Neutronics Benchmarks for the Utilization of Mixed-Oxide Fuel: Joint U.S./Russian Progress Report for Fiscal Year 1997

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

Akkurt, H

2001-01-11

In 1967, a series of critical experiments were conducted at the Westinghouse Reactor Evaluation Center (WREC) using mixed-oxide (MOX) PuO{sub 2}-UO{sub 2} and/or UO{sub 2} fuels in various lattices and configurations . These experiments were performed under the joint sponsorship of the Empire State Atomic Development Associates (ESADA) plutonium program and Westinghouse . The purpose of these experiments was to develop experimental data to validate analytical methods used in the design of a plutonium-bearing replacement fuel for water reactors. Three different fuels were used during the experimental program: two MOX fuels and a low-enriched UO{sub 2} fuel. The MOX fuelsmore » were distinguished by their {sup 240}Pu content: 8 wt% {sup 240}Pu and 24 wt% {sup 240}Pu. Both MOX fuels contained 2.0 wt % PuO{sub 2} in natural UO{sub 2} . The UO{sub 2} fuel with 2.72 wt % enrichment was used for comparison with the plutonium data and for use in multiregion experiments.« less

Plutonium isotopes in the Hungarian environment.

PubMed

Varga, Beata; Tarján, Sandor; Vajda, Nora

2008-04-01

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

Heterogeneity Effects in Plutonium Contaminated Soil

DTIC Science & Technology

2009-03-01

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

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

PubMed

Thakur, P; Ballard, S; Nelson, R

2012-05-01

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

Tritium and plutonium in waters from the Bering and Chukchi Seas

USGS Publications Warehouse

Landa, E.R.; Beals, D.M.; Halverson, J.E.; Michel, R.L.; Cefus, G.R.

1999-01-01

During the summer of 1993, seawater in the Bering and Chukchi Seas was sampled on a joint Russian-American cruise [BERPAC] of the RV Okean to determine concentrations of tritium, 239Pu and 240Pu. Concentrations of tritium were determined by electrolytic enrichment and liquid scintilation counting. Tritium levels ranged up to 420 mBq L-1 showed no evidence of inputs other than those attribute atmospheric nuclear weapons testing. Plutonium was recovered from water samples by ferric hydroxide precipitation, and concentrations were determined by thermal ionization mass spectrometry. 239+240Pu concentrations ranged from <1 to 5.5 [mu]Bq L-1. These concentrations are lower than those measured in water samples from other parts of the ocean during the mid-1960's to the late 1980's. The 240Pu:239Pu ratios, although associated with large uncertainties, suggest that most of the plutonium is derived from world-wide fallout. As points of comparison, the highest concentrations of tritium and plutonium observed here were about five orders of magnitude lower than the maximum permissible concentrations allowed in water released to the off-site environs from licensed nuclear facilities in the United States. This study and others sponsored by the International Atomic Energy Agency and the Office of Naval Research's Arctic Nuclear Waste Assessment Program are providing data for the assessment of potential radiological impacts in the Arctic regions associated with nuclear waste disposal by the former Soviet Union.

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

PubMed

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

2008-04-01

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

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

PubMed

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

2008-10-01

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

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

PubMed

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

2017-07-15

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

Sources of plutonium in the atmosphere and stratosphere-troposphere mixing

PubMed Central

Hirose, Katsumi; Povinec, Pavel P.

2015-01-01

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

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

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

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

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

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

PubMed

Shabana, E I; Al-Shammari, H L

2001-01-01

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

The instrumental method of plutonium determination

NASA Astrophysics Data System (ADS)

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

2003-01-01

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

Characterization and source term assessments of radioactive particles from Marshall Islands using non-destructive analytical techniques

NASA Astrophysics Data System (ADS)

Jernström, J.; Eriksson, M.; Simon, R.; Tamborini, G.; Bildstein, O.; Marquez, R. Carlos; Kehl, S. R.; Hamilton, T. F.; Ranebo, Y.; Betti, M.

2006-08-01

Six plutonium-containing particles stemming from Runit Island soil (Marshall Islands) were characterized by non-destructive analytical and microanalytical methods. Composition and elemental distribution in the particles were studied with synchrotron radiation based micro X-ray fluorescence spectrometry. Scanning electron microscope equipped with energy dispersive X-ray detector and with wavelength dispersive system as well as a secondary ion mass spectrometer were used to examine particle surfaces. Based on the elemental composition the particles were divided into two groups: particles with pure Pu matrix, and particles where the plutonium is included in Si/O-rich matrix being more heterogenously distributed. All of the particles were identified as nuclear fuel fragments of exploded weapon components. As containing plutonium with low 240Pu/ 239Pu atomic ratio, less than 0.065, which corresponds to weapons-grade plutonium or a detonation with low fission yield, the particles were identified to originate from the safety test and low-yield tests conducted in the history of Runit Island. The Si/O-rich particles contained traces of 137Cs ( 239 + 240 Pu/ 137Cs activity ratio higher than 2500), which indicated that a minor fission process occurred during the explosion. The average 241Am/ 239Pu atomic ratio in the six particles was 3.7 × 10 - 3 ± 0.2 × 10 - 3 (February 2006), which indicated that plutonium in the different particles had similar age.

Plutonium-239 + 240 and Americium-241 in soils east of Rocky Flats, Colorado

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

Litaor, M.I.; Barth, G.R.; Molzer, P.C.

1994-11-01

Soils east of the Rocky Flats (RF) near Golden, CO, were contaminated with Pu-239 + 240 and Am-241 as a result of past waste-storage practices. The physiocochemical parameters that govern the actinides distribution in the soil are poorly understood. Twenty-six soil pits at various distances and directions from a contaminated site at RF were excavated, sampled, and analyzed for actinide activities as well as selected physical, chemical, and mineralogical attributes. Plutonium-239+240 and Am-241 activities in the soils ranged form 164 280 Bq/kg to 0.0037 Bq/kg, decreasing with distance from the source. More than 90% of the Pu-239 + 240 andmore » Am-241 activities were confined to the upper 12 cm of the soil, regardless of the soil characteristics, or distance and direction from the source. Evidence of preferential transport in macropores formed along decayed root channels was observed in four soil pits and had translocated Pu-239 + 240 to a depth of 90 cm. This transport mechanism increased by a factor of 30 the level of Pu-239 + 240 activity at this depth. Earthworm activity is probably important in the redistribution of actinides in the upper 40 cm of many of the soils investigated. Planning of future remedial activities at RF should consider the findings of this contaminant-transport study. 34 refs., 5 figs., 2 tabs.« less

Distribution and migration of 239+240Pu in abiotic components of the Black Sea ecosystems during the post-Chernobyl period.

PubMed

Tereshchenko, N N; Gulin, S B; Proskurnin, V Yu

2018-08-01

Distribution of 239,240 Pu in abiotic components (water and bottom sediment) of the Black Sea ecosystems was studied during the post-Chernobyl period at different offshore and near-shore locations. The trends of these radionuclides accumulation by sediments were analyzed. The spatial-temporal changes in the 239,240 Pu distribution as well as effective half-life for these radionuclides in the Black Sea surface water in deep-sea area are presented. The estimations of the average annual removal fluxes of the 239,240 Pu into the bottom sediments were obtained. The Black Sea sediments were characterized by a higher 239,240 Pu concentration factor (C f  ≈ n·10 4 -n·10 6 ) and radiocapacity factor (F( 239,240 Pu) was about 99.9% on the shelf, 94.5-99.1% on deep-sea basin for silty and 94.6-98.9% on the shelf for sandy bottom sediments) as compared with C f and F for 137 Cs and 90 Sr. Silty bottom sediments play the role of 239,240 Pu main depot in the Black Sea ecosystem. The studied radioecological characteristics of Pu allowed us to define the type of plutonium biogeochemical behavior in the Black Sea as a pedotropic one. The results of this complex radioecological monitoring of 239+240 Pu contamination in the Black Sea and their analysis makes it possible to understand the plutonium redistribution pathways which will enable to carry out the tracing of its migration within the ecosystems. Copyright © 2017 Elsevier Ltd. All rights reserved.

On the presence of plutonium in Madagascar following the SNAP-9A satellite failure.

PubMed

Rääf, C; Holm, E; Rabesiranana, N; Garcia-Tenorio, R; Chamizo, E

2017-10-01

This study examined the 238 Pu and 239+240 Pu activity concentration and the 240 Pu/ 239 Pu atomic ratio in peat bogs sampled in 2012 from marshlands in central Madagascar. The purpose was to investigate the presence of plutonium isotopes, 238, 239, 240 Pu, from the 1964 satellite failure carrying a SNAP-9A radiothermal generator. With an average 238 Pu/ 239+240 Pu activity ratio of 0.165 ± 0.02 (decay corrected to 1964), the peat bogs in Madagascar exhibit similar values as the ones found in the southeastern African continent, except they are one order of magnitude higher than expected (0.025) from global fallout in the Southern Hemisphere. The 240 Pu/ 239 Pu atomic ratio showed a distinct decrease for layers dating back to the mid-1960s (down to 0.069 compared with an anticipated ratio of 0.17 for global fallout), indicating that the SNAP-9A failure also resulted in an elevated deposition of 239 Pu. The obtained results demonstrate that further Pu analysis in Madagascar and in southeastern continental Africa is necessary to fully account for the regional Pu deposition from the SNAP-9A event. Copyright © 2017 Elsevier Ltd. All rights reserved.

The uptake of plutonium-238, 239, 240, americium-241, strontium-90 and caesium-137 into potatoes.

PubMed

Popplewell, D S; Ham, G J; Johnson, T E; Stather, J W; Sumner, S A

1984-09-01

Transfer factors have been measured for 239 Pu + 240 Pu, 241 Am, 90 Sr and 137 Cs into potatoes grown in a blend of soil which included silt polluted with radioactive waste discharged into the Irish Sea. The experiment has been carried out over four seasons and attempts to assess the radiological consequences to the consumer which would arise if potatoes were to be grown in land heavily contaminated with the silt. During the course of the experiment plutonium and americium became less available for uptake, 90 Sr became slightly more available and 137 Cs remained nearly constant in its availability. The values of the transfer factors are among the lowest reported for these radionuclides into potatoes.

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

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

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

2002-01-01

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

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

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

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

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

Plutonium age dating reloaded

NASA Astrophysics Data System (ADS)

Sturm, Monika; Richter, Stephan; Aregbe, Yetunde; Wellum, Roger; Mayer, Klaus; Prohaska, Thomas

2014-05-01

Although the age determination of plutonium is and has been a pillar of nuclear forensic investigations for many years, additional research in the field of plutonium age dating is still needed and leads to new insights as the present work shows: Plutonium is commonly dated with the help of the 241Pu/241Am chronometer using gamma spectrometry; in fewer cases the 240Pu/236U chronometer has been used. The age dating results of the 239Pu/235U chronometer and the 238Pu/234U chronometer are scarcely applied in addition to the 240Pu/236U chronometer, although their results can be obtained simultaneously from the same mass spectrometric experiments as the age dating result of latter. The reliability of the result can be tested when the results of different chronometers are compared. The 242Pu/238U chronometer is normally not evaluated at all due to its sensitivity to contamination with natural uranium. This apparent 'weakness' that renders the age dating results of the 242Pu/238U chronometer almost useless for nuclear forensic investigations, however turns out to be an advantage looked at from another perspective: the 242Pu/238U chronometer can be utilized as an indicator for uranium contamination of plutonium samples and even help to identify the nature of this contamination. To illustrate this the age dating results of all four Pu/U clocks mentioned above are discussed for one plutonium sample (NBS 946) that shows no signs of uranium contamination and for three additional plutonium samples. In case the 242Pu/238U chronometer results in an older 'age' than the other Pu/U chronometers, contamination with either a small amount of enriched or with natural or depleted uranium is for example possible. If the age dating result of the 239Pu/235U chronometer is also influenced the nature of the contamination can be identified; enriched uranium is in this latter case a likely cause for the missmatch of the age dating results of the Pu/U chronometers.

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

PubMed

Todd, Andrew S; Sattelberg, R Mark

2005-11-01

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

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

PubMed

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

1999-09-30

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

Source and long-term behavior of transuranic aerosols in the WIPP environment.

PubMed

Thakur, P; Lemons, B G

2016-10-01

Source and long-term behavior transuranic aerosols ((239+240)Pu, (238)Pu, and (241)Am) in the ambient air samples collected at and near the Waste Isolation Pilot Plant (WIPP) deep geologic repository site were investigated using historical data from an independent monitoring program conducted by the Carlsbad Environmental Monitoring and Research Center and an oversight monitoring program conducted by the management and operating contractor for WIPP at and near the facility. An analysis of historical data indicates frequent detections of (239+240)Pu and (241)Am, whereas (238)Pu is detected infrequently. Peaks in (239+240)Pu and (241)Am concentrations in ambient air generally occur from March to June timeframe, which is when strong and gusty winds in the area frequently give rise to blowing dust. Long-term measurements of plutonium isotopes (1985-2015) in the WIPP environment suggest that the resuspension of previously contaminated soils is likely the primary source of plutonium in the ambient air samples from WIPP and its vicinity. There is no evidence that WIPP is a source of environmental contamination that can be considered significant by any health-based standard.

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

PubMed

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

2010-09-01

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

PRESSURIZED WATER REACTOR CORE WITH PLUTONIUM BURNUP

DOEpatents

Puechl, K.H.

1963-09-24

A pressurized water reactor is described having a core containing Pu/sup 240/ in which the effective microscopic neutronabsorption cross section of Pu/sup 240/ in unconverted condition decreases as the time of operation of the reactor increases, in order to compensate for loss of reactivity resulting from fission product buildup during reactor operation. This means serves to improve the efficiency of the reactor operation by reducing power losses resulting from control rods and burnable poisons. (AEC)

High-Precision Plutonium Isotopic Compositions Measured on Los Alamos National Laboratory’s General’s Tanks Samples: Bearing on Model Ages, Reactor Modelling, and Sources of Material. Further Discussion of Chronometry

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

Spencer, Khalil J.; Rim, Jung Ho; Porterfield, Donivan R.

2015-06-29

In this study, we re-analyzed late-1940’s, Manhattan Project era Plutonium-rich sludge samples recovered from the ''General’s Tanks'' located within the nation’s oldest Plutonium processing facility, Technical Area 21. These samples were initially characterized by lower accuracy, and lower precision mass spectrometric techniques. We report here information that was previously not discernable: the two tanks contain isotopically distinct Pu not only for the major (i.e., 240Pu, 239Pu) but trace ( 238Pu , 241Pu, 242Pu) isotopes. Revised isotopics slightly changed the calculated 241Am- 241Pu model ages and interpretations.

Plutonium and americium in the foodchain lichen-reindeer-man

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

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

1977-01-01

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

Twenty-four years of follow-up for a Hanford plutonium wound case.

PubMed

Carbaugh, Eugene H; Lynch, Timothy P; Antonio, Cheryl L; Medina-Del Valle, Fernando

2010-10-01

A 1985 plutonium puncture wound resulted in the initial deposition of 48 kBq of transuranic alpha activity, primarily 239+240Pu and 241Am, in a worker's right index finger. Surgical excisions in the week following reduced the long-term residual wound activity to 5.4 kBq, and 164 DTPA chelation therapy administrations over 17 mo resulted in urinary excretion of about 7 kBq. The case was published in 1988, but now 24 y of follow-up data are available. Annual bioassays have included in-vivo measurements of 241Am in the wound, skeleton, liver, lung, and axillary lymph nodes, and urinalyses for plutonium and 241Am. These measurements have shown relatively stable levels of 241Am at the wound site, with gradually increasing amounts of 241Am detected in the skeleton. Liver measurements have shown erratic detection of 241Am, and the lung measurements indicate Am but as interference from activity in the axillary lymph nodes and skeleton rather than activity in the lung. Urine excretion of Pu since termination of chelation therapy has typically ranged from 10 to 20 mBq d, with Am excretion about 10% of that for 239+240Pu. Annual routine medical exams have not identified any adverse health effects associated with the intake.

AMS of the Minor Plutonium Isotopes

NASA Astrophysics Data System (ADS)

Steier, P.; Hrnecek, E.; Priller, A.; Quinto, F.; Srncik, M.; Wallner, A.; Wallner, G.; Winkler, S.

2013-01-01

VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure 239Pu, 240Pu, 241Pu, 242Pu and 244Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of 244Pu/239Pu = (5.7 ± 1.0) × 10-5 based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the 242Pu/240Pu ratio as an estimate of the initial 241Pu/239Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method.

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.

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

Lell, R. M.; Morman, J. A.; Schaefer, R.W.

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,more » 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 component to construct a central core zone with a composition closer to that in an LMFBR core with high burnup. The high {sup 240}Pu configuration was constructed for two reasons. First, the composition of the high {sup 240}Pu zone more closely matched the composition of LMFBR cores anticipated in design work in 1970. Second, comparison of measurements in the ZPR-6/7 uniform core with corresponding measurements in the high {sup 240}Pu zone provided an assessment of some of the effects of long-term {sup 240}Pu buildup in LMFBR cores. The uniform core version of ZPR-6/7 is evaluated in ZPR-LMFR-EXP-001. This document only addresses measurements in the high {sup 240}Pu core version of ZPR-6/7. Many types of measurements were performed as part of the ZPR-6/7 program. Measurements of criticality, sodium void worth, control rod worth and reaction rate distributions in the high {sup 240}Pu core configuration are evaluated here. For each category of measurements, the uncertainties are evaluated, and benchmark model data are provided.« less

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

USGS Publications Warehouse

Knobel, LeRoy L.; Mann, Larry J.

1988-01-01

Sampling for radionuclides in groundwater was conducted at the Idaho National Engineering Laboratory during September to November 5 1987. Water samples from 80 wells that obtain water from the Snake River Plain aquifer and 1 well that obtains water from a shallow, discontinuous perched-water body at the Radioactive Waste Management Complex were collected and analyzed for tritium, strontium-90, plutonium-238, plutonium-239, -240 (undivided), americium-241, cesium-137, cobalt-60, and potassium-40--a naturally occurring radionuclide. The groundwater samples were analyzed at the Idaho National Engineering Laboratory in Idaho. Tritium and strontium-90 concentrations ranged from below the reporting level to 80.6 +/-0.000005 and 193 +/-5x10 to the minus eight micrograms Ci/ml, respectively. Water from a disposal well at Test Area North--which has not been used to dispose of waste water since September 1972--contained 122 +/-9x10 to the minus eleven micrograms Ci/ml of plutonium-238, 500 +/-20x10 to the minus eleven of plutonium-239, -240 (undivided), 21 +/-4x10 to the minus eleven micrograms Ci/ml of americium-241, and 750 +/-20x10 to the minus eight micrograms Ci/ml cesium-137; the presence of these radionuclides was verified by resampling and reanalysis. The disposal well had 8.9 +/-0.0000009 micrograms Ci/ml of cobalt-60 on October 28, 1987, but cobalt-60 was not detected when the well was resampled on January 11, 1988. Potassium-40 concentrations were less than the reporting level in all wells. (USGS)

Sedimentary record of plutonium in the North Yellow Sea and the response to catchment environmental changes of inflow rivers.

PubMed

Xu, Yihong; Pan, Shaoming; Gao, Jianhua; Hou, Xiaolin; Ma, Yongfu; Hao, Yongpei

2018-09-01

Plutonium (Pu) isotopes were first determined in surface and core sediment samples collected from the northern North Yellow Sea (NYS) to elucidate their source terms and deposition process as well as the response to catchment environmental changes of inflow rivers. 240 Pu/ 239 Pu atom ratios in all sediments showed the typical global fallout value of ∼0.18 without any influences from the nuclear weapons tests conducted recently in the North Korea or early in the Pacific Proving Ground. The large variation of 239+240 Pu activities (0.022-0.515 mBq/g) observed in surface sediments should be mainly attributed to the re-suspension and transportation of fine sediments influenced by the Liaonan Costal Current. Based on the two 239+249 Pu depth profiles with easily observed onset fallout levels (1952) and global fallout peaks (1963), 239+240 Pu served as a valid time mark in the coastal sedimentary system. Riverine input Pu contributed only 15-27% to the total global fallout inventory (92.5-108.8 Bq/m 2 ) in the northern NYS, much lower than that in the Yangtze River estuary (77-80%), indicating a better soil conservation in the northeast China due to higher forest coverage compared to the Yangtze River's drainage basin. The increase of riverine input Pu after 1980s reflected the more intense soil erosion degree caused by the land use and cover change due to the increment of human activities in the northeast China at the same period. Our results demonstrated that plutonium is a good indicator for studying sedimentary process and its response to the environment in the coastal area. Copyright © 2018 Elsevier Ltd. All rights reserved.

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

PubMed

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

2018-05-04

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

Fabrication of 12% {sup 240}Pu calorimetry standards

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

Long, S.M.; Hildner, S.; Gutierrez, D.

1995-08-01

Throughout the DOE complex, laboratories are performing calorimetric assays on items containing high burnup plutonium. These materials contain higher isotopic range and higher wattages than materials previously encountered in vault holdings. Currently, measurement control standards have been limited to utilizing 6% {sup 240}Pu standards. The lower isotopic and wattage value standards do not complement the measurement of the higher burnup material. Participants of the Calorimetry Exchange (CALEX) Program have identified the need for new calorimetric assay standards with a higher wattage and isotopic range. This paper describes the fabrication and verification measurements of the new CALEX standard containing 12% {supmore » 240}Pu oxide with a wattage of about 6 to 8 watts.« less

Baseline Caesium-137 and Plutonium-239+240 inventory assessment for Central Europe

NASA Astrophysics Data System (ADS)

Meusburger, Katrin; Borelli, Pasquale; Evrard, Olivier; Ketterer, Michael; Mabit, Lionel; van Oost, Kristof; Alewell, Christine; Panagos, Panos

2017-04-01

Artificial fallout radionuclides (FRNs) such as Caesium-137 and Plutonium-239+240 released as products of the thermonuclear weapons testing that took place from the mid-1950s to the early 1980s and from nuclear power plant accidents (e.g. Chernobyl) are useful tools to quantify soil redistribution. In combination with geostatistics, FRNs may have the potential to bridge the gap between small scale process oriented studies and modelling that simplifies processes and effects over large spatial scales. An essential requirement for the application of FRNs as soil erosion tracers is the establishment of the baseline fallout at undisturbed sites before its comparison to those inventories found at sites undergoing erosion/accumulation. For this purpose, undisturbed topsoil (0-20cm) samples collected in 2009 within the framework of the Land Use/Cover Area frame Survey (LUCAS) have been measured by gamma-spectrometry and ICP-MS to determine 137Cs (n=145) and 239+240Pu (n=108) activities. To restrict the analysis to undisturbed reference sites a geospatial database query selecting only sites having a slope angle <2 degree, outside riparian zones (to avoid depositional sites) and under permanent grassland cover (according to CORINE Land Cover and Landsat) was applied. This study reports preliminary results on the feasibility of establishing a 137Cs and 239+240Pu baseline inventory map for Central Europe. The 137Cs/239+240Pu activity ratios will further allow assessing the rate and the spatial variability of 137Cs Chernobyl fallout. The establishment of such baseline inventory map will provide a unique opportunity to assess soil redistribution for a comparable time-frame (1953-2009) following a harmonised methodological protocol across national boundaries.

Determination of origin and intended use of plutonium metal using nuclear forensic techniques.

PubMed

Rim, Jung H; Kuhn, Kevin J; Tandon, Lav; Xu, Ning; Porterfield, Donivan R; Worley, Christopher G; Thomas, Mariam R; Spencer, Khalil J; Stanley, Floyd E; Lujan, Elmer J; Garduno, Katherine; Trellue, Holly R

2017-04-01

Nuclear forensics techniques, including micro-XRF, gamma spectrometry, trace elemental analysis and isotopic/chronometric characterization were used to interrogate two, potentially related plutonium metal foils. These samples were submitted for analysis with only limited production information, and a comprehensive suite of forensic analyses were performed. Resulting analytical data was paired with available reactor model and historical information to provide insight into the materials' properties, origins, and likely intended uses. Both were super-grade plutonium, containing less than 3% 240 Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modeling feedback and trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. Based on this investigation, the most likely intended use for these plutonium foils was 239 Pu fission foil targets for physics experiments, such as cross-section measurements, etc. Copyright © 2017 Elsevier B.V. All rights reserved.

Determination of origin and intended use of plutonium metal using nuclear forensic techniques

DOE PAGES

Rim, Jung H.; Kuhn, Kevin J.; Tandon, Lav; ...

2017-04-01

Nuclear forensics techniques, including micro-XRF, gamma spectrometry, trace elemental analysis and isotopic/chronometric characterization were used to interrogate two, potentially related plutonium metal foils. These samples were submitted for analysis with only limited production information, and a comprehensive suite of forensic analyses were performed. Resulting analytical data was paired with available reactor model and historical information to provide insight into the materials’ properties, origins, and likely intended uses. Both were super-grade plutonium, containing less than 3% 240Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modelling feedback andmore » trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. In conclusion, based on this investigation, the most likely intended use for these plutonium foils was 239Pu fission foil targets for physics experiments, such as cross-section measurements, etc.« less

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

PubMed

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

2009-05-01

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

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

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

Steve Hoeffner

2003-12-31

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

Concentrations of plutonium and americium in plankton from the western Mediterranean Sea.

PubMed

Sanchez-Cabeza, Joan-Albert; Merino, Juan; Masqué, Pere; Mitchell, Peter I; Vintró, L León; Schell, William R; Cross, Lluïsa; Calbet, Albert

2003-07-20

Understanding the transfer of radionuclides through the food chain leading to man and in particular, the uptake of transuranic nuclides by plankton, is basic to assess the potential radiological risk of the consumption of marine products by man. The main sources of transuranic elements in the Mediterranean Sea in the past were global fallout and the Palomares accident, although at present smaller amounts are released from nuclear establishments in the northwestern region. Plankton from the western Mediterranean Sea was collected and analyzed for plutonium and americium in order to study their biological uptake. The microplankton fractions accounted for approximately 50% of the total plutonium contents in particulate form. At Garrucha (Palomares area), microplankton showed much higher 239,240 Pu activity, indicating the contamination with plutonium from the bottom sediments. Concentration factors were within the range of the values recommended by the International Atomic Energy Agency. Continental shelf mesoplankton was observed to efficiently concentrate transuranics. In open seawaters, concentrations were much lower. We speculate that sediments might play a role in the transfer of transuranics to mesoplankton in coastal waters, although we cannot discard that the difference in species composition may also play a role. In Palomares, both 239,240 Pu and 241Am showed activities five times higher than the mean values observed in continental shelf mesoplankton. As the plutonium isotopic ratios in the contaminated sample were similar to those found in material related to the accident, the contamination was attributed to bomb debris from the Palomares accident. Concentration factors in mesoplankton were also in relatively good agreement with the ranges recommended by IAEA. In the Palomares station the highest concentration factor was observed in the sample that showed predominance of the dynoflagellate Ceratium spp. Mean values of the enrichment factors showed, on average, discrimination rather than enrichment in the primary producer trophic chain.

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

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

Conant, Andrew; Erickson, Anna; Robel, Martin

Nuclear forensics has a broad task to characterize recovered nuclear or radiological material and interpret the results of investigation. One approach to isotopic characterization of nuclear material obtained from a reactor is to chemically separate and perform isotopic measurements on the sample and verify the results with modeling of the sample history, for example, operation of a nuclear reactor. The major actinide plutonium and fission product cesium are commonly measured signatures of the fuel history in a reactor core. This study investigates the uncertainty of the plutonium and cesium isotope ratios of a fuel rod discharged from a research pressurizedmore » water reactor when the location of the sample is not known a priori. A sensitivity analysis showed overpredicted values for the 240Pu/ 239Pu ratio toward the axial center of the rod and revealed a lower probability of the rod of interest (ROI) being on the periphery of the assembly. The uncertainty analysis found the relative errors due to only the rod position and boron concentration to be 17% to 36% and 7% to 15% for the 240Pu/ 239Pu and 137Cs/ 135Cs ratios, respectively. Lastly, this study provides a method for uncertainty quantification of isotope concentrations due to the location of the ROI. Similar analyses can be performed to verify future chemical and isotopic analyses.« less

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

DOE PAGES

Conant, Andrew; Erickson, Anna; Robel, Martin; ...

2017-02-03

Nuclear forensics has a broad task to characterize recovered nuclear or radiological material and interpret the results of investigation. One approach to isotopic characterization of nuclear material obtained from a reactor is to chemically separate and perform isotopic measurements on the sample and verify the results with modeling of the sample history, for example, operation of a nuclear reactor. The major actinide plutonium and fission product cesium are commonly measured signatures of the fuel history in a reactor core. This study investigates the uncertainty of the plutonium and cesium isotope ratios of a fuel rod discharged from a research pressurizedmore » water reactor when the location of the sample is not known a priori. A sensitivity analysis showed overpredicted values for the 240Pu/ 239Pu ratio toward the axial center of the rod and revealed a lower probability of the rod of interest (ROI) being on the periphery of the assembly. The uncertainty analysis found the relative errors due to only the rod position and boron concentration to be 17% to 36% and 7% to 15% for the 240Pu/ 239Pu and 137Cs/ 135Cs ratios, respectively. Lastly, this study provides a method for uncertainty quantification of isotope concentrations due to the location of the ROI. Similar analyses can be performed to verify future chemical and isotopic analyses.« less

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

PubMed

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

2006-02-01

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

Plutonium as a tracer for soil erosion assessment in northeast China.

PubMed

Xu, Yihong; Qiao, Jixin; Pan, Shaoming; Hou, Xiaolin; Roos, Per; Cao, Liguo

2015-04-01

Soil erosion is one of the most serious environmental and agricultural problems faced by human society. Assessing intensity is an important issue for controlling soil erosion and improving eco-environmental quality. The suitability of the application of plutonium (Pu) as a tracer for soil erosion assessment in northeast China was investigated by comparing with that of 137Cs. Here we build on preliminary work, in which we investigated the potential of Pu as a soil erosion tracer by sampling additional reference sites and potential erosive sites, along the Liaodong Bay region in northeast China, for Pu isotopes and 137Cs. 240Pu/239Pu atomic ratios in all samples were approximately 0.18, which indicated that the dominant source of Pu was the global fallout. Pu showed very similar distribution patterns to those of 137Cs at both uncultivated and cultivated sites. 239+240Pu concentrations in all uncultivated soil cores followed an exponential decline with soil depth, whereas at cultivated sites, Pu was homogenously distributed in plow horizons. Factors such as planted crop types, as well as methods and frequencies of irrigation and tillage were suggested to influence the distribution of radionuclides in cultivated land. The baseline inventories of 239+240Pu and 137Cs were 88.4 and 1688 Bq m(-2) respectively. Soil erosion rates estimated by 239+240Pu tracing method were consistent with those obtained by the 137Cs method, confirming that Pu is an effective tracer with a similar tracing behavior to that of 137Cs for soil erosion assessment. Copyright © 2014 Elsevier B.V. All rights reserved.

