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.)

Industrial safety and applied health physics. Annual report for 1980

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

Not Available

1981-11-01

Information is reported in sections entitled: radiation monitoring; Environmental Management Program; radiation and safety surveys; industrial safety and special projects; Office of Operational Safety; and training, lectures, publications, and professional activities. There were no external or internal exposures to personnel which exceeded the standards for radiation protection as defined in DOE Manual Chapter 0524. Only 35 employees received whole body dose equivalents of 10 mSv (1 rem) or greater. There were no releases of gaseous waste from the Laboratory which were of a level that required an incident report to DOE. There were no releases of liquid radioactive waste frommore » the Laboratory which were of a level that required an incident report to DOE. The quantity of those radionuclides of primary concern in the Clinch River, based on the concentration measured at White Oak Dam and the dilution afforded by the Clinch River, averaged 0.16 percent of the concentration guide. The average background level at the Perimeter Air Monitoring (PAM) stations during 1980 was 9.0 ..mu..rad/h (0.090 ..mu..Gy/h). Soil samples were collected at all perimeter and remote monitoring stations and analyzed for eleven radionuclides including plutonium and uranium. Plutonium-239 content ranged from 0.37 Bq/kg (0.01 pCi/g) to 1.5 Bq/kg (0.04 pCi/g), and the uranium-235 content ranged from 0.7 Bq/kg (0.02 pCi/g) to 16 Bq/kg (0.43 pCi/g). Grass samples were collected at all perimeter and remote monitoring stations and analyzed for twelve radionuclides including plutonium and uranium. Plutonium-239 content ranged from 0.04 Bq/kg (0.001 pCi/g) to 0.07 Bq/kg (0.002 pCi/g), and the uranium-235 content ranged from 0.37 Bq/kg (0.01 pCi/g) to 12 Bq/kg (0.33 pCi/g).« less

Analysis of Tank 38H (HTF-38-16-80, 81) and Tank 43H (HTF-43-16-82, 83) Samples for Support of the Enrichment Control and Corrosion Control Programs

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

Hay, M.

2016-10-24

SRNL analyzed samples from Tank 38H and Tank 43H to support ECP and CCP. The total uranium in the Tank 38H surface sample was 57.6 mg/L, while the sub-surface sample was 106 mg/L. The Tank 43H samples ranged from 50.0 to 51.9 mg/L total uranium. The U-235 percentage was consistent for all four samples at 0.62%. The total uranium and percent U-235 results appear consistent with recent Tank 38H and Tank 43H uranium measurements. The Tank 38H plutonium results show a large difference between the surface and sub-surface sample concentrations and somewhat higher concentrations than previous samples. The Pu-238 concentrationmore » is more than forty times higher in the Tank 38H sub-surface sample than the surface sample. The surface and sub-surface Tank 43H samples contain similar plutonium concentrations and are within the range of values measured on previous samples. The four samples analyzed show silicon concentrations somewhat higher than the previous sample with values ranging from 104 to 213 mg/L.« less

Measurement of plutonium isotope ratios in nuclear fuel samples by HPLC-MC-ICP-MS

NASA Astrophysics Data System (ADS)

Günther-Leopold, I.; Waldis, J. Kobler; Wernli, B.; Kopajtic, Z.

2005-04-01

Radioactive isotopes are traditionally quantified by means of radioactivity counting techniques ([alpha], [beta], [gamma]). However, these methods often require extensive matrix separation and sample purification before the identification of specific isotopes and their relative abundance is possible as it is necessary in the frame of post-irradiation examinations on nuclear fuel samples. The technique of multicollector inductively coupled plasma mass spectrometry (MC-ICP-MS) is attracting much attention because it permits the precise measurement of the isotope compositions for a wide range of elements combined with excellent limits of detection due to high ionization efficiencies. The present paper describes one of the first applications of an online high-performance liquid chromatographic separation system coupled to a MC-ICP-MS in order to overcome isobaric interferences for the determination of the plutonium isotope composition and concentrations in irradiated nuclear fuels. The described chromatographic separation is sufficient to prevent any isobaric interference between 238Pu present at trace concentrations and 238U present as the main component of the fuel samples. The external reproducibility of the uncorrected plutonium isotope ratios was determined to be between 0.04 and 0.2% (2 s) resulting in a precision in the [per mille sign] range for the isotopic vectors of the irradiated fuel samples.

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

PubMed

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

2012-01-01

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

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

Theory of Positron Annihilation in Helium-Filled Bubbles in Plutonium

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

Sterne, P A; Pask, J E

2003-02-13

Positron annihilation lifetime spectroscopy is a sensitive probe of vacancies and voids in materials. This non-destructive measurement technique can identify the presence of specific defects in materials at the part-per-million level. Recent experiments by Asoka-Kumar et al. have identified two lifetime components in aged plutonium samples--a dominant lifetime component of around 182 ps and a longer lifetime component of around 350-400ps. This second component appears to increase with the age of the sample, and accounts for only about 5 percent of the total intensity in 35 year-old plutonium samples. First-principles calculations of positron lifetimes are now used extensively to guidemore » the interpretation of positron lifetime data. At Livermore, we have developed a first-principles finite-element-based method for calculating positron lifetimes for defects in metals. This method is capable of treating system cell sizes of several thousand atoms, allowing us to model defects in plutonium ranging in size from a mono-vacancy to helium-filled bubbles of over 1 nm in diameter. In order to identify the defects that account for the observed lifetime values, we have performed positron lifetime calculations for a set of vacancies, vacancy clusters, and helium-filled vacancy clusters in delta-plutonium. The calculations produced values of 143ps for defect-free delta-Pu and 255ps for a mono-vacancy in Pu, both of which are inconsistent with the dominant experimental lifetime component of 182ps. Larger vacancy clusters have even longer lifetimes. The observed positron lifetime is significantly shorter than the calculated lifetimes for mono-vacancies and larger vacancy clusters, indicating that open vacancy clusters are not the dominant defect in the aged plutonium samples. When helium atoms are introduced into the vacancy cluster, the positron lifetime is reduced due to the increased density of electrons available for annihilation. For a mono-vacancy in Pu containing one helium atom, the calculated lifetime is 190 ps, while a di-vacancy containing two helium atoms has a positron lifetime of 205 ps. In general, increasing the helium density in a vacancy cluster or He-filled bubble reduces the positron lifetime, so that the same lifetime value can arise fi-om a range of vacancy cluster sizes with different helium densities. In order to understand the variation of positron lifetime with vacancy cluster size and helium density in the defect, we have performed over 60 positron lifetime calculations with vacancy cluster sizes ranging from 1 to 55 vacancies and helium densities ranging fi-om zero to five helium atoms per vacancy. The results indicate that the experimental lifetime of 182 ps is consistent with the theoretical value of 190 ps for a mono-vacancy with a single helium atom, but that slightly better agreement is obtained for larger clusters of 6 or more vacancies containing 2-3 helium atoms per vacancy. For larger vacancy clusters with diameters of about 3-5 nm or more, the annihilation with helium electrons dominates the positron annihilation rate; the observed lifetime of 180ps is then consistent with a helium concentration in the range of 3 to 3.5 Hehacancy, setting an upper bound on the helium concentration in the vacancy clusters. In practice, the single lifetime component is most probably associated with a family of helium-filled bubbles rather than with a specific unique defect size. The longer 350-400ps lifetime component is consistent with a relatively narrow range of defect sizes and He concentration. At zero He concentration, the lifetime values are matched by small vacancy clusters containing 6-12 vacancies. With increasing vacancy cluster size, a small amount of He is required to keep the lifetime in the 350-400 ps range, until the value saturates for larger helium bubbles of more than 50 vacancies (bubble diameter > 1.3 nm) at a helium concentration close to 1 He/vacancy. These results, taken together with the experimental data, indicate that the features observed in TEM data by Schwartz et al are not voids, but are in fact helium-filled bubbles with a helium pressure of around 2-3 helium atoms per vacancy, depending on the bubble size. This is consistent with the conclusions of recently developed models of He-bubble growth in aged plutonium.« less

Effectiveness of sheltering in buildings and vehicles for plutonium

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

Engelmann, R.J.

1990-07-30

The purpose of this paper is to collect and present current knowledge relevant to the protection offered by sheltering against exposure to plutonium particles released to the atmosphere during accidents. For those many contaminants for which effects are linear with the airborne concentration, it is convenient to define a Dose Reduction Factor (DRF). In the past, the DRF has been defined as the ratio of the radiological dose that may be incurred within the shelter to that in the outdoors. As such, it includes the dose through shine from plumes aloft and from material deposited on the surface. For thismore » paper, which is concerned only with the inhalation pathway, the DRF is the ratio of the time-integrated concentration inside the shelter to that outdoors. It is important to note that the range over which effects are linear with concentration may be limited for many contaminants. Examples are when concentrations produce effects that are irreversible, or when concentrations are below effects threshold levels. 71 refs., 4 figs., 8 tabs.« less

PLUTONIUM CLEANING PROCESS

DOEpatents

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

DOEpatents

Garner, C.S.

1959-01-13

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

Plutonium and cesium baseline concentrations in seawater from northern Arabian Gulf.

PubMed

Uddin, S; Aba, A; Behbehani, M; Al-Ghadban, A N; Al-Zekri, W; Al-Shammari, H

2017-07-15

The Arabian Gulf is a semi-enclosed water body that has witnessed accelerated anthropogenic activity, in terms of commissioning of nuclear power plants, desalination facilities, oil refineries and extensive coastal development. Furthermore, three wars during the past three decades is a potential worry. This study presents the first plutonium baseline in seawater from the Northern Arabian Gulf. The 239+240 Pu concentrations in seawater vary, between 2.9 and 4.9mBqm -3 , a range that is comparable to other water masses at this latitude. The 238 Pu ranged between 0.04 and 0.05mBqm -3 and the 137 Cs concentration between 1.04 and 1.18Bqm -3 . The ratio of 238 Pu/ 239+240 Pu at all eight sampling stations was 0.01, while the ratio of 239+240 Pu/ 137 Cs varied between 0.01 and 0.02. The presence of 137 Cs and 239+240 Pu in seawater from this region can mainly be attributed to the global atmospheric deposition and fluvial transport. The seawater concentration of 239+240 Pu is five order of magnitude lower than bottom sediments in the area. Copyright © 2017 Elsevier Ltd. All rights reserved.

Plutonium isotopes in the Hungarian environment.

PubMed

Varga, Beata; Tarján, Sandor; Vajda, Nora

2008-04-01

More than 50 soil samples were analysed from different parts of the country, the activity concentration of 239+240Pu was in the range of 0.01-0.84 Bq/kg dry soil with the average of 0.10 Bq/kg. 238Pu could be detected only in few moss samples and 238Pu/239+240Pu ratio determines the origin of plutonium. 241Pu was determined by liquid scintillation spectrometry. The activity concentration of this isotope in the soil is between 0.04 and 3.74 Bq/kg with the average of 0.82 Bq/kg, while in the moss is also similar 0.01-2.07 Bq/kg fresh mass with the average of 0.43 Bq/kg. Significant difference could not be observed between the different types of soils occurring in the country, but the results could be sorted according to the sampling carried out on undisturbed or cultivated area. The isotope ratios 241Pu/239+240Pu prove that the origin of the plutonium in Hungary is the global fallout determined by the atmospheric nuclear weapon tests.

Fuel bundle design for enhanced usage of plutonium fuel

DOEpatents

Reese, Anthony P.; Stachowski, Russell E.

1995-01-01

A nuclear fuel bundle includes a square array of fuel rods each having a concentration of enriched uranium and plutonium. Each rod of an interior array of the rods also has a concentration of gadolinium. The interior array of rods is surrounded by an exterior array of rods void of gadolinium. By this design, usage of plutonium in the nuclear reactor is enhanced.

Fuel bundle design for enhanced usage of plutonium fuel

DOEpatents

Reese, A.P.; Stachowski, R.E.

1995-08-08

A nuclear fuel bundle includes a square array of fuel rods each having a concentration of enriched uranium and plutonium. Each rod of an interior array of the rods also has a concentration of gadolinium. The interior array of rods is surrounded by an exterior array of rods void of gadolinium. By this design, usage of plutonium in the nuclear reactor is enhanced. 10 figs.

SEPARATION OF PLUTONIUM

DOEpatents

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.

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

PubMed

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

2008-04-01

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

PLUTONIUM-CERIUM-COBALT AND PLUTONIUM-CERIUM-NICKEL ALLOYS

DOEpatents

Coffinberry, A.S.

1959-08-25

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

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

PubMed

Donard, O F X; Bruneau, F; Moldovan, M; Garraud, H; Epov, V N; Boust, D

2007-03-28

Among the transuranic elements present in the environment, plutonium isotopes are mainly attached to particles, and therefore they present a great interest for the study and modelling of particle transport in the marine environment. Except in the close vicinity of industrial sources, plutonium concentration in marine sediments is very low (from 10(-4) ng kg(-1) for (241)Pu to 10 ng kg(-1) for (239)Pu), and therefore the measurement of (238)Pu, (239)Pu, (240)Pu, (241)Pu and (242)Pu in sediments at such concentration level requires the use of very sensitive techniques. Moreover, sediment matrix contains huge amounts of mineral species, uranium and organic substances that must be removed before the determination of plutonium isotopes. Hence, an efficient sample preparation step is necessary prior to analysis. Within this work, a chemical procedure for the extraction, purification and pre-concentration of plutonium from marine sediments prior to sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS) analysis has been optimized. The analytical method developed yields a pre-concentrated solution of plutonium from which (238)U and (241)Am have been removed, and which is suitable for the direct and simultaneous measurement of (239)Pu, (240)Pu, (241)Pu and (242)Pu by SF-ICP-MS.

Plutonium segregation in glassy aerodynamic fallout from a nuclear weapon test

DOE PAGES

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

2017-01-11

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

SEPARATION OF PLUTONIUM HYDROXIDE FROM BISMUTH HYDROXIDE

DOEpatents

Watt, G.W.

1958-08-19

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

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

PubMed

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

2018-05-04

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

SEPARATION OF PLUTONIUM FROM AQUEOUS SOLUTIONS BY ION-EXCHANGE

DOEpatents

Schubert, J.

1958-06-01

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

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

DOEpatents

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

1960-08-23

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

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

DOEpatents

Krot, Nikolai N.; Charushnikova, Iraida A.

1997-01-01

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

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

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

DOEpatents

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

1957-10-29

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

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

USGS Publications Warehouse

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

1988-01-01

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

Soil plutonium and cesium in stream channels and banks of Los Alamos liquid effluent-receiving areas.

PubMed

Nyhan, J W; White, G C; Trujillo, G

1982-10-01

Stream channel sediments and adjacent bank soils found in three intermittent streams used for treated liquid effluent disposal at Los Alamos, New Mexico were sampled to determine the distribution of 238Pu, 239,240Pu and 137Cs. Radionuclide concentrations and inventories were determined as functions of distance downstream from the waste outfall and from the center of the stream channel, soil sampling depth, stream channel-bank physiography, and the waste use history of each disposal area. Radionuclide concentrations in channel sediments were inversely related to distances up to 10 km downstream from the outfalls. For sites receiving appreciable waste effluent additions, contaminant concentrations in bank soils decreased with perpendicular distances greater than 0.38 m from the stream channel, and with stream bank sampling depths greater than 20-40 cm. Concentrations and total inventories of radionuclides in stream bank soils generally decreased as stream bank height increased. Inventory estimates of radionuclides in channel sediments exhibited coefficients of variation that ranged 0.41-2.6, reflecting the large variation in radionuclide concentrations at each site. Several interesting temporal relationships of these radionuclides in intermittent streams were gleaned from the varying waste use histories of the three effluent-receiving areas. Eleven yr after liquid wastes were added to one canyon, the major radionuclide inventories were found in the stream bank soils, unlike most of the other currently-used receiving areas. A period of time greater than 6 yr seems to be required before the plutonium in liquid wastes currently added to the canyon is approximately equilibrated with the plutonium in the bank soils. These observations are discussed relative to waste management practices in these southwestern intermittent streams.

Radionuclides in ground water at the Idaho National Engineering Laboratory, Idaho

USGS Publications Warehouse

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)

Environmental monitoring at Mound: 1986 report

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

Carfagno, D.G.; Farmer, B.M.

1987-05-11

The local environment around Mound was monitored for tritium and plutonium-238. The results are reported for 1986. Environmental media analyzed included air, water, vegetation, foodstuffs, and sediment. The average concentrations of plutonium-238 and tritium were within the DOE interim air and water Derived Concentration Guides (DCG) for these radionuclides. The average incremental concentrations of plutonium-238 and tritium oxide in air measured at all offsite locations during 1986 were 0.03% and 0.01%, respectively, of the DOE DCGs for uncontrolled areas. The average incremental concentration of plutonium-238 measured at all locations in the Great Miami River during 1986 was 0.0005% of themore » DOE DCG. The average incremental concentration of tritium measured at all locations in the Great Miami River during 1986 was 0.005% of the DOE DCG. The average incremental concentrations of plutonium-238 found during 1986 in surface and area drinking water were less than 0.00006% of the DOE DCG. The average incremental concentration of tritium in surface water was less than 0.005% of the DOE DCG. All tritium in drinking water data is compared to the US EPA Drinking Water Standard. The average concentrations in local private and municipal drinking water systems were less than 25% and 1.5%, respectively. Although no DOE DCG is available for foodstuffs, the average concentrations are a small fraction of the water DCG (0.04%). The concentrations of sediment samples obtained at offsite surface water sampling locations were extremely low and therefore represent no adverse impact to the environment. The dose equivalent estimates for the average air, water, and foodstuff concentrations indicate that the levels are within 1% of the DOE standard of 100 mrem. None of these exceptions, however, had an adverse impact on the water quality of the Great Miami River or caused the river to exceed Ohio Stream Standards. 20 refs., 5 figs., 31 tabs.« less

URANOUS IODATE AS A CARRIER FOR PLUTONIUM

DOEpatents

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

1959-12-15

A process is described for precipitating plutonium on a uranous iodate carrier from an aqueous acid solution conA plutonium solution more concentrated than the original solution can then be obtained by oxidizing the uranium to the hexavalent state and dissolving the precipitate, after separating the latter from the original solution, by means of warm nitric acid.

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

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

Brown, K.W.

1979-03-01

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

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

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

Morales-Arteaga, Maria

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

CONCENTRATION OF Pu USING AN IODATE PRECIPITATE

DOEpatents

Fries, B.A.

1960-02-23

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

IMPROVED PROCESS OF PLUTONIUM CARRIER PRECIPITATION

DOEpatents

Faris, B.F.

1959-06-30

This patent relates to an improvement in the bismuth phosphate process for separating and recovering plutonium from neutron irradiated uranium, resulting in improved decontamination even without the use of scavenging precipitates in the by-product precipitation step and subsequently more complete recovery of the plutonium in the product precipitation step. This improvement is achieved by addition of fluomolybdic acid, or a water soluble fluomolybdate, such as the ammonium, sodium, or potassium salt thereof, to the aqueous nitric acid solution containing tetravalent plutonium ions and contaminating fission products, so as to establish a fluomolybdate ion concentration of about 0.05 M. The solution is then treated to form the bismuth phosphate plutonium carrying precipitate.

Concentration and purification of plutonium or thorium

DOEpatents

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.

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

METHOD OF DISSOLVING MASSIVE PLUTONIUM

DOEpatents

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

1960-06-28

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

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

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

Delegard, Calvin H.; Schmitt, Bruce E.; Schmidt, Andrew J.

2006-08-01

This report establishes the technical bases for using a ''slow uptake'' instead of a ''moderate uptake'' transportability class for americium-241 (241Am) for the K Basin Sludge Treatment Project (STP) dose consequence analysis. Slow uptake classes are used for most uranium and plutonium oxides. A moderate uptake class has been used in prior STP analyses for 241Am based on the properties of separated 241Am and its associated oxide. However, when 241Am exists as an ingrown progeny (and as a small mass fraction) within plutonium mixtures, it is appropriate to assign transportability factors of the predominant plutonium mixtures (typically slow) to themore » Am241. It is argued that the transportability factor for 241Am in sludge likewise should be slow because it exists as a small mass fraction as the ingrown progeny within the uranium oxide in sludge. In this report, the transportability class assignment for 241Am is underpinned with radiochemical characterization data on K Basin sludge and with studies conducted with other irradiated fuel exposed to elevated temperatures and conditions similar to the STP. Key findings and conclusions from evaluation of the characterization data and published literature are summarized here. Plutonium and 241Am make up very small fractions of the uranium within the K Basin sludge matrix. Plutonium is present at about 1 atom per 500 atoms of uranium and 241Am at about 1 atom per 19000 of uranium. Plutonium and americium are found to remain with uranium in the solid phase in all of the {approx}60 samples taken and analyzed from various sources of K Basin sludge. The uranium-specific concentrations of plutonium and americium also remain approximately constant over a uranium concentration range (in the dry sludge solids) from 0.2 to 94 wt%, a factor of {approx}460. This invariability demonstrates that 241Am does not partition from the uranium or plutonium fraction for any characterized sludge matrix. Most of the K Basin sludge characterization data is derived spent nuclear fuel corroded within the K Basins at 10-15?C. The STP process will place water-laden sludges from the K Basin in process vessels at {approx}150-180 C. Therefore, published studies with other irradiated (uranium oxide) fuel were examined. From these studies, the affinity of plutonium and americium for uranium in irradiated UO2 also was demonstrated at hydrothermal conditions (150 C anoxic liquid water) approaching those proposed for the STP process and even for hydrothermal conditions outside of the STP operating envelope (e.g., 150 C oxic and 100 C oxic and anoxic liquid water). In summary, by demonstrating that the chemical and physical behavior of 241Am in the sludge matrix is similar to that of the predominant species (uranium and for the plutonium from which it originates), a technical basis is provided for using the slow uptake transportability factor for 241Am that is currently used for plutonium and uranium oxides. The change from moderate to slow uptake for 241Am could reduce the overall analyzed dose consequences for the STP by more than 30%.« less

Environmental monitoring at Mound: 1987 report

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

Carfagno, D.G.; Farmer, B.M.

1988-04-25

The local environment around Mound as monitored primarily for tritium and plutonium-238. The results are reported for 1987. Environmental media analyzed included air, water, vegetation, food-stuffs, and sediment. The average concentrations of plutonium 238 and tritium were within the DOE interim air and water Derived Concentration Guides (DCG) for these radionuclides. The average incremental concentrations of plutonium-238 and tritium oxide in air measured at all offsite locations during 1987 were 4.6 x 10/sup -18/ ..mu..Ci/mL and 12.9 x 10/sup -12/ ..mu..Ci/mL, respectively. These correspond to 0.02% and 0.01%, respectively, of the DOE DCGs for uncontrolled areas. The average incremental concentrationmore » of plutonium-238 measured at all locations in the Great Miami River during 1987 was 1.4 x 10/sup - 12/ ..mu..Ci/mL which is 0.0004% of the DOE DCG. The average incremental concentration of tritium measured at all locations in the Great Miami River during 1987 was 0.07 x 10/sup -6/ ..mu..Ci/mL which is 0.004% of the DOE DCG. The dose equivalent estimates for the average air, water, and foodstuff concentrations indicate that the levels are 1% of the DOE standard of 100 mrem. 23 refs., 5 figs., 34 tabs.« less

DELTA PHASE PLUTONIUM ALLOYS

DOEpatents

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

1960-03-22

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

Experimental Methods to Estimate Accumulated Solids in Nuclear Waste Tanks - 13313

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

Duignan, Mark R.; Steeper, Timothy J.; Steimke, John L.

2013-07-01

The Department of Energy has a large number of nuclear waste tanks. It is important to know if fissionable materials can concentrate when waste is transferred from staging tanks prior to feeding waste treatment plants. Specifically, there is a concern that large, dense particles, e.g., plutonium containing, could accumulate in poorly mixed regions of a blend tank heel for tanks that employ mixing jet pumps. At the request of the DOE Hanford Tank Operations Contractor, Washington River Protection Solutions, the Engineering Development Laboratory of the Savannah River National Laboratory performed a scouting study in a 1/22-scale model of a wastemore » tank to investigate this concern and to develop measurement techniques that could be applied in a more extensive study at a larger scale. Simulated waste tank solids and supernatant were charged to the test tank and rotating liquid jets were used to remove most of the solids. Then the volume and shape of the residual solids and the spatial concentration profiles for the surrogate for plutonium were measured. This paper discusses the overall test results, which indicated heavy solids only accumulate during the first few transfer cycles, along with the techniques and equipment designed and employed in the test. Those techniques include: - Magnetic particle separator to remove stainless steel solids, the plutonium surrogate from a flowing stream. - Magnetic wand used to manually remove stainless steel solids from samples and the tank heel. - Photographs were used to determine the volume and shape of the solids mounds by developing a composite of topographical areas. - Laser range finders to determine the volume and shape of the solids mounds. - Core sampler to determine the stainless steel solids distribution within the solids mounds. - Computer driven positioner that placed the laser range finders and the core sampler over solids mounds that accumulated on the bottom of a scaled staging tank in locations where jet velocities were low. These devices and techniques were very effective to estimate the movement, location, and concentrations of the solids representing plutonium and are expected to perform well at a larger scale. The operation of the techniques and their measurement accuracies will be discussed as well as the overall results of the accumulated solids test. (authors)« less

SEPARATION OF PLUTONIUM FROM FISSION PRODUCTS BY A COLLOID REMOVAL PROCESS

DOEpatents

Schubert, J.

1960-05-24

A method is given for separating plutonium from uranium fission products. An acidic aqueous solution containing plutonium and uranium fission products is subjected to a process for separating ionic values from colloidal matter suspended therein while the pH of the solution is maintained between 0 and 4. Certain of the fission products, and in particular, zirconium, niobium, lanthanum, and barium are in a colloidal state within this pH range, while plutonium remains in an ionic form, Dialysis, ultracontrifugation, and ultrafiltration are suitable methods of separating plutonium ions from the colloids.

Measurements of actinides in soil, sediments, water and vegetation in Northern New Mexico

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

Gallaher, B. M.; Efurd, D. W.

2002-01-01

This study was undertaken during 1991 - 1998 to identify the origin of plutonium uranium in northern New Mexico Rio Grande and tributary stream sediments. Isotopic fingerprinting techniques help distinguish radioactivity from Los Alamos National Laboratory (LANL) and from global fallout or natural sources. The geographic area covered by the study extended from the headwaters of the Rio Grande in southern Colorado to Elephant Butte Reservoir in southern New Mexico. Over 100 samples of stream channel and reservoir bottom sediments were analyzed for the atom ratios of plutonium and uranium isotopes using thermal ionization mass spectrometry (TIMS). Comparison of thesemore » ratios against those for fallout or natural sources allowed for quantification of the Laboratory impact. Of the seven major drainages crossing LANL, movement of LANL plutonium into the Rio Grande can only be traced via Los Alamos Canyon. The majority of sampled locations within and adjacent to LANL have little or no input of plutonium from the Laboratory. Samples collected upstream and distant to L A N show an average (+ s.d.) fallout 240Pu/239Pauto m ratio of 0.169 + 0.012, consistent with published worldwide global fallout values. These regional background ratios differ significantly from the 240Pu/239Pu atom ratio of 0.015 that is representative of LANL-derived plutonium entering the Rio Grande at Los Alamos Canyon. Mixing calculations of these sources indicate that the largest proportion (60% to 90%) of the plutonium in the Rio Grande sediments is from global atmospheric fallout, with an average of about 25% from the Laboratory. The LANL plutonium is identifiable intermittently along the 35-km reach of the Rio Grande to Cochiti Reservoir. The source of the LANL-derived plutonium in the Rio Grande was traced primarily to pre-1960 discharges of liquid effluents into a canyon bottom at a distance approximately 20 km upstream of the river. Plutonium levels decline exponentially with distance downstream after mixing with cleaner sediments, yet the LANL isotopic fingerprint remains distinct for at least 55 km from the effluent source. Plutonium isotopes in Rio Grande and Pajarito Plateau sediments are not at levels known to adversely affect public health. Activities of 239+240pwui thin this sample set ranged from 0.001- 0.046 pCUg in the Rio Grande to 3.7 pCi/g near the effluent discharge point. Levels in the Rio Grande are usually more than 1000 times. lower than prescribed cleanup standards. Uranium in stream and reservoir sediments is predominantly within natural concentration ranges and is of natural uranium isotopic composition. None of the sediments from the Rio Grande show identifiable Laboratory uranium, using the isotopic ratios. These results suggest that the mass of Laboratory-derived uranium entering the Rio Grande is small relative to the natural load carried with river sediments.« less

METHOD FOR OBTAINING PLUTONIUM METAL FROM ITS TRICHLORIDE

DOEpatents

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

1962-08-14

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

Evaluation of continuous air monitor placement in a plutonium facility.

PubMed

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

1997-05-01

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

Analysis of tank 38H (HTF-38-17-18, -19) and tank 43H (HTF-43-17-20, -21) samples for support of the enrichment control and corrosion control programs

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

Hay, M. S.; Coleman, C. J.; Diprete, D. P.

SRNL analyzed samples from Tank 38H and Tank 43H to support ECP and CCP. The total uranium in the Tank 38H samples ranged from 53.7 mg/L for the surface sample to 57.0 mg/L in the sub-surface sample. The Tank 43H samples showed uranium concentrations of 46.2 mg/L for the surface sample and 45.7 mg/L in the sub-surface sample. The U-235 percentage was 0.63% in the Tank 38H samples and 0.62% in the Tank 43H samples. The total uranium and percent U-235 results appear consistent with recent Tank 38H and Tank 43H uranium measurements. The plutonium results for the Tank 38Hmore » surface sample are slightly higher than recent sample results, while the Tank 43H plutonium results are within the range of values measured on previous samples. The Cs-137 results for the Tank 38H surface and subsurface samples are slightly higher than the concentrations measured in recent samples. The Cs-137 results for the two Tank 43H samples are within the range of values measured on previous samples. The comparison of the sum of the cations in each sample versus the sum of the anions shows a difference of 23% for the Tank 38H surface sample and 18% for the Tank 43H surface sample. The four samples show silicon concentrations somewhat lower than the previous samples with values ranging from 80.2 to 105 mg/L.« less

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

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

None, None

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

RECOVERY OF Pu VALUES BY FLUORINATION AND FRACTIONATION

DOEpatents

Brown, H.S.; Webster, D.S.

1959-01-20

A method is presented for the concentration and recovery of plutonium by fluorination and fractionation. A metallic mass containing uranium and plutonium is heated to 250 C and contacted with a stream of elemental fluorine. After fluorination of the metallic mass, the rcaction products are withdrawn and subjected to a distillation treatment to separate the fluorination products of uranium and to obtain a residue containing the fluorination products of plutonium.

PROCESS FOR EXTRACTING NEPTUNIUM AND PLUTONIUM FROM NITRIC ACID SOLUTIONS OF SAME CONTAINING URANYL NITRATE WITH A TERTIARY AMINE

DOEpatents

Sheppard, J.C.

1962-07-31

A process of selectively extracting plutonium nitrate and neptunium nitrate with an organic solution of a tertiary amine, away from uranyl nitrate present in an aqueous solution in a maximum concentration of 1M is described. The nitric acid concentration is adjusted to about 4M and nitrous acid is added prior to extraction. (AEC)

Sources of plutonium in the atmosphere and stratosphere-troposphere mixing

PubMed Central

Hirose, Katsumi; Povinec, Pavel P.

2015-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

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

PubMed

Skipperud, Lindis

2004-06-18

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

Actinides in deer tissues at the rocky flats environmental technology site.

PubMed

Todd, Andrew S; Sattelberg, R Mark

2005-11-01

Limited hunting of deer at the future Rocky Flats National Wildlife Refuge has been proposed in U.S. Fish and Wildlife planning documents as a compatible wildlife-dependent public use. Historically, Rocky Flats site activities resulted in the contamination of surface environmental media with actinides, including isotopes of americium, plutonium, and uranium. In this study, measurements of actinides [Americium-241 (241Am); Plutonium-238 (238Pu); Plutonium-239,240 (239,240Pu); uranium-233,244 (233,234U); uranium-235,236 (235,236U); and uranium-238 (238U)] were completed on select liver, muscle, lung, bone, and kidney tissue samples harvested from resident Rocky Flats deer (N = 26) and control deer (N = 1). In total, only 17 of the more than 450 individual isotopic analyses conducted on Rocky Flats deer tissue samples measured actinide concentrations above method detection limits. Of these 17 detects, only 2 analyses, with analytical uncertainty values added, exceeded threshold values calculated around a 1 x 10(-6) risk level (isotopic americium, 0.01 pCi/g; isotopic plutonium, 0.02 pCi/g; isotopic uranium, 0.2 pCi/g). Subsequent, conservative risk calculations suggest minimal human risk associated with ingestion of these edible deer tissues. The maximum calculated risk level in this study (4.73 x 10(-6)) is at the low end of the U.S. Environmental Protection Agency's acceptable risk range.

Heterogeneity Effects in Plutonium Contaminated Soil

DTIC Science & Technology

2009-03-01

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

CARBONATE METHOD OF SEPARATION OF TETRAVALENT PLUTONIUM FROM FISSION PRODUCT VALUES

DOEpatents

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

1959-02-01

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

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

DOEpatents

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

1962-07-10

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

Whole-Organism Concentration Ratios for Plutonium in Wildlife from Past US Nuclear Research Data

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

johansen, M.; Kamboj; Kuhne, W.

Whole-organism concentration ratios (CR{sub wo-media}) for plutonium (Pu) in wildlife were calculated using data from the broad range of organism types and environmental settings of the US nuclear research program. Original sources included site-specific reports and scientific journal articles typically from 1960s to 80s research. Most of the calculated CR{sub wo-media} values are new to existing data sets, and, for some wildlife categories, serve to fill gaps or add to sparse data including those for terrestrial reptile; freshwater bird, crustacean and zooplankton; and marine crustacean and zooplankton. Ratios of Pu concentration in the whole-organism to that in specific tissues andmore » organs are provided here for a range of freshwater and marine fish. The CR{sub wo-media} values in fish living in liquid discharge ponds were two orders of magnitude higher than those for similar species living in lakes receiving Pu from atmospheric fallout, suggesting the physico-chemical form of the source Pu can dominate over other factors related to transfer, such as organism size and feeding behavior. Small rodent data indicated one to two order of magnitude increases when carcass, pelt, and gastrointestinal tract were included together in the whole-organism calculation compared to that for carcass alone. Only 4% of Pu resided in the carcass of small rodents compared to 75% in the gastrointestinal tract and 21% in the pelt.« less

Americium, plutonium and uranium contamination and speciation in well waters, streams and atomic lakes in the Sarzhal region of the Semipalatinsk Nuclear Test Site, Kazakhstan.

PubMed

León Vintró, L; Mitchell, P I; Omarova, A; Burkitbayev, M; Jiménez Nápoles, H; Priest, N D

2009-04-01

New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel'kem 1 and Tel'kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that (241)Am, (239,240)Pu and (238)U concentrations in well waters within the study area are in the range 0.04-87mBq dm(-3), 0.7-99mBq dm(-3), and 74-213mBq dm(-3), respectively, and for (241)Am and (239,240)Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01mBq dm(-3), 0.08mBq dm(-3) and 0.32mBq dm(-3) for (241)Am, (239,240)Pu and (238)U, respectively. The (235)U/(238)U isotopic ratio in almost all well and stream waters is slightly elevated above the 'best estimate' value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53-85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11-42microSv (mean 21microSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel'kem explosions.

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

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

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

1992-12-31

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

Plutonium dissolution process

DOEpatents

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

1996-01-01

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

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

PubMed

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

2008-10-01

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

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.

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

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

PubMed

Priest, N D; Hunt, B W

1979-05-01

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

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

PubMed

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

2002-01-01

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

Determining the release of radionuclides from tank waste residual solids. FY2015 report

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

King, William D.; Hobbs, David T.

Methodology development for pore water leaching studies has been continued to support Savannah River Site High Level Waste tank closure efforts. For FY2015, the primary goal of this testing was the achievement of target pH and Eh values for pore water solutions representative of local groundwater in the presence of grout or grout-representative (CaCO 3 or FeS) solids as well as waste surrogate solids representative of residual solids expected to be present in a closed tank. For oxidizing conditions representative of a closed tank after aging, a focus was placed on using solid phases believed to be controlling pH andmore » E h at equilibrium conditions. For three pore water conditions (shown below), the target pH values were achieved to within 0.5 pH units. Tank 18 residual surrogate solids leaching studies were conducted over an E h range of approximately 630 mV. Significantly higher Eh values were achieved for the oxidizing conditions (ORII and ORIII) than were previously observed. For the ORII condition, the target Eh value was nearly achieved (within 50 mV). However, E h values observed for the ORIII condition were approximately 160 mV less positive than the target. E h values observed for the RRII condition were approximately 370 mV less negative than the target. Achievement of more positive and more negative E h values is believed to require the addition of non-representative oxidants and reductants, respectively. Plutonium and uranium concentrations measured during Tank 18 residual surrogate solids leaching studies under these conditions (shown below) followed the general trends predicted for plutonium and uranium oxide phases, assuming equilibrium with dissolved oxygen. The highest plutonium and uranium concentrations were observed for the ORIII condition and the lowest concentrations were observed for the RRII condition. Based on these results, it is recommended that these test methodologies be used to conduct leaching studies with actual Tank 18 residual solids material. Actual waste testing will include leaching evaluations of technetium and neptunium, as well as plutonium and uranium.« less

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

NASA Astrophysics Data System (ADS)

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

2013-10-01

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

Plutonium release from the 903 pad at Rocky Flats.

PubMed

Mongan, T R; Ripple, S R; Winges, K D

1996-10-01

The Colorado Department of Public Health and Environment (CDH) sponsored a study to reconstruct contaminant doses to the public from operations at the Rocky Flats nuclear weapons plant. This analysis of the accidental release of plutonium from the area known as the 903 Pad is part of the CDH study. In the 1950's and 1960's, 55-gallon drums of waste oil contaminated with plutonium, and uranium were stored outdoors at the 903 Pad. The drums corroded, leaking contaminated oil onto soil subsequently carried off-site by the wind. The plutonium release is estimated using environmental data from the 1960's and 1970's and an atmospheric transport model for fugitive dust. The best estimate of total plutonium release to areas beyond plant-owned property is about 0.26 TBq (7 Ci). Off-site airborne concentrations and deposition of plutonium are estimated for dose calculation purposes. The best estimate of the highest predicted off-site effective dose is approximately 72 microSv (7.2 mrem).

Method for dissolving delta-phase plutonium

DOEpatents

Karraker, David G.

1992-01-01

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

Raman spectroscopy characterization of actinide oxides (U 1-yPu y)O 2: Resistance to oxidation by the laser beam and examination of defects

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.

A rapid method for quantification of 242Pu in urine using extraction chromatography and ICP-MS

DOE PAGES

Gallardo, Athena Marie; Than, Chit; Wong, Carolyn; ...

2017-01-01

Occupational exposure to plutonium is generally monitored through analysis of urine samples. Typically, plutonium is separated from the sample and other actinides, and the concentration is determined using alpha spectroscopy. Current methods for separations and analysis are lengthy and require long count times. A new method for monitoring occupational exposure levels of plutonium has been developed, which requires fewer steps and overall less time than the alpha spectroscopy method. In this method, the urine is acidified, and a 239Pu internal standard is added. The urine is digested in a microwave oven, and plutonium is separated using an Eichrom TRU Resinmore » column. The plutonium is eluted, and the eluant is injected directly into the Inductively Coupled Plasma–Mass Spectrometer (ICP-MS). Compared to a direct “dilute and shoot” method, a 30-fold improvement in sensitivity is achieved. This method was validated by analyzing several batches of spiked samples. Based on these analyses, a combined standard uncertainty plot, which relates uncertainty to concentration, was produced. As a result, the MDA 95 was calculated to be 7.0 × 10 –7 μg L –1, and the Lc95 was calculated to be 3.5 × 10 –7 μg L –1 for this method.« less

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

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

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

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

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

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

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

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

Determination of Plutonium Isotope Ratios at Very Low Levels by ICP-MS using On-Line Electrochemically Modulated Separations

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

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

NASA Astrophysics Data System (ADS)

Fisenko, Anatoliy I.; Lemberg, Vladimir F.

