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Sample records for plutonium isotopes

  1. The radiological hazard of plutonium isotopes and specific plutonium mixtures

    SciTech Connect

    Heindel, G.; Clow, J.; Inkret, W.; Miller, G.

    1995-11-01

    The US Department of Energy defines the hazard categories of its nuclear facilities based upon the potential for accidents to have significant effects on specific populations and the environment. In this report, the authors consider the time dependence of hazard category 2 (significant on-site effects) for facilities with inventories of plutonium isotopes and specific weapons-grade and heat-source mixtures of plutonium isotopes. The authors also define relative hazard as the reciprocal of the hazard category 2 threshold value and determine its time dependence. The time dependence of both hazard category 2 thresholds and relative hazards are determined and plotted for 10,000 years to provide useful information for planning long-term storage or disposal facilities.

  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

    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. PMID:23565016

  4. 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

  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. Plutonium Isotopic Gamma-Ray Analysis

    Energy Science and Technology Software Center (ESTSC)

    1992-01-08

    The MGA8 (Multiple Group Analysis) program determines the relative abundances of plutonium and other actinide isotopes in different materials. The program analyzes spectra taken of such samples using a 4096-channel germanium (Ge) gamma-ray spectrometer. The code can be run in a one or two detector mode. The first spectrum, which is required and must be taken at a gain of 0.075 Kev/channel with a high resolution planar detector, contains the 0-300 Kev energy region. Themore » second spectrum, which is optional, must be taken at a gain of 0.25 Kev/channel; it becomes important when analyzing high burnup samples (concentration of Pu241 greater than one percent). Isotopic analysis precisions of one percent or better can be obtained, and no calibrations are required. The system also measures the abundances of U235, U238, Np237, and Am241. A special calibration option is available to perform a one-time peak-shape characterization when first using a new detector system.« less

  7. Isotopic Measurements: Interpretation and Implications of Plutonium Data

    SciTech Connect

    Luksic, Andrzej T.; Collins, Brian A.; Friese, Judah I.; Schwantes, Jon M.; Starner, Jason R.; Wacker, John F.

    2010-08-11

    One of the fundamental activities within the field of nuclear forensics is the laboratory analysis of nuclear material; one aspect is providing the isotopic composition of the material under investigation. For both plutonium and uranium, this includes a unique suite of isotopes that, individually and collectively (i.e. an isotopic vector), will help characterize these materials, and potentially provide insight into their mode of production, intended utilization, and processing history. A full understanding of how this information is used provides the basis for defining the need for these measurements and helps determine the precision and accuracy requirements for those measurements. This paper provides an overview of this process as it applies to plutonium, discussing how reactor design and operating parameters can impact the resultant plutonium vector, thereby giving us the ability to infer those reactor traits based on isotopic measurements.

  8. 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.

  9. 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

    2016-01-01

    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., (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. PMID:26898531

  10. 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.

  11. Determination of plutonium isotopic composition by gamma-ray spectroscopy

    SciTech Connect

    Sampson, T.E.; Hsue, S.T.; Parker, J.L.; Johnson, S.S.; Bowersox, D.F.

    1981-01-01

    We discuss the general approach, computerized data analysis methods, and results of measurements used to determine the isotopic composition of plutonium by gamma-ray spectroscopy. The simple techniques are designed to be applicable to samples of arbitrary size, geometry, age, chemical, and isotopic composition. The combination of the gamma spectroscopic measurement of isotopic composition coupled with calorimetric measurement of total sample power is shown to give a totally nondestructive determination of sample plutonium mass with a precision of 0.6% for 1000-g samples of PuO/sub 2/ with 12% /sup 240/Pu content. The precision of isotopic measurements depends upon many factors, including sample size, sample geometry, and isotopic content. Typical ranges are found to be /sup 238/Pu, 1 to 10%; /sup 239/Pu, 0.1 to 0.5%; /sup 240/Pu, 2 to 5%; /sup 241/Pu, 0.3 to 0.7%; /sup 242/Pu (determined by isotopic correlation); and /sup 241/Am, 0.2 to 10%.

  12. 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.

  13. PC/FRAM plutonium isotopic analysis of CdTe gamma-ray spectra

    NASA Astrophysics Data System (ADS)

    Vo, D. T.; Russo, P. A.

    2002-07-01

    This paper reports the results of isotopics measurements of plutonium with the new CdTe gamma-ray spectrometer. These are the first wide-range plutonium gamma-ray isotopics analysis results obtained with other than germanium spectrometers. The CdTe spectrometer measured small plutonium reference samples in reasonable count times, covering the range from low to high burnup. The complete experimental hardware included the new, commercial, portable CdTe detector and two commercial portable multichannel analyzers. Version 4 of FRAM is the software that performed the isotopics analysis.

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

    PubMed

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

    2014-12-01

    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. PMID:25350948

  15. 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)

  16. RAPID FUSION METHOD FOR DETERMINATION OF PLUTONIUM ISOTOPES IN LARGE RICE SAMPLES

    SciTech Connect

    Maxwell, S.

    2013-03-01

    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.

  17. An isotopic analysis system for plutonium samples enriched in sup 238 Pu

    SciTech Connect

    Ruhter, W.D.; Camp, D.C.

    1991-08-01

    We have designed and built a gamma-ray spectrometer system that measures the relative plutonium isotopic abundances of plutonium oxide enriched in {sup 238}Pu. The first system installed at Westinghouse Savannah River Company was tested and evaluated on plutonium oxide in stainless steel EP60/61 containers. {sup 238}Pu enrichments ranged from 20% to 85%. Results show that 200 grams of plutonium oxide in an EP60.61 container can be measured with {plus minus}0.3% precision and better than {plus minus}1.0% accuracy in the specific power using a counting time of 50 minutes. 3 refs., 2 figs.

  18. 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.

  19. Evaluation of TASTEX task H: measurement of plutonium isotopic abundances by gamma-ray spectrometry

    SciTech Connect

    Gunnink, R.; Prindle, A.L.; Asakura, Y.; Masui, J.; Ishiguro, N.; Kawasaki, A.; Kataoka, S.

    1981-10-01

    This report describes a computer-based gamma spectrometer system that was developed for measuring isotopic and total plutonium concentrations in nitric acid solutions. The system was installed at the Tokai reprocessing plant where it is undergoing testing and evaluation as part of the Tokai Advanced Safeguards Exercise (TASTEX). Objectives of TASTEX Task H, High-Resolution Gamma Spectrometer for Plutonium Isotopic Analysis, the methods and equipment used, the installation and calibration of the system, and the measurements obtained from several reprocessing campaigns are discussed and described. In general, we find that measurements for gamma spectroscopy agree well with those of mass spectrometry and of other chemical analysis. The system measures both freshly processed plutonium from the product accountability tank and aged plutonium solutions from storage tanks. 14 figures, 15 tables.

  20. 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.

  1. 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

  2. Determination of plutonium isotopes in low activity waste of NPP origin

    NASA Astrophysics Data System (ADS)

    Nikiforova, A.; Taskaeva, I.; Veleva, B.; Valova, Tz.; Slavchev, B.; Dimitrova, D.

    2006-01-01

    The inventory analysis of the alkaline low level liquid radioactive waste collected during more than 30 years of NPP “Kozloduy” operation requires determination of eighteen radioactive isotopes with different decay properties. Plutonium isotopes of interest are Pu-238, Pu-239/Pu-240, and Pu-242. The preliminary investigations of the supernatant phase of model and authentic waste samples showed essential challenges for determination of plutonium due to its various oxidation states and low concentration in the complex matrix. Plutonium concentration was determined in precipitate and supernatant after the calcium phosphate precipitation and in the different fractions of the anion exchange steps. The separation by anion exchange and final purification of plutonium fraction by extraction chromatography on TEVA resin (EiChroM Industries) was studied by variation of plutonium oxidation states. The sources were prepared by micro precipitation with NdF3 and counted by alpha spectrometry. As a result from the performed experiments, plutonium determination procedure was optimized and applied to real waste samples.

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

    PubMed

    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. Graphical Abstract ᅟ. PMID:27032649

  4. 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.

    2016-03-01

    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.

  5. 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.

  6. Testing the plutonium isotopic analysis code FRAM with various CdTe detectors.

    SciTech Connect

    Vo, Duc T.; Russo, P. A.

    2002-01-01

    The isotopic analysis code Fixed-energy Response-function Analysis with Multiple efficiency (FRAM)1,2 has been proven to successfully analyze plutonium spectra taken with a portable CdTe detector with Peltier cooling, the first results of this kind for a noncryogenic detector.3 These are the first wide-range plutonium gamma-ray isotopics analysis results obtained with other than Ge spectrometers. The CdTe spectrometer measured small plutonium reference samples in reasonable count times, covering the range from low to high burnup. This paper describes further testing of FRAM with two CdTe detectors of different sizes and resolutions using different analog and digital, portable multichannel analyzers (MCAs).

  7. 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.

  8. 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.

  9. Plutonium isotopic assay from alpha spectroscopy: A progress report

    SciTech Connect

    Baran, D.T.

    1995-12-31

    The Non-Destructive Assay (NDA) group at New Brunswick Laboratory (NBL) continues to develop and refine a computer program ALPHAFIT, a sophisticated peak-fitting routine for use in determining the isotopic abundances of Pu and U samples. The program uses up to seven parameters per peak fit and up to 12 peaks per region of interest to de-convolute typical complicated Pu a spectra. Preliminary results show decent fits for major peaks in the spectrum and calculated isotopic abundances of the major isotopes to {+-} 4%.

  10. 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.

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

    DOE PAGESBeta

    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. 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

  12. 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.

  13. 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. PMID:16856723

  14. 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.

  15. 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.

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

    NASA Astrophysics Data System (ADS)

    Bays, Samuel Eugene

    2008-10-01

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

  17. 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.

  18. 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.

  19. 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

    2015-02-01

    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. PMID:25535652

  20. 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. PMID:25014620

  1. 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. PMID:16124281

  2. 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. PMID:23683959

  3. Isotopic analysis of single uranium and plutonium particles by chemical treatment and mass spectrometry

    NASA Astrophysics Data System (ADS)

    Shinonaga, T.; Esaka, F.; Magara, M.; Klose, D.; Donohue, D.

    2008-11-01

    The isotopic composition of single uranium and plutonium particles was measured with an inductively coupled plasma mass spectrometer (ICP-MS) and a thermal ionization mass spectrometer (TIMS). Particles deposited on a carbon planchet were first analyzed with an energy dispersive X-ray spectrometer (EDX) attached to a scanning electron microscope (SEM) and then transferred on to a silicon wafer using a manipulator. The particle on the silicon wafer was dissolved with nitric acid and the isotopic ratios of U and Pu were measured with ICP-MS and TIMS. The results obtained by both methods for particles of certified reference materials showed good agreement with the certified values within the expected uncertainty. The measurement uncertainties obtained in this study were similar for both mass spectrometric methods. This study was performed to establish the method of particle analysis with SEM, EDX, the particle manipulation and chemical preparation technique, and the measurement of isotopic ratios of U and Pu in a single particle by mass spectrometry.

  4. Isotope ratio measurements of pg-size plutonium samples using TIMS in combination with "multiple ion counting" and filament carburization

    NASA Astrophysics Data System (ADS)

    Jakopic, Rozle; Richter, Stephan; Kühn, Heinz; Benedik, Ljudmila; Pihlar, Boris; Aregbe, Yetunde

    2009-01-01

    A sample preparation procedure for isotopic measurements using thermal ionization mass spectrometry (TIMS) was developed which employs the technique of carburization of rhenium filaments. Carburized filaments were prepared in a special vacuum chamber in which the filaments were exposed to benzene vapour as a carbon supply and carburized electrothermally. To find the optimal conditions for the carburization and isotopic measurements using TIMS, the influence of various parameters such as benzene pressure, carburization current and the exposure time were tested. As a result, carburization of the filaments improved the overall efficiency by one order of magnitude. Additionally, a new "multi-dynamic" measurement technique was developed for Pu isotope ratio measurements using a "multiple ion counting" (MIC) system. This technique was combined with filament carburization and applied to the NBL-137 isotopic standard and samples of the NUSIMEP 5 inter-laboratory comparison campaign, which included certified plutonium materials at the ppt-level. The multi-dynamic measurement technique for plutonium, in combination with filament carburization, has been shown to significantly improve the precision and accuracy for isotopic analysis of environmental samples with low-levels of plutonium.

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

    DOE PAGESBeta

    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 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

  6. 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.

  7. 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. PMID:27450248

  8. 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.

  9. 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.

  10. 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. PMID:25479434

  11. Rapid, quantitative analysis of americium, curium and plutonium isotopes in Hanford samples using extraction chromatography and precipitation plating

    SciTech Connect

    Kaye, J.H.; Strebin, R.S.; Orr, R.D.

    1994-04-01

    Recently developed methods for the rapid, quantitative analysis of americium (Am), curium (Cm), and plutonium (Pu) isotopes in Hanford soil, sludge, and waste-tank samples are described. After dissolution, dilutions are made as necessary based on alpha-energy analysis of a small aliquot of the original solution. isotopic tracers are then added and Am-Cm and Pu are separated by extraction chromatography, coprecipitated with neodymium fluoride, and counted. Examples of alpha spectra are given, and results obtained for Hanford sludge samples are presented.

  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. Cesium, americium and plutonium isotopes in ground level air of vilnius

    NASA Astrophysics Data System (ADS)

    Lujaniene, G.; Šapolaite, J.; Remeikis, V.; Lujanas, V.; Jermolajev, A.; Aninkevičius, V.

    2006-01-01

    Systematic observations of radionuclide composition and concentration in the atmosphere have been carried out at the Institute of Physics in Vilnius since 1963. Increases in activity concentration of radionuclides in the atmosphere were observed after nuclear weapon tests and the Chernobyl NPP accident. At present the radiation situation in Lithuania is determined by two main sources of radionuclides, forest fire and resuspension products transferred from highly polluted region of the Ukraine and Belarus. The activity concentrations of 137Cs were measured in two to three days samples while plutonium and americium in monthly samples. The extremely high activity concentrations of 238Pu, 239,240Pu, 241Am determined in the atmosphere during the Chernobyl accident can be explained by transport of “hot particles” of different composition. Activity concentration in 1995 2003 of 241Am and 239,240Pu isotopes ranged from 0.3 to 500 and from 1 to 500 nBq/m3, respectively. 238Pu/239,240Pu activity ratio in measured samples differs from 0.03 to 0.45. A decrease in 240Pu/239Pu atomic ratio from 0.30 to 0.19 was observed in 1995 2003.

  14. Optimized Chemical Separation and Measurement by TE TIMS Using Carburized Filaments for Uranium Isotope Ratio Measurements Applied to Plutonium Chronometry.

    PubMed

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

    2016-06-21

    An optimized method is described for U/Pu separation and subsequent measurement of the amount contents of uranium isotopes by total evaporation (TE) TIMS with a double filament setup combined with filament carburization for age determination of plutonium samples. The use of carburized filaments improved the signal behavior for total evaporation TIMS measurements of uranium. Elevated uranium ion formation by passive heating during rhenium signal optimization at the start of the total evaporation measurement procedure was found to be a result from byproducts of the separation procedure deposited on the filament. This was avoided using carburized filaments. Hence, loss of sample before the actual TE data acquisition was prevented, and automated measurement sequences could be accomplished. Furthermore, separation of residual plutonium in the separated uranium fraction was achieved directly on the filament by use of the carburized filaments. Although the analytical approach was originally tailored to achieve reliable results only for the (238)Pu/(234)U, (239)Pu/(235)U, and (240)Pu/(236)U chronometers, the optimization of the procedure additionally allowed the use of the (242)Pu/(238)U isotope amount ratio as a highly sensitive indicator for residual uranium present in the sample, which is not of radiogenic origin. The sample preparation method described in this article has been successfully applied for the age determination of CRM NBS 947 and other sulfate and oxide plutonium samples. PMID:27240571

  15. 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.

  16. 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.

  17. The MGA code for the determination of the isotopic composition of plutonium and MOX by gamma spectrometry — A performance study

    NASA Astrophysics Data System (ADS)

    Abousahl, S.; Michiels, A.; Bickel, M.; Gunnink, R.; Verplancke, J.

    1996-01-01

    Plutonium is a special nuclear material which must be accurately measured and accounted for, both with respect to mass and isotopic composition. The MGA code for evaluation of plutonium gamma spectra has been tested in this work with respect to its dependence on various instrumental and sample parameters. Results show that the code is generally reliable under the tested conditions. Recommendations for the equipment to be applied are given.

  18. 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.

  19. 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.

  20. 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.

  1. 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.

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

    SciTech Connect

    Ruhter, W.D.; DeWitt, K.W.; Pederson, K.B.; Watkins, J.A.

    1990-06-01

    This hardware manual is addressed to Savannah River Site supervisors and to authorized mechanical and electrical maintenance and service personnel. 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 Pu-238 isotopic analysis system. Chapter 2 lists major components of the system and includes electronic block and wiring diagrams. Commercial nuclear instrument modules and their required settings are described in Chapter 3. Chapter 4 contains service and preventive maintenance procedures, as well as a troubleshooting log. In Chapter 5 is a list of spare parts and all relevant mechanical drawings for the system. Chapter 6 contains reference articles. 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, troubleshooting, and maintenance of this commercial equipment. 31 figs., 1 tab.

  3. 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.

  4. 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

  5. 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. PMID:24401459

  6. 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

  7. 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.

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

    DOE PAGESBeta

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

  9. 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.

  10. 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.

  11. 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.

  12. 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

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

    PubMed

    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 (129m)Te, (131)I, (134)Cs, (136)Cs and (137)Cs 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 (241)Pu/(239+240)Pu (> 100) from the Fukushima DNPP accident highlights the need for long-term (241)Pu dose assessment, and the ingrowth of (241)Am. The results are important for the estimation of reactor damage and have significant implication in the strategy of decontamination. PMID:22403743

  14. 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.

  15. Presence of plutonium isotopes, 239Pu and 240Pu, in soils from Chile

    NASA Astrophysics Data System (ADS)

    Chamizo, E.; García-León, M.; Peruchena, J. I.; Cereceda, F.; Vidal, V.; Pinilla, E.; Miró, C.

    2011-12-01

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

  16. Trawsfynydd Plutonium Estimate

    SciTech Connect

    Reid, Bruce D.; Gerlach, David C.; Heasler, Patrick G.; Livingston, J.

    2009-11-20

    Report serves to document an estimate of the cumulative plutonium production of the Trawsfynydd Unit II reactor (Traws II) over its operating life made using the Graphite Isotope Ratio Method (GIRM). The estimate of the plutonium production in Traws II provided in this report has been generated under blind conditions. In other words, the estimate ofthe Traws II plutonium production has been generated without the knowledge of the plutonium production declared by the reactor operator (Nuclear Electric). The objective of this report is to demonstrate that the GIRM can be employed to serve as an accurate tool to verify weapons materials production declarations.

  17. 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.

  18. 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.

