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.

Neutron Capture Cross Section Measurement on $$^{238}$$Pu at DANCE

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

Chyzh, A; Wu, C Y

2011-02-14

The proposed neutron capture measurement for {sup 238}Pu was carried out in Nov-Dec, 2010, using the DANCE array at LANSCE, LANL. The total beam-on-target time is about 14 days plus additional 5 days for the background measurement. The target was prepared at LLNL with the new electrplating cell capable of plating the {sup 238}Pu isotope simultaneously on both sides of the 3-{micro}m thick Ti backing foil. A total mass of 395 {micro}g with an activity of 6.8 mCi was deposited onto the area of 7 mm in diameter. The {sup 238}Pu sample was enriched to 99.35%. The target was coveredmore » by 1.4 {micro}m double-side aluminized mylar and then inserted into a specially designed vacuum-tight container, shown in Fig. 1, for the {sup 238}Pu containment. The container was tested for leaks in the vacuum chamber at LLNL. An identical container without {sup 238}Pu was made as well and used as a blank for the background measurement.« less

Short Lived Fission Product Yield Measurements in 235U, 238U and 239Pu

NASA Astrophysics Data System (ADS)

Silano, Jack; Tonchev, Anton; Tornow, Werner; Krishichayan, Fnu; Finch, Sean; Gooden, Matthew; Wilhelmy, Jerry

2017-09-01

Yields of short lived fission products (FPYs) with half lives of a few minutes to an hour contain a wealth of information about the fission process. Knowledge of short lived FPYs would contribute to existing data on longer lived FPY mass and charge distributions. Of particular interest are the relative yields between the ground states and isomeric states of FPYs since these isomeric ratios can be used to determine the angular momentum of the fragments. Over the past five years, a LLNL-TUNL-LANL collaboration has made precision measurements of FPYs from quasi-monoenergetic neutron induced fission of 235U, 238U and 239Pu. These efforts focused on longer lived FPYs, using a well characterized dual fission chamber and several days of neutron beam exposure. For the first time, this established technique will be applied to measuring short lived FPYs, with half lives of minutes to less than an hour. A feasibility study will be performed using irradiation times of < 1 hour, improving the sensitivity to short lived FPYs by limiting the buildup of long lived isotopes. Results from this exploratory study will be presented, and the implications for isomeric ratio measurements will be discussed. This work was performed under the auspices of US DOE by LLNL under Contract DE-AC52-07NA27344.

Data Evaluation of Actinide Cross Sections: 238Pu, 237Pu, and 236Pu

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

Guaglioni, S.; Jurgenson, E.; Descalle, M. A.

This report documents the recent evaluation of the 236Pu, 237Pu, and 238Pu cross section sets. Nuclear data evaluation is the fundamental interface that takes measured nuclear cross section data and turns them into a continuous curve that 1) is consistent with other measurements and nuclear reaction theory/models, and 2) is required by down-stream users. All experiments that generate nuclear data need to include an evaluation step for their data to be broadly useful to the end users.

Economical Production of Pu-238: NIAC Phase I Final Report

NASA Technical Reports Server (NTRS)

Howe, Steven D.; Crawford, Douglas; Navarro, Jorge; O'Brien, Robert C.; Katalenich, Jeff; Ring, Terry

2016-01-01

All space exploration missions traveling beyond Jupiter must use radioisotopic power sources for electrical power. The best isotope to power these sources is plutonium-238 (Pu-238). The US supply of Pu-238 is almost exhausted and will be gone within the next decade. The Department of Energy has initiated a production program with a $10M allocation from NASA but the cost is estimated at over $100M to get to production levels. The Center for Space Nuclear Research (CSNR) has conceived of a potentially better process to produce Pu-238 earlier and for significantly less cost. Potentially, the front end capital costs could be provided by private industry such that the government only had to pay for the product produced. In the Phase I NIAC (NASA Innovative Advanced Concepts) grant, the CSNR has evaluated the feasibility of using a low power, commercially available nuclear reactor to produce 1.5 kg of Pu-238 per year. The impact on the neutronics of the reactor have been assessed, the amount of Neptunium target material estimated, and the production rates calculated. In addition, the size of the post-irradiation processing facility has been established. Finally, as the study progressed, a new method for fabricating the Pu-238 product into the form used for power sources has been identified to reduce the cost of the final product. In short, the concept appears to be viable, can produce the amount of Pu-238 needed to support the NASA missions, can be available within a few years, and will cost significantly less than the current DOE program.

Equipment upgrades for the Pu-238 program

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

Congdon, J.W.; Stephens, W.D.; Marra, J.E.

1990-02-14

Much of the equipment and instrumentation in the Pu-238 production facilities is more than 15 years old. Significant improvements have been made in the available instrumentation, in particular, due to the application of microprocessors and lasers. The Actinide Technology Section of SRL has selected and is in the process of evaluating several state-of-the-art instruments which have potential applications in the Pu-238 program. The ease of operation and the accuracy of the instruments have been improved and, in most cases, the cost of the instruments have decreased. 5 refs.

The Association of Inbreeding With Lung Fibrosis Incidence in Beagle Dogs That Inhaled 238PuO2 or 239PuO2.

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

Wilson, Dulaney A.; Brigantic, Andrea M.; Morgan, William F.

Studies of health effects in animals after exposure to internally deposited radionuclides were intended to supplement observational studies in humans. Both nuclear workers and Beagle dogs have exhibited plutonium associated lung fibrosis; however, the dogs smaller gene pool may limit the applicability of findings to humans. Data on Beagles that inhaled either plutonium-238 dioxide (238PuO2) or plutonium-239 dioxide (239PuO2) were analyzed. Wright's Coefficient of Inbreeding was used to measure genetic or familial susceptibility and was assessed as an explanatory variable when modeling the association between lung fibrosis incidence and plutonium exposure. Lung fibrosis was diagnosed in approximately 80% of themore » exposed dogs compared with 23.7% of the control dogs. The maximum degree of inbreeding was 9.4%. Regardless of isotope, the addition of inbreeding significantly improved the model in female dogs but not in males. In female dogs an increased inbreeding coefficient predicted decreased hazard of a lung fibrosis diagnosis. Lung fibrosis was common in these dogs with inbreeding affecting models of lung fibrosis incidence in females but not in males. The apparent protective effect in females predicted by these models of lung fibrosis incidence is likely to be minimal given the small degree of inbreeding in these groups.« less

Photo-fission Product Yield Measurements at Eγ=13 MeV on 235U, 238U, and 239Pu

NASA Astrophysics Data System (ADS)

Tornow, W.; Bhike, M.; Finch, S. W.; Krishichayan, Fnu; Tonchev, A. P.

2016-09-01

We have measured Fission Product Yields (FPYs) in photo-fission of 235U, 238U, and 239Pu at TUNL's High-Intensity Gamma-ray Source (HI γS) using mono-energetic photons of Eγ = 13 MeV. Details of the experimental setup and analysis procedures will be discussed. Yields for approximately 20 fission products were determined. They are compared to neutron-induced FPYs of the same actinides at the equivalent excitation energies of the compound nuclear systems. In the future photo-fission data will be taken at Eγ = 8 . 0 and 10.5 MeV to find out whether photo-fission exhibits the same so far unexplained dependence of certain FPYs on the energy of the incident probe, as recently observed in neutron-induced fission, for example, for the important fission product 147Nd. Work supported by the U. S. Dept. of Energy, under Grant No. DE-FG02-97ER41033, and by the NNSA, Stewardship Science Academic Alliances Program, Grant No. DE-NA0001838 and the Lawrence Livermore, National Security, LLC under Contract No. DE-AC52-07NA27344.

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.

European roe deer antlers as an environmental archive for fallout (236)U and (239)Pu.

PubMed

Froehlich, M B; Steier, P; Wallner, G; Fifield, L K

2016-01-01

Anthropogenic (236)U and (239)Pu were measured in European roe deer antlers hunted between 1955 and 1977 which covers and extends beyond the period of intensive nuclear weapons testing (1954-1962). The antlers were hunting trophies, and hence the hunting area, the year of shooting and the approximate age of each animal is given. Uranium and plutonium are known to deposit in skeletal tissue. Since antler histology is similar to bone, both elements were expected in antlers. Furthermore, roe deer shed their antlers annually, and hence antlers may provide a time-resolved environmental archive for fallout radionuclides. The radiochemical procedure is based on a Pu separation step by anion exchange (Dowex 1 × 8) and a subsequent U purification by extraction chromatography using UTEVA(®). The samples were measured by Accelerator Mass Spectrometry at the VERA facility (University of Vienna). In addition to the (236)U and (239)Pu concentrations, the (240)Pu/(239)Pu isotopic ratios were determined with a mean value of 0.172 ± 0.023 which is in agreement with the ratio of global fallout (∼0.18). Rather high (236)U/(238)U ratios of the order of 10(-6) were observed. These measured ratios, where the (236)U arises only from global fallout, have implications for the use of the (236)U/(238)U ratio as a fingerprint for nuclear accidents or releases from nuclear facilities. Our investigations have shown the potential to use antlers as a temporally resolved archive for the uptake of actinides from the environment. Copyright © 2015 Elsevier Ltd. All rights reserved.

Characterization of Pu-238 Heat Source Granule Containment

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

Richardson, Paul Dean II; Sanchez, Joey Leo; Wall, Angelique Dinorah

The Milliwatt Radioisotopic Themoelectric Generator (RTG) provides power for permissive-action links. Essentially these are nuclear batteries that convert thermal energy to electrical energy using a doped silicon-germanium thermopile. The thermal energy is provided by a heat source made of 238Pu, in the form of 238PuO 2 granules. The granules are contained by 3 layers of encapsulation. A thin T-111 liner surrounds the 238PuO 2 granules and protects the second layer (strength member) from exposure to the fuel granules. An outer layer of Hastalloy-C protects the T-111 from oxygen embrittlement. The T-111 strength member is considered the critical component in thismore » 238PuO 2 containment system. Any compromise in the strength member seen during destructive testing required by the RTG surveillance program is characterized. The T-111 strength member is characterized through Scanning Electron Microscopy (SEM), and Metallography. SEM is used in the Secondary Electron mode to reveal possible grain boundary deformation and/or cracking in the region of the strength member weld. Deformation and cracking uncovered by SEM are further characterized by Metallography. Metallography sections are mounted and polished, observed using optical microscopy, then documented in the form of microphotographs. SEM mat further be used to examine polished Metallography mounts to characterize elements using the SEM mode of Energy Dispersive X-ray spectroscopy (EDS).« less

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

NASA Astrophysics Data System (ADS)

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

2005-02-01

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

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

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

Remerowski, Mary Lynn; Dozhier, C.; Krenek, K.

2005-02-06

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

Rapid dating of recent aquatic sediments using Pu activities and 240Pu/239Pu as determined by quadrupole inductively coupled plasma mass spectrometry.

PubMed

Ketterer, Michael E; Watson, Bridgette R; Matisoff, Gerald; Wilsont, Christopher G

2002-03-15

Quadrupole inductively coupled plasma mass spectrometry has been used to rapidly establish the chronology of recent aquatic sediments via measurements of the activities of 239Pu, 240Pu, and the atom ratio 240Pu/239Pu. Following addition of 0.007 Bq of a 242Pu spike isotope, Pu is leached from 3-20 g aliquots of dry-ashed sediments with HNO3. A selective anion exchanger is used to preconcentrate Pu into approximately 2 mL aliquots, which are directly analyzed using a pneumatic nebulizer and double-pass spraychamber operating at 60 microL/min solution uptake rate. The ICPMS data collection is performed for 10 min per sample. The U concentrations were 0.01-0.05 microg/L in the analyzed solutions, and the interference of 238U1H+ upon 239Pu+ was negligible. The method has been applied to determining Pu activities, inventory, and 240Pu/239Pu in a complete sediment core from Old Woman Creek (Huron, OH). The Pu activity profiles, obtained in approximately 6 h of instrumental measurement time, are in agreement with a y spectrometric 137Cs profile. Peak 239+240Pu and 137Cs activities in the core were 1.60 +/- 0.02 and 47.8 +/- 0.8 Bq/kg, respectively; inventories were 108 +/- 2 Bq/m2 239+240Pu and 2710 +/- 40 Bq/m2 137Cs. Detection limits, based upon the analysis of 20 g samples, were 0.004 Bq/kg 239Pu, 0.012 Bq/kg 240Pu, and 0.012 Bq/kg 239+240Pu. 240Pu/239Pu atom ratios of 0.16-0.19 were obtained for all core intervals containing detectable Pu, which indicates that global fallout is the source of these radionuclides.

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

Exploratory study of fission product yields of neutron-induced fission of U 235 ,   U 238 , and Pu 239 at 8.9 MeV

DOE PAGES

Bhatia, C.; Fallin, B. F.; Gooden, M. E.; ...

2015-06-05

Using dual-fission chambers each loaded with a thick (200–400–mg/cm 2) actinide target of 235,238U or 239Pu and two thin (~10–100–μg/cm 2) reference foils of the same actinide, the cumulative yields of fission products ranging from 92Sr to 147Nd have been measured at E n = 8.9MeV. The 2H(d,n) 3He reaction provided the quasimonoenergetic neutron beam. Here, the experimental setup and methods used to determine the fission product yield (FPY) are described, and results for typically eight high-yield fission products are presented.

Characterization of Pu-238 heat source granule containment

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

Richardson Ii, P D; Thronas, D L; Romero, J P

2008-01-01

The Milliwatt Radioisotopic Thermoelectric Generator (RTG) provides power for permissive-action links. These nuclear batteries convert thermal energy to electrical energy using a doped silicon-germanium thermopile. The thermal energy is provided by a heat source made of {sup 238}Pu, in the form of {sup 238}PuO{sub 2} granules. The granules are contained in 3 layers of encapsulation. A thin T-111 liner surrounds the {sup 238}PuO{sub 2} granules and protects the second layer (strength member) from exposure to the fuel granules. The T-111 strength member contains the fuel under impact condition. An outer clad of Hastelloy-C protects the T-111 from oxygen embrittlement. Themore » T-111 strength member is considered the critical component in this {sup 238}PuO{sub 2} containment system. Any compromise in the strength member is something that needs to be characterized. Consequently, the T-111 strength member is characterized upon it's decommissioning through Scanning Electron Microscopy (SEM), and Metallography. SEM is used in Secondary Electron mode to reveal possible grain boundary deformation and/or cracking in the region of the strength member weld. Deformation and cracking uncovered by SEM are further characterized by Metallography. Metallography sections are mounted and polished, observed using optical microscopy, then documented in the form of photomicrographs. SEM may further be used to examine polished Metallography mounts to characterize elements using the SEM mode of Energy Dispersive X-ray Spectroscopy (EDS). This paper describes the characterization of the metallurgical condition of decommissioned RTG heat sources.« less

Plutonium 238/239 Decorporation Model

DTIC Science & Technology

2014-10-01

distribution in tissue compartments over time with and without treatment, excretion rates, and radiation doses to critical organs. Calculations from...kPa) pound- mass -foot2 (moment of inertia) 4.214 011 x E – 2 kilogram-meter2 (kg*m2) pound- mass /foot3 1.601 846 x E + 1 kilogram/m3 (kg/m3) rad...45 Figure 21. Acute Doses to Critical Organs from Pu-238 and Pu-239 Over 90 Days ................... 46 Figure 22. Doses

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 and /sup 242/Pu relative /sup 235/U at 14. 74 MeV neutron energy

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

Meadows, J.W.

1986-12-01

The measurement of the fission cross section ratios of nine isotopes relative to /sup 235/U at an average neutron energy of 14.74 MeV is described with particular attention to the determination of corrections and to sources of error. The results are compared to ENDF/B-V and to other measurements of the past decade. The ratio of the neutron induced fission cross section for these isotopes to the fission cross section for /sup 235/U are: /sup 230/Th - 0.290 +- 1.9%; /sup 232/Th - 0.191 +- 1.9%; /sup 233/U - 1.132 +- 0.7%; /sup 234/U - 0.998 +- 1.0%; /sup 236/U -more » 0.791 +- 1.1%; /sup 238/U - 0.587 +- 1.1%; /sup 237/Np - 1.060 +- 1.4%; /sup 239/Pu - 1.152 +- 1.1%; /sup 242/Pu - 0.967 +- 1.0%. 40 refs., 11 tabs., 9 figs.« less

Determining Pu-239 content by resonance transmission analysis using a filtered reactor beam.

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

Klann, R. T.

A novel technique has been developed at Argonne National Laboratory to determine the {sup 239}Pu content in EBR-II blanket elements using resonance transmission analysis (RTA) with a filtered reactor beam. The technique uses cadmium and gadolinium filters along with a {sup 239}Pu fission chamber to isolate the 0.3 eV resonance in {sup 239}Pu. In the energy range from 0.1 to 0.5 eV, the total microscopic cross-section of {sup 239}Pu is significantly larger than the cross-sections of {sup 238}U and {sup 235}U. This large difference in cross-section allows small amounts of {sup 239}Pu to be detected in uranium samples. Tests usingmore » a direct beam from a 250 kW TRIGA reactor have been performed with stacks of depleted uranium and {sup 239}Pu foils. Preliminary measurement results are in good agreement with the predicted results up to about two weight percent of {sup 239}Pu in the sample. In addition, measured {sup 239}Pu masses were in agreement with actual sample masses with uncertainties less than 3.8 percent.« less

High-Resolution Inductively Coupled Plasma Optical Emission Spectrometry for (234)U/(238)Pu Age Dating of Plutonium Materials and Comparison to Sector Field Inductively Coupled Plasma Mass Spectrometry.

PubMed

Krachler, Michael; Alvarez-Sarandes, Rafael; Rasmussen, Gert

2016-09-06

Employing a commercial high-resolution inductively coupled plasma optical emission spectrometry (HR-ICP-OES) instrument, an innovative analytical procedure for the accurate determination of the production age of various Pu materials (Pu powder, cardiac pacemaker battery, (242)Cm heat source, etc.) was developed and validated. This undertaking was based on the fact that the α decay of (238)Pu present in the investigated samples produced (234)U and both mother and daughter could be identified unequivocally using HR-ICP-OES. Benefiting from the high spectral resolution of the instrument (<5 pm) and the isotope shift of the emission lines of both nuclides, (234)U and (238)Pu were selectively and directly determined in the dissolved samples, i.e., without a chemical separation of the two analytes from each other. Exact emission wavelengths as well as emission spectra of (234)U centered around λ = 411.590 nm and λ = 424.408 nm are reported here for the first time. Emission spectra of the isotopic standard reference material IRMM-199, comprising about one-third each of (233)U, (235)U, and (238)U, confirmed the presence of (234)U in the investigated samples. For the assessment of the (234)U/(238)Pu amount ratio, the emission signals of (234)U and (238)Pu were quantified at λ = 424.408 nm and λ = 402.148 nm, respectively. The age of the investigated samples (range: 26.7-44.4 years) was subsequently calculated using the (234)U/(238)Pu chronometer. HR-ICP-OES results were crossed-validated through sector field inductively coupled plasma mass spectrometry (SF-ICPMS) analysis of the (234)U/(238)Pu amount ratio of all samples applying isotope dilution combined with chromatographic separation of U and Pu. Available information on the assumed ages of the analyzed samples was consistent with the ages obtained via the HR-ICP-OES approach. Being based on a different physical detection principle, HR-ICP-OES provides an alternative strategy to the well-established mass

Automated Metrology System for Pu 238

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

Wunderlich, Richard J.

Under a collaborative partnership between the NASA and DOE, a new automated measurement system developed by ORNL will ensure quality production of plutonium-238 while reducing handling by workers. NASA has funded ORNL and other national laboratories to develop a process that will restore US production capability of Pu-238 for the first time since the late 1980s when the Savannah River Plant ceased production. ORNL has produced and separated about 100 grams of the material and plans to scale up the process over the next several years to meet demand to power NASA deep space missions.

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

PubMed

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

2017-10-01

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

Isotopic fission-fragment distributions of 238U, 239Np, 240Pu, 244Cm, and 250Cf produced through inelastic scattering, transfer, and fusion reactions in inverse kinematics

NASA Astrophysics Data System (ADS)

Ramos, D.; Caamaño, M.; Farget, F.; Rodríguez-Tajes, C.; Audouin, L.; Benlliure, J.; Casarejos, E.; Clement, E.; Cortina, D.; Delaune, O.; Derkx, X.; Dijon, A.; Doré, D.; Fernández-Domínguez, B.; de France, G.; Heinz, A.; Jacquot, B.; Navin, A.; Paradela, C.; Rejmund, M.; Roger, T.; Salsac, M.-D.; Schmitt, C.

2018-05-01

Transfer- and fusion-induced fission in inverse kinematics has proved to be a powerful tool to investigate nuclear fission, widening information on the fission fragments and access to unstable fissioning systems with respect to other experimental approaches. An experimental campaign is being carried out at GANIL with this technique since 2008. In these experiments, a beam of 238U, accelerated to 6.1 MeV/u, impinges on a 12C target. Fissioning systems from U to Cf are populated through inelastic scattering, transfer, and fusion reactions, with excitation energies that range from a few MeV up to 46 MeV. The use of inverse kinematics, the SPIDER telescope, and the VAMOS spectrometer allow the characterization of the fissioning system in terms of mass, nuclear charge, and excitation energy, and the isotopic identification of the full fragment distribution. This work reports on new data from the second experiment of the campaign on fission-fragment yields of the heavy actinides 238U, 239Np, 240Pu, 244Cm, and 250Cf, which are of interest from both fundamental and application points of view.

Alpha and conversion electron spectroscopy of 238,239Pu and 241Am and alpha-conversion electron coincidence measurements

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

Dion, Michael P.; Miller, Brian W.; Warren, Glen A.

2016-09-01

A technique to determine the isotopics of a mixed actinide sample has been proposed by measuring the coincidence of the alpha particle during radioactive decay with the conversion electron (or Auger) emitted during the relaxation of the daughter isotope. This presents a unique signature to allow the deconvolution of isotopes that possess overlapping alpha particle energy. The work presented here are results of conversion electron spectroscopy of 241Am, 238Pu and 239Pu using a dual-stage peltier-cooled 25 mm2 silicon drift detector. A passivated ion implanted planar silicon detector provided measurements of alpha spectroscopy. The conversion electron spectra were evaluated from 20–55more » keV based on fits to the dominant conversion electron emissions, which allowed the relative conversion electron emission intensities to be determined. These measurements provide crucial singles spectral information to aid in the coincident measurement approach.« less

Search for electron and gamma-ray decay of the ^238fPu fission

NASA Astrophysics Data System (ADS)

Beausang, C. W.; Gurdal, G.; Ressler, J.; Barton, C. J.; Caprio, M. A.; Casten, R. F.; Cooper, J. R.; Hecht, A. A.; Hutter, C.; Zamfir, N. V.; Hauschild, K.; Korten, W.; Mergel, E.

2002-04-01

The reaction ^9Be + ^232Th arrow ^241Pu, at beam energies of 50 and 55 MeV, was used in an attempt to populate states in the second minimum (fission isomer) of ^238Pu via the 3n evaporation channel. Prompt gamma-rays, detected using YRAST Ball and conversion electrons, detected using ICE Ball, were collected in coincidence with delayed fission events measured using elements of the Yale SCARY array of solar cell detectors. The solar cell detectors were shielded so as not to view the large prompt fission flux from the target. Instead the detectors were located so that they could detect delayed fission events, originating from the 6 ns fission isomer state in ^238Pu, which occur downstream from the target position. Data analysis is in progress and results to date will be presented. This work is partly supported by the U.S. DOE under grant numbers DE-FG02-91ER-40609, DE-FG02-88ER-40417.

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

NASA Astrophysics Data System (ADS)

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

2006-08-01

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

Pu-239 and Pu-240 inventories and Pu-240/ Pu-239 atom ratios in the water column off Sanriku, Japan.

NASA Astrophysics Data System (ADS)

Yamada, Masatoshi; Zheng, Jian; Aono, Tatsuo

2013-04-01

A magnitude 9.0 earthquake and subsequent tsunami occurred in the Pacific Ocean off northern Honshu, Japan, on 11 March 2011 which caused severe damage to the Fukushima Dai-ichi Nuclear Power Plant. This accident has resulted in a substantial release of radioactive materials to the atmosphere and ocean, and has caused extensive contamination of the environment. However, no information is available on the amounts of radionuclides such as Pu isotopes released into the ocean at this time. Investigating the background baseline concentration and atom ratio of Pu isotopes in seawater is important for assessment of the possible contamination in the marine environment. Pu-239 (half-life: 24,100 years), Pu-240 (half-life: 6,560 years) and Pu-241 (half-life: 14.325 years) mainly have been released into the environment as the result of atmospheric nuclear weapons testing. The atom ratio of Pu-240/Pu-239 is a powerful fingerprint to identify the sources of Pu in the ocean. The Pu-239 and Pu-240 inventories and Pu-240/Pu-239 atom ratios in seawater samples collected in the western North Pacific off Sanriku before the accident at Fukushima Dai-ichi Nuclear Power Plant will provide useful background baseline data for understanding the process controlling Pu transport and for distinguishing additional Pu sources. Seawater samples were collected with acoustically triggered quadruple PVC sampling bottles during the KH-98-3 cruise of the R/V Hakuho-Maru. The Pu-240/Pu-239 atom ratios were measured with a double-focusing SF-ICP-MS, which was equipped with a guard electrode to eliminate secondary discharge in the plasma and to enhance overall sensitivity. The Pu-239 and Pu-240 concentrations were 2.07 and 1.67 mBq/m3 in the surface water, respectively, and increased with depth; a subsurface maximum was identified at 750 m depth, and the concentrations decreased with depth, then increased at the bottom layer. The total Pu-239+240 inventory in the entire water column (depth interval 0

Modeling of selected ceramic processing parameters employed in the fabrication of 238PuO 2 fuel pellets

DOE PAGES

Brockman, R. A.; Kramer, D. P.; Barklay, C. D.; ...

2011-10-01

Recent deep space missions utilize the thermal output of the radioisotope plutonium-238 as the fuel in the thermal to electrical power system. Since the application of plutonium in its elemental state has several disadvantages, the fuel employed in these deep space power systems is typically in the oxide form such as plutonium-238 dioxide ( 238PuO 2). As an oxide, the processing of the plutonium dioxide into fuel pellets is performed via ''classical'' ceramic processing unit operations such as sieving of the powder, pressing, sintering, etc. Modeling of these unit operations can be beneficial in the understanding and control of processingmore » parameters with the goal of further enhancing the desired characteristics of the 238PuO 2 fuel pellets. A finite element model has been used to help identify the time-temperature-stress profile within a pellet during a furnace operation taking into account that 238PuO 2 itself has a significant thermal output. The results of the modeling efforts will be discussed.« less

Analysis of 238Pu and 56Fe Evaluated Data for Use in MYRRHA

NASA Astrophysics Data System (ADS)

Díez, C. J.; Cabellos, O.; Martínez, J. S.; Stankovskiy, A.; Van den Eynde, G.; Schillebeeckx, P.; Heyse, J.

2014-04-01

A sensitivity analysis on the multiplication factor, keff, to the cross section data has been carried out for the MYRRHA critical configuration in order to show the most relevant reactions. With these results, a further analysis on the 238Pu and 56Fe cross sections has been performed, comparing the evaluations provided in the JEFF-3.1.2 and ENDF/B-VII.1 libraries for these nuclides. Then, the effect in MYRRHA of the differences between evaluations are analysed, presenting the source of the differences. With these results, recommendations for the 56Fe and 238Pu evaluations are suggested. These calculations have been performed with SCALE6.1 and MCNPX-2.7e.

Chemical resolution of Pu+ from U+ and Am+ using a band-pass reaction cell inductively coupled plasma mass spectrometer.

PubMed

Tanner, Scott D; Li, Chunsheng; Vais, Vladimir; Baranov, Vladimir I; Bandura, Dmitry R

2004-06-01

Determination of the concentration and distribution of the Pu and Am isotopes is hindered by the isobaric overlaps between the elements themselves and U, generally requiring time-consuming chemical separation of the elements. A method is described in which chemical resolution of the elemental ions is obtained through ion-molecule reactions in a reaction cell of an ICPMS instrument. The reactions of "natural" U(+), (242)Pu(+), and (243)Am(+) with ethylene, carbon dioxide, and nitric oxide are reported. Since the net sensitivities to the isotopes of an element are similar, chemical resolution is inferred when one isobaric element reacts rapidly with a given gas and the isobar (or in this instance surrogate isotope) is unreactive or slowly reactive. Chemical resolution of the m/z 238 isotopes of U and Pu can be obtained using ethylene as a reaction gas, but little improvement in the resolution of the m/z 239 isobars is obtained. However, high efficiency of reaction of U(+) and UH(+) with CO(2), and nonreaction of Pu(+), allows the sub-ppt determination of (239)Pu, (240)Pu, and (242)Pu (single ppt for (238)Pu) in the presence of 7 orders of magnitude excess U matrix without prior chemical separation. Similarly, oxidation of Pu(+) by NO, and nonreaction of Am(+), permit chemical resolution of the isobars of Pu and Am over 2-3 orders of magnitude relative concentration. The method provides the potential for analysis of the actinides with reduced sample matrix separation.

Nuclear weapons produced 236U, 239Pu and 240Pu archived in a Porites Lutea coral from Enewetak Atoll.

PubMed

Froehlich, M B; Tims, S G; Fallon, S J; Wallner, A; Fifield, L K

2017-11-01

A slice from a Porites Lutea coral core collected inside the Enewetak Atoll lagoon, within 15 km of all major nuclear tests conducted at the atoll, was analysed for 236 U, 239 Pu and 240 Pu over the time interval 1952-1964 using a higher time resolution than previously reported for a parallel slice from the same core. In addition two sediment samples from the Koa and Oak craters were analysed. The strong peaks in the concentrations of 236 U and 239 Pu in the testing years are confirmed to be considerably wider than the flushing time of the lagoon. This is likely due to the growth mechanism of the coral. Following the last test in 1958 atom concentrations of both 236 U and 239 Pu decreased from their peak values by more than 95% and showed a seasonal signal thereafter. Between 1959 and 1964 the weighted average of the 240 Pu/ 239 Pu atom ratio is 0.124 ± 0.008 which is similar to that in the lagoon sediments (0.129 ± 0.006) but quite distinct from the global fallout value of ∼0.18. This, and the high 239,240 Pu and 236 U concentrations in the sediments, provides clear evidence that the post-testing signal in the coral is dominated by remobilisation of the isotopes from the lagoon sediments rather than from global fallout. Copyright © 2017 Elsevier Ltd. All rights reserved.

Energy Dependence of Fission Product Yields from 235U, 238U and 239Pu for Incident Neutron Energies Between 0.5 and 14.8 MeV

NASA Astrophysics Data System (ADS)

Gooden, Matthew; Bredeweg, Todd; Fowler, Malcolm; Vieira, David; Wilhelmy, Jerry; Tonchev, Anton; Stoyer, Mark; Bhike, Megha; Finch, Sean; Krishichayan, Fnu; Tornow, Werner

2017-09-01

The energy dependence of a number of cumulative fission product yields (FPY) have been measured using quasi- monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combi- nation of fission counting using specially designed dual-fission chambers and -ray counting. Each dual-fission chamber is a back-to-back ioniza- tion chamber encasing an activation target in the center with thin de- posits of the same target isotope in each chamber. This method allows for the direct measurement of the total number of fissions in the activa- tion target with no reference to the fission cross-section, thus reducing uncertainties. γ-ray counting of the activation target was performed on well-shielded HPGe detectors over a period of 2 months post irradiation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 3.6, 4.6 and 14.8 MeV. New data in the second chance fission region of 5.5 - 9 MeV are included. Work performed for the U.S. Department of Energy by Los Alamos National Security, LLC under Contract DE-AC52-06NA25396.

Energy dependence of fission product yields from 235U, 238U, and 239Pu with monoenergetic neutrons between thermal and 14.8 MeV

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

Gooden, Matthew; Arnold, Charles; Bhike, Megha

Under a joint collaboration between TUNL-LANL-LLNL, a set of absolute fission product yield measurements has been performed. The energy dependence of a number of cumulative fission product yields (FPY) have been measured using quasi-monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combination of fission counting using specially designed dual-fission chambers and γ-ray counting. Each dual-fission chamber is a back-to-back ionization chamber encasing an activation target in the center with thin deposits of the same target isotope in each chamber. This method allows for the direct measurementmore » of the total number of fissions in the activation target with no reference to the fission cross-section, thus reducing uncertainties. γ-ray counting of the activation target was performed on well-shielded HPGe detectors over a period of two months post irradiation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 3.6, 4.6, 5.5, 7.5, 8.9 and 14.8 MeV. Preliminary results from thermal irradiations at the MIT research reactor will also be presented and compared to present data and evaluations.« less

Energy dependence of fission product yields from 235U, 238U, and 239Pu with monoenergetic neutrons between thermal and 14.8 MeV

DOE PAGES

Gooden, Matthew; Arnold, Charles; Bhike, Megha; ...

2017-09-13

Under a joint collaboration between TUNL-LANL-LLNL, a set of absolute fission product yield measurements has been performed. The energy dependence of a number of cumulative fission product yields (FPY) have been measured using quasi-monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combination of fission counting using specially designed dual-fission chambers and γ-ray counting. Each dual-fission chamber is a back-to-back ionization chamber encasing an activation target in the center with thin deposits of the same target isotope in each chamber. This method allows for the direct measurementmore » of the total number of fissions in the activation target with no reference to the fission cross-section, thus reducing uncertainties. γ-ray counting of the activation target was performed on well-shielded HPGe detectors over a period of two months post irradiation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 3.6, 4.6, 5.5, 7.5, 8.9 and 14.8 MeV. Preliminary results from thermal irradiations at the MIT research reactor will also be presented and compared to present data and evaluations.« less

Energy Dependence of Fission Product Yields from 235U, 238U and 239Pu for Incident Neutron Energies Between 0.5 and 14.8 MeV

NASA Astrophysics Data System (ADS)

Gooden, M.; Arnold, C.; Bredeweg, T.; Vieira, D.; Wilhelmy, J.; Tonchev, A.; Stoyer, M.; Bhike, M.; Krishichayan, F.; Tornow, W.; Fowler, M.

2015-10-01

Under a joint collaboration between TUNL-LANL-LLNL, a set of absolute fission product yield measurements has been performed. The energy dependence of a number of cumulative fission product yields (FPY) have been measured using quasi-monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combination of fission counting using specially designed dual-fission chambers and ?-ray counting. Each dual-fission chamber is a back-to-back ionization chamber encasing an activation target in the center with thin deposits of the same target isotope in each chamber. This method allows for the direct measurement of the total number of fissions in the activation target with no reference to the fission cross-section, thus reducing uncertainties. ?-ray counting of the activation target was performed on well-shielded HPGe detectors over a period of 2 months post irradiation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 3.6, 4.6, 5.5, 7.5, 8.9 and 14.8 MeV. These results are compared to previous measurements and theoretical estimates. This work was performed under the auspices of the USDoE by Los Alamos National Security, LLC under Contract DE-AC52-06NA25396.

Environmental aspects of the transuranics: a selected, annotated bibliography. [Pu-238, Pu-239

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

Ensminger, J.T.; Martin, F.M.; Fore, C.S.

This eighth published bibliography of 427 references is compiled from the Nevada Applied Ecology Information Center's Data Base on the Environmental Aspects of the Transuranics. The data base was built to provide information support to the Nevada Applied Ecology Group (NAEG) of ERDA's Nevada Operations Office. The general scope covers environmental aspects of uranium and the transuranic elements, with emphasis on plutonium. This bibliography highlights literature on plutonium 238 and 239 and americium in the critical organs of man and animals. Supporting information on ecology of the Nevada Test Site and reviews and summarizing literature on other radionuclides have beenmore » included at the request of the NAEG. The references are arranged by subject category with leading authors appearing alphabetically in each category. Indexes are provided for author(s), geographic location, keyword(s), taxon, title, and publication description.« less

Precise 238U(n,2n)237U reaction cross-section measurements using the activation facility at TUNL

NASA Astrophysics Data System (ADS)

Krishichayan, Fnu; Bhike, M.; Tornow, W.

2014-09-01

Accurate neutron-induced 238U(n,2n)237U reaction data are required for many practical applications, especially in the field of nuclear energy, including advanced heavy water reactors, where 238U is used as the breeding material to regenerate the fissile material 239Pu. Precise (n,2n) cross-section measurements of 238U are underway at TUNL with mono-energetic neutrons in the 8.0 to 14.0 MeV energy range in steps of 0.25 MeV using the activation technique. After activation of the 0.5 inch diameter and 442 mg 238U foil, the activity of the 208 keV characteristic γ-line is tracked for 6 weeks with a high efficient HPGe clover detector to determine the initial activity needed for the cross-section determination. Results of the cross-section measurements, determined relative to 27Al and 197Au neutron activation monitor foils, and the comparison with theoretical models will be presented during the meeting.

Direct fabrication of /sup 238/PuO/sub 2/ fuel forms

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

Burney, G.A.; Congdon, J.W.

1982-07-01

The current process for the fabrication of /sup 238/PuO/sub 2/ heat sources includes precipitation of small particle plutonium oxalate crystals (4 to 6 ..mu..m diameter), a calcination to PuO/sub 2/, ball milling, cold pressing, granulation (60 to 125 ..mu..m), and granule sintering prior to hot pressing the fuel pellet. A new two-step direct-strike Pu(III) oxalate precipitation method which yields mainly large well-developed rosettes (50 to 100 ..mu..m diameter) has been demonstrated in the laboratory and in the plant. These large rosettes are formed by agglomeration of small (2 to 4 ..mu..m) crystals, and after calcining and sintering, were directly hotmore » pressed into fuel forms, thus eliminating several of the powder conditioning steps. Conditions for direct hot pressing of the large heat-treated rosettes were determined and a full-scale General Purpose Heat Source pellet was fabricated. The pellet had the desired granule-type microstructure to provide dimensional stability at high temperature. 27 figures.« less

239Pu fallout across continental Australia: Implications on 239Pu use as a soil tracer.

PubMed

Lal, R; Fifield, L K; Tims, S G; Wasson, R J

2017-11-01

At present there is a need for the development of new radioisotopes for soil erosion and sediment tracing especially as fallout 137 Cs levels become depleted. Recent studies have shown that 239 Pu can be a useful new soil erosion and sediment radioisotope tracer. 239 Pu was released in the major atmospheric nuclear weapons tests of 1950's and 1960's. However 239 Pu has a half-life of 24110 years and more than 99% of this isotope is still present in the environment today. In contrast 137 Cs with a half-life of 30.07 year has decayed to <35% of initially deposited activities and this isotope will become increasingly difficult to measure in the coming decades especially in the southern hemisphere, which received only about a third of the total global fallout from the atmospheric tests (UNSCEAR, 2000). In this study an assessment of the 239 Pu fallout in Australia was carried out from comparison of measured 239 Pu inventories with expected 239 Pu inventories from fallout models. 239 Pu inventories were also compared with rainfall and measured 240 Pu/ 239 Pu ratios across Australia. 239 Pu fallout inventories ranged from 430 to 1461 μB/cm 2 . Central Australia, with fallout 107% in excess of expected values, seems to be strongly impacted by local fallout deposition. In comparison other sites typically show 5-40% variation between expected and measured fallout values. The fallout inventories were found to weakly correlate (using power functions, y = ax b ) with rainfall with r 2  = 0.50 across the southern catchments (25-40°S latitude band). Across the northern catchments (10-25°S latitude band) fallout showed greater variability with rainfall with r 2  = 0.24. Central Australia and Alice Springs which seem to be strongly impacted by local fallout are excluded from the rainfall correlation data (with these sites included r 2  = 0.08 and r 2  < 0.01 respectively). 240 Pu/ 239 Pu atom ratios range from 0.045 to 0.197, with averages of 0.139(0.017), 0

Evaluation of Aqueous and Powder Processing Techniques for Production of Pu-238-Fueled General Purpose Heat Sources

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

Not Available

2008-06-01

This report evaluates alternative processes that could be used to produce Pu-238 fueled General Purpose Heat Sources (GPHS) for radioisotope thermoelectric generators (RTG). Fabricating GPHSs with the current process has remained essentially unchanged since its development in the 1970s. Meanwhile, 30 years of technological advancements have been made in the fields of chemistry, manufacturing, ceramics, and control systems. At the Department of Energy’s request, alternate manufacturing methods were compared to current methods to determine if alternative fabrication processes could reduce the hazards, especially the production of respirable fines, while producing an equivalent GPHS product. An expert committee performed the evaluationmore » with input from four national laboratories experienced in Pu-238 handling.« less

Energy Dependence of Fission Product Yields from 235 U, 238U, and 239Pu for Incident Neutron Energies Between 0.5 and 14.8 MeV

NASA Astrophysics Data System (ADS)

Gooden, Matthew Edgell

A joint collaboration between the Triangle Universities Nuclear Laboratory (TUNL), Los Alamos National Laboratory (LANL) and Lawrence Livermore National Laboratory (LLNL) has performed a set of absolute Fission Product Yield (FPY) measurements. Using monoenergetic neutron at energies between 0.5 and 14.8 MeV, the excitation functions of a number of fission products from 235U, 238U and 239Pu have begun to be mapped out. This work has practical applications for the determination of weapon yields and the rate of burn-up in nuclear reactors, while also providing important insight into the fission process. Combining the use of a dual-fission ionization chamber and gamma-ray spectroscopy, absolute FPYs have been determined for approximately 15 different fission products. The dual-fission chamber is a back-to-back ionization chamber system with a 'thin' actinide foil in each chamber as a monitor or reference foil. The chamber holds a 'thick' target in the center of the system such that the target and reference foils are of the same actinide isotope. This allows for simple mass scaling between the recorded number of fissions in the individual chambers and the number of fissions in the center thick target, eliminating the need for the knowledge of the absolute fission cross section and its uncertainty. The 'thick' target was removed after activation and gamma-rays counted with well shielded High Purity Germanium (HPGe) detectors for a period of 1.5 - 2 months.

