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.
PLUTONIUM-CUPFERRON COMPLEX AND METHOD OF REMOVING PLUTONIUM FROM SOLUTION
Potratz, H.A.
1959-01-13
A method is presented for separating plutonium from fission products present in solutions of neutronirradiated uranium. The process consists in treating such acidic solutions with cupferron so that the cupferron reacts with the plutonium present to form an insoluble complex. This plutonium cupferride precipitates and may then be separated from the solution.
PROCESS FOR THE RECOVERY OF PLUTONIUM
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.
Neptunium and plutonium complexes with a sterically encumbered triamidoamine (TREN) scaffold
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.
PROCESS FOR THE SEPARATION OF HEAVY METALS
Gofman, J.W.; Connick, R.E.; Wahl, A.C.
1959-01-27
A method is presented for thc separation of plutonium from uranium and the fission products with which it is associated. The method is based on the fact that hexavalent plutonium forms an insoluble complex precipitate with sodium acetate, as does the uranyl ion, while reduced plutonium is not precipitated by sodium acetate. Several embodiments are shown, e.g., a solution containing plutonium and uranium in the hexavalent state may be contacted with sodium acetate causing the formation of a sodium uranyl acetate precipitate which carries the plutonium values while the fission products remain in solution. If the original solution is treated with a reducing agent, so that the plutonium is reduced while the uranium remains in the hexavalent state, and sodium and acetate ions are added, the uranium will precipitutc while the plutonium remains in solution effecting separation of the Pu from urarium.
Beaufait, L.J. Jr.; Stevenson, F.R.; Rollefson, G.K.
1958-11-18
The recovery of plutonium ions from neutron irradiated uranium can be accomplished by bufferlng an aqueous solutlon of the irradiated materials containing tetravalent plutonium to a pH of 4 to 7, adding sufficient acetate to the solution to complex the uranyl present, adding ferric nitrate to form a colloid of ferric hydroxide, plutonlum, and associated fission products, removing and dissolving the colloid in aqueous nitric acid, oxldizlng the plutonium to the hexavalent state by adding permanganate or dichromate, treating the resultant solution with ferric nitrate to form a colloid of ferric hydroxide and associated fission products, and separating the colloid from the plutonlum left in solution.
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
CARBONATE METHOD OF SEPARATION OF TETRAVALENT PLUTONIUM FROM FISSION PRODUCT VALUES
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.
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.
Ferric ion as a scavenging agent in a solvent extraction process
Bruns, Lester E.; Martin, Earl C.
1976-01-01
Ferric ions are added into the aqueous feed of a plutonium scrap recovery process that employs a tributyl phosphate extractant. Radiolytic degradation products of tributyl phosphate such as dibutyl phosphate form a solid precipitate with iron and are removed from the extraction stages via the waste stream. Consequently, the solvent extraction characteristics are improved, particularly in respect to minimizing the formation of nonstrippable plutonium complexes in the stripping stages. The method is expected to be also applicable to the partitioning of plutonium and uranium in a scrap recovery process.
Dissolution of aerosol particles collected from nuclear facility plutonium production process
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.
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.
SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS
Boyd, G.E.; Adamson, A.W.; Schubert, J.; Russell, E.R.
1958-10-01
A chromatographic adsorption process is presented for the separation of plutonium from other fission products formed by the irradiation of uranium. The plutonium and the lighter element fission products are adsorbed on a sulfonated phenol-formaldehyde resin bed from a nitric acid solution containing the dissolved uranium. Successive washes of sulfuric, phosphoric, and nitric acids remove the bulk of the fission products, then an eluate of dilute phosphoric and nitric acids removes the remaining plutonium and fission products. The plutonium is selectively removed by passing this solution through zirconium phosphate, from which the plutonium is dissolved with nitric acid. This process provides a convenient and efficient means for isolating plutonium.
PRODUCTION OF PLUTONIUM FLUORIDE FROM BISMUTH PHOSPHATE PRECIPITATE CONTAINING PLUTONIUM VALUES
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.
SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Boyd, G.E.; Adamson, A.W.; Schubert, J.
A chromatographic adsorption process is presented for the separation of plutonium from other fission products formed by the irradiation of uranium. The plutonium and the lighter element fission products are adsorbed on a sulfonated phenol-formaldehyde resin bed from a nitric acid solution containing the dissolved uranium. Successive washes of sulfuric, phosphoric, and nitric acids remove the bulk of the fission products, then an eluate of dilute phosphoric and nitric acids removes the remaining plutonium and fission products. The plutonium is selectively removed by passing this solution through zirconium phosphate, from which the plutonium is dissolved with nitric acid. This processmore » provides a convenient and efficient means for isolating plutonium.« less
Method of separating thorium from plutonium
Clifton, David G.; Blum, Thomas W.
1984-01-01
A method of chemically separating plutonium from thorium. Plutonium and thorium to be separated are dissolved in an aqueous feed solution, preferably as the nitrate salts. The feed solution is acidified and sodium nitrite is added to the solution to adjust the valence of the plutonium to the +4 state. A chloride salt, preferably sodium chloride, is then added to the solution to induce formation of an anionic plutonium chloride complex. The anionic plutonium chloride complex and the thorium in solution are then separated by ion exchange on a strong base anion exchange column.
Method of separating thorium from plutonium
Clifton, D.G.; Blum, T.W.
A method of chemically separating plutonium from thorium is claimed. Plutonium and thorium to be separated are dissolved in an aqueous feed solution, preferably as the nitrate salts. The feed solution is acidified and sodium nitrite is added to the solution to adjust the valence of the plutonium to the +4 state. A chloride salt, preferably sodium chloride, is then added to the solution to induce formation of an anionic plutonium chloride complex. The anionic plutonium chloride complex and the thorium in solution are then separated by ion exchange on a strong base anion exchange column.
Method of separating thorium from plutonium
Clifton, D.G.; Blum, T.W.
1984-07-10
A method is described for chemically separating plutonium from thorium. Plutonium and thorium to be separated are dissolved in an aqueous feed solution, preferably as the nitrate salts. The feed solution is acidified and sodium nitrite is added to the solution to adjust the valence of the plutonium to the +4 state. A chloride salt, preferably sodium chloride, is then added to the solution to induce formation of an anionic plutonium chloride complex. The anionic plutonium chloride complex and the thorium in solution are then separated by ion exchange on a strong base anion exchange column.
Maddock, A.G.; Smith, F.
1959-08-25
A method is described for separating plutonium from uranium and fission products by treating a nitrate solution of fission products, uranium, and hexavalent plutonium with a relatively water-insoluble fluoride to adsorb fission products on the fluoride, treating the residual solution with a reducing agent for plutonium to reduce its valence to four and less, treating the reduced plutonium solution with a relatively insoluble fluoride to adsorb the plutonium on the fluoride, removing the solution, and subsequently treating the fluoride with its adsorbed plutonium with a concentrated aqueous solution of at least one of a group consisting of aluminum nitrate, ferric nitrate, and manganous nitrate to remove the plutonium from the fluoride.
PROCESSES FOR SEPARATING AND RECOVERING CONSTITUENTS OF NEUTRON IRRADIATED URANIUM
Connick, R.E.; Gofman, J.W.; Pimentel, G.C.
1959-11-10
Processes are described for preparing plutonium, particularly processes of separating plutonium from uranium and fission products in neutron-irradiated uraniumcontaining matter. Specifically, plutonium solutions containing uranium, fission products and other impurities are contacted with reducing agents such as sulfur dioxide, uranous ion, hydroxyl ammonium chloride, hydrogen peroxide, and ferrous ion whereby the plutoninm is reduced to its fluoride-insoluble state. The reduced plutonium is then carried out of solution by precipitating niobic oxide therein. Uranium and certain fission products remain behind in the solution. Certain other fission products precipitate along with the plutonium. Subsequently, the plutonium and fission product precipitates are redissolved, and the solution is oxidized with oxidizing agents such as chlorine, peroxydisulfate ion in the presence of silver ion, permanganate ion, dichromate ion, ceric ion, and a bromate ion, whereby plutonium is oxidized to the fluoride-soluble state. The oxidized solution is once again treated with niobic oxide, thus precipitating the contamirant fission products along with the niobic oxide while the oxidized plutonium remains in solution. Plutonium is then recovered from the decontaminated solution.
PLUTONIUM-HYDROGEN REACTION PRODUCT, METHOD OF PREPARING SAME AND PLUTONIUM POWDER THEREFROM
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.
Method for dissolving plutonium dioxide
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.
Removal of plutonium from hepatic tissue
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.
SEPARATION OF PLUTONIUM FROM FISSION PRODUCTS BY A COLLOID REMOVAL PROCESS
Schubert, J.
1960-05-24
A method is given for separating plutonium from uranium fission products. An acidic aqueous solution containing plutonium and uranium fission products is subjected to a process for separating ionic values from colloidal matter suspended therein while the pH of the solution is maintained between 0 and 4. Certain of the fission products, and in particular, zirconium, niobium, lanthanum, and barium are in a colloidal state within this pH range, while plutonium remains in an ionic form, Dialysis, ultracontrifugation, and ultrafiltration are suitable methods of separating plutonium ions from the colloids.
PROCESS FOR SEPARATION OF HEAVY METALS
Duffield, R.B.
1958-04-29
A method is described for separating plutonium from aqueous acidic solutions of neutron-irradiated uranium and the impurities associated therewith. The separation is effected by adding, to the solution containing hexavalent uranium and plutonium, acetate ions and the ions of an alkali metal and those of a divalent metal and thus forming a complex plutonium acetate salt which is carried by the corresponding complex of uranium, such as sodium magnesium uranyl acetate. The plutonium may be separated from the precipitated salt by taking the same back into solution, reducing the plutonium to a lower valent state on reprecipitating the sodium magnesium uranyl salt, removing the latter, and then carrying the plutonium from ihe solution by means of lanthanum fluoride.
PROCESS USING BISMUTH PHOSPHATE AS A CARRIER PRECIPITATE FOR FISSION PRODUCTS AND PLUTONIUM VALUES
Finzel, T.G.
1959-03-10
A process is described for separating plutonium from fission products carried therewith when plutonium in the reduced oxidation state is removed from a nitric acid solution of irradiated uranium by means of bismuth phosphate as a carrier precipitate. The bismuth phosphate carrier precipitate is dissolved by treatment with nitric acid and the plutonium therein is oxidized to the hexavalent oxidation state by means of potassium dichromate. Separation of the plutonium from the fission products is accomplished by again precipitating bismuth phosphate and removing the precipitate which now carries the fission products and a small percentage of the plutonium present. The amount of plutonium carried in this last step may be minimized by addition of sodium fluoride, so as to make the solution 0.03N in NaF, prior to the oxidation and prccipitation step.
ION EXCHANGE ADSORPTION PROCESS FOR PLUTONIUM SEPARATION
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.
SEPARATION OF RUTHENIUM FROM AQUEOUS SOLUTIONS
Callis, C.F.; Moore, R.L.
1959-09-01
>The separation of ruthenium from aqueous solutions containing uranium plutonium, ruthenium, and fission products is described. The separation is accomplished by providing a nitric acid solution of plutonium, uranium, ruthenium, and fission products, oxidizing plutonium to the hexavalent state with sodium dichromate, contacting the solution with a water-immiscible organic solvent, such as hexone, to extract plutonyl, uranyl, ruthenium, and fission products, reducing with sodium ferrite the plutonyl in the solvent phase to trivalent plutonium, reextracting from the solvent phase the trivalent plutonium, ruthenium, and some fission products with an aqueous solution containing a salting out agent, introducing ozone into the aqueous acid solution to oxidize plutonium to the hexavalent state and ruthenium to ruthenium tetraoxide, and volatizing off the ruthenium tetraoxide.
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
12. Architectural Floor Plans, 233S, U.S. Atomic Energy Commission, Hanford ...
12. Architectural Floor Plans, 233-S, U.S. Atomic Energy Commission, Hanford Atomic Products Operations, General Electric Company, Dwg. H-2-30464, 1956. - Reduction-Oxidation Complex, Plutonium Concentration Facility, 200 West Area, Richland, Benton County, WA
11. Architectural ELevations & Sections, 233S, U.S. Atomic Energy Commission, ...
11. Architectural ELevations & Sections, 233-S, U.S. Atomic Energy Commission, Hanford Atomic Products Operations, General Electric Company, Dwg. No. H-2-30465, 1956. - Reduction-Oxidation Complex, Plutonium Concentration Facility, 200 West Area, Richland, Benton County, WA
Volatile fluoride process for separating plutonium from other materials
Spedding, F. H.; Newton, A. S.
1959-04-14
The separation of plutonium from uranium and/or fission products by formation of the higher fluorides off uranium and/or plutonium is described. Neutronirradiated uranium metal is first converted to the hydride. This hydrided product is then treated with fluorine at about 315 deg C to form and volatilize UF/sub 6/ leaving plutonium behind. Thc plutonium may then be separated by reacting the residue with fluorine at about 5004DEC and collecting the volatile plutonium fluoride thus formed.
VOLATILE FLUORIDE PROCESS FOR SEPARATING PLUTONIUM FROM OTHER MATERIALS
Spedding, F.H.; Newton, A.S.
1959-04-14
The separation of plutonium from uranium and/or tission products by formation of the higher fluorides of uranium and/or plutonium is discussed. Neutronirradiated uranium metal is first convcrted to the hydride. This hydrided product is then treatced with fluorine at about 315 deg C to form and volatilize UF/sup 6/ leaving plutonium behind. The plutonium may then be separated by reacting the residue with fluorine at about 500 deg C and collecting the volatile plutonium fluoride thus formed.
PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINATING ELEMENTS
Sutton, J.B.
1958-02-18
This patent relates to an improved method for the decontamination of plutonium. The process consists broadly in an improvement in a method for recovering plutonium from radioactive uranium fission products in aqueous solutions by decontamination steps including byproduct carrier precipitation comprising the step of introducing a preformed aqueous slurry of a hydroxide of a metal of group IV B into any aqueous acidic solution which contains the plutonium in the hexavalent state, radioactive uranium fission products contaminant and a by-product carrier precipitate and separating the metal hydroxide and by-product precipitate from the solution. The process of this invention is especially useful in the separation of plutonium from radioactive zirconium and columbium fission products.
SEPARATION PROCESS USING COMPLEXING AND ADSORPTION
Spedding, J.H.; Ayers, J.A.
1958-06-01
An adsorption process is described for separating plutonium from a solution of neutron-irradiated uranium containing ions of a compound of plutonium and other cations. The method consists of forming a chelate complex compound with plutoniunn ions in the solution by adding a derivative of 8- hydroxyquinoline, which derivative contains a sulfonic acid group, and adsorbing the remaining cations from the solution on a cation exchange resin, while the complexed plutonium remains in the solution.
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.
10. Architectural Door Details & Plot Plan, 233S, U.S. Atomic ...
10. Architectural Door Details & Plot Plan, 233-S, U.S. Atomic Energy Commission, Hanford Atomic Products Operations, General Electric Company, Dwg. No. H-2-30469, 1956. - Reduction-Oxidation Complex, Plutonium Concentration Facility, 200 West Area, Richland, Benton County, WA
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.
Lithium metal reduction of plutonium oxide to produce plutonium metal
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.
Method for the recovery of actinide elements from nuclear reactor waste
Horwitz, E. Philip; Delphin, Walter H.; Mason, George W.
1979-01-01
A process for partitioning and recovering actinide values from acidic waste solutions resulting from reprocessing of irradiated nuclear fuels by adding hydroxylammonium nitrate and hydrazine to the waste solution to adjust the valence of the neptunium and plutonium values in the solution to the +4 oxidation state, thus forming a feed solution and contacting the feed solution with an extractant of dihexoxyethyl phosphoric acid in an organic diluent whereby the actinide values, most of the rare earth values and some fission product values are taken up by the extractant. Separation is achieved by contacting the loaded extractant with two aqueous strip solutions, a nitric acid solution to selectively strip the americium, curium and rare earth values and an oxalate solution of tetramethylammonium hydrogen oxalate and oxalic acid or trimethylammonium hydrogen oxalate to selectively strip the neptunium, plutonium and fission product values. Uranium values remain in the extractant and may be recovered with a phosphoric acid strip. The neptunium and plutonium values are recovered from the oxalate by adding sufficient nitric acid to destroy the complexing ability of the oxalate, forming a second feed, and contacting the second feed with a second extractant of tricaprylmethylammonium nitrate in an inert diluent whereby the neptunium and plutonium values are selectively extracted. The values are recovered from the extractant with formic acid.
PLUTONIUM PURIFICATION PROCESS EMPLOYING THORIUM PYROPHOSPHATE CARRIER
King, E.L.
1959-04-28
The separation and purification of plutonium from the radioactive elements of lower atomic weight is described. The process of this invention comprises forming a 0.5 to 2 M aqueous acidffc solution containing plutonium fons in the tetravalent state and elements with which it is normally contaminated in neutron irradiated uranium, treating the solution with a double thorium compound and a soluble pyrophosphate compound (Na/sub 4/P/sub 2/O/sub 7/) whereby a carrier precipitate of thorium A method is presented of reducing neptunium and - trite is advantageous since it destroys any hydrazine f so that they can be removed from solutions in which they are contained is described. In the carrier precipitation process for the separation of plutonium from uranium and fission products including zirconium and columbium, the precipitated blsmuth phosphate carries some zirconium, columbium, and uranium impurities. According to the invention such impurities can be complexed and removed by dissolving the contaminated carrier precipitate in 10M nitric acid, followed by addition of fluosilicic acid to about 1M, diluting the solution to about 1M in nitric acid, and then adding phosphoric acid to re-precipitate bismuth phosphate carrying plutonium.
Density functional theory study of defects in unalloyed δ-Pu
Hernandez, S. C.; Freibert, F. J.; Wills, J. M.
2017-03-19
Using density functional theory, we explore in this paper various classical point and complex defects within the face-centered cubic unalloyed δ-plutonium matrix that are potentially induced from self-irradiation. For plutonium only defects, the most energetically stable defect is a distorted split-interstitial. Gallium, the δ-phase stabilizer, is thermodynamically stable as a substitutional defect, but becomes unstable when participating in a complex defect configuration. Finally, complex uranium defects may thermodynamically exist as uranium substitutional with neighboring plutonium interstitial and stabilization of uranium within the lattice is shown via partial density of states and charge density difference plots to be 5f hybridization betweenmore » uranium and plutonium.« less
Density functional theory study of defects in unalloyed δ-Pu
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hernandez, S. C.; Freibert, F. J.; Wills, J. M.
Using density functional theory, we explore in this paper various classical point and complex defects within the face-centered cubic unalloyed δ-plutonium matrix that are potentially induced from self-irradiation. For plutonium only defects, the most energetically stable defect is a distorted split-interstitial. Gallium, the δ-phase stabilizer, is thermodynamically stable as a substitutional defect, but becomes unstable when participating in a complex defect configuration. Finally, complex uranium defects may thermodynamically exist as uranium substitutional with neighboring plutonium interstitial and stabilization of uranium within the lattice is shown via partial density of states and charge density difference plots to be 5f hybridization betweenmore » uranium and plutonium.« less
Method for cleaning solution used in nuclear fuel reprocessing
Tallent, O.K.; Crouse, D.J.; Mailen, J.C.
1980-12-17
Nuclear fuel processing solution consisting of tri-n-butyl phosphate and dodecane, with a complex of uranium, plutonium, or zirconium and with a solvent degradation product such as di-n-butyl phosphate therein, is contacted with an aqueous solution of a salt formed from hydrazine and either a dicarboxylic acid or a hydroxycarboxylic acid, thereby removing the aforesaid complex from the processing solution.
Method for cleaning solution used in nuclear fuel reprocessing
Tallent, Othar K.; Crouse, David J.; Mailen, James C.
1982-01-01
Nuclear fuel processing solution consisting of tri-n-butyl phosphate and dodecane, with a complex of uranium, plutonium, or zirconium and with a solvent degradation product such as di-n-butyl phosphate therein, is contacted with an aqueous solution of a salt formed from hydrazine and either a dicarboxylic acid or a hydroxycarboxylic acid, thereby removing the aforesaid complex from the processing solution.
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.
31. VIEW OF A WORKER HOLDING A PLUTONIUM 'BUTTON.' PLUTONIUM, ...
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
IMPROVED PROCESS OF PLUTONIUM CARRIER PRECIPITATION
Faris, B.F.
1959-06-30
This patent relates to an improvement in the bismuth phosphate process for separating and recovering plutonium from neutron irradiated uranium, resulting in improved decontamination even without the use of scavenging precipitates in the by-product precipitation step and subsequently more complete recovery of the plutonium in the product precipitation step. This improvement is achieved by addition of fluomolybdic acid, or a water soluble fluomolybdate, such as the ammonium, sodium, or potassium salt thereof, to the aqueous nitric acid solution containing tetravalent plutonium ions and contaminating fission products, so as to establish a fluomolybdate ion concentration of about 0.05 M. The solution is then treated to form the bismuth phosphate plutonium carrying precipitate.
ADSORPTION-BISMUTH PHOSPHATE METHOD FOR SEPARATING PLUTONIUM
Russell, E.R.; Adamson, A.W.; Boyd, G.E.
1960-06-28
A process is given for separating plutonium from uranium and fission products. Plutonium and uranium are adsorbed by a cation exchange resin, plutonium is eluted from the adsorbent, and then, after oxidation to the hexavalent state, the plutonium is contacted with a bismuth phosphate carrier precipitate.
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.
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.
1. West facade of Plutonium Concentration Facility (Building 233S), ReductionOxidation ...
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
23. AERIAL VIEW LOOKING SOUTHEAST AT THE PLUTONIUM OPERATION BUILDINGS ...
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
PURIFICATION OF PLUTONIUM USING A CERIUM PRECIPITATE AS A CARRIER FOR FISSION PRODUCTS
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.
METHOD OF SEPARATION OF PLUTONIUM FROM CARRIER PRECIPITATES
Dawson, I.R.
1959-09-22
The recovery of plutonium from fluoride carrier precipitates is described. The precipitate is dissolved in zirconyl nitrate, ferric nitrate, aluminum nitrate, or a mixture of these complexing agents, and the plutonium is then extracted from the aqueous solution formed with a water-immiscible organic solvent.
SEPARATION OF FISSION PRODUCT VALUES FROM THE HEXAVALENT PLUTONIUM BY CARRIER PRECIPITATION
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.
COMPLEX FLUORIDES OF PLUTONIUM AND AN ALKALI METAL
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.
RECOVERY OF Pu VALUES BY FLUORINATION AND FRACTIONATION
Brown, H.S.; Webster, D.S.
1959-01-20
A method is presented for the concentration and recovery of plutonium by fluorination and fractionation. A metallic mass containing uranium and plutonium is heated to 250 C and contacted with a stream of elemental fluorine. After fluorination of the metallic mass, the rcaction products are withdrawn and subjected to a distillation treatment to separate the fluorination products of uranium and to obtain a residue containing the fluorination products of plutonium.
Method of immobilizing weapons plutonium to provide a durable, disposable waste product
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.
PLATINUM HEXAFLUORIDE AND METHOD OF FLUORINATING PLUTONIUM CONTAINING MIXTURES THERE-WITH
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.
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
METHOD FOR OBTAINING PLUTONIUM METAL AND ALLOYS OF PLUTONIUM FROM PLUTONIUM TRICHLORIDE
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)
BASIC PEROXIDE PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINANTS
Seaborg, G.T.; Perlman, I.
1959-02-10
A process is described for the separation from each other of uranyl values, tetravalent plutonium values and fission products contained in an aqueous acidic solution. First the pH of the solution is adjusted to between 2.5 and 8 and hydrogen peroxide is then added to the solution causing precipitation of uranium peroxide which carries any plutonium values present, while the fission products remain in solution. Separation of the uranium and plutonium values is then effected by dissolving the peroxide precipitate in an acidic solution and incorporating a second carrier precipitate, selective for plutonium. The plutonium values are thus carried from the solution while the uranium remains flissolved. The second carrier precipitate may be selected from among the group consisting of rare earth fluorides, and oxalates, zirconium phosphate, and bismuth lihosphate.
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
PREPARATION OF PLUTONIUM TRIFLUORIDE
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.
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.
SEPARATION OF URANIUM, PLUTONIUM AND FISSION PRODUCTS
Nicholls, C.M.; Wells, I.; Spence, R.
1959-10-13
The separation of uranium and plutonium from neutronirradiated uranium is described. The neutron-irradiated uranium is dissolved in nitric acid to provide an aqueous solution 3N in nitric acid. The fission products of the solution are extruded by treating the solution with dibutyl carbitol substantially 1.8N in nitric acid. The organic solvent phase is separated and neutralized with ammonium hydroxide and the plutonium reduced with hydroxylamine base to the trivalent state. Treatment of the mixture with saturated ammonium nitrate extracts the reduced plutonium and leaves the uranium in the organic solvent.
SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS BY ADSORPTION
Seaborg, G.T.; Willard, J.E.
1958-01-01
A method is presented for the separation of plutonium from solutions containing that element in a valence state not higher than 41 together with uranium ions and fission products. This separation is accomplished by contacting the solutions with diatomaceous earth which preferentially adsorbs the plutonium present. Also mentioned as effective for this adsorbtive separation are silica gel, filler's earth and alumina.
PROCESS OF FORMING PLUOTONIUM SALTS FROM PLUTONIUM EXALATES
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.
PROCESS USING POTASSIUM LANTHANUM SULFATE FOR FORMING A CARRIER PRECIPITATE FOR PLUTONIUM VALUES
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 recovery from spent reactor fuel by uranium displacement
Ackerman, John P.
1992-01-01
A process for separating uranium values and transuranic values from fission products containing rare earth values when the values are contained together in a molten chloride salt electrolyte. A molten chloride salt electrolyte with a first ratio of plutonium chloride to uranium chloride is contacted with both a solid cathode and an anode having values of uranium and fission products including plutonium. A voltage is applied across the anode and cathode electrolytically to transfer uranium and plutonium from the anode to the electrolyte while uranium values in the electrolyte electrolytically deposit as uranium metal on the solid cathode in an amount equal to the uranium and plutonium transferred from the anode causing the electrolyte to have a second ratio of plutonium chloride to uranium chloride. Then the solid cathode with the uranium metal deposited thereon is removed and molten cadmium having uranium dissolved therein is brought into contact with the electrolyte resulting in chemical transfer of plutonium values from the electrolyte to the molten cadmium and transfer of uranium values from the molten cadmium to the electrolyte until the first ratio of plutonium chloride to uranium chloride is reestablished.
METHOD FOR REMOVING CONTAMINATION FROM PRECIPITATES
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.
SEPARATION OF FISSION PRODUCTS FROM PLUTONIUM BY PRECIPITATION
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.
METHOD OF SEPARATING PLUTONIUM
Heal, H.G.
1960-02-16
BS>A method of separating plutonium from aqueous nitrate solutions of plutonium, uranium. and high beta activity fission products is given. The pH of the aqueous solution is adjusted between 3.0 to 6.0 with ammonium acetate, ferric nitrate is added, and the solution is heated to 80 to 100 deg C to selectively form a basic ferric plutonium-carrying precipitate.
SEPARATION OF PLUTONIUM VALUES FROM URANIUM AND FISSION PRODUCT VALUES
Maddock, A.G.; Booth, A.H.
1960-09-13
Separation of plutonium present in small amounts from neutron irradiated uranium by making use of the phenomenon of chemisorption is described. Plutonium in the tetravalent state is chemically absorbed on a fluoride in solid form. The steps for the separation comprise dissolving the irradiated uranium in nitric acid, oxidizing the plutonium in the resulting solution to the hexavalent state, adding to the solution a soluble calcium salt which by the common ion effect inhibits dissolution of the fluoride by the solution, passing the solution through a bed or column of subdivided calcium fluoride which has been sintered to about 8OO deg C to remove the chemisorbable fission products, reducing the plutonium in the solution thus obtained to the tetravalent state, and again passing the solution through a similar bed or column of calcium fluoride to selectively absorb the plutonium, which may then be recovered by treating the calcium fluoride with a solution of ammonium oxalate.
METHOD OF SEPARATING URANIUM, PLUTONIUM AND FISSION PRODUCTS BY BROMINATION AND DISTILLATION
Jaffey, A.H.; Seaborg, G.T.
1958-12-23
The method for separation of plutonium from uranium and radioactive fission products obtained by neutron irradiation of uranlum consists of reacting the lrradiated material with either bromine, hydrogen bromide, alumlnum bromide, or sulfur and bromine at an elevated temperature to form the bromides of all the elements, then recovering substantlally pure plutonium bromide by dlstillatlon in combinatlon with selective condensatlon at prescribed temperature and pressure.