2016-09-01

The knowledge of thermal radiative and thermodynamic properties of uranium and plutonium carbides under extreme conditions is essential for designing a new metallic fuel materials for next generation of a nuclear reactor. The present work is devoted to the study of the thermal radiative and thermodynamic properties of liquid and solid uranium and plutonium carbides at their melting/freezing temperatures. The Stefan-Boltzmann law, total energy density, number density of photons, Helmholtz free energy density, internal energy density, enthalpy density, entropy density, heat capacity at constant volume, pressure, and normal total emissivity are calculated using experimental data for the frequency dependence of the normal spectral emissivity of liquid and solid uranium and plutonium carbides in the visible-near infrared range. It is shown that the thermal radiative and thermodynamic functions of uranium carbide have a slight difference during liquid-to-solid transition. Unlike UC, such a difference between these functions have not been established for plutonium carbide. The calculated values for the normal total emissivity of uranium and plutonium carbides at their melting temperatures is in good agreement with experimental data. The obtained results allow to calculate the thermal radiative and thermodynamic properties of liquid and solid uranium and plutonium carbides for any size of samples. Based on the model of Hagen-Rubens and the Wiedemann-Franz law, a new method to determine the thermal conductivity of metals and carbides at the melting points is proposed.

Fission- and alpha-track study of biogeochemistry of plutonium and uranium in carbonates of bikini and enewetak atolls. Final report

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

Levy, Y.; Friedman, G. M.; Miller, D. S.

1978-12-31

Results of the analysis of uranium concentrations in the 8 coral heads sampled from the Bikini and Enewetak lagoons lead to the following conclusions: (1) no parallel increase in uranium concentration was found in the corals contaminated by Pu and Am; (2) in the noncontaminated corals, the fission track analysis shows wider ranges of uranium concentrations (1.8 to 3.1). Thus, in the corals not contaminated by Pu and Am, uranium concentrations similar to the uranium concentration in the contaminated corals were found; (3) uranium content in all corals analyzed was rather homogeneously distributed, i.e., no hot spots, stars, or areasmore » differing in concentration by more than a few percent were detected by the fission track analyses.« less

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

PubMed

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

1997-01-01

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

Plutonium and uranium in human bones from areas surrounding the Semipalatinsk nuclear test site.

PubMed

Yamamoto, Masayoshi; Hoshi, Masaharu; Sakaguchi, Aya; Shinohara, Kunihiko; Kurihara, Osamu; Apsalikov, Kazbek N; Gusev, Boris I

2006-02-01

To evaluate the present levels of 239,240Pu and U in residents living near the Semipalatinsk nuclear test site, more than 70 bone samples were obtained at autopsy. The subjects ranged in age from 30 to 86 years (mean 59.3+/-12.9). Most of the samples consisted of victims who died of various diseases. Plutonium and U were radiochemically separated and determined by alpha-ray spectrometry. The mean concentrations of 239,240Pu and 238U observed were 0.050+/-0.041 mBq/g-ash (vertebrae 71, long-bones 18) and 0.28+/-0.13 mBq/g-ash (22.8+/-10.6 microg U/kg-ash) (vertebrae 58, long bones 16), respectively. The present 239,240Pu levels were within the range found for human bone samples from other countries due solely to global fallout in the early 1980s. The average U concentration was close to the estimate (mean 22.5 microg U/kg-ash) for the UK, and about 10 times higher than those estimated for residents in New York City and Japan. By assuming that the average concentration of 239,240Pu in bone samples is the value at 45 years after instantaneous inhalation in 1955, the initial total intake and the effective dose for 45 years were estimated as 10 Bq and 0.2 mSv, respectively. The annual intake of total U (234,235,238U) and its effective dose for 60 years were estimated as 30 Bq for adult and 0.1 mSv, respectively, for chronic ingestion.

SPRAY CALCINATION REACTOR

DOEpatents

Johnson, B.M.

1963-08-20

A spray calcination reactor for calcining reprocessin- g waste solutions is described. Coaxial within the outer shell of the reactor is a shorter inner shell having heated walls and with open regions above and below. When the solution is sprayed into the irner shell droplets are entrained by a current of gas that moves downwardly within the inner shell and upwardly between it and the outer shell, and while thus being circulated the droplets are calcined to solids, whlch drop to the bottom without being deposited on the walls. (AEC) H03 H0233412 The average molecular weights of four diallyl phthalate polymer samples extruded from the experimental rheometer were redetermined using the vapor phase osmometer. An amine curing agent is required for obtaining suitable silver- filled epoxy-bonded conductive adhesives. When the curing agent was modified with a 47% polyurethane resin, its effectiveness was hampered. Neither silver nor nickel filler impart a high electrical conductivity to Adiprenebased adhesives. Silver filler was found to perform well in Dow-Corning A-4000 adhesive. Two cascaded hot-wire columns are being used to remove heavy gaseous impurities from methane. This purified gas is being enriched in the concentric tube unit to approximately 20% carbon-13. Studies to count low-level krypton-85 in xenon are continuing. The parameters of the counting technique are being determined. The bismuth isotopes produced in bismuth irradiated for polonium production are being determined. Preliminary data indicate the presence of bismuth207 and bismuth-210m. The light bismuth isotopes are probably produced by (n,xn) reactions bismuth-209. The separation of uranium-234 from plutonium-238 solutions was demonstrated. The bulk of the plutonium is removed by anion exchange, and the remainder is extracted from the uranium by solvent extraction techniques. About 99% of the plutonium can be removed in each thenoyltrifluoroacetone extraction. The viscosity, liquid density, and selfdiffusion coefficient for lanthanum, cerium, and praseodymium were determined. The investigation of phase relationships in the plutonium-cerium-copper ternary system was continued on samples containing a high concentration of copper. These analyses indicate that complete solid solution exists between the binary compounds CeCu/sub 2/ and PuCu/sub 2/, thus forming a quasi-binary system. The study of high temperature ceramic fuel materials has continued with the homogenization and microspheroidization of binary mixtures of plutonium dioxide and zirconium dioxide. Sintering a die-pressed pellet of the mixed powders for one hour at 1450 deg C was not sufficient to completely react the constituents. Complete homogenization was obtained when the pellet was melted in the plasma flame. In addition to the plutonium dioxide-zirconium dioxide microspheres, pure beryllium oxide microspheres were produced in the plasma torch. The electronic distribution functions for the 10% by weight PuO/sub 2/ dissolved in a silicate glass were determined. The plutonium-oxygen interaction at about 2.2A is less than the plutonium-oxygen distance for the 5% PuO/sub 2/. The decrease in the interionic distance is indicative of a stronger plutonium-oxygen association for the more concentrated composition. Potassium plutonium sulfate is being evaluated as a reagent to quantitatively separate plutonium from aqueous solutions. The compound containing two waters of hydration was prepared for thermogravimetric studies using analytically pure plutonium-239. Because of the stability of this compound, it is being evaluated as a calorimetric standard for plutonium-238. (auth)

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

PubMed

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

2017-10-01

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

8. VIEW OF GLOVE BOXES USED IN THE ANION EXCHANGE ...

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

8. VIEW OF GLOVE BOXES USED IN THE ANION EXCHANGE PROCESS. THE ANION EXCHANGE PROCESS PURIFIED AND CONCENTRATED PLUTONIUM-BEARING NITRIC ACID SOLUTIONS TO MAKE THEM ACCEPTABLE AS FEED FOR CONVERSION TO METAL. (6/20/60) - Rocky Flats Plant, Plutonium Recovery & Fabrication Facility, North-central section of plant, Golden, Jefferson County, CO

The solubility of hydrogen in plutonium in the temperature range 475 to 825 degrees centigrade

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

Allen, T.H.

1991-01-01

The solubility of hydrogen (H) in plutonium metal (Pu) was measured in the temperature range of 475 to 825{degree}C for unalloyed Pu (UA) and in the temperature range of 475 to 625{degree}C for Pu containing two-weight-percent gallium (TWP). For TWP metal, in the temperature range 475 to 600{degree}C, the saturated solution has a maximum hydrogen to plutonium ration (H/Pu) of 0.00998 and the standard enthalpy of formation ({Delta}H{degree}{sub f(s)}) is (-0.128 {plus minus} 0.0123) kcal/mol. The phase boundary of the solid solution in equilibrium with plutonium dihydride (PuH{sub 2}) is temperature independent. In the temperature range 475 to 625{degree}C, UAmore » metal has a maximum solubility at H/Pu = 0.011. The phase boundary between the solid solution region and the metal+PuH{sub 2} two-phase region is temperature dependent. The solubility of hydrogen in UA metal was also measured in the temperature range 650 to 825{degree}C with {Delta}H{degree}{sub f(s)} = (-0.104 {plus minus} 0.0143) kcal/mol and {Delta}S{degree}{sub f(s)} = 0. The phase boundary is temperature dependent and the maximum hydrogen solubility has H/Pu = 0.0674 at 825{degree}C. 52 refs., 28 figs., 9 tabs.« less

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

USGS Publications Warehouse

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

2004-01-01

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

Investigation of Pu(IV)-acetohydroxamic acid complex by solvent extraction with di(2-ethylhexyl) phosphoric acid

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.

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

NASA Astrophysics Data System (ADS)

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

2009-12-01

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

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

PubMed

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

2017-12-01

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

The United States Transuranium and Uranium Registries. Revision 1, [Annual] report, October 1, 1990--April 1992

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

Kathren, R.L.

1992-09-01

This paper describes the history, organization, activities and recent scientific accomplishments of the United States Transuranium and Uranium Registries. Through voluntary donations of tissue obtained at autopsies, the Registries carry out studies of the concentration, distribution and biokinetics of plutonium in occupationally exposed persons. Findings from tissue analyses from more than 200 autopsies include the following: a greater proportion of the americium intake, as compared with plutonium, was found in the skeleton; the half-time of americium in liver is significantly shorter than that of plutonium; the concentration of actinide in the skeleton is inversely proportional to the calcium and ashmore » content of the bone; only a small percentage of the total skeletal deposition of plutonium is found in the marrow, implying a smaller risk from irradiation of the marrow relative to the bone surfaces; estimates of plutonium body burden made from urinalysis typically exceed those made from autopsy data; pathologists were unable to discriminate between a group of uranium workers and persons without known occupational exposure on the basis of evaluation of microscopic kidney slides; the skeleton is an important long term depot for uranium, and that the fractional uptake by both skeleton and kidney may be greater than indicated by current models. These and other findings and current studies are discussed in depth.« less

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

DOE PAGES

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

2016-02-22

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

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

PubMed Central

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

2016-01-01

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

Second NBL measurement evaluation program meeting: A summary

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

Spaletto, M.I.; Clapper, M.; Tolbert, M.E.M.

New Brunswick Laboratory (NBL), the US government`s nuclear materials measurements and reference materials laboratory, administers interlaboratory measurement evaluation programs to evaluate the quality and adequacy of safeguards measurements. The NBL Measurement Evaluation Program covers several types of safeguards analytical measurements. The Safeguards Measurement Evaluation (SME) program distributes test materials destructive measurements of uranium for both elemental concentration and isotopic abundances, and of plutonium for isotopic abundances. The Calorimetry Exchange (CalEx) Program tests the quality of nondestructive measurements of plutonium isotopic abundances by gamma spectroscopy and plutonium concentration by calorimetry. In May 1997, more than 30 representatives from the Department ofmore » Energy (DOE), its contractor laboratories, and Nuclear Regulatory Commission licensees met at NBL in Argonne, Illinois, for the annual meeting of the Measurement Evaluation Program. The summary which follows details key points that were discussed or presented at the meeting.« less

Lens of Eye Dosimetry

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

Mallett, Michael Wesley

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

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

DOE PAGES

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

2017-10-05

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

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

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

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

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

Radioecologycal study of {sup 239/240}Pu in Bangka Island and Muria Peninsula: Determination of {sup 239/240}Pu in marine sediment and seawater as part of baseline data collecting for sitting of candidates of first Indonesia NPP

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

Suseno, Heny, E-mail: henis@batan.go.id; Wisnubroto, Djarot S.

Radioisotope Pu-239/240 are alpha emitting nuclides important indicators of radioactive contamination of the marine environment. Global fallout is the main source of plutonium in the marine environment. There are very limited study on {sup 239/240}Pu in Indonesia coastal environments. The data of this radioisotopes is needed for baseline data of nuclear power plant (NPP) site candidates both in Bangka Island and Muria Peninsula. Bottom sediments play an important role in radioecological studies of the marine environment because a large proportion of radioactive substances entering the sea is adsorbed over time onto suspended particulate matter and deposited in sediments. Plutonium ismore » particle reactive and deposited in marine sediment. Radioisotope {sup 239/240}Pu was determinated by alpha spectrometry after radiochemical procedure that was performed in both water and marine sediment from Bangka Island and Muria Peninsula. The sediment baseline of concentration {sup 239/240}Pu in Bangka Island and Muria Peninsula were range from 0.013 to 0.021 Bq.kg{sup −1} and 0.018 to 0.024 Bq.kg{sup −1} respectively. The water baseline concentration this isotope were range from 2.73 to 4.05 mBq.m{sup −3} and 2.98 to 4.50 mBq.m{sup −3}.« less

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

PubMed

Xing, Shan; Zhang, Weichao; Qiao, Jixin; Hou, Xiaolin

2018-09-01

In order to measure trace plutonium and its isotopes ratio ( 240 Pu/ 239 Pu) in environmental samples with a high uranium, an analytical method was developed using radiochemical separation for separation of plutonium from matrix and interfering elements including most of uranium and ICP-MS for measurement of plutonium isotopes. A novel measurement method was established for extensively removing the isobaric interference from uranium ( 238 U 1 H and 238 UH 2 + ) and tailing of 238 U, but significantly improving the measurement sensitivity of plutonium isotopes by employing NH 3 /He as collision/reaction cell gases and MS/MS system in the triple quadrupole ICP-MS instrument. The results show that removal efficiency of uranium interference was improved by more than 15 times, and the sensitivity of plutonium isotopes was increased by a factor of more than 3 compared to the conventional ICP-MS. The mechanism on the effective suppress of 238 U interference for 239 Pu measurement using NH 3 -He reaction gases was explored to be the formation of UNH + and UNH 2 + in the reactions of UH + and U + with NH 3 , while no reaction between NH 3 and Pu + . The detection limits of this method were estimated to be 0.55 fg mL -1 for 239 Pu, 0.09 fg mL -1 for 240 Pu. The analytical precision and accuracy of the method for Pu isotopes concentration and 240 Pu/ 239 Pu atomic ratio were evaluated by analysis of sediment reference materials (IAEA-385 and IAEA-412) with different levels of plutonium and uranium. The developed method were successfully applied to determine 239 Pu and 240 Pu concentrations and 240 Pu/ 239 Pu atomic ratios in soil samples collected in coastal areas of eastern China. Copyright © 2018 Elsevier B.V. All rights reserved.

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

Migration of conservative and sorbing radionuclides in heterogeneous fractured rock aquifers at the Nevada Test Site

NASA Astrophysics Data System (ADS)

Boryta, J. R.; Wolfsberg, A. V.

2003-12-01

The Nevada Test Site (NTS) is the United States continental nuclear weapons testing site. The larger underground tests, including BENHAM and TYBO, were conducted at Pahute Mesa. The BENHAM test, conducted in 1968, was detonated 1.4 km below the surface and the TYBO test, conducted in 1975, was detonated at a depth of 765 m. Between 1996 and 1998, several radionuclides were discovered in trace concentrations in a monitoring well complex 273 m from TYBO and 1300 m from BENHAM. Previous studies associated with these measurements have focused primarily on a) plutonium discovered in the observation wells, which was identified through isotopic finger printing as originating at BENHAM, b) colloid-facilitated plutonium transport processes, and c) vertical convection in subsurface nuclear test collapse chimneys. In addition to plutonium, several other non-, weakly-, and strongly-sorbing radionuclides were discovered in trace concentrations in the observation wells, including tritium, carbon-14, chlorine-36, iodine-129, technetium-99, neptunium-237, strontium-90, cesium-137, americium-241, and europium-152,154,155. The range in retardation processes affecting these different radionuclides provides additional information for assessing groundwater solute transport model formulations. For all radionuclides, simulation results are most sensitive to the fracture porosity and fracture aperture. Additionally, for weakly sorbing Np, simulation results are highly sensitive to the matrix sorption coefficient. For strongly sorbing species, migration in the absence of colloids can only be simulated if fracture apertures are set very large, reducing the amount of diffusion that can occur. For these species, colloid-facilitated transport appears to be a more likely explanation for the measurements. This is corroborated with colloid-transport model simulations.

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

DOE PAGES

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

2015-01-16

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

Preliminary Assessment for CAU 485: Cactus Spring Ranch Pu and Du Site, CAS No. TA-39-001-TAGR: Soil Contamination, Tonapah Test Range, Nevada

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

ITLV

1998-07-01

Corrective Action Unit 485, Corrective Action Site TA-39-001-TAGR, the Cactus Spring Ranch Soil Contamination Area, is located approximately six miles southwest of the Area 3 Compound at the eastern mouth of Sleeping Column Canyon in the Cactus Range on the Tonopah Test Range. This site was used in conjunction with animal studies involving the biological effects of radionuclides (specifically plutonium) associated with Operation Roller Coaster. According to field records, a hardened layer of livestock feces ranging from 2.54 centimeters (cm) (1 inch [in.]) to 10.2 cm (4 in.) thick is present in each of the main sheds. IT personnel conductedmore » a field visit on December 3, 1997, and noted that the only visible feces were located within the east shed, the previously fenced area near the east shed, and a small area southwest of the west shed. Other historical records indicate that other areas may still be covered with animal feces, but heavy vegetation now covers it. It is possible that radionuclides are present in this layer, given the history of operations in this area. Chemicals of concern may include plutonium and depleted uranium. Surface soil sampling was conducted on February 18, 1998. An evaluation of historical documentation indicated that plutonium should not be and depleted uranium could not be present at levels significantly above background as the result of test animals being penned at the site. The samples were analyzed for isotopic plutonium using method NAS-NS-3058. The results of the analysis indicated that plutonium levels of the feces and surface soil were not significantly elevated above background.« less

Source-term characterisation and solid speciation of plutonium at the Semipalatinsk NTS, Kazakhstan.

PubMed

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.

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

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

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

DOE PAGES

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

2016-12-05

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

Determination of 240Pu/239Pu isotopic ratios in human tissues collected from areas around the Semipalatinsk Nuclear Test Site by sector-field high resolution ICP-MS.

PubMed

Yamamoto, M; Oikawa, S; Sakaguchi, A; Tomita, J; Hoshi, M; Apsalikov, K N

2008-09-01

Information on the 240Pu/239Pu isotope ratios in human tissues for people living around the Semipalatinsk Nuclear Test Site (SNTS) was deduced from 9 sets of soft tissues and bones, and 23 other bone samples obtained by autopsy. Plutonium was radiochemically separated and purified, and plutonium isotopes (239Pu and 240Pu) were determined by sector-field high resolution inductively coupled plasma-mass spectrometry. For most of the tissue samples from the former nine subjects, low 240Pu/239Pu isotope ratios were determined: bone, 0.125 +/- 0.018 (0.113-0.145, n = 4); lungs, 0.063 +/- 0.010 (0.051-0.078, n = 5); and liver, 0.148 +/- 0.026 (0.104-0.189, n = 9). Only 239Pu was detected in the kidney samples; the amount of 240Pu was too small to be measured, probably due to the small size of samples analyzed. The mean 240Pu/239Pu isotope ratio for bone samples from the latter 23 subjects was 0.152 +/- 0.034, ranging from 0.088 to 0.207. A significant difference (a two-tailed Student's t test; 95% significant level, alpha = 0.05) between mean 240Pu/239Pu isotope ratios for the tissue samples and for the global fallout value (0.178 +/- 0.014) indicated that weapons-grade plutonium from the atomic bombs has been incorporated into the human tissues, especially lungs, in the residents living around the SNTS. The present 239,240Pu concentrations in bone, lung, and liver samples were, however, not much different from ranges found for human tissues from other countries that were due solely to global fallout during the 1970's-1980's.

Spatial distributions of (137)Cs and (239+240)Pu in surface seawater within the Exclusive Economic Zone of East Coast Peninsular Malaysia.

PubMed

Ahmad, Zaharudin; Mei-Wo, Yii; Abu Bakar, Ahmad Sanadi; Shahar, Hidayah

2010-09-01

The studies of (137)Cs and (239+240)Pu distributions in surface seawater at South China Sea within the Exclusive Economic Zone (EEZ) of Peninsular Malaysia were carried out in June 2008. The analysis results will serve as additional information to the expanded baseline data for Malaysia's marine environment. Thirty locations from extended study area were identified in the EEZ from which large volumes of surface seawater samples were collected. Different co-precipitation techniques were employed to concentrate cesium and plutonium separately. A known amount of (134)Cs and (242)Pu tracers were used as yield determinant. The precipitate slurry was collected and oven dried at 60(o)C for 1-2 days. Cesium precipitate was fine-ground and counted using gamma-ray spectrometry system at 661.62keV, while plutonium was separated from other radionuclides using anion exchange, electrodeposited and counted using alpha spectrometry. The activity concentrations of (137)Cs and (239+240)Pu were in the range of 3.40-5.89Bq/m(3) and 2.3-7.9mBq/m(3), respectively. The (239+240)Pu/(137)Cs ratios indicate that there are no new inputs of these radionuclides into the area.

PROCESS OF REDUCING PLUTONIUM TO TETRAVALENT TRIVALENT STATE

DOEpatents

Mastick, D.F.

1960-05-10

The reduction of hexavalent and tetravalert plutonium ions to the trivalent state in strong nitric acid can be accomplished with hydrogen peroxide. The trivalent state may be stabilized as a precipitate by including oxalate or fluoride ions in the solution. The acid should be strong to encourage the reduction from the plutonyl to the trivalent state (and discourage the opposed oxidation reaction) and prevent the precipitation of plutonium peroxide, although the latter may be digested by increasing the acid concentration. Although excess hydrogen peroxide will oxidize plutonlum to the plutonyl state, complete reduction is insured by gently warming the solution to break down such excess H/ sub 2/O/sub 2/. The particular advantage of hydrogen peroxide as a reductant lies in the precipitation technique, where it introduces no contaminating ions. The process is adaptable to separate plutonium from uranium and impurities by proper adjustment of the sequence of insoluble anion additions and the hydrogen peroxide addition.

Closure Report for Corrective Action Unit 412: Clean Slate I Plutonium Dispersion (TTR) Tonopah Test Range, Nevada, Revision 0

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

Matthews, Patrick

This Closure Report (CR) presents information supporting the clean closure of Corrective Action Unit (CAU) 412: Clean Slate I Plutonium Dispersion (TTR), located on the Tonopah Test Range, Nevada. CAU 412 consists of a release of radionuclides to the surrounding soil from a storage–transportation test conducted on May 25, 1963. Corrective action investigation (CAI) activities were performed in April and May 2015, as set forth in the Streamlined Approach for Environmental Restoration (SAFER) Plan for Corrective Action Unit 412: Clean Slate I Plutonium Dispersion (TTR), Tonopah Test Range, Nevada; and in accordance with the Soils Activity Quality Assurance Plan. Themore » purpose of the CAI was to fulfill data needs as defined during the data quality objectives process. The CAU 412 dataset of investigation results was evaluated based on a data quality assessment. This assessment demonstrated the dataset is complete and acceptable for use in fulfilling the data needs identified by the data quality objectives process. This CR provides documentation and justification for the clean closure of CAU 412 under the FFACO without further corrective action. This justification is based on historical knowledge of the site, previous site investigations, implementation of the 1997 interim corrective action, and the results of the CAI. The corrective action of clean closure was confirmed as appropriate for closure of CAU 412 based on achievement of the following closure objectives: Radiological contamination at the site is less than the final action level using the ground troops exposure scenario (i.e., the radiological dose is less than the final action level): Removable alpha contamination is less than the high contamination area criterion: No potential source material is present at the site, and any impacted soil associated with potential source material has been removed so that remaining soil contains contaminants at concentrations less than the final action levels: and There is sufficient information to characterize investigation and remediation waste for disposal.« less

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

NASA Astrophysics Data System (ADS)

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

2000-07-01

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

Sorption/Desorption Interactions of Plutonium with Montmorillonite

NASA Astrophysics Data System (ADS)

Begg, J.; Zavarin, M.; Zhao, P.; Kersting, A. B.

2012-12-01

Plutonium (Pu) release to the environment through nuclear weapon development and the nuclear fuel cycle is an unfortunate legacy of the nuclear age. In part due to public health concerns over the risk of Pu contamination of drinking water, predicting the behavior of Pu in both surface and sub-surface water is a topic of continued interest. Typically it was assumed that Pu mobility in groundwater would be severely restricted, as laboratory adsorption studies commonly show that naturally occurring minerals can effectively remove plutonium from solution. However, evidence for the transport of Pu over significant distances at field sites highlights a relative lack of understanding of the fundamental processes controlling plutonium behavior in natural systems. At several field locations, enhanced mobility is due to Pu association with colloidal particles that serve to increase the transport of sorbed contaminants (Kersting et al., 1999; Santschi et al., 2002, Novikov et al., 2006). The ability for mineral colloids to transport Pu is in part controlled by its oxidation state and the rate of plutonium adsorption to, and desorption from, the mineral surface. Previously we have investigated the adsorption affinity of Pu for montmorillonite colloids, finding affinities to be similar over a wide range of Pu concentrations. In the present study we examine the stability of adsorbed Pu on the mineral surface. Pu(IV) at an initial concentration of 10-10 M was pre-equilibrated with montmorillonite in a background electrolyte at pH values of 4, 6 and 8. Following equilibration, aliquots of the suspensions were placed in a flow cell and Pu-free background electrolyte at the relevant pH was passed through the system. Flow rates were varied in order to investigate the kinetics of desorption and hence gain a mechanistic understanding of the desorption process. The flow cell experiments demonstrate that desorption of Pu from the montmorillonite surface cannot be modeled as a simple first order process. Furthermore, a pH dependence was observed, with less desorbed at pH 4 compared to pH 8. We suggest the pH dependence is likely controlled by reoxidation of Pu(IV) to Pu(V) and aqueous speciation. We will present models used to describe desorption behavior and discuss the implications for Pu transport. References: Kersting, A.B.; Efurd, D.W.; Finnegan, D.L.; Rokop, D.J.; Smith, D.K.; Thompson J.L. (1999) Migration of plutonium in groundwater at the Nevada Test Site, Nature, 397, 56-59. Novikov A.P.; Kalmykov, S.N.; Utsunomiya, S.; Ewing, R.C.; Horreard, F.; Merkulov, A.; Clark, S.B.; Tkachev, V.V.; Myasoedov, B.F. (2006) Colloid transport of plutonium in the far-field of the Mayak Production Association, Russia, Science, 314, 638-641. Santschi, P.H.; Roberts, K.; Guo, L. (2002) The organic nature of colloidal actinides transported in surface water environments. Environ. Sci. Technol., 36, 3711-3719. This work was funded by U. S. DOE Office of Biological & Environmental Sciences, Subsurface Biogeochemistry Research Program, and performed under the auspices of the U. S. Department of Energy by Lawrence Livermore National Security, LLC under Contract DE-AC52-07NA27344. LLNL-ABS-570161

Accelerated Analyte Uptake on Single Beads in Microliter-scale Batch Separations using Acoustic Streaming: Plutonium Uptake by Anion Exchange for Analysis by Mass Spectrometry

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

Paxton, Walter F.; O'Hara, Matthew J.; Peper, Shane M.

2008-06-01

The use of acoustic streaming as a non-contact mixing platform to accelerate mass transport-limited diffusion processes in small volume heterogeneous reactions has been investigated. Single bead anion exchange of plutonium at nanomolar and sub-picomolar concentrations in 20 microliter liquid volumes was used to demonstrate the effect of acoustic mixing. Pu uptake rates on individual ~760 micrometer diameter AG 1x4 anion exchange resin beads were determined using acoustic mixing and compared with Pu uptake rates achieved by static diffusion alone. An 82 MHz surface acoustic wave (SAW) device was placed in contact with the underside of a 384-well microplate containing flat-bottomedmore » semiconical wells. Acoustic energy was coupled into the solution in the well, inducing acoustic streaming. Pu uptake rates were determined by the plutonium remaining in solution after specific elapsed time intervals, using liquid scintillation counting (LSC) for nanomolar concentrations and thermal ionization mass spectrometry (TIMS) analysis for the sub-picomolar concentration experiments. It was found that this small batch uptake reaction could be accelerated by a factor of about five-fold or more, depending on the acoustic power applied.« less

Recent advances in the detection of specific natural organic compounds as carriers for radionuclides in soil and water environments, with examples of radioiodine and plutonium

DOE PAGES

Santschi, P. H.; Xu, C.; Zhang, S.; ...

2017-03-09

Among the key environmental factors influencing the fate and transport of radionuclides in the environment is natural organic matter (NOM). While this has been known for decades, there still remains great uncertainty in predicting NOM-radionuclide interactions because of lack of understanding of radionuclide interactions with the specific organic moieties within NOM. Furthermore, radionuclide-NOM studies conducted using modelled organic compounds or elevated radionuclide concentrations provide compromised information related to true environmental conditions. Thus, sensitive techniques are required not only for the detection of radionuclides, and their different species, at ambient and/or far-field concentrations, but also for potential trace organic compounds thatmore » are chemically binding these radionuclides. GC-MS and AMS techniques developed in our lab are reviewed in this paper that aim to assess how two radionuclides, iodine and plutonium, form strong bonds with NOM by entirely different mechanisms; iodine tends to bind to aromatic functionalities, whereas plutonium binds to N-containing hydroxamate siderophores at ambient concentrations. While low-level measurements are a prerequisite for assessing iodine and plutonium migration at nuclear waste sites and as environmental tracers, it is necessary to determine their in-situ speciation, which ultimately controls their mobility and transport in natural environments. Finally and more importantly, advanced molecular-level instrumentation (e.g., nuclear magnetic resonance (NMR) and Fourier-transform ion cyclotron resonance coupled with electrospray ionization (ESI-FTICRMS) were applied to resolve either directly or indirectly the molecular environments in which the radionuclides are associated with the NOM.« less

Recent advances in the detection of specific natural organic compounds as carriers for radionuclides in soil and water environments, with examples of radioiodine and plutonium

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

Santschi, P. H.; Xu, C.; Zhang, S.

Among the key environmental factors influencing the fate and transport of radionuclides in the environment is natural organic matter (NOM). While this has been known for decades, there still remains great uncertainty in predicting NOM-radionuclide interactions because of lack of understanding of radionuclide interactions with the specific organic moieties within NOM. Furthermore, radionuclide-NOM studies conducted using modelled organic compounds or elevated radionuclide concentrations provide compromised information related to true environmental conditions. Thus, sensitive techniques are required not only for the detection of radionuclides, and their different species, at ambient and/or far-field concentrations, but also for potential trace organic compounds thatmore » are chemically binding these radionuclides. GC-MS and AMS techniques developed in our lab are reviewed in this paper that aim to assess how two radionuclides, iodine and plutonium, form strong bonds with NOM by entirely different mechanisms; iodine tends to bind to aromatic functionalities, whereas plutonium binds to N-containing hydroxamate siderophores at ambient concentrations. While low-level measurements are a prerequisite for assessing iodine and plutonium migration at nuclear waste sites and as environmental tracers, it is necessary to determine their in-situ speciation, which ultimately controls their mobility and transport in natural environments. Finally and more importantly, advanced molecular-level instrumentation (e.g., nuclear magnetic resonance (NMR) and Fourier-transform ion cyclotron resonance coupled with electrospray ionization (ESI-FTICRMS) were applied to resolve either directly or indirectly the molecular environments in which the radionuclides are associated with the NOM.« less

PROCESS FOR SEGREGATING URANIUM FROM PLUTONIUM AND FISSION-PRODUCT CONTAMINATION

DOEpatents

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.

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

PubMed

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

2018-07-01

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

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

MOSTELLER, RUSSELL D.

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

Design and fabrication of 55-gallon drum shuffler standards

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

Long, S.M.; Hsue, F.; Hoth, C.

1994-08-01

To analyze waste with varying levels of nuclear material, suitable standards are needed to calibrate analytical instrumentation. At the Los Alamos Plutonium Facility, the authors have designed and fabricated a single drum standard for a passive-active neutron counter (shuffler). The standard is modified simply by adding or subtracting plutonium of uranium cylinders to adapt to a range of nuclear material. The plutonium or uranium oxide was placed into small cylindrical containers (1-in. diameter by 5-in. long) and diluted with diatomaceous earth. The cylinders were welded closed and removed from the glove box environment without any external contamination. The containers weremore » leak tested and then placed on a segmented gamma scanner to assure homogeneous distribution of the nuclear material. The cylinders are now placed into the drum to achieve the needed ranges for calibration of the instruments.« less

Statistical analysis of $sup 239-240$Pu and $sup 241$Am contamination of soil and vegetation on NAEG study sites

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

Gilbert, R.O.; Eberhardt, L.L.; Fowler, E.B.

Reported here are results of the statistical design and analysis work conducted during Calendar Year 1974 for the Nevada Applied Ecology Group (NAEG) at plutonium study sites on the Nevada Test Site (NTS) and the Tonopah Test Range (TTR). Estimates of $sup 239-240$Pu inventory in surface soil (0 to 5-cm depth) are given for each of the NAEG intensive study sites, together with activity maps based on FIDLER surveys showing the field areas to which these estimates apply. There is evidence of a preliminary nature to suggest that the plutonium present in surface soil may be covered by a thinmore » (less than 2.5 cm) layer of soil whose alpha activity is considerably less than that directly below. Computer-drawn $sup 239-240$Pu concentration contours and three-dimensional surfaces in soil and vegetation are given for Area 13 and GMX as a first attempt at estimating the geographical distribution of $sup 239-240$Pu at these sites. (CH)« less

Influence of point defects and impurities on the dynamical stability of δ-plutonium

NASA Astrophysics Data System (ADS)

Dorado, B.; Bieder, J.; Torrent, M.

2017-06-01

We use first-principles calculations to provide direct evidence of the effect of aluminum, gallium, iron and uranium on the dynamical stability of δ-plutonium. We first show that the δ phase is dynamically unstable at low temperature, as seen in experiments, and that this stability directly depends on the plutonium 5f orbital occupancies. Then, we demonstrate that both aluminum and gallium stabilize the δ phase, contrary to iron. As for uranium, which is created during self-irradiation and whose effect on plutonium has yet to be understood, we show that it leaves a few unstable vibrational modes and that higher concentrations lead to an almost complete stabilization. Finally, we provide an attempt at a consistent analysis of the experimental Pu-Ga phonon density of states. We show that the presence of gallium can reproduce only partially the experimental measurements, and we investigate how point defects, such as interstitials and vacancies, affect the calculated phonon density of states.

Influence of point defects and impurities on the dynamical stability of δ-plutonium.

PubMed

Dorado, B; Bieder, J; Torrent, M

2017-06-21

We use first-principles calculations to provide direct evidence of the effect of aluminum, gallium, iron and uranium on the dynamical stability of δ-plutonium. We first show that the δ phase is dynamically unstable at low temperature, as seen in experiments, and that this stability directly depends on the plutonium 5f orbital occupancies. Then, we demonstrate that both aluminum and gallium stabilize the δ phase, contrary to iron. As for uranium, which is created during self-irradiation and whose effect on plutonium has yet to be understood, we show that it leaves a few unstable vibrational modes and that higher concentrations lead to an almost complete stabilization. Finally, we provide an attempt at a consistent analysis of the experimental Pu-Ga phonon density of states. We show that the presence of gallium can reproduce only partially the experimental measurements, and we investigate how point defects, such as interstitials and vacancies, affect the calculated phonon density of states.

In-vitro analysis of the dissolution kinetics and systemic availability of plutonium ingested in the form of 'hot' particles from the Semipalatinsk NTS.

PubMed

Conway, M; León Vintró, L; Mitchell, P I; García-Tenorio, R; Jimenez-Ramos, M C; Burkitbayev, M; Priest, N D

2009-05-01

In-vitro leaching of radioactive 'hot' particles isolated from soils sampled at the Semipalatinsk Nuclear Test Site has been carried out in order to evaluate the fraction of plutonium activity released into simulated human stomach and small intestine fluids during digestion. Characterisation of the particles (10-100 Bq(239,240)Pu) and investigation of their dissolution kinetics in simulated fluids has been accomplished using a combination of high-resolution alpha-spectrometry, gamma-spectrometry and liquid scintillation counting. The results of these analyses indicate that plutonium transfer across the human gut following the ingestion of 'hot' particles can be up to two orders of magnitude lower than that expected for plutonium in a more soluble form, and show that for areas affected by local fallout, use of published ingestion dose coefficients, together with bulk radionuclide concentrations in soil, may lead to a considerable overestimation of systemic uptake via the ingestion pathway.

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

Preliminary Study on LiF4-ThF4-PuF4 Utilization as Fuel Salt of miniFUJI Molten Salt Reactor

NASA Astrophysics Data System (ADS)

Waris, Abdul; Aji, Indarta K.; Pramuditya, Syeilendra; Widayani; Irwanto, Dwi

2016-08-01

miniFUJI reactor is molten salt reactor (MSR) which is one type of the Generation IV nuclear energy systems. The original miniFUJI reactor design uses LiF-BeF2-ThF4-233UF4 as a fuel salt. In the present study, the use of LiF4-ThF4-PuF4 as fuel salt instead of LiF-BeF2-ThF4-UF4 will be discussed. The neutronics cell calculation has been performed by using PIJ (collision probability method code) routine of SRAC 2006 code, with the nuclear data library is JENDL-4.0. The results reveal that the reactor can attain the criticality condition with the plutonium concentration in the fuel salt is equal to 9.16% or more. The conversion ratio diminishes with the enlarging of plutonium concentration in the fuel. The neutron spectrum of miniFUJI MSR with plutonium fuel becomes harder compared to that of the 233U fuel.

Method for dissolving plutonium oxide with HI and separating plutonium

DOEpatents

Vondra, Benedict L.; Tallent, Othar K.; Mailen, James C.

1979-01-01

PuO.sub.2 -containing solids, particularly residues from incomplete HNO.sub.3 dissolution of irradiated nuclear fuels, are dissolved in aqueous HI. The resulting solution is evaporated to dryness and the solids are dissolved in HNO.sub.3 for further chemical reprocessing. Alternatively, the HI solution containing dissolved Pu values, can be contacted with a cation exchange resin causing the Pu values to load the resin. The Pu values are selectively eluted from the resin with more concentrated HI.

Colloid formation during waste form reaction: Implications for nuclear waste disposal

USGS Publications Warehouse

Bates, J. K.; Bradley, J.; Teetsov, A.; Bradley, C. R.; Buchholtz ten Brink, Marilyn R.

1992-01-01

Insoluble plutonium- and americium-bearing colloidal particles formed during simulated weathering of a high-level nuclear waste glass. Nearly 100 percent of the total plutonium and americium in test ground water was concentrated in these submicrometer particles. These results indicate that models of actinide mobility and repository integrity, which assume complete solubility of actinides in ground water, underestimate the potential for radionuclide release into the environment. A colloid-trapping mechanism may be necessary for a waste repository to meet long-term performance specifications.

Gum-compliant uncertainty propagations for Pu and U concentration measurements using the 1st-prototype XOS/LANL hiRX instrument; an SRNL H-Canyon Test Bed performance evaluation project

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

Holland, Michael K.; O'Rourke, Patrick E.

An SRNL H-Canyon Test Bed performance evaluation project was completed jointly by SRNL and LANL on a prototype monochromatic energy dispersive x-ray fluorescence instrument, the hiRX. A series of uncertainty propagations were generated based upon plutonium and uranium measurements performed using the alpha-prototype hiRX instrument. Data reduction and uncertainty modeling provided in this report were performed by the SRNL authors. Observations and lessons learned from this evaluation were also used to predict the expected uncertainties that should be achievable at multiple plutonium and uranium concentration levels provided instrument hardware and software upgrades being recommended by LANL and SRNL are performed.

Evaluation of background concentrations of selected chemical and radiochemical constituents in water from the eastern Snake River Plain aquifer at and near the Idaho National Laboratory, Idaho

USGS Publications Warehouse

Bartholomay, Roy C.; L. Flint Hall,

2016-05-05

The upper limit of background concentrations for radiochemical constituents for eastern regional water was 5.43 ±0.574 pCi/L for tritium, 0.0002048 ±0.0000054 pCi/L for chlorine-36, 0.000000865 ±0.000000015 pCi/L for iodine-129, <0.0000054 pCi/L for technetium-99, 0 pCi/L for strontium-90, plutonium-238, plutonium-239, -240 (undivided), and americium-241, 1.32 ±0.77 pCi/L for uranium-234, 0.016 ±0.012 pCi/L for uranium-235, and 0.477 ±0.044 pCi/L for uranium-238.