Energy dependence of fission product yields from 235U, 238U, and 239Pu with monoenergetic neutrons between thermal and 14.8 MeV

NASA Astrophysics Data System (ADS)

Gooden, Matthew; Arnold, Charles; Bhike, Megha; Bredeweg, Todd; Fowler, Malcolm; Krishichayan; Tonchev, Anton; Tornow, Werner; Stoyer, Mark; Vieira, David; Wilhelmy, Jerry

2017-09-01

Under a joint collaboration between TUNL-LANL-LLNL, a set of absolute fission product yield measurements has been performed. The energy dependence of a number of cumulative fission product yields (FPY) have been measured using quasi-monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combination of fission counting using specially designed dual-fission chambers and γ-ray counting. Each dual-fission chamber is a back-to-back ionization chamber encasing an activation target in the center with thin deposits of the same target isotope in each chamber. This method allows for the direct measurement of the total number of fissions in the activation target with no reference to the fission cross-section, thus reducing uncertainties. γ-ray counting of the activation target was performed on well-shielded HPGe detectors over a period of two months post irradiation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 3.6, 4.6, 5.5, 7.5, 8.9 and 14.8 MeV. Preliminary results from thermal irradiations at the MIT research reactor will also be presented and compared to present data and evaluations. This work was performed under the auspices of the U.S. Department of Energy by Los Alamos National Security, LLC under contract DE-AC52-06NA25396, Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344 and by Duke University and Triangle Universities Nuclear Laboratory through NNSA Stewardship Science Academic Alliance grant No. DE-FG52-09NA29465, DE-FG52-09NA29448 and Office of Nuclear Physics Grant No. DE-FG02-97ER41033.

Measurements Conducted on an Unknown Object Labeled Pu-239

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

Hoteling, Nathan

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

International comparison of activity measurements of a solution of 238Pu

NASA Astrophysics Data System (ADS)

Ratel, G.; Michotte, C.

2018-01-01

This report concerns an international comparison of measurements of a solution of 238Pu that was carried out by 12 participants in 2001. The report includes the degrees of equivalence. Main text To reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database kcdb.bipm.org/. The final report has been peer-reviewed and approved for publication by the CCRI, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).

Carcinogenesis From Inhaled (PuO2)-Pu-239 in Beagles: Evidence for Radiation Homeostasis at Low Doses?

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

Fisher, Darrell R.; Weller, Richard E.

From the early 1970s to the late 1980s, Pacific Northwest National Laboratory conducted life-span studies in beagle dogs on the biological effects of inhaled plutonium (239PuO2, 238PuO2, and 239Pu[NO3]4) to help predict risks associated with accidental intakes in workers. Years later, the purpose of the present follow-up study is to reassess the dose-response relationship for lung cancer induction in the 239PuO2 dogs compared to controls, with particular focus on the dose-response at low lung doses. A 239PuO2 aerosol (2.3 μm AMAD, 1.9 μm GSD) was administered to six groups of 20 young (18-month old) beagle dogs (10 males and 10more » females) by inhalation at six different activity levels, as previously described in Laboratory reports. Control dogs were sham-exposed. In dose level 1, initial pulmonary lung depositions were 130 ± 48 Bq (3.5 ± 1.3 nCi), corresponding to 1 Bq g-1 lung tissue (0.029 ± 0.001 nCi g-1. Groups 2 through 6 received initial lung depositions (mean values) of 760, 2724, 10345, 37900, and 200000 Bq (22, 79, 300, 1100, and 5800 nCi) 239PuO2, respectively. For each dog, the absorbed dose to lungs was calculated from the initial lung burden and the final lung burden at time of death and lung mass, assuming a single, long-term retention function. Insoluble plutonium oxide exhibited long retention times in the lungs. Increased dose-dependent mortality due to lung cancer (bronchiolar-alveolar carcinoma, adenocarcinoma, epidermoid carcinoma) and radiation pneumonitis (highest exposures group) was observed in dogs exposed to 239PuO2. Calculated lung doses ranged from a few cGy in early-sacrificed dogs to 7764 cGy in dogs that experienced early deaths from radiation pneumonitis. Data were regrouped by lifetime lung dose and plotted as a function of lung tumor incidence. Lung tumor incidence in controls and zero-dose exposed dogs was 18% (5/28). However, no lung tumors were observed in 16 dogs with the lowest lung doses (8 to 22 cGy, mean 14.4 �

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.

Analysis of Operating Strategies Using Different Target Designs For 238Pu Production

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

Thomas, Tomcy; Sherman, Steven R; Sawhney, Dr. Rapinder

2017-01-01

An engineering effort is underway to re-establish capability to produce 238Pu oxide at the kilogram scale in the United States. A multi-step batch process is being developed to produce this important material. Recently, a portion of this process was studied using discrete-event simulation tools to determine whether the conceptual process might achieve its yearly production goal. The study showed the conceptual process can meet the yearly production goal under some circumstances, but process improvements would be needed to ensure greater likelihood of success. This study extends the work performed previously by examining the effects of changing the reactor target designmore » on the yearly process output. Two new reactor target configurations are considered an aluminum-clad reactor target containing 50% greater 237Np oxide content than the original target, and a zirconium alloy-clad target using no aluminum. The results indicate that use of the new aluminum-clad target configuration may allow the process to achieve the same yearly production goal in less time using fewer targets. If the zirconium alloy-clad target is used, then even fewer targets would be needed to reach the production goal, but some process changes would be required to handle the zirconium cladding. The number of days needed to process a target batch to completion, and the steady state 238Pu oxide production rate, for each configuration are compared to the results from the initial simulation study.« less

238Pu recovery and salt disposition from the molten salt oxidation process

NASA Astrophysics Data System (ADS)

Remerowski, M. L.; Stimmel, Jay J.; Wong, Amy S.; Ramsey, Kevin B.

2000-07-01

We have begun designing and optimizing our recovery and recycling processes by experimenting with samples of "spent salt" produced by MSO treatment of surrogate waste in the reaction vessel at the Naval Surface Warfare Center-Indian Head. One salt was produced by treating surrogate waste containing pyrolysis ash spiked with cerium. The other salt contains residues from MSO treatment of materials similar to those used in 238Pu processing, e.g., Tygon tubing, PVC bagout bags, HDPE bottles. Using these two salt samples, we will present results from our investigations.

CAPABILITY TO RECOVER PLUTONIUM-238 IN H-CANYON/HB-LINE

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

Fuller, Kenneth S. Jr.; Smith, Robert H. Jr.; Goergen, Charles R.

2013-01-09

Plutonium-238 is used in Radioisotope Thermoelectric Generators (RTGs) to generate electrical power and in Radioisotope Heater Units (RHUs) to produce heat for electronics and environmental control for deep space missions. The domestic supply of Pu-238 consists of scrap material from previous mission production or material purchased from Russia. Currently, the United States has no significant production scale operational capability to produce and separate new Pu-238 from irradiated neptunium-237 targets. The Department of Energy - Nuclear Energy is currently evaluating and developing plans to reconstitute the United States capability to produce Pu-238 from irradiated Np-237 targets. The Savannah River Site hadmore » previously produced and/or processed all the Pu-238 utilized in Radioisotope Thermoelectric Generators (RTGs) for deep space missions up to and including the majority of the plutonium for the Cassini Mission. The previous full production cycle capabilities included: Np-237 target fabrication, target irradiation, target dissolution and Np-237 and Pu-238 separation and purification, conversion of Np-237 and Pu-238 to oxide, scrap recovery, and Pu-238 encapsulation. The capability and equipment still exist and could be revitalized or put back into service to recover and purify Pu-238/Np-237 or broken General Purpose Heat Source (GPHS) pellets utilizing existing process equipment in HB-Line Scrap Recovery, and H-anyon Frame Waste Recovery processes. The conversion of Np-237 and Pu-238 to oxide can be performed in the existing HB-Line Phase-2 and Phase-3 Processes. Dissolution of irradiated Np-237 target material, and separation and purification of Np-237 and Pu-238 product streams would be possible at production rates of ~ 2 kg/month of Pu-238 if the existing H-Canyon Frames Process spare equipment were re-installed. Previously, the primary H-Canyon Frames equipment was removed to be replaced: however, the replacement project was stopped. The spare

Isotopic compositions of (236)U and Pu isotopes in "black substances" collected from roadsides in Fukushima prefecture: fallout from the Fukushima Dai-ichi nuclear power plant accident.

PubMed

Sakaguchi, Aya; Steier, Peter; Takahashi, Yoshio; Yamamoto, Masayoshi

2014-04-01

Black-colored road dusts were collected in high-radiation areas in Fukushima Prefecture. Measurement of (236)U and Pu isotopes and (134,137)Cs in samples was performed to confirm whether refractory elements, such as U and Pu, from the fuel core were discharged and to ascertain the extent of fractionation between volatile and refractory elements. The concentrations of (134,137)Cs in all samples were exceptionally high, ranging from 0.43 to 17.7 MBq/kg, respectively. (239+240)Pu was detected at low levels, ranging from 0.15 to 1.14 Bq/kg, and with high (238)Pu/(239+240)Pu activity ratios of 1.64-2.64. (236)U was successfully determined in the range of (0.28 to 6.74) × 10(-4) Bq/kg. The observed activity ratios for (236)U/(239+240)Pu were in reasonable agreement with those calculated for the fuel core inventories, indicating that trace amounts of U from the fuel cores were released together with Pu isotopes but without large fractionation. The quantities of U and (239+240)Pu emitted to the atmosphere were estimated as 3.9 × 10(6) Bq (150 g) and 2.3 × 10(9) Bq (580 mg), respectively. With regard to U, this is the first report to give a quantitative estimation of the amount discharged. Appreciable fractionation between volatile and refractory radionuclides associated with the dispersal/deposition processes with distance from the Fukushima Dai-ichi Nuclear Power Plant was found.

Variations in Pu isotopic composition in soils from the Spitsbergen (Norway): Three potential pollution sources of the Arctic region.

PubMed

Łokas, E; Anczkiewicz, R; Kierepko, R; Mietelski, J W

2017-07-01

Although the polar regions have not been industrialised, numerous contaminants originating from human activity are detectable in the Arctic environment. This study reports evidence of 240 Pu/ 239 Pu atomic ratios in the tundra and initial soils from different parts of west and central Spitsbergen and recognizes possible environmental inputs of non-global fallout Pu. The average atomic ratio of 240 Pu/ 239 Pu equal to 0.179 (ranging between 0.129 and 0.201) in tundra soils are comparable to the characteristic ratio for global fallout (0.180). However, the 240 Pu/ 239 Pu atomic ratios in the initial soils from proglacial zone of glaciers change within wide range between 0.1281 and 0.234 with the mean value of 0.169. By combining alpha and mass spectrometry, the three-sources model was used to identify the Pu sources in initial soils. Our study indicated that the main source of Pu is nuclear tests and that a second source with lower Pu ratio may come from weapons grade Pu (unexploded weapons grade Pu ie. material from bomb which didn't undergo nuclear explosions for example for security tests). Additionally, we found samples with high 238 Pu/ 239+240 Pu activity ratios and with typical global fallout 240 Pu/ 239 Pu atomic ratios, which are associated with separate sources of pure 238 Pu from the SNAP-9A satellite burn up in the atmosphere. Copyright © 2017 Elsevier Ltd. All rights reserved.

First measurements of (236)U concentrations and (236)U/(239)Pu isotopic ratios in a Southern Hemisphere soil far from nuclear test or reactor sites.

PubMed

Srncik, M; Tims, S G; De Cesare, M; Fifield, L K

2014-06-01

The variation of the (236)U and (239)Pu concentrations as a function of depth has been studied in a soil profile at a site in the Southern Hemisphere well removed from nuclear weapon test sites. Total inventories of (236)U and (239)Pu as well as the (236)U/(239)Pu isotopic ratio were derived. For this investigation a soil core from an undisturbed forest area in the Herbert River catchment (17°30' - 19°S) which is located in north-eastern Queensland (Australia) was chosen. The chemical separation of U and Pu was carried out with a double column which has the advantage of the extraction of both elements from a relatively large soil sample (∼20 g) within a day. The samples were measured by Accelerator Mass Spectrometry using the 14UD pelletron accelerator at the Australian National University. The highest atom concentrations of both (236)U and (239)Pu were found at a depth of 2-3 cm. The (236)U/(239)Pu isotopic ratio in fallout at this site, as deduced from the ratio of the (236)U and (239)Pu inventories, is 0.085 ± 0.003 which is clearly lower than the Northern Hemisphere value of ∼0.2. The (236)U inventory of (8.4 ± 0.3) × 10(11) at/m(2) was more than an order of magnitude lower than values reported for the Northern Hemisphere. The (239)Pu activity concentrations are in excellent agreement with a previous study and the (239+240)Pu inventory was (13.85 ± 0.29) Bq/m(2). The weighted mean (240)Pu/(239)Pu isotopic ratio of 0.142 ± 0.005 is slightly lower than the value for global fallout, but our results are consistent with the average ratio of 0.173 ± 0.027 for the southern equatorial region (0-30°S). Copyright © 2014 Elsevier Ltd. All rights reserved.

Capability to Recover Plutonium-238 in H-Canyon/HB-Line - 13248

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

Fuller, Kenneth S. Jr.; Smith, Robert H. Jr.; Goergen, Charles R.

2013-07-01

Plutonium-238 is used in Radioisotope Thermoelectric Generators (RTGs) to generate electrical power and in Radioisotope Heater Units (RHUs) to produce heat for electronics and environmental control for deep space missions. The domestic supply of Pu-238 consists of scrap material from previous mission production or material purchased from Russia. Currently, the United States has no significant production scale operational capability to produce and separate new Pu-238 from irradiated neptunium-237 targets. The Department of Energy - Nuclear Energy is currently evaluating and developing plans to reconstitute the United States capability to produce Pu-238 from irradiated Np-237 targets. The Savannah River Site hadmore » previously produced and/or processed all the Pu-238 utilized in Radioisotope Thermoelectric Generators (RTGs) for deep space missions up to and including the majority of the plutonium for the Cassini Mission. The previous full production cycle capabilities included: Np- 237 target fabrication, target irradiation, target dissolution and Np-237 and Pu-238 separation and purification, conversion of Np-237 and Pu-238 to oxide, scrap recovery, and Pu-238 encapsulation. The capability and equipment still exist and could be revitalized or put back into service to recover and purify Pu-238/Np-237 or broken General Purpose Heat Source (GPHS) pellets utilizing existing process equipment in HB-Line Scrap Recovery, and H-Canyon Frame Waste Recovery processes. The conversion of Np-237 and Pu-238 to oxide can be performed in the existing HB-Line Phase-2 and Phase- 3 Processes. Dissolution of irradiated Np-237 target material, and separation and purification of Np-237 and Pu-238 product streams would be possible at production rates of ∼2 kg/month of Pu-238 if the existing H-Canyon Frames Process spare equipment were re-installed. Previously, the primary H-Canyon Frames equipment was removed to be replaced: however, the replacement project was stopped. The spare

Determination of the activity concentration of a 238 Pu solution by the defined solid angle method utilizing a novel dual diaphragm-detector assembly.

PubMed

Aguiar, Julio C; Galiano, Eduardo; Arenillas, Pablo

2005-08-01

The activity concentration of a (238)Pu solution was measured by the determined solid angle method employing a novel dual diaphragm-detector assembly, which has been previously described. Due to the special requirements of the detector, a new type of source holder was developed, which consisted of sandwiching the radioisotope between two organic films called VYNS. It was experimentally demonstrated that the VYNS films do not absorb alpha particles, but reduce their energy by an average of 22 keV.A mean activity concentration for (238)Pu of 359.10+/-0.8 kBq/g was measured.

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.

Investigating Pu and U isotopic compositions in sediments: a case study in Lake Obuchi, Rokkasho Village, Japan using sector-field ICP-MS and ICP-QMS.

PubMed

Zheng, Jian; Yamada, Masatoshi

2005-08-01

The objectives of the present work were to study isotope ratios and the inventory of plutonium and uranium isotope compositions in sediments from Lake Obuchi, which is in the vicinity of several nuclear fuel facilities in Rokkasho, Japan. Pu and its isotopes were determined using sector-field ICP-MS and U and its isotopes were determined with ICP-QMS after separation and purification with a combination of ion-exchange and extraction chromatography. The observed (240)Pu/(239)Pu atom ratio (0.186 +/- 0.016) was similar to that of global fallout, indicating that the possible early tropospheric fallout Pu did not deliver Pu from the Pacific Proving Ground to areas above 40 degrees N. The previously reported higher Pu inventory in the deep water area of Lake Obuchi could be attributed to the lateral transportation of Pu deposited in the shallow area which resulted from the migration of deposited global fallout Pu from the land into the lake by river runoff and from the Pacific Ocean by tide movement and sea water scavenging, as well as from direct soil input by winds. The (235)U/(238)U atom ratios ranged from 0.00723 to 0.00732, indicating the natural origin of U in the sediments. The average (234)U/(238)U activity ratio of 1.11 in a sediment core indicated a significant sea water U contribution. No evidence was found for the release of U containing wastes from the nearby nuclear facilities. These results will serve as a reference baseline on the levels of Pu and U in the studied site so that any further contamination from the spent nuclear fuel reprocessing plants, the radioactive waste disposal and storage facilities, and the uranium enrichment plant can be identified, and the impact of future release can be rapidly assessed.

Controlling Pu behavior on Titania: Implications for LEU Fission-Based Mo-99 Production

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

Youker, Amanda J.; Brown, M. Alex; Heltemes, Thad A.

Molybdenum-99 is the parent isotope of the most widely used isotope, technetium-99m, in all diagnostic nuclear medicine procedures. Due to proliferation concerns associated with the use of highly enriched uranium (HEU), the preferred method of fission-based Mo-99 production uses low enriched uranium (LEU) targets. Using LEU versus HEU for Mo-99 production produces similar to 30 times more Pu-239, due to neutron capture on U-238 to produce Np-239, which ultimately decays to Pu-239 (t(1/2) = 24,110 yr). Argonne National Laboratory is supporting a potential US Mo-99 producer in their efforts to produce Mo-99 from an LEU solution. In order to mitigatemore » the generation of large volumes of greater-than-class-C (GTCC) low level waste (Pu-239 concentrations greater than 1 nCi/g), we have focused our efforts on the separation chemistry of Pu and Mo with a titania sorbent in sulfate media. Results from batch and column experiments show that temperature and acid wash concentration can be used to control Pu behavior on titania.« less

Precision measurement of the 238 Pu ( n , γ ) cross section

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

Chyzh, A.; Wu, C. Y.; Kwan, E.

2013-10-14

Here, the neutron-capture cross section for 238Pu was measured by using the detector for advanced neutron-capture experiments (DANCE) array, which is a highly segmented and highly efficient 4π γ-ray calorimeter. The neutron-capture events were recognized by the total γ-ray energy deposited in DANCE, which is equal to the reaction Q value plus the incident neutron energy. The absolute neutron-capture cross section was derived as a function of incident neutron energy from thermal to about 30 keV. The measured cross section for incident neutron energy below 18 eV was performed for the first time by using the direct method and doesmore » not support the most recently adopted changes in endf/b-vii.1 where the neutron-capture cross section was lowered by as much as a factor of ~3 in the neighborhood of 0.3 eV from those evaluated in ENDF/B-VII.0.« less

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

U-PuO2, U-PuC, U-PuN cermet fuel for fast reactor

NASA Astrophysics Data System (ADS)

Mishra, Sudhir; Kaity, Santu; Banerjee, Joydipta; Nandi, Chiranjeet; Dey, G. K.; Khan, K. B.

2018-02-01

Cermet fuel combines beneficial properties of both ceramic and metal and attracts global interest for research as a candidate fuel for nuclear reactors. In the present study, U matrix PuC/PuN/PuO2 cermet for fast reactor have been fabricated on laboratory scale by the powder metallurgy route. Characterization of the fuel has been carried out using Dilatometer, Differential Thermal analysis (DTA), X-ray diffractometer and Optical microscope. X ray diffraction study of the fuel reveals presence of different phases. The PuN dispersed cermet was observed to have high solidus temperature as compared to PuC and PuO2 dispersed cermet. Swelling was observed in U matrix PuO2 cermet which also showed higher thermal expansion. Among the three cermets studied, U matrix PuC cermet showed maximum thermal conductivity.

Soft tissue tumors induced by monomeric {sup 239}Pu

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

Lloyd, R.D.; Angus, W.; Taylor, G.N.

1995-10-01

Individual records of soft tissue tumor occurrence (lifetime incidence) among 236 beagles injected with {sup 239}Pu citrate as young adults and 131 comparable control beagles given no radioactivity enabled us to analyze the possible effects on soft tissue tumor induction resulting from internal exposure to {sup 239}Pu. A significant trend was identified in the proportion of animals having malignant liver tumors with increasing radiation dose from {sup 239}. There was also a significant difference in the relative numbers of both malignant liver tumors (18.1 expected, 66 observed). Malignant tumors of the mouth, pancreas, and skin were more frequent among controlsmore » than among the dogs given {sup 239}Pu as well as tumors (malignant plus benign) of the mouth, pancreas, testis, and vagina. For all other tumor sites or types, there was no significant difference for both malignant and all (malignant plus benign) tumors. Mammary tumor occurrence appeared not to be associated with {sup 239}Pu incorporation. We conclude that the only soft-tissue neoplasia induced by the intake of {sup 239}Pu directly into blood is probably a liver tumor. 20 refs., 6 tabs.« less

Nuclear reactor for breeding U.sup.233

DOEpatents

Bohanan, Charles S.; Jones, David H.; Raab, Jr., Harry F.; Radkowsky, Alvin

1976-01-01

A light-water-cooled nuclear reactor capable of breeding U.sup.233 for use in a light-water breeder reactor includes physically separated regions containing U.sup.235 fissile material and U.sup.238 fertile material and Th.sup.232 fertile material and Pu.sup.239 fissile material, if available. Preferably the U.sup.235 fissile material and U.sup.238 fertile material are contained in longitudinally movable seed regions and the Pu.sup.239 fissile material and Th.sup.232 fertile material are contained in blanket regions surrounding the seed regions.

Chronology of Pu isotopes and 236U in an Arctic ice core.

PubMed

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

2013-09-01

In the present work, state of the art isotopic fingerprinting techniques are applied to an Arctic ice core in order to quantify deposition of U and Pu, and to identify possible tropospheric transport of debris from former Soviet Union test sites Semipalatinsk (Central Asia) and Novaya Zemlya (Arctic Ocean). An ice core chronology of (236)U, (239)Pu, and (240)Pu concentrations, and atom ratios, measured by accelerator mass spectrometry in a 28.6m deep ice core from the Austfonna glacier at Nordaustlandet, Svalbard is presented. The ice core chronology corresponds to the period 1949 to 1999. The main sources of Pu and (236)U contamination in the Arctic were the atmospheric nuclear detonations in the period 1945 to 1980, as global fallout, and tropospheric fallout from the former Soviet Union test sites Novaya Zemlya and Semipalatinsk. Activity concentrations of (239+240)Pu ranged from 0.008 to 0.254 mBq cm(-2) and (236)U from 0.0039 to 0.053 μBq cm(-2). Concentrations varied in concordance with (137)Cs concentrations in the same ice core. In contrast to previous published results, the concentrations of Pu and (236)U were found to be higher at depths corresponding to the pre-moratorium period (1949 to 1959) than to the post-moratorium period (1961 and 1962). The (240)Pu/(239)Pu ratio ranged from 0.15 to 0.19, and (236)U/(239)Pu ranged from 0.18 to 1.4. The Pu atom ratios ranged within the limits of global fallout in the most intensive period of nuclear atmospheric testing (1952 to 1962). To the best knowledge of the authors the present work is the first publication on biogeochemical cycles with respect to (236)U concentrations and (236)U/(239)Pu atom ratios in the Arctic and in ice cores. Copyright © 2013 Elsevier B.V. All rights reserved.

Time-resolved record of 236U and 239,240Pu isotopes from a coral growing during the nuclear testing program at Enewetak Atoll (Marshall Islands).

PubMed

Froehlich, M B; Chan, W Y; Tims, S G; Fallon, S J; Fifield, L K

2016-12-01

A comprehensive series of nuclear tests were carried out by the United States at Enewetak Atoll in the Marshall Islands, especially between 1952 and 1958. A Porites Lutea coral that was growing in the Enewetak lagoon within a few km of all of the high-yield tests contains a continuous record of isotopes, which are of interest (e.g. 14 C, 236 U, 239,240 Pu) through the testing period. Prior to the present work, 14 C measurements at ∼2-month resolution had shown pronounced peaks in the Δ 14 C data that coincided with the times at which tests were conducted. Here we report measurements of 236 U and 239,240 Pu on the same coral using accelerator mass spectrometry, and again find prominent peaks in the concentrations of these isotopes that closely follow those in 14 C. Consistent with the 14 C data, the magnitudes of these peaks do not, however, correlate well with the explosive yields of the corresponding tests, indicating that smaller tests probably contributed disproportionately to the debris that fell in the lagoon. Additional information about the different tests can also be obtained from the 236 U/ 239 Pu and 240 Pu/ 239 Pu ratios, which are found to vary dramatically over the testing period. In particular, the first thermonuclear test, Ivy-Mike, has characteristic 236 U/ 239 Pu and 240 Pu/ 239 Pu signatures which are diagnostic of the first arrival of nuclear test material in various archives. Copyright © 2016 Elsevier Ltd. All rights reserved.

Anlysis capabilities for plutonium-238 programs

NASA Astrophysics Data System (ADS)

Wong, A. S.; Rinehart, G. H.; Reimus, M. H.; Pansoy-Hjelvik, M. E.; Moniz, P. F.; Brock, J. C.; Ferrara, S. E.; Ramsey, S. S.

2000-07-01

In this presentation, an overview of analysis capabilities that support 238Pu programs will be discussed. These capabilities include neutron emission rate and calorimetric measurements, metallography/ceramography, ultrasonic examination, particle size determination, and chemical analyses. The data obtained from these measurements provide baseline parameters for fuel clad impact testing, fuel processing, product certifications, and waste disposal. Also several in-line analyses capabilities will be utilized for process control in the full-scale 238Pu Aqueous Scrap Recovery line in FY01.

Studies of Plutonium-238 Production at the High Flux Isotope Reactor

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

Lastres, Oscar; Chandler, David; Jarrell, Joshua J

The High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL) is a versatile 85 MW{sub th}, pressurized, light water-cooled and -moderated research reactor. The core consists of two fuel elements, an inner fuel element (IFE) and an outer fuel element (OFE), each constructed of involute fuel plates containing high-enriched-uranium (HEU) fuel ({approx}93 wt% {sup 235}U/U) in the form of U{sub 3}O{sub 8} in an Al matrix and encapsulated in Al-6061 clad. An over-moderated flux trap is located in the center of the core, a large beryllium reflector is located on the outside of the core, and two controlmore » elements (CE) are located between the fuel and the reflector. The flux trap and reflector house numerous experimental facilities which are used for isotope production, material irradiation, and cold/thermal neutron scattering. Over the past five decades, the US Department of Energy (DOE) and its agencies have been producing radioisotope power systems used by the National Aeronautics and Space Administration (NASA) for unmanned, long-term space exploration missions. Plutonium-238 is used to power Radioisotope Thermoelectric Generators (RTG) because it has a very long half-life (t{sub 1/2} {approx} 89 yr.) and it generates about 0.5 watts/gram when it decays via alpha emission. Due to the recent shortage and uncertainty of future production, the DOE has proposed a plan to the US Congress to produce {sup 238}Pu by irradiating {sup 237}Np as early as in fiscal year 2011. An annual production rate of 1.5 to 2.0 kg of {sup 238}Pu is expected to satisfy these needs and could be produced in existing national nuclear facilities like HFIR and the Advanced Test Reactor (ATR) at the Idaho National Laboratory (INL). Reactors at the Savannah River Site were used in the past for {sup 238}Pu production but were shut down after the last production in 1988. The nation's {sup 237}Np inventory is currently stored at INL. A plan for producing {sup 238}Pu at US research

Air concentrations of /sup 239/Pu and /sup 240/Pu and potential radiation doses to persons living near Pu-contaminated areas in Palomares, Spain

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

Iranzo, E.; Salvador, S.; Iranzo, C.E.

1987-04-01

On 17 January 1966, an accident during a refueling operation resulted in the destruction of an air force KC-135 tanker and a B-52 bomber carrying four thermonuclear weapons. Two weapons, whose parachutes opened, were found intact. The others experienced non-nuclear explosion with some burning and release of the fissile fuel at impact. Joint efforts by the United States and Spain resulted in remedial action and a long-term program to monitor the effectiveness of the cleanup. Air concentrations of /sup 239/Pu and /sup 240/Pu have been continuously monitored since the accident. The average annual air concentration for each location was usedmore » to estimate committed dose equivalents for individuals living and working around the air sampling stations. The average annual /sup 239/Pu and /sup 240/Pu air concentrations during the 15-y period corresponding to 1966-1980 and the potential committed dose equivalents for various tissues due to the inhalation of the /sup 239/Pu and /sup 240/Pu average annual air concentration during this period are shown and discussed in the report.« less

Rapid Method for Sodium Hydroxide Fusion of Asphalt ...

EPA Pesticide Factsheets

Technical Brief--Addendum to Selected Analytical Methods (SAM) 2012 Rapid method developed for analysis of Americium-241 (241Am), plutonium-238 (238Pu), plutonium-239 (239Pu), radium-226 (226Ra), strontium-90 (90Sr), uranium-234 (234U), uranium-235 (235U) and uranium-238 (238U) in asphalt roofing material samples

A comparison of untagged gamma-ray and tagged-neutron yields from 241AmBe and 238PuBe sources.

PubMed

Scherzinger, J; Al Jebali, R; Annand, J R M; Fissum, K G; Hall-Wilton, R; Koufigar, S; Mauritzson, N; Messi, F; Perrey, H; Rofors, E

2017-09-01

Untagged gamma-ray and tagged-neutron yields from 241 AmBe and 238 PuBe mixed-field sources have been measured. Gamma-ray spectroscopy measurements from 1 to 5MeV were performed in an open environment using a CeBr 3 detector and the same experimental conditions for both sources. The shapes of the distributions are very similar and agree well with previous data. Tagged-neutron measurements from 2 to 6MeV were performed in a shielded environment using a NE-213 liquid-scintillator detector for the neutrons and a YAP(Ce) detector to tag the 4.44MeVgamma-rays associated with the de-excitation of the first-excited state of 12 C. Again, the same experimental conditions were used for both sources. The shapes of these distributions are also very similar and agree well with previous data, each other, and the ISO recommendation. Our 238 PuBe source provides approximately 2.6 times more 4.44MeVgamma-rays and 2.4 times more neutrons over the tagged-neutron energy range, the latter in reasonable agreement with the original full-spectrum source-calibration measurements performed at the time of their acquisition. Copyright © 2017 The Authors. Published by Elsevier Ltd.. All rights reserved.

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

NASA Astrophysics Data System (ADS)

Wang, Zhong-liang; Yamada, Masatoshi

2005-05-01

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

A Method for Continuous (239)Pu Determinations in Arctic and Antarctic Ice Cores.

PubMed

Arienzo, M M; McConnell, J R; Chellman, N; Criscitiello, A S; Curran, M; Fritzsche, D; Kipfstuhl, S; Mulvaney, R; Nolan, M; Opel, T; Sigl, M; Steffensen, J P

2016-07-05

Atmospheric nuclear weapons testing (NWT) resulted in the injection of plutonium (Pu) into the atmosphere and subsequent global deposition. We present a new method for continuous semiquantitative measurement of (239)Pu in ice cores, which was used to develop annual records of fallout from NWT in ten ice cores from Greenland and Antarctica. The (239)Pu was measured directly using an inductively coupled plasma-sector field mass spectrometer, thereby reducing analysis time and increasing depth-resolution with respect to previous methods. To validate this method, we compared our one year averaged results to published (239)Pu records and other records of NWT. The (239)Pu profiles from the Arctic ice cores reflected global trends in NWT and were in agreement with discrete Pu profiles from lower latitude ice cores. The (239)Pu measurements in the Antarctic ice cores tracked low latitude NWT, consistent with previously published discrete records from Antarctica. Advantages of the continuous (239)Pu measurement method are (1) reduced sample preparation and analysis time; (2) no requirement for additional ice samples for NWT fallout determinations; (3) measurements are exactly coregistered with all other chemical, elemental, isotopic, and gas measurements from the continuous analytical system; and (4) the long half-life means the (239)Pu record is stable through time.

Temporal evolution of 137Cs, 237Np, and 239+240Pu and estimated vertical 239+240Pu export in the northwestern Mediterranean Sea.

PubMed

Bressac, M; Levy, I; Chamizo, E; La Rosa, J J; Povinec, P P; Gastaud, J; Oregioni, B

2017-10-01

The evolution of 137 Cs, 237 Np and 239+240 Pu at the DYFAMED station (NW Mediterranean) is discussed in relation to physical processes, downward fluxes of particles, and changes in the main input sources. The data set presented in this study represents the first complete 237 Np vertical profiles (0.12-0.27μBqL -1 ), and constitutes a baseline measurement to assess future changes. A similar behavior of Cs and Np has been evidenced, confirming that Np behaves conservatively. While the 137 Cs decrease has been driven by its radioactive decay, the vertical distribution of 237 Np has not substantially changed over the last decade. In the absence of recent major inputs, a homogenization of their vertical distribution occurred, partly due to deep convection events that became more intense during the last decade. In contrast, 239+240 Pu surface levels in the NW Mediterranean waters have fallen in the past four decades by a factor of 5. This decrease in surface has been balanced by higher concentrations in the deep-water layers. A first estimate of the downward 239+240 Pu fluxes in the NW Mediterranean Sea is proposed over more than two decades. This estimation, based on the DYFAMED sediment trap time-series data and published 239+240 Pu flux measurements, suggests that sinking particles have accounted for 60-90% of the upper layer (0-200m) Pu inventory loss over the period 1989-2013. The upper layer residence time of Pu is estimated to be ~28years, twice as long as the residence time estimated for the whole western Mediterranean (~15years). This difference highlights the slow removal of Pu in the open waters of the NW Mediterranean and confirms that most of the Pu removal occurs along the coastal margin where sedimentation rates are high. Copyright © 2017 Elsevier B.V. All rights reserved.

Fission fragment yield distribution in the heavy-mass region from the 239Pu (nth,f ) reaction

NASA Astrophysics Data System (ADS)

Gupta, Y. K.; Biswas, D. C.; Serot, O.; Bernard, D.; Litaize, O.; Julien-Laferrière, S.; Chebboubi, A.; Kessedjian, G.; Sage, C.; Blanc, A.; Faust, H.; Köster, U.; Ebran, A.; Mathieu, L.; Letourneau, A.; Materna, T.; Panebianco, S.

2017-07-01

The fission fragment yield distribution has been measured in the 239Pu(nth,f ) reaction in the mass region of A =126 to 150 using the Lohengrin recoil-mass spectrometer. Three independent experimental campaigns were performed, allowing a significant reduction of the uncertainties compared to evaluated nuclear data libraries. The long-standing discrepancy of around 10% for the relative yield of A =134 reported in JEF-2.2 and JEFF-3.1.1 data libraries is finally solved. Moreover, the measured mass distribution in thermal neutron-induced fission does not show any significant dip around the shell closure (A =136 ) as seen in heavy-ion fission data of 208Pb(18O, f ) and 238U(18O, f ) reactions. Lastly, comparisons between our experimental data and the predictions from Monte Carlo codes (gef and fifrelin) are presented and discussed.

Energy Dependence of Fission Product Yields from 235U, 238U and 239Pu for Incident Neutron Energies Between 0.5 and 14.8 MeV

NASA Astrophysics Data System (ADS)

Gooden, M. E.; Arnold, C. W.; Becker, J. A.; Bhatia, C.; Bhike, M.; Bond, E. M.; Bredeweg, T. A.; Fallin, B.; Fowler, M. M.; Howell, C. R.; Kelley, J. H.; Krishichayan; Macri, R.; Rusev, G.; Ryan, C.; Sheets, S. A.; Stoyer, M. A.; Tonchev, A. P.; Tornow, W.; Vieira, D. J.; Wilhelmy, J. B.

2016-01-01

Fission Product Yields (FPY) have historically been one of the most observable features of the fission process. They are known to have strong variations that are dependent on the fissioning species, the excitation energy, and the angular momentum of the compound system. However, consistent and systematic studies of the variation of these FPY with energy have proved challenging. This is caused primarily by the nature of the experiments that have traditionally relied on radiochemical procedures to isolate specific fission products. Although radiochemical procedures exist that can isolate all products, each element presents specific challenges and introduces varying degrees of systematic errors that can make inter-comparison of FPY uncertain. Although of high importance in fields such as nuclear forensics and Stockpile Stewardship, accurate information about the energy dependence of neutron induced FPY are sparse, due primarily to the lack of suitable monoenergetic neutron sources. There is a clear need for improved data, and to address this issue, a collaboration was formed between Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL) and the Triangle Universities Nuclear Laboratory (TUNL) to measure the energy dependence of FPY for 235U, 238U and 239Pu. The measurements have been performed at TUNL, using a 10 MV Tandem Van de Graaff accelerator to produce monoenergetic neutrons at energies between 0.6 MeV to 14.8 MeV through a variety of reactions. The measurements have utilized a dual-fission chamber, with thin (10-100 μg/cm2) reference foils of similar material to a thick (100-400 mg) activation target held in the center between the chambers. This method allows for the accurate determination of the number of fissions that occurred in the thick target without requiring knowledge of the fission cross section or neutron fluence on target. Following activation, the thick target was removed from the dual-fission chamber and gamma

Energy dependence of fission product yields from 235U, 238U and 239Pu for incident neutron energies between 0.5 and 14.8 MeV

DOE PAGES

Gooden, M. E.; Arnold, C. W.; Becker, J. A.; ...

2016-01-06

In this study, Fission Product Yields (FPY) have historically been one of the most observable features of the fission process. They are known to have strong variations that are dependent on the fissioning species, the excitation energy, and the angular momentum of the compound system. However, consistent and systematic studies of the variation of these FPY with energy have proved challenging. This is caused primarily by the nature of the experiments that have traditionally relied on radiochemical procedures to isolate specific fission products. Although radiochemical procedures exist that can isolate all products, each element presents specific challenges and introduces varyingmore » degrees of systematic errors that can make inter-comparison of FPY uncertain. Although of high importance in fields such as nuclear forensics and Stockpile Stewardship, accurate information about the energy dependence of neutron induced FPY are sparse, due primarily to the lack of suitable monoenergetic neutron sources. There is a clear need for improved data, and to address this issue, a collaboration was formed between Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL) and the Triangle Universities Nuclear Laboratory (TUNL) to measure the energy dependence of FPY for 235U, 238U and 239Pu. The measurements have been performed at TUNL, using a 10 MV Tandem Van de Graaff accelerator to produce monoenergetic neutrons at energies between 0.6 MeV to 14.8 MeV through a variety of reactions. The measurements have utilized a dual-fission chamber, with thin (10-100 μg/cm2) reference foils of similar material to a thick (100-400 mg) activation target held in the center between the chambers. This method allows for the accurate determination of the number of fissions that occurred in the thick target without requiring knowledge of the fission cross section or neutron fluence on target. Following activation, the thick target was removed from the dual

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.