Plutonium Finishing Plant (PFP) Final Safety Analysis Report (FSAR) [SEC 1 THRU 11
DOE Office of Scientific and Technical Information (OSTI.GOV)
ULLAH, M K
2001-02-26
The Plutonium Finishing Plant (PFP) is located on the US Department of Energy (DOE) Hanford Site in south central Washington State. The DOE Richland Operations (DOE-RL) Project Hanford Management Contract (PHMC) is with Fluor Hanford Inc. (FH). Westinghouse Safety Management Systems (WSMS) provides management support to the PFP facility. Since 1991, the mission of the PFP has changed from plutonium material processing to preparation for decontamination and decommissioning (D and D). The PFP is in transition between its previous mission and the proposed D and D mission. The objective of the transition is to place the facility into a stablemore » state for long-term storage of plutonium materials before final disposition of the facility. Accordingly, this update of the Final Safety Analysis Report (FSAR) reflects the current status of the buildings, equipment, and operations during this transition. The primary product of the PFP was plutonium metal in the form of 2.2-kg, cylindrical ingots called buttoms. Plutonium nitrate was one of several chemical compounds containing plutonium that were produced as an intermediate processing product. Plutonium recovery was performed at the Plutonium Reclamation Facility (PRF) and plutonium conversion (from a nitrate form to a metal form) was performed at the Remote Mechanical C (RMC) Line as the primary processes. Plutonium oxide was also produced at the Remote Mechanical A (RMA) Line. Plutonium processed at the PFP contained both weapons-grade and fuels-grade plutonium materials. The capability existed to process both weapons-grade and fuels-grade material through the PRF and only weapons-grade material through the RMC Line although fuels-grade material was processed through the line before 1984. Amounts of these materials exist in storage throughout the facility in various residual forms left from previous years of operations.« less
METHOD OF SEPARATING TETRAVALENT PLUTONIUM VALUES FROM CERIUM SUB-GROUP RARE EARTH VALUES
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.
Plutonium recovery from spent reactor fuel by uranium displacement
Ackerman, J.P.
1992-03-17
A process is described for separating uranium values and transuranic values from fission products containing rare earth values when the values are contained together in a molten chloride salt electrolyte. A molten chloride salt electrolyte with a first ratio of plutonium chloride to uranium chloride is contacted with both a solid cathode and an anode having values of uranium and fission products including plutonium. A voltage is applied across the anode and cathode electrolytically to transfer uranium and plutonium from the anode to the electrolyte while uranium values in the electrolyte electrolytically deposit as uranium metal on the solid cathode in an amount equal to the uranium and plutonium transferred from the anode causing the electrolyte to have a second ratio of plutonium chloride to uranium chloride. Then the solid cathode with the uranium metal deposited thereon is removed and molten cadmium having uranium dissolved therein is brought into contact with the electrolyte resulting in chemical transfer of plutonium values from the electrolyte to the molten cadmium and transfer of uranium values from the molten cadmium to the electrolyte until the first ratio of plutonium chloride to uranium chloride is reestablished.
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...
Continuous plutonium dissolution apparatus
Meyer, F.G.; Tesitor, C.N.
1974-02-26
This invention is concerned with continuous dissolution of metals such as plutonium. A high normality acid mixture is fed into a boiler vessel, vaporized, and subsequently condensed as a low normality acid mixture. The mixture is then conveyed to a dissolution vessel and contacted with the plutonium metal to dissolve the plutonium in the dissolution vessel, reacting therewith forming plutonium nitrate. The reaction products are then conveyed to the mixing vessel and maintained soluble by the high normality acid, with separation and removal of the desired constituent. (Official Gazette)
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. )
METHOD FOR SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS BY SOLVENT EXTRACTION
Seaborg, G.T.; Blaedel, W.J.; Walling, M.T. Jr.
1960-08-23
A process is given for separating from each other uranium, plutonium, and fission products in an aqueous nitric acid solution by the so-called Redox process. The plutonium is first oxidized to the hexavalent state, e.g., with a water-soluble dichromate or sodium bismuthate, preferably together with a holding oxidant such as potassium bromate. potassium permanganate, or an excess of the oxidizing agent. The solution is then contacted with a water-immiscible organic solvent, preferably hexone. whereby uranium and plutonium are extracted while the fission products remain in the aqueous solution. The separated organic phase is then contacted with an aqueous solution of a reducing agent, with or without a holding reductant (e.g., with a ferrous salt plus hydrazine or with ferrous sulfamate), whereby plutonium is reduced to the trivalent state and back- extracted into the aqueous solution. The uranium may finally be back-extracted from the organic solvent (e.g., with a 0.1 N nitric acid).
SEPARATION OF PLUTONIUM HYDROXIDE FROM BISMUTH HYDROXIDE
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.
METHOD OF MAINTAINING PLUTONIUM IN A HIGHER STATE OF OXIDATION DURING PROCESSING
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.
PROCESSING OF NEUTRON-IRRADIATED URANIUM
Hopkins, H.H. Jr.
1960-09-01
An improved "Purex" process for separating uranium, plutonium, and fission products from nitric acid solutions of neutron-irradiated uranium is offered. Uranium is first extracted into tributyl phosphate (TBP) away from plutonium and fission products after adjustment of the acidity from 0.3 to 0.5 M and heating from 60 to 70 deg C. Coextracted plutonium, ruthenium, and fission products are fractionally removed from the TBP by three scrubbing steps with a 0.5 M nitric acid solution of ferrous sulfamate (FSA), from 3.5 to 5 M nitric acid, and water, respectively, and the purified uranium is finally recovered from the TBP by precipitation with an aqueous solution of oxalic acid. The plutonium in the 0.3 to 0.5 M acid solution is oxidized to the tetravalent state with sodium nitrite and extracted into TBP containing a small amount of dibutyl phosphate (DBP). Plutonium is then back-extracted from the TBP-DBP mixture with a nitric acid solution of FSA, reoxidized with sodium nitrite in the aqueous strip solution obtained, and once more extracted with TBP alone. Finally the plutonium is stripped from the TBP with dilute acid, and a portion of the strip solution thus obtained is recycled into the TBPDBP for further purification.
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
TRANSURANIC ELEMENT, COMPOSITION THEREOF, AND METHODS FOR PRODUCING SEPARATING AND PURIFYING SAME
Wahl, A.C.
1961-09-19
A process of separating plutonium from fission products contained in an aqueous solution is described. Plutonium, in the tri- or tetravalent state, and the fission products are coprecipitated on lanthanum fluoride, lanthanum oxalate, cerous fluoride, cerous phosphate, ceric iodate, zirconyl phosphate, thorium iodate, or thorium fluoride. The precipitate is dissolved in acid, and the plutonium is oxidized to the hexavalent state. The fission products are selectively precipitated on a carrier of the above group but different from that used for the coprecipitation. The plutonium in the solution, after removal of the fission product precipitate, is reduced to at least the tetravalent state and precipitated on lanthanum fluoride, lanthanum phosphate, lanthanum oxalate, lanthanum hydroxide, cerous fluoride, cerous phosphate, cerous oxalate, cerous hydroxide, ceric iodate, zirconyl phosphate, zirconyl iodate, zirconium hydroxide, thorium fluoride, thorium oxalate, thorium iodate, thorium peroxide, uranium iodate, uranium oxalate, or uranium peroxide, again using a different carrier than that used for the precipitation of the fission products.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Neu, Mary Patricia
The coordination chemistry and solution behavior of the toxic ions lead(II) and plutonium(IV, V, VI) have been investigated. The ligand pK as and ligand-lead(II) stability constants of one hydroxamic acid and four thiohydroaxamic acids were determined. Solution thermodynamic results indicate that thiohydroxamic acids are more acidic and slightly better lead chelators than hydroxamates, e.g., N-methylthioaceto-hydroxamic acid, pK a = 5.94, logβ 120 = 10.92; acetohydroxamic acid, pK a = 9.34, logβ 120 = 9.52. The syntheses of lead complexes of two bulky hydroxamate ligands are presented. The X-ray crystal structures show the lead hydroxamates are di-bridged dimers with irregular five-coordinatemore » geometry about the metal atom and a stereochemically active lone pair of electrons. Molecular orbital calculations of a lead hydroxamate and a highly symmetric pseudo octahedral lead complex were performed. The thermodynamic stability of plutonium(IV) complexes of the siderophore, desferrioxamine B (DFO), and two octadentate derivatives of DFO were investigated using competition spectrophotometric titrations. The stability constant measured for the plutonium(IV) complex of DFO-methylterephthalamide is logβ 120 = 41.7. The solubility limited speciation of 242Pu as a function of time in near neutral carbonate solution was measured. Individual solutions of plutonium in a single oxidation state were added to individual solutions at pH = 6.0, T = 30.0, 1.93 mM dissolved carbonate, and sampled over intervals up to 150 days. Plutonium solubility was measured, and speciation was investigated using laser photoacoustic spectroscopy and chemical methods.« less
25. Plutonium Recovery From Contaminated Materials, Architectural Plans & Details, ...
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, ...
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 & ...
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 ...
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
Seaborg, G.T.
1957-10-29
Methods for separating plutonium from the fission products present in masses of neutron irradiated uranium are reported. The neutron irradiated uranium is first dissolved in an aqueous solution of nitric acid. The plutonium in this solution is present as plutonous nitrate. The aqueous solution is then agitated with an organic solvent, which is not miscible with water, such as diethyl ether. The ether extracts 90% of the uraryl nitrate leaving, substantially all of the plutonium in the aqueous phase. The aqueous solution of plutonous nitrate is then oxidized to the hexavalent state, and agitated with diethyl ether again. In the ether phase there is then obtained 90% of plutonium as a solution of plutonyl nitrate. The ether solution of plutonyl nitrate is then agitated with water containing a reducing agent such as sulfur dioxide, and the plutonium dissolves in the water and is reduced to the plutonous state. The uranyl nitrate remains in the ether. The plutonous nitrate in the water may be recovered by precipitation.
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.
SEPARATION OF URANIUM, PLUTONIUM AND FISSION PRODUCTS FROM NEUTRON- BOMBARDED URANIUM
Martin, A.E.; Johnson, I.; Burris, L. Jr.; Winsch, I.O.; Feder, H.M.
1962-11-13
A process is given for removing plutonium and/or fission products from uranium fuel. The fuel is dissolved in molten zinc--magnesium (10 to 18% Mg) alloy, more magnesium is added to obtain eutectic composition whereby uranium precipitates, and the uranium are separated from the Plutoniumand fission-product- containing eutectic. (AEC)
SCAVENGER AND PROCESS OF SCAVENGING
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.
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.
Developing a physiologically based approach for modeling plutonium decorporation therapy with DTPA.
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.
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
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.
10. VIEW OF CALCINER IN ROOM 146148. THE CALCINER HEATED ...
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
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.
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
Forensic investigation of plutonium metal: a case study of CRM 126
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.
Selective Extraction of Uranium from Liquid or Supercritical Carbon Dioxide
DOE Office of Scientific and Technical Information (OSTI.GOV)
Farawila, Anne F.; O'Hara, Matthew J.; Wai, Chien M.
2012-07-31
Current liquid-liquid extraction processes used in recycling irradiated nuclear fuel rely on (1) strong nitric acid to dissolve uranium oxide fuel, and (2) the use of aliphatic hydrocarbons as a diluent in formulating the solvent used to extract uranium. The nitric acid dissolution process is not selective. It dissolves virtually the entire fuel meat which complicates the uranium extraction process. In addition, a solvent washing process is used to remove TBP degradation products, which adds complexity to the recycling plant and increases the overall plant footprint and cost. A liquid or supercritical carbon dioxide (l/sc -CO2) system was designed tomore » mitigate these problems. Indeed, TBP nitric acid complexes are highly soluble in l/sc -CO2 and are capable of extracting uranium directly from UO2, UO3 and U3O8 powders. This eliminates the need for total acid dissolution of the irradiated fuel. Furthermore, since CO2 is easily recycled by evaporation at room temperature and pressure, it eliminates the complex solvent washing process. In this report, we demonstrate: (1) A reprocessing scheme starting with the selective extraction of uranium from solid uranium oxides into a TBP-HNO3 loaded Sc-CO2 phase, (2) Back extraction of uranium into an aqueous phase, and (3) Conversion of recovered purified uranium into uranium oxide. The purified uranium product from step 3 can be disposed of as low level waste, or mixed with enriched uranium for use in a reactor for another fuel cycle. After an introduction on the concept and properties of supercritical fluids, we first report the characterization of the different oxides used for this project. Our extraction system and our online monitoring capability using UV-Vis absorbance spectroscopy directly in sc-CO2 is then presented. Next, the uranium extraction efficiencies and kinetics is demonstrated for different oxides and under different physical and chemical conditions: l/sc -CO2 pressure and temperature, TBP/HNO3 complex used, reductant or complexant used for selectivity, and ionic liquids used as supportive media. To complete the extraction and recovery cycle, we then demonstrate uranium back extraction from the TBP loaded sc-CO2 phase into an aqueous phase and the characterization of the uranium complex formed at the end of this process. Another aspect of this project was to limit proliferation risks by either co-extracting uranium and plutonium, or by leaving plutonium behind by selectively extracting uranium. We report that the former is easily achieved, since plutonium is in the tetravalent or hexavalent oxidation state in the oxidizing environment created by the TBP-nitric acid complex, and is therefore co-extracted. The latter is more challenging, as a reductant or complexant to plutonium has to be used to selectively extract uranium. After undertaking experiments on different reducing or complexing systems (e.g., AcetoHydroxamic Acid (AHA), Fe(II), ascorbic acid), oxalic acid was chosen as it can complex tetravalent actinides (Pu, Np, Th) in the aqueous phase while allowing the extraction of hexavalent uranium in the sc-CO2 phase. Finally, we show results using an alternative media to commonly used aqueous phases: ionic liquids. We show the dissolution of uranium in ionic liquids and its extraction using sc-CO2 with and without the presence of AHA. The possible separation of trivalent actinides from uranium is also demonstrated in ionic liquids using neodymium as a surrogate and diglycolamides as the extractant.« less
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
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.
Cation exchange concentraion of the Americium product from TRUEX
DOE Office of Scientific and Technical Information (OSTI.GOV)
Barney, G.S.; Cooper, T.D.; Fisher, F.D.
1991-06-01
A transuranic extraction (TRUEX) process has been developed to separate and recover plutonium, americium, and other transuranic (TRU) elements from acid wastes. The main objective of the process is to reduce the effluent to below the TRU limit for actinide concentrations (<100 nCi/g of material) so it can be disposed of inexpensively. The process yields a dilute nitric acid stream containing low concentrations of the extracted americium product. This solution also contains residual plutonium and trace amounts of iron. The americium will be absorbed into a cation exchange resin bed to concentrate it for disposal or for future use. Themore » overall objective of these laboratory tests was to determine the performance of the cation exchange process under expected conditions of the TRUEX process. Effects of acid, iron, and americium concentrations on americium absorption on the resin were determined. Distribution coefficients for americium absorption from acide solutions on the resin were measured using batch equilibrations. Batch equilibrations were also used to measure americium absorption in the presence of complexants. This data will be used to identify complexants and solution conditions that can be used to elute the americium from the columns. The rate of absorption was measured by passing solutions containing americium through small columns of resin, varying the flowrates, and measuring the concentrations of americium in the effluent. The rate data will be used to estimate the minimum bed size of the columns required to concentrate the americium product. 11 refs. , 10 figs., 2 tabs.« less
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
SEPARATION OF URANIUM, PLUTONIUM, AND FISSION PRODUCTS
Spence, R.; Lister, M.W.
1958-12-16
Uranium and plutonium can be separated from neutron-lrradiated uranium by a process consisting of dissolvlng the lrradiated material in nitric acid, saturating the solution with a nitrate salt such as ammonium nitrate, rendering the solution substantially neutral with a base such as ammonia, adding a reducing agent such as hydroxylamine to change plutonium to the trivalent state, treating the solution with a substantially water immiscible organic solvent such as dibutoxy diethylether to selectively extract the uranium, maklng the residual aqueous solutlon acid with nitric acid, adding an oxidizing agent such as ammonlum bromate to oxidize the plutonium to the hexavalent state, and selectlvely extracting the plutonium by means of an immlscible solvent, such as dibutoxy dlethyletber.
Hande, M Prakash; Azizova, Tamara V; Burak, Ludmilla E; Khokhryakov, Valentin F; Geard, Charles R; Brenner, David J
2005-09-01
Long-lived, sensitive, and specific biomarkers of particular mutagenic agents are much sought after and potentially have broad applications in the fields of cancer biology, epidemiology, and prevention. Many clastogens induce a spectrum of chromosome aberrations, and some of them can be exploited as biomarkers of exposure. Densely ionizing radiation, for example, alpha particle radiation (from radon or plutonium) and neutron radiation, preferentially induces complex chromosome aberrations, which can be detected by the 24-color multifluor fluorescence in situ hybridization (mFISH) technique. We report the detection and quantification of stable complex chromosome aberrations in lymphocytes of healthy former nuclear-weapons workers, who were exposed many years ago to plutonium, gamma rays, or both, at the Mayak weapons complex in Russia. We analyzed peripheral-blood lymphocytes from these individuals for the presence of persistent complex chromosome aberrations. A significantly elevated frequency of complex chromosome translocations was detected in the highly exposed plutonium workers but not in the group exposed only to high doses of gamma radiation. No such differences were found for simple chromosomal aberrations. The results suggest that stable complex chromosomal translocations represent a long-lived, quantitative, low-background biomarker of densely ionizing radiation for human populations exposed many years ago. (c) 2005 Wiley-Liss, Inc.
Separation by solvent extraction
Holt, Jr., Charles H.
1976-04-06
17. A process for separating fission product values from uranium and plutonium values contained in an aqueous solution, comprising adding an oxidizing agent to said solution to secure uranium and plutonium in their hexavalent state; contacting said aqueous solution with a substantially water-immiscible organic solvent while agitating and maintaining the temperature at from -1.degree. to -2.degree. C. until the major part of the water present is frozen; continuously separating a solid ice phase as it is formed; separating a remaining aqueous liquid phase containing fission product values and a solvent phase containing plutonium and uranium values from each other; melting at least the last obtained part of said ice phase and adding it to said separated liquid phase; and treating the resulting liquid with a new supply of solvent whereby it is practically depleted of uranium and plutonium.
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.
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
The valence-fluctuating ground state of plutonium
Janoschek, Marc; Das, Pinaki; Chakrabarti, Bismayan; ...
2015-07-10
A central issue in material science is to obtain understanding of the electronic correlations that control complex materials. Such electronic correlations frequently arise because of the competition of localized and itinerant electronic degrees of freedom. Although the respective limits of well-localized or entirely itinerant ground states are well understood, the intermediate regime that controls the functional properties of complex materials continues to challenge theoretical understanding. We have used neutron spectroscopy to investigate plutonium, which is a prototypical material at the brink between bonding and nonbonding configurations. In addition, our study reveals that the ground state of plutonium is governed bymore » valence fluctuations, that is, a quantum mechanical superposition of localized and itinerant electronic configurations as recently predicted by dynamical mean field theory. Our results not only resolve the long-standing controversy between experiment and theory on plutonium’s magnetism but also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.« less
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 PREPARING PLUTONIUM TETRAFLUORIDE
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.
Concentration and purification of plutonium or thorium
Hayden, John A.; Plock, Carl E.
1976-01-01
In this invention a first solution obtained from such as a plutonium/thorium purification process or the like, containing plutonium (Pu) and/or thorium (Th) in such as a low nitric acid (HNO.sub.3) concentration may have the Pu and/or Th separated and concentrated by passing an electrical current from a first solution having disposed therein an anode to a second solution having disposed therein a cathode and separated from the first solution by a cation permeable membrane, the Pu or Th cation permeating the cation membrane and forming an anionic complex within the second solution, and electrical current passage affecting the complex formed to permeate an anion membrane separating the second solution from an adjoining third solution containing disposed therein an anode, thereby effecting separation and concentration of the Pu and/or Th in the third solution.
PROCESS FOR PRODUCTION OF PLUTONIUM FROM ITS OXIDES
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.
Retrospective dosimetry related to chronic environmental exposure
NASA Technical Reports Server (NTRS)
Degteva, M. O.; Kozheurov, V. P.; Tolstykh, E. I.; Neta, R. (Principal Investigator)
1998-01-01
Radioactive contamination of the environment occurred in the early fifties as a result of the releases from the Mayak plutonium production complex (Southern Urals, Russia). The releases of liquid wastes into the Techa river resulted in chronic exposure of 30,000 residents of the riverside communities. Since 1951 90Sr body burdens have been measured for over half of this cohort. This paper presents the analysis of data on 90Sr in humans and describes the reconstruction of internal doses for these people.
Retrospective dosimetry related to chronic environmental exposure.
Degteva, M O; Kozheurov, V P; Tolstykh, E I
1998-01-01
Radioactive contamination of the environment occurred in the early fifties as a result of the releases from the Mayak plutonium production complex (Southern Urals, Russia). The releases of liquid wastes into the Techa river resulted in chronic exposure of 30,000 residents of the riverside communities. Since 1951 90Sr body burdens have been measured for over half of this cohort. This paper presents the analysis of data on 90Sr in humans and describes the reconstruction of internal doses for these people.
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)
METHOD OF RECOVERING PLUTONIUM VALUES FROM AQUEOUS SOLUTIONS BY CARRIER PRECIPITATION
James, R.A.; Thompson, S.G.
1959-11-01
A process is presented for pretreating aqueous nitric acid- plutonium solutions containing a small quantity of hydrazine that has formed as a decomposition product during the dissolution of neutron-bombarded uranium in nitric acid and that impairs the precipitation of plutonium on bismuth phosphate. The solution is digested with alkali metal dichromate or potassium permanganate at between 75 and 100 deg C; sulfuric acid at approximately 75 deg C and sodium nitrate, oxaiic acid plus manganous nitrate, or hydroxylamine are added to the solution to secure the plutonium in the tetravalent state and make it suitable for precipitation on BiPO/sub 4/.
METHOD AND MEANS FOR ELECTROLYTIC PURIFICATION OF PLUTONIUM
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.
Nonproliferation and Threat Reduction Assistance: U.S, Programs in the Former Soviet Union
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
Anthropogenic plutonium-244 in the environment: Insights into plutonium’s longest-lived isotope
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
Anthropogenic plutonium-244 in the environment: Insights into plutonium’s longest-lived isotope
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
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
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kushnikov, V.
1996-05-01
The Russian strategy for radioactive waste and plutonium management is based on the concept of the closed fuel cycle that has been adopted in Russia, and, to a great degree, falls under the jurisdiction of the existing Russian nuclear energy structures. From its very beginning, Russian atomic energy policy was based on finding the most effective method of developing the new fuel direction with the maximum possible utilization of the energy potential from the fission of heavy atoms and the achievement of fuel self-sufficiency through the recycling of secondary fuel. Although there can be no doubt about the importance ofmore » economic considerations (for the future), concerns for the safety of the environment are currently of the utmost importance. In this context, spent NPP fuel can be viewed as a waste to be buried only if there is persuasive evidence that such an approach is both economically and environmentally sound. The production of I GW of energy per year is accompanied by the accumulation of up to 800-1000 kg of highly radioactive fission products and approximately 250 kg of plutonium. Currently, spent fuel from the VVER 100 and the RBNK reactors contains approximately 25 tons of plutonium. There is an additional 30 tons of fuel-grade plutonium in the form of purified oxide, separated from spent fuels used in VVER440 reactors and other power production facilities, as well as approximately 100 tons of weapons-grade plutonium from dismantled warheads. The spent fuel accumulates significant amounts of small actinoids - neptunium americium, and curium. Science and technology have not yet found technical solutions for safe and secure burial of non-reprocessed spent fuel with such a broad range of products, which are typically highly radioactive and will continue to pose a threat for hundreds of thousands of years.« less
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.
Determination of origin and intended use of plutonium metal using nuclear forensic techniques.
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.
Determination of origin and intended use of plutonium metal using nuclear forensic techniques
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
DOE R&D Accomplishments Database
Seaborg, G. T.
1981-09-01
The first nuclear synthesis and identification (i.e., the discovery) of the synthetic transuranium element plutonium (isotope /sup 238/Pu) and the demonstration of its fissionability with slow neutrons (isotope /sup 239/Pu) took place at the University of California, Berkeley, through the use of the 60-inch and 37-inch cyclotrons, in late 1940 and early 1941. This led to the development of industrial scale methods in secret work centered at the University of Chicago's Metallurgical Laboratory and the application of these methods to industrial scale production, at manufacturing plants in Tennessee and Washington, during the World War II years 1942 to 1945. The chemical properties of plutonium, needed to devise the procedures for its industrial scale production, were studied by tracer and ultramicrochemical methods during this period on an extraordinarily urgent basis. This work, and subsequent investigations on a worldwide basis, have made the properties of plutonium very well known. Its well studied electronic structure and chemical properties give it a very interesting position in the actinide series of inner transition elements.
Leo Szilard Lectureship Award Talk: Controlling and eliminating nuclear-weapon materials
NASA Astrophysics Data System (ADS)
von Hippel, Frank
2010-02-01
Fissile material -- in practice plutonium and highly enriched uranium (HEU) -- is the essential ingredient in nuclear weapons. Controlling and eliminating fissile material and the means of its production is therefore the common denominator for nuclear disarmament, nuclear non-proliferation and the prevention of nuclear terrorism. From a fundamentalist anti-nuclear-weapon perspective, the less fissile material there is and the fewer locations where it can be found, the safer a world we will have. A comprehensive fissile-material policy therefore would have the following elements: *Consolidation of all nuclear-weapon-usable materials at a minimum number of high-security sites; *A verified ban on the production of HEU and plutonium for weapons; *Minimization of non-weapon uses of HEU and plutonium; and *Elimination of all excess stocks of plutonium and HEU. There is activity on all these fronts but it is not comprehensive and not all aspects are being pursued vigorously or competently. It is therefore worthwhile to review the situation. )
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
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.
CONTINUOUS CHELATION-EXTRACTION PROCESS FOR THE SEPARATION AND PURIFICATION OF METALS
Thomas, J.R.; Hicks, T.E.; Rubin, B.; Crandall, H.W.
1959-12-01
A continuous process is presented for separating metal values and groups of metal values from each other. A complex mixture. e.g., neutron-irradiated uranium, can be resolved into component parts. In the present process the values are dissolved in an acidic solution and adjusted to the proper oxidation state. Thenceforth the solution is contacted with an extractant phase comprising a fluorinated beta -diketone in an organic solvent under centain pH conditions whereupon plutonium and zirconium are extracted. Plutonium is extracted from the foregoing extract with reducing aqueous solutions or under specified acidic conditions and can be recovered from the aqueous solution. Zirconium is then removed with an oxalic acid aqueous phase. The uranium is recovered from the residual original solution using hexone and hexone-diketone extractants leaving residual fission products in the original solution. The uranium is extracted from the hexone solution with dilute nitric acid. Improved separations and purifications are achieved using recycled scrub solutions and the "self-salting" effect of uranyl ions.
PROCESS FOR SEGREGATING URANIUM FROM PLUTONIUM AND FISSION-PRODUCT CONTAMINATION
Ellison, C.V.; Runion, T.C.
1961-06-27
An aqueous nitric acid solution containing uranium, plutonium, and fission product values is contacted with an organic extractant comprised of a trialkyl phosphate and an organic diluent. The relative amounts of trialkyl phosphate and uranium values are controlled to achieve a concentration of uranium values in the organic extractant of at least 0.35 moles uranium per mole of trialkyl phosphate, thereby preferentially extracting uranium values into the organic extractant.
General statistical considerations
DOE Office of Scientific and Technical Information (OSTI.GOV)
Eberhardt, L L; Gilbert, R O
From NAEG plutonium environmental studies program meeting; Las Vegas, Nevada, USA (2 Oct 1973). The high sampling variability encountered in environmental plutonium studies along with high analytical costs makes it very important that efficient soil sampling plans be used. However, efficient sampling depends on explicit and simple statements of the objectives of the study. When there are multiple objectives it may be difficult to devise a wholly suitable sampling scheme. Sampling for long-term changes in plutonium concentration in soils may also be complex and expensive. Further attention to problems associated with compositing samples is recommended, as is the consistent usemore » of random sampling as a basic technique. (auth)« less
IMPROVEMENT UPON THE CARRIER PRECIPITATION OF PLUTONIUM IONS FROM NITRIC ACID SOLUTIONS
James, R.A.; Thompson, S.G.
1958-12-23
A process is reported for improving the removal of plutonlum by carrier precipitation by the addition of nitrite ions to a nitrlc acid solutlon of neutronirradiated unanium so as to destroy any hydrazine that may be present in the solution since the hydrazine tends to complex the tetravalent plutonium and prevents removal by the carrier precipltate, such as bismuth phospbate.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Powell, Brian; Kaplan, Daniel I; Arai, Yuji
2016-12-29
This university lead SBR project is a collaboration lead by Dr. Brian Powell (Clemson University) with co-principal investigators Dan Kaplan (Savannah River National Laboratory), Yuji Arai (presently at the University of Illinois), Udo Becker (U of Michigan) and Rod Ewing (presently at Stanford University). Hypothesis: The underlying hypothesis of this work is that strong interactions of plutonium with mineral surfaces are due to formation of inner sphere complexes with a limited number of high-energy surface sites, which results in sorption hysteresis where Pu(IV) is the predominant sorbed oxidation state. The energetic favorability of the Pu(IV) surface complex is strongly influencedmore » by positive sorption entropies, which are mechanistically driven by displacement of solvating water molecules from the actinide and mineral surface during sorption. Objectives: The overarching objective of this work is to examine Pu(IV) and Pu(V) sorption to pure metal (oxyhydr)oxide minerals and sediments using variable temperature batch sorption, X-ray absorption spectroscopy, electron microscopy, and quantum-mechanical and empirical-potential calculations. The data will be compiled into a self-consistent surface complexation model. The novelty of this effort lies largely in the manner the information from these measurements and calculations will be combined into a model that will be used to evaluate the thermodynamics of plutonium sorption reactions as well as predict sorption of plutonium to sediments from DOE sites using a component additivity approach.« less
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.
A CHEMICAL METHOD OF TREATING FISSIONABLE MATERIAL
Olson, C.M.