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

Carmack, Jon; Hayes, Steven; Walters, L. C.

This document explores startup fuel options for a proposed test/demonstration fast reactor. The fuel options considered are the metallic fuels U-Zr and U-Pu-Zr and the ceramic fuels UO 2 and UO 2-PuO 2 (MOX). Attributes of the candidate fuel choices considered were feedstock availability, fabrication feasibility, rough order of magnitude cost and schedule, and the existing irradiation performance database. The reactor-grade plutonium bearing fuels (U-Pu-Zr and MOX) were eliminated from consideration as the initial startup fuels because the availability and isotopics of domestic plutonium feedstock is uncertain. There are international sources of reactor grade plutonium feedstock but isotopics and availabilitymore » are also uncertain. Weapons grade plutonium is the only possible source of Pu feedstock in sufficient quantities needed to fuel a startup core. Currently, the available U.S. source of (excess) weapons-grade plutonium is designated for irradiation in commercial light water reactors (LWR) to a level that would preclude diversion. Weapons-grade plutonium also contains a significant concentration of gallium. Gallium presents a potential issue for both the fabrication of MOX fuel as well as possible performance issues for metallic fuel. Also, the construction of a fuel fabrication line for plutonium fuels, with or without a line to remove gallium, is expected to be considerably more expensive than for uranium fuels. In the case of U-Pu-Zr, a relatively small number of fuel pins have been irradiated to high burnup, and in no case has a full assembly been irradiated to high burnup without disassembly and re-constitution. For MOX fuel, the irradiation database from the Fast Flux Test Facility (FFTF) is extensive. If a significant source of either weapons-grade or reactor-grade Pu became available (i.e., from an international source), a startup core based on Pu could be reconsidered.« less

Oxygen potential of uranium--plutonium oxide as determined by controlled- atmosphere thermogravimetry

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

Swanson, Gerald C.

1975-10-01

The oxygen-to-metal atom ratio, or O/M, of solid solution uranium- plutonium oxide reactor fuel is a measure of the concentration of crystal defects in the oxide which affect many fuel properties, particularly, fuel oxygen potential. Fabrication of a high-temperature oxygen electrode, employing an electro-active tip of oxygen-deficient solid-state electrolyte, intended to confirm gaseous oxygen potentials is described. Uranium oxide and plutonium oxide O/M reference materials were prepared by in situ oxidation of high purity metals in the thermobalance. A solid solution uranium-plutonium oxide O/M reference material was prepared by alloying the uranium and plutonium metals in a yttrium oxide cruciblemore » at 1200°C and oxidizing with moist He at 250°C. The individual and solid solution oxides were isothermally equilibrated with controlled oxygen potentials between 800 and 1300°C and the equilibrated O/ M ratios calculated with corrections for impurities and buoyancy effects. Use of a reference oxygen potential of -100 kcal/mol to produce an O/M of 2.000 is confirmed by these results. However, because of the lengthy equilibration times required for all oxides, use of the O/M reference materials rather than a reference oxygen potential is recommended for O/M analysis methods calibrations.« less

Combined radiochemical procedure for determination of plutonium, americium and strontium-90 in the soil samples from SNTS

NASA Astrophysics Data System (ADS)

Kazachevskii, I. V.; Lukashenko, S. N.; Chumikov, G. N.; Chakrova, E. T.; Smirin, L. N.; Solodukhin, V. P.; Khayekber, S.; Berdinova, N. M.; Ryazanova, L. A.; Bannyh, V. I.; Muratova, V. M.

1999-01-01

The results of combined radiochemical procedure for the determination of plutonium, americium and90Sr (via measurement of90Y) in the soil samples from SNTS are presented. The processes of co-precipitation of these nuclides with calcium fluoride in the strong acid solutions have been investigated. The conditions for simultaneous separation of americium and yttrium using extraction chromatography have been studied. It follows from analyses of real soil samples that the procedure developed provides the chemical recovery of plutonium and yttrium in the range of 50-95% and 60-95%, respectively. The execution of the procedure requires 3.5 working days including a sample decomposition study.

DOUBLE TRACKS Test Site interim corrective action plan

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

NONE

The DOUBLE TRACKS site is located on Range 71 north of the Nellis Air Force Range, northwest of the Nevada Test Site (NTS). DOUBLE TRACKS was the first of four experiments that constituted Operation ROLLER COASTER. On May 15, 1963, weapons-grade plutonium and depleted uranium were dispersed using 54 kilograms of trinitrotoluene (TNT) explosive. The explosion occurred in the open, 0.3 m above the steel plate. No fission yield was detected from the test, and the total amount of plutonium deposited on the ground surface was estimated to be between 980 and 1,600 grams. The test device was composed primarilymore » of uranium-238 and plutonium-239. The mass ratio of uranium to plutonium was 4.35. The objective of the corrective action is to reduce the potential risk to human health and the environment and to demonstrate technically viable and cost-effective excavation, transportation, and disposal. To achieve these objectives, Bechtel Nevada (BN) will remove soil with a total transuranic activity greater then 200 pCI/g, containerize the soil in ``supersacks,`` transport the filled ``supersacks`` to the NTS, and dispose of them in the Area 3 Radioactive Waste Management Site. During this interim corrective action, BN will also conduct a limited demonstration of an alternative method for excavation of radioactive near-surface soil contamination.« less

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

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

Cantrell, Kirk J.

2009-08-20

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

Characterization of representative materials in support of safe, long term storage of surplus plutonium in DOE-STD-3013 containers

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

Long-range tropospheric transport of uranium and plutonium weapons fallout from Semipalatinsk nuclear test site to Norway.

PubMed

Wendel, Cato Christian; Fifield, L Keith; Oughton, Deborah H; Lind, Ole Christian; Skipperud, Lindis; Bartnicki, Jerzy; Tims, Stephen G; Høibråten, Steinar; Salbu, Brit

2013-09-01

A combination of state-of-the-art isotopic fingerprinting techniques and atmospheric transport modelling using real-time historical meteorological data has been used to demonstrate direct tropospheric transport of radioactive debris from specific nuclear detonations at the Semipalatinsk test site in Kazakhstan to Norway via large areas of Europe. A selection of archived air filters collected at ground level at 9 stations in Norway during the most intensive atmospheric nuclear weapon testing periods (1957-1958 and 1961-1962) has been screened for radioactive particles and analysed with respect to the concentrations and atom ratios of plutonium (Pu) and uranium (U) using accelerator mass spectrometry (AMS). Digital autoradiography screening demonstrated the presence of radioactive particles in the filters. Concentrations of (236)U (0.17-23nBqm(-3)) and (239+240)Pu (1.3-782μBqm(-3)) as well as the atom ratios (240)Pu/(239)Pu (0.0517-0.237) and (236)U/(239)Pu (0.0188-0.7) varied widely indicating several different sources. Filter samples from autumn and winter tended to have lower atom ratios than those sampled in spring and summer, and this likely reflects a tropospheric influence in months with little stratospheric fallout. Very high (236)U, (239+240)Pu and gross beta activity concentrations as well as low (240)Pu/(239)Pu (0.0517-0.077), (241)Pu/(239)Pu (0.00025-0.00062) and (236)U/(239)Pu (0.0188-0.046) atom ratios, characteristic of close-in and tropospheric fallout, were observed in filters collected at all stations in Nov 1962, 7-12days after three low-yield detonations at Semipalatinsk (Kazakhstan). Atmospheric transport modelling (NOAA HYSPLIT_4) using real-time meteorological data confirmed that long range transport of radionuclides, and possibly radioactive particles, from Semipalatinsk to Norway during this period was plausible. The present work shows that direct tropospheric transport of fallout from atmospheric nuclear detonations periodically may have had much larger influence on radionuclide air concentrations and deposition than previously anticipated. Copyright © 2013 Elsevier Ltd. All rights reserved.

Effect of temperature and radiation damage on the local atomic structure of elemental plutonium and related compounds

DOE PAGES

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

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

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

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

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

2007-05-01

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

Continuous transport of Pacific-derived anthropogenic radionuclides towards the Indian Ocean

PubMed Central

Pittauer, Daniela; Tims, Stephen G.; Froehlich, Michaela B.; Fifield, L. Keith; Wallner, Anton; McNeil, Steven D.; Fischer, Helmut W.

2017-01-01

Unusually high concentrations of americium and plutonium have been observed in a sediment core collected from the eastern Lombok Basin between Sumba and Sumbawa Islands in the Indonesian Archipelago. Gamma spectrometry and accelerator mass spectrometry data together with radiometric dating of the core provide a high-resolution record of ongoing deposition of anthropogenic radionuclides. A plutonium signature characteristic of the Pacific Proving Grounds (PPG) dominates in the first two decades after the start of the high yield atmospheric tests in 1950’s. Approximately 40–70% of plutonium at this site in the post 1970 period originates from the PPG. This sediment record of transuranic isotopes deposition over the last 55 years provides evidence for the continuous long-distance transport of particle-reactive radionuclides from the Pacific Ocean towards the Indian Ocean. PMID:28304374

Nevada Applied Ecology Group publications. [Bibliography of radioecological studies at NTS with special reference to plutonium

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

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.

On radiocarbon and plutonium leakage to groundwater in the vicinity of a shallow-land radioactive waste repository.

PubMed

Gudelis, A; Gvozdaite, R; Kubareviciene, V; Druteikiene, R; Lukosevicius, S; Sutas, A

2010-06-01

A shallow-land radioactive waste repository operated in boggy forest environment from 1963 to 1989. During the operation period, a considerable amount of technogenic radionuclides, in solidified state, was disposed into the vault established in the geological structure at the depth of up to 3m. Environmental monitoring activities started after the closure of the repository in 1989. Recent investigations revealed transfer of radiocarbon and plutonium to the groundwater in the prevailing flow direction. Activity concentration of (239,240)Pu in non-filtered fraction of the groundwater from observation well no. 4 determined by alpha-spectrometry was 6.4 x 10(-5) Bq l(-1) in 2005, and 3.2 x 10(-4) Bq l(-1) in 2006. Further analysis of colloid-facilitated transport of plutonium is planned. Variation of (14)C activity concentration in the same well was monitored in 2006. It varied from 0.2+/-0.1 Bq l(-1) in October to 2.8+/-0.6 Bq l(-1) in June and July. Results imply further research into radiocarbon transfer to atmosphere and selected plant species. Copyright (c) 2008 Elsevier Ltd. All rights reserved.

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

Cournoyer, Michael E; George, Gerald L; Dodge, Robert L

Programmatic operations at the Los Alamos National Laboratory Plutonium Facility (TA-55) involve working with various amounts of plutonium and other highly toxic, alpha-emitting materials. The spread of radiological contamination on surfaces, airborne contamination, and excursions of contaminants into the operator's breathing zone are prevented through the use of a variety of gloveboxes (the glovebox, coupled with an adequate negative pressure gradient, provides primary confinement). Radiation shielding is commonly used to protect the glovebox worker from unintentional direct and secondary radiation exposure, while working with plutonium-238 and plutonium-239. In these environments, low-energy photons, i.e., those less than 250 keY, are encountered.more » Shielding glove box gloves are traditionally composed of lead-based materials, but these are now considered hazardous waste. This has prompted the development of new, nonhazardous- shielding gJovebox gloves. No studies, however, have investigated the effectiveness of these new glovebox gloves. We examined both leaded and nonhazardous- shielding glovebox gloves and compared their attenuation effectiveness over the energy range of interest at TA-55. All measurements are referenced to lead sheets, allowing direct comparisons to the common industry standard of 0.1 mm lead equivalent material. The attenuation properties of both types of glovebox gloves vary with energy, making it difficult for manufacturers to claim lead equivalency across the entire energy range used at TA-55. The positions of materials' photon energy absorption edges, which are particularly important to improved attenuation performance, depending upon the choice of radiation energy range, are discussed. This effort contributes to the Los Alamos National Laboratory Continuous Improvement Program by improving the efficiency, cost effectiveness, and formality of glovebox operations.« less

Excess plutonium disposition: The deep borehole option

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

Ferguson, K.L.

1994-08-09

This report reviews the current status of technologies required for the disposition of plutonium in Very Deep Holes (VDH). It is in response to a recent National Academy of Sciences (NAS) report which addressed the management of excess weapons plutonium and recommended three approaches to the ultimate disposition of excess plutonium: (1) fabrication and use as a fuel in existing or modified reactors in a once-through cycle, (2) vitrification with high-level radioactive waste for repository disposition, (3) burial in deep boreholes. As indicated in the NAS report, substantial effort would be required to address the broad range of issues relatedmore » to deep bore-hole emplacement. Subjects reviewed in this report include geology and hydrology, design and engineering, safety and licensing, policy decisions that can impact the viability of the concept, and applicable international programs. Key technical areas that would require attention should decisions be made to further develop the borehole emplacement option are identified.« less

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

Leaching of plutonium from a radioactive waste glass by eight groundwaters from the western United States

USGS Publications Warehouse

Rees, T.F.; Cleveland, J.M.; Nash, K.L.

1985-01-01

The leachability of a radioactive waste glass formulated to Battelle Pacific Northwest Laboratory specification 80-270 has been studied using eight actual groundwaters with a range of chemical compositions as leachants. Waters collected from the Grande Ronde Basalt (Washington State) and from alluvial deposits in the Hualapai Valley (Arizona) were the most effective at removing plutonium from this glass. Leaching was shown to be incongruent; plutonium was removed from the glass more slowly than the overall glass matrix. The results of these experiments indicate the need to study the leachability of actual waste forms using the actual projected groundwaters that are most likely to come into contact with the waste should a radioactive waste repository be breached.

Biomedical aspects of natural and manufactured environmental radioactivity

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

Hodge, V.

1996-12-31

While weapons testing has altered natural radioactivity background, manufactured radioactivity in most parts of the world constitutes but a very small fraction of the total alpha, beta, and gamma radioactivity in soil, air, water, and the biota. For example, in the early 1970s, we found what appeared to be the highest natural concentration of radioactivity ever reported in fish while attempting to measure the manufactured plutonium ({sup 239}Pu and {sup 240}Pu) in organs of oceanic tuna. The natural alpha emitter polonium ({sup 210}Po) was discovered in the same organs at orders of magnitude higher concentrations. In particular, the caecum, whichmore » is a digestive organ composed of many small closed-ended sacs, contained concentrations of polonium as high as 79 pCi/g of wet tissue and lesser amounts of two manufactured isotopes: 0.0001 pCi/g of plutonium and 0.01 pCi/g of radiocesium ({sup 137}Cs). This equates to {approximately}80 rem/yr of radiation dose to this organ, overwhelmingly from the natural polonium, or {approximately}5000 times higher than is found in the human liver, the highest polonium concentration in man. The average background radiation for humans, for comparison, is {approximately}0.2 rem/yr, but the dose for Japanese, whose diet is high in seafood, is {approximately}15 rem/yr. The question arose: {open_quotes}Are these high concentrations of natural polonium limited to oceanic fish?{close_quotes} To answer this question, polonium was determined in the organs of striped bass and catfish from Lake Mead. In a related study, the plutonium and radiocesium ({sup 137}Cs) distributions in soils were determined to ascertain the impact of weapons testing on the natural background radioactivity of soils.« less

Plutonium activities and 240Pu/ 239Pu atom ratios in sediment cores from the east China sea and Okinawa Trough: Sources and inventories

NASA Astrophysics Data System (ADS)

Wang, Zhong-liang; Yamada, Masatoshi

2005-05-01

Plutonium concentrations and 240Pu/ 239Pu atom ratios in the East China Sea and Okinawa Trough sediment cores were determined by isotope dilution inductively coupled plasma mass spectrometry after separation using ion-exchange chromatography. The results showed that 240Pu/ 239Pu atom ratios in the East China Sea and Okinawa Trough sediments, ranging from 0.21 to 0.33, were much higher than the reported value of global fallout (0.18). The highest 240Pu/ 239Pu ratios (0.32-0.33) were observed in the deepest Okinawa Trough sediment samples. These ratios suggested the US nuclear weapons tests in the early 1950s at the Pacific Proving Grounds in the Marshall Islands were a major source of plutonium in the East China Sea and Okinawa Trough sediments, in addition to the global fallout source. It was proposed that close-in fallout plutonium was delivered from the Pacific Proving Grounds test sites via early direct tropospheric fallout and transportation by the North Pacific Equatorial Circulation system and Kuroshio Current into the Okinawa Trough and East China Sea. The total 239 + 240 Pu inventories in the cores were about 150-200% of that expected from direct global fallout; about 46-67% of the total inventories were delivered from the Pacific Proving Grounds. Much higher 239 + 240 Pu inventories were observed in the East China Sea sediments than in sediments of the Okinawa Trough, because in the open oceans, part of the 239 + 240 Pu was still retained in the water column, and continued Pu scavenging was higher over the margin than the trough. According to the vertical distributions of 239 + 240 Pu activities and 240Pu/ 239Pu atom ratios in these cores, it was concluded that sediment mixing was the dominant process in controlling profiles of plutonium in this area. Faster mixing in the coastal samples has homogenized the entire 240Pu/ 239Pu ratio record today; slightly slower mixing and less scavenging in the Okinawa Trough have left the surface sediment ratios closer to the modern North Pacific water end member and higher ratios (0.30-0.34) at the bottom of the cores.

Development of Metallic Magnetic Calorimeters for Nuclear Safeguards Applications

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

Bates, Cameron Russell

2015-03-11

Many nuclear safeguards applications could benefit from high-resolution gamma-ray spectroscopy achievable with metallic magnetic calorimeters. This dissertation covers the development of a system for these applications based on gamma-ray detectors developed at the University of Heidelberg. It demonstrates new calorimeters of this type, which achieved an energy resolution of 45.5 eV full-width at half-maximum at 59.54 keV, roughly ten times better than current state of the art high purity germanium detectors. This is the best energy resolution achieved with a gamma-ray metallic magnetic calorimeter at this energy to date. In addition to demonstrating a new benchmark in energy resolution, anmore » experimental system for measuring samples with metallic magnetic calorimeters was constructed at Lawrence Livermore National Laboratory. This system achieved an energy resolution of 91.3 eV full-width at half-maximum at 59.54 keV under optimal conditions. Using this system it was possible to characterize the linearity of the response, the count-rate limitations, and the energy resolution as a function of temperature of the new calorimeter. With this characterization it was determined that it would be feasible to measure 242Pu in a mixed isotope plutonium sample. A measurement of a mixed isotope plutonium sample was performed over the course of 12 days with a single two-pixel metallic magnetic calorimeter. The relative concentration of 242Pu in comparison to other plutonium isotopes was determined by direct measurement to less than half a percent accuracy. This is comparable with the accuracy of the best-case scenario using traditional indirect methods. The ability to directly measure the relative concentration of 242Pu in a sample could enable more accurate accounting and detection of indications of undeclared activities in nuclear safeguards, a better constraint on source material in forensic samples containing plutonium, and improvements in verification in a future plutonium disposition treaty.« less

Goethite colloid enhanced Pu transport through a single saturated fracture in granite.

PubMed

Lin, Jianfeng; Dang, Haijun; Xie, Jinchuan; Li, Mei; Zhou, Guoqing; Zhang, Jihong; Zhang, Haitao; Yi, Xiaowei

2014-08-01

α-FeOOH, a stable iron oxide in nature, can strongly absorb the low-solubility plutonium (Pu) in aquifers. However, whether Pu transports though a single saturated fracture can be enhanced in the presence of α-FeOOH colloids remains unknown. Experimental studies were carried out to evaluate Pu mobilization at different water flow velocity, as affected by goethite colloids with various concentrations. Goethite nanorods were used to prepare (α-FeOOH)-associated Pu suspensions with α-FeOOH concentration of (0-150) mgL(-1). The work experimentally evidenced that α-FeOOH colloid does enhance transport of Pu through fractured granites. The fraction of mobile (239)Pu (RPu, m=41.5%) associated with the α-FeOOH of an extremely low colloid concentration (0.2mgL(-1)) is much larger than that in absence of α-FeOOH (RPu, m=6.98%). However, plutonium mobility began to decrease when α-FeOOH concentration was increased to 1.0mgL(-1). On the other hand, the fraction of mobile Pu increased gradually with the water flow velocity. Based on the experimental data, the mechanisms underlying the (α-FeOOH)-associated plutonium transport are comprehensively discussed in view of its dynamic deposition onto the granite surfaces, which is decided mainly by the relative interaction between the colloid particle and the immobile surface. This interaction is a balance of electrostatic force (may be repulsive or attractive), the van der Walls force, and the shear stress of flow. Copyright © 2014 Elsevier B.V. All rights reserved.

DISSOLVED CONCENTRATION LIMITS OF RADIOACTIVE ELEMENTS

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

P. Bernot

The purpose of this study is to evaluate dissolved concentration limits (also referred to as solubility limits) of elements with radioactive isotopes under probable repository conditions, based on geochemical modeling calculations using geochemical modeling tools, thermodynamic databases, field measurements, and laboratory experiments. The scope of this activity is to predict dissolved concentrations or solubility limits for elements with radioactive isotopes (actinium, americium, carbon, cesium, iodine, lead, neptunium, plutonium, protactinium, radium, strontium, technetium, thorium, and uranium) relevant to calculated dose. Model outputs for uranium, plutonium, neptunium, thorium, americium, and protactinium are provided in the form of tabulated functions with pH andmore » log fCO{sub 2} as independent variables, plus one or more uncertainty terms. The solubility limits for the remaining elements are either in the form of distributions or single values. Even though selection of an appropriate set of radionuclides documented in Radionuclide Screening (BSC 2002 [DIRS 160059]) includes actinium, transport of Ac is not modeled in the total system performance assessment for the license application (TSPA-LA) model because of its extremely short half-life. Actinium dose is calculated in the TSPA-LA by assuming secular equilibrium with {sup 231}Pa (Section 6.10); therefore, Ac is not analyzed in this report. The output data from this report are fundamental inputs for TSPA-LA used to determine the estimated release of these elements from waste packages and the engineered barrier system. Consistent modeling approaches and environmental conditions were used to develop solubility models for the actinides discussed in this report. These models cover broad ranges of environmental conditions so they are applicable to both waste packages and the invert. Uncertainties from thermodynamic data, water chemistry, temperature variation, and activity coefficients have been quantified or otherwise addressed.« less

Neutralization of Plutonium and Enriched Uranium Solutions Containing Gadolinium as a Neutron Poison

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

BRONIKOWSKI, MG.

2004-04-01

Materials currently being dissolved in the HB-Line Facility will result in an accumulated solution containing an estimated uranium:plutonium (U:Pu) ratio of 4.3:1 and an 235U enrichment estimated at 30 per cent The U:Pu ratio and the enrichment are outside the evaluated concentration range for disposition to high level waste (HLW) using gadolinium (Gd) as a neutron poison. To confirm that the solution generated during the current HB-Line dissolving campaign can be poisoned with Gd, neutralized and discarded to the Savannah River Site (SRS) high level waste (HLW) system without undue nuclear safety concerns the caustic precipitation of surrogate solutions wasmore » examined. Experiments were performed with a U/Pu/Gd solution representative of the HB-Line estimated concentration ratio and also a U/Gd solution. Depleted U was used in the experiments as the enrichment of the U will not affect the chemical behavior during neutralization, but will affect the amount of Gd added to the solution. Settling behavior of the neutralized solutions was found to be comparable to previous studies. The neutralized solutions mixed easily and had expected densities of typical neutralized waste. The neutralized solids were found to be homogeneous and less than 20 microns in size. Partially neutralized solids were more amorphous than the fully neutralized solids. Based on the results of these experiments, Gd was found to be a viable poison for neutralizing a U/Pu/Gd solution with a U:Pu mass ratio of 4.3:1 thus extending the U:Pu mass ratio from the previously investigated 0-3:1 to 4.3:1. However, further work is needed to allow higher U concentrations or U:Pu ratios greater than investigated in this work.« less

Depth profiling of Pu, 241Am and 137Cs in soils from southern Belarus measured by ICP-MS and alpha and gamma spectrometry.

PubMed

Boulyga, Sergei F; Zoriy, Myroslav; Ketterer, Michael E; Becker, J Sabine

2003-08-01

The depth distribution of plutonium, americium, and 137Cs originating from the 1986 accident at the Chernobyl Nuclear Power Plant (NPP) was investigated in several soil profiles in the vicinity from Belarus. The vertical migration of transuranic elements in soils typical of the 30 km relocation area around Chernobyl NPP was studied using inductively coupled plasma mass spectrometry (ICP-MS), alpha spectrometry, and gamma spectrometry. Transuranic concentrations in upper soil layers ranged from 6 x 10(-12) g g(-1) to 6 x 10(-10) g g(-1) for plutonium and from 1.8 x 10(-13) g g(-1) to 1.6 x 10(-11) g g(-1) for americium. These concentrations correspond to specific activities of (239+240)Pu of 24-2400 Bq kg(-1) and specific activity of 241Am of 23-2000 Bq kg(-1), respectively. Transuranics in turf-podzol soil migrate slowly to the deeper soil layers, thus, 80-95%, of radionuclide inventories were present in the 0-3 cm intervals of turf-podzol soils collected in 1994. In peat-marsh soil migration processes occur more rapidly than in turf-podzol and the maximum concentrations are found beneath the soil surface (down to 3-6 cm). The depth distributions of Pu and Am are essentially identical for a given soil profile. (239+240)Pu/137Cs and 241Am/137Cs activity ratios vary by up to a factor of 5 at some sites while smaller variations in these ratios were observed at a site close to Chernobyl, suggesting that 137Cs is dominantly particle associated close to Chernobyl but volatile species of 137Cs are of relatively greater importance at the distant sites.

Plutonium(IV) and (V) sorption to goethite at sub-femtomolar to micromolar concentrations: Redox transformations and surface precipitation

DOE PAGES

Zhao, Pihong; Begg, James D.; Zavarin, Mavrik; ...

2016-06-06

Here, Pu(IV) and Pu(V) sorption to goethite was investigated over a concentration range of 10 –15–10 –5 M at pH 8. Experiments with initial Pu concentrations of 10 –15 – 10 –8 M produced linear Pu sorption isotherms, demonstrating that Pu sorption to goethite is not concentration-dependent across this concentration range. Equivalent Pu(IV) and Pu(V) sorption Kd values obtained at 1 and 2-week sampling time points indicated that Pu(V) is rapidly reduced to Pu(IV) on the goethite surface. Further, it suggested that Pu surface redox transformations are sufficiently rapid to achieve an equilibrium state within 1 week, regardless of themore » initial Pu oxidation state. At initial concentrations >10 –8 M, both Pu oxidation states exhibited deviations from linear sorption behavior and less Pu was adsorbed than at lower concentrations. NanoSIMS and HRTEM analysis of samples with initial Pu concentrations of 10 –8 – 10 –6 M indicated that Pu surface and/or bulk precipitation was likely responsible for this deviation. In 10 –6 M Pu(IV) and Pu(V) samples, HRTEM analysis showed the formation of a body centered cubic (bcc) Pu 4O 7 structure on the goethite surface, confirming that reduction of Pu(V) had occurred on the mineral surface and that epitaxial distortion previously observed for Pu(IV) sorption occurs with Pu(V) as well.« less

DISSOLUTION OF PLUTONIUM METAL IN 8-10 M NITRIC ACID

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

Rudisill, T.; Pierce, R.

2012-02-21

The H-Canyon facility will be used to dissolve Pu metal for subsequent purification and conversion to plutonium dioxide (PuO{sub 2}) using Phase II of HB-Line. To support the new mission, the development of a Pu metal dissolution flowsheet which utilizes concentrated (8-10 M) nitric acid (HNO{sub 3}) solutions containing potassium fluoride (KF) is required. Dissolution of Pu metal in concentrated HNO{sub 3} is desired to eliminate the need to adjust the solution acidity prior to purification by anion exchange. The preferred flowsheet would use 8-10 M HNO{sub 3}, 0.015-0.07 M KF, and 0.5-1.0 g/L Gd to dissolve the Pu upmore » to 6.75 g/L. An alternate flowsheet would use 8-10 M HNO{sub 3}, 0.1-0.2 M KF, and 1-2 g/L B to dissolve the Pu. The targeted average Pu metal dissolution rate is 20 mg/min-cm{sup 2}, which is sufficient to dissolve a 'standard' 2250-g Pu metal button in 24 h. Plutonium metal dissolution rate measurements showed that if Gd is used as the nuclear poison, the optimum dissolution conditions occur in 10 M HNO{sub 3}, 0.04-0.05 M KF, and 0.5-1.0 g/L Gd at 112 to 116 C (boiling). These conditions will result in an estimated Pu metal dissolution rate of {approx}11-15 mg/min-cm{sup 2} and will result in dissolution times of 36-48 h for standard buttons. The recommended minimum and maximum KF concentrations are 0.03 M and 0.07 M, respectively. The maximum KF concentration is dictated by a potential room-temperature Pu-Gd-F precipitation issue at low Pu concentrations. The purpose of the experimental work described in this report was two-fold. Initially a series of screening experiments was performed to measure the dissolution rate of Pu metal as functions of the HNO{sub 3}, KF, and Gd or B concentrations. The objective of the screening tests was to propose optimized conditions for subsequent flowsheet demonstration tests. Based on the rate measurements, this study found that optimal dissolution conditions in solutions containing 0.5-1.0 g/L Gd occurred in 8-10 M HNO{sub 3} with 0.04-0.05 M KF at 112 to 116 C (boiling). The testing also showed that solutions containing 8-10 M HNO{sub 3}, 0.1-0.2 M KF, and 1-2 g/L B achieved acceptable dissolution rates in the same temperature range. To confirm that conditions identified by the dissolution rate measurements for solutions containing Gd or B can be used to dissolve Pu metal up to 6.75 g/L in the presence of Fe, demonstration experiments were performed using concentrations in the optimal ranges. In two of the demonstration experiments using Gd and in one experiment using B, the offgas generation during the dissolution was measured and samples were analyzed for H{sub 2}. The experimental methods used to perform the dissolution rate measurements and flowsheet demonstrations and a discussion of the results are presented.« less

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

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

NASA Astrophysics Data System (ADS)

Manara, D.; De Bruycker, F.; Boboridis, K.; Tougait, O.; Eloirdi, R.; Malki, M.

2012-07-01

In this work, an experimental study of the radiance of liquid and solid uranium and plutonium carbides at wavelengths 550 nm ⩽ λ ⩽ 920 nm is reported. A fast multi-channel spectro-pyrometer has been employed for the radiance measurements of samples heated up to and beyond their melting point by laser irradiation. The melting temperature of uranium monocarbide, soundly established at 2780 K, has been taken as a radiance reference. Based on it, a wavelength-dependence has been obtained for the high-temperature spectral emissivity of some uranium carbides (1 ⩽ C/U ⩽ 2). Similarly, the peritectic temperature of plutonium monocarbide (1900 K) has been used as a reference for plutonium monocarbide and sesquicarbide. The present spectral emissivities of solid uranium and plutonium carbides are close to 0.5 at 650 nm, in agreement with previous literature values. However, their high temperature behaviour, values in the liquid, and carbon-content and wavelength dependencies in the visible-near infrared range have been determined here for the first time. Liquid uranium carbide seems to interact with electromagnetic radiation in a more metallic way than does the solid, whereas a similar effect has not been observed for plutonium carbides. The current emissivity values have also been used to convert the measured radiance spectra into real temperature, and thus perform a thermal analysis of the laser heated samples. Some high-temperature phase boundaries in the systems U-C and Pu-C are shortly discussed on the basis of the current results.

Transport of plutonium in snowmelt run-off

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

Purtymun, W.D.; Peters, R.; Maes, M.N.

1990-07-01

Plutonium in treated low-level radioactive effluents released into intermittent streams is bound by ion exchange or adsorption to bed sediments in the stream channel. These sediments are subject to transport with summer and spring snowmelt run-off. A study was made of the transport of plutonium during seven spring run-off events in Los Alamos and Pueblo canyons from the Laboratory boundary to Otowi on the Rio Grande. The melting of the snowpack during these years resulted in run-off that was large enough to reach the eastern edge of the Laboratory. Of these seven run-off events recorded at the Laboratory boundary, onlymore » five had sufficient flow to reach the Rio Grande. The volume of the five events that reached the river ranged from 5 {times} 10{sup 3} m{sup 3} to 104 {times} 10{sup 3} m{sup 3}. The five run-off events carried 119 {times} 10{sup 3} kg of suspended sediments and 1073 {times} 10{sup 3} kg of bed sediments, and transported 598 {mu}Ci of plutonium to the river. Of the 598 {mu}Ci of plutonium, 3% was transported in solution, 57% with suspended sediments, and 40% with bed sediments. 13 refs., 3 figs., 6 tabs.« less

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

A high converter concept for fuel management with blanket fuel assemblies in boiling water reactors

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

Martinez-Frances, N.; Timm, W.; Rossbach, D.

2012-07-01

Studies on the natural Uranium saving and waste reduction potential of a multiple-plant BWR system were performed. The BWR High Converter system should enable a multiple recycling of MOX fuel in current BWR plants by introducing blanket fuel assemblies and burning Uranium and MOX fuel separately. The feasibility of Uranium cores with blankets and full-MOX cores with Plutonium qualities as low as 40% were studied. The power concentration due to blanket insertion is manageable with modern fuel and acceptable values for the thermal limits and reactivity coefficients were obtained. While challenges remain, full-MOX cores also complied with the main designmore » criteria. The combination of Uranium and Plutonium burners in appropriate proportions could enable obtaining as much as 40% more energy out of Uranium ore. Moreover, a proper adjustment of blanket average stay and Plutonium qualities could lead to a system with nearly no Plutonium left for final disposal. The achievement of such goals with current light water technology makes the BWR HC concept an attractive option to improve the fuel cycle until Gen-IV designs are mature. (authors)« less

Risk Assessment for Emergency Planning Related to Nuclear Weapons Accidents

DTIC Science & Technology

1985-09-25

accidents is higher than many of the other accidents, several reviewers thought it appropriate to evaluate these accidents in more detail. In particular, it...consequences is presented in Table 2-5. The plutonium releases in the 1F-3F gram range are due to plutonium burning in Type A weapons, while the higher ...explosion given a tanker casualty varies from 0.05 (in harbor) to 0.16 (at pier) to 0.19 (at sea). Although these numbers are somewhat higher than the

PU-ICE Summary Information.

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

Moore, Michael

The Generator Knowledge Report for the Plutonium Isentropic Compression Experiment Containment Systems (GK Report) provides information for the Plutonium Isentropic Compression Experiment (Pu- ICE) program to support waste management and characterization efforts. Attachment 3-18 presents generator knowledge (GK) information specific to the eighteenth Pu-ICE conducted in August 2015, also known as ‘Shot 18 (Aug 2015) and Pu-ICE Z-2841 (1).’ Shot 18 (Aug 2015) was generated on August 28, 2015 (1). Calculations based on the isotopic content of Shot 18 (Aug 2015) and the measured mass of the containment system demonstrate the post-shot containment system is low-level waste (LLW). Therefore, thismore » containment system will be managed at Sandia National Laboratory/New Mexico (SNL/NM) as LLW. Attachment 3-18 provides documentation of the TRU concentration and documents the concentration of any hazardous constituents.« less

CONCENTRATION OF Pu USING OXALATE TYPE CARRIER

DOEpatents

Ritter, D.M.; Black, R.P.S.

1960-04-19

A method is given for dissolving and reprecipitating an oxalate carrier precipitate in a carrier precipitation process for separating and recovering plutonium from an aqueous solution. Uranous oxalate, together with plutonium being carried thereby, is dissolved in an aqueous alkaline solution. Suitable alkaline reagents are the carbonates and oxulates of the alkali metals and ammonium. An oxidizing agent selected from hydroxylamine and hydrogen peroxide is then added to the alkaline solution, thereby oxidizing uranium to the hexavalent state. The resulting solution is then acidified and a source of uranous ions provided in the acidified solution, thereby forming a second plutoniumcarrying uranous oxalate precipitate.

Supercritical Fluid Extraction and Separation of Uranium from Other Actinides

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

Donna L. Quach; Bruce J. Mincher; Chien M. Wai

2014-06-01

This paper investigates the feasibility of separating uranium from other actinides by using supercritical fluid carbon dioxide (sc-CO2) as a solvent modified with tri-n-butylphosphate (TBP) for the development of an extraction and counter current stripping technique, which would be a more efficient and environmentally benign technology for used nuclear fuel reprocessing compared to traditional solvent extraction. Several actinides (U(VI), Np(VI), Pu(IV), and Am(III)) were extracted in sc-CO2 modified with TBP over a range of nitric acid concentrations and then the actinides were exposed to reducing and complexing agents to suppress their extractability. According to this study, the separation of uraniummore » from plutonium in sc-CO2 modified with TBP was successful at nitric acid concentrations of less than 3 M in the presence of acetohydroxamic acid or oxalic acid, and the separation of uranium from neptunium was successful at nitric acid concentrations of less than 1 M in the presence of acetohydroxamic acid, oxalic acid, or sodium nitrite.« less

Determination of 241Pu in low-level radioactive wastes from reactors.

PubMed

Martin, J E

1986-11-01

Plutonium-241 is unique in low-level radioactive wastes (LLW) from nuclear power plants because it is the only significant beta-emitting transuranic nuclide in LLW, has a relatively short half-life of 14.4 y, and has a fairly high allowable concentration for shallow land burial. Radiochemical separation of Pu followed by liquid scintillation analysis was used to quantitate 241Pu in a wide range of solid, semi-solid, and liquid LLW samples from two nuclear plants in Michigan. The 241Pu concentrations varied considerably by sample type and reactor operational period as did their correlation with 137Cs, 144Ce, 239Pu and 240Pu concentrations in the same sample. These patterns were also found in reported data for 241Pu in LLW from other reactors, raising the difficulty of accurately determining the inventory (or source term) in a LLW shallow land burial site and its implications for predicting and controlling the future environmental and public health impacts of such disposal.

Location analysis and strontium-90 concentrations in deer antlers on the Hanford Site

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

Tiller, B L; Eberhardt, L E; Poston, T M

1995-05-01

The primary objective of this study was to examine the levels of strontium-90 ({sup 90}Sr) in deer antlers collected from near previously active reactor sites and distant from the reactor sites along that portion of the Columbia River which borders the Hanford Site. A second objective was to analyze the movements and home-ranges of mule deer residing within these areas and determine to what extent this information contributes to the observed {sup 90}Sr concentrations. {sup 90}Sr is a long-lived radionuclide (29.1 year half life) produced by fission in irradiated fuel in plutonium production reactors on the Hanford Site. It ismore » also a major component of atmospheric fallout from weapons testing. Concentrations of radionuclides found in the developed environment onsite do not pose a health concern to humans or various wildlife routinely monitored. However, elevated levels of radionuclides in found biota may indicate routes of exposure requiring attention.« less

Cleaning up the Legacy of the Cold War: Plutonium Oxides and the Role of Synchrotron Radiation Research

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

Clark, David Lewis

2015-01-21

The deceptively simple binary formula of AnO 2 belies an incredibly complex structural nature, and propensity to form mixed-valent, nonstoichiometric phases of composition AnO 2±x. For plutonium, the very formation of PuO 2+x has challenged a long-established dogma, and raised fundamental questions for long-term storage and environmental migration. This presentation covers two aspects of Los Alamos synchrotron radiation studies of plutonium oxides: (1) the structural chemistry of laboratory-prepared AnO 2+x systems (An = U, Pu; 0 ≤ x ≤ 0.25) determined through a combination of x-ray absorption fine structure spectroscopy (XAFS) and x-ray scattering of laboratory prepared samples; and (2)more » the application of synchrotron radiation towards the decontamination and decommissioning of the Rocky Flats Environmental Technology Site. Making the case for particle transport mechanisms as the basis of plutonium and americium mobility, rather than aqueous sorption-desorption processes, established a successful scientific basis for the dominance of physical transport processes by wind and water. The scientific basis was successful because it was in agreement with general theory on insolubility of PuO 2 in oxidation state IV, results of ultrafiltration analyses of field water/sediment samples, XAFS analyses of soil, sediment, and concrete samples, and was also in general agreement with on-site monitoring data. This understanding allowed Site contractors to rapidly move to application of soil erosion and sediment transport models as the means of predicting plutonium and americium transport, which led to design and application of site-wide soil erosion control technology to help control downstream concentrations of plutonium and americium in streamflow.« less

Gaseous and particulate emissions from a DC arc melter.

