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Sample records for plutonium isotopes

  1. A particulate isotopic standard of plutonium in an aluminosilicate matrix

    SciTech Connect

    Stoffels, J.J.; Cannon, W.C.; Robertson, D.M. )

    1991-01-01

    Plutonium isotopic microstandard particles have been produced for mass spectrometer calibration. The particles may also be useful as an elemental standard for calibration of electron and ion microprobe instruments. The standard consists of spherical, micrometer-size aluminosilicate particles loaded with plutonium of known isotopic distribution. The morphology, elemental composition, and plutonium isotopic composition of the particles have been characterized.

  2. Measurement of Plutonium Isotopic Composition - MGA

    SciTech Connect

    Vo, Duc Ta

    2015-08-21

    In this module, we will use the Canberra InSpector-2000 Multichannel Analyzer with a high-purity germanium detector (HPGe) and the MGA isotopic anlysis software to assay a variety of plutonium samples. The module provides an understanding of the MGA method, its attributes and limitations. You will assess the system performance by measuring a range of materials similar to those you may assay in your work. During the final verification exercise, the results from MGA will be combined with the 240Pueff results from neutron coincidence or multiplicity counters so that measurements of the plutonium mass can be compared with the operator-declared (certified) values.

  3. AMS of the Minor Plutonium Isotopes

    PubMed Central

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

    2013-01-01

    VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure 239Pu, 240Pu, 241Pu, 242Pu and 244Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of 244Pu/239Pu = (5.7 ± 1.0) × 10−5 based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the 242Pu/240Pu ratio as an estimate of the initial 241Pu/239Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method. PMID:23565016

  4. AMS of the Minor Plutonium Isotopes.

    PubMed

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

    2013-01-01

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

  5. Uranium and plutonium isotopes in the atmosphere

    SciTech Connect

    Sakuragi, Y.; Meason, J.L.; Kuroda, P.K.

    1983-04-20

    Uranium 234 and 235 were found to be highly enriched relative to uranium 238 in several rain samples collected at Fayetteville, Arkansas, during the months of April and May 1980. The anomalous uranium appears to have originated from the Soviet satellite Cosmos-954, which fell over Canada on January 24, 1978. The uranium fallout occurred just about the time Mount St. Helens erupted on May 18, 1980. The concentration of /sup 238/U in rain increased markedly after the eruption of Mount St. Helens, and it appeared as if a large quantity of natural uranium was injected into the atmosphere by the volcanic eruption. The pattern of variation of the concentrations of uranium in rain after the eruption of Mount St. Helens was found to be similar to that of plutonium isotopes.

  6. Anthropogenic plutonium-244 in the environment: Insights into plutonium's longest-lived isotope.

    PubMed

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

    2016-02-22

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

  7. Guide to plutonium isotopic measurements using gamma-ray spectrometry

    SciTech Connect

    Lemming, J.F.; Rakel, D.A.

    1982-08-26

    Purpose of this guide is to assist those responsible for plutonium isotopic measurements in the application of gamma-ray spectrometry. Objectives are to promote an understanding of the measurement process, including its limitations and applicability, by reviewing the general features of a plutonium spectrum and identifying the quantities which must be extracted from the data; to introduce state-of-the-art analysis techniques by reviewing four isotopic analysis packages and identifying their differences; to establish the basis for measurement control and assurance by discussing means of authenticating the performance of a measurement system; and to prepare for some specific problems encountered in plutonium isotopic analyses by providing solutions from the practical experiences of several laboratories. 29 references, 12 figures, 17 tables.

  8. Plutonium isotope ratio variations in North America

    SciTech Connect

    Steiner, Robert E; La Mont, Stephen P; Eisele, William F; Fresquez, Philip R; Mc Naughton, Michael; Whicker, Jeffrey J

    2010-12-14

    Historically, approximately 12,000 TBq of plutonium was distributed throughout the global biosphere by thermo nuclear weapons testing. The resultant global plutonium fallout is a complex mixture whose {sup 240}Pu/{sup 239}Pu atom ratio is a function of the design and yield of the devices tested. The average {sup 240}Pu/{sup 239}Pu atom ratio in global fallout is 0.176 + 014. However, the {sup 240}Pu/{sup 239}Pu atom ratio at any location may differ significantly from 0.176. Plutonium has also been released by discharges and accidents associated with the commercial and weapons related nuclear industries. At many locations contributions from this plutonium significantly alters the {sup 240}Pu/{sup 239}Pu atom ratios from those observed in global fallout. We have measured the {sup 240}Pu/{sup 239}Pu atom ratios in environmental samples collected from many locations in North America. This presentation will summarize the analytical results from these measurements. Special emphasis will be placed on interpretation of the significance of the {sup 240}Pu/{sup 239}Pu atom ratios measured in environmental samples collected in the Arctic and in the western portions of the United States.

  9. A study on determination of potentially hazardous plutonium isotopes in environmental samples.

    PubMed

    Strumińska-Parulska, Dagmara I

    2013-01-01

    Due to the lack of stable plutonium isotopes, and the high mobility as well as long half-life, plutonium is considered one of the most important radioelement in safety assessment of environmental radioactivity and nuclear waste management. A number of analytical methods have been developed over the past decades for determination of plutonium in environmental samples. The article discusses different analytical techniques and presents the results of plutonium isotopes determination by alpha spectrometry and accelerator mass spectrometry in environmental samples. The concentrations of plutonium isotopes in analyzed samples indicates its measurement is of great importance for environmental and safety assessment, especially in contaminated areas.

  10. Plutonium isotopic determination from gamma-ray spectra

    SciTech Connect

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

    1998-12-31

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

  11. Uranium and plutonium isotopic analysis using MGA++

    SciTech Connect

    Buckley, W; Clark, D; Friensehner, A; Parker, W; Raschke, K; Romine, W; Ruhter, W; Wang, T-F; kreek, S

    1998-07-01

    The Lawrence Livermore National Laboratory develops sophisticated gamma-ray analysis codes for the isotopic analysis of nuclear materials based on the principles used in the original MultiGroup Analysis (MGA) code. Over the years, the MGA methodology has been upgraded and expanded far beyond its original capabilities and is now comprised of a suite of codes known as MGA++. The early MGA code analyzed Pu gamma-ray data collected with high-purity germanium (HPGe) detectors to yield Pu isotopic ratios. While the original MGA code relied solely on the lower-energy gamma rays (around 100 keV), the most recent addition to the MGA++ code suite, MGAHI, analyzes Pu data using higher-energy gamma rays (200 keV and higher) and is particulatly useful for Pu samples - that are enclosed in thick-walled containers. The MGA++ suite also includes capabilities to perform U isotopic analysis on data collected with either HPGe or cadmium-zinc-tellutide (CZT) detectors. These codes are commercially available and are known as U235 and CZTU, respectively. A graphical user interface has also been developed for viewing the data and the fitting procedure. In addition, we are developing new codes that will integrate into the MGA++ suite. These will include Pu isotopic analysis capabilities for data collected with CZT detectors, U isotopic analysis with HPGe detectors which utilizes only higher energy gamma rays, and isotopic analyses on mixtures of Pu and U.

  12. Development of isotope dilution gamma-ray spectrometry for plutonium analysis

    SciTech Connect

    Li, T.K.; Parker, J.L. ); Kuno, Y.; Sato, S.; Kurosawa, A.; Akiyama, T. )

    1991-01-01

    We are studying the feasibility of determining the plutonium concentration and isotopic distribution of highly radioactive, spent-fuel dissolver solutions by employing high-resolution gamma-ray spectrometry. The study involves gamma-ray plutonium isotopic analysis for both dissolver and spiked dissolver solution samples, after plutonium is eluted through an ion-exchange column and absorbed in a small resin bead bag. The spike is well characterized, dry plutonium containing {approximately}98% of {sup 239}Pu. By using measured isotopic information, the concentration of elemental plutonium in the dissolver solution can be determined. Both the plutonium concentration and the isotopic composition of the dissolver solution obtained from this study agree well with values obtained by traditional isotope dilution mass spectrometry (IDMS). Because it is rapid, easy to operate and maintain, and costs less, this new technique could be an alternative method to IDMS for input accountability and verification measurements in reprocessing plants. 7 refs., 4 figs., 4 tabs.

  13. Plutonium isotopes as tracers for ocean processes: a review.

    PubMed

    Lindahl, Patric; Lee, Sang-Han; Worsfold, Paul; Keith-Roach, Miranda

    2010-03-01

    Since the first nuclear weapons tests in the 1940s, pulsed inputs of plutonium isotopes have served as excellent tracers for understanding sources, pathways, dynamics and the fate of pollutants and particles in the marine environment. Due to the well-defined spatial and temporal inputs of Pu, the long half-lives of (240)Pu and (239)Pu and its unique chemical properties, Pu is a potential tracer for various physical and biogeochemical ocean processes, including circulation, sedimentation and biological productivity, and hence a means of assessing the impacts of global climate change. Due to the source dependency of the Pu isotopic signature, plutonium isotopes are beginning to be exploited as tools for the evaluation and improvement of regional and global ocean models that will enhance understanding of past and future changes in the oceans. This paper addresses the major sources of Pu and the physical and biogeochemical behaviour in the marine environment. Finally, the use of Pu isotopes as tracers for various oceanic processes (e.g. water mass transport, particle export, and sedimentation) is considered.

  14. Plutonium, (137)Cs and uranium isotopes in Mongolian surface soils.

    PubMed

    Hirose, K; Kikawada, Y; Igarashi, Y; Fujiwara, H; Jugder, D; Matsumoto, Y; Oi, T; Nomura, M

    2017-01-01

    Plutonium ((238)Pu and (239,240)Pu), (137)Cs and plutonium activity ratios ((238)Pu/(239,240)Pu) as did uranium isotope ratio ((235)U/(238)U) were measured in surface soil samples collected in southeast Mongolia. The (239,240)Pu and (137)Cs concentrations in Mongolian surface soils (<53 μm of particle size) ranged from 0.42 ± 0.03 to 3.53 ± 0.09 mBq g(-1) and from 11.6 ± 0.7 to 102 ± 1 mBq g(-1), respectively. The (238)Pu/(239,240)Pu activity ratios in the surface soils (0.013-0.06) coincided with that of global fallout. The (235)U/(238)U atom ratios in the surface soil show the natural one. There was a good correlation between the (239,240)Pu and (137)Cs concentrations in the surface soils. We introduce the migration depth to have better understanding of migration behaviors of anthropogenic radionuclides in surface soil. We found a difference of the migration behavior between (239,240)Pu and (137)Cs from (137)Cs/(239,240)Pu - (137)Cs plots for the Mongolian and Tsukuba surface soils; plutonium in surface soil is migrated easier than (137)Cs.

  15. Isotopic ratio correlation for the isotopic composition analysis of plutonium in Am-Pu mixed samples having high americium content.

    PubMed

    Patra, Sabyasachi; Agarwal, Chhavi; Chaudhury, Sanhita; Newton Nathaniel, T; Gathibandhe, M; Goswami, A

    2013-08-01

    Interference of high amount of americium in the plutonium isotopic composition analysis has been studied by simulating gamma-ray spectra for Am-Pu samples over a wide composition range (5-97% (241)Am) for both power and research reactor grade plutonium. An alternate way for isotopic composition analysis has been proposed by correlating the isotopic ratios available in our old database with the experimentally obtained (241)Pu/(239)Pu isotopic ratio. The proposed method has been validated using simulated spectra of known isotopic compositions.

  16. Implications of Plutonium isotopic separation on closed fuel cycles and repository design

    SciTech Connect

    Forsberg, C.

    2013-07-01

    Advances in laser enrichment may enable relatively low-cost plutonium isotopic separation. This would have large impacts on LWR closed fuel cycles and waste management. If Pu-240 is removed before recycling plutonium as mixed oxide (MOX) fuel, it would dramatically reduce the buildup of higher plutonium isotopes, Americium, and Curium. Pu-240 is a fertile material and thus can be replaced by U-238. Eliminating the higher plutonium isotopes in MOX fuel increases the Doppler feedback, simplifies reactor control, and allows infinite recycle of MOX plutonium in LWRs. Eliminating fertile Pu-240 and Pu-242 reduces the plutonium content in MOX fuel and simplifies fabrication. Reducing production of Pu-241 reduces production of Am-241 - the primary heat generator in spent nuclear fuels after several decades. Reducing heat generating Am-241 would reduce repository cost and waste toxicity. Avoiding Am- 241 avoids its decay product Np-237, a nuclide that partly controls long-term oxidizing repository performance. Most of these benefits also apply to LWR plutonium recycled into fast reactors. There are benefits for plutonium isotopic separation in fast reactor fuel cycles (particularly removal of Pu-242) but the benefits are less. (author)

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

    PubMed

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

    2010-12-15

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

  18. Rapid fusion method for determination of plutonium isotopes in large rice samples

    SciTech Connect

    Maxwell, Sherrod L.; Culligan, Brian K.; Hutchison, Jay B.

    2013-04-30

    A new rapid fusion method for the determination of plutonium in large rice samples has been developed at the Savannah River National Laboratory (Aiken, SC, USA) that can be used to determine very low levels of plutonium isotopes in rice. The recent accident at Fukushima Nuclear Power Plant in March, 2011 reinforces the need to have rapid, reliable radiochemical analyses for radionuclides in environmental and food samples. Public concern regarding foods, particularly foods such as rice in Japan, highlights the need for analytical techniques that will allow very large sample aliquots of rice to be used for analysis so that very low levels of plutonium isotopes may be detected. The new method to determine plutonium isotopes in large rice samples utilizes a furnace ashing step, a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step, and a column separation process with TEVA Resin cartridges. The method can be applied to rice sample aliquots as large as 5 kg. Plutonium isotopes can be determined using alpha spectrometry or inductively-coupled plasma mass spectrometry (ICP-MS). The method showed high chemical recoveries and effective removal of interferences. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory plutonium particles are effectively digested. The MDA for a 5 kg rice sample using alpha spectrometry is 7E-5 mBq g{sup -1}. The method can easily be adapted for use by ICP-MS to allow detection of plutonium isotopic ratios.

  19. Impact of environmental curium on plutonium migration and isotopic signatures.

    PubMed

    Kurosaki, Hiromu; Kaplan, Daniel I; Clark, Sue B

    2014-12-02

    Plutonium (Pu), americium (Am), and curium (Cm) activities were measured in sediments from a former radioactive waste disposal basin located on the Savannah River Site, South Carolina, and in subsurface aquifer sediments collected downgradient from the basin. In situ Kd values (Pu concentration ratio of sediment/groundwater) derived from this field data and previously reported groundwater concentration data compared well to laboratory Kd values reported in the literature. Pu isotopic signatures confirmed multiple sources of Pu contamination. The ratio of (240)Pu/(239)Pu was appreciably lower for sediment samples compared to the associated groundwater. This isotopic ratio difference may be explained by the following: (1) (240)Pu produced by decay of (244)Cm may exist predominantly in high oxidation states (Pu(V)O2(+) and Pu(VI)O2(2+)) compared to Pu derived from the disposed waste effluents, and (2) oxidized forms of Pu sorb less to sediments than reduced forms of Pu. Isotope-specific Kd values calculated from measured Pu activities in the sediments and groundwater indicated that (240)Pu, which is derived primarily from the decay of (244)Cm, had a value of 10 ± 2 mL g(-1), whereas (239)Pu originating from the waste effluents discharged at the site had a value of 101 ± 8 mL g(-1). One possible explanation for the isotope-specific sorption behavior is that (240)Pu likely existed in the weaker sorbing oxidation states, +5 or +6, than (239)Pu, which likely existed in the +3 or +4 oxidation states. Consequently, remediation strategies for radioactively contaminated systems must consider not only the discharged contaminants but also their decay products. In this case, mitigation of Cm as well as Pu will be required to completely address Pu migration from the source term.

  20. Determination of plutonium isotopes in seawater reference materials using isotope-dilution ICP-MS.

    PubMed

    Zheng, Jian; Yamada, Masatoshi

    2012-09-01

    We analyzed the activities of (239)Pu, (240)Pu, (239+240)Pu, (241)Pu, the ratio of number of atoms (atom ratio) for (240)Pu/(239)Pu, and the activity ratio of (241)Pu/(239+240)Pu in seawater reference materials, IAEA-443 and IAEA-381, using a highly sensitive isotope dilution sector field inductively coupled plasma mass spectrometry method. With a mean chemical yield of 65% determined with (242)Pu as a tracer, we found that the experimentally established values in IAEA-443 for (239)Pu, (240)Pu, (241)Pu and (239+240)Pu activities are almost the same as those in IAEA-381. Regarding the (239+240)Pu activity, we provided the most precise and accurate result among the twelve laboratories, which participated in the interlaboratory comparison. In addition, for the (240)Pu/(239)Pu atom ratio, our results for IAEA-381 (0.2315±0.0008) and IAEA-443 (0.2325±0.0008) are in good agreement with the IAEA information value (0.229±0.006), but have much smaller uncertainty. Since the new seawater reference material, IAEA-443, is commercially available, it can be used not only for method validation for seawater plutonium isotope ratio and activity analysis, but also for more general use as a plutonium isotope standard for mass discrimination correction for other environmental samples.

  1. On the equilibrium isotopic composition of the thorium-uranium-plutonium fuel cycle

    NASA Astrophysics Data System (ADS)

    Marshalkin, V. Ye.; Povyshev, V. M.

    2016-12-01

    The equilibrium isotopic compositions and the times to equilibrium in the process of thorium-uranium-plutonium oxide fuel recycling in VVER-type reactors using heavy water mixed with light water are estimated. It is demonstrated thEhfat such reactors have a capacity to operate with self-reproduction of active isotopes in the equilibrium mode.

  2. On the equilibrium isotopic composition of the thorium–uranium–plutonium fuel cycle

    SciTech Connect

    Marshalkin, V. Ye. Povyshev, V. M.

    2016-12-15

    The equilibrium isotopic compositions and the times to equilibrium in the process of thorium–uranium–plutonium oxide fuel recycling in VVER-type reactors using heavy water mixed with light water are estimated. It is demonstrated thEhfat such reactors have a capacity to operate with self-reproduction of active isotopes in the equilibrium mode.

  3. Spent fuel temperature and age determination from the analysis of uranium and plutonium isotopics

    SciTech Connect

    Scott, Mark R; Eccleston, George W; Bedell, Jeffrey J; Lockard, Chanelle M

    2009-01-01

    The capability to determine the age (time since irradiation) of spent fuel can be useful for verification and safeguards. While the age of spent fuel can be determined based on measurements of short-lived fission products, these measurements are not routinely done nor generally reported. As an alternative, age can also be determined if the uranium (U) and plutonium (Pu) isotopic values are available. Uranium isotopics are not strongly affected by fuel temperature, and bumup is determined from the {sup 235}U and {sup 236}U isotopic values. Age is calculated after estimating the {sup 241}Pu at the end of irradiation while accounting for the fuel temperature, which is determined from {sup 239}Pu or {sup 240}Pu. Burnup and age determinations are calibrated to reactor models that provide uranium and plutonium isotopics over the range of fuel irradiation. The reactor model must contain sufficient fidelity on details of the reactor type, fuel burnup, irradiation history, initial fuel enrichment and fuel temperature to obtain accurate isotopic calculations. If the latter four are unknown, they can be derived from the uranium and plutonium isotopics. Fuel temperature has a significant affect on the production of plutonium isotopics; therefore, one group cross section reactor models, such as ORIGEN, cannot be used for these calculations. Multi-group cross section set codes, such as Oak Ridge National Laboratory's TRITON code, must be used.

  4. Displacements Isotopiques Relatifs et Moments Quadrupolaires Intrinseques des Isotopes du Plutonium

    NASA Astrophysics Data System (ADS)

    Gerstenkorn, S.; Luc, P.; Tomkins, F.

    1985-09-01

    Extensive isotope shifts measurements in the 3910-9160 Å region of the plutonium spectrum were made. This enables us to determine with precision the value of the Relative Isotope Shift (R.I.S.) between the 244-242 and 242-240 couples of isotopes. The value found for the R.I.S. is 1.03 ± 0.02. Based on the optical R.I.S. of the plutonium isotopes (from 238 to 244) the inherent quadrupole moments of the odd isotopes were determined, using the known values of the quadrupole moments of the even isotopes (deduced from Coulomb excitation). They were found to be respectively equal (in barns) to: Q239 = 11.3 ± 1.0, Q241 = 11.5 ± 0.5, Q243 = 11.6 ± 0.5.

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

    PubMed Central

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

    2016-01-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-02-01

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

  7. Determination of plutonium content in high burnup pressurized water reactor fuel samples and its use for isotope correlations for isotopic composition of plutonium.

    PubMed

    Joe, Kihsoo; Jeon, Young-Shin; Han, Sun-Ho; Lee, Chang-Heon; Ha, Yeong-Keong; Song, Kyuseok

    2012-06-01

    The content of plutonium isotopes in high burnup pressurized water reactor fuel samples was examined using both alpha spectrometry and mass spectrometry after anion exchange separation. The measured values were compared with results calculated by the ORIGEN-2 code. On average, the ratios (m/c) of the measured values (m) over the calculated values (c) were 1.22±0.16 for (238)Pu, 1.02±0.14 for (239)Pu, 1.08±0.06 for (240)Pu, 1.06±0.16 for (241)Pu, and 1.13±0.08 for (242)Pu. Using the Pu data obtained in this work, correlations were derived between the alpha activity ratios of (238)Pu/((239)Pu+(240)Pu), the alpha specific activities of Pu, and the atom % abundances of the Pu isotopes. Using these correlations, the atom % abundances of the plutonium isotopes in the target samples were calculated. These calculated results agreed within a range from 2 to 8% of the experimentally derived values according to the isotopes of plutonium.

  8. Plutonium

    NASA Astrophysics Data System (ADS)

    Clark, David L.; Hecker, Siegfried S.; Jarvinen, Gordon D.; Neu, Mary P.

    The element plutonium occupies a unique place in the history of chemistry, physics, technology, and international relations. After the initial discovery based on submicrogram amounts, it is now generated by transmutation of uranium in nuclear reactors on a large scale, and has been separated in ton quantities in large industrial facilities. The intense interest in plutonium resulted fromthe dual-use scenario of domestic power production and nuclear weapons - drawing energy from an atomic nucleus that can produce a factor of millions in energy output relative to chemical energy sources. Indeed, within 5 years of its original synthesis, the primary use of plutonium was for the release of nuclear energy in weapons of unprecedented power, and it seemed that the new element might lead the human race to the brink of self-annihilation. Instead, it has forced the human race to govern itself without resorting to nuclear war over the past 60 years. Plutonium evokes the entire gamut of human emotions, from good to evil, from hope to despair, from the salvation of humanity to its utter destruction. There is no other element in the periodic table that has had such a profound impact on the consciousness of mankind.

  9. Laser ablation absorption spectroscopy for isotopic analysis of plutonium: Spectroscopic properties and analytical performance

    NASA Astrophysics Data System (ADS)

    Miyabe, M.; Oba, M.; Jung, K.; Iimura, H.; Akaoka, K.; Kato, M.; Otobe, H.; Khumaeni, A.; Wakaida, I.

    2017-08-01

    Spectroscopic properties of atomic species of plutonium were investigated by combining laser ablation and resonance absorption techniques for the analysis of a plutonium oxide sample. For 17 transitions of Pu atoms and ions, the absorbance, isotope shift, and hyperfine splitting were determined via Voigt profile fitting of the recorded absorption spectra. Three transitions were selected as candidates for analytical use. Using these transitions, we investigated the analytical performance that was attainable and determined a correlation coefficient R2 between the absorbance and plutonium concentration of 0.9999, a limit of detection of 30-130 ppm, and a relative standard deviation of approximately 6% for an abundance of 240Pu of 2.4%. These results demonstrate that laser ablation absorption spectroscopy is applicable to the remote isotopic analysis of highly radioactive nuclear fuels and waste materials containing multiple actinide elements.

  10. Static, mixed-array total evaporation for improved quantitation of plutonium minor isotopes in small samples

    SciTech Connect

    Stanley, F. E.; Byerly, Benjamin L.; Thomas, Mariam R.; Spencer, Khalil J.

    2016-03-31

    Actinide isotope measurements are a critical signature capability in the modern nuclear forensics “toolbox”, especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (<10-6) within already limited quantities of sample. Herein, we investigate the application of static, mixed array total evaporation techniques as a straightforward means of improving plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Furthermore, results are presented for small sample (~20 ng) applications involving a well-known plutonium isotope reference material, CRM-126a, and compared with traditional total evaporation methods.

  11. Static, Mixed-Array Total Evaporation for Improved Quantitation of Plutonium Minor Isotopes in Small Samples

    NASA Astrophysics Data System (ADS)

    Stanley, F. E.; Byerly, Benjamin L.; Thomas, Mariam R.; Spencer, Khalil J.

    2016-06-01

    Actinide isotope measurements are a critical signature capability in the modern nuclear forensics "toolbox", especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (<10-6) within already limited quantities of sample. Herein, we investigate the application of static, mixed array total evaporation techniques as a straightforward means of improving plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Results are presented for small sample (~20 ng) applications involving a well-known plutonium isotope reference material, CRM-126a, and compared with traditional total evaporation methods.

  12. Plutonium isotopic analysis system for plutonium samples enriched in sup 238 Pu in EP 60/61 containers

    SciTech Connect

    Ruhter, W.D.

    1990-06-01

    This user's manual is addressed to the Savannah River Site personnel (routine operators and supervisors) who perform measurements with the Pu-238 isotopic analysis system. Each chapter begins with a table of contents that lists the section title, illustrations, and tabular data presented in that chapter. The first chapter in this manual is an introduction to the system. Chapter 2 lists required settings for the system's commercial nuclear instrument modules. System operating procedures are given in Chapter 3. Chapter 4 contains routine and supervisorial operator interactions. Chapter 5 describes the system's short- and long-printout output formats. Chapter 6 gives instructions for changing system parameters. Error messages are listed and described Chapter 7. Chapter 8 contains a reference article on measuring relative plutonium isotopics in plutonium samples enriched in Pu-238. All commercial items mentioned in this manual are assumed to be functioning correctly for the purposes of system operation. Users are referred to individual equipment manufacturers' manuals for details of operation, trouble-shooting, and maintenance of this commercial equipment.

  13. Plutonium isotopes offer an alternative approach to establishing chronological profiles in coarse sediments

    NASA Astrophysics Data System (ADS)

    Pondell, C.; Kuehl, S. A.; Canuel, E. A.

    2016-12-01

    There are several methodologies used to determine chronologies for sediments deposited within the past 100 years, including 210Pb and 137Cs radioisotopes and organic and inorganic contaminants. These techniques are quite effective in fine sediments, which generally have a high affinity for metals and organic compounds. However, the application of these chronological tools becomes limited in systems where coarse sediments accumulate. Englebright Lake is an impoundment in northern California where sediment accumulation is characterized by a combination of fine and coarse sediments. This combination of sediment grain size complicated chronological analysis using the more traditional 137Cs chronological approach. This study established a chronology of these sediments using 239+240Pu isotopes. While most of the 249+240Pu activity was measured in the fine grain size fraction (<63 microns), up to 25% of the plutonium activity was detected in the coarse size fractions of sediments from Englebright Lake. Profiles of 239+240Pu were similar to available 137Cs profiles, verifying the application of plutonium isotopes for determining sediment chronologies and expanding the established geochronology for Englebright Lake sediments. This study of sediment accumulation in Englebright Lake demonstrates the application of plutonium isotopes in establishing chronologies in coarse sediments and highlights the potential for plutonium to offer new insights into patterns of coarse sediment accumulation.

  14. PC/FRAM: New capabilities for the gamma-ray spectrometry measurement of plutonium isotopic composition

    SciTech Connect

    Sampson, T.E.; Kelley, T.A.; Cremers, T.L.; Konkel, T.R.; Friar, R.J.

    1995-10-01

    We describe the new capability of and.present measurement results from the PC/FRAM plutonium isotopic analysis code. This new code allows data acquisition from a single coaxial germanium detector and analysis over an energy range from 120 keV to above I MeV. For the first time we demonstrate a complete isotopic analysis using only gamma rays greater than 200 keV in energy. This new capability allows the measurement of the plutonium isotopic composition of items inside shielded or heavy-walled containers without having to remove the items from the container. This greatly enhances worker safety by reducing handling and the resultant radiation exposure. Another application allows international inspectors to verify the contents of items inside sealed, long-term storage containers that may not be opened for national security or treaty compliance reasons. We present measurement results for traditional planar germanium detectors as well as coaxial detectors measuring shielded and unshielded samples.

  15. Feasibility study of plutonium isotopic analysis of resin beads by nondestructive gamma-ray spectroscopy

    SciTech Connect

    Li, T.K.

    1985-01-01

    We have initiated a feasibility study on the use of nondestructive low-energy gamma-ray spectroscopy for plutonium isotopic analysis on resin beads. Seven resin bead samples were measured, with each sample containing an average of 9 ..mu..g of plutonium; the isotopic compositions of the samples varied over a wide range. The gamma-ray spectroscopy results, obtained from 4-h counting-time measurements, were compared with mass spectrometry results. The average ratios of gamma-ray spectroscopy to mass spectrometry were 1.014 +- 0.025 for /sup 238/Pu//sup 239/Pu, 0.996 +- 0.018 for /sup 240/Pu//sup 239/Pu, and 0.980 +- 0.038 for /sup 241/Pu//sup 239/Pu. The rapid, automated, and accurate nondestructive isotopic analysis of resin beads may be very useful to process technicians and International Atomic Energy Agency inspectors. 3 refs., 1 fig., 3 tabs.

  16. Detection of plutonium isotopes at lowest quantities using in-source resonance ionization mass spectrometry.

    PubMed

    Raeder, S; Hakimi, A; Stöbener, N; Trautmann, N; Wendt, K

    2012-11-01

    The in-source resonance ionization mass spectrometry technique was applied for quantification of ultratrace amounts of plutonium isotopes as a proof of principle study. In addition to an overall detection limit of 10(4) to 10(5) atoms, this method enables the unambiguous identification and individual quantification of the plutonium isotopes (238)Pu and (241)Pu which are of relevance for dating of radiogenic samples. Due to the element-selective ionization process, these isotopes can be measured even under a high surplus of isobaric contaminations from (238)U or (241)Am, which considerably simplifies chemical preparation. The technique was developed, tested, and characterized on a variety of synthetic and calibration samples and is presently applied to analyze environmental samples.

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

    EPA Pesticide Factsheets

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

  18. EPA Method EMSL-33: Isotopic Determination of Plutonium, Uranium, and Thorium in Water, Soil, Air, and Biological Tissue

    EPA Pesticide Factsheets

    SAM lists this method to provide for the analysis of isotopic plutonium, uranium and thorium, together or individually, in drinking water, aqueous/liquid, soil/sediment, surface wipe and/or air filter samples by alpha spectrometry.

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

    PubMed

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

    2008-10-01

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

  20. PLUTONIUM ISOTOPIC ANALYSIS WITH FRAM V4 IN THE LOW ENERGY REGION.

    SciTech Connect

    Vo, Duc T.; Li, T. K.

    2001-01-01

    Low-Energy Gamma-ray Spectroscopy (LEGS) is a nondestructive assay (NDA) technique developed in the 1980s. In 1999, it was modified to include a physical-based model for the energy dependent efficiency. It uses the gamma rays in the energy range from approximately 30 keV to 210 keV, except the 100-keV region. This energy region provides intense, well-separated gamma rays from the principal isotopes of plutonium. For applications involving small quantities (mg to g) of freshly separated plutonium in various chemical forms, it is ideally suited for accurate real-time or near real-time isotopic analysis. Since the last modification, LEGS has been incorporated into the FRAM code (Fixed-energy Response-function Analysis with Multiple efficiency), version 4. FRAM v4 is capable of analyzing the peaks in the whole energy range from 30 keV to 1 MeV, including the X-ray region. The new capability of analyzing the peaks in the 100-keV region greatly enhances the plutonium analysis in the 30 keV to 210 keV ranges of the traditional LEGS. We now can analyze both the freshly separated and aged plutonium with greater accuracy.

  1. Static, mixed-array total evaporation for improved quantitation of plutonium minor isotopes in small samples

    DOE PAGES

    Stanley, F. E.; Byerly, Benjamin L.; Thomas, Mariam R.; ...

    2016-03-31

    Actinide isotope measurements are a critical signature capability in the modern nuclear forensics “toolbox”, especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (<10-6) within already limited quantities of sample. Herein, we investigate the application of static, mixed array total evaporation techniques as a straightforward means of improving plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Furthermore, results are presented for small sample (~20 ng) applications involving a well-known plutoniummore » isotope reference material, CRM-126a, and compared with traditional total evaporation methods.« less

  2. Isotopes of uranium and plutonium in the atmosphere. [Cosmos-954 fall in Canada

    SciTech Connect

    Sakuragi, Y.

    1982-01-01

    The activities of /sup 234/U, /sup 235/U and /sup 238/U were measured in 24 individual rain samples and two composite rains collected at Fayetteville, Arkansas, during the months of March 1979 and March 1980 through May 1981. Uranium-234 and -235 were found to be highly enriched in several rain samples collected during the months of April and May 1980. Uranium-238 concentrations, on the other hand, were unusually high during the months of July, August and early September 1980. The concentrations of /sup 238/Pu and /sup 238/ /sup 240/Pu were measured in 76 individual rain samples and two composite rains which were collected at Fayetteville, Arkansas, during the period from February 1979 through December 1980. Plutonium-238 and plutonium-239,240 concentrations were found to be extremely high during the months of July, August and early September 1980. The anomalous uranium highly enriched in the light isotopes of uranium appears to have originated from the Soviet satellite Cosmos-954 which fell over Canada on 24 January 1978. The uranium fallout occurred just about the time Mount St. Helens erupted on 18 May 1980 and began to inject a large amount of natural uranium into the atmosphere. The pattern of variations of the concentrations of /sup 238/U in rain after the eruption of Mount St. Helens was found to be similar to that of plutonium isotopes.

  3. Plutonium isotopes in settling particles: transport and scavenging of Pu in the western Northwest Pacific.

    PubMed

    Zheng, Jian; Yamada, Masatoshi

    2006-07-01

    We examined the vertical distributions of 239+240Pu activity and 240Pu/239Pu atom ratio in settling particles and quantified the particulate 239+240Pu fluxes in the water column in the western Northwest Pacific. Settling particle samples were collected using sediment traps. Plutonium isotopes were analyzed using a sector field high-resolution ICP-MS. To the best of our knowledge, this is the first time that both Pu activity and Pu isotope ratio data have been obtained for settling particles in the Pacific Ocean. The high (>0.18) 240Pu/239Pu atom ratios in settling particles indicate that plutonium from the Pacific Proving Grounds (PPG) source in the central Pacific is transported toward the western Northwest Pacific. Evidence indicates that Pu scavenging onto the settling particles is strongly dependent upon the bulk mass flux. The results suggest that advective lateral transport of dissolved Pu from the open ocean to the ocean margin and removal of Pu into the margin sediments by particle scavenging is a common phenomenon in the Pacific Ocean. Plutonium can be considered as a useful tracer to study the transport and fate of other contaminants that readily adsorb to particles in marine environments.

  4. Broadband non-selective excitation of plutonium isotopes for isotope ratio measurements in resonance ionization mass spectrometry: a theoretical study.

    PubMed

    Sankari, M

    2012-10-15

    Making isotope ratio measurements with minimum isotope bias has always been a challenging task to mass spectrometrists, especially for the specific case of plutonium, owing to the strategic importance of the element. In order to use resonance ionization mass spectrometry (RIMS) as a tool for isotope ratio measurements, optimization of the various laser parameters and other atomic and system parameters is critical to minimize isotopic biases. Broadband simultaneous non-selective excitation of the isotopes of plutonium in the triple resonance excitation scheme with λ(1) = 420.77 nm, λ(2) = 847.28 nm, and λ(3) = 767.53 nm based on density matrix formalism has been theoretically computed for the determination of isotope ratios. The effects of the various laser parameters and other factors such as the atomization temperature and the dimensions of the atomic beam on the estimation of isotope ratios were studied. The effects of Doppler broadening, and time-dependent excitation parameters such as Rabi frequencies, ionization rate and the effect of non-Lorenztian lineshape have all been incorporated. The average laser powers and bandwidths for the three-excitation steps were evaluated for non-selective excitation. The laser intensity required to saturate the three-excitation steps were studied. The two-dimensional lineshape contour and its features were investigated, while the reversal of peak asymmetry of two-step and two-photon excitation peaks under these conditions is discussed. Optimized powers for the non-selective ionization of the three transitions were calculated as 545 mW, 150 mW and 545 mW and the laser bandwidth for all the three steps was ~20 GHz. The isotopic bias between the resonant and off-resonant isotope under the optimized conditions was no more than 9%, which is better than an earlier reported value. These optimized laser power and bandwidth conditions are better than in the earlier experimental work since these comprehensive calculations yield

  5. Separation Of Uranium And Plutonium Isotopes For Measurement By Multi Collector Inductively Coupled Plasma Mass Spectroscopy

    SciTech Connect

    Martinelli, R E; Hamilton, T F; Williams, R W; Kehl, S R

    2009-03-29

    Uranium (U) and plutonium (Pu) isotopes in coral soils, contaminated by nuclear weapons testing in the northern Marshall Islands, were isolated by ion-exchange chromatography and analyzed by mass spectrometry. The soil samples were spiked with {sup 233}U and {sup 242}Pu tracers, dissolved in minerals acids, and U and Pu isotopes isolated and purified on commercially available ion-exchange columns. The ion-exchange technique employed a TEVA{reg_sign} column coupled to a UTEVA{reg_sign} column. U and Pu isotope fractions were then further isolated using separate elution schemes, and the purified fractions containing U and Pu isotopes analyzed sequentially using multi-collector inductively coupled plasma mass spectrometer (MCICP-MS). High precision measurements of {sup 234}U/{sup 235}U, {sup 238}U/{sup 235}U, {sup 236}U/{sup 235}U, and {sup 240}Pu/{sup 239}Pu in soil samples were attained using the described methodology and instrumentation, and provide a basis for conducting more detailed assessments of the behavior and transfer of uranium and plutonium in the environment.

  6. Development of a plutonium solution-assay instrument with isotopic capability

    SciTech Connect

    Hsue, S.T.; Marks, T.

    1992-09-01

    A new generation of solution-assay instrument has been developed to satisfy all the assay requirements of an aqueous plutonium-recovery operation. The assay is based on a transmission-corrected passive assay technique. We have demonstrated that the system can cover a concentration range of 0.5--300 g/{ell} with simultaneous isotopic determination. The system can be used to assay input and eluate streams of the recovery operation. The system can be modified to measure low-concentration effluent solutions from the recovery operation covering 0.01--40 g/{ell}. The same system has also been modified to assay plutonium solutions enriched in {sup 242}Pu. 6 refs.

  7. Gamma radiation characteristics of plutonium dioxide fuel

    NASA Technical Reports Server (NTRS)

    Gingo, P. J.

    1969-01-01

    Investigation of plutonium dioxide as an isotopic fuel for Radioisotope Thermoelectric Generators yielded the isotopic composition of production-grade plutonium dioxide fuel, sources of gamma radiation produced by plutonium isotopes, and the gamma flux at the surface.

  8. A new ground-level fallout record of uranium and plutonium isotopes for northern temperate latitudes

    NASA Astrophysics Data System (ADS)

    Warneke, Thorsten; Croudace, Ian W.; Warwick, Phillip E.; Taylor, Rex N.

    2002-11-01

    Plutonium and uranium isotope ratios can be used to differentiate the sources of nuclear contamination from nuclear weapon establishments (Environ. Sci. Technol. 34 (2000) 4496; Internal Report for AWRE Aldermaston, UK (1961)), weapon fallout (Geochim. Cosmochim. Acta 51 (1987) 2623; Earth Planet. Sci. Lett. 63 (1983) 202; Earth Planet. Sci. Lett. 22 (1974) 111; Geochim. Cosmochim. Acta 64 (2000) 989), reprocessing plants, reactor or satellite accidents (Science 105 (1979) 583; Science 238 (1987) 512) and in addition they provide markers for post-1952 geochronology of environmental systems. A good record of plutonium and uranium isotope ratios of the background resulting from atmospheric nuclear testing is essential for source characterisation studies. Using recently developed mass spectrometric techniques (J. Anal. At. Spectrom. 16 (2001) 279) we present here the first complete records between 1952 and the present day of northern temperate latitude 240Pu/ 239Pu and 238U/ 235U atom ratios for atmospheric deposition. Such information was not derived directly during the period of atmospheric testing because suitable mass spectrometric capability was not available. The currently derived records are based on an annual herbage archive and a core from an Alpine glacier. These studies reveal hitherto unseen fluctuations in the 238U/ 235U atmospheric fallout record, some of which are directly related to nuclear testing. In addition, they also provide the first evidence that plutonium contamination originating from Nevada Desert atmospheric weapon tests in 1952 and 1953 extended eastwards as far as northwestern Europe. The results presented here demonstrate that we now have the capability to detect and precisely identify sources of plutonium in the environment with implications for the development of atmospheric transport models, recent geochronology and environmental studies.

  9. Plutonium isotopic analysis system for plutonium samples enriched in sup 238 Pu in EP 60/61 and fuel-clad containers

    SciTech Connect

    Ruhter, W.D.

    1991-07-01

    This software manual is addressed to the Westinghouse Hanford's Radioisotope Power Systems Facility personnel (programmers and supervisors) who maintain the software on the Pu-238 isotopic analysis system. The document is divided into two parts. Part 1 describes the computer codes that control the system, analyze the spectral data, and determine the relative plutonium abundances. Part 2 contains the software listing of the analysis codes.

  10. Plutonium isotopic analysis system for plutonium samples enriched in {sup 238}Pu in EP 60/61 and fuel-clad containers. Volume 3, Part 2: Software listings

    SciTech Connect

    Ruhter, W.D.

    1991-07-01

    This software manual is addressed to the Westinghouse Hanford`s Radioisotope Power Systems Facility personnel (programmers and supervisors) who maintain the software on the Pu-238 isotopic analysis system. The document is divided into two parts. Part 1 describes the computer codes that control the system, analyze the spectral data, and determine the relative plutonium abundances. Part 2 contains the software listing of the analysis codes.

  11. Plutonium isotopes in the terrestrial environment at the Savannah River Site, USA: a long-term study.

    PubMed

    Armstrong, Christopher R; Nuessle, Patterson R; Brant, Heather A; Hall, Gregory; Halverson, Justin E; Cadieux, James R

    2015-02-03

    This work presents the findings of a long-term plutonium (Pu) study at Savannah River Site (SRS) conducted between 2003 and 2013. Terrestrial environmental samples were obtained at the Savannah River National Laboratory (SRNL) in the A-Area. Plutonium content and isotopic abundances were measured over this time period by α particle and thermal ionization mass spectrometry (3STIMS). We detail the complete process of the sample collection, radiochemical separation, and measurement procedure specifically targeted to trace plutonium in bulk environmental samples. Total plutonium activities were determined to be not significantly above atmospheric global fallout. However, the (238)Pu/(239+240)Pu activity ratios attributed to SRS are substantially different than fallout due to past (238)Pu production on the site. The (240)Pu/(239)Pu atom ratios are reasonably consistent from year to year and are lower than fallout indicating an admixture of weapons-grade material, while the (242)Pu/(239)Pu atom ratios are higher than fallout values, again due to actinide production activities. Overall, the plutonium signatures obtained in this study reflect a distinctive mixture of weapons-grade, heat source, and higher burn-up plutonium with fallout material. This study provides a unique opportunity for developing and demonstrating a blue print for long-term low-level monitoring of trace plutonium in the environment.

  12. Production and analysis of mass-deficient neptunium and plutonium isotopes

    NASA Astrophysics Data System (ADS)

    Whittaker, B.

    1984-06-01

    Neptunium-235, 236Pu and 237Pu are produced by cyclotron-irradiation of high-enrichment 238U or 235U targets. Plutonium-236 may be directly assayed and partially analysed by means of alpha-counting and spectrometry techniques, but 235Np and 237Pu are assayed indirectly by their 235U and 237Np ground-state X-ray and gamma emissions, respectively. For 235Np combined alpha, gamma and X-ray analysis is necessary to positively identify and quantify this isotope since 234Np produces an identical X-ray spectrum. The need for new nuclear-data measurements of 237Pu absolute gamma intensities, 235Np alpha branching, and 235Np half-life is stressed. Product isotopic purity is discussed in the context of target material purity and beam energy.

  13. High-resolution laser spectroscopy of long-lived plutonium isotopes

    NASA Astrophysics Data System (ADS)

    Voss, A.; Sonnenschein, V.; Campbell, P.; Cheal, B.; Kron, T.; Moore, I. D.; Pohjalainen, I.; Raeder, S.; Trautmann, N.; Wendt, K.

    2017-03-01

    Long-lived isotopes of plutonium were studied using two complementary techniques, high-resolution resonance ionization spectroscopy (HR-RIS) and collinear laser spectroscopy (CLS). Isotope shifts have been measured on the 5 f67 s27F0→5 f56 d27 s (J =1 ) and 5 f67 s27F1→5 f67 s 7 p (J =2 ) atomic transitions using the HR-RIS method and the hyperfine factors have been extracted for the odd mass nuclei Pu,241239. CLS was performed on the 5 f67 s 8F1 /2→J =1 /2 (27 523.61 cm-1) ionic transition with the hyperfine A factors measured for 239Pu. Changes in mean-squared charge radii have been extracted and show a good agreement with previous nonoptical methods, with an uncertainty improvement by approximately one order of magnitude. Plutonium represents the heaviest element studied to date using collinear laser spectroscopy.

  14. Examination of the effect of alpha radiolysis on plutonium(V) sorption to quartz using multiple plutonium isotopes.

    PubMed

    Hixon, Amy E; Arai, Yuji; Powell, Brian A

    2013-08-01

    The objective of this research was to determine if radiolysis at the mineral surface was a plausible mechanism for surface-mediated reduction of plutonium. Batch sorption experiments were used to monitor the amount of plutonium sorbed to high-purity quartz as a function of time, pH, and total alpha radioactivity. Three systems were prepared using both (238)Pu and (242)Pu in order to increase the total alpha radioactivity of the mineral suspensions while maintaining a constant plutonium concentration. The fraction of sorbed plutonium increased with increasing time and pH regardless of the total alpha radioactivity of the system. Increasing the total alpha radioactivity of the solution had a negligible effect on the sorption rate. This indicated that surface-mediated reduction of Pu(V) in these systems was not due to radiolysis. Additionally, literature values for the Pu(V) disproportionation rate constant did not describe the experimental results. Therefore, Pu(V) disproportionation was also not a main driver for surface-mediated reduction of plutonium. Batch desorption experiments and X-ray absorption near edge structure spectroscopy were used to show that Pu(IV) was the dominant oxidation state of sorbed plutonium. Thus, it appears that the observed surface-mediated reduction of Pu(V) in the presence of high-purity quartz was based on the thermodynamic favorability of a Pu(IV) surface complex.

  15. Neutron-induced fission of even- and odd-mass plutonium isotopes within a four-dimensional Langevin framework

    NASA Astrophysics Data System (ADS)

    Pahlavani, M. R.; Mirfathi, S. M.

    2017-07-01

    Neutron multiplicity prior to scission and evaluation of mass distribution of fission fragments with the fission time scale for neutron induced fission of plutonium isotopes are investigated using a dynamical Langevin approach. Also, mass yield of fragments and prompt neutron multiplicity in different time scales of the fission process are compared with experimental data. Reasonable agreement is achieved between calculated and available experimental data.