1959-09-01
One step of a process for separating plutonium from uranium and fission products is presented. A nitric acid solution containing these constituents is treated with formic acid to reduce simultaneously the plutonium to a valence state of not greater than +4 and destroy and eliminate the excess nitric acid.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Iseki, Tadahiro; Inaba, Makoto; Takahashi, Naoki
During the second and third steps of Active Test at Rokkasho Reprocessing Plant (RRP), the performances of the Separation Facility have been checked; (A) diluent washing efficiency, (B) plutonium stripping efficiency, (C) decontamination factor of fission products and (D) plutonium and uranium leakage into raffinate and spent solvent. Test results were equivalent to or better than expected. (authors)
REDUCTION IN Pu RECOVERY PROCESSES
Ritter, D.M.; Black, R.P.S.
1959-09-29
A method is described for reducing plutonium from the hexavalent to the tetravalent state in a carrier precipitation process for separating plutonium and nuclear fission products. In accordance with the invention oxalate ions are incorporated in the hexavalent plutoniumcontaining solution prior to a step of precipitating lanthanum fluoride in the solution.
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
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
ZIRCONIUM PHOSPHATE ADSORPTION METHOD
Russell, E.R.; Adamson, A.S.; Schubert, J.; Boyd, G.E.
1958-11-01
A method is presented for separating plutonium values from fission product values in aqueous acidic solution. This is accomplished by flowing the solutlon containing such values through a bed of zirconium orthophosphate. Any fission products adsorbed can subsequently be eluted by washing the column with a solution of 2N HNO/sub 3/ and O.lN H/sub 3/PO/sub 4/. Plutonium values may subsequently be desorbed by contacting the column with a solution of 7N HNO/sub 3/ .
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
Removal of dissolved actinides from alkaline solutions by the method of appearing reagents
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.
Coffinberry, A.S.
1962-04-10
A process for removing fission products from reactor liquid fuel without interfering with the reactor's normal operation or causing a significant change in its fuel composition is described. The process consists of mixing a liquid scavenger alloy composed of about 44 at.% plutoniunm, 33 at.% lanthanum, and 23 at.% nickel or cobalt with a plutonium alloy reactor fuel containing about 3 at.% lanthanum; removing a portion of the fuel and scavenger alloy from the reactor core and replacing it with an equal amount of the fresh scavenger alloy; transferring the portion to a quiescent zone where the scavenger and the plutonium fuel form two distinct liquid layers with the fission products being dissolved in the lanthanum-rich scavenger layer; and the clean plutonium-rich fuel layer being returned to the reactor core. (AEC)
Investigation Of In-Line Monitoring Options At H Canyon/HB Line For Plutonium Oxide Production
DOE Office of Scientific and Technical Information (OSTI.GOV)
Sexton, L.
2015-10-14
H Canyon and HB Line have a production goal of 1 MT per year of plutonium oxide feedstock for the MOX facility by FY17 (AFS-2 mission). In order to meet this goal, steps will need to be taken to improve processing efficiency. One concept for achieving this goal is to implement in-line process monitoring at key measurement points within the facilities. In-line monitoring during operations has the potential to increase throughput and efficiency while reducing costs associated with laboratory sample analysis. In the work reported here, we mapped the plutonium oxide process, identified key measurement points, investigated alternate technologies thatmore » could be used for in-line analysis, and initiated a throughput benefit analysis.« less
Baseline process description for simulating plutonium oxide production for precalc project
DOE Office of Scientific and Technical Information (OSTI.GOV)
Pike, J. A.
Savannah River National Laboratory (SRNL) started a multi-year project, the PreCalc Project, to develop a computational simulation of a plutonium oxide (PuO 2) production facility with the objective to study the fundamental relationships between morphological and physicochemical properties. This report provides a detailed baseline process description to be used by SRNL personnel and collaborators to facilitate the initial design and construction of the simulation. The PreCalc Project team selected the HB-Line Plutonium Finishing Facility as the basis for a nominal baseline process since the facility is operational and significant model validation data can be obtained. The process boundary as wellmore » as process and facility design details necessary for multi-scale, multi-physics models are provided.« less
Nuclear Weapons: Comprehensive Test Ban Treaty
2006-07-10
continued...) The complex could contain explosions up to 500 pounds of explosive and associated plutonium. Another SCE, “ Unicorn ,” is to be conducted...scheduled for FY2006, as noted below. SCEs try to determine if radioactive decay of aged plutonium would degrade weapon performance. Several SCEs...Richardson called SCEs “a key part of our scientific program to provide new tools and data that assess age -related complications and maintain the reliability
SULFIDE METHOD PLUTONIUM SEPARATION
Duffield, R.B.
1958-08-12
A process is described for the recovery of plutonium from neutron irradiated uranium solutions. Such a solution is first treated with a soluble sullide, causing precipitation of the plutoniunn and uraniunn values present, along with those impurities which form insoluble sulfides. The precipitate is then treated with a solution of carbonate ions, which will dissolve the uranium and plutonium present while the fission product sulfides remain unaffected. After separation from the residue, this solution may then be treated by any of the usual methods, such as formation of a lanthanum fluoride precipitate, to effect separation of plutoniunn from uranium.
Nash, K.L.; Cleveland, J.M.; Sullivan, J.C.; Woods, M.
1986-01-01
The rate of reduction of plutonium(VI) and neptunium(VI) by bisulfide ion in neutral and mildly alkaline solutions has been investigated by the stopped-flow technique. The reduction of both of these ions to the pentavalent oxidation state appears to occur in an intramolecular reaction involving an unusual actinide(VI)-hydroxide-bisulfide complex. For plutonium the rate of reduction is 27.4 (??4.1) s-1 at 25??C with ??H* = +33.2 (??1.0) kJ/mol and ??S* = -106 (??4) J/(mol K). The apparent stability constant for the transient complex is 4.66 (??0.94) ?? 103 M-1 at 25??C with associated thermodynamic parameters of ??Hc = +27.7 (??0.4) kJ/mol and ??Sc = +163 (??2) J/(mol K). The corresponding rate and stability constants are determined for the neptunium system at 25??C (k3 = 139 (??30) s-1, Kc. = 1.31 (??0.32) ?? 103 M-1), but equivalent parameters cannot be determined at reduced temperatures. The reaction rate is decreased by bicarbonate ion. At pH > 10.5, a second reaction mechanism, also involving a sulfide complex, is indicated. ?? 1986 American Chemical Society.
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Byerly, Benjamin L.; Stanley, Floyd; Spencer, Khal
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.
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
9. VIEW LOOKING SOUTHEAST AT THE 771 AREA COMPLEX. ...
9. VIEW LOOKING SOUTHEAST AT THE 771 - AREA COMPLEX. THE 711 COMPLEX, ORIGINALLY KNOWN AS PLANT C, HOUSED ALL THE PLUTONIUM PROCESSES UNTIL 1956 WHEN BUILDING 776/777 BECAME OPERATIONAL. - Rocky Flats Plant, Bounded by Indiana Street & Routes 93, 128 & 72, Golden, Jefferson County, CO
IMPROVEMENTS IN OR RELATING TO THE PRODUCTION OF SINTERED URANIUM DIOXIDE
DOE Office of Scientific and Technical Information (OSTI.GOV)
Russell, L.E.; Harrison, J.D.L.; Brett, N.H.
A method is described for producing a dense sintered body of uranium dioxide or a mixture thereof with plutonium dioxide. Compacted uranium dioxide or a compacted uranium dioxide-plutonium dioxide mixture is heated to at least 1300 deg C in an atmosphere of carbon dioxide or carbon dioxide mixed with carbon monoxide. (R.J.S.)
FUSED SALT PROCESS FOR RECOVERY OF VALUES FROM USED NUCLEAR REACTOR FUELS
Moore, R.H.
1960-08-01
A process is given for recovering plutonium from a neutron-irradiated uranium mass (oxide or alloy) by dissolving the mass in an about equimolar alkali metalaluminum double chloride, adding aluminum metal to the mixture obtained at a temperature of between 260 and 860 deg C, and separating a uranium-containing metal phase and a plutonium-chloride- and fission-product chloridecontaining salt phase. Dissolution can be expedited by passing carbon tetrachloride vapors through the double salt. Separation without reduction of plutonium from neutron- bombarded uranium and that of cerium from uranium are also discussed.
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.
PEROXIDE PROCESS FOR SEPARATION OF RADIOACTIVE MATERIALS
Seaborg, G.T.; Perlman, I.
1958-09-16
reduced state, from hexavalent uranium. It consists in treating an aqueous solution containing such uranium and plutonium ions with sulfate ions in order to form a soluble uranium sulfate complex and then treating the solution with a soluble thorium compound and a soluble peroxide compound in order to ferm a thorium peroxide carrier precipitate which carries down with it the plutonium peroxide present. During this treatment the pH of the solution must be maintained between 2 and 3.
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
METHOD OF MAKING ALLOYS OF BERYLLIUM WITH PLUTONIUM AND THE LIKE
Runnals, O.J.C.
1959-02-24
The production of alloys of beryllium with one or more of the metals uranium, plutonium, actinium, americium, curium, thorium, and cerium are described. A halide salt of the metal to be alloyed with the beryllium is heated at 1300 deg C in the presence of beryllium to reduce the halide to metal and cause the latter to alloy directly with the beryllium. Although the heavy metal halides are more stable, thermodynamically, than the beryllium halides, the reducing reaction proceeds to completion if the beryllium halide product is continuously removed by vacuum distillation.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Rim, Jung H.; Kuhn, Kevin J.; Tandon, Lav
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
Distillation of cadmium from uranium plutonium cadmium alloy
NASA Astrophysics Data System (ADS)
Kato, Tetsuya; Iizuka, Masatoshi; Inoue, Tadashi; Iwai, Takashi; Arai, Yasuo
2005-04-01
Uranium-plutonium alloy was prepared by distillation of cadmium from U-Pu-Cd ternary alloy. The initial ternary alloy contained 2.9 wt% U and 8.7 wt% Pu other than Cd, which were recovered by molten salt electrolysis with liquid Cd cathode. The distillation experiments were conducted in 10 g scale of the initial alloy using a small-scale distillation furnace equipped with an evaporator and a condenser in a vacuum vessel. After distillation at 1073 K, the weight of the residue was in good agreement with that of the loaded actinides, where the content of Cd decreased to less than 0.05 wt%. The uranium-plutonium alloy product was recovered without adhering to the yttria crucible. The cross section of the product was observed using electron probe micro-analyzer and it was found to consist of a dense material. Almost all of the evaporated Cd was recovered in the condenser and so enclosed well in the apparatus.
a Plutonium Ceramic Target for Masha
NASA Astrophysics Data System (ADS)
Wilk, P. A.; Shaughnessy, D. A.; Moody, K. J.; Kenneally, J. M.; Wild, J. F.; Stoyer, M. A.; Patin, J. B.; Lougheed, R. W.; Ebbinghaus, B. B.; Landingham, R. L.; Oganessian, Yu. Ts.; Yeremin, A. V.; Dmitriev, S. N.
2005-09-01
We are currently developing a plutonium ceramic target for the MASHA mass separator. The MASHA separator will use a thick plutonium ceramic target capable of tolerating temperatures up to 2000 °C. Promising candidates for the target include oxides and carbides, although more research into their thermodynamic properties will be required. Reaction products will diffuse out of the target into an ion source, where they will then be transported through the separator to a position-sensitive focal-plane detector array. Experiments on MASHA will allow us to make measurements that will cement our identification of element 114 and provide for future experiments where the chemical properties of the heaviest elements are studied.
Source-term characterisation and solid speciation of plutonium at the Semipalatinsk NTS, Kazakhstan.
Nápoles, H Jiménez; León Vintró, L; Mitchell, P I; Omarova, A; Burkitbayev, M; Priest, N D; Artemyev, O; Lukashenko, S
2004-01-01
New data on the concentrations of key fission/activation products and transuranium nuclides in samples of soil and water from the Semipalatinsk Nuclear Test Site are presented and interpreted. Sampling was carried out at Ground Zero, Lake Balapan, the Tel'kem craters and reference locations within the test site boundary well removed from localised sources. Radionuclide ratios have been used to characterise the source term(s) at each of these sites. The geochemical partitioning of plutonium has also been examined and it is shown that the bulk of the plutonium contamination at most of the sites examined is in a highly refractory, non-labile form.
The North Korean nuclear dilemma.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hecker, Siegfried S.
2004-01-01
The current nuclear crisis, the second one in ten years, erupted when North Korea expelled international nuclear inspectors in December 2002, then withdrew from the Nuclear Nonproliferation Treaty (NPT), and claimed to be building more nuclear weapons with the plutonium extracted from the spent fuel rods heretofore stored under international inspection. These actions were triggered by a disagreement over U.S. assertions that North Korea had violated the Agreed Framework (which froze the plutonium path to nuclear weapons to end the first crisis in 1994) by clandestinely developing uranium enrichment capabilities providing an alternative path to nuclear weapons. With Stanford Universitymore » Professor John Lewis and three other Americans, I was allowed to visit the Yongbyon Nuclear Center on Jan. 8, 2004. We toured the 5 MWe reactor, the 50 MWe reactor construction site, the spent fuel pool storage building, and the radiochemical laboratory. We concluded that North Korea has restarted its 5 MWe reactor (which produces roughly 6 kg of plutonium annually), it removed the 8000 spent fuel rods that were previously stored under IAEA safeguards from the spent fuel pool, and that it most likely extracted the 25 to 30 kg of plutonium contained in these fuel rods. Although North Korean officials showed us what they claimed was their plutonium metal product from this reprocessing campaign, we were not able to conclude definitively that it was in fact plutonium metal and that it came from the most recent reprocessing campaign. Nevertheless, our North Korean hosts demonstrated that they had the capability, the facility and requisite capacity, and the technical expertise to produce plutonium metal. On the basis of our visit, we were not able to address the issue of whether or not North Korea had a 'deterrent' as claimed - that is, we were not able to conclude that North Korea can build a nuclear device and that it can integrate nuclear devices into suitable delivery systems. However, based on the capabilities we saw, we must assume that North Korea has the capability to produce a crude nuclear device. On the matter of uranium enrichment programs, our host categorically denied that North Korea has a uranium enrichment program - he said, 'we have no program, no equipment, and no technical expertise for uranium enrichment.' The denials were not convincing at the time and since then have proven to be quite hollow by the revelations of A.Q. Khan's nuclear black market activities. There is no easy solution to the nuclear crisis in North Korea. A military strike to eliminate the nuclear facilities was never very attractive and now has been overcome by events. The principal threat is posed by a stockpile of nuclear weapons and weapons-grade plutonium. We have no way of finding where either may be hidden. A diplomatic solution remains the only path forward, but it has proven elusive. All sides have proclaimed a nuclear weapons-free Korean Peninsula as the end goal. The U.S. Government has chosen to negotiate with North Korea by means of the six-party talks. It has very clearly outlined its position of insisting on complete, verifiable, irreversible dismantlement of all North Korean nuclear programs. North Korea has offered several versions of 're-freezing' its plutonium program while still denying a uranium enrichment program. It has insisted on simultaneous and reciprocal steps to a final solution. Regardless of which diplomatic path is chosen, the scientific challenges of eliminating the North Korean nuclear weapons programs (and its associated infrastructure) in a safe, secure, and verifiable manner are immense. The North Korean program is considerably more complex and developed than the fledgling Iraqi program of 1991 and Libyan program of 2004. It is more along the lines, but more complex than that of South Africa in the early 1990s. Actions taken or not taken by the North Koreans at their nuclear facilities during the course of the ongoing diplomatic discussions are key to whether or not the nuclear program can be eliminated safely and securely, and they will greatly influence the price tag for such operations. Moreover, they will determine whether or not one can verify complete elimination. Hence, cooperation of the North Koreans now and during the dismantlement and elimination stages is crucial. Technical discussions among specialists, perhaps within the framework of the working groups of the six-party talks, could be very productive in setting the stage for an effective, verifiable elimination of North Korea's nuclear weapons program.« less
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.
Falling Behind: International Scrutiny of the Peaceful Atom
2008-02-01
confused with critical masses .5 Significant quantity values currently in use by the IAEA are given in Table 1. In a previous Natural Resources... actinides and fission products would not add significantly to the plutonium mass , the state could divert the spiked plutonium to a small clandestine...and manufacturing processes and should not be 152 confused with critical masses . Significant quantities are used in establishing the quantity
The measurement of U(VI) and Np(IV) mass transfer in a single stage centrifugal contactor
NASA Astrophysics Data System (ADS)
May, I.; Birkett, E. J.; Denniss, I. S.; Gaubert, E. T.; Jobson, M.
2000-07-01
BNFL currently operates two reprocessing plants for the conversion of spent nuclear fuel into uranium and plutonium products for fabrication into uranium oxide and mixed uranium and plutonium oxide (MOX) fuels. To safeguard the future commercial viability of this process, BNFL is developing novel single cycle flowsheets that can be operated in conjunction with intensified centrifugal contactors.
SEPARATION OF TRANSURANIC ELEMENTS FROM RARE EARTH COMPOUNDS
Kohman, T.P.
1961-11-21
A process of separating neptunium and plutonium values from rare earths and alkaline earth fission products present on a solid mixed actinide carrier (Th or U(IV) oxalate or fluoride) --fission product carrier (LaF/sub 3/, CeF/sub 3/, SrF/sub 2/, CaF/sub 2/, YF/sub 3/, La oxalate, cerous oxalate, Sr oxalate, Ca oxalate or Y oxalate) by extraction of the actinides at elevated temperature with a solution of ammonium fluoride and/or ammonium oxalate is described. Separation of the fission-product-containing carriers from the actinide solution formed and precipitation of the neptunium and plutonium from the solution with mineral acid are also accomplished. (AEC)
Seismic analyses of equipment in 2736-Z complex. Revision 1
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ocoma, E.C.
1995-04-01
This report documents the structural qualification for the existing equipment when subjected to seismic loading in the Plutonium Storage Complex. It replaces in entirety Revision 0 and reconciles the U.S. Department of Energy (DOE) comments on Revision 0. The Complex consists of 2736-Z Building (plutonium storage vault), 2736-ZA Building (vault ventilation equipment building), and 2736-ZB Building (shipping/receiving, repackaging activities). The existing equipment structurally qualified in this report are the metal storage racks for 7 inch and lard cans in room 2 of Building 2736-Z; the cubicles, can holders and pedestals in rooms 1, 3, and 4 of Building 2736-Z; themore » ventilation duct including exhaust fans/motors, emergency diesel generator, and HEPA filter housing in Building 2736-ZA; the repackaging glovebox in Building 2736-ZB; and the interface duct between Buildings 2736-Z and 2736-ZA.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
None
1960-01-01
Thirty-one papers and 10 summaries of papers presented at the Third Conference on Analytical Chemistry in Nuclear Reactor Technology held at Gatlinburg, Tennessee, October 26 to 29, 1959, are given. The papers are grouped into four sections: general, analytical chemistry of fuels, analytical chemistry of plutonium and the transplutonic elements, and the analysis of fission-product mixtures. Twenty-seven of the papers are covered by separate abstracts. Four were previously abstracted for NSA. (M.C.G.)
Method of making alloys of beryllium with plutonium and the like
Runnals, O J.C.
1959-02-24
The production or alloys of beryllium with one or more of the metals uranium, plutonium, actinium, americium, curium, thorium, and cerium is described. A halide salt or the metal to be alloyed with the beryllium is heated at l3O0 deg C in the presence of beryllium to reduce the halide to metal and cause the latter to alloy directly with the beryllium. Although the heavy metal halides are more stable, thermodynamically, than the beryllium halides, the reducing reaction proceeds to completion if the beryllium halide product is continuously removed by vacuum distillation.
Radioisotope contaminations from releases of the Tomsk-Seversk nuclear facility (Siberia, Russia).
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.
A Plutonium Ceramic Target for MASHA
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wilk, P A; Shaughnessy, D A; Moody, K J
2004-07-06
We are currently developing a plutonium ceramic target for the MASHA mass separator. The MASHA separator will use a thick plutonium ceramic target capable of tolerating temperatures up to 2000 C. Promising candidates for the target include oxides and carbides, although more research into their thermodynamic properties will be required. Reaction products will diffuse out of the target into an ion source, where they will then be transported through the separator to a position-sensitive focal-plane detector array. Experiments on MASHA will allow us to make measurements that will cement our identification of element 114 and provide for future experiments wheremore » the chemical properties of the heaviest elements are studied.« 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
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
White, M.G.; Pfuderer, H.A.
This bibliography serves as a guide to the environmental studies sponsored by the Nevada Applied Ecology Group (NAEG) at the Department of Energy Nevada Test Site nuclear weapons complex. The NAEG is part of the Nevada Operations Office of the United States Department of Energy. The references included in the bibliography reflect the interests of the NAEG (e.g., hazard evaluation of the nuclear safety-shot sites). The objectives of the NAEG plutonium studies at the Nevada Test Site were defined as follows: (1) delineate locations of contamination; (2) determine concentrations in ecosystem components; (3) quantify rates of movements among ecosystem components;more » (4) evaluate radiological hazards of plutonium; (5) identify areas which need to be cleaned up or treated; and (6) develop techniques for cleanup or treatment.« less
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
Preparation of plutonium-bearing ceramics via mechanically activated precursor
NASA Astrophysics Data System (ADS)
Chizhevskaya, S. V.; Stefanovsky, S. V.
2000-07-01
The problem of excess weapons plutonium disposition is suggested to be solved by means of its incorporation in stable ceramics with high chemical durability and radiation resistivity. The most promising host phases for plutonium as well as uranium and neutron poisons (gadolinium, hafnium) are zirconolite, pyrochlore, zircon, zirconia [1,2], and murataite [3]. Their production requires high temperatures and a fine-grained homogeneous precursor to reach final waste form with high quality and low leachability. Currently various routes to homogeneous products preparation such as sol-gel technology, wet-milling, and grinding in a ball or planetary mill are used. The best result demonstrates sol-gel technology but this route is very complicated. An alternative technology for preparation of ceramic precursors is the treatment of the oxide batch with high mechanical energy [4]. Such a treatment produces combination of mechanical (fine milling with formation of various defects, homogenization) and chemical (split bonds with formation of active centers—free radicals, ion-radicals, etc.) effects resulting in higher reactivity of the activated batch.
Effect of Natural Organic Matter on Plutonium Sorption to Goethite
Conroy, Nathan A.; Zavarin, Mavrik; Kersting, Annie B.; ...
2016-11-21
For this research, the effect of citric acid (CA), desferrioxamine B (DFOB), fulvic acid (FA), and humic acid (HA) on plutonium (Pu) sorption to goethite was studied as a function of organic carbon concentration and pH using batch sorption experiments at 5 mg C·L –1 and 50 mg C·L –1 natural organic matter (NOM), 10 –9–10 –10 M 238Pu, and 0.1 g·L –1 goethite concentrations, at pH 3, 5, 7, and 9. Low sorption of ligands coupled with strong Pu complexation decreased Pu sorption at pH 5 and 7, relative to a ligand-free system. Conversely, CA, FA, and HA increasedmore » Pu sorption to goethite at pH 3, suggesting ternary complex formation or, in the case of humic acid, incorporation into HA aggregates. Mechanisms for ternary complex formation were characterized by Fourier transform infrared spectroscopy in the absence of Pu. CA and FA demonstrated clear surface interactions at pH 3, HA appeared unchanged suggesting HA aggregates had formed, and no DFOB interactions were observed. Plutonium sorption decreased in the presence of DFOB (relative to a ligand free system) at all pH values examined. Thus, DFOB does not appear to facilitate formation of ternary Pu-DFOB-goethite complexes. At pH 9, Pu sorption in the presence of all NOM increased relative to pH 5 and 7; speciation models attributed this to Pu(IV) hydrolysis competing with ligand complexation, increasing sorption. In conclusion, the results indicate that in simple Pu-NOM-goethite ternary batch systems, NOM will decrease Pu sorption to goethite at all but particularly low pH conditions.« less
Effect of Natural Organic Matter on Plutonium Sorption to Goethite
DOE Office of Scientific and Technical Information (OSTI.GOV)
Conroy, Nathan A.; Zavarin, Mavrik; Kersting, Annie B.
For this research, the effect of citric acid (CA), desferrioxamine B (DFOB), fulvic acid (FA), and humic acid (HA) on plutonium (Pu) sorption to goethite was studied as a function of organic carbon concentration and pH using batch sorption experiments at 5 mg C·L –1 and 50 mg C·L –1 natural organic matter (NOM), 10 –9–10 –10 M 238Pu, and 0.1 g·L –1 goethite concentrations, at pH 3, 5, 7, and 9. Low sorption of ligands coupled with strong Pu complexation decreased Pu sorption at pH 5 and 7, relative to a ligand-free system. Conversely, CA, FA, and HA increasedmore » Pu sorption to goethite at pH 3, suggesting ternary complex formation or, in the case of humic acid, incorporation into HA aggregates. Mechanisms for ternary complex formation were characterized by Fourier transform infrared spectroscopy in the absence of Pu. CA and FA demonstrated clear surface interactions at pH 3, HA appeared unchanged suggesting HA aggregates had formed, and no DFOB interactions were observed. Plutonium sorption decreased in the presence of DFOB (relative to a ligand free system) at all pH values examined. Thus, DFOB does not appear to facilitate formation of ternary Pu-DFOB-goethite complexes. At pH 9, Pu sorption in the presence of all NOM increased relative to pH 5 and 7; speciation models attributed this to Pu(IV) hydrolysis competing with ligand complexation, increasing sorption. In conclusion, the results indicate that in simple Pu-NOM-goethite ternary batch systems, NOM will decrease Pu sorption to goethite at all but particularly low pH conditions.« less
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
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
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
241Am Ingrowth and Its Effect on Internal Dose
Konzen, Kevin
2016-07-01
Generally, plutonium has been manufactured to support commercial and military applications involving heat sources, weapons and reactor fuel. This work focuses on three typical plutonium mixtures, while observing the potential of 241Am ingrowth and its effect on internal dose. The term “ingrowth” is used to describe 241Am production due solely from the decay of 241Pu as part of a plutonium mixture, where it is initially absent or present in a smaller quantity. Dose calculation models do not account for 241Am ingrowth unless the 241Pu quantity is specified. This work suggested that 241Am ingrowth be considered in bioassay analysis when theremore » is a potential of a 10% increase to the individual’s committed effective dose. It was determined that plutonium fuel mixtures, initially absent of 241Am, would likely exceed 10% for typical reactor grade fuel aged less than 30 years; however, heat source grade and aged weapons grade fuel would normally fall below this threshold. In conclusion, although this work addresses typical plutonium mixtures following separation, it may be extended to irradiated commercial uranium fuel and is expected to be a concern in the recycling of spent fuel.« less
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
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
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
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
Nonproliferation and Threat Reduction Assistance: U.S. Programs in the Former Soviet Union
2009-07-31
seeks to help Russia reconfigure its large - scale former BW-related facilities so that they can perform peaceful research issues such as infectious...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 consume, would undermine
Nonproliferation and Threat Reduction Assistance: U.S. Programs in the Former Soviet Union
2011-04-26
large - scale former BW-related facilities so that they can perform peaceful research issues such as infectious diseases. The Global Threat Reduction...indicated that it may not pursue the MOX 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
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hellesen, C.; Grape, S.; Haakanson, A.
2013-07-01
Fertile blankets can be used in fast reactors to enhance the breeding gain as well as the passive safety characteristics. However, such blankets typically result in the production of weapons grade plutonium. For this reason they are often excluded from Generation IV reactor designs. In this paper we demonstrate that using blankets manufactured directly from spent light water (LWR) reactor fuel it is possible to produce a plutonium product with non-proliferation characteristics on a par with spent LWR fuel of 30-50 MWd/kg burnup. The beneficial breeding and safety characteristics are retained. (authors)
The role of troublesome components in plutonium vitrification
DOE Office of Scientific and Technical Information (OSTI.GOV)
Li, Hong; Vienna, J.D.; Peeler, D.K.
1996-05-01
One option for immobilizing surplus plutonium is vitrification in a borosilicate glass. Two advantages of the glass form are (1) high tolerance to feed variability and, (2) high solubility of some impurity components. The types of plutonium-containing materials in the United States inventory include: pits, metals, oxides, residues, scrap, compounds, and fuel. Many of them also contain high concentrations of carbon, chloride, fluoride, phosphate, sulfate, and chromium oxide. To vitrify plutonium-containing scrap and residues, it is critical to understand the impact of each component on glass processing and chemical durability of the final product. This paper addresses glass processing issuesmore » associated with these troublesome components. It covers solubility limits of chlorine, fluorine, phosphate, sulfate, and chromium oxide in several borosilicate based glasses, and the effect of each component on vitrification (volatility, phase segregation, crystallization, and melt viscosity). Techniques (formulation, pretreatment, removal, and/or dilution) to mitigate the effect of these troublesome components are suggested.« less
Kazzi, Ziad N; Heyl, Alexander; Ruprecht, Johann
2012-08-01
The accidental or intentional release of plutonium or americium can cause acute and long term adverse health effects if they enter the human body by ingestion, inhalation, or injection. These effects can be prevented by rapid removal of these radionuclides by chelators such as calcium or zinc diethylenetriaminepentaacetate (calcium or zinc DTPA). These compounds have been shown to be efficacious in enhancing the elimination of members of the actinide family particularly plutonium and americium when administered intravenously or by nebulizer. The efficacy and adverse effects profile depend on several factors that include the route of internalization of the actinide, the type, and route time of administration of the chelator, and whether the calcium or zinc salt of DTPA is used. Current and future research efforts should be directed at overcoming limitations associated with the use of these complex drugs by using innovative methods that can enhance their structural and therapeutic properties.
