using alpha spectrometry is 7E-5 mBq g{sup -1}. The method can easily be adapted for use by ICP-MS to allow detection of plutonium isotopic ratios.« less

Thermal radiative and thermodynamic properties of solid and liquid uranium and plutonium carbides in the visible-near-infrared range

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.

Amarillo National Resource Center for Plutonium quarterly technical progress report, August 1, 1997--October 31, 1997

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

This report summarizes activities of the Amarillo National Resource Center for Plutonium during the quarter. The report describes the Electronic Resource Library; DOE support activities; current and future environmental health and safety programs; pollution prevention and pollution avoidance; communication, education, training, and community involvement programs; and nuclear and other material studies, including plutonium storage and disposition studies.

Fuel bundle design for enhanced usage of plutonium fuel

DOEpatents

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

DOEpatents

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.

PLUTONIUM PROCESSING OPTIMIZATION IN SUPPORT OF THE MOX FUEL PROGRAM

DOE Office of Scientific and Technical Information (OSTI.GOV)

GRAY, DEVIN W.; COSTA, DAVID A.

2007-02-02

After Los Alamos National Laboratory (LANL) personnel completed polishing 125 Kg of plutonium as highly purified PuO{sub 2} from surplus nuclear weapons, Duke, COGEMA, Stone, and Webster (DCS) required as the next process stage, the validation and optimization of all phases of the plutonium polishing flow sheet. Personnel will develop the optimized parameters for use in the upcoming 330 kg production mission.

Nuclear Matters. A Practical Guide

DTIC Science & Technology

2008-01-01

plutonium science and engineering. Figure 4.6 depicts LANL workers in Technical Area (TA)-55, the Los Alamos plutonium facility. LANL oversees...facility at Los Alamos to produce plutonium pits in a laboratory environment, with a capacity to produce a small number of pits per year . At that...Office of Secure Transportation (OST). Technical Advisors represent the following organizations: Los Alamos National Chair ATSD(NCB) Vice-Chair

The Alliance of Advanced Process Control and Accountability – A Future Safeguards-By-Design Tool

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lumetta, Gregg J.; Bresee, James C.; Paviet, Patricia D.

For any chemical separation process producing a valuable product, a material balance is an important process control measurement. That is particularly true for the separation of actinides from irradiated nuclear fuel, not only for their intrinsic value but also because an incomplete material balance may indicate diversion for unauthorized use. The DOE Office of Nuclear Energy is currently carrying out at the Pacific Northwest National Laboratory an experimental measurement of how well and with what precision current technologies can implement near real-time actinide material balances. This measurement effort is called the CoDCon project. It involves the separation of a productmore » with a 70/30 uranium/plutonium mass ratio. Initial tests will use dissolved fuel simulants prepared with pure uranium and plutonium nitrates at the same input ratios as irradiated fuel. Subsequent testing with actual irradiated fuel would be done to verify the results obtained with simulants. The experiments will use advanced on-line instrumentation supported by dynamic process models. Since accountability uncertainties could mask diversions, the aim of the project is not only to measure present-day capabilities but also, through sensitivity analyses, to identify those measurements with the greatest potential for overall material-balance improvements. The latter results will help identify priorities for future fuel cycle R&D programs. Advanced separations process control and material accountability technologies thus have a common goal: to provide the best tools available for safeguards-by-design [defined by the International Atomic Energy Agency (IAEA) as the integration of the design of a new nuclear facility through planning, construction, operation and decommissioning]. Since the potential domestic use of CoDCon results may be later than their possible foreign applications, arrangements may be feasible for possible bilateral or multinational cooperation in the CoDCon project.« less

Density functional theory study of defects in unalloyed δ-Pu

DOE PAGES

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

Determination of plutonium in nitric acid solutions using energy dispersive L X-ray fluorescence with a low power X-ray generator

NASA Astrophysics Data System (ADS)

Py, J.; Groetz, J.-E.; Hubinois, J.-C.; Cardona, D.

2015-04-01

This work presents the development of an in-line energy dispersive L X-ray fluorescence spectrometer set-up, with a low power X-ray generator and a secondary target, for the determination of plutonium concentration in nitric acid solutions. The intensity of the L X-rays from the internal conversion and gamma rays emitted by the daughter nuclei from plutonium is minimized and corrected, in order to eliminate the interferences with the L X-ray fluorescence spectrum. The matrix effects are then corrected by the Compton peak method. A calibration plot for plutonium solutions within the range 0.1-20 g L-1 is given.

Preparation of high purity plutonium oxide for radiochemistry instrument calibration standards and working standards

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wong, A.S.; Stalnaker, N.D.

1997-04-01

Due to the lack of suitable high level National Institute of Standards and Technology (NIST) traceable plutonium solution standards from the NIST or commercial vendors, the CST-8 Radiochemistry team at Los Alamos National Laboratory (LANL) has prepared instrument calibration standards and working standards from a well-characterized plutonium oxide. All the aliquoting steps were performed gravimetrically. When a {sup 241}Am standardized solution obtained from a commercial vendor was compared to these calibration solutions, the results agreed to within 0.04% for the total alpha activity. The aliquots of the plutonium standard solutions and dilutions were sealed in glass ampules for long termmore » storage.« 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

SPRAY CALCINATION REACTOR

DOEpatents

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)

METHOD FOR SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS BY SOLVENT EXTRACTION

DOEpatents

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).

Second-order Kinetics of DTPA and Plutonium in Rat Plasma

DOE Office of Scientific and Technical Information (OSTI.GOV)

Miller, Guthrie; Poudel, Deepesh; Klumpp, John Allan

We report that in 2008, Serandour et al. reported on their in vitro experiment involving rat plasma samples obtained after an intravenous intake of plutonium citrate. Different amounts of DTPA were added to the plasma samples and the percentage of low-molecular-weight plutonium measured. Only when the DTPA dosage was three orders of magnitude greater than the recommended 30 μmol/kg was 100% of the plutonium apparently in the form of chelate. These data were modeled assuming three competing chemical reactions with other molecules that bind with plutonium. Here, time-dependent second-order kinetics of these reactions are calculated, intended eventually to become partmore » of a complete biokinetic model of DTPA action on actinides in laboratory animals or humans. The probability distribution of the ratio of stability constants for the reactants was calculated using Markov Chain Monte Carlo. In conclusion, these calculations substantiate that the inclusion of more reactions is needed in order to be in agreement with known stability constants.« less

Long-term retrievability and safeguards for immobilized weapons plutonium in geologic storage

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peterson, P.F.

1996-05-01

If plutonium is not ultimately used as an energy source, the quantity of excess weapons plutonium (w-Pu) that would go into a US repository will be small compared to the quantity of plutonium contained in the commercial spent fuel in the repository, and the US repository(ies) will likely be only one (or two) locations out of many around the world where commercial spent fuel will be stored. Therefore excess weapons plutonium creates a small perturbation to the long-term (over 200,000 yr) global safeguard requirements for spent fuel. There are details in the differences between spent fuel and immobilized w-Pu wastemore » forms (i.e. chemical separation methods, utility for weapons, nuclear testing requirements), but these are sufficiently small to be unlikely to play a significant role in any US political decision to rebuild weapons inventories, or to change the long-term risks of theft by subnational groups.« less

Second-order Kinetics of DTPA and Plutonium in Rat Plasma

DOE PAGES

Miller, Guthrie; Poudel, Deepesh; Klumpp, John Allan; ...

2017-11-15

We report that in 2008, Serandour et al. reported on their in vitro experiment involving rat plasma samples obtained after an intravenous intake of plutonium citrate. Different amounts of DTPA were added to the plasma samples and the percentage of low-molecular-weight plutonium measured. Only when the DTPA dosage was three orders of magnitude greater than the recommended 30 μmol/kg was 100% of the plutonium apparently in the form of chelate. These data were modeled assuming three competing chemical reactions with other molecules that bind with plutonium. Here, time-dependent second-order kinetics of these reactions are calculated, intended eventually to become partmore » of a complete biokinetic model of DTPA action on actinides in laboratory animals or humans. The probability distribution of the ratio of stability constants for the reactants was calculated using Markov Chain Monte Carlo. In conclusion, these calculations substantiate that the inclusion of more reactions is needed in order to be in agreement with known stability constants.« less

Plutonium Immobilization Project System Design Description for Can Loading System

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kriikku, E.

2001-02-15

The purpose of this System Design Description (SDD) is to specify the system and component functions and requirements for the Can Loading System and provide a complete description of the system (design features, boundaries, and interfaces), principles of operation (including upsets and recovery), and the system maintenance approach. The Plutonium Immobilization Project (PIP) will immobilize up to 13 metric tons (MT) of U.S. surplus weapons usable plutonium materials.

DISSOLUTION OF PLUTONIUM CONTAINING CARRIER PRECIPITATE BY CARBONATE METATHESIS AND SEPARATION OF SULFIDE IMPURITIES THEREFROM BY SULFIDE PRECIPITATION

DOEpatents

Duffield, R.B.

1959-07-14

A process is described for recovering plutonium from foreign products wherein a carrier precipitate of lanthanum fluoride containing plutonium is obtained and includes the steps of dissolving the carrier precipitate in an alkali metal carbonate solution, adding a soluble sulfide, separating the sulfide precipitate, adding an alkali metal hydroxide, separating the resulting precipitate, washing, and dissolving in a strong acid.

METHOD OF SEPARATING URANIUM, PLUTONIUM AND FISSION PRODUCTS BY BROMINATION AND DISTILLATION

DOEpatents

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.

Update on the Department of Energy's 1994 plutonium vulnerability assessment for the plutonium finishing plant

DOE Office of Scientific and Technical Information (OSTI.GOV)

HERZOG, K.R.

1999-09-01

A review of the environmental, safety, and health vulnerabilities associated with the continued storage of PFP's inventory of plutonium bearing materials and other SNM. This report re-evaluates the five vulnerabilities identified in 1994 at the PFP that are associated with SNM storage. This new evaluation took a more detailed look and applied a risk ranking process to help focus remediation efforts.

METHOD OF PREPARING METAL HALIDES

DOEpatents

Hendrickson, A.V.

1958-11-18

The conversion of plutonium halides from plutonium peroxide can be done by washing the peroxide with hydrogen peroxide, drying the peroxide, passing a dry gaseous hydrohalide over the surface of the peroxide at a temperature of about lOO icient laborato C until the reaction rate has stabillzed, and then ralsing the reaction temperature to between 400 and 600 icient laborato C until the conversion to plutonium halide is substantially complete.

REDUCTION OF PLUTONIUM TO Pu$sup +3$ BY SODIUM DITHIONITE IN POTASSIUM CARBONATE

DOEpatents

Miller, D.R.; Hoekstra, H.R.

1958-12-16

Plutonium values are reduced in an alkaline aqueous medlum to the trlvalent state by means of sodium dlthionite. Plutonlum values are also separated from normally assoclated contaminants by metathesizing a lanthanum fluoride carrier precipitate containing plutonium with a hydroxide solution, performing the metathesis in the presence of about 0.2 M sodium dithionite at a temperature of between 40 and 90 icient laborato C.

METHOD FOR DISSOLVING LANTHANUM FLUORIDE CARRIER FOR PLUTONIUM

DOEpatents

Koshland, D.E. Jr.; Willard, J.E.

1961-08-01

A method is described for dissolving lanthanum fluoride precipitates which is applicable to lanthanum fluoride carrier precipitation processes for recovery of plutonium values from aqueous solutions. The lanthanum fluoride precipitate is contacted with an aqueous acidic solution containing dissolved zirconium in the tetravalent oxidation state. The presence of the zirconium increases the lanthanum fluoride dissolved and makes any tetravalent plutonium present more readily oxidizable to the hexavalent state. (AEC)

Literature Review: Crud Formation at the Liquid/Liquid Interface of TBP-Based Solvent-Extraction Processes

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.

RECOVERY OF Pu VALUES BY FLUORINATION AND FRACTIONATION

DOEpatents

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.

METHOD OF PREPARING PLUTONIUM TETRAFLUORIDE

DOEpatents

Beede, R.L.; Hopkins, H.H. Jr.

1959-11-17

C rystalline plutonium tetrafluoride is precipitated from aqueous up to 1.6 N mineral acid solutions of a plutorium (IV) salt with fluosilicic acid anions, preferably at room temperature. Hydrogen fluoride naay be added after precipitation to convert any plutonium fluosilicate to the tetrafluoride and any silica to fluosilicic acid. This process results in a purer product, especially as to iron and aluminum, than does the precipitation by the addition of hydrogen fluoride.

Method of immobilizing weapons plutonium to provide a durable, disposable waste product

DOEpatents

Ewing, Rodney C.; Lutze, Werner; Weber, William J.

1996-01-01

A method of atomic scale fixation and immobilization of plutonium to provide a durable waste product. Plutonium is provided in the form of either PuO.sub.2 or Pu(NO.sub.3).sub.4 and is mixed with and SiO.sub.2. The resulting mixture is cold pressed and then heated under pressure to form (Zr,Pu)SiO.sub.4 as the waste product.

Radiation damage and annealing in plutonium tetrafluoride

DOE Office of Scientific and Technical Information (OSTI.GOV)

McCoy, Kaylyn; Casella, Amanda; Sinkov, Sergey

Plutonium tetrafluoride that was separated prior to 1966 at the Hanford Site in Washington State was analyzed at the Pacific Northwest National Laboratory (PNNL) in 2015 and 2016. The plutonium tetrafluoride, as received, was an off-normal color and considering the age of the plutonium, there were questions about the condition of the material. These questions had to be answered in order to determine the suitability of the material for future use or long-term storage. Therefore, Thermogravimetric/Differential Thermal Analysis and X-ray Diffraction evaluations were conducted to determine the plutonium’s crystal structure, oxide content, and moisture content; these analyses reported that themore » plutonium was predominately amorphous and tetrafluoride, with an oxide content near ten percent. Freshly fluorinated plutonium tetrafluoride is known to be monoclinic. During the initial Thermogravimetric/Differential Thermal analyses, it was discovered that an exothermic event occurred within the material near 414°C. X-ray Diffraction analyses were conducted on the annealed tetrafluoride. The X-ray Diffraction analyses indicated that some degree of recrystallization occurred in conjunction with the 414°C event. The following commentary describes the series of Thermogravimetric/Differential Thermal and X-ray Diffraction analyses that were conducted as part of this investigation at PNNL, in collaboration with the University of Utah Nuclear Engineering Program.« less

Resuspension studies in the Marshall Islands.