  19. 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. PMID:18270417

  20. 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.

  1. 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.

  2. 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.

  3. Portable computer to reduce gamma-ray spectra for plutonium isotopic ratios

    SciTech Connect

    Ruhter, W.D.; Camp, D.C.

    1981-05-15

    In response to Task A.63 of the International Safeguards Project Office (ISPO), to upgrade measurement technology used by the International Atomic Energy Agency (IAEA), a portable data-reduction microprocessor was designed and programmed which allows in-field reduction of gamma-ray spectra and interfaces with the IAEA's multichannel analyzers - the 1000 or 2000-channel memory Silena BS27/N. This report describes the components used in assembling the microprocessor unit: hardware, software used to control the unit, and the mathematical formulation used to obtain isotopic ratios from the gamma-ray data. A simple overview is presented of the unit's operation and the results of tests on gamma-ray spectra that sought to verify the unit's operating characteristics and to determine the precision and effectiveness of the software developed for data reduction.

  4. 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. PMID:21950768

  5. 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.

  6. 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.

  7. 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.

  8. 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. PMID:21709507

  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 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.

  10. 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.

  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. A case of wound intake of plutonium isotopes and 241Am in a human: application and improvement of the NCRP wound model.

    PubMed

    Schadilov, Anatoly E; Belosokhov, Maxim V; Levina, Elena S

    2010-10-01

    Plutonium isotopes (239Pu and 238Pu, and 241Am) with a total activity of 269 kBq were accidentally deposited in a puncture wound of the right index finger of a nuclear worker at the Mayak Production Association. Tissues surrounding the wound site contaminated with radionuclides were excised 4.5 h after the injury. Residual contamination within the wound amounted to 0.05% of the initial contamination. The 10-d therapy with CaNa3-diethylene triamine pentaacetate acid (CaNa3-DTPA) was performed in parallel with in vivo measurements of the wound site and daily urine bioassays. The wound intake of radionuclides was consistent with two forms of radioactive materials detected within the wound site, i.e., soluble compounds and a large fragment, which was completely removed by excision. On day 9 after the injury, the clearance rate from the wound site was 1.8 times higher than the rate predicted by the National Council on Radiation Protection and Measurements (NCRP) model for soluble compounds of plutonium and americium. The NCRP model parameters of transfer rates from the colloid and intermediate state (CIS) into soluble, and particles, aggregates and bound state (PABS) compartments were modified to eliminate any difference. As a result, a difference between the observed wound site radionuclide content and the value predicted by the modified wound model did not exceed 14% up to 9 days after the injury. For a longer period from 7 to 24 months, the value predicted by the modified model was consistent with results of the corresponding in vivo measurements. The treatment reduced the effective dose (50 years) from internal exposure by at least 480 times. The dose estimated (without accounting for a contribution of exposure dose to the regional lymph nodes draining the wound site) did not exceed 11 mSv. PMID:20838099

  13. 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.

  14. 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

  15. Predicted discharge plutonium isotopics for LEU [low-enriched uranium] test pebble irradiated in the AVR [Arbeitsgemeinschaft Versuchsreaktor

    SciTech Connect

    Lane, R.K.; Lefler, W.L.

    1988-06-01

    A Subprogram Plan related to the Arbeitsgemeinschaft Versuchsreaktor (AVR) Test Program is in place and describes cooperative work being carried out under the United States/Federal Republic of Germany (US/FRG) Implementing Agreement for Cooperation in Gas-Cooled Reactor Development. The AVR information to be provided as described in the plan will provide a basis for examining the accuracy of computational methods used for performance and safety analysis. The purpose of the cooperation is to obtain experimental information from the AVR relevant to the performance and safety of modular gas-cooled reactors, and to compare measured results with predictions of analytical tools. This report provides a progress report on the prediction of plutonium buildup in LEU fuel in a high-enriched uranium (HEU) core and also describes the method for calculating the U-238 resonance integral (cross section). 4 refs., 5 figs., 11 tabs.

  16. Determination of plutonium-239, thorium-232, and natural uranium isotopic concentrations in biological samples using photofission track analysis

    NASA Astrophysics Data System (ADS)

    Parry, James Roswell

    Fission track analysis (FTA) has many uses in the scientific community including but not limited to geological dating, neutron flux mapping, and dose reconstruction. The common method of fission for FTA is through neutrons from a nuclear reactor. This dissertation investigates the use of bremsstrahlung radiation produced from an electron linear accelerator to induce fission in FTA samples. This provides a means of simultaneously measuring the amount of Pu-239, U-nat, and Th-232 in a single sample. The benefit of measuring the three isotopes simultaneously is the possible elimination of costly and time consuming chemical processing for dose reconstruction samples. Samples containing the three isotopes were irradiated in two different bremsstrahlung spectra and a neutron spectrum to determine the amount of Pu-239, U-nat, and Th-232 in the samples. The reaction rate from the calibration samples and the counted fission tracks on the samples were used in determining the concentration of each isotope in the samples. The results were accurate to within a factor of two or three, showing that the method can work to predict the concentrations of multiple isotopes in a sample. The limitations of current accelerators and detectors limits the application of this specific procedure to higher concentrations of isotopes. The method detection limits for Pu-239, U-nat, and Th-232 are 20 pCi, 1 fCi, and 0.4 flCI respectively. Analysis of extremely low concentrations of isotopes would require the use of different detectors such as quartz due to the embrittlement encountered in the Lexan at high exposures. Cracking of the Texan detectors started to appear at a fluence of about 2 x 1018 electrons from the accelerator. This may be partly due to the beam stop not being an adequate thickness. The procedure is likely limited to specialty applications for the near term. However, with the world concerns of exposure to depleted uranium, this procedure may find applications in this area since

  17. 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

  18. 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. PMID:19804923

  19. 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.

  20. 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.

  1. In-plant measurements of gamma-ray transmissions for precise K-edge and passive assay of plutonium concentration and isotopic fractions in product solutions. Final report on TASTEX Task G

    SciTech Connect

    Russo, P.A.; Hsue, S.T.; Sprinkle, J.K. Jr.; Johnson, S.S.; Asakura, Y.; Kondo, I.; Masui, J.; Shoji, K.

    1982-08-01

    An instrument based upon high-resolution gamma-ray measurements has been tested for more than 1 year at the Tokai Reprocessing Facility for determination of plutonium concentration by K-edge absorption densitometry and for determination of plutonium isotopic fractions by transmission-corrected passive gamma-ray spectrometry. The nondestructive assay instrument was designed and built at Los Alamos National Laboratory for the Tokai Advanced Safeguards Technology Exercise (TASTEX). It was used at Tokai for the timely assay of more than 100 product solution samples during the TASTEX evaluations. The results were compared to reference values obtained by conventional destructive analysis of these samples. The precision and accuracy of plutonium concentrations measured by the K-edge technique are shown to be within 0.6% (1delta) in these applications. The precisions and accuracies of the isotopic fractions determined by these passive gamma-ray methods are shown to be within 0.4% for /sup 239/Pu, 1% for /sup 240/Pu and /sup 241/Pu, and 10% for /sup 242/Pu.

  2. Considerations in the Application of Multiple Ion Counting for the Trace Analysis of Plutonium and Uranium Isotope Ratios Using Thermal Ionization and Inductively-Coupled Plasma Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Riciputi, L. R.

    2008-12-01

    The use of simultaneous multiple-ion counting for the analysis of small samples of plutonium and uranium has been investigated using three different instruments, the ThermoElectron Neptune inductively-coupled plasma mass spectrometer, the ThermoElectron Triton thermal ionization mass spectrometer, and the Isotopex Iso-T thermal ionization mass spectrometer. The Neptune and Triton instruments utilize identical multiple ion counter arrays, with ions impinging directly on the channeltron surface. The Isotopex instruments utilize a different style of channeltron detector. The most significant difference in the Isotopex detectors is the presence of a conversion dynode at the entrance to the channeltron. Results suggest that the performance of the ThermoElectron MIC system varies between the Neptune and Triton instruments, which probably reflects both differences in the inherent characteristics of plasma and thermal sources and the performance of the MICS themselves. Differences in performance and stability between the '"naked"' and conversion dynode equipped channeltrons on the two thermal ionization instruments support these observations. These differences suggest that different analytical approaches to calibration of the multiple-ion counters may be required. Differences in potential analytical strategies employing multiple ion counters on the different instruments, including calibration schemes, precision and accuracy limits, and analytical strategies that can be employed, will be discussed. Results from both thermal ionization and inductively-coupled plasma sources suggest that the dominant source of uncertainty in isotope ratio measurement using multiple ion counting shifts from counting limitations for very small signals to uncertainties in gain calibration and detector drift among the ion counters at higher count rates. These characteristics place limits on the applicability of multiple ion counters; results from mixed Faraday/multiple ion counting analysis will

  3. 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

  4. 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.

  5. 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

    2015-01-01

    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+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. PMID:25881009

  6. Plutonium aging

    SciTech Connect

    Olivas, J.D.

    1999-03-01

    The author describes the plutonium aging program at the Los Alamos National Laboratory. The aging of plutonium components in the US nuclear weapons stockpile has become a concern due to several events: the end of the cold war, the cessation of full scale underground nuclear testing as a result of the Comprehensive Test Ban Treaty (CTBT) and the closure of the Rocky Flats Plant--the site where the plutonium components were manufactured. As a result, service lifetimes for nuclear weapons have been lengthened. Dr. Olivas will present a brief primer on the metallurgy of plutonium, and will then describe the technical approach to ascertaining the long-term changes that may be attributable to self-radiation damage. Facilities and experimental techniques which are in use to study aging will be described. Some preliminary results will also be presented.

  7. Plutonium pyrophoricity

    SciTech Connect

    Stakebake, J.L.

    1992-06-02

    A review of the published literature on ignition and burning of plutonium metal was conducted in order to better define the characteristic of pyrophoric plutonium. The major parameter affecting ignition is the surface area/mass ratio of the sample. Based on this parameter, plutonium metal can be classified into four categories: (1) bulk metal, (2) film and foils, (3) chips and turnings, and (4) powder. Other parameters that can alter the ignition of the metal include experimental, chemical, physical, and environmental effects. These effects are reviewed in this report. It was concluded from this review that pyrophoric plutonium can be conservatively defined as: Plutonium metal that will ignite spontaneously in air at a temperature of 150{degrees}C or below in the absence of external heat, shock, or friction. The 150{degrees}C temperature was used to compensate for the self-heating of plutonium metal. For a practical definition of whether any given metal is pyrophoric, all of the factors affecting ignition must be considered.

  8. Provenance of unknown plutonium material.

    PubMed

    Nicolaou, G

    2008-10-01

    The determination of the provenance of 'unknown' plutonium material is demonstrated through a simulation study based on an isotopic fingerprinting approach. Plutonium of known provenance was considered as the 'unknown' nuclear material in order to evaluate the potential of the approach and verify its predictive capabilities. Factor analysis was used to compare the Pu isotopic composition of the 'unknown' material with Pu isotopic compositions simulating well known spent fuels from a range of commercial nuclear power stations. The provenance of the 'unknown material' is assigned to the commercial fuel with which exhibits the highest degree of similarity with respect to the Pu composition. The approach appears promising since it accurately predicted the provenance of the one 'unknown' sample considered; nevertheless, the approach is still at the development stage. Important challenging issues related to the simulation uncertainties and its testing on real laboratory samples have to be explored prior to evaluating the potential of the approach. PMID:18639370

  9. 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.

  10. 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.

  11. On-line monitoring of plutonium in mixed uranium-plutonium solutions. [Coprocessing

    SciTech Connect

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

    1980-03-01

    The measurement of the total and isotopic plutonium concentrations in mixed uranium-plutonium solutions blended with highly radioactive fission product nuclides and other radionuclides (e.g., Cs-137 and Co-60) has been investigated at the Barnwell Nuclear Fuel Plant (BNFP). An on-line total and isotopic plutonium monitoring system is being tested for its ability to assay the plutonium abundances in solutions as might be found in the process streams of a light water reactor (LWR) spent fuel processing plant. The monitoring system is fully automated and designed to be maintained remotely. It is capable of near real-time inventory of plutonium in process streams and provides the basis for on-line computerized accounting of special nuclear materials.

  12. 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.

  13. 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.

  14. 10 CFR 71.88 - Air transport of plutonium.

    Code of Federal Regulations, 2013 CFR

    2013-01-01

    ... citation of 49 CFR chapter I, as may be applicable, the licensee shall assure that plutonium in any form... carrier, require compliance with 49 CFR 175.704, U.S. Department of Transportation regulations applicable... shipped in a single package containing no more than an A2 quantity of plutonium in any isotope or...

  15. 10 CFR 71.88 - Air transport of plutonium.

    Code of Federal Regulations, 2011 CFR

    2011-01-01

    ... citation of 49 CFR chapter I, as may be applicable, the licensee shall assure that plutonium in any form... carrier, require compliance with 49 CFR 175.704, U.S. Department of Transportation regulations applicable... shipped in a single package containing no more than an A2 quantity of plutonium in any isotope or...

  16. 10 CFR 71.88 - Air transport of plutonium.

    Code of Federal Regulations, 2014 CFR

    2014-01-01

    ... citation of 49 CFR chapter I, as may be applicable, the licensee shall assure that plutonium in any form... carrier, require compliance with 49 CFR 175.704, U.S. Department of Transportation regulations applicable... shipped in a single package containing no more than an A2 quantity of plutonium in any isotope or...

  17. 10 CFR 71.88 - Air transport of plutonium.

    Code of Federal Regulations, 2012 CFR

    2012-01-01

    ... citation of 49 CFR chapter I, as may be applicable, the licensee shall assure that plutonium in any form... carrier, require compliance with 49 CFR 175.704, U.S. Department of Transportation regulations applicable... shipped in a single package containing no more than an A2 quantity of plutonium in any isotope or...

  18. 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))))))))

  19. 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

  20. 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.

  1. 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.

  2. 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.

  3. 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.

  4. Excess Plutonium: Weapons Legacy or National Asset?

    SciTech Connect

    Klipa, G.; Boeke, S.; Hottel, R.

    2002-02-27

    The Nuclear Materials Stewardship Initiative was established in January, 2000, to accelerate the work of achieving integration and cutting long-term costs associated with the management of nuclear materials. As part of that initiative, the Department of Energy (DOE), Office of Environmental Management (EM), has established Nuclear Material Management Groups for the management of excess nuclear materials. As one of these groups, the Plutonium Material Management Group (PMMG) has been chartered to serve as DOE's complex wide resource and point of contact for technical coordination and program planning support in the safe and efficient disposition of the nations excess Plutonium 239. This paper will explain the mission, goals, and objectives of the PMMG. In addition, the paper will provide a broad overview of the status of the plutonium inventories throughout the DOE complex. The DOE currently manages approximately 99.5 MT of plutonium isotopes. Details of the various categories of plutonium, from material designated for national security needs through material that has been declared excess, will be explained. For the plutonium that has been declared excess, the various pathways to disposition (including reuse, recycling, sale, transfer, treatment, consumption, and disposal) will be discussed. At this time 52.5 MT of plutonium has been declared excess and the method of disposition for that material is the subject of study and evaluation within DOE. The role of the PMMG in those evaluations will be outlined.

  5. 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

    2013-09-01

    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. PMID:23899337

  6. 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.

  7. 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. PMID:26688367

  8. 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.

  9. Automated monitoring of in-process plutonium concentration

    SciTech Connect

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

    1982-01-01

    An automated low-level plutonium monitor capable of measuring total and isotopic plutonium abundances in solutions is described. To demonstrate near real-time assay of in-process plutonium, we installed a monitor on a flowing stream of a laboratory experimental facility. The stream was composed of uranium and plutonium in nitric acid at concentrations typical of a plant using a Purex flowsheet modified to permit coprocessing of spent nuclear fuel. The plutonium isotopic abundances were typical of those found in light water reactor grade fuel. The plutonium isotopic concentrations in the stream with the exception of /sup 242/Pu were determined by direct lambda-ray spectrometry. The /sup 242/Pu abundance was calculated by isotope correlation techniques. Additional data were obtained on coprocessed uranium-plutonium solutions denatured with fission products (/sup 103/Ru, /sup 144/Ce//sup 144/Pr, and /sup 95/Zr//sup 95/Nb). /sup 239/Pu and /sup 240/Pu concentrations can be determined to within 2% and 5%, respectively, of the concentrations determined by mass spectrometry.

  10. 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. PMID:19722516

  11. Plutonium Immobilization Puck Handling

    SciTech Connect

    Kriikku, E.

    1999-01-26

    The Plutonium Immobilization Project (PIP) will immobilize excess plutonium and store the plutonium in a high level waste radiation field. To accomplish these goals, the PIP will process various forms of plutonium into plutonium oxide, mix the oxide powder with ceramic precursors, press the mixture into pucks, sinter the pucks into a ceramic puck, load the pucks into metal cans, seal the cans, load the cans into magazines, and load the magazines into a Defense Waste Processing Facility (DPWF) canister. These canisters will be sent to the DWPF, an existing Savannah River Site (SRS) facility, where molten high level waste glass will be poured into the canisters encapsulating the ceramic pucks. Due to the plutonium radiation, remote equipment will perform these operations in a contained environment. The Plutonium Immobilization Project is in the early design stages and the facility will begin operation in 2005. This paper will discuss the Plutonium Immobilization puck handling conceptual design and the puck handling equipment testing.

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. Plutonium immobilization -- Can loading

    SciTech Connect

    Kriikku, E.

    2000-02-17

    The Savannah River Site (SRS) will immobilize excess plutonium in the proposed Plutonium Immobilization Project (PIP). The PIP adds the excess plutonium to ceramic pucks, loads the pucks into cans, and places the cans into DWPF canisters. This paper discusses the PIP process steps, the can loading conceptual design, can loading equipment design, and can loading work completed.

  18. 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/.

  19. Resonance ionization mass spectrometry of ion beam sputtered neutrals for element- and isotope-selective analysis of plutonium in micro-particles.

    PubMed

    Erdmann, N; Kratz, J-V; Trautmann, N; Passler, G

    2009-11-01

    Micro-particles containing actinides are of interest for risk assessments of contaminated areas, nuclear forensic analyses, and IAEA as well as Euratom safeguards programs. For their analysis, secondary ion mass spectrometry (SIMS) has been established as the state-of-the-art standard technique. In the case of actinide mixtures within the particles, however, SIMS suffers from isobaric interferences (e.g., (238)U/(238)Pu, (241)Am/(241)Pu). This can be eliminated by applying resonance ionization mass spectrometry which is based on stepwise resonant excitation and ionization of atoms with laser light, followed by mass spectrometric detection of the produced ions, combining high elemental selectivity with the analysis of isotopic compositions. This paper describes the instrumental modifications for coupling a commercial time-of-flight (TOF)-SIMS apparatus with three-step resonant post-ionization of the sputtered neutrals using a high-repetition-rate (kHz) Nd:YAG laser pumped tunable titanium:sapphire laser system. Spatially resolved ion images obtained from actinide-containing particles in TOF-SIMS mode demonstrate the capability for isotopic and spatial resolution. Results from three-step resonant post-ionization of bulk Gd and Pu samples successfully demonstrate the high elemental selectivity of this process. PMID:19557397

  20. The Concentration of (236)Pu Daughters in Plutonium for Application to MOX Production from Plutonium from Dismantled US Nuclear Weapons

    SciTech Connect

    Sampson, T.E.; Cremers, T.L.