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
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.
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
Balanced program plan. Analysis for biomedical and environmental research
DOE Office of Scientific and Technical Information (OSTI.GOV)
Not Available
1976-06-01
Major issues associated with the use of nuclear power are health hazards of exposure to radioactive materials; sources of radiation exposure; reactor accidents; sabotage of nuclear facilities; diversion of fissile material and its use for extortion; and the presence of plutonium in the environment. Fission fuel cycle technology is discussed with regard to milling, UF/sub 6/ production, uranium enrichment, plutonium fuel fabrication, power production, fuel processing, waste management, and fuel and waste transportation. The following problem areas of fuel cycle technology are briefly discussed: characterization, measurement, and monitoring; transport processes; health effects; ecological processes and effects; and integrated assessment. Estimatedmore » program unit costs are summarized by King-Muir Category. (HLW)« less
Status summary of chemical processing development in plutonium-238 supply program
DOE Office of Scientific and Technical Information (OSTI.GOV)
Collins, Emory D.; Benker, Dennis; Wham, Robert M.
This document summarizes the status of development of chemical processing in the Plutonium-238 Supply Program (PSP) near the end of Demonstration 1. The objective of the PSP is “to develop, demonstrate, and document a production process that meets program objectives and to prepare for its operation” (Frazier et al. 2016). Success in the effort includes establishing capability using the current infrastructure to produce Np targets for irradiation in Department of Energy research reactors, chemically processing the irradiated targets to separate and purify the produced Pu and transferring the PuO 2 product to Los Alamos National Laboratory (LANL) at an averagemore » rate of 1.5 kg/y.« less
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.
Graphene-based filament material for thermal ionization
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hewitt, J.; Shick, C.; Siegfried, M.
The use of graphene oxide materials for thermal ionization mass spectrometry analysis of plutonium and uranium has been investigated. Filament made from graphene oxide slurries have been 3-D printed. A method for attaching these filaments to commercial thermal ionization post assemblies has been devised. Resistive heating of the graphene based filaments under high vacuum showed stable operation in excess of 4 hours. Plutonium ion production has been observed in an initial set of filaments spiked with the Pu 128 Certified Reference Material.
Booth, Corwin H.; Olive, Daniel Thomas
2016-10-26
This focused review provides an overview and a framework for understanding local structure in metallic plutonium (especially the metastable fcc δ-phase alloyed with Ga) as it relates to self-irradiation damage. Of particular concern is the challenge of understanding self-irradiation damage in plutonium-bearing materials where theoretical challenges of the unique involvement of the 5f electrons in bonding limit the efficacy of molecular dynamics simulations and experimental challenges of working with radioactive material have limited the ability to confirm the results of such simulations and to further push the field forward. The main concentration is on extended X-ray absorption fine-structure measurements ofmore » -phase Pu, but the scope is broadened to include certain studies on plutonium intermetallics and oxides insofar as they inform the physics of damage and healing processes in elemental Pu. Here, the studies reviewed here provide insight into lattice distortions and their production, damage annealing and defect migration, and the importance of understanding and controlling sample morphology when interpreting such experiments.« less
MIS High-Purity Plutonium Oxide Hydride Product 5501579 (SSR124): 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 5501579 represents process plutonium oxides from hydride oxide from Rocky Flats that are currently stored in 3013 containers. After calcination to 950°C, the material contained 87.42% 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 a 3013 container. Gas compositions were measured periodically overmore » a six year period. The maximum observed gas pressure was 124 kPa. The increase over the initial pressure of 70 kPa was primarily due to generation of nitrogen and carbon dioxide gas. 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.« less
Supplying the nuclear arsenal: Production reactor technology, management, and policy, 1942--1992
DOE Office of Scientific and Technical Information (OSTI.GOV)
Carlisle, R.P.; Zenzen, J.M.
1994-01-01
This book focuses on the lineage of America`s production reactors, those three at Hanford and their descendants, the reactors behind America`s nuclear weapons. The work will take only occasional sideways glances at the collateral lines of descent, the reactor cousins designed for experimental purposes, ship propulsion, and electric power generation. Over the decades from 1942 through 1992, fourteen American production reactors made enough plutonium to fuel a formidable arsenal of more than twenty thousand weapons. In the last years of that period, planners, nuclear engineers, and managers struggled over designs for the next generation of production reactors. The story ofmore » fourteen individual machines and of the planning effort to replace them might appear relatively narrow. Yet these machines lay at the heart of the nation`s nuclear weapons complex. The story of these machines is the story of arming the winning weapon, supplying the nuclear arms race. This book is intended to capture the history of the first fourteen production reactors, and associated design work, in the face of the end of the Cold War.« less
13. Elevations, 233S, U.S. Atomic Energy Commission, Hanford Works, General ...
13. Elevations, 233-S, U.S. Atomic Energy Commission, Hanford Works, General Electric Company, Dwg. No. H-2-7203, 1956. - Reduction-Oxidation Complex, Plutonium Concentration Facility, 200 West Area, Richland, Benton County, WA
Instrumentation for studying binder burnout in an immobilized plutonium ceramic wasteform
DOE Office of Scientific and Technical Information (OSTI.GOV)
Mitchell, M; Pugh, D; Herman, C
The Plutonium Immobilization Program produces a ceramic wasteform that utilizes organic binders. Several techniques and instruments were developed to study binder burnout on full size ceramic samples in a production environment. This approach provides a method for developing process parameters on production scale to optimize throughput, product quality, offgas behavior, and plant emissions. These instruments allow for offgas analysis, large-scale TGA, product quality observation, and thermal modeling. Using these tools, results from lab-scale techniques such as laser dilametry studies and traditional TGA/DTA analysis can be integrated. Often, the sintering step of a ceramification process is the limiting process step thatmore » controls the production throughput. Therefore, optimization of sintering behavior is important for overall process success. Furthermore, the capabilities of this instrumentation allows better understanding of plant emissions of key gases: volatile organic compounds (VOCs), volatile inorganics including some halide compounds, NO{sub x}, SO{sub x}, carbon dioxide, and carbon monoxide.« less
Time-dependent local and average structural evolution of δ-phase 239Pu-Ga alloys
Smith, Alice I.; Page, Katharine L.; Siewenie, Joan E.; ...
2016-08-05
Here, plutonium metal is a very unusual element, exhibiting six allotropes at ambient pressure, between room temperature and its melting point, a complicated phase diagram, and a complex electronic structure. Many phases of plutonium metal are unstable with changes in temperature, pressure, chemical additions, or time. This strongly affects structure and properties, and becomes of high importance, particularly when considering effects on structural integrity over long periods of time [1]. This paper presents a time-dependent neutron total scattering study of the local and average structure of naturally aging δ-phase 239Pu-Ga alloys, together with preliminary results on neutron tomography characterization.
NASA Astrophysics Data System (ADS)
Dautray, Robert
2001-12-01
Electronuclear energy associated with hydrogen production can replace fossil fuels while emitting as few greenhouse gases as renewable energies. Besides waste management for which a solution has to be rapidly demonstrated, other key issues are to be examined to complete the demonstration of the viability of electronuclear energy. First, waste management and evolution of plutonium and its daughters must be considered together. A basic study has already been performed but what else to be done is huge and cannot be achieved in France (because of its geological and geographic features, because of the rural distribution of its population, etc.), except if a substantial and quite focused endeavour could bring concerned populations and workers, protection and confidence - which requires from the latter, represented by their elected representatives and thus by a public authority, that they work out "a general protection and confidence criterion for concerned populations and workers". The unique solution in order to protect public health from a potential major danger is to bury as soon as possible all of the ultimate waste products, keeping in mind all of the unfavourable factors such as residual power of these products, their mobility in the confining geological beds and then through aquifers. There are so many categories of waste products whose treatment requires different durations, that storing is necessary in order to make them compatible after sorting by means of chemical separation (called reprocessing). Among all of these potential risks, the present-day most serious one, by far, is that of plutonium and its daughters, which are the most potentially radiotoxic. The unique solution consists in a separation of plutonium (and its daughters), followed by its fissions until a rather complete reduction in a product able to be buried after dilution in a matrix (for example, vitrification). But that solution faces serious handicaps. The examination of waste products and especially of the potentially most dangerous and difficult to treat, that is plutonium (and its daughters), leads thus necessarily to a 'plutonium (and its daughters) plan'. Nuclear safety is a major preoccupation. The French electronuclear stock is a recognized success and when it will be necessary to replace the latter, it will be possible to use the European Pressurized Reactor French-German project; the latter includes protections against very unlikely events and its implementation would be a factor of substantial progress for nuclear safety. Radioprotection, as well as its scientific bases, epidemiology and radiobiology, have funding that is not at the level of the funding devoted to the technical and industrial realizations. As for proliferation, it can be noticed that the countries that have recently at their disposal nuclear weapons have done it independently of their eventual electronuclear stock and furthermore each of the latter used a different scientific and technical process. As for the eventual relations between reprocessing and proliferation, the problem should be solved if the total produced plutonium could be denatured in the reactors of the electronuclear stock. It must be noticed that the major potential danger would rather be the dispersion of radiotoxic products about which the department of ONU in charge of all of these questions is aware of increasing contraband from eastern Europe since some years.
Fire hazard analysis for Plutonium Finishing Plant complex
DOE Office of Scientific and Technical Information (OSTI.GOV)
MCKINNIS, D.L.
1999-02-23
A fire hazards analysis (FHA) was performed for the Plutonium Finishing Plant (PFP) Complex at the Department of Energy (DOE) Hanford site. The scope of the FHA focuses on the nuclear facilities/structures in the Complex. The analysis was conducted in accordance with RLID 5480.7, [DOE Directive RLID 5480.7, 1/17/94] and DOE Order 5480.7A, ''Fire Protection'' [DOE Order 5480.7A, 2/17/93] and addresses each of the sixteen principle elements outlined in paragraph 9.a(3) of the Order. The elements are addressed in terms of the fire protection objectives stated in paragraph 4 of DOE 5480.7A. In addition, the FHA also complies with WHC-CM-4-41,more » Fire Protection Program Manual, Section 3.4 [1994] and WHC-SD-GN-FHA-30001, Rev. 0 [WHC, 1994]. Objectives of the FHA are to determine: (1) the fire hazards that expose the PFP facilities, or that are inherent in the building operations, (2) the adequacy of the fire safety features currently located in the PFP Complex, and (3) the degree of compliance of the facility with specific fire safety provisions in DOE orders, related engineering codes, and standards.« less
Recovery of fissile materials from nuclear wastes
Forsberg, Charles W.
1999-01-01
A process for recovering fissile materials such as uranium, and plutonium, and rare earth elements, from complex waste feed material, and converting the remaining wastes into a waste glass suitable for storage or disposal. The waste feed is mixed with a dissolution glass formed of lead oxide and boron oxide resulting in oxidation, dehalogenation, and dissolution of metal oxides. Carbon is added to remove lead oxide, and a boron oxide fusion melt is produced. The fusion melt is essentially devoid of organic materials and halogens, and is easily and rapidly dissolved in nitric acid. After dissolution, uranium, plutonium and rare earth elements are separated from the acid and recovered by processes such as PUREX or ion exchange. The remaining acid waste stream is vitrified to produce a waste glass suitable for storage or disposal. Potential waste feed materials include plutonium scrap and residue, miscellaneous spent nuclear fuel, and uranium fissile wastes. The initial feed materials may contain mixtures of metals, ceramics, amorphous solids, halides, organic material and other carbon-containing material.
Migliori, Albert; Söderlind, Per; Landa, Alexander; ...
2016-09-19
The electronic and thermodynamic complexity of plutonium has resisted a fundamental understanding for this important elemental metal. critical test of any theory is the unusual softening of the bulk modulus with increasing temperature, a result that is counterintuitive because no or very little change in the atomic volume is observed upon heating. This unexpected behavior has in the past been attributed to competing but never-observed electronic states with different bonding properties similar to the scenario with magnetic states in Invar alloys. When using the recent observation of plutonium dynamic magnetism, we construct a theory for plutonium that agrees with relevantmore » measurements by using density-functional-theory (DFT) calculations with no free parameters to compute the effect of longitudinal spin fluctuations on the temperature dependence of the bulk moduli in δ-Pu. We also show that the softening with temperature can be understood in terms of a continuous distribution of thermally activated spin fluctuations.« less
Method of separating short half-life radionuclides from a mixture of radionuclides
Bray, Lane A.; Ryan, Jack L.
1999-01-01
The present invention is a method of removing an impurity of plutonium, lead or a combination thereof from a mixture of radionuclides that contains the impurity and at least one parent radionuclide. The method has the steps of (a) insuring that the mixture is a hydrochloric acid mixture; (b) oxidizing the acidic mixture and specifically oxidizing the impurity to its highest oxidation state; and (c) passing the oxidized mixture through a chloride form anion exchange column whereupon the oxidized impurity absorbs to the chloride form anion exchange column and the 22.sup.9 Th or 2.sup.27 Ac "cow" radionuclide passes through the chloride form anion exchange column. The plutonium is removed for the purpose of obtaining other alpha emitting radionuclides in a highly purified form suitable for medical therapy. In addition to plutonium; lead, iron, cobalt, copper, uranium, and other metallic cations that form chloride anionic complexes that may be present in the mixture; are removed from the mixture on the chloride form anion exchange column.
Method of separating short half-life radionuclides from a mixture of radionuclides
Bray, L.A.; Ryan, J.L.
1999-03-23
The present invention is a method of removing an impurity of plutonium, lead or a combination thereof from a mixture of radionuclides that contains the impurity and at least one parent radionuclide. The method has the steps of (a) insuring that the mixture is a hydrochloric acid mixture; (b) oxidizing the acidic mixture and specifically oxidizing the impurity to its highest oxidation state; and (c) passing the oxidized mixture through a chloride form anion exchange column whereupon the oxidized impurity absorbs to the chloride form anion exchange column and the {sup 229}Th or {sup 227}Ac ``cow`` radionuclide passes through the chloride form anion exchange column. The plutonium is removed for the purpose of obtaining other alpha emitting radionuclides in a highly purified form suitable for medical therapy. In addition to plutonium, lead, iron, cobalt, copper, uranium, and other metallic cations that form chloride anionic complexes that may be present in the mixture are removed from the mixture on the chloride form anion exchange column. 8 figs.
Tawussi, Frank; Gupta, Dharmendra K; Mühr-Ebert, Elena L; Schneider, Stephanie; Bister, Stefan; Walther, Clemens
2017-11-01
Bioavailability and plant uptake of radionuclides depend on various factors. Transfer into different plant parts depends on chemical and physical processes, which need to be known for realistic ingestion dose modelling when these plants are used for food. Within the scope of the present work, the plutonium uptake by potato plants (Solanum tuberosum L.) was investigated in hydroponic solution of low concentration [Pu] = 10 -9 mol L -1 . Particular attention was paid to the speciation of radionuclides in the solution which was modelled by the speciation code PHREEQC. The speciation, the solubility and therefore the plant availability of radionuclides mainly depend on the pH value and the redox potential of the solution. During the contamination period, the redox potential did not change significantly. In contrast, the pH value showed characteristic changes depending on exudates excreted by the plants. Plant roots took up high amounts of plutonium (37%-50% of the added total amount). In addition to the uptake into the roots, the radionuclides can also adsorb to the exterior root surface. The solution-to-plant transfer factor showed values between 0.03 and 0.80 (Bq kg -1 / Bq L -1 ) for the potato tubers. By addition of the complexing agent EDTA (10 -4 mol L-1), the plutonium uptake from solution increased by 58% in tubers and by 155% in shoots/leaves. The results showed that excreted substances by plants affect bioavailability of radionuclides at low concentration, on the one hand. On the other hand, the uptake of plutonium by roots and the accumulation in different plant parts can lead to non-negligible ingestion doses, even at low concentration. We are aware of the limited transferability of data obtained in hydroponic solutions to plants growing in soil. However, the aim of this study is twofold: First we want to investigate the influence of Pu speciation on plant uptake in a rather well defined system which can be modelled using available thermodynamic data. Second, techniques developed here shall be applied to the investigation of plants growing in soil in the future. The present work contributes to the basic understanding how plant induced effects on nutrient solution influence bioavailability of radionuclides and fosters the need for more detailed investigations of the complex uptake and accumulation processes of radionuclides into plants. Copyright © 2017 Elsevier Ltd. All rights reserved.
PRODUCTION OF PLUTONIUM FROM PLUTONIUM FLUORIDE
Baker, R.D.
1959-06-01
Reduction of PuF/sub 4/ to metal is described. In the example given, PuF/sub 4/ is mixed with 0.3 mole I/sub 2/ per mole of Pu and Ca powder 25% in excess of that required for eduction of the Pu salt, and I/sub 2/ is added. The mixture is charged to a magnesia-lined steel bomb which is heated until reacted in a furnace. The Pu is reduced to metal and recovered as a slug after the bomb is cooled and opened. About 90% yield is obtained. (T.R.H.)
CONVERSION OF PLUTONIUM TRIFLUORIDE TO PLUTONIUM TETRAFLUORIDE
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.
Groundwater monitoring in the Savannah River Plant Low Level Waste Burial Ground
DOE Office of Scientific and Technical Information (OSTI.GOV)
Carlton, W.H.
1983-12-31
This document describes chemical mechanisms that may affect trace-level radionuclide migration through acidic sandy clay soils in a humid environment, and summarizes the extensive chemical and radiochemical analyses of the groundwater directly below the SRP Low-Level Waste (LLW) Burial Ground (643-G). Anomalies were identified in the chemistry of individual wells which appear to be related to small amounts of fission product activity that have reached the water table. The chemical properties which were statistically related to trace level transport of Cs-137 and Sr-90 were iron, potassium, sodium and calcium. Concentrations on the order of 100 ppM appear sufficient to affectmore » nuclide migration. Several complexation mechanisms for plutonium migration were investigated.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Narlesky, Joshua E.; Stroud, Mary Ann; Smith, Paul Herrick
2013-02-15
The Surveillance and Monitoring Program is a joint Los Alamos National Laboratory/Savannah River Site effort funded by the Department of Energy-Environmental Management to provide the technical basis for the safe, long-term storage (up to 50 years) of over 6 metric tons of plutonium stored in over 5,000 DOE-STD-3013 containers at various facilities around the DOE complex. The majority of this material is plutonium that is surplus to the nuclear weapons program, and much of it is destined for conversion to mixed oxide fuel for use in US nuclear power plants. The form of the plutonium ranges from relatively pure metalmore » and oxide to very impure oxide. The performance of the 3013 containers has been shown to depend on moisture content and on the levels, types and chemical forms of the impurities. The oxide materials that present the greatest challenge to the storage container are those that contain chloride salts. Other common impurities include oxides and other compounds of calcium, magnesium, iron, and nickel. Over the past 15 years the program has collected a large body of experimental data on 54 samples of plutonium, with 53 chosen to represent the broader population of materials in storage. This paper summarizes the characterization data, moisture analysis, particle size, surface area, density, wattage, actinide composition, trace element impurity analysis, and shelf life surveillance data and includes origin and process history information. Limited characterization data on fourteen nonrepresentative samples is also presented.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Smith, Paul H; Narlesky, Joshua E; Worl, Laura A
2010-01-01
The Surveillance and Monitoring Program (SMP) is a joint LANL/SRS effort funded by DOE/EM to provide the technical basis for the safe, long-term storage (up to 50 years) of over 6 metric tons of plutonium stored in over 5000 DOE-STD-3013 containers at various facilities around the DOE complex. The majority of this material is plutonium that is surplus to the nuclear weapons program, and much of it is destined for conversion to mixed oxide fuel for use in US nuclear power plants. The form of the plutonium ranges from relatively pure metal and oxide to very impure oxide. The performancemore » of the 3013 containers has been shown to depend on moisture content and on the levels, types and chemical forms of the impurities. The oxide materials that present the greatest challenge to the storage container are those that contain chloride salts. The chlorides (NaCl, KCl, CaCl{sub 2}, and MgCl{sub 2}) range from less than half of the impurities present to nearly all the impurities. Other common impurities include oxides and other compounds of calcium, magnesium, iron, and nickel. Over the past 15 years the program has collected a large body of experimental data on over 60 samples of plutonium chosen to represent the broader population of materials in storage. This paper will summarize the characterization data, including the origin and process history, particle size, surface area, density, calorimetry, chemical analysis, moisture analysis, prompt gamma, gas generation and corrosion behavior.« less
Plutonium weathering on Johnston Atoll
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wolf, S.E.; Bates, J.K.; Buck, E.C.
1995-12-31
Johnston Atoll was contaminated with transuranic elements, particularly plutonium, by atmospheric nuclear weapons tests and aborted nuclear devices. Initial cleanup operations and and an extensive soil remediation program were performed. However, many areas contained a low-level continuum of activity, and subsurface contamination has been detected. Discrete hot particles and contaminated soil were characterized to determine whether the spread of activity was caused by weathering. Analytical techniques included gamma spectrometry, alpha spectrometry, and inductively coupled plasma-mass spectrometry to determine transuranic elemental and isotopic composition. Ultrafiltration and small-particle handling techniques were employed to isolate individual particles. Optical microscopy, scanning electron microscopy, analyticalmore » transmission electron microscopy, energy dispersive X-ray spectroscopy, and electron energy loss spectroscopy were used to characterize individual particles. Analyses of the hot particles showed that they are aborted nuclear warhead fragments that been melted and weathered in the presence of water and CaCO{sub 3}. It was concluded that the formation of aqueous ionic (Pu/Am)-CO{sub 3} coordinated complexes, during environmental exposure to large volumes of rainwater and carbonate-satured seawater, enhanced the solubility of transuranic elements. The (Pu/Am)-CO{sub 3} complexes sorbed onto colloidal CaCO{sub 3} and coral soil surfaces as they were exposed to rain and seawater. This mechanism led to greater dispersal of plutonium and americium than would be expected by physical transport of discrete hot particles alone.« less
Pyrochemical process for extracting plutonium from an electrolyte salt
Mullins, L.J.; Christensen, D.C.
1982-09-20
A pyrochemical process for extracting plutonium from a plutonium-bearing salt is disclosed. The process is particularly useful in the recovery of plutonium for electrolyte salts which are left over from the electrorefining of plutonium. In accordance with the process, the plutonium-bearing salt is melted and mixed with metallic calcium. The calcium reduces ionized plutonium in the salt to plutonium metal, and also causes metallic plutonium in the salt, which is typically present as finely dispersed metallic shot, to coalesce. The reduced and coalesced plutonium separates out on the bottom of the reaction vessel as a separate metallic phase which is readily separable from the overlying salt upon cooling of the mixture. Yields of plutonium are typically on the order of 95%. The stripped salt is virtually free of plutonium and may be discarded to low-level waste storage.
Pyrochemical process for extracting plutonium from an electrolyte salt
Mullins, Lawrence J.; Christensen, Dana C.
1984-01-01
A pyrochemical process for extracting plutonium from a plutonium-bearing salt is disclosed. The process is particularly useful in the recovery of plutonium from electrolyte salts which are left over from the electrorefining of plutonium. In accordance with the process, the plutonium-bearing salt is melted and mixed with metallic calcium. The calcium reduces ionized plutonium in the salt to plutonium metal, and also causes metallic plutonium in the salt, which is typically present as finely dispersed metallic shot, to coalesce. The reduced and coalesced plutonium separates out on the bottom of the reaction vessel as a separate metallic phase which is readily separable from the overlying salt upon cooling of the mixture. Yields of plutonium are typically on the order of 95%. The stripped salt is virtually free of plutonium and may be discarded to low-level waste storage.
Thompson, S.G.; Miller, D.R.; James, R.A.
1961-06-20
A process is described for precipitating Pu from an aqueous solution as the arsenate, either per se or on a bismuth arsenate carrier, whereby a separation from uranium and fission products, if present in solution, is accomplished.
Spent nuclear fuel recycling with plasma reduction and etching
Kim, Yong Ho
2012-06-05
A method of extracting uranium from spent nuclear fuel (SNF) particles is disclosed. Spent nuclear fuel (SNF) (containing oxides of uranium, oxides of fission products (FP) and oxides of transuranic (TRU) elements (including plutonium)) are subjected to a hydrogen plasma and a fluorine plasma. The hydrogen plasma reduces the uranium and plutonium oxides from their oxide state. The fluorine plasma etches the SNF metals to form UF6 and PuF4. During subjection of the SNF particles to the fluorine plasma, the temperature is maintained in the range of 1200-2000 deg K to: a) allow any PuF6 (gas) that is formed to decompose back to PuF4 (solid), and b) to maintain stability of the UF6. Uranium (in the form of gaseous UF6) is easily extracted and separated from the plutonium (in the form of solid PuF4). The use of plasmas instead of high temperature reactors or flames mitigates the high temperature corrosive atmosphere and the production of PuF6 (as a final product). Use of plasmas provide faster reaction rates, greater control over the individual electron and ion temperatures, and allow the use of CF4 or NF3 as the fluorine sources instead of F2 or HF.
PLUTONIUM-CERIUM-COBALT AND PLUTONIUM-CERIUM-NICKEL ALLOYS
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.
NASA Astrophysics Data System (ADS)
Maggs, William Ward
Calling the Department of Energy's management of the nation's crippled nuclear weapons production complex “a 35-year secret chemical war waged against people living near DOE's sites,” Representative Thomas Luken (D-OH) opened a congressional hearing on February 23 with an appeal to DOE Secretary-designate James Watkins to release secret health records of workers at the plants. In testimony that followed, Comptroller General Charles Bowsher told a subcommittee of the House Energy and Commerce Committee that President Bush's new budget does not go far enough on the long and costly road of cleaning up and modernizing the contaminated and aging facilities. The renovation is expected to cost up to $155 billion.By next month, 11 of the 17 installations that make up the DOE complex will be on the EPA's Superfund list of the nation's most contaminated waste sites. Some o f the DOE facilities, including the Rocky Flats plant in Denver, Colo., the Hanford Reservation in eastern Washington, and the Savannah River plant in South Carolina, are among the most polluted sites ever identified by EPA. The principal function of the facilities, the production of tritium and plutonium for nuclear weapons, has stopped, creating what DOE has characterized as a looming national security crisis.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dougherty, D.; Fainberg, A.; Sanborn, J.
On 27 September 1993, President Clinton proposed {open_quotes}... a multilateral convention prohibiting the production of highly enriched uranium or plutonium for nuclear explosives purposes or outside of international safeguards.{close_quotes} The UN General Assembly subsequently adopted a resolution recommending negotiation of a non-discriminatory, multilateral, and internationally and effectively verifiable treaty (hereinafter referred to as {open_quotes}the Cutoff Convention{close_quotes}) banning the production of fissile material for nuclear weapons. The matter is now on the agenda of the Conference on Disarmament, although not yet under negotiation. This accord would, in effect, place all fissile material (defined as highly enriched uranium and plutonium) produced aftermore » entry into force (EIF) of the accord under international safeguards. {open_quotes}Production{close_quotes} would mean separation of the material in question from radioactive fission products, as in spent fuel reprocessing, or enrichment of uranium above the 20% level, which defines highly enriched uranium (HEU). Facilities where such production could occur would be safeguarded to verify that either such production is not occurring or that all material produced at these facilities is maintained under safeguards.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Adamov, E.O.; Lebedev, V.A.; Kuznetsov, Yu.N.
Zheleznogorsk is situated near the territorial center -- Krasnoyarsk on the Yenisei river. Mining and chemical complex is the main industrial enterprise of the town, which has been constructed for generation and used for isolation of weapons-grade plutonium. Heat supply to the chemical complex and town at the moment is largely provided by nuclear co-generation plant (NCGP) on the basis of the ADEh-2 dual-purpose reactor, generating 430 Gcal/h of heat and, partially, by coal backup peak-load boiler houses. NCGP also provides 73% of electric power consumed. In line with agreements between Russia and USA on strategic arms reduction and phasingmore » out of weapons-grade plutonium production, decommissioning of the ADEh-2 reactor by 2000 is planned. Thus, a problem arises relative to compensation for electric and thermal power generation for the needs of the town and industrial enterprises, which is now supplied by the reactor. A nuclear power plant constructed on the same site as a substituting power source should be considered as the most practical option. Basic requirements to the reactor of substituting nuclear power plant are as follows. It is to be a new generation reactor on the basis of verified technologies, having an operating prototype optimal for underground siting and permitting utmost utilization of the available mining workings and those being disengaged. NCGP with the reactor is to be constructed in the time period required and is to become competitive with other possible power sources. Analysis has shown that the VK-300 simplified vessel-type boiling reactor meets the requirements made in the maximum extent. Its design is based on the experience of the VK-50 reactor operation for a period of 30 years in Dimitrovgrad (Russia) and allows for experience in the development of the SBWR type reactors. The design of the reactor is discussed.« less
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)
Creutz, E.C.; Ohlinger, L.A.; Weinberg, A.M.; Wigner, E.P.; Young, G.J.
1959-10-27
BS>A reactor cooled by water, biphenyl, helium, or other fluid with provision made for replacing the fuel rods with the highest plutonium and fission product content without disassembling the entire core and for promptly cooling the rods after their replacement in order to prevent build-up of heat from fission product activity is described.