Historical Development of the U.S. Geological Survey Hydrologic Monitoring and Investigative Programs at the Idaho National Engineering and Environmental Laboratory, Idaho, 1949 to 2001

DTIC Science & Technology

2005-01-01

Cesium- 137 , Cobalt-60, and Chromium-51 ………………………………………… 12 Plutonium-238, Plutonium-239, -240 (undivided), and Americium-241 ……………… 12 Iodine-129...1992) presented water-level data from the ESRPA collected from 1983 through 1990 from 137 wells. At the end of 2000, water levels in 203 aquifer and...Cesium- 137 , Cobalt-60, and Chromium-51 The USGS has routinely monitored ground water at the INEEL for gamma radiation since 1962. Gamma

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

Rim, Jung H.; Kuhn, Kevin J.; Tandon, Lav

Nuclear forensics techniques, including micro-XRF, gamma spectrometry, trace elemental analysis and isotopic/chronometric characterization were used to interrogate two, potentially related plutonium metal foils. These samples were submitted for analysis with only limited production information, and a comprehensive suite of forensic analyses were performed. Resulting analytical data was paired with available reactor model and historical information to provide insight into the materials’ properties, origins, and likely intended uses. Both were super-grade plutonium, containing less than 3% 240Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modelling feedback andmore » trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. In conclusion, based on this investigation, the most likely intended use for these plutonium foils was 239Pu fission foil targets for physics experiments, such as cross-section measurements, etc.« less

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

PubMed

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

2017-11-01

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

The efficacy of denaturing actinide elements as a means of decreasing materials attractiveness

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

Hase, K.R.; Bathke, C.G.; Ebbinghaus, B.B.

2013-07-01

This study considers the concept of denaturing as applied to the actinide elements present in spent fuel as a means to reduce materials attractiveness. Highly attractive materials generally have low values of bare critical mass, heat content, and dose. To denature an attractive element, its spent-fuel isotopic composition (isotopic vector) is intentionally modified by introducing sufficient quantities of a significantly less attractive isotope to dilute the concentration of a highly attractive isotope so that the overall attractiveness of the element is reduced. The authors used FOM (Figure of Merit) formula as the material attractiveness metric for their parametric determination ofmore » the attractiveness of the Pu and U. Materials attractiveness needs to be considered in three distinct phases in the process to construct a nuclear explosive device (NED): the acquisition phase, processing phase, and utilization phase. The results show that denaturing uranium with {sup 238}U is actually an effective means of reducing the attractiveness. For uranium with a large minority of {sup 235}U, a mixture of 80% {sup 238}U to 20% {sup 235}U is required to reduce the attractiveness to low. For uranium with a large concentration of {sup 233}U, a mixture of 88% {sup 238}U to 12% {sup 233}U is required to reduce the attractiveness to low. The results also show that denaturing plutonium with {sup 238}Pu is less effective than denaturing uranium with {sup 238}U. Using {sup 238}Pu as the denaturing agent would require 80% or more by mass in order to reduce the attractiveness to low. No amount of {sup 240}Pu is enough to reduce the plutonium attractiveness below medium. The combination of {sup 238}Pu and {sup 240}Pu would require approximately 70% {sup 238}Pu and 25% {sup 240}Pu by mass to reduce the plutonium attractiveness to low.« less

Ultra-trace determination of plutonium in marine samples using multi-collector inductively coupled plasma mass spectrometry.

PubMed

Lindahl, Patric; Keith-Roach, Miranda; Worsfold, Paul; Choi, Min-Seok; Shin, Hyung-Seon; Lee, Sang-Hoon

2010-06-25

Sources of plutonium isotopes to the marine environment are well defined, both spatially and temporally, which makes Pu a potential tracer for oceanic processes. This paper presents the selection, optimisation and validation of a sample preparation method for the ultra-trace determination of Pu isotopes ((240)Pu and (239)Pu) in marine samples by multi-collector (MC) ICP-MS. The method was optimised for the removal of the interference from (238)U and the chemical recovery of Pu. Comparison of various separation strategies using AG1-X8, TEVA, TRU, and UTEVA resins to determine Pu in marine calcium carbonate samples is reported. A combination of anion-exchange (AG1-X8) and extraction chromatography (UTEVA/TRU) was the most suitable, with a radiochemical Pu yield of 87+/-5% and a U decontamination factor of 1.2 x 10(4). Validation of the method was accomplished by determining Pu in various IAEA certified marine reference materials. The estimated MC-ICP-MS instrumental limit of detection for (239)Pu and (240)Pu was 0.02 fg mL(-1), with an absolute limit of quantification of 0.11 fg. The proposed method allows the determination of ultra-trace Pu, at femtogram levels, in small size marine samples (e.g., 0.6-2.0 g coral or 15-20 L seawater). Finally, the analytical method was applied to determining historical records of the Pu signature in coral samples from the tropical Northwest Pacific and (239+240)Pu concentrations and (240)Pu/(239)Pu atom ratios in seawater samples as part of the 2008 GEOTRACES intercalibration exercise. Copyright 2010 Elsevier B.V. All rights reserved.

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

PubMed

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

2013-10-01

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

Determination of (236)U and transuranium elements in depleted uranium ammunition by alpha-spectrometry and ICP-MS.

PubMed

Desideri, D; Meli, M A; Roselli, C; Testa, C; Boulyga, S F; Becker, J S

2002-11-01

It is well known that ammunition containing depleted uranium (DU) was used by NATO during the Balkan conflict. To evaluate the origin of DU (the enrichment of natural uranium or the reprocessing of spent nuclear fuel) it is necessary to directly detect the presence of activation products ((236)U, (239)Pu, (240)Pu, (241)Am, and (237)Np) in the ammunition. In this work the analysis of actinides by alpha-spectrometry was compared with that by inductively coupled plasma mass spectrometry (ICP-MS) after selective separation of ultratraces of transuranium elements from the uranium matrix. (242)Pu and (243)Am were added to calculate the chemical yield. Plutonium was separated from uranium by extraction chromatography, using tri- n-octylamine (TNOA), with a decontamination factor higher than 10(6); after elution plutonium was determined by ICP-MS ((239)Pu and (240)Pu) and alpha-spectrometry ((239+240)Pu) after electroplating. The concentration of Pu in two DU penetrator samples was 7 x 10(-12) g g(-1) and 2 x 10(-11) g g(-1). The (240)Pu/(239)Pu isotope ratio in one penetrator sample (0.12+/-0.04) was significantly lower than the (240)Pu/(239)Pu ratios found in two soil samples from Kosovo (0.35+/-0.10 and 0.27+/-0.07). (241)Am was separated by extraction chromatography, using di(2-ethylhexyl)phosphoric acid (HDEHP), with a decontamination factor as high as 10(7). The concentration of (241)Am in the penetrator samples was 2.7 x 10(-14) g g(-1) and <9.4 x 10(-15) g g(-1). In addition (237)Np was detected at ultratrace levels. In general, ICP-MS and alpha-spectrometry results were in good agreement. The presence of anthropogenic radionuclides ((236)U, (239)Pu,(240)Pu, (241)Am, and (237)Np) in the penetrators indicates that at least part of the uranium originated from the reprocessing of nuclear fuel. Because the concentrations of radionuclides are very low, their radiotoxicological effect is negligible.

Sources and accumulation of plutonium in a large Western Pacific marginal sea: The South China Sea.

PubMed

Wu, Junwen; Dai, Minhan; Xu, Yi; Zheng, Jian

2018-01-01

In order to examine the sources of plutonium (Pu) and elaborate its scavenging and accumulation processes, 240 Pu/ 239 Pu atom ratios and 239+240 Pu activities in the water column of the South China Sea (SCS) were determined and compared with our previously reported data for the sediments. Consistently high 240 Pu/ 239 Pu atom ratios that ranged from 0.184-0.250 (average=0.228±0.015), indicative of non-global fallout Pu sources were observed both in the surface water and at depth during 2012-2014. The spatial distribution of the 240 Pu/ 239 Pu atom ratio in the SCS showed a decreasing trend away from the Luzon Strait, which was very consistent with the introduction pathway of the Kuroshio Current. The Kuroshio had an even heavier Pu isotopic ratio ranging from 0.250-0.263 (average=0.255±0.006), traceable to the non-global fallout Pu signature from the Pacific Proving Grounds (PPG). Using a simple two end-member mixing model, we further revealed that this PPG source contributed 41±17% of the Pu in the SCS water column. The 239+240 Pu activities in the SCS surface seawater varied from 1.59 to 2.94mBqm -3 , with an average of 2.34±0.38mBqm -3 . Such an activity level was ~40% higher than that in the Kuroshio. The distribution of 239+240 Pu in the surface seawater further showed a general trend of increase from the Kuroshio to the SCS basin, suggesting significant accumulation of Pu within the SCS. The 239+240 Pu inventory of the water column in the SCS basin at the SEATS station with a total depth of ~3840m was estimated to be ~29Bqm -2 , which was substantially higher than the sediment core estimates made for the SCS basin (3.75Bqm -2 ) but much lower than the sediment core estimates made for the shelf of the northern SCS (365.6Bqm -2 ). Such differences were determined by the lower scavenging efficiency of Pu in the SCS basin compared to the northern SCS shelf. Copyright © 2017 Elsevier B.V. All rights reserved.

Determination of Low Level Alpha and Beta Emitters Using Liquid-Liquid Extraction and a Liquid Scintillation Spectrometer

NASA Astrophysics Data System (ADS)

Yu, Yu-Fu; BjØRnstad, H. E.; Salbu, B.

Two radiochemical procedures for determination of low level strontium-90 and plutonium-239+240 in environmental and biological materials using combined selective solvent extraction with low level liquid scintillation counting have been presented. Y-90, the daughter nuclide of Sr-90, and Pu-239+240 are selectively extracted from nitric acid solution into 5% di(-2ethylhexyl)phosphoric acid (HDEHP) in toluene and the radionuclides of interest in organic phase are counted with an ultra low level scintillation counter "Quantulus". The lower detection limits for Sr-90 and Pu-239+240 are estimated to be 20 mBq and 0.3 mBq respectively. The developed procedures have been tested for soma environmental and biological samples and the preminarly results show that they are more simple and time-saving than traditional methods.

Age determination of single plutonium particles after chemical separation

NASA Astrophysics Data System (ADS)

Shinonaga, T.; Donohue, D.; Ciurapinski, A.; Klose, D.

2009-01-01

Age determination of single plutonium particles was demonstrated using five particles of the standard reference material, NBS 947 (Plutonium Isotopic Standard. National Bureau of Standards, Washington, D.C. 20234, August 19, 1982, currently distributed as NBL CRM-137) and the radioactive decay of 241Pu into 241Am. The elemental ratio of Am/Pu in Pu particles found on a carbon planchet was measured by wavelength dispersive X-ray spectrometry (WDX) coupled to a scanning electron microscope (SEM). After the WDX measurement, each plutonium particle, with an average size of a few μm, was picked up and relocated to a silicon wafer inside the SEM chamber using a micromanipulator. The silicon wafer was then transferred to a quartz tube for dissolution in an acid solution prior to chemical separation. After the Pu was chemically separated from Am and U, the isotopic ratios of Pu ( 240Pu/ 239Pu, 241Pu/ 239Pu and 242Pu/ 239Pu) were measured with a thermal ionization mass spectrometer (TIMS) for the calculation of Pu age. The age of particles determined in this study was in good agreement with the expected age (35.9 a) of NBS 947 within the measurement uncertainty.

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

PubMed

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.

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

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

Cantrell, Kirk J.

2009-08-20

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

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

USGS Publications Warehouse

Bartholomay, Roy C.; L. Flint Hall,

2016-05-05

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

Distribution of neptunium and plutonium in New Mexico lichen samples ( Usnea arizonica) contaminated by atmospheric fallout

DOE PAGES

Oldham, Jr., Warren J.; Hanson, Susan K.; Lavelle, Kevin B.; ...

2015-08-30

In this study, the concentrations of 237Np, 239Pu and 240Pu were determined in lichen samples ( Usnea arizonica) that were collected from ten locations in New Mexico between 2011 and 2013 using isotope dilution inductively-coupled plasma mass spectrometry (ID-ICP-MS). The observed isotopic ratios for 237Np/ 239Pu and 240Pu/ 239Pu indicate trace contamination from global and regional fallout (e.g. Trinity test and atmospheric testing at the Nevada Test Site). The fact that actinide contamination is detected in recent lichen collections suggests continuous re-suspension of fallout radionuclides even 50 years after ratification of the Limited Test Ban Treaty.

Ustur whole body case 0269: demonstrating effectiveness of i.v. CA-DTPA for Pu.

PubMed

James, A C; Sasser, L B; Stuit, D B; Glover, S E; Carbaugh, E H

2007-01-01

This whole body donation case (USTUR Registrant) involved a single acute inhalation of an acidic Pu(NO3)4 solution in the form of an aerosol 'mist'. Chelation treatment with intravenously (i.v.) Ca-EDTA was initiated on the day of the intake, and continued intermittently over 6 months. After 2.5 y with no further treatment, a course of i.v. Ca-DTPA was administered. A total of 400 measurements of 239+240Pu excreted in urine were recorded; starting on the first day (both before and during the initial Ca-EDTA chelation) and continuing for 37 y. This sampling included all intervals of chelation. In addition, 91 measurements of 239+240Pu-in-feces were recorded over this whole period. The Registrant died about 38 y after the intake, at age 79 y, with extensive carcinomatosis secondary to adenocarcinoma of the prostate gland. At autopsy, all major soft tissue organs were harvested for radiochemical analyses of their 238Pu, 239+240Pu and 241Am content. Also, all types of bone (comprising about half the skeleton) were harvested for radiochemical analyses, as well as samples of skin, subcutaneous fat and muscle. This comprehensive data set has been applied to derive 'chelation-enhanced' transfer rates in the ICRP Publication 67 plutonium biokinetic model, representing the behaviour of blood-borne and tissue-incorporated plutonium during intervals of therapy. The resulting model of the separate effects of i.v. Ca-EDTA and Ca-DTPA chelation shows that the therapy administered in this case succeeded in reducing substantially the long-term burden of plutonium in all body organs, except for the lungs. The calculated reductions in organ content at the time of death are approximately 40% for the liver, 60% for other soft tissues (muscle, skin, glands, etc.), 50% for the kidneys and 50% for the skeleton. Essentially, all of the substantial reduction in skeletal burden occurred in trabecular bone. This modelling exercise demonstrated that 3-y-delayed Ca-DTPA therapy was as effective as promptly administered Ca-EDTA.

USTUR WHOLE BODY CASE 0269: DEMONSTRATING EFFECTIVENESS OF I.V. CA-DTPA FOR PU

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

James, Anthony C.; Sasser , Lyle B.; Stuit, Dorothy B.

2008-01-28

This whole body donation case (USTUR Registrant) involved a single acute inhalation of an acidic Pu(NO3)4 solution in the form of an aerosol ‘mist.’ Chelation treatment with i.v. Ca-EDTA was initiated on the day of the intake, and continued intermittently over 6 months. After 2½ years with no further treatment, a course of i.v. Ca-DTPA was administered. A total of 400 measurements of 239+240Pu excreted in urine were recorded; starting on the first day (both before and during the initial Ca-EDTA chelation), and continuing for 37 years. This sampling included all intervals of chelation. In addition, 91 measurements of 239+240Pu-in-fecesmore » were recorded over this whole period. The Registrant died about 38 years after the intake, at age 79 y, with extensive carcinomatosis secondary to adenocarcinoma of the prostate gland. At autopsy, all major soft tissue organs were harvested for radiochemical analyses of their 238Pu, 239+240Pu and 241Am content. Also, all types of bone (comprising about half the skeleton) were harvested for radiochemical analyses, as well as samples of skin, subcutaneous fat and muscle. This comprehensive dataset has been applied to derive ‘chelation-enhanced’ transfer rates in the ICRP Publication 67 plutonium biokinetic model, representing the behaviour of blood-borne and tissue-incorporated plutonium during intervals of therapy. The resulting model of the separate effects of i.v. Ca-EDTA and Ca-DTPA chelation shows that the therapy administered in this case succeeded in reducing substantially the long-term burden of plutonium in all body organs, except for the lungs. The calculated reductions in organ content at the time of death are approximately 40% for the liver, 60% for other soft tissues (muscle, skin, glands, etc.), 50% for the kidneys, and 50% for the skeleton. Essentially all of the substantial reduction in skeletal burden occurred in trabecular bone. This modeling exercise demonstrated that 3-y-delayed Ca-DTPA therapy was as effective as promptly administered Ca-EDTA.« less

Radiation Detection and Classification of Heavy Oxide Inorganic Scintillator Crystals for Detection of Fast Neutrons

DTIC Science & Technology

2016-06-01

of these three pillars, yet current detectors for fast neutrons from nuclear weapons materials are bulky, expensive, and have low efficiencies, well...passive fast neutron emissions. Similarly, isotopes present in weapons grade Plutonium (which is predominantly Pu-239), especially Pu-240, are... weapons material, and the propensity of the neutrons resulting from their fission to inelastically scatter, defines the interactions of interest

ANALYSIS AND EXAMINATION OF MOX FUEL FROM NONPROLIFERATION PROGRAMS

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

McCoy, Kevin; Machut, Dr McLean; Morris, Robert Noel

The U.S. Department of Energy has decided to dispose of a portion of the nation s surplus plutonium by reconstituting it into mixed oxide (MOX) fuel and irradiating it in commercial power reactors. Four lead assemblies were manufactured and irradiated to a maximum fuel rod burnup of 47.3 MWd/kg heavy metal. This was the first commercial irradiation of MOX fuel with a 240Pu/239Pu ratio of 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. The performance of the rodsmore » was analyzed with AREVA s next-generation GALILEO code. The results of the analysis confirmed that the fuel rods had performed safely and predictably, and that GALILEO is applicable to MOX fuel with a low 240Pu/239Pu ratio as well as to standard MOX. The results are presented and compared to the GALILEO database. In addition, the fuel cladding was tested to confirm that traces of gallium in the fuel pellets had not affected the mechanical properties of the cladding. The irradiated cladding was found to remain ductile at both room temperature and 350 C for both the axial and circumferential directions.« less

Trench 'bathtubbing' and surface plutonium contamination at a legacy radioactive waste site.

PubMed

Payne, Timothy E; Harrison, Jennifer J; Hughes, Catherine E; Johansen, Mathew P; Thiruvoth, Sangeeth; Wilsher, Kerry L; Cendón, Dioni I; Hankin, Stuart I; Rowling, Brett; Zawadzki, Atun

2013-01-01

Radioactive waste containing a few grams of plutonium (Pu) was disposed between 1960 and 1968 in trenches at the Little Forest Burial Ground (LFBG), near Sydney, Australia. A water sampling point installed in a former trench has enabled the radionuclide content of trench water and the response of the water level to rainfall to be studied. The trench water contains readily measurable Pu activity (~12 Bq/L of (239+240)Pu in 0.45 μm-filtered water), and there is an associated contamination of Pu in surface soils. The highest (239+240)Pu soil activity was 829 Bq/kg in a shallow sample (0-1 cm depth) near the trench sampling point. Away from the trenches, the elevated concentrations of Pu in surface soils extend for tens of meters down-slope. The broader contamination may be partly attributable to dispersion events in the first decade after disposal, after which a layer of soil was added above the trenched area. Since this time, further Pu contamination has occurred near the trench-sampler within this added layer. The water level in the trench-sampler responds quickly to rainfall and intermittently reaches the surface, hence the Pu dispersion is attributed to saturation and overflow of the trenches during extreme rainfall events, referred to as the 'bathtub' effect.

Variants of Regenerated Fissile Materials Usage in Thermal Reactors as the First Stage of Fuel Cycle Closing

NASA Astrophysics Data System (ADS)

Andrianova, E. A.; Tsibul'skiy, V. F.

2017-12-01

At present, 240 000 t of spent nuclear fuel (SF) has been accumulated in the world. Its long-term storage should meet safety conditions and requires noticeable finances, which grow every year. Obviously, this situation cannot exist for a long time; in the end, it will require a final decision. At present, several variants of solution of the problem of SF management are considered. Since most of the operating reactors and those under construction are thermal reactors, it is reasonable to assume that the structure of the nuclear power industry in the near and medium-term future will be unchanged, and it will be necessary to utilize plutonium in thermal reactors. In this study, different strategies of SF management are compared: open fuel cycle with long-term SF storage, closed fuel cycle with MOX fuel usage in thermal reactors and subsequent long-term storage of SF from MOX fuel, and closed fuel cycle in thermal reactors with heterogeneous fuel arrangement. The concept of heterogeneous fuel arrangement is considered in detail. While in the case of traditional fuel it is necessary to reprocess the whole amount of spent fuel, in the case of heterogeneous arrangement, it is possible to separate plutonium and 238U in different fuel rods. In this case, it is possible to achieve nearly complete burning of fissile isotopes of plutonium in fuel rods loaded with plutonium. These fuel rods with burned plutonium can be buried after cooling without reprocessing. They would contain just several percent of initially loaded plutonium, mainly even isotopes. Fuel rods with 238U alone should be reprocessed in the usual way.

A multiple ion counter total evaporation (MICTE) method for precise analysis of plutonium by thermal ionization mass spectrometry

DOE PAGES

Inglis, Jeremy D.; Maassen, Joel; Kara, Azim; ...

2017-04-28

This study presents a total evaporation method for the analysis of sub-picogram quantities of Pu, utilizing an array of multiple ion counters. Data from three standards are presented to assess the utility of the technique. An external precision of 1.5% RSD (2σ) was achieved on aliquots approaching 100 fg for the minor 240Pu isotope. Accurate analysis of <1 femtogram of 240Pu, is achievable, with an external reproducibility of better than 10% RSD (2σ). Finally, this new technique represents a significant advance in the total evaporation method and will allow routine measurement of femtogram sized Pu samples by thermal ionization massmore » spectrometry.« less

Measurement of 240Pu/239Pu isotopic ratios in soils from the Marshall Islands using ICP-MS.

PubMed

Muramatsu, Y; Hamilton, T; Uchida, S; Tagami, K; Yoshida, S; Robison, W

2001-10-20

Nuclear weapons tests conducted by the United States in the Marshall Islands produced significant quantities of regional or tropospheric fallout contamination. Here we report on some preliminary inductively coupled plasma-mass spectrometry (ICP-MS) measurements of plutonium isolated from seven composite soil samples collected from Bikini, Enewetak and Rongelap Atolls in the northern Marshall Islands. These data show that 240Pu/239Pu isotopic signatures in surface soils from the Marshall Island vary significantly and could potentially be used to help quantify the range and extent of fallout deposition (and associated impacts) from specific weapons tests. 137Cs and 60Co were also determined on the same set of soil samples for comparative purposes.

A multiple ion counter total evaporation (MICTE) method for precise analysis of plutonium by thermal ionization mass spectrometry

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

Inglis, Jeremy D.; Maassen, Joel; Kara, Azim

This study presents a total evaporation method for the analysis of sub-picogram quantities of Pu, utilizing an array of multiple ion counters. Data from three standards are presented to assess the utility of the technique. An external precision of 1.5% RSD (2σ) was achieved on aliquots approaching 100 fg for the minor 240Pu isotope. Accurate analysis of <1 femtogram of 240Pu, is achievable, with an external reproducibility of better than 10% RSD (2σ). Finally, this new technique represents a significant advance in the total evaporation method and will allow routine measurement of femtogram sized Pu samples by thermal ionization massmore » spectrometry.« less

Sources of plutonium to the tropical Northwest Pacific Ocean (1943-1999) identified using a natural coral archive

NASA Astrophysics Data System (ADS)

Lindahl, Patric; Asami, Ryuji; Iryu, Yasufumi; Worsfold, Paul; Keith-Roach, Miranda; Choi, Min-Seok

2011-03-01

The Pu isotopes, 239Pu and 240Pu, were determined in annually-banded skeletons of an accurately dated (1943-1999) modern coral ( Porites lobata) from Guam Island to identify historical Pu sources to the tropical Northwest Pacific Ocean. Activity concentrations of 239+240Pu and 240Pu/ 239Pu atom ratios were determined in the dated coral bands using multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). Close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands and global fallout were identified as the two main sources. The Guam site was dominated by PPG close-in fallout in the 1950s, with an average 240Pu/ 239Pu atom ratio of 0.315 ± 0.005. In addition, a higher 240Pu/ 239Pu atom ratio (0.456 ± 0.020) was observed that could be attributed to fallout from the "Ivy Mike" thermonuclear detonation in 1952. The atom ratio decreased in the 1960s and 1970s due to increase in the global fallout with a low 240Pu/ 239Pu atom ratio (˜0.18). Recent coral bands (1981-1999) are dominated by the transport of remobilised Pu, with high 240Pu/ 239Pu atom ratios, from the Marshall Islands to Guam Island along the North Equatorial Current (NEC). This remobilised Pu was estimated to comprise 69% of the total Pu in the recent coral bands, although its contribution was variable over time.

Plutonium Isotopes (239-241Pu) Dissolved in Pacific Ocean Waters Detected by Accelerator Mass Spectrometry: No Effects of the Fukushima Accident Observed.

PubMed

Hain, Karin; Faestermann, Thomas; Fimiani, Leticia; Golser, Robin; Gómez-Guzmán, José Manuel; Korschinek, Gunther; Kortmann, Florian; Lierse von Gostomski, Christoph; Ludwig, Peter; Steier, Peter; Tazoe, Hirofumi; Yamada, Masatoshi

2017-02-21

The concentration of plutonium (Pu) and the isotopic ratios of 240 Pu to 239 Pu and 241 Pu to 239 Pu were determined by accelerator mass spectrometry (AMS) in Pacific Ocean water samples (20 L each) collected in late 2012. The isotopic Pu ratios are important indicators of different contamination sources and were used to identify a possible release of Pu into the ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. In particular, 241 Pu is a well-suited indicator for a recent entry of Pu because 241 Pu from fallout of nuclear weapon testings has already significantly decayed. A total of 10 ocean water samples were prepared at the Radiochemie München of the TUM and analyzed at the Vienna Environmental Research Laboratory (VERA). Several samples showed a slightly elevated 240 Pu/ 239 Pu ratio of up to 0.22 ± 0.02 compared to global fallout ( 240 Pu/ 239 Pu = 0.180 ± 0.007), whereas all measured 241 Pu-to- 239 Pu ratios were consistent with nuclear weapon fallout ( 241 Pu/ 239 Pu < 2.4 × 10 -3 ), which means that no impact from the Fukushima accident was detected. From the average 241 Pu-to- 239 Pu ratio of 8 -2 +3 ×10 -4 at a sampling station located at a distance of 39.6 km to FDNPP, the 1-σ upper limit for the FDNPP contribution to the 239 Pu inventory in the water column was estimated to be 0.2%. Pu, with the signature of weapon-grade Pu was found in a single sample collected around 770 km off the west coast of the United States.

Determination of plutonium and its isotopic ratio in marine sediment samples using quadrupole ICP-MS with the shield torch system under normal plasma conditions.

PubMed

Zheng, Jian; Yamada, Masatoshi; Wang, Zhongliang; Aono, Tatsuo; Kusakabe, Masashi

2004-06-01

An analytical method for determining (239)Pu and (240)Pu in marine sediment samples, which uses quadrupole ICP-MS, was developed in this work. A simple anion-exchange chromatography system was employed for the separation and purification of Pu from the sample matrix. A sufficient decontamination factor of 1.4 x 10(4) for U, which interferes with the determination of (239)Pu, was achieved. High sensitivity Pu determination was obtained, which led to an extremely low concentration detection limit of approximately 8 fg/ml (0.019 mBq/ml for (239)Pu; 0.071 mBq/ml for (240)Pu) in a sample solution, or an absolute detection limit of 42 fg in a 5 ml sample solution, by using the shield torch technique. Analytical results for the determination of the (239+240)Pu and the (240)Pu/(239)Pu ratio in IAEA 368 (ocean sediment) reference material indicated that the accuracy of the method was satisfactory. The method developed was successfully applied to a study of Pu behavior in the sediments from Sagami Bay, Japan. The observed high (240)Pu/(239)Pu ratio in the sediment core indicated that there was additional Pu input derived from close-in fallout in addition to the global fallout.

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

PubMed

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

2009-04-01

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

Excess Lead-210 and Plutonium-239+240: Two suitable radiogenic soil erosion tracers for mountain grassland sites.

PubMed

Meusburger, K; Porto, P; Mabit, L; La Spada, C; Arata, L; Alewell, C

2018-01-01

The expected growing population and challenges associated with globalisation will increase local food and feed demands and enhance the pressure on local and regional upland soil resources. In light of these potential future developments it is necessary to define sustainable land use and tolerable soil loss rates with methods applicable and adapted to mountainous areas. Fallout-radionuclides (FRNs) are proven techniques to increase our knowledge about the status and resilience of agro-ecosystems. However, the use of the Caesium-137 ( 137 Cs) method is complicated in the European Alps due to its heterogeneous input and the timing of the Chernobyl fallout, which occurred during a few single rain events on partly snow covered ground. Other radioisotopic techniques have been proposed to overcome these limitations. The objective of this study is to evaluate the suitability of excess Lead-210 ( 210 Pb ex ) and Plutonium-239+240 ( 239+240 Pu) as soil erosion tracers for three different grassland management types at the steep slopes (slope angles between 35 and 38°) located in the Central Swiss Alps. All three FRNs identified pastures as having the highest mean (± standard deviation) net soil loss of -6.7 ± 1.1, -9.8 ± 6.8 and -7.0 ± 5.2 Mg ha -1 yr -1 for 137 Cs, 210 Pb ex and 239+240 Pu, respectively. A mean soil loss of -5.7 ± 1.5, -5.2 ± 1.5 and-5.6 ± 2.1 was assessed for hayfields and the lowest rates were established for pastures with dwarf-shrubs (-5.2 ± 2.5, -4.5 ± 2.5 and -3.3 ± 2.4 Mg ha -1 yr -1 for 137 Cs, 210 Pb ex and 239+240 Pu, respectively). These rates, evaluated at sites with an elevated soil erosion risk exceed the respective soil production rates. Among the three FRN methods used, 239+240 Pu appears as the most promising tracer in terms of measurement uncertainty and reduced small scale variability (CV of 13%). Despite a higher level of uncertainty, 210 Pb ex produced comparable results, with a wide range of erosion rates sensitive to changes in grassland management. 210 Pb ex can then be as well considered as a suitable soil tracer to investigate alpine agroecosystems. Copyright © 2017 The Authors. Published by Elsevier Inc. All rights reserved.