Primary liver tumors in beagle dogs exposed by inhalation to aerosols of plutonium-238 dioxide

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

Gillett, N.A.; Muggenburg, B.A.; Mewhinney, J.A.

1988-11-01

Primary liver tumors developed in Beagle dogs exposed by inhalation to aerosols of /sup 238/PuO/sub 2/. Initial deposition of /sup 238/PuO/sub 2/ in the respiratory tract was followed by translocation of a portion of the /sup 238/Pu to the liver and skeleton, which resulted in a large dose commitment and tumor risk to all three tissues. In a population of 144 dogs exposed to /sup 238/PuO/sub 2/, 112 dogs died or were killed 4000 days after /sup 238/Pu exposure, 100 dogs had osteosarcoma, and 28 dogs had lung cancers. At increasing times after exposure, however, liver lesions have become moremore » pronounced. Ten primary liver tumors in nine animals were diagnosed in the dogs dying before 4000 days after exposure. An additional five primary liver tumors in three dogs occurred in 9 animals killed after 4000 days after exposure. The majority of these tumors have been fibrosarcomas. The liver tumors were usually not the cause of death, and rarely metastasized. The occurrence of liver tumors in this study indicates that /sup 238/Pu is an effective hepatic carcinogen. Liver carcinogenesis is assuming an increasing importance in this study at late times after inhalation exposure. These results suggest that the liver may be an important organ at risk for the development of neoplasia in humans at time periods long after inhalation of /sup 238/Pu.« less

Development of an Efficient Approach to Perform Neutronics Simulations for Plutonium-238 Production

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

Chandler, David; Ellis, Ronald James

Conversion of 238Pu decay heat into usable electricity is imperative to power National Aeronautics and Space Administration (NASA) deep space exploration missions; however, the current stockpile of 238Pu is diminishing and the quality is less than ideal. In response, the US Department of Energy and NASA have undertaken a program to reestablish a domestic 238Pu production program and a technology demonstration sub-project has been initiated. Neutronics simulations for 238Pu production play a vital role in this project because the results guide reactor safety-basis, target design and optimization, and post-irradiation examination activities. A new, efficient neutronics simulation tool written in Pythonmore » was developed to evaluate, with the highest fidelity possible with approved tools, the time-dependent nuclide evolution and heat deposition rates in 238Pu production targets irradiated in the High Flux Isotope Reactor (HFIR). The Python Activation and Heat Deposition Script (PAHDS) was developed specifically for experiment analysis in HFIR and couples the MCNP5 and SCALE 6.1.3 software quality assured tools to take advantage of an existing high-fidelity MCNP HFIR model, the most up-to-date ORIGEN code, and the most up-to-date nuclear data. Three cycle simulations were performed with PAHDS implementing ENDF/B-VII.0, ENDF/B-VII.1, and the Hybrid Library GPD-Rev0 cross-section libraries. The 238Pu production results were benchmarked against VESTA-obtained results and the impact of various cross-section libraries on the calculated metrics were assessed.« less

Chelation of /sup 238/Pu(IV) in vivo by 3,4,3-LICAM(C): Effects of ligand methylation and pH

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

Durbin, P.W.; White, D.L.; Jeung, N.L.

1989-06-01

The linear tetracarboxycatecholate ligand, 3,4,3-LICAM(C) N1,N5,N10,N14-tetrakis(2,3-dihydroxy-4-carboxybenzoyl-tetraaza tet radecane, tetra sodium salt) injected within 1 h after injection of Pu(IV) citrate, removes about the same fraction of Pu from animals as CaNa3-DTPA but removes less inhaled Pu than CaNa3-DTPA and leaves a Pu residue in the renal cortex. However, the formation constant of the expected Pu-3,4,3-LICAM(C) complexes are orders of magnitude greater than that of Pu-DTPA, and 3,4,3-LICAM(C) is 100 times more efficient than CaNa3-DTPA for removing Pu from transferrin in vitro. Because the formation constants of their actinide complexes are central to in vivo actinide chelation, ligand design strategies aremore » dominated by the search for ligands with large Pu complex stabilities, and it was necessary to explain the failure of 3,4,3-LICAM(C) to achieve its thermodynamic potential in vivo. All the batches of 3,4,3-LICAM(C) prepared at Berkeley or in France (Euro-LICAM(C)) were found by high-pressure liquid chromatography to be mixtures of the pure ligand (55% in Berkeley preparations, 8.5% in Euro-LICAM(C)) and its four methylesters. A revised synthesis for 3,4,3-LICAM(C) is appended to this report. All of the incompletely hydrolyzed 3,4,3-LICAM(C) preparations and the pure ligand were tested for removal of Pu from mice (238Pu(IV) citrate intravenous, 30 mumol kg-1 of ligand at 1 h, kill at 24 h, radioanalyze tissues and separated excretal). The presence of methylesters did not significantly impair the ability of the ligands to remove Pu from mice, and it did not alter the fraction of injected Pu deposited in kidneys. Temporary elevation (reduction) of plasma and urine pH of mice by 0.5 mL of 0.1 M NaHCO3 (NH4Cl) injected before or simultaneously with pure 3,4,3-LICAM(C) somewhat improved (significantly reduced) Pu excretion but had little influence on Pu deposition in kidneys.« less

Cryoconites from Alpine glaciers: Radionuclide accumulation and age estimation with Pu and Cs isotopes and 210Pb.

PubMed

Wilflinger, T; Lettner, H; Hubmer, A; Bossew, P; Sattler, B; Slupetzky, H

2018-06-01

Cryoconites ("cold dust", derived from the Greek) are aeolian sediments accumulated on glacier surfaces. In cryoconites from the surface of the Stubacher Sonnblickkees, a temperate Austrian glacier, extremely high activity concentrations of artificial and natural radionuclides were found. Artificial radionuclides stem from two clearly distinguishable sources, global fallout from the nuclear weapons testing era deposited over a period of years until roughly 1966 and the fallout from Chernobyl in 1986, which was essentially deposited as a single input during one week. Anthropogenic radionuclides identified were 137 Cs, 134 Cs, 238 Pu, 239+240 Pu, 90 Sr, 241 Am, 60 Co, 125 Sb, 154 Eu, and 207 Bi. The naturally occurring radionuclides detected were the long-lived radon decay product 210 Pb, the primordial radionuclide 4  K and the cosmogenic 7 Be. Isotopic ratios of 134 Cs/ 137 Cs and 239+240 Pu/ 238 Pu were used to separate the nuclide inventory into the contributions of the two aforementioned sources, which show varying degrees of mixing and provide information on the mixing age of the cryoconites. Since isotopic ratios of Pu often have high uncertainties due to low absolute concentrations, age estimation based on this method can be quite inaccurate. Additional information about the age of cryoconites was obtained through analysis of 210 Pb, which is constantly deposited over time. Copyright © 2017. Published by Elsevier Ltd.

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

High-temperature deformation of stoichiometric /sup 239/PuO/sub 2/

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

Petrovic, J.J.; Land, C.C.

1980-03-01

The deformation behavior of stoichiometric /sup 239/PuO/sub 2/ was examined at 800/sup 0/ to 1500/sup 0/C, using direct and diametral compression. Maximum ductility was observed at 1000/sup 0/C, but above this temperature both strength and ductility decreased and the fracture mode changed from transgranular to intergranular. The deformation activation energy measured at 1000/sup 0/C was 598 kJ/mol. Comparison to the deformation behavior of hypostoichiometric /sup 239/PuO/sub 2-x/ suggests that high-temperature dislocation motion becomes more difficult with increasing O/Pu ratio due to effects of stoichiometry on diffusion rates. Deformation mechanisms in /sup 239/PuO/sub 2/ appear to be a combination of dislocationmore » motion and grain-boundary sliding.« less

²³⁹Pu and ²⁴⁰Pu inventories and ²⁴⁰Pu/²³⁹Pu atom ratios in the equatorial Pacific Ocean water column.

PubMed

Yamada, Masatoshi; Zheng, Jian

2012-07-15

The (239+240)Pu concentrations and (240)Pu/(239)Pu atom ratios were determined by alpha spectrometry and inductively coupled plasma mass spectrometry for seawater samples from two stations, one at the equator and the other in the equatorial South Pacific. To better understand the fate of Pu isotopes, this study dealt with the contribution of the close-in fallout Pu from the Pacific Proving Grounds (PPG) in water columns of the Pacific Ocean. The (239)Pu, (240)Pu and (239+240)Pu inventories over the depth interval 0-3000 m at the equator station were 10.4, 8.9 and 19.3 Bq m(-2), respectively. Further, no noticeable difference was observed in (239)Pu, (240)Pu and (239+240)Pu inventories over the depth interval 0-3000 m between the two stations. The total (239+240)Pu inventories were significantly higher than the expected cumulative deposition density of global fallout. Water column (239+240)Pu inventories measured in this study were lower than those reported for comparable stations in the Geochemical Ocean Sections Study, indicating that these inventories have been decreasing at average rates of 0.89 ± 0.07 and 0.16 ± 0.07 Bq m(-2)yr(-1) at the equator and equatorial South Pacific stations, respectively, from 1973 to 1990. The obtained (240)Pu/(239)Pu atom ratios were higher than the mean global fallout ratio of 0.18. These high atom ratios proved the existence of close-in tropospheric fallout Pu from the PPG in the Marshall Islands. The (239+240)Pu inventories originating from the close-in fallout in the entire water column were estimated to be 11.1 Bq m(-2) at the equator station and 7.1 Bq m(-2) at the equatorial South Pacific Ocean station, and the relative percentages of close-in fallout Pu were 40% at the former and 34% at the latter. A significant amount of close-in fallout Pu originating from the PPG has been transported to deep layers below the 1000 m depth in the equatorial Pacific Ocean. Copyright © 2012 Elsevier B.V. All rights reserved.

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

PubMed

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

2008-09-01

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

An Update on the Status of the Supply of Plutonium-238 for Future NASA Missions

NASA Astrophysics Data System (ADS)

Wham, R. M.

2016-12-01

For more than five decades, Radioisotope Power Systems (RPSs) have enabled space missions to operate in locations where the Sun's intensity is too weak, obscured, or otherwise inadequate for solar power or other conventional power‒generation technologies. The natural decay heat (0.57 W/g) from the radioisotope, plutonium-238 (238Pu), provides the thermal energy source used by an RPS to generate electricity for operation of instrumentation, as well as heat to keep key subsystems warm for missions such as Voyagers 1 and 2, the Cassini mission to Saturn, the New Horizons flyby of Pluto, and the Mars Curiosity rover which were sponsored by the National Aeronautics and Space Administration (NASA). Plutonium-238 is produced by irradiation of neptunium-237 in a nuclear reactor a relatively high neutron flux. The United States has not produced new quantities of 238Pu since the early 1990s. RPS‒powered missions have continued since then using existing 238Pu inventory managed by the U.S. Department of Energy (DOE), including material purchased from Russia. A new domestic supply is needed to ensure the continued availability of RPSs for future NASA missions. NASA and DOE are currently executing a project to reestablish a 238Pu supply capability using its existing facilities and reactors, which are much smaller than the large-scale production reactors and processing canyon equipment used previously. The project is led by the Oak Ridge National Laboratory (ORNL). Target rods, containing NpO2, will be fabricated at ORNL and irradiated in the ORNL High Flux Isotope Reactor and the Advanced Test Reactor at Idaho National Laboratory. Irradiated targets will be processed in chemical separations at the ORNL Radiochemical Engineering Center to recover the plutonium product and unconverted neptunium for recycle. The 238PuO2 product will be shipped to Los Alamos National Laboratory for fabrication of heat source pellets. Key activities, such as transport of the neptunium to ORNL

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

Transfer of aged Pu to cattle grazing on a contaminated environment

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

Gilbert, R.O.; Engel, D.W.; Smith, D.D.

1988-03-01

Estimates are obtained of the fraction of ingested or inhaled 239+240Pu transferred to blood and tissues of a reproducing herd of beef cattle, individuals of which grazed within fenced enclosures for up to 1064 d under natural conditions with no supplemental feeding at an arid site contaminated 16 y previously with Pu oxide. The estimated (geometric mean (GM)) fraction of Pu transferred from the gastrointestinal tract to blood serum was about 5 x 10(-6) (geometric standard error (GSE) = 1.4) with an approximate upper bound of about 2 x 10(-5). These results are in reasonable agreement with the value ofmore » 1 x 10(-5) recommended for human radiation protection purposes by the International Commission on Radiological Protection (ICRP) for insoluble Pu oxides that are free of very small particles. Also, results from a laboratory study by Stanley (St75), in which large doses of /sup 238/Pu were orally administered daily to dairy cattle for 19 consecutive days, suggest that aged 239+240Pu at this arid grazing site may not be more biologically available to blood serum than fresh 239+240Pu oxide. The estimated fractions of 239+240Pu transferred from blood serum to tissues of adult grazing cattle were: femur (3.2 X 10(-2), 1.8; GM, GSE), vertebra (1.4 X 10(-1), 1.6), liver (2.3 X 10(-1), 2.0), muscle (1.3 X 10(-1), 1.9), female gonads (7.9 X 10(-5), 1.5), and kidney (1.4 X 10(-3), 1.7). The blood-to-tissue fractional transfers for cattle initially exposed in utero were greater than those exposed only as adults by a factor of about 4 for femur (statistically significant) and of about 2 for other tissues (not significant). The estimated (GM) fraction of inhaled Pu initially deposited in the pulmonary lung was 0.34 (GSE = 1.3) for adults and 0.15 (GSE = 1.3) for cattle initially exposed in utero (a statistically significant difference).« less

Extension of 239+240Pu sediment geochronology to coarse-grained marine sediments

USGS Publications Warehouse

Kuehl, Steven A.; Ketterer, Michael E.; Miselis, Jennifer L.

2012-01-01

Sediment geochronology of coastal sedimentary environments dominated by sand has been extremely limited because concentrations of natural and bomb-fallout radionuclides are often below the limit of measurement using standard techniques. ICP-MS analyses of 239+240Pu from two sites representative of traditionally challenging (i.e., low concentration) environments provide a "proof of concept" and demonstrate a new application for bomb-fallout radiotracers in the study of sandy shelf-seabed dynamics. A kasten core from the New Zealand shelf in the Southern Hemisphere (low fallout), and a vibracore from the sandy nearshore of North Carolina (low particle surface area) both reveal measurable 239+240Pu activities at depth. In the case of the New Zealand site, independently verified steady-state sedimentation results in a 239+240Pu profile that mimics the expected atmospheric fallout. The depth profile of 239+240Pu in the North Carolina core is more uniform, indicating significant sediment resuspension, which would be expected in this energetic nearshore environment. This study, for the first time, demonstrates the utility of 239+240Pu in the study of sandy environments, significantly extending the application of bomb-fallout isotopes to coarse-grained sediments, which compose the majority of nearshore regions.

Neutron capture cross-section measurements for 238U between 0.4 and 1.4 MeV

NASA Astrophysics Data System (ADS)

Krishichayan, Fnu; Finch, S. W.; Howell, C. R.; Tonchev, A. P.; Tornow, W.

2017-09-01

Neutron-induced radiative-capture cross-section data of 238U are crucial for fundamental nuclear physics as well as for Stewardship Science, for advanced-fuel-cycle calculations, and for nuclear astrophysics. Based on different techniques, there are a large number of 238U(n, γ) 239U cross-section data available in the literature. However, there is a lack of systematic and consistent measurements in the 0.1 to 3.0 MeV energy range. The goal of the neutron-capture project at TUNL is to provide accurate 238U(n, γ) 239U cross-section data in this energy range. The 238U samples, sandwiched between gold foils of the same size, were irradiated for 8-14 hours with monoenergetic neutrons. To avoid any contribution from thermal neutrons, the 238U and 197Au targets were placed inside of a thin-walled pill-box made of 238U. Finally, the whole pill-box was wrapped in a gold foil as well. After irradiation, the samples were gamma-counted at the TUNL's low-background counting facility using high-efficient HPGe detectors. The 197Au monitor foils were used to calculate the neutron flux. The experimental technique and 238U(n, γ) 239U cross-section results at 6 energies will be discussed during the meeting.

A Signature Distinguishing Fissile From Non-Fissile Materials Using Linearly Polarized Gamma Rays

NASA Astrophysics Data System (ADS)

Mueller, J. M.; Ahmed, M. W.; Karwowski, H. J.; Myers, L. S.; Sikora, M. H.; Stave, S.; Tompkins, J. R.; Zimmerman, W. R.; Weller, H. R.

2013-04-01

Photofission of ^233,235,238U, ^239,240Pu, and ^232Th was induced by nearly 100% linearly polarized, high intensity (˜10^7 γs per second), and nearly-monoenergetic γ-ray beams of energies between 5.6 and 7.3 MeV at the High Intensity γ-ray Source (HIγS). An array of 18 liquid scintillating detectors was used to measure prompt fission neutron angular distributions. The ratio of prompt fission neutron yields parallel to the plane of beam polarization to the yields perpendicular to this plane was measured as a function of beam and neutron energy, as described in a recent publication showing results from ^235,238U, ^239Pu, and ^232Th [1]. A ratio near unity was found for ^233,235U and ^239Pu while a significant ratio (˜1.5-3) was found for ^238U, ^240Pu, and ^232Th. This large difference could be used to distinguish fissile isotopes (such as ^233,235U and ^239Pu) from non-fissile isotopes (such as ^238U, ^240Pu, and ^232Th). Polarization ratios as a function of the relative abundance of fissile to non-fissile isotopes will be presented. [4pt] [1] J. M. Mueller et al., Phys. Rev. C 85, 014605 (2012).

Energy Dependence of Fission Product Yields from {sup 235}U, {sup 238}U and {sup 239}Pu for Incident Neutron Energies Between 0.5 and 14.8 MeV

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

Gooden, M.E., E-mail: m_gooden@lanl.gov; Arnold, C.W.; Becker, J.A.

2016-01-15

Fission Product Yields (FPY) have historically been one of the most observable features of the fission process. They are known to have strong variations that are dependent on the fissioning species, the excitation energy, and the angular momentum of the compound system. However, consistent and systematic studies of the variation of these FPY with energy have proved challenging. This is caused primarily by the nature of the experiments that have traditionally relied on radiochemical procedures to isolate specific fission products. Although radiochemical procedures exist that can isolate all products, each element presents specific challenges and introduces varying degrees of systematicmore » errors that can make inter-comparison of FPY uncertain. Although of high importance in fields such as nuclear forensics and Stockpile Stewardship, accurate information about the energy dependence of neutron induced FPY are sparse, due primarily to the lack of suitable monoenergetic neutron sources. There is a clear need for improved data, and to address this issue, a collaboration was formed between Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL) and the Triangle Universities Nuclear Laboratory (TUNL) to measure the energy dependence of FPY for {sup 235}U, {sup 238}U and {sup 239}Pu. The measurements have been performed at TUNL, using a 10 MV Tandem Van de Graaff accelerator to produce monoenergetic neutrons at energies between 0.6 MeV to 14.8 MeV through a variety of reactions. The measurements have utilized a dual-fission chamber, with thin (10-100 μg/cm2) reference foils of similar material to a thick (100-400 mg) activation target held in the center between the chambers. This method allows for the accurate determination of the number of fissions that occurred in the thick target without requiring knowledge of the fission cross section or neutron fluence on target. Following activation, the thick target was removed from the dual

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

Surrogate 239Pu(n, fxn) and 241Pu(n, fxn) average fission-neutron-multiplicity measurements

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

Burke, J. T.; Alan, B. S.; Akindele, O. A.

2017-09-26

We have constructed a new neutron-charged-particle detector array called NeutronSTARS. It has been described extensively in LLNL-TR-703909 [1] and Akindele et al [2]. We have used this new neutron-charged-particle array to measure the 241Pu and 239Pu fissionneutron multiplicity as a function of equivalent incident-neutron energy from 100 keV to 20 MeV. The experimental approach, detector array, data analysis, and results are summarized in the following sections.

Chelation therapy of incorporated plutonium-238 and americium-241: comparison of LICAM(C), DTPA and DFOA in rats, hamsters and mice.

PubMed

Volf, V

1986-03-01

The carboxylated catechoylamide 3,4,3-LICAM(C) was tested for removal of 238Pu and 241Am from small laboratory rodents. The effectiveness of treatment was compared with that of two ligand preparations approved for clinical use: calcium-trisodium diethylenetriaminepentaacetate (DTPA) and desferrioxamine (DFOA). With early treatment and at the dosage used clinically for the decorporation of actinides with DTPA (30 mumol/kg body weight) LICAM(C) was superior to DFOA but when compared with DTPA, the effect of LICAM(C) on 238Pu was greater only in bone; as little as 1 mumol LICAM(C)/kg was as effective as 30 mumol DTPA/kg. However, in all animals treated with LICAM(C) there was a large increase in the 238Pu content of the kidney. With 241Am the effect of DTPA was always superior to that of LICAM(C). The best overall results early (1 day) after injection of 238Pu and 241Am were achieved by a combination of a single injection of LICAM(C) and DTPA with subsequent continuous administration of DTPA in drinking water. LICAM(C) affected the retention of 238Pu even if given orally; the data suggested that about 3 per cent of ingested LICAM(C) was absorbed. When the beginning of treatment was delayed, LICAM(C) became equally effective or less effective than DTPA even as far as 238Pu retention in bone was concerned, but it still increased the accumulation of 238Pu in the kidneys.

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.

Pu-239+240 and Cs-137 in Montenegro soil: their correlation and origin.

PubMed

Antovic, Nevenka M; Vukotic, Perko; Svrkota, Nikola; Andrukhovich, Sergey K

2012-08-01

The (239+240)Pu activity concentrations in soil from Montenegro (six samples from three localities) have been measured for the first time. The alpha and gamma-spectrometric measurements are used to determine the (239+240)Pu/(137)Cs activity ratio, and it was found to be with an average of 0.02 and standard deviation of 0.007. This average activity ratio was applied to estimate (239+240)Pu in soil samples from the other 21 localities at which (137)Cs activity concentrations were measured. In this research obtained (either experimentally or estimated) (239+240)Pu activity concentrations (0.036-8.265 Bq kg(-1)) are comparable with those measured in some other European countries. On the basis of the results obtained in the present study and a survey of relevant literature, it is possible to conclude that Chernobyl contribution to (137)Cs contamination of Montenegro soils is dominant, whilst Pu contamination comes from the global fallout of nuclear weapon tests. Copyright © 2012 Elsevier Ltd. All rights reserved.

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

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

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

1975-01-01

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

Results of the Excreta Bioassay Quality Control Program for April 1, 2009 through March 31, 2010

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

Antonio, Cheryl L.

2012-07-19

A total of 58 urine samples and 10 fecal samples were submitted during the report period (April 1, 2009 through March 31, 2010) to General Engineering Laboratories, South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for Sr, 238Pu, 239Pu, 241Am, 243Am 235U, 238U, elemental uranium and fecal analyses for 241Am, 238Pu and 239Pu were tested this year as well as four tissue samples for 238Pu, 239Pu, 241Am and 241Pu. The number of QC urine samples submitted during the report period represented 1.3% of the total samplesmore » submitted. In addition to the samples provided by IDP, GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 33% of the analyses processed by GEL during the third year of this contract were quality control samples. GEL tested the performance of 21 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty (Table 4).« less

Neutron induced fission cross section measurements of 240Pu and 242Pu

NASA Astrophysics Data System (ADS)

Belloni, F.; Eykens, R.; Heyse, J.; Matei, C.; Moens, A.; Nolte, R.; Plompen, A. J. M.; Richter, S.; Sibbens, G.; Vanleeuw, D.; Wynants, R.

2017-09-01

Accurate neutron induced fission cross section of 240Pu and 242Pu are required in view of making nuclear technology safer and more efficient to meet the upcoming needs for the future generation of nuclear power plants (GEN-IV). The probability for a neutron to induce such reactions figures in the NEA Nuclear Data High Priority Request List [1]. A measurement campaign to determine neutron induced fission cross sections of 240Pu and 242Pu at 2.51 MeV and 14.83 MeV has been carried out at the 3.7 MV Van De Graaff linear accelerator at Physikalisch-Technische Bundesanstalt (PTB) in Braunschweig. Two identical Frisch Grid fission chambers, housing back to back a 238U and a APu target (A = 240 or A = 242), were employed to detect the total fission yield. The targets were molecular plated on 0.25 mm aluminium foils kept at ground potential and the employed gas was P10. The neutron fluence was measured with the proton recoil telescope (T1), which is the German primary standard for neutron fluence measurements. The two measurements were related using a De Pangher long counter and the charge as monitors. The experimental results have an average uncertainty of 3-4% at 2.51 MeV and for 6-8% at 14.81 MeV and have been compared to the data available in literature.

Multinucleon transfer in central collisions of 238U+238U

NASA Astrophysics Data System (ADS)

Ayik, S.; Yilmaz, B.; Yilmaz, O.; Umar, A. S.; Turan, G.

2017-08-01

Quantal diffusion mechanism of nucleon exchange is studied in the central collisions of 238U+238U in the framework of the stochastic mean-field (SMF) approach. For bombarding energies considered in this work, the dinuclear structure is maintained during the collision. Hence, it is possible to describe nucleon exchange as a diffusion process for mass and charge asymmetry. Quantal neutron and proton diffusion coefficients, including memory effects, are extracted from the SMF approach and the primary fragment distributions are calculated.

Chemical potential of oxygen in (U, Pu) mixed oxide with Pu/(U+Pu) = 0.46

NASA Astrophysics Data System (ADS)

Dawar, Rimpi; Chandramouli, V.; Anthonysamy, S.

2016-05-01

Chemical potential of oxygen in (U,Pu) mixed oxide with Pu/(U + Pu) = 0.46 was measured for the first time using H2/H2O gas equilibration combined with solid electrolyte EMF technique at 1073, 1273 and 1473 K covering an oxygen potential range of -525 to -325 kJ mol-1. The effect of oxygen potential on the oxygen to metal ratio was determined. Increase in oxygen potential increases the O/M. In this study the minimum O/M obtained was 1.985 below which reduction was not possible. Partial molar enthalpy ΔHbar O2 and entropy ΔSbar O2 of oxygen were calculated from the oxygen potential data. The values of -752.36 kJ mol-1 and 0.25 kJ mol-1 were obtained for ΔHbar O2 and ΔSbar O2 respectively.

Feasibility study of 235U and 239Pu characterization in radioactive waste drums using neutron-induced fission delayed gamma rays

NASA Astrophysics Data System (ADS)

Nicol, T.; Pérot, B.; Carasco, C.; Brackx, E.; Mariani, A.; Passard, C.; Mauerhofer, E.; Collot, J.

2016-10-01

This paper reports a feasibility study of 235U and 239Pu characterization in 225 L bituminized waste drums or 200 L concrete waste drums, by detecting delayed fission gamma rays between the pulses of a deuterium-tritium neutron generator. The delayed gamma yields were first measured with bare samples of 235U and 239Pu in REGAIN, a facility dedicated to the assay of 118 L waste drums by Prompt Gamma Neutron Activation Analysis (PGNAA) at CEA Cadarache, France. Detectability in the waste drums is then assessed using the MCNPX model of MEDINA (Multi Element Detection based on Instrumental Neutron Activation), another PGNAA cell dedicated to 200 L drums at FZJ, Germany. For the bituminized waste drum, performances are severely hampered by the high gamma background due to 137Cs, which requires the use of collimator and shield to avoid electronics saturation, these elements being very penalizing for the detection of the weak delayed gamma signal. However, for lower activity concrete drums, detection limits range from 10 to 290 g of 235U or 239Pu, depending on the delayed gamma rays of interest. These detection limits have been determined by using MCNPX to calculate the delayed gamma useful signal, and by measuring the experimental gamma background in MEDINA with a 200 L concrete drum mock-up. The performances could be significantly improved by using a higher interrogating neutron emission and an optimized experimental setup, which would allow characterizing nuclear materials in a wide range of low and medium activity waste packages.

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.

Predictive model of early mortality following acute inhalation of PuO/sub 2/ aerosols. [Extrapolation of beagle data to man

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

Raabe, O.G.; Goldman, M.

Since data on the pulmonary toxicity of plutonium in people are not available, estimates must be based upon available experimental animal data. For this purpose, inhalation studies with beagle dogs exposed to aerosols of /sup 238/PuO/sub 2/ and /sup 239/PuO/sub 2/ were analyzed and a simple model has been proposed to describe apparent dose-response relationships. It was found that for each aerosol and radionuclide form, the cumulative absorbed lung dose that leads to death from lung damage up to 1000 days could be assumed to have a log-normal distribution of values that was independent of time to death. The datamore » was satisfactorily fit to a model in which the time of death postexposure is given by: t = (K/D), with the time to death, the cumulative dose to lung tissue (the killing dose), and anti D the average dose rate to lung tissue from time of exposure to death. The ratios of median K values, normalized to the value for /sup 90/Sr--Y FAP, indicate a relative biological effectiveness (RBE) of 14 for /sup 239/PuO/sub 2/ particles and 5 for /sup 238/PuO/sub 2/ particles. This demonstrates an effect of particle specific activity on relative biological effectiveness for early mortality, since an increase in specific activity of particles leads to a lower apparent RBE.« less

Certified reference materials for radionuclides in Bikini Atoll sediment (IAEA-410) and Pacific Ocean sediment (IAEA-412).

PubMed

Pham, M K; van Beek, P; Carvalho, F P; Chamizo, E; Degering, D; Engeler, C; Gascó, C; Gurriaran, R; Hanley, O; Harms, A V; Herrmann, J; Hult, M; Ikeuchi, Y; Ilchmann, C; Kanisch, G; Kis-Benedek, G; Kloster, M; Laubenstein, M; Llaurado, M; Mas, J L; Nakano, M; Nielsen, S P; Osvath, I; Povinec, P P; Rieth, U; Schikowski, J; Smedley, P A; Suplinska, M; Sýkora, I; Tarjan, S; Varga, B; Vasileva, E; Zalewska, T; Zhou, W

2016-03-01

The preparation and characterization of certified reference materials (CRMs) for radionuclide content in sediments collected offshore of Bikini Atoll (IAEA-410) and in the open northwest Pacific Ocean (IAEA-412) are described and the results of the certification process are presented. The certified radionuclides include: (40)K, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (232)Th, (234)U, (238)U, (239)Pu, (239+240)Pu and (241)Am for IAEA-410 and (40)K, (137)Cs, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (232)Th, (235)U, (238)U, (239)Pu, (240)Pu and (239+240)Pu for IAEA-412. The CRMs can be used for quality assurance and quality control purposes in the analysis of radionuclides in sediments, for development and validation of analytical methods and for staff training. Copyright © 2015 Elsevier Ltd. All rights reserved.

Estimates of (239+240)Pu inventories in Gdańsk Bay and Gdańsk basin.

PubMed

Skwarzec, Bogdan; Strumińska, Dagmara I; Prucnal, Małgorzata

2003-01-01

This paper presents and discusses the results of (239+240)Pu determinations in different components of Gdańsk bay and Gdańsk basin ecosystem, as well as estimated sources and inventories of plutonium in these basins. The total plutonium (239+240)Pu activities deposited in Gdańsk bay and Gdańsk basin sediments are 1.18 TBq and 3.77 TBq, respectively. Two rivers, the Vistula and Neman rivers, and atmospheric fallout were distinguished as the main sources of plutonium in these basins. In seawater (with suspended matter included) there is about 2.33 GBq (239+240)Pu (0.2% of total activity) in Gdańsk bay and 9.92 GBq (239+240)Pu (0.3% of total activity) in Gdańsk basin. In both cases, 56% of (239+240)Pu is associated with suspended matter. Organisms contain 3.81 MBq in Gdańsk bay and 7.45 MBq (239+240)Pu in Gdańsk basin. From this value in Gdańsk bay 82.1% of plutonium is associated with zoobenthos, 13.6% with phytobenthos, 1.6% with phytoplankton, 1.5% with zooplankton and 1.2% with fish. In Gdańsk basin, 83.2% is associated with zoobenthos, 7.5% with phytobenthos, 3.6% with phytoplankton, 3.2% with zooplankton and 2.5% with fish.

Evaluations of Energy Spectra of Neutrons Emitted Promptly in Neutron-induced Fission of 235 U and 239 Pu

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

Neudecker, Denise; Talou, Patrick; Kawano, Toshihiko

The energy spectra of neutrons emitted promptly in the neutron-induced fission reactions of 235U and 239Pu were re-evaluated for ENDF/B-VIII.0. The evaluations presented here are based on a careful modeling of all relevant physics processes, an extensive analysis of experimental data and a detailed quantification of pertinent uncertainties. Energy spectra of neutrons emitted in up to fourth chance fission are considered and both compound and pre-equilibrium processes are included. Also, important nuclear model parameters, such as the average total kinetic energy of the fission fragments and the multiple chance fission probabilities, and their uncertainties are estimated based on experimental knowledge,more » model information and evaluated data. In addition to experimental information already available for ENDF/B-VII.1, these new evaluations make use of recently published experimental data either of high precision or spanning a broad incident energy range, information on legacy measurements explaining discrepancies and recently measured data of the average total kinetic energy as a function of incident neutron energy. The resulting evaluated data and covariances agree well with the experimental database used for the evaluation. However, the evaluated spectra are softer than the 235U and 239Pu ENDF/B-VII.1, JENDL-4.0 and JEFF-3.2 evaluations for incident neutron energies E inc ≤ 1.5 MeV and E inc ≤ 5 MeV, respectively. For E inc > 5 MeV, the evaluated spectra show structures due to the improved modeling which are not present in ENDF/B-VII.1 and JEFF-3.2 but can be observed in JENDL-4.0 evaluations. Part of these new evaluations were adopted for ENDF/B-VIII.0, while the ENDF/B-VII.1 239Pu PFNS was retained for E inc ≤ 5 MeV awaiting more conclusive experimental evidence.« less

Evaluations of Energy Spectra of Neutrons Emitted Promptly in Neutron-induced Fission of 235 U and 239 Pu

DOE PAGES

Neudecker, Denise; Talou, Patrick; Kawano, Toshihiko; ...

2018-02-01

The energy spectra of neutrons emitted promptly in the neutron-induced fission reactions of 235U and 239Pu were re-evaluated for ENDF/B-VIII.0. The evaluations presented here are based on a careful modeling of all relevant physics processes, an extensive analysis of experimental data and a detailed quantification of pertinent uncertainties. Energy spectra of neutrons emitted in up to fourth chance fission are considered and both compound and pre-equilibrium processes are included. Also, important nuclear model parameters, such as the average total kinetic energy of the fission fragments and the multiple chance fission probabilities, and their uncertainties are estimated based on experimental knowledge,more » model information and evaluated data. In addition to experimental information already available for ENDF/B-VII.1, these new evaluations make use of recently published experimental data either of high precision or spanning a broad incident energy range, information on legacy measurements explaining discrepancies and recently measured data of the average total kinetic energy as a function of incident neutron energy. The resulting evaluated data and covariances agree well with the experimental database used for the evaluation. However, the evaluated spectra are softer than the 235U and 239Pu ENDF/B-VII.1, JENDL-4.0 and JEFF-3.2 evaluations for incident neutron energies E inc ≤ 1.5 MeV and E inc ≤ 5 MeV, respectively. For E inc > 5 MeV, the evaluated spectra show structures due to the improved modeling which are not present in ENDF/B-VII.1 and JEFF-3.2 but can be observed in JENDL-4.0 evaluations. Part of these new evaluations were adopted for ENDF/B-VIII.0, while the ENDF/B-VII.1 239Pu PFNS was retained for E inc ≤ 5 MeV awaiting more conclusive experimental evidence.« less

Evaluations of Energy Spectra of Neutrons Emitted Promptly in Neutron-induced Fission of 235U and 239Pu

NASA Astrophysics Data System (ADS)

Neudecker, D.; Talou, P.; Kawano, T.; Kahler, A. C.; White, M. C.; Taddeucci, T. N.; Haight, R. C.; Kiedrowski, B.; O'Donnell, J. M.; Gomez, J. A.; Kelly, K. J.; Devlin, M.; Rising, M. E.

2018-02-01

The energy spectra of neutrons emitted promptly in the neutron-induced fission reactions of 235U and 239Pu were re-evaluated for ENDF/B-VIII.0. These evaluations are based on a careful modeling of all relevant physics processes, an extensive analysis of experimental data and a detailed quantification of pertinent uncertainties. Energy spectra of neutrons emitted in up to fourth chance fission are considered and both compound and pre-equilibrium processes are included. Also, important nuclear model parameters, such as the average total kinetic energy of the fission fragments and the multiple chance fission probabilities, and their uncertainties are estimated based on experimental knowledge, model information and evaluated data. In addition to experimental information already available for ENDF/B-VII.1, these new evaluations make use of recently published experimental data either of high precision or spanning a broad incident energy range, information on legacy measurements explaining discrepancies and recently measured data of the average total kinetic energy as a function of incident neutron energy. The resulting evaluated data and covariances agree well with the experimental database used for the evaluation. However, the evaluated spectra are softer than the 235U and 239Pu ENDF/B-VII.1, JENDL-4.0 and JEFF-3.2 evaluations for incident neutron energies Einc ≤ 1.5 MeV and Einc ≤ 5 MeV, respectively. For Einc > 5 MeV, the evaluated spectra show structures due to the improved modeling which are not present in ENDF/B-VII.1 and JEFF-3.2 but can be observed in JENDL-4.0 evaluations. Part of these new evaluations were adopted for ENDF/B-VIII.0, while the ENDF/B-VII.1 239Pu PFNS was retained for Einc ≤ 5 MeV awaiting more conclusive experimental evidence.

Nuclear-powered pacemaker fuel cladding study. [Difficulty of dissolving cladding and /sup 238/PuO/sub 2/ for obtaining materials for acts of terrorism

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

Shoup, R.L.

1976-07-01

The fabrication of fuel capsules with refractory metal and alloy clads used in nuclear-powered cardiac pacemakers precludes the expedient dissolution of the clad in inorganic acid solutions. An experiment to measure penetration rates of acids on commonly used fuel pellet clads indicated that it is not impossible, but that it would be very difficult to dissolve the multiple cladding. This work was performed because of a suggestion that a /sup 238/PuO/sub 2/-powered pacemaker could be transformed into a terrorism weapon.

Tumorigenic target cell regions in bone marrow studied by localized dosimetry of 239Pu, 241Am and 233U in the mouse femur.

PubMed

Lord, B I; Austin, A L; Ellender, M; Haines, J W; Harrison, J D

2001-06-01

To study the temporal change in microdistribution of plutonium-239, americium-241 and uranium-233 in the mouse distal femur and to compare and combine calculated radiation doses with those obtained previously for the femoral shaft. Also, to relate doses to relative risks of osteosarcoma and acute myeloid leukaemia. Computer-based image analysis of neutron-induced and alpha-track autoradiographs of sections of mouse femora was used to quantify the microdistribution of (239)Pu, (241)Am and (233)U from 1 to 448 days after intraperitoneal injection. Localized dose-rates and cumulative doses over this period were calculated for different regions of the marrow spaces in trabecular bone. The results were then combined with previous data for doses to the cortical marrow of the femoral shaft. A morphometric analysis of the distal femur was carried out. Initial deposition on endosteal surfaces and dose-rates near to the trabecular surfaces at 1 day were two to four times greater than corresponding results for cortical bone. Burial was most rapid for (233)U, about twice the rate in cortical bone. As in cortical bone, subsequent uptake into the marrow was seen for (239)Pu and (241)Am but not (233)U. Cumulative doses to 448 days for different regions of trabecular marrow were greater than corresponding values for cortical marrow for each radionuclide. Combined doses reflected the greater overall volume of cortical marrow. Cumulative radiation doses to the 10 microm thick band of marrow adjacent to all endosteal surfaces were in the ratio of approximately 7:3:1 for (239)Pu:(241)Am:(233)U. This ratio is not inconsistent with observed incidences of osteosarcoma induction by the three nuclides. Analysis of doses to different depths of marrow, however, showed that although ratios were probably not significantly different to that for a 10 microm depth, better correlations with osteosarcomagenic risk were obtained with 20-40 microm depths. For acute myeloid leukaemia, the closest

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.

(236)U and (239,)(240)Pu ratios from soils around an Australian nuclear weapons test site.

