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Sample records for 239pu 240pu 241pu

  1. 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

  2. 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.

  3. Nevada test site fallout atom ratios: /sup 240/Pu//sup 239/Pu and /sup 241/Pu//sup 239/Pu

    SciTech Connect

    Hicks, H.G.; Barr, D.W.

    1984-02-01

    The exposure of the population in Utah to external gamma radiation from the fallout from nuclear weapons tests carried out between 1951 and 1958 at the Nevada Test Site (NTS) has been reconstructed from recent measurements of /sup 137/Cs and plutonium in soil. The fraction of /sup 137/Cs in the fallout from NTS events was calculated from the total plutonium and the /sup 240/Pu//sup 239/Pu ratios measured in the soil, using the values of 0.180 +- 0.006 and 0.032 +- 0.003 for that ratio in global fallout and NTS fallout, respectively. The total population exposure from NTS events was then calculated on the basis of exposure rates resulting from short-lived radionuclides associated with the /sup 137/Cs at the time of deposition. While the /sup 240/Pu//sup 239/Pu ratio is constant in global fallout, this ratio varies greatly in the fallout from individual events. While the composition of fallout on Utah from NTS events is rather uniform, the Off-Site Radiation Exposure Review Project is currently reconstructing radiation exposures for locations close to NTS where the fallout may be predominantly from one event. Therefore, the authors compiled the pertinent ratios in order to provide information concerning the exposure resulting from any individual event. The plutonium ratios measured at 30 days postshot were compiled from unpublished values in the archives of the Nuclear Chemistry Division of LLNL and INC-11 of LANL. These ratios are pertinent to fallout data. Dates for each event were taken from a publication by the Nevada Operations Office of the Department of Energy. 3 references.

  4. Determination of (239)Pu, (240)Pu, (241)Pu and (242)Pu at femtogram and attogram levels - evidence for the migration of fallout plutonium in an ombrotrophic peat bog profile.

    PubMed

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

    2013-04-01

    The isotopic composition of plutonium ((239)Pu, (240)Pu, (241)Pu and (242)Pu) was investigated in a ∼0.5 m long peat core from an ombrotrophic bog (Black Forest, Germany) using clean room procedures and accelerator mass spectrometry (AMS). This sophisticated analytical approach was ultimately needed to detect reliably the Pu concentrations present in the peat samples at femtogram (fg) and attogram (ag) levels. The mean (240)Pu/(239)Pu isotopic ratio of 0.19 ± 0.02 (N = 32) in the peat layers, representing approximately the last 80 years, was in good agreement with the accepted value of 0.18 for the global fallout in the Northern Hemisphere. This finding is largely supported by the corresponding and rather constant (241)Pu/(239)Pu (0.0012 ± 0.0005) and (242)Pu/(239)Pu (0.004 ± 0.001) ratios. Since the Pu isotopic composition characteristic of the global fallout was also identified in peat samples pre-dating the period of atmospheric atom bomb testing (AD 1956-AD 1980), migration of Pu within the peat profile is clearly indicated. These results highlight, for the first time, the mobility of Pu in a peat bog with implications for the migration of Pu in other acidic, organic rich environments such as forest soils and other wetland types. These findings constitute a direct observation of the behaviour of Pu at fg and ag levels in the environment. The AMS measurements of Pu concentrations (referring to a corresponding activity of (240+239)Pu from 0.07 mBq g(-1) to 5 mBq g(-1)) essentially confirm our a priori estimates based on existing (241)Am and (137)Cs data in the investigated peat core and agree well with the global fallout levels from the literature. Exclusively employing the Pu isotope ratios established for the peat samples, the date of the Pu irradiation (AD 1956, correctable to AD 1964) was calculated and subsequently compared to the (210)Pb age of the peat layers; this comparison provided an additional hint that global fallout derived Pu is not fixed in

  5. A method of measurement of (239)Pu, (240)Pu, (241)Pu in high U content marine sediments by sector field ICP-MS and its application to Fukushima sediment samples.

    PubMed

    Bu, Wenting; Zheng, Jian; Guo, Qiuju; Aono, Tatsuo; Tazoe, Hirofumi; Tagami, Keiko; Uchida, Shigeo; Yamada, Masatoshi

    2014-01-01

    An accurate and precise analytical method is highly needed for the determination of Pu isotopes in marine sediments for the long-term marine environment monitoring that is being done since the Fukushima Dai-ichi Nuclear Power Plant accident. The elimination of uranium from the sediment samples needs to be carefully checked. We established an analytical method based on anion-exchange chromatography and SF-ICP-MS in this work. A uranium decontamination factor of 2 × 10(6) was achieved, and the U concentrations in the final sample solutions were typically below 4 pg mL(-1), thus no extra correction of (238)U interferences from the Pu spectra was needed. The method was suitable for the analysis of (241)Pu in marine sediments using large sample amounts (>10 g). We validated the method by measuring marine sediment reference materials and our results agreed well with the certified and the literature values. Surface sediments and one sediment core sample collected after the nuclear accident were analyzed. The characterization of (241)Pu/(239)Pu atom ratios in the surface sediments and the vertical distribution of Pu isotopes showed that there was no detectable Pu contamination from the nuclear accident in the marine sediments collected 30 km off the plant site. PMID:24328266

  6. A method of measurement of (239)Pu, (240)Pu, (241)Pu in high U content marine sediments by sector field ICP-MS and its application to Fukushima sediment samples.

    PubMed

    Bu, Wenting; Zheng, Jian; Guo, Qiuju; Aono, Tatsuo; Tazoe, Hirofumi; Tagami, Keiko; Uchida, Shigeo; Yamada, Masatoshi

    2014-01-01

    An accurate and precise analytical method is highly needed for the determination of Pu isotopes in marine sediments for the long-term marine environment monitoring that is being done since the Fukushima Dai-ichi Nuclear Power Plant accident. The elimination of uranium from the sediment samples needs to be carefully checked. We established an analytical method based on anion-exchange chromatography and SF-ICP-MS in this work. A uranium decontamination factor of 2 × 10(6) was achieved, and the U concentrations in the final sample solutions were typically below 4 pg mL(-1), thus no extra correction of (238)U interferences from the Pu spectra was needed. The method was suitable for the analysis of (241)Pu in marine sediments using large sample amounts (>10 g). We validated the method by measuring marine sediment reference materials and our results agreed well with the certified and the literature values. Surface sediments and one sediment core sample collected after the nuclear accident were analyzed. The characterization of (241)Pu/(239)Pu atom ratios in the surface sediments and the vertical distribution of Pu isotopes showed that there was no detectable Pu contamination from the nuclear accident in the marine sediments collected 30 km off the plant site.

  7. Vertical distributions of radionuclides ((239+240)Pu, (240)Pu/(239)Pu, and (137)Cs) in sediment cores of Lake Bosten in Northwestern China.

    PubMed

    Liao, Haiqing; Bu, Wenting; Zheng, Jian; Wu, Fengchang; Yamada, Masatoshi

    2014-04-01

    Artificial radionuclides ((137)Cs, (239+240)Pu, (241)Pu, (241)Am) deposited in lacustrine sediments have been used for dating as well as radionuclide source identification. In the present work, we investigated the vertical distributions of (239+240)Pu and (137)Cs activities, (240)Pu/(239)Pu atom ratios, and (239+240)Pu/(137)Cs activity ratios in sediment cores collected from Lake Bosten, which is the lake closest to the Lop Nor Chinese Nuclear Weapon Test site in northwestern China. Uniformly high concentrations of (239+240)Pu and (137)Cs were found in the upper layers deposited since 1964 in the sediment cores, and these were controlled by the resuspension of soil containing radionuclides from the nearby land surface. As the Chinese nuclear tests varied remarkably in yield, the mixing of the tropospheric deposition from these tests and the stratospheric deposition of global fallout has led to a (240)Pu/(239)Pu atom ratio that is similar to that of global fallout and to a (239+240)Pu/(137)Cs activity ratio that is slightly higher than that of global fallout. However, a low (240)Pu/(239)Pu atom ratio of 0.080 and high (239+240)Pu/(137)Cs activity ratio of 0.087, significantly different from the global fallout values, were observed in one sediment core (07BS10-2), indicating the inhomogenous tropospheric deposition from the Chinese nuclear tests in Lake Bosten during 1967-1973. These results are important to understand the influence of the CNTs on the radionuclide contamination in Lake Bosten.

  8. 240Pu/239Pu mass ratio in environmental samples in Finland.

    PubMed

    Salminen-Paatero, S; Nygren, U; Paatero, J

    2012-11-01

    The (240)Pu/(239)Pu mass ratio was determined with SF-ICP-MS in lichen, peat, grass, air filter, and hot particle samples obtained in Finland. The main part of the air filters were sampled in northern Finland in 1963, whereas all the other samples were collected in southern and central Finland immediately after the Chernobyl accident in 1986. The (240)Pu/(239)Pu mass ratio varied between 0.13 ± 0.01 and 0.53 ± 0.03 in the environmental samples analyzed. The values for the (240)Pu/(239)Pu ratio confirm previous estimations, based on the (238)Pu/(239+240)Pu alpha activity ratio in the same samples, that global fallout from nuclear weapons testing and deposition from the Chernobyl accident have been the main Pu contamination sources in the environment in Finland. PMID:22776691

  9. Room-temperature electron spectroscopy of 239Pu and 240Pu

    NASA Astrophysics Data System (ADS)

    Ahmad, I.; Kondev, F. G.; Greene, J. P.; Zhu, S.

    2015-06-01

    Passivated, implanted, planar silicon (PIPS) detectors have been used for the measurement of electron spectra. The commercially available PIPS detectors, available in thicknesses of 100 μm, 300 μm, and 500 μm, have an energy resolution (FWHM) of ~ 2.2 keV, which is essentially the same as that of PIN diodes. Alpha and electron spectra of mass-separated 239Pu and 240Pu sources have been measured with a 300-μm thick PIPS detector and the electron to alpha ratios for the conversion lines of the 51.62- and 45.24-keV transitions have been determined. A procedure has been developed to determine the amount of 239Pu and 240Pu in a mixed source. The α-particle emission rate of the mixed source is measured, which is the sum of individual rates. From the electron spectrum of the mixed source, measured with the same setup as the alpha spectrum, the rates of 239Pu electron lines are determined. Using the electron rate of the 239Pu line and the electron to alpha ratio measured for the pure source, the α-particle emission rate of 239Pu is determined. The difference from the total α-particle emission rate gives the α-particle emission rate of 240Pu. In addition, electron intensities and conversion coefficients of the 239Pu and 240Pu transitions have been measured.

  10. Determination of 240Pu/239Pu atom ratio in seawaters from the East China Sea.

    PubMed

    Yamada, Masatoshi; Zheng, Jian

    2011-07-01

    The (240)Pu/(239)Pu atom ratios in seawater samples on the East China Sea continental shelf were measured. These ratios for surface and bottom waters had no significant difference. They were significantly higher than the average global fallout ratio of 0.18. It was proposed that the oceanic currents are accounted for delivery of close-in Pu from the Pacific Proving Grounds (PPG) to the studied areas. The contribution of the PPG close-in fallout was calculated to be 40 % on average. The (240)Pu/(239)Pu atom ratios should provide useful background data before the expected expansion of nuclear power capacity in East and South Asian countries and for distinguishing future sources of Pu.

  11. 240Pu/239Pu isotopic ratios and 239 + 240Pu total measurements in surface and deep waters around Mururoa and Fangataufa atolls compared with Rangiroa atoll (French Polynesia).

    PubMed

    Chiappini, R; Pointurier, F; Millies-Lacroix, J C; Lepetit, G; Hemet, P

    1999-09-30

    The average values of 240Pu/239Pu mass isotopic ratios of plutonium deposited in Mururoa and Fangataufa atoll sediments by French atmospheric nuclear tests range from 3.5 to 5%. In order to assess the near field and far field influence of those deposits in the open ocean, two water profiles were measured for 239 + 240Pu and 240Pu/239Pu using, for the first time, an Inductively Coupled Plasma Mass Spectrometer which was developed to achieve femtogram detection limits. One site was located at the limit of the French territorial waters, which is 22 km distant from Mururoa. The second site was located close to Rangiroa atoll, at a distance of approximately 1200-km from French nuclear test sites. The sample volumes were approximately 500 litres and plutonium was purified prior to mass spectrometry and alpha spectrometry measurements. In Rangiroa, the 239 + 240Pu profile is comparable with those already determined in world open oceans but the maximum detected activity, 9 mBq/m3 at 500-600 m is a lot lower than those measured in the northern hemisphere. 240Pu/239Pu ratios were measured between 500 and 1000 m and were not statistically different from the typical 0.18 +/- 0.01 ratio which characterises the global fallout. Consequently, any influence of plutonium from the tests in Mururoa and Fangataufa is not apparent at Rangiroa. The vertical distribution of 239 + 240Pu near Mururoa shows similar changes with depth but with a slight increase in concentration. 240Pu/239Pu mass ratios vary with depth, from 7 to 10% in the upper 500 m and in the deep waters (below 1000 m) to 15-16% between 600 and 1000 m. A contribution from plutonium deposited in the sediments at Mururoa and Fangataufa is observed at the limit of territorial waters, especially in surface and deep waters.

  12. 239+240Pu concentration and isotope ratio (240Pu/239Pu) in aerosols during high dust (Yellow Sand) period, Korea.

    PubMed

    Choi, Man Sik; Lee, Dong-Soo; Choi, Jae-Cheon; Cha, Hyun-Ju; Yi, Hee-Il

    2006-10-15

    Concentration and isotope ratio of Pu were analyzed for aerosols collected at Anmyeondo located in the western coast of Korea using multiple collector inductively coupled plasma mass spectrometer equipped with desolvated micro-concentric nebulizer. Aerosols were collected from June 2001 to April 2002 using high volume air sampler. The samples consist of high dust samples (Yellow Sand), and also low dust samples; maximum Al concentration was 74.2 microg/m(3) and minimum was 0.17 microg/m(3). Pu was concentrated using 0.1 ml TEVA resin columns after conc. HNO(3) extraction. Isotope dilution using (242)Pu spike and mass bias correction using (233)U and (236)U mixed solution enabled the quantification of Pu and measurement of isotope ratio simultaneously. The contribution of (238)U from both spikes and samples was minimized by careful chemical separation and optimization of spike concentration. The (238)U(1)H and tail contribution on (239)Pu peak were about 0.75 x 10(-5) and 1 x 10(-5) of (238)U intensity, respectively, and they were corrected from (239)Pu using externally determined ((238)U(1)H + tailing)/(238)U ratio and (238)U measurement during acquisition. The detection limits of this analytical procedure were 0.61 fg/ml and 0.56 fg/ml for (239)Pu and (240)Pu, respectively (4 nBq/m(3) and 12 nBq/m(3) for (239)Pu and (240)Pu, respectively). The precision of isotope ratio measurement was better than 2% for larger quantity than 20 fg of (239)Pu. In spring, maximum concentration of 0.580 microBq/m(3) for (239)Pu and 0.404 microBq/m(3) for (240)Pu was observed when Al concentration was maximum, so called as Yellow Sand event. Pu concentrations in aerosols are well correlated with Al, a tracer of soil dust. The ratios of Pu/Al were 0.0082 (microBq/microg) and 0.0055 (microBq/microg) for (239)Pu/Al and (240)Pu/Al, respectively. Isotope ratios of Pu ((240)Pu/(239)Pu) in Yellow Sand samples show 0.191+/-0.014 close to those of global fallout. These facts indicate that

  13. Performance of Cladding on MOX Fuel with Low 240Pu/239Pu Ratio

    SciTech Connect

    McCoy, Kevin; Blanpain, Patrick; Morris, Robert Noel

    2014-01-01

    The U.S. Department of Energy has decided to dispose of a portion of its surplus plutonium by reconstituting it into mixed oxide (MOX) fuel and irradiating it in commercial power reactors. As part of fuel qualification, four lead assemblies were manufactured and irradiated to a maximum fuel rod average burnup of 47.3 MWd/kg heavy metal. This was the world s first commercial irradiation of MOX fuel with a 240Pu/239Pu ratio less than 0.10. Five fuel rods with varying burnups and plutonium contents were selected from one of the assemblies and shipped to Oak Ridge National Laboratory for hot cell examination. This paper discusses the results of those examinations with emphasis on cladding performance. Exams relevant to the cladding included visual and eddy current exams, profilometry, microscopy, hydrogen analysis, gallium analysis, and mechanical testing. There was no discernible effect of the type of MOX fuel on the performance of the cladding.

  14. Measurement of plutonium isotopes, 239Pu and 240Pu, in air-filter samples from Seville (2001-2002)

    NASA Astrophysics Data System (ADS)

    Chamizo, E.; García-León, M.; Enamorado, S. M.; Jiménez-Ramos, M. C.; Wacker, L.

    2010-05-01

    Since the last nuclear atmospheric test carried out by the People Republic of China in 1980 and since the Chernobyl accident in 1986, the plutonium hasn't been directly released into the atmosphere. However, nowadays, it is still present in the troposphere. This is due to plutonium-bearing soil particles physical resuspension processes. In this work, we study for the first time the temporal variation of plutonium isotopes, 239Pu and 240Pu, baseline concentrations on a monthly basis in surface air from Seville (Spain), and their correlation with some tracers of mineral dust, during 2001 and 2002. The Pu analyses were performed by low-energy Accelerator Mass Spectrometry (AMS). The 239Pu plus 240Pu ( 239+240Pu) activity levels achieved maximums during the summer period, characterized by the absence of rains, and minimums during the rainy seasons, laying in the range 1-20 nBq m -3. The 240Pu/ 239Pu two-year average atomic ratio was 0.18 ± 0.03, in agreement with the fallout plutonium. A good correlation with Pu and Al and Ti levels is observed. They are crustal components usually used as tracers of African dust over European countries. The hypothesis of the influence of the Saharan dust intrusions is supported as well through the study of Total Ozone Mass Spectrometer (TOMS) daily images.

  15. Study of neutron-deficient isotopes of Fl in the 239Pu, 240Pu + 48Ca reactions

    NASA Astrophysics Data System (ADS)

    Voinov, A. A.; Utyonkov, V. K.; Brewer, N. T.; Oganessian, Yu Ts; Rykaczewski, K. P.; Abdullin, F. Sh; Dmitriev, S. N.; Grzywacz, R. K.; Itkis, M. G.; Miernik, K.; Polyakov, A. N.; Roberto, J. B.; Sagaidak, R. N.; Shirokovsky, I. V.; Shumeiko, M. V.; Tsyganov, Yu S.; Subbotin, V. G.; Sukhov, A. M.; Sabelnikov, A. V.; Vostokin, G. K.; Hamilton, J. H.; Stoyer, M. A.; Strauss, S. Y.

    2016-07-01

    The results of the experiments aimed at the synthesis of Fl isotopes in the 239Pu + 48Ca and 240Pu + 48Ca reactions are presented. The experiment was performed using the Dubna gas-filled recoil separator at the U400 cyclotron. In the 239Pu+48Ca experiment one decay of spontaneously fissioning 284Fl was detected at 245-MeV beam energy. In the 240Pu+48Ca experiment three decay chains of 285Fl were detected at 245 MeV and four decays were assigned to 284Fl at the higher 48Ca beam energy of 250 MeV. The α-decay energy of 285Fl was measured for the first time and decay properties of its descendants 281Cn, 277Ds, 273Hs, 269Sg, and 265Rf were determined more precisely. The cross section of the 239Pu(48Ca,3n)284Fl reaction was observed to be about 20 times lower than those predicted by theoretical models and 50 times less than the value measured in the 244Pu+48Ca reaction. The cross sections of the 240Pu(48Ca,4-3n)284,285Fl at both 48Ca energies are similar and exceed that observed in the reaction with lighter isotope 239Pu by a factor of 10. The decay properties of the synthesized nuclei and their production cross sections indicate rapid decrease of stability of superheavy nuclei with departing from the neutron number N=184 predicted to be the next magic number.

  16. Determination of Plutonium Activity Concentrations and 240Pu/239Pu Atom Ratios in Brown Algae (Fucus distichus) Collected from Amchitka Island, Alaska.

    SciTech Connect

    Hamilton, T F; Brown, T A; Marchetti, A A; Martinelli, R E; Kehl, S R

    2005-05-02

    Plutonium-239 ({sup 239}Pu) and plutonium-240 ({sup 240}Pu) activity concentrations and {sup 240}Pu/{sup 239}Pu atom ratios are reported for Brown Algae (Fucus distichus) collected from the littoral zone of Amchitka Island (Alaska) and at a control site on the Alaskan peninsula. Plutonium isotope measurements were performed in replicate using Accelerator Mass Spectrometry (AMS). The average {sup 240}Pu/{sup 239}Pu atom ratio observed in dried Fucus d. collected from Amchitka Island was 0.227 {+-} 0.007 (n=5) and compares with the expected {sup 240}Pu/{sup 239}Pu atom ratio in integrated worldwide fallout deposition in the Northern Hemisphere of 0.1805 {+-} 0.0057 (Cooper et al., 2000). In general, the characteristically high {sup 240}Pu/{sup 239}Pu content of Fucus d. analyzed in this study appear to indicate the presence of a discernible basin-wide secondary source of plutonium entering the marine environment. Of interest to the study of plutonium source terms within the Pacific basin are reports of elevated {sup 240}Pu/{sup 239}Pu atom ratios in fallout debris from high-yield atmospheric nuclear tests conducted in the Marshall Islands during the 1950s (Diamond et al., 1960), the wide range of {sup 240}Pu/{sup 239}Pu atom ratio values (0.19 to 0.34) observed in sea water, sediments, coral and other environmental media from the North Pacific Ocean (Hirose et al., 1992; Buesseler, 1997) and updated estimates of the relative contributions of close-in and intermediate fallout deposition on oceanic inventories of radionuclidies, especially in the Northern Pacific Ocean (Hamilton, 2004).

  17. Distribution of nuclear bomb Pu in Nishiyama area, Nagasaki, estimated by accurate and precise determination of 240Pu/239Pu ratio in soils.

    PubMed

    Yoshida, S; Muramatsu, Y; Yamazaki, S; Ban-Nai, T

    2007-01-01

    Plutonium isotopes in forest soils collected in Nishiyama area, Nagasaki, were successfully determined by high resolution inductively coupled plasma mass spectrometry after the treatment with a microwave decomposition system. The (240)Pu/(239)Pu atom ratios observed in the samples in the Nishiyama area were obviously lower than the range of the global fallout. The low ratios (minimum 0.032) observed in Nishiyama area indicated the influence of detonation of the Pu nuclear weapon in 1945. Since the area is contaminated also by global fallout, the (240)Pu/(239)Pu atom ratio can be more sensitive indicator of bomb-derived Pu than Pu activity concentration.

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

    PubMed

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

    2001-10-20

    Nuclear weapons tests conducted by the United States in the Marshall Islands produced significant quantities of regional or tropospheric fallout contamination. Here we report on some preliminary inductively coupled plasma-mass spectrometry (ICP-MS) measurements of plutonium isolated from seven composite soil samples collected from Bikini, Enewetak and Rongelap Atolls in the northern Marshall Islands. These data show that 240Pu/239Pu isotopic signatures in surface soils from the Marshall Island vary significantly and could potentially be used to help quantify the range and extent of fallout deposition (and associated impacts) from specific weapons tests. 137Cs and 60Co were also determined on the same set of soil samples for comparative purposes. PMID:11669263

  19. Determination of (235)U, (239)Pu, (240)Pu, and (241)Am in a nuclear bomb particle using a position-sensitive α-γ coincidence technique.

    PubMed

    Peräjärvi, Kari A; Ihantola, Sakari; Pöllänen, Roy C; Toivonen, Harri I; Turunen, Jani A

    2011-02-15

    A nuclear bomb particle containing 1.6 ng of Pu was investigated nondestructively with a position-sensitive α detector and a broad-energy HPGe γ-ray detector. An event-mode data acquisition system was used to record the data. α-γ coincidence counting was shown to be well suited to nondestructive isotope ratio determination. Because of the very small background, the 51.6 keV γ rays of (239)Pu and the 45.2 keV γ rays of (240)Pu were identified, which enabled isotopic ratio calculations. In the present work, the (239)Pu/((239)Pu+(240)Pu) atom ratio was determined to be 0.950 ± 0.010. The uncertainties were much smaller than in the previous more conventional nondestructive studies on this particle. Obtained results are also in good agreement with the data from the destructive mass spectrometric studies obtained previously by other investigators.

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

    PubMed

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

    1987-04-01

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

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

    SciTech Connect

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

    1987-04-01

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

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

    PubMed

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

    1987-04-01

    On 17 January 1966, an accident during a refueling operation resulted in the destruction of an air force KC-135 tanker and a B-52 bomber carrying four thermonuclear weapons. Two weapons, whose parachutes opened, were found intact. The others experienced non-nuclear explosion with some burning and release of the fissile fuel at impact. Joint efforts by the United States and Spain resulted in remedial action and a long-term program to monitor the effectiveness of the cleanup. Air concentrations of 239Pu and 240Pu have been continuously monitored since the accident. The average annual air concentration for each location was used to estimate committed dose equivalents for individuals living and working around the air sampling stations. The average annual 239Pu and 240Pu air concentrations during the 15-y period corresponding to 1966-1980 and the potential committed dose equivalents for various tissues due to the inhalation of the 239Pu and 240Pu average annual air concentration during this period are shown and discussed in the report. PMID:3570788

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

    PubMed

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

    2013-10-01

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

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

    PubMed

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

    2013-10-01

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

  5. Concentrations of 137Cs, 90Sr, 108m Ag, 239+240 Pu and atom ratio of 240Pu/239Pu in tanner crabs, Chionoecetes japonicus and Chionoecetes opilio collected around Japan.

    PubMed

    Morita, Takami; Ohtsuka, Yoshihito; Fujimoto, Ken; Minamisako, Yoko; Iida, Rika; Nakamura, Masae; Kayama, Toshiharu

    2010-12-01

    The anthropogenic radionuclides, (137)Cs, (90)Sr, (108m)Ag, (239+240)Pu, were measured in two Chionoecetes species, red queen crab (Chionoecetes japonicus) and snow crab (Chionoecetes opilio) collected around Japan during 1996-2007. There was no increase in the concentrations of these radionuclides and no large variation of the atom ratio of (240)Pu/(239)Pu during this research period. These results indicated that the source of the radionuclides was not the radioactive wastes dumped by the former USSR and Russia and originated from past nuclear weapon tests. The higher atom ratio in the crab species than that from global fallout would be contributed by the Pacific Proving Grounds close-in fallout. The variability of the concentration of radionuclides in the crab species would result from the variability of the composition and quantity in the diet. However, the decrease in the concentration of radionuclides with sampling depth would depend on the concentration in the seawater and diet.

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

    DOE PAGES

    Hoover, Andrew S.; Bond, Evelyn M.; Croce, Mark P.; Holesinger, Terry G.; Kunde, Gerd J.; Rabin, Michael W.; Wolfsberg, Laura E.; Bennett, Douglas A.; Hays-Wehle, James P.; Schmidt, Dan R.; et al

    2015-02-27

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

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

    PubMed

    Hoover, Andrew S; Bond, Evelyn M; Croce, Mark P; Holesinger, Terry G; Kunde, Gerd J; Rabin, Michael W; Wolfsberg, Laura E; Bennett, Douglas A; Hays-Wehle, James P; Schmidt, Dan R; Swetz, Daniel; Ullom, Joel N

    2015-04-01

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

  8. 137Cs, 239+240Pu and 240Pu/239Pu atom ratios in the surface waters of the western North Pacific Ocean, eastern Indian Ocean and their adjacent seas.

    PubMed

    Yamada, Masatoshi; Zheng, Jian; Wang, Zhong-Liang

    2006-07-31

    Surface seawater samples were collected along the track of the R/V Hakuho-Maru cruise (KH-96-5) from Tokyo to the Southern Ocean. The (137)Cs activities were determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas, the eastern Indian Ocean, the Bay of Bengal, the Andaman Sea, and the South China Sea. The (137)Cs activities showed a wide variation with values ranging from 1.1 Bq m(-3) in the Antarctic Circumpolar Region of the Southern Ocean to 3 Bq m(-3) in the western North Pacific Ocean and the South China Sea. The latitudinal distributions of (137)Cs activity were not reflective of that of the integrated deposition density of atmospheric global fallout. The removal rates of (137)Cs from the surface waters were roughly estimated from the two data sets of Miyake et al. [Miyake Y, Saruhashi K, Sugimura Y, Kanazawa T, Hirose K. Contents of (137)Cs, plutonium and americium isotopes in the Southern Ocean waters. Pap Meteorol Geophys 1988;39:95-113] and this study to be 0.016 yr(-1) in the Sulu and Indonesian Seas, 0.033 yr(-1) in the Bay of Bengal and Andaman Sea, and 0.029 yr(-1) in the South China Sea. These values were much lower than that in the coastal surface water of the western Northwest Pacific Ocean. This was likely due to less horizontal and vertical mixing of water masses and less scavenging. (239+240)Pu activities and (240)Pu/(239)Pu atom ratios were also determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas and the South China Sea. The (240)Pu/(239)Pu atom ratios ranged from 0.199+/-0.026 to 0.248+/-0.027 on average, and were significantly higher than the global stratospheric fallout ratio of 0.18. The contributions of the North Pacific Proving Grounds close-in fallout Pu were estimated to be 20% for the western North Pacific Ocean, 39% for the Sulu and Indonesian Seas and 42% for the South China Sea by using the two end-member mixing model. The higher (240)Pu/(239)Pu

  9. 137Cs, 239+240Pu and 240Pu/239Pu atom ratios in the surface waters of the western North Pacific Ocean, eastern Indian Ocean and their adjacent seas.

    PubMed

    Yamada, Masatoshi; Zheng, Jian; Wang, Zhong-Liang

    2006-07-31

    Surface seawater samples were collected along the track of the R/V Hakuho-Maru cruise (KH-96-5) from Tokyo to the Southern Ocean. The (137)Cs activities were determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas, the eastern Indian Ocean, the Bay of Bengal, the Andaman Sea, and the South China Sea. The (137)Cs activities showed a wide variation with values ranging from 1.1 Bq m(-3) in the Antarctic Circumpolar Region of the Southern Ocean to 3 Bq m(-3) in the western North Pacific Ocean and the South China Sea. The latitudinal distributions of (137)Cs activity were not reflective of that of the integrated deposition density of atmospheric global fallout. The removal rates of (137)Cs from the surface waters were roughly estimated from the two data sets of Miyake et al. [Miyake Y, Saruhashi K, Sugimura Y, Kanazawa T, Hirose K. Contents of (137)Cs, plutonium and americium isotopes in the Southern Ocean waters. Pap Meteorol Geophys 1988;39:95-113] and this study to be 0.016 yr(-1) in the Sulu and Indonesian Seas, 0.033 yr(-1) in the Bay of Bengal and Andaman Sea, and 0.029 yr(-1) in the South China Sea. These values were much lower than that in the coastal surface water of the western Northwest Pacific Ocean. This was likely due to less horizontal and vertical mixing of water masses and less scavenging. (239+240)Pu activities and (240)Pu/(239)Pu atom ratios were also determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas and the South China Sea. The (240)Pu/(239)Pu atom ratios ranged from 0.199+/-0.026 to 0.248+/-0.027 on average, and were significantly higher than the global stratospheric fallout ratio of 0.18. The contributions of the North Pacific Proving Grounds close-in fallout Pu were estimated to be 20% for the western North Pacific Ocean, 39% for the Sulu and Indonesian Seas and 42% for the South China Sea by using the two end-member mixing model. The higher (240)Pu/(239)Pu

  10. Transuranic concentrations in reef and pelagic fish from the Marshall Islands. [/sup 239/Pu, /sup 240/Pu

    SciTech Connect

    Noshkin, V.E.; Eagle, R.J.; Wong, K.M.; Jokela, T.A.

    1980-09-01

    Concentrations of /sup 239 + 240/Pu are reported in tissues of several species of reef and pelagic fish caught at 14 different atolls in the northern Marshall Islands. Several regularities that are species dependent are evident in the distribution of /sup 239 + 240/Pu among different body tissues. Concentrations in liver always exceeded those in bone and concentrations were lowest in the muscle of all fish analyzed. A progressive discrimination against /sup 239 + 240/Pu was observed at successive trophic levels at all atolls except Bikini and Enewetak, where it was difficult to conclude if any real difference exists between the average concentration factor for /sup 239 + 240/Pu among all fish, which include bottom feeding and grazing herbivores, bottom feeding carnivores, and pelagic carnivores from different atoll locations. The average concentration of /sup 239 + 240/Pu in the muscle of surgeonfish from Bikini and Enewetak was not significantly different from the average concentrations determined in these fish at the other, lesser contaminated atolls. Concentrations among all 3rd, 4th, and 5th trophic level species are highest at Bikini where higher environmental concentrations are found. The reasons for the anomalously low concentrations in herbivores from Bikini and Enewetak are not known.

  11. Determination of 239Pu and 240Pu isotope ratio for a nuclear bomb particle using X-ray spectrometry in conjunction with γ-ray spectrometry and non-destructive α-particle spectrometry

    NASA Astrophysics Data System (ADS)

    Pöllänen, R.; Ruotsalainen, K.; Toivonen, H.

    2009-11-01

    A nuclear bomb particle from Thule containing Pu and U was analyzed using X-ray spectrometry in combination with γ-ray spectrometry and non-destructive α-spectrometry. The main objective was to investigate the possibility to determine the 239Pu and 240Pu isotope ratios. Previously, X-ray spectrometry together with the above-mentioned methods has been successfully applied for radiochemically processed samples, but not for individual particles. In the present paper we demonstrate the power of non-destructive analysis. The 239Pu/( 239Pu+ 240Pu) atom ratio for the Thule particle was determined, using two different approaches, to be 0.93±0.07 and 0.91±0.05. These results are consistent with weapons-grade material and the results obtained by other investigators.

  12. Spatial distribution of (241)Am, (137)Cs, (238)Pu, (239,240)Pu and (241)Pu over 17 year periods in the Ravenglass saltmarsh, Cumbria, UK.

    PubMed

    Oh, J-S; Warwick, P E; Croudace, I W

    2009-01-01

    Ninety five surface scrape samples were collected at the Ravenglass saltmarsh and analysed for radionuclides by alpha spectrometry ((238)Pu and (239,240)Pu), gamma spectrometry ((241)Am and (137)Cs) and liquid scintillation counting ((241)Pu). Both (241)Am and (137)Cs activities are compared with those reported by Horrill [1983. Concentrations and spatial distribution of radioactivity in an ungrazed saltmarsh. In: Coughtrey, P.J. (Ed.), Ecological Aspects of Radionuclide Release. British Ecological Society Special Publication No. 3. Blackwell, Oxford, pp. 119-215.] Significant decreases in activities for both radionuclides were observed which is caused by the declining levels of discharges from the Sellafield nuclear reprocessing plant since the 1980s. It has been concluded that the spatial distribution of these radionuclides are controlled by the tidal currents and the clay contents in the sediments. There is evidence of surface erosion of the saltmarsh and redistribution of radionuclides in the saltmarsh using isotopic ratios of measured Pu.

  13. Spatial distribution of (241)Am, (137)Cs, (238)Pu, (239,240)Pu and (241)Pu over 17 year periods in the Ravenglass saltmarsh, Cumbria, UK.

    PubMed

    Oh, J-S; Warwick, P E; Croudace, I W

    2009-01-01

    Ninety five surface scrape samples were collected at the Ravenglass saltmarsh and analysed for radionuclides by alpha spectrometry ((238)Pu and (239,240)Pu), gamma spectrometry ((241)Am and (137)Cs) and liquid scintillation counting ((241)Pu). Both (241)Am and (137)Cs activities are compared with those reported by Horrill [1983. Concentrations and spatial distribution of radioactivity in an ungrazed saltmarsh. In: Coughtrey, P.J. (Ed.), Ecological Aspects of Radionuclide Release. British Ecological Society Special Publication No. 3. Blackwell, Oxford, pp. 119-215.] Significant decreases in activities for both radionuclides were observed which is caused by the declining levels of discharges from the Sellafield nuclear reprocessing plant since the 1980s. It has been concluded that the spatial distribution of these radionuclides are controlled by the tidal currents and the clay contents in the sediments. There is evidence of surface erosion of the saltmarsh and redistribution of radionuclides in the saltmarsh using isotopic ratios of measured Pu. PMID:19285416

  14. Comparative study of the fragments' mass and energy characteristics in the spontaneous fussion of 238Pu, 240Pu and 242Pu and in the thermal-neutron-induced fission of 239Pu

    NASA Astrophysics Data System (ADS)

    Schillebeeckx, P.; Wagemans, C.; Deruytter, A. J.; Barthélémy, R.

    1992-08-01

    The energy and mass distribution and their correlations have been studied for the spontaneous fission of 238, 240, 242Pu and for the thermal-neutron-induced fission of 239Pu. A comparison of 240Pu(s.f.) and 239Pu(nth,f) shows that the increase in excitation energy mainly results in an increase of the intrinsic excitation energy. A comparison of the results for 238Pu, 240Pu and 242Pu(s.f.) demonstrates the occurence of different fission modes with varying relative probability. These results are discussed in terms of the scission point model as well as in terms of the fission channel model with random neck-rupture.

  15. Ultra-trace determination of (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu by triple quadruple collision/reaction cell-ICP-MS/MS: Establishing a baseline for global fallout in Qatar soil and sediments.

    PubMed

    Amr, Mohamed A; Helal, Abdul-Fattah I; Al-Kinani, Athab T; Balakrishnan, Perumal

    2016-03-01

    The development of practical, fast, and reliable methods for the ultra-trace determination of anthropogenic radionuclides (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu by triple quadruple collision/reaction cell inductively coupled plasma mass spectrometry (CRC-ICP-MS/MS) were investigated in term of its accuracy and precision for producing reliable results. The radionuclides were extracted from 1 kg of the environmental soil samples by concentrated nitric and hydrochloric acids. The leachate solutions were measured directly by triple quadrupole CRC-ICP-MS/MS. For quality assurance, a chemical separation of the concerned radionuclides was conducted and then measured by single quadrupole-ICP-MS. The developed methods were next applied to measure the anthropogenic radionuclides (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu in soil samples collected throughout the State of Qatar. The average concentrations of (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu were 0.606 fg/g (3.364 Bq/kg), 0.619 fg/g (2.038 Bq/kg), 0.034 fg/g (0.0195 Bq/kg), 65.59 fg/g (0.150 Bq/kg), and 12.06 fg/g (0.103 Bq/kg), respectively. PMID:26736181

  16. Ultra-trace determination of (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu by triple quadruple collision/reaction cell-ICP-MS/MS: Establishing a baseline for global fallout in Qatar soil and sediments.

    PubMed

    Amr, Mohamed A; Helal, Abdul-Fattah I; Al-Kinani, Athab T; Balakrishnan, Perumal

    2016-03-01

    The development of practical, fast, and reliable methods for the ultra-trace determination of anthropogenic radionuclides (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu by triple quadruple collision/reaction cell inductively coupled plasma mass spectrometry (CRC-ICP-MS/MS) were investigated in term of its accuracy and precision for producing reliable results. The radionuclides were extracted from 1 kg of the environmental soil samples by concentrated nitric and hydrochloric acids. The leachate solutions were measured directly by triple quadrupole CRC-ICP-MS/MS. For quality assurance, a chemical separation of the concerned radionuclides was conducted and then measured by single quadrupole-ICP-MS. The developed methods were next applied to measure the anthropogenic radionuclides (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu in soil samples collected throughout the State of Qatar. The average concentrations of (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu were 0.606 fg/g (3.364 Bq/kg), 0.619 fg/g (2.038 Bq/kg), 0.034 fg/g (0.0195 Bq/kg), 65.59 fg/g (0.150 Bq/kg), and 12.06 fg/g (0.103 Bq/kg), respectively.

  17. 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

  18. 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

  19. Evaluation of Measurements of 238Pu, 239Pu and 240Pu in Urine at the Microbecquerel Level Using Thermal Ionization Mass Spectrometry and Alpha Spectrometry at Los Alamos National Laboratory: Results of a Two Year Comparison Test (LA-UR-06-8055)

    SciTech Connect

    Bores, Norman; Schultz, Michael K

    2008-01-01

    The Intercomparison Studies Program (ISP) at the Oak Ridge National Laboratory (ORNL, Oak Ridge, TN, USA) provides natural-matrix urine quality-assurance/quality-control (QA/QC) samples to radiobioassay analysis laboratories. In 2003, a single laboratory (Los Alamos National Laboratory LANL, Los Alamos NM USA) requested a change in the test-samples provided previously by the ISP. The change was requested to evaluate measurement performance for analyses conducted using thermal-ionization mass spectrometry (TIMS). Radionuclides included {sup 239}Pu at two activity levels (75-150 {micro}Bq {sm_bullet} sample{sup -1} and 1200-1600 {micro}Bq {sm_bullet} sample{sup -1}) and {sup 238}Pu (3700-7400 {micro}Bq {sm_bullet} sample{sup -1}). In addition, {sup 240}Pu was added to the samples so that the {sup 239+240}Pu specific activity was 3700-7400 {micro}Bq {sm_bullet} sample{sup -1}. In this paper, the results of testing during the period May, 2003 through September, 2005 are presented and discussed.

  20. Vertical distribution of (241)Pu in the southern Baltic Sea sediments.

    PubMed

    Strumińska-Parulska, Dagmara I

    2014-12-15

    The vertical distribution of plutonium (241)Pu in marine sediments can assist in determining the deposition history and sedimentation process of analyzed regions. In addition, (241)Pu/(239+240)Pu activity ratio could be used as a sensitive fingerprint for radioactive source identification. The present preliminary studies on vertical distribution of (241)Pu in sediments from four regions of the southern Baltic Sea are presented. The distribution of (241)Pu was not uniform and depended on sediment geomorphology and depth as well as location. The highest concentrations of plutonium were found in the surface layers of all analyzed sediments and originated from the Chernobyl accident. PMID:25455816

  1. Vertical distribution of (241)Pu in the southern Baltic Sea sediments.

    PubMed

    Strumińska-Parulska, Dagmara I

    2014-12-15

    The vertical distribution of plutonium (241)Pu in marine sediments can assist in determining the deposition history and sedimentation process of analyzed regions. In addition, (241)Pu/(239+240)Pu activity ratio could be used as a sensitive fingerprint for radioactive source identification. The present preliminary studies on vertical distribution of (241)Pu in sediments from four regions of the southern Baltic Sea are presented. The distribution of (241)Pu was not uniform and depended on sediment geomorphology and depth as well as location. The highest concentrations of plutonium were found in the surface layers of all analyzed sediments and originated from the Chernobyl accident.

  2. Measurement of 239Pu in soil and plants in the Nishiyama District of Nagasaki.

    PubMed

    Okajima, S; Shimasaki, T; Kubo, T

    1990-05-01

    Nishiyama district in Nagasaki is located approximately 3000 m east of the hypocenter of the atomic bomb that was dropped on 9 August 1945. This district is also known as an area where there was a concentrated radioactive fallout with the black rain that was carried by a westerly wind. The Nagasaki atomic bomb was a Pu bomb, and the fallout must have included 239Pu without fission in addition to fission products. The presence of 239Pu in Nishiyama district has been confirmed previously. In this study, the distribution of 239 + 240Pu concentration in the uncultivated soil and the transfer factor of 239 + 240Pu to agricultural products in Nishiyama district were examined. The concentration of 239 + 240Pu in the uncultivated soil was 20 Bq kg-1, which was approximately eight times as high as that in the control districts. The transfer factor of 239 + 240Pu to agricultural products was 10(-4) - 10(-3), which was 1/100-1/200 of that of 137Cs.