On the distribution and inventories of radionuclides in dated sediments around the Swedish coast.

PubMed

Olszewski, Grzegorz; Andersson, Pål; Lindahl, Patric; Eriksson, Mats

2018-06-01

The activity concentrations and distribution of 137 Cs, 238 Pu, 239+240 Pu, 241 Am, and 210 Pb was determined by the analysis of six sediment cores from the Baltic Sea and Kattegat. The chronology of the sediment cores has been used to evaluate the origin and time trend of the radionuclide sources in these sediments. The sediment cores were dated with a 210 Pb model and the results were validated with fallout peaks, assumed to originate from the global nuclear weapons testing and the Chernobyl accident. Source identification, using the isotopic and radionuclide activity ratios, showed that the Chernobyl accident is the main source of 137 Cs in the Baltic Sea; for 239+240 Pu and 241 Am the dominant source was shown to be fallout from nuclear weapons tests. For 238 Pu and 241 Am the Chernobyl accident had a significant impact on the direct fallout into the Baltic Proper, with up to a 65% contribution in the sediment slices dated to 1986. In these sediment slices the maximum activity ratios of 238 Pu/ 239+240 Pu and 241 Am/ 239+240 Pu were 0.314 ± 0.008 and 1.29 ± 0.06, respectively. The ratios clearly deviate from the corresponding ratios for global nuclear weapons fallout (around 0.028 and 0.54, respectively). Calculated inventories were 63-175 Bq·m -2 for 239+240 Pu, 2.8-7.8 for 238 Pu Bq·m -2 and 0.92-44.4 kBq·m -2 for 137 Cs. Different fallout patterns for 137 Cs and plutonium isotopes from the Chernobyl accident were confirmed through depth profiles analyses. The maximum inventory of 137 Cs was observed in the Bothnian Sea, while Chernobyl-derived plutonium was found to be mostly present in Northern Baltic Proper. The radionuclides distribution in the depth profiles shows how contaminated water affects the sediment as it passes sampling stations according to the current circulation pattern in the Baltic Sea. Additionally, the effect of increased activity concentrations from of river discharges in the most contaminated area in the Bothnian Sea was observed. Copyright © 2017 Elsevier Ltd. All rights reserved.

Trench ‘Bathtubbing’ and Surface Plutonium Contamination at a Legacy Radioactive Waste Site

PubMed Central

2013-01-01

Radioactive waste containing a few grams of plutonium (Pu) was disposed between 1960 and 1968 in trenches at the Little Forest Burial Ground (LFBG), near Sydney, Australia. A water sampling point installed in a former trench has enabled the radionuclide content of trench water and the response of the water level to rainfall to be studied. The trench water contains readily measurable Pu activity (∼12 Bq/L of 239+240Pu in 0.45 μm-filtered water), and there is an associated contamination of Pu in surface soils. The highest 239+240Pu soil activity was 829 Bq/kg in a shallow sample (0–1 cm depth) near the trench sampling point. Away from the trenches, the elevated concentrations of Pu in surface soils extend for tens of meters down-slope. The broader contamination may be partly attributable to dispersion events in the first decade after disposal, after which a layer of soil was added above the trenched area. Since this time, further Pu contamination has occurred near the trench-sampler within this added layer. The water level in the trench-sampler responds quickly to rainfall and intermittently reaches the surface, hence the Pu dispersion is attributed to saturation and overflow of the trenches during extreme rainfall events, referred to as the ‘bathtub’ effect. PMID:24256473

[Interest and limits of inductively coupled plasma mass spectrometry (ICP-MS) for urinary diagnosis of radionuclide internal contamination].

PubMed

Lecompte, Yannick; Bohand, Sandra; Laroche, Pierre; Cazoulat, Alain

2013-01-01

After a review of radiometric reference methods used in radiotoxicology, analytical performance of inductively coupled plasma mass spectrometry (ICP-MS) for the workplace urinary diagnosis of internal contamination by radionuclides are evaluated. A literature review (covering the period from 2000 to 2012) is performed to identify the different applications of ICP-MS in radiotoxicology for urine analysis. The limits of detection are compared to the recommendations of the International commission on radiological protection (ICRP 78: "Individual monitoring for internal exposure of workers"). Except one publication describing the determination of strontium-90 (β emitter), all methods using ICP-MS reported in the literature concern actinides (α emitters). For radionuclides with a radioactive period higher than 10(4) years, limits of detection are most often in compliance with ICRP publication 78 and frequently lower than radiometric methods. ICP-MS allows the specific determination of plutonium-239 + 240 isotopes which cannot be discriminated by α spectrometry. High resolution ICP-MS can also measure uranium isotopic ratios in urine for total uranium concentrations lower than 20 ng/L. The interest of ICP-MS in radiotoxicology concerns essentially the urinary measurement of long radioactive period actinides, particularly for uranium isotope ratio determination and 239 and 240 plutonium isotopes discrimination. Radiometric methods remain the most efficient for the majority of other radionuclides.

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

PubMed

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

2010-06-01

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

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

USGS Publications Warehouse

Wegner, S.J.

1989-01-01

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

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

PubMed

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

2013-09-01

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

Resolving global versus local/regional Pu sources in the environment using sector ICP-MS

USGS Publications Warehouse

Ketterer, M.E.; Hafer, K.M.; Link, C.L.; Kolwaite, D.; Wilson, Jim; Mietelski, J.W.

2004-01-01

Sector inductively coupled plasma mass spectrometry is a versatile method for the determination of plutonium activities and isotopic compositions in samples containing this element at fallout levels. Typical detection limits for 239+240Pu are 0.1, 0.02 and 0.002 Bq kg -1Pu for samples sizes of 0.5 g, 3 g, and 50 g of soil, respectively. The application of sector ICP-MS-based Pu determinations is demonstrated in studies in sediment chronology, soil Pu inventory and depth distribution, and the provenance of global fallout versus local or regional Pu sources. A sediment core collected from Sloans Lake (Denver, Colorado, USA) exhibits very similar 137Cs and 239+240Pu activity profiles; 240Pu/239Pu atom ratios indicate possible small influences from the Nevada Test Site and/or the Rocky Flats Environmental Technology Site. An undisturbed soil profile from Lockett Meadow (Flagstaff, Arizona, USA) exhibits an exponential decrease in 239+240Pu activity versus depth; 240Pu/239Pu in the top 3 cm is slightly lower than the global fallout range of 0.180 ?? 0.014 due to possible regional influence of Nevada Test Site fallout. The 239??240Pu inventory at Lockett Meadow is 56 ?? 4 Bq m-2, consistent with Northern Hemisphere mid-latitude fallout. Archived NdF3 sources, prepared from Polish soils, demonstrate that substantial 239+240Pu from the 1986 Chernobyl disaster has been deposited in north eastern regions of Poland; compared to global fallout, Chernobyl Pu exhibits higher abundances of 240Pu and 241Pu. The ratios 240Pu/239pu and 241Pu/239Pu co-vary and range from 0.186-0.348 and 0.0029-0.0412, respectively, in forest soils (241Pu/239Pu = 0.2407??[240Pu/239Pu] - 0.0413; r2 = 0.9924). ?? The Royal Society of Chemistry 2004.

Distribution and flux of 238Pu, 239,240Pu, 241Am, 137Cs and 210Pb to high arctic lakes in the Thule district (Greenland).

PubMed

Eriksson, M; Holm, E; Roos, P; Dahlgaard, H

2004-01-01

Environmental samples (soil, sediment and lake water) in the Thule area (NW Greenland) have been studied to assess the contamination of radionuclides originating from a nuclear weapons accident (the Thule accident in 1968). Four lakes were chosen at different distances from the point of impact with the Thule air base community situated in between. The sedimentation rates in the lakes varied from 0.4 mm a(-1) (5 mg cm(-2) a(-1)) to 1.6 mm a(-1) (82 mg cm(-2) a(-1)). With these sedimentation rates, it is not possible to resolve the (239,240)Pu global fallout peak from a possible (239,240)Pu "accident" peak in the sediment depth profiles. However, the (239,240)Pu/(137)Cs and the (238)Pu/(239,240)Pu ratios agreed well with global fallout ratios, indicating that plutonium originating from the accident had not reached these lakes. This also indicates that the Thule air base community has probably only been exposed to radionuclides from the accident to a very limited extent. A limited study showed that (210)Pb could not be used as a normalizing nuclide to explain the transport of transuranic elements from the catchment area to the lake, i.e. (210)Pb has a different transport mechanism from that of the transuranic elements studied in this investigation.

Transport of (137)Cs, (241)Am and Pu isotopes in the Curonian Lagoon and the Baltic Sea.

PubMed

Lujanienė, G; Remeikaitė-Nikienė, N; Garnaga, G; Jokšas, K; Šilobritienė, B; Stankevičius, A; Šemčuk, S; Kulakauskaitė, I

2014-01-01

Activities of (137)Cs, (241)Am and (239,240)Pu were analyzed with special emphasis on better understanding of radionuclide transport from land via the Neman River estuaries to the Baltic Sea and behavior in the marine environment. Although activity concentrations of (137)Cs in water samples collected the Baltic Sea were almost 100 times higher as compared to the Curonian Lagoon, its activities in the bottom sediments were found to be comparable. Activity (238)Pu/(239,240)Pu and atom (240)Pu/(239)Pu ratios indicated a different contribution of the Chernobyl-originated Pu to the suspended particulate matter (SPM) and bottom sediments. The largest amount of the Chernobyl-derived Pu was found in the smallest suspended matter particles of 0.2-1 μm in size collected in the Klaipeda Strait in 2011-2012. The decrease of characteristic activity (238)Pu/(239,240)Pu and atom (240)Pu/(239)Pu ratios towards the global fallout ones in surface soil and the corresponding increase of plutonium (Pu) ratios in the suspended particulate matter and bottom sediments have indicated that the Chernobyl-derived Pu, primarily deposited on the soil surface, was washed out and transported to the Baltic Sea. Behavior of (241)Am was found to be similar to that of Pu isotopes. Copyright © 2013 Elsevier Ltd. All rights reserved.

Off-Site Radiation Exposure Review Project: Phase 2 soils program

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

McArthur, R.D.; Miller, F.L. Jr.

1989-12-01

To help estimate population doses of radiation from fallout originating at the Nevada Test Site, soil samples were collected throughout the western United States. Each sample was prepared by drying and ball-milling, then analyzed by gamma-spectrometry to determine the amount of {sup 137}Cs it contained. Most samples were also analyzed by chemical separation and alpha-spectrometry to determine {sup 239 + 240}Pu and by isotope mass spectroscopy to determine the ratios of {sup 240}Pu to {sup 239}Pu and {sup 241}Pu to {sup 239}Pu. The total inventories of cesium and plutonium at 171 sites were computed from the results. This report describesmore » the sample collection, processing, and analysis, presents the analytical results, and assesses the quality of the data. 10 refs., 9 figs., 12 tabs.« less

Uranium and plutonium in anoxic marine sediments of the Santiago River mouth (Eastern Pacific, Mexico).

PubMed

Almazán-Torres, María Guadalupe; Ordóñez-Regil, Eduardo; Ruiz-Fernández, Ana Carolina

2016-11-01

The uranium (U) and plutonium (Pu) content with depth in a sediment core collected in the continental shelf off the mouth of the Santiago River in the Mexican Pacific was studied to evaluate the contamination effects of the effluent of the Santiago-Lerma River as it moves into the sea. The large mass of terrestrial detritus delivered by the river influences the physicochemical and geochemical processes in the seafloor. Abnormal concentrations of U and Pu in sediments were examined as indicative of the effects of anoxic conditions. One of the indicators of pollution of seawater is the bacterial activity of the shallow seabed layer; and among the prevailing bacteria, the magnetotactic ones induce the formation of euhedral and framboidal shapes (pyrite). These pyrite entities are by-products of anoxic environments loaded with decomposing detrital material and are very abundant in the surface layers of the sediment core analyzed. The pyrite formation is the result of a biochemical reaction between iron and organic sulphur reduced by bacteria, and the pyrite entities precipitate to the seafloor. In the same upper zone of the profile, 238 U is readily immobilized, while 234 U is oxidized and dissolved in seawater by the effect of hot atom chemistry. This may cause the activity ratio (AR) 234 U/ 238 U disequilibrium (near 0.41). Furthermore, in the shallow layer of the sediment core, an abnormally high concentration of 239+240 Pu was detected. In this upper layer, the activity concentrations found were 3.19 Bq kg -1 for 238 U, 1.32 kg -1 for 234 U and 2.78 Bq kg -1 for 239+240 Pu. In the lower fractions of the sediment core, normal values of AR 234 U/ 238 U (≈1) were found, with traces of 239+240 Pu. Copyright © 2016 Elsevier Ltd. All rights reserved.

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

None, None

Operations of Sandia National Laboratories, Nevada (SNL/NV) at the Tonopah Test Range (TTR) resulted in no planned point radiological releases during 1996. Other releases from SNL/NV included diffuse transuranic sources consisting of the three Clean Slate sites. Air emissions from these sources result from wind resuspension of near-surface transuranic contaminated soil particulates. The total area of contamination has been estimated to exceed 20 million square meters. Soil contamination was documented in an aerial survey program in 1977 (EG&G 1979). Surface contamination levels were generally found to be below 400 pCi/g of combined plutonium-238, plutonium-239, plutonium-240, and americium-241 (i.e., transuranic) activity.more » Hot spot areas contain up to 43,000 pCi/g of transuranic activity. Recent measurements confirm the presence of significant levels of transuranic activity in the surface soil. An annual diffuse source term of 0.39 Ci of transuranic material was calculated for the cumulative release from all three Clean Slate sites. A maximally exposed individual dose of 1.1 mrem/yr at the TTR airport area was estimated based on the 1996 diffuse source release amounts and site-specific meteorological data. A population dose of 0.86 person-rem/yr was calculated for the local residents. Both dose values were attributable to inhalation of transuranic contaminated dust.« less

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

PubMed

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

2001-05-01

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

Presence of plutonium contamination in soils from Palomares (Spain).

PubMed

Jiménez-Ramos, M C; García-Tenorio, R; Vioque, I; Manjón, G; García-León, M

2006-08-01

More than 30 years after the occurrence of an aircraft accident which involved the detonation of two nuclear weapons in the surrounding area of the village of Palomares (Spain), the affected terrestrial area has been investigated for remaining transuranic contamination. Evidence from the presence of this contamination was initially found through the analysis of the 241Am inventories in superficial soil samples collected in the region, and was confirmed through the analysis of the (239+240)Pu inventories and their associated 238Pu/(239+240)Pu activity ratios in the same samples. However, it was also observed that a considerable fraction of the remaining contamination in the area was present in particulate form, i.e. as "hot particles". The work performed in our laboratory for identification, isolation and characterisation of these "hot particles" as well as some conclusions obtained from these analyses are outlined in this paper.

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

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

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

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

Model testing of radioactive contamination by 90Sr, 137Cs and 239,240Pu of water and bottom sediments in the Techa River (Southern Urals, Russia).

PubMed

Kryshev, I I; Boyer, P; Monte, L; Brittain, J E; Dzyuba, N N; Krylov, A L; Kryshev, A I; Nosov, A V; Sanina, K D; Zheleznyak, M I

2009-03-15

This paper presents results of testing models for the radioactive contamination of river water and bottom sediments by (90)Sr, (137)Cs and (239,240)Pu. The scenario for the model testing was based on data from the Techa River (Southern Urals, Russia), which was contaminated as a result of discharges of liquid radioactive waste into the river. The endpoints of the scenario were model predictions of the activity concentrations of (90)Sr, (137)Cs and (239,240)Pu in water and bottom sediments along the Techa River in 1996. Calculations for the Techa scenario were performed by six participant teams from France (model CASTEAUR), Italy (model MARTE), Russia (models TRANSFER-2, CASSANDRA, GIDRO-W) and Ukraine (model RIVTOX), all using different models. As a whole, the radionuclide predictions for (90)Sr in water for all considered models, (137)Cs for MARTE and TRANSFER-2, and (239,240)Pu for TRANSFER-2 and CASSANDRA can be considered sufficiently reliable, whereas the prediction for sediments should be considered cautiously. At the same time the CASTEAUR and RIVTOX models estimate the activity concentrations of (137)Cs and (239,240)Pu in water more reliably than in bottom sediments. The models MARTE ((239,240)Pu) and CASSANDRA ((137)Cs) evaluated the activity concentrations of radionuclides in sediments with about the same agreement with observations as for water. For (90)Sr and (137)Cs the agreement between empirical data and model predictions was good, but not for all the observations of (239,240)Pu in the river water-bottom sediment system. The modelling of (239,240)Pu distribution proved difficult because, in contrast to (137)Cs and (90)Sr, most of models have not been previously tested or validated for plutonium.

Characterization of selected radionuclides in sediment and surface water in Standley Lake, Great Western Reservoir, and Mower Reservoir, Jefferson County, Colorado, 1992

USGS Publications Warehouse

Clow, D.W.; Johncox, D.A.

1995-01-01

Lake sediment and surface water from Standley Lake, Great Western Reservoir, and Mower Reservoir, near Denver, Colorado, were sampled and analyzed for selected radionuclides during August through October, 1992. Sample concentrations were summarized and compared to results from a study conducted in 1983-84. Median plutonium-239,240 (239,240Pu) concentrations in lake-sediment grab samples from Standley Lake, Great Western Reservoir, and Mower Reservoir were 0.037, 0.105, and 0.351 picocuries per gram (pCi/g). The maximum concen- tration of 239,240Pu dissolved in lake water was 0.009 picocuries per liter, substantially below limits suggested by the Colorado Department of Health and the Environment. Dissolved concentrations of gross alpha and uranium isotopes were below National Drinking Water Standards in all water samples. There was no statistically significant difference between 239,240Pu concentration in lake-sediment grab samples collected from Standley Lake in 1983-84 and in 1992; however, there was a small, but statistically significant, difference at Great Western Reservoir (p<0.05). In 1992 at Great Western Reservoir, median 239,240Pu concentrations were 0.040 pCi/g lower than in 1983-84. There was a small, but statistically significant (p<0.05) difference in 239,240Pu concentrations in lake- bottom-sediment cores collected in 1983-84 and in 1992. Measured concentrations tended to be higher in 1983-84 than in 1992. The differences were greatest at concentrations above 1.5 pCi/g; in those samples concentrations were 10 to 30% higher in 1983-84 than in 1992.

Transfer of aged 239+240Pu, 238Pu, 241Am, and 137Cs to cattle grazing a contaminated arid environment.

PubMed

Gilbert, R O; Engel, D W; Anspaugh, L R

1989-09-01

In this paper, estimates are obtained of the fraction of ingested 239+240Pu, 238Pu, 241Am and 137Cs transferred to blood, muscle, liver, kidney, femur, vertebra, and gonads of a reproducing herd of 17 beef cattle, individuals of which grazed within fenced enclosures for up to 1064 days under natural conditions with no supplemental feeding at an arid site contaminated 16 years previously with transuranic radionuclides. The estimated geometric mean (GM) GI-to-blood fractional transfer of 238Pu (0.0001) was about 20 times larger than the estimated transfer of 239+240Pu (0.000005), while the estimated transfer of 241Am (0.00001) was about 2 times larger than that of 239+240Pu. These GM GI-to-blood transfers were smaller than the GI-to-blood transfer value of 0.001 recommended by the International Commission on Radiological Protection (ICRP) for humans exposed via food chains or occupationally from unknown mixtures or compounds of plutonium and americium. Statistical tests indicated significantly (p less than 0.05) larger GI-to-tissue transfers of (1) 238Pu as compared to 239+240Pu for all tissues examined, (2) of 238Pu as compared to 241Am for muscle, liver, femur, and vertebra, and (3) of 241Am as compared to 239+240Pu for blood serum, femur, and kidney. The estimated GM fractional transfers of 137Cs from GI to muscle and liver were 0.03 (n = 8) and 0.001 (n = 3), respectively, assuming a 50-day biological half-time of 137Cs in cattle tissue.

Historical changes in 239Pu and 240Pu sources in sedimentary records in the East China Sea: Implications for provenance and transportation

NASA Astrophysics Data System (ADS)

Wang, Jinlong; Baskaran, Mark; Hou, Xiaolin; Du, Jinzhou; Zhang, Jing

2017-05-01

Concentrations and isotopic compositions of plutonium (Pu) are widely used for its source identification and to determine transport processes of Pu-associated particulate matter and water. We investigated the concentrations of 239Pu and 240Pu and their ratios in a number of sediment samples from the East China Sea (ECS) collected in the summer of 2013 (August 6-28). The 239+240Pu activity concentrations in surface sediment samples were found to range between 0.048 and 0.492 Bq kg-1 and the 240Pu/239Pu atom ratios showed a similar trend as that of the 239, 240Pu activities; the Pu atom ratios ranged from 0.158 to 0.297 and were mostly higher than the mean global fallout value of 0.18. The 239, 240Pu inventories in the ECS varied widely, from 2 to 807 Bq m-2, with the highest values commonly found in the coastal areas. In the Yangtze Estuary, the mean 239+240Pu activity concentration is close to the estimated value of the suspended material from the Yangtze River catchment (0.18 Bq kg-1), and the 240Pu/239Pu atom ratio was found to be ∼0.18, which indicates that the Yangtze River input is the dominant source of Pu for this area. The total annual Yangtze River input of 239+240Pu was estimated to be 2.4 ×1010 Bq, which is small compared to the total amount of 239+240Pu buried, 3.1 ×1013 Bq in the whole ECS. The Pacific Proving Ground input appears to be the dominant source of Pu to the ECS, accounting for 45%-52% of the total inventory. The fractional amount of 239+240Pu scavenged from the total 239+240Pu transported by the Kuroshio Current (KC) and Taiwan Warm Current (TWC) into ECS sediments is estimated to be ∼10%. Our study shows that the 240Pu/239Pu atom ratio is useful not only to obtain a better insight of the biogeochemistry influenced by the KC, but also to trace the long-range transport of other particle-reactive species. Besides, the sedimentation rates obtained based on the penetration depths of 239+240Pu and vertical profiles of excess 210Pb agree within uncertainties, which suggests that 239+240Pu can potentially be used as a chronostratigraphic time marker in the marine environment.

Natural radionuclide and plutonium content in Black Sea bottom sediments

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

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

1996-01-01

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

Production of plutonium, yttrium and strontium tracers for using in environmental research

NASA Astrophysics Data System (ADS)

Arzumanov, A.; Batischev, V.; Berdinova, N.; Borissenko, A.; Chumikov, G.; Lukashenko, S.; Lysukhin, S.; Popov, Yu.; Sychikov, G.

2001-12-01

Summary of cyclotron production methods of 237Pu (45,2 d), 88Y (106,65 d) and 85Sr (64,84 d) tracers via nuclear reactions with protons and alphas on 235U, 88Sr and 85Rb targets in wide energy range is given. Chemical methods of separation and purification of the tracers from the irradiated uranium, strontium and rubidium targets are described. The tracers were used for determination of Pu (239-240), Sr-90 and Am-241 in the samples (soil, plants, underground waters) from Semipalatinsk Test Site. Obtained results are discussed.

Soil and sediment sample analysis for the sequential determination of natural and anthropogenic radionuclides.

PubMed

Michel, H; Levent, D; Barci, V; Barci-Funel, G; Hurel, C

2008-02-15

A new sequential method for the determination of both natural (U, Th) and anthropogenic (Sr, Cs, Pu, Am) radionuclides has been developed for application to soil and sediment samples. The procedure was optimised using a reference sediment (IAEA-368) and reference soils (IAEA-375 and IAEA-326). Reference materials were first digested using acids (leaching), 'total' acids on hot plate, and acids in microwave in order to compare the different digestion technique. Then, the separation and purification were made by anion exchange resin and selective extraction chromatography: transuranic (TRU) and strontium (SR) resins. Natural and anthropogenic alpha radionuclides were separated by uranium and tetravalent actinide (UTEVA) resin, considering different acid elution medium. Finally, alpha and gamma semiconductor spectrometer and liquid scintillation spectrometer were used to measure radionuclide activities. The results obtained for strontium-90, cesium-137, thorium-232, uranium-238, plutonium-239+240 and americium-241 isotopes by the proposed method for the reference materials provided excellent agreement with the recommended values and good chemical recoveries. Plutonium isotopes in alpha spectrometry planchet deposits could be also analysed by ICPMS.

Characteristics of radionuclide accumulation in benthic organisms and fish of the Barents and Kara Seas

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

Matishov, G.G.; Matishov, D.G.; Rissanen, C.

1995-05-01

Artificial radionuclides play a specific role in the hydrochemical, geochemical, and hydrobiological processes that are currently occurring in the western Arctic. The existing data on radioactive contamination of different plant and animal species inhabiting the sea shelf are fragmentary. Hence, it was difficult to follow the transformation of radionuclides during their transmission along food chains, from phyto- and zoo-plankton to benthos, fish, birds, and marine mammals. In 1990-1994, the Murmansk Institute of Marine Biology organized expeditions to collect samples of residues on the sea floor and also of benthos, benthic fish, macrophytes, and other organisms inhabiting the shelf of themore » Barents and Kara Seas. These samples were tested for cesium-137, cesium-134, strontium-90, plutonium-239, plutonium-240, americium-241, and cobalt-60 in Rovaniemi (Finland) by the regional radiation administration of the Finnish Centre for Radiation and Nuclear Safety. Over 1000 tests were made. Their results provided new data on the content and distribution of these radionuclides among different components of marine ecosystems. 7 refs.« less

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

PubMed

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

2003-08-01

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

U, Pu, and Am nuclear signatures of the Thule hydrogen bomb debris.

PubMed

Eriksson, Mats; Lindahl, Patric; Roos, Per; Dahlgaard, Henning; Holm, Elis

2008-07-01

This study concerns an arctic marine environment that was contaminated by actinide elements after a nuclear accident in 1968, the so-called Thule accident In this study we have analyzed five isolated hot particles as well as sediment samples containing particles from the weapon material for the determination of the nuclear fingerprint of the accident. We report that the fissile material in the hydrogen weapons involved in the Thule accident was a mixture of highly enriched uranium and weapon-grade plutonium and that the main fissile material was 235U (about 4 times more than the mass of 239Pu). In the five hot particles examined, the measured uranium atomic ratio was 235U/238U = 1.02 +/- 0.16 and the Pu-isotopic ratios were as follows: 24Pu/239Pu = 0.0551 +/- 0.0008 (atom ratio), 238Pu/239+240Pu = 0.0161 +/- 0.0005 (activity ratio), 241Pu/239+240Pu = 0.87 +/- 0.12 (activity ratio), and 241Am/ 239+240Pu = 0.169 +/- 0.005 (activity ratio) (reference date 2001-10-01). From the activity ratios of 241Pu/241Am, we estimated the time of production of this weapon material to be from the late 1950s to the early 1960s. The results from reanalyzed bulk sediment samples showed the presence of more than one Pu source involved in the accident, confirming earlier studies. The 238Pu/239+240PU activity ratio and the 240Pu/ 239Pu atomic ratio were divided into at least two Pu-isotopic ratio groups. For both Pu-isotopic ratios, one ratio group had identical ratios as the five hot particles described above and for the other groups the Pu isotopic ratios were lower (238Pu/ 239+240PU activity ratio approximately 0.01 and the 240Pu/P239Pu atomic ratio 0.03). On the studied particles we observed that the U/Pu ratio decreased as a function of the time these particles were present in the sediment. We hypothesis that the decrease in the ratio is due to a preferential leaching of U relative to Pu from the particle matrix.

Role of natural organic matter on iodine and (239)(,240)Pu distribution and mobility in environmental samples from the northwestern Fukushima Prefecture, Japan.

PubMed

Xu, Chen; Zhang, Saijin; Sugiyama, Yuko; Ohte, Nobuhito; Ho, Yi-Fang; Fujitake, Nobuhide; Kaplan, Daniel I; Yeager, Chris M; Schwehr, Kathleen; Santschi, Peter H

2016-03-01

In order to assess how environmental factors are affecting the distribution and migration of radioiodine and plutonium that were emitted from the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, we quantified iodine and (239,240)Pu concentration changes in soil samples with different land uses (urban, paddy, deciduous forest and coniferous forest), as well as iodine speciation in surface water and rainwater. Sampling locations were 53-63 km northwest of the FDNPP within a 75-km radius, in close proximity of each other. A ranking of the land uses by their surface soil (<4 cm) stable (127)I concentrations was coniferous forest > deciduous forest > urban > paddy, and (239,240)Pu concentrations ranked as deciduous forest > coniferous forest > paddy ≥ urban. Both were quite distinct from that of (134)Cs and (137)Cs: urban > coniferous forest > deciduous forest > paddy, indicating differences in their sources, deposition phases, and biogeochemical behavior in these soil systems. Although stable (127)I might not have fully equilibrated with Fukushima-derived (129)I, it likely still works as a proxy for the long-term fate of (129)I. Surficial soil (127)I content was well correlated to soil organic matter (SOM) content, regardless of land use type, suggesting that SOM might be an important factor affecting iodine biogeochemistry. Other soil chemical properties, such as Eh and pH, had strong correlations to soil (127)I content, but only within a given land use (e.g., within urban soils). Organic carbon (OC) concentrations and Eh were positively, and pH was negatively correlated to (127)I concentrations in surface water and rain samples. It is also noticeable that (127)I in the wet deposition was concentrated in both the deciduous and coniferous forest throughfall and stemfall water, respectively, comparing to the bulk rainwater. Further, both forest throughfall and stemflow water consisted exclusively of organo-iodine, suggesting all inorganic iodine in the original bulk deposition (∼ 28.6% of total iodine) have been completely converted to organo-iodine. Fukushima-derived (239,240)Pu was detectable at a distance ∼ 61 km away, NW of FDNPP. However, it is confined to the litter layer, even three years after the FDNPP accident-derived emissions. Plutonium-239,240 activities were significantly correlated with soil OC and nitrogen contents, indicating Pu may be associated with nitrogen-containing SOM, similar to what has been observed at other locations in the United States. Together, these finding suggest that natural organic matter (NOM) plays a key role in affecting the fate and transport of I and Pu and may warrant greater consideration for predicting long-term stewardship of contaminated areas and evaluating various remediation options in Japan. Copyright © 2016 Elsevier Ltd. All rights reserved.