    2001-05-01

    The isotope {sup 236}Pu in the weapons-grade plutonium to be used in the US MOX (mixed-oxide) plant is of concern because the daughter products of {sup 236}Pu are sources of high-energy gamma rays. The {sup 208}Tl daughter of {sup 236}Pu emits intense, high-energy gamma rays that are important for radiation exposure calculations for plant design. It is generally thought that the concentrations of {sup 236}Pu and its daughters are well below 10{sup {minus}10}, but these concentrations are generally below the detection limits of most analytical techniques. One technique that can be used to determine the concentration {sup 208}Tl is the direct measurement of the intensity of the {sup 208}Tl gamma rays in the gamma-ray spectrum from plutonium. Thallium-208 will be in equilibrium with {sup 228}Th, and may very well be in equilibrium with {sup 232}U for most aged plutonium samples. We have used the FRAM isotopic analysis software to analyze dozens of archived high-resolution gamma ray spectra from various samples of US and foreign plutonium. We are able to quantify the ratio of minor isotopes with measurable gamma-ray emissions to the major isotope of plutonium and hence, through the measurement of the plutonium isotopic distribution of the sample, to elemental plutonium itself. Excluding items packaged in fluoropolymer vials, all samples analyzed with {sup 240}Pu < 9% gave {sup 228}Th/Pu ratios < 3.4 e-012 and all samples of US-produced plutonium, including {sup 240}Pu values up to 16.4%, gave {sup 228}Th/Pu ratios < 9.4 e-012. None of these values is significant from a radiation dose standpoint.

  1. 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.

  2. 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.

  3. I. Nuclear Production Reaction and Chemical Isolation Procedure for Americium-240 II. New Superheavy Element Isotopes: Plutonium-242(Calcium-48,5n)(285)114

    NASA Astrophysics Data System (ADS)

    Ellison, Paul Andrew

    2011-12-01

    Part I discusses the study of a new nuclear reaction and chemical separation procedure for the production of 240Am. Thin 242Pu, natTi, and natNi targets were coincidently activated with protons from the 88-Inch Cyclotron, producing 240Am, 48V, and 57Ni, respectively. The radioactive decay of these isotopes was monitored using high-purity Ge gamma ray detectors in the weeks following irradiation. The excitation function for the 242 Pu(p, 3n)240Am nuclear reaction was measured to be lower than theoretical predictions, but high enough to be the most viable nuclear reaction for the large-scale production of 240 Am. Details of the development of a chemical separation procedure for isolating 240Am from proton-irradiated 242Pu are discussed. The separation procedure, which includes two anion exchange columns and two extraction chromatography columns, was experimentally investi- gated using tracer-level 241Am, 239Pu, and model proton-induced fission products 95Zr, 95Nb, 125Sb, and 152Eu. The separation procedure was shown to have an Am/Pu separation factor of >2x10 7 and an Am yield of ˜70%. The separation procedure was found to purify the Am sample from >99.9% of Eu, Zr, Nb, and Sb. The procedure is well suited for the processing of ˜1 gram of proton-irradiated 242Pu to produce a neutron-induced fission target consisting of tens of nanograms of 240Am. Part II describes the use of the Berkeley Gas-filled Separator at the Lawrence Berkeley National Laboratory 88-Inch Cyclotron for the study of the 242Pu(48Ca,5n)285114 nuclear re- action. The new, neutron-deficient, superheavy element isotope 285114 was produced in 48Ca irradiations of 242Pu targets at a center-of-target beam energy of 256 MeV ( E* = 50 MeV). The alpha decay of 285114 was followed by the sequential alpha decay of four daughter nuclides, 281Cn, 277Ds, 273Hs, and 269 Sg. 265Rf was observed to decay by spontaneous fission. The measured alpha-decay Q-values were compared with those from a macroscopic

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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)

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

    SciTech Connect

    Litaor, M.I.

    1999-02-01

    Spatial analysis of the {sup 240}Pu:{sup 239}Pu 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 {ge}0.155, this were minimally impacted by the plant activity; (2) he study area east of Rocky Flats Plant exhibited a plutonium isotopic ratio {le}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.

  11. 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. PMID:9929128

  12. 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.

  13. 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.

  14. PROCESS OF OXIDIZING PLUTONIUM

    DOEpatents

    Coryell, C.D.

    1959-08-25

    The oxidation of plutonium to the plus six valence state is described. The oxidation is accomplished by treating the plutonium in aqueous solution with a solution above 0.01 molar in argentic ion, above 1.1 molar in nitric acid, and above 0.02 molar in argentous ion.

  15. 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.

  16. 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.

  17. 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.

  18. 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

  19. 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.

  20. 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.

  1. 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

  2. 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.

  3. Plutonium radiation surrogate

    DOEpatents

    Frank, Michael I.

    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.

  4. 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.

  5. 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.

  6. 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)

  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. PMID:16096501

  8. 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.

  9. 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.

  10. Plutonium microstructures, part 1

    NASA Astrophysics Data System (ADS)

    Cramer, E. M.; Bergin, J. B.

    1981-09-01

    Illustrations of inclusions that are seen in plutonium metal as a consequence of inherent and tramp impurities, alloy additions, and thermal or mechanical treatments are presented. This part includes illustrations of nonmetallic and intermetallic inclusions characteristic of major impurity elements as an aid to identifying unknowns are included. Historical aspects of the increased purity of laboratory plutonium samples are described and the composition of the etchant solutions are given. The etching procedure used in the preparation of each illustrated sample is described.

  11. 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…

  12. 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.

  13. 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.

  14. Plutonium disproportionation: the ambiguity phenomenon.

    PubMed

    Silver, G L

    2003-05-01

    Plutonium oxidation-state studies may yield ambiguous results if the parameters are not carefully chosen. The effect can be related to environmental plutonium as illustrated by an example. PMID:12735968

  15. INTERCOMPARISON OF PLUTONIUM-239 MEASUREMENTS

    EPA Science Inventory

    In 1977 the U.S. Environmental Protection Agency distributed calibrated solutions of plutonium-239 to laboratories interested in participating in an intercomparison study of plutonium analysis. Participants were asked to perform a quantitative radioactivity analysis of the soluti...

  16. 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.

  17. 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.

  18. 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.

  19. 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.

  20. 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.

  1. Plutonium microstructures. Part 1

    SciTech Connect

    Cramer, E.M.; Bergin, J.B.

    1981-09-01

    This report is the first of three parts in which Los Alamos and Lawrence Livermore National Laboratory metallographers exhibit a consolidated set of illustrations of inclusions that are seen in plutonium metal as a consequence of inherent and tramp impurities, alloy additions, and thermal or mechanical treatments. This part includes illustrations of nonmetallic and intermetallic inclusions characteristic of major impurity elements as an aid to identifying unknowns. It also describes historical aspects of the increased purity of laboratory plutonium samples, and it gives the composition of the etchant solutions and describes the etching procedure used in the preparation of each illustrated sample. 25 figures.

  2. 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.

  3. 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)

  4. 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.

  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. A probabilistic risk assessment of the LLNL Plutonium Facility`s evaluation basis fire operational accident. Revision 1

    SciTech Connect

    Brumburgh, G. P.

    1995-02-27

    The Lawrence Livermore National Laboratory (LLNL) Plutonium Facility conducts numerous programmatic activities involving plutonium to include device fabrication, development of improved and/or unique fabrication techniques, metallurgy research, and laser isotope separation. A Safety Analysis Report (SAR) for the building 332 Plutonium Facility was completed in July 1994 to address operational safety and acceptable risk to employees, the public, government property, and the environmental. This paper outlines the PRA analysis of the Evaluation Basis Fire (EBF) operational accident. The EBF postulates the worst-case programmatic impact event for the Plutonium Facility.

  7. 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.

  8. 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.

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

    PubMed

    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 (239,240)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. PMID:26508010

  10. 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

  11. Toward a Deeper Understanding of Plutonium

    SciTech Connect

    Schwartz, A J; Wolfer, W G

    2007-06-21

    computing power have enabled remarkable progress in our abilities to model many of the anomalous properties of Pu. This special issue of the Journal of Computer-Aided Materials Design highlights a number of these advances in the area of the aging of plutonium. This aging is a long-term process due to the slow radioactive decay with a long half-life of 24400 years for the major isotope of plutonium. The challenge then is to predict the changes in properties of plutonium and its alloys from experimental results of plutonium aged only for a few decades and from theory and computational models that are build on a thorough, first-principle understanding of all the complex phenomena displayed by this material. We hope that progress and success of this enterprise will guide other endeavors in Computer-Aided Materials Design and prediction of materials performance.

  12. 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.

  13. 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.

  14. 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

  15. 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.

  16. 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.

  17. Oxidation of plutonium dioxide.

    PubMed

    Korzhavyi, Pavel A; Vitos, Levente; Andersson, David A; Johansson, Börje

    2004-04-01

    The physics and chemistry of the actinide elements form the scientific basis for rational handling of nuclear materials. In recent experiments, most unexpectedly, plutonium dioxide has been found to react with water to form higher oxides up to PuO(2.27), whereas PuO(2) had always been thought to be the highest stable oxide of plutonium. We perform a theoretical analysis of this complicated situation on the basis of total energies calculated within density functional theory combined with well-established thermodynamic data. The reactions of PuO(2) with either O(2) or H(2)O to form PuO(2+delta) are calculated to be endothermic: that is, in order to occur they require a supply of energy. However, our calculations show that PuO(2+delta) can be formed, as an intermediate product, by reactions with the products of radiolysis of water, such as H(2)O(2). PMID:15034561

  18. 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.

  19. 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). PMID:17543430

  20. 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

  1. 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.

  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. 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.

  4. 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.

  5. 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)

  6. 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.

  7. 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.

  8. 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.

  9. 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.

  10. 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.

  11. 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)

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. Plutonium oxide dissolution

    SciTech Connect

    Gray, J.H.

    1992-09-30

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

  19. Plutonium oxide dissolution

    SciTech Connect

    Gray, J.H.

    1992-09-30

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

  20. 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)

  1. 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.

  2. 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.

  3. 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.

  4. 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.

  5. 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)

  6. 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

  7. 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

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

    NASA Astrophysics Data System (ADS)

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

    2013-10-01

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

  9. 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

    2013-01-01

    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

  10. 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.

  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. 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.

  13. Survey of plutonium and uranium atom ratios and activity levels in Mortandad Canyon

    SciTech Connect

    Gallaher, B.M.; Efurd, D.W.; Rokop, D.J.; Benjamin, T.M.; Stoker, A.K.

    1997-10-01

    For more than three decades, Mortandad Canyon has been the primary release area of treated liquid radioactive waste from the Los Alamos National Laboratory (Laboratory). In this survey, six water samples and seven stream sediment samples collected in Mortandad Canyon were analyzed by thermal ionization mass spectrometry to determine the plutonium and uranium activity levels and atom ratios. By measuring the {sup 240}Pu/{sup 239}Pu atom ratios, the Laboratory plutonium component was evaluated relative to that from global fallout. Measurements of the relative abundance of {sup 235}U and {sup 236}U were also used to identify non-natural components. The survey results indicate that the Laboratory plutonium and uranium concentrations in waters and sediments decrease relatively rapidly with distance downstream from the major industrial sources. Plutonium concentrations in shallow alluvial groundwater decrease by approximately 1,000-fold along a 3,000-ft distance. At the Laboratory downstream boundary, total plutonium and uranium concentrations were generally within regional background ranges previously reported. Laboratory-derived plutonium is readily distinguished from global fallout in on-site waters and sediments. The isotopic ratio data indicate off-site migration of trace levels of Laboratory plutonium in stream sediments to distances approximately two miles downstream of the Laboratory boundary.

  14. Survey of plutonium and uranium atom ratios and activity levels in Mortandad Canyon

    SciTech Connect

    Gallaher, B.M.; Benjamin, T.M.; Rokop, D.J.; Stoker, A.K.

    1997-09-22

    For more than three decades Mortandad Canyon has been the primary release area of treated liquid radioactive waste from the Los Alamos National Laboratory (Laboratory). In this survey, six water samples and seven stream sediment samples collected in Mortandad Canyon were analyzed by thermal ionization mass spectrometry (TIMS) to determine the plutonium and uranium activity levels and atom ratios. Be measuring the {sup 240}Pu/{sup 239}Pu atom ratios, the Laboratory plutonium component was evaluated relative to that from global fallout. Measurements of the relative abundance of {sup 235}U and {sup 236}U were also used to identify non-natural components. The survey results indicate the Laboratory plutonium and uranium concentrations in waters and sediments decrease relatively rapidly with distance downstream from the major industrial sources. Plutonium concentrations in shallow alluvial groundwater decrease by approximately 1000 fold along a 3000 ft distance. At the Laboratory downstream boundary, total plutonium and uranium concentrations were generally within regional background ranges previously reported. Laboratory derived plutonium is readily distinguished from global fallout in on-site waters and sediments. The isotopic ratio data indicates off-site migration of trace levels of Laboratory plutonium in stream sediments to distances approximately two miles downstream of the Laboratory boundary.

  15. Age determination of single plutonium particles after chemical separation

    NASA Astrophysics Data System (ADS)

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

    2009-01-01

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

  16. Plutonium as a tracer of soil and sediment movement in the Herbert River, Australia

    NASA Astrophysics Data System (ADS)

    Tims, S. G.; Everett, S. E.; Fifield, L. K.; Hancock, G. J.; Bartley, R.

    2010-04-01

    Plutonium fallout from atmospheric nuclear-weapons testing in the 1950s and 1960s constitutes an artificial tracer suitable for the study of recent soil erosion and sediment accumulation rates. Traditionally 137Cs has been the fallout isotope of choice for such studies, but the plutonium isotopes confer a number of advantages, which can be realised using the ultra-sensitive detection technique of Accelerator Mass Spectrometry (AMS). As a first application of plutonium to a whole-of-basin study, Pu has been measured in both soil and sediment across the catchment of the Herbert River, which is one of the major rivers draining into Australia's Great Barrier Reef Lagoon. Its catchment includes undisturbed areas as well as regions of pasture and sugar cultivation. The Pu measurements allow the relative contributions of surface and gully erosion from the different land use areas to be determined, and permit the discharged material to be apportioned between the relevant sources.

  17. 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.

  18. Plutonium Immobilization Can Inspection System

    SciTech Connect

    Kriikku, E.

    2000-12-12

    The Savannah River Site (SRS) will immobilize excess plutonium in the proposed Plutonium Immobilization Plant (PIP) as part of Department of Energy's two-track approach for the disposition of weapons-usable plutonium. The PIP will utilize the ceramic can-in-canister technology in a process that mixes plutonium with ceramic formers and neutron absorbers, presses the mixture into a ceramic puck-like form, sinters the pucks in a furnace, loads the pucks into cans, and places the cans into large canisters. The canisters will subsequently be filled with high level waste glass in the Defense Waste Processing Facility for eventual disposal in a geologic repository. This paper will discuss the PIP can inspection components, control system, and test results.

  19. 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.

  20. 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.

  1. SOURCES AND MIGRATION OF PLUTONIUM IN GROUNDWATER AT THE SAVANNAH RIVER SITE

    EPA Science Inventory

    We examined the isotopic composition, size distribution, and redox speciation of plutonium (Pu) in the groundwater of the F-area seepage basins at the US Department of Energy Savannah River Site (SRS). Sampling was designed to follow a groundwater plume downstream from the seepag...

  2. 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

  3. 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)).

  4. 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.

  5. 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.

  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. Development of an "Isotopic" Pulser

    SciTech Connect

    Luke, S J; Schmid, G; Beckedahl, D; Pohl, B; White, G

    2002-06-04

    We have developed a pulser that is able to generate a simulated signal from a high-purity germanium (HPGe) detector for various plutonium isotopes. In this paper we describe the development of an ''isotopics'' pulser for the simulation of signals that are produced by an HPGe detector. The present pulser generates the waveforms that are produced by an HPGe detector both before and after the preamplifier. These signals have been input into a normal MCA and the result closely simulates a genuine pulse-height distribution.

  8. 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.

  9. 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).

  10. 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. PMID:22420016

  11. Zone refining of plutonium metal

    SciTech Connect

    1997-05-01

    The purpose of this study was to investigate zone refining techniques for the purification of plutonium metal. The redistribution of 10 impurity elements from zone melting was examined. Four tantalum boats were loaded with plutonium impurity alloy, placed in a vacuum furnace, heated to 700{degrees}C, and held at temperature for one hour. Ten passes were made with each boat. Metallographic and chemical analyses performed on the plutonium rods showed that, after 10 passes, moderate movement of certain elements were achieved. Molten zone speeds of 1 or 2 inches per hour had no effect on impurity element movement. Likewise, the application of constant or variable power had no effect on impurity movement. The study implies that development of a zone refining process to purify plutonium is feasible. Development of a process will be hampered by two factors: (1) the effect on impurity element redistribution of the oxide layer formed on the exposed surface of the material is not understood, and (2) the tantalum container material is not inert in the presence of plutonium. Cold boat studies are planned, with higher temperature and vacuum levels, to determine the effect on these factors. 5 refs., 1 tab., 5 figs.

  12. 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.

  13. 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.

  14. 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

  15. 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.

  16. 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.

  17. 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.

  18. 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.

  19. Field test of New TASTEX system for plutonium product verification at the Tokai Reprocessing Plant

    SciTech Connect

    Kuno, Y.; Shigeoka, K.; Nishida, K.; Ikeda, H.; Hayashi, N.; Wachi, I.; Hsue, S.T.; Sprinkle, J.K.; Gunnink, R.; Ruhter, W.D.

    1988-01-01

    This report describes the field test results of the New TASTEX system. This system consisting of the high resolution gamma spectrometer and the k-edge densitometer can measure both isotopic abundances and concentration of plutonium simultaneously. Entire system is controlled by the multichannel analyzer and a multi-user computer. The system was designed and built under the Japan Support Program for Agency Safeguards (JASPAS). The software of this system developed at LANL and LLNL has been installed in the system assembled at the Tokai reprocessing plant (TRP) in July 1985. In the course of campaigns from 1985 until 1988, field tests have been carried out on plutonium product solutions of TRP. The results of plutonium concentration and isotopic abundances obtained by the k-edge densitometer and the high resolution gamma spectrometer (HRGS) have been compared with those by controlled potential coulometer and mass spectrometer respectively. Precision of plutonium determination with k-edge densitometer is estimated approximately 0.7% and 1.0% for the freshly processed plutonium and the aged plutonium respectively. The scatters in the relative differences between HRGS and the destructive analysis (DA) detected on the results of freshly processed plutonium sample were 1.6%, 0.4%, 0.5%, 1.1%, 8.0% for Pu-238, Pu-239, Pu-240, Pu-241, and Pu-242 respectively, whereas those on the results of aged sample were 1.4%, 0.5%, 1.1%, 1.1% for Pu-238, Pu-239, Pu-240, and Pu-241 respectively. 9 refs., 15 figs., 7 tabs.