  3. A multi-radionuclide approach to evaluate the suitability of (239+240)Pu as soil erosion tracer.

    PubMed

    Meusburger, Katrin; Mabit, Lionel; Ketterer, Michael; Park, Ji-Hyung; Sandor, Tarjan; Porto, Paolo; Alewell, Christine

    2016-10-01

    Fallout radionuclides have been used successfully worldwide as tracers for soil erosion, but relatively few studies exploit the full potential of plutonium (Pu) isotopes. Hence, this study aims to explore the suitability of the plutonium isotopes (239)Pu and (240)Pu as a method to assess soil erosion magnitude by comparison to more established fallout radionuclides such as (137)Cs and (210)Pbex. As test area an erosion affected headwater catchment of the Lake Soyang (South Korea) was selected. All three fallout radionuclides confirmed high erosion rates for agricultural sites (>25tha(-1)yr(-1)). Pu isotopes further allowed determining the origin of the fallout. Both (240)Pu/(239)Pu atomic ratios and (239+240)Pu/(137)Cs activity ratios were close to the global fallout ratio. However, the depth profile of the (239+240)Pu/(137)Cs activity ratios in undisturbed sites showed lower ratios in the top soil increments, which might be due to higher migration rates of (239+240)Pu. The activity ratios further indicated preferential transport of (137)Cs from eroded sites (higher ratio compared to the global fallout) to the depositional sites (smaller ratio). As such the (239+240)Pu/(137)Cs activity ratio offered a new approach to parameterize a particle size correction factor that can be applied when both (137)Cs and (239+240)Pu have the same fallout source. Implementing this particle size correction factor in the conversion of (137)Cs inventories resulted in comparable estimates of soil loss for (137)Cs and (239+240)Pu. The comparison among the different fallout radionuclides highlights the suitability of (239+240)Pu through less preferential transport compared to (137)Cs and the possibility to gain information regarding the origin of the fallout. In conclusion, (239+240)Pu is a promising soil erosion tracer, however, since the behaviour i.e. vertical migration in the soil and lateral transport during water erosion was shown to differ from that of (137)Cs, there is a clear

  4. A multi-radionuclide approach to evaluate the suitability of (239+240)Pu as soil erosion tracer.

    PubMed

    Meusburger, Katrin; Mabit, Lionel; Ketterer, Michael; Park, Ji-Hyung; Sandor, Tarjan; Porto, Paolo; Alewell, Christine

    2016-10-01

    Fallout radionuclides have been used successfully worldwide as tracers for soil erosion, but relatively few studies exploit the full potential of plutonium (Pu) isotopes. Hence, this study aims to explore the suitability of the plutonium isotopes (239)Pu and (240)Pu as a method to assess soil erosion magnitude by comparison to more established fallout radionuclides such as (137)Cs and (210)Pbex. As test area an erosion affected headwater catchment of the Lake Soyang (South Korea) was selected. All three fallout radionuclides confirmed high erosion rates for agricultural sites (>25tha(-1)yr(-1)). Pu isotopes further allowed determining the origin of the fallout. Both (240)Pu/(239)Pu atomic ratios and (239+240)Pu/(137)Cs activity ratios were close to the global fallout ratio. However, the depth profile of the (239+240)Pu/(137)Cs activity ratios in undisturbed sites showed lower ratios in the top soil increments, which might be due to higher migration rates of (239+240)Pu. The activity ratios further indicated preferential transport of (137)Cs from eroded sites (higher ratio compared to the global fallout) to the depositional sites (smaller ratio). As such the (239+240)Pu/(137)Cs activity ratio offered a new approach to parameterize a particle size correction factor that can be applied when both (137)Cs and (239+240)Pu have the same fallout source. Implementing this particle size correction factor in the conversion of (137)Cs inventories resulted in comparable estimates of soil loss for (137)Cs and (239+240)Pu. The comparison among the different fallout radionuclides highlights the suitability of (239+240)Pu through less preferential transport compared to (137)Cs and the possibility to gain information regarding the origin of the fallout. In conclusion, (239+240)Pu is a promising soil erosion tracer, however, since the behaviour i.e. vertical migration in the soil and lateral transport during water erosion was shown to differ from that of (137)Cs, there is a clear

  5. Measurement of fallout radionuclides, (239)(,240)Pu and (137)Cs, in soil and creek sediment: Sydney Basin, Australia.

    PubMed

    Smith, B S; Child, D P; Fierro, D; Harrison, J J; Heijnis, H; Hotchkis, M A C; Johansen, M P; Marx, S; Payne, T E; Zawadzki, A

    2016-01-01

    Soil and sediment samples from the Sydney basin were measured to ascertain fallout radionuclide activity concentrations and atom ratios. Caesium-137 ((137)Cs) was measured using gamma spectroscopy, and plutonium isotopes ((239)Pu and (240)Pu) were quantified using accelerator mass spectrometry (AMS). Fallout radionuclide activity concentrations were variable ranging from 0.6 to 26.1 Bq/kg for (137)Cs and 0.02-0.52 Bq/kg for (239+240)Pu. Radionuclides in creek sediment samples were an order of magnitude lower than in soils. (137)Cs and (239+240)Pu activity concentration in soils were well correlated (r(2) = 0.80) although some deviation was observed in samples collected at higher elevations. Soil ratios of (137)Cs/(239+240)Pu (decay corrected to 1/1/2014) ranged from 11.5 to 52.1 (average = 37.0 ± 12.4) and showed more variability than previous studies. (240)Pu/(239)Pu atom ratios ranged from 0.117 to 0.165 with an average of 0.146 (±0.013) and an error weighted mean of 0.138 (±0.001). These ratios are lower than a previously reported ratio for Sydney, and lower than the global average. However, these ratios are similar to those reported for other sites within Australia that are located away from former weapons testing sites and indicate that atom ratio measurements from other parts of the world are unlikely to be applicable to the Australian context. PMID:26344369

  6. Measurement of fallout radionuclides, (239)(,240)Pu and (137)Cs, in soil and creek sediment: Sydney Basin, Australia.

    PubMed

    Smith, B S; Child, D P; Fierro, D; Harrison, J J; Heijnis, H; Hotchkis, M A C; Johansen, M P; Marx, S; Payne, T E; Zawadzki, A

    2016-01-01

    Soil and sediment samples from the Sydney basin were measured to ascertain fallout radionuclide activity concentrations and atom ratios. Caesium-137 ((137)Cs) was measured using gamma spectroscopy, and plutonium isotopes ((239)Pu and (240)Pu) were quantified using accelerator mass spectrometry (AMS). Fallout radionuclide activity concentrations were variable ranging from 0.6 to 26.1 Bq/kg for (137)Cs and 0.02-0.52 Bq/kg for (239+240)Pu. Radionuclides in creek sediment samples were an order of magnitude lower than in soils. (137)Cs and (239+240)Pu activity concentration in soils were well correlated (r(2) = 0.80) although some deviation was observed in samples collected at higher elevations. Soil ratios of (137)Cs/(239+240)Pu (decay corrected to 1/1/2014) ranged from 11.5 to 52.1 (average = 37.0 ± 12.4) and showed more variability than previous studies. (240)Pu/(239)Pu atom ratios ranged from 0.117 to 0.165 with an average of 0.146 (±0.013) and an error weighted mean of 0.138 (±0.001). These ratios are lower than a previously reported ratio for Sydney, and lower than the global average. However, these ratios are similar to those reported for other sites within Australia that are located away from former weapons testing sites and indicate that atom ratio measurements from other parts of the world are unlikely to be applicable to the Australian context.

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

    NASA Astrophysics Data System (ADS)

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

    2010-12-01

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

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

    USGS Publications Warehouse

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

    1998-01-01

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

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

    PubMed

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

    2016-01-01

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

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

    PubMed

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

    2016-01-01

    Anthropogenic (236)U and (239)Pu were measured in European roe deer antlers hunted between 1955 and 1977 which covers and extends beyond the period of intensive nuclear weapons testing (1954-1962). The antlers were hunting trophies, and hence the hunting area, the year of shooting and the approximate age of each animal is given. Uranium and plutonium are known to deposit in skeletal tissue. Since antler histology is similar to bone, both elements were expected in antlers. Furthermore, roe deer shed their antlers annually, and hence antlers may provide a time-resolved environmental archive for fallout radionuclides. The radiochemical procedure is based on a Pu separation step by anion exchange (Dowex 1 × 8) and a subsequent U purification by extraction chromatography using UTEVA(®). The samples were measured by Accelerator Mass Spectrometry at the VERA facility (University of Vienna). In addition to the (236)U and (239)Pu concentrations, the (240)Pu/(239)Pu isotopic ratios were determined with a mean value of 0.172 ± 0.023 which is in agreement with the ratio of global fallout (∼0.18). Rather high (236)U/(238)U ratios of the order of 10(-6) were observed. These measured ratios, where the (236)U arises only from global fallout, have implications for the use of the (236)U/(238)U ratio as a fingerprint for nuclear accidents or releases from nuclear facilities. Our investigations have shown the potential to use antlers as a temporally resolved archive for the uptake of actinides from the environment. PMID:26119579

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

    PubMed

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

    2014-06-01

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

  12. Prompt fission γ -ray spectrum characteristics from 240Pu(sf ) and 242Pu(sf )

    NASA Astrophysics Data System (ADS)

    Oberstedt, S.; Oberstedt, A.; Gatera, A.; Göök, A.; Hambsch, F.-J.; Moens, A.; Sibbens, G.; Vanleeuw, D.; Vidali, M.

    2016-05-01

    In this paper we present first results for prompt fission γ -ray spectra (PFGS) characteristics from the spontaneous fission (sf) of 240Pu and 242Pu. For 242Pu(sf ) we obtained, after proper unfolding of the detector response, an average energy per photon ɛ¯γ=(0.843 ±0.012 ) MeV, an average multiplicity M¯γ=(6.72 ±0.07 ) , and an average total γ -ray energy release per fission E¯γ ,tot = (5.66 ± 0.06) MeV. The 240Pu(sf ) emission spectrum was obtained by applying a so-called detector-response transformation function determined from the 242Pu spectrum measured in exactly the same geometry. The results are an average energy per photon ɛ¯γ=(0.80 ±0.07 ) MeV, the average multiplicity M¯γ = (8.2 ± 0.4), and an average total γ -ray energy release per fission E¯γ ,tot = (6.6 ± 0.5) MeV. The PFGS characteristics for 242Pu(sf ) are in very good agreement with those from thermal-neutron-induced fission on 241Pu and scales well with the corresponding prompt neutron multiplicity. Our results in the case of 240Pu(sf ), although drawn from a limited number of events, show a significantly enhanced average multiplicity and average total energy, but may be understood from a different fragment yield distribution in 240Pu(sf ) compared to that of 242Pu(sf ).

  13. 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.

  14. 239Pu Resonance Evaluation for Thermal Benchmark System Calculations

    NASA Astrophysics Data System (ADS)

    Leal, L. C.; Noguere, G.; de Saint Jean, C.; Kahler, A. C.

    2014-04-01

    Analyses of thermal plutonium solution critical benchmark systems have indicated a deficiency in the 239Pu resonance evaluation. To investigate possible solutions to this issue, the Organisation for Economic Co-operation and Development (OECD) Nuclear Energy Agency (NEA) Working Party for Evaluation Cooperation (WPEC) established Subgroup 34 to focus on the reevaluation of the 239Pu resolved resonance parameters. In addition, the impacts of the prompt neutron multiplicity (νbar) and the prompt neutron fission spectrum (PFNS) have been investigated. The objective of this paper is to present the results of the 239Pu resolved resonance evaluation effort.

  15. Second interlaboratory comparison study for the analysis of 239Pu in synthetic urine at the microBq (-100 aCi) level by mass spectrometry

    SciTech Connect

    McCurdy, D; Lin, Z; Inn, K W; Bell III, R; Wagner, S; Efurd, D W; Steiner, R; Duffy, C; Hamilton, T F; Brown, T A; Marchetti, A A

    2005-01-28

    As a follow up to the initial 1998 intercomparison study, a second study was initiated in 2001 as part of the ongoing evaluation of the capabilities of various ultra-sensitive methods to analyze {sup 239}Pu in urine samples. The initial study was sponsored by the Department of Energy, Office of International Health Programs to evaluate and validate new technologies that may supersede the existing fission tract analysis (FTA) method for the analysis of {sup 239}Pu in urine at the {micro}Bq/l level. The ultra-sensitive techniques evaluated in the second study included accelerator mass spectrometry (AMS) by LLNL, thermal ionization mass spectrometry (TIMS) by LANL and FTA by the University of Utah. Only the results for the mass spectrometric methods will be presented. For the second study, the testing levels were approximately 4, 9, 29 and 56 {micro}Bq of {sup 239}Pu per liter of synthetic urine. Each test sample also contained {sup 240}Pu at a {sup 240}Pu/{sup 239}Pu atom ratio of {approx}0.15 and natural uranium at a concentration of 50 {micro}Bq/ml. From the results of the two studies, it can be inferred that the best performance at the {micro}Bq level is more laboratory specific than method specific. The second study demonstrated that LANL-TIMS and LLNL-AMS had essentially the same quantification level for both isotopes. Study results for bias and precision and acceptable performance compared to ANSI N13.30 and ANSI N42.22 have been compiled.

  16. [ECG indices in dogs after inhalation of 239Pu].

    PubMed

    Karpova, V N

    1985-11-01

    Dogs of both sexes aged 2 to 4 were subjected to inhalation inoculation with polymer 239Pu or submicron 239PuO2 aerosols in amounts close to acute, subacute and chronically effective ones. ECG was recorded in standard, amplified and single leads (V3). All calculations were done by lead II. Signs of the right heart overburdening were noted in the presence of the P-pulmonale complex, deep S1 wave or cardiac electrical axis of SI-SII-SIII type. Signs of the right heart overburdening were revealed after inhalation of polimer 239Pu (70%). The absence of similar changes in damage caused by 239Pu could be attributed to its fast resorption from the lungs resulting in more moderate lesion of the respiratory organs.

  17. Microscopic Calculations of 240Pu Fission

    SciTech Connect

    Younes, W; Gogny, D

    2007-09-11

    Hartree-Fock-Bogoliubov calculations have been performed with the Gogny finite-range effective interaction for {sup 240}Pu out to scission, using a new code developed at LLNL. A first set of calculations was performed with constrained quadrupole moment along the path of most probable fission, assuming axial symmetry but allowing for the spontaneous breaking of reflection symmetry of the nucleus. At a quadrupole moment of 345 b, the nucleus was found to spontaneously scission into two fragments. A second set of calculations, with all nuclear moments up to hexadecapole constrained, was performed to approach the scission configuration in a controlled manner. Calculated energies, moments, and representative plots of the total nuclear density are shown. The present calculations serve as a proof-of-principle, a blueprint, and starting-point solutions for a planned series of more comprehensive calculations to map out a large set of scission configurations, and the associated fission-fragment properties.

  18. Distribution and source of (129)I, (239)(,240)Pu, (137)Cs in the environment of Lithuania.

    PubMed

    Ežerinskis, Ž; Hou, X L; Druteikienė, R; Puzas, A; Šapolaitė, J; Gvozdaitė, R; Gudelis, A; Buivydas, Š; Remeikis, V

    2016-01-01

    Fifty five soil samples collected in the Lithuania teritory in 2011 and 2012 were analyzed for (129)I, (137)Cs and Pu isotopes in order to investigate the level and distribution of artificial radioactivity in Lithuania. The activity and atomic ratio of (238)Pu/((239,24)0)Pu, (129)I/(127)I and (131)I/(137)Cs were used to identify the origin of these radionuclides. The (238)Pu/(239+240)Pu and (240)Pu/(239)Pu ratios in the soil samples analyzed varied in the range of 0.02-0.18 and 0.18-0.24, respectively, suggesting the global fallout as the major source of Pu in Lithuania. The values of 10(-9) to 10(-6) for (129)I/(127)I atomic ratio revealed that the source of (129)I in Lithuania is global fallout in most cases though several sampling sites shows a possible impact of reprocessing releases. Estimated (129)I/(131)I ratio in soil samples from the southern part of Lithuania shows negligible input of the Chernobyl fallout. No correlation of the (137)Cs and Pu isotopes with (129)I was observed, indicating their different sources terms. Results demonstrate uneven distribution of these radionuclides in the Lithuanian territory and several sources of contamination i.e. Chernobyl accident, reprocessing releases and global fallout.

  19. Induction of liver tumors by /sup 239/Pu citrate of /sup 239/PuO/sub 2/ particles in the Chinese hamster

    SciTech Connect

    Brooks, A.L.; Benjamin, S.A.; Hahn, F.F.; Brownstein, D.G.; Griffith, W.C.; McClellan, R.O.

    1983-10-01

    The influence of radiation dose distribution on the frequency of /sup 239/Pu-induced liver tumors was evaluated in the Chinese hamster. Different concentrations of /sup 239/Pu citrate or /sup 239/PuO/sub 2/ particles of known sizes were injected intravenously via the jugular vein. About 60% of the injected /sup 23/Pu citrate was deposited in the liver and 40% in the bone. The /sup 239/Pu citrate was rather uniformly distributed throughout the liver parenchyma. Injected plutonium oxide particles were taken up by the reticuloendothelial system with 90% of the body burden deposited in the liver. The /sup 239/PuO/sub 2/ particles were localized in the Kupffer cells and produced nonuniform dose distributions that were dependent on particle size. There was an activity- and dose-dependent increase in the incidence of total liver parenchymal cell tumors following injection with either plutonium particles or citrate. Plutonium citrate also produced hemangiosarcomas of the liver and tumors in bone and bone marrow. The latent period for liver tumor appearance in animals exposed to /sup 239/Pu citrate or /sup 239/PuO/sub 2/ particles increased as the injected activity decreased. These data indicate that, in Chinese hamster liver, local radiation dose distribution is less important in altering tumor incidence than injected activity or average dose. However, the more uniform irradiation from /sup 239/Pu citrate administration was more effective in cancer production than the nonuniform irradiation from /sup 239/PuO/sub 2/ particle.

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

    PubMed

    Zheng, Jian; Yamada, Masatoshi

    2012-09-01

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

  1. Neutron Resonance Parameters and Covariance Matrix of 239Pu

    SciTech Connect

    Derrien, Herve; Leal, Luiz C; Larson, Nancy M

    2008-08-01

    In order to obtain the resonance parameters in a single energy range and the corresponding covariance matrix, a reevaluation of 239Pu was performed with the code SAMMY. The most recent experimental data were analyzed or reanalyzed in the energy range thermal to 2.5 keV. The normalization of the fission cross section data was reconsidered by taking into account the most recent measurements of Weston et al. and Wagemans et al. A full resonance parameter covariance matrix was generated. The method used to obtain realistic uncertainties on the average cross section calculated by SAMMY or other processing codes was examined.

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

    USGS Publications Warehouse

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

    2004-01-01

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

  3. Bioturbation depths, rates and processes in Massachusetts Bay sediments inferred from modeling of 210Pb and 239 + 240Pu profiles

    USGS Publications Warehouse

    Crusius, John; Bothner, Michael H.; Sommerfield, Christopher K.

    2004-01-01

    Profiles of 210Pb and 239 + Pu from sediment cores collected throughout Massachusetts Bay (water depths of 36-192 m) are interpreted with the aid of a numerical sediment-mixing model to infer bioturbation depths, rates and processes. The nuclide data suggest extensive bioturbation to depths of 25-35 cm. Roughly half the cores have 210Pb and 239 + 240Pu profiles that decrease monotonically from the surface and are consistent with biodiffusive mixing. Bioturbation rates are reasonably well constrained by these profiles and vary from ~0.7 to ~40 cm2 yr-1. As a result of this extensive reworking, however, sediment ages cannot be accurately determined from these radionuclides and only upper limits on sedimentation rates (of ~0.3 cm yr-1) can be inferred. The other half of the radionuclide profiles are characterized by subsurface maxima in each nuclide, which cannot be reproduced by biodiffusive mixing models. A numerical model is used to demonstrate that mixing caused by organisms that feed at the sediment surface and defecate below the surface can cause the subsurface maxima, as suggested by previous work. The deep penetration depths of excess 210Pb and 239 + 240Pu suggest either that the organisms release material over a range of >15 cm depth or that biodiffusive mixing mediated by other organisms is occurring at depth. Additional constraints from surficial sediment 234Th data suggest that in this half of the cores, the vast majority of the present-day flux of recent, nuclide-bearing material to these core sites is transported over a timescale of a month or more to a depth of a few centimeters below the sediment surface. As a consequence of the complex mixing processes, surface sediments include material spanning a range of ages and will not accurately record recent changes in contaminant deposition.

  4. Gamma-ray Output Spectra from 239 Pu Fission

    DOE PAGES

    Ullmann, John

    2015-05-25

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

  5. Gamma-ray Output Spectra from 239Pu Fission

    NASA Astrophysics Data System (ADS)

    Ullmann, John

    2015-05-01

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

  6. Mechanical resuspension of /sup 239/Pu from unpaved roads

    SciTech Connect

    Hodgin, C.R.

    1982-01-01

    The impacts of resuspended plutonium from two unpaved roads at the Rocky Flats Plant on nearby air samplers were investigated. Because the sources were complex fugitive dust emitters and because of the small source-receptor distances, traditional dispersion modeling techniques could not be employed. Thus two specialized techniques, one for fugitive dust emissions and one for near distance dispersion, were developed and used to calculate atmospheric dust concentrations at the subject air samplers. Atmospheric /sup 239/Pu impacts were then determined from measurements of plutonium concentrations in the resuspendible dust on the road surfaces. As a final step in the process the calculated plutonium impacts were compared to the 1980 annual average /sup 239/Pu concentration at four samplers. The impact calculated for the Gunnery Range Road represented 2.1 percent of the observed annual concentration, with a 95 percent confidence interval of 1.1 to 7.9 percent. The Southeast Perimeter Road produced a more substantial effect with a point estimate of 3.8 percent. The 95 percent confidence interval for this source was 2.0 to 9.1 percent. The combined impact of the two roads on the subject samplers was 5.9 percent of the observed plutonium concentration, with a 95 percent confidence interval of 3.2 to 17.0 percent. Thus it was shown that fugitive plutonium emissions from the Gunnery Range Road and Southeast Perimeter Road are not substantial contributors to the plutonium concentrations observed at the subject samplers. Even an increase in dust control efficiency to 90 percent (as with paving) would result in only a four percent decrease in the overall atmosperic plutonium concentration at the site.

  7. Chronic cigarette smoke exposure increases the pulmonary retention and radiation dose of {sup 239}Pu inhaled as {sup 239}PuO{sub 2} by F344 rats

    SciTech Connect

    Finch, G.L.; Lundgren, D.L.; Barr, E.B.; Chen, B.T.; Griffith, W.C.; Hobbs, C.H.; Hoover, M.D.; Nikula, K.J.; Mauderly, J.L.

    1998-12-01

    As a portion of a study to examine how chronic cigarette smoke exposure might alter the risk of lung tumors from inhaled {sup 239}PuO{sub 2} in rats, the effects of smoke exposure on alpha-particle lung dosimetry over the life-span of exposed rats were determined. Male and female rats were exposed to inhaled {sup 239}PuO{sub 2} alone or in combination with cigarette smoke. Animals exposed to filtered air along served as controls for the smoke exposure. Whole-body exposure to mainstream smoke diluted to concentrations of either 100 or 250 mg total particulate matter m{sup {minus}3} began at 6 wk of age and continued for 6 h d{sup {minus}1}, 5 d wk{sup {minus}1}, for 30 mo. A single, pernasal, acute exposure to {sup 239}PuO{sub 2} was given to all rats at 12 wk of age. Exposure to cigarette smoke caused decreased body weight gains in a concentration dependent manner. Lung-to-body weight ratios were increased in smoke-exposed rats. Rats exposed to cigarette smoke before the {sup 239}PuO{sub 2} exposure deposited less {sup 239}Pu in the lung than did controls. Except for male rats exposed to LCS, exposure to smoke retarded the clearance of {sup 239}Pu from the lung compared to control rats through study termination at 870 d after {sup 239}PuO{sub 2} exposure. Radiation doses to lungs were calculated by sex and by exposure group for rats on study for at least 360 d using modeled body weight changes, lung-to-body weight ratios, and standard dosimetric calculations. For both sexes, estimated lifetime radiation doses from the time of {sup 239}PuO{sub 2} exposure to death were 3.8 Gy, 4.4 Gy, or 6.7 Gy for the control, LCS, or HCS exposure groups, respectively. Assuming an approximately linear dose-response relationship between radiation dose and lung neoplasm incidence, approximate increases of 20% or 80% in tumor incidence over controls would be expected in rats exposed to {sup 239}PuO{sub 2} and LCS or {sup 239}PuO{sub 2} and HCS, respectively.

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

    PubMed

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

    2016-01-01

    The isotopes (236)U, (239)Pu and (240)Pu are present in surface soils as a result of global fallout from nuclear weapons tests carried out in the 1950's and 1960's. These isotopes potentially constitute artificial tracers of recent soil erosion and sediment movement. Only Accelerator Mass Spectrometry has the requisite sensitivity to measure all three isotopes at these environmental levels. Coupled with its relatively high throughput capabilities, this makes it feasible to conduct studies of erosion across the geographical extent of the Australian continent. In the Australian context, however, global fallout is not the only source of these isotopes. As part of its weapons development program the United Kingdom carried out a series of atmospheric and surface nuclear weapons tests at Maralinga, South Australia in 1956 and 1957. The tests have made a significant contribution to the Pu isotopic abundances present in the region around Maralinga and out to distances ∼1000 km, and impact on the assessment techniques used in the soil and sediment tracer studies. Quantification of the relative fallout contribution derived from detonations at Maralinga is complicated owing to significant contamination around the test site from numerous nuclear weapons safety trials that were also carried out around the site. We show that (236)U can provide new information on the component of the fallout that is derived from the local nuclear weapons tests, and highlight the potential of (236)U as a new fallout tracer. PMID:26141189

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

    PubMed

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

    2016-01-01

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

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

    PubMed

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

    2016-07-01

    Atmospheric nuclear weapons testing (NWT) resulted in the injection of plutonium (Pu) into the atmosphere and subsequent global deposition. We present a new method for continuous semiquantitative measurement of (239)Pu in ice cores, which was used to develop annual records of fallout from NWT in ten ice cores from Greenland and Antarctica. The (239)Pu was measured directly using an inductively coupled plasma-sector field mass spectrometer, thereby reducing analysis time and increasing depth-resolution with respect to previous methods. To validate this method, we compared our one year averaged results to published (239)Pu records and other records of NWT. The (239)Pu profiles from the Arctic ice cores reflected global trends in NWT and were in agreement with discrete Pu profiles from lower latitude ice cores. The (239)Pu measurements in the Antarctic ice cores tracked low latitude NWT, consistent with previously published discrete records from Antarctica. Advantages of the continuous (239)Pu measurement method are (1) reduced sample preparation and analysis time; (2) no requirement for additional ice samples for NWT fallout determinations; (3) measurements are exactly coregistered with all other chemical, elemental, isotopic, and gas measurements from the continuous analytical system; and (4) the long half-life means the (239)Pu record is stable through time. PMID:27244483

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

    PubMed

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

    2016-07-01

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

  12. Prompt Fission Neutron Emission in Resonance Fission of 239Pu

    SciTech Connect

    Hambsch, Franz-Josef; Oberstedt, Stephan; Varapai, Natallia; Serot, Olivier

    2005-05-24

    The prompt neutron emission probability from neutron-induced fission in the resonance region is being investigated at the time-of-flight facility GELINA of the IRMM. A double Frisch-gridded ionization chamber is used as a fission-fragment detector. For the data acquisition of both the fission-fragment signals as well as the neutron detector signals the fast digitization technique has been applied. For the neutron detection, large-volume liquid scintillation detectors from the DEMON collaboration are used. A specialized data analysis program taking advantage of the digital filtering technique has been developed to treat the acquired data.Neutron multiplicity investigations for actinides, especially in resonance neutron-induced fission, are rather scarce. They are, however, important for reactor control and safety issues as well as for understanding the basic physics of the fission process. Fission yield measurements on both 235U and 239Pu without prompt neutron emission coincidence have shown that fluctuation of the fission-fragment mass distribution exists from resonance to resonance, larger in the case of 235U. To possibly explain these observations, the question now is whether the prompt neutron multiplicity shows similar fluctuations with resonance energy.

  13. Osteosarcomas among beagles exposed to /sup 239/Pu

    SciTech Connect

    Whittemore, A.S.; McMillan, A.

    1982-04-01

    A Weibull distribution was fit to the osteosarcoma death times of beagles given single intravenous injections of /sup 239/Pu. For injected doses in the range 0-1..mu..Ci/kg the osteosarcoma incidence rate h(t) at t days after injection can be fit by a quadratic function of injected dose d: h(t) = 2.61 X 10/sup -18/ d/sup 2/t/sup 4.91/. The best-fitting linear function was rejected by the data (P < 0.001). A different formula for h(t), derived from a multistage theory for osteosarcoma induction, was also fit to these data. For this purpose microdosimetry calculations were used to estimate the dose to the cells at risk in the endosteal layer (endosteal dose). According to the best fit, h(t) is a quadratic function of endosteal dose at low doses. A linear dose-response relationship was again rejected. The absence of a linear component at low doses might be explained by the fact that 108 of the 185 animals injected at the lowest doses (<0.02 ..mu..Ci/kg) were still alive at the time these data were collected.

  14. Characterization of Pu concentration and its isotopic composition in a reference fallout material.

    PubMed

    Zhang, Yongsan; Zheng, Jian; Yamada, Masatoshi; Wu, Fengchang; Igarashi, Yasuhito; Hirose, Katsumi

    2010-02-01

    Because there is no reference material for fallout plutonium isotope monitoring, preparation of such a material is necessary for quality control of fallout radionuclides analysis for atmospheric environmental studies. In this work, we report the characterization of Pu activity and its isotopic composition in a reference fallout material prepared by the Meteorological Research Institute (MRI), Japan. This material was prepared from samples collected at 14 stations throughout Japan in 1963-1979, with reference values of (137)Cs, (90)Sr and (239)(+)(240)Pu activities. We analyzed the activities of (239)(+)(240)Pu and (241)Pu, and the atom ratios of (240)Pu/(239)Pu and (241)Pu/(239)Pu using an isotope dilution sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS). The (239)(+)(240)Pu activities in this fallout material using acid leaching and total digestion were 6.56+/-0.20 mBq/g and 6.79+/-0.16 mBq/g, respectively. Atom ratios of (240)Pu/(239)Pu were 0.1915+/-0.0030 and 0.1922+/-0.0044, respectively. Both (240)Pu/(239)Pu and (241)Pu/(239)Pu atom ratios were slightly higher than those of global fallout, which could be attributed to the deposition of fallout radionuclides resulting from the Chinese nuclear weapons tests conducted in the 1970s. The dominant host phases of (239)(+)(240)Pu were found to be organic matter-sulfides (70%) with a relative high (240)Pu/(239)Pu atom ratio, and Fe-Mn oxides (19%) using a sequential extraction method.

  15. A comparison of fallout (236)U and (239)Pu uptake by Australian vegetation.

    PubMed

    Froehlich, M B; Dietze, M M A; Tims, S G; Fifield, L K

    2016-01-01

    The isotopes (236)U and (239)Pu, both produced during nuclear weapons tests carried out in the 1950s and 1960s, are present in the environment and may be used as tracers for soil erosion studies. Although these radionuclides occur only at ultra-trace levels in nature, they can be readily measured by accelerator mass spectrometry with the 14UD heavy ion accelerator at the Australian National University. We have analysed a series of vegetation samples for their (236)U and (239)Pu concentration and compared the results with those found in the surrounding soil. (236)U could be measured in all collected samples whereas (239)Pu could not be detected in several vegetation samples due to its very low concentration, although it was readily detectable in the soil. We find that, relative to plutonium, (236)U is preferentially taken up by plants with enrichment factors ((236)U/(239)Pu)veg/((236)U/(239)Pu)soil that range between 7 and 52 in the present study. PMID:26141188

  16. A comparison of fallout (236)U and (239)Pu uptake by Australian vegetation.

    PubMed

    Froehlich, M B; Dietze, M M A; Tims, S G; Fifield, L K

    2016-01-01

    The isotopes (236)U and (239)Pu, both produced during nuclear weapons tests carried out in the 1950s and 1960s, are present in the environment and may be used as tracers for soil erosion studies. Although these radionuclides occur only at ultra-trace levels in nature, they can be readily measured by accelerator mass spectrometry with the 14UD heavy ion accelerator at the Australian National University. We have analysed a series of vegetation samples for their (236)U and (239)Pu concentration and compared the results with those found in the surrounding soil. (236)U could be measured in all collected samples whereas (239)Pu could not be detected in several vegetation samples due to its very low concentration, although it was readily detectable in the soil. We find that, relative to plutonium, (236)U is preferentially taken up by plants with enrichment factors ((236)U/(239)Pu)veg/((236)U/(239)Pu)soil that range between 7 and 52 in the present study.

  17. Sensitivities of five alpha continuous air monitors for detection of airborne sup 239 Pu

    SciTech Connect

    McIsaac, C.V.; Amaro, C.R.

    1992-07-01

    Results of measurements of the sensitivities of five alpha continuous air monitors (CAMs) for detection of airborne {sup 239}Pu are presented. Four commercially available alpha CAMs (Kurz model 8311, Merlin Gerin Edgar, RADeCO model 452, and Victoreen model 758) and a prototype alpha CAM currently in use at Argonne National Laboratory- West (ANL-W) were tested sampling natural ambient air and laboratory-generated atmospheres laden with either blank dust or dust containing nCi/g concentrations of {sup 239}Pu. Cumulative alpha spectra were stored at 30 or 60 minute intervals during each sampling and were subsequently analyzed using three different commonly used alpha spectrum analysis algorithms. The effect of airborne dust concentration and sample filter porosity on detector resolution and sensitivity for airborne {sup 239}Pu are described.

  18. Sensitivities of five alpha continuous air monitors for detection of airborne {sup 239}Pu

    SciTech Connect

    McIsaac, C.V.; Amaro, C.R.

    1992-07-01

    Results of measurements of the sensitivities of five alpha continuous air monitors (CAMs) for detection of airborne {sup 239}Pu are presented. Four commercially available alpha CAMs (Kurz model 8311, Merlin Gerin Edgar, RADeCO model 452, and Victoreen model 758) and a prototype alpha CAM currently in use at Argonne National Laboratory- West (ANL-W) were tested sampling natural ambient air and laboratory-generated atmospheres laden with either blank dust or dust containing nCi/g concentrations of {sup 239}Pu. Cumulative alpha spectra were stored at 30 or 60 minute intervals during each sampling and were subsequently analyzed using three different commonly used alpha spectrum analysis algorithms. The effect of airborne dust concentration and sample filter porosity on detector resolution and sensitivity for airborne {sup 239}Pu are described.

  19. Characterization of (241)Pu occurrence, distribution, and bioaccumulation in seabirds from northern Eurasia.

    PubMed

    Strumińska-Parulska, Dagmara I; Skwarzec, Bogdan

    2015-05-01

    The paper presents unique data of plutonium (241)Pu study in seabirds from northern Eurasia, permanently or temporally living at the southern Baltic Sea coast. Together, ten marine birds species were examined, as follows: three species that permanently reside at the southern Baltic, four species of wintering birds, and three species of migrating birds; 366 samples were analyzed. The obtained results indicated plutonium was non-uniformly distributed in organs and tissues of analyzed seabirds. The highest (241)Pu content was found in the digestion organs and feathers, the lowest in muscles. Also, the internal radiation doses from (241)Pu were evaluated.

  20. Potential of Vetiveria zizanoides L. Nash for phytoremediation of plutonium ((239)Pu): Chelate assisted uptake and translocation.

    PubMed

    Singh, Shraddha; Fulzele, D P; Kaushik, C P

    2016-10-01

    Plants have demonstrated a great potential to remove toxic elements from soils and solutions and been successfully used for phytoremediation of important radionuclides. Uptake potential of vetiver plants (V. zizanoides) for the remediation of (239)Pu in hydroponic and soil conditions was studied in the present work. High efficiency of V. zizanoides for the removal of (239)Pu was recorded with 66.2% being removed from the hydroponic solution after 30 days. However, remediation of (239)Pu from soil was limited. Remediation of (239)Pu from soil was increased with the addition of chelating agents citric acid (CA) and diethylenetriaminepentaacetic acid (DTPA). Accumulation of (239)Pu was recorded higher in roots than shoots, however its translocation from roots to shoots increased in the presence of chelators in hydroponic as well as soil conditions. DTPA was found more effective than CA showing higher translocation index (TI). Increase in TI was observed 8 and 6 times in the solution and soil respectively when plants were exposed to (239)Pu-DTPA in comparison to only (239)Pu. The present study demonstrates that V. zizanoides plant is a potential plant for phytoremediation of (239)Pu. PMID:27318195

  1. Potential of Vetiveria zizanoides L. Nash for phytoremediation of plutonium ((239)Pu): Chelate assisted uptake and translocation.

    PubMed

    Singh, Shraddha; Fulzele, D P; Kaushik, C P

    2016-10-01

    Plants have demonstrated a great potential to remove toxic elements from soils and solutions and been successfully used for phytoremediation of important radionuclides. Uptake potential of vetiver plants (V. zizanoides) for the remediation of (239)Pu in hydroponic and soil conditions was studied in the present work. High efficiency of V. zizanoides for the removal of (239)Pu was recorded with 66.2% being removed from the hydroponic solution after 30 days. However, remediation of (239)Pu from soil was limited. Remediation of (239)Pu from soil was increased with the addition of chelating agents citric acid (CA) and diethylenetriaminepentaacetic acid (DTPA). Accumulation of (239)Pu was recorded higher in roots than shoots, however its translocation from roots to shoots increased in the presence of chelators in hydroponic as well as soil conditions. DTPA was found more effective than CA showing higher translocation index (TI). Increase in TI was observed 8 and 6 times in the solution and soil respectively when plants were exposed to (239)Pu-DTPA in comparison to only (239)Pu. The present study demonstrates that V. zizanoides plant is a potential plant for phytoremediation of (239)Pu.

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

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

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

  3. Influence of thermal and resonance neutron on fast neutron flux measurement by 239Pu fission chamber

    NASA Astrophysics Data System (ADS)

    Zeng, Li-Na; Wang, Qiang; Song, Ling-Li; Zheng, Chun

    2015-01-01

    The 239Pu fission chambers are widely used to measure fission spectrum neutron flux due to a flat response to fast neutrons. However, in the meantime the resonance and thermal neutrons can cause a significant influence on the measurement if they are moderated, which could be eliminated by using 10B and Cd covers. At a column enriched uranium fast neutron critical assembly, the fission reaction rates of 239Pu are measured as 1.791×10-16, 2.350×10-16 and 1.385×10-15 per second for 15 mm thick 10B cover, 0.5 mm thick Cd cover, and no cover respectively, while the fission reaction rate of 239Pu is rapidly increased to 2.569×10-14 for a 20 mm thick polythene covering fission chamber. The average 239Pu fission cross-section of thermal and resonance neutrons is calculated to be 500 b and 24.95 b with the assumption of 1/v and 1/E spectra respectively, then thermal, resonance and fast neutron flux are achieved to be 2.30×106, 2.24×106 and 1.04×108 cm-2·s-1.

  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.

  5. 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.

  6. 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

  7. 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

  8. Determination of /sup 239,240/Pu in bottom sediments of the Baltic Sea

    SciTech Connect

    Kuznetsov, Yu.V.; Legin, V.K.; Pospelov, Yu.N.; Simonyak, Z.N.

    1988-11-01

    We present a technique for determining the /sup 239,240/Pu content, using /sup 236/Pu as the monitor of chemical yield, in samples of soils and bottom sediments - objects of the external environment. Plutonium is extracted from the matrix material by leaching with a mixture of concentrated acids HCl-HNO/sub 3/, after which it is separated by ion-exchange methods. After electrodeposition onto stainless steel discs the activity of the nuclides of plutonium is measured by the method of alpha-spectrometry. The average chemical yields during the analysis of the samples was 40-60%, the relative standard deviation was 10%, and the lower limit of detectability was 0.3 Bq. We present results of the determination of the /sup 239,240/Pu content in surface samples of bottom sediments from the Gulf of Finland and that past of the Baltic Sea which adjoins the territory of the USSR. It is found that the unit activity of /sup 239,240/Pu in the bottom sediments varies within the limits of 0.4-1.2 Bq/kg and lies at the global level. Global genesis of /sup 239,240/Pu in the bottom sediments of the Gulf of Finland and the open parts of the Baltic Sea is also confirmed by the values which are found for the ratios /sup 238/Pu//sup 239,240/Pu and /sup 239,240/Pu//sup 137/Cs.

  9. Measurement of fallout {sup 239}Pu levels in urine samples by fission track analysis

    SciTech Connect

    Moorthy, A.R.; Doty, R.M.

    1996-11-01

    A Fission Track Analysis (FTA) method for assessing 239Pu in urine samples was first developed at Brookhaven National Laboratory (BNL) in 1988; it then had a detection limit of 100 aCi (3.7 {micro}Bq). Since that time, several steps were introduced that increased chemical recovery and lowered the detection limit to less than 1O aCi per sample. These improvements include a process of micro-column separation of plutonium in the final stages. The improved FTA method was applied to 22 urine samples from male staff at BNL. The results showed that 239Pu from fallout excreted in urine was 33 +/- 11 aCi (1.2 {micro}Bq) per day.

  10. Determination of 241Pu in nuclear waste slurries: a comparative study using LSC and ICP-MS.

    PubMed

    Jäggi, M; Röllin, S; Alvarado, J A Corcho; Eikenberg, J

    2012-02-01

    (241)Pu was determined in slurry samples from a nuclear reactor decommissioning project at the Paul Scherrer Institute (Switzerland). To validate the results, the (241)Pu activities of five samples were determined by LSC (TriCarb and Quantulus) and ICP-MS, with each instrument at a different laboratory. In lack of certified reference materials for (241)Pu, the methods were further validated using the (241)Pu information values of two reference sediments (IAEA-300 and IAEA-384). Excellent agreement with the results was found between LSC and ICP-MS in the nuclear waste slurries and the reference sediments.

  11. Determination of 241Pu in nuclear waste slurries: a comparative study using LSC and ICP-MS.

    PubMed

    Jäggi, M; Röllin, S; Alvarado, J A Corcho; Eikenberg, J

    2012-02-01

    (241)Pu was determined in slurry samples from a nuclear reactor decommissioning project at the Paul Scherrer Institute (Switzerland). To validate the results, the (241)Pu activities of five samples were determined by LSC (TriCarb and Quantulus) and ICP-MS, with each instrument at a different laboratory. In lack of certified reference materials for (241)Pu, the methods were further validated using the (241)Pu information values of two reference sediments (IAEA-300 and IAEA-384). Excellent agreement with the results was found between LSC and ICP-MS in the nuclear waste slurries and the reference sediments. PMID:22079960

  12. Prompt γ-ray production in neutron-induced fission of 239Pu

    NASA Astrophysics Data System (ADS)

    Ullmann, J. L.; Bond, E. M.; Bredeweg, T. A.; Couture, A.; Haight, R. C.; Jandel, M.; Kawano, T.; Lee, H. Y.; O'Donnell, J. M.; Hayes, A. C.; Stetcu, I.; Taddeucci, T. N.; Talou, P.; Vieira, D. J.; Wilhelmy, J. B.; Becker, J. A.; Chyzh, A.; Gostic, J.; Henderson, R.; Kwan, E.; Wu, C. Y.

    2013-04-01

    Background: The prompt gamma-ray spectrum from fission is important for understanding the physics of nuclear fission, and also in applications involving fission. Relatively few measurements of the prompt gamma spectrum from 239Pu(n,f) have been published.Purpose: This experiment measured the multiplicity, individual gamma energy spectrum, and total gamma energy spectrum of prompt fission gamma rays from 239Pu(n,f) in the neutron energy range from thermal to 30 keV, to test models of fission and to provide information for applications.Method: Gamma rays from neutron-induced fission of 239Pu were measured using the DANCE gamma-ray calorimeter. Fission events were tagged by detecting fission products in a parallel-plate avalanche counter in the center of DANCE. The measurements were corrected for detector response using a geant4 model of DANCE. A detailed analysis for the gamma rays from the 1+ resonance complex at 10.93 eV is presented.Results: A six-parameter analytical parametrization of the fission gamma-ray spectrum was obtained. A Monte Carlo Hauser-Feshbach calculation provided good general agreement with the data, but some differences remain to be resolved.Conclusions: An analytic parametrization can be made of the gamma-ray multiplicity, energy distribution, and total-energy distribution for the prompt gamma rays following neutron-induced fission of 239Pu. This parametrization may be useful for applications. Modern Monte Carlo Hauser-Feshbach calculations can do a good job of calculating the fission gamma-ray emission spectrum, although some details remain to be understood.

  13. [State of cellular immunity effectors of the lung after inhalation of 239Pu polymer nitrate].

    PubMed

    Sokol'nikov, M E

    1992-01-01

    Wistar rats, who inhaled 239Pu (IV) at a dose that did not reduce the average life expectancy (the initial level in the lung was 0.77 kBq) did not exhibit any essential changes in the quality and functional activity of the alveolar macrophages. Revealed were the injuries to cells of bifurcation lymph nodes, the severity of which was a function of dose absorbed in the lung.

  14. A Time Projection Chamber for precision 239Pu(n,f) cross section measurement

    SciTech Connect

    Heffner, M

    2008-01-14

    High precision measurements of the {sup 239}Pu(n,f) cross section have been identified as important for the Global Nuclear Energy Partnership (GNEP) and other programs. Currently the uncertainty on this cross section is of the order 2-3% for neutron energies below 14 MeV and the goal is to reduce this to less than 1%. The Time Projection Chamber (TPC) has been identified as a possible tool to make this high precision measurement.