PubMed

Tims, S G; Froehlich, M B; Fifield, L K; Wallner, A; De Cesare, M

2016-01-01

The isotopes (236)U, (239)Pu and (240)Pu are present in surface soils as a result of global fallout from nuclear weapons tests carried out in the 1950's and 1960's. These isotopes potentially constitute artificial tracers of recent soil erosion and sediment movement. Only Accelerator Mass Spectrometry has the requisite sensitivity to measure all three isotopes at these environmental levels. Coupled with its relatively high throughput capabilities, this makes it feasible to conduct studies of erosion across the geographical extent of the Australian continent. In the Australian context, however, global fallout is not the only source of these isotopes. As part of its weapons development program the United Kingdom carried out a series of atmospheric and surface nuclear weapons tests at Maralinga, South Australia in 1956 and 1957. The tests have made a significant contribution to the Pu isotopic abundances present in the region around Maralinga and out to distances ∼1000 km, and impact on the assessment techniques used in the soil and sediment tracer studies. Quantification of the relative fallout contribution derived from detonations at Maralinga is complicated owing to significant contamination around the test site from numerous nuclear weapons safety trials that were also carried out around the site. We show that (236)U can provide new information on the component of the fallout that is derived from the local nuclear weapons tests, and highlight the potential of (236)U as a new fallout tracer. Crown Copyright © 2015. Published by Elsevier Ltd. All rights reserved.

Fractionation of 238U/235U by reduction during low temperature uranium mineralisation processes

NASA Astrophysics Data System (ADS)

Murphy, Melissa J.; Stirling, Claudine H.; Kaltenbach, Angela; Turner, Simon P.; Schaefer, Bruce F.

2014-02-01

Investigations of ‘stable’ uranium isotope fractionation during low temperature, redox transformations may provide new insights into the usefulness of the 238U/235U isotope system as a tracer of palaeoredox processes. Sandstone-hosted uranium deposits accumulate at an oxidation/reduction interface within an aquifer from the low temperature reduction of soluble U(VI) complexes in groundwaters, forming insoluble U(IV) minerals. This setting provides an ideal environment in which to investigate the effects of redox transformations on 238U/235U fractionation. Here we present the first coupled measurements of 238U/235U isotopic compositions and U concentrations for groundwaters and mineralised sediment samples from the same redox system in the vicinity of the high-grade Pepegoona sandstone-hosted uranium deposit, Australia. The mineralised sediment samples display extremely variable 238U/235U ratios (herein expressed as δUCRM145238, the per-mil deviation from the international NBL standard CRM145). The majority of mineralised sediment samples have δUCRM145238 values between -1.30±0.05 and 0.55±0.12‰, spanning a ca. 2‰ range. However, one sample has an unusually light isotopic composition of -4.13±0.05‰, which suggests a total range of U isotopic variability of up to ca. 5‰, the largest variation found thus far in a single natural redox system. The 238U/235U isotopic signature of the mineralised sediments becomes progressively heavier (enriched in 238U) along the groundwater flow path. The groundwaters show a greater than 2‰ variation in their 238U/235U ratios, ranging from δUCRM145238 values of -2.39±0.07 to -0.71±0.05‰. The majority of the groundwater data exhibit a clear systematic relationship between 238U/235U isotopic composition and U concentration; samples with the lowest U concentrations have the lowest 238U/235U ratios. The preferential incorporation of 238U during reduction of U(VI) to U(IV) and precipitation of uranium minerals leaves

PLANTS AS BIO-MONITORS FOR 137CS, 238PU, 239, 240PU AND 40K AT THE SAVANNAH RIVER SITE

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

Caldwell, E.; Duff, M.; Ferguson, C.

2010-12-16

The nuclear fuel cycle generates a considerable amount of radioactive waste, which often includes nuclear fission products, such as strontium-90 ({sup 90}Sr) and cesium-137 ({sup 137}Cs), and actinides such as uranium (U) and plutonium (Pu). When released into the environment, large quantities of these radionuclides can present considerable problems to man and biota due to their radioactive nature and, in some cases as with the actinides, their chemical toxicity. Radionuclides are expected to decay at a known rate. Yet, research has shown the rate of elimination from an ecosystem to differ from the decay rate due to physical, chemical andmore » biological processes that remove the contaminant or reduce its biological availability. Knowledge regarding the rate by which a contaminant is eliminated from an ecosystem (ecological half-life) is important for evaluating the duration and potential severity of risk. To better understand a contaminants impact on an environment, consideration should be given to plants. As primary producers, they represent an important mode of contamination transfer from sediments and soils into the food chain. Contaminants that are chemically and/or physically sequestered in a media are less likely to be bio-available to plants and therefore an ecosystem.« less

Distribution of skeletal malignancies in beagles injected with 239Pu citrate.

PubMed

Lloyd, R D; Taylor, G N; Angus, W; Miller, S C; Bruenger, F W; Jee, W S

1994-04-01

The distribution of skeletal malignancies among our beagles injected with 239Pu as young adults roughly seems to follow the distribution of skeletal mass and skeletal 239Pu. These findings are similar to those we reported previously for a group of dogs given 26Ra. Although there were differences in tumor distribution between the animals given 226Ra and those given 239Pu, most of them were not statistically significant; however, the radium dogs seemed to show a greater sensitivity to bone tumor origin in the tibia, while there may have been a tendency among the plutonium dogs toward increased relative sensitivity in the scapula, lumbar vertebrae, sacrum, and ribs. In contrast, the most common site for the formation of naturally-occurring bone malignancy in the dog is the distal radius. Perhaps there were too few tumors and too few dogs to establish statistical significance. A correlation between tumor location and at least two anatomical-physiological factors in the skeleton indicated that these two factors (site-specific bone turnover rate and percent of red marrow at the site, which is correlated with vascularity) may influence the appearance of malignancies both individually and in combination. Except for the femur, there appeared to be no difference between the relative distribution of skeletal malignancies of low-level (30 Bq-2 Bq kg-1 injected) and high-level (3-122 kBq kg-1) dogs. Distribution of bone tumors between the axial and appendicular skeleton was 50% vs. 50% for 239Pu (42 and 42), but it was 39% axial vs. 61% appendicular (22 and 35, respectively) for dogs given 226Ra. This difference was not significant (p > 0.2).

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.

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

Evaluation of phases in Pu-C-O and (U, Pu)-C-O systems by X-ray diffractometry and chemical analysis

NASA Astrophysics Data System (ADS)

Jain, G. C.; Ganguly, C.

1993-12-01

Preparation and characterisation of the carbides of uranium, plutonium and mixed uranium and plutonium form a part of advanced fuel development programs for fast breeder reactors. In the present study, the compositions of the phases of Pu-C-O and (U.Pu)-C-O systems have been determined by chemical analysis and lattice parameter measurement. The carbide samples have been prepared by vacuum carbothermic synthesis of tabletted oxide-graphite powder mixture. Dependence of stoichiometry of Pu 2C 3 phase on the oxygen content of Pu(C,O) phase in Pu(C,O) + Pu 2C 3 phase mixture has been evaluated. Stoichiometry and oxygen solubility of (U 0.3Pu 0.7)(C,O) phase in multiple phase mixture have been determined. Segregation of plutonium in (U,Pu) 2C 3 phase of (U,Pu)(C,O) + (U,Pu) 2C 3 phase mixture and its dependence on the oxygen content of (U,Pu)(C,O) phase have also been determined from the measurement of the lattice parameter of (U,Pu) 2C 3 phase.

Estimates for Pu-239 loadings in burial ground culverts based on fast/slow neutron measurements

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

Winn, W.G.; Hochel, R.C.; Hofstetter, K.J.

1989-08-15

This report provides guideline estimates for Pu-239 mass loadings in selected burial ground culverts. The relatively high recorded Pu-239 contents of these culverts have been appraised as suspect relative to criticality concerns, because they were assayed only with the solid waste monitor (SWM) per gamma-ray counting. After 1985, subsequent waste was also assayed with the neutron coincidence counter (NCC), and a comparison of the assay methods showed that the NCC generally yielded higher assays than the SWM. These higher NCC readings signaled a need to conduct non-destructive/non-intrusive nuclear interrogations of these culverts, and a technical team conducted scoping measurements tomore » illustrate potential assay methods based on neutron and/or gamma counting. A fast/slow neutron method has been developed to estimate the Pu-239 in the culverts. In addition, loading records include the SWM assays of all Pu-239 cuts of some of the culvert drums and these data are useful in estimating the corresponding NCC drum assays from NCC vs SWM data. Together, these methods yield predictions based on direct measurements and statistical inference.« less

Production and investigation of thin films of metal actinides (Pu, Am, Cm, Bk, Cf)

NASA Astrophysics Data System (ADS)

Radchenko, V. M.; Ryabinin, M. A.; Stupin, V. A.

2010-03-01

Under limited availability of transplutonium metals some special techniques and methods of their production have been developed that combine the process of metal reduction from a chemical compound and preparation of a sample for examination. In this situation the evaporation and condensation of metal onto a substrate becomes the only possible technology. Thin film samples of metallic 244Cm, 248Cm and 249Bk were produced by thermal reduction of oxides with thorium followed by deposition of the metals in the form of thin layers on tantalum substrates. For the production of 249Cf metal in the form of a thin layer the method of thermal reduction of oxide with lanthanum was used. 238Pu and 239Pu samples in the form of films were prepared by direct high temperature evaporation and condensation of the metal onto a substrate. For the production of 241Am films a gram sample of plutonium-241 metal was used containing about 18 % of americium at the time of production. Thermal decomposition of Pt5Am intermetallics in vacuum was used to produce americium metal with about 80% yield. Resistivity of the metallic 249Cf film samples was found to decrease exponentially with increasing temperature. The 249Cf metal demonstrated a tendency to form preferably a DHCP structure with the sample mass increasing. An effect of high specific activity on the crystal structure of 238Pu nuclide thin layers was studied either.

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

NASA Astrophysics Data System (ADS)

Jégou, C.; Caraballo, R.; Peuget, S.; Roudil, D.; Desgranges, L.; Magnin, M.

2010-10-01

Structural changes in four (U 1-yPu y)O 2 materials with very different plutonium concentrations (0 ⩽ y ⩽ 1) and damage levels (up to 110 dpa) were studied by Raman spectroscopy. The novel experimental approach developed for this purpose consisted in using a laser beam as a heat source to assess the reactivity and structural changes of these materials according to the power supplied locally by the laser. The experiments were carried out in air and in water with or without hydrogen peroxide. As expected, the material response to oxidation in air depends on the plutonium content of the test oxide. At the highest power levels U 3O 8 generally forms with UO 2 whereas no significant change in the spectra indicating oxidation is observed for samples with high plutonium content ( 239PuO 2). Samples containing 25 wt.% plutonium exhibit intermediate behavior, typified mainly by a higher-intensity 632 cm -1 peak and the disappearance of the 1LO peak at 575 cm -1. This can be attributed to the presence of anion sublattice defects without any formation of higher oxides. The range of materials examined also allowed us to distinguish partly the chemical effects of alpha self-irradiation. The results obtained with water and hydrogen peroxide (a water radiolysis product) on a severely damaged 238PuO 2 specimen highlight a specific behavior, observed for the first time.

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.

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.

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

PubMed

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

1989-10-01

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

Spatial patterns and ratios of ¹³⁷Cs, ⁹⁰Sr, and Pu isotopes in the top layer of undisturbed meadow soils as indicators for contamination origin.

PubMed

Lukšienė, Benedikta; Puzas, Andrius; Remeikis, Vidmantas; Druteikienė, Rūta; Gudelis, Arūnas; Gvozdaitė, Rasa; Buivydas, Šarūnas; Davidonis, Rimantas; Kandrotas, Gintautas

2015-05-01

Spatial distribution of activity concentrations of (137)Cs, (90)Sr, and (239,240)Pu in the top layer of undisturbed meadow soils was compared between two regional transects across Lithuania: one in the SW region, more affected by the Chernobyl radioactive fallout, and the other in the NE region. Radiochemical, γ-, α-, β-, and mass spectrometric methods were used to determine the radionuclide activity. Our results validate that higher activity concentrations in the top soil layer were present in the SW region, despite the fact that sampling was performed after 22 years of the Chernobyl Nuclear Power Plant (NPP) accident. Using the activity concentration ratio (137)Cs/(239,240)Puglobal, the contribution of the Chernobyl NPP accident to the total radiocesium activity concentrations in these meadow soils was evaluated and found to be in the range of 6.5-59.1%. Meanwhile, the activity concentration ratio (238)Pu/(239,240)Pu showed that Chernobyl-derived Pu occurred at almost half of the sampling sites. The locations with maximal values of 47% of Chernobyl-derived Pu material were close to northeastern Poland, where deposition of most of non-volatile radioisotopes from the Chernobyl plume was determined.

Evidence of extinct 244Pu in ancient terrestrial zircons

NASA Astrophysics Data System (ADS)

Harrison, T. M.; Turner, G.; Holland, G.; Gilmour, J. D.; Mojzsis, S. J.

2003-04-01

The Pu/U ratio of the early Earth is an important parameter in models of mantle evolution based on noble gas isotopes. Current estimates assume the Earth accreted with a chondritic Pu/U and are based on analyses of the chondrite St Severin and the achondrite Angra dos Reis. These estimates are poorly constrained, ranging from 0.004 to 0.008. On account of its short, 82 Ma, half-life, 244Pu was essentially extinct 3,900 Ma ago, and consequently there exists no reliable measurement of Pu/U for the Earth. The discovery of zircons dating from the period when 244Pu was "live" offers the first opportunity to measure the former terrestrial abundance of 244Pu directly. Xenon isotopes are produced by spontaneous fission and, in principle, are readily distinguishable from those produced by 238U-fission (e.g. 131Xe/136Xe = 0.24 and 0.08 respectively). However the expected levels of fission xenon in individual zircons, weighing 1 - 2 μg and containing 100 - 200 ppm U, are below, or at best comparable to, the Xe blank levels (˜10-15 ccSTP) typical of conventional noble gas mass spectrometers. In order to analyse these minute amounts of xenon we have made use of a uniquely sensitive instrument, developed in Manchester, based on the principle of laser resonance ionisation. RELAX (Refrigerator Enhanced Laser Analyser for Xenon) is capable of analysing samples of only a few thousand atoms, some two orders of magnitude smaller than conventional mass spectrometers. We have carried out preliminary analyses of 4 individual 4,150 Ma zircons and one 3,600 Ma zircon from Jack Hills, Western Australia, and obtained five clear fission spectra. All but one were essentially free from significant atmospheric blank (the average 130Xe blank was 3× 10-18 ccSTP, i.e. 80 atoms). The spectra of the older zircons clearly demonstrated the presence of varying amounts of 244Pu fission xenon. The highest 131Xe/136Xe, 0.136 ± 0.003, corresponds to an initial Pu/U ratio of 0.0057. The lower ratios

40 CFR 86.238-94-86.239-94 - [Reserved

Code of Federal Regulations, 2010 CFR

2010-07-01

... PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES Emission Regulations for 1994 and Later Model Year Gasoline-Fueled New Light-Duty Vehicles, New Light-Duty Trucks and New Medium-Duty Passenger Vehicles; Cold Temperature Test Procedures §§ 86.238-94—86.239-94 [Reserved] ...

Characterization of U/Pu Particles Originating From the Nuclear Weapon Accidents at Palomares, Spain, 1966 And Thule, Greenland, 1968

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

Lind, O.C.; Salbu, B.; Janssens, K.

2007-07-10

Following the USAF B-52 bomber accidents at Palomares, Spain in 1966 and at Thule, Greenland in 1968, radioactive particles containing uranium (U) and plutonium (Pu) were dispersed into the environment. To improve long-term environmental impact assessments for the contaminated ecosystems, particles from the two sites have been isolated and characterized with respect to properties influencing particle weathering rates. Low [239]Pu/[235]U (0.62-0.78) and [240]Pu/[239]Pu (0.055-0.061) atom ratios in individual particles from both sites obtained by Inductively Coupled Plasma Mass Spectrometry (ICP-MS) show that the particles contain highly enriched U and weapon-grade Pu. Furthermore, results from electron microscopy with Energy Dispersive X-raymore » analysis (EDX) and synchrotron radiation (SR) based micrometer-scale X-ray fluorescence ({micro}-XRF) 2D mapping demonstrated that U and Pu coexist throughout the 1-50 {micro}m sized particles, while surface heterogeneities were observed in EDX line scans. SR-based micrometer-scale X-ray Absorption Near Edge Structure Spectroscopy ({micro}-XANES) showed that the particles consisted of an oxide mixture of U (predominately UO[2] with the presence ofU[3][8]) and Pu ((III)/(IV), (V)/(V) or (III), (IV) and (V)). Neither metallic U or Pu nor uranyl or Pu(VI) could be observed. Characteristics such as elemental distributions, morphology and oxidation states are remarkably similar for the Palomares and Thule particles, reflecting that they originate from similar source and release scenarios. Thus, these particle characteristics are more dependent on the original material from which the particles are derived (source) and the formation of particles (release scenario) than the environmental conditions to which the particles have been exposed since the late 1960s.« less

Results of The Excreta Bioassay Quality Control Program For April 1, 2010 Through March 31, 2011

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

Antonio, Cheryl L.

2012-07-19

A total of 76 urine samples and 10 spiked fecal samples were submitted during the report period (April 1, 2010 through March 31, 2011) to GEL Laboratories, LLC in South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for 14C, Sr, for 238Pu, 239Pu, 241Am, 243Am, 235U, 238U, 238U-mass and fecal analyses for 241Am, 238Pu and 239Pu were tested this year. The number of QC urine samples submitted during the report period represented 1.1% of the total samples submitted. In addition to the samples provided by IDP,more » GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 31% of the analyses processed by GEL during the first year of contract 112512 were quality control samples. GEL tested the performance of 23 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty except the slightly elevated relative bias for 243,244Cm (Table 4).« less

Measurement of the 242Pu neutron capture cross section

NASA Astrophysics Data System (ADS)

Buckner, M. Q.; Wu, C. Y.; Henderson, R. A.; Bucher, B.; Bredeweg, T. A.; Baramsai, B.; Couture, A.; Jandel, M.; Mosby, S.; O'Donnell, J. M.; Ullmann, J. L.; Chyzh, A.; Dance Collaboration

2015-10-01

Precision (n,f) and (n, γ) cross sections are important for the network calculations of the radiochemical diagnostic chain for the U.S. DOE's Stockpile Stewardship Program. 242Pu(n, γ) cross section is relevant to the network calculations of Pu and Am. Additionally, new reactor concepts have catalyzed considerable interest in the measurement of improved cross sections for neutron-induced reactions on key actinides. To date, little or no experimental data has been reported on 242Pu(n, γ) for incident neutron energy below 50 keV. A new measurement of the 242Pu(n, γ) reaction was performed with the DANCE together with an improved PPAC for fission-fragment detection at LANSCE during FY14. The relative scale of the 242Pu(n, γ) cross section spans four orders of magnitude for incident neutron energies from thermal to ~ 30 keV. The absolute scale of the 242Pu(n, γ) cross section is set according to the measured 239Pu(n,f) resonance at 7.8 eV; the target was spiked with 239Pu for this measurement. The absolute 242Pu(n, γ) neutron capture cross section is ~ 30% higher than the cross section reported in ENDF for the 2.7 eV resonance. Latest results to be reported. Funded by U.S. DOE Contract No. DE-AC52-07NA27344 (LLNL) and DE-AC52-06NA25396 (LANL). U.S. DOE/NNSA Office of Defense Nuclear Nonproliferation Research and Development. Isotopes (ORNL).

A new Mantle Source Tapped During Episode 55 of the Pu'u O'o Eruption From Kilauea Volcano

NASA Astrophysics Data System (ADS)

Marske, J. P.; Pietruszka, A. J.; Garcia, M. O.; Rhodes, J. M.

2005-12-01

Over 22 years of continuous geochemical monitoring of lavas from the current Pu'u O'o eruption allows us to probe the mantle and crustal processes beneath Kilauea Volcano in unparalleled detail. Episode 55 (1997-present) marks the longest and most voluminous Pu'u O'o eruptive interval. Here we present new Pb, Sr, and Nd isotopic ratios and major- and trace-element abundances for the most recent lavas (1999-2005). MgO variation diagrams show that most of the major-element variations are related to olivine fractionation. However, Pu'u O'o lavas display longer-term systematic decreases in their TiO2, K2O, P2O5 and CaO abundances (at a given MgO) due to changes in the parental magma composition. Incompatible element ratios (K2O/TiO2, Nb/Y, Nb/Zr) and MgO-normalized abundances (Sr, Rb, K) in episode 55 lavas delimit the lowest values observed during the Pu'u O'o eruption. Earlier Pu'u O'o lavas displayed a temporal decrease in highly over moderately incompatible trace-element ratios, near constant SiO2 contents, and a gradual increase in 87Sr/86Sr. However, episode 55 lavas (between days 5500-6500) record an increase in MgO-normalized SiO2 contents and even higher 87Sr/86Sr with near constant incompatible trace-element ratios. Neither a single mantle source composition nor a change in partial melting conditions can explain these observations. Based on 226Ra-230Th-238U disequilibria and partial melting modeling of trace elements, we conclude that Pu'u O'o lavas originate from at least two distinct mantle source components: (1) a recently depleted component that was subsequently remelted to explain the overall decreases of incompatible major- and trace-element ratios and abundances, and (2) a compositionally and isotopically distinct mantle component that was not previously melted within the Hawaiian plume to explain the temporal increase in 87Sr/86Sr and SiO2 abundances and the flattening trend of incompatible trace-element ratios. This second component lies within

Distinguishing Fissile From Non-Fissile Materials Using Linearly Polarized Gamma Rays

NASA Astrophysics Data System (ADS)

Mueller, J. M.; Ahmed, M. W.; Karwowski, H. J.; Myers, L. S.; Sikora, M. H.; Weller, H. R.; Zimmerman, W. R.; Randrup, J.; Vogt, R.

2014-03-01

Photofission of 232Th, 233 , 235 , 238U, 237Np, and 239,240Pu was induced by nearly 100% linearly polarized, high intensity (~107 γs per second), and nearly-monoenergetic γ-ray beams of energies between 5.3 and 7.6 MeV at the High Intensity γ-ray Source (HI γS). An array of 12-18 liquid scintillating detectors was used to measure prompt fission neutron yields. The ratio of prompt fission neutron yields parallel to the plane of beam polarization to the yields perpendicular to this plane was measured as a function of beam and neutron energy. A ratio near unity was found for 233,235U, 237Np, and 239Pu while a significant ratio (~1.5-3) was found for 232Th, 238U, and 240Pu. This large difference could be used to distinguish fissile isotopes (such as 233,235U and 239Pu) from non-fissile isotopes (such as 232Th, 238U, and 240Pu). The measured ratios agree with the results of a fission calculation (FREYA) which used with previously measured photofission fragment angular distributions as input. Partially supported by DHS (2010-DN-077-ARI046-02), DOE (DE-AC52-07NA27344 and DE-AC02-05CH11231), and the DOE Office of Science Graduate Fellowship Program (DOE SCGF).

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.

Use of anthropogenic radioisotopes to estimate rates of soil redistribution by wind II: The potential for future use of 239+240Pu

NASA Astrophysics Data System (ADS)

Van Pelt, R. Scott; Ketterer, Michael E.

2013-06-01

In the previous paper, the use of soilborne 137Cs from atmospheric fallout to estimate rates of soil redistribution, particularly by wind, was reviewed. This method relies on the assumption that the source of 137Cs in the soil profile is from atmospheric fallout following the period of atmospheric weapons testing so that the temporal and, to a certain extent, the spatial patterns of 137Cs deposition are known. One of the major limitations occurs when local or regional sources of 137Cs contamination mask the pulse from global fallout, making temporal estimates of redistribution difficult or impossible. Like 137Cs, Pu exhibits strong affinity for binding to soil particle surfaces, and therefore, re-distribution of Pu inventory indicates inferred soil re-distribution. Compared to 137Cs, 239Pu and 240Pu offer several important advantages: (a) the two major Pu isotopes have much longer half-lives than 137Cs and (b) the ratio 240Pu/239Pu is used to examine whether the Pu is from stratospheric fallout. In this paper, we review the literature concerning Pu in soil and of current attempts to use this tracer to estimate rates of soil redistribution. We also present preliminary, unpublished data from a pilot study designed to test whether or not 239+240Pu can be used to estimate rates of soil redistribution by wind. Based on similarities of profile distribution and relative inventories between 137Cs measurements and 239+240Pu measurements of split samples from a series of fields with documented wind erosion histories, we conclude that 239+240Pu may well be the anthropogenic radioisotope of choice for future soil redistribution investigations.

A generalized method for characterization of 235U and 239Pu content using short-lived fission product gamma spectroscopy

DOE PAGES

Knowles, Justin R.; Skutnik, Steven E.; Glasgow, David C.; ...

2016-06-23

Rapid non-destructive assay methods for trace fissile material analysis are needed in both nuclear forensics and safeguards communities. To address these needs, research at the High Flux Isotope Reactor Neutron Activation Analysis laboratory has developed a generalized non-destructive assay method to characterize materials containing fissile isotopes. This method relies on gamma-ray emissions from short-lived fission products and capitalizes off of differences in fission product yields to identify fissile compositions of trace material samples. Although prior work has explored the use of short-lived fission product gamma-ray measurements, the proposed method is the first to provide a holistic characterization of isotopic identification,more » mass ratios, and absolute mass determination. Successful single fissile isotope mass recoveries of less than 6% error have been conducted on standards of 235U and 239Pu as low as 12 nanograms in less than 10 minutes. Additionally, mixtures of fissile isotope standards containing 235U and 239Pu have been characterized as low as 229 nanograms of fissile mass with less than 12% error. The generalizability of this method is illustrated by evaluating different fissile isotopes, mixtures of fissile isotopes, and two different irradiation positions in the reactor. Furthermore, it is anticipated that this method will be expanded to characterize additional fissile nuclides, utilize various irradiation sources, and account for increasingly complex sample matrices.« less

A generalized method for characterization of 235U and 239Pu content using short-lived fission product gamma spectroscopy

NASA Astrophysics Data System (ADS)

Knowles, Justin; Skutnik, Steven; Glasgow, David; Kapsimalis, Roger

2016-10-01

Rapid nondestructive assay methods for trace fissile material analysis are needed in both nuclear forensics and safeguards communities. To address these needs, research at the Oak Ridge National Laboratory High Flux Isotope Reactor Neutron Activation Analysis facility has developed a generalized nondestructive assay method to characterize materials containing fissile isotopes. This method relies on gamma-ray emissions from short-lived fission products and makes use of differences in fission product yields to identify fissile compositions of trace material samples. Although prior work has explored the use of short-lived fission product gamma-ray measurements, the proposed method is the first to provide a complete characterization of isotopic identification, mass ratios, and absolute mass determination. Successful single fissile isotope mass recoveries of less than 6% recovery bias have been conducted on standards of 235U and 239Pu as low as 12 ng in less than 10 minutes. Additionally, mixtures of fissile isotope standards containing 235U and 239Pu have been characterized as low as 198 ng of fissile mass with less than 7% recovery bias. The generalizability of this method is illustrated by evaluating different fissile isotopes, mixtures of fissile isotopes, and two different irradiation positions in the reactor. It is anticipated that this method will be expanded to characterize additional fissile nuclides, utilize various irradiation facilities, and account for increasingly complex sample matrices.

A generalized method for characterization of 235U and 239Pu content using short-lived fission product gamma spectroscopy

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

Knowles, Justin R.; Skutnik, Steven E.; Glasgow, David C.

Rapid non-destructive assay methods for trace fissile material analysis are needed in both nuclear forensics and safeguards communities. To address these needs, research at the High Flux Isotope Reactor Neutron Activation Analysis laboratory has developed a generalized non-destructive assay method to characterize materials containing fissile isotopes. This method relies on gamma-ray emissions from short-lived fission products and capitalizes off of differences in fission product yields to identify fissile compositions of trace material samples. Although prior work has explored the use of short-lived fission product gamma-ray measurements, the proposed method is the first to provide a holistic characterization of isotopic identification,more » mass ratios, and absolute mass determination. Successful single fissile isotope mass recoveries of less than 6% error have been conducted on standards of 235U and 239Pu as low as 12 nanograms in less than 10 minutes. Additionally, mixtures of fissile isotope standards containing 235U and 239Pu have been characterized as low as 229 nanograms of fissile mass with less than 12% error. The generalizability of this method is illustrated by evaluating different fissile isotopes, mixtures of fissile isotopes, and two different irradiation positions in the reactor. Furthermore, it is anticipated that this method will be expanded to characterize additional fissile nuclides, utilize various irradiation sources, and account for increasingly complex sample matrices.« less

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.

Unifying measurement of 239Pu(n ,γ ) in the keV to MeV energy regime

NASA Astrophysics Data System (ADS)

Mosby, S.; Bredeweg, T. A.; Couture, A.; Jandel, M.; Kawano, T.; Ullmann, J. L.; Henderson, R. A.; Wu, C. Y.

2018-04-01

A single, unifying measurement of the 239Pu capture cross section from 1 keV to 1.3 MeV has been performed for the first time using the Detector for Advanced Neutron Capture Experiments (DANCE) at the Los Alamos Neutron Science Center (LANSCE). The experimental method combines a prior experiment's characterization of prompt fission γ rays in conjunction with a fission tagging detector with a separate experiment using a thick 239Pu sample to extract the neutron capture cross section in ratio to 239Pu(n ,f ) . We have made new predictions of the capture cross section taking into account recent results for the M 1 scissors mode present in other actinides. The results show deviations from current evaluations which are 30% higher at the highest energies, and will be used to improve calculations relevant for several applications.

Heterogeneity in the 238U/235U Ratios of Angrites.

NASA Astrophysics Data System (ADS)

Tissot, F.; Dauphas, N.; Grove, T. L.

2016-12-01

Angrites are differentiated meteorites of basaltic composition, of either volcanic or plutonic origin, that display minimal post-crystallization alteration, metamorphism, shock or impact brecciation. Because quenched angrites cooled very rapidly, all radiochronometric systems closed simultaneously in these samples. Quenched angrites are thus often used as anchors for cross-calibrating short-lived dating methods (e.g., 26Al-26Mg) and the absolute dating techniques (e.g, Pb-Pb). Due to the constancy of the 238U/235U ratio in natural samples, Pb-Pb ages have long been calculated using a "consensus" 238U/235U ratio, but the discovery of resolvable variations in the 238U/235U ratio of natural samples, means that the U isotopic composition of the material to date also has to be determined in order to obtain high-precision Pb-Pb ages. We set out (a) to measure at high-precision the 238U/235U ratio of a large array of angrites to correct their Pb-Pb ages, and (b) to identify whether all angrites have a similar U isotopic composition, and, if not, what were the processes responsible for this variability. Recently, Brennecka & Wadhwa (2012) suggested that the angrite-parent body had a homogeneous 238U/235U ratio. They reached this conclusion partly because they propagated the uncertainties of the U isotopic composition of the various U double spikes that they used onto the final 238U/235U ratio the sample. Because this error is systematic (i.e., it affects all samples similarly), differences in the δ238U values of samples corrected by the same double spike are better known than one would be led to believe if uncertainties on the spike composition are propagated. At the conference, we will present the results of the high-precision U isotope analyses for six angrite samples: NWA 4590, NWA 4801, NWA 6291, Angra dos Reis, D'Orbigny, and Sahara 99555. We will show that there is some heterogeneity in the δ238U values of the angrites and will discuss the possible processes by

Extended optical model for fission

DOE PAGES

Sin, M.; Capote, R.; Herman, M. W.; ...

2016-03-07

A comprehensive formalism to calculate fission cross sections based on the extension of the optical model for fission is presented. It can be used for description of nuclear reactions on actinides featuring multi-humped fission barriers with partial absorption in the wells and direct transmission through discrete and continuum fission channels. The formalism describes the gross fluctuations observed in the fission probability due to vibrational resonances, and can be easily implemented in existing statistical reaction model codes. The extended optical model for fission is applied for neutron induced fission cross-section calculations on 234,235,238U and 239Pu targets. A triple-humped fission barrier ismore » used for 234,235U(n,f), while a double-humped fission barrier is used for 238U(n,f) and 239Pu(n,f) reactions as predicted by theoretical barrier calculations. The impact of partial damping of class-II/III states, and of direct transmission through discrete and continuum fission channels, is shown to be critical for a proper description of the measured fission cross sections for 234,235,238U(n,f) reactions. The 239Pu(n,f) reaction can be calculated in the complete damping approximation. Calculated cross sections for 235,238U(n,f) and 239Pu(n,f) reactions agree within 3% with the corresponding cross sections derived within the Neutron Standards least-squares fit of available experimental data. Lastly, the extended optical model for fission can be used for both theoretical fission studies and nuclear data evaluation.« less

Study of 236U/238U ratio at CIRCE using a 16-strip silicon detector with a TOF system

NASA Astrophysics Data System (ADS)

De Cesare, M.; De Cesare, N.; D'Onofrio, A.; Gialanella, L.; Terrasi, F.

2015-04-01

Accelerator Mass Spectrometry (AMS) is presently the most sensitive technique for the measurement of long-lived actinides, e.g. 236U and xPu isotopes. A new actinide AMS system, based on a 3-MV pelletron tandem accelerator, is operated at the Center for Isotopic Research on Cultural and Environmental Heritage (CIRCE) in Caserta, Italy. In this paper we report on the procedure adopted to increase the 236U abundance sensitivity as low as possible. The energy and position determinations of the 236U ions, using a 16-strip silicon detector have been obtained. A 236U/238U isotopic ratio background level of about 2.9×10-11 was obtained, summing over all the strips, using a Time of Flight-Energy (TOF-E) system with a 16-strip silicon detector (4.9×10-12 just with one strip).

Transport of 137Cs and 239,240Pu with ice-rafted debris in the Arctic Ocean

USGS Publications Warehouse

Landa, E.R.; Reimnitz, E.; Beals, D.M.; Pochkowski, J.M.; Winn, W.G.; Rigor, I.

1998-01-01

Ice rafting is the dominant mechanism responsible for the transport of fine-grained sediments from coastal zones to the deep Arctic Basin. Therefore, the drift of ice-rafted debris (IRD) could be a significant transport mechanism from the shelf to the deep basin for radionuclides originating from nuclear fuel cycle activities and released to coastal Arctic regions of the former Soviet Union. In this study, 28 samples of IRD collected from the Arctic ice pack during expeditions in 1989-95 were analyzed for 137Cs by gamma spectrometry and for 239Pu and 240Pu by thermal ionization mass spectrometry. 137Cs concentrations in the IRD ranged from less than 0.2 to 78 Bq??kg-1 (dry weight basis). The two samples with the highest 137Cs concentrations were collected in the vicinity of Franz Josef Land, and their backward trajectories suggest origins in the Kara Sea. Among the lowest 137Cs values are seven measured on sediments entrained on the North American shelf in 1989 and 1995, and sampled on the shelf less than six months later. Concentrations of 239Pu + 240Pu ranged from about 0.02 to 1.8 Bq??kg-1. The two highest values came from samples collected in the central Canada Basin and near Spitsbergen; calculated backward trajectories suggest at least 14 years of circulation in the Canada Basin in the former case, and an origin near Severnaya Zemlya (at the Kara Sea/Laptev Sea boundary) in the latter case. While most of the IRD samples showed 240Pu/239Pu ratios near the mean global fallout value of 0.185, five of the samples had lower ratios, in the 0.119 to 0.166 range, indicative of mixtures of Pu from fallout and from the reprocessing of weapons-grade Pu. The backward trajectories of these five samples suggest origins in the Kara Sea or near Severnaya Zemlya.

Unifying measurement of Pu 239 ( n , γ ) in the keV to MeV energy regime

DOE PAGES

Mosby, S.; Bredeweg, T. A.; Couture, A.; ...

2018-04-23

A single, unifying measurement of the 239Pu capture cross section from 1 keV to 1.3 MeV has been performed for the first time using the Detector for Advanced Neutron Capture Experiments (DANCE) at the Los Alamos Neutron Science Center (LANSCE). The experimental method combines a prior experiment's characterization of prompt fission γ rays in conjunction with a fission tagging detector with a separate experiment using a thick 239Pu sample to extract the neutron capture cross section in ratio to 239Pu (n, f). We have made new predictions of the capture cross section taking into account recent results for the M1more » scissors mode present in other actinides. The results show deviations from current evaluations which are 30% higher at the highest energies, and will be used to improve calculations relevant for several applications.« less

Nondestructive assay of EBR-II blanket elements using resonance transmission analysis

NASA Astrophysics Data System (ADS)

Klann, Raymond Todd

1998-10-01

Resonance transmission analysis utilizing a filtered reactor beam was examined as a means of determining the 239Pu content in Experimental Breeder Reactor - II depleted uranium blanket elements. The technique uses cadmium and gadolinium filters along with a 239Pu fission chamber to isolate the 0.3 eV resonance in 239Pu. In the energy range of this resonance (0.1 eV to 0.5 eV), the total microscopic cross-section of 239Pu is significantly greater than the cross- sections of 238U and 235U. This large difference allows small changes in the 239Pu content of a sample to result in large changes in the mass signal response. Tests with small stacks of depleted uranium and 239Pu foils indicate a significant change in response based on the 239Pu content of the foil stack. In addition, the tests indicate good agreement between the measured and predicted values of 239Pu up to approximately two weight percent.

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.

CORRELATIONS OF EFFECTIVE TEMPERATURES FOR NEUTRON SPECTRA EMITTED IN U$sup 235$ AND Pu$sup 239$ FISSION BY FAST AND SLOW NEUTRONS (in Russian)

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

Smirenkin, G.M.

1959-12-01

The method of threshold indicators was used for determining the magnitude of dT/sub ef//dE/sub n/. The fission neutrons were produced by fast and slow neutron bombardment. tron bombardment was accomplished in a paraffin block. Hollow metallic U/sup 235/ (90% enriched) and Pu/sup 239/ specimens with 50 mm outside diameters and 10 mm thick contained the threshold activator Ag/sup 107/(n,2n)Ag/sup 106m/. Measurements were made of the neutron flux above the threshold (9.5 Mev) of the Ag/sup 107/(n,2n)Ag/sup 106m/ reaction and the number of fission in the sphere (N/sub gamma /). The final data showed that for U/sup 235/ dT/sub ef//dE/sub n/more » = 0.008 plus or minus 0.004 and for Pu/sup 239/ dT/ sub ef/ /dE/sub n/ = tron fission distributions explain part of the error of the measurement. (R.V.J.)« less

Radionuclide concentrations in benthic invertebrates from Amchitka and Kiska Islands in the Aleutian Chain, Alaska.

PubMed

Burger, Joanna; Gochfeld, Michael; Jewett, Stephen C

2007-05-01

Concentrations of 13 radionuclides (137Cs, 129I, 60Co, 152Eu, 90Sr, 99Tc, 241Am, 238Pu, 239,249Pu, 234U, 235U, 236U, 238U) were examined in seven species of invertebrates from Amchitka and Kiska Islands, in the Aleutian Chain of Alaska, using gamma spectroscopy, inductively coupled plasma mass spectroscopy, and alpha spectroscopy. Amchitka Island was the site of three underground nuclear test (1965-1971), and we tested the null hypotheses that there were no differences in radionuclide concentrations between Amchitka and the reference site (Kiska) and there were no differences among species. The only radionuclides where composite samples were above the Minimum Detectable Activity (MDA) were 137Cs, 241Am, 239,249Pu, 234U, 235U, 236U, and 238U. Green sea urchin (Strongylocentrotus polyacanthus), giant chiton (Cryptochiton stelleri), plate limpets (Tectura scutum) and giant Pacific octopus (Enteroctopus dofleini) were only tested for 137Cs; octopus was the only species with detectable levels of 137Cs (0.262 +/- 0.029 Bq/kg, wet weight). Only rock jingle (Pododesmus macroschisma), blue mussel (Mytilus trossulus) and horse mussel (Modiolus modiolus) were analyzed for the actinides. There were no interspecific differences in 241Am and 239,240Pu, and almost no samples above the MDA for 238Pu and 236U. Horse mussels had significantly higher concentrations of 234U (0.844 +/- 0.804 Bq/kg) and 238U (0.730 +/- 0.646) than the other species (both isotopes are naturally occurring). There were no differences in actinide concentrations between Amchitka and Kiska. In general, radionuclides in invertebrates from Amchitka were similar to those from uncontaminated sites in the Northern Hemisphere, and below those from the contaminated Irish Sea. There is a clear research need for authors to report the concentrations of radionuclides by species, rather than simply as 'shellfish', for comparative purposes in determining geographical patterns, understanding possible effects, and for

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

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

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.