PubMed

Shinn, J H; Homan, D N; Robison, W L

1997-07-01

The contribution of inhalation exposure to the total dose for residents of the Marshall Islands was monitored at occasions of opportunity on several islands in the Bikini and Enewetak Atolls. To determine the long-term potential for inhalation exposure, and to understand the mechanisms of redistribution and personal exposure, additional investigations were undertaken on Bikini Island under modified and controlled conditions. Experiments were conducted to provide key parameters for the assessment of inhalation exposure from plutonium-contaminated dust aerosols: characterization of the contribution of plutonium in soil-borne aerosols as compared to sea spray and organic aerosols, determination of plutonium resuspension rates as measured by the meteorological flux-gradient method during extreme conditions of a bare-soil vs. a stabilized surface, determination of the approximate individual exposures to resuspended plutonium by traffic, and studies of exposures to individuals in different occupational environments simulated by personal air sampling of workers assigned to a variety of tasks. Enhancement factors (defined as ratios of the plutonium-activity of suspended aerosols relative to the plutonium-activity of the soil) were determined to be less than 1 (typically 0.4 to 0.7) in the undisturbed, vegetated areas, but greater than 1 (as high as 3) for the case studies of disturbed bare soil, roadside travel, and for occupational duties in fields and in and around houses.

Environmental consequences of postulate plutonium releases from Atomics International's Nuclear Materials Development Facility (NMDF), Santa Susana, California, as a result of severe natural phenomena

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jamison, J.D.; Watson, E.C.

1982-02-01

Potential environmental consequences in terms of radiation dose to people are presented for postulated plutonium releases caused by severe natural phenomena at the Atomics International's Nuclear Materials Development Facility (NMDF), in the Santa Susana site, California. The severe natural phenomena considered are earthquakes, tornadoes, and high straight-line winds. Plutonium deposition values are given for significant locations around the site. All important potential exposure pathways are examined. The most likely 50-year committed dose equivalents are given for the maximum-exposed individual and the population within a 50-mile radius of the plant. The maximum plutonium deposition values likely to occur offsite are alsomore » given. The most likely calculated 50-year collective committed dose equivalents are all much lower than the collective dose equivalent expected from 50 years of exposure to natural background radiation and medical x-rays. The most likely maximum residual plutonium contamination estimated to be deposited offsite following the earthquake, and the 150-mph and 170-mph tornadoes are above the Environmental Protection Agency's (EPA) proposed guideline for plutonium in the general environment of 0.2 ..mu..Ci/m/sup 2/. The deposition values following the 110-mph and the 130-mph tornadoes are below the EPA proposed guideline.« less

Environmental consequences of postulated plutonium releases from General Electric Company Vallecitos Nuclear Center, Vallecitos, California, as a result of severe natural phenomena

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jamison, J.D.; Watson, E.C.

1980-11-01

Potential environmental consequences in terms of radiation dose to people are presented for postulated plutonium releases caused by severe natural phenomena at the General Electric Company Vallecitos Nuclear Center, Vallecitos, California. The severe natural phenomena considered are earthquakes, tornadoes, and high straight-line winds. Maximum plutonium deposition values are given for significant locations around the site. All important potential exposure pathways are examined. The most likely 50-year committed dose equivalents are given for the maximum-exposed individual and the population within a 50-mile radius of the plant. The maximum plutonium deposition values likely to occur offsite are also given. The most likelymore » calculated 50-year collective committed dose equivalents are all much lower than the collective dose equivalent expected from 50 years of exposure to natural background radiation and medical x-rays. The most likely maximum residual plutonium contamination estimated to be deposited offsite following the earthquakes, and the 180-mph and 230-mph tornadoes are above the Environmental Protection Agency's (EPA) proposed guideline for plutonium in the general environment of 0.2 ..mu..Ci/m/sup 2/. The deposition values following the 135-mph tornado are below the EPA proposed guidelines.« less

Plutonium interaction studies with the Mont Terri Opalinus Clay isolate Sporomusa sp. MT-2.99: changes in the plutonium speciation by solvent extractions.

PubMed

Moll, Henry; Cherkouk, Andrea; Bok, Frank; Bernhard, Gert

2017-05-01

Since plutonium could be released from nuclear waste disposal sites, the exploration of the complex interaction processes between plutonium and bacteria is necessary for an improved understanding of the fate of plutonium in the vicinity of such a nuclear waste disposal site. In this basic study, the interaction of plutonium with cells of the bacterium, Sporomusa sp. MT-2.99, isolated from Mont Terri Opalinus Clay, was investigated anaerobically (in 0.1 M NaClO 4 ) with or without adding Na-pyruvate as an electron donor. The cells displayed a strong pH-dependent affinity for Pu. In the absence of Na-pyruvate, a strong enrichment of stable Pu(V) in the supernatants was discovered, whereas Pu(IV) polymers dominated the Pu oxidation state distribution on the biomass at pH 6.1. A pH-dependent enrichment of the lower Pu oxidation states (e.g., Pu(III) at pH 6.1 which is considered to be more mobile than Pu(IV) formed at pH 4) was observed in the presence of up to 10 mM Na-pyruvate. In all cases, the presence of bacterial cells enhanced removal of Pu from solution and accelerated Pu interaction reactions, e.g., biosorption and bioreduction.

Improved plutonium identification and characterization results with NaI(Tl) detector using ASEDRA

NASA Astrophysics Data System (ADS)

Detwiler, R.; Sjoden, G.; Baciak, J.; LaVigne, E.

2008-04-01

The ASEDRA algorithm (Advanced Synthetically Enhanced Detector Resolution Algorithm) is a tool developed at the University of Florida to synthetically enhance the resolved photopeaks derived from a characteristically poor resolution spectra collected at room temperature from scintillator crystal-photomultiplier detector, such as a NaI(Tl) system. This work reports on analysis of a side-by-side test comparing the identification capabilities of ASEDRA applied to a NaI(Tl) detector with HPGe results for a Plutonium Beryllium (PuBe) source containing approximately 47 year old weapons-grade plutonium (WGPu), a test case of real-world interest with a complex spectra including plutonium isotopes and 241Am decay products. The analysis included a comparison of photopeaks identified and photopeak energies between the ASEDRA and HPGe detector systems, and the known energies of the plutonium isotopes. ASEDRA's performance in peak area accuracy, also important in isotope identification as well as plutonium quality and age determination, was evaluated for key energy lines by comparing the observed relative ratios of peak areas, adjusted for efficiency and attenuation due to source shielding, to the predicted ratios from known energy line branching and source isotopics. The results show that ASEDRA has identified over 20 lines also found by the HPGe and directly correlated to WGPu energies.

The plutonium isotopic composition of marine biota on Enewetak Atoll: a preliminary assessment.

PubMed

Hamilton, Terry F; Martinelli, Roger E; Kehl, Steven R; McAninch, Jeffrey E

2008-10-01

We have determined the level and distribution of gamma-emitting radionuclides, plutonium activity concentrations, and 240Pu/239Pu atom ratios in tissue samples of giant clam (Tridacna gigas and Hippopus hippopus), a top snail (Trochus nilaticas) and sea cucumber (Holothuria atra) collected from different locations around Enewetak Atoll. The plutonium isotopic measurements were performed using ultra-high sensitivity accelerator mass spectrometry (AMS). Elevated levels of plutonium were observed in the stomachs (includes the stomach lining) of Tridacna clam (0.62 to 2.98 Bq kg(-1), wet wt.), in the soft parts (edible portion) of top snails (0.25 to 1.7 Bq kg(-1)), wet wt.) and, to a lesser extent, in sea cucumber (0.015 to 0.22 Bq kg(-1), wet wt.) relative to muscle tissue concentrations in clam (0.006 to 0.021 Bq kg(-1), wet wt.) and in comparison with previous measurements of plutonium in fish. These data and information provide a basis for re-evaluating the relative significance of dietary intakes of plutonium from marine foods on Enewetak Atoll and, perhaps most importantly, demonstrate that discrete 240Pu239Pu isotope signatures might well provide a useful investigative tool to monitor source-term attribution and consequences on Enewetak Atoll. One potential application of immediate interest is to monitor and assess the health and ecological impacts of leakage of plutonium (as well as other radionuclides) from a low-level radioactive waste repository on Runit Island relative to background levels of fallout contamination in Enewetak Atoll lagoon.

Verification of Plutonium Content in PuBe Sources Using MCNP® 6.2.0 Beta with TENDL 2012 Libraries

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lockhart, Madeline Louise; McMath, Garrett Earl

Although the production of PuBe neutron sources has discontinued, hundreds of sources with unknown or inaccurately declared plutonium content are in existence around the world. Institutions have undertaken the task of assaying these sources, measuring, and calculating the isotopic composition, plutonium content, and neutron yield. The nominal plutonium content, based off the neutron yield per gram of pure 239Pu, has shown to be highly inaccurate. New methods of measuring the plutonium content allow a more accurate estimate of the true Pu content, but these measurements need verification. Using the TENDL 2012 nuclear data libraries, MCNP6 has the capability to simulatemore » the (α, n) interactions in a PuBe source. Theoretically, if the source is modeled according to the plutonium content, isotopic composition, and other source characteristics, the calculated neutron yield in MCNP can be compared to the experimental yield, offering an indication of the accuracy of the declared plutonium content. In this study, three sets of PuBe sources from various backgrounds were modeled in MCNP6 1.2 Beta, according to the source specifications dictated by the individuals who assayed the source. Verification of the source parameters with MCNP6 also serves as a means to test the alpha transport capabilities of MCNP6 1.2 Beta with TENDL 2012 alpha transport libraries. Finally, good agreement in the comparison would indicate the accuracy of the source parameters in addition to demonstrating MCNP's capabilities in simulating (α, n) interactions.« less

Verification of Plutonium Content in PuBe Sources Using MCNP® 6.2.0 Beta with TENDL 2012 Libraries

DOE PAGES

Lockhart, Madeline Louise; McMath, Garrett Earl

2017-10-26

Although the production of PuBe neutron sources has discontinued, hundreds of sources with unknown or inaccurately declared plutonium content are in existence around the world. Institutions have undertaken the task of assaying these sources, measuring, and calculating the isotopic composition, plutonium content, and neutron yield. The nominal plutonium content, based off the neutron yield per gram of pure 239Pu, has shown to be highly inaccurate. New methods of measuring the plutonium content allow a more accurate estimate of the true Pu content, but these measurements need verification. Using the TENDL 2012 nuclear data libraries, MCNP6 has the capability to simulatemore » the (α, n) interactions in a PuBe source. Theoretically, if the source is modeled according to the plutonium content, isotopic composition, and other source characteristics, the calculated neutron yield in MCNP can be compared to the experimental yield, offering an indication of the accuracy of the declared plutonium content. In this study, three sets of PuBe sources from various backgrounds were modeled in MCNP6 1.2 Beta, according to the source specifications dictated by the individuals who assayed the source. Verification of the source parameters with MCNP6 also serves as a means to test the alpha transport capabilities of MCNP6 1.2 Beta with TENDL 2012 alpha transport libraries. Finally, good agreement in the comparison would indicate the accuracy of the source parameters in addition to demonstrating MCNP's capabilities in simulating (α, n) interactions.« less

Survey of glass plutonium contents and poison selection

DOE Office of Scientific and Technical Information (OSTI.GOV)

Plodinec, M.J.; Ramsey, W.G.; Ellison, A.J.G.

1996-05-01

If plutonium and other actinides are to be immobilized in glass, then achieving high concentrations in the glass is desirable. This will lead to reduced costs and more rapid immobilization. However, glasses with high actinide concentrations also bring with them undersirable characteristics, especially a greater concern about nuclear criticality, particularly in a geologic repository. The key to achieving a high concentration of actinide elements in a glass is to formulate the glass so that the solubility of actinides is high. At the same time, the glass must be formulated so that the glass also contains neutron poisons, which will preventmore » criticality during processing and in a geologic repository. In this paper, the solubility of actinides, particularly plutonium, in three types of glasses are discussed. Plutonium solubilities are in the 2-4 wt% range for borosilicate high-level waste (HLW) glasses of the type which will be produced in the US. This type of glass is generally melted at relatively low temperatures, ca. 1150{degrees}C. For this melting temperature, the glass can be reformulated to achieve plutonium solubilities of at least 7 wt%. This low melting temperature is desirable if one must retain volatile cesium-137 in the glass. If one is not concerned about cesium volatility, then glasses can be formulated which can contain much larger amounts of plutonium and other actinides. Plutonium concentrations of at least 15 wt% have been achieved. Thus, there is confidence that high ({ge}5 wt%) concentrations of actinides can be achieved under a variety of conditions.« less

Quantitative determination of environmental levels of uranium, thorium and plutonium in bone by solvent extraction and alpha spectrometry

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%.

An independent evaluation of plutonium body burdens in populations near Los Alamos Laboratory using human autopsy data.

PubMed

Gaffney, Shannon H; Donovan, Ellen P; Shonka, Joseph J; Le, Matthew H; Widner, Thomas E

2013-06-01

In the mid-1940s, the United States began producing atomic weapon components at the Los Alamos National Laboratory (LANL). In an attempt to better understand historical exposure to nearby residents, this study evaluates plutonium activity in human tissue relative to residential location and length of time at residence. Data on plutonium activity in the lung, vertebrae, and liver of nearby residents were obtained during autopsies as a part of the Los Alamos Tissue Program. Participant residential histories and the distance from each residence to the primary plutonium processing buildings at LANL were evaluated in the analysis. Summary statistics, including Student t-tests and simple regressions, were calculated. Because the biological half-life of plutonium can vary significantly by organ, data were analyzed separately by tissue type (lung, liver, vertebrae). The ratios of plutonium activity (vertebrae:liver; liver:lung) were also analyzed in order to evaluate the importance of timing of exposure. Tissue data were available for 236 participants who lived in a total of 809 locations, of which 677 were verified postal addresses. Residents of Los Alamos were found to have higher plutonium activities in the lung than non-residents. Further, those who moved to Los Alamos before 1955 had higher lung activities than those who moved there later. These trends were not observed with the liver, vertebrae, or vertebrae:liver and liver:lung ratio data, however, and should be interpreted with caution. Although there are many limitations to this study, including the amount of available data and the analytical methods used to analyze the tissue, the overall results indicate that residence (defined as the year that the individual moved to Los Alamos) may have had a strong correlation to plutonium activity in human tissue. This study is the first to present the results of Los Alamos Autopsy Program in relation to residential status and location in Los Alamos. Copyright © 2012 Elsevier GmbH. All rights reserved.

Study of plutonium disposition using the GE Advanced Boiling Water Reactor (ABWR)

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

1994-04-30

The end of the cold war and the resulting dismantlement of nuclear weapons has resulted in the need for the U.S. to disposition 50 to 100 metric tons of excess of plutonium in parallel with a similar program in Russia. A number of studies, including the recently released National Academy of Sciences (NAS) study, have recommended conversion of plutonium into spent nuclear fuel with its high radiation barrier as the best means of providing long-term diversion resistance to this material. The NAS study {open_quotes}Management and Disposition of Excess Weapons Plutonium{close_quotes} identified light water reactor spent fuel as the most readilymore » achievable and proven form for the disposition of excess weapons plutonium. The study also stressed the need for a U.S. disposition program which would enhance the prospects for a timely reciprocal program agreement with Russia. This summary provides the key findings of a GE study where plutonium is converted into Mixed Oxide (MOX) fuel and a 1350 MWe GE Advanced Boiling Water Reactor (ABWR) is utilized to convert the plutonium to spent fuel. The ABWR represents the integration of over 30 years of experience gained worldwide in the design, construction and operation of BWRs. It incorporates advanced features to enhance reliability and safety, minimize waste and reduce worker exposure. For example, the core is never uncovered nor is any operator action required for 72 hours after any design basis accident. Phase 1 of this study was documented in a GE report dated May 13, 1993. DOE`s Phase 1 evaluations cited the ABWR as a proven technical approach for the disposition of plutonium. This Phase 2 study addresses specific areas which the DOE authorized as appropriate for more in-depth evaluations. A separate report addresses the findings relative to the use of existing BWRs to achieve the same goal.« less

Further evaluations of the toxicity of irradiated advanced heavy water reactor fuels.