  15. Modifying effects of preexisting pulmonary fibrosis on biological responses of rats to inhaled 239PuO2

    SciTech Connect

    Lundgren, D.L.; Mauderly, J.L.; Rebar, A.H.; Gillett, N.A.; Hahn, F.F. )

    1991-03-01

    We investigated the modifying effects of preexisting, bleomycin-induced pulmonary fibrosis on the deposition, retention, and biological effects of inhaled 239PuO2 in the rat. Among rats exposed to similar airborne concentrations of 239PuO2, initial lung burdens of 239Pu per kilogram body mass were similar whether or not pulmonary fibrosis was present. However, clearance of 239Pu from the lungs was significantly decreased in the rats with preexisting pulmonary fibrosis. The incidence of lung lesions (epithelial hyperplasia, diffuse macrophage increases and aggregation, and loose and dense connective tissue) was significantly greater among rats with preexisting pulmonary fibrosis than among the exposed controls. Rats with preexisting fibrosis had shorter life spans than 239PuO2-exposed control rats. When groups of rats with similar alpha doses to the lungs were compared, the incidences of neoplastic lesions in the lung, the times to death of rats with lung neoplasms, and the risk of lung tumors per unit of alpha dose to the lungs in rats with or without pulmonary fibrosis were similar. The results of this study suggest that humans with uncomplicated pulmonary fibrosis may not be more sensitive to the carcinogenic effects of inhaled 239PuO2 than are individuals with normal lungs, assuming that the total alpha doses to the lungs are similar.

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

    USGS Publications Warehouse

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

    2012-01-01

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

  17. 239+240Pu, 90Sr and 137Cs inventories in surface soils of Vietnam.

    PubMed

    Quang, N H; Long, N Q; Lieu, D B; Mai, T T; Ha, N T; Nhan, D D; Hien, P D

    2004-01-01

    Fallout 239+240Pu, 238Pu, 90Sr and 137Cs inventories in surface soils were measured for 20 locations in northern Vietnam yielding the mean values (+/- standard error) of 26.5+/-3.8 Bq m(-2) for 239+240Pu, 1048+/-143 Bq m(-2) for 137Cs and 212+/-28 Bq m(-2) for 90Sr. The concentrations of 137Cs and plutonium isotopes strongly correlate with each other resulting in a stable 239+240Pu/137Cs inventory ratio of 0.025+/-0.002. Among soil parameters, organic matter and fulvic acids strongly correlate with caesium and plutonium isotopes, especially in the 0-10 cm layer. 137Cs and 239+240Pu are distributed rather similarly over the 0-10 cm and 10-20 cm layers. At locations with high contents of sand (82-93%) along the South China Sea coast, the downward percolation by rainwater results in a higher accumulation of 239+240Pu and 137Cs in the 10-20 cm layer. The mean 137Cs/ 90Sr inventory ratio is 9.3+/-2.2, and the correlation is weak between these isotopes.

  18. Modeling and production of 240Am by deuteron-induced activation of a 240Pu target

    SciTech Connect

    Finn, Erin C.; McNamara, Bruce K.; Greenwood, Lawrence R.; Wittman, Richard S.; Soderquist, Chuck Z.; Woods, Vincent T.; VanDevender, Brent A.; Metz, Lori A.; Friese, Judah I.

    2015-02-01

    A novel reaction pathway for production of 240Am is reported. Models of reaction cross-sections in EMPIRE II suggests that deuteron-induced activation of a 240Pu target produces maximum yields of 240Am from 11.5 MeV incident deuterons. This activation had not been previously reported in the literature. A 240Pu target was activated under the modeled optimum conditions to produce 240Am. The modeled cross-section for the 240Pu(d, 2n)240Am reaction is on the order of 20-30 mbarn, but the experimentally estimated value is 5.3 ± 0.2 mbarn. We discuss reasons for the discrepancy as well as production of other Am isotopes that contaminate the final product.

  19. 137Cs and (239+240)Pu levels in the Asia-Pacific regional seas.

    PubMed

    Duran, E B; Povinec, P P; Fowler, S W; Airey, P L; Hong, G H

    2004-01-01

    137Cs and (239+240)Pu data in seawater, sediment and biota from the regional seas of Asia-Pacific extending from 50 degrees N to 60 degrees S latitude and 60 degrees E to 180 degrees E longitude based on the Asia-Pacific Marine Radioactivity Database (ASPAMARD) are presented and discussed. 137Cs levels in surface seawater have been declining to its present median value of about 3 Bq/m3 due mainly to radioactive decay, transport processes, and the absence of new significant inputs. (239+240)Pu levels in surface seawater are much lower, with a median of about 6 mBq/m3. (239+240)Pu appears to be partly scavenged by particles and is therefore more readily transported down the water column. As with seawater, (239+240)Pu concentrations are lower than 137Cs in surface sediment. The median 137Cs concentration in surface sediment is 1.4 Bq/kg dry, while that of (239+240)Pu is only 0.2 Bq/kg dry. The vertical profiles of both 137Cs and (239+240)Pu in the sediment column of coastal areas are different from deep seas which can be attributed to the higher sedimentation rates and additional contribution of run-offs from terrestrial catchment areas in the coastal zone. Comparable data for biota are far less extensive than those for seawater and sediment. The median 137Cs concentration in fish (0.2 Bq/kg wet) is higher than in crustaceans (0.1 Bq/kg wet) or mollusks (0.1 Bq/kg wet). Benchmark values (as of 2001) for 137Cs and (239+240)Pu concentrations in seawater, sediment and biota are established to serve as reference values against which the impact of future anthropogenic inputs can be assessed. ASPAMARD represents one of the most comprehensive compilations of available data on 137Cs and (239+240)Pu in particular, and other anthropogenic as well as natural radionuclides in seawater, sediment and biota from the Asia-Pacific regional seas. PMID:15245845

  20. Comprehensive appraisal of {sup 239+240}Pu in soils around Rocky Flats, Colorado

    SciTech Connect

    Litaor, M.I.; Allen, L.; Ellerbroek, D.

    1995-12-01

    Plutonium contamination of soils around Rocky Flats Environmental & Technology Site, near Golden, Colorado, resulted from past outdoor storage practices and subsequent remobilization due to inadequate cleanup practices. Until now human-health risk assessment has not been performed because of a lack of sufficient information regarding the spatial extent of {sup 239+240}Pu in soils. The purpose of this work was to elucidate the extent of plutonium contamination in surface soils, and to assess the uncertainty associated with the spatial distribution of {sup 239+240}Pu around Rocky Flats Environmental & Technology Site.

  1. Commentary on Inhaled 239PuO2 in Dogs — A Prophylaxis against Lung Cancer?

    DOE PAGES

    Cuttler, Jerry M.; Feinendegen, Ludwig E.

    2015-01-01

    Several studies on the effect of inhaled plutonium-dioxide particulates and the incidence of lung tumors in dogs reveal beneficial effects when the cumulative alpha-radiation dose is low. There is a threshold at an exposure level of about 100 cGy for excess tumor incidence and reduced lifespan. The observations conform to the expectations of the radiation hormesis dose-response model and contradict the predictions of the LNT hypothesis. These studies suggest investigating the possibility of employing low-dose alpha-radiation, such as from 239PuO2 inhalation, as a prophylaxis against lung cancer.

  2. /sup 235/U and /sup 239/Pu sample-mass determinations and intercomparisons

    SciTech Connect

    Poenitz, W.P.; Meadows, J.W.

    1983-11-01

    The masses of fifteen /sup 235/U samples obtained from seven laboratories were determined and intercompared. The present results indicate that sample masses are well enough known (+- 0.3%) for the required high-accuracy-fission cross-section measurements. A comparison of four /sup 239/Pu samples indicates problems in the order of 1 to 3% which are more likely, to be related to counting efficiencies than to sample masses. The half-life of /sup 234/U was determined as (2.457 +- 0.005) . 10/sup 5/ yrs. 27 references.

  3. Surrogate Reaction Measurement of Angular Dependent 239Pu (n , f) Probabilities

    NASA Astrophysics Data System (ADS)

    Koglin, Johnathon; Burke, Jason; Casperson, Robert; Jovanovic, Igor

    2015-10-01

    The surrogate method has previously been used to measure (n , f) cross sections of difficult to produce actinide isotopes. These measurements have inaccuracies at excitation energies below 1.5 MeV where the distribution of angular momentum states populated in the compound nucleus created by neutron absorption significantly differs from that arising from direct reactions. A method to measure the fission probability of individual angular momentum states arising from 239Pu (d , pf) and 239Pu (α ,α' f) reactions has been developed. This experimental apparatus consists of charged particle detectors with 40 keV FWHM resolution at 13 angles up and downstream of the particle beam. A segmented array of photovoltaic (solar) cells is used to measure the angular distribution of fission fragments. This distribution uniquely identifies the populated angular momentum states. These are fit to expected distributions to determine the contribution of each state. The charged particle and fission rates matrix obtained from this analysis determines fission probabilities of specific angular momentum states in the transition nucleus. Development of this scheme and first results will be discussed.

  4. Consistent Data Assimilation of Actinide Isotopes: 235U and 239Pu

    SciTech Connect

    G. Palmiottti; H. Hiruta; M. Salvatores

    2011-09-01

    In this annual report we illustrate the methodology of the consistent data assimilation that allows to use the information coming from integral experiments for improving the basic nuclear parameters used in cross section evaluation. A series of integral experiments were analyzed using the EMPIRE evaluated files for {sup 235}U, {sup 238}U, and {sup 239}Pu. Inmost cases the results have shown quite large worse results with respect to the corresponding existing evaluations available for ENDF/B-VII. The observed discrepancies between calculated and experimental results were used in conjunction with the computed sensitivity coefficients and covariance matrix for nuclear parameters in a consistent data assimilation. Only the GODIVA and JEZEBEL experimental results were used, in order to exploit information relative to the isotope of interest that are, in this particular case: {sup 235}U and {sup 239}Pu. The results obtained by the consistent data assimilation indicate that with reasonable modifications (mostly within the initial standard deviation) it is possible to eliminate the original large discrepancies on the K{sub eff} of the two critical configurations. However, some residual discrepancy remains for a few fission spectral indices that are, most likely, to be attributed to the detector cross sections.

  5. Ultra-trace analysis of plutonium by thermal ionization mass spectrometry with a continuous heating technique without chemical separation.

    PubMed

    Lee, Chi-Gyu; Suzuki, Daisuke; Esaka, Fumitaka; Magara, Masaaki; Song, Kyuseok

    2015-08-15

    Thermal ionization mass spectrometry (TIMS) with a continuous heating technique is known as an effective method for measuring the isotope ratio in trace amounts of uranium. In this study, the analytical performance of thermal ionization mass spectrometry with a continuous heating technique was investigated using a standard plutonium solution (SRM 947). The influence of the heating rate of the evaporation filament on the precision and accuracy of the isotope ratios was examined using a plutonium solution sample at the fg level. Changing the heating rate of the evaporation filament on samples ranging from 0.1fg to 1000fg revealed that the influence of the heating rate on the precision and accuracy of the isotope ratios was slight around the heating rate range of 100-250mA/min. All of the isotope ratios of plutonium (SRM 947), (238)Pu/(239)Pu, (240)Pu/(239)Pu, (241)Pu/(239)Pu and (242)Pu/(239)Pu, were measured down to sample amounts of 70fg. The ratio of (240)Pu/(239)Pu was measured down to a sample amount of 0.1fg, which corresponds to a PuO2 particle with a diameter of 0.2μm. Moreover, the signals of (239)Pu could be detected with a sample amount of 0.03fg, which corresponds to the detection limit of (239)Pu of 0.006fg as estimated by the 3-sigma criterion. (238)Pu and (238)U were clearly distinguished owing to the difference in the evaporation temperature between (238)Pu and (238)U. In addition, (241)Pu and (241)Am formed by the decay of (241)Pu can be discriminated owing to the difference in the evaporation temperature. As a result, the ratios of (238)Pu/(239)Pu and (241)Pu/(239)Pu as well as (240)Pu/(239)Pu and (242)Pu/(239)Pu in plutonium samples could be measured by TIMS with a continuous heating technique and without any chemical separation processes.

  6. Ultra-trace analysis of plutonium by thermal ionization mass spectrometry with a continuous heating technique without chemical separation.

    PubMed

    Lee, Chi-Gyu; Suzuki, Daisuke; Esaka, Fumitaka; Magara, Masaaki; Song, Kyuseok

    2015-08-15

    Thermal ionization mass spectrometry (TIMS) with a continuous heating technique is known as an effective method for measuring the isotope ratio in trace amounts of uranium. In this study, the analytical performance of thermal ionization mass spectrometry with a continuous heating technique was investigated using a standard plutonium solution (SRM 947). The influence of the heating rate of the evaporation filament on the precision and accuracy of the isotope ratios was examined using a plutonium solution sample at the fg level. Changing the heating rate of the evaporation filament on samples ranging from 0.1fg to 1000fg revealed that the influence of the heating rate on the precision and accuracy of the isotope ratios was slight around the heating rate range of 100-250mA/min. All of the isotope ratios of plutonium (SRM 947), (238)Pu/(239)Pu, (240)Pu/(239)Pu, (241)Pu/(239)Pu and (242)Pu/(239)Pu, were measured down to sample amounts of 70fg. The ratio of (240)Pu/(239)Pu was measured down to a sample amount of 0.1fg, which corresponds to a PuO2 particle with a diameter of 0.2μm. Moreover, the signals of (239)Pu could be detected with a sample amount of 0.03fg, which corresponds to the detection limit of (239)Pu of 0.006fg as estimated by the 3-sigma criterion. (238)Pu and (238)U were clearly distinguished owing to the difference in the evaporation temperature between (238)Pu and (238)U. In addition, (241)Pu and (241)Am formed by the decay of (241)Pu can be discriminated owing to the difference in the evaporation temperature. As a result, the ratios of (238)Pu/(239)Pu and (241)Pu/(239)Pu as well as (240)Pu/(239)Pu and (242)Pu/(239)Pu in plutonium samples could be measured by TIMS with a continuous heating technique and without any chemical separation processes. PMID:25966386

  7. Partial (gamma)-Ray Cross Sections for the Reaction 239Pu(n,2n(gamma)i) and the 239Pu(n,2n) Cross Section

    SciTech Connect

    Beacker, J.A.; Bernstein, L.A.; Younes, W.; McNabb, D.P.; Garrett, P.E.; Archer, D.; McGrath, C.A.; Stoyer, M.A.; Chen, H.; Ormand, W.E.; Nelson, R.O.; Chadwick, M.B.; Johns, G.D.; Drake, D.; Young, P.G.; Devlin, M.; Fotiades, N.; Wilburn, W.S.

    2001-09-14

    Absolute partial {gamma}-ray cross sections for production of discrete {gamma} rays in the {sup 239}Pu(n,2n{gamma}i){sup 238}Pu reaction have been measured. The experiments were performed at LANSCE/WNR on the 60R flight line. Reaction {gamma}-rays were measured using the large-scale Compton-suppressed array of Ge detectors, GEANIE. The motivation for this experiment, an overview of the partial {gamma}-ray cross-section measurement, and an introduction to the main experimental issues will be presented. The energy resolution of the Ge detectors allowed identification of reaction {gamma} rays above the background of sample radioactivity and fission {gamma} rays. The use of planar Ge detectors with their reduced sensitivity to neutron interactions and improved line shape was also important to the success of this experiment. Absolute partial {gamma}-ray cross sections are presented for the 6{sub 1}{sup +} {yields} 4{sub 1}{sup +} member of the ground state rotational band in {sup 238}Pu, together with miscellaneous other {gamma}-ray partial cross sections. The n,2n reaction cross section shape and magnitude as a function of neutron energy was extracted from these partial cross sections using nuclear modeling (enhanced Hauser-Feshbach) to relate partial {gamma}-ray cross sections to the n,2n cross section. The critical nuclear modeling issue is the ratio of a partial cross section to the reaction channel cross section, and not the prediction of the absolute magnitude.

  8. Large particle flux of 239+240Pu on the continental margin of the East China Sea.

    PubMed

    Yamada, Masatoshi; Aono, Tatsuo

    2002-03-15

    Settling particles were collected from three locations in the East China Sea continental margin and analyzed for 239+240Pu. Two types of sediment traps were used, cylindrical traps and conical time-series traps. Surface sediment samples collected from five locations were also analyzed for 239+240Pu. Data from cylindrical traps showed there was a clear tendency for total mass fluxes to increase with depth at all three stations, and there was an especially large increase near the bottom. 239+240Pu concentrations in settling particles increased with depth from 1.76 mBq/g at 97-m depth to 3.0 mBq/g at 120-m depth and ranged from approximately 3 to 4 mBq/g at depths greater than 120 m. 239+240Pu concentrations collected in the near-bottom traps were approximately two times higher than those in the underlying surface sediments. Like total mass fluxes there was a clear tendency for 239+240Pu fluxes to increase with depth at every station, and the highest 239+240Pu fluxes were observed near the bottom. 239+240Pu concentrations in the time-series traps had little variation throughout the sampling period, though the total mass fluxes showed a large variation. A high variability of 239+240Pu fluxes occurred in very short period of time (1/2 day). The large fluxes of 239+240Pu might be attributed to episodic lateral transport of particles that flow down the continental slope with the nepheloid layer which was considered to be significant for 239+240Pu transport on the continental slope in the East China Sea.

  9. Exposure of F344 rats to aerosols of {sup 239}PuO{sub 2} and chronically inhaled cigarette smoke

    SciTech Connect

    Finch, G.L.; Nikula, K.J.; Barr, E.B.; Bechtold, W.E.; Chen, B.T.; Griffith, W.C.; Hobbs, C.H.; Hoover, M.D.; Mauderly, J.L.

    1994-11-01

    Nuclear workers may be accidently exposed to radioactive materials such as {sup 239}PuO{sub 2} by inhalation, and thus have increased risk for lung cancer compared to the general population. Of additional concern is the possibility that interactions between radionuclides and other carcinogens may increase the risk of cancer induction. An important and common lung carcinogen is cigarette smoke. This study is being conducted to better determine the combined effects of inhaled {sup 239}PuO{sub 2} and cigarette smoke on the induction of lung cancer in rats.

  10. Microdistribution and retention of injected /sup 239/Pu on trabecular bone surfaces of the beagle: implications for the induction of osteosarcoma

    SciTech Connect

    Wronski, T.J.; Smith, J.M.; Jee, W.S.S.

    1980-07-01

    A study was initiated to investigate the relationship between skeletal remodeling and the microdistribution and retention of /sup 239/Pu on trabecular bone surfaces of the beagle, and the contribution of these parameters to the nonuniform skeletal distribution of /sup 239/Pu-induced osteosarcomas. Young adult beagles were administered single iv injections of approx. 0.016 ..mu..Ci/kg monomeric /sup 239/Pu citrate and sacrificed at various times to 1 year after injection. The /sup 239/Pu concentration on trabecular bone surfaces was determined by counting fission fragment tracks in neutron-induced autoradiographs produced from thick (approx. 400 ..mu..m) bone sections. The rate of trabecular bone formation was calculated from an ultraviolet microscopic analysis of fluorescent tetracycline labels. The lumbar vertebra, pelvis, and proximal humerus, each of which exhibits a high incidence of /sup 239/Pu-induced osteosarcoma, were found to have a high intial concentration of /sup 239/Pu on their trabecular surfaces (approx. 7-8 pCi/cm/sup 2/) and a relatively high rate of trabecular bone formation. The /sup 239/Pu concentration at these sites decreased to approx. 2-3 pCi/cm/sup 2/ at the end of the first year. On the other hand, the proximal ulna and distal humerus, skeletal sites with a low tumor incidence, had a low intial concentration of /sup 239/Pu on their trabecular surfaces(approx. 1-2 pCi/cm/sup 2/) and a significantly lower rate of trabecular bone formation (P < 0.01). The /sup 239/Pu concentration at these sites remained nearly constant throughout the experimental period. These data suggest that the degree of the initial deposition of /sup 239/Pu on trabecular bone surfaces and the rate of trabecular bone turnover may play a role in the genesis of /sup 239/Pu-induced osteosarcomas.

  11. Bayesian estimation of the relative toxicity of (239)Pu and (226)Ra with dependent competing risks

    NASA Astrophysics Data System (ADS)

    Xiao, Shili

    The purpose of this dissertation research is to compare the toxicity of the alpha-emitting, bone-seeking radionuclides sp{239}Pu and sp{226}Ra, develop a model for radiation induced osteosarcomas, and analyze the survival data of beagles exposed to these radionuclides. This research integrates the knowledge of radiation protection, survival theory and methods (competing risks, maximum likelihood estimation, and Bayesian techniques), numerical integration techniques (Monte Carlo, Lattice rule and Gauss-quadrature) and object-oriented programming in C++. The outline of this research is: (1) survival data preprocessing, (2) model identification and selection, (3) introduction of FGM model, the dependent competing risk model created by Farlie, Gumbel and Morgenstern, to the study of survival data with dependent competing risks: osteosarcomas and other diseases, development of the crude density of the FGM model and construction of the likelihood function for the FGM model, (4) Bayesian estimates of the posterior marginal density of the toxicity ratio in the FGM model using several numerical integration techniques (Monte Carlo, Lattice rule and Gaussian Quadrature), (5) construction of the likelihood function for the independent competing risk model, Bayesian estimate of the posterior marginal density of toxicity ratio in the model using Monte Carlo method, which is compared with the posterior marginal densities for the toxicity ratio obtained from the FGM model, (6) Bayesian estimates of all other parameters in the FGM model using Monte Carlo method, (7) Comparison of the cumulative hazard for sp{239}Pu calculated according to the model with Nelson's cumulative hazard plot under Bayesian point estimates of parameters and the mean activity in each injection level, (8) Comparison of the toxicity of plutonium in osteosarcoma with that of radium under Bayesian point estimates of parameters an d the selected activit of 0.85 muCsbi, (7) discuss Bayesian prediction of the

  12. Relationship between dose of injected /sup 239/Pu and bone sarcoma mortality in young adult beagles

    SciTech Connect

    Peterson, A.V.; Prentice, R.L.; Marek, P.

    1982-04-01

    The effect of /sup 239/Pu on bone sarcoma mortality in young adult beagles is examined using data from a follow-up study conducted at the Radiobiology Laboratory at the University of Utah. A (proportional-hazards) model, which specifies that bone sarcoma mortality depends on both dose of injected plutonium and time since injection as the product of a dose factor and a time factor, is used both for describing the data and for performing inference about the relationship between dose of plutonium and bone sarcoma mortality. Relative bone sarcoma mortality rates are found to be approximately linear as a function of dose. There is evidence that relative bone sarcoma mortality decreases with time since injection.

  13. Quantitative scanning electron microscopic autoradiography of inhaled /sup 239/PuO/sub 2/

    SciTech Connect

    Sanders, C.L.; Lauhala, K.E.; McDonald, K.E.

    1989-03-01

    We have applied the scanning electron microscope (SEM) to obtain autoradiographs of particles of /sup 239/PuO/sub 2/ deposited in rat lung. The technique was used to obtain quantitative information on the clearance rates of particles from the alveoli, bronchioles and trachea up to 240 d after exposure. At all times, the concentration of particles on the surface of the bronchioles was an order of magnitude greater than on the tracheal surface. The clearance of Pu from both regions followed a biphasic pattern, similar to that obtained by radiometric analysis of the whole lung. Most of the radiation dose to the bronchiolar epithelium originated from Pu particles in peribronchiolar alveoli in which they were preferentially retained, compared to other alveolar regions. The prolonged retention of particles in the peribronchiolar alveoli may be a significant factor in the induction of lung carcinomas.

  14. Calculation of 239Pu fission observables in an event-by-event simulation

    SciTech Connect

    Vogt, R; Randrup, J; Pruet, J; Younes, W

    2010-03-31

    The increased interest in more exclusive fission observables has demanded more detailed models. We describe a new computational model, FREYA, that aims to meet this need by producing large samples of complete fission events from which any observable of interest can then be extracted consistently, including any interesting correlations. The various model assumptions are described and the potential utility of the model is illustrated. As a concrete example, we use formal statistical methods, experimental data on neutron production in neutron-induced fission of {sup 239}Pu, along with FREYA, to develop quantitative insights into the relation between reaction observables and detailed microscopic aspects of fission. Current measurements of the mean number of prompt neutrons emitted in fission taken together with less accurate current measurements for the prompt post-fission neutron energy spectrum, up to the threshold for multi-chance fission, place remarkably fine constraints on microscopic theories.

  15. Release of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant accident to the marine environment was negligible.

    PubMed

    Bu, Wenting; Fukuda, Miho; Zheng, Jian; Aono, Tatsuo; Ishimaru, Takashi; Kanda, Jota; Yang, Guosheng; Tagami, Keiko; Uchida, Shigeo; Guo, Qiuju; Yamada, Masatoshi

    2014-08-19

    Atmospheric deposition of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident has been observed in the terrestrial environment around the FDNPP site; however, their deposition in the marine environment has not been studied. The possible contamination of Pu in the marine environment has attracted great scientific and public concern. To fully understand this possible contamination of Pu isotopes from the FDNPP accident to the marine environment, we collected marine sediment core samples within the 30 km zone around the FDNPP site in the western North Pacific about two years after the accident. Pu isotopes ((239)Pu, (240)Pu, and (241)Pu) and radiocesium isotopes ((134)Cs and (137)Cs) in the samples were determined. The high activities of radiocesium and the (134)Cs/(137)Cs activity ratios with values around 1 (decay corrected to 15 March 2011) suggested that these samples were contaminated by the FDNPP accident-released radionuclides. However, the activities of (239+240)Pu and (241)Pu were low compared with the background level before the FDNPP accident. The Pu atom ratios ((240)Pu/(239)Pu and (241)Pu/(239)Pu) suggested that global fallout and the pacific proving ground (PPG) close-in fallout are the main sources for Pu contamination in the marine sediments. As Pu isotopes are particle-reactive and they can be easily incorporated with the marine sediments, we concluded that the release of Pu isotopes from the FDNPP accident to the marine environment was negligible.

  16. Vertical distribution and inventories of (239+240)Pu and mercury in Sagua la Grande estuary, Cuba.

    PubMed

    Alonso-Hernández, C M; Martin-Perez, J; Gasco, C; Díaz-Asencio, M; Bolanos-Álvarez, Y; Gómez-Batista, M

    2012-10-01

    The vertical activity distribution and inventories of (239+240)Pu profile and Hg were determined in Sagua la Grande estuary, Cuba. The shape of the (239+240)Pu profile in the core column resembled very closely the history of atmospheric nuclear weapons' testing, and the maximum deposition in 1963 was recorded in the sediment core history. The (239+240)Pu activity concentrations in the surface layer sediments varied from 0.163 to 0.611 mBq g(-1). The inventory of (239+240)Pu was 42 ± 5.6 Bq m(-2), a value close to that expected from direct global fallout. Using the (239+240)Pu as a chronomarker the mass sedimentation rate in the area for the last 60 years was calculated, reaching values of 0.173 g cm(-2) y(-1). The mercury profile reflects the history of anthropogenic pollution in the estuary and perfectly describes the operation of the mercury-cell chlor-alkali plant, for production of NaOH, which began operations in 1980. The inventory of Hg was 2.42 ± 0.19 μg cm(-2). These results contribute to the scarce regional database for pollutants and anthropogenic radionuclides in the Caribbean marine environment, particularly in relation to (239+240)Pu. PMID:22484472

  17. 239Pu Prompt Fission Neutron Spectra Impact on a Set of Criticality and Experimental Reactor Benchmarks

    NASA Astrophysics Data System (ADS)

    Peneliau, Y.; Litaize, O.; Archier, P.; De Saint Jean, C.

    2014-04-01

    A large set of nuclear data are investigated to improve the calculation predictions of the new neutron transport simulation codes. With the next generation of nuclear power plants (GEN IV projects), one expects to reduce the calculated uncertainties which are mainly coming from nuclear data and are still very important, before taking into account integral information in the adjustment process. In France, future nuclear power plant concepts will probably use MOX fuel, either in Sodium Fast Reactors or in Gas Cooled Fast Reactors. Consequently, the knowledge of 239Pu cross sections and other nuclear data is crucial issue in order to reduce these sources of uncertainty. The Prompt Fission Neutron Spectra (PFNS) for 239Pu are part of these relevant data (an IAEA working group is even dedicated to PFNS) and the work presented here deals with this particular topic. The main international data files (i.e. JEFF-3.1.1, ENDF/B-VII.0, JENDL-4.0, BRC-2009) have been considered and compared with two different spectra, coming from the works of Maslov and Kornilov respectively. The spectra are first compared by calculating their mathematical moments in order to characterize them. Then, a reference calculation using the whole JEFF-3.1.1 evaluation file is performed and compared with another calculation performed with a new evaluation file, in which the data block containing the fission spectra (MF=5, MT=18) is replaced by the investigated spectra (one for each evaluation). A set of benchmarks is used to analyze the effects of PFNS, covering criticality cases and mock-up cases in various neutron flux spectra (thermal, intermediate, and fast flux spectra). Data coming from many ICSBEP experiments are used (PU-SOL-THERM, PU-MET-FAST, PU-MET-INTER and PU-MET-MIXED) and French mock-up experiments are also investigated (EOLE for thermal neutron flux spectrum and MASURCA for fast neutron flux spectrum). This study shows that many experiments and neutron parameters are very sensitive to

  18. Photofission product yields of 238U and 239Pu with 22-MeV bremsstrahlung

    NASA Astrophysics Data System (ADS)

    Wen, Xianfei; Yang, Haori

    2016-06-01

    In homeland security and nuclear safeguards applications, non-destructive techniques to identify and quantify special nuclear materials are in great demand. Although nuclear materials naturally emit characteristic radiation (e.g. neutrons, γ-rays), their intensity and energy are normally low. Furthermore, such radiation could be intentionally shielded with ease or buried in high-level background. Active interrogation techniques based on photofission have been identified as effective assay approaches to address this issue. In designing such assay systems, nuclear data, like photofission product yields, plays a crucial role. Although fission yields for neutron-induced reactions have been well studied and readily available in various nuclear databases, data on photofission product yields is rather scarce. This poses a great challenge to the application of photofission techniques. In this work, short-lived high-energy delayed γ-rays from photofission of 238U were measured in between linac pulses. In addition, a list-mode system was developed to measure relatively long-lived delayed γ-rays from photofission of 238U and 239Pu after the irradiation. Time and energy information of each γ-ray event were simultaneously recorded by this system. Cumulative photofission product yields were then determined using the measured delayed γ-ray spectra.

  19. Using 239Pu as a tracer for fine sediment sources in the Daly River, Northern Australia

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

    The Daly River drains a large (52500 km2) and mainly undisturbed catchment in the Australian wet-dry tropics. Clearing and cropping since 2002 have raised concerns about possible increased sediment input into the river and motivated this study of its fine sediment sources. Using 239Pu as a tracer it is shown that the fine sediments originate mainly from erosion by gullying and channel change. Although the results also indicate that the surface soil contribution to the river channel sediments from sheet erosion has increased to 5-22% for the Daly River and 7-28% for the Douglas River (a tributary of the Daly River) in 2009 vs. 3-6% for the Daly River and 4-9% for the Douglas River in 2005. This excess top soil likely originates from thecleared land adjacent to the Daly River since 2005. However, channel widening largely as a result of hydrologic change is still the dominant sediment source in this catchment.

  20. [Acceleration of the excretion of monomeric 239Pu-citrate from the body as effected by pentacyne encapsulated in liposomes].

    PubMed

    Il'in, L A; Smirnov, A A; Ivannikov, A T; Parfenova, I M

    1983-01-01

    Liposomes, obtained by a modified procedure involving reverse phases, contained 2-3-times more 14C-pentacyne than the multilayer Banchem;s liposomes. Efficiency of pentacyne encapsulated in liposomes was higher, as compared with a non-encapsulated preparation in studies of urinary excretion of monomeric 239Pu-citrate in rats. Liposomal pentacyne increased most effectively the rate of the radionuclide excretion from liver tissue and skeleton as compared with the action of non-encapsulated complex-forming agent; as a result of which the radionuclide was excreted from liver tissue at a 1.6-2-times and from skeleton--with the 1.4-times higher rates. The both preparations increased the 239Pu excretion with urine and feces. The liposomal pentacyne accelerated an additional excretion of the nuclide with urine. PMID:6353751

  1. Relationship between bronchiolar dose and lung carcinoma induction following inhalation of /sup 239/PuO/sub 2/ in rats

    SciTech Connect

    Sanders, C.L.; Lauhala, K.E.; McDonald, K.E.

    1988-08-01

    This manuscript describes preliminary observations in a lifespan and serial sacrifice study with 3332 female, Wistar rats exposed to high-fired /sup 239/PuO/sub 2/ aerosols. Sufficient numbers of sham-control and low dose (equivalent to maximal permissible occupational lung deposition of 0.6 kBq in standard man) animals are provided to statistically estimate lung cancer risk and define the cellular-microdosimetric relationships leading to lung tumor formation. Whole-body counting for /sup 169/Yb tagged /sup 239/PuO/sub 2/ aerosol provided a very accurate method for determining Pu ILB in individual rats (Sanders et al., 1986). The experimental design, methodology and early results of the lifespan study have been previously reported (Sanders et al., 1986, 1988a). 7 refs., 3 figs.

  2. Microscopic modeling of mass and charge distributions in the spontaneous fission of 240Pu

    NASA Astrophysics Data System (ADS)

    Sadhukhan, Jhilam; Nazarewicz, Witold; Schunck, Nicolas

    2016-01-01

    We propose a methodology to calculate microscopically the mass and charge distributions of spontaneous fission yields. We combine the multidimensional minimization of collective action for fission with stochastic Langevin dynamics to track the relevant fission paths from the ground-state configuration up to scission. The nuclear potential energy and collective inertia governing the tunneling motion are obtained with nuclear density functional theory in the collective space of shape deformations and pairing. We obtain a quantitative agreement with experimental data and find that both the charge and mass distributions in the spontaneous fission of 240Pu are sensitive both to the dissipation in collective motion and to adiabatic fission characteristics.

  3. Comprehensive appraisal of 239 + 240Pu in soils around Rocky Flats, Colorado.

    PubMed

    Litaor, M I; Ellerbroek, D; Allen, L; Dovala, E

    1995-12-01

    Plutonium contamination of soils around Rocky Flats Environmental & Technology Site, near Golden, Colorado, resulted from past outdoor storage practices and subsequent remobilization due to inadequate cleanup practices. Until now human-health risk assessment has not been performed because of a lack of sufficient information regarding the spatial extent of 239 + 240Pu in soils. The purpose of this work was to elucidate the extent of plutonium contamination in surface soils, and to assess the uncertainty associated with the spatial distribution of 239 + 240Pu around Rocky Flats Environmental & Technology Site. Four data sets were collected or compiled for this investigation: (1) samples collected from 240 plots of 1.01- or 4.05-hectare by compositing 25 evenly-spaced samples from the upper 0.64 cm in each plot; (2) samples collected from the upper 5 cm of soil in 167 of the same 240 plots by compositing 10 samples from the center of each plot; (3) historical data compiled from samples collected between 1969 and 1973, considered to be the most indicative of the original release; and (4) the exhaustive data set that contains the samples from 1, 2, and 3 and other published data sets collected between 1974 and 1994. These latter samples varied in depth and method of sampling. Plutonium activity reported in the exhaustive data set ranged from 0.03 Bq kg-1 to 407,000 Bq kg-1 with a mean of 1,443 Bq kg-1, median of 6.6 Bq kg-1, standard deviation of 18,463 Bq kg-1, and a coefficient of variation of 12.6. The technique of nonparametric indicator kriging was used to model four conditional cumulative distribution functions of 239 + 240Pu in soils around Rocky Flats Environmental & Technology Site. Each of the conditional cumulative distribution functions was used to generate an E-type (mean of the conditional cumulative distribution functions) surface. The resulted surfaces were consistent with the hypothesis that the westerly winds were the dominant mechanism of plutonium

  4. Probing energy dissipation, γ-ray and neutron multiplicity in the thermal neutron-induced fission of 239Pu

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

    The incorporation of the four-dimensional Langevin equations led to an integrative description of fission cross-section, fragment mass distribution and the multiplicity and energy distribution of prompt neutrons and γ-rays in the thermal neutron-induced fission of 239Pu. The dynamical approach presented in this paper thoroughly reproduces several experimental observables of the fission process at low excitation energy.

  5. 241Pu and 241Am in sediments from coastal basins off California and Mexico

    NASA Astrophysics Data System (ADS)

    Koide, Minoru; Goldberg, Edward D.; Hodge, Vernon F.

    1980-07-01

    In sediments deposited in the coastal basins off the western North American continent since the early 1960's, there is more 241Am activity than one would predict if its presence was solely due to the decay of 241Pu that was produced during the testing of weapons in 1961-1962 (taken as July 1, 1962 for calculations). This excess can be accounted for by the decay of 241Pu, if pre-1962 fallout (fallout from the pre-moratorium testing) has been continuously introduced into the recent sediments along with fallout from post-moratorium testing. This hypothesis is supported by the plutonium depth profiles which do not reflect direct fallout from the atmosphere, as characterized by two peaks corresponding to the two major weapons testing periods, but continuously increasing plutonium and americium concentrations from 1954 to 1974. Thus, the nuclides may be coming from a large reservoir that has accumulated and mixed fallout since 1952. Such a concentration gradient for all of the nuclides requires their immobilization in the sediment after deposition.

  6. Fission Product Yields for 14 MeV Neutrons on 235U, 238U and 239Pu

    NASA Astrophysics Data System (ADS)

    Mac Innes, M.; Chadwick, M. B.; Kawano, T.

    2011-12-01

    We report cumulative fission product yields (FPY) measured at Los Alamos for 14 MeV neutrons on 235U, 238U and 239Pu. The results are from historical measurements made in the 1950s-1970s, not previously available in the peer reviewed literature, although an early version of the data was reported in the Ford and Norris review. The results are compared with other measurements and with the ENDF/B-VI England and Rider evaluation. Compared to the Laurec (CEA) data and to ENDF/B-VI evaluation, good agreement is seen for 235U and 238U, but our FPYs are generally higher for 239Pu. The reason for the higher plutonium FPYs compared to earlier Los Alamos assessments reported by Ford and Norris is that we update the measured values to use modern nuclear data, and in particular the 14 MeV 239Pu fission cross section is now known to be 15-20% lower than the value assumed in the 1950s, and therefore our assessed number of fissions in the plutonium sample is correspondingly lower. Our results are in excellent agreement with absolute FPY measurements by Nethaway (1971), although Nethaway later renormalized his data down by 9% having hypothesized that he had a normalization error. The new ENDF/B-VII.1 14 MeV FPY evaluation is in good agreement with our data.

  7. Event-by-event study of prompt neutrons from 239Pu(n,f)

    SciTech Connect

    Vogt, R; Randrup, J; Pruet, J; Younes, W

    2009-07-23

    Employing a recently developed Monte-Carlo model, we study the fission of {sup 240}Pu induced by neutrons with energies from thermal to just below the threshold for second chance fission. Current measurements of the mean number of prompt neutrons emitted in fission, together with less accurate measurements of the neutron energy spectra, place remarkably fine constraints on predictions of microscopic calculations. In particular, the total excitation energy of the nascent fragments must be specified to within 1MeV to avoid disagreement with measurements of the mean neutron multiplicity. The combination of the Monte-Carlo fission model with a statistical likelihood analysis also presents a powerful tool for the evaluation of fission neutron data. Of particular importance is the fission spectrum, which plays a key role in determining reactor criticality. We show that our approach can be used to develop an estimate of the fission spectrum with uncertainties several times smaller than current experimental uncertainties for outgoing neutron energies of less than 2 MeV.

  8. Event-by-Event Study of Prompt Neutrons from 239Pu

    SciTech Connect

    Vogt, R; Randrup, J; Pruet, J; Younes, W

    2010-01-15

    Employing a recently developed Monte Carlo model, we study the fission of {sup 240}Pu induced by neutrons with energies from thermal to just below the threshold for second chance fission. Current measurements of the mean number of prompt neutrons emitted in fission, together with less accurate measurements of the neutron energy spectra, place remarkably fine constraints on predictions of microscopic calculations. In particular, the total excitation energy of the nascent fragments must be specified to within 1 MeV to avoid disagreement with measurements of the mean neutron multiplicity. The combination of the Monte Carlo fission model with a statistical likelihood analysis also presents a powerful tool for the evaluation of fission neutron data. Of particular importance is the fission spectrum, which plays a key role in determining reactor criticality. We show that our approach can be used to develop an estimate of the fission spectrum with uncertainties several times smaller than current experimental uncertainties for outgoing neutron energies of less than 2 MeV.

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

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

    We compare the suitability of the anthropogenic FRNs, 137Cs and 239+240Pu as soil erosion tracers in two alpine valleys of Switzerland (Ursern Valley, Canton Uri, Central Swiss Alps and Val Piora, Ticino, Southern Alps). We sampled reference and potentially erosive sites in transects along both valleys. 137Cs measurements of soil samples were done with a Li-drifted Germanium detector and 239+240Pu with ICP-MS. Our data indicates a heterogeneous deposition of the 137Cs, since most of the fallout origins from the Chernobyl April/May 1986 accident, when large parts of the European Alps were still snow-covered. In contrast, 239+240Pu fallout originated mainly from 1950's-1960's atmospheric nuclear weapons tests, resulting in a more homogenous distribution and thus seems to be a more suitable tracer in mountainous grasslands. Soil erosion assessment using 239+240Pu as a tracer pointed to a huge dynamic and high heterogeneity of erosive processes (between sedimentation of 0.9 to 6.4 t ha1yr1 and erosion of 2.3 to 14.1 t ha1yr1 in the Ursern Valley and sedimentation of 0.7 to 77 t ha1yr1 and erosion of 1 to 5.3 t ha1yr1at Val Piora). Our study represents a novel, successful application of 239+240Pu as a tracer of soil erosion in a mountain environment.

  10. Activity ratios of 137Cs, 90Sr and 239+240Pu in environmental samples.

    PubMed

    Bossew, P; Lettner, H; Hubmer, A; Erlinger, C; Gastberger, M

    2007-01-01

    Both global and Chernobyl fallout have resulted in environmental contamination with radionuclides such as 137Cs, 90Sr and 239+240Pu. In environmental samples, 137Cs and 239+240Pu can be divided into the contributions of either source, if also the isotopes 134Cs and 238Pu are measurable, based on the known isotopic ratios in global and Chernobyl fallout. No analogous method is available for 90Sr. The activity ratios of Sr to Cs and Pu, respectively, are known for the actual fallout mainly from air filter measurements; but due to the high mobility of Sr in the environment, compared to Cs and Pu, these ratios generally do not hold for the inventory many years after deposition. In this paper we suggest a method to identify the mean contributions of global and Chernobyl fallout to total Sr in soil, sediment and cryoconite samples from Alpine and pre-Alpine regions of Austria, based on a statistical evaluation of Sr/Cs/Pu radionuclide activity ratios. Results are given for Sr:Cs, Sr:Pu and Cs:Pu ratios. Comparison with fallout data shows a strong depletion of Sr against Cs and Pu. PMID:17407799

  11. Alpha-particle emission probabilities in the decay of 240Pu.

    PubMed

    Sibbens, G; Pommé, S; Altzitzoglou, T; García-Toraño, E; Janssen, H; Dersch, R; Ott, O; Sánchez, A Martín; Montero, M P Rubio; Loidl, M; Coron, N; de Marcillac, P; Semkow, T M

    2010-01-01

    Sources of enriched (240)Pu were prepared by vacuum evaporation on quartz substrates. High-resolution alpha-particle spectrometry of (240)Pu was performed with high statistical accuracy using silicon detectors and with low statistical accuracy using a bolometer. The alpha-particle emission probabilities of six transitions were derived from the spectra and compared with literature values. Additionally, some alpha-particle emission probabilities were derived from gamma-ray intensity measurements with a high-purity germanium detector. The alpha-particle emission probabilities of the three main transitions at 5168.1, 5123.6 and 5021.2 keV were derived from seven aggregate spectra analysed with five different fit functions and the results were compatible with evaluated data. Two additional weak peaks at 4863.5 and 4492.0 keV were fitted separately, using the exponential of a polynomial function to represent the underlying tailing of the larger peaks. The peak at 4655 keV could not be detected by alpha-particle spectrometry, while gamma-ray spectrometry confirms that its intensity is much lower than expected from literature.

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

    SciTech Connect

    Sampson, T.E.