  20. 49 CFR 175.704 - Plutonium shipments.

    Code of Federal Regulations, 2012 CFR

    2012-10-01

    ... 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 package... 49 Transportation 2 2012-10-01 2012-10-01 false Plutonium shipments. 175.704 Section...

  1. 49 CFR 175.704 - Plutonium shipments.

    Code of Federal Regulations, 2014 CFR

    2014-10-01

    ... 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 package... 49 Transportation 2 2014-10-01 2014-10-01 false Plutonium shipments. 175.704 Section...

  2. Plutonium immobilization -- Can loading. Revision 1

    SciTech Connect

    Kriikku, E.

    2000-03-13

    The Savannah River Site (SRS) will immobilize excess plutonium in the proposed Plutonium Immobilization Project (PIP). The PIP adds the excess plutonium to ceramic pucks, loads the pucks into cans, and places the cans into DWPF canisters. This paper discusses the PIP process steps, the can loading conceptual design, can loading equipment design, and can loading work completed.

  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. 49 CFR 175.704 - Plutonium shipments.

    Code of Federal Regulations, 2013 CFR

    2013-10-01

    ... 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 package... 49 Transportation 2 2013-10-01 2013-10-01 false Plutonium shipments. 175.704 Section...

  5. 49 CFR 175.704 - Plutonium shipments.

    Code of Federal Regulations, 2011 CFR

    2011-10-01

    ... 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 package... 49 Transportation 2 2011-10-01 2011-10-01 false Plutonium shipments. 175.704 Section...

  6. 49 CFR 175.704 - Plutonium shipments.

    Code of Federal Regulations, 2010 CFR

    2010-10-01

    ... 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 package... 49 Transportation 2 2010-10-01 2010-10-01 false Plutonium shipments. 175.704 Section...

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

    DOE PAGESBeta

    Byerly, Benjamin L.; Stanley, Floyd; Spencer, Khal; Colletti, Lisa; Garduno, Katherine; Kuhn, Kevin; Lujan, Elmer; Martinez, Alex; Porterfield, Donivan; Rim, Jung; et al

    2016-06-27

    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.

  8. 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.

  9. 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.

  10. 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.

  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 Speciation, Solubilization and Migration in Soils

    SciTech Connect

    Neu, M.; Runde, W.

    1999-06-01

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

  14. 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.

  15. 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.

  16. 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.

  17. Plutonium concentrations in lichens of Rocky Flats environs

    SciTech Connect

    Thomas, R.S.; Ibrahim, S.A.

    1995-03-01

    Xanthoparmelia spp. lichens were used to study the spatial distribution of plutonium concentrations in nonvascular plants surrounding the Rocky Flats nuclear weapons facility with respect to distance, direction, age, and washing. Plutonium concentrations in lichens were inversely related to distance from the initial contamination site with a directional component which corroborated wind-borne transport as the primary means of dispersion. Ultrasonic washing and the relative age of the lichen proved to be significant only at p = 0.21 and p = 0.96, respectively. Isotopic ratios of {sup 239,240}Pu to {sup 238}Pu were highly variable at low activities but remained consistent at 62.6 for samples with high total plutonium activity. Correlation of Xanthoparmelia spp. lichen {sup 239,240}Pu concentrations to surface soil concentrations showed a direct relationship (r = 0.767; p < 0.001). The correlation was supported by soil retention studies which revealed a lichen soil content ranging from 11 to 18% on a dry mass basis with a possible particle size selectivity in the different concentration ratios adjacent to and away from the initial contamination site. Results suggest that further study into the in situ biomonitoring of surface soil by Xanthoparmelia spp. lichens is promising. 38 refs., 4 figs., 3 tabs.

  18. Plutonium concentrations in lichens of Rocky Flats environs.

    PubMed

    Thomas, R S; Ibrahim, S A

    1995-03-01

    Xanthoparmelia spp. lichens were used to study the spatial distribution of plutonium concentrations in nonvascular plants surrounding the Rocky Flats nuclear weapons facility with respect to distance, direction, age, and washing. Plutonium concentrations in lichens were inversely related to distance from the initial contamination site with a directional component which corroborated wind-borne transport as the primary means of dispersion. Ultrasonic washing and the relative age of the lichen proved to be significant only at p = 0.21 and p = 0.96, respectively. Isotopic ratios of 239,240Pu to 238Pu were highly variable at low activities but remained consistent at 62.6 for samples with high total plutonium activity. Correlation of Xanthoparmelia spp. lichen 239,240Pu concentrations to surface soil concentrations showed a direct relationship (r = 0.767; p < 0.001). The correlation was supported by soil retention studies which revealed a lichen soil content ranging from 11 to 18% on a dry mass basis with a possible particle size selectivity in the different concentration ratios adjacent to and away from the initial contamination site. Results suggest that further study into the in situ biomonitoring of surface soil by Xanthoparmelia spp. lichens is promising. PMID:7860301

  19. 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.

  20. 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.

  1. Safe disposal of surplus plutonium

    NASA Astrophysics Data System (ADS)

    Gong, W. L.; Naz, S.; Lutze, W.; Busch, R.; Prinja, A.; Stoll, W.

    2001-06-01

    About 150 tons of weapons grade and weapons usable plutonium (metal, oxide, and in residues) have been declared surplus in the USA and Russia. Both countries plan to convert the metal and oxide into mixed oxide fuel for nuclear power reactors. Russia has not yet decided what to do with the residues. The US will convert residues into a ceramic, which will then be over-poured with highly radioactive borosilicate glass. The radioactive glass is meant to provide a deterrent to recovery of plutonium, as required by a US standard. Here we show a waste form for plutonium residues, zirconia/boron carbide (ZrO 2/B 4C), with an unprecedented combination of properties: a single, radiation-resistant, and chemically durable phase contains the residues; billion-year-old natural analogs are available; and criticality safety is given under all conceivable disposal conditions. ZrO 2/B 4C can be disposed of directly, without further processing, making it attractive to all countries facing the task of plutonium disposal. The US standard for protection against recovery can be met by disposal of the waste form together with used reactor fuel.

  2. 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.

  3. 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.

  4. 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)

  5. 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

  6. Evolving Density and Static Mechanical Properties in Plutonium from Self-Irradiation

    SciTech Connect

    Chung, B W; Thompson, S R; Lema, K E; Hiromoto, D S; Ebbinghaus, B B

    2008-07-31

    Plutonium, because of its self-irradiation by alpha decay, ages by means of lattice damage and helium in-growth. These integrated aging effects result in microstructural and physical property changes. Because these effects would normally require decades to measure, studies are underway to assess the effects of extended aging on the physical properties of plutonium alloys by incorporating roughly 7.5 weight % of highly specific activity isotope {sup 238}Pu into the {sup 239}Pu metal to accelerate the aging process. This paper presents updated results of self-irradiation effects on {sup 238}Pu-enriched alloys measured by immersion density, dilatometry, and tensile tests. After nearly 90 equivalent years of aging, both the immersion density and dilatometry show that the enriched alloys continue to decreased in density by {approx}0.002% per year, without void swelling. Quasi-static tensile measurements show that the aging process increases the strength of plutonium alloys.

  7. Chemical, mass spectrometric, spectrochemical, nuclear, and radiochemical analysis of nuclear-grade plutonium nitrate solutions

    SciTech Connect

    Not Available

    1981-01-01

    These analytical procedures are designed to show whether a given material meets the purchaser's specifications as to plutonium content, effective fissile content, and impurity content. The following procedures are described in detail: plutonium by controlled-potential coulometry; plutonium by amperometric titration with iron(II); free acid by titration in an oxalate solution; free acid by iodate precipitation-potentiometric titration method; uranium by Arsenazo I spectrophotometric method; thorium by thorin spectrophotometric method; iron by 1,10-phenanthroline spectrophotometric method; chloride by thiocyanate spectrophotometric method; fluoride by distillation-spectrophotometric method; sulfate by barium sulfate turbidimetric method; isotopic composition by mass spectrometry; americium-241 by extraction and gamma counting; americium-241 by gamma counting; gamma-emitting fission products, uranium, and thorium by gamma-ray spectroscopy; rare earths by copper spark spectrochemical method; tungsten, niobium (columbium), and tantalum by spectrochemical method; simple preparation by spectrographic analysis for general impurities. (JMT)

  8. Plutonium metal exchange program : current status and statistical analysis

    SciTech Connect

    Tandon, L.; Eglin, J. L.; Michalak, S. E.; Picard, R. R.; Temer, D. J.

    2004-01-01

    The Rocky Flats Plutonium (Pu) Metal Sample Exchange program was conducted to insure the quality and intercomparability of measurements such as Pu assay, Pu isotopics, and impurity analyses. The Rocky Flats program was discontinued in 1989 after more than 30 years. In 2001, Los Alamos National Laboratory (LANL) reestablished the Pu Metal Exchange program. In addition to the Atomic Weapons Establishment (AWE) at Aldermaston, six Department of Energy (DOE) facilities Argonne East, Argonne West, Livermore, Los Alamos, New Brunswick Laboratory, and Savannah River are currently participating in the program. Plutonium metal samples are prepared and distributed to the sites for destructive measurements to determine elemental concentration, isotopic abundance, and both metallic and nonmetallic impurity levels. The program provides independent verification of analytical measurement capabilies for each participating facility and allows problems in analytical methods to be identified. The current status of the program will be discussed with emphasis on the unique statistical analysis and modeling of the data developed for the program. The discussion includes the definition of the consensus values for each analyte (in the presence and absence of anomalous values and/or censored values), and interesting features of the data and the results.

  9. Measurement and interpretation of plutonium spectra

    SciTech Connect

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

    1983-01-01

    The atomic spectroscopic data available for plutonium are among the richest of any in the periodic system. They include high-resolution grating and Fourier-transform spectra as well as extensive Zeeman and isotope-shift studies. The present status of the term analysis is summarized, and the configurations that have been identified are cited. 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. 46 references, 9 figures, 7 tables.

  10. 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.

  11. Isotopic Biogeochemistry

    NASA Technical Reports Server (NTRS)

    Hayes, J. M.

    1985-01-01

    An overview is provided of the biogeochemical research. The funding, productivity, personnel and facilities are reviewed. Some of the technical areas covered are: carbon isotopic records; isotopic studies of banded iron formations; isotope effects in microbial systems; studies of organic compounds in ancient sediments; and development in isotopic geochemistry and analysis.

  12. 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.

  13. Plutonium Immobilization Project -- Can loading

    SciTech Connect

    Kriikku, E.

    2000-01-18

    The Savannah River Site (SRS) will immobilize excess plutonium in the proposed Plutonium Immobilization Project (PIP). The PIP scope includes unloading transportation containers, preparing the feed streams, converting the metal feed to an oxide, adding the ceramic precursors, pressing the pucks, inspecting pucks, and sintering pucks. The PIP scope also includes loading the pucks into metal cans, sealing the cans, inspecting the cans, loading the cans into magazines, loading magazines into Defense Waste Processing Facility (DWPF) canisters, and transporting the canisters to the DWPF. The DWPF fills the canister with a mixture of high level radioactive waste and glass for permanent storage. Due to the radiation, remote equipment must perform PIP operations in a contained environment.

  14. 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.

  15. 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. PMID:27575347

  16. 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.

  17. Kläui ligand thin films for rapid plutonium analysis by alpha spectrometry.

    PubMed

    Hanson, Susan K; Mueller, Alexander H; Oldham, Warren J

    2014-01-21

    As part of a nuclear forensics capability, rapid and effective methods to analyze for plutonium and other actinide metals are needed. A key requirement of these methods is that they afford a high chemical yield while still providing isotopic information necessary for forensic evaluation. Toward this objective, a new method for binding plutonium for analysis by alpha spectrometry has been developed. Thin films of Kläui-type tripodal oxygen donor ligands were prepared by spin-casting solutions onto glass substrates. Three different ligands were evaluated for plutonium binding, and the best results were obtained using the ethyl-substituted complex Na[Cp*Co(P(O)(OEt)2)3], which bound 80-88% of the dissolved Pu under equilibrium conditions. The thin films are simple and inexpensive to prepare and exhibit excellent alpha spectral resolution, having line widths of ~33 keV. The method has been successfully applied to analyze for plutonium in both an archived nuclear debris sample and a certified environmental soil sample. The results obtained from the soil analysis are in good agreement with the certified values, demonstrating the effectiveness of the method for rapid plutonium analysis. PMID:24397315

  18. Plutonium stabilization and disposition focus area, FY 1999 and FY 2000 multi-year program plan

    SciTech Connect

    1998-03-01

    Consistent with the Environmental Management`s (EM`s) plan titled, ``Accelerating Cleanup: Paths to Closure``, and ongoing efforts within the Executive Branch and Congress, this Multi-Year Program Plan (MYPP) for the Plutonium Focus Area was written to ensure that technical gap projects are effectively managed and measured. The Plutonium Focus Area (PFA) defines and manages technology development programs that contribute to the effective stabilization of nuclear materials and their subsequent safe storage and final disposition. The scope of PFA activities includes the complete spectrum of plutonium materials, special isotopes, and other fissile materials. The PFA enables solutions to site-specific and complex-wide technology issues associated with plutonium remediation, stabilization, and preparation for disposition. The report describes the current technical activities, namely: Plutonium stabilization (9 studies); Highly enriched uranium stabilization (2 studies); Russian collaboration program (2 studies); Packaging and storage technologies (6 studies); and PFA management work package/product line (3 studies). Budget information for FY 1999 and FY 2000 is provided.

  19. 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.

  20. Air transport of plutonium metal : content expansion initiative for the Plutonium Air Transportable (PAT-1) packaging.

    SciTech Connect

    Mann, Paul T.; Caviness, Michael L.; Yoshimura, Richard Hiroyuki

    2010-06-01

    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.

  1. Zone refining of plutonium metal

    SciTech Connect

    Blau, M.S.

    1994-08-01

    The zone refining process was applied to Pu metal containing known amounts of impurities. Rod specimens of plutonium metal were melted into and contained in tantalum boats, each of which was passed horizontally through a three-turn, high-frequency coil in such a manner as to cause a narrow molten zone to pass through the Pu metal rod 10 times. The impurity elements Co, Cr, Fe, Ni, Np, U were found to move in the same direction as the molten zone as predicted by binary phase diagrams. The elements Al, Am, and Ga moved in the opposite direction of the molten zone as predicted by binary phase diagrams. As the impurity alloy was zone refined, {delta}-phase plutonium metal crystals were produced. The first few zone refining passes were more effective than each later pass because an oxide layer formed on the rod surface. There was no clear evidence of better impurity movement at the slower zone refining speed. Also, constant or variable coil power appeared to have no effect on impurity movement during a single run (10 passes). This experiment was the first step to developing a zone refining process for plutonium metal.

  2. 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.

  3. 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.

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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.

  10. Work and disproportionation for aqueous plutonium.

    PubMed

    Silver, G L

    2003-10-01

    The relation of two plutonium work integrals has recently been illustrated. One of the integrals applies to the work of disproportionation of tetravalent plutonium in 1 M acid and the other to the work of oxidation of plutonium from the trivalent to a higher oxidation state. This paper generalizes the disproportionation work integral so that it can be applied to tetravalent plutonium at any acid concentration. An equation is provided that can be used to verify work estimations obtained by integration. It applies to oxidation and disproportionation processes and it is easy to use. PMID:14522227

  11. 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.

  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. Plutonium 238 facilities at Los Alamos

    NASA Astrophysics Data System (ADS)

    Rinehart, Gary H.

    1991-01-01

    Plutonium 238 operations at Los Alamos are performed at the Plutonium Facility (TA-55), the Chemistry and Metallurgy Research (CMR) Building, and the Radioisotope Fuels Impact Test Facility. The plutonium 238 facilities at Los Alamos support a wide variety of heat source activities including development of new fuel forms and containment materials, research on the high temperature properties of containment materials, investigation of the high temperature compatibility of fuels with potential container materials, processing plutonium 238 fuel forms, manufacture of heat sources under quality assurance surveillance, and performing safety testing on heat sources and radioisotope thermoelectric generators.

  14. Plutonium-238 facilities at Los Alamos

    NASA Astrophysics Data System (ADS)

    Rinehart, Gary H.

    Plutonium-238 operations at Los Alamos are performed at the Plutonium Facility (TA-55), the Chemistry and Metallurgy Research (CMR) Building, and the Radioisotope Fuels Impact Test Facility. The plutonium-238 facilities at Los Alamos support a wide variety of heat source activities including development of new fuel forms and containment materials, research on the high temperature properties of containment materials, investigation of the high temperature compatibility of fuels with potential container materials, processing plutonium-238 fuel forms, manufacture of heat sources under quality assurance surveillance, and performing safety testing on heat sources and radioisotope thermoelectric generators.

  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. Resonance Ionization Mass Spectrometry (RIMS) with Pulsed and CW-Lasers on Plutonium

    NASA Astrophysics Data System (ADS)

    Kunz, P.; Huber, G.; Passler, G.; Trautmann, N.; Wendt, K.

    2005-04-01

    The detection of long-lived plutonium isotopes in ultra-trace amounts by resonance ionization mass spectrometry (RIMS) is a well-established routine method. Detection limits of 106 to 107 atoms and precise measurements of the isotopic composition have been achieved. In this work multi-step resonance ionization of plutonium atoms has been performed with tunable lasers having very different output intensities and spectral properties. In order to compare different ways for the resonance ionization of plutonium broadband pulsed dye and titanium:sapphire lasers as well as narrow-band cw-diode and titanium:sapphire lasers have been applied for a number of efficient excitation schemes. It has been shown, that for identical excitation schemes the optical isotope selectivity can be improved by using cw-lasers (bandwidths < 10 MHz) instead of pulsed lasers (bandwidths > 2 GHz). Pulsed and cw-laser systems have been used simultaneously for resonance ionization enabling direct comparisons of pulsed and continuous ionization processes. So far, a three-step, three-color laser excitation scheme has been proven to be most practical in terms of efficiency, selectivity and laser wavelengths. Alternatively a newly discovered three-step, two-color excitation scheme which includes a strong two-photon transition from an excited state into a high-lying autoionizing state yields similar ionization efficiencies. This two-photon transition was characterized with respect to saturation behavior and line width.

  17. 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.

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

    DOE PAGESBeta

    Lavelle, Kevin B.; Miller, Jeffrey L.; Hanson, Susan K.; Connick, William B.; Spitz, Henry B.; Glover, Samuel E.; Oldham, Warren J.

    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.

  19. 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.

  20. 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.

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

    DOE PAGESBeta

    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.