PubMed

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.

METHOD OF MAINTAINING PLUTONIUM IN A HIGHER STATE OF OXIDATION DURING PROCESSING

DOEpatents

Thompson, S.G.; Miller, D.R.

1959-06-30

This patent deals with the oxidation of tetravalent plutonium contained in an aqueous acid solution together with fission products to the hexavalent state, prior to selective fission product precipitation, by adding to the solution bismuthate or ceric ions as the oxidant and a water-soluble dichromate as a holding oxidant. Both oxidant and holding oxidant are preferably added in greater than stoichiometric quantities with regard to the plutonium present.

Exploding the myths about the fast breeder reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Burns, S.

1979-01-01

This paper discusses the facts and figures about the effects of conservation policies, the benefits of the Clinch River Breeder Reactor demonstration plant, the feasibility of nuclear weapons manufacture from reactor-grade plutonium, diversion of plutonium from nuclear plants, radioactive waste disposal, and the toxicity of plutonium. The paper concludes that the U.S. is not proceeding with a high confidence strategy for breeder development because of a variety of false assumptions.

NUCLEAR CLEANUP: Progress Made at Rocky Flats, but Closure by 2006 Is Unlikely, and Costs May Increase

DTIC Science & Technology

2001-02-01

liquids or residues from process pipes and tanks. The contractor also dismantled plutonium - processing furnaces, stripped out contaminated process...Soil Cleanup Levels on the Scope and Cost of the 903 Pad Cleanup 30 Figures Figure 1: Workers in Protective Clothing Handling Plutonium - Contaminated ...activities—shipping nuclear materials such as plutonium - contaminated metals and powders—is expected to be completed in 2002. Another activity

SEPARATION OF PLUTONIUM VALUES FROM OTHER METAL VALUES IN AQUEOUS SOLUTIONS BY SELECTIVE COMPLEXING AND ADSORPTION

DOEpatents

Beaton, R.H.

1960-06-28

A process is given for separating tri- or tetravalent plutonium from fission products in an aqueous solution by complexing the fission products with oxalate, tannate, citrate, or tartrate anions at a pH value of at least 2.4 (preferably between 2.4 and 4), and contacting a cation exchange resin with the solution whereby the plutonium is adsorbed while the complexed fission products remain in solution.

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.

Heterogeneity Effects in Plutonium Contaminated Soil

DTIC Science & Technology

2009-03-01

masses up to one kilogram once the ratio of Americium - 241 (Am- 241 ) and plutonium concentrations was established (Rademacher, 2001). Alpha...with a sample number and tared weight with a non-smearing marker. A standard control was then set using a point source of Americium - 241 on an aluminum...During the fire the weapons grade plutonium (Pu- 239, Pu-240, and Pu- 241 ) ignited and was released into the surrounding area, due to both

SEPARATION PROCESS USING COMPLEXING AND ADSORPTION

DOEpatents

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.

PURIFICATION OF PLUTONIUM USING A CERIUM PRECIPITATE AS A CARRIER FOR FISSION PRODUCTS

DOEpatents

Faris, B.F.; Olson, C.M.

1961-07-01

Bismuth phosphate carrier precipitation processes are described for the separation of plutonium from fission products wherein in at least one step bismuth phosphate is precipitated in the presence of hexavalent plutonium thereby carrying a portion of the fission products from soluble plu tonium values. In this step, a cerium phosphate precipitate is formed in conjunction with the bismuth phosphate precipitate, thereby increasing the amount of fission products removed from solution.

Electrolysis of plutonium nitride in LiCl-KCl eutectic melts

NASA Astrophysics Data System (ADS)

Shirai, O.; Iwai, T.; Shiozawa, K.; Suzuki, Y.; Sakamura, Y.; Inoue, T.

2000-01-01

The electrolysis of plutonium nitride, PuN, was investigated in the LiCl-KCl eutectic salt with 0.54 wt% PuCl 3 at 773 K in order to understand the dissolution of PuN at the anode and the deposition of metal at the cathode from the viewpoint of the application of a pyrochemical process to nitride fuel cycle. It was found from cyclic voltammetry that the electrochemical dissolution of PuN began nearly at the theoretically evaluated potential and this reaction was irreversible. Several grams of plutonium metal were successfully recovered at the molybdenum electrode as a deposit with a current efficiency of about 90%, although some fractions of the deposited plutonium often fell from the molybdenum electrode.

Removal of dissolved actinides from alkaline solutions by the method of appearing reagents

DOEpatents

Krot, Nikolai N.; Charushnikova, Iraida A.

1997-01-01

A method of reducing the concentration of neptunium and plutonium from alkaline radwastes containing plutonium and neptunium values along with other transuranic values produced during the course of plutonium production. The OH.sup.- concentration of the alkaline radwaste is adjusted to between about 0.1M and about 4M. [UO.sub.2 (O.sub.2).sub.3 ].sup.4- ion is added to the radwastes in the presence of catalytic amounts of Cu.sup.+2, Co.sup.+2 or Fe.sup.+2 with heating to a temperature in excess of about 60.degree. C. or 85.degree. C., depending on the catalyst, to coprecipitate plutonium and neptunium from the radwaste. Thereafter, the coprecipitate is separated from the alkaline radwaste.

PYROMETALLURGICAL METHOD

DOEpatents

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.

Lung Cancer Risk from Plutonium: A Pooled Analysis of the Mayak and Sellafield Worker Cohorts.

PubMed

Gillies, Michael; Kuznetsova, Irina; Sokolnikov, Mikhail; Haylock, Richard; O'Hagan, Jackie; Tsareva, Yulia; Labutina, Elena

2017-12-01

In this study, lung cancer risk from occupational plutonium exposure was analyzed in a pooled cohort of Mayak and Sellafield workers, two of the most informative cohorts in the world with detailed plutonium urine monitoring programs. The pooled cohort comprised 45,817 workers: 23,443 Sellafield workers first employed during 1947-2002 with follow-up until the end of 2005 and 22,374 Mayak workers first employed during 1948-1982 with follow-up until the end of 2008. In the pooled cohort 1,195 lung cancer deaths were observed (789 Mayak, 406 Sellafield) but only 893 lung cancer incidences (509 Mayak, 384 Sellafield, due to truncated follow-up in the incidence analysis). Analyses were performed using Poisson regression models, and were based on doses derived from individual radiation monitoring data using an updated dose assessment methodology developed in the study. There was clear evidence of a linear association between cumulative internal plutonium lung dose and risk of both lung cancer mortality and incidence in the pooled cohort. The pooled point estimates of the excess relative risk (ERR) from plutonium exposure for both lung cancer mortality and incidence were within the range of 5-8 per Gy for males at age 60. The ERR estimates in relationship to external gamma radiation were also significantly raised and in the range 0.2-0.4 per Gy of cumulative gamma dose to the lung. The point estimates of risk, for both external and plutonium exposure, were comparable between the cohorts, which suggests that the pooling of these data was valid. The results support point estimates of relative biological effectiveness (RBE) in the range of 10-25, which is in broad agreement with the value of 20 currently adopted in radiological protection as the radiation weighting factor for alpha particles, however, the uncertainty on this value (RBE = 21; 95% CI: 9-178) is large. The results provide direct evidence that the plutonium risks in each cohort are of the same order of magnitude but the uncertainty on the Sellafield cohort plutonium risk estimates is large, with observed risks consistent with no plutonium risk, and risks five times larger than those observed in the Mayak cohort.

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

A review of plutonium oxalate decomposition reactions and effects of decomposition temperature on the surface area of the plutonium dioxide product

NASA Astrophysics Data System (ADS)

Orr, R. M.; Sims, H. E.; Taylor, R. J.

2015-10-01

Plutonium (IV) and (III) ions in nitric acid solution readily form insoluble precipitates with oxalic acid. The plutonium oxalates are then easily thermally decomposed to form plutonium dioxide powder. This simple process forms the basis of current industrial conversion or 'finishing' processes that are used in commercial scale reprocessing plants. It is also widely used in analytical or laboratory scale operations and for waste residues treatment. However, the mechanisms of the thermal decompositions in both air and inert atmospheres have been the subject of various studies over several decades. The nature of intermediate phases is of fundamental interest whilst understanding the evolution of gases at different temperatures is relevant to process control. The thermal decomposition is also used to control a number of powder properties of the PuO2 product that are important to either long term storage or mixed oxide fuel manufacturing. These properties are the surface area, residual carbon impurities and adsorbed volatile species whereas the morphology and particle size distribution are functions of the precipitation process. Available data and experience regarding the thermal and radiation-induced decompositions of plutonium oxalate to oxide are reviewed. The mechanisms of the thermal decompositions are considered with a particular focus on the likely redox chemistry involved. Also, whilst it is well known that the surface area is dependent on calcination temperature, there is a wide variation in the published data and so new correlations have been derived. Better understanding of plutonium (III) and (IV) oxalate decompositions will assist the development of more proliferation resistant actinide co-conversion processes that are needed for advanced reprocessing in future closed nuclear fuel cycles.

PLUTONIUM CARRIER METATHESIS WITH ORGANIC REAGENT

DOEpatents

Thompson, S.G.

1958-07-01

A method is described for converting a plutonium containing bismuth phosphate carrier precipitate Into a compositton more readily soluble in acid. The method consists of dissolving the bismuth phosphate precipitate in an aqueous solution of alkali metal hydroxide, and adding one of a certaia group of organic compounds, e.g., polyhydric alcohols or a-hydrorycarboxylic acids. The mixture is then heated causiing formation of a bismuth hydroxide precipitate containing plutonium which may be readily dissolved in nitric acid for further processing.

Nonproliferation and Threat Reduction Assistance: U.S, Programs in the Former Soviet Union

DTIC Science & Technology

2008-03-26

reconfigure its large - scale former BW-related facilities so that they can perform peaceful research issues such as infectious diseases. For FY2004, the Bush...program to eliminate its plutonium, opting instead for the construction of fast breeder reactors that could burn plutonium directly for energy production...The United States might not fund this effort, as many in the United States argue that breeder reactors , which produce more plutonium than they

Utilization of non-weapons-grade plutonium and highly enriched uranium with breeding of the 233U isotope in the VVER reactors using thorium and heavy water

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.

Anthropogenic plutonium-244 in the environment: Insights into plutonium’s longest-lived isotope

DOE PAGES

Armstrong, Christopher R.; Brant, Heather A.; Nuessle, Patterson R.; ...

2016-02-22

Owing to the rich history of heavy element production in the unique high flux reactors that operated at the Savannah River Site, USA (SRS) decades ago, trace quantities of plutonium with highly unique isotopic characteristics still persist today in the SRS terrestrial environment. Development of an effective sampling, processing, and analysis strategy enables detailed monitoring of the SRS environment, revealing plutonium isotopic compositions, e.g., 244Pu, that reflect the unique legacy of plutonium production at SRS. This work describes the first long-term investigation of anthropogenic 244Pu occurrence in the environment. Environmental samples, consisting of collected foot borne debris, were taken atmore » SRS over an eleven year period, from 2003 to 2014. Separation and purification of trace plutonium was carried out followed by three stage thermal ionization mass spectrometry (3STIMS) measurements for plutonium isotopic content and isotopic ratios. Furthermore, significant 244Pu was measured in all of the years sampled with the highest amount observed in 2003. The 244Pu content, in femtograms (fg = 10 –15 g) per gram, ranged from 0.31 fg/g to 44 fg/g in years 2006 and 2003 respectively. In all years, the 244Pu/ 239Pu atom ratios were significantly higher than global fallout, ranging from 0.003 to 0.698 in years 2014 and 2003 respectively.« less

The benefits of an advanced fast reactor fuel cycle for plutonium management

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hannum, W.H.; McFarlane, H.F.; Wade, D.C.

1996-12-31

The United States has no program to investigate advanced nuclear fuel cycles for the large-scale consumption of plutonium from military and civilian sources. The official U.S. position has been to focus on means to bury spent nuclear fuel from civilian reactors and to achieve the spent fuel standard for excess separated plutonium, which is considered by policy makers to be an urgent international priority. Recently, the National Research Council published a long awaited report on its study of potential separation and transmutation technologies (STATS), which concluded that in the nuclear energy phase-out scenario that they evaluated, transmutation of plutonium andmore » long-lived radioisotopes would not be worth the cost. However, at the American Nuclear Society Annual Meeting in June, 1996, the STATS panelists endorsed further study of partitioning to achieve superior waste forms for burial, and suggested that any further consideration of transmutation should be in the context of energy production, not of waste management. 2048 The U.S. Department of Energy (DOE) has an active program for the short-term disposition of excess fissile material and a `focus area` for safe, secure stabilization, storage and disposition of plutonium, but has no current programs for fast reactor development. Nevertheless, sufficient data exist to identify the potential advantages of an advanced fast reactor metallic fuel cycle for the long-term management of plutonium. Advantages are discussed.« less

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

Technical Basis Document: A Statistical Basis for Interpreting Urinary Excretion of Plutonium Based on Accelerator Mass Spectrometry (AMS) for Selected Atoll Populations in the Marshall Islands

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bogen, K; Hamilton, T F; Brown, T A

2007-05-01

We have developed refined statistical and modeling techniques to assess low-level uptake and urinary excretion of plutonium from different population group in the northern Marshall Islands. Urinary excretion rates of plutonium from the resident population on Enewetak Atoll and from resettlement workers living on Rongelap Atoll range from <1 to 8 {micro}Bq per day and are well below action levels established under the latest Department regulation 10 CFR 835 in the United States for in vitro bioassay monitoring of {sup 239}Pu. However, our statistical analyses show that urinary excretion of plutonium-239 ({sup 239}Pu) from both cohort groups is significantly positivelymore » associated with volunteer age, especially for the resident population living on Enewetak Atoll. Urinary excretion of {sup 239}Pu from the Enewetak cohort was also found to be positively associated with estimates of cumulative exposure to worldwide fallout. Consequently, the age-related trends in urinary excretion of plutonium from Marshallese populations can be described by either a long-term component from residual systemic burdens acquired from previous exposures to worldwide fallout or a prompt (and eventual long-term) component acquired from low-level systemic intakes of plutonium associated with resettlement of the northern Marshall Islands, or some combination of both.« less

Anthropogenic plutonium-244 in the environment: Insights into plutonium’s longest-lived isotope

PubMed Central

Armstrong, Christopher R.; Brant, Heather A.; Nuessle, Patterson R.; Hall, Gregory; Cadieux, James R.