PubMed

Overcamp, Thomas J; Speer, Matthew P; Griner, Stewart J; Cash, Douglas M

2003-01-01

Tests treating soils contaminated with metal compounds and radionuclide surrogates were conducted in a DC arc melter. The soil melted, and glassy or ceramic waste forms with a separate metal phase were produced. Tests were run in the melter plenum with either air or N2 purge gases. In addition to nitrogen, the primary emissions of gases were CO2, CO, oxygen, methane, and oxides of nitrogen (NO(x)). Although the gas flow through the melter was low, the particulate concentrations ranged from 32 to 145 g/m3. Cerium, a nonradioactive surrogate for plutonium and uranium, was not enriched in the particulate matter (PM). The PM was enriched in cesium and highly enriched in lead.

APPROACHING CRYOGENIC GE PERFORMANCE WITH PELTIER COOLED CDTE

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

Khusainov, A. K.; Iwanczyk, J. S.; Patt, B. E.

A new class of hand-held, portable spectrometers based on large area (lcm2) CdTe detectors of thickness up to 3mm has been demonstrated to produce energy resolution of between 0.3 and 0.5% FWHM at 662 keV. The system uses a charge loss correction circuit for improved efficiency, and detector temperature stabilization to ensure consistent operation of the detector during field measurements over a wide range of ambient temperature. The system can operate continuously for up to 8hrs on rechargeable batteries. The signal output from the charge loss corrector is compatible with most analog and digital spectroscopy amplifiers and multi channel analyzers.more » Using a detector measuring 11.2 by 9.1 by 2.13 mm3, we have recently been able to obtain the first wide-range plutonium gamma-ray isotopic analysis with other than a cryogenically cooled germanium spectrometer. The CdTe spectrometer is capable of measuring small plutonium reference samples in about one hour, covering the range from low to high burnup. The isotopic analysis software used to obtain these results was FRAM, Version 4 from LANL. The new spectrometer is expected to be useful for low-grade assay, as well as for some in-situ plutonium gamma-ray isotopics in lieu of cryogenically cooled Ge.« less

Assessment of the global fallout of plutonium isotopes and americium-241 in the soil of the central region of Saudi Arabia.

PubMed

Shabana, E I; Al-Shammari, H L

2001-01-01

A radiochemical technique for determination of plutonium isotopes and 241Am in soil samples is tested against IAEA-standard reference materials to determine its accuracy and precision for reliable results. The technique is then used in the investigation of topsoil samples, collected from the natural environment of the central region of Saudi Arabia, to assess the effect of fallout accumulation of these radionuclides in the region. Plutonium and americium were sequentially separated from all other components of the sample by anion-exchange chromatography and co-precipitated with Nd3+ as fluorides. The precipitates were mounted on membrane filters and measured using a high-resolution alpha-spectrometer. The results of the analysis of the reference materials showed satisfactory sensitivity and precision of the technique. The results of the analyzed soil samples show activity levels ranging from < LLD to 0.089 and from

Analysis of the 2H-evaporator scale samples (HTF-17-56, -57)

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

Hay, M.; Coleman, C.; Diprete, D.

Savannah River National Laboratory analyzed scale samples from both the wall and cone sections of the 242-16H Evaporator prior to chemical cleaning. The samples were analyzed for uranium and plutonium isotopes required for a Nuclear Criticality Safety Assessment of the scale removal process. The analysis of the scale samples found the material to contain crystalline nitrated cancrinite and clarkeite. Samples from both the wall and cone contain depleted uranium. Uranium concentrations of 16.8 wt% 4.76 wt% were measured in the wall and cone samples, respectively. The ratio of plutonium isotopes in both samples is ~85% Pu-239 and ~15% Pu-238 bymore » mass and shows approximately the same 3.5 times higher concentration in the wall sample versus the cone sample as observed in the uranium concentrations. The mercury concentrations measured in the scale samples were higher than previously reported values. The wall sample contains 19.4 wt% mercury and the cone scale sample 11.4 wt% mercury. The results from the current scales samples show reasonable agreement with previous 242-16H Evaporator scale sample analysis; however, the uranium concentration in the current wall sample is substantially higher than previous measurements.« less

ELECTRONICS UPGRADE TO THE SAVANNAH RIVER NATIONAL LABORATORY COULOMETER FOR PLUTONIUM AND NEPTUNIUM ASSAY

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

Cordaro, J.; Holland, M.; Reeves, G.

The Savannah River Site (SRS) has the analytical measurement capability to perform high-precision plutonium concentration measurements by controlled-potential coulometry. State-of-the-art controlled-potential coulometers were designed and fabricated by the Savannah River National Laboratory and installed in the Analytical Laboratories process control laboratory. The Analytical Laboratories uses coulometry for routine accountability measurements of and for verification of standard preparations used to calibrate other plutonium measurement systems routinely applied to process control, nuclear safety, and other accountability applications. The SRNL Coulometer has a demonstrated measurement reliability of {approx}0.05% for 10 mg samples. The system has also been applied to the characterization of neptuniummore » standard solutions with a comparable reliability. The SRNL coulometer features: a patented current integration system; continuous electrical calibration versus Faraday's Constants and Ohm's Law; the control-potential adjustment technique for enhanced application of the Nernst Equation; a wide operating room temperature range; and a fully automated instrument control and data acquisition capability. Systems have been supplied to the International Atomic Energy Agency (IAEA), Russia, Japanese Atomic Energy Agency (JAEA) and the New Brunswick Laboratory (NBL). The most recent vintage of electronics was based on early 1990's integrated circuits. Many of the components are no longer available. At the request of the IAEA and the Department of State, SRNL has completed an electronics upgrade of their controlled-potential coulometer design. Three systems have built with the new design, one for the IAEA which was installed at SAL in May 2011, one system for Los Alamos National Laboratory, (LANL) and one for the SRS Analytical Laboratory. The LANL and SRS systems are undergoing startup testing with installation scheduled for this summer.« less

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

Plutonium in the WIPP environment: its detection, distribution and behavior.

PubMed

Thakur, P; Ballard, S; Nelson, R

2012-05-01

The Waste Isolation Pilot Plant (WIPP) is the only operating deep underground geologic nuclear repository in the United States. It is located in southeastern New Mexico, approximately 655 m (2150 ft) below the surface of the Earth in a bedded Permian evaporite salt formation. This mined geologic repository is designed for the safe disposal of transuranic (TRU) wastes generated from the US defense program. Aerosol and soil samples have been collected near the WIPP site to investigate the sources of plutonium in the WIPP environment since the late 1990s, well before WIPP received its first shipment. Activities of (238)Pu, (239+240)Pu and (241)Am were determined by alpha spectrometry following a series of chemical separations. The concentrations of Al and U were determined in a separate set of samples by inductively coupled plasma mass spectrometry. The annual airborne concentrations of (239+240)Pu during the period from 1998 to 2010 show no systematic interannual variations. However, monthly (239+240)Pu particulate concentrations show a typical seasonal variation with a maximum in spring, the time when strong and gusty winds frequently give rise to blowing dust. Resuspension of soil particles containing weapons fallout is considered to be the predominant source of plutonium in the WIPP area. Further, this work characterizes the source, temporal variation and its distribution with depth in a soil profile to evaluate the importance of transport mechanisms affecting the fate of these radionuclides in the WIPP environment. The mean (137)Cs/(239+240)Pu, (241)Am/(239+240)Pu activity ratio and (240)Pu/(239)Pu atom ratio observed in the WIPP samples are consistent with the source being largely global fallout. There is no evidence of any release from the WIPP contributing to radionuclide concentrations in the environment.

Assessment of need for transport tubes when continuously monitoring for radioactive aerosols.

PubMed

Whicker, J J; Rodgers, J C; Lopez, R C

1999-09-01

Aerosol transport tubes are often used to draw aerosol from desirable sampling locations to nearby air sampling equipment that cannot be placed at that location. In many plutonium laboratories at Los Alamos National Laboratory, aerosol transport tubes are used to transport aerosol from the front of room ventilation exhaust registers to continuous air monitors (CAMs) that are mounted on nearby walls. Transport tubes are used because past guidance suggests that extraction of aerosol samples from exhaust locations provides the most sensitive and reliable detection under conditions where the rooms have unpredictable release locations and significant spatial variability in aerosol concentrations after releases, and where CAMs cannot be located in front of exhaust registers without blocking worker walkways. Despite designs to minimize particle loss in tubes, aerosol transport model predictions suggest losses occur lowering the sensitivity of CAMs to accidentally released plutonium aerosol. The goal of this study was to test the hypotheses that the reliability, speed, and sensitivity of aerosol detection would be equal whether the sample was extracted from the front of the exhaust register or from the wall location of CAMs. Polydisperse oil aerosols were released from multiple locations in two plutonium laboratories to simulate plutonium aerosol releases. Networked laser particle counters (LPCs) were positioned to simultaneously measure time-resolved aerosol concentrations at each exhaust register (representative of sampling with transport tubes) and at each wall-mounted CAM location (representative of sampling without transport tubes). Results showed no significant differences in detection reliability, speed, or sensitivity for LPCs positioned at exhaust locations when compared to LPCs positioned at the CAM wall location. Therefore, elimination of transport tubes would likely improve CAM performance.

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

PubMed

Griffiths, N M; Van der Meeren, A; Fritsch, P; Abram, M-C; Bernaudin, J-F; Poncy, J L

2010-09-01

Accidental exposure by inhalation to alpha-emitting particles from mixed oxide (MOX: uranium and plutonium oxide) fuels is a potential long-term health risk to workers in nuclear fuel fabrication plants. For MOX fuels, the risk of lung cancer development may be different from that assigned to individual components (plutonium, uranium) given different physico-chemical characteristics. The objective of this study was to investigate late effects in rat lungs following inhalation of MOX aerosols of similar particle size containing 2.5 or 7.1% plutonium. Conscious rats were exposed to MOX aerosols and kept for their entire lifespan. Different initial lung burdens (ILBs) were obtained using different amounts of MOX. Lung total alpha activity was determined by external counting and at autopsy for total lung dose calculation. Fixed lung tissue was used for anatomopathological, autoradiographical, and immunohistochemical analyses. Inhalation of MOX at ILBs ranging from 1-20 kBq resulted in lung pathologies (90% of rats) including fibrosis (70%) and malignant lung tumors (45%). High ILBs (4-20 kBq) resulted in reduced survival time (N = 102; p < 0.05) frequently associated with lung fibrosis. Malignant tumor incidence increased linearly with dose (up to 60 Gy) with a risk of 1-1.6% Gy for MOX, similar to results for industrial plutonium oxide alone (1.9% Gy). Staining with antibodies against Surfactant Protein-C, Thyroid Transcription Factor-1, or Oct-4 showed differential labeling of tumor types. In conclusion, late effects following MOX inhalation result in similar risk for development of lung tumors as compared with industrial plutonium oxide.

Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics

PubMed Central

Booth, C.H.; Jiang, Yu; Wang, D.L.; Mitchell, J.N.; Tobash, P.H.; Bauer, E.D.; Wall, M.A.; Allen, P.G.; Sokaras, D.; Nordlund, D.; Weng, T.-C.; Torrez, M.A.; Sarrao, J.L.

2012-01-01

Uranium and plutonium’s 5f electrons are tenuously poised between strongly bonding with ligand spd-states and residing close to the nucleus. The unusual properties of these elements and their compounds (e.g., the six different allotropes of elemental plutonium) are widely believed to depend on the related attributes of f-orbital occupancy and delocalization for which a quantitative measure is lacking. By employing resonant X-ray emission spectroscopy (RXES) and X-ray absorption near-edge structure (XANES) spectroscopy and making comparisons to specific heat measurements, we demonstrate the presence of multiconfigurational f-orbital states in the actinide elements U and Pu and in a wide range of uranium and plutonium intermetallic compounds. These results provide a robust experimental basis for a new framework toward understanding the strongly-correlated behavior of actinide materials. PMID:22706643

13. Elevations, 233S, U.S. Atomic Energy Commission, Hanford Works, General ...

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

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

Method of uranium reclamation from aqueous systems by reactive ion exchange. [US DOE patent application; anion exchange resin of copolymerized divinyl-benzene and styrene having quarternary ammonium groups and bicarbonate ligands

DOEpatents

Maya, L.

1981-11-05

A reactive ion exchange method for separation and recovery of values of uranium, neptunium, plutonium, or americium from substantially neutral aqueous systems of said metals comprises contacting said system with an effective amount of a basic anion exchange resin of copolymerized divinyl-benzene and styrene having quarternary ammonium groups and bicarbonate ligands to achieve nearly 100% sorption of said actinyl ion onto said resin and an aqueous system practically free of said actinyl ions. The method is operational over an extensive range of concentrations from about 10/sup -6/ M to 1.0 M actinyl ion and a pH range of about 4 to 7. The method has particulr application to treatment of waste streams from Purex-type nuclear fuel reprocessing facilities and hydrometallurgical processes involving U, Np, P, or Am.

Hydrothermal Alteration of Glass from Underground Nuclear Tests: Formation and Transport of Pu-clay Colloids at the Nevada National Security Site

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

Zavarin, M.; Zhao, P.; Joseph, C.

2015-05-27

The testing of nuclear weapons at the Nevada National Security Site (NNSS), formerly the Nevada Test Site (NTS), has led to the deposition of substantial quantities of plutonium into the environment. Approximately 2.8 metric tons (3.1×10 4 TBq) of Pu were deposited in the NNSS subsurface as a result of underground nuclear testing. While 3H is the most abundant anthropogenic radionuclide deposited in the NNSS subsurface (4.7×10 6 TBq), plutonium is the most abundant from a molar standpoint. The only radioactive elements in greater molar abundance are the naturally occurring K, Th, and U isotopes. 239Pu and 240Pu represent themore » majority of alpha-emitting Pu isotopes. The extreme temperatures associated with underground nuclear tests and the refractory nature of Pu results in most of the Pu (98%) being sequestered in melted rock, referred to as nuclear melt glass (Iaea, 1998). As a result, Pu release to groundwater is controlled, in large part, by the leaching (or dissolution) of nuclear melt glass over time. The factors affecting glass dissolution rates have been studied extensively. The dissolution of Pu-containing borosilicate nuclear waste glasses at 90ºC has been shown to lead to the formation of dioctahedral smectite colloids. Colloid-facilitated transport of Pu at the NNSS has been observed. Recent groundwater samples collected from a number of contaminated wells have yielded a wide range of Pu concentrations from 0.00022 to 2.0 Bq/L. While Pu concentrations tend to fall below the Maximum Contaminant Level (MCL) established by the Environmental Protection Agency (EPA) for drinking water (0.56 Bq/L), we do not yet understand what factors limit the Pu concentration or its transport behavior. To quantify the upper limit of Pu concentrations produced as a result of melt glass dissolution and determine the nature of colloids and Pu associations, we performed a 3 year nuclear melt glass dissolution experiment across a range of temperatures (25-200 °C) that represent hydrothermal conditions representative of the underground nuclear test cavities (when groundwater has re-saturated the nuclear melt glass and glass dissolution occurs). Colloid loads and Pu concentrations were monitored along with the mineralogy of both the colloids and the secondary mineral phases. The intent was to establish an upper limit for Pu concentrations at the NNSS, provide context regarding the Pu concentrations observed at the NNSS to date and the Pu concentrations that may be observed in the future. The results provide a conceptual model for the risks posed by Pu migration at the NNSS.« less

CONVERSION OF PLUTONIUM TRIFLUORIDE TO PLUTONIUM TETRAFLUORIDE

DOEpatents

Fried, S.; Davidson, N.R.

1957-09-10

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

Sub-micron Hard X-ray Fluorescence Imaging of Synthetic Elements

PubMed Central

Jensen, Mark P.; Aryal, Baikuntha P.; Gorman-Lewis, Drew; Paunesku, Tatjana; Lai, Barry; Vogt, Stefan; Woloschak, Gayle E.

2013-01-01

Synchrotron-based X-ray fluorescence microscopy (SXFM) using hard X-rays focused into sub-micron spots is a powerful technique for elemental quantification and mapping, as well as microspectroscopic measurement such as μ-XANES (X-ray absorption near edge structure). We have used SXFM to image and simultaneously quantify the transuranic element plutonium at the L3 or L2 edge as well as lighter biologically essential elements in individual rat pheochromocytoma (PC12) cells after exposure to the long-lived plutonium isotope 242Pu. Elemental maps reveal that plutonium localizes principally in the cytoplasm of the cells and avoids the cell nucleus, which is marked by the highest concentrations of phosphorus and zinc, under the conditions of our experiments. The minimum detection limit under typical acquisition conditions for an average 202 μm2 cell is 1.4 fg Pu/cell or 2.9 × 10−20 moles Pu/μm2, which is similar to the detection limit of K-edge SXFM of transition metals at 10 keV. Copper electron microscopy grids were used to avoid interference from gold X-ray emissions, but traces of strontium present in naturally occurring calcium can still interfere with plutonium detection using its Lα X-ray emission. PMID:22444530

Closure Report for Corrective Action Unit 415: Project 57 No. 1 Plutonium Dispersion (NTTR) Nevada Test and Training Range, Nevada, Revision 0 with ROTC-1

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

Cabble, Kevin J.; Boehlecke, Robert F.

This Closure Report (CR) presents information supporting the closure of Corrective Action Unit (CAU) 415: Project 57 No. 1 Plutonium Dispersion, which is located on Range 4808A of the Nevada Test and Training Range (NTTR). This CR complies with the requirements of the Federal Facility Agreement and Consent Order (FFACO) that was agreed to by the State of Nevada; U.S. Department of Energy (DOE), Environmental Management; U.S. Department of Defense; and DOE, Legacy Management. CAU 415 comprises one corrective action site (CAS): NAFR-23-02, Pu Contaminated Soil. The purpose of this CR is to provide justification and documentation supporting the recommendationmore » that no further corrective action is needed for CAU 415 based on the implementation of the corrective action of Closure in Place.« less

Determination of the 240Pu/ 239Pu atomic ratio in soils from Palomares (Spain) by low-energy accelerator mass spectrometry

NASA Astrophysics Data System (ADS)

Chamizo, E.; García-León, M.; Synal, H.-A.; Suter, M.; Wacker, L.

2006-08-01

In 1966, the nuclear fuel of two thermonuclear bombs was released over the Spanish region of Palomares, due to a B52 bomber accident during a refuelling operation. Since then, much effort has been made to assess its impact to the different environmental compartments of this area in South-East Spain, mostly by measuring the 239+240Pu activity concentration and the 238Pu/239+240Pu activity ratio. Nevertheless, these measurements do not give enough information on the problem. In order to recognize unambiguously small traces of the weapon-grade plutonium released in the accident, the ratio of the two major isotopes of plutonium, 240Pu/239Pu, has to be determined. In this work, this ratio has been measured in low- and high-activity samples from Palomares by means of low-energy accelerator mass spectrometry (AMS). That way, we will show the potential of the new generation of compact AMS facilities in terms of plutonium characterization at ultra-trace levels.

Pyrochemical process for extracting plutonium from an electrolyte salt

DOEpatents

Mullins, L.J.; Christensen, D.C.

1982-09-20

A pyrochemical process for extracting plutonium from a plutonium-bearing salt is disclosed. The process is particularly useful in the recovery of plutonium for electrolyte salts which are left over from the electrorefining of plutonium. In accordance with the process, the plutonium-bearing salt is melted and mixed with metallic calcium. The calcium reduces ionized plutonium in the salt to plutonium metal, and also causes metallic plutonium in the salt, which is typically present as finely dispersed metallic shot, to coalesce. The reduced and coalesced plutonium separates out on the bottom of the reaction vessel as a separate metallic phase which is readily separable from the overlying salt upon cooling of the mixture. Yields of plutonium are typically on the order of 95%. The stripped salt is virtually free of plutonium and may be discarded to low-level waste storage.

Pyrochemical process for extracting plutonium from an electrolyte salt

DOEpatents

Mullins, Lawrence J.; Christensen, Dana C.

1984-01-01

A pyrochemical process for extracting plutonium from a plutonium-bearing salt is disclosed. The process is particularly useful in the recovery of plutonium from electrolyte salts which are left over from the electrorefining of plutonium. In accordance with the process, the plutonium-bearing salt is melted and mixed with metallic calcium. The calcium reduces ionized plutonium in the salt to plutonium metal, and also causes metallic plutonium in the salt, which is typically present as finely dispersed metallic shot, to coalesce. The reduced and coalesced plutonium separates out on the bottom of the reaction vessel as a separate metallic phase which is readily separable from the overlying salt upon cooling of the mixture. Yields of plutonium are typically on the order of 95%. The stripped salt is virtually free of plutonium and may be discarded to low-level waste storage.

METHOD OF SEPARATING Pu FROM METATHESIZED BiPO$sub 4$ CARRIER

DOEpatents

Knox, W.J.; Thompson, S.G.

1960-05-31

A process is given for separating uranium, neptunium, and/or plutonium from a bismuth hydroxide carrier by selective dissolution of these actinides with nitric acid of a concentration of from 0.05 to 0.5N.

Streamlined Approach for Environmental Restoration (SAFER) Plan for Corrective Action Unit 415: Project 57 No. 1 Plutonium Dispersion (NTTR), Nevada, Revision 0

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

Matthews, Patrick; Burmeister, Mark

2014-04-01

This Streamlined Approach for Environmental Restoration (SAFER) Plan addresses the actions needed to achieve closure for Corrective Action Unit (CAU) 415, Project 57 No. 1 Plutonium Dispersion (NTTR). CAU 415 is located on Range 4808A of the Nevada Test and Training Range (NTTR) and consists of one corrective action site: NAFR-23-02, Pu Contaminated Soil. The CAU 415 site consists of the atmospheric release of radiological contaminants to surface soil from the Project 57 safety experiment conducted in 1957. The safety experiment released plutonium (Pu), uranium (U), and americium (Am) to the surface soil over an area of approximately 1.9 squaremore » miles. This area is currently fenced and posted as a radiological contamination area. Vehicles and debris contaminated by the experiment were subsequently buried in a disposal trench within the surface-contaminated, fenced area and are assumed to have released radiological contamination to subsurface soils. Potential source materials in the form of pole-mounted electrical transformers were also identified at the site and will be removed as part of closure activities.« less

Uptake of Plutonium-238 into Solanum tuberosum L. (potato plants) in presence of complexing agent EDTA.

PubMed

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.

ACTUAL WASTE TESTING OF GYCOLATE IMPACTS ON THE SRS TANK FARM

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

Martino, C.

2014-05-28

Glycolic acid is being studied as a replacement for formic acid in the Defense Waste Processing Facility (DWPF) feed preparation process. After implementation, the recycle stream from DWPF back to the high-level waste Tank Farm will contain soluble sodium glycolate. Most of the potential impacts of glycolate in the Tank Farm were addressed via a literature review and simulant testing, but several outstanding issues remained. This report documents the actual-waste tests to determine the impacts of glycolate on storage and evaporation of Savannah River Site high-level waste. The objectives of this study are to address the following: Determine the extentmore » to which sludge constituents (Pu, U, Fe, etc.) dissolve (the solubility of sludge constituents) in the glycolate-containing 2H-evaporator feed. Determine the impact of glycolate on the sorption of fissile (Pu, U, etc.) components onto sodium aluminosilicate solids. The first objective was accomplished through actual-waste testing using Tank 43H and 38H supernatant and Tank 51H sludge at Tank Farm storage conditions. The second objective was accomplished by contacting actual 2H-evaporator scale with the products from the testing for the first objective. There is no anticipated impact of up to 10 g/L of glycolate in DWPF recycle to the Tank Farm on tank waste component solubilities as investigated in this test. Most components were not influenced by glycolate during solubility tests, including major components such as aluminum, sodium, and most salt anions. There was potentially a slight increase in soluble iron with added glycolate, but the soluble iron concentration remained so low (on the order of 10 mg/L) as to not impact the iron to fissile ratio in sludge. Uranium and plutonium appear to have been supersaturated in 2H-evaporator feed solution mixture used for this testing. As a result, there was a reduction of soluble uranium and plutonium as a function of time. The change in soluble uranium concentration was independent of added glycolate concentration. The change in soluble plutonium content was dependent on the added glycolate concentration, with higher levels of glycolate (5 g/L and 10 g/L) appearing to suppress the plutonium solubility. The inclusion of glycolate did not change the dissolution of or sorption onto actual-waste 2H-evaporator pot scale to an extent that will impact Tank Farm storage and concentration. The effects that were noted involved dissolution of components from evaporator scale and precipitation of components onto evaporator scale that were independent of the level of added glycolate.« less

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

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

Ganivet, M.

1960-06-29

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

Multivariate Analysis for Quantification of Plutonium(IV) in Nitric Acid Based on Absorption Spectra

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

Lines, Amanda M.; Adami, Susan R.; Sinkov, Sergey I.

Development of more effective, reliable, and fast methods for monitoring process streams is a growing opportunity for analytical applications. Many fields can benefit from on-line monitoring, including the nuclear fuel cycle where improved methods for monitoring radioactive materials will facilitate maintenance of proper safeguards and ensure safe and efficient processing of materials. On-line process monitoring with a focus on optical spectroscopy can provide a fast, non-destructive method for monitoring chemical species. However, identification and quantification of species can be hindered by the complexity of the solutions if bands overlap or show condition-dependent spectral features. Plutonium (IV) is one example ofmore » a species which displays significant spectral variation with changing nitric acid concentration. Single variate analysis (i.e. Beer’s Law) is difficult to apply to the quantification of Pu(IV) unless the nitric acid concentration is known and separate calibration curves have been made for all possible acid strengths. Multivariate, or chemometric, analysis is an approach that allows for the accurate quantification of Pu(IV) without a priori knowledge of nitric acid concentration.« less

Sensitivity and Uncertainty Analysis of Plutonium and Cesium Isotopes in Modeling of BR3 Reactor Spent Fuel

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

Evidence of plutonium bioavailability in pristine freshwaters of a karst system of the Swiss Jura Mountains

NASA Astrophysics Data System (ADS)

Cusnir, Ruslan; Christl, Marcus; Steinmann, Philipp; Bochud, François; Froidevaux, Pascal

2017-06-01

The interaction of trace environmental plutonium with dissolved natural organic matter (NOM) plays an important role on its mobility and bioavailability in freshwater environments. Here we explore the speciation and biogeochemical behavior of Pu in freshwaters of the karst system in the Swiss Jura Mountains. Chemical extraction and ultrafiltration methods were complemented by diffusive gradients in thin films technique (DGT) to measure the dissolved and bioavailable Pu fraction in water. Accelerator mass spectrometry (AMS) was used to accurately determine Pu in this pristine environment. Selective adsorption of Pu (III, IV) on silica gel showed that 88% of Pu in the mineral water is found in +V oxidation state, possibly in a highly soluble [PuO2+(CO3)n]m- form. Ultrafiltration experiments at 10 kDa yielded a similar fraction of colloid-bound Pu in the organic-rich and in mineral water (18-25%). We also found that the concentrations of Pu measured by DGT in mineral water are similar to the bulk concentration, suggesting that dissolved Pu is readily available for biouptake. Sequential elution (SE) of Pu from aquatic plants revealed important co-precipitation of potentially labile Pu (60-75%) with calcite fraction within outer compartment of the plants. Hence, we suggest that plutonium is fully available for biological uptake in both mineral and organic-rich karstic freshwaters.

Sensitivity and Uncertainty Analysis of Plutonium and Cesium Isotopes in Modeling of BR3 Reactor Spent Fuel

DOE PAGES

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

12. Architectural Floor Plans, 233S, U.S. Atomic Energy Commission, Hanford ...

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

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, ...

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

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

Bi-Modal Model for Neutron Emissions from PuO{sub 2} and MOX Holdup

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

Menlove, Howard; Lafleur, Adrienne

2015-07-01

The measurement of uranium and plutonium holdup in plants during process activity and for decommissioning is important for nuclear safeguards and material control. The amount of plutonium and uranium holdup in glove-boxes, pipes, ducts, and other containers has been measured for several decades using both neutron and gamma-ray techniques. For the larger containers such as hot cells and glove-boxes that contain processing equipment, the gamma-ray techniques are limited by self-shielding in the sample as well as gamma absorption in the equipment and associated shielding. The neutron emission is more penetrating and has been used extensively to measure the holdup formore » the large facilities such as the MOX processing and fabrication facilities in Japan and Europe. In some case the totals neutron emission rates are used to determine the holdup mass and in other cases the coincidence rates are used such as at the PFPF MOX fabrication plant in Japan. The neutron emission from plutonium and MOX has 3 primary source terms: 1) Spontaneous fission (SF) from the plutonium isotopes, 2) The (α,n) reactions from the plutonium alpha particle emission reacting with the oxygen and other impurities, and 3) Neutron multiplication (M) in the plutonium and uranium as a result of neutrons created by the first two sources. The spontaneous fission yield per gram is independent of thickness, whereas, the above sources 2) and 3) are very dependent on the thickness of the deposit. As the effective thickness of the deposit becomes thin relative to the alpha particle range, the (α,n) reactions and neutrons from multiplication (M) approach zero. In any glove-box, there will always be two primary modes of holdup accumulation, namely direct powder contact and non-contact by air dispersal. These regimes correspond to surfaces in the glove-box that have come into direct contact with the process MOX powder versus surface areas that have not had direct contact with the powder. The air dispersal of PuO{sub 2} particles has been studied for several decades by health physicists, because the primary health hazard of plutonium is breathing the airborne particles. The air dispersal mechanism results from the smaller particles in the top layer of powder that are lifted into the air by the electrostatic charge buildup from the alpha decay process, and the air convection carries the particles to new more distant locations. If there is open plutonium powder in a glove-box, the surfaces at more distant locations will become contaminated over time. The range of an alpha particle in a solid or powder is a function of the particle energy, the material density, and the atomic number A of the material. The average energy of a plutonium alpha particle is ∼5.2 MeV and the range in air is ∼37 mm. The range in other materials can be estimated via the Bragg-Kleenman equation. For plutonium, A is 94, and the typical density for a single particle is ∼11.5 g/cm{sup 3}, but for a powder, the density would be less because of the air packing fraction. The significance of the small diameter is that the range of the alpha particle is ∼50 μm for powder density 2.5 and significantly less for a single particle with density 11.5, so the thin deposit of separate small particles will have a greatly reduced (α,n) yield. The average alpha transit length to the surface in the isolated MOX particle would be < 2.5 μm; whereas, the range of the alpha particle is much longer. Thus, most of the alpha particles would escape from the MOX particle and be absorbed by the walls and air. The air dispersal particles will have access to a large surface area that includes the walls, whereas, the powder contact surface area will be orders of magnitude smaller. Thus, the vast majority of the glove-box surface area does not produce the full (α,n) reaction neutron yield, even from the O{sub 2} in the PuO{sub 2} as well as any impurity contamination such as H{sub 2}O. To obtain a more quantitative estimate of the neutron (α,n) yields as a function of holdup deposit thickness, we have used MCNPX calculations to estimate the absorption of alpha particles in PuO{sub 2} holdup deposits. The powder thickness was varied from 0.1 μm to 5000 μm and the alpha particle escape probability was calculated. As would be expected, as the thickness approaches zero, the escape probability approaches 1.0, and as the thickness gets much greater than the alpha particle range (∼50 μm), the escape probability becomes small. Typically, the neutron holdup calibration measurement are performed using sealed containers of thick MOX that has all 3 sources of neutrons [SF, (α,n), and M], and no significant impurities. Thus, the calibration counting rates need to include corrections for M and (α,n) yields that are different for the holdup compared with the calibration samples. If totals neutron counting is used for the holdup measurements, the variability of the (α,n) term needs to be considered.« less

Evaluating Alternatives for Drinking Water at Deployed Locations

DTIC Science & Technology

2006-03-01

Tucker and Sands, 1999; Beering , 2002). 1986 Plutonium was found in the New York city drinking water system. Though the concentrations were...based approach called Hazard Analysis and Critical Control Point ( HACCP ). This approach holds that avoidance is practical and effective where other

10. Architectural Door Details & Plot Plan, 233S, U.S. Atomic ...

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

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

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

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

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

Comparison of radionuclide levels in soil, sagebrush, plant litter, cryptogams, and small mammals

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

Landeen, D.S.

1994-09-01

Soil, sagebrush, plant litter, cryptogam, and small mammal samples were collected and analyzed for cesium-137, strontium-90, plutonium-238, plutonium 239/240, technetium-99, and iodine-129 from 1981 to 1986 at the US Department of Energy Hanford Site in southeastern Washington State as part of site characterization and environmental monitoring activities. Samples were collected on the 200 Areas Plateau, downwind from ongoing waste management activities. Plant litter, cryptogams, and small mammals are media that are not routinely utilized in monitoring or characterization efforts for determination of radionuclide concentrations. Studies at Hanford, other US Department of Energy sites, and in eastern Europe have indicated thatmore » plant litter and cryptogams may serve as effective ``natural`` monitors of air quality. Plant litter in this study consists of fallen leaves from sagebrush and ``cryptogams`` describes that portion of the soil crust composed of mosses, lichens, algae, and fungi. Comparisons of cesium-137 and strontium-90 concentrations in the soil, sagebrush, litter, and cryptogams revealed significantly higher (p<0.05) levels in plant litter and cryptogams. Technetium-99 values were the highest in sagebrush and litter. Plutonium-238 and 239/40 and iodine-129 concentrations never exceeded 0.8 pCi/gm in all media. No evidence of any significant amounts of any radionuclides being incorporated into the small mammal community was discovered. The data indicate that plant litter and cryptogams may be better, indicators of environmental quality than soil or vegetation samples. Augmenting a monitoring program with samples of litter and cryptogams may provide a more accurate representation of radionuclide environmental uptake and/or contamination levels in surrounding ecosystems. The results of this study may be applied directly to other radioecological monitoring conducted at other nuclear sites and to the monitoring of other pollutants.« less

Submicron hard X-ray fluorescence imaging of synthetic elements.

PubMed

Jensen, Mark P; Aryal, Baikuntha P; Gorman-Lewis, Drew; Paunesku, Tatjana; Lai, Barry; Vogt, Stefan; Woloschak, Gayle E

2012-04-13

Synchrotron-based X-ray fluorescence microscopy (XFM) using hard X-rays focused into sub-micron spots is a powerful technique for elemental quantification and mapping, as well as microspectroscopic measurements such as μ-XANES (X-ray absorption near edge structure). We have used XFM to image and simultaneously quantify the transuranic element plutonium at the L(3) or L(2)-edge as well as Th and lighter biologically essential elements in individual rat pheochromocytoma (PC12) cells after exposure to the long-lived plutonium isotope (242)Pu. Elemental maps demonstrate that plutonium localizes principally in the cytoplasm of the cells and avoids the cell nucleus, which is marked by the highest concentrations of phosphorus and zinc, under the conditions of our experiments. The minimum detection limit under typical acquisition conditions with an incident X-ray energy of 18 keV for an average 202 μm(2) cell is 1.4 fg Pu or 2.9×10(-20) moles Pu μm(-2), which is similar to the detection limit of K-edge XFM of transition metals at 10 keV. Copper electron microscopy grids were used to avoid interference from gold X-ray emissions, but traces of strontium present in naturally occurring calcium can still interfere with plutonium detection using its L(α) X-ray emission. Copyright © 2012 Elsevier B.V. All rights reserved.

Vertical and horizontal fluxes of plutonium and americium in the western Mediterranean and the Strait of Gibraltar.

PubMed

León Vintró, L; Mitchell, P I; Condren, O M; Downes, A B; Papucci, C; Delfanti, R

1999-09-30

New data on the vertical distributions of plutonium and americium in the waters of the western Mediterranean and the Strait of Gibraltar are examined in terms of the processes governing their delivery to, transport in and removal from the water column within the basin. Residence times for plutonium and americium in surface waters of approximately 15 and approximately 3 years, respectively, are deduced, and it is shown that by the mid 1990s only approximately 35% of the 239,240Pu and approximately 5% of the 241Am deposited as weapons fallout still resided in the water column. Present 239,240Pu inventories in the water column and the underlying sediments are estimated to be approximately 25 TBq and approximately 40 TBq, respectively, which reconcile well with the time-integrated fallout deposition in this zone, taken to be approximately 69 TBq. The data show that there are significant net outward fluxes of plutonium and americium from the basin through the Strait of Gibraltar at the present time. These appear to be compensated by net inward fluxes of similar magnitude through the Strait of Sicily. Thus, the time-integrated fallout deposition in the western basin can be accounted for satisfactorily in terms of present water column and sediment inventories. Enhanced scavenging on the continental shelves, as evidenced by the appreciably higher transuranic concentrations in shelf sediments, supports this contention.

Estimating Radiological Doses to Predators Foraging in a Low-Level Radioactive Waste Management Area

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

L.Soholt; G.Gonzales; P.Fresquez

2003-03-01

Since 1957, Los Alamos National Laboratory has operated Area G as its low-level, solid radioactive waste management and disposal area. Although the waste management area is developed, plants, small mammals, and avian and mammalian predators still occupy the less disturbed and revegetated portions of the land. For almost a decade, we have monitored the concentrations of selected radionuclides in soils, plants, and small mammals at Area G. The radionuclides tritium, plutonium-238, and plutonium-239 are regularly found at levels above regional background in all three media. Based on radionuclide concentrations in mice collected from 1994 to 1999, we calculated doses tomore » higher trophic levels (owl, hawk, kestrel, and coyote) that forage on the waste management area. These predators play important functions in the regional ecosystems and are an important part of local Native American traditional tales that identify the uniqueness of their culture. The estimated doses are compared to Department of Energy's interim limit of 0.1 rad/day for the protection of terrestrial wildlife. We used exposure parameters that were derived from the literature for each receptor, including Environmental Protection Agency's exposure factors handbook. Estimated doses to predators ranged from 9E-06 to 2E-04 rad/day, assuming that they forage entirely on the waste management area. These doses are greater than those calculated for predators foraging exclusively in reference areas, but are still well below the interim dose limit. We believe that these calculated doses represent upper-bound estimates of exposure for local predators because the larger predators forage over areas that are much greater than the 63-acre waste management area. Based on these results, we concluded that predators foraging on this area do not face a hazard from radiological exposure under current site conditions.« less

Distribution coefficients (Kd's) for use in risk assessment models of the Kara Sea.

PubMed

Carroll, J; Boisson, F; Teyssie, J L; King, S E; Krosshavn, M; Carroll, M L; Fowler, S W; Povinec, P P; Baxter, M S

1999-07-01

As a prerequisite for most evaluations of radionuclide transport pathways in marine systems, it is necessary to obtain basic information on the sorption potential of contaminants onto particulate matter. Kd values for use in modeling radionuclide dispersion in the Kara Sea have been determined as part of several international programs addressing the problem of radioactive debris residing in Arctic Seas. Field and laboratory Kd experiments were conducted for the following radionuclides associated with nuclear waste: americium, europium, plutonium, cobalt, cesium and strontium. Emphasis has been placed on two regions in the Kara Sea: (i) the Novaya Zemlya Trough (NZT) and (ii) the mixing zones of the Ob and Yenisey Rivers (RMZ). Short-term batch Kd experiments were performed at-sea on ambient water column samples and on samples prepared both at-sea and in the laboratory by mixing filtered bottom water with small amounts of surficial bottom sediments (particle concentrations in samples = 1-30 mg/l). Within both regions, Kd values for individual radionuclides vary over two to three orders of magnitude. The relative particle affinities for radionuclides in the two regions are americium approximately equal to europium > plutonium > cobalt > cesium > strontium. The values determined in this study agree with minimum values given in the IAEA Technical Report [IAEA, 1985. Sediment Kd's and Concentration Factors for Radionuclides in the Marine Environment. Technical Report No. 247. International Atomic Energy Agency, Vienna.]. Given the importance of Kd's in assessments of critical transport pathways for radionuclide contaminants, we recommend that Kd ranges of values for specific elements rather than single mean values be incorporated into model simulations of radionuclide dispersion.

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

PubMed

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

2013-03-01

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

Monitor of the concentration of particles of dense radioactive materials in a stream of air

DOEpatents

Yule, Thomas J.