    1992-05-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2013-04-01

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

  14. Microscopic modeling of mass and charge distributions in the spontaneous fission of 240Pu

    DOE PAGES

    Sandhukhan, Jhilam; Nazarewicz, Witold; Schunck, Nicolas

    2016-01-20

    We propose a methodology to calculate microscopically the mass and charge distributions of spontaneous fission yields. We combine the multidimensional minimization of collective action for fission with stochastic Langevin dynamics to track the relevant fission paths from the ground-state configuration up to scission. The nuclear potential energy and collective inertia governing the tunneling motion are obtained with nuclear density functional theory in the collective space of shape deformations and pairing. As a result, we obtain a quantitative agreement with experimental data and find that both the charge and mass distributions in the spontaneous fission of 240Pu are sensitive both tomore » the dissipation in collective motion and to adiabatic fission characteristics.« less

  15. Induced Fission of (240)Pu within a Real-Time Microscopic Framework.

    PubMed

    Bulgac, Aurel; Magierski, Piotr; Roche, Kenneth J; Stetcu, Ionel

    2016-03-25

    We describe the fissioning dynamics of ^{240}Pu from a configuration in the proximity of the outer fission barrier to full scission and the formation of the fragments within an implementation of density functional theory extended to superfluid systems and real-time dynamics. The fission fragments emerge with properties similar to those determined experimentally, while the fission dynamics appears to be quite complex, with many excited shape and pairing modes. The evolution is found to be much slower than previously expected, and the ultimate role of the collective inertia is found to be negligible in this fully nonadiabatic treatment of nuclear dynamics, where all collective degrees of freedom (CDOF) are included (unlike adiabatic treatments with a small number of CDOF).

  16. ZPR-6 assembly 7 high {sup 240} PU core : a cylindrical assemby with mixed (PU, U)-oxide fuel and a central high {sup 240} PU zone.

    SciTech Connect

    Lell, R. M.; Schaefer, R. W.; McKnight, R. D.; Tsiboulia, A.; Rozhikhin, Y.; Nuclear Engineering Division; Inst. of Physics and Power Engineering

    2007-10-01

    Over a period of 30 years more than a hundred Zero Power Reactor (ZPR) critical assemblies were constructed at Argonne National Laboratory. The ZPR facilities, ZPR-3, ZPR-6, ZPR-9 and ZPPR, were all fast critical assembly facilities. The ZPR critical assemblies were constructed to support fast reactor development, but data from some of these assemblies are also well suited to form the basis for criticality safety benchmarks. Of the three classes of ZPR assemblies, engineering mockups, engineering benchmarks and physics benchmarks, the last group tends to be most useful for criticality safety. Because physics benchmarks were designed to test fast reactor physics data and methods, they were as simple as possible in geometry and composition. The principal fissile species was {sup 235}U or {sup 239}Pu. Fuel enrichments ranged from 9% to 95%. Often there were only one or two main core diluent materials, such as aluminum, graphite, iron, sodium or stainless steel. The cores were reflected (and insulated from room return effects) by one or two layers of materials such as depleted uranium, lead or stainless steel. Despite their more complex nature, a small number of assemblies from the other two classes would make useful criticality safety benchmarks because they have features related to criticality safety issues, such as reflection by soil-like material. The term 'benchmark' in a ZPR program connotes a particularly simple loading aimed at gaining basic reactor physics insight, as opposed to studying a reactor design. In fact, the ZPR-6/7 Benchmark Assembly (Reference 1) had a very simple core unit cell assembled from plates of depleted uranium, sodium, iron oxide, U3O8, and plutonium. The ZPR-6/7 core cell-average composition is typical of the interior region of liquid-metal fast breeder reactors (LMFBRs) of the era. It was one part of the Demonstration Reactor Benchmark Program,a which provided integral experiments characterizing the important features of demonstration

  17. ZPR-6 assembly 7 high {sup 240}Pu core experiments : a fast reactor core with mixed (Pu,U)-oxide fuel and a centeral high{sup 240}Pu zone.

    SciTech Connect

    Lell, R. M.; Morman, J. A.; Schaefer, R.W.; McKnight, R.D.; Nuclear Engineering Division

    2009-02-23

    ZPR-6 Assembly 7 (ZPR-6/7) encompasses a series of experiments performed at the ZPR-6 facility at Argonne National Laboratory in 1970 and 1971 as part of the Demonstration Reactor Benchmark Program (Reference 1). Assembly 7 simulated a large sodium-cooled LMFBR with mixed oxide fuel, depleted uranium radial and axial blankets, and a core H/D near unity. ZPR-6/7 was designed to test fast reactor physics data and methods, so configurations in the Assembly 7 program were as simple as possible in terms of geometry and composition. ZPR-6/7 had a very uniform core assembled from small plates of depleted uranium, sodium, iron oxide, U{sub 3}O{sub 8} and Pu-U-Mo alloy loaded into stainless steel drawers. The steel drawers were placed in square stainless steel tubes in the two halves of a split table machine. ZPR-6/7 had a simple, symmetric core unit cell whose neutronic characteristics were dominated by plutonium and {sup 238}U. The core was surrounded by thick radial and axial regions of depleted uranium to simulate radial and axial blankets and to isolate the core from the surrounding room. The ZPR-6/7 program encompassed 139 separate core loadings which include the initial approach to critical and all subsequent core loading changes required to perform specific experiments and measurements. In this context a loading refers to a particular configuration of fueled drawers, radial blanket drawers and experimental equipment (if present) in the matrix of steel tubes. Two principal core configurations were established. The uniform core (Loadings 1-84) had a relatively uniform core composition. The high {sup 240}Pu core (Loadings 85-139) was a variant on the uniform core. The plutonium in the Pu-U-Mo fuel plates in the uniform core contains 11% {sup 240}Pu. In the high {sup 240}Pu core, all Pu-U-Mo plates in the inner core region (central 61 matrix locations per half of the split table machine) were replaced by Pu-U-Mo plates containing 27% {sup 240}Pu in the plutonium

  18. Reactor Decay Heat in {sup 239}Pu: Solving the {gamma} Discrepancy in the 4-3000-s Cooling Period

    SciTech Connect

    Algora, A.; Jordan, D.; Tain, J. L.; Rubio, B.; Agramunt, J.; Perez-Cerdan, A. B.; Molina, F.; Caballero, L.; Nacher, E.; Krasznahorkay, A.; Hunyadi, M. D.; Gulyas, J.; Vitez, A.; Csatlos, M.; Csige, L.; Aeysto, J.; Penttilae, H.; Moore, I. D.; Eronen, T.; Jokinen, A.

    2010-11-12

    The {beta} feeding probability of {sup 102,104,105,106,107}Tc, {sup 105}Mo, and {sup 101}Nb nuclei, which are important contributors to the decay heat in nuclear reactors, has been measured using the total absorption technique. We have coupled for the first time a total absorption spectrometer to a Penning trap in order to obtain sources of very high isobaric purity. Our results solve a significant part of a long-standing discrepancy in the {gamma} component of the decay heat for {sup 239}Pu in the 4-3000 s range.

  19. Time-dependent local and average structural evolution of δ-phase 239Pu-Ga alloys

    DOE PAGES

    Smith, Alice I.; Page, Katharine L.; Siewenie, Joan E.; Losko, Adrian S.; Vogel, Sven C.; Gourdon, Olivier A.; Richmond, Scott; Saleh, Tarik A.; Ramos, Michael; Schwartz, Daniel S.

    2016-08-05

    Here, plutonium metal is a very unusual element, exhibiting six allotropes at ambient pressure, between room temperature and its melting point, a complicated phase diagram, and a complex electronic structure. Many phases of plutonium metal are unstable with changes in temperature, pressure, chemical additions, or time. This strongly affects structure and properties, and becomes of high importance, particularly when considering effects on structural integrity over long periods of time [1]. This paper presents a time-dependent neutron total scattering study of the local and average structure of naturally aging δ-phase239Pu-Ga alloys, together with preliminary results on neutron tomography characterization.

  20. Reactor decay heat in 239Pu: solving the γ discrepancy in the 4-3000-s cooling period.

    PubMed

    Algora, A; Jordan, D; Taín, J L; Rubio, B; Agramunt, J; Perez-Cerdan, A B; Molina, F; Caballero, L; Nácher, E; Krasznahorkay, A; Hunyadi, M D; Gulyás, J; Vitéz, A; Csatlós, M; Csige, L; Aysto, J; Penttilä, H; Moore, I D; Eronen, T; Jokinen, A; Nieminen, A; Hakala, J; Karvonen, P; Kankainen, A; Saastamoinen, A; Rissanen, J; Kessler, T; Weber, C; Ronkainen, J; Rahaman, S; Elomaa, V; Rinta-Antila, S; Hager, U; Sonoda, T; Burkard, K; Hüller, W; Batist, L; Gelletly, W; Nichols, A L; Yoshida, T; Sonzogni, A A; Peräjärvi, K

    2010-11-12

    The β feeding probability of (102,104,105,106,107)Tc, 105Mo, and 101Nb nuclei, which are important contributors to the decay heat in nuclear reactors, has been measured using the total absorption technique. We have coupled for the first time a total absorption spectrometer to a Penning trap in order to obtain sources of very high isobaric purity. Our results solve a significant part of a long-standing discrepancy in the γ component of the decay heat for 239Pu in the 4-3000 s range. PMID:21231223

  1. Energy dependence of mass, charge, isotopic, and energy distributions in neutron-induced fission of 235U and 239Pu

    NASA Astrophysics Data System (ADS)

    Pasca, H.; Andreev, A. V.; Adamian, G. G.; Antonenko, N. V.; Kim, Y.

    2016-05-01

    The mass, charge, isotopic, and kinetic-energy distributions of fission fragments are studied within an improved scission-point statistical model in the reactions 235U+n and 239Pu+n at different energies of the incident neutron. The charge and mass distributions of the electromagnetic- and neutron-induced fission of 214,218Ra, 230,232,238U are also shown. The available experimental data are well reproduced and the energy-dependencies of the observable characteristics of fission are predicted for future experiments.

  2. Comparative distribution of 241 Am and 239,240 Pu in soils around the Rocky Flats Environmental Technology Site.

    PubMed

    Ibrahim, S A; Schierman, M J; Whicker, F W

    1996-04-01

    The distribution and behavior of 241 Am and 239,240 Pu in soils from the buffer zone of the Rocky Flats Environmental Technology Site have been investigated. Concentrations of both radionuclides decreased at similar rates with soil depth. More than 80% of the total inventory of both contaminants was found in the upper 9 cm of the soils with over 50% of the inventory residing in the top 3 cm. Comparison with earlier studies indicate that the plutonium depth profile has not changed significantly over the last 25 y. The inventories of 241 Am and 239,240 Pu decreased with distance from the 903 Pad (a former waste storage site) according to a power function, and the plume extended mainly toward the east. The lateral movement of the two contaminants away from the 903 Pad was not significantly different. The median activity ratio of 241 Am: 239,240 Pu ranged from 17 to 19% and was independent of sampling location and soil depth. This observation provided further evidence that the movement of both contaminants is indistinguishable in the study area. Because of the strong correlation between the two radionuclides, 241 Am concentrations can then be used to infer 239,240 Pu by counting the 241 Am via gamma spectroscopy. PMID:8617592

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

    PubMed

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

    2014-05-01

    Anthropogenic radionuclides have been distributed globally due to nuclear weapons testing, nuclear accidents, nuclear weapons fabrication, and nuclear fuel reprocessing. While the negative consequences of this radioactive contamination are self-evident, the ubiquitous fallout radionuclides (FRNs) distribution form the basis for the use as tracers in ecological studies, namely for soil erosion assessment. Soil erosion is a major threat to mountain ecosystems worldwide. We compare the suitability of the anthropogenic FRNs, 137Cs and 239+240Pu as soil erosion tracers in two alpine valleys of Switzerland (Urseren Valley, Canton Uri, Central Swiss Alps and Val Piora, Ticino, Southern Alps). We sampled reference and potentially erosive sites in transects along both valleys. 137Cs measurements of soil samples were performed with a Li-drifted Germanium detector and 239+240Pu with ICP-MS. Our data indicates a heterogeneous deposition of the 137Cs, since most of the fallout origins from the Chernobyl April/May 1986 accident, when large parts of the European Alps were still snow-covered. In contrast, 239+240Pu fallout originated mainly from 1950s to 1960s atmospheric nuclear weapons tests, resulting in a more homogenous distribution and thus seems to be a more suitable tracer in mountainous grasslands. Soil erosion assessment using 239+240Pu as a tracer pointed to a huge dynamic and high heterogeneity of erosive processes (between sedimentation of 1.9 and 7 t ha(-1) yr(-1) and erosion of 0.2-16.4 t ha(-1) yr(-1) in the Urseren Valley and sedimentation of 0.4-20.3 t ha(-1) yr(-1) and erosion of 0.1-16.4 t ha(-1) yr(-1) at Val Piora). Our study represents a novel and successful application of 239+240Pu as a tracer of soil erosion in a mountain environment. PMID:24374184

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

    PubMed

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

    2014-05-01

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

  5. Promotion of pulmonary carcinogenesis by plutonium particle aggregation following inhalation of /sup 239/PuO/sub 2/

    SciTech Connect

    Sanders, C.L.; McDonald, K.E.; Lauhala, K.E.

    1988-12-01

    Promotion of lung tumor formation from inhaled /sup 239/PuO/sub 2/ in rats may be associated with aggregation of plutonium particles near bronchioles. The relationship of plutonium particle aggregation in the lung and the development of lung tumors after inhalation of /sup 239/PuO/sub 2/ was studied in 664 life span rats with mean lung doses ranging from 0.35 to 20 Gy. Plutonium particle concentration and aggregation were determined from autoradiographic sections of the left lung lobe. The increase in particles/cm2 and mean number of particles per aggregate up to 20 Gy were directly proportional to lung dose. Aggregates with greater than 25 particles increased linearly with dose from 0.2% at 1.4 Gy to 8.2% at 20 Gy, in a pattern similar to increasing severity of pulmonary fibrosis and incidence of lung tumors. Lung tumor incidence increased from about 6% at 1.4 Gy to 83% at 8 Gy; no further increase in lung tumors was seen at doses greater than 8 Gy. Maximum lung tumor incidence at 8 Gy corresponded to a particle concentration of 130/cm2 and four particles/aggregate with 4% of aggregates having greater than 25 particles. Aggregation of inhaled plutonium particles in clusters of greater than 25 particles resulted in daily doses of only a few centigray to focal tissue regions containing clustered particles, yet these doses appeared sufficient to cause pulmonary fibrosis and promotion of pulmonary carcinogenesis.

  6. Measurement of 239Pu in urine samples at ultra-trace levels using a 1 MV compact AMS system

    NASA Astrophysics Data System (ADS)

    Hernández-Mendoza, H.; Chamizo, E.; Yllera, A.; García-León, M.; Delgado, A.

    2010-04-01

    Routine bioassay monitoring of Pu intake in exposed workers of research and nuclear industry is usually performed by alpha spectrometry. This technique involves large sample volumes of urine and time-consuming preparative and counting protocols. Compact accelerator mass spectrometry (AMS) facilities make feasible the determination of ultra low-level Pu activity concentrations and Pu isotopic ratios in biological samples (blood, urine and feces), being a rapid and cost-effective measurement technique. The plutonium results in urine samples presented here have been obtained on the 1 MV compact AMS system sited at the Centro Nacional de Aceleradores (CNA), in Seville, Spain. In this work, a different methodological approach has been developed alternative to the "classical" preparation of urine samples for alpha spectrometry. The procedure avoids the Pu precipitation step, and involves acid sample evaporation and acid digestion in a microwave oven. Finally, purification of plutonium was achieved by using chromatography columns filled up with BioRad AG1X2 anion exchange resin (Bio-Rad Laboratories Inc.). The total time needed for analysis is about 10 h, unlike the "classical" methods based on alpha spectrometry which need about 1 week. At present, it has been demonstrated that this method allows quantifying 239Pu activity concentrations in urine of, at least, 30 μBq (13 fg 239Pu). We can conclude that the procedure would be suitable to perform in vitro routine bioassay measurements. Moreover, the innovative application of AMS opens new and interesting analytical alternatives in this field.

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

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

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

    DOE PAGES

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

    2016-06-23

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

  9. Pulmonary retention and tissue distribution of {sup 239}Pu nitrate in F344 rats and syrian hamsters inhaling carbon tetrachloride

    SciTech Connect

    Benson, J.M.; Barr, E.B.; Lundgren, D.L.; Nikula, K.J.

    1994-11-01

    Carbon tetrachloride (CCl{sub 4}) has been used extensively in the nuclear weapons industry, so it is possible that nuclear plant workers have been exposed to CCl{sub 4} and plutonium compounds. Potential for future exposure exists during {open_quotes}cleanup{close_quotes} operations at weapon production sites such as the Hanford, Washington, and Rocky Flats, Colorado, facilities. The current Threshold Limit Value for CCl{sub 4} is 5 ppm; however, concentrations of CCl{sub 4} occurring in the nuclear weapons facilities over the past 40-50 y are unknown and may have exceeded this value. The pilot study described in this report is designed to determine whether subchronic inhalation of CCl{sub 4} by CDF{sup register}(F-344)/CrlBR rats and Syrian golden hamsters, at concentrations expected to produce some histologic changes in liver, alters the hepatic retention and toxic effects of inhaled {sup 239}Pu nitrate {sup 239}Pu(NO{sub 3}){sub 4}.

  10. Comparison of early mortality in baboons and dogs after inhalation of /sup 239/PuO/sub 2/

    SciTech Connect

    Bair, W.J.; Metivier, H.; Park, J.F.; Masse, R.; Stevens, D.L.; Lafuma, J.; Watson, C.R.; Nolibe, D.

    1980-06-01

    Results from experiments with baboons were compared with those from experiments with dogs to determine the relative sensitivity of the two species to early mortality from inhaled /sup 239/PuO/sub 2/. To ensure a valid comparison of data developed at two laboratories, methodology differences were minimized by establishing a common pool of raw data, using the same computer programs to analyze the data, and standardizing assumptions regarding the calculation of plutonium concentration in lungs. Several comparison methods were used involving variations in estimating different parameters used in these calculations. Although nearly all comparisons suggested baboons were slightly more sensitive, none of the methods for comparing the relationship between dose and survival time showed consistently significant differences between baboons and dogs. Although the baboons were physiologically and morphologically immature when exposed to plutonium, whereas the dogs were mature, we concluded that adult baboons and dogs are similarly sensitive to the early effects of inhaled /sup 239/PuO/sub 2/. Since only early mortality was considered in this comparison, the results do not apply to possible late effects caused by much lower levels of plutonium than were used in these experiments.

  11. Mass Yields and Average Total Kinetic Energy Release in Fission for 235U, 238U, and 239Pu

    NASA Astrophysics Data System (ADS)

    Duke, Dana

    2015-10-01

    Mass yield distributions and average total kinetic energy (TKE) in neutron induced fission of 235U, 238U, and 239Pu targets were measured with a gridded ionization chamber. Despite decades of fission research, our understanding of how fragment mass yields and TKE depend on incident neutron energy is limited, especially at higher energies (above 5-10 MeV). Improved accuracy in these quantities is important for nuclear technology as it enhances our simulation capabilities and increases the confidence in diagnostic tools. The data can also guide and validate theoretical fission models where the correlation between the fragment mass and TKE is of particular value for constraining models. The Los Alamos Neutron Science Center - Weapons Neutron Research (LANSCE - WNR) provides a neutron beam with energies from thermal to hundreds of MeV, well-suited for filling in the gaps in existing data and exploring fission behavior in the fast neutron region. The results of the studies on target nuclei 235U, 238U, and 239Pu will be presented with a focus on exploring data trends as a function of neutron energy from thermal through 30 MeV. Results indicate clear evidence of structure due to multi-chance fission in the TKE . LA-UR-15-24761.

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

    SciTech Connect

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

    1989-12-01

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

  13. 239,240Pu and inorganic substances in aerosols from the vicinity of a waste isolation pilot plant: the importance of resuspension.

    PubMed

    Arimoto, R; Kirchner, T; Webb, J; Conley, M; Stewart, B; Schoep, D; Walthall, M

    2002-10-01

    Aerosol samples were collected and analyzed to characterize the spatial and temporal variations in the concentrations of plutonium and selected inorganic substances in the atmosphere around the Waste Isolation Pilot Plant (WIPP). High-volume aerosol sampling was conducted at three sites: (1) On Site, (2) Near Field, and (3) Cactus Flats. 239,240Pu was determined by alpha spectrometry following chemical separations; mass loadings were determined gravimetrically. A separate set of low-volume aerosol samples was analyzed for major ions using ion chromatography and for trace elements by inductively-coupled plasma emission spectrometry and mass spectrometry. The average 239,240Pu activity concentrations in total suspended particle (TSP) samples (12 to 16 nBq m(-3)) were consistent with those previously reported, but they varied strongly with season, with the highest values generally in spring. Further, the 239,240Pu activity concentrations were comparable among the three sites, and therefore there was no evidence for elevated 239,240Pu activities due to WIPP operations. The fraction of the 239,240Pu activity concentrations in the PM10, samples (particles less than 10 microm diameter) relative to TSP was lower than the corresponding PM10/TSP ratios of either high-volume mass or several inorganics (sulfate, aluminum or lead), indicating that 239,240Pu tends to be on large particles. Aerosol mass loadings (microg m(-3)) and 239,240Pu activity concentrations were correlated for all sets of samples, but at On Site, the TSP samples showed higher mass to 239,240Pu ratios than the other sites. Thus activities or processes occurring at or near the WIPP site evidently produced aerosols that contributed to the mass loadings but contained less 239,244Pu than ambient aerosols. About 63% of the variability in 239,240Pu activity concentrations was explained by wind travel, sampling location, length of the sampling interval, and aerosol mass. 239,240Pu activity concentrations also were

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

    SciTech Connect

    Suseno, Heny; Wisnubroto, Djarot S.

    2014-03-24

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

  15. Evaluating the 239Pu prompt fission neutron spectrum induced by thermal to 30 MeV neutrons

    DOE PAGES

    Neudecker, Denise; Talou, Patrick; Kawano, Toshihiko; Kahler, Albert Comstock; Rising, Michael Evan; White, Morgan Curtis

    2016-03-15

    We present a new evaluation of the 239Pu prompt fission neutron spectrum (PFNS) induced by thermal to 30 MeV neutrons. Compared to the ENDF/B-VII.1 evaluation, this one includes recently published experimental data as well as an improved and extended model description to predict PFNS. For instance, the pre-equilibrium neutron emission component to the PFNS is considered and the incident energy dependence of model parameters is parametrized more realistically. Experimental and model parameter uncertainties and covariances are estimated in detail. Also, evaluated covariances are provided between all PFNS at different incident neutron energies. In conclusion, selected evaluation results and first benchmarkmore » calculations using this evaluation are briefly discussed.« less

  16. Applicability of 239Pu as a tracer for soil erosion in the wet-dry tropics of northern Australia

    NASA Astrophysics Data System (ADS)

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

    2013-01-01

    The technique of accelerator mass spectroscopy (AMS) has been employed to determine modern soil loss rates through the analysis of 239Pu profiles in soil cores from the Daly basin in Northern Territory, Australia. In areas in which soil conservation banks were not present or were only added recently (<25a) and which had a history of grazing and cultivation the measured soil loss rates over the past ∼50 years were 7.5-19.5 t ha-1 a-1. The measured rates are up to 5 times higher compared to agricultural and uncultivated areas within soil conservation banks in other parts of the catchment. High intensity seasonal rainfall combined with reduction in land cover due to grazing and episodic bush fires are primary factors influencing erosion although other impacts on the landscape such as tillage generated runoff and land clearing seem to be responsible for accelerated sediment production.

  17. Evaluating the 239Pu Prompt Fission Neutron Spectrum Induced by Thermal to 30 MeV Neutrons

    NASA Astrophysics Data System (ADS)

    Neudecker, D.; Talou, P.; Kawano, T.; Kahler, A. C.; Rising, M. E.; White, M. C.

    2016-03-01

    We present a new evaluation of the 239Pu prompt fission neutron spectrum (PFNS) induced by thermal to 30 MeV neutrons. Compared to the ENDF/B-VII.1 evaluation, this one includes recently published experimental data as well as an improved and extended model description to predict PFNS. For instance, the pre-equilibrium neutron emission component to the PFNS is considered and the incident energy dependence of model parameters is parametrized more realistically. Experimental and model parameter uncertainties and covariances are estimated in detail. Also, evaluated covariances are provided between all PFNS at different incident neutron energies. Selected evaluation results and first benchmark calculations using this evaluation are briefly discussed.

  18. Fission Product Yield Study of 235U, 238U and 239Pu Using Dual-Fission Ionization Chambers

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

    To resolve long-standing differences between LANL and LLNL regarding the correct fission basis for analysis of nuclear test data [M.B. Chadwick et al., Nucl. Data Sheets 111, 2891 (2010); H. Selby et al., Nucl. Data Sheets 111, 2891 (2010)], a collaboration between TUNL/LANL/LLNL has been established to perform high-precision measurements of neutron induced fission product yields. The main goal is to make a definitive statement about the energy dependence of the fission yields to an accuracy better than 2-3% between 1 and 15 MeV, where experimental data are very scarce. At TUNL, we have completed the design, fabrication and testing of three dual-fission chambers dedicated to 235U, 238U, and 239Pu. The dual-fission chambers were used to make measurements of the fission product activity relative to the total fission rate, as well as for high-precision absolute fission yield measurements. The activation method was employed, utilizing the mono-energetic neutron beams available at TUNL. Neutrons of 4.6, 9.0, and 14.5 MeV were produced via the 2H(d,n)3He reaction, and for neutrons at 14.8 MeV, the 3H(d,n)4He reaction was used. After activation, the induced γ-ray activity of the fission products was measured for two months using high-resolution HPGe detectors in a low-background environment. Results for the yield of seven fission fragments of 235U, 238U, and 239Pu and a comparison to available data at other energies are reported. For the first time results are available for neutron energies between 2 and 14 MeV.

  19. Sources and distributions of 137Cs, 238Pu, 239,240Pu radionuclides in the north-western Barents Sea.

    PubMed

    Zaborska, Agata; Mietelski, Jerzy Wojciech; Carroll, JoLynn; Papucci, Carlo; Pempkowiak, Janusz

    2010-04-01

    Sediment deposits are the ultimate sink for anthropogenic radionuclides entering the marine environment. The major sources of anthropogenic radionuclides to the Barents Sea are fallout from nuclear weapons tests, long range transport from other seas, and river and non-point freshwater supplies. In this study we investigated activity concentrations, ratios, and inventories of the anthropogenic radionuclides, 137Cs, 238Pu, 239,240Pu in dated sediment cores collected along a north-south transect in the northwestern Barents Sea. The data were used to evaluate the influence of different sources on the derived spatial and temporal patterns of anthropogenic radionuclides in seafloor sediment deposits. Activity concentrations of 137Cs ranged from <0.1 Bq/kg to 10.5 Bq/kg while 239,240Pu ranged from <0.01 Bq/kg to 2.74 Bq/kg and 238Pu activity concentrations ranged from <0.01 Bq/kg to 0.22 Bq/kg. Total inventories of 137Cs ranged from 29.5+/-1.5 Bq/m2 to 152.7+/-5.6 Bq/m2 and for 239,240Pu inventories (6 sediment layers only) ranged from 9.5+/-0.3 Bq/m2 to 29.7+/-0.4 Bq/m2. Source contributions varied among stations and between the investigated radionuclides. The 238Pu/239,240Pu ratios up to 0.18 indicate discharges from nuclear fuel reprocessing plants as a main contributor of plutonium. Based on 238Pu/239,240Pu ratio, it was calculated that up to 19-27% of plutonium is supplied from sources other than atmospheric global fallout. Taking into account Atlantic current flow trajectories and that both activity concentrations and inventories of plutonium negatively correlate with latitude, Sellafield is a major source for the Barents Sea. Concentrations and inventories of 137Cs correlate positively with latitude and negatively with distance from the Svalbard archipelago. The 137Cs concentrations are highest in an area of intensive melting of sea ice formed along the Siberian coast. Thus, sea ice and supplies from Svalbard may be important source of 137Cs to the Barents Sea

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

    NASA Astrophysics Data System (ADS)

    Yamada, Masatoshi; Zheng, Jian; Aono, Tatsuo

    2013-04-01

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

  1. 238Pu, 239,240Pu, 241Am, 90Sr and 137Cs in soils around nuclear research centre Rez, near Prague.

    PubMed

    Hölgye, Z; Schlesingerová, E; Tecl, J; Filgas, R

    2004-01-01

    Forty-four soil samples were taken around the nuclear research centre Rez, near Prague. The mean activity concentrations of 238Pu, 239,240Pu, 241Am, 90Sr and 137Cs in uncultivated soil were 0.010, 0.26, 0.12, 2.7 and 23 Bq.kg(-1), respectively. Contents of radionuclides in cultivated soil were lower and in forest soil higher than in uncultivated soil. The mean activity ratios of 238Pu/239,240Pu, 241Am/239,240Pu, 90Sr/239,240Pu and 239,240Pu/137Cs in uncultivated soil were 0.041, 0.47, 10.9 and 0.013, respectively. The mean activity ratios in cultivated and forest soils were close to the values given above. It follows from the results that the source of 239,240Pu, 90Sr and 137Cs in the studied area is deposition from atmospheric nuclear tests, in the case of 137Cs also deposition from Chernobyl accident. The contribution of the research centre effluents was not proved for these radionuclides. Increased activity ratio of 241Am/239,240Pu indicates the presence of 241Am in the soils studied emanating from sources other than nuclear tests. Uniform distribution of the 241Am/239,240Pu activity ratio around the nuclear research centre and the absence of an area with evidently higher activity ratio, including at sites lying in the main wind direction, suggest that the additional activity of 241Am does not originate from the nuclear research centre. The additional source might be the deposition following the Chernobyl accident.

  2. 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

  3. Characterization of ^{239,240}Pu Radionuclide Adsorption to Soil Particles and Mineral Dust Aerosols

    NASA Astrophysics Data System (ADS)

    Tatro, D. P.; Arimoto, R.; McMillan, N. J.; Barnes, M.

    2006-12-01

    The release of ^{239,240}Pu into the environment by nuclear weapons testing 50 years ago initiated the cyclic mobilization of Pu-contaminated soil particles via the resuspension of dust resulting in a widespread distribution of Pu and other radionuclides. It is unclear what enables the aeolian transport of Pu in the environment; plausible hypotheses of Pu binding to dust and soil particles include Pu adsorption to iron oxides/hydroxides, organic acids, or silicate minerals such as clays. To investigate the connections between surface soils, dust and radionuclides, samples of soil and/or dust were collected from the Project Gnome Site in Eddy County, NM, the Jemez Mountains near Los Alamos, NM, and two 50-year old attics and wind-blown dust in Big Spring, TX. This study tests the hypothesis that Pu is adsorbed onto Fe oxides and hydroxides that coat dust/soil particles. The samples are generally low in organic carbon (0.2 - 4.8%, except for the unburned Los Alamos sample at 9.4%), as measured by LOI (Loss On Ignition) at 360 °C. The citrate-bicarbonate-dithionite method (CDB) of Fe oxide removal, first proposed by Mehra and Jackson in 1960, was used to selectively extract Fe oxides from the samples while leaving silicate Fe intact. Chemical digestion of each sample creates two fractions, the extracted supernatant and a solid pellet residue. If the Pu were associated with Fe oxides, then Fe and Pu should both be selectively removed from the bulk sample during the CBD process, leaving the pellet depleted in Fe and Pu and the supernatant enriched. For Fe, this was confirmed by scanning electron microscope and petrographic analyses. Preliminary radiochemical analyses of Pu activity also verify this hypothesis. Pu activity is significantly lower in pellets than bulk samples (Pu activitypellet/Pu activitybulk average = 0.07, range 0.02-0.12); Pu activity in supernatants is significantly higher than in bulk samples (Pu activitysupernatant/Pu activitybulk average = 4

  4. Comparison of {sup 241}Am, {sup 239,240}Pu, and {sup 137}Cs concentrations in soil around Rocky Flats

    SciTech Connect

    Hulse, S.E.; Ibrahim, S.A.; Whicker, F.W.; Chapman, P.L.

    1999-03-01

    Gamma spectroscopy measurements were used to estimate concentrations of {sup 241}Am and {sup 137}Cs in soil profiles to depths of 21 cm at on-site and off-site locations around the Rocky Flats Environmental Technology Site and at regional background locations east of the Front Range between Colorado`s borders with New Mexico and Wyoming. Concentrations of these radionuclides were compared with concentrations of {sup 239,240}Pu in the same samples. Concentrations of {sup 241}Am in soil from depths of 0 to 3 cm decreased in an easterly direction from more than 5.3 kBq kg{sup {minus}1} 5 to 7 km away at a rate that was nearly proportional to the inverse square of distance. Deposits of {sup 137}Cs were ubiquitous, averaging 0.12 kBq kg{sup {minus}1} in soil from depths of 0 to 3 cm, but were unevenly distributed around Rocky Flats and the regional background locations. Deviations from the uniform exponential rate at which soil concentrations of {sup 137}Cs typically decreased with depth, {minus}0.25 cm{sup {minus}1} at undisturbed sites, enabled the authors to determine that about 10% of their sampling sites had been disturbed by erosion, tillage, or other factors. The mean rate at which {sup 239,240}Pu decreased with depth was about the same, {minus}0.23 cm{sup {minus}1}, throughout the study area. Soil concentrations of {sup 241}Am decreased with depth at a similar mean rate of {minus}0.22 cm{sup {minus}1} at locations close to the 903 pad where measurements were robust. Ratios between {sup 241}Am or {sup 239,240}Pu and {sup 137}Cs proved more useful for delineating the extent and pattern of contamination from Rocky Flats than did activity concentrations in soil.

  5. Comparison of 241Am, (239,240)Pu and 137Cs concentrations in soil around rocky flats.

    PubMed

    Hulse, S E; Ibrahim, S A; Whicker, F W; Chapman, P L

    1999-03-01

    Gamma spectroscopy measurements were used to estimate concentrations of 241Am and 137Cs in soil profiles to depths of 21 cm at on-site and off-site locations around the Rocky Flats Environmental Technology Site and at regional background locations east of the Front Range between Colorado's borders with New Mexico and Wyoming. Concentrations of these radionuclides were compared with concentrations of (239,240)Pu in the same samples. Concentrations of 241Am in soil from depths of 0 to 3 cm decreased in an easterly direction from more than 5.3 kBq kg(-1) near the 903 pad to background levels of 1.3 Bq kg(-1) 5 to 7 km away at a rate that was nearly proportional to the inverse square of distance. Deposits of 137Cs were ubiquitous, averaging 0.12 kBq kg(-1) in soil from depths of 0 to 3 cm, but were unevenly distributed around Rocky Flats and the regional background locations. Deviations from the uniform exponential rate at which soil concentrations of 137Cs typically decreased with depth, -0.25 cm(-1) at undisturbed sites, enabled us to determine that about 10% of our sampling sites had been disturbed by erosion, tillage, or other factors. The mean rate at which (239,240)Pu decreased with depth was about the same, -0.23 cm(-1), throughout the study area. Soil concentrations of 241Am decreased with depth at a similar mean rate of -0.22 cm(-1) at locations close to the 903 pad where measurements were robust. Ratios between 241Am or (239,240)Pu and 137Cs proved more useful for delineating the extent and pattern of contamination from Rocky Flats than did activity concentrations in soil. PMID:10025653

  6. [Chromosome and cytome analysis of the somatic cells of nuclear-chemical production workers with incorporated 239Pu].

    PubMed

    Timoshevskiĭ, V A; Lebedev, I N; Vasil'ev, S A; Sukhanova, N N; Iakovleva, Iu S; Torkhova, N B; Puzyrev, V P

    2010-01-01

    The analysis of plutonium production factors has been carried out by using two methodical approaches: assessment of chromosomal aberrations level in routine and G-banded metaphases and molecular-cytogenetic investigation of aneugenic/clastogenic damages in cytokinesis-block binuclear lymphocytes by FISH with centromere specific DNA probes. The obtaining data point out for the first time about both aneugenic and clastogenic influences of incorporated 239Pu with activity range from 0.37 to 6.95 kBq. Correlation analysis of chromosome aberrations with cytome abnormalities allowed finding significant connection between number parameters of metaphase and interphase approaches. The results of this study support the suggestion that aberrant chromosomes are involved preferable in aneugenic events. The FISH technique in binucleated cytokinesis-blocked lymphocytes allows extending of detecting spectrum of chromosome damages and glance of aneugenic mechanisms. Correlations between metaphase and interphase-FISH results point out a high sensitivity of FISH cytome assay, which could be used as an independent test for detection both clastogenic and aneugenic environment influences.

  7. Relative effectiveness of {sup 239}Pu and some other internal emitters for bone cancer induction in beagles

    SciTech Connect

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

    1994-10-01

    The toxicity ratio (relative effectiveness per gray of average skeletal dose) has been estimated for bone cancer induction in beagles injected as young adults with a number of bone-seeking internal emitters. These experiments yielded calculated toxicity ratios ({+-} SD) relative to {sup 226}Ra = 1.0 of {sup 239}Pu = 16 {+-} 5 (single exposure to monomeric Pu) and 32 {+-} 10 (continuous exposure from an extraskeletal deposit in the body), {sup 224}Ra = 16 {+-} 5 (chronic exposure) and approximately 6 {+-} 2 (single exposure), {sup 228}Th = 8.5 {+-} 2.3, {sup 241}Am = 6 {+-} 0.8, {sup 228}Ra = 2.0 {+-} 0.5, {sup 249}Cf = 6 {+-} 3, {sup 252}Cf = 4 {+-}2, {sup 90}Sr = 1.0 {+-} 0.5 (for high doses) and 0.05 {+-} 0.03 (for low doses) and 0.01 {+-} 0.01 (for extremely low doses). Because no skeletal malignancies were observed among beagles given only {sup 253}Es, the toxicity ratio is undefined. 43 refs., 2 tabs.

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

    NASA Astrophysics Data System (ADS)

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

    2016-09-01

    A technique to determine the isotopic constituents of a mixed actinide sample has been proposed by a coincident alpha-conversion electron measurement. This presents a unique signature to allow the unfolding of isotopes that possess overlapping alpha particle energy and reduce backgrounds of an unseparated sample. The work presented here are results of conversion electron spectroscopy of 241Am, 238Pu and 239Pu using a dual-stage peltier-cooled 25 mm2 silicon drift detector and alpha spectroscopy with a passivated ion implanted planar silicon detector. The conversion electron spectra were evaluated from 20-55 keV based on fits to the dominant conversion electron emissions, which allowed the relative conversion electron emission intensities to be determined. These measurements provide crucial singles spectral information and calibration to aid in the coincident measurement approach. Furthermore, an alpha-conversion electron spectrometer was assembled using the silicon based detectors described and results of a coincident spectrum analysis is reported for 241Am.

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

    PubMed

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

    2008-07-01

    This study concerns an arctic marine environment that was contaminated by actinide elements after a nuclear accident in 1968, the so-called Thule accident In this study we have analyzed five isolated hot particles as well as sediment samples containing particles from the weapon material for the determination of the nuclear fingerprint of the accident. We report that the fissile material in the hydrogen weapons involved in the Thule accident was a mixture of highly enriched uranium and weapon-grade plutonium and that the main fissile material was 235U (about 4 times more than the mass of 239Pu). In the five hot particles examined, the measured uranium atomic ratio was 235U/238U = 1.02 +/- 0.16 and the Pu-isotopic ratios were as follows: 24Pu/239Pu = 0.0551 +/- 0.0008 (atom ratio), 238Pu/239+240Pu = 0.0161 +/- 0.0005 (activity ratio), 241Pu/239+240Pu = 0.87 +/- 0.12 (activity ratio), and 241Am/ 239+240Pu = 0.169 +/- 0.005 (activity ratio) (reference date 2001-10-01). From the activity ratios of 241Pu/241Am, we estimated the time of production of this weapon material to be from the late 1950s to the early 1960s. The results from reanalyzed bulk sediment samples showed the presence of more than one Pu source involved in the accident, confirming earlier studies. The 238Pu/239+240PU activity ratio and the 240Pu/ 239Pu atomic ratio were divided into at least two Pu-isotopic ratio groups. For both Pu-isotopic ratios, one ratio group had identical ratios as the five hot particles described above and for the other groups the Pu isotopic ratios were lower (238Pu/ 239+240PU activity ratio approximately 0.01 and the 240Pu/P239Pu atomic ratio 0.03). On the studied particles we observed that the U/Pu ratio decreased as a function of the time these particles were present in the sediment. We hypothesis that the decrease in the ratio is due to a preferential leaching of U relative to Pu from the particle matrix. PMID:18677996

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

    PubMed

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

    2008-07-01

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

  11. [Quantitative evaluation of 90Sr, 137Cs, 239Pu, 241Am transfer from polluted soil to gastric and intestine juice of cows].

    PubMed

    Chizhevskiĭ, I V

    2001-01-01

    Quantitative parameters of 90Sr, 137Cs, 239Pu and 241Am transfer from solid phase of soil to gastric, intestine juice of cows as well as to imitating solutions have been estimated on the base of results of laboratory incubation experiments. A prevailing role of enzyme complex and microflora of gastrointestinal tract in radionuclides transfer from solid phase of soil to solution has been shown. PMID:11605246

  12. /sup 237/Np and /sup 239/Pu solution behavior during hydrothermal testing of simulated nuclear waste glass with basalt and steel

    SciTech Connect

    Schramke, J.A.; Simonson, S.A.; Coles, D.G.

    1984-09-01

    A series of hydrothermal experiments were carried out on /sup 237/Np- and /sup 239/Pu-doped PNL 76-68 glass, synthetic basalt groundwater, basalt, and cast steel. Experiments of duration were conducted in Dickson-type rocking autoclaves at 200/sup 0/C and 30 MPa, with an initial fluid to solid weight ratio of 10:1. The tests carried out were: glass and groundwater; glass, basalt, and groundwater; glass, steel, and groundwater; and glass, steel, basalt, and groundwater. Unfiltered, 4000 A filtered, and 18 A filtered solutions were analyzed to determine the concentrations of radionuclides in solution and those associated with colloids. In all four experiments, /sup 237/Np and /sup 239/Pu were present in solution in quantities at or below the analytical detection limits. The only detectable differences in radionuclide concentrations between the four experiments were brought about by changes in the amounts of colloidally associated radionuclides. Besalt added to the glass and groundwater system increased the quantities of the colloidally associated /sup 237/Np and /sup 239/Pu by an order of magnitude. The addition of steel to the glass and groundwater system reduced the colloidally associated radionuclides to levels below detection limits. The effects of both steel and basalt on the glass and groundwater system seemed to cancel out, and the colloidally associated radionuclide concentrations were similar to the observed levels in the glass plus groundwater system. These variations in the quantities of the colloidally associated radionuclides did not appear to be correlated with other changes in the quantities or composition of the colloidal material in solution. Other than /sup 237/Np and /sup 239/Pu, silica was the only constituent of the colloids in these experiments. The amounts of colloidal silica did not vary significantly between the four experiments. 7 references, 7 figures.

  13. Migration of (137)Cs, (90)Sr, and (239+240)Pu in Mediterranean forests: influence of bioavailability and association with organic acids in soil.

    PubMed

    Guillén, J; Baeza, A; Corbacho, J A; Muñoz-Muñoz, J G

    2015-06-01

    The understanding of downward migration of anthropogenic radionuclides in soil is a key factor in the assessment of their environmental behavior. There are several factors that can affect this process, such as the radionuclide source, their chemical form, soil and environmental characteristics, etc. Two Mediterranean pinewood ecosystems in Spain, which were affected mainly by global fallout, were selected to assess the migration of (137)Cs, (90)Sr, and (239+240)Pu. Using auxiliary modeling (diffusion-convection equation and compartmental model), it followed from field observations that the migration velocities of (90)Sr and (239+240)Pu were similar and higher than that of (137)Cs. The downward migration of radionuclides can be considered a consequence of their association with soil particles. A sequential speciation procedure also confirmed that (90)Sr was the most bioavailable radionuclide followed by (239+240)Pu and (137)Cs. Although this can explain the different velocity of (90)Sr and (137)Cs, bioavailability could not explain by itself the similar velocities of (239+240)Pu and (90)Sr. The presence of organic acids in the soil can also influence the migration of radionuclides attached to them, which decreased in the order: (239+240)Pu > (90)Sr > (137)Cs. Thus, the joint consideration of bioavailable and humic + fulvic acid fractions can explain the observed differences in the downward velocities. PMID:25827576

  14. Migration of (137)Cs, (90)Sr, and (239+240)Pu in Mediterranean forests: influence of bioavailability and association with organic acids in soil.