2016-01-01

Owing to the rich history of heavy element production in the unique high flux reactors that operated at the Savannah River Site, USA (SRS) decades ago, trace quantities of plutonium with highly unique isotopic characteristics still persist today in the SRS terrestrial environment. Development of an effective sampling, processing, and analysis strategy enables detailed monitoring of the SRS environment, revealing plutonium isotopic compositions, e.g., 244Pu, that reflect the unique legacy of plutonium production at SRS. This work describes the first long-term investigation of anthropogenic 244Pu occurrence in the environment. Environmental samples, consisting of collected foot borne debris, were taken at SRS over an eleven year period, from 2003 to 2014. Separation and purification of trace plutonium was carried out followed by three stage thermal ionization mass spectrometry (3STIMS) measurements for plutonium isotopic content and isotopic ratios. Significant 244Pu was measured in all of the years sampled with the highest amount observed in 2003. The 244Pu content, in femtograms (fg = 10−15 g) per gram, ranged from 0.31 fg/g to 44 fg/g in years 2006 and 2003 respectively. In all years, the 244Pu/239Pu atom ratios were significantly higher than global fallout, ranging from 0.003 to 0.698 in years 2014 and 2003 respectively. PMID:26898531

Multi-isotopic determination of plutonium (239Pu, 240Pu, 241Pu and 242Pu) in marine sediments using sector-field inductively coupled plasma mass spectrometry.

PubMed

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.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Friesen, H.N.

This summary document presents results in a broad context; it is not limited to findings of the Nevada Applied Ecology Group. This book is organized to present the findings of the Nevada Applied Ecology Group and correlative programs in accordance with the originally stated objectives of the Nevada Applied Ecology Group. This plan, in essence, traces plutonium from its injection into the environment to movement in the ecosystem to development of cleanup techniques. Information on other radionuclides was also obtained and will be presented briefly. Chapter 1 presents a brief description of the ecological setting of the Test Range Complex.more » The results of investigations for plutonium distribution are presented in Chapter 2 for the area surrounding the Test Range Complex and in Chapter 3 for on-site locations. Chapters 4 and 5 present the results of investigations concerned with concentrations and movement, respectively, of plutonium in the ecosystem of the Test Range Complex, and Chapter 6 summarizes the potential hazard from this plutonium. Development of techniques for cleanup and treatment is presented in Chapter 7, and the inventory of radionuclides other than plutonium is presented briefly in Chapter 8.« less

Evaluation of continuous air monitor placement in a plutonium facility.

PubMed

Whicker, J J; Rodgers, J C; Fairchild, C I; Scripsick, R C; Lopez, R C

1997-05-01

Department of Energy appraisers found continuous air monitors at Department of Energy plutonium facilities alarmed less than 30% of the time when integrated room plutonium air concentrations exceeded 500 DAC-hours. Without other interventions, this alarm percentage suggests the possibility that workers could be exposed to high airborne concentrations without continuous air monitor alarms. Past research has shown that placement of continuous air monitors is a critical component in rapid and reliable detection of airborne releases. At Los Alamos National Laboratory and many other Department of Energy plutonium facilities, continuous air monitors have been primarily placed at ventilation exhaust points. The purpose of this study was to evaluate and compare the effectiveness of exhaust register placement of workplace continuous air monitors with other sampling locations. Polydisperse oil aerosols were released from multiple locations in two plutonium laboratories at Los Alamos National Laboratory. An array of laser particle counters positioned in the rooms measured time-resolved aerosol dispersion. Results showed alternative placement of air samplers generally resulted in aerosol detection that was faster, often more sensitive, and equally reliable compared with samplers at exhaust registers.

Safe disposal of surplus plutonium

NASA Astrophysics Data System (ADS)

Gong, W. L.; Naz, S.; Lutze, W.; Busch, R.; Prinja, A.; Stoll, W.

2001-06-01

About 150 tons of weapons grade and weapons usable plutonium (metal, oxide, and in residues) have been declared surplus in the USA and Russia. Both countries plan to convert the metal and oxide into mixed oxide fuel for nuclear power reactors. Russia has not yet decided what to do with the residues. The US will convert residues into a ceramic, which will then be over-poured with highly radioactive borosilicate glass. The radioactive glass is meant to provide a deterrent to recovery of plutonium, as required by a US standard. Here we show a waste form for plutonium residues, zirconia/boron carbide (ZrO 2/B 4C), with an unprecedented combination of properties: a single, radiation-resistant, and chemically durable phase contains the residues; billion-year-old natural analogs are available; and criticality safety is given under all conceivable disposal conditions. ZrO 2/B 4C can be disposed of directly, without further processing, making it attractive to all countries facing the task of plutonium disposal. The US standard for protection against recovery can be met by disposal of the waste form together with used reactor fuel.

Methods to improve routine bioassay monitoring for freshly separated, poorly transported plutonium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bihl, D.E.; Lynch, T.P.; Carbaugh, E.H.

1988-09-01

Several human cases involving inhalation of plutonium oxide at Hanford have shown clearance half-times from the lung that are much longer than the 500-day half-time recommended for class Y plutonium in Publication 30 of the International Commission on Radiological Protection(ICRP). The more tenaciously retained material is referred to as super class Y plutonium. The ability to detect super class Y plutonium by current routine bioassay measurements is shown to be poor. Pacific Northwest Laboratory staff involved in the Hanford Internal Dosimetry Program investigated four methods to se if improvements in routine monitoring of workers for fresh super class Y plutoniummore » are feasible. The methods were lung counting, urine sampling, fecal sampling, and use of diethylenetriaminepentaacetate (DTPA) to enhance urinary excretion. Use of DTPA was determined to be not feasible. Routine fecal sampling was found to be feasible but not recommended. Recommendations were made to improve the detection level for routine annual urinalysis and routine annual lung counting. 12 refs., 9 figs., 7 tabs.« less

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

Digital pile-up rejection for plutonium experiments with solution-grown stilbene

NASA Astrophysics Data System (ADS)

Bourne, M. M.; Clarke, S. D.; Paff, M.; DiFulvio, A.; Norsworthy, M.; Pozzi, S. A.

2017-01-01

A solution-grown stilbene detector was used in several experiments with plutonium samples including plutonium oxide, mixed oxide, and plutonium metal samples. Neutrons from different reactions and plutonium isotopes are accompanied by numerous gamma rays especially by the 59-keV gamma ray of 241Am. Identifying neutrons correctly is important for nuclear nonproliferation applications and makes neutron/gamma discrimination and pile-up rejection necessary. Each experimental dataset is presented with and without pile-up filtering using a previously developed algorithm. The experiments were simulated using MCNPX-PoliMi, a Monte Carlo code designed to accurately model scintillation detector response. Collision output from MCNPX-PoliMi was processed using the specialized MPPost post-processing code to convert neutron energy depositions event-by-event into light pulses. The model was compared to experimental data after pulse-shape discrimination identified waveforms as gamma ray or neutron interactions. We show that the use of the digital pile-up rejection algorithm allows for accurate neutron counting with stilbene to within 2% even when not using lead shielding.

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.

Plutonium

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.

49 CFR 176.2 - Definitions.

Code of Federal Regulations, 2012 CFR

2012-10-01

..., spillage, or other accident. INF cargo means packaged irradiated nuclear fuel, plutonium or high-level... Irradiated Nuclear Fuel, Plutonium and High-Level Radioactive Wastes on Board Ships” (INF Code) contained in...

Electrorefining process and apparatus for recovery of uranium and a mixture of uranium and plutonium from spent fuels

DOEpatents

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.

Electrorefining process and apparatus for recovery of uranium and a mixture of uranium and plutonium from spent fuels

DOEpatents

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.

Ceramics: Durability and radiation effects

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ewing, R.C.; Lutze, W.; Weber, W.J.

1996-05-01

At present, there are three seriously considered options for the disposition of excess weapons plutonium: (1) incorporation, partial burn-up and direct disposal of MOX-fuel; (2) vitrification with defense waste and disposal as glass {open_quotes}logs{close_quotes}; (3) deep borehole disposal. The first two options provide a safeguard due to the high activity of fission products in the irradiated fuel and the defense waste. The latter option has only been examined in a preliminary manner, and the exact form of the plutonium has not been identified. In this paper, we review the potential for the immobilization of plutonium in highly durable crystalline ceramicsmore » apatite, pyrochlore, zirconolite, monazite and zircon. Based on available data, we propose zircon as the preferred crystalline ceramic for the permanent disposition of excess weapons plutonium.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

The Department of Energy (DOE) has contracted with Asea Brown Boveri-Combustion Engineering (ABB-CE) to provide information on the capability of ABB-CE`s System 80 + Advanced Light Water Reactor (ALWR) to transform, through reactor burnup, 100 metric tonnes (MT) of weapons grade plutonium (Pu) into a form which is not readily useable in weapons. This information is being developed as part of DOE`s Plutonium Disposition Study, initiated by DOE in response to Congressional action. This document, Volume 1, presents a technical description of the various elements of the System 80 + Standard Plant Design upon which the Plutonium Disposition Study wasmore » based. The System 80 + Standard Design is fully developed and directly suited to meeting the mission objectives for plutonium disposal. The bass U0{sub 2} plant design is discussed here.« less

Risks of fatal cancer from inhalation of 239,240plutonium by humans: a combined four-method approach with uncertainty evaluation.

PubMed

Grogan, H A; Sinclair, W K; Voillequé, P G

2001-05-01

The risk per unit dose to the four primary cancer sites for plutonium inhalation exposure (lung, liver, bone, bone marrow) is estimated by combining the risk estimates that are derived from four independent approaches. Each approach represents a fundamentally different source of data from which plutonium risk estimates can be derived. These are: (1) epidemiologic studies of workers exposed to plutonium; (2) epidemiologic studies of persons exposed to low-LET radiation combined with a factor for the relative biological effectiveness (RBE) of plutonium alpha particles appropriate for each cancer site of concern; (3) epidemiologic studies of persons exposed to alpha-emitting radionuclides other than plutonium; and (4) controlled studies of animals exposed to plutonium and other alpha-emitting radionuclides extrapolated to humans. This procedure yielded the following organ-specific estimates of the distribution of mortality risk per unit dose from exposure to plutonium expressed as the median estimate with the 5th to 95th percentiles of the distribution in parentheses: lung 0.13 Gy(-1) (0.022-0.53 Gy(-1)); liver 0.057 Gy(-1) (0.011-0.47 Gy(-1)); bone 0.0013 Gy(-1) (0.000060-0.025 Gy(-1)); bone marrow (leukemia), 0.013 Gy(-1) (0.00061-0.05 Gy(-1)). Because the different tissues do not receive the same dose following an inhalation exposure, the mortality risk per unit intake of activity via inhalation of a 1-microm AMAD plutonium aerosol also was determined. To do this, inhalation dose coefficients based on the most recent ICRP models and accounting for input parameter uncertainties were combined with the risk coefficients described above. The following estimates of the distribution of mortality risk per unit intake were determined for a 1-microm AMAD plutonium aerosol with a geometric standard deviation of 2.5: lung 5.3 x 10(-7) Bq(-1) (0.65-35 x 10(-7) Bq(-1)), liver 1.2 x 10(-7) Bq(-1) (0.091-20 x 10(-7) Bq(-1)), bone 0.11 x 10(-7) Bq(-1) (0.0030-4.3 x 10(-7) Bq(-1)), bone marrow (leukemia) 0.049 x 10(-7) Bq(-1) (0.0017-0.59 x 10(-7) Bq(-1)). The cancer mortality risk for all sites was estimated to be 10 x 10(-7) Bq(-1) (2.1-55 x 10(-7) Bq(-1))--a result that agrees very well with other recent estimates. The large uncertainties in the risks per unit intake of activity reflect the combined uncertainty in the dose and risk coefficients.

Plutonium Bioassay Testing of U.S. Atmospheric Nuclear Test Participants and U.S. Occupation Forces of Hiroshima and Nagasaki, Japan

DTIC Science & Technology

2015-10-30

with nuclear weapons testing or plutonium work. The results for the 100 atomic veterans were compared to those of the unexposed population, and...as a marker for significant internal intakes of other associated radionuclides in nuclear weapons debris due to its low natural background. However...isotope in weapons grade plutonium, is important from a health perspective, its presence within a given urine sample being analyzed by FTA can only

PRECIPITATION METHOD OF SEPARATION OF NEPTUNIUM

DOEpatents

Magnusson, L.B.

1958-07-01

A process is described for the separation of neptunium from plutonium in an aqueous solution containing neptunium ions in a valence state not greater than +4, plutonium ioms in a valence state not greater than +4, and sulfate ions. The Process consists of adding hypochlorite ions to said solution in order to preferentially oxidize the neptunium and then adding lanthanum ions and fluoride ions to form a precipitate of LaF/sub 3/ carrying the plutonium, and thereafter separating the supernatant solution from the precipitate.

Lens of Eye Dosimetry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mallett, Michael Wesley

An analysis of LANL occupational dose measurements was made with respect to lens of eye dose (LOE), in particular, for plutonium workers. Table 1 shows the reported LOE as a ratio of the “deep” (photon only) and “deep+neutron” dose for routine monitored workers at LANL for the past ten years. The data compares the mean and range of these values for plutonium workers* and non-routine plutonium workers. All doses were reported based on measurements with the LANL Model 8823 TLD.

Some neutron and gamma radiation characteristics of plutonium cermet fuel for isotopic power sources

NASA Technical Reports Server (NTRS)

Neff, R. A.; Anderson, M. E.; Campbell, A. R.; Haas, F. X.

1972-01-01

Gamma and neutron measurements on various types of plutonium sources are presented in order to show the effects of O-17, O-18 F-19, Pu-236, age of the fuel, and size of the source on the gamma and neutron spectra. Analysis of the radiation measurements shows that fluorine is the main contributor to the neutron yields from present plutonium-molybdenum cermet fuel, while both fluorine and Pu-236 daughters contribute significantly to the gamma ray intensities.

Utilization of non-weapons-grade plutonium and highly enriched uranium with breeding of the {sup 233}U isotope in the VVER reactors using thorium and heavy water

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.

Natural Transmutation of Actinides via the Fission Reaction in the Closed Thorium-Uranium-Plutonium Fuel Cycle

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.

METHOD OF SEPARATING URANIUM VALUES, PLUTONIUM VALUES AND FISSION PRODUCTS BY CHLORINATION

DOEpatents

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.

SCAVENGER AND PROCESS OF SCAVENGING

DOEpatents

Olson, C.M.

1960-04-26

Carrier precipitation processes are given for the separation and recovery of plutonium from aqueous acidic solutions containing plutonium and fission products. Bismuth phosphate is precipitated in the acidic solution while plutonlum is maintained in the hexavalent oxidation state. Preformed, uncalcined, granular titanium dioxide is then added to the solution and the fission product-carrying bismuth phosphate and titanium dioxide are separated from the resulting mixture. Fluosilicic acid, which dissolves any remaining titanium dioxide particles, is then added to the purified plutonium-containing solution.

