Presence of plutonium isotopes, {sup 239}Pu and {sup 240}Pu, in soils from Chile

Energy Technology Data Exchange (ETDEWEB)

Chamizo, E., E-mail: echamizo@us.es [Centro Nacional de Aceleradores, Avda. Thomas Alba Edison, 7, 41092 Sevilla (Spain); Garcia-Leon, M., E-mail: manugar@us.es [Departamento de Fisica Atomica, Molecular y Nuclear, Universidad de Sevilla, Avda. Reina Mercedes sn, 41012 Seville (Spain); Peruchena, J.I., E-mail: jiperuchena@gmail.com [Centro Nacional de Aceleradores, Avda. Thomas Alba Edison, 7, 41092 Sevilla (Spain); Cereceda, F., E-mail: francisco.cereceda@usm.cl [Laboratorio de Quimica Ambiental, Centro de Tecnologias Ambientales (CETAM), Universidad Tecnica Federico Santa Maria, Casilla 110-V, Valparaiso (Chile); Vidal, V., E-mail: victor.vidal@usm.cl [Laboratorio de Quimica Ambiental, Centro de Tecnologias Ambientales (CETAM), Universidad Tecnica Federico Santa Maria, Casilla 110-V, Valparaiso (Chile); Pinilla, E., E-mail: epinilla@unex.es [Departamento de Quimica Analitica, Facultad de Ciencias, Universidad de Extremadura, Avda. de Elvas sn, 06071 Badajoz (Spain); Miro, C., E-mail: cmiro@unex.es [Departamento de Fisica Aplicada, Universidad de Extremadura, Avda. de la Universidad sn, 10071 Caceres (Spain)

2011-12-15

Plutonium is present in every environmental compartment, due to a variety of nuclear activities. The Southern Hemisphere has received about 20% of the global {sup 239}Pu and {sup 240}Pu environmental inventory, with an important contribution of the so-called tropospheric fallout from both the atmospheric nuclear tests performed in the French Polynesia and in Australia by France and United Kingdom, respectively. In this work we provide new data on the impact of these tests to South America through the study of {sup 239}Pu and {sup 240}Pu in soils from different areas of Northern, Central and Southern Chile. The obtained results point out to the presence of debris from the French tests in the 20-40 Degree-Sign Southern latitude range, with {sup 240}Pu/{sup 239}Pu atomic ratios quite heterogeneous and ranging from 0.02 to 0.23. They are significantly different from the expected one for the global fallout in the Southern Hemisphere for the 30-53 Degree-Sign S latitude range (0.185 {+-} 0.047), but they follow the same trend as the reported values by the Department of Energy of United States for other points with similar latitudes. The {sup 239+240}Pu activity inventories show as well a wider variability range in that latitude range, in agreement with the expected heterogeneity of the contamination.

Comparison of U-Pu-Mo, U-Pu-Nb, U-Pu-Ti and U-Pu-Zr alloys; Comparaison des alliages U-Pu-Mo, U-Pu-Nb, U-Pu-Ti, U-Pu-Zr

Energy Technology Data Exchange (ETDEWEB)

Boucher, R; Barthelemy, P [Commissariat a l' Energie Atomique, Fontenay-aux-Roses (France). Centre d' Etudes Nucleaires

1964-07-01

The data concerning the U-Pu, U-Pu-Mo and U-Pu-Nb are recalled. The results obtained with U-Pu-Ti and U-Pu-Zr alloys containing 15-20 per cent Pu and 10 wt. per cent ternary element are reported. The transformation temperatures, the expansion coefficients, the nature of phases, the thermal cycling behaviour have been determined. A list of the principal properties of these different alloys is presented and the possibilities of their use as fast reactor's fuel element are considered. The U-Pu-Ti alloys seem to be quite promising: easiness of fabrication, large thermal stability, excellent behaviour in air, small quantity of zeta phase, temperature of solidus superior to 1100 deg. C. (authors) [French] On rappelle brievement les connaissances acquises sur les alliages U-Pu, U-Pu-Mo et U-Pu-Nb. On presente les resultats obtenus avec les alliages U-Pu-Ti et U-Pu-Zr pour des teneurs de 15 a 20 pour cent de plutonium et 10 pour cent en poids d'element ternaire. On a determine les temperatures de transformation, les coefficients de dilatation, la nature des phases, la conductibilite thermique a 20 deg. C, la tenue au cyclage thermique et diverses autres proprietes. Un tableau resume les principales proprietes des divers alliages. On considere les possibilites d'emploi de ces alliages comme combustibles de reacteur rapide. Les alliages U-Pu-Ti paraissent particulierement interessants: facilite d'elaboration, stabilite thermique etendue, tenue dans l'air excellente, faible quantite de la phase U-Pu zeta, temperature de fusion commencante superieure a 1100 deg. C. (auteurs)

Solubility of reactor fuels in the mouse lung with respect to their U/Pu and 238Pu/239Pu ratios

International Nuclear Information System (INIS)

Talbot, R.J.; Baker, S.T.

1989-01-01

The studies reported were designed to assess the comparative in vivo solubilities of a range of plutonium containing reactor fuels. To simulate these fuels, mixed U/Pu oxides were prepared and calcined at 1600 0 C. A plutonium content of 3% w/w was chosen as typical of water-cooled reactor fuel. Higher concentrations of plutonium (10, 20 and 30%) were included to simulate fast reactor fuel. As it is known that 238 PuO 2 , with high specific activity, is translocated more rapidly from lung than 239 PuO 2 , the effect of isotopic composition of plutonium in simulated reactor fuels was also investigated. For this purpose, both the water-cooled and fast-reactor fuels were prepared with plutonium containing 2% of 238 Pu by weight. The resulting oxides had about 6 times the specific activity of those prepared with 239 Pu. Groups of mice were killed at 1, 3, 6, 12 and 18 months after inhaling aerosols of the simulated reactor fuels. After 3 months, measurements of Pu retention in the lung showed no marked differences between materials. After 6 months, measurements of plutonium deposited in the liver and skeleton showed that mixed U/Pu oxides were more soluble in vivo than 239 PuO 2 . Their solubility was inversely related to their plutonium content. The addition of 238 Pu to the plutonium resulted in enhanced translocation of plutonium from the lung, in the cases of water-cooled reactor fuel by a factor of two. (author)

DOE plutonium disposition study: Pu consumption in ALWRs. Volume 2, Final report

Energy Technology Data Exchange (ETDEWEB)

1993-05-15

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

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

Energy Technology Data Exchange (ETDEWEB)

None, None

2017-11-07

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 solution 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.

Thorium utilization as a Pu-burner: proposal of Plutonium-Thorium Mixed Oxide (PT-MOX) Project

International Nuclear Information System (INIS)

Aizawa, Otohiko

2000-01-01

In this paper, a Pu-Th mixed oxide (PT-MOX) project is proposed for a thorium utilization and a plutonium burning. None of plutonium can be newly produced from PT-MOX fuel, and the plutonium mass of about 1 ton can be consumed with one reactor (total heavy metal assumed: 100 tons) for 1 year. In order to consume plutonium produced from usual Light Water Reactor, it should be better to operate one PT-MOX reactor for three to five Light Water Reactors. (author)

The ingestion of plutonium and americium by range cattle

International Nuclear Information System (INIS)

Blincoe, C.; Bohman, V.R.; Smith, D.D.

1981-01-01

The intake of plutonium and americium in the diet of cattle grazing on plutonium contaminated desert range was determined. Daily feed intake of the grazing animals was also determined so that the amount of nuclides ingested daily could be ascertained. Soil ingested by range cattle constituted the principal and possibly only source of ingested plutonium and americium and resulted in a daily intake of 3600-6600 pCi 238 Pu, 85,000-400,000 pCi 239 Pu, and 11,000-31,000 pCi 241 Am daily. Determining transuranic intake by direct measurement and from the composition and contamination of the diet gave identical results. (author)

Pathology associated with inhaled plutonium in beagles

International Nuclear Information System (INIS)

Dagle, G.E.; Park, J.F.; Weller, R.E.; Ragan, H.A.; Stevens, D.L.

1986-01-01

The pathology associated with the inhalation of plutonium was studied in beagle dogs given a single exposure to aerosols of 239 PuO 2 , 238 PuO 2 , or 239 Pu(NO 3 ) 4 . The temporal-spatial relationships between plutonium deposition and the development of lesions in dogs were evaluated up to 11 years, 8 years, or 5 years, respectively, after exposures, resulting in initial lung burdens ranging from ∼2 to ∼5500 nCi. Exposure of the lung to high dose levels produced a spectrum of progressively more severe morphological changes, ranging from radiation pneumonitis to fibrosis. Lung tumors occurred at exposure levels that did not result in early death from radiation pneumonitis or fibrosis. Bronchiolar-alveolar carcinomas, papillary adenocarcinomas, epidermoid carcinomas, and combined epidermoid and adenocarcinomas were observed. Sclerosing tracheobronchial lymphadenitis, radiation osteodystrophy, osteosarcoma, and hepatic adenomatous hyperplasia were the principal extrapulmonary lesions resulting from translocation of plutonium. 15 refs., 2 tabs

Toxicology of plutonium

International Nuclear Information System (INIS)

Bair, W.J.

1974-01-01

Data are reviewed from studies on the toxicity of Pu in experimental animals. Of the several plutonium isotopes, only 238 Pu and 239 Pu have been studied well. Sufficient results have been obtained to show that the behavior of 238 Pu in biological systems and the resulting biological effects cannot be precisely predicted from studies of 239 Pu. This probably applies also to other radiologically important plutonium isotopes which have half-lives ranging from 45 days to 10 7 years and decay by β-emission, electron capture, and spontaneous fission, as well as by emission of α-particles. All the biological effects of plutonium described in this review are attributed to alpha-particle radiation emitted by the plutonium. However, since plutonium is a chemically active heavy metal, one cannot ignore the possibility of chemical toxicity of the low-specific-activity isotopes, 239 Pu, 242 Pu, and 244 Pu. The preponderance of our knowledge of plutonium toxicology has come from short-term studies of relatively high dosage levels in several animal species. The consequences of high-level internal exposures can be predicted with confidence in experimental animals and probably also in man. However, considering the care with which plutonium is handled in the nuclear industry, a high-level contamination event is unlikely. Considerably less is known about the long-term effects of low levels of contamination. (250 references) (U.S.)

EPR study of sodium plutonyl acetate NaPuO2(CH3COO)3 and plutonium thenoyl trifluoroacetonate Pu(TTA)4: self-irradiation effects

International Nuclear Information System (INIS)

Krishnamurty, M.V.

1978-01-01

High energy radiations are emitted in the radioactive disintegration of plutonium isotopes. These radiations mainly consisting of α-particles interact with the surrounding ligands in the case of plutonium compounds. The ligand molecules undergo electronic excitation, ionization and fragmentation resulting in extensive radiation damage. Electron paramagnetic resonance technique is utilised to indentify and estimate these molecular products formed as a result of self-irradiation in the case of sodium plutonyl acetate, NaPuO 2 (CH 3 COO) 3 , and plutonium thenoyl trifluoroacetonate, Pu(TTA) 4 . The observed EPR spectra are interpreted to be due to acetate and thenoyl trifluoroacetonate radicals with the unpaired electron localized on oxygens of carboxyl group and carbonyl group, respectively. The efficiency parameter, eta, defined as the ratio of the number of paramagnetic species/defects to the total number of radioactive disintegrations has been determined to be 0.83 and 16.9 for the case of the acetate and thenoyl trifluoroacetonate, respectivly. (author)

Plutonium isotopes in the environment

International Nuclear Information System (INIS)

Holm, E.

1977-12-01

Determination of plutonium and americium by ion exchange and alpha-spectrometry. Deposition of global fall-out and accumulated area-content of 238 Pu, 239 Pu, 240 Pu, 241 Pu, 242 Pu and 241 Am in central Sweden (62.3 deg N, 12.4 deg E), by using the lichen species Cladonia alpestris as bioindicator. Retention and distribution of plutonium in carpets of lichen and soil. Transfer of plutonium from lichen to reindeer and man. Absorbed dose in reindeer and man from plutonium. Basic studies of plutonium and americium in the western Mediterranean surface waters, with emphases on particulate form of the transuranics. (author)

Reversed phase chromatographic behaviour of Pu (III), Pu (IV) and Pu (VI) in presence of α-hydroxyisobutyric acid

International Nuclear Information System (INIS)

Jaison, P.G.; Telmore, V.M.; Kumar, Pranaw

2016-01-01

Understanding the aqueous chemistry of plutonium is important in process conditions as well as in environmental conditions. Since plutonium possesses multiple oxidation states which can coexist in solution, a reliable method for the identification of these oxidation states is essential to understand its physical and chemical processes. The identification of plutonium oxidation states is conventionally determined through a series of liquid-liquid extraction procedures using selective extractants. Spectroscopic and laser based techniques also have been used for the identification of its oxidation state in solutions. Liquid chromatographic behavior of different oxidation states of Pu and other actinide ions is reported to correlate their retention behaviour with stability constants. Objective of the present work is to study the reversed phase chromatography behavior of the three oxidation states of plutonium viz. Pu(III), Pu(IV) and Pu(VI) in presence of á-hydroxyisobutyric acid (HIBA) as an eluent

Results of the international Pu-2000 exercise for plutonium isotopic composition measurements

International Nuclear Information System (INIS)

Morel, J.; Bickel, M.; Hill, C.; Verbruggen, A.

2004-01-01

An international comparison for plutonium isotopic composition measurement, known as the Pu-2000 exercise, was organized by the ESARDA NDA-WG (European Safeguards Research and Development Association, Working Group on Techniques and Standards for Non-Destructive Assay). The aim of this comparison was to test X- and γ-ray spectrometry methods over a large range of isotopic ratios. These methods are based on the complex analysis of several X- and γ-rays in the KX region of the plutonium spectrum and also in the 120-700 keV energy range. The results obtained by the participants with their corresponding uncertainties are presented in this document and compared to the declared values. The main conclusions of the work are also given. No important bias due to an inadequate knowledge of the nuclear data for plutonium isotopes was observed

Study of uranium - 20 Wt per cent plutonium-niobium alloys (1963); Etude d'alliages U-Pu-Nb a 20 pour cent en poids de plutonium (1963)

Energy Technology Data Exchange (ETDEWEB)

Abgrall, J; Barthelemy, P; Boucher, R [Commissariat a l' Energie Atomique, Fontenay-aux-Roses (France). Centre d' Etudes Nucleaires

1963-07-01

U-Pu-Nb alloys containing 20 wt per cent Pu and 10 - 20 - 30 - 40 - 50 or 60 wt per cent Nb have been studied principally to determine the feasibility of their use as fuel element. The fabrication, casting and homogenisation presented certain difficulties due specially to niobium. The transformation temperatures, thermal expansion coefficients and nature of phases have been determined by thermal analysis, dilatometry, micrography and X Rays diffraction. For similar compositions, U-Pu-Mo and U-Pu-Nb alloys have many common points concerning the presence of zeta phase (up to 40 wt per cent Nb), the coefficients of expansion, the good behaviour during thermal cycling and the good resistance to air oxidation in spite of zeta phase. In consequence, irradiation tests in EL{sub 3} reactor (Saclay) will be carried out in the near future. (authors) [French] Les alliages a 20 pour cent de plutonium, 10 - 20 - 30 - 40 - 50 - 60 pour cent de niobium et le complement en uranium ont ete etudies du point de vue de leur possibilite d'emploi comme combustible. Les problemes d'elaboration, de mise en forme et d'homogeneisation sont presentes. Ils sont relativement delicats. On a determine par analyse thermique, dilatometrie, micrographie et diffraction des rayons X les temperatures de transformation a l'etat solide, les coefficients de dilatation et la nature des phases. Pour des teneurs analogues, on retrouve de nombreux points communs avec les alliages U-Pu-Mo: presence de la phase zeta des U-Pu a temperature moyenne, coefficients de dilatation analogues, bonne tenue en cyclage thermique et bonne resistance a l'oxydation dans l'air malgre la presence de la phase zeta. Des essais d'irradiation dans EL{sub 3} vont etre entrepris. (auteurs)

An ab initio study of plutonium oxides surfaces; Etude ab initio des surfaces d'oxydes de Pu

Energy Technology Data Exchange (ETDEWEB)

Jomard, G.; Bottin, F.; Amadon, B

2007-07-01

By means of first-principles calculations, we have studied the atomic structure as well as the thermodynamic stability of various plutonium dioxide surfaces in function of their environment (in terms of oxygen partial pressure and temperature). All these simulations have been performed with the ABINIT code. It is well known that DFT fails to describe correctly plutonium-based materials since 5f electrons in such systems are strongly correlated. In order to go beyond DFT, we have treated PuO{sub 2} and {beta}-Pu{sub 2}O{sub 3} in a DFT+U framework. We show that the couple of parameters (U,J) that works well for pure Pu is also well designed for describing ground state (GS) properties of these two oxides. The major improvement with respect with DFT is that we are able to predict an insulating GS in agreement with experiments. The presence of a gap in the DOS (Density of States) of plutonium oxides should play a significant role in the predicted surface reactivity. However, performing DFT+U calculations on surfaces of plutonium oxide from scratch was too ambitious. That is why we decided, as a first step, to study the stability of the (100), (110) and (111) surfaces of PuO{sub 2} in a DFT-GGA framework. For each of these orientations, we considered various terminations. These ab initio results have been introduced in a thermodynamic model which allows us to predict the relative stability of the different terminations as a function of temperature and oxygen partial pressure (p{sub O{sub 2}}). We conclude that at room temperature and for p{sub O{sub 2}}{approx}10 atm., the polar O{sub 2}-(100) termination is favoured. The stabilization of such a polar stoichiometric surface is surprising and should be confirmed by DFT+U calculations before any final conclusion. (authors)

Study of uranium - 20 Wt per cent plutonium-niobium alloys (1963); Etude d'alliages U-Pu-Nb a 20 pour cent en poids de plutonium (1963)

Energy Technology Data Exchange (ETDEWEB)

Abgrall, J.; Barthelemy, P.; Boucher, R. [Commissariat a l' Energie Atomique, Fontenay-aux-Roses (France). Centre d' Etudes Nucleaires

1963-07-01

U-Pu-Nb alloys containing 20 wt per cent Pu and 10 - 20 - 30 - 40 - 50 or 60 wt per cent Nb have been studied principally to determine the feasibility of their use as fuel element. The fabrication, casting and homogenisation presented certain difficulties due specially to niobium. The transformation temperatures, thermal expansion coefficients and nature of phases have been determined by thermal analysis, dilatometry, micrography and X Rays diffraction. For similar compositions, U-Pu-Mo and U-Pu-Nb alloys have many common points concerning the presence of zeta phase (up to 40 wt per cent Nb), the coefficients of expansion, the good behaviour during thermal cycling and the good resistance to air oxidation in spite of zeta phase. In consequence, irradiation tests in EL{sub 3} reactor (Saclay) will be carried out in the near future. (authors) [French] Les alliages a 20 pour cent de plutonium, 10 - 20 - 30 - 40 - 50 - 60 pour cent de niobium et le complement en uranium ont ete etudies du point de vue de leur possibilite d'emploi comme combustible. Les problemes d'elaboration, de mise en forme et d'homogeneisation sont presentes. Ils sont relativement delicats. On a determine par analyse thermique, dilatometrie, micrographie et diffraction des rayons X les temperatures de transformation a l'etat solide, les coefficients de dilatation et la nature des phases. Pour des teneurs analogues, on retrouve de nombreux points communs avec les alliages U-Pu-Mo: presence de la phase zeta des U-Pu a temperature moyenne, coefficients de dilatation analogues, bonne tenue en cyclage thermique et bonne resistance a l'oxydation dans l'air malgre la presence de la phase zeta. Des essais d'irradiation dans EL{sub 3} vont etre entrepris. (auteurs)

The Transport of Close-In Fallout Plutonium in the Northwest Pacific Ocean: Tracing the Water Mass Movement Using {sup 240}Pu/{sup 239}Pu Atom Ratio

Energy Technology Data Exchange (ETDEWEB)

Lee, Sang-Han [Korea Research Institute of Standards and Science, Daejeon (Korea, Republic of); Hong, Gi-Hoon; Suk, Moon-Sik [Korea Ocean Research and Development Institute, Seoul (Korea, Republic of); Gastaud, J. [International Atomic Energy Agency, Marine Environment Laboratory (Monaco); La Rosa, J. [National Institute of Standards and Technology, Ionizing Radiation Division, Gaithersburg, Maryland (United States); Kim, Chul-Soo [Environmental Laboratories, International Atomic Energy Agency, Seibersdorf (Austria); Wyse, E. [New Brunswick Laboratory Argonne, IL (United States); Povinec, P. P. [Comenius University, Faculty of Mathematics and Physics, Bratislava (Slovakia)

2013-07-15

{sup 240}Pu/{sup 239}Pu atom ratios in seawater and surface sediment collected from the northwest (NW) Pacific Ocean from 1992 to 1997 were determined using ICP-sector field mass spectrometry (ICP-MS). In whole water columns, the atom ratios of {sup 240}Pu/{sup 239}Pu were higher than the global fallout ratio (0.18). It is noted that the atom ratios of {sup 240}Pu/2{sup 39}Pu in the seawater increase with depth. Such elevated {sup 240}Pu/{sup 239}Pu atom ratios indicate that the close-in fallout plutonium isotopes originating from the Pacific Proving Grounds (PPGs) due to the U.S. tests are prevailing in the seawater in the NW Pacific Ocean. However, the {sup 240}Pu/{sup 239}Pu atom ratios in the surface sediment from the NW Pacific Ocean varied with the sampling locations. As a consequence, this study will provide the information that the water mass along with the current plays a key role in driving the distribution of Pu and in transporting Pu from the PPGs to the far eastern marginal sea in the NW Pacific Ocean. (author)

Reactivity of the uranium (U(IV)/U(VI)) and the plutonium (Pu(III)/Pu(IV)) in nitric aqueous solution under ultrasound

International Nuclear Information System (INIS)

Venault, L.

1998-01-01

To minimize the volumes of solid waste and industrial effluents generated at the end of cycle, particularly in the spent nuclear fuel reprocessing industry, research is currently under way on so-called innovative processes, designed to induce chemical reactions without adding reagent to the media. Among these processes, the use of ultrasound can prove advantageous, and the purpose of this study is to assess accurately the potential for its application. In the present context, this work shows that the transmission of an ultrasonic wave in aqueous nitric acid solution leads to: the accumulation of nitrous acid in solution, until a steady-sate concentration is reached; the removal of nitrogen monoxide and nitrogen dioxide in the gas stream. The initial kinetics of the formation of HNO 2 in solution was quantified as a function of the nitric acid concentration and the ultrasound intensity. It was also shown than an excess of nitrous acid in nitric solution decomposes under the effect of ultrasound. It is also possible to accumulate hydrogen peroxide in solution during the ultrasonic irradiation of aqueous nitric acid solutions in the presence of a chemical species N 2 H 5 + , NH 2 SO 3 H...) which reacts rapidly with HNO 2 , preventing the reduction of H 2 O 2 by HNO 2 . The mechanisms of HNO 2 formation and decomposition, and the mechanism of H 2 O 2 formation during the ultrasonic irradiation of aqueous nitric acid solutions, are presented. Control of H 2 O 2 or HNO 2 in a nitric acid medium under the effect of an ultrasonic wave can be exploited to control redox reactions of uranium and plutonium ions, particularly with respect to the oxidation of U and Pu (U(IV)→ U(IV) or Pu(III) → Pu(IV)) and the reduction of Pu (Pu(IV)→ Pu(III). The redox behavior of uranium and plutonium ions in aqueous nitric solution subject to an ultrasonic flux is interpreted in term of effects induced on the reaction medium, and reveals the potential for using ultrasound to cause

Pu and Am determination in the environment method development

International Nuclear Information System (INIS)

Afonin, M.; Simonoff, M.; Donard, O.; Michel, H.; Ardisson, G.

2002-01-01

A few articles were published in the recent years regarding the application of ICP MS HR to the determination of ultratrace Pu in the environment. Si removal was not applied in recent publications. It is well known from marine biology that some microorganisms use Si derivatives in their metabolism. This implies that important amounts of Pu will not be dissolved and instead will rest in the solid residue. In our work we chose a combination of methods from EML-300 Handbook: Pu-02-RC Plutonium in Soil Samples, Pu-03-RC Plutonium in Soil Residue - Total Dissolution Method, Pu-11-RC Plutonium Purification - Ion Exchange Technique, Pu-12-RC Plutonium and/or Americium in Soil or Sediments. A high resolution inductively coupled plasma mass spectrometric method was developed for the determination of Am and the 240 Pu/ 239 Pu isotope ratio. The total plutonium concentrations ( 239+240 Pu) measured in environmental samples by this method were in good agreement with recommended data obtained from alpha-spectrometry. A reduction in the time of analysis over 33% was achieved

Plutonium separation by reduction stripping. Application to processing of mixed oxide (U,Pu)O2 fuel fabrication wastes

International Nuclear Information System (INIS)

Arnal, Thierry; Cousinou, Gerard; Ganivet, Michel.

1978-11-01

A procedure is described for separating plutonium from a uranium VI and plutonium IV mixture contained in an organic phase (tributyl phosphate diluted in dodecane). This separation is obtained by extracting the plutonium III using two organic reducers: hydrazine and paraminophenol. Paraminophenol has excellent reducing qualities, similar to those of ferrous sulphamate, but has the added advantage of not contaminating extracted plutonium. This procedure is currently used in processing production wastes from mixed oxide (U,Pu)O 2 fuels; the installation using this procedure is described in detail in this paper. Operating results show the remarkable efficiency of this procedure: the separated plutonium and uranium mass flows have been increased to 185 and 350 g.h -1 respectively; the uranium contains less than 0.1 ppm of plutonium on completion of the purification cycle [fr

Plutonium spectrophotometric analysis

International Nuclear Information System (INIS)

Esteban, A.; Cassaniti, P.; Orosco, E.H.

1990-01-01

Plutonium ions in solution have absorption spectra so different that it is possible to use them for analytical purposes. Detailed studies have been performed in nitric solutions. Some very convenient methods for the determination of plutonium and its oxidation states, especially the ratios Pu(III):Pu(IV) and Pu(IV):Pu(VI) in a mixture of both, have been developed. These methods are described in this paper, including: a) Absorption spectra for plutonium (III), (IV), (VI) and mixtures. b) Relative extinction coefficients for the above mentioned species. c) Dependences of the relative extinction coefficients on the nitric acid concentration and the plutonium VI deviation from the Beer-Lambert law. The developed methods are simple and rapid and then, suitable in process control. Accuracy is improved when relative absorbance measurements are performed or controlled the variables which have effect on the spectra and extinction coefficients. (Author) [es

Plutonium (Pu)

International Nuclear Information System (INIS)

2002-01-01

This pedagogical document presents the properties and uses of plutonium: where does it come from, the history of its discovery, its uses and energy content, its recycling and reuse in MOX fuels, its half-life, toxicity and presence in the environment. (J.S.)

Reaction of plutonium with water kinetic and equilibrium behavior of binary and ternary phases in the Pu + O + H system

International Nuclear Information System (INIS)

Haschke, J.M.; Hodges, A.E. III; Bixby, G.E.; Lucas, R.L.

1983-01-01

The kinetic and equilibrium behavior of the Pu + O + H system has been studied by measuring the production of hydrogen gas formed by a sequence of hydrolysis reactions. The kinetic dependence of the Pu + H 2 O reaction on salt concentration and temperature has been defined. The metal is quantitatively converted to a fine black powder which has been identified as plutonium monoxide monohydride, PuOH. Other hydrolysis products formed in aqueous media include a second oxide hydride, Pu 7 O 9 H 3 , and the oxides Pu 2 O 3 , Pu 7 O 12 , Pu 9 O 16 , Pu 10 O 18 , Pu 12 O 22 , and PuO 2 . Thermal decomposition products of PuOH include Pu 2 O 2 H and PuO. A tentative phase diagram for Pu + O + H is presented and structural relationships of the oxide hydrides and oxides are discussed. 10 figures, 5 tables

Assessment of 238Pu and 239+240Pu, in marine sediments of the oceans Atlantic and Pacific of Guatemala

International Nuclear Information System (INIS)

Mendez Ochaita, L.

2000-01-01

In this investigation samples of marine sediments were taken from 14 places representatives of the oceans coast of Guatemala. For the assesment of 238 Pu and 239+240 Pu in sediments a radiochemical method was used to mineralize sediments and by ionic interchange it was separated from other elements, after that an electrodeposition of plutonium was made in metallic discs. The radioactivity of plutonium was measured by alpha spectrometry system and the alpha spectrums were obtained. The levels of plutonium are not higher than other countries that shown contamination. The contamination of isotope of 239+240 Pu is higher than 238 Pu and the contamination by two isotopes of plutonium is higher in the Atlantic than the Pacific ocean

Reactivity of the uranium (U(IV)/U(VI)) and the plutonium (Pu(III)/Pu(IV)) in nitric aqueous solution under ultrasound; De l'influence des ultrasons sur la reactivite de l'uranium (U(IV)/U(VI)) et du plutonium (PU(III)/PU(IV)) en solution aqueuse nitrique

Energy Technology Data Exchange (ETDEWEB)

Venault, L

1998-07-01

To minimize the volumes of solid waste and industrial effluents generated at the end of cycle, particularly in the spent nuclear fuel reprocessing industry, research is currently under way on so-called innovative processes, designed to induce chemical reactions without adding reagent to the media. Among these processes, the use of ultrasound can prove advantageous, and the purpose of this study is to assess accurately the potential for its application. In the present context, this work shows that the transmission of an ultrasonic wave in aqueous nitric acid solution leads to: the accumulation of nitrous acid in solution, until a steady-sate concentration is reached; the removal of nitrogen monoxide and nitrogen dioxide in the gas stream. The initial kinetics of the formation of HNO{sub 2} in solution was quantified as a function of the nitric acid concentration and the ultrasound intensity. It was also shown than an excess of nitrous acid in nitric solution decomposes under the effect of ultrasound. It is also possible to accumulate hydrogen peroxide in solution during the ultrasonic irradiation of aqueous nitric acid solutions in the presence of a chemical species (N{sub 2}H{sub 5}{sup +}, NH{sub 2}SO{sub 3}H...) which reacts rapidly with HNO{sub 2}, preventing the reduction of H{sub 2}O{sub 2} by HNO{sub 2}. The mechanisms of HNO{sub 2} formation and decomposition, and the mechanism of H{sub 2}O{sub 2} formation during the ultrasonic irradiation of aqueous nitric acid solutions, are presented. Control of H{sub 2}O{sub 2} or HNO{sub 2} in a nitric acid medium under the effect of an ultrasonic wave can be exploited to control redox reactions of uranium and plutonium ions, particularly with respect to the oxidation of U and Pu (U(IV){yields} U(IV) or Pu(III) {yields} Pu(IV)) and the reduction of Pu (Pu(IV){yields} Pu(III). The redox behavior of uranium and plutonium ions in aqueous nitric solution subject to an ultrasonic flux is interpreted in term of effects

Plutonium speciation affected by environmental bacteria

International Nuclear Information System (INIS)

Neu, M.P.; Icopini, G.A.; Boukhalfa, H.

2005-01-01

Plutonium has no known biological utility, yet it has the potential to interact with bacterial cellular and extracellular structures that contain metal-binding groups, to interfere with the uptake and utilization of essential elements, and to alter cell metabolism. These interactions can transform plutonium from its most common forms, solid, mineral-adsorbed, or colloidal Pu(IV), to a variety of biogeochemical species that have much different physico-chemical properties. Organic acids that are extruded products of cell metabolism can solubilize plutonium and then enhance its environmental mobility, or in some cases facilitate plutonium transfer into cells. Phosphate- and carboxylate-rich polymers associated with cell walls can bind plutonium to form mobile biocolloids or Pu-laden biofilm/mineral solids. Bacterial membranes, proteins or redox agents can produce strongly reducing electrochemical zones and generate molecular Pu(III/IV) species or oxide particles. Alternatively, they can oxidize plutonium to form soluble Pu(V) or Pu(VI) complexes. This paper reviews research on plutonium-bacteria interactions and closely related studies on the biotransformation of uranium and other metals. (orig.)

Aqueous Solution Chemistry of Plutonium

Energy Technology Data Exchange (ETDEWEB)

Clark, David L. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

2014-01-28

Things I have learned working with plutonium: Chemistry of plutonium is complex; Redox equilibria make Pu solution chemistry particularly challenging in the absence of complexing ligands; Understanding this behavior is key to successful Pu chemistry experiments; There is no suitable chemical analog for plutonium.

Absorption of plutonium from the gastrointestinal tract of rats and guinea pigs after ingestion of alfalfa containing 238Pu

International Nuclear Information System (INIS)

Sullivan, M.F.; Garland, T.R.; Cataldo, D.A.; Wildung, R.E.; Drucker, H.

1980-01-01

The absorption of inorganic compounds of plutonium from the GI tract is so low that ingestion of this radionuclide does not appear to present a major health hazard. However, combining this actinide with organic compounds, such as chelating agents, can markedly increase absorption. Similarly, when Pu or other long-lived nuclides are released into the environment and incorporated into plants they may be complexed with naturally occurring organic ligands. It might then be possible for these nuclides to more effectively enter into the food chain. To test for this possibility, alfalfa was grown in the presence of inorganic plutonium, the plant tissue was fed to animals, and a comparison was made of the absorption from the gut of this plant-incorporated Pu relative to inorganic Pu. The results of these experiments, while not conclusive, do support the view that information is needed on food chain behavior of the actinide nuclear fuels as a precaution against exceeding dose limits. (author)

Characterization of a Pu-bearing zirconolite-rich synroc

International Nuclear Information System (INIS)

Buck, E.C.; Ebbinghaus, B.; Bakel, A.J.; Bates, J.K.

1996-01-01

A titanate-based ceramic waste form, rich in phases structurally related to zirconolite (CaZrTi 2 O 7 ), is being developed as a possible method for immobilizing excess plutonium from dismantled nuclear weapons. As part of this program, Lawrence Livermore National Laboratory (LLNL) produced several ceramics that were then characterized at Argonne National Laboratory (ANL). The plutonium- loaded ceramic was found to contain a Pu-Gd zirconolite phase but also contained plutonium titanates, Gd-polymignyte, and a series of other phases. In addition, much of the Pu was remained as PuO 2- x . The Pu oxidation state in the zirconolite was determined to be mainly Pu 4+ , although some Pu 3+ was believed to be present

Study of the Effect of (U0.8Pu0.2O2 Uranium–Plutonium Mixed Fuel Fission Products on a Living Organism

Directory of Open Access Journals (Sweden)

Ayagoz Baimukhanova

2016-08-01

Full Text Available The article describes the results of experiments conducted on pigs to determine the effect of plutonium, which is the most radiotoxic and highly active element in the range of mixed fuel (U0.8Pu0.2O2 fission products, on living organisms. The results will allow empirical prediction of the emergency plutonium radiation dose for various organs and tissues of humans in case of an accident in a reactor running on mixed fuel (U0.8Pu0.2O2.

The application of data derived from autoradiographic studies with 241Pu in the formulation of a bone dosimetric model for 239Pu

International Nuclear Information System (INIS)

Priest, N.D.; Hunt, B.W.

1979-01-01

Recently a dosimetric model for 239 Pu in bone has been published which in conjunction with the general ICRP dosimetric model for actinides is used to calculate annual limits of intake for 239 Pu. This model allows for the burial of plutonium in bone, for the recycling of plutonium within the skeleton and for the retention of plutonium in the bone marrow. The model was based upon published descriptions of the distribution and redistribution patterns of plutonium in bone and on evidence obtained from autoradiographic studies of bone from animals injected with 241 Pu. The experiments with 241 Pu demonstrated the initial uptake of plutonium by bone surfaces. As a result of the growth and drift processes much of this plutonium became either buried in the bone or was retained within macrophages in the bone marrow. (author)

Computing and physical methods to calculate Pu

International Nuclear Information System (INIS)

Mohamed, Ashraf Elsayed Mohamed

2013-01-01

Main limitations due to the enhancement of the plutonium content are related to the coolant void effect as the spectrum becomes faster, the neutron flux in the thermal region tends towards zero and is concentrated in the region from 10 Ke to 1 MeV. Thus, all captures by 240 Pu and 242 Pu in the thermal and epithermal resonance disappear and the 240 Pu and 242 Pu contributions to the void effect became positive. The higher the Pu content and the poorer the Pu quality, the larger the void effect. The core control in nominal or transient conditions Pu enrichment leads to a decrease in (B eff.), the efficiency of soluble boron and control rods. Also, the Doppler effect tends to decrease when Pu replaces U, so, that in case of transients the core could diverge again if the control is not effective enough. As for the voiding effect, the plutonium degradation and the 240 Pu and 242 Pu accumulation after multiple recycling lead to spectrum hardening and to a decrease in control. One solution would be to use enriched boron in soluble boron and shutdown rods. In this paper, I discuss and show the advanced computing and physical methods to calculate Pu inside the nuclear reactors and glovebox and the different solutions to be used to overcome the difficulties that effect, on safety parameters and on reactor performance, and analysis the consequences of plutonium management on the whole fuel cycle like Raw materials savings, fraction of nuclear electric power involved in the Pu management. All through two types of scenario, one involving a low fraction of the nuclear park dedicated to plutonium management, the other involving a dilution of the plutonium in all the nuclear park. (author)

Base case Pu-nitrate to Pu-oxide conversion plant

International Nuclear Information System (INIS)

1978-10-01

This paper explains that the plutonium recovered in the course of reprocessing spent fuel is obtained in the form of plutonium nitrate, whereas PuO 2 is required for the fabrication of fuel rods. The reference conversion plant described in the paper converts plutonium nitrate into plutonium dioxide powder by precipitation with oxalic acid followed by calcination. The paper also describes the main features of the safety, maintenance and safeguards philosophy used in its design

Studies of plutonium-iron and uranium-plutonium-iron alloys; Etudes d'alliages plutonium-fer et d'alliages uranium-plutonium-fer

Energy Technology Data Exchange (ETDEWEB)

Avivi, Ehud [Commissariat a l' Energie Atomique, Fontenay-aux-Roses (France). Centre d' Etudes Nucleaires

1964-01-15

We study the plutonium-iron system, by means of dilatometry, X rays and metallography, especially in the domain between PuFe{sub 2} and Fe. We determine the solubilities of Fe in PuFe{sub 2} and of Pu in Fe. We show the presence of an hexagonal PuFe{sub 2} phase and we propose a modification in the Pu-Fe phase diagram. Some low iron concentration U-Pu-Fe alloys have also been investigated. We characterise the different phases. We confirm that adding some iron lowers the quantity of the zeta U-Pu phase. We emphasize some characteristics of the alloys having the global concentration (U, Pu){sub 6} Fe. (authors) [French] On etudie par dilatometrie, rayons X et micrographie le systeme plutonium-fer, principalement dans la region comprise entre PuFe{sub 2} et Fe, On determine les solubilites du fer dans PuFe{sub 2}, et de Pu dans Fe. On met en evidence une phase PuFe{sub 2} hexagonale et on propose une modification du diagramme d'equilibre Pu-Fe. Certains alliages U-Pu-Fe a faibles concentrations en fer sont egalement etudies. On caracterise les phases en presence. On confirme que l'addition de fer diminue rapidement la quantite de phase U-Pu zeta. Enfin on revele certaines caracteristiques des alliages de composition globale (U, Pu){sub 6} Fe. (auteurs)

Transuranic and tracer simulant resuspension. [/sup 238/Pu, /sup 239/Pu, /sup 240/Pu

Energy Technology Data Exchange (ETDEWEB)

Sehmel, G. A.

1977-07-01

Plutonium resuspension results are summarized for experiments conducted at Rocky Flats, onsite on the Hanford reservation, and for winds blowing from offsite onto the Hanford reservation near the Prosser barricade boundary. In each case, plutonium resuspension was shown by increased airborne plutonium concentrations as a function of either wind speed or as compared to fallout levels. All measured airborne concentrations were below maximum permissible concentrations (MPC). Both plutonium and cesium concentrations on airborne soil were normalized by the quantity of airborne soil sampled. Airborne radionuclide concentrations in ..mu..Ci/g were related to published values for radionuclide concentrations on surface soils. For this ratio of radionuclide concentration per gram on airborne soil divided by that for ground surface soil, there are eight orders of magnitude uncertainty from 10/sup -4/ to 10/sup 4/. Horizontal plutonium fluxes on airborne nonrespirable soils at all three sites were bracketed within the same three to four orders of magnitude from 10/sup -7/ to 10/sup -3/ ..mu..Ci/(m/sup 2/ day) for plutonium-239 and 10/sup -8/ to 10/sup -5/ ..mu..Ci/(m/sup 2/ day) for plutonium-238. These are the entire experimental base for nonrespirable airborne plutonium transport. Airborne respirable plutonium-239 concentrations increased with wind speed for a southeast wind direction coming from offsite near the Hanford reservation Prosser barricade. Airborne plutonium fluxes on nonrespirable particles had isotopic ratios, /sup 240/Pu//sup 239 +240/Pu, similar to weapons grade plutonium rather than fallout plutonium. Resuspension rates were summarized for controlled inert particle tracer simulant experiments. Wind resuspension rates for tracers increased with wind speed to about the fifth power.

239, 240, 241Pu fingerprinting of plutonium in western US soils using ICPMS: solution and laser ablation measurements

International Nuclear Information System (INIS)

Cizdziel, James V.; Ketterer, Michael E.; Farmer, Dennis; Faller, Scott H.; Hodge, Vernon F.

2008-01-01

Sector field inductively coupled plasma mass spectrometry (SF-ICPMS) has been used with analysis of solution samples and laser ablation (LA) of electrodeposited alpha sources to characterize plutonium activities and atom ratios prevalent in the western USA. A large set of surface soils and attic dusts were previously collected from many locations in the states of Nevada, Utah, Arizona, and Colorado; specific samples were analyzed herein to characterize the relative contributions of stratospheric fallout vs. Nevada Test Site (NTS) plutonium. This study illustrates two different ICPMS-based analytical strategies that are successful in fingerprinting Pu in environmental soils and dusts. Two specific datasets have been generated: (1) soils are leached with HNO 3 -HCl, converted into electrodeposited alpha sources, counted by alpha spectrometry, then re-analyzed using laser ablation SF-ICPMS; (2) samples are completely dissolved by treatment with HNO 3 -HF-H 3 BO 3 , Pu fractions are prepared by extraction chromatography, and analyzed by SF-ICPMS. Optimal laser ablation and ICPMS conditions were determined for the re-analysis of archived alpha spectrometry ''planchette'' sources. The best ablation results were obtained using a large spot size (200 μm), a defocused beam, full repetition rate (20 Hz) and scan rate (200 μm s -1 ); LA-ICPMS data were collected with a rapid electrostatic sector scanning experiment. Less than 10% of the electroplated surface area is consumed in the LA-ICPMS analysis, which would allow for multiple re-analyses. Excellent agreement was found between 239+240 Pu activities determined by LA-ICPMS vs. activity results obtained by alpha spectrometry for the same samples ten years earlier. LA-ICPMS atom ratios for 240 Pu/ 239 Pu and 241 Pu/ 239 Pu range from 0.038-0.132 and 0.00034-0.00168, respectively, and plot along a two-component mixing line ( 241 Pu/ 239 Pu = 0.013 [ 240 Pu/ 239 Pu] - 0.0001; r 2 = 0.971) with NTS and global fallout end

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

Science.gov (United States)

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

2014-08-11

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

DFT and two-dimensional correlation analysis methods for evaluating the Pu3+–Pu4+ electronic transition of plutonium-doped zircon

International Nuclear Information System (INIS)

Bian, Liang; Dong, Fa-qin; Song, Mian-xin; Dong, Hai-liang; Li, Wei-Min; Duan, Tao; Xu, Jin-bao; Zhang, Xiao-yan

2015-01-01

Highlights: • Effect of Pu f-shell electron on the electronic property of zircon is calculated via DFT and 2D-CA techniques. • Reasons of Pu f-shell electron influencing on electronic properties are systematically discussed. • Phase transitions are found at two point 2.8 mol% and 7.5 mol%. - Abstract: Understanding how plutonium (Pu) doping affects the crystalline zircon structure is very important for risk management. However, so far, there have been only a very limited number of reports of the quantitative simulation of the effects of the Pu charge and concentration on the phase transition. In this study, we used density functional theory (DFT), virtual crystal approximation (VCA), and two-dimensional correlation analysis (2D-CA) techniques to calculate the origins of the structural and electronic transitions of Zr 1−c Pu c SiO 4 over a wide range of Pu doping concentrations (c = 0–10 mol%). The calculations indicated that the low-angular-momentum Pu-f xy -shell electron excites an inner-shell O-2s 2 orbital to create an oxygen defect (V O-s ) below c = 2.8 mol%. This oxygen defect then captures a low-angular-momentum Zr-5p 6 5s 2 electron to form an sp hybrid orbital, which exhibits a stable phase structure. When c > 2.8 mol%, each accumulated V O-p defect captures a high-angular-momentum Zr-4d z electron and two Si-p z electrons to create delocalized Si 4+ → Si 2+ charge disproportionation. Therefore, we suggest that the optimal amount of Pu cannot exceed 7.5 mol% because of the formation of a mixture of ZrO 8 polyhedral and SiO 4 tetrahedral phases with the orientation (10-1). This study offers new perspective on the development of highly stable zircon-based solid solution materials

Plutonium-236 traces determination in plutonium-238 by α spectrometry

International Nuclear Information System (INIS)

Acena, M.L.; Pottier, R.; Berger, R.

1969-01-01

Two methods are described in this report for the determination of plutonium-236 traces in plutonium-238 by a spectrometry using semi-conductor detectors. The first method involves a direct comparison of the areas under the peaks of the α spectra of plutonium-236 and plutonium-238. The electrolytic preparation of the sources is carried out after preliminary purification of the plutonium. The second method makes it possible to determine the 236 Pu/ 238 Pu ratio by comparing the areas of the α peaks of uranium-232 and uranium-234, which are the decay products of the two plutonium isotopes respectively. The uranium in the source, also deposited by electrolysis, is separated from a 1 mg amount of plutonium either by a T.L.A. extraction, or by the use of ion-exchange resins. The report ends with a discussion of the results obtained with plutonium of two different origins. (authors) [fr

Anaerobic Biotransformation and Mobility of Pu and Pu-EDTA

International Nuclear Information System (INIS)

Bolton, H. Jr.; Rai, D.; Xun, L.

2005-01-01

The complexation of radionuclides (e.g., plutonium (Pu) and 60 Co) by codisposed ethylenediaminetetraacetate (EDTA) has enhanced their transport in sediments at DOE sites. Our previous NABIR research investigated the aerobic biodegradation and biogeochemistry of Pu(IV)-EDTA. Plutonium(IV) forms stable complexes with EDTA under aerobic conditions and an aerobic EDTA degrading bacterium can degrade EDTA in the presence of Pu and decrease Pu mobility. However, our recent studies indicate that while Pu(IV)-EDTA is stable in simple aqueous systems, it is not stable in the presence of relatively soluble Fe(III) compounds (i.e., Fe(OH) 3 (s)--2-line ferrihydrite). Since most DOE sites have Fe(III) containing sediments, Pu(IV) in likely not the mobile form of Pu-EDTA in groundwater. The only other Pu-EDTA complex stable in groundwater relevant to DOE sites would be Pu(III)-EDTA, which only forms under anaerobic conditions. Research is therefore needed in this brand new project to investigate the biotransformation of Pu and Pu-EDTA under anaerobic conditions. The biotransformation of Pu and Pu-EDTA under various anaerobic regimes is poorly understood including the reduction kinetics of Pu(IV) to Pu(III) from soluble (Pu(IV)-EDTA) and insoluble Pu(IV) as PuO2(am) by metal reducing bacteria, the redox conditions required for this reduction, the strength of the Pu(III)-EDTA complex, how the Pu(III)-EDTA complex competes with other dominant anoxic soluble metals (e.g., Fe(II)), and the oxidation kinetics of Pu(III)-EDTA. Finally, the formation of a stable soluble Pu(III)-EDTA complex under anaerobic conditions would require degradation of the EDTA complex to limit Pu(III) transport in geologic environments. Anaerobic EDTA degrading microorganisms have not been isolated. These knowledge gaps preclude the development of a mechanistic understanding of how anaerobic conditions will influence Pu and Pu-EDTA fate and transport to assess, model, and design approaches to stop Pu

The plutonium-oxygen and uranium-plutonium-oxygen systems: A thermochemical assessment

International Nuclear Information System (INIS)

1967-01-01

The report of a panel of experts convened by the IAEA in Vienna in March 1964. It reviews the structural and thermodynamic data for the Pu-O and U-Pu-O systems and presents the conclusions of the panel. The report gives information on preparation, phase diagrams, thermodynamic and vaporization behaviour of plutonium oxides, uranium-plutonium oxides and PuO 2 -MeO x (Me=Be, Mg, Al, Si, W, Th, Eu, Zr, Ce) systems. 167 refs, 27 figs, 17 tabs

Gamma-ray isotopic ratio measurements for the plutonium inventory verification program

International Nuclear Information System (INIS)

Lemming, J.F.; Haas, F.X.; Jarvis, J.Y.

1976-01-01

The Plutonium Inventory Verification Program at Mound Laboratory provides a nondestructive means of assaying bulk plutonium-bearing material. The assay is performed by combining the calorimetrically determined heat output of the sample and the relative abundances of the heat-producing isotopes. This report describes the method used for the nondestructive determination of plutonium-238, -240, -241 and americium-241 relative to plutonium-239 using gamma-ray spectroscopy for 93 percent plutonium-239 material. Comparison of chemical data on aliquots of samples to the nondestructive data shows accuracies of +-7 percent for 238 Pu/ 239 Pu, +-15 percent for 240 Pu/ 239 Pu, +- 3 percent for 241 Pu/ 239 Pu, and +-7 percent for 241 Am/ 239 Pu

Biological behaviour of plutonium inhaled by baboons as plutonium n-tributylphosphate complex. Comparison with ICRP models

International Nuclear Information System (INIS)

Metivier, H.; Duserre, C.; Rateau, G.; Legendre, N.; Masse, R.; Piechowski, J.; Menoux, B.