Sm-Nd-Pu timepieces in the Angra dos Reis meteorite

NASA Technical Reports Server (NTRS)

Lugmair, G. W.; Marti, K.

1977-01-01

Isotope ratios and age estimations are presented for the ultramafic pyroxenite Angra dos Reis meteorite. A pyroxene-phosphate internal isochron age of 4.55 plus or minus 0.04 eons was obtained, in agreement with reported Pb-Pb ages. It is suggested that Sm-146 decay led to an increase in the ratio of Nd-142 to Nd-144 in pyroxene, which is greater than the ratio of the Nd isotopes in phosphates. The effect of Pu-244 on the fission xenon components in pyroxene and phosphate is examined. The ratios of Pu-244 to Nd, U-238, and Th-232 are compared for pyroxene and phosphate separates. The exposure age of the meteorite, as obtained by the Kr-81 to Kr-83 method, was found to be 55.5 plus or minus 1.2 million years.

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

PubMed

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

1989-01-01

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

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

Vaporization chemistry of hypo-stoichiometric (U,Pu)O 2

NASA Astrophysics Data System (ADS)

Viswanathan, R.; Krishnaiah, M. V.

2001-04-01

Calculations were performed on hypo-stoichiometric uranium plutonium di-oxide to examine its vaporization behavior as a function of O/ M ( M= U+ Pu) ratio and plutonium content. The phase U (1- y) Pu yO z was treated as an ideal solid solution of (1- y)UO 2+ yPuO (2- x) such that x=(2- z)/ y. Oxygen potentials for different desired values of y, z, and temperature were used as the primary input to calculate the corresponding partial pressures of various O-, U-, and Pu-bearing gaseous species. Relevant thermodynamic data for the solid phases UO 2 and PuO (2- x) , and the gaseous species were taken from the literature. Total vapor pressure varies with O/M and goes through a minimum. This minimum does not indicate a congruently vaporizing composition. Vaporization behavior of this system can at best be quasi-congruent. Two quasi-congruently vaporizing compositions (QCVCs) exist, representing the equalities (O/M) vapor=(O/M) mixed-oxide and (U/Pu) vapor=(U/Pu) mixed-oxide, respectively. The (O/M) corresponding to QCVC1 is lower than that corresponding to QCVC2, but very close to the value where vapor pressure minimum occurs. The O/M values of both QCVCs increase with decrease in plutonium content. The vaporization chemistry of this system, on continuous vaporization under dynamic condition, is discussed.

Circulatory kinetics of intravenously injected {sup 238}Pu(IV) citrate and {sup 14}C-CaNa{sub 3}-DTPA in mice: Comparison with rat, dog, and Reference Man

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

Durbin, P.W.; Kullgren, B.; Schmidt, C.T.

1997-02-01

New ligands for in vivo chelation of Pu(IV) are being synthesized and evaluated in mice for efficacy and toxicity. Biokinetic studies of the new ligands, CaNa{sub 3}-DTPA, and Pu(IV) are major components of those investigations. Young adult female mice were injected intravenously (iv) with {sup 3}H-inulin, {sup 14}C-CaNa{sub 3}-DTPA, or {sup 238}Pu(IV) citrate to provide base- line data for plasma clearance, tissue uptake, and excretion rates and to determine the dilution volume (VOD) and renal clearance rate (RC) of filterable substances. Published plasma clearance data in Reference Man, dog, and rat were collected. Based on combined data for {sup 3}H-inulinmore » and {sup 14}C-CaNa{sub 3}-DTPA, VOD = 17% of body weight and RC = 18 mL kg{sup -1} min{sup -1} for mice. Retention of {sup 14}C-CaNa{sub 3}-DTPA in the four species is proportional to body weight and inversely proportional to RC: Integrals of the retention of {sup 14}C-CaNa{sub 3}-DTPA from R(t) = 1.0 to R(t) = 0.05 are 108, 43, 28, and 10 DF min, respectively, for Reference Man, dog, rat, and mouse. Clearances of iv-injected Pu(IV) citrate from plasma are in the same order: The plasma curve integrals from injection to 1440 min are 840, 640, 280, and 67 DF min, respectively, for Reference Man, dog, rat, and mouse. In mice, a large fraction of newly injected Pu(IV) is rapidly transferred to the interstitial water of bulk soft tissue (excluding liver and kidneys), from which it is cleared at the same rate as from the plasma. Rapid plasma clearance, escape into interstitial water (22%ID at 20 min), significant early urinary excretion (8%ID in 12 h), and prompt deposition in liver and skeleton (complete in 12 h) are evidence of inefficient binding to plasma protein of newly injected Pu(IV) in mice. Slow plasma clearance, little early urinary excretion, and delayed deposition in liver and skeleton reflect more efficient binding of newly injected Pu(IV) in Reference Man and dog. 39 refs., 6 figs., 3 tabs.« less

Reexamining the role of the ( n , γ f ) process in the low-energy fission of U 235 and Pu 239

DOE PAGES

Lynn, J. E.; Talou, P.; Bouland, O.

2018-06-01

In this paper, themore » $$(n,{\\gamma}f)$$ process is reviewed in light of modern nuclear reaction calculations in both slow and fast neutron-induced fission reactions on $$^{235}\\mathrm{U}$$ and $$^{239}\\mathrm{Pu}$$. Observed fluctuations of the average prompt fission neutron multiplicity and average total $${\\gamma}$$-ray energy below 100-eV incident neutron energy are interpreted in this framework. The surprisingly large contribution of the $M1$ transitions to the prefission $${\\gamma}$$-ray spectrum of $$^{239}\\mathrm{Pu}$$ is explained by the dominant fission probabilities of $${0}^{+}$$ and $${2}^{+}$$ transition states, which can only be accessed from compound nucleus states formed by the interaction of $s$-wave neutrons with the target nucleus in its ground state, and decaying through $M1$ transitions. The impact of an additional low-lying $M1$ scissors mode in the photon strength function is analyzed. We review experimental evidence for fission fragment mass and kinetic-energy fluctuations in the resonance region and their importance in the interpretation of experimental data on prompt neutron data in this region. In conclusion, calculations are extended to the fast energy range where $$(n,{\\gamma}f)$$ corrections can account for up to 3% of the total fission cross section and about 20% of the capture cross section.« less

Reexamining the role of the (n ,γ f ) process in the low-energy fission of 235U and 239Pu

NASA Astrophysics Data System (ADS)

Lynn, J. E.; Talou, P.; Bouland, O.

2018-06-01

The (n ,γ f ) process is reviewed in light of modern nuclear reaction calculations in both slow and fast neutron-induced fission reactions on 235U and 239Pu. Observed fluctuations of the average prompt fission neutron multiplicity and average total γ -ray energy below 100-eV incident neutron energy are interpreted in this framework. The surprisingly large contribution of the M 1 transitions to the prefission γ -ray spectrum of 239Pu is explained by the dominant fission probabilities of 0+ and 2+ transition states, which can only be accessed from compound nucleus states formed by the interaction of s -wave neutrons with the target nucleus in its ground state, and decaying through M 1 transitions. The impact of an additional low-lying M 1 scissors mode in the photon strength function is analyzed. We review experimental evidence for fission fragment mass and kinetic-energy fluctuations in the resonance region and their importance in the interpretation of experimental data on prompt neutron data in this region. Finally, calculations are extended to the fast energy range where (n ,γ f ) corrections can account for up to 3% of the total fission cross section and about 20% of the capture cross section.

Reexamining the role of the ( n , γ f ) process in the low-energy fission of U 235 and Pu 239

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

Lynn, J. E.; Talou, P.; Bouland, O.

In this paper, themore » $$(n,{\\gamma}f)$$ process is reviewed in light of modern nuclear reaction calculations in both slow and fast neutron-induced fission reactions on $$^{235}\\mathrm{U}$$ and $$^{239}\\mathrm{Pu}$$. Observed fluctuations of the average prompt fission neutron multiplicity and average total $${\\gamma}$$-ray energy below 100-eV incident neutron energy are interpreted in this framework. The surprisingly large contribution of the $M1$ transitions to the prefission $${\\gamma}$$-ray spectrum of $$^{239}\\mathrm{Pu}$$ is explained by the dominant fission probabilities of $${0}^{+}$$ and $${2}^{+}$$ transition states, which can only be accessed from compound nucleus states formed by the interaction of $s$-wave neutrons with the target nucleus in its ground state, and decaying through $M1$ transitions. The impact of an additional low-lying $M1$ scissors mode in the photon strength function is analyzed. We review experimental evidence for fission fragment mass and kinetic-energy fluctuations in the resonance region and their importance in the interpretation of experimental data on prompt neutron data in this region. In conclusion, calculations are extended to the fast energy range where $$(n,{\\gamma}f)$$ corrections can account for up to 3% of the total fission cross section and about 20% of the capture cross section.« less

Sintering of compacts of UN, (U,Pu)N, and PuN

DOEpatents

Tennery, V.J.; Godfrey, T.G.; Bomar, E.S.

1973-10-16

>A method is provided for preparing a densified compact of a metal nitride selected from the group consisting of UN, (U,Pu)N, and PuN which comprises heating a green compact of at least one selected nitride in the mononitride single-phase region, as displayed by a phase diagram of the mononitride of said compact, in a nitrogen atmosphere at a pressure of nitrogen less than 760 torr. At a given temperature, this process produces a singlephase structure and a maximal sintered density as measured by mercury displacement. (Official Gazette)

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.

Natural and man-made radioactivity in soils and plants around the research reactor of Inshass.

PubMed

Higgy, R H; Pimpl, M

1998-12-01

The specific radioactivities of the U-series, 232Th, 137Cs and 40K were measured in soil samples around the Inshass reactor in Cairo, using a gamma-ray spectrometer with a HpGe detector. The alpha activity of 238U, 234U and 235U was measured in the same soil samples by surface barrier detectors after radiochemical separation and the obtained results were compared with the specific activities determined by gamma-measurements. The alpha-activity of 238Pu, 239+240Pu, 241Am, 242Cm and 244Cm was measured after radiochemical separation by surface barrier detectors for both soil and plant samples. Then beta-activity of 241Pu was measured using liquid scintillation spectrometry.

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

Nuclear resonance fluorescence in U-238 using LaBr detectors for nuclear security

NASA Astrophysics Data System (ADS)

Hayakawa, Takehito; Negm, Hani; Ohgaki, Hideaki; Daito, Izuru; Kii, Toshiteru; Zen, Heishun; Omer, Mohamed; Shizuma, Toshiyuki; Hajima, Ryoichi

2014-09-01

Recently, a nondestructive measurement method of shielded fissional isotopes such as 235U or 239Pu has been proposed for the nuclear security. These isotopes are measured by using nuclear resonance fluorescence (NRF) with monochromatic energy gamma-ray beams generated by laser Compton-scattering (LCS). We have proposed that one measure scattered gamma-rays from NRF with LCS gamma-ray beams using the LaBr3(Ce) detectors. The LaBr3(Ce) crystals include internal radioisotopes of a meta-stable isotope 138La and alpha decay chains from some actinides as 227Ac. There is a broad pump at about 2 MeV. This pump is considered to be an overlap of alpha-rays from decay chains of some actinides but its detailed structure has not been established. Here we have measured NRF spectra of 238U using the LCS gamma-rays with energy of about 2.5 MeV at the HIgS facility of the Duke University. The background has been evaluated using a simulation code GEAT4. The 9 peaks, 8 NRF gamma-rays plus the Compton scattered gamma-ray of the incident beam, are finally assigned in an energy range of about 200 keV at about 2.5 MeV. The 8 integrated NRF cross-sections measured by LaBr3(Ce) have been consistent with results by an HPGe detector. The three levels are newly assigned using the HPGe detector. Two of them are also measured by LaBr3(Ce).

Electrowinning of U-Pu onto inert solid cathode in LiCl-KCl eutectic melts containing UCl3 and PuCl3

NASA Astrophysics Data System (ADS)

Sakamura, Yoshiharu; Murakami, Tsuyoshi; Tada, Kohei; Kitawaki, Shinichi

2018-04-01

Electrowinning process was investigated for extracting actinides from molten salts used for the pyrochemical reprocessing of spent nuclear fuels. The separation of actinides from lanthanides is expected to be enhanced by employing inert solid cathodes due to larger potential differences on these cathodes. In this study, the co-deposition behavior of Pu and U metals onto an inert solid cathode made of tungsten was examined in LiCl-KCl eutectic melts containing UCl3 and PuCl3 at 773 K. The standard potential of U3+/U is 0.31 V more positive than that of Pu3+/Pu. The U3+ concentration was varied in the range of 0.11-0.66 wt%, while the Pu3+ concentration was maintained at approximately 2.9 wt%. When the U3+ concentration was not sufficiently low, the deposited U metal readily grew outward from the electrode surface and the electrode surface area rapidly increased, which facilitated only the deposition of U metal. It was estimated that metallic Pu can be efficiently collected along with U at U3+ concentrations lower than ∼0.2 wt%.

Sediment budget for Murder Creek, Georgia, USA, from Pu239+240 - determined soil erosion rates

NASA Astrophysics Data System (ADS)

Stubblefield, A. P.; Matissoff, G.; Ketterer, M. E.; Whiting, P. J.

2005-12-01

Soil inventories of the radionuclides Cs137 and Pb210 have been used in a variety of environments as indicators for erosion and depositional processes. Development of sediment budgets for entire watersheds from radionuclide data has been somewhat constrained because limited sample numbers may not adequately characterize the wide range of geomorphic conditions and land uses found in heterogeneous environments. The measurement of Pu239+240 shows great potential for developing quantitative watershed sediment budgets. With inductively-coupled plasma mass spectrometry, hundreds of samples may be processed in dramatically shorter times than the gamma spectrometry method used for Cs137 or alpha spectrometry method used for Pb210. We collected surface soil samples from Murder Creek in the Piedmont region of Georgia, USA, to compare Pu239+240 inventories with Cs137 and Pb210 inventories for a range of land uses in a predominantly forested watershed. Excellent correlations were found for radionuclide inventories (r2 =0.88, n = 38) and high resolution (4 mm) depth profiles. The second objective was to generate a sediment budget using the full Pu239+240 dataset (n = 309). Average Pu239+240 inventories were 70.0 Bq/m2 for hardwood forest, 60.0 Bq/m2 for pine plantation, 65.1 Bq/m2 for pine forest, 66.7 Bq/m2 for row crop agriculture and 67.9 Bq/m2 for pasture. The sediment budget will be constructed by converting inventories into site-specific erosion rates. Erosion rates will be scaled up to the watershed scale using GIS coverages of land use, soil, slope, and slope position. Results will be compared with Murder Creek sediment budgets in the scientific literature generated from RUSLE erosion modeling, USGS monitoring networks and reservoir sedimentation.

Biological availability of (238)U, (234)U and (226)Ra for wild berries and meadow grasses in natural ecosystems of Belarus.

PubMed

Sokolik, G A; Ovsiannikova, S V; Voinikava, K V; Ivanova, T G; Papenia, M V

2014-01-01

This work is devoted to investigation of behavior of (234)U, (238)U and (226)Ra by determining the soil to plant transfer under different natural conditions such as forest or swamped areas and meadow lands with different soil types. The paper summarizes the data on investigation of uranium and radium uptake by wild berries and natural meadow grasses in the typical conditions of Belarus. Parameters characterizing the biological availability of (234)U, (238)U and (226)Ra for bilberry (Vaccinium myrtillus), lingonberry (Vaccinium viti-idaea), blueberry (Vaccinium iliginosum) and cranberry (Vaccinium oxycoccus palustris) as well as for widely occurring mixed meadow vegetation, which belongs to the sedge-grass or grass-sedge associations and forbs, have been established. In the sites under investigation, the deposition levels of (238+239+240)Pu were less than 0.37 kBq m(-2) and (137)Cs deposition ranged between less than 0.37 and 37 kBq m(-2). It was found that activity concentrations of radionuclides in berries varied in the ranges of 0.037-0.11 for (234)U, 0.036-0.10 for (238)U and 0.11-0.43 Bq kg(-1) for (226)Ra, but in the mixed meadow grasses they were 0.32-4.4, 0.24-3.9 and 0.14-6.9 Bq kg(-1) accordingly. The (234)U/(238)U activity ratios were 1.02 ± 0.01 for wild berries, 1.20 ± 0.09 for underground meadow grasses and 1.02 ± 0.02 for proper soils. The concentration ratios (CRs, dry weight basis) of (234)U and (238)U for mixed meadow grasses were 0.036-0.42 and 0.041-0.46 respectively. The correspondent geometric means (GM) were 0.13 and 0.15 with geometric standard deviations (GSD) of 2.4. The CRs of (226)Ra for meadow grasses were 0.031-1.0 with GM 0.20 and GSD 2.6. The CRs of (234)U, (238)U and (226)Ra for wild berries ranged within 0.0018-0.008 (GM is 0.0034, GSD is 1.8), 0.0018-0.008 (GM is 0.0035, GSD is 1.8) and 0.005-0.033 (GM is 0.016, GSD is 2.1) accordingly. The highest CR values of uranium for mixed meadow grasses were found in the

Solid state reactions of CeO 2, PuO 2, (U,Ce)O 2 and (U,Pu)O 2 with K 2S 2O 8

NASA Astrophysics Data System (ADS)

Keskar, Meera; Kasar, U. M.; Mudher, K. D. Singh; Venugopal, V.

2004-09-01

Solid state reactions of CeO 2, PuO 2 and mixed oxides (U,Ce)O 2 and (U,Pu)O 2 containing different mol.% of Ce and Pu, were carried out with K 2S 2O 8 at different temperatures to identify the formation of various products and to investigate their dissolution behaviour. X-ray, chemical and thermal analysis methods were used to characterise the products formed at various temperatures. The products obtained by heating two moles of K 2S 2O 8 with one mole each of CeO 2, PuO 2, (U,Ce)O 2 and (U,Pu)O 2 at 400 °C were identified as K 4Ce(SO 4) 4, K 4Pu(SO 4) 4, K 4(U,Ce)(SO 4) 4 and K 4(U,Pu)(SO 4) 4, respectively. K 4Ce(SO 4) 4 further decomposed to form K 4Ce(SO 4) 3.5 at 600 °C and mixture of K 2SO 4 and CeO 2 at 950 °C. Thus the products formed during the reaction of 2K 2S 2O 8 + CeO 2 show that cerium undergoes changes in oxidation state from +4 to +3 and again to +4. XRD data of K 4Ce(SO 4) 4 and K 4Ce(SO 4) 3.5 were indexed on triclinic and monoclinic system, respectively. PuO 2 + 2K 2S 2O 8 reacts at 400 °C to form K 4Pu(SO 4) 4 which was stable upto 750 °C and further decomposes to form K 2SO 4 + PuO 2 at 1000 °C. The products formed at 400 °C during the reactions of the oxides and mixed oxides were found to be readily soluble in 1-2 M HNO 3.

Suitability of 239+240Pu and 137Cs as tracers for soil erosion assessment in mountain grasslands.

PubMed

Alewell, Christine; Meusburger, Katrin; Juretzko, Gregor; Mabit, Lionel; Ketterer, Michael E

2014-05-01

Anthropogenic radionuclides have been distributed globally due to nuclear weapons testing, nuclear accidents, nuclear weapons fabrication, and nuclear fuel reprocessing. While the negative consequences of this radioactive contamination are self-evident, the ubiquitous fallout radionuclides (FRNs) distribution form the basis for the use as tracers in ecological studies, namely for soil erosion assessment. Soil erosion is a major threat to mountain ecosystems worldwide. We compare the suitability of the anthropogenic FRNs, 137Cs and 239+240Pu as soil erosion tracers in two alpine valleys of Switzerland (Urseren Valley, Canton Uri, Central Swiss Alps and Val Piora, Ticino, Southern Alps). We sampled reference and potentially erosive sites in transects along both valleys. 137Cs measurements of soil samples were performed with a Li-drifted Germanium detector and 239+240Pu with ICP-MS. Our data indicates a heterogeneous deposition of the 137Cs, since most of the fallout origins from the Chernobyl April/May 1986 accident, when large parts of the European Alps were still snow-covered. In contrast, 239+240Pu fallout originated mainly from 1950s to 1960s atmospheric nuclear weapons tests, resulting in a more homogenous distribution and thus seems to be a more suitable tracer in mountainous grasslands. Soil erosion assessment using 239+240Pu as a tracer pointed to a huge dynamic and high heterogeneity of erosive processes (between sedimentation of 1.9 and 7 t ha(-1) yr(-1) and erosion of 0.2-16.4 t ha(-1) yr(-1) in the Urseren Valley and sedimentation of 0.4-20.3 t ha(-1) yr(-1) and erosion of 0.1-16.4 t ha(-1) yr(-1) at Val Piora). Our study represents a novel and successful application of 239+240Pu as a tracer of soil erosion in a mountain environment. Copyright © 2013 The Authors. Published by Elsevier Ltd.. All rights reserved.

Use of DTPA for increasing the rate of elimination of plutonium-238 and americium-241 from rodents after their inhalation as the nitrates.

PubMed

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

1985-11-01

This study has shown that: both inhaled (2 mumol/kg) and injected (30 mumol/kg) diethylenetriaminepenta-acetic acid (DTPA) can reduce the lung deposit of 238 Pu and 241 Am inhaled as nitrate to about 1% of that in untreated controls; injection of DTPA is more effective than aerosolized DTPA for reducing deposits of 238Pu and 241Am in the liver and skeleton; combined treatment involving early inhalation of DTPA followed by repeated intravenous injections is likely to be the most effective treatment for workers who have accidentally inhaled plutonium and americium nitrates.

Chemical thermodynamic representation of (U, Pu, Am)O 2- x

NASA Astrophysics Data System (ADS)

Osaka, Masahiko; Namekawa, Takashi; Kurosaki, Ken; Yamanaka, Shinsuke

2005-09-01

The oxygen potential isotherms of (U, Pu, Am)O 2- x were represented by a chemical thermodynamic model proposed by Lindemer et al. It was assumed in the present model that (U, Pu, Am)O 2- x consisted of the chemical species [UO 2], [PuO 2], [Pu 4/3O 2], [AmO 2] and [Am 5/4O 2] in a pseudo-quaternary system by treating the reduction rates of Pu and Am as identical; furthermore an interaction between [Am 5/4O 2] and [UO 2] was introduced. The agreement between analytical and experimental isotherms was good, but the analytical values slightly overestimated the experimental values especially in the case of lower Am content. Adding an interaction between [Am 5/4O 2] and [PuO 2] to the model resulted in a better representation.

242Pu absolute neutron-capture cross section measurement

NASA Astrophysics Data System (ADS)

Buckner, M. Q.; Wu, C. Y.; Henderson, R. A.; Bucher, B.; Chyzh, A.; Bredeweg, T. A.; Baramsai, B.; Couture, A.; Jandel, M.; Mosby, S.; O'Donnell, J. M.; Ullmann, J. L.

2017-09-01

The absolute neutron-capture cross section of 242Pu was measured at the Los Alamos Neutron Science Center using the Detector for Advanced Neutron-Capture Experiments array along with a compact parallel-plate avalanche counter for fission-fragment detection. During target fabrication, a small amount of 239Pu was added to the active target so that the absolute scale of the 242Pu(n,γ) cross section could be set according to the known 239Pu(n,f) resonance at En,R = 7.83 eV. The relative scale of the 242Pu(n,γ) cross section covers four orders of magnitude for incident neutron energies from thermal to ≈ 40 keV. The cross section reported in ENDF/B-VII.1 for the 242Pu(n,γ) En,R = 2.68 eV resonance was found to be 2.4% lower than the new absolute 242Pu(n,γ) cross section.

Prompt fission neutron spectra from fission induced by 1 to 8 MeV neutrons on U235 and Pu239 using the double time-of-flight technique

NASA Astrophysics Data System (ADS)

Noda, S.; Haight, R. C.; Nelson, R. O.; Devlin, M.; O'Donnell, J. M.; Chatillon, A.; Granier, T.; Bélier, G.; Taieb, J.; Kawano, T.; Talou, P.

2011-03-01

Prompt fission neutron spectra from U235 and Pu239 were measured for incident neutron energies from 1 to 200 MeV at the Weapons Neutron Research facility (WNR) of the Los Alamos Neutron Science Center, and the experimental data were analyzed with the Los Alamos model for the incident neutron energies of 1-8 MeV. A CEA multiple-foil fission chamber containing deposits of 100 mg U235 and 90 mg Pu239 detected fission events. Outgoing neutrons were detected by the Fast Neutron-Induced γ-Ray Observer array of 20 liquid organic scintillators. A double time-of-flight technique was used to deduce the neutron incident energies from the spallation target and the outgoing energies from the fission chamber. These data were used for testing the Los Alamos model, and the total kinetic energy parameters were optimized to obtain a best fit to the data. The prompt fission neutron spectra were also compared with the Evaluated Nuclear Data File (ENDF/B-VII.0). We calculate average energies from both experimental and calculated fission neutron spectra.

Field Application of 238U/235U Measurements To Detect Reoxidation and Mobilization of U(IV).

PubMed

Jemison, Noah E; Shiel, Alyssa E; Johnson, Thomas M; Lundstrom, Craig C; Long, Philip E; Williams, Kenneth H

2018-03-20

Biostimulation to induce reduction of soluble U(VI) to relatively immobile U(IV) is an effective strategy for decreasing aqueous U(VI) concentrations in contaminated groundwater systems. If oxidation of U(IV) occurs following the biostimulation phase, U(VI) concentrations increase, challenging the long-term effectiveness of this technique. However, detecting U(IV) oxidation through dissolved U concentrations alone can prove difficult in locations with few groundwater wells to track the addition of U to a mass of groundwater. We propose the 238 U/ 235 U ratio of aqueous U as an independent, reliable tracer of U(IV) remobilization via oxidation or mobilization of colloids. Reduction of U(VI) produces 238 U-enriched U(IV), whereas remobilization of solid U(IV) should not induce isotopic fractionation. The incorporation of remobilized U(IV) with a high 238 U/ 235 U ratio into the aqueous U(VI) pool produces an increase in 238 U/ 235 U of aqueous U(VI). During several injections of nitrate to induce U(IV) oxidation, 238 U/ 235 U consistently increased, suggesting 238 U/ 235 U is broadly applicable for detecting mobilization of U(IV).

Uranium-series constraints on radionuclide transport and groundwater flow at the Nopal I uranium deposit, Sierra Pena Blanca, Mexico.

PubMed

Goldstein, Steven J; Abdel-Fattah, Amr I; Murrell, Michael T; Dobson, Patrick F; Norman, Deborah E; Amato, Ronald S; Nunn, Andrew J

2010-03-01

Uranium-series data for groundwater samples from the Nopal I uranium ore deposit were obtained to place constraints on radionuclide transport and hydrologic processes for a nuclear waste repository located in fractured, unsaturated volcanic tuff. Decreasing uranium concentrations for wells drilled in 2003 are consistent with a simple physical mixing model that indicates that groundwater velocities are low ( approximately 10 m/y). Uranium isotopic constraints, well productivities, and radon systematics also suggest limited groundwater mixing and slow flow in the saturated zone. Uranium isotopic systematics for seepage water collected in the mine adit show a spatial dependence which is consistent with longer water-rock interaction times and higher uranium dissolution inputs at the front adit where the deposit is located. Uranium-series disequilibria measurements for mostly unsaturated zone samples indicate that (230)Th/(238)U activity ratios range from 0.005 to 0.48 and (226)Ra/(238)U activity ratios range from 0.006 to 113. (239)Pu/(238)U mass ratios for the saturated zone are <2 x 10(-14), and Pu mobility in the saturated zone is >1000 times lower than the U mobility. Saturated zone mobility decreases in the order (238)U approximately (226)Ra > (230)Th approximately (239)Pu. Radium and thorium appear to have higher mobility in the unsaturated zone based on U-series data from fractures and seepage water near the deposit.

New prompt fission gamma-ray spectral data from 239Pu(nth, f) in response to a high priority request from OECD Nuclear Energy Agency

NASA Astrophysics Data System (ADS)

Gatera, Angélique; Belgya, Tamás; Geerts, Wouter; Göök, Alf; Hambsch, Franz-Josef; Lebois, Matthieu; Maróti, Boglárka; Oberstedt, Stephan; Oberstedt, Andreas; Postelt, Frederik; Qi, Liqiang; Szentmiklósi, Laszló; Vidali, Marzio; Zeiser, Fabio

2017-09-01

Benchmark reactor calculations have revealed an underestimation of γ-heat following fission of up to 28%. To improve the modelling of new nuclear reactors, the OECD/NEA initiated a nuclear data High Priority Request List (HPRL) entry for the major isotopes (235U, 239Pu). In response to that HPRL entry, we executed a dedicated measurement program on prompt fission γ-rays employing state-of-the-art lanthanum bromide (LaBr3) detectors with superior timing and good energy resolution. Our new results from 252Cf(sf), 235U(nth,f) and 241Pu(nth,f) provide prompt fission γ-ray spectra characteristics : average number of photons per fission, average total energy per fission and mean photon energy; all within 2% of uncertainty. We present preliminary results on 239Pu(nth,f), recently measured at the Budapest Neutron Centre and supported by the CHANDA Trans-national Access Activity, as well as discussing our different published results in comparison to the historical data and what it says about the discrepancy observed in the benchmark calculations.

Sources and pathways of artificial radionuclides to soils at a High Arctic site.

PubMed

Lokas, E; Bartmiński, P; Wachniew, P; Mietelski, J W; Kawiak, T; Srodoń, J

2014-11-01

Activity concentrations, inventories and activity ratios of (137)Cs, (238)Pu, (239 + 240)Pu and (241)Am in soil profiles were surveyed in the dry tundra and the adjoining proglacial zones of glaciers at a High Arctic site on Svalbard. Vertical profiles of radionuclide activities were determined in up to 14-cm-thick soil sequences. Additionally, soil properties (pH, organic matter, texture, mineral composition and sorption capacity) were analyzed. Results obtained in this study revealed a large range of activity concentrations and inventories of the fallout radionuclides from the undetectable to the uncommonly high levels (inventories of 30,900 ± 940, 47 ± 6, 886 ± 80 and 296 ± 19 Bq/m(2) for (137)Cs, (238)Pu, (239 + 240)Pu and (241)Am, respectively) found in two profiles from the proglacial zone. Concentration of these initially airborne radionuclides in the proglacial zone soils is related to their accumulation in cryoconites that have a large ability to concentrate trace metals. The cryoconites develop on the surface of glaciers, and the material they accumulate is deposited on land surface after the glaciers retreat. The radionuclide inventories in the tundra soils, which effectively retain radionuclides due to high organic matter contents, were comparable to the global fallout deposition for this region of the world. The (238)Pu/(239 + 240)Pu activity ratios for tundra soils suggested global fallout as the dominant source of Pu. The (238)Pu/(239 + 240)Pu and (239 + 240)Pu/(137)Cs activity ratios in the proglacial soils pointed to possible contributions of these radionuclides from other, unidentified sources.

Prospects of heavy and superheavy element production via inelastic nucleus-nucleus collisions - from 238U+238U to18O+254Es

NASA Astrophysics Data System (ADS)

Schädel, Matthias

2016-12-01

Multi-nucleon transfer reactions, frequently termed deep-inelastic, between heavy-ion projectiles and actinide targets provide prospects to synthesize unknown isotopes of heavy actinides and superheavy elements with neutron numbers beyond present limits. The 238U on 238U reaction, which revealed essential aspects of those nuclear reactions leading to surviving heavy nuclides, mainly produced in 3n and 4n evaporation channels, is discussed in detail. Positions and widths of isotope distributions are compared. It is shown, as a general rule, that cross sections peak at irradiation energies about 10% above the Coulomb barrier. Heavy target nuclei are essential for maximizing cross sections. Experimental results from the 238U on 248Cm reaction, including empirical extrapolations, are compared with theoretical model calculations predicting relatively high cross sections for neutron-rich nuclei. Experiments to test the validity of such predictions are proposed. Comparisons between rather symmetric heavy-ion reactions like 238U on 248Cm (or heavier targets up to 254Es) with very asymmetric ones like 18O on 254Es reveal that the ones with 238U as a projectile have the highest potential in the superheavy element region while the latter ones can be advantageous for the synthesis of heavy actinide isotopes. Concepts for highly efficient recoil separators designed for transfer products are presented.

The Application of 238U/235U as a Redox-Proxy for Past Ocean Chemistry

NASA Astrophysics Data System (ADS)

Andersen, M. B.; Westermann, S.; Bahniuk, A.; Vasconcelos, C.; McKenzie, J. A.; Föllmi, K. B.; Vance, D.

2014-12-01

The recent discovery of significant variation in 238U/235U caused by redox change at the surface Earth has led to its use to extract information on the oxygenation state of ancient oceans from marine sediments [e.g. 1]. Recent studies have focused on improving the understanding of the 238U/235U signature in modern marine carbonates [2] and black shales [3] to improve the robustness of this tracer. To further advance its use we have focused on improving our understanding of 238U/235U systematics in modern dolomite, another commonly occurring rock-type in the geological record, before turning to 238U/235U signatures in ancient sediments. The measured dolomite samples, precipitated in modern environments of coastal hypersaline lagoons in Brazil, all exhibit 238U/235U values that deviate from the seawater composition [3]. Observed values are both lighter (ca. 130 ppm; as also observed in dolomite from tidal-ponds on Bahamas [2]) and heavier (50-180 ppm). These distinct 238U/235U values for different dolomite-precipitates likely attest to the particular formation style, as well as early diagenetic processes. We use such modern settings to discuss the utility of 238U/235U in ancient sediments, the singularity of any observed 238U/235U signal, its relation to global ocean chemistry and potential diagenetic overprinting. These constraints are then used to evaluate a well-preserved marine carbonate section [4] and published black shale 238U/235U data [1], both deposited during the Oceanic Anoxic Event 2 (93 Ma). We discuss the capabilities of both the carbonate and black shale section for retaining information on the 238U/235U composition in the ocean during OAE 2. [1] Montoya-Pino et al. (2010) Geology, 38, 315-318 [2] Romaniello et al. (2013) 362, 305-316 [3] Andersen et al. (2014) EPSL, 400, 184-194 [4] Westermann et al. (2010) Cret. Res., 31, 500-514

Activity disequilibrium between 234U and 238U isotopes in natural environment.

PubMed

Boryło, Alicja; Skwarzec, Bogdan

The aim of this work was to calculate the values of the 234 U/ 238 U activity ratio in natural environment (water, sediments, Baltic organisms and marine birds from various regions of the southern Baltic Sea; river waters (the Vistula and the Oder River); plants and soils collected near phosphogypsum waste heap in Wiślinka (Northern Poland) and deer-like animals from Northern Poland. On the basis of the studies it was found that the most important processes of uranium geochemical migration in the southern Baltic Sea ecosystem are the sedimentation of suspended material and the vertical diffusion from the sediments into the bottom water. Considerable values of the 234 U/ 238 U are characterized for the Vistula and Oder Rivers and its tributaries. The values of the 234 U/ 238 U activity ratio in different tissues and organs of the Baltic organisms, sea birds and wild deer are varied. Such a large variation value of obtained activity ratios indicates different behavior of uranium isotopes in the tissues and organisms of sea birds and wild animals. This value shows that uranium isotopes can be disposed at a slower or faster rate. The values of the 234 U/ 238 U activity ratio in the analyzed plants, soils and mosses collected in the vicinity of phosphogypsum dumps in Wiślinka are close to one and indicate the phosphogypsum origin of the analyzed nuclides. Uranium isotopes 234 U and 238 U are not present in radioactive equilibrium in the aquatic environment, which indicates that their activities are not equal. The inverse relationship is observed in the terrestrial environment, where the value of the of the 234 U/ 238 U activity ratio really oscillates around unity.

28 CFR 2.38 - Community supervision by U.S. Probation Officers.

Code of Federal Regulations, 2011 CFR

2011-07-01

... 28 Judicial Administration 1 2011-07-01 2011-07-01 false Community supervision by U.S. Probation Officers. 2.38 Section 2.38 Judicial Administration DEPARTMENT OF JUSTICE PAROLE, RELEASE, SUPERVISION AND... § 2.38 Community supervision by U.S. Probation Officers. (a) Pursuant to sections 3655 and 4203(b)(4...

28 CFR 2.38 - Community supervision by U.S. Probation Officers.

Code of Federal Regulations, 2013 CFR

2013-07-01

... 28 Judicial Administration 1 2013-07-01 2013-07-01 false Community supervision by U.S. Probation Officers. 2.38 Section 2.38 Judicial Administration DEPARTMENT OF JUSTICE PAROLE, RELEASE, SUPERVISION AND... § 2.38 Community supervision by U.S. Probation Officers. (a) Pursuant to sections 3655 and 4203(b)(4...

28 CFR 2.38 - Community supervision by U.S. Probation Officers.

Code of Federal Regulations, 2010 CFR

2010-07-01

... 28 Judicial Administration 1 2010-07-01 2010-07-01 false Community supervision by U.S. Probation Officers. 2.38 Section 2.38 Judicial Administration DEPARTMENT OF JUSTICE PAROLE, RELEASE, SUPERVISION AND... § 2.38 Community supervision by U.S. Probation Officers. (a) Pursuant to sections 3655 and 4203(b)(4...

(234)U/(238)U signatures associated with uranium ore bodies: part 1 Ranger 3.

PubMed

Lowson, Richard T; McIntyre, Mark G

2013-04-01

The Ranger 3 ore body is an early Proterozoic U ore body in the Alligator Rivers U province, Northern Territory, Australia. It has surface expression with a redox front located between 30 and 50 m below the surface. The ground water U concentration and (234)U/(238)U AR signature in the top 10 m of the weathered zone are reported for 357 samples collected over 4 wet seasons, at 5 depths, along a transect in-line with the hydraulic gradient and along the centre line of the ore body and its associated dispersion halo. The results show that the weathered zone displays a general U isotope feature for this type of ore body with the (234)U/(238)U AR for the ground water and amorphous phase of the solid matrix being less than 1. The ground water (234)U/(238)U AR is independent of the annual monsoonal climate and depth within the range surface to 10 m. In the vicinity of the U ore body the ground water (234)U/(238)U AR is 0.75 and is very similar to the (234)U/(238)U AR of the amorphous phase of the solid (0.76). The (234)U/(238)U ARs of the amorphous phase and ground water rise and separate to values of 0.88 and 1.02 at the end of the transect. The rise and separation in (234)U/(238)U AR are interpreted as evidence that the source of the U in the ground water is from the water-soluble sub-phase of the amorphous phase and that the ground water flow is too fast to allow the processes occurring across the solid-water interface to reach chemical equilibrium. The data set is a robust characterisation of the coarse and fine detail of the (234)U/(238)U AR signature in the weathered zone of U ore bodies. Copyright © 2012 Elsevier Ltd. All rights reserved.

Prompt fissionγ-ray characteristics from neutron-induced fission on 239Pu and the time-dependence of prompt-γray emission

NASA Astrophysics Data System (ADS)

Gatera, Angélique; Göök, Alf; Hambsch, Franz-Josef; Moens, André; Oberstedt, Andreas; Oberstedt, Stephan; Sibbens, Goedele; Vanleeuw, David; Vidali, Marzio

2018-03-01

Recent years have seen an increased interest in prompt fission γ-ray (PFG) measurements motivated by a high priority request of the OECD/NEA for high precision data, mainly for the nuclear fuel isotopes 235U and 239Pu. Our group has conducted a PFG measurement campaign using state-of-the-art lanthanum halide detectors for all the main actinides to a precision better than 3%. The experiments were performed in a coincidence setup between a fission trigger and γ-ray detectors. The time-of-flight technique was used to discriminate photons, traveling at the speed of light, and prompt fission neutrons. For a full rejection of all neutrons below 20 MeV, the PFG time window should not be wider than a few nanoseconds. This window includes most PFG, provided that no isomeric states were populated during the de-excitation process. When isomeric states are populated, PFGs can still be emitted up to 1 yus after the instant of fission or later. To study these γ-rays, the detector response to neutrons had to be determined and a correction had to be applied to the γ-ray spectra. The latest results for PFG characteristics from the reaction 239Pu(nth,f) will be presented, together with an analysis of PFGs emitted up to 200 ns after fission in the spontaneous fission of 252Cf as well as for thermal-neutron induced fission on 235U and 239Pu. The results are compared with calculations in the framework of the Hauser-Feshbach Monte Carlo code CGMF and FIFRELIN.