  2. 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. PMID:15982894

  3. 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.

  4. 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.

  5. 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.

  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. Plutonium disproportionation: the relation of work integrals.

    PubMed

    Silver, G L

    2003-04-01

    Two plutonium work integrals have been demonstrated in recent years. One of them applies to the work of disproportionation and the other to the work of oxidation of plutonium from the trivalent to a higher oxidation state. This paper illustrates the connection of the integrals by an example and a diagram. PMID:12672623

  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. Plutonium Immobilization Project -- Robotic canister loading

    SciTech Connect

    Hamilton, L.

    2000-04-28

    The Plutonium Immobilization Program (PIP) is a joint venture between the Savannah River Site, Lawrence Livermore National Laboratory, Argonne National Laboratory, and Pacific Northwest National Laboratory. When operational in 2008, the PIP will fulfill the nation's nonproliferation commitment by placing surplus weapons-grade plutonium in a permanently stable ceramic form.

  10. 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.

  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. 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.

  13. 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.

  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. 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.

  16. 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.

  17. 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.

  18. 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

  19. 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.

  20. Thermal Analysis on the Shipment of Russian Plutonium Fuel

    SciTech Connect

    Or, Chuen T; Skrabek, Emanuel A; Carpenter, Robert T

    1995-01-01

    Paper presented at the 12th Symposium on Space Nuclear Power and Propulsion in Albuquerque, NM in January 1995. The Mound 9516 shipping package was designed for the shipment of Plutonium-238 fuel. One of the shipping configurations is the Russian Pu-238 powder can. Computer models using SINDA were created to predict the temperatures of the package under normal conditions of transport (NCT: 38oC ambient temperature), under hypothetical accident conditions (HAC: engulfed in fire for 30 minutes), and inside a standard cargo container. Pressure increases inside the package due to the expansion of the trapped gases and helium gas generation from isotope decay were also analyzed. There is a duplicate copy and also a copy in the ESD Files.

  1. 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).

  2. 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.

  3. 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...

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

    Code of Federal Regulations, 2010 CFR

    2010-01-01

    ... 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. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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)

  10. 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.'

  11. 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.

  12. 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.

  13. 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.

  14. 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

  15. 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.

  16. 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.

  17. 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)

  18. Chemical, mass spectrometric, spectrochemical, nuclear and radiochemical analysis of nuclear-grade plutonium metal

    SciTech Connect

    Not Available

    1981-01-01

    These analytical procedures are designed to show whether a given material meets the purchaser's specifications as to plutonium content, effective fissile content, and impurity content. The following procedures are described in detail: dissolution procedure; plutonium by controlled-potential coulometry; plutonium by amperometric titration with iron(II); plutonium by ceric sulfate titration method; uranium by Arsenazo I spectrophotometric method; thorium by thorin spectrophotometric method; iron by 1,10-phenanthroline spectrophotometric method; iron by 2,2'-bipyridyl spectrophotometric method; chloride by the thiocyanate spectrophotometric method; fluoride by distillation-spectrophotometric method; nitrogen by distillation-Nessler reagent spectrophotometric method; carbon by the direct combustion-thermal conductivity method; sulfur by distillation-spectrophotometric method; isotopic composition by mass spectrometry; Americium-241 by extraction and gamma counting; Americium-241 by gamma counting; gamma-emitting fission products, uranium, and thorium by gamma-ray spectroscopy; rare earths by copper spark spectrochemical method; tungsten, niobium (columbium) and tantalum by spectrochemical method; sample preparation for spectrographic analysis for trace impurities. (JMT)

  19. 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.

  20. 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

  1. 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.

  2. 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.

  3. What is plutonium stabilization, and what is safe storage of plutonium?

    SciTech Connect

    Forsberg, C.W.

    1995-06-29

    The end of the cold war has resulted in the shutdown of nuclear weapons production and the start of dismantlement of significant numbers of nuclear weapons. This, in turn, is creating an inventory of plutonium requiring interim and long-term storage. A key question is, ``What is required for safe, multidecade, plutonium storage?`` The requirements for storage, in turn, define what is needed to stabilize the plutonium from its current condition into a form acceptable for interim and long-term storage. Storage requirements determine if research is required to (1) define required technical conditions for interim and long-term storage and (2) develop or improve current stabilization technologies. Storage requirements depend upon technical, policy, and economic factors. The technical issues are complicated by several factors. Plutonium in aerosol form is highly hazardous. Plutonium in water is hazardous. The plutonium inventory is in multiple chemical forms--some of which are chemically reactive. Also, some of the existing storage forms are clearly unsuitable for storage periods over a few years. Gas generation by plutonium compounds complicates storage: (1) all plutonium slowly decays creating gaseous helium and (2) the radiation from plutonium decay can initiate many chemical reactions-some of which generate significant quantities of gases. Gas generation can pressurize sealed storage packages. Last nuclear criticality must be avoided.

  4. 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.

  5. Rapid Separation Methods to Characterize Actinides and Metallic Impurities in Plutonium Scrap Materials at SRS

    SciTech Connect

    Maxwell, S.L. III; Jones, V.D.

    1998-07-01

    The Nuclear Materials Stabilization and Storage Division at SRS plans to stabilize selected plutonium scrap residue materials for long term storage by dissolution processing and plans to stabilize other plutonium vault materials via high-temperature furnace processing. To support these nuclear material stabilization activities, the SRS Analytical Laboratories Department (ALD) will provide characterization of materials required prior to the dissolution or the high-firing of these materials. Lab renovations to install new analytical instrumentation are underway to support these activities that include glove boxes with simulated-process dissolution and high- pressure microwave dissolution capability. Inductively-coupled plasma atomic emission spectrometry (ICP-AES), inductively- coupled mass spectrometry (ICP-MS) and thermal-ionization mass spectrometry (TIMS) will be used to measure actinide isotopics and metallic impurities. New high-speed actinide separation methods have been developed that will be applied to isotopic characterization of nuclear materials by TIMS and ICP-MS to eliminate isobaric interferences between Pu-238 /U- 238 and Pu-241/Am-241. TEVA Resin, UTEVA Resin, and TRU Resin columns will be used with vacuum-assisted flow rates to minimize TIMS and ICP-MS sample turnaround times. For metallic impurity analysis, rapid column removal methods using UTEVA Resin, AGMP-1 anion resin and AG MP-50 cation resin have also been developed to remove plutonium and uranium matrix interferences prior to ICP-AES and ICP- MS measurements.

  6. Isotope separation

    DOEpatents

    Bartlett, Rodney J.; Morrey, John R.

    1978-01-01

    A method and apparatus is described for separating gas molecules containing one isotope of an element from gas molecules containing other isotopes of the same element in which all of the molecules of the gas are at the same electronic state in their ground state. Gas molecules in a gas stream containing one of the isotopes are selectively excited to a different electronic state while leaving the other gas molecules in their original ground state. Gas molecules containing one of the isotopes are then deflected from the other gas molecules in the stream and thus physically separated.

  7. Design-only conceptual design report: Plutonium Immobilization Plant

    SciTech Connect

    DiSabatino, A A

    2000-05-01

    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 Plutonium Immobilization Plant will be located at the Savannah River Site pursuant to the Surplus Plutonium Disposition Final Environmental Impact Statement Record of Decision, January 4, 2000. This document reflects a new facility using the ceramic immobilization technology and the can-in-canister approach. The Plutonium Immobilization Plant accepts plutonium oxide from pit conversion and plutonium and plutonium oxide 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; it must also be suitable for geologic disposal. Plutonium immobilization at the Savannah River Site uses a new building, the Plutonium Immobilization Plant, which will receive and store feed materials, convert non-pit surplus plutonium to an oxide form suitable for the immobilization process, immobilize the plutonium oxide in a titanate-based ceramic form, place cans of the plutonium-ceramic forms into magazines, and load the magazines into a canister. The existing Defense Waste Processing Facility is used for the pouring of high-level waste glass into the canisters. The Plutonium Immobilization Plant uses existing Savannah River Site infrastructure for analytical laboratory services, waste handling, fire protection, training, and other support utilities and services. This design-only conceptual design report also provides the cost for a Plutonium Immobilization Plant which would process

  8. 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

  9. International shipment of plutonium by air

    SciTech Connect

    Mercado, J.E.; McGrogan, J.P.

    1995-05-01

    In support of the United States (US) Government`s decision to place excess plutonium oxide at the US Department of Energy`s (DOE) Hanford Site under International Atomic Energy Agency (IAEA) safeguards, the Department of State notified the Congress that a plutonium storage vault at the Plutonium Finishing Plant at the Hanford Site would be added to the eligible facilities list. As part of the preparations to transfer the plutonium oxide under IAEA safeguards, samples of the powder were taken from the inventory to be shipped to the IAEA headquarters in Vienna, Austria, for laboratory analysis. The analysis of these samples was of high priority, and the IAEA requested that the material be shipped by aircraft, the most expeditious method.

  10. 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.

  11. 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.

  12. 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.

  13. Interaction between stainless steel and plutonium metal

    SciTech Connect

    Dunwoody, John T; Mason, Richard E; Freibert, Franz J; Willson, Stephen P; Veirs, Douglas K; Worl, Laura A; Archuleta, Alonso; Conger, Donald J

    2010-01-01

    Long-term storage of excess plutonium is of great concern in the U.S. as well as abroad. The current accepted configuration involves intimate contact between the stored material and an iron-bearing container such as stainless steel. While many safety scenario studies have been conducted and used in the acceptance of stainless steel containers, little information is available on the physical interaction at elevated temperatures between certain forms of stored material and the container itself. The bulk of the safety studies has focused on the ability of a package to keep the primary stainless steel containment below the plutonium-iron eutectic temperature of approximately 410 C. However, the interactions of plutonium metal with stainless steel have been of continuing interest. This paper reports on a scoping study investigating the interaction between stainless steel and plutonium metal in a pseudo diffusion couple at temperatures above the eutectic melt-point.

  14. 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

  15. Plutonium-238 processing at Savannah River Plant

    SciTech Connect

    Burney, G.A.

    1983-01-01

    Plutonium-238 is produced by irradiating NpO/sub 2/-Al cermet slugs or tubes with neutrons. The neptunium-237 is produced as a by-product when natural or enriched uranium is irradiated with neutrons. The neptunium is separated by solvent extraction and ion exchange and precipitated as neptunium oxalate. Neptunium oxalate is calcined to neptunium oxide and fabricated into targets for irradiation. The irradiation conditions are controlled to produce plutonium with 80 to 90 wt % /sup 238/Pu.

  16. 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.

  17. 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.

  18. 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.

  19. PLUTONIUM FINISHING PLANT (PFP) STABILIZATION & PACKAGING PROJECT

    SciTech Connect

    GERBER, M.S.

    2004-01-14

    Fluor Hanford is pleased to submit the Plutonium Finishing Plant (PFP) Stabilization and Packaging Project (SPP) for consideration by the Project Management Institute as Project of the Year for 2004. The SPP thermally stabilized and/or packaged nearly 18 metric tons (MT) of plutonium and plutonium-bearing materials left in PFP facilities from 40 years of nuclear weapons production and experimentation. The stabilization of the plutonium-bearing materials substantially reduced the radiological risk to the environment and security concerns regarding the potential for terrorists to acquire the non-stabilized plutonium products for nefarious purposes. The work was done In older facilities which were never designed for the long-term storage of plutonium, and required working with materials that were extremely radioactive, hazardous, pyrophoric, and In some cases completely unique. I n some Instances, one-of-a-kind processes and equipment were designed, installed, and started up. The SPP was completed ahead of schedule, substantially beating all Interim progress milestone dates set by the Defense Nuclear Facilities Safety Board (DNFSB) and in the Hanford Site's Federal Facility Agreement and Consent Order (Tri-Party Agreement or TPA), and finished $1-million under budget.

  20. 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. PMID:26144994

  1. Physics studies of weapons plutonium disposition in the IFR closed fuel cycle

    SciTech Connect

    Hill, R.N.; Wade, D.C.; Liaw, J.R.; Fujita, E.K.

    1994-03-01

    The core performance impact of weapons plutonium introduction into the IFR closed fuel cycle is investigated by comparing three disposition scenarios: a power production mode, a moderate destruction mode, and a maximum destruction mode all at a constant heat rating of 840 MWt. For each scenario, two fuel cycle models are evaluated: cores using weapons material as the sole source of transuranics in a once-through mode, and recycle corns using weapons material only as required for a make-up feed. Calculated results include mass flows, detailed isotopic distributions, neutronic performance characteristics, and reactivity feedback coefficients. In general, it is shown that weapons plutonium feed does not have an adverse impact on IFR core performance characteristics.

  2. 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.

  3. Plutonium measurements by accelerator mass spectrometry at LLNL

    SciTech Connect

    McAninch, J E; Hamilton, T F; Broan, T A; Jokela, T A; Knezovich, T J; Ognibene, T J; Proctor, I D; Roberts, M L; Southon, J R; Vogel, J S; Sideras-Haddad, E

    1999-10-26

    Mass spectrometric methods provide sensitive, routine, and cost-effective analyses of long-lived radionuclides. Here the authors report on the status of work at Lawrence Livermore National Laboratory (LLNL) to develop a capability for actinide measurements by accelerator mass spectrometry (AMS) to take advantage of the high potential of AMS for rejection of interferences. This work demonstrates that the LLNL AMS spectrometer is well-suited for providing high sensitivity, robust, high throughput measurements of plutonium concentrations and isotope ratios. Present backgrounds are {approximately}2 x 10{sup 7}atoms per sample for environmental samples prepared using standard alpha spectrometry protocols. Recent measurements of {sup 239+240}Pu and {sup 241}Pu activities and {sup 240}Pu/{sup 239}Pu isotope ratios in IAEA reference materials agree well with IAEA reference values and with alpha spectrometry and recently published ICP-MS results. Ongoing upgrades of the AMS spectrometer are expected to reduce backgrounds below 1 x 10{sup 6} atoms per sample while allowing simplifications of the sample preparation chemistry. These simplifications will lead to lower per-sample costs, higher throughput, faster turn around and, ultimately, to larger and more robust data sets.

  4. 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 .

  5. 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.

  6. 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.

  7. Plutonium dioxide dissolution in glass

    SciTech Connect

    Vienna, J.D.; Alexander, D.L.; Li, Hong

    1996-09-01

    In the aftermath of the Cold War, the U.S. Department of Energy`s (DOE) Office of Fissile Materials Disposition (OFMD) is charged with providing technical support for evaluation of disposition options for excess fissile materials manufactured for the nation`s defense. One option being considered for the disposition of excess plutonium (Pu) is immobilization by vitrification. The vitrification option entails immobilizing Pu in a host glass and waste package that are criticality-safe (immune to nuclear criticality), proliferation-resistant, and environmentally acceptable for long-term storage or disposal. To prove the technical and economic feasibility of candidate vitrification options it is necessary to demonstrate that PuO{sub 2} feedstock can be dissolved in glass in sufficient quantity. The OFMD immobilization program has set a Pu solubility goal of 10 wt% in glass. The life cycle cost of the vitrification options are strongly influenced by the rate at which PUO{sub 2} dissolves in glass. The total number of process lines needed for vitrification of 50 t of Pu in 10 years is directly dependent upon the time required for Pu dissolution in glass. The objective of this joint Pacific Northwest National Laboratory (PNNL) - Savannah River Technology Center (SRTC) study was to demonstrate a high Pu solubility in glass and to identify on a rough scale the time required for Pu dissolution in the glass. This study was conducted using a lanthanide borosilicate (LaBS) glass composition designed at the SRTC for the vitrification of actinides.

  8. 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.

  9. 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.

  10. 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.

  11. 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

  12. 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

  13. The Optimum Plutonium Fuel Form in Light Water Reactors

    NASA Astrophysics Data System (ADS)

    Tulenko, James S.; Savela, Michael; Gueorguiev, Gueorgui

    2003-07-01

    The University of Florida has underway a research program to validate the benefits of developing a Pu/ZrH/U matrix fuel for the irradiation of the U.S. weapons plutonium and European reprocessed plutonium from an economic, operational, and performance basis. Thermal reactors using plutonium as a fuel are inherently undermoderated because of the large absorption cross sections of plutonium and the presence of large absorption resonances for plutonium in the thermal and near-thermal energy ranges. The use of the proven TRIGA ZrHx-based fuel with plutonium has shown an extremely large (>20%) increase in reactivity over the conventional UO2/PuO2 fuel form currently being considered, with an additional major increase in the destruction of plutonium, rendering it an extremely attractive fuel form for plutonium disposition.

  14. Tested method to minimize plutonium assay discrepancies between laboratories

    SciTech Connect

    Seiler, R.J.; Goss, R.L.; Rodenburg, W.W.; Rogers, D.R.

    1982-01-29

    Plutonium assay differences are frequently observed between laboratories exchanging plutonium dioxide powders. These differences are commonly the result of chemical changes and/or nonhomogeneities in sampled materials. The irregularities are often caused by moisture absorption during sampling, packaging, shipment, and storage of the materials. A method is proposed which eliminates the effects of chemical change in samples, particularly moisture absorption, and minimizes sampling error. A nondestructive thermal watts/gram test on every preweighed sampled and total dissolution of these samples for chemical assay are the primary features which make this method effective. Because this method minimizes the error related to exchange material, it is possible to design an interlaboratory exchange program which demonstrates the assay capabiliies of the participants. In an experiment performed to demonstrate the effectiveness of this method, three PuO/sub 2/ batches of varying isotopic composition were synthesized at Mound to be used in the exchange tess. Powder sample aliquots from each batch were weighed directly into their vials under controlled atmospheric conditions. Calorimetric heat measurements were made on each vial to test homogeneity and verify sample weight. Six vials of each batch were chemically assayed at Mound and six at NBL (New Brunswick Laboratory). Both laboratories chose controlled-potential coulometry as the chemical assay technique because of its demonstrated precision and accuracy. Total dissolution of preweighed exchange samples eliminated the need for laborious and usually futile heating to return the material to its original condition. The mean chemical assay values obtained by Mound and NBL agree to within 0.01% for each of the compositions tested. Testing of both chemical assay and calorimetric data revealed no sampling error throughout the experiment.

  15. Isotopic chirality

    SciTech Connect

    Floss, H.G.

    1994-12-01

    This paper deals with compounds that are chiral-at least in part, due to isotope substitution-and their use in tracing the steric course of enzyme reaction in vitro and in vivo. There are other applications of isotopically chiral compounds (for example, in analyzing the steric course of nonenzymatic reactions and in probing the conformation of biomolecules) that are important but they will not be discussed in this context.

  16. Transuranium isotopes

    SciTech Connect

    Hoffman, D.C.

    1985-12-01

    The needs of the research community for the production of transuranium isotopes, the quantities required, the continuity of production desired, and what a new steady state neutron source would have to provide to satisfy these needs are discussed. Examples of past frontier research which need these isotopes as well as an outline of the proposed Large Einsteinium Activation Program, LEAP, which requires roughly ten times the current production of /sup 254/Es are given. 15 refs., 5 figs., 4 tabs.