1989-01-01

In order to devise a model capable of calculating committed doses for workers contaminated by inhalation of plutonium tributylphosphate complex during reprocessing, we investigated the biokinetics of plutonium in baboons after inhalation of this chemical form. The animals were killed 0.6, 3, 15, 30, 90 and 365 days post inhalation. Urine and faeces were collected daily. After killing, the main organs were collected for chemical analysis. In order to improve our knowledge of the behaviour of systemic plutonium, three baboons were given an intravenous injection of Pu-TBP and were respectively killed 2, 30 and 365 days post injection. We observed that Pu-TBP could be classified as a W compound, with a half-time for lung clearance of 150 days. Urinary Pu excretion was 3 times higher than was expected from Durbin's model, suggesting that Pu introduced as Pu-TBP, is extremely mobile, and that the complex formed with blood proteins differs from the one formed after inhalation of plutonium nitrate. (author)

Plutonium gastrointestinal absorption by adults baboons

International Nuclear Information System (INIS)

Lataillade, G.; Madic, C.; Willemot, J.M.; Germain, P.; Colle, C.; Metivier, H.

1991-01-01

Gastrointestinal absorption of plutonium was investigated in baboons after ingestion of plutonium solution (oxidation states III; IV; V; VI), and plutonium incorporated in soya bean and winkles. We studied the effects of oxidation state and ingested mass for masses ranging from 0.35 μg to 51.6 x 10 +3 μg (4 x 10 -2 to 7776 μg of plutonium per kg of body weight). No clear increase in plutonium retention was shown for concentrations of plutonium smaller than 1 μg/kg. From 1 μg/kg to 1 mg/kg no effects of mass or oxidation state was observed and the mean fractional retention value was 10 -4 . For ingested masses higher than 1 mg/kg the fractional retention values respectively increased for Pu(V) and Pu(III) to (0.9 + 0.2) x 10 -2 and (7.4 + 4.1) x 10 -4 of the ingested mass. This increase might be due to the weak hydrolysis of these oxidation states which would increase gastrointestinal absorption by decrease of hydroxide formation. The fraction of plutonium retained after ingestion of soya bean was (3.0 + 0.5) x 10 -4 about 3 fold higher than the value for 238 Pu nitrate solution. No clear increase in plutonium retention was shown after ingestion of winkles containing 238 Pu. In conclusion, except for high masses of ingested Pu, the retention of which could reach 1% of the ingested dose, our results show that the gastrointestinal transfer factor of 10 -4 proposed by ICRP for gastrointestinal absorption of soluble form of Pu is acceptable, but 10 -3 would provide better safety margin [fr

Plutonium oxide dissolution

International Nuclear Information System (INIS)

Gray, J.H.

1992-01-01

Several processing options for dissolving plutonium oxide (PuO 2 ) from high-fired materials have been studied. The scoping studies performed on these options were focused on PuO 2 typically generated by burning plutonium metal and PuO 2 produced during incineration of alpha contaminated waste. At least two processing options remain applicable for dissolving high-fired PuO 2 in canyon dissolvers. The options involve solid solution formation of PuO 2 With uranium oxide (UO 2 ) and alloying incinerator ash with aluminum. An oxidative dissolution process involving nitric acid solutions containing a strong oxidizing agent, such as cerium (IV), was neither proven nor rejected. This uncertainty was due to difficulty in regenerating cerium (IV) ions during dissolution. However, recent work on silver-catalyzed dissolution of PuO 2 with persulfate has demonstrated that persulfate ions regenerate silver (II). Use of persulfate to regenerate cerium (IV) or bismuth (V) ions during dissolution of PuO 2 materials may warrant further study

Plutonium in coniferous forests

International Nuclear Information System (INIS)

Rantavaara, A.; Kostiainen, E.

2002-01-01

Our aim was to study the uptake of plutonium by trees, undervegetation and some wild foods. The ratio of 238 Pu/ 239,240 Pu in soil samples was determined for comparisons of the fallout origin. In twelve years the Chernobyl derived plutonium has not reached the mineral soil. This refers to a very slow downward migration in podsolic soil. The study confirmed also the low Pu uptake by vegetation and an insignificant contribution to human doses through wild foods. (au)

Process for recovery of plutonium from fabrication residues of mixed fuels consisting of uranium oxide and plutonium oxide

International Nuclear Information System (INIS)

Heremanns, R.H.; Vandersteene, J.J.

1983-01-01

The invention concerns a process for recovery of plutonium from fabrication residues of mixed fuels consisting of uranium oxide and plutonium oxide in the form of PuO 2 . Mixed fuels consisting of uranium oxide and plutonium oxide are being used more and more. The plants which prepare these mixed fuels have around 5% of the total mass of fuels as fabrication residue, either as waste or scrap. In view of the high cost of plutonium, it has been attempted to recover this plutonium from the fabrication residues by a process having a purchase price lower than the price of plutonium. The problem is essentially to separate the plutonium, the uranium and the impurities. The residues are fluorinated, the UF 6 and PuF 6 obtained are separated by selective absorption of the PuF 6 on NaF at a temperature of at least 400 0 C, the complex obtained by this absorption is dissolved in nitric acid solution, the plutonium is precipitated in the form of plutonium oxalate by adding oxalic acid, and the precipitated plutonium oxalate is calcined

Light water breeder reactor using a uranium-plutonium cycle

International Nuclear Information System (INIS)

Radkowsky, A.; Chen, R.

1990-01-01

This patent describes a light water receptor (LWR) for breeding fissile material using a uranium-plutonium cycle. It comprises: a prebreeder section having plutonium fuel containing a Pu-241 component, the prebreeder section being operable to produce enriched plutonium having an increased Pu-241 component; and a breeder section for receiving the enriched plutonium from the prebreeder section, the breeder section being operable for breeding fissile material from the enriched plutonium fuel. This patent describes a method of operating a light water nuclear reactor (LWR) for breeding fissile material using a uranium-plutonium cycle. It comprises: operating the prebreeder to produce enriched plutonium fuel having an increased Pu-241 component; fueling a breeder section with the enriched plutonium fuel to breed the fissile material

Perturbation in the 240Pu/239Pu global fallout ratio in local sediment following the nuclear accidents at Thule (Greenland) and Palomares (Spain)

International Nuclear Information System (INIS)

Mitchell, P.I.; Vintro, L.L.; Gasco, C.; Sanchez-Cabeza, J.A.

1995-01-01

It is well established that the main source of the plutonium found in marine sediments throughout the Northern Hemisphere is global stratospheric fallout, characterized by a typical 240 Pu/ 239 Pu atom ratio of ∼0.18. Measurements of perturbations in this ratio at various sites which had been subjected to close-in fallout, mainly from surface-based testing, has confirmed the feasibility of using this ratio to distinguish plutonium from different fallout sources. In the present study, the 240 Pu/ 239 Pu ratio has been examined in samples of sediment collected at Thule (Greenland) and Palomares (Spain), where accidents involving the release and dispersion of plutonium from fractured nuclear weapons occurred in 1968 and 1966, respectively. The 240 Pu/ 239 Pu ratio was measured by high-resolution alpha spectrometry and spectral deconvolution. The analytical results showed that at Thule the mean 240 Pu/ 239 Pu atom ratio was 0.033±0.004, while at Palomares the equivalent ratio appeared to be significantly higher at 0.056±0.003. Both ratios are consistent with those reported for soils samples at the Nevada site and Nagasaki, and are clearly indicative of weapons-grade plutonium. 27 refs., 1 fig., 2 tabs

Phonon anharmonicity and Gruneisen parameters of alpha-plutonium

International Nuclear Information System (INIS)

Filanovich, A.N.; Povzner, A.A.

2015-01-01

A self-consistent thermodynamic model of alpha-phase of plutonium is constructed. The calculations of thermal and elastic properties of α-Pu, carried out within this model, demonstrate that anomalously strong temperature dependence of the bulk modulus and unusually high value of the coefficient of thermal expansion of α-Pu are caused by its strong lattice anharmonicity. The isothermal and isobaric Gruneisen parameters of α-Pu and δ-Pu Pu_0_._9_6Ga_0_._0_4 are calculated. It is shown that wide spread of the values of Gruneisen parameter of α-Pu, obtained previously from different experimental data, is explained by the dependence of Gruneisen parameter of α-Pu on temperature. - Highlights: • A self-consistent thermodynamic model of alpha-plutonium is developed. • Thermal and elastic properties of alpha-plutonium are calculated. • The reason of spread in the values of Gruneisen parameter of alpha-Pu is established. • Different types of phonon anharmonicity in alpha-Pu and delta-Pu are revealed.

Solubility of plutonium dioxide aerosols, in vitro

International Nuclear Information System (INIS)

Newton, G.J.; Kanapilly, G.M.

1976-01-01

Solubility of plutonium aerosols is an important parameter in establishing risk estimates for industrial workers who might accidentally inhale these materials and in evaluating environmental health impacts associated with Pu. In vitro solubility of industrial plutonium aerosols in a simulated lung fluid is compared to similar studies with ultrafine aerosols from laser ignition of delta phase plutonium metal and laboratory-produced spherical particles of 238 PuO 2 and 239 PuO 2 . Although relatively insoluble, industrial plutonium-mixed oxide aerosols were much more soluble than laboratory-produced plutonium dioxide particles. Chain agglomerate aerosols from laser ignition of metallic Pu indicated in vitro dissolution half-times of 10 and 50 days for activity median aerodynamic diameter (AMAD) of 0.7 and 2.3 μm, respectively. Plutonium-containing mixed oxide aerosols indicated dissolution half-times of 40 to 500 days for particles formed by industrial powder comminution and blending. Centerless grinding of fuel pellets yielded plutonium-containing aerosols with dissolution half-times of 1200 to 8000 days. All mixed oxide particles were in the size range 1.0 μm to 2.5 μm AMAD

238Pu based energy micro-generation sources for medical applications

International Nuclear Information System (INIS)

Boucher, Rene

1968-10-01

Pace-makers are frequently implanted in the human body. The existing apparatus are, actually, equipped with chemical piles with a lifetime of about 15 months. The use of 238 Pu will provide a pace-maker with an autonomy of 10 years at least. Principal problems of security due to the use of plutonium are considered. It is advisable to improve the properties of pure plutonium by small additions of elements such as cerium, scandium, indium, gallium or americium. A number of the most important properties for a pace-maker source are presented. Finally, the fabrication and canning of the source are surveyed. (author) [fr

Plutonium chemistry: a synthesis of experimental data and a quantitative model for plutonium oxide solubility

International Nuclear Information System (INIS)

Haschke, J.M.; Oversby, V.M.

2002-01-01

The chemistry of plutonium is important for assessing potential behavior of radioactive waste under conditions of geologic disposal. This paper reviews experimental data on dissolution of plutonium oxide solids, describes a hybrid kinetic-equilibrium model for predicting steady-state Pu concentrations, and compares laboratory results with predicted Pu concentrations and oxidation-state distributions. The model is based on oxidation of PuO 2 by water to produce PuO 2+x , an oxide that can release Pu(V) to solution. Kinetic relationships between formation of PuO 2+x , dissolution of Pu(V), disproportionation of Pu(V) to Pu(IV) and Pu(VI), and reduction of Pu(VI) are given and used in model calculations. Data from tests of pyrochemical salt wastes in brines are discussed and interpreted using the conceptual model. Essential data for quantitative modeling at conditions relevant to nuclear waste repositories are identified and laboratory experiments to determine rate constants for use in the model are discussed

Plutonium vulnerability issues at Hanford's Plutonium Finishing Plant

International Nuclear Information System (INIS)

Feldt, E.; Templeton, D.W.; Tholen, E.

1995-01-01

The Plutonium Finishing Plant (PFP) at the Hanford, Washington Site was operated to produce plutonium (Pu) metal and oxide for national defense purposes. Due to the production requirements and methods utilized to meet national needs and the abrupt shutdown of the plant in the late 1980s, the plant was left in a condition that poses a risk of radiation exposure to plant workers, of accidental radioactive material release to the environment, and of radiation exposure to the public. In early 1994, an Environmental Impact Statement (EIS) to determine the best methods for cleaning out and stabilizing Pu materials in the PFP was started. While the EIS is being prepared, a number of immediate actions have been completed or are underway to significantly reduce the greatest hazards in the PFP. Recently, increased attention his been paid to Pu risks at Department of Energy (DOE) facilities resulting in the Department-wide Plutonium Vulnerability Assessment and a recommendation by the Defense Nuclear Facilities Safety Board (DNFSB) for DOE to develop integrated plans for managing its nuclear materials

Radiolysis of aqueous solution of plutonium; Radiolyse des solutions aqueuses de plutonium

Energy Technology Data Exchange (ETDEWEB)

Pages nee Flon, M [Commissariat a l' Energie Atomique, Saclay (France). Centre d' Etudes Nucleaires

1960-07-01

reduction of IV into III was measured with HClO{sub 4}. (author) [French] On a etudie l'action des rayons gamma sur les solutions aqueuses de plutonium a divers etats de valence, en milieu sulfurique, perchlorique, nitrique et chlorhydrique. Le phenomene principal est la reduction de Pu VI en Pu V suivie de la dismutation de la valence V en VI et IV. Pour les solutions d'acide sulfurique et perchlorique 0,2N on a donne le mecanisme des reactions: la radiolyse de l'eau conduit aux produits OH, H{sub 2}O{sub 2}, H et H{sub 2}. Pu VI est reduit par H and H{sub 2}O{sub 2} tandis que Pu V est reoxyde par OH. Cependant l'action de l'eau oxygenee est lente et provoque un effet prolonge. Une etude menee parallelement sur l'action de H{sub 2}O{sub 2} a confirme ceci. Les mesures de disparition de Pu VI et d'apparition de Pu IV faites par spectrophotometrie ont conduit a determiner G{sub H{sub 2}}{sub O{sub 2}} = 0,8 et G{sub H} - G{sub OH} = 0,8. Par microanalyse de gaz on a mesure G{sub H{sub 2}} = 0,41. Ces donnees permettent de calculer le rendement de radiolyse de l'eau G{sub {sup -}}{sub H{sub 2}}{sub O} = 4,35. Les ions sulfate ont une influence complexe sur la reoxydation de Pu V comme le montrent les resultats obtenus sur des solutions plus concentrees en H{sub 2}SO{sub 4}. La reduction se poursuit jusqu'a la valence Ill en milieu perchlorique. Les ions Cl{sup -} et surtout NO{sub 3}{sup -} inhibent la reduction et peuvent la supprimer completement. L'action des particules {alpha} du plutonium et du polonium est tres analogue a celle de l'eau oxygenee. La reduction a lieu apres des periodes d'induction plus ou moins longues selon l'anion (surtout HSO{sub 4}{sup -} ). Elles sont liees a l'accumulation de H{sub 2}O{sub 2} et (ou) de peroxyde de plutonium. Aux faibles acidites le peroxyde de Pu IV a tendance a conduire a des formes polymerisees. Dans les cas les plus simples (H{sub 2}SO{sub 4} et HClO{sub 4} 0,2N) les rendements suivants ont ete obtenus ou calcules: G

Precipitation of plutonium (III) oxalate and calcination to plutonium oxide

International Nuclear Information System (INIS)

Esteban, A.; Orosco, E.H.; Cassaniti, P.; Greco, L.; Adelfang, P.

1989-01-01

The plutonium based fuel fabrication requires the conversion of the plutonium nitrate solution from nuclear fuel reprocessing into pure PuO2. The conversion method based on the precipitation of plutonium (III) oxalate and subsequent calcination has been studied in detail. In this procedure, plutonium (III) oxalate is precipitated, at room temperature, by the slow addition of 1M oxalic acid to the feed solution, containing from 5-100 g/l of plutonium in 1M nitric acid. Before precipitation, the plutonium is adjusted to trivalent state by addition of 1M ascorbic acid in the presence of an oxidation inhibitor such as hydrazine. Finally, the precipitate is calcinated at 700 deg C to obtain PuO2. A flowsheet is proposed in this paper including: a) A study about the conditions to adjust the plutonium valence. b) Solubility data of plutonium (III) oxalate and measurements of plutonium losses to the filtrate and wash solution. c) Characterization of the obtained products. Plutonium (III) oxalate has several potential advantages over similar conversion processes. These include: 1) Formation of small particle sizes powder with good pellets fabrication characteristics. 2) The process is rather insensitive to most process variables, except nitric acid concentration. 3) Ambient temperature operations. 4) The losses of plutonium to the filtrate are less than in other conversion processes. (Author) [es

Analysis and composition of the first U-Pu charge (0,043 per cent of Pu); Analyse et constitution du 1. jeu U-Pu (0,043 pour cent de Pu)

Energy Technology Data Exchange (ETDEWEB)

Brunet, J P; Lapparent, D de; Lourme, P [Commissariat a l' Energie Atomique, Saclay (France). Centre d' Etudes Nucleaires

1965-07-01

Checking the homogeneity in the content of plutonium of 0,043 per cent Pu-natural uranium alloy slugs has been made by Pu 240 and U 238 spontaneous fissions neutrons counting. The purpose of the test was to select groups of slugs to be correctly associated into fuel rods for critical experiments. General technic for spontaneous fissions counting, then elaboration of data in view of ranking the slugs are described. Results are given for this particular case. (authors) [French] On a effectue un controle d'homogeneite de teneur en plutonium sur des billettes d'alliage 0,043 pour cent Pu-uranium naturel, par comptage des fissions spontanees du plutonium 240 et de l'uranium 238. Le but du controle etait de permettre une association correcte de ces billettes a l'interieur des elements combustibles destines a servir dans des experiences critiques. On indique la methode generale de comptage des fissions spontanees, puis le depouillement des donnees en vue du classement des barreaux. Les resultats pour ce cas particulier sont donnes dans le rapport. (auteurs)

Mortality study of Los Alamos workers with higher exposures to plutonium

International Nuclear Information System (INIS)

Voelz, G.L.; Wilkinson, G.S.; Healy, J.W.; McInroy, J.F.; Tietjen, G.L.

1983-01-01

A group of white male workers with the highest internal depositions of plutonium at the Los Alamos National Laboratory was selected in 1974 for a study of mortality. This group of 224 persons includes all those with an estimated deposition (in 1974) of 10 nanocuries or more of plutonium, principally 239 Pu but also in some cases 238 Pu. Follow-up of these workers is 100% complete through 1980. Smoking histories were obtained on all persons. Exposure histories for external radiation and plutonium were reviewed for each subject. Standardized mortality ratios (SMR) were calculated using rates for white males in the United States population, adjusted for age and year of death. SMRs are low for all causes of death (56; 95% CI 40, 75) or for all malignant neoplasms (54; 95% CI 23,106). Cancers of interest for plutonium exposures, including cancers of bone, lung, liver, and bone marrow/lymphatic systems, were infrequent or absent. The absence of a detectable excess of cancer deaths is consistent with the low calculated risk to these workers using current radiation risk coefficients. An alternate theory that suggests much higher risk of lung cancer due to synergistic effects of smoking and inhaled insoluble plutonium particles is not supported by this study

Observations of surface-mediated reduction of Pu(VI) to Pu(IV) on hematite nanoparticles by ATR FT-IR

Energy Technology Data Exchange (ETDEWEB)

Emerson, Hilary P. [Florida International Univ., Applied Research Center, Miami, FL (United States); Powell, Brian A. [Clemson Univ., Dept. of Enviromental Engineering and Earth Sciences, Anderson, SC (United States)

2015-07-01

Previous studies have shown that mineral surfaces may facilitate the reduction of plutonium though the mechanisms of the reduction are still unknown. The objective of this study is to use batch sorption and attenuated total reflectance Fourier transform infrared spectroscopy experiments to observe the surface-mediated reduction of plutonium on hematite nanoparticles. These techniques allow for in situ measurement of reduction of plutonium with time and may lead to a better understanding of the mechanisms of surface mediated reduction of plutonium. For the first time, ATR FT-IR peaks for Pu(VI) sorbed to hematite are measured at ∝ 916 cm{sup -1}, respectively. The decrease in peak intensity with time provides a real-time, direct measurement of Pu(VI) reduction on the hematite surface. In this work pseudo first order rate constants estimated at the high loadings (22 mg{sub Pu}/g{sub hematite}, 1.34 x 10{sup -6} M{sub Pu}/m{sup 2}) for ATR FT-IR are approximately 10 x slower than at trace concentrations based on previous work. It is proposed that the reduced rate constant at higher Pu loadings occurs after the reduction capacity due to trace Fe(II) has been exhausted and is dependent on the oxidation of water and possibly electron shuttling based on the semiconducting nature of hematite. Therefore, the reduction rate at higher loadings is possibly due to the thermodynamic favorability of Pu(IV)-hydroxide complexes.

Skeletal lesions from inhaled plutonium in beagles

International Nuclear Information System (INIS)

Dagle, G.E.; Park, J.F.; Weller, R.E.; Ragan, H.A.; McClanahan, B.J.; Fisher, D.R.

1984-10-01

The report briefly reviews the skeletal effects observed in ongoing lifespan studies in beagle dogs at 13, 10, and 7 years, respectively, after inhalation exposure to 239 Pu oxide and nitrate or 238 Pu oxide. Plutonium nitrate was chosen to represent soluble material more readily translocated to bone and other tissues than the oxide. Bone lesions related to plutonium exposure were observed only in dogs exposed to 238 Pu oxide and 239 Pu nitrate. The skeleton accumulated approximately 2% ( 239 Pu oxide), 45% ( 238 Pu oxide) or 50% ( 239 Pu nitrate) of the final body burdens at 13, 10, and 7 years, respectively, after exposure. 11 references, 2 figures

The solubility of hydrogen and deuterium in alloyed, unalloyed and impure plutonium metal

Energy Technology Data Exchange (ETDEWEB)

Richmond, Scott [Los Alamos National Laboratory; Bridgewater, Jon S [Los Alamos National Laboratory; Ward, John W [Los Alamos National Laboratory; Allen, Thomas A [Los Alamos National Laboratory

2009-01-01

Pressure-Composition-Temperature (PCT) data are presented for the plutonium-hydrogen (Pu-H) and plutonium-deuterium (Pu-D) systems in the solubility region up to terminal solubility (precipitation of PuH{sub 2}). The heats of solution for PuH{sub s} and PuD{sub s} are determined from PCT data in the ranges 350-625 C for gallium alloyed Pu and 400-575 C for unalloyed Pu. The solubility of high purity plutonium alloyed with 2 at.% gallium is compared to high purity unalloyed plutonium. Significant differences are found in hydrogen solubility for unalloyed Pu versus gallium alloyed Pu. Differences in hydrogen solubility due to an apparent phase change are observable in the alloyed and unalloyed solubilities. The effect of iron impurities on Pu-Ga alloyed Pu is shown via hydrogen solubility data as preventing complete homogenization.

The solubility of hydrogen and deuterium in alloyed, unalloyed and impure plutonium metal

International Nuclear Information System (INIS)

Richmond, S; Bridgewater, J S; Ward, J W; Allen, T H

2010-01-01

Pressure-Composition-Temperature (PCT) data are presented for the plutonium-hydrogen (Pu-H) and plutonium-deuterium (Pu-D) systems in the solubility region up to terminal solubility (precipitation of PuH 2 ). The heats of solution for PuH S and PuD S are determined from PCT data in the ranges 350-625 deg. C for gallium alloyed Pu and 400-575 deg. C for unalloyed Pu. The solubility of high purity plutonium alloyed with 2 at.% gallium is compared to high purity unalloyed plutonium. Significant differences are found in hydrogen solubility for unalloyed Pu versus gallium alloyed Pu. Differences in hydrogen solubility due to an apparent phase change are observable in the alloyed and unalloyed solubilities. The effect of iron impurities on Pu-Ga alloyed Pu is shown via hydrogen solubility data as preventing complete homogenization.

ZPR-6 assembly 7 high {sup 240}Pu core experiments : a fast reactor core with mixed (Pu,U)-oxide fuel and a centeral high{sup 240}Pu zone.

Energy Technology Data Exchange (ETDEWEB)

Lell, R. M.; Morman, J. A.; Schaefer, R.W.; McKnight, R.D.; Nuclear Engineering Division

2009-02-23

ZPR-6 Assembly 7 (ZPR-6/7) encompasses a series of experiments performed at the ZPR-6 facility at Argonne National Laboratory in 1970 and 1971 as part of the Demonstration Reactor Benchmark Program (Reference 1). Assembly 7 simulated a large sodium-cooled LMFBR with mixed oxide fuel, depleted uranium radial and axial blankets, and a core H/D near unity. ZPR-6/7 was designed to test fast reactor physics data and methods, so configurations in the Assembly 7 program were as simple as possible in terms of geometry and composition. ZPR-6/7 had a very uniform core assembled from small plates of depleted uranium, sodium, iron oxide, U{sub 3}O{sub 8} and Pu-U-Mo alloy loaded into stainless steel drawers. The steel drawers were placed in square stainless steel tubes in the two halves of a split table machine. ZPR-6/7 had a simple, symmetric core unit cell whose neutronic characteristics were dominated by plutonium and {sup 238}U. The core was surrounded by thick radial and axial regions of depleted uranium to simulate radial and axial blankets and to isolate the core from the surrounding room. The ZPR-6/7 program encompassed 139 separate core loadings which include the initial approach to critical and all subsequent core loading changes required to perform specific experiments and measurements. In this context a loading refers to a particular configuration of fueled drawers, radial blanket drawers and experimental equipment (if present) in the matrix of steel tubes. Two principal core configurations were established. The uniform core (Loadings 1-84) had a relatively uniform core composition. The high {sup 240}Pu core (Loadings 85-139) was a variant on the uniform core. The plutonium in the Pu-U-Mo fuel plates in the uniform core contains 11% {sup 240}Pu. In the high {sup 240}Pu core, all Pu-U-Mo plates in the inner core region (central 61 matrix locations per half of the split table machine) were replaced by Pu-U-Mo plates containing 27% {sup 240}Pu in the plutonium

Plutonium uptake by plants from soil containing plutonium-238 dioxide particles. Final report

International Nuclear Information System (INIS)

Brown, K.W.; McFarlane, J.C.

1977-05-01

Three plant species--alfalfa, lettuce, and radishes were grown in soils contaminated with plutonium-238 dioxide (238)PuO2 at concentrations of 23, 69, 92, and 342 nanocuries per gram (nCi/g). The length of exposure varied from 60 days for the lettuce and radishes to 358 days for the alfalfa. The magnitude of plutonium incorporation as indicated by the discrimination ratios for these species, after being exposed to the relatively insoluble PuO2, was similar to previously reported data using different chemical forms of plutonium. Evidence indicates that the predominant factor in plutonium uptake by plants may involve the chelation of plutonium contained in the soils by the action of compounds such as citric acid and/or other similar chelating agents released from the plant roots

Stability with temperature of mixed uranium plutonium monocarbides

International Nuclear Information System (INIS)

Riglet-Martial, Ch.; Dumas, J.C.; Piron, J.P.; Gueneau, Ch.

2008-01-01

Full text: Among the different advanced fuel materials of concern for Generation IV systems, the mixed carbide of uranium and plutonium fuel is considered as one of the key materials for Gas Fast Reactors (GFR) systems. For purposes of optimising its fabrication process as well as its performances in various operating conditions, the losses of gaseous plutonium specially at elevated temperatures have to be controlled and minimized. The paper is therefore concerned with a parametric analysis of the stability with temperature of mixed carbides of uranium and plutonium. Previous published experimental studies have shown that mixed (U ,Pu) carbides undergo a highly incongruent sublimation at high temperatures: the vapour phase in equilibrium with the solid is mainly composed of gaseous plutonium (P Pu /P total > 99 % ) while the contribution of gaseous U and C remains very low. The composition of the system U 1-z Pu z C 1+x ' (z =Pu/(U+Pu) and x C/(U+Pu)), the temperature (T) and the expansion volume (V) of the gas are the main parameters in the loss of gaseous Pu. The calculations are carried out using the SAGE (Solgasmix Advanced Gibbs Energy) software, by assuming ideal solid solutions between UC and PuC, as well as between U 2 C 3 and Pu 2 C 3 . The validity of the model is previously tested using published equilibrium vapour pressure data. This work gives rise to a large description of the variations of Pu losses from mixed uranium plutonium carbides and leads to some basic recommendations in connection with the use of this advanced fuel materials

DFT and two-dimensional correlation analysis methods for evaluating the Pu{sup 3+}–Pu{sup 4+} electronic transition of plutonium-doped zircon

Energy Technology Data Exchange (ETDEWEB)

Bian, Liang, E-mail: bianliang@ms.xjb.ac.cn [Key Laboratory of Functional Materials and Devices for Special Environments, Chinese Academy of Sciences, Urumqi 830011, Xinjiang (China); Laboratory for Extreme Conditions Matter Properties, South West University of Science and Technology, Mianyang 621010, Sichuan (China); Dong, Fa-qin; Song, Mian-xin [Laboratory for Extreme Conditions Matter Properties, South West University of Science and Technology, Mianyang 621010, Sichuan (China); Dong, Hai-liang [Department of Geology and Environmental Earth Science, Miami University, Oxford, OH 45056 (United States); Li, Wei-Min [Key Laboratory of Functional Materials and Devices for Special Environments, Chinese Academy of Sciences, Urumqi 830011, Xinjiang (China); Duan, Tao; Xu, Jin-bao [Laboratory for Extreme Conditions Matter Properties, South West University of Science and Technology, Mianyang 621010, Sichuan (China); Zhang, Xiao-yan [Key Laboratory of Functional Materials and Devices for Special Environments, Chinese Academy of Sciences, Urumqi 830011, Xinjiang (China); Laboratory for Extreme Conditions Matter Properties, South West University of Science and Technology, Mianyang 621010, Sichuan (China)

2015-08-30

Highlights: • Effect of Pu f-shell electron on the electronic property of zircon is calculated via DFT and 2D-CA techniques. • Reasons of Pu f-shell electron influencing on electronic properties are systematically discussed. • Phase transitions are found at two point 2.8 mol% and 7.5 mol%. - Abstract: Understanding how plutonium (Pu) doping affects the crystalline zircon structure is very important for risk management. However, so far, there have been only a very limited number of reports of the quantitative simulation of the effects of the Pu charge and concentration on the phase transition. In this study, we used density functional theory (DFT), virtual crystal approximation (VCA), and two-dimensional correlation analysis (2D-CA) techniques to calculate the origins of the structural and electronic transitions of Zr{sub 1−c}Pu{sub c}SiO{sub 4} over a wide range of Pu doping concentrations (c = 0–10 mol%). The calculations indicated that the low-angular-momentum Pu-f{sub xy}-shell electron excites an inner-shell O-2s{sup 2} orbital to create an oxygen defect (V{sub O-s}) below c = 2.8 mol%. This oxygen defect then captures a low-angular-momentum Zr-5p{sup 6}5s{sup 2} electron to form an sp hybrid orbital, which exhibits a stable phase structure. When c > 2.8 mol%, each accumulated V{sub O-p} defect captures a high-angular-momentum Zr-4d{sub z} electron and two Si-p{sub z} electrons to create delocalized Si{sup 4+} → Si{sup 2+} charge disproportionation. Therefore, we suggest that the optimal amount of Pu cannot exceed 7.5 mol% because of the formation of a mixture of ZrO{sub 8} polyhedral and SiO{sub 4} tetrahedral phases with the orientation (10-1). This study offers new perspective on the development of highly stable zircon-based solid solution materials.

Determination of thorium and plutonium in AHWR experimental (Th, 1%Pu)O2 MOX fuel after microwave dissolution

International Nuclear Information System (INIS)

Fulzele, Ajit K.; Malav, R.K.; Pandey, Ashish; Kapoor, Y.S.; Kumar, Manish; Singh, Mamta; Das, D.K.; Prakash, Amrit; Behere, P.G.; Afzal, Mohd

2013-01-01

This paper describes determination of thorium and plutonium in experimental (Th, 1%Pu)O 2 AHWR (Advanced Heavy Water Reactor) MOX fuel samples after dissolution by microwave. Time taken to dissolve ∼ 2g of MOX sample by conventional IR heating technique in conc. HNO 3 + 0.05 M HF mixture is about 35-40 hours while using microwave dissolution technique it is ∼ 2 hours. Hence, with the help of microwave dissolution technique analysis time for each sample has been reduced from week to a day. The PuO 2 content (wt%) in the MOX pellets was within specification limit, (1.0±0.1)%. (author)

Measurement of plutonium isotopic composition by gamma-ray spectroscopy

International Nuclear Information System (INIS)

Kim, J. S.; Shin, J. S.; Ahn, J. S.

1998-01-01

The technology of the analysis of plutonium isotopic ratio is independent of the measurement geometry and applicable to samples of physical and chemical composition. Three standard plutonium samples were measured in the HPGe system. The results showed that CRM 136 and CRM 137 containing 238 Pu(0.223%) and 238 Pu(0.268%) were 18.4% and 14.2% error and CRM 138 of 238 Pu(0.01%) was 76% error. However the analysis represented less than 1.6% and 9% error in the three standard samples of highly involved 239 Pu and 240 Pu. Therefore, gamma-ray spectroscopy is very effective in the plutonium isotope analysis, having greater than 10% in content

Determination of plutonium in soils by mass spectrometry

International Nuclear Information System (INIS)

Storms, H.A.; Carlson, D.C.; Hunter, F.F.

1974-01-01

A procedure is described in which mass spectrometry is utilized for the determination of plutonium in soils. Using this procedure we have measured plutonium isotopic compositions at concentrations as low as 2 x 10 -14 grams Pu per gram soil. A thermal ionization source with canoe-shaped rhenium filament, is utilized in the mass spectrometer. The plutonium, when loaded onto the filament, is contained in a single Dowex-1 resin bead which is about 350 micrometers in diameter. Concentrating the plutonium within this single bead is a key step in the procedure and produces a relatively clean plutonium fraction. The resin bead also serves as an effective diffusion barrier such that the plutonium is prevented from being removed with the lower boiling impurities. The Pu remains in the bead until the temperature is sufficiently high for efficient production of Pu + ions. Plutonium ionization efficiencies as high as 2.5 percent have been measured

Radiological safety aspects of handling plutonium

International Nuclear Information System (INIS)

Sundararajan, A.R.

2016-01-01

Department of Atomic Energy in its scheme of harnessing the nuclear energy for electrical power generation and strategic applications has given a huge role to utilization of plutonium. In the power production programme, fast reactors with plutonium as fuel are expected to play a major role. This would require establishing fuel reprocessing plants to handle both thermal and fast reactor fuels. So in the nuclear fuel cycle facilities variety of chemical, metallurgical, mechanical operations have to be carried out involving significant inventories of "2"3"9 Pu and associated radionuclides. Plutonium is the most radiotoxic radionuclide and therefore any facility handling it has to be designed and operated with utmost care. Two problems of major concern in the protection of persons working in plutonium handling facilities are the internal exposure to the operating personnel from uptake of plutonium and transplutonic nuclides as they are highly radiotoxic and the radiation exposure of hands and eye lens during fuel fabrication operations especially while handling recycled high burn up plutonium. In view of the fact that annual limit for intake is very small for "2"3"9Pu and its radiation emission characteristics are such that it is a huge challenge for the health physicists to detect Pu in air and in workers. This paper discusses the principles and practices followed in providing radiological surveillance to workers in plutonium handling areas. The challenges in protecting the workers from receiving exposures to hands and eye lens in handling high burn up plutonium are also discussed. The sites having Pu fuel cycle facilities should have trained medical staff to handle cases involving excessive intake of plutonium. (author)

The toxicological study of plutonium: tumor-inducing effect of plutonium in rats

International Nuclear Information System (INIS)

Chen Rusong; Zhao Yongchan; Wang Shoufang; Li Maohe

1992-09-01

The carcinogenic effects of Pu compounds through different routs of administration are introduced. The following results have been obtained: (1) Pu is really a powerful carcinogenic radionuclide. (2) Osteosarcoma can be induced in rats by plutonium nitrate at low level radiation. The incidence is from 38.9% to 42.9% in the 185 kBq/kg group. (3) Lung cancer can be induced by plutonium dioxide and the biological effect of TLN (thoracic lymph node) is significant. (4) Under the combined treatment of 239 Pu, 90 Sr and 144 Ce, the carcinogenic effects is much greater than their separative effect on rats. (5) By using the method of comparative toxicology, the risk of osteosarcoma induced by Pu in human is about 600/(10 6 man·cGy) which is extrapolated from animal to human. The above conclusions are important for evaluating the potential hazard of Pu to human beings

Density of Plutonium Turnings Generated from Machining Activities

Energy Technology Data Exchange (ETDEWEB)

Gonzales, John Robert [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Vigil, Duane M. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Jachimowski, Thomas A. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Archuleta, Alonso [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Arellano, Gerald Joseph [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Melton, Vince Lee [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

2016-10-20

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.

Inhaled plutonium oxide in dogs

International Nuclear Information System (INIS)

Anon.

1981-01-01

This project is concerned with long-term experiments to determine the life-span dose-effect relationships of inhaled 239 PuO 2 and 238 PuO 2 in beagles. The data will be used to estimate the health effects of inhaled transuranics. The tissue distribution of plutonium, radiation effects in the lung and hematologic changes in plutonium-exposed beagles with lung tumors were evaluated

Simultaneous measurement of {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, and {sup 242}Pu by high resolution inductively coupled plasma mass spectrometer (HR ICP-MS) in marine sediments; Mesure des isotopes du plutonium des sediments marins par spectrometrie de masse a plasma couple inductivement haute resolution (HR ICP-MS)

Energy Technology Data Exchange (ETDEWEB)

Bruneau, F

1999-07-01

Transuranics elements are of particular interest in radioecological studies because of their radiotoxicity and their potential use to decipher source fingerprints and transport processes. The simultaneous measurement of {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, and {sup 242}Pu in environmental samples requires a specific chemical procedure. This work deals with an analytical procedure which yields a very high grade of purification of Pu suitable for ultra low level detection by HR ICP-MS, from marine sediments. After the elimination of major elements (Fe, Al, Mg...) by a first chromatographic separation, a new device of purification by solvent extraction and concentration by a second chromatographic separation is used to obtain a concentrated and high purified solution of plutonium. The chemical procedure have been validated on IAEA certified sediment samples and on sediment samples collected in the roads of Cherbourg which had been previously analysed by other techniques (a spectrometry and thermo-ionisation mass spectrometer). (author)

The U-Pu inspector, a new instrument to determine the isotopic compositions of uranium and plutonium

International Nuclear Information System (INIS)

Verplancke, J.; Van Dyck, R.; Tench, O.; Sielaff, B.

1994-01-01

The U/Pu-InSpector is a new integrated, portable instrument that can measure the isotopic composition of samples containing uranium and/or plutonium without prior calibration and without the need for skilled operators. It consists of a Low Energy Germanium detector in a Multi-attitude Cryostat (MAC). A shield and collimator are built-in, directly around the detector element, reducing the weight of this detector and shield to approximately 8 kg with a full dewar. The dewar can quickly and easily be filled with a self-pressurizing funnel. The detector is connected to a small portable battery operated analyzer and a Notebook computer. The spectra are automatically stored and analyzed with the help of the MGA codes for plutonium and/or for uranium. 5 refs., 1 fig

Application of ICP-MS and AMS for determination of Pu- and U-isotope ratios for source identification

Energy Technology Data Exchange (ETDEWEB)

Skipperud, L. (Norwegian Univ. of Life Sciences, Isotope Lab.. Dept. of Plant and Environmental Sciences, AAs (Norway))

2010-03-15

Full text: 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 have resulted in a relatively uniform, underlying global distribution of plutonium. Plutonium isotope ratios are known to vary with reactor type, nuclear fuel-burn up time, neutron flux, and energy, and for fallout from nuclear detonations, weapon type and yield. Weapons-grade plutonium is characterized by a low content of the 240Pu isotope, with 240Pu/239Pu isotope ratio less than 0.05. In contrast, both global weapons fallout and spent nuclear fuel from civil reactors have higher 240Pu/239Pu isotope ratios (civil nuclear power reactors have 240Pu/239Pu atom ratios of between about 0.2-1). Thus, different sources often exhibit characteristic plutonium isotope ratios and these ratios can be used to identify the origin of contamination, calculate inventories, or follow the migration of contaminated sediments and waters. The measurement of the plutonium-isotope ratios in these studies 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. The present paper presents results from determination of plutonium concentrations and isotope ratios in sediment samples collected during various expeditions to the Kara Sea, the Ob and Yenisey estuaries and their river systems and also Pu isotope ratios in the near area of Mayak PA. Weapons-grade plutonium is characterized by a low content of the Pu-240 isotope, with Pu-240/Pu-239 isotope ratio less than 0.05. In contrast, both global weapons fallout and spent nuclear fuel from civil reactors have higher Pu-240/Pu-239 isotope ratios, and

Finite element analysis of local overheating within plutonium enriched UO2 fuel rods caused by PuO2 islands

International Nuclear Information System (INIS)

Sarmiento, G.S.

1980-01-01

Within natural UO 2 fuel elements enriched with plutonium, this last material should form PuO 2 solid solutions inside the UO 2 pellets, in a wide range of concentrations. If the solutions are obtained by mechanical mixing of the oxides, PuO 2 islands are formed in the UO 2 matrix. These islands may be the source of several problems in the fuel behaviour, the most important being the overheating of the matrix in the neighbourhood of the particles. It is caused by the large fission cross section of plutonium compared with that of uranium. A detailed study of the thermal effects produced by PuO 2 particles in the UO 2 matrix and the cladding is then important for the specification of their permissible size. A portion of the fuel rods with spherical particles in the most significant places was studied. In order to obtain the dimensionless overheating of the fuel and cladding produced by the presence of those particles, the spatial distribution of temperature was calculated, solving the stationary and linear bidimensional equation of heat conducting using a finite element code. Several geometrical variables and material properties have been taken as dimensionless parameters. A satisfactory convergence of the numerical results to an asymptotic limit with a well-known exact solution, has been obtained. (orig.)

Plutonium in a grassland ecosystem

International Nuclear Information System (INIS)

Little, C.A.

1976-01-01

This study was concerned with plutonium contamination of grassland at the U.S. Energy Research and Development Administration Rocky Flats plant northwest of Denver, Colorado. Of interest were: the definition of major plutonium-containing ecosystem compartments; the relative amounts in those compartments; how those values related to studies done in other geogrphical areas; whether or not the predominant isotopes, 238 Pu and 239 Pu, behaved differently; and what mechanisms might have allowed for the observed patterns of contamination. Samples of soil, litter, vegetation, arthropods, and small mammals were collected for plutonium analysis and mass determination from each of two macroplots. Small aliquots (5 g or less) were analyzed by a rapid liquid scintillation technique and by alpha spectrometry. Of the compartments sampled, greater than 99% of the total plutonium was contained in the soil. The concentrations of plutonium in soil were significantly inversely correlated with distance from the contamination source, depth of the sample, and particle size of the sieved soil samples. The soil data suggested that the distribution of contamination largely resulted from physical transport processes. A mechanism of agglomerated submicron plutonium oxide particles and larger (1-500 μm) host soil particles was proposed. Concentrations of Pu in litter and vegetation were inversely correlated to distance from the source and directly correlated to soil concentrations at the same location. Comparatively high concentration ratios of vegetation to soil suggested wind resuspension of contamination as an important transport mechanism. Arthropod and small mammal samples were highly skewed, kurtotic, and quite variable, having coefficients of variation (standard deviation/mean) as high as 600%. Bone Pu concentrations were lower than other tissues. Hide, GI, and lung were generally not higher in Pu than kidney, liver and muscle

The US plutonium materials conversion program in Russia

International Nuclear Information System (INIS)

Zygmunt, S.J.; Mason, C.F.V.; Hahn, W.K.

2000-01-01

Progress has been made in Russia towards the conversion of weapons-grade plutonium (w-Pu) into plutonium oxide (PuO 2 ) suitable for further manufacture into mixed oxide (MOX) fuels. This program was started in 1998 in response to US proliferation concerns and the acknowledged international need to decrease the available weapons-grade Pu. A similar agenda is being followed in the US to address disposition of US surplus weapons-grade Pu. In Russia a conversion process has been selected and a site proposed. This paper discusses the present state of the program in support of this future operating facility that will process up to 5 metric tons of plutonium a year. (authors)

Electronic structure of Pu-Ce(-Ga) and Pu-Am(-Ga) alloys, stabilized in the {delta} phase; Structure electronique d'alliages Pu-Ce(-Ga) et Pu-Am(-Ga) stabilises en phase {delta}

Energy Technology Data Exchange (ETDEWEB)

Dormeval, M

2001-09-01

The behaviour of {delta}-plutonium, stable between 319 and 451 deg C, exhibits numerous singularities which are still a mystery for both physicists and metallurgists. This is due to its complex electronic structure, and in particular to the 5f electrons, which are at the edge between localization and delocalization. The stability domain of the {delta} phase can be extended down to room temperature by alloying with so called 'deltagen atoms' such as gallium (Ga), aluminum (A1), cerium (Ce) or americium (Am). The present work deals, one the one hand, with the influence of cerium and americium solutes regarding the localization of the 5f electrons of {delta}-plutonium, in binary Pu-Ce and Pu-Am alloys. On the other hand, the effect of two different deltagen solutes, simultaneously present, on the stability of the {delta} phase has been studied in ternary Pu-Am-Ga and Pu-Ce-Ga alloys. The electronic structure being strongly related to the crystalline organization, characterization methods such as X-Ray diffraction and EXAFS measurements were used together with electrical resistivity and magnetic susceptibility experiments. These showed that the roles of cerium and americium, supposed to be similar at the beginning of this investigation, are actually very different. Moreover, the additive effect of cerium and gallium, and, americium and gallium, has been demonstrated. Studying plutonium alloys, which are radioactive, also means following their evolution in time. The characteristics of the alloys have then been followed which allowed to detect, in Pu-Ce(-Ga) alloys, a destabilization of the {delta} phase and, to observe, in Pu-Am(-Ga) alloys, the influence of self-irradiation defects on the magnetic response. (author)

Plutonium speciation and isotope ratios in Yenisey and Ob river and Yenisey estuary

International Nuclear Information System (INIS)

Skipperud, L.; Oughton, DH.; Fifield, K.; Lind, O.C.; Salbu, B.; Brown, J.

2004-01-01

Plutonium isotope ratios are known to vary with reactor type, nuclear fuel-burn up time, neutron flux, and energy, and for fallout from nuclear detonations, weapon type and yield. Weapons-grade plutonium is characterized by a low content of the 240 Pu isotope, with 240 Pu/ 239 Pu isotope ratio less than 0.05. In contrast, both global weapons fallout and spent nuclear fuel from civil reactors have higher 240 Pu/ 239 Pu isotope ratios (civil nuclear power reactors have 240 Pu/ 239 Pu atom ratios of between about 0.2-1). Thus, different sources often exhibit characteristic plutonium isotope ratios and these ratios can be used to identify the origin of contamination, calculate inventories, or follow the migration of contaminated sediments and waters. Together with activity measurements and isotope ratios, knowledge of plutonium speciation in the Ob and Yenisey rivers and processes controlling its behaviour in estuarine systems is a prerequisite for predicting the transfer and subsequent environmental impact to Arctic Seas. With this in mind, the study had two objectives: first to determine whether discharges from nuclear installations in the river catchment areas are having any influence on Pu levels in the estuaries; and, second, to investigate the transfer and mobility of plutonium in the Yenisey river and estuary. Plutonium 240/239 ratios were determined using accelerator mass spectrometry (AMS). The data indicated a clear influence from a low 240 Pu: 239 Pu source in surface sediments collected from the Yenisey Estuary, whereas plutonium in the Ob Estuary sediments are dominated by global fallout. The results also show an increase in plutonium concentration and a decrease in isotope ratio going upstream from the estuary. Sequential extractions of sediments indicate that up 70% of the Pu in the Yenisey river is easily mobilized with weak oxidizing agents, which indicates that the Pu is organically bound, while the Pu is more strongly irreversible bound further out

Specification analysis of plutonium fuels : a potentiometric method for the determination of plutonium

International Nuclear Information System (INIS)

Vaidyanathan, S.; Natarajan, P.R.

1977-01-01

A potentiometric method for the routine determination of plutonium in the specification analysis of plutonium fuels is described. Plutonium is oxidized to Pu(VI) with AgO and Pu(VI) is reduced with Fe(II) after the destruction of excess AgO with sulphamic acid. The excess Fe(II) is titrated potentiometrically against K 2 Cr 2 O 7 , the titration being carried out by adding a concentrated titrant solution from a weight burette and a suitably diluted solution from another weight burette near the end. The overall relative standard deviation obtained in 326 analyses of a working standard solution by eight experimenters is 0.14 percent. (author)

An intercomparison experiment on isotope dilution thermal ionisation mass spectrometry using plutonium-239 spike for the determination of plutonium concentration in dissolver solution of irradiated fuel

International Nuclear Information System (INIS)

Aggarwal, S.K.; Shah, P.M.; Saxena, M.K.; Jain, H.C.; Gurba, P.B.; Babbar, R.K.; Udagatti, S.V.; Moorthy, A.D.; Singh, R.K.; Bajpai, D.D.

1996-01-01

Determination of plutonium concentration in the dissolver solution of irradiated fuel is one of the key measurements in the nuclear fuel cycle. This report presents the results of an intercomparison experiment performed between Fuel Chemistry Division (FCD) at BARC and PREFRE, Tarapur for determining plutonium concentration in dissolver solution of irradiated fuel using 239 Pu spike in isotope dilution thermal ionisation mass spectrometry (ID-TIMS). The 239 Pu spike method was previously established at FCD as viable alternative to the imported enriched 242 Pu or 244 Pu; the spike used internationally for plutonium concentration determination by IDMS in dissolver solution of irradiated fuel. Precision and accuracy achievable for determining plutonium concentration are compared under the laboratory and the plant conditions using 239 Pu spike in IDMS. For this purpose, two different dissolver solutions with 240 Pu/ 239 Pu atom ratios of about 0.3 and 0.07 corresponding, respectively, to high and low burn-up fuels, were used. The results of the intercomparison experiment demonstrate that there is no difference in the precision values obtained under the laboratory and the plant conditions; with mean precision values of better than 0.2%. Further, the plutonium concentration values determined by the two laboratories agreed within 0.3%. This exercise, therefore, demonstrates that ID-TIMS method using 239 Pu spike can be used for determining plutonium concentration in dissolver solution of irradiated fuel, under the plant conditions. 7 refs., 8 tabs

PU-ICE Summary Information.