Direct measurement of 235U in spent fuel rods with Gamma-ray mirrors
NASA Astrophysics Data System (ADS)
Ruz, J.; Brejnholt, N. F.; Alameda, J. B.; Decker, T. A.; Descalle, M. A.; Fernandez-Perea, M.; Hill, R. M.; Kisner, R. A.; Melin, A. M.; Patton, B. W.; Soufli, R.; Ziock, K.; Pivovaroff, M. J.
2015-03-01
Direct measurement of plutonium and uranium X-rays and gamma-rays is a highly desirable non-destructive analysis method for the use in reprocessing fuel environments. The high background and intense radiation from spent fuel make direct measurements difficult to implement since the relatively low activity of uranium and plutonium is masked by the high activity from fission products. To overcome this problem, we make use of a grazing incidence optic to selectively reflect Kα and Kβ fluorescence of Special Nuclear Materials (SNM) into a high-purity position-sensitive germanium detector and obtain their relative ratios.
METHOD OF PREPARING COMPLEXES OF PLUTONIUM WITH DIKETONES
Dixon, J.S.; Katz, J.J.; Orlemann, E.F.
1961-06-20
A process is described for sepsrating Pu from an aqueous alkaline solution by either precipitating with a beta -diketone or extracting into a solution of the beta -dixetone in an organic water-immiscible solvent. Acetyl acetone and benzoyl acetone are the beta -diketones used.
20. VIEW OF WASTE TREATMENT CONTROL ROOM IN BUILDING 374. ...
20. VIEW OF WASTE TREATMENT CONTROL ROOM IN BUILDING 374. THE BUILDING 371/374 COMPLEX WAS DESIGNED TO EMPHASIZE AUTOMATICALLY CONTROLLED, REMOTELY OPERATED PROCESSES. (1/80) - Rocky Flats Plant, Plutonium Recovery Facility, Northwest portion of Rocky Flats Plant, Golden, Jefferson County, CO
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hicks, H.G.
1981-02-12
This report identifies all nuclear events in Nevada that are known to have sent radioactivity beyond the borders of the test range complex. There have been 177 such tests, representing seven different types: nuclear detonations in the atmosphere, nuclear excavation events, nuclear safety events, underground nuclear events that inadvertently seeped or vented to the atmosphere, dispersion of plutonium and/or uranium by chemical high explosives, nuclear rocket engine tests, and nuclear ramjet engine tests. The source term for each of these events is given, together with the data base from which it was derived (except where the data are classified). Themore » computer programs used for organizing and processing the data base and calculating radionuclide production are described and included, together with the input and output data and details of the calculations. This is the basic formation needed to make computer modeling studies of the fallout from any of these 177 events.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Liezers, Martin; Lehn, Scott A; Olsen, Khris B
2009-10-01
Electrochemically modulated separations (EMS) are shown to be a rapid and selective means of extracting and concentrating Pu from complex solutions prior to isotopic analysis by inductively coupled plasma mass spectrometry (ICP-MS). This separation is performed in a flow injection mode, on-line with the ICP-MS. A three-electrode, flow-by electrochemical cell is used to accumulate Pu at an anodized glassy carbon electrode by redox conversion of Pu(III) to Pu (IV&VI). The entire process takes place in 2% v/v (0.46M) HNO 3. No redox chemicals or acid concentration changes are required. Plutonium accumulation and release is redox dependent and controlled by themore » applied cell potential. Thus large transient volumetric concentration enhancements can be achieved. Based on more negative U(IV) potentials relative to Pu(IV), separation of Pu from uranium is efficient, thereby eliminating uranium hydride interferences. EMS-ICP-MS isotope ratio measurement performance will be presented for femtogram to attogram level plutonium concentrations.« less
Siderocalin-mediated recognition, sensitization, and cellular uptake of actinides.
Allred, Benjamin E; Rupert, Peter B; Gauny, Stacey S; An, Dahlia D; Ralston, Corie Y; Sturzbecher-Hoehne, Manuel; Strong, Roland K; Abergel, Rebecca J
2015-08-18
Synthetic radionuclides, such as the transuranic actinides plutonium, americium, and curium, present severe health threats as contaminants, and understanding the scope of the biochemical interactions involved in actinide transport is instrumental in managing human contamination. Here we show that siderocalin, a mammalian siderophore-binding protein from the lipocalin family, specifically binds lanthanide and actinide complexes through molecular recognition of the ligands chelating the metal ions. Using crystallography, we structurally characterized the resulting siderocalin-transuranic actinide complexes, providing unprecedented insights into the biological coordination of heavy radioelements. In controlled in vitro assays, we found that intracellular plutonium uptake can occur through siderocalin-mediated endocytosis. We also demonstrated that siderocalin can act as a synergistic antenna to sensitize the luminescence of trivalent lanthanide and actinide ions in ternary protein-ligand complexes, dramatically increasing the brightness and efficiency of intramolecular energy transfer processes that give rise to metal luminescence. Our results identify siderocalin as a potential player in the biological trafficking of f elements, but through a secondary ligand-based metal sequestration mechanism. Beyond elucidating contamination pathways, this work is a starting point for the design of two-stage biomimetic platforms for photoluminescence, separation, and transport applications.
Siderocalin-mediated recognition, sensitization, and cellular uptake of actinides
Allred, Benjamin E.; Rupert, Peter B.; Gauny, Stacey S.; An, Dahlia D.; Ralston, Corie Y.; Sturzbecher-Hoehne, Manuel; Strong, Roland K.; Abergel, Rebecca J.
2015-01-01
Synthetic radionuclides, such as the transuranic actinides plutonium, americium, and curium, present severe health threats as contaminants, and understanding the scope of the biochemical interactions involved in actinide transport is instrumental in managing human contamination. Here we show that siderocalin, a mammalian siderophore-binding protein from the lipocalin family, specifically binds lanthanide and actinide complexes through molecular recognition of the ligands chelating the metal ions. Using crystallography, we structurally characterized the resulting siderocalin–transuranic actinide complexes, providing unprecedented insights into the biological coordination of heavy radioelements. In controlled in vitro assays, we found that intracellular plutonium uptake can occur through siderocalin-mediated endocytosis. We also demonstrated that siderocalin can act as a synergistic antenna to sensitize the luminescence of trivalent lanthanide and actinide ions in ternary protein–ligand complexes, dramatically increasing the brightness and efficiency of intramolecular energy transfer processes that give rise to metal luminescence. Our results identify siderocalin as a potential player in the biological trafficking of f elements, but through a secondary ligand-based metal sequestration mechanism. Beyond elucidating contamination pathways, this work is a starting point for the design of two-stage biomimetic platforms for photoluminescence, separation, and transport applications. PMID:26240330
PROCESS OF PRODUCING Cm$sup 244$ AND Cm$sup 24$$sup 5$
Manning, W.M.; Studier, M.H.; Diamond, H.; Fields, P.R.
1958-11-01
A process is presented for producing Cm and Cm/sup 245/. The first step of the process consists in subjecting Pu/sup 2339/ to a high neutron flux and subsequently dissolving the irradiated material in HCl. The plutonium is then oxidized to at least the tetravalent state and the solution is contacted with an anion exchange resin, causing the plutonium values to be absorbed while the fission products and transplutonium elements remain in the effluent solution. The effluent solution is then contacted with a cation exchange resin causing the transplutonium, values to be absorbed while the fission products remain in solution. The cation exchange resin is then contacted with an aqueous citrate solution and tbe transplutonium elements are thereby differentially eluted in order of decreasing atomic weight, allowing collection of the desired fractions.
Solvent extraction system for plutonium colloids and other oxide nano-particles
Soderholm, Lynda; Wilson, Richard E; Chiarizia, Renato; Skanthakumar, Suntharalingam
2014-06-03
The invention provides a method for extracting plutonium from spent nuclear fuel, the method comprising supplying plutonium in a first aqueous phase; contacting the plutonium aqueous phase with a mixture of a dielectric and a moiety having a first acidity so as to allow the plutonium to substantially extract into the mixture; and contacting the extracted plutonium with second a aqueous phase, wherein the second aqueous phase has a second acidity higher than the first acidity, so as to allow the extracted plutonium to extract into the second aqueous phase. The invented method facilitates isolation of plutonium polymer without the formation of crud or unwanted emulsions.
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
DOE Office of Scientific and Technical Information (OSTI.GOV)
CHARBONEAU, S.L.
The Plutonium Finishing Plant (PFP) consists of a number of process and support buildings for handling plutonium. Building construction began in the late 1940's to meet national priorities and became operational in 1950 producing refined plutonium salts and metal for the United States nuclear weapons program. The primary mission of the PFP was to provide plutonium used as special nuclear material for fabrication into a nuclear device for the war effort. Subsequent to the end of World War II, the PFP's mission expanded to support the Cold War effort through plutonium production during the nuclear arms race. PFP has nowmore » completed its mission and is fully engaged in deactivation, decontamination and decommissioning (D&D). At this time the PFP buildings are planned to be reduced to ground level (slab-on-grade) and the site remediated to satisfy national, Department of Energy (DOE) and Washington state requirements. The D&D of a highly contaminated plutonium processing facility presents a plethora of challenges. PFP personnel approached the D&D mission with a can-do attitude. They went into D&D knowing they were facing a lot of challenges and unknowns. There were concerns about the configuration control associated with drawings of these old process facilities. There were unknowns regarding the location of electrical lines and process piping containing chemical residues such as strong acids and caustics. The gloveboxes were highly contaminated with plutonium and chemical residues. Most of the glovebox windows were opaque with splashed process chemicals that coated the windows or etched them, reducing visibility to near zero. Visibility into the glovebox was a serious worker concern. Additionally, all the gloves in the gloveboxes were degraded and unusable. Replacing gloves in gloveboxes was necessary to even begin glovebox cleanout. The sheer volume of breathing air needed was also an issue. These and other challenges and PFP's approach to overcome these challengers are described. Many of the challenges to the D&D work at PFP were met with innovative approaches based on new science and/or technology and many were also based on the creativity and motivation of the work force personnel.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Charboneau, S.; Klos, B.; Heineman, R.
The Plutonium Finishing Plant (PFP) consists of a number of process and support buildings for handling plutonium. Building construction began in the late 1940's to meet national priorities and became operational in 1950 producing refined plutonium salts and metal for the United States nuclear weapons program The primary mission of the PFP was to provide plutonium used as special nuclear material for fabrication into a nuclear device for the war effort. Subsequent to the end of World War II, the PFP's mission expanded to support the Cold War effort through plutonium production during the nuclear arms race. PFP has nowmore » completed its mission and is fully engaged in deactivation, decontamination and decommissioning (D and D). At this time the PFP buildings are planned to be reduced to ground level (slab-on-grade) and the site remediated to satisfy national, Department of Energy (DOE) and Washington state requirements. The D and D of a highly contaminated plutonium processing facility presents a plethora of challenges. PFP personnel approached the D and D mission with a can-do attitude. They went into D and D knowing they were facing a lot of challenges and unknowns. There were concerns about the configuration control associated with drawings of these old process facilities. There were unknowns regarding the location of electrical lines and the condition and contents of process piping containing chemical residues such as strong acids and caustics. The gloveboxes were highly contaminated with plutonium and chemical residues. Most of the glovebox windows were opaque with splashed process chemicals that coated the windows or etched them, reducing visibility to near zero. Visibility into the glovebox was a serious worker concern. Additionally, all the gloves in the gloveboxes were degraded and unusable. Replacing gloves in gloveboxes was necessary to even begin glovebox clean-out. The sheer volume of breathing air needed was also an issue. These and other challenges and PFP's approach to overcome these challengers are described. Many of the challenges to the D and D work at PFP were met with innovative approaches based on new science and/or technology and many were also based on the creativity and motivation of the work force personnel. (authors)« less
Ceria-thoria pellet manufacturing in preparation for plutonia-thoria LWR fuel production
NASA Astrophysics Data System (ADS)
Drera, Saleem S.; Björk, Klara Insulander; Sobieska, Matylda
2016-10-01
Thorium dioxide (thoria) has potential to assist in niche roles as fuel for light water reactors (LWRs). One such application for thoria is its use as the fertile component to burn plutonium in a mixed oxide fuel (MOX). Thor Energy and an international consortium are currently irradiating plutonia-thoria (Th-MOX) fuel in an effort to produce data for its licensing basis. During fuel-manufacturing research and development (R&D), surrogate materials were utilized to highlight procedures and build experience. Cerium dioxide (ceria) provides a good surrogate platform to replicate the chemical nature of plutonium dioxide. The project's fuel manufacturing R&D focused on powder metallurgical techniques to ensure manufacturability with the current commercial MOX fuel production infrastructure. The following paper highlights basics of the ceria-thoria fuel production including powder milling, pellet pressing and pellet sintering. Green pellets and sintered pellets were manufactured with average densities of 67.0% and 95.5% that of theoretical density respectively.
Federal Register 2010, 2011, 2012, 2013, 2014
2013-01-09
... for Accomplishing Expanded Civilian Nuclear Energy Research and Development and Isotope Production...-75), Office of Nuclear Energy, U.S. Department of Energy, 1000 Independence Ave. SW., Washington, DC 20585, Phone 301- 903-6062, [email protected]nuclear.energy.gov . For information on NEPA analysis for Pu...
Lung, liver and bone cancer mortality after plutonium exposure in beagle dogs and nuclear workers.
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.
METHOD OF SEPARATING PLUTONIUM
Brown, H.S.; Hill, O.F.
1958-02-01
Plutonium hexafluoride is a satisfactory fluorinating agent and may be reacted with various materials capable of forming fluorides, such as copper, iron, zinc, etc., with consequent formation of the metal fluoride and reduction of the plutonium to the form of a lower fluoride. In accordance with the present invention, it has been found that the reactivity of plutonium hexafluoride with other fluoridizable materials is so great that the process may be used as a method of separating plutonium from mixures containing plutonium hexafluoride and other vaporized fluorides even though the plutonium is present in but minute quantities. This process may be carried out by treating a mixture of fluoride vapors comprising plutonium hexafluoride and fluoride of uranium to selectively reduce the plutonium hexafluoride and convert it to a less volatile fluoride, and then recovering said less volatile fluoride from the vapor by condensation.
Natural chelating agents for radionuclide decorporation
Premuzic, E.T.
1985-06-11
This invention relates to the production of metal-binding compounds useful for the therapy of heavy metal poisoning, for biological mining and for decorporation of radionuclides. The present invention deals with an orderly and effective method of producing new therapeutically effective chelating agents. This method uses challenge biosynthesis for the production of chelating agents that are specific for a particular metal. In this approach, the desired chelating agents are prepared from microorganisms challenged by the metal that the chelating agent is designed to detoxify. This challenge induces the formation of specific or highly selective chelating agents. The present invention involves the use of the challenge biosynthetic method to produce new complexing/chelating agents that are therapeutically useful to detoxify uranium, plutonium, thorium and other toxic metals. The Pseudomonas aeruginosa family of organisms is the referred family of microorganisms to be used in the present invention to produce the new chelating agent because this family is known to elaborate strains resistant to toxic metals.
Renovation of the hot press in the Plutonium Experimental Facility
DOE Office of Scientific and Technical Information (OSTI.GOV)
Congdon, J.W.; Nelson, G.H.
1990-03-05
The Plutonium Experimental Facility (PEF) will be used to develop a new fuel pellet fabrication process and to evaluate equipment upgrades. The facility was used from 1978 until 1982 to optimize the parameters for fuel pellet production using a process which was developed at Los Alamos National Laboratory. The PEF was shutdown and essentially abandoned until mid-1987 when the facility renovations were initiated by the Actinide Technology Section (ATS) of SRL. A major portion of the renovation work was related to the restart of the hot press system. This report describes the renovations and modifications which were required to restartmore » the PEF hot press. The primary purpose of documenting this work is to help provide a basis for Separations to determine the best method of renovating the hot press in the Plutonium Fuel Fabrication (PuFF) facility. This report also includes several SRL recommendations concerning the renovation and modification of the PuFF hot press. 4 refs.« less
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.
STRIPPING PROCESS FOR PLUTONIUM
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.
The production and certification of a plutonium equal-atom reference material: NBL CRM 128
DOE Office of Scientific and Technical Information (OSTI.GOV)
Crawford, D.W.; Gradle, C.G.; Soriano, M.D.
This report describes the design, production, and certification of the New Brunswick Laboratory plutonium equal-atom certified reference material (CRM), NBL CRM 128. The primary use of this CRM is for the determination of bias corrections encountered in the operation of a mass spectrometer. This reference material is available to the US Department of Energy contractor-operated and government-operated laboratories, as well as to the international nuclear safeguards community. The absolute, or unbiased, certified value for the CRM's Pu-242/Pu-239 ratio is 1.00063 {plus minus} 0.00026 (95% confidence interval) as of October 1, 1984. This value was obtained through the quantitative blending ofmore » high-purity, chemically and isotopically characterized separated isotopes, as well as through intercomparisons of CRM samples with calibration mixtures using thermal ionization mass spectrometry. 32 tabs.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Schwantes, Jon M.; Douglas, Matthew; Bonde, Steven E.
2009-02-15
During World War II, the Hanford Site in Washington was chosen for plutonium production. In 2004, a bottle containing a sample of plutonium was recovered from a Hanford waste trench. Isotopic age dating indicated the sample was separated from the fuel pellet 64 ±2.8 years earlier. Detectable products of secondary nuclear reactions, such as 22Na, proved useful as 1) a detectable analog for alpha emitting actinides, 2) an indicator of sample splitting, and 3) a measure of the time since sample splitting. The sample origin was identified as the X-10 reactor, Oak Ridge, TN. Corroborated by historical documents, we concludedmore » this sample was part of the first batch of Pu separated at T-Plant, Hanford, the world’s first industrial-scale reprocessing facility, on December 9, 1944.« less
SEPARATION OF PLUTONIUM FROM LANTHANUM BY CHELATION-EXTRACTION
James, R.A.; Thompson, S.G.
1958-12-01
Plutonium can be separated from a mixture of plutonlum and lanthanum in which the lanthanum to plutonium molal ratio ls at least five by adding the ammonium salt of N-nitrosoarylhydroxylamine to an aqueous solution having a pH between about 3 and 0.2 and containing the plutonium in a valence state of at least +3, to form a plutonium chelate compound of N-nitrosoarylhydroxylamine. The plutonium chelate compound may be recovered from the solution by extracting with an immiscible organic solvent such as chloroform.
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Narlesky, Joshua E; Padilla, Dennis D; Watts, Joe
2009-01-01
Throughout the 1960s and 1970s, the former Soviet Union produced and exported Plutonium-Beryllium (PuBe) neutron sources to various Eastern European countries. The Russian sources consist of an intermetallic compound of plutonium and beryllium encapsulated in an inner welded, sealed capsule and consisting of a body and one or more covers. The amount of plutonium in the sources ranges from 0.002 g up to 15 g. A portion of the sources was originally exported to East Germany. A portion of these sources were acquired by Los Alamos National Laboratory (LANL) in the late 1990s for destruction in the Offsite Source Recoverymore » Program. When the OSRP was canceled, the remaining 88 PuBe neutron sources were packaged and stored in a 55-gal drum at T A-55. This storage configuration is no longer acceptable for PuBe sources, and the sources must either be repackaged or disposed of. Repackaging would place the sources into Hagan container, and depending on the dose rates, some sources may be packaged individually increasing the footprint and cost of storage. In addition, each source will be subject to leak-checking every six months. Leaks have already been detected in some of the sources, and due to the age of these sources, it is likely that additional leaks may be detected over time, which will increase the overall complexity of handling and storage. Therefore, it was decided that the sources would be disposed of at the Waste Isolation Pilot Plant (WIPP) due to the cost and labor associated with continued storage at TA-55. However, the plutonium in the sources is of Russian origin and needs to be preserved for research purposes. Therefore, it is important that a representative sample of the sources retained and archived for future studies. This report describes the criteria used to obtain a representative sample of the sources. Nine Russian PuBe neutron sources have been selected out of a collection of 77 sources for inclusion in the NMIP archive. Selection criteria were developed so that the largest sources that are representative of the collection are included. One representative source was chosen for every 20 sources in the collection, and effort was made to preserve sources unique to the collection. In total, four representative sources and five unique sources were selected for the archive. The archive samples contain 40 grams of plutonium with an isotopic composition similar to that of weapon grade material and three grams of plutonium with an isotopic composition similar to that of reactor grade plutonium.« less
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.
Feasibility study of a magnetic fusion production reactor
NASA Astrophysics Data System (ADS)
Moir, R. W.
1986-12-01
A magnetic fusion reactor can produce 10.8 kg of tritium at a fusion power of only 400 MW —an order of magnitude lower power than that of a fission production reactor. Alternatively, the same fusion reactor can produce 995 kg of plutonium. Either a tokamak or a tandem mirror production plant can be used for this purpose; the cost is estimated at about 1.4 billion (1982 dollars) in either case. (The direct costs are estimated at 1.1 billion.) The production cost is calculated to be 22,000/g for tritium and 260/g for plutonium of quite high purity (1%240Pu). Because of the lack of demonstrated technology, such a plant could not be constructed today without significant risk. However, good progress is being made in fusion technology and, although success in magnetic fusion science and engineering is hard to predict with assurance, it seems possible that the physics basis and much of the needed technology could be demonstrated in facilities now under construction. Most of the remaining technology could be demonstrated in the early 1990s in a fusion test reactor of a few tens of megawatts. If the Magnetic Fusion Energy Program constructs a fusion test reactor of approximately 400 MW of fusion power as a next step in fusion power development, such a facility could be used later as a production reactor in a spinoff application. A construction decision in the late 1980s could result in an operating production reactor in the late 1990s. A magnetic fusion production reactor (MFPR) has four potential advantages over a fission production reactor: (1) no fissile material input is needed; (2) no fissioning exists in the tritium mode and very low fissioning exists in the plutonium mode thus avoiding the meltdown hazard; (3) the cost will probably be lower because of the smaller thermal power required; (4) and no reprocessing plant is needed in the tritium mode. The MFPR also has two disadvantages: (1) it will be more costly to operate because it consumes rather than sells electricity, and (2) there is a risk of not meeting the design goals.
On the multi-reference nature of plutonium oxides: PuO22+, PuO2, PuO3 and PuO2(OH)2.
Boguslawski, Katharina; Réal, Florent; Tecmer, Paweł; Duperrouzel, Corinne; Gomes, André Severo Pereira; Legeza, Örs; Ayers, Paul W; Vallet, Valérie
2017-02-08
Actinide-containing complexes present formidable challenges for electronic structure methods due to the large number of degenerate or quasi-degenerate electronic states arising from partially occupied 5f and 6d shells. Conventional multi-reference methods can treat active spaces that are often at the upper limit of what is required for a proper treatment of species with complex electronic structures, leaving no room for verifying their suitability. In this work we address the issue of properly defining the active spaces in such calculations, and introduce a protocol to determine optimal active spaces based on the use of the Density Matrix Renormalization Group algorithm and concepts of quantum information theory. We apply the protocol to elucidate the electronic structure and bonding mechanism of volatile plutonium oxides (PuO 3 and PuO 2 (OH) 2 ), species associated with nuclear safety issues for which little is known about the electronic structure and energetics. We show how, within a scalar relativistic framework, orbital-pair correlations can be used to guide the definition of optimal active spaces which provide an accurate description of static/non-dynamic electron correlation, as well as to analyse the chemical bonding beyond a simple orbital model. From this bonding analysis we are able to show that the addition of oxo- or hydroxo-groups to the plutonium dioxide species considerably changes the π-bonding mechanism with respect to the bare triatomics, resulting in bent structures with a considerable multi-reference character.
Actinide Waste Forms and Radiation Effects
NASA Astrophysics Data System (ADS)
Ewing, R. C.; Weber, W. J.
Over the past few decades, many studies of actinides in glasses and ceramics have been conducted that have contributed substantially to the increased understanding of actinide incorporation in solids and radiation effects due to actinide decay. These studies have included fundamental research on actinides in solids and applied research and development related to the immobilization of the high level wastes (HLW) from commercial nuclear power plants and processing of nuclear weapons materials, environmental restoration in the nuclear weapons complex, and the immobilization of weapons-grade plutonium as a result of disarmament activities. Thus, the immobilization of actinides has become a pressing issue for the twenty-first century (Ewing, 1999), and plutonium immobilization, in particular, has received considerable attention in the USA (Muller et al., 2002; Muller and Weber, 2001). The investigation of actinides and
Radionuclide Basics: Plutonium
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
Progress Update: Stack Project Complete
Cody, Tom
2017-12-12
Progress update from the Savannah River Site. The 75 foot 293 F Stack, built for plutonium production, was cut down to size in order to prevent injury or release of toxic material if the structure were to collapse due to harsh weather.
The behaviour of tributyl phosphate in an organic diluent
NASA Astrophysics Data System (ADS)
Leay, Laura; Tucker, Kate; Del Regno, Annalaura; Schroeder, Sven L. M.; Sharrad, Clint A.; Masters, Andrew J.
2014-09-01
Tributyl phosphate (TBP) is used as a complexing agent in the Plutonium Uranium Extraction (PUREX) liquid-liquid phase extraction process for recovering uranium and plutonium from spent nuclear reactor fuel. Here, we address the molecular and microstructure of the organic phases involved in the extraction process, using molecular dynamics to show that when TBP is mixed with a paraffinic diluent, the TBP self-assembles into a bi-continuous phase. The underlying self-association of TBP is driven by intermolecular interaction between its polar groups, resulting in butyl moieties radiating out into the organic solvent. Simulation predicts a TBP diffusion constant that is anomalously low compared to what might normally be expected for its size; experimental nuclear magnetic resonance (NMR) studies also indicate an extremely low diffusion constant, consistent with a molecular aggregation model. Simulation of TBP at an oil/water interface shows the formation of a bilayer system at low TBP concentrations. At higher concentrations, a bulk bi-continuous structure is observed linking to this surface bilayer. We suggest that this structure may be intimately connected with the surprisingly rapid kinetics of the interfacial mass transport of uranium and plutonium from the aqueous to the organic phase in the PUREX process.
Cusnir, Ruslan; Steinmann, Philipp; Christl, Marcus; Bochud, François; Froidevaux, Pascal
2015-11-09
The biological uptake of plutonium (Pu) in aquatic ecosystems is of particular concern since it is an alpha-particle emitter with long half-life which can potentially contribute to the exposure of biota and humans. The diffusive gradients in thin films technique is introduced here for in-situ measurements of Pu bioavailability and speciation. A diffusion cell constructed for laboratory experiments with Pu and the newly developed protocol make it possible to simulate the environmental behavior of Pu in model solutions of various chemical compositions. Adjustment of the oxidation states to Pu(IV) and Pu(V) described in this protocol is essential in order to investigate the complex redox chemistry of plutonium in the environment. The calibration of this technique and the results obtained in the laboratory experiments enable to develop a specific DGT device for in-situ Pu measurements in freshwaters. Accelerator-based mass-spectrometry measurements of Pu accumulated by DGTs in a karst spring allowed determining the bioavailability of Pu in a mineral freshwater environment. Application of this protocol for Pu measurements using DGT devices has a large potential to improve our understanding of the speciation and the biological transfer of Pu in aquatic ecosystems.
An Update on the Status of the Supply of Plutonium-238 for Future NASA Missions
NASA Astrophysics Data System (ADS)
Wham, R. M.
2016-12-01
For more than five decades, Radioisotope Power Systems (RPSs) have enabled space missions to operate in locations where the Sun's intensity is too weak, obscured, or otherwise inadequate for solar power or other conventional power‒generation technologies. The natural decay heat (0.57 W/g) from the radioisotope, plutonium-238 (238Pu), provides the thermal energy source used by an RPS to generate electricity for operation of instrumentation, as well as heat to keep key subsystems warm for missions such as Voyagers 1 and 2, the Cassini mission to Saturn, the New Horizons flyby of Pluto, and the Mars Curiosity rover which were sponsored by the National Aeronautics and Space Administration (NASA). Plutonium-238 is produced by irradiation of neptunium-237 in a nuclear reactor a relatively high neutron flux. The United States has not produced new quantities of 238Pu since the early 1990s. RPS‒powered missions have continued since then using existing 238Pu inventory managed by the U.S. Department of Energy (DOE), including material purchased from Russia. A new domestic supply is needed to ensure the continued availability of RPSs for future NASA missions. NASA and DOE are currently executing a project to reestablish a 238Pu supply capability using its existing facilities and reactors, which are much smaller than the large-scale production reactors and processing canyon equipment used previously. The project is led by the Oak Ridge National Laboratory (ORNL). Target rods, containing NpO2, will be fabricated at ORNL and irradiated in the ORNL High Flux Isotope Reactor and the Advanced Test Reactor at Idaho National Laboratory. Irradiated targets will be processed in chemical separations at the ORNL Radiochemical Engineering Center to recover the plutonium product and unconverted neptunium for recycle. The 238PuO2 product will be shipped to Los Alamos National Laboratory for fabrication of heat source pellets. Key activities, such as transport of the neptunium to ORNL, irradiation of neptunium, and chemical processing to recover the newly generated 238Pu, have begun and have been demonstrated with the initial amounts (50-100 g) produced. Product samples have been shipped to LANL for evaluation, including chemical impurity analysis. This paper will provide an overview of the approach to the project and its progress to date.