1979-01-01

A monitor of the concentration of particles of radioactive materials such as plutonium oxide in diameters as small as 1/2 micron includes in combination a first stage comprising a plurality of virtual impactors, a second stage comprising a further plurality of virtual impactors, a collector for concentrating particulate material, a radiation detector disposed near the collector to respond to radiation from collected material and means for moving a stream of air, possibly containing particulate contaminants, through the apparatus.

/sup 239/Pu contamination in snakes inhabiting the Rocky Flats Plant site

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

Geiger, R.A.; Winsor, T.F.

1975-01-01

For approximately four years studies have been under way at the Rocky Flats plant to determine contamination patterns and concentrations of Pu in the biota. Contamination of the Rocky Flats environs has resulted from at least three incidents, a September 1957 fire, a May 1969 fire, and leaking barrels containing plutonium-laden cutting oil. The latter incident was considered by far the major source of the plutonium contamination. Results are reported from a study conducted to determine whether snake tissues of the area contained detectable amounts of /sup 239/Pu and, if so, at what concentrations. Eastern yellow-bellied racers (Coluber constrictor flaviventris,more » bullsnakes (Pituophis melanoleucus sayi, and prairie rattlesnakes (Crotalus viridis viridis, were collected for /sup 239/Pu bioassay of lung, liver, and bone tissues. Snakes were captured using drift fences terminating in funnel traps and by opportunistic sampling. Results led to the conclusion that snakes are not an important organism in the redistribution of /sup 239/Pu. (CH)« less

An update of hydrologic conditions and distribution of selected constituents in water, Snake River Plain aquifer and perched groundwater zones, Idaho National Laboratory, Idaho, emphasis 2006-08

USGS Publications Warehouse

Davis, Linda C.

2010-01-01

Since 1952, radiochemical and chemical wastewater discharged to infiltration ponds (also called percolation ponds), evaporation ponds, and disposal wells at the Idaho National Laboratory (INL) has affected water quality in the eastern Snake River Plain aquifer and perched groundwater zones underlying the INL. The U.S. Geological Survey, in cooperation with the U.S. Department of Energy, maintains groundwater monitoring networks at the INL to determine hydrologic trends, and to delineate the movement of radiochemical and chemical wastes in the aquifer and in perched groundwater zones. This report presents an analysis of water-level and water-quality data collected from aquifer and perched groundwater wells in the USGS groundwater monitoring networks during 2006-08. Water in the Snake River Plain aquifer primarily moves through fractures and interflow zones in basalt, generally flows southwestward, and eventually discharges at springs along the Snake River. The aquifer primarily is recharged from infiltration of irrigation water, infiltration of streamflow, groundwater inflow from adjoining mountain drainage basins, and infiltration of precipitation. From March-May 2005 to March-May 2008, water levels in wells generally remained constant or rose slightly in the southwestern corner of the INL. Water levels declined in the central and northern parts of the INL. The declines ranged from about 1 to 3 feet in the central part of the INL, to as much as 9 feet in the northern part of the INL. Water levels in perched groundwater wells around the Advanced Test Reactor Complex (ATRC) also declined. Detectable concentrations of radiochemical constituents in water samples from wells in the Snake River Plain aquifer at the INL generally decreased or remained constant during 2006-08. Decreases in concentrations were attributed to decreased rates of radioactive-waste disposal, radioactive decay, changes in waste-disposal methods, and dilution from recharge and underflow. In April or October 2008, reportable concentrations of tritium in groundwater ranged from 810 ? 70 to 8,570 ? 190 picocuries per liter (pCi/L), and the tritium plume extended south-southwestward in the general direction of groundwater flow. Tritium concentrations in water from wells completed in shallow perched groundwater at the ATRC were less than the reporting levels. Tritium concentrations in deep perched groundwater exceeded the reporting level in 11 wells during at least one sampling event during 2006-08 at the ATRC. Tritium concentrations from one or more zones in each well were reportable in water samples collected at various depths in six wells equipped with multi-level WestbayTM packer sampling systems. Concentrations of strontium-90 in water from 24 of 52 aquifer wells sampled during April or October 2008 exceeded the reporting level. Concentrations ranged from 2.2 ? 0.7 to 32.7 ? 1.2 pCi/L. Strontium-90 has not been detected within the eastern Snake River Plain aquifer beneath the ATRC partly because of the exclusive use of waste-disposal ponds and lined evaporation ponds rather than using the disposal well for radioactive-wastewater disposal at ATRC. At the ATRC, the strontium-90 concentration in water from one well completed in shallow perched groundwater was less than the reporting level. During at least one sampling event during 2006-08, concentrations of strontium-90 in water from nine wells completed in deep perched groundwater at the ATRC were greater than reporting levels. Concentrations ranged from 2.1?0.7 to 70.5?1.8 pCi/L. At the Idaho Nuclear Technology and Engineering Center (INTEC), the reporting level was exceeded in water from two wells completed in deep perched groundwater. During 2006-08, concentrations of cesium-137, plutonium-238, and plutonium-239, -240 (undivided), and americium-241 were less than the reporting level in water samples from all wells and all zones in wells equipped with multi-level WestbayTM packer sampling systems

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

DOEpatents

Soderholm, Lynda; Wilson, Richard E; Chiarizia, Renato; Skanthakumar, Suntharalingam

2014-06-03

The invention provides a method for extracting plutonium from spent nuclear fuel, the method comprising supplying plutonium in a first aqueous phase; contacting the plutonium aqueous phase with a mixture of a dielectric and a moiety having a first acidity so as to allow the plutonium to substantially extract into the mixture; and contacting the extracted plutonium with second a aqueous phase, wherein the second aqueous phase has a second acidity higher than the first acidity, so as to allow the extracted plutonium to extract into the second aqueous phase. The invented method facilitates isolation of plutonium polymer without the formation of crud or unwanted emulsions.

Effect of Americium-241 Content on Plutonium Radiation Source Terms

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

Rainisch, R.

1998-12-28

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

Integrating the stabilization of nuclear materials

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

Dalton, H.F.

1996-05-01

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

Method for dissolving plutonium dioxide

DOEpatents

Tallent, Othar K.

1978-01-01

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

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

DOEpatents

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

1962-11-13

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

Plutonium concentration and (240)Pu/(239)Pu atom ratio in biota collected from Amchitka Island, Alaska: recent measurements using ICP-SFMS.

PubMed

Bu, Kaixuan; Cizdziel, James V; Dasher, Douglas

2013-10-01

Three underground nuclear tests, including the Unites States' largest, were conducted on Amchitka Island, Alaska. Monitoring of the radiological environment around the island is challenging because of its remote location. In 2008, the Department of Energy (DOE) Office of Legacy Management (LM) became responsible for the long term maintenance and surveillance of the Amchitka site. The first DOE LM environmental survey occurred in 2011 and is part of a cycle of activities that will occur every 5 years. The University of Alaska Fairbanks, a participant in the 2011 study, provided the lichen (Cladonia spp.), freshwater moss (Fontinalis neomexicanus), kelp (Eualaria fistulosa) and horse mussel (Modiolus modiolus) samples from Amchitka Island and Adak Island (a control site). These samples were analyzed for (239)Pu and (240)Pu concentration and (240)Pu/(239)Pu atom ratio using inductively coupled plasma sector field mass spectrometry (ICP-SFMS). Plutonium concentrations and (240)Pu/(239)Pu atom ratios were generally consistent with previous terrestrial and marine studies in the region. The ((239)+)(240)Pu levels (mBq kg(-1), dry weight) ranged from 3.79 to 57.1 for lichen, 167-700 for kelp, 27.9-148 for horse mussel, and 560-573 for moss. Lichen from Adak Island had higher Pu concentrations than Amchitka Island, the difference was likely the result of the higher precipitation at Adak compared to Amchitka. The (240)Pu/(239)Pu atom ratios were significantly higher in marine samples compared to terrestrial and freshwater samples (t-test, p < 0.001); lichen and moss averaged 0.184 ± 0.007, similar to the integrated global fallout ratio, whereas kelp and mussel (soft tissue) averaged 0.226 ± 0.003. These observations provide supporting evidence that a large input of isotopically heavier Pu occurred into the North Pacific Ocean, likely from the Marshall Island high yield nuclear tests, but other potential sources, such as the Kamchatka Peninsula Rybachiy Naval Base and Amchitka Island underground nuclear test site cannot be ruled out. Copyright © 2013 Elsevier Ltd. All rights reserved.

Characterization of Representative Materials in Support of Safe, Long Term Storage of Surplus Plutonium in DOE-STD-3013 Containers

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

METHOD OF SEPARATING PLUTONIUM

DOEpatents

Brown, H.S.; Hill, O.F.

1958-02-01

Plutonium hexafluoride is a satisfactory fluorinating agent and may be reacted with various materials capable of forming fluorides, such as copper, iron, zinc, etc., with consequent formation of the metal fluoride and reduction of the plutonium to the form of a lower fluoride. In accordance with the present invention, it has been found that the reactivity of plutonium hexafluoride with other fluoridizable materials is so great that the process may be used as a method of separating plutonium from mixures containing plutonium hexafluoride and other vaporized fluorides even though the plutonium is present in but minute quantities. This process may be carried out by treating a mixture of fluoride vapors comprising plutonium hexafluoride and fluoride of uranium to selectively reduce the plutonium hexafluoride and convert it to a less volatile fluoride, and then recovering said less volatile fluoride from the vapor by condensation.

Determination of total plutonium content in spent nuclear fuel assemblies with the differential die-away self-interrogation instrument

NASA Astrophysics Data System (ADS)

Kaplan, Alexis C.; Henzl, Vladimir; Menlove, Howard O.; Swinhoe, Martyn T.; Belian, Anthony P.; Flaska, Marek; Pozzi, Sara A.

2014-11-01

As a part of the Next Generation Safeguards Initiative Spent Fuel project, we simulate the response of the Differential Die-away Self-Interrogation (DDSI) instrument to determine total elemental plutonium content in an assayed spent nuclear fuel assembly (SFA). We apply recently developed concepts that relate total plutonium mass with SFA multiplication and passive neutron count rate. In this work, the multiplication of the SFA is determined from the die-away time in the early time domain of the Rossi-Alpha distributions measured directly by the DDSI instrument. We utilize MCNP to test the method against 44 pressurized water reactor SFAs from a simulated spent fuel library with a wide dynamic range of characteristic parameters such as initial enrichment, burnup, and cooling time. Under ideal conditions, discounting possible errors of a real world measurement, a root mean square agreement between true and determined total Pu mass of 2.1% is achieved.

ADSORPTION-BISMUTH PHOSPHATE METHOD FOR SEPARATING PLUTONIUM

DOEpatents

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

1960-06-28

A process is given for separating plutonium from uranium and fission products. Plutonium and uranium are adsorbed by a cation exchange resin, plutonium is eluted from the adsorbent, and then, after oxidation to the hexavalent state, the plutonium is contacted with a bismuth phosphate carrier precipitate.

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

DOEpatents

Fried, S.; Baumbach, H.L.

1959-12-01

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

A Calibration to Predict the Concentrations of Impurities in Plutonium Oxide by Prompt Gamma Analysis Revision 2

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

Narlesky, Joshua Edward; Kelly, Elizabeth J.

2015-09-10

This report documents the new PG calibration regression equation. These calibration equations incorporate new data that have become available since revision 1 of “A Calibration to Predict the Concentrations of Impurities in Plutonium Oxide by Prompt Gamma Analysis” was issued [3] The calibration equations are based on a weighted least squares (WLS) approach for the regression. The WLS method gives each data point its proper amount of influence over the parameter estimates. This gives two big advantages, more precise parameter estimates and better and more defensible estimates of uncertainties. The WLS approach makes sense both statistically and experimentally because themore » variances increase with concentration, and there are physical reasons that the higher measurements are less reliable and should be less influential. The new magnesium calibration includes a correction for sodium and separate calibration equation for items with and without chlorine. These additional calibration equations allow for better predictions and smaller uncertainties for sodium in materials with and without chlorine. Chlorine and sodium have separate equations for RICH materials. Again, these equations give better predictions and smaller uncertainties chlorine and sodium for RICH materials.« less

Chemical Disposition of Plutonium in Hanford Site Tank Wastes

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

Delegard, Calvin H.; Jones, Susan A.

2015-05-07

This report examines the chemical disposition of plutonium (Pu) in Hanford Site tank wastes, by itself and in its observed and potential interactions with the neutron absorbers aluminum (Al), cadmium (Cd), chromium (Cr), iron (Fe), manganese (Mn), nickel (Ni), and sodium (Na). Consideration also is given to the interactions of plutonium with uranium (U). No consideration of the disposition of uranium itself as an element with fissile isotopes is considered except tangentially with respect to its interaction as an absorber for plutonium. The report begins with a brief review of Hanford Site plutonium processes, examining the various means used tomore » recover plutonium from irradiated fuel and from scrap, and also examines the intermediate processing of plutonium to prepare useful chemical forms. The paper provides an overview of Hanford tank defined-waste–type compositions and some calculations of the ratios of plutonium to absorber elements in these waste types and in individual waste analyses. These assessments are based on Hanford tank waste inventory data derived from separately published, expert assessments of tank disposal records, process flowsheets, and chemical/radiochemical analyses. This work also investigates the distribution and expected speciation of plutonium in tank waste solution and solid phases. For the solid phases, both pure plutonium compounds and plutonium interactions with absorber elements are considered. These assessments of plutonium chemistry are based largely on analyses of idealized or simulated tank waste or strongly alkaline systems. The very limited information available on plutonium behavior, disposition, and speciation in genuine tank waste also is discussed. The assessments show that plutonium coprecipitates strongly with chromium, iron, manganese and uranium absorbers. Plutonium’s chemical interactions with aluminum, nickel, and sodium are minimal to non-existent. Credit for neutronic interaction of plutonium with these absorbers occurs only if they are physically proximal in solution or the plutonium present in the solid phase is intimately mixed with compounds or solutions of these absorbers. No information on the potential chemical interaction of plutonium with cadmium was found in the technical literature. Definitive evidence of sorption or adsorption of plutonium onto various solid phases from strongly alkaline media is less clear-cut, perhaps owing to fewer studies and to some well-attributed tests run under conditions exceeding the very low solubility of plutonium. The several studies that are well-founded show that only about half of the plutonium is adsorbed from waste solutions onto sludge solid phases. The organic complexants found in many Hanford tank waste solutions seem to decrease plutonium uptake onto solids. A number of studies show plutonium sorbs effectively onto sodium titanate. Finally, this report presents findings describing the behavior of plutonium vis-à-vis other elements during sludge dissolution in nitric acid based on Hanford tank waste experience gained by lab-scale tests, chemical and radiochemical sample characterization, and full-scale processing in preparation for strontium-90 recovery from PUREX sludges.« less

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

PubMed

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

2004-02-01

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

Preparation of alpha-emitting nuclides by electrodeposition

NASA Astrophysics Data System (ADS)

Lee, M. H.; Lee, C. W.

2000-06-01

A method is described for electrodepositing the alpha-emitting nuclides. To determine the optimum conditions for plating plutonium, the effects of electrolyte concentration, chelating reagent, current, pH of electrolyte and the time of plating on the electrodeposition were investigated on the base of the ammonium oxalate-ammonium sulfate electrolyte containing diethyl triamino pentaacetic acid. An optimized electrodeposition procedure for the determination of plutonium was validated by application to environmental samples. The chemical yield of the optimized method of electrodeposition step in the environmental sample was a little higher than that of Talvitie's method. The developed electrodeposition procedure in this study was applied to determine the radionuclides such as thorium, uranium and americium that the electrodeposition yields were a little higher than those of the conventional method.

The potential for chromium to affect the fertilization process of Chinook salmon (Oncorhynchus tshawytscha) in the Hanford reach of the Columbia River, Washington, USA.

PubMed

Farag, A M; Harper, D D; Cleveland, L; Brumbaugh, W G; Little, E E

2006-05-01

The Hanford Nuclear Reservation in south central Washington was claimed by the federal government as a site for the production of plutonium. During the course of production and operation of the facilities at Hanford, radionuclides and chromium were discharged directly into the river and also contaminated the groundwater. This study was designed to assess the effects of chromium (Cr) on Chinook salmon (Oncorhynchus tshawytscha) fertilization under exposure conditions similar to those of the Hanford Reach of the Columbia River. Chinook salmon gametes were exposed to aqueous Cr concentrations ranging from 0 to 266 microg Cr l(-1). The current ambient water-quality criteria (AWQC) established for the protection of aquatic life (United States Environmental Protection Agency [USEPA] 1986) is 11 microg Cr l(-1). Cr has been measured in pore water from bottom sediments of the Columbia River at concentrations >600 microg Cr l(-1). Under exposure conditions designed to closely mimic events that occur in the river, the fertilization of Chinook salmon eggs was not affected by concentrations of Cr ranging from 11 to 266 microg Cr l(-1). Data suggest that the instantaneous nature of fertilization likely limits the potential effects of Cr on fertilization success. As a result, the current AWQC of 11 mug Cr l(-1) is most likely protective of Chinook salmon fertilization.

The potential for chromium to affect the fertilization process of Chinook salmon (Oncorhynchus tshawytscha) in the Hanford Reach of the Columbia River, Washington, USA

USGS Publications Warehouse

Farag, A.M.; Harper, D.D.; Cleveland, L.; Brumbaugh, W.G.; Little, E.E.

2006-01-01

The Hanford Nuclear Reservation in south central Washington was claimed by the federal government as a site for the production of plutonium. During the course of production and operation of the facilities at Hanford, radionuclides and chromium were discharged directly into the river and also contaminated the groundwater. This study was designed to assess the effects of chromium (Cr) on Chinook salmon (Oncorhynchus tshawytscha) fertilization under exposure conditions similar to those of the Hanford Reach of the Columbia River. Chinook salmon gametes were exposed to aqueous Cr concentrations ranging from 0 to 266 μg Cr l−1. The current ambient water-quality criteria (AWQC) established for the protection of aquatic life (United States Environmental Protection Agency [USEPA] 1986) is 11 μg Cr l−1. Cr has been measured in pore water from bottom sediments of the Columbia River at concentrations >600 μg Cr l−1. Under exposure conditions designed to closely mimic events that occur in the river, the fertilization of Chinook salmon eggs was not affected by concentrations of Cr ranging from 11 to 266 μg Cr l−1. Data suggest that the instantaneous nature of fertilization likely limits the potential effects of Cr on fertilization success. As a result, the current AWQC of 11 μg Cr l−1 is most likely protective of Chinook salmon fertilization.

PRODUCTION OF PLUTONIUM METAL

DOEpatents

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

1961-01-17

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

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

Radioactive waste management and plutonium recovery within the context of the development of nuclear energy in Russia

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

PROCESS OF FORMING PLUOTONIUM SALTS FROM PLUTONIUM EXALATES

DOEpatents

Garner, C.S.

1959-02-24

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

EXAFS/XANES studies of plutonium-loaded sodalite/glass waste forms

NASA Astrophysics Data System (ADS)

Richmann, Michael K.; Reed, Donald T.; Kropf, A. Jeremy; Aase, Scott B.; Lewis, Michele A.

2001-09-01

A sodalite/glass ceramic waste form is being developed to immobilize highly radioactive nuclear wastes in chloride form, as part of an electrochemical cleanup process. Two types of simulated waste forms were studied: where the plutonium was alone in an LiCl/KCl matrix and where simulated fission-product elements were added representative of the electrometallurgical treatment process used to recover uranium from spent nuclear fuel also containing plutonium and a variety of fission products. Extended X-ray absorption fine structure spectroscopy (EXAFS) and X-ray absorption near-edge spectroscopy (XANES) studies were performed to determine the location, oxidation state, and particle size of the plutonium within these waste form samples. Plutonium was found to segregate as plutonium(IV) oxide with a crystallite size of at least 4.8 nm in the non-fission-element case and 1.3 nm with fission elements present. No plutonium was observed within the sodalite in the waste form made from the plutonium-loaded LiCl/KCl eutectic salt. Up to 35% of the plutonium in the waste form made from the plutonium-loaded simulated fission-product salt may be segregated with a heavy-element nearest neighbor other than plutonium or occluded internally within the sodalite lattice.

EXPERIMENTAL METHODS TO ESTIMATE ACCUMULATED SOLIDS IN NUCLEAR WASTE TANKS

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

Duignan, M.; Steeper, T.; Steimke, J.

2012-12-10

The Department of Energy has a large number of nuclear waste tanks. It is important to know if fissionable materials can concentrate when waste is transferred from staging tanks prior to feeding waste treatment plants. Specifically, there is a concern that large, dense particles, e.g., plutonium containing, could accumulate in poorly mixed regions of a blend tank heel for tanks that employ mixing jet pumps. At the request of the DOE Hanford Tank Operations Contractor, Washington River Protection Solutions, the Engineering Development Laboratory of the Savannah River National Laboratory performed a scouting study in a 1/22-scale model of a wastemore » tank to investigate this concern and to develop measurement techniques that could be applied in a more extensive study at a larger scale. Simulated waste tank solids and supernatant were charged to the test tank and rotating liquid jets were used to remove most of the solids. Then the volume and shape of the residual solids and the spatial concentration profiles for the surrogate for plutonium were measured. This paper discusses the overall test results, which indicated heavy solids only accumulate during the first few transfer cycles, along with the techniques and equipment designed and employed in the test. Those techniques include: Magnetic particle separator to remove stainless steel solids, the plutonium surrogate from a flowing stream; Magnetic wand used to manually remove stainless steel solids from samples and the tank heel; Photographs were used to determine the volume and shape of the solids mounds by developing a composite of topographical areas; Laser rangefinders to determine the volume and shape of the solids mounds; Core sampler to determine the stainless steel solids distribution within the solids mounds; Computer driven positioner that placed the laser rangefinders and the core sampler over solids mounds that accumulated on the bottom of a scaled staging tank in locations where jet velocities were low. These devices and techniques were very effective to estimate the movement, location, and concentrations of the solids representing plutonium and are expected to perform well at a larger scale. The operation of the techniques and their measurement accuracies will be discussed as well as the overall results of the accumulated solids test.« less

Device and method for accurately measuring concentrations of airborne transuranic isotopes

DOEpatents

McIsaac, Charles V.; Killian, E. Wayne; Grafwallner, Ervin G.; Kynaston, Ronnie L.; Johnson, Larry O.; Randolph, Peter D.

1996-01-01

An alpha continuous air monitor (CAM) with two silicon alpha detectors and three sample collection filters is described. This alpha CAM design provides continuous sampling and also measures the cumulative transuranic (TRU), i.e., plutonium and americium, activity on the filter, and thus provides a more accurate measurement of airborne TRU concentrations than can be accomplished using a single fixed sample collection filter and a single silicon alpha detector.

Device and method for accurately measuring concentrations of airborne transuranic isotopes

DOEpatents

McIsaac, C.V.; Killian, E.W.; Grafwallner, E.G.; Kynaston, R.L.; Johnson, L.O.; Randolph, P.D.

1996-09-03

An alpha continuous air monitor (CAM) with two silicon alpha detectors and three sample collection filters is described. This alpha CAM design provides continuous sampling and also measures the cumulative transuranic (TRU), i.e., plutonium and americium, activity on the filter, and thus provides a more accurate measurement of airborne TRU concentrations than can be accomplished using a single fixed sample collection filter and a single silicon alpha detector. 7 figs.

STRIPPING PROCESS FOR PLUTONIUM

DOEpatents

Kolodney, M.

1959-10-01

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

PLUTONIUM-CUPFERRON COMPLEX AND METHOD OF REMOVING PLUTONIUM FROM SOLUTION

DOEpatents

Potratz, H.A.

1959-01-13

A method is presented for separating plutonium from fission products present in solutions of neutronirradiated uranium. The process consists in treating such acidic solutions with cupferron so that the cupferron reacts with the plutonium present to form an insoluble complex. This plutonium cupferride precipitates and may then be separated from the solution.

NNSS Soils Monitoring: Plutonium Valley (CAU 366) FY2013 and FY2014

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

Miller, Julianne J.; Nikolich, George; Mizell, Steve

The Desert Research Institute (DRI) is conducting a field assessment of the potential for contaminated soil transport from the Plutonium Valley Contamination Area (CA) as a result of wind transport and storm runoff in support of Nevada Nuclear Security Administration (NNSA) efforts to complete regulatory closure of the contamination areas. The DRI work is intended to confirm the likely mechanism(s) of transport and determine the meteorological conditions that might cause movement of contaminated soils. Emphasis is given to collecting sediment transported by channelized storm runoff at the Plutonium Valley investigation sites. These data will inform closure plans that are beingmore » developed, which will facilitate appropriate closure design and postclosure monitoring. Desert Research Institute installed two meteorological monitoring stations south (station number 1) and north (station number 2) of the Plutonium Valley CA and a runoff sediment sampling station within the CA in 2011. Temperature, wind speed, wind direction, relative humidity, precipitation, solar radiation, barometric pressure, soil temperature, and airborne particulate concentration are collected at both meteorological stations. The maximum, minimum, and average or total (as appropriate) for each of these parameters is recorded for each 10-minute interval. The sediment sampling station includes an automatically activated ISCO sampling pump with collection bottles for suspended sediment, which is activated when sufficient flow is present in the channel, and passive traps for bedload material that is transported down the channel during runoff events. This report presents data collected from these stations during FY2013 and FY2014.« less

NNSS Soils Monitoring: Plutonium Valley (CAU 366) FY2015

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

Nikolich, George; Mizell, Steve; McCurdy, Greg

Desert Research Institute (DRI) is conducting a field assessment of the potential for contaminated soil transport from the Plutonium Valley Contamination Area (CA) as a result of wind transport and storm runoff in support of National Nuclear Security Administration (NNSA) efforts to complete regulatory closure of the contamination areas. The DRI work is intended to confirm the likely mechanism(s) of transport and determine the meteorological conditions that might cause movement of contaminated soils. The emphasis of the work is on collecting sediment transported by channelized storm runoff at the Plutonium Valley investigation sites. These data will inform closure plans thatmore » are being developed, which will facilitate the appropriate closure design and post-closure monitoring. In 2011, DRI installed two meteorological monitoring stations south (station #1) and north (station #2) of the Plutonium Valley CA and a runoff sediment sampling station within the CA. Temperature, wind speed, wind direction, relative humidity, precipitation, solar radiation, barometric pressure, soil temperature, and airborne particulate concentration are collected at both meteorological stations. The maximum, minimum, and average or total (as appropriate) for each of these parameters are recorded for each 10-minute interval. The sediment sampling station includes an automatically activated ISCO sampling pump with collection bottles for suspended sediment, which is activated when sufficient flow is present in the channel, and passive traps for bedload material that is transported down the channel during runoff events. This report presents data collected from these stations during fiscal year (FY) 2015.« less

Lithium metal reduction of plutonium oxide to produce plutonium metal

DOEpatents

Coops, Melvin S.

1992-01-01

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

SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS

DOEpatents

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

1958-10-01

A chromatographic adsorption process is presented for the separation of plutonium from other fission products formed by the irradiation of uranium. The plutonium and the lighter element fission products are adsorbed on a sulfonated phenol-formaldehyde resin bed from a nitric acid solution containing the dissolved uranium. Successive washes of sulfuric, phosphoric, and nitric acids remove the bulk of the fission products, then an eluate of dilute phosphoric and nitric acids removes the remaining plutonium and fission products. The plutonium is selectively removed by passing this solution through zirconium phosphate, from which the plutonium is dissolved with nitric acid. This process provides a convenient and efficient means for isolating plutonium.

Volatile fluoride process for separating plutonium from other materials

DOEpatents

Spedding, F. H.; Newton, A. S.

1959-04-14

The separation of plutonium from uranium and/or fission products by formation of the higher fluorides off uranium and/or plutonium is described. Neutronirradiated uranium metal is first converted to the hydride. This hydrided product is then treated with fluorine at about 315 deg C to form and volatilize UF/sub 6/ leaving plutonium behind. Thc plutonium may then be separated by reacting the residue with fluorine at about 5004DEC and collecting the volatile plutonium fluoride thus formed.

VOLATILE FLUORIDE PROCESS FOR SEPARATING PLUTONIUM FROM OTHER MATERIALS

DOEpatents

Spedding, F.H.; Newton, A.S.

1959-04-14

The separation of plutonium from uranium and/or tission products by formation of the higher fluorides of uranium and/or plutonium is discussed. Neutronirradiated uranium metal is first convcrted to the hydride. This hydrided product is then treatced with fluorine at about 315 deg C to form and volatilize UF/sup 6/ leaving plutonium behind. The plutonium may then be separated by reacting the residue with fluorine at about 500 deg C and collecting the volatile plutonium fluoride thus formed.

SEPARATION OF PLUTONIUM FROM LANTHANUM BY CHELATION-EXTRACTION

DOEpatents

James, R.A.; Thompson, S.G.

1958-12-01

Plutonium can be separated from a mixture of plutonlum and lanthanum in which the lanthanum to plutonium molal ratio ls at least five by adding the ammonium salt of N-nitrosoarylhydroxylamine to an aqueous solution having a pH between about 3 and 0.2 and containing the plutonium in a valence state of at least +3, to form a plutonium chelate compound of N-nitrosoarylhydroxylamine. The plutonium chelate compound may be recovered from the solution by extracting with an immiscible organic solvent such as chloroform.

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

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

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

2010-01-01

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

An Update of Hydrologic Conditions and Distribution of Selected Constituents in Water, Snake River Plain Aquifer and Perched-Water Zones, Idaho National Laboratory, Idaho, Emphasis 2002-05

USGS Publications Warehouse

Davis, Linda C.

2008-01-01

Radiochemical and chemical wastewater discharged since 1952 to infiltration ponds, evaporation ponds, and disposal wells at the Idaho National Laboratory (INL) has affected water quality in the Snake River Plain aquifer and perched-water zones underlying the INL. The U.S. Geological Survey, in cooperation with the U.S. Department of Energy, maintains ground-water monitoring networks at the INL to determine hydrologic trends, and to delineate the movement of radiochemical and chemical wastes in the aquifer and in perched-water zones. This report presents an analysis of water-level and water-quality data collected from aquifer and perched-water wells in the USGS ground-water monitoring networks during 2002-05. Water in the Snake River Plain aquifer primarily moves through fractures and interflow zones in basalt, generally flows southwestward, and eventually discharges at springs along the Snake River. The aquifer is recharged primarily from infiltration of irrigation water, infiltration of streamflow, ground-water inflow from adjoining mountain drainage basins, and infiltration of precipitation. From March-May 2001 to March-May 2005, water levels in wells declined throughout the INL area. The declines ranged from about 3 to 8 feet in the southwestern part of the INL, about 10 to 15 feet in the west central part of the INL, and about 6 to 11 feet in the northern part of the INL. Water levels in perched water wells declined also, with the water level dropping below the bottom of the pump in many wells during 2002-05. For radionuclides, concentrations that equal 3s, wheres s is the sample standard deviation, represent a measurement at the minimum detectable concentration, or 'reporting level'. Detectable concentrations of radiochemical constituents in water samples from wells in the Snake River Plain aquifer at the INL generally decreased or remained constant during 2002-05. Decreases in concentrations were attributed to decreased rates of radioactive-waste disposal, radioactive decay, changes in waste-disposal methods, and dilution from recharge and underflow. In October 2005, reportable concentrations of tritium in ground water ranged from 0.51+or-0.12 to 11.5+or-0.6 picocuries per milliliter and the tritium plume extended south-southwestward in the general direction of ground-water flow. Tritium concentrations in water from several wells southwest of the Idaho Nuclear Technology and Engineering Center (INTEC) decreased or remained constant as they had during 1998-2001, with the exception of well USGS 47, which increased a few picocuries per milliliter. Most wells completed in shallow perched water at the Reactor Technology Complex (RTC) were dry during 2002---05. Tritium concentrations in deep perched water exceeded the reporting level in nine wells at the RTC. The tritium concentration in water from one deep perched water well exceeded the reporting level at the INTEC. Concentrations of strontium-90 in water from 14 of 34 wells sampled during October 2005 exceeded the reporting level. Concentrations ranged from 2.2+or-0.7 to 33.1+or-1.2 picocuries per liter. However, concentrations from most wells remained relatively constant or decreased since 1989. Strontium-90 has not been detected within the eastern Snake River Plain aquifer beneath the RTC partly because of the exclusive use of waste-disposal ponds and lined evaporation ponds rather than the disposal well for radioactive-wastewater disposal at RTC. At the RTC, strontium-90 concentrations in water from six wells completed in deep perched ground water exceeded the reporting level during 2002-05. At the INTEC, the reporting level was exceeded in water from three wells completed in deep perched ground water. During 2002-05, concentrations of plutonium-238, and plutonium-239, -240 (undivided), and americium-241 were less than the reporting level in water samples from all wells sampled at the INL. During 2002-05, concentrations of cesium-137 in water from all wells sa

Radionuclide Basics: Plutonium

EPA Pesticide Factsheets

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

Plutonium inventories for stabilization and stabilized materials

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

Williams, A.K.

1996-05-01

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

Strength and fracture of uranium, plutonium and several their alloys under shock wave loading

NASA Astrophysics Data System (ADS)

Golubev, V. K.

2012-08-01

Results on studying the spall fracture of uranium, plutonium and several their alloys under shock wave loading are presented in the paper. The problems of influence of initial temperature in a range of - 196 - 800∘C and loading time on the spall strength and failure character of uranium and two its alloys with molybdenum and both molybdenum and zirconium were studied. The results for plutonium and its alloy with gallium were obtained at a normal temperature and in a temperature range of 40-315∘C, respectively. The majority of tests were conducted with the samples in the form of disks 4 mm in thickness. They were loaded by the impact of aluminum plates 4 mm thick through a copper screen 12 mm thick serving as the cover or bottom part of a special container. The character of spall failure of materials and the damage degree of samples were observed on the longitudinal metallographic sections of recovered samples. For a concrete test temperature, the impact velocity was sequentially changed and therefore the loading conditions corresponding to the consecutive transition from microdamage nucleation up to complete macroscopic spall fracture were determined. The conditions of shock wave loading were calculated using an elastic-plastic computer program. The comparison of obtained results with the data of other researchers on the spall fracture of examined materials was conducted.

Risk of Lung Cancer Mortality in Nuclear Workers from Internal Exposure to Alpha Particle-emitting Radionuclides

PubMed Central

Atkinson, Will; Bérard, Philippe; Bingham, Derek; Birchall, Alan; Blanchardon, Eric; Bull, Richard; Guseva Canu, Irina; Challeton-de Vathaire, Cécile; Cockerill, Rupert; Do, Minh T.; Engels, Hilde; Figuerola, Jordi; Foster, Adrian; Holmstock, Luc; Hurtgen, Christian; Laurier, Dominique; Puncher, Matthew; Riddell, Anthony E.; Samson, Eric; Thierry-Chef, Isabelle; Tirmarche, Margot; Vrijheid, Martine; Cardis, Elisabeth

2017-01-01

Background: Carcinogenic risks of internal exposures to alpha-emitters (except radon) are poorly understood. Since exposure to alpha particles—particularly through inhalation—occurs in a range of settings, understanding consequent risks is a public health priority. We aimed to quantify dose–response relationships between lung dose from alpha-emitters and lung cancer in nuclear workers. Methods: We conducted a case–control study, nested within Belgian, French, and UK cohorts of uranium and plutonium workers. Cases were workers who died from lung cancer; one to three controls were matched to each. Lung doses from alpha-emitters were assessed using bioassay data. We estimated excess odds ratio (OR) of lung cancer per gray (Gy) of lung dose. Results: The study comprised 553 cases and 1,333 controls. Median positive total alpha lung dose was 2.42 mGy (mean: 8.13 mGy; maximum: 316 mGy); for plutonium the median was 1.27 mGy and for uranium 2.17 mGy. Excess OR/Gy (90% confidence interval)—adjusted for external radiation, socioeconomic status, and smoking—was 11 (2.6, 24) for total alpha dose, 50 (17, 106) for plutonium, and 5.3 (−1.9, 18) for uranium. Conclusions: We found strong evidence for associations between low doses from alpha-emitters and lung cancer risk. The excess OR/Gy was greater for plutonium than uranium, though confidence intervals overlap. Risk estimates were similar to those estimated previously in plutonium workers, and in uranium miners exposed to radon and its progeny. Expressed as risk/equivalent dose in sieverts (Sv), our estimates are somewhat larger than but consistent with those for atomic bomb survivors. See video abstract at, http://links.lww.com/EDE/B232. PMID:28520643

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

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

Bouzigues, H.; Reneaud, J.-M.

1963-01-01

A method and a special apparatus are described which make it possible to detach the insoluble plutonium salt deposits in the extraction chain of an irradiated fuel treatment plant. The process chosen allows the detection, in the extraction batteries or in the highly active chemical engineering equipment, of plutonium quantities of a few grams. After four years operation it has been impossible to detect measurable quantities of plutonium in any part of the extraction chain. The results have been confirmed by visual examinations carried out with a specially constructed endoscope. (auth)

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

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

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

1989-09-07

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

SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS

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

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

A chromatographic adsorption process is presented for the separation of plutonium from other fission products formed by the irradiation of uranium. The plutonium and the lighter element fission products are adsorbed on a sulfonated phenol-formaldehyde resin bed from a nitric acid solution containing the dissolved uranium. Successive washes of sulfuric, phosphoric, and nitric acids remove the bulk of the fission products, then an eluate of dilute phosphoric and nitric acids removes the remaining plutonium and fission products. The plutonium is selectively removed by passing this solution through zirconium phosphate, from which the plutonium is dissolved with nitric acid. This processmore » provides a convenient and efficient means for isolating plutonium.« less

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

PROCESS FOR SEPARATING PLUTONIUM FROM IMPURITIES

DOEpatents

Wahl, A.C.

1957-11-12

A method is described for separating plutonium from aqueous solutions containing uranium. It has been found that if the plutonium is reduced to its 3+ valence state, and the uranium present is left in its higher valence state, then the differences in solubility between certain salts (e.g., oxalates) of the trivalent plutonium and the hexavalent uranium can be used to separate the metals. This selective reduction of plutonium is accomplished by adding iodide ion to the solution, since iodide possesses an oxidation potential sufficient to reduce plutonium but not sufficient to reduce uranium.

PRODUCTION OF PLUTONIUM FLUORIDE FROM BISMUTH PHOSPHATE PRECIPITATE CONTAINING PLUTONIUM VALUES

DOEpatents

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

1961-05-01

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

PLUTONIUM COMPOUNDS AND PROCESS FOR THEIR PREPARATION

DOEpatents

Wolter, F.J.; Diehl, H.C. Jr.

1958-01-01

This patent relates to certain new compounds of plutonium, and to the utilization of these compounds to effect purification or separation of the plutonium. The compounds are organic chelate compounds consisting of tetravalent plutonium together with a di(salicylal) alkylenediimine. These chelates are soluble in various organic solvents, but not in water. Use is made of this property in extracting the plutonium by contacting an aqueous solution thereof with an organic solution of the diimine. The plutonium is chelated, extracted and effectively separated from any impurities accompaying it in the aqueous phase.

Method of separating thorium from plutonium

DOEpatents

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

DOEpatents

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

DOEpatents

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.

137Cs and plutonium isotopes accumulation/retention in bottom sediments and soil in Lithuania: A case study of the activity concentration of anthropogenic radionuclides and their provenance before the start of operation of the Belarusian Nuclear Power Plant (NPP).