  16. Tracing the dispersion of contaminated sediment with plutonium isotope measurements in coastal catchments of Fukushima Prefecture

    NASA Astrophysics Data System (ADS)

    Evrard, Olivier; Pointurier, Fabien; Onda, Yuichi; Chartin, Caroline; Hubert, Amélie; Lepage, Hugo; Pottin, Anne-Claire; Lefèvre, Irène; Bonté, Philippe; Laceby, J. Patrick; Ayrault, Sophie

    2015-04-01

    The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident led to important releases of radionuclides into the environment, and trace levels of plutonium (Pu) were detected in northeastern Japan. However, measurement of Pu isotopic atom and activity ratios is required to differentiate between the contributions of global nuclear test fallout and FDNPP emissions. In this study, we measured Pu isotopic ratios in recently deposited sediments along rivers draining the most contaminated part of the inland radioactive plume. To this end, we carried out a thorough chemical purification and concentration of Pu from sediment samples (5 g dry material) and precise isotopic measurements using a double-focusing sector field ICP-MS. Results showed that the entire range of measured Pu isotopes (i.e., 239Pu, 240Pu, 241Pu, and 242Pu) were detected in all samples, although in extremely low concentrations. The 241Pu/239Pu atom ratios measured in sediment deposits (0.0017-0.0884) were significantly higher than the corresponding values attributed to the global fallout (0.00113±0.00008 on average in the Northern Hemisphere between 31°-71°N). The results indicated the presence of Pu from FDNPP, in slight excess compared to the Pu background from global fallout, representing up to ca. 60% of Pu in the analyzed samples. These results demonstrate that this radionuclide has been transported relatively long distances (45 km) from FDNPP and deposited in rivers representing a potential source of Pu to the ocean.

  17. Novel insights into Fukushima nuclear accident from isotopic evidence of plutonium spread along coastal rivers.

    PubMed

    Evrard, Olivier; Pointurier, Fabien; Onda, Yuichi; Chartin, Caroline; Hubert, Amélie; Lepage, Hugo; Pottin, Anne-Claire; Lefèvre, Irène; Bonté, Philippe; Laceby, J Patrick; Ayrault, Sophie

    2014-08-19

    The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident led to important releases of radionuclides into the environment, and trace levels of plutonium (Pu) were detected in northeastern Japan. However, measurements of Pu isotopic atom and activity ratios are required to differentiate between the contributions of global nuclear test fallout and FDNPP emissions. In this study, we used a double-focusing sector field ICP-MS to measure Pu atom and activity ratios in recently deposited sediment along rivers draining the most contaminated part of the inland radioactive plume. Results showed that plutonium isotopes (i.e., (239)Pu, (240)Pu, (241)Pu, and (242)Pu) were detected in all samples, although in extremely low concentrations. The (241)Pu/(239)Pu atom ratios measured in sediment deposits (0.0017-0.0884) were significantly higher than the corresponding values attributed to the global fallout (0.00113 ± 0.00008 on average for the Northern Hemisphere between 31°-71° N: Kelley, J. M.; Bond, L. A.; Beasley, T. M. Global distribution of Pu isotopes and (237)Np. Sci. Total. Env. 1999, 237/238, 483-500). The results indicated the presence of Pu from FDNPP, in slight excess compared to the Pu background from global fallout that represented up to ca. 60% of Pu in the analyzed samples. These results demonstrate that this radionuclide has been transported relatively long distances (∼45 km) from FDNPP and been deposited in rivers representing a potential source of Pu to the ocean. In future, the high (241)Pu/(239)Pu atom ratio of the Fukushima accident sourced-Pu should be measured to quantify the supply of continental-originating material from Fukushima Prefecture to the Pacific Ocean.

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

    DOE PAGES

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

    2015-01-16

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

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

    SciTech Connect

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

    2015-01-16

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

  20. Gamma-ray isotopic analysis of plutonium within highly attenuating shipping containers

    SciTech Connect

    Hypes, P. A.; Mercer, D. J.; Dinwiddie, D. R.

    2001-01-01

    Isotopic measurements of items stored in shielded shipping containers presents a challenge to standard, nondestructive high-resolution gamma spectroscopy analysis. For example, some plutonium oxide material that will be shipped from Rocky Flats will be packaged in a combination of containers that places more than 12 mm of lead and 25 mm of steel between the material and the detector. This shielding effectively eliminates gamma rays below approximately 300 keV. Spectra were taken through simulated containers and analyzed using FRAM version 4.0 and a parameter set developed for use with highly attenuated items. The results indicate that 10% precision in measured {sup 240}Pu content should be achievable with 2-hour measurements.

  1. Utilization of non-weapons-grade plutonium and highly enriched uranium with breeding of the 233U isotope in the VVER reactors using thorium and heavy water

    NASA Astrophysics Data System (ADS)

    Marshalkin, V. E.; Povyshev, V. M.

    2015-12-01

    A method for joint utilization of non-weapons-grade plutonium and highly enriched uranium in the thorium-uranium—plutonium oxide fuel of a water-moderated reactor with a varying water composition (D2O, H2O) is proposed. The method is characterized by efficient breeding of the 233U isotope and safe reactor operation and is comparatively simple to implement.

  2. Activities of Pu and Am isotopes and isotopic ratios in a soil contaminated by weapons-grade plutonium.

    PubMed

    Lee, M H; Clark, S B

    2005-08-01

    An accident and fire at the former McGuire Air Force Base and Boeing Michigan Aeronautical Research Center (BOMARC) site in New Jersey resulted in dispersion of weapons-grade plutonium in particulate form to the local environment. Soil samples collected at the BOMARC site were measured for their activities and isotopic ratios of Pu and Am isotopes by radioanalytical techniques. The activities of the Pu and Am isotopes in the BOMARC soil were markedly higher than fallout levels, and they decreased nearly exponentially with increasing particle size of the soil. The measured (241)Am activity was compared to calculated values based on decay of (241)Pu. The activity ratios of (238)Pu/(239,240)Pu, (241)Pu/(239,240)Pu, and (241)Am/(239,240)Pu observed in the BOMARC soil were much lower than those attributed to nuclear reprocessing plants and Chernobyl fallout. From the activity ratios of (241)Pu/(239,240)Pu and (241)Am/(239,240)Pu, the origin of the Pu isotopes was identified as weapons-grade and the time since production of the material was estimated. Furthermore, the atomic ratio of (240)Pu/(239)Pu in the BOMARC soil was remarkably lower than the fallout value influenced by nuclear weapons testing and the Chernobyl accident. The atomic ratio of (240)Pu/(239)Pu was very close to the value of the weapons-grade Pu detected from the Thule accident in Greenland. This work demonstrates the utility of radioanalytical measurements and decay calculations for defining characteristics of the source term and discriminating multiple processes that contribute to a source. Such an approach would also be needed to respond to a terrorist event involving an improvised nuclear device or radiological dispersal device.

  3. Enclosure from DOE letter dated 7/20/07 - Table 5-2, Isotopic Compositions of Rocky Flats Plutonium and Uranium

    EPA Pesticide Factsheets

    This enclosure from a DOE letter to EPA regarding a waste container disposed at the WIPP from the Advanced Mixed Waste Treatment Project includes Table 5-2, Isotopic Compositions of Rocky Flats Plutonium and Uranium.

  4. Plutonium isotopic analysis system for plutonium samples enriched in sup 238 Pu in EP 60/61 and fuel-clad containers

    SciTech Connect

    Ruhter, W.D.

    1991-07-01

    This user's manual is addressed to the Hanford Site personnel (routine operators and supervisors) who perform measurements with the Pu-238 isotopic analysis system. Each chapter begins with a table of contents that lists the section titles, illustrations, and tabular data presented in that chapter. The first chapter in this manual is an introduction to the system. Chapter 2 lists required settings for the system's commercial nuclear instrument modules. System operating procedures are given in Chapter 3. Chapter 4 contains routine and supervisorial operator interactions. Chapter 5 describes the system's short- and long-printout output formats. Chapter 6 gives instructions for changing system parameters. Error messages are listed and described in Chapter 7. Chapter 8 contains reference articles on measuring relative plutonium isotopics in solid samples.

  5. Critical Need for Plutonium and Uranium Isotopic Standards with Lower Uncertainties

    DOE PAGES

    Mathew, Kattathu Joseph; Stanley, Floyd E.; Thomas, Mariam R.; ...

    2016-09-23

    Certified reference materials (CRMs) traceable to national and international safeguards database are a critical prerequisite for ensuring that nuclear measurement systems are free of systematic biases. CRMs are used to validate measurement processes associated with nuclear analytical laboratories. Diverse areas related to nuclear safeguards are impacted by the quality of the CRM standards available to analytical laboratories. These include: nuclear forensics, radio-chronometry, national and international safeguards, stockpile stewardship, nuclear weapons infrastructure and nonproliferation, fuel fabrication, waste processing, radiation protection, and environmental monitoring. For the past three decades the nuclear community is confronted with the strange situation that improvements in measurementmore » data quality resulting from the improved accuracy and precision achievable with modern multi-collector mass spectrometers could not be fully exploited due to large uncertainties associated with CRMs available from New Brunswick Laboratory (NBL) that are used for instrument calibration and measurement control. Similar conditions prevail for both plutonium and uranium isotopic standards and for impurity element standards in uranium matrices. Herein, the current status of U and Pu isotopic standards available from NBL is reviewed. Critical areas requiring improvement in the quality of the nuclear standards to enable the U. S. and international safeguards community to utilize the full potential of modern multi-collector mass spectrometer instruments are highlighted.« less

  6. Critical Need for Plutonium and Uranium Isotopic Standards with Lower Uncertainties

    SciTech Connect

    Mathew, Kattathu Joseph; Stanley, Floyd E.; Thomas, Mariam R.; Spencer, Khalil J.; Colletti, Lisa Michelle; Tandon, Lav

    2016-09-23

    Certified reference materials (CRMs) traceable to national and international safeguards database are a critical prerequisite for ensuring that nuclear measurement systems are free of systematic biases. CRMs are used to validate measurement processes associated with nuclear analytical laboratories. Diverse areas related to nuclear safeguards are impacted by the quality of the CRM standards available to analytical laboratories. These include: nuclear forensics, radio-chronometry, national and international safeguards, stockpile stewardship, nuclear weapons infrastructure and nonproliferation, fuel fabrication, waste processing, radiation protection, and environmental monitoring. For the past three decades the nuclear community is confronted with the strange situation that improvements in measurement data quality resulting from the improved accuracy and precision achievable with modern multi-collector mass spectrometers could not be fully exploited due to large uncertainties associated with CRMs available from New Brunswick Laboratory (NBL) that are used for instrument calibration and measurement control. Similar conditions prevail for both plutonium and uranium isotopic standards and for impurity element standards in uranium matrices. Herein, the current status of U and Pu isotopic standards available from NBL is reviewed. Critical areas requiring improvement in the quality of the nuclear standards to enable the U. S. and international safeguards community to utilize the full potential of modern multi-collector mass spectrometer instruments are highlighted.

  7. Critical Need for Plutonium and Uranium Isotopic Standards with Lower Uncertainties

    SciTech Connect

    Mathew, Kattathu Joseph; Stanley, Floyd E.; Thomas, Mariam R.; Spencer, Khalil J.; Colletti, Lisa Michelle; Tandon, Lav

    2016-09-23

    Certified reference materials (CRMs) traceable to national and international safeguards database are a critical prerequisite for ensuring that nuclear measurement systems are free of systematic biases. CRMs are used to validate measurement processes associated with nuclear analytical laboratories. Diverse areas related to nuclear safeguards are impacted by the quality of the CRM standards available to analytical laboratories. These include: nuclear forensics, radio-chronometry, national and international safeguards, stockpile stewardship, nuclear weapons infrastructure and nonproliferation, fuel fabrication, waste processing, radiation protection, and environmental monitoring. For the past three decades the nuclear community is confronted with the strange situation that improvements in measurement data quality resulting from the improved accuracy and precision achievable with modern multi-collector mass spectrometers could not be fully exploited due to large uncertainties associated with CRMs available from New Brunswick Laboratory (NBL) that are used for instrument calibration and measurement control. Similar conditions prevail for both plutonium and uranium isotopic standards and for impurity element standards in uranium matrices. Herein, the current status of U and Pu isotopic standards available from NBL is reviewed. Critical areas requiring improvement in the quality of the nuclear standards to enable the U. S. and international safeguards community to utilize the full potential of modern multi-collector mass spectrometer instruments are highlighted.

  8. Direct isotope ratio analysis of individual uranium-plutonium mixed particles with various U/Pu ratios by thermal ionization mass spectrometry.

    PubMed

    Suzuki, Daisuke; Esaka, Fumitaka; Miyamoto, Yutaka; Magara, Masaaki

    2015-02-01

    Uranium and plutonium isotope ratios in individual uranium-plutonium (U-Pu) mixed particles with various U/Pu atomic ratios were analyzed without prior chemical separation by thermal ionization mass spectrometry (TIMS). Prior to measurement, micron-sized particles with U/Pu ratios of 1, 5, 10, 18, and 70 were produced from uranium and plutonium certified reference materials. In the TIMS analysis, the peaks of americium, plutonium, and uranium ion signals were successfully separated by continuously increasing the evaporation filament current. Consequently, the uranium and plutonium isotope ratios, except the (238)Pu/(239)Pu ratio, were successfully determined for the particles at all U/Pu ratios. This indicates that TIMS direct analysis allows for the measurement of individual U-Pu mixed particles without prior chemical separation.

  9. Ultra-low level plutonium isotopes in the NIST SRM 4355A (Peruvian Soil-1).

    PubMed

    Inn, Kenneth G W; LaRosa, Jerome; Nour, Svetlana; Brooks, George; LaMont, Steve; Steiner, Rob; Williams, Ross; Patton, Brad; Bostick, Debbie; Eiden, Gregory; Petersen, Steve; Douglas, Matthew; Beals, Donna; Cadieux, James; Hall, Greg; Goldberg, Steve; Vogt, Stephan

    2009-05-01

    For more than 20 years, countries and their agencies which monitor radionuclide discharge sites and storage facilities have relied on the National Institute of Standards and Technology (NIST) Standard Reference Material (SRM) 4355 Peruvian Soil. Its low fallout contamination makes it an ideal soil blank for measurements associated with terrestrial-pathway-to-man studies. Presently, SRM 4355 is out of stock, and a new batch of the Peruvian soil is currently under development as future NIST SRM 4355A. Both environmental radioanalytical laboratories and mass spectrometry communities will benefit from the use of this SRM. The former must assess their laboratory procedural contamination and measurement detection limits by measurement of blank sample material. The Peruvian Soil is so low in anthropogenic radionuclide content that it is a suitable virtual blank. On the other hand, mass spectrometric laboratories have high sensitivity instruments that are capable of quantitative isotopic measurements at low plutonium levels in the SRM 4355 (first Peruvian Soil SRM) that provided the mass spectrometric community with the calibration, quality control, and testing material needed for methods development and legal defensibility. The quantification of the ultra-low plutonium content in the SRM 4355A was a considerable challenge for the mass spectrometric laboratories. Careful blank control and correction, isobaric interferences, instrument stability, peak assessment, and detection assessment were necessary. Furthermore, a systematic statistical evaluation of the measurement results and considerable discussions with the mass spectroscopy metrologists were needed to derive the certified values and uncertainties. The one sided upper limit of the 95% tolerance with 95% confidence for the massic (239)Pu content in SRM 4355A is estimated to be 54,000 atoms/g.

  10. Preparation of a multi-isotope plutonium AMS standard and preliminary results of a first inter-lab comparison

    NASA Astrophysics Data System (ADS)

    Dittmann, B.-A.; Dunai, T. J.; Dewald, A.; Heinze, S.; Feuerstein, C.; Strub, E.; Fifield, L. K.; Froehlich, M. B.; Tims, S. G.; Wallner, A.; Christl, M.

    2015-10-01

    The motivation of this work is to establish a new multi-isotope plutonium standard for isotopic ratio measurements with accelerator mass spectrometry (AMS), since stocks of existing solutions are declining. To this end, certified reference materials (CRMs) of each of the individual isotopes 239Pu, 240Pu, 242Pu and 244Pu were obtained from JRC IRMM (Joint Research Center Institute for Reference Materials and Measurements). These certified reference materials (IRMM-081a, IRMM-083, IRMM-043 and IRMM-042a) were diluted with nitric acid and mixed to obtain a stock standard solution with an isotopic ratio of approximately 1.0:1.0:1.0:0.1 (239Pu:240Pu:242Pu:244Pu). From this stock solution, samples were prepared for measurement of the plutonium isotopic composition by AMS. These samples have been measured in a round-robin exercise between the AMS facilities at CologneAMS, at the ANU Canberra and ETH Zurich to verify the isotopic ratio and to demonstrate the reproducibility of the measurements. The results show good agreement both between the different AMS measurements and with the gravimetrically determined nominal ratios.

  11. Plutonium isotopes in the atmosphere of Central Europe: Isotopic composition and time evolution vs. circulation factors.

    PubMed

    Kierepko, Renata; Mietelski, Jerzy W; Ustrnul, Zbigniew; Anczkiewicz, Robert; Wershofen, Herbert; Holgye, Zoltan; Kapała, Jacek; Isajenko, Krzysztof

    2016-11-01

    This paper reports evidence of Pu isotopes in the lower part of the troposphere of Central Europe. The data were obtained based on atmospheric aerosol fraction samples collected from four places in three countries (participating in the informal European network known as the Ring of Five (Ro5)) forming a cell with a surface area of about 200,000km(2). We compared our original data sets from Krakow (Poland, 1990-2007) and Bialystok (Poland, 1991-2007) with the results from two other locations, Prague (Czech Republic; 1997-2004) and Braunschweig (Germany; 1990-2003) to find time evolution of the Pu isotopes. The levels of the activity concentration for (238)Pu and for ((239+240))Pu were estimated to be a few and some tens of nBqm(-3), respectively. However, we also noted some results were much higher (even about 70 times higher) than the average concentration of (238)Pu in the atmosphere. The achieved complex data sets were used to test a new approach to the problem of solving mixing isotopic traces from various sources (here up to three) in one sample. Results of our model, supported by mesoscale atmospheric circulation parameters, suggest that Pu from nuclear weapon accidents or tests and nuclear burnt-up fuel are present in the air.

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

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

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

  13. Plutonium isotopes derived from Nagasaki atomic bomb in the sediment of Nishiyama reservoir at Nagasaki, Japan.

    PubMed

    Saito-Kokubu, Y; Esaka, F; Yasuda, K; Magara, M; Miyamoto, Y; Sakurai, S; Usuda, S; Yamazaki, H; Yoshikawa, S; Nagaoka, S

    2007-04-01

    The source of plutonium in sediments deposited at Nishiyama reservoir at Nagasaki was characterized by their (240)Pu/(239)Pu atom ratio. The average ratio was approximately 0.03, except in two layers. The main source of the plutonium was the Nagasaki atomic bomb. The plutonium continues to flow into the reservoir even now. The (240)Pu/(239)Pu atom ratios in two layers were higher than the average, which showed that plutonium in these layers were made of those of nuclear tests added to those of the atomic bomb.

  14. Determination of plutonium isotopes ((238,239,240)Pu) and strontium ((90)Sr) 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.

  15. MGA (Multi-Group Analysis): A gamma-ray spectrum analysis code for determining plutonium isotopic abundances

    SciTech Connect

    Gunnink, R

    1990-04-03

    Nondestructive measurements of x-ray and gamma-ray emissions can be used to analyze a sample for plutonium. This report describes the methods and algorithms we have developed for analyzing gamma-ray spectra obtained by using a germanium detector system to accurately determine the relative abundances of various actinide isotopes in a sample. Our methodology requires no calibrations and can be used to measure virtually any size and type of plutonium sample. Measurement times can be as short as a few minutes; measurements are frequently accurate to within 1%. Our methods have been programmed into a computerized analysis code called MGA (Multi-Group Analysis). Our current versions can be run on personal computers (IBM type) and on the DEC VAX microcomputer. Spectral analysis times are usually far less than a minute. 28 refs., 26 figs., 1 tab.

  16. Utilization of non-weapons-grade plutonium and highly enriched uranium with breeding of the {sup 233}U isotope in the VVER reactors using thorium and heavy water

    SciTech Connect

    Marshalkin, V. E. Povyshev, V. M.

    2015-12-15

    A method for joint utilization of non-weapons-grade plutonium and highly enriched uranium in the thorium–uranium—plutonium oxide fuel of a water-moderated reactor with a varying water composition (D{sub 2}O, H{sub 2}O) is proposed. The method is characterized by efficient breeding of the {sup 233}U isotope and safe reactor operation and is comparatively simple to implement.

  17. A Heterogeneous Sodium Fast Reactor Designed to Transmute Minor Actinide Actinide Waste Isotopes into Plutonium Fuel

    SciTech Connect

    Samuel E. Bays

    2011-02-01

    An axial heterogeneous sodium fast reactor design is developed for converting minor actinide waste isotopes into plutonium fuel. The reactor design incorporates zirconium hydride moderating rods in an axial blanket above the active core. The blanket design traps the active core’s axial leakage for the purpose of transmuting Am-241 into Pu-238. This Pu-238 is then co-recycled with the spent driver fuel to make new driver fuel. Because Pu-238 is significantly more fissile than Am-241 in a fast neutron spectrum, the fissile worth of the initial minor actinide material is upgraded by its preconditioning via transmutation in the axial targets. Because, the Am-241 neutron capture worth is significantly stronger in a moderated epithermal spectrum than the fast spectrum, the axial targets serve as a neutron trap which recovers the axial leakage lost by the active core. The sodium fast reactor proposed by this work is designed as an overall transuranic burner. Therefore, a low transuranic conversion ratio is achieved by a degree of core flattening which increases axial leakage. Unlike a traditional “pancake” design, neutron leakage is recovered by the axial target/blanket system. This heterogeneous core design is constrained to have sodium void and Doppler reactivity worth similar to that of an equivalent homogeneous design. Because minor actinides are irradiated only once in the axial target region; elemental partitioning is not required. This fact enables the use of metal targets with electrochemical reprocessing. Therefore, the irradiation environment of both drivers and targets was constrained to ensure applicability of the established experience database for metal alloy sodium fast reactor fuels.

  18. Using radiosilver and plutonium isotopes to trace the dispersion of contaminated sediment in Fukushima coastal catchments

    NASA Astrophysics Data System (ADS)

    Evrard, O.; Ayrault, S.; Pointurier, F.; Onda, Y.; Laceby, J. P.; Lepage, H.; Chartin, C.; Cirella, M.; Pottin, A. C.; Hubert, A.; Lefèvre, I.

    2015-12-01

    The Fukushima Dai-ichi nuclear power plant (FDNPP) accident in March 2011 resulted in a 3000-km² radioactive pollution plume consisting predominantly of radiocesium (137Cs and 134Cs). This plume is drained by several rivers to the Pacific Ocean after flowing through less contaminated, but densely inhabited coastal plains. As the redistribution of radionuclide contaminated sediment could expose the local population to higher radiation rates, novel fingerprinting methods were developed to trace the downstream dispersion of contaminated sediment. First, the heterogeneous deposition of metastable silver-110 (110mAg) across these coastal catchments was used to investigate sediment migration. In particular, the 110mAg/137Cs activity ratio was measured in soils and river sediment demonstrating the occurrence of a seasonal cycle of soil erosion during typhoons and spring snowmelt in 2011 and 2012. However, due to the rapid decay of 110mAg (half-life of 250 days), alternative methods were required to continue tracking sediment from 2013 onwards. One promising method includes the analyses of plutonium isotopes to further understand sediment migration in the Fukushima region. For example, 241Pu/239Pu atom ratios measured in sediment collected in Fukushima coastal rivers shortly after the accident were shown to be significantly higher (0.0017 - 0.0884) than corresponding values attributed to the global fallout (0.00113 ± 0.00008). Additional analyses were conducted on sediment sampled in 2013 and 2014 after the start of decontamination works. These analyses show that the 241Pu/239Pu atom ratios decreased towards the global fallout values in rivers draining decontaminated paddy fields, demonstrating the effectiveness of remediation works.

  19. Some neutron and gamma radiation characteristics of plutonium cermet fuel for isotopic power sources

    NASA Technical Reports Server (NTRS)

    Neff, R. A.; Anderson, M. E.; Campbell, A. R.; Haas, F. X.

    1972-01-01

    Gamma and neutron measurements on various types of plutonium sources are presented in order to show the effects of O-17, O-18 F-19, Pu-236, age of the fuel, and size of the source on the gamma and neutron spectra. Analysis of the radiation measurements shows that fluorine is the main contributor to the neutron yields from present plutonium-molybdenum cermet fuel, while both fluorine and Pu-236 daughters contribute significantly to the gamma ray intensities.

  20. Use of plutonium isotope activity ratios in dating recent sediments. [/sup 238/Pu//sup 239/Pu + /sup 240/Pu

    SciTech Connect

    Beasley, T. M.

    1982-01-01

    The majority of plutonium presently in the biosphere has come from the testing of nuclear devices. In the early 1950s, the Pu-238/239+240 activity ratio of fallout debris was > 0.04; in the more extensive test series of 1961 to 1962, the Pu-238/239+240 activity ratios were quite consistent at 0.02 to 0.03 and maximum fallout delivery occurred in mid-1963. A significant perturbation in Pu isotope activity ratios occurred in mid-1966 with the deposition of Pu-238 from the SNAP-9A reentry and burn-up. Recently deposited sediments have recorded these events and where accumulation rates are rapid (> 1 cm/y), changes in Pu isotope activity ratios can be used as a geochronological tool.

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

    SciTech Connect

    Liezers, Martin; Olsen, Khris B.; Mitroshkov, Alexandre V.; Duckworth, Douglas C.

    2010-08-11

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

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

    SciTech Connect

    Liezers, Martin; Lehn, Scott A; Olsen, Khris B; Farmer, Orville T; Duckworth, Douglas C

    2009-10-01

    Electrochemically modulated separations (EMS) are shown to be a rapid and selective means of extracting and concentrating Pu from complex solutions prior to isotopic analysis by inductively coupled plasma mass spectrometry (ICP-MS). This separation is performed in a flow injection mode, on-line with the ICP-MS. A three-electrode, flow-by electrochemical cell is used to accumulate Pu at an anodized glassy carbon electrode by redox conversion of Pu(III) to Pu (IV&VI). The entire process takes place in 2% v/v (0.46M) HNO3. No redox chemicals or acid concentration changes are required. Plutonium accumulation and release is redox dependent and controlled by the applied cell potential. Thus large transient volumetric concentration enhancements can be achieved. Based on more negative U(IV) potentials relative to Pu(IV), separation of Pu from uranium is efficient, thereby eliminating uranium hydride interferences. EMS-ICP-MS isotope ratio measurement performance will be presented for femtogram to attogram level plutonium concentrations.

  3. Thermal Safety Analyses for the Production of Plutonium-238 at the High Flux Isotope Reactor

    SciTech Connect

    Hurt, Christopher J.; Freels, James D.; Hobbs, Randy W.; Jain, Prashant K.; Maldonado, G. Ivan

    2016-08-01

    There has been a considerable effort over the previous few years to demonstrate and optimize the production of plutonium-238 (238Pu) at the High Flux Isotope Reactor (HFIR). This effort has involved resources from multiple divisions and facilities at the Oak Ridge National Laboratory (ORNL) to demonstrate the fabrication, irradiation, and chemical processing of targets containing neptunium-237 (237Np) dioxide (NpO2)/aluminum (Al) cermet pellets. A critical preliminary step to irradiation at the HFIR is to demonstrate the safety of the target under irradiation via documented experiment safety analyses. The steady-state thermal safety analyses of the target are simulated in a finite element model with the COMSOL Multiphysics code that determines, among other crucial parameters, the limiting maximum temperature in the target. Safety analysis efforts for this model discussed in the present report include: (1) initial modeling of single and reduced-length pellet capsules in order to generate an experimental knowledge base that incorporate initial non-linear contact heat transfer and fission gas equations, (2) modeling efforts for prototypical designs of partially loaded and fully loaded targets using limited available knowledge of fabrication and irradiation characteristics, and (3) the most recent and comprehensive modeling effort of a fully coupled thermo-mechanical approach over the entire fully loaded target domain incorporating burn-up dependent irradiation behavior and measured target and pellet properties, hereafter referred to as the production model. These models are used to conservatively determine several important steady-state parameters including target stresses and temperatures, the limiting condition of which is the maximum temperature with respect to the melting point. The single pellet model results provide a basis for the safety of the irradiations, followed by parametric analyses in the initial prototypical designs that were necessary due to the

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

    PubMed

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

    2007-03-28

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

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

    SciTech Connect

    Lastres, Oscar; Chandler, David; Jarrell, Joshua J; Maldonado, G. Ivan

    2011-01-01

    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 control 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 reactor

  6. Determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using radiochemical separation combined with radiometric and mass spectrometric measurements.

    PubMed

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

    2014-02-01

    This paper reports an analytical method for the determination of plutonium isotopes ((238)Pu, (239)Pu, (240)Pu, (241)Pu) in environmental samples using anion exchange chromatography in combination with extraction chromatography for chemical separation of Pu. Both radiometric methods (liquid scintillation counting and alpha spectrometry) and inductively coupled plasma mass spectrometry (ICP-MS) were applied for the measurement of plutonium isotopes. The decontamination factors for uranium were significantly improved up to 7.5 × 10(5) for 20 g soil compared to the level reported in the literature, this is critical for the measurement of plutonium isotopes using mass spectrometric technique. Although the chemical yield of Pu in the entire procedure is about 55%, the analytical results of IAEA soil 6 and IAEA-367 in this work are in a good agreement with the values reported in the literature or reference values, revealing that the developed method for plutonium determination in environmental samples is reliable. The measurement results of (239+240)Pu by alpha spectrometry agreed very well with the sum of (239)Pu and (240)Pu measured by ICP-MS. ICP-MS can not only measure (239)Pu and (240)Pu separately but also (241)Pu. However, it is impossible to measure (238)Pu using ICP-MS in environmental samples even a decontamination factor as high as 10(6) for uranium was obtained by chemical separation.

  7. Plutonium story

    SciTech Connect

    Seaborg, G T

    1981-09-01

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

  8. Plutonium Story

    DOE R&D Accomplishments Database

    Seaborg, G. T.

    1981-09-01

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

  9. Combined application of alpha-track and fission-track techniques for detection of plutonium particles in environmental samples prior to isotopic measurement using thermo-ionization mass spectrometry.

    PubMed

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

    2011-07-15

    The fission track technique is a sensitive detection method for particles which contain radio-nuclides like (235)U or (239)Pu. However, when the sample is a mixture of plutonium and uranium, discrimination between uranium particles and plutonium particles is difficult using this technique. In this study, we developed a method for detecting plutonium particles in a sample mixture of plutonium and uranium particles using alpha track and fission track techniques. The specific radioactivity (Bq/g) for alpha decay of plutonium is several orders of magnitude higher than that of uranium, indicating that the formation of the alpha track due to alpha decay of uranium can be disregarded under suitable conditions. While alpha tracks in addition to fission tracks were detected in a plutonium particle, only fission tracks were detected in a uranium particle, thereby making the alpha tracks an indicator for detecting particles containing plutonium. In addition, it was confirmed that there is a linear relationship between the numbers of alpha tracks produced by plutonium particles made of plutonium certified standard material and the ion intensities of the various plutonium isotopes measured by thermo-ionization mass spectrometry. Using this correlation, the accuracy in isotope ratios, signal intensity and measurement errors is presumable from the number of alpha tracks prior to the isotope ratio measurements by thermal ionization mass spectrometry. It is expected that this method will become an effective tool for plutonium particle analysis. The particles used in this study had sizes between 0.3 and 2.0 μm.

  10. MGA: A gamma-ray spectrum analysis code for determining plutonium isotopic abundances. Volume 3, FORTRAN listing of the GA code

    SciTech Connect

    Gunnink, R

    1991-09-01

    Nondestructive measurements of x-ray and gamma-ray emissions can be used to determine the abundances of various actinides in a sample. Volume 1 of this report describes the methods and algorithms we have developed to determine the relative isotopic abundances of actinides in a sample, by analyzing gamma-ray spectra obtained using germanium detector systems. Volume 2 is a guide to using the MGA (Multiple Group Analysis) computer program we have written to perform plutonium isotopic analyses. This report contains a listing of the FORTRAN instructions of the code.

  11. Identifying Sources of Non-fallout Nuclear Contamination in Hudson River Sediments by Plutonium and Neptunium isotope ratios.

    NASA Astrophysics Data System (ADS)

    Kenna, T. C.; Chillrud, S. N.

    2002-12-01

    In an effort to identify and characterize nuclear contaminants released from sources contained within the Hudson River drainage basin, Pu isotopes and 237Np have been measured in a series of sediment cores collected from various locations within the region. During the last several decades, the Hudson River has received input of radioactive contamination from several sources. The first and most significant, has been global fallout, which was a result of atmospheric testing of nuclear weapons primarily by governments of the United States and Former Soviet Union in the 1950s and 1960s. The second, is contamination resulting from reactor releases at the Indian Point Nuclear Power Plant (IPNPP) located on the Hudson River about 35 miles north of New York City. This facility began operation in 1962. A third source of radioactive contamination to the region is contamination resulting from activities at the Knolls Atomic Power Laboratory (KAPL) located on the Mohawk River, which began operation in 1946. Our research entails identifying different sources of nuclear contamination by measurement of plutonium and neptunium isotopic ratios by inductively coupled plasma mass spectrometry (ICP-MS). The isotopic composition of a nuclear contaminant is a sensitive indicator of its origin. By comparing the isotopic composition measured in fluvial sediments to mean values reported for global fallout (i.e. 240Pu/239Pu = 0.18 ñ 0.014, 237Np/239Pu = 0.48 ñ 0.07, and 241Pu/239Pu = .00194 ñ 00028) it is possible to identify contaminants as non-fallout in origin. To date, we have analyzed selected samples from 3 sediment cores collected from the following locations: 1) the Mohawk River downstream of KAPL, 2) the Hudson River above its confluence with the Mohawk River, and 3) the lower Hudson River at a location in close proximity to IPNPP. Isotopic analysis of sediments from the Mohawk River indicates contamination that is clearly non-fallout in origin (240Pu/239Pu ranges between 0

  12. Plutonium 239 Equivalency Calculations

    SciTech Connect

    Wen, J

    2011-05-31

    This document provides the basis for converting actual weapons grade plutonium mass to a plutonium equivalency (PuE) mass of Plutonium 239. The conversion can be accomplished by performing calculations utilizing either: (1) Isotopic conversions factors (CF{sub isotope}), or (2) 30-year-old weapons grade conversion factor (CF{sub 30 yr}) Both of these methods are provided in this document. Material mass and isotopic data are needed to calculate PuE using the isotopic conversion factors, which will provide the actual PuE value at the time of calculation. PuE is the summation of the isotopic masses times their associated isotopic conversion factors for plutonium 239. Isotopic conversion factors are calculated by a normalized equation, relative to Plutonium 239, of specific activity (SA) and cumulated dose inhalation affects based on 50-yr committed effective dose equivalent (CEDE). The isotopic conversion factors for converting weapons grade plutonium to PuE are provided in Table-1. The unit for specific activity (SA) is curies per gram (Ci/g) and the isotopic SA values come from reference [1]. The cumulated dose inhalation effect values in units of rem/Ci are based on 50-yr committed effective dose equivalent (CEDE). A person irradiated by gamma radiation outside the body will receive a dose only during the period of irradiation. However, following an intake by inhalation, some radionuclides persist in the body and irradiate the various tissues for many years. There are three groups CEDE data representing lengths of time of 0.5 (D), 50 (W) and 500 (Y) days, which are in reference [2]. The CEDE values in the (W) group demonstrates the highest dose equivalent value; therefore they are used for the calculation.

  13. Preparation, certification and validation of a stable solid spike of uranium and plutonium coated with a cellulose derivative for the measurement of uranium and plutonium content in dissolved nuclear fuel by isotope dilution mass spectrometry.

    PubMed

    Surugaya, Naoki; Hiyama, Toshiaki; Verbruggen, André; Wellum, Roger

    2008-02-01

    A stable solid spike for the measurement of uranium and plutonium content in nitric acid solutions of spent nuclear fuel by isotope dilution mass spectrometry has been prepared at the European Commission Institute for Reference Materials and Measurements in Belgium. The spike contains about 50 mg of uranium with a 19.838% (235)U enrichment and 2 mg of plutonium with a 97.766% (239)Pu abundance in each individual ampoule. The dried materials were covered with a thin film of cellulose acetate butyrate as a protective organic stabilizer to resist shocks encountered during transportation and to eliminate flaking-off during long-term storage. It was found that the cellulose acetate butyrate has good characteristics, maintaining a thin film for a long time, but readily dissolving on heating with nitric acid solution. The solid spike containing cellulose acetate butyrate was certified as a reference material with certified quantities: (235)U and (239)Pu amounts and uranium and plutonium amount ratios, and was validated by analyzing spent fuel dissolver solutions of the Tokai reprocessing plant in Japan. This paper describes the preparation, certification and validation of the solid spike coated with a cellulose derivative.

  14. Improved precision and accuracy in quantifying plutonium isotope ratios by RIMS

    SciTech Connect

    Isselhardt, B. H.; Savina, M. R.; Kucher, A.; Gates, S. D.; Knight, K. B.; Hutcheon, I. D.

    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 presence of a significant quantity of 238U in the samples.

  15. 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 presence ofmore » a significant quantity of 238U in the samples.« less

  16. Improved precision and accuracy in quantifying plutonium isotope ratios by RIMS

    SciTech Connect

    Isselhardt, B. H.; Savina, M. R.; Kucher, A.; Gates, S. D.; Knight, K. B.; Hutcheon, I. D.

    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 Pu-240/Pu-239 ratios of 0.7 and 0.58 %, with precisions (95 % confidence intervals) of 1.49 and 0.91 %. The minor isotope Pu-238 was also quantified despite the presence of a significant quantity of U-238 in the samples.

  17. Characterisation of the plutonium isotopic composition of a sediment core from Palomares, Spain, by low-energy AMS and alpha-spectrometry

    NASA Astrophysics Data System (ADS)

    Chamizo, E.; Jiménez-Ramos, M. C.; Enamorado, S. M.; García-León, M.; García-Tenorio, R.; Mas, J. L.; Masqué, P.; Merino, J.; Sanchez-Cabeza, J. A.

    2010-04-01

    The measurement of plutonium isotopes, 239Pu and 240Pu, at 670 kV on the compact accelerator mass spectrometry (AMS) system at the Centro Nacional de Aceleradores (CNA) in Seville, Spain, is now a reality. In this work, we present first Pu AMS results for environmental samples: a sediment core collected in a submarine canyon in the Mediterranean coast of the Spanish region of Palomares, affected by a nuclear accident in 1966. From the study of the 240Pu/ 239Pu atomic ratio profile, showing on average levels lower than 11%, we confirm that the weapon-grade plutonium released on land during the accident, with a characteristic 240Pu/ 239Pu atomic ratio of 5.8%, has found its way into the marine environment. A two-plutonium sources mixture model (Palomares and fallout) is used to elucidate the percentage of the plutonium coming from the accident. As a validation exercise of the Pu AMS measuring technique and in order to obtain the 238Pu/ (239+240)Pu activity ratios, samples were also studied by alpha-spectrometry (AS). The obtained AS 239+240Pu activity concentration results fit in with the AMS ones in a wide dynamic range, thus validating the AMS technique.

  18. Measurement of uranium and plutonium in solid waste by passive photon or neutron counting and isotopic neutron source interrogation

    SciTech Connect

    Crane, T.W.

    1980-03-01

    A summary of the status and applicability of nondestructive assay (NDA) techniques for the measurement of uranium and plutonium in 55-gal barrels of solid waste is reported. The NDA techniques reviewed include passive gamma-ray and x-ray counting with scintillator, solid state, and proportional gas photon detectors, passive neutron counting, and active neutron interrogation with neutron and gamma-ray counting. The active neutron interrogation methods are limited to those employing isotopic neutron sources. Three generic neutron sources (alpha-n, photoneutron, and /sup 252/Cf) are considered. The neutron detectors reviewed for both prompt and delayed fission neutron detection with the above sources include thermal (/sup 3/He, /sup 10/BF/sub 3/) and recoil (/sup 4/He, CH/sub 4/) proportional gas detectors and liquid and plastic scintillator detectors. The instrument found to be best suited for low-level measurements (< 10 nCi/g) is the /sup 252/Cf Shuffler. The measurement technique consists of passive neutron counting followed by cyclic activation using a /sup 252/Cf source and delayed neutron counting with the source withdrawn. It is recommended that a waste assay station composed of a /sup 252/Cf Shuffler, a gamma-ray scanner, and a screening station be tested and evaluated at a nuclear waste site. 34 figures, 15 tables.

  19. Extraction Chromatographic Methods in the Sample Preparation Sequence for Thermal Ionization Mass Spectrometric Analysis of Plutonium Isotopes

    SciTech Connect

    Grate, Jay W.; O'Hara, Matthew J.; Farawila, Anne F.; Douglas, Matthew; Haney, Morgan M.; Peterson, Steve L.; Maiti, Tapas C.; Aardahl, Christopher L.

    2011-10-17

    A sample preparation sequence for actinide isotopic analysis by TIMS is described that includes column-based extraction chromatography as the first separation step, followed by anion exchange column separations. The sequence is designed to include a wet ashing step after the extraction chromatography to prevent any leached extractant or oxalic acid eluent reagents from interfering with subsequent separations, source preparation, or TIMS ionization. TEVA-resin and DGA-resin materials, containing extractants that consist only of C, N, O, and H atoms, were investigated for isolation of plutonium. Radiotracer level studies confirmed expected high yields from column-based separation procedures. Femtogram-level studies were carried out with TIMS detection, using multiple isotopic spikes through the separation sequence. Pu recoveries were 87% and 86% for TEVA- and DGA-resins separations respectively. The Pu recoveries from 400 {mu}L anion-exchange column separations were 89% and 93% for trial sequences incorporating TEVA and DGA-resin. Thus, a prior extraction chromatography step in the sequence did not interfere with the subsequent anion exchange separation when a simple wet ash step was carried out in between these column separations. The average measurement efficiency, for Pu, encompassing the chemical separation recoveries and the TIMS ionization efficiency, was 2.73 {+-} 0.77% (2-sigma) for the DGA-resin trials and 2.67 {+-} 0.54% for the TEVA-resin trials, compared to 3.41% and 2.37% (average 2.89%) for two spikes in the experimental set. These compare with an average measurement efficiency of 2.78 {+-} 1.70%, n = 33 from process benchmark analyses using Pu spikes processed through a sequence of oxalate precipitation, wet ash, iron hydroxide precipitation, and anion exchange column separations. We conclude that extraction chromatography can be a viable separation procedure as part of a multistep sequence for TIMS sample preparation.

  20. Sequential isotopic determination of plutonium, thorium, americium, strontium and uranium in environmental and bioassay samples.

    PubMed

    Wang, Jeng-Jong; Chen, Ing-Jane; Chiu, Jih-Hung

    2004-01-01

    A procedure has been developed to provide sequential analysis of 238Pu, 230Th, 241Am, 238U, and 90Sr in environmental and bioassay samples. Tracers and/or carriers (242Pu, 243Am, 232U, and stable strontium) are added into the sample as chemical yield monitors, and then, plutonium, thorium, strontium, americium, and uranium are sequentially separated and purified by Dowex ion-exchange resin, EiChroM Sr-resin, EiChroM TRU-resin, and Chelate-100 resin, respectively. The radioactivities of 90Sr and the actinides are measured using the liquid scintillation counter and alpha-particle spectrometer, respectively. Acidified water, glass-fiber air filter, soil, synthetic urine and synthetic feces samples of US National Institute of Standard and Technology Radiochemical Intercomparison Program(NRIP) were analyzed to verify this method. All the analytical results of 238Pu, 230Th, 90Sr, 241Am and 238U meet the traceability limit per ANSI N42.22, and when appropriate, evaluation of radiobioassay measurement bias and precision per ANSI N13.30.

  1. The effect of isotope on the dosimetry of inhaled plutonium oxide

    SciTech Connect

    Guilmette, R.A., Griffith, W.C.; Hickman, A.W.

    1991-12-31

    Results of experimental studies in which animals inhaled {sup 238}PuO{sub 2} or {sup 239}PuO{sub 2} aerosols have shown that the biokinetics and associated radiation dose patterns for these two isotopes differ significantly due to differences in in-vivo solubility caused by the 260-fold difference in specific activity between {sup 238}PuO{sub 2} and {sup 239}PuO{sub 2}. We have adapted a biokinetics and dosimetry model derived from results of the ITRI dog studies to humans and have calculated dose commitments and annual limits on intake (ALI) for both Pu isotopes. Our results show that the ALI calculated in this study is one-third that for class Y {sup 238}Pu from ICRP 30, and one-half or equal to that for class Y {sup 239}Pu, depending on how activity in the thoracic lymph nodes is treated dosimetrically.

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

    PubMed Central

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

    2012-01-01

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

  3. Determination of the Galaxy age by the method of uranium-thorium-plutonium isotopic ratios

    NASA Astrophysics Data System (ADS)

    Panov, I. V.; Lutostansky, Yu. S.; Eichler, M.; Thielemann, F.-K.

    2017-07-01

    The dependence of the Galaxy age ( T G), as determined by the method of uranium-thorium isotopic ratios, on the parameters of the nucleosynthesis model is studied within the theory of galactic nucleosynthesis. It is shown that TG depends strongly both on the scenario of the production of nuclei in the r-process and those features of neutron-rich nuclei that are used in the respective analysis and on galactic-nucleosynthesis parameters. The effect of a sudden nucleosynthesis spike before the formation of a solar system on the Galaxy age is evaluated. The region of admissible values of the parameters of galacticnucleosynthesis theory is discussed. The method of uranium-thorium isotopic ratios is supplemented with the 244Pu/238U ratio for yet another cosmochronometer pair, and the Galaxy age is estimated on the basis of the model modified in this way.

  4. Analysis of plutonium isotope ratios including (238)Pu/(239)Pu in individual U-Pu mixed oxide particles by means of a combination of alpha spectrometry and ICP-MS.

    PubMed

    Esaka, Fumitaka; Yasuda, Kenichiro; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki

    2017-04-01

    Isotope ratio analysis of individual uranium-plutonium (U-Pu) mixed oxide particles contained within environmental samples taken from nuclear facilities is proving to be increasingly important in the field of nuclear safeguards. However, isobaric interferences, such as (238)U with (238)Pu and (241)Am with (241)Pu, make it difficult to determine plutonium isotope ratios in mass spectrometric measurements. In the present study, the isotope ratios of (238)Pu/(239)Pu, (240)Pu/(239)Pu, (241)Pu/(239)Pu, and (242)Pu/(239)Pu were measured for individual Pu and U-Pu mixed oxide particles by a combination of alpha spectrometry and inductively coupled plasma mass spectrometry (ICP-MS). As a consequence, we were able to determine the (240)Pu/(239)Pu, (241)Pu/(239)Pu, and (242)Pu/(239)Pu isotope ratios with ICP-MS after particle dissolution and chemical separation of plutonium with UTEVA resins. Furthermore, (238)Pu/(239)Pu isotope ratios were able to be calculated by using both the (238)Pu/((239)Pu+(240)Pu) activity ratios that had been measured through alpha spectrometry and the (240)Pu/(239)Pu isotope ratios determined through ICP-MS. Therefore, the combined use of alpha spectrometry and ICP-MS is useful in determining plutonium isotope ratios, including (238)Pu/(239)Pu, in individual U-Pu mixed oxide particles. Copyright © 2016 Elsevier B.V. All rights reserved.