Status summary of chemical processing development in plutonium-238 supply program

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

Collins, Emory D.; Benker, Dennis; Wham, Robert M.

This document summarizes the status of development of chemical processing in the Plutonium-238 Supply Program (PSP) near the end of Demonstration 1. The objective of the PSP is “to develop, demonstrate, and document a production process that meets program objectives and to prepare for its operation” (Frazier et al. 2016). Success in the effort includes establishing capability using the current infrastructure to produce Np targets for irradiation in Department of Energy research reactors, chemically processing the irradiated targets to separate and purify the produced Pu and transferring the PuO 2 product to Los Alamos National Laboratory (LANL) at an averagemore » rate of 1.5 kg/y.« less

Anomalous levels of 90Sr and 239,240Pu in Florida corals: Evidence of coastal processes

NASA Astrophysics Data System (ADS)

Purdy, Caroline B.; Druffel, Ellen R. M.; Livingston, Hugh D.

1989-06-01

Strontium-90, a radionuclide whose primary source is fallout from nuclear weapons testing, serves as a tritium-like tracer of ocean circulation. The historical record of 90Sr activities in the annual bands of island corals have been shown by other investigators to reflect the 90Sr concentration in surface waters at those site. Strontium-90 activities measured in annual bands in Montastrea annularis from the Florida Keys are 30-120% higher than those in corresponding peak activity years (1960-1965) of a Bermuda coral ( Diploria). The Bermuda 90Sr activity record reflects the fallout source only, whereas the additional 90Sr activity in the Florida Keys is expected to reflect a coastal runoff source as well as the fallout. The coastal circulation patterns off the northern and western edge of the Florida Current further act to concentrate and prolong the exposure of the runoff 90Sr to the corals. Six measured 239,240Pu activities in the Florida coral are 30% of 239,240Pu activities in island coral records previously reported. Since Pu is expected to be scavenged by particles in coastal waters, this decrease in 239,240Pu substantiates the importance of coastal influences in the Florida 90Sr record. Strontium-90 activities measured in subannual coral bands from 1973 to 1974 reflect seasonal changes in the 90Sr concentrations in the surface layer of the coastal waters. This may reflect Loop Current intrusion events. The seasonal and long-term coral 90Sr data presented in this paper suggests that coastal 90Sr coral time series may be very useful for documenting coastal circulation patterns.

A study of nuclear structure for 244Cm, 241Am, 238Pu, 210Po, 147Pm, 137Cs, 90Sr and 63Ni nuclei used in nuclear battery

NASA Astrophysics Data System (ADS)

Artun, Ozan

2017-07-01

In this paper, we intend to extend the nuclear data of 244Cm, 241Am, 238Pu, 210Po, 147Pm, 137Cs, 90Sr and 63Ni nuclei used in nuclear battery technology, because, these nuclei are quite important for space investigations in radioisotope thermoelectric generator (RTG) and for microelectronic technologies in betavoltaic batteries. Therefore, the nuclear structure properties of nuclei such as separation energies, neutron skin thicknesses, proton, charge and neutron density distributions as a function of radius, the root mean square (rms) proton, charge and neutron radii, binding energies per particle, have been investigated by Hartree-Fock with eight different Skyrme forces. The obtained results have been compared with the experimental data in literature and relativistic mean field theory (RMFT) results.

Minimum pickup velocity ( U pu) of nanoparticles in gas-solid pneumatic conveying

NASA Astrophysics Data System (ADS)

Anantharaman, Aditya; van Ommen, J. Ruud; Chew, Jia Wei

2015-12-01

This paper is the first systematic study of the pneumatic conveying of nanoparticles. The minimum pickup velocity, U pu, of six nanoparticle species of different materials [i.e., silicon dioxide (SiO2), aluminum oxide (Al2O3), and titanium dioxide (TiO2)] and surfaces (i.e., apolar and polar) was determined by the weight loss method. Results show that (1) due to relative lack of hydrogen bonding, apolar nanoparticles had higher mass loss values at the same velocities, mass loss curves with accentuated S-shaped profiles, and lower U pu values, (2) among the three species, SiO2, which has the lowest Hamaker coefficient, exhibited the greatest discrepancy between apolar and polar surfaces with respect to both mass loss curves and U pu values, (3) U mf,polar/ U mf,apolar was between 1 and 3.5 times that of U pu,polar/ U pu,apolar due to greater extents of hydrogen bonding associated with U mf, (4) U pu values were at least an order-of-magnitude lower than that expected from the well-acknowledged U pu correlation (Kalman et al., Powder Technol 160:103-113, 2005) due to agglomeration, (5) although nanoparticles should be categorized as Zone III (Kalman et al. 2005) (or Geldart group C, Powder Technol 7:285-292, 1973), the nanoparticles, and primary and complex agglomerates agreed more with the Zone I (or Geldart group B) correlation.

Background reduction in 236U/238U measurements

NASA Astrophysics Data System (ADS)

Buompane, Raffaele; De Cesare, Mario; De Cesare, Nicola; Di Leva, Antonino; D'Onofrio, Antonio; Fifield, L. Keith; Fröhlich, Michaela; Gialanella, Lucio; Marzaioli, Fabio; Sabbarese, Carlo; Terrasi, Filippo; Tims, Stephen; Wallner, Anton

2015-10-01

The measurements of actinide isotopic ratios, in particular 236U/238U, in environmental samples requires high sensitivity. In particular, special effort must be devoted to the suppression of interfering nuclides, such as 235,238U, when measuring 236U. At the AMS facility of CIRCE, isotopic ratios down to ∼10-10 are currently measured using a gas E - ΔE detector. In order to push this limit lower towards natural levels, a time-of-flight system is used, featuring a micro-channel plate start detector and a Si stop detector. As the mass resolution of the latter is limited by the layout, an attempt to reduce the abundant isotope interference by other means has been undertaken. In this study, we report preliminary results on the characterization of the presence of molecular interferences when using UO-, UC- and UC2- as injected molecular ions. In particular the possibility to stabilize the current yield from carbide cathodes has been investigated: it was found that the best cathode preparation procedure is obtained pressing U salts baked at 800 °C mixed with graphite and Al powder. Moreover, the 238U background in 236U measurements is strongly reduced injecting UC- ions, as verified using a time-of-flight detection system. On the other hand, 235U interference is larger with respect to UO- injection, but this increase is smaller than expected on the basis of abundances of 13C and 17O in UC and UC2 molecules on one side and UO, on the other.

Relativistic Coulomb Fission

NASA Technical Reports Server (NTRS)

Norbury, John W.

1992-01-01

Nuclear fission reactions induced by the electromagnetic field of relativistic nuclei are studied for energies relevant to present and future relativistic heavy ion accelerators. Cross sections are calculated for U-238 and Pu-239 fission induced by C-12, Si-28, Au-197, and U-238 projectiles. It is found that some of the cross sections can exceed 10 b.

Inelastic neutron scattering from {sup 238}U

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

Moxon, M.C.; Wartena, J.A.; Weigmann, H.

1994-12-31

A measurement of the neutron inelastic scattering cross-section of {sup 238}U at 4 distant neutron energies in the low keV region has been undertaken using a 30m flight path on the pulsed neutron source GELINA. The scattered neutrons are detected in a plastic scintillator after passing through a 270 mm iron filter. The values obtained for the cross-section to the first excited 2{sup +} state in {sup 238}U are 293{+-}31, 660{+-}296, 978{+-}73 and 1176{+-}95 mb at neutron energies of 68.2, 126.6, 182.4 and 213.6 keV respectively.

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.

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

90Sr, 137Cs and (239,240)Pu concentration surface water time series in the Pacific and Indian Oceans--WOMARS results.

PubMed

Povinec, Pavel P; Aarkrog, Asker; Buesseler, Ken O; Delfanti, Roberta; Hirose, Katsumi; Hong, Gi Hoon; Ito, Toshimichi; Livingston, Hugh D; Nies, Hartmut; Noshkin, Victor E; Shima, Shigeki; Togawa, Orihiko

2005-01-01

Under an IAEA's Co-ordinated Research Project "Worldwide Marine Radioactivity Studies (WOMARS)" 90Sr, 137Cs and (239,240)Pu concentration surface water time series in the Pacific and Indian Oceans have been investigated. The Pacific and Indian Oceans were divided into 17 latitudinal boxes according to ocean circulation, global fallout patterns and the location of nuclear weapons test sites. The present levels and time trends in radionuclide concentrations in surface water for each box were studied and the corresponding effective half-lives were estimated. For the year 2000, the estimated average 90Sr, 137Cs and (239,240)Pu concentrations in surface waters of the Pacific and Indian Oceans varied from 0.1 to 1.5 mBq/L, 0.1 to 2.8 mBq/L, and 0.1 to 5.2 microBq/L, respectively. The mean effective half-lives for 90Sr and 137Cs in surface water were 12+/-1 years for the North, 20+/-1 years for the South and 21+/-2 years for the Equatorial Pacific. For (239,240)Pu the corresponding mean effective half-lives were 7+/-1 years for the North, 12+/-4 years for the South and 10+/-2 years for the Equatorial Pacific. For the Indian Ocean the mean effective half-lives of 137Cs and (239,240)Pu were 21+/-2 years and 9+/-1 years, respectively. There is evidence that fallout removal rates before 1970 were faster than those observed during recent decades. The estimated surface water concentrations of 90Sr, 137Cs and (239,240)Pu in latitudinal belts of the Pacific and Indian Oceans for the year 2000 may be used as the average levels so that any new contribution from nuclear facilities, nuclear weapons test sites, radioactive waste dumping sites and from possible nuclear accidents can be identified.

Neutron-induced fission cross section of 242Pu from 15 MeV to 20 MeV

NASA Astrophysics Data System (ADS)

Jovančević, N.; Salvador-Castineira, P.; Daraban, L.; Vidali, M.; Heyse, J.; Oberstedt, S.; Hambsch, F.-J.; Bonaldi, C.; Geerts, W.

2017-09-01

Accurate nuclear-data needs in the fast-neutron-energy region have been recently addressed for the development of next generation nuclear power plants (GEN-IV) by the OECD Nuclear Energy Agency (NEA). This sensitivity study has shown that of particular interest is the 242Pu(n,f) cross section for fast reactor systems. Measurements have been performed with quasi-monoenergetic neutrons in the energy range from 15 MeV to 20 MeV produced by the Van de Graaff accelerator of the JRC-Geel. A twin Frisch-grid ionization chamber has been used in a back-to-back configuration as fission fragment detector. The 242Pu(n,f) cross section has been normalized to 238U(n,f) cross section data. The results were compared with existing literature data and show acceptable agreement within 5%.

Thermodynamic assessments and inter-relationships between systems involving Al, Am, Ga, Pu, and U

DOE PAGES

Perron, A.; Turchi, P. E. A.; Landa, A.; ...

2016-12-01

We present a newly developed self-consistent CALPHAD thermodynamic database involving Al, Am, Ga, Pu, and U. A first optimization of the slightly characterized Am-Al and completely unknown Am-Ga phase diagrams is proposed. To this end, phase diagram features as crystal structures, stoichiometric compounds, solubility limits, and melting temperatures have been studied along the U-Al → Pu-Al → Am-Al, and U-Ga → Pu-Ga → Am-Ga series, and the thermodynamic assessments involving Al and Ga alloying are compared. In addition, two distinct optimizations of the Pu-Al phase diagram are proposed to account for the low temperature and Pu-rich region controversy. We includedmore » the previously assessed thermodynamics of the other binary systems (Am-Pu, Am-U, Pu-U, and Al-Ga) in the database and is briefly described in the present work. In conclusion, predictions on phase stability of ternary and quaternary systems of interest are reported to check the consistency of the database.« less

Thermodynamic assessments and inter-relationships between systems involving Al, Am, Ga, Pu, and U

NASA Astrophysics Data System (ADS)

Perron, A.; Turchi, P. E. A.; Landa, A.; Oudot, B.; Ravat, B.; Delaunay, F.

2016-12-01

A newly developed self-consistent CALPHAD thermodynamic database involving Al, Am, Ga, Pu, and U is presented. A first optimization of the slightly characterized Am-Al and completely unknown Am-Ga phase diagrams is proposed. To this end, phase diagram features as crystal structures, stoichiometric compounds, solubility limits, and melting temperatures have been studied along the U-Al → Pu-Al → Am-Al, and U-Ga → Pu-Ga → Am-Ga series, and the thermodynamic assessments involving Al and Ga alloying are compared. In addition, two distinct optimizations of the Pu-Al phase diagram are proposed to account for the low temperature and Pu-rich region controversy. The previously assessed thermodynamics of the other binary systems (Am-Pu, Am-U, Pu-U, and Al-Ga) is also included in the database and is briefly described in the present work. Finally, predictions on phase stability of ternary and quaternary systems of interest are reported to check the consistency of the database.

238U/235U determinations of some commonly used reference materials and U-bearing accessory minerals (Invited)

NASA Astrophysics Data System (ADS)

Condon, D.; Noble, S.; McLean, N.; Bowring, S. A.

2009-12-01

We have determined 238U/235U ratios for a suite of commonly used natural (CRM 112a, SRM 950a, HU-1) and synthetic (IRMM 184 and CRM U500) uranium reference materials in addition to several U-bearing accessory phases (zircon and monazite) by thermal ionisation mass-spectrometry (TIMS) using the IRMM 3636 233U-236U double spike to accurately correct for mass fractionation. The 238U/235U values for the natural uranium reference materials differ, by up to 0.1%, from the widely used ‘consensus’ value (137.88) with all having 238U/235U values less than 137.88. Similarly, initial 238U/235U data from zircon and monazite yield 238U/235U values that are lower than the ‘consensus’ value. The data obtained from U-bearing minerals is used to assess how the uncertainty in the 238U/235U ratio contributes to the systematic discordance observed in 238U/206Pb and 235U/207Pb dates (Mattinson, 2000; Schoene et al., 2006) which has traditionally been wholly attributed to error in the U decay constants. The 238U/235U determinations made on the synthetic reference materials yield results that are considerably more precise and accurate than the certified values (0.02% vs. 0.1% for CRM U500). The calibration of isotopic tracers used for U-daughter geochronology that are partially based upon these reference materials, and the resultant age determinations, will benefit from increased accuracy and precision. Mattinson, J.M., 2000. Revising the “gold standard”—the uranium decay constants of Jaffey et al., 1971. Eos Trans. AGU, Spring Meet. Suppl., Abstract V61A-02. Schoene B., Crowley J.L., Condon D.C., Schmitz M.D., Bowring S.A., 2006, Reassessing the uranium decay constants for geochronology using ID-TIMS U-Pb data. Geochimica et Cosmochimica Acta 70: 426-445

Geochemistry of speleothem records from southern Illinois: Development of (234U)/(238U) as a proxy for paleoprecipitation

USGS Publications Warehouse

Zhou, Juanzuo; Lundstrom, C.C.; Fouke, B.; Panno, S.; Hackley, K.; Curry, B.

2005-01-01

Natural waters universally show fractionation of uranium series (U-series) parent-daughter pairs, with the disequilibrium between 234U and 238U (234U)/(238U) commonly used as a tracer of groundwater flow. Because speleothems provide a temporal record of geochemical variations in groundwater precipitating calcite, (234U)/(238U) variations in speleothems provide a unique method of investigating water-rock interaction processes over millennium time scales. We present high precision Thermal Ionization Mass Spectrometric (TIMS) U-series analyses of speleothems and drip waters from Fogelpole Cave in southern Illinois. Data from all speleothems from the cave show an inverse correlation between (234U)/(238U) and U concentration, following the pattern observed in groundwaters globally. Within a 65-cm-long stalagmite, concordant 234U-238 U-230Th and 235U-231Pa ages for 5 samples indicate accurate chronology from 78.5 ka to 30 ka. Notably, (234U)/(238U)o which differs from most speleothems by having (234U)/(238U)o <1, positively correlates with speleothem growth rate. We generalize this to the observation that speleothems globally show (234U)/ (238U)o deviating farther from secular equilibrium at lower growth rates and approaching secular equilibrium at higher grow rates. Based on the Fogelpole observations, we suggest that groundwater (234U)/(238U) is controlled by the U oxidation state, the U concentration of the water and the fluid velocity. A transport model whereby U-series nuclides react and exchange with mineral surfaces can reproduce the observed trend between growth rate and (234U)/(238U)o. Based on this result, we suggest that (234U)/(238U)o in speleothems may record changes in hydrologic flux with time and thus could provide a useful proxy for long term records of paleoprecipitation. ?? 2005 Elsevier B.V. All rights reserved.

(234)U/(238)U signatures associated with uranium ore bodies: part 3 Koongarra.

PubMed

Lowson, Richard T

2013-04-01

The Koongarra ore body is an early Proterozoic U ore body in the Alligator Rivers U province, Northern Territory, Australia. It has surface expression with a redox front located ∼30 m below the surface. The (234)U/(238)U activity ratios (AR) for the ground water and the amorphous phase of the solid have been analysed for the ore zone and dispersion halo as a function of depth. The results display a (234)U/(238)U AR signature with depth which may be common to all U ore bodies. The (234)U/(238)U AR is depressed below secular equilibrium in the weathered material above the redox front; rises significantly above secular equilibrium in the vicinity of the redox front; and is followed by a gradual decrease with depth below the redox front. The amplitude of the profile is a function of local conditions. A model is proposed for the signature in which oxidising waters preferentially leach the (234)U sites at the redox front due to preconditioning of the (234)U sites by α recoil during the decay of (23)(8)U to (23)(4)U. Mass balance requires the solid material left behind the redox front to have a (234)U/(238)U AR reduced below 1. Local second order effects may be superimposed on the signature. The signature may have application to calibrating scenarios for nuclear waste repositories, assisting in understanding historical climates, economic evaluation of U ore bodies and U exploration. Copyright © 2012 Elsevier Ltd. All rights reserved.

(234)U/(238)U signatures associated with uranium ore bodies: part 2 Manyingee.

PubMed

Lowson, Richard T; McIntyre, Mark G

2013-04-01

The Manyingee ore body is a roll-front U ore body located at depth in the Cretaceous sandstone sediments of a Proterozoic palaeo valley. It is located in a confined aquifer. The aquifer is recharged 4 km upstream by the Ashburton River. Groundwater samples were collected at and up to 4.7 km downstream of the ore body. The ground water (234)U/(238)U activity ratios (AR) were elevated to 1.86 in the vicinity of the ore body and then declined to 1.06 over the 4.7 km transect. The elevated (234)U/(238)U ARs are attributed to selective leaching of (234)U sites by oxidising waters, with α recoil as a necessary precursor to produce activated (234)U sites. Direct ejection into another phase following α recoil is considered to be a minor contributor to (234)U -(238)U disequilibrium in this environment. The profile is considered to be typical of the (234)U/(238)U AR profile at and down gradient of the redox front of a U ore body. Crown Copyright © 2012. Published by Elsevier Ltd. All rights reserved.

Reexamining the heavy-ion reactions 238U+238U and 238U+248Cm and actinide production close to the barrier

NASA Astrophysics Data System (ADS)

Kratz, J. V.; Schädel, M.; Gäggeler, H. W.

2013-11-01

Recent theoretical work has renewed interest in radiochemically determined isotope distributions in reactions of 238U projectiles with heavy targets that had previously been published only in parts. These data are being reexamined. The cross sections σ(Z) below the uranium target have been determined as a function of incident energy in thick-target bombardments. These are compared to predictions by a diffusion model whereby consistency with the experimental data is found in the energy intervals 7.65-8.30 MeV/u and 6.06-7.50 MeV/u. In the energy interval 6.06-6.49 MeV/u, the experimental data are lower by a factor of 5 compared to the diffusion model prediction indicating a threshold behavior for massive charge and mass transfer close to the barrier. For the intermediate energy interval, the missing mass between the primary fragment masses deduced from the generalized Qgg systematics including neutron pair-breaking corrections and the centroid of the experimental isotope distributions as a function of Z have been used to determine the average excitation energy as a function of Z. From this, the Z dependence of the average total kinetic-energy loss (TKEL¯) has been determined. This is compared to that measured in a thin-target counter experiment at 7.42 MeV/u. For small charge transfers, the values of TKEL¯ of this work are typically about 30 MeV lower than in the thin-target experiment. This difference is decreasing with increasing charge transfer developing into even slightly larger values in the thick-target experiment for the largest charge transfers. This is the expected behavior which is also found in a comparison of the partial cross sections for quasielastic and deep-inelastic reactions in both experiments. The cross sections for surviving heavy actinides, e.g., 98Cf, 99Es, and 100Fm indicate that these are produced in the low-energy tails of the dissipated energy distributions, however, with a low-energy cutoff at about 35 MeV. Excitation functions show

DFT+U Study of Chemical Impurities in PuO 2

DOE PAGES

Hernandez, Sarah C.; Holby, Edward F.

2016-05-24

In this paper, we employ density functional theory to explore the effects of impurities in the fluorite crystal structure of PuO 2. The impurities that were considered are known impurities that exist in metallic δ-phase Pu, including H, C, Fe, and Ga. These impurities were placed at various high-symmetry sites within the PuO 2 structure including an octahedral interstitial site, an interstitial site with coordination to two neighboring O atoms, an O substitutional site, and a Pu substitutional site. Incorporation energies were calculated to be energetically unfavorable for all sites except the Pu substitutional site. When impurities were placed inmore » a Pu substitutional site, complexes incorporating the impurities and O formed within the PuO 2 structure. The observed defect-oxygen structures were OH, CO 3, FeO 5, and GaO 3. The presence of these defects led to distortion of the surrounding O atoms within the structure, producing long-range disorder of O atoms. In contrast, perturbations of Pu atoms had a relatively short-range effect on the relaxed structures. These effects are demonstrated via radial distribution functions for O and Pu vacancies. Calculated electronic structure revealed hybridization of the impurity atom with the O valence states and a relative decrease in the Pu 5f states. Minor differences in band gaps were observed for the defected PuO 2 structures containing H, C, and Ga. Finally, Fe-containing structures, however, were calculated to have a significantly decreased band gap, where the implementation of a Hubbard U parameter on the Fe 3d orbitals will maintain the calculated PuO 2 band gap.« less

Spatial and temporal distribution of Pu in the Northwest Pacific Ocean using modern coral archives.

PubMed

Lindahl, Patric; Andersen, Morten B; Keith-Roach, Miranda; Worsfold, Paul; Hyeong, Kiseong; Choi, Min-Seok; Lee, Sang-Hoon

2012-04-01

Historical (239)Pu activity concentrations and (240)Pu/(239)Pu atom ratios were determined in skeletons of dated modern corals collected from three locations (Chuuk Lagoon, Ishigaki Island and Iki Island) to identify spatial and temporal variations in Pu inputs to the Northwest Pacific Ocean. The main Pu source in the Northwest Pacific is fallout from atmospheric nuclear weapons testing which consists of global fallout and close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands. PPG close-in fallout dominated the Pu input in the 1950s, as was observed with higher (240)Pu/(239)Pu atom ratios (>0.30) at the Ishigaki site. Specific fallout Pu contamination from the Nagasaki atomic bomb and the Ivy Mike thermonuclear detonation at the PPG were identified at Ishigaki Island from the (240)Pu/(239)Pu atom ratios of 0.07 and 0.46, respectively. During the 1960s and 1970s, global fallout was the major Pu source to the Northwest Pacific with over 60% contribution to the total Pu. After the cessation of the atmospheric nuclear tests, the PPG again dominated the Pu input due to the continuous transport of remobilised Pu from the Marshall Islands along the North Equatorial Current and the subsequent Kuroshio Current. The Pu contributions from the PPG in recent coral bands (1984 onwards) varied over time with average estimated PPG contributions between 54% and 72% depending on location. Copyright © 2011 Elsevier Ltd. All rights reserved.

137Cs, 239,240Pu and 241Am in boreal forest soil and their transfer into wild mushrooms and berries.

PubMed

Lehto, Jukka; Vaaramaa, Kaisa; Leskinen, Anumaija

2013-02-01

Profiles of podzolic soil from boreal forests were sampled from eight sites in Finland and the distribution of (137)Cs in the soil layers was determined. In addition, (239,240)Pu and (241)Am were determined from two soil profiles taken at one sampling site. Inventories of (137)Cs in the soil profiles varied between 1.7 kBq/m(2) and 42 kBq/m(2), reflecting known variation in (137)Cs fallout from the Chernobyl accident. The highest proportions of the radionuclides were found in the organic layer at a depth of less than 5 cm, which on average contained 47% of (137)Cs, 76% of (239,240)Pu and 79% of (241)Am. In the litter, clearly higher proportions of (137)Cs were found compared to (239,240)Pu and (241)Am, probably indicating its more effective recycling from the organic layer back to the surface. Only very minor proportions of (137)Cs were recorded below 20 cm. The concentration of (137)Cs in the soil profiles could be approximated with a declining logarithmic trend. The activity concentrations of (137)Cs were determined for six wild mushroom species and three wild berry species at two sites, as well as the aggregated transfer factors and the distribution of (137)Cs between their various parts. In addition, (239,240)Pu and (241)Am were determined in one mushroom and three berry species at one site. Very high concentrations of (137)Cs, up to 20 kBq/kg (d.w.), were found in mushrooms, and their transfer factors were between 0.1 m(2)/kg and 1.0 m(2)/kg. In berries, the transfer factors were an order of magnitude lower. (137)Cs accumulated more in the caps of mushrooms and in the fruits of berries than in other parts. Transfer factors for (239,240)Pu and (241)Am were two to three orders of magnitude lower than those of (137)Cs. Copyright © 2012 Elsevier Ltd. All rights reserved.

Criticality Safety Controls for 55-Gallon Drums with a Mass Limit of 200 grams Pu-239

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

Chou, P

The following 200-gram Pu drum criticality safety controls are applicable to RHWM drum storage operations: (1) Mass (Fissile/Pu) - each 55-gallon drum or its equivalent shall be limited to 200 gram Pu or Pu equivalent; (2) Moderation - Hydrogen materials with a hydrogen density greater than that (0.133 g H/cc) of polyethylene and paraffin are not allowed and hydrogen materials with a hydrogen density no greater than that of polyethylene and paraffin are allowed with unlimited amounts; (3) Interaction - a spacing of 30-inches (76 cm) is required between arrays and 200-gram Pu drums shall be placed in arrays formore » 200-gram Pu drums only (no mingling of 200-gram Pu drums with other drums not meeting the drum controls associated with the 200-gram limit); (4) Reflection - no beryllium and carbon/graphite (other than the 50-gram waiver amount) is allowed, (note that Nat-U exceeding the waiver amount is allowed when its U-235 content is included in the fissile mass limit of 200 grams); and (5) Geometry - drum geometry, only 55-gallon drum or its equivalent shall be used and array geometry, 55-gallon drums are allowed for 2-high stacking. Steel waste boxes may be stacked 3-high if constraint.« less

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.

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.

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.

Reaction paths and host phases of uranium isotopes (235U; 238U), Saanich Inlet

NASA Astrophysics Data System (ADS)

Amini, M.; Holmden, C. E.; Francois, R. H.

2009-12-01

In recent times, Uranium has become increasingly the focus of stable isotope fractionation studies. Variations in 238U/235U have been reported as a result of redox reactions [1,2] from the nuclear field shift effect [3], and a mass-dependent, microbially-mediated, kinetic isotope effect [4]. The 238U/235U variability caused by changes in environmental redox conditions leads to an increase in the 238U/235U ratios of the reduced U species sequestered into marine sediments. This points to U isotope variability as a new tool to study ancient ocean redox changes. However, the process by which reduced sediments become enriched in the heavy isotopes of U is not yet known, and hence the utility of 238U/235U as a redox tracer remains to be demonstrated. In order to further constrain sedimentary U enrichment and related isotope effect, we are investigating U isotopic compositions of water samples and fresh surface sediment grab samples over a range of redox conditions in the seasonally anoxic Saanich Inlet, on the east coast of Vancouver Island. U was sequentially extracted from sediments in order to characterize specific fractions for their isotopic composition. The measurements were carried out by MC-ICPMS using 233U/236U-double spike technique. The data are reported as δ238U relative to NBL 112a with a 238U/235U ratio of 137.88 (2sd). External precision is better than 0.10‰ (2sd). Fifteeen analyses of seawater yielded δ238U of -0.42±0.08‰ (2sd). The results for the water samples indicate a homogenous δ238U value throughout the Saanich Inlet water column that matches the global seawater signature. All of the water samples from above and below average -0.42±0.05‰ (2sd). In contrast, a plankton net sample yielded a distinctly different, (about 0.5‰ lighter) isotope value. Bacterial reduction experiments [4] have also shown isotope enrichment factors of about -0.3‰. In addition, metal isotope fractionation occurs during adsorption with the light isotope being

MTS-6 detectors calibration by using ²³⁹Pu-Be neutron source.

PubMed

Wrzesień, Małgorzata; Albiniak, Łukasz; Al-Hameed, Hiba

2017-10-17

Thermoluminescent detectors, type MTS-6, containing isotope ⁶Li (lithium) are sensitive in the range of thermal neutron energy; the ²³⁹Pu-Be (plutonium-and-beryllium) source emits neutrons in the energy range from 1 to 11 MeV. These seemingly contradictory elements may be combined by using the paraffin moderator, a determined density of thermal neutrons in the paraffin block and a conversion coefficient neutron flux to kerma, not forgetting the simultaneous registration of the photon radiation inseparable from the companion neutron radiation. The main aim of this work is to present the idea of calibration of thermoluminescent detectors that consist of a ⁶Li isotope, by using ²³⁹Pu-Be neutron radiation source. In this work, MTS-6 and MTS-7 thermoluminescent detectors and a plutonium-and-beryllium (²³⁹Pu-Be) neutron source were used. Paraffin wax fills the block, acting as a moderator. The calibration idea was based on the determination of dose equivalent rate based on the average kerma rate calculated taking into account the empirically determined function describing the density of thermal neutron flux in the paraffin block and a conversion coefficient neutron flux to kerma. The calculated value of the thermal neutron flux density was 1817.5 neutrons/cm²/s and the average value of kerma rate determined on this basis amounted to 244 μGy/h, and the dose equivalent rate 610 μSv/h. The calculated value allowed for the assessment of the length of time of exposure of the detectors directly in the paraffin block. The calibration coefficient for the used batch of detectors is (6.80±0.42)×10^-7 Sv/impulse. Med Pr 2017;68(6):705-710. This work is available in Open Access model and licensed under a CC BY-NC 3.0 PL license.

The Effect of Early Diagenesis on the 238U/235U Ratio of Platform Carbonates.

NASA Astrophysics Data System (ADS)

Tissot, F.; Chen, C.; Go, B. M.; Naziemiec, M.; Healy, G.; Swart, P. K.; Dauphas, N.

2017-12-01

In the past 15 years, the so-called non-traditional stable isotopes systems (e.g., Mg, Fe, Mo, U) have emerged as powerful tracers of both high-T and low-T geochemical processes (e.g., [1]). Of particular interest for paleoredox studies is the ratio of "stable" isotopes of U (238U/235U), which has the potential to track the global extent of oceanic anoxia (e.g., [2, 3]). Indeed, in the modern ocean, U exists in two main oxidation states, soluble U6+ and insoluble U4+, and has a mean residence time of 400 kyr ([4]), much longer than the global ocean mixing time (1-2 kyr). As such the salinity-normalized ocean is homogeneous with regards to both U concentrations and isotopes (δ238USW = -0.392±0.005 ‰, [2]). The value of δ238USW at any given time is therefore the balance between U input to the ocean, mainly from rivers, and U removal, mostly into biogenic carbonates, anoxic/euxinic sediments and suboxic/hypoxic sediments (e.g., [2, 5]). Because the 238U/235U ratio of the past ocean cannot be measured directly, it has to be estimated from the measurement of the 238U/235U ratio of a sedimentary rock and assuming a constant fractionation factor. Carbonates appear as a promising record since they span most of Earth's history, and the δ238U values of modern primary carbonate precipitates and well-preserved fossil aragonitic coral up to 600 ka are indistinguishable from that of seawater (e.g., [2, 6, 7]). Yet, the effect of secondary processes on the δ238U values of non-coral carbonates, which represent the bulk of the rock record, has only been studied in a handful of shallow samples (down to 40cm, [6]) and remains poorly understood. To investigate the effect of early diagenesis on the 238U/235U ratio of carbonates on the 30kyr to 1Myr timescale, we measured δ13C, δ18O, and δ238U in samples from a 220m long drill core from the Bahamas carbonate platform. In order to separate lattice bound U from secondary U we developed a leaching protocol applicable to carbonate

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.

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

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.

Pacific Northwest Laboratory annual report for 1976 to the ERDA Assistant Administrator for Environment and Safety. Part 1. Biomedical Sciences

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

Thompson, R.C.

1977-05-01

Separate abstracts were prepared for individual sections of this publication. In addition to research reports the publication also contains organization charts, author index, and appendixes showing data on selected parameters relative to life-span dose-effect studies with inhaled /sup 239/PuO/sub 2/, /sup 238/PuO/sub 2/, and /sup 239/Pu in beagles. (HLW)

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.

Initial Eccentricity in Deformed 197Au+197Au and 238U+238U Collisions at RHIC

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

Filip, Peter; Lednicky, Richard; Masui, Hiroshi

2010-07-07

Initial eccentricity and eccentricity fluctuations of the interaction volume created in relativistic collisions of deformed {sup 197}Au and {sup 238}U nuclei are studied using optical and Monte-Carlo (MC) Glauber simulations. It is found that the non-sphericity noticeably influences the average eccentricity in central collisions and eccentricity fluctuations are enhanced due to deformation. Quantitative results are obtained for Au+Au and U+U collisions at energy {radical}s{sub NN} = 200 GeV.

Real time studies of Elastic Moduli Pu Aging using Resonant Ultrasound Spectroscopy

NASA Astrophysics Data System (ADS)

Maiorov, Boris

Elastic moduli are fundamental thermodynamic susceptibilities that connect directly to thermodynamics, electronic structure and give important information about mechanical properties. To determine the time evolution of the elastic properties in 239Pu and it Ga alloys, is imperative to study its phase stability and self-irradiation damage process. The most-likely sources of these changes include a) ingrowth of radioactive decay products like He and U, b) the introduction of radiation damage, c) δ-phase instabilities towards α-Pu or to Pu3Ga. The measurement of mechanical resonance frequencies can be made with extreme precision and used to compute the elastic moduli without corrections giving important insight in this problem. Using Resonant Ultrasound Spectroscopy, we measured the time dependence of the mechanical resonance frequencies of fine-grained polycrystalline δ-phase 239Pu, from 300K up to 480K. At room temperature, the shear modulus shows an increase in time (stiffening), but the bulk modulus decreases (softening). These are the first real-time measurements of room temperature aging of the elastic moduli, and the changes are consistent with elastic moduli measurements performed on 44 year old δ-Pu. As the temperature is increased, the rate of change increases exponentially, with both moduli becoming stiffer with time. For T>420K an abrupt change in the time dependence is observed indicating that the bulk and shear moduli have opposite rates of change. Our measurements provide a basis for ruling out the decomposition of δ-Pu towards α-Pu or Pu3Ga, and indicate a complex defect-related scenario from which we are gathering important clues.

Pu and 137Cs in the Yangtze River estuary sediments: distribution and source identification.

PubMed

Liu, Zhiyong; Zheng, Jian; Pan, Shaoming; Dong, Wei; Yamada, Masatoshi; Aono, Tatsuo; Guo, Qiuju

2011-03-01

Pu isotopes and (137)Cs were analyzed using sector field ICP-MS and γ spectrometry, respectively, in surface sediment and core sediment samples from the Yangtze River estuary. (239+240)Pu activity and (240)Pu/(239)Pu atom ratios (>0.18) shows a generally increasing trend from land to sea and from north to south in the estuary. This spatial distribution pattern indicates that the Pacific Proving Grounds (PPG) source Pu transported by ocean currents was intensively scavenged into the suspended sediment under favorable conditions, and mixed with riverine sediment as the water circulated in the estuary. This process is the main control for the distribution of Pu in the estuary. Moreover, Pu is also an important indicator for monitoring the changes of environmental radioactivity in the estuary as the river basin is currently the site of extensive human activities and the sea level is rising because of global climate changes. For core sediment samples the maximum peak of (239+240)Pu activity was observed at a depth of 172 cm. The sedimentation rate was estimated on the basis of the Pu maximum deposition peak in 1963-1964 to be 4.1 cm/a. The contributions of the PPG close-in fallout Pu (44%) and the riverine Pu (45%) in Yangtze River estuary sediments are equally important for the total Pu deposition in the estuary, which challenges the current hypothesis that the riverine Pu input was the major source of Pu budget in this area.

Gamma-ray Output Spectra from 239 Pu Fission

DOE PAGES

Ullmann, John

2015-05-25

The gamma-ray multiplicities, individual gamma-ray energy spectra, and total gamma energy spectra following neutron-induced fission of 239Pu were measured using the DANCE detector at Los Alamos. Corrections for detector response were made using a forward-modeling technique based on propagating sets of gamma rays generated from a paramaterized model through a GEANT model of the DANCE array and adjusting the parameters for best fit to the measured spectra. The results for the gamma-ray spectrum and multiplicity are in general agreement with previous results, but the measured total gamma-ray energy is about 10% higher. We found that a dependence of the gamma-raymore » spectrum on the gamma-ray multplicity was also observed. Finally, global model calculations of the multiplicity and gamma energy distributions are in good agreement with the data, but predict a slightly softer total-energy distribution.« less

Prompt fission gamma-ray emission spectral data for 239Pu(n,f) using fast directional neutrons from the LICORNE neutron source

NASA Astrophysics Data System (ADS)

Qi, L.; Wilson, J. N.; Lebois, M.; Al-Adili, A.; Chatillon, A.; Choudhury, D.; Gatera, A.; Georgiev, G.; Göök, A.; Laurent, B.; Maj, A.; Matea, I.; Oberstedt, A.; Oberstedt, S.; Rose, S. J.; Schmitt, C.; Wasilewska, B.; Zeiser, F.

2018-03-01

Prompt fission gamma-ray spectra (PFGS) have been measured for the 239Pu(n,f) reaction using fast neutrons at Ēn=1.81 MeV produced by the LICORNE directional neutron source. The setup makes use of LaBr3 scintillation detectors and PARIS phoswich detectors to measure the emitted prompt fission gamma rays (PFG). The mean multiplicity, average total energy release per fission and average energy of photons are extracted from the unfolded PFGS. These new measurements provide complementary information to other recent work on thermal neutron induced fission of 239Pu and spontaneous fission of 252Cf.

Fission product yield measurements using monoenergetic photon beams

NASA Astrophysics Data System (ADS)

Krishichayan; Bhike, M.; Tonchev, A. P.; Tornow, W.

2017-09-01

Measurements of fission products yields (FPYs) are an important source of information on the fission process. During the past couple of years, a TUNL-LANL-LLNL collaboration has provided data on the FPYs from quasi monoenergetic neutron-induced fission on 235U, 238U, and 239Pu and has revealed an unexpected energy dependence of both asymmetric fission fragments at energies below 4 MeV. This peculiar FPY energy dependence was more pronounced in neutron-induced fission of 239Pu. In an effort to understand and compare the effect of the incoming probe on the FPY distribution, we have carried out monoenergetic photon-induced fission experiments on the same 235U, 238U, and 239Pu targets. Monoenergetic photon beams of Eγ = 13.0 MeV were provided by the HIγS facility, the world's most intense γ-ray source. In order to determine the total number of fission events, a dual-fission chamber was used during the irradiation. These irradiated samples were counted at the TUNL's low-background γ-ray counting facility using high efficient HPGe detectors over a period of 10 weeks. Here we report on our first ever photofission product yield measurements obtained with monoenegetic photon beams. These results are compared with neutron-induced FPY data.

Concordant 241Pu-241Am Dating of Environmental Samples: Results from Forest Fire Ash

NASA Astrophysics Data System (ADS)

Goldstein, S. J.; Oldham, W. J.; Murrell, M. T.; Katzman, D.