  17. 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.

  18. 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.

  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. Plutonium transport in the environment.

    PubMed

    Kersting, Annie B

    2013-04-01

    The recent estimated global stockpile of separated plutonium (Pu) worldwide is about 500 t, with equal contributions from nuclear weapons and civilian nuclear energy. Independent of the United States' future nuclear energy policy, the current large and increasing stockpile of Pu needs to be safely isolated from the biosphere and stored for thousands of years. Recent laboratory and field studies have demonstrated the ability of colloids (1-1000 nm particles) to facilitate the migration of strongly sorbing contaminants such as Pu. In understanding the dominant processes that may facilitate the transport of Pu, the initial source chemistry and groundwater chemistry are important factors, as no one process can explain all the different field observations of Pu transport. Very little is known about the molecular-scale geochemical and biochemical mechanisms controlling Pu transport, leaving our conceptual model incomplete. Equally uncertain are the conditions that inhibit the cycling and mobility of Pu in the subsurface. Without a better mechanistic understanding for Pu at the molecular level, we cannot advance our ability to model its transport behavior and achieve confidence in predicting long-term transport. Without a conceptual model that can successfully predict long-term Pu behavior and ultimately isolation from the biosphere, the public will remain skeptical that nuclear energy is a viable and an attractive alternative to counter global warming effects of carbon-based energy alternatives. This review summarizes our current understanding of the relevant conditions and processes controlling the behavior of Pu in the environment, gaps in our scientific knowledge, and future research needs. PMID:23458827

  1. 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.

  2. 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

  3. 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.

  4. 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.

  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. 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...

  7. 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...

  8. 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...

  9. 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

  10. 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

  11. Removal of Uranium from Plutonium Solutions by Anion Exchange

    SciTech Connect

    Rudisill, T.S.

    2002-03-22

    The anion exchange capacity in the HB-Line Phase II Facility will be used to purify plutonium solutions potentially containing significant quantities of depleted uranium. Following purification, the plutonium will be precipitated as an oxalate and calcined to plutonium oxide (PuO2) for storage until final disposition.

  12. 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...

  13. 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...

  14. 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.

  15. 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)

  16. A Plutonium Ceramic Target for MASHA

    SciTech Connect

    Wilk, P A; Shaughnessy, D A; Moody, K J; Kenneally, J M; Wild, J F; Stoyer, M A; Patin, J B; Lougheed, R W; Ebbinghaus, B B; Landingham, R L; Oganessian, Y T; Yeremin, A V; Dmitriev, S N

    2004-07-06

    We are currently developing a plutonium ceramic target for the MASHA mass separator. The MASHA separator will use a thick plutonium ceramic target capable of tolerating temperatures up to 2000 C. Promising candidates for the target include oxides and carbides, although more research into their thermodynamic properties will be required. Reaction products will diffuse out of the target into an ion source, where they will then be transported through the separator to a position-sensitive focal-plane detector array. Experiments on MASHA will allow us to make measurements that will cement our identification of element 114 and provide for future experiments where the chemical properties of the heaviest elements are studied.

  17. Closure Welding of Plutonium Bearing Storage Containers

    SciTech Connect

    Cannell, G.R.

    2002-02-28

    A key element in the Department of Energy (DOE) strategy for the stabilization, packaging and storage of plutonium-bearing materials involves closure welding of DOE-STD-3013 Outer Containers (3013 container). The 3013 container provides the primary barrier and pressure boundary preventing release of plutonium-bearing materials to the environment. The final closure (closure weld) of the 3013 container must be leaktight, structurally sound and meet DOE STD 3013 specified criteria. This paper focuses on the development, qualification and demonstration of the welding process for the closure welding of Hanford PFP 3013 outer containers.

  18. 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.

  19. 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.

  20. 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.

  1. Isotopic signatures by bulk analyses

    SciTech Connect

    Efurd, D.W.; Rokop, D.J.

    1997-12-01

    Los Alamos National Laboratory has developed a series of measurement techniques for identification of nuclear signatures by analyzing bulk samples. Two specific applications for isotopic fingerprinting to identify the origin of anthropogenic radioactivity in bulk samples are presented. The first example is the analyses of environmental samples collected in the US Arctic to determine the impact of dumping of radionuclides in this polar region. Analyses of sediment and biota samples indicate that for the areas sampled the anthropogenic radionuclide content of sediments was predominantly the result of the deposition of global fallout. The anthropogenic radionuclide concentrations in fish, birds and mammals were very low. It can be surmised that marine food chains are presently not significantly affected. The second example is isotopic fingerprinting of water and sediment samples from the Rocky Flats Facility (RFP). The largest source of anthropogenic radioactivity presently affecting surface-waters at RFP is the sediments that are currently residing in the holding ponds. One gram of sediment from a holding pond contains approximately 50 times more plutonium than 1 liter of water from the pond. Essentially 100% of the uranium in Ponds A-1 and A-2 originated as depleted uranium. The largest source of radioactivity in the terminal Ponds A-4, B-5 and C-2 was naturally occurring uranium and its decay product radium. The uranium concentrations in the waters collected from the terminal ponds contained 0.05% or less of the interim standard calculated derived concentration guide for uranium in waters available to the public. All of the radioactivity observed in soil, sediment and water samples collected at RFP was naturally occurring, the result of processes at RFP or the result of global fallout. No extraneous anthropogenic alpha, beta or gamma activities were detected. The plutonium concentrations in Pond C-2 appear to vary seasonally.

  2. 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).

  3. 10 CFR 140.107 - Appendix G-Form of indemnity agreement with licensees processing plutonium for use in plutonium...

    Code of Federal Regulations, 2012 CFR

    2012-01-01

    ... processing plutonium for use in plutonium processing and fuel fabrication plants and furnishing insurance... plutonium processing and fuel fabrication plants and furnishing insurance policies as proof of financial... death, or loss of or damage to property, or loss of use of property, arising out of or resulting...

  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... for use in plutonium processing and fuel fabrication plants and furnishing proof of financial... death, or loss of or damage to property, or loss of use of property, arising out of or resulting...

  5. 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... for use in plutonium processing and fuel fabrication plants and furnishing proof of financial... death, or loss of or damage to property, or loss of use of property, arising out of or resulting...

  6. 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... for use in plutonium processing and fuel fabrication plants and furnishing proof of financial... death, or loss of or damage to property, or loss of use of property, arising out of or resulting...

  7. 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.

  8. Using magnetization measurements to detect small amounts of plutonium hydride formation in plutonium metal

    NASA Astrophysics Data System (ADS)

    Mielke, C. H.; Kim, J. W.; Mun, E.-D.; Baiardo, J. P.; Smith, A. I.; Richmond, S.; Mitchell, J.; Schwartz, D.; Zapf, V. S.

    2015-03-01

    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. 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.

  11. 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.

  12. 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.

  13. 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.

  14. ISOTOPE SEPARATORS

    DOEpatents

    Bacon, C.G.

    1958-08-26

    An improvement is presented in the structure of an isotope separation apparatus and, in particular, is concerned with a magnetically operated shutter associated with a window which is provided for the purpose of enabling the operator to view the processes going on within the interior of the apparatus. The shutier is mounted to close under the force of gravity in the absence of any other force. By closing an electrical circuit to a coil mouated on the shutter the magnetic field of the isotope separating apparatus coacts with the magnetic field of the coil to force the shutter to the open position.

  15. 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.

  16. Plutonium Management in the Medium Term

    SciTech Connect

    Hesketh, Kevin; Schlosser, Gerhard; Porsch, Dieter F.; Wolf, Timm; Koeberl, Oliver; Lance, Benoit; Chawla, Rakesh; Gehin, Jess C.; Ellis, Ron; Uchikawa, Sadao; Sato, Osamu; Okubo, Tsutomu; Mineo, Hideaki; Yamamoto, Toru; Sagayama, Yutaka; Sartori, Enrico

    2004-12-15

    For many years various countries with access to commercial reprocessing services have been routinely recycling plutonium as UO{sub 2}/PuO{sub 2} mixed oxide (MOX) fuel in light water reactors (LWRs). This LWR MOX recycle strategy is still widely regarded as an interim step leading to the eventual establishment of sustainable fast reactor fuel cycles. The OECD/NEA Working Party on the Physics of Plutonium Fuels and Innovative Fuel Cycles (WPPR) has recently completed a review of the technical options for plutonium management in what it refers to as the 'medium term'. For the purpose of the review, the WPPR considers the medium term to cover the period from now up to the point at which fast reactor fuel cycles are established on a commercial scale. The review identified a number of different designs of innovative plutonium fuel assemblies intended to be used in current LWR cores, in LWRs with significantly different moderation properties, as well as in high-temperature gas reactors. The full review report describes these various options and highlights their respective advantages and disadvantages. This paper briefly summarizes the main findings of the review.

  17. 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.

  18. 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.

  19. 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.

  20. PLUTONIUM SPECIATION, SOLUBILIZATION, AND MIGRATION IN SOILS

    EPA Science Inventory

    The DOE is currently conducting cleanup activities at its nuclear weapons development sites, many of which have accumulated plutonium (Pu) in soils for 50 years. There is scientific uncertainty about the levels of risk to human health posed by this accumulation and whether Pu is ...

  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. 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.

  3. 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)

  4. 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.

  5. 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.

  6. Clues in the rare gas isotopes to early solar system history

    NASA Technical Reports Server (NTRS)

    Reynolds, J. H.

    1974-01-01

    Rare gases in meteorites and lunar samples are discussed stimulating the discovery of the solar wind. Radioactive isotopes are examined, making a correlation to the origin of the solar system. It is shown that the heights of the peaks above the horizontal lines represent the spectrum of the fissiogenic sample. Nuclear tracks of iodine, xenon, and plutonium detected in lunar rocks are also explained.

  7. 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

  8. Crystalline plutonium hosts derived from high-level waste formulations.

    SciTech Connect

    O'Holleran, T. P.

    1998-04-24

    The Department of Energy has selected immobilization for disposal in a repository as one approach for disposing of excess plutonium (1). Materials for immobilizing weapons-grade plutonium for repository disposal must meet the ''spent fuel standard'' by providing a radiation field similar to spent fuel (2). Such a radiation field can be provided by incorporating fission products from high-level waste into the waste form. Experiments were performed to evaluate the feasibility of incorporating high-level waste (HLW) stored at the Idaho Chemical Processing Plant (ICPP) into plutonium dispositioning materials to meet the spent fuel standard. A variety of materials and preparation techniques were evaluated based on prior experience developing waste forms for immobilizing HLW. These included crystalline ceramic compositions prepared by conventional sintering and hot isostatic pressing (HIP), and glass formulations prepared by conventional melting. Because plutonium solubility in silicate melts is limited, glass formulations were intentionally devitrified to partition plutonium into crystalline host phases, thereby allowing increased overall plutonium loading. Samarium, added as a representative rare earth neutron absorber, also tended to partition into the plutonium host phases. Because the crystalline plutonium host phases are chemically more inert, the plutonium is more effectively isolated from the environment, and its attractiveness for proliferation is reduced. In the initial phase of evaluating each material and preparation method, cerium was used as a surrogate for plutonium. For promising materials, additional preparation experiments were performed using plutonium to verify the behavior of cerium as a surrogate. These experiments demonstrated that cerium performed well as a surrogate for plutonium. For the most part, cerium and plutonium partitioned onto the same crystalline phases, and no anomalous changes in oxidation state were observed. The only observed

  9. 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. )

  10. Determining Spent Nuclear Fuel's Plutonium Content, Initial Enrichment, Burnup, and Cooling Time

    SciTech Connect

    Cheatham, Jesse R; Francis, Matthew W

    2011-01-01

    The Next Generation of Safeguards Initiative is examining nondestructive assay techniques to determine the total plutonium content in spent nuclear fuel. The goal of this research was to develop new techniques that can independently verify the plutonium content in a spent fuel assembly without relying on an operator's declarations. Fundamentally this analysis sought to answer the following questions: (1) do spent fuel assemblies contain unique, identifiable isotopic characteristics as a function of their burnup, cooling time, and initial enrichment; (2) how much variation can be seen in spent fuel isotopics from similar and dissimilar reactor power operations; and (3) what isotopes (if any) could be used to determine burnup, cooling time, and initial enrichment? To answer these questions, 96,000 ORIGEN cases were run that simulated typical two-cycle operations with burnups ranging from 21,900 to 72,000 MWd/MTU, cooling times from 5 to 25 years, and initial enrichments between 3.5 and 5.0 weight percent. A relative error coefficient was determined to show how numerically close a reference solution has to be to another solution for the two results to be indistinguishable. By looking at the indistinguishable solutions, it can be shown how a precise measurement of spent fuel isotopics can be inconclusive when used in the absence of an operator's declarations. Using this Method of Indistinguishable Solutions (MIS), we evaluated a prominent method of nondestructive analysis - gamma spectroscopy. From this analysis, a new approach is proposed that demonstrates great independent forensic examination potential for spent nuclear fuel by examining both the neutron emissions of Cm-244 and the gamma emissions of Cs-134 and Eu-154.

  11. 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

  12. 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)

  13. Plutonium, Mineralogy and Radiation Effects

    NASA Astrophysics Data System (ADS)

    Ewing, R. C.

    2006-05-01

    During the past fifty years, more than 1,800 metric tonnes of Pu and substantial quantities of other "minor" actinides, such as Np, Am and Cm, have been generated in nuclear reactors. Some of these transuranic elements can be a source of energy in fission reactions (e.g., 239Pu), a source of fissile material for nuclear weapons (e.g., 239Pu and 237Np), or are of environmental concern because of their long half- lives and radiotoxicity (e.g., 239Pu, t1/2 = 24,100 years, and 237Np, t1/2 = 2.1 million years). There are two basic strategies for the disposition of these elements: 1.) to "burn" or transmute the actinides using nuclear reactors or accelerators; 2.) to "sequester" the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. There has been substantial interest in the use of actinide-bearing minerals, such as zircon or isometric pyrochlore, A2B2O7 (A = rare earths; B = Ti, Zr, Sn, Hf; Fd3m; Z=8), for the immobilization of actinides, particularly plutonium. One of the principal concerns has been the accumulation of structural damage caused by alpha-decay events, particularly from the recoil nucleus. Systematic ion beam irradiation studies of rare-earth pyrochlores have led to the discovery that certain compositions (B = Zr, Hf) are stable to very high fluences of alpha-decay event damage. Some compositions, Gd2Ti2O7, are amorphized at relatively low doses (0.2 displacements per atom, dpa, at room temperature), while other compositions, Gd2Zr2O7, do not amorphize (even at doses of > 40 dpa at 25K), but instead disorder to a defect fluorite structure. By changing the composition of the A-site (e.g., substitution of different rare earth elements), the temperature above which the pyrochlore composition can no longer be amorphized, Tc, varies by >600 K (e.g., Lu2Ti2O7: Tc = 480 K; Gd2Ti2O7: Tc = 1120 K). The variation in response to irradiation as a function of composition can be used to model the long

  14. Destructive analysis capabilities for plutonium and uranium characterization at Los Alamos National Laboratory

    SciTech Connect

    Tandon, Lav; Kuhn, Kevin J; Drake, Lawrence R; Decker, Diana L; Walker, Laurie F; Colletti, Lisa M; Spencer, Khalil J; Peterson, Dominic S; Herrera, Jaclyn A; Wong, Amy S

    2010-01-01

    Los Alamos National Laboratory's (LANL) Actinide Analytical Chemistry (AAC) group has been in existence since the Manhattan Project. It maintains a complete set of analytical capabilities for performing complete characterization (elemental assay, isotopic, metallic and non metallic trace impurities) of uranium and plutonium samples in different forms. For a majority of the customers there are strong quality assurance (QA) and quality control (QC) objectives including highest accuracy and precision with well defined uncertainties associated with the analytical results. Los Alamos participates in various international and national programs such as the Plutonium Metal Exchange Program, New Brunswick Laboratory's (NBL' s) Safeguards Measurement Evaluation Program (SME) and several other inter-laboratory round robin exercises to monitor and evaluate the data quality generated by AAC. These programs also provide independent verification of analytical measurement capabilities, and allow any technical problems with analytical measurements to be identified and corrected. This presentation will focus on key analytical capabilities for destructive analysis in AAC and also comparative data between LANL and peer groups for Pu assay and isotopic analysis.

  15. RAPID METHOD FOR PLUTONIUM, AMERICIUM AND CURIUM IN VERY LARGE SOIL SAMPLES

    SciTech Connect

    Maxwell, S

    2007-01-08

    The analysis of actinides in environmental soil and sediment samples is very important for environmental monitoring. There is a need to measure actinide isotopes with very low detection limits. A new, rapid actinide separation method has been developed and implemented that allows the measurement of plutonium, americium and curium isotopes in very large soil samples (100-200 g) with high chemical recoveries and effective removal of matrix interferences. This method uses stacked TEVA Resin{reg_sign}, TRU Resin{reg_sign} and DGA-Resin{reg_sign} cartridges from Eichrom Technologies (Darien, IL, USA) that allows the rapid separation of plutonium (Pu), americium (Am), and curium (Cm) using a single multistage column combined with alpha spectrometry. The method combines an acid leach step and innovative matrix removal using cerium fluoride precipitation to remove the difficult soil matrix. This method is unique in that it provides high tracer recoveries and effective removal of interferences with small extraction chromatography columns instead of large ion exchange resin columns that generate large amounts of acid waste. By using vacuum box cartridge technology with rapid flow rates, sample preparation time is minimized.

  16. Occurrence of naturally enriched {sup 235}U: Implications for plutonium behavior in natural environments

    SciTech Connect

    Bros, R.; Gauthier-Lafaye, F.; Stille, P.; Turpin, L.; Holliger, Ph.

    1993-03-01

    It is generally accepted that uranium and most of the fission products, with the exception of the alkalis, alkaline earths and rare gases, remained in the irradiated uranium oxides during the nuclear reactions that took place 2.0 Ga ago in the Oklo uranium deposit (Gabon). New isotope investigations show that clay minerals from argillaceous rocks neighboring the natural fission reactor 10 at Oklo have depleted {sup 235}U with {sup 235}U/{sup 238}U ratios ranging between 0.00560 and the common natural value of 0.00725. One sample, however, is enriched in {sup 235}U with a {sup 235}U/{sup 238}U ratio of 0.007682. Leach experiments of this sample with dilute 1N HCl revealed that the {sup 235}U enrichment is actually restricted to the insoluble residue ({sup 235}U/{sup 238}U = 0.010511), whereas the leachate remains depleted in {sup 235}U. This unique discovery of very enriched uranium, together with samarium, neodymium, rubidium, and strontium isotopic analyses, indicate that a small amount of plutonium could have been more mobile than uranium in the reactor 10, and it is suggested that plutonium was incorporated in the crystallographic structure of clay minerals such as the chlorites. 28 refs., 3 figs., 1 tab.