  5. Discrimination of source reactor type by multivariate statistical analysis of uranium and plutonium isotopic concentrations in unknown irradiated nuclear fuel material.

    PubMed

    Robel, Martin; Kristo, Michael J

    2008-11-01

    The problem of identifying the provenance of unknown nuclear material in the environment by multivariate statistical analysis of its uranium and/or plutonium isotopic composition is considered. Such material can be introduced into the environment as a result of nuclear accidents, inadvertent processing losses, illegal dumping of waste, or deliberate trafficking in nuclear materials. Various combinations of reactor type and fuel composition were analyzed using Principal Components Analysis (PCA) and Partial Least Squares Discriminant Analysis (PLSDA) of the concentrations of nine U and Pu isotopes in fuel as a function of burnup. Real-world variation in the concentrations of (234)U and (236)U in the fresh (unirradiated) fuel was incorporated. The U and Pu were also analyzed separately, with results that suggest that, even after reprocessing or environmental fractionation, Pu isotopes can be used to determine both the source reactor type and the initial fuel composition with good discrimination.

  6. Possible differences in biological availability of isotopes of plutonium: Report of a workshop

    SciTech Connect

    Kercher, J.R.; Gallegos, G.M.

    1993-09-01

    This paper presents the results of a workshop conducted on the apparent different bioavailability of isotopes {sup 238}Pu and {sup 239}Pu. There is a substantial body of evidence that {sup 238}Pu as commonly found in the environment is more biologically available than {sup 239}Pu. Studies of the Trinity Site, Nevada Test Site from nonnuclear and nuclear events, Rocky Flats, Enewetak and Bikini, and the arctic tundra support this conclusion and indicate that the bioavailability of {sup 238}Pu is more than an order of magnitude greater than that of {sup 239}Pu. Plant and soil studies from controlled environments and from Savannah River indicate no isotopic difference in availability of Pu to plants; whereas studies at the Trinity Site do suggest a difference. While it is possible that these observations can be explained by problems in the experimental procedure and analytical techniques, this possibility is remote given the ubiquitous nature of the observations. Studies of solubility of Pu in the stomach contents of cattle grazing at the Nevada Test Site and from fish from Bikini Atoll both found that {sup 238}Pu was more soluble than {sup 239}Pu. Studies of the Los Alamos effluent stream indicate that as particle size decreases, the content of {sup 238}Pu relative to {sup 239}Pu increases.

  7. Uranium, plutonium, and thorium isotopes in the atmosphere and the lithosphere

    SciTech Connect

    Essien, I.O.

    1983-01-01

    Concentration of /sup 238/U in rain and snow collected at Fayetteville (36/sup 0/N, 94/sup 0/W), Arkansas, showed a marked increase during the summer months of 1980, while Mount St. Helens remained active. This observed increase of /sup 238/U can be explained as due to the fallout of natural uranium from the eruption of Mount St. Helens. Large increases in the concentration of thorium isotopes detected in rain and snow samples during the last months of 1982 and early months of 1983 probably originated from the eruption of El Chichon volcano, which occurred on 28 March 1982. About 450 Ci of /sup 232/Th is estimated to have been injected into the atmosphere by this eruption. Isotopic anomalies were observed in atmospheric samples such as rain and snow. These anomalies can be attributed to various natural as well as man-made sources: nuclear weapon tests, nuclear accidents involving the burn-up of nuclear powered satellites, and volcanic eruptions. The variation of /sup 234/U//sup 238/U ratios in radioactive minerals when leached with nitric acid were also noticed and this variation, while /sup 235/U//sup 238/U remained fairly constant, can be explained in terms of the ..cap alpha..-recoil effect and changes in oxidation state of uranium. Difference found in /sup 239/Pu//sup 238/U ratios in terrestrial samples and uranium minerals can be explained as due to fallout contamination.

  8. Anomalous plutonium isotopic ratios in sediments of Lake Qinghai from the Qinghai-Tibetan Plateau, China.

    PubMed

    Wu, Fengchang; Zheng, Jian; Liao, Haiqing; Yamada, Masatoshi; Wan, Guojiang

    2011-11-01

    The vertical profiles of (239+240)Pu and (137)Cs activities and (240)Pu/(239)Pu isotopic ratios are determined for three sediment cores of Lake Qinghai from the Qinghai-Tibetan Plateau, China, and compared with those in sediments of another three lakes (Lakes Bosten, Sugan, and Shuangta), the only existing ones closest to Lop Nor area, China's nuclear weapons test site in the northwestern part of the country. The mean inventory of 47.7 ± 18.7 MBq km(-2) for (239+240)Pu activity in Lake Qinghai is comparable to the average value of global fallout expected at the same latitude, yet the mean inventory of 1112.0 ± 78.0 MBq km(-2) for (137)Cs is slightly lower than that of global fallout. Anomalously low (240)Pu/(239)Pu isotopic ratios (0.038-0.125) were found in the 3-6.5 cm deep sediment layers, indicating the trace Pu input from early nuclear weapons research activities at Atomic City in the lake's watershed during the 1950-60s. Model calculation indicated that the Pu input accounted for approximately 5-16% of the total Pu inventory. The observation of low (240)Pu/(239)Pu ratio in the deep sediment layer provided a new time marker for recent sediment dating in the lake and around the area. The results are of great significance to the further understanding of sources, records, and environmental impacts of global and regional nuclear activities in the environment and provide important chronological information for further studies on the water eutrophication process and climatic change, and reconstruction of pollution history of organic contaminants and heavy metals in the watershed of Lake Qinghai.

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

    NASA Astrophysics Data System (ADS)

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

    2016-06-01

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

  10. Study of radioactive isotopes of beryllium, polonium, uranium, and plutonium in the atmosphere

    SciTech Connect

    Lee, S.C.

    1986-01-01

    Radiochemical measurements were carried out for /sup 239.240/Pu in a total of 94 rain and snow samples collected at Fayetteville (36/sup 0/ N, 94/sup 0/W), Arkansas, during the period between May 1983 and November 1985. The concentrations of /sup 7/Be in most of these samples were also measured and these results were compared with previous samples. Average concentrations of cosmic-ray-produced radionuclide /sup 7/Be in rain remained fairly constant year after year. The annual rate of /sup 7/Be deposition at Fayetteville, Arkansas, was calculated from these data to be 5.2 dpm/cm/sup 2//year, which corresponds to a value of 2.8 x 10/sup -2/ atoms/cm/sup 2//second for the /sup 7/Be production rate in the atmosphere. The concentrations of bomb-produced radionuclides such as /sup 89/Sr, /sup 90/Sr and /sup 239.240/Pu in rain have drastically decreased since the last nuclear test explosion was conducted by the government of People's Republic of China in 1980. The concentrations of uranium isotopes and radon daughters in rain, on the other hand, were found to be affected by atmospheric injections of volcanic ashes from the 1980 eruption of Mount St. Helens and the 1982 eruption of El Chichon volcano in Mexico. Moreover, the burnups of the nuclear-powered Soviet satellites have caused marked increases in the levels of /sup 235/U and /sup 234/U in some of the rain samples. A sharp increase in the /sup 210/Po//sup 7/Be ratio in rain samples collected toward the end of 1980 and the beginning of 1981 was attributed to an atmospheric injection of /sup 210/Po from a series of major eruptions of Mount St. Helens.

  11. Plutonium controversy

    SciTech Connect

    Richmond, C.R.

    1980-01-01

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

  12. Rapid determination of (237)Np and plutonium isotopes in urine by inductively-coupled plasma mass spectrometry and alpha spectrometry.

    PubMed

    Maxwell, Sherrod L; Culligan, Brian K; Jones, Vernon D; Nichols, Sheldon T; Noyes, Gary W; Bernard, Maureen A

    2011-08-01

    A new rapid separation method was developed for the measurement of plutonium and neptunium in urine samples by inductively-coupled plasma mass spectrometry (ICP-MS) and/or alpha spectrometry with enhanced uranium removal. This method allows separation and preconcentration of plutonium and neptunium in urine samples using stacked extraction chromatography cartridges and vacuum box flow rates to facilitate rapid separations. There is an increasing need to develop faster analytical methods for emergency response samples. There is also enormous benefit to having rapid bioassay methods in the event that a nuclear worker has an uptake (puncture wound, etc.) to assess the magnitude of the uptake and guide efforts to mitigate dose (e.g., tissue excision and chelation therapy). This new method focuses only on the rapid separation of plutonium and neptunium with enhanced removal of uranium. For ICP-MS, purified solutions must have low salt content and low concentration of uranium due to spectral interference of (238)U(1)H(+) on m/z 239. Uranium removal using this method is enhanced by loading plutonium and neptunium initially onto TEVA resin, then moving plutonium to DGA resin where additional purification from uranium is performed with a decontamination factor of almost 1×10(5). If UTEVA resin is added to the separation scheme, a decontamination factor of ~3 × 10(6) can be achieved.

  13. Plutonium isotopic analysis system for plutonium samples enriched in sup 238 Pu in EP 60/61 and fuel-clad containers

    SciTech Connect

    Ruhter, W.D.

    1991-07-01

    This two-part manual describes and provides instructions for installing software for Lawrence Livermore National Laboratory's Pu-238 isotopic analysis system built for Westinghouse Hanford's Radioisotope Power Systems Facility. Part 1 contains descriptions of all the subroutines found in the main software program, WHC.ASY238. Also provided in this part are general instructions for modifying a subroutine and specific directions for relinking the WHC.ASY238 program, as well as information on the supporting program PU238.CHNG. Part 2 contains listings of the Pu-238 isotopic analysis system codes. The system uses a large (20% rel. efficiency), coaxial, n-type germanium detector (COAX). Parameter files for the detector have filenames with IS8 extensions. Spectral data files also have WH8 and I01, I02, etc. filename extensions.

  14. Isotopic and elemental composition of plutonium/americium oxides influence pulmonary and extra-pulmonary distribution after inhalation in rats.

    PubMed

    Van der Meeren, A; Grémy, O

    2010-09-01

    The biodistribution of plutonium and americium has been studied in a rat model after inhalation of two PuO(2) powders in lungs and extra-pulmonary organs from 3 d to 3 mo. The main difference between the two powders was the content of americium (approximately 46% and 4.5% of total alpha activity). The PuO(2) with a higher proportion of americium shows an accelerated transfer of activity from lungs to blood as compared to PuO(2) with the lower americium content, illustrated by increased urinary excretion and higher bone and liver actinide retention. The total alpha activity measured reflects mostly the americium biological behavior. The activity contained in epithelial lining fluid, recovered in the acellular phase of broncho-alveolar lavages, mainly contains americium, whereas plutonium remains trapped in macrophages. Epithelial lining fluid could represent a transitional pulmonary compartment prior to translocation of actinides to the blood and subsequent deposition in extra-pulmonary retention organs. In addition, differential behaviors of plutonium and americium are also observed between the PuO(2) powders with a higher dissolution rate for both plutonium and americium being obtained for the PuO(2) with the highest americium content. Our results indicate that the biological behavior of plutonium and americium after translocation into blood differ two-fold: (1) for the two actinides for the same PuO(2) aerosol, and (2) for the same actinide from the two different aerosols. These results highlight the importance of considering the specific behavior of each contaminant after accidental pulmonary intake when assessing extra-pulmonary deposits from the level of activity excreted in urine or for therapeutic strategy decisions.

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

    PubMed

    Shabana, E I; Al-Shammari, H L

    2001-01-01

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

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

    SciTech Connect

    Spencer, Khalil J.; Rim, Jung Ho; Porterfield, Donivan R.; Roback, Robert Clifford; Boukhalfa, Hakim; Stanley, Floyd E.

    2015-06-29

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

  17. Lawrence Livermore National Laboratory Measurements of Plutonium-bearing Oxide in DOE-STD-3013-2000 Containers Using Calorimetry and Gamma Isotopic Analyses

    SciTech Connect

    Dearborn, D M; Keeton, S C

    2004-06-23

    Lawrence Livermore National Laboratory (LLNL) routinely uses calorimetry and gamma isotopic analyses (Cal/Iso) for the accountability measurement of plutonium (Pu) bearing items. In the past 15 years, the vast majority of those items measured by Cal/Iso were contained in a thin-walled convenience can enclosed in another thin-walled outer container. However, LLNL has recently begun to use DOE-STD-3013-2000 containers as well. These DOE-STD-3013-2000 containers are comprised of a stainless steel convenience can enclosed in welded stainless steel primary and secondary containers. In addition to the fact that the wall thickness of the DOE-STD-3013-2000 containers is much greater than that of other containers in our experience, the DOE-STD-3013-2000 containers appear to have larger thermal insulation characteristics. To date, we have derived Pu-mass values from Cal/Iso measurements of 74 different DOE-STD-3013-2000 containers filled with Pu-bearing oxide or mixed uranium-plutonium (U-Pu) oxide material. Both water-bath and air-bath calorimeters were used for these measurements and both use software to predict when thermal equilibrium is attained. Our experience has shown that after apparent equilibrium has been attained, at least one more complete cycle, and sometimes two or three more complete cycles, is required to gain a measure of true thermal equilibrium. Otherwise, the derived Pu-mass values are less than would be expected from a combination of previously measured Pu-bearing items and would contribute to increased loss in our inventory difference determinations. Conclusions and recommendations drawn from LLNL experience with measurements of Pu mass in Pu-bearing oxide or mixed U-Pu oxide in DOE-STD-3013-2000 containers using the Cal/Iso technique are included.

  18. Aqueous Chloride Operations Overview: Plutonium and Americium Purification/Recovery

    SciTech Connect

    Kimball, David Bryan; Skidmore, Bradley Evan

    2016-06-22

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

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

    PubMed

    Konegger-Kappel, Stefanie; Prohaska, Thomas

    2016-01-01

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

  20. Design of the improved plutonium canister assay system (IPCAS)

    SciTech Connect

    Abhold, M. E.; Baker, M. C.; Bourret, S. C.; Polk, P. J.; Vo, Duc T.

    2001-01-01

    The improved Plutonium Canister Assay System (iPCAS) is designed to detect gross and partial defects in the declared plutonium content of plutonium and MOX storage canisters during transfer to storage and process areas of the MOX fuel fabrication facility in Kokkasho, Japan. In addition, an associated Gamma Isotopics System (GIS) will be used to confirm facility-declared plutonium isotopics with accuracy sufficient to reduce the amount of destructive isotopic analysis needed. The design of the iPCAS instrument and its associated GIS is described and the expected performance of the instrument is discussed.

  1. Plutonium Isotopes ((239-241)Pu) 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.

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

    SciTech Connect

    Blandinskiy, V. Yu.

    2014-12-15

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

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

    NASA Astrophysics Data System (ADS)

    Blandinskiy, V. Yu.

    2014-12-01

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

  4. Depositional behaviors of plutonium and thorium isotopes at Tsukuba and Mt. Haruna in Japan indicate the sources of atmospheric dust.

    PubMed

    Hirose, K; Igarashi, Y; Aoyama, M; Inomata, Y

    2010-02-01

    Monthly plutonium and thorium depositions at Tsukuba (28m asl) and Mt. Haruna (1370m asl) were measured during 2006 and 2007 (Jan 2006-Dec 2007 at Tsukuba, Nov 2006-Dec 2007 at Mt. Haruna). The monthly (239,240)Pu depositions ranged from 0.044 to 2.67mBq m(-2) at Tsukuba and from 0.05 to 0.9mBq m(-2) at Mt. Haruna during the measurement periods. Monthly (239,240)Pu deposition did not differ markedly between the two sites except in April 2007. Seasonal pattern of monthly (239,240)Pu depositions at both sites showed high in spring and low in summer, and typical of seasonal variations in northeastern Asia. Thorium deposition at Tsukuba was higher than that at Mt. Haruna except in May and June 2007. (230)Th/(232)Th activity ratios were used to partition deposition samples into locally and remotely derived fractions. The results revealed that a major proportion of total (239,240)Pu and Th deposits are derived from remote sources, especially in spring.

  5. Determining Sources and Transport of Nuclear Contamination in Hudson River Sediments with Plutonium, Neptunium, and Cesium isotope ratios

    NASA Astrophysics Data System (ADS)

    Kenna, T. C.; Chillrud, S. N.; Chaky, D. A.; Simpson, H. J.; McHugh, C. M.; Shuster, E. L.; Bopp, R. F.

    2004-12-01

    Different sources of radioactive contamination contain characteristic and identifiable isotopic signatures, which can be used to study sediment transport. We focus on Pu-239, Pu-240, Np-237 and Cs-137, which are strongly bound to fine grained sediments. The Hudson River drainage basin has received contamination from at least three separate sources: 1) global fallout from atmospheric testing of nuclear weapons, which contributed Pu, Np and Cs; 2) contamination resulting from reactor releases at the Indian Point Nuclear Power Plant (IPNPP) located on the Hudson River Estuary ˜70km north of New York Harbor, where records document releases of Cs-137; 3) contamination resulting from activities at the Knolls Atomic Power Laboratory (KAPL) located on the Mohawk River, where incomplete records document releases of Cs-137 but no mention is made of Pu or Np. Here we report measurements of Pu isotopes, Np-237 and Cs-137 for a series of sediment cores collected from various locations within the drainage basin: 1) Mohawk River downstream of KAPL, 2) Hudson River upstream of its confluence with the Mohawk River, and 3) lower Hudson River at a location in close proximity to IPNPP. In addition, we present data from selected samples from two other lower Hudson River locations: One site located ˜30km downstream of IPNPP and another ˜30km upstream of IPNPP. By comparing the isotopic ratios Pu-240/Pu-239, Np-237/Pu-239, and Cs-137/Pu-239, measured in fluvial sediments to mean global fallout values, it is possible to identify and resolve different sources of non-fallout contamination. To date, isotopic data for sediments indicate non-fallout sources of Pu-239, Pu-240, and Cs-137; Np-237, however, appears to originate from global fallout only. Mohawk River sediments downstream of KAPL exhibit enrichments in Pu-239, Pu-240, and Cs-137 that are 7 to 20 times higher than levels expected from global fallout as indicated from Np-237. The elevated levels, non-fallout isotopic signatures

  6. Quantitative ion-exchange separation of plutonium from impurities

    SciTech Connect

    Pietri, C.E.; Freeman, B.P.; Weiss, J.R.

    1981-09-01

    The methods used at the New Brunswick Laboratory for the quantitative ion exchange separation of plutonium from impurities prior to plutonium assay are described. Other ion exchange separation procedures for impurity determination and for isotopic abundance measurements are given. The primary technique used consists of sorption of plutonium(IV) in 8N HNO/sub 3/ on Dowex-1 anion exchange resin and elution of the purified plutonium with 0.3N HCl-0.01N HF. Other methods consist of the anion exchange separation of plutonium(IV) in 12N HCl and the cation exchange separation of plutonium(III) in 0.2 N HNO/sub 3/. The application of these procedures to the subsequent assay of plutonium, isotopic analysis, and impurity determination is described.

  7. CONVERSION OF PLUTONIUM TRIFLUORIDE TO PLUTONIUM TETRAFLUORIDE

    DOEpatents

    Fried, S.; Davidson, N.R.

    1957-09-10

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

  8. Plutonium stabilization and packaging system

    SciTech Connect

    1996-05-01

    This document describes the functional design of the Plutonium Stabilization and Packaging System (Pu SPS). The objective of this system is to stabilize and package plutonium metals and oxides of greater than 50% wt, as well as other selected isotopes, in accordance with the requirements of the DOE standard for safe storage of these materials for 50 years. This system will support completion of stabilization and packaging campaigns of the inventory at a number of affected sites before the year 2002. The package will be standard for all sites and will provide a minimum of two uncontaminated, organics free confinement barriers for the packaged material.

  9. New Fecal Method for Plutonium and Americium

    SciTech Connect

    Maxwell, S.L. III

    2000-06-27

    A new fecal analysis method that dissolves plutonium oxide was developed at the Westinghouse Savannah River Site. Diphonix Resin (Eichrom Industries), is used to pre-concentrate the actinides from digested fecal samples. A rapid microwave digestion technique is used to remove the actinides from the Diphonix Resin, which effectively extracts plutonium and americium from acidic solutions containing hydrofluoric acid. After resin digestion, the plutonium and americium are recovered in a small volume of nitric acid that is loaded onto small extraction chromatography columns, TEVA Resin and TRU Resin (Eichrom Industries). The method enables complete dissolution of plutonium oxide and provides high recovery of plutonium and americium with good removal of thorium isotopes such as thorium-228.

  10. Radionuclide Basics: Plutonium

    EPA Pesticide Factsheets

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

  11. Plutonium concentration and isotopic ratio in soil samples from central-eastern Japan collected around the 1970s.

    PubMed

    Yang, Guosheng; Zheng, Jian; Tagami, Keiko; Uchida, Shigeo

    2015-04-16

    Obtaining Pu background data in the environment is essential for contamination source identification and assessment of environmental impact of Pu released from the Fukushima Daiichi nuclear power plant (FDNPP) accident. However, no baseline information on Pu isotopes in Fukushima Prefecture has been reported. Here we analyzed 80 surface soil samples collected from the central-eastern Japan during 1969-1977 for (239+240)Pu activity concentration and (240)Pu/(239)Pu atom ratio to establish the baseline before the FDNPP accident. We found that (239+240)Pu activity concentrations ranged from 0.004 -1.46 mBq g(-1), and (240)Pu/(239)Pu atom ratios varied narrowly from 0.148 to 0.229 with a mean of 0.186 ± 0.015. We also reconstructed the surface deposition density of (241)Pu using the (241)Pu/(239)Pu atom ratio in the Japanese fallout reference material. The obtained results indicated that, for the FDNPP-accident released (241)Pu, a similar radiation impact can be estimated as was seen for the global fallout deposited (241)Pu in the last decades.

  12. Plutonium concentration and isotopic ratio in soil samples from central-eastern Japan collected around the 1970s

    PubMed Central

    Zheng, Jian; Tagami, Keiko; Uchida, Shigeo

    2015-01-01

    Obtaining Pu background data in the environment is essential for contamination source identification and assessment of environmental impact of Pu released from the Fukushima Daiichi nuclear power plant (FDNPP) accident. However, no baseline information on Pu isotopes in Fukushima Prefecture has been reported. Here we analyzed 80 surface soil samples collected from the central-eastern Japan during 1969–1977 for 239+240Pu activity concentration and 240Pu/239Pu atom ratio to establish the baseline before the FDNPP accident. We found that 239+240Pu activity concentrations ranged from 0.004 –1.46 mBq g−1, and 240Pu/239Pu atom ratios varied narrowly from 0.148 to 0.229 with a mean of 0.186 ± 0.015. We also reconstructed the surface deposition density of 241Pu using the 241Pu/239Pu atom ratio in the Japanese fallout reference material. The obtained results indicated that, for the FDNPP-accident released 241Pu, a similar radiation impact can be estimated as was seen for the global fallout deposited 241Pu in the last decades. PMID:25881009

  13. Plutonium concentration and isotopic ratio in soil samples from central-eastern Japan collected around the 1970s

    NASA Astrophysics Data System (ADS)

    Yang, Guosheng; Zheng, Jian; Tagami, Keiko; Uchida, Shigeo

    2015-04-01

    Obtaining Pu background data in the environment is essential for contamination source identification and assessment of environmental impact of Pu released from the Fukushima Daiichi nuclear power plant (FDNPP) accident. However, no baseline information on Pu isotopes in Fukushima Prefecture has been reported. Here we analyzed 80 surface soil samples collected from the central-eastern Japan during 1969-1977 for 239+240Pu activity concentration and 240Pu/239Pu atom ratio to establish the baseline before the FDNPP accident. We found that 239+240Pu activity concentrations ranged from 0.004 -1.46 mBq g-1, and 240Pu/239Pu atom ratios varied narrowly from 0.148 to 0.229 with a mean of 0.186 +/- 0.015. We also reconstructed the surface deposition density of 241Pu using the 241Pu/239Pu atom ratio in the Japanese fallout reference material. The obtained results indicated that, for the FDNPP-accident released 241Pu, a similar radiation impact can be estimated as was seen for the global fallout deposited 241Pu in the last decades.

  14. Plutonium isotopes concentration in seawater and bottom sediment off the Pacific coast of Aomori sea area during 1991-2005.

    PubMed

    Oikawa, Shinji; Watabe, Teruhisa; Inatomi, Naohiko; Isoyama, Naohiko; Misonoo, Jun; Suzuki, Chiyoshi; Nakahara, Motokazu; Nakamura, Ryoichi; Morizono, Shigemitsu; Fujii, Seiji; Hara, Takeya; Kido, Katsutoshi

    2011-03-01

    A radioactivity survey was launched in 1991 to determine the background levels of ²³⁹+²⁴⁰Pu in the marine environment off a commercial spent nuclear fuel reprocessing plant before full operation of the facility. Particular attention was focused on the ²⁴⁰Pu/²³⁹Pu atom ratio in seawater and bottom sediment to identify the origins of Pu isotopes. The concentration of ²³⁹+²⁴⁰Pu was almost uniform in surface water, decreasing slowly over time. Conversely, the ²³⁹+²⁴⁰Pu concentration varied markedly in the bottom water and was dependent upon the sampling point, with higher concentrations of ²³⁹+²⁴⁰Pu observed in the bottom water sample at sampling points having greater depth. The ²⁴⁰Pu/²³⁹Pu atom ratio in the seawater and sediment samples was higher than that of global fallout Pu, and comparable with the data in the other sea area around Japan which has likely been affected by close-in fallout Pu originating from the Pacific Proving Grounds. The ²⁴⁰Pu/²³⁹Pu atom ratio in bottom sediment samples decreased with sea depth. The land-originated Pu is not considered as the reason of the increasing ²³⁹+²⁴⁰Pu concentration and also decreasing the ²⁴⁰Pu/²³⁹Pu atom ratio with sea depth, and further study is required to clarify it.

  15. Plutonium in the atmosphere: A global perspective.

    PubMed

    Thakur, P; Khaing, H; Salminen-Paatero, S

    2017-09-01

    A number of potential source terms have contributed plutonium isotopes to the atmosphere. The atmospheric nuclear weapon tests conducted between 1945 and 1980 and the re-entry of the burned SNAP-9A satellite in 1964, respectively. It is generally believed that current levels of plutonium in the stratosphere are negligible and compared with the levels generally found at surface-level air. In this study, the time trend analysis and long-term behavior of plutonium isotopes ((239+240)Pu and (238)Pu) in the atmosphere were assessed using historical data collected by various national and international monitoring networks since 1960s. An analysis of historical data indicates that (239+240)Pu concentration post-1984 is still frequently detectable, whereas (238)Pu is detected infrequently. Furthermore, the seasonal and time-trend variation of plutonium concentration in surface air followed the stratospheric trends until the early 1980s. After the last Chinese test of 1980, the plutonium concentrations in surface air dropped to the current levels, suggesting that the observed concentrations post-1984 have not been under stratospheric control, but rather reflect the environmental processes such as resuspension. Recent plutonium atmospheric air concentrations data show that besides resuspension, other environmental processes such as global dust storms and biomass burning/wildfire also play an important role in redistributing plutonium in the atmosphere. Copyright © 2017 Elsevier Ltd. All rights reserved.

  16. PLUTONIUM ALLOYS

    DOEpatents

    Chynoweth, W.

    1959-06-16

    The preparation of low-melting-point plutonium alloys is described. In a MgO crucible Pu is placed on top of the lighter alloying metal (Fe, Co, or Ni) and the temperature raised to 1000 or 1200 deg C. Upon cooling, the alloy slug is broke out of the crucible. With 14 at. % Ni the m.p. is 465 deg C; with 9.5 at. % Fe the m.p. is 410 deg C; and with 12.0 at. % Co the m.p. is 405 deg C. (T.R.H.) l6262 l6263 ((((((((Abstract unscannable))))))))

  17. PRODUCTION OF PLUTONIUM METAL

    DOEpatents

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

    1961-01-17

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

  18. SEPARATION OF PLUTONIUM

    DOEpatents

    Maddock, A.G.; Smith, F.

    1959-08-25

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

  19. Probing Phonons in Plutonium

    NASA Astrophysics Data System (ADS)

    Wong, Joe

    2004-03-01

    The phonon spectra of plutonium and its alloys have been sought after in the past few decades following the discovery of this actinide element in 1941, but with no success. This was due to a combination of the high neutron absorption cross section of 239Pu, the common isotope, and non-availability of large single crystals of any Pu-bearing materials. We have recent designed a high resolution inelastic x-ray scattering experiment using a bright synchrotron x-ray beam at the European Sychrotron Radiation Facility (ESRF), Grenoble and mapped the full phonon dispersion curves of an fcc delta-phase polycrystalline Pu-Ga alloy (1). Several unusual features including, a large elastic anisotropy, a small shear elastic modulus C', a Kohn-like anomaly in the T1[011] branch, and a pronounced softening of the [111] transverse modes are found. These features can be related to the phase transitions of plutonium and to strong coupling between the lattice structure and the 5f valence instabilities. Our results also provide a critical test for theoretical treatments of highly correlated 5f electron systems as exemplified by recent dynamical mean field theory (DMFT) calculations for d-plutonium.(2) This work was performed in collaboration with Dr. M. Krisch (ESRF)) and Prof. T.-C. Chiang (UIU), and under the auspices of the U. S. Department of Energy by the University of California, Lawrence Livermore National Laboratory under Contract No. W-7405-Eng-48. 1. Joe Wong et al. Science, vol.301, 1078 (2003) 2. X. Dai et al. Science, vol.300, 953 (2003)

  20. STRIPPING PROCESS FOR PLUTONIUM

    DOEpatents

    Kolodney, M.

    1959-10-01

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

  1. Preserving Plutonium-244 as a National Asset

    SciTech Connect

    Patton, Bradley D; Alexander, Charles W; Benker, Dennis; Collins, Emory D; Romano, Catherine E; Wham, Robert M

    2011-01-01

    Plutonium-244 (244 Pu) is an extremely rare and long-lived isotope of plutonium with a half-life of 80 million years. Measureable amounts of 244 Pu are found in neither reactor-grade nor weapons-grade plutonium. Production of this isotope requires a very high thermal flux to permit the two successive neutron captures that convert 242 Pu to 243 Pu to 244 Pu, particularly given the short (about 5 hour) half-life of 243 Pu. Such conditions simply do not exist in plutonium production processes. Therefore, 244 Pu is ideal for precise radiochemical analyses measuring plutonium material properties and isotopic concentrations in items containing plutonium. Isotope dilution mass spectrometry is about ten times more sensitive when using 244 Pu rather than 242 Pu for determining plutonium isotopic content. The isotope can also be irradiated in small quantities to produce superheavy elements. The majority of the existing global inventory of 244 Pu is contained in the outer housing of Mark-18A targets at the Savannah River Site (SRS). The total inventory is about 20 grams of 244 Pu in about 400 grams of plutonium distributed among the 65 targets. Currently, there are no specific plans to preserve these targets. Although the cost of separating and preserving this material would be considerable, it is trivial in comparison to new production costs. For all practical purposes, the material is irreplaceable, because new production would cost billions of dollars and require a series of irradiation and chemical separation cycles spanning up to 50 years. This paper will discuss a set of options for overcoming the significant challenges to preserve the 244 Pu as a National Asset: (1) the need to relocate the material from SRS in a timely manner, (2) the need to reduce the volume of material to the extent possible for storage, and (3) the need to establish an operational capability to enrich the 244 Pu in significant quantities. This paper suggests that if all the Mark-18A plutonium is

  2. Analysis of Uranium and Plutonium by MC-ICPMS

    SciTech Connect

    Williams, R W

    2005-02-23

    This procedure is written as general guidance for the measurement of elemental isotopic composition by plasma-source inorganic mass spectrometry. Analytical methods for uranium and plutonium are given as examples.

  3. METHOD OF SEPARATING PLUTONIUM

    DOEpatents

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

    1958-02-01

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

  4. Plutonium Training Opportunities

    SciTech Connect

    Balatsky, Galya Ivanovna; Wolkov, Benjamin

    2015-03-26

    This report was created to examine the current state of plutonium training in the United States and to discover ways in which to ensure that the next generation of plutonium workers are fully qualified.

  5. PREPARATION OF PLUTONIUM TRIFLUORIDE

    DOEpatents

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

    1961-07-11

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

  6. Method for calibration of plutonium NDA

    SciTech Connect

    Lemming, J.F.; Campbell, A.R.; Rodenburg, W.W.

    1980-01-01

    Calibration materials characterized by calorimetric assay can be a practical alternative to synthetic standards for the calibration of plutonium nondestructive assay. Calorimetric assay is an effective measurement system for the characterization because: it can give an absolute assay from first principles when the isotopic composition is known, it is insensitive to most matrix effects, and its traceability to international measurement systems has been demonstrated.

  7. PROCESS FOR PURIFYING PLUTONIUM

    DOEpatents

    Mastick, D.F.; Wigner, E.P.

    1958-05-01

    A method is described of separating plutonium from small amounts of uranium and other contaminants. An acidic aqueous solution of higher valent plutonium and hexavalent uranium is treated with a soluble iodide to obtain the plutonium in the plus three oxidation state while leaving the uranium in the hexavalent state, adding a soluble oxalate such as oxalic acid, and then separating the insoluble plus the plutonium trioxalate from the solution.

  8. A Note on the Reaction of Hydrogen and Plutonium

    SciTech Connect

    Noone, Bailey C

    2012-08-15

    fluorite to hexagonal. This change in crystal structure as a result of adding hydrogen is a shared characteristic with other actinide elements. Americium is isostructural with plutonium because they both form cubic dihyrides and hexagonal trihydrides. Reacting hydrogen with plutonium has the practical application of separating plutonium from other materials that don't react as well with hydrogen. When plutonium is placed in a chamber where there is very little oxygen, it can react with hydrogen without igniting. The hydrogen plutonium reaction can then be reversed, thus regaining the separated plutonium. Another application of this reaction is that it can be used to predict how plutonium reacts with other substances. Deuterium and tritium are two isotopes of hydrogen that are of interest. They are known to react likewise to hydrogen because they have similar properties. The reaction of plutonium and isotopes of hydrogen can prove to be very informative.

  9. PLUTONIUM CLEANING PROCESS

    DOEpatents

    Kolodney, M.

    1959-12-01

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

  10. PLUTONIUM-THORIUM ALLOYS

    DOEpatents

    Schonfeld, F.W.

    1959-09-15

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

  11. On the sequential separation and quantification of (237)Np, (241)Am, thorium, plutonium, and uranium isotopes in environmental and urine samples.

    PubMed

    Vasile, M; Jacobs, K; Bruggeman, M; Van Hoecke, K; Dobney, A; Verrezen, F

    2017-07-13

    The implementation of the one-pass-through separation technique using two stacked chromatography columns of TEVA - TRU resins for the separation of (237)Np, (241)Am, thorium, plutonium and uranium from environmental and urine samples was investigated. The sequential separation technique proved to be successful and gave similar results to those obtained when using individual separations. The analysis time was considerably improved. The amount of chemical waste was also reduced by 50% and the use of HClO4 was avoided. The technique of ICP-MS was also investigated as a complementary technique to alpha-spectrometry. Copyright © 2017 Elsevier Ltd. All rights reserved.

  12. ESTIMATING IMPURITIES IN SURPLUS PLUTONIUM FOR DISPOSITION

    SciTech Connect

    Allender, J.; Moore, E.

    2013-07-17

    The United States holds at least 61.5 metric tons (MT) of plutonium that is permanently excess to use in nuclear weapons programs, including 47.2 MT of weapons-grade plutonium. Surplus inventories will be stored safely by the Department of Energy (DOE) and then transferred to facilities that will prepare the plutonium for permanent disposition. The Savannah River National Laboratory (SRNL) operates a Feed Characterization program for the Office of Fissile Materials Disposition of the National Nuclear Security Administration and the DOE Office of Environmental Management. Many of the items that require disposition are only partially characterized, and SRNL uses a variety of techniques to predict the isotopic and chemical properties that are important for processing through the Mixed Oxide Fuel Fabrication Facility and alternative disposition paths. Recent advances in laboratory tools, including Prompt Gamma Analysis and Peroxide Fusion treatment, provide data on the existing inventories that will enable disposition without additional, costly sampling and destructive analysis.

  13. METHOD OF SEPARATING PLUTONIUM

    DOEpatents

    Heal, H.G.

    1960-02-16

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

  14. PREPARATION OF PLUTONIUM HALIDES

    DOEpatents

    Davidson, N.R.; Katz, J.J.

    1958-11-01

    A process ls presented for the preparation of plutonium trihalides. Plutonium oxide or a compound which may be readily converted to plutonlum oxide, for example, a plutonium hydroxide or plutonlum oxalate is contacted with a suitable halogenating agent. Speciflc agents mentioned are carbon tetrachloride, carbon tetrabromide, sulfur dioxide, and phosphorus pentachloride. The reaction is carried out under superatmospberic pressure at about 300 icient laborato C.

  15. PLUTONIUM-ZIRCONIUM ALLOYS

    DOEpatents

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

    1960-08-30

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

  16. PREPARATION OF PLUTONIUM

    DOEpatents

    Kolodney, M.

    1959-07-01

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

  17. Continuous plutonium dissolution apparatus

    DOEpatents

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

    1974-02-26

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

  18. North Korean plutonium production

    SciTech Connect

    Albright, D.

    1994-12-01

    In 1992, as part of its obligations under the Nuclear Non-Proliferation Treaty, North Korea declared that it had earlier separated about 100 grams of plutonium from damaged fuel rods removed from a 25 megawatt-thermal (MW{sub t}) gas-graphite reactor at Yongbyon. The plutonium was separated at the nearby {open_quotes}Radiochemical Laboratory.{close_quotes} Separated plutonium is the raw ingredient for making nuclear weapons, but 100 grams is too little to make a crude bomb. Based on intelligence reports and IAEA inspections, North Korea may have separated enough plutonium for a nuclear weapon. Regardless of whether this is true, there is no doubt that North Korea has enough weapons-grade plutonium in spent fuel to make four or five nuclear weapons. But it cannot turn this plutonium into nuclear weapons unless it separates the plutonium from the spent fuel. Preventing the North from separating any more plutonium must remain a global priority. The IAEA must also be able to verify North Korea`s past nuclear activities and determine the amount of plutonium North Korea may have diverted in the past.

  19. Release of plutonium isotopes into the environment from the Fukushima Daiichi Nuclear Power Plant accident: what is known and what needs to be known.

    PubMed

    Zheng, Jian; Tagami, Keiko; Uchida, Shigeo

    2013-09-03

    The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident has caused serious contamination in the environment. The release of Pu isotopes renewed considerable public concern because they present a large risk for internal radiation exposure. In this Critical Review, we summarize and analyze published studies related to the release of Pu from the FDNPP accident based on environmental sample analyses and the ORIGEN model simulations. Our analysis emphasizes the environmental distribution of released Pu isotopes, information on Pu isotopic composition for source identification of Pu releases in the FDNPP-damaged reactors or spent fuel pools, and estimation of the amounts of Pu isotopes released from the FDNPP accident. Our analysis indicates that a trace amount of Pu isotopes (∼2 × 10(-5)% of core inventory) was released into the environment from the damaged reactors but not from the spent fuel pools located in the reactor buildings. Regarding the possible Pu contamination in the marine environment, limited studies suggest that no extra Pu input from the FDNPP accident could be detected in the western North Pacific 30 km off the Fukushima coast. Finally, we identified knowledge gaps remained on the release of Pu into the environment and recommended issues for future studies.

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

    SciTech Connect

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

    1989-09-07

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

  1. DELTA PHASE PLUTONIUM ALLOYS

    DOEpatents

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

    1960-03-22

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

  2. PLUTONIUM-CERIUM ALLOY

    DOEpatents

    Coffinberry, A.S.

    1959-01-01

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

  3. ELECTRODEPOSITION OF PLUTONIUM

    DOEpatents

    Wolter, F.J.

    1957-09-10

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

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

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

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

  5. PLUTONIUM-CERIUM-COBALT AND PLUTONIUM-CERIUM-NICKEL ALLOYS

    DOEpatents

    Coffinberry, A.S.

    1959-08-25

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

  6. Plutonium storage criteria

    SciTech Connect

    Chung, D.; Ascanio, X.

    1996-05-01

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

  7. Plutonium bioaccumulation in seabirds.

    PubMed

    Strumińska-Parulska, Dagmara I; Skwarzec, Bogdan; Fabisiak, Jacek

    2011-12-01

    The aim of the paper was plutonium (²³⁸Pu and ²³⁹⁺²⁴⁰Pu) determination in seabirds, permanently or temporarily living in northern Poland at the Baltic Sea coast. Together 11 marine birds species were examined: 3 species permanently residing in the southern Baltic, 4 species of wintering birds and 3 species of migrating birds. The obtained results indicated plutonium is non-uniformly distributed in organs and tissues of analyzed seabirds. The highest plutonium content was found in the digestion organs and feathers, the smallest in skin and muscles. The plutonium concentration was lower in analyzed species which feed on fish and much higher in herbivorous species. The main source of plutonium in analyzed marine birds was global atmospheric fallout.

  8. Plutonium Immobilization Canister Loading

    SciTech Connect

    Hamilton, E.L.

    1999-01-26

    This disposition of excess plutonium is determined by the Surplus Plutonium Disposition Environmental Impact Statement (SPD-EIS) being prepared by the Department of Energy. The disposition method (Known as ''can in canister'') combines cans of immobilized plutonium-ceramic disks (pucks) with vitrified high-level waste produced at the SRS Defense Waste Processing Facility (DWPF). This is intended to deter proliferation by making the plutonium unattractive for recovery or theft. The envisioned process remotely installs cans containing plutonium-ceramic pucks into storage magazines. Magazines are then remotely loaded into the DWPF canister through the canister neck with a robotic arm and locked into a storage rack inside the canister, which holds seven magazines. Finally, the canister is processed through DWPF and filled with high-level waste glass, thereby surrounding the product cans. This paper covers magazine and rack development and canister loading concepts.

  9. Method for dissolving plutonium dioxide

    DOEpatents

    Tallent, Othar K.

    1978-01-01

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

  10. A preliminary study for the development of reference material using oyster for determination of (137)Cs, (90)Sr and plutonium isotopes.

    PubMed

    Lee, Sang-Han; Oh, Jung-Suk; Lee, Jong-Man; Lee, Kyung-Bum; Park, Tae-Soon; Lee, Min-Kie; Kim, Seung-Hwan; Choi, Jong-Ki

    2016-03-01

    A new reference material for the determination of (137)Cs, (90)Sr and Pu isotopes ((238)Pu and (239,240)Pu) is being developed using dried oyster matrix by Korea Research Institute of Standards and Science (KRISS). The oyster was collected from Tongyoung harbour, southern part of Korea and the artificial radionuclides ((137)Cs, (90)Sr, (238)Pu and (239,240)Pu) were spiked into the material. After pretreatment and processing, the material was tested for homogeneity and massic activities were determined by measuring (137)Cs, (90)Sr, (238)Pu and (239,240)Pu. The reference value and extended uncertainty for those isotopes will be reported later. Copyright © 2015 Elsevier Ltd. All rights reserved.

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

    PubMed

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

    2017-09-13

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

  12. Chemical Disposition of Plutonium in Hanford Site Tank Wastes

    SciTech Connect

    Delegard, Calvin H.; Jones, Susan A.

    2015-05-07

    This report examines the chemical disposition of plutonium (Pu) in Hanford Site tank wastes, by itself and in its observed and potential interactions with the neutron absorbers aluminum (Al), cadmium (Cd), chromium (Cr), iron (Fe), manganese (Mn), nickel (Ni), and sodium (Na). Consideration also is given to the interactions of plutonium with uranium (U). No consideration of the disposition of uranium itself as an element with fissile isotopes is considered except tangentially with respect to its interaction as an absorber for plutonium. The report begins with a brief review of Hanford Site plutonium processes, examining the various means used to recover plutonium from irradiated fuel and from scrap, and also examines the intermediate processing of plutonium to prepare useful chemical forms. The paper provides an overview of Hanford tank defined-waste–type compositions and some calculations of the ratios of plutonium to absorber elements in these waste types and in individual waste analyses. These assessments are based on Hanford tank waste inventory data derived from separately published, expert assessments of tank disposal records, process flowsheets, and chemical/radiochemical analyses. This work also investigates the distribution and expected speciation of plutonium in tank waste solution and solid phases. For the solid phases, both pure plutonium compounds and plutonium interactions with absorber elements are considered. These assessments of plutonium chemistry are based largely on analyses of idealized or simulated tank waste or strongly alkaline systems. The very limited information available on plutonium behavior, disposition, and speciation in genuine tank waste also is discussed. The assessments show that plutonium coprecipitates strongly with chromium, iron, manganese and uranium absorbers. Plutonium’s chemical interactions with aluminum, nickel, and sodium are minimal to non-existent. Credit for neutronic interaction of plutonium with these absorbers

  13. The distribution and history of nuclear weapons related contamination in sediments from the Ob River, Siberia as determined by isotopic ratios of plutonium and neptunium.

    PubMed

    Kenna, T C; Sayles, F L

    2002-01-01

    Isotopic ratios of Pu and Np measured in sediment cores from 5 locations in the Ob River drainage basin show clear evidence of input from sources other than global fallout (non-fallout sources). Historical contaminant records obtained by combining isotopic ratio information with chronological information indicate that non-fallout inputs are from several sources that have varied significantly over the past 50 years. Unique isotopic signatures observed in sediments from tributaries that drain areas containing known or suspected sources of non-fallout contamination are used to identify the source of materials in sediments collected at downstream locations. These data can lead to a better understanding of the transport behavior, fate, and relative importance of particle reactive, weapons related contaminants originating from the nuclear facilities Mayak. Tomsk-7, and Semipalitinsk, which lie within the drainage basin. From our work to date, we draw the following conclusions: (1) Persistent non-fallout contamination is observed in the Ob River above its confluence with the Irtysh River, indicating contamination from the Tomsk-7 facility. (2) Non-fallout contamination in the Tobol River above its confluence with the Irtysh River indicates contamination from the Mayak facility. (3) Non-fallout contamination in the Irtysh River above its confluence with the Tobol River indicates contamination from the Semipalitinsk weapons test site. (4) The occurrence of isotopic ratios in Ob Delta sediments that are similar to those observed in source tributaries suggests that contamination from at least two sources has been transported along the length of the river system. (5) Global fallout, a result of high-yield atmospheric weapons tests conducted by the FSU and USA primarily, is the dominant source of Pu and Np to the region; however, there have been brief periods when inputs from non-fallout sources exceeded those from global fallout.

  14. Rapid determination of plutonium isotopes in environmental samples using sequential injection extraction chromatography and detection by inductively coupled plasma mass spectrometry.

    PubMed

    Qiao, Jixin; Hou, Xiaolin; Roos, Per; Miró, Manuel

    2009-10-01

    This article presents an automated method for the rapid determination of 239Pu and 240Pu in various environmental samples. The analytical method involves the in-line separation of Pu isotopes using extraction chromatography (TEVA) implemented in a sequential injection (SI) network followed by detection of isolated analytes with inductively coupled plasma mass spectrometry (ICP-MS). The method has been devised for the determination of Pu isotopes at environmentally relevant concentrations, whereby it has been successfully applied to the analyses of large volumes/amounts of samples, for example, 100-200 g of soil and sediment, 20 g of seaweed, and 200 L of seawater following analyte preconcentration. The investigation of the separation capability of the assembled SI system revealed that up to 200 g of soil or sediment can be treated using a column containing about 0.70 g of TEVA resin. The analytical results of Pu isotopes in the reference materials showed good agreement with the certified or reference values at the 0.05 significance level. Chemical yields of Pu ranged from 80 to 105%, and the decontamination factors for uranium, thorium, mercury and lead were all above 10(4). The duration of the in-line extraction chromatographic run was <1.5 h, and the proposed setup was able to handle up to 20 samples (14 mL each) in a fully automated mode using a single chromatographic column. The SI manifold is thus suitable for rapid and automated determination of Pu isotopes in environmental risk assessment and emergency preparedness scenarios.