METHOD FOR REMOVING CONTAMINATION FROM PRECIPITATES

DOEpatents

Stahl, G.W.

1959-01-01

An improvement in the bismuth phosphate carrier precipitation process is presented for the recovery and purification of plutonium. When plutonium, in the tetravalent state, is carried on a bismuth phosphate precipitate, amounts of centain of the fission products are carried along with the plutonium. The improvement consists in washing such fission product contaminated preeipitates with an aqueous solution of ammonium hydrogen fluoride. since this solution has been found to be uniquely effective in washing fission production contamination from the bismuth phosphate precipitate.

METHOD OF PREPARING URANIUM, THORIUM, OR PLUTONIUM OXIDES IN LIQUID BISMUTH

DOEpatents

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.

Two Dihydroxo-Bridged Plutonium(IV) Nitrate Dimers and Their Relevance to Trends in Tetravalent Ion Hydrolysis and Condensation

DOE PAGES

Knope, Karah E.; Skanthakumar, S.; Soderholm, L.

2015-10-13

We report the room temperature synthesis and structural characterization of a μ2-hydroxobridged PuIV dimer obtained from an acidic, nitric acid solution. The discrete Pu 2(OH) 2(NO 3) 6(H 2O) 4 moiety crystallized with two distinct crystal structures, (1) [Pu 2(OH) 2(NO 3) 6(H 2O) 4] 2·11H 2O and (2) Pu 2(OH) 2(NO 3) 6(H 2O) 4·2H 2O, which differ primarily in the number of incorporated water molecules. High-energy X-ray scattering (HEXS) data obtained from the mother liquor showed evidence of a correlation at 3.7(10) Å but only after concentration of the stock solution. This distance is consistent with the dihydroxo-bridgedmore » distance of 3.799(1) Å seen in the solid-state structure as well as with the known Pu-Pu distance in PuO 2. The structural characterization of a dihydroxo-bridged Pu moiety is discussed in terms of its relevance to the underlying mechanisms of tetravalent-metal-ion condensation« less

Transuranic Contamination in Sediment and Groundwater at the U.S. DOE Hanford Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cantrell, Kirk J.

2009-08-20

A review of transuranic radionuclide contamination in sediments and groundwater at the DOE’s Hanford Site was conducted. The review focused primarily on plutonium-239/240 and americium-241; however, other transuranic nuclides were discussed as well, including neptunium-237, plutonium-238, and plutonium-241. The scope of the review included liquid process wastes intentionally disposed to constructed waste disposal facilities such as trenches and cribs, burial grounds, and unplanned releases to the ground surface. The review did not include liquid wastes disposed to tanks or solid wastes disposed to burial grounds. It is estimated that over 11,800 Ci of plutonium-239, 28,700 Ci of americium-241, and 55more » Ci of neptunium-237 have been disposed as liquid waste to the near surface environment at the Hanford Site. Despite the very large quantities of transuranic contaminants disposed to the vadose zone at Hanford, only minuscule amounts have entered the groundwater. Currently, no wells onsite exceed the DOE derived concentration guide for plutonium-239/240 (30 pCi/L) or any other transuranic contaminant in filtered samples. The DOE derived concentration guide was exceeded by a small fraction in unfiltered samples from one well (299-E28-23) in recent years (35.4 and 40.4 pCi/L in FY 2006). The primary reason that disposal of these large quantities of transuranic radionuclides directly to the vadose zone at the Hanford Site has not resulted in widespread groundwater contamination is that under the typical oxidizing and neutral to slightly alkaline pH conditions of the Hanford vadose zone, transuranic radionuclides (plutonium and americium in particular) have a very low solubility and high affinity for surface adsorption to mineral surfaces common within the Hanford vadose zone. Other important factors are the fact that the vadose zone is typically very thick (hundreds of feet) and the net infiltration rate is very low due to the desert climate. In some cases where transuranic radionuclides have been co-disposed with acidic liquid waste, transport through the vadose zone for considerable distances has occurred. For example, at the 216-Z-9 Crib, plutonium-239 and americium-241 have moved to depths in excess of 36 m (118 ft) bgs. Acidic conditions increase the solubility of these contaminants and reduce adsorption to mineral surfaces. Subsequent neutralization of the acidity by naturally occurring calcite in the vadose zone (particularly in the Cold Creek unit) appears to have effectively stopped further migration. The vast majority of transuranic contaminants disposed to the vadose zone on the Hanford Site (10,200 Ci [86%] of plutonium-239; 27,900 Ci [97%] of americium-241; and 41.8 Ci [78%] of neptunium-237) were disposed in sites within the PFP Closure Zone. This closure zone is located within the 200 West Area (see Figures 1.1 and 3.1). Other closure zones with notably high quantities of transuranic contaminant disposal include the T Farm Zone with 408 Ci (3.5%) plutonium-239, the PUREX Zone with 330 Ci (2.8%) plutonium-239, 200-W Ponds Zone with 324 Ci (2.8%) plutonium-239, B Farm Zone with 183 Ci (1.6%) plutonium-239, and the REDOX Zone with 164 Ci (1.4%) plutonium 239. Characterization studies for most of the sites reviewed in the document are generally limited. The most prevalent characterization methods used were geophysical logging methods. Characterization of a number of sites included laboratory analysis of borehole sediment samples specifically for radionuclides and other contaminants, and geologic and hydrologic properties. In some instances, more detailed research level studies were conducted. Results of these studies were summarized in the document.« less

Transportability Class of Americium in K Basin Sludge under Ambient and Hydrothermal Processing Conditions

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

METHOD OF DISSOLVING MASSIVE PLUTONIUM

DOEpatents

Facer, J.F.; Lyon, W.L.

1960-06-28

Massive plutonium can be dissolved in a hot mixture of concentrated nitric acid and a small quantity of hydrofluoric acid. A preliminary oxidation with water under superatmospheric pressure at 140 to 150 deg C is advantageous

Pu-Zr alloy for high-temperature foil-type fuel

DOEpatents

McCuaig, Franklin D.

1977-01-01

A nuclear reactor fuel alloy consists essentially of from slightly greater than 7 to about 4 w/o zirconium, balance plutonium, and is characterized in that the alloy is castable and is rollable to thin foils. A preferred embodiment of about 7 w/o zirconium, balance plutonium, has a melting point substantially above the melting point of plutonium, is rollable to foils as thin as 0.0005 inch thick, and is compatible with cladding material when repeatedly cycled to temperatures above 650.degree. C. Neutron reflux densities across a reactor core can be determined with a high-temperature activation-measurement foil which consists of a fuel alloy foil core sandwiched and sealed between two cladding material jackets, the fuel alloy foil core being a 7 w/o zirconium, plutonium foil which is from 0.005 to 0.0005 inch thick.

Pu-ZR Alloy high-temperature activation-measurement foil

DOEpatents

McCuaig, Franklin D.

1977-08-02

A nuclear reactor fuel alloy consists essentially of from slightly greater than 7 to about 4 w/o zirconium, balance plutonium, and is characterized in that the alloy is castable and is rollable to thin foils. A preferred embodiment of about 7 w/o zirconium, balance plutonium, has a melting point substantially above the melting point of plutonium, is rollable to foils as thin as 0.0005 inch thick, and is compatible with cladding material when repeatedly cycled to temperatures above 650.degree. C. Neutron flux densities across a reactor core can be determined with a high-temperature activation-measurement foil which consists of a fuel alloy foil core sandwiched and sealed between two cladding material jackets, the fuel alloy foil core being a 7 w/o zirconium, plutonium foil which is from 0.005 to 0.0005 inch thick.

Separation by solvent extraction

DOEpatents

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.

Plutonium and uranium determination in environmental samples: combined solvent extraction-liquid scintillation method.

PubMed

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.

High temperature radiance spectroscopy measurements of solid and liquid uranium and plutonium carbides

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.

HB-Line Plutonium Oxide Data Collection Strategy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Watkins, R.; Varble, J.; Jordan, J.

2015-05-26

HB-Line and H-Canyon will handle and process plutonium material to produce plutonium oxide for feed to the Mixed Oxide Fuel Fabrication Facility (MFFF). However, the plutonium oxide product will not be transferred to the MFFF directly from HB-Line until it is packaged into a qualified DOE-STD-3013-2012 container. In the interim, HB-Line will load plutonium oxide into an inner, filtered can. The inner can will be placed in a filtered bag, which will be loaded into a filtered outer can. The outer can will be loaded into a certified 9975 with getter assembly in compliance with onsite transportation requirement, for subsequentmore » storage and transfer to the K-Area Complex (KAC). After DOE-STD-3013-2012 container packaging capabilities are established, the product will be returned to HB-Line to be packaged into a qualified DOE-STD-3013-2012 container. To support the transfer of plutonium oxide to KAC and then eventually to MFFF, various material and packaging data will have to be collected and retained. In addition, data from initial HB-Line processing operations will be needed to support future DOE-STD-3013-2012 qualification as amended by the HB-Line DOE Standard equivalency. As production increases, the volume of data to collect will increase. The HB-Line data collected will be in the form of paper copies and electronic media. Paper copy data will, at a minimum, consist of facility procedures, nonconformance reports (NCRs), and DCS print outs. Electronic data will be in the form of Adobe portable document formats (PDFs). Collecting all the required data for each plutonium oxide can will be no small effort for HB-Line, and will become more challenging once the maximum annual oxide production throughput is achieved due to the sheer volume of data to be collected. The majority of the data collected will be in the form of facility procedures, DCS print outs, and laboratory results. To facilitate complete collection of this data, a traveler form will be developed which identifies the required facility procedures, DCS print outs, and laboratory results needed to assemble a final data package for each HB-Line plutonium oxide interim oxide can. The data traveler may identify the specific values (data) required to be extracted from the collected facility procedures and DCS print outs. The data traveler may also identify associated criteria to be checked. Inevitably there will be procedure anomalies during the course of the HB-Line plutonium oxide campaign that will have to be addressed in a timely manner.« less

241Am Ingrowth and Its Effect on Internal Dose

DOE PAGES

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

MIS High-Purity Plutonium Oxide Metal Oxidation Product TS707001 (SSR123): Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Veirs, Douglas Kirk; Stroud, Mary Ann; Berg, John M.

A high-purity plutonium dioxide material from the Material Identification and Surveillance (MIS) Program inventory has been studied with regard to gas generation and corrosion in a storage environment. Sample TS707001 represents process plutonium oxides from several metal oxidation operations as well as impure and scrap plutonium from Hanford that are currently stored in 3013 containers. After calcination to 950°C, the material contained 86.98% plutonium with no major impurities. This study followed over time, the gas pressure of a sample with nominally 0.5 wt% water in a sealed container with an internal volume scaled to 1/500th of the volume of amore » 3013 container. Gas compositions were measured periodically over a six year period. The maximum observed gas pressure was 138 kPa. The increase over the initial pressure of 80 kPa was primarily due to generation of nitrogen and carbon dioxide gas in the first six months. Hydrogen and oxygen were minor components of the headspace gas. At the completion of the study, the internal components of the sealed container showed signs of corrosion, including pitting.« 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

PLUTONIUM PURIFICATION PROCESS EMPLOYING THORIUM PYROPHOSPHATE CARRIER

DOEpatents

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.

Fuel Sustainability And Actinide Production Of Doping Minor Actinide In Water-Cooled Thorium Reactor

NASA Astrophysics Data System (ADS)

Permana, Sidik

2017-07-01

Fuel sustainability of nuclear energy is coming from an optimum fuel utilization of the reactor and fuel breeding program. Fuel cycle option becomes more important for fuel cycle utilization as well as fuel sustainability capability of the reactor. One of the important issues for recycle fuel option is nuclear proliferation resistance issue due to production plutonium. To reduce the proliferation resistance level, some barriers were used such as matrial barrier of nuclear fuel based on isotopic composition of even mass number of plutonium isotope. Analysis on nuclear fuel sustainability and actinide production composition based on water-cooled thorium reactor system has been done and all actinide composition are recycled into the reactor as a basic fuel cycle scheme. Some important parameters are evaluated such as doping composition of minor actinide (MA) and volume ratio of moderator to fuel (MFR). Some feasible parameters of breeding gains have been obtained by additional MA doping and some less moderation to fuel ratios (MFR). The system shows that plutonium and MA are obtained low compositions and it obtains some higher productions of even mass plutonium, which is mainly Pu-238 composition, as a control material to protect plutonium to be used as explosive devices.

75 FR 61225 - Energy Northwest; Columbia Generating Station Environmental Assessment and Finding of No...

Federal Register 2010, 2011, 2012, 2013, 2014

2010-10-04

..., fission products, some plutonium-contaminated waste, and toxicological waste. The DOE intends to remediate... through 1967 and contains low- to high-activity waste, fission products, some plutonium-contaminated waste...

Development of the Direct Fabrication Process for Plutonium Immobilization

DOE Office of Scientific and Technical Information (OSTI.GOV)

Congdon, J.W.

2001-07-10

The current baseline process for fabricating pucks for the Plutonium Immobilization Program includes granulation of the milled feed prior to compaction. A direct fabrication process was demonstrated that eliminates the need for granulation.

Plutonium oxalate precipitation for trace elemental determination in plutonium materials

DOE PAGES

Xu, Ning; Gallimore, David; Lujan, Elmer; ...

2015-05-26

In this study, an analytical chemistry method has been developed that removes the plutonium (Pu) matrix from the dissolved Pu metal or oxide solution prior to the determination of trace impurities that are present in the metal or oxide. In this study, a Pu oxalate approach was employed to separate Pu from trace impurities. After Pu(III) was precipitated with oxalic acid and separated by centrifugation, trace elemental constituents in the supernatant were analyzed by inductively coupled plasma-optical emission spectroscopy with minimized spectral interferences from the sample matrix.

Ferric ion as a scavenging agent in a solvent extraction process

DOEpatents

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.

A continuous plutonium aerosol monitor for use in high radon environments.

PubMed

Li, HuiBin; Jia, MingYan; Li, GuoShen; Wang, YinDong

2012-01-01

Radon concentration is very high in underground basements and other facilities. Radon concentration in a nuclear facility locates in the granite tunnel can be as high as 10(4) Bq m(-3) in summer. Monitoring plutonium aerosol in this circumstance is seriously interfered by radon daughters. In order to solve this problem, a new continuous aerosol monitor that can monitor very low plutonium aerosol concentration in high radon background was developed. Several techniques were used to reduce interference of radon daughters, and the minimum detectable concentrations in various radon concentrations were measured.

Forensic investigation of plutonium metal: a case study of CRM 126

DOE PAGES

Byerly, Benjamin L.; Stanley, Floyd; Spencer, Khal; ...

2016-11-01

In our study, a certified plutonium metal reference material (CRM 126) with a known production history is examined using analytical methods that are commonly employed in nuclear forensics for provenancing and attribution. Moreover, the measured plutonium isotopic composition and actinide assay are consistent with values reported on the reference material certificate. Model ages from U/Pu and Am/Pu chronometers agree with the documented production timeline. Finally, these results confirm the utility of these analytical methods and highlight the importance of a holistic approach for forensic study of unknown materials.