On the use of thermal NF3 as the fluorination and oxidation agent in treatment of used nuclear fuels
NASA Astrophysics Data System (ADS)
Scheele, Randall; McNamara, Bruce; Casella, Andrew M.; Kozelisky, Anne
2012-05-01
This paper presents results of our investigation on the use of nitrogen trifluoride as a fluorination or fluorination/oxidation agent for separating valuable constituents from used nuclear fuels by exploiting the different volatilities of the constituent fission product and actinide fluorides. Our thermodynamic calculations show that nitrogen trifluoride has the potential to produce volatile fission product and actinide fluorides from oxides and metals that can form volatile fluorides. Simultaneous thermogravimetric and differential thermal analyses show that the oxides of lanthanum, cerium, rhodium, and plutonium are fluorinated but do not form volatile fluorides when treated with nitrogen trifluoride at temperatures up to 550 °C. However, depending on temperature, volatile fluorides or oxyfluorides can form from nitrogen trifluoride treatment of the oxides of niobium, molybdenum, ruthenium, tellurium, uranium, and neptunium. Thermoanalytical studies demonstrate near-quantitative separation of uranium from plutonium in a mixed 80% uranium and 20% plutonium oxide. Our studies of neat oxides and metals suggest that the reactivity of nitrogen trifluoride may be adjusted by temperature to selectively separate the major volatile fuel constituent uranium from minor volatile constituents, such as Mo, Tc, Ru and from the non-volatile fuel constituents based on differences in their reaction temperatures and kinetic behaviors. This reactivity is novel with respect to that reported for other fluorinating reagents F2, BrF5, ClF3.
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)
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.
Accelerator-driven Transmutation of Waste
NASA Astrophysics Data System (ADS)
Venneri, Francesco
1998-04-01
Nuclear waste from commercial power plants contains large quantities of plutonium, other fissionable actinides, and long-lived fission products that are potential proliferation concerns and create challenges for the long-term storage. Different strategies for dealing with nuclear waste are being followed by various countries because of their geologic situations and their views on nuclear energy, reprocessing and non-proliferation. The current United States policy is to store unprocessed spent reactor fuel in a geologic repository. Other countries are opting for treatment of nuclear waste, including partial utilization of the fissile material contained in the spent fuel, prior to geologic storage. Long-term uncertainties are hampering the acceptability and eventual licensing of a geologic repository for nuclear spent fuel in the US, and driving up its cost. The greatest concerns are with the potential for radiation release and exposure from the spent fuel for tens of thousands of years and the possible diversion and use of the actinides contained in the waste for weapons construction. Taking advantage of the recent breakthroughs in accelerator technology and of the natural flexibility of subcritical systems, the Accelerator-driven Transmutation of Waste (ATW) concept offers the United States and other countries the possibility to greatly reduce plutonium, higher actinides and environmentally hazardous fission products from the waste stream destined for permanent storage. ATW does not eliminate the need for, but instead enhances the viability of permanent waste repositories. Far from being limited to waste destruction, the ATW concept also brings to the table new technologies that could be relevant for next-generation power producing reactors. In the ATW concept, spent fuel would be shipped to the ATW site where the plutonium, transuranics and selected long-lived fission products would be destroyed by fission or transmutation in their first and only pass through the facility, using an accelerator-driven subcritical burner cooled by liquid lead/bismuth and limited pyrochemical treatment of the spent fuel and residual waste. This approach contrasts with the present-day practices of aqueous reprocessing (Europe and Japan), in which high purity plutonium is produced and used in the fabrication of fresh mixed oxide fuel (MOX) that is shipped off-site for use in light water reactors.
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
DOE Office of Scientific and Technical Information (OSTI.GOV)
Johnson, Bradley R.
The Hidden Cost of Nuclear Weapons The Cold War arms race drove an intense plutonium production program in the U.S. This campaign produced approximately 100 tons of plutonium over 40 years. The epicenter of plutonium production in the United States was the Hanford site, a 586 square mile reservation owned by the Department of Energy and located on the Colombia River in Southeastern Washington. Plutonium synthesis relied on nuclear reactors to convert uranium to plutonium within the reactor fuel rods. After a sufficient amount of conversion occurred, the rods were removed from the reactor and allowed to cool. They weremore » then dissolved in an acid bath and chemically processed to separate and purify plutonium from the rest of the constituents in the used reactor fuel. The acidic waste was then neutralized using sodium hydroxide and the resulting mixture of liquids and precipitates (small insoluble particles) was stored in huge underground waste tanks. The byproducts of the U.S. plutonium production campaign include over 53 million gallons of high-level radioactive waste stored in 177 large underground tanks at Hanford and another 34 million gallons stored at the Savannah River Site in South Carolina. This legacy nuclear waste represents one of the largest environmental clean-up challenges facing the world today. The nuclear waste in the Hanford tanks is a mixture of liquids and precipitates that have settled into sludge. Some of these tanks are now over 60 years old and a small number of them are leaking radioactive waste into the ground and contaminating the environment. The solution to this nuclear waste challenge is to convert the mixture of solids and liquids into a durable material that won't disperse into the environment and create hazards to the biosphere. What makes this difficult is the fact that the radioactive half-lives of some of the radionuclides in the waste are thousands to millions of years long. (The half-life of a radioactive substance is the amount of time it takes for one-half of the material to undergo radioactive decay.) In general, the ideal material would need to be durable for approximately 10 half-lives to allow the activity to decay to negligible levels. However, the potential health effects of each radionuclide vary depending on what type of radiation is emitted, the energy of that emission, and the susceptibility for the human body to accumulate and concentrate that particular element. Consequently, actual standards tend to be based on limiting the dose (energy deposited per unit mass) that is introduced into the environment. The Environmental Protection Agency (EPA) has the responsibility to establish standards for nuclear waste disposal to protect the health and safety of the public. For example, the Energy Policy Act of 1992 directed the EPA to establish radiation protection standards for the Yucca Mountain geologic repository for nuclear wastes. The standards for Yucca Mountain were promulgated in 2008, and limit the dose to 15 millirem per year for the first 10,000 years, and 100 milirem per year between 10,000 years and 1 million years (40 CFR Part 197; http://www.epa.gov/radiation/yucca/2008factsheet.html). So, the challenge is two-fold: (1) develop a material (a waste form) that is capable of immobilizing the waste over geologic time scales, and (2) develop a process to convert the radioactive sludge in the tanks into this durable waste form material. Glass: Hard, durable, inert, and with infinite chemical versatility Molten glass is a powerful solvent liquid, which can be designed to dissolve almost anything. When solidified, it can be one of the most chemically inert substances known to man. Nature's most famous analogue to glass is obsidian, a vitreous product of volcanic activity; formations over 17 million years old have been found. Archaeologists have found man-made glass specimens that are five thousand years old.« less
PROCESS FOR SEPARATING PLUTONIUM FROM IMPURITIES
Wahl, A.C.
1957-11-12
A method is described for separating plutonium from aqueous solutions containing uranium. It has been found that if the plutonium is reduced to its 3+ valence state, and the uranium present is left in its higher valence state, then the differences in solubility between certain salts (e.g., oxalates) of the trivalent plutonium and the hexavalent uranium can be used to separate the metals. This selective reduction of plutonium is accomplished by adding iodide ion to the solution, since iodide possesses an oxidation potential sufficient to reduce plutonium but not sufficient to reduce uranium.
PLUTONIUM COMPOUNDS AND PROCESS FOR THEIR PREPARATION
Wolter, F.J.; Diehl, H.C. Jr.
1958-01-01
This patent relates to certain new compounds of plutonium, and to the utilization of these compounds to effect purification or separation of the plutonium. The compounds are organic chelate compounds consisting of tetravalent plutonium together with a di(salicylal) alkylenediimine. These chelates are soluble in various organic solvents, but not in water. Use is made of this property in extracting the plutonium by contacting an aqueous solution thereof with an organic solution of the diimine. The plutonium is chelated, extracted and effectively separated from any impurities accompaying it in the aqueous phase.
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
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
DOE Office of Scientific and Technical Information (OSTI.GOV)
Jaffke, Patrick John
This acts as a short note on the effects of varying the value of the endpoints of the thermal, epithermal, and fast flux groups. As expected, varying these endpoints can alter the value of the cross-section for a given nuclide. This effect is quantified in this note for an important nuclide in reactor simulations, 238U. Uranium-238 is responsible for the production of Plutonium in most reactors, making it critical to understand all of the 238U capture modes leading to Plutonium. We explicitly quantify the reaction rates for 238U that are altered when we use a given research reactor fluxmore » and vary the endpoint definitions of said flux as well as the reactor position.« less
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.
Reactors as a Source of Antineutrinos: Effects of Fuel Loading and Burnup for Mixed-Oxide Fuels
NASA Astrophysics Data System (ADS)
Bernstein, Adam; Bowden, Nathaniel S.; Erickson, Anna S.
2018-01-01
In a conventional light-water reactor loaded with a range of uranium and plutonium-based fuel mixtures, the variation in antineutrino production over the cycle reflects both the initial core fissile inventory and its evolution. Under an assumption of constant thermal power, we calculate the rate at which antineutrinos are emitted from variously fueled cores, and the evolution of that rate as measured by a representative ton-scale antineutrino detector. We find that antineutrino flux decreases with burnup for low-enriched uranium cores, increases for full mixed-oxide (MOX) cores, and does not appreciably change for cores with a MOX fraction of approximately 75%. Accounting for uncertainties in the fission yields in the emitted antineutrino spectra and the detector response function, we show that the difference in corewide MOX fractions at least as small as 8% can be distinguished using a hypothesis test. The test compares the evolution of the antineutrino rate relative to an initial value over part or all of the cycle. The use of relative rates reduces the sensitivity of the test to an independent thermal power measurement, making the result more robust against possible countermeasures. This rate-only approach also offers the potential advantage of reducing the cost and complexity of the antineutrino detectors used to verify the diversion, compared to methods that depend on the use of the antineutrino spectrum. A possible application is the verification of the disposition of surplus plutonium in nuclear reactors.
Nuclear Fuel Reprocessing: U.S. Policy Development
2006-11-29
to the chemical separation of fissionable uranium and plutonium from irradiated nuclear fuel. The World War II-era Manhattan Project developed...created the Atomic Energy Commission (AEC) and transferred production and control of fissionable materials from the Manhattan Project . As the exclusive
METHOD FOR RECOVERING PLUTONIUM VALUES FROM SOLUTION USING A BISMUTH HYDROXIDE CARRIER PRECIPITATE
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.
Radionuclides in ground water at the Idaho National Engineering Laboratory, Idaho
Knobel, LeRoy L.; Mann, Larry J.
1988-01-01
Sampling for radionuclides in groundwater was conducted at the Idaho National Engineering Laboratory during September to November 5 1987. Water samples from 80 wells that obtain water from the Snake River Plain aquifer and 1 well that obtains water from a shallow, discontinuous perched-water body at the Radioactive Waste Management Complex were collected and analyzed for tritium, strontium-90, plutonium-238, plutonium-239, -240 (undivided), americium-241, cesium-137, cobalt-60, and potassium-40--a naturally occurring radionuclide. The groundwater samples were analyzed at the Idaho National Engineering Laboratory in Idaho. Tritium and strontium-90 concentrations ranged from below the reporting level to 80.6 +/-0.000005 and 193 +/-5x10 to the minus eight micrograms Ci/ml, respectively. Water from a disposal well at Test Area North--which has not been used to dispose of waste water since September 1972--contained 122 +/-9x10 to the minus eleven micrograms Ci/ml of plutonium-238, 500 +/-20x10 to the minus eleven of plutonium-239, -240 (undivided), 21 +/-4x10 to the minus eleven micrograms Ci/ml of americium-241, and 750 +/-20x10 to the minus eight micrograms Ci/ml cesium-137; the presence of these radionuclides was verified by resampling and reanalysis. The disposal well had 8.9 +/-0.0000009 micrograms Ci/ml of cobalt-60 on October 28, 1987, but cobalt-60 was not detected when the well was resampled on January 11, 1988. Potassium-40 concentrations were less than the reporting level in all wells. (USGS)
DOE Office of Scientific and Technical Information (OSTI.GOV)
Essington, E.H.; Gilbert, R.O.; Wireman, D.L.
Blow-sand mounds or miniature sand dunes and mounds created by burrowing activities of animals were investigated by the Nevada Applied Ecology Group (NAEG) to determine the influence of mounds on plutonium, americium, and uranium distributions and inventories in areas of the Nevada Test Site and Tonopah Test Range. Those radioactive elements were added to the environment as a result of safety experiments of nuclear devices. Two studies were conducted. The first was to estimate the vertical distribution of americium in the blow-sand mounds and in the desert pavement surrounding the mounds. The second was to estimate the amount or concentrationmore » of the radioactive materials accumulated in the mound relative to the desert pavement. Five mound types were identified in which plutonium, americium, and uranium concentrations were measured: grass, shrub, complex, animal, and diffuse. The mount top (that portion above the surrounding land surface datum), the mound bottom (that portion below the mound to a depth of 5 cm below the surrounding land surface datum), and soil from the immediate area surrounding the mound were compared separately to determine if the radioactive elements had concentrated in the mounds. Results of the studies indicate that the mounds exhibit higher concentrations of plutonium, americium, and uranium than the immediate surrounding soil. The type of mound does not appear to have influenced the amount of the radioactive material found in the mound except for the animal mounds where the burrowing activities appear to have obliterated distribution patterns.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Pierce, R.; Peters, T.
2011-11-01
Between September 2009 and January 2011, the Savannah River National Laboratory (SRNL) and the Savannah River Site (SRS) HB-Line Facility designed, developed, tested, and successfully deployed a production-scale system for the distillation of sodium chloride (NaCl) and potassium chloride (KCl) from plutonium oxide (PuO{sub 2}). Subsequent efforts adapted the vacuum salt distillation (VSD) technology for the removal of chloride and fluoride from less-volatile halide salts at the same process temperature and vacuum. Calcium chloride (CaCl{sub 2}), calcium fluoride (CaF{sub 2}), and plutonium fluoride (PuF{sub 3}) were of particular concern. To enable the use of the same operating conditions for themore » distillation process, SRNL employed in situ exchange reactions to convert the less-volatile halide salts to compounds that facilitated the distillation of halide without removal of plutonium. SRNL demonstrated the removal of halide from CaCl{sub 2}, CaF{sub 2} and PuF{sub 3} below 1000 C using VSD technology.« 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
DOE Office of Scientific and Technical Information (OSTI.GOV)
Popa, Karin; Raison, Philippe E., E-mail: philippe.raison@ec.europa.eu; Martel, Laura
2015-10-15
PuPO{sub 4} was prepared by a solid state reaction method and its crystal structure at room temperature was solved by powder X-ray diffraction combined with Rietveld refinement. High resolution XANES measurements confirm the +III valence state of plutonium, in agreement with valence bond derivation. The presence of the americium (as β{sup −} decay product of plutonium) in the +III oxidation state was determined based on XANES spectroscopy. High resolution solid state {sup 31}P NMR agrees with the XANES results and the presence of a solid-solution. - Graphical abstract: A full structural analysis of PuPO{sub 4} based on Rietveld analysis ofmore » room temperature X-ray diffraction data, XANES and MAS NMR measurements was performed. - Highlights: • The crystal structure of PuPO{sub 4} monazite is solved. • In PuPO{sub 4} plutonium is strictly trivalent. • The presence of a minute amount of Am{sup III} is highlighted. • We propose PuPO{sub 4} as a potential reference material for spectroscopic and microscopic studies.« less
Kolodney, M.
1959-12-01
A method is described for rapidly removing iron, nickel, and zinc coatings from plutonium objects while simultaneously rendering the plutonium object passive. The method consists of immersing the coated plutonium object in an aqueous acid solution containing a substantial concentration of nitrate ions, such as fuming nitric acid.
METHOD OF MAKING PLUTONIUM DIOXIDE
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
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.
Short History of Oak Ridge National Laboratory (1943 - 1993) Los Alamos, New Mexico * Selected as Atomic Weapons Laboratory * Site Selection * History @ Los Alamos Hanford, Washington * Selected as Plutonium Production Facility * History of the Hanford Site 1943 - 1990 Chicago, Illinois * Promethean Boldness at
10 CFR 110.41 - Executive Branch review.
Code of Federal Regulations, 2011 CFR
2011-01-01
.... (6) An export involving assistance to end uses related to isotope separation, chemical reprocessing, heavy water production, advanced reactors, or the fabrication of nuclear fuel containing plutonium... equipment to a foreign reactor. (8) An export involving radioactive waste. (9) An export to any country...
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.
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.
Overview of reductants utilized in nuclear fuel reprocessing/recycling
DOE Office of Scientific and Technical Information (OSTI.GOV)
Patricia Paviet-Hartmann; Catherine Riddle; Keri Campbell
2013-10-01
Most of the aqueous processes developed, or under consideration worldwide for the recycling of used nuclear fuel (UNF) utilize the oxido-reduction properties of actinides to separate them from other radionuclides. Generally, after acid dissolution of the UNF, (essentially in nitric acid solution), actinides are separated from the raffinate by liquid-liquid extraction using specific solvents, associated along the process, with a particular reductant that will allow the separation to occur. For example, the industrial PUREX process utilizes hydroxylamine as a plutonium reductant. Hydroxylamine has numerous advantages: not only does it have the proper attributes to reduce Pu(IV) to Pu(III), but itmore » is also a non-metallic chemical that is readily decomposed to innocuous products by heating. However, it has been observed that the presence of high nitric acid concentrations or impurities (such as metal ions) in hydroxylamine solutions increase the likelihood of the initiation of an autocatalytic reaction. Recently there has been some interest in the application of simple hydrophilic hydroxamic ligands such as acetohydroxamic acid (AHA) for the stripping of tetravalent actinides in the UREX process flowsheet. This approach is based on the high coordinating ability of hydroxamic acids with tetravalent actinides (Np and Pu) compared with hexavalent uranium. Thus, the use of AHA offers a route for controlling neptunium and plutonium in the UREX process by complexant based stripping of Np(IV) and Pu(IV) from the TBP solvent phase, while U(VI) ions are not affected by AHA and remain solvated in the TBP phase. In the European GANEX process, AHA is also used to form hydrophilic complexes with actinides and strip them from the organic phase into nitric acid. However, AHA does not decompose completely when treated with nitric acid and hampers nitric acid recycling. In lieu of using AHA in the UREX + process, formohydroxamic acid (FHA), although not commercially available, hold promises as a replacement for AHA. FHA undergoes hydrolysis to formic acid which is volatile, thus allowing the recycling of nitric acid. Unfortunately, FHA powder was not stable in the experiments we ran in our laboratory. In addition, AHA and FHA also decompose to hydroxylamine which may undergo an autocatalytic reaction. Other reductants are available and could be extremely useful for actinides separation. The review presents the current plutonium reductants used in used nuclear fuel reprocessing and will introduce innovative and novel reductants that could become reducers for future research on UNF separation.« less
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
Brown, H.S.; Hill, O.F.
1958-09-01
A process is presented for recovering plutonium values from aqueous solutions. It comprises forming a uranous hydroxide precipitate in such a plutonium bearing solution, at a pH of at least 5. The plutonium values are precipitated with and carried by the uranium hydroxide. The carrier precipitate is then redissolved in acid solution and the pH is adjusted to about 2.5, causing precipitation of the uranous hydroxide but leaving the still soluble plutonium values in solution.
COLUMBIC OXIDE ADSORPTION PROCESS FOR SEPARATING URANIUM AND PLUTONIUM IONS
Beaton, R.H.
1959-07-14
A process is described for separating plutonium ions from a solution of neutron irradiated uranium in which columbic oxide is used as an adsorbert. According to the invention the plutonium ion is selectively adsorbed by Passing a solution containing the plutonium in a valence state not higher than 4 through a porous bed or column of granules of hydrated columbic oxide. The adsorbed plutonium is then desorbed by elution with 3 N nitric acid.
DISSOLUTION OF LANTHANUM FLUORIDE PRECIPITATES
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.
Interaction of aerobic soil bacteria with plutonium(VI)
DOE Office of Scientific and Technical Information (OSTI.GOV)
Panak, Petra J.; Nitsche, Heino
2000-08-22
We studied the interaction of Pu(VI) with Pseudomonas stutzeri ATCC 17588 and Bacillus sphaericus ATCC 14577, representatives of the main aerobic groups of soil bacteria present in the upper soil layers. The accumulation studies have shown that these soil bacteria accumulate high amounts of Pu(VI). The sorption efficiency toward Pu(VI) decreased with increasing biomass concentration due to increased agglomeration of the bacteria resulting in a decreased total surface area and number of available complexing groups. Spores of Bacillus sphaericus showed a higher biosorption than the vegetative cells at low biomass concentration which decreased significantly with increasing biomass concentration. At highermore » biomass concentrations (> 0.7 g/L), the vegetative cells of both strains and the spores of B. sphaericus showed comparable sorption efficiencies. Investigations on the pH dependency of the biosorption and extraction studies with 0.01 M EDTA solution have shown that the biosorption of plutonium is a reversible process and the plutonium is bound by surface complexation. Optical absorption spectroscopy showed that one third of the initially present Pu(VI) was reduced to Pu(V) after 24 hours. Kinetic studies and solvent extraction to separate different oxidation states of Pu after contact with the biomass provided further information on the yield and the kinetics of the bacteria-mediated reduction. Long-term studies showed that also 16% of Pu(IV) was formed after one month. The comparison of the amount of Pu(IV) formed during that time period with literature data of the Pu(V) disproportionation, indicated that the Pu(IV) seemed to be rather the result of the disproportionation of the formed Pu(V) than of a further microbial reduction.« less
Code of Federal Regulations, 2010 CFR
2010-01-01
... 10 Energy 2 2010-01-01 2010-01-01 false Reports of loss or theft or attempted theft or... Requirements § 74.11 Reports of loss or theft or attempted theft or unauthorized production of special nuclear... plutonium shall notify the NRC Operations Center within 1 hour of discovery of any loss or theft or other...
FISSION PRODUCT REMOVAL FROM ORGANIC SOLUTIONS
Moore, R.H.
1960-05-10
The decontamination of organic solvents from fission products and in particular the treatment of solvents that were used for the extraction of uranium and/or plutonium from aqueous acid solutions of neutron-irradiated uranium are treated. The process broadly comprises heating manganese carbonate in air to a temperature of between 300 and 500 deg C whereby manganese dioxide is formed; mixing the manganese dioxide with the fission product-containing organic solvent to be treated whereby the fission products are precipitated on the manganese dioxide; and separating the fission product-containing manganese dioxide from the solvent.
NON-AQUEOUS DISSOLUTION OF MASSIVE PLUTONIUM
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
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
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.
Production and recovery of Americium-241
DOE Office of Scientific and Technical Information (OSTI.GOV)
Navratil, J.D.
1984-01-01
Americium-241, one of the most useful actinide isotopes, is produced as a by-product of plutonium scrap recovery operations. Rocky Flats (RF) has supplied high-purity americium oxide to the US Department of Energy's Isotope Pool since 1962. Over the years, the evolving separation and purification processes have included such diverse operations as aqueous precipitation, ion exchange, and both molten-salt and organic-solvent extraction. A review is presented of the production and recovery processes of americium-241. 5 references.
Interim Safe Storage of Plutonium Production Reactors at the US DOE Hanford Site - 13438
DOE Office of Scientific and Technical Information (OSTI.GOV)
Schilperoort, Daryl L.; Faulk, Darrin
2013-07-01
Nine plutonium production reactors located on DOE's Hanford Site are being placed into an Interim Safe Storage (ISS) period that extends to 2068. The Environmental Impact Statement (EIS) for ISS [1] was completed in 1993 and proposed a 75-year storage period that began when the EIS was finalized. Remote electronic monitoring of the temperature and water level alarms inside the safe storage enclosure (SSE) with visual inspection inside the SSE every 5 years are the only planned operational activities during this ISS period. At the end of the ISS period, the reactor cores will be removed intact and buried inmore » a landfill on the Hanford Site. The ISS period allows for radioactive decay of isotopes, primarily Co-60 and Cs-137, to reduce the dose exposure during disposal of the reactor cores. Six of the nine reactors have been placed into ISS by having an SSE constructed around the reactor core. (authors)« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Jostsons, A.; Ridal, A.; Mercer, D.J.
1996-05-01
The Synroc Demonstration Plant (SDP) was designed and constructed at Lucas Heights to demonstrate the feasibility of Synroc production on a commercial scale (10 kg/hr) with simulated Purex liquid HLW. Since commissioning of the SDP in 1987, over 6000 kg of Synroc has been fabricated with a range of feeds and waste loadings. The SDP utilises uniaxial hot-pressing to consolidate Synroc. Pressureless sintering and hot-isostatic pressing have also been studied at smaller scales. The results of this extensive process development have been incorporated in a conceptual design for a radioactive plant to condition HLW from a reprocessing plant with amore » capacity to treat 800 tpa of spent LWR fuel. Synroic containing TRU, including Pu, and fission products has been fabricated and characterised in a glove-box facility and hot cells, respectively. The extensive experience in processing of Synroc over the past 15 years is summarised and its relevance to immobilization of surplus plutonium is discussed.« less
NASA Astrophysics Data System (ADS)
Remerowski, Mary Lynn; Dozhier, C.; Krenek, K.; VanPelt, C. E.; Reimus, M. A.; Spengler, D.; Matonic, J.; Garcia, L.; Rios, E.; Sandoval, F.; Herman, D.; Hart, R.; Ewing, B.; Lovato, M.; Romero, J. P.
2005-02-01
Pu-238 heat sources are used to fuel radioisotope thermoelectric generators (RTG) used in space missions. The demand for this fuel is increasing, yet there are currently no domestic sources of this material. Much of the fuel is material reprocessed from other sources. One rich source of Pu-238 residual material is that from contaminated combustible materials, such as cheesecloth, ion exchange resins and plastics. From both waste minimization and production efficiency standpoints, the best solution is to recover this material. One way to accomplish separation of the organic component from these residues is a flameless oxidation process using molten salt as the matrix for the breakdown of the organic to carbon dioxide and water. The plutonium is retained in the salt, and can be recovered by dissolution of the carbonate salt in an aqueous solution, leaving the insoluble oxide behind. Further aqueous scrap recovery processing is used to purify the plutonium oxide. Recovery of the plutonium from contaminated combustibles achieves two important goals. First, it increases the inventory of Pu-238 available for heat source fabrication. Second, it is a significant waste minimization process. Because of its thermal activity (0.567 W per gram), combustibles must be packaged for disposition with much lower amounts of Pu-238 per drum than other waste types. Specifically, cheesecloth residues in the form of pyrolyzed ash (for stabilization) are being stored for eventual recovery of the plutonium.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Remerowski, Mary Lynn; Dozhier, C.; Krenek, K.
2005-02-06
Pu-238 heat sources are used to fuel radioisotope thermoelectric generators (RTG) used in space missions. The demand for this fuel is increasing, yet there are currently no domestic sources of this material. Much of the fuel is material reprocessed from other sources. One rich source of Pu-238 residual material is that from contaminated combustible materials, such as cheesecloth, ion exchange resins and plastics. From both waste minimization and production efficiency standpoints, the best solution is to recover this material. One way to accomplish separation of the organic component from these residues is a flameless oxidation process using molten salt asmore » the matrix for the breakdown of the organic to carbon dioxide and water. The plutonium is retained in the salt, and can be recovered by dissolution of the carbonate salt in an aqueous solution, leaving the insoluble oxide behind. Further aqueous scrap recovery processing is used to purify the plutonium oxide. Recovery of the plutonium from contaminated combustibles achieves two important goals. First, it increases the inventory of Pu-238 available for heat source fabrication. Second, it is a significant waste minimization process. Because of its thermal activity (0.567 W per gram), combustibles must be packaged for disposition with much lower amounts of Pu-238 per drum than other waste types. Specifically, cheesecloth residues in the form of pyrolyzed ash (for stabilization) are being stored for eventual recovery of the plutonium.« less
NASA Astrophysics Data System (ADS)
Jégou, C.; Caraballo, R.; Peuget, S.; Roudil, D.; Desgranges, L.; Magnin, M.
2010-10-01
Structural changes in four (U 1-yPu y)O 2 materials with very different plutonium concentrations (0 ⩽ y ⩽ 1) and damage levels (up to 110 dpa) were studied by Raman spectroscopy. The novel experimental approach developed for this purpose consisted in using a laser beam as a heat source to assess the reactivity and structural changes of these materials according to the power supplied locally by the laser. The experiments were carried out in air and in water with or without hydrogen peroxide. As expected, the material response to oxidation in air depends on the plutonium content of the test oxide. At the highest power levels U 3O 8 generally forms with UO 2 whereas no significant change in the spectra indicating oxidation is observed for samples with high plutonium content ( 239PuO 2). Samples containing 25 wt.% plutonium exhibit intermediate behavior, typified mainly by a higher-intensity 632 cm -1 peak and the disappearance of the 1LO peak at 575 cm -1. This can be attributed to the presence of anion sublattice defects without any formation of higher oxides. The range of materials examined also allowed us to distinguish partly the chemical effects of alpha self-irradiation. The results obtained with water and hydrogen peroxide (a water radiolysis product) on a severely damaged 238PuO 2 specimen highlight a specific behavior, observed for the first time.
PROCESS FOR SEPARATING PLUTONIUM BY REPEATED PRECIPITATION WITH AMPHOTERIC HYDROXIDE CARRIERS
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.
Reactive spark plasma synthesis of CaZrTi2O7 zirconolite ceramics for plutonium disposition
NASA Astrophysics Data System (ADS)
Sun, Shi-Kuan; Stennett, Martin C.; Corkhill, Claire L.; Hyatt, Neil C.