Energy Technology Data Exchange (ETDEWEB)

Moore, Michael [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

2017-05-01

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, this 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.

Hematologic effects of inhaled plutonium in beagles

International Nuclear Information System (INIS)

Ragan, H.A.; Buschbom, R.L.; Park, J.F.; Dagle, G.E.; Weller, R.E.

1986-01-01

Beagle dogs were exposed, by inhalation, 5 to 11 years ago, to aerosols of 239 PuO 2 , 238 PuO 2 , or 239 Pu(NO 3 ) 4 , at six dose levels resulting in initial lung burdens ranging from ∼2 to ∼5500 nCi. Translocation of the plutonium to extrapulmonary sites was related to the physical-chemical characteristics of the plutonium compound. The highly insoluble 239 PuO 2 was retained primarily in the lung and associated lymph nodes, whereas 239 Pu(NO 3 ) 4 was much more soluble and translocated relatively rapidly to the skeleton and other extrapulmonary tissues. The 238 PuO 2 was intermediate in solubility and translocation characteristics. The hematologic effects of plutonium inhalation were most pronounced on lymphocyte populations. Evidence suggests that these effects result from irradiation of lymphocytes via the pulmonary lymph nodes with insoluble 239 PuO 2 , and via these same lymph nodes, extrapulmonary lymph nodes, and bone marrow lymphocytes with the more soluble forms, i.e., 238 PuO 2 and 239 Pu(NO 3 ) 4 . There is no evidence suggesting that these exposures increase the risk of developing myeloid or lymphoid neoplasia. 8 refs., 4 figs., 3 tabs

Thermophysical properties of solid and liquid pure and alloyed Pu: A review

Energy Technology Data Exchange (ETDEWEB)

Boivineau, M., E-mail: michel.boivineau@cea.f [CEA, Centre de Valduc, Departement de Recherches sur les Materiaux Nucleaires, F-21120 Is-sur-Tille (France)

2009-08-01

The thermophysical properties of both solid and liquid pure and alloyed plutonium have been investigated up to 4000 K by use of a resistive pulse heating technique, the so-called isobaric expansion experiment (IEX). Electrical resistivity, specific volume (density), latent heats of transformations, heat of fusion have been measured and extended in the whole liquid region. Additional static measurements have been also performed in order to determine the heat transport properties such as heat capacity, thermal diffusivity and thermal conductivity of plutonium alloys. After a first part devoted to additional results on pure Pu under rapid heating, this paper mostly deals with studies on different delta-stabilized Pu alloys in the high temperature range, particularly in the liquid state which is the principal originality of this work. In addition to the thermophysical data mentioned above, an attention is also paid onto sound velocity measurements on these alloys in the solid and liquid states. Hence, an anomalous behavior such as elastic softening is confirmed in the delta phase as already reported previously. Moreover, sound velocity and equation of state parameters (adiabatic and thermal bulk moduli, Grueneisen parameter, and specific heats ratio) have been investigated on liquid alloyed Pu. Such results confirm previous works on liquid pure Pu by presenting an atypical dual behavior of sound velocity, and are discussed in terms of delocalization process of the 5f electrons of both liquid pure and alloyed Pu.

Electronic structure of Pu-Ce(-Ga) and Pu-Am(-Ga) alloys, stabilized in the {delta} phase; Structure electronique d'alliages Pu-Ce(-Ga) et Pu-Am(-Ga) stabilises en phase {delta}

Energy Technology Data Exchange (ETDEWEB)

Dormeval, M

2001-09-01

The behaviour of {delta}-plutonium, stable between 319 and 451 deg C, exhibits numerous singularities which are still a mystery for both physicists and metallurgists. This is due to its complex electronic structure, and in particular to the 5f electrons, which are at the edge between localization and delocalization. The stability domain of the {delta} phase can be extended down to room temperature by alloying with so called 'deltagen atoms' such as gallium (Ga), aluminum (A1), cerium (Ce) or americium (Am). The present work deals, one the one hand, with the influence of cerium and americium solutes regarding the localization of the 5f electrons of {delta}-plutonium, in binary Pu-Ce and Pu-Am alloys. On the other hand, the effect of two different deltagen solutes, simultaneously present, on the stability of the {delta} phase has been studied in ternary Pu-Am-Ga and Pu-Ce-Ga alloys. The electronic structure being strongly related to the crystalline organization, characterization methods such as X-Ray diffraction and EXAFS measurements were used together with electrical resistivity and magnetic susceptibility experiments. These showed that the roles of cerium and americium, supposed to be similar at the beginning of this investigation, are actually very different. Moreover, the additive effect of cerium and gallium, and, americium and gallium, has been demonstrated. Studying plutonium alloys, which are radioactive, also means following their evolution in time. The characteristics of the alloys have then been followed which allowed to detect, in Pu-Ce(-Ga) alloys, a destabilization of the {delta} phase and, to observe, in Pu-Am(-Ga) alloys, the influence of self-irradiation defects on the magnetic response. (author)

Relationships among plutonium contents of soil, vegetation and animals collected on and adjacent to an integrated nuclear complex in the humid southeastern United States of America

International Nuclear Information System (INIS)

McLendon, H.R.

1976-01-01

Twenty-three representative sampling locations on and adjacent to the Savannah River Plant (SRP) site were selected to obtain information on plutonium movement in the food chain under southeastern US environmental conditions. Soil, a resuspendible fraction of the soil, honeysuckle (Lonicera japonica), and camphor weed (Heterotheca subaxillaris) were collected at each location. Grasshoppers and cotton rats (Sigmodon hispidus) were collected at some locations. The plutonium concentrations in soil at the selected locations ranged from 1.5 to 171fCi/g and alpha percentages of 238 Pu ranged from 2 to 66. The concentration of plutonium in the vegetation and on the leaves ranged from 0.17 to 76.1fCi/g and the alpha percentages of 238 Pu from 3 to 61. The concentration of plutonium in cotton rats and grasshoppers ranged from 0.07 to 3.58fCi/g and the alpha percentages of 238 Pu ranged from 22 to 80. The average ratio of plutonium concentration of vegetation to that of the surrounding soil was 10 -1 ; the corresponding ratio for cotton rats and soil was 10 -2 . These ratios appear to be independent of the plutonium concentration in the soil. Deposition on the surfaces of leaves and stems was the principal mechanism of plutonium contamination of vegetation. Comparisons among the plutonium values of the vegetation, soil and resuspendible fraction suggest the use of a proposed resuspendible measurement technique as a monitoring method to indicate subtle changes in the plutonium concentration of the soil surface that are not detectable by routine soil sampling. Although the 238 Pu data in the various ecosystem components were not conclusive, they do support evidence presented in other studies that there is an apparent increase in the biological availability of 238 Pu relative to that of sup(239,240)Pu in the environment. The plutonium concentrations of all ecosystem components decreased as the distance from the reprocessing plants increased. (author)

Individual economical value of plutonium isotopes and analysis of the reprocessing of irradiated fuel

International Nuclear Information System (INIS)

Gomes, I.C.; Rubini, L.A.; Barroso, D.E.G.

1983-01-01

An economical analysis of plutonium recycle in a PWR reactor, without any modification, is done, supposing an open market for the plutonium. The individual value of the plutonium isotopes is determined solving a system with four equations, which the unknow factors are the Pu-239, Pu-240, pu-241 and Pu-242 values. The equations are obtained equalizing the cost of plutonium fuel cycle of four different isotope mixture to the cost of the uranium fuel cycle. (E.G.) [pt

Selecting a plutonium vitrification process

Energy Technology Data Exchange (ETDEWEB)

Jouan, A. [Centre d`Etudes de la Vallee du Rhone, Bagnols sur Ceze (France)

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 of 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.

Calculation of keff for plutonium in high-level waste packages

International Nuclear Information System (INIS)

Zielinski, P.R.; Culbreth, W.G.

1994-01-01

The proposed national high-level nuclear waste repository will be designed to store approximately 70,000 tons of commercial spent fuel, but other forms of waste will also be considered for ultimate storage at this site. Plutonium in the form of PuO 2 may be added to borosilicate glass for ultimate disposal in the repository. The maximum amount of this fissile that may be added to a glass ''log'' will be limited by its ability to sustain a chain reaction. In this study, the removal of neutron absorbers from a glass log and the subsequent possibility of water infiltration were studied to find corresponding neutron multiplication factors. Weight fractions of 1%, 2%, and 3% PuO 2 were analyzed in the study. The results show the maximum amount of plutonium fissile that may be safely added to a glass log under conditions that lead to leaching of the principal neutron absorbers from the glass

Assay of low-level plutonium effluents

International Nuclear Information System (INIS)

Hsue, S.T.; Hsue, F.; Bowersox, D.F.

1981-01-01

In the plutonium recovery section at the Los Alamos National Laboratory, an effluent solution is generated that contains low plutonium concentration and relatively high americium concentration. Nondestructive assay of this solution is demonstrated by measuring the passive L x-rays following alpha decay. Preliminary results indicate that an average deviation of 30% between L x-ray and alpha counting can be achieved for plutonium concentrations above 10 mg/L and Am/Pu ratios of up to 3; for plutonium concentrations less than 10 mg/L, the average deviation is 40%. The sensitivity of the L x-ray assay is approx. 1 mg Pu/L

Vapor pressure of plutonium carbide adsorbed on graphite

International Nuclear Information System (INIS)

Tallent, O.K.; Wichner, R.P.; Towns, R.L.; Godsey, T.T.

1984-09-01

An investigation was conducted to obtain data needed to make realistic estimates of plutonium contamination in the primary coolant system in High Temperature Gas-Cooled Reactors (HTGRs). The vapor pressure of plutonium over plutonium sesquicarbide (Pu 2 C 3 ) adsorbed on the surface of H-451 graphite was found to be defined by adsorption isotherms at test temperatures of 1000, 1200, and 1400 0 C. The vapor pressures at low concentrations of Pu 2 C 3 on the surface of the graphite were up to three orders of magnitude below that of pure Pu 2 C 3 at a given temperature. The heat of adsorption increases with decreasing Pu 2 C 3 surface coverage with the measured value at 0.05 μmol Pu 2 C 3 /m 2 being 107.9 kcal/mol. The Pu 2 C 3 concentration required for monolayer surface coverage on the graphite was found to be 3.27 μmol/m 2

Reaction of alkali nitrates with PuO2

International Nuclear Information System (INIS)

Yamashita, T.; Ohuchi, K.; Takahashi, K.; Fujino, T.

1990-01-01

Improvement of solubility of plutonium dioxide (PuO 2 ) in acid solution is important to establish the nuclear fuel reprocessing technique for uranium-plutonium mixed oxide fuels. If insoluble PuO 2 can be converted into any soluble plutonium compounds, problems arising from the fuel dissolution process will be reduced to a great extent. Alkali metal plutonates and alkaline-earth plutonates are known to have enhanced solubility in mineral acids. However, the reaction conditions to form such plutonates and characterization thereof are not well elucidated. Then the reactivity and reaction conditions to form lithium and sodium plutonates from their nitrates and PuO 2 were studied at temperatures between 500 and 900 degree C and alkali metal to plutonium atom ratios between 0.5 and 6 by means of thermogravimetry as well as X-ray diffraction technique. The reaction behavior of alkali plutonates will be discussed in comparison with corresponding alkali uranates

Plutonium isotopic determination from gamma-ray spectra

International Nuclear Information System (INIS)

Skourikhine, A.N.; Strittmatter, R.B.; Zardecki, A.

1998-01-01

The use of low- and medium-resolution room-temperature detectors for the nondestructive assay of nuclear materials has widespread applications to the safeguarding of nuclear materials. The challenge to using these detectors is the inherent difficulty of the spectral analysis to determine the amount of specific nuclear materials in the measured samples. This is especially true for extracting plutonium isotopic content from low- and medium-resolution spectral lines that are not well resolved. In this paper, neural networks trained by stochastic and singular value decomposition algorithms are applied to retrieve the plutonium isotopic content from a simulated NaI spectra. The simulated sample consists of isotopes 238 Pu, 239 Pu, 240 Pu, 241 Pu, 242 Pu, and 241 Am. It is demonstrated that the neutral network optimized by singular value decomposition (SVD) and stochastic training algorithms is capable of estimating plutonium content consistently resulting in an average error much smaller than the error previously reported

Plutonium in Southern Hemisphere Ocean Waters

Energy Technology Data Exchange (ETDEWEB)

Hirose, K. [Sophia University, Tokyo (Japan); Aoyama, M. [Meteorological Research Institute, Tsukuba (Japan); Gastaud, J.; Levy, I. [Marine Environment Laboratories, International Atomic Energy Agency (Monaco); Fukasawa, M. [Japan Agency for Marine-Earth Science and Technology Yokosuka (Japan); Kim, C. -S. [Environment Laboratories, International Atomic Energy Agency, Seibersdorf (Austria); Povinec, P. P. [Comenius University, Bratislava (Slovakia); Roos, P. [Riso National Laboratory, Roskilde (Denmark); Sanchez-Cabeza, J. A. [Universitat Autonoma de Barcelona, Bellaterra (Spain); Yim, S. A. [Korea Institute of Nuclear Safety, Daejeon (Korea, Republic of)

2013-07-15

Plutonium in seawater collected by the BEAGLE2003 cruise was determined using ICP-SF-MS and alpha spectrometry after Fe co-precipitation and radiochemical purification. Levels and distributions of dissolved plutonium activity concentrations in Southern Hemisphere ocean waters are summarized here, including historical data. Pu-239 concentrations in surface water of the central South Pacific (32.5{sup o}S) in 2003 were around 1 mBq/m{sup 3}. The {sup 239}Pu concentrations in the Indian Ocean surface waters (20{sup o}S) were similar to that in the South Pacific, whereas the {sup 239}Pu concentrations in the South Atlantic surface waters (30{sup o}S) were markedly lower than those in the South Pacific and Indian Oceans. The {sup 239}Pu vertical profile pattern was similar to that in the North Pacific subtropical gyre, although {sup 239}Pu concentrations in the deep South Pacific were significantly lower than those in the North Pacific. One of the dominant factors controlling plutonium distributions in the Southern Hemisphere oceans is biogeochemical processes including particle scavenging. (author)

Comments on the note by L.S. Nelson: ''unusually high (oxidizer/Pu) ratios in the macro-residues from plutonium droplet combustion''

International Nuclear Information System (INIS)

Allen, M.D.; Morgan, L.G.

1982-01-01

An alternative explanation for unusually high ratios of oxidizers/plutonium in the residues from plutonium droplet combustion is offered in response to a note by L.S. Nelson. Two additional experiments are suggested that would be helpful in clarifying the high oxidizer/Pu ratios. The first would be to measure the true surface area for a spherule after its explosion. The second is an experiment analogous to a gas analysis experiment. The conclusion is put forth that adsorbed gases are the most likely cause of the high O/M ratios described by Nelson

The study of reductive reextraction of plutonium in the Purex process

International Nuclear Information System (INIS)

Poczynajlo, A.

1985-01-01

The methods of separation of U and Pu in the Purex process and the thermodynamic and kinetic properties of Pu(4) reductants are discussed. The kinetic equation of the process of reductive reextraction of plutonium for the first order reaction with respect to Pu(4) is derived. The kinetics of plutonium reextraction with the use of uranium (4), ascorbic acid and other reductants has been studied. The necessity of application of the stoichiometric excess of reductant has been explained by simultaneously occured reoxidation process of plutonium. The method of calculation of the steady- state plutonium concentration profiles has been elaborated for counter-current separation of U and Pu in multistage contactor. 90 refs., 20 tabs., 29 figs. (author)

Determination of plutonium 241 in solutions of nuclear wastes

International Nuclear Information System (INIS)

Raymond, A.; Bilcot, J.B.; Poletiko, C.

1990-09-01

Determination of plutonium 241 in nuclear wastes is important because of long period and high energy of some daughter products. In this report are presented two quantitative analysis methods using both scintillation techniques: A complete method, in any case, by selective extraction of plutonium on an anionic resin allowing simultaneous determination of Pu 241 and the sum of other plutonium isotopes; a simplified method when alpha activity is higher than beta/gamma activity by liquid extraction with TTA. These methods are applied for analysis of 4 waste types: cement encapsulated wastes, bitumen encapsulated wastes, incineration ashes, leaching of encapsulated incineration ashes. In these 4 examples, Pu 241 activity is equal or higher than the sum of alpha plutonium isotope activity. Separation efficiency, measured from Pu 239 or with Pu 236 as tracer, is between 90 and 99% [fr

Criticality of mixtures of plutonium and high enriched uranium

International Nuclear Information System (INIS)

Grolleau, E.; Lein, M.; Leka, G.; Maidou, B.; Klenov, P.

2003-01-01

This paper presents a criticality evaluation of moderated homogeneous plutonium-uranium mixtures. The fissile media studied are homogeneous mixtures of plutonium and high enriched uranium in two chemical forms: aqueous mixtures of metal and mixtures of nitrate solutions. The enrichment of uranium considered are 93.2wt.% 235 U and 100wt.% 235 U. The 240 Pu content in plutonium varies from 0wt.% 240 Pu to 12wt.% 240 Pu. The critical parameters (radii and masses of a 20 cm water reflected sphere) are calculated with the French criticality safety package CRISTAL V0. The comparison of the calculated critical parameters as a function of the moderator-to-fuel atomic ratio shows significant ranges in which high enriched uranium systems, as well as plutonium-uranium mixtures, are more reactive than plutonium systems. (author)

Separation of Pu from soil prior to determination by ICP-MS

International Nuclear Information System (INIS)

Nygren, U.; Baxter, D.C.

2002-01-01

In the determination of plutonium in environmental materials by ICP-MS, chemical separation is often needed to remove, e.g., heavy sample matrices and interference from UH + on m/z 239. This separation can be, and often is, performed in the same way as for alpha-spectrometric analysis. There are, however, somewhat different demands on separation for ICP-MS compared to alpha-spectrometry, but so far little has been published on the optimisation of separation procedures for plutonium determination by ICP-MS. This paper describes the development of a separation procedure especially suited for the determination of Pu by ICP-MS. Focus has been on parameters such as chemical yield of plutonium and decontamination from uranium, as well as time requirements and ease of performance. The separation of plutonium was performed using various resins, such as anion exchange resin and extraction chromatographic materials. The procedures were carried out on water spiked with 238 U and 240 Pu to concentrations of approximately 300 ppb and 50 ppt, respectively. The basic separation procedure was: 1. Adjustment of oxidation state for Pu 2. Loading on column 3. Rinsing using 4*5 free column volumes (FCVs) of load solution - if needed in combination with 1*5 FCVs of an other rinsing agent 4. Elution of Pu - if needed followed by evaporation and dissolution in a solution suitable for ICP-MS determination 5. Determination by high resolution ICP-MS The elution of plutonium was performed using various media, based on either reduction of Pu(IV) to Pu(III) or complex formation. The chemical yield of plutonium and the decontamination from uranium for various resin/elution combinations can be seen in Figs. 1 and 2. It was found that the most efficient separation procedure in terms of yield and uranium decontamination was the combination of two extraction chromatographic materials, UTEVA followed by TRU, and elution of Pu by 0.1 % 1-hydroxyethane-1,1-diphosphonic acid (HEDPA). In this procedure

Spectroscopy of plutonium-organic complexes

International Nuclear Information System (INIS)

Richmann, M.K.; Reed, D.T.

1995-01-01

Information on the spectroscopy of plutonium-organic complexes is needed to help establish the speciation of these complexes under environmentally relevant conditions. Laser photoacoustic spectroscopy (LPAS) and absorption spectrometry were used to characterize the Pu(IV)-citrate and Pu(IV)-nitrilotriacetic acid (NTA) complexes at concentrations of 10 -3 --10 -7 M in aqueous solution. Good agreement was observed between the band shape of the LPAS and absorption spectra for the Pu(IV)-NTA complex. Agreement for the Pu(IV)-citrate complex was not quite as good. In both cases, a linear dependence of the LPAS signal on laser power and total concentration of the complexes was noted. This work is part of an ongoing research effort to study key subsurface interactions of plutonium-organic complexes

Trans-Uranium Doping Utilization for Increasing Protected Plutonium Proliferation of Small Long Life Reactor

Energy Technology Data Exchange (ETDEWEB)

Permana, Sidik [Research Laboratory for Nuclear Reactors, Tokyo Institute of Technology 2-12-1-N1-17, O-okayama, Meguro-ku, Tokyo 152-8550 (Japan); Nuclear and Biophysics Research Group, Department of Physics, Bandung Institute of Technology, Gedung Fisika, Jl. Ganesha 10, Bandung 40132 (Indonesia); Suud, Zaki [Nuclear and Biophysics Research Group, Department of Physics, Bandung Institute of Technology, Gedung Fisika, Jl. Ganesha 10, Bandung 40132 (Indonesia); Suzuki, Mitsutoshi [Japan Atomic Energy Agency, Nuclear Non-proliferation Science and Technology Center, 2-4 Shirane Shirakata, Tokai-mura, Ibaraki, 319-1195 (Japan)

2009-06-15

Scientific approaches are performed by adopting some methodologies in order to increase a material 'barrier' in plutonium isotope composition by increasing the even mass number of plutonium isotope such as Pu-238, Pu-240 and Pu-242. Higher difficulties (barrier) or more complex requirement for peaceful use of nuclear materials, material fabrication and handling and isotopic enrichment can be achieved by a higher isotopic barrier. Higher barrier which related to intrinsic properties of plutonium isotopes with even mass number (Pu-238, Pu-240 and Pu-242), in regard to their intense decay heat (DH) and high spontaneous fission neutron (SFN) rates were used as a parameter for improving the proliferation resistance of plutonium itself. Pu-238 has relatively high intrinsic characteristics of DH (567 W/kg) and SFN rate of 2660 n/g/s can be used for making a plutonium characteristics analysis. Similar characteristics with Pu-238, other even mass number of plutonium isotopes such as Pu-240 and Pu-242 have been shown in regard to SFN values. Those even number mass of plutonium isotope contribute to some criteria of plutonium characterization which will be adopted for present study such as IAEA, Pellaud and Kessler criteria (IAEA, 1972; Pellaud, 2002; and Kessler, 2004). The study intends to evaluate the trans-uranium doping effect for increasing protected plutonium proliferation in long-life small reactors. The development of small and medium reactor (SMR) is one of the options which have been adopted by IAEA as future utilization of nuclear energy especially for less developed countries (Kuznetsov, 2008). The preferable feature for small reactors (SMR) is long life operation time without on-site refueling and in the same time, it includes high proliferation resistance feature. The reactor uses MOX fuel as driver fuel for two different core types (inner and outer core) with blanket fuel arrangement. Several trans-uranium doping and some doping rates are evaluated

Uncertainty assessment in gamma spectrometric measurements of plutonium isotope ratios and age

Energy Technology Data Exchange (ETDEWEB)

Ramebaeck, H., E-mail: henrik.ramebeck@foi.se [Swedish Defence Research Agency, FOI, Division of CBRN Defence and Security, SE-901 82 Umea (Sweden); Chalmers University of Technology, Department of Chemical and Biological Engineering, Nuclear Chemistry, SE-412 96 Goeteborg (Sweden); Nygren, U.; Tovedal, A. [Swedish Defence Research Agency, FOI, Division of CBRN Defence and Security, SE-901 82 Umea (Sweden); Ekberg, C.; Skarnemark, G. [Chalmers University of Technology, Department of Chemical and Biological Engineering, Nuclear Chemistry, SE-412 96 Goeteborg (Sweden)

2012-09-15

A method for the assessment of the combined uncertainty in gamma spectrometric measurements of plutonium composition and age was evaluated. Two materials were measured. Isotope dilution inductively coupled plasma sector field mass spectrometry (ID-ICP-SFMS) was used as a reference method for comparing the results obtained with the gamma spectrometric method for one of the materials. For this material (weapons grade plutonium) the measurement results were in agreement between the two methods for all measurands. Moreover, the combined uncertainty in all isotope ratios considered in this material (R{sub Pu238/Pu239}, R{sub Pu240/Pu239}, R{sub Pu241/Pu239}, and R{sub Am241/Pu241} for age determination) were limited by counting statistics. However, the combined uncertainty for the other material (fuel grade plutonium) were limited by the response fit, which shows that the uncertainty in the response function is important to include in the combined measurement uncertainty of gamma spectrometric measurements of plutonium.

Cost-benefit analysis of unfired PuO2 pellets as an alternative plutonium shipping form

International Nuclear Information System (INIS)

Mishima, J.; Brackenbush, L.W.; Libby, R.A.; Soldat, K.L.; White, G.D.

1983-10-01

A limited cost-benefit evaluation was performed concerning use of unfired plutonium dioxide pellets as a shipping form. Two specific processing operations are required for this use, one to form the pellet (pelletizing) and a second to reconstitute an acceptable powder upon receipt (reconstitution). The direct costs for the pelletizing operation are approximately $208,000 for equipment and its installation and $122 per kg of plutonium processed (based upon a 20-kg plutonium/day facility). The direct costs for reconstitution are approximately $90,000 for equipment and its installation and $81 per kg of plutonium processed. The indirect cost considered was personnel exposure from these operations. Whole body exposures ranged from 0.04 man-rem per 100 kg of low-exposure plutonium reconstituted to 0.9 man-rem per 100 kg of average-exposure plutonium pelletized. Hand exposures were much higher - 17 man-rem power 100 kg of low-exposure plutonium reconstituted to 67 man-rem per 100 kg of average plutonium pelletized. The principal benefit is a potential twentyfold reduction of airborne release in the event of an accident. An experimental plan is outlined to fill the data gaps uncovered during this study in the areas of pelletizing and reconstitution process parameters and pellet response behavior to accident-generated stresses. A study to enhance the containment potential of the inner packaging used during shipment is also outlined

Separation of plutonium oxide nanoparticles and colloids

Energy Technology Data Exchange (ETDEWEB)

Wilson, Richard E.; Skanthakumar, S.; Soderholm, L. [Argonne National Laboratory, IL (United States). Chemical Sciences and Engineering Division

2011-11-18

Colloidal plutonium is an important component of Pu aqueous speciation. Pu colloids are problematic in nuclear separations and are a potential transport vector in the environment. Using a mixture of n-octanol and trichloroacetic acid a selective and reversible separation of these particles can be achieved by exploiting their surface reactivity. [German] Kolloidales Plutonium ist ein wichtiger Bestandteil in waessrigen Pu-Bereitungen. Pu-Kolloide sind problematisch bei der Wiederaufbereitung von Kernmaterial und bilden einen potenziellen Transportvektor in die Umwelt. Mit einem Loesungsmittelgemisch aus n-Octanol und Trichloressigsaeure gelingt die selektive und reversible Trennung dieser Partikel durch Ausnutzung ihrer Oberflaechenreaktivitaet.

The growth and evolution of thin oxide films on delta-plutonium surfaces

Energy Technology Data Exchange (ETDEWEB)

Garcia Flores, Harry G [Los Alamos National Laboratory; Pugmire, David L [Los Alamos National Laboratory

2009-01-01

The common oxides of plutonium are the dioxide (PuO{sub 2}) and the sesquioxide (Pu{sub 2}O{sub 3}). The structure of an oxide on plutonium metal under air at room temperature is typically described as a thick PuO{sub 2} film at the gas-oxide interface with a thinner PuO{sub 2} film near the oxide-metal substrate interface. In a reducing environment, such as ultra high vacuum, the dioxide (Pu{sup 4+}; O/Pu = 2.0) readily converts to the sesquioxide (Pu{sup 3+}; O/Pu = 1.5) with time. In this work, the growth and evolution of thin plutonium oxide films is studied with x-ray photoelectron spectroscopy (XPS) under varying conditions. The results indicate that, like the dioxide, the sesquioxide is not stable on a very clean metal substrate under reducing conditions, resulting in substoichiometric films (Pu{sub 2}O{sub 3-y}). The Pu{sub 2}O{sub 3-y} films prepared exhibit a variety of stoichiometries (y = 0.2-1) as a function of preparation conditions, highlighting the fact that caution must be exercised when studying plutonium oxide surfaces under these conditions and interpreting resulting data.

Long time contamination from plutonium

International Nuclear Information System (INIS)

Fueloep, M.; Patzeltova, N.; Ragan, P.; Matel, L.

1995-01-01

Plutonium isotopes in the organism of the patient (who had participated in the liquidation works after the Chernobyl accident; for three month he had stayed in the epicenter, where he acted as a chauffeur driving a radioactive material to the place of destination) from urine were determined. For determination of the concentration of Pu-239, Pu-240 in urine a modified radiochemical method was used. After mineralization the sample was separated as an anion-nitrate complex with contact by the anion form of the resin in the column. The resin was washed by 8 M HNO 3 , the 8 M HCl with 0.3 M HNO 3 for removing the other radionuclides. The solution 0.36 M HCl with 0.01 M HF was used for the elution of plutonium. Using the lanthanum fluoride technique the sample was filtrated through a membrane filter. The plutonium was detected in the dry sample. The Pu-239 tracer was used for the evaluation of the plutonium separation efficiency. The alpha spectrometric measurements were carried out with a large area silicon detector. The samples were measured and evaluated in the energy region 4.98-5.18 MeV. The detection limit of alpha spectrometry measurements has been 0.01 Bq dm -3 . The concentration of plutonium in the 24-hour urine was determined three times in the quarter year intervals. The results are: 54 mBq, 63.2 mBq, 53 mBq, with average 56,7 mBq. From the results of the analyses of plutonium depositions calculated according to ICRP 54 the intake of this radionuclide for the patient was 56.7 kBq. To estimate a committed effective dose (50 years) from the intake of plutonium was used a conversion factor 6.8.10 -5 Sv.Bq -1 (class W). So the expressed committed effective dose received from the plutonium intake is 3.8 Sv. This number is relatively high and all the effective dose will be higher, because the patient was exposed to the other radionuclides too. For example the determination of the rate radionuclides Am-241/Pu-239,Pu-240 was 32-36 % in the fallout after the Chernobyl

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

Science.gov (United States)

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.

Solid-phase extraction of plutonium in various oxidation states from simulated groundwater using N-benzoylphenylhydroxylamine

International Nuclear Information System (INIS)

Perevalov, S.A.; Malofeeva, G.I.; Kuzovkina, E.V.; Spivakov, B.Ya.

2013-01-01

Solid-phase extraction of plutonium in different individual and mixed oxidation states from simulated groundwater (pH 8.5) was studied. The extraction of plutonium species was carried out in a dynamic mode using DIAPAK C16 cartridges modified by N-benzoylphenylhydroxylamine (BPHA). It was shown that the extent of recovery depends on the oxidation state of plutonium. The extraction of Pu(IV) was at the level of 98-99% regardless of the volume and flow-rate of the sample solution. Pu(V) was extracted by 90-95% and 75-80% from 10- and 100-mL aliquots of the samples, respectively, whereas the extraction of Pu(VI) did not exceed 45-50%. An equimolar mixture of Pu(IV), Pu(V), and Pu(VI) was extracted by 74%. The distribution coefficients (K d ) and kinetic exchange capacities (S) of plutonium in various oxidation states were measured. It was found that during the sorption process, Pu(V) was reduced to Pu(IV) by 80-90% after an hour-long contact with the solid phase. Pu(VI) is reduced to Pu(V) by 34% and to Pu(IV) by 55%. In the case of mixed-valent solution of plutonium, only Pu(V) and Pu(IV) were found in the effluents. (author)

Adsorption-desorption characteristics of plutonium and americium with sediment particles in the estuarine environment: studies using plutonium-237 and americium-241

International Nuclear Information System (INIS)

Murray, C.N.; Fukai, R.

1975-01-01

The particle formation of plutonium and americium, their adsorption onto fresh water sediments and the desorption from the sediments in sea water were studied in the Laboratory under simulated river-estuary conditions, using γ-emitting plutonium-237 and americium-241. The results of the experiments show that the particle formation of plutonium depends on its valence states, on pH and on the salinity of the medium. For river water at pH4, some 25%, 20% and 30% of the added 237 Pu was in particulate form, larger than 0.45 μm, for Pu (III), Pu (IV) and Pu (VI), respectively, while 65%, 90% and 50% of the respective valence states was associated with particles at pH 8. In sea water the general pattern remains similar, although Pu (VI) is more soluble in sea water owing to higher ligand concentrations for carbonate and bicarbonate complexes. The pH-dependency of particle formation of Am (III) is more steep than that of plutonium and seems to be influenced by colloidal substances occurring in the experimental media. The adsorption-desorption characteristics of plutonium and americium with the sediment in river water as well as sea water reflect the characteristics of their particle formation, being dependent upon such properties as valence states, the pH and salinity of the medium. A sewage effluent added to the media has small but measurable effects on the adsorption-desorption processes of plutonium. (author)

Electrochemical investigations of Pu(IV)/Pu(III) redox reaction using graphene modified glassy carbon electrodes and a comparison to the performance of SWCNTs modified glassy carbon electrodes

International Nuclear Information System (INIS)

Gupta, Ruma; Gamare, Jayashree; Sharma, Manoj K.; Kamat, J.V.

2016-01-01

Highlights: • First report of aqueous electrochemistry of Plutonium on graphene modified electrode. • Graphene is best electrocatalytic material for Pu(IV)/Pu(III) redox couple among the reported modifiers viz. reduced graphene oxide (rGO) and SWCNT’s. • The electrochemical reversibility of Pu(IV)/Pu(III) redox couple improves significantly on graphene modified electrode compared to previously reported rGO & SWCNTs modified electrodes • Donnan interaction between plutonium species and graphene surface offers a possibility for designing a highly sensitive sensor for plutonium • Graphene modified electrode shows higher sensitivity for the determination of plutonium compared to glassy carbon and single walled carbon nanotube modified electrode - Abstract: The work reported in this paper demonstrates for the first time that graphene modified glassy carbon electrode (Gr/GC) show remarkable electrocatalysis towards Pu(IV)/Pu(III) redox reaction and the results were compared with that of single-walled carbon nanotubes modified GC (SWCNTs/GC) and glassy carbon (GC) electrodes. Graphene catalyzes the exchange of current of the Pu(IV)/Pu(III) couple by reducing both the anodic and cathodic overpotentials. The Gr/GC electrode shows higher peak currents (i p ) and smaller peak potential separation (ΔE p ) values than the SWCNTs/GC and GC electrodes. The heterogeneous electron transfer rate constants (k s ), charge transfer coefficients (α) and the diffusion coefficients (D) involved in the electrocatalytic redox reaction were determined. Our observations show that graphene is best electrocatalytic material among both the SWCNTs and GC to study Pu(IV)/Pu(III) redox reaction.

Determination of the stability constant for the Pu(IV)-dinitrato complex using UV-VIS spectrophotometry

International Nuclear Information System (INIS)

Smith, C.A.; Veirs, D.K.

1994-01-01

Efficiency of the anion exchange process for the separation of plutonium is critically dependent upon the formation of the specific Pu(IV) nitrate complexes. Previous work is ambiguous as to the identification of the principal Pu(IV)-nitrate species present in nitric acid solutions. In this work, the authors study the nitrate complexes within the inner coordination sphere of Pu(IV) using absorption spectroscopy (nitrates in the outer coordination sphere probably do not affect the Pu(IV) absorption spectrum). The authors show that the Pu(IV)-aquo and -dinitrato species are associated with major peaks in the absorption spectrum at 469 and 476 nm, respectively. Absorption data from solutions where the nitrate concentration is varied at constant ionic strength are used to calculate stability constants for the dinitrato species, β 2 . Calculation of the stability constant at zero ionic strength and ion interaction coefficients are discussed

PLUTONIUM LOADING CAPACITY OF REILLEX HPQ ANION EXCHANGE COLUMN - AFS-2 PLUTONIUM FLOWSHEET FOR MOX

Energy Technology Data Exchange (ETDEWEB)

Kyser, E.; King, W.; O' Rourke, P.

2012-07-26

Radioactive plutonium (Pu) anion exchange column experiments using scaled HB-Line designs were performed to investigate the dependence of column loading performance on the feed composition in the H-Canyon dissolution process for plutonium oxide (PuO{sub 2}) product shipped to the Mixed Oxide (MOX) Fuel Fabrication Facility (MFFF). These loading experiments show that a representative feed solution containing {approx}5 g Pu/L can be loaded onto Reillex{trademark} HPQ resin from solutions containing 8 M total nitrate and 0.1 M KF provided that the F is complexed with Al to an [Al]/[F] molar ratio range of 1.5-2.0. Lower concentrations of total nitrate and [Al]/[F] molar ratios may still have acceptable performance but were not tested in this study. Loading and washing Pu losses should be relatively low (<1%) for resin loading of up to 60 g Pu/L. Loading above 60 g Pu/L resin is possible, but Pu wash losses will increase such that 10-20% of the additional Pu fed may not be retained by the resin as the resin loading approaches 80 g Pu/L resin.

Reduction of uranium and plutonium oxides by aluminum. Application to the recycling of plutonium; Reduction des oxydes d'uranium et de plutonium par l'aluminium application au recyclage du plutonium

Energy Technology Data Exchange (ETDEWEB)

Gallay, J [Commissariat a l' Energie Atomique, Valduc (France). Centre d' Etudes

1968-07-01

A process for treating plutonium oxide calcined at high temperatures (1000 to 2000 deg. C) with a view to recovering the metal consists in the reduction of this oxide dissolved in a mixture of aluminium, sodium and calcium fluorides by aluminium at about 1180 deg. C. The first part of the report presents the results of reduction tests carried out on the uranium oxides UO{sub 2} and U{sub 3}O{sub 8}; these are in agreement with the thermodynamic calculations of the exchange reaction at equilibrium. The second part describes the application of this method to plutonium oxides. The Pu-Al alloy obtained (60 per cent Pu) is then recycled in an aqueous medium. (author) [French] Un procede de traitement de l'oxyde de plutonium calcine a haute temperature (1000 deg. C a 2000 deg. C), en vue de la recuperation du metal, consiste a reduire cet oxyde dissous dans un melange de fluorures d'aluminium, de sodium et de calcium, par l'aluminium vers 1180 deg. C. Une premiere partie du rapport presente les resultats des essais de reduction des oxydes d'uranium UO{sub 2} et U{sub 3}O{sub 8}, en accord avec les resultats du calcul thermodynamique de la reaction d'echange a l'equilibre. Une seconde partie rend compte de l'application de cette methode a l'oxyde de plutonium. L'alliage Pu-Al obtenu (60 pour cent Pu) est ensuite recycle par voie aqueuse. (auteur)

Plutonium isotopes in the surface air in Japan

International Nuclear Information System (INIS)

Hirose, K.; Sugimura, Y.

1990-01-01

Plutonium isotope concentrations in the surface air at Tsukuba, Japan are reported during the period from 1981 to the end of 1986. The 239,240 Pu concentration in the surface air, which showed a marked seasonal variation with a spring maximum and fall minimum, decreased until the end of 1985 according to the stratospheric residence time of 1.15 years. In May 1986, elevated 239,240 Pu concentrations with high 238 Pu/ 239,240 Pu activity ratios were observed. The serial trend of plutonium concentration in the surface air is similar to the concentrations of the Chernobyl-released radionuclides. These findings suggest that a significant part of the plutonium in the surface air in May 1986 was due to the Chernobyl fallout. (author) 15 refs.; 2 figs.; 3 tabs

Airborne plutonium transported during southwesterly winds near the Hanford Prosser Barricade

International Nuclear Information System (INIS)

Sehmel, G.A.

1980-01-01

Airborne plutonium could result from resuspension of nuclear-weapons-testing stratospheric fallout deposition. To determine this possible resuspension at the Hanford site, two field experiments between April 12 to june 29, 1976 and August 12, 1976 to January 11, 1977 were conducted near the Prosser Barricade in the Hanford area about 19 to 22 km southeast (140 0 to 160 0 ) of the fuel-processing areas. The primary objective of these experimentss was to determine if stratospheric fallout resuspension was reflected by airborne plutonium concentrations increasing with increasing wind speed. A secondary objective was to confirm the source of the airborne plutonium by determining the plutonium-240 isotopic content or the plutonium-240/plutonium-239-mass ratio. Stratospheric fallout can be identified by the ratio of 240 Pu to other plutonium isotopes in surface soils. Plutonium was transported during southwesterly winds during the two study periods at the Prosser Barricade. Airborne 239 240 Pu concentrations varied as powers of wind speed (U):U -0 2 to U 7 8 . The airborne solids content ranged from 6 x 10 -8 to 1.7 x 10 -6 μCi/g. The 240 Pu isotopic content ranged from 5.6 to 8.1 atom percent and the 240 Pu/ 239 Pu mass ratio ranged from 0.065 to 0.089. The estimated fraction of stratospheric fallout plutonium in these samples was less than 0.24. The remaining airborne plutonium was probably of Hanford origin. Airborne plutonium probably represents resuspension of plutonium from undetermined sites by mechanisms and events not clear at present. An increasing airborne plutonium concentration with increasing wind speed might be expected for an upwind resuspension source(s). However, the geographical source(s) location was not investigated in this study

Electrochemistry of plutonium in molten halides

International Nuclear Information System (INIS)

McCurry, L.E.; Moy, G.M.M.; Bowersox, D.F.

1987-01-01

The electrochemistry of plutonium in molten halides is of technological importance as a method of purification of plutonium. Previous authors have reported that plutonium can be purified by electrorefining impure plutonium in various molten haldies. Work to eluciate the mechanism of the plutonium reduction in molten halides has been limited to a chronopotentiometric study in LiCl-KCl. Potentiometric studies have been carried out to determine the standard reduction potential for the plutonium (III) couple in various molten alkali metal halides. Initial cyclic voltammetric experiments were performed in molten KCL at 1100 K. A silver/silver chloride (10 mole %) in equimolar NaCl-KCl was used as a reference electrode. Working and counter electrodes were tungsten. The cell components and melt were contained in a quartz crucible. Background cyclic voltammograms of the KCl melt at the tungsten electrode showed no evidence of electroactive impurities in the melt. Plutonium was added to the melt as PuCl/sub 3/, which was prepared by chlorination of the oxide. At low concentrations of PuCl/sub 3/ in the melt (0.01-0.03 molar), no reduction wave due to the reduction of Pu(III) was observed in the voltammograms up to the potassium reduction limit of the melt. However on scan reversal after scanning into the potassium reduction limit a new oxidation wave was observed

Plutonium uptake by the green alga Scenedesmus obliquus (Turp) Kutz, as a function of isotope and oxidation state

Energy Technology Data Exchange (ETDEWEB)

Tkacik, M.F.

1977-01-01

This study was designed to determine the effect of plutonium chemical valence state on the availability of small concentrations of /sup 238/Pu and /sup 239/Pu to algae. The uptake experiments involved the green alga Scenedesmus obliquus, grown in batch cultures. Plutonium concentrations accumulated by this alga were linearly related to plutonium concentrations. There was no significant difference (rho = 0.05) in algal plutonium accumulations, on a mass basis, of either /sup 238/Pu or /sup 239/Pu in either Pu/sup +4/ or Pu/sup +6/ oxidation state at the concentrations studied.

Plutonium uptake by the green alga Scenedesmus obliquus (Turp) Kutz, as a function of isotope and oxidation state

International Nuclear Information System (INIS)

Tkacik, M.F.

1977-01-01

This study was designed to determine the effect of plutonium chemical valence state on the availability of small concentrations of 238 Pu and 239 Pu to algae. The uptake experiments involved the green alga Scenedesmus obliquus, grown in batch cultures. Plutonium concentrations accumulated by this alga were linearly related to plutonium concentrations. There was no significant difference (rho = 0.05) in algal plutonium accumulations, on a mass basis, of either 238 Pu or 239 Pu in either Pu +4 or Pu +6 oxidation state at the concentrations studied

Studies of plutonium and the lymphatic system: six years of progress at Colorado State University

International Nuclear Information System (INIS)

Lebel, J.L.; Bistline, R.W.; Schallberger, J.A.; Dagle, G.E.; Gomez, L.S.

1976-01-01

Air-oxidized PuO 2 , high-fired (850 0 C) PuO 2 , Pu(NO 3 ) 4 , PuF 4 , and PuCl 3 , all of which had known amounts of 241 Am, were implanted over the left metacarpus of beagles. The concentration of plutonium and 241 Am in various tissues was measured as a function of time. The effect of diethylenetriaminepentaacetate (DTPA) therapy on organ deposition was studied. Significant differences in the translocation dynamics of air-oxidized PuO 2 , high-fired PuO 2 , and Pu(NO 3 ) 4 in the left superficial cervical lymph node (LSCLN) were observed by in vivo measurement and radiochemical analysis. A 3 percent buildup of plutonium was observed 2 weeks after implantation of air-oxidized PuO 2 , with an exponential buildup to 17 percent at 1 year. With Pu(NO 3 ) 4 and high-fired PuO 2 , the activity accumulation built up to a peak of 31 and 20 percent, respectively, at 30 and 60 days after implantation, followed by a gradual regression. At the implant site 1 year postimplant, a 70 percent reduction in activity was observed with Pu(NO 3 ) 4 , a 90 percent reduction with PuO 2 (high-fired), and only a 20 percent reduction with air-oxidized PuO 2 . The effect of larger particle size on the movement of plutonium from a wound site was speculated. Chemical form and physical form appear to change the rate of translocation and relative depositions of plutonium and americium in various organs.Particle size was not found to be an important factor in the total movement of plutonium in afferent and efferent lymph. More plutonium moves in the cellular fraction of afferent and efferent lymph regardless of particle size. The clearance of plutonium particles from the lymph nodes was associated with necrosis of macrophages. The effect of DTPA therapy on plutonium concentration was greater for the nitrate than for the other chemical forms

Partial equilibrium in induced redox reactions of plutonium

Energy Technology Data Exchange (ETDEWEB)

Nikol' skii, B P; Posvol' skii, M V; Krylov, L I; Morozova, Z P

1975-01-01

A study was made of oxidation-reduction reactions of Pu in buffer solutions containing bichromate and a reducing agent which reacted with hexavalent chromium at pH=3.5. In most cases sodium nitrite was used. A rather slow reduction of Pu (6) with NaNO/sub 2/ in the course of which tetravalent plutonium was formed via disproportionation reaction of plutonium (5), became very rapid upon the addition of bichromate to the solution. The yield of tetravalent plutonium increased with an increase in the concentration of NaNO/sub 2/ and the bichromate but never reached 100%. This was due to a simultaneous occurrenc of the induced oxidation reaction of Pu(4), leading to a partial equilibrium between the valence forms of plutonium in the nitrite-bichromate system which on the whole was in a nonequilibrium state. It was shown that in the series of reactions leading to the reduction of plutonium the presence of bivalent chromium was a necessary link.

Radiolysis of Salts and Long-Term Storage Issues for Both Pure and Impure PuO{sub 2} Materials in Plutonium Storage Containers

Energy Technology Data Exchange (ETDEWEB)

Lav Tandon

2000-05-01

The Material Identification and Surveillance (MIS) project sponsored a literature search on the effects of radiation on salts, with focus on alkali chlorides. The goal of the survey was to provide a basis for estimating the magnitude of {alpha} radiation effects on alkali chlorides that can accompany plutonium oxide (PuO{sub 2}) into storage. Chloride radiolysis can yield potentially corrosive gases in plutonium storage containers that can adversely affect long-term stability. This literature search was primarily done to provide a tutorial on this topic, especially for personnel with nonradiation chemistry backgrounds.

Diffusion and Kirkendall effect in plutonium-zirconium system; Diffusion et effet Kirkendall dans le systeme plutonium-zirconium

Energy Technology Data Exchange (ETDEWEB)

Remy, C [Commissariat a l' Energie Atomique, Fontenay-aux-Roses (France). Centre d' Etudes Nucleaires

1968-10-01

Results are reported for the chemical diffusion in {epsilon}{beta} phase (bcc) over the range 10 - 70 atomic per cent plutonium. Concentration-penetration curves, obtained by using electron microprobe, have been analysed by Hall and Matano methods. Chemical diffusion coefficients, measured from 650 to 900 deg. C., increase with plutonium concentration and follow the Arrhenius law. Activation energies range from 18000 up to 44000 cal/mole for plutonium concentrations from 60 to 20 atomic per cent plutonium. Kirkendall effect has been observed by the shift of inert markers located originally at the Zr-PuZr interface. Analysis of intrinsic diffusion coefficients variation, flux of the two species and lattice velocity has been carried out by the incremental couples technique by using Darken and Heumann equations. It was found that D{sub Pu} > D{sub Zr}; the ratio D{sub Pu}/D{sub Zr} increases from 1 to 6 over the range 15 - 60 atomic per cent Pu. Activation energies for intrinsic diffusion coefficients vary between 25 and 50 Kcal/mole. (author) [French] Nous donnons des resultats sur la diffusion chimique en phase {epsilon}{beta} (cc) de 10 a 70 pour cent atomique en plutonium. Les courbes concentration-penetration, obtenues par microanalyse X ont ete depouillees par les methodes de HALL et de MATANO. Les coefficients de diffusion chimique mesures de 650 deg. C a 900 deg. C., augmentent avec la concentration en plutonium et suivent la loi d'ARRHENIUS. Les energies d'activation passent de 18000 a 44000 calories par mole pour des concentrations de 60 a 20 pour cent atomique en plutonium. L'existence d'un effet KIRKENDALL a ete mis en evidence par le deplacement de fils inertes places initialement dans le plan de soudure. L'analyse de la variation des coefficients de diffusion intrinseques, des flux des deux especes et de la vitesse du reseau a ete faite par la technique des couples incrementaux en utilisant les equations de DARKEN et de HEUMANN. On trouve D{sub Pu} > D

Recent trends of plutonium facilities and their control

Energy Technology Data Exchange (ETDEWEB)

Muto, T [Power Reactor and Nuclear Fuel Development Corp., Tokai, Ibaraki (Japan). Tokai Works

1974-02-01

Much interest has been focussed on Pu recycle since the oil crisis because of an expected shortage of enriched uranium. Plutonium handling techniques and plutonium fuel fabricating facilities should be developed to meet the future demand of plutonium, but the radioactive property of plutonium to be reprocessed from spent fuel and recycled plutonium is remarkably different, and it has to be handled safely. Technical criteria for plutonium facilities are specified in the USAEC regulatory guides and other rules. Some of these criteria are location condition, quality of confinement, protection against accidents and so on. The control conditions for plutonium facilities are exposure control, criticality control, measurement control and new system of safeguard. These problems are under development to meet the future requirement for the safe handling of Pu material.