    PubMed

    Guillén, J; Baeza, A; Corbacho, J A; Muñoz-Muñoz, J G

    2015-06-01

    The understanding of downward migration of anthropogenic radionuclides in soil is a key factor in the assessment of their environmental behavior. There are several factors that can affect this process, such as the radionuclide source, their chemical form, soil and environmental characteristics, etc. Two Mediterranean pinewood ecosystems in Spain, which were affected mainly by global fallout, were selected to assess the migration of (137)Cs, (90)Sr, and (239+240)Pu. Using auxiliary modeling (diffusion-convection equation and compartmental model), it followed from field observations that the migration velocities of (90)Sr and (239+240)Pu were similar and higher than that of (137)Cs. The downward migration of radionuclides can be considered a consequence of their association with soil particles. A sequential speciation procedure also confirmed that (90)Sr was the most bioavailable radionuclide followed by (239+240)Pu and (137)Cs. Although this can explain the different velocity of (90)Sr and (137)Cs, bioavailability could not explain by itself the similar velocities of (239+240)Pu and (90)Sr. The presence of organic acids in the soil can also influence the migration of radionuclides attached to them, which decreased in the order: (239+240)Pu > (90)Sr > (137)Cs. Thus, the joint consideration of bioavailable and humic + fulvic acid fractions can explain the observed differences in the downward velocities.

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

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

  16. Energy measurement of prompt fission neutrons in 239Pu(n,f) for incident neutron energies from 1 to 200 MeV

    SciTech Connect

    Haight, Robert C; Devlin, Matthew J; Nelson, Ronald O; O' Donnell, John M; Chatillon, Audrey; Granier, Thierry; Taieb, Julien; Belier, Gilbert; Laurent, Benoit; Noda, Shusaku

    2010-01-01

    An experimental campaign was started in 2002 in the framework of a collaboration belween CEA-DAM and the Los Alamos National Laboratory to measure the prompt fission neutron spectra (PFNS) for incident neutron energies from 1 to 200 MeV with consistent error uncertainties over the whole energy range. The prompt neutron spectra in {sup 235,238}U(n,f) and {sup 237}Np(n,f) have been already studied successfully. A first attempt to characterize the prompt neutrons emitted during the fission of the {sup 239}Pu was done in 2007. This contribution will focus on the results obtained during the final experiment to measure the PFNS in {sup 239}Pu(n,f) performed in 2008. Prompt fission neutron spectra in the neutron-induced fission of {sup 239}Pu have been measured for incident neutron energies from 1 to 200 MeV at the Los Alamos Neutron Science Center. Mean energies obtained from the spectra are discussed and compared to theoretical model calculation.

  17. Determination of fission neutron transmission through waste matrix material using neutron signal correlation from active assay of {sup 239}Pu

    SciTech Connect

    Hollas, C.L.; Arnone, G.; Brunson, G.; Coop, K.

    1996-09-01

    The accuracy of TRU (transuranic) waste assay using the differential die-away technique depends upon significant corrections to compensate for the effects of the matrix material in which the TRU waste is located. The authors have used a new instrument, the Combined Thermal/Epithermal Neutron (CTEN) instrument for the assay of TRU waste, to develop methods to improve the accuracy of these corrections. Neutrons from a pulsed 14-MeV neutron generator are moderated in the walls of the CTEN cavity and induce fission in the TRU material. The prompt neutrons from these fission events are detected in cadmium-wrapped {sup 3}He neutron detectors. They report new methods of data acquisition and analysis to extract correlation in the neutron signals resulting form fission during active interrogation. They use the correlation information in conjunction with the total number of neutrons to determine the fraction of fission neutrons transmitted through the matrix material into the {sup 3}He detectors. This determination allows them to cleanly separate the matrix effects into two processes: matrix modification upon the neutron interrogating flux and matrix modification upon the fraction of fission neutrons transmitted to the neutron detectors. This transmission information is also directly applied in a neutron multiplicity analysis in the passive assay of {sup 240}Pu.

  18. Determination of (241)Pu by the method of disturbed radioactive equilibrium using 2πα-counting and precision gamma-spectrometry.

    PubMed

    Alekseev, I; Kuzmina, T

    2016-04-01

    A simple technique is proposed for the determination of the content of (241)Pu, which is based on disturbance of radioactive equilibrium in the genetically related (237)U←(241)Pu→(241)Am decay chain of radionuclides, with the subsequent use of 2πα-counting and precision gamma-spectroscopy for monitoring the process of restoration of that equilibrium. It has been shown that the data on dynamics of accumulation of the daughter (241)Am, which were obtained from the results of measurements of α- and γ-spectra of the samples, correspond to the estimates calculated for the chain of two genetically related radionuclides, the differences in the estimates of (241)Pu radioactivity not exceeding 2%. Combining the different methods of registration (2πα-counting, semiconductor alpha- and gamma-spectrometry) enables the proposed method to be efficiently applied both for calibration of (241)Pu-sources (from several hundreds of kBq and higher) and for radioisotopic analysis of plutonium mixtures. In doing so, there is a deep purification of (241)Pu from its daughter decay products required due to unavailability of commercial detectors that could make it possible, based only on analysis of alpha-spectra, to conduct quantitative analysis of the content of (238)Pu and (241)Am. PMID:26868275

  19. Determination of (241)Pu by the method of disturbed radioactive equilibrium using 2πα-counting and precision gamma-spectrometry.

    PubMed

    Alekseev, I; Kuzmina, T

    2016-04-01

    A simple technique is proposed for the determination of the content of (241)Pu, which is based on disturbance of radioactive equilibrium in the genetically related (237)U←(241)Pu→(241)Am decay chain of radionuclides, with the subsequent use of 2πα-counting and precision gamma-spectroscopy for monitoring the process of restoration of that equilibrium. It has been shown that the data on dynamics of accumulation of the daughter (241)Am, which were obtained from the results of measurements of α- and γ-spectra of the samples, correspond to the estimates calculated for the chain of two genetically related radionuclides, the differences in the estimates of (241)Pu radioactivity not exceeding 2%. Combining the different methods of registration (2πα-counting, semiconductor alpha- and gamma-spectrometry) enables the proposed method to be efficiently applied both for calibration of (241)Pu-sources (from several hundreds of kBq and higher) and for radioisotopic analysis of plutonium mixtures. In doing so, there is a deep purification of (241)Pu from its daughter decay products required due to unavailability of commercial detectors that could make it possible, based only on analysis of alpha-spectra, to conduct quantitative analysis of the content of (238)Pu and (241)Am.

  20. Study of Photon Strength Function of Actinides: the Case of (235)U, (238)Np and (241)Pu

    SciTech Connect

    Guerrero, C.; Koehler, Paul Edward; N_TOF collaboration,

    2011-01-01

    The decay from excited levels in medium and heavy nuclei can be described in a statistical approach by means of Photon Strength Functions and Level Density distributions. The study of electromagnetic cascades following neutron capture based on the use of high efficiency detectors has been shown to be well suited for probing the properties of the Photon Strength Function of heavy (high level density) and/or radioactive (high background) nuclei. In this work we have investigated for the first time the validity of the recommended PSF of actinides, in particular {sup 235}U, {sup 238}Np and {sup 241}Pu. Our study includes the search for resonance structures in the PSF below Sn and draws conclusions regarding their existence and their characteristics in terms of energy, width and electromagnetic nature.

  1. Determination of plutonium and other transuranic elements by inductively coupled plasma mass spectrometry: A historical perspective and new frontiers in the environmental sciences

    NASA Astrophysics Data System (ADS)

    Ketterer, Michael E.; Szechenyi, Scott C.

    2008-07-01

    Inductively coupled plasma mass spectrometry (ICPMS), particularly with sector field mass analyzers (SF-ICPMS), has emerged in the past several years as an excellent analytical technique for rapid, highly sensitive determination of transuranic elements (TRU) in environmental samples. SF-ICPMS has advantages of simplicity of sample preparation, high sample throughput, widespread availability in laboratories worldwide, and relatively straightforward operation when compared to other competing mass spectrometric techniques. Arguably, SF-ICPMS is the preferred technique for routine, high-throughput determination of 237Np and the Pu isotopes, excepting 238Pu, at fg-pg levels in environmental samples. Many research groups have now demonstrated the SF-ICPMS determination of 239 + 240 Pu activities, 240Pu/ 239Pu and other Pu atom ratios in several different application areas. Many studies have examined the relative contribution of global fallout vs. local/regional Pu sources in the environment through measurement of 240Pu/ 239Pu and, in some cases, 241Pu/ 239Pu and 242Pu/ 239Pu. "Stratospheric fallout", which was deposited from thermonuclear tests, conducted largely during the 1952-1964 time period, is characterized by a well-defined 240Pu/ 239Pu of ~ 0.18, while most other sources have different ratios. Examples of local/regional Pu sources are the Nevada Test Site, the Chernobyl plume, and accidents at Palomares, Spain and Thule, Greenland. The determination of Pu activities and atom ratios has stimulated much interest in the use of Pu as a marine tracer; several studies have shown that Pu is transported over long distances by ocean currents. 240Pu/ 239Pu ratios > 0.20 in sediments and seawater of the North Pacific are ascribed to ocean current transport of fallout from the Pacific Proving Ground. In nuclear forensics, much effort is focused on detection and fingerprinting of small amounts of TRU in environmental samples consisting of bulk material or individual isolated

  2. References to Studies of 137Cs, 90Sr and 239+240Pu in the Pacific Ocean a Bibliography

    SciTech Connect

    Noshkin, V.E.

    2001-02-01

    This report contains a listing of publications known to this author on reported concentrations, reviews and discussions of {sup 137}Cs, {sup 90}Sr and {sup 239+240}Pu in seawater, sediment and the biota from parts of the North and South Pacific Ocean. Each reference has been assigned an accession number consisting of the first three letters of the first author's last name followed by the first letter of the first name, the year of the publication and an assigned number. Studies in both the coastal areas and the open ocean are included as well as those providing data within lagoons of coral atolls. Some references to the radionuclides in the Indian Ocean are also provided.

  3. A comparative study of (239,240)Pu in soil near the former Rocky Flats Nuclear Weapons Facility, Golden, CO.

    PubMed

    Margulies, Todd D; Schonbeck, Niels D; Morin-Voillequé, Normie C; James, Katherine A; LaVelle, James M

    2004-01-01

    The Rocky Flats Nuclear Weapons Plant near Golden, CO released plutonium into the environment during almost 40 years of operation. Continuing concern over possible health impacts of these releases has been heightened by lack of public disclosure of the US Department of Energy (DOE) activities. A dose reconstruction study for the Rocky Flats facilities, begun in 1990, provided a unique opportunity for concerned citizens to design and implement field studies without participation of the DOE, its contractors, or other government agencies. The Citizens Environmental Sampling Committee was formed in late 1992 and conducted a field sampling program in 1994. Over 60 soil samples, including both surface and core samples, were collected from 28 locations where past human activities would have minimal influence on contaminant distributions in soil. Cesium-137 activity was used as a means to assess whether samples were collected in undisturbed locations. The distribution of plutonium (as (239,240)Pu) in soil was consistent with past sampling conducted by DOE, the Colorado Department of Public Health and Environment, and others. Elevated levels of (239,240)Pu were found immediately east of the Rocky Flats Plant, with concentrations falling rapidly with distance from the plant to levels consistent with background from fallout. Samples collected in areas south, west, and north of the plant were generally consistent with background from fallout. No biases in past sampling due to choice of sampling locations or sampling methodology were evident. The study shows that local citizens, when provided sufficient resources, can design and implement technical studies that directly address community concerns where trust in the regulated community and/or regulators is low. PMID:15172724

  4. Fission fragment charge and mass distributions in 239Pu(n ,f ) in the adiabatic nuclear energy density functional theory

    NASA Astrophysics Data System (ADS)

    Regnier, D.; Dubray, N.; Schunck, N.; Verrière, M.

    2016-05-01

    Background: Accurate knowledge of fission fragment yields is an essential ingredient of numerous applications ranging from the formation of elements in the r process to fuel cycle optimization for nuclear energy. The need for a predictive theory applicable where no data are available, together with the variety of potential applications, is an incentive to develop a fully microscopic approach to fission dynamics. Purpose: In this work, we calculate the pre-neutron emission charge and mass distributions of the fission fragments formed in the neutron-induced fission of 239Pu using a microscopic method based on nuclear density functional theory (DFT). Methods: Our theoretical framework is the nuclear energy density functional (EDF) method, where large-amplitude collective motion is treated adiabatically by using the time-dependent generator coordinate method (TDGCM) under the Gaussian overlap approximation (GOA). In practice, the TDGCM is implemented in two steps. First, a series of constrained EDF calculations map the configuration and potential-energy landscape of the fissioning system for a small set of collective variables (in this work, the axial quadrupole and octupole moments of the nucleus). Then, nuclear dynamics is modeled by propagating a collective wave packet on the potential-energy surface. Fission fragment distributions are extracted from the flux of the collective wave packet through the scission line. Results: We find that the main characteristics of the fission charge and mass distributions can be well reproduced by existing energy functionals even in two-dimensional collective spaces. Theory and experiment agree typically within two mass units for the position of the asymmetric peak. As expected, calculations are sensitive to the structure of the initial state and the prescription for the collective inertia. We emphasize that results are also sensitive to the continuity of the collective landscape near scission. Conclusions: Our analysis confirms

  5. Event-by-event evaluation of the prompt fission neutron spectrum from 239Pu(n,f)

    SciTech Connect

    Vogt, R; Randrup, J; Brown, D A; Descalle, M A; Ormand, W E

    2011-11-28

    We have developed an improved evaluation method for the spectrum of neutrons emitted in fission of {sup 239}Pu induced by incident neutrons with energies up to 20 MeV. The covariance data, including incident energy correlations introduced by the evaluation method, were used to fix the input parameters in our event-by-event model of fission, FREYA, by applying formal statistical methods. Formal estimates of uncertainties in the evaluation were developed by randomly sampling model inputs and calculating likelihood functions based on agreement with the evaluated . Our approach is able to employ a greater variety of fission measurements than the relatively coarse spectral data alone. It also allows the study of numerous fission observables for more accurate model validation. The combination of an event-by-event Monte Carlo fission model with a statistical-likelihood analysis is thus a powerful tool for evaluation of fission-neutron data. Our empirical model FREYA follows the complete fission event from birth of the excited fragments through their decay via neutron emission until the fragment excitation energy is below the neutron separation energy when neutron emission can no longer occur. The most recent version of FREYA incorporates pre-equilibrium neutron emission, the emission of the first neutron before equilibrium is reached in the compound nucleus, and multi-chance fission, neutron evaporation prior to fission when the incident neutron energy is above the neutron separation energy. Energy, momentum, charge and mass number are conserved throughout the fission process. The best available values of fragment masses and total kinetic energies are used as inputs to FREYA. We fit three parameters that are not well under control from previous measurements: the shift in the total fragment kinetic energy; the energy scale of the asymptotic level density parameter, controlling the fragment 'temperature' for neutron evaporation; and the relative excitation of the

  6. Fission Product Data Measured at Los Alamos for Fission Spectrum and Thermal Neutrons on 239Pu, 235U, 238U

    NASA Astrophysics Data System (ADS)

    Selby, H. D.; Mac Innes, M. R.; Barr, D. W.; Keksis, A. L.; Meade, R. A.; Burns, C. J.; Chadwick, M. B.; Wallstrom, T. C.

    2010-12-01

    where the present results are about 4%-relative higher for neutrons incident on 239Pu and 235U. Additionally, our results illustrate the importance of representing the incident energy dependence of fission product yields over the fast neutron energy range for high-accuracy work, for example the 147Nd from neutron reactions on plutonium. An upgrade to the ENDF library, for ENDF/B-VII.1, based on these and other data, is described in a companion paper to this work.

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

    NASA Astrophysics Data System (ADS)

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

    2015-06-01

    Using dual-fission chambers each loaded with a thick (200 -400 -mg /c m2) actinide target of 235 ,238U or 239Pu and two thin (˜10 -100 -μ g /c m2) reference foils of the same actinide, the cumulative yields of fission products ranging from 92Sr to 147Nd have been measured at En= 8.9 MeV . The 2H(d ,n ) 3He reaction provided the quasimonoenergetic neutron beam. The experimental setup and methods used to determine the fission product yield (FPY) are described, and results for typically eight high-yield fission products are presented. Our FPYs for 235U(n ,f ) , 238U(n ,f ) , and 239Pu(n ,f ) at 8.9 MeV are compared with the existing data below 8 MeV from Glendenin et al. [Phys. Rev. C 24, 2600 (1981), 10.1103/PhysRevC.24.2600], Nagy et al. [Phys. Rev. C 17, 163 (1978), 10.1103/PhysRevC.17.163], Gindler et al. [Phys. Rev. C 27, 2058 (1983), 10.1103/PhysRevC.27.2058], and those of Mac Innes et al. [Nucl. Data Sheets 112, 3135 (2011), 10.1016/j.nds.2011.11.009] and Laurec et al. [Nucl. Data Sheets 111, 2965 (2010), 10.1016/j.nds.2010.11.004] at 14.5 and 14.7 MeV, respectively. This comparison indicates a negative slope for the energy dependence of most fission product yields obtained from 235U and 239Pu , whereas for 238U the slope issue remains unsettled.

  8. Cross-section measurements for 239Pu(n,f) and 6Li(n, α) with a lead slowing-down spectrometer

    NASA Astrophysics Data System (ADS)

    Rochman, D.; Haight, R. C.; O'Donnell, J. M.; Wender, S. A.; Vieira, D. J.; Bond, E. M.; Bredeweg, T. A.; Wilhelmy, J. B.; Granier, T.; Ethvignot, T.; Petit, M.; Danon, Y.; Romano, C.

    2006-08-01

    We present fission cross-section measurements with ˜10 ng of 239Pu performed using the LANSCE Lead Slowing-Down Spectrometer. Results of Li6(n,α) measurements with a sample size of 760 ng of 6Li are also reported. This technical achievement demonstrates the feasibility of measuring neutron-induced fission cross-section on samples with 10 ng of fissile actinides that are available on ultra-small quantities. Furthermore, results on neutron-induced alpha emission show that measurements for astrophysics purposes are feasible with the LSDS.

  9. Report on the effectiveness of flocculation for removal of {sup 239}Pu at concentrations of 1 pCi/L and 0.1 pCi/L. RFP Pond Water Characterization and Treatment (LATO-EG&G-91-022): Task C deliverables: 5.1.2 and 5.2.2

    SciTech Connect

    Triay, I.R.; Bayhurst, G.K.; Mitchell, A.J.; Cisneros, M.R.; Efurd, D.W.; Roensch, F.R.; Rokop, D.J.; Aguilar, R.D.; Attrep, M.; Nuttall, H.E.

    1993-08-01

    The objective of this work is to assess the effectiveness of flocculation for the removal of Pu from Rocky Flats Plant (RFP) pond waters spiked with {sup 239}Pu at the 1.0 and 0.1 pCi/L level. The flocculation treatment procedure is described in detail. Results are presented for treatment studies for the removal of Pu from C-2 pond water spiked with {sup 239}Pu and from distilled water spiked with {sup 239}Pu.

  10. A study of 239Pu production rate in a water cooled natural uranium blanket mock-up of a fusion-fission hybrid reactor

    NASA Astrophysics Data System (ADS)

    Feng, Song; Liu, Rong; Lu, Xinxin; Yang, Yiwei; Xu, Kun; Wang, Mei; Zhu, Tonghua; Jiang, Li; Qin, Jianguo; Jiang, Jieqiong; Han, Zijie; Lai, Caifeng; Wen, Zhongwei

    2016-03-01

    The 239Pu production rate is important data in neutronics design for a natural uranium blanket of a fusion-fission hybrid reactor, and the accuracy and reliability should be validated by integral experiments. The distribution of 239Pu production rates in a subcritical natural uranium blanket mock-up was obtained for the first time with a D-T neutron generator by using an activation technique. Natural uranium foils were placed in different spatial locations of the mock-up, the counts of 277.6 keV γ-rays emitted from 239Np generated by 238U capture reaction were measured by an HPGe γ spectrometer, and the self-absorption of natural uranium foils was corrected. The experiment was analyzed using the Super Monte Carlo neutron transport code SuperMC2.0 with recent nuclear data of 238U from the ENDF/B-VII.0, ENDF/B-VII.1, JENDL-4.0u2, JEFF-3.2 and CENDL-3.1 libraries. Calculation results with the JEFF-3.2 library agree with the experimental ones best, and they agree within the experimental uncertainty in general with the average ratios of calculation results to experimental results (C/E) in the range of 0.93 to 1.01.

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

    DOE PAGES

    Neudecker, Denise; Taddeucci, Terry Nicholas; Haight, Robert Cameron; Lee, Hye Young; White, Morgan Curtis; Rising, Michael Evans

    2016-01-06

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

  12. Relative radiosensitivity of bone tumor induction among beagles as a function of age at injection of {sup 239}Pu or {sup 226}Ra

    SciTech Connect

    Lloyd, R.D.; Taylor, G.N.; Jee, W.S.S.; Miller, S.C.

    1999-01-01

    A comparison was made of the response to induction of skeletal malignancy from exposure of beagles to monomeric {sup 239}Pu or to {sup 226}Ra as juveniles (3 mo of age), young adults (1.5 y of age), or mature adults (5 y of age). This indicated that of these age groups, animals injected as young adults are most sensitive per Gy of average skeletal dose evaluated at 1 y before death. Dogs exposed either as juveniles or as mature adults appeared to be less sensitive. Relative radiosensitivities (RRS) of juvenile and mature beagles ranged between about 0.3 and 0.7 that of dogs injected as young adults. Mean values of RRS for both radionuclides were about 0.5, but RRS values derived from dogs given monomeric {sup 239}Pu appeared to be most reliable and were 0.27 {+-} 0.09 for dogs injected as juveniles and 0.41 {+-} 0.13 for animals exposed as mature adults.

  13. Measurement/Evaluation Techniques and Nuclear Data Associated with Fission of 239Pu by Fission Spectrum Neutrons

    SciTech Connect

    Baisden, P; Bauge, E; Ferguson, J; Gilliam, D; Granier, T; Jeanloz, R; McMillan, C; Robertson, D; Thompson, P; Verdon, C; Wilkerson, C; Young, P

    2010-03-16

    This Panel was chartered to review and assess new evaluations of work on fission product data, as well as the evaluation process used by the two U.S. nuclear weapons physics laboratories. The work focuses on fission product yields resulting from fission spectrum neutrons incident on plutonium, and includes data from measurements that had not been previously published as well as new or revised fission product cumulative yield data, and related quantities such as Q values and R values. This report documents the Panel's assessment of the work presented by Los Alamos National Laboratory (LANL) and Lawrence Livermore National Laboratory (LLNL). Based on the work presented we have seven key observations: (1) Experiments conducted in the 1970s at LANL, some of which were performed in association with a larger, NIST-led, program, have recently been documented. A preliminary assessment of this work, which will be referred to in this document as ILRR-LANL, shows it to be technically sound. (2) LLNL has done a thorough, unbiased review and evaluation of the available literature and is in the process of incorporating the previously unavailable LANL data into its evaluation of key fission product yields. The results of the LLNL effort, which includes a preliminary evaluation of the ILRR-LANL data, have been documented. (3) LANL has also conducted an evaluation of fission product yields for fission spectrum neutrons on plutonium including a meta-analysis of benchmark data as part of a planned upgrade to the ENDF/B compilation. We found that the approach of using meta-analysis provides valuable additional insight for evaluating the sparse data sets involved in this assessment. (4) Both laboratories have provided convincing evidence for energy dependence in the fission product yield of {sup 147}Nd produced from the bombardment of {sup 239}Pu with fission spectrum neutrons over an incident neutron energy range of 0.2 to 1.9 MeV. (5) Consistent, complete, and explicit treatment of

  14. A comparison of the natural survival of beagle dogs injected intravenously with low levels of 239Pu, 226Ra, 228Ra, 228Th, or 90Sr.

    PubMed

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

    1991-06-01

    The natural survival, relative to properly chosen controls, of 26 beagle dogs injected once intravenously with an average of 0.58 +/- 0.04 kBq 239Pu/kg, 23 dogs injected with 2.31 +/- 0.43 kBq 226Ra/kg, 13 dogs injected with 1.84 +/- 0.26 kBq 228Ra/kg, 12 dogs injected with 0.56 +/- 0.030 kBq 228Th/kg, and 12 dogs injected with 21.13 +/- 1.74 kBq 90Sr/kg was evaluated statistically. The amounts of these radionuclides are related directly to the estimated maximum permissible body burdens for humans suggested in ICRP II (1959). They constitute a level of exposure that initially was assumed to cause no deleterious effects in dogs. This study had two objectives: (1) identification of homogeneous control groups against which to evaluate the survival of the irradiated groups and (2) comparison of the survival characteristics and estimation of mortality or hazard rate ratios for control dogs vs dogs injected with the baseline dosages given above. It was shown, by goodness-of-fit plots, that the Cox proportional hazards model was an appropriate method of analysis. Therefore, covariates that possibly could influence survival were tested for significance. Only the effects of grand mal seizure, which is caused in epileptic dogs by an external stimulus and can be fatal if untreated, were significant (P less than 0.0001). Consequently, in the final model, death from grand mal seizure was considered as accidental. After censoring the dogs dying from grand mal seizure, it was established that the data for the control groups from previous and contemporary experiments could be pooled. The change in hazard rates relative to controls resulting from exposure to the baseline radionuclide level was modest, 1.6 times for 239Pu (P = 0.033), 1.0(4) for 226Ra (P = 0.86), 1.9 for 228Ra (P = 0.035), 2.5 for 228Th (P less than 0.001), and 0.52 for 90Sr (P = 0.041). Bone tumor induction was clearly elevated in dogs injected with 239Pu and 228Th. When the effect of these bone tumors on survival

  15. Minimum Critical Values Study

    SciTech Connect

    Fox, P.B.

    2005-07-11

    This report provides minimum critical values for various 30-cm water-reflected uranium and plutonium oxide and nitrate aqueous mixtures as calculated by the SCALE CSAS1X sequence using the 238-group ENDF/B-V neutron cross-section library. The minimum values were determined through parametric searches in one-dimensional geometry. The calculations have been performed to obtain the minimum values: critical volume and mass for spheres, critical radius for cylinders, critical thickness for slabs, and minimum critical concentration (infinite geometry) for the following homogeneous mixtures: (1) UO{sub 2}-H{sub 2}O for 3, 4, 5, 20, and 100 wt % {sup 235}U; (2) UNH for 3, 4, 5, 20, and 100 wt % {sup 235}U; (3) PuO{sub 2}-H{sub 2}O for 100/0/0, 95/5/0, 90/5/5, 80/10/10, and 71/17/11/1 wt % of {sup 239}Pu/{sup 240}Pu/{sup 241}Pu(/{sup 242}Pu); and (4) PuNH for 100/0/0, 95/5/0, 90/5/5, 80/10/10, and 71/17/11/1 wt % of {sup 239}Pu/{sup 240}Pu/{sup 241}Pu(/{sup 242}Pu). All bounding surfaces were fully reflected by 30 cm of H{sub 2}O.

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

    SciTech Connect

    Cooper, L. W.; Kelley, J. M.; Bond, L. A.; Orlandini, K. A.; Grebmeier, J. M.; Environmental Research; ORNL; PNNL; Univ. of Tennessee

    2000-01-01

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

  17. Comparative studies on the lysosomal association of monomeric /sup 239/Pu and /sup 241/Am in rat and Chinese hamster liver: analysis with sucrose, metrizamide, and Percoll density gradients of subcellular binding as dependent on time

    SciTech Connect

    Suetterlin, U.; Thies, W.G.; Haffner, H.; Seidel, A.

    1984-05-01

    The binding of /sup 239/Pu and /sup 241/Am in the livers of Chinese hamsters and rats was analyzed by centrifugation of a mitochondrial-lysosomal fraction in sucrose, metrizamide, and Percoll density gradients at intervals between 4 and 70 days after nuclide injection. The behavior of /sup 239/Pu and /sup 241/Am during the centrifugation experiments was very similar. In contrast to the results for rats, the median densities of the nuclide fraction liberated by addition of Triton X-100, and the nuclide profiles do not respond typically to Triton WR 1339 treatment of the animals. It was concluded from the results that the major fraction of /sup 239/Pu and /sup 241/Am remained bound to typical lysosomes in rat liver, whereas those in hamster liver may be transformed into telolysosomes. Possibly, a vesicular biliary transport system for certain heavy metals, for which evidence exists in rat liver, does not occur in Chinese hamster liver.

  18. Fission track analysis of plutonium in small specimens of biological material: Ultrasensitive analysis for sup 239 Pu in 50 urine samples from the Marshall Islands furnished by Brookhaven National Laboratory

    SciTech Connect

    Wrenn, M.E.; Singh, N.P.; Xue, Ying-Hua.

    1990-11-20

    A neutron induced fission track method was successfully developed for assaying {sup 239}Pu in human urine. The technique involves means to remove potentially interfering natural uranium from the sample and reagents. The method was applied to 50 urine samples including an unknown number of spikes and controls from the Marshall Islands. 49 samples were successfully analyzed. The mean activity for the 47 samples which were not positive for {sup 239}Pu did not differ significantly from the mean for our control samples, which consisted of urines collected from six young adult Utah residents. 2 figs., 12 tabs.

  19. [Accumulation of 238, 239 + 240Pu and 241Am in Boar Organs and Tissues on the Territory of the Belarusian Part of the ChNPP Exclusion Zone].

    PubMed

    Bondar, Yu I; Zabrotski, V N; Sadchikov, V I; Kalinin, V N

    2015-01-01

    The paper is devoted to determination of α-emitting radionuclides of 238, 239 + 240Pu and 241Am in liver, lungs, muscular and bone tissues of the boars on the territory of the Belarusian part of the ChNPP exclusion zone. It is shown that the content of Pu and Am isotopes in boar organs and tissues decreases in the following order: liver > bone tissues > lungs ≥ muscular tissues. The results received allow evaluation of penetration of 238, 239 + 240Pu and 241Am through the biological chain "soil-ration-organs and tissues". It is calculated that 1.7% of a boar's ration falls on the soil getting into the stomach with food. Translocation and accumulation coefficients characterizing the transfer of radionuclides through the chain "soil-vegetation-organs and tissues" were calculated. The conclusion about accumulation of Pu in the boar's body is made. PMID:26964350

  20. [Accumulation of 238, 239 + 240Pu and 241Am in Boar Organs and Tissues on the Territory of the Belarusian Part of the ChNPP Exclusion Zone].

    PubMed

    Bondar, Yu I; Zabrotski, V N; Sadchikov, V I; Kalinin, V N

    2015-01-01

    The paper is devoted to determination of α-emitting radionuclides of 238, 239 + 240Pu and 241Am in liver, lungs, muscular and bone tissues of the boars on the territory of the Belarusian part of the ChNPP exclusion zone. It is shown that the content of Pu and Am isotopes in boar organs and tissues decreases in the following order: liver > bone tissues > lungs ≥ muscular tissues. The results received allow evaluation of penetration of 238, 239 + 240Pu and 241Am through the biological chain "soil-ration-organs and tissues". It is calculated that 1.7% of a boar's ration falls on the soil getting into the stomach with food. Translocation and accumulation coefficients characterizing the transfer of radionuclides through the chain "soil-vegetation-organs and tissues" were calculated. The conclusion about accumulation of Pu in the boar's body is made.

  1. 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.

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

    PubMed

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

    2010-09-01

    The studies of (137)Cs and (239+240)Pu distributions in surface seawater at South China Sea within the Exclusive Economic Zone (EEZ) of Peninsular Malaysia were carried out in June 2008. The analysis results will serve as additional information to the expanded baseline data for Malaysia's marine environment. Thirty locations from extended study area were identified in the EEZ from which large volumes of surface seawater samples were collected. Different co-precipitation techniques were employed to concentrate cesium and plutonium separately. A known amount of (134)Cs and (242)Pu tracers were used as yield determinant. The precipitate slurry was collected and oven dried at 60(o)C for 1-2 days. Cesium precipitate was fine-ground and counted using gamma-ray spectrometry system at 661.62keV, while plutonium was separated from other radionuclides using anion exchange, electrodeposited and counted using alpha spectrometry. The activity concentrations of (137)Cs and (239+240)Pu were in the range of 3.40-5.89Bq/m(3) and 2.3-7.9mBq/m(3), respectively. The (239+240)Pu/(137)Cs ratios indicate that there are no new inputs of these radionuclides into the area. PMID:20430636

  3. Examining (239+240)Pu, (210)Pb and historical events to determine carbon, nitrogen and phosphorus burial in mangrove sediments of Moreton Bay, Australia.

    PubMed

    Sanders, Christian J; Santos, Isaac R; Maher, Damien T; Breithaupt, Joshua L; Smoak, Joseph M; Ketterer, Michael; Call, Mitchell; Sanders, Luciana; Eyre, Bradley D

    2016-01-01

    Two sediment cores were collected in a mangrove forest to construct geochronologies for the previous century using natural and anthropogenic radionuclide tracers. Both sediment cores were dated using (239+240)Pu global fallout signatures as well as (210)Pb, applying both the Constant Initial Concentration (CIC) and the Constant Rate of Supply (CRS) models. The (239+240)Pu and CIC model are interpreted as having comparable sediment accretion rates (SAR) below an apparent mixed region in the upper ∼5 to 10 cm. In contrast, the CRS dating method shows high sediment accretion rates in the uppermost intervals, which is substantially reduced over the lower intervals of the 100-year record. A local anthropogenic nutrient signal is reflected in the high total phosphorus (TP) concentration in younger sediments. The carbon/nitrogen molar ratios and δ(15)N values further support a local anthropogenic nutrient enrichment signal. The origin of these signals is likely the treated sewage discharge to Moreton Bay which began in the early 1970s. While the (239+240)Pu and CIC models can only produce rates averaged over the intervals of interest within the profile, the (210)Pb CRS model identifies elevated rates of sediment accretion, organic carbon (OC), nitrogen (N), and TP burial from 2000 to 2013. From 1920 to 2000, the three dating methods provide similar OC, N and TP burial rates, ∼150, 10 and 2 g m(-2) year(-1), respectively, which are comparable to global averages.

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

    PubMed

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

    2010-09-01

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

  5. Estimating Reaction Cross Sections from Measured (Gamma)-Ray Yields: The 238U(n,2n) and 239Pu(n,2n) Cross Sections

    SciTech Connect

    Younes, W

    2002-11-18

    A procedure is presented to deduce the reaction-channel cross section from measured partial {gamma}-ray cross sections. In its simplest form, the procedure consists in adding complementary measured and calculated contributions to produce the channel cross section. A matrix formalism is introduced to provide a rigorous framework for this approach. The formalism is illustrated using a fictitious product nucleus with a simple level scheme, and a general algorithm is presented to process any level scheme. In order to circumvent the cumbersome algebra that can arise in the matrix formalism, a more intuitive graphical procedure is introduced to obtain the same reaction cross-section estimate. The features and limitations of the method are discussed, and the technique is applied to extract the {sup 235}U (n,2n) and {sup 239}Pu(n,2n) cross sections from experimental partial {gamma}-ray cross sections, coupled with (enhanced) Hauser-Feshbach calculations.

  6. The influence of internally deposited alpha ({sup 239}Pu) or beta-gamma ({sup 144}Ce) emitting radionuclides on the sensitivity of Chinese hamster bone marrow cells to {sup 60}CO induced chromosome aberrations

    SciTech Connect

    Brooks, A.L.; McDonald, K.E.; Kitchin, R.M.

    1994-12-31

    The current study was designed to determine if protracted low-dose-rate exposures from either high-({sup 239}Pu) or low-({sup 144}Ce) LET radiation from internally deposited radioactive materials changes the frequency of chromosome aberrations induced by acute {sup 60}Co exposure. THe potential for interaction was evaluated 30 days after injection with either 0 or 0.85 kBq {sup 144}Ce g{sup -1} body weight or 0.0 or 2.2 Bq of {sup 239}Pu g{sup -1}. Injection with {sup 239}Pu or {sup 144}Ce resulted in few aberrations in bone marrow cells 30 days after injection. The presence of internally deposited {sup 239}Pu or {sup 144}Ce did not significantly alter the total frequency of {sup 60}Co induced aberrations. However, the frequency of {sup 60}Co induced chromatid exchanges was significantly greater (P=0.03) in bone marrow cells of animals with {sup 144}Ce body burdens (0.14{+-}0.03 chromatid exchanges/cell). Such data illustrates that changes in cellular responsiveness may be dependent on the LET of the isotope, the dose rate of the primary dose and the type of damage being evaluated.

  7. Radionuclide concentrations in soils and vegetation at Low-Level Radioactive Waste Disposal Area G during the 1998 growing season (with a cumulative summary of {sup 3}H and {sup 239}Pu over time)

    SciTech Connect

    P. R. Fresquez; M. H. Ebinger; R. J. Wechsler; L. Naranjo, Jr.

    1999-11-01

    Soils and unwashed overstory and understory vegetation were collected at eight locations within and around Area G, a disposal facility for low-level, radioactive solid waste at Los Alamos National Laboratory. The samples were analyzed for {sup 3}H, {sup 238}Pu, {sup 239}Pu, {sup 90}Sr, {sup 241}Am, {sup 137}Cs, {sup tot}U. Most of the radionuclide concentrations in soils and vegetation were within the upper 95% level of background concentrations except for {sup 3}H and {sup 239}Pu. Tritium concentrations in vegetation from most sites were greater than background concentrations of about 2 pCi mL{sup {minus}1}. The concentrations of {sup 239}Pu in soils and understory vegetation were largest in samples collected several meters north of the transuranic waste pad area and were consistent with previous results. Based on {sup 3}H and {sup 239}Pu data through 1998, it was shown that concentrations were (1) significantly greater than background concentrations (p < 0.05) in soils and vegetation collected from most locations at Area G, and (2) there was no systematic increase or decrease in concentrations with time apparent in the data.

  8. Parity splitting and E1/E2 branching in the alternating parity band of {sup 240}Pu from two-center octupole wave functions using supersymmetric quantum mechanics

    SciTech Connect

    Jolos, R. V.; Brentano, P. von

    2011-08-15

    An interpretation is suggested of the recently published experimental data on the alternating parity bands in {sup 240}Pu. The interpretation is based on the assumption that the main role in the description of the properties of the alternating parity bands plays the octupole mode which preserves the axial symmetry. The mathematical technique of the supersymmetric quantum mechanics is used for the realization of the model with the two-center octupole wave functions. A good description of the parity splitting and of the ratio of the dipole and quadrupole transitional moments is obtained for the first two bands.

  9. Selectivity of 90Sr urine bioassay technique over 241Am, 238/239PU, 210PO, 137CS and 60CO.

    PubMed

    Sadi, Baki B; Li, Chunsheng; Bahraini, Negar; Lai, Edward P C; Kramer, Gary H

    2010-09-01

    The selectivity of a rapid (90)Sr bioassay technique over (241)Am, (238/239)Pu, (210)Po, (137)Cs and (60)Co has been investigated. Similar to (90)Sr, these radionuclides are likely to be used in radiological dispersive devices. The purpose of this study was to demonstrate the degree to which the (90)Sr bioassay technique is free from interference by these radionuclides if present in a urine matrix. The interfering radionuclides were removed (from (90)Sr) by their retention on an anion exchange column. While, recovery of the target radionuclide ((90)Sr) was found to be >or= 90 %, contributions from (241)Am, (242)Pu and (208)Po were found to be

  10. Determination of Fission Product Yields of 235U, 238U and 239Pu for Neutron Energies from 0.5 to 14.8 MeV

    NASA Astrophysics Data System (ADS)

    Gooden, Matthew; Arnold, Charles; Becker, John; Bhatia, Chitra; Bhike, Megha; Fallin, Brent; Fowler, Malcolm; Howell, Calvin; Kelley, John; Stoyer, Mark; Tonchev, Anton; Tornow, Werner; Viera, David; Wilhelmy, Jerry

    2013-10-01

    A joint TUNL-LANL-LLNL collaboration has been formed to study the issue of possible energy dependences for fission product isotopes. Work has been carried out at the TUNL 10 MV Tandem accelerator which produces nearly mono-energetic neutrons via either 2H(d,n)3He,3H(d,n)4He, or 3H(p,n)3He reactions. Three dual fission ionization chambers dedicated to 235U, 238U and 239Pu thick target foils and thin monitor foils respectively, were exposed to the neutron beams. After irradiation, thick target foils were gamma counted over a period of 1-2 months and characteristic gamma rays from fission products were recorded using HPGe detectors at TUNL's low background counting area. Using the dual fission chambers fission product yields relative to total number of fissions were determined at a high precision of 2-3% as well as absolute fission product yields at a lower precision of 5-6%. Results will be presented for a number of fission product isotopes at 1.38, 4.6 and 14.8 MeV as well as preliminary results at 9 MeV.

  11. Energy Dependence of Neutron-Induced Fission Product Yields of 235U, 238U and 239Pu Between 0.5 and 14.8 MeV

    NASA Astrophysics Data System (ADS)

    Gooden, Matthew; Tornow, Werner; Tonchev, Anton; Vieira, Dave; Wilhelmy, Jerry; Arnold, Charles; Fowler, Malcolm; Stoyer, Mark

    2014-09-01

    Under a joint collaboration between TUNL-LANL-LLNL, a set of absolute fission product yield measurements have been performed. The energy dependence of a number of cumulative fission products between 0.5 and 14.8 MeV have been measured using quasi-monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combination of activation utilizing specially designed dual-fission chambers and γ-ray counting. The dual-fission chambers are back-to-back ionization chambers encasing a target with thin deposits of the same target isotope in each chamber. This method allows for the direct measurement of the fission rate in the activation target with no reference to the fission cross-section, reducing uncertainties. γ-ray counting was performed on well-shield HPGe detectors over a period of 2 months per activation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 4.6 and 14.8 MeV.

  12. Determination of Fission Product Yields of 235U, 238U and 239Pu for Neutron Energies from 0.5 to 14.8 MeV

    NASA Astrophysics Data System (ADS)

    Gooden, Matthew; Arnold, Charles; Becker, John; Bhatia, Chitra; Bhike, Megha; Fowler, Malcolm; Howell, Calvin; Kelley, John; Stoyer, Mark; Tonchev, Anton; Tornow, Werner; Vieira, Dave; Wilhelmy, Jerry

    2014-03-01

    A joint TUNL-LANL-LLNL collaboration has been formed to study the issue of possible energy dependences for certain fission product isotopes. Work has been carried out at the TUNL 10 MV Tandem accelerator which produces nearly mono-energetic neutrons via either 2H(d,n)3He,3H(d,n)4He,or3H(p,n)3He reactions. Three dual fission ionization chambers dedicated to 235U, 238U and 239Pu thick target foils and thin monitor foils respectively, were exposed to the neutron beams. After irradiation, thick target foils were gamma counted over a period of 1-2 months and characteristic gamma rays from fission products were recorded using HPGe detectors at TUNL's low background counting area. Using the dual fission chambers, relative fission product yield were determined at a high precision of 2-3 % as well as absolute fission product yields at a lower precision of 5-6 %. Preliminary results will be presented for a number of fission product isotopes over the incident neutron energy range of 0.5 to 14.8 MeV.

  13. Microdistribution and long-term retention of 239Pu (NO3)4 in the respiratory tracts of an acutely exposed plutonium worker and experimental beagle dogs.

    PubMed

    Nielsen, Christopher E; Wilson, Dulaney A; Brooks, Antone L; McCord, Stacey L; Dagle, Gerald E; James, Anthony C; Tolmachev, Sergei Y; Thrall, Brian D; Morgan, William F

    2012-11-01

    The long-term retention of inhaled soluble forms of plutonium raises concerns as to the potential health effects in persons working in nuclear energy or the nuclear weapons program. The distributions of long-term retained inhaled plutonium-nitrate [(239)Pu (NO(3))(4)] deposited in the lungs of an accidentally exposed nuclear worker (Human Case 0269) and in the lungs of experimentally exposed beagle dogs with varying initial lung depositions were determined via autoradiographs of selected histologic lung, lymph node, trachea, and nasal turbinate tissue sections. These studies showed that both the human and dogs had a nonuniform distribution of plutonium throughout the lung tissue. Fibrotic scar tissue effectively encapsulated a portion of the plutonium and prevented its clearance from the body or translocation to other tissues and diminished dose to organ parenchyma. Alpha radiation activity from deposited plutonium in Human Case 0269 was observed primarily along the subpleural regions while no alpha activity was seen in the tracheobronchial lymph nodes of this individual. However, relatively high activity levels in the tracheobronchial lymph nodes of the beagles indicated the lymphatic system was effective in clearing deposited plutonium from the lung tissues. In both the human case and beagle dogs, the appearance of retained plutonium within the respiratory tract was inconsistent with current biokinetic models of clearance for soluble forms of plutonium. Bound plutonium can have a marked effect on the dose to the lungs and subsequent radiation exposure has the potential to increase cancer risk. PMID:22962267

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

    SciTech Connect

    Nielsen, Christopher E.; Wilson, Dulaney A.; Brooks, Antone L.; McCord, Stacey; Dagle, Gerald E.; James, Anthony C.; Tolmachev, Sergei Y.; Thrall, Brian D.; Morgan, William F.