  15. Uranium Isotopic Analysis with the FRAM Isotopic Analysis Code

    SciTech Connect

    Duc T. Vo; Thomas E. Sampson

    1999-05-01

    FRAM is the acronym for Fixed-energy Response-function Analysis with Multiple efficiency. This software was developed at Los Alamos National Laboratory originally for plutonium isotopic analysis. Later, it was adapted for uranium isotopic analysis in addition to plutonium. It is a code based on a self-calibration using several gamma-ray peaks for determining the isotopic ratios. The versatile-parameter database structure governs all facets of the data analysis. User editing of the parameter sets allows great flexibility in handling data with different isotopic distributions, interfering isotopes, and different acquisition parameters such as energy calibration and detector type.

  16. Plutonium contamination in soils in open space and residential areas near Rocky Flats, Colorado.

    PubMed

    Litaor, M I

    1999-02-01

    Spatial analysis of the 240Pu:239Pu isotopic ratio of 42 soil samples collected around Rocky Flats Plant near Golden, Colorado, was conducted to assess the effect of Rocky Flats Plant activity on the soil environment. Two probability maps that quantified the uncertainty of the spatial distribution of plutonium isotopic ratios were constructed using the sequential Gaussian simulation technique (sGs). Assuming a plutonium isotopic ratio range of 0.152+/-0.003 to 0.169+/-0.009 is characteristic to global fallout in Colorado, and a mean value of 0.155 is representative for the Rocky Flats Plant area, the main findings of the current work were (1) the areas northwest and southwest of Rocky Flats Plant exhibited a plutonium ratio > or = 0.155, thus were minimally impacted by the plant activity; (2) the study area east of Rocky Flats Plant (approximately 120 km2) exhibited a plutonium isotopic ratio < or = 0.155, which is a definitive indicator of Rocky Flats Plant-derived plutonium; and (3) inventory calculations across the study area exhibited large standard error of estimates. These errors were originated from the high variability in plutonium activity over a small sampling scale and the uncertainty in the global fallout isotopic ratio. Using the mean simulated estimates of plutonium isotopic ratio, coupled with plutonium activity measured at 11 soil pits and additional plutonium information published elsewhere, the plutonium loading on the open space and residential areas amounted to 111.2 GBq, with a standard error of estimate of 50.8 GBq.

  17. Plutonium Vulnerability Management Plan

    SciTech Connect

    1995-03-01

    This Plutonium Vulnerability Management Plan describes the Department of Energy`s response to the vulnerabilities identified in the Plutonium Working Group Report which are a result of the cessation of nuclear weapons production. The responses contained in this document are only part of an overall, coordinated approach designed to enable the Department to accelerate conversion of all nuclear materials, including plutonium, to forms suitable for safe, interim storage. The overall actions being taken are discussed in detail in the Department`s Implementation Plan in response to the Defense Nuclear Facilities Safety Board (DNFSB) Recommendation 94-1. This is included as Attachment B.

  18. Progress on plutonium stabilization

    SciTech Connect

    Hurt, D.

    1996-05-01

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

  19. PLUTONIUM SEPARATION METHOD

    DOEpatents

    Beaufait, L.J. Jr.; Stevenson, F.R.; Rollefson, G.K.

    1958-11-18

    The recovery of plutonium ions from neutron irradiated uranium can be accomplished by bufferlng an aqueous solutlon of the irradiated materials containing tetravalent plutonium to a pH of 4 to 7, adding sufficient acetate to the solution to complex the uranyl present, adding ferric nitrate to form a colloid of ferric hydroxide, plutonlum, and associated fission products, removing and dissolving the colloid in aqueous nitric acid, oxldizlng the plutonium to the hexavalent state by adding permanganate or dichromate, treating the resultant solution with ferric nitrate to form a colloid of ferric hydroxide and associated fission products, and separating the colloid from the plutonlum left in solution.

  20. PLUTONIUM ELECTROREFINING CELLS

    DOEpatents

    Mullins, L.J. Jr.; Leary, J.A.; Bjorklund, C.W.; Maraman, W.J.

    1963-07-16

    Electrorefining cells for obtaining 99.98% plutonium are described. The cells consist of an impure liquid plutonium anode, a molten PuCl/sub 3/-- alkali or alkaline earth metal chloanode, a molten PuCl/sub 3/-alkali or alkaline earth metal chloride electrolyte, and a nonreactive cathode, all being contained in nonreactive ceramic containers which separate anode from cathode by a short distance and define a gap for the collection of the purified liquid plutonium deposited on the cathode. Important features of these cells are the addition of stirrer blades on the anode lead and a large cathode surface to insure a low current density. (AEC)

  1. Plutonium radiation surrogate

    DOEpatents

    Frank, Michael I [Dublin, CA

    2010-02-02

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

  2. Plutonium dissolution process

    DOEpatents

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

    1996-01-01

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

  3. Plutonium: Requiem or reprieve

    SciTech Connect

    Pillay, K.K.S.

    1996-01-01

    Many scientific discoveries have had profound effects on humanity and its future. However, the discovery of fissionable characteristics of a man-made element, plutonium, discovered in 1941 by Glenn Seaborg and associates, has probably had the greatest impact on world affairs. Although about 20 new elements have been synthesized since 1940, element 94 unarguably had the most dramatic impact when it was introduced to the world as the core of the nuclear bomb dropped on Nagasaki. Ever since, large quantities of this element have been produced, and it has had a major role in maintaining peace during the past 50 years. in addition, the rapid spread of nuclear power technology worldwide contributed to major growth in the production of plutonium as a by-product. This article discusses the following issues related to plutonium: plutonium from Nuclear Power Generation; environmental safety and health issues; health effects; safeguards issues; extended storage; disposal options.

  4. Analysis of 236U and plutonium isotopes, 239,240Pu, on the 1 MV AMS system at the Centro Nacional de Aceleradores, as a potential tool in oceanography

    NASA Astrophysics Data System (ADS)

    Chamizo, Elena; López-Lora, Mercedes; Villa, María; Casacuberta, Núria; López-Gutiérrez, José María; Pham, Mai Khanh

    2015-10-01

    The performance of the 1 MV AMS system at the CNA (Centro Nacional de Aceleradores, Seville, Spain) for 236U and 239,240Pu measurements has been extensively investigated. A very promising 236U/238U abundance sensitivity of about 3 × 10-11 has been recently achieved, and background figures for 239Pu of about 106 atoms were reported in the past. These promising results lead to the use of conventional low energy AMS systems for the analysis of 236U and 239Pu and its further application in environmental studies. First 236U results obtained on our AMS system for marine samples (sediments and water) are presented here. Results of two new IAEA reference materials (IAEA-410 and IAEA-412, marine sediments from Pacific Ocean) are reported. The obtained 236U/239Pu atom ratios, of 0.12 and 0.022, respectively, show a dependency with the contamination source (i.e. local fallout from the US tests performed at the Bikini Atoll and general fallout). The results obtained for a third IAEA reference material (IAEA-381, seawater from the Irish Sea), are also presented. In the following, the uranium and plutonium isotopic compositions obtained on a set of 5 intercomparison seawater samples from the Arctic Ocean provided by the ETH Zürich are discussed. By comparing them with the obtained results on the 600 kV AMS facility Tandy at the ETH Zürich, we demonstrate the solidity of the CNA technique for 236U/238U determinations at, at least, 7 × 10-10 level. Finally, these results are discussed in their environmental context.

  5. High-resolution gamma-ray isotopic measurements of uranium plutonium samples at IPPE in support of physical inventory taking activities

    SciTech Connect

    Bezhunov, G; Kreek, S A; Mikhailov, G; Parker, W E; Sampson, T F; Savlov, A

    1999-07-01

    Measurement of various U and Pu samples by gamma-ray spectrometry were performed at the Institute of Physics and Power Engineering to support physical-inventory-taking activities under the Joint US-Russian MPC and A Program. The resulting data was analyzed by several different methods which included Canberra's MGA9.63 (Pu and MOX analysis) and MGAU (U analysis), EG and G Ortec's MGA++ (Pu and MOX analysis) and U235 (U analysis), and FRAM v2.2 (U and Pu analysis) provided by Los Alamos. The results indicate that all of these codes are capable of performing the isotopic analysis adequately. However, some additional modifications may be required to permit better measurement of some of the more unusual components in the Institute of Physics and Power Engineering (IPPE) inventory to meet the demands of inventory-taking activities.

  6. Automated gravimetric sample pretreatment using an industrial robot for the high-precision determination of plutonium by isotope dilution mass spectrometry.

    PubMed

    Surugaya, Naoki; Hiyama, Toshiaki; Watahiki, Masaru

    2008-06-01

    A robotized sample-preparation method for the determination of Pu, which is recovered by extraction reprocessing of spent nuclear fuel, by isotope dilution mass spectrometry (IDMS) is described. The automated system uses a six-axis industrial robot, whose motility is very fast, accurate, and flexible, installed in a glove box. The automation of the weighing and dilution steps enables operator-unattended sample pretreatment for the high-precision analysis of Pu in aqueous solutions. Using the developed system, the Pu concentration in a HNO(3) medium was successfully determined using a set of subsequent mass spectrometric measurements. The relative uncertainty in determining the Pu concentration by IDMS using this system was estimated to be less than 0.1% (k = 2), which is equal to that expected of a talented analyst. The operation time required was the same as that for a skilled operator.

  7. Plutonium contamination in soils and sediments at Mayak PA, Russia.

    PubMed

    Skipperud, Lindis; Salbu, Brit; Oughton, Deborah H; Drozcho, Eugeny; Mokrov, Yuri; Strand, Per

    2005-09-01

    The Mayak Production Association (Mayak PA) was established in the late 1940's to produce plutonium for the Soviet Nuclear Weapons Programme. In total, seven reactors and two reprocessing plants have been in operation. Today, the area comprises both military and civilian reactors as well as reprocessing and metallurgical plants. Authorized and accidental releases of radioactive waste have caused severe contamination to the surrounding areas. In the present study, [alpha]-spectrometry and inductively coupled plasma-mass spectrometry (ICP-MS) have been used to determine plutonium activities and isotope ratios in soil and sediment samples collected from reservoirs of the Techa River at the Mayak area and downstream Techa River. The objective of the study was to determine the total inventory of plutonium in the reservoirs and to identify the different sources contributing to the plutonium contamination. Results based on [alpha]-spectrometry and ICP-MS measurements show the presence of different sources and confirmed recent reports of civilian reprocessing at Mayak. Determination of activity levels and isotope ratios in soil and sediment samples from the Techa River support the hypothesis that most of the plutonium, like other radionuclides in the Techa River, originated from the very early waste discharges to the Techa River between 1949 and 1951. Analysis of reservoir sediment samples suggest that about 75% of the plutonium isotopes could have been released to Reservoir 10 during the early weapons production operation of the plant, and that the majority of plutonium in Reservoir 10 originates from discharges from power production or reprocessing. Enhanced 240Pu/239Pu atom ratios in river sediment upper layers (0-2 cm) between 50 and 250 km downstream from the plant indicate a contribution from other, non-fallout sources.

  8. Plutonium burdens in people living around the Rocky Flats plant. Final report 1976-79

    SciTech Connect

    Cobb, J.C.; Eversole, B.C.; Archer, P.G.; Taggart, R.; Efurd, D.W.

    1982-11-01

    A study was conducted to determine whether the tissues of people who lived near to or downwind from the Rocky Flats nuclear weapons facility in Colorado contained more plutonium than the tissues from people who lived farther away. Information was collected on the age, sex, smoking history, residence history, presence of disease, and plutonium level in selected tissues from individuals autopsied in various Eastern Colorado hospitals. The 236, 238, 239 and 240 isotopes of plutonium were determined. Plutonium levels in lung and liver tissues were affected by age and smoking history more than by distance from the Rocky Flats Plant. Though the measured 240/239 isotope ratio indicated a small contribution from Rocky Flats, the total amount of plutonium in the samples was no different than in similar samples collected from other areas of the U.S.

  9. A Graphical Examination of Uranium and Plutonium Fissility

    ERIC Educational Resources Information Center

    Reed, B. Cameron

    2008-01-01

    The issue of why only particular isotopes of uranium and plutonium are suitable for use in nuclear weapons is analyzed with the aid of graphs and semiquantitative discussions of parameters such as excitation energies, fission barriers, reaction cross-sections, and the role of processes such as [alpha]-decay and spontaneous fission. The goal is to…

  10. A Graphical Examination of Uranium and Plutonium Fissility

    ERIC Educational Resources Information Center

    Reed, B. Cameron

    2008-01-01

    The issue of why only particular isotopes of uranium and plutonium are suitable for use in nuclear weapons is analyzed with the aid of graphs and semiquantitative discussions of parameters such as excitation energies, fission barriers, reaction cross-sections, and the role of processes such as [alpha]-decay and spontaneous fission. The goal is to…

  11. METHOD OF MAKING PLUTONIUM DIOXIDE

    DOEpatents

    Garner, C.S.

    1959-01-13

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

  12. METHOD OF PRODUCING PLUTONIUM TETRAFLUORIDE

    DOEpatents

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

    1959-12-15

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

  13. Plutonium Disposition Now!

    SciTech Connect

    Buckner, M.R.

    1995-05-24

    A means for use of existing processing facilities and reactors for plutonium disposition is described which requires a minimum capital investment and allows rapid implementation. The scenario includes interim storage and processing under IAEA control, and fabrication into MOX fuel in existing or planned facilities in Europe for use in operating reactors in the two home countries. Conceptual studies indicate that existing Westinghouse four-loop designs can safety dispose of 0.94 MT of plutonium per calendar year. Thus, it would be possible to consume the expected US excess stockpile of about 50 MT in two to three units of this type, and it is highly likely that a comparable amount of the FSU excess plutonium could be deposed of in a few VVER-1000`s. The only major capital project for this mode of plutonium disposition would be the weapons-grade plutonium processing which could be done in a dedicated international facility or using existing facilities in the US and FSU under IAEA control. This option offers the potential for quick implementation at a very low cost to the governments of the two countries.

  14. Aqueous Solution Chemistry of Plutonium

    SciTech Connect

    Clark, David L.

    2014-01-28

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

  15. Lithium metal reduction of plutonium oxide to produce plutonium metal

    DOEpatents

    Coops, Melvin S.

    1992-01-01

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

  16. SULFIDE METHOD PLUTONIUM SEPARATION

    DOEpatents

    Duffield, R.B.

    1958-08-12

    A process is described for the recovery of plutonium from neutron irradiated uranium solutions. Such a solution is first treated with a soluble sullide, causing precipitation of the plutoniunn and uraniunn values present, along with those impurities which form insoluble sulfides. The precipitate is then treated with a solution of carbonate ions, which will dissolve the uranium and plutonium present while the fission product sulfides remain unaffected. After separation from the residue, this solution may then be treated by any of the usual methods, such as formation of a lanthanum fluoride precipitate, to effect separation of plutoniunn from uranium.

  17. Superconductivity in plutonium compounds

    NASA Astrophysics Data System (ADS)

    Sarrao, J. L.; Bauer, E. D.; Mitchell, J. N.; Tobash, P. H.; Thompson, J. D.

    2015-07-01

    Although the family of plutonium-based superconductors is relatively small, consisting of four compounds all of which crystallize in the tetragonal HoCoGa5 structure, these materials serve as an important bridge between the known Ce- and U-based heavy fermion superconductors and the high-temperature cuprate superconductors. Further, the partial localization of 5f electrons that characterizes the novel electronic properties of elemental plutonium appears to be central to the relatively high superconducting transition temperatures that are observed in PuCoGa5, PuRhGa5, PuCoIn5, and PuRhIn5.

  18. Plutonium in Concentrated Solutions

    SciTech Connect

    Clark, Sue B.; Delegard, Calvin H.

    2002-08-01

    Complex, high ionic strength media are used throughout the plutonium cycle, from its processing and purification in nitric acid, to waste storage and processing in alkaline solutions of concentrated electrolytes, to geologic disposal in brines. Plutonium oxidation/reduction, stability, radiolysis, solution and solid phase chemistry have been studied in such systems. In some cases, predictive models for describing Pu chemistry under such non-ideal conditions have been developed, which are usually based on empirical databases describing specific ion interactions. In Chapter 11, Non-Ideal Systems, studies on the behavior of Pu in various complex media and available model descriptions are reviewed.

  19. Management of plutonium contaminated waste

    SciTech Connect

    Grover, J.R.

    1982-01-01

    This study surveys the current management schemes for plutonium contaminated wastes arising from a reference mixed oxide fuel fabrication plant, and identifies possible areas of future research. It also outlines strategies for the future management of plutonium contaminated wastes. Topics of discussion include: the quantities and characteristics of various plutonium contaminated wastes produced by a plant; the current waste management practices for both solid and liquid plutonium contaminated wastes, considering measurement methods, transportation, storage and disposal; current practice for the problems of decommissioning and decontamination, and possible methods for the recovery of plutonium contaminated wastes.

  20. MA Doping Analysis on Breeding Capability and Protected Plutonium Production of Large FBR

    NASA Astrophysics Data System (ADS)

    Permana, Sidik; Suzuki, Mitsutoshi; Kuno, Yusuke

    2010-06-01

    Spent fuel from LWR can be seen as long-live waste if it is not recycled or as a "new fuel" resource if it is recycled into the reactors. Uranium and plutonium have been used for "new fuel" resources from LWR spent fuel as MOX fuel type which is loaded into thermal reactor or fast reactor types. Other actinides from the spent fuel such as neptunium, americium and curium as minor actinide (MA) are considered to be loaded into the reactors for specific purposes, recently. Those purposes such as for increasing protected plutonium production and breeding capability for protected plutonium as well as in the same time those amount of MA can be reduced to a small quantity as a burner or transmutation purpose. Some investigations and scientific approaches are performed in order to increase a material "barrier" in plutonium isotope composition by increasing the even mass number of plutonium isotope such as Pu-238, Pu-240 and Pu-242 as plutonium protected composition. Higher material barrier which related to intrinsic properties of plutonium isotopes with even mass number (Pu-238, Pu-240 and Pu-242), are recognized because of their intense decay heat (DH) and high spontaneous fission neutron (SFN) rates. Those even number mass of plutonium isotope contribute to some criteria of plutonium characterization which will be adopted for present study such as IAEA, Pellaud and Kessler criteria (IAEA, 1972; Pellaud, 2002; and Kessler, 2007). The present paper intends to evaluate the breeding capability as a fuel sustainability index of the reactors and to analyze the composition of protected plutonium production of large power reactor based on the FaCT FBR as reference (Ohki, et al., 2008). Three dimensional FBR core configuration has been adopted which is based on the core optimization calculation of SRAC-CITATION code as reactor core analysis and JENDL-3.3 is adopted for nuclear data library. Some MA doping materials are loaded into the blanket regions which can be considered as

  1. MA Doping Analysis on Breeding Capability and Protected Plutonium Production of Large FBR

    SciTech Connect

    Permana, Sidik; Suzuki, Mitsutoshi; Kuno, Yusuke

    2010-06-22

    Spent fuel from LWR can be seen as long-live waste if it is not recycled or as a 'new fuel' resource if it is recycled into the reactors. Uranium and plutonium have been used for 'new fuel' resources from LWR spent fuel as MOX fuel type which is loaded into thermal reactor or fast reactor types. Other actinides from the spent fuel such as neptunium, americium and curium as minor actinide (MA) are considered to be loaded into the reactors for specific purposes, recently. Those purposes such as for increasing protected plutonium production and breeding capability for protected plutonium as well as in the same time those amount of MA can be reduced to a small quantity as a burner or transmutation purpose. Some investigations and scientific approaches are performed in order to increase a material ''barrier'' in plutonium isotope composition by increasing the even mass number of plutonium isotope such as Pu-238, Pu-240 and Pu-242 as plutonium protected composition. Higher material barrier which related to intrinsic properties of plutonium isotopes with even mass number (Pu-238, Pu-240 and Pu-242), are recognized because of their intense decay heat (DH) and high spontaneous fission neutron (SFN) rates. Those even number mass of plutonium isotope contribute to some criteria of plutonium characterization which will be adopted for present study such as IAEA, Pellaud and Kessler criteria (IAEA, 1972; Pellaud, 2002; and Kessler, 2007). The present paper intends to evaluate the breeding capability as a fuel sustainability index of the reactors and to analyze the composition of protected plutonium production of large power reactor based on the FaCT FBR as reference (Ohki, et al., 2008). Three dimensional FBR core configuration has been adopted which is based on the core optimization calculation of SRAC-CITATION code as reactor core analysis and JENDL-3.3 is adopted for nuclear data library. Some MA doping materials are loaded into the blanket regions which can be considered as

  2. Plutonium Disposition by Immobilization

    SciTech Connect

    Gould, T.; DiSabatino, A.; Mitchell, M.

    2000-03-07

    The ultimate goal of the Department of Energy (DOE) Immobilization Project is to develop, construct, and operate facilities that will immobilize between 17 to 50 tonnes (MT) of U.S. surplus weapons-usable plutonium materials in waste forms that meet the ''spent fuel'' standard and are acceptable for disposal in a geologic repository. Using the ceramic can-in-canister technology selected for immobilization, surplus plutonium materials will be chemically combined into ceramic forms which will be encapsulated within large canisters of high level waste (HLW) glass. Deployment of the immobilization capability should occur by 2008 and be completed within 10 years. In support of this goal, the DOE Office of Fissile Materials Disposition (MD) is conducting development and testing (D&T) activities at four DOE laboratories under the technical leadership of Lawrence Livermore National Laboratory (LLNL). The Savannah River Site has been selected as the site for the planned Plutonium Immobilization Plant (PIP). The D&T effort, now in its third year, will establish the technical bases for the design, construction, and operation of the U. S. capability to immobilize surplus plutonium in a suitable and cost-effective manner. Based on the D&T effort and on the development of a conceptual design of the PIP, automation is expected to play a key role in the design and operation of the Immobilization Plant. Automation and remote handling are needed to achieve required dose reduction and to enhance operational efficiency.

  3. Plutonium: An introduction

    SciTech Connect

    Condit, R.H.

    1993-10-01

    This report is a summary of the history and properties of plutonium. It presents information on the atoms, comparing chemical and nuclear properties. It looks at the history of the atom, including its discovery and production methods. It summarizes the metallurgy and chemistry of the element. It also describes means of detecting and measuring the presence and quantity of the element.

  4. Atomic spectrum of plutonium

    SciTech Connect

    Blaise, J.; Fred, M.; Gutmacher, R.G.

    1984-08-01

    This report contains plutonium wavelengths, energy level classifications, and other spectroscopic data accumulated over the past twenty years at Laboratoire Aime Cotton (LAC) Argonne National Laboratory (ANL), and Lawrence Livermore National Laboratory (LLNL). The primary purpose was term analysis: deriving the energy levels in terms of quantum numbers and electron configurations, and evaluating the Slater-Condon and other parameters from the levels.

  5. Characterizing Surplus US Plutonium for Disposition - 13199

    SciTech Connect

    Allender, Jeffrey S.; Moore, Edwin N.

    2013-07-01

    The United States (US) has identified 61.5 metric tons (MT) of plutonium that is permanently excess to use in nuclear weapons programs, including 47.2 MT of weapons-grade plutonium. Surplus inventories will be stored safely by the Department of Energy (DOE) and then transferred to facilities that will prepare the plutonium for permanent disposition. The Savannah River National Laboratory (SRNL) operates a Feed Characterization program for the Office of Fissile Materials Disposition (OFMD) of the National Nuclear Security Administration (NNSA) and the DOE Office of Environmental Management (DOE-EM). SRNL manages a broad program of item tracking through process history, laboratory analysis, and non-destructive assay. A combination of analytical techniques allows SRNL to predict the isotopic and chemical properties that qualify materials for disposition through the Mixed Oxide (MOX) Fuel Fabrication Facility (MFFF). The research also defines properties that are important for other disposition paths, including disposal to the Waste Isolation Pilot Plant (WIPP) as transuranic waste (TRUW) or to high-level waste (HLW) systems. (authors)

  6. Characterizing surplus US plutonium for disposition

    SciTech Connect

    Allender, Jeffrey S.; Moore, Edwin N.

    2013-02-26

    The United States (US) has identified 61.5 metric tons (MT) of plutonium that is permanently excess to use in nuclear weapons programs, including 47.2 MT of weapons-grade plutonium. Surplus inventories will be stored safely by the Department of Energy (DOE) and then transferred to facilities that will prepare the plutonium for permanent disposition. The Savannah River National Laboratory (SRNL) operates a Feed Characterization program for the Office of Fissile Materials Disposition (OFMD) of the National Nuclear Security Administration (NNSA) and the DOE Office of Environmental Management (DOE-EM). SRNL manages a broad program of item tracking through process history, laboratory analysis, and non-destructive assay. A combination of analytical techniques allows SRNL to predict the isotopic and chemical properties that qualify materials for disposition through the Mixed Oxide (MOX) Fuel Fabrication Facility (MFFF). The research also defines properties that are important for other disposition paths, including disposal to the Waste Isolation Pilot Plant (WIPP) as transuranic waste (TRUW) or to high-level waste (HLW) systems.

  7. Plutonium Finishing Plant. Interim plutonium stabilization engineering study

    SciTech Connect

    Sevigny, G.J.; Gallucci, R.H.; Garrett, S.M.K.; Geeting, J.G.H.; Goheen, R.S.; Molton, P.M.; Templeton, K.J.; Villegas, A.J.; Nass, R.

    1995-08-01

    This report provides the results of an engineering study that evaluated the available technologies for stabilizing the plutonium stored at the Plutonium Finishing Plant located at the hanford Site in southeastern Washington. Further processing of the plutonium may be required to prepare the plutonium for interim (<50 years) storage. Specifically this document provides the current plutonium inventory and characterization, the initial screening process, and the process descriptions and flowsheets of the technologies that passed the initial screening. The conclusions and recommendations also are provided. The information contained in this report will be used to assist in the preparation of the environmental impact statement and to help decision makers determine which is the preferred technology to process the plutonium for interim storage.

  8. Plutonium utilisation in future UK PWRs

    SciTech Connect

    Thomas, G. M.; Worrall, A.

    2006-07-01

    Plutonium recycling in the form of Mixed Oxide (MOX) fuels is already a reality in over 30 reactors in Europe (in Belgium, Switzerland, Germany and France). Japan also plans to use MOX in approximately 30% of its reactors in the near future[1]. This paper describes potential near to mid-term disposition strategies for the United Kingdom's stockpile of plutonium. In order to be confident that MOX fuel can be utilised effectively in Pressurised Water Reactors (PWRs) in the UK, details are given of studies carried out recently at Nexia Solutions on PWR cores loaded with MOX containing typical UK plutonium isotopic compositions. Three dimensional steady state neutronic models of a standard Westinghouse four loop PWR design are constructed using state of the art tools (Studsvik of America's Core Management System[2, 3, 4]). Initially, a standard 18-month equilibrium UO{sub 2} fuel cycle is generated, followed by safety analyses and fuel performance calculations to demonstrate its feasibility. This equilibrium UO{sub 2} core is then gradually transitioned through loading patterns containing increasing MOX core loading fractions. Finally, an equilibrium MOX core loading pattern is determined. Technical safety analyses are also carried out on the transition cores and the final equilibrium scenario to ensure that all of the MOX cores are robust from a technical and safety viewpoint. Once these studies are completed the annual fuel throughputs for each scenario can be determined and used to produce options for managing the UK's plutonium stockpile. This work is part of a wider exercise currently being carried out by Nexia Solutions to explore the options for the safe disposition of the UK civil stockpile of separated PUO{sub 2}. (authors)

  9. 4. VIEW OF PLUTONIUM CANISTER ON CHAINVEYOR. SCRAP PLUTONIUM WAS ...

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

    4. VIEW OF PLUTONIUM CANISTER ON CHAINVEYOR. SCRAP PLUTONIUM WAS COLLECTED INTO CANS AT INDIVIDUAL WORKSTATIONS. THE CANS WERE TRANSFERRED VIA THE CHAIN CONVEYOR TO A WORKSTATION IN MODULE C WHERE THE MATERIAL WAS COMPRESSED INTO BRIQUETTES FOR LATER USE. (6/20/93) - Rocky Flats Plant, Plutonium Manufacturing Facility, North-central section of Plant, just south of Building 776/777, Golden, Jefferson County, CO

  10. [Rapid analysis of the radionuclides plutonium and americium-241 in soils].

    PubMed

    Egorov, A V; Klochkova, N V

    2009-01-01

    The paper shows it possible to perform a rapid analysis of the isotopes of plutomium and americium-241. The basis of the developed rapid analysis is X-spectrometric determination of the amount of plutonium isotopes and gamma-spectrometric determination of the radionuclide 241AM.

  11. 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.

  12. Surprising Coordination for Plutonium in the First Plutonium (III) Borate

    SciTech Connect

    Wang, Shuao; Alekseev, Evgeny V.; Depmeier, Wulf; Albrecht-Schmitt, Thomas E.

    2011-02-22

    The first plutonium(III) borate, Pu2[B12O18(OH)4Br2(H2O)3]·0.5H2O, has been prepared by reacting plutonium(III) with molten boric acid under strictly anaerobic conditions. This compound contains a three-dimensional polyborate network with triangular holes that house the plutonium(III) sites. The plutonium sites in this compound are 9- and 10-coordinate and display atypical geometries.

  13. SELECTION OF SURPLUS PLUTONIUM MATERIALS FOR DISPOSITION TO WIPP

    SciTech Connect

    Allender, J.; Mcclard, J.; Christopher, J.

    2012-06-08

    The U.S. Department of Energy (DOE) is preparing a Surplus Plutonium Disposition (SPD) Supplemental Environmental Impact Statement (SEIS). Included in the evaluation are up to 6 metric tons (MT) of plutonium in the form of impure oxides and metals for which a disposition plan has not been decided, among options that include preparation as feed for the Mixed Oxide Fuel Fabrication Facility; disposing to high-level waste through the Savannah River Site (SRS) HB Line and H Canyon; can-in-canister disposal using the SRS Defense Waste Processing Facility; and preparation for disposal at the Waste Isolation Pilot Plant (WIPP). DOE and SRS have identified at least 0.5 MT of plutonium that, because of high levels of chemical and isotopic impurities, is impractical for disposition by methods other than the WIPP pathway. Characteristics of these items and the disposition strategy are discussed.

  14. Plutonium process monitoring (PPM) system

    NASA Astrophysics Data System (ADS)

    Wong, A. S.; Ricketts, T. E.; Pansoy-Hejlvik, M. E.; Ramsey, K. B.; Hansel, K. M.; Romero, M. K.

    2000-07-01

    In mid-1980, Marsh and Pope developed an online gamma system to monitor americium, uranium and plutonium gamma rays during anion-exchange process for plutonium aqueous recovery operations. It has been shown that the real-time elution profiles of actinide impurities are important for plutonium loss via break-through, waste minimization, and process monitoring. However, the current monitoring equipment and data acquisition software are obsolete and are frequently problematic. In 1999, we redesigned the on-line gamma monitoring system in collaboration with Perkin-Elmer ORTEC (Oak Ridge, TN) to enhance and upgrade the current system. This paper describes the new integrated plutonium process monitoring (PPM) system for the aqueous plutonium recovery and anion-exchange processes at the Los Alamos Plutonium Facility.

  15. Plutonium recovery from organic materials

    DOEpatents

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

    1973-12-11

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

  16. PROCESS OF PRODUCING SHAPED PLUTONIUM

    DOEpatents

    Anicetti, R.J.

    1959-08-11

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

  17. Manufacturing of Plutonium Tensile Specimens

    SciTech Connect

    Knapp, Cameron M

    2012-08-01

    Details workflow conducted to manufacture high density alpha Plutonium tensile specimens to support Los Alamos National Laboratory's science campaigns. Introduces topics including the metallurgical challenge of Plutonium and the use of high performance super-computing to drive design. Addresses the utilization of Abaqus finite element analysis, programmable computer numerical controlled (CNC) machining, as well as glove box ergonomics and safety in order to design a process that will yield high quality Plutonium tensile specimens.

  18. Sources of plutonium in the atmosphere and stratosphere-troposphere mixing.

    PubMed

    Hirose, Katsumi; Povinec, Pavel P

    2015-10-28

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

  19. Sources of plutonium in the atmosphere and stratosphere-troposphere mixing

    NASA Astrophysics Data System (ADS)

    Hirose, Katsumi; Povinec, Pavel P.

    2015-10-01

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

  20. Sources of plutonium in the atmosphere and stratosphere-troposphere mixing

    PubMed Central

    Hirose, Katsumi; Povinec, Pavel P.

    2015-01-01

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

  1. PLUTONIUM-URANIUM ALLOY

    DOEpatents

    Coffinberry, A.S.; Schonfeld, F.W.

    1959-09-01

    Pu-U-Fe and Pu-U-Co alloys suitable for use as fuel elements tn fast breeder reactors are described. The advantages of these alloys are ease of fabrication without microcracks, good corrosion restatance, and good resistance to radiation damage. These advantages are secured by limitation of the zeta phase of plutonium in favor of a tetragonal crystal structure of the U/sub 6/Mn type.

  2. MOLDS FOR CASTING PLUTONIUM

    DOEpatents

    Anderson, J.W.; Miley, F.; Pritchard, W.C.

    1962-02-27

    A coated mold for casting plutonium comprises a mold base portion of a material which remains solid and stable at temperatures as high as the pouring temperature of the metal to be cast and having a thin coating of the order of 0.005 inch thick on the interior thereof. The coating is composed of finely divided calcium fluoride having a particle size of about 149 microns. (AEC)

  3. Welding Plutonium Storage Containers

    SciTech Connect

    HUDLOW, SL

    2004-04-20

    The outer can welder (OCW) in the FB-Line Facility at the Savannah River Site (SRS) is a Gas Tungsten Arc Weld (GTAW) system used to create outer canisters compliant with the Department of Energy 3013 Standard, DOE-STD-3013-2000, Stabilization, Packaging, and Storage of Plutonium-Bearing Materials. The key welding parameters controlled and monitored on the outer can welder Data Acquisition System (DAS) are weld amperage, weld voltage, and weld rotational speed. Inner 3013 canisters from the Bagless Transfer System that contain plutonium metal or plutonium oxide are placed inside an outer 3013 canister. The canister is back-filled with helium and welded using the outer can welder. The completed weld is screened to determine if it is satisfactory by reviewing the OCW DAS key welding parameters, performing a helium leak check, performing a visual examination by a qualified weld inspector, and performing digital radiography of the completed weld. Canisters with unsatisfactory welds are cut open and repackaged. Canisters with satisfactory welds are deemed compliant with the 3013 standard for long-term storage.

  4. The blending strategy for the plutonium immobilization program

    SciTech Connect

    Ebbinghaus, B B; Edmunds, T A; Gentry, S; Gray, L W; Riley, D C; Spingarn, J; VanKonynenburg, R A

    1999-02-12

    The Department of Energy (DOE) has declared approximately 38.2 tonnes of weapons-grade plutonium to be excess to the needs of national security, 14.3 tonnes of fuel- and reactor-grade plutonium excess to DOE needs, and anticipates an additional 7 tonnes to be declared excess to national security needs. Of this 59.5 tonnes, DOE anticipates that {approximately} 7.5 tonnes will be dispositioned as spent fuel at the Geologic Repository and {approximately} 2 tonnes will be declared below the safeguards termination limit and be discard3ed as TRU waste at WIPP. The remaining 50 tonnes of excess plutonium exists in many forms and locations around the country, and is under the control of several DOE offices. In addition to the plutonium, the feed stock also contains about 17 tonnes of depleted uranium, about 600 kg of highly enriched uranium, and many kilograms of neptunium and thorium and about 8 to 10 tonnes of tramp impurities. The Materials Disposition Program (MD) will be received materials packaged by these other Programs to disposition in a manor that meets the spent fuel standard. To minimize the cost of characterization of the feedstock and to minimize purification processes, a blending strategy will be followed. The levelization of the impurities, the plutonium isotopics, and the actinide impurities will also provide some benefits in the area of proliferation resistance. The overall strategy will be outlined and the benefits of following a blending instead of a purification program will be discussed.

  5. Simultaneous measurements of plutonium and uranium in spent-fuel dissolver solutions

    SciTech Connect

    Li, T.K.; Kuno, T.; Kitagawa, O.; Sato, S.; Kurosawa, A.; Kuno, Y.

    1997-11-01

    The authors have studied the isotope dilution gamma-ray spectrometry (IDGS) technique for simultaneous measurements of elemental concentrations and isotopic compositions for both plutonium and uranium in input spent-fuel dissolver solutions at a reprocessing plant. The technique under development includes both sample preparation and analysis methods. For simultaneous measurements of both plutonium and uranium, a critical issue is to develop a new method to keep both plutonium and uranium in the sample after they are separated from fission products. Furthermore, it is equally important to improve the analysis method so that the precision and accuracy of the plutonium analysis remain unaffected while uranium is retained in the sample. To keep both plutonium and uranium in the sample for simultaneous measurements, extraction chromatography is being studied and shows promise to achieve the goal of cosegregation of the plutonium and uranium. The technique uses U/TEVA{center_dot}Spec resin to separate fission products and recover both uranium and plutonium in the resin from dissolver solutions for subsequent measuring using high-resolution gamma-ray spectrometry. Owing to the fact that the U/Pu ratio is altered during the fission product separation phase, it is necessary to develop a method which could accurately correct for this effect. Such a method was developed using the unique decay properties of {sup 241}Pu to {sup 237}U and shows considerable promise in allowing for accurate determination of the {sup 235}U concentrations before the chemical extraction.

  6. Application of ICP-QMS for the determination of plutonium in environmental samples for safeguards purposes.

    PubMed

    Godoy, Maria Luiza D P; Godoy, José Marcus; Roldão, Luiz Alfredo

    2007-01-01

    Aiming to determine the plutonium amount as well as its isotopic composition, in particular, in swipe samples for safeguards purposes, an analytical method was developed with a plutonium separation step based on extraction chromatography using 2 cm TEVA columns and detection with quadrupole ICP-MS applying an ultra-sonic nebulizer coupled with membrane desolvation system. The method was successfully applied to New Brunswick plutonium certified reference materials as well as to Lawrence Livermore National Laboratory round robin samples, based on the round robin samples provided by the Institute for Reference Materials and Measurements (Belgium), as part of the Regular European Interlaboratory Measurement Evaluation Programme (REIMEP), campaign 16 (isotopic abundances of plutonium in plutonium nitrate samples), with a total plutonium amount between 1 and 0.25 ng per sample. After the introduction of an additional separation step, it was also possible to carry out precise and accurate total plutonium, (240)Pu/(239)Pu, (241)Pu/(239)Pu and (242)Pu/(239)Pu atom ratios determination in sediment sample showing its applicability to environmental samples in general, reaching a detection limit equivalent to 5 mBq(239)Pu kg(-1).

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

    SciTech Connect

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

    2007-06-18

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

  8. MASS MEASUREMENT UNCERTAINTY FOR PLUTONIUM ALIQUOTS ASSAYED BY CONTROLLED-POTENTIAL COULOMETRY

    SciTech Connect

    Holland, M.; Cordaro, J.

    2009-03-18

    Minimizing plutonium measurement uncertainty is essential to nuclear material control and international safeguards. In 2005, the International Organization for Standardization (ISO) published ISO 12183 'Controlled-potential coulometric assay of plutonium', 2nd edition. ISO 12183:2005 recommends a target of {+-}0.01% for the mass of original sample in the aliquot because it is a critical assay variable. Mass measurements in radiological containment were evaluated and uncertainties estimated. The uncertainty estimate for the mass measurement also includes uncertainty in correcting for buoyancy effects from air acting as a fluid and from decreased pressure of heated air from the specific heat of the plutonium isotopes.

  9. Fractionation of plutonium in environmental and bio-shielding concrete samples using dynamic sequential extraction.

    PubMed

    Qiao, Jixin; Hou, Xiaolin

    2010-03-01

    Fractionation of plutonium isotopes ((238)Pu, (239,240)Pu) in environmental samples (i.e. soil and sediment) and bio-shielding concrete from decommissioning of nuclear reactor were carried out by dynamic sequential extraction using an on-line sequential injection (SI) system combined with a specially designed extraction column. Plutonium in the fractions from the sequential extraction was separated by ion exchange chromatography and measured using alpha spectrometry. The analytical results show a higher mobility of plutonium in bio-shielding concrete, which means attention should be paid to the treatment and disposal of nuclear waste from decommissioning.

  10. Plutonium and the Rio Grande: Environmental Change and Contamination in the Nuclear Age

    NASA Astrophysics Data System (ADS)

    Leipnik, Mark

    Plutonium and the Rio Grande begins with an evocative description of the tranquility that prevailed along the Rio Grande in the halcyon days before the Manhattan Project changed the environment of this corner of New Mexico forever. Graf presents a methodology for studying the environmental impacts of the plutonium releases from facilities at Los Alamos. Specifically, he quantifies releases of various isotopes of plutonium and tracks their fate in the sediments and water bodies of the Rio Grande. Despite access to ample reliable data, his task is challenging: it requires regional-scale analysis and applications of techniques from disciplines including geomorphology, hydrology, environmental chemistry, plant physiology, and historical research.

  11. Plutonium worker dosimetry.

    PubMed

    Birchall, Alan; Puncher, M; Harrison, J; Riddell, A; Bailey, M R; Khokryakov, V; Romanov, S

    2010-05-01

    Epidemiological studies of the relationship between risk and internal exposure to plutonium are clearly reliant on the dose estimates used. The International Commission on Radiological Protection (ICRP) is currently reviewing the latest scientific information available on biokinetic models and dosimetry, and it is likely that a number of changes to the existing models will be recommended. The effect of certain changes, particularly to the ICRP model of the respiratory tract, has been investigated for inhaled forms of (239)Pu and uncertainties have also been assessed. Notable effects of possible changes to respiratory tract model assumptions are (1) a reduction in the absorbed dose to target cells in the airways, if changes under consideration are made to the slow clearing fraction and (2) a doubling of absorbed dose to the alveolar region for insoluble forms, if evidence of longer retention times is taken into account. An important factor influencing doses for moderately soluble forms of (239)Pu is the extent of binding of dissolved plutonium to lung tissues and assumptions regarding the extent of binding in the airways. Uncertainty analyses have been performed with prior distributions chosen for application in epidemiological studies. The resulting distributions for dose per unit intake were lognormal with geometric standard deviations of 2.3 and 2.6 for nitrates and oxides, respectively. The wide ranges were due largely to consideration of results for a range of experimental data for the solubility of different forms of nitrate and oxides. The medians of these distributions were a factor of three times higher than calculated using current default ICRP parameter values. For nitrates, this was due to the assumption of a bound fraction, and for oxides due mainly to the assumption of slower alveolar clearance. This study highlights areas where more research is needed to reduce biokinetic uncertainties, including more accurate determination of particle transport rates

  12. Application of Prompt Gamma-Ray Analysis to Identify Electrorefining Salt-Bearing Plutonium Oxide at the Plutonium Finishing Plant

    SciTech Connect

    Fazzari, Dennis M.; Jones, Susan A.; Delegard, Calvin H. )

    2003-09-25

    Prompt gamma-ray analysis is being implemented at the Plutonium Finishing Plant (PFP) to screen impure plutonium oxide inventory items, received in the mid-1980s from the Rocky Flats Plant, for the presence of sodium chloride and potassium chloride salts from the electrorefining process. A large fraction of these items are suspected to contain electrorefining salts. Because the salts evaporate at the=950C stabilization temperature mandated for long-term storage under the U.S. Department of Energy plutonium oxide stabilization and storage criteria to plug and corrode process equipment, items found to have these salts qualify for thermal stabilization at 750C. The prompt gamma ray energies characteristic of sodium, potassium, chlorine, and other low atomic weight elements arise from the interaction the light elements with alpha radiation from plutonium and americium radioactive decay. High-resolution gamma ray spectrometers designed to detect energies up to {approx}4.5 MeV are used to gather the high-energy prompt gamma spectra.Observation of the presence of the high-energy gamma peaks representing the natural chlorine-35, sodium-23, and potassium-39 isotopes and the sodium-to-chlorine peak area ratios in the range for plutonium oxide materials known to contain the electrorefining salts give the evidence needed to identify plutonium oxide materials at the PFP that qualify for the lower-temperature processing. Conversely, the absence of these telltale signals in the prompt gamma analysis provides evidence that the materials do not contain the electrorefining salts. Furthermore, based on calibrations using known assayed items, semiquantitative measurement of the quantity of chlorine present in materials containing electrorefining salt also can be performed by using the count rates observed for the chlorine peak, the plutonium quantity present in the measured item, and the plutonium- and chlorine-specific response of the gamma detection system. The origin and

  13. Plutonium Focus Area research and development plan. Revision 1

    SciTech Connect

    1996-11-01

    The Department of Energy (DOE) committed to a research and development program to support the technology needs for converting and stabilizing its nuclear materials for safe storage. The R and D Plan addresses five of the six material categories from the 94-1 Implementation Plan: plutonium (Pu) solutions, plutonium metals and oxides, plutonium residues, highly enriched uranium, and special isotopes. R and D efforts related to spent nuclear fuel (SNF) stabilization were specifically excluded from this plan. This updated plan has narrowed the focus to more effectively target specific problem areas by incorporating results form trade studies. Specifically, the trade studies involved salt; ash; sand, slag, and crucible (SS and C); combustibles; and scrub alloy. The plan anticipates possible disposition paths for nuclear materials and identifies resulting research requirements. These requirements may change as disposition paths become more certain. Thus, this plan represents a snapshot of the current progress and will continue to be updated on a regular basis. The paper discusses progress in safeguards and security, plutonium stabilization, special isotopes stabilization, highly-enriched uranium stabilization--MSRE remediation project, storage technologies, engineered systems, core technology, and proposed DOE/Russian technology exchange projects.

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

    DOEpatents

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

    1962-11-13

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

  15. Measurement of plutonium in spent nuclear fuel by self-induced x-ray fluorescence

    SciTech Connect

    Hoover, Andrew S; Rudy, Cliff R; Tobin, Steve J; Charlton, William S; Stafford, A; Strohmeyer, D; Saavadra, S

    2009-01-01

    Direct measurement of the plutonium content in spent nuclear fuel is a challenging problem in non-destructive assay. The very high gamma-ray flux from fission product isotopes overwhelms the weaker gamma-ray emissions from plutonium and uranium, making passive gamma-ray measurements impossible. However, the intense fission product radiation is effective at exciting plutonium and uranium atoms, resulting in subsequent fluorescence X-ray emission. K-shell X-rays in the 100 keV energy range can escape the fuel and cladding, providing a direct signal from uranium and plutonium that can be measured with a standard germanium detector. The measured plutonium to uranium elemental ratio can be used to compute the plutonium content of the fuel. The technique can potentially provide a passive, non-destructive assay tool for determining plutonium content in spent fuel. In this paper, we discuss recent non-destructive measurements of plutonium X-ray fluorescence (XRF) signatures from pressurized water reactor spent fuel rods. We also discuss how emerging new technologies, like very high energy resolution microcalorimeter detectors, might be applied to XRF measurements.