The chemistry of plutonium in sol-gel processes

International Nuclear Information System (INIS)

Lloyd, M.H.; Haire, R.G.

1978-01-01

Studies of plutonium chemical behavior conducted in conjunction with plutonia sol-gel process development at ORNL are described. The colloidal solutions produced consist of 'Pu(IV) polymer,' and this is therefore the study of polymeric plutonium behavior. Spectrophotometric, electron diffraction, and electron microscopy studies, in addition to specific studies that were concerned with the colloidal behavior of Pu(IV) polymer, indicate several characteristics of polymer that are not generally recognized. The particle nature of Pu(IV) polymer indicated by electron microscopy, the amorphous-crystalline characteristics of primary polymer particles demonstrated by electron diffraction, and the reversible and irreversible aggregation of the primary particles shown by spectrophotometric techniques present a useful view of the nature of Pu(IV) polymer that has been helpful in solving or understanding various types of processing problems involving plutonium hydrolytic behavior. The colloidal characteristics of Pu(IV) polymer and crystallite growth of primary polymer particles by thermal denitration are also described. (orig.) [de

Comparison of U-Pu-Mo, U-Pu-Nb, U-Pu-Ti and U-Pu-Zr alloys

International Nuclear Information System (INIS)

Boucher, R.; Barthelemy, P.

1964-01-01

The data concerning the U-Pu, U-Pu-Mo and U-Pu-Nb are recalled. The results obtained with U-Pu-Ti and U-Pu-Zr alloys containing 15-20 per cent Pu and 10 wt. per cent ternary element are reported. The transformation temperatures, the expansion coefficients, the nature of phases, the thermal cycling behaviour have been determined. A list of the principal properties of these different alloys is presented and the possibilities of their use as fast reactor's fuel element are considered. The U-Pu-Ti alloys seem to be quite promising: easiness of fabrication, large thermal stability, excellent behaviour in air, small quantity of zeta phase, temperature of solidus superior to 1100 deg. C. (authors) [fr

Sorption of 237Pu by the diatom Asterionella formosa

International Nuclear Information System (INIS)

Conway, H.L.; Wahlgren, M.A.; Peterson, N.; Nelson, D.M.

1976-01-01

Knowledge of the behavior of the man-made radionuclide plutonium within aquatic environments is of fundamental importance in assessing its potential hazards and ecological impact. The sorption of plutonium by phytoplankton and other algae is the dominant factor in the biological transport of plutonium in the aquatic environment, and it has been suggested that sorption by phytoplankton may be responsible for the seasonal loss of plutonium from the epilimnion of Lake Michigan. A unialgal diatom culture was spiked with 237 Pu tracer solution in an attempt to simulate the behavior of fallout plutonium observed in field studies. The results were encouraging in that the 237 Pu in the filtered lake water medium exhibited strongly anionic properties similar to fallout plutonium in Lake Michigan, with limited sorption on container walls. The purpose of the present study was to extend the investigations of the sorption of plutonium by phytoplankton in a controlled environment using continuous culture techniques

``Distribution and behaviour of plutonium in the waters of the channel and of the seine estuary``; ``Distribution et comportement du plutonium dans les eaux de la manche et de l`estuaire de la seine``

Energy Technology Data Exchange (ETDEWEB)

Garcia, K

1998-12-31

Excess dissolved plutonium has been measured in the coastal waters of the Channel, from Granville to Boulogne, probably due to sorption-desorption processus. In the Seine estuary, in situ measurements and experimental studies showed that the plutonium desorbs himself from particles in low salinity waters. The desorbed plutonium originates in marine and/or fluvial dissolved Pu. Marine dissolved Pu(V), originating from La Hague plant discharges and from atlantic waters, is reduced and sorbed when the salinity decreases onto estuarial particles: Isotopic Activity Ration {sup 238}Pu/{sup 239}, Pu(IR) of marine dissolved Pu(V) is about 0.7. Fluvial dissolved plutonium originates from atmospheric fallout and from an internal river source: fallout plutonium (IR=0.05) is unreactive with salinity while 45% of river plutonium (IR>1.7) flocculates at 0.5 g l{sup -1}. Desorbed plutonium may have various origins, depending on the Seine liquid discharges and on the tidal coefficient. When the marine waters do not migrate upstream, the low salinity waters encounters particles marked essentially with marine plutonium and the IR of desorbed Pu is about 0.7. The activities of desorbed plutonium are too low to have any influence on the distribution of plutonium in the coastal waters on the Seine Bay. When the marine waters migrate upstream, the low salinity waters meet particles marked essentially with river plutonium (IR>1.7) and desorbed plutonium has a very high IR. These estuarine conditions are encountered five to seven month a year and implicate an increase of the IR of 0.1 of the plutonium present in the coastal waters of the Seine bay (1.2.-1.3.). (author).

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

Science.gov (United States)

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

Science.gov (United States)

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

239 240Pu in Lake Michigan: 1971 to 1978

International Nuclear Information System (INIS)

Wahlgren, M.A.; Nelson, D.M.; Orlandini, K.A.; Kucera, E.T.

1978-01-01

The plutonium concentration data presented previously have consisted primarily of results from studies of short-term variations, i.e., the annual plutonium cycle conducted at Lake Michigan station ANL-5, 12 km SW of Grand Haven, Michigan. In this report, mean annual concentrations of total plutonium in unfiltered water from far off-shore (> 30 km) stations for the period 1971 through 1977, and from station ANL-5 (1975 through 1978) are summarized to establish the long-term trend in plutonium concentration in Lake Michigan. The results presented show that the mean annual concentration in the water column is similar at ANL-5 and at offshore stations and has decreased at the rate of only 6% per year during the period 1972 through 1978. The nearly constant concentration indicates that steady-state equilibria exist between plutonium inputs to the lake and the loss of plutonium from the water column. Observations suggest the existence of an active redox cycle for Pu in Lake Michigan. In this cycle, Pu IV atoms in solution are continually taken up by particulate materials but may be oxidized within microzones of the particles such as freshly deposited manganese coatings and also in solution by agents such as dissolved oxygen. In turn, the concentration of Pu VI in solution may be limited by reaction with reducing constituents of the coloidal-sized fraction (or decomposer organisms such as bacteria or fungi, which might have been present after filtration) and with planktonic organisms in the environment to produce Pu IV and thus maintain the cycle

Plutonium in intertidal coastal and estuarine sediments in the Northern Irish Sea

International Nuclear Information System (INIS)

Aston, S.R.; Assinder, D.J.; Kelly, M.

1985-01-01

Surface intertidal sediments from 35 sites in the Irish Sea have been analysed for their 238 Pu and sup(239,240)Pu activities, together with an intensive study of plutonium in sediments of the Esk Estuary (NW England). The range of plutonium activities for the whole survey were 0.14-4118 and 1.3-16 026 Bq kg -1 for 238 Pu and sup(239,240)Pu, respectively. The levels of Pu activity, derived from the Sellafield nuclear fuel reprocessing effluents, in sediments are controlled by lithological factors and the influence of transport and post-depositional processes. Grain size distribution is particularly important, the major part of plutonium activity being in the mud fraction of all sediments. The data suggest that over the Irish Sea coastline, dynamic mixing of sediment grains by reworking and resuspension and/or by dispersion in tidal currents are important in determining plutonium distributions. The exponential decrease in sediment plutonium activities away from the Sellafield source is attributed to the progressive mixing with older contaminated and uncontaminated sediments. (author)

Importance of 241 Am Determination in the Characterization of PuO2 Standards for Calorimetric Assay.

Energy Technology Data Exchange (ETDEWEB)

Sampson, Thomas E.

2005-01-01

Plutonium dioxide (PuO{sub 2}) standards are often used both as heat standards and isotopic standards for calorimetric assay. Calorimetric assay is the combination of the power in watts measured in a calorimeter with the effective specific power (P{sub eff}) in watts/g Pu, determined either by nondestructive gamma-ray assay or by destructive mass spectrometry, to yield the total elemental plutonium mass in the sample. To use a PuO{sub 2} sample as a heat standard for calorimetry, one must determine both the plutonium mass and P{sub eff} with very small uncertainties and then calculate the sample watts from the known plutonium mass, specific powers, and isotopic composition. Well-characterized PuO{sub 2} standards have plutonium mass values determined by analytical chemistry with a precision and accuracy on the order of 0.1%-0.2% relative to the total mass of the sample. Mass spectrometry, typically used to determine the isotopic fractions of plutonium standards, is very accurate and precise for the major isotopes but is somewhat less precise for low-abundance isotopes. The characterization of the {sup 241}Am/Pu ratio in the standard is also of great importance because {sup 241}Am can contribute significantly to P{sub eff} and to the heat output of the standard. The determination of the {sup 241}Am/Pu ratio in a plutonium-bearing sample is a process that is less standardized than mass spectrometry. There are no certified reference materials (CRMs) traceable to the national measurement system for {sup 241}Am in plutonium, and routine analytical {sup 241}Am/Pu ratio measurements often exhibit uncertainties of several percent relative to the total plutonium or greater.

Reduction stripping of plutonium (IV) with hydroxylamine nitrate in the centrifugal contactor

International Nuclear Information System (INIS)

Zhang Zefu; Ding Dachun; Fei Hongcheng

1989-01-01

Reduction stripping of Pu(IV) with hydroxylamine nitrate under conditions of Purex 3B contactor is carried out with 16-stage mixer-centrifugal settler in laboratory scale. Results show that the apparent recovery of Pu is more than 99.9%. But there is a great difference in the concentration of plutonium of every stage in extraction equipment at different temperature. For example, plutonium concentrations in organic phase of several stages near the organic effluent at 45-50 deg C are lower than that at 20-24 deg C. Thus, recovery efficiency of plutonium can be assured only for the former. However, plutonium will probably be lost, if operating conditions are fluctuated. In addition, plutonium accumulated in the extraction equipment increased appreciably for the case of 20-24 deg C. Therefore, in order to ensure recovery efficiency of Pu, reduction stripping of Pu should be made at higher temperature

Analytical determination of plutonium in the presence of complexing agents

International Nuclear Information System (INIS)

Nebel', D.

1975-01-01

The complexing of Pu(4) and Pu(6) with citrate and lactate were studied to establish possibilities which are provided by the complexing for analytical determination of plutonium in a solution. Plutonium in the sample analyzed is preliminarily reduced up to trivalent state. Then trivalent plutonium is oxidized up to tetravalent on the platinum electrode at +1.05 V. To avoid further oxidation complexing agents are added. The value of pH=2-4 is maintained to stabilize the oxidation degree. If hexavalent plutonium should be obtained, the oxidation is performed at the voltage of +1.5 V in the absence of complexing agents. Based on a detailed study of absorption spectra of plutonium complexes of various oxidation degrees it is stated that the most suitable for analytical purposes is the oxidation degree of Pu=4

Simulation study for purification, recovery of plutonium and uranium from plant streams of Fast Reactor Fuel Reprocessing Plant

International Nuclear Information System (INIS)

Sukumar, S.; Siva Kumar, P.; Radhika, R.; Subbuthai, S.; Mohan, S.V.; Subha Rao, R.V.

2005-01-01

A method for removal of plutonium from the lean organic streams obtained after co-stripping of uranium -plutonium was developed. Plutonium from lean organic phase was stripped using U 4+ /hydrazine as the stripping agent. The effect of concentrations of stripping agent U 4+ and feed Pu concentration in the lean organic phase was studied. Lean organic phases having higher plutonium concentration require three stages of stripping to bring plutonium concentration 4+ stabilized by hydrazine reduces Pu (IV) to Pu (III) thereby stripping plutonium from the organic phase. The non-extractability of Pu (III) by TBP was utilized for development of flow sheet for obtaining a uranium product lean of plutonium for ease of handling. (author)

Reanalysis of gastrointestinal absorption factors for plutonium and other actinide elements

International Nuclear Information System (INIS)

Bhattacharyya, M.H.; Larsen, R.P.; Toohey, R.E.; Moretti, E.S.; Oldham, R.D.; Spaletto, M.I.; Engel, M.C.

1981-01-01

This project studies the gastrointestinal absorption of plutonium and other actinide elements relevant to nuclear power production, at concentrations at or below their respective maximum permissible concentrations (MPC's) in drinking water, using high specific activity isotopes. The gastrointestinal absorption of plutonium is measured in mice, rats, and dogs exposed to plutonium either via drinking water or by gavage. Plutonium concentrations are determined in liver and eviscerated carcass at 6 days (mice and rats) or 4 weeks (dogs). Administered solutions are 1 x 10 -10 M in Pu (the molar concentration at MPC for 239 Pu) and contain one of several high specific activity isotopes ( 237 Pu, 47-day half-life; 236 Pu, 2.8-year half-life; 238 Pu, 86-year half-life). Fasted mice and rats, administered plutonium solutions that are: (1) low in concentration (10- 10 M); and (2) carefully prepared to assure a given oxidation state and to avoid hydrolysis and polymes, and major policy issues. The first HEED for near-term battery energy storage systems (lead/acid, nickel/zinc, and nickel/iron) astention being paid to potential releases of radionuclides at relatively short times after disposal

Plutonium determination by isotope dilution

International Nuclear Information System (INIS)

Lucas, M.

1980-01-01

The principle is to add to a known amount of the analysed solution a known amount of a spike solution consisting of plutonium 242. The isotopic composition of the resulting mixture is then determined by surface ionization mass spectrometry, and the plutonium concentration in the solution is deduced, from this measurement. For irradiated fuels neutronic studies or for fissile materials balance measurements, requiring the knowledge of the ratio U/Pu or of concentration both uranium and plutonium, it is better to use the double spike isotope dilution method, with a spike solution of known 233 U- 242 Pu ratio. Using this method, the ratio of uranium to plutonium concentration in the irradiated fuel solution can be determined without any accurate measurement of the mixed amounts of sample and spike solutions. For fissile material balance measurements, the uranium concentration is determined by using single isotope dilution, and the plutonium concentration is deduced from the ratio Pu/U and U concentration. The main advantages of isotope dilution are its selectivity, accuracy and very high sensitivity. The recent improvements made to surface ionization mass spectrometers have considerably increased the precision of the measurements; a relative precision of about 0.2% to 0.3% is obtained currently, but it could be reduced to 0.1%, in the future, with a careful control of the experimental procedures. The detection limite is around 0.1 ppb [fr

Influence of chemical form, feeding regimen, and animal species on the gastrointestinal absorption of plutonium

International Nuclear Information System (INIS)

Bhattacharyya, M.H.; Larsen, R.P.; Cohen, N.; Ralston, L.G.; Oldham, R.D.; Moretti, E.S.; Ayres, L.

1985-01-01

We evaluated the effect of chemical form and feeding regimen on the gastrointestinal (GI) absorption of plutonium in adult mice at plutonium concentrations relevant to the establishment of drinking water standards. Mean fractional GI absorption values in fasted adult mice were: Pu(VI) bicarbonate, 15 x 10 -4 ; Pu(IV) bicarbonate, 20 x 10 -4 ; Pu(IV) nitrate (pH2), 17 x 10 -4 ; Pu(IV) citrate, 24 x 10 -4 ; and Pu(IV) polymer, 3 x 10 -4 . Values in fed adult mice were: Pu(VI) bicarbonate, 1.4 x 10 -4 ; Pu(IV) polymer, 0.3 x 10 -4 . Pu(VI) is the oxidation state in chlorinated drinking waters and Pu(IV) is the oxidation state in many untreated natural waters. To assess the validity of extrapolating data from mice to humans, we also determined the GI absorption of Pu(VI) bicarbonate in adult baboons with a dual-isotope method that does not require animal sacrifice. Fractional GI absorption values obtained by this method were 23 +- 10 x 10 -4 for fasted baboons (n=5) and 1.4 +- 0.9 x 10 -4 for fed baboons (n=3). We have so far validated this method in one baboon and are currently completing validation in two additional animals. At low plutonium concentrations, plutonium oxidation state [Pu(VI) vs Pu(IV)] and administration medium (bicarbonate vs nitrate vs citrate) had little effect on the GI absorption of plutonium in mice. Formation of Pu(IV) polymers and animal feeding decreased the GI absorption of plutonium 5- to 10-fold. The GI absorption of Pu(VI) bicarbonate in both fed and fasted adult baboons appeared to be the same as in fed and fasted adult mice, respectively. 17 refs., 2 tabs

Vertical distribution of (241)Pu in the southern Baltic Sea sediments.

Science.gov (United States)

Strumińska-Parulska, Dagmara I

2014-12-15

The vertical distribution of plutonium (241)Pu in marine sediments can assist in determining the deposition history and sedimentation process of analyzed regions. In addition, (241)Pu/(239+240)Pu activity ratio could be used as a sensitive fingerprint for radioactive source identification. The present preliminary studies on vertical distribution of (241)Pu in sediments from four regions of the southern Baltic Sea are presented. The distribution of (241)Pu was not uniform and depended on sediment geomorphology and depth as well as location. The highest concentrations of plutonium were found in the surface layers of all analyzed sediments and originated from the Chernobyl accident. Copyright © 2014 Elsevier Ltd. All rights reserved.

Evaluating 239Pu levels using field detectors

International Nuclear Information System (INIS)

Wahl, L.E.; Smith, W.J. II; Martin, B.

1996-01-01

At Los Alamos National Laboratory, cleanup was planned at three septic tanks where surface soil in the outfall drainage areas was found to be contaminated with 239 Pu. To meet budget and deadline constraints, a technique was developed that used field instruments to verify 239 Pu soil contamination at levels less than 2.8 Bq g -1 , the established cleanup level. The drainage areas were surveyed using a low-energy gamma probe to identify likely areas of 239 Pu contamination. Between 40 and 135 0.1-min gamma radiation measurements were obtained from each drainage area. From these data, locations were identified for subsequent screening for alpha radioactivity. Soil samples from between 11 and 18 locations at each drainage area were placed in petri dishes, dried, and counted for 10 minutes using an alpha probe. Alpha counts were then related to 239 Pu concentrations using a curve developed from local soils containing known concentrations of 239 Pu. Up to six soil samples from each drainage area, representing a range of alpha radioactivity levels, were sent for laboratory analysis of isotopic plutonium to confirm field measurement results. Analytical and field results correlated well at all but one outfall area. At this area, field measurements predicted more 239 Pu than was measured in the laboratory, indicating the presence of another alpha-emitting radionuclide that might have been missed if only laboratory analyses for plutonium had been used. This technique, which combined a large number of gamma radioactivity measurements, a moderate number of alpha radioactivity measurements, and a few isotopic plutonium measurements, allowed quick and inexpensive comparison of 239 Pu with the cleanup level

Investigation on the attribute detection of plutonium oxide

International Nuclear Information System (INIS)

Liu Suping; Hao Fanhua; Gong Jian; Wu Huailong; Hu Guangchun; Hu Yongbo

2006-01-01

A long-term detection of the 871 keV gamma-ray emitted from two PuO 2 samples (100 g recovered powder and 8 g pure powder) has been conduced with a high resolution HPGe spectrometer in a lead-shielded chamber. An on-site detection of the 871 keV gamma-ray emitted from 200 g recovered PuO 2 powder has also been performed. Although the 871 keV peak can be observed in all 3 samples, other characteristic gamma-rays related to the existence of oxygen are not seen. The 871 keV peak is absent in spectra acquired from metal plutonium samples, which can answer whether the plutonium material in a sealed container is metal plutonium or plutonium oxide, i.e. the 871 keV gamma-ray can be an evidence for the absence of metal plutonium. The 871 keV peak is strong in the spectrum of 200 g recovered PuO 2 sample. A software of plutonium abundance and age analysis developed by ourselves can identify the 871 keV peak from a spectrum of 10 min. If the system is appropriately improved, it can be used to detect attribute of plutonium oxide through identifying 871 keV gamma-ray peak. (authors)

Plutonium in the air in Kurchatov, Kazakhstan

Energy Technology Data Exchange (ETDEWEB)

Lehto, J.; Salminen, S.; Jaakkola, T.; Outola, I.; Pulli, S. [Laboratory of Radiochemistry, P.O. Box 55, FIN-00014 University of Helsinki, Helsinki (Finland); Paatero, J. [Finnish Meteorological Institute, Helsinki (Finland); Tarvainen, M.; Ristonmaa, S. [Finnish Authority for Nuclear and Radiation Safety, Helsinki (Finland); Zilliacus, R. [Technical Research Centre of Finland, Espoo (Finland); Ossintsev, A.; Larin, V. [Institute of Radiation Safety and Ecology, Kurchatov (Kazakhstan)

2006-07-31

Weekly air samples of 25000 m{sup 3} volume were taken with two air samplers over a period of one year in 2000-2001 in the town of Kurchatov in Kazakhstan. For another three-month period in 2001, the samplers were run in the city of Astana, about 500 km west of Kurchatov. {sup 137}Cs, Pu and U concentrations were determined from the filters. Pu activities in Kurchatov varied in a 100-fold range; median {sup 239,240}Pu activities were 100 nBq/m{sup 3} and {sup 238}Pu activities 34 nBq/m{sup 3}. The corresponding values for Astana were considerably lower: 29 and 9 nBq/m{sup 3}, respectively, and in half of the filters the {sup 238}Pu activity was below the detection limit. Plutonium concentration correlated with the amount of dust retained on the filters only at the highest dust loads. Also no correlation between wind speed and the plutonium activity in the filters was observed. Thus, resuspension does not seem to be the mechanism responsible for the airborne plutonium. No clear seasonal variation of Pu air concentration was observed, though levels were somewhat elevated in February to April. There was no correlation between the plutonium and {sup 137}Cs concentrations. In most of the filters the cesium concentration was below the detection limit, but in those filters where it could be detected the cesium concentration was practically constant at 3.9+/-1.6 {mu}Bq/m{sup 3}. Dose estimation for the inhalation of the airborne plutonium gave a low value of 0.018 {mu}Sv/a for the inhabitants in Kurchatov, which is about a thousand times lower than the dose caused by the naturally occurring {sup 210}Po. Air parcel trajectory analysis indicated that the observed Pu activities in the air could not unambiguously be attributed to the most contaminated areas at the Semipalatinsk Test Site. (author)

Plutonium sorption by the green algae Scenedesmus obliquus (Tuerp) Kuetz

International Nuclear Information System (INIS)

Tkacik, M.F.; Giesy, J.P.; Corey, J.C.

1978-01-01

As part of the continuing study of the possible impact of released radioisotopes to the Savannah River Plant (SRP) environment, the interaction between a biological system and plutonium was investigated. Specifically, an algal culture, Scenedesmus obliquus, was exposed to the +4 and +6 oxidation states of 238 Pu and 239-240 Pu at three plutonium concentration levels. There was no significant different (p 3) 0.05) between 238 Pu and 239-240 Pu accumulation by the algae at equivalent concentrations or at different oxidation states

Protected Plutonium Production by Transmutation of Minor Actinides for Peace and Sustainable Prosperity [O1] - Fundamentals of P{sup 3} Mechanism and Methodology Development for Plutonium Categorization

Energy Technology Data Exchange (ETDEWEB)

Saito, Masaki [Research Laboratory for Nuclear Reactor, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro, Tokyo, 1528550 (Japan)

2009-06-15

'Protected Plutonium Production (P{sup 3})' has been proposed to enhance the proliferation resistance of plutonium by the transmutation of Minor Actinides (MAs). Doping the small amount of MAs such as {sup 237}Np or {sup 241}Am with large neutron capture cross-section into the uranium fuel to enhance the production of {sup 238}Pu or {sup 242}Pu, which have high spontaneous fission neutron source or also high decay heat to makes the process of the nuclear weapon manufacture and maintenance technologically difficult, can be effective for improving the isotopic barrier of proliferation resistance of the plutonium in thermal reactors. Super weapon grade plutonium could be produced in the blanket of a conventional FBR. However, by increasing the {sup 238}Pu or {sup 242}Pu ratio in the total plutonium by MAs doping into the fresh blanket, the protected plutonium with high proliferation-resistance can be bred. A new evaluation function, 'attractiveness', defined as a ratio of potential of fission yield to the technological difficulties of nuclear explosive device, has been proposed to evaluate the proliferation resistance of Pu based on the nuclear material property for Plutonium Categorization. In the conference, the fundamentals of P{sup 3} mechanism by transmutation of MA, and the comparison of the 'attractiveness' of the Pu produced in advanced reactors based on P{sup 3} mechanism and in the conventional reactors will be presented. Instead of the geological disposal or just their burning of MAs by the fission reaction, they should be treated as valuable fertile materials to enhance the proliferation resistance of plutonium produced in the thermal and fast breeder reactors for peace and sustainable prosperity in future. Acknowledgement: Some parts of this work have been supported by the Ministry of Education, Culture, Sports, Science and Technology in Japan. (authors)

Plutonium in Southern Hemisphere ocean Waters

DEFF Research Database (Denmark)

Hirose, K.; Aoyama, M.; Gastaud, J.

2013-01-01

Plutonium in seawater collected by the BEAGLE2003 cruise was determined using ICP- SF-MS and alpha spectrometry after Fe co-precipitation and radiochemical purification. Levels and distributions of dissolved plutonium activity concentrations in Southern Hemisphere ocean waters are summarized here......, including historical data. Pu-239 concentrations in surface water----of the central South Pacific (32.5 °S) in 2003 were around 1 mBq/m3. The 239Pu concentrations in the Indian Ocean surface waters (20°S) were similar to that in the South Pacific, whereas the 239Pu concentrations in the South Atlantic...... surface waters (30°S) were markedly lower than those in the South Pacific and Indian Oceans. The 239Pu vertical profile pattern was similar to that in the North Pacific subtropical gyre, although 239Pu concentrations in the deep South Pacific were significantly lower than those in the North Pacific. One...

First-principles elastic constants and phonons of delta-Pu

DEFF Research Database (Denmark)

Söderlind, P.; Landa, A.; Sadigh, B.

2004-01-01

Elastic constants and zone-boundary phonons of delta-plutonium have been calculated within the density-functional theory. The paramagnetic state of delta-Pu is modeled by disordered magnetism utilizing either the disordered local moment or the special quasirandom structure techniques. The anomalo......Elastic constants and zone-boundary phonons of delta-plutonium have been calculated within the density-functional theory. The paramagnetic state of delta-Pu is modeled by disordered magnetism utilizing either the disordered local moment or the special quasirandom structure techniques....... The anomalously soft C-' as well as a large anisotropy ratio (C-44/C-') of delta-Pu is reproduced by this theoretical model. Also the recently measured phonons for delta-Pu compare relatively well with their theoretical counterpart at the zone boundaries....

Investigation of plutonium (4) hydroxoformates

International Nuclear Information System (INIS)

Andryushin, V.G.; Belov, V.A.; Galaktionov, S.V.; Kozhevnikov, P.B.; Matyukha, V.A.; Shmidt, V.S.

1982-01-01

Deposition processes of plutonium (4) hydroxoformates in the system Pu(NO 3 ) 4 -HNO 3 -HCoOH-N6 4 OH-H 2 O have been studied in pH range 0.2-10.7 at total plutonium concentration in the system 100 g/l. It is shown that under the conditions plutonium (4) hydrolysis takes place with the formation of hydroxoformates. A local maximum of plutonium (4) hydroxoformate solubility in the range pH=3.8-4.8, which is evidently conditioned by the formation of soluble formate complex of plutonium in the region, is pointed out. The basic plutonium (4) formates of the composition PuOsub(x)(OH)sub(y)(COOH)sub(4-2x-y)xnHsub(2)O, where 1,3 >=x >= 0.7, 1.7 >= y >= 1.0 and n=1.5-7.0, are singled out, their thermal stability being studied. Density of the crystals and plutonium dioxide, formed during their thermal decomposition, is measured. It is established that for plutonium (4) hydroxoformates common regularities of the influence of salt composition (OH - -, CHOO - - and H 2 O-group numbers in the mulecule) on position of temperature decomposition effects and on the density of compounds, which have been previously found during the study of thorium and plutonium hydroxosalts are observed. It is shown that the density of plutonium dioxide decreases with the increase of hydration and hydrolysis degree of the initial plutonium hydroxoformate

Vertical distribution of 241Pu in the southern Baltic Sea sediments

International Nuclear Information System (INIS)

Strumińska-Parulska, Dagmara I.

2014-01-01

Highlights: • The unique study on 241 Pu in sediments from the southern Baltic Sea was presented. • 241 Pu was determined using alpha spectrometry by indirect method. • The biggest amount of 241 Pu existed in the surface layers of all analyzed sediments. • The highest 241 Pu amount comes from the Chernobyl accident. - Abstract: The vertical distribution of plutonium 241 Pu in marine sediments can assist in determining the deposition history and sedimentation process of analyzed regions. In addition, 241 Pu/ 239+240 Pu activity ratio could be used as a sensitive fingerprint for radioactive source identification. The present preliminary studies on vertical distribution of 241 Pu in sediments from four regions of the southern Baltic Sea are presented. The distribution of 241 Pu was not uniform and depended on sediment geomorphology and depth as well as location. The highest concentrations of plutonium were found in the surface layers of all analyzed sediments and originated from the Chernobyl accident

''Distribution and behaviour of plutonium in the waters of the channel and of the seine estuary''

International Nuclear Information System (INIS)

Garcia, K.

1997-01-01

Excess dissolved plutonium has been measured in the coastal waters of the Channel, from Granville to Boulogne, probably due to sorption-desorption processus. In the Seine estuary, in situ measurements and experimental studies showed that the plutonium desorbs himself from particles in low salinity waters. The desorbed plutonium originates in marine and/or fluvial dissolved Pu. Marine dissolved Pu(V), originating from La Hague plant discharges and from atlantic waters, is reduced and sorbed when the salinity decreases onto estuarial particles: Isotopic Activity Ration 238 Pu/ 239 , Pu(IR) of marine dissolved Pu(V) is about 0.7. Fluvial dissolved plutonium originates from atmospheric fallout and from an internal river source: fallout plutonium (IR=0.05) is unreactive with salinity while 45% of river plutonium (IR>1.7) flocculates at 0.5 g l -1 . Desorbed plutonium may have various origins, depending on the Seine liquid discharges and on the tidal coefficient. When the marine waters do not migrate upstream, the low salinity waters encounters particles marked essentially with marine plutonium and the IR of desorbed Pu is about 0.7. The activities of desorbed plutonium are too low to have any influence on the distribution of plutonium in the coastal waters on the Seine Bay. When the marine waters migrate upstream, the low salinity waters meet particles marked essentially with river plutonium (IR>1.7) and desorbed plutonium has a very high IR. These estuarine conditions are encountered five to seven month a year and implicate an increase of the IR of 0.1 of the plutonium present in the coastal waters of the Seine bay (1.2.-1.3.). (author)

Current status of life-span studies with inhaled plutonium in beagles at Pacific Northwest Laboratory

International Nuclear Information System (INIS)

Park, J.F.; Dagle, G.E.; Ragan, H.A.; Weller, R.E.; Stevens, D.L.

1986-01-01

Beagles that inhaled 239 PuO 2 , 238 PuO 2 , or 239 Pu(NO 3 ) 4 , in dose-level groups of 20 dogs, with initial lung burdens of ∼2, 15, 70, 300, 1100, or 5500 nCi, are now 11, 9, or 5 years postexposure. Lung tumors, bone tumors, and radiation pneumonitis, the plutonium-exposure-related causes of death observed to date, have occurred in the two, three, and four highest dose-level groups exposed to 238 PuO 2 , 239 Pu(NO 3 ) 4 , and 239 PuO 2 , respectively. No plutonium-exposure-related deaths have thus far been observed in dose-level groups exposed to less than ∼40 times the current maximum permissible lung dose for a plutonium worker. Plutonium-exposure-related effects not directly related to the cause of death include chronic lymphopenia, chronic neutropenia, sclerosis of the tracheobronchial lymph nodes, focal radiation pneumonitis, adenomatous hyperplasia in the liver, and dystrophic osteolytic lesions in the skeleton. No plutonium-exposure-related effects have thus far been observed in dose-level groups that received less than ∼15 times the current maximum permissible lung dose for a plutonium worker. 10 refs., 5 figs., 4 tabs

The effect of oxidation state on the absorption of ingested or inhaled plutonium

International Nuclear Information System (INIS)

Sullivan, M.F.; Gorham, L.S.; Ryan, J.L.

1980-01-01

Rats received plutonium nitrate (as 239 Pu(IV) or 239 Pu(VI) by gavage or nose-only exposure. Some of the animals were deprived of food before and/or after exposure. Results obtained indicate that there was increased retention of plutonium after exposure to 239 Pu(VI) in comparison with 239 Pu(IV). The absence of food either before and/or after inhalation exposure had no effect on the amount of 239 Pu retained by the liver and carcass. It was concluded that plutonium in its hexavalent state may under certain conditions be more readily absorbed from the GI tract, but that these conditions are unlikely to occur in human exposure. (H.K.)

On-line monitoring of low-level plutonium concentrations

International Nuclear Information System (INIS)

Hofstetter, K.J.; Huff, G.A.; Rebagay, T.V.

1979-10-01

An on-line monitor has been developed to assay plutonium in nitric acid solutions. The performance of the monitor has been assessed by a laboratory experimentation program using solutions with plutonium concentrations from 0.1 to 10 g/l. These conditions are typical of the plutonium solutions in an input stream to a plutonium-purification cycle in a reprocessing plant following uranium/plutonium partitioning. The monitoring system can be fully automated and shows great promise for detecting and quantifying plutonium in situ, thus minimizing the reliance on traditional sampling and laboratory-analysis techniques. The total concentration and isotopic abundance of plutonium are determined by measuring the absolute intensities of the low-energy gamma rays characteristics of 238 Pu, 239 Pu, and 240 Pu nuclides by direct gamma-ray spectroscopy and computer analysis of the spectral data. The addition of a monitoring system of this type to the input stream of a plutonium-purification cycle along with other suitable monitors on the waste streams and on the product stream provides the basis for a near real-time materials control and inventory system. Results of the laboratory-evaluation program employing plutonium in solutions with isotopic compositions typical of those involved in processing light water reactor fuels are presented. The detailed design of a monitoring cell and detection system is given. The precision and accuracy of the results relative to those measured by mass spectrometry and controlled potential coulometry are also summarized

Plutonium oxychalcogenides Pu2O2X (X=O, S, Se, Te) crystal chemistry, magnetic and electrical properties. 5f electrons delocalization

International Nuclear Information System (INIS)

Costantini, Jean-Marc.

1980-05-01

We have studied the influence of the chalcogen X on the bonding and on the magnetic and electrical properties of the oxychalcogenides Pu 2 O 2 X. These compounds are isostructural with hexagonal La 2 O 3 for X=O, S, Se and with tetragonal La 2 O 2 Te for X=Te. Comparison of Nd 2 O 2 X and Pu 2 O 2 X cell volumes showed that plutonium crystal radius decreases from Pu 2 O 3 through Pu 2 O 2 Te with increasing 5f electrons delocalization and 5f-np overlap. Superexchange interactions through O 2- and X 2- were thought to be responsible for the observed antiferromagnetic ordering. Neel temperatures increase from Pu 2 O 3 through Pu 2 O 2 Te showing that these interactions and subsequent 5f-np covalency are strengthened as chalcogen electronegativity decreases. Hexagonal Pu 2 O 3 is an insulator while the other compounds are semi-conductors with energy gaps around 0.6 eV which were interpreted as the separation between the 6d-7s conduction band and the np valence band. The localized 5f states were located just below the np band, partially overlapping it [fr

Plutonium story

International Nuclear Information System (INIS)

Seaborg, G.T.

1981-09-01

The first nuclear synthesis and identification (i.e., the discovery) of the synthetic transuranium element plutonium (isotope 238 Pu) and the demonstration of its fissionability with slow neutrons (isotope 239 Pu) took place at the University of California, Berkeley, through the use of the 60-inch and 37-inch cyclotrons, in late 1940 and early 1941. This led to the development of industrial scale methods in secret work centered at the University of Chicago's Metallurgical Laboratory and the application of these methods to industrial scale production, at manufacturing plants in Tennessee and Washington, during the World War II years 1942 to 1945. The chemical properties of plutonium, needed to devise the procedures for its industrial scale production, were studied by tracer and ultramicrochemical methods during this period on an extraordinarily urgent basis. This work, and subsequent investigations on a worldwide basis, have made the properties of plutonium very well known. Its well studied electronic structure and chemical properties give it a very interesting position in the actinide series of inner transition elements

Vertical distributions of particulate plutonium in the western North Pacific Ocean

International Nuclear Information System (INIS)

Okubo, Ayako; Zheng, Jian; Aono, Tatsuo; Kaeriyama, Hideki; Nakanishi, Takahiro; Yamada, Masatoshi; Kusakabe, Masashi

2007-01-01

We examined the vertical distributions of 239+240 Pu activity and 240 Pu / 239 Pu atom ratio in particles collected by large volume water in-situ pump in the western North Pacific Ocean (off Rokkasho, Japan). This is the first information of vertical distribution of plutonium activity and Plutonium atom ratio in small particle (1-70 μm) and large particle (>70 μm). (author)

Recovery of 238PuO2 by Molten Salt Oxidation Processing of 238PuO2 Contaminated Combustibles (Part II)

Science.gov (United States)

Remerowski, Mary Lynn; Dozhier, C.; Krenek, K.; VanPelt, C. E.; Reimus, M. A.; Spengler, D.; Matonic, J.; Garcia, L.; Rios, E.; Sandoval, F.; Herman, D.; Hart, R.; Ewing, B.; Lovato, M.; Romero, J. P.

2005-02-01

Pu-238 heat sources are used to fuel radioisotope thermoelectric generators (RTG) used in space missions. The demand for this fuel is increasing, yet there are currently no domestic sources of this material. Much of the fuel is material reprocessed from other sources. One rich source of Pu-238 residual material is that from contaminated combustible materials, such as cheesecloth, ion exchange resins and plastics. From both waste minimization and production efficiency standpoints, the best solution is to recover this material. One way to accomplish separation of the organic component from these residues is a flameless oxidation process using molten salt as the matrix for the breakdown of the organic to carbon dioxide and water. The plutonium is retained in the salt, and can be recovered by dissolution of the carbonate salt in an aqueous solution, leaving the insoluble oxide behind. Further aqueous scrap recovery processing is used to purify the plutonium oxide. Recovery of the plutonium from contaminated combustibles achieves two important goals. First, it increases the inventory of Pu-238 available for heat source fabrication. Second, it is a significant waste minimization process. Because of its thermal activity (0.567 W per gram), combustibles must be packaged for disposition with much lower amounts of Pu-238 per drum than other waste types. Specifically, cheesecloth residues in the form of pyrolyzed ash (for stabilization) are being stored for eventual recovery of the plutonium.

Recovery of 238PuO2 by Molten Salt Oxidation Processing of 238PuO2 Contaminated Combustibles (Part II)

International Nuclear Information System (INIS)

Remerowski, Mary Lynn; Dozhier, C.; Krenek, K.; VanPelt, C. E.; Reimus, M. A.; Spengler, D.; Matonic, J.; Garcia, L.; Rios, E.; Sandoval, F.; Herman, D.; Hart, R.; Ewing, B.; Lovato, M.; Romero, J. P.

2005-01-01

Pu-238 heat sources are used to fuel radioisotope thermoelectric generators (RTG) used in space missions. The demand for this fuel is increasing, yet there are currently no domestic sources of this material. Much of the fuel is material reprocessed from other sources. One rich source of Pu-238 residual material is that from contaminated combustible materials, such as cheesecloth, ion exchange resins and plastics. From both waste minimization and production efficiency standpoints, the best solution is to recover this material. One way to accomplish separation of the organic component from these residues is a flameless oxidation process using molten salt as the matrix for the breakdown of the organic to carbon dioxide and water. The plutonium is retained in the salt, and can be recovered by dissolution of the carbonate salt in an aqueous solution, leaving the insoluble oxide behind. Further aqueous scrap recovery processing is used to purify the plutonium oxide. Recovery of the plutonium from contaminated combustibles achieves two important goals. First, it increases the inventory of Pu-238 available for heat source fabrication. Second, it is a significant waste minimization process. Because of its thermal activity (0.567 W per gram), combustibles must be packaged for disposition with much lower amounts of Pu-238 per drum than other waste types. Specifically, cheesecloth residues in the form of pyrolyzed ash (for stabilization) are being stored for eventual recovery of the plutonium

Ultra trace plutonium isotopic analyse by thermo ionization mass spectrometry

International Nuclear Information System (INIS)

Liu Xuemei; Long Kaiming; Yang Tianli

2008-06-01

An anion exchange combined with TTA extraction decontamination method was established. The nanogram quantity Plutonium was separated from milligram uranium and the decontamination coefficient achieved 10 7 , the recovery coefficient >95%. The active carbon powder was chosen as the ionization intensifier to increase the plutonium ion flow. Used 6.7 pg Plutonium standard as sample to measured by TIMS and the RSD of the 240 Pu/ 239 Pu ≤3.6%. (authors)

Liquid chromatographic studies on the behaviour of Pu(III), Pu(IV) and Pu(VI) on a RP stationary phase in presence of α-hydroxyisobutyric acid as a chelating agent

Energy Technology Data Exchange (ETDEWEB)

Jaison, P.G.; Kumar, Pranaw; Telmore, Vijay M. [Bhabha Atomic Research Centre, Mumbai (India). Fuel Chemistry Division

2017-06-01

Since plutonium possesses multiple oxidation states which can coexist in solution, a method for the identification of these oxidation states is important to understand its chemical processes. Liquid chromatographic studies were carried out to compare the chromatographic behaviour of different oxidation states of Pu in presence of the eluent, α-hydroxyisobutyric acid (HIBA). The three oxidation states of Pu viz. Pu(III), Pu(IV) and Pu(VI) were separated under optimised conditions. It was seen that the presence of the complexing agent influences the equilibrium of Pu(III)/(IV) as well as Pu(IV)/(VI) systems. Pu(III) to Pu(IV) conversion was found to be enhanced by high pH and concentration of HIBA whereas a relatively low pH and high concentration of HIBA promotes the conversion of Pu(VI) to Pu(IV).

Probing phonons in plutonium

International Nuclear Information System (INIS)

Wong, Joe; Krisch, M.; Farber, D.; Occelli, F.; Schwartz, A.; Chiang, T.C.; Wall, M.; Boro, C.; Xu, Ruqing

2010-01-01

Plutonium (Pu) is well known to have complex and unique physico-chemical properties. Notably, the pure metal exhibits six solid-state phase transformations with large volume expansions and contractions along the way to the liquid state: α → β → γ → (delta) → (delta)(prime) → (var e psilon) → liquid. Unalloyed Pu melts at a relatively low temperature ∼640 C to yield a higher density liquid than that of the solid from which it melts, (Figure 1). Detailed understanding of the properties of plutonium and plutonium-based alloys is critical for the safe handling, utilization, and long-term storage of these important, but highly toxic materials. However, both technical and and safety issues have made experimental observations extremely difficult. Phonon dispersion curves (PDCs) are key experimenta l data to the understanding of the basic properties of Pu materials such as: force constants, sound velocities, elastic constants, thermodynamics, phase stability, electron-phonon coupling, structural relaxation, etc. However, phonon dispersion curves (PDCs) in plutonium (Pu) and its alloys have defied measurement for the past few decades since the discovery of this element in 1941. This is due to a combination of the high thermal-neutron absorption cross section of plutonium and the inability to grow the large single crystals (with dimensions of a few millimeters) necessary for inelastic neutron scattering. Theoretical simulations of the Pu PDC continue to be hampered by the lack of suitable inter -atomic potentials. Thus, until recently the PDCs for Pu and its alloys have remained unknown experimentally and theoretically. The experimental limitations have recently been overcome by using a tightly focused undulator x-ray micro-beam scattered from single -grain domains in polycrystalline specimens. This experimental approach has been applied successfully to map the complete PDCs of an fcc d-Pu-Ga alloy using the high resolution inelastic x-ray scattering (HRIXS

Non-destructive assay of 242Pu by resonance neutron capture

International Nuclear Information System (INIS)

Kane, W.R.; Lu, Ming-Shih; Aronson, A.; Forman, L.; Vanier, P.E.

1995-01-01

For the accurate assay of plutonium by neutron correlation measurements, especially for material derived from high-burnup reactor fuel, the content of 242 Pu in a sample must be determined. Since 242 Pu has a long half-life (387,000 yr) and decays to 238 U by alpha particle emission with the accompanying emission of only weak, low-energy gamma rays, gamma-ray spectrometry methods which are ordinarily employed to determine the isotopic composition of a plutonium sample are not feasible for 242 Pu. The existence of a resonance in the neutron capture cross section of 242 Pu at an energy of 2.67 electron volts (eV) with a large (72, 000 barn) cross section affords the possibility for the quantitative assay of this isotope by epithermal neutron capture. Essential for this purpose is an appropriately designed geometry of neutron moderators and absorbers which will provide maximum flux in the eV region while suppressing thermal neutron capture by the fissile plutonium isotopes. Signatures for neutron capture in 242 Pu include the decay of 243 Pu (4.9 hr), prompt capture gamma rays (total energy 5.034 MeV), and the decay of an isomeric state (330 nanosecond). Experiments to determine the feasibility of this approach are currently in progress

Molecular dynamics study of a nuclear waste glass matrix with plutonium

International Nuclear Information System (INIS)

Meis, C.; Delaye, J.M.; Ghaleb, D.

1999-01-01

Molecular dynamics simulation techniques were applied to model the incorporation of plutonium in the French nuclear waste glass matrix. Born-Mayer-Huggins analytical potentials were established to characterize short-range interactions between Pu-O and Pu-Pu pairs; the potentials were fitted to the structural properties of plutonium dioxide in the light of a recent experimental study showing that plutonium is found as Pu(IV) in the glass. The transferability of the established potentials to the glass structure is discussed, and the potential parameters are further refined by molecular dynamics simulations in an aluminoborosilicate glass to obtain mean Pu-O interatomic distances and first-neighbor coordination numbers matching the experimental values as closely as possible. Previously published Born-Mayer-Huggins potentials supplemented by Stillinger-Weber three-body terms were used for oxygen-cation and cation-cation interactions. The difficulties encountered in establishing a Pu-O potential that provides satisfactory results in both oxides and glasses are also discussed

Gastrointestinal absorption of plutonium in mice, rats, and dogs: application to establishing values of f1 for soluble plutonium

International Nuclear Information System (INIS)

Bhattacharyya, M.H.; Larsen, R.P.; Oldham, R.D.; Moretti, E.S.; Spaletto, M.I.

1985-04-01

The gastrointestinal (GI) absorption of plutonium was measured in mice, rats, and dogs under conditions relevant to setting drinking water standards. The fractional GI absorption of Pu(VI) in adult mice was 2 x 10 -4 (0.02%) in fed mice and 2 x 10 -3 (0.2%) in fasted mice. The GI absorption of plutonium was independent of plutonium oxidation state, administration medium, and plutonium concentration; absorption was dependent upon animal species, state of animal fasting, state of Pu(IV) hydrolysis, and age of the animal. Fractional GI absorption values ranged from 3 x 10 -5 (0.003%) for hydrolyzed Pu(IV) administered to fed adult mice to 7 x 10 -3 (0.7%) for Pu(VI) administered to fed neonatal rats. From analysis of our data, we suggested values of f 1 (the fraction transferred from gut to blood in humans) for use in establishment of oral limits of exposure to plutonium. For an acute exposure in the occupational setting, we proposed one value of f 1 for fed (2 x 10 -4 ) and one for fasted (2 x 10 -3 ) individuals. For the environmental setting, we developed two approaches to obtaining values of f 1 ; suggested values were 6 x 10 -4 and 4 x 10 -3 , respectively. Both approaches took into account effects of animal age and fasting. We discussed uncertainties in proposed values of f 1 and made recommendations for further research. 41 refs., 8 figs., 24 tabs

The gastrointestinal absorption of organically bound forms of plutonium in fed and fasted hamsters

International Nuclear Information System (INIS)

Harrison, J.D.; Cooper, J.R.; Bomford, J.A.; David, A.J.

1986-01-01

Values of about 0.005-0.01% were obtained for the absorption in fed hamsters of plutonium ingested as Pu 4+ citrate, isocitrate, phytate and malate complexes and Pu 3+ ascorbate compared with about 0.003-0.004% for Pu 4+ nitrate. Replacing drinking water with tea did not affect the result for Pu 4+ nitrate. Fasting hamsters for 8 h before the administration of plutonium citrate increased absorption to 0.1-0.2%. An extra period of fasting for 4 h after administration did not lead to a further increase in absorption. Similar values were also obtained when plutonium citrate was administered after a 24 h fast, followed either by immediate access to food or a further 4 h fast. In hamsters fasted for 24 h before administration of either Pu 3+ ascorbate or Pu 4+ nitrate, about 6-7 per cent of the ingested plutonium was retained in the gastrointestinal tract after one week. At three weeks after ingestion of Pu 3+ ascorbate, gastrointestinal retention had fallen 100-fold without an increase in absorption. (author)

Environmental behaviour of plutonium accidentally released at Thule, Greenland

International Nuclear Information System (INIS)

Aarkrog, A.