SULFIDE METHOD PLUTONIUM SEPARATION

DOEpatents

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.

[Contents of plutonium and microelements in the hair of Belarus inhabitants living in the areas contaminated during the Chernobyl AES accident].

PubMed

Malenchenko, A F; Bazhanova, N N; Kanash, N V; Zhuk, I V; Lomonosova, E M; Bulyga, S F

1997-01-01

The levels of plutonium were studied in the body of inhabitants of the Minsk and Gomel Regions. Their hair was used as the indicator of its levels. The hair concentrations of plutonium correlated with its content in the ribs. The hair levels of lead in the inhabitants of some populated localities of the Gomel Region were found to be higher than those in the residents of unpolluted areas and industrial centers of the Republic of Belarus.

Isotopic Analysis of Plutonium by Optical Spectroscopy; ANALYSE ISOTOPIQUE DU PLUTONIUM PAR SPECTROSCOPIE OPTIQUE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Artaud, J.; Chaput, M.; Gerstenkorn, S.

1961-01-01

Isotopic analyses of mixtures of plutonium-239 and -240 were carried out by means of the photoelectric spectrometer, the source being a hollow cathode cooled by liquid nitrogen. The relative precision is of the order of 2%, for samples containieg 3% of Pu/sup 240/. The study of the reproductibility of the measurements should make it possible to increase the precision; the relative precision which can be expected from the method should be 1% for mixtures containing 1% of Pu/sup 240/. (auth)

Neptunium and plutonium complexes with a sterically encumbered triamidoamine (TREN) scaffold

DOE PAGES

Brown, Jessie L.; Gaunt, Andrew J.; King, David M.; ...

2016-03-11

Here, the syntheses and characterization of isostructural neptunium(IV) and plutonium(IV) complexes [M IV(TREN TIPS)(Cl)] [An = Np, Pu; TREN TIPS = {N(CH 2CH 2NSiPr i 3) 3} 3] are reported, along with the demonstration that they are likely reduced to the corresponding neptunium(III) and plutonium(III) products [M III(TREN TIPS)]; this chemistry provides new platforms from which to target a plethora of unprecedented molecular functionalities in transuranic chemistry and the neptunium(IV) molecule is the first structurally characterized neptunium(IV)–amide complex.

The instrumental method of plutonium determination

NASA Astrophysics Data System (ADS)

Knyazev, B. B.; Kazachevskiy, I. V.; Solodukhin, V. P.; Lukashenko, S. N.; Knatova, M. K.; Kashirskiy, V. V.

2003-01-01

A method of direct instrumental determination of plutonium isotopes in soil samples is described. For the method a special program of spectra processing and activity calculation had to be prepared. The detection limit of 239+240Pu in absence of interfering radiation is about 200 Bq/kg (by 3.3σ criteria). Examples are given of the method application for the study of radionuclide soil composition in separate objects of Semipalatinsk Nuclear Test Site (SNTS). It is shown that for different objects under study the correlation degree between plutonium and americium activities may change rather substantially.

Dehydration of plutonium or neptunium trichloride hydrate

DOEpatents

Foropoulos, Jr., Jerry; Avens, Larry R.; Trujillo, Eddie A.

1992-01-01

A process of preparing anhydrous actinide metal trichlorides of plutonium or neptunium by reacting an aqueous solution of an actinide metal trichloride selected from the group consisting of plutonium trichloride or neptunium trichloride with a reducing agent capable of converting the actinide metal from an oxidation state of +4 to +3 in a resultant solution, evaporating essentially all the solvent from the resultant solution to yield an actinide trichloride hydrate material, dehydrating the actinide trichloride hydrate material by heating the material in admixture with excess thionyl chloride, and recovering anhydrous actinide trichloride is provided.

Dehydration of plutonium or neptunium trichloride hydrate

DOEpatents

Foropoulos, J. Jr.; Avens, L.R.; Trujillo, E.A.

1992-03-24

A process is described for preparing anhydrous actinide metal trichlorides of plutonium or neptunium by reacting an aqueous solution of an actinide metal trichloride selected from the group consisting of plutonium trichloride or neptunium trichloride with a reducing agent capable of converting the actinide metal from an oxidation state of +4 to +3 in a resultant solution, evaporating essentially all the solvent from the resultant solution to yield an actinide trichloride hydrate material, dehydrating the actinide trichloride hydrate material by heating the material in admixture with excess thionyl chloride, and recovering anhydrous actinide trichloride.

URANIUM DECONTAMINATION WITH RESPECT TO ZIRCONIUM

DOEpatents

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.

Volatile molecule PuO 3 observed from subliming plutonium dioxide

NASA Astrophysics Data System (ADS)

Ronchi, C.; Capone, F.; Colle, J. Y.; Hiernaut, J. P.

2000-06-01

Mass spectrometric measurements of effusing vapours over PuO 2 and (U, Pu)O 2 indicate the presence of volatile PuO 3 (g) molecules. The formation of plutonium trioxide vapour is due to a chemical process involving oxygen adsorbed during oxidation of the sample. Although in the examined samples, the fraction of trioxide effusing in vacuo was of the order of 0.02 ppm of the plutonium content, under steady-state oxidation conditions it has been shown that the process can have a relevant effect on the sublimation rate of the dioxide.

METHOD FOR PREPARING URANIUM MONOCARBIDE-PLUTONIUM MONOCARBIDE SOLID SOLUTION

DOEpatents

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)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

The Department of Energy (DOE) has contracted with Asea Brown Boveri-Combustion Engineering (ABB-CE) to provide information on the capability of ABB-CE`s System 80 + Advanced Light Water Reactor (ALWR) to transform, through reactor burnup, 100 metric tonnes (MT) of weapons grade plutonium (Pu) into a form which is not readily useable in weapons. This information is being developed as part of DOE`s Plutonium Disposition Study, initiated by DOE in response to Congressional action. This document Volume 2, provides a discussion of: Plutonium Fuel Cycle; Technology Needs; Regulatory Considerations; Cost and Schedule Estimates; and Deployment Strategy.

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

Decorporation Approach after Rat Lung Contamination with Plutonium: Evaluation of the Key Parameters Influencing the Efficacy of a Protracted Chelation Treatment.

PubMed

Grémy, Olivier; Coudert, Sylvie; Renault, Daniel; Miccoli, Laurent

2017-11-01

While the efficacy of a protracted zinc (Zn)- or calcium (Ca)-diethylenetriaminepentaacetic acid (DTPA) treatment in reducing transuranic body burden has already been demonstrated, questions about therapeutic variables remain. In response to this, we designed animal experiments primarily to assess both the effect of fractionation of a given dose and the effect of the frequency of dose fraction, with the same total dose. In our study, rats were contaminated intravenously with plutonium (Pu) then treated several days later with Ca-DTPA given at once or in various split-dose regimens cumulating to the same total dose and spread over several days. Similar efficacies were induced by the injection of the total dose or by splitting the dose in several smaller doses, independent of the number of doses and the dose level per injection. In a second study, rats were pulmonary contaminated, and three weeks later they received a Ca-DTPA dose 11-fold higher than the maximal daily recommended dose, administered either as a single bolus or as numerous multiple injections cumulating to the same dose, based on different injection frequency schedules. Independent of frequency schedule, the various split-dose regimens spread over weeks/months were as efficient as single delivery of the total dose in mobilizing lung plutonium, and had a therapeutic advantage for removal of retained hepatic and bone plutonium burdens. We concluded that cumulative dose level was a therapeutic variable of greater importance than the distribution of split doses for the success of a repeated treatment regimen on retained tissue plutonium. In addition, pulmonary administration of clodronate, which aims at killing alveolar macrophages and subsequently releasing their plutonium content, and which is associated with a continuous Ca-DTPA infusion regimen, suggested that the efficacy of injected Ca-DTPA in decorporating lung deposit is limited, due to its restricted penetration into alveolar macrophages and not because plutonium, as a physicochemical form, is unavailable for chelation.

Plutonium age dating reloaded

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.

Determination of ultra-low level plutonium isotopes (239Pu, 240Pu) in environmental samples with high uranium.

PubMed

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.

Process for immobilizing plutonium into vitreous ceramic waste forms

DOEpatents

Feng, Xiangdong; Einziger, Robert E.

1997-01-01

Disclosed is a method for converting spent nuclear fuel and surplus plutonium into a vitreous ceramic final waste form wherein spent nuclear fuel is bound in a crystalline matrix which is in turn bound within glass.

Process for immobilizing plutonium into vitreous ceramic waste forms

DOEpatents

Feng, X.; Einziger, R.E.

1997-08-12

Disclosed is a method for converting spent nuclear fuel and surplus plutonium into a vitreous ceramic final waste form wherein spent nuclear fuel is bound in a crystalline matrix which is in turn bound within glass.

Process for immobilizing plutonium into vitreous ceramic waste forms

DOEpatents

Feng, X.; Einziger, R.E.

1997-01-28

Disclosed is a method for converting spent nuclear fuel and surplus plutonium into a vitreous ceramic final waste form wherein spent nuclear fuel is bound in a crystalline matrix which is in turn bound within glass.

68. INTERIOR SHOT OF ENTRANCE TO BUILDING 272 (PLUTONIUM STORAGE ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

68. INTERIOR SHOT OF ENTRANCE TO BUILDING 272 (PLUTONIUM STORAGE BUILDING) LOOKING WEST. - Loring Air Force Base, Weapons Storage Area, Northeastern corner of base at northern end of Maine Road, Limestone, Aroostook County, ME

Selected environmental plutonium research reports of the NAEG

DOE Office of Scientific and Technical Information (OSTI.GOV)

White, M.G.; Dunaway, P.B.

Twenty-one papers were presented on various aspects of plutonium and radioisotope ecology at the Nevada Test Site. This includes studies of wildlife, microorganisms, and the plant-soil system. Analysis and sampling techniques are also included.

Lattice dynamics and elasticity for ε-plutonium [First-principles lattice dynamics for ε-plutonium

DOE PAGES

Söderlind, Per

2017-04-25

Here, lattice dynamics and elasticity for the high-temperature ε phase (body-centered cubic; bcc) of plutonium is predicted utilizing first-principles electronic structure coupled with a self-consistent phonon method that takes phonon-phonon interaction and strong anharmonicity into account. These predictions establish the first sensible lattice-dynamics and elasticity data on ε-Pu. The atomic forces required for the phonon scheme are highly accurate and derived from the total energies obtained from relativistic and parameter-free density-functional theory. The results appear reasonable but no data exist to compare with except those from dynamical mean-field theory that suggest ε-plutonium is mechanically unstable. Fundamental knowledge and understanding ofmore » the high-temperature bcc phase, that is generally present in all actinide metals before melting, is critically important for a proper interpretation of the phase diagram as well as practical modeling of high-temperature properties.« less

Guide of good practices for occupational radiological protection in plutonium facilities

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

1998-06-01

This Technical Standard (TS) does not contain any new requirements. Its purpose is to provide guides to good practice, update existing reference material, and discuss practical lessons learned relevant to the safe handling of plutonium. the technical rationale is given to allow US Department of Energy (DOE) health physicists to adapt the recommendations to similar situations throughout the DOE complex. Generally, DOE contractor health physicists will be responsible to implement radiation protection activities at DOE facilities and DOE health physicists will be responsible for oversight of those activities. This guidance is meant to be useful for both efforts. This TSmore » replaces PNL-6534, Health Physics Manual of Good Practices for Plutonium Facilities, by providing more complete and current information and by emphasizing the situations that are typical of DOE`s current plutonium operations; safe storage, decontamination, and decommissioning (environmental restoration); and weapons disassembly.« less

Verification study of an emerging fire suppression system

DOE PAGES

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

DOEpatents

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.

Plutonium working group report on environmental, safety and health vulnerabilities associated with the department`s plutonium storage. Volume II, Appendix B, Part 9: Oak Ridge site site team report

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

1994-09-01

This report provides the input to and results of the Department of Energy (DOE) - Oak Ridge Operations (ORO) DOE Plutonium Environment, Safety and Health (ES & H) Vulnerability Assessment (VA) self-assessment performed by the Site Assessment Team (SAT) for the Oak Ridge National Laboratory (ORNL or X-10) and the Oak Ridge Y-12 Plant (Y-12) sites that are managed by Martin Marietta Energy Systems, Inc. (MMES). As initiated (March 15, 1994) by the Secretary of Energy, the objective of the VA is to identify and rank-order DOE-ES&H vulnerabilities associated for the purpose of decision making on the interim safe managementmore » and ultimate disposition of fissile materials. This assessment is directed at plutonium and other co-located transuranics in various forms.« less

Fuzzy-probabilistic model for risk assessment of radioactive material railway transportation.

PubMed

Avramenko, M; Bolyatko, V; Kosterev, V

2005-01-01

Transportation of radioactive materials is obviously accompanied by a certain risk. A model for risk assessment of emergency situations and terrorist attacks may be useful for choosing possible routes and for comparing the various defence strategies. In particular, risk assessment is crucial for safe transportation of excess weapons-grade plutonium arising from the removal of plutonium from military employment. A fuzzy-probabilistic model for risk assessment of railway transportation has been developed taking into account the different natures of risk-affecting parameters (probabilistic and not probabilistic but fuzzy). Fuzzy set theory methods as well as standard methods of probability theory have been used for quantitative risk assessment. Information-preserving transformations are applied to realise the correct aggregation of probabilistic and fuzzy parameters. Estimations have also been made of the inhalation doses resulting from possible accidents during plutonium transportation. The obtained data show the scale of possible consequences that may arise from plutonium transportation accidents.

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

Late-occurring pulmonary pathologies following inhalation of mixed oxide (uranium + plutonium oxide) aerosol in the rat.

PubMed

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.

Rapid Method for Sodium Hydroxide Fusion of Asphalt ...

EPA Pesticide Factsheets

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.

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.

PREPARATION OF PuF$sub 3$

DOEpatents

Benz, R.

1964-03-01

A process for preparing pure plutonium trifluoride is described in which a refractory plutonium compound is contacted with ammonium fluoride in a closed container at a pressure of at least 10 atmospheres and a temperature of about 550 deg C. (AEC)

A relativistic density functional study of the role of 5f electrons in atomic and molecular adsorptions on actinide surfaces

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.

SEPARATION OF FISSION PRODUCTS FROM PLUTONIUM BY PRECIPITATION

DOEpatents

Seaborg, G.T.; Thompson, S.G.; Davidson, N.R.

1959-09-01

Fission product separation from hexavalent plutonium by bismuth phosphate precipitation of the fission products is described. The precipitation, according to this invention, is improved by coprecipitating ceric and zirconium phosphates (0.05 to 2.5 grams/liter) with the bismuth phosphate.