PubMed

Marčiulionienė, D; Lukšienė, B; Montvydienė, D; Jefanova, O; Mažeika, J; Taraškevičius, R; Stakėnienė, R; Petrošius, R; Maceika, E; Tarasiuk, N; Žukauskaitė, Z; Kazakevičiūtė, L; Volkova, M

2017-11-01

Knowledge of the background activity concentrations of anthropogenic radionuclides before the start of operations of the new nuclear facilities in Belarus is of great value worldwide. Inland water bodies in Lithuania (specifically the Neris River, the Nemunas River and the Curonian Lagoon) are near the site of the Belarusian NPP under construction and, for this reason, sediments and flooded soils from these sensitive areas were analysed for radiocesium and plutonium isotopes (macrophytes were analysed only for 137 Cs) in 2011-2012. The 137 Cs and 239+240 Pu activity concentrations in bottom sediments from the Nemunas River, sampled in 1995-1996 and re-calculated to the year 2016, were compared with those of 2011-2012. The obtained activity of 137 Cs in bottom sediments of the Nemunas River and Curonian Lagoon varied from 1 Bq/kg to 47.0 Bq/kg. The activity of 137 Cs in the tested soils ranged from 5.3 B g/kg to 32.9 Bq/kg. The 239+240 Pu activity in bottom sediments of the studied sampling sites varied between 0.016 and 0.34 Bq/kg and in flooded soils from 0.064 to 0.55 Bq/kg. The 238 Pu activity values were very low or lower than the detection limit. The activity of 137 Cs in macrophytes varied from values lower than the detection limit to 6 Bq/kg. A strong positive linear correlation for bottom sediments was calculated between: 239+240 Pu and total organic carbon (TOC), r = 0.86, p-value 0.01; 239+240 Pu and silt, r = 0.80, p-value 0.029; 137 Cs and silt, r = 0.78, p-value 0.04; and 137 Cs and TOC, r = 0.85, p-value 0.015. The similar peculiarities of 137 Cs and 239+240 Pu accumulation in bottom sediments and flooded soil allow us to assume that 137 Cs can be used as a tracer for 239+240 Pu in the initial stage of searching for radionuclide accumulation zones. A remaining impact of the Chernobyl fallout in average comprised: in the Lower Nemunas River and Curonian Lagoon sediments - 51%, in the Middle Nemunas River -90% and in the floodplains of the Nemunas River - 59%, while the provenance of plutonium in studied bottom sediments and flooded soil was the global fallout. Copyright © 2017 Elsevier Ltd. All rights reserved.

Locating trace plutonium in contaminated soil using micro-XRF imaging

DOE PAGES

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

2014-06-01

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

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

Separation of plutonium from lanthanum by electrolysis in LiCl KCl onto molten bismuth electrode

NASA Astrophysics Data System (ADS)

Serp, J.; Lefebvre, P.; Malmbeck, R.; Rebizant, J.; Vallet, P.; Glatz, J.-P.

2005-04-01

This work presents a study on the electroseparation of plutonium from lanthanum using molten bismuth electrodes in LiCl-KCl eutectic at 733 K. The reduction potentials of Pu3+ and La3+ ions were measured on a Bi thin film electrode using cyclic voltammetry (CV). A difference between the peak potentials for the formation of PuBi2 and LaBi2 of approximately 100 mV was found. Separation tests were then carried out using different current densities and salt phase compositions between a plutonium rod anode and an unstirred molten Bi cathode in order to evaluate the efficiency of an electrolytic separation process. At a current density of 12 mA/cm2/wt% (Pu3+), only Pu3+ ions are reduced into the molten Bi electrode, leaving La3+ ions in the salt melt. Similar results were found at two different Pu/La concentration ratios ([Pu]/[La] = 4 and 10). At a current density of 26 mA/cm2/wt% (Pu3+), co-reduction of Pu and La was observed as expected by the large negative potential of the Bi cathode during the separation test.

Patents – Melvin Calvin

Science.gov Websites

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

Stabilizing stored PuO2 with addition of metal impurities

NASA Astrophysics Data System (ADS)

Moten, Shafaq; Huda, Muhammad

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

PROCESSES FOR SEPARATING AND RECOVERING CONSTITUENTS OF NEUTRON IRRADIATED URANIUM

DOEpatents

Connick, R.E.; Gofman, J.W.; Pimentel, G.C.

1959-11-10

Processes are described for preparing plutonium, particularly processes of separating plutonium from uranium and fission products in neutron-irradiated uraniumcontaining matter. Specifically, plutonium solutions containing uranium, fission products and other impurities are contacted with reducing agents such as sulfur dioxide, uranous ion, hydroxyl ammonium chloride, hydrogen peroxide, and ferrous ion whereby the plutoninm is reduced to its fluoride-insoluble state. The reduced plutonium is then carried out of solution by precipitating niobic oxide therein. Uranium and certain fission products remain behind in the solution. Certain other fission products precipitate along with the plutonium. Subsequently, the plutonium and fission product precipitates are redissolved, and the solution is oxidized with oxidizing agents such as chlorine, peroxydisulfate ion in the presence of silver ion, permanganate ion, dichromate ion, ceric ion, and a bromate ion, whereby plutonium is oxidized to the fluoride-soluble state. The oxidized solution is once again treated with niobic oxide, thus precipitating the contamirant fission products along with the niobic oxide while the oxidized plutonium remains in solution. Plutonium is then recovered from the decontaminated solution.

Air Monitoring Network at Tonopah Test Range: Network Description and Capabilities

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

Jeffrey Tappen; George Nikolich; Ken Giles

2010-05-18

During the period April to June 2008, at the behest of the U.S. Department of Energy (DOE) National Nuclear Security Administration, Nevada Site Office (NNSA/NSO); the Desert Research Institute (DRI) constructed and deployed two portable environmental monitoring stations at the Tonopah Test Range (TTR) as part of the Environmental Restoration Project Soils Sub-Project. The TTR is located within the boundaries of the Nevada Test and Training Range (NTTR) near the northern edge, and covers an area of approximately 725.20 km2 (179,200 acres). The primary objective of the monitoring stations is to evaluate whether and under what conditions there is windmore » transport of radiological contaminants from one of the three Soil Sub-Project Corrective Action Units (CAUs) associated with Operation Roller Coaster on TTR. Operation Roller Coaster was a series of tests, conducted in 1963, designed to examine the stability and dispersal of plutonium in storage and transportation accidents. These tests did not result in any nuclear explosive yield. However, the tests did result in the dispersal of plutonium and contamination of surface soils in the surrounding area.« less

TECHNICAL EVALUATION OF REMEDIATION TECHNOLOGIES FOR PLUTONIUM-CONTAMINATED SOILS AT THE NEVADA TEST SITE (NTS)

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

Steve Hoeffner

2003-12-31

The Clemson Environmental Technologies Laboratory (CETL) was contracted by the National Energy Technology Center to evaluate technologies that might be used to reduce the volume of plutonium-contaminated soil at the Nevada Test Site. The project has been systematically approached. A thorough review and summary was completed for: (1) The NTS soil geological, geochemical and physical characteristics; (2) The characteristics and chemical form of the plutonium that is in these soils; (3) Previous volume reduction technologies that have been attempted on the NTS soils; (4) Vendors with technology that may be applicable; and (5) Related needs at other DOE sites. Soilsmore » from the Nevada Test Site were collected and delivered to the CETL. Soils were characterized for Pu-239/240, Am-241 and gross alpha. In addition, wet sieving and the subsequent characterization were performed on soils before and after attrition scrubbing to determine the particle size distribution and the distribution of Pu-239/240 and gross alpha as a function of particle size. Sequential extraction was performed on untreated soil to provide information about how tightly bound the plutonium was to the soil. Magnetic separation was performed to determine if this could be useful as part of a treatment approach. Using the information obtained from these reviews, three vendors were selected to demonstration their volume reduction technologies at the CETL. Two of the three technologies, bioremediation and soil washing, met the performance criteria. Both were able to significantly reduce the concentration plutonium in the soil from around 1100 pCi/g to 200 pCi/g or less with a volume reduction of around 95%, well over the target 70%. These results are especially encouraging because they indicate significant improvement over that obtained in these earlier pilot and field studies. Additional studies are recommended.« less

CHEMICAL DIFFERENCES BETWEEN SLUDGE SOLIDS AT THE F AND H AREA TANK FARMS

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

Reboul, S.

2012-08-29

The primary source of waste solids received into the F Area Tank Farm (FTF) was from PUREX processing performed to recover uranium and plutonium from irradiated depleted uranium targets. In contrast, two primary sources of waste solids were received into the H Area Tank Farm (HTF): a) waste from PUREX processing; and b) waste from H-modified (HM) processing performed to recover uranium and neptunium from burned enriched uranium fuel. Due to the differences between the irradiated depleted uranium targets and the burned enriched uranium fuel, the average compositions of the F and H Area wastes are markedly different from onemore » another. Both F and H Area wastes contain significant amounts of iron and aluminum compounds. However, because the iron content of PUREX waste is higher than that of HM waste, and the aluminum content of PUREX waste is lower than that of HM waste, the iron to aluminum ratios of typical FTF waste solids are appreciably higher than those of typical HTF waste solids. Other constituents present at significantly higher concentrations in the typical FTF waste solids include uranium, nickel, ruthenium, zinc, silver, cobalt and copper. In contrast, constituents present at significantly higher concentrations in the typical HTF waste solids include mercury, thorium, oxalate, and radionuclides U-233, U-234, U-235, U-236, Pu-238, Pu-242, Cm-244, and Cm-245. Because of the higher concentrations of Pu-238 in HTF, the long-term concentrations of Th-230 and Ra-226 (from Pu-238 decay) will also be higher in HTF. The uranium and plutonium distributions of the average FTF waste were found to be consistent with depleted uranium and weapons grade plutonium, respectively (U-235 comprised 0.3 wt% of the FTF uranium, and Pu-240 comprised 6 wt% of the FTF plutonium). In contrast, at HTF, U-235 comprised 5 wt% of the uranium, and Pu-240 comprised 17 wt% of the plutonium, consistent with enriched uranium and high burn-up plutonium. X-ray diffraction analyses of various FTF and HTF samples indicated that the primary crystalline compounds of iron in sludge solids are Fe{sub 2}O{sub 3}, Fe{sub 3}O{sub 4}, and FeO(OH), and the primary crystalline compounds of aluminum are Al(OH){sub 3} and AlO(OH). Also identified were carbonate compounds of calcium, magnesium, and sodium; a nitrated sodium aluminosilicate; and various uranium compounds. Consistent with expectations, oxalate compounds were identified in solids associated with oxalic acid cleaning operations. The most likely oxidation states and chemical forms of technetium are assessed in the context of solubility, since technetium-99 is a key risk driver from an environmental fate and transport perspective. The primary oxidation state of technetium in SRS sludge solids is expected to be Tc(IV). In salt waste, the primary oxidation state is expected to be Tc(VII). The primary form of technetium in sludge is expected to be a hydrated technetium dioxide, TcO{sub 2} {center_dot} xH{sub 2}O, which is relatively insoluble and likely co-precipitated with iron. In salt waste solutions, the primary form of technetium is expected to be the very soluble pertechnetate anion, TcO{sub 4}{sup -}. The relative differences between the F and H Tank Farm waste provide a basis for anticipating differences that will occur as constituents of FTF and HTF waste residue enter the environment over the long-term future. If a constituent is significantly more dominant in one of the Tank Farms, its long-term environmental contribution will likely be commensurately higher, assuming the environmental transport conditions of the two Tank Farms share some commonality. It is in this vein that the information cited in this document is provided - for use during the generation, assessment, and validation of Performance Assessment modeling results.« less

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

DOEpatents

Faris, B.F.

1961-04-25

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

Real-Time, Fast Neutron Coincidence Assay of Plutonium With a 4-Channel Multiplexed Analyzer and Organic Scintillators

NASA Astrophysics Data System (ADS)

Joyce, Malcolm J.; Gamage, Kelum A. A.; Aspinall, M. D.; Cave, F. D.; Lavietes, A.

2014-06-01

The design, principle of operation and the results of measurements made with a four-channel organic scintillator system are described. The system comprises four detectors and a multiplexed analyzer for the real-time parallel processing of fast neutron events. The function of the real-time, digital multiple-channel pulse-shape discrimination analyzer is described together with the results of laboratory-based measurements with 252Cf, 241Am-Li and plutonium. The analyzer is based on a single-board solution with integrated high-voltage supplies and graphical user interface. It has been developed to meet the requirements of nuclear materials assay of relevance to safeguards and security. Data are presented for the real-time coincidence assay of plutonium in terms of doubles count rate versus mass. This includes an assessment of the limiting mass uncertainty for coincidence assay based on a 100 s measurement period and samples in the range 0-50 g. Measurements of count rate versus order of multiplicity for 252Cf and 241Am-Li and combinations of both are also presented.

Project 57 Air Monitoring Report: January 1 through December 31, 2015

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

Mizell, Steve A; Nikolich, George; Shadel, Craig

2017-01-01

On April 24, 1957, the Atomic Energy Commission (AEC, now the Department of Energy [DOE]) conducted the Project 57 safety experiment in western Emigrant Valley north east of the Nevada National Security Site (NNSS, formerly the Nevada Test Site) on lands withdrawn by the Department of Defense (DOD) for the Nevada Test and Training Range (NTTR). The test was undertaken to develop (1) a means of estimating plutonium distribution resulting from a non-nuclear detonation; (2) biomedical evaluation techniques for use in plutonium-laden environments; (3) methods of surface decontamination; and (4) instruments and field procedures for prompt estimation of alpha contaminationmore » (Shreve, 1958). Although the test did not result in the fission of nuclear materials, it did disseminate plutonium across the land surface. Following the experiment, the AEC fenced the contaminated area and returned control of the surrounding land to the DOD. Various radiological surveys were performed in the area and in 2007, the DOE expanded the demarked Contamination Area by posting signs 200 to 400 feet (60 to 120 meters) outside of the original fence.« less

Project 57 Air Monitoring Report: January 1 through December 31, 2016

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

Mizell, Steve A.; Nikolich, George; Shadel, Craig

On April 24, 1957, the Atomic Energy Commission (AEC, now the Department of Energy [DOE]) conducted the Project 57 safety experiment in western Emigrant Valley northeast of the Nevada National Security Site (NNSS, formerly the Nevada Test Site) on lands withdrawn by the Department of Defense (DOD) for the Nevada Test and Training Range (NTTR). The test was undertaken to develop (1) a means of estimating plutonium distribution resulting from a non-nuclear detonation; (2) biomedical evaluation techniques for use in plutonium-laden environments; (3) methods of surface decontamination; and (4) instruments and field procedures for prompt estimation of alpha contamination (Shreve,more » 1958). Although the test did not result in the fission of nuclear materials, it did disseminate plutonium across the land surface. Following the experiment, the AEC fenced the contaminated area and returned control of the surrounding land to the DOD. Various radiological surveys were performed in the area and in 2007, the DOE expanded the demarked Contamination Area (CA) by posting signs 200 to 400 ft (60 to 120 m) outside of the original fence.« less

Processing of irradiated, enriched uranium fuels at the Savannah River Plant

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

Hyder, M L; Perkins, W C; Thompson, M C

Uranium fuels containing /sup 235/U at enrichments from 1.1% to 94% are processed and recovered, along with neptunium and plutonium byproducts. The fuels to be processed are dissolved in nitric acid. Aluminum-clad fuels are disssolved using a mercury catalyst to give a solution rich in aluminum. Fuels clad in more resistant materials are dissolved in an electrolytic dissolver. The resulting solutions are subjected to head-end treatment, including clarification and adjustment of acid and uranium concentration before being fed to solvent extraction. Uranium, neptunium, and plutonium are separated from fission products and from one another by multistage countercurrent solvent extraction withmore » dilute tri-n-butyl phosphate in kerosene. Nitric acid is used as the salting agent in addition to aluminum or other metal nitrates present in the feed solution. Nuclear safety is maintained through conservative process design and the use of monitoring devices as secondary controls. The enriched uranium is recovered as a dilute solution and shipped off-site for further processing. Neptunium is concentrated and sent to HB-Line for recovery from solution. The relatively small quantities of plutonium present are normally discarded in aqueous waste, unless the content of /sup 238/Pu is high enough to make its recovery desirable. Most of the /sup 238/Pu can be recovered by batch extraction of the waste solution, purified by counter-current solvent extraction, and converted to oxide in HB-Line. By modifying the flowsheet, /sup 239/Pu can be recovered from low-enriched uranium in the extraction cycle; neptunium is then not recovered. The solvent is subjected to an alkaline wash before reuse to remove degraded solvent and fission products. The aqueous waste is concentrated and partially deacidified by evaporation before being neutralized and sent to the waste tanks; nitric acid from the overheads is recovered for reuse.« less

Application of isotope-dilution laser ablation ICP-MS for direct determination of Pu concentrations in soils at pg g(-1) levels.

PubMed

Boulyga, Sergei F; Tibi, Markus; Heumann, Klaus G

2004-01-01

The methods available for determination of environmental contamination by plutonium at ultra-trace levels require labor-consuming sample preparation including matrix removal and plutonium extraction in both nuclear spectroscopy and mass spectrometry. In this work, laser-ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) was applied for direct analysis of Pu in soil and sediment samples. Application of a LINA-Spark-Atomizer system (a modified laser ablation system providing high ablation rates) coupled with a sector-field ICP-MS resulted in detection limits as low as 3x10(-13) g g(-1) for Pu isotopes in soil samples containing uranium at a concentration of a few microg g(-1). The isotope dilution (ID) technique was used for quantification, which compensated for matrix effects in LA-ICP-MS. Interferences by UH+ and PbO2+ ions and by the peak tail of 238U+ ions were reduced or separated by use of dry plasma conditions and a mass resolution of 4000, respectively. No other effects affecting measurement accuracy, except sample inhomogeneity, were revealed. Comparison of results obtained for three contaminated soil samples by use of alpha-spectrometry, ICP-MS with sample decomposition, and LA-ICP-IDMS showed, in general, satisfactory agreement of the different methods. The specific activity of (239+240)Pu (9.8 +/- 3.0 mBq g(-1)) calculated from LA-ICP-IDMS analysis of SRM NIST 4357 coincided well with the certified value of 10.4 +/- 0.2 mBq g(-1). However, the precision of LA-ICP-MS for determination of plutonium in inhomogeneous samples, i.e. if "hot" particles are present, is limited. As far as we are aware this paper reports the lowest detection limits and element concentrations yet measured in direct LA-ICP-MS analysis of environmental samples.

METHOD OF PRODUCING PLUTONIUM TETRAFLUORIDE

DOEpatents

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

1959-12-15

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

Measurement system for alpha emitters in solution

NASA Astrophysics Data System (ADS)

Robert, A.; Sella, C.; Heindl, R.

1984-08-01

The measurement of alpha emitter concentrations in solution corresponds to a need felt in particular by laboratories working on actinides and in the spent fuel reprocessing industry. The instrument present here allows this measurement continuously by the use of a new scintillator that is insensitive to corrosive liquids. The extreme thinness of the scintillator guarantees good detection selectivity of alpha particles in the presence of beta and gamma emissions. Examples of uranium-233, plutonium-239 and americium-241 concentration measurements are presented.

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

Tabulated Neutron Emission Rates for Plutonium Oxide

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

Shores, Erik Frederick

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

PROCESS OF SEPARATING PLUTONIUM FROM URANIUM

DOEpatents

Brown, H.S.; Hill, O.F.

1958-09-01

A process is presented for recovering plutonium values from aqueous solutions. It comprises forming a uranous hydroxide precipitate in such a plutonium bearing solution, at a pH of at least 5. The plutonium values are precipitated with and carried by the uranium hydroxide. The carrier precipitate is then redissolved in acid solution and the pH is adjusted to about 2.5, causing precipitation of the uranous hydroxide but leaving the still soluble plutonium values in solution.

COLUMBIC OXIDE ADSORPTION PROCESS FOR SEPARATING URANIUM AND PLUTONIUM IONS

DOEpatents

Beaton, R.H.

1959-07-14

A process is described for separating plutonium ions from a solution of neutron irradiated uranium in which columbic oxide is used as an adsorbert. According to the invention the plutonium ion is selectively adsorbed by Passing a solution containing the plutonium in a valence state not higher than 4 through a porous bed or column of granules of hydrated columbic oxide. The adsorbed plutonium is then desorbed by elution with 3 N nitric acid.

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

DOEpatents

Finzel, T.G.

1959-03-10

A process is described for separating plutonium from fission products carried therewith when plutonium in the reduced oxidation state is removed from a nitric acid solution of irradiated uranium by means of bismuth phosphate as a carrier precipitate. The bismuth phosphate carrier precipitate is dissolved by treatment with nitric acid and the plutonium therein is oxidized to the hexavalent oxidation state by means of potassium dichromate. Separation of the plutonium from the fission products is accomplished by again precipitating bismuth phosphate and removing the precipitate which now carries the fission products and a small percentage of the plutonium present. The amount of plutonium carried in this last step may be minimized by addition of sodium fluoride, so as to make the solution 0.03N in NaF, prior to the oxidation and prccipitation step.

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

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

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

2000-09-28

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

PROCESS FOR THE SEPARATION OF HEAVY METALS

DOEpatents

Gofman, J.W.; Connick, R.E.; Wahl, A.C.

1959-01-27

A method is presented for thc separation of plutonium from uranium and the fission products with which it is associated. The method is based on the fact that hexavalent plutonium forms an insoluble complex precipitate with sodium acetate, as does the uranyl ion, while reduced plutonium is not precipitated by sodium acetate. Several embodiments are shown, e.g., a solution containing plutonium and uranium in the hexavalent state may be contacted with sodium acetate causing the formation of a sodium uranyl acetate precipitate which carries the plutonium values while the fission products remain in solution. If the original solution is treated with a reducing agent, so that the plutonium is reduced while the uranium remains in the hexavalent state, and sodium and acetate ions are added, the uranium will precipitutc while the plutonium remains in solution effecting separation of the Pu from urarium.

Radionuclide Concentrations in Terrestrial Vegetation and Soil Samples On and Around the Hanford Site, 1971 Through 2008

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

Simmons, Mary Ann; Poston, Ted M.; Fritz, Brad G.

2011-07-29

Environmental monitoring is conducted on the U.S. Department of Energy (DOE) Hanford Site to comply with DOE Orders and federal and state regulations. Major objectives of the monitoring are to characterize contaminant levels in the environment and to determine site contributions to the contaminant inventory. This report focuses on surface soil and perennial vegetation samples collected between 1971 and 2008 as part of the Pacific Northwest National Laboratory Surface Environmental Surveillance Project performed under contract to DOE. Areas sampled under this program are located on the Hanford Site but outside facility boundaries and on public lands surrounding the Hanford Site.more » Additional samples were collected during the past 8 years under DOE projects that evaluated parcels of land for radiological release. These data were included because the same sampling methodology and analytical laboratory were used for the projects. The spatial and temporal trends of six radionuclides collected over a 38-year period were evaluated. The radionuclides----cobalt-60, cesium-137, strontium-90, plutonium-238, plutonium-239/240, and uranium (reported either as uranium-238 or total uranium)----were selected because they persist in the environment and are still being monitored routinely and reported in Hanford Site environmental reports. All these radionuclides were associated with plutonium production and waste management of activities occurring on the site. Other sources include fallout from atmospheric testing of nuclear weapons, which ended in 1980, and the Chernobyl explosion in 1986. Uranium is also a natural component of the soil. This assessment of soil and vegetation data provides important information on the distribution of radionuclides in areas adjacent to industrial areas, established perimeter locations and buffer areas, and more offsite nearby and distant locations. The concentrations reflect a tendency for detection of some radionuclides close to where they were utilized onsite, but as one moves to unindustrialized areas on the site, surrounding buffer areas and perimeter location into the more distant sites, concentrations of these radionuclides approach background and cannot be distinguished from fallout activity. More importantly, concentrations in soil and vegetation samples did not exceed environmental benchmark concentrations, and associated exposure to human and ecological receptors were well below levels that are demonstratively hazardous to human health and the environment.« less

Selection of Russian Plutonium Beryllium Sources for Inclusion in the Nuclear Mateirals Information Program Archive

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

NON-AQUEOUS DISSOLUTION OF MASSIVE PLUTONIUM

DOEpatents

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

1959-05-12

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

OXIDATIVE METHOD OF SEPARATING PLUTONIUM FROM NEPTUNIUM

DOEpatents

Beaufait, L.J. Jr.

1958-06-10

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

PROCESS OF ELIMINATING HYDROGEN PEROXIDE IN SOLUTIONS CONTAINING PLUTONIUM VALUES

DOEpatents

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

1960-09-27

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

Continuous plutonium dissolution apparatus

DOEpatents

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)

Room airflow studies using sonic anemometry.

PubMed

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%.

Certification of Plutonium Standards for KAMS Neutron Multiplicity Counter

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

Salaymeh, S.R.

2002-05-31

As part of the implementation of the PEIS record of decision in January of 1997, DOE will pursue two technologies to disposition fifty metric tons of its stockpile of plutonium. As a result of this and in order to expedite the closure of Rocky Flats Environmental Technology Site in Colorado, DOE decided to use existing facilities at the Savannah River Site (SRS) for storing all material containing plutonium at KAMS. A neutron multiplicity counter was designed and built to carry out receipt verification measurement at the facility. Since the material covers a wide range and different levels of impurities, itmore » is essential that we obtain a set of working standards. An agreement was drafted to select the first drums to be these standards. A plan was developed for the certification of these standards using Rocky Flat's existing nondestructive assay equipment. This paper will discuss the types of materials to be shipped to SRS, number of standards to certify for each type of material, and the certification plan. It will also discuss the activities necessary to determine the nuclear content of these working standards to be used at SRS facilities in support of shipment and receipt of the Pu containing materials. Definition of instrument qualifications, measurement control processes, measurement methodologies, and calculations necessary to report the gram quantities and their uncertainties for plutonium, americium-241, uranium-235 (if present) and neptunium-237 (if present) will also be presented.« less

Re-solution of xenon clusters in plutonium dioxide under the collision cascade impact: A molecular dynamics simulation

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.

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

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

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

PROCESS FOR SEPARATING PLUTONIUM BY REPEATED PRECIPITATION WITH AMPHOTERIC HYDROXIDE CARRIERS

DOEpatents

Faris, B.F.

1960-04-01

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

PROCESS FOR SEPARATION OF HEAVY METALS

DOEpatents

Duffield, R.B.

1958-04-29

A method is described for separating plutonium from aqueous acidic solutions of neutron-irradiated uranium and the impurities associated therewith. The separation is effected by adding, to the solution containing hexavalent uranium and plutonium, acetate ions and the ions of an alkali metal and those of a divalent metal and thus forming a complex plutonium acetate salt which is carried by the corresponding complex of uranium, such as sodium magnesium uranyl acetate. The plutonium may be separated from the precipitated salt by taking the same back into solution, reducing the plutonium to a lower valent state on reprecipitating the sodium magnesium uranyl salt, removing the latter, and then carrying the plutonium from ihe solution by means of lanthanum fluoride.

PROCESS FOR THE RECOVERY OF PLUTONIUM

DOEpatents

Ritter, D.M.

1959-01-13

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

Stabilization and immobilization of military plutonium: A non-proliferation perspective

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

Leventhal, P.

1996-05-01

The Nuclear Control Institute welcomes this DOE-sponsored technical workshop on stabilization and immobilization of weapons plutonium (W Pu) because of the significant contribution it can make toward the ultimate non-proliferation objective of eliminating weapons-usable nuclear material, plutonium and highly enriched uranium (HEU), from world commerce. The risk of theft or diversion of these materials warrants concern, as only a few kilograms in the hands of terrorists or threshold states would give them the capability to build nuclear weapons. Military plutonium disposition questions cannot be addressed in isolation from civilian plutonium issues. The National Academy of Sciences has urged that {open_quotes}furthermore » steps should be taken to reduce the proliferation risks posed by all of the world`s plutonium stocks, military and civilian, separated and unseparated...{close_quotes}. This report discusses vitrification and a mixed oxide fuels option, and the effects of disposition choices on civilian plutonium fuel cycles.« less

PRECIPITATION OF PLUTONOUS PEROXIDE

DOEpatents

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

1961-08-15

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

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

DOEpatents

Angerman, A.A.

1958-10-21

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

PLUTONIUM-THORIUM ALLOYS

DOEpatents

Schonfeld, F.W.

1959-09-15

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

The Fireball integrated code package

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

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

1997-07-01

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

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

PubMed

Esaka, Fumitaka; Magara, Masaaki; Suzuki, Daisuke; Miyamoto, Yutaka; Lee, Chi-Gyu; Kimura, Takaumi

2010-12-15

Information on plutonium isotope ratios in individual particles is of great importance for nuclear safeguards, nuclear forensics and so on. Although secondary ion mass spectrometry (SIMS) is successfully utilized for the analysis of individual uranium particles, the isobaric interference of americium-241 to plutonium-241 makes difficult to obtain accurate isotope ratios in individual plutonium particles. In the present work, an analytical technique by a combination of chemical separation and inductively coupled plasma mass spectrometry (ICP-MS) is developed and applied to isotope ratio analysis of individual sub-micrometer plutonium particles. The ICP-MS results for individual plutonium particles prepared from a standard reference material (NBL SRM-947) indicate that the use of a desolvation system for sample introduction improves the precision of isotope ratios. In addition, the accuracy of the (241)Pu/(239)Pu isotope ratio is much improved, owing to the chemical separation of plutonium and americium. In conclusion, the performance of the proposed ICP-MS technique is sufficient for the analysis of individual plutonium particles. Copyright © 2010 Elsevier B.V. All rights reserved.

Plutonium recovery from spent reactor fuel by uranium displacement

DOEpatents

Ackerman, John P.

1992-01-01

A process for separating uranium values and transuranic values from fission products containing rare earth values when the values are contained together in a molten chloride salt electrolyte. A molten chloride salt electrolyte with a first ratio of plutonium chloride to uranium chloride is contacted with both a solid cathode and an anode having values of uranium and fission products including plutonium. A voltage is applied across the anode and cathode electrolytically to transfer uranium and plutonium from the anode to the electrolyte while uranium values in the electrolyte electrolytically deposit as uranium metal on the solid cathode in an amount equal to the uranium and plutonium transferred from the anode causing the electrolyte to have a second ratio of plutonium chloride to uranium chloride. Then the solid cathode with the uranium metal deposited thereon is removed and molten cadmium having uranium dissolved therein is brought into contact with the electrolyte resulting in chemical transfer of plutonium values from the electrolyte to the molten cadmium and transfer of uranium values from the molten cadmium to the electrolyte until the first ratio of plutonium chloride to uranium chloride is reestablished.

Effect of Natural Organic Matter on Plutonium Sorption to Goethite

DOE PAGES

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

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

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

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

PubMed Central

Froidevaux, Pascal; Haldimann, Max

2008-01-01

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

REMOVAL OF LEGACY PLUTONIUM MATERIALS FROM SWEDEN

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

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

2013-08-18

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

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

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

METHOD OF SEPARATING PLUTONIUM

DOEpatents

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.

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

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

Grison, E.

1961-01-01

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

Siegfried S. Hecker, Plutonium, and Nonproliferation

Science.gov Websites

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

PLUTONIUM RECOVERY FROM NEUTRON-BOMBARDED URANIUM FUEL

DOEpatents

Moore, R.H.

1962-04-10

A process of recovering plutonium from neutronbombarded uranium fuel by dissolving the fuel in equimolar aluminum chloride-potassium chloride; heating the mass to above 700 deg C for decomposition of plutonium tetrachloride to the trichloride; extracting the plutonium trichloride into a molten salt containing from 40 to 60 mole % of lithium chloride, from 15 to 40 mole % of sodium chloride, and from 0 to 40 mole % of potassium chloride or calcium chloride; and separating the layer of equimolar chlorides containing the uranium from the layer formed of the plutonium-containing salt is described. (AEC)

SEPARATION OF RUTHENIUM FROM AQUEOUS SOLUTIONS

DOEpatents

Callis, C.F.; Moore, R.L.

1959-09-01

>The separation of ruthenium from aqueous solutions containing uranium plutonium, ruthenium, and fission products is described. The separation is accomplished by providing a nitric acid solution of plutonium, uranium, ruthenium, and fission products, oxidizing plutonium to the hexavalent state with sodium dichromate, contacting the solution with a water-immiscible organic solvent, such as hexone, to extract plutonyl, uranyl, ruthenium, and fission products, reducing with sodium ferrite the plutonyl in the solvent phase to trivalent plutonium, reextracting from the solvent phase the trivalent plutonium, ruthenium, and some fission products with an aqueous solution containing a salting out agent, introducing ozone into the aqueous acid solution to oxidize plutonium to the hexavalent state and ruthenium to ruthenium tetraoxide, and volatizing off the ruthenium tetraoxide.

Pyrochemical recovery of plutonium from calcium fluoride reduction slag

DOEpatents

Christensen, D.C.

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

Johnston Atoll Plutonium Contaminated Soil Cleanup Project. 5th quarterly report, 1 August 94 to 31 October 1994. Technical report, 1 August-31 October 1994

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

Pyrochlore-rich titanate ceramics for the immobilization of plutonium: redox effects on phase equilibria in cerium- and thorium- substituted analogs

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

Ryerson, F J; Ebbinghaus, B

2000-05-25

Three compositions representing plutonium-free analogs of a proposed Ca-Ti-Gd-Hf-U-PU oxide ceramic for the immobilization of plutonium were equilibrated at 1 atm, 1350 C over a range of oxygen fugacities between air and that equivalent to the iron-wuestite buffer. The cerium analog replaces Pu on a mole-per-mole basic with Ce; the thorium analog replaces Pu with Th. A third material has 10 wt% Al{sub 2}O{sub 3} added to the cerium analog to encourage the formation of a Hf-analog of, CaHfTi{sub 2}O{sub 7}, zirconolite, which is referred to as hafnolite. The predominant phase produced in each formulation under all conditions is pyrochlore,more » A{sub 2}T{sub 2}O{sub 7}, where the T site is filled by Ti, and Ca, the lanthanides, Hf, U and Pu are accommodated on the A-site. Other lanthanide and uranium-bearing phases encountered include brannerite (UTi{sub 2}O{sub 6}), hafnolite (CaHfTi{sub 2}O{sub 7}), perovskite (CaTiO{sub 3}) and a calcium-lanthanide aluminotitanate with nominal stoichiometry (Ca,Ln)Ti{sub 2}Al{sub 9}O{sub 19}, where Ln is a lanthanide. The phase compositions show progressive shifts with decreasing oxygen fugacity. All of the phases observed have previously been identified in titanate-based high-level radioactive waste ceramics and demonstrate the flexibility of these ceramics to variations in processing parameters. The main variation is an increase in the uranium concentrations of pyrochlore and brannerite which must be accommodated by variations in modal abundance. Pyrochlore compositions are consistent with existing spectroscopic data suggesting that uranium is predominantly pentavalent in samples synthesized in air. A simple model based on ideal stoichiometry suggests the U{sup +4}/{Sigma}U varies linearly with log fO{sub 2} and that all of the uranium is quadravalent at the iron-wuestite buffer.« less

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

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

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

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

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

PubMed Central

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

2010-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2017-01-01

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

Natural radionuclide and plutonium content in Black Sea bottom sediments

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

Strezov, A.; Stoilova, T.; Yordanova, I.

1996-01-01

The content of uranium, thorium, radium, lead, polonium, and plutonium in bottom sediments and algae from two locations at the Bulgarian Black Sea coast have been determined. Some parent:progeny ratios for evaluation of the geochemical behavior of the nuclides have been estimated as well. The extractable and total uranium and thorium are determined by two separate radiochemical procedures to differentiate the more soluble chemical forms of the elements and to estimate the potential hazard for the biosphere and for humans. No distinct seasonal variation as well as no significant change in total and extractable uranium (also for {sup 226}Ra) contentmore » is observed. The same is valid for extractable thorium while the total thorium content in the first two seasons is slightly higher. Our data show that {sup 210}Po content is accumulated more in the sediments than {sup 210}Pb, and the evaluated disequilibria suggest that the two radionuclides belong to more recent sediment layers deposited in the slime samples compared to the silt ones for the different seasons. The obtained values for plutonium are in the lower limits of the data cited in literature, which is quite clear as there are no plutonium discharge facilities at the Bulgarian Black Sea coast. The obtained values for the activity ratio {sup 238}Pu: {sup 239+240}Pu are higher for Bjala sediments compared to those of Kaliakra. The ratio values are out of the variation range for the global contamination with weapon tests fallout plutonium which is probably due to Chernobyl accident contribution. The dependence of natural radionuclide content on the sediment type as well as the variation of nuclide accumulation for two types of algae in two sampling locations for five consecutive seasons is evaluated. No serious contamination with natural radionuclides in the algae is observed. 38 refs., 6 figs., 7 tabs.« less

Air Monitoring Network at Tonopah Test Range: Network Description, Capabilities, and Analytical Results

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

Hartwell, William T.; Daniels, Jeffrey; Nikolich, George

2012-01-01

During the period April to June 2008, at the behest of the Department of Energy (DOE), National Nuclear Security Administration, Nevada Site Office (NNSA/NSO); the Desert Research Institute (DRI) constructed and deployed two portable environmental monitoring stations at the Tonopah Test Range (TTR) as part of the Environmental Restoration Project Soils Activity. DRI has operated these stations since that time. A third station was deployed in the period May to September 2011. The TTR is located within the northwest corner of the Nevada Test and Training Range (NTTR), and covers an area of approximately 725.20 km2 (280 mi2). The primarymore » objective of the monitoring stations is to evaluate whether and under what conditions there is wind transport of radiological contaminants from Soils Corrective Action Units (CAUs) associated with Operation Roller Coaster on TTR. Operation Roller Coaster was a series of tests, conducted in 1963, designed to examine the stability and dispersal of plutonium in storage and transportation accidents. These tests did not result in any nuclear explosive yield. However, the tests did result in the dispersal of plutonium and contamination of surface soils in the surrounding area.« less

Methodology using a portable X-ray fluorescence device for on-site and rapid evaluation of heavy-atom contamination in wounds: a model study for application to plutonium contamination.

PubMed

Yoshii, Hiroshi; Yanagihara, Kouta; Imaseki, Hitoshi; Hamano, Tsuyoshi; Yamanishi, Hirokuni; Inagaki, Masayo; Sakai, Yasuhiro; Sugiura, Nobuyuki; Kurihara, Osamu; Sakai, Kazuo

2014-01-01

Workers decommissioning the Fukushima-Daiichi nuclear power plant damaged from the Great East Japan Earthquake and resulting tsunami are at risk of injury with possible contamination from radioactive heavy atoms including actinides, such as plutonium. We propose a new methodology for on-site and rapid evaluation of heavy-atom contamination in wounds using a portable X-ray fluorescence (XRF) device. In the present study, stable lead was used as the model contaminant substitute for radioactive heavy atoms. First, the wound model was developed by placing a liquid blood phantom on an epoxy resin wound phantom contaminated with lead. Next, the correlation between the concentration of contaminant and the XRF peak intensity was formulated considering the thickness of blood exiting the wound. Methods to determine the minimum detection limit (MDL) of contaminants at any maximal equivalent dose to the wound by XRF measurement were also established. For example, in this system, at a maximal equivalent dose of 16.5 mSv to the wound and blood thickness of 0.5 mm, the MDL value for lead was 1.2 ppm (3.1 nmol). The radioactivity of 239Pu corresponding to 3.1 nmol is 1.7 kBq, which is lower than the radioactivity of 239Pu contaminating puncture wounds in previous severe accidents. In conclusion, the established methodology could be beneficial for future development of a method to evaluate plutonium contamination in wounds. Highlights: Methodology for evaluation of heavy-atom contamination in a wound was established. A portable X-ray fluorescence device enables on-site, rapid and direct evaluation. This method is expected to be used for evaluation of plutonium contamination in wounds.

PLUTONIUM-ZIRCONIUM ALLOYS

DOEpatents

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

1960-08-30

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

Plutonium recovery from spent reactor fuel by uranium displacement

DOEpatents

Ackerman, J.P.

1992-03-17

A process is described for separating uranium values and transuranic values from fission products containing rare earth values when the values are contained together in a molten chloride salt electrolyte. A molten chloride salt electrolyte with a first ratio of plutonium chloride to uranium chloride is contacted with both a solid cathode and an anode having values of uranium and fission products including plutonium. A voltage is applied across the anode and cathode electrolytically to transfer uranium and plutonium from the anode to the electrolyte while uranium values in the electrolyte electrolytically deposit as uranium metal on the solid cathode in an amount equal to the uranium and plutonium transferred from the anode causing the electrolyte to have a second ratio of plutonium chloride to uranium chloride. Then the solid cathode with the uranium metal deposited thereon is removed and molten cadmium having uranium dissolved therein is brought into contact with the electrolyte resulting in chemical transfer of plutonium values from the electrolyte to the molten cadmium and transfer of uranium values from the molten cadmium to the electrolyte until the first ratio of plutonium chloride to uranium chloride is reestablished.

METHOD OF RECOVERING TRANSURANIC ELEMENTS OF AN ATOMIC NUMBER BELOW 95

DOEpatents

Seaborg, G.T.; James, R.A.