Modelling Deposition and Erosion rates with RadioNuclides (MODERN) - Part 2: A comparison of different models to convert 239+240Pu inventories into soil redistribution rates at unploughed sites.

PubMed

Arata, Laura; Alewell, Christine; Frenkel, Elena; A'Campo-Neuen, Annette; Iurian, Andra-Rada; Ketterer, Michael E; Mabit, Lionel; Meusburger, Katrin

2016-10-01

Sheet erosion is one of the major threats to alpine soils. To quantify its role and impact in the degradation processes of alpine grasslands, the application of Fallout Radionuclides (FRN) showed very promising results. The specific characteristics of plutonium 239 + 240 ( 239+240 Pu), such as the homogeneous fallout distribution, the long half-life and the cost and time effective measurements make this tracer application for investigating soil degradation in Alpine grasslands more suitable than any other FRN (e.g. 137 Cs). However, the conversion of 239+240 Pu inventories into soil erosion rates remains a challenge. Currently available conversion models have been developed mainly for 137 Cs with later adaptation to other FRN (e.g. Excess 210 Pb, and 7 Be), each model being defined for specific land use (ploughed and/or unploughed) and processes (erosion or deposition). As such, they may fail in describing correctly the distribution of Pu isotopes in the soil. A new conversion model, MODERN, with an adaptable algorithm to estimate erosion and deposition rates from any FRN inventory changes was recently proposed (Arata et al., 2016). In this complementary contribution, the authors compare the application of MODERN to other available conversion models. The results show a good agreement between soil redistribution rates obtained from MODERN and from the models currently used by the FRN scientific community (i.e. the Inventory Method). Copyright © 2016 The Authors. Published by Elsevier Ltd.. All rights reserved.

Isolation of 236U and 239,240Pu from seawater samples and its determination by Accelerator Mass Spectrometry.

PubMed

López-Lora, Mercedes; Chamizo, Elena; Villa-Alfageme, María; Hurtado-Bermúdez, Santiago; Casacuberta, Núria; García-León, Manuel

2018-02-01

In this work we present and evaluate a radiochemical procedure optimised for the analysis of 236 U and 239,240 Pu in seawater samples by Accelerator Mass Spectrometry (AMS). The method is based on Fe(OH) 3 co-precipitation of actinides and uses TEVA® and UTEVA® extraction chromatography resins in a simplified way for the final U and Pu purification. In order to improve the performance of the method, the radiochemical yields are analysed in 1 to 10L seawater volumes using alpha spectrometry (AS) and Inductively Coupled Plasma Mass Spectrometry (ICP-MS). Robust 80% plutonium recoveries are obtained; however, it is found that Fe(III) concentration in the precipitation solution and sample volume are the two critical and correlated parameters influencing the initial uranium extraction through Fe(OH) 3 co-precipitation. Therefore, we propose an expression that optimises the sample volume and Fe(III) amounts according to both the 236 U and 239,240 Pu concentrations in the samples and the performance parameters of the AMS facility. The method is validated for the current setup of the 1MV AMS system (CNA, Sevilla, Spain), where He gas is used as a stripper, by analysing a set of intercomparison seawater samples, together with the Laboratory of Ion Beam Physics (ETH, Zürich, Switzerland). Copyright © 2017 Elsevier B.V. All rights reserved.

Measurement of the 240Pu/ 239Pu mass ratio using a transition-edge-sensor microcalorimeter for total decay energy spectroscopy

DOE PAGES

Hoover, Andrew S.; Bond, Evelyn M.; Croce, Mark P.; ...

2015-02-27

In this study, we have developed a new category of sensor for measurement of the 240Pu/ 239Pu mass ratio from aqueous solution samples with advantages over existing methods. Aqueous solution plutonium samples were evaporated and encapsulated inside of a gold foil absorber, and a superconducting transition-edge-sensor microcalorimeter detector was used to measure the total reaction energy (Q-value) of nuclear decays via heat generated when the energy is thermalized. Since all of the decay energy is contained in the absorber, we measure a single spectral peak for each isotope, resulting in a simple spectral analysis problem with minimal peak overlap. Wemore » found that mechanical kneading of the absorber dramatically improves spectral quality by reducing the size of radioactive inclusions within the absorber to scales below 50 nm such that decay products primarily interact with atoms of the host material. Due to the low noise performance of the microcalorimeter detector, energy resolution values of 1 keV fwhm (full width at half-maximum) at 5.5 MeV have been achieved, an order of magnitude improvement over α-spectroscopy with conventional silicon detectors. We measured the 240Pu/ 239Pu mass ratio of two samples and confirmed the results by comparison to mass spectrometry values. These results have implications for future measurements of trace samples of nuclear material.« less

Statistical design and analysis of environmental studies for plutonium and other transuranics at NAEG ''safety-shot'' sites

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

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

This paper is centered around the use of stratified random sampling for estimating the total amount (inventory) of $sup 239-240$Pu and uranium in surface soil at ten ''safety-shot'' sites on the Nevada Test Site (NTS) and Tonopah Test Range (TTR) that are currently being studied by the Nevada Applied Ecology Group (NAEG). The use of stratified random sampling has resulted in estimates of inventory at these desert study sites that have smaller standard errors than would have been the case had simple random sampling (no stratification) been used. Estimates of inventory are given for $sup 235$U, $sup 238$U, and $supmore » 239-240$Pu in soil at A Site of Area 11 on the NTS. Other results presented include average concentrations of one or more of these isotopes in soil and vegetation and in soil profile samples at depths to 25 cm. The regression relationship between soil and vegetation concentrations of $sup 235$U and $sup 238$U at adjacent sampling locations is also examined using three different models. The applicability of stratified random sampling to the estimation of concentration contours of $sup 239-240$Pu in surface soil using computer algorithms is also investigated. Estimates of such contours are obtained using several different methods. The planning of field sampling plans for estimating inventory and distribution is discussed. (auth)« less

Certified reference materials and reference methods for nuclear safeguards and security.

PubMed

Jakopič, R; Sturm, M; Kraiem, M; Richter, S; Aregbe, Y

2013-11-01

Confidence in comparability and reliability of measurement results in nuclear material and environmental sample analysis are established via certified reference materials (CRMs), reference measurements, and inter-laboratory comparisons (ILCs). Increased needs for quality control tools in proliferation resistance, environmental sample analysis, development of measurement capabilities over the years and progress in modern analytical techniques are the main reasons for the development of new reference materials and reference methods for nuclear safeguards and security. The Institute for Reference Materials and Measurements (IRMM) prepares and certifices large quantities of the so-called "large-sized dried" (LSD) spikes for accurate measurement of the uranium and plutonium content in dissolved nuclear fuel solutions by isotope dilution mass spectrometry (IDMS) and also develops particle reference materials applied for the detection of nuclear signatures in environmental samples. IRMM is currently replacing some of its exhausted stocks of CRMs with new ones whose specifications are up-to-date and tailored for the demands of modern analytical techniques. Some of the existing materials will be re-measured to improve the uncertainties associated with their certified values, and to enable laboratories to reduce their combined measurement uncertainty. Safeguards involve the quantitative verification by independent measurements so that no nuclear material is diverted from its intended peaceful use. Safeguards authorities pay particular attention to plutonium and the uranium isotope (235)U, indicating the so-called 'enrichment', in nuclear material and in environmental samples. In addition to the verification of the major ratios, n((235)U)/n((238)U) and n((240)Pu)/n((239)Pu), the minor ratios of the less abundant uranium and plutonium isotopes contain valuable information about the origin and the 'history' of material used for commercial or possibly clandestine purposes, and have therefore reached high level of attention for safeguards authorities. Furthermore, IRMM initiated and coordinated the development of a Modified Total Evaporation (MTE) technique for accurate abundance ratio measurements of the "minor" isotope-amount ratios of uranium and plutonium in nuclear material and, in combination with a multi-dynamic measurement technique and filament carburization, in environmental samples. Currently IRMM is engaged in a study on the development of plutonium reference materials for "age dating", i.e. determination of the time elapsed since the last separation of plutonium from its daughter nuclides. The decay of a radioactive parent isotope and the build-up of a corresponding amount of daughter nuclide serve as chronometer to calculate the age of a nuclear material. There are no such certified reference materials available yet. Copyright © 2013 Elsevier Ltd. All rights reserved.

A survey of radioactive fallout data in Alaska

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

DePhillips, M.P.

1995-10-23

Considerable attention has been directed by the scientific community to assessing the levels and fate of radionuclides in Arctic ecosystems. The following text and tables present available data and discussion of radionuclide fallout in Alaska. A literature search of 23 on-line databases (Table 1) using Alaska, Strontium (Sr), Cesium (Cs), Plutonium (Pu) and Radionuclide as constraint terms responded with 177 possible citations. After eliminating duplicate citations, 31 articles were available: 17 were relevant to the subject matter; the remainder addressed geologic issues. All of the cited literature addressed {sup 137}Cs, {sup 90}Sr and {sup 239,240}Pu as a result of radionuclidemore » fallout from nuclear testing or accidental release.« less

Fission cross sections of some thorium, uranium, neptunium and plutonium isotopes relative to /sup 235/U

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

Meadows, J W

1983-10-01

Earlier results from the measurements, at this Laboratory, of the fission cross sections of /sup 230/Th, /sup 232/Th, /sup 233/U, /sup 234/U, /sup 236/U, /sup 238/U, /sup 237/Np, /sup 239/Pu, /sup 240/Pu, and /sup 242/Pu relative to /sup 235/U are reviewed with revisions to include changes in data processing procedures, alpha half lives and thermal fission cross sections. Some new data have also been included. The current experimental methods and procedures and the sample assay methods are described in detail and the sources of error are presented in a systematic manner. 38 references.

No Fukushima Dai-ichi derived plutonium signal in marine sediments collected 1.5-57km from the reactors.

PubMed

Wendel, C C S; Lind, O C; Fifield, L K; Tims, S G; Salbu, B; Oughton, D H

2017-11-01

Based on AMS analysis, it is shown that no Pu signals from the Fukushima accident could be discerned in marine sediments collected 1.5-57km away from the Fukushima Da-ichi power plant (FDNPP), which were clearly influenced by accident-derived radiocesium. The 240 Pu/ 239 Pu atom ratios (0.21-0.28) were significantly higher than terrestrial global fallout (0.182 ± 0.005), but still in agreement with pre-FDNPP accident baseline data for Pu in near coastal seawaters influenced by global fallout and long-range transport of Pu from the Pacific Proving Grounds. Copyright © 2017 Elsevier Ltd. All rights reserved.

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

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

Reboul, S.

2012-08-29

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

The effect of carbonate soil on transport and dose estimates for long-lived radionuclides at a U.S. Pacific test site

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

Conrado, C L; Hamilton, T F; Robison, W L

1999-01-01

The US conducted a series of nuclear tests from 1946 to 1958 at Bikini, a coral atoll, in the Marshall Islands (MI). The aquatic and terrestrial environments of the atoll are still contaminated with several long-lived radionuclides that were generated during testing. The four major radionuclides found in terrestrial plants and soils are Cesium-137 ({sup 137}Cs), Strontium-90 ({sup 90}Sr), Plutonium-239+240 ({sup 239+240}Pu) and Americium-241 ({sup 241}Am). {sup 137}Cs in the coral soils is more available for uptake by plants than {sup 137}Cs associated with continental soils of North America or Europe. Soil-to-plant {sup 137}Cs median concentration ratios (CR) (kBq kg{supmore » {minus}1} dry weight plant/kBq kg{sup {minus}1} dry weight soil) for tropical fruits and vegetables range between 0.8 and 36, much larger than the range of 0.005 to 0.5 reported for vegetation in temperate zones. Conversely, {sup 90}Sr median CRs range from 0.006 to 1.0 at the atoll versus a range from 0.02 to 3.0 for continental silica-based soils. Thus, the relative uptake of {sup 137}Cs and {sup 90}Sr by plants in carbonate soils is reversed from that observed in silica-based soils. The CRs for {sup 239+240}Pu and {sup 241}Am are very similar to those observed in continental soils. Values range from 10{sup {minus}6} to 10{sup {minus}4} for both {sup 239+240}Pu and {sup 241}Am. No significant difference is observed between the two in coral soil.« less

University of Washington's radioecological studies in the Marshall Islands, 1946-1977.

PubMed

Donaldson, L R; Seymour, A H; Nevissi, A E

1997-07-01

Since 1946, personnel from the School of Fisheries, University of Washington (Applied Fisheries Laboratory, 1943-1958; Laboratory of Radiation Biology, 1958-1967; and Laboratory of Radiation Ecology, since 1967), have studied the effects of nuclear detonations and the ensuing radioactivity on the marine and terrestrial environments throughout the Central Pacific. A collection of reports and publications about these activities plus a collection of several thousand samples from these periods are kept at the School of Fisheries. General findings from the surveys show that (1) fission products were prevalent in organisms of the terrestrial environment whereas activation products were prevalent in marine organisms; (2) the best biological indicators of fallout radionuclides by environments were (a) terrestrial-coconuts, land crabs; (b) reef-algae, invertebrates; and (c) marine-plankton, fish. Studies of plutonium and americium in Bikini Atoll showed that during 1971-1977 the highest concentrations of 241Am, 2.85 Bq g(-1) (77 pCi g(-1)) and 239,240Pu, 4.44 Bq g(-1) (120 pCi g(-1)), in surface sediments were found in the northwest part of the lagoon. The concentrations in the bomb craters were substantially lower than these values. Concentrations of soluble and particulate plutonium and americium in surface and deep water samples showed distributions similar to the sediment samples. That is, the highest concentration of these radionuclides in the water column were at locations with highest sediment concentration. Continuous circulation of water in the lagoon and exchange of water with open ocean resulted in removal of 111 G Bq y(-1) (3 Ci y(-1)) 241Am and 222 G Bq y(-1) (6 Ci y(-1)) 239,240Pu into the North Equatorial Current. A summary of the surveys, findings, and the historical role of the Laboratory in radioecological studies of the Marshall Islands are presented.

Biomedical aspects of natural and manufactured environmental radioactivity

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

Hodge, V.

1996-12-31

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

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

PubMed

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

1982-10-01

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

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

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

Landeen, D.S.

1994-09-01

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

Depth profile of 236U/238U in soil samples in La Palma, Canary Islands

PubMed Central

Srncik, M.; Steier, P.; Wallner, G.

2011-01-01

The vertical distribution of the 236U/238U isotopic ratio was investigated in soil samples from three different locations on La Palma (one of the seven Canary Islands, Spain). Additionally the 240Pu/239Pu atomic ratio, as it is a well establish tool for the source identification, was determined. The radiochemical procedure consisted of a U separation step by extraction chromatography using UTEVA® Resin (Eichrom Technologies, Inc.). Afterwards Pu was separated from Th and Np by anion exchange using Dowex 1x2 (Dow Chemical Co.). Furthermore a new chemical procedure with tandem columns to separate Pu and U from the matrix was tested. For the determination of the uranium and plutonium isotopes by alpha spectrometry thin sources were prepared by microprecipitation techniques. Additionally these fractions separated from the soil samples were measured by Accelerator Mass Spectrometry (AMS) to get information on the isotopic ratios 236U/238U, 240Pu/239Pu and 236U/239Pu, respectively. The 236U concentrations [atoms/g] in each surface layer (∼2 cm) were surprisingly high compared to deeper layers where values around two orders of magnitude smaller were found. Since the isotopic ratio 240Pu/239Pu indicated a global fallout signature we assume the same origin as the probable source for 236U. Our measured 236U/239Pu value of around 0.2 is within the expected range for this contamination source. PMID:21481502

Isotopic composition and distribution of plutonium in northern South China Sea sediments revealed continuous release and transport of Pu from the Marshall Islands.

PubMed

Wu, Junwen; Zheng, Jian; Dai, Minhan; Huh, Chih-An; Chen, Weifang; Tagami, Keiko; Uchida, Shigeo

2014-03-18

The (239+240)Pu activities and (240)Pu/(239)Pu atom ratios in sediments of the northern South China Sea and its adjacent Pearl River Estuary were determined to examine the spatial and temporal variations of Pu inputs. We clarified that Pu in the study area is sourced from a combination of global fallout and close-in fallout from the Pacific Proving Grounds in the Marshall Islands where above-ground nuclear weapons testing was carried out during the period of 1952-1958. The latter source dominated the Pu input in the 1950s, as evidenced by elevated (240)Pu/(239)Pu atom ratios (>0.30) in a dated sediment core. Even after the 1950s, the Pacific Proving Grounds was still a dominant Pu source due to continuous transport of remobilized Pu from the Marshall Islands, about 4500 km away, along the North Equatorial Current followed by the transport of the Kuroshio current and its extension into the South China Sea through the Luzon Strait. Using a simple two end-member mixing model, we have quantified the contributions of Pu from the Pacific Proving Grounds to the northern South China Sea shelf and the Pearl River Estuary are 68% ± 1% and 30% ± 5%, respectively. This study also confirmed that there were no clear signals of Pu from the Fukushima Daiichi Nuclear Power Plant accident impacting the South China Sea.

Plutonium isotopes and 241Am in the atmosphere of Lithuania: A comparison of different source terms

NASA Astrophysics Data System (ADS)

Lujanienė, G.; Valiulis, D.; Byčenkienė, S.; Šakalys, J.; Povinec, P. P.

2012-12-01

137Cs, 241Am and Pu isotopes collected in aerosol samples during 1994-2011 were analyzed with special emphasis on better understanding of Pu and Am behavior in the atmosphere. The results from long-term measurements of 240Pu/239Pu atom ratios showed a bimodal frequency distribution with median values of 0.195 and 0.253, indicating two main sources contributing to the Pu activities at the Vilnius sampling station. The low Pu atom ratio of 0.141 could be attributed to the weapon-grade plutonium derived from the nuclear weapon test sites. The frequency of air masses arriving from the North-West and North-East correlated with the Pu atom ratio indicating the input from the sources located in these regions (the Novaya Zemlya test site, Siberian nuclear plants), while no correlation with the Chernobyl region was observed. Measurements carried out during the Fukushima accident showed a negligible impact of this source with Pu activities by four orders of magnitude lower as compared to the Chernobyl accident. The activity concentration of actinides measured in the integrated sample collected in March-April, 2011 showed a small contribution of Pu with unusual activity and atom ratios indicating the presence of the spent fuel of different origin than that of the Chernobyl accident.

Radiochemical determination of 237NP in soil samples contaminated with weapon grade plutonium

NASA Astrophysics Data System (ADS)

Antón, M. P.; Espinosa, A.; Aragón, A.

2006-01-01

The Palomares terrestrial ecosystem (Spain) constitutes a natural laboratory to study transuranics. This scenario is partially contaminated with weapon-grade plutonium since the burnout and fragmentation of two thermonuclear bombs accidentally dropped in 1966. While performing radiometric measurements in the field, the possible presence of 237Np was observed through its 29 keV gamma emission. To accomplish a detailed characterization of the source term in the contaminated area using the isotopic ratios Pu-Am-Np, the radiochemical isolation and quantification by alpha spectrometry of 237Np was initiated. The selected radiochemical procedure involves separation of Np from Am, U and Pu with ionic resins, given that in soil samples from Palomares 239+240Pu levels are several orders of magnitude higher than 237Np. Then neptunium is isolated using TEVA organic resins. After electrodeposition, quantification is performed by alpha spectrometry. Different tests were done with blank solutions spiked with 236Pu and 237Np, solutions resulting from the total dissolution of radioactive particles and soil samples. Results indicate that the optimal sequential radionuclide separation order is Pu-Np, with decontamination percentages obtained with the ionic resins ranging from 98% to 100%. Also, the addition of NaNO2 has proved to be necessary, acting as a stabilizer of Pu-Np valences.

Fallout radioactivity in soil and food samples in the Ukraine: Measurements of iodine, plutonium, cesium, and strontium isotopes

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

Hoshi, Masaharu; Yamamoto, Masayoshi; Kawamura, Hisao

1994-08-01

To estimate the level and distribution of fallout attributable to the Chernobyl accident in the Ukraine, the authors sampled several kinds of substances at Korosten, Zhitomir and at Katyuzhanka, Vishgorod, Kiev in the Ukraine, and measured {sup 137}Cs, {sup 134}Cs, {sup 90}Sr, {sup 129}I, {sup 238}Pu, {sup 239,240}Pu, and the density of {sup 127}I (stable). The substances investigated were soil, dry milk, wheat, rye, drinking water, and mushrooms. Except for the mushrooms collected, which were sampled at Katyuzhanka, Vishgorod, and at Kiev, all substances were at Korosten, Zhitomir. The activity of {sup 137}Cs, {sup 134}Cs, {sup 90}Sr, {sup 238}Pu, andmore » {sup 239,240}Pu were all higher in soil and mushrooms than in the other four substances. The activity of {sup 137}Cs was 960 and 1,210 Bq kg{sup {minus}1} in the two soil samples and 6,110 of Bq kg{sup {minus}1} in the mushrooms. The activity of {sup 134}Cs was {approximately} 15% of {sup 137}Cs in the two soil samples while <3% of {sup 137}Cs in the mushrooms. The activity concentration level of {sup 90}Sr as compared to {sup 137}Cs concentration was 15-31% in food samples other than mushrooms but only 1.9% in mushrooms and 1.4 and 1.2% in the two soil samples. The radioactivity ratios, {sup 238}Pu:{sup 239,240}Pu and {sup 239,240}Pu:{sup 137}Cs, suggested that the proportion of cesium radioisotopes and {sup 239,240}Pu in the soil attributable to the Chernobyl accident was {approximately}100% and 10-20%, respectively, while {approximately} 100% of {sup 239,240}Pu in the mushrooms was attributable to the accident. The activity of {sup 129}I was small but the ratio of {sup 129}I:{sup 127}I in the two soil samples was 4.3x10{sup {minus}8} and 1.0x10{sup {minus}7}, which is {approximately} 10 times larger than that in the global fallout. These results suggest that the areas where the soil was sampled are iodine-deficient and were contaminated slightly by the Chernobyl accident. 12 refs., 1 fig., 3 tabs.« less

Fate of 137Cs, 90Sr and 239+240Pu in soil profiles at a water recharge site in Basel, Switzerland.

PubMed

Abraham, Johannes; Meusburger, Katrin; Waldis, Judith Kobler; Ketterer, Michael E; Zehringer, Markus

2018-02-01

An important process in the production of drinking water is the recharge of the withdrawn ground water with river water at protected recharge fields. While it is well known that undisturbed soils are efficiently filtering and adsorbing radionuclides, the goal of this study was to investigate their behaviour in an artificial recharge site that may receive rapid and additional input of radionuclides by river water (particularly when draining a catchment including nuclear power plants (NPP)). Soil profiles of recharge sites were drilled and analysed for radionuclides, specifically radiocesium ( 137 Cs), radiostrontium ( 90 Sr) and plutonium ( 239+240 Pu). The distribution of the analysed radionuclides were compared with an uncultivated reference soil outside the recharge site. The main activity of 137 Cs was located in the top soil (4.5-7.5 cm) and reached down to a depth of 84 cm and 48 cm for the recharge and the reference site, respectively. The found activities of 239+240 Pu originate from the global fallout after 1950. 239+240 Pu appeared to be strongly adsorbed onto soil particles. The shape of the depth profile was similar to 137 Cs, but also similar between the recharge and the reference site. In contrast, 90 Sr showed a uniform distribution over the entire depth of the recharge and reference profiles indicating that 90 Sr already entered the gravel zone and the ground water. Elevated inventories of the radionuclides were observed for the recharge site. The soil of the recharge field exhibited a threefold higher activity of 137 Cs compared to the reference soil. Also for 239+240 Pu higher inventories where observed for the recharge sites (40%). 90 Sr behaved differently, showing similar inventories between reference and recharge site. We estimate that 75-89% of the total inventory of 137 Cs in the soil at the recharge site (7.000 Bq/m 2 ) originated from the fallout of the Chernobyl accident and from emissions of Swiss NPPs. This estimate is based on the actual activity ratio of 137 Cs/ 239+240 Pu of 22 for global fallout. The investigations identified radiostrontium as potential threat to the ground water. Copyright © 2017 Elsevier Ltd. All rights reserved.

Improved precision and accuracy in quantifying plutonium isotope ratios by RIMS

DOE PAGES

Isselhardt, B. H.; Savina, M. R.; Kucher, A.; ...

2015-09-01

Resonance ionization mass spectrometry (RIMS) holds the promise of rapid, isobar-free quantification of actinide isotope ratios in as-received materials (i.e. not chemically purified). Recent progress in achieving this potential using two Pu test materials is presented. RIMS measurements were conducted multiple times over a period of two months on two different Pu solutions deposited on metal surfaces. Measurements were bracketed with a Pu isotopic standard, and yielded absolute accuracies of the measured 240Pu/ 239Pu ratios of 0.7% and 0.58%, with precisions (95% confidence intervals) of 1.49% and 0.91%. In conclusion, the minor isotope 238Pu was also quantified despite the presencemore » of a significant quantity of 238U in the samples.« less

Particulate, colloidal, and dissolved-phase associations of plutonium and americium in a water sample from well 1587 at the Rocky Flats Plant, Colorado

USGS Publications Warehouse

Harnish, R.A.; McKnight, Diane M.; Ranville, James F.

1994-01-01

In November 1991, the initial phase of a study to determine the dominant aqueous phases that control the transport of plutonium (Pu), americium (Am), and uranium (U) in surface and groundwater at the Rocky Flats Plant was undertaken by the U.S. Geological Survey. By use of the techniques of stirred-cell spiral-flow filtration and crossflow ultrafiltration, particles of three size fractions were collected from a 60-liter sample of water from well 1587 at the Rocky Flats Plant. These samples and corresponding filtrate samples were analyzed for Pu and Am. As calculated from the analysis of filtrates, 65 percent of Pu 239 and 240 activity in the sample was associated with particulate and largest colloidal size fractions. Particulate (22 percent) and colloidal (43 percent) fractions were determined to have significant activities in relation to whole-water Pu activity. Am and Pu 238 activities were too low to be analyzed. Examination and analyses of the particulate and colloidal phases indicated the presence of mineral species (iron oxyhydroxides and clay minerals) and natural organic matter that can facilitate the transport of actinides in ground water. High concentrations of the transition metals copper and zinc in the smallest colloid fractions strongly indicate a potential for organic complexation of metals, and potentially of actinides, in this size fraction.

ARRAYS OF BOTTLES OF PLUTONIUM NITRATE SOLUTION

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

Margaret A. Marshall

2012-09-01

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

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

PubMed

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

2004-01-01

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

40K, 137Cs, 90Sr, 238,239+240Pu and 241Am in mammals' skulls from owls' pellets and owl skeletons in Poland.

PubMed

Gaca, Paweł; Mietelski, Jerzy W; Kitowski, Ignacy; Grabowska, Sylwia; Tomankiewicz, Ewa

2005-01-01

Skulls of small mammals belonging to two species of rodents and three species of insectivores collected in Eastern Poland were the subject of the present investigation. The skulls were separated from owl pellets. Activities of 40K, 137Cs, 90Sr, 238,239+240Pu and 241Am were determined by means of gamma spectrometry as well as liquid scintillation spectrometry or alpha spectrometry along with relevant radiochemical procedures. A detailed description of the procedures is provided. The research was supplied with the analysis of three skeletons of owls. No measurable difference between the skulls of rodents and insectivorous animals with regard to activity of any of the examined radionuclides was found. No accumulation effect in the owl skeletons was detected. Though measured activities of 137Cs and 40K for the skulls were of the same magnitude as those found previously for large wild herbivorous animals from typical locations in Poland, those for 90Sr were even lower than previously determined. A big difference was found for activities of plutonium and americium isotopes. Their mean activities were higher by an order of magnitude when compared to the examined previously values. The maximum 239+240Pu activity was equal to 97.5+/-7.7 mBq/kg, with 65% of it originating from global fallout. Relatively high content of transuranic elements found for rodents and insectivorous mammals seems to be unrelated to their feeding habits and should rather be attributed to the living conditions. It is suggested that small mammals, together with tiny soil particles present in mid-soil living tunnels, can inhale the transuranic elements.

Analysis of actinides in an ombrotrophic peat core - evidence of post-depositional migration of fallout radionuclides

NASA Astrophysics Data System (ADS)

Quinto, Francesca; Hrnecek, Erich; Krachler, Michael; Shotyk, William; Steier, Peter; Winkler, Stephan R.

2013-04-01

Plutonium (239Pu, 240Pu, 241Pu, 242Pu) and uranium (236U, 238U) isotopes were analyzed in an ombrotrophic peat core from the Black Forest, Germany, representing the last 80 years of atmospheric deposition. The reliable determination of these isotopes at ultra-trace levels was possible using ultra-clean laboratory procedures and accelerator mass spectrometry. The 240Pu/239Pu isotopic ratios are constant along the core with a mean value of 0.19 ±0.02 (N = 32). This result is consistent with the acknowledged average 240Pu/239Pu isotopic ratio from global fallout in the Northern Hemisphere. The global fallout origin of Pu is confirmed by the corresponding 241Pu/239Pu (0.0012 ±0.0005) and 242Pu/239Pu (0.004 ± 0.001) isotopic ratios. The identification of the Pu isotopic composition characteristic for global fallout in peat layers pre-dating the period of atmospheric atom bomb testing (AD 1956 - AD 1980) is a clear evidence of the migration of Pu downwards the peat profile. The maximum of global fallout derived 236U is detected in correspondence to the age/depth layer of maximum stratospheric fallout (AD 1963). This finding demonstrates that the 236U bomb peak can be successfully used as an independent chronological marker complementing the 210Pb dating of peat cores. The profiles of the global fallout derived 236U and 239Pu are compared with those of 137Cs and 241Am. As typical of ombrothrophic peat, the temporal fallout pattern of 137Cs is poorly retained. Similarly like for Pu, post-depositional migration of 241Am in peat layers preceding the era of atmospheric nuclear tests is observed.

CONVERSION OF PLUTONIUM TRIFLUORIDE TO PLUTONIUM TETRAFLUORIDE

DOEpatents

Fried, S.; Davidson, N.R.

1957-09-10

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

Pyrochemical process for extracting plutonium from an electrolyte salt

DOEpatents

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

1982-09-20

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

Pyrochemical process for extracting plutonium from an electrolyte salt

DOEpatents

Mullins, Lawrence J.; Christensen, Dana C.

1984-01-01

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

Effect of carbonate soil on transport and dose estimates from long-lived radionuclides at U. S. Pacific Test Site

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

Conrado, C.L.; Hamilton, T.F.; Robison, W.L.