2018-03-01
Near single phase zirconolite ceramics, prototypically CaZrTi2O7, were fabricated by reactive spark plasma sintering (RSPS), from commercially available CaTiO3, ZrO2 and TiO2 reagents, after processing at 1200 °C for only 1 h. Ceramics were of theoretical density and formed with a controlled mean grain size of 1.9 ± 0.6 μm. The reducing conditions of RSPS afforded the presence of paramagnetic Ti3+, as demonstrated by EPR spectroscopy. Overall, this study demonstrates the potential for RSPS to be a disruptive technology for disposition of surplus separated plutonium stockpiles in ceramic wasteforms, given its inherent advantage of near net shape products and rapid throughput.
NASA Astrophysics Data System (ADS)
Seitov, D. D.; Nekrasov, K. A.; Kupryazhkin, A. Ya.; Gupta, S. K.; Akilbekov, A. T.
2017-09-01
The interaction of xenon clusters with the collision cascades in the PuO2 crystals is investigated using the molecular dynamics simulation and the approximation of the pair interaction potentials. The potentials of interaction of Xe atoms with the surrounding particles in the crystal lattice are suggested, that are valid in the range of high collision energies. The cascades created by the recoil 235U ions formed as the plutonium α-decay product are considered, and the influence of such cascades on the structure of the xenon clusters is analyzed. It is shown, that the cascade-cluster interaction leads to release of the xenon atoms from the clusters and their subsequent re-solution in the crystal bulk.
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
Production and study of radionuclides at the research institute of atomic reactors (NIIAR)
DOE Office of Scientific and Technical Information (OSTI.GOV)
Karelin, E.A.; Gordeev, Y.N.; Filimonov, V.T.
1995-01-01
The main works of the Radionuclide Sources and Preparations Department (ORIP) of the Research Institute of Atomic Reactors (NIIAR) are summarized. The major activity of the Radionuclide Sources and Preparations Department (ORIP) is aimed at production of radioactive preparations of trans-plutonium elements (TPE) and also of lighter elements (from P to Ir), manufacture of ionizing radiation sources thereof, and scientific research to develop new technologies. One of the radionuclides that recently has received major attention is gadolinium-153. Photon sources based on it are used in densimeters for diagnostics of bone deseases. The procedure for separating gadolinium and europium, which ismore » currently used at the Research Institute of Atomic Reactors (NILAR), is based on europium cementation with the use of sodium amalgam. The method, though efficient, did not until recently permit an exhaustive removal of radioactive europium from {sup 153}Gd. The authors have thoroughly studied the separation process in semi-countercurrent mode, using citrate solutions. A special attention was given to the composition of europium complex species.« less
PRECIPITATION OF PLUTONOUS PEROXIDE
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)
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/.
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.
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.
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
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
Improving the Estimates of Waste from the Recycling of Used Nuclear Fuel - 13410
DOE Office of Scientific and Technical Information (OSTI.GOV)
Phillips, Chris; Willis, William; Carter, Robert
2013-07-01
Estimates are presented of wastes arising from the reprocessing of 50 GWD/tonne, 5 year and 50 year cooled used nuclear fuel (UNF) from Light Water Reactors (LWRs), using the 'NUEX' solvent extraction process. NUEX is a fourth generation aqueous based reprocessing system, comprising shearing and dissolution in nitric acid of the UNF, separation of uranium and mixed uranium-plutonium using solvent extraction in a development of the PUREX process using tri-n-butyl phosphate in a kerosene diluent, purification of the plutonium and uranium-plutonium products, and conversion of them to uranium trioxide and mixed uranium-plutonium dioxides respectively. These products are suitable for usemore » as new LWR uranium oxide and mixed oxide fuel, respectively. Each unit process is described and the wastes that it produces are identified and quantified. Quantification of the process wastes was achieved by use of a detailed process model developed using the Aspen Custom Modeler suite of software and based on both first principles equilibrium and rate data, plus practical experience and data from the industrial scale Thermal Oxide Reprocessing Plant (THORP) at the Sellafield nuclear site in the United Kingdom. By feeding this model with the known concentrations of all species in the incoming UNF, the species and their concentrations in all product and waste streams were produced as the output. By using these data, along with a defined set of assumptions, including regulatory requirements, it was possible to calculate the waste forms, their radioactivities, volumes and quantities. Quantification of secondary wastes, such as plant maintenance, housekeeping and clean-up wastes, was achieved by reviewing actual operating experience from THORP during its hot operation from 1994 to the present time. This work was carried out under a contract from the United States Department of Energy (DOE) and, so as to enable DOE to make valid comparisons with other similar work, a number of assumptions were agreed. These include an assumed reprocessing capacity of 800 tonnes per year, the requirement to remove as waste forms the volatile fission products carbon-14, iodine-129, krypton-85, tritium and ruthenium-106, the restriction of discharge of any water from the facility unless it meets US Environmental Protection Agency drinking water standards, no intentional blending of wastes to lower their classification, and the requirement for the recovered uranium to be sufficiently free from fission products and neutron-absorbing species to allow it to be re-enriched and recycled as nuclear fuel. The results from this work showed that over 99.9% of the radioactivity in the UNF can be concentrated via reprocessing into a fission-product-containing vitrified product, bottles of compressed krypton storage and a cement grout containing the tritium, that together have a volume of only about one eighth the volume of the original UNF. The other waste forms have larger volumes than the original UNF but contain only the remaining 0.1% of the radioactivity. (authors)« less
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
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
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
PLUTONIUM RECOVERY FROM NEUTRON-BOMBARDED URANIUM FUEL
Moore, R.H.
1962-04-10
A process of recovering plutonium from neutronbombarded uranium fuel by dissolving the fuel in equimolar aluminum chloride-potassium chloride; heating the mass to above 700 deg C for decomposition of plutonium tetrachloride to the trichloride; extracting the plutonium trichloride into a molten salt containing from 40 to 60 mole % of lithium chloride, from 15 to 40 mole % of sodium chloride, and from 0 to 40 mole % of potassium chloride or calcium chloride; and separating the layer of equimolar chlorides containing the uranium from the layer formed of the plutonium-containing salt is described. (AEC)
Pyrochemical recovery of plutonium from calcium fluoride reduction slag
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.
10 CFR 110.41 - Executive Branch review.
Code of Federal Regulations, 2010 CFR
2010-01-01
... export involving assistance to end uses related to isotope separation, chemical reprocessing, heavy water production, advanced reactors, or the fabrication of nuclear fuel containing plutonium, except for exports of... foreign reactor. (8) An export involving radioactive waste. (9) An export to any country listed in § 110...
Mechanistic approach for nitride fuel evolution and fission product release under irradiation
NASA Astrophysics Data System (ADS)
Dolgodvorov, A. P.; Ozrin, V. D.
2017-01-01
A model for describing uranium-plutonium mixed nitride fuel pellet burning was developed. Except fission products generating, the model includes impurities of oxygen and carbon. Nitrogen behaviour in nitride fuel was analysed and the nitrogen chemical potential in solid solution with uranium-plutonium nitride was constructed. The chemical program module was tested with the help of thermodynamic equilibrium phase distribution calculation. Results were compared with analogous data in literature, quite good agreement was achieved, especially for uranium sesquinitride, metallic species and some oxides. Calculation of a process of nitride fuel burning was also conducted. Used mechanistic approaches for fission product evolution give the opportunity to find fission gas release fractions and also volumes of intergranular secondary phases. Calculations present that the most massive secondary phases are the oxide and metallic phases. Oxide phase contain approximately 1 % wt of substance over all time of burning with slightly increasing of content. Metallic phase has considerable rising of mass and by the last stage of burning it contains about 0.6 % wt of substance. Intermetallic phase has less increasing rate than metallic phase and include from 0.1 to 0.2 % wt over all time of burning. The highest element fractions of released gaseous fission products correspond to caesium and iodide.
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
QUANTITATIVE PLUTONIUM MICRODISTRIBUTION IN BONE TISSUE OF VERTEBRA FROM A MAYAK WORKER
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
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: Advancing our Understanding to Support Sustainable Nuclear Fuel Cycles
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lines, Amanda M.; Adami, Susan R.; Casella, Amanda
With Global energy needs increasing, real energy solutions to meet demands now, are needed. Fossil fuels are not an ideal candidate to meet these needs because of their negative impact on the environment. Renewables such as wind and solar have huge potential, but still need major technological advancements (particularly in the area of battery storage) before they can effectively meet growing world needs. The best option for meeting large energy needs without a large carbon footprint is nuclear energy. Of course, nuclear energy can face a fair amount of opposition and concern. However, through modern engineering and science many ofmore » these concerns can now be addressed. Many safety concerns can be met by engineering advancements, but perhaps the biggest area of concern is what to do with the used nuclear fuel after it is removed from the reactor. Currently the United States (and several other countries) utilize an open fuel cycle, meaning fuel is only used once and then discarded. It should be noted that fuel coming out of a reactor has utilized approximately 1% of the total energy that could be produced by the uranium in the fuel rod. The answer here is to close the fuel cycle and recycle the nuclear materials. By reprocessing used nuclear fuel, all the U can be repurposed without requiring disposal. The various fission products can be removed and either discarded (hugely reduced waste volume) or more reasonably, utilized in specialty reactors to make more energy or needed research/medical isotopes. While reprocessing technology is currently advanced enough to meet energy needs, completing research to improve and better understand these techniques is still needed. Better understanding behavior of fission products is one area of important research. Despite it being discovered over 75 years ago, plutonium is still an exciting element to study because of the complex solution chemistry it exhibits. In aqueous solutions Pu can exist simultaneously in multiple oxidation states, including 3+, 4+, and 6+. It also readily forms a variety of metal-ligand complexes depending on solution pH and available ligands. Understanding of the behavior of Pu in solution remains an important area of research today, with relevance to developing sustainable nuclear fuel cycles, minimizing its impact on the environment, and detecting and preventing the spread of nuclear weapons technology.« less
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.
Concentrations of plutonium and americium in plankton from the western Mediterranean Sea.
Sanchez-Cabeza, Joan-Albert; Merino, Juan; Masqué, Pere; Mitchell, Peter I; Vintró, L León; Schell, William R; Cross, Lluïsa; Calbet, Albert
2003-07-20
Understanding the transfer of radionuclides through the food chain leading to man and in particular, the uptake of transuranic nuclides by plankton, is basic to assess the potential radiological risk of the consumption of marine products by man. The main sources of transuranic elements in the Mediterranean Sea in the past were global fallout and the Palomares accident, although at present smaller amounts are released from nuclear establishments in the northwestern region. Plankton from the western Mediterranean Sea was collected and analyzed for plutonium and americium in order to study their biological uptake. The microplankton fractions accounted for approximately 50% of the total plutonium contents in particulate form. At Garrucha (Palomares area), microplankton showed much higher 239,240 Pu activity, indicating the contamination with plutonium from the bottom sediments. Concentration factors were within the range of the values recommended by the International Atomic Energy Agency. Continental shelf mesoplankton was observed to efficiently concentrate transuranics. In open seawaters, concentrations were much lower. We speculate that sediments might play a role in the transfer of transuranics to mesoplankton in coastal waters, although we cannot discard that the difference in species composition may also play a role. In Palomares, both 239,240 Pu and 241Am showed activities five times higher than the mean values observed in continental shelf mesoplankton. As the plutonium isotopic ratios in the contaminated sample were similar to those found in material related to the accident, the contamination was attributed to bomb debris from the Palomares accident. Concentration factors in mesoplankton were also in relatively good agreement with the ranges recommended by IAEA. In the Palomares station the highest concentration factor was observed in the sample that showed predominance of the dynoflagellate Ceratium spp. Mean values of the enrichment factors showed, on average, discrimination rather than enrichment in the primary producer trophic chain.
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
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
The role of surfaces, chemical interfaces, and disorder on plutonium incorporation in pyrochlores
Perriot, Romain; Dholabhai, Pratik P.; Uberuaga, Blas P.
2016-07-27
Pyrochlores, a class of complex oxides with formula A 2B 2O 7, are one of the candidates for nuclear waste encapsulation, due to the natural occurrence of actinide-bearing pyrochlore minerals and laboratory observations of high radiation tolerance. In this work, we use atomistic simulations to determine the role of surfaces, chemical interfaces, and cation disorder on the plutonium immobilization properties of pyrochlores as a function of pyrochlore chemistry. We find that both Pu 3+ and Pu 4+ segregate to the surface for the four low-index pyrochlore surfaces considered, and that the segregation energy varies with the chemistry of the compound.more » We also find that pyrochlore/pyrochlore bicrystals A 2B 2O 7/A 2'B 2'O 7 can be used to immobilize Pu 3+ and Pu 4+ either in the same or separate phases of the compound, depending on the chemistry of the material. Finally, we find that Pu 4+ segregates to the disordered phase of an order/disorder bicrystal, driven by the occurrence of local oxygen-rich environments. However, Pu 3+ is weakly sensitive to the oxygen environment, and therefore only slightly favors the disordered phase. This behavior suggests that, at some concentration, Pu incorporation can destabilize the pyrochlore structure. Together, these results provide new insight into the ability of pyrochlore compounds to encapsulate Pu and suggest new considerations in the development of waste forms based on pyrochlores. Particularly, the phase structure of a multi-phase pyrochlore composite can be used to independently getter decay products based on their valence and size.« less
NASA Astrophysics Data System (ADS)
Cheng, Ting; Baney, Ronald H.; Tulenko, James
2010-10-01
Silicon carbide is one of the prime candidates as a matrix material in inert matrix fuels (IMF) being designed to reduce the plutonium inventories. Since complete fission and transmutation is not practical in a single in-core run, it is necessary to separate the non-transmuted actinide materials from the silicon carbide matrix for recycling. In this work, SiC was corroded in sodium carbonate (Na 2CO 3) and potassium carbonate (K 2CO 3), to form water soluble sodium or potassium silicate. Separation of the transuranics was achieved by dissolving the SiC corrosion product in boiling water. Ceria (CeO 2), which was used as a surrogate for plutonium oxide (PuO 2), was not corroded in these molten salt environments. The molten salt depth, which is a distance between the salt/air interface to the upper surface of SiC pellets, significantly affected the rate of corrosion. The corrosion was faster in K 2CO 3 than in Na 2CO 3 molten salt at 1050 °C, when the initial molten salt depths were kept the same for both salts.
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. ...
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 ...
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.
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.
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.
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)
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lopez-Menchero, E.; Centeno, J.; Magni, G.
1962-03-01
The extraction of traces of Ru, Zr, Nb, Ce, and U at low concentrations (5 mg/l in aqueous solution) from nitric acid solutions using trilauryl amine (TLA) has been experimentally studied. TLA will eventually be used for final purification of plutonium. Room-temperature data on plutonium contaminant distribution between aqueous solutions of varying nitric acid concentrations and a Shellsol-T solution containing l0% TlA and 5% octyl alcohol are presented. Within the temperature and nitric acid concentration ranges tested, the extractability of uranium increased with increased acid concentrations, although acid concentration in the aqueous phase had no effect on the decontamination factorsmore » for the main fission products. (H.G.G.)« less
SEPARATION OF PLUTONIUM IONS FROM SOLUTION BY ADSORPTION ON ZIRCONIUM PYROPHOSPHATE
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
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.
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
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
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.
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.
Where Radiobiology Began in Russia: A Physician’s Perspective
2010-09-01
radiation incidents at the MPA and conduct studies of long-term health effects of radiation exposure on that population and also the general public along...White Archipelago”) (Gubarev, 2004): “Visiting a number of production facilities that worked with plutonium and polonium - 210 , I was struck by the...were established for major food products. These standards, of course, were higher than the Union-wide public health standards. They did not begin
DOE Office of Scientific and Technical Information (OSTI.GOV)
Le Mer, J.; Garzenne, C.; Lemasson, D.
In the frame of the French Act of June 28, 2006 on 'a sustainable management of nuclear materials and radioactive waste' EDF R and D assesses various research scenarios of transition between the actual French fleet and a Generation IV fleet with a closed fuel cycle where plutonium is multi-recycled. The basic scenarios simulate a deployment of 60 GWe of Sodium-cooled Fast Reactors (SFRs) in two steps: one third from 2040 to 2050 and the rest from 2080 to 2100 (scenarios 2040). These research scenarios assume that SFR technology will be ready for industrial deployment in 2040. One of themore » many sensitivity analyses that EDF, as a nuclear power plant operator, must evaluate is the impact of a delay of SFR technology in terms of uranium consumptions, plutonium needs and fuel cycle utilities gauging. The sensitivity scenarios use the same assumptions as scenarios 2040 but they simulate a different transition phase: SFRs are deployed in one step between 2080 and 2110 (scenarios 2080). As the French Act states to conduct research on minor actinides (MA) management, we studied different options for 2040 and 2080 scenarios: no MA transmutation, americium transmutation in heterogeneous mode based on americium Bearing Blankets (AmBB) in SFRs and all MA transmutation in heterogeneous mode based on MA Bearing Blankets (MABB). Moreover, we studied multiple parameters that could impact the deployment of these reactors (SFR load factor, increase of the use of MOX in Light Water Reactors, increase of the cooling time in spent nuclear fuel storage...). Each scenario has been computed with the EDF R and D fuel cycle simulation code TIRELIRE-STRATEGIE and optimized to meet various fuel cycle constraints such as using the reprocessing facility with long period of constant capacity, keeping the temporary stored mass of plutonium and MA under imposed limits, recycling older assemblies first... These research scenarios show that the transition from the current PWR fleet to an equivalent fleet of Generation IV SFR can follow different courses. The design of SFR-V2B that we used in our studies needs a high inventory of plutonium resulting in tension on this resource. Several options can be used in order to loosen this tension: our results lead to favour the use of axial breeding blanket in SFR. Load factor of upcoming reactors has to be regarded with attention as it has a high impact on plutonium resource for a given production of electricity. The deployment of SFRs beginning in 2080 instead of 2040 following the scenarios we described creates higher tensions on reprocessing capacity, separated plutonium storage and spent fuel storage. In the frame of the French Act, we studied minor actinides transmutation. The flux of MA in all fuel cycle plants is really high, which will lead to decay heat, a and neutron emission related problems. In terms of reduction of MA inventories, the deployment of MA transmutation cycle must not delay the installation of SFRs. The plutonium production in MABB and AmBB does not allow reducing the use of axial breeding blankets. The impact of MA or Am transmutation over the high level waste disposal is more important if the SFRs are deployed later. Transmutation option (americium or all MA) does not have a significant impact on the number of canister produced nor on its long-term thermal properties. (authors)« less
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
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.
CONCENTRATION OF Pu USING AN IODATE PRECIPITATE
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.
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
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
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
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 ...
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
AMINE EXTRACTION OF PLUTONIUM FROM NITRIC ACID SOLUTIONS LOADING AND STRIPPING EXPERIMENTS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wilson, A.S.
1961-01-19
Information is presented on a suitable amine processing system for plutonium nitrate. Experiments with concentrated plutonium nitrate solutions show that trilaurylamine (TLA) - xylene solvent systems did not form a second organic phase. Experiments are also reported with tri-noctylamine (TnOA)-xylene and TLA-Amsco - octyl alcohol. Two organic phases appear in both these systems at high plutonium nitrate concentrations. Data are tabulated from loading and stripping experiments. (J.R.D.)
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
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.
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
plutonium from uranium and fission products in an aqueous acidic solution by use of a chelating agent. The concentration is adjusted to about 1 N bar. The aqueous solution is then contacted with a water-immiscible organic solvent solution and the chelating agent. The chelating agents covered by this invention comprise
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kippen, Karen Elizabeth
This is Los Alamos National Laboratory's (LANL) June 2016 newsletter of the Materials Science and Technology Division. The following are major topics in this newsletter: MST-8 scientists guide national efforts to overcome nuclear energy technical challenges, first-ever scanning probe microscopy capabilities for plutonium, laboratory metallurgists make thorium targets for production of cancer-fighting isotopes, and a spotlight on Veronica Livescu.
Environmental radiation and the lung
Hamrick, Philip E.; Walsh, Phillip J.
1974-01-01
Environmental sources of radioactive materials and their relation to lung doses and lung burdens are described. The approaches used and the problems encountered in estimating lung doses are illustrated. Exposure to radon daughter products is contrasted to exposure to plutonium as particular examples of the hazards associated with radioactive materials of different chemical and physical characteristics. PMID:4620334
The nuclear arsenals and nuclear disarmament.
Barnaby, F
1998-01-01
Current world stockpiles of nuclear weapons and the status of treaties for nuclear disarmament and the ultimate elimination of nuclear weapons are summarised. The need for including stockpiles of civil plutonium in a programme for ending production and disposing of fissile materials is emphasized, and the ultimate difficulty of disposing of the last few nuclear weapons discussed.
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
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.
69. INTERIOR, BUILDING 272 (PLUTONIUM STORAGE BUILDING) LOOKING SOUTHWEST THROUGH ...
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
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
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.
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
Using Downhole Probes to Locate and Characterize Buried Transuranic and Mixed Low Level Waste
DOE Office of Scientific and Technical Information (OSTI.GOV)
Steinman, Donald K; Bramblett, Richard L; Hertzog, Russel C
2012-06-25
Borehole logging probes were developed and tested to locate and quantify transuranic elements in subsurface disposal areas and in contaminated sites at USDOE Weapons Complex sites. A new method of measuring very high levels of chlroine in the subsurface was developed using pulsed neutron technology from oilfield applications. The probes were demonstrated at the Hanford site in wells containing plutonium and other contaminants.
METHOD OF REDUCING PLUTONIUM COMPOUNDS
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 ...
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
Synthesis of actinide nitrides, phosphides, sulfides and oxides
Van Der Sluys, William G.; Burns, Carol J.; Smith, David C.
1992-01-01
A process of preparing an actinide compound of the formula An.sub.x Z.sub.y wherein An is an actinide metal atom selected from the group consisting of thorium, uranium, plutonium, neptunium, and americium, x is selected from the group consisting of one, two or three, Z is a main group element atom selected from the group consisting of nitrogen, phosphorus, oxygen and sulfur and y is selected from the group consisting of one, two, three or four, by admixing an actinide organometallic precursor wherein said actinide is selected from the group consisting of thorium, uranium, plutonium, neptunium, and americium, a suitable solvent and a protic Lewis base selected from the group consisting of ammonia, phosphine, hydrogen sulfide and water, at temperatures and for time sufficient to form an intermediate actinide complex, heating said intermediate actinide complex at temperatures and for time sufficient to form the actinide compound, and a process of depositing a thin film of such an actinide compound, e.g., uranium mononitride, by subliming an actinide organometallic precursor, e.g., a uranium amide precursor, in the presence of an effectgive amount of a protic Lewis base, e.g., ammonia, within a reactor at temperatures and for time sufficient to form a thin film of the actinide compound, are disclosed.
Environmental Information Document: L-reactor reactivation
DOE Office of Scientific and Technical Information (OSTI.GOV)
Mackey, H.E. Jr.
1982-04-01
Purpose of this Environmental Information Document is to provide background for assessing environmental impacts associated with the renovation, restartup, and operation of L Reactor at the Savannah River Plant (SRP). SRP is a major US Department of Energy installation for the production of nuclear materials for national defense. The purpose of the restart of L Reactor is to increase the production of nuclear weapons materials, such as plutonium and tritium, to meet projected needs in the nuclear weapons program.
Coprocessed nuclear fuels containing (U, Pu) values as oxides, carbides or carbonitrides
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
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.
Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA. A Long-Term Study
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.
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.
PYROCHEMICAL DECONTAMINATION METHOD FOR REACTOR FUEL
Buyers, A.G.
1959-06-30
A pyro-chemical method is presented for decontaminating neutron irradiated uranium and separating plutonium therefrom by contact in the molten state with a metal chloride salt. Uranium trichloride and uranium tetrachloride either alone or in admixture with alkaline metal and alkaline eanth metal fluorides under specified temperature and specified phase ratio conditions extract substantially all of the uranium from the irradiated uranium fuel together with certain fission products. The phases are then separated leaving purified uranium metal. The uranium and plutonium in the salt phase can be reduced to forin a highly decontaminated uraniumplutonium alloy. The present method possesses advantages for economically decontaminating irradiated nuclear fuel elements since irradiated fuel may be proccessed immediately after withdrawal from the reactor and the uranium need not be dissolved and later reduced to the metallic form. Accordingly, the uranium may be economically refabricated and reinserted into the reactor.
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)
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 ...
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
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.
SOLVENT EXTRACTION PROCESS FOR PLUTONIUM
Seaborg, G.T.
1959-04-14
The separation of plutonium from aqueous inorganic acid solutions by the use of a water immiscible organic extractant liquid is described. The plutonium must be in the oxidized state, and the solvents covered by the patent include nitromethane, nitroethane, nitropropane, and nitrobenzene. The use of a salting out agents such as ammonium nitrate in the case of an aqueous nitric acid solution is advantageous. After contacting the aqueous solution with the organic extractant, the resulting extract and raffinate phases are separated. The plutonium may be recovered by any suitable method.
Complexation of lanthanides and actinides by acetohydroxamic acid
DOE Office of Scientific and Technical Information (OSTI.GOV)
Taylor, R.J.; Sinkov, S.I.; Choppin, G.R.
2008-07-01
Acetohydroxamic acid (AHA) has been proposed as a suitable reagent for the complexant-based, as opposed to reductive, stripping of plutonium and neptunium ions from the tributylphosphate solvent phase in advanced PUREX or UREX processes designed for future nuclear-fuel reprocessing. Stripping is achieved by the formation of strong hydrophilic complexes with the tetravalent actinides in nitric acid solutions. To underpin such applications, knowledge of the complexation constants of AHA with all relevant actinide (5f) and lanthanide (4f) ions is therefore important. This paper reports the determination of stability constants of AHA with the heavier lanthanide ions (Dy-Yb) and also U(IV) andmore » Th(IV) ions. Comparisons with our previously published AHA stability-constant data for 4f and 5f ions are made. (authors)« less
Sources of plutonium in the atmosphere and stratosphere-troposphere mixing
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
DOE Office of Scientific and Technical Information (OSTI.GOV)
Doane, R.W.; Grant, R.H.
1996-09-01
Thermo NUtech is the prime contractor for the Defense Nuclear Agency (DNA), responsible for the operation and maintenance of the Johnston Atoll plutonium Contaminated Soil Cleanup Project. During this production period, the Scope of Work included movement of soil to and from the plant, processing contaminated soil through the Segmented Gate System (SGS) and Soil Washing System, packaging of waste soil for shipment, identification and implementation of process improvements, data collection and validation, and compliance with all applicable regulations governing environmental safety and health. The SGS utilizes arrays of sensitive radiation detectors coupled with sophisticated computer software to segregate contaminatedmore » soil from a moving feed supply on conveyor belts. Contaminated soil is diverted to a `hot path` for plutonium particles greater than 5000 Becquerels or to a supplemental soil washing process designed to remove dispersed low leve%l contamination from a soil faction consisting of very small particles. Low to intermediate levels of contamination are removed from the soil to meet DNA`s criteria for unrestricted use of less than 500 Becquerels per kilogram of soil, with no hot particles. The low level concentrate is expected to be packaged for shipment to an approved defense waste disposal site.« less
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Robertson, Janeen Denise
In a mortality study of white males who had worked at the Rocky Flats Nuclear Weapons Plant between 1952 and 1979, an increased number of deaths from benign and unspecified intracranial neoplasms was found. A case-control study nested within this cohort investigated the hypothesis that an association existed between brain tumor death and exposure to either internally deposited plutonium or external ionizing radiation. There was no statistically significant association found between estimated radiation exposure from internally deposited plutonium and the development of brain tumors. Exposure by job or work area showed no significant difference between the cohort and the controlmore » groups. An update of the study found elevated risk estimates for (1) all lymphopoietic neoplasms, and (2) all causes of death in employees with body burdens greater than or equal to two nanocuries of plutonium. There was an excess of brain tumors for the entire cohort. Similar cohort studies conducted on worker populations from other plutonium handling facilities have not yet shown any elevated risks for brain tumors. Historically, the Rocky Flats Nuclear Weapons Plant used large quantities of chemicals in their production operations. The use of solvents, particularly carbon tetrachloride, was unique to Rocky Flats. No investigation of the possible confounding effects of chemical exposures was done in the initial studies. The objectives of the present study are to (1) investigate the history of chemical use at the Rocky Flats facility; (2) locate and analyze chemical monitoring information in order to assess employee exposure to the chemicals that were used in the highest volume; and (3) determine the feasibility of establishing a chemical exposure assessment model that could be used in future epidemiology studies.« less
Plutonium release from the 903 pad at Rocky Flats.
Mongan, T R; Ripple, S R; Winges, K D
1996-10-01
The Colorado Department of Public Health and Environment (CDH) sponsored a study to reconstruct contaminant doses to the public from operations at the Rocky Flats nuclear weapons plant. This analysis of the accidental release of plutonium from the area known as the 903 Pad is part of the CDH study. In the 1950's and 1960's, 55-gallon drums of waste oil contaminated with plutonium, and uranium were stored outdoors at the 903 Pad. The drums corroded, leaking contaminated oil onto soil subsequently carried off-site by the wind. The plutonium release is estimated using environmental data from the 1960's and 1970's and an atmospheric transport model for fugitive dust. The best estimate of total plutonium release to areas beyond plant-owned property is about 0.26 TBq (7 Ci). Off-site airborne concentrations and deposition of plutonium are estimated for dose calculation purposes. The best estimate of the highest predicted off-site effective dose is approximately 72 microSv (7.2 mrem).