70. INTERIOR, BUILDING 272 (PLUTONIUM STORAGE BUILDING) LOOKING WEST INTO ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

70. INTERIOR, BUILDING 272 (PLUTONIUM STORAGE BUILDING) LOOKING WEST INTO STORAGE AREA SHOWING THE FOUR STORAGE ROOM ENTRANCES. - Loring Air Force Base, Weapons Storage Area, Northeastern corner of base at northern end of Maine Road, Limestone, Aroostook County, ME

Dissolution of aerosol particles collected from nuclear facility plutonium production process

DOE PAGES

Xu, Ning; Martinez, Alexander; Schappert, Michael Francis; ...

2015-08-14

Here, a simple, robust analytical chemistry method has been developed to dissolve plutonium containing particles in a complex matrix. The aerosol particles collected on Marple cascade impactor substrates were shown to be dissolved completely with an acid mixture of 12 M HNO 3 and 0.1 M HF. A pressurized closed vessel acid digestion technique was utilized to heat the samples at 130 °C for 16 h to facilitate the digestion. The dissolution efficiency for plutonium particles was 99 %. The resulting particle digestate solution was suitable for trace elemental analysis and isotope composition determination, as well as radiochemistry measurements.

Calculation of effective plutonium cross sections and check against the oscillation experiment CESAR-II

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schaal, H.; Bernnat, W.

1987-10-01

For calculations of high-temperature gas-cooled reactors with low-enrichment fuel, it is important to know the plutonium cross sections accurately. Therefore, a calculational method was developed, by which the plutonium cross-section data of the ENDF/B-IV library can be examined. This method uses zero- and one-dimensional neutron transport calculations to collapse the basic data into one-group cross sections, which then can be compared with experimental values obtained from integral tests. For comparison the data from the critical experiment CESAR-II of the Centre d'Etudes Nucleaires, Cadarache, France, were utilized.

XANES Identification of Plutonium Speciation in RFETS Samples

DOE Office of Scientific and Technical Information (OSTI.GOV)

LoPresti, V.; Conradson, S.D.; Clark, D.L.

2009-06-03

Using primarily X-ray absorption near edge spectroscopy (XANES) with standards run in tandem with samples, probable plutonium speciation was determined for 13 samples from contaminated soil, acid-splash or fire-deposition building interior surfaces, or asphalt pads from the Rocky Flats Environmental Technology Site (RFETS). Save for extreme oxidizing situations, all other samples were found to be of Pu(IV) speciation, supporting the supposition that such contamination is less likely to show mobility off site. EXAFS analysis conducted on two of the 13 samples supported the validity of the XANES features employed as determinants of the plutonium valence.

Validation of MCNP6 Version 1.0 with the ENDF/B-VII.1 Cross Section Library for Plutonium Metals, Oxides, and Solutions on the High Performance Computing Platform Moonlight

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chapman, Bryan Scott; Gough, Sean T.

This report documents a validation of the MCNP6 Version 1.0 computer code on the high performance computing platform Moonlight, for operations at Los Alamos National Laboratory (LANL) that involve plutonium metals, oxides, and solutions. The validation is conducted using the ENDF/B-VII.1 continuous energy group cross section library at room temperature. The results are for use by nuclear criticality safety personnel in performing analysis and evaluation of various facility activities involving plutonium materials.

FUSED SALT PROCESS FOR RECOVERY OF VALUES FROM USED NUCLEAR REACTOR FUELS

DOEpatents

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.

Multiple recycle of REMIX fuel based on reprocessed uranium and plutonium mixture in thermal reactors

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)

A rapid method for quantification of 242Pu in urine using extraction chromatography and ICP-MS

DOE PAGES

Gallardo, Athena Marie; Than, Chit; Wong, Carolyn; ...

2017-01-01

Occupational exposure to plutonium is generally monitored through analysis of urine samples. Typically, plutonium is separated from the sample and other actinides, and the concentration is determined using alpha spectroscopy. Current methods for separations and analysis are lengthy and require long count times. A new method for monitoring occupational exposure levels of plutonium has been developed, which requires fewer steps and overall less time than the alpha spectroscopy method. In this method, the urine is acidified, and a 239Pu internal standard is added. The urine is digested in a microwave oven, and plutonium is separated using an Eichrom TRU Resinmore » column. The plutonium is eluted, and the eluant is injected directly into the Inductively Coupled Plasma–Mass Spectrometer (ICP-MS). Compared to a direct “dilute and shoot” method, a 30-fold improvement in sensitivity is achieved. This method was validated by analyzing several batches of spiked samples. Based on these analyses, a combined standard uncertainty plot, which relates uncertainty to concentration, was produced. As a result, the MDA 95 was calculated to be 7.0 × 10 –7 μg L –1, and the Lc95 was calculated to be 3.5 × 10 –7 μg L –1 for this method.« less

Plutonium isotopes offer an alternative approach to establishing chronological profiles in coarse sediments

NASA Astrophysics Data System (ADS)

Pondell, C.; Kuehl, S. A.; Canuel, E. A.

2016-12-01

There are several methodologies used to determine chronologies for sediments deposited within the past 100 years, including 210Pb and 137Cs radioisotopes and organic and inorganic contaminants. These techniques are quite effective in fine sediments, which generally have a high affinity for metals and organic compounds. However, the application of these chronological tools becomes limited in systems where coarse sediments accumulate. Englebright Lake is an impoundment in northern California where sediment accumulation is characterized by a combination of fine and coarse sediments. This combination of sediment grain size complicated chronological analysis using the more traditional 137Cs chronological approach. This study established a chronology of these sediments using 239+240Pu isotopes. While most of the 249+240Pu activity was measured in the fine grain size fraction (<63 microns), up to 25% of the plutonium activity was detected in the coarse size fractions of sediments from Englebright Lake. Profiles of 239+240Pu were similar to available 137Cs profiles, verifying the application of plutonium isotopes for determining sediment chronologies and expanding the established geochronology for Englebright Lake sediments. This study of sediment accumulation in Englebright Lake demonstrates the application of plutonium isotopes in establishing chronologies in coarse sediments and highlights the potential for plutonium to offer new insights into patterns of coarse sediment accumulation.

Preparation, certification and validation of a stable solid spike of uranium and plutonium coated with a cellulose derivative for the measurement of uranium and plutonium content in dissolved nuclear fuel by isotope dilution mass spectrometry.

PubMed

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.

Transport of plutonium in snowmelt run-off

DOE Office of Scientific and Technical Information (OSTI.GOV)

Purtymun, W.D.; Peters, R.; Maes, M.N.

1990-07-01

Plutonium in treated low-level radioactive effluents released into intermittent streams is bound by ion exchange or adsorption to bed sediments in the stream channel. These sediments are subject to transport with summer and spring snowmelt run-off. A study was made of the transport of plutonium during seven spring run-off events in Los Alamos and Pueblo canyons from the Laboratory boundary to Otowi on the Rio Grande. The melting of the snowpack during these years resulted in run-off that was large enough to reach the eastern edge of the Laboratory. Of these seven run-off events recorded at the Laboratory boundary, onlymore » five had sufficient flow to reach the Rio Grande. The volume of the five events that reached the river ranged from 5 {times} 10{sup 3} m{sup 3} to 104 {times} 10{sup 3} m{sup 3}. The five run-off events carried 119 {times} 10{sup 3} kg of suspended sediments and 1073 {times} 10{sup 3} kg of bed sediments, and transported 598 {mu}Ci of plutonium to the river. Of the 598 {mu}Ci of plutonium, 3% was transported in solution, 57% with suspended sediments, and 40% with bed sediments. 13 refs., 3 figs., 6 tabs.« less

Determination of filter pore size for use in HB line phase II production of plutonium oxide

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shehee, T.; Crowder, M.; Rudisill, T.

2014-08-01

H-Canyon and HB-Line are tasked with the production of plutonium oxide (PuO 2) from a feed of plutonium (Pu) metal. The PuO 2 will provide feed material for the Mixed Oxide (MOX) Fuel Fabrication Facility. After dissolution of the Pu metal in H-Canyon, plans are to transfer the solution to HB-Line for purification by anion exchange. Anion exchange will be followed by plutonium(IV) oxalate precipitation, filtration, and calcination to form PuO 2. The filtrate solutions, remaining after precipitation, contain low levels of Pu ions, oxalate ions, and may include solids. These solutions are transferred to H-Canyon for disposition. To mitigatemore » the criticality concern of Pu solids in a Canyon tank, past processes have used oxalate destruction or have pre-filled the Canyon tank with a neutron poison. The installation of a filter on the process lines from the HB-Line filtrate tanks to H-Canyon Tank 9.6 is proposed to remove plutonium oxalate solids. This report describes SRNL’s efforts to determine the appropriate pore size for the filters needed to perform this function. Information provided in this report aids in developing the control strategies for solids in the process.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Armstrong, Christopher R.; Brant, Heather A.; Nuessle, Patterson R.

Owing to the rich history of heavy element production in the unique high flux reactors that operated at the Savannah River Site, USA (SRS) decades ago, trace quantities of plutonium with highly unique isotopic characteristics still persist today in the SRS terrestrial environment. Development of an effective sampling, processing, and analysis strategy enables detailed monitoring of the SRS environment, revealing plutonium isotopic compositions, e.g., 244Pu, that reflect the unique legacy of plutonium production at SRS. This work describes the first long-term investigation of anthropogenic 244Pu occurrence in the environment. Environmental samples, consisting of collected foot borne debris, were taken atmore » SRS over an eleven year period, from 2003 to 2014. Separation and purification of trace plutonium was carried out followed by three stage thermal ionization mass spectrometry (3STIMS) measurements for plutonium isotopic content and isotopic ratios. Furthermore, significant 244Pu was measured in all of the years sampled with the highest amount observed in 2003. The 244Pu content, in femtograms (fg = 10 –15 g) per gram, ranged from 0.31 fg/g to 44 fg/g in years 2006 and 2003 respectively. In all years, the 244Pu/ 239Pu atom ratios were significantly higher than global fallout, ranging from 0.003 to 0.698 in years 2014 and 2003 respectively.« less

Oxygen potential of uranium--plutonium oxide as determined by controlled- atmosphere thermogravimetry

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

A perspective on the proliferation risks of plutonium mines

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lyman, E.S.

1996-05-01

The program of geologic disposal of spent fuel and other plutonium-containing materials is increasingly becoming the target of criticism by individuals who argue that in the future, repositories may become low-cost sources of fissile material for nuclear weapons. This paper attempts to outline a consistent framework for analyzing the proliferation risks of these so-called {open_quotes}plutonium mines{close_quotes} and putting them into perspective. First, it is emphasized that the attractiveness of plutonium in a repository as a source of weapons material depends on its accessibility relative to other sources of fissile material. Then, the notion of a {open_quotes}material production standard{close_quotes} (MPS) ismore » proposed: namely, that the proliferation risks posed by geologic disposal will be acceptable if one can demonstrate, under a number of reasonable scenarios, that the recovery of plutonium from a repository is likely to be as difficult as new production of fissile material. A preliminary analysis suggests that the range of circumstances under which current mined repository concepts would fail to meet this standard is fairly narrow. Nevertheless, a broad application of the MPS may impose severe restrictions on repository design. In this context, the relationship of repository design parameters to easy of recovery is discussed.« less

The First Weighing of Plutonium

DOE R&D Accomplishments Database

Seaborg, Glenn T.

1967-09-10

Recollections and reminiscences at the 25th Anniversary of the First Weighing of Plutonium, Chicago, IL, September 10, 1967, tell an important part of the story of this fascinating new element that is destined to play an increasingly significant role in the future of man.

Cleaning up the Legacy of the Cold War: Plutonium Oxides and the Role of Synchrotron Radiation Research

DOE Office of Scientific and Technical Information (OSTI.GOV)

Clark, David Lewis

2015-01-21

The deceptively simple binary formula of AnO 2 belies an incredibly complex structural nature, and propensity to form mixed-valent, nonstoichiometric phases of composition AnO 2±x. For plutonium, the very formation of PuO 2+x has challenged a long-established dogma, and raised fundamental questions for long-term storage and environmental migration. This presentation covers two aspects of Los Alamos synchrotron radiation studies of plutonium oxides: (1) the structural chemistry of laboratory-prepared AnO 2+x systems (An = U, Pu; 0 ≤ x ≤ 0.25) determined through a combination of x-ray absorption fine structure spectroscopy (XAFS) and x-ray scattering of laboratory prepared samples; and (2)more » the application of synchrotron radiation towards the decontamination and decommissioning of the Rocky Flats Environmental Technology Site. Making the case for particle transport mechanisms as the basis of plutonium and americium mobility, rather than aqueous sorption-desorption processes, established a successful scientific basis for the dominance of physical transport processes by wind and water. The scientific basis was successful because it was in agreement with general theory on insolubility of PuO 2 in oxidation state IV, results of ultrafiltration analyses of field water/sediment samples, XAFS analyses of soil, sediment, and concrete samples, and was also in general agreement with on-site monitoring data. This understanding allowed Site contractors to rapidly move to application of soil erosion and sediment transport models as the means of predicting plutonium and americium transport, which led to design and application of site-wide soil erosion control technology to help control downstream concentrations of plutonium and americium in streamflow.« less

In search of plutonium: A nonproliferation journey

NASA Astrophysics Data System (ADS)

Hecker, Siegfried

2010-02-01

In February 1992, I landed in the formerly secret city of Sarov, the Russian Los Alamos, followed a few days later by a visit to Snezhinsk, their Livermore. The briefings we received of the Russian nuclear weapons program and tours of their plutonium, reactor, explosives, and laser facilities were mind boggling considering the Soviet Union was dissolved only two months earlier. This visit began a 17-year, 41 journey relationship with the Russian nuclear complex dedicated to working with them in partnership to protect and safeguard their weapons and fissile materials, while addressing the plight of their scientists and engineers. In the process, we solved a forty-year disagreement about the plutonium-gallium phase diagram and began a series of fundamental plutonium science workshops that are now in their tenth year. At the Yonbyon reprocessing facility in January 2004, my North Korean hosts had hoped to convince me that they have a nuclear deterrent. When I expressed skepticism, they asked if I wanted to see their ``product.'' I asked if they meant the plutonium; they replied, ``Well, yes.'' Thus, I wound up holding 200 grams of North Korean plutonium (in a sealed glass jar) to make sure it was heavy and warm. So began the first of my six journeys to North Korea to provide technical input to the continuing North Korean nuclear puzzle. In Trombay and Kalpakkam a few years later I visited the Indian nuclear research centers to try to understand how India's ambitious plans for nuclear power expansion can be accomplished safely and securely. I will describe these and other attempts to deal with the nonproliferation legacy of the cold war and the new challenges ahead. )

Variants of Regenerated Fissile Materials Usage in Thermal Reactors as the First Stage of Fuel Cycle Closing

NASA Astrophysics Data System (ADS)

Andrianova, E. A.; Tsibul'skiy, V. F.