1998-09-01

The United States conducted a series of nuclear tests from 1946 to 1958 at Bikini, a coral atoll, in the Marshall Islands (MI). The aquatic and terrestrial environments of the atoll are still contaminated with several long-lived radionuclides that were generated during testing. The four major radionuclides found in terrestrial plants and soils are Cesium-137 ({sup 137} Cs), Strontium-90 ({sup 90} Sr), Plutonium-239+ 240 ({sup 239+240}Pu) and Americium-241 ({sup 241}Am). {sup 137}Cs in the coral soils is more available for uptake by plants than {sup 137}Cs associated with continental soils of North America or Europe. Soil-to-plant {sup 137}Cs median concentrationmore » ratios (CR) (kBq kg{sup {minus}1} dry weight plant/kBq kg {sup {minus}1} dry weight soil) for tropical fruits and vegetables range between 0.8 and 36, much larger than the range of 0.005 to 0.5 reported for vegetation in temperate zones. Conversely, {sup 90}Sr median CRs range from 0.006 to 1.0 at the atoll versus a range from 0.02 to 3.0 for continental silica-based soils. Thus, the relative uptake of {sup 137}Cs and {sup 90}Sr by plants in carbonate soils is reversed from that observed in silica-based soils. The CRs for {sup 239+240}Pu and {sup 241}Am are very similar to those observed in continental soils. Values range from 10{sup {minus}6} to 10{sup {minus}4} for both {sup 239+240}Pu and {sup 241}Am. No significant difference is observed between the two in coral soil. The uptake of {sup 137}Cs by plants is enhanced because of the absence of mineral binding sites and the low concentration of potassium in the coral soil. {sup 137}Cs is bound to the organic fraction of the soil, whereas {sup 90}Sr, {sup 239+240}Pu and {sup 241}Am are primarily bound to soil particles. Assessment of plant uptake for {sup 137}Cs and {sup 90}Sr into locally grown food crops was a major contributing factor in (1) reliably predicting the radiological dose for returning residents, and (2) developing a strategy to limit the availability and uptake of {sup 137}Cs into locally g« less

Quantitative Analysis of Plutonium Content in Particles Collected from a Certified Reference Material by Total Nuclear Reaction Energy (Q Value) Spectroscopy

NASA Astrophysics Data System (ADS)

Croce, M. P.; Hoover, A. S.; Rabin, M. W.; Bond, E. M.; Wolfsberg, L. E.; Schmidt, D. R.; Ullom, J. N.

2016-08-01

Microcalorimeters with embedded radioisotopes are an emerging category of sensor with advantages over existing methods for isotopic analysis of trace-level nuclear materials. For each nuclear decay, the energy of all decay products captured by the absorber (alpha particles, gamma rays, X-rays, electrons, daughter nuclei, etc.) is measured in one pulse. For alpha-decaying isotopes, this gives a measurement of the total nuclear reaction energy (Q value) and the spectra consist of well-separated, narrow peaks. We have demonstrated a simple mechanical alloying process to create an absorber structure consisting of a gold matrix with small inclusions of a radioactive sample. This absorber structure provides an optimized energy thermalization environment, resulting in high-resolution spectra with minimal tailing. We have applied this process to the analysis of particles collected from the surface of a plutonium metal certified reference material (CRM-126A from New Brunswick Laboratory) and demonstrated isotopic analysis by microcalorimeter Q value spectroscopy. Energy resolution from the Gaussian component of a Bortels function fit was 1.3 keV FWHM at 5244 keV. The collected particles were integrated directly into the detector absorber without any chemical processing. The ^{238}Pu/^{239}Pu and ^{240}Pu/^{239}Pu mass ratios were measured and the results confirmed against the certificate of analysis for the reference material. We also demonstrated inter-element analysis capability by measuring the ^{241}Am/^{239}Pu mass ratio.

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

DOEpatents

Coffinberry, A.S.

1959-08-25

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

Transuranics in bone of deceased former residents of Rongelap Atoll, Marshall Islands.

PubMed

Franke, B; Schupfner, R; Schüttelkopf, H; Spennemann, D H

1995-11-01

Rongelap Atoll received intensive fallout from the 1 March 1954 Bravo thermonuclear test 105 miles upwind at Bikini. Fearful of their continued exposure to radiation, the residents of Rongelap Atoll went into voluntary exile in 1985. Transuranic soil concentrations on Rongelap Island are about 2-3 orders of magnitude greater than the average for the Northern hemisphere; the three dominating transuranics are 239,240Pu and 241Am. Only conflicting information has been available about the extent of transuranic uptake by the Rongelap community. As part of the Rongelap Resettlement Project, the community endorsed the exhumation of bones of deceased former atoll residents to provide an independent estimate of plutonium intake. This approach has the advantage of reducing the uncertainties associated with pathway modeling and the interpretation of urine data. Six graves (4 adults, 2 children) were selected for exhumation. Femora and tibiae were selected as well as humeri from the children's graves. The rest of the remains was left undisturbed. The results of the analysis of 239,240Pu and 241Am are presented. Assuming that the data can be considered as representative for the Rongelap population as a whole, the contamination with transuranics on Rongelap Atoll appears to result in radiation exposures in the order of 1% of the compliance limit of 100 mrem (1 mSv) effective dose equivalent per year.

Vertical migration of plutonium-239 + -240, americium-241 and caesium-137 fallout in a forest soil under spruce.

PubMed

Bunzl, K; Kracke, W; Schimmack, W

1992-03-01

The vertical activity distributions of fallout 238Pu, 239+240Pu, 241Am, 134Cs and 137Cs in a forest soil (Hapludult) were determined at several locations in a spruce stand separately according to their origin (global fallout or Chernobyl fallout). To determine the rate of migration of these radionuclides in each soil horizon, the observed depth profiles of the radionuclides were evaluated with a compartment model. In the top organic horizons (LOf1 and Of2), the migration rates for all radionuclides from both sources were above 0.5 cm per year. In the Oh horizon the migration rates observed for global fallout Pu, Am and Cs were similar (0.2-0.4 cm per year). Compared with Pu, however, the mobility of Am is slightly, but statistically significantly, enhanced. The highest rate in this layer was found for Chernobyl-derived radiocaesium (2 cm per year). In the layers of the mineral horizon (depth 0-2, 2-5 and 5-10 cm) the observed migration rates were very similar for global fallout Pu (0.08-0.7 cm per year) and Am (0.1-2 cm per year). In comparison, the migration rate of global fallout radiocaesium was about half in each layer. The highest rate was observed again for Chernobyl-derived radiocaesium (0.5-3 cm per year).

Radioactive pollution of the waters of the baltic sea during 1986

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

Lazarev, L.N.; Kuznetsov, Yu.V.; Gedeonov, L.I.

Results are presented from an investigation of radioactive pollution of the waters of the Baltic Sea during 1986. Inhomogeneities in the pollution of this area of water, due to varying density of atmospheric radioactive fallout, are detected. It is found that among the radionuclides entering the surface of the Baltic Sea in 1986 as a result of atmospheric transport, the main one in terms of radiation dose is cesium-137. Comparisons are made of the level of cesium-137 content in the waters of the Baltic Sea in 1986 and in preceding years. It is noted that even in the most pollutedmore » regions of the sea the cesium-137 content was 500 times less than the maximum allowable concentration (MAC) in the USSR for drinking water. The first results of the determination of plutonium-239 and 240 in the Baltic Sea are presented.« less

Residual radioactivity in the soil of the Semipalatinsk Nuclear Test Site in the former USSR.

PubMed

Yamamoto, M; Tsukatani, T; Katayama, Y

1996-08-01

This paper deals with our efforts to survey residual radioactivity in the soil sampled at the Semipalatinsk Nuclear Test Site and at off-site areas in Kazakhstan. The soil was sampled at the hypocenter where the first Soviet nuclear explosion was carried out on 29 August 1949, and at the bank of the crater called "Bolapan," which was formed by an underground nuclear detonation on 15 January 1965 along the Shagan River. As a comparison, other soil was also sampled in the cities of Kurchatov and Almaty. These data have allowed a preliminary evaluation of the contemporary radioactive contamination of the land in and around the test site. At the first nuclear explosion site and at Bolapan, higher than background levels of 239,240Pu with weapons-grade plutonium were detected together with fission and activation products such as 137Cs, 60Co, 152Eu, and 154Eu.

Some ecological attributes and plutonium contents of perennial vegetation in Area 13

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

Romney, E.M.; Wallace, A.; Gilbert, R.O.

1973-11-01

Progress is reported on work conducted at the Nevada Test Site under the auspices of the Nevada Applied Ecology Group, Office of Effects Evaluation, USAEC Nevada Operations Office, Las Vegas. Nevada. Included are data on some ecological attributes of the vegetation within thc fenced portion of the Project 57 fallout pattern in Area 13. Also included are some preliminary data on the / sup 239/-240/Pu and /sup 241/Am in samples of vegetation collected in conjunction with the soil sampling program. Prominent shrub and grass species in the fallout pattern of Area 13 include Artemisia spinescens, Atriplex canescens, Atriplex confertifolia, Eurotiamore » lanata, Grayia spinosa, Kochia americana, Lycium andersonii, and Oryzopsis hymenoides. Individual or co-dominant species distinguished local association pattarns of varied size within the fenced study area. Vegetation cover estimates in sample study plots ranged from 12.8 to 25.3 percent. Shrub densities ranged from 11.2 x 10/sup 3/ to 17.9 x 10/sup 3/ plants per hectare, and the standing shrub biomass ranged from 1592 to 4255 kilograms per hectare (0.7 to 1.9 tons per acre). Preliminary results showed rather uniform distributions of /sup 239-240/Pu and /sup 241/Am among indiividual samples of the same plant species collected within an intensive study plot. However, there was considerable variation in the contamination levels between different species, presumably from superficial entrapment of resuspended particulate material. Concentrations in Eurotia lanata were three to five times higher than in other species sampled from the same study site. The /sup 239-240/ Pu and /sup 241/Am generally tended to decrease in samples of vegetation collected at increasing distances from ground zero, but there were poor correlations between vegetation and soil /sup 239-240/Pu concertrations in isopleth strat within the fenced grazing area. Results showed inconsistencies in the Pu/Am ratios for vegettion and soil. Lower ratios found in vegetation samples indicate that preferential uptake and concentration of /sup 241/Am through plant roots might have occurred in the Project 57 fallout area. (auth)« less

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

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

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

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

DOEpatents

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

2014-06-03

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

SEPARATION OF PLUTONIUM

DOEpatents

Maddock, A.G.; Smith, F.

1959-08-25

A method is described for separating plutonium from uranium and fission products by treating a nitrate solution of fission products, uranium, and hexavalent plutonium with a relatively water-insoluble fluoride to adsorb fission products on the fluoride, treating the residual solution with a reducing agent for plutonium to reduce its valence to four and less, treating the reduced plutonium solution with a relatively insoluble fluoride to adsorb the plutonium on the fluoride, removing the solution, and subsequently treating the fluoride with its adsorbed plutonium with a concentrated aqueous solution of at least one of a group consisting of aluminum nitrate, ferric nitrate, and manganous nitrate to remove the plutonium from the fluoride.

Effect of Americium-241 Content on Plutonium Radiation Source Terms

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

Rainisch, R.

1998-12-28

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

Integrating the stabilization of nuclear materials

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

Dalton, H.F.

1996-05-01

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

Characterization of 618-11 solid waste burial ground, disposed waste, and description of the waste generating facilities

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

Hladek, K.L.

1997-10-07

The 618-11 (Wye or 318-11) burial ground received transuranic (TRTJ) and mixed fission solid waste from March 9, 1962, through October 2, 1962. It was then closed for 11 months so additional burial facilities could be added. The burial ground was reopened on September 16, 1963, and continued operating until it was closed permanently on December 31, 1967. The burial ground received wastes from all of the 300 Area radioactive material handling facilities. The purpose of this document is to characterize the 618-11 solid waste burial ground by describing the site, burial practices, the disposed wastes, and the waste generatingmore » facilities. This document provides information showing that kilogram quantities of plutonium were disposed to the drum storage units and caissons, making them transuranic (TRU). Also, kilogram quantities of plutonium and other TRU wastes were disposed to the three trenches, which were previously thought to contain non-TRU wastes. The site burial facilities (trenches, caissons, and drum storage units) should be classified as TRU and the site plutonium inventory maintained at five kilograms. Other fissile wastes were also disposed to the site. Additionally, thousands of curies of mixed fission products were also disposed to the trenches, caissons, and drum storage units. Most of the fission products have decayed over several half-lives, and are at more tolerable levels. Of greater concern, because of their release potential, are TRU radionuclides, Pu-238, Pu-240, and Np-237. TRU radionuclides also included slightly enriched 0.95 and 1.25% U-231 from N-Reactor fuel, which add to the fissile content. The 618-11 burial ground is located approximately 100 meters due west of Washington Nuclear Plant No. 2. The burial ground consists of three trenches, approximately 900 feet long, 25 feet deep, and 50 feet wide, running east-west. The trenches constitute 75% of the site area. There are 50 drum storage units (five 55-gallon steel drums welded together) buried in three rows in the northeast comer. In addition, five eight-foot diameter caissons are located at the west end of the center row of the drum storage units. Initially, wastes disposed to the caissons and drum storage units were from the 325 and 327 building hot cells. Later, a small amount of remote-handled (RH) waste from the 309 building Plutonium Recycle Test Reactor (PRTR) cells, and the newly built 324 building hot cells, was disposed at the site.« less

Method for dissolving plutonium dioxide

DOEpatents

Tallent, Othar K.

1978-01-01

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

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

DOEpatents

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

1962-11-13

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

METHOD OF SEPARATING PLUTONIUM

DOEpatents

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

1958-02-01

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

ADSORPTION-BISMUTH PHOSPHATE METHOD FOR SEPARATING PLUTONIUM

DOEpatents

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

1960-06-28

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

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

DOEpatents

Fried, S.; Baumbach, H.L.

1959-12-01

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

Chemical Disposition of Plutonium in Hanford Site Tank Wastes

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

Delegard, Calvin H.; Jones, Susan A.

2015-05-07

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

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

PubMed

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

2004-02-01

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

PRODUCTION OF PLUTONIUM METAL

DOEpatents

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

1961-01-17

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

Feasibility study of a magnetic fusion production reactor

NASA Astrophysics Data System (ADS)

Moir, R. W.

1986-12-01

A magnetic fusion reactor can produce 10.8 kg of tritium at a fusion power of only 400 MW —an order of magnitude lower power than that of a fission production reactor. Alternatively, the same fusion reactor can produce 995 kg of plutonium. Either a tokamak or a tandem mirror production plant can be used for this purpose; the cost is estimated at about 1.4 billion (1982 dollars) in either case. (The direct costs are estimated at 1.1 billion.) The production cost is calculated to be 22,000/g for tritium and 260/g for plutonium of quite high purity (1%240Pu). Because of the lack of demonstrated technology, such a plant could not be constructed today without significant risk. However, good progress is being made in fusion technology and, although success in magnetic fusion science and engineering is hard to predict with assurance, it seems possible that the physics basis and much of the needed technology could be demonstrated in facilities now under construction. Most of the remaining technology could be demonstrated in the early 1990s in a fusion test reactor of a few tens of megawatts. If the Magnetic Fusion Energy Program constructs a fusion test reactor of approximately 400 MW of fusion power as a next step in fusion power development, such a facility could be used later as a production reactor in a spinoff application. A construction decision in the late 1980s could result in an operating production reactor in the late 1990s. A magnetic fusion production reactor (MFPR) has four potential advantages over a fission production reactor: (1) no fissile material input is needed; (2) no fissioning exists in the tritium mode and very low fissioning exists in the plutonium mode thus avoiding the meltdown hazard; (3) the cost will probably be lower because of the smaller thermal power required; (4) and no reprocessing plant is needed in the tritium mode. The MFPR also has two disadvantages: (1) it will be more costly to operate because it consumes rather than sells electricity, and (2) there is a risk of not meeting the design goals.

PROCESS OF FORMING PLUOTONIUM SALTS FROM PLUTONIUM EXALATES

DOEpatents

Garner, C.S.

1959-02-24

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

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

NASA Astrophysics Data System (ADS)

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

2001-09-01

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

Background Radioactivity in River and Reservoir Sediments near Los Alamos, New Mexico

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

S.G.McLin; D.W. Lyons

2002-05-05

As part of its continuing Environmental Surveillance Program, regional river and lake-bottom sediments have been collected annually by Los Alamos National Laboratory (the Laboratory) since 1974 and 1979, respectively. These background samples are collected from three drainage basins at ten different river stations and five reservoirs located throughout northern New Mexico and southern Colorado. Radiochemical analyses for these sediments include tritium, strontium-90, cesium-137, total uranium, plutonium-238, plutonium-239,-240, americium-241, gross alpha, gross beta, and gross gamma radioactivity. Detection-limit radioactivity originates as worldwide fallout from aboveground nuclear weapons testing and satellite reentry into Earth's atmosphere. Spatial and temporal variations in individual analytemore » levels originate from atmospheric point-source introductions and natural rate differences in airborne deposition and soil erosion. Background radioactivity values on sediments reflect this variability, and grouped river and reservoir sediment samples show a range of statistical distributions that appear to be analyte dependent. Traditionally, both river and reservoir analyte data were blended together to establish background levels. In this report, however, we group background sediment data according to two criteria. These include sediment source (either river or reservoir sediments) and station location relative to the Laboratory (either upstream or downstream). These grouped data are statistically evaluated through 1997, and background radioactivity values are established for individual analytes in upstream river and reservoir sediments. This information may be used to establish the existence and areal extent of trace-level environmental contamination resulting from historical Laboratory research activities since the early 1940s.« less

Airborne Plutonium and non-natural Uranium from the Fukushima DNPP found at 120 km distance a few days after reactor hydrogen explosions.

PubMed

Shinonaga, Taeko; Steier, Peter; Lagos, Markus; Ohkura, Takehisa

2014-04-01

Plutonium (Pu) and non-natural uranium (U) originating from the Fukushima Daiichi Nuclear Power Plant (FDNPP) were identified in the atmosphere at 120 km distance from the FDNPP analyzing the ratio of number of atoms, following written as n(isotope)/n(isotope), of Pu and U. The n((240)Pu)/n((239)Pu), n((241)Pu)/n((239)Pu), n((234)U)/n((238)U), n((235)U)/n((238)U) and n((236)U)/n((238)U) in aerosol samples collected before and after the FDNPP incident were analyzed by accelerator mass spectrometry (AMS) and inductively coupled plasma mass spectrometry (ICPMS). The activity concentrations of (137)Cs and (134)Cs in the same samples were also analyzed by gamma spectrometry before the destructive analysis. Comparing the time series of analytical data on Pu and U obtained in this study with previously reported data on Pu, U, and radioactive Cs, we concluded that Pu and non-natural U from the FDNPP were transported in the atmosphere directly over a 120 km distance by aerosol and wind within a few days after the reactor hydrogen explosions. Effective dose of Pu were calculated using the data of Pu: (130 ± 21) nBq/m(3), obtained in this study. We found that the airborne Pu contributes only negligibly to the total dose at the time of the incident. However the analytical results show that the amount of Pu and non-natural U certainly increased in the environment after the incident.

STRIPPING PROCESS FOR PLUTONIUM

DOEpatents

Kolodney, M.

1959-10-01

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

PLUTONIUM-CUPFERRON COMPLEX AND METHOD OF REMOVING PLUTONIUM FROM SOLUTION

DOEpatents

Potratz, H.A.

1959-01-13

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

Plants as bio-monitors for Cs-137, Pu-238, Pu-239,240 and K-40 at the Savannah River Site.

PubMed

Caldwell, Eric Frank; Duff, Martine C; Ferguson, Caitlin E; Coughlin, Daniel P

2011-05-01

The Savannah River Site was constructed in South Carolina to produce plutonium (Pu) in the 1950s. Discharges associated with these now-ceased operations have contaminated large areas within the site, particularly streams associated with reactor cooling basins. Evaluating the exposure risk of contamination to an ecosystem requires methodologies that can assess the bioavailability of contaminants. Plants, as primary producers, represent an important mode of transfer of contaminants from soils and sediments into the food chain. The objective of this study was to identify local area plants for their ability to act as bio-monitors of radionuclides. The concentrations of cesium-137 ((137)Cs), potassium-40 ((40)K), (238)Pu and (239,240)Pu in plants and their associated soils were determined using γ and α spectrometry. The ratio of contamination concentration found in the plant relative to the soil was calculated to assess a concentration ratio (CR). The highest CR for (137)Cs was found in Pinus palustris needles (CR of 2.18). The correlation of soil and plant (137)Cs concentration was strong (0.76) and the R(2) (0.58) from the regression was significant (p = 0.006). This suggests the ability to predict the degree of (137)Cs contamination of a soil through analysis of the pine needles. The (238)Pu and (239,240)Pu concentrations were most elevated within the plant roots. Extremely high CR values were found in Sparganium americanum (bur-reed) roots with a value of 5.86 for (238)Pu and 5.66 for (239,240)Pu. The concentration of (40)K was measured as a known congener of (137)C. Comparing (40)K and (137)C concentrations in each plant revealed an inverse relationship for these radioisotopes. Correlating (40)K and (137)Cs was most effective in identifying plants that have a high affinity for (137)Cs uptake. The P. palustris and S. americanum proved to be particularly strong accumulators of all K congeners from the soil. Some species that were measured, warrant further investigation, are the carnivorous plant Utricularia inflata (bladderwort) and the emergent macrophyte Juncus effusus. For U. inflata, the levels of (137)Cs, (238)Pu, and (239,240)Pu (which were 3922, 8399, and 803 Bq kg(-1), respectively) in the leaves were extremely high. The highest (137)Cs concentration from the study was measured in the J. effusus root (5721 Bq kg(-1)).

Lithium metal reduction of plutonium oxide to produce plutonium metal

DOEpatents

Coops, Melvin S.

1992-01-01

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

SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS

DOEpatents

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

1958-10-01

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

Volatile fluoride process for separating plutonium from other materials

DOEpatents

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

1959-04-14

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

VOLATILE FLUORIDE PROCESS FOR SEPARATING PLUTONIUM FROM OTHER MATERIALS

DOEpatents

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

1959-04-14

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

SEPARATION OF PLUTONIUM FROM LANTHANUM BY CHELATION-EXTRACTION

DOEpatents

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

1958-12-01

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

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

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

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

2010-01-01

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

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

PubMed

Priest, N D; Hunt, B W

1979-05-01

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

Neutron coincidence counting based on time interval analysis with one- and two-dimensional Rossi-alpha distributions: an application for passive neutron waste assay

NASA Astrophysics Data System (ADS)

Bruggeman, M.; Baeten, P.; De Boeck, W.; Carchon, R.

1996-02-01

Neutron coincidence counting is commonly used for the non-destructive assay of plutonium bearing waste or for safeguards verification measurements. A major drawback of conventional coincidence counting is related to the fact that a valid calibration is needed to convert a neutron coincidence count rate to a 240Pu equivalent mass ( 240Pu eq). In waste assay, calibrations are made for representative waste matrices and source distributions. The actual waste however may have quite different matrices and source distributions compared to the calibration samples. This often results in a bias of the assay result. This paper presents a new neutron multiplicity sensitive coincidence counting technique including an auto-calibration of the neutron detection efficiency. The coincidence counting principle is based on the recording of one- and two-dimensional Rossi-alpha distributions triggered respectively by pulse pairs and by pulse triplets. Rossi-alpha distributions allow an easy discrimination between real and accidental coincidences and are aimed at being measured by a PC-based fast time interval analyser. The Rossi-alpha distributions can be easily expressed in terms of a limited number of factorial moments of the neutron multiplicity distributions. The presented technique allows an unbiased measurement of the 240Pu eq mass. The presented theory—which will be indicated as Time Interval Analysis (TIA)—is complementary to Time Correlation Analysis (TCA) theories which were developed in the past, but is from the theoretical point of view much simpler and allows a straightforward calculation of deadtime corrections and error propagation. Analytical expressions are derived for the Rossi-alpha distributions as a function of the factorial moments of the efficiency dependent multiplicity distributions. The validity of the proposed theory is demonstrated and verified via Monte Carlo simulations of pulse trains and the subsequent analysis of the simulated data.

Sources of the transuranic elements plutonium and neptunium in arctic marine sediments.

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

Cooper, L. W.; Kelley, J. M.; Bond, L. A.

2000-01-01

We report here thermal ionization mass spectrometry measurements of {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, {sup 242}Pu, and {sup 237}Np isolated from oceanic, estuarine, and riverine sediments from the Arctic Ocean Basin. {sup 238}Pu/{sup 239+240}Pu activity ratios are also reported for alpha spectrometric analyses undertaken on a subset of these samples. Our results indicate that the Pu in sediments on the Alaskan shelf and slope, as well as that in the deep basins (Amerasian and Eurasian) of the Arctic Ocean, has its origin in stratospheric and tropospheric fallout. Sediments from the Ob and Yenisei Rivers show isotopic Pu signatures thatmore » are distinctly different from those of northern-hemisphere stratospheric fallout and indicate the presence of weapons-grade Pu originating from nuclear fuel reprocessing wastes generated at Russian facilities within these river catchments. Consequently, sediments of the Eurasian Arctic Ocean, particularly those in the Barents and Kara Seas, probably contain a mixture of Pu from stratospheric fallout, tropospheric fallout, and fuel-reprocessing wastes of riverine origin. In particular, the {sup 241}Pu/{sup 239}Pu ratios observed in these sediments are inconsistent with significant contributions of Pu to the arctic sediments studied from western European reprocessing facilities, principally Sellafield in the UK. Several other potential sources of Pu to arctic sediments can also be excluded as significant based upon the transuranic isotope ratios presented.« less

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

Paton, Ian

The Rocky Flats Environmental Technology Site (RFETS) is a Department of Energy facility located approximately 16 miles northwest of Denver, Colorado. Processing and fabrication of nuclear weapons components occurred at Rocky Flats from 1952 through 1989. Operations at the Site included the use of several radionuclides, including plutonium-239/240 (Pu), americium-241 (Am), and various uranium (U) isotopes, as well as several types of chlorinated solvents. The historic operations resulted in legacy contamination, including contaminated facilities, process waste lines, buried wastes and surface soil contamination. Decontamination and removal of buildings at the site was completed in late 2005, culminating more than tenmore » years of active environmental remediation work. The Corrective Action Decision/Record of Decision was subsequently approved in 2006, signifying regulatory approval and closure of the site. The use of RFETS as a National Wildlife Refuge is scheduled to be in full operation by 2012. To develop a plan for remediating different types of radionuclide contaminants present in the RFETS environment required understanding the different environmental transport pathways for the various actinides. Developing this understanding was the primary objective of the Actinide Migration Evaluation (AME) project. Findings from the AME studies were used in the development of RFETS remediation strategies. The AME project focused on issues of actinide behavior and mobility in surface water, groundwater, air, soil and biota at RFETS. For the purposes of the AME studies, actinide elements addressed included Pu, Am, and U. The AME program, funded by DOE, brought together personnel with a broad range of relevant expertise in technical investigations. The AME advisory panel identified research investigations and approaches that could be used to solve issues related to actinide migration at the Site. An initial step of the AME was to develop a conceptual model to provide a qualitative description of the relationships among potential actinide sources and transport pathways at RFETS. One conceptual model was developed specifically for plutonium and americium, because of their similar geochemical and transport properties. A separate model was developed for uranium because of its different properties and mobility in the environment. These conceptual models were guidelines for quantitative analyses described in the RFETS Pathway Analysis Report, which used existing data from the literature as well as site-specific analyses, including field, laboratory and modeling studies to provide quantitative estimates of actinide migration in the RFETS environment. For pathways where more than one method was used to estimate offsite loads for a specific pathway, the method yielding the highest estimated off-site was used for comparison purposes. For all actinides studied, for pre-remediation conditions, air and surface water were identified to be the dominant transport mechanisms. The estimated annual airborne plutonium-239/240 load transported off site exceeded the surface water load by roughly a factor of 40. However, despite being the largest transport pathway, airborne radionuclide concentrations at the monitoring location with the highest measurements during the period studied were less than two percent of the allowable 10 milli-rem standard governing DOE facilities. Estimated actinide loads for other pathways were much less. Shallow groundwater was approximately two orders of magnitude lower, or 1/100 of the load conveyed in surface water. The estimated biological pathway load for plutonium was approximately five orders of magnitude less, or 1/100,000, of the load estimated for surface-water. The pathway analysis results were taken into consideration during subsequent remediation activities that occurred at the site. For example, when the 903 Pad area was remediated to address elevated concentrations of Pu and Am in the surface soil, portable tent structures were constructed to prevent wind and water erosion from occurring while remediation activities took place. Following remediation of the 903 Pad and surrounding area, coconut erosion blankets were installed to mitigate erosion effects while vegetation was reestablished [2]. These measures were effective tools to address the primary transport mechanisms identified, coupling the scientific understanding of the site with the remediation strategy.« less

Plutonium inventories for stabilization and stabilized materials

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

Williams, A.K.

1996-05-01

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

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

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

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

1963-01-01

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

SEPARATION OF PLUTONIUM HYDROXIDE FROM BISMUTH HYDROXIDE

DOEpatents

Watt, G.W.

1958-08-19

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

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

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

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

1989-09-07

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

SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS

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

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

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

Plutonium Finishing Plant (PFP) Final Safety Analysis Report (FSAR) [SEC 1 THRU 11

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

ULLAH, M K

2001-02-26

The Plutonium Finishing Plant (PFP) is located on the US Department of Energy (DOE) Hanford Site in south central Washington State. The DOE Richland Operations (DOE-RL) Project Hanford Management Contract (PHMC) is with Fluor Hanford Inc. (FH). Westinghouse Safety Management Systems (WSMS) provides management support to the PFP facility. Since 1991, the mission of the PFP has changed from plutonium material processing to preparation for decontamination and decommissioning (D and D). The PFP is in transition between its previous mission and the proposed D and D mission. The objective of the transition is to place the facility into a stablemore » state for long-term storage of plutonium materials before final disposition of the facility. Accordingly, this update of the Final Safety Analysis Report (FSAR) reflects the current status of the buildings, equipment, and operations during this transition. The primary product of the PFP was plutonium metal in the form of 2.2-kg, cylindrical ingots called buttoms. Plutonium nitrate was one of several chemical compounds containing plutonium that were produced as an intermediate processing product. Plutonium recovery was performed at the Plutonium Reclamation Facility (PRF) and plutonium conversion (from a nitrate form to a metal form) was performed at the Remote Mechanical C (RMC) Line as the primary processes. Plutonium oxide was also produced at the Remote Mechanical A (RMA) Line. Plutonium processed at the PFP contained both weapons-grade and fuels-grade plutonium materials. The capability existed to process both weapons-grade and fuels-grade material through the PRF and only weapons-grade material through the RMC Line although fuels-grade material was processed through the line before 1984. Amounts of these materials exist in storage throughout the facility in various residual forms left from previous years of operations.« less

PROCESS FOR SEPARATING PLUTONIUM FROM IMPURITIES

DOEpatents

Wahl, A.C.