  16. Study of the IDGS technique for mixed plutonium-uranium (MOX) samples

    SciTech Connect

    Li, T. K.; Vo, Duc T.; Sumi, M.; Suzuki, T.

    2004-01-01

    The isotope dilution gamma-ray spectrometry (IDGS) technique has been demonstrated for simultaneously measuring concentrations and isotopic compositions of plutonium in spent-fuel input dissolver solutions. For timely analyzing nuclear materials on the purpose of material accountancy and quality control/assurance, we have performed a feasibility study to implement the IDGS for measuring mixed plutonium-uranium oxide (MOX) samples at the Plutonium Fuel Center (PFC) of Japan Nuclear Cycle Development Institute (JNC). Proof-of-principle experiments and analysis have been conducted for developing simultaneous plutonium and uranium measurements in MOX samples with wide variation of Pu/U ratios including powder, pellets and process scraps from the MOX fuel fabrication plant at PFC. We have shown that FRAM can be used with the IDGS technique to simultaneously determine plutonium and uranium isotopic compositions and concentrations in MOX samples at PFC, JNC. The uncertainties of the results are somewhat large due to weak statistics. If better statistics are obtained by either using more plutonium in the measurements, acquire the data for longer time, or using higher efficiency detector then the results can be better. The accuracy of the results can also be improved by a factor of 2-3 by using the generalized IDGS technique instead of this traditional IDGS.

  17. PREPARATION OF HALIDES OF PLUTONIUM

    DOEpatents

    Garner, C.S.; Johns, I.B.

    1958-09-01

    A dry chemical method is described for preparing plutonium halides, which consists in contacting plutonyl nitrate with dry gaseous HCl or HF at an elevated temperature. The addition to the reaction gas of a small quantity of an oxidizing gas or a reducing gas will cause formation of the tetra- or tri-halide of plutonium as desired.

  18. Photochemical preparation of plutonium pentafluoride

    DOEpatents

    Rabideau, Sherman W.; Campbell, George M.

    1987-01-01

    The novel compound plutonium pentafluoride may be prepared by the photodissociation of gaseous plutonium hexafluoride. It is a white solid of low vapor pressure, which consists predominantly of a face-centered cubic structure with a.sub.o =4.2709.+-.0.0005 .ANG..

  19. PLUTONIUM-URANIUM-TITANIUM ALLOYS

    DOEpatents

    Coffinberry, A.S.

    1959-07-28

    A plutonium-uranium alloy suitable for use as the fuel element in a fast breeder reactor is described. The alloy contains from 15 to 60 at.% titanium with the remainder uranium and plutonium in a specific ratio, thereby limiting the undesirable zeta phase and rendering the alloy relatively resistant to corrosion and giving it the essential characteristic of good mechanical workability.

  20. METHOD OF REDUCING PLUTONIUM COMPOUNDS

    DOEpatents

    Johns, I.B.

    1958-06-01

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

  1. SEPARATION OF PLUTONIUM FROM URANIUM

    DOEpatents

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

    1959-12-15

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

  2. SOLVENT EXTRACTION PROCESS FOR PLUTONIUM

    DOEpatents

    Anderson, H.H.; Asprey, L.B.

    1960-02-01

    A process of separating plutonium in at least the tetravalent state from fission products contained in an aqueous acidic solution by extraction with alkyl phosphate is reported. The plutonium can then be back-extracted from the organic phase by contact with an aqueous solution of sulfuric, phosphoric, or oxalic acid as a complexing agent.

  3. PLUTONIUM-CERIUM-COPPER ALLOYS

    DOEpatents

    Coffinberry, A.S.

    1959-05-12

    A low melting point plutonium alloy useful as fuel is a homogeneous liquid metal fueled nuclear reactor is described. Vessels of tungsten or tantalum are useful to contain the alloy which consists essentially of from 10 to 30 atomic per cent copper and the balance plutonium and cerium. with the plutontum not in excess of 50 atomic per cent.

  4. Plutonium Multiple Recycling In PWRs

    SciTech Connect

    Nigon, Jean-Louis; Lenain, Richard; Zaetta, Alain

    2002-07-01

    Reprocessing and recycling open the road to a sustainable management of nuclear materials and an environment friendly management of nuclear waste. However, long or very long term recycling implies fast neutron reactors. High burn-ups of irradiated standard UO{sub 2} fuel as well as recycling of plutonium fuel in thermal reactors lead to a 'degradation' of plutonium that means a low fissile content, which is hardly compatible with recycling in LWRs. Thus the question of plutonium management has been raised; although there are some limitations, a truly large variety of options do exist; no one of the presently selected ways of plutonium management is a dead end road. Among these various options, some are fully compatible with the existing reactors and may be considered for the mid term future; they offer a competitive management of plutonium during the transition from thermal to fast reactors. (authors)

  5. System design document for the plutonium stabilization and packaging system

    SciTech Connect

    1996-05-08

    The objective of this system is to stabilize and package plutonium metals and oxides of greater than 50% wt, as well as other selected isotopes, in accordance with the requirements for DOE standards for safe storage of these materials for 50 years. This document describes the highest level design information and user characteristics from an operational perspective. It provides guidance for developing procurement and installation specifications, interface requirements, and test plans.

  6. Improved plutonium identification and characterization results with NaI(Tl) detector using ASEDRA

    NASA Astrophysics Data System (ADS)

    Detwiler, R.; Sjoden, G.; Baciak, J.; LaVigne, E.

    2008-04-01

    The ASEDRA algorithm (Advanced Synthetically Enhanced Detector Resolution Algorithm) is a tool developed at the University of Florida to synthetically enhance the resolved photopeaks derived from a characteristically poor resolution spectra collected at room temperature from scintillator crystal-photomultiplier detector, such as a NaI(Tl) system. This work reports on analysis of a side-by-side test comparing the identification capabilities of ASEDRA applied to a NaI(Tl) detector with HPGe results for a Plutonium Beryllium (PuBe) source containing approximately 47 year old weapons-grade plutonium (WGPu), a test case of real-world interest with a complex spectra including plutonium isotopes and 241Am decay products. The analysis included a comparison of photopeaks identified and photopeak energies between the ASEDRA and HPGe detector systems, and the known energies of the plutonium isotopes. ASEDRA's performance in peak area accuracy, also important in isotope identification as well as plutonium quality and age determination, was evaluated for key energy lines by comparing the observed relative ratios of peak areas, adjusted for efficiency and attenuation due to source shielding, to the predicted ratios from known energy line branching and source isotopics. The results show that ASEDRA has identified over 20 lines also found by the HPGe and directly correlated to WGPu energies.

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

    NASA Astrophysics Data System (ADS)

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

    2017-01-01

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

  8. The use of carbohydrazide for plutonium concentration stripping in separator with inert packing

    SciTech Connect

    Dvoeglazov, K.; Volk, V.; Zverev, D.; Veselov, S.; Krivitskiy, Y.; Alekseenko, S.; Alekseenko, V.

    2013-07-01

    For the purpose of removing plutonium from uranium- plutonium extract it is proposed to employ concentration stripping process with the use of separator and a new reducing reagent: Carbohydrazide CO(N{sub 2}H{sub 3}){sub 2}. Using plutonium stripping from solution simulating the composition of extract of spent nuclear fuel from VVER-1000 reactor (without γ-emitting isotopes), with O: A ratio of = 28, a product solution was obtained containing 17.8 g/l of plutonium, 29.2 g/l of uranium and more than 1 g/l of technetium. The experiment on real spent fuel from VVER-1000 with burn-up of more than 50 GW*d/t of uranium after 17 year exposure, performed in the shielded box of FSUE 'MCP', confirmed the effectiveness and feasibility of the proposed process. Through concentration stripping (O:A = 20), a plutonium product solution was obtained with a part of uranium with the following composition: [U] = 150 g/l; [Pu] = 23,5 g/l; [Np] = 1,7 g/l, [Tc] = 1.5 g/l; gamma exposure rate - 0,022 mR/s*l. Direct extraction of plutonium in this operation was 95.3%, the rest of plutonium is refluxing to the preceding stage of the extraction cycle. A process flow diagram with organization of plutonium recycling is proposed, allowing for its complete removal into a single stream. Carbohydrazide is an effective reducing agent of plutonium (IV), ensuring the stability of uranium-plutonium separation process. (authors)

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

    DOEpatents

    Fried, S.; Baumbach, H.L.

    1959-12-01

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

  10. Solubility of Plutonium (IV) Oxalate During Americium/Curium Pretreatment

    SciTech Connect

    Rudisill, T.S.

    1999-08-11

    Approximately 15,000 L of solution containing isotopes of americium and curium (Am/Cm) will undergo stabilization by vitrification at the Savannah River Site (SRS). Prior to vitrification, an in-tank pretreatment will be used to remove metal impurities from the solution using an oxalate precipitation process. Material balance calculations for this process, based on solubility data in pure nitric acid, predict approximately 80 percent of the plutonium in the solution will be lost to waste. Due to the uncertainty associated with the plutonium losses during processing, solubility experiments were performed to measure the recovery of plutonium during pretreatment and a subsequent precipitation process to prepare a slurry feed for a batch melter. A good estimate of the plutonium content of the glass is required for planning the shipment of the vitrified Am/Cm product to Oak Ridge National Laboratory (ORNL).The plutonium solubility in the oxalate precipitation supernate during pretreatment was 10 mg/mL at 35 degrees C. In two subsequent washes with a 0.25M oxalic acid/0.5M nitric acid solution, the solubility dropped to less than 5 mg/mL. During the precipitation and washing steps, lanthanide fission products in the solution were mostly insoluble. Uranium, and alkali, alkaline earth, and transition metal impurities were soluble as expected. An elemental material balance for plutonium showed that greater than 94 percent of the plutonium was recovered in the dissolved precipitate. The recovery of the lanthanide elements was generally 94 percent or higher except for the more soluble lanthanum. The recovery of soluble metal impurities from the precipitate slurry ranged from 15 to 22 percent. Theoretically, 16 percent of the soluble oxalates should have been present in the dissolved slurry based on the dilution effects and volumes of supernate and wash solutions removed. A trace level material balance showed greater than 97 percent recovery of americium-241 (from the beta dec

  11. Low temperature oxidation of plutonium

    SciTech Connect

    Nelson, Art J.; Roussel, Paul

    2013-05-15

    The initial oxidation of gallium stabilized {delta}-plutonium metal at 193 K has been followed using x-ray photoelectron spectroscopy. On exposure to Langmuir quantities of oxygen, plutonium rapidly forms a trivalent oxide followed by a tetravalent plutonium oxide. The growth modes of both oxides have been determined. Warming the sample in vacuum, the tetravalent oxide reduces to the trivalent oxide. The kinetics of this reduction reaction have followed and the activation energy has been determined to be 38.8 kJ mol{sup -1}.

  12. SOLVENT EXTRACTION PROCESS FOR PLUTONIUM

    DOEpatents

    Seaborg, G.T.

    1959-04-14

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

  13. Tags to Track Illicit Uranium and Plutonium

    SciTech Connect

    Haire, M. Jonathan; Forsberg, Charles W.

    2007-07-01

    With the expansion of nuclear power, it is essential to avoid nuclear materials from falling into the hands of rogue nations, terrorists, and other opportunists. This paper examines the idea of detection and attribution tags for nuclear materials. For a detection tag, it is proposed to add small amounts [about one part per billion (ppb)] of {sup 232}U to enriched uranium to brighten its radioactive signature. Enriched uranium would then be as detectable as plutonium and thus increase the likelihood of intercepting illicit enriched uranium. The use of rare earth oxide elements is proposed as a new type of 'attribution' tag for uranium and thorium from mills, uranium and plutonium fuels, and other nuclear materials. Rare earth oxides are chosen because they are chemically compatible with the fuel cycle, can survive high-temperature processing operations in fuel fabrication, and can be chosen to have minimal neutronic impact within the nuclear reactor core. The mixture of rare earths and/or rare earth isotopes provides a unique 'bar code' for each tag. If illicit nuclear materials are recovered, the attribution tag can identify the source and lot of nuclear material, and thus help police reduce the possible number of suspects in the diversion of nuclear materials based on who had access. (authors)

  14. Plutonium Detection with Straw Neutron Detectors

    SciTech Connect

    Mukhopadhyay, Sanjoy; Maurer, Richard; Guss, Paul

    2014-03-27

    A kilogram of weapons grade plutonium gives off about 56,000 neutrons per second of which 55,000 neutrons come from spontaneous fission of 240Pu (~6% by weight of the total plutonium). Actually, all even numbered isotopes (238Pu, 240Pu, and 242Pu) produce copious spontaneous fission neutrons. These neutrons induce fission in the surrounding fissile 239Pu with an approximate multiplication of a factor of ~1.9. This multiplication depends on the shape of the fissile materials and the surrounding material. These neutrons (typically of energy 2 MeV and air scattering mean free path >100 meters) can be detected 100 meters away from the source by vehicle-portable neutron detectors. [1] In our current studies on neutron detection techniques, without using 3He gas proportional counters, we designed and developed a portable high-efficiency neutron multiplicity counter using 10B-coated thin tubes called straws. The detector was designed to perform like commercially available fission meters (manufactured by Ortec Corp.) except instead of using 3He gas as a neutron conversion material, we used a thin coating of 10B.

  15. Probing phonons in plutonium

    SciTech Connect

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

    2010-11-16

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

  16. Geometry-based multiplication-corrected analysis for neutron coincidence assay of impure plutonium materials

    SciTech Connect

    Langner, D.G.; Russo, P.A.

    1991-01-01

    We have developed a technique to assay impure, plutonium-bearing materials using passive neutron coincidence counting. The technique can be applied to any impure, plutonium-bearing material category whose matrix constituents are approximately constant, whose self- multiplication is low-to-moderate, whose plutonium isotopic composition is known and not substantially varying, and whose bulk geometry is measurable or can be derived. The technique requires a set of reference materials with well-characterized plutonium contents. The reference materials are measured once to derive a calibration that is specific to the neutron detector and the material category. This technique has been applied to four categories of material: molten salt extraction residues; plutonium fluoride samples having a variable salt matrix; impure plutonium oxides; and, for comparison, pure plutonium oxides. Assays accurate to 4% (1{sigma}) were obtained for these impure materials measured in an HLNCII. Better results should be obtainable with neutron detectors with better response characteristics. 11 refs., 6 figs., 6 tabs.

  17. Measurement and interpretation of plutonium spectra

    SciTech Connect

    Blaise, J.; Fred, M.S.; Carnall, W.T.; Crosswhite, H.M.; Crosswhite, H.

    1982-01-01

    The atomic spectroscopic data available for plutonium are among the rickest of any in the periodic system. They include high-resolution grating and Fourier-transform spectra as well as extensive Zeeman and isotope-shift studies. We summarize the present status of the term analysis and cite the configurations that have been identified. A least-squares adjustment of a parametric Hamiltonian for configurations of both Pu I and Pu II has shown that almost all of the expected low levels are now known. The use of a model Hamiltonian applicable to both lanthanide and actinide atomic species has been applied to the low configurations of Pu I and Pu II making use of trends predicted by ab initio calculations. This same model has been used to describe the energy levels of Pu/sup 3 +/ in LaCl/sub 3/, and an extension has permitted preliminary calculations of the spectra of other valence states.

  18. Crashworthy sealed pressure vessel for plutonium transport

    SciTech Connect

    Andersen, J.A.

    1980-01-01

    A rugged transportation package for the air shipment of radioisotopic materials was recently developed. This package includes a tough, sealed, stainless steel inner containment vessel of 1460 cc capacity. This vessel, intended for a mass load of up to 2 Kg PuO/sub 2/ in various isotopic forms (not to exceed 25 watts thermal activity), has a positive closure design consisting of a recessed, shouldered lid fastened to the vessel body by twelve stainless-steel bolts; sealing is accomplished by a ductile copper gasket in conjunction with knife-edge sealing beads on both the body and lid. Follow-on applications of this seal in newer, smaller packages for international air shipments of plutonium safeguards samples, and in newer, more optimized packages for greater payload and improved efficiency and utility, are briefly presented.

  19. Analysis of naturally produced technetium and plutonium in geologic materials.

    PubMed

    Dixon, P; Curtis, D B; Musgrave, J; Roensch, F; Roach, J; Rokop, D

    1997-05-01

    In uncontaminated natural materials, plutonium and technetium exist exclusively as products (daughters) of nuclear reactions in which uranium is the principal reactant (parent). Under conditions of chemical stability over geologic periods of time, the relative abundances of daughter and parent elements are fixed by the rates of nuclear reactions and the decay of the daughter radionuclide. The state of this nuclear secular equilibrium condition is the primary basis of the geochemical study of these elements in nature. Thus, it is critical that nuclear parent and daughter abundances are measured in the same sample. We have developed a quantitative procedure for measuring subpicogram quantities of plutonium and technetium in gram quantities of geologic matrices such as uranium ores. The procedure takes advantage of the aggressive properties of sodium peroxide/hydroxide fusion to ensure complete dissolution and homogenization of complex materials, the precision provided by isotope dilution techniques, and the extreme sensitivity offered by thermal ionization mass spectrometry. Using this technique, a quantitative aliquot can be removed for uranium analysis by isotope dilution thermal ionization mass spectrometry or α spectrometry. Although the application of the procedure is unique, the analytical concepts may find more general application in studies of environmental contamination by nuclear materials. To assess the precision and accuracy of the analytical results, blanks and standards were analyzed routinely for a 1-year period to ensure quality control of our sample analyses. The average technetium blank is 5 ± 4 fg (n = 8), and that for plutonium is 0.17 ± 0.15 pg (n = 7). Thus, the detection limit for technetium (defined as 3 times the standard deviation of the average blank) is 11 fg, and that for plutonium is 0.44 pg. To assess the procedural precision, Canadian Reference Material BL-5 was analyzed routinely with samples. The results of seven replicate

  20. TERNARY ALLOY-CONTAINING PLUTONIUM

    DOEpatents

    Waber, J.T.

    1960-02-23

    Ternary alloys of uranium and plutonium containing as the third element either molybdenum or zirconium are reported. Such alloys are particularly useful as reactor fuels in fast breeder reactors. The alloy contains from 2 to 25 at.% of molybdenum or zirconium, the balance being a combination of uranium and plutonium in the ratio of from 1 to 9 atoms of uranlum for each atom of plutonium. These alloys are prepared by melting the constituent elements, treating them at an elevated temperature for homogenization, and cooling them to room temperature, the rate of cooling varying with the oomposition and the desired phase structure. The preferred embodiment contains 12 to 25 at.% of molybdenum and is treated by quenching to obtain a body centered cubic crystal structure. The most important advantage of these alloys over prior binary alloys of both plutonium and uranium is the lack of cracking during casting and their ready machinability.

  1. METHOD OF PREPARING PLUTONIUM TETRAFLUORIDE

    DOEpatents

    Beede, R.L.; Hopkins, H.H. Jr.

    1959-11-17

    C rystalline plutonium tetrafluoride is precipitated from aqueous up to 1.6 N mineral acid solutions of a plutorium (IV) salt with fluosilicic acid anions, preferably at room temperature. Hydrogen fluoride naay be added after precipitation to convert any plutonium fluosilicate to the tetrafluoride and any silica to fluosilicic acid. This process results in a purer product, especially as to iron and aluminum, than does the precipitation by the addition of hydrogen fluoride.

  2. IODATE METHOD FOR PURIFYING PLUTONIUM

    DOEpatents

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

    1958-10-14

    A method is presented for removing radioactive fission products from aqueous solutions containing such fission products together with plutonium. This is accomplished by incorporating into such solutions a metal iodate precipitate to remove fission products which form insoluble iodates. Suitable metal iodates are those of thorium and cerium. The plutonium must be in the hexavalent state and the pH of the solution must be manintained at less than 2.

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

    PubMed

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

    2013-10-18

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

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

    PubMed Central

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

    2013-01-01

    The contamination of Japan after the Fukushima accident has been investigated mainly for volatile fission products, but only sparsely for actinides such as plutonium. Only small releases of actinides were estimated in Fukushima. Plutonium is still omnipresent in the environment from previous atmospheric nuclear weapons tests. We investigated soil and plants sampled at different hot spots in Japan, searching for reactor-borne plutonium using its isotopic ratio 240Pu/239Pu. By using accelerator mass spectrometry, we clearly demonstrated the release of Pu from the Fukushima Daiichi power plant: While most samples contained only the radionuclide signature of fallout plutonium, there is at least one vegetation sample whose isotope ratio (0.381 ± 0.046) evidences that the Pu originates from a nuclear reactor (239+240Pu activity concentration 0.49 Bq/kg). Plutonium content and isotope ratios differ considerably even for very close sampling locations, e.g. the soil and the plants growing on it. This strong localization indicates a particulate Pu release, which is of high radiological risk if incorporated. PMID:24136192

  5. Final Report on Isotope Ratio Techniques for Light Water Reactors

    SciTech Connect

    Gerlach, David C.; Gesh, Christopher J.; Hurley, David E.; Mitchell, Mark R.; Meriwether, George H.; Reid, Bruce D.

    2009-07-01

    The Isotope Ratio Method (IRM) is a technique for estimating the energy or plutonium production in a fission reactor by measuring isotope ratios in non-fuel reactor components. The isotope ratios in these components can then be directly related to the cumulative energy production with standard reactor modeling methods.

  6. The Dynamic Movement of Plutonium in an Underground Nuclear Test with Implications for the Contamination of Groundwater

    SciTech Connect

    Smith, D K; Williams, R W

    2003-03-25

    The recent discovery of the migration of plutonium in groundwater away from underground nuclear tests at the Nevada Test Site has spawned considerable interest in the mechanisms by which plutonium may be released to the environment by a nuclear test. A suite of solid debris samples was collected during drilling through an expended test cavity and the overlying collapse chimney. Uranium and plutonium were analyzed for isotope ratios and concentration using high precision magnetic sector inductively coupled mass spectrometry. The data unequivocally shows that plutonium may be dispersed throughout the cavity and chimney environment at the time of the detonation. The {sup 239}Pu/{sup 240}Pu ratios are also fractionated relative to initial plutonium isotope ratio for the test device. Fractionation is the result of the volatilization of uranium and production of {sup 239}Pu by the reaction {sup 238}U (n,{gamma}). We conclude that for the test under consideration plutonium was deposited outside of the confines of the cavity by dynamic processes in early-time and it is this plutonium that is most likely first transferred to the groundwater regime.

  7. Photochemical isotope separation

    DOEpatents

    Robinson, C.P.; Jensen, R.J.; Cotter, T.P.; Greiner, N.R.; Boyer, K.

    1987-04-28

    A process is described for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium and plutonium. 8 figs.

  8. Photochemical isotope separation

    DOEpatents

    Robinson, C. Paul; Jensen, Reed J.; Cotter, Theodore P.; Greiner, Norman R.; Boyer, Keith

    1987-01-01

    A process for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium and plutonium.

  9. Recent plutonium science and technology at ORNL

    SciTech Connect

    Bell, J.T.

    1985-01-01

    Plutonium research and development (R and D) at ORNL has generally followed development of the nuclear fuel cycle. Basic plutonium chemistry studies have diminished since the mid-1970s; however, significant efforts have been made recently to determine fundamental characteristics of the aqueous plutonium polymer and to develop thermodynamic representations of plutonium oxides. Some studies have also been made on plutonium phosphates related to waste isolation and on definition of the oxidation states of environmental plutonium. The remaining work has been supported by the Consolidated Fuel Reprocessing Program (CFRP) and includes: (1) establishment of boundary limits for polymer formation in Purex systems; (2) preparation of mixed uranium-plutonium oxide microspheres by internal gelation sol-gel techniques; (3) direct thermal denitration of aqueous systems; and (4) plutonium/uranium extraction from spent fast reactor fuels.

  10. Plutonium and americium separation from salts

    DOEpatents

    Hagan, Paul G.; Miner, Frend J.

    1976-01-01

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

  11. Plutonium focus area

    SciTech Connect

    1996-08-01

    To ensure research and development programs focus on the most pressing environmental restoration and waste management problems at the U.S. Department of Energy (DOE), the Assistant Secretary for the Office of Environmental Management (EM) established a working group in August 1993 to implement a new approach to research and technology development. As part of this new approach, EM developed a management structure and principles that led to the creation of specific Focus Areas. These organizations were designed to focus the scientific and technical talent throughout DOE and the national scientific community on the major environmental restoration and waste management problems facing DOE. The Focus Area approach provides the framework for intersite cooperation and leveraging of resources on common problems. After the original establishment of five major Focus Areas within the Office of Technology Development (EM-50, now called the Office of Science and Technology), the Nuclear Materials Stabilization Task Group (EM-66) followed the structure already in place in EM-50 and chartered the Plutonium Focus Area (PFA). The following information outlines the scope and mission of the EM, EM-60, and EM-66 organizations as related to the PFA organizational structure.

  12. Plutonium solution analyzer

    SciTech Connect

    Burns, D.A.

    1994-09-01

    A fully automated analyzer has been developed for plutonium solutions. It was assembled from several commercially available modules, is based upon segmented flow analysis, and exhibits precision about an order of magnitude better than commercial units (0.5%-O.05% RSD). The system was designed to accept unmeasured, untreated liquid samples in the concentration range 40-240 g/L and produce a report with sample identification, sample concentrations, and an abundance of statistics. Optional hydraulics can accommodate samples in the concentration range 0.4-4.0 g/L. Operating at a typical rate of 30 to 40 samples per hour, it consumes only 0.074 mL of each sample and standard, and generates waste at the rate of about 1.5 mL per minute. No radioactive material passes through its multichannel peristaltic pump (which remains outside the glovebox, uncontaminated) but rather is handled by a 6-port, 2-position chromatography-type loop valve. An accompanying computer is programmed in QuickBASIC 4.5 to provide both instrument control and data reduction. The program is truly user-friendly and communication between operator and instrument is via computer screen displays and keyboard. Two important issues which have been addressed are waste minimization and operator safety (the analyzer can run in the absence of an operator, once its autosampler has been loaded).

  13. PROCESS OF SEPARATING PLUTONIUM FROM URANIUM

    DOEpatents

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

    1958-09-01

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

  14. Plutonium Proliferation: The Achilles Heel of Disarmament

    SciTech Connect

    Leventhal, Paul

    2001-02-07

    Plutonium is a byproduct of nuclear fission, and it is produced at the rate of about 70 metric tons a year in the world's nuclear power reactors. Concerns about civilian plutonium ran high in the 1970s and prompted enactment of the Nuclear Non-Proliferation Act of 1978 to give the United States a veto over separating plutonium from U.S.-supplied uranium fuel. Over the years, however, so-called reactor-grade plutonium has become the orphan issue of nuclear non-proliferation, largely as a consequence of pressures from plutonium-separating countries. The demise of the fast breeder reactor and the reluctance of utilities to introduce plutonium fuel in light-water reactors have resulted in large surpluses of civilian, weapons-usable plutonium, which now approach in size the 250 tons of military plutonium in the world. Yet reprocessing of spent fuel for recovery and use of plutonium proceeds apace outside the United States and threatens to overwhelm safeguards and security measures for keeping this material out of the hands of nations and terrorists for weapons. A number of historical and current developments are reviewed to demonstrate that plutonium commerce is undercutting efforts both to stop the spread of nuclear weapons and to work toward eliminating existing nuclear arsenals. These developments include the breakdown of U.S. anti-plutonium policy, the production of nuclear weapons by India with Atoms-for-Peace plutonium, the U.S.-Russian plan to introduce excess military plutonium as fuel in civilian power reactors, the failure to include civilian plutonium and bomb-grade uranium in the proposed Fissile Material Cutoff Treaty, and the perception of emerging proliferation threats as the rationale for development of a ballistic missile defense system. Finally, immobilization of separated plutonium in high-level waste is explored as a proliferation-resistant and disarmament-friendly solution for eliminating excess stocks of civilian and military plutonium.

  15. Selecting a plutonium vitrification process

    SciTech Connect

    Jouan, A.

    1996-05-01

    Vitrification of plutonium is one means of mitigating its potential danger. This option is technically feasible, even if it is not the solution advocated in France. Two situations are possible, depending on whether or not the glass matrix also contains fission products; concentrations of up to 15% should be achievable for plutonium alone, whereas the upper limit is 3% in the presence of fission products. The French continuous vitrification process appears to be particularly suitable for plutonium vitrification: its capacity is compatible with the required throughout, and the compact dimensions of the process equipment prevent a criticality hazard. Preprocessing of plutonium metal, to convert it to PuO{sub 2} or to a nitric acid solution, may prove advantageous or even necessary depending on whether a dry or wet process is adopted. The process may involve a single step (vitrification of Pu or PuO{sub 2} mixed with glass frit) or may include a prior calcination step - notably if the plutonium is to be incorporated into a fission product glass. It is important to weigh the advantages and drawbacks of all the possible options in terms of feasibility, safety and cost-effectiveness.

  16. Overview of Modeling and Simulations of Plutonium Aging

    SciTech Connect

    Schwartz, A J; Wolfer, W G

    2007-04-24

    Computer-aided materials research is now an integral part of science and technology. It becomes particularly valuable when comprehensive experimental investigations and materials testing are too costly, hazardous, or of excessive duration; then, theoretical and computational studies can supplement and enhance the information gained from limited experimental data. Such is the case for improving our fundamental understanding of the properties of aging plutonium in the nuclear weapons stockpile. The question of the effects of plutonium aging on the safety, security, and reliability of the nuclear weapons stockpile emerged after the United States closed its plutonium manufacturing facility in 1989 and decided to suspend any further underground testing of nuclear weapons in 1992. To address this, the Department of Energy's National Nuclear Security Administration (NNSA) initiated a research program to investigate plutonium aging, i.e., the changes with time of properties of Pu-Ga alloys employed in the nuclear weapons and to develop models describing these changes sufficiently reliable to forecast them for several decades. The November 26, 2006 press release by the NNSA summarizes the conclusions of the investigation, '...there appear to be no serious or sudden changes occurring, or expected to occur, in plutonium that would affect performance of pits beyond the well-understood, gradual degradation of plutonium materials'. Furthermore, 'These studies show that the degradation of plutonium in our nuclear weapons will not affect warhead reliability for decades', then NNSA Administrator Linton Brooks said. 'It is now clear that although plutonium aging contributes, other factors control the overall life expectancy of nuclear weapons systems'. The origin of plutonium aging is the natural decay of certain plutonium isotopes. Specifically, it is the process of alpha decay in which a plutonium atom spontaneously splits into a 5 MeV alpha particle and an 85keV uranium recoil

  17. 49 CFR 175.704 - Plutonium shipments.

    Code of Federal Regulations, 2013 CFR

    2013-10-01

    ... 49 Transportation 2 2013-10-01 2013-10-01 false Plutonium shipments. 175.704 Section 175.704... Regulations Applicable According to Classification of Material § 175.704 Plutonium shipments. Shipments of plutonium which are subject to 10 CFR 71.88(a)(4) must comply with the following: (a) Each...

  18. 49 CFR 175.704 - Plutonium shipments.

    Code of Federal Regulations, 2014 CFR

    2014-10-01

    ... 49 Transportation 2 2014-10-01 2014-10-01 false Plutonium shipments. 175.704 Section 175.704... Regulations Applicable According to Classification of Material § 175.704 Plutonium shipments. Shipments of plutonium which are subject to 10 CFR 71.88(a)(4) must comply with the following: (a) Each...

  19. 49 CFR 175.704 - Plutonium shipments.

    Code of Federal Regulations, 2010 CFR

    2010-10-01

    ... 49 Transportation 2 2010-10-01 2010-10-01 false Plutonium shipments. 175.704 Section 175.704... Regulations Applicable According to Classification of Material § 175.704 Plutonium shipments. Shipments of plutonium which are subject to 10 CFR 71.88(a)(4) must comply with the following: (a) Each...

  20. 49 CFR 175.704 - Plutonium shipments.

    Code of Federal Regulations, 2011 CFR

    2011-10-01

    ... 49 Transportation 2 2011-10-01 2011-10-01 false Plutonium shipments. 175.704 Section 175.704... Regulations Applicable According to Classification of Material § 175.704 Plutonium shipments. Shipments of plutonium which are subject to 10 CFR 71.88(a)(4) must comply with the following: (a) Each...

  1. Rapid Radiochemical Method for Plutonium-238 and ...

    EPA Pesticide Factsheets

    Technical Fact Sheet Technique: Alpha spectrometry Method Developed for: Plutonium-238 and plutonium-239 in building materials Method Selected for: SAM lists this method for qualitative analysis of plutonium-238 and -239 in concrete or brick building materials. Summary of subject analytical method which will be posted to the SAM website to allow access to the method.

  2. 49 CFR 175.704 - Plutonium shipments.

    Code of Federal Regulations, 2012 CFR

    2012-10-01

    ... 49 Transportation 2 2012-10-01 2012-10-01 false Plutonium shipments. 175.704 Section 175.704... Regulations Applicable According to Classification of Material § 175.704 Plutonium shipments. Shipments of plutonium which are subject to 10 CFR 71.88(a)(4) must comply with the following: (a) Each...

  3. Plutonium Oxide Process Capability Work Plan

    SciTech Connect

    Meier, David E.; Tingey, Joel M.

    2014-02-28

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

  4. 238Pu: accumulation, tissue distribution, and excretion in Mayak workers after exposure to plutonium aerosols.

    PubMed

    Suslova, Klara G; Sokolova, Alexandra B; Khokhryakov, Viktor V; Miller, Scott C

    2012-03-01

    The alpha spectrometry measurements of specific activity of 238Pu and 239Pu in urine from bioassay examinations of 1,013 workers employed at the radiochemical and plutonium production facilities of the Mayak Production Association and in autopsy specimens of lung, liver, and skeleton from 85 former nuclear workers who died between 1974-2009, are summarized.The accumulation fraction of 238Pu in the body and excreta has not changed with time in workers involved in production of weapons-grade plutonium production (e.g., the plutonium production facility and the former radiochemical facility). The accumulation fraction of 238Pu in individuals exposed to plutonium isotopes at the newer Spent Nuclear Fuel Reprocessing Plant ranged from 0.13% up to 27.5% based on the autopsy data. No statistically significant differences between 238Pu and 239Pu in distribution by the main organs of plutonium deposition were found in the Mayak workers. Based on the bioassay data,the fraction of 238Pu activity in urine is on average 38-69% of the total activity of 238Pu and 239Pu, which correlates with the isotopic composition in workplace air sampled at the Spent Nuclear Fuel Reprocessing Plant. In view of the higher specific activity of 238Pu, the contribution of 238Pu to the total internal dose, particularly in the skeleton and liver, might be expected to continue to increase, and continued surveillance is recommended.

  5. Global plutonium management: A security option

    SciTech Connect

    Sylvester, K.W.B.

    1998-12-31

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

  6. PROCESS FOR SEPARATING PLUTONIUM FROM IMPURITIES

    DOEpatents

    Wahl, A.C.

    1957-11-12

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

  7. PLUTONIUM COMPOUNDS AND PROCESS FOR THEIR PREPARATION

    DOEpatents

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

    1958-01-01

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

  8. Plutonium inventory characterization technical evaluation report

    SciTech Connect

    Wittman, G.R., Westinghouse Hanford

    1996-07-10

    This is a technical report on the data, gathered to date, under WHC- SD-CP-TP-086, Rev. 1, on the integrity of the food pack cans currently being used to store plutonium or plutonium compounds at the Plutonium Finishing Plant. Workplan PFP-96-VO-009, `Inspection of Special Nuclear Material Using X-ray`, was used to gather data on material and containment conditions using real time radiography. Some of those images are included herein. A matrix found in the `Plutonium Inventory Characterization Implementation Plan` was used to categorize different plutonium items based upon the type of material being stored and the life expectancy of the containers.

  9. Method of separating thorium from plutonium

    DOEpatents

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

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

  10. Plutonium immobilization feed batching system concept report

    SciTech Connect

    Erickson, S.

    2000-07-19

    The Plutonium Immobilization Facility will encapsulate plutonium in ceramic pucks and seal the pucks inside welded cans. Remote equipment will place these cans in magazines and the magazines in a Defense Waste Processing Facility (DWPF) canister. The DWPF will fill the canister with high level waste glass for permanent storage. Feed batching is one of the first process steps involved with first stage plutonium immobilization. It will blend plutonium oxide powder before it is combined with other materials to make pucks. This report discusses the Plutonium Immobilization feed batching process preliminary concept, batch splitting concepts, and includes a process block diagram, concept descriptions, a preliminary equipment list, and feed batching development areas.

  11. Method of separating thorium from plutonium

    DOEpatents

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

    1984-07-10

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

  12. Method of separating thorium from plutonium

    DOEpatents

    Clifton, David G.; Blum, Thomas W.

    1984-01-01

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

  13. Plutonium inventories for stabilization and stabilized materials

    SciTech Connect

    Williams, A.K.

    1996-05-01

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

  14. The First Weighing of Plutonium

    DOE R&D Accomplishments Database

    Seaborg, Glenn T.

    1967-09-10

    Recollections and reminiscences at the 25th Anniversary of the First Weighing of Plutonium, Chicago, IL, September 10, 1967, tell an important part of the story of this fascinating new element that is destined to play an increasingly significant role in the future of man.

  15. Plutonium disposition and storage model

    SciTech Connect

    Krupa, J.F.

    2000-03-01

    An EXTEND/SDI-Industry model of DOE plutonium disposition and storage has been created which can easily accommodate changes in scenarios by changing input parameters. It matches well with hand-crafted spreadsheet analyses, and has the advantage that it shows system logic and can be documented easily.

  16. Plutonium disposition and storage model

    SciTech Connect

    Krupa, J.F.

    1999-12-06

    An EXTEND/SDI-Industry model of DOE plutonium disposition and storage has been created which can easily accommodate changes in scenarios by changing input parameters. It matches well with hand-crafted spreadsheet analyses, and has the advantage that it shows system logic and can be documented easily.

  17. Plutonium Recycle: The Fateful Step

    ERIC Educational Resources Information Center

    Speth, J. Gustave; And Others

    1974-01-01

    Calls attention to the fact that if the Atomic Energy Commission proceeds with its plans to authorize the nuclear power industry to use plutonium as a fuel in commercial nuclear reactors around the country, this will result in a dramatic escalation in the risks posed by nuclear power. (PEB)

  18. Plutonium Recycle: The Fateful Step

    ERIC Educational Resources Information Center

    Speth, J. Gustave; And Others

    1974-01-01

    Calls attention to the fact that if the Atomic Energy Commission proceeds with its plans to authorize the nuclear power industry to use plutonium as a fuel in commercial nuclear reactors around the country, this will result in a dramatic escalation in the risks posed by nuclear power. (PEB)

  19. Plutonium waste incineration using pyrohydrolysis

    SciTech Connect

    Meyer, M.L.

    1991-12-31

    Waste generated by Savannah River Site (SRS) plutonium operations includes a contaminated organic waste stream. A conventional method for disposing of the organic waste stream and recovering the nuclear material is by incineration. When the organic material is burned, the plutonium remains in the incinerator ash. Plutonium recovery from incinerator ash is highly dependent on the maximum temperature to which the oxide is exposed. Recovery via acid leaching is reduced for a high fired ash (>800{degree}C), while plutonium oxides fired at lower decomposition temperatures (400--800{degrees}C) are more soluble at any given acid concentration. To determine the feasibility of using a lower temperature process, tests were conducted using an electrically heated, controlled-air incinerator. Nine nonradioactive, solid, waste materials were batch-fed and processed in a top-heated cylindrical furnace. Waste material processing was completed using a 19-liter batch over a nominal 8-hour cycle. A processing cycle consisted of 1 hour for heating, 4 hours for reacting, and 3 hours for chamber cooling. The water gas shift reaction was used to hydrolyze waste materials in an atmosphere of 336% steam and 4.4% oxygen. Throughput ranged from 0.14 to 0.27 kg/hr depending on the variability in the waste material composition and density.

  20. Plutonium waste incineration using pyrohydrolysis

    SciTech Connect

    Meyer, M.L.

    1991-01-01

    Waste generated by Savannah River Site (SRS) plutonium operations includes a contaminated organic waste stream. A conventional method for disposing of the organic waste stream and recovering the nuclear material is by incineration. When the organic material is burned, the plutonium remains in the incinerator ash. Plutonium recovery from incinerator ash is highly dependent on the maximum temperature to which the oxide is exposed. Recovery via acid leaching is reduced for a high fired ash (>800{degree}C), while plutonium oxides fired at lower decomposition temperatures (400--800{degrees}C) are more soluble at any given acid concentration. To determine the feasibility of using a lower temperature process, tests were conducted using an electrically heated, controlled-air incinerator. Nine nonradioactive, solid, waste materials were batch-fed and processed in a top-heated cylindrical furnace. Waste material processing was completed using a 19-liter batch over a nominal 8-hour cycle. A processing cycle consisted of 1 hour for heating, 4 hours for reacting, and 3 hours for chamber cooling. The water gas shift reaction was used to hydrolyze waste materials in an atmosphere of 336% steam and 4.4% oxygen. Throughput ranged from 0.14 to 0.27 kg/hr depending on the variability in the waste material composition and density.

  1. Forensic investigation of plutonium metal: a case study of CRM 126

    SciTech Connect

    Byerly, Benjamin L.; Stanley, Floyd; Spencer, Khal; Colletti, Lisa; Garduno, Katherine; Kuhn, Kevin; Lujan, Elmer; Martinez, Alex; Porterfield, Donivan; Rim, Jung; Schappert, Mike; Thomas, Mariam; Townsend, Lisa; Xu, Ning; Tandon, Lav

    2016-11-01

    In our study, a certified plutonium metal reference material (CRM 126) with a known production history is examined using analytical methods that are commonly employed in nuclear forensics for provenancing and attribution. Moreover, the measured plutonium isotopic composition and actinide assay are consistent with values reported on the reference material certificate. Model ages from U/Pu and Am/Pu chronometers agree with the documented production timeline. Finally, these results confirm the utility of these analytical methods and highlight the importance of a holistic approach for forensic study of unknown materials.

  2. Dissolution of aerosol particles collected from nuclear facility plutonium production process

    DOE PAGES

    Xu, Ning; Martinez, Alexander; Schappert, Michael Francis; ...

    2015-08-14

    Here, a simple, robust analytical chemistry method has been developed to dissolve plutonium containing particles in a complex matrix. The aerosol particles collected on Marple cascade impactor substrates were shown to be dissolved completely with an acid mixture of 12 M HNO3 and 0.1 M HF. A pressurized closed vessel acid digestion technique was utilized to heat the samples at 130 °C for 16 h to facilitate the digestion. The dissolution efficiency for plutonium particles was 99 %. The resulting particle digestate solution was suitable for trace elemental analysis and isotope composition determination, as well as radiochemistry measurements.

  3. Dissolution of aerosol particles collected from nuclear facility plutonium production process

    SciTech Connect

    Xu, Ning; Martinez, Alexander; Schappert, Michael Francis; Montoya, Dennis Patrick; Martinez, Patrick Thomas; Tandon, Lav

    2015-08-14

    Here, a simple, robust analytical chemistry method has been developed to dissolve plutonium containing particles in a complex matrix. The aerosol particles collected on Marple cascade impactor substrates were shown to be dissolved completely with an acid mixture of 12 M HNO3 and 0.1 M HF. A pressurized closed vessel acid digestion technique was utilized to heat the samples at 130 °C for 16 h to facilitate the digestion. The dissolution efficiency for plutonium particles was 99 %. The resulting particle digestate solution was suitable for trace elemental analysis and isotope composition determination, as well as radiochemistry measurements.

  4. Nonproliferation analysis of the reduction of excess separated plutonium and high-enriched uranium

    SciTech Connect

    Persiani, P.J.

    1995-08-01

    The purpose of this preliminary investigation is to explore alternatives and strategies aimed at the gradual reduction of the excess inventories of separated plutonium and high-enriched uranium (HEU) in the civilian nuclear power industry. The study attempts to establish a technical and economic basis to assist in the formation of alternative approaches consistent with nonproliferation and safeguards concerns. The analysis addresses several options in reducing the excess separated plutonium and HEU, and the consequences on nonproliferation and safeguards policy assessments resulting from the interacting synergistic effects between fuel cycle processes and isotopic signatures of nuclear materials.

  5. Analysis of civilian processing programs in reduction of excess separated plutonium and high-enriched uranium

    SciTech Connect

    Persiani, P.J.

    1995-12-31

    The purpose of this preliminary investigation is to explore alternatives and strategies aimed at the gradual reduction of the excess inventories of separated plutonium and high-enriched uranium (HEU) in the civilian nuclear power industry. The study attempts to establish a technical and economic basis to assist in the formation of alternative approaches consistent with nonproliferation and safeguards concerns. The analysis addresses several options in reducing the excess separated plutonium and HEU, and the consequences on nonproliferation and safeguards policy assessments resulting from the interacting synergistic effects between fuel cycle processes and isotopic signatures of nuclear materials.

  6. Low-level determination of plutonium by gamma and L x-ray spectroscopy

    SciTech Connect

    Nitsche, H.; Gatti, R.C.; Lee, S.C.

    1991-04-01

    we have developed an analytical method for detection of {sup 239}Pu in aqueous samples at concentrations as low as 10{sup {minus}10} M. This nuclear counting technique utilizes the uranium L X-rays, which follow the alpha decay of plutonium. Because L X-rays are specific for the element and not for the individual isotopes, the isotopic composition of the plutonium sample must be known. The counting efficiency in the 11--23 keV range is determined from a plutonium standard, and the concentration of the sample is then calculated from the L X-ray count and the isotopic composition. The total L X-ray count is corrected for possible contributions from other radionuclides present as impurities by measuring the low-energy gamma spectrum for each contaminant to establish specific photon/X-ray ratios. The ratios are important when {sup 241}Pu and {sup 242}Pu are measured, because the respective decay chain members produce non-U L X-rays. This new method can replace the use of labor-intensive radiochemical separation techniques and elaborate activation methods for analysis of {sup 239}Pu in aqueous samples. It is also applicable for assaying plutonium in liquid wastes that pose possible hazards to the environment.

  7. HIGH ENERGY DELAYED GAMMA SPECTROSCOPY FOR PLUTONIUM ASSAY OF SPENT REACTOR FUEL

    SciTech Connect

    Campbell, Luke W.; Smith, L. E.; Misner, Alex C.

    2011-07-18

    Nuclear safeguards requires accountancy of plutonium present in spent reactor fuels. Current non-destructive methods do not directly measure plutonium content but instead rely on indirect measurements that require operator declarations of the fuel history. Delayed gamma spectroscopy is one method being investigated which can overcome these limitations. Delayed gamma rays from fission depend on the isotopic fission yield of the fissile isotope, and thus can be used to fingerprint the isotopes undergoing fission. However, difficulties arise because of the intense background due to long lived fission radionuclides already present in the fuel. We report on progress on simulated measurements of the delayed gamma spectrum in the presence of this background, using neutrons from a D-T source thermalized in an interrogation chamber slipped over a fuel assembly. By focusing on delayed gammas in the 3 to 4 MeV range, the passive spectrum becomes negligible, while allowing the preferential attenuation of the passive background to acceptable levels.