Xu, C; Santschi, P H; Zhong, J Y; Hatcher, P G; Francis, A J; Dodge, C J; Roberts, K A; Hung, C C; Honeyman, B D
2008-11-15
Relatively recently, inorganic colloids have been invoked to reconcile the apparent contradictions between expectations based on classical dissolved-phase Pu transport and field observations of "enhanced" Pu mobility (Kersting et al. Nature 1999, 397, 56-59). A new paradigm for Pu transport is mobilization and transport via biologically produced ligands. This study for the first time reports a new finding of Pu being transported, at sub-pM concentrations, by a cutin-like natural substance containing siderophore-like moieties and virtually all mobile Pu. Most likely, Pu is complexed by chelating groups derived from siderophores that are covalently bound to a backbone of cutin-derived soil degradation products, thus revealing the history of initial exposure to Pu. Features such as amphiphilicity and small size make this macromolecule an ideal collector for actinides and other metals and a vector for their dispersal. Cross-linking to the hydrophobic domains (e.g., by polysaccharides) gives this macromolecule high mobility and a means of enhancing Pu transport. This finding provides a new mechanism for Pu transport through environmental systems that would not have been predicted by Pu transport models.
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
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
DOE Office of Scientific and Technical Information (OSTI.GOV)
Crowder, M.; Pierce, R.
2012-08-22
H-Canyon and HB-Line are tasked with the production of PuO{sub 2} from a feed of plutonium metal. The PuO{sub 2} will provide feed material for the MOX Fuel Fabrication Facility. After dissolution of the Pu metal in H-Canyon, the solution will be transferred to HB-Line for purification by anion exchange. Subsequent unit operations include Pu(IV) oxalate precipitation, filtration and calcination to form PuO{sub 2}. This report details the results from SRNL anion exchange, precipitation, filtration, calcination, and characterization tests, as requested by HB-Line1 and described in the task plan. This study involved an 80-g batch of Pu and employed testmore » conditions prototypical of HB-Line conditions, wherever feasible. In addition, this study integrated lessons learned from earlier anion exchange and precipitation and calcination studies. H-Area Engineering selected direct strike Pu(IV) oxalate precipitation to produce a more dense PuO{sub 2} product than expected from Pu(III) oxalate precipitation. One benefit of the Pu(IV) approach is that it eliminates the need for reduction by ascorbic acid. The proposed HB-Line precipitation process involves a digestion time of 5 minutes after the time (44 min) required for oxalic acid addition. These were the conditions during HB-line production of neptunium oxide (NpO{sub 2}). In addition, a series of small Pu(IV) oxalate precipitation tests with different digestion times were conducted to better understand the effect of digestion time on particle size, filtration efficiency and other factors. To test the recommended process conditions, researchers performed two nearly-identical larger-scale precipitation and calcination tests. The calcined batches of PuO{sub 2} were characterized for density, specific surface area (SSA), particle size, moisture content, and impurities. Because the 3013 Standard requires that the calcination (or stabilization) process eliminate organics, characterization of PuO{sub 2} batches monitored the presence of oxalate by thermogravimetric analysis-mass spectrometry (TGA-MS). To use the TGA-MS for carbon or oxalate content, some method development will be required. However, the TGA-MS is already used for moisture measurements. Therefore, SRNL initiated method development for the TGA-MS to allow quantification of oxalate or total carbon. That work continues at this time and is not yet ready for use in this study. However, the collected test data can be reviewed later as those analysis tools are available.« less
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.
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
``Recycling'' Nuclear Power Plant Waste: Technical Difficulties and Proliferation Concerns
NASA Astrophysics Data System (ADS)
Lyman, Edwin
2007-04-01
One of the most vexing problems associated with nuclear energy is the inability to find a technically and politically viable solution for the disposal of long-lived radioactive waste. The U.S. plan to develop a geologic repository for spent nuclear fuel at Yucca Mountain in Nevada is in jeopardy, as a result of managerial incompetence, political opposition and regulatory standards that may be impossible to meet. As a result, there is growing interest in technologies that are claimed to have the potential to drastically reduce the amount of waste that would require geologic burial and the length of time that the waste would require containment. A scenario for such a vision was presented in the December 2005 Scientific American. While details differ, these technologies share a common approach: they require chemical processing of spent fuel to extract plutonium and other long-lived actinide elements, which would then be ``recycled'' into fresh fuel for advanced reactors and ``transmuted'' into shorter-lived fission products. Such a scheme is the basis for the ``Global Nuclear Energy Partnership,'' a major program unveiled by the Department of Energy (DOE) in early 2006. This concept is not new, but has been studied for decades. Major obstacles include fundamental safety issues, engineering feasibility and cost. Perhaps the most important consideration in the post-9/11 era is that these technologies involve the separation of plutonium and other nuclear weapon-usable materials from highly radioactive fission products, providing opportunities for terrorists seeking to obtain nuclear weapons. While DOE claims that it will only utilize processes that do not produce ``separated plutonium,'' it has offered no evidence that such technologies would effectively deter theft. It is doubtful that DOE's scheme can be implemented without an unacceptable increase in the risk of nuclear terrorism.
Hunt, Paul; Lawson, Janice
2018-06-22
A video series presenting an overview of the Savannah River Site (SRS) mission and operations. Each episode features a specific area/operation and how it contributes to help make the world safer. This episode features K Area's mission and operations. K area is the former production reactor that's been re-purposed to serve as a plutonium processing and storage facility.
18. VIEW OF THE NORTH ELEVATION OF BUILDING 71 (771) ...
18. VIEW OF THE NORTH ELEVATION OF BUILDING 71 (771) UNDER CONSTRUCTION IN 1952. BUILDING 71 WAS THE ORIGINAL PLUTONIUM OPERATIONS BUILDING. PRODUCTION BUILDINGS WERE BUILT INTO HILLSIDES AND/OR BELOW GRADE AS A SAFETY MEASURE AGAINST RUSSIAN ATTACK (3/2/52). - Rocky Flats Plant, Bounded by Indiana Street & Routes 93, 128 & 72, Golden, Jefferson County, CO
Code of Federal Regulations, 2014 CFR
2014-01-01
... dissolution, solvent extraction, and process liquor storage. There may also be equipment for thermal denitration of uranium nitrate, conversion of plutonium nitrate to oxide metal, and treatment of fission product waste liquor to a form suitable for long term storage or disposal. However, the specific type and...
Code of Federal Regulations, 2013 CFR
2013-01-01
... dissolution, solvent extraction, and process liquor storage. There may also be equipment for thermal denitration of uranium nitrate, conversion of plutonium nitrate to oxide metal, and treatment of fission product waste liquor to a form suitable for long term storage or disposal. However, the specific type and...
Code of Federal Regulations, 2012 CFR
2012-01-01
... dissolution, solvent extraction, and process liquor storage. There may also be equipment for thermal denitration of uranium nitrate, conversion of plutonium nitrate to oxide metal, and treatment of fission product waste liquor to a form suitable for long term storage or disposal. However, the specific type and...
Critical review of analytical techniques for safeguarding the thorium-uranium fuel cycle
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hakkila, E.A.
1978-10-01
Conventional analytical methods applicable to the determination of thorium, uranium, and plutonium in feed, product, and waste streams from reprocessing thorium-based nuclear reactor fuels are reviewed. Separations methods of interest for these analyses are discussed. Recommendations concerning the applicability of various techniques to reprocessing samples are included. 15 tables, 218 references.
Study on reduction and back extraction of Pu(IV) by urea derivatives in nitric acid conditions
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ye, G.A.; Xiao, S.T.; Yan, T.H.
2013-07-01
The reduction kinetics of Pu(IV) by hydroxyl-semicarbazide (HSC), hydroxyurea (HU) and di-hydroxyurea (DHU) in nitric acid solutions were investigated separately with adequate kinetic equations. In addition, counter-current cascade experiments were conducted for Pu split from U in nitric acid media using three kinds of reductant, respectively. The results show that urea derivatives as a kind of novel salt-free reductant can reduce Pu(IV) to Pu(III) rapidly in the nitric acid solutions. The stripping experimental results showed that Pu(IV) in the organic phase can be stripped rapidly to the aqueous phase by the urea derivatives, and the separation factors of plutonium /uraniummore » can reach more than 10{sup 4}. This indicates that urea derivatives is a kind of promising salt-free agent for uranium/plutonium separation. In addition, the complexing effect of HSC with Np(IV) was revealed, and Np(IV) can be back-extracted by HSC with a separation factor of about 20.« less
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
NASA Technical Reports Server (NTRS)
Vorobiova, M. I.; Degteva, M. O.; Neta, M. O. (Principal Investigator)
1999-01-01
The Techa River (Southern Urals, Russia) was contaminated in 1949-1956 by liquid radioactive wastes from the Mayak complex, the first Russian facility for the production of plutonium. The measurements of environmental contamination were started in 1951. A simple model describing radionuclide transport along the free-flowing river and the accumulation of radionuclides by bottom sediments is presented. This model successfully correlates the rates of radionuclide releases as reconstructed by the Mayak experts, hydrological data, and available environmental monitoring data for the early period of contamination (1949-1951). The model was developed to reconstruct doses for people who lived in the riverside communities during the period of the releases and who were chronically exposed to external and internal irradiation. The model fills the data gaps and permits reconstruction of external gamma-exposure rates in air on the river bank and radionuclide concentrations in river water used for drinking and other household needs in 1949-1951.
Methods to Collect, Compile, and Analyze Observed Short-lived Fission Product Gamma Data
DOE Office of Scientific and Technical Information (OSTI.GOV)
Finn, Erin C.; Metz, Lori A.; Payne, Rosara F.
2011-09-29
A unique set of fission product gamma spectra was collected at short times (4 minutes to 1 week) on various fissionable materials. Gamma spectra were collected from the neutron-induced fission of uranium, neptunium, and plutonium isotopes at thermal, epithermal, fission spectrum, and 14-MeV neutron energies. This report describes the experimental methods used to produce and collect the gamma data, defines the experimental parameters for each method, and demonstrates the consistency of the measurements.
RECOVERY OF PLUTONIUM BY CARRIER PRECIPITATION
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.
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
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
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
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.
Rapid Method for Sodium Hydroxide Fusion of Concrete and ...
Technical Fact Sheet Analysis Purpose: Qualitative analysis Technique: Alpha spectrometry Method Developed for: Americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in concrete and brick samples Method Selected for: SAM lists this method for qualitative analysis of americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in concrete or brick building materials. Summary of subject analytical method which will be posted to the SAM website to allow access to the method.
METHOD OF SEPARATING PLUTONIUM FROM LANTHANUM FLUORIDE CARRIER
Watt, G.W.; Goeckermann, R.H.
1958-06-10
An improvement in oxidation-reduction type methods of separating plutoniunn from elements associated with it in a neutron-irradiated uranium solution is described. The method relates to the separating of plutonium from lanthanum ions in an aqueous 0.5 to 2.5 N nitric acid solution by 'treating the solution, at room temperature, with ammonium sulfite in an amount sufficient to reduce the hexavalent plutonium present to a lower valence state, and then treating the solution with H/sub 2/O/sub 2/ thereby forming a tetravalent plutonium peroxide precipitate.
1. VIEW OF THE CONTROL ROOM FOR THE XY RETRIEVER. ...
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
PROCESS OF MAKING A NEUTRONIC REACTOR FUEL ELEMENT COMPOSITION
Alter, H.W.; Davidson, J.K.; Miller, R.S.; Mewherter, J.L.
1959-01-13
A process is presented for making a ceramic-like material suitable for use as a nuclear fuel. The material consists of a solid solution of plutonium dioxide in uranium dioxide and is produced from a uranyl nitrate -plutonium nitrate solution containing uraniunm and plutonium in the desired ratio. The uranium and plutonium are first precipitated from the solution by addition of NH/ sub 4/OH and the dried precipitate is then calcined at 600 C in a hydrogen atmosphere to yield the desired solid solution of PuO/sub 2/ in UO/sub 2/.
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
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
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.
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.
Radiation damage and annealing in plutonium tetrafluoride
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
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.
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.
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.
Room airflow studies using sonic anemometry.
Wasiolek, P T; Whicker, J J; Gong, H; Rodgers, J C
1999-06-01
To ensure prompt response by real-time air monitors to an accidental release of toxic aerosols in a workplace, safety professionals should understand airflow patterns. This understanding can be achieved with validated computational fluid dynamics (CFD) computer simulations, or with experimental techniques, such as measurements with smoke, neutrally buoyant markers, trace gases, or trace aerosol particles. As a supplementary technique to quantify airflows, the use of a state-of-the art, three-dimensional sonic anemometer was explored. This instrument allows for the precise measurements of the air-velocity vector components in the range of a few centimeters per second, which is common in many indoor work environments. Measurements of air velocities and directions at selected locations were made for the purpose of providing data for characterizing fundamental aspects of indoor air movement in two ventilated rooms and for comparison to CFD model predictions. One room was a mockup of a plutonium workroom, and the other was an actual functioning plutonium workroom. In the mockup room, air-velocity vector components were measured at 19 locations at three heights (60, 120 and 180 cm) with average velocities varying from 1.4 cm s-1 to 9.7 cm s-1. There were complex flow patterns observed with turbulence intensities from 39% up to 108%. In the plutonium workroom, measurements were made at the breathing-zone height, recording average velocities ranging from 9.9 cm s-1 to 35.5 cm s-1 with turbulence intensities from 33% to 108%.
NASA Astrophysics Data System (ADS)
Brown, M. Alex; Paulenova, Alena; Tkac, Peter
2010-03-01
The stability constant of the Pu(IV)-acetohydroxamic acid complex Pu(AHA)3+ at 1 M ionic strength (pH = 0) has been investigated by method of solvent extraction. Di(2-ethylhexyl) phosphoric acid (HDEHP) was used to extract Pu(IV) from perchloric and nitric acid media at various AHA concentrations. Distribution ratios over a range of ligand concentrations were used in conjunction with graphical methods to obtain logβ1 = 14.3 ± 0.03 in perchloric acid. The stability constant determined from solutions in nitric acid was excluded because of the uncertainty in plutonium speciation.
METHOD OF OPERATING NUCLEAR REACTORS
Untermyer, S.
1958-10-14
A method is presented for obtaining enhanced utilization of natural uranium in heavy water moderated nuclear reactors by charging the reactor with an equal number of fuel elements formed of natural uranium and of fuel elements formed of uranium depleted in U/sup 235/ to the extent that the combination will just support a chain reaction. The reactor is operated until the rate of burnup of plutonium equals its rate of production, the fuel elements are processed to recover plutonium, the depleted uranium is discarded, and the remaining uranium is formed into fuel elements. These fuel elements are charged into a reactor along with an equal number of fuel elements formed of uranium depleted in U/sup 235/ to the extent that the combination will just support a chain reaction, and reuse of the uranium is continued as aforesaid until it wlll no longer support a chain reaction when combined with an equal quantity of natural uranium.
PLUTONIUM-CERIUM-COPPER ALLOYS
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 ...
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 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
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...
PREPARATION OF HALIDES OF PLUTONIUM
Garner, C.S.; Johns, I.B.
1958-09-01
A dry chemical method is described for preparing plutonium halides, which consists in contacting plutonyl nitrate with dry gaseous HCl or HF at an elevated temperature. The addition to the reaction gas of a small quantity of an oxidizing gas or a reducing gas will cause formation of the tetra- or tri-halide of plutonium as desired.
Enhanced ionization efficiency in TIMS analyses of plutonium and americium using porous ion emitters
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
ARIES Oxide Production Program Assessment of Risk to Long-term Sustainable Production Rate
DOE Office of Scientific and Technical Information (OSTI.GOV)
Whitworth, Julia; Lloyd, Jane Alexandria; Majors, Harry W.
2017-05-04
This report describes an assessment of risks and the development of a risk watch list for the ARIES Oxide Production Program conducted in the Plutonium Facility at LANL. The watch list is an active list of potential risks and opportunities that the management team periodically considers to maximize the likelihood of program success. The initial assessments were made in FY 16. The initial watch list was reviewed in September 2016. The initial report was not issued. Revision 1 has been developed based on management review of the original watch list and includes changes that occurred during FY-16.
Automated Metrology System for Pu 238
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wunderlich, Richard J.
Under a collaborative partnership between the NASA and DOE, a new automated measurement system developed by ORNL will ensure quality production of plutonium-238 while reducing handling by workers. NASA has funded ORNL and other national laboratories to develop a process that will restore US production capability of Pu-238 for the first time since the late 1980s when the Savannah River Plant ceased production. ORNL has produced and separated about 100 grams of the material and plans to scale up the process over the next several years to meet demand to power NASA deep space missions.
Real-time monitoring of plutonium content in uranium-plutonium alloys
Li, Shelly Xiaowei; Westphal, Brian Robert; Herrmann, Steven Douglas
2015-09-01
A method and device for the real-time, in-situ monitoring of Plutonium content in U--Pu Alloys comprising providing a crucible. The crucible has an interior non-reactive to a metallic U--Pu alloy within said interior of said crucible. The U--Pu alloy comprises metallic uranium and plutonium. The U--Pu alloy is heated to a liquid in an inert or reducing atmosphere. The heated U--Pu alloy is then cooled to a solid in an inert or reducing atmosphere. As the U--Pu alloy is cooled, the temperature of the U--Pu alloy is monitored. A solidification temperature signature is determined from the monitored temperature of the U--Pu alloy during the step of cooling. The amount of Uranium and the amount of Plutonium in the U--Pu alloy is then determined from the determined solidification temperature signature.
Plutonium segregation in glassy aerodynamic fallout from a nuclear weapon test
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
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
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
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.
Economic Analysis of Complex Nuclear Fuel Cycles with NE-COST
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ganda, Francesco; Dixon, Brent; Hoffman, Edward
The purpose of this work is to present a new methodology, and associated computational tools, developed within the U.S. Department of Energy (U.S. DOE) Fuel Cycle Option Campaign to quantify the economic performance of complex nuclear fuel cycles. The levelized electricity cost at the busbar is generally chosen to quantify and compare the economic performance of different baseload generating technologies, including of nuclear: it is the cost of electricity which renders the risk-adjusted discounted net present value of the investment cash flow equal to zero. The work presented here is focused on the calculation of the levelized cost of electricitymore » of fuel cycles at mass balance equilibrium, which is termed LCAE (Levelized Cost of Electricity at Equilibrium). To alleviate the computational issues associated with the calculation of the LCAE for complex fuel cycles, a novel approach has been developed, which has been called the “island approach” because of its logical structure: a generic complex fuel cycle is subdivided into subsets of fuel cycle facilities, called islands, each containing one and only one type of reactor or blanket and an arbitrary number of fuel cycle facilities. A nuclear economic software tool, NE-COST, written in the commercial programming software MATLAB®, has been developed to calculate the LCAE of complex fuel cycles with the “island” computational approach. NE-COST has also been developed with the capability to handle uncertainty: the input parameters (both unit costs and fuel cycle characteristics) can have uncertainty distributions associated with them, and the output can be computed in terms of probability density functions of the LCAE. In this paper NE-COST will be used to quantify, as examples, the economic performance of (1) current Light Water Reactors (LWR) once-through systems; (2) continuous plutonium recycling in Fast Reactors (FR) with driver and blanket; (3) Recycling of plutonium bred in FR into LWR. For each fuel cycle, the contributions to the total LCAE of the main cost components will be identified.« less
Process chemistry of americium-241
DOE Office of Scientific and Technical Information (OSTI.GOV)
Navratil, J.D.
1983-01-01
Americium-241, one of the most useful actinide isotopes, is produced as a by-product of plutonium scrap recovery operations. Rocky Flats has supplied high purity americium oxide to the US Department of Energy's Isotope Pool since 1962. Over the years, the evolving separation and purification processes have included such diverse operations as ion exchange, aqueous precipitation, and both molten-salt and organic-solvent extraction.
NASA Astrophysics Data System (ADS)
Ogorodnikov, B. I.
2018-06-01
The results of the physicochemical studies of radioactive aerosols inside and outside the Shelter construction at the Arch construction stage of the Chernobyl Nuclear Power Plant (ChNPP) in 2000-2015 were presented. The dominant isotopes were shown to be cesium, strontium, americium, plutonium, and uranium. They are carried by disperse particles of 2-7 μm. In subreactor rooms, in particular, 012/7, the composition of aerosols is affected by the erosion of the fuel-containing mass formed in 1986. Submicron cesium carrier aerosols appear as a result of evaporation and condensation during fires and welding works. Radiocesium is a well-soluble component of aerosols, while plutonium isotopes are not readily soluble components. In several rooms, the contents of radon, thoron, and their daughter products exceeded the permissible values. In April-June 2011, the intake of radionuclides from the accident at the Japanese Fukushima-1 NPP, which had AMAD of 0.5 μm, was detected and tracked using Petryanov multilayer filters. The productivity of filtration units under the dusty conditions in the exclusion zone of ChNPP and in fogs and haze was investigated. Hydrophilic prefilters with 7-10 μm fibers were recommended.
URANOUS IODATE AS A CARRIER FOR PLUTONIUM
Miller, D.R.; Seaborg, G.T.; Thompson, S.G.
1959-12-15
A process is described for precipitating plutonium on a uranous iodate carrier from an aqueous acid solution conA plutonium solution more concentrated than the original solution can then be obtained by oxidizing the uranium to the hexavalent state and dissolving the precipitate, after separating the latter from the original solution, by means of warm nitric acid.
PLUTONIUM-URANIUM-TITANIUM ALLOYS
Coffinberry, A.S.
1959-07-28
A plutonium-uranium alloy suitable for use as the fuel element in a fast breeder reactor is described. The alloy contains from 15 to 60 at.% titanium with the remainder uranium and plutonium in a specific ratio, thereby limiting the undesirable zeta phase and rendering the alloy relatively resistant to corrosion and giving it the essential characteristic of good mechanical workability.
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
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
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
DOE Office of Scientific and Technical Information (OSTI.GOV)
Conant, Andrew; Erickson, Anna; Robel, Martin
Nuclear forensics has a broad task to characterize recovered nuclear or radiological material and interpret the results of investigation. One approach to isotopic characterization of nuclear material obtained from a reactor is to chemically separate and perform isotopic measurements on the sample and verify the results with modeling of the sample history, for example, operation of a nuclear reactor. The major actinide plutonium and fission product cesium are commonly measured signatures of the fuel history in a reactor core. This study investigates the uncertainty of the plutonium and cesium isotope ratios of a fuel rod discharged from a research pressurizedmore » water reactor when the location of the sample is not known a priori. A sensitivity analysis showed overpredicted values for the 240Pu/ 239Pu ratio toward the axial center of the rod and revealed a lower probability of the rod of interest (ROI) being on the periphery of the assembly. The uncertainty analysis found the relative errors due to only the rod position and boron concentration to be 17% to 36% and 7% to 15% for the 240Pu/ 239Pu and 137Cs/ 135Cs ratios, respectively. Lastly, this study provides a method for uncertainty quantification of isotope concentrations due to the location of the ROI. Similar analyses can be performed to verify future chemical and isotopic analyses.« less
Conant, Andrew; Erickson, Anna; Robel, Martin; ...
2017-02-03
Nuclear forensics has a broad task to characterize recovered nuclear or radiological material and interpret the results of investigation. One approach to isotopic characterization of nuclear material obtained from a reactor is to chemically separate and perform isotopic measurements on the sample and verify the results with modeling of the sample history, for example, operation of a nuclear reactor. The major actinide plutonium and fission product cesium are commonly measured signatures of the fuel history in a reactor core. This study investigates the uncertainty of the plutonium and cesium isotope ratios of a fuel rod discharged from a research pressurizedmore » water reactor when the location of the sample is not known a priori. A sensitivity analysis showed overpredicted values for the 240Pu/ 239Pu ratio toward the axial center of the rod and revealed a lower probability of the rod of interest (ROI) being on the periphery of the assembly. The uncertainty analysis found the relative errors due to only the rod position and boron concentration to be 17% to 36% and 7% to 15% for the 240Pu/ 239Pu and 137Cs/ 135Cs ratios, respectively. Lastly, this study provides a method for uncertainty quantification of isotope concentrations due to the location of the ROI. Similar analyses can be performed to verify future chemical and isotopic analyses.« less
Comparison of actinide production in traveling wave and pressurized water reactors
DOE Office of Scientific and Technical Information (OSTI.GOV)
Osborne, A.G.; Smith, T.A.; Deinert, M.R.
The geopolitical problems associated with civilian nuclear energy production arise in part from the accumulation of transuranics in spent nuclear fuel. A traveling wave reactor is a type of breed-burn reactor that could, if feasible, reduce the overall production of transuranics. In one possible configuration, a cylinder of natural or depleted uranium would be subjected to a fast neutron flux at one end. The neutrons would transmute the uranium, producing plutonium and higher actinides. Under the right conditions, the reactor could become critical, at which point a self-stabilizing fission wave would form and propagate down the length of the reactormore » cylinder. The neutrons from the fission wave would burn the fissile nuclides and transmute uranium ahead of the wave to produce additional fuel. Fission waves in uranium are driven largely by the production and fission of {sup 239}Pu. Simulations have shown that the fuel burnup can reach values greater than 400 MWd/kgIHM, before fission products poison the reaction. In this work we compare the production of plutonium and minor actinides produced in a fission wave to that of a UOX fueled light water reactor, both on an energy normalized basis. The nuclide concentrations in the spent traveling wave reactor fuel are computed using a one-group diffusion model and are verified using Monte Carlo simulations. In the case of the pressurized water reactor, a multi-group collision probability model is used to generate the nuclide quantities. We find that the traveling wave reactor produces about 0.187 g/MWd/kgIHM of transuranics compared to 0.413 g/MWd/kgIHM for a pressurized water reactor running fuel enriched to 4.95 % and burned to 50 MWd/kgIHM. (authors)« less
PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINATING ELEMENTS
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.
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
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)
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.
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Napier, Bruce A.
2014-01-01
Beginning in 1948, the Soviet Union initiated a program for production of nuclear materials for a weapons program. The first facility for production of plutonium was constructed in the central portion of the country east of the southern Ural Mountains, about halfway between the major industrial cities of Ekaterinburg and Chelyabinsk. The facility now known as the Mayak Production Association and its associated town, now known as Ozersk, were built to irradiate uranium in reactors, separate the resulting plutonium in reprocessing plants, and prepare plutonium metal. The rush to production, coupled with inexperience in handling radioactive materials, lead to largemore » radiation exposures, not only to the workers in the facilities, but also to the surrounding public. Fuel processing started with no controls on releases, and fuel dissolution and accidents in reactors resulted in release of about 37 PBq (1015 Bq) of 131I between 1948 and 1967. Designed disposals of low- and intermediate-level liquid radioactive wastes, and accidental releases via cooling water from tank farms of high-level liquid radioactive wastes, into the small Techa River caused significant contamination and exposures to residents of numerous small riverside villages downstream of the site. Discovery of the magnitude of the aquatic contamination in late 1951 caused revisions to the waste handling regimes, but not before over 200 PBq of radionuclides (with large contributions of 90Sr and 137Cs) were released. Liquid wastes were diverted to tiny Lake Karachay (which today holds over 4 EBq); cooling water was stopped in the tank farms. In 1957, one of the tanks in the tank farm overheated and exploded; over 70 PBq, disproportionately 90Sr, was blown over a large area to the northeast of the site; a large area was contaminated and many villages evacuated. This area today is known as the East Urals Radioactive Trace (EURT). Each of these releases was significant; together they have created a group of cohorts unrivaled in the world for their chronic, low-dose-rate radiation exposure. The 26,000 workers at Mayak were highly exposed to external gamma and inhaled plutonium. A cohort of individuals raised as children in Ozersk is under evaluation for their exposures to radioiodine. The Techa River Cohort consists of over 30,000 people who were born before the start of exposure in 1949 and lived along the Techa River. The Techa River Offspring Cohort consists of about 21,000 persons born to one or more exposed parents of this group - many of whom also lived along the contaminated river. The EURT Cohort consists of about 18,000 people who were evacuated from the EURT soon after the 1957 explosion and another 8000 who remained. These groups together are the focus of dose reconstruction and epidemiological studies funded by the US, Russia, and the European Union to address the question “Are doses delivered at low dose rates as effective in producing health effects as the same doses delivered at high dose rates?”« less
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
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.
PLUTONIUM FUEL RODS FOR PREPARATION OF TRANSPLUTONIC ELEMENTS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bailey, W.J.
1962-02-01
Production by coextrusion of metallurgically bonded, Alclad, Al-7.35 wt% Pu alloy fuel rods with integral ends is discussed. The rods had a diameter of 0.94 in., length of, 60 in., and a nominal cladding thickness of 0.070 in. The Pu concentration was maintained at 83.3 g/rod. The coextrusion billets can be assembled with fuel cores in the as-cast condition. The casting hot-tops can be returned to the process stream. The process is useful for preparing transplutonic elements and production of high-exposure Pu. (J.R.D.)
NASA Astrophysics Data System (ADS)
Furukawa, Kazuo; Kato, Yoshio; Chigrinov, Sergey E.
1995-09-01
For practical/industrial disposition of Pu(TRU) by accelerator facility, not only physical soundness and safety but also the following technological rationality should be required: (1) few R&D items including radiation damage, heat removal and material compatibility: (2) few operation/maintenance/processing works; (3) few reproduction of radioactivity; (4) effective energy production in parallel. This will be achieved by the new modification of Th-fertilizing Single-Fluid type Accelerator Molten-Salt Breeder (AMSB), by which a global nuclear energy strategy for next century might be prepared.
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.