  17. Achievements in testing of the MGA and FRAM isotopic software codes under the DOE/NNSA-IRSN cooperation of gamma-ray isotopic measurement systems

    SciTech Connect

    Vo, Duc; Wang, Tzu - Fang; Funk, Pierre; Weber, Anne - Laure; Pepin, Nicolas; Karcher, Anna

    2009-01-01

    DOE/NNSA and IRSN collaborated on a study of gamma-ray instruments and analysis methods used to perform isotopic measurements of special nuclear materials. The two agencies agreed to collaborate on the project in response to inconsistencies that were found in the various versions of software and hardware used to determine the isotopic abundances of uranium and plutonium. IRSN used software developed internally to test the MGA and FRAM isotopic analysis codes for criteria used to stop data acquisition. The stop-criterion test revealed several unusual behaviors in both the MGA and FRAM software codes.

  18. Characterization of plutonium particles originating from the BOMARC accident - 1960

    NASA Astrophysics Data System (ADS)

    Gostic, Richard Charles

    Within the U.S. arsenal, 32 accidents with nuclear weapons were reported between 1950 and 1980. One of these accidents occurred at McGuire AFB in 1960. A BOMARC missile armed with a nuclear warhead caught on fire and as a result the warhead was destroyed. Sub-millimeter particles consisting of weapons grade plutonium (WGPu) produced by this accident were distributed around the site and remained in the environment for 47 years. Soil cores known to contain WGPu particles produced by this accident were obtained. The particles were localized and removed from the soil with the aid of high resolution computed tomography. The isotopic composition of the particles and the date of manufacture of the Pu were estimated using a combination of alpha and gamma spectroscopy. Scanning electron microscopy was used to study the surface morphology of the particles; energy dispersive spectroscopy and synchrotron based x-ray fluorescence were used to determine the composition and elemental distributions of the particles. The results of these experiments and their application to the field of nuclear forensic analysis are discussed in this thesis.

  19. Interim Storage of Plutonium in Existing Facilities

    SciTech Connect

    Woodsmall, T.D.

    1999-05-10

    'In this era of nuclear weapons disarmament and nonproliferation treaties, among many problems being faced by the Department of Energy is the safe disposal of plutonium. There is a large stockpile of plutonium at the Rocky Flats Environmental Technology Center and it remains politically and environmentally strategic to relocate the inventory closer to a processing facility. Savannah River Site has been chosen as the final storage location, and the Actinide Packaging and Storage Facility (APSF) is currently under construction for this purpose. With the ability of APSF to receive Rocky Flats material an estimated ten years away, DOE has decided to use the existing reactor building in K-Area of SRS as temporary storage to accelerate the removal of plutonium from Rocky Flats. There are enormous cost savings to the government that serve as incentive to start this removal as soon as possible, and the KAMS project is scheduled to receive the first shipment of plutonium in January 2000. The reactor building in K-Area was chosen for its hardened structure and upgraded seismic qualification, both resulting from an effort to restart the reactor in 1991. The KAMS project has faced unique challenges from Authorization Basis and Safety Analysis perspectives. Although modifying a reactor building from a production facility to a storage shelter is not technically difficult, the nature of plutonium has caused design and safety analysis engineers to make certain that the design of systems, structures and components included will protect the public, SRS workers, and the environment. A basic overview of the KAMS project follows. Plutonium will be measured and loaded into DOT Type-B shipping packages at Rocky Flats. The packages are 35-gallon stainless steel drums with multiple internal containment boundaries. DOE transportation vehicles will be used to ship the drums to the KAMS facility at SRS. They will then be unloaded, stacked and stored in specific locations throughout the

  20. 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.

  1. Plutonium process control using an advanced on-line gamma monitor for uranium, plutonium, and americium

    SciTech Connect

    Marsh, S.F.; Miller, M.C.

    1987-05-01

    An on-line gamma monitor has been developed to profile uranium, plutonium, and americium in waste and product streams of the anion exchange process used to recover and purify plutonium at the Los Alamos Plutonium Facility. The gamma monitor employs passive gamma spectrometry to measure /sup 241/Am and /sup 239/Pu, based on their 59.5-keV and 129-keV gamma rays, respectively. Because natural and depleted uranium present in typical process streams have no gamma rays suitable for measurement by such passive methods, uranium measurement requires a novel and less direct technique. Plutonium-241, which is always present in plutonium processed at Los Alamos, decays primarily by beta emission to form /sup 241/Am. However, a small fraction of /sup 241/Pu decays by alpha emission to 6.8-day /sup 237/U. The short half-life and 208-keV gamma energy of /sup 237/U make it an ideal radiotracer to mark the position of macro amounts of uranium impurity in the separation process. The real-time data obtained from an operating process allow operators to optimize many process parameters. The gamma monitor also provides a permanent record of the daily performance of each ion exchange system. 2 refs., 12 figs.

  2. Rapid isolation of plutonium in environmental solid samples using sequential injection anion exchange chromatography followed by detection with inductively coupled plasma mass spectrometry.

    PubMed

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

    2011-01-31

    This paper reports an automated analytical method for rapid determination of plutonium isotopes ((239)Pu and (240)Pu) in environmental solid extracts. Anion exchange chromatographic columns were incorporated in a sequential injection (SI) system to undertake the automated separation of plutonium from matrix and interfering elements. The analytical results most distinctly demonstrated that the crosslinkage of the anion exchanger is a key parameter controlling the separation efficiency. AG 1-×4 type resin was selected as the most suitable sorbent material for analyte separation. Investigation of column size effect upon the separation efficiency revealed that small-sized (2 mL) columns sufficed to handle up to 50 g of environmental soil samples. Under the optimum conditions, chemical yields of plutonium exceeded 90% and the decontamination factors for uranium, thorium and lead ranged from 10(3) to 10(4). The determination of plutonium isotopes in three standard/certified reference materials (IAEA-375 soil, IAEA-135 sediment and NIST-4359 seaweed) and two reference samples (Irish Sea sediment and Danish soil) revealed a good agreement with reference/certified values. The SI column-separation method is straightforward and less labor intensive as compared with batch-wise anion exchange chromatographic procedures. Besides, the automated method features low consumption of ion-exchanger and reagents for column washing and elution, with the consequent decrease in the generation of acidic waste, thus bearing green chemical credentials. PMID:21168558

  3. a Plutonium Ceramic Target for Masha

    NASA Astrophysics Data System (ADS)

    Wilk, P. A.; Shaughnessy, D. A.; Moody, K. J.; Kenneally, J. M.; Wild, J. F.; Stoyer, M. A.; Patin, J. B.; Lougheed, R. W.; Ebbinghaus, B. B.; Landingham, R. L.; Oganessian, Yu. Ts.; Yeremin, A. V.; Dmitriev, S. N.

    2005-09-01

    We are currently developing a plutonium ceramic target for the MASHA mass separator. The MASHA separator will use a thick plutonium ceramic target capable of tolerating temperatures up to 2000 °C. Promising candidates for the target include oxides and carbides, although more research into their thermodynamic properties will be required. Reaction products will diffuse out of the target into an ion source, where they will then be transported through the separator to a position-sensitive focal-plane detector array. Experiments on MASHA will allow us to make measurements that will cement our identification of element 114 and provide for future experiments where the chemical properties of the heaviest elements are studied.

  4. CRITICALITY CURVES FOR PLUTONIUM HYDRAULIC FLUID MIXTURES

    SciTech Connect

    WITTEKIND WD

    2007-10-03

    This Calculation Note performs and documents MCNP criticality calculations for plutonium (100% {sup 239}Pu) hydraulic fluid mixtures. Spherical geometry was used for these generalized criticality safety calculations and three geometries of neutron reflection are: {sm_bullet}bare, {sm_bullet}1 inch of hydraulic fluid, or {sm_bullet}12 inches of hydraulic fluid. This document shows the critical volume and critical mass for various concentrations of plutonium in hydraulic fluid. Between 1 and 2 gallons of hydraulic fluid were discovered in the bottom of HA-23S. This HA-23S hydraulic fluid was reported by engineering to be Fyrquel 220. The hydraulic fluid in GLovebox HA-23S is Fyrquel 220 which contains phosphorus. Critical spherical geometry in air is calculated with 0 in., 1 in., or 12 inches hydraulic fluid reflection.

  5. Concentration and purification of plutonium or thorium

    DOEpatents

    Hayden, John A.; Plock, Carl E.

    1976-01-01

    In this invention a first solution obtained from such as a plutonium/thorium purification process or the like, containing plutonium (Pu) and/or thorium (Th) in such as a low nitric acid (HNO.sub.3) concentration may have the Pu and/or Th separated and concentrated by passing an electrical current from a first solution having disposed therein an anode to a second solution having disposed therein a cathode and separated from the first solution by a cation permeable membrane, the Pu or Th cation permeating the cation membrane and forming an anionic complex within the second solution, and electrical current passage affecting the complex formed to permeate an anion membrane separating the second solution from an adjoining third solution containing disposed therein an anode, thereby effecting separation and concentration of the Pu and/or Th in the third solution.

  6. Plutonium stabilization and handling (PuSH)

    SciTech Connect

    Weiss, E.V.

    1997-01-23

    This Functional Design Criteria (FDC) addresses construction of a Stabilization and Packaging System (SPS) to oxidize and package for long term storage remaining plutonium-bearing special nuclear materials currently in inventory at the Plutonium Finishing Plant (PFP), and modification of vault equipment to allow storage of resulting packages of stabilized SNM for up to fifty years. The major sections of the project are: site preparation; SPS Procurement, Installation, and Testing; storage vault modification; and characterization equipment additions. The SPS will be procured as part of a Department of Energy nationwide common procurement. Specific design crit1460eria for the SPS have been extracted from that contract and are contained in an appendix to this document.

  7. [Plutonium-239 metabolism in chemical skin burns].

    PubMed

    Il'in, L A; Beliaev, I K

    1983-01-01

    Certain peculiarities of metabolism of plutonium-239 were revealed after skin applications there of in solutions of nitrogen acid, tributyl phosphate and hexychloro-butadiene. It was shown that the absorption of plutonium-239 in 0.1 NHO3 solution for 3 days made up 0.02% of the quantity applied. The increase in the acid concentration up to 0.5-10 N was accompanied by a 2.5-5-fold increase in the resorption. The application of the nuclide in organic solvents was characterized by a 4-5-fold increase in its accretion within the body. There was a 25-fold increase in the absorption of 239Pu after the combined effect of the acid and the organic solvents on the skin. PMID:6657939

  8. Spectroscopy of plutonium-organic complexes

    SciTech Connect

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

    1995-12-31

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

  9. 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.

  10. Dose estimates of alternative plutonium pyrochemical processes.

    SciTech Connect

    Kornreich, D. E.; Jackson, J. W.; Boerigter, S. T.; Averill, W. A.; Fasel, J. H.

    2002-01-01

    We have coupled our dose calculation tool Pandemonium with a discrete-event, object-oriented, process-modeling system ProMosO to analyze a set of alternatives for plutonium purification operations. The results follow expected trends and indicate, from a dose perspective, that an experimental flowsheet may warrant further research to see if it can be scaled to industrial levels. Flowsheets that include fluoride processes resulted in the largest doses.

  11. Plutonium Immobilization Program cold pour tests

    SciTech Connect

    Hovis, G.L.; Stokes, M.W.; Smith, M.E.; Wong, J.W.

    1999-07-01

    The Plutonium Immobilization Program (PIP) is a joint venture between the Savannah River Site, Lawrence Livermore National Laboratory, Argonne National Laboratory, and Pacific Northwest National Laboratory to carry out the disposition of excess weapons-grade plutonium. This program uses the can-in-canister (CIC) approach. CIC involves encapsulating plutonium in ceramic forms (or pucks), placing the pucks in sealed stainless steel cans, placing the cans in long cylindrical magazines, latching the magazines to racks inside Defense Waste Processing Facility (DWPF) canisters, and filling the DWPF canisters with high-level waste glass. This process puts the plutonium in a stable form and makes it attractive for reuse. At present, the DWPF pours glass into empty canisters. In the CIC approach, the addition of a stainless steel rack, magazines, cans, and ceramic pucks to the canisters introduces a new set of design and operational challenges: All of the hardware installed in the canisters must maintain structural integrity at elevated (molten-glass) temperatures. This suggests that a robust design is needed. However, the amount of material added to the DWPF canister must be minimized to prevent premature glass cooling and excessive voiding caused by a large internal thermal mass. High metal temperatures, minimizing thermal mass, and glass flow paths are examples of the types of technical considerations of the equipment design process. To determine the effectiveness of the design in terms of structural integrity and glass-flow characteristics, full-scale testing will be conducted. A cold (nonradioactive) pour test program is planned to assist in the development and verification of a baseline design for the immobilization canister to be used in the PIP process. The baseline design resulting from the cold pour test program and CIC equipment development program will provide input to Title 1 design for second-stage immobilization. The cold pour tests will be conducted in two

  12. Surplus Plutonium Disposition (SPD) Environmental Data Summary

    SciTech Connect

    Fledderman, P.D.

    2000-08-24

    This document provides an overview of existing environmental and ecological information at areas identified as potential locations of the Savannah River Site's (SRS) Surplus Plutonium Disposition (SPD) facilities. This information is required to document existing environmental and baseline conditions from which SPD construction and operation impacts can be defined. It will be used in developing the required preoperational monitoring plan to be used at specific SPD facilities construction sites.

  13. Proposed Modification to the Plutonium Systemic Model.

    PubMed

    Konzen, Kevin; Miller, Scott; Brey, Richard

    2015-10-01

    The currently accepted biokinetic model for plutonium distribution within the human body was recommended by the International Commission on Radiological Protection in publication 67. This model was developed from human and animal studies and behavioral knowledge acquired from other known bone-seeking radionuclides. The biokinetic model provides a mathematical means of predicting the distribution, retention, and clearance of plutonium within the human body that may be used in deriving organ, tissue, and whole body dose. This work proposed a modification to the ICRP 67 systemic model for plutonium that incorporated the latest knowledge acquired from recent human injection studies with physiologically based improvements. In summary, the changes included a separation of the liver compartments, removed the intermediate soft tissue-to-bladder pathway, and added pathways from the blood compartment to both the cortical and trabecular bone volumes. The proposed model provided improved predictions for several bioassay indicators compared to the ICRP 67 model while also maintaining its basic structure. Additionally, the proposed model incorporated physiologically based improvements for the liver and skeleton and continued to ensure efficient coupling with intake biokinetic models. PMID:26313589

  14. PLUTONIUM METALLIC FUELS FOR FAST REACTORS

    SciTech Connect

    STAN, MARIUS; HECKER, SIEGFRIED S.

    2007-02-07

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

  15. A Plutonium-Contaminated Wound, 1985, USA

    SciTech Connect

    Doran M. Christensen, DO, REAC /TS Associate Director and Staff Physician Eugene H. Carbaugh, CHP, Staff Scientist, Internal Dosimetry Manager, Pacific Northwest National Laboratory, Richland, Washington

    2012-02-02

    A hand injury occurred at a U.S. facility in 1985 involving a pointed shaft (similar to a meat thermometer) that a worker was using to remove scrap solid plutonium from a plastic bottle. The worker punctured his right index finger on the palm side at the metacarpal-phalangeal joint. The wound was not through-and- through, although it was deep. The puncture wound resulted in deposition of ~48 kBq of alpha activity from the weapons-grade plutonium mixture with a nominal 12 to 1 Pu-alpha to {sup 241}Am-alpha ratio. This case clearly showed that DTPA was very effective for decorporation of plutonium and americium. The case is a model for management of wounds contaminated with transuranics: (1) a team approach for dealing with all of the issues surrounding the incident, including the psychological, (2) early surgical intervention for foreign-body removal, (3) wound irrigation with DTPA solution, and (4) early and prolonged DTPA administration based upon bioassay and in vivo dosimetry.

  16. Plutonium immobilization in glass and ceramics

    SciTech Connect

    Knecht, D.A.; Murphy, W.M.

    1996-05-01

    The Materials Research Society Nineteenth Annual Symposium on the Scientific Basis for Nuclear Waste Management was held in Boston on November 27 to December 1, 1995. Over 150 papers were presented at the Symposium dealing with all aspects of nuclear waste management and disposal. Fourteen oral sessions and on poster session included a Plenary session on surplus plutonium dispositioning and waste forms. The proceedings, to be published in April, 1996, will provide a highly respected, referred compilation of the state of scientific development in the field of nuclear waste management. This paper provides a brief overview of the selected Symposium papers that are applicable to plutonium immobilization and plutonium waste form performance. Waste forms that were described at the Symposium cover most of the candidate Pu immobilization options under consideration, including borosilicate glass with a melting temperature of 1150 {degrees}C, a higher temperature (1450 {degrees}C) lanthanide glass, single phase ceramics, multi-phase ceramics, and multi-phase crystal-glass composites (glass-ceramics or slags). These Symposium papers selected for this overview provide the current status of the technology in these areas and give references to the relevant literature.

  17. Plutonium Immobilization Project -- Robotic canister loading

    SciTech Connect

    Hamilton, R.L.

    2000-01-04

    The Plutonium Immobilization Program (PIP) is a joint venture between the Savannah River Site (SRS), Lawrence Livermore National Laboratory (LLNL), Argonne National Laboratory (ANL), and Pacific Northwest National Laboratory (PNNL). When operational in 2008, the PIP will fulfill the nation's nonproliferation commitment by placing surplus weapons-grade plutonium in a permanently stable ceramic form and making it unattractive for reuse. Since there are significant radiation and security concerns, the program team is developing novel and unique technology to remotely perform plutonium immobilization tasks. The remote task covered in this paper employs a jointed arm robot to load seven 3.5 inch diameter, 135-pound cylinders (magazines) through the 4 inch diameter neck of a stainless steel canister. Working through the narrow canister neck, the robot secures the magazines into a specially designed rack pre-installed in the canister. To provide the deterrent effect, the canisters are filled with a mixture of high-level waste and glass at the Defense Waste Processing Facility (DWPF).

  18. TRACKING SURPLUS PLUTONIUM FROM WEAPONS TO DISPOSITION

    SciTech Connect

    Allender, J.; Beams, J.; Sanders, K.; Myers, L.

    2013-07-16

    Supporting nuclear nonproliferation and global security principles, beginning in 1994 the United States has withdrawn more than 50 metric tons (MT) of government-controlled plutonium from potential use in nuclear weapons. The Department of Energy (DOE), including the National Nuclear Security Administration, established protocols for the tracking of this "excess" and "surplus" plutonium, and for reconciling the current storage and utilization of the plutonium to show that its management is consistent with the withdrawal policies. Programs are underway to ensure the safe and secure disposition of the materials that formed a major part of the weapons stockpile during the Cold War, and growing quantities have been disposed as waste, after which they are not included in traditional nuclear material control and accountability (NMC&A) data systems. A combination of resources is used to perform the reconciliations that form the basis for annual reporting to DOE, to U.S. Department of State, and to international partners including the International Atomic Energy Agency.

  19. 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.

  20. 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

  1. 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.

  2. 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.

  3. Plutonium release from pressed plutonium oxide fuel pellets in aquatic environments

    SciTech Connect

    Patterson, J.H.; Steinkruger, F.J.; Matlack, G.M.; Heaton, R.C.; Coffelt, K.P.; Herrera, B.

    1983-12-01

    Plutonium oxide pellets (80% /sup 238/Pu, 40 g each) were exposed to fresh water and sea water at two temperatures for 3 y in enclosed glass chambers. The concentrations of plutonium observed in the waters increased linearly with time throughout the experiment. However, the observed release rates were inversely dependent on temperature and salinity, ranging from 160 ..mu..Ci/day for cold fresh water to 1.4 ..mu..Ci/day for warm sea water. The total releases, including the chamber residues, showed similar dependencies. A major portion (typically greater than 50%) of the released plutonium passed through a 0.1-..mu..m filter, with even larger fractions (greater than 80%) for the fresh water systems.

  4. Real-time monitoring of plutonium content in uranium-plutonium alloys

    SciTech Connect

    Li, Shelly Xiaowei; Westphal, Brian Robert; Herrmann, Steven Douglas

    2015-09-01

    A method and device for the real-time, in-situ monitoring of Plutonium content in U--Pu Alloys comprising providing a crucible. The crucible has an interior non-reactive to a metallic U--Pu alloy within said interior of said crucible. The U--Pu alloy comprises metallic uranium and plutonium. The U--Pu alloy is heated to a liquid in an inert or reducing atmosphere. The heated U--Pu alloy is then cooled to a solid in an inert or reducing atmosphere. As the U--Pu alloy is cooled, the temperature of the U--Pu alloy is monitored. A solidification temperature signature is determined from the monitored temperature of the U--Pu alloy during the step of cooling. The amount of Uranium and the amount of Plutonium in the U--Pu alloy is then determined from the determined solidification temperature signature.

  5. Precision of gamma-ray measurements of the effective specific power and effective {sup 240}Pu fraction of plutonium

    SciTech Connect

    Sampson, T.E.

    1992-05-01

    This paper uses gamma-ray spectrometry data from replicate measurements on 40 plutonium-bearing samples to examine the repeatability of the effective {sup 240}Pu fraction ({sup 240}Pu{sub eff}) and the effective specific power (P{sub eff}) calculated from the isotopic distribution analyzed with gamma-ray spectrometry codes. The measurements were used to identify the error component arising from repeatability in the determination of the isotopic composition of plutonium in the sample and the contribution of the error component to the uncertainty in total plutonium mass measurements from neutron coincidence counting ({sup 240}Pu{sub eff}) and calorimetry (P{sub eff}). The 40 samples had {sup 240}Pu{sub eff} percentages ranging from 2 to 39% and P{sub eff} values ranging from 2 to 16 mW/g Pu. Four different gamma-ray spectrometry codes (FRAM, MGA, Blue Box, and PUJRC) were used to analyze the data (not all samples were analyzed with each code). All analyses showed that the % relative standard deviation of P{sub eff} was smaller than that of {sup 240}Pu{sub eff}. This result coupled with a cursory examination of uncertainties in coincidence counting of well-characterized samples and water-bath calorimetry errors for the same types of samples lead to the conclusion that smaller uncertainties will be present in the total plutonium mass determined by the combination of calorimetry/gamma-ray spectrometry than in the mass determined by coincidence counting/gamma-ray spectrometry. An additional examination of the biases arising from the {sup 240}Pu correlation used in the gamma-ray spectrometry codes also supported this conclusion. 17 refs.

  6. Initial Report for the Aquifer Background Study: Summary of Uranium and Plutonium Data from INEEL Groundwater Samples

    SciTech Connect

    Robert C. Roback; Don L. Koeppen

    2003-06-01

    As part of the “Aquifer Background Study,” Los Alamos National Laboratory (LANL) under contract with the Idaho National Engineering and Environmental Laboratory (INEEL) has undertaken a study to determine uranium and plutonium abundances and isotopic composition in groundwater samples collected at the INEEL. To date, four samples have been analyzed for uranium and plutonium and an additional nine samples have been analyzed for uranium. It is expected that several more samples will be analyzed for this study. This report summarizes the results from this initial set of samples. Of the 13 samples analyzed for uranium, four samples have 238U/235U ratios that differ from the natural value of 137.88. These four samples and two additional samples also contain 236U at 3-sigma level above detection limits. The presence of 236U and the non-natural 238U/235U ratios unequivocally indicate the presence of anthropic uranium in four of the samples. A small component of anthropic uranium is also present in two additional samples with positive 236U detection but natural 238U/235U isotope ratios. Two of the samples with anthropic uranium, as well as two samples with no detectable anthropic uranium were analyzed for plutonium. No plutonium was detected in these four samples at detection limits of approximately 5E7 239Pu atoms for three of the samples and approximately 1E8 239Pu atoms for the forth sample. These detection limits correspond to (239+240)Pu activity ratios (assuming a 240Pu/239Pu atom ratio of 0.18) of 0.002 and 0.004 pCi/L respectively.

  7. Geomorphology of plutonium in the Northern Rio Grande

    SciTech Connect

    Graf, W.L.

    1993-03-01

    Nearly all of the plutonium in the natural environment of the Northern Rio Grande is associated with soils and sediment, and river processes account for most of the mobility of these materials. A composite regional budget for plutonium based on multi-decadal averages for sediment and plutonium movement shows that 90 percent of the plutonium moving into the system is from atmospheric fallout. The remaining 10 percent is from releases at Los Alamos. Annual variation in plutonium flux and storage exceeds 100 percent. The contribution to the plutonium budget from Los Alamos is associated with relatively coarse sediment which often behaves as bedload in the Rio Grande. Infusion of these materials into the main stream were largest in 1951, 1952, 1957, and 1968. Because of the schedule of delivery of plutonium to Los Alamos for experimentation and weapons manufacturing, the latter two years are probably the most important. Although the Los Alamos contribution to the entire plutonium budget was relatively small, in these four critical years it constituted 71--86 percent of the plutonium in bedload immediately downstream from Otowi.

  8. PLUTONIUM RECOVERY FROM NEUTRON-BOMBARDED URANIUM FUEL

    DOEpatents

    Moore, R.H.

    1962-04-10

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

  9. Weapons-grade plutonium dispositioning. Volume 1: Executive summary

    SciTech Connect

    Parks, D.L.; Sauerbrun, T.J.

    1993-06-01

    The Secretary of Energy requested the National Academy of Sciences (NAS) Committee on International Security and Arms Control to evaluate dispositioning options for weapons-grade plutonium. The Idaho National Engineering Laboratory (INEL) assisted NAS in this evaluation by investigating the technical aspects of the dispositioning options and their capability for achieving plutonium annihilation levels greater than 90%. Additionally, the INEL investigated the feasibility of using plutonium fuels (without uranium) for disposal in existing light water reactors and provided a preconceptual analysis for a reactor specifically designed for destruction of weapons-grade plutonium. This four-volume report was prepared for NAS to document the findings of these studies. Volume 2 evaluates 12 plutonium dispositioning options. Volume 3 considers a concept for a low-temperature, low-pressure, low-power-density, low-coolant-flow-rate light water reactor that quickly destroys plutonium without using uranium or thorium. This reactor concept does not produce electricity and has no other mission than the destruction of plutonium. Volume 4 addresses neutronic performance, fabrication technology, and fuel performance and compatibility issues for zirconium-plutonium oxide fuels and aluminum-plutonium metallic fuels. This volumes gives summaries of Volumes 2--4.

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

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

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

  11. Technical considerations and policy requirements for plutonium management

    SciTech Connect

    Christensen, D.C.; Dinehart, S.M.; Yarbro, S.L.

    1995-12-31

    The goals for plutonium management have changed dramatically over the past few years. Today, the challenge is focused on isolating plutonium from the environment and preparing it for permanent disposition. In parallel, the requirements for managing plutonium are rapidly changing. For example, there is a significant increase in public awareness on how facilities operate, increased attention to environmental safety and health (ES and H) concerns, greater interest in minimizing waste, more emphasis on protecting material from theft, providing materials for international inspection, and a resurgence of interest in using plutonium as an energy source. Of highest concern, in the immediate future, is protecting plutonium from theft or diversion, while the national policy on disposition is debated. These expanded requirements are causing a broadening of responsibilities within the Department of Energy (DOE) to include at least seven organizations. An unavoidable consequence is the divergence in approach and short-term goals for managing similar materials within each organization. The technology base does exist, properly, safely, and cost effectively to extract plutonium from excess weapons, residues, waste, and contaminated equipment and facilities, and to properly stabilize it. Extracting the plutonium enables it to be easily inventoried, packaged, and managed to minimize the risk of theft and diversion. Discarding excess plutonium does not sufficiently reduce the risk of diversion, and as a result, long-term containment of plutonium from the environment may not be able to be proven to the satisfaction of the public.

  12. High temperature adsorption process for solidification of plutonium and neptunium

    SciTech Connect

    Korchenkin, K.; Mashkin, A.; Nardova, A.

    1995-12-31

    The problem of plutonium and neptunium converting into solid form has been considered. It was recently been discovered that plutonium and neptunium absorbed well on inorganic porous matrices (silica gel) under definite conditions. In the work presented in this paper plutonium and neptunium sorption on silica gel followed by calcining saturated granules was experimentally investigated. Calcination may proceed at the different temperatures to give the solid dustless plutonium and neptunium compounds suitable both for controlled temporary storage (with possible return radionuclides in nuclear fuel cycle) and for long life disposal.

  13. Sources and migration of plutonium in groundwater at the Savannah River site.

    PubMed

    Dai, Minhan; Kelley, James M; Buesseler, Ken O

    2002-09-01

    The isotopic composition, size distribution, and redox speciation of plutonium (Pu) in the groundwater in the vicinity of the F-area seepage basins at the U.S. Department of Energy Savannah River Site (SRS) were examined. A low 240Pu/239Pu ratio in the upstream control well signifies a Pu source otherthan global fallout and indicates reactor-produced Pu. Elevated 240Pu/239Pu atom ratios downstream from the seepage basins are due to the decay of transplutonium isotopes, mainly 244Cm to 240Pu, which were generated at the SRS. Evidence suggests that the migration of basin-released Pu isotopes is minor. Rather, it is the transplutonium isotopes that migrate preferentially downstream and in the process decay to yield progeny Pu isotopes. Size fractionation studies with cross-flow ultrafiltration show that <4% of the 239Pu or 240Pu is found in the colloidal fraction, a finding that is consistent with the higher Pu oxidation states observed in the SRS groundwater. The observation of a low abundance of colloid-associated Pu in SRS groundwater cannot be extrapolated to all sites, but is in contrast to the conclusions of prior groundwater Pu studies at the SRS and elsewhere. This work is unique in its application of a novel combination of sampling and processing protocols as well as its use of thermal ionization mass spectrometry for the detection of Pu isotopes. This allows quantification of the Pu source terms and better determination of the ambient Pu size and redox speciation representative of in situ conditions. PMID:12322739

  14. Plutonium and Cesium Colloid Mediated Transport

    NASA Astrophysics Data System (ADS)

    Boukhalfa, H.; Dittrich, T.; Reimus, P. W.; Ware, D.; Erdmann, B.; Wasserman, N. L.; Abdel-Fattah, A. I.

    2013-12-01

    Plutonium and cesium have been released to the environment at many different locations worldwide and are present in spent fuel at significant levels. Accurate understanding of the mechanisms that control their fate and transport in the environment is important for the management of contaminated sites, for forensic applications, and for the development of robust repositories for the disposal of spent nuclear fuel and nuclear waste. Plutonium, which can be present in the environment in multiple oxidations states and various chemical forms including amorphous oxy(hydr)oxide phases, adsorbs/adheres very strongly to geological materials and is usually immobile in all its chemical forms. However, when associated with natural colloids, it has the potential to migrate significant distances from its point of release. Like plutonium, cesium is not very mobile and tends to remain adhered to geological materials near its release point, although its transport can be enhanced by natural colloids. However, the reactivity of plutonium and cesium are very different, so their colloid-mediated transport might be significantly different in subsurface environments. In this study, we performed controlled experiments in two identically-prepared columns; one dedicated to Pu and natural colloid transport experiments, and the other to Cs and colloid experiments. Multiple flow-through experiments were conducted in each column, with the effluent solutions being collected and re-injected into the same column two times to examine the persistence and scaling behavior of the natural colloids, Pu and Cs. The data show that that a significant fraction of colloids were retained in the first elution through each column, but the eluted colloids collected from the first run transported almost conservatively in subsequent runs. Plutonium transport tracked natural colloids in the first run but deviated from the transport of natural colloids in the second and third runs. Cesium transport tracked natural

  15. Use of IsoProbe for Uranium and Plutonium Analysis in Environmental Samples

    SciTech Connect

    Russ, G.P.; Williams, R.

    2000-10-02

    The ability to detect and isotopically characterize uranium and plutonium in environmental samples is of primary importance in the search for nuclear proliferation. The utility of isotope ratio measurements for environmental monitoring is limited by sample preparation costs, measurement precision, and sensitivity. This is particularly true for wide-area monitoring where the number of samples required varies inversely with obtainable precision and sensitivity. This report summarizes an initial evaluation of the applicability of a new technique, magnetic-sector, multicollector, inductively-coupled-plasma mass spectrometry, to environmental sample analysis. This technique is embodied at Lawrence Livermore National Laboratory in the form of a commercially available instrument, the IsoProbe, manufactured by micromass, LTD. (United Kingdom). This is the second of the current generation of such instruments installed in the United States and the first within the Department of Energy complex. Inductively-coupled plasma mass spectrometry (ICPMS) using quadrupole mass filters has existed for roughly 15 years. Magnet sector instruments have also existed for about half that time and multicollector instruments have existed for nearly as long. Among the things that make the new generation of instruments, and the IsoProbe in particular, unique are (1) the use of a gas-collision cell to reduce the energy spread of the ions and to remove ions associated with the plasma gas and (2) the introduction of multiple electron-multiplier detection systems. The net effect of these features is to increase sensitivity and precision. Historically uranium and plutonium isotopic compositions have been determined by thermal ionization mass spectrometry (TIMS). While requiring extensive sample preparation, no other technique matched its precision and sensitivity for such measurements. The purposes of this project are to evaluate whether the IsoProbe can replace TIMS for environmental monitoring

  16. SEPARATION OF PLUTONIUM IONS FROM SOLUTION BY ADSORPTION ON ZIRCONIUM PYROPHOSPHATE

    DOEpatents

    Stoughton, R.W.

    1961-01-31

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

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

    SciTech Connect

    Lavelle, Kevin B.; Miller, Jeffrey L.; Hanson, Susan K.; Connick, William B.; Spitz, Henry B.; Glover, Samuel E.; Oldham, Warren J.

    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.

  18. Combined use of medium mass resolution and desolvation introduction system for accurate plutonium determination in the femtogram range by inductively coupled plasma-sector-field mass spectrometry

    NASA Astrophysics Data System (ADS)

    Pointurier, Fabien; Pottin, Anne-Claire; Hémet, Philippe; Hubert, Amélie

    2011-03-01

    Formation of a polyatomic species made of an atom of a heavy element like lead, mercury or iridium, and atoms abundant in plasma (argon, nitrogen, oxygen, and hydrogen) when using an inductively coupled plasma-sector-field mass spectrometer (ICP-SFMS) may lead to false detection of femtograms (fg) of plutonium or bias in the measured concentrations. Mathematical corrections, based on the measurement of heavy element concentrations in the sample solutions and determination of the extents of formation of the polyatomic interferences, are efficient but time-consuming and degrade detection limits. We describe and discuss a new method based on the combination of, on the one hand, medium mass resolution (MR) of the ICP-SFMS to separate plutonium isotopes physically from interfering polyatomic species, and, on the other, use of a desolvation introduction system (DIS) to enhance sensitivity, thus partly compensating for the loss of transmission due to use of a higher resolution. Plutonium peaks are perfectly separated from the major interfering species (PbO 2, HgAr, and IrO 3) with a mass resolution of ~ 4000. The resulting nine-fold transmission loss is partly compensated by a five-fold increase in sensitivity obtained with the DIS and a lower background. The instrumental detection limits for plutonium isotopes, calculated for measurements of pure synthetic solutions, of the new method (known as MR-DIS method) and of the one currently used in the laboratory (LR method), based on a low mass resolution equal to 360, a microconcentric nebulizer and two in-line cooled spray chambers, are roughly equivalent, at around 0.2 fg ml - 1 . Regarding the measurement of real-life samples, the results obtained with both methods agree and the corresponding analytical detection limits for plutonium isotopes 239Pu, 240Pu and 241Pu are of a few fg·ml - 1 of sample solution, slightly lower with the MR-DIS method than with the current LR method. Although less sensitive than other plutonium

  19. Chemical species of plutonium in Hanford radioactive tank waste

    SciTech Connect

    Barney, G.S.

    1997-10-22

    Large quantities of radioactive wastes have been generated at the Hanford Site over its operating life. The wastes with the highest activities are stored underground in 177 large (mostly one million gallon volume) concrete tanks with steel liners. The wastes contain processing chemicals, cladding chemicals, fission products, and actinides that were neutralized to a basic pH before addition to the tanks to prevent corrosion of the steel liners. Because the mission of the Hanford Site was to provide plutonium for defense purposes, the amount of plutonium lost to the wastes was relatively small. The best estimate of the amount of plutonium lost to all the waste tanks is about 500 kg. Given uncertainties in the measurements, some estimates are as high as 1,000 kg (Roetman et al. 1994). The wastes generally consist of (1) a sludge layer generated by precipitation of dissolved metals from aqueous wastes solutions during neutralization with sodium hydroxide, (2) a salt cake layer formed by crystallization of salts after evaporation of the supernate solution, and (3) an aqueous supernate solution that exists as a separate layer or as liquid contained in cavities between sludge or salt cake particles. The identity of chemical species of plutonium in these wastes will allow a better understanding of the behavior of the plutonium during storage in tanks, retrieval of the wastes, and processing of the wastes. Plutonium chemistry in the wastes is important to criticality and environmental concerns, and in processing the wastes for final disposal. Plutonium has been found to exist mainly in the sludge layers of the tanks along with other precipitated metal hydrous oxides. This is expected due to its low solubility in basic aqueous solutions. Tank supernate solutions do not contain high concentrations of plutonium even though some tanks contain high concentrations of complexing agents. The solutions also contain significant concentrations of hydroxide which competes with other

  20. PLUTONIUM UPTAKE BY PLANTS FROM SOIL CONTAINING PLUTONIUM-238 DIOXIDE PARTICLES

    EPA Science Inventory

    Three plant species--alfalfa, lettuce, and radishes were grown in soils contaminated with plutonium-238 dioxide (238)PuO2 at concentrations of 23, 69, 92, and 342 nanocuries per gram (nCi/g). The length of exposure varied from 60 days for the lettuce and radishes to 358 days for ...