1977-01-01

The environmental contamination resulting from the B-52 accident in 1968 at Thule was studied by scientific expeditions in 1968, 1970 and 1974. The contamination was mainly confined to the marine environment, where plutonium was preferentially located in the sediments and the benthic fauna. Plutonium concentrations down through the sediment layers decayed exponentially with a half-depth of 1 to 2 cm. The horizontal distribution of the plutonium may be described by an exponential expression: mCi sup(239,240)Pu km -2 = 460sub(e)sup(-0.28R) or by a power function: mCisup(239,240)Pu km -2 = 370 Rsup(-1.2), where R is the distance in km from the point of impact. The inventory of sup(239,240)Pu in the marine environment from the accident was estimated at 25 to 30 Ci. The amount of 238 Pu was approximately 0.5 Ci. The bottom animals, such as worms and molluscs, showed a horizontal distribution of radioactivity similar to that of the sediments. From 1968 to 1970 the sup(239,240)Pu concentrations in the biota decreased by an order of magnitude, since 1970 the decrease has been less evident. In 1970 and 1974 there were no indications of increased plutonium concentrations in surface seawater or in sea plants or zooplankton. Higher animals such as fish, seabirds and marine mammals have shown no tendency to increasing plutonium levels since the accident. (author)

Review of major plutonium pyrochemical technology

International Nuclear Information System (INIS)

Moser, W.S.; Navratil, J.D.

1983-01-01

The past twenty years have seen significant growth in the development and application of pyrochemical technology for processing of plutonium. For particular feedstocks and specific applications, non-aqueous high-temperature processes offer key advantages over conventional hydrometallurgical systems. Major processes in use today include: (1) direct oxide reduction for conversion of PuO 2 to metal, (2) molten salt extraction for americium removal from plutonium, (3) molten salt electrorefining for Pu purification, and (4) hydriding to remove plutonium from host substrates. This paper reviews current major pyrochemical processes from the classical calcination-hydrofluorination-bomb reduction sequence through new techniques under development. Each process is presented and brief descriptions of production equipment are given. 47 references, 5 figures

Cation exchange process for recovery of plutonium from laboratory solutions containing chloride

International Nuclear Information System (INIS)

Gray, L.W.

1978-10-01

A cation exchange technique was developed for the separation of plutonium from laboratory solutions containing either Pu(III) or Pu(III)--Pu(IV) mixtures in acidic solutions containing chloride ions. The procedure consists of adjusting the acid concentration to less than one molar and adjusting the valence of the plutonium ion to the (III) state, if necessary. The adjusted solution is fed to a cation exchange column and washed with distilled water to remove residual chlorides from the column. Plutonium is then eluted from the column with 5M nitric acid containing 0.34M sulfamic acid. This procedure was used to separate plutonium from 1.2M chloride solution on a production-scale column. Typical plutonium recovery was 99.97%, while greater than 96% of the original chloride was rejected

Early retention of 237Pu + 239Pu in mature beagles

International Nuclear Information System (INIS)

Lloyd, R.D.; McFarland, S.S.; Atherton, D.R.; Bruenger, F.W.; Taylor, G.N.; Mays, C.W.

1978-01-01

Five mature beagles, ranging in age from 57 to 84 months, were injected intravenously with about 0.05-0.1 μCi/kg of 239 Pu(IV) citrate to which tracer amounts of the photon-emitter 237 Pu had been added. Plutonium retention in liver and in non-liver tissue (mainly skeleton) was measured periodically in the living dogs for nearly 4 months after injection by a combination of total-body and partial-body counting. All excreta were collected during the first 21 days and analysed for their Pu content. One dog was sacrificed at 14 days and another at 118 days for distribution studies. About 17% (14-20%) of the injected Pu was excreted in the urine and feces in the first 3 weeks, about the same as that excreted in a corresponding time by beagles injected as young adults (14%), but substantially more than beagles injected as juveniles (11%). In contrasts to juvenile beagles injected at 3 months of age, in which early retention was about 12% in liver and 68% in the skeleton, mature beagles retained about 30% in liver and 50% in the skeleton. Retention in young adult beagles injected at 17 months of age was similar to that of mature dogs. Relative distribution of skeletal plutonium among various bones was similar in the mature animals to that seen previously in young adults, but quite different from that of juveniles. A notable exception was the humerus for which there was no significant difference (P>0.2) in the % of retained skeletal Pu represented by the humerus among the juvenile, young adult and mature dogs. (author)

Quantitative dissolution of (U, Pu)O2 MOX (0.4% to 44% PuO2) using microwave heating technique

International Nuclear Information System (INIS)

Malav, R.K.; Fulzele, Ajit K.; Prakash, Amrit; Afzal, Md.; Panakkal, J.P.

2011-01-01

AFFF has fabricated the (U, Pu)O 2 mixed oxide fuels for PHWRs, BWRs, PFBRs and FBTRs. The quantitative dissolution of the fuel samples are required within time for accurate determination of uranium-plutonium in chemical quality control laboratory. This paper describes the use of microwave heating technique in quantitative dissolution of (U, Pu)O 2 MOX (from 0.4% to 44% PuO 2 ). (author)

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.

Science.gov (United States)

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.

Plutonium in a grassland ecosystem

International Nuclear Information System (INIS)

Little, C.A.

1976-08-01

A study was made of plutonium contamination of grassland at the Rocky Flats plant northwest of Denver, Colorado. Of interest were: the definition of major plutonium-containing ecosystem compartments; the relative amounts in those compartments; how those values related to studies done in other geographical areas; whether or not the predominant isotopes, 238 Pu and 239 Pu, behaved differently; and what mechanisms might have allowed for the observed patterns of contamination. Samples of soil, litter, vegetation, arthropods, and small mammals were collected for Pu analysis and mass determination from each of two macroplots. Small aliquots (5 g or less) were analyzed by a rapid liquid scintillation technique and by alpha spectrometry. Of the compartments sampled, greater than 99 percent of the total plutonium was contained in the soil and the concentrations were significantly inversely correlated with distance from the contamination source, depth of the sample, and particle size of the sieved soil samples. The soil data suggested that the distribution of contamination largely resulted from physical transport processes

The absorption spectra of Pu(VI), -(V) and -(IV) produced electrochemically in carbonate-bicarbonate media

International Nuclear Information System (INIS)

Wester, D.W.; Sullivan, J.C.

1983-01-01

Absorption spectra in carbonate and bicarbonate media have been measured for various oxidation states of plutonium. The oxidation state of plutonium was adjusted electrochemically (Pu(VI)-V), Esub(f)=+0.11 V vs. SCE) to avoid contamination by redox reagents. In carbonate medium the spectra of Pu(VI) and Pu(V) showed marked differences from the spectra of the same oxidation state in acidic solutions. In bicarbonate the spectra of Pu(VI) and Pu(IV) also differed from the corresponding spectra in acidic media. Reduction to Pu(III) resulted in a precipitate in both carbonate and bicarbonate media. (author)

Cancer hazard from inhaled plutonium

International Nuclear Information System (INIS)

Gofman, J.W.

1975-01-01

The best estimate of the lung cancer potential in humans for inhaled insoluble compounds of plutonium (such as PuO 2 particles) has been grossly underestimated by such authoritative bodies as the International Commission on Radiological Protection and the British Medical Research Council. Calculations are presented of lung cancer induction by 239 Pu as insoluble particles and for deposited reactor-grade Pu. The reason for the gross underestimate of the carcinogenic effects of Pu by ICRP or the British Medical Research Council (BMRC) is their use of a totally unrealistic idealized model for the clearance of deposited Pu from the lungs and bronchi plus their non-recognition of the bronchi as the true site for most human lung cancers. The erroneous model used by such organizations also fails totally to take into account the effect of cigarette-smoking upon the physiological function of human lungs. Plutonium nuclides, such as 239 Pu, or other alpha particle-emitting nuclides, in an insoluble form represent an inhalation cancer hazard in a class some 100,000 times more potent than the potent chemical carcinogens, weight for weight. The already-existing lung cancer data for beagle dogs inhaling insoluble PuO 2 particles is clearly in order of magnitude agreement with calculations for humans

Complementary technologies for verification of excess plutonium

International Nuclear Information System (INIS)

Langner, D.G.; Nicholas, N.J.; Ensslin, N.; Fearey, B.L.; Mitchell, D.J.; Marlow, K.W.; Luke, S.J.; Gosnell, T.B.

1998-01-01

Three complementary measurement technologies have been identified as candidates for use in the verification of excess plutonium of weapons origin. These technologies: high-resolution gamma-ray spectroscopy, neutron multiplicity counting, and low-resolution gamma-ray spectroscopy, are mature, robust technologies. The high-resolution gamma-ray system, Pu-600, uses the 630--670 keV region of the emitted gamma-ray spectrum to determine the ratio of 240 Pu to 239 Pu. It is useful in verifying the presence of plutonium and the presence of weapons-grade plutonium. Neutron multiplicity counting is well suited for verifying that the plutonium is of a safeguardable quantity and is weapons-quality material, as opposed to residue or waste. In addition, multiplicity counting can independently verify the presence of plutonium by virtue of a measured neutron self-multiplication and can detect the presence of non-plutonium neutron sources. The low-resolution gamma-ray spectroscopic technique is a template method that can provide continuity of knowledge that an item that enters the a verification regime remains under the regime. In the initial verification of an item, multiple regions of the measured low-resolution spectrum form a unique, gamma-radiation-based template for the item that can be used for comparison in subsequent verifications. In this paper the authors discuss these technologies as they relate to the different attributes that could be used in a verification regime

Development of a Self-Consistent Model of Plutonium Sorption: Quantification of Sorption Enthalpy and Ligand-Promoted Dissolution

Energy Technology Data Exchange (ETDEWEB)

Powell, Brian [Clemson Univ., SC (United States); Kaplan, Daniel I [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Arai, Yuji [Univ. of Illinois, Urbana-Champaign, IL (United States); Becker, Udo [Univ. of Michigan, Ann Arbor, MI (United States); Ewing, Rod [Stanford Univ., CA (United States)

2016-12-29

This university lead SBR project is a collaboration lead by Dr. Brian Powell (Clemson University) with co-principal investigators Dan Kaplan (Savannah River National Laboratory), Yuji Arai (presently at the University of Illinois), Udo Becker (U of Michigan) and Rod Ewing (presently at Stanford University). Hypothesis: The underlying hypothesis of this work is that strong interactions of plutonium with mineral surfaces are due to formation of inner sphere complexes with a limited number of high-energy surface sites, which results in sorption hysteresis where Pu(IV) is the predominant sorbed oxidation state. The energetic favorability of the Pu(IV) surface complex is strongly influenced by positive sorption entropies, which are mechanistically driven by displacement of solvating water molecules from the actinide and mineral surface during sorption. Objectives: The overarching objective of this work is to examine Pu(IV) and Pu(V) sorption to pure metal (oxyhydr)oxide minerals and sediments using variable temperature batch sorption, X-ray absorption spectroscopy, electron microscopy, and quantum-mechanical and empirical-potential calculations. The data will be compiled into a self-consistent surface complexation model. The novelty of this effort lies largely in the manner the information from these measurements and calculations will be combined into a model that will be used to evaluate the thermodynamics of plutonium sorption reactions as well as predict sorption of plutonium to sediments from DOE sites using a component additivity approach.

Some Thermodynamic Features of Uranium-Plutonium Nitride Fuel in the Course of Burnup

Science.gov (United States)

Rusinkevich, A. A.; Ivanov, A. S.; Belov, G. V.; Skupov, M. V.

2017-12-01

Calculation studies on the effect of carbon and oxygen impurities on the chemical and phase compositions of nitride uranium-plutonium fuel in the course of burnup are performed using the IVTANTHERMO code. It is shown that the number of moles of UN decreases with increasing burnup level, whereas UN1.466, UN1.54, and UN1.73 exhibit a considerable increase. The presence of oxygen and carbon impurities causes an increase in the content of the UN1.466, UN1.54 and UN1.73 phases in the initial fuel by several orders of magnitude, in particular, at a relatively low temperature. At the same time, the presence of impurities abruptly reduces the content of free uranium in unburned fuel. Plutonium in the considered system is contained in form of Pu, PuC, PuC2, Pu2C3, and PuN. Plutonium carbides, as well as uranium carbides, are formed in small amounts. Most of the plutonium remains in the form of nitride PuN, whereas unbound Pu is present only in the areas with a low burnup level and high temperatures.

Preliminary safety evaluation for the plutonium stabilization and packaging system

International Nuclear Information System (INIS)

Shapley, J.E.

1997-01-01

This Preliminary Safety Evaluation (PSE) describes and analyzes the installation and operation of the Plutonium Stabilization and Packaging System (SPS) at the Plutonium Finishing Plant (PFP). The SPS is a combination of components required to expedite the safe and timely storage of Plutonium (Pu) oxide. The SPS program will receive site Pu packages, process the Pu for storage, package the Pu into metallic containers, and safely store the containers in a specially modified storage vault. The location of the SPS will be in the 2736- ZB building and the storage vaults will be in the 2736-Z building of the PFP, as shown in Figure 1-1. The SPS will produce storage canisters that are larger than those currently used for Pu storage at the PFP. Therefore, the existing storage areas within the PFP secure vaults will require modification. Other modifications will be performed on the 2736-ZB building complex to facilitate the installation and operation of the SPS

Partitioning of plutonium and uranium in aqueous medium using hydroxyurea as reducing agent

International Nuclear Information System (INIS)

Sivakumar, P.; Subba Rao, R.V.; Meenakshi, S.

2012-01-01

A new process for the partitioning of plutonium and uranium during the reprocessing of spent fuel discharged from fast reactor was optimised using hydroxyurea (HU) as a reductant. Stoichiometric ratio of HU required for the reduction of Pu(IV) was studied. The effect of concentration of uranium, plutonium and acidity on the distribution ratio (Kd) of Pu in the presence of HU was studied. The effect of HU in further purification of Pu such as solvent extraction and precipitation of plutonium as oxalate was also studied. The results of the study indicate that Pu and U can be separated from each other using HU as reductant. (author)

Study of plutonium sorption in aluminia column in the system HNO3-HF

International Nuclear Information System (INIS)

Araujo, J.A. de.

1977-01-01

The column chromatographic method using alumina has been applied successfully to study the sorption-desorption behavior of plutonium traces in HNO 3 -HF and HNO 3 -HF-UO 2 (NO 3 ) 2 systems, aiming to elaborate a process for recovering plutonium traces from reprocessing wastes, mainly in existing solutions where uranium is presented in macro quantities. Basically, the method consists in the sorption of plutonium by percolating a solution containing HNO 3 (0,1 to 0,8M) or uranyl nitrate (1-50 gU/l) and HF(0,1 to 0,3M) through an Al 2 O 3 collumn. The plutonium is fixed on Al 2 O 3 whereas the uranyl ions is collected in the efluent. The adsorption of Pu-III, Pu-IV and Pu-VI in the presence of HF was determined and Pu-IV can be almost completely sorbed. The Pu-IV is eluted by reduction to Pu-III in the column using 3 M HNO 3 -0,005M FeSO 4 at 50 0 C as elutrient. This method is very simple and can be applied for separation and purification of plutonium (traces) from uranyl nitrate or others coming solutions from wet chemistry of irradiated fuels [pt

Review of criticality safety benchmark data of plutonium solution in ICSBEP handbook

International Nuclear Information System (INIS)

Yamamoto, Toshihiro; Miyoshi, Yoshinori; Okubo, Kiyoshi

2003-01-01

The criticality data of plutonium solutions published in the ICSBEP Handbook were reviewed. Criticality data for lower plutonium concentration and higher 240 Pu content, which correspond to a reprocessing process condition, are very scarce and hence the criticality data in this area are desired. While the calculated k eff 's with ENDF/B-V show the dependence of the plutonium concentration, the dependence has been corrected in JENDL-3.3 because of energy distribution of the capture cross section of 239 Pu. Based on the generalized perturbation theory, the sensitivity coefficient of k eff with respect to fission and capture cross section in plutonium solutions were obtained. In a plutonium solution with a lower concentration, cross sections in the thermal energy less than 0.1 eV have significant effects on the criticality. On the other hand, the criticality of higher concentration plutonium solutions is mostly dominated by cross sections in the energy range larger than 0.1 eV. Regarding the effect of 240 Pu on criticality, the capture cross section 240 Pu around the resonance peak near 1 eV is dominant regardless of the concentration. (author)

Life-span studies of inhaled plutonium in beagle dogs

International Nuclear Information System (INIS)

Bair, W.J.

1990-04-01

In 1970 a life-span study with over 300 beagle dogs was begun to gain an understanding of long-term health effects resulting from respiratory tract intakes of plutonium and to derive risk estimates that might be applied to plutonium and other transuranic elements. Groups of beagle dogs were given single exposures to 239 PuO 2 , 238 PuO 2 , or 239 Pu(NO 3 ) 4 to obtain graded levels of initial lung burdens ranging from 1 to 1800 Bq lung. The objective of this paper is to give you a progress report on the current life-span studies of inhaled plutonium in beagle dogs at the Pacific Northwest Laboratory. I will describe the biokinetics of inhaled plutonium in dogs and the resulting health effects. I will also mention some studies directed towards understanding the mechanism leading to these effects. Finally, I will discuss the current risk estimates derived from these studies and how they might relate to plutonium exposures in humans. 5 refs., 13 figs., 4 tabs

Water Solubility of Plutonium and Uranium Compounds and Residues at TA-55

International Nuclear Information System (INIS)

Reilly, Sean Douglas; Smith, Paul Herrick; Jarvinen, Gordon D.; Prochnow, David Adrian; Schulte, Louis D.; DeBurgomaster, Paul Christopher; Fife, Keith William; Rubin, Jim; Worl, Laura Ann

2016-01-01

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 the 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 3 O 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

Water Solubility of Plutonium and Uranium Compounds and Residues at TA-55

Energy Technology Data Exchange (ETDEWEB)

Reilly, Sean Douglas [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Smith, Paul Herrick [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Jarvinen, Gordon D. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Prochnow, David Adrian [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Schulte, Louis D. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; DeBurgomaster, Paul Christopher [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Fife, Keith William [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Rubin, Jim [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Worl, Laura Ann [Los Alamos National Lab. (LANL), Los Alamos, NM (United States

2016-06-13

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 the 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), U₃O₈ (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 PuCl₃, 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

Plutonium isotopes/137Cs activity ratios for soil in Montenegro

International Nuclear Information System (INIS)

Antovic, N. M.; Vukotic, P.; Svrkota, N.; Andrukhovich, S.K.

2011-01-01

Plutonium isotopes/ 137 Cs activity ratios were determined for six soil samples from Montenegro, using the results of alpha-spectrometric measurements of 239+240 Pu and 238 Pu, as well as gamma-spectrometric cesium measurements. An average 239+240 Pu/ 137 Cs activity ratio is found to be 0.02, as the 238 Pu/ 137 Cs and 238 Pu/ 239+240 Pu one - 0.0006 and 0.03, respectively. It follows from the results that the source of plutonium in Montenegro soil is nuclear weapon testing during the fifties and sixties of the twentieth century. On the other hand, there is a contribution of the accident at the Chernobyl nuclear power plant to the soil contamination with 137 Cs isotope. [sr

Simultaneous measurement of 239Pu, 240Pu, 241Pu, and 242Pu by high resolution inductively coupled plasma mass spectrometer (HR ICP-MS) in marine sediments

International Nuclear Information System (INIS)

Bruneau, F.

1999-01-01

Transuranics elements are of particular interest in radioecological studies because of their radiotoxicity and their potential use to decipher source fingerprints and transport processes. The simultaneous measurement of 239 Pu, 240 Pu, 241 Pu, and 242 Pu in environmental samples requires a specific chemical procedure. This work deals with an analytical procedure which yields a very high grade of purification of Pu suitable for ultra low level detection by HR ICP-MS, from marine sediments. After the elimination of major elements (Fe, Al, Mg...) by a first chromatographic separation, a new device of purification by solvent extraction and concentration by a second chromatographic separation is used to obtain a concentrated and high purified solution of plutonium. The chemical procedure have been validated on IAEA certified sediment samples and on sediment samples collected in the roads of Cherbourg which had been previously analysed by other techniques (a spectrometry and thermo-ionisation mass spectrometer). (author)

Accumulation of plutonium from fallout in southern Finns and Lapps

International Nuclear Information System (INIS)

Mussalo-Rauhamaa, H.

1981-01-01

The body burden of 239 , 240 Pu and 238 Pu from fallout in southern Finns and Lapps was determined by ion exchange and alpha-spectrometry through analyses of autopsy tissue samples. Comparing the body burden against the inhalation and ingestion intake of plutonium of these population groups the fractional absorption factor for plutonium from the human gastrointestinal tract and lungs was estinated. In addition, the determined tissue values were compared with those computed with the aid of the ICRP lung model and plutonium content of surface air in the Helsinki area. The 239 , 240 Pu concentrations per wet weight of tissue descended in the order liver>lymph nodes>bone>lung>testes>muscle. A dependence of plutonium content of tissues on the amount of air inhaled by the person during the fallout period and, thus, on the age of the person, was shown. The skeletal distribution of plutonium in man was roughly similar to that reported for animals. The ratio of 239 , 240 Pu content in vertebrae to that in ribs was 1.4, on the average, and the rib/femur ratio 1.0. The average body burden of 239 , 240 Pu in adult southern Finn and Lapp males was estimated to be 1.2 pCi (44.4 mBq), of which about 51 per cent was located in liver and 40 per cent in skeleton. The estimates for the ingestion and inhalation intake of 239 , 240 Pu during the period 1945-78 were 36 and 18 pCi (1.3, 0.67 Bq) and 540 and 13 pCi (19.9, 0.48 Bq) for southern Finn and Lapp males, respectively. The estimated fractional absorption factor of plutonium in humn GI-tract was of the order (6-9)x10 -4 and in lungs (7.5-8.5)x10 -2 . (author)

X-ray absorption near-edge spectroscopy of plutonium solid species

International Nuclear Information System (INIS)

Kropf, A. J.

1998-01-01

We present XANES at the L III edge for four plutonium solid phases: Pu(III)F 3 , Pu(IV)O 2 , NaPu(V)O 2 CO 3 , and Ba 3 Pu(VI)O 6 . These correspond to the four important oxidation states in the process chemistry and environmental chemistry of plutonium. By a fitting method that uses an arc tangent function and gaussian curves, it was possible to reproducibly determine the edge energy and distinguish among the four oxidation states. These data demonstrate a 1.85 ± 0.20 eV shift per oxidation state

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

Science.gov (United States)

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

1996-01-01

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

Hydrometallurgical treatment of plutonium. Bearing salt baths waste

International Nuclear Information System (INIS)

Bros, P.; Gozlan, J.P.; Lecomte, M.; Bourges, J.

1993-01-01

The salt flux issuing from the electrorefining of plutonium metal alloy in salt baths (KCI + NaCI) poses a difficult problem of the back-end alpha waste management. An alternative to the salt process promoted by Los Alamos Laboratory is to develop a hydrometallurgical treatment. A new process based on the electrochemistry technique in aqueous solution has been defined and tested successfully in the CEA. The diagram of the process exhibits two principal steps: in the head-end, a dissolution in HNO 3 medium accompanied with an electrolytic dechlorination leading to a quantitative elimination of chloride as CI 2 gas followed by its trapping one soda lime cartridge, a complete oxidative dissolution of the refractory Pu residues by electrogenerated Ag(II), in the back-end: the Pu and Am recoveries by chromatographic extractions. (authors). 10 figs., 9 refs

Determination of low level of plutonium and uranium isotopes in safeguard swipe sample

Energy Technology Data Exchange (ETDEWEB)

Lee, Myung Ho; Park, Jong Ho; Oh, Seong Yong; Lee, Chang Heon; Ahn, Hong Ju; Song, Kyu Seok [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

2011-10-15

For the determination of radionuclides, the separation techniques based on the principles of anion exchange, liquid-liquid extraction or column extraction chromatography are frequently used in nuclear analytical applications. Recently, a novel extraction chromatographic resin has been developed by Horwitz and co-workers, which are capable of selective extraction of the actinides. General separation of plutonium and uranium with extraction chromatographic techniques are focused on the environmental or radioactive waste samples. Also, the chemical yields for Pu and U isotopes with extraction chromatographic method sometimes are variable. For effective extraction of Pu isotopes in the very level of plutonium sample with UTEVA resin, the valence adjustment of Pu isotopes in the sample solution requires due to unstability in the oxidation state of Pu isotopes during separation step. Therefore, it is necessary to develop a simple and robust radiochemical separation method for nano- or pico gram amounts of uranium and plutonium in safeguard swipe samples. Chemical yields of plutonium and uranium with extraction chromatographic method of Pu and U upgrades in this study were compared with several separation methods for Pu and U generally used in the radiochemistry field. Also, the redox reactions of hydrogen peroxide with plutonium in the nitric acid media were investigated by UV-Vis-NIR absorption spectroscopy. Based on general extraction chromatography method with UTEVA resin, the separation method of nano- and picogram amounts of uranium and plutonium in safeguard swipe samples was developed in this study

Plutonium mobilization from sedimentary sources to solution in the marine environment

International Nuclear Information System (INIS)

Noshkin, V.E.; Wong, K.M.

1979-01-01

Inventories of plutonium radionuclides greatly in excess of global fallout levels persists in the benthic environments of Bikini and Eniwetok Atolls. It now appears that the atolls have reached a chemical steadystate condition with respect to the partitioning of 239+240 Pu between solution and solid phases of the environment. The mobilized 239+240 Pu has solute-like characteristics, passes rapidly and readily through dialysis membranes, has adsorption characteristics similar to those of fallout plutonium in the open ocean, and exists in solution primarily as some oxidized +5 or +6 chemical species. Water-column profiles of 239+240 Pu taken outside the atolls show a plutonium excess in the deep water mass. This remobilized 239+240 Pu possibly originates from the contaminated sediments previously deposited on the outer slopes of the atolls and surrounding basins

Electrochemical studies on plutonium in molten salts

International Nuclear Information System (INIS)

Bourges, G.; Lambertin, D.; Rochefort, S.; Delpech, S.; Picard, G.

2007-01-01

Electrochemical studies on plutonium have been supporting the development of pyrochemical processes involving plutonium at CEA. The electrochemical properties of plutonium have been studied in molten salts - ternary eutectic mixture NaCl-KCl-BaCl 2 , equimolar mixture NaCl-KCl and pure CaCl 2 - and in liquid gallium at 1073 K. The formal, or apparent, standard potential of Pu(III)/Pu redox couple in eutectic mixture of NaCl-KCl-BaCl 2 at 1073 K determined by potentiometry is equal to -2.56 V (versus Cl 2 , 1 atm/Cl - reference electrode). In NaCl-KCl eutectic mixture and in pure CaCl 2 the formal standard potentials deduced from cyclic voltammetry are respectively -2.54 V and -2.51 V. These potentials led to the calculation of the activity coefficients of Pu(III) in the molten salts. Chronoamperometry on plutonium in liquid gallium using molten chlorides - CaCl 2 and equimolar NaCl/KCl - led to the determination of the activity coefficient of Pu in liquid Ga, log γ = -7.3. This new data is a key parameter to assess the thermodynamic feasibility of a process using gallium as solvent metal. By comparing gallium with other solvent metals - cadmium, bismuth, aluminum - gallium appears to be, with aluminum, more favorable for the selectivity of the separation at 1073 K of plutonium from cerium. In fact, compared with a solid tungsten electrode, none of these solvent liquid metals is a real asset for the selectivity of the separation. The role of a solvent liquid metal is mainly to trap the elements

Target fuels for plutonium and minor actinide transmutation in pressurized water reactors

International Nuclear Information System (INIS)

Washington, J.; King, J.; Shayer, Z.

2017-01-01

Highlights: • We evaluate transmutation fuels for plutonium and minor actinide destruction in LWRs. • We model a modified AP1000 fuel assembly in SCALE6.1. • We evaluate spectral shift absorber coatings to improve transmutation performance. - Abstract: The average nuclear power plant produces twenty metric tons of used nuclear fuel per year, containing approximately 95 wt% uranium, 1 wt% plutonium, and 4 wt% fission products and transuranic elements. Fast reactors are a preferred option for the transmutation of plutonium and minor actinides; however, an optimistic deployment time of at least 20 years indicates a need for a nearer-term solution. This study considers a method for plutonium and minor actinide transmutation in existing light water reactors and evaluates a variety of transmutation fuels to provide a common basis for comparison and to determine if any single target fuel provides superior transmutation properties. A model developed using the NEWT module in the SCALE 6.1 code package provided performance data for the burnup of the target fuel rods in the present study. The target fuels (MOX, PuO_2, Pu_3Si_2, PuN, PuUZrH, PuZrH, PuZrHTh, and PuZrO_2) are evaluated over a 1400 Effective Full Power Days (EFPD) interval to ensure each assembly remained critical over the entire burnup period. The MOX (5 wt% PuO_2), Pu_0_._3_1ZrH_1_._6Th_1_._0_8, and PuZrO_2MgO (8 wt% Pu) fuels result in the highest rate of plutonium transmutation with the lowest rate of curium-244 production. This study selected eleven different burnable absorbers (B_4C, CdO, Dy_2O_3, Er_2O_3, Eu_2O_3, Gd_2O_3, HfO_2, In_2O_3, Lu_2O_3, Sm_2O_3, and TaC) for evaluation as spectral shift absorber coatings on the outside of the fuel pellets to determine if an absorber coating can improve the transmutation properties of the target fuels. The PuZrO_2MgO (8 wt% Pu) target fuel with a coating of Lu_2O_3 resulted in the highest rate of plutonium transmutation with the greatest reduction in curium

Target fuels for plutonium and minor actinide transmutation in pressurized water reactors

Energy Technology Data Exchange (ETDEWEB)

Washington, J., E-mail: jwashing@gmail.com [Nuclear Science and Engineering Program, Colorado School of Mines, 1500 Illinois St., Golden, CO 80401 (United States); King, J., E-mail: kingjc@mines.edu [Nuclear Science and Engineering Program, Colorado School of Mines, 1500 Illinois St., Golden, CO 80401 (United States); Shayer, Z., E-mail: zshayer@mines.edu [Department of Physics, Colorado School of Mines, 1500 Illinois St., Golden, CO 80401 (United States)

2017-03-15

Highlights: • We evaluate transmutation fuels for plutonium and minor actinide destruction in LWRs. • We model a modified AP1000 fuel assembly in SCALE6.1. • We evaluate spectral shift absorber coatings to improve transmutation performance. - Abstract: The average nuclear power plant produces twenty metric tons of used nuclear fuel per year, containing approximately 95 wt% uranium, 1 wt% plutonium, and 4 wt% fission products and transuranic elements. Fast reactors are a preferred option for the transmutation of plutonium and minor actinides; however, an optimistic deployment time of at least 20 years indicates a need for a nearer-term solution. This study considers a method for plutonium and minor actinide transmutation in existing light water reactors and evaluates a variety of transmutation fuels to provide a common basis for comparison and to determine if any single target fuel provides superior transmutation properties. A model developed using the NEWT module in the SCALE 6.1 code package provided performance data for the burnup of the target fuel rods in the present study. The target fuels (MOX, PuO{sub 2}, Pu{sub 3}Si{sub 2}, PuN, PuUZrH, PuZrH, PuZrHTh, and PuZrO{sub 2}) are evaluated over a 1400 Effective Full Power Days (EFPD) interval to ensure each assembly remained critical over the entire burnup period. The MOX (5 wt% PuO{sub 2}), Pu{sub 0.31}ZrH{sub 1.6}Th{sub 1.08}, and PuZrO{sub 2}MgO (8 wt% Pu) fuels result in the highest rate of plutonium transmutation with the lowest rate of curium-244 production. This study selected eleven different burnable absorbers (B{sub 4}C, CdO, Dy{sub 2}O{sub 3}, Er{sub 2}O{sub 3}, Eu{sub 2}O{sub 3}, Gd{sub 2}O{sub 3}, HfO{sub 2}, In{sub 2}O{sub 3}, Lu{sub 2}O{sub 3}, Sm{sub 2}O{sub 3}, and TaC) for evaluation as spectral shift absorber coatings on the outside of the fuel pellets to determine if an absorber coating can improve the transmutation properties of the target fuels. The PuZrO{sub 2}MgO (8 wt% Pu) target

Plutonium Oxide Process Capability Work Plan

Energy Technology Data Exchange (ETDEWEB)

Meier, David E. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Tingey, Joel M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

2014-02-28

Pacific Northwest National Laboratory (PNNL) has been tasked to develop a Pilot-scale Plutonium-oxide Processing Unit (P3U) providing a flexible capability to produce 200g (Pu basis) samples of plutonium oxide using different chemical processes for use in identifying and validating nuclear forensics signatures associated with plutonium production. Materials produced can also be used as exercise and reference materials.

Radiative capture on $^{242}$Pu for MOX fuel reactors

CERN Multimedia

The use of MOX fuel (mixed-oxide fuel made of UO$_{2}$ and PuO$_{2}$) in nuclear reactors allows substituting a large fraction of the enriched Uranium by Plutonium reprocessed from spent fuel. Indeed around 66% of the plutonium from spent fuel is made of $^{239}$Pu and $^{241}$Pu, which are fissile in thermal reactors. A typical reactor of this type uses a fuel with 7% reprocessed Pu and 93% depleted U, thus profiting from both the spent fuel and the remaining $^{238}$U following the $^{235}$U enrichment. With the use of such new fuel compositions rich in Pu the better knowledge of the capture and fission cross sections of the Pu isotopes becomes very important. This is clearly stated in the recent OECD NEA’s “High Priority Request List” and in the WPEC-26 “Uncertainty and target accuracy assessment for innovative systems using recent covariance data evaluations” report. In particular, a new series of cross section evaluations have been recently carried out jointly by the European (JEFF) and United ...

Liquid waste processing from plutonium (III) oxalate precipitation

International Nuclear Information System (INIS)

Esteban, A.; Cassaniti, P.; Orosco, E.H.

1990-01-01

Plutonium (III) oxalate filtrates contain about 0.2M oxalic acid, 0.09M ascorbic acid, 0.05M hydrazine, 1M nitric acid and 20-100 mg/l of plutonium. The developed treatment of liquid wastes consist in two main steps: a) Distillation to reduce up to 10% of the initial volume and refluxing to destroy organic material. Then, the treated solution is suitable to adjust the plutonium at the tetravalent state by addition of hydrogen peroxide and the nitric molarity up to 8.6M. b) Recovery and purification of plutonium by anion exchange using two columns in series containing Dowex 1-X4 resin. With the proposed process, it is possible to transform 38 litres of filtrates with 40mg/l of Pu into 0.1 l of purified solution with 15-20g/l of Pu. This solution is suitable to be recycled in the Pu (III) oxalate precipitation process. This process has several potential advantages over similar liquid waste treatments. These include: 1) It does not increase the liquid volume. 2) It consumes only few reagents. 3) The operations involved are simple, requiring limited handling and they are feasible to automatization. 4) The Pu recovery factor is about 99%. (Author) [es

238Pu concentrations in the marine environment at San Clemente Island

International Nuclear Information System (INIS)

Noshkin, V.E.; Brunk, J.L.; Jokela, T.A.; Wong, K.M.

1981-01-01

The concentration of plutonium and other radionuclides measured in samples of surface sediments, seawater and brown algae collected offshore from North Light Harbor Pier at San Clemente Island, CA, are presented. From 1967 to 1978, different forms of nuclear fuels used in operational or proposed SNAP (Systems for Nuclear Auxillary Power) devices were tested at this site to evaluate the effects of seawater on the heat sources. The principle radionuclide in the heat sources tested was 238 Pu. During these tests, small amounts of 238 Pu dissolved and migrated from the test chambers to the local marine environment. Currents dispersed this released 238 Pu so that at present a small increase in concentration above that of fallout background is evident in the surface 3.0-cm layer of near shore sediment that extends over a 3.0-km 2 area surrounding the pier. The 238 Pu associated with this sediment is slowly redissolving and can be taken up by marine algae. Except for a 0.025-km 2 region around the pier, the total plutonium ( 238 Pu + 239+240 Pu) in the surface 3.0-cm layer of sediment is within the range of total fallout plutonium reported in Atlantic and Pacific surface deposits from water depths less than 100 m. (author)

Determination of plutonium and uranium in the same aliquot by potentiometric titration

International Nuclear Information System (INIS)

Karekar, C.V.; Chander, Keshav; Nair, G.M.; Natarajan, P.R.

1986-01-01

A potentiometric titration method was developed for the determination of plutonium and uranium in the same aliquot in nitric acid medium. Plutonium was first determined by oxidation to Pu(VI) by fuming with HClO 4 . Pu(VI) was reduced to Pu(IV) with known excess of Fe(II). Uranium in the same solution was determined by reduction to U(IV) with Fe(II) in H 3 PO 4 medium. For the quantity of plutonium and uranium in the range of 3-5 mg per aliquot a precision of +-0.2% and +-0.4%, respectively, was obtained. (author)

Ultra-sensitive detection of plutonium by accelerator mass spectrometry

Energy Technology Data Exchange (ETDEWEB)

Fifield, L K; Cresswell, R G; Ophel, T R; Ditada, M [Australian National Univ., Canberra, ACT (Australia). Dept. of Nuclear Physics; Day, J P; Clacher, A [Manchester Univ. (United Kingdom). Dept. of Chemistry; Priest, N D [AEA Technology, Harwell (United Kingdom)

1997-12-31

On the bases of the measurements performed to date, a sensitivity of 10{sup 6} atoms is achievable with accelerator mass spectroscopy (AMS) for each of the plutonium isotopes. Not only does this open the way to the sort of study outlined, but it also makes possible other novel applications, of which two examples are given: (i)the ration of {sup 240}Pu to {sup 239}Pu as a sensitive indicator of the source of the plutonium; (ii) the biochemistry of plutonium in humans. The ultra-sensitive atom counting capability of AMS will make it possible to use the very long-lived {sup 244}Pu (8x10{sup 7}a) in human volunteer studies without any significant increase in radiation body burden. This paper will describe the AMS technique as applied to plutonium using the ANU`s 14UD accelerator, will present the results obtained to date, and will discuss the prospects for the future.

Ultra-sensitive detection of plutonium by accelerator mass spectrometry

Energy Technology Data Exchange (ETDEWEB)

Fifield, L.K.; Cresswell, R.G.; Ophel, T.R.; Ditada, M. [Australian National Univ., Canberra, ACT (Australia). Dept. of Nuclear Physics; Day, J.P.; Clacher, A. [Manchester Univ. (United Kingdom). Dept. of Chemistry; Priest, N.D. [AEA Technology, Harwell (United Kingdom)

1996-12-31

On the bases of the measurements performed to date, a sensitivity of 10{sup 6} atoms is achievable with accelerator mass spectroscopy (AMS) for each of the plutonium isotopes. Not only does this open the way to the sort of study outlined, but it also makes possible other novel applications, of which two examples are given: (i)the ration of {sup 240}Pu to {sup 239}Pu as a sensitive indicator of the source of the plutonium; (ii) the biochemistry of plutonium in humans. The ultra-sensitive atom counting capability of AMS will make it possible to use the very long-lived {sup 244}Pu (8x10{sup 7}a) in human volunteer studies without any significant increase in radiation body burden. This paper will describe the AMS technique as applied to plutonium using the ANU`s 14UD accelerator, will present the results obtained to date, and will discuss the prospects for the future.

Plutonium in nature; Le plutonium dans la nature

Energy Technology Data Exchange (ETDEWEB)

Madic, C.

1994-12-31

Plutonium in nature comes from natural sources and anthropogenic ones. Plutonium at the earth surface comes principally from anthropogenic sources. It is easily detectable in environment. The plutonium behaviour in environment is complex. It seems necessary for the future to reduce releases in environment, to improve predictive models of plutonium behaviour in geosphere, to precise biological impact of anthropogenic plutonium releases.

Advances on reverse strike co-precipitation method of uranium-plutonium mixed solutions

International Nuclear Information System (INIS)

Menghini, Jorge E.; Marchi, Daniel E.; Orosco, Edgardo H.; Greco, Luis

2000-01-01

The reverse strike coprecipitation of uranium-plutonium mixed solutions, is an alternative way to obtain MOX fuel pellets. Previous tests, carried out in the Alpha Laboratory, included a stabilization step for transforming 100 % of plutonium into Pu +4 . Therefore, the plutonium precipitated as Pu(OH) 4 . In this second step, the stabilization process was suppressed. In this way, besides Pu(OH) 4 , a part of the precipitated is composed of a mixed salt: AD(U,Pu). Then, a homogeneous solid solution is formed in the early steps of the process. The powders showed higher tap density, better performance during the pressing and lower sinterability than the powders obtained in previous tests. The advantageous and disadvantageous effects of the stabilization step are analyzed in this paper. (author)

Plutonium determination in solution with excess hydrofluoric acid

International Nuclear Information System (INIS)

Krtil, J.; Kuvik, V.; Spevackova, V.

1975-01-01

The determination is described of plutonium in solutions in the presence of fluoride ions resulting from the hydrolysis of PuF 6 . The method is based on reduction of Pu(VI) by excess of Fe(II) and on re-titration of Fe(II) with ceric salt. The effect of fluoride ions on plutonium determination was studied. It was found that a 3 mole excess of HF with respect to Pu decreased the results of Pu determination. The interference of fluoride ions was eliminated by a two-fold evaporation of the solution to be titrated with HNO 3 to dryness or by complex formation with boric arid. The amount of 20.50 mg Pu in the presence of a 10 mole excess of fluoride ions (17 mg HF) was determined with an error of +- 0.09 mg ). (author)

Radiolytic and thermal stability of selected plutonium salts containing nitrate groups

International Nuclear Information System (INIS)

Bryan, G.H.

1976-04-01

(Pu(NO 3 ) 4 . XH 2 O, K 2 Pu(NO 3 ) 6 , and (NH 4 ) 2 Pu(NO 3 ) 6 ) were studied to evaluate their ability to serve as shipping forms that meet criteria. The radiolytic gas evolution study eliminated (NH 4 ) 2 Pu(NO 3 ) 6 from further consideration. None of the compounds produced H 2 or O 2 in sufficient quantity to produce a flammable mixture, except Pu(NO 3 ) 4 . XH 2 O which produced O 2 and H 2 in a ratio that is above explosive limits after long storage time. The ammonium salt decomposition appears to be about the same as that observed upon heating of NH 4 NO 3 to produce N 2 , H 2 O, and nitrous oxides. Plutonium nitrate contains hydration water. This water is of some concern due to the production of hydrogen by alpha-radiolysis. Two waters of hydration appear to be the lower limit to which Pu(NO 3 ) 4 . XH 2 O may be taken before decomposition of the solid begins. TGA results indicate the simple nitrate (Pu(NO 3 ) 4 . XH 2 O) is somewhat less thermally stable than either the ammonium or potassium hexanitrato plutonate which detracts somewhat from its suitability as a shipping form. Maintaining large quantities of this compound with a high 238 Pu content (less than 1 percent 238 Pu) may require specially designed and larger containers to prevent thermal degradation and gas pressure buildup problems. The informaion was presented to plutonium processors; the final consensus of this group was that in spite of some thermal instability of Pu(NO 3 ) 4 . XH 2 O at fairly low temperatures, it was preferable to K 2 Pu(NO 3 ) 6 due to the additional waste disposal problems the potassium would present. (Pu(NO 3 ) 4 . XH 2 O also has several other advantages. A possible problem that could arise due to the variable weight of plutonium nitrate could be in plutonium accountability, but this would be prevented if the plutonium content of the solution prior to evaporation to the solid is known

Sources of plutonium to the great Miami River

International Nuclear Information System (INIS)

Bartelt, G.E.; Kennedy, C.W.; Bobula, C.M. III.

1978-01-01

Progress is reported in the study of 238 Pu, in the Great Miami River watershed the contribution of various sources to the total 238 Pu transported by the river. Periodic discharges of industrial wastewater from Mound Laboratory from 1973 to 1975 have released approximately 20 mCi of 238 Pu each year to the Great Miami River. Changes in the wastewater treatment system in 1976 have reduced the annual discharge to less than 3 mCi/year. However, despite this sevenfold reduction of plutonium in the wastewater discharge, the annual flux of 238 Pu down the river has remained relatively constant and is approximately 10 times greater than can be accounted for by the reported effluent discharges. Therefore, other sources of the 238 Pu in the Great Miami River exist. A second possible source of plutonium is the resuspension of sediments enriched by earlier waste water releases and deposited in the river. However, since there appear to be few areas where large accumulations of sediment could occur, it seems improbable that resuspension of earlier sediment deposits would continue to be a significant contributor to the annual flux of plutonium. A much more likely source is the continuing erosion of soil from a canal and stream system contaminated with approx. 5 Ci of 238 Pu, 7 which connects directly to the river 6.9 km upstream from Franklin. Results from samples analyzed in 1978 show the average concentration of 238 Pu in suspended sediments from the canal to be approximately 10 3 times greater than suspended sediment concentrations in the river and waste water effluent.Thus the main contributor to the total amount of plutonium transported by the Great Miami River appears to be highly enriched sediment from the canal, which is eroded into the river where it is then diluted by uncontaminated sediments

Breeding and plutonium characterization analysis on actinides closed water-cooled thorium reactor

International Nuclear Information System (INIS)

Permana, Sidik; Sekimoto, Hiroshi; Takaki, Naoyuki

2009-01-01

Higher difficulties (barrier) or more complex design of nuclear weapon, material fabrication and handling and isotopic enrichment can be achieved by a higher isotopic barrier. The isotopic material barrier includes critical mass, heat-generation rate, spontaneous neutron generation and radiation. Those isotopic barriers in case of plutonium isotope is strongly depend on the even mass number of plutonium isotope such as 238 Pu, 240 Pu and 242 Pu and for 233 U of thorium cycle depends on 232 U. In this present study, fuel sustainability as fuel breeding capability and plutonium characterization as main focus of proliferation resistance analysis have been analyzed. Minor actinide (MA) is used as doping material to be loaded into the reactors with thorium fuel. Basic design parameters are based on actinide closed-cycle reactor cooled by heavy water. The evaluation use equilibrium burnup analysis coupled with cell calculation of SRAC and nuclear data library is JENDL.32. Parametrical survey has been done to analyze the effect of MA doping rate, different moderation ratio for several equilibrium burnup cases. Plutonium characterization which based on plutonium isotope composition is strongly depending on MA doping concentration and different moderation conditions. Breeding condition can be achieved and high proliferation resistance level can be obtained by the present reactor systems. Higher isotopic plutonium composition of Pu-238 (more than 40%) can be obtained compared with other plutonium isotopes. In addition, higher moderation ratio gives the isotope composition of 238 Pu increases, however, it obtains lower composition when MA doping is increased and it slightly lower composition for higher burnup. Meanwhile, higher 240 Pu composition can be achieved by higher MA doping rate as well as for obtaining higher breeding capability. (author)

EXAFS study of plutonium sorption onto kaolinite

International Nuclear Information System (INIS)

Reich, T.Y.; Banik, L.; Buda, R.A.; Amayri, S.; Drebert, J.; Kratz, J.V.; Trautmann, N.; Reich, T.; Ageev, A.L.; Korshunov, M.E.

2007-01-01

The uptake mechanism of plutonium by kaolinite was investigated by applying X-ray absorption spectroscopy to batch sorption samples (total Pu concentrations 1 and 10 μM; 4 g kaolinite/L in 0.1 M NaClO 4 ; 1 ≤ pH ≤ 9; presence and absence of ambient CO 2 ). For XAFS measurements, one sample was prepared from a Pu(III) solution at pH 6 under argon atmosphere. Three samples were obtained by sorption of Pu(IV) at pH I, 4, and 9 in an air-equilibrated system. The Pu L III -edge XANES spectra indicated that in all samples, including the Pu(III) sample, plutonium is sorbed at the kaolinite surface as Pu(IV). The Pu L III -edge k 3 -weighted EXAFS spectra showed eight oxygen atoms at an average Pu-O distance of 2.3 angstrom. Two Pu atoms were detected at ∼ 3.7 angstrom in all spectra, indicating the formation of polynuclear Pu(IV) species at the kaolinite surface. For the sample prepared from Pu(III) solution, an additional Pu-O shell at 3.2 angstrom was observed. The spectra of samples prepared from Pu(IV) included a Pu-Al/Si co-ordination shell at approximately 3.6 angstrom, indicating formation of inner-sphere sorption complexes. The structural models used in the least-squares fits were confirmed by an alternative EXAFS data analysis approach based on a modified Tikhonov regularization method. (authors)

Plutonium fallout at Fayetteville, AR

International Nuclear Information System (INIS)

Sandoval, D.N.; Essien, I.O.; Kuroda, P.K.

1985-01-01

It is well established that atmospheric Pu fallout has its origin in the testing of nuclear devices and satellite accidents. Monitoring injections of Pu during the testing of nuclear devices can be useful in characterizing the detonation and subsequently tagging its global fallout. Since Pu uptake pathway into humans is mainly through the respiratory and digestive systems, it is important to know about the behavior of Pu in the atmosphere. Snow and rain samples were collected between Jan 1981 and April 1983, and analyzed for plutonium

MICROBIAL TRANSFORMATIONS OF PLUTONIUM AND IMPLICATIONS FOR ITS MOBILITY.

Energy Technology Data Exchange (ETDEWEB)

FRANCIS, A.J.

2000-09-30

The current state of knowledge of the effect of plutonium on microorganisms and microbial activity is reviewed, and also the microbial processes affecting its mobilization and immobilization. The dissolution of plutonium is predominantly due to their production of extracellular metabolic products, organic acids, such as citric acid, and sequestering agents, such as siderophores. Plutonium may be immobilized by the indirect actions of microorganisms resulting in changes in Eh and its reduction from a higher to lower oxidation state, with the precipitation of Pu, its bioaccumulation by biomass, and bioprecipitation reactions. In addition, the abundance of microorganisms in Pu-contaminated soils, wastes, natural analog sites, and backfill materials that will be used for isolating the waste and role of microbes as biocolloids in the transport of Pu is discussed.