1959-12-15

The concentration of neptanium or plutonium by two carrier precipitation steps with identical carriers but using (after dissolution of the first carrier in nitric acid) a reduced quantity of carrier for the second precipitation is discussed. Carriers suitable are uranium(IV) hypophosphate, uranium(IV) pyrophosphate, uranium(IV) oxalate, thorium oxalate, thorium citrate, thorium tartrate, thorium sulfide, and uranium(IV) sulfide.

Validation of Electrochemically Modulated Separations Performed On-Line with MC-ICP-MS for Uranium and Plutonium Isotopic Analyses

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

Liezers, Martin; Olsen, Khris B.; Mitroshkov, Alexandre V.

2010-08-11

The most time consuming process in uranium or plutonium isotopic analyses is performing the requisite chromatographic separation of the actinides. Filament preparation for thermal ionization (TIMS) adds further delays, but is generally accepted due to the unmatched performance in trace isotopic analyses. Advances in Multi-Collector Inductively Coupled Plasma Mass Spectrometry (MC-ICP-MS) are beginning to rival the performance of TIMS. Methods, such as Electrochemically Modulated Separations (EMS) can efficiently pre-concentrate U or Pu quite selectively from small solution volumes in a matrix of 0.5 M nitric acid. When performed in-line with ICP-MS, the rapid analyte release from the electrode is fast,more » and large transient analyte signal enhancements of >100 fold can be achieved as compared to more conventional continuous nebulization of the original starting solution. This makes the approach ideal for very low level isotope ratio measurements. In this paper, some aspects of EMS performance are described. These include low level Pu isotope ratio behavior versus concentration by MC-ICP-MS and uranium rejection characteristics that are also important for reliable low level Pu isotope ratio determinations.« less

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

PubMed

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

2014-11-01

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

BASIC PEROXIDE PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINANTS

DOEpatents

Seaborg, G.T.; Perlman, I.

1959-02-10

A process is described for the separation from each other of uranyl values, tetravalent plutonium values and fission products contained in an aqueous acidic solution. First the pH of the solution is adjusted to between 2.5 and 8 and hydrogen peroxide is then added to the solution causing precipitation of uranium peroxide which carries any plutonium values present, while the fission products remain in solution. Separation of the uranium and plutonium values is then effected by dissolving the peroxide precipitate in an acidic solution and incorporating a second carrier precipitate, selective for plutonium. The plutonium values are thus carried from the solution while the uranium remains flissolved. The second carrier precipitate may be selected from among the group consisting of rare earth fluorides, and oxalates, zirconium phosphate, and bismuth lihosphate.

PREPARATION OF PLUTONIUM

DOEpatents

Kolodney, M.

1959-07-01

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

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

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

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

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

EPA Pesticide Factsheets

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

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

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

NONE

1996-05-01

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

Plutonium controversy

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

Richmond, C.R.

1980-01-01

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

Recent advances in f-element separations based on a new method for the production of pentavalent americium in acidic solution

DOE PAGES

Mincher, Bruce J.; Schmitt, Nicholas C.; Schuetz, Brian K.; ...

2015-03-11

The peroxydisulfate anion has long been used for the preparation of hexavalent americium (Am VI) from the normally stable Am III valence state in mildly acidic solutions. However, there has been no satisfactory means to directly prepare the pentavalent state (Am V) in that medium. Some early literature reports indicated that the peroxydisulfate oxidation was incomplete, and silver ion catalysis in conjunction with peroxydisulfate became accepted as the means to ensure quantitative generation of Am VI. Incomplete oxidation would be expected to leave residual Am III, or to produce Am V in treated solutions. However, until recently, the use ofmore » peroxydisulfate as an Am V reagent has not been reported. Here, parameters influencing the oxidation were investigated, including peroxydisulfate and acid concentration, temperature, duration of oxidative treatment, and the presence of higher concentrations of other redox active metals such as plutonium. Using optimized conditions determined here, quantitative Am V was prepared in an acidic solution and the UV/Vis extinction coefficients of the Am V 513 nm peak were measured over a range of nitric acid concentrations. Furthermore, the utility of Am V for separations from the lanthanides and curium by solvent extraction, organic column chromatography and inorganic ion exchangers was also investigated.« less

Radionuclide concentrations in honey bees from Area G at TA-54 during 1997. Progress report

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

Haarmann, T.K.; Fresquez, P.R.

Honey bees were collected from two colonies located at Los Alamos National Laboratory`s Area G, Technical Area 54, and from one control (background) colony located near Jamez Springs, NM. Samples were analyzed for the following: cesium ({sup 137}Cs), americium ({sup 241}Am), plutonium ({sup 238}Pu and {sup 239,240}Pu), tritium ({sup 3}H), total uranium, and gross gamma activity. Area G sample results from both colonies were higher than the upper (95%) level background concentration for {sup 238}Pu and {sup 3}H.

Johnston Atoll Plutonium Cleanup Project. Contract bridge report. Technical report, 1 June-5 August 1993

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

Hellier, C.L.; Doane, R.W.

1995-04-01

This report continues the documentation of the operation of TMA/Eberline`s Segmented Gate System technology for removing mixed plutonium and americium contamination at DNA`s Johnston Atoll site. Contaminated feed is conveyed under arrays of radiation detectors coupled with sophisticated computer software developed by Eberline Instrument Corporation. Segmented gates (chutes) on pneumatically-driven pistons move forward when contamination is detected to remove only the contaminated portion from the main flow of feed material. Only about one pint of contaminant is removed during each diversion event. At the JA site, a 98% volume reduction has been achieved, with the remediated soil cleaned to DNA`smore » criteria for release for unrestricted use of 500 Bq/kg total transuranic alpha contamination and no hot particles of greater than 5000 Becquerrels. The low level waste concentrate is expected to be packaged for shipment to an approved defense waste disposal site.« less

1990 Environmental monitoring report, Tonopah Test Range, Tonopah, Nevada

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

Hwang, A.; Phelan, J.; Wolff, T.

1991-05-01

There is no routine radioactive emission from Sandia National Laboratories, Tonopah Test Range (SNL, TTR). However, based on the types of test activities such as air drops, gun firings, ground- launched rockets, air-launched rockets, and other explosive tests, possibilities exist that small amounts of depleted uranium (DU) (as part of weapon components) may be released to the air or to the ground because of unusual circumstances (failures) during testing. Four major monitoring programs were used in 1990 to assess radiological impact on the public. The EPA Air Surveillance Network (ASN) found that the only gamma ({gamma}) emitting radionuclide on themore » prefilters was beryllium-7 ({sup 7}Be), a naturally-occurring spallation product formed by the interaction of cosmic radiation with atmospheric oxygen and nitrogen. The weighted average results were consistent with the area background concentrations. The EPA Thermoluminescent Dosimetry (TLD) Network and Pressurized Ion Chamber (PIC) reported normal results. In the EPA Long-Term Hydrological Monitoring Program (LTHMP), analytical results for tritium ({sup 3}H) in well water were reported and were well below DOE-derived concentration guides (DCGs). In the Reynolds Electrical and Engineering Company (REECo) Drinking Water Sampling Program, analytical results for {sup 3}H, gross alpha ({alpha}), beta ({beta}), and {gamma} scan, strontium-90 ({sup 90}Sr) and plutonium-239 ({sup 239}Pu) were within the EPA's primary drinking water standards. 29 refs., 5 figs., 15 tabs.« less

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

Herring, G. M.; Vaughan, Janet; Williamson, Margaret

Characteristics of bone surfaces are discussed in relation to the uptake of bone-seeking isotopes. The alkaline earths are concentrated behind the osteoid border of active surfaces. Yttrium, americium, and plutonium are concentrated on quiescent and resorbing surfaces; traces only occur in and beneath the osteoid border. In view of evidence of mucoproteins at sites where the latter elemerts are found in concentration, a separation of the mucoproteins in cortical bone was undertaken. Mucosubstances have been isolated which give the same reaction with certain reagents as the bone surfaces in question. One of these, a sialoprotein, might be expected, in viewmore » of its acidic nature, to be capable of metal binding.« less

PREPARATION OF PLUTONIUM TRIFLUORIDE

DOEpatents

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

1961-07-11

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

MCNP Parametric Studies of Plutonium Metal and Various Interstitial Moderating Materials

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

Glazener, Natasha; Kamm, Ryan James

2017-03-31

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

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

PubMed

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

2014-11-01

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

TYBO/BENHAM: Model Analysis of Groundwater Flow and Radionuclide Migration from Underground Nuclear Tests in Southwestern Pahute Mesa, Nevada

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

Andrew Wolfsberg; Lee Glascoe; Guoping Lu

Recent field studies have led to the discovery of trace quantities of plutonium originating from the BENHAM underground nuclear test in two groundwater observation wells on Pahute Mesa at the Nevada Test Site. These observation wells are located 1.3 km from the BENHAM underground nuclear test and approximately 300 m from the TYBO underground nuclear test. In addition to plutonium, several other conservative (e.g. tritium) and reactive (e.g. cesium) radionuclides were found in both observation wells. The highest radionuclide concentrations were found in a well sampling a welded tuff aquifer more than 500m above the BENHAM emplacement depth. These measurementsmore » have prompted additional investigations to ascertain the mechanisms, processes, and conditions affecting subsurface radionuclide transport in Pahute Mesa groundwater. This report describes an integrated modeling approach used to simulate groundwater flow, radionuclide source release, and radionuclide transport near the BENHAM and TYBO underground nuclear tests on Pahute Mesa. The components of the model include a flow model at a scale large enough to encompass many wells for calibration, a source-term model capable of predicting radionuclide releases to aquifers following complex processes associated with nonisothermal flow and glass dissolution, and site-scale transport models that consider migration of solutes and colloids in fractured volcanic rock. Although multiple modeling components contribute to the methodology presented in this report, they are coupled and yield results consistent with laboratory and field observations. Additionally, sensitivity analyses are conducted to provide insight into the relative importance of uncertainty ranges in the transport parameters.« less

SEPARATION OF PLUTONIUM IONS FROM SOLUTION BY ADSORPTION ON ZIRCONIUM PYROPHOSPHATE

DOEpatents

Stoughton, R.W.

1961-01-31

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

Plutonium and americium separation from salts

DOEpatents

Hagan, Paul G.; Miner, Frend J.

1976-01-01

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

Plutonium storage criteria

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

Chung, D.; Ascanio, X.

1996-05-01

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

PROCESS OF PRODUCING SHAPED PLUTONIUM

DOEpatents

Anicetti, R.J.

1959-08-11

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

WET METHOD OF PREPARING PLUTONIUM TRIBROMIDE

DOEpatents

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

1958-11-11

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

Spectrophotometers for plutonium monitoring in HB-line

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

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

2016-02-12

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

Plutonium radiation surrogate

DOEpatents

Frank, Michael I [Dublin, CA

2010-02-02

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

Independent Verification Survey of the Clean Coral Storage Pile at the Johnston Atoll Plutonium-Contaminated Soil Remediation Project

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

Wilson-Nichols, M.J.

2000-12-07

The Oak Ridge National Laboratory (ORNL) Environmental Technology Section conducted an independent verification (IV) survey of the clean storage pile at the Johnston Atoll Plutonium Contaminated Soil Remediation Project (JAPCSRP) from January 18-25, 1999. The goal of the JAPCSRP is to restore a 24-acre area that was contaminated with plutonium oxide particles during nuclear testing in the 1960s. The selected remedy was a soil sorting operation that combined radiological measurements and mining processes to identify and sequester plutonium-contaminated soil. The soil sorter operated from about 1990 to 1998. The remaining clean soil is stored on-site for planned beneficial use onmore » Johnston Island. The clean storage pile currently consists of approximately 120,000 m{sup 3} of coral. ORNL conducted the survey according to a Sampling and Analysis Plan, which proposed to provide an IV of the clean pile by collecting a minimum number (99) of samples. The goal was to ascertain with 95% confidence whether 97% of the processed soil is less than or equal to the accepted guideline (500-Bq/kg or 13.5-pCi/g) total transuranic (TRU) activity. In previous IV tasks, ORNL has (1) evaluated and tested the soil sorter system software and hardware and (2) evaluated the quality control (QC) program used at the soil sorter plant. The IV has found that the soil sorter decontamination was effective and significantly reduced plutonium contamination in the soil processed at the JA site. The Field Command Defense Threat Reduction Agency currently plans to re-use soil from the clean pile as a cover to remaining contamination in portions of the radiological control area. Therefore, ORNL was requested to provide an IV. The survey team collected samples from 103 random locations within the top 4 ft of the clean storage pile. The samples were analyzed in the on-site radioanalytical counting laboratory with an American Nuclear Systems (ANS) field instrument used for the detection of low-energy radiation. Nine results exceeded the JA soil screening guideline for distributed contamination of 13.5 pCi/g for total TRUs, ranging from 13.7 to 125.9 pCi/g. Because of these results, the goal of showing with 95% confidence that 97% of the processed soil is less than or equal to 13.5 pCi/g-TRU activity cannot be met. The value of 13.5 pCi/g represents the 88th percentile rather than the 95th percentile in a nonparametric one-sided upper 90% confidence limit. Therefore, at the 95% confidence level, 88% of the clean pile is projected to be below the 13.5-pCi/g goal. The Multi-Agency Radiation Survey and Site Investigation Manual recommends use of a nonparametric statistical ''Sign Test'' to demonstrate compliance with release criteria for TRU. Although this survey was not designed to use the sign test, the data herein would demonstrate that the median (50%) of the clean storage pile is below the l3.5-pCi/g derived concentration guideline level. In other words, with the caveat that additional investigation of elevated concentrations was not performed, the data pass the sign test at the 13.5-pCi/g level. Additionally, the lateral extent of the pile was gridded, and 10% of the grid blocks was scanned with field instruments for the detection of low-energy radiation coupled to ratemeter/scalers to screen for the presence of hot particles. No hot particles were detected in the top 1 cm of the grid blocks surveyed.« less

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

DOEpatents

Thomas, J.R.

1958-08-26

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

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

NASA Astrophysics Data System (ADS)

Blandinskiy, V. Yu.

2014-12-01

This paper presents the results of a numerical investigation into burnup and breeding of nuclides in metallic fuel consisting of a mixture of plutonium and depleted uranium in a fast reactor with sodium coolant. The feasibility of using plutonium contained in spent nuclear fuel from domestic thermal reactors and weapons-grade plutonium is discussed. It is shown that the largest production of secondary fuel and the least change in the reactivity over the reactor lifetime can be achieved when employing plutonium contained in spent nuclear fuel from a reactor of the RBMK-1000 type.

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

DOEpatents

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

1959-02-01

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

ION EXCHANGE ADSORPTION PROCESS FOR PLUTONIUM SEPARATION

DOEpatents

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

1961-07-11

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

Concentrations of selected radionuclides and their spatial distribution in marine sediments from the northwestern Gulf, Kuwait.

PubMed

Uddin, Saif; Behbehani, Montaha

2018-02-01

This study focuses on creating a baseline for 40 K, 210 Pb, 137 Cs, 90 Sr, 226 Ra, 228 Ra, 238 U, 235 U, 234 U, 239+240 Pu and 238 Pu in marine sediments in the northwestern Gulf. The respective measured concentration ranges were 386-489, 32.3-48.8, 1.5-2.9, 4.53-5.42, 18.3-23.1, 18.8-23.0, 22.3-30.5, 0.99-1.33, 25.6-34.8, 0.30-0.93, and 0.0008-0.00018Bqkg -1 . The levels of these radionuclides are generally comparable to values reported for other marine waters in the northern hemisphere. The 137 Cs activity in the Gulf sediments offshore Kuwait is an order of magnitude lower compared to sediments from northeastern Iran. Other than that finding, no hot spots were observed in sediments adjacent to power and desalination plants, oil and gas industrial activities or wastewater treatment facilities. These data will serve as a baseline to gauge possible future inputs of radionuclides in the northern Gulf. The calculated average ratio of 235 U/ 238 U activity in the area is in agreement with the reported figure of the natural uranium ratio, suggesting the absence of depleted uranium (DU) at all the stations. The low concentration of 239+240 Pu suggests that there is no significant source of plutonium except that from atmospheric fallout from weapon testing and possible dry deposition via long-range dust transport. Copyright © 2017 Elsevier Ltd. All rights reserved.

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

DOE PAGES

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

2017-01-18

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

JOWOG 22/2 - Actinide Chemical Technology (July 9-13, 2012)

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

Jackson, Jay M.; Lopez, Jacquelyn C.; Wayne, David M.

2012-07-05

The Plutonium Science and Manufacturing Directorate provides world-class, safe, secure, and reliable special nuclear material research, process development, technology demonstration, and manufacturing capabilities that support the nation's defense, energy, and environmental needs. We safely and efficiently process plutonium, uranium, and other actinide materials to meet national program requirements, while expanding the scientific and engineering basis of nuclear weapons-based manufacturing, and while producing the next generation of nuclear engineers and scientists. Actinide Process Chemistry (NCO-2) safely and efficiently processes plutonium and other actinide compounds to meet the nation's nuclear defense program needs. All of our processing activities are done in amore » world class and highly regulated nuclear facility. NCO-2's plutonium processing activities consist of direct oxide reduction, metal chlorination, americium extraction, and electrorefining. In addition, NCO-2 uses hydrochloric and nitric acid dissolutions for both plutonium processing and reduction of hazardous components in the waste streams. Finally, NCO-2 is a key team member in the processing of plutonium oxide from disassembled pits and the subsequent stabilization of plutonium oxide for safe and stable long-term storage.« less

PLUTONIUM-CERIUM ALLOY

DOEpatents

Coffinberry, A.S.

1959-01-01

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

Plutonium recovery from organic materials

DOEpatents

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

1973-12-11

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

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

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

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

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

DOEpatents

Steindler, M.J.

1962-07-24

A process was developed for separating uranium hexafluoride from plutonium hexafluoride by the selective reduction of the plutonium hexafluoride to the tetrafluoride with sulfur tetrafluoride at 50 to 120 deg C, cooling the mixture to --60 to -100 deg C, and volatilizing nonreacted sulfur tetrafluoride and sulfur hexafluoride formed at that temperature. The uranium hexafluoride is volatilized at room temperature away from the solid plutonium tetrafluoride. (AEC)

THE CHEMICAL ANALYSIS OF TERNARY ALLOYS OF PLUTONIUM WITH MOLYBDENUM AND URANIUM

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

Phillips, G.; Woodhead, J.; Jenkins, E.N.

1958-09-01

It is shown that the absorptiometric determination of molybdenum as thiocyanate may be used in the presence of plutonium. Molybdenum interferes with previously published methods for determining uranium and plutonium but conditlons have been established for its complete removal by solvent extraction of the compound with alpha -benzoin oxime. The previous methods for uranium and plutonium are satisfactory when applied to the residual aqueous phase following this solvent extraction. (auth)

PROCESS OF SEPARATING PLUTONIUM VALUES BY ELECTRODEPOSITION

DOEpatents

Whal, A.C.

1958-04-15

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

SEPARATION OF PLUTONIUM VALUES FROM URANIUM AND FISSION PRODUCT VALUES

DOEpatents

Maddock, A.G.; Booth, A.H.

1960-09-13

Separation of plutonium present in small amounts from neutron irradiated uranium by making use of the phenomenon of chemisorption is described. Plutonium in the tetravalent state is chemically absorbed on a fluoride in solid form. The steps for the separation comprise dissolving the irradiated uranium in nitric acid, oxidizing the plutonium in the resulting solution to the hexavalent state, adding to the solution a soluble calcium salt which by the common ion effect inhibits dissolution of the fluoride by the solution, passing the solution through a bed or column of subdivided calcium fluoride which has been sintered to about 8OO deg C to remove the chemisorbable fission products, reducing the plutonium in the solution thus obtained to the tetravalent state, and again passing the solution through a similar bed or column of calcium fluoride to selectively absorb the plutonium, which may then be recovered by treating the calcium fluoride with a solution of ammonium oxalate.

Using Biomolecules to Separate Plutonium

NASA Astrophysics Data System (ADS)

Gogolski, Jarrod

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

PROCESS FOR PRODUCTION OF PLUTONIUM FROM ITS OXIDES

DOEpatents

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

1959-10-13

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

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

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

Jardine, L J; Borisov, G B

2004-07-21

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

Colloids from the aqueous corrosion of uranium nuclear fuel

NASA Astrophysics Data System (ADS)

Kaminski, M. D.; Dimitrijevic, N. M.; Mertz, C. J.; Goldberg, M. M.

2005-12-01

Colloids may enhance the subsurface transport of radionuclides and potentially compromise the long-term safe operation of the proposed radioactive waste repository at Yucca Mountain. Little data is available on colloid formation for the many different waste forms expected to be buried in the repository. This work expands the sparse database on colloids formed during the corrosion of metallic uranium nuclear fuel. We characterized spherical UO 2 and nickel-rich montmorilonite smectite-clay colloids formed during the corrosion of uranium metal fuel under bathtub conditions at 90 °C. Iron and chromium oxides and calcium carbonate colloids were present but were a minor population. The estimated upper concentration of the UO 2 and clays was 4 × 10 11 and 7 × 10 11-3 × 10 12 particles/L, respectively. However, oxygen eventually oxidized the UO 2 colloids, forming long filaments of weeksite K 2(UO 2) 2Si 6O 15 · 4H 2O that settled from solution, reducing the UO 2 colloid population and leaving predominantly clay colloids. The smectite colloids were not affected by oxygen. Plutonium was not directly observed within the UO 2 colloids but partitioned completely to the colloid size fraction. The plutonium concentration in the colloidal fraction was slightly higher than the value used in the viability assessment model, and does not change in concentration with exposure to oxygen. This paper provides conclusive evidence for single-phase radioactive colloids composed of UO 2. However, its impact on repository safety is probably small since oxygen and silica availability will oxidize and effectively precipitate the UO 2 colloids from concentrated solutions.

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

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

NONE

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

SEPARATION OF PLUTONIUM FROM URANIUM

DOEpatents

Feder, H.M.; Nuttall, R.L.

1959-12-15

A process is described for extracting plutonium from powdered neutron- irradiated urarium metal by contacting the latter, while maintaining it in the solid form, with molten magnesium which takes up the plutonium and separating the molten magnesium from the solid uranium.

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

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

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

SEPARATION OF URANIUM, PLUTONIUM, AND FISSION PRODUCTS

DOEpatents

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.

Volatile Impurities in the Plutonium Immobilization Ceramic Wasteform

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

Cozzi, A.D.

1999-10-15

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

PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINATING ELEMENTS

DOEpatents

Sutton, J.B.

1958-02-18

This patent relates to an improved method for the decontamination of plutonium. The process consists broadly in an improvement in a method for recovering plutonium from radioactive uranium fission products in aqueous solutions by decontamination steps including byproduct carrier precipitation comprising the step of introducing a preformed aqueous slurry of a hydroxide of a metal of group IV B into any aqueous acidic solution which contains the plutonium in the hexavalent state, radioactive uranium fission products contaminant and a by-product carrier precipitate and separating the metal hydroxide and by-product precipitate from the solution. The process of this invention is especially useful in the separation of plutonium from radioactive zirconium and columbium fission products.

The application of Caesium-137 and Plutonium-239+240 measurements to investigate floodplain deposition in a semi-arid, low-fallout environment

NASA Astrophysics Data System (ADS)

Amos, K. J.; Croke, J. C.; Timmers, H.; Owens, P. N.

2009-04-01

Floodplains comprise geomorphologically important sources and sinks for sediments and associated pollutants, yet the sedimentology of large dryland floodplains is not well understood. Processes occurring on such floodplains are often difficult to observe, and techniques used to investigate smaller perennial floodplains are often not practical in these environments. This study assesses the utility of Cs-137 inventory and depth-profile techniques for determining relative amounts of floodplain sedimentation in the Fitzroy River, north-eastern Australia; a 143 000 km2 semi-arid river system. Caesium-137 inventories were calculated for floodplain and reference location bulk soil cores collected from four sites. Depth profiles of Cs-137 concentration from each floodplain site and a reference location were recorded. The areal density of Cs-137 at reference locations ranged from 13-978 Bq m-2 (0-1367 Bq m-2 at the 95% confidence interval), and the mean value ± 2(standard error of the mean) was 436±264 Bq m-2, similar to published data from other southern hemisphere locations. Floodplain inventories ranged from 68-1142 Bq m-2 (0-1692 Bq m-2 at the 95% confidence interval), essentially falling within the range of reference inventory values, thus preventing calculation of erosion or deposition. Depth-profiles of Cs-137 concentration indicate erosion at one site and over 66 cm of deposition at another since 1954. Analysis of 239+240Pu concentrations in a depositional core substantiated the interpretation made from Cs-137 data, and depict a more tightly constrained peak in concentration. Average annual deposition rates range from 0-15 mm. The similarity between floodplain and reference bulk inventories does not necessarily indicate a lack of erosion or deposition, due to low Cs-137 fallout in the region and associated high measurement uncertainties, and a likely influence of gully and bank eroded sediments with no or limited adsorbed Cs-137. In this low-fallout environment, detailed depth-profile data are necessary for investigating sedimentation using Cs-137.

Progress on plutonium stabilization

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

Hurt, D.

1996-05-01

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

NON-CORROSIVE PLUTONIUM FUEL SYSTEMS

DOEpatents

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

1962-10-23

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

Development of a Si-PM based alpha camera for plutonium detection in nuclear fuel facilities

NASA Astrophysics Data System (ADS)

Morishita, Yuki; Yamamoto, Seiichi; Izaki, Kenji; Kaneko, Junichi H.; Toi, Kohei; Tsubota, Youichi

2014-05-01

Alpha particles are monitored for detecting nuclear fuel material (i.e., plutonium and uranium) at nuclear fuel facilities. Currently, for monitoring the airborne contamination of nuclear fuel, only energy information measured by Si-semiconductor detectors is used to distinguish nuclear fuel material from radon daughters. In some cases, however, such distinguishing is difficult when the radon concentration is high. In addition, a Si-semiconductor detector is generally sensitive to noise. In this study, we developed a new alpha-particle imaging system by combining a Si-PM array, which is insensitive to noise, with a Ce-doped Gd3Al2Ga3O12(GAGG) scintillator, and evaluated our developed system's fundamental performance. The scintillator was 0.1-mm thick, and the light guide was 3.0 mm thick. An 241Am source was used for all the measurements. We evaluated the spatial resolution by taking an image of a resolution chart. A 1.6 lp/mm slit was clearly resolved, and the spatial resolution was estimated to be less than 0.6-mm FWHM. The energy resolution was 13% FWHM. A slight distortion was observed in the image, and the uniformity near its center was within ±24%. We conclude that our developed alpha-particle imaging system is promising for plutonium detection at nuclear fuel facilities.

METHOD OF REDUCING PLUTONIUM COMPOUNDS

DOEpatents

Johns, I.B.

1958-06-01

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

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

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

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

Project 57 Air Monitoring Report: October 1, 2013, through December 31, 2014

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

Mizell, Steve A.; Nikolich, George; McCurdy, Greg

On April 24, 1957, the Atomic Energy Commission (AEC, now the Department of Energy [DOE]) conducted the Project 57 safety experiment in western Emigrant Valley north east of the Nevada National Security Site (NNSS, formerly the Nevada Test Site) on lands withdrawn by the Department of Defense (DoD) for the Nevada Test and Training Range (NTTR). The test was undertaken to develop (1) a means of estimating plutonium distribution resulting from a nonnuclear detonation; (2) biomedical evaluation techniques for use in plutonium-laden environments; (3) methods of surface decontamination; and (4) instruments and field procedures for prompt estimation of alpha contaminationmore » (Shreve, 1958). Although the test did not result in the fission of nuclear materials, it did disseminate plutonium across the land surface. Following the experiment, the AEC fenced the contaminated area and returned control of the surrounding land to the DoD. Various radiological surveys have been performed in the area and in 2007, the DOE expanded the demarked contamination area by posting signs 200 to 400 feet (60 to 120 meters) outside of the original fence. Plutonium in soil is thought to attach preferentially to smaller particles. Therefore, redistribution of soil particulates by wind (dust) is the mechanism most likely to transport plutonium beyond the boundary of the Project 57 contamination area. In 2011, DRI installed two instrumentation towers to measure radiological, meteorological, and dust conditions. The monitoring activity was implemented to determine if radionuclide contamination was detectable in samples of airborne dust and characterize meteorological and environmental parameters that influence dust transport. Collected data also permits comparison of radiological conditions at the Project 57 monitoring stations to conditions observed at Community Environmental Monitoring Program (CEMP) stations around the NTTR. Biweekly samples of airborne particulates are submitted for laboratory assessment of gross alpha and gross beta radioactivity and for determination of gamma-emitting radionuclides. Annual average gross alpha values at the Project 57 monitoring stations are in the same range as the highest two values reported for the CEMP stations surrounding the NTTR. Annual average gross beta values at the Project 57 monitoring stations are slightly higher than the lowest value reported for the CEMP stations surrounding the NTTR. Gamma spectroscopy analyses on samples collected from the Project 57 stations identified only naturally occurring radionuclides. No manmade radionuclides were detected. Thermoluminescent dosimeters (TLDs) indicated that the average annual radioactivity dose at the monitoring stations is higher than the dose determined at surrounding CEMP stations but approximately half of the estimated national average dose received by the general public as a result of exposure to natural sources. The TLDs at the Project 57 monitoring stations are exposed to both natural sources (terrestrial and cosmic) and radioactive releases from the Project 57 contamination area. These comparisons show that the gross alpha, gross beta, and gamma spectroscopy levels at the Project 57 monitoring stations are similar to levels observed at the CEMP stations but that the average annual dose rate is higher than at the CEMP stations. Winds in excess of approximately 15 mph begin to generate dust movement by saltation (migration of sand at the ground surface) or direct suspension in the air. Saltated sand, PM10 (inhalable) dust, and PM2.5 (fine particulate dust) exhibit an approximately exponential increase with increasing wind speed. The greatest concentrations of dust occur for winds exceeding 20 mph. During the reporting period, winds in excess of 20 mph occurred approximately 1.6 percent of the time. Preliminary assessment of individual wind events suggests that dust generation is highly variable likely because of the influence of other meteorological and environmental parameters. Although winds sufficient to generate significant amounts of dust occur at the Project 57 site, they are infrequent and of short duration. Additionally, the potential for wind transport of dust is dependent on other parameters whose influence have not yet been assessed.« 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.

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

DOEpatents

Seaborg, G.T.

1961-08-01

A process is described for extracting tetravalent plutonium from an aqueous acid solution with methyl ethyl ketone, methyl isobutyl ketone, or acetophenone and with the extraction of either tetravalent or hexavalent plutonium into menthone. (AEC)

10 CFR 830.3 - Definitions.

Code of Federal Regulations, 2010 CFR

2010-01-01

.... Critical assembly means special nuclear devices designed and used to sustain nuclear reactions, which may... reaction becomes self-sustaining. Design features means the design features of a nuclear facility specified... reaction (e.g., uranium-233, uranium-235, plutonium-238, plutonium-239, plutonium-241, neptunium-237...

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

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

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

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

DOEpatents

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

1959-07-01

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

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

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

Marsh, S.F.; Spall, W.D.; Abernathey, R.M.

1976-11-01

Relationships are provided to compute the decreasing plutonium content and changing isotopic distribution of plutonium materials for the radioactive decay of /sup 238/Pu, /sup 239/Pu, /sup 240/Pu and /sup 242/Pu to long-lived uranium daughters and of /sup 241/Pu to /sup 241/Am. This computation is important to the use of plutonium reference materials to calibrate destructive and nondestructive methods for assay and isotopic measurements, as well as to accountability inventory calculations.

SOLVENT EXTRACTION PROCESS FOR PLUTONIUM

DOEpatents

Seaborg, G.T.

1959-04-14

The separation of plutonium from aqueous inorganic acid solutions by the use of a water immiscible organic extractant liquid is described. The plutonium must be in the oxidized state, and the solvents covered by the patent include nitromethane, nitroethane, nitropropane, and nitrobenzene. The use of a salting out agents such as ammonium nitrate in the case of an aqueous nitric acid solution is advantageous. After contacting the aqueous solution with the organic extractant, the resulting extract and raffinate phases are separated. The plutonium may be recovered by any suitable method.

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

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

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

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

None, None

Operations of Sandia National Laboratories, Nevada (SNL/NV) at the Tonopah Test Range (TTR) resulted in no planned point radiological releases during 1996. Other releases from SNL/NV included diffuse transuranic sources consisting of the three Clean Slate sites. Air emissions from these sources result from wind resuspension of near-surface transuranic contaminated soil particulates. The total area of contamination has been estimated to exceed 20 million square meters. Soil contamination was documented in an aerial survey program in 1977 (EG&G 1979). Surface contamination levels were generally found to be below 400 pCi/g of combined plutonium-238, plutonium-239, plutonium-240, and americium-241 (i.e., transuranic) activity.more » Hot spot areas contain up to 43,000 pCi/g of transuranic activity. Recent measurements confirm the presence of significant levels of transuranic activity in the surface soil. An annual diffuse source term of 0.39 Ci of transuranic material was calculated for the cumulative release from all three Clean Slate sites. A maximally exposed individual dose of 1.1 mrem/yr at the TTR airport area was estimated based on the 1996 diffuse source release amounts and site-specific meteorological data. A population dose of 0.86 person-rem/yr was calculated for the local residents. Both dose values were attributable to inhalation of transuranic contaminated dust.« less

Twenty-four years of follow-up for a Hanford plutonium wound case.

PubMed

Carbaugh, Eugene H; Lynch, Timothy P; Antonio, Cheryl L; Medina-Del Valle, Fernando

2010-10-01

A 1985 plutonium puncture wound resulted in the initial deposition of 48 kBq of transuranic alpha activity, primarily 239+240Pu and 241Am, in a worker's right index finger. Surgical excisions in the week following reduced the long-term residual wound activity to 5.4 kBq, and 164 DTPA chelation therapy administrations over 17 mo resulted in urinary excretion of about 7 kBq. The case was published in 1988, but now 24 y of follow-up data are available. Annual bioassays have included in-vivo measurements of 241Am in the wound, skeleton, liver, lung, and axillary lymph nodes, and urinalyses for plutonium and 241Am. These measurements have shown relatively stable levels of 241Am at the wound site, with gradually increasing amounts of 241Am detected in the skeleton. Liver measurements have shown erratic detection of 241Am, and the lung measurements indicate Am but as interference from activity in the axillary lymph nodes and skeleton rather than activity in the lung. Urine excretion of Pu since termination of chelation therapy has typically ranged from 10 to 20 mBq d, with Am excretion about 10% of that for 239+240Pu. Annual routine medical exams have not identified any adverse health effects associated with the intake.

Twenty-four Years of Follow-Up for a Hanford Plutonium Wound Case

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

Carbaugh, Eugene H.; Lynch, Timothy P.; Antonio, Cheryl L.

2010-10-01

A 1985 plutonium puncture wound resulted in the initial deposition of 48 kBq of transuranic alpha activity, primarily 239Pu and 241Am, in a worker’s right index finger. Surgical excisions in the week following reduced the long-term residual wound activity to 5.4 kBq, and 164 DTPA chelation therapy administrations over a 17-month period resulted in urinary excretion of about 7 kBq. The case was published in 1988, but now 20 additional years of follow-up data are available. Annual bioassay measurements have included wound counts, skeleton counts, liver counts, lung counts, axillary lymph node counts, and urinalyses for plutonium and 241Am. Thesemore » measurements have shown relatively stable levels of 241Am at the wound site, with gradually increasing amounts of 241Am detected in the skeleton. Liver counts has shown erratic detection of 241Am, and lung counts indicate 241Am as shine from the axillary lymph nodes and skeleton. Urine excretion of 239Pu since termination of chelation therapy has typically ranged from 10 to 20 mBq d-1, with 241Am excretion being about 10% of that for 239Pu. In addition, the worker has undergone annual routine medical exams, which have not identified any adverse health effects associated with the intake.« less

Toxicity of inhaled plutonium dioxide in beagle dogs

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

Muggenburg, M.A.; Guilmette, R.A.; Mewhinney, J.A.

This study was conducted to determine the biological effects of inhaled {sup 238}PuO{sub 2} over the life spans of 144 beagle dogs. The dogs inhaled one of two sizes of monodisperse aerosols of {sup 238}PuO{sub 2} to achieve graded levels of initial lung burden (ILB). The aerosols also contained {sup 169}Yb to provide a {gamma}-ray-emitting label for the {sup 238}Pu inhaled by each dog. Excreta were collected periodically over each dog`s life span to estimate plutonium excretion; at death, the tissues were analyzed radiochemically for plutonium activity. The tissue content and the amount of plutonium excreted were used to estimatemore » the ILB. These data for each dog were used in a dosimetry model to estimate the ILB. These data for each dog were used in a dosimetry model to estimate tissue doses. The lung, skeleton and liver received the highest {alpha}-particle doses, ranging from 0.16-68 Gy for the liver. At death, all dogs were necropsied, and all organs and lesions were sampled and examined by histopathology. Findings of non-neoplastic changes included neutropenia and lymphopenia that developed in a dose-related fashion soon after inhalation exposure. These effects persisted for up to 5 years in some animals, but no other health effects could be related to the blood changes observed. Radiation pneumonitis was observed among the dogs with the highest ILBs. Deaths from radiation pneumonitis occurred from 1.5 to 5.4 years after exposure. Tumors of the lung, skeleton and liver occurred beginning at about 3 years after exposure. These findings in dogs suggest that similar dose-related biological effects could be expected in humans accidentally exposed to {sup 238}PuO{sub 2}. 89 refs., 10 figs., 11 tab.« less

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

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

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

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

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

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

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

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

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

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

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

13. VIEW OF THE MOLTEN SALT EXTRACTION LINE. THE MOLTEN SALT EXTRACTION PROCESS WAS USED TO PURIFY PLUTONIUM BY REMOVING AMERICIUM, A DECAY BY-PRODUCT OF PLUTONIUM. (1/98) - Rocky Flats Plant, Plutonium Fabrication, Central section of Plant, Golden, Jefferson County, CO

METHOD OF SEPARATION OF PLUTONIUM FROM CARRIER PRECIPITATES

DOEpatents

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.

EXTRACTION METHOD FOR SEPARATING URANIUM, PLUTONIUM, AND FISSION PRODUCTS FROM COMPOSITIONS CONTAINING SAME

DOEpatents

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.

REGENERATION OF REACTOR FUEL ELEMENTS

DOEpatents

Roake, W.E.; Lyon, W.L.

1960-03-29

A process of concentrating by electrolysis the uraatum and/or plutonium of an aluminum alloy containing these actinides after the actinide has been partially consumed by neutron bombardment in a reactor is given. The alloy is made the anode in a system having an aluminum cathode and a cryolite electrolyte. Electrolysis from 22 to 28 ampere-hours removes a sufficient quantity of aluminum from the alloy to make it suitable for reuse.

SEPARATION OF PLUTONYL IONS

DOEpatents

Connick, R.E.; McVey, Wm.H.

1958-07-15

A process is described for separating plutonyl ions from the acetate ions with which they are associated in certaln carrier precipitation methods of concentrating plutonium. The method consists in adding alkaline earth metal ions and subsequently alkalizing the solution, causing formation of an alkaltne earth plutonate precipitate. Barium hydroxide is used in a preferred embodiment since it provides alkaline earth metal ion and alkalizes the solution in one step forming insoluble barium platonate.

242-A Evaporator/plutonium uranium extraction (PUREX) effluent treatment facility (ETF) nonradioactive air emission test report

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

Hill, J.S., Westinghouse Hanford

1996-05-10

This report shows the methods used to test the stack gas outlet concentration and emission rate of Volatile Organic Compounds as Total Non-Methane Hydrocarbons in parts per million by volume,grams per dry standard cubic meter, and grams per minute from the PUREX ETF stream number G6 on the Hanford Site. Test results are shown in Appendix B.1.