  8. Neutron Resonance Transmission Analysis (NRTA): Initial Studies of a Method for Assaying Plutonium in Spent Fuel

    SciTech Connect

    David L. Chichester; James W. Sterbentz

    2011-05-01

    Neutron Resonance Transmission Analysis (NRTA) is an analytical technique that uses neutrons to assay the isotopic content of bulk materials. The technique uses a pulsed accelerator to produce an intense, short pulse of neutrons in a time-of-flight configuration. These neutrons, traveling at different speeds according to their energy, can be used to interrogate a spent fuel (SF) assembly to determine its plutonium content. Neutron transmission through the assembly is monitored as a function of neutron energy (time after the pulse), similar to the way neutron cross-section data is often collected. The transmitted neutron intensity is recorded as a function of time, with faster (higher-energy) neutrons arriving first and slower (lower-energy) neutrons arriving later. The low-energy elastic scattering and absorption resonances of plutonium and other isotopes modulate the transmitted neutron spectrum. Plutonium content in SF can be determined by analyzing this attenuation. Work is currently underway at Idaho National Laboratory, as a part of United States Department of Energy's Next Generation Safeguards Initiative (NGSI), to investigate the NRTA technique and to assess its feasibility for quantifying the plutonium content in SF and for determining the diversion of SF pins from assemblies. Preliminary results indicate that NRTA has great potential for being able to assay intact SF assemblies. Operating in the 1-40 eV range, it can identify four plutonium isotopes (239, 240, 241, & 242Pu), three uranium isotopes (235, 236, & 238U), and six resonant fission products (99Tc, 103Rh, 131Xe, 133Cs, 145Nd, and 152Sm). It can determine the areal density or mass of these isotopes in single- or multiple-pin integral transmission scans. Further, multiple observables exist to allow the detection of material diversion (pin defects) including fast-neutron and x-ray radiography, gross-transmission neutron counting, plutonium resonance absorption analysis, and fission-product resonance

  9. FRAM's Isotopic Uncertainty Analysis.

    SciTech Connect

    Vo, Duc T.

    2005-01-01

    The Fixed-Energy Response-Function Analysis with Multiple Efficiency (FRAM) code was developed at Los Alamos National Laboratory to measure the gamma-ray spectrometry of the isotopic composition of plutonium, uranium, and other actinides. They have studied and identified two different kinds of errors from FRAM analysis: random and systematic. The random errors come mainly from statistics and are easily determined. The systematic errors can come from a variety of sources and can be very difficult to determine. The authors carefully examined the FRAM analytical results of the archival plutonium data and of the data specifically acquired for this isotopic uncertainty analysis project, and found the relationship between the systematic errors and other parameters. They determined that the FRAM's systematic errors could be expressed as functions of the peak resolution and shape, region of analysis, and burnup (for plutonium) or enrichment (for uranium). All other parameters such as weight, matrix material, shape, size, container, electronics, detector, input rate, etc., contribute little to the systematic error or they contribute to the peak resolution and shape and then their contributions can be determined from the peak resolution and shape.

  10. Analysis of the effects of inter-individual variation in the distribution of plutonium in skeleton and liver.

    PubMed

    Klein, W; Breustedt, B

    2014-01-01

    One important parameter for biokinetic plutonium modelling is the ratio between the contents of plutonium in liver and skeleton. Autopsy data show a vast inter-individual variation in the partitioning between these organs. The capacity of recent biokinetic models for plutonium to reproduce these variations was studied. Autopsy data for plutonium amounts in liver and skeleton for both (238)Pu and (239)Pu isotopes can be merged into a single data set following several statistical tests. Simulations with different parameter values generate a mapping between the autopsy values and the model parameters. The observed partitioning distribution can be transformed into a distribution of transfer rates, which would result in the observed data. Besides, the variation in the partitioning between liver and skeleton leads via biliary pathway to a variation in the excretion ratio. This can be used to estimate an individual partitioning factor, which can be used in individual case assessments.

  11. Separation of plutonium from uranium using reactive chemistry in a bandpass reaction cell of an inductively coupled plasma mass spectrometer.

    PubMed

    Vais, Vladimir; Li, Chunsheng; Cornett, Jack

    2004-09-01

    Oxygen and ammonia were evaluated as reaction gases for the chemical separation between uranium and plutonium in the bandpass reaction cell or dynamic reaction cell (DRC) of the ELAN DRC II mass spectrometer. Both uranium and plutonium demonstrated similar reactivity with oxygen giving rise to corresponding oxides. At the same time, remarkable selectivity in the reaction with ammonia was observed. While uranium was rapidly converted into UNH 2+ and UN2H 4+, plutonium remained unreactive in the DRC pressurized with ammonia. This difference in the reactivity allowed the determination of plutonium isotopes in urine and water samples containing excess uranium without preceding separation procedure. Detection limits of 0.245, 0.092, 0.270 and 0.237 ng L(-1) were obtained for 238Pu, 239Pu, 240Pu and 242Pu, respectively, in urine spiked with 10 microg L(-1) of U.

  12. Decay Heat Calculations for PWR and BWR Assemblies Fueled with Uranium and Plutonium Mixed Oxide Fuel using SCALE

    SciTech Connect

    Ade, Brian J; Gauld, Ian C

    2011-10-01

    In currently operating commercial nuclear power plants (NPP), there are two main types of nuclear fuel, low enriched uranium (LEU) fuel, and mixed-oxide uranium-plutonium (MOX) fuel. The LEU fuel is made of pure uranium dioxide (UO{sub 2} or UOX) and has been the fuel of choice in commercial light water reactors (LWRs) for a number of years. Naturally occurring uranium contains a mixture of different uranium isotopes, primarily, {sup 235}U and {sup 238}U. {sup 235}U is a fissile isotope, and will readily undergo a fission reaction upon interaction with a thermal neutron. {sup 235}U has an isotopic concentration of 0.71% in naturally occurring uranium. For most reactors to maintain a fission chain reaction, the natural isotopic concentration of {sup 235}U must be increased (enriched) to a level greater than 0.71%. Modern nuclear reactor fuel assemblies contain a number of fuel pins potentially having different {sup 235}U enrichments varying from {approx}2.0% to {approx}5% enriched in {sup 235}U. Currently in the United States (US), all commercial nuclear power plants use UO{sub 2} fuel. In the rest of the world, UO{sub 2} fuel is still commonly used, but MOX fuel is also used in a number of reactors. MOX fuel contains a mixture of both UO{sub 2} and PuO{sub 2}. Because the plutonium provides the fissile content of the fuel, the uranium used in MOX is either natural or depleted uranium. PuO{sub 2} is added to effectively replace the fissile content of {sup 235}U so that the level of fissile content is sufficiently high to maintain the chain reaction in an LWR. Both reactor-grade and weapons-grade plutonium contains a number of fissile and non-fissile plutonium isotopes, with the fraction of fissile and non-fissile plutonium isotopes being dependent on the source of the plutonium. While only RG plutonium is currently used in MOX, there is the possibility that WG plutonium from dismantled weapons will be used to make MOX for use in US reactors. Reactor-grade plutonium

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

    PubMed

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

    2017-04-01

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

  14. PRECIPITATION METHOD FOR THE SEPARATION OF PLUTONIUM AND RARE EARTHS

    DOEpatents

    Thompson, S.G.

    1960-04-26

    A method of purifying plutonium is given. Tetravalent plutonium is precipitated with thorium pyrophosphate, the plutonium is oxidized to the tetravalent state, and then impurities are precipitated with thorium pyrophosphate.

  15. Surprising coordination for plutonium in the first plutonium(III) borate.

    PubMed

    Wang, Shuao; Alekseev, Evgeny V; Depmeier, Wulf; Albrecht-Schmitt, Thomas E

    2011-03-21

    The first plutonium(III) borate, Pu(2)[B(12)O(18)(OH)(4)Br(2)(H(2)O)(3)]·0.5H(2)O, has been prepared by reacting plutonium(III) with molten boric acid under strictly anaerobic conditions. This compound contains a three-dimensional polyborate network with triangular holes that house the plutonium(III) sites. The plutonium sites in this compound are 9- and 10-coordinate and display atypical geometries.

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

    SciTech Connect

    Caviness, Michael L; Mann, Paul T

    2010-01-01

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

  17. SEPARATION OF PLUTONIUM HYDROXIDE FROM BISMUTH HYDROXIDE

    DOEpatents

    Watt, G.W.

    1958-08-19

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

  18. Multi-generational stewardship of plutonium

    SciTech Connect

    Pillay, K.K.S.

    1997-10-01

    The post-cold war era has greatly enhanced the interest in the long-term stewardship of plutonium. The management of excess plutonium from proposed nuclear weapons dismantlement has been the subject of numerous intellectual discussions during the past several years. In this context, issues relevant to long-term management of all plutonium as a valuable energy resource are also being examined. While there are differing views about the future role of plutonium in the economy, there is a recognition of the environmental and health related problems and proliferation potentials of weapons-grade plutonium. The long-term management of plutonium as an energy resource will require a new strategy to maintain stewardship for many generations to come.

  19. Biokinetics of Plutonium in Nonhuman Primates.

    PubMed

    Poudel, Deepesh; Guilmette, Raymond A; Gesell, Thomas F; Harris, Jason T; Brey, Richard R

    2016-10-01

    A major source of data on metabolism, excretion and retention of plutonium comes from experimental animal studies. Although old world monkeys are one of the closest living relatives to humans, certain physiological differences do exist between these nonhuman primates and humans. The objective of this paper was to describe the metabolism of plutonium in nonhuman primates using the bioassay and retention data obtained from macaque monkeys injected with plutonium citrate. A biokinetic model for nonhuman primates was developed by adapting the basic model structure and adapting the transfer rates described for metabolism of plutonium in adult humans. Significant changes to the parameters were necessary to explain the shorter retention of plutonium in liver and skeleton of the nonhuman primates, differences in liver to bone partitioning ratio, and significantly higher excretion of plutonium in feces compared to that in humans.

  20. PROCESS FOR THE RECOVERY OF PLUTONIUM

    DOEpatents

    Potratz, H.A.

    1958-12-16

    A process for the separation of plutonium from uranlum and other associated radioactlve fission products ls descrlbed conslstlng of contacting an acid solution containing plutonium in the tetravalent state and uranium in the hexavalent state with enough ammonium carbonate to form an alkaline solution, adding cupferron to selectlvely form plutonlum cupferrlde, then recoverlng the plutonium cupferride by extraction with a water lmmiscible organic solvent such as chloroform.

  1. PROCESS OF SEPARATING PLUTONIUM VALUES BY ELECTRODEPOSITION

    DOEpatents

    Whal, A.C.

    1958-04-15

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

  2. WET METHOD OF PREPARING PLUTONIUM TRIBROMIDE

    DOEpatents

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

    1958-11-11

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

  3. PLUTONIUM METAL: OXIDATION CONSIDERATIONS AND APPROACH

    SciTech Connect

    Estochen, E.

    2013-03-20

    Plutonium is arguably the most unique of all metals when considered in the combined context of metallurgical, chemical, and nuclear behavior. Much of the research in understanding behavior and characteristics of plutonium materials has its genesis in work associated with nuclear weapons systems. However, with the advent of applications in fuel materials, the focus in plutonium science has been more towards nuclear fuel applications, as well as long term storage and disposition. The focus of discussion included herein is related to preparing plutonium materials to meet goals consistent with non-proliferation. More specifically, the emphasis is on the treatment of legacy plutonium, in primarily metallic form, and safe handling, packaging, and transport to meet non-proliferation goals of safe/secure storage. Elevated temperature oxidation of plutonium metal is the treatment of choice, due to extensive experiential data related to the method, as the oxide form of plutonium is one of only a few compounds that is relatively simple to produce, and stable over a large temperature range. Despite the simplicity of the steps required to oxidize plutonium metal, it is important to understand the behavior of plutonium to ensure that oxidation is conducted in a safe and effective manner. It is important to understand the effect of changes in environmental variables on the oxidation characteristics of plutonium. The primary purpose of this report is to present a brief summary of information related to plutonium metal attributes, behavior, methods for conversion to oxide, and the ancillary considerations related to processing and facility safety. The information provided is based on data available in the public domain and from experience in oxidation of such materials at various facilities in the United States. The report is provided as a general reference for implementation of a simple and safe plutonium metal oxidation technique.

  4. PLUTONIUM-CUPFERRON COMPLEX AND METHOD OF REMOVING PLUTONIUM FROM SOLUTION

    DOEpatents

    Potratz, H.A.

    1959-01-13

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

  5. Disposition options for separated plutonium

    SciTech Connect

    Hippel, F. von; Feiveson, H. )

    1993-01-01

    Russia and the United States expect to dismantle [approximately]50,000 nuclear warheads containing [approximately]150 tonnes of plutonium as a result of the drastic reductions in tactical nuclear weapons announced by Presidents Bush and Gorbachev during the fall of 1991 and the reductions in strategic weapons agreed to in the START I and START II Treaties. In addition, if current plans for reprocessing spent light water reactor (LWR) fuel are carried out (mainly in Britain and France) [approximately]200 tonnes of civilian plutonium will be separated during the 1990s. This paper addresses the public-policy issues in the U.S. and abroad regarding disposition options as well as some technical aspects for options.

  6. Plutonium Immobilization Can Loading Concepts

    SciTech Connect

    Kriikku, E.; Ward, C.; Stokes, M.; Randall, B.; Steed, J.; Jones, R.; Hamilton, L.; Rogers, L.; Fiscus, J.; Dyches, G.

    1998-05-01

    The Plutonium Immobilization Facility will encapsulate plutonium in ceramic pucks and seal the pucks inside welded cans. Remote equipment will place these cans in magazines and the magazines in a Defense Waste Processing Facility (DWPF) canister. The DWPF will fill the canister with glass for permanent storage. This report discusses five can loading conceptual designs and the lists the advantages and disadvantages for each concept. This report identifies loading pucks into cans and backfilling cans with helium as the top priority can loading development areas. The can loading welder and cutter are very similar to the existing Savannah River Site (SRS) FB-Line bagless transfer welder and cutter and thus they are a low priority development item.

  7. Plutonium Immobilization Project Baseline Formulation

    SciTech Connect

    Ebbinghaus, B.

    1999-02-01

    A key milestone for the Immobilization Project (AOP Milestone 3.2a) in Fiscal Year 1998 (FY98) is the definition of the baseline composition or formulation for the plutonium ceramic form. The baseline formulation for the plutonium ceramic product must be finalized before the repository- and plant-related process specifications can be determined. The baseline formulation that is currently specified is given in Table 1.1. In addition to the baseline formulation specification, this report provides specifications for two alternative formulations, related compositional specifications (e.g., precursor compositions and mixing recipes), and other preliminary form and process specifications that are linked to the baseline formulation. The preliminary specifications, when finalized, are not expected to vary tremendously from the preliminary values given.

  8. Neutron radiation characteristics of plutonium dioxide fuel

    NASA Technical Reports Server (NTRS)

    Taherzadeh, M.

    1972-01-01

    The major sources of neutrons from plutonium dioxide nuclear fuel are considered in detail. These sources include spontaneous fission of several of the Pu isotopes, (alpha, n) reactions with low Z impurities in the fuel, and (alpha, n) reactions with O-18. For spontaneous fission neutrons a value of (1.95 + or - 0.07) X 1,000 n/s/g PuO2 is obtained. The neutron yield from (alpha, n) reactions with oxygen is calculated by integrating the reaction rate equation over all alpha-particle energies and all center-of-mass angles. The results indicate a neutron emission rate of (1.14 + or - 0.26) X 10,000 n/s/g PuO2. The neutron yield from (alpha, n) reactions with low Z impurities in the fuel is presented in tabular form for one part part per million of each impurity. The total neutron yield due to the combined effects of all the impurities depends upon the fractional weight concentration of each impurity. The total neutron flux emitted from a particular fuel geometry is estimated by adding the neutron yield due to the induced fission to the other neutron sources.

  9. Neutron Radiation Characteristics of Plutonium Dioxide Fuel

    NASA Technical Reports Server (NTRS)

    Taherzadeh, M.

    1972-01-01

    The major sources of neutrons from plutonium dioxide nuclear fuel are considered in detail. These sources include spontaneous fission of several of the Pu isotopes, reactions with low Z impurities in the fuel, and reactions with O-18. For spontaneous fission neutrons a value of (1.95 plus or minus 0.07) X 1,000 n/s/q PuO2 is obtained. The neutron yield from (alpha, neutron) reactions with oxygen is calculated by integrating the reaction rate equation over all alpha particle energies and all center-of-mass angles. The results indicate a neutron emission rate of (1.42 plus or minus 0.32) X 10,000 n/s/q PuO2. The neutron yield from (alpha, neutron) reactions with low Z impurities in the fuel is presented in tabular form for one part per million of each impurity. The total neutron flux emitted from a particular fuel geometry is estimated by adding the neutron yield due to the induced fission to the other neutron sources.

  10. Simultaneous determination of radiocesium ((135)Cs, (137)Cs) and plutonium ((239)Pu, (240)Pu) isotopes in river suspended particles by ICP-MS/MS and SF-ICP-MS.

    PubMed

    Cao, Liguo; Zheng, Jian; Tsukada, Hirofumi; Pan, Shaoming; Wang, Zhongtang; Tagami, Keiko; Uchida, Shigeo

    2016-10-01

    Due to radioisotope releases in the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, long-term monitoring of radiocesium ((135)Cs and (137)Cs) and Pu isotopes ((239)Pu and (240)Pu) in river suspended particles is necessary to study the transport and fate of these long-lived radioisotopes in the land-ocean system. However, it is expensive and technically difficult to collect samples of suspended particles from river and ocean. Thus, simultaneous determination of multi-radionuclides remains as a challenging topic. In this study, for the first time, we report an analytical method for simultaneous determination of radiocesium and Pu isotopes in suspended particles with small sample size (1-2g). Radiocesium and Pu were sequentially pre-concentrated using ammonium molybdophosphate and ferric hydroxide co-precipitation, respectively. After the two-stage ion-exchange chromatography separation from the matrix elements, radiocesium and Pu isotopes were finally determined by ICP-MS/MS and SF-ICP-MS, respectively. The interfering elements of U ((238)U(1)H(+) and (238)U(2)H(+) for (239)Pu and (240)Pu, respectively) and Ba ((135)Ba(+) and (137)Ba(+) for (135)Cs and (137)Cs, respectively) were sufficiently removed with the decontamination factors of 1-8×10(6) and 1×10(4), respectively, with the developed method. Soil reference materials were utilized for method validation, and the obtained (135)Cs/(137)Cs and (240)Pu/(239)Pu atom ratios, and (239+240)Pu activities showed a good agreement with the certified/information values. In addition, the developed method was applied to analyze radiocesium and Pu in the suspended particles of land water samples collected from Fukushima Prefecture after the FDNPP accident. The (135)Cs/(137)Cs atom ratios (0.329-0.391) and (137)Cs activities (23.4-152Bq/g) suggested radiocesium contamination of the suspended particles mainly originated from the accident-released radioactive contaminates, while similar Pu contamination of suspended

  11. Plutonium transmutation in thorium fuel cycle

    SciTech Connect

    Necas, Vladimir; Breza, Juraj |; Darilek, Petr

    2007-07-01

    The HELIOS spectral code was used to study the application of the thorium fuel cycle with plutonium as a supporting fissile material in a once-through scenario of the light water reactors PWR and VVER-440 (Russian design). Our analysis was focused on the plutonium transmutation potential and the plutonium radiotoxicity course of hypothetical thorium-based cycles for current nuclear power reactors. The paper shows a possibility to transmute about 50% of plutonium in analysed reactors. Positive influence on radiotoxicity after 300 years and later was pointed out. (authors)

  12. NON-AQUEOUS DISSOLUTION OF MASSIVE PLUTONIUM

    DOEpatents

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

    1959-05-12

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

  13. METHOD OF REDUCING PLUTONIUM WITH FERROUS IONS

    DOEpatents

    Dreher, J.L.; Koshland, D.E.; Thompson, S.G.; Willard, J.E.

    1959-10-01

    A process is presented for separating hexavalent plutonium from fission product values. To a nitric acid solution containing the values, ferrous ions are added and the solution is heated and held at elevated temperature to convert the plutonium to the tetravalent state via the trivalent state and the plutonium is then selectively precipitated on a BiPO/sub 4/ or LaF/sub 3/ carrier. The tetravalent plutonium formed is optionally complexed with fluoride, oxalate, or phosphate anion prior to carrier precipitation.

  14. OXIDATIVE METHOD OF SEPARATING PLUTONIUM FROM NEPTUNIUM

    DOEpatents

    Beaufait, L.J. Jr.

    1958-06-10

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

  15. ION EXCHANGE ADSORPTION PROCESS FOR PLUTONIUM SEPARATION

    DOEpatents

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

    1961-07-11

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

  16. Plutonium-catalyzed oxidative DNA damage in the absence of significant alpha-particle decay

    SciTech Connect

    Claycamp, H.G.; Luo, D.

    1994-01-01

    Plutonium is considered to be a carcinogen because it emits {alpha} particles that may result in the irradiation of stem cell population. In the present study we show that plutonium can also catalyze reactions that induce hydroxyl radicals in the absence of significant {alpha}-particle irradiation. Using the low specific activity isotope, {sup 242}Pu, experiments were performed under conditions in which chemical generation of hydroxyl radicals was expected to exceed the radiolytic generation by 10{sup 5}-fold. The results showed that markers of oxidative DNA base damage, thymine glycol and 8-oxoguanine could be induced from plutonium-catalyzed reactions of hydrogen peroxide and ascorbate similarly to those occurring in the presence of iron catalysts. Plutonium-242, as a neutralized nitrate in phosphate buffer, was 4.8-fold more efficient than iron at catalyzing the oxidation of ascorbate at pH 7. The results suggest that plutonium complexes could participate in reactions at pH 7 that induce oxidative stress - a significant tumor-promoting factor in generally accepted models of carcinogenesis. 16 refs., 3 figs.

  17. Pyrochemical process for extracting plutonium from an electrolyte salt

    DOEpatents

    Mullins, Lawrence J.; Christensen, Dana C.

    1984-01-01

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

  18. Pyrochemical process for extracting plutonium from an electrolyte salt

    DOEpatents

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

    1982-09-20

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

  19. Discovery of isotopes of the transuranium elements with 93≤Z≤98

    SciTech Connect

    Fry, C.; Thoennessen, M.

    2013-01-15

    One hundred and five isotopes of the transuranium elements neptunium, plutonium, americium, curium, berkelium, and californium have been observed so far; the discovery of these isotopes is described. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  20. Discovery of isotopes of the transuranium elements with 93≤Z≤98

    NASA Astrophysics Data System (ADS)

    Fry, C.; Thoennessen, M.

    2013-01-01

    One hundred and five isotopes of the transuranium elements neptunium, plutonium, americium, curium, berkelium, and californium have been observed so far; the discovery of these isotopes is described. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  1. Isotope separation by laser means

    DOEpatents

    Robinson, C. Paul; Jensen, Reed J.; Cotter, Theodore P.; Greiner, Norman R.; Boyer, Keith

    1982-06-15

    A process for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium and plutonium.

  2. Plutonium oxalate precipitation for trace elemental determination in plutonium materials

    SciTech Connect

    Xu, Ning; Gallimore, David; Lujan, Elmer; Garduno, Katherine; Walker, Laurie; Taylor, Fiona; Thompson, Pam; Tandon, Lav

    2015-05-26

    In this study, an analytical chemistry method has been developed that removes the plutonium (Pu) matrix from the dissolved Pu metal or oxide solution prior to the determination of trace impurities that are present in the metal or oxide. In this study, a Pu oxalate approach was employed to separate Pu from trace impurities. After Pu(III) was precipitated with oxalic acid and separated by centrifugation, trace elemental constituents in the supernatant were analyzed by inductively coupled plasma-optical emission spectroscopy with minimized spectral interferences from the sample matrix.

  3. Plutonium oxalate precipitation for trace elemental determination in plutonium materials

    DOE PAGES

    Xu, Ning; Gallimore, David; Lujan, Elmer; ...

    2015-05-26

    In this study, an analytical chemistry method has been developed that removes the plutonium (Pu) matrix from the dissolved Pu metal or oxide solution prior to the determination of trace impurities that are present in the metal or oxide. In this study, a Pu oxalate approach was employed to separate Pu from trace impurities. After Pu(III) was precipitated with oxalic acid and separated by centrifugation, trace elemental constituents in the supernatant were analyzed by inductively coupled plasma-optical emission spectroscopy with minimized spectral interferences from the sample matrix.

  4. Chemical and Radiochemical Composition of Thermally Stabilized Plutonium Oxide from the Plutonium Finishing Plant Considered as Alternate Feedstock for the Mixed Oxide Fuel Fabrication Facility

    SciTech Connect

    Tingey, Joel M.; Jones, Susan A.

    2005-07-01

    PFP. Samples varied in appearance depending on the original source of material. Rocky Flats items were mostly dark olive green with clumps that crushed easily with a mortar and pestle. PRF/RMC items showed more variability. These items were mostly rust colored. One sample contained white particles that were difficult to crush, and another sample was a dark grey with a mixture of fines and large, hard fragments. The appearance and feel of the fragments indicated they might be an alloy. The color of the solution samples was indicative of the impurities in the sample. The double-pass filtrate solution was a brown color indicative of the iron impurities in the sample. The other solution sample was light gray in color. Radiochemical analyses, including thermal ionization mass spectrometry (TIMS), alpha and gamma energy analysis (AEA and GEA), and kinetic phosphorescence analysis (KPA), indicate that these materials are all weapons-grade plutonium with consistent plutonium isotopics. A small amount of uranium (<0.14 wt%) is also present in these samples. The isotopic composition of the uranium varied widely but was consistent among each category of material. The primary water-soluble anions in these samples were Cl-, NO3-, SO42-, and PO43-. The only major anion observed in the Rocky Flats materials was Cl-, but the PRF/RMC samples had significant quantities of all of the primary anions observed. Prompt gamma measurements provide a representative analysis of the Cl- concentration in the bulk material. The primary anions observed in the solution samples were NO3-, and PO43-. The concentration of these anions did not exceed the mixed oxide (MOX) specification limits. Cations that exceeded the MOX specification limits included Cr, Fe, Ni, Al, Cu, and Si. All of the samples exceeded at least the 75% specification limit in one element.

  5. RECOVERY OF PLUTONIUM BY CARRIER PRECIPITATION

    DOEpatents

    Goeckermann, R.H.

    1961-04-01

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

  6. URANOUS IODATE AS A CARRIER FOR PLUTONIUM

    DOEpatents

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

    1959-12-15

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

  7. Surplus Plutonium Disposition Final Environmental Impact Statement

    SciTech Connect

    N /A

    1999-11-19

    In December 1996, the U.S. Department of Energy (DOE) published the ''Storage and Disposition of Weapons-Usable Fissile Materials Final Programmatic Environmental Impact Statement (Storage and Disposition PEIS)'' (DOE 1996a). That PEIS analyzes the potential environmental consequences of alternative strategies for the long-term storage of weapons-usable plutonium and highly enriched uranium (HEU) and the disposition of weapons-usable plutonium that has been or may be declared surplus to national security needs. The Record of Decision (ROD) for the ''Storage and Disposition PEIS'', issued on January 14, 1997 (DOE 1997a), outlines DOE's decision to pursue an approach to plutonium disposition that would make surplus weapons-usable plutonium inaccessible and unattractive for weapons use. DOE's disposition strategy, consistent with the Preferred Alternative analyzed in the ''Storage and Disposition PEIS'', allows for both the immobilization of some (and potentially all) of the surplus plutonium and use of some of the surplus plutonium as mixed oxide (MOX) fuel in existing domestic, commercial reactors. The disposition of surplus plutonium would also involve disposal of both the immobilized plutonium and the MOX fuel (as spent nuclear fuel) in a potential geologic repository.

  8. MOLTEN PLUTONIUM FUELED FAST BREEDER REACTOR

    DOEpatents

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

    1962-06-26

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

  9. Uses for plutonium: Weapons, reactors, and other

    SciTech Connect

    Condit, R.H.

    1994-05-01

    This document begins with a introduction on criticality and supercriticality. Then, types and components, design and engineering, yields, and disassembly of nuclear weapons are discussed. Plutonium is evaluated as a reactor fuel, including neutronics and chemistry considerations. Finally, other uses of plutonium are analyzed.

  10. Source Book on Plutonium and Its Decontamination

    DTIC Science & Technology

    1973-09-24

    Data Entered) UNCLASIFIED 20. ABSTRACT (Continued) |development of the coupled differential equations, based on the 1965 and the proposed 1973...61 XV Some Foreign Plutonium Decontamination Standards . . ...... 63 XVI Variability of Sol Sampling Data .... ..... .... 64 XVII Criteria for...Scheduling Feces Samples . . .......... 66 XVIII Types of Data which may be Coliected for Plutonium Inhalation Incidents . 66 XIX Percent Efficiencies for

  11. Nondestructive assay methods for solids containing plutonium

    SciTech Connect

    Macmurdo, K.W.; Gray, L.W.; Gibbs, A.

    1984-06-01

    Specific nondestructive assay (NDA) methods, e.g. calorimetry, coincidence neutron counting, singles neutron counting, and gamma ray spectrometry, were studied to provide the Savannah River Plant with an NDA method to measure the plutonium content of solid scrap (slag and crucible) generated in the JB-Line plutonium metal production process. Results indicate that calorimetry can be used to measure the plutonium content to within about 3% in 4 to 6 hours by using computerized equilibrium sample power predictive models. Calorimetry results confirm that a bias exists in the present indirect measurement method used to estimate the plutonium content of slag and crucible. Singles neutron counting of slag and crucible can measure plutonium to only +-30%, but coincidence neutron counting methods improve measurement precision to better than +-10% in less than ten minutes. Only four portions of a single slag and crucible sample were assayed, and further study is recommended.

  12. Application of PGNAA to plutonium surveillance

    SciTech Connect

    Prettyman, T.H.; Foster, L.A.; Staples, P.

    1997-12-01

    Prompt gamma-ray neutron activation analysis (PGNAA) is a well-established tool for nondestructive elemental analysis of bulk samples. At Los Alamos National Laboratory we are investigating the use of PGNAA as a diagnostic tool for a number of applications, particularly matrix characterization for nondestructive assay and plutonium surveillance. Surveillance is an essential feature of most plutonium facility operations, including routine material processing and research, short-term storage, and processing operations prior to disposal or long-term storage. The ability to identify and assay specific elements from gamma-ray-produced active neutron interrogation (e.g., by neutron capture, nonelastic scattering, and the decay of activation products) makes PGNAA an ideal tool for surveillance. For example, PGNAA can help confirm item descriptions (for example, plutonium chloride versus plutonium oxide). This feature is particularly important in operations involving poorly characterized legacy materials where the material form could adversely impact plutonium-processing operations.

  13. PROCESS FOR THE RECOVERY OF PLUTONIUM

    DOEpatents

    Ritter, D.M.

    1959-01-13

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

  14. REMOVAL OF LEGACY PLUTONIUM MATERIALS FROM SWEDEN

    SciTech Connect

    Dunn, Kerry A.; Bellamy, J. Steve; Chandler, Greg T.; Iyer, Natraj C.; Koenig, Rich E.; Leduc, D.; Hackney, B.; Leduc, Dan R.; McClard, J. W.

    2013-08-18

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

  15. ADSORPTION-BISMUTH PHOSPHATE METHOD FOR SEPARATING PLUTONIUM

    DOEpatents

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

    1960-06-28

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

  16. Plutonium Uptake and Distribution in Mammalian Cells: Molecular vs Polymeric Plutonium

    PubMed Central

    ARYAL, BAIKUNTHA P.; GORMAN-LEWIS, DREW; PAUNESKU, TATJANA; WILSON, RICHARD E.; LAI, BARRY; VOGT, STEFAN; WOLOSCHAK, GAYLE E.; JENSEN, MARK P.

    2013-01-01

    Purpose To study the cellular responses to molecular and polymeric forms of plutonium using PC12 cells derived from rat adrenal glands. Materials and methods Serum starved PC12 cells were exposed to polymeric and molecular forms of plutonium for three hours. Cells were washed with 10 mM EGTA, 100 mM NaCl at pH 7.4 to remove surface sorbed plutonium. Localization of plutonium in individual cell was quantitatively analyzed by synchrotron X-ray fluorescence (XRF) microscopy. Results Molecular plutonium complexes introduced to cell growth media in the form of NTA, citrate, or transferrin complexes were taken up by PC12 cells, and mostly co-localized with iron within the cells. Polymeric plutonium prepared separately was not internalized by PC12 cells but it was always found on the cell surface as big agglomerates; however polymeric plutonium formed in situ was mostly found within the cells as agglomerates. Conclusions PC12 cells can differentiate molecular and polymeric forms of plutonium. Molecular plutonium is taken up by PC12 cells and mostly co-localized with iron but aged polymeric plutonium is not internalized by the cells. PMID:21770702

  17. Plutonium uptake and distribution in mammalian cells: molecular vs. polymeric plutonium.

    PubMed

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

    2011-10-01

    To study the cellular responses to molecular and polymeric forms of plutonium using PC12 cells derived from a rat pheochromocytoma. Serum starved PC12 cells were exposed to polymeric and molecular forms of plutonium for 3 h. Cells were washed with 10 mM ethylene glycol tetraacetic acid (EGTA), 100 mM NaCl at pH 7.4 to remove surface sorbed plutonium. Localization of plutonium in individual cell was quantitatively analyzed by synchrotron X-ray fluorescence (XRF) microscopy. Molecular plutonium complexes introduced to cell growth media in the form of nitrilotriacetic acid (NTA), citrate, or transferrin complexes were taken up by PC12 cells, and mostly colocalized with iron within the cells. Aged polymeric plutonium prepared separately was not internalized by PC12 cells but it was always found on the cell surface as big agglomerates; however, polymeric plutonium formed in situ was mostly found within the cells as agglomerates. PC12 cells can differentiate molecular and polymeric forms of plutonium. Molecular plutonium is taken up by PC12 cells and mostly co-localizes with iron but aged polymeric plutonium is not internalized by the cells.

  18. Potentiometric determination of plutonium by sodium bismuthate oxidation.

    PubMed

    Charyulu, M M; Rao, V K; Natarajan, P R

    1984-12-01

    A potentiometric method for the determination of plutonium is described, in which the plutonium is quantitatively oxidized to plutonium(VI) with sodium bismuthate in nitric acid medium, the excess of oxidant is destroyed chemically and plutonium(VI) is reduced to plutonium(IV) with a measured excess of iron(II), the surplus of which is back-titrated with dichromate. For 3-5 mg of plutonium the error is less than 0.2%. For submilligram quantities of plutonium in presence of macro-amounts of uranium the error is below 2.0%.

  19. Laboratory-scale evaluations of alternative plutonium precipitation methods

    SciTech Connect

    Martella, L.L.; Saba, M.T.; Campbell, G.K.

    1984-02-08

    Plutonium(III), (IV), and (VI) carbonate; plutonium(III) fluoride; plutonium(III) and (IV) oxalate; and plutonium(IV) and (VI) hydroxide precipitation methods were evaluated for conversion of plutonium nitrate anion-exchange eluate to a solid, and compared with the current plutonium peroxide precipitation method used at Rocky Flats. Plutonium(III) and (IV) oxalate, plutonium(III) fluoride, and plutonium(IV) hydroxide precipitations were the most effective of the alternative conversion methods tested because of the larger particle-size formation, faster filtration rates, and the low plutonium loss to the filtrate. These were found to be as efficient as, and in some cases more efficient than, the peroxide method. 18 references, 14 figures, 3 tables.

  20. Ceramification: A plutonium immobilization process

    SciTech Connect

    Rask, W.C.; Phillips, A.G.

    1996-05-01

    This paper describes a low temperature technique for stabilizing and immobilizing actinide compounds using a combination process/storage vessel of stainless steel, in which measured amounts of actinide nitrate solutions and actinide oxides (and/or residues) are systematically treated to yield a solid article. The chemical ceramic process is based on a coating technology that produces rare earth oxide coatings for defense applications involving plutonium. The final product of this application is a solid, coherent actinide oxide with process-generated encapsulation that has long-term environmental stability. Actinide compounds can be stabilized as pure materials for ease of re-use or as intimate mixtures with additives such as rare earth oxides to increase their degree of proliferation resistance. Starting materials for the process can include nitrate solutions, powders, aggregates, sludges, incinerator ashes, and others. Agents such as cerium oxide or zirconium oxide may be added as powders or precursors to enhance the properties of the resulting solid product. Additives may be included to produce a final product suitable for use in nuclear fuel pellet production. The process is simple and reduces the time and expense for stabilizing plutonium compounds. It requires a very low equipment expenditure and can be readily implemented into existing gloveboxes. The process is easily conducted with less associated risk than proposed alternative technologies.

  1. Plutonium focus area. Technology summary

    SciTech Connect

    1997-09-01

    The Assistant Secretary for the Office of Environmental Management (EM) at the U.S. Department of Energy (DOE) chartered the Plutonium Focus Area (PFA) in October 1995. The PFA {open_quotes}...provides for peer and technical reviews of research and development in plutonium stabilization activities...{close_quotes} In addition, the PFA identifies and develops relevant research and technology. The purpose of this document is to focus attention on the requirements used to develop research and technology for stabilization, storage, and preparation for disposition of nuclear materials. The PFA Technology Summary presents the approach the PFA uses to identify, recommend, and review research. It lists research requirements, research being conducted, and gaps where research is needed. It also summarizes research performed by the PFA in the traditional research summary format. This document encourages researchers and commercial enterprises to do business with PFA by submitting research proposals or {open_quotes}white papers.{close_quotes} In addition, it suggests ways to increase the likelihood that PFA will recommend proposed research to the Nuclear Materials Stabilization Task Group (NMSTG) of DOE.

  2. 10 CFR 140.108 - Appendix H-Form of indemnity agreement with licensees possessing plutonium for use in plutonium...

    Code of Federal Regulations, 2013 CFR

    2013-01-01

    ... possessing plutonium for use in plutonium processing and fuel fabrication plants and furnishing proof of... Appendixes to Part 140 § 140.108 Appendix H—Form of indemnity agreement with licensees possessing plutonium for use in plutonium processing and fuel fabrication plants and furnishing proof of...

  3. 10 CFR 140.108 - Appendix H-Form of indemnity agreement with licensees possessing plutonium for use in plutonium...

    Code of Federal Regulations, 2014 CFR

    2014-01-01

    ... possessing plutonium for use in plutonium processing and fuel fabrication plants and furnishing proof of... Appendixes to Part 140 § 140.108 Appendix H—Form of indemnity agreement with licensees possessing plutonium for use in plutonium processing and fuel fabrication plants and furnishing proof of...

  4. 10 CFR 140.108 - Appendix H-Form of indemnity agreement with licensees possessing plutonium for use in plutonium...

    Code of Federal Regulations, 2012 CFR

    2012-01-01

    ... possessing plutonium for use in plutonium processing and fuel fabrication plants and furnishing proof of... Appendixes to Part 140 § 140.108 Appendix H—Form of indemnity agreement with licensees possessing plutonium for use in plutonium processing and fuel fabrication plants and furnishing proof of...

  5. 10 CFR 140.108 - Appendix H-Form of indemnity agreement with licensees possessing plutonium for use in plutonium...

    Code of Federal Regulations, 2011 CFR

    2011-01-01

    ... possessing plutonium for use in plutonium processing and fuel fabrication plants and furnishing proof of... Appendixes to Part 140 § 140.108 Appendix H—Form of indemnity agreement with licensees possessing plutonium for use in plutonium processing and fuel fabrication plants and furnishing proof of...

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

    SciTech Connect

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

    1985-01-01

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

  7. Measuring SNM Isotopic Distributions using FRAM

    SciTech Connect

    Geist, William H.

    2015-12-02

    The first group of slides provides background information on the isotopic composition of plutonium. It is shown that 240Pu is the critical isotope in neutron coincidence/multiplicity counting. Next, response function analysis to determine isotopic composition is discussed. The isotopic composition can be determined by measuring the net peak counts from each isotope and then taking the ratio of the counts for each isotope relative to the total counts for the element. Then FRAM (Fixed energy Response function Analysis with Multiple efficiencies) is explained. FRAM can control data acquisition, automatically analyze newly acquired data, analyze previously acquired data, provide information on the quality of the analysis, and facilitate analysis in unusual situations (non-standard energy calibrations, gamma rays from non-SNM isotopes, poor spectra (within limits)).

  8. Volatile fluoride process for separating plutonium from other materials

    DOEpatents

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

    1959-04-14

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

  9. VOLATILE FLUORIDE PROCESS FOR SEPARATING PLUTONIUM FROM OTHER MATERIALS

    DOEpatents

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

    1959-04-14

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

  10. Measurements of plutonium, 237Np, and 137Cs in the BCR 482 lichen reference material

    DOE PAGES

    Lavelle, Kevin B.; Miller, Jeffrey L.; Hanson, Susan K.; ...

    2015-10-01

    Select anthropogenic radionuclides were measured in lichen reference material, BCR 482. This material was originally collected in Axalp, Switzerland in 1991 and is composed of the epiphytic lichen Pseudevernia furfuracea. Samples from three separate bottles of BCR 482 were analyzed for uranium, neptunium, and plutonium isotopes by inductively coupled plasma mass spectrometry (ICP-MS) and analyzed for cesium-137 by gamma-ray spectrometry. The isotopic composition of the radionuclides measured in BCR 482 suggests contributions from both global fallout resulting from historical nuclear weapons testing and more volatile materials released following the Chernobyl accident.

  11. Plutonium Finishing Plant (PFP) Waste Composition and High Efficiency Particulate Air Filter Loading

    SciTech Connect

    ZIMMERMAN, B.D.

    2000-12-11

    This analysis evaluates the effect of the Plutonium Finishing Plant (PFP) waste isotopic composition on Tank Farms Final Safety Analysis Report (FSAR) accidents involving high-efficiency particulate air (HEPA) filter failure in Double-Contained Receiver Tanks (DCRTs). The HEPA Filter Failure--Exposure to High Temperature or Pressure, and Steam Intrusion From Interfacing Systems accidents are considered. The analysis concludes that dose consequences based on the PFP waste isotopic composition are bounded by previous FSAR analyses. This supports USQD TF-00-0768.

  12. Gastrointestinal absorption of plutonium, uranium and neptunium in fed and fasted adult baboons: Application to humans

    SciTech Connect

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

    1992-03-01

    Gastrointestinal (GI) absorption values of plutonium, uranium, and neptunium were determined in fed and fasted adult baboons. A dual isotope method of determining GI absorption, which does not require animal sacrifice, was validated and shown to compare well with the sacrifice method (summation of oral isotope in urine with that in tissues at sacrifice). For all three elements, mean GI absorption values were significantly high (5- to 50-fold) in 24-hour (h)-fasted animals than in fed animals, and GI absorption values for baboons agreed well with those for humans.

  13. How much plutonium does North Korea have?

    SciTech Connect

    Albright, D.

    1994-09-01

    U.S. intelligence discovered in the 1980s that North Korea was building a small nuclear reactor. The reactor was described as a gas-cooled, graphite-moderated model similar to those Britian and France used to produce electric power as well as plutonium for nuclear weapons. When Western nations expressed concern about the reactor Russia pressed North Korea to sign the Non-Proliferation Treaty (NPT) which it did on December 12, 1985. However, North Korea stalled on signing the required safeguards agreement that allows the International Atomic Energy Agency (IAEA) to inspect nuclear facilities until January 1992. Inspections by the IAEA revealed discrepancies with the amounts of plutonium separated as declared by the North Koreans. The IAEA also received reports that two North Korean waste sites were hidden. By February 1993 the IAEA and the North Koreans has reached an impasse: North Koreas initial declarations of plutonium inventory could not be confirmed and North Korea refused to cooperate. At the least, North Korea admits to having separated 100 grams of plutonium. At the most, worst case estimate, they could have a total of 6 - 13 kilograms of separated plutonium. A first nuclear weapon can require up to 10 kilograms of weapon-grade plutonium. Any settlement needs to include a way to insure that the IAEA can verify North Korea`s past nuclear activities and determine the amount of plutonium that may have been separated in the past. 2 refs.

  14. Analysis of IAEA Environmental Samples for Plutonium and Uranium by ICP/MS in Support Of International Safeguards

    SciTech Connect

    Farmer, Orville T.; Olsen, Khris B.; Thomas, May-Lin P.; Garofoli, Stephanie J.

    2008-05-01

    A method for the separation and determination of total and isotopic uranium and plutonium by ICP-MS was developed for IAEA samples on cellulose-based media. Preparation of the IAEA samples involved a series of redox chemistries and separations using TRU® resin (Eichrom). The sample introduction system, an APEX nebulizer (Elemental Scientific, Inc), provided enhanced nebulization for a several-fold increase in sensitivity and reduction in background. Application of mass bias (ALPHA) correction factors greatly improved the precision of the data. By combining the enhancements of chemical separation, instrumentation and data processing, detection levels for uranium and plutonium approached high attogram levels.

  15. Excess Weapons Plutonium Immobilization in Russia

    SciTech Connect

    Jardine, L.; Borisov, G.B.

    2000-04-15

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

  16. RECOVERY OF PLUTONIUM FROM AQUEOUS SOLUTIONS

    DOEpatents

    Reber, E.J.

    1959-09-01

    A process is described for recovering plutonium values from aqueous solutions by precipitation on bismuth phosphate. The plutonium is secured in its tetravalent state. bismuth salt is added to the solution, and ant excess of phosphoric acid anions is added to the solution in two approximately equal installments. The rate of addition of the first installment is about two to three times as high as the rate of addition of the second installment, whereby a precipitate of bismuth phosphate forms, the precipitate carrying the plutonium values. The precipitate is separated from the solution.

  17. SEPARATION OF URANIUM, PLUTONIUM AND FISSION PRODUCTS

    DOEpatents

    Nicholls, C.M.; Wells, I.; Spence, R.

    1959-10-13

    The separation of uranium and plutonium from neutronirradiated uranium is described. The neutron-irradiated uranium is dissolved in nitric acid to provide an aqueous solution 3N in nitric acid. The fission products of the solution are extruded by treating the solution with dibutyl carbitol substantially 1.8N in nitric acid. The organic solvent phase is separated and neutralized with ammonium hydroxide and the plutonium reduced with hydroxylamine base to the trivalent state. Treatment of the mixture with saturated ammonium nitrate extracts the reduced plutonium and leaves the uranium in the organic solvent.

  18. Immobilization of excess weapons plutonium in Russia

    SciTech Connect

    Borisov, G B; Jardine, L J; Mansourov, O A

    1999-01-25

    In this paper, we examine the logic and framework for the development of a capability to immobilize excess Russian weapons plutonium by the year 2004. The initial activities underway in Russia, summarized here, include engineering feasibility studies of the immobilization of plutonium-containing materials at the Krasnoyarsk and Mayak industrial sites. In addition, research and development (R&D) studies are underway at Russian institutes to develop glass and ceramic forms suitable for the immobilization of plutonium-containing materials, residues, and wastes and for their geologic disposal.

  19. Removal of plutonium from hepatic tissue

    DOEpatents

    Lindenbaum, Arthur; Rosenthal, Marcia W.

    1979-01-01

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

  20. HENC performance evaluation and plutonium calibration

    SciTech Connect

    Menlove, H.O.; Baca, J.; Pecos, J.M.; Davidson, D.R.; McElroy, R.D.; Brochu, D.B.

    1997-10-01

    The authors have designed a high-efficiency neutron counter (HENC) to increase the plutonium content in 200-L waste drums. The counter uses totals neutron counting, coincidence counting, and multiplicity counting to determine the plutonium mass. The HENC was developed as part of a Cooperative Research and Development Agreement between the Department of Energy and Canberra Industries. This report presents the results of the detector modifications, the performance tests, the add-a-source calibration, and the plutonium calibration at Los Alamos National Laboratory (TA-35) in 1996.

  1. Plutonium Immobilization Can Loading Conceptual Design

    SciTech Connect

    Kriikku, E.

    1999-05-13

    'The Plutonium Immobilization Facility will encapsulate plutonium in ceramic pucks and seal the pucks inside welded cans. Remote equipment will place these cans in magazines and the magazines in a Defense Waste Processing Facility (DWPF) canister. The DWPF will fill the canister with glass for permanent storage. This report discusses the Plutonium Immobilization can loading conceptual design and includes a process block diagram, process description, preliminary equipment specifications, and several can loading issues. This report identifies loading pucks into cans and backfilling cans with helium as the top priority can loading development areas.'

  2. NON-CORROSIVE PLUTONIUM FUEL SYSTEMS

    DOEpatents

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

    1962-10-23

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

  3. Weapons-grade plutonium dispositioning. Volume 4. Plutonium dispositioning in light water reactors

    SciTech Connect

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

    1993-06-01

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

  4. Determination of plutonium in environmental samples by AMS and alpha spectrometry.

    PubMed

    Hrnecek, E; Steier, P; Wallner, A

    2005-01-01

    Environmental samples from nuclear weapons test sites at the atolls of Mururoa and Fangataufa (French Polynesia, south Pacific) have been analyzed for their content of plutonium isotopes by applying the independent techniques of decay counting (Alpha Spectrometry) and accelerator mass spectrometry (AMS). Here, we propose the combination of both techniques which results in a maximum of information on the isotopic signature of Pu in environmental samples. Plutonium was chemically separated from the bulk material by anion exchange. (242)Pu was used as an internal standard for both AMS and alpha spectrometry. The samples for alpha spectrometry were prepared by micro-precipitation with NdF(3). After alpha spectrometry, the samples were reprocessed for AMS. Pu was co-precipitated with Fe(OH)(3) and finally, solid samples were prepared. At the VERA (Vienna Environmental Research Accelerator) facility, the various Pu isotopes were separated by their isotopic masses and quantified by the AMS technique. A good agreement of the results obtained from the AMS measurements was found with those obtained from Alpha Spectrometry. Overall, the data agree on average within 10% of each other. Isotope ratios for (238)Pu, (239)Pu and (240)Pu can be extracted from our investigations. Alpha spectrometry delivers data for the (238)Pu and the combination of ((239+240))Pu concentrations in those samples. In addition, the AMS technique provides information on the individual concentrations of (240)Pu and (239)Pu.

  5. Spectrophotometric determination of plutonium-239 based on the spectrum of plutonium(III) chloride

    SciTech Connect

    Temer, D.J.; Walker, L.F.

    1994-07-01

    This report describes a spectrophotometric method for determining plutonium-239 (Pu-239) based on the spectrum of Pu(III) chloride. The authors used the sealed-reflux technique for the dissolution of plutonium oxide with hydrochloric acid (HCl) and small amounts of nitric and hydrofluoric acids. To complex the fluoride, they added zirconium, and to reduce plutonium to Pu(III), they added ascorbic acid. They then adjusted the solution to a concentration of 2 M HCl and measured the absorbances at five wavelengths of the Pu(III) chloride spectrum. This spectrophotometric determination can also be applied to samples of plutonium metal dissolved in HCl.

  6. PRODUCTION OF PLUTONIUM FLUORIDE FROM BISMUTH PHOSPHATE PRECIPITATE CONTAINING PLUTONIUM VALUES

    DOEpatents

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

    1961-05-01

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

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

    SciTech Connect

    Narlesky, Joshua E; Padilla, Dennis D; Watts, Joe

    2009-01-01

    developed so that the largest sources that are representative of the collection are included. One representative source was chosen for every 20 sources in the collection, and effort was made to preserve sources unique to the collection. In total, four representative sources and five unique sources were selected for the archive. The archive samples contain 40 grams of plutonium with an isotopic composition similar to that of weapon grade material and three grams of plutonium with an isotopic composition similar to that of reactor grade plutonium.

  8. New, room-temperature gamma-ray detector for improved assay of plutonium

    SciTech Connect

    Russo, P.A.; Meier, A.P.; Rawool-Sullivan, M.

    1997-11-01

    Gamma-ray spectroscopy for portable and unattended assay of nuclear materials requires rugged, reliable, room-temperature detectors that are stable in variable environments and detect gamma rays with good efficiency and energy resolution. For portable assays especially, compact detectors address needs for large numbers of measurements performed in rapid succession with heavy shielding and collimation by a user who must carry the spectroscopy equipment. Most measurements are made with compact NaI detectors. The assay of variable-burnup plutonium and other plutonium materials of variable isotopic composition challenges low-resolution gamma-ray spectroscopy in numerous safeguards applications including holdup measurements, safeguards inspections, monitoring, and safeguards close-out in decontamination and decommissioning. A new, commercial-prototype coplanar-grid CdZnTe detector has been evaluated using the assay of variable-burnup plutonium as a metric indicator to show the substantial benefit of its improved performance compared to results of the same measurements performed with the compact NaI detector. Detector performance, spectrum-quality, and assay results as well as gamma-ray spectra of reference sources are compared for the coplanar-grid CdZnTe and compact NaI detectors to illustrate the advantages of the new room-temperature gamma-ray detector. Isotope identification with the coplanar-grid CdZnTe detector is demonstrated. Preliminary calculations (Monte Carlo coupled to simulations of radiation transport and charge collection) of the spectral response of the detector to plutonium indicate promise for the use of the coplanar-grid CdZnTe detector for further improvements in the accuracy of assays and for analysis of gamma-ray isotopic distributions.

  9. SUBSURFACE MOBILE PLUTONIUM SPECIATION: SAMPLING ARTIFACTS FOR GROUNDWATER COLLOIDS

    SciTech Connect

    Kaplan, D.; Buesseler, K.

    2010-06-29

    A recent review found several conflicting conclusions regarding colloid-facilitated transport of radionuclides in groundwater and noted that colloids can both facilitate and retard transport. Given these contrasting conclusions and the profound implications even trace concentrations of plutonium (Pu) have on the calculated risk posed to human health, it is important that the methodology used to sample groundwater colloids be free of artifacts. The objective of this study was: (1) to conduct a field study and measure Pu speciation, ({sup 239}Pu and {sup 240}Pu for reduced-Pu{sub aq}, oxidized-Pu{sub aq}, reduced-Pu{sub colloid}, and oxidized-Pu{sub colloid}), in a Savannah River Site (SRS) aquifer along a pH gradient in F-Area, (2) to determine the impact of pumping rate on Pu concentration, Pu speciation, and Pu isotopic ratios, (3) determine the impact of delayed sample processing (as opposed to processing directly from the well).

  10. Monte Carlo simulations of plutonium gamma-ray spectra

    SciTech Connect

    Koenig, Z.M.; Carlson, J.B.; Wang, Tzu-Fang; Ruhter, W.D.

    1993-07-16

    Monte Carlo calculations were investigated as a means of simulating the gamma-ray spectra of Pu. These simulated spectra will be used to develop and evaluate gamma-ray analysis techniques for various nondestructive measurements. Simulated spectra of calculational standards can be used for code intercomparisons, to understand systematic biases and to estimate minimum detection levels of existing and proposed nondestructive analysis instruments. The capability to simulate gamma-ray spectra from HPGe detectors could significantly reduce the costs of preparing large numbers of real reference materials. MCNP was used for the Monte Carlo transport of the photons. Results from the MCNP calculations were folded in with a detector response function for a realistic spectrum. Plutonium spectrum peaks were produced with Lorentzian shapes, for the x-rays, and Gaussian distributions. The MGA code determined the Pu isotopes and specific power of this calculated spectrum and compared it to a similar analysis on a measured spectrum.

  11. Opportunities in Plutonium Metallurgical Research

    SciTech Connect

    Schwartz, A J

    2006-12-19

    This is an exciting time to be involved in plutonium metallurgical research. Over the past few years, there have been significant advances in our understanding of the fundamental materials science of this unusual metal, particularly in the areas of self-irradiation induced aging of Pu, the equilibrium phase diagram, the homogenization of {delta}-phase alloys, the crystallography and morphology of the {alpha}{prime}-phase resulting from the isothermal martensitic phase transformation, and the phonon dispersion curves, among many others. In addition, tremendous progress has been made, both experimentally and theoretically, in our understanding of the condensed matter physics and chemistry of the actinides, particularly in the area of electronic structure. Although these communities have made substantial progress, many challenges still remain. This brief overview will address a number of important challenges that we face in fully comprehending the metallurgy of Pu with a specific focus on aging and phase transformations.

  12. PLUTONIUM METALLOGRAPHY AT LOS ALAMOS

    SciTech Connect

    PEREYRA, RAMIRO A.; LOVATO, DARRYL

    2007-01-08

    From early days of the Manhattan program to today, scientists and engineers have continued to investigate the metallurgical properties of plutonium (Pu). Although issues like aging was not a concern to the early pioneers, today the reliability of our aging stockpile is of major focus. And as the country moves toward a new generation of weapons similar problems that the early pioneers faced such as compatibility, homogeneity and malleability have come to the forefront. And metallography will continue to be a principle tool for the resolution of old and new issues. Standard metallographic techniques are used for the preparation of plutonium samples. The samples are first cut with a slow speed idamond saw. After mounting in Epon 815 epoxy resin, the samples are ground through 600 grit silicon carbide paper. PF 5070 (a Freon substitute) is used as a coolant, lubricant, and solvent for most operations. Rough mechanical polished is done with 9-{mu} diamond using a nap less cloth, for example nylon or cotton. Final polish is done with 1-{mu} diamond on a nappy cloth such as sylvet. Ethyl alcohol is then used ultrasonically to clean the samples before electro polishing. The sample is then electro-polished and etched in an electrolyte containing 10% nitric acid, and 90% dimethyleneformalmide. Ethyl alcohol is used as a final cleaning agent. Although standard metallographic preparation techniques are used, there are several reasons why metallography of Pu is difficult and challenging. Firstly, because of the health hazards associated with its radioactive properties, sample preparation is conducted in glove boxes. Figure 1 shows the metallography line, in an R and D facility. Since they are designed to be negative in pressure to the laboratory, cross-contamination of abrasives is a major problem. In addition, because of safety concerns and waste issues, there is a limit to the amount of solvent that can be used. Secondly, Pu will readily hydride or oxidize when in contact

  13. A Plutonium Storage Container Pressure Measurement Technique

    SciTech Connect

    Grim, T.J.

    2002-05-10

    Plutonium oxide and metal awaiting final disposition are currently stored at the Savannah River Site in crimp sealed food pack cans. Surveillances to ensure continued safe storage of the cans include periodic lid deflection measurements using a mechanical device.

  14. SEPARATION OF URANIUM, PLUTONIUM, AND FISSION PRODUCTS

    DOEpatents

    Spence, R.; Lister, M.W.

    1958-12-16

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

  15. IMPROVED PROCESS OF PLUTONIUM CARRIER PRECIPITATION

    DOEpatents

    Faris, B.F.

    1959-06-30

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

  16. Recent plutonium metal production experience at Hanford

    SciTech Connect

    Gibson, M.W.; Nyman, D.H. )

    1989-11-01

    Plutonium metal is produced at the Hanford site in the remote mechanical C (RMC) line. The line is housed in the plutonium finishing plant (PFP). The PFP is operated by the Westinghouse Hanford Company for the U.S. Department of Energy. The RMC line was built in the early 1960s and operated until 1973 when it was shut down. The line was restarted in 1985 and has operated on a campaign basis since that time. The RMC line converts plutonium nitrate solution to plutonium metal in the classic precipitation/calcination/fluorination/reduction process. The operations are contained in glove boxes with a dry air atmosphere. Most of the process is remotely controlled from a central control room. Numerous process improvements were made in the line before initiating operations in 1985 and in 1988. These changes, in conjunction with improved conduct of operations, have resulted in improved yields.

  17. Pulmonary carcinogenesis from plutonium-containing particles

    SciTech Connect

    Thomas, R.G.; Smith, D.M.; Anderson, E.C.

    1980-01-01

    Plutonium administered as an alpha radiation source to the respiratory tracts of Syrian hamsters has resulted in various incidences of neoplasia. Adenomas are the primary lung tumor observed, but adenocarcinomas are also prevalent.

  18. Design and evaluation of plutonium electrorefining cells

    SciTech Connect

    Not Available

    1987-01-01

    A plutonium electrorefining cell was designed for stationary furnace operation. This cell and the LANL electrorefining cell were evaluated. Results of this evaluation and comparison to existing production electrorefining at Rocky Flats are presented.

  19. Plutonium finishing plant dangerous waste training plan

    SciTech Connect

    ENTROP, G.E.

    1999-05-24

    This training plan describes general requirements, worker categories, and provides course descriptions for operation of the Plutonium Finish Plant (PFP) waste generation facilities, permitted treatment, storage and disposal (TSD) units, and the 90-Day Accumulation Areas.

  20. Leaching behavior of particulate plutonium oxide

    SciTech Connect

    Kosiewicz, S.T.; Heaton, R.C.

    1985-08-01

    Different size cuts of /sup 238/PuO/sub 2/ particles were mixed with deionized water at two temperatures in a shaker bath. The gross plutonium concentration in the water was measured, as well as that portion of the plutonium retained on a 0.1-..mu..m pore filter. The concentration of the plutonium released was primarily a function of the surface area of the particles. The release rate of plutonium into the water for the size cut with particles having diameters between 30 and 20 ..mu..m was 3 ng/m/sup 2//s; this rate is within the range observed in past experiments involving aquatic environments. The amount of material retained by the 0.1-..mu..m filters decreased with increasing time, suggesting that size reduction or removal processes occurred. 6 refs., 3 figs., 9 tabs.

  1. Plutonium focus area: Technology summary

    SciTech Connect

    1996-03-01

    To ensure research and development programs focus on the most pressing environmental restoration and waste management problems at the U.S. Department of Energy (DOE), the Assistant Secretary for the Office of Environmental Management (EM) established a working group in August 1993 to implement a new approach to research and technology development. As part of this approach, EM developed a management structure and principles that led to creation of specific focus areas. These organizations were designed to focus scientific and technical talent throughout DOE and the national scientific community on major environmental restoration and waste management problems facing DOE. The focus area approach provides the framework for inter-site cooperation and leveraging of resources on common problems. After the original establishment of five major focus areas within the Office of Technology Development (EM-50), the Nuclear Materials Stabilization Task Group (NMSTG, EM-66) followed EM-50`s structure and chartered the Plutonium Focus Area (PFA). NMSTG`s charter to the PFA, described in detail later in this book, plays a major role in meeting the EM-66 commitments to the Defense Nuclear Facilities Safety Board (DNFSB). The PFA is a new program for FY96 and as such, the primary focus of revision 0 of this Technology Summary is an introduction to the Focus Area; its history, development, and management structure, including summaries of selected technologies being developed. Revision 1 to the Plutonium Focus Area Technology Summary is slated to include details on all technologies being developed, and is currently planned for release in August 1996. The following report outlines the scope and mission of the Office of Environmental Management, EM-60, and EM-66 organizations as related to the PFA organizational structure.

  2. Plutonium and minor actinide utilisation in a pebble-bed high temperature reactor

    SciTech Connect

    Petrov, B. Y.; Kuijper, J. C.; Oppe, J.; De Haas, J. B. M.

    2012-07-01

    This paper contains results of the analysis of the pebble-bed high temperature gas-cooled PUMA reactor loaded with plutonium and minor actinide (Pu/MA) fuel. Starting from knowledge and experience gained in the Euratom FP5 projects HTR-N and HTR-N1, this study aims at demonstrating the potential of high temperature reactors to utilize or transmute Pu/MA fuel. The work has been performed within the Euratom FP6 project PUMA. A number of different fuel types and fuel configurations have been analyzed and compared with respect to incineration performance and safety-related reactor parameters. The results show the excellent plutonium and minor actinide burning capabilities of the high temperature reactor. The largest degree of incineration is attained in the case of an HTR fuelled by pure plutonium fuel as it remains critical at very deep burnup of the discharged pebbles. Addition of minor actinides to the fuel leads to decrease of the achievable discharge burnup and therefore smaller fraction of actinides incinerated during reactor operation. The inert-matrix fuel design improves the transmutation performance of the reactor, while the 'wallpaper' fuel does not have advantage over the standard fuel design in this respect. After 100 years of decay following the fuel discharge, the total amount of actinides remains almost unchanged for all of the fuel types considered. Among the plutonium isotopes, only the amount of Pu-241 is reduced significantly due to its relatively short half-life. (authors)

  3. A Program to Stabilize Nuclear Materials as Managed by the Plutonium Focus Area

    SciTech Connect

    B. Kenley; B. Scott; B. Seidel; D. Knecht; F. Southworth; K. Osborne; N. Chipman; T. Creque

    1999-03-01

    This paper describes the program to stabilize nuclear materials, consistent with the Department of Energy Office of Environmental Management (EM) plan, Accelerating Cleanup: Paths to Closure. The program is managed by the Plutonium Stabilization and Disposition Focus Area, which defines and manages technology development programs to stabilize nuclear materials and assure their subsequent safe storage and final disposition. The scope of the Plutonium Stabilization and Disposition Focus Area (PFA) activities includes non-weapons plutonium materials, special isotopes, and other fissile materials. The PFA provides solutions to site-specific and complex wide technology issues associated with plutonium remediation, stabilization, and preparation for disposition. Our paper describes an important programmatic function of the Department of Energy nuclear materials stabilization program, including the tie-in of policy to research needs and funding for the nuclear materials disposition area. The PFA uses a rigorous systems engineering determination of technology needs and gaps, under the guidance of a Technical Advisory Panel, consisting of complex-wide experts. The Research and Development planning provides an example for other waste areas and should be of interest to Research and Development managers. The materials disposition maps developed by the PFA and described in this paper provide an evaluation of research needs, data gaps and subsequent guidance for the development of technologies for nuclear materials disposition. This paper also addresses the PFA prioritization methodology and its ability to forecast actual time to implementation.

  4. PLUTONIUM CARRIER METATHESIS WITH ORGANIC REAGENT

    DOEpatents

    Thompson, S.G.

    1958-07-01

    A method is described for converting a plutonium containing bismuth phosphate carrier precipitate Into a compositton more readily soluble in acid. The method consists of dissolving the bismuth phosphate precipitate in an aqueous solution of alkali metal hydroxide, and adding one of a certaia group of organic compounds, e.g., polyhydric alcohols or a-hydrorycarboxylic acids. The mixture is then heated causiing formation of a bismuth hydroxide precipitate containing plutonium which may be readily dissolved in nitric acid for further processing.

  5. Plutonium: The first 50 years. United States plutonium production, acquisition, and utilization from 1944 through 1994

    SciTech Connect

    1996-02-01

    The report contains important newly declassified information regarding the US production, acquisition, and removals of plutonium. This new information, when combined with previously declassified data, has allowed the DOE to issue, for the first time, a truly comprehensive report on the total DOE plutonium inventory. At the December 7, 1993, Openness Press Conference, the DOE declassified the plutonium inventories at eight locations totaling 33.5 metric tons (MT). This report declassifies the remainder of the DOE plutonium inventory. Newly declassified in this report is the quantity of plutonium at the Pantex Site, near Amarillo, Texas, and in the US nuclear weapons stockpile of 66.1 MT, which, when added to the previously released inventory of 33.5 MT, yields a total plutonium inventory of 99.5 MT. This report will document the sources which built up the plutonium inventory as well as the transactions which have removed plutonium from that inventory. This report identifies four sources that add plutonium to the DOE/DoD inventory, and seven types of transactions which remove plutonium from the DOE/DoD inventory. This report also discusses the nuclear material control and accountability system which records all nuclear material transactions, compares records with inventory and calculates material balances, and analyzes differences to verify that nuclear materials are in quantities as reported. The DOE believes that this report will aid in discussions in plutonium storage, safety, and security with stakeholders as well as encourage other nations to declassify and release similar data. These data will also be available for formulating policies with respect to disposition of excess nuclear materials. The information in this report is based on the evaluation of available records. The information contained in this report may be updated or revised in the future should additional or more detailed data become available.

  6. Preparation of Small Well Characterized Plutonium Oxide Reference Materials and Demonstration of the Usefulness of Such Materials for Nondestructive Analysis

    SciTech Connect

    B.A. Guillen; S.T. Hsue; J.Y Huang; P.A. Hypes; S.M. Long; C.R. Rudy; P.A. Russo; J.E. Stewart; D.J. Temer

    2003-01-01

    Calibration of neutron coincidence and multiplicity counters for passive nondestructive analysis (NDA) of plutonium requires knowledge of the detector efficiency parameters. These are most often determined empirically. Bias from multiplication and unknown impurities may be incurred even with small plutonium metal samples. Five sets of small, pure plutonium metal standards prepared with well-known geometry and very low levels of impurities now contribute to determining accurate multiplication corrections. Recent measurements of these metal standards, with small but well-defined multiplication and negligible yield of other than fission neutrons, demonstrate an improved characterization and calibration of neutron coincidence/multiplicity counters. The precise knowledge of the mass and isotopic composition of each standard also contributes significantly to verifying the accuracy of the most precise calorimetry and gamma-ray spectroscopy measurements.

  7. A DGT technique for plutonium bioavailability measurements.

    PubMed

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

    2014-09-16

    The toxicity of heavy metals in natural waters is strongly dependent on the local chemical environment. Assessing the bioavailability of radionuclides predicts the toxic effects to aquatic biota. The technique of diffusive gradients in thin films (DGT) is largely exploited for bioavailability measurements of trace metals in waters. However, it has not been applied for plutonium speciation measurements yet. This study investigates the use of DGT technique for plutonium bioavailability measurements in chemically different environments. We used a diffusion cell to determine the diffusion coefficients (D) of plutonium in polyacrylamide (PAM) gel and found D in the range of 2.06-2.29 × 10(-6) cm(2) s(-1). It ranged between 1.10 and 2.03 × 10(-6) cm(2) s(-1) in the presence of fulvic acid and in natural waters with low DOM. In the presence of 20 ppm of humic acid of an organic-rich soil, plutonium diffusion was hindered by a factor of 5, with a diffusion coefficient of 0.50 × 10(-6) cm(2) s(-1). We also tested commercially available DGT devices with Chelex resin for plutonium bioavailability measurements in laboratory conditions and the diffusion coefficients agreed with those from the diffusion cell experiments. These findings show that the DGT methodology can be used to investigate the bioaccumulation of the labile plutonium fraction in aquatic biota.

  8. Disposal of Surplus Weapons Grade Plutonium

    SciTech Connect

    H. Alsaed; P. Gottlieb

    2000-09-12

    The Office of Fissile Materials Disposition is responsible for disposing of inventories of surplus US weapons-usable plutonium and highly enriched uranium as well as providing, technical support for, and ultimate implementation of, efforts to obtain reciprocal disposition of surplus Russian plutonium. On January 4, 2000, the Department of Energy issued a Record of Decision to dispose of up to 50 metric tons of surplus weapons-grade plutonium using two methods. Up to 17 metric tons of surplus plutonium will be immobilized in a ceramic form, placed in cans and embedded in large canisters containing high-level vitrified waste for ultimate disposal in a geologic repository. Approximately 33 metric tons of surplus plutonium will be used to fabricate MOX fuel (mixed oxide fuel, having less than 5% plutonium-239 as the primary fissile material in a uranium-235 carrier matrix). The MOX fuel will be used to produce electricity in existing domestic commercial nuclear reactors. This paper reports the major waste-package-related, long-term disposal impacts of the two waste forms that would be used to accomplish this mission. Particular emphasis is placed on the possibility of criticality. These results are taken from a summary report published earlier this year.

  9. Plutonium Finishing Plant safety evaluation report

    SciTech Connect

    Not Available

    1995-01-01

    The Plutonium Finishing Plant (PFP) previously known as the Plutonium Process and Storage Facility, or Z-Plant, was built and put into operation in 1949. Since 1949 PFP has been used for various processing missions, including plutonium purification, oxide production, metal production, parts fabrication, plutonium recovery, and the recovery of americium (Am-241). The PFP has also been used for receipt and large scale storage of plutonium scrap and product materials. The PFP Final Safety Analysis Report (FSAR) was prepared by WHC to document the hazards associated with the facility, present safety analyses of potential accident scenarios, and demonstrate the adequacy of safety class structures, systems, and components (SSCs) and operational safety requirements (OSRs) necessary to eliminate, control, or mitigate the identified hazards. Documented in this Safety Evaluation Report (SER) is DOE`s independent review and evaluation of the PFP FSAR and the basis for approval of the PFP FSAR. The evaluation is presented in a format that parallels the format of the PFP FSAR. As an aid to the reactor, a list of acronyms has been included at the beginning of this report. The DOE review concluded that the risks associated with conducting plutonium handling, processing, and storage operations within PFP facilities, as described in the PFP FSAR, are acceptable, since the accident safety analyses associated with these activities meet the WHC risk acceptance guidelines and DOE safety goals in SEN-35-91.

  10. Complementary technologies for verification of excess plutonium

    SciTech Connect

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

    1998-12-31

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

  11. Recovery of plutonium from nitric acid waste

    SciTech Connect

    Muscatello, A.C.; Saba, M.T.; Navratil, J.D.

    1986-12-21

    Seven candidate materials, each contained in a static-bed column, have been evaluated for removing plutonium from nitric acid waste. Three materials have insufficient capacity for plutonium: TBP (tri-n-butylphosphate) sorbed on Amberlite XAD-4 resin, O phi D(IB)CMPO (octylphenyl-N, N-diisobutylcarbamoylmethylphosphine oxide) sorbed on XAD-4, and Amberlite IRA-938 anion exchange resin. The remaining four materials reduced 10/sup -3/ g/l plutonium in 7.2M HNO/sub 3/ to low 10/sup -5/ g/l for 80 bed volumes (BV). The 10% breakthrough capacities for 3 x 10/sup -2/ g/l plutonium are: TOPO (tri-n-octylphosphine oxide) on XAD-4 - 1800 BV, DHDECMP (dihexyl-N, N-diethylcarbamoylmethylphosphonate) on XAD-4 - 960 BV, Dowex 1 x 4 - 840 BV, and DHDECMP + TBP - 640 BV. Based on these results and generally poor elution of all materials, TOPO on XAD-4 is recommended as the best candidate for recovery of plutonium followed by acid digestion or combustion of the TOPO to recover the concentrated plutonium.

  12. Plutonium Speciation, Solubilization,And Migration in soils

    SciTech Connect

    Neu, Mary P.

    2000-12-31

    using improved data and better defined site conditions can be used to predict long-term contaminant behavior and can suggest particular Pu species for further study. Within this context, the specific tasks described in our original proposal are the following: l Site Characterization. The total plutonium content in soils surrounding the Rocky Flats Environmental Technology Site (RFETS) had been thoroughly characterized previously; however, less work has been done to separate plutonium in these soils into its sources (site activities at Rocky Flats or global fallout) and no work has successfully determined the speciation of the plutonium. Personnel at the site supported this effort by providing information, samples, and mechanisms to disseminate our results. Task 1--Characterize the plutonium in soils and groundwaters from the RFETS site, determining both the speciation, including concentration, isotopic ratio (239/240), oxidation state and specific chemical form, and the distribution, from a microscopic level (particle size, association with other elements) to a macroscopic level (depth in soil, location). To our knowledge, characterization with this level of detail has never been done for an environmental plutonium sample. Task 2--Communicate these results to the site to assist in site management, remediation, and stewardship.

  13. Plutonium and Uranium Atom Ratios and Activity Levels in Cochiti Lake Bottom Sediments Provided by Pueblo de Cochiti

    SciTech Connect

    Gallaher, B.M.; Efurd, D.W.; Rokop, D.J.; Benjamin, T.M.

    1999-05-01

    Historical operations at the Los Alamos National Laboratory have contaminated stream sediments with plutonium and other radionuclides. A small portion of these contaminated sediments has been carried by floods into the Rio Grande drainage system, eventually to be trapped by Cochiti Lake located on Pueblo de Cochiti lands approximately 8 km downstream of the Laboratory. In this study, lake bottom sediment samples provided by the Pueblo de Cochiti were analyzed by thermal ionization mass spectrometry to determine plutonium and uranium activity levels and isotopic atom ratios. This specialized analytical method allows us to take isotopic fingerprints of radionuclides found in the sediment and to determine how much plutonium and uranium came from the Laboratory and how much was deposited by worldwide fallout or is natural. Two distinct types of samples were processed: segments of a continuous vertical core of the entire accumulated sediment sequence and other samples from across the lake bottom at the water/sediment interface. Based on measurement of the {sup 240}Pu/{sup 239}Pu atom ratio, Laboratory-derived plutonium is present in eight of nine samples at the core site. On a depth-weighted basis, approximately one-half of the {sup 239}Pu and {sup 240}Pu came from early operations at the Laboratory; the remaining plutonium came from fallout dispersed by above-ground nuclear tests. In contrast to the core site, the samples from the other locations showed little or no evidence of Laboratory-derived plutonium, with more than 90 percent of the plutonium attributable to fallout. The overall amount of plutonium in all the samples is of the same magnitude as other reservoirs in the region. The net increase in plutonium over upstream reservoirs unaffected by Laboratory activities is a maximum of 0.014 pCi/g or 3.5 times. All of the samples reflect natural uranium compositions. Laboratory-derived uranium is not identifiable, presumably because the sediment contains abundant

  14. PROCESS OF FORMING PLUOTONIUM SALTS FROM PLUTONIUM EXALATES

    DOEpatents

    Garner, C.S.

    1959-02-24

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

  15. SEPARATION OF PLUTONIUM FROM URANIUM AND FISSION PRODUCTS

    DOEpatents

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

    1958-10-01

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

  16. Purification of aqueous plutonium chloride solutions via precipitation and washing.

    SciTech Connect

    Stroud, M. A.; Salazar, R. R.; Abney, Kent David; Bluhm, E. A.; Danis, J. A.

    2003-01-01

    Pyrochemical operations at Los Alamos Plutonium Facility (TA-55) use high temperature melt s of calcium chloride for the reduction of plutonium oxide to plutonium metal and hi gh temperature combined melts of sodium chloride and potassium chloride mixtures for the electrorefining purification of plutonium metal . The remaining plutonium and americium are recovered from thes e salts by dissolution in concentrated hydrochloric acid followed by either solvent extraction or io n exchange for isolation and ultimately converted to oxide after precipitation with oxalic acid . Figur e 1 illustrates the current aqueous chloride flow sheet used for plutonium processing at TA-55 .

  17. Plutonium measurements on the 1 MV AMS system at the Centro Nacional de Aceleradores (CNA)

    NASA Astrophysics Data System (ADS)

    Chamizo, Elena; Enamorado, Santiago Miguel; García-León, Manuel; Suter, Martin; Wacker, Lukas

    2008-11-01

    Plutonium isotopes have been recently added to the list of radionuclides that can be measured with the new generation of compact AMS facilities. In this paper we present first experimental results concerning the development of the plutonium AMS technique at 680 kV on the 1 MV AMS system at the Centro Nacional de Aceleradores (CNA) in Sevilla, Spain. This is the first compact AMS machine designed and manufactured by High Voltage Engineering Europa. As we demonstrate, the obtained backgrounds for 239,240Pu, of about 10 6 atoms, and the 239Pu/ 238U mass suppression factor, in the range of 10 -9, compare to the ones achieved on other AMS facilities. With the measurement of reference materials provided by the International Atomic Energy Agency (IAEA-375, IAEA-Soil-6, IAEA-381) and samples already studied on the 600 kV compact ETH/PSI AMS system at Zürich, we show that the CNA system can be perfectly used for the routine measurement of plutonium isotopes at environmental levels.

  18. Calculating Relative Ionization Probabilities of Plutonium for Resonance Ionization Mass Spectrometry to Support Nuclear Forensic Investigations

    NASA Astrophysics Data System (ADS)

    Lensegrav, Craig; Smith, Craig; Isselhardt, Brett

    2015-03-01

    Ongoing work seeks to apply the technology of Resonance Ionization Mass Spectrometry (RIMS) to problems related to nuclear forensics and, in particular, to the analysis and quantification of debris from nuclear detonations. As part of this effort, modeling and simulation methods are being applied to analyze and predict the potential for ionization by laser excitation of isotopes of both uranium and plutonium. Early work focused on the ionization potential of isotopes of uranium, and the present effort has expanded and extended the previous work by identifying and integrating new data for plutonium isotopes. In addition to extending the effort to this important new element, we have implemented more accurate descriptions of the spatial distribution of the laser beams to improve the accuracy of model predictions compared with experiment results as well as an ability to readily incorporate new experimental data as they become available. The model is used to estimate ionization cross sections and to compare relative excitation on two isotopes as a function of wavelength. This allows the study of sensitivity of these measurements to fluctuations in laser wavelength, irradiance, and bandwidth. We also report on initial efforts to include predictions of americium ionization probabilities into our modeling package. I would like to thank my co-authors, Gamani Karunasiri and Fabio Alves. My success is a product of their support and guidance.

  19. Assessing the Feasibility of Using Neutron Resonance Transmission Analysis (NRTA) for Assaying Plutonium in Spent Fuel Assemblies

    SciTech Connect

    D. L. Chichester; J. W. Sterbentz

    2012-07-01

    Neutron resonance transmission analysis (NRTA) is an active-interrogation nondestructive assay (NDA) technique capable of assaying spent nuclear fuel to determine plutonium content. Prior experimental work has definitively shown the technique capable of assaying plutonium isotope composition in spent-fuel pins to a precision of approximately 3%, with a spatial resolution of a few millimeters. As a Grand Challenge to investigate NDA options for assaying spent fuel assemblies (SFAs) in the commercial fuel cycle, Idaho National Laboratory has explored the feasibility of using NRTA to assay plutonium in a whole SFA. The goal is to achieve a Pu assay precision of 1%. The NRTA technique uses low-energy neutrons from 0.1-40 eV, at the bottom end of the actinide-resonance range, in a time-of-flight arrangement. Isotopic composition is determined by relating absorption of the incident neutrons to the macroscopic cross-section of the actinides of interest in the material, and then using this information to determine the areal density of the isotopes in the SFA. The neutrons used for NRTA are produced using a pulsed, accelerator-based neutron source. Distinguishable resonances exist for both the plutonium (239,240,241,242Pu) and uranium (235,236,238U) isotopes of interest in spent fuel. Additionally, in this energy range resonances exists for six important fission products (99Tc, 103Rh, 131Xe, 133Cs, 145Nd, and 152Sm) which provide additional information to support spent fuel plutonium assay determinations. Based on extensive modeling of the problem using Monte Carlo-based simulation codes, our preliminary results suggest that by rotating an SFA to acquire four symmetric views, sufficient neutron transmission can be achieved to assay a SFA. In this approach multiple scan information for the same pins may also be unfolded to potentially allow the determination of plutonium for sub-regions of the assembly. For a 17 ? 17 pressurized water reactor SFA, a simplistic preliminary

  20. Nonproliferation and safeguards aspects of fuel cycle programs in reduction of excess separated plutonium and high-enriched uranium

    SciTech Connect

    Persiani, P.J.

    1995-06-01

    The purpose of this preliminary investigation is to explore alternatives and strategies aimed at the gradual reduction of the excess inventories of separated plutonium and high-enriched uranium (HEU) in the civilian nuclear power industry. The study attempts to establish a technical and economic basis to assist in the formation of alternative approaches consistent with nonproliferation and safeguards concerns. Reference annual mass flows and inventories for a representative 1,400 Mwe Pressurized Water Reactor (PWR) fuel cycle have been investigated for three cases: the 100 percent uranium oxide UO{sub 2} fuel loading once through cycle, and the 33 percent mixed oxide MOX loading configuration for a first and second plutonium recycle. The analysis addresses fuel cycle developments; plutonium and uranium inventory and flow balances; nuclear fuel processing operations; UO{sub 2} once-through and MOX first and second recycles; and the economic incentives to draw-down the excess separated plutonium stores. The preliminary analysis explores several options in reducing the excess separated plutonium arisings and HEU, and the consequences of the interacting synergistic effects between fuel cycle processes and isotopic signatures of nuclear materials on nonproliferation and safeguards policy assessments.

  1. Characteristics of Spent Fuel from Plutonium Disposition Reactors, Vol. 1: The Combustion Engineering System 80+ Pressurized-Water-Reactor Design

    SciTech Connect

    Murphy, B.D.

    1993-01-01

    This report discusses a simulation study of the burnup of mixed-oxide fuel in a Combustion Engineering System 80+ Pressurized-Water Reactor. The mixed oxide was composed of uranium and plutonium oxides where the plutonium was of weapons-grade composition. The study was part of the Fissile Materials Disposition Program that considered the possibility of fueling commercial reactors with weapons plutonium. The isotopic composition of the spent fuel is estimated at various times following discharge. Actinides and all significant fission products are considered. The activities, decay-heat values, and gamma-ray fluxes associated with the spent fuel are also discussed. It is clear from the analysis that following discharge the plutonium is no longer of weapons-grade composition. The characteristics of the mixed-oxide fuel at various times following discharge indicate its behavior under long-term storage. As a counterpoint to the mixed-oxide fuel case, the situation with a similar reactor fueled with uranium oxide alone is analyzed. The comparisons serve to emphasize the significance of the plutonium as part of the fuel. For the mixed-oxide case, the burnup was 42,200 MWd/MTHM; in the pure-uranium case, it was 47,800 MWd/MTHM.

  2. Novel drug delivery systems for actinides (uranium and plutonium) decontamination agents.

    PubMed

    Fattal, Elias; Tsapis, Nicolas; Phan, Guillaume

    2015-08-01

    The possibility of accidents in the nuclear industry or of nuclear terrorist attacks makes the development of new decontamination strategies crucial. Among radionuclides, actinides such as uranium and plutonium and their different isotopes are considered as the most dangerous contaminants, plutonium displaying mostly a radiological toxicity whereas uranium exhibits mainly a chemical toxicity. Contamination occurs through ingestion, skin or lung exposure with subsequent absorption and distribution of the radionuclides to different tissues where they induce damaging effects. Different chelating agents have been synthesized but their efficacy is limited by their low tissue specificity and high toxicity. For these reasons, several groups have developed smart delivery systems to increase the local concentration of the chelating agent or to improve its biodistribution. The aim of this review is to highlight these strategies.

  3. 16. VIEW OF GLOVE BOX WORKSTATIONS WITHIN THE PLUTONIUM BUTTON ...

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

    16. VIEW OF GLOVE BOX WORKSTATIONS WITHIN THE PLUTONIUM BUTTON BREAKOUT ROOM. (9/82) - Rocky Flats Plant, Plutonium Recovery Facility, Northwest portion of Rocky Flats Plant, Golden, Jefferson County, CO

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

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

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

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

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

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

  6. 17. VIEW OF THE FIRST PLUTONIUM BUTTON PRODUCED FROM THE ...

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

    17. VIEW OF THE FIRST PLUTONIUM BUTTON PRODUCED FROM THE BUILDING 371 AQUEOUS RECOVERY OPERATION. (9/30/83) - Rocky Flats Plant, Plutonium Recovery Facility, Northwest portion of Rocky Flats Plant, Golden, Jefferson County, CO

  7. Magnetic excitations in plutonium monoantimonide

    SciTech Connect

    Lander, G.H.; Stirling, W.G.; Mignod, J.R.; Spirlet, J.C.; Rebezant, J.; Vogt, O.

    1985-01-01

    Neutron inelastic scattering studies of uranium compounds have illustrated the complexity of the interactions in this part of periodic table. Recently, large crystals of plutonium compounds have been grown at the Transuranium Institute, and we report here the first neutron inelastic scattering on PuSb. A monodomain sample of ferromagnetic PuSb was prepared by cooling in a field with H vector parallel to (001). We observe an almost dispersionless magnetic transition, assigned to arise within the GAMMA/sub 8/ ground state, with an energy of 4.3 THz. Surprisingly, the lowest frequency (3.5 THz) excitation occurs at the zone boundary, with a polarization along the wavevector. Theoretical predictions give the spin-wave gap and GAMMA/sub 8/-GAMMA/sub 7/ crystal field splitting (> 12 THz experimentally), but are presently unable to explain the lifting of the degeneracy of the longitudinal and transverse modes and the minimum of the former at the zone boundary. 7 refs., 3 figs.

  8. PROCESS OF ELIMINATING HYDROGEN PEROXIDE IN SOLUTIONS CONTAINING PLUTONIUM VALUES

    DOEpatents

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

    1960-09-27

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

  9. COLUMBIC OXIDE ADSORPTION PROCESS FOR SEPARATING URANIUM AND PLUTONIUM IONS

    DOEpatents

    Beaton, R.H.

    1959-07-14

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

  10. Dispersion of plutonium from contaminated pond sediments

    USGS Publications Warehouse

    Rees, T.F.; Cleveland, J.M.; Carl, Gottschall W.

    1978-01-01

    Sediment-water distributions of plutonium as a function of pH and contact time are investigated in a holding pond at the Rocky Flats plant of the Department of Energy. Although plutonium has been shown to sorb from natural waters onto sediments, the results of this study indicate that under the proper conditions it can be redispersed at pH 9 and above. Concentrations greater than 900 pCi Pu/L result after 34 h contact at pH 11 or 12 and the distribution coefficient, defined as the ratio of concentration in the sediment to that in the liquid, decreases from 1.1 ?? 105 at pH 7 to 1.2 ?? 103 at pH 11. The plutonium is probably dispersed as discrete colloids or as hydrolytic species adsorbed onto colloidal sediment particles whose average size decreases with increasing pH above pH 9. About 5% of the total plutonium is dispersed at pH 12, and the dispersion seems to readsorb on the sediment with time. Consequently, migration of plutonium from the pond should be slow, and it would be difficult to remove this element completely from pond sediment by leaching with high pH solutions. ?? 1978 American Chemical Society.

  11. Plutonium Chemistry in the UREX+ Separation Processes

    SciTech Connect

    ALena Paulenova; George F. Vandegrift, III; Kenneth R. Czerwinski

    2009-10-01

    The project "Plutonium Chemistry in the UREX+ Separation Processes” is led by Dr. Alena Paulenova of Oregon State University under collaboration with Dr. George Vandegrift of ANL and Dr. Ken Czerwinski of the University of Nevada at Las Vegas. The objective of the project is to examine the chemical speciation of plutonium in UREX+ (uranium/tributylphosphate) extraction processes for advanced fuel technology. Researchers will analyze the change in speciation using existing thermodynamics and kinetic computer codes to examine the speciation of plutonium in aqueous and organic phases. They will examine the different oxidation states of plutonium to find the relative distribution between the aqueous and organic phases under various conditions such as different concentrations of nitric acid, total nitrates, or actinide ions. They will also utilize techniques such as X-ray absorbance spectroscopy and small-angle neutron scattering for determining plutonium and uranium speciation in all separation stages. The project started in April 2005 and is scheduled for completion in March 2008.

  12. 15. VIEW OF THE SAFE GEOMETRY PLUTONIUM METAL STORAGE PALLETS ...

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

    15. VIEW OF THE SAFE GEOMETRY PLUTONIUM METAL STORAGE PALLETS FROM THE INSIDE OF AN INPUT-OUTPUT STATION. INDIVIDUAL CONTAINERS OF PLUTONIUM ARE STORED IN THE WATER-FILLED, DOUBLE-WALLED STAINLESS STEEL TUBES THAT ARE WELDED ONTO THE PALLETS. (12/3/88) - Rocky Flats Plant, Plutonium Recovery Facility, Northwest portion of Rocky Flats Plant, Golden, Jefferson County, CO

  13. 10 CFR 71.88 - Air transport of plutonium.

    Code of Federal Regulations, 2014 CFR

    2014-01-01

    ... 10 Energy 2 2014-01-01 2014-01-01 false Air transport of plutonium. 71.88 Section 71.88 Energy... Controls and Procedures § 71.88 Air transport of plutonium. (a) Notwithstanding the provisions of any... citation of 49 CFR chapter I, as may be applicable, the licensee shall assure that plutonium in any...

  14. 10 CFR 71.63 - Special requirement for plutonium shipments.

    Code of Federal Regulations, 2014 CFR

    2014-01-01

    ... 10 Energy 2 2014-01-01 2014-01-01 false Special requirement for plutonium shipments. 71.63 Section... MATERIAL Package Approval Standards § 71.63 Special requirement for plutonium shipments. Shipments containing plutonium must be made with the contents in solid form, if the contents contain greater than...

  15. VIEW OF THE INTERIOR OF THE PLUTONIUM LABORATORY IN BUILDING ...

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

    VIEW OF THE INTERIOR OF THE PLUTONIUM LABORATORY IN BUILDING 559. THE LABORATORY WAS USED TO ANALYZE THE PURITY OF PLUTONIUM. PLUTONIUM SAMPLES WERE CONTAINED WITHIN GLOVE BOXES - Rocky Flats Plant, Chemical Analytical Laboratory, North-central section of Plant, Golden, Jefferson County, CO

  16. 10 CFR 71.63 - Special requirement for plutonium shipments.

    Code of Federal Regulations, 2012 CFR

    2012-01-01

    ... 10 Energy 2 2012-01-01 2012-01-01 false Special requirement for plutonium shipments. 71.63 Section... MATERIAL Package Approval Standards § 71.63 Special requirement for plutonium shipments. Shipments containing plutonium must be made with the contents in solid form, if the contents contain greater than...

  17. 10 CFR 71.63 - Special requirement for plutonium shipments.

    Code of Federal Regulations, 2011 CFR

    2011-01-01

    ... 10 Energy 2 2011-01-01 2011-01-01 false Special requirement for plutonium shipments. 71.63 Section... MATERIAL Package Approval Standards § 71.63 Special requirement for plutonium shipments. Shipments containing plutonium must be made with the contents in solid form, if the contents contain greater than...

  18. 10 CFR 71.63 - Special requirement for plutonium shipments.

    Code of Federal Regulations, 2010 CFR

    2010-01-01

    ... 10 Energy 2 2010-01-01 2010-01-01 false Special requirement for plutonium shipments. 71.63 Section... MATERIAL Package Approval Standards § 71.63 Special requirement for plutonium shipments. Shipments containing plutonium must be made with the contents in solid form, if the contents contain greater than...

  19. 10 CFR 71.63 - Special requirement for plutonium shipments.

    Code of Federal Regulations, 2013 CFR

    2013-01-01

    ... 10 Energy 2 2013-01-01 2013-01-01 false Special requirement for plutonium shipments. 71.63 Section... MATERIAL Package Approval Standards § 71.63 Special requirement for plutonium shipments. Shipments containing plutonium must be made with the contents in solid form, if the contents contain greater than...

  20. 10 CFR 71.88 - Air transport of plutonium.

    Code of Federal Regulations, 2011 CFR

    2011-01-01

    ... 10 Energy 2 2011-01-01 2011-01-01 false Air transport of plutonium. 71.88 Section 71.88 Energy... Controls and Procedures § 71.88 Air transport of plutonium. (a) Notwithstanding the provisions of any... citation of 49 CFR chapter I, as may be applicable, the licensee shall assure that plutonium in any...

  1. Electrochemical investigation into the mechanism of plutonium reduction in electrorefining

    SciTech Connect

    McCurry, L.E.; Moy, G.M.M.

    1987-01-01

    Currently impure plutonium metal is purified at Los Alamos National Laboratory by a molten salt electrorefining process. Electrorefining is an effective method for producing high-purity plutonium metal (> 99.95%). In general this process involves the oxidation of impure plutonium metal from a molten plutonium anode or a solvent metal/plutonium anode, transport of plutonium ions through a molten salt electrolyte, and reduction of the plutonium ions at a tungsten cathode to pure plutonium metal. Purification of the plutonium metal from impurities is based on the difference in free energies of formation between the various metallic impurities associated with plutonium. To obtain a better understanding of the overall electrorefining process and its inefficiencies, an electrochemical investigation into the mechanism for plutonium reduction in a typical electrorefining environment was undertaken. Cyclic voltammetry was selected as the method for determining the electrode mechanism for plutonium reduction at tungsten electrodes. In addition to the standard electrorefining melt (equimolar NaCl-KCl), additional melts that were being investigated in our solvent anode work were also investigated. With insight gained from this investigation, it was hoped that a better selection of electrorefining operating parameters could be obtained.