    2012-11-01

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

  15. Inhaled /sup 239/PuO/sub 2/ and/or total-body gamma radiation: Early mortality and morbidity in rats and dogs

    SciTech Connect

    Filipy, R.E.; Decker, J.R.; Lai, Y.L.; Lauhala, K.E.; Buschbom, R.L.; Hiastala, M.P.; McGee, D.R.; Park, J.F.; Kuffel, E.G.; Ragan, H.A.; Cannon, W.C.; Yaniv, S.S.; Scott, B.R.

    1988-08-01

    Rats and beagle dogs were given doses of /sup 60/Co gamma radiation and/or body burdens of /sup 239/PuO/sub 2/ within lethal ranges in an experiment to determine and compare morbidity and mortality responses of both species within 1 year after exposure. Radiation-induced morbidity was assessed by measuring changes in body weights, hematologic parameters, and pulmonary-function parameters. Gamma radiation caused transient morbidity, reflected by immediately depressed blood cell concentrations and by long-term loss of body weight and diminished pulmonary function in animals of both species that survived the acute gamma radiation syndrome. Inhaled plutonium caused a loss of body weight and diminished pulmonary function in both species, but its only effect on blood cell concentrations was lymphocytopenia in dogs. Combined gamma irradiation and plutonium lung burdens were synergistic, in that animals receiving both radiation insults had higher morbidity and mortality rates than would be predicted based on the effect of either kind of radiation alone. Plutonium lung burdens enhanced the effect of gamma radiation in rats within the first 30 days of exposure, and gamma radiation enhanced the long-term effect of plutonium lung burdens in both species. Rats were less sensitive to both kinds of radiation, whether administered alone or in combination. 71 refs., 105 figs., 48 tabs.

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

    SciTech Connect

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

    2011-09-12

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

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

    NASA Astrophysics Data System (ADS)

    Pamfiloff, Eugene

    2006-10-01

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

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

    NASA Astrophysics Data System (ADS)

    Pamfiloff, Eugene

    2006-10-01

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

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

    NASA Astrophysics Data System (ADS)

    Pamfiloff, Eugene

    2006-11-01

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

  20. Microdistribution and long-term retention of 239Pu (NO3)4 in the respiratory tracts of an acutely exposed plutonium worker and experimental beagle dogs.

    PubMed

    Nielsen, Christopher E; Wilson, Dulaney A; Brooks, Antone L; McCord, Stacey L; Dagle, Gerald E; James, Anthony C; Tolmachev, Sergei Y; Thrall, Brian D; Morgan, William F

    2012-11-01

    The long-term retention of inhaled soluble forms of plutonium raises concerns as to the potential health effects in persons working in nuclear energy or the nuclear weapons program. The distributions of long-term retained inhaled plutonium-nitrate [(239)Pu (NO(3))(4)] deposited in the lungs of an accidentally exposed nuclear worker (Human Case 0269) and in the lungs of experimentally exposed beagle dogs with varying initial lung depositions were determined via autoradiographs of selected histologic lung, lymph node, trachea, and nasal turbinate tissue sections. These studies showed that both the human and dogs had a nonuniform distribution of plutonium throughout the lung tissue. Fibrotic scar tissue effectively encapsulated a portion of the plutonium and prevented its clearance from the body or translocation to other tissues and diminished dose to organ parenchyma. Alpha radiation activity from deposited plutonium in Human Case 0269 was observed primarily along the subpleural regions while no alpha activity was seen in the tracheobronchial lymph nodes of this individual. However, relatively high activity levels in the tracheobronchial lymph nodes of the beagles indicated the lymphatic system was effective in clearing deposited plutonium from the lung tissues. In both the human case and beagle dogs, the appearance of retained plutonium within the respiratory tract was inconsistent with current biokinetic models of clearance for soluble forms of plutonium. Bound plutonium can have a marked effect on the dose to the lungs and subsequent radiation exposure has the potential to increase cancer risk.

  1. 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.

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

    PubMed

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

    2013-09-01

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

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

    PubMed

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

    2013-09-01

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

  4. Quantification of Uncertainties due to 235,238U, 239,240,241Pu and Fission Products Nuclear Data Uncertainties for a PWR Fuel Assembly

    NASA Astrophysics Data System (ADS)

    da Cruz, D. F.; Rochman, D.; Koning, A. J.

    2014-04-01

    Uncertainty analysis on reactivity and discharged inventory for a typical PWR fuel element as a result of uncertainties in 235,238U, 239,240,241Pu, and fission products nuclear data was performed. The Total Monte-Carlo (TMC) method was applied using the deterministic transport code DRAGON. The nuclear data used in this study is from the JEFF-3.1 evaluations, with the exception of the nuclear data files for U, Pu and fission products isotopes, which are taken from the nuclear data library TENDL-2012. Results show that the calculated total uncertainty in keff (as result of uncertainties in nuclear data of the considered isotopes) is virtually independent on fuel burnp and amounts to 700 pcm. The uncertainties in inventory of the discharged fuel is dependent on the element considered and lies in the range 1-15% for most fission products, and is below 5% for the most important actinides.

  5. Advanced Monte Carlo modeling of prompt fission neutrons for thermal and fast neutron-induced fission reactions on {sup 239}Pu

    SciTech Connect

    Talou, P.; Kawano, T.; Becker, B.; Danon, Y.; Chadwick, M. B.

    2011-06-15

    Prompt fission neutrons following the thermal and 0.5 MeV neutron-induced fission reaction of {sup 239}Pu are calculated using a Monte Carlo approach to the evaporation of the excited fission fragments. Exclusive data such as the multiplicity distribution P({nu}), the average multiplicity as a function of fragment mass {nu}-bar(A), and many others are inferred in addition to the most used average prompt fission neutron spectrum {chi}(E{sub in},E{sub out}), as well as average neutron multiplicity {nu}-bar. Experimental information on these more exclusive data help constrain the Monte Carlo model parameters. The calculated average total neutron multiplicity is {nu}-bar{sub c}=2.871 in very close agreement with the evaluated value {nu}-bar{sub e}=2.8725 present in the ENDF/B-VII.0 library. The neutron multiplicity distribution P({nu}) is in very good agreement with the evaluation by Holden and Zucker. The calculated average spectrum differs in shape from the ENDF/B-VII.0 spectrum, evaluated with the Madland-Nix model. In particular, we predict more neutrons in the low-energy tail of the spectrum (below about 300 keV) than the Madland-Nix calculations, casting some doubts on how much scission neutrons contribute to the shape of the low-energy tail of the spectrum. The spectrum high-energy tail is very sensitive to the total kinetic energy distribution of the fragments as well as to the total excitation energy sharing at scission. Present experimental uncertainties on measured spectra above 6 MeV are too large to distinguish between various theoretical hypotheses. Finally, comparisons of the Monte Carlo results with experimental data on {nu}-bar(A) indicate that more neutrons are emitted from the light fragments than the heavy ones, in agreement with previous works.

  6. Procedures for the use of Lexan and Makrofol SSNTDs in the detection of environmental concentrations of {sup 235}U and {sup 239}Pu

    SciTech Connect

    Henderson, C.L.

    1993-03-01

    Solid State Nuclear Track Detectors are used to study a variety of atomic particles. Polycarbonate SSNTD is used to study environmental concentrations of {sup 235}U and {sup 239}Pu in human urine and feces through fission track analysis. The samples of interest are deposited upon a Lexan slide, covered with a piece of Makrofol and exposed to a neutron fluence of 1.1 X 10{sup 17}. The fissile isotopes in the sample fission and the resulting fission fragments pass through either the surface of the Lexan or the surface of the Makrofol. The positive Coulombic attraction of the ionized fission fragments causes the electrons of the polycarbonate lattice to move towards the path of these particles, resulting in the breakage of chemical bonds in the lattice. The detector is then chemically etched in 6.5 N KOH that preferentially dissolves the damaged polycarbonate left in the path of the fission fragment. The chemically etched fission tracks are permanent records of the path of the fission fragment. The etched fission tracks in Lexan are optically counted using a microscope and the fission tracks in Makrofol are counted using a Spark Chamber. The amount of fissile material in the original sample can be calculated from the number of fission tracks. This paper presents further details of procedures for etching fission tracks in Lexan and Makrofol and for operating a Spark Chamber to count etched fission tracks in Makrofol. The physics of fission track formation in dielectric detectors is also discussed, as well as the physics of the Spark Chamber.

  7. 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.

  8. Analytical method for the determination of Np and Pu in sea water by AMS with respect to the Fukushima accident

    NASA Astrophysics Data System (ADS)

    Hain, K.; Faestermann, T.; Famulok, N.; Fimiani, L.; Gómez-Guzmán, J. M.; Korschinek, G.; Kortmann, F.; Lierse v. Gostomski, Ch.; Ludwig, P.; Shinonaga, T.

    2015-10-01

    A chemical separation procedure for plutonium (Pu) and neptunium (Np) was developed using extraction chromatography, mass spectrometry and radiometric analysis to determine their concentrations and isotopic ratios in sea water. 241Am, which causes isobaric background to 241Pu in mass spectrometric measurements, was successfully separated from the Pu fraction by this method. Water samples which were spiked with 242Pu and 237Np or 239Np, respectively, were used for chemical yield determination. The chemical yields of Pu and Np, which were determined by alpha and gamma spectrometry at the Radiochemie München (RCM), of more than 85% were obtained. The developed method was applied to analyze the concentration of Pu and Np in the certified reference material, IAEA-443, by Accelerator Mass Spectrometry (AMS) at the Maier-Leibnitz-Laboratory (MLL) to check the applicability of the method to sea water samples. The concentrations of 240Pu, 241Pu and 237Np obtained in this study are in agreement with the certified and literature values within the uncertainties. Due to strong isotopic interference of 239Pu with 238U, it was not possible to analyze the concentration of 239Pu. Some modifications of the chemical separation method to suppress the uranium (U) fraction are under consideration. This method can be used for the analysis of Pu and Np in Pacific Ocean water samples collected after the Fukushima accident.

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

    PubMed

    Pommé, S; Paepen, J; Peräjärvi, K; Turunen, J; Pöllänen, R

    2016-03-01

    An electron spectrometry set-up was built at IRMM consisting of a vacuum chamber with a moveable source holder and windowless Peltier-cooled silicon drift detector (SDD). The SDD is well suited for measuring low-energy x rays and electrons emitted from thin radioactive sources with low self-absorption. The attainable energy resolution is better than 0.5keV for electrons of 30keV. It has been used to measure the conversion electron spectra of three plutonium isotopes, i.e. (238)Pu, (239)Pu, (240)Pu, as well as (241)Am (being a decay product of (241)Pu). The obtained mixed x-ray and electron spectra are compared with spectra obtained with a close-geometry set-up using another SDD in STUK and spectra measured with a Si(Li) detector at IRMM. The potential of conversion electron spectrometry for isotopic analysis of mixed plutonium samples is investigated. With respect to the (240)Pu/(239)Pu isotopic ratio, the conversion electron peaks of both isotopes are more clearly separated than their largely overlapping peaks in alpha spectra. PMID:26651177

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

    PubMed

    Pommé, S; Paepen, J; Peräjärvi, K; Turunen, J; Pöllänen, R

    2016-03-01

    An electron spectrometry set-up was built at IRMM consisting of a vacuum chamber with a moveable source holder and windowless Peltier-cooled silicon drift detector (SDD). The SDD is well suited for measuring low-energy x rays and electrons emitted from thin radioactive sources with low self-absorption. The attainable energy resolution is better than 0.5keV for electrons of 30keV. It has been used to measure the conversion electron spectra of three plutonium isotopes, i.e. (238)Pu, (239)Pu, (240)Pu, as well as (241)Am (being a decay product of (241)Pu). The obtained mixed x-ray and electron spectra are compared with spectra obtained with a close-geometry set-up using another SDD in STUK and spectra measured with a Si(Li) detector at IRMM. The potential of conversion electron spectrometry for isotopic analysis of mixed plutonium samples is investigated. With respect to the (240)Pu/(239)Pu isotopic ratio, the conversion electron peaks of both isotopes are more clearly separated than their largely overlapping peaks in alpha spectra.

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

    PubMed

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

    2012-06-01

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

  12. Study on Prompt Fission Neutron Spectra and Associated Covariances for 235U(nth,f) and 239Pu(nth,f)

    NASA Astrophysics Data System (ADS)

    Berge, L.; Litaize, O.; Serot, O.; Jean, C. De Saint; Archier, P.; Peneliau, Y.

    normalization of experimental spectra, and the uncertainty on the energy-dependent neutron detection efficiency. We show the resulting PFNS and associated covariance matrix in the case of thermal neutron-induced fission of 235U and 239Pu.

  13. Determination of total content and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes by ICP-QMS.

    PubMed

    Godoy, Maria Luiza Duarte Pinto; Godoy, José Marcus; Roldão, Luiz Alfredo; Tauhata, Luiz

    2009-08-01

    The aim of this work was to determine the concentrations and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes. An analytical method was developed with a plutonium and uranium separation procedure based on extraction chromatography (using 2mL TEVA and UTEVA columns) and detection with a quadrupole ICP-MS applying an ultra-sonic nebulizer coupled with a membrane desolvation system. Starting from blank swipes, the background equivalent concentration (BEC) was 8fg for (239)Pu and 1ng (238)U. The method was successfully applied to certified reference materials as well as to round robin samples obtained in the framework of the inter-laboratory exercise program, promoted by the Brazilian-Argentine Agency for Accounting and Control of Nuclear Materials (ABACC), together with the US Department of Energy (USDOE). After the introduction of an additional ion-exchange separation step, the methodology was applied to the IAEA-384 sediment reference sample with precise and accurate total plutonium and uranium, (240)Pu/(239)Pu, (241)Pu/(239)Pu, (234)U/(238)U and (235)U/(238)U atomic ratio results. PMID:19500890

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

    PubMed

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

    2016-03-01

    In order to assess how environmental factors are affecting the distribution and migration of radioiodine and plutonium that were emitted from the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, we quantified iodine and (239,240)Pu concentration changes in soil samples with different land uses (urban, paddy, deciduous forest and coniferous forest), as well as iodine speciation in surface water and rainwater. Sampling locations were 53-63 km northwest of the FDNPP within a 75-km radius, in close proximity of each other. A ranking of the land uses by their surface soil (<4 cm) stable (127)I concentrations was coniferous forest > deciduous forest > urban > paddy, and (239,240)Pu concentrations ranked as deciduous forest > coniferous forest > paddy ≥ urban. Both were quite distinct from that of (134)Cs and (137)Cs: urban > coniferous forest > deciduous forest > paddy, indicating differences in their sources, deposition phases, and biogeochemical behavior in these soil systems. Although stable (127)I might not have fully equilibrated with Fukushima-derived (129)I, it likely still works as a proxy for the long-term fate of (129)I. Surficial soil (127)I content was well correlated to soil organic matter (SOM) content, regardless of land use type, suggesting that SOM might be an important factor affecting iodine biogeochemistry. Other soil chemical properties, such as Eh and pH, had strong correlations to soil (127)I content, but only within a given land use (e.g., within urban soils). Organic carbon (OC) concentrations and Eh were positively, and pH was negatively correlated to (127)I concentrations in surface water and rain samples. It is also noticeable that (127)I in the wet deposition was concentrated in both the deciduous and coniferous forest throughfall and stemfall water, respectively, comparing to the bulk rainwater. Further, both forest throughfall and stemflow water consisted exclusively of organo-iodine, suggesting all inorganic iodine in the

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

    PubMed

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

    2016-03-01

    In order to assess how environmental factors are affecting the distribution and migration of radioiodine and plutonium that were emitted from the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, we quantified iodine and (239,240)Pu concentration changes in soil samples with different land uses (urban, paddy, deciduous forest and coniferous forest), as well as iodine speciation in surface water and rainwater. Sampling locations were 53-63 km northwest of the FDNPP within a 75-km radius, in close proximity of each other. A ranking of the land uses by their surface soil (<4 cm) stable (127)I concentrations was coniferous forest > deciduous forest > urban > paddy, and (239,240)Pu concentrations ranked as deciduous forest > coniferous forest > paddy ≥ urban. Both were quite distinct from that of (134)Cs and (137)Cs: urban > coniferous forest > deciduous forest > paddy, indicating differences in their sources, deposition phases, and biogeochemical behavior in these soil systems. Although stable (127)I might not have fully equilibrated with Fukushima-derived (129)I, it likely still works as a proxy for the long-term fate of (129)I. Surficial soil (127)I content was well correlated to soil organic matter (SOM) content, regardless of land use type, suggesting that SOM might be an important factor affecting iodine biogeochemistry. Other soil chemical properties, such as Eh and pH, had strong correlations to soil (127)I content, but only within a given land use (e.g., within urban soils). Organic carbon (OC) concentrations and Eh were positively, and pH was negatively correlated to (127)I concentrations in surface water and rain samples. It is also noticeable that (127)I in the wet deposition was concentrated in both the deciduous and coniferous forest throughfall and stemfall water, respectively, comparing to the bulk rainwater. Further, both forest throughfall and stemflow water consisted exclusively of organo-iodine, suggesting all inorganic iodine in the

  16. Pre-operational radio-environmental studies of Plant Vogtle

    SciTech Connect

    Winn, W.G.; Sigg, R.A.

    1989-05-01

    This baseline study evaluates radioactivity in the environment near Plant Vogtle before initial reactor startup in 1987. These data will distinguish between any future radio-environmental effects from SRS and Plant Vogtle. Alpha, beta, and gamma-spectrometric methods analyzed river, stream, sediment, and soil samples. The study detected manmade radionuclides {sup 3}H, {sup 60}Co, {sup 134}Cs, {sup 137}Cs, {sup 239}Pu, {sup 240}Pu, and {sup 241}Pu. However, all concentration levels are extremely low and are consistent with levels expected from fallout and from SRS operations in its early years. The measurements begun in this study continue to be used to monitor Vogtle post-startup effluents. 12 refs., 6 figs., 7 tabs.

  17. MANTRA: An Integral Reactor Physics Experiment to Infer Actinide Capture Cross-sections from Thorium to Californium with Accelerator Mass Spectrometry

    SciTech Connect

    G. Youinou; C. McGrath; G. Imel; M. Paul; R. Pardo; F. Kondev; M. Salvatores; G. Palmiotti

    2011-08-01

    The principle of the proposed experiment is to irradiate very pure actinide samples in the Advanced Test Reactor at INL and, after a given time, determine the amount of the different transmutation products. The determination of the nuclide densities before and after neutron irradiation will allow inference of effective neutron capture cross-sections. This approach has been used in the past and the novelty of this experiment is that the atom densities of the different transmutation products will be determined using the Accelerator Mass Spectrometry technique at the ATLAS facility located at ANL. It is currently planned to irradiate the following isotopes: 232Th, 235U, 236U, 238U, 237Np, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, 241Am, 243Am, 244Cm and 248Cm.

  18. AN INTEGRAL REACTOR PHYSICS EXPERIMENT TO INFER ACTINIDE CAPTURE CROSS-SECTIONS FROM THORIUM TO CALIFORNIUM WITH ACCELERATOR MASS SPECTROMETRY

    SciTech Connect

    G. Youinou; M. Salvatores; M. Paul; R. Pardo; G. Palmiotti; F. Kondev; G. Imel

    2010-04-01

    The principle of the proposed experiment is to irradiate very pure actinide samples in the Advanced Test Reactor (ATR) at INL and, after a given time, determine the amount of the different transmutation products. The determination of the nuclide densities before and after neutron irradiation will allow inference of effective neutron capture cross-sections. This approach has been used in the past and the novelty of this experiment is that the atom densities of the different transmutation products will be determined using the Accelerator Mass Spectroscopy (AMS) technique at the ATLAS facility located at ANL. It is currently planned to irradiate the following isotopes: 232Th, 235U, 236U, 238U, 237Np, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, 241Am, 243Am and 248Cm.

  19. Prompt fission neutron spectra from fission induced by 1 to 8 MeV neutrons on {sup 235}U and {sup 239}Pu using the double time-of-flight technique

    SciTech Connect

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

    2011-03-15

    Prompt fission neutron spectra from {sup 235}U and {sup 239}Pu were measured for incident neutron energies from 1 to 200 MeV at the Weapons Neutron Research facility (WNR) of the Los Alamos Neutron Science Center, and the experimental data were analyzed with the Los Alamos model for the incident neutron energies of 1-8 MeV. A CEA multiple-foil fission chamber containing deposits of 100 mg {sup 235}U and 90 mg {sup 239}Pu detected fission events. Outgoing neutrons were detected by the Fast Neutron-Induced {gamma}-Ray Observer array of 20 liquid organic scintillators. A double time-of-flight technique was used to deduce the neutron incident energies from the spallation target and the outgoing energies from the fission chamber. These data were used for testing the Los Alamos model, and the total kinetic energy parameters were optimized to obtain a best fit to the data. The prompt fission neutron spectra were also compared with the Evaluated Nuclear Data File (ENDF/B-VII.0). We calculate average energies from both experimental and calculated fission neutron spectra.

  20. Comparative toxicity of /sup 226/Ra, /sup 239/Pu, /sup 241/Am, /sup 249/Cf, and /sup 252/Cf in C57BL/Do black and albino mice

    SciTech Connect

    Taylor, G.N.; Mays, C.W.; Lloyd, R.D.; Gardner, P.A.; TAlbot, L.R.; McFarland, S.S.; Pollard, T.A.; Atherton, D.R.; vanMoorhem, D.; Brammer, D.

    1983-09-01

    Groups of C57BL/Do (black and albino) mice were injected with graded activities of /sup 226/Ra, /sup 239/Pu, /sup 241/Am, /sup 249/Cf, or /sup 252/Cf and were followed throughout life. Bone sarcoma was the principal radiation-induced end point, and the risks associated with average skeletal doses of the four transuranium radionuclides, relative to radium, were determined. The relative biological effectiveness (RBE) was calculated for each emitter by dividing its risk coefficient (bone sarcomas per 10/sup 6/ mouse-rad) by the risk coefficient for /sup 226/Ra. Combined data for males and females in both black and albino mice gave the following values +- SD for the RBE relative to /sup 226/Ra = 1.0: /sup 239/Pu = 15.3 +- 3.9, /sup 241/Am = 4.9 +- 1.4, /sup 249/Cf = 5.0 +- 1.4, and /sup 252/Cf = 2.6 +- 0.8. About 70% of the tumors occurred in the axial skeleton, and the risk coefficient for females averaged about four times higher than for males when all five nuclides were included. The RBE of fission fragment irradiation from /sup 252/Cf for cancer induction, relative to ..cap alpha.. irradiation, for the combined data in all of the animals given /sup 252/Cf and /sup 249/Cf, was 0.02 +- 0.28, in agreement with the calculated theoretical value of 0.03, based on the ratio of summed track lengths in tissue.

  1. Comparative toxicity of /sup 226/Ra, /sup 239/Pu, /sup 241/Am, /sup 249/Cf, and /sup 252/Cf in C57BL/Do black and albino mice

    SciTech Connect

    Taylor, G.N.; Mays, C.W.; Lloyd, R.D.; Gardner, P.A.; Talbot, L.R.; McFarland, S.S.; Pollard, I.A.; Atherton, D.R.; VanMoorhem, D.; Brammer, D.

    1983-09-01

    Groups of C57BL/Do (black and albino) mice were injected with graded activities of /sup 226/Ra, /sup 239/Pu, /sup 241/Am, /sup 249/Cf, or /sup 252/Cf and were followed throughout life. Bone sarcoma was the principal radiation-induced end point, and the risks associated with average skeletal doses of the four transuranium radionuclides, relative to radium, were determined. The relative biological effectiveness (RBE) was calculated for each emitter by dividing its risk coefficient (bone sarcomas per 10(/sup 6/) mouse-rad) by the risk coefficient for /sup 226/Ra. Combined data for males and females in both black and albino mice gave the following values +/- SD for the RBE relative to /sup 226/Ra . 1.0: /sup 239/Pu . 15.3 +/- 3.9, /sup 241/Am . 4.9 +/- 1.4, /sup 249/Cf . 5.0 +/- 1.4, and /sup 252/Cf . 2.6 +/- 0.8. About 70% of the tumors occurred in the axial skeleton, and the risk coefficient for females averaged about four times higher than for males when all five nuclides were included. The RBE of fission fragment irradiation from /sup 252/Cf for cancer induction, relative to alpha irradiation, for the combined data in all of the animals given /sup 252/Cf and /sup 249/Cf, was 0.02 +/- 0.28, in agreement with the calculated theoretical value of 0.03, based on the ratio of summed track lengths in tissue.

  2. [90Sr, 137Cs, 238Pu, 239+240Pu, and 241Am radionuclides in macrophytes within the Krasnensky flood plain: species specificity of concentration and distribution in phytocenosis components].

    PubMed

    Gudkov, D I; Zub, L N; Derevets, V V; Kuz'menko, M I; Nazarov, A B; Kaglian, A E; Savitskiĭ, A L

    2002-01-01

    The analysis of the content of radionuclides 90Sr, 137Cs, 238Pu, 239 + 240Pu and 241Am in water vegetation of flood plain reservoirs has allowed studing features of radionuclide accumulation by various species of macrophytes and revealing bioindicators of radionuclide contamination. Thus species-specificity of radionuclide accumulation can essentially change the contribution of different species to a percentage ratio of the radionuclide content in phytomass of reservoirs in comparison with fund of higher aquatic plants.

  3. Influences of parameter uncertainties within the ICRP-66 respiratory tract model: regional tissue doses for 239PuO2 and 238UO2/238U3O8.

    PubMed

    Farfán, Eduardo B; Huston, Thomas E; Bolch, W Emmett; Vernetson, William G; Bolch, Wesley E

    2003-04-01

    This paper extends an examination of the influence of parameter uncertainties on regional doses to respiratory tract tissues for short-ranged alpha particles using the ICRP-66 respiratory tract model. Previous papers examined uncertainties in the deposition and clearance aspects of the model. The critical parameters examined in this study included target tissue depths, thicknesses, and masses, particularly within the thoracic or lung regions of the respiratory tract. Probability density functions were assigned for the parameters based on published data. The probabilistic computer code LUDUC (Lung Dose Uncertainty Code) was used to assess regional and total lung doses from inhaled aerosols of 239PuO2 and 238UO2/238U3O8. Dose uncertainty was noted to depend on the particle aerodynamic diameter. Additionally, dose distributions were found to follow a lognormal distribution pattern. For 239PuO2 and 238UO2/238U3O8, this study showed that the uncertainty in lung dose increases by factors of approximately 50 and approximately 70 for plutonium and uranium oxides, respectively, over the particle size range from 0.1 to 20 microm. For typical exposure scenarios involving both radionuclides, the ratio of the 95% dose fractile to the 5% dose fractile ranged from approximately 8-10 (corresponding to a geometric standard deviation, or GSD, of about 1.7-2) for particle diameters of 0.1 to 1 microm. This ratio increased to about 370 for plutonium oxide (GSD approximately 4.5) and to about 600 for uranium oxide (GSD approximately 5) as the particle diameter approached 20 microm. However, thoracic tissue doses were quite low at larger particle sizes because most of the deposition occurred in the extrathoracic airways. For 239PuO2, median doses from LUDUC were found be in general agreement with those for Reference Man (via deterministic LUDEP 2.0 calculations) in the particle range of 0.1 to 5 microm. However, median doses to the basal cell nuclei of the bronchial airways (BB

  4. New measurements of (n,γ) and (n,fission) cross sections and capture-to-fission ratios for ^233,235U and ^239Pu using the DANCE 4π BaF2 array

    NASA Astrophysics Data System (ADS)

    Bredeweg, T. A.; Jandel, M.; Fowler, M. M.; Bond, E. M.; Haight, R. C.; Keksis, A. L.; O'Donnell, J. M.; Reifarth, R.; Rundberg, R. S.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Wouters, J. M.; Becker, J. A.; Parker, W. E.; Wu, C. Y.; Baker, J. D.; McGrath, C. A.

    2009-10-01

    Accurate neutron nuclear data are important to many issues in stockpile stewardship, nuclear reactor design and re-certification, nuclear non-proliferation and nuclear forensics. Of particular interest are the production and destruction reactions for all of the major and most of the minor actinides. The competition between capture and fission in many of the actinides presents both an obstacle and an opportunity for large γ detector arrays such as DANCE. Additional instrumentation is required to deconvolve the two contributions to the total observed γ-ray spectrum. However, conducting a simultaneous measurement can simplify background treatment and other sources of systematic uncertainty. An outline of the current experimental program will be presented along with results from neutron capture measurements on ^233,235U and ^239Pu.

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

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

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

  6. New measurements of (n,γ) and (n,fission) cross sections and capture-to-fission ratios for ^233,235U and ^239Pu using the DANCE 4π BaF2 array

    NASA Astrophysics Data System (ADS)

    Bredeweg, T. A.; Jandel, M.; Fowler, M. M.; Bond, E. M.; Haight, R. C.; Keksis, A. L.; O'Donnell, J. M.; Reifarth, R.; Rundberg, R. S.; Slemmons, A. K.; Ullmann, J. L.; Vieira, D. J.; Wouters, J. M.; Becker, J. A.; Wu, C. Y.; Baker, J. D.; McGrath, C. A.

    2010-11-01

    Accurate neutron-induced reaction data are important to many issues in stockpile stewardship, nuclear reactor design and re-certification, nuclear non-proliferation and nuclear forensics. Of particular interest are the production and destruction reactions for all of the major and most of the minor actinides, including both neutron-induced capture and fission. The competition between capture and fission presents both an obstacle and an opportunity for large γ detector arrays such as the DANCE array (Detector for Advanced Neutron Capture Experiments), which cannot clearly differentiate γ-rays resulting from the two exit channels. With the addition of a high efficiency, 4π fission-tagging detector it is possible to deconvolve the two contributions to the total γ-ray spectrum. Using these tools we are able to conduct simultaneous fission/capture measurements which can simplify background treatment and other sources of systematic uncertainty. An outline of the current experimental program will be presented along with results from neutron capture measurements on ^233,235U and ^239Pu.

  7. 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%.

  8. Northern Marshall Islands radiological survey: sampling and analysis summary

    SciTech Connect

    Robison, W.L.; Conrado, C.L.; Eagle, R.J.; Stuart, M.L.

    1981-07-23

    A radiological survey was conducted in the Northern Marshall Islands to document reamining external gamma exposures from nuclear tests conducted at Enewetak and Bikini Atolls. An additional program was later included to obtain terrestrial and marine samples for radiological dose assessment for current or potential atoll inhabitants. This report is the first of a series summarizing the results from the terrestrial and marine surveys. The sample collection and processing procedures and the general survey methodology are discussed; a summary of the collected samples and radionuclide analyses is presented. Over 5400 samples were collected from the 12 atolls and 2 islands and prepared for analysis including 3093 soil, 961 vegetation, 153 animal, 965 fish composite samples (average of 30 fish per sample), 101 clam, 50 lagoon water, 15 cistern water, 17 groundwater, and 85 lagoon sediment samples. A complete breakdown by sample type, atoll, and island is given here. The total number of analyses by radionuclide are 8840 for /sup 241/Am, 6569 for /sup 137/Cs, 4535 for /sup 239 +240/Pu, 4431 for /sup 90/Sr, 1146 for /sup 238/Pu, 269 for /sup 241/Pu, and 114 each for /sup 239/Pu and /sup 240/Pu. A complete breakdown by sample category, atoll or island, and radionuclide is also included.

  9. Plutonium measurements by accelerator mass spectrometry at LLNL

    SciTech Connect

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

    1999-10-26

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

  10. Mechanical environmental transport of actinides and ¹³⁷Cs from an arid radioactive waste disposal site.

    PubMed

    Snow, Mathew S; Clark, Sue B; Morrison, Samuel S; Watrous, Matthew G; Olson, John E; Snyder, Darin C

    2015-10-01

    Aeolian and pluvial processes represent important mechanisms for the movement of actinides and fission products at the Earth's surface. Soil samples taken in the early 1970's near a Department of Energy radioactive waste disposal site (the Subsurface Disposal Area, SDA, located in southeastern Idaho) provide a case study for studying the mechanisms and characteristics of environmental actinide and (137)Cs transport in an arid environment. Multi-component mixing models suggest actinide contamination within 2.5 km of the SDA can be described by mixing between 2 distinct SDA end members and regional nuclear weapons fallout. The absence of chemical fractionation between (241)Am and (239+240)Pu with depth for samples beyond the northeastern corner and lack of (241)Am in-growth over time (due to (241)Pu decay) suggest mechanical transport and mixing of discrete contaminated particles under arid conditions. Occasional samples northeast of the SDA (the direction of the prevailing winds) contain anomalously high concentrations of Pu with (240)Pu/(239)Pu isotopic ratios statistically identical to those in the northeastern corner. Taken together, these data suggest flooding resulted in mechanical transport of contaminated particles into the area between the SDA and a flood containment dike in the northeastern corner, following which subsequent contamination spreading in the northeastern direction resulted from wind transport of discrete particles.

  11. Mechanical environmental transport of actinides and ¹³⁷Cs from an arid radioactive waste disposal site.

    PubMed

    Snow, Mathew S; Clark, Sue B; Morrison, Samuel S; Watrous, Matthew G; Olson, John E; Snyder, Darin C

    2015-10-01

    Aeolian and pluvial processes represent important mechanisms for the movement of actinides and fission products at the Earth's surface. Soil samples taken in the early 1970's near a Department of Energy radioactive waste disposal site (the Subsurface Disposal Area, SDA, located in southeastern Idaho) provide a case study for studying the mechanisms and characteristics of environmental actinide and (137)Cs transport in an arid environment. Multi-component mixing models suggest actinide contamination within 2.5 km of the SDA can be described by mixing between 2 distinct SDA end members and regional nuclear weapons fallout. The absence of chemical fractionation between (241)Am and (239+240)Pu with depth for samples beyond the northeastern corner and lack of (241)Am in-growth over time (due to (241)Pu decay) suggest mechanical transport and mixing of discrete contaminated particles under arid conditions. Occasional samples northeast of the SDA (the direction of the prevailing winds) contain anomalously high concentrations of Pu with (240)Pu/(239)Pu isotopic ratios statistically identical to those in the northeastern corner. Taken together, these data suggest flooding resulted in mechanical transport of contaminated particles into the area between the SDA and a flood containment dike in the northeastern corner, following which subsequent contamination spreading in the northeastern direction resulted from wind transport of discrete particles. PMID:26107287

  12. Beta and gamma decay heat measurements between 0.1s - 50,000s for neturon fission of {sup 235}U, {sup 238}U and {sup 239}Pu. Progress report, June 1, 1992--December 31, 1994

    SciTech Connect

    Schier, W.A.; Couchell, G.P.

    1997-05-01

    In the investigations reported here, a helium-jet/tape-transport system was used for the rapid transfer of fission products to a low-background environment where their aggregate beta and gamma-ray spectra were measured as a function of delay time after neutron induced fission of {sup 235}U, {sup 238}U and {sup 239}Pu. Beta and gamma-ray energy distributions have been deduced for delay times as short as 0.2 s and extending out to 100,000s. Instrumentation development during the initial phase of the project included: (1) assembly and characterization of a NaI(Tl) spectrometer for determining aggregate gamma-ray energy distributions, (2) development and characterization of a beta spectrometer (having excellent gamma-ray rejection) for measuring aggregate beta-particle energy distributions, (3) assembly and characterization of a Compton-suppressed HPGe spectrometer for determining gamma-ray intensities of individual fission products to deduce fission-product yields. Spectral decomposition and analysis codes were developed for deducing energy distributions from measured aggregate beta and gamma spectra. The aggregate measurements in the time interval 0.2 - 20s after fission are of special importance since in this region data from many short-lived nuclei are missing and summation calculations in this region rely on model calculations for a large fraction of their predicted beta and gamma decay heat energy spectra. Comparison with ENDF/B-VI fission product data was performed in parallel with the measurements through a close collaboration with Dr. T. England at LANL, assisted by one of our graduate students. Such aggregate measurements provide tests of the Gross Theory of beta decay used to calculated missing contributions to this data base. Fission-product yields deduced from the HPGe studies will check the accuracy of the semi-empirical Gaussian dispersion model used presently by evaluators in the absence of measured yields.

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

    NASA Astrophysics Data System (ADS)

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

    2016-01-01

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

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

    DOE PAGES

    Gooden, M. E.; Arnold, C. W.; Becker, J. A.; Bhatia, C.; Bhike, M.; Bond, E. M.; Bredeweg, T. A.; Fallin, B.; Fowler, M. M.; Howell, C. R.; et al

    2016-01-06

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

  15. 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.

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

    DOE PAGES

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

    2015-08-30

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

  17. Contributions of Rocky Flats releases to the total plutonium in regional soils.

    PubMed

    Ibrahim, S A; Webb, S B; Whicker, F W

    1997-01-01

    Total 239,240Pu and the 240Pu:239Pu atom ratio were measured in soil samples from around the Rocky Flats Environmental Technology Site (RFETS) during 1992-1994. Mass isotopic data provided a sensitive technique to resolve low levels of RFETS 239,240Pu superimposed on plutonium from global fallout. Concentrations of 239,240Pu within this sample set ranged from 1.1 Bq kg(-1) offsite to 57 Bq kg(-1) onsite, and the 240Pu:239Pu atom ratio increased from 0.055 onsite to 0.123 at approximately 19 km east of the RFETS boundary. The relationship between 24OPu:239Pu atom ratios and distance indicated that a measurable RFETS contribution may have extended to > or = 19 km offsite in the easterly direction. Although the RFETS contribution to total plutonium at the offsite locations ranged from 24-90%, the overall inventory was relatively small. Total inventory estimates, for one transect, based on 239,240Pu and from 240Pu:239Pu atom ratio measurements were not significantly different. PMID:8972825

  18. TRU Waste Assay Methodology with the Combined Thermal Epithermal Neutron (CTEN) System

    SciTech Connect

    Veilleux, J. M.; Enter, J. A.

    2003-02-27

    The CTEN assay system is designed to measure plutonium bearing 208-L waste drums and make the transuranic versus low-level waste determination. The system was certified for Waste Isolation Pilot Plant operations and the Environmental Protection Agency approved the CTEN in 2002. It is the only system capable of making the transuranic/low-level waste (TRU/LLW) determination since it can routinely assay below 100 nCi/g. The system conducts a measurement by using either (or both) an active 14 MeV neutron pulse to induce fission in 239Pu and 241Pu or measures the spontaneous fission properties of 238Pu, 240Pu and 242Pu. When the coincidence neutron signal is combined with mass fraction data from a gamma system, the result is the total plutonium mass. The system's lower limit of detection is as low as 2 mg of weapons grade plutonium, making it an ideal platform to make the TRU/LLW determination. Analysis of an assay is made with visual basic application driven subroutines and Micros oft Excel spreadsheets. Input values and calculations include: the raw neutron scaler and coincidence counts; mass fraction information; plutonium mass; alpha, total and TRU activity; thermal power, 239Pu Equivalent Curies; fissile gram equivalent mass; decay heat; and uncertainties associated with each parameter. A general diagnostic analysis is performed for each assay to facilitate a technical review of the results. The results of analysis from 372 waste drums are summarized. The results indicate that modifying current operating procedures involving the use of acceptable knowledge isotope data and use of the lower detection limit could increase the number of certifiable assays from 38% to 66%.

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

    PubMed

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

    2014-04-01

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

  20. Verification of a Depletion Method in SCALE for the Advanced High Temperature Reactor

    SciTech Connect

    KELLY, RYAN; Ilas, Dan

    2013-01-01

    This study describes a new approach employing the Dancoff correction method to model the TRISO-based fuel form used by the Advanced High-Temperature Reactor (AHTR) reactor design concept. The Dancoff correction method is used to perform isotope depletion analysis using the TRITON sequence of SCALE and is verified by code-to-code comparisons. The current AHTR fuel design has TRISO particles concentrated along the edges of a slab fuel element. This geometry prevented the use of the DOUBLEHET treatment, previously developed in SCALE to model spherical and cylindrical fuel. The new method permits fuel depletion on complicated geometries that traditionally can be handled only by continuous energy based depletion code systems. The method was initially tested on a fuel configuration typical of the Next Generation Nuclear Plant (NGNP), where DOUBLEHET treatment is possible. A confirmatory study was performed on the AHTR reference core geometry using the VESTA code, which uses the continuous energy MCNP5 code as a transport solver and ORIGEN2.2 code for depletion calculations. Comparisons of the results indicate good agreement of whole core characteristics, such as the multiplication factor and the isotopics, including their spatial distribution. Key isotopes analyzed included 235U, 239Pu, 240Pu, and 241Pu. The results from this study indicate that the Dancoff factor method can generate estimates of core characteristics with reasonable precision for scoping studies of configurations where DOUBLEHET treatment cannot be performed.

  1. Verification of a Depletion Method in SCALE for the Advanced High Temperature Reactor

    SciTech Connect

    KELLY, RYAN; Ilas, Dan

    2012-01-01

    This study describes a new method utilizing the Dancoff factor to model a non-standard TRISO fuel form characteristic of the AHTR reactor design concept for depletion analysis using the TRITON sequence of SCALE and the validation of this method by code-to-code comparisons. The fuel used in AHTR has the TRISO particles concentrated along the edges of a slab fuel element. This particular geometry prevented the use of a standard DOUBLEHET treatment, previously developed in SCALE to handle NGNP-designed fuel. The new method permits fuel depletion on complicated geometries that traditionally can be handled only by continuous energy based depletion code systems. The method was initially tested on a fuel design typical of the NGNP, where the DOUBLEHET treatment is available. A more comprehensive study was performed using the VESTA code that uses the continuous energy MCNP5 code as a transport solver and ORIGEN2.2 code for depletion calculations. Comparisons of the results indicate good agreement of whole core characteristics, such as the multiplication factor, and the isotopics, including their spatial distribution. Key isotopes analyzed included 235U, 239Pu, 240Pu and 241Pu. The results from this study indicate that the Dancoff factor method can generate estimates of core characteristics with reasonable precision for scoping studies of configurations where the DOUBLEHET treatment is unavailable.

  2. Compilation of fission product yields Vallecitos Nuclear Center

    SciTech Connect

    Rider, B.F.

    1980-01-01

    This document is the ninth in a series of compilations of fission yield data made at Vallecitos Nuclear Center in which fission yield measurements reported in the open literature and calculated charge distributions have been utilized to produce a recommended set of yields for the known fission products. The original data with reference sources, as well as the recommended yields are presented in tabular form for the fissionable nuclides U-235, Pu-239, Pu-241, and U-233 at thermal neutron energies; for U-235, U-238, Pu-239, and Th-232 at fission spectrum energies; and U-235 and U-238 at 14 MeV. In addition, U-233, U-236, Pu-240, Pu-241, Pu-242, Np-237 at fission spectrum energies; U-233, Pu-239, Th-232 at 14 MeV and Cf-252 spontaneous fission are similarly treated. For 1979 U234F, U237F, Pu249H, U234He, U236He, Pu238F, Am241F, Am243F, Np238F, and Cm242F yields were evaluated. In 1980, Th227T, Th229T, Pa231F, Am241T, Am241H, Am242Mt, Cm245T, Cf249T, Cf251T, and Es254T are also evaluated.

  3. 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.

  4. Radioactivity in trinitite six decades later.

    PubMed

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

    2006-01-01

    The first nuclear explosion test, named the Trinity test, was conducted on July 16, 1945 near Alamogordo, New Mexico. In the tremendous heat of the explosion, the radioactive debris fused with the local soil into a glassy material named Trinitite. Selected Trinitite samples from ground zero (GZ) of the test site were investigated in detail for radioactivity. The techniques used included alpha spectrometry, high-efficiency gamma-ray spectrometry, and low-background beta counting, following the radiochemistry for selected radionuclides. Specific activities were determined for fission products (90Sr, 137Cs), activation products (60Co, 133Ba, 152Eu, 154Eu, 238Pu, 241Pu), and the remnants of the nuclear fuel (239Pu, 240Pu). Additionally, specific activities of three natural radionuclides (40K, 232Th, 238U) and their progeny were measured. The determined specific activities of radionuclides and their relationships are interpreted in the context of the fission process, chemical behavior of the elements, as well as the nuclear explosion phenomenology. PMID:16102878

  5. Preparation of actinide specimens for the US/UK joint experiment in the Dounreay Prototype Fast Reactor

    SciTech Connect

    Quinby, T C; Adair, H L; Kobisk, E H

    1982-05-01

    A joint research program involving the United States and the United Kingdom was initiated about four years ago for the purpose of studying the fuel behavior of higher actinides using in-core irradiation in the fast reactor at Dounreay, Scotland. Simultaneously, determination of integral cross sections of a wide variety of higher actinide isotopes (physics specimens) was proposed. Coincidental neutron flux and energy spectral measurements were to be made using vanadium encapsulated dosimetry materials in the immediate region of the fuel pellets and physics samples. The higher actinide samples chosen for the fuel study were /sup 241/Am and /sup 244/Cm in the forms of Am/sub 2/O/sub 3/, Cm/sub 2/O/sub 3/, and Am/sub 6/Cm(RE)/sub 7/O/sub 21/, where (RE) represents a mixture of lanthanides. Milligram quantities of actinide oxides of /sup 248/Cm, /sup 246/Cm, /sup 244/Cm, /sup 243/Cm, /sup 243/Am, /sup 241/Am, /sup 244/Pu, /sup 242/Pu, /sup 241/Pu, /sup 240/Pu, /sup 239/Pu, /sup 238/Pu, /sup 237/Np, /sup 238/U, /sup 236/U, /sup 235/U, /sup 234/U, /sup 233/U, /sup 232/Th, /sup 230/Th, and /sup 231/Pa were encapsulated to obtain nuclear cross section and reaction rate data for these materials.