Study of the magnetic susceptibilities of some plutonium derivatives; Etude des susceptibilites magnetiques de quelques derives du plutonium

Energy Technology Data Exchange (ETDEWEB)

Raphael, G [Commissariat a l' Energie Atomique, Fontenay-aux-Roses (France). Centre d' Etudes Nucleaires

1969-06-01

We present a detailed description of an automatic recording apparatus for magnetic susceptibility measurement of radioactive samples in the temperature range 4 K - 1200 K. We have measured the magnetic susceptibility of various plutonium compounds: - PuO{sub 2}, Pu{sub 2}O{sub 3}, PuO{sub 2-x}, - PuS, Pu{sub 2}S{sub 3}, Pu{sub 3}S{sub 4}, (U{sub x}Pu{sub 1-x})S - PuN - PuC{sub 1-x}(N,O,H,vacancy), Pu{sub 2}C{sub 3}, (U{sub 0.85}Pu{sub 0.15})C. The curves of susceptibilities versus temperature show many magnetic transitions. The interpretation of these results shows the existence of magnetic moments carried by the 5 f electrons and localized on the metallic sites as well as the great influence of the 'crystal field' in all these compounds. (author) [French] Nous decrivons d'une facon detaillee un appareil permettant de mesurer d'une facon continue et automatique des susceptibilites magnetiques sur des echantillons radioactifs dans un domaine de temperature s'etalant de 4 K a 1200 K. Nous avons mesure les susceptibilites magnetiques de certains composes du plutonium tels que: - PuO{sub 2}, Pu{sub 2}O{sub 3}, PuO{sub 2-x} - PuS, Pu{sub 2}S{sub 3}, Pu{sub 3}S{sub 4}, (U{sub x}Pu{sub 1-x})S - PuN - PuC{sub 1-x}(N,O,H,vacancy), Pu{sub 2}C{sub 3}, (U{sub 0.85}Pu{sub 0.15})C. Les courbes de susceptibilite magnetique en fonction de la temperature mettent en evidence de nombreuses transitions magnetiques. L'interpretation de ces resultats a montre l'existence de moments magnetiques portes par les electrons f et localises sur les sites metalliques ainsi que l'influence tres grande du champ cristallin. (auteur)

Concentration of plutonium in desert plants from contaminated area

International Nuclear Information System (INIS)

Xu Hui; Jin Yuren; Tian Mei; Li Weiping; Zeng Ke; Wang Yaoqin; Wang Yu

2012-01-01

The investigation of plutonium in desert plants from contaminated sites contributes to the evaluation of its pollution situation and to the survey of plutonium hyper accumulator. The concentration of 239 Pu in desert plants collected from a contaminated site was determined, and the influence factors were studied. The concentration of 239 Pu in plants was (1.8±4.9) Bq/kg in dry weight, and it means that the plants were contaminated, moreover, the resuspension results in dramatic plutonium pollution of plant surface. The concentration of plutonium in plants depends on species, live stages and the content of plutonium in the rhizosphere soil. The concentration of plutonium in herbage is higher than that in woody plant, and for the seven species of desert plants investigated, it decreases in the order of Hexinia polydichotoma, Phragmites australis, Halostashys caspica, Halogeton arachnoideus, Lycium ruthenicum, Tamarix hispida and Calligonum aphyllum. (authors)

Adsorption and diffusion of plutonium in soil

International Nuclear Information System (INIS)

Brown, D.A.

The behavior of plutonium (Pu) was studied in three soils that varied in texture, CEC, pH, organic matter content and mineralogy (Fuquay, Muscatine, Burbank). Two isotopes, 238 Pu and 239 Pu, were used in order to detect Pu over a range of several orders of magnitude. Unless added in a chelated form, Pu was added to the soil as a nitrate in .01 N HNO 3 to simulate the release of acidic waste on the soil and to prevent rapid Pu hydrolysis or polymerization

The removal of inhaled 239Pu and 238Pu from beagle dogs by lung lavage and chelation treatment

International Nuclear Information System (INIS)

Muggenburg, B.A.; Mewhinney, J.A.; Miglio, J.J.; Slauson, D.O.; McClellan, R.O.

1976-01-01

Studies were conducted in beagle dogs to determine the efficiency of treatment by lung lavage and injections of chelating agents in removing inhaled plutonium of varied chemical forms and particle sizes. Polydisperse aerosols of 239 Pu were produced at different temperatures from 325 0 C to 1150 0 C to evaluate the effect of the chemical form of the particles. Aerosols of 238 Pu were produced at 1150 0 C only but were of different particle size or size distributions. Three dogs that inhaled each different plutonium aerosol were treated by lung lavages starting two days after the exposure. Subsequent lavages were performed on days 7, 10, 14, 21, 28, 35, 42, and 49 after exposure. Intravenous injections of 100 mg of diethylenetriaminepentaacetic acid (DTPA) as the calcium salt were given on days 1, 2, 3 and 4 after exposure and twice weekly thereafter to the time of sacrifice, 56 days after exposure. The 10 lung lavages removed from 18 to 49% of the initial lung burden of plutonium. The recovery of plutonium by lavage was similar irrespective of the temperature at which the aerosol was produced, however, lavage recovery decreased somewhat with increasing particle size. The efficacy of DTPA treatment increased with decreasing production temperature of the 239 Pu. Treatment with DTPA was not affected by particle size of the 0.8- and 1.9-μm monodisperse 239 Pu aerosol. The effectiveness of lung lavage decreased as the solubility of the aerosol particles increased whereas the effectiveness of the DTPA treatment increased as the solubility of the inhaled aerosol increased as shown by the lowest temperature aerosol and the aerosol-containing soluble fraction. These findings correlated qualitatively with a 2-hour in-vitro solubility test on the exposure aerosols. (author)

Behavior of plutonium isotopes in the marine environment of Enewetak atoll

International Nuclear Information System (INIS)

Noshkin, V.E.; Robison, W.L.; Eagle, R.J.

1998-01-01

There continue to be reports in the literature that suggest a difference in the behavior of 239+240 Pu and 238 Pu in some aquatic environments. Plutonium isotopes have been measured in marine samples collected over 3 decades form Enewetak atoll, one of the sites in the Marshall Islands used by the United States between 1946 and 1958 to test nuclear devices. The plutonium isotopes originated from a variety of complex sources and could possibly coexist in this environment as different physical-chemical species. However results indicate little difference in the mobility and biological availability of 239+240 Pu and 238 Pu. (author)

Color center formation in plutonium electrorefining residues

International Nuclear Information System (INIS)

Morris, D.E.; Eller, P.G.; Hobart, D.E.; Eastman, M.P.; McCurry, L.E.

1989-01-01

Plutonium electrorefining residues containing Pu(III) in KCl exhibit dramatic reversible, light-induced color changes. Similar color changes were observed in Ln-doped (Ln = La, Nd, Gd, and Lu) and undoped KCl samples which were subjected to intense gamma irradiation. Diffuse reflectance electronic and electron paramagnetic resonance spectroscopies were used to show conclusively that Pu(III) is present in both the bleached and unbleached plutonium-bearing residues and the spectacular color changes are the result of color center formation and alternation by visible light. (orig.)

Decontamination of alpha-bearing solid wastes and plutonium recovery

International Nuclear Information System (INIS)

Koehly, G.; Madic, C.; Lecomte, M.; Bourges, J.; Saulze, J.L.; Broudic, J.C.

1993-01-01

Nuclear activities in the Radiochemistry building of Fontenay-aux-Roses Nuclear Research Center concern principally the study of fuel reprocessing and the production of transuranium isotopes. During these activities solid wastes are produced. In order to improve the management of these wastes, it has been decided to build new facilities: a group of three glove-boxes named ELISE for the treatment of α active solid waste and a hot-cell, PROLIXE, for the treatment of solid wastes. Leaching processes were developed in order to: decontaminate these wastes and recover actinide elements, particularly the highly valuable plutonium, from the leachates. The processes developed are sufficiently flexible to be able to accommodate solid wastes produced in other facilities. Laboratory studies were conducted to develop the leaching process based on the use of electrogenerated Ag(II) species which is particularly suitable to provoke the dissolution of PuO 2 . Successful exhaustive Pu decontaminations with DF(Pu) higher than 10 4 were achieved for the first time during the treatment of stainless steel PuO 2 cans (future MELOX plant) by electrogenerated Ag (II) in nitric acid medium

Absorption, transport, and chemical fate of plutonium in soybean plants

International Nuclear Information System (INIS)

Garland, T.R.; Cataldo, D.A.; Wildung, R.E.

1981-01-01

Absorption of plutonium (Pu) by soybean plants (Glycine max cv. Williams) is limited by Pu solubility in soils. Changes in Pu concentration in different tissues with time to senescence indicate Pu is freely transported through the xylem during growth but not subject to remobilization on flowering. Studies in which the DTPA complex of 238 Pu was supplied to the plant suggest a change in chemical form following root absorption. Of the Pu in roots, stems, and leaves at senescence, 28, 54, and 67%, respectively, were soluble. The Pu in the solluble fraction was primarily associated with components of >10000 equivalent molecular weight in leaves and roots, whereas stems exhibited an equal distribution between components in the >10000 and <500 molecular weight fractions. Plutonium associated with mature seeds is concentrated in the seed hull (85%) and cotyledons (14%). The Pu associated with the cotyledon was primarily in the insoluble residues and soluble soy whey

Average Structure Evolution of δ-phase Pu-Ga Alloys

Energy Technology Data Exchange (ETDEWEB)

Smith, Alice Iulia [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Page, Katharine L. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); Gourdon, Olivier [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Siewenie, Joan E. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); Richmond, Scott [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Saleh, Tarik A. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Ramos, Michael [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Schwartz, Daniel S. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

2015-03-30

[Full Text] Plutonium metal is a highly unusual element, exhibiting six allotropes at ambient pressure, from room temperature to its melting point. Many phases of plutonium metal are unstable with temperature, pressure, chemical additions, and time. This strongly affects structure and properties, and becomes of high importance, particularly when considering effects on structural integrity over long time periods. The fcc δ-phase deserves additional attention, not only in the context of understanding the electronic structure of Pu, but also as one of the few high-symmetry actinide phases that can be stabilized down to ambient pressure and room temperature by alloying it with trivalent elements. We will present results on recent work on aging of Pu-2at.%Ga and Pu-7at.%Ga alloys

Plutonium concentrations in airborne soil at Rocky Flats and Hanford determined during resuspension experiments

International Nuclear Information System (INIS)

Sehmel, G.A.

1978-01-01

Plutonium resuspension results are summarized for experiments conducted by the author at Rocky Flats, onsite on the Hanford reservation, and for winds blowing from offsite onto the Hanford reservation near the Prosser barricade boundary. In each case, plutonium resuspension was shown by increased airborne plutonium concentrations as a function of either wind speed or as compared to fallout levels. All measured airborne concentrations were far below maximum permissible concentrations (MPC). Both plutonium and cesium concentrations on airborne soil were normalized by the quantity of airborne soil sampled. Airborne radionuclide concentrations in μCi/g were related to published values for radionuclide concentrations on surface soils. For this ratio of radionuclide concentration per gram on airborne soil divided by that for ground surface soil, there are eight orders of magnitude uncertainty from 10 -4 to 10 4 . This uncertainty in the equality between plutonium concentrations per gram on airborne and surface soils is caused by only a fraction of the collected airborne soil being transported from offsite rather than all being resuspended from each study site and also by the great variabilities in surface contamination. Horizontal plutonium fluxes on airborne nonrespirable soils at all three sites were bracketed within the same four orders of magnitude from 10 -7 to 10 -3 μCi/(m 2 day) for 239 Pu and 10 -8 to 10 -5 μCi/(m 2 day) for 238 Pu. Airborne respirable 239 Pu concentrations increased with wind speed for a southwest wind direction coming from offsite near the Hanford reservation Prosser barricade. Airborne plutonium fluxes on nonrespirable particles had isotopic ratios, 240 Pu/ 239 240 Pu, similar to weapons grade plutonium rather than fallout plutonium

Direct spectrophotometric analysis of low level Pu (III) in Pu(IV) nitrate solution

International Nuclear Information System (INIS)

Mageswaran, P.; Suresh Kumar, K.; Kumar, T.; Gayen, J.K.; Shreekumar, B.; Dey, P.K.

2010-01-01

Among the various methods demonstrated for the conversion of plutonium nitrate to its oxide, the oxalate precipitation process either as Pu (III) or Pu (IV) oxalate gained wide acceptance. Since uranous nitrate is the most successful partitioning agent used in the PUREX process for the separation of Pu from the bulk amount of U, the Pu (III) oxalate precipitation of the purified nitrate solution will not give required decontamination from U. Hence Pu IV oxalate precipitation process is a better option to achieve the end user's specified PuO 2 product. Prior to the precipitation process, ensuring of the Pu (IV) oxidation state is essential. Hence monitoring of the level of Pu oxidation state either Pu (III) or Pu (IV) in the feed solution plays a significant role to establish complete conversion of Pu (III). The method in vogue to estimate Pu(lV) content is extractive radiometry using Theonyl Trifluoro Acetone (TTA). As the the method warrants a sample preparation with respect to acidity, a precise measurement of Pu (IV) without affecting the Pu(III) level in the feed sample is difficult. Present study is focused on the exploration of direct spectrophotometry using an optic fiber probe of path length of 40mm to monitor the low level of Pu(III) after removing the bulk Pu(lV) which interfere in the Pu(III) absorption spectrum, using TTA-TBP synergistic mixture without changing the sample acidity

Biological behaviour of plutonium given as a trilaurylamine complex. Comparison with plutonium-tributylphosphate

International Nuclear Information System (INIS)

Nolibe, D.; Duserre, C.; Gil, I.; Rateau, G.; Metivier, H.

1989-01-01

The biokinetics of plutonium (Pu) were compared in rats after its administration by inhalation or intramuscular injection as Pu-trilaurylamine (Pu-TLA) or Pu-tri-n-butylphosphate (Pu-TBP). To study the mass effect, 238 Pu and 239 Pu were used. Translocation from the lungs and injection site was faster for 238 Pu than 239 Pu, and faster for Pu-TLA than Pu-TBP. The skeleton was always the main organ of deposition of the transferable Pu fraction. At 50 days after inhalation, the skeletal content, in per cent of the body content at death was 10% for 239 Pu-TBP, 54% for 238 Pu-TBP, 24% for 239 Pu-TLA and 62% for 238 Pu-TLA. The amounts in the liver were respectively 2, 6, 3, and 10% of the body content. Thirty days after intramuscular injection of 239 Pu-TLA, more Pu was translocated than after 239 Pu-TBP (26% versus 16%) and the skeletal deposit was 10 times the deposit in the liver. DTPA therapy after inhalation or injection of 238 Pu-TLA reduced the skeletal content by 35-58% with a corresponding increase in urinary excretion. (author)

Calculation of thermodynamic equilibrium for reactions of plutonium with air

International Nuclear Information System (INIS)

Zou Lexi; Sun Ying; Luo Deli; Xue Weidong; Zhu Zhenghe; Wang Rong

2000-01-01

There are six independent component with 4 chemical elements, i.e. PuH 2.7 (s), PuN(s), Pu 2 O 3 (s), N 2 (g) and H 2 (g), therefore, the system described involves of 2 independent reactions, both ΔG degree << O. The mass balances calculated for gas and solid phases are in good agreement with those of experimental, indicating the chemical equilibrium is nearly approached. So, it is believed that the reaction ratio of plutonium hydride with air is extremely rapid. The results are meaningful to the storage of plutonium

A 233U/236U/242Pu/244Pu spike for isotopic and isotope dilution analysis by mass spectrometry with internal calibration

International Nuclear Information System (INIS)

Stepanov, A.; Belyaev, B.; Buljanitsa, L.

1989-11-01

The Khlopin Radium Institute prepared on behalf of the IAEA a synthetic mixture of 233 U, 236 U, 242 Pu and 244 Pu isotopes. The isotopic composition and elemental concentration of uranium and plutonium were certified on the basis of analyses done by four laboratories of the IAEA Network, using mass spectrometry with internal standardization. The certified values for 233 U/ 236 U ratio and the 236 U chemical concentration have a coefficient of variation of 0.05%. The latter is fixed by the uncertainty in the 235 U/ 238 U ratio of NBS500 used as internal standard. The coefficients of variation of the 244 Pu/ 242 Pu ratio and the 242 Pu chemical concentration are respectively 0.10% and 0.16% and limited by the uncertainty in the 240 Pu/ 239 Pu ratio of NBS947. This four isotope mixture was used as an internal standard as well as a spike, to analyze 30 batches of LWR spent fuel solutions. The repeatability of the mass spectrometric measurements have a coefficient of variation of 0.025% for the uranium concentration, and of 0.039% for the plutonium concentration. The spiking and treatment errors had a coefficient of variation of 0.048%. (author). Refs, figs and tabs

Calculation of Plutonium content in RSG-GAS spent fuel using IAFUEL computer code

International Nuclear Information System (INIS)

Mochamad-Imron

2003-01-01

It has been calculated the contain of isotopes Pu-239, Pu-240, Pu-241, and isotope Pu-242 in MTR reactor fuel types which have U-235 contain about 250 gram. The calculation was performed in three steps. The first step is to determine the library of calculation output of BOC (Beginning of Cycle). The second step is to determine the core isotope density, the weight of plutonium for one core, and one fuel isotope density. The third step is to calculate weight of plutonium in gram. All calculation is performed by IAFUEL computer code. The calculation was produced content of each Pu isotopes were Pu-239 is 6.7666 gr, Pu-240 is 1.4628 gr, Pu-241 is 0.52951 gr, and Pu-242 is 0.068952 gr

A rapid and specific titrimetric method for the precise determination of plutonium using redox indicator

International Nuclear Information System (INIS)

Chitnis, R.T.; Dubey, S.C.

1976-01-01

A simple and rapid method for the determination of plutonium in plutonium nitrate solution and its application to the purex process solutions is discussed. The method involves the oxidation of plutonium to Pu(VI) with the help of argentic oxide followed by the destruction of the excess argentic oxide by means of sulphamic acid. The determination of plutonium is completed by adding ferrous ammonium sulphate solution which reduces Pu(VI) to Pu(IV) and titrating the excess ferrous with standard potassium dichromate solution using sodium diphenylamine sulphonate as the internal indicator. The effect of the various reagents add during the oxidation and reduction of plutonium, on the final titration has been investigated. The method works satisfactorily for the analysis of plutonium in the range of 0.5 to 5 mg. The precision of the method is found to be within 0.1%. (author)

Chemical speciation of plutonium in the radioactive waste burial ground at the Savannah River Plant

International Nuclear Information System (INIS)

Wilhite, E.L.

1978-08-01

The plutonium chemical species in two types of samples from the Savannah River Plant burial ground for radioactive waste were identified. Samples analyzed were water and sediment from burial ground monitoring well C-17 and soil from an alpha waste burial trench. Soluble plutonium in the monitoring well was less than 12A in diameter, was cationic, and contained about 43% Pu(VI) and 25% Pu(IV). The equilibrium distribution coefficient (K /sub d/) for soluble plutonium from the well water (pH 7) to burial ground soil was about 60. Soil plutonium from the waste trench was not cation-exchanged; 78% of the soil plutonium was associated with metallic oxides in the soil. Approximately 9% of the Pu was contained in the crystalline soil matrix. Thus, about 87% of the plutonium in the soil was in a relatively immobile form. Ion-exchangeable and organic acid forms of plutonium amounted to only about 2.5% each. The bulk of the plutonium now on burial ground soils will be immobile except for movement of soil particles containing plutonium. 6 tables

Plutonium Consumption Program, CANDU Reactor Project final report

Energy Technology Data Exchange (ETDEWEB)

1994-07-31

DOE is investigating methods for long term dispositioning of weapons grade plutonium. One such method would be to utilize the plutonium in Mixed OXide (MOX) fuel assemblies in existing CANDU reactors. CANDU (Canadian Deuterium Uranium) reactors are designed, licensed, built, and supported by Atomic Energy of Canada Limited (AECL), and currently use natural uranium oxide as fuel. The MOX spent fuel assemblies removed from the reactor would be similar to the spent fuel currently produced using natural uranium fuel, thus rendering the plutonium as unattractive as that in the stockpiles of commercial spent fuel. This report presents the results of a study sponsored by the DOE for dispositioning the plutonium using CANDU technology. Ontario Hydro`s Bruce A was used as reference. The fuel design study defined the optimum parameters to disposition 50 tons of Pu in 25 years (or 100 tons). Two alternate fuel designs were studied. Safeguards, security, environment, safety, health, economics, etc. were considered. Options for complete destruction of the Pu were also studied briefly; CANDU has a superior ability for this. Alternative deployment options were explored and the potential impact on Pu dispositioning in the former Soviet Union was studied. An integrated system can be ready to begin Pu consumption in 4 years, with no changes required to the reactors other than for safe, secure storage of new fuel.

Plutonium Consumption Program, CANDU Reactor Project final report

International Nuclear Information System (INIS)

1994-01-01

DOE is investigating methods for long term dispositioning of weapons grade plutonium. One such method would be to utilize the plutonium in Mixed OXide (MOX) fuel assemblies in existing CANDU reactors. CANDU (Canadian Deuterium Uranium) reactors are designed, licensed, built, and supported by Atomic Energy of Canada Limited (AECL), and currently use natural uranium oxide as fuel. The MOX spent fuel assemblies removed from the reactor would be similar to the spent fuel currently produced using natural uranium fuel, thus rendering the plutonium as unattractive as that in the stockpiles of commercial spent fuel. This report presents the results of a study sponsored by the DOE for dispositioning the plutonium using CANDU technology. Ontario Hydro's Bruce A was used as reference. The fuel design study defined the optimum parameters to disposition 50 tons of Pu in 25 years (or 100 tons). Two alternate fuel designs were studied. Safeguards, security, environment, safety, health, economics, etc. were considered. Options for complete destruction of the Pu were also studied briefly; CANDU has a superior ability for this. Alternative deployment options were explored and the potential impact on Pu dispositioning in the former Soviet Union was studied. An integrated system can be ready to begin Pu consumption in 4 years, with no changes required to the reactors other than for safe, secure storage of new fuel

Compositions of airborne plutonium-bearing particles from a plutonium finishing operation

International Nuclear Information System (INIS)

Sanders, S.M. Jr.

1976-11-01

The elemental composition of 111 plutonium-bearing particles was determined (using an electron microprobe) as part of a program to investigate the origin and behavior of the long-lived transuranic radionuclides released from fuel reprocessing facilities at the Savannah River Plant. These particles, collected from wet-cabinet and room-air exhausts from the plutonium finishing operation (JB-Line), were between 0.4 and 36 μm in diameter. Ninety-nine of the particles were found to be aggregates of various minerals and metals, six were quartz, and six were small (less than 2-μm-diameter) pieces of iron oxide. Collectively, these particles contained less minerals and more metals than natural dusts contain. The metallic constituents included elements normally not found in dusts, e.g., chromium, nickel, copper, and zinc. Concentrations of aluminum and iron exceeded those normally found in minerals. Elemental concentrations in individual particles covered a wide range: one 2-μm-diameter particle contained 97 percent NiO, a 9-μm-diameter particle contained 72 percent Cr 2 O 3 . Although the particles were selected because they produced plutonium fission tracks, the plutonium concentration was too low to be estimated by microprobe analysis in all but a 1-μm-diameter particle. This plutonium-bearing particle contained 73 percent PuO 2 by weight in combination with Fe 2 O 3 and mica; its activity was estimated at 0.17 pCi of 239 Pu

Reduction of uranium and plutonium oxides by aluminum. Application to the recycling of plutonium

International Nuclear Information System (INIS)

Gallay, J.

1968-01-01

A process for treating plutonium oxide calcined at high temperatures (1000 to 2000 deg. C) with a view to recovering the metal consists in the reduction of this oxide dissolved in a mixture of aluminium, sodium and calcium fluorides by aluminium at about 1180 deg. C. The first part of the report presents the results of reduction tests carried out on the uranium oxides UO 2 and U 3 O 8 ; these are in agreement with the thermodynamic calculations of the exchange reaction at equilibrium. The second part describes the application of this method to plutonium oxides. The Pu-Al alloy obtained (60 per cent Pu) is then recycled in an aqueous medium. (author) [fr

Inherent protection of plutonium by doping minor actinide in thermal neutron spectra

International Nuclear Information System (INIS)

Peryoga, Yoga; Sagara, Hiroshi; Saito, Masaki; Ezoubtchenko, Alexey

2005-01-01

The present study focuses on the exploration of the effect of minor actinide (MA) addition into uranium oxide fuels of different enrichment (5% 235 U and 20% 235 U) as ways of increasing fraction of even-mass-number plutonium isotopes. Among plutonium isotopes, 238 Pu, 240 Pu and 242 Pu have the characteristics of relatively high decay heat and spontaneous fission neutron rate that can improve proliferation-resistant properties of a plutonium composition. Two doping options were proposed, i.e. doping of all MA elements (Np, Am and Cm) and doping of only Np to observe their effect on plutonium proliferation-resistant properties. Pressurized water reactor geometry has been chosen for fuels irradiation environment where irradiation has been extended beyond critical to explore the subcritical system potential. Results indicate that a large amount of MA doping within subcritical operation highly improves the proliferation-resistant properties of the plutonium with high total plutonium production. Doping of 1% MA or Np into 5% 235 U enriched uranium fuel appears possible for critical operation of the current commercial light water reactor with reasonable improvement in the plutonium proliferation-resistant properties. (author)

Low-Level Plutonium Bioassay Measurements at the Lawrence Livermore National Laboratory

Energy Technology Data Exchange (ETDEWEB)

Hamilton, T; Brown, T; Hickman, D; Marchetti, A; Williams, R; Kehl, S

2007-06-18

Plutonium-239 ({sup 239}Pu) and plutonium-240 ({sup 240}Pu) are important alpha emitting radionuclides contained in radioactive debris from nuclear weapons testing. {sup 239}Pu and {sup 240}Pu are long-lived radionuclides with half-lives of 24,400 years and 6580 years, respectively. Concerns over human exposure to plutonium stem from knowledge about the persistence of plutonium isotopes in the environment and the high relative effectiveness of alpha-radiation to cause potential harm to cells once incorporated into the human body. In vitro bioassay tests have been developed to assess uptakes of plutonium based on measured urinary excretion patterns and modeled metabolic behaviors of the absorbed radionuclides. Systemic plutonium absorbed by the deep lung or from the gastrointestinal tract after ingestion is either excreted or distributed to other organs, primarily to the liver and skeleton, where it is retained for biological half-times of around 20 and 50 years, respectively. Dose assessment and atoll rehabilitation programs in the Marshall Islands have historically given special consideration to residual concentrations of plutonium in the environment even though the predicted dose from inhalation and/or ingestion of plutonium accounts for less than 5% of the annual effective dose from exposure to fallout contamination. Scientists from the Lawrence Livermore National Laboratory (LLNL) have developed a state-of-the-art bioassay test to assess urinary excretion rates of plutonium from Marshallese populations. This new heavy-isotope measurement system is based on Accelerator Mass Spectrometry (AMS). The AMS system at LLNL far exceeds the standard measurement requirements established under the latest United States Department of Energy (DOE) regulation, 10CFR 835, for occupational monitoring of plutonium, and offers several advantages over classical as well as competing new technologies for low-level detection and measurement of plutonium isotopes. The United States

Distribution of 238Pu and 239240Pu in aquatic macrophytes from a midwestern watershed

International Nuclear Information System (INIS)

Wayman, C.W.; Bartelt, G.E.; Alberts, J.J.

1977-01-01

Aquatic macrophytes were collected in the Great Miami River, Ohio, above and below Miamisburg and in the canal and ponds, near the Mound Laboratory, which contain sediments of a high activity (approximately 10 3 to 10 6 times) relative to the river sediments. Macrophytes collected in the river below Miamisburg have higher activities of 238 Pu than those collected from above the city. Macrophytes from the canal and ponds contain high specific activities of 238 Pu and 239 , 240 Pu with the exception of cattails grown in the ponds. Concentration factors are reported and discussed with reference to possible modes of plutonium accumulation and distribution within the plants

Initial synthesis of area 13 239Pu data and other statistical analyses

International Nuclear Information System (INIS)

Gilbert, R.O.; Eberhardt, L.L.

1976-02-01

An initial effort is made here to synthesize the 239-240 Pu data currently available from Area 13 (Project 57). Plutonium concentrations for soil, vegetation, small vertebrates, and various tissues in beef cattle (grazed on the Pu contaminated vegetation) are plotted on a single graph for visual comparison. Hypothetical 239-240 Pu concentrations for lungs, skeletal bone, and kidney of a Standard Man assumed to live in and obtain most of his food from the area are also plotted. These hypothetical values were obtained using results from the plutonium transport and dose estimation model of Martin and Bloom (1975)

GLASS FABRICATION AND PRODUCT CONSISTENCY TESTING OF LANTHANIDE BOROSHILICATE FRIT X COMPOSITION FOR PLUTONIUM DISPOSITION

Energy Technology Data Exchange (ETDEWEB)

Marra, J

2006-11-21

The Department of Energy Office of Environmental Management (DOE/EM) plans to conduct the Plutonium Disposition Project at the Savannah River Site (SRS) to disposition excess weapons-usable plutonium. A plutonium glass waste form is the preferred option for immobilization of the plutonium for subsequent disposition in a geologic repository. A reference glass composition (Lanthanide Borosilicate (LaBS) Frit B) was developed during the Plutonium Immobilization Program (PIP) to immobilize plutonium in the late 1990's. A limited amount of performance testing was performed on this baseline composition before efforts to further pursue Pu disposition via a glass waste form ceased. Recent FY05 studies have further investigated the LaBS Frit B formulation as well as development of a newer LaBS formulation denoted as LaBS Frit X. The objectives of this present task were to fabricate plutonium loaded LaBS Frit X glass and perform corrosion testing to provide near-term data that will increase confidence that LaBS glass product is suitable for disposal in the Yucca Mountain Repository. Specifically, testing was conducted in an effort to provide data to Yucca Mountain Project (YMP) personnel for use in performance assessment calculations. Plutonium containing LaBS glass with the Frit X composition with a 9.5 wt% PuO{sub 2} loading was prepared for testing. Glass was prepared to support Product Consistency Testing (PCT) at Savannah River National Laboratory (SRNL). The glass was thoroughly characterized using x-ray diffraction (XRD) and scanning electron microscopy coupled with energy dispersive spectroscopy (SEM/EDS) prior to performance testing. A series of PCTs were conducted at SRNL using quenched Pu Frit X glass with varying exposed surface areas. Effects of isothermal and can-in-canister heat treatments on the Pu Frit X glass were also investigated. Another series of PCTs were performed on these different heat-treated Pu Frit X glasses. Leachates from all these PCTs

242Pu as tracer for simultaneous determination of 237Np and 239,240Pu in environmental samples

DEFF Research Database (Denmark)

Chen, Q.J.; Dahlgaard, H.; Nielsen, S.P.

2002-01-01

A procedure has been developed using Pu-242 as tracer for simultaneous determination of Np-237 and Pu-239,Pu-240 in environmental samples. The validity of the method has been demonstrated by ICPMS and alpha-spectroscopy for up to 10 gram soil and sediment, seawater up to 200 litres. The paper...... from Np and Pu) R-before/R-after = 1.004 +/- 3.3% (S.D n = 20) and 1 litre seawater R-before/R-after = 1.019+/-1.9% (S.D., n = 12). Results from the intercomparison samples LAEA-135, LAEA-381 and from environmental samples are presented....... describes a suitable chemical procedure for Np and Pu including a quantitative pre-concentration of neptunium and plutonium, preparation of Np4+ and Pu4+, NP(NO3)(6)(2-) and Pu(NO3)(6)(2-), The ratio of Np-237/Pu-242 (or Np-237/Pu-239) before and after the procedure has been determined using 10 g soil (free...

Measurements Conducted on an Unknown Object Labeled Pu-239

International Nuclear Information System (INIS)

Hoteling, Nathan

2013-01-01

Measurements were carried out on 12 November 2013 to determine whether Pu-239 was present on an object discovered in a plastic bag with label ''Pu-239 6 uCi''. Following initial survey measurements to verify that the object was not leaking or contaminated, spectra were collected with a High Purity Germanium (HPGe) detector with object positioned in two different configurations. Analysis of the spectra did not yield any direct evidence of Pu-239. From the measured spectra, minimum detectable activity (MDA) was determined to be approximately 2 uCi for the gamma ray measurements. Although there was no direct evidence of Pu-239, a peak at 60 keV characteristic of Am-241 decay was observed. Since it is very likely that Am-241 would be present in aged plutonium samples, this was interpreted as indirect evidence for the presence of plutonium on the object. Analysis of this peak led to an estimated Pu-239 activity of 0.02-0.04 uCi, or <1x10 -6 grams.

Determination of {sup 240}Pu/{sup 239}Pu ratio and its significance in environmental studies

Energy Technology Data Exchange (ETDEWEB)

Muramatsu, Yasuyuki [National Inst. of Radiological Sciences, Chiba (Japan)

1999-03-01

Analytical procedures for the determination of Pu concentrations and its isotopic ratios in environmental samples were developed by using ICP-MS. Detection limit of Pu by ICP-MS was about 0.02 pg ml{sup -1} (0.05 mBq ml{sup -1} for {sup 239}Pu; 0.17 mBq ml{sup -1} for {sup 240}Pu) in the sample solution. Analytical results of {sup 239+240}Pu in IAEA standard reference materials indicated that the accuracy of this method was satisfactory. Data on the {sup 240}Pu/{sup 239}Pu atom ratios, which are rare in the literature, were also obtained for soil and sediment samples (including IAEA standard reference materials) from different areas such as Irish Sea, Mururoa Atoll, Marshall Islands, Chernobyl, Kyshtym, Nagasaki and some other places in Japan. The range of the {sup 240}Pu/{sup 239}Pu ratios was about 0.04-0.4, and the ratios are depending on the origin of the materials. Analytical results for the {sup 240}Pu/{sup 239}Pu atom ratios provide information about the source of the contamination and the transfer of plutonium in the environment. (author)

Plutonium diffusion in advanced fuels (U,Pu)(C,O) and (U,Pu)(C,N)

International Nuclear Information System (INIS)

Bradbury, M.H.; Matzke, H.

1983-01-01

The self-diffusion of 238 Pu was measured in an oxicarbide (U,Pu)(C,O) and a carbonitride (U,Pu) (C,N). The activation enthalpies were 447 and 347 kJ mol -1 , respectively. The carbonitrides were confirmed to fall into three classes: carbide-like compositions with less than 30% nitrogen in the metalloid lattice, nitride-like composition with more than 70% nitrogen and with reduced atomic mobilities, and carbonitrides with about 50% nitrogen showing an intermediate behavior. The oxicarbide showed diffusion coefficients slightly larger than those of pure carbides

Some of the properties of plutonium and the aluminium-plutonium alloy; Quelques proprietes du plutonium et de l'alliage aluminium-plutonium

Energy Technology Data Exchange (ETDEWEB)

Abramson, R; Boucher, R; Fabre, R; Monti, H [Commissariat a l' Energie Atomique, Saclay (France). Centre d' Etudes Nucleaires

1959-07-01

1- Study of the physical properties of plutonium. 1) Study of the allotropy of plutonium. a) Thermal analysis: the apparatus used and the measurement technique are briefly described. The transition point temperatures and the corresponding heats of transformation have been determined. Finally, the results of the particular study of certain transition points are given. b) Dilatometry. The dilatometric analysis of the phase changes of plutonium has been carried out by means of the Chevenard dilatometer with photographic recording. The testing conditions (heating and cooling speeds, isotherm plateaux) have been varied in order to determine accurately the characteristics of each transition, particularly the {delta} {yields} {gamma} transition on cooling. 2) Micrography of plutonium. For the accurate preparation of metallographic samples the electrolytic polishing must be rapid, which implies a mechanical polishing of excellent quality. Information is given on new attacking reagents which show the structure of the metal very clearly. 2- Study of aluminium-plutonium alloys. Comparative study of Al-Pu and Al-U alloys rich in aluminium. a) Thermal analysis. The liquids and fusion temperatures of the eutectic Al-XAl{sub 4}, have been accurately determined. From the measurement of the heats of fusion the exact composition of the eutectic alloy has been determined. b) Thermal treatments. The eutectic coalescence kinetics have been studied by a micrographic method and by following the evolution of hardness. The results obtained show that the phenomenon is more rapid in Al-Pu alloys than in Al-U alloys. c) Micrographic study of the transition XAl{sub 3} {yields} XAl{sub 4}. The peritectic reaction XAl{sub 3} + liq. {yields} XAl{sub 4} has been suppressed by quenching. The transformation of the XAl{sub 3} phase to the solid phase has been studied as well as the effect of small additions of silicon on the kinetics of this reaction. (author) [French] 1- Etude des proprietes

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

Science.gov (United States)

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.

Characterization of airborne plutonium-bearing particles from a nuclear fuel reprocessing plant

International Nuclear Information System (INIS)

Sanders, S.M. Jr.

1977-11-01

The elemental compositions, sizes, structures, and 239 Pu contents were determined for 299 plutonium-bearing particles isolated from airborne particles collected at various locations in the exhaust from a nuclear fuel reprocessing facility. These data were compared with data from natural aerosol particles. Most of the collected particles were composed of aggregates of crustal materials. Seven percent of the particles were organic and 3% were metallic, viz., iron, chromium, and nickel. High enrichment factors for titanium, manganese, chromium, nickel, zinc, and copper were evidence of the anthropic nature of some of the particles. The amount of plutonium in most particles was very small (less than one femtocurie of 239 Pu). Plutonium concentrations were determined by the fission track counting method. Only one particle contained sufficient plutonium for detection by electron microprobe analysis. This was a 1-μm-diameter particle containing 73% PuO 2 by weight (estimated to be 170 fCi of 239 Pu) in combination with Fe 2 O 3 and mica. The plutonium-bearing particles were generally larger than natural aerosols. The geometric mean diameter of those collected from the mechanical line exhaust point where plutonium is converted to the metal was larger than that of particles collected from the wet cabinet exhaust (13.7 μm vs. 4.6 μm). Particles from the mechanical line also contained more plutonium per particle than those from the wet cabinets

Chemical characterization of local and stratospheric plutonium in Ohio soils

International Nuclear Information System (INIS)

Muller, R.N.

1978-01-01

The chemical nature of plutonium derived from stratospheric fallout and industrial sources was studied in three agricultural soils. The majority of the soil plutonium was associated with a reductant-soluble, hydrous oxide phase that, under most conditions of terrestrial ecosystems, remains essentially immobile. The proportion of plutonium associated with organic matter (0.1N NaOH-extractable) varied among soils, and increased with decreasing particle size in the same soil. In a soil containing 238 Pu from a local fabrication facility and 239 , 240 Pu from stratospheric fallout, isotopic ratios between the NaOH-extractable and residual phases were essentially constant, indicating that, in these soils, plutonium from both sources behaves similarly. The distribution of soil plutonium with particle size appears to be most directly related to the mass of the soil particle

Determination of plutonium-241 half-life by mass spectrometric measurement

International Nuclear Information System (INIS)

Hiyama, Takashi; Wada, Yukio; Onishi, Koichi

1982-01-01

Much data for Pu-241 half-life have been reported, but these values range from 13.8 years to 15.1 years depending on investigators. In order to define the half-life of Pu-241, the half-life was calculated by analyzing the mass spectrometry data obtained in the author's laboratory over the past six years on Plutonium Isotopic Standard Reference Materials prepared at the National Bureau of Standards (NBS). The sample used for this work consisted of SRM-947 and SRM-948 prepared at NBS. Before mass spectrometric analysis, the plutonium aliquot was separated from its Am-241 daughter by anion exchange chromatography, since Am-241 is not distinguished from Pu-241 in the mass spectrometer. 241 Pu/ 239 Pu and 241 Pu/ 240 Pu ratios were calculated from the values of mass spectrometric measurement. From the relation of log N to time, the half-life of Pu-241 was determined, based on the slope using a least squares fit. The half-life of Pu-241 was estimated to be 14.29+-0.15 years. (Yoshitake, I.)

Chloride-catalyzed corrosion of plutonium in glovebox atmospheres

International Nuclear Information System (INIS)

Burgess, M.; Haschke, J.M.; Allen, T.H.; Morales, L.A.; Jarboe, D.M.; Puglisi, C.V.

1998-04-01

Characterization of glovebox atmospheres and the black reaction product formed on plutonium surfaces shows that the abnormally rapid corrosion of components in the fabrication line is consistent with a complex salt-catalyzed reaction involving gaseous hydrogen chloride (HCl) and water. Analytical data verify that chlorocarbon and HCl vapors are presented in stagnant glovebox atmospheres. Hydrogen chloride concentrations approach 7 ppm at some locations in the glovebox line. The black corrosion product is identified as plutonium monoxide monohydride (PuOH), a product formed by hydrolysis of plutonium in liquid water and salt solutions at room temperature. Plutonium trichloride (PuCl 3 ) produced by reaction of HCl at the metal surface is deliquescent and apparently forms a highly concentrated salt solution by absorbing moisture from the glovebox atmosphere. Rapid corrosion is attributed to the ensuing salt-catalyzed reaction between plutonium and water. Experimental results are discussed, possible involvement of hydrogen fluoride (HF) is examined, and methods of corrective action are presented in this report

Plutonium in Atlantic coastal estuaries in the southeastern United States

International Nuclear Information System (INIS)

Hayes, D.W.; LeRoy, J.H.; Cross, F.A.

1975-01-01

A survey was made to begin to provide baseline information on the Pu distribution of representative estuarine and coastal areas of the southeastern United States. Sediments and marsh grass (Spartina) were collected and analyzed from three locations within a tidal marsh. In three estuaries (Savannah, Neuse, and Newport), the suspended particulate matter (1 μm and greater) was filtered from waters with different salinities, and the plutonium content of the particulates determined. The Savannah River estuary, in addition to fallout Pu, has received up to 0.3 Ci of Pu from the Savannah River Plant (SRP) of the U. S. Energy Research and Development Administration. The SRP plutonium has a variable isotopic composition that can influence Pu isotopic ratios in the estuarine system. The other estuaries do not have nuclear installations upstream. Data are included on the content of 238 Pu, 239 Pu, and 240 Pu in sediments and marsh grass of the Savannah River estuary

Routes of plutonium uptake and their relation to biomagnification in starfish

International Nuclear Information System (INIS)

Guary, J.-C.; Fowler, S.W.; Beasley, T.M.

1982-01-01

The distribution of 239+240 Pu and 238 Pu in environmental samples of starfish tissues is identical to the tissue distribution observed in experimental animals following uptake of plutonium directly from water. Plutonium in sea water has a strong affinity for the mucus-rich epidermal layer of starfish which contributes substantially to the relatively high levels of this transuranium nuclide measured in these invertebrates. Transfer of plutonium to starfish via food also occurs; however, the resultant tissue distribution is not consistent with that found in the natural environment where plutonium is available from both contaminated food and water. These data suggest that food chain biomagnification of plutonium by starfish does not occur in nature as has been previously hypothesized. (author)

The isotopic signature of fallout plutonium in the North Pacific

International Nuclear Information System (INIS)

Buesseler, K.O.

1997-01-01

Plutonium analyses of a dated coral record from the French Frigate Shoals in the central North Pacific indicate that there are two major sources of Pu in this basin: close-in (tropospheric) fallout from nuclear weapons testing at the Pacific Proving Grounds in the Marshall Islands in the 1950s and global (stratospheric) fallout which peaked in 1962. Furthermore, the 240 Pu/ 239 Pu atom ratio of fallout from the Pacific Proving Grounds is characteristically higher (0.24) than that of global fallout Pu (0.18-0.19). Seawater and sediment samples from the North Pacific exhibit a wide range of 240 Pu/ 239 Pu values (0.19-0.34), with a trend towards higher ratios in the subsurface waters and sediment. Deep water 240 Pu/ 239 Pu ratios are higher in the vicinity of the Marshall Islands relative to stations further from this close-in fallout source. These preliminary data suggest that fallout Pu from the Pacific Proving Grounds is more rapidly removed from the surface waters than is global fallout Pu. Plutonium geochemistry appears to be related to the physical/chemical form of Pu-bearing particles generated by different fallout sources. (author)

Use of combined alpha-spectrometry and fission track analysis for the determination of 240Pu/239Pu ratios in human tissue

International Nuclear Information System (INIS)

Love, S.F.; Filby, R.H.; Glover, S.E.; Stuit, D.B.; Kathren, R.L.

1998-01-01

Plutonium and other actinides were determined in human autopsy tissues of occupationally exposed workers who were registrants of the United States Transuranium and Uranium Registries (USTUR). In this study, Pu was purified and isolated from Am, U and Th, after drying and wet-ashing of the tissues, and the addition of 238 Pu as a radiotracer. After electrodeposition onto vanadium planchets, the 239+240 Pu activity was determined by alpha-spectrometry. A fission track method was developed to determine 239 Pu in the presence of 238 Pu and 240 Pu, using Lexan TM polycarbonate detectors. Combining the two techniques allowed the determination of the 240 Pu/ 239 Pu activity and atom ratios. Data from selected USTUR cases are presented. (author)

Aqueous recovery of plutonium from pyrochemical processing residues

International Nuclear Information System (INIS)

Gray, L.W.; Gray, J.H.

1984-01-01

Pyrochemical processes provide rapid methods to reclaim plutonium from scrap residues. Frequently, however, these processes yield an impure plutonium product and waste residues that are contaminated with actinides and are therefore nondiscardable. The Savannah River Laboratory and Plant and the Rocky Flats Plant are jointly developing new processes using both pyrochemistry and aqueous chemistry to generate pure product and discardable waste. An example of residue being treated is that from the molten salt extraction (MSE), a mixture of NaCl, KCl, MgCl 2 , PuCl 3 , AmCl 3 , PuO 2 , and Pu 0 . This mixture is scrubbed with molten aluminum containing a small amount of magnesium to produce a nonhomogeneous Al-Pu-Am-Mg alloy. This process, which rejects most of the NaCl-KCl-MgCl 2 salts, results in a product easily dissolved in 6M HNO 3 -0.1M HF. Any residual chloride in the product is removed by precipitation with Hg(I) followed by centrifuging. Plutonium and americium are then separated by the standard Purex process. The americium, initially diverted to the solvent extraction waste stream, can either be recovered or sent to waste

Plutonium concentrations in airborne soil at Rocky Flats and Hanford determined during resuspension experiments

Energy Technology Data Exchange (ETDEWEB)

Sehmel, G.A.

1978-01-01

Plutonium resuspension results are summarized for experiments conducted by the author at Rocky Flats, onsite on the Hanford reservation, and for winds blowing from offsite onto the Hanford reservation near the Prosser barricade boundary. In each case, plutonium resuspension was shown by increased airborne plutonium concentrations as a function of either wind speed or as compared to fallout levels. All measured airborne concentrations were far below maximum permissible concentrations (MPC). Both plutonium and cesium concentrations on airborne soil were normalized by the quantity of airborne soil sampled. Airborne radionuclide concentrations in ..mu..Ci/g were related to published values for radionuclide concentrations on surface soils. For this ratio of radionuclide concentration per gram on airborne soil divided by that for ground surface soil, there are eight orders of magnitude uncertainty from 10/sup -4/ to 10/sup 4/. This uncertainty in the equality between plutonium concentrations per gram on airborne and surface soils is caused by only a fraction of the collected airborne soil being transported from offsite rather than all being resuspended from each study site and also by the great variabilities in surface contamination. Horizontal plutonium fluxes on airborne nonrespirable soils at all three sites were bracketed within the same four orders of magnitude from 10/sup -7/ to 10/sup -3/ ..mu..Ci/(m/sup 2/ day) for /sup 239/Pu and 10/sup -8/ to 10/sup -5/ ..mu..Ci/(m/sup 2/ day) for /sup 238/Pu. Airborne respirable /sup 239/Pu concentrations increased with wind speed for a southwest wind direction coming from offsite near the Hanford reservation Prosser barricade. Airborne plutonium fluxes on nonrespirable particles had isotopic ratios, /sup 240/Pu//sup 239/ /sup 240/Pu, similar to weapons grade plutonium rather than fallout plutonium.

Controlled-potential coulometric determination of plutonium with a hydrochloric acid-sulfamic acid electrolyte and phosphate complexing

International Nuclear Information System (INIS)

Jackson, D.D.; Hollen, R.M.; Roensch, F.R.; Rein, J.E.

1981-01-01

Total plutonium is selectively determined by a controlled-potential coulometric method in which plutonium is reduced to Pu(III) at 0.25 V (vs. SCE) in a 5.5 M hydrochloric acid-0.015 M sulfamic acid electrolyte, diverse ions are oxidized at 0.57 V, phosphate is added to reduce the Pu(III)-Pu(IV) potential, and Pu(III) is oxidized to Pu(IV) at 0.68 V. None of more than 50 metal ions present in nuclear fuel-cycle material interferes. Many anions are without effect and most interfering ones are removed by preliminary fuming with perchloric acid. The apparatus described consists mainly of commercial components. The relative standard deviation is < 0.1% at the 5-mg plutonium level

Contamination of living environment and human organism with plutonium

International Nuclear Information System (INIS)

Benes, J.

1981-01-01

The applicability of 239 Pu in nuclear power is discussed. The radiotoxic properties of plutonium, its tissue distribution and the effects of internal and external contamination are described. The contamination of the atmosphere, water, and soil with plutonium isotopes is discussed. Dosimetry is described of plutonium in the living and working environments as is plutonium determination in the human organism. (H.S.)

Savannah River Laboratory monthly report: 238Pu fuel form processes

International Nuclear Information System (INIS)

1976-01-01

Progress in the Savannah River 238 Pu Fuel Form Program is discussed. Goals of the Savannah River Laboratory (SRL) program are to provide technical support for the transfer of the 238 Pu fuel form fabrication operations from Mound Laboratory to new facilities being built at the Savannah River Plant (SRP), to provide the technical basis for 238 Pu scrap recovery at SRP, and to assist in sustaining plant operations. During the period it was found that the density of hot-pressed 238 PuO 2 pellets decreased as the particle size of ball-milled powder decreased;the surface area of calcined 238 PuO 2 powder increased with increasing precipitation temperature and may be related to the variation in ball-milling response observed among different H Area B-Line batches; calcined PuO 2 produced by Pu(III) reverse-strike precipitation was directly fabricated into a pellet without ball milling, slugging, or sharding. The pellet had good appearance with acceptable density and dimensional stability, and heat transfer measurements and calculations showed that the use of hollow aluminum sleeves in the plutonium fuel fabrication (PuFF) storage vault reduced the temperature of shipping cans to 170 0 C and will reduce the temperature at the center of pure plutonium oxide (PPO) spheres to 580 0 C

Plutonium and minor actinides recycling in PWRs with new APA concepts

International Nuclear Information System (INIS)

Golfier, H.; Rohart, M.; Aniel, S.; Bergeron, J.; Deffain, J.P.

2001-01-01

In the frame of the studies required by the French law of 1991, CEA have launched a wide range of assessments on waste management for different reactors (PWR, FBR). Considerable R and D work has already been performed in order to improve the use of Plutonium (Pu) in PWRs. In this context, the Advanced Plutonium Assembly (APA) aims to improve the use of Plutonium (Pu) in PWRs while minimizing Minor Actinides (MA) production, with only slight modifications of the core design. From a neutronic point of view, the overall studied cases lead to the stabilization of the Pu inventory with approximately 30% of the park refueled with APA assemblies in full APA cores. Multi-recycling could satisfy the stabilization of Pu+ (Am+Cm) inventory by the implementation of approximately 40% APA reactors in a conventional PWRs park. After 7 or 8 recycles, the equilibrium is reached. The Pu inventory in the fuel cycle ranges from 210 tons to 270 tons for Pu multi-recycling, and from 240 tons to 290 tons for Pu+(Am+Cm) multi-recycling. The saving in Natural Uranium and Separative Work Units (SWU) due to the use of APA reactors would be between 30% and 15% in comparison with the UO 2 open cycle. This paper presents a selection of the main preliminary Pu recycling results of the joint study program COGEMA-CEA. (author)

Performance of cladding on MOX fuel with low 240Pu/239Pu ratio

International Nuclear Information System (INIS)

McCoy, K.; Blanpain, P.; Morris, R.

2015-01-01

The U.S. Department of Energy has decided to dispose of a portion of its surplus plutonium by reconstituting it into mixed oxide (MOX) fuel and irradiating it in commercial power reactors. As part of fuel qualification, four lead assemblies were manufactured and irradiated to a maximum fuel rod average burnup of 47.3 MWd/kg heavy metal. This was the world's first commercial irradiation of MOX fuel with a 240 Pu/ 239 Pu ratio less than 0.10. Five fuel rods with varying burnups and plutonium contents were selected from one of the assemblies and shipped to Oak Ridge National Laboratory for hot cell examination. This paper discusses the results of those examinations with emphasis on cladding performance. Exams relevant to the cladding included visual and eddy current exams, profilometry, microscopy, hydrogen analysis, gallium analysis, and mechanical testing. There was no discernible effect of the type of MOX fuel on the performance of the cladding. (authors)

Isotope ratios of 240Pu/239Pu in soil samples from different areas

International Nuclear Information System (INIS)

Muramatsu, Yasuyuki; Yoshida, Satoshi; Yamazaki, Shinnosuke

2003-01-01

Plutonium concentrations and 240 Pu/ 239 Pu atom ratios in soil samples from Japan and other areas in the world (including IAEA standard reference materials) were determined by ICP-MS. The range of 240 Pu/ 239 Pu atom ratios observed in 21 Japanese soil samples was 0.155 - 0.194 and the average was 0.180 ± 0.011, which is comparable to the global fallout value. A low ratio of about 0.05, which is derived from Pu-bomb, was found in samples from Nishiyama (Nagasaki) and Mururoa Atoll (IAEA-368), while a high ratio of about 0.31 was found in a sample from Bikini Atoll (Marshall Islands). The ratio for Irish Sea sediment (IAEA-135) was 0.21, which was higher than the global fallout value, suggesting the influence by the contamination from the Sellafield facility. The 240 Pu/ 239 Pu atom ratios in soils from the Chernobyl area were determined, and the ratio was found to be very high (about 0.4), indicating the high burn-up grade of the reactor fuel. These results show that the 240 Pu/ 239 Pu ratio can be used as a finger print to identify the source of the contamination. (author)

Long time contamination from plutonium

Energy Technology Data Exchange (ETDEWEB)

Fueloep, M; Patzeltova, N; Ragan, P [Inst. of Preventive and Clinical Medicine, Bratislava (Slovakia); Matel, L [Comenius Univ., Bratislava (Slovakia). Department of Nuclear Chemistry

1996-12-31

Plutonium isotopes in the organism of the patient (who had participated in the liquidation works after the Chernobyl accident; for three month he had stayed in the epicenter, where he acted as a chauffeur driving a radioactive material to the place of destination) from urine were determined. For determination of the concentration of Pu-239, Pu-240 in urine a modified radiochemical method was used. After mineralization the sample was separated as an anion-nitrate complex with contact by the anion form of the resin in the column. The resin was washed by 8 M HNO{sub 3}, the 8 M HCl with 0.3 M HNO{sub 3} for removing the other radionuclides. The solution 0.36 M HCl with 0.01 M HF was used for the elution of plutonium. Using the lanthanum fluoride technique the sample was filtrated through a membrane filter. The plutonium was detected in the dry sample. The Pu-239 tracer was used for the evaluation of the plutonium separation efficiency. The alpha spectrometric measurements were carried out with a large area silicon detector. The samples were measured and evaluated in the energy region 4.98-5.18 MeV. The detection limit of alpha spectrometry measurements has been 0.01 Bq dm{sup -3}. The concentration of plutonium in the 24-hour urine was determined three times in the quarter year intervals. The results are: 54 mBq, 63.2 mBq, 53 mBq, with average 56,7 mBq. From the results of the analyses of plutonium depositions calculated according to ICRP 54 the intake of this radionuclide for the patient was 56.7 kBq. To estimate a committed effective dose (50 years) from the intake of plutonium was used a conversion factor 6.8.10{sup -5} Sv.Bq{sup -1} (class W). So the expressed committed effective dose received from the plutonium intake is 3.8 Sv. This number is relatively high and all the effective dose will be higher, because the patient was exposed to the other radionuclides too. (Abstract Truncated)

Synthesis of complex plutonium oxides with alkaline-earth metals

International Nuclear Information System (INIS)

Suzuki, Yasufumi; Nakajima, Kunihisa; Iwai, Takashi; Ohmichi, Toshihiko; Yamawaki, Michio.

1995-03-01

Complex plutonium(IV) oxides with strontium and barium, SuPuO 3 and BaPuO 3 , were synthesized and their crystal structure was analyzed. Compacted mixture of plutonium dioxide powder and the carbonate of strontium or barium was heated in a stream of argon gas using a cell with a small orifice. The products obtained were found to be composed of a nearly single phase showing the structure of orthorhombic slightly distorted from cubic. (author)

Redox reactions of Pu(IV) and Pu(III) in the presence of acetohydroxamic acid in HNO(3) solutions.

Science.gov (United States)

Tkac, Peter; Precek, Martin; Paulenova, Alena

2009-12-21

The reduction of Pu(IV) in the presence of acetohydroxamic acid (HAHA) was monitored by vis-NIR spectroscopy. All experiments were performed under low HAHA/Pu(IV) ratios, where only the Pu(IV)-monoacetohydroxamate complex and Pu uncomplexed with HAHA were present in relevant concentrations. Time dependent concentrations of all absorbing species were resolved using molar extinction coefficients for Pu(IV), Pu(III), and the Pu(AHA)(3+) complex by deconvolution of spectra. From fitting of the experimental data by rate equations integrated by a numeric method three reactions were proposed to describe a mechanism responsible for the reduction and oxidation of plutonium in the presence of HAHA and HNO(3). Decomposition of Pu(AHA)(3+) follows a second order reaction mechanism with respect to its own concentration and leads to the formation of Pu(III). At low HAHA concentrations, a two-electron reduction of uncomplexed Pu(IV) with HAHA also occurs. Formed Pu(III) is unstable and slowly reoxidizes back to Pu(IV), which, at the point when all HAHA is decomposed, can be catalyzed by the presence of nitrous acid.

Natural Pu-traces within the continental crust

International Nuclear Information System (INIS)

Ganz, M.; Barth, H.; Fuest, M.; Molzahn, D.; Brandt, R.

1991-01-01

Pu-traces are observed in the environmental all over the world, 'man made'-Pu as well as 'natural' Pu ( 239 Pu). 239 Pu occurs within a range of about 10 -12 g Pu/g sample in pitchblende. In the FRG, the deep-drilling project 'KTB, Kontinentales Tiefbohrprogramm', was started with the aim to obtain a very deep hole (14 km). We wanted to establish upper concentration limits for plutonium in samples from KTB. For a first investigation, we obtained a 400 g sample of granite from a pre-drill of KTB. Its Pu-concentration was ≤ (4.5 ± 2.5)x10 -16 g 239 Pu/g sample. To compare this result to the Pu-content in geological brines, we obtained a sample from a borehole at the Salton Sea Geothermal field (Southeastern California). In this sample we found an upper concentration limit of (2.1 ± 1.0)x10 -16 g 239 Pu/g sample. (orig.)

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

Energy Technology Data Exchange (ETDEWEB)

Nielsen, Christopher E.; Wilson, Dulaney A.; Brooks, Antone L.; McCord, Stacey; Dagle, Gerald E.; James, Anthony C.; Tolmachev, Sergei Y.; Thrall, Brian D.; Morgan, William F.

2012-11-01

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. Fibrotic 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.

Disposal criticality analysis for immobilized plutonium: Internal configurations

International Nuclear Information System (INIS)

Gottlieb, P.; Massari, J.R.; Cloke, P.L.

1998-03-01

The analysis for immobilized Pu follows the disposal criticality analysis methodology. In this study the focus is on determining the range of chemical compositions of the configurations which can occur following the aqueous degradation processes, particularly with respect to the concentrations of uranium, plutonium, and the principal neutron absorber, gadolinium. The principal analysis tool is a mass balance program that computes the amounts of plutonium, uranium, gadolinium, and chromium in solution as a function of time with inputs from a range of possible waste form dissolution rates, stainless steel corrosion rates, and compound solubilities for the neutronically significant elements. For the waste forms and degradation modes considered here, it is possible to preclude the possibility of criticality by maintaining a plutonium loading limit. Since the presence of hafnium is shown to increase this loading limit, the defense-in-depth policy would suggest the maximization of the amount of Hf as a backup criticality control material. At the end of 1997, after this study was completed, the ceramic waste form was downselected and a new formulation was developed, with the amount of Hf increased to the point where internal criticality may no longer be possible. In addition, recent calculations indicate that GdPO 4 is insoluble over a much broader range of pH than is Gd 2 O 3 , so that its use as the Gd carrier in the waste form would provide an extra margin of defense-in-depth

Weapons-grade plutonium dispositioning. Volume 4

International Nuclear Information System (INIS)

Sterbentz, J.W.; Olsen, C.S.; Sinha, U.P.

1993-06-01

This study is in response to a request by the Reactor Panel Subcommittee of the National Academy of Sciences (NAS) Committee on International Security and Arms Control (CISAC) to evaluate the feasibility of using plutonium fuels (without uranium) for disposal in existing conventional or advanced light water reactor (LWR) designs and in low temperature/pressure LWR designs that might be developed for plutonium disposal. Three plutonium-based fuel forms (oxides, aluminum metallics, and carbides) are evaluated for neutronic performance, fabrication technology, and material and compatibility issues. For the carbides, only the fabrication technologies are addressed. Viable plutonium oxide fuels for conventional or advanced LWRs include plutonium-zirconium-calcium oxide (PuO 2 -ZrO 2 -CaO) with the addition of thorium oxide (ThO 2 ) or a burnable poison such as erbium oxide (Er 2 O 3 ) or europium oxide (Eu 2 O 3 ) to achieve acceptable neutronic performance. Thorium will breed fissile uranium that may be unacceptable from a proliferation standpoint. Fabrication of uranium and mixed uranium-plutonium oxide fuels is well established; however, fabrication of plutonium-based oxide fuels will require further development. Viable aluminum-plutonium metallic fuels for a low temperature/pressure LWR include plutonium aluminide in an aluminum matrix (PuAl 4 -Al) with the addition of a burnable poison such as erbium (Er) or europium (Eu). Fabrication of low-enriched plutonium in aluminum-plutonium metallic fuel rods was initially established 30 years ago and will require development to recapture and adapt the technology to meet current environmental and safety regulations. Fabrication of high-enriched uranium plate fuel by the picture-frame process is a well established process, but the use of plutonium would require the process to be upgraded in the United States to conform with current regulations and minimize the waste streams

Impurity diffusion of cobalt in plutonium

International Nuclear Information System (INIS)

Charissoux, Christian; Calais, Daniel.

1975-01-01

The sectioning method for investigation of the impurity diffusion of 60 Co in the fcc and bcc phases of plutonium gives the following results: 344-426 deg C: D=1.2x10 -2 exp(-12700/RT)cm 2 /s in delta Pu(fcc); 484-621 deg C: D=1.4x10 -3 exp(-9900/RT)cm 2 /s in epsilon Pu(bcc). Cobalt is a fast diffuser in plutonium; the diffusion coefficient being unaffected by phase changes delta'→delta; delta'→epsilon, the diffusion mechanism is probably dissociative in both phases, the solute becoming interstitial by: solute (substitution) reversible solute (interstitial) + vacancy [fr

Plutonium-238 alpha-decay damage study of the ceramic waste form

International Nuclear Information System (INIS)

Frank, S. M.; Barber, T. L.; Cummings, D.G.; DiSanto, T.; Esh, D.W.; Giglio, J. J.; Goff, K. M.; Johnson, S.G.; Kennedy, J.R.; Jue, J-F; Noy, M.; O'Holleran, T.P.; Sinkler, W.

2006-01-01

An accelerated alpha-decay damage study of a glass-bonded sodalite ceramic waste form has recently been completed. The purpose of this study was to investigate the physical and chemical durability of the waste form after significant exposure to alpha decay. This accelerated alpha-decay study was performed by doping the ceramic waste form with 238 Pu which has a much greater specific activity than 239 Pu that is normally present in the waste form. The alpha-decay dose at the end of the four year study was approximately 1 x 10 18 alpha-decays/gram of material. An equivalent time period for a similar dose of 239 Pu would require approximately 1100 years. After four years of exposure to 238 Pu alpha decay, the investigation observed little change to the physical or chemical durability of the ceramic waste form (CWF). Specifically, the 238 Pu-loaded CWF maintained it's physical integrity, namely that the density remained constant and no cracking or phase de-bonding was observed. The materials chemical durability and phase stability also did not change significantly over the duration of the study. The only significant measured change was an increase of the unit-cell lattice parameters of the plutonium oxide and sodalite phases of the material and an increase in the release of salt components and plutonium of the waste form during leaching tests, but, as mentioned, these did not lead to any overall loss of waste form durability. The principal findings from this study are: (1) 238 Pu-loaded CWF is similar in microstructure and phase composition to referenced waste form. (2) Pu was observed primarily as oxide comprised of aggregates of nano crystals with aggregates ranging in size from submicron to twenty microns in diameter. (3) Pu phases were primarily found in the intergranular glassy regions. (4) PuO phase shows expected unit cell volume expansion due to alpha decay damage of approximately 0.7%, and the sodalite phase unit cell volume has expanded slightly by 0.3% again

Adsorption-Desorption Characteristics of Plutonium and Americium with Sediment Particles in the Estuarine Environment

International Nuclear Information System (INIS)

Murray, C.N.; Fukai, R.

1976-01-01

The particle formation of plutonium and americium, their adsorption onto fresh water sediments and the desorption from the sediments in sea water were studied in the Laboratory under simulated river-estuary conditions, using γ-emitting plutonium-237 and americium-241. The results of the experiments show that the particle formation of plutonium depends on its valence states, on pH and on the salinity of the medium. For river water at pH4, some 25%, 20% and 30% of the added 237 Pu was in particulate form, larger than 0.45pm, for Pu (III), Pu (IV) and Pu (VI), respectively, while 65%, 90% and 50% of the respective valence states was associated with particles at pH 8. In sea water the general pattern remains similar, although Pu (VI) is more soluble in sea water owing to higher ligand concentrations for carbonate and bicarbonate complexes. The pH-dependency of particle formation of Am (III) is more steep than that of plutonium and seems to be influenced by colloidal substances occurring in the experimental media. The adsorption-desorption characteristics of plutonium and americium with the sediment in river water as well as sea water reflect the characteristics of their particle formation, being dependent upon such properties as valence states, the pH and salinity of the medium. A sewage effluent added to the media has small but measurable effects on the adsorption-desorption processes of plutonium. (author)

Characterization of (241)Pu occurrence, distribution, and bioaccumulation in seabirds from northern Eurasia.

Science.gov (United States)

Strumińska-Parulska, Dagmara I; Skwarzec, Bogdan

2015-05-01

The paper presents unique data of plutonium (241)Pu study in seabirds from northern Eurasia, permanently or temporally living at the southern Baltic Sea coast. Together, ten marine birds species were examined, as follows: three species that permanently reside at the southern Baltic, four species of wintering birds, and three species of migrating birds; 366 samples were analyzed. The obtained results indicated plutonium was non-uniformly distributed in organs and tissues of analyzed seabirds. The highest (241)Pu content was found in the digestion organs and feathers, the lowest in muscles. Also, the internal radiation doses from (241)Pu were evaluated.

Routine radiochemical method for the determination of 90Sr, 238Pu, 239+240Pu, 241Am and 244Cm in environmental samples

International Nuclear Information System (INIS)

Ageyev, V.A.; Sajeniouk, A.D.

2005-01-01

Routine analytical procedures have been developed for the reliable simultaneous determination of 90 Sr, 238 Pu, 239+240 Pu, 241 Am and 242-244 Cm, Chernobyl derived radioisotopes and fallout after nuclear weapon tests in a wide range of environmental samples: soil (100-200 g), sediments, aerosols, water and vegetation. This procedure has been applied to thousands of soil and sediment samples and hundreds of biological and water samples taken in the exclusive zone of Chernobyl NPP and different regions of Ukraine from 1989 to the present. After the sample has been properly prepared and isotopic tracers added, plutonium, americium and curium are precipitated with calcium oxalate and then lanthanum fluoride. Plutonium is separated from americium and curium by anion-exchange. Americium and curium are separated from rare earths by cation-exchange with gradient elute α-hydroxy-iso-butyric acid. During projects by AQCS IAEA 'Evaluation of Methods for 90 Sr in a Mineral Matrix' and 'Proficiency Test for 239 Pu, 241 Pu and 241 Am Measurement in a Mineral Matrix' accuracy and precision for 90 Sr, 239 Pu and 241 Am by present procedure was evaluated. Advantages, difficulties and limitations of the method are discussed. (author)

Chemical speciation of Pu in natural waters

International Nuclear Information System (INIS)

Nelson, D.M.; Larsen, R.P.; Penrose, W.R.

1983-01-01

The behavior of plutonium in natural waters is determined to a major degree by the chemical forms which are present. We have characterized the ambient Pu in a number of surface waters with regard to its oxidation state and association with natural colloidal organic carbon compounds using a combination of field measurements and laboratory experiments. Both of these factors are shown to have a profound effect on the adsorption of Pu to natural sediments, since both complexation with organic matter and oxidation compete with adsorption. The concentration of organic carbon in the water is the key variable influencing both oxidation state and organic binding. The adsorption process conforms to the laws applicable to a reversible equilibrium with values of the distribution coefficient, K/sub D/, measured in laboratory experiments being similar to those observed for ambient Pu. Experiments using natural waters and sediments in which the Pu concentration was varied show the forms present at typical ambient concentrations (10 -17 - 10 -14 M) are the same as those found at concentrations up to 10 -7 M. Moreover, the affinity for sediments did not change with concentration indicating the binding sites for Pu had not become saturated. Thus, the behavior observed for Pu at ultratrace concentrations should remain unchanged throughout this concentration range. The studies in this report all deal with Pu in exchangeable (and hence source independent) forms and should therefore reflect the behavior toward which the plutonium from any source will tend with time. 13 references, 7 figures, 10 tables

Aqueous Chloride Operations Overview: Plutonium and Americium Purification/Recovery

Energy Technology Data Exchange (ETDEWEB)

Kimball, David Bryan [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Skidmore, Bradley Evan [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

2016-06-22

Acqueous Chloride mission is to recover plutonium and americium from pyrochemical residues (undesirable form for utilization and storage) and generate plutonium oxide and americium oxide. Plutonium oxide is recycled into Pu metal production flowsheet. It is suitable for storage. Americium oxide is a valuable product, sold through the DOE-OS isotope sales program.

Activities concentration of 239+240Pu in sediment in Sabah and Sarawak coastal area

International Nuclear Information System (INIS)

Jalal Sharib; Zaharudin Ahmad; Yii Mei Wo; Ahmad Sanadi Abu Bakar; Norfaizal Mohamed; Kamarozaman Ishak; Zulkifli Daud

2008-08-01

The determination of plutonium, 239+240 Pu activity concentration and their distributions along the coastal area of the Sabah and Sarawak have been performed using alpha spectrometry counting system. The sampling coastal sediment for this study was carried out in July 2004 as part of the Marine Radioactivity Database Development Project for Malaysia. This results show that the distribution of Plutonium, 239+240 Pu radionuclides in coastal sediment is consistent, their activities are depending on the sampling locations. Generally, the 239+240 Pu activities measured in Sabah and Sarawak coastal sediment are in the range of BDL - 1.83 Bq/kg and 0.11 - 0.841 Bq/kg dry weights, respectively. The sampling stations, Persisiran Lubok Sabanan, SB 15 and Sungai Similajau, SR 13 showed the highest plutonium, 239+240 Pu radionuclides isotopes activity in Sabah and Sarawak. Meanwhile, these two stations shows higher activity compare to West Coast of Peninsular of Malaysia station for the Marine Radioactivity Database Development Project for Malaysia. (Author)

Magnetism, superconductivity and Fermi surfaces of plutonium compounds

International Nuclear Information System (INIS)

Haga, Y.; Aoki, D.; Yamagami, H.; Matsuda, T.D.; Nakajima, K.; Arai, Y.; Homma, Y.; Shiokawa, Y.; Yamamoto, E.; Nakamura, A.; Onuki, Y.

2007-01-01

Single crystals of plutonium compounds PuRhGa 5 and PuIn 3 are successfully grown. For PuRhGa 5 , anisotropy of the superconducting upper critical field was found and analyzed by the anisotropic mass model, consistent with quasi-two-dimensional electronic states predicted by band calculations. On the other hand, the de Haas-van Alphen oscillation was observed in PuIn 3 . By comparing with the band calculations, it is concluded that 5f electrons are itinerant in PuIn 3

Potential of thorium-based fuel cycle for PWR core to reduce plutonium and long-term toxicity

Energy Technology Data Exchange (ETDEWEB)

Joo, Hyung Kook; Kim, Taek Kyum; Kim, Young Jin [Korea Atomic Energy Research Institute, Taejon (Korea)

1999-01-01

The cross section libraries and calculation methods of the participants were inter-compared through the first stage benchmark calculation. The multiplication factor of unit cell benchmark are in good agreement, but there is significant discrepancies of 2.3 to 3.5 %k at BOC and at EOC between the calculated infinite multiplication factors of each participants for the assembly benchmark. Our results with HELIOS show a reasonable agreement with the others except the MTC value at EOC. To verify the potential of the thorium-based fuel to consume the plutonium and to reduce the radioactivity from the spent fuel, the conceptual core with ThO{sub 2}-PuO{sub 2} or MOX fuel were constructed. The composition and quantity of plutonium isotopes and the radioactivity level of spent fuel for conceptual cores were analyzed, and the neutronic characteristics of conceptual cores were also calculated. The nuclear characteristics for ThO{sub 2}-PuO{sub 2} thorium fueled core was similar to MOX fueled core, mainly due to the same seed fuel material, plutonium. For the capability of plutonium consumption, ThO{sub 2}-PuO{sub 2} thorium fuel can consume plutonium 2.1-2.4 times MOX fuel. The fraction of fissile plutonium in the spent ThO{sub 2}-PuO{sub 2} thorium fuel is more favorable in view of plutonium consumption and non-proliferation than MOX fuel. The radioactivity of spent ThO{sub 2}-PuO{sub 2} thorium and MOX fuel batches were calculated. Since plutonium isotopes are dominant for the long-term radioactivity, ThO{sub 2}-PuO{sub 2} thorium has almost the same level of radioactivity as in MOX fuel for a long-term perspective. (author). 22 figs., 11 tabs.

Design of the Laboratory-Scale Plutonium Oxide Processing Unit in the Radiochemical Processing Laboratory

Energy Technology Data Exchange (ETDEWEB)

Lumetta, Gregg J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Meier, David E. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Tingey, Joel M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Casella, Amanda J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Delegard, Calvin H. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Edwards, Matthew K. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Orton, Robert D. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Rapko, Brian M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Smart, John E. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

2015-05-01

This report describes a design for a laboratory-scale capability to produce plutonium oxide (PuO₂) for use in identifying and validating nuclear forensics signatures associated with plutonium production, as well as for use as exercise and reference materials. This capability will be located in the Radiochemical Processing Laboratory at the Pacific Northwest National Laboratory. The key unit operations are described, including PuO₂ dissolution, purification of the Pu by ion exchange, precipitation, and re-conversion to PuO₂ by calcination.

Characterization of plutonium-bearing wastes by chemical analysis and analytical electron microscopy

International Nuclear Information System (INIS)

Behrens, R.G.; Buck, E.C.; Dietz, N.L.; Bates, J.K.; Van Deventer, E.; Chaiko, D.J.

1995-09-01

This report summarizes the results of characterization studies of plutonium-bearing wastes produced at the US Department of Energy weapons production facilities. Several different solid wastes were characterized, including incinerator ash and ash heels from Rocky Flats Plant and Los Alamos National Laboratory; sand, stag, and crucible waste from Hanford; and LECO crucibles from the Savannah River Site. These materials were characterized by chemical analysis and analytical electron microscopy. The results showed the presence of discrete PuO 2 PuO 2-x , and Pu 4 O 7 phases, of about 1μm or less in size, in all of the samples examined. In addition, a number of amorphous phases were present that contained plutonium. In all the ash and ash heel samples examined, plutonium phases were found that were completely surrounded by silicate matrices. Consequently, to achieve optimum plutonium recovery in any chemical extraction process, extraction would have to be coupled with ultrafine grinding to average particle sizes of less than 1 μm to liberate the plutonium from the surrounding inert matrix

Study of plutonium and its alloys with III B elements

International Nuclear Information System (INIS)

Robert, Gregory

2003-12-01

The objective of this research thesis is to understand phenomena which intervene in the delta phase stabilisation of plutonium alloys, and to build phase diagrams for PuAl, PuGa, and PuIn. After a presentation of some properties of plutonium and of its compounds, the author presents the adopted approach: the 'ab initio' approach to the fundamental state based on the density functional theory (DFT). Then, a numerical method used within the framework of the DFT is developed, and results obtained by using the developed code are presented for the different studied materials (Al, Ga, In, Pu). A gradient correction is applied to the alloys by using the Generalised Gradient Approximation (GGA) with spin polarisation. It allows the determination of the formation energy of compounds. Hybridisation effects between plutonium and delta-generating elements (Al, Ga, In) are assessed. A statistic approach (cluster variation method, CVM) is used to assess the influence of the chemical order at short distance on the stability of the fcc solid solution, and to obtain theoretical binary alloy diagrams

Plutonium in nature

International Nuclear Information System (INIS)

Madic, C.

1994-01-01

Plutonium in nature comes from natural sources and anthropogenic ones. Plutonium at the earth surface comes principally from anthropogenic sources. It is easily detectable in environment. The plutonium behaviour in environment is complex. It seems necessary for the future to reduce releases in environment, to improve predictive models of plutonium behaviour in geosphere, to precise biological impact of anthropogenic plutonium releases

Plutonium scrap processing at the Los Alamos Scientific Laboratory

International Nuclear Information System (INIS)

Nixon, A.E.; McKerley, B.J.; Christensen, E.L.

1980-01-01

The Los Alamos Scientific Laboratory currently has the newest plutonium handling facility in the nation. Los Alamos has been active in the processing of plutonium almost since the discovery of this man-made element in 1941. One of the functions of the new facility is the processing of plutonium scrap generated at LASL and other sites. The feed for the scrap processing program is extremely varied, and a wide variety of contaminants are often encountered. Depending upon the scrap matrix and contaminants present, the majority of material receives a nitric acid/hydrofluoric acid or nitric acid/calcium fluoride leach. The plutonium nitrate solutions are then loaded onto an anion exchange column charged with DOWEX 1 x 4, 50 to 100 mesh, nitrate form resin. The column is eluted with 0.48 M hydroxyl amine nitrate. The Pu(NO 3 ) 3 is then precipitated as plutonium III oxalate which is calcined at 450 to 500 0 C to yield a purified PuO 2 product

Investigation of plutonium behaviour in artificially contaminated soil

International Nuclear Information System (INIS)

Lukshiene, B.; Druteikiene, R.

2006-01-01

The vertical migration and transformation of plutonium chemical forms artificially supplied to sandy loam columns after its exposure to natural conditions for about one year was investigated. An analysis of artificially contaminated samples after one year had shown that 81% of 239 Pu 4+ and 44% of 239 Pu 3+ were accumulated in the 0-5 cm layer of sandy loam. The data of sequential analysis of the same type of soil at the adequate artificial contamination level after one month exposure under laboratory conditions are presented as well. Pu 239 binding to soil geochemical fractions was rather uneven. The largest amount of Pu 239 (60 %) was determined in the residual fraction. Consequently, it can be assumed that organic substances and some inorganic compounds, which usually are the main components of a residual fraction, affects the retention and migration of plutonium in the soil. (authors)

Investigation of plutonium behaviour in artificially contaminated soil

International Nuclear Information System (INIS)

Luksiene, B.; Druteikiene, R.

2006-01-01

The vertical migration and transformation of plutonium chemical forms artificially supplied to sandy loam columns after its exposure to natural conditions for about one year was investigated. An analysis of artificially contaminated samples after one year had shown that 81% of 239 Pu 4+ and 44% of 239 Pu 3+ were accumulated in the 0-5 cm layer of sandy loam. The data of sequential analysis of the same type of soil at the adequate artificial contamination level after one month exposure under laboratory conditions are presented as well. Pu 239 binding to soil geochemical fractions was rather uneven. The largest amount of Pu 239 (60%) was determined in the residual fraction. Consequently, it can be assumed that organic substances and some inorganic compounds, which usually are the main components of a residual fraction, affects the retention and migration of plutonium in the soil. (authors)

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

Science.gov (United States)

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.

Separation of uranium and common impurities from solid analytical waste containing plutonium

International Nuclear Information System (INIS)

Pathak, Nimai; Kumar, Mithlesh; Thulasidas, S.K.; Hon, N.S.; Kulkarni, M.J.; Mhatre, Amol; Natarajan, V.

2014-07-01

The report describes separation of uranium (U) and common impurities from solid analytical waste containing plutonium (Pu). This will be useful in recovery of Pu from nuclear waste. This is an important activity of any nuclear program in view of the strategic importance of Pu. In Radiochemistry Division, the trace metal analysis of Pu bearing fuel materials such as PuO 2 , (U,Pu)O 2 and (U,Pu)C are being carried out using the DC arc-Carrier Distillation technique. During these analyses, solid analytical waste containing Pu and 241 Am is generated. This comprises of left-over of samples and prepared charges. The main constituents of this waste are uranium oxide, plutonium oxide and silver chloride used as carrier. This report describes the entire work carried out to separate gram quantities of Pu from large amounts of U and mg quantities of 241 Am and the effect of leaching of the waste with nitric acid as a function of batch size. The effect of leaching the solid analytical waste of (U,Pu)O 2 and AgCl with concentrated nitric acid for different time intervals was also studied. Later keeping the time constant, the effect of nitric acid molarity on the leaching of U and Pu was investigated. Four different lots of the waste having different amounts were subjected to multiple leaching with 8 M nitric acid, each for 15 minutes duration. In all the experiments the amount of Uranium, Plutonium and other impurities leached were determined using ICP as an excitation source. The results are discussed in this report. (author)

The isotopic signature of fallout plutonium in the North Pacific

Energy Technology Data Exchange (ETDEWEB)

Buesseler, K.O. [Woods Hole Oceanographic Institution, MA (United States)

1997-07-01

Plutonium analyses of a dated coral record from the French Frigate Shoals in the central North Pacific indicate that there are two major sources of Pu in this basin: close-in (tropospheric) fallout from nuclear weapons testing at the Pacific Proving Grounds in the Marshall Islands in the 1950s and global (stratospheric) fallout which peaked in 1962. Furthermore, the {sup 240}Pu/{sup 239}Pu atom ratio of fallout from the Pacific Proving Grounds is characteristically higher (0.24) than that of global fallout Pu (0.18-0.19). Seawater and sediment samples from the North Pacific exhibit a wide range of {sup 240}Pu/{sup 239}Pu values (0.19-0.34), with a trend towards higher ratios in the subsurface waters and sediment. Deep water {sup 240}Pu/{sup 239}Pu ratios are higher in the vicinity of the Marshall Islands relative to stations further from this close-in fallout source. These preliminary data suggest that fallout Pu from the Pacific Proving Grounds is more rapidly removed from the surface waters than is global fallout Pu. Plutonium geochemistry appears to be related to the physical/chemical form of Pu-bearing particles generated by different fallout sources. (author).

238Pu fuel form activities, March 1-September 30, 1985

International Nuclear Information System (INIS)

1986-01-01

The SRP portion of this report summarizes production 238 PuO 2 fuel forms for use in radioisotopic thermoelectric generators (RTG's) in the Plutonium Fuel Form (PuFF) Facility at the Savannah River Plant. The PuFF Facility began producing iridium-encapsulated, 62.5-watt 238 PuO 2 right circular cylinders for GPHS (General Purpose Heat Source) RTG's in June 1980; this program was completed in December 1983. The PuFF Facility has been placed in a production readiness mode of operation pending funding of additional heat source programs

α spectrometry on thick sources. Application to Pu dosing in U-Pu alloys with a low Pu content

International Nuclear Information System (INIS)

Guery, Marcel

1969-06-01

After having noticed that alpha spectrometry of thick sources has been not much studied, the author reports the application of this type of alpha spectrometry to a problem of plutonium dosing in uranium-plutonium alloys with low plutonium content. Four measurement and test campaigns, each being few month long, have been performed. During the first three ones, the best measurement conditions have been determined, the necessary apparatus has been acquired, and data compilation has been elaborated. This report addresses the last campaign during which exploitable results have been obtained. After some generalities about alpha rays from thick sources, the author reports a detailed examination of measurements made on U-Pu alloys, and of corrections to be made, notably those due to the Am-241 content, to stacking and to oxidation. The method appears to be very sensitive, with a precision better than 1 per cent. Improvements seem possible [fr

Plans and equipment for criticality measurements on plutonium-uranium nitrate solutions

International Nuclear Information System (INIS)

Lloyd, R.C.; Clayton, E.D.; Durst, B.M.

1982-01-01

Data from critical experiments are required on the criticality of plutonium-uranium nitrate solutions to accurately establish criticality control limits for use in processing and handling of breeder type fuels. Since the fuel must be processed both safely and economically, it is necessary that criticality considerations be based on accurate experimental data. Previous experiments have been reported on plutonium-uranium solutions with Pu weight ratios extending up to some 38 wt %. No data have been presented, however, for plutonium-uranium nitrate solutions beyond this Pu weight ratio. The current research emphasis is on the procurement of criticality data for plutonium-uranium mixtures up to 60 wt % Pu that will serve as the basis for handling criticality problems subsequently encountered in the development of technology for the breeder community. Such data also will provide necessary benchmarks for data testing and analysis on integral criticality experiments for verification of the analytical techniques used in support of criticality control. Experiments are currently being performed with plutonium-uranium nitrate solutions in stainless steel cylindrical vessels and an expandable slab tank system. A schematic of the experimental systems is presented

The toxicity of inhaled particles of 238PuO2 in dogs

International Nuclear Information System (INIS)

Muggenburg, B.A.; Guilmette, R.A.; Griffith, W.C. Jr.; Hahn, F.F.; Boecker, B.B.

1991-01-01

This study was conducted to determine the toxicity of inhaled 238 PuO 2 in the dog. Inhalation was selected because it is the mostly likely route of human exposure in the event of an accidental airborne release. Of 166 dog in the study, 72 inhaled 1.5μm and 72 inhaled 3.0 μm activity median aerodynamic diameter particles of 238 PuO 2 . Another 24 dogs inhaled the aerosol vector without plutonium. The aerosol exposures resulted in initial pulmonary burdens ranging from 37 to 0.11 and 55.5 to 0.37 kBq of 238 Pu/kg body mass, of 1.5 μm and 3.0 μ, particles, respectively. The particles dissolved slowly resulting in translocation of the Pu to liver, bone and other sites. The dogs were observed for biological effects over their life span. Necropsies were performed at death, and tissues were examined microscopically. The principal late-occurring effects were tumors of the lung, skeleton, and liver. Risk factors estimated for these cancers were 2800 lung cancers/10 4 Gy, 800 liver cancers/10 4 Gy, and 6200 bone cancers/10 4 Gy for dogs. The potential hazard from 238 Pu to humans may include tumors of the lung, bone and liver because of the likelihood of similarity of the dose patterns for the two species. 10 refs., 1 fig., 3 tabs

Radiolytic gas generation in plutonium contaminated waste materials

International Nuclear Information System (INIS)

Kazanjian, A.R.

1976-01-01

Many plutonium contaminated waste materials decompose into gaseous products because of exposure to alpha radiation. The gases generated (usually hydrogen) over long-storage periods may create hazardous conditions. To determine the extent of such hazards, knowing the gas generation yields is necessary. These yields were measured by contacting some common Rocky Flats Plant waste materials with plutonium and monitoring the enclosed atmospheres for extensive periods of time. The materials were Plexiglas, polyvinyl chloride, glove-box gloves, machining oil, carbon tetrachloride, chlorothene VG solvent, Kimwipes (dry and wet), polyethylene, Dowex-1 resin, and surgeon's gloves. Both 239 Pu oxide and 238 Pu oxide were used as radiation sources. The gas analyses were made by mass spectrometry and the results obtained were the total gas generation, the hydrogen generation, the oxygen consumption rate, and the gas composition over the entire storage period. Hydrogen was the major gas produced in most of the materials. The total gas yields varied from 0.71 to 16 cm 3 (standard temperature pressure) per day per curie of plutonium. The oxygen consumption rates varied from 0.0088 to 0.070 millimoles per day per gram of plutonium oxide-239 and from 0.0014 to 0.0051 millimoles per day per milligram 238 Pu

Equilibrium, kinetic and reactive transport models for Pu: employing numerical methods to uncover the nature of the intrinsic colloid

International Nuclear Information System (INIS)

Schwantes, Jon M.; Batchelor, Bill

2000-01-01

Future missions for the Department of Defense include processing plutonium for vitrification and conversion to mixed oxide fuels for commercial use. Such processing could result in the production of Pu-containing waste and unplanned releases of Pu to the environment. Some releases related to plutonium processing have occurred in the past. However, scientists are currently not able to explain the observed behavior of plutonium in natural systems. For example, classical filtration theory predicts that plutonium transport within groundwater should be limited to a few tens of meters. Experimental observations, however, show that plutonium is present in groundwater at distances orders of magnitude farther away from its source than predicted. Before adequate disposal practices can be designed for plutonium, its behavior in these systems must be better understood. The overall goal of this project is to develop equilibrium, kinetic and reactive transport models that describe the behavior of Pu in aqueous systems and to apply these models to natural and engineered systems

The AS-76 interlaboratory experiment on the alpha spectrometric determinaion of Pu-238. Part 3: Preparation and characterization of samples

International Nuclear Information System (INIS)

Bortels, G.; Broothaerts, J.; Bievre, P. de

1980-01-01

Four plutonium samples containing 0.2, 0.8, 1.6 and 0.9 atom % of 238 Pu have been prepared for the Interlaboratory Experiment AS-76. Of these three were input solutions from a reprocessing plant. The fourth sample was from a plutonium product solution. These samples have been characterized by two alpha spectrometry laboratories and two mass spectrometry laboratories to certify the ratio of alpha activities 238 Pu/( 239 Pu + 240 Pu) and the isotopic composition, respectively

Estimation of 239Pu in urine, influence of Sulkowich reagent

International Nuclear Information System (INIS)

Kalaiselvan, S.; Prasad, M.V.R.; Jeevanram, R.K.

1988-01-01

Plutonium is known to be co-precipitated with Sulkowich reagent as calcium ammonium oxalate. In adopting this technique for bio-assay of plutonium, its accuracy depends on the self-absorption of the resulting precipitate in each urine sample. Pu recovery experiments were carried out with varying concentration of Ca and Mg, using different volumes of Sulkowich reagent. When the sample volume is 500 ml, Pu in urine can be estimated with an accuracy and precision of 74.38%+-7.4%, with a detection limit of 0.06 Bq (1.6 pCi) per dm 3 . (author) 3 refs.; 2 figs.; 2 tabs

Bone tumors induced by inhalation of 238PuO2 in dogs

International Nuclear Information System (INIS)

Park, J.F.; Lund, J.E.; Ragan, H.A.; Hackett, P.L.; Frazier, M.E.

1976-01-01

Plutonium-238, an alpha-emitting radionuclide, is used as a heat source in thermoelectric power generators such as have been employed on lunar expeditions of communications satellites and in cardiac pacemakers. It has an 86.4 year half-life and emits 5.5 MeV alpha particles. Beagle dogs were given single 10 to 30 minute exposures to 238 PuO 2 aerosols to study the long-term translocation of plutonium and biologicl effects. Dogs with a terminal body burden ranging from 7 to 260 MuCi were euthanized due to respiratory insufficiency related to plutonium-induced pneumonitis during the first 3 years after exposure. Nine of the 11 dogs euthanized during the 4 to 6 year postexposure period had osteosarcomas. The terminal plutonium body burden in the tumor-bearing dogs ranged from 0.5 to 2.6 muCi with 30 to 55 percent of the plutonium in the skeleton. Experiments are in progress to further define the dose-effect relationship of inhaled 238 PuO 2 and investigate the mechanisms of plutonium-induced neoplasia

Plutonium roundtable discussion

International Nuclear Information System (INIS)

Penneman, R.A.

1982-01-01

The roundtable discussion began with remarks by the chairman who pointed out the complicated nature of plutonium chemistry. Judging from the papers presented at this symposium, he noticed a pattern which indicated to him the result of diminished funding for investigation of basic plutonium chemistry and funding focused on certain problem areas. Dr. G.L. silver pointed to plutonium chemists' erroneous use of a simplified summary equation involving the disproportionation of Pu(EV) and their each of appreciation of alpha coefficients. To his appreciation of alpha coefficients. To his charges, Dr. J.T. Bell spoke in defense of the chemists. This discussion was followed by W.W. Schulz's comments on the need for experimental work to determine solubility data for plutonium in its various oxidation states under geologic repository conditions. Discussion then turned to plutonium pyrachemical process with Dana C. Christensen as the main speaker. This paper presents edited versions of participants' written version

Plutonium isotopic measurements by gamma-ray spectroscopy

International Nuclear Information System (INIS)

Gunnink, R.

1973-11-01

A method is reported for analysis of isotopic and total plutonium by detecting and analyzing gamma rays emitted by the sample. A computerized prototype-system was developed and is now being routinely used at the Savannah River Plant for the nondestructive assay of solution samples. The analyses for 238 Pu, 239 Pu, 240 Pu, 241 Pu, and for 241 Am, when it is present, can be made in counting times as short as 10 to 15 minutes under optimum conditions. Comparison of isotopic ratio values with mass spectrometry generally shows agreement within 0.1 percent for 239 Pu and about 1 percent for 240 Pu and 241 Pu. Some preliminary isotopic measurements on solids are also discussed. (U.S.)

Plutonium in a grassland ecosystem. [Rocky Flats Plant

Energy Technology Data Exchange (ETDEWEB)

Little, C.A.

1976-08-01

A study was made of plutonium contamination of grassland at the Rocky Flats plant northwest of Denver, Colorado. Of interest were: the definition of major plutonium-containing ecosystem compartments; the relative amounts in those compartments; how those values related to studies done in other geographical areas; whether or not the predominant isotopes, /sup 238/Pu and /sup 239/Pu, behaved differently; and what mechanisms might have allowed for the observed patterns of contamination. Samples of soil, litter, vegetation, arthropods, and small mammals were collected for Pu analysis and mass determination from each of two macroplots. Small aliquots (5 g or less) were analyzed by a rapid liquid scintillation technique and by alpha spectrometry. Of the compartments sampled, greater than 99 percent of the total plutonium was contained in the soil and the concentrations were significantly inversely correlated with distance from the contamination source, depth of the sample, and particle size of the sieved soil samples. The soil data suggested that the distribution of contamination largely resulted from physical transport processes.

Conceptual Design for the Pilot-Scale Plutonium Oxide Processing Unit in the Radiochemical Processing Laboratory

Energy Technology Data Exchange (ETDEWEB)

Lumetta, Gregg J.; Meier, David E.; Tingey, Joel M.; Casella, Amanda J.; Delegard, Calvin H.; Edwards, Matthew K.; Jones, Susan A.; Rapko, Brian M.

2014-08-05

This report describes a conceptual design for a pilot-scale capability to produce plutonium oxide for use as exercise and reference materials, and for use in identifying and validating nuclear forensics signatures associated with plutonium production. This capability is referred to as the Pilot-scale Plutonium oxide Processing Unit (P3U), and it will be located in the Radiochemical Processing Laboratory at the Pacific Northwest National Laboratory. The key unit operations are described, including plutonium dioxide (PuO2) dissolution, purification of the Pu by ion exchange, precipitation, and conversion to oxide by calcination.

Qualitative chemical analysis of plutonium by Alpha spectroscopy

International Nuclear Information System (INIS)

Ramirez G, J Qumica.J.

1994-01-01

In this work the separation and purification of plutonium from irradiated uranium was done. The plutonium, produced by the irradiation of uranium in a nuclear reactor and the β decay of 239 Np, was stabilized to Pu +4 with sodium nitrite. Plutonium was separated from the fission products and uranium by ion exchange using the resin Ag 1 X 8. It was electrodeposited on stainless steel discs and the alpha radioactivity of plutonium was measured in a surface barrier detector. The results showed that plutonium was separated with a radiochemical purity higher than 99 %. (Author)

Standard test method for plutonium assay by plutonium (III) diode array spectrophotometry

CERN Document Server

American Society for Testing and Materials. Philadelphia

2002-01-01

1.1 This test method describes the determination of total plutonium as plutonium(III) in nitrate and chloride solutions. The technique is applicable to solutions of plutonium dioxide powders and pellets (Test Methods C 697), nuclear grade mixed oxides (Test Methods C 698), plutonium metal (Test Methods C 758), and plutonium nitrate solutions (Test Methods C 759). Solid samples are dissolved using the appropriate dissolution techniques described in Practice C 1168. The use of this technique for other plutonium-bearing materials has been reported (1-5), but final determination of applicability must be made by the user. The applicable concentration range for plutonium sample solutions is 10–200 g Pu/L. 1.2 The values stated in SI units are to be regarded as standard. No other units of measurement are included in this standard. 1.3 This standard does not purport to address all of the safety concerns, if any, associated with its use. It is the responsibility of the user of this standard to establish appropria...

Determination of Pu in soil samples; Determinacion de Pu en muestras de suelo

Energy Technology Data Exchange (ETDEWEB)

Torres C, C. O.; Hernandez M, H.; Romero G, E. T. [ININ, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico); Vega C, H. R., E-mail: carioli_32907@hotmail.com [Universidad Autonoma de Zacatecas, Unidad Academica de Estudios Nucleares, Cipres No. 10, Fracc. La Penuela, 98068 Zacatecas, Zac. (Mexico)

2016-10-15

The irreversible consequences of accidents occurring in nuclear plants and in nuclear fuel reprocessing sites are mainly the distribution of different radionuclides in different matrices such as the soil. The distribution in the superficial soil is related to the internal and external exposure to the radiation of the affected population. The internal contamination with radionuclides such as Pu is of great relevance to the nuclear forensic science, where is important to know the chemical and isotopic compositions of nuclear materials. The objective of this work is to optimize the radiochemical separation of plutonium (Pu) from soil samples and to determine their concentration. The soil samples were prepared using acid digestion assisted by microwave; purification of Pu was carried out with AG1X8 resin using ion exchange chromatography. Pu isotopes were measured using ICP-SFMS. In order to reduce the interference due to the presence of {sup 238}UH {sup +} in the samples, a solvent removal system (Apex) was used. In addition, the limit of detection and quantification of Pu was determined. It was found that the recovery efficiency of Pu in soil samples ranges from 70 to 93%. (Author)

BenzoDODA grafted polymeric resin—Plutonium selective solid sorbent

Energy Technology Data Exchange (ETDEWEB)

Ruhela, R., E-mail: riteshr@barc.gov.in [Materials Processing Division, Materials Group, Bhabha Atomic Research Centre, Trombay, Mumbai 400085 (India); Panja, S., E-mail: surajit@barc.gov.in [Fuel Reprocessing Division, Nuclear Fuels Group, Bhabha Atomic Research Centre, Trombay, Mumbai 400085 (India); Singh, A.K. [Materials Processing Division, Materials Group, Bhabha Atomic Research Centre, Trombay, Mumbai 400085 (India); Dhami, P.S.; Gandhi, P.M. [Fuel Reprocessing Division, Nuclear Fuels Group, Bhabha Atomic Research Centre, Trombay, Mumbai 400085 (India)

2016-11-15

Highlights: • BenzoDODA grafted polymeric resin was synthesized and evaluated for sorption of Pu(IV). • Fast sorption kinetics for ‘Pu(IV)’. • Ease of back extraction of ‘Pu’ form loaded resin. • Ease of recyclability and fair stability in HNO{sub 3} medium. - Abstract: A new ligand grafted polymeric resin (BenzoDODA SDVB) was synthesized by covalently attaching plutonium selective ligand (BenzoDODA) on to styrene divinyl benzene (SDVB) polymer matrix. BenzoDODA SDVB resin was evaluated for separation and recovery of plutonium(IV) from nitric acid medium. Sorption of Pu(IV) was found to decrease with the increase in nitric acid concentration, with very small sorption above 7.0 M HNO{sub 3}. Sorption kinetics was fast enough to achieve the equilibrium within 60 min of contact where the kinetic data fitted well to pseudo-second-order model. Sorption isotherm data fitted well to Langmuir model suggesting chemical interaction between the BenzoDODA moiety and plutonium(IV) ions. Sorption studies with some of representative radionuclides of high level waste showed that BenzoDODA SDVB is selective and therefore could be a promising solid sorbent for separation and recovery of plutonium. Further, the theoretical calculations done on BenzoDODA SDVB resin suggested Pu(NO{sub 3}){sub 4}·BenzoDODA (1:1) sorbed complex conformed to generally observed square antiprism geometry of the plutonium complexes, with contributions from oxygen atoms of four nitrate ions as well as from four oxygen atoms present in BenzoDODA (two phenolic ether oxygen atoms and two carbonyl oxygen atoms of amidic moiety).

Base case short-term Pu-oxide store. 2. Pt

International Nuclear Information System (INIS)

1978-08-01

This paper describes the interim storage of plutonium oxide after its conversion from plutonium nitrate and before fabrication into fuel elements. The capacity of the store is 3 tons Pu. A description of the major handling, criticality, maintenance and physical protection philosophy is given, together with comments on the safety of the store and its impact on the environment

Determination of americium and plutonium in autopsy tissue: methods and problems

International Nuclear Information System (INIS)

Boyd, H.A.; Eutsler, B.C.; McInroy, J.F.

1979-01-01

The current methods used by the tissue analysis program at LASL for the determination of americium and plutonium in autopsy tissue are described. Problems affecting radiochemical yield are discussed. Included are problems associated with sample preparation, separation of plutonium from large amounts of bone ash, and reagent contamination. The average 242 Pu tracer yield for 1800 Pu determinations is 78 +- 12%. The average 242 Am tracer yield is 85 +- 7% for 40 determinations

High 240Pu FTR/EMC experiments and analysis: Carbide fuel and UO2 blanket subassembly worths

International Nuclear Information System (INIS)

Ombrellaro, P.A.

1977-06-01

Carbide-plutonium fuel and UO 2 blanket subassembly worth measurements performed at ANL in the EMC/LWR were analyzed. Composition exchange worth calculations were performed for: (a) the replacement of high- 240 Pu fuel composition for low- 240 Pu fuel composition and carbide-plutonium fuel composition, successively, in the center subassembly of the core; (b) the replacement of low- 240 Pu fuel composition for carbide--plutonium fuel composition in one outer driver subassembly; and (c) the replacement of the radial reflector composition with UO 2 blanket composition in one subassembly of the radial reflector. The composition exchange worth calculations were performed in two-dimensional x,y geometry, using diffusion theory and perturbation theory. Each method produces about the same calculated-to-experimental bias factors

Plutonium 238/239 Decorporation Model

Science.gov (United States)

2014-10-01

4. Transfer Coefficients for the DTPA Biokinetic Model (Breustedt 2009) ...................... 25 Table 5. Decay Properties of Pu-238 and Pu-239...volume 2), cesium-137 (volume 3), F. tularensis (volume 4), sulfur mustard (volume 5), americium-241 (volume 6), Y. pestis (volume 7), botulinum ... toxin (volume 8), plutonium-238/239 (volume 9) and vesicants (volume 10, an expansion on volume 5). This paper presents an inhalation exposure model for

Americium and plutonium in water, biota, and sediment from the central Oregon coast

International Nuclear Information System (INIS)

Nielsen, R.D.

1982-06-01

Plutonium-239, 240 and americium-241 were measured in the mussel Mytilus californianus from the region of Coos Bay, OR. The flesh of this species has a plutonium concentration of about 90 fCi/kg, and an Am-241/Pu-239, 240 ratio that is high relative to mixed fallout, ranging between two and three. Transuranic concentrations in sediment, unfiltered water, and filterable particulates were also measured; none of these materials has an Am/Pu ratio as greatly elevated as the mussels, and there is no apparent difference in the Am/Pu ratio of terrestrial runoff and coastal water. Sediment core profiles do not allow accumulation rates or depositional histories to be identified, but it does not appear that material characterized by a high Am/Pu ratio has ever been introduced to this estuary. Other bivalves (Tresus capax and Macoma nasuta) and a polychaete (Abarenicola sp.) do not have an elevated Am/Pu ratio, although the absolute activity of plutonium in the infaunal bivalves is roughly four times that in the mussels

PLUTONIUM METALLIC FUELS FOR FAST REACTORS

Energy Technology Data Exchange (ETDEWEB)

STAN, MARIUS [Los Alamos National Laboratory; HECKER, SIEGFRIED S. [Los Alamos National Laboratory

2007-02-07

Early interest in metallic plutonium fuels for fast reactors led to much research on plutonium alloy systems including binary solid solutions with the addition of aluminum, gallium, or zirconium and low-melting eutectic alloys with iron and nickel or cobalt. There was also interest in ternaries of these elements with plutonium and cerium. The solid solution and eutectic alloys have most unusual properties, including negative thermal expansion in some solid-solution alloys and the highest viscosity known for liquid metals in the Pu-Fe system. Although metallic fuels have many potential advantages over ceramic fuels, the early attempts were unsuccessful because these fuels suffered from high swelling rates during burn up and high smearing densities. The liquid metal fuels experienced excessive corrosion. Subsequent work on higher-melting U-PuZr metallic fuels was much more promising. In light of the recent rebirth of interest in fast reactors, we review some of the key properties of the early fuels and discuss the challenges presented by the ternary alloys.

Conversion electron spectrometry of Pu isotopes with a silicon drift detector.

Science.gov (United States)

Pommé, S; Paepen, J; Peräjärvi, K; Turunen, J; Pöllänen, R

2016-03-01

An electron spectrometry set-up was built at IRMM consisting of a vacuum chamber with a moveable source holder and windowless Peltier-cooled silicon drift detector (SDD). The SDD is well suited for measuring low-energy x rays and electrons emitted from thin radioactive sources with low self-absorption. The attainable energy resolution is better than 0.5keV for electrons of 30keV. It has been used to measure the conversion electron spectra of three plutonium isotopes, i.e. (238)Pu, (239)Pu, (240)Pu, as well as (241)Am (being a decay product of (241)Pu). The obtained mixed x-ray and electron spectra are compared with spectra obtained with a close-geometry set-up using another SDD in STUK and spectra measured with a Si(Li) detector at IRMM. The potential of conversion electron spectrometry for isotopic analysis of mixed plutonium samples is investigated. With respect to the (240)Pu/(239)Pu isotopic ratio, the conversion electron peaks of both isotopes are more clearly separated than their largely overlapping peaks in alpha spectra. Copyright © 2015 The Authors. Published by Elsevier Ltd.. All rights reserved.

Plutonium storage study

International Nuclear Information System (INIS)

1979-01-01

This Spanish study gives a more detailed analysis of a possible store for plutonium oxide. The capacity of the store is assumed to be 30 t Pu and the minimum storage time 2 years. The study includes a general description of the store and its design philosophy; comments on the quality and properties of the material stored; a detailed criticality study and comments on gas and heat generation and shielding requirements; and a brief cost evaluation. Costs are estimated to be about $110/kg PuO 2 /year

Artificial radioactivity and marine environment. Study of 238Pu, 239Pu+240Pu, 241Pu and 241Am in the Mediterranean sea

International Nuclear Information System (INIS)

Ballestra, Serge.

1980-10-01

This paper is in two parts. Part one is about the methods for analyzing transuranium elements particularly the development of an analytical process for plutonium and for perfecting an Americium analyzing method, capable of treating samples of 200 litres of sea water, 100 grams of sediment and 100 grams of biological matter. Part two concerns the in situ determinations carried out within the scope of the study on the distribution and behaviour of transuranium elements in the Mediterranean sea. The high sea studies concerned the effects of atmospheric fall out and the vertical distribution of Pu and Am. Studies along the coasts enabled a quantitative study to be made of the contribution of rivers to the Mediterranean and to study the distribution of Pu along the French Mediterranean coast line [fr

Thermodynamics properties of plutonium in NaCl-KCl and CaCl2 at 1073 K and in liquid gallium

International Nuclear Information System (INIS)

Lambertin, D.; Ched'homme, S.; Bourges, G.; Pescayre, L.; Sanchez, S.; Picard, G.

2004-01-01

Cadmium and bismuth metal are mostly used as solvent in nuclear pyrochemical processes and especially in actinides/lanthanides separations. Gallium metal has been chosen because no literature values are available with plutonium and its regeneration by refining at low temperature is possible. Electrochemical window of gallium metal and activity coefficient of plutonium in gallium have been determined by using potentiometric method. Secondly, the electrochemical properties of plutonium have been studied in molten equimolar NaCl/KCl and CaCl 2 at 1073 K by cyclic voltammetry. The standard potentials of Pu(III)/Pu redox couple, respectively, -2,54 V and -2,51 V, led to the calculation of the activity coefficients of Pu(III). In CaCl 2 the complexation of Pu(III) ions is lower and the voltage gap between Pu(III)/Pu couple and the solvent limit is higher. The new data on plutonium electrochemistry in molten chlorides and liquid gallium media combined with literature data on lanthanides suggest that gallium can be a good solvent metal for pyro-chemistry separation. (authors)

The determination of Plutonium content in urine using anion exchange resin method

International Nuclear Information System (INIS)

Mukh-Syaifudin

1996-01-01

The possibility of internal contamination by plutonium is usually determined through urine analysis. The technique involved the co-precipitation of plutonium with rhodizonic acid by the addition of sodium hydroxide, the re-extraction of Pu into concentrated HCl, dissolution of Pu in 8 N HCI + Cl 2 solution, and the purification of plutonium through AGI-X8 anion exchange resin in columns with a diameter of 4 and 7 mm. The eluent was evaporated and the residu was dissolved in 8 N HCI and then deposited directly onto a Lexan slide or electrodeposited onto a stainless steel disc and the alpha emission of Pu was counted by using alpha spectrometry. The results showed that the recoveries of Pu-242 tracer by using column 7 mm and direct deposition and electrodeposition methods were 28.783% and 16.444%, respectively. The recoveries of Pu-242 by using column 4 mm and direct deposition and electrodeposition methods were 64.834% and 55.661%, respectively. From the percentage of recovery, it can be concluded that the direct deposition method was relatively better than the electrodeposition method. The recovery of Pu-242 by using column of 4 mm in diameter was higher than that of column 7 mm

The application of N,N-dimethylhydroxylamine as reductant for the separation of plutonium from uranium

International Nuclear Information System (INIS)

Jinping Liu; Hui He; Hongbin Tang; Yanxin Chen

2011-01-01

Both single stage and multi-stages experiments on stripping plutonium with N,N-dimethylhydroxylamine (DMHAN) as reductant with methylhydrozine (MMH) as supporting reductant were carried out. The effect of contact time, temperature, acidity, concentration of DMHAN on back-extraction rate of plutonium was investigated in the single stage experiment. The results demonstrated that the reaction of stripping Pu(IV) in the organic phase (30% TBP-kerosene) 1BF solutions by DMHAN exhibits excellent stripping efficiency. Under the given conditions, the back-extraction rate of plutonium reaches 90% within 2 min. Higher temperature, lower acidity and the increased concentration of DMHAN benefit the stripping reaction. The concentration profile of HNO 3 , uranium and plutonium were determined in a multi-stages mixer-settler after the steady state of the back-extraction, and the multi-stages results show that the plutonium can be separated effectively from uranium. The recovery of plutonium and uranium reach 99.995% or over 99.99% respectively. The separation factor of U from Pu (SF Pu/U ) is about 2 x 10 4 . (author)

Gas adsorption during storage of plutonium dioxide powders

International Nuclear Information System (INIS)

Cuillerdier, C.; Cossonnet, C.; Germain, M.

1984-10-01

Adsorption phenomena occuring in plutonium dioxide containers are studied for the determination of safe conditions for storage and transportation of plutonium dioxide powders. Adsorption on dried PuO 2 of air individual gases, influence of powder isotopic composition, chemisorption, effect of moisture are determined. Adsorption of dry air obeys an Elovich's law for its kinetics it is greatly exchange by α radiolysis. Pressure in the container can be reduced by storage under dry inert gas (Ar), decreasing the PuO 2 load and using powder containing preadsorbed water or wet air then radiolysis may occur (H 2 formation)

Ecological behavior of plutonium and americium in a freshwater pond

International Nuclear Information System (INIS)

Emery, R.M.; Klopfer, D.C.; Garland, T.R.; Weimer, W.C.

1976-01-01

A plutonium (Pu) processing waste pond on the Hanford Reservation has been studied since mid-1973 to characterize the pond's limnology and determine the ecological behavior of transuranics in this ecosystem. This ultra-eutrophic pond has a water inflow rate of 10 m 3 /min, of which 95% leaves the pond by percolation. Macrophytes (mainly Potamogeton), algae (mainly Cladophora), benthic invertebrates (mainly dipteran and odonate larvae, hemipterans, amphipods and gastropods) and goldfish are the major biotic components of the system. Sediments appear to be the principal repository of Pu and Am, having mean concentrations for 238 Pu, 239 240 Pu and 241 Am of 112, 121 and 71 pCi/g (dry), respectively. Mean ratios of isotopes in the sediments are 0.85 for 238 Pu to 239 240 Pu, and 0.49 for 241 Am to 239 240 Pu. Algal floc (decomposing algal material) is the major concentrator of Pu and Am in the pond having mean concentrations of 238 Pu of 986 pCi/g, for 239 240 Pu of 615 pCi/g, and for 241 Am of 256 pCi/g. Watercress (Rorippa) had Pu levels about equal to those of the sediments, while dragonfly larvae (Libellula) and snails (Lymnaea) along with watercress had Am levels approximating those of the sediments. The remaining biota had Pu and Am levels which were generally well below those of the sediments.Preliminary in situ experiments indicate that goldfish reach an equilibrium level for Pu of about 15 pCi/g within a few days of exposure to the pond, after which they may remain active in the pond for many months without further accumulation. Experimental goldfish established ratios of 238 Pu to 239 240 Pu and 241 Am to 239 240 Pu that were similar to all other pond biota within 2 weeks of pond residence, suggesting a common source of biologically available Pu and Am

Influence of iron redox transformations on plutonium sorption to sediments

Energy Technology Data Exchange (ETDEWEB)

Hixon, A.E.; Powell, B.A. [Environmental Engineering and Earth Sciences, Clemson Univ., Clemson, SC (United States); Hu, Y.J.; Nitsche, H. [Dept. of Chemistry, Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab., Berkeley, CA (United States); Kaplan, D.I. [Savannah River National Lab., Aiken, SC (United States); Kukkadapu, R.K.; Qafoku, O. [Pacific Northwest National Lab., Richland, WA (United States)

2010-07-01

Plutonium subsurface mobility is primarily controlled by its oxidation state, which in turn is loosely coupled to the oxidation state of iron in the system. Experiments were conducted to examine the effect of sediment iron mineral composition and oxidation state on plutonium sorption and reduction. A pH 6.3 vadose zone sediment containing iron oxides and iron-containing phyllosilicates was treated with various complexants (ammonium oxalate) and reductants (hydroxylamine hydrochloride and dithionite-citrate-bicarbonate (DCB)) to selectively leach and/or reduce iron oxide and phyllosilicate/clay Fe(III). {sup 57}Fe-Moessbauer spectroscopy was used to identify initial iron mineral composition of the sediment and monitor dissolution and reduction of iron oxides and reduction of phyllosilicate Fe(III). {sup 57}Fe-Moessbauer spectroscopy showed that the Fe-mineral composition of the untreated sediment is: 25-30% hematite, 60-65% small-particle/Al-goethite, and < 10% Fe(III) in phyllosilicate; there was no detectable Fe(II). Upon reduction with a strong chemical reductant (dithionite-citrate-bicarbonate buffer), much of the hematite and goethite was removed. Partial reduction of phyllosilicate Fe(III) was evident in the sediments subjected to DCB treatment. Sorption of Pu(V) was monitored over one week for the untreated and each of five treated sediment fractions. Plutonium oxidation state speciation in the aqueous and solid phases was monitored using solvent extraction, coprecipitation, and XANES. The rate of sorption appears to correlate with the fraction of Fe(II) in the sediment (untreated or treated). Pu(V) was the only oxidation state measured in the aqueous phase, irrespective of treatment, whereas Pu(IV) and much smaller amounts of Pu(V) and Pu(VI) were measured in the solid phase. Surface-mediated reduction of Pu(V) to Pu(IV) occurred in treated and untreated sediment samples; Pu(V) remained on untreated sediment surface for two days before reducing to Pu

Two convenient low-temperature routes to single crystals of plutonium dioxide

Energy Technology Data Exchange (ETDEWEB)

Meredith, Nathan A. [Departments of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, IN 46556 (United States); Wang, Shuao; Diwu, Juan [School of Radiation Medicine and Protection and School of Radiological and Interdisciplinary Sciences, Soochow University, Suzhou, Jiangsu 215123 (China); Albrecht-Schmitt, Thomas E., E-mail: talbrechtschmitt@gmail.com [Department of Chemistry and Biochemistry, Florida State University, Tallahassee, FL 32306 (United States)

2014-11-15

Highlights: • Two low-temperature routes to the growth single crystals of plutonium dioxide. • Safer methods of preparing PuO{sub 2} single crystals that do not involve solid-state synthetic techniques. • Solvothermal crystal growth of plutonium dioxide. - Abstract: During the solvothermal synthesis of a low-dimensional borate, KB{sub 5}O{sub 7}(OH){sub 2}⋅2H{sub 2}O, in the presence of Pu(III), single crystals of plutonium dioxide unexpectedly formed. Single crystals of PuO{sub 2} also formed during the hydrothermal synthesis of another borate, Na{sub 2}B{sub 5}O{sub 8}(OH)⋅2H{sub 2}O, in the presence of Pu(III). The reactions were conducted at 170 °C and 150 °C, respectively, which are much lower temperature than previously reported preparations of crystalline PuO{sub 2}. Yellow–green crystals with a tablet habit were characterized by single crystal X-ray diffraction and solid-state UV–vis–NIR absorption spectroscopy. The crystal structure was solved by direct methods with R{sub 1} = 1.26% for 19 unique observed reflections. PuO{sub 2} is cubic, space group Fm3{sup ‾}m, and adopts the fluorite structure type. The lattice parameter was determined to be a = 5.421(5) Å giving a volume of 159.3(2) Å{sup 3}. The absorption spectrum is consistent with Pu(IV)

Determination of 238Pu, 239+240Pu, 241Pu and 241Am in radioactive waste from IPEN reactor

International Nuclear Information System (INIS)

Geraldo, Bianca; Taddei, Maria Helena T.; Cheberle, Sandra M.; Ferreira, Marcelo T.

2011-01-01

Ion exchange resin is a common type of radioactive waste arising from treatment of coolant water of the main circuit of research and nuclear power reactors. This waste contains high concentrations of fission and activation products. The management of this waste includes its characterization in order to determine and quantify specific radionuclides including those known as difficult-to-measure radionuclides (RDM). The analysis of RDMs generally involves expensive and time-consuming complex radiochemical analysis for purification and separation of the radionuclides. The objective of this work is to show an easy methodology for quantifying plutonium and americium isotopes in spent ion exchange resin, used for purification of the cooling water of the IEA-R1 reactor located at the Nuclear and Energy Research Institute, IPEN-CNEN/SP. The resins were destroyed by acid digestion, followed by purification and separation of the Pu and Am isotopes with anionic and chromatographic resins. 238 Pu, 239 + 24 '0Pu, and 24 '1Am isotopes were analyzed in an alpha spectrometer equipped with surface barrier detectors. 241 Pu isotope was analyzed by liquid scintillation counting. Chemical recovery yield ranged from 73 to 98% for Pu and 77 to 98% for Am, demonstrating that the methodology is suitable for identification and quantification of the isotopes studied in spent resins. (author)

Plutonium interactions with soil microbial metabolites: effect on plutonium sorption by soil

International Nuclear Information System (INIS)

Wildung, R.E.; Garland, T.R.; Rogers, J.E.

1987-01-01

To develop an understanding of the mechanisms of plutonium (Pu) complexation and solubilization by soil microorganisms, a broad range of bacteria and fungi were isolated in pure cultures from soil on the basis of metal tolerance and carbon requirements. The organisms were then used in investigations to examine Pu cellular transport, Pu complexation by extracellular metabolites, and the effects of complexation on Pu valence state, chemical form, and solubility in soil. Of the 239 bacteria and 250 fungi isolated from soil, 19 bacteria and 60 fungi were selected for detailed study. Of these organisms, 15 bacteria and 18 fungi grew to form extracellular Pu complexes that increased the concentration of Pu in soil column eluates relative to controls. Elution through soil effectively removed positively charged Pu complexes. Increased Pu mobility in soil resulted from the formation of neutral and negatively charged Pu complexes, which differed with organism type. In the presence of known microbial metabolites and synthetic ligands (DTPA, EDTA, EDDHA), Pu(VI) was reduced to Pu(IV) before complexation, suggesting that Pu(IV) would be the dominant valence state associated with organic complexes in soils. Studies on selected organisms indicated that both active Pu transport and Pu sorption on the cell occurred, and these phenomena, as well as complexation by extracellular metabolites of Pu, were a function of the form of Pu supplied, the organism type and growth characteristics, and the ability of the organism to alter extracellular pH. 18 references, 6 figures, 7 tables

Comparative behavior of plutonium and americium in the equatorial Pacific

International Nuclear Information System (INIS)

Noshkin, V.E.; Wong, K.M.; Jokela, T.A.; Brunk, J.L.; Eagle, R.J.

1983-01-01

Inventories of 239 + 240 Pu and 241 Am greatly in excess of global fallout levels persist in the benthic environments of Bikini and Enewetak Atolls. The amount of 239 + 240 Pu mobilized to solution at the atolls can be predicted from a distribution coefficient K/sub d/ of 2.3 x 10 5 and the mean sediment concentrations. The mobilized 239 + 240 Pu has solute-like characteristics and different valence states coexist in solution - the largest fraction of the soluble plutonium is in an oxidized form (+V,VI). The adsorption of plutonium to sediments is not completely reversible because of changes that occur in the relative amounts of the mixed oxidation states in solution with time. Characteristics of 239 + 240 Pu described at one location may not necessarily describe its behavior elsewhere. The relative amounts of 241 Am to 239 + 240 Pu may be altered in future years because of mobilization and radiological decay

Plutonium distribution and remobilization in sediments of the Rhone River mouth (North-Western Mediterranean); Distribution et remobilisation du plutonium dans les sediments du prodelta du Rhone (Mediterranee nord-occidentale)

Energy Technology Data Exchange (ETDEWEB)

Lansard, B

2004-06-15

The aim of the present study was to describe the distribution and remobilization of plutonium (Pu) in the sediments off the Rhone river mouth. Most of the {sup 238}Pu and {sup 239,240}Pu isotopes introduced into the Rhone River were discharged by the liquid effluents released from the Marcoule reprocessing plant, located 120 km upstream the river mouth. Due to its high affinity for particles and its long half life, {sup 238}Pu is a promising tracer to follow the dispersion of particulate matter from the Rhone River to the Mediterranean Sea. During the 3 REMORA cruises, sediment samples were specifically collected in the Rhone pro-delta area and more offshore on the whole continental shelf of the Gulf of Lions. The measurements of alpha emitters gave a first detailed spatial distribution of Pu isotope concentrations in surface sediments off the Rhone mouth. Using {sup 137}Cs concentrations and their correlations with Pu isotopes, we were able to give a first estimate of Pu inventories for the sediments of the study area. In 2001, plutonium inventories were estimated to 92 {+-} 7 GBq of {sup 238}Pu and 522 {+-} 44 GBq of {sup 239,240}Pu for an area of 500 km{sup 2} in front of the Rhone River mouth. Roughly, 50 % of these inventories are trapped in an area of 100 km{sup 2} corresponding to the extent of the Rhone pro-delta zone. In spring 2002, an ADCP, with current velocity and wave measurements, was moored off the Rhone River mouth. This unique in situ dataset highlights the major role of South-East swells in the erosion of pro-deltaic sediments and their dispersion to the South-Westward direction. Plutonium remobilization was examined using a new experimental design based on sediment resuspension processes studied within a linear recirculating flume. For Gulf of Lions sediments and for a given hydrodynamic stress, remobilization fluxes raised a maximum of 0.08 Bq.m{sup -2}.h{sup -1} for {sup 238}Pu and 0.64 Bq.m{sup -2}.h{sup -1} for {sup 239,240}Pu. A first

Plutonium Speciation, Solubilization and Migration in Soils

International Nuclear Information System (INIS)

Neu, M.; Runde, W.

1999-01-01

This report summarizes research completed in the first half of a three-year project. As outlined in the authors' proposal they are focusing on (1) characterizing the plutonium at an actinide contaminated site, RFETS, including determining the origin, dispersion, and speciation of the plutonium, (2) studying environmentally important plutonium complexes, primarily hydroxides and carbonates, and (3) examining the interactions of plutonium species with manganese minerals. In the first year the authors focused on site based studies. This year they continue to characterize samples from the RFETS, study the formation and structural and spectroscopic features of environmentally relevant Pu species, and begin modeling the environmental behavior of plutonium

Translocation dynamics of Pu(NO3)4 and PuO2 from puncture wounds to lymph nodes and major organs of beagles

International Nuclear Information System (INIS)

Bistline, R.W.; Lebel, J.L.; Dagle, G.E.

1976-01-01

The translocation dynamics of plutonium and americium from simulated puncture wounds in the paws of beagle dogs following contamination with Pu(NO 3 ) 4 and high-fired PuO 2 was studied. Fractions of initial implant transported to the first major lymph node and to major body organs were measured with in vivo counting equipment and by radiochemical analysis of tissue material collected at necropsy. Samples were obtained from serial necropsies ranging from 2 weeks to 1 year after implant. The difference in lymph node and organ-accumulation dynamics between the two chemical forms and the effects of diethylenetriaminepentaacetate (DTPA) chelation treatment are presented. Active mechanisms to transport plutonium to and from the lymph system appear to exist. Equations for buildup in the lymph nodes and organs are included. The data suggest a buildup in the lymph node to a maximum, followed by a long negative slope, and a possible dose-rate effect from Pu(NO 3 ) 4 in lymph nodes

239Pu contamination in snakes inhabiting the Rocky Flats Plant site

International Nuclear Information System (INIS)

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 239 Pu and, if so, at what concentrations. Eastern yellow-bellied racers (Coluber constrictor flaviventris, bullsnakes (Pituophis melanoleucus sayi, and prairie rattlesnakes (Crotalus viridis viridis, were collected for 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 239 Pu

Qualitative and quantitative analysis of plutonium in solid waste drums

International Nuclear Information System (INIS)

Anno, Jacques; Escarieux, Emile

1977-01-01

An assessment of the results given by a study carried out for the development of qualitative and quantitative analysis, by γ spectrometry, of plutonium in solid waste drums is presented. After having reminded the standards and their incidence on the quantities of plutonium to be measured (application at industrial Pu: 20% of Pu 240 ) the equipment used is described. Measurement station provided with a mechanical system consisting of: a rail and a pulley block to bring the drums; a pit and a hydraulic jack with a rotating platform. The detection instrumentation consisting of: a high volume coaxial Ge(Li) detector with a γ ray resolution of 2 keV; an associated electronic; a processing of data by a 'Plurimat 20' minicomputer. Principles of the identification and measurements are specified and supported by experimental results. They are the following: determination of the quality of Pu by measuring the ratio between the γ ray intensities of the 239 Pu 129 keV and of the 241 Pu 148 keV; measurement of the 239 Pu mass by estimating the γ ray counting rate of the 375 keV from the calibrating curves given by plutonium samples varying from 32 mg to 80 g; correction of the results versus the source position into the drum and versus the filling in plastic materials into this drum. The experimental results obtained over 40 solid waste drums are presented along with the error estimates [fr

Some investigations into the behaviour of plutonium in the marine environment

International Nuclear Information System (INIS)

Hetherington, J.A.; Jefferies, D.F.; Lovett, M.B.

1975-01-01

Plutonium and other transuranic elements are produced during the operation of magnox reactors, although they do not usually present any problems of waste management until the fuel reaches the reprocessing stage. At this stage one of the chief aims is to separate and recover the plutonium from the depleted uranium and the fission products, the incentive being the value of plutonium itself as a nuclear fuel particularly for the fast breeder reactors. For this reason the amounts of plutonium appearing in the low activity waste streams for discharge to the environment are usually small, and their radiological impact insignificant compared with that of the more abundant fission products. However, with the prospect of use of large quantities of plutonium in the fast reactors, considerable interest surrounds all aspects of the properties of plutonium, and in an attempt to give a fuller understanding of the behaviour of plutonium in the marine environment use has been made of the small amounts which have been discharged in recent years to the north-east Irish Sea from the fuel reprocessing plant at Windscale in Cumbria. Details of the amounts of 239 Pu and 240 Pu discharged to sea are given and the resultant measured concentrations of the isotopes in the water throughout the Irish Sea are shown. The distribution of plutonium in sea water is shown to follow the same basic pattern as the fission products, details of which have been reported previously. By comparing the concentration gradients with distance from the point of discharge for plutonium and caesium, a value for the rate of loss of plutonium from the water to the other important compartment, namely the sediment, has been deduced. Measurements have been made of 239 Pu and 240 Pu in seabed and estuarine sediments and by combining these with the water data values of the concentration factor for the nuclide in sediment have been calculated. The results of a number of core samples have been used to calculate an

Review of thermal expansion and density of uranium and plutonium carbides

International Nuclear Information System (INIS)

Andrew, J.F.; Latimer, T.W.

1975-07-01

The published literature on linear thermal expansion and density of uranium and plutonium carbide nuclear fuels, including UC, PuC, (U,Pu)C, U 2 C 3 , Pu 2 C 3 , and (U,Pu) 2 C 3 , is critically reviewed. Recommended values are given in tabular form and additional experimental studies needed for completeness are outlined. 16 tables, 52 references

Assembly-level analysis of heterogeneous Th–Pu PWR fuel

International Nuclear Information System (INIS)

Zainuddin, Nurjuanis Zara; Parks, Geoffrey T.; Shwageraus, Eugene

2017-01-01

Highlights: • We directly compare homogeneous and heterogeneous Th–Pu fuel. • Examine whether there is an increase in Pu incineration in the latter. • Homogeneous fuel was able to achieve much higher Pu incineration. • In the heterogeneous case, U-233 breeding is faster (larger power fraction), thus decreasing incineration of Pu. - Abstract: This study compares homogeneous and heterogeneous thorium–plutonium (Th–Pu) fuel assemblies (with high Pu content – 20 wt%), and examines whether there is an increase in Pu incineration in the latter. A seed-blanket configuration based on the Radkowsky thorium reactor concept is used for the heterogeneous assembly. This separates the thorium blanket from the uranium seed, or in this case a plutonium seed. The seed supplies neutrons to the subcritical thorium blanket which encourages the in situ breeding and burning of "2"3"3U, allowing the fuel to stay critical for longer, extending burnup of the fuel. While past work on Th–Pu seed-blanket units shows superior Pu incineration compared to conventional U–Pu mixed oxide fuel, there is no literature to date that directly compares the performance of homogeneous and heterogeneous Th–Pu assembly configurations. Use of exactly the same fuel loading for both configurations allows the effects of spatial separation to be fully understood. It was found that the homogeneous fuel with and without burnable poisons was able to achieve much higher Pu incinerations than the heterogeneous fuel configurations, while still attaining a reasonably high discharge burnup. This is because in the heterogeneous cases, "2"3"3U breeding is faster, thereby contributing to a much larger fraction of total power produced by the assembly. In contrast, "2"3"3U build-up is slower in the homogeneous case and therefore Pu burning is greater. This "2"3"3U begins to contribute a significant fraction of power produced only towards the end of life, thus extending criticality, allowing more Pu to

Plutonium peroxide precipitation: review and current research

International Nuclear Information System (INIS)

Hagan, P.G.; Miner, F.J.

1980-01-01

Increasing the HNO 3 concentration decreases the filtration time but increases the plutonium concentration in the filtrate. A compromise was therefore necessary. If a minimum plutonium concentration is required in the filtrate, the acidity could be lowered to 1.9M with an approximate doubling in the filtration time. The H 2 O 2 concentration has little effect on filtration time. However, the higher the H 2 O 2 concentration, the less plutonium lost to the filtrate. Concentrations higher than the 22 moles/mole Pu recommended (at least up to 30 molar which was the highest investigated) would be beneficial if reagent costs are not excessive and production capacity exists for destroying the excess H 2 O 2 in the filtrate. Although the effect is not large, filtration time is shorter and the plutonium concentration in the filtrate is lower if metallic impurities are present. The slowest rate of H 2 O 2 addition investigated gives a plutonium peroxide precipitate with the fastest filtration time. The rate of addition has very little effect on the plutonium concentration in the filtrate. The temperature has little effect on the filtration time. 14 0 C is recommended since decomposition of H 2 O 2 would be slower at 14 0 C than at 22 0 C (min. Pu content in the filtrate). The effect of digestion time on both the filtration time and the plutonium content in the filtrate is minor, so the shortest digestion time investigated is recommended

Implications of plutonium and americium recycling on MOX fuel fabrication

International Nuclear Information System (INIS)

Renard, A.; Pilate, S.; Maldague, Th.; La Fuente, A.; Evrard, G.

1995-01-01

The impact of the multiple recycling of plutonium in power reactors on the radiation dose rates is analyzed for the most critical stage in a MOX fuel fabrication plant. The limitation of the number of Pu recycling in light water reactors would rather stem from reactor core physics features. The case of recovering americium with plutonium is also considered and the necessary additions of shielding are evaluated. A comparison between the recycling of Pu in fast reactors and in light water reactors is presented. (author)

MEANS FOR PRODUCING PLUTONIUM CHAIN REACTIONS

Science.gov (United States)

Wigner, E.P.; Weinberg, A.M.

1961-01-24

A neutronic reactor is described with an active portion capable of operating at an energy level of 0.5 to 1000 ev comprising discrete bodies of Pu/ sup 239/ disposed in a body of water which contains not more than 5 molecules of water to one atom of plutonium, the total amount of Pu/sup 239/ being sufficient to sustain a chain reaction. (auth)

Solubilization of plutonium hydrous oxide by iron-reducing bacteria

International Nuclear Information System (INIS)

Rusin, P.A.; Quintana, L.; Brainard, J.R.; Strietelmeler, B.A.; Tait, C.D.; Ekberg, S.A.; Palmer, P.D.; Newton, T.W.; Clark, D.L.

1994-01-01

The removal of plutonium from soils id challenging because of its strong sorption to soils and limited solubility, Microbial reduction of metals is known to affect the speciation and solubility of sparingly soluble metals in the environment, notably iron and manganese. The similarity in reduction potential for α-FeOOH(s) and hydrous PuO 2 (s) suggests that iron-reducing bacteria may also reduce and solubilize plutonium. Bacillus strains were used to demonstrate that iron-reducing bacteria mediate the solubilization of hydrous PuO 2 (s) under anaerobic conditions. Up to ∼90% of the PuO 2 was biosolubilized in the presence of nitrilotriacetic acid (NTA) within 6-7 days. Biosolubilization occurred to a lesser extent (∼ 40%) in the absence of NTA. Little PuO 2 solubilization occurred in sterile culture media or in the presence of a non-iron-reducing Escherichia coli. These observations suggest a potentially attractive, environmentally benign strategy for the remediation of Pu-contaminated soils. 26 refs., 5 figs., 2 tabs

Thermodynamics properties of plutonium in NaCl-KCl and CaCl{sub 2} at 1073 K and in liquid gallium

Energy Technology Data Exchange (ETDEWEB)

Lambertin, D.; Ched' homme, S.; Bourges, G.; Pescayre, L.; Sanchez, S.; Picard, G

2004-07-01

Cadmium and bismuth metal are mostly used as solvent in nuclear pyrochemical processes and especially in actinides/lanthanides separations. Gallium metal has been chosen because no literature values are available with plutonium and its regeneration by refining at low temperature is possible. Electrochemical window of gallium metal and activity coefficient of plutonium in gallium have been determined by using potentiometric method. Secondly, the electrochemical properties of plutonium have been studied in molten equimolar NaCl/KCl and CaCl{sub 2} at 1073 K by cyclic voltammetry. The standard potentials of Pu(III)/Pu redox couple, respectively, -2,54 V and -2,51 V, led to the calculation of the activity coefficients of Pu(III). In CaCl{sub 2} the complexation of Pu(III) ions is lower and the voltage gap between Pu(III)/Pu couple and the solvent limit is higher. The new data on plutonium electrochemistry in molten chlorides and liquid gallium media combined with literature data on lanthanides suggest that gallium can be a good solvent metal for pyro-chemistry separation. (authors)

Studies and manufacture of plutonium fuel

International Nuclear Information System (INIS)

Bussy, P.; Mustelier, J.P.; Pascard, R.

1964-01-01

The studies carried out at the C.E.A. on the properties of fast neutron reactor fuels, the manufacture of fuel elements and their behaviour under irradiation are broadly outlined. The metal fuels studied are the ternary alloys U Pu Mo, U Pu Nb, U Pa Ti, U Pa Zr, the ceramic fuels being mixed uranium and plutonium oxides, carbides and nitrides obtained by sintering. Results are given on the manufacture of uranium fuel elements containing a small proportion of plutonium, used in a critical experiment, and on the first experiments in the manufacture of fuel elements for the reactor Rapsodie. Finally the results of irradiation tests carried out on the prototype fuel pins for Rapsodie are described. (authors) [fr

PLUTONIUM SOLUBILITY IN HIGH-LEVEL WASTE ALKALI BOROSILICATE GLASS

Energy Technology Data Exchange (ETDEWEB)

Marra, J.; Crawford, C.; Fox, K.; Bibler, N.

2011-01-04

The solubility of plutonium in a Sludge Batch 6 (SB6) reference glass and the effect of incorporation of Pu in the glass on specific glass properties were evaluated. A Pu loading of 1 wt % in glass was studied. Prior to actual plutonium glass testing, surrogate testing (using Hf as a surrogate for Pu) was conducted to evaluate the homogeneity of significant quantities of Hf (Pu) in the glass, determine the most appropriate methods to evaluate homogeneity for Pu glass testing, and to evaluate the impact of Hf loading in the glass on select glass properties. Surrogate testing was conducted using Hf to represent between 0 and 1 wt % Pu in glass on an equivalent molar basis. A Pu loading of 1 wt % in glass translated to {approx}18 kg Pu per Defense Waste Processing Facility (DWPF) canister, or about 10X the current allowed limit per the Waste Acceptance Product Specifications (2500 g/m{sup 3} of glass or about 1700 g/canister) and about 30X the current allowable concentration based on the fissile material concentration limit referenced in the Yucca Mountain Project License Application (897 g/m{sup 3}3 of glass or about 600 g Pu/canister). Based on historical process throughput data, this level was considered to represent a reasonable upper bound for Pu loading based on the ability to provide Pu containing feed to the DWPF. The task elements included evaluating the distribution of Pu in the glass (e.g. homogeneity), evaluating crystallization within the glass, evaluating select glass properties (with surrogates), and evaluating durability using the Product Consistency Test -- Method A (PCT-A). The behavior of Pu in the melter was evaluated using paper studies and corresponding analyses of DWPF melter pour samples.The results of the testing indicated that at 1 wt % Pu in the glass, the Pu was homogeneously distributed and did not result in any formation of plutonium-containing crystalline phases as long as the glass was prepared under 'well-mixed' conditions

Plutonium Solubility In High-Level Waste Alkali Borosilicate Glass

International Nuclear Information System (INIS)

Marra, J.; Crawford, C.; Fox, K.; Bibler, N.

2011-01-01

The solubility of plutonium in a Sludge Batch 6 (SB6) reference glass and the effect of incorporation of Pu in the glass on specific glass properties were evaluated. A Pu loading of 1 wt % in glass was studied. Prior to actual plutonium glass testing, surrogate testing (using Hf as a surrogate for Pu) was conducted to evaluate the homogeneity of significant quantities of Hf (Pu) in the glass, determine the most appropriate methods to evaluate homogeneity for Pu glass testing, and to evaluate the impact of Hf loading in the glass on select glass properties. Surrogate testing was conducted using Hf to represent between 0 and 1 wt % Pu in glass on an equivalent molar basis. A Pu loading of 1 wt % in glass translated to ∼18 kg Pu per Defense Waste Processing Facility (DWPF) canister, or about 10X the current allowed limit per the Waste Acceptance Product Specifications (2500 g/m 3 of glass or about 1700 g/canister) and about 30X the current allowable concentration based on the fissile material concentration limit referenced in the Yucca Mountain Project License Application (897 g/m 3 3 of glass or about 600 g Pu/canister). Based on historical process throughput data, this level was considered to represent a reasonable upper bound for Pu loading based on the ability to provide Pu containing feed to the DWPF. The task elements included evaluating the distribution of Pu in the glass (e.g. homogeneity), evaluating crystallization within the glass, evaluating select glass properties (with surrogates), and evaluating durability using the Product Consistency Test -- Method A (PCT-A). The behavior of Pu in the melter was evaluated using paper studies and corresponding analyses of DWPF melter pour samples.The results of the testing indicated that at 1 wt % Pu in the glass, the Pu was homogeneously distributed and did not result in any formation of plutonium-containing crystalline phases as long as the glass was prepared under 'well-mixed' conditions. The incorporation of 1 wt

Global plutonium management: A security option

International Nuclear Information System (INIS)

Sylvester, K.W.B.

1998-01-01

The US surplus plutonium disposition program was created to reduce the proliferation risk posed by the fissile material from thousands of retired nuclear weapons. The Department of Energy has decided to process its Put into a form as secure as Pu in civilian spent fuel. While implementation issues have been considered, a major one (Russian reciprocity) remains unresolved. Russia has made disposition action conditional on extracting the fuel value of its Pu but lacks the infrastructure to do so. Assistance in the construction of the required facilities would conflict with official US policy opposing the development of a Pu fuel cycle. The resulting stagnation provides impetus for a reevaluation of US nonproliferation objectives and Pu disposition options. A strategy for satisfying Russian fuel value concerns and reducing the proliferation risk posed by surplus weapons-grade plutonium (WGPu) is proposed. The effectiveness of material alteration (e.g., isotopic, chemical, etc.hor-ellipsis) at reducing the desire, ability and opportunity for proliferation is assessed. Virtually all the security benefits attainable by material processing can be obtained by immobilizing Pu in large unit size/mass monoliths without a radiation barrier. Russia would be allowed to extract the Pu at a future date for use as fuel in a verifiable manner. Remote tracking capability, if proven feasible, would further improve safeguarding capability. As an alternate approach, the US could compensate Russia for its Pu, allowing it to be disposed of or processed elsewhere. A market based method for pricing Pu is proposed. Surplus Pu could represent access to nuclear fuel at a fixed price at a future date. This position can be replicated in the uranium market and priced using derivative theory. The proposed strategy attempts to meet nonproliferation objectives by recognizing technical limitations and satisfying political constraints

Process for plutonium rextraction in aqueous solution from an organic solvent, especially for uranium plutonium partition

International Nuclear Information System (INIS)

Germain, M.; Gillet, B.; Pasquiou, J.Y.

1989-01-01

The organic solvent containing plutonium is contacted with an aqueous solution of a uranous salt, for instance uranous nitrate, and a hydroxylamine salt, for instance the nitrate. In these conditions uranous nitrate is a reducing agent of Pu III and hydroxylamine nitrate stabilizes Pu III and U IV in the aqueous phase. Performances are similar to these of the U IV-hydrazine nitrate without interference of hydrazine nitrate degradation products [fr

Preparation of plutonium hexafluoride. Recovery of plutonium from waste dross (1962); Preparation de l'hexafluorure de plutonium. Recuperation du plutonium des scories d'elaboration (1962)

Energy Technology Data Exchange (ETDEWEB)

Gendre, R [Commissariat a l' Energie Atomique, Saclay (France). Centre d' Etudes Nucleaires

1962-07-01

The object of this work is to study the influence of various physical factors on the rate of fluorination of solid plutonium tetrafluoride by fluorine. In a horizontal oven with a circulation for pure fluorine at atmospheric pressure and 520 deg. C, at a fluorine rate of 9 litres/hour, it is possible to transform 3 g of tetrafluoride to hexafluoride with about 100 per cent transformation and a recovery yield of over 90 per cent, in 4 to 5 hours. The fluorination rate is a function of the temperature, of the fluorine flow-rate, of the crucible surface, of the depth of the tetrafluoride layer and of the reaction time. It does not depend on the diffusion of the fluorine into the solid but is determined by the reaction at the gas-solid interface and obeys the kinetic law (1 - T{sub T}){sup 1/3} = kt + 1. The existence of intermediate fluorides, in particular Pu{sub 4} F{sub 17}, is confirmed by a break in the Arrhenius plot at about 370 deg. C, by differences in the fluorination rates inside the tetrafluoride layer, and by reversible colour changes. The transformation to hexafluoride occurs with a purification with respect of the foreign elements present in the initial plutonium. Recovery of plutonium from waste dross: The study is based on the transformation of occluded plutonium particles to gaseous hexafluoride which is then decomposed thermally to the tetrafluoride which can be reintroduced directly in the production circuit. Under the conditions considered this process is not applicable industrially. After milling, it is possible to separate the dross into enriched (75 per cent Pu in 2.6 per cent by weight of dross) and depleted portions. By prolonged fluorination (16 hours) of the various fractions it is possible to recover about 80 per cent of the plutonium. A treatment plant using fluidization, as described at the end of this study, should make it possible to substantially improve the yield. (author) [French] L'objet de l'etude est l'influence des differents

ZZ WPPR-FR-MOX/BNCMK, Benchmark on Pu Burner Fast Reactor

International Nuclear Information System (INIS)

Garnier, J.C.; Ikegami, T.

1993-01-01

Description of program or function: In order to intercompare the characteristics of the different reactors considered for Pu recycling, in terms of neutron economy, minor actinide production, uranium content versus Pu burning, the NSC Working Party on Physics of Plutonium Recycling (WPPR) is setting up several benchmark studies. They cover in particular the case of the evolution of the Pu quality and Pu fissile content for Pu recycling in PWRs; the void coefficient in PWRs partly fuelled with MOX versus Pu content; the physics characteristics of non-standard fast reactors with breeding ratios around 0.5. The following benchmarks are considered here: - Fast reactors: Pu Burner MOX fuel, Pu Burner metal fuel; - PWRs: MOX recycling (bad quality Pu), Multiple MOX recycling

Corrosion tests with uranium- and plutonium-loaded ceramic waste forms

International Nuclear Information System (INIS)

Morss, L. R.; Johnson, S. G.; Ebert, W. L.; DiSanto, T.; Frank, S. M.; Holly, J. L.; Kropf, A. J.; Mertz, C. J.; O'Holleran, T. P.; Richmann, M. K.; Sinkler, W.; Tsai, Y.; Warren, A. R.; Noy, M.

2003-01-01

Tests were conducted with ceramic waste form (CWF) materials that contained small amounts of uranium and plutonium to study their release behavior as the CWF corroded. Materials made using the hot isostatic press (HIP) and pressureless consolidation (PC) methods were examined and tested. Four different materials were made using the HIP method with two salts having different U:Pu mole ratios and two zeolite reagents having different residual water contents. Tests with the four HIP U,Pu-loaded CWF materials were conducted at 90 and 120 C, at CWF-to-water mass ratios of 1:10 and 1:20, and for durations between 7 and 365 days. Materials made using two PC processing conditions were also tested. Tests with the two PC U,Pu-loaded CWF materials were conducted at 90 and 120 C, at a CWF-to-water mass ratio of 1:10, and for durations between 7 and 182 days. The releases of matrix elements, U, and Pu in tests conducted under different test conditions and with different materials are compared to evaluate the effects of composition and processing conditions on the release behavior of U and Pu and the chemical durabilities of the different materials. The distributions of released elements among the fractions that were dissolved, in colloidal form in the solution, and fixed to test vessel walls were measured and compared. Characterization of Pu-bearing colloidal particles recovered from the test solutions using solids analysis techniques are also reported. The principal findings from this study are: (1) The release of U and Pu is about 10X less than the release of Si and 50X less than the release of B under all test conditions. This implies that U and Pu are in a phase that is less soluble than the sodalite and binder glass matrix. (2) Almost all of the plutonium that is released from U,Pu-loaded CWF is present either as colloidal-sized particles in the size range between 5 and 100 nm in the test solution (about 15% of the total) or becomes fixed on stainless steel test vessel

Mechanical resuspension of 239Pu from unpaved roads

International Nuclear Information System (INIS)

Hodgin, C.R.

1982-01-01

The impacts of resuspended plutonium from two unpaved roads at the Rocky Flats Plant on nearby air samplers were investigated. Because the sources were complex fugitive dust emitters and because of the small source-receptor distances, traditional dispersion modeling techniques could not be employed. Thus two specialized techniques, one for fugitive dust emissions and one for near distance dispersion, were developed and used to calculate atmospheric dust concentrations at the subject air samplers. Atmospheric 239 Pu impacts were then determined from measurements of plutonium concentrations in the resuspendible dust on the road surfaces. As a final step in the process the calculated plutonium impacts were compared to the 1980 annual average 239 Pu concentration at four samplers. The impact calculated for the Gunnery Range Road represented 2.1 percent of the observed annual concentration, with a 95 percent confidence interval of 1.1 to 7.9 percent. The Southeast Perimeter Road produced a more substantial effect with a point estimate of 3.8 percent. The 95 percent confidence interval for this source was 2.0 to 9.1 percent. The combined impact of the two roads on the subject samplers was 5.9 percent of the observed plutonium concentration, with a 95 percent confidence interval of 3.2 to 17.0 percent. Thus it was shown that fugitive plutonium emissions from the Gunnery Range Road and Southeast Perimeter Road are not substantial contributors to the plutonium concentrations observed at the subject samplers. Even an increase in dust control efficiency to 90 percent (as with paving) would result in only a four percent decrease in the overall atmosperic plutonium concentration at the site

Repository and deep borehole disposition of plutonium