2017-12-01

At present, 240 000 t of spent nuclear fuel (SF) has been accumulated in the world. Its long-term storage should meet safety conditions and requires noticeable finances, which grow every year. Obviously, this situation cannot exist for a long time; in the end, it will require a final decision. At present, several variants of solution of the problem of SF management are considered. Since most of the operating reactors and those under construction are thermal reactors, it is reasonable to assume that the structure of the nuclear power industry in the near and medium-term future will be unchanged, and it will be necessary to utilize plutonium in thermal reactors. In this study, different strategies of SF management are compared: open fuel cycle with long-term SF storage, closed fuel cycle with MOX fuel usage in thermal reactors and subsequent long-term storage of SF from MOX fuel, and closed fuel cycle in thermal reactors with heterogeneous fuel arrangement. The concept of heterogeneous fuel arrangement is considered in detail. While in the case of traditional fuel it is necessary to reprocess the whole amount of spent fuel, in the case of heterogeneous arrangement, it is possible to separate plutonium and 238U in different fuel rods. In this case, it is possible to achieve nearly complete burning of fissile isotopes of plutonium in fuel rods loaded with plutonium. These fuel rods with burned plutonium can be buried after cooling without reprocessing. They would contain just several percent of initially loaded plutonium, mainly even isotopes. Fuel rods with 238U alone should be reprocessed in the usual way.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bhattacharyya, M.H.; Larsen, R.P.; Oldham, R.D.

The fraction of plutonium absorbed after oral administration of Pu(VI) to 24-h-fasted mice was 19 X 10(-4), 13-fold higher than in fed mice, 1.4 X 10(-4). We have investigated the relevance of the high gastrointestinal (GI) absorption value for the 24-h-fasted animals in setting drinking water standards for humans. When fasting was initiated at the beginning of the active phase of the mouse's daily activity cycle (when they would normally eat), plutonium GI absorption rose from 2.8 X 10(-4) at zero-time to a level typical of the 24-h-fasted mouse after only 2 h of fasting. In contrast, in mice allowedmore » to eat for 4 h into their active phase prior to initiation of the fast (meal-fed mice), 8 h of fasting were required before GI absorption rose to a level similar to that of the 24-h-fasted mouse. The fraction of plutonium retained after gavage administration of Pu(VI) to 1-day-old rats was 74 X 10(-4), 70-fold higher than the value for fed adults. Retention after GI absorption in neonates remained 30- to 70-fold higher than in adults until weaning. One week after weaning, the fraction absorbed and retained by fed weanling rats was the same as that for fed adults, 1 X 10(-4). Drinking water standards for plutonium have been set based on GI absorption values for fed adult animals. The 10- to 100-fold increases in plutonium absorption in young and fasted animals reported by ourselves and others, and the rapid rise to fasted levels of absorption at the start of the animal's active phase, indicate that consideration should be given to elevated levels of plutonium absorption in young and fasted individuals.« less

Investigation of the system ThO 2-NpO 2-P 2O 5. Solid solutions of thorium-neptunium (IV) phosphate-diphosphate

NASA Astrophysics Data System (ADS)

Dacheux, N.; Thomas, A. C.; Brandel, V.; Genet, M.

1998-11-01

Considering that phosphate matrices could be potential candidates for the immobilization of actinides or for the final disposal of the excess plutonium from dismantled nuclear weapons, the chemistry of thorium phosphates has been re-examined. In the ThO 2-P 2O 5 system, the thorium phosphate-diphosphate Th 4(PO 4) 4P 2O 7 (TPD) can be synthesized by wet and dry chemical processes. The substitution of thorium by other tetravalent actinides like uranium or plutonium can be obtained for 0 < x < 3.0 and 0 < x < 1.63, respectively. In this work, we report the chemical conditions of synthesis of thorium-neptunium (IV) phosphate-diphosphate solid solutions Th 4- xNp x(PO 4) 4P 2O 7 (TNPD) with 0 < x < 1.6 from a mixture of thorium and neptunium (IV) nitrates and concentrated phosphoric acid. From the variation of the cell parameters and volume, the maximum substitution of Th 4+ by Np 4+ in the TPD structure is evaluated to 2.08 (which corresponds to about 52 mol% of thorium replaced by neptunium (IV)). The field of existence of solid solutions Th 4- xU- xNp- xPuU xUNp xNpPu xPu(PO 4)4P 2O 7 has been calculated. These solid solutions should be synthesized for 5 xU+7 xNp+9 xPu⩽15. In the NpO 2-P 2O 5 system, the unit cell parameters of Np 2O(PO 4) 2 were refined by analogy with U 2O(PO 4) 2 which crystallographic data have been published recently. For Np 2O(PO 4) 2 the unit cell is orthorhombic with the following cell parameters: a=7.033(2) Å, b=9.024(3) Å, c=12.587(6) Å and V=799(1) Å 3. The unit cell parameter obtained for α-NpP 2O 7 ( a=8.586(1) Å) is in good agreement with those already reported in literature.

15. VIEW OF LABORATORY EQUIPMENT IN THE BUILDING 771 ANALYTICAL ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

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

PLUTONIUM METALLIC FUELS FOR FAST REACTORS

DOE Office of Scientific and Technical Information (OSTI.GOV)

STAN, MARIUS; HECKER, SIEGFRIED S.

2007-02-07

Early interest in metallic plutonium fuels for fast reactors led to much research on plutonium alloy systems including binary solid solutions with the addition of aluminum, gallium, or zirconium and low-melting eutectic alloys with iron and nickel or cobalt. There was also interest in ternaries of these elements with plutonium and cerium. The solid solution and eutectic alloys have most unusual properties, including negative thermal expansion in some solid-solution alloys and the highest viscosity known for liquid metals in the Pu-Fe system. Although metallic fuels have many potential advantages over ceramic fuels, the early attempts were unsuccessful because these fuelsmore » suffered from high swelling rates during burn up and high smearing densities. The liquid metal fuels experienced excessive corrosion. Subsequent work on higher-melting U-PuZr metallic fuels was much more promising. In light of the recent rebirth of interest in fast reactors, we review some of the key properties of the early fuels and discuss the challenges presented by the ternary alloys.« less

TA-55 change control manual

DOE Office of Scientific and Technical Information (OSTI.GOV)

Blum, T.W.; Selvage, R.D.; Courtney, K.H.

This manual is the guide for initiating change at the Plutonium Facility, which handles the processing of plutonium as well as research on plutonium metallurgy. It describes the change and work control processes employed at TA-55 to ensure that all proposed changes are properly identified, reviewed, approved, implemented, tested, and documented so that operations are maintained within the approved safety envelope. All Laboratory groups, their contractors, and subcontractors doing work at TA-55 follow requirements set forth herein. This manual applies to all new and modified processes and experiments inside the TA-55 Plutonium Facility; general plant project (GPP) and line itemmore » funded construction projects at TA-55; temporary and permanent changes that directly or indirectly affect structures, systems, or components (SSCs) as described in the safety analysis, including Facility Control System (FCS) software; and major modifications to procedures. This manual does not apply to maintenance performed on process equipment or facility SSCs or the replacement of SSCs or equipment with documented approved equivalents.« less

A Plutonium-Contaminated Wound, 1985, USA

DOE Office of Scientific and Technical Information (OSTI.GOV)

Doran M. Christensen, DO, REAC /TS Associate Director and Staff Physician Eugene H. Carbaugh, CHP, Staff Scientist, Internal Dosimetry Manager, Pacific Northwest National Laboratory, Richland, Washington

2012-02-02

A hand injury occurred at a U.S. facility in 1985 involving a pointed shaft (similar to a meat thermometer) that a worker was using to remove scrap solid plutonium from a plastic bottle. The worker punctured his right index finger on the palm side at the metacarpal-phalangeal joint. The wound was not through-and- through, although it was deep. The puncture wound resulted in deposition of ~48 kBq of alpha activity from the weapons-grade plutonium mixture with a nominal 12 to 1 Pu-alpha to {sup 241}Am-alpha ratio. This case clearly showed that DTPA was very effective for decorporation of plutonium andmore » americium. The case is a model for management of wounds contaminated with transuranics: (1) a team approach for dealing with all of the issues surrounding the incident, including the psychological, (2) early surgical intervention for foreign-body removal, (3) wound irrigation with DTPA solution, and (4) early and prolonged DTPA administration based upon bioassay and in vivo dosimetry.« less

Determination of origin and intended use of plutonium metal using nuclear forensic techniques.

PubMed

Rim, Jung H; Kuhn, Kevin J; Tandon, Lav; Xu, Ning; Porterfield, Donivan R; Worley, Christopher G; Thomas, Mariam R; Spencer, Khalil J; Stanley, Floyd E; Lujan, Elmer J; Garduno, Katherine; Trellue, Holly R

2017-04-01

Nuclear forensics techniques, including micro-XRF, gamma spectrometry, trace elemental analysis and isotopic/chronometric characterization were used to interrogate two, potentially related plutonium metal foils. These samples were submitted for analysis with only limited production information, and a comprehensive suite of forensic analyses were performed. Resulting analytical data was paired with available reactor model and historical information to provide insight into the materials' properties, origins, and likely intended uses. Both were super-grade plutonium, containing less than 3% 240 Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modeling feedback and trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. Based on this investigation, the most likely intended use for these plutonium foils was 239 Pu fission foil targets for physics experiments, such as cross-section measurements, etc. Copyright © 2017 Elsevier B.V. All rights reserved.

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.

PubMed

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.

Environmental consequences of postulated plutonium releases from Westinghouse PFDL, Cheswick, Pennsylvania, as a result of severe natural phenomena

DOE Office of Scientific and Technical Information (OSTI.GOV)

McPherson, R.B.; Watson, E.C.

1979-06-01

Potential environmental consequences in terms of radiation dose to people are presented for postulated accidents due to earthquakes, tornadoes, high straight-line winds, and floods. Maximum plutonium deposition values are given for significant locations around the site. All important potential exposure pathways are examined. The most likely calculated 50-year collective committed dose equivalents are all much lower than the collective dose equivalent expected from 50 years of exposure to natural background radiation and medical x-rays except Earthquake No. 4 and the 260-mph tornado. The most likely maximum residual plutonium contamination estimated to be deposited offsite following Earthquake No. 4, and themore » 200-mph and 260-mph tornadoes are above the Environmental Protection Agency's (EPA) proposed guideline for plutonium in the general environment of 0.2 ..mu..Ci/m/sup 2/. The deposition values following the other severe natural phenomena are below the EPA proposed guideline.« less

Isotopic fractionation studies of uranium and plutonium using porous ion emitters as thermal ionization mass spectrometry sources

DOE PAGES

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

DOEpatents

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.

Determination of origin and intended use of plutonium metal using nuclear forensic techniques

DOE PAGES

Rim, Jung H.; Kuhn, Kevin J.; Tandon, Lav; ...

2017-04-01

Nuclear forensics techniques, including micro-XRF, gamma spectrometry, trace elemental analysis and isotopic/chronometric characterization were used to interrogate two, potentially related plutonium metal foils. These samples were submitted for analysis with only limited production information, and a comprehensive suite of forensic analyses were performed. Resulting analytical data was paired with available reactor model and historical information to provide insight into the materials’ properties, origins, and likely intended uses. Both were super-grade plutonium, containing less than 3% 240Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modelling feedback andmore » trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. In conclusion, based on this investigation, the most likely intended use for these plutonium foils was 239Pu fission foil targets for physics experiments, such as cross-section measurements, etc.« less

In-vitro analysis of the dissolution kinetics and systemic availability of plutonium ingested in the form of 'hot' particles from the Semipalatinsk NTS.

PubMed

Conway, M; León Vintró, L; Mitchell, P I; García-Tenorio, R; Jimenez-Ramos, M C; Burkitbayev, M; Priest, N D

2009-05-01

In-vitro leaching of radioactive 'hot' particles isolated from soils sampled at the Semipalatinsk Nuclear Test Site has been carried out in order to evaluate the fraction of plutonium activity released into simulated human stomach and small intestine fluids during digestion. Characterisation of the particles (10-100 Bq(239,240)Pu) and investigation of their dissolution kinetics in simulated fluids has been accomplished using a combination of high-resolution alpha-spectrometry, gamma-spectrometry and liquid scintillation counting. The results of these analyses indicate that plutonium transfer across the human gut following the ingestion of 'hot' particles can be up to two orders of magnitude lower than that expected for plutonium in a more soluble form, and show that for areas affected by local fallout, use of published ingestion dose coefficients, together with bulk radionuclide concentrations in soil, may lead to a considerable overestimation of systemic uptake via the ingestion pathway.

Isotopic fractionation studies of uranium and plutonium using porous ion emitters as thermal ionization mass spectrometry sources

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

Excess plutonium disposition: The deep borehole option

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ferguson, K.L.

1994-08-09

This report reviews the current status of technologies required for the disposition of plutonium in Very Deep Holes (VDH). It is in response to a recent National Academy of Sciences (NAS) report which addressed the management of excess weapons plutonium and recommended three approaches to the ultimate disposition of excess plutonium: (1) fabrication and use as a fuel in existing or modified reactors in a once-through cycle, (2) vitrification with high-level radioactive waste for repository disposition, (3) burial in deep boreholes. As indicated in the NAS report, substantial effort would be required to address the broad range of issues relatedmore » to deep bore-hole emplacement. Subjects reviewed in this report include geology and hydrology, design and engineering, safety and licensing, policy decisions that can impact the viability of the concept, and applicable international programs. Key technical areas that would require attention should decisions be made to further develop the borehole emplacement option are identified.« less

Comparison of premortem and postmortem estimates of plutonium deposited in the skeleton and liver of six individuals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sula, M.J.; Bihl, D.E.; Carbaugh, E.H.

1988-04-01

Assessment of organ burdens after internal exposures to radionuclides is often necessary to evaluate the health and regulatory implications of the exposure. The assessment of plutonium activity in skeleton and liver is usually estimated from measurements of plutonium excreted via urine. As part of the overall evaluation of internal dose assessment techniques, it is useful to compare the results of organ burden estimates made from evaluation of urinary excretion data with those made at death from tissue samples collected posthumously from the individual. Estimates of plutonium in the skeleton and liver, based on postmortem analysis of tissue samples for sixmore » individuals, were obtained from the US Transuranium Registry (USTR). Bioassay data and other radiation exposure information obtained from the individuals' files were used to estimate their skeleton and liver burdens at the times of their deaths, and these estimates were compared to those obtained through tissue analysis. 6 refs., 2 tabs.« less

Safeguardability of the vitrification option for disposal of plutonium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pillay, K.K.S.

1996-05-01

Safeguardability of the vitrification option for plutonium disposition is rather complex and there is no experience base in either domestic or international safeguards for this approach. In the present treaty regime between the US and the states of the former Soviet Union, bilaterial verifications are considered more likely with potential for a third-party verification of safeguards. There are serious technological limitations to applying conventional bulk handling facility safeguards techniques to achieve independent verification of plutonium in borosilicate glass. If vitrification is the final disposition option chosen, maintaining continuity of knowledge of plutonium in glass matrices, especially those containing boron andmore » those spike with high-level wastes or {sup 137}Cs, is beyond the capability of present-day safeguards technologies and nondestructive assay techniques. The alternative to quantitative measurement of fissile content is to maintain continuity of knowledge through a combination of containment and surveillance, which is not the international norm for bulk handling facilities.« less