  6. Value of burnup credit beyond actinides

    SciTech Connect

    Lancaster, D.; Fuentes, E.; Kang, Chi

    1997-12-01

    DOE has submitted a topical report to the NRC justifying burnup credit based only on actinide isotopes (U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, and Am-241). When this topical report is approved, it will allow a great deal of the commercial spent nuclear fuel to be transported in significantly higher capacity casks. A cost savings estimate for shipping fuel in 32 assembly (burnup credit) casks as opposed to 24 assembly (non-burnup credit) casks was previously presented. Since that time, more detailed calculations have been performed using the methodology presented in the Actinide-Only Burnup Credit Topical Report. Loading curves for derated casks have been generated using actinide-only burnup credit and are presented in this paper. The estimates of cost savings due to burnup credit for shipping fuel utilizing 32, 30, 28, and 24 assembly casks where only the 24 assembly cask does not burnup credit have been created and are discussed. 4 refs., 2 figs.

  7. Lead Slowing-Down Spectrometry Time Spectral Analysis for Spent Fuel Assay: FY11 Status Report

    SciTech Connect

    Kulisek, Jonathan A.; Anderson, Kevin K.; Bowyer, Sonya M.; Casella, Andrew M.; Gesh, Christopher J.; Warren, Glen A.

    2011-09-30

    Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration, of which PNNL is a part, to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertainty considerably lower than the approximately 10% typical of today's confirmatory assay methods. This document is a progress report for FY2011 PNNL analysis and algorithm development. Progress made by PNNL in FY2011 continues to indicate the promise of LSDS analysis and algorithms applied to used fuel. PNNL developed an empirical model based on calibration of the LSDS to responses generated from well-characterized used fuel. The empirical model, which accounts for self-shielding effects using empirical basis vectors calculated from the singular value decomposition (SVD) of a matrix containing the true self-shielding functions of the used fuel assembly models. The potential for the direct and independent assay of the sum of the masses of 239Pu and 241Pu to within approximately 3% over a wide used fuel parameter space was demonstrated. Also, in FY2011, PNNL continued to develop an analytical model. Such efforts included the addition of six more non-fissile absorbers in the analytical shielding function and the non-uniformity of the neutron flux across the LSDS assay chamber. A hybrid analytical-empirical approach was developed to determine the mass of total Pu (sum of the masses of 239Pu, 240Pu, and 241Pu), which is an important quantity in safeguards. Results using this hybrid method were of approximately the same accuracy as the pure

  8. Characterization of Pu concentration and its isotopic composition in soils of Gansu in northwestern China.

    PubMed

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

    2009-01-01

    The total 239+240Pu activities and 240Pu/239Pu atom ratios in surface soil samples (0-5cm) in the Kumtag Desert in western Gansu Province, and in a soil core sample in Lanzhou were investigated using a sector-field ICP-MS. In the surface soil samples, 239+240Pu activities in fine particles (<150microm) were 1.3-2.1 times of those in coarse particles (150microm-1mm) which ranged from 0.005 to 0.157mBq/g. Atom ratios of 240Pu/239Pu in the surface soils ranged from 0.168 to 0.192 with a mean of 0.182+/-0.008. The mean ratio was similar to the typical global fallout value although the Kumtag Desert was believed to have received close-in fallout derived from Chinese nuclear weapons tests mainly conducted in the 1970s. Furthermore, the mean 240Pu/239Pu atom ratio observed in the soil core sample in Lanzhou was similar to the typical global fallout value. In the soil core sample, 239+240Pu activities in the various layers ranged from 0.012 to 0.23mBq/g, and the inventory of 239+240Pu (32.4Bq/m2, 0-23cm) was slightly lower than that expected from global fallout (42Bq/m2) at the same latitude. Rapid downward migration of Pu isotopes was observed in Lanzhou soil core sample layers. The contribution of the 10-cm deep top layers of surface soils to total inventory was only 17%, while the contribution of deeper layers (10-23cm) was as high as 83%. The 239+240Pu activity levels and 240Pu/239Pu atom ratios in soils in Gansu Province, China are similar to those in atmospheric deposition samples collected in the spring in recent years in Japan.

  9. Self-regulating neutron coincidence counter

    DOEpatents

    Baron, N.

    1980-06-16

    A device for accurately measuring the mass of /sup 240/Pu and /sup 239/Pu in a sample having arbitrary moderation and mixed with various contaminants. The device utilizes a thermal neutron well counter which has two concentric rings of neutron detectors separated by a moderating material surrounding the well. Neutron spectroscopic information derived by the two rings of detectors is used to measure the quantity of /sup 239/Pu and /sup 240/Pu in device which corrects for background radiation, deadtime losses of the detector and electronics and various other constants of the system.

  10. Anthropogenic plutonium in the North Jiangsu tidal flats of the Yellow Sea in China.

    PubMed

    Liu, Zhiyong; Zheng, Jian; Pan, Shaoming; Gao, Jianhua

    2013-08-01

    The (239+240)Pu activities and (240)Pu/(239)Pu atom ratios were analyzed using a double-focusing SF-ICP-MS for sediment core samples obtained in 2007-2008 from the North Jiangsu tidal flats in the Yellow Sea in China. Particular attention was focused on the (240)Pu/(239)Pu atom ratios in the sediment to identify the origins of Pu isotopes. The profiles of (239+240)Pu activities in the sediment cores are similar to those of the (137)Cs activities. The (240)Pu/(239)Pu atom ratios in the tidal flats showed typical global fallout values, indicating that this area did not receive the possible early direct close-in fallout or oceanic current transported Pu from the Pacific Proving Grounds (PPG). If any, the contribution of the PPG source Pu to the total Pu inventory is negligible. This is different from the sediments in the Yangtze River estuary in the East China Sea, where the PPG source Pu contributed ca. 45 % to the total inventory. In addition, the observation of the global fallout origin Pu in the North Jiangsu tidal flats indicated that the nuclear power plant in the region was not causing any alteration/contamination to the (240)Pu/(239)Pu atom ratios. The (239+240)Pu and (137)Cs activities/inventories in the sediment cores showed correlation to the mean clay sediment compositions (fine particles) in the tidal flats. Therefore, mud deposits are served as sinks for the anthropogenic radionuclides in the tidal flats and the Yellow Sea. Integrated with the previously reported spatial distributions of (239+240)Pu and (137)Cs activities in the surface sediments of the Yellow Sea, the mechanism of Pu transport with the ocean currents and the scavenging characteristics in the Yellow Sea were discussed.

  11. Anthropogenic plutonium in the North Jiangsu tidal flats of the Yellow Sea in China.

    PubMed

    Liu, Zhiyong; Zheng, Jian; Pan, Shaoming; Gao, Jianhua

    2013-08-01

    The (239+240)Pu activities and (240)Pu/(239)Pu atom ratios were analyzed using a double-focusing SF-ICP-MS for sediment core samples obtained in 2007-2008 from the North Jiangsu tidal flats in the Yellow Sea in China. Particular attention was focused on the (240)Pu/(239)Pu atom ratios in the sediment to identify the origins of Pu isotopes. The profiles of (239+240)Pu activities in the sediment cores are similar to those of the (137)Cs activities. The (240)Pu/(239)Pu atom ratios in the tidal flats showed typical global fallout values, indicating that this area did not receive the possible early direct close-in fallout or oceanic current transported Pu from the Pacific Proving Grounds (PPG). If any, the contribution of the PPG source Pu to the total Pu inventory is negligible. This is different from the sediments in the Yangtze River estuary in the East China Sea, where the PPG source Pu contributed ca. 45 % to the total inventory. In addition, the observation of the global fallout origin Pu in the North Jiangsu tidal flats indicated that the nuclear power plant in the region was not causing any alteration/contamination to the (240)Pu/(239)Pu atom ratios. The (239+240)Pu and (137)Cs activities/inventories in the sediment cores showed correlation to the mean clay sediment compositions (fine particles) in the tidal flats. Therefore, mud deposits are served as sinks for the anthropogenic radionuclides in the tidal flats and the Yellow Sea. Integrated with the previously reported spatial distributions of (239+240)Pu and (137)Cs activities in the surface sediments of the Yellow Sea, the mechanism of Pu transport with the ocean currents and the scavenging characteristics in the Yellow Sea were discussed. PMID:23264060

  12. Decay Data Evaluation Project (DDEP): evaluation of the main 243Cm and 245Cm decay characteristics.

    PubMed

    Chechev, Valery P

    2012-09-01

    The results of new decay data evaluations are presented for (243)Cm (α) decay to nuclear levels in (239)Pu and (245)Cm (α) decay to nuclear levels in (241)Pu. These evaluated data have been obtained within the Decay Data Evaluation Project using information published up to 2011.

  13. [239Pu and chromosomal aberrations in human peripheral blood lymphocytes].

    PubMed

    Okladnikova, N D; Osovets, S V; Kudriavtseva, T I

    2009-01-01

    The genome status in somatic cells was assessed using the chromosomal aberration (CA) test in peripheral blood lymphocytes from 194 plutonium workers exposed to occupational radiation mainly from low-transportable compounds of airborne 230Pu. Pu body burden at the time of cytogenetic study varied from values close to the method sensitivity to values multiply exceeding the permissible level. Standard (routine) methods of peripheral blood lymphocytes cultivation were applied. Chromatid- and chromosomal-type structural changes were estimated. Aberrations were estimated per 100 examined metaphase cells. The quantitative relationship between the CA frequency and Pu body burden and the absorbed dose to the lung was found. Mathematical processing of results was carried out based on the phenomenological model. The results were shown as theoretical and experimental curves. The threshold of the CA yield was 0.43 +/- 0.03 kBq (Pu body burden) and 6.12 +/- 1.20 cGy (absorbed dose to the lung).

  14. Toxicological versus Radiological Hazards of {sup 239}Pu

    SciTech Connect

    Tansky, R.R.

    2001-07-26

    Plutonium is frequently referred to as ''the most toxic substance known to man''. While there are other chemicals that cause more immediately serious health consequences, plutonium does have the lowest permissible levels for any of the radioactive elements. Concentration limits for plutonium and its compounds are based on its radiotoxicity, specifically carcinogenicity, not on its chemical toxicity.

  15. Ultra-trace plutonium determination in small volume seawater by sector field inductively coupled plasma mass spectrometry with application to Fukushima seawater samples.

    PubMed

    Bu, Wenting; Zheng, Jian; Guo, Qiuju; Aono, Tatsuo; Tagami, Keiko; Uchida, Shigeo; Tazoe, Hirofumi; Yamada, Masatoshi

    2014-04-11

    Long-term monitoring of Pu isotopes in seawater is required for assessing Pu contamination in the marine environment from the Fukushima Dai-ichi Nuclear Power Plant accident. In this study, we established an accurate and precise analytical method based on anion-exchange chromatography and SF-ICP-MS. This method was able to determine Pu isotopes in seawater samples with small volumes (20-60L). The U decontamination factor was 3×10(7)-1×10(8), which provided sufficient removal of interfering U from the seawater samples. The estimated limits of detection for (239)Pu and (240)Pu were 0.11fgmL(-1) and 0.08fgmL(-1), respectively, which corresponded to 0.01mBqm(-3) for (239)Pu and 0.03mBqm(-3) for (240)Pu when a 20L volume of seawater was measured. We achieved good precision (2.9%) and accuracy (0.8%) for measurement of the (240)Pu/(239)Pu atom ratio in the standard Pu solution with a (239)Pu concentration of 11fgmL(-1) and (240)Pu concentration of 2.7fgmL(-1). Seawater reference materials were used for the method validation and both the (239+240)Pu activities and (240)Pu/(239)Pu atom ratios agreed well with the expected values. Surface and bottom seawater samples collected off Fukushima in the western North Pacific since March 2011 were analyzed. Our results suggested that there was no significant variation of the Pu distribution in seawater in the investigated areas compared to the distribution before the accident.

  16. A fast semi-quantitative method for Plutonium determination in an alpine firn/ice core

    NASA Astrophysics Data System (ADS)

    Gabrieli, J.; Cozzi, G.; Vallelonga, P.; Schwikowski, M.; Sigl, M.; Boutron, C.; Barbante, C.

    2009-04-01

    Plutonium is present in the environment as a consequence of atmospheric nuclear tests carried out in the 1960s, nuclear weapons production and releases by the nuclear industry over the past 50 years. Plutonium, unlike uranium, is essentially anthropogenic and it was first produced and isolated in 1940 by deuteron bombardment of uranium in the cyclotron of Berkeley University. It exists in five main isotopes, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, derived from civilian and military sources (weapons production and detonation, nuclear reactors, nuclear accidents). In the environment, 239Pu is the most abundant isotope. Approximately 6 tons of 239Pu have been released into the environment as a result of 541 atmospheric weapon tests Nuclear Pu fallout has been studied in various environmental archives, such as sediments, soil and herbarium grass. Mid-latitude ice cores have been studied as well, on Mont Blanc, the Western Alps and on Belukha Glacier, Siberian Altai. We present a Pu record obtained by analyzing 52 discrete samples of an alpine firn/ice core from Colle Gnifetti (M. Rosa, 4450 m a.s.l.), dating from 1945 to 1991. The239Pu signal was recorded directly, without preliminary cleaning or preconcentration steps, using an ICP-SFMS (Thermo Element2) equipped with a desolvation system (APEX). 238UH+ interferences were negligible for U concentrations lower than 50 ppt as verified both in spiked fresh snow and pre-1940 ice samples. The shape of 239Pu profile reflects the three main periods of atmospheric nuclear weapons testing: the earliest peak starts in 1954/55 to 1958 and includes the first testing period which reached a maximum in 1958. Despite a temporary halt in testing in 1959/60, the Pu concentration decreased only by half with respect to the 1958 peak. In 1961/62 Pu concentrations rapidly increased reaching a maximum in 1963, which was about 40% more intense than the 1958 peak. After the sign of the "Limited Test Ban Treaty" between USA and URSS in 1964, Pu

  17. Temporal record of Pu isotopes in inter-tidal sediments from the northeastern Irish Sea.

    PubMed

    Lindahl, Patric; Worsfold, Paul; Keith-Roach, Miranda; Andersen, Morten B; Kershaw, Peter; Leonard, Kins; Choi, Min-Seok; Boust, Dominique; Lesueur, Patrick

    2011-11-01

    A depth profile of (239)Pu and (240)Pu specific activities and isotope ratios was determined in an inter-tidal sediment core from the Esk Estuary in the northeastern Irish Sea. The study site has been impacted with plutonium through routine radionuclide discharges from the Sellafield nuclear reprocessing plant in Cumbria, NW England. A pronounced sub-surface maximum of ~10 k Bq kg(-1) was observed for (239+240)Pu, corresponding to the peak in Pu discharge from Sellafield in 1973, with a decreasing trend with depth down to ~0.04 k Bq kg(-1) in the deeper layers. The depth profile of (239+240)Pu specific activities together with results from gamma-ray spectrometry for (137)Cs and (241)Am was compared with reported releases from the Sellafield plant in order to estimate a reliable sediment chronology. The upper layers (1992 onwards) showed higher (239+240)Pu specific activities than would be expected from the direct input of annual Sellafield discharges, indicating that the main input of Pu is from the time-integrated contaminated mud patch of the northeastern Irish Sea. The (240)Pu/(239)Pu atom ratios ranged from ~0.03 in the deepest layers to >0.20 in the sub-surface layers with an activity-weighted average of 0.181. The decreasing (240)Pu/(239)Pu atom ratio with depth reflects the changing nature of operations at the Sellafield plant from weapons-grade Pu production to reprocessing spent nuclear fuel with higher burn-up times in the late 1950s. In addition, recent annual (240)Pu/(239)Pu atom ratios in winkles collected during 2003-2008 from three stations along the Cumbrian coastline showed no significant spatial or temporal differences with an overall average of 0.204, which supports the hypothesis of diluted Pu input from the contaminated mud patch.

  18. Temporal record of Pu isotopes in inter-tidal sediments from the northeastern Irish Sea.

    PubMed

    Lindahl, Patric; Worsfold, Paul; Keith-Roach, Miranda; Andersen, Morten B; Kershaw, Peter; Leonard, Kins; Choi, Min-Seok; Boust, Dominique; Lesueur, Patrick

    2011-11-01

    A depth profile of (239)Pu and (240)Pu specific activities and isotope ratios was determined in an inter-tidal sediment core from the Esk Estuary in the northeastern Irish Sea. The study site has been impacted with plutonium through routine radionuclide discharges from the Sellafield nuclear reprocessing plant in Cumbria, NW England. A pronounced sub-surface maximum of ~10 k Bq kg(-1) was observed for (239+240)Pu, corresponding to the peak in Pu discharge from Sellafield in 1973, with a decreasing trend with depth down to ~0.04 k Bq kg(-1) in the deeper layers. The depth profile of (239+240)Pu specific activities together with results from gamma-ray spectrometry for (137)Cs and (241)Am was compared with reported releases from the Sellafield plant in order to estimate a reliable sediment chronology. The upper layers (1992 onwards) showed higher (239+240)Pu specific activities than would be expected from the direct input of annual Sellafield discharges, indicating that the main input of Pu is from the time-integrated contaminated mud patch of the northeastern Irish Sea. The (240)Pu/(239)Pu atom ratios ranged from ~0.03 in the deepest layers to >0.20 in the sub-surface layers with an activity-weighted average of 0.181. The decreasing (240)Pu/(239)Pu atom ratio with depth reflects the changing nature of operations at the Sellafield plant from weapons-grade Pu production to reprocessing spent nuclear fuel with higher burn-up times in the late 1950s. In addition, recent annual (240)Pu/(239)Pu atom ratios in winkles collected during 2003-2008 from three stations along the Cumbrian coastline showed no significant spatial or temporal differences with an overall average of 0.204, which supports the hypothesis of diluted Pu input from the contaminated mud patch. PMID:21911246

  19. Highly enriched isotope samples of uranium and transuranium elements for scientific investigation

    NASA Astrophysics Data System (ADS)

    Vesnovskii, Stanislav P.; Polynov, Vladimir N.; Danilin, Lev. D.

    1992-02-01

    The paper describes the production of highly enriched isotopes of uranium, plutonium, americium and curium by electromagnetic separation for scientific and applied researches in physics, chemistry, geology, medicine, biology and other fields. Using the equipment described, the isotopes are produced in quantities sufficient to set up nuclear physical experiments, to produce nuclear reference materials and standard sources for calibration of radiometrical and mass spectrometrical equipment, in radionuclide metrology, etc. For the following isotopes the indicated degrees of isotopic enrichment were achieved: 233U - 99.97%; 235U - 99.97%; 236U - 98.0%; 238U - 99.997%; 238Pu - 99.6%; 239Pu - 99.9977%; 240Pu - 99.9-100%; 241Pu - 96.998%; 242Pu - 97.8-99.96%; 244Pu - 96.7%; 241Am - 99.6%; 242Am - 73.6%; 243Am - 99.2-99.94%; 243Cm - 99.99%; 245Cm - 99.998%; 246Cm - 99.8%; 247Cm - 90%; 248Cm - 97%. Methods for preparing layers of highly enriched isotopes on various substances are presented: - electrochemical deposition of transuranic elements from aqueous-organic and organic media and vacuum spraying: - the method of foil and coating formation via compounds in the vapour phase; - the method of fabrication of layers of transuranic elements on superthin (1-2 μm) metal substrates with additional isolating polymer-metal coatings (0.2-0.4 μm), that substantially decrease material transfer from the active layer and increase safety of product handling.

  20. Performance assessment requirements for the identification and tracking of transuranic waste intended for disposal at the Waste Isolation Pilot Plant

    SciTech Connect

    Snider, C.A.; Weston, W.W.

    1997-11-01

    To demonstrate compliance with environmental radiation protection standards for management and disposal of transuranic (TRU) radioactive wastes, a performance assessment (PA) of the Waste Isolation Pilot Plant (WIPP) was made of waste-waste and waste-repository interactions and impacts on disposal system performance. An estimate of waste components and accumulated quantities was derived from a roll-up of the generator/storage sites` TRU waste inventories. Waste components of significance, and some of negligible effect, were fixed input parameters in the model. The results identified several waste components that require identification and tracking of quantities to ensure that repository limits are not exceeded. The rationale used to establish waste component limits based on input estimates is discussed. The distinction between repository limits and waste container limits is explained. Controls used to ensure that no limits are exceeded are identified. For waste components with no explicit repository based limits, other applicable limits are contained in the WIPP Waste Acceptance Criteria (WAC). The 10 radionuclides targeted for identification and tracking on either a waste container or a waste stream basis include Am-241, Pu-238, Pu-239, Pu-240, Pu-242, U-233, U-234, U-238, Sr-90, and Cs-137. The accumulative activities of these radionuclides are to be inventoried at the time of emplacement in the WIPP. Changes in inventory curie content as a function of radionuclide decay and ingrowth over time will be calculated and tracked. Due to the large margin of compliance demonstrated by PA with the 10,000 year release limits specified, the quality assurance objective for radioassay of the 10 radionuclides need to be no more restrictive than those already identified for addressing the requirements imposed by transportation and WIPP disposal operations in Section 9 of the TRU Waste Characterization Quality Assurance Program Plan. 6 refs.

  1. OSMOSE program : statistical review of oscillation measurements in the MINERVE reactor R1-UO2 configuration.

    SciTech Connect

    Stoven, G.; Klann, R.; Zhong, Z.; Nuclear Engineering Division

    2007-08-28

    The OSMOSE program is a collaboration on reactor physics experiments between the United States Department of Energy and the France Commissariat Energie Atomique. At the working level, it is a collaborative effort between the Argonne National Laboratory and the CEA Cadarache Research Center. The objective of this program is to measure very accurate integral reaction rates in representative spectra for the actinides important to future nuclear system designs, and to provide the experimental data for improving the basic nuclear data files. The main outcome of the OSMOSE measurement program will be an experimental database of reactivity-worth measurements in different neutron spectra for the heavy nuclides. This database can then be used as a benchmark to verify and validate reactor analysis codes. The OSMOSE program (Oscillation in Minerve of isotopes in Eupraxic Spectra) aims at improving neutronic predictions of advanced nuclear fuels through oscillation measurements in the MINERVE facility on samples containing the following separated actinides: {sup 232}Th, {sup 233}U, {sup 234}U, {sup 235}U, {sup 236}U, {sup 238}U, {sup 237}Np, {sup 238}Pu, {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, {sup 242}Pu, {sup 241}Am, {sup 243}Am, {sup 244}Cm, and {sup 245}Cm. The first part of this report provides an overview of the experimental protocol and the typical processing of a series of experimental results which is currently performed at CEA-Cadarache. In the second part of the report, improvements to this technique are presented, as well as the program that was created to process oscillation measurement results from the MINERVE facility in the future.

  2. Distribution characteristics of ¹³⁷Cs, Pu isotopes and ²⁴¹Am in soil in Korea.

    PubMed

    Lee, S H; Oh, J S; Lee, J M; Lee, K B; Park, T S; Lujaniene, G; Valiulis, D; Sakalys, J

    2013-11-01

    Cesium-137, Plutonium isotopes and (241)Am were studied in soil samples collected from Korea between 2006 and 2008 to provide information on the distribution and origin of Pu isotopes and (241)Am. The vertical profiles of radionuclides showed higher activity concentrations at the surface layer and then gradually decreased with depth. A good correlation between (137)Cs and (239,240)Pu was observed, whereas a poor relationship between (137)Cs and (241)Am was found. The (238)Pu/(239,240)Pu, (241)Am/(239,240)Pu and (239,240)Pu/(137)Cs activity ratios were concordant to those of the global fallout ratios. Furthermore, the atomic ratios of (240)Pu/(239)Pu in the samples provided the information of Pu depositional history and the origin of Pu isotopes in Korea.

  3. 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.

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

    PubMed

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

    2016-03-01

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

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

    PubMed

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

    2016-03-01

    The preparation and characterization of certified reference materials (CRMs) for radionuclide content in sediments collected offshore of Bikini Atoll (IAEA-410) and in the open northwest Pacific Ocean (IAEA-412) are described and the results of the certification process are presented. The certified radionuclides include: (40)K, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (232)Th, (234)U, (238)U, (239)Pu, (239+240)Pu and (241)Am for IAEA-410 and (40)K, (137)Cs, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (232)Th, (235)U, (238)U, (239)Pu, (240)Pu and (239+240)Pu for IAEA-412. The CRMs can be used for quality assurance and quality control purposes in the analysis of radionuclides in sediments, for development and validation of analytical methods and for staff training. PMID:26631455

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

    PubMed

    Yamada, Masatoshi; Zheng, Jian

    2012-07-15

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

  7. Distributions of Pu isotopes in seawater and bottom sediments in the coast of the Japanese archipelago before and soon after the Fukushima Dai-ichi Nuclear Power Station accident.

    PubMed

    Oikawa, Shinji; Watabe, Teruhisa; Takata, Hyoe

    2015-04-01

    A radioactivity measurement survey was carried out from 24 April 2008 to 3 June 2011 to determine the levels of plutonium isotopes and (240)Pu/(239)Pu atom ratios in the marine environments off the sites of commercial nuclear power stations around the Japanese islands; the sampling period extended to two months after the Fukushima Dai-ichi Nuclear Power Station accident. In our previous study (Oikawa et al., 2015), data on Pu isotopes and (241)Am in sediments have already been reported. In this study, we report those on Pu isotopes in seawater as well as sediments, and the characteristics of sediments in addition (e.g., ignition loss and biogenic opals). Concentrations of (239+240)Pu in seawater and bottom sediments remained nearly constant at all sampling locations during the survey period. In addition, no regional differences were observed in the (239+240)Pu concentrations in surface waters. Higher (239+240)Pu concentrations were found in bottom waters at deeper sampling locations, but the (240)Pu/(239)Pu atom ratios were nearly constant regardless of the water depth. Higher (239+240)Pu concentrations were also found in bottom sediments at deeper sampling locations, but vice versa for (240)Pu/(239)Pu atom ratios as reported in the previous report. The sediments samples from deeper locations showed the higher percentage of ignition loss as well as the higher content of biogenic opal. There was likely to be some driving force participating in the transfer of Pu isotopes associated with biogenic substances to the deeper seabed. The present survey showed that the accident at the Fukushima Dai-ichi Nuclear Power Station did not contribute much to the inventory of Pu isotopes in the adjacent sea area. PMID:25659922

  8. Distributions of Pu isotopes in seawater and bottom sediments in the coast of the Japanese archipelago before and soon after the Fukushima Dai-ichi Nuclear Power Station accident.

    PubMed

    Oikawa, Shinji; Watabe, Teruhisa; Takata, Hyoe

    2015-04-01

    A radioactivity measurement survey was carried out from 24 April 2008 to 3 June 2011 to determine the levels of plutonium isotopes and (240)Pu/(239)Pu atom ratios in the marine environments off the sites of commercial nuclear power stations around the Japanese islands; the sampling period extended to two months after the Fukushima Dai-ichi Nuclear Power Station accident. In our previous study (Oikawa et al., 2015), data on Pu isotopes and (241)Am in sediments have already been reported. In this study, we report those on Pu isotopes in seawater as well as sediments, and the characteristics of sediments in addition (e.g., ignition loss and biogenic opals). Concentrations of (239+240)Pu in seawater and bottom sediments remained nearly constant at all sampling locations during the survey period. In addition, no regional differences were observed in the (239+240)Pu concentrations in surface waters. Higher (239+240)Pu concentrations were found in bottom waters at deeper sampling locations, but the (240)Pu/(239)Pu atom ratios were nearly constant regardless of the water depth. Higher (239+240)Pu concentrations were also found in bottom sediments at deeper sampling locations, but vice versa for (240)Pu/(239)Pu atom ratios as reported in the previous report. The sediments samples from deeper locations showed the higher percentage of ignition loss as well as the higher content of biogenic opal. There was likely to be some driving force participating in the transfer of Pu isotopes associated with biogenic substances to the deeper seabed. The present survey showed that the accident at the Fukushima Dai-ichi Nuclear Power Station did not contribute much to the inventory of Pu isotopes in the adjacent sea area.

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

    PubMed

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

    2012-04-01

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

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

    PubMed

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

    2012-04-01

    Historical (239)Pu activity concentrations and (240)Pu/(239)Pu atom ratios were determined in skeletons of dated modern corals collected from three locations (Chuuk Lagoon, Ishigaki Island and Iki Island) to identify spatial and temporal variations in Pu inputs to the Northwest Pacific Ocean. The main Pu source in the Northwest Pacific is fallout from atmospheric nuclear weapons testing which consists of global fallout and close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands. PPG close-in fallout dominated the Pu input in the 1950s, as was observed with higher (240)Pu/(239)Pu atom ratios (>0.30) at the Ishigaki site. Specific fallout Pu contamination from the Nagasaki atomic bomb and the Ivy Mike thermonuclear detonation at the PPG were identified at Ishigaki Island from the (240)Pu/(239)Pu atom ratios of 0.07 and 0.46, respectively. During the 1960s and 1970s, global fallout was the major Pu source to the Northwest Pacific with over 60% contribution to the total Pu. After the cessation of the atmospheric nuclear tests, the PPG again dominated the Pu input due to the continuous transport of remobilised Pu from the Marshall Islands along the North Equatorial Current and the subsequent Kuroshio Current. The Pu contributions from the PPG in recent coral bands (1984 onwards) varied over time with average estimated PPG contributions between 54% and 72% depending on location. PMID:21890207

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

    PubMed

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

    2014-01-01

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

  12. LA-ICP-MS for Pu source identification at Mayak PA, the Urals, Russia.

    PubMed

    Cagno, S; Hellemans, K; Lind, O C; Skipperud, L; Janssens, K; Salbu, B

    2014-02-01

    Information on Pu in environmental samples is traditionally based on the determination of the (240+239)Pu activity via Alpha Spectrometry (AS). A large number of alpha spectrometry sources (planchettes) containing radiochemically separated Pu are therefore stored worldwide and are available for further analyses. These archive samples represent a resource from which valuable information on isotopic composition of alpha emitters including Pu can be obtained. The relative abundances of Pu isotopes can be used to trace specific Pu sources and characterize the relative contributions of different Pu sources in a sample. Thus, in addition to the total (239+240)Pu activity, determination of the (240)Pu/(239)Pu ratio can provide valuable information on the nature of the Pu emitting sources. The Pu isotopic ratios can be determined by mass spectrometry techniques such as Sector Field Inductively Coupled Plasma Mass Spectrometry (SF-ICPMS) or Accelerator Mass Spectrometry (AMS) that require dissolution and complete destruction of the material deposited on the planchettes. In this study Laser Ablation (LA)-quadrupole-ICP-MS has been employed for the analysis of (239)Pu/(240)Pu ratios from alpha-planchettes prepared from samples originating from the Mayak PA nuclear facility, Russia. The results are compared with data from AMS and show that the (240)Pu/(239)Pu ratios obtained by LA-ICP-MS can be utilized to distinguish weapons-grade Pu from civil reprocessing sources. Moreover, isotope ratio mapping can also be performed across the planchettes, allowing e.g. the visualization of possible inhomogeneities in the Pu-isotope distribution on their surface. Thus, this solid sample technique can be applied to extract additional information from existing archives of samples. PMID:24424783

  13. LA-ICP-MS for Pu source identification at Mayak PA, the Urals, Russia.

    PubMed

    Cagno, S; Hellemans, K; Lind, O C; Skipperud, L; Janssens, K; Salbu, B

    2014-02-01

    Information on Pu in environmental samples is traditionally based on the determination of the (240+239)Pu activity via Alpha Spectrometry (AS). A large number of alpha spectrometry sources (planchettes) containing radiochemically separated Pu are therefore stored worldwide and are available for further analyses. These archive samples represent a resource from which valuable information on isotopic composition of alpha emitters including Pu can be obtained. The relative abundances of Pu isotopes can be used to trace specific Pu sources and characterize the relative contributions of different Pu sources in a sample. Thus, in addition to the total (239+240)Pu activity, determination of the (240)Pu/(239)Pu ratio can provide valuable information on the nature of the Pu emitting sources. The Pu isotopic ratios can be determined by mass spectrometry techniques such as Sector Field Inductively Coupled Plasma Mass Spectrometry (SF-ICPMS) or Accelerator Mass Spectrometry (AMS) that require dissolution and complete destruction of the material deposited on the planchettes. In this study Laser Ablation (LA)-quadrupole-ICP-MS has been employed for the analysis of (239)Pu/(240)Pu ratios from alpha-planchettes prepared from samples originating from the Mayak PA nuclear facility, Russia. The results are compared with data from AMS and show that the (240)Pu/(239)Pu ratios obtained by LA-ICP-MS can be utilized to distinguish weapons-grade Pu from civil reprocessing sources. Moreover, isotope ratio mapping can also be performed across the planchettes, allowing e.g. the visualization of possible inhomogeneities in the Pu-isotope distribution on their surface. Thus, this solid sample technique can be applied to extract additional information from existing archives of samples.

  14. Plutonium AMS measurements in Yangtze River estuary sediment

    NASA Astrophysics Data System (ADS)

    Tims, S. G.; Pan, S. M.; Zhang, R.; Fifield, L. K.; Wang, Y. P.; Gao, J. H.

    2010-04-01

    The Yangtze River is the largest single source of sediment to the continental shelf of the East China Sea. The quantity of material exported by the river is expected to decrease substantially as a consequence of an extensive continuing program of dam construction within the river catchment. We report here AMS measurements of plutonium isotope concentrations and ratios for selected depth increments from a sediment core, collected from the sub-aqueous delta of the Yangtze River estuary. The Pu derives from atmospheric nuclear weapons testing in the 1950s and 1960s, and is potentially a useful tracer of sediment deposition times in the marine environment. The results show considerable structure in the depth-concentration profile, and offer an excellent opportunity to compare Pu with the more commonly used 137Cs isotopic tracer. The AMS data show superior sensitivity and indicate that the 240Pu/ 239Pu ratio can provide a check on the deposition dates. The changes in the 240Pu and 239Pu concentrations and the 240Pu/ 239Pu ratios with sediment depth all indicate the possibility of using Pu as a geochronological tool for coastal sediment studies.

  15. 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

  16. Determination of plutonium isotopes in freshwater lake sediments by sector-field ICP-MS after separation using ion-exchange chromatography.

    PubMed

    Liao, Haiqing; Zheng, Jian; Wu, Fengchang; Yamada, Masatoshi; Tan, Mingguang; Chen, Jianmin

    2008-08-01

    The determination of Pu isotopes in lake sediments is important for many studies, such as Pu pollution source identification, sediment mixing estimation, erosion evaluation and establishment of deposition chronology in lakes. In this paper, a simple analytical method using sector field inductively coupled plasma mass spectrometry (ICP-MS) combined with two-stage chromatographic separation and purification of Pu was developed based on the optimization and adaptation of the previously published method for marine samples with an emphasis on the study of the elimination of interferences for the analysis of freshwater lake sediments. A strong base anion-exchange resin (AG MP-1M) was used to purify Pu isotopes with concentrated HBr as the final eluent for Pu elution. The chemical yields were ca. 64% and the decontamination factor for U was ca. 10(5). The developed method was validated using a freshwater lake sediment reference material (SRM-4354) and a marine sediment reference material (IAEA-368), and applied to the determination of Pu isotopes in sediment samples of Lake Poyang, East China. For the analysis of certified reference materials, both 239+240Pu activity of 31.6 mBq g(-1) and 240Pu/239Pu atom ratio of 0.033 for IAEA-368 were comparable to the certified value and/or literature values. As for SRM-4354, 239+240Pu activity of 3.90 mBq g(-1) agreed well with the certified value. However, the mean 240Pu/239Pu atom ratio of 0.144 was lower than those reported by other laboratories. This difference suggested that this material may be isotopically inhomogeneous. 240Pu/239Pu atom ratios of Poyang Lake sediment samples ranged from 0.185 to 0.192 with a mean value of 0.187+/-0.004, indicating that plutonium pollution originated from global fallout. PMID:18276148

  17. Arctic Ocean sea ice drift origin derived from artificial radionuclides.

    PubMed

    Cámara-Mor, P; Masqué, P; Garcia-Orellana, J; Cochran, J K; Mas, J L; Chamizo, E; Hanfland, C

    2010-07-15

    Since the 1950s, nuclear weapon testing and releases from the nuclear industry have introduced anthropogenic radionuclides into the sea, and in many instances their ultimate fate are the bottom sediments. The Arctic Ocean is one of the most polluted in this respect, because, in addition to global fallout, it is impacted by regional fallout from nuclear weapon testing, and indirectly by releases from nuclear reprocessing facilities and nuclear accidents. Sea-ice formed in the shallow continental shelves incorporate sediments with variable concentrations of anthropogenic radionuclides that are transported through the Arctic Ocean and are finally released in the melting areas. In this work, we present the results of anthropogenic radionuclide analyses of sea-ice sediments (SIS) collected on five cruises from different Arctic regions and combine them with a database including prior measurements of these radionuclides in SIS. The distribution of (137)Cs and (239,240)Pu activities and the (240)Pu/(239)Pu atom ratio in SIS showed geographical differences, in agreement with the two main sea ice drift patterns derived from the mean field of sea-ice motion, the Transpolar Drift and Beaufort Gyre, with the Fram Strait as the main ablation area. A direct comparison of data measured in SIS samples against those reported for the potential source regions permits identification of the regions from which sea ice incorporates sediments. The (240)Pu/(239)Pu atom ratio in SIS may be used to discern the origin of sea ice from the Kara-Laptev Sea and the Alaskan shelf. However, if the (240)Pu/(239)Pu atom ratio is similar to global fallout, it does not provide a unique diagnostic indicator of the source area, and in such cases, the source of SIS can be constrained with a combination of the (137)Cs and (239,240)Pu activities. Therefore, these anthropogenic radionuclides can be used in many instances to determine the geographical source area of sea-ice.

  18. Topical report on actinide-only burnup credit for PWR spent nuclear fuel packages. Revision 1

    SciTech Connect

    None, None

    1997-04-01

    A methodology for performing and applying nuclear criticality safety calculations, for PWR spent nuclear fuel (SNF) packages with actinide-only burnup credit, is described. The changes in the U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, and Am-241 concentration with burnup are used in burnup credit criticality analyses. No credit for fission product neutron absorbers is taken. The methodology consists of five major steps. (1) Validate a computer code system to calculate isotopic concentrations of SNF created during burnup in the reactor core and subsequent decay. A set of chemical assay benchmarks is presented for this purpose as well as a method for assessing the calculational bias and uncertainty, and conservative correction factors for each isotope. (2) Validate a computer code system to predict the subcritical multiplication factor, k{sub eff}, of a spent nuclear fuel package. Fifty-seven UO{sub 2}, UO{sub 2}/Gd{sub 2}O{sub 3}, and UO{sub 2}/PuO{sub 2} critical experiments have been selected to cover anticipated conditions of SNF. The method uses an upper safety limit on k{sub eff} (which can be a function of the trending parameters) such that the biased k{sub eff}, when increased for the uncertainty is less than 0.95. (3) Establish bounding conditions for the isotopic concentration and criticality calculations. Three bounding axial profiles have been established to assure the ''end effect'' is accounted for conservatively. (4) Use the validated codes and bounding conditions to generate package loading criteria (burnup credit loading curves). Burnup credit loading curves show the minimum burnup required for a given initial enrichment. The utility burnup record is compared to this requirement after the utility accounts for the uncertainty in its record. Separate curves may be generated for each assembly design, various minimum cooling times and burnable absorber histories. (5) Verify that SNF assemblies meet the package loading criteria

  19. Very High Temperature Reactor (VHTR) Deep Burn Core and Fuel Analysis -- Complete Design Selection for the Pebble Bed Reactor

    SciTech Connect

    B. Boer; A. M. Ougouag

    2010-09-01

    The Deep-Burn (DB) concept focuses on the destruction of transuranic nuclides from used light water reactor fuel. These transuranic nuclides are incorporated into TRISO coated fuel particles and used in gas-cooled reactors with the aim of a fractional fuel burnup of 60 to 70% in fissions per initial metal atom (FIMA). This high performance is expected through the use of multiple recirculation passes of the fuel in pebble form without any physical or chemical changes between passes. In particular, the concept does not call for reprocessing of the fuel between passes. In principle, the DB pebble bed concept employs the same reactor designs as the presently envisioned low-enriched uranium core designs, such as the 400 MWth Pebble Bed Modular Reactor (PBMR-400). Although it has been shown in the previous Fiscal Year (2009) that a PuO2 fueled pebble bed reactor concept is viable, achieving a high fuel burnup, while remaining within safety-imposed prescribed operational limits for fuel temperature, power peaking and temperature reactivity feedback coefficients for the entire temperature range, is challenging. The presence of the isotopes 239-Pu, 240-Pu and 241-Pu that have resonances in the thermal energy range significantly modifies the neutron thermal energy spectrum as compared to a ”standard,” UO2-fueled core. Therefore, the DB pebble bed core exhibits a relatively hard neutron energy spectrum. However, regions within the pebble bed that are near the graphite reflectors experience a locally softer spectrum. This can lead to power and temperature peaking in these regions. Furthermore, a shift of the thermal energy spectrum with increasing temperature can lead to increased absorption in the resonances of the fissile Pu isotopes. This can lead to a positive temperature reactivity coefficient for the graphite moderator under certain operating conditions. The effort of this task in FY 2010 has focused on the optimization of the core to maximize the pebble discharge

  20. Characterization of plutonium in deep-sea sediments of the Sulu and South China Seas.

    PubMed

    Dong, Wei; Zheng, Jian; Guo, Qiuju; Yamada, Masatoshi; Pan, Shaoming

    2010-08-01

    Anthropogenic Pu isotopes are important geochemical tracers for sediment studies. Their distributions and sources in the water columns as well as the sediments of the North Pacific have been intensively studied; however, information about Pu in the Southeast Asian seas is limited. To study the isotopic composition of Pu, and thus to identify its sources, we collected sediment core samples in the South China Sea and the Sulu Sea during the KH-96-5 Cruise of the R/V Hakuho Maru. We analysed the activities of (239+240)Pu and the atom ratios of (240)Pu/(239)Pu using isotope dilution sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS). The (240)Pu/(239)Pu atom ratios in the sediments of both areas (inventory weighted mean: 0.251 for the South China Sea and 0.280 for the Sulu Sea) were higher than the global fallout value (0.178+/-0.019), suggesting the existence of Pu from the Pacific Proving Grounds in the North Pacific. Low inventories of (239+240)Pu in sediments were observed in the South China Sea (3.75 Bq/m(2)) and the Sulu Sea (1.38 Bq/m(2)). Most of the Pu input is still present in the water column. Scavenging and benthic mixing processes were considered to be the main processes controlling the distribution of Pu in the deep-sea sediments of both study areas.

  1. Modelling the distribution of plutonium in the Pacific Ocean.

    PubMed

    Nakano, Masanao; Povinec, Pavel P

    2003-01-01

    An Oceanic General Circulation Model (OGCM) including a plutonium scavenging model as well as an advection-diffusion model has been developed for modelling the distribution of plutonium in the Pacific Ocean. Calculated 239, 240Pu water profile concentrations and 239, 240Pu inventories in water and sediment of the Pacific Ocean have showed a reasonable agreement with the experimental results. The presence of local fallout plutonium in central North Pacific waters has been confirmed. The observed 240Pu/239Pu mass ratios confirm that plutonium originating from local fallout from nuclear weapons tests carried out at Bikini and Enewetak Atolls is more rapidly removed from surface waters to deeper waters than plutonium originating from global fallout. The developed OGCM can be used for modelling the dispersion of other non-conservative tracers in the ocean as well. PMID:12860091

  2. Using sequential extraction techniques to assess the partitioning of plutonium and neptunium-237 from multiple sources in sediments from the Ob River (Siberia).