1957-11-12

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

PRODUCTION OF PLUTONIUM FLUORIDE FROM BISMUTH PHOSPHATE PRECIPITATE CONTAINING PLUTONIUM VALUES

DOEpatents

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

1961-05-01

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

PLUTONIUM COMPOUNDS AND PROCESS FOR THEIR PREPARATION

DOEpatents

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

1958-01-01

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

Method of separating thorium from plutonium

DOEpatents

Clifton, David G.; Blum, Thomas W.

1984-01-01

A method of chemically separating plutonium from thorium. Plutonium and thorium to be separated are dissolved in an aqueous feed solution, preferably as the nitrate salts. The feed solution is acidified and sodium nitrite is added to the solution to adjust the valence of the plutonium to the +4 state. A chloride salt, preferably sodium chloride, is then added to the solution to induce formation of an anionic plutonium chloride complex. The anionic plutonium chloride complex and the thorium in solution are then separated by ion exchange on a strong base anion exchange column.

Method of separating thorium from plutonium

DOEpatents

Clifton, D.G.; Blum, T.W.

A method of chemically separating plutonium from thorium is claimed. Plutonium and thorium to be separated are dissolved in an aqueous feed solution, preferably as the nitrate salts. The feed solution is acidified and sodium nitrite is added to the solution to adjust the valence of the plutonium to the +4 state. A chloride salt, preferably sodium chloride, is then added to the solution to induce formation of an anionic plutonium chloride complex. The anionic plutonium chloride complex and the thorium in solution are then separated by ion exchange on a strong base anion exchange column.

Method of separating thorium from plutonium

DOEpatents

Clifton, D.G.; Blum, T.W.

1984-07-10

A method is described for chemically separating plutonium from thorium. Plutonium and thorium to be separated are dissolved in an aqueous feed solution, preferably as the nitrate salts. The feed solution is acidified and sodium nitrite is added to the solution to adjust the valence of the plutonium to the +4 state. A chloride salt, preferably sodium chloride, is then added to the solution to induce formation of an anionic plutonium chloride complex. The anionic plutonium chloride complex and the thorium in solution are then separated by ion exchange on a strong base anion exchange column.

Locating trace plutonium in contaminated soil using micro-XRF imaging

DOE PAGES

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

2014-06-01

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

Stabilizing stored PuO2 with addition of metal impurities

NASA Astrophysics Data System (ADS)

Moten, Shafaq; Huda, Muhammad

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

PROCESSES FOR SEPARATING AND RECOVERING CONSTITUENTS OF NEUTRON IRRADIATED URANIUM

DOEpatents

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

1959-11-10

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

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

DOEpatents

Faris, B.F.

1961-04-25

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

Isotopic evidence of plutonium release into the environment from the Fukushima DNPP accident

PubMed Central

Zheng, Jian; Tagami, Keiko; Watanabe, Yoshito; Uchida, Shigeo; Aono, Tatsuo; Ishii, Nobuyoshi; Yoshida, Satoshi; Kubota, Yoshihisa; Fuma, Shoichi; Ihara, Sadao

2012-01-01

The Fukushima Daiichi nuclear power plant (DNPP) accident caused massive releases of radioactivity into the environment. The released highly volatile fission products, such as 129mTe, 131I, 134Cs, 136Cs and 137Cs were found to be widely distributed in Fukushima and its adjacent prefectures in eastern Japan. However, the release of non-volatile actinides, in particular, Pu isotopes remains uncertain almost one year after the accident. Here we report the isotopic evidence for the release of Pu into the atmosphere and deposition on the ground in northwest and south of the Fukushima DNPP in the 20–30 km zones. The high activity ratio of 241Pu/239+240Pu (> 100) from the Fukushima DNPP accident highlights the need for long-term 241Pu dose assessment, and the ingrowth of 241Am. The results are important for the estimation of reactor damage and have significant implication in the strategy of decontamination. PMID:22403743

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

PubMed

Martin, J E

1986-11-01

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

Plutonium, curium, and other radionuclide uptake by the rice plant from a naturally weathered, contaminated soil

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

Adriano, D.C.; McLeod, K.W.; Ciravolo, T.G.

1981-07-01

A greenhouse study using three United States rice varieties (Belle Patna, Nato, and Starbonnet) varying in maturity period and a widely used Asian variety (IR-1561) indicates that, with the exception of /sup 137/Cs, no significant differences were obtained among varieties in the foliage uptake of selected gamma-emitters. On the average, /sup 137/Cs and /sup 40/K were translocated less to the grain than to the foliage. The concentration ratio (CR) values for the gamma-emitters, with the exception of /sup 40/K, were approximately one order of magnitude higher than those for subterranean crops grown in experimental plots adjacent to a chemical separationsmore » facility at the Savannah River Plant. The CR values for /sup 238/Pu and /sup 244/Cm are within the range of values published in the open literature. The CR values for /sup 239/ /sup 240/Pu, however, were higher than the normally reported values for plants grown in nonamended soils.« less

Spatially resolved analysis of plutonium isotopic signatures in environmental particle samples by laser ablation-MC-ICP-MS.

PubMed

Konegger-Kappel, Stefanie; Prohaska, Thomas

2016-01-01

Laser ablation-multi-collector-inductively coupled plasma mass spectrometry (LA-MC-ICP-MS) was optimized and investigated with respect to its performance for determining spatially resolved Pu isotopic signatures within radioactive fuel particle clusters. Fuel particles had been emitted from the Chernobyl nuclear power plant (ChNPP) where the 1986 accident occurred and were deposited in the surrounding soil, where weathering processes caused their transformation into radioactive clusters, so-called micro-samples. The size of the investigated micro-samples, which showed surface alpha activities below 40 mBq, ranged from about 200 to 1000 μm. Direct single static point ablations allowed to identify variations of Pu isotopic signatures not only between distinct fuel particle clusters but also within individual clusters. The resolution was limited to 100 to 120 μm as a result of the applied laser ablation spot sizes and the resolving power of the nuclear track radiography methodology that was applied for particle pre-selection. The determined (242)Pu/(239)Pu and (240)Pu/(239)Pu isotope ratios showed a variation from low to high Pu isotope ratios, ranging from 0.007(2) to 0.047(8) for (242)Pu/(239)Pu and from 0.183(13) to 0.577(40) for (240)Pu/(239)Pu. In contrast to other studies, the applied methodology allowed for the first time to display the Pu isotopic distribution in the Chernobyl fallout, which reflects the differences in the spent fuel composition over the reactor core. The measured Pu isotopic signatures are in good agreement with the expected Pu isotopic composition distribution that is typical for a RBMK-1000 reactor, indicating that the analyzed samples are originating from the ill-fated Chernobyl reactor. The average Pu isotope ratios [(240)Pu/(239)Pu = 0.388(86), (242)Pu/(239)Pu = 0.028(11)] that were calculated from all investigated samples (n = 48) correspond well to previously published results of Pu analyses in contaminated samples from the vicinity of the Chernobyl NPP [e.g. (240)Pu/(239)Pu = 0.394(2) and (242)Pu/(239)Pu = 0.027(1); Nunnemann et al. (J Alloys Compd 271-273:45-48, 1998)].

PLUTONIUM CLEANING PROCESS

DOEpatents

Kolodney, M.

1959-12-01

A method is described for rapidly removing iron, nickel, and zinc coatings from plutonium objects while simultaneously rendering the plutonium object passive. The method consists of immersing the coated plutonium object in an aqueous acid solution containing a substantial concentration of nitrate ions, such as fuming nitric acid.

METHOD OF MAKING PLUTONIUM DIOXIDE

DOEpatents

Garner, C.S.

1959-01-13

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

METHOD OF PRODUCING PLUTONIUM TETRAFLUORIDE

DOEpatents

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

1959-12-15

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

Lymph node clearance of plutonium from subcutaneous wounds in beagles

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

Dagle, G.E.

1973-08-01

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

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

PubMed

Skipperud, Lindis

2004-06-18

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

Tabulated Neutron Emission Rates for Plutonium Oxide

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

Shores, Erik Frederick

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

PROCESS OF SEPARATING PLUTONIUM FROM URANIUM

DOEpatents

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

1958-09-01

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

COLUMBIC OXIDE ADSORPTION PROCESS FOR SEPARATING URANIUM AND PLUTONIUM IONS

DOEpatents

Beaton, R.H.

1959-07-14

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

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

DOEpatents

Finzel, T.G.

1959-03-10

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

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

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

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

2000-09-28

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

PROCESS FOR THE SEPARATION OF HEAVY METALS

DOEpatents

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

1959-01-27

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

DISSOLUTION OF LANTHANUM FLUORIDE PRECIPITATES

DOEpatents

Fries, B.A.

1959-11-10

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

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

USGS Publications Warehouse

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

1988-01-01

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

Source-dependent and source-independent controls on plutonium oxidation state and colloid associations in groundwater.

PubMed

Buesseler, Ken O; Kaplan, Daniel I; Dai, Minhan; Pike, Steven

2009-03-01

Plutonium (Pu) was characterized for its isotopic composition, oxidation states, and association with colloids in groundwater samples near disposal basins in F-Area of the Savannah River Site and compared to similar samples collected six years earlier. Two sources of Pu were identified, the disposal basins, which contained a 24Pu/l39Pu isotopic signature consistent with weapons grade Pu, and 244Cm, a cocontaminant that is a progenitor radionuclide of 24Pu. 24Pu that originated primarily from 244Cm tended to be appreciably more oxidized (Pu(V/VI)), less associated with colloids (approximately 1 kDa - 0.2 microm), and more mobile than 239Pu, as suggested by our prior studies at this site. This is not evidence of isotope fractionation but rather "source-dependent" controls on 240Pu speciation which are processes that are not at equilibrium, i.e., processes that appear kinetically hindered. There were also "source-independent" controls on 239Pu speciation, which are those processes that follow thermodynamic equilibrium with their surroundings. For example, a groundwater pH increase in one well from 4.1 in 1998 to 6.1 in 2004 resulted in an order of magnitude decrease in groundwater 239Pu concentrations. Similarly, the fraction of 239Pu in the reduced Pu(III/IV) and colloidal forms increased systematically with decreases in redox condition in 2004 vs 1998. This research demonstrates the importance of source-dependent and source-independent controls on Pu speciation which would impact Pu mobility during changes in hydrological, chemical, or biological conditions on both seasonal and decadal time scales, and over short spatial scales. This implies more dynamic shifts in Pu speciation, colloids association, and transport in groundwater than commonly believed.

Analysis on fuel breeding capability of FBR core region based on minor actinide recycling doping

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

Permana, Sidik; Novitrian,; Waris, Abdul

Nuclear fuel breeding based on the capability of fuel conversion capability can be achieved by conversion ratio of some fertile materials into fissile materials during nuclear reaction processes such as main fissile materials of U-233, U-235, Pu-239 and Pu-241 and for fertile materials of Th-232, U-238, and Pu-240 as well as Pu-238. Minor actinide (MA) loading option which consists of neptunium, americium and curium will gives some additional contribution from converted MA into plutonium such as conversion Np-237 into Pu-238 and it's produced Pu-238 converts to Pu-239 via neutron capture. Increasing composition of Pu-238 can be used to produce fissilemore » material of Pu-239 as additional contribution. Trans-uranium (TRU) fuel (Mixed fuel loading of MOX (U-Pu) and MA composition) and mixed oxide (MOX) fuel compositions are analyzed for comparative analysis in order to show the effect of MA to the plutonium productions in core in term of reactor criticality condition and fuel breeding capability. In the present study, neptunium (Np) nuclide is used as a representative of MAin trans-uranium (TRU) fuel composition as Np-MOX fuel type. It was loaded into the core region gives significant contribution to reduce the excess reactivity in comparing to mixed oxide (MOX) fuel and in the same time it contributes to increase nuclear fuel breeding capability of the reactor. Neptunium fuel loading scheme in FBR core region gives significant production of Pu-238 as fertile material to absorp neutrons for reducing excess reactivity and additional contribution for fuel breeding.« less

NON-AQUEOUS DISSOLUTION OF MASSIVE PLUTONIUM

DOEpatents

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

1959-05-12

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

OXIDATIVE METHOD OF SEPARATING PLUTONIUM FROM NEPTUNIUM

DOEpatents

Beaufait, L.J. Jr.

1958-06-10

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

PROCESS OF ELIMINATING HYDROGEN PEROXIDE IN SOLUTIONS CONTAINING PLUTONIUM VALUES

DOEpatents

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

1960-09-27

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

Continuous plutonium dissolution apparatus

DOEpatents

Meyer, F.G.; Tesitor, C.N.

1974-02-26

This invention is concerned with continuous dissolution of metals such as plutonium. A high normality acid mixture is fed into a boiler vessel, vaporized, and subsequently condensed as a low normality acid mixture. The mixture is then conveyed to a dissolution vessel and contacted with the plutonium metal to dissolve the plutonium in the dissolution vessel, reacting therewith forming plutonium nitrate. The reaction products are then conveyed to the mixing vessel and maintained soluble by the high normality acid, with separation and removal of the desired constituent. (Official Gazette)

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

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

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

PROCESS FOR SEPARATING PLUTONIUM BY REPEATED PRECIPITATION WITH AMPHOTERIC HYDROXIDE CARRIERS

DOEpatents

Faris, B.F.

1960-04-01

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

PROCESS FOR SEPARATION OF HEAVY METALS

DOEpatents

Duffield, R.B.

1958-04-29

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

PROCESS FOR THE RECOVERY OF PLUTONIUM

DOEpatents

Ritter, D.M.

1959-01-13

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

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

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

Leventhal, P.

1996-05-01

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

PRECIPITATION OF PLUTONOUS PEROXIDE

DOEpatents

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

1961-08-15

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

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

DOEpatents

Angerman, A.A.

1958-10-21

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

PLUTONIUM-THORIUM ALLOYS

DOEpatents

Schonfeld, F.W.

1959-09-15

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

The Fireball integrated code package

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

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

1997-07-01

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

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

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

PubMed

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

2010-12-15

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

Plutonium recovery from spent reactor fuel by uranium displacement

DOEpatents

Ackerman, John P.

1992-01-01

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

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

PubMed Central

Froidevaux, Pascal; Haldimann, Max

2008-01-01

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

REMOVAL OF LEGACY PLUTONIUM MATERIALS FROM SWEDEN

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

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

2013-08-18

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

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

Reilly, Sean Douglas; Smith, Paul Herrick; Jarvinen, Gordon D.

Understanding the water solubility of plutonium and uranium compounds and residues at TA-55 is necessary to provide a technical basis for appropriate criticality safety, safety basis and accountability controls. Individual compound solubility was determined using published solubility data and solution thermodynamic modeling. Residue solubility was estimated using a combination of published technical reports and process knowledge of constituent compounds. The scope of materials considered includes all compounds and residues at TA-55 as of March 2016 that contain Pu-239 or U-235 where any single item in the facility has more than 500 g of nuclear material. This analysis indicates that themore » following materials are not appreciably soluble in water: plutonium dioxide (IDC=C21), plutonium phosphate (IDC=C66), plutonium tetrafluoride (IDC=C80), plutonium filter residue (IDC=R26), plutonium hydroxide precipitate (IDC=R41), plutonium DOR salt (IDC=R42), plutonium incinerator ash (IDC=R47), uranium carbide (IDC=C13), uranium dioxide (IDC=C21), U 3O 8 (IDC=C88), and uranium filter residue (IDC=R26). This analysis also indicates that the following materials are soluble in water: plutonium chloride (IDC=C19) and uranium nitrate (IDC=C52). Equilibrium calculations suggest that PuOCl is water soluble under certain conditions, but some plutonium processing reports indicate that it is insoluble when present in electrorefining residues (R65). Plutonium molten salt extraction residues (IDC=R83) contain significant quantities of PuCl 3, and are expected to be soluble in water. The solubility of the following plutonium residues is indeterminate due to conflicting reports, insufficient process knowledge or process-dependent composition: calcium salt (IDC=R09), electrorefining salt (IDC=R65), salt (IDC=R71), silica (IDC=R73) and sweepings/screenings (IDC=R78). Solution thermodynamic modeling also indicates that fire suppression water buffered with a commercially-available phosphate buffer would significantly reduce the solubility of PuCl 3 by the precipitation of PuPO 4.« less

Excess Weapons Plutonium Immobilization in Russia

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

Jardine, L.; Borisov, G.B.

2000-04-15

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

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

PubMed

Uddin, Saif; Behbehani, Montaha

2018-02-01

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

Effect of Potassium on Uptake of 137Cs in Food Crops Grown on Coral Soils: Annual Crops at Bikini Atoll

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

Stone, E R; Robinson, W

2002-02-01

In 1954 a radioactive plume from the thermonuclear device code named BRAVO contaminated the principal residential islands, Eneu and Bikini, of Bikini Atoll (11{sup o} 36 minutes N; 165{sup o} 22 minutes E), now part of the Republic of the Marshall Islands. The resulting soil radioactivity diminished greatly over the three decades before the studies discussed below began. By that time the shorter-lived isotopes had all but disappeared, but strontium-90 ({sup 90}Sr), and cesium-137, ({sup 137}Cs) were reduced by only one half-life. Minute amounts of the long-lived isotopes, plutonium-239+240 ({sup 239+240}Pu) and americium-241 ({sup 241}Am), were present in soil, butmore » were found to be inconsequential in the food chain of humans and land animals. Rather, extensive studies demonstrated that the major concern for human health was {sup 137}Cs in the terrestrial food chain (Robison et al., 1983; Robison et al., 1997). The following papers document results from several studies between 1986 and 1997 aimed at minimizing the {sup 137}Cs content of annual food crops. The existing literature on radiocesium in soils and plant uptake is largely a consequence of two events: the worldwide fallout of 1952-58, and the fallout from Chernobyl. The resulting studies have, for the most part, dealt either with soils containing some amount of silicate clays and often with appreciable K, or with the short-term development of plants in nutrient cultures.« less

Lingering radioactivity at the Bikini and Enewetak Atolls.

PubMed

Buesseler, Ken O; Charette, Matthew A; Pike, Steven M; Henderson, Paul B; Kipp, Lauren E

2018-04-15

We made an assessment of the levels of radionuclides in the ocean waters, seafloor and groundwater at Bikini and Enewetak Atolls where the US conducted nuclear weapons tests in the 1940's and 50's. This included the first estimates of submarine groundwater discharge (SGD) derived from radium isotopes that can be used here to calculate radionuclide fluxes in to the lagoon waters. While there is significant variability between sites and sample types, levels of plutonium ( 239,240 Pu) remain several orders of magnitude higher in lagoon seawater and sediments than what is found in rest of the world's oceans. In contrast, levels of cesium-137 ( 137 Cs) while relatively elevated in brackish groundwater are only slightly higher in the lagoon water relative to North Pacific surface waters. Of special interest was the Runit dome, a nuclear waste repository created in the 1970's within the Enewetak Atoll. Low seawater ratios of 240 Pu/ 239 Pu suggest that this area is the source of about half of the Pu in the Enewetak lagoon water column, yet radium isotopes suggest that SGD from below the dome is not a significant Pu source. SGD fluxes of Pu and Cs at Bikini were also relatively low. Thus radioactivity associated with seafloor sediments remains the largest source and long term repository for radioactive contamination. Overall, Bikini and Enewetak Atolls are an ongoing source of Pu and Cs to the North Pacific, but at annual rates that are orders of magnitude smaller than delivered via close-in fallout to the same area. Copyright © 2017 The Authors. Published by Elsevier B.V. All rights reserved.

METHOD OF SEPARATING PLUTONIUM

DOEpatents

Heal, H.G.

1960-02-16

BS>A method of separating plutonium from aqueous nitrate solutions of plutonium, uranium. and high beta activity fission products is given. The pH of the aqueous solution is adjusted between 3.0 to 6.0 with ammonium acetate, ferric nitrate is added, and the solution is heated to 80 to 100 deg C to selectively form a basic ferric plutonium-carrying precipitate.

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

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

Grison, E.

1961-01-01

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

Siegfried S. Hecker, Plutonium, and Nonproliferation

Science.gov Websites

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

SEPARATION OF PLUTONIUM FROM FISSION PRODUCTS BY A COLLOID REMOVAL PROCESS

DOEpatents

Schubert, J.

1960-05-24

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

PLUTONIUM RECOVERY FROM NEUTRON-BOMBARDED URANIUM FUEL

DOEpatents

Moore, R.H.

1962-04-10

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

SEPARATION OF RUTHENIUM FROM AQUEOUS SOLUTIONS

DOEpatents

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

1959-09-01

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

Pyrochemical recovery of plutonium from calcium fluoride reduction slag

DOEpatents

Christensen, D.C.

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

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

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

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

2011-07-29

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

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

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

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

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

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

DOEpatents

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

1960-08-23

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

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

PubMed Central

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

2010-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2017-01-01

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

PLUTONIUM-ZIRCONIUM ALLOYS

DOEpatents

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

1960-08-30

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

Plutonium recovery from spent reactor fuel by uranium displacement

DOEpatents

Ackerman, J.P.

1992-03-17

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

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

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

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

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

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

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

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

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

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

PubMed

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

2014-11-01

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

BASIC PEROXIDE PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINANTS

DOEpatents

Seaborg, G.T.; Perlman, I.

1959-02-10

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

PREPARATION OF PLUTONIUM

DOEpatents

Kolodney, M.

1959-07-01

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

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

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

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

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

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

NONE

1996-05-01

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

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

DOEpatents

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

1957-10-29

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

Plutonium controversy

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

Richmond, C.R.

1980-01-01

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

PREPARATION OF PLUTONIUM TRIFLUORIDE

DOEpatents

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

1961-07-11

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

MCNP Parametric Studies of Plutonium Metal and Various Interstitial Moderating Materials

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

Glazener, Natasha; Kamm, Ryan James

2017-03-31

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

SEPARATION OF PLUTONIUM IONS FROM SOLUTION BY ADSORPTION ON ZIRCONIUM PYROPHOSPHATE

DOEpatents

Stoughton, R.W.

1961-01-31

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

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

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

Onishi, Y.; Recknagle, K.

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

Plutonium and americium separation from salts

DOEpatents

Hagan, Paul G.; Miner, Frend J.

1976-01-01

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

Plutonium storage criteria

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

Chung, D.; Ascanio, X.

1996-05-01

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

PROCESS OF PRODUCING SHAPED PLUTONIUM

DOEpatents

Anicetti, R.J.

1959-08-11

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

WET METHOD OF PREPARING PLUTONIUM TRIBROMIDE

DOEpatents

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

1958-11-11

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

Spectrophotometers for plutonium monitoring in HB-line

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

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

2016-02-12

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

Plutonium radiation surrogate

DOEpatents

Frank, Michael I [Dublin, CA

2010-02-02

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

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

DOEpatents

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

1962-07-10

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

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

DOEpatents

Thomas, J.R.

1958-08-26

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

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

NASA Astrophysics Data System (ADS)

Blandinskiy, V. Yu.

2014-12-01

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

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

DOEpatents

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

1959-02-01

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

CONCENTRATION OF Pu USING AN IODATE PRECIPITATE

DOEpatents

Fries, B.A.

1960-02-23

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

ION EXCHANGE ADSORPTION PROCESS FOR PLUTONIUM SEPARATION

DOEpatents

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

1961-07-11

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

IMPROVED PROCESS OF PLUTONIUM CARRIER PRECIPITATION

DOEpatents

Faris, B.F.

1959-06-30

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

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

DOE PAGES

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

2017-01-18

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

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

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

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

2012-07-05

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

PLUTONIUM-CERIUM ALLOY

DOEpatents

Coffinberry, A.S.

1959-01-01

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

Plutonium recovery from organic materials

DOEpatents

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

1973-12-11

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

SEPARATION OF PLUTONIUM FROM AQUEOUS SOLUTIONS BY ION-EXCHANGE

DOEpatents

Schubert, J.

1958-06-01

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

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

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

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

AMINE EXTRACTION OF PLUTONIUM FROM NITRIC ACID SOLUTIONS LOADING AND STRIPPING EXPERIMENTS

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

Wilson, A.S.

1961-01-19

Information is presented on a suitable amine processing system for plutonium nitrate. Experiments with concentrated plutonium nitrate solutions show that trilaurylamine (TLA) - xylene solvent systems did not form a second organic phase. Experiments are also reported with tri-noctylamine (TnOA)-xylene and TLA-Amsco - octyl alcohol. Two organic phases appear in both these systems at high plutonium nitrate concentrations. Data are tabulated from loading and stripping experiments. (J.R.D.)

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

DOEpatents

Steindler, M.J.

1962-07-24

A process was developed for separating uranium hexafluoride from plutonium hexafluoride by the selective reduction of the plutonium hexafluoride to the tetrafluoride with sulfur tetrafluoride at 50 to 120 deg C, cooling the mixture to --60 to -100 deg C, and volatilizing nonreacted sulfur tetrafluoride and sulfur hexafluoride formed at that temperature. The uranium hexafluoride is volatilized at room temperature away from the solid plutonium tetrafluoride. (AEC)

THE CHEMICAL ANALYSIS OF TERNARY ALLOYS OF PLUTONIUM WITH MOLYBDENUM AND URANIUM

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

Phillips, G.; Woodhead, J.; Jenkins, E.N.

1958-09-01

It is shown that the absorptiometric determination of molybdenum as thiocyanate may be used in the presence of plutonium. Molybdenum interferes with previously published methods for determining uranium and plutonium but conditlons have been established for its complete removal by solvent extraction of the compound with alpha -benzoin oxime. The previous methods for uranium and plutonium are satisfactory when applied to the residual aqueous phase following this solvent extraction. (auth)

PROCESS OF SEPARATING PLUTONIUM VALUES BY ELECTRODEPOSITION

DOEpatents

Whal, A.C.

1958-04-15

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

SEPARATION OF PLUTONIUM VALUES FROM URANIUM AND FISSION PRODUCT VALUES

DOEpatents

Maddock, A.G.; Booth, A.H.

1960-09-13

Separation of plutonium present in small amounts from neutron irradiated uranium by making use of the phenomenon of chemisorption is described. Plutonium in the tetravalent state is chemically absorbed on a fluoride in solid form. The steps for the separation comprise dissolving the irradiated uranium in nitric acid, oxidizing the plutonium in the resulting solution to the hexavalent state, adding to the solution a soluble calcium salt which by the common ion effect inhibits dissolution of the fluoride by the solution, passing the solution through a bed or column of subdivided calcium fluoride which has been sintered to about 8OO deg C to remove the chemisorbable fission products, reducing the plutonium in the solution thus obtained to the tetravalent state, and again passing the solution through a similar bed or column of calcium fluoride to selectively absorb the plutonium, which may then be recovered by treating the calcium fluoride with a solution of ammonium oxalate.

Using Biomolecules to Separate Plutonium

NASA Astrophysics Data System (ADS)

Gogolski, Jarrod

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

CARBONATE METHOD OF SEPARATION OF TETRAVALENT PLUTONIUM FROM FISSION PRODUCT VALUES

DOEpatents

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

1959-02-01

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

PROCESS FOR PRODUCTION OF PLUTONIUM FROM ITS OXIDES

DOEpatents

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

1959-10-13

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

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

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

Jardine, L J; Borisov, G B

2004-07-21

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

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

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

NONE

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

SEPARATION OF PLUTONIUM FROM URANIUM

DOEpatents

Feder, H.M.; Nuttall, R.L.

1959-12-15

A process is described for extracting plutonium from powdered neutron- irradiated urarium metal by contacting the latter, while maintaining it in the solid form, with molten magnesium which takes up the plutonium and separating the molten magnesium from the solid uranium.

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

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

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

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

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

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

SEPARATION OF URANIUM, PLUTONIUM, AND FISSION PRODUCTS

DOEpatents

Spence, R.; Lister, M.W.

1958-12-16

Uranium and plutonium can be separated from neutron-lrradiated uranium by a process consisting of dissolvlng the lrradiated material in nitric acid, saturating the solution with a nitrate salt such as ammonium nitrate, rendering the solution substantially neutral with a base such as ammonia, adding a reducing agent such as hydroxylamine to change plutonium to the trivalent state, treating the solution with a substantially water immiscible organic solvent such as dibutoxy diethylether to selectively extract the uranium, maklng the residual aqueous solutlon acid with nitric acid, adding an oxidizing agent such as ammonlum bromate to oxidize the plutonium to the hexavalent state, and selectlvely extracting the plutonium by means of an immlscible solvent, such as dibutoxy dlethyletber.

Volatile Impurities in the Plutonium Immobilization Ceramic Wasteform

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

Cozzi, A.D.

1999-10-15

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

PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINATING ELEMENTS

DOEpatents

Sutton, J.B.

1958-02-18

This patent relates to an improved method for the decontamination of plutonium. The process consists broadly in an improvement in a method for recovering plutonium from radioactive uranium fission products in aqueous solutions by decontamination steps including byproduct carrier precipitation comprising the step of introducing a preformed aqueous slurry of a hydroxide of a metal of group IV B into any aqueous acidic solution which contains the plutonium in the hexavalent state, radioactive uranium fission products contaminant and a by-product carrier precipitate and separating the metal hydroxide and by-product precipitate from the solution. The process of this invention is especially useful in the separation of plutonium from radioactive zirconium and columbium fission products.

Progress on plutonium stabilization

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

Hurt, D.

1996-05-01

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

NON-CORROSIVE PLUTONIUM FUEL SYSTEMS

DOEpatents

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

1962-10-23

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

In-gas-cell laser ionization studies of plutonium isotopes at IGISOL

NASA Astrophysics Data System (ADS)

Pohjalainen, I.; Moore, I. D.; Kron, T.; Raeder, S.; Sonnenschein, V.; Tomita, H.; Trautmann, N.; Voss, A.; Wendt, K.

2016-06-01

In-gas-cell resonance laser ionization has been performed on long-lived isotopes of Pu at the IGISOL facility, Jyväskylä. This initiates a new programme of research towards high-resolution optical spectroscopy of heavy actinide elements which can be produced in sufficient quantities at research reactors and transported to facilities elsewhere. In this work a new gas cell has been constructed for fast extraction of laser-ionized elements. Samples of 238-240,242Pu and 244Pu have been evaporated from Ta filaments, laser ionized, mass separated and delivered to the collinear laser spectroscopy station. Here we report on the performance of the gas cell through studies of the mass spectra obtained in helium and argon, before and after the radiofrequency quadrupole cooler-buncher. This provides valuable insight into the gas phase chemistry exhibited by Pu, which has been additionally supported by measurements of ion time profiles. The resulting monoatomic yields are sufficient for collinear laser spectroscopy. A gamma-ray spectroscopic analysis of the Pu samples shows a good agreement with the assay provided by the Mainz Nuclear Chemistry department.

Concurrent determination of 237Np and Pu isotopes using ICP-MS: analysis of NIST environmental matrix standard reference materials 4357, 1646a, and 2702.

PubMed

Matteson, Brent S; Hanson, Susan K; Miller, Jeffrey L; Oldham, Warren J

2015-04-01

An optimized method was developed to analyze environmental soil and sediment samples for (237)Np, (239)Pu, and (240)Pu by ICP-MS using a (242)Pu isotope dilution standard. The high yield, short time frame required for analysis, and the commercial availability of the (242)Pu tracer are significant advantages of the method. Control experiments designed to assess method uncertainty, including variation in inter-element fractionation that occurs during the purification protocol, suggest that the overall precision for measurements of (237)Np is typically on the order of ± 5%. Measurements of the (237)Np concentration in a Peruvian Soil blank (NIST SRM 4355) spiked with a known concentration of (237)Np tracer confirmed the accuracy of the method, agreeing well with the expected value. The method has been used to determine neptunium and plutonium concentrations in several environmental matrix standard reference materials available from NIST: SRM 4357 (Radioactivity Standard), SRM 1646a (Estuarine Sediment) and SRM 2702 (Inorganics in Marine Sediment). Copyright © 2015 Elsevier Ltd. All rights reserved.

METHOD OF REDUCING PLUTONIUM COMPOUNDS

DOEpatents

Johns, I.B.

1958-06-01

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

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

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

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

Electronic structure, phase transitions and diffusive properties of elemental plutonium

NASA Astrophysics Data System (ADS)

Setty, Arun; Cooper, B. R.

2003-03-01

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

Radiation damage and annealing in plutonium tetrafluoride

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Feasibility of Colliding-beam fast-fission reactor via 238U80++238 U80+ --> 4 FF + 5n + 430 MeV beam with suppressed plutonium and direct conversion of fission fragment (FF) energy into electricity and/or Rocket propellant with high specific impulse

NASA Astrophysics Data System (ADS)

Maglich, Bogdan; Hester, Tim; Calsec Collaboration

2015-10-01

Uranium-uranium colliding beam experiment1, used fully ionized 238U92+ at energy 100GeV --> <-- 100 GeV, has measured total σ = 487 b. Reaction rate of colliding beams is proportional to neutron flux-squared. First functional Auto-Collider3-6, a compact Migma IV, 1 m in diameter, had self-colliding deuterons, D+, of 725 KeV --> <-- 725 KeV, resulting in copious production of T and 3He. U +U Autocollider``EXYDER'' will use strong-focusing magnet7, which would increase reaction rate by 104. 80 times ionized U ions accelerated through 3 MV accelerator, will collide beam 240 MeV --> <-- 240 MeV. Reaction is: 238U80+ +238 U80+ --> 4 FF + 5n + 430 MeV. Using a simple model1 fission σf ~ 100 b. Suppression of Pu by a factor of 106 will be achieved because NO thermal neutron fission can take place; only fast, 1-3 MeV, where σabs is negligible. Direct conversion of 95% of 430 MeV produced is carried by electrically charged FFs which are magnetically funneled for direct conversion of energy of FFs via electrostatic decelerators4,11. 90% of 930 MeV is electrically recoverable. Depending on the assumptions, we project electric _ power density production of 20 to 200 MWe m-3, equivalent to Thermal 1.3 - 13 GWthm-3. If one-half of unburned U is used for propulsion while rest powers system, heavy FF ion mass provides specific impulse Isp = 106 sec., 103 times higher than current rocket engines.

Measurements of Pu and Ra isotopes in soils and sediments by AMS

NASA Astrophysics Data System (ADS)

Tims, S. G.; Hancock, G. J.; Wacker, L.; Fifield, L. K.

2004-08-01

Plutonium fallout from atmospheric nuclear weapons testing in the 1950s and 1960s constitutes an artificial tracer suitable for the study of recent soil erosion and sediment accumulation rates. Long-lived Pu isotopes provide an alternative tracer to the more widely used 137Cs (t1/2=30 a), the concentration of which is decaying at a rate that will limit its long-term application to these studies. For 239,240Pu, the sensitivity of AMS is more than an order of magnitude better than that afforded by α-spectroscopy. Furthermore, AMS can provide a simple, direct measure of the 240Pu/239Pu ratio. Sample profiles from two sites along eastern Australia have been determined with both AMS and α-spectroscopy to provide comparative measurements of the sediment accumulation rate in water bodies and of the soil erosion rate. The two methods are in good agreement. The 228Ra/226Ra ratio potentially provides a probe for tracing the dispersion of uranium mining residues into the neighboring environment. Soil depth profiles of the ratio may provide information on the rate at which mining-derived radioactivity is spread by surface waters, and could be used to assess the effectiveness of remediation and rehabilitation technologies. AMS offers several advantages over the more usual α- and γ-spectroscopy techniques in that it can directly and quickly measure both isotopes in a sample of small size and with simple sample preparation. We show that AMS can be used to measure these isotopes of radium at the sensitivity required for environmental samples using RaC2- as the injected beam species.

Fate and transport of plutonium-239 + 240 and Americium-241 in the soil of Rocky Flats, Colorado

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

Litaor, M.I.; Barth, G.R.; Zika, E.M.

1996-07-01

Actinides contamination of soils around Rocky Flats, CO, resulted from leaking drums of Pu-contaminated oil stored at an outdoor site. The transport of these actinides through the soil to groundwater was studied using an advanced monitoring system (MS). The fully automated, remotely controlled MS gathered real-time data on soil water content, groundwater level, and timing of gravitationally flowing water. Controlled rain simulations coupled with measurements of volume flux and actinide activities provided essential information about the fate and transport of Pu-239 + 240 and Am-241. Volume fluxes at most sampling locations were similar, regardless of the antecedent moisture or themore » duration, frequency, and intensity of the simulated rain. Actinide activities were not correlated with the measured volume flux, or the duration, frequency, and intensity of the simulated rain. Flow was facilitated primarily via macropore channeling. The relatively short residence time precluded a continuous interaction between the soil and the flowing water, which minimized the movement of actinides in the soil. Actinide activities in the interstitial water collected from the upper 20 cm of the soil were significantly higher (P>0.001) than water collected at deeper sampling depths (20-70 cm). Actinide activity in water samples from the deepest sampling depth (40-70 cm) did not exceed 0.4 Bq/L. These results suggest that, under the experimental conditions, the movement of actinides was restricted to the top 20 cm. A transport mechanism involving discrete Pu oxide particles, coupled with macropore channeling is proposed to explain the observed actinide activities in the soil. 31 refs., 6 figs., 7 tabs.« less

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

DOEpatents

Seaborg, G.T.

1961-08-01

A process is described for extracting tetravalent plutonium from an aqueous acid solution with methyl ethyl ketone, methyl isobutyl ketone, or acetophenone and with the extraction of either tetravalent or hexavalent plutonium into menthone. (AEC)

10 CFR 830.3 - Definitions.

Code of Federal Regulations, 2010 CFR

2010-01-01

.... Critical assembly means special nuclear devices designed and used to sustain nuclear reactions, which may... reaction becomes self-sustaining. Design features means the design features of a nuclear facility specified... reaction (e.g., uranium-233, uranium-235, plutonium-238, plutonium-239, plutonium-241, neptunium-237...

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

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

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

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

DOEpatents

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

1959-07-01

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

SOLVENT EXTRACTION PROCESS FOR PLUTONIUM

DOEpatents

Seaborg, G.T.

1959-04-14

The separation of plutonium from aqueous inorganic acid solutions by the use of a water immiscible organic extractant liquid is described. The plutonium must be in the oxidized state, and the solvents covered by the patent include nitromethane, nitroethane, nitropropane, and nitrobenzene. The use of a salting out agents such as ammonium nitrate in the case of an aqueous nitric acid solution is advantageous. After contacting the aqueous solution with the organic extractant, the resulting extract and raffinate phases are separated. The plutonium may be recovered by any suitable method.

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

PubMed

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

2018-07-01

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

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

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

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

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

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

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

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

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

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

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

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

13. VIEW OF THE MOLTEN SALT EXTRACTION LINE. THE MOLTEN SALT EXTRACTION PROCESS WAS USED TO PURIFY PLUTONIUM BY REMOVING AMERICIUM, A DECAY BY-PRODUCT OF PLUTONIUM. (1/98) - Rocky Flats Plant, Plutonium Fabrication, Central section of Plant, Golden, Jefferson County, CO

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

DOEpatents

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

1960-06-14

A process for concentrating plutonium is given in which plutonium is first precipitated with bismuth phosphate and then, after redissolution, precipitated with a different carrier such as lanthanum fluoride, uranium acetate, bismuth hydroxide, or niobic oxide.

METHOD OF SEPARATION OF PLUTONIUM FROM CARRIER PRECIPITATES

DOEpatents

Dawson, I.R.

1959-09-22

The recovery of plutonium from fluoride carrier precipitates is described. The precipitate is dissolved in zirconyl nitrate, ferric nitrate, aluminum nitrate, or a mixture of these complexing agents, and the plutonium is then extracted from the aqueous solution formed with a water-immiscible organic solvent.

EXTRACTION METHOD FOR SEPARATING URANIUM, PLUTONIUM, AND FISSION PRODUCTS FROM COMPOSITIONS CONTAINING SAME

DOEpatents

Seaborg, G.T.

1957-10-29

Methods for separating plutonium from the fission products present in masses of neutron irradiated uranium are reported. The neutron irradiated uranium is first dissolved in an aqueous solution of nitric acid. The plutonium in this solution is present as plutonous nitrate. The aqueous solution is then agitated with an organic solvent, which is not miscible with water, such as diethyl ether. The ether extracts 90% of the uraryl nitrate leaving, substantially all of the plutonium in the aqueous phase. The aqueous solution of plutonous nitrate is then oxidized to the hexavalent state, and agitated with diethyl ether again. In the ether phase there is then obtained 90% of plutonium as a solution of plutonyl nitrate. The ether solution of plutonyl nitrate is then agitated with water containing a reducing agent such as sulfur dioxide, and the plutonium dissolves in the water and is reduced to the plutonous state. The uranyl nitrate remains in the ether. The plutonous nitrate in the water may be recovered by precipitation.

Plutonium release from the 903 pad at Rocky Flats.

PubMed

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

1996-10-01

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

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

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

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

1989-01-01

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

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

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

Delegard, Calvin H.

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

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

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

Whicker, F.W.

1977-08-01

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

COMPLEX FLUORIDES OF PLUTONIUM AND AN ALKALI METAL

DOEpatents

Seaborg, G.T.

1960-08-01

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

DELTA PHASE PLUTONIUM ALLOYS

DOEpatents

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

1960-03-22

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

RECOVERY OF PLUTONIUM BY CARRIER PRECIPITATION

DOEpatents

Goeckermann, R.H.

1961-04-01

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

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

EPA Pesticide Factsheets

SAM lists this method for the qualitative determination of Americium-241, Radium-226, Plutonium-238, Plutonium-239 and isotopic uranium in drinking water samples using alpha spectrometry and radiostrontium using beta counting.

METHOD FOR OBTAINING PLUTONIUM METAL FROM ITS TRICHLORIDE

DOEpatents

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

1962-08-14

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

MOLTEN PLUTONIUM FUELED FAST BREEDER REACTOR

DOEpatents

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

1962-06-26

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

ELECTRODEPOSITION OF PLUTONIUM

DOEpatents

Wolter, F.J.

1957-09-10

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

Removal of plutonium from hepatic tissue

DOEpatents

Lindenbaum, Arthur; Rosenthal, Marcia W.

1979-01-01

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

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

EPA Pesticide Factsheets

Technical Fact Sheet Analysis Purpose: Qualitative analysis Technique: Alpha spectrometry Method Developed for: Americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in concrete and brick samples Method Selected for: SAM lists this method for qualitative analysis of americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in concrete or brick building materials. Summary of subject analytical method which will be posted to the SAM website to allow access to the method.

METHOD OF SEPARATING PLUTONIUM FROM LANTHANUM FLUORIDE CARRIER

DOEpatents

Watt, G.W.; Goeckermann, R.H.

1958-06-10

An improvement in oxidation-reduction type methods of separating plutoniunn from elements associated with it in a neutron-irradiated uranium solution is described. The method relates to the separating of plutonium from lanthanum ions in an aqueous 0.5 to 2.5 N nitric acid solution by 'treating the solution, at room temperature, with ammonium sulfite in an amount sufficient to reduce the hexavalent plutonium present to a lower valence state, and then treating the solution with H/sub 2/O/sub 2/ thereby forming a tetravalent plutonium peroxide precipitate.

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

DOEpatents

Balthis, J.H.

1961-07-18

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

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

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

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

PROCESS OF MAKING A NEUTRONIC REACTOR FUEL ELEMENT COMPOSITION

DOEpatents

Alter, H.W.; Davidson, J.K.; Miller, R.S.; Mewherter, J.L.

1959-01-13

A process is presented for making a ceramic-like material suitable for use as a nuclear fuel. The material consists of a solid solution of plutonium dioxide in uranium dioxide and is produced from a uranyl nitrate -plutonium nitrate solution containing uraniunm and plutonium in the desired ratio. The uranium and plutonium are first precipitated from the solution by addition of NH/ sub 4/OH and the dried precipitate is then calcined at 600 C in a hydrogen atmosphere to yield the desired solid solution of PuO/sub 2/ in UO/sub 2/.

SEPARATION OF URANIUM, PLUTONIUM AND FISSION PRODUCTS

DOEpatents

Nicholls, C.M.; Wells, I.; Spence, R.

1959-10-13

The separation of uranium and plutonium from neutronirradiated uranium is described. The neutron-irradiated uranium is dissolved in nitric acid to provide an aqueous solution 3N in nitric acid. The fission products of the solution are extruded by treating the solution with dibutyl carbitol substantially 1.8N in nitric acid. The organic solvent phase is separated and neutralized with ammonium hydroxide and the plutonium reduced with hydroxylamine base to the trivalent state. Treatment of the mixture with saturated ammonium nitrate extracts the reduced plutonium and leaves the uranium in the organic solvent.

Radiation from plutonium 238 used in space applications

NASA Technical Reports Server (NTRS)

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

1972-01-01

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

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

DOE PAGES

Rim, Jung H.; Peterson, Dominic S.; Armenta, Claudine E.; ...

2015-05-08

We describe a new analyte extraction technique using Polymer Ligand Film (PLF). PLFs were synthesized to perform direct sorption of analytes onto its surface for direct counting using alpha spectroscopy. The main focus of the new technique is to shorten and simplify the procedure for chemically isolating radionuclides for determination through a radiometric technique. 4'(5')-di-t-butylcyclohexano 18-crown-6 (DtBuCH 18C 6) and 2-ethylhexylphosphonic acid (HEH[EHP]) were examined for plutonium extraction. Di(2-ethyl hexyl) phosphoric acid (HDEHP) were examined for plutonium and uranium extraction. DtBuCH 18C 6 and HEH[EHP] were not effective in plutonium extraction. HDEHP PLFs were effective for plutonium but not formore » uranium.« less

METHOD OF FORMING PLUTONIUM-BEARING CARRIER PRECIPITATES AND WASHING SAME

DOEpatents

Faris, B.F.

1959-02-24

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

Plutonium dissolution process

DOEpatents

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

1996-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2000-07-01

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

Radiation damage and annealing in plutonium tetrafluoride

DOE PAGES

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

2017-08-03

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

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

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

Rudisill, T.S.

1999-08-11

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

Radiological analysis of plutonium glass batches with natural/enriched boron

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

Rainisch, R.

2000-06-22

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

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

NASA Astrophysics Data System (ADS)

Pistner, C.; Liebert, W.; Fujara, F.

2006-06-01

Inert matrix fuels (IMF) with plutonium may play a significant role to dispose of stockpiles of separated plutonium from military or civilian origin. For reasons of reactivity control of such fuels, burnable poisons (BP) will have to be used. The impact of different possible BP candidates (B, Eu, Er and Gd) on the achievable burnup as well as on safety and non-proliferation aspects of IMF are analyzed. To this end, cell burnup calculations have been performed and burnup dependent reactivity coefficients (boron worth, fuel temperature and moderator void coefficient) were calculated. All BP candidates were analyzed for one initial BP concentration and a range of different initial plutonium-concentrations (0.4-1.0 g cm-3) for reactor-grade plutonium isotopic composition as well as for weapon-grade plutonium. For the two most promising BP candidates (Er and Gd), a range of different BP concentrations was investigated to study the impact of BP concentration on fuel burnup. A set of reference fuels was identified to compare the performance of uranium-fuels, MOX and IMF with respect to (1) the fraction of initial plutonium being burned, (2) the remaining absolute plutonium concentration in the spent fuel and (3) the shift in the isotopic composition of the remaining plutonium leading to differences in the heat and neutron rate produced. In the case of IMF, the remaining Pu in spent fuel is unattractive for a would be proliferator. This underlines the attractiveness of an IMF approach for disposal of Pu from a non-proliferation perspective.

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

PubMed

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

2003-11-01

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

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

NASA Astrophysics Data System (ADS)

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

2018-02-01

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

PLUTONIUM-CERIUM-COPPER ALLOYS

DOEpatents

Coffinberry, A.S.

1959-05-12

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

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2012 CFR

2012-01-01

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

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2014 CFR

2014-01-01

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

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2013 CFR

2013-01-01

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

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

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

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

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

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

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

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2010 CFR

2010-01-01

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

Removal of plutonium and americium from alkaline waste solutions

DOEpatents

Schulz, Wallace W.

1979-01-01

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

10 CFR 71.88 - Air transport of plutonium.

Code of Federal Regulations, 2011 CFR

2011-01-01

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

PREPARATION OF HALIDES OF PLUTONIUM

DOEpatents

Garner, C.S.; Johns, I.B.

1958-09-01

A dry chemical method is described for preparing plutonium halides, which consists in contacting plutonyl nitrate with dry gaseous HCl or HF at an elevated temperature. The addition to the reaction gas of a small quantity of an oxidizing gas or a reducing gas will cause formation of the tetra- or tri-halide of plutonium as desired.

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

DOEpatents

Davies, T.H.

1959-12-15

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

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

DOE PAGES

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

2016-12-05

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

Mortality among workers with chronic radiation sickness

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

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

1996-07-01

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

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

DOEpatents

Li, Shelly Xiaowei; Westphal, Brian Robert; Herrmann, Steven Douglas

2015-09-01

A method and device for the real-time, in-situ monitoring of Plutonium content in U--Pu Alloys comprising providing a crucible. The crucible has an interior non-reactive to a metallic U--Pu alloy within said interior of said crucible. The U--Pu alloy comprises metallic uranium and plutonium. The U--Pu alloy is heated to a liquid in an inert or reducing atmosphere. The heated U--Pu alloy is then cooled to a solid in an inert or reducing atmosphere. As the U--Pu alloy is cooled, the temperature of the U--Pu alloy is monitored. A solidification temperature signature is determined from the monitored temperature of the U--Pu alloy during the step of cooling. The amount of Uranium and the amount of Plutonium in the U--Pu alloy is then determined from the determined solidification temperature signature.

Plutonium segregation in glassy aerodynamic fallout from a nuclear weapon test

DOE PAGES

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

2017-01-11

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

K West Basin Sand Filter Backwash Sample Analysis

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

Fiskum, Sandra K.; Smoot, Margaret R.; Coffey, Deborah S.

A sand filter is used to help maintain water clarity at the K West Basin where highly radioactive sludge is stored. Eventually that sand filter will require disposal. The radionuclide content of the solids trapped in the sand filter will affect the selection of the sand filter disposal pathway. The Pacific Northwest National Laboratory (PNNL) was contracted by the K Basin Operations & Plateau Remediation Project (operations contractor CH2M Hill) to analyze the radionuclide content of the solids collected from the backwash of the K West Basin sand filter. The radionuclide composition in the sand filter backwash solids will bemore » used by CH2M Hill to determine if the sand filter media and retained sludge solids will be designated as transuranic waste for disposal purposes or can be processed through less expensive means. On October 19, 2015, K Basin Operations & Plateau Remediation Project staff backwashed the sand filter into the North Load-Out Pit (NLOP) and immediately collected sample slurry from a sampling tube positioned 24 in. above the NLOP floor. The 764 g sand filter backwash slurry sample, KW-105 SFBW-001, was submitted to PNNL for analysis on October 20, 2015. Solids from the slurry sample were consolidated into two samples (i.e., a primary and a duplicate sample) by centrifuging and measured for mass (0.82 g combined – wet centrifuged solids basis) and volume (0.80 mL combined). The solids were a dark brown/orange color, consistent with iron oxide/hydroxide. The solids were dried; the combined dry solids mass was 0.1113 g, corresponding to 0.0146 weight percent (wt%) solids in the original submitted sample slurry. The solids were acid-digested using nitric and hydrochloric acids. Insoluble solids developed upon dilution with 0.5 M HNO 3, corresponding to an average 6.5 wt% of the initial dry solids content. The acid digestate and insoluble solids were analyzed separately by gamma spectrometry. Nominally, 7.7% of the 60Co was present in the insoluble solids; less than 1% of other gamma-emitters (i.e., 137Cs, 154/155Eu, and 241Am) were present in the insoluble solids. Aliquots of the acid digestate were analyzed directly using gamma energy analysis (GEA) and after separations for 238Pu, 239+240Pu, 237Np, and 241Am radioisotopes using alpha energy analysis (AEA). The 90Sr was measured by liquid scintillation counting (LSC) on the Sr-separated fraction. The plutonium isotopic distribution of the acid digestate was analyzed following Pu separations by thermal ionization mass spectrometry (TIMS). A table summarizes the results for the primary and duplicate samples. The 239+240Pu concentration (µCi/g dry) relative to 90Sr and to 137Cs concentrations (µCi/g dry) was examined. The K West Basin sludge has a 239+240Pu/ 90Sr ranging from 0.1 to 1.2 and the 239+240Pu/ 137Cs ratio ranging from 0.10 to 0.47. In contrast, the sand filter backwash solids 239+240Pu/ 90Sr ratio was 10.6 and the 239+240Pu/ 137Cs ratio was 2.0. The ratio differences indicate a relative enhancement of the Pu concentration in the sand filter solids relative to the 137Cs and 90Sr sludge concentrations currently in the K West Basin. A dose-to-curie radioisotope evaluation of the sand filter waste form may need to consider this dissimilarity.« less

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

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

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

1992-12-31

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

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

NASA Astrophysics Data System (ADS)

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

2009-12-01

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

PLUTONIUM ELECTROREFINING CELLS

DOEpatents

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

1963-07-16

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

PLUTONIUM SEPARATION METHOD

DOEpatents

Beaufait, L.J. Jr.; Stevenson, F.R.; Rollefson, G.K.

1958-11-18

The recovery of plutonium ions from neutron irradiated uranium can be accomplished by bufferlng an aqueous solutlon of the irradiated materials containing tetravalent plutonium to a pH of 4 to 7, adding sufficient acetate to the solution to complex the uranyl present, adding ferric nitrate to form a colloid of ferric hydroxide, plutonlum, and associated fission products, removing and dissolving the colloid in aqueous nitric acid, oxldizlng the plutonium to the hexavalent state by adding permanganate or dichromate, treating the resultant solution with ferric nitrate to form a colloid of ferric hydroxide and associated fission products, and separating the colloid from the plutonlum left in solution.

Development of first ever scanning probe microscopy capabilities for plutonium

NASA Astrophysics Data System (ADS)

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

2017-04-01

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

Development of first ever scanning probe microscopy capabilities for plutonium

DOE PAGES

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

2017-04-01

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

URANOUS IODATE AS A CARRIER FOR PLUTONIUM

DOEpatents

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

1959-12-15

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

PLUTONIUM-URANIUM-TITANIUM ALLOYS

DOEpatents

Coffinberry, A.S.

1959-07-28

A plutonium-uranium alloy suitable for use as the fuel element in a fast breeder reactor is described. The alloy contains from 15 to 60 at.% titanium with the remainder uranium and plutonium in a specific ratio, thereby limiting the undesirable zeta phase and rendering the alloy relatively resistant to corrosion and giving it the essential characteristic of good mechanical workability.

High-Temperature Oxidation of Plutonium Surrogate Metals and Alloys

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

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

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

The underwater coincidence counter (UWCC) for plutonium measurements in mixed oxide fuels

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

Eccleston, G.W.; Menlove, H.O.; Abhold, M.

1998-12-31

The use of fresh uranium-plutonium mixed oxide (MOX) fuel in light-water reactors (LWR) is increasing in Europe and Japan and it is necessary to verify the plutonium content in the fuel for international safeguards purposes. The UWCC is a new instrument that has been designed to operate underwater and nondestructively measure the plutonium in unirradiated MOX fuel assemblies. The UWCC can be quickly configured to measure either boiling-water reactor (BWR) or pressurized-water reactor (PWR) fuel assemblies. The plutonium loading per unit length is measured using the UWCC to precisions of less than 1% in a measurement time of 2 tomore » 3 minutes. Initial calibrations of the UWCC were completed on measurements of MOX fuel in Mol, Belgium. The MCNP-REN Monte Carlo simulation code is being benchmarked to the calibration measurements to allow accurate simulations for extended calibrations of the UWCC.« less

TERNARY ALLOY-CONTAINING PLUTONIUM

DOEpatents

Waber, J.T.

1960-02-23

Ternary alloys of uranium and plutonium containing as the third element either molybdenum or zirconium are reported. Such alloys are particularly useful as reactor fuels in fast breeder reactors. The alloy contains from 2 to 25 at.% of molybdenum or zirconium, the balance being a combination of uranium and plutonium in the ratio of from 1 to 9 atoms of uranlum for each atom of plutonium. These alloys are prepared by melting the constituent elements, treating them at an elevated temperature for homogenization, and cooling them to room temperature, the rate of cooling varying with the oomposition and the desired phase structure. The preferred embodiment contains 12 to 25 at.% of molybdenum and is treated by quenching to obtain a body centered cubic crystal structure. The most important advantage of these alloys over prior binary alloys of both plutonium and uranium is the lack of cracking during casting and their ready machinability.

Microprobe Analysis of Pu-Ga Standards

DOE PAGES

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

2017-08-04

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

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

NASA Astrophysics Data System (ADS)

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

2000-07-01

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

Microprobe Analysis of Pu-Ga Standards

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

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

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

PRECIPITATION METHOD OF SEPARATING PLUTONIUM FROM CONTAMINATING ELEMENTS

DOEpatents

Duffield, R.B.

1959-02-24

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

Density of Plutonium Turnings Generated from Machining Activities

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

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

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

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

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

Sehmel, G.A.

1978-01-01

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

PLUTONIUM RECOVERY FROM NEUTRON-BOMBARDED URANIUM FUEL

DOEpatents

Moore, R.H.

1964-03-24

A process of recovering plutonium from fuel by dissolution in molten KAlCl/sub 4/ double salt is described. Molten lithium chloride plus stannous chloride is added to reduce plutonium tetrachloride to the trichloride, which is dissolved in a lithium chloride phase while the uranium, as the tetrachloride, is dissolved in a double-salt phase. Separation of the two phases is discussed. (AEC)

SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS BY ADSORPTION

DOEpatents

Seaborg, G.T.; Willard, J.E.

1958-01-01

A method is presented for the separation of plutonium from solutions containing that element in a valence state not higher than 41 together with uranium ions and fission products. This separation is accomplished by contacting the solutions with diatomaceous earth which preferentially adsorbs the plutonium present. Also mentioned as effective for this adsorbtive separation are silica gel, filler's earth and alumina.

METHOD OF RECOVERING PLUTONIUM VALUES FROM AQUEOUS SOLUTIONS BY CARRIER PRECIPITATION

DOEpatents

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

1959-11-01

A process is presented for pretreating aqueous nitric acid- plutonium solutions containing a small quantity of hydrazine that has formed as a decomposition product during the dissolution of neutron-bombarded uranium in nitric acid and that impairs the precipitation of plutonium on bismuth phosphate. The solution is digested with alkali metal dichromate or potassium permanganate at between 75 and 100 deg C; sulfuric acid at approximately 75 deg C and sodium nitrate, oxaiic acid plus manganous nitrate, or hydroxylamine are added to the solution to secure the plutonium in the tetravalent state and make it suitable for precipitation on BiPO/sub 4/.

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

DOE PAGES

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

2017-10-07

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

METHOD AND MEANS FOR ELECTROLYTIC PURIFICATION OF PLUTONIUM

DOEpatents

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

1960-02-01

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

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

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

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

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

PROCESSING OF NEUTRON-IRRADIATED URANIUM

DOEpatents

Hopkins, H.H. Jr.

1960-09-01

An improved "Purex" process for separating uranium, plutonium, and fission products from nitric acid solutions of neutron-irradiated uranium is offered. Uranium is first extracted into tributyl phosphate (TBP) away from plutonium and fission products after adjustment of the acidity from 0.3 to 0.5 M and heating from 60 to 70 deg C. Coextracted plutonium, ruthenium, and fission products are fractionally removed from the TBP by three scrubbing steps with a 0.5 M nitric acid solution of ferrous sulfamate (FSA), from 3.5 to 5 M nitric acid, and water, respectively, and the purified uranium is finally recovered from the TBP by precipitation with an aqueous solution of oxalic acid. The plutonium in the 0.3 to 0.5 M acid solution is oxidized to the tetravalent state with sodium nitrite and extracted into TBP containing a small amount of dibutyl phosphate (DBP). Plutonium is then back-extracted from the TBP-DBP mixture with a nitric acid solution of FSA, reoxidized with sodium nitrite in the aqueous strip solution obtained, and once more extracted with TBP alone. Finally the plutonium is stripped from the TBP with dilute acid, and a portion of the strip solution thus obtained is recycled into the TBPDBP for further purification.

Selecting a plutonium vitrification process

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

Jouan, A.

1996-05-01

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

Preserving Plutonium-244 as a National Asset

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

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

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

Photoemission Spectroscopy of Delta- Plutonium: Experimental Review

NASA Astrophysics Data System (ADS)

Tobin, J. G.

2002-03-01

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

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

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

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

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

NASA Astrophysics Data System (ADS)

Fisenko, Anatoliy I.; Lemberg, Vladimir F.

2016-09-01

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

Radiation release at the nation's only operating deep geological repository--an independent monitoring perspective.

PubMed

Thakur, P; Ballard, S; Hardy, R

2014-11-04

Recent incidents at the nation's only operating deep geologic nuclear waste repository, the Waste Isolation Pilot Plant (WIPP), resulted in the release of americium and plutonium from one or more defense-related transuranic (TRU) waste containers into the environment. WIPP is a U.S. Department of Energy mined geologic repository that has been in operation since March, 1999. Over 85,000 m3 of waste in various vented payload containers have been emplaced in the repository. The primary radionuclides within the disposed waste are 239+240Pu and 241Am, which account for more than 99% of the total TRU radioactivity disposed and scheduled for disposal in the repository. For the first time in its 15 years of operation, there was an airborne radiation release from the WIPP at approximately 11:30 PM Mountain Standard Time (MST) on Friday, February 14, 2014. The radiation release was likely caused by a chemical reaction inside a TRU waste drum that contained nitrate salts and organic sorbent materials. In a recent news release, DOE announced that photos taken of the waste underground showed evidence of heat and gas pressure resulting in a deformed lid, in material expelled through that deformation, and in melted plastic and rubber and polyethylene in the vicinity of that drum. Recent entries into underground Panel 7 have confirmed that at least one waste drum containing a nitrate salt bearing waste stream from Los Alamos National Laboratory was breached underground and was the most likely source of the release. Further investigation is underway to determine if other containers contributed to the release. Air monitoring across the WIPP site intensified following the first reports of radiation detection underground to ascertain whether or not there were releases to the ground surface. Independent analytical results of air filters from sampling stations on and near the WIPP facility have been released by us at the Carlsbad Environmental Monitoring & Research Center and confirmed trace amounts of 241Am and 239+240Pu, at ratios reflecting the suspect waste stream. The highest activity detected offsite was 115.2 μBq/m3 for 241Am and 10.2 μBq/m3 for 239+240 Pu. These concentrations in air were very small, localized, and below any level of public health or environmental concern.

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

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

NONE

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

Fuel bundle design for enhanced usage of plutonium fuel

DOEpatents

Reese, Anthony P.; Stachowski, Russell E.

1995-01-01

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

Fuel bundle design for enhanced usage of plutonium fuel

DOEpatents

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

1995-08-08

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

PLUTONIUM PROCESSING OPTIMIZATION IN SUPPORT OF THE MOX FUEL PROGRAM

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

GRAY, DEVIN W.; COSTA, DAVID A.

2007-02-02

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

Nuclear Matters. A Practical Guide

DTIC Science & Technology

2008-01-01

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

Density functional theory study of defects in unalloyed δ-Pu

DOE PAGES

Hernandez, S. C.; Freibert, F. J.; Wills, J. M.

2017-03-19

Using density functional theory, we explore in this paper various classical point and complex defects within the face-centered cubic unalloyed δ-plutonium matrix that are potentially induced from self-irradiation. For plutonium only defects, the most energetically stable defect is a distorted split-interstitial. Gallium, the δ-phase stabilizer, is thermodynamically stable as a substitutional defect, but becomes unstable when participating in a complex defect configuration. Finally, complex uranium defects may thermodynamically exist as uranium substitutional with neighboring plutonium interstitial and stabilization of uranium within the lattice is shown via partial density of states and charge density difference plots to be 5f hybridization betweenmore » uranium and plutonium.« less

Method for dissolving delta-phase plutonium

DOEpatents

Karraker, David G.

1992-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2015-04-01

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

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

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

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

1997-04-01

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

Density functional theory study of defects in unalloyed δ-Pu

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

Hernandez, S. C.; Freibert, F. J.; Wills, J. M.

Using density functional theory, we explore in this paper various classical point and complex defects within the face-centered cubic unalloyed δ-plutonium matrix that are potentially induced from self-irradiation. For plutonium only defects, the most energetically stable defect is a distorted split-interstitial. Gallium, the δ-phase stabilizer, is thermodynamically stable as a substitutional defect, but becomes unstable when participating in a complex defect configuration. Finally, complex uranium defects may thermodynamically exist as uranium substitutional with neighboring plutonium interstitial and stabilization of uranium within the lattice is shown via partial density of states and charge density difference plots to be 5f hybridization betweenmore » uranium and plutonium.« less

SPRAY CALCINATION REACTOR

DOEpatents

Johnson, B.M.

1963-08-20

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

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

DOEpatents

Seaborg, G.T.; Blaedel, W.J.; Walling, M.T. Jr.

1960-08-23

A process is given for separating from each other uranium, plutonium, and fission products in an aqueous nitric acid solution by the so-called Redox process. The plutonium is first oxidized to the hexavalent state, e.g., with a water-soluble dichromate or sodium bismuthate, preferably together with a holding oxidant such as potassium bromate. potassium permanganate, or an excess of the oxidizing agent. The solution is then contacted with a water-immiscible organic solvent, preferably hexone. whereby uranium and plutonium are extracted while the fission products remain in the aqueous solution. The separated organic phase is then contacted with an aqueous solution of a reducing agent, with or without a holding reductant (e.g., with a ferrous salt plus hydrazine or with ferrous sulfamate), whereby plutonium is reduced to the trivalent state and back- extracted into the aqueous solution. The uranium may finally be back-extracted from the organic solvent (e.g., with a 0.1 N nitric acid).

Second-order Kinetics of DTPA and Plutonium in Rat Plasma

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

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

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

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

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

Peterson, P.F.

1996-05-01

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

Second-order Kinetics of DTPA and Plutonium in Rat Plasma

DOE PAGES

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

2017-11-15

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

Plutonium Immobilization Project System Design Description for Can Loading System

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

Kriikku, E.

2001-02-15

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

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

DOEpatents

Duffield, R.B.

1959-07-14

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

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

DOEpatents

Jaffey, A.H.; Seaborg, G.T.

1958-12-23

The method for separation of plutonium from uranium and radioactive fission products obtained by neutron irradiation of uranlum consists of reacting the lrradiated material with either bromine, hydrogen bromide, alumlnum bromide, or sulfur and bromine at an elevated temperature to form the bromides of all the elements, then recovering substantlally pure plutonium bromide by dlstillatlon in combinatlon with selective condensatlon at prescribed temperature and pressure.

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

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

HERZOG, K.R.

1999-09-01

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

METHOD OF PREPARING METAL HALIDES

DOEpatents

Hendrickson, A.V.

1958-11-18

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

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

DOEpatents

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

1958-12-16

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

METHOD FOR DISSOLVING LANTHANUM FLUORIDE CARRIER FOR PLUTONIUM

DOEpatents

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

1961-08-01

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

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

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

Delegard, Calvin H.; Casella, Amanda J.

2016-09-30

This report summarizes the literature reviewed on crud formation at the liquid:liquid interface of solvent extraction processes. The review is focused both on classic PUREX extraction for industrial reprocessing, especially as practiced at the Hanford Site, and for those steps specific to plutonium purification that were used at the Plutonium Reclamation Facility (PRF) within the Plutonium Finishing Plant (PFP) at the Hanford Site.

RECOVERY OF Pu VALUES BY FLUORINATION AND FRACTIONATION

DOEpatents

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

1959-01-20

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

METHOD OF PREPARING PLUTONIUM TETRAFLUORIDE

DOEpatents

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

1959-11-17

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

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

DOEpatents

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

1996-01-01

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

Radiation damage and annealing in plutonium tetrafluoride

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

McCoy, Kaylyn; Casella, Amanda; Sinkov, Sergey

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

Resuspension studies in the Marshall Islands.

PubMed

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

1997-07-01

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

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

PubMed

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

2014-08-11

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

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

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

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

1982-02-01

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

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

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

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

1980-11-01

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

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

PubMed

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

2017-05-01

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

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

NASA Astrophysics Data System (ADS)

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

2008-04-01

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

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

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

Lockhart, Madeline Louise; McMath, Garrett Earl

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

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

DOE PAGES

Lockhart, Madeline Louise; McMath, Garrett Earl

2017-10-26

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

Survey of glass plutonium contents and poison selection

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

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

1996-05-01

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

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

NASA Astrophysics Data System (ADS)

Singh, Narayani P.; Zimmerman, Carol J.; Lewis, Laura L.; Wrenn, McDonald E.

1984-06-01

Solvent extraction and alpha-spectrometry have been emplyed in the quantitative simultaneous determination of uranium. thorium and plutonium. The bone specimens, spiked with 232U, 229Th and 242Pu tracers, are wet ashed with HNO 3 followed by alternate additions of a new drops of HNO 3 and H 2O 2. Uranium is reduced to the tetravalent state with 200 mg SnCl 2 and 25 ml HI. Uranium, thorium and plutonium are then coprecipitated with calcium as oxalate, heated to 550°C, dissolved in 50 ml HCl, and the acidity adjusted to 10 M. Uranium and plutonium are extracted into a 20% tri-lauryl amine (TLA) solution in xylene, leaving thorium in the aqueous phase. Plutonium is first back-extracted from the TLA phase by shaking with a 1:1.5 volume of 0.05 M NH 4I in 8 M HCl, which reduces Pu(IV) to Pu(III). Uranium is then back-extracted with an equal volume of 0.1 M HCl. Thorium, which was left in the aqueous phase, is evaporated to dryness, dissolved in 4 M HNO 3, and the acidity adjusted to 4 M. Thorium is then extracted into 20% TLA solution in xylene pre-equilibrated with 4 M HNO 3, and back-extracted with 10 M HCl. Uranium, thorium, and plutonium are then electrodeposited separately onto platinum discs and counted by an alpha-spectrometer with a multi-channel analyzer and surface barrier silicon diodes. The mean recoveries of uranium, thorium, and plutonium in bovine, dog, and human bones were over 70%.

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

PubMed

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

2013-06-01

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

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

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

NONE

1994-04-30

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

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

PubMed

Edwards, Geoffrey W R; Priest, Nicholas D

2014-11-01

The neutron economy and online refueling capability of heavy water moderated reactors enable them to use many different fuel types, such as low enriched uranium, plutonium mixed with uranium, or plutonium and/or U mixed with thorium, in addition to their traditional natural uranium fuel. However, the toxicity and radiological protection methods for fuels other than natural uranium are not well established. A previous paper by the current authors compared the composition and toxicity of irradiated natural uranium to that of three potential advanced heavy water fuels not containing plutonium, and this work uses the same method to compare irradiated natural uranium to three other fuels that do contain plutonium in their initial composition. All three of the new fuels are assumed to incorporate plutonium isotopes characteristic of those that would be recovered from light water reactor fuel via reprocessing. The first fuel investigated is a homogeneous thorium-plutonium fuel designed for a once-through fuel cycle without reprocessing. The second fuel is a heterogeneous thorium-plutonium-U bundle, with graded enrichments of U in different parts of a single fuel assembly. This fuel is assumed to be part of a recycling scenario in which U from previously irradiated fuel is recovered. The third fuel is one in which plutonium and Am are mixed with natural uranium. Each of these fuels, because of the presence of plutonium in the initial composition, is determined to be considerably more radiotoxic than is standard natural uranium. Canadian nuclear safety regulations require that techniques be available for the measurement of 1 mSv of committed effective dose after exposure to irradiated fuel. For natural uranium fuel, the isotope Pu is a significant contributor to the committed effective dose after exposure, and thermal ionization mass spectrometry is sensitive enough that the amount of Pu excreted in urine is sufficient to estimate internal doses, from all isotopes, as low as 1 mSv. In addition, if this method is extended so that Pu is also measured, then the combined amount of Pu and Pu is sufficiently high in the thorium-plutonium fuel that a committed effective dose of 1 mSv would be measurable. However, the fraction of Pu and Pu in the other two fuels is sufficiently low that a 1 mSv dose would remain below the detection limit using this technique. Thus new methods, such as fecal measurements of Pu (or other alpha emitters), will be required to measure exposure to these new fuels.

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

DOEpatents

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

1959-06-30

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

Exploding the myths about the fast breeder reactor

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

Burns, S.

1979-01-01

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

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

DTIC Science & Technology

2001-02-01

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

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

DOEpatents

Beaton, R.H.

1960-06-28

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

Aqueous Chloride Operations Overview: Plutonium and Americium Purification/Recovery

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

Gardner, Kyle Shelton; Kimball, David Bryan; Skidmore, Bradley Evan

These are a set of slides intended for an information session as part of recruiting activities at Brigham Young University. It gives an overview of aqueous chloride operations, specifically on plutonium and americium purification/recovery. This presentation details the steps taken perform these processes, from plutonium size reduction, dissolution, solvent extraction, oxalate precipitation, to calcination. For americium recovery, it details the CLEAR (chloride extraction and actinide recovery) Line, oxalate precipitation and calcination.

SEPARATION PROCESS USING COMPLEXING AND ADSORPTION

DOEpatents

Spedding, J.H.; Ayers, J.A.

1958-06-01

An adsorption process is described for separating plutonium from a solution of neutron-irradiated uranium containing ions of a compound of plutonium and other cations. The method consists of forming a chelate complex compound with plutoniunn ions in the solution by adding a derivative of 8- hydroxyquinoline, which derivative contains a sulfonic acid group, and adsorbing the remaining cations from the solution on a cation exchange resin, while the complexed plutonium remains in the solution.

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

DOEpatents

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

1961-07-01

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

Electrolysis of plutonium nitride in LiCl-KCl eutectic melts

NASA Astrophysics Data System (ADS)

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

2000-01-01

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

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

DOEpatents

Krot, Nikolai N.; Charushnikova, Iraida A.

1997-01-01

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

PYROMETALLURGICAL METHOD

DOEpatents

Nelson, P.A.

1961-07-18

The liquid--liquid extraction of plutonium by magnesium from uranium or uranium--chromium alloy is described. Calcium is added to magnesium in about eutectic proportions, which results in a purer plutonium.

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

PubMed

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

2017-12-01

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

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

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

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

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

NASA Astrophysics Data System (ADS)

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

2015-10-01

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

PLUTONIUM CARRIER METATHESIS WITH ORGANIC REAGENT

DOEpatents

Thompson, S.G.

1958-07-01

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

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

DTIC Science & Technology

2008-03-26

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

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

NASA Astrophysics Data System (ADS)

Marshalkin, V. E.; Povyshev, V. M.

2015-12-01

A method for joint utilization of non-weapons-grade plutonium and highly enriched uranium in the thorium-uranium—plutonium oxide fuel of a water-moderated reactor with a varying water composition (D2O, H2O) is proposed. The method is characterized by efficient breeding of the 233U isotope and safe reactor operation and is comparatively simple to implement.

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

DOE PAGES

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

2016-02-22

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

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

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

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

1996-12-31

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

Introduction to Pits and Weapons Systems (U)

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

Kautz, D.

2012-07-02

A Nuclear Explosive Package includes the Primary, Secondary, Radiation Case and related components. This is the part of the weapon that produces nuclear yield and it converts mechanical energy into nuclear energy. The pit is composed of materials that allow mechanical energy to be converted to electromagnetic energy. Fabrication processes used are typical of any metal fabrication facility: casting, forming, machining and welding. Some of the materials used in pits include: Plutonium, Uranium, Stainless Steel, Beryllium, Titanium, and Aluminum. Gloveboxes are used for three reasons: (1) Protect workers and public from easily transported, finely divided plutonium oxides - (a) Plutoniummore » is very reactive and produces very fine particulate oxides, (b) While not the 'Most dangerous material in the world' of Manhattan Project lore, plutonium is hazardous to health of workers if not properly controlled; (2) Protect plutonium from reactive materials - (a) Plutonium is extremely reactive at ambient conditions with several components found in air: oxygen, water, hydrogen, (b) As with most reactive metals, reactions with these materials may be violent and difficult to control, (c) As with most fabricated metal products, corrosion may significantly affect the mechanical, chemical, and physical properties of the product; and (3) Provide shielding from radioactive decay products: {alpha}, {gamma}, and {eta} are commonly associated with plutonium decay, as well as highly radioactive materials such as {sup 241}Am and {sup 238}Pu.« less

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

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

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

2007-05-01

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

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

PubMed Central

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

2016-01-01

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

LWR First Recycle of TRU with Thorium Oxide for Transmutation and Cross Sections

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

Andrea Alfonsi; Gilles Youinou; Sonat Sen

2013-02-01

Thorium has been considered as an option to uranium-based fuel, based on considerations of resource utilization (thorium is approximately three times more plentiful than uranium) and as a result of concerns about proliferation and waste management (e.g. reduced production of plutonium, etc.). Since the average composition of natural Thorium is dominated (100%) by the fertile isotope Th-232, Thorium is only useful as a resource for breeding new fissile materials, in this case U-233. Consequently a certain amount of fissile material must be present at the start-up of the reactor in order to guarantee its operation. The thorium fuel can bemore » used in both once-through and recycle options, and in both fast and thermal spectrum systems. The present study has been aimed by the necessity of investigating the option of using reprocessed plutonium/TRU, from a once-through reference LEU scenario (50 GWd/ tIHM), mixed with natural thorium and the need of collect data (mass fractions, cross-sections etc.) for this particular fuel cycle scenario. As previously pointed out, the fissile plutonium is needed to guarantee the operation of the reactor. Four different scenarios have been considered: • Thorium – recycled Plutonium; • Thorium – recycled Plutonium/Neptunium; • Thorium – recycled Plutonium/Neptunium/Americium; • Thorium – recycled Transuranic. The calculations have been performed with SCALE6.1-TRITON.« less

LWR First Recycle of TRU with Thorium Oxide for Transmutation and Cross Sections

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

Andrea Alfonsi; Gilles Youinou

2012-07-01

Thorium has been considered as an option to uranium-based fuel, based on considerations of resource utilization (thorium is approximately three times more plentiful than uranium) and as a result of concerns about proliferation and waste management (e.g. reduced production of plutonium, etc.). Since the average composition of natural Thorium is dominated (100%) by the fertile isotope Th-232, Thorium is only useful as a resource for breeding new fissile materials, in this case U-233. Consequently a certain amount of fissile material must be present at the start-up of the reactor in order to guarantee its operation. The thorium fuel can bemore » used in both once-through and recycle options, and in both fast and thermal spectrum systems. The present study has been aimed by the necessity of investigating the option of using reprocessed plutonium/TRU, from a once-through reference LEU scenario (50 GWd/ tIHM), mixed with natural thorium and the need of collect data (mass fractions, cross-sections etc.) for this particular fuel cycle scenario. As previously pointed out, the fissile plutonium is needed to guarantee the operation of the reactor. Four different scenarios have been considered: • Thorium – recycled Plutonium; • Thorium – recycled Plutonium/Neptunium; • Thorium – recycled Plutonium/Neptunium/Americium; • Thorium – recycled Transuranic. The calculations have been performed with SCALE6.1-TRITON.« less

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

Friesen, H.N.

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

Evaluation of continuous air monitor placement in a plutonium facility.

PubMed

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

1997-05-01

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

Safe disposal of surplus plutonium

NASA Astrophysics Data System (ADS)

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

2001-06-01

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

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

PubMed

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

2005-02-01

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

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

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

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

1988-09-01

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

Crystalline matrices for the immobilization of plutonium and actinides

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

Anderson, E.B.; Burakov, E.E.; Galkin, Ya.B.

1996-05-01

The management of weapon plutonium, disengaged as a result of conversion, is considered together with the problem of the actinide fraction of long-lived high level radioactive wastes. It is proposed to use polymineral ceramics based on crystalline host-phases: zircon ZrSiO{sub 4} and zirconium dioxide ZrO{sub 2}, for various variants of the management of plutonium and actinides (including the purposes of long-term safe storage or final disposal from the human activity sphere). It is shown that plutonium and actinides are able to form with these phases on ZrSiO{sub 4} and ZrO{sub 2} was done on laboratory level by the hot pressingmore » method, using the plasmochemical calcination technology. To incorporate simulators of plutonium into the structure of ZrSiO{sub 4} and ZrO{sub 2} in the course of synthesis, an original method developed by the authors as a result of studying the high-uranium zircon (Zr,U) SiO{sub 4} form Chernobyl {open_quotes}lavas{close_quotes} was used.« less

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

NASA Astrophysics Data System (ADS)

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

2017-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Plutonium

NASA Astrophysics Data System (ADS)

Clark, David L.; Hecker, Siegfried S.; Jarvinen, Gordon D.; Neu, Mary P.

The element plutonium occupies a unique place in the history of chemistry, physics, technology, and international relations. After the initial discovery based on submicrogram amounts, it is now generated by transmutation of uranium in nuclear reactors on a large scale, and has been separated in ton quantities in large industrial facilities. The intense interest in plutonium resulted fromthe dual-use scenario of domestic power production and nuclear weapons - drawing energy from an atomic nucleus that can produce a factor of millions in energy output relative to chemical energy sources. Indeed, within 5 years of its original synthesis, the primary use of plutonium was for the release of nuclear energy in weapons of unprecedented power, and it seemed that the new element might lead the human race to the brink of self-annihilation. Instead, it has forced the human race to govern itself without resorting to nuclear war over the past 60 years. Plutonium evokes the entire gamut of human emotions, from good to evil, from hope to despair, from the salvation of humanity to its utter destruction. There is no other element in the periodic table that has had such a profound impact on the consciousness of mankind.

49 CFR 176.2 - Definitions.

Code of Federal Regulations, 2012 CFR

2012-10-01

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

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

DOEpatents

Ackerman, John P.; Miller, William E.

1989-01-01

An electrorefining process and apparatus for the recovery of uranium and a mixture of uranium and plutonium from spent fuel using an electrolytic cell having a lower molten cadmium pool containing spent nuclear fuel, an intermediate electrolyte pool, an anode basket containing spent fuel, and two cathodes, the first cathode composed of either a solid alloy or molten cadmium and the second cathode composed of molten cadmium. Using this cell, additional amounts of uranium and plutonium from the anode basket are dissolved in the lower molten cadmium pool, and then substantially pure uranium is electrolytically transported and deposited on the first alloy or molten cadmium cathode. Subsequently, a mixture of uranium and plutonium is electrotransported and deposited on the second molten cadmium cathode.

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

DOEpatents

Ackerman, J.P.; Miller, W.E.

1987-11-05

An electrorefining process and apparatus for the recovery of uranium and a mixture of uranium and plutonium from spent fuels is disclosed using an electrolytic cell having a lower molten cadmium pool containing spent nuclear fuel, an intermediate electrolyte pool, an anode basket containing spent fuels, two cathodes and electrical power means connected to the anode basket, cathodes and lower molten cadmium pool for providing electrical power to the cell. Using this cell, additional amounts of uranium and plutonium from the anode basket are dissolved in the lower molten cadmium pool, and then purified uranium is electrolytically transported and deposited on a first molten cadmium cathode. Subsequently, a mixture of uranium and plutonium is electrotransported and deposited on a second cathode. 3 figs.

Ceramics: Durability and radiation effects

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

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

1996-05-01

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

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

Not Available

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

A fast semi-quantitative method for Plutonium determination in an alpine firn/ice core

NASA Astrophysics Data System (ADS)

Gabrieli, J.; Cozzi, G.; Vallelonga, P.; Schwikowski, M.; Sigl, M.; Boutron, C.; Barbante, C.

2009-04-01

Plutonium is present in the environment as a consequence of atmospheric nuclear tests carried out in the 1960s, nuclear weapons production and releases by the nuclear industry over the past 50 years. Plutonium, unlike uranium, is essentially anthropogenic and it was first produced and isolated in 1940 by deuteron bombardment of uranium in the cyclotron of Berkeley University. It exists in five main isotopes, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, derived from civilian and military sources (weapons production and detonation, nuclear reactors, nuclear accidents). In the environment, 239Pu is the most abundant isotope. Approximately 6 tons of 239Pu have been released into the environment as a result of 541 atmospheric weapon tests Nuclear Pu fallout has been studied in various environmental archives, such as sediments, soil and herbarium grass. Mid-latitude ice cores have been studied as well, on Mont Blanc, the Western Alps and on Belukha Glacier, Siberian Altai. We present a Pu record obtained by analyzing 52 discrete samples of an alpine firn/ice core from Colle Gnifetti (M. Rosa, 4450 m a.s.l.), dating from 1945 to 1991. The239Pu signal was recorded directly, without preliminary cleaning or preconcentration steps, using an ICP-SFMS (Thermo Element2) equipped with a desolvation system (APEX). 238UH+ interferences were negligible for U concentrations lower than 50 ppt as verified both in spiked fresh snow and pre-1940 ice samples. The shape of 239Pu profile reflects the three main periods of atmospheric nuclear weapons testing: the earliest peak starts in 1954/55 to 1958 and includes the first testing period which reached a maximum in 1958. Despite a temporary halt in testing in 1959/60, the Pu concentration decreased only by half with respect to the 1958 peak. In 1961/62 Pu concentrations rapidly increased reaching a maximum in 1963, which was about 40% more intense than the 1958 peak. After the sign of the "Limited Test Ban Treaty" between USA and URSS in 1964, Pu deposition decreased very sharply reaching a minimum in 1967. The third period (1967-1975) is characterized by irregular Pu profiles with smaller peaks (about 20-30% compared to the 1964 peak) which could be due to French and Chinese tests. Comparison with the Pu profiles obtained from the Col du Dome and Belukha ice cores by AMS (Accelerator Mass Spectrometry) shows very good agreement. Considering the semi-quantitative method and the analytical uncertainty, the results are also quantitatively comparable. However, the Pu concentrations at Colle Gnifetti are normally 2-3 times greater than in Col du Dome. This could be explained by different air mass transport or, more likely, different accumulation rates at each site.

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

DTIC Science & Technology

2015-10-30

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

PRECIPITATION METHOD OF SEPARATION OF NEPTUNIUM

DOEpatents

Magnusson, L.B.

1958-07-01

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

Lens of Eye Dosimetry

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

Mallett, Michael Wesley

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

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

NASA Technical Reports Server (NTRS)

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

1972-01-01

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

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

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

Marshalkin, V. E., E-mail: marshalkin@vniief.ru; Povyshev, V. M.

A method for joint utilization of non-weapons-grade plutonium and highly enriched uranium in the thorium–uranium—plutonium oxide fuel of a water-moderated reactor with a varying water composition (D{sub 2}O, H{sub 2}O) is proposed. The method is characterized by efficient breeding of the {sup 233}U isotope and safe reactor operation and is comparatively simple to implement.

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

NASA Astrophysics Data System (ADS)

Marshalkin, V. Ye.; Povyshev, V. M.

2017-12-01

It is shown for a closed thorium-uranium-plutonium fuel cycle that, upon processing of one metric ton of irradiated fuel after each four-year campaign, the radioactive wastes contain 54 kg of fission products, 0.8 kg of thorium, 0.10 kg of uranium isotopes, 0.005 kg of plutonium isotopes, 0.002 kg of neptunium, and "trace" amounts of americium and curium isotopes. This qualitatively simplifies the handling of high-level wastes in nuclear power engineering.

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

DOEpatents

Brown, H.S.; Seaborg, G.T.

1959-02-24

The separation of plutonium and uranium from each other and from other substances is described. In general, the method comprises the steps of contacting the uranium with chlorine in the presence of a holdback material selected from the group consisting of lanthanum oxide and thorium oxide to form a uranium chloride higher than uranium tetrachloride, and thereafter heating the uranium chloride thus formed to a temperature at which the uranium chloride is volatilized off but below the volatilizalion temperature of plutonium chloride.

SCAVENGER AND PROCESS OF SCAVENGING

DOEpatents

Olson, C.M.

1960-04-26

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

METHOD FOR REMOVING CONTAMINATION FROM PRECIPITATES

DOEpatents

Stahl, G.W.

1959-01-01

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

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

DOEpatents

Davidson, J.K.; Robb, W.L.; Salmon, O.N.

1960-11-22

A method is given for forming compositions, as well as the compositions themselves, employing uranium hydride in a liquid bismuth composition to increase the solubility of uranium, plutonium and thorium oxides in the liquid bismuth. The finely divided oxide of uranium, plutonium. or thorium is mixed with the liquid bismuth and uranium hydride, the hydride being present in an amount equal to about 3 at. %, heated to about 5OO deg C, agitated and thereafter cooled and excess resultant hydrogen removed therefrom.

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

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

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

2006-08-01

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

METHOD OF DISSOLVING MASSIVE PLUTONIUM

DOEpatents

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

1960-06-28

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

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

DOEpatents

McCuaig, Franklin D.

1977-01-01

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

Pu-ZR Alloy high-temperature activation-measurement foil

DOEpatents

McCuaig, Franklin D.

1977-08-02

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

Separation by solvent extraction

DOEpatents

Holt, Jr., Charles H.

1976-04-06

17. A process for separating fission product values from uranium and plutonium values contained in an aqueous solution, comprising adding an oxidizing agent to said solution to secure uranium and plutonium in their hexavalent state; contacting said aqueous solution with a substantially water-immiscible organic solvent while agitating and maintaining the temperature at from -1.degree. to -2.degree. C. until the major part of the water present is frozen; continuously separating a solid ice phase as it is formed; separating a remaining aqueous liquid phase containing fission product values and a solvent phase containing plutonium and uranium values from each other; melting at least the last obtained part of said ice phase and adding it to said separated liquid phase; and treating the resulting liquid with a new supply of solvent whereby it is practically depleted of uranium and plutonium.

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

PubMed

McDowell, W J; Farrar, D T; Billings, M R

1974-12-01

A method for the determination of uranium and plutonium by a combined high-resolution liquid scintillation-solvent extraction method is presented. Assuming a sample count equal to background count to be the detection limit, the lower detection limit for these and other alpha-emitting nuclides is 1.0 dpm with a Pyrex sample tube, 0.3 dpm with a quartz sample tube using present detector shielding or 0.02 d.p.m. with pulse-shape discrimination. Alpha-counting efficiency is 100%. With the counting data presented as an alpha-energy spectrum, an energy resolution of 0.2-0.3 MeV peak half-width and an energy identification to +/-0.1 MeV are possible. Thus, within these limits, identification and quantitative determination of a specific alpha-emitter, independent of chemical separation, are possible. The separation procedure allows greater than 98% recovery of uranium and plutonium from solution containing large amounts of iron and other interfering substances. In most cases uranium, even when present in 10(8)-fold molar ratio, may be quantitatively separated from plutonium without loss of the plutonium. Potential applications of this general analytical concept to other alpha-counting problems are noted. Special problems associated with the determination of plutonium in soil and water samples are discussed. Results of tests to determine the pulse-height and energy-resolution characteristics of several scintillators are presented. Construction of the high-resolution liquid scintillation detector is described.