2010-12-01

We have measured the Pu, 237Np, 241Am, and 151Sm isotopic systematics for a set of forest fire ash samples from various locations in the western U.S. including Montana, Wyoming, Idaho, and New Mexico. The goal of this study is to develop a concordant 241Pu (t1/2 = 14.4 y)-241Am dating method for environmental collections. Environmental samples often contain mixtures of components including global fallout. There are a number of approaches for subtracting the global fallout component for such samples. One approach is to use 242Pu/239Pu as a normalizing isotope ratio in a three-isotope plot, where this ratio for the non-global fallout component can be estimated or assumed to be small. This study investigates a new, complementary method of normalization using the long-lived fission product, 151Sm (t1/2 = 90 y). We find that forest fire ash concentrates actinides and fission products with ~1E10 atoms 239Pu/g and ~1E8 atoms 151Sm/g, allowing us to measure these nuclides by mass spectrometric (MIC-TIMS) and radiometric (liquid scintillation counting) methods. The forest fire ash samples are characterized by a western U.S. regional isotopic signature representing varying mixtures of global fallout with a local component from atmospheric testing of nuclear weapons at the Nevada Test Site (NTS). Our results also show that 151Sm is well correlated with the Pu nuclides in the forest fire ash, suggesting that these nuclides have similar geochemical behavior in the environment. Results of this correlation indicate that the 151Sm/239Pu atom ratio for global fallout is ~0.164, in agreement with an independent estimate of 0.165 based on 137Cs fission yields for atmospheric weapons tests at the NTS. 241Pu-241Am dating of the non-global fallout component in the forest fire ash samples yield ages in the late 1950’s-early 1960’s, consistent with a peak in NTS weapons testing at that time. The age results for this component are in agreement using both 242Pu and 151Sm normalizations

Analysis of oxygen potential of (U 0.7Pu 0.3)O 2±x and (U 0.8Pu 0.2)O 2±x based on point defect chemistry

NASA Astrophysics Data System (ADS)

Kato, Masato; Konashi, Kenji; Nakae, Nobuo

2009-06-01

Stoichiometries in (U 0.7Pu 0.3)O 2±x and (U 0.8Pu 0.2)O 2±x were analyzed with the experimental data of oxygen potential based on point defect chemistry. The relationship between the deviation x of stoichiometric composition and the oxygen partial pressure P was evaluated using a Kröger-Vink diagram. The concentrations of the point defects in uranium and plutonium mixed oxide (MOX) were estimated from the measurement data of oxygen potentials as functions of temperature and P. The analysis results showed that x was proportional to PO2±1/2 near the stoichiometric region of both (U 0.7Pu 0.3)O 2±x and (U 0.8Pu 0.2)O 2±x, which suggested that intrinsic ionization was the dominant defect. A model to calculate oxygen potential was derived and it represented the experimental data accurately. Further, the model estimated the thermodynamic data, ΔH and ΔS, of stoichiometric (U 0.7Pu 0.3)O 2.00 and (U 0.8Pu 0.2)O 2.00 as -552.5 kJ·mol -1 and -149.7 J·mol -1, and -674.0 kJ · mol -1 and -219.4 J · mol -1, respectively.

Analysis of $sup 239$Pu and $sup 241$Am in NAEG large-sized bovine samples

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

Major, W.J.; Lee, K.D.; Wessman, R.A.

Methods are described for the analysis of environmental levels of $sup 239$Pu and $sup 241$Am in large-sized bovine samples. Special procedure modifications to overcome the complexities of sample preparation and analyses and special techniques employed to prepare and analyze different types of bovine samples, such as muscle, blood, liver, and bone are discussed. (CH)

Dissolution behaviour of 238U, 234U and 230Th deposited on filters from personal dosemeters.

PubMed

Becková, Vera; Malátová, Irena

2008-01-01

Kinetics of dissolution of (238)U, (234)U and (230)Th dust deposited on filters from personal alpha dosemeters was studied by means of a 26-d in vitro dissolution test with a serum ultrafiltrate simulant. Dosemeters had been used by miners at the uranium mine 'Dolní Rozínka' at Rozná, Czech Republic. The sampling flow-rate as declared by the producer is 4 l h(-1) and the sampling period is typically 1 month. Studied filters contained 125 +/- 6 mBq (238)U in equilibrium with (234)U and (230)Th; no (232)Th series nuclides were found. Half-time of rapid dissolution of 1.4 d for (238)U and (234)U and slow dissolution half-times of 173 and 116 d were found for (238)U and (234)U, respectively. No detectable dissolution of (230)Th was found.

239Pu(n,γ) from 10 eV to 1.3 MeV

NASA Astrophysics Data System (ADS)

Mosby, S.; Bredeweg, T. A.; Couture, A.; Jandel, M.; Kawano, T.; Ullmann, J.; Henderson, R. A.; Wu, C. Y.

2018-02-01

The 239Pu(n,γ) cross section has been measured from 10 eV to 1.3 MeV as part of an experimental campaign using the Detector for Advanced Neutron Capture Experiments (DANCE). The work represents a significant advance in experimental technique, with improved systematic uncertainties in key regions in the keV to MeV regime. In general the results of prior work are confirmed with improved uncertainties, particularly at the highest incident neutron energies.

Chemical bonds and vibrational properties of ordered (U, Np, Pu) mixed oxides

NASA Astrophysics Data System (ADS)

Yang, Yu; Zhang, Ping

2013-01-01

We use density functional theory +U to investigate the chemical bonding characters and vibrational properties of the ordered (U, Np, Pu) mixed oxides (MOXs), UNpO4,NpPuO4, and UPuO4. It is found that the 5f electronic states of different actinide elements keep their localized characters in all three MOXs. The occupied 5f electronic states of different actinide elements do not overlap with each other and tend to distribute over the energy band gap of the other actinide element's 5f states. As a result, the three ordered MOXs all show smaller band gaps than those of the component dioxides, with values of 0.91, 1.47, and 0.19 eV for UNpO4,NpPuO4, and UPuO4, respectively. Through careful charge density analysis, we further show that the U-O and Pu-O bonds in MOXs show more ionic character than in UO2 and PuO2, while the Np-O bonds show more covalent character than in NpO2. The change in covalencies in the chemical bonds leads to vibrational frequencies of oxygen atoms that are different in MOXs.

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

Fractionation in the solar nebula. II - Condensation of Th, U, Pu and Cm

NASA Technical Reports Server (NTRS)

Boynton, W. V.

1978-01-01

Reasonable assumptions concerning activity coefficients allow the calculation of the relative volatility of the actinide elements under conditions expected during the early history of the solar system. Several of the light rare earths have volatilities similar to Pu and Cm and can be used as indicators of the degree of fractionation of these extinct elements. Uranium is considerably more volatile than either Pu or Cm, leading to fractionations of about a factor of 50 and 90 in the Pu/U and Cm/U ratio in the earliest condensates from the solar nebula. Ca,Al-rich inclusions from the Allende meteorite, including the coarse-grained inclusions, have a depletion of U relative to La of about a factor of three, suggesting that these inclusions may have been isolated from the nebular gas before condensation of U was complete. The inclusions, however, can be used to determine solar Pu/U and Cm/U ratios if the rare earth patterns are determined in addition to the other normal measurements.

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

Formation of the 50-Year Element 94 from Deuteron Bombardment of U{sup 238}

DOE R&D Accomplishments Database

Kennedy, J. W.; Perlman, M. L.; Segre, E.; Wahl, A. C.

1942-06-01

It has been shown by bombardment with deuterons of a sample of U{sup 238}, greatly depleted in U{sup 235} and U{sup 234}, that the 50-year 94 activity and 2.0 day 93 activity are formed in approximately the same yield as with the natural mixture of uranium isotopes. The activities are thus shown to arise from the U{sup 238} nucleus, and from considerations of the energy of the compound nucleus (U{sup 238} + d).

Prospects for improved understanding of isotopic reactor antineutrino fluxes

NASA Astrophysics Data System (ADS)

Gebre, Y.; Littlejohn, B. R.; Surukuchi, P. T.

2018-01-01

Predictions of antineutrino fluxes produced by fission isotopes in a nuclear reactor have recently received increased scrutiny due to observed differences in predicted and measured inverse beta decay (IBD) yields, referred to as the "reactor antineutrino flux anomaly." In this paper, global fits are applied to existing IBD yield measurements to produce constraints on antineutrino production by individual plutonium and uranium fission isotopes. We find that fits including measurements from highly U 235 -enriched cores and fits including Daya Bay's new fuel evolution result produce discrepant best-fit IBD yields for U 235 and Pu 239 . This discrepancy can be alleviated in a global analysis of all data sets through simultaneous fitting of Pu 239 , U 235 , and U 238 yields. The measured IBD yield of U 238 in this analysis is (7.02 ±1.65 )×10-43 cm2/fission , nearly two standard deviations below existing predictions. Future hypothetical IBD yield measurements by short-baseline reactor experiments are examined to determine their possible impact on the global understanding of isotopic IBD yields. It is found that future improved short-baseline IBD yield measurements at both high-enriched and low-enriched cores can significantly improve constraints for U 235 , U 238 , and Pu 239 , providing comparable or superior precision to existing conversion- and summation-based antineutrino flux predictions. Systematic and experimental requirements for these future measurements are also investigated.

Enhanced nucleon transfer in tip collisions of 238U+124Sn

NASA Astrophysics Data System (ADS)

Sekizawa, Kazuyuki

2017-10-01

Multinucleon transfer processes in low-energy heavy ion reactions have attracted increasing interest in recent years aiming at the production of new neutron-rich isotopes. Clearly, it is an imperative task to further develop understanding of underlying reaction mechanisms to lead experiments to success. In this paper, from systematic time-dependent Hartree-Fock calculations for the 238U+124Sn reaction, it is demonstrated that transfer dynamics depend strongly on the orientations of 238U, quantum shells, and collision energies. Two important conclusions are obtained: (i) Experimentally observed many-proton transfer from 238U to 124Sn can be explained by a multinucleon transfer mechanism governed by enhanced neck evolution in tip collisions; (ii) novel reaction dynamics are observed in tip collisions at energies substantially above the Coulomb barrier, where a number of nucleons are transferred from 124Sn to 238U, producing transuranium nuclei as primary reaction products, which could be a means to synthesize superheavy nuclei. Both results indicate the importance of the neck (shape) evolution dynamics, which are sensitive to orientations, shell effects, and collision energies, for exploring possible pathways to produce new unstable nuclei.

Separation of uranium from (U, Th)O 2 and (U, Pu)O 2 by solid state reactions route

NASA Astrophysics Data System (ADS)

Keskar, Meera; Mudher, K. D. Singh; Venugopal, V.

2005-01-01

Solid state reactions of UO 2, ThO 2, PuO 2 and their mixed oxides (U, Th)O 2 and (U, Pu)O 2 were carried out with sodium nitrate upto 900 °C, to study the formation of various phases at different temperatures, which are amenable for easy dissolution and separation of the actinide elements in dilute acid. Products formed by reacting unsintered as well as sintered UO 2 with NaNO 3 above 500 °C were readily soluble in 2 M HNO 3, whereas ThO 2 and PuO 2 did not react with NaNO 3 to form any soluble products. Thus reactions of mixed oxides (U, Th)O 2 and (U, Pu)O 2 with NaNO 3 were carried out to study the quantitative separation of U from (U, Th)O 2 and (U, Pu)O 2. X-ray diffraction, X-ray fluorescence, thermal analysis and chemical analysis techniques were used for the characterization of the products formed during the reactions.

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.

239Pu(n,γ) from 10 eV to 1.3 MeV

DOE PAGES

Mosby, Shea Morgan; Bredeweg, Todd Allen; Couture, Aaron Joseph; ...

2018-02-01

In this study, the 239Pu(n,γ) cross section has been measured from 10 eV to 1.3 MeV as part of an experimental campaign using the Detector for Advanced Neutron Capture Experiments (DANCE). The work represents a significant advance in experimental technique, with improved systematic uncertainties in key regions in the keV to MeV regime. In general the results of prior work are confirmed with improved uncertainties, particularly at the highest incident neutron energies.

Accelerate the transition of radioisotopes and unwanted weapons-grade ^239Pu into stable nuclei with a system of high frequency modulation for a net energy gain

NASA Astrophysics Data System (ADS)

Pamfiloff, Eugene

2006-10-01

A process of high frequency stimulation of nucleons can be utilized for the accelerated fission, decay or controlled transition of unstable isotopes. ^238U could be persuaded to transition promptly into the stable ^206Pb isotope, where a portion of the total mass difference of 29873.802 MeV per nucleus becomes available energy. The proposals of this paper describe an effective system for nuclei stimulation configured to accelerate such a series of 14 transitions over several milliseconds, instead of 4.47 x 10^9 years. Positive ions or ionized capsules of fuel suspended by magnetic fields and subjected to the system of correlated frequency modulation of multiple beam lines, tailored to the specific target, will emit sufficient energy to stimulate subsequent targets. The system can be applied to all radioisotopes, nuclear waste product isotopes such as ^239Pu, and a variety of other suitable unstable or stable nuclei. Through the proposed confinement system and application of high frequency stimulation in the 10^22 to 10^24 Hz regime, the change in mass can be applied to both the fragmentation of subsequent, periodically injected targets, and the production of heat, making a continuous supply of energy possible. The system allows the particle fragmentation process to be brought into the lab and provides potential solutions to the safe disposal of fissile material.

Accelerate the transition of radioisotopes or unwanted weapons-grade ^239Pu into stable nuclei with a system of high frequency modulation for a net energy gain

NASA Astrophysics Data System (ADS)

Pamfiloff, Eugene

2006-10-01

A process of high frequency stimulation of nucleons can be utilized for the accelerated fission, decay or controlled transition of unstable isotopes. For example ^238U could be persuaded to transition promptly into ^206Pb, where portions of the total mass difference of 29873.802 MeV per nucleus becomes available energy. The proposals of this paper describe an effective system for nuclei stimulation configured to accelerate such a series of 14 transitions over several milliseconds, instead of 4.47 x 10^9 years. Positive ions or ionized capsules of fuel suspended by magnetic fields and subjected to the system of correlated frequency modulation of multiple beam lines, tailored to the specific target, will emit sufficient energy to stimulate subsequent targets. The system can be applied to all radioisotopes, including ^232Th, nuclear waste product isotopes such as ^239Pu, and a variety of other suitable unstable or stable nuclei. Through the proposed confinement system and application of high frequency stimulation in the 10^22 to 10^24 Hz regime, the change in rest mass can be applied to both the fragmentation of subsequent, periodically injected targets, and the production of heat, making a continuous supply of energy possible. The system allows the particle fragmentation process to be brought into the laboratory and provides potential solutions to the safe disposal of fissile material.

Accelerate the transition of radioisotopes and unwanted weapons-grade ^239Pu into stable nuclei with a system of high frequency modulation for a net energy gain

NASA Astrophysics Data System (ADS)

Pamfiloff, Eugene

2006-11-01

A process of high frequency stimulation of nucleons can be utilized for the accelerated fission, decay or controlled transition of unstable isotopes. ^238U could be persuaded to transition promptly into the stable ^206Pb isotope, where a portion of the total mass difference of 29873.802 MeV per nucleus becomes available energy. The proposals of this paper describe an effective system for nuclei stimulation configured to accelerate such a series of 14 transitions over several milliseconds, instead of 4.47 x 10^9 years. Positive ions or ionized capsules of fuel suspended by magnetic fields and subjected to the system of correlated frequency modulation of multiple beam lines, tailored to the specific target, will emit sufficient energy to stimulate subsequent targets. The system can be applied to all radioisotopes, nuclear waste product isotopes such as ^239Pu, and a variety of other suitable unstable or stable nuclei. Through the proposed confinement system and application of high frequency stimulation in the 10^22 to 10^24 Hz regime, the change in mass can be applied to both the fragmentation of subsequent, periodically injected targets, and the production of heat, making a continuous supply of energy possible. The system allows the particle fragmentation process to be brought into the lab and provides potential solutions to the safe disposal of fissile material.

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.

A rapid and accurate method for the determination of plutonium in food using magnetic sector ICP-MS with an ultra-sonic nebuliser and ion chromatography.

PubMed

Evans, P; Elahi, S; Lee, K; Fairman, B

2003-02-01

In the event of a nuclear incident it is essential that analytical information on the distribution and level of contamination is available. An ICP-MS method is described which can provide data on plutonium contamination in food within 3 h of sample receipt without compromising detection limits or accuracy relative to traditional counting methods. The method can also provide simultaneous determinations of americium and neptunium. Samples were prepared by HNO3 closed-vessel microwave digestion, evaporated to dryness and diluted into a mobile phase comprising 1.5 M HNO3 and 0.1 mM 2,6-pyridinedicarboxylic acid. A commercially available polystyrene-divinylbenzene ion chromatography column provides on-line separation of 239Pu and 238U reducing the impact of the 238U1H interference. Oxidation of the sample using H2O2 ensures all Pu is in the Pu(+4) state. The oxidation also displaces Np away from the solvent front by changing the oxidation state from Np(+3) to Np(+4) and produces the insoluble Am(+4) ion. Simultaneous Pu, Am and Np analyses therefore require omission of the oxidation stage and some loss of Pu data quality. Analyses were performed using a magnetic sector ICP-MS (Finnigan MAT Element). The sample is introduced to the plasma via an ultrasonic nebuliser-desolvation unit (Cetac USN 6000AT+). This combination achieves an instrumental sensitivity of 238U > 2 x 10(7) cps/ppb and removes hydrogen from the sample gas, which also inhibits the formation of 238U1H. The net effect of the improved sample introduction conditions is to achieve detection levels for Pu of 0.020 pg g(-1) (4.6 x 10(-2) Bq kg(-1)) which is significantly below 1/10th of the most stringent EU (European Union) legislation, currently 0.436 pg g(-1) (1 Bq kg(-1)) set for baby food. The new method was evaluated with a range of biological samples ranging from cabbage to milk and meat. Recovery of Pu agrees with published values (100% +/- 20%).

Laboratory studies of the diagenesis and mobility of 239,240pu and 137Cs in nearshore sediments

NASA Astrophysics Data System (ADS)

Sholkovitz, Edward R.; Cochran, J. Kirk; Carey, Anne E.

1983-08-01

Controlled laboratory experiments have been used to study the diagenetic chemistry of 239,240Pu 137Cs, and 55Fe. Experiments using Buzzards Bay sediments in small tanks show that sulfate reduction is accompanied by the production of large pore water concentration gradients of alkalinity, phosphate, ammonia and dissolved organic carbon and the formation of subsurface maxima in Fe and Mn. These pore water profiles demonstrate that bacterially-mediated processes of organic matter degradation and redox reactions can be simulated in the laboratory. A vertical profile of 55Fe in pore waters is reported for the first time: it follows the profile of stable Fe and as such has a large (200 dpm/100 kg) subsurface maximum between 2-4 cm depth. Comparison of 55Fe/Fe ratios in sediments and pore waters shows that there is preferential solubilization of 55Fe over stable Fe. The pore water activities of 239,240Pu show no gradients within the large uncertainties of the counting statistics, but are two to four times higher than Buzzards Bay seawater (0.05 dpm/100 kg). The activity of 137Cs in the pore water profile is constant (40 dpm/100 kg) within the large counting uncertainties and is twice that of Buzzards Bay seawater. Cs-137 does not appear to be involved in diagenetic chemistry but may increase in pore waters as a result of ion exchange reactions. Flux estimates based on the pore water data show that remobilization and transport of 239,240 Pu in coastal sediments are not significant processes while the transport of l37Cs may be.

Pu-239 organ specific dosimetric model applied to non-human biota

NASA Astrophysics Data System (ADS)

Kaspar, Matthew Jason

There are few locations throughout the world, like the Maralinga nuclear test site located in south western Australia, where sufficient plutonium contaminate concentration levels exist that they can be utilized for studies of the long-term radionuclide accumulation in non-human biota. The information obtained will be useful for the potential human users of the site while also keeping with international efforts to better understand doses to non-human biota. In particular, this study focuses primarily on a rabbit sample set collected from the population located within the site. Our approach is intended to employ the same dose and dose rate methods selected by the International Commission on Radiological Protection and adapted by the scientific community for similar research questions. These models rely on a series of simplifying assumptions on biota and their geometry; in particular; organisms are treated as spherical and ellipsoidal representations displaying the animal mass and volume. These simplifications assume homogeneity of all animal tissues. In collaborative efforts between Colorado State University and the Australian Nuclear Science and Technology Organisation (ANSTO), we are expanding current knowledge on radionuclide accumulation in specific organs causing organ-specific dose rates, such as Pu-239 accumulating in bone, liver, and lungs. Organ-specific dose models have been developed for humans; however, little has been developed for the dose assessment to biota, in particular rabbits. This study will determine if it is scientifically valid to use standard software, in particular ERICA Tool, as a means to determine organ-specific dosimetry due to Pu-239 accumulation in organs. ERICA Tool is normally applied to whole organisms as a means to determine radiological risk to whole ecosystems. We will focus on the aquatic model within ERICA Tool, as animal organs, like aquatic organisms, can be assumed to lie within an infinite uniform medium. This model would

A DFT+U study of Pu immobilization in Gd2Zr2O7

NASA Astrophysics Data System (ADS)

Zhao, F. A.; Xiao, H. Y.; Jiang, M.; Liu, Z. J.; Zu, X. T.

2015-12-01

The solubility of Pu in Gd2Zr2O7 has been investigated by the density functional theory plus Hubbard U correction. It is found that the formation of PuGdZr2O7, Gd2PuZrO7 and Gd2Pu1.5Zr0.5O7 are exothermic, whereas Pu0.5Gd1.5Zr2O7, Pu1.5Gd0.5Zr2O7 and Gd2Pu0.5Zr1.5O7 are energetically less stable than their respective separated states. The calculations show that both the Gd and Zr lattice sites can be substituted by the Pu, which is consistent with the immobilization behavior of uranium in Gd2Zr2O7 observed experimentally. The site preference of Pu in Gd2Zr2O7 is found to be dependent on the chemical environment, i.e., Pu prefers to substitute for Gd-site under Gd-rich and O2-rich conditions and for Zr-site under Zr-rich and O2-rich conditions.

Effect of chemical pollution on forms of 137Cs, 90Sr and 239,240Pu in arctic soil studied by sequential extraction.

PubMed

Puhakainen, M; Riekkinen, I; Heikkinen, T; Jaakkola, T; Steinnes, E; Rissanen, K; Suomela, M; Thørring, H

2001-01-01

The aim of the present study was to determine the forms of 137Cs, 90Sr and 239,240Pu occurring in different soil horizons using sequential extraction of samples taken from four sites located along a pollution gradient from the copper-nickel smelter at Monchegorsk in the Kola Peninsula, Russia, and from a reference site in Finnish Lapland in 1997. A selective sequential-leaching procedure was employed using a modification of the method of Tessier, Cambell and Bisson ((1979). Analytical Chemistry, 51, 844-851). For 137Cs the organic (O) and uppermost mineral (E1) layer were studied, for 90Sr and 239,240Pu only the uppermost organic layer (Of). The fraction of 137Cs occurring in readily exchangeable form in the organic layer was about 50% at the reference site and decreased as a function of pollution, being 15% at the most polluted site in the Kola Peninsula. There was a clear positive correlation in the O layer between the distance from the smelter and the percentage of 137Cs extracted in the readily exchangeable fraction (Spearman correlation rsp = 0.7805, p = 0.0001), whereas in the E1 layer no correlation was evident. The distribution of 90Sr in the Of layer was similar at all sites, with the highest amounts occurring in exchangeable form and bound to organic matter, whereas stable Sr showed a somewhat different distribution with the highest amount in the oxide fraction. Most of the 239,240Pu was bound to organic matter. Chemical pollution affected the exchangeable fraction of 239,240Pu, which was about 1% at the most polluted site and 4-6% at the other sites.

Almost twenty years' search of transuranium isotopes in effluents discharged to air from nuclear power plants with VVER reactors.

PubMed

Hölgye, Z; Filgas, R

2006-04-01

Airborne effluents of 5 stacks (stacks 1-5) of three nuclear power plants, with 9 pressurized water reactors VVER of 4,520 MWe total power, were searched for transuranium isotopes in different time periods. The search started in 1985. The subject of this work is a presentation of discharge data for the period of 1998-2003 and a final evaluation. It was found that 238Pu, 239,240Pu, 241Am, 242Cm, and 244Cm can be present in airborne effluents. Transuranium isotope contents in most of the quarterly effluent samples from stacks 2, 4 and 5 were not measurable. Transuranium isotopes were present in the effluents from stack l during all 9 years of the study and from stack 3 since the 3rd quarter of 1996 as a result of a defect in the fuel cladding. A relatively high increase of transuranium isotopes in effluents from stack 3 occurred in the 3rd quarter of 1999, and a smaller increase occurred in the 3rd quarter of 2003. In each instance 242Cm prevailed in the transuranium isotope mixtures. 238Pu/239,240Pu, 241Am/239,240Pu, 242Cm/239,240Pu, and 244Cm/239,240Pu ratios in fuel for different burn-up were calculated, and comparison of these ratios in fuel and effluents was performed.

Group Constants Generation of the Pseudo Fission Products for Fast Reactor Burnup Calculations

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

Gil, Choong-Sup; Kim, Do Heon; Chang, Jonghwa

The pseudo fission products for the burnup calculations of the liquid metal fast reactor were generated. The cross-section data and fission product yield data of ENDF/B-VI were used for the pseudo fission product data of U-235, U-238, Pu-239, Pu-240, Pu-241, and Pu-242. The pseudo fission product data can be used with the KAFAX-F22 or -E66, which are the MATXS-format libraries for analyses of the liquid metal fast reactor at KAERI and were distributed through the OECD/NEA. The 80-group MATXS-format libraries of the 172 fission products were generated and the burnup chains for generation of the pseudo fission products were prepared.

Bone cancer occurrence among beagles given 239Pu as young adults.

PubMed

Lloyd, R D; Taylor, G N; Angus, W; Bruenger, F W; Miller, S C

1993-01-01

The occurrence of skeletal malignancies has been documented among 234 young adult beagles given single intravenous injections of monomeric 239Pu citrate. Occurrence has also been documented among 132 comparable control group animals surviving the minimum latent time period of 2.79 y for radiation-induced bone cancer, who were maintained for lifespan observation. Injected amounts ranged from about 0.02-106 kBq kg-1 body mass with factors of 2 or 3 between dose levels. There were 84 radiographically apparent bone tumors in 76 plutonium-injected dogs and one tumor in a control group dog. Most of these were osteosarcomas except for seven chondrosarcomas, one liposarcoma, and one plasma cell myeloma of bone. The relationship between percent of dogs at any dose level with bone malignancy and average skeletal dose at the presumed time of tumor initiation of 1 y before death appeared to be linear below about 1.3 Gy average skeletal dose. The observed data can be approximated by the expression A = 0.76 + 75 D, where A = percent of dogs with bone cancer at any dose level, D = average skeletal dose in Gy (for doses up to 1.3 Gy) at tumor initiation, and 0.76 represents the percent tumor response in the control animals not given plutonium. Similar analysis of our corresponding data for beagles given 226Ra, excluding the two highest dose levels (approximately 100% occurrence), yielded the expression A = 0.76 + 4.7 D, where D = the average skeletal dose in Gy (for doses up to 20 Gy) at 1 y before death. The ratio of coefficients indicates the effectiveness for bone cancer induction of 239Pu relative to 226Ra, or [(75 +/- 22.5)(4.7 +/- 0.47)-1] = 16 +/- 5 for a single, brief intake of either nuclide into blood.

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

Estimates of amounts of soil removal for clean-up of transuranics at NAEG offsite safety-shot sites

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

Kinnison, R.R.; Gilbert, R.O.

Rough estimates are given for the amount of soil removal necessary to decontaminate five representative safety-shot areas. In order to decontaminate to levels of less than 160 pCi /sup 239/Pu per gram of surface soil, it is estimated that over one-half million tons of soil would have to be removed from the five areas. This is a preliminary estimate based on summary data and concentration contour maps readily available in NAEG publications. More accurate estimates could be obtained by applying Kriging techniques to available soil data if the need arises. The inclusion of /sup 241/Am and /sup 238/Pu activities domore » not significantly increase the soil tonnage estimates obtained for /sup 239/ /sup 240/Pu because of their relatively small contributions to total transuranic activity. The magnitude of the errors inherent in our use of summary data to obtain rough estimates also suggests that a revision of the tonnage estimates for /sup 239/ /sup 240/Pu to include /sup 241/Am and /sup 238/Pu is not warranted.« less

Pu isotopes in the western North Pacific Ocean before the accident at Fukushima Dai-ichi Nuclear Power Station

NASA Astrophysics Data System (ADS)

Yamada, M.; Zheng, J.; Aono, T.

2011-12-01

Anthropogenic radionuclides such as Pu-239 (half-life: 24100 yr), Pu-240 (half-life: 6560 yr) and Pu-241 (half-life: 14.325 yr) mainly have been released into the environment as the result of atmospheric nuclear weapons testing. In the North Pacific Ocean, two distinct sources of Pu isotopes can be identified; i.e., the global stratospheric fallout and close-in tropospheric fallout from nuclear weapons testing at the Pacific Proving Grounds in the Marshall Islands. The atom ratio of Pu-240/Pu-239 is a powerful fingerprint to identify the sources of Pu in the ocean. The Pu-240/Pu-239 atom ratios in seawater and marine sediment samples collected in the western North Pacific before the accident at Fukushima Dai-ichi Nuclear Power Station will provide useful background data for understanding the process controlling Pu transport and for distinguishing future Pu sources. The atom ratios of Pu-240/Pu-239 in water columns from the Yamato and Tsushima Basins in the Japan Sea were significantly higher than the mean global fallout ratio of 0.18; however, there were no temporal variation of atom ratios during the period from 1984 to 1993 in the Japan Sea. The total Pu-239+240 inventories in the whole water columns were approximately doubled during the period from 1984 to 1993 in the two basins. The atom ratio of Pu-240/Pu-239 in surface water from Sagami Bay, western North Pacific Ocean, was 0.224 and showed no notable variation from the surface to the bottom with the mean atom ratio being 0.234. The atom ratios for the Pacific coast, near the Rokkasho nuclear fuel reprocessing plant, were approximately the same as the 0.224 ratio obtained from Sagami Bay, western North Pacific margin. The atom ratios in the surficial sediments from Sagami Bay ranged from 0.229 to 0.247. The mean atom ratio in the sediment columns in the East China Sea ranged from 0.248 for the Changjiang estuary to 0.268 for the shelf edge. The observed atom ratios were significantly higher than the mean

Neutron-induced fission cross section of 240Pu from 0.5 MeV to 3 MeV

NASA Astrophysics Data System (ADS)

Salvador-Castiñeira, P.; Bryś, T.; Eykens, R.; Hambsch, F.-J.; Göök, A.; Moens, A.; Oberstedt, S.; Sibbens, G.; Vanleeuw, D.; Vidali, M.; Pretel, C.

2015-07-01

240Pu has recently been pointed out by a sensitivity study of the Organization for Economic Cooperation and Development (OECD) Nuclear Energy Agency (NEA) to be one of the isotopes whose fission cross section lacks accuracy to meet the upcoming needs for the future generation of nuclear power plants (GEN-IV). In the High Priority Request List (HPRL) of the OECD, it is suggested that the knowledge of the 240Pu(n ,f ) cross section should be improved to an accuracy within 1-3 %, compared to the present 5%. A measurement of the 240Pu cross section has been performed at the Van de Graaff accelerator of the Joint Research Center (JRC) Institute for Reference Materials and Measurements (IRMM) using quasi-monoenergetic neutrons in the energy range from 0.5 MeV to 3 MeV. A twin Frisch-grid ionization chamber (TFGIC) has been used in a back-to-back configuration as fission fragment detector. The 240Pu(n ,f ) cross section has been normalized to three different isotopes: 237Np(n ,f ) , 235U (n ,f ) , and 238U (n ,f ) . Additionally, the secondary standard reactions were benchmarked through measurements against the primary standard reaction 235U (n ,f ) in the same geometry. A comprehensive study of the corrections applied to the data and the associated uncertainties is given. The results obtained are in agreement with previous experimental data at the threshold region. For neutron energies higher than 1 MeV, the results of this experiment are slightly lower than the ENDF/B-VII.1 evaluation, but in agreement with the experiments of Laptev et al. (2004) as well as Staples and Morley (1998).

Radioactivity in trinitite six decades later.

PubMed

Parekh, Pravin P; Semkow, Thomas M; Torres, Miguel A; Haines, Douglas K; Cooper, Joseph M; Rosenberg, Peter M; Kitto, Michael E

2006-01-01

The first nuclear explosion test, named the Trinity test, was conducted on July 16, 1945 near Alamogordo, New Mexico. In the tremendous heat of the explosion, the radioactive debris fused with the local soil into a glassy material named Trinitite. Selected Trinitite samples from ground zero (GZ) of the test site were investigated in detail for radioactivity. The techniques used included alpha spectrometry, high-efficiency gamma-ray spectrometry, and low-background beta counting, following the radiochemistry for selected radionuclides. Specific activities were determined for fission products (90Sr, 137Cs), activation products (60Co, 133Ba, 152Eu, 154Eu, 238Pu, 241Pu), and the remnants of the nuclear fuel (239Pu, 240Pu). Additionally, specific activities of three natural radionuclides (40K, 232Th, 238U) and their progeny were measured. The determined specific activities of radionuclides and their relationships are interpreted in the context of the fission process, chemical behavior of the elements, as well as the nuclear explosion phenomenology.

234U/238U evidence for local recharge and patterns of groundwater flow in the vicinity of Yucca Mountain, Nevada, USA

USGS Publications Warehouse

Paces, J.B.; Ludwig, K. R.; Peterman, Z.E.; Neymark, L.A.

2002-01-01

Uranium concentrations and 234U/238U ratios in saturated-zone and perched ground water were used to investigate hydrologic flow and downgradient dilution and dispersion in the vicinity of Yucca Mountain, a potential high-level radioactive waste disposal site. The U data were obtained by thermal ionization mass spectrometry on more than 280 samples from the Death Valley regional flow system. Large variations in both U concentrations (commonly 0.6-10 ??g 1-1) and 234U/238U activity ratios (commonly 1.5-6) are present on both local and regional scales; however, ground water with 234U/238U activity ratios from 7 up to 8.06 is restricted largely to samples from Yucca Mountain. Data from ground water in the Tertiary volcanic and Quaternary alluvial aquifers at and adjacent to Yucca Mountain plot in 3 distinct fields of reciprocal U concentration versus 234U/238U activity ratio correlated to different geographic areas. Ground water to the west of Yucca Mountain has large U concentrations and moderate 234U/238U whereas ground water to the east in the Fortymile flow system has similar 234U/238U, but distinctly smaller U concentrations. Ground water beneath the central part of Yucca Mountain has intermediate U concentrations but distinctive 234U/238U activity ratios of about 7-8. Perched water from the lower part of the unsaturated zone at Yucca Mountain has similarly large values of 234U/238U. These U data imply that the Tertiary volcanic aquifer beneath the central part of Yucca Mountain is isolated from north-south regional flow. The similarity of 234U/238U in both saturated- and unsaturated-zone ground water at Yucca Mountain further indicates that saturated-zone ground water beneath Yucca Mountain is dominated by local recharge rather than regional flow. The distinctive 234U/238U signatures also provide a natural tracer of downgradient flow. Elevated 234U/238U in ground water from two water-supply wells east of Yucca Mountain are interpreted as the result of induced

Elastic moduli of δ-Pu 239 reveal aging in real time

DOE PAGES

Maiorov, Boris; Betts, Jonathan B.; Söderlind, Per; ...

2017-03-28

We study the time evolution (aging) of the elastic moduli of an eight-year-old polycrystalline δ- Pu 2.0 at % Ga alloy (δ-Pu:Ga ) from 295K to nearly 500K in real time using Resonant Ultrasound Spectroscopy (RUS). After 8 years of aging at 295K, the bulk and shear moduli increase at a normalized rate of 0.2%/year and 0.6%/year respectively. As the temperature is raised, two time dependences are observed, an exponential one of about a week, followed by a linear one (constant rate). The linear rate is thermally activated with an activation energy of 0.33+0.06 eV. Above 420K a qualitative changemore » in the time evolution is observed; the bulk modulus decreases with time while the shear modulus continues to stiffen. No change is observed as the α-β transition temperature is crossed as would be expected if a decomposition of δ-Pu:Ga to α-Pu and Pu 3Ga occurred over the temperature range studied. Our results indicate that the main mechanism of aging is creation of defects that are partially annealed starting at T = 420 K.« less

Elastic moduli of δ-Pu 239 reveal aging in real time

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

Maiorov, Boris; Betts, Jonathan B.; Söderlind, Per

We study the time evolution (aging) of the elastic moduli of an eight-year-old polycrystalline δ- Pu 2.0 at % Ga alloy (δ-Pu:Ga ) from 295K to nearly 500K in real time using Resonant Ultrasound Spectroscopy (RUS). After 8 years of aging at 295K, the bulk and shear moduli increase at a normalized rate of 0.2%/year and 0.6%/year respectively. As the temperature is raised, two time dependences are observed, an exponential one of about a week, followed by a linear one (constant rate). The linear rate is thermally activated with an activation energy of 0.33+0.06 eV. Above 420K a qualitative changemore » in the time evolution is observed; the bulk modulus decreases with time while the shear modulus continues to stiffen. No change is observed as the α-β transition temperature is crossed as would be expected if a decomposition of δ-Pu:Ga to α-Pu and Pu 3Ga occurred over the temperature range studied. Our results indicate that the main mechanism of aging is creation of defects that are partially annealed starting at T = 420 K.« less

Internal dose assessment of 238U contaminated soils based on in-vitro gastrointestinal protocol

NASA Astrophysics Data System (ADS)

Perama, Yasmin Mohd Idris; Rashid, Nur Shahidah Abdul; Majid, Amran Ab.; Siong, Khoo Kok

2017-01-01

Human exposure to natural radioactive uranium has been a great interest as more industrial rapidly growing contributes to radiation risks. The aim of this case study was to determine the internal dose in humans incorporated with ingestion of 238U contaminated soils. A gastrointestinal analogue test was employed to simulate the human digestive tract. In-vitro approach via German DIN 19738 model was developed in order to estimate the internal exposure of 238U due to ingestion of different types of soils. Synthetic gastrointestinal fluids assay via in-vitro method were produced to determine the concentration of 238U in various soils using ICP-MS. Based on the results, concentration of 238U in BRIS, laterite, peat and alluvium soils were in ranged between (0.0061 ± 0.0057 - 0.0488 ± 0.0148) ppm and (0.0005 ± 0.0004 - 0.0046 ± 0.0007) ppm in gastric and gastrointestinal phase respectively. Types of soil compositions and pH medium were some of the factors that influence mobilization and solubility of 238U contaminanted soil into the digestive juices that resembles human gastrointestinal tract. For the purpose of internal dose assessment, the committed efective dose from 238U intake in soils ranged between 1.237 × 10-11 - 9.8993 × 10-11 Sv y-1 for gastric phase and 1.0184 × 10-12 - 9.3294 × 10-12 Sv y-1 for gastric-intestinal phase. The internal dose measurements from this study were much lower from the recommended values. Hence, ingestion of 238U contaminated soils would not be expected to pose major health risk to humans.

Hypoadrenocorticism in beagles exposed to aerosols of plutonium-238 dioxide by inhalation

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

Weller, R.E.; Buschbom, R.L.; Dagle, G.E.

1996-12-01

Hypoadrenocorticism, known as Addison`s disease in humans, was diagnosed in six beagles after inhalation of at least 1.7 kBq/g lung of {sup 238}PuO{sub 2}. Histological examination of adrenal gland specimens obtained at necropsy revealed marked adrenal cortical atrophy in all cases. Autoadiographs showed only slight {alpha}-particle activity. Although the pathogenesis of adrenal cortical atrophy in these dogs is unclear, there is evidence to suggest an automimmune disorder linked to damage resulting from {alpha}-particle irradiation to the lymphatic system.

Ultra-Sensitive Elemental Analysis Using Plasmas 4.Application of Inductively Coupled Plasma Mass Spectrometry to the Study of Environmental Radioactivity

NASA Astrophysics Data System (ADS)

Yoshida, Satoshi

Applications of inductively coupled plasma mass spectrometry (ICP-MS) to the determination of long-lived radionuclides in environmental samples were summarized. In order to predict the long-term behavior of the radionuclides, related stable elements were also determined. Compared with radioactivity measurements, the ICP-MS method has advantages in terms of its simple analytical procedures, prompt measurement time, and capability of determining the isotope ratio such as240Pu/239Pu, which can not be separated by radiation. Concentration of U and Th in Japanese surface soils were determined in order to determine the background level of the natural radionuclides. The 235U/238U ratio was successfully used to detect the release of enriched U from reconversion facilities to the environment and to understand the source term. The 240Pu/239Pu ratios in environmental samples varied widely depending on the Pu sources. Applications of ICP-MS to the measurement of I and Tc isotopes were also described. The ratio between radiocesium and stable Cs is useful for judging the equilibrium of deposited radiocesium in a forest ecosystem.

238U and 235U isotope fractionation upon oxidation of uranium-bearing rocks by fracture waters

NASA Astrophysics Data System (ADS)

Chernyshev, I. V.; Golubev, V. N.; Chugaev, A. V.; Mandzhieva, G. V.

2016-10-01

The variations in 238U/235U values accompanying mobilization of U by fracture waters from uranium-bearing rocks, in which U occurs as a fine impregnation of oxides and silicates, were studied by the high-precision (±0.07‰) MC-ICP-MS method. Transition of U into the aqueous phase in the oxidized state U(VI) is accompanied by its isotope fractionation with enrichment of dissolved U(VI) in the heavy isotope 238U up to 0.32‰ in relation to the composition of the solid phases. According to the sign, this effect is consistent with the tendency of the behavior of 238U and 235U upon interaction of river waters with rocks of the catchment areas [11] and with the effect observed during oxidation of uraninite by the oxygen-bearing NaHCO3 solution [12].

Determination of 90Sr and Pu isotopes in contaminated groundwater samples by inductively coupled plasma mass spectrometry

NASA Astrophysics Data System (ADS)

Zoriy, Miroslav V.; Ostapczuk, Peter; Halicz, Ludwik; Hille, Ralf; Becker, J. Sabine

2005-04-01

A sensitive analytical method for determining the artificial radionuclides 90Sr, 239Pu and 240Pu at the ultratrace level in groundwater samples from the Semipalatinsk Test Site area in Kazakhstan by double-focusing sector field inductively coupled plasma mass spectrometry (ICP-SFMS) was developed. In order to avoid possible isobaric interferences at m/z 90 for 90Sr determination (e.g. 90Zr+, 40Ar50Cr+, 36Ar54Fe+, 58Ni16O2+, 180Hf2+, etc.), the measurements were performed at medium mass resolution under cold plasma conditions. Pu was separated from uranium by means of extraction chromatography using Eichrom TEVA resin with a recovery of 83%. The limits of detection for 90Sr, 239Pu and 240Pu in water samples were determined as 11, 0.12 and 0.1 fg ml-1, respectively. Concentrations of 90Sr and 239Pu in contaminated groundwater samples ranged from 18 to 32 and from 28 to 856 fg ml-1, respectively. The 240Pu/239Pu isotopic ratio in groundwater samples was measured as 0.17. This isotope ratio indicates that the most probable source of contamination of the investigated groundwater samples was the nuclear weapons tests at the Semipalatinsk Test Site conducted by the USSR in the 1960s.

Biodegradation of PuEDTA and Impacts on Pu Mobility

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

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

The contamination of many DOE sites by Pu presents a long-term problem because of its long half-life (240,000 yrs) and the low drinking water standard (<10{sup -12} M). EDTA was co-disposed with radionuclides (e.g., Pu, {sup 60}Co), formed strong complexes, and enhanced radionuclide transport at several DOE sites. Biodegradation of EDTA should decrease Pu mobility. One objective of this project was to determine the biodegradation of EDTA in the presence of PuEDTA complexes. The aqueous system investigated at pH 7 (10{sup -4} M EDTA and 10{sup -6} M Pu) contained predominantly Pu(OH){sub 2}EDTA{sup 2-}. The EDTA was degraded at amore » faster rate in the presence of Pu. As the total concentration of both EDTA and PuEDTA decreased (i.e., 10{sup -5} M EDTA and 10{sup -7} M PuEDTA), the presence of Pu decreased the biodegradation rate of the EDTA. It is currently unclear why the concentration of Pu directly affects the increase/decrease in rate of EDTA biodegradation. The soluble Pu concentration decreased, in agreement with thermodynamic predictions, as the EDTA was biodegraded, indicating that biodegradation of EDTA will decrease Pu mobility when the Pu is initially present as Pu(IV)EDTA. A second objective was to investigate how the presence of competing metals, commonly encountered in geologic media, will influence the speciation and biodegradation of Pu(IV)-EDTA. Studies on the solubilities of Fe(OH){sub 3}(s) and of Fe(OH){sub 3}(s) plus PuO{sub 2}(am) in the presence of EDTA and as a function of pH showed that Fe(III) out competes the Pu(IV) for the EDTA complex, thereby showing that Pu(IV) will not form stable complexes with EDTA for enhanced transport of Pu in Fe(III) dominated subsurface systems. A third objective is to investigate the genes and enzymes involved in EDTA biodegradation. BNC1 can use EDTA and another synthetic chelating agent nitrilotriacetate (NTA) as sole carbon and nitrogen sources. The same catabolic enzymes are responsible for both EDTA

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.

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

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

Shunji Homma; Jun-ichi Ishii; Jiro Koga

2006-07-01

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

Absolute measurement of the 242Pu neutron-capture cross section

DOE PAGES

Buckner, M. Q.; Wu, C. Y.; Henderson, R. A.; ...

2016-04-21

Here, the absolute neutron-capture cross section of 242Pu was measured at the Los Alamos Neutron Science Center using the Detector for Advanced Neutron-Capture Experiments array along with a compact parallel-plate avalanche counter for fission-fragment detection. The first direct measurement of the 242Pu(n,γ) cross section was made over the incident neutron energy range from thermal to ≈ 6 keV, and the absolute scale of the (n,γ) cross section was set according to the known 239Pu(n,f) resonance at E n,R = 7.83 eV. This was accomplished by adding a small quantity of 239Pu to the 242Pu sample. The relative scale of themore » cross section, with a range of four orders of magnitude, was determined for incident neutron energies from thermal to ≈ 40 keV. Our data, in general, are in agreement with previous measurements and those reported in ENDF/B-VII.1; the 242Pu(n,γ) cross section at the E n,R = 2.68 eV resonance is within 2.4% of the evaluated value. However, discrepancies exist at higher energies; our data are ≈30% lower than the evaluated data at E n ≈ 1 keV and are approximately 2σ away from the previous measurement at E n ≈ 20 keV.« less

IAEA CIELO Evaluation of Neutron-induced Reactions on 235U and 238U Targets

DOE PAGES

Capote, R.; Trkov, A.; Sin, M.; ...

2018-02-01

Evaluations of nuclear reaction data for the major uranium isotopes 238U and 235U were performed within the scope of the CIELO Project on the initiative of the OECD/NEA Data Bank under Working Party on Evaluation Co-operation (WPEC) Subgroup 40 coordinated by the IAEA Nuclear Data Section. Both the mean values and covariances are evaluated from 10 -5 eV up to 30 MeV. The resonance parameters of 238U and 235U were re-evaluated with the addition of newly available data to the existing experimental database. The evaluations in the fast neutron range are based on nuclear model calculations with the code EMPIRE–3.2more » Malta above the resonance range up to 30 MeV. 235U(n,f), 238U(n,f), and 238U(n,γ) cross sections and 235U(n th,f) prompt fission neutron spectrum (PFNS) were evaluated within the Neutron Standards project and are representative of the experimental state-of-the-art measurements. The Standards cross sections were matched in model calculations as closely as possible to guarantee a good predictive power for cross sections of competing neutron scattering channels. 235U(n,γ) cross section includes fluctuations observed in recent experiments. 235U(n,f) PFNS for incident neutron energies from 500 keV to 20 MeV were measured at Los Alamos Chi-Nu facility and re-evaluated using all available experimental data. While respecting the measured differential data, several compensating errors in previous evaluations were identified and removed so that the performance in integral benchmarks was restored or improved. Covariance matrices for 235U and 238U cross sections, angular distributions, spectra and neutron multiplicities were evaluated using the GANDR system that combines experimental data with model uncertainties. Unrecognized systematic uncertainties were considered in the uncertainty quantification for fission and capture cross sections above the thermal range, and for neutron multiplicities. Evaluated files were extensively benchmarked to ensure good

IAEA CIELO Evaluation of Neutron-induced Reactions on 235U and 238U Targets

NASA Astrophysics Data System (ADS)

Capote, R.; Trkov, A.; Sin, M.; Pigni, M. T.; Pronyaev, V. G.; Balibrea, J.; Bernard, D.; Cano-Ott, D.; Danon, Y.; Daskalakis, A.; Goričanec, T.; Herman, M. W.; Kiedrowski, B.; Kopecky, S.; Mendoza, E.; Neudecker, D.; Leal, L.; Noguere, G.; Schillebeeckx, P.; Sirakov, I.; Soukhovitskii, E. S.; Stetcu, I.; Talou, P.

2018-02-01

Evaluations of nuclear reaction data for the major uranium isotopes 238U and 235U were performed within the scope of the CIELO Project on the initiative of the OECD/NEA Data Bank under Working Party on Evaluation Co-operation (WPEC) Subgroup 40 coordinated by the IAEA Nuclear Data Section. Both the mean values and covariances are evaluated from 10-5 eV up to 30 MeV. The resonance parameters of 238U and 235U were re-evaluated with the addition of newly available data to the existing experimental database. The evaluations in the fast neutron range are based on nuclear model calculations with the code EMPIRE-3.2 Malta above the resonance range up to 30 MeV. 235U(n,f), 238U(n,f), and 238U(n,γ) cross sections and 235U(nth,f) prompt fission neutron spectrum (PFNS) were evaluated within the Neutron Standards project and are representative of the experimental state-of-the-art measurements. The Standards cross sections were matched in model calculations as closely as possible to guarantee a good predictive power for cross sections of competing neutron scattering channels. 235U(n,γ) cross section includes fluctuations observed in recent experiments. 235U(n,f) PFNS for incident neutron energies from 500 keV to 20 MeV were measured at Los Alamos Chi-Nu facility and re-evaluated using all available experimental data. While respecting the measured differential data, several compensating errors in previous evaluations were identified and removed so that the performance in integral benchmarks was restored or improved. Covariance matrices for 235U and 238U cross sections, angular distributions, spectra and neutron multiplicities were evaluated using the GANDR system that combines experimental data with model uncertainties. Unrecognized systematic uncertainties were considered in the uncertainty quantification for fission and capture cross sections above the thermal range, and for neutron multiplicities. Evaluated files were extensively benchmarked to ensure good performance in

IAEA CIELO Evaluation of Neutron-induced Reactions on 235U and 238U Targets

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

Capote, R.; Trkov, A.; Sin, M.

Evaluations of nuclear reaction data for the major uranium isotopes 238U and 235U were performed within the scope of the CIELO Project on the initiative of the OECD/NEA Data Bank under Working Party on Evaluation Co-operation (WPEC) Subgroup 40 coordinated by the IAEA Nuclear Data Section. Both the mean values and covariances are evaluated from 10 -5 eV up to 30 MeV. The resonance parameters of 238U and 235U were re-evaluated with the addition of newly available data to the existing experimental database. The evaluations in the fast neutron range are based on nuclear model calculations with the code EMPIRE–3.2more » Malta above the resonance range up to 30 MeV. 235U(n,f), 238U(n,f), and 238U(n,γ) cross sections and 235U(n th,f) prompt fission neutron spectrum (PFNS) were evaluated within the Neutron Standards project and are representative of the experimental state-of-the-art measurements. The Standards cross sections were matched in model calculations as closely as possible to guarantee a good predictive power for cross sections of competing neutron scattering channels. 235U(n,γ) cross section includes fluctuations observed in recent experiments. 235U(n,f) PFNS for incident neutron energies from 500 keV to 20 MeV were measured at Los Alamos Chi-Nu facility and re-evaluated using all available experimental data. While respecting the measured differential data, several compensating errors in previous evaluations were identified and removed so that the performance in integral benchmarks was restored or improved. Covariance matrices for 235U and 238U cross sections, angular distributions, spectra and neutron multiplicities were evaluated using the GANDR system that combines experimental data with model uncertainties. Unrecognized systematic uncertainties were considered in the uncertainty quantification for fission and capture cross sections above the thermal range, and for neutron multiplicities. Evaluated files were extensively benchmarked to ensure good

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.

Summary of Plutonium-238 Production Alternatives Analysis Final Report

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

James Werner; Wade E. Bickford; David B. Lord

The Team implemented a two-phase evaluation process. During the first phase, a wide variety of past and new candidate facilities and processing methods were assessed against the criteria established by DOE for this assessment. Any system or system element selected for consideration as an alternative within the project to reestablish domestic production of Pu-238 must meet the following minimum criteria: Any required source material must be readily available in the United States, without requiring the development of reprocessing technologies or investments in systems to separate material from identified sources. It must be cost, schedule, and risk competitive with existing baselinemore » technology. Any identified facilities required to support the concept must be available to the program for the entire project life cycle (notionally 35 years, unless the concept is so novel as to require a shorter duration). It must present a solution that can generate at least 1.5 Kg of Pu-238 oxide per year, for at least 35 years. It must present a low-risk, near-term solution to the National Aeronautics and Space Administration’s urgent mission need. DOE has implemented this requirement by eliminating from project consideration any alternative with key technologies at less than Technology Readiness Level 5. The Team evaluated the options meeting these criteria using a more detailed assessment of the reasonable facility variations and compared them to the preferred option, which consists of target irradiation at the Advanced Test Reactor (ATR) and the High Flux Isotope Reactor (HFIR), target fabrication and chemical separations processing at the ORNL Radiochemical Engineering Development Center, and neptunium 237 storage at the Materials and Fuels Complex at INL. This preferred option is consistent with the Records of Decision from the earlier National Environmental Policy Act (NEPA) documentation« less

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

Simpson, H.J.; Trier, R.M.

We have obtained a large set of sediment cores from the Hudson estuary through much of the ambient salinity range. A number of core sections and samples of suspended particles have been analyzed for /sup 137/Cs, /sup 134/Cs and /sup 60/Co by direct gamma counting, and /sup 239/Pu, /sup 240/Pu, and /sup 238/Pu by alpha spectrometry. The distribution of both /sup 137/Cs and /sup 239/Pu, /sup 240/Pu indicates rapid accumulation in marginal cover areas, and especially in the harbor region adjacent to New York City. The distributions of both /sup 137/Cs and /sup 239/Pu, /sup 240/Pu are similar in surfacemore » sediments and with depth in cores, but there are deviations from the fallout ratio due to addition of reactor /sup 137/Cs and loss of /sup 137/Cs from the particle phases at higher salinities. Measureable amounts of reactor-derived /sup 134/Cs and /sup 60/Co are found in nearly all sediment samples containing appreciable /sup 137/Cs, between 15 km upstream of Indian Point and the downstream extent of our sampling, 70 km south of the reactor. Accumulations of /sup 239/Pu, /sup 240/Pu in New York harbor sediments are more than an order of magnitude greater than the fallout delivery rate. The most likely explanation is accumulation of fine particles in the harbor which have been transported from upstream areas of the Hudson. Our evidence so far indicates that Indian Point is probably not a significant source of /sup 239/Pu, /sup 240/Pu or /sup 238/Pu compared with the fallout burden of these nuclides already in the sediments.« less

High resolution gamma-ray spectrometry of culverts containing transuranic waste at the Savannah River Site

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

Hofstetter, K.J.; Sigg, R.

1990-12-31

A number of concrete culverts used to retrievably store drummed, dry, radioactive waste at the Savannah River Site (SRS), were suspected of containing ambiguous quantities of transuranic (TRU) nuclides. These culverts were assayed in place for Pu-239 content using thermal and fast neutron counting techniques. High resolution gamma-ray spectroscopy on 17 culverts, having neutron emission rates several times higher than expected, showed characteristic gamma-ray signatures of neutron emitters other than Pu-239 (e.g., Pu-238, Pu/Be, or Am/Be neutron sources). This study confirmed the Pu-239 content of the culverts with anomalous neutron rates and established limits on the Pu-239 mass in eachmore » of the 17 suspect culverts by in-field, non-intrusive gamma-ray measurements.« less

High resolution gamma-ray spectrometry of culverts containing transuranic waste at the Savannah River Site

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

Hofstetter, K.J.; Sigg, R.

1990-01-01

A number of concrete culverts used to retrievably store drummed, dry, radioactive waste at the Savannah River Site (SRS), were suspected of containing ambiguous quantities of transuranic (TRU) nuclides. These culverts were assayed in place for Pu-239 content using thermal and fast neutron counting techniques. High resolution gamma-ray spectroscopy on 17 culverts, having neutron emission rates several times higher than expected, showed characteristic gamma-ray signatures of neutron emitters other than Pu-239 (e.g., Pu-238, Pu/Be, or Am/Be neutron sources). This study confirmed the Pu-239 content of the culverts with anomalous neutron rates and established limits on the Pu-239 mass in eachmore » of the 17 suspect culverts by in-field, non-intrusive gamma-ray measurements.« less

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

Exploratory study of fission product yield determination from photofission of Pu 239 at 11 MeV with monoenergetic photons

DOE PAGES

Bhike, Megha; Tornow, W.; Krishichayan, -; ...

2017-02-14

Here, measurements of fission product yields play an important role for the understanding of fundamental aspects of the fission process. Recently, neutron-induced fission product-yield data of  239Pu at energies below 4 MeV revealed an unexpected energy dependence of certain fission fragments. In order to investigate whether this observation is prerogative to neutron-induced fission, a program has been initiated to measure fission product yields in photoinduced fission. Here we report on the first ever photofission product yield measurement with monoenergetic photons produced by Compton back-scattering of FEL photons. The experiment was performed at the High-Intensity Gamma-ray Source at Triangle Universities Nuclear Laboratorymore » on  239Pu at E γ = 11 MeV. In this exploratory study the yield of eight fission products ranging from  91Sr to  143Ce has been obtained.« less

Exploratory study of fission product yield determination from photofission of Pu 239 at 11 MeV with monoenergetic photons

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

Bhike, Megha; Tornow, W.; Krishichayan, -

Here, measurements of fission product yields play an important role for the understanding of fundamental aspects of the fission process. Recently, neutron-induced fission product-yield data of  239Pu at energies below 4 MeV revealed an unexpected energy dependence of certain fission fragments. In order to investigate whether this observation is prerogative to neutron-induced fission, a program has been initiated to measure fission product yields in photoinduced fission. Here we report on the first ever photofission product yield measurement with monoenergetic photons produced by Compton back-scattering of FEL photons. The experiment was performed at the High-Intensity Gamma-ray Source at Triangle Universities Nuclear Laboratorymore » on  239Pu at E γ = 11 MeV. In this exploratory study the yield of eight fission products ranging from  91Sr to  143Ce has been obtained.« 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.

Some questions concerning safety on emergency landing in dense layers of the atmosphere of radionuclide energy sources based on plutonium-238 for autonomous station ``MARS-94/96''

NASA Astrophysics Data System (ADS)

Makhorin, Oleg I.; Pustovalov, Alexey A.; Zhabin, Vladimir N.; Greenberg, Edward I.; Nilolaev, Vadim S.; Sokolov, Nikolay A.

1996-03-01

This paper describes results of investigations of questions concerning integrity keeping for an ampula containing radionuclide fuel (Pu-238) under conditions of emergency landing in dense layers of the atmosphere and under conditions of fire on launching pad.

Melting behavior of mixed U-Pu oxides under oxidizing conditions

NASA Astrophysics Data System (ADS)

Strach, Michal; Manara, Dario; Belin, Renaud C.; Rogez, Jacques

2016-05-01

In order to use mixed U-Pu oxide ceramics in present and future nuclear reactors, their physical and chemical properties need to be well determined. The behavior of stoichiometric (U,Pu)O2 compounds is relatively well understood, but the effects of oxygen stoichiometry on the fuel performance and stability are often still obscure. In the present work, a series of laser melting experiments were carried out to determine the impact of an oxidizing atmosphere, and in consequence the departure from a stoichiometric composition on the melting behavior of six mixed uranium plutonium oxides with Pu content ranging from 14 to 62 wt%. The starting materials were disks cut from sintered stoichiometric pellets. For each composition we have performed two laser melting experiments in pressurized air, each consisting of four shots of different duration and intensity. During the experiments we recorded the temperature at the surface of the sample with a pyrometer. Phase transitions were qualitatively identified with the help of a reflected blue laser. The observed phase transitions occur at a systematically lower temperature, the lower the Pu content of the studied sample. It is consistent with the fact that uranium dioxide is easily oxidized at elevated temperatures, forming chemical species rich in oxygen, which melt at a lower temperature and are more volatile. To our knowledge this campaign is a first attempt to quantitatively determine the effect of O/M on the melting temperature of MOX.

Oxygen potentials, oxygen diffusion coefficients and defect equilibria of nonstoichiometric (U,Pu)O2±x

NASA Astrophysics Data System (ADS)

Kato, Masato; Watanabe, Masashi; Matsumoto, Taku; Hirooka, Shun; Akashi, Masatoshi

2017-04-01

Oxygen potential of (U,Pu)O2±x was evaluated based on defect chemistry using an updated experimental data set. The relationship between oxygen partial pressure and deviation x in (U,Pu)O2±x was analyzed, and equilibrium constants of defect formation were determined as functions of Pu content and temperature. Brouwer's diagrams were constructed using the determined equilibrium constants, and a relational equation to determine O/M ratio was derived as functions of O/M ratio, Pu content and temperature. In addition, relationship between oxygen potential and oxygen diffusion coefficients were described.

Transuranic sealed source recovery project.

PubMed

Tompkins, J A; Pearson, M W

2001-11-01

If you have transuranic sealed sources (239Pu, 238Pu, or 241Am) that have no potential for recycle or commercial disposal, the Off Site Source Recovery Project at LANL can assist in recovering the sealed sources from your facility to a DOE storage site.

Atmospheric fallout radionuclides in peatland from Southern Poland.

PubMed

Mróz, Tomasz; Łokas, Edyta; Kocurek, Justyna; Gąsiorek, Michał

2017-09-01

Two peat profiles were collected in a peat bog located in Southern Poland and their geochronology were determined using 210 Pb, 238,239+240 Pu and 137 Cs radiometric techniques. The 210 Pb chronologies were established using the constant rate of supply model (CRS) and are in good agreement with the Pu isotopes and 137 Cs time markers. Maximum activities of Pu isotopes were found at a depth corresponding to the early 1960s, which is the period characterized by the maximum nuclear weapon tests. The results showed that the 210 Pb method is the most accurate technique for the determination age and accumulation rate of a peat. The next part of this study calculated linear accumulation rates by analyzing 238,239+240 Pu and 137 Cs vertical distributions in the profiles. Activities of fallout isotopes were also measured in plants covering the peatland. The highest activities of 137 Cs and 210 Pb were found in Calluna vulgaris samples, and 239+240 Pu were found only in two samples (C. vulgaris and leaves of Oxycoccus quadripelatus). Copyright © 2017 Elsevier Ltd. All rights reserved.

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.

238U, and its decay products, in grasses from an abandoned uranium mine

NASA Astrophysics Data System (ADS)

Childs, Edgar; Maskall, John; Millward, Geoffrey

2016-04-01

Bioaccumulation of radioactive contaminants by plants is of concern particularly where the sward is an essential part of the diet of ruminants. The abandoned South Terras uranium mine, south west England, had primary deposits of uraninite (UO2) and pitchblende (U3O8), which contained up to 30% uranium. When the mine was active uranium and radium were extracted but following closure it was abandoned without remediation. Waste rock and gangue, consisting of inefficiently processed minerals, were spread around the site, including a field where ruminants are grazed. Here we report the activity concentrations of 238U, 235U 214,210Pb, and the concentrations of selected metals in the soils, roots and leaves of grasses taken from the contaminated field. Soil samples were collected at the surface, and at 30 cm depth, using an auger along a 10-point transect in the field from the foot of a waste heap. Whole, individual grass plants were removed with a spade, ensuring that their roots were intact. The soils and roots and grass leaves were freeze-dried. Activity concentrations of the radionuclides were determined by gamma spectroscopy, following 30 days incubation for development of secular equilibrium. Dried soils, roots and grasses were also digested in aqua regia and the concentrations of elements determined by ICP techniques. Maximum activity concentrations of 238U, 235U, 214Pb and 210Pb surface soils were 63,300, 4,510, 23,300 and 49,400 Bq kg-1, respectively. The mean 238U:235U ratio was 11.8 ± 1.8, an order of magnitude lower than the natural value of 138, indicating disequilibrium within the decay chain due to mineral processing. Radionuclides in the roots had 5 times lower concentration and only grass leaves in the vicinity of the waste heap had measureable values. The mean soil to root transfer factor for 238U was 36%, the mean root to leaf was 3% and overall only 0.7% of 238U was transferred from the soil to the leaves. The roots contained 0.8% iron, possibly as

The self-absorption effect of gamma rays in /sup 239/Pu

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

Hsu, Hsiao-Hua

1989-01-01

Nuclear materials assay with gamma-ray spectrum measurement is a well-established method for safeguards. However, for a thick source, the self-absorption of characteristic low-energy gamma rays has been a handicap to accurate assay. I have carried out Monte Carlo simulations to study this effect using the /sup 239/Pu ..cap alpha..-decay gamma-ray spectrum as an example. The thickness of a plutonium metal source can be considered a function of gamma-ray intensity ratios. In a practical application, gamma-ray intensity ratios can be obtained from a measured spectrum. With the help of calculated curves, scientists can find the source thickness and make corrections tomore » gamma-ray intensities, which then lead to an accurate quantitative determination of radioactive isotopes in the material. 2 refs., 9 figs.« less

Extinct 244Pu in ancient zircons.

PubMed

Turner, Grenville; Harrison, T Mark; Holland, Greg; Mojzsis, Stephen J; Gilmour, Jamie

2004-10-01

We have found evidence, in the form of fissiogenic xenon isotopes, for in situ decay of 244Pu in individual 4.1- to 4.2-billion-year-old zircons from the Jack Hills region of Western Australia. Because of its short half-life, 82 million years, 244Pu was extinct within 600 million years of Earth's formation. Detrital zircons are the only known relics to have survived from this period, and a study of their Pu geochemistry will allow us to date ancient metamorphic events and determine the terrestrial Pu/U ratio for comparison with the solar ratio.

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

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

Marsh, S.F.; Spall, W.D.; Abernathey, R.M.

1976-11-01

Relationships are provided to compute the decreasing plutonium content and changing isotopic distribution of plutonium materials for the radioactive decay of /sup 238/Pu, /sup 239/Pu, /sup 240/Pu and /sup 242/Pu to long-lived uranium daughters and of /sup 241/Pu to /sup 241/Am. This computation is important to the use of plutonium reference materials to calibrate destructive and nondestructive methods for assay and isotopic measurements, as well as to accountability inventory calculations.

Heterogeneous sodium fast reactor designed for transmuting minor actinide waste isotopes into plutonium fuel

NASA Astrophysics Data System (ADS)

Bays, Samuel Eugene

2008-10-01

In the past several years there has been a renewed interest in sodium fast reactor (SFR) technology for the purpose of destroying transuranic waste (TRU) produced by light water reactors (LWR). The utility of SFRs as waste burners is due to the fact that higher neutron energies allow all of the actinides, including the minor actinides (MA), to contribute to fission. It is well understood that many of the design issues of LWR spent nuclear fuel (SNF) disposal in a geologic repository are linked to MAs. Because the probability of fission for essentially all the "non-fissile" MAs is nearly zero at low neutron energies, these isotopes act as a neutron capture sink in most thermal reactor systems. Furthermore, because most of the isotopes produced by these capture reactions are also non-fissile, they too are neutron sinks in most thermal reactor systems. Conversely, with high neutron energies, the MAs can produce neutrons by fast fission. Additionally, capture reactions transmute the MAs into mostly plutonium isotopes, which can fission more readily at any energy. The transmutation of non-fissile into fissile atoms is the premise of the plutonium breeder reactor. In a breeder reactor, not only does the non-fissile "fertile" U-238 atom contribute fast fission neutrons, but also transmutes into fissile Pu-239. The fissile value of the plutonium produced by MA transmutation can only be realized in fast neutron spectra. This is due to the fact that the predominate isotope produced by MA transmutation, Pu-238, is itself not fissile. However, the Pu-238 fission cross section is significantly larger than the original transmutation parent, predominately: Np-237 and Am-241, in the fast energy range. Also, Pu-238's fission cross section and fission-to-capture ratio is almost as high as that of fissile Pu-239 in the fast neutron spectrum. It is also important to note that a neutron absorption in Pu-238, that does not cause fission, will instead produce fissile Pu-239. Given this

Natural and artificial radionuclides in a marine core. First results of 236U in North Atlantic Ocean sediments.

PubMed

Villa-Alfageme, M; Chamizo, E; Santos-Arévalo, F J; López-Gutierrez, J M; Gómez-Martínez, I; Hurtado-Bermúdez, S

2018-06-01

There are very few data available of 236 U in marine sediment cores. In this study we present the results from the first oceanic depth profile of 236 U in a sediment core sampled in the North Atlantic Ocean, at the PAP site (4500 m depth, Porcupine Abyssal Plain (PAP) site, 49°0' N, 16°30' W). Additionally, the sediment core was radiologically characterized through the measurement of anthropogenic 137 Cs, 239 Pu, 240 Pu, 129 I and 14 C and natural 210 Pb, 40 K and 226 Ra. The measured 236 U concentrations decrease from about 90·10 6  at g -1 at the seafloor down to 0.5·10 6  at g -1 at 6 cm depth. They are several orders of magnitude lower than the reported values for soils from the Northern Hemisphere solely influenced by global fallout (i.e. from 2700·10 6 to 7500·10 6  at g -1 ). 236 U/ 238 U atom ratios measured are at least three orders of magnitude above the estimated level for the naturally occurring dissolved uranium. The obtained inventories are 1·10 12  at m -2 for 236 U, 80 Bq m -2 for 137 Cs, 45 Bq m -2 for 239+240 Pu and 2.6·10 12  at m -2 for 129 I. Atomic ratios for 236 U/ 239 Pu, 137 Cs/ 236 U and 129 I/ 236 U, obtained from the inventories are 0.036, 0.11 and 2.5 respectively. Concentration profiles show mobilization probably due to bioturbation from the abundant detritivore holothurian species living at the PAP site sea-floor. The range of 236 U, 137 Cs, 239+240 Pu and 129 I values, inventories and ratios of these anthropogenic radionuclides are more similar to the values due to fall-out than values from a contribution from the Nuclear Fuel Reprocessing Plants dispersed to the south-west of the North Atlantic Ocean. However, signs of an additional source are detected and might be associated to the nuclear wastes dumped on the Eastern North Atlantic Ocean. Copyright © 2017 Elsevier Ltd. All rights reserved.

Can 239 + 240Pu replace 137Cs as an erosion tracer in agricultural landscapes contaminated with Chernobyl fallout?

PubMed

Schimmack, W; Auerswald, K; Bunzl, K

2001-01-01

Erosion studies often use 137Cs from the global fallout (main period: 1953-1964) as a tracer in the soil. In many European countries, where 137Cs was deposited in considerable amounts also by the Chernobyl fallout in 1986, the global fallout fraction (GF-Cs) has to be separated from the Chernobyl fraction by means of the isotope 134Cs. In a few years, this will no longer be possible due to the short half-life of 134Cs (2 yr). Because GF-Cs in the soil can then no longer be determined, the potential of using 239 + 240Pu as a tracer is evaluated. This radionuclide originates in most European countries essentially only from the global fallout. The activities and spatial distributions of Pu and GF-Cs were compared in the soil of a steep field (inclination about 20%, area ca. 3 ha, main soil type Dystric Eutrochrept), sampled at 48 nodes of a 25 x 25 m2 grid. The reference values were determined at 12 points adjacent to the field. Their validity was assured by an inventory study of radiocaesium in a 70 ha area surrounding the field sampling 275 nodes of a 50 x 50 m2 grid. In the field studied, the activity concentrations of GF-Cs and Pu in the Ap horizon were not correlated (Spearman correlation coefficient R = 0.20, p > 0.05), and the activity balance of Pu differed from that of GF-Cs. Whereas no net loss of GF-Cs from the field was observed as compared to the reference site, Pu was more mobile with an average loss of ca. 11% per unit area. In addition, the spatial pattern of GF-Cs and Pu in the field differed significantly. The reason may be that due to their different associations with soil constituents, Pu and Cs represent different fractions of the soil, exhibiting different properties with respect to erosion/deposition processes. This indicates that both radionuclides or one of them may not be appropriate to quantity past erosion. When tracer losses are used to calibrate or verify erosion prediction models, systematic deviations may not only stem from model

The influence of age at time of exposure to sup 226 Ra or sup 239 Pu on distribution, retention, postinjection survival, and tumor induction in beagle dogs

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

Bruenger, F.W.; Lloyd, R.D.; Miller, S.C.

The influence of age at injection of 226Ra or 239Pu on skeletal deposition and local distribution, the pattern of bone tumor formation, and postinjection survival was assessed in parallel short-term studies of mechanisms and lifetime toxicity. Beagles received a single intravenous injection of 226Ra or 239Pu at 3 months (juveniles), 17-19 months (young adults) or 60 months (mature). Data from short-term studies of mechanisms and dosimetry and from one dosage level of each of the toxicity experiments were compared. Skeletal growth and turnover produced differential initial deposition and distribution patterns typical for each age group. At 1 week after injection,more » skeletal retention of 226Ra or 239Pu was 68 and 68%, respectively, in the juveniles, 32 and 46% in the young adults, and 31 and 43% in the mature dogs. Comparing individual bones in the juveniles, gradients in the concentration of 239Pu were small since all bones were actively growing, but substantial gradients, corresponding to centers of ossification, were present within individual bones. In other age groups, local concentration gradients were less pronounced, but much larger differences were present among the various bones. In the toxicity study all animals injected with either 41 kBq 226Ra/kg or 11 kBq 239Pu/kg have died. The cumulative average skeletal doses to the presumed time of start of tumor growth (1 year before death) were 25 and 4 Gy, respectively, for the juveniles, 22 and 5 Gy for the young adults, and 15 and 4 Gy for the mature dogs. The highest bone tumor incidence was seen in the young adult groups. Differences were observed in location of bone tumors between dogs in the same age group given radium or plutonium and among age groups injected with either radionuclide, some of which could be explained by differences in local dose distributions.« less

Trace metal cycling and 238U/235U in New Zealand's fjords: Implications for reconstructing global paleoredox conditions in organic-rich sediments

NASA Astrophysics Data System (ADS)

Hinojosa, Jessica L.; Stirling, Claudine H.; Reid, Malcolm R.; Moy, Christopher M.; Wilson, Gary S.

2016-04-01

Reconstructing the history of ocean oxygenation provides insight into links between ocean anoxia, biogeochemical cycles, and climate. Certain redox-sensitive elements respond to changes in marine oxygen content through phase shifts and concomitant isotopic fractionation, providing new diagnostic proxies of past ocean hypoxia. Here we explore the behavior and inter-dependence of a suite of commonly utilized redox-sensitive trace metals (U, Mo, Fe, and Mn) and the emerging ;stable; isotope system of U (238U/235U, or δ238U) in New Zealand fjords. These semi-restricted basins have chemical conditions spanning the complete redox spectrum from fully oxygenated to suboxic to intermittently anoxic/euxinic. In the anoxic water column, U and Mo concentrations decrease, while Fe and Mn concentrations increase. Similarly, signals of past euxinic conditions can be found by U, Mo, Fe, and Mn enrichment in the underlying sediments. The expected U isotopic shift toward a lower δ238U in the anoxic water column due to U(VI)-U(IV) reduction is not observed; instead, water column δ238U profiles are consistent in fjords of all oxygen content, falling within previously reported ranges for open ocean seawater (δ238U = -0.42 ± 0.07‰). Additionally, surface sediment δ238U results show evidence for competing U isotope fractionation processes. One site indicates increased export of 238U from seawater to the underlying sediments (fractionation between aqueous seawater U and particulate sediment U, or ΔU(aq)-U(solid) = -0.25‰), consistent with redox-driven fractionation. Another site suggests potential U(VI) adsorption-driven fractionation, reflecting increased export of 235U from seawater to sediments (ΔU(aq)-U(solid) = 0.25‰). We discuss several potential factors that could alter δ238U in waters and sediments beyond redox-driven shifts, including adsorption to organic matter in waters of high primary productivity, reaction rates for competing processes of U adsorption and

Accumulation of atmospheric radionuclides and heavy metals in cryoconite holes on an Arctic glacier.

PubMed

Łokas, Edyta; Zaborska, Agata; Kolicka, Małgorzata; Różycki, Michał; Zawierucha, Krzysztof

2016-10-01

Surface of glaciers is covered by mineral and organic dust, together with microorganisms forming cryoconite granules. Despite fact that glaciers and ice sheets constitute significance part of land surface, reservoir of freshwater, and sites of high biological production, the knowledge on the cryoconite granules still remain unsatisfactory. This study presents information on radionuclide and heavy metal contents in cryoconites. Cryoconites collected from the Hans Glacier in SW Spitsbergen reveal high activity concentrations of anthropogenic ((238,239,240)Pu, (137)Cs, (90)Sr) and natural ((210)Pb) radionuclides. The (238)Pu/(239+240)Pu activity ratios in these cryoconites significantly exceed the mean global fallout ratio (0.025). The (238)Pu/(239+240)Pu ranged from 0.064 to 0.118. The (239+240)Pu/(137)Cs varied from 0.011 ± 0.003 to 0.030 ± 0.007. Such activity ratios as observed in these cryoconites were significantly higher than the values characterizing global fallout, pointing to possible contributions of these radionuclides from other sources. Heavy metals (Pb, Cd, Cu, Zn, Fe, and Mn) in cryoconites exceed both UCC concentrations and local rocks' concentrations, particularly for cadmium. The concentration ratios of stable lead isotopes ((206)Pb/(207)Pb, (208)Pb/(206)Pb) were determined to discriminate between the natural and anthropogenic sources of Pb in cryoconites and to confirm the strong anthropogenic contribution to heavy metal deposition in the Arctic. In investigated cryoconite holes, two groups of invertebrates, both extremophiles, Tardigrada and Rotifera were detected. Our study indicate that cryoconites are aggregates of mineral and organic substances on surfaces of glaciers are able to accumulate large amounts of airborne pollutants bound to extracellular polymeric substances secreted by microorganisms. Copyright © 2016 Elsevier Ltd. All rights reserved.

The need for precise and well-documented experimental data on prompt fission neutron spectra from neutron-induced fission of 239Pu

DOE PAGES

Neudecker, Denise; Taddeucci, Terry Nicholas; Haight, Robert Cameron; ...

2016-01-06

The spectrum of neutrons emitted promptly after 239Pu(n,f)—a so-called prompt fission neutron spectrum (PFNS)—is a quantity of high interest, for instance, for reactor physics and global security. However, there are only few experimental data sets available that are suitable for evaluations. In addition, some of those data sets differ by more than their 1-σ uncertainty boundaries. We present the results of MCNP studies indicating that these differences are partly caused by underestimated multiple scattering contributions, over-corrected background, and inconsistent deconvolution methods. A detailed uncertainty quantification for suitable experimental data was undertaken including these effects, and test-evaluations were performed with themore » improved uncertainty information. The test-evaluations illustrate that the inadequately estimated effects and detailed uncertainty quantification have an impact on the evaluated PFNS and associated uncertainties as well as the neutron multiplicity of selected critical assemblies. A summary of data and documentation needs to improve the quality of the experimental database is provided based on the results of simulations and test-evaluations. Furthermore, given the possibly substantial distortion of the PFNS by multiple scattering and background effects, special care should be taken to reduce these effects in future measurements, e.g., by measuring the 239Pu PFNS as a ratio to either the 235U or 252Cf PFNS.« less

Heptavalent Actinide Tetroxides NpO 4 – and PuO 4 –: Oxidation of Pu(V) to Pu(VII) by Adding an Electron to PuO 4

DOE PAGES

Gibson, John K.; de Jong, Wibe A.; Dau, Phuong D.; ...

2017-11-14

The highest known actinide oxidation states are Np(VII) and Pu(VII), both of which have been identified in solution and solid compounds. Recently a molecular Np(VII) complex, NpO 3(NO 3) 2-, was prepared and characterized in the gas phase. In accord with the lower stability of heptavalent Pu, no Pu(VII) molecular species has been identified. Reported here are the gas-phase syntheses and characterizations of NpO 4 - and PuO 4 -. Reactivity studies and density functional theory computations indicate the heptavalent metal oxidation state in both. This is the first instance of Pu(VII) in the absence of stabilizing effects due tomore » condensed phase solvation or crystal fields. Here, the results indicate that addition of an electron to neutral PuO 4, which has a computed electron affinity of 2.56 eV, counterintuitively results in oxidation of Pu(V) to Pu(VII), concomitant with superoxide reduction.« less