    PubMed

    Kenna, Timothy C

    2009-07-01

    Sequential extraction techniques have been developed to assess partitioning of anthropogenic radionuclides ((240)Pu, (239)Pu, and (237)Np), originating from a variety of sources, as identified by using bulk sediment isotopic composition. Sediments were leached sequentially with a series of six chemical treatments designed to approximate different environmental processes that may occur or to selectively extract trace metals contained in different solid phases of the sediments (i.e., exchangeable, reducible, carbonate, organic, acid leachable, and refractory). Results indicate the majority of Pu and Np is similarly distributed within many of the extracted fractions, with the largest percentage (66-97%) of both elements being observed in sediments treated with buffered citrate dithionite (CDB), which targets easily reduced constituents such as Mn and Fe hydrous oxides. While these results do indicate an association of Pu and Np with redox sensitive elements, the environmental implications are unclear given that the CDB treatment is more extreme than naturally occurring conditions. Minor amounts of Np partition differently from Pu in sediments. The NH(4)-acetate treatment, which is designed to liberate trace metals that are loosely adsorbed onto the surfaces of sedimentary materials such as hydrated iron oxides and humic substances, or present at exchangeable sites in clay minerals, mobilized approximately 12% of the total Np while Pu levels were below detection. The H(2)O(2) treatment, which is designed to liberate trace metals bound to organic matter, mobilized approximately 8 and approximately 1% of Np and Pu, respectively. These results indicate that a minor portion of the total Np may be affected by environmental conditions that have little or no effect on Pu. Between 7 and 24% of the Pu was observed in treatments designed to liberate Pu and Np that are tightly bound to lithogenic phases or refractory silicates. The (240)Pu/(239)Pu observed in accessible and

  3. Determination of Pu isotopes and 241Am in a reference fallout material using SF-ICP-MS.

    PubMed

    Zheng, Jian; Zhang, Yongsan; Yamada, Masatoshi; Wu, Fengchang; Igarashi, Yasuhito; Hirose, Katsumi

    2011-07-01

    This paper reports on the characterisation of activities of Pu and (241)Am, and Pu isotopic composition in a reference fallout material prepared by the Meteorological Research Institute (MRI), Japan, from samples collected at 14 stations throughout Japan in 1963-1979. The acid leaching and total digestion were used to compare whether there is difference in Pu and (241)Am activities and Pu isotopic composition between these two methods. The results of activities of (239+240)Pu and (241)Pu, and Pu isotopic composition have been reported in the previous work (Sci. Total Environ. 2010, 408, 1139-1144). In this study, the (241)Am activity and (241)Am/(239+240)Pu activity ratio in the reference fallout material are reported, and the usefulness of Pu atom ratios and (241)Am/(239+240)Pu activity ratio for source identification is discussed.

  4. The 239 Pu(n,2n)238Pu cross section: preliminary calculations

    SciTech Connect

    Chen, H; Reffo, G; Ross, M A; White, R M

    1999-03-12

    The primary motivation for the present work is to provide theoretical values for the ratio of the partial 239Pu(n,2nx{gamma})238Pu to total 239 Pu(n,2n)238Pu cross section for several discrete gamma transitions. Results and conclusions of preliminary calculations from threshold to 20 MeV are presented. Calculations are based on theoretical models with parameters obtained from the literature or from our ad hoc systematics. Optical model cross sections and transmission coefficients were determined using the coupled-channels method. The calculations included a preequilibrium component followed by multiple particle and gamma-ray emissions. Fission competition was included at all stages of de-excitation. Suggestions for further verifications and possible improvements are provided.

  5. Matrix effects corrections in DDT assay of {sup 239}Pu with the CTEN instrument

    SciTech Connect

    Hollas, C.L.; Arnone, G.; Brunson, G.; Coop, K.

    1997-11-01

    The accuracy of transuranic (TRU) waste assay using the differential die-away technique depends upon significant corrections to compensate for the effects of the matrix material in which the TRU waste is located. We have used a new instrument, the combined thermal/epithermal neutron (CTEN) instrument for the assay of TRU waste, to develop methods to improve the accuracy of these corrections. Neutrons from a pulsed 14-MeV neutron generator are moderated in the walls of the CTEN cavity and induce fission in the TRU material. The prompt neutrons from these fission events are detected in cadmium-wrapped {sup 3}He neutron detectors. We have developed methods of data acquisition and analysis to extract correlation in the neutron signals resulting from fission during active interrogation. This correlation information, in conjunction with the total number of neutrons detected, is used to determine the fraction of fission neutrons transmitted through the matrix material into the {sup 3}He detectors. This determination allows us to cleanly separate the matrix effects into two processes: matrix modification upon the neutron interrogating flux and matrix modification upon the fraction of fission neutrons transmitted to the neutron detectors. Recent results indicate that for some matrix systems, corrections for position dependent effects within the matrix are possible. 7 refs., 7 figs., 1 tab.

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

    PubMed

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

    2013-09-01

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

  7. Differential die-away technique for determination of the fissile contents in spent fuel assembly

    SciTech Connect

    Lee, Tachoon; Menlove, Howard O; Swinhoe, Nartyn T; Tobin, Stephen J

    2010-01-01

    Monte Carlo simulations were performed for the differential die-away (DDA) technique to quantify its capability to measure the fissile contents in spent fuel assemblies of 64 different cases in terms of initial enrichment, burnup, and cooling time. The DDA count rate varies according to the contents of fissile isotopes such as {sup 235}U, {sup 239}Pu, and {sup 241}Pu contained in the spent fuel assembly. The effective {sup 239}Pu concept was introduced to quantify the total fissile mass of spent fuel by weighting the relative signal contributions of {sup 235}U and {sup 241}Pu compared to that of {sup 239}Pu. The Monte Carlo simulation results show that the count rate of the DDA instrument for a spent fuel assembly of 4% initial enrichment, 45 GWD/MTU burnup, and 5 year cooling time is {approx} 9.8 x 10{sup 4} counts per second (c/s) with the 100-Hz repeated interrogation pattern of 0 to 10 {micro}s interrogation, 0.2 ms to 1 ms counting time, and 1 x 10{sup 9} n/s neutron source. The {sup 244}Cm neutron background count rate for this counting time scheme is {approx} 1 x 10{sup 4} c/s, and thus the signal to background ratio is {approx}10.

  8. Bioreduction amenability testing of actinide contaminated soils. The systems: Am{sup 241}-Pu{sup 238}, Am{sup 241}-Pu{sup 239/40}, U

    SciTech Connect

    Korich, D.G.; Sharp, J.E.

    1995-01-01

    Bioreductive processing of actinide contaminated soils can achieve extraction levels in excess of 97% for both plutonium and uranium contaminants. Reasonable reaction rates of 4 to 6 day resident times for Pu-Am have been demonstrated on 4 gram sample charges. Longer reaction times of 17 days required for uranium extraction can be improved by soil sample preconditioning and/or an increase in process reagent concentrations. The environmentally benign treatment process operates at pH 6--7, preserves the original soil matrix, and utilizes standard processing equipment. The process reagent component (inoculum SD-1 and biological growth medium PX100{trademark}) are available for utilization in an integrated system. Process techniques developed by MBX, involving graduated volume bioreactors have been proven to alleviate biological toxicity problems in treatment leachates. Bioreduction processing of actinide contaminated soils, preconditioning of soil charges, and recycling or vegetation of unacceptable tailings can be combined to provide an effective and environmentally attractive method of remediation. The soil test program was designed to determine the applicability of the MBX bioreductive technology to solubilize Pu and Am from RFP, Mound and LANL soils and uranium from Hanford and Fernald soils.

  9. 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

  10. 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.

  11. Nuclear and dosimetric features of an isotopic neutron source

    NASA Astrophysics Data System (ADS)

    Vega-Carrillo, H. R.; Hernández-Dávila, V. M.; Rivera, T.; Sánchez, A.

    2014-02-01

    A multisphere neutron spectrometer was used to determine the features of a 239PuBe neutron source that is used to operate the ESFM-IPN Subcritical Reactor. To determine the source main features it was located a 100 cm from the spectrometer which was a 6LiI(Eu) scintillator and 2, 3, 5, 8, 10 and 12 in.-diameter polyethylene spheres. Count rates obtained with the spectrometer were unfolded using the NSDUAZ code and neutron spectrum, total fluence, and ambient dose equivalent were determined. A Monte Carlo calculation was carried out to estimate the spectrum and integral features being less than values obtained experimentally due to the presence of 241Pu in the Pu used to fabricate the source. Actual neutron yield and the mass fraction of 241Pu was estimated.

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

    PubMed

    Hrnecek, E; Steier, P; Wallner, A

    2005-01-01

    Environmental samples from nuclear weapons test sites at the atolls of Mururoa and Fangataufa (French Polynesia, south Pacific) have been analyzed for their content of plutonium isotopes by applying the independent techniques of decay counting (Alpha Spectrometry) and accelerator mass spectrometry (AMS). Here, we propose the combination of both techniques which results in a maximum of information on the isotopic signature of Pu in environmental samples. Plutonium was chemically separated from the bulk material by anion exchange. (242)Pu was used as an internal standard for both AMS and alpha spectrometry. The samples for alpha spectrometry were prepared by micro-precipitation with NdF(3). After alpha spectrometry, the samples were reprocessed for AMS. Pu was co-precipitated with Fe(OH)(3) and finally, solid samples were prepared. At the VERA (Vienna Environmental Research Accelerator) facility, the various Pu isotopes were separated by their isotopic masses and quantified by the AMS technique. A good agreement of the results obtained from the AMS measurements was found with those obtained from Alpha Spectrometry. Overall, the data agree on average within 10% of each other. Isotope ratios for (238)Pu, (239)Pu and (240)Pu can be extracted from our investigations. Alpha spectrometry delivers data for the (238)Pu and the combination of ((239+240))Pu concentrations in those samples. In addition, the AMS technique provides information on the individual concentrations of (240)Pu and (239)Pu. PMID:15982894

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

    PubMed

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

    2014-03-18

    The (239+240)Pu activities and (240)Pu/(239)Pu atom ratios in sediments of the northern South China Sea and its adjacent Pearl River Estuary were determined to examine the spatial and temporal variations of Pu inputs. We clarified that Pu in the study area is sourced from a combination of global fallout and close-in fallout from the Pacific Proving Grounds in the Marshall Islands where above-ground nuclear weapons testing was carried out during the period of 1952-1958. The latter source dominated the Pu input in the 1950s, as evidenced by elevated (240)Pu/(239)Pu atom ratios (>0.30) in a dated sediment core. Even after the 1950s, the Pacific Proving Grounds was still a dominant Pu source due to continuous transport of remobilized Pu from the Marshall Islands, about 4500 km away, along the North Equatorial Current followed by the transport of the Kuroshio current and its extension into the South China Sea through the Luzon Strait. Using a simple two end-member mixing model, we have quantified the contributions of Pu from the Pacific Proving Grounds to the northern South China Sea shelf and the Pearl River Estuary are 68% ± 1% and 30% ± 5%, respectively. This study also confirmed that there were no clear signals of Pu from the Fukushima Daiichi Nuclear Power Plant accident impacting the South China Sea. PMID:24564849

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

    PubMed

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

    2014-03-18

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

  15. Tritium and plutonium in waters from the Bering and Chukchi seas.

    PubMed

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

    1999-12-01

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

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

    PubMed

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

    2013-08-01

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

  17. Plutonium in Colorado residents: results of autopsy bone samples collected during 1975-1979.

    PubMed

    Ibrahim, S A; Warren, G M; Whicker, F W; Efurd, D W

    2002-08-01

    Concentrations of (239,240)Pu and the 240Pu/239Pu atom ratios were measured in rib samples from 55 non-occupationally exposed Colorado residents. Samples were collected at autopsy during 1975-1979 under an earlier study intended to compare plutonium levels in liver and lung of people who lived at various proximities to the Rocky Flats Environmental Technology Site (RFETS) near Denver. Overall, median (239,240)Pu concentrations from rib samples were 100, 80, and 57 microBq g(-1) ash weight for area locations A, B, and C, respectively. Area A encompassed subjects who lived within 25 km of RFETS, area B was between 25 and 50 km from RFETS, and area C included all of Colorado outside 50 km from the site and east of the continental divide. The corresponding median plutonium skeletal burdens estimated for these area locations were 146, 93, and 71 mBq, respectively. A statistically significant difference was noted only between plutonium concentrations in male rib samples and their skeletal burdens from area A compared to area C. However, based on a regression analysis of all study subjects, distance from RFETS was not statistically correlated to plutonium rib concentrations or skeletal burdens in this sample. Overall, median 240Pu/239Pu atom ratios were 0.20, 0.18, and 0.17 for areas A, B, and C, respectively. Although higher (239,240)Pu concentrations and skeletal burdens were indicated in area A males than area C males, we cannot conclude that RFETS releases may have caused this difference. The decreasing trends in the 240Pu/239Pu ratios with distance from RFETS are contrary with such a conclusion and strongly indicate that the material was primarily global fallout rather than weapons-grade plutonium that was processed at RFETS. Furthermore, there are other plausible explanations for the differences observed between area A and C residents. These include a decreasing trend in global fallout from the Rocky Mountain foothills eastward, smoking history differences, sample

  18. /sup 239/ /sup 240/Pu and /sup 238/Pu in sediments of the Hudson River estuary

    SciTech Connect

    Linsalata, P.; Wrenn, M.E.; Cohen, N.; Singh, N.P.

    1980-12-01

    Plutonium-239,240 and plutonium-238 were determined in 59 Hudson River sediment dredge samples collected during 1973-77 in the vicinity of the Indian Point Nuclear Power Station. Acid leaching followed by solvent extraction, electrodeposition, and alpha-spectrometry were used to extract, purify, and quantitate plutonium isotopes present in these samples. Annual median plutonium-238/plutonium-239,240 isotopic activity ratios in surficial sediments were 0.032 (1973-74), 0.035 (1975), 0.042 (1976), and 0.040 (1977). The source of these nuclides in the estuary was identified by analysis of the sample isotopic activity ratios. On the basis of the sampling regimen and the methods used, it is concluded that no input, other than that of fallout, has contributed significantly to the plutonium burden in Hudson sediments. (1 map, 9 references, 9 tables)

  19. Assay of long-lived radionuclides in low-level wastes from power reactors

    SciTech Connect

    Cline, J.E.; Noyce, J.R.; Coe, L.J.; Wright, K.W.

    1985-04-01

    The 10 CFR Part 61 waste classification system includes several nuclides which are difficult to assay without expensive radiochemical methods. In order for waste generators to classify wastes practically, NRC Staff has recommended the use of correlation factors to scale the difficult-to-measure nuclides with nuclides which can be measured more easily (i.e., gamma emitters such as /sup 60/Co or /sup 137/Cs). In this study, Science Applications International Corporation (SAIC) performed complete radiochemical assays for all the 10 CFR Part 61 waste classification nuclides on over 100 samples. These data, along with almost 800 other samples in the SAIC data base, were used to assess the validity of correlation factors suggested for use in nuclear power plant wastes. Specific generic correlation factors are recommended with other approaches to correlate nuclides for which generic scaling factors are not defensible. The primary nuclide correlations studied were /sup 14/C, /sup 55/Fe, /sup 59/Ni, /sup 63/Ni, and /sup 94/Nb, with /sup 60/Co; /sup 90/Sr, /sup 99/Tc, /sup 129/I, /sup 135/Cs, and /sup 239, 240/Pu with /sup 137/Cs; /sup 238/Pu, /sup 239, 240/Pu, /sup 241/Pu, /sup 241/Am, /sup 242/Cm, and /sup 243, 244/Cm with /sup 144/Ce; and /sup 238/Pu, /sup 241/Pu, /sup 241/Am, /sup 242/Cm and /sup 243, 244/Cm with /sup 239, 240/Pu.

  20. Plutonium aerosol fluxes and pulmonary exposure rates during resuspension from bare soils near a chemical separation facility

    SciTech Connect

    Shinn, J.H.; Homan, D.N.; Gay, D.D.

    1982-11-01

    The purpose of this study was to examine the plutonium aerosol fluxes (Curies per ground area per unit time) from a bare soil near a chemical separation facility and to determine the characteristics of the plutonium-bearing aerosols, which are of consequence in deposition of the alpha-emitters into the lung. These characteristics are the plutonium aerosol concentration (Curies per unit volume of air), the particle size distribution, the radioactivity size distribution, the enhancement factors, and others. The site was the agricultural field adjacent to H-area of Savannah River Plant near Aiken, South Carolina, where low-level releases of /sup 239/Pu and /sup 240/Pu occurred from 1967 through 1974. The releases then changed primarily to /sup 238/Pu. Results indicate that plutonium aerosol concentrations were not greatly increased by removing the vegetation and cultivating the field. Following a rain which stabilized the surface /sup 239/Pu concentrations were 37% of normal to 144% of normal as the field dried. The /sup 239/Pu concentration was broadly distributed over particle sizes and had MAD 2.7 ..mu..m. The /sup 239/Pu concentration distributions were found to be 12% respirable and the maximum concentration observed, 4.94 x 10/sup -17/ Ci m/sup -3/, amounted to an inconsequential exposure of less than 10/sup -5/ lifetime background dose for 100 days exposure. /sup 239/Pu flux was not greatly increased as the dust flux increased because /sup 239/Pu activity of the aerosols decreased with time to counteract the increased dust flux.

  1. Comparative food-chain behavior and distribution of actinide elements in and around a contaminated fresh-water pond

    SciTech Connect

    Garten, C.T. Jr.; Trabalka, J.R.; Bogle, M.A.

    1981-01-01

    The bioaccumulation of /sup 233/ /sup 234/U, /sup 238/U, /sup 238/Pu, /sup 239/ /sup 240/Pu, /sup 241/Am, and /sup 244/Cm in both native and introduced biota was studied at Pond 3513, a former low-level radioactive waste settling basin at Oak Ridge National Laboratory. This system, which was decommissioned in 1976 after more than 30 years use, contains approximately 5 Ci of /sup 239/ /sup 240/Pu; inventories of other actinide isotopes are considerably less. Significantly higher concentrations of actinides in fish that were allowed access to sediments indicated that sedimentary particulates may be the primary source of transuranics to biota in shallow fresh-water ecosystems. Our study determined habitat, in particular the degree of association of an organism with the sediment-water interface, to be the primary factor in controlling transuranic concentrations in aquatic biota. In most of the biological samples analyzed, excluding samples suspected of being contaminated by sediment, /sup 241/Am//sup 239/Pu, /sup 244/Cm//sup 239/Pu, and /sup 238/U//sup 239/Pu ratios were greater than the respective ratio in sediment while /sup 233/ /sup 234/U//sup 238/U, and /sup 239/ /sup 240/Pu//sup 238/Pu ratios were not different from the respective ratios in sediment. The relative uptake of actinides from contaminated sediment by aquatic and terrestrial biota at this site was U > Cm greater than or equal to Am > Pu. The relative extractability of actinides from shoreline sediment was U > Cm approx. = Am > Pu; we also observed the same relative ranking for sediment-water exchange in situ. Concentrations of transuranics in water, terrestrial vegetation, and vertebrate carcasses were less than 10% of the recommended public exposure maximum permissible concentration (MPC) of the ICRP.

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

    PubMed Central

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

    2012-01-01

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

  3. Superconducting calorimetric alpha particle sensors for nuclear nonproliferation applications

    SciTech Connect

    Horansky, Robert D.; Ullom, Joel N.; Beall, James A.; Hilton, Gene C.; Irwin, Kent D.; Dry, Donald E.; Hastings, Elizabeth P.; Lamont, Stephen P.; Rudy, Clifford R.; Rabin, Michael W.

    2008-09-22

    Identification of trace nuclear materials is usually accomplished by alpha spectrometry. Current detectors cannot distinguish critical elements and isotopes. We have developed a detector called a microcalorimeter, which achieves a resolution of 1.06 keV for 5.3 MeV alphas, the highest resolving power of any energy dispersive measurement. With this exquisite resolution, we can unambiguously identify the {sup 240}Pu/{sup 239}Pu ratio in Pu, a critical measurement for ascertaining the intended use of nuclear material. Furthermore, we have made a direct measurement of the {sup 209}Po ground state decay.

  4. 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

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

    SciTech Connect

    Meadows, J W

    1983-10-01

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

  6. 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

  7. Certified Reference Material IAEA-446 for radionuclides in Baltic Sea seaweed.

    PubMed

    Pham, M K; Benmansour, M; Carvalho, F P; Chamizo, E; Degering, D; Engeler, C; Gascó, C; Gwynn, J P; Harms, A V; Hrnecek, E; Ibanez, F L; Ilchmann, C; Ikaheimonen, T; Kanisch, G; Kloster, M; Llaurado, M; Mauring, A; Møller, B; Morimoto, T; Nielsen, S P; Nies, H; Norrlid, L D R; Pettersson, H B L; Povinec, P P; Rieth, U; Samuelsson, C; Schikowski, J; Silobritiene, B V; Smedley, P A; Suplinska, M; Vartti, V-P; Vasileva, E; Wong, J; Zalewska, T; Zhou, W

    2014-05-01

    A Certified Reference Material (CRM) for radionuclides in seaweed (Fucus vesiculosus) from the Baltic Sea (IAEA-446) is described and the results of the certification process are presented. The (40)K, (137)Cs, (234)U and (239+240)Pu radionuclides were certified for this material, and information values for 12 other radionuclides ((90)Sr, (99)Tc, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (230)Th, (232)Th, (235)U, (238)U, (239)Pu and (240)Pu) are presented. The CRM can be used for Quality Assurance/Quality Control of analysis of radionuclides in seaweed and other biota samples, as well as for development and validation of analytical methods, and for training purposes.

  8. Certified Reference Material IAEA-446 for radionuclides in Baltic Sea seaweed.

    PubMed

    Pham, M K; Benmansour, M; Carvalho, F P; Chamizo, E; Degering, D; Engeler, C; Gascó, C; Gwynn, J P; Harms, A V; Hrnecek, E; Ibanez, F L; Ilchmann, C; Ikaheimonen, T; Kanisch, G; Kloster, M; Llaurado, M; Mauring, A; Møller, B; Morimoto, T; Nielsen, S P; Nies, H; Norrlid, L D R; Pettersson, H B L; Povinec, P P; Rieth, U; Samuelsson, C; Schikowski, J; Silobritiene, B V; Smedley, P A; Suplinska, M; Vartti, V-P; Vasileva, E; Wong, J; Zalewska, T; Zhou, W

    2014-05-01

    A Certified Reference Material (CRM) for radionuclides in seaweed (Fucus vesiculosus) from the Baltic Sea (IAEA-446) is described and the results of the certification process are presented. The (40)K, (137)Cs, (234)U and (239+240)Pu radionuclides were certified for this material, and information values for 12 other radionuclides ((90)Sr, (99)Tc, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (230)Th, (232)Th, (235)U, (238)U, (239)Pu and (240)Pu) are presented. The CRM can be used for Quality Assurance/Quality Control of analysis of radionuclides in seaweed and other biota samples, as well as for development and validation of analytical methods, and for training purposes. PMID:24291528

  9. First results on 236U levels in global fallout.

    PubMed

    Sakaguchi, A; Kawai, K; Steier, P; Quinto, F; Mino, K; Tomita, J; Hoshi, M; Whitehead, N; Yamamoto, M

    2009-07-01

    The global fallout (236)U level in soil was deduced from measurements of (236)U, (239+240)Pu and (137)Cs in surface soils which are solely influenced by global fallout. A total of 12 soil cores from the depths of 0-10, 0-20 and 0-30 cm were collected at a flat forest area in Japan. Concentrations of (239+240)Pu and (238)U were determined by alpha-particle spectrometry, while the (236)U/(238)U ratio was measured with accelerator mass spectrometry (AMS). Consistent (236)U/(239)Pu ratios between 0.212 and 0.253 were found. Using this ratio, the total global fallout of (236)U on the earth is estimated to be as much as ca. 900 kg. This knowledge will contribute to the promotion of research on U isotopes, including (236)U, for the fields of geo-resources, waste management and geochemistry. PMID:19406452

  10. Comparative skeletal distribution of Am and Pu in man, monkey, and baboon

    SciTech Connect

    Lynch, T.P.; Kathren, R.L.; Dagle, G.E.; McInroy, J.F. )

    1989-01-01

    The skeletal distribution of Am and Pu in four human cases was compared with the skeletal distributions of these radioelements in baboons and monkeys. Excellent agreement was noted among the four human cases; data were available for Am in all four and Pu in three. A statistically significant correlation was found between the {sup 241}Am and {sup 239}Pu + {sup 240}Pu skeletal distributions in the humans and those in nonhuman primates. Trabecular bone had the highest concentrations of {sup 241}Am and {sup 239+240}Pu in humans, baboons, and monkeys. Scaling factors are proposed to convert the percentages of skeletal activity in animal bones to the corresponding percentages in the bones of the human skeleton.

  11. Global fallout Pu recorded in lacustrine sediments in Lake Hongfeng, SW China.

    PubMed

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

    2008-03-01

    Studies on the distribution and isotope compositions of fallout Pu are important for source characterization of possible future non-fallout Pu contamination in aquatic environments, and useful for dating of recent sediments to understand the pollution history of environmental contaminants. We present the historical record of atmospheric Pu fallout reconstructed from a sediment core from Lake Hongfeng, China. The Pu activity profile was in agreement with the 137Cs profile. Inventories were 50.7 Bq m(-2) for 239+240Pu and 1586 Bq m(-2) for 137Cs. The average 240Pu/239Pu atom ratio was 0.185+/-0.009, indicating that Pu originated from global stratospheric fallout rather than from direct tropospheric or close-in fallout from the Chinese nuclear testing conducted in the 1970s. Our data suggested that Lake Hongfeng would be an ideal setting for monitoring atmospheric fallout and environmental changes in this region.

  12. First results on 236U levels in global fallout.

    PubMed

    Sakaguchi, A; Kawai, K; Steier, P; Quinto, F; Mino, K; Tomita, J; Hoshi, M; Whitehead, N; Yamamoto, M

    2009-07-01

    The global fallout (236)U level in soil was deduced from measurements of (236)U, (239+240)Pu and (137)Cs in surface soils which are solely influenced by global fallout. A total of 12 soil cores from the depths of 0-10, 0-20 and 0-30 cm were collected at a flat forest area in Japan. Concentrations of (239+240)Pu and (238)U were determined by alpha-particle spectrometry, while the (236)U/(238)U ratio was measured with accelerator mass spectrometry (AMS). Consistent (236)U/(239)Pu ratios between 0.212 and 0.253 were found. Using this ratio, the total global fallout of (236)U on the earth is estimated to be as much as ca. 900 kg. This knowledge will contribute to the promotion of research on U isotopes, including (236)U, for the fields of geo-resources, waste management and geochemistry.

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

    PubMed

    Thakur, P; Ballard, S; Nelson, R

    2012-05-01

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

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

    PubMed

    Thakur, P; Ballard, S; Nelson, R

    2012-05-01

    The Waste Isolation Pilot Plant (WIPP) is the only operating deep underground geologic nuclear repository in the United States. It is located in southeastern New Mexico, approximately 655 m (2150 ft) below the surface of the Earth in a bedded Permian evaporite salt formation. This mined geologic repository is designed for the safe disposal of transuranic (TRU) wastes generated from the US defense program. Aerosol and soil samples have been collected near the WIPP site to investigate the sources of plutonium in the WIPP environment since the late 1990s, well before WIPP received its first shipment. Activities of (238)Pu, (239+240)Pu and (241)Am were determined by alpha spectrometry following a series of chemical separations. The concentrations of Al and U were determined in a separate set of samples by inductively coupled plasma mass spectrometry. The annual airborne concentrations of (239+240)Pu during the period from 1998 to 2010 show no systematic interannual variations. However, monthly (239+240)Pu particulate concentrations show a typical seasonal variation with a maximum in spring, the time when strong and gusty winds frequently give rise to blowing dust. Resuspension of soil particles containing weapons fallout is considered to be the predominant source of plutonium in the WIPP area. Further, this work characterizes the source, temporal variation and its distribution with depth in a soil profile to evaluate the importance of transport mechanisms affecting the fate of these radionuclides in the WIPP environment. The mean (137)Cs/(239+240)Pu, (241)Am/(239+240)Pu activity ratio and (240)Pu/(239)Pu atom ratio observed in the WIPP samples are consistent with the source being largely global fallout. There is no evidence of any release from the WIPP contributing to radionuclide concentrations in the environment. PMID:22549140

  15. Plutonium in Soils from Northeast China and Its Potential Application for Evaluation of Soil Erosion

    PubMed Central

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

    2013-01-01

    Surface and soil core samples from northeast China were analyzed for Pu isotopes. The measured 240Pu/239Pu atomic ratios and 239 + 240Pu/137Cs activity ratios revealed that the global fallout is the dominant source of Pu and 137Cs at these sites. Migration behavior of Pu varying with land type and human activities resulted in different distribution of Pu in surface soils. A sub-surface maximum followed by exponential decline of 239 + 240Pu concentrations was observed in an undisturbed soil core, with a total 239 + 240Pu inventory of 86.9 Bq/m2 and more than 85% accumulated in 0 ~ 20 cm layers. While only half inventory of Pu was obtained in another soil core and no sub-surface maximum value occurred. Erosion of topsoil in the site should be the most possible reason for the significantly lower Pu inventory, which is also supported by the reported 137Cs profiles. These results demonstrated that Pu could be applied as an ideal substitute of 137Cs for soil erosion study in the future. PMID:24336360

  16. DETERMINATION OF REPORTABLE RADIONUCLIDES FOR DWPF SLUDGE BATCH 5 (MACROBATCH 6)

    SciTech Connect

    Bannochie, C.; Bibler, N.; Diprete, D.

    2010-02-04

    The Waste Acceptance Product Specifications (WAPS) 1.2 require that ''The Producer shall report the inventory of radionuclides (in Curies) that have half-lives longer than 10 years and that are, or will be, present in concentrations greater than 0.05 percent of the total inventory for each waste type indexed to the years 2015 and 3115''. As part of the strategy to comply with WAPS 1.2, the Defense Waste Processing Facility (DWPF) will report for each waste type, all radionuclides (with half-lives greater than 10 years) that have concentrations greater than 0.01 percent of the total inventory from time of production through the 1100 year period from 2015 through 3115. The initial listing of radionuclides to be included is based on the design-basis glass as identified in the Waste Form Compliance Plan (WCP) and Waste Form Qualification Report (WQR). However, it is required that this list be expanded if other radionuclides with half-lives greater than 10 years are identified that may meet the greater than 0.01% criterion for Curie content. Specification 1.6 of the WAPS, International Atomic Energy Agency (IAEA) Safeguards Reporting for High Level Waste (HLW), requires that the ratio by weights of the following uranium and plutonium isotopes be reported: U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, and Pu-242. Therefore, the complete set of reportable radionuclides must also include this set of U and Pu isotopes. The DWPF is receiving radioactive sludge slurry from HLW Tank 40. The radioactive sludge slurry in Tank 40 is a blend of the heel from Tank 40 (Sludge Batch 4 (SB4)), Sludge Batch 5 (SB5) that was transferred to Tank 40 from Tank 51, and H-Canyon Np transfers completed after the start of processing. The blend of sludge in Tank 40 is also referred to as Macrobatch 6 (MB6). This report develops the list of reportable radionuclides and associated activities and determines the radionuclide activities as a function of time. The DWPF will use

  17. DETERMINATION OF REPORTABLE RADIONUCLIDES FOR DWPF SLUDGE BATCH 4 MACROBATCH 5

    SciTech Connect

    Bannochie, C; Ned Bibler, N; David Diprete, D

    2008-05-30

    The Waste Acceptance Product Specifications (WAPS)1 1.2 require that 'The Producer shall report the inventory of radionuclides (in Curies) that have half-lives longer than 10 years and that are, or will be, present in concentrations greater than 0.05 percent of the total inventory for each waste type indexed to the years 2015 and 3115'. As part of the strategy to meet WAPS 1.2, the Defense Waste Processing Facility (DWPF) will report for each waste type, all radionuclides (with half-lives greater than 10 years) that have concentrations greater than 0.01 percent of the total inventory from time of production through the 1100 year period from 2015 through 3115. The initial listing of radionuclides to be included is based on the design-basis glass as identified in the Waste Form Compliance Plan (WCP)2 and Waste Form Qualification Report (WQR)3. However, it is required that this list be expanded if other radionuclides with half-lives greater than 10 years are identified that may meet the greater than 0.01% criterion for Curie content. Specification 1.6 of the WAPS, International Atomic Energy Agency (IAEA) Safeguards Reporting for High Level Waste (HLW), requires that the ratio by weights of the following uranium and plutonium isotopes be reported: U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, and Pu-242. Therefore, the complete set of reportable radionuclides must also include this set of U and Pu isotopes. The DWPF is receiving radioactive sludge slurry from HLW Tank 40. The radioactive sludge slurry in Tank 40 is a blend of the previous contents of Tank 40 (Sludge Batch 3) and the sludge that was transferred to Tank 40 from Tank 51. The blend of sludge from Tank 51 and Tank 40 defines Sludge Batch 4 (also referred to as Macrobatch 5 (MB5)). This report develops the list of reportable radionuclides and associated activities and determines the radionuclide activities as a function of time. The DWPF will use this list and the activities as one of

  18. Fission Product Yields from Fission Spectrum n+{sup 239}Pu for ENDF/B-VII.1

    SciTech Connect

    Chadwick, M.B.; Kawano, T.; Barr, D.W.; Mac Innes, M.R.; Kahler, A.C.; Graves, T.; Selby, H.; Burns, C.J.; Inkret, W.C.; Keksis, A.L.; Lestone, J.P.; Sierk, A.J.; Talou, P.

    2010-12-15

    We describe a new cumulated fission product yield (FPY) evaluation for fission spectrum neutrons on plutonium that updates the ENDF/B-VI evaluation by England and Rider, for the forthcoming ENDF/B-VII.1 database release. We focus on FPs that are needed for high accuracy burnup assessments; that is, for inferring the number of fissions in a neutron environment. Los Alamos conducted an experiment in the 1970s in the Bigten fast critical assembly to determine fission product yields as part of the Interlaboratory Reaction Rate (ILRR) collaboration, and this has defined the Laboratory's fission standard to this day. Our evaluation includes use of the LANL-ILRR measurements (not previously available to evaluators) as well as other Laboratory FPY measurements published in the literature, especially the high-accuracy mass spectrometry data from Maeck and others. Because the measurement database for some of the FPs is small - especially for {sup 99}Mo - we use a meta-analysis that incorporates insights from other accurately-measured benchmark FP data, using R-value ratio measurements. The meta-analysis supports the FP measurements from the LANL-ILRR experiment. Differences between our new evaluations and ENDF/B-VI are small for some FPs (less than 1-2%-relative for {sup 95}Zr, {sup 140}Ba, {sup 144}Ce), but are larger for {sup 99}Mo (4%-relative) and {sup 147}Nd (5%-relative, at 1.5 MeV) respectively. We present evidence for an incident neutron energy dependence to the {sup 147}Nd fission product yield that accounts for observed differences in the FPY at a few-hundred keV average energy in fast reactors versus measurements made at higher average neutron energies in Los Alamos' fast critical assemblies. Accounting for such FPY neutron energy dependencies is important if one wants to reach a goal of determining the number of fissions to accuracies of 1-2%. An evaluation of the energy-dependence of fission product yields is given for all A values based on systematical trends in the measured data, with a focus on the energy dependence over the fast neutron energy range from 0.2-2 MeV. Based on these trends, we present an evaluation of the FPY data at 0.5 and 2.0 MeV average incident neutron energies. This new set of ENDF/B-VII data will enable users to linearly interpolate between the pooled FPY data at {approx}0.5 MeV and our new data at 2 MeV to obtain FPYs at other energies.

  19. Fission fragment charge and mass distributions in 239Pu(n, f ) in the adiabatic nuclear energy density functional theory

    DOE PAGES

    Regnier, D.; Dubray, N.; Schunck, N.; Verriere, M.

    2016-05-13

    Here, accurate knowledge of fission fragment yields is an essential ingredient of numerous applications ranging from the formation of elements in the r process to fuel cycle optimization for nuclear energy. The need for a predictive theory applicable where no data are available, together with the variety of potential applications, is an incentive to develop a fully microscopic approach to fission dynamics.

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

    SciTech Connect

    Antonio, Cheryl L.

    2012-07-19

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

  1. OSMOSE experiment representativity studies.

    SciTech Connect

    Aliberti, G.; Klann, R.; Nuclear Engineering Division

    2007-10-10

    The OSMOSE program aims at improving the neutronic predictions of advanced nuclear fuels through measurements in the MINERVE facility at the CEA-Cadarache (France) on samples containing the following separated actinides: Th-232, U-233, U-234, U-235, U-236, U-238, Np-237, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, Am-241, Am-243, Cm-244 and Cm-245. The goal of the experimental measurements is to produce a database of reactivity-worth measurements in different neutron spectra for the separated heavy nuclides. This database can then be used as a benchmark for integral reactivity-worth measurements to verify and validate reactor analysis codes and integral cross-section values for the isotopes tested. In particular, the OSMOSE experimental program will produce very accurate sample reactivity-worth measurements for a series of actinides in various spectra, from very thermalized to very fast. The objective of the analytical program is to make use of the experimental data to establish deficiencies in the basic nuclear data libraries, identify their origins, and provide guidelines for nuclear data improvements in coordination with international programs. To achieve the proposed goals, seven different neutron spectra can be created in the MINERVE facility: UO2 dissolved in water (representative of over-moderated LWR systems), UO2 matrix in water (representative of LWRs), a mixed oxide fuel matrix, two thermal spectra containing large epithermal components (representative of under-moderated reactors), a moderated fast spectrum (representative of fast reactors which have some slowing down in moderators such as lead-bismuth or sodium), and a very hard spectrum (representative of fast reactors with little moderation from reactor coolant). The different spectra are achieved by changing the experimental lattice within the MINERVE reactor. The experimental lattice is the replaceable central part of MINERVE, which establishes the spectrum at the sample location. This configuration

  2. Final Report on Utilization of TRU TRISO Fuel as Applied to HTR Systems Part I: Pebble Bed Reactors

    SciTech Connect

    Brian Boer; Abderrafi M. Ougouag

    2011-03-01

    The Deep-Burn (DB) concept [ ] focuses on the destruction of transuranic nuclides from used light water reactor (LWR) fuel. These transuranic nuclides are incorporated into tri-isotopic (TRISO) coated fuel particles and used in gas-cooled reactors with the aim of a fractional fuel burnup of 60 to 70% in fissions per initial metal atom (FIMA). This high performance is expected through the use of multiple recirculation passes of the fuel in pebble form without any physical or chemical changes between passes. In particular, the concept does not call for reprocessing of the fuel between passes. In principle, the DB pebble bed concept employs the same reactor designs as the presently envisioned low-enriched uranium core designs, such as the 400 MWth Pebble Bed Modular Reactor (PBMR-400) [ ]. Although it has been shown in the previous Fiscal Year (FY) (2009) that a PuO2 fueled pebble bed reactor concept is viable, achieving a high fuel burnup while remaining within safety-imposed prescribed operational limits for fuel temperature, power peaking, and temperature reactivity feedback coefficients for the entire temperature range, is challenging. The presence of the isotopes 239Pu, 240Pu, and 241Pu that have resonances in the thermal energy range significantly modifies the neutron thermal energy spectrum as compared to a standard, UO2-fueled core. Therefore, the DB pebble bed core exhibits a relatively hard neutron energy spectrum. However, regions within the pebble bed that are near the graphite reflectors experience a locally softer spectrum. This can lead to power and temperature peaking in these regions. Furthermore, a shift of the thermal energy spectrum with increasing temperature can lead to increased absorption in the resonances of the fissile Pu isotopes. This can lead to a positive temperature reactivity coefficient for the graphite moderator under certain operating conditions. Regarding the coated particle performance, the FY 2009 investigations showed that no

  3. ANALYSIS AND EXAMINATION OF MOX FUEL FROM NONPROLIFERATION PROGRAMS

    SciTech Connect

    McCoy, Kevin; Machut, Dr McLean; Morris, Robert Noel; Blanpain, Patrick; Hemrick, James Gordon

    2013-01-01

    The U.S. Department of Energy has decided to dispose of a portion of the nation s surplus plutonium by reconstituting it into mixed oxide (MOX) fuel and irradiating it in commercial power reactors. Four lead assemblies were manufactured and irradiated to a maximum fuel rod burnup of 47.3 MWd/kg heavy metal. This was the first commercial irradiation of MOX fuel with a 240Pu/239Pu ratio of less than 0.10. Five fuel rods with varying burnups and plutonium contents were selected from one of the assemblies and shipped to Oak Ridge National Laboratory for hot cell examination. The performance of the rods was analyzed with AREVA s next-generation GALILEO code. The results of the analysis confirmed that the fuel rods had performed safely and predictably, and that GALILEO is applicable to MOX fuel with a low 240Pu/239Pu ratio as well as to standard MOX. The results are presented and compared to the GALILEO database. In addition, the fuel cladding was tested to confirm that traces of gallium in the fuel pellets had not affected the mechanical properties of the cladding. The irradiated cladding was found to remain ductile at both room temperature and 350 C for both the axial and circumferential directions.

  4. 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.

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

    DOE PAGES

    Armstrong, Christopher R.; Nuessle, Patterson R.; Brant, Heather A.; 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. Characterization and source term assessments of radioactive particles from Marshall Islands using non-destructive analytical techniques

    NASA Astrophysics Data System (ADS)

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

    2006-08-01

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

  7. 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.

  8. MATERIAL PROPERTIES OF PLUTONIUM-BEARING OXIDES STORED IN STAINLESS STEEL CONTAINERS

    SciTech Connect

    Kessinger, G.; Almond, P.; Bridges, N.; Bronikowski, M.; Crowder, M.; Duffey, J.; Livingston, R.; Mcelwee, M.; Missimer, D.; Scogin, J.; Summer, M.; Jurgensen, A.

    2010-02-01

    The destructive examination (DE) of 3013 containers after storage is part of the Surveillance and Monitoring Program based on the Department of Energy's standard for long-term storage of Pu (DOE-STD-3013). The stored, Pu-bearing materials may contain alkali halide contamination that varies from trace amounts of salt to about 50 weight percent, with smaller fractions of other compounds and oxides. These materials were characterized prior to packaging, and surveillance characterizations are conducted to determine the behavior of the materials during long term storage. The surveillance characterization results are generally in agreement with the pre-surveillance data. The predominant phases identified by X-ray diffraction are in agreement with the expected phase assemblages of the as-received materials. The measured densities are in reasonable agreement with the expected densities of materials containing the fraction of salts and actinide oxide specified by the pre-surveillance data. The radiochemical results are generally in good agreement with the pre-surveillance data for mixtures containing 'weapons grade' Pu (nominally 94% {sup 239}Pu and 6% {sup 240}Pu); however, the ICP-MS results from the present investigation generally produce lower concentrations of Pu than the pre-surveillance analyses. For mixtures containing 'fuel grade' Pu (nominally 81-93% {sup 239}Pu and 7-19% {sup 240}Pu), the ICP-MS results from the present investigation appear to be in better agreement with the pre-surveillance data than the radiochemistry results.

  9. Measurements of low-level anthropogenic radionuclides from soils around Maralinga

    NASA Astrophysics Data System (ADS)

    Tims, Stephen G.; Tsifakis, Dimitrios; Srncik, Michaela; Fifield, L. Keith; Hancock, Gary J.; De Cesare, Mario

    2013-12-01

    The isotopes 239Pu and 240Pu are present in surface soils as a result of global fallout from nuclear weapons tests carried out in the 1950's and 1960's. These isotopes constitute artificial tracers of recent soil erosion and sediment movement. In practice the high throughput capabilities and high sensitivity of the AMS technique makes the study of Australia's geographically large areas viable using Pu isotopes. As part of its weapons development program the United Kingdom carried out a series of atmospheric and surface nuclear weapons tests at Maralinga, South Australia in 1956 and 1957. The contribution from the Maralinga tests to the Pu isotopic abundances present in the region around Maralinga is largely unknown. In global fallout, for example, the 240Pu/239Pu ratio is typically in the range 0.17 - 0.19, but the influence of the regional tests could lead to values outside this range. This would impact on the assessment techniques used in the soil and sediment tracer studies. We report recent measurements on soil samples collected from across the Maralinga Test site.

  10. First AID (Atom counting for Isotopic Determination).

    SciTech Connect

    Roach, J. L.; Israel, K. M.; Steiner, R. E.; Duffy, C. J.; Roench, F. R.

    2002-01-01

    Los Alamos National Laboratory (LANL) has established an in vitro bioassay monitoring program in compliance with the requirements in the Code of Federal Regulations, 10 CFR 835, Occupational Radiation Protection. One aspect of this program involves monitoring plutonium levels in at-risk workers. High-risk workers are monitored using the ultra-sensitive Therrnal Ionization Mass Spectrometry (TIMