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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

    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.

  4. 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

  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.

    2016-03-01

    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.

  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. 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.

  14. 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

  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. 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.

  13. 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.

  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. 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

  12. 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.

  13. 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

  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. 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.

  2. 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.

  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. 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.

  13. 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

  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

    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.

  4. 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

  5. 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

  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. 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

  5. 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.

  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. 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.

  12. 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.

  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 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.

  17. 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.

  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. 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

  3. 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.

  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. 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)

  9. 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.

  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. 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.

  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. 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.

  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 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)

  3. 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.

  4. 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.

  5. 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.

  6. 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.

  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.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.

  13. 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.

  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. 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.

  20. 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.

  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 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

  10. 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

  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. 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)

  1. PLUTONIUM-URANIUM ALLOY

    DOEpatents

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

    1959-09-01

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

  2. 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.

  3. 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

  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. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  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. 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}.

  11. 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.

  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. 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.

  18. 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.

  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. 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)).

  3. 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

  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