  2. OVERVIEW OF CALORIMETRIC ASSAY OF PLUTONIUM IN THE UNITED STATES

    SciTech Connect

    Rudy, C. R.

    2001-01-01

    Calorimetry is a primary measurement technique for assay of quantities of plutonium in the United States. It is the most accurate NDA technique for many forms of plutonium-bearing materials. This paper provides an overview of the use of calorimetry in combination with high-resolution gamma-ray spectroscopy for accurate plutonium mass determinations.

  3. Treatment of accidental intakes of plutonium and americium: guidance notes.

    PubMed

    Ménétrier, F; Grappin, L; Raynaud, P; Courtay, C; Wood, R; Joussineau, S; List, V; Stradling, G N; Taylor, D M; Bérard, Ph; Morcillo, M A; Rencova, J

    2005-06-01

    The scientific basis for the treatment of the contamination of the human body by plutonium, americium and other actinides is reviewed. Guidance Notes are presented for the assistance of physicians and others who may be called upon to treat workers or members of the public who may become contaminated internally with inhaled plutonium nitrate, plutonium tributyl phosphate, americium nitrate or americium oxide.

  4. Plutonium AMS measurements in Yangtze River estuary sediment

    NASA Astrophysics Data System (ADS)

    Tims, S. G.; Pan, S. M.; Zhang, R.; Fifield, L. K.; Wang, Y. P.; Gao, J. H.

    2010-04-01

    The Yangtze River is the largest single source of sediment to the continental shelf of the East China Sea. The quantity of material exported by the river is expected to decrease substantially as a consequence of an extensive continuing program of dam construction within the river catchment. We report here AMS measurements of plutonium isotope concentrations and ratios for selected depth increments from a sediment core, collected from the sub-aqueous delta of the Yangtze River estuary. The Pu derives from atmospheric nuclear weapons testing in the 1950s and 1960s, and is potentially a useful tracer of sediment deposition times in the marine environment. The results show considerable structure in the depth-concentration profile, and offer an excellent opportunity to compare Pu with the more commonly used 137Cs isotopic tracer. The AMS data show superior sensitivity and indicate that the 240Pu/ 239Pu ratio can provide a check on the deposition dates. The changes in the 240Pu and 239Pu concentrations and the 240Pu/ 239Pu ratios with sediment depth all indicate the possibility of using Pu as a geochronological tool for coastal sediment studies.

  5. Characterization of Delta Phase Plutonium Metal

    SciTech Connect

    Rudisill, T.S.

    2000-09-21

    The FB-Line facility has developed the capability to recast plutonium metal using an M-18 reduction furnace with a new casting chamber. Plutonium metal is recast by charging a standard FB-Line magnesia crucible and placing the charge in the casting chamber. The loaded casting chamber is raised into the M-18 reduction furnace and sealed against the furnace head using a copper gasket following the same procedure used for a bomb reduction run. The interior volume of the chamber is evacuated and backfilled with argon gas. The M-18 motor-generator set is used to heat the surface of the casting chamber to nominally 750 Degrees C. Within about 2 hr, the plutonium metal reaches its melting temperature of approximately 640 Degrees C.

  6. Excess plutonium disposition using ALWR technology

    SciTech Connect

    Phillips, A.; Buckner, M.R.; Radder, J.A.; Angelos, J.G.; Inhaber, H.

    1993-02-01

    The Office of Nuclear Energy of the Department of Energy chartered the Plutonium Disposition Task Force in August 1992. The Task Force was created to assess the range of practicable means of disposition of excess weapons-grade plutonium. Within the Task Force, working groups were formed to consider: (1) storage, (2) disposal,and(3) fission options for this disposition,and a separate group to evaluate nonproliferation concerns of each of the alternatives. As a member of the Fission Working Group, the Savannah River Technology Center acted as a sponsor for light water reactor (LWR) technology. The information contained in this report details the submittal that was made to the Fission Working Group of the technical assessment of LWR technology for plutonium disposition. The following aspects were considered: (1) proliferation issues, (2) technical feasibility, (3) technical availability, (4) economics, (5) regulatory issues, and (6) political acceptance.

  7. Method for dissolving delta-phase plutonium

    DOEpatents

    Karraker, David G.

    1992-01-01

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

  8. The United States Plutonium Balance, 1944 - 2009

    SciTech Connect

    2012-06-01

    This report updates the report -Plutonium: The first 50 years- which was released by the U.S.Department of Energy (DOE) in 1996. The topic of both reports is plutonium, sometimes referred to as Pu-239, which is capable of sustaining a nuclear chain reaction and is used in nuclear weapons and for nuclear power production. This report updates 1994 data through 2009. The four most significant changes since 1994 include: (a) the completion of cleanup activities at the Rocky Flats Plant in 2005; (b) material consolidation and disposition activities, especially shipments from Hanford to the Savannah River Site; (c) the 2007 declaration of an additional 9.0 MT of weapons grade plutonium to be surplus to defense needs in the coming decades; and (d) the opening of the Waste Isolation Pilot Plant (WIPP) near Carlsbad, New Mexico in 1999.

  9. Excess plutonium disposition using ALWR technology

    SciTech Connect

    Phillips, A.; Buckner, M.R.; Radder, J.A.; Angelos, J.G.; Inhaber, H.

    1993-02-01

    The Office of Nuclear Energy of the Department of Energy chartered the Plutonium Disposition Task Force in August 1992. The Task Force was created to assess the range of practicable means of disposition of excess weapons-grade plutonium. Within the Task Force, working groups were formed to consider: (1) storage, (2) disposal,and(3) fission options for this disposition,and a separate group to evaluate nonproliferation concerns of each of the alternatives. As a member of the Fission Working Group, the Savannah River Technology Center acted as a sponsor for light water reactor (LWR) technology. The information contained in this report details the submittal that was made to the Fission Working Group of the technical assessment of LWR technology for plutonium disposition. The following aspects were considered: (1) proliferation issues, (2) technical feasibility, (3) technical availability, (4) economics, (5) regulatory issues, and (6) political acceptance.

  10. Excess plutonium disposition: The deep borehole option

    SciTech Connect

    Ferguson, K.L.

    1994-08-09

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

  11. Interaction of divalent plutonium and curium

    SciTech Connect

    Mikheev, N.B.; Kazakevich, M.Z.; Rumer, I.A.

    1988-11-01

    It has been established that at plutonium concentrations ranging from 10/sup -5/ to 10/sup -4/ mole % the oxidation potentials of the Pu/sup 3 +//Pu/sup 2 +/ and Cm/sup 3 +//Cm/sup 2 +/ pairs increased by 0.15-0.2 V due to the dimerization of Pu/sup 2 +/ and the formation of mixed dimers of plutonium and curium. Promethium(2+) does not have a similar ability to form mixed dimers owing to the fact that Pm/sup 2 +/ does not have a free d electron. The oxidation potential of the Pm/sup 3 +//Pm/sup 2 +/ pair does not vary in the presence of massive quantities of plutonium

  12. Disposition of plutonium in deep boreholes

    SciTech Connect

    Halsey, W.G.; Jardine, L.J.; Walter, C.E.

    1995-05-01

    Substantial inventories of excess plutonium are expected to result from dismantlement of U.S. and Russian nuclear weapons. Disposition of this material should be a high priority in both countries. A variety of disposition options are under consideration. One option is to place the plutonium either directly or in an immobilized form at the bottom of a deep borehole that is then sealed. Deep-borehole disposition involves placing plutonium several kilometers deep into old, stable, rock formations that have negligible free water present. Containment assurance is based on the presence of ancient groundwater indicating lack of migration and communication with the biosphere. Recovery would be extremely difficult (costly) and impossible to accomplish clandestinely.

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

    DOEpatents

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

    1962-07-10

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

  14. Study of the formation, prevention, and recovery of plutonium from plutonium esters in the Purex process

    SciTech Connect

    Gray, L. W.; Burney, G. A.

    1981-01-01

    The Savannah River Plant uses the basic Purex process to separate /sup 239/Pu from /sup 238/U and fission products. Dark-brown, dense solids containing up to 30% Pu have previously occurred in rotameters in the plutonium finishing operations. The kinetics of formation of this mixture of DBP- and MBP-Pu esters suggest two methods to prevent the formation of the solids. A selective dissolution method using NaOH metathesis has been developed to separate the phosphate ester from the plutonium before dissolution of the residual plutonium hydroxide in a HNO/sub 3/-HF medium.

  15. Alternating layers of plutonium and lead or indium as surrogate for plutonium

    SciTech Connect

    Rudin, Sven Peter

    2009-01-01

    Elemental plutonium (Pu) assumes more crystal structures than other elements, plausibly due to bonding f electrons becoming non-bonding. Complex geometries hamper understanding of the transition in Pu, but calculations predict this transition in a system with simpler geometry: alternating layers either of plutonium and lead or of plutonium and indium. Here the transition occurs via a pairing-up of atoms within Pu layers. Calculations stepping through this pairing-up reveal valuable details of the transition, for example that the transition from bonding to non-bonding proceeds smoothly.

  16. Plutonium Speciation, Solubilization, and Migration in soils

    SciTech Connect

    Neu, Mary; Haire, Richard G.

    1999-06-01

    The DOE is currently conducting cleanup activities at its nuclear weapons development sites, many of which have accumulated plutonium in soils for 50 years. To properly control Pu migration in soils within Federal sites and onto public lands, better evaluate the public risk, and design effective remediation strategies, a fundamental understanding of Pu speciation and environmental transport, and release mechanisms is needed. The key scientific goals of this project are: to determine Pu concentrations and speciation at a contaminated DOE site; to study the formation, stability, and structural and spectroscopic features of environmentally relevant Pu species; to determine the mechanism(s) of interaction between Pu and Mn/Fe minerals and the potential release of Pu via redox cycling; and to model the environmental behavior of plutonium. Our long-term goal is to use characterization, thermodynamic, mineral interaction, and mobility data to develop better models of radionuclide transport and risk assessment, and to enable the development of science-based decontamination strategies. This research will fill important gaps between basic actinide science and the problems impeding site clean-up, plutonium disposition, and accurate risk assessment. Information gained will allow for the development of technologies and clean-up approaches targeting particular plutonium contaminants and improved assessment of risks associated with actinide migration, site remediation, and decontamination. By combining very specific study of plutonium at the Rocky Flats Environmental Test Site (RFETS), a well characterized contaminated site, with laboratory studies on the most important plutonium and mineral component systems, we will provide essential knowledge of contaminant characteristics and distinguish critical geochemical processes and mechanisms.

  17. CHARACTERIZATION OF SURPLUS PLUTONIUM FOR DISPOSITION OPTIONS

    SciTech Connect

    Allender, J; Edwin Moore, E; Scott Davies, S

    2008-07-15

    The United States (U.S.) has identified 61.5 metric tons (MT) of plutonium that is permanently excess to use in nuclear weapons programs, including 47.2 MT of weapons-grade plutonium. Except for materials that remain in use for programs outside of national defense, including programs for nuclear-energy development, the surplus inventories will be stored safely by the Department of Energy (DOE) and then transferred to facilities that will prepare the plutonium for permanent disposition. Some items will be disposed as transuranic waste, low-level waste, or spent fuel. The remaining surplus plutonium will be managed through: (1) the Mixed Oxide (MOX) Fuel Fabrication Facility (FFF), to be constructed at the Savannah River Site (SRS), where the plutonium will be converted to fuel that will be irradiated in civilian power reactors and later disposed to a high-level waste (HLW) repository as spent fuel; (2) the SRS H-Area facilities, by dissolving and transfer to HLW systems, also for disposal to the repository; or (3) alternative immobilization techniques that would provide durable and secure disposal. From the beginning of the U.S. program for surplus plutonium disposition, DOE has sponsored research to characterize the surplus materials and to judge their suitability for planned disposition options. Because many of the items are stored without extensive analyses of their current chemical content, the characterization involves three interacting components: laboratory sample analysis, if available; non-destructive assay data; and rigorous evaluation of records for the processing history for items and inventory groups. This information is collected from subject-matter experts at inventory sites and from materials stabilization and surveillance programs, in cooperation with the design agencies for the disposition facilities. This report describes the operation and status of the characterization program.

  18. Modeling of Diffusion of Plutonium in Other Metals and of Gaseous Species in Plutonium-Based Systems

    SciTech Connect

    Bernard R. Cooper; Gayanath W. Fernando; S. Beiden; A. Setty; E.H. Sevilla

    2004-07-02

    Establish standards for temperature conditions under which plutonium, uranium, or neptunium from nuclear wastes permeates steel, with which it is in contact, by diffusion processes. The primary focus is on plutonium because of the greater difficulties created by the peculiarities of face-centered-cubic-stabilized (delta) plutonium (the form used in the technology generating the waste).

  19. REVIEW OF PLUTONIUM OXIDATION LITERATURE

    SciTech Connect

    Korinko, P.

    2009-11-12

    A brief review of plutonium oxidation literature was conducted. The purpose of the review was to ascertain the effect of oxidation conditions on oxide morphology to support the design and operation of the PDCF direct metal oxidation (DMO) furnace. The interest in the review was due to a new furnace design that resulted in oxide characteristics that are different than those of the original furnace. Very little of the published literature is directly relevant to the DMO furnace operation, which makes assimilation of the literature data with operating conditions and data a convoluted task. The oxidation behavior can be distilled into three regimes, a low temperature regime (RT to 350 C) with a relatively slow oxidation rate that is influenced by moisture, a moderate temperature regime (350-450 C) that is temperature dependent and relies on more or less conventional oxidation growth of a partially protective oxide scale, and high temperature oxidation (> 500 C) where the metal autocatalytically combusts and oxidizes. The particle sizes obtained from these three regimes vary with the finest being from the lowest temperature. It is surmised that the slow growth rate permits significant stress levels to be achieved that help break up the oxides. The intermediate temperatures result in a fairly compact scale that is partially protective and that grows to critical thickness prior to fracturing. The growth rate in this regime may be parabolic or paralinear, depending on the oxidation time and consequently the oxide thickness. The high temperature oxidation is invariant in quiescent or nearly quiescent conditions due to gas blanketing while it accelerates with temperature under flowing conditions. The oxide morphology will generally consist of fine particles (<15 {micro}m), moderately sized particles (15 < x < 250 {micro}m) and large particles (> 250 {micro}m). The particle size ratio is expected to be < 5%, 25%, and 70% for fine, medium and large particles, respectively, for

  20. Dehydration of plutonium or neptunium trichloride hydrate

    DOEpatents

    Foropoulos, J. Jr.; Avens, L.R.; Trujillo, E.A.

    1992-03-24

    A process is described for preparing anhydrous actinide metal trichlorides of plutonium or neptunium by reacting an aqueous solution of an actinide metal trichloride selected from the group consisting of plutonium trichloride or neptunium trichloride with a reducing agent capable of converting the actinide metal from an oxidation state of +4 to +3 in a resultant solution, evaporating essentially all the solvent from the resultant solution to yield an actinide trichloride hydrate material, dehydrating the actinide trichloride hydrate material by heating the material in admixture with excess thionyl chloride, and recovering anhydrous actinide trichloride.

  1. Dehydration of plutonium or neptunium trichloride hydrate

    DOEpatents

    Foropoulos, Jr., Jerry; Avens, Larry R.; Trujillo, Eddie A.

    1992-01-01

    A process of preparing anhydrous actinide metal trichlorides of plutonium or neptunium by reacting an aqueous solution of an actinide metal trichloride selected from the group consisting of plutonium trichloride or neptunium trichloride with a reducing agent capable of converting the actinide metal from an oxidation state of +4 to +3 in a resultant solution, evaporating essentially all the solvent from the resultant solution to yield an actinide trichloride hydrate material, dehydrating the actinide trichloride hydrate material by heating the material in admixture with excess thionyl chloride, and recovering anhydrous actinide trichloride is provided.

  2. Waste measurements at a plutonium facility

    SciTech Connect

    Wachter, J.R.

    1992-01-01

    Solid plutonium contaminated wastes are often highly heterogeneous, span a wide range of chemical compositions and matrix types, and are packaged in a variety of container sizes. NDA analysis of this waste depends on operator knowledge of these parameters so that proper segregation, instrument selection, quality assurance, and uncertainty estimation can take place. This report describes current waste measurement practices and uncertainty estimates at a US plutonium scrap recovery facility and presents a program for determining reproducibility and bias in NDA measurements. Following this, an operator's perspective on desirable NDA upgrades is offered.

  3. Method of isotope separation by chemi-ionization

    DOEpatents

    Wexler, Sol; Young, Charles E.

    1977-05-17

    A method for separating specific isotopes present in an isotopic mixture by aerodynamically accelerating a gaseous compound to form a jet of molecules, and passing the jet through a stream of electron donor atoms whereby an electron transfer takes place, thus forming negative ions of the molecules. The molecular ions are then passed through a radiofrequency quadrupole mass filter to separate the specific isotopes. This method may be used for any compounds having a sufficiently high electron affinity to permit negative ion formation, and is especially useful for the separation of plutonium and uranium isotopes.

  4. SEPARATION OF PLUTONIUM FROM LANTHANUM BY CHELATION-EXTRACTION

    DOEpatents

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

    1958-12-01

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

  5. Plutonium dispersal in fires: Summary of what is known

    SciTech Connect

    Condit, R.H.

    1993-07-01

    In view of the great public apprehension about plutonium and nuclear weapons we should explore ways to prevent, limit, or mitigate possible plutonium dispersals. This review is primarily a tutorial on what is known about plutonium dispersal in fires. It concludes that in most types of fires involving plutonium the amount released will not be an immediate danger to life. Indeed, in many cases very few personnel will receive more than the lung burden allowed by current regulations for plutonium workers. However, the dangers may be significant in special situations, unusual terrains, certain meteorological conditions, and very high burn temperatures.

  6. Plutonium and uranium contamination in soils from former nuclear weapon test sites in Australia

    NASA Astrophysics Data System (ADS)

    Child, D. P.; Hotchkis, M. A. C.

    2013-01-01

    The British government performed a number of nuclear weapon tests on Australian territory from 1952 through to 1963 with the cooperation of the Australian government. Nine fission bombs were detonated in South Australia at Emu Junction and Maralinga, and a further three fission weapons were detonated in the Monte Bello Islands off the coast of Western Australia. A number of soil samples were collected by the Australian Radiation Laboratories in 1972 and 1978 during field surveys at these nuclear weapon test sites. They were analysed by gamma spectrometry and, for a select few samples, by alpha spectrometry to measure the remaining activities of fission products, activation products and weapon materials. We have remeasured a number of these Montebello Islands and Emu Junction soil samples using the ANTARES AMS facility, ANSTO. These samples were analysed for plutonium and uranium isotopic ratios and isotopic concentrations. Very low 240Pu/239Pu ratios were measured at both sites (∼0.05 for Alpha Island and ∼0.02 for Emu Field), substantially below global fallout averages. Well correlated but widely varying 236U and plutonium concentrations were measured across both sites, but 233U did not correlate with these other isotopes and instead showed correlation with distance from ground zero, indicating in situ production in the soils.

  7. Detailed Destructive Post-Irradiation Examinations of Mixed Uranium and Plutonium Oxide Fuel

    SciTech Connect

    Delashmitt, Jeffrey {Jeff} S; Keever, Tamara {Tammy} Jo; Smith, Rob R; Hexel, Cole R; Ilgner, Ralph H

    2010-01-01

    The United States Department of Energy (DOE) Fissile Materials Disposition Program (FMDP) is pursuing disposal of surplus weapons-usable plutonium by reactor irradiation as the fissile constituent of MOX fuel. Lead test assemblies (LTAs) have been irradiated for approximately 36 months in Duke Energy's Catawba-1 nuclear power plant (NPP). Per the mixed oxide (MOX) fuel topical report, approved by the U.S. Nuclear Regulatory Commission (NRC), destructive post-irradiation examinations (PIEs) are to be performed on second cycle rods (irradiated to an average burnup of approximately 45 GWd/MTHM). The Radiochemical Analysis Group (RAG) at Oak Ridge National Laboratory (ORNL) is currently performing the detailed destructive post-irradiation examinations (PIE) on four of the mixed uranium and plutonium oxide fuel rods. The analytical process involves dissolution of designated fuel segments in a shielded hot cell for high precision quantification of select fission products and actinide isotopes employing isotope dilution mass spectrometry (IDMS) among other analyses. The hot cell dissolution protocol to include the collection and subsequent alkaline fusion digestion of the fuel's acid resistant metallic particulates will be presented. Although the IDMS measurements of the fission products and actinide isotopes will not be completed by the time of the 51st INMM meeting, the setup and testing of the HPLC chromatographic separations in preparation for these measurements will be discussed.

  8. Using magnetization measurements to detect small amounts of plutonium hydride formation in plutonium metal

    SciTech Connect

    Kim, Jae Wook; Mielke, Charles H.; Zapf, Vivien; Baiardo, Joseph P.; Mitchell, Jeremy N.; Richmond, Scott; Schwartz, Daniel S.; Mun, Eun D.; Smith, Alice Iulia

    2014-10-20

    We report the formation of plutonium hydride in 2 at % Ga-stabilized δ-Pu, with 1 atomic % H charging. We show that magnetization measurements are a sensitive, quantitative measure of ferromagnetic plutonium hydride against the nonmagnetic background of plutonium. It was previously shown that at low hydrogen concentrations, hydrogen forms super-abundant vacancy complexes with plutonium, resulting in a bulk lattice contraction. Here we use magnetization, X-ray and neutron diffraction measurements to show that in addition to forming vacancy complexes, at least 30% of the H atoms bond with Pu to precipitate PuHx, largely on the surface of the sample with x ~ 1.9. We observe magnetic hysteresis loops below 40 K with magnetic remanence, consistent with precipitates of ferromagnetic PuH1.9.

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

    SciTech Connect

    Jardine, L J; Borisov, G B

    2004-07-21

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

  10. Weapons-grade plutonium dispositioning. Volume 2: Comparison of plutonium disposition options

    SciTech Connect

    Brownson, D.A.; Hanson, D.J.; Blackman, H.S.

    1993-06-01

    The Secretary of Energy requested the National Academy of Sciences (NAS) Committee on International Security and Arms Control to evaluate disposition options for weapons-grade plutonium. The Idaho National Engineering Laboratory (INEL) offered to assist the NAS in this evaluation by investigating the technical aspects of the disposition options and their capability for achieving plutonium annihilation levels greater than 90%. This report was prepared for the NAS to document the gathered information and results from the requested option evaluations. Evaluations were performed for 12 plutonium disposition options involving five reactor and one accelerator-based systems. Each option was evaluated in four technical areas: (1) fuel status, (2) reactor or accelerator-based system status, (3) waste-processing status, and (4) waste disposal status. Based on these evaluations, each concept was rated on its operational capability and time to deployment. A third rating category of option costs could not be performed because of the unavailability of adequate information from the concept sponsors. The four options achieving the highest rating, in alphabetical order, are the Advanced Light Water Reactor with plutonium-based ternary fuel, the Advanced Liquid Metal Reactor with plutonium-based fuel, the Advanced Liquid Metal Reactor with uranium-plutonium-based fuel, and the Modular High Temperature Gas-Cooled Reactor with plutonium-based fuel. Of these four options, the Advanced Light Water Reactor and the Modular High Temperature Gas-Cooled Reactor do not propose reprocessing of their irradiated fuel. Time constraints and lack of detailed information did not allow for any further ratings among these four options. The INEL recommends these four options be investigated further to determine the optimum reactor design for plutonium disposition.

  11. Adsorption of plutonium oxide nanoparticles.

    PubMed

    Schmidt, Moritz; Wilson, Richard E; Lee, Sang Soo; Soderholm, L; Fenter, P

    2012-02-07

    Adsorption of monodisperse cubic plutonium oxide nanoparticles ("Pu-NP", [Pu(38)O(56)Cl(x)(H(2)O)(y)]((40-x)+), with a fluorite-related lattice, approximately 1 nm in edge size) to the muscovite (001) basal plane from aqueous solutions was observed in situ (in 100 mM NaCl background electrolyte at pH 2.6). Uptake capacity of the surface quantified by α-spectrometry was 0.92 μg Pu/cm(2), corresponding to 10.8 Pu per unit cell area (A(UC)). This amount is significantly larger than that of Pu(4+) needed for satisfying the negative surface charge (0.25 Pu(4+) for 1 e(-)/A(UC)). The adsorbed Pu-NPs cover 17% of the surface area, determined by X-ray reflectivity (XR). This correlates to one Pu-NP for every 14 unit cells of muscovite, suggesting that each particle compensates the charge of the unit cells onto which it adsorbs as well as those in its direct proximity. Structural investigation by resonant anomalous X-ray reflectivity distinguished two different sorption states of Pu-NPs on the surface at two different regimes of distance from the surface. A fraction of Pu is distributed within 11 Å from the surface. The distribution width matches the Pu-NP size, indicating that this species represents Pu-NPs adsorbed directly on the surface. Beyond the first layer, an additional fraction of sorbed Pu was observed to extend more broadly up to more than 100 Å from the surface. This distribution is interpreted as resulting from "stacking" or aggregation of the nanoparticles driven by sorption and accumulation of Pu-NPs at the interface although these Pu-NPs do not aggregate in the solution. These results are the first in situ observation of the interaction of nanoparticles with a charged mineral-water interface yielding information important to understanding the environmental transport of Pu and other nanophase inorganic species.

  12. Design-Only Conceptual Design Report: Plutonium Immobilization Plant

    SciTech Connect

    DiSabatino, A.; Loftus, D.

    1999-01-01

    This design-only conceptual design report was prepared to support a funding request by the Department of Energy Office of Fissile Materials Disposition for engineering and design of the Plutonium Immobilization Plant, which will be used to immobilize up to 50 tonnes of surplus plutonium. The siting for the Plutonium Immobilization Plant will be determined pursuant to the site-specific Surplus Plutonium Disposition Environmental Impact Statement in a Plutonium Deposition Record of Decision in early 1999. This document reflects a new facility using the preferred technology (ceramic immobilization using the can-in-canister approach) and the preferred site (at Savannah River). The Plutonium Immobilization Plant accepts plutonium from pit conversion and from non-pit sources and, through a ceramic immobilization process, converts the plutonium into mineral-like forms that are subsequently encapsulated within a large canister of high-level waste glass. The final immobilized product must make the plutonium as inherently unattractive and inaccessible for use in nuclear weapons as the plutonium in spent fuel from commercial reactors and must be suitable for geologic disposal. Plutonium immobilization at the Savannah River Site uses: (1) A new building, the Plutonium Immobilization Plant, which will convert non-pit surplus plutonium to an oxide form suitable for the immobilization process, immobilize plutonium in a titanate-based ceramic form, place cans of the plutonium-ceramic forms into magazines, and load the magazines into a canister; (2) The existing Defense Waste Processing Facility for the pouring of high-level waste glass into the canisters; and (3) The Actinide Packaging and Storage Facility to receive and store feed materials. The Plutonium Immobilization Plant uses existing Savannah River Site infra-structure for analytical laboratory services, waste handling, fire protection, training, and other support utilities and services. The Plutonium Immobilization Plant

  13. Plutonium Immobilization Can Loading Equipment Review

    SciTech Connect

    Kriikku, E.; Ward, C.; Stokes, M.; Randall, B.; Steed, J.; Jones, R.; Hamilton, L.

    1998-05-01

    This report lists the operations required to complete the Can Loading steps on the Pu Immobilization Plant Flow Sheets and evaluates the equipment options to complete each operation. This report recommends the most appropriate equipment to support Plutonium Immobilization Can Loading operations.

  14. Overview of surplus weapons plutonium disposition

    SciTech Connect

    Rudy, G.

    1996-05-01

    The safe disposition of surplus weapons useable plutonium is a very important and urgent task. While the functions of long term storage and disposition directly relate to the Department`s weapons program and the environmental management program, the focus of this effort is particularly national security and nonproliferation.

  15. Recovery of Plutonium by Carrier Precipitation

    DOEpatents

    Goeckermann, R. H.

    1961-04-01

    The recovery of plutonium from an aqueous nitric acid Zr-containing solution of 0.2 to 1N acidity is accomplished by adding fluoride anions (1.5 to 5 mg/l), and precipitating the Pu with an excess of H/sub 2/0/sub 2/ at 53 to 65 deg C. (AEC)

  16. NNSS Soils Monitoring: Plutonium Valley (CAU366)

    SciTech Connect

    Miller, Julianne J.; Mizell, Steve A.; Nikolich, George; Campbell, Scott

    2012-02-01

    The U.S. Department of Energy (DOE) National Nuclear Security Administration (NNSA), Nevada Site Office (NSO), Environmental Restoration Soils Activity has authorized the Desert Research Institute (DRI) to conduct field assessments of potential sediment transport of contaminated soil from Corrective Action Unit (CAU) 366, Area 11 Plutonium Valley Dispersion Sites Contamination Area (CA) during precipitation runoff events.

  17. 233-S plutonium concentration facility hazards assessment

    SciTech Connect

    Broz, R.E.

    1994-12-19

    This document establishes the technical basis in support of Emergency Planning activities for the 233-S Plutonium Concentration Facility on the Hanford Site. The document represents an acceptable interpretation of the implementing guidance document for DOE ORDER 5500.3A. Through this document, the technical basis for the development of facility specific Emergency Action Levels and the Emergency Planning Zone is demonstrated.

  18. Heterogeneity Effects in Plutonium Contaminated Soil

    DTIC Science & Technology

    2009-03-01

    masses up to one kilogram once the ratio of Americium -241 (Am-241) and plutonium concentrations was established (Rademacher, 2001). Alpha...with a sample number and tared weight with a non-smearing marker. A standard control was then set using a point source of Americium -241 on an aluminum

  19. Regulatory issues for deep borehole plutonium disposition

    SciTech Connect

    Halsey, W.G.

    1995-03-01

    As a result of recent changes throughout the world, a substantial inventory of excess separated plutonium is expected to result from dismantlement of US nuclear weapons. The safe and secure management and eventual disposition of this plutonium, and of a similar inventory in Russia, is a high priority. A variety of options (both interim and permanent) are under consideration to manage this material. The permanent solutions can be categorized into two broad groups: direct disposal and utilization. The deep borehole disposition concept involves placing excess plutonium deep into old stable rock formations with little free water present. Issues of concern include the regulatory, statutory and policy status of such a facility, the availability of sites with desirable characteristics and the technologies required for drilling deep holes, characterizing them, emplacing excess plutonium and sealing the holes. This white paper discusses the regulatory issues. Regulatory issues concerning construction, operation and decommissioning of the surface facility do not appear to be controversial, with existing regulations providing adequate coverage. It is in the areas of siting, licensing and long term environmental protection that current regulations may be inappropriate. This is because many current regulations are by intent or by default specific to waste forms, facilities or missions significantly different from deep borehole disposition of excess weapons usable fissile material. It is expected that custom regulations can be evolved in the context of this mission.

  20. Electrochemically Modulated Separation for Plutonium Safeguards

    SciTech Connect

    Pratt, Sandra H.; Breshears, Andrew T.; Arrigo, Leah M.; Schwantes, Jon M.; Duckworth, Douglas C.

    2013-12-31

    Accurate and timely analysis of plutonium in spent nuclear fuel is critical in nuclear safeguards for detection of both protracted and rapid plutonium diversions. Gamma spectroscopy is a viable method for accurate and timely measurements of plutonium provided that the plutonium is well separated from the interfering fission and activation products present in spent nuclear fuel. Electrochemically modulated separation (EMS) is a method that has been used successfully to isolate picogram amounts of Pu from nitric acid matrices. With EMS, Pu adsorption may be turned "on" and "off" depending on the applied voltage, allowing for collection and stripping of Pu without the addition of chemical reagents. In this work, we have scaled up the EMS process to isolate microgram quantities of Pu from matrices encountered in spent nuclear fuel during reprocessing. Several challenges have been addressed including surface area limitations, radiolysis effects, electrochemical cell performance stability, and chemical interferences. After these challenges were resolved, 6 µg Pu was deposited in the electrochemical cell with approximately an 800-fold reduction of fission and activation product levels from a spent nuclear fuel sample. Modeling showed that these levels of Pu collection and interference reduction may not be sufficient for Pu detection by gamma spectroscopy. The main remaining challenges are to achieve a more complete Pu isolation and to deposit larger quantities of Pu for successful gamma analysis of Pu. If gamma analyses of Pu are successful, EMS will allow for accurate and timely on-site analysis for enhanced Pu safeguards.

  1. Plutonium Immobilization Can Loading Preliminary Specifications

    SciTech Connect

    Kriikku, E.

    1998-11-25

    This report discusses the Plutonium Immobilization can loading preliminary equipment specifications and includes a process block diagram, process description, equipment list, preliminary equipment specifications, plan and elevation sketches, and some commercial catalogs. This report identifies loading pucks into cans and backfilling cans with helium as the top priority can loading development areas.

  2. PLUTONIUM PURIFICATION PROCESS EMPLOYING THORIUM PYROPHOSPHATE CARRIER

    DOEpatents

    King, E.L.

    1959-04-28

    The separation and purification of plutonium from the radioactive elements of lower atomic weight is described. The process of this invention comprises forming a 0.5 to 2 M aqueous acidffc solution containing plutonium fons in the tetravalent state and elements with which it is normally contaminated in neutron irradiated uranium, treating the solution with a double thorium compound and a soluble pyrophosphate compound (Na/sub 4/P/sub 2/O/sub 7/) whereby a carrier precipitate of thorium A method is presented of reducing neptunium and - trite is advantageous since it destroys any hydrazine f so that they can be removed from solutions in which they are contained is described. In the carrier precipitation process for the separation of plutonium from uranium and fission products including zirconium and columbium, the precipitated blsmuth phosphate carries some zirconium, columbium, and uranium impurities. According to the invention such impurities can be complexed and removed by dissolving the contaminated carrier precipitate in 10M nitric acid, followed by addition of fluosilicic acid to about 1M, diluting the solution to about 1M in nitric acid, and then adding phosphoric acid to re-precipitate bismuth phosphate carrying plutonium.

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

    DOE PAGES

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

    2017-04-01

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

  4. In search of plutonium: A nonproliferation journey

    NASA Astrophysics Data System (ADS)

    Hecker, Siegfried

    2010-02-01

    In February 1992, I landed in the formerly secret city of Sarov, the Russian Los Alamos, followed a few days later by a visit to Snezhinsk, their Livermore. The briefings we received of the Russian nuclear weapons program and tours of their plutonium, reactor, explosives, and laser facilities were mind boggling considering the Soviet Union was dissolved only two months earlier. This visit began a 17-year, 41 journey relationship with the Russian nuclear complex dedicated to working with them in partnership to protect and safeguard their weapons and fissile materials, while addressing the plight of their scientists and engineers. In the process, we solved a forty-year disagreement about the plutonium-gallium phase diagram and began a series of fundamental plutonium science workshops that are now in their tenth year. At the Yonbyon reprocessing facility in January 2004, my North Korean hosts had hoped to convince me that they have a nuclear deterrent. When I expressed skepticism, they asked if I wanted to see their ``product.'' I asked if they meant the plutonium; they replied, ``Well, yes.'' Thus, I wound up holding 200 grams of North Korean plutonium (in a sealed glass jar) to make sure it was heavy and warm. So began the first of my six journeys to North Korea to provide technical input to the continuing North Korean nuclear puzzle. In Trombay and Kalpakkam a few years later I visited the Indian nuclear research centers to try to understand how India's ambitious plans for nuclear power expansion can be accomplished safely and securely. I will describe these and other attempts to deal with the nonproliferation legacy of the cold war and the new challenges ahead. )

  5. PLUTONIUM CONTAMINATION VALENCE STATE DETERMINATION USING X-RAY ABSORPTION FINE STRUCTURE PERMITS CONCRETE RECYCLE

    SciTech Connect

    Ervin, P. F.; Conradson, S. D.

    2002-02-25

    This paper describes the determination of the speciation of plutonium contamination present on concrete surfaces at the Rocky Flats Environmental Technology Site (RFETS). At RFETS, the plutonium processing facilities have been contaminated during multiple events over their 50 year operating history. Contamination has resulted from plutonium fire smoke, plutonium fire fighting water, milling and lathe operation aerosols, furnace operations vapors and plutonium ''dust'' diffusion.

  6. Isotope separation and advanced manufacturing technology

    NASA Astrophysics Data System (ADS)

    Carpenter, J.; Kan, T.

    This is the fourth issue of a semiannual report for the Isotope Separation and Advanced Materials Manufacturing (ISAM) Technology Program at Lawrence Livermore National Laboratory. Primary objectives include: (1) the Uranium Atomic Vapor Laser Isotope Separation (UAVLIS) process, which is being developed and prepared for deployment as an advanced uranium enrichment capability; (2) Advanced manufacturing technologies, which include industrial laser and E-beam material processing and new manufacturing technologies for uranium, plutonium, and other strategically important materials in support of DOE and other national applications. This report features progress in the ISAM Program from October 1993 through March 1994.

  7. Determination of plutonium metal origins

    SciTech Connect

    Moody, K.J.

    1995-02-01

    Forensic signatures are present in any Pu sample that can determine the sample`s origin: isotopic ratio of Pu, progeny species that grow into the sample, and contaminant species left over from incomplete purification of the Pu in fuel reprocessing. In the context of intelligence information, this can result in attribution of responsibility for the product of clandestine proliferant operations or material smuggled from existing stockpiles. A list of signature elements and what can be determined from them have been developed. Work needs to be done in converting concentrations of signature species into a quantitative forensic analysis, particularly in regard to reactor performance, but this should require only a small effort. A radiochemical analysis scheme has been developed for measuring these nuclides; more work is needed, particularly for determining fission product concentrations. A sample of Pu metal has been analyzed and several parameters determined that are strong indicators of its point of origin.

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

    PubMed

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

    2003-07-20

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

  9. Total Measurement Uncertainty for the Plutonium Finishing Plant (PFP) Segmented Gamma Scan Assay System

    SciTech Connect

    WESTSIK, G.A.

    2001-06-06

    This report presents the results of an evaluation of the Total Measurement Uncertainty (TMU) for the Canberra manufactured Segmented Gamma Scanner Assay System (SGSAS) as employed at the Hanford Plutonium Finishing Plant (PFP). In this document, TMU embodies the combined uncertainties due to all of the individual random and systematic sources of measurement uncertainty. It includes uncertainties arising from corrections and factors applied to the analysis of transuranic waste to compensate for inhomogeneities and interferences from the waste matrix and radioactive components. These include uncertainty components for any assumptions contained in the calibration of the system or computation of the data. Uncertainties are propagated at 1 sigma. The final total measurement uncertainty value is reported at the 95% confidence level. The SGSAS is a gamma assay system that is used to assay plutonium and uranium waste. The SGSAS system can be used in a stand-alone mode to perform the NDA characterization of a container, particularly for low to medium density (0-2.5 g/cc) container matrices. The SGSAS system provides a full gamma characterization of the container content. This document is an edited version of the Rocky Flats TMU Report for the Can Scan Segment Gamma Scanners, which are in use for the plutonium residues projects at the Rocky Flats plant. The can scan segmented gamma scanners at Rocky Flats are the same design as the PFP SGSAS system and use the same software (with the exception of the plutonium isotopics software). Therefore, all performance characteristics are expected to be similar. Modifications in this document reflect minor differences in the system configuration, container packaging, calibration technique, etc. These results are supported by the Quality Assurance Objective (QAO) counts, safeguards test data, calibration data, etc. for the PFP SGSAS system. Other parts of the TMU analysis utilize various modeling techniques such as Monte Carlo N

  10. Materials identification and surveillance project item evaluation. Item: Impure mixture of plutonium oxide and uranium oxide (PUUOXBC05)

    SciTech Connect

    Allen, T.; Appert, Q.; Davis, C.

    1997-06-01

    In this report Los Alamos researchers characterize properties relevant to storage of an impure mixture of plutonium oxide and uranium oxide (impure mixed oxide (MOX) that is composed of 43.8 mass % plutonium and 17.8 mass % uranium) in accordance with the department of Energy (DOE) standard DOE-STD-3013-96. This is the first sample of an impure mixture of plutonium oxide and uranium oxide to be evaluated by the materials identification and surveillance project. Methods used to characterize the mixture include mass loss-on-calcination measurements, mass loss-on-ignition (LOI) measurements, elemental analysis, plutonium and uranium isotopic analysis, particle analyses measurements, X-ray powder diffraction, thermal desorption mass spectrometry (TDMS), and surface-area analyses. LOI measurements show a steady decrease in magnitude as the calcining temperature is increased. In contrast, calcining at progressively increasing temperatures does not appear to significantly change the specific surface area of the impure MOX. The LOI value for the powder after final 950 C calcination is 0.4 mass %. Water and carbon dioxide are the major gaseous products formed at all temperatures.

  11. Neptunium as a Tool for Reducing Proliferation Risks with Plutonium: A Technical Analysis of its Efficiency and its Drawbacks

    SciTech Connect

    Greneche, Dominique; Ng, Selena; Guesdon, Bernard; Vinoche, Richard; Delpech, Marc; Golfier, Herve; Dolci, Florence; Poinot-Salanon, Christine

    2006-07-01

    Introducing neptunium into the nuclear fuel cycle has been proposed in the past as a way to impede the diversion or the direct use of plutonium to fabricate a nuclear explosive device. This paper aims to technically analyze the industrial consequences should this proposal be implemented. Two scenarios are considered: 1) adding neptunium to fresh uranium oxide (UOX) fuel before irradiation in a light water reactor; 2) separating neptunium together with plutonium from used UOX fuel and using this combined oxide to fabricate mixed oxide (MOX) fuel before subsequent irradiation in a light water reactor. In both cases, assembly calculations for a pressurized water reactor using fresh fuel doped with neptunium are presented for a wide range of neptunium proportions. Consequences on core and fuel performances and the fuel cycle are analyzed. These are weighed against the potential proliferation resistance benefits of adding neptunium due to the increased quantity of the plutonium isotope {sup 238}Pu in the discharged fuel, or due to the potentially increased detectability through gamma ray emissions of a plutonium-neptunium oxide mixture. Finally, the proliferation risk presented by neptunium itself is discussed. (authors)

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

    DOEpatents

    Faris, B.F.

    1961-04-25

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

  13. Process modeling of plutonium conversion and MOX fabrication for plutonium disposition

    SciTech Connect

    Schwartz, K. L.

    1998-10-01

    Two processes are currently under consideration for the disposition of 35 MT of surplus plutonium through its conversion into fuel for power production. These processes are the ARIES process, by which plutonium metal is converted into a powdered oxide form, and MOX fuel fabrication, where the oxide powder is combined with uranium oxide powder to form ceramic fuel. This study was undertaken to determine the optimal size for both facilities, whereby the 35 MT of plutonium metal will be converted into fuel and burned for power. The bounding conditions used were a plutonium concentration of 3-7%, a burnup of 20,000-40,000 MWd/MTHM, a core fraction of 0.1 to 0.4, and the number of reactors ranging from 2-6. Using these boundary conditions, the optimal cost was found with a plutonium concentration of 7%. This resulted in an optimal throughput ranging from 2,000 to 5,000 kg Pu/year. The data showed minimal costs, resulting from throughputs in this range, at 3,840, 2,779, and 3,497 kg Pu/year, which results in a facility lifetime of 9.1, 12.6, and 10.0 years, respectively.

  14. Plutonium disposition via immobilization in ceramic or glass

    SciTech Connect

    Gray, L.W.; Kan, T.; Shaw, H.F.; Armantrout, A.

    1997-03-05

    The management of surplus weapons plutonium is an important and urgent task with profound environmental, national, and international security implications. In the aftermath of the Cold War, Presidential Policy Directive 13, and various analyses by renown scientific, technical, and international policy organizations have brought about a focused effort within the Department of Energy to identify and implement paths for the long term disposition of surplus weapons- usable plutonium. The central goal of this effort is to render surplus weapons plutonium as inaccessible and unattractive for reuse in nuclear weapons as the much larger and growing stock of plutonium contained in spent fuel from civilian reactors. One disposition option being considered for surplus plutonium is immobilization, in which the plutonium would be incorporated into a glass or ceramic material that would ultimately be entombed permanently in a geologic repository for high-level waste.

  15. The production and certification of a plutonium equal-atom reference material: NBL CRM 128

    SciTech Connect

    Crawford, D.W. . Office of Safeguards and Security); Gradle, C.G.; Soriano, M.D. )

    1990-07-01

    This report describes the design, production, and certification of the New Brunswick Laboratory plutonium equal-atom certified reference material (CRM), NBL CRM 128. The primary use of this CRM is for the determination of bias corrections encountered in the operation of a mass spectrometer. This reference material is available to the US Department of Energy contractor-operated and government-operated laboratories, as well as to the international nuclear safeguards community. The absolute, or unbiased, certified value for the CRM's Pu-242/Pu-239 ratio is 1.00063 {plus minus} 0.00026 (95% confidence interval) as of October 1, 1984. This value was obtained through the quantitative blending of high-purity, chemically and isotopically characterized separated isotopes, as well as through intercomparisons of CRM samples with calibration mixtures using thermal ionization mass spectrometry. 32 tabs.

  16. Improved Radiation Dosimetry/Risk Estimates to Facilitate Environmental Management of Plutonium-Contaminated Sites

    SciTech Connect

    Scott, Bobby R.; Tokarskaya, Zoya B.; Zhuntova, Galina V.; Osovets, Sergey V.; Syrchikov, Victor A., Belyaeva, Zinaida D.

    2007-12-14

    This report summarizes 4 years of research achievements in this Office of Science (BER), U.S. Department of Energy (DOE) project. The research described was conducted by scientists and supporting staff at Lovelace Respiratory Research Institute (LRRI)/Lovelace Biomedical and Environmental Research Institute (LBERI) and the Southern Urals Biophysics Institute (SUBI). All project objectives and goals were achieved. A major focus was on obtaining improved cancer risk estimates for exposure via inhalation to plutonium (Pu) isotopes in the workplace (DOE radiation workers) and environment (public exposures to Pu-contaminated soil). A major finding was that low doses and dose rates of gamma rays can significantly suppress cancer induction by alpha radiation from inhaled Pu isotopes. The suppression relates to stimulation of the body's natural defenses, including immunity against cancer cells and selective apoptosis which removes precancerous and other aberrant cells.

  17. Plutonium speciation in water from Mono Lake, California

    USGS Publications Warehouse

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

    1983-01-01

    The solubility of plutonium in Mono Lake water is enhanced by the presence of large concentrations of indigenous carbonate ions and moderate concentrations of fluoride ions. In spite of the complex chemical composition of this water, only a few ions govern the behavior of plutonium, as demonstrated by the fact that it was possible to duplicate plutonium speciation in a synthetic water containing only the principal components of Mono Lake water.

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

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

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

  19. SEPARATION OF PLUTONIUM FROM AQUEOUS SOLUTIONS BY ION-EXCHANGE

    DOEpatents

    Schubert, J.

    1958-06-01

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

  20. Spectrophotometers for plutonium monitoring in HB-line

    SciTech Connect

    Lascola, R. J.; O'Rourke, P. E.; Kyser, E. A.; Immel, D. M.; Plummer, J. R.; Evans, E. V.

    2016-02-12

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