Heterogeneous sodium fast reactor designed for transmuting minor actinide waste isotopes into plutonium fuel

NASA Astrophysics Data System (ADS)

Bays, Samuel Eugene

2008-10-01

In the past several years there has been a renewed interest in sodium fast reactor (SFR) technology for the purpose of destroying transuranic waste (TRU) produced by light water reactors (LWR). The utility of SFRs as waste burners is due to the fact that higher neutron energies allow all of the actinides, including the minor actinides (MA), to contribute to fission. It is well understood that many of the design issues of LWR spent nuclear fuel (SNF) disposal in a geologic repository are linked to MAs. Because the probability of fission for essentially all the "non-fissile" MAs is nearly zero at low neutron energies, these isotopes act as a neutron capture sink in most thermal reactor systems. Furthermore, because most of the isotopes produced by these capture reactions are also non-fissile, they too are neutron sinks in most thermal reactor systems. Conversely, with high neutron energies, the MAs can produce neutrons by fast fission. Additionally, capture reactions transmute the MAs into mostly plutonium isotopes, which can fission more readily at any energy. The transmutation of non-fissile into fissile atoms is the premise of the plutonium breeder reactor. In a breeder reactor, not only does the non-fissile "fertile" U-238 atom contribute fast fission neutrons, but also transmutes into fissile Pu-239. The fissile value of the plutonium produced by MA transmutation can only be realized in fast neutron spectra. This is due to the fact that the predominate isotope produced by MA transmutation, Pu-238, is itself not fissile. However, the Pu-238 fission cross section is significantly larger than the original transmutation parent, predominately: Np-237 and Am-241, in the fast energy range. Also, Pu-238's fission cross section and fission-to-capture ratio is almost as high as that of fissile Pu-239 in the fast neutron spectrum. It is also important to note that a neutron absorption in Pu-238, that does not cause fission, will instead produce fissile Pu-239. Given this fast fissile quality and also the fact that Pu-238 is transmuted from Np-237 and Am-241, these MAs are regarded as fertile material in the SFR design proposed by this dissertation. This dissertation demonstrates a SFR design which is dedicated to plutonium breeding by targeting Am-241 transmutation. This SFR design uses a moderated axial transmutation target that functions primarily as a pseudo-blanket fuel, which is reprocessed with the active driver fuel in an integrated recycling strategy. This work demonstrates the cost and feasibility advantages of plutonium breeding via MA transmutation by adopting reactor, reprocessing and fuel technologies previously demonstrated for traditional breeder reactors. The fuel cycle proposed seeks to find a harmony between the waste management advantages of transuranic burning SFRs and the resource sustainability of traditional plutonium breeder SFRs. As a result, the enhanced plutonium conversion from MAs decreases the burner SFR's fuel costs, by extracting more fissile value from the initial TRU purchased through SNF reprocessing.

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

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

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

1989-01-01

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

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

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

Whicker, F.W.

1977-08-01

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

Spatial analysis of plutonium-239 + 240 and Americium-241 in soils around Rocky Flats, Colorado

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

Litaor, M.I.

1995-05-01

Plutonium and american contamination of soils around Rocky Flats, Colorado resulted from past outdoor storage practices. Four previous studies produce four different Pu isopleth maps. Spatial estimation techniques were not used in the construction of these maps and were also based on an extremely small number of soil samples. The purpose of this study was to elucidate the magnitude of Pu-239 + 240 and Am-241 dispersion in the soil environment east of Rocky Flats using robust spatial estimation techniques. Soils were sampled from 118 plots of 1.01 and 4.05 ha by compositing 25 evenly spaced samples in each plot frommore » the top 0.64 cm. Plutonium-239 + 240 activity ranged from 1.85 to 53 560 Bq/kg with a mean of 1924 Bq/kg and a standard deviation of 6327 Bq/kg. Americium-241 activity ranged from 0.18 to 9990 Bq/kg with a mean of 321 Bq/kg and a standard deviation of 1143 Bq/kg. Geostatistical techniques were used to model the spatial dependency and construct isopleth maps showing Pu-239 + 240 and Am-241 distribution. The isopleth configuration was consistent with the hypothesis that the dominant dispersal mechanism of Pu-239 + 240 was wind dispersion from west to east. The Pu-239 + 240 isopleth map proposed to this study differed significantly in the direction and distance of dispersal from the previously published maps. This ispleth map as well as the Am-241 map should be used as the primary data for future risk assessment associated with public exposure to Pu-239 + 240 and Am-241. 37 refs., 7 figs., 2 tabs.« less

COMPLEX FLUORIDES OF PLUTONIUM AND AN ALKALI METAL

DOEpatents

Seaborg, G.T.

1960-08-01

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

The efficacy of denaturing actinide elements as a means of decreasing materials attractiveness

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

Hase, K.R.; Bathke, C.G.; Ebbinghaus, B.B.

2013-07-01

This study considers the concept of denaturing as applied to the actinide elements present in spent fuel as a means to reduce materials attractiveness. Highly attractive materials generally have low values of bare critical mass, heat content, and dose. To denature an attractive element, its spent-fuel isotopic composition (isotopic vector) is intentionally modified by introducing sufficient quantities of a significantly less attractive isotope to dilute the concentration of a highly attractive isotope so that the overall attractiveness of the element is reduced. The authors used FOM (Figure of Merit) formula as the material attractiveness metric for their parametric determination ofmore » the attractiveness of the Pu and U. Materials attractiveness needs to be considered in three distinct phases in the process to construct a nuclear explosive device (NED): the acquisition phase, processing phase, and utilization phase. The results show that denaturing uranium with {sup 238}U is actually an effective means of reducing the attractiveness. For uranium with a large minority of {sup 235}U, a mixture of 80% {sup 238}U to 20% {sup 235}U is required to reduce the attractiveness to low. For uranium with a large concentration of {sup 233}U, a mixture of 88% {sup 238}U to 12% {sup 233}U is required to reduce the attractiveness to low. The results also show that denaturing plutonium with {sup 238}Pu is less effective than denaturing uranium with {sup 238}U. Using {sup 238}Pu as the denaturing agent would require 80% or more by mass in order to reduce the attractiveness to low. No amount of {sup 240}Pu is enough to reduce the plutonium attractiveness below medium. The combination of {sup 238}Pu and {sup 240}Pu would require approximately 70% {sup 238}Pu and 25% {sup 240}Pu by mass to reduce the plutonium attractiveness to low.« less

Plutonium Interactions with Pseudomonas sp. and its Extracellular Polymeric Substances (Sorption and Reduction of Plutonium by Bacterial Extracellular Polymeric Substances)

DOE PAGES

Boggs, Mark A.; Jiao, Yongqin; Dai, Zurong; ...

2016-09-30

Safe and effective nuclear waste disposal, as well as accidental radionuclide releases, necessitates our understanding of the fate of radionuclides in the environment, including their interaction with microorganisms. We examined the sorption of Pu(IV) and Pu(V) toPseudomonassp. strain EPS-1W, an aerobic bacterium isolated from plutonium (Pu) contaminated groundwater collected in the United States at the Nevada National Security Site (NNSS), Nevada. We compared Pu sorption to cells with and without bound extracellular polymeric substances (EPS). Wild type cells with intact EPS sorbed Pu(V) more effectively than cells with EPS removed. In contrast, cells with and without EPS showed the samemore » sorption affinity for Pu(IV).In vitroexperiments with extracted EPS revealed rapid reduction of Pu(V) to Pu(IV). Transmission Electron Microscopy indicated that 2-3 nm nanocrystalline Pu(IV)O 2formed on cells equilibrated with high concentrations of Pu(IV) but not Pu(V). Thus, EPS, while facilitating Pu(V) reduction, inhibit the formation of nanocrystalline Pu(IV) precipitates. ImportanceOur results indicate that EPS are an effective reductant for Pu(V) and sorbent for Pu(IV), and may impact Pu redox cycling and mobility in the environment. Additionally, the resulting Pu morphology associated with EPS will depend on the concentration and initial Pu oxidation state. While our results are not directly applicable to the Pu transport situation at the NNSS, the results suggest that, in general, stationary microorganisms and biofilms will tend to limit the migration of Pu and provide an important Pu retardation mechanism in the environment. In a broader sense, our results along with a growing body of literature highlight the important role of microorganisms as producers of redox-active organic ligands and therefore as modulators of radionuclide redox transformations and complexation in the subsurface.« less

Plutonium Interactions with Pseudomonas sp. and its Extracellular Polymeric Substances (Sorption and Reduction of Plutonium by Bacterial Extracellular Polymeric Substances)

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

Boggs, Mark A.; Jiao, Yongqin; Dai, Zurong

Safe and effective nuclear waste disposal, as well as accidental radionuclide releases, necessitates our understanding of the fate of radionuclides in the environment, including their interaction with microorganisms. We examined the sorption of Pu(IV) and Pu(V) toPseudomonassp. strain EPS-1W, an aerobic bacterium isolated from plutonium (Pu) contaminated groundwater collected in the United States at the Nevada National Security Site (NNSS), Nevada. We compared Pu sorption to cells with and without bound extracellular polymeric substances (EPS). Wild type cells with intact EPS sorbed Pu(V) more effectively than cells with EPS removed. In contrast, cells with and without EPS showed the samemore » sorption affinity for Pu(IV).In vitroexperiments with extracted EPS revealed rapid reduction of Pu(V) to Pu(IV). Transmission Electron Microscopy indicated that 2-3 nm nanocrystalline Pu(IV)O 2formed on cells equilibrated with high concentrations of Pu(IV) but not Pu(V). Thus, EPS, while facilitating Pu(V) reduction, inhibit the formation of nanocrystalline Pu(IV) precipitates. ImportanceOur results indicate that EPS are an effective reductant for Pu(V) and sorbent for Pu(IV), and may impact Pu redox cycling and mobility in the environment. Additionally, the resulting Pu morphology associated with EPS will depend on the concentration and initial Pu oxidation state. While our results are not directly applicable to the Pu transport situation at the NNSS, the results suggest that, in general, stationary microorganisms and biofilms will tend to limit the migration of Pu and provide an important Pu retardation mechanism in the environment. In a broader sense, our results along with a growing body of literature highlight the important role of microorganisms as producers of redox-active organic ligands and therefore as modulators of radionuclide redox transformations and complexation in the subsurface.« less

An update of hydrologic conditions and distribution of selected constituents in water, Snake River Plain aquifer, Idaho National Laboratory, Idaho, Emphasis 1999-2001

USGS Publications Warehouse

Davis, Linda C.

2006-01-01

Radiochemical and chemical wastewater discharged since 1952 to infiltration ponds, evaporation ponds, and disposal wells at the Idaho National Laboratory (INL) has affected water quality in the Snake River Plain aquifer underlying the INL. The U.S. Geological Survey (USGS), in cooperation with the U.S. Department of Energy, maintains ground-water monitoring networks at the INL to determine hydrologic trends, and to delineate the movement of radiochemical and chemical wastes in the aquifer. This report presents an analysis of water-level and water-quality data collected from wells in the USGS ground-water monitoring networks during 1999-2001. Water in the Snake River Plain aquifer moves principally through fractures and interflow zones in basalt, generally flows southwestward, and eventually discharges at springs along the Snake River. The aquifer is recharged principally from infiltration of irrigation water, infiltration of streamflow, ground-water inflow from adjoining mountain drainage basins, and infiltration of precipitation. Water levels in wells rose in the northern and west-central parts of the INL by 1 to 3 feet, and declined in the southwestern parts of the INL by up to 4 feet during 1999-2001. Detectable concentrations of radiochemical constituents in water samples from wells in the Snake River Plain aquifer at the INL generally decreased or remained constant during 1999-2001. Decreases in concentrations were attributed to decreased rates of radioactive-waste disposal, radioactive decay, changes in waste-disposal methods, and dilution from recharge. Tritium concentrations in water samples decreased as much as 8.3 picocuries per milliliter (pCi/mL) during 1999-2001, ranging from 0.43?0.14 to 13.6?0.6 pCi/mL in October 2001. Tritium concentrations in five wells near the Idaho Nuclear Technology and Engineering Center (INTEC) increased a few picocuries per milliliter from October 2000 to October 2001. Strontium-90 concentrations decreased or remained constant during 1999-2001, ranging from 2.1?0.6 to 42.4?1.4 pCi/L in October 2001. During 1999-2001, concentrations of cesium-137, plutonium-238, and plutonium-239, -240 (undivided) were less than the reporting level in water samples from all wells sampled at the INL. The concentration of americium-241 in one sample was 0.003?0.001 pCi/L, the reporting level for that constituent. Cobalt-60 was not detected in any samples collected during 1999-2001. Changes in detectable concentrations of nonradioactive chemical constituents in water from the Snake River Plain aquifer at the INL varied during 1999-2001. In October 2001, water from one well south of the Reactor Technology Complex (RTC) [known as the Test Reactor Area (TRA) until 2005] contained 139 micrograms per liter (?g/L) of chromium, a decrease from the concentration of 168 ?g/L detected in October 1998. Other water samples contained from less than 16.7 to 21.3 ?g/L of chromium. In October 2001, concentrations of sodium in water samples from most of the wells in the southern part of the INL were larger than the background concentration of 10 mg/L, but were similar to or slightly less than October 1998 concentrations. The largest sodium concentration was 75 milligrams per liter (mg/L) in water from well USGS 113. In 2001, chloride concentrations in most water samples from the INTEC and the Central Facilities Area (CFA) exceeded ambient concentrations of 10 and 20 mg/L, respectively. Chloride concentrations in water from wells near the RTC were less than 20 mg/L. At the Radioactive Waste Management Complex (RWMC), chloride concentrations in water from wells USGS 88, 89, and 120 were 81, 40, and 23 mg/L, respectively. Concentrations of chloride in all other wells near the RWMC were less than 19 mg/L. During 2001, concentrations of sulfate in water from two wells near the RTC, two wells near the RWMC, and one well near the CFA exceeded 40 mg/L, the estimated background concentration of sulfate in the Snake River

RECOVERY OF PLUTONIUM BY CARRIER PRECIPITATION

DOEpatents

Goeckermann, R.H.

1961-04-01

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

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

EPA Pesticide Factsheets

SAM lists this method for the qualitative determination of Americium-241, Radium-226, Plutonium-238, Plutonium-239 and isotopic uranium in drinking water samples using alpha spectrometry and radiostrontium using beta counting.

MOLTEN PLUTONIUM FUELED FAST BREEDER REACTOR

DOEpatents

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

1962-06-26

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

ELECTRODEPOSITION OF PLUTONIUM

DOEpatents

Wolter, F.J.

1957-09-10

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

Removal of plutonium from hepatic tissue

DOEpatents

Lindenbaum, Arthur; Rosenthal, Marcia W.

1979-01-01

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

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

EPA Pesticide Factsheets

Technical Fact Sheet Analysis Purpose: Qualitative analysis Technique: Alpha spectrometry Method Developed for: Americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in concrete and brick samples Method Selected for: SAM lists this method for qualitative analysis of americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in concrete or brick building materials. Summary of subject analytical method which will be posted to the SAM website to allow access to the method.

METHOD OF SEPARATING PLUTONIUM FROM LANTHANUM FLUORIDE CARRIER

DOEpatents

Watt, G.W.; Goeckermann, R.H.

1958-06-10

An improvement in oxidation-reduction type methods of separating plutoniunn from elements associated with it in a neutron-irradiated uranium solution is described. The method relates to the separating of plutonium from lanthanum ions in an aqueous 0.5 to 2.5 N nitric acid solution by 'treating the solution, at room temperature, with ammonium sulfite in an amount sufficient to reduce the hexavalent plutonium present to a lower valence state, and then treating the solution with H/sub 2/O/sub 2/ thereby forming a tetravalent plutonium peroxide precipitate.

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

DOEpatents

Balthis, J.H.

1961-07-18

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

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

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

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

PROCESS OF MAKING A NEUTRONIC REACTOR FUEL ELEMENT COMPOSITION

DOEpatents

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/.

SEPARATION OF URANIUM, PLUTONIUM AND FISSION PRODUCTS

DOEpatents

Nicholls, C.M.; Wells, I.; Spence, R.

1959-10-13

The separation of uranium and plutonium from neutronirradiated uranium is described. The neutron-irradiated uranium is dissolved in nitric acid to provide an aqueous solution 3N in nitric acid. The fission products of the solution are extruded by treating the solution with dibutyl carbitol substantially 1.8N in nitric acid. The organic solvent phase is separated and neutralized with ammonium hydroxide and the plutonium reduced with hydroxylamine base to the trivalent state. Treatment of the mixture with saturated ammonium nitrate extracts the reduced plutonium and leaves the uranium in the organic solvent.

Radiation from plutonium 238 used in space applications

NASA Technical Reports Server (NTRS)

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

1972-01-01

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

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

DOE PAGES

Rim, Jung H.; Peterson, Dominic S.; Armenta, Claudine E.; ...

2015-05-08

We describe a new analyte extraction technique using Polymer Ligand Film (PLF). PLFs were synthesized to perform direct sorption of analytes onto its surface for direct counting using alpha spectroscopy. The main focus of the new technique is to shorten and simplify the procedure for chemically isolating radionuclides for determination through a radiometric technique. 4'(5')-di-t-butylcyclohexano 18-crown-6 (DtBuCH 18C 6) and 2-ethylhexylphosphonic acid (HEH[EHP]) were examined for plutonium extraction. Di(2-ethyl hexyl) phosphoric acid (HDEHP) were examined for plutonium and uranium extraction. DtBuCH 18C 6 and HEH[EHP] were not effective in plutonium extraction. HDEHP PLFs were effective for plutonium but not formore » uranium.« less

METHOD OF FORMING PLUTONIUM-BEARING CARRIER PRECIPITATES AND WASHING SAME

DOEpatents

Faris, B.F.

1959-02-24

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

Radiation damage and annealing in plutonium tetrafluoride

DOE PAGES

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

2017-08-03

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

Analysis of trace neptunium in the vicinity of underground nuclear tests at the Nevada National Security Site

DOE PAGES

Zhao, P.; Tinnacher, R. M.; Zavarin, M.; ...

2014-11-01

A high sensitivity analytical method for 237Np analysis was developed and applied to groundwater samples from the Nevada National Security Site (NNSS) using short-lived 239Np as a yield tracer and HR magnetic sector ICP-MS. The 237Np concentrations in the vicinity of the Almendro, Cambric, Dalhart, Cheshire, and Chancellor underground nuclear test locations range from <4 × 10 -4 to 2.6 mBq/L (6 × 10 -17–4.2 × 10 -13 mol/L). All measured 237Np concentrations are well below the drinking water maximum contaminant level for alpha emitters identified by the U.S. EPA (560 mBq/L). Nevertheless, 237Np remains an important indicator for radionuclidemore » transport rates at the NNSS. Retardation factor ratios were used to compare the mobility of 237Np to that of other radionuclides. The results suggest that 237Np is less mobile than tritium and other non-sorbing radionuclides ( 14C, 36Cl, 99Tc and 129I) as expected. Surprisingly, 237Np and plutonium ( 239,240Pu) retardation factors are very similar. It is possible that Np(IV) exists under mildly reducing groundwater conditions and exhibits a retardation behavior that is comparable to Pu(IV). Independent of the underlying process, 237Np is migrating downgradient from NNSS underground nuclear tests at very low but measureable concentrations.« less

Statistical design and analysis of environmental studies for plutonium and other transuranics at NAEG ''safety-shot'' sites

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

Gilbert, R.O.; Eberhardt, L.L.; Fowler, E.B.

This paper is centered around the use of stratified random sampling for estimating the total amount (inventory) of $sup 239-240$Pu and uranium in surface soil at ten ''safety-shot'' sites on the Nevada Test Site (NTS) and Tonopah Test Range (TTR) that are currently being studied by the Nevada Applied Ecology Group (NAEG). The use of stratified random sampling has resulted in estimates of inventory at these desert study sites that have smaller standard errors than would have been the case had simple random sampling (no stratification) been used. Estimates of inventory are given for $sup 235$U, $sup 238$U, and $supmore » 239-240$Pu in soil at A Site of Area 11 on the NTS. Other results presented include average concentrations of one or more of these isotopes in soil and vegetation and in soil profile samples at depths to 25 cm. The regression relationship between soil and vegetation concentrations of $sup 235$U and $sup 238$U at adjacent sampling locations is also examined using three different models. The applicability of stratified random sampling to the estimation of concentration contours of $sup 239-240$Pu in surface soil using computer algorithms is also investigated. Estimates of such contours are obtained using several different methods. The planning of field sampling plans for estimating inventory and distribution is discussed. (auth)« less

Reconstructed plutonium fallout in the GV7 firn core from Northern Victoria Land, East Antarctica

NASA Astrophysics Data System (ADS)

Hwang, H.; Han, Y.; Kang, J.; Lee, K.; Hong, S.; Hur, S. D.; Narcisi, B.; Frezzotti, M.

2017-12-01

Atmospheric nuclear explosions during the period from the 1940s to the 1980s are the major anthropogenic source of plutonium (Pu) in the environment. In this work, we analyzed fg g-1 levels of artificial Pu, released predominantly by atmospheric nuclear weapons tests. We measured 351 samples which collected a 78 m-depth fire core at the site of GV7 (S 70°41'17.1", E 158°51'48.9", 1950 m a.s.l.), Northern Victoria Land, East Antarctica. To determine the Pu concentration in the samples, we used an inductively coupled plasma sector field mass spectrometry coupled with an Apex high-efficiency sample introduction system, which has the advantages of small sample consumption and simple sample preparation. We reconstructed the firn core Pu fallout record for the period after 1954 CE shows a significant fluctuation in agreement with past atmospheric nuclear testing. These data will contribute to ice core research by providing depth-age information.

Johnston Atoll Plutonium Cleanup Project, plant modification and operation. Volume 1. Annual report option year 2. Technical report, 1 October 1992-24 May 1993

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

Moroney, K.S.; Moroney, J.D.; Johnson, N.R.

1995-04-01

This report continues the documentation of the operation of TMA/Eberline`s Segmented Gate System technology for removing mixed plutonium and americium contamination at DNA`s Johnston Atoll site. Contaminated feed is conveyed under arrays of radiation detectors coupled with sophisticated computer software developed by Eberline Instrument Corporation. Segmented gates (chutes) on pneumatically-driven pistons move forward when contamination is detected to remove only the contaminated portion from the main flow of feed material. Only about one pint of contaminant is removed during each diversion event. At the JA site, a 98% volume reduction has been achieved, with the remediated soil cleaned to DNA`smore » criteria for release for unrestricted use of 500 Bq/kg total tnansuranic alpha contamination and no hot particles of greater than 5000 Becquerrels. The low level waste concentrate is expected to be packaged for shipment to an approved defense waste disposal site.« less

Johnston Atoll Plutonium Cleanup Project. Plant modification and operation. Volume 2. Annual report option year 2. Appendix A. Technical report, 1 October 1992-24 May 1993

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

Moroney, K.S.; Moroney, J.D.; Johnson, N.R.

1995-04-01

This report continues the documentation of the operation of TMA/Eberline`s Segmented Gate System technology for removing mixed plutonium and americium contamination at DNA`s Johnston Atoll site. Contaminated feed is conveyed under arrays of radiation detectors coupled with sophisticated computer software developed by Eberline Instrument Corporation. Segmented gates (chutes) on pneumatically-driven pistons move forward when contamination is detected to remove only the contaminated portion from the main flow of feed material. Only about one pint of contaminant is removed during each diversion event. At the JA site, a 98% volume reduction has been achieved, with the remediated soil cleaned to DNA`smore » criteria for release for unrestricted use of 500 Bq/kg total transuranic alpha contamination and no hot particles of greater than 5000 Becquerrels. The low level waste concentrate is expected to be packaged for shipment to an approved defense waste disposal site.« less

Johnston Atoll Plutonium Cleanup Project, plant modification and operation. Volume 3. Annual report option year 2. Appendices b through h. Technical report, 1 October 1992-24 May 1993

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

Moroney, K.S.; Moroney, J.D.; Johnson, N.R.

1995-04-01

This report continues the documentation of the operation of TMA/Eberline`s Segmented Gate System technology for removing mixed plutonium and americium contamination at DNA`s Johnston Atoll site. Contaminated feed is conveyed under arrays of radiation detectors coupled with sophisticated computer software developed by Eberline Instrument Corporation. Segmented gates (chutes) on pneumatically-driven pistons move forward when contamination is detected to remove only the contaminated portion from the main flow of feed material. Only about one pint of contaminant is removed during each diversion event. At the JA site, a 98% volume reduction has been achieved, with the remediated soil cleaned to DNA`smore » criteria for release for unrestricted use of 500 Bq/kg total transuranic alpha contamination and no hot particles of greater than 5000 Becquerrels. The low level waste concentrate is expected to be packaged for shipment to an approved defense waste disposal site.« less

Plutonium, curium, and other radionuclide uptake by the rice plant from a naturally weathered, contaminated soil

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

Adriano, D.C.; McLeod, K.W.; Ciravolo, T.G.

1981-07-01

A greenhouse study using three United States rice varieties (Belle Patna, Nato, and Starbonnet) varying in maturity period and a widely used Asian variety (IR-1561) indicates that, with the exception of /sup 137/Cs, no significant differences were obtained among varieties in the foliage uptake of selected gamma-emitters. On the average, /sup 137/Cs and /sup 40/K were translocated less to the grain than to the foliage. The concentration ratio (CR) values for the gamma-emitters, with the exception of /sup 40/K, were approximately one order of magnitude higher than those for subterranean crops grown in experimental plots adjacent to a chemical separationsmore » facility at the Savannah River Plant. The CR values for /sup 238/Pu and /sup 244/Cm are within the range of values published in the open literature. The CR values for /sup 239/ /sup 240/Pu, however, were higher than the normally reported values for plants grown in nonamended soils.« 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

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

PubMed

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

2003-11-01

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

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

NASA Astrophysics Data System (ADS)

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

2018-02-01

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

Oxygen diffusion model of the mixed (U,Pu)O2 ± x: Assessment and application

NASA Astrophysics Data System (ADS)

Moore, Emily; Guéneau, Christine; Crocombette, Jean-Paul

2017-03-01

The uranium-plutonium (U,Pu)O2 ± x mixed oxide (MOX) is used as a nuclear fuel in some light water reactors and considered for future reactor generations. To gain insight into fuel restructuring, which occurs during the fuel lifetime as well as possible accident scenarios understanding of the thermodynamic and kinetic behavior is crucial. A comprehensive evaluation of thermo-kinetic properties is incorporated in a computational CALPHAD type model. The present DICTRA based model describes oxygen diffusion across the whole range of plutonium, uranium and oxygen compositions and temperatures by incorporating vacancy and interstitial migration pathways for oxygen. The self and chemical diffusion coefficients are assessed for the binary UO2 ± x and PuO2 - x systems and the description is extended to the ternary mixed oxide (U,Pu)O2 ± x by extrapolation. A simulation to validate the applicability of this model is considered.

PLUTONIUM-CERIUM-COPPER ALLOYS

DOEpatents

Coffinberry, A.S.

1959-05-12

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

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2012 CFR

2012-01-01

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

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2014 CFR

2014-01-01

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

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2013 CFR

2013-01-01

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

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

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

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

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

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

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

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2010 CFR

2010-01-01

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

Removal of plutonium and americium from alkaline waste solutions

DOEpatents

Schulz, Wallace W.

1979-01-01

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

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2011 CFR

2011-01-01

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

PREPARATION OF HALIDES OF PLUTONIUM

DOEpatents

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.

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

DOEpatents

Davies, T.H.

1959-12-15

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

Mortality among workers with chronic radiation sickness

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

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

1996-07-01

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

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

DOEpatents

Li, Shelly Xiaowei; Westphal, Brian Robert; Herrmann, Steven Douglas

2015-09-01

A method and device for the real-time, in-situ monitoring of Plutonium content in U--Pu Alloys comprising providing a crucible. The crucible has an interior non-reactive to a metallic U--Pu alloy within said interior of said crucible. The U--Pu alloy comprises metallic uranium and plutonium. The U--Pu alloy is heated to a liquid in an inert or reducing atmosphere. The heated U--Pu alloy is then cooled to a solid in an inert or reducing atmosphere. As the U--Pu alloy is cooled, the temperature of the U--Pu alloy is monitored. A solidification temperature signature is determined from the monitored temperature of the U--Pu alloy during the step of cooling. The amount of Uranium and the amount of Plutonium in the U--Pu alloy is then determined from the determined solidification temperature signature.

Estimation of the formation rates of polyatomic species of heavy metals in plutonium analyses using a multicollector ICP-MS with a desolvating nebulizer

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

Mitroshkov, Alexandre V.; Olsen, Khris B.; Thomas, Linda M.

2015-01-01

The analyses of IAEA and environmental samples for Plutonium isotopic content are conducted normally at very low concentrations of Pu–usually in the range of part per trillion level and even more often at the parts per quadrillion level. To analyze such low concentrations, the interferences in the analytical solution must be reduced as much as possible. Polyatomic interferences (PIs), formed by the heavy metals (HMs) from Hf to Bi are known to create the problems for Pu isotopic analyses, because even the relatively high resolution of a modern multicollector ICP-MS is not enough to separate Pu isotopes from this PIsmore » in most of the cases. Desolvating nebulizers (DSN) (e.g. APEX and AridusII) reduce significantly the formation of PIs compare to the use of wet plasma. The purpose of this work was to investigate the rate of formation of PIs, produced by HMs, when high resolution MC ICP-MS with desolvating nebulizer was used for Pu isotopic analyses and to estimate the influence of the metals present in the sample on the results of analyses. The NU Plasma HR Multicollector and AridusII desolvating nebulizer were used in this investigation. This investigation was done for all Pu isotopes normally analyzed by ICP-MS, including ²⁴⁴Pu, with the exception of ²³⁸Pu, which most of the time can’t be analyzed by ICP-MS, because of the overwhelming presence of ²³⁸U in the solutions. The PI formation rates were determined and reported for all 12 HMs from Hf to Bi. Selected IAEA samples were scanned for the presence of HMs and the influence of HMs on the results of Pu isotopic analyses was evaluated. It was found that the implemented separation procedure provides sufficient separation of HM from Pu, although the effect of PIs on the measurement of low level isotopes like ²⁴¹Pu and ²⁴²Pu in some cases can still be observed.« less

Application of 129I/127I Ratios in Groundwater Studies Conducted at Los Alamos National Laboratory, New Mexico

NASA Astrophysics Data System (ADS)

Longmire, P.; Dale, M.; Granzow, K.; Yanicak, S. M.

2014-12-01

Los Alamos National Laboratory (LANL) is an operating nuclear site that has released treated effluents from three plutonium-processing facilities since the mid 1940s. The radioisotope 129I (T1/2 = 15.7 Myrs) derived from235U and 239Pu processing at LANL is locally detected in groundwater above background concentrations. This isotope provides a unique tracer for groundwater investigations conducted at LANL that helps to identify source releases linked to groundwater-flow paths in aquifers subject to binary and ternary mixing of natural- and industrial-derived waters containing chromate and other chemicals. Bromide, chlorate, chloride, nitrate, perchlorate, sulfate, and tritium were associated with multiple outfalls at LANL and, therefore, do not provide unique chemical signatures identifying a specific point of release or source. Natural and anthropogenic ratios of 129I/127I measured in groundwater samples collected at LANL were quantified using accelerator mass spectrometry at Purdue Rare Isotope Measurement Laboratory, Purdue University. Anthropogenic ratios of 129I/127I range from 1,531 X 10-15 to 10,323 X 10-15 within perched-intermediate groundwater present in volcanoclastic and basalt aquifers (210 - 216 m depth). Anthropogenic ratios of 129I/127I range from 359 X 10-15 to 4,350 X 10-15 within the regional aquifer (280 m depth) consisting of volcanoclastic sediments of variable hydraulic properties. Local background ratios of 129I/127I have a narrow range of 171 X 10-15 to 378 X 10-15 in the regional aquifer. Dissolved iodide measured in groundwater at LANL is stable dominantly as iodate. Background concentrations of dissolved iodate (0.1 to 33.2 nM) are less variable compared to anthropogenic iodate (8.0 to 246 nM) in groundwater at the site. Variability in concentrations of anthropogenic iodate is controlled by heterogeneous source releases of iodate over time and non-uniform mixing of groundwater in the different aquifers.

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

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

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

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

PLUTONIUM ELECTROREFINING CELLS

DOEpatents

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

1963-07-16

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

PLUTONIUM SEPARATION METHOD

DOEpatents

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.

Development of first ever scanning probe microscopy capabilities for plutonium

NASA Astrophysics Data System (ADS)

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

2017-04-01

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

Development of first ever scanning probe microscopy capabilities for plutonium

DOE PAGES

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

2017-04-01

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

Metal concentrations, foraging distances, and fledging success of great blue herons nesting along the Hanford Reach of the Columbia River.

PubMed

Tiller, Brett L; Marco, J D; Rickard, W H

2005-05-01

An ecological risk assessment of the spatial distribution of metal concentrations along the Hanford Reach of the free-flowing Columbia River in southcentral Washington, identified great blue herons, Ardea herodias, at potential risk through the ingestion of contaminated riverine biota, especially fish. We measured metal concentrations in livers of pre-flight herons from the Hanford Reach and excrement samples taken from the same nests. Nests were distributed among three colonies situated upstream and downstream from nine retired plutonium production reactors along the river where metals in reactor coolant waters had been released directly into the river or disposed to shoreline retention basins and ditches. Distances traveled by parent herons to foraging areas along the river shore were determined by visually tracking parent birds as they flew from nests to upriver and downriver foraging sites. Foraging flight distances varied between colonies with mean distances ranging between 0.7 and 3.1 km. Cadmium, Cr, and Pb concentrations were higher in excrement than in the livers of pre-flight herons but the opposite was noted for Cu, Hg, and Zn. Highest metal concentrations of Cr, Cu, Zn, Cd, and Pb, were measured in excrement taken from heron nests at the colony located upstream from all reactors. These results were consistent with metal concentrations reported in river sediment from the same regions, indicating excrement from the heron nests may be a useful indicator of dietary uptake of metals by herons. Fledging success and eggshell thickness measurements were used as an index of health of the local heron population. The results indicate that the reproductive health of great blue herons nesting along the Hanford Reach is among the highest reported in the continental United States.

PLUTONIUM-URANIUM-TITANIUM ALLOYS

DOEpatents

Coffinberry, A.S.

1959-07-28

A plutonium-uranium alloy suitable for use as the fuel element in a fast breeder reactor is described. The alloy contains from 15 to 60 at.% titanium with the remainder uranium and plutonium in a specific ratio, thereby limiting the undesirable zeta phase and rendering the alloy relatively resistant to corrosion and giving it the essential characteristic of good mechanical workability.

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

High-Temperature Oxidation of Plutonium Surrogate Metals and Alloys

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

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

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

The underwater coincidence counter (UWCC) for plutonium measurements in mixed oxide fuels

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

Eccleston, G.W.; Menlove, H.O.; Abhold, M.

1998-12-31

The use of fresh uranium-plutonium mixed oxide (MOX) fuel in light-water reactors (LWR) is increasing in Europe and Japan and it is necessary to verify the plutonium content in the fuel for international safeguards purposes. The UWCC is a new instrument that has been designed to operate underwater and nondestructively measure the plutonium in unirradiated MOX fuel assemblies. The UWCC can be quickly configured to measure either boiling-water reactor (BWR) or pressurized-water reactor (PWR) fuel assemblies. The plutonium loading per unit length is measured using the UWCC to precisions of less than 1% in a measurement time of 2 tomore » 3 minutes. Initial calibrations of the UWCC were completed on measurements of MOX fuel in Mol, Belgium. The MCNP-REN Monte Carlo simulation code is being benchmarked to the calibration measurements to allow accurate simulations for extended calibrations of the UWCC.« less

TERNARY ALLOY-CONTAINING PLUTONIUM

DOEpatents

Waber, J.T.

1960-02-23

Ternary alloys of uranium and plutonium containing as the third element either molybdenum or zirconium are reported. Such alloys are particularly useful as reactor fuels in fast breeder reactors. The alloy contains from 2 to 25 at.% of molybdenum or zirconium, the balance being a combination of uranium and plutonium in the ratio of from 1 to 9 atoms of uranlum for each atom of plutonium. These alloys are prepared by melting the constituent elements, treating them at an elevated temperature for homogenization, and cooling them to room temperature, the rate of cooling varying with the oomposition and the desired phase structure. The preferred embodiment contains 12 to 25 at.% of molybdenum and is treated by quenching to obtain a body centered cubic crystal structure. The most important advantage of these alloys over prior binary alloys of both plutonium and uranium is the lack of cracking during casting and their ready machinability.

Microprobe Analysis of Pu-Ga Standards

DOE PAGES

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

2017-08-04

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

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

NASA Astrophysics Data System (ADS)

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

2000-07-01

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

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

Measured solubilities and speciations from oversaturation experiments of neptunium, plutonium, and americium in UE-25p No. 1 well water from the Yucca Mountain region: Milestone report 3329-WBS1.2.3.4.1.3.1

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

Nitsche, H.; Roberts, K.; Prussin, T.

1994-04-01

Solubility and speciation are important in understanding aqueous radionuclide transport through the geosphere. They define the source term for transport retardation processes such as sorption and colloid formation. Solubility and speciation data are useful in verifying the validity of geochemical codes that are a part of predictive transport models. Results are presented from solubility and speciation experiments of {sup 237}NpO{sub 2}{sup +}, {sup 239}Pu{sup 4+}, and {sup 241}Am{sup 3+}/Nd{sup 3+} in a modified UE-25p No. 1 groundwater (from the Yucca Mountain region, Nevada, which is being investigated as a potential high-level nuclear waste disposal site) at two different temperatures (25{degree}more » and 60{degree}C) and three pH values (6.0, 7.0, 8.5). The solubility-controlling steady-state solids were identified and the speciation and/or oxidation states present in the supernatant solutions were determined. The neptunium solubility decreased with increasing temperature and pH. Plutonium concentrations significantly decreased with increasing temperature at pH 6 and 7. The concentration at pH 8.5 hardly decreased at all with increasing temperature. At both temperatures the concentrations were highest at pH 8.5, lowest at pH 7, and in between at pH 6. For the americium/neodymium solutions, the solubility decreased significantly with increasing temperature and increased somewhat with increasing pH.« less

Spall fracture and strength of uranium, plutonium and their alloys under shock wave loading

NASA Astrophysics Data System (ADS)

Golubev, Vladimir

2015-06-01

Numerous results on studying the spall fracture phenomenon of uranium, two its alloys with molybdenum and zirconium, plutonium and its alloy with gallium under shock wave loading are presented in the paper. The majority of tests were conducted with the samples in the form of disks 4mm in thickness. They were loaded by the impact of aluminum plates 4mm thick through a copper screen serving as the cover or bottom part of a special container. The initial temperature of samples was changed in the range of -196 - 800 C degree for uranium and 40 - 315 C degree for plutonium. The character of spall failure of materials and the degree of damage for all tested samples were observed on the longitudinal metallographic sections of recovered samples. For a concrete test temperature, the impact velocity was sequentially changed and therefore the loading conditions corresponding to the consecutive transition from microdamage nucleation up to complete macroscopic spall fracture were determined. Numerical calculations of the conditions of shock wave loading and spall fracture of samples were performed in the elastoplastic approach. Several two- and three-dimensional effects of loading were taken into account. Some results obtained under conditions of intensive impulse irradiation and intensive explosive loading are presented too. The rather complete analysis and comparison of obtained results with the data of other researchers on the spall fracture of examined materials were conducted.

Spent nuclear fuel recycling with plasma reduction and etching

DOEpatents

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.

PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINATING ELEMENTS

DOEpatents

Duffield, R.B.

1959-02-24

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

PLUTONIUM RECOVERY FROM NEUTRON-BOMBARDED URANIUM FUEL

DOEpatents

Moore, R.H.

1964-03-24

A process of recovering plutonium from fuel by dissolution in molten KAlCl/sub 4/ double salt is described. Molten lithium chloride plus stannous chloride is added to reduce plutonium tetrachloride to the trichloride, which is dissolved in a lithium chloride phase while the uranium, as the tetrachloride, is dissolved in a double-salt phase. Separation of the two phases is discussed. (AEC)

SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS BY ADSORPTION

DOEpatents

Seaborg, G.T.; Willard, J.E.

1958-01-01

A method is presented for the separation of plutonium from solutions containing that element in a valence state not higher than 41 together with uranium ions and fission products. This separation is accomplished by contacting the solutions with diatomaceous earth which preferentially adsorbs the plutonium present. Also mentioned as effective for this adsorbtive separation are silica gel, filler's earth and alumina.

METHOD OF RECOVERING PLUTONIUM VALUES FROM AQUEOUS SOLUTIONS BY CARRIER PRECIPITATION

DOEpatents

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/.

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

DOE PAGES

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

2017-10-07

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

METHOD AND MEANS FOR ELECTROLYTIC PURIFICATION OF PLUTONIUM

DOEpatents

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

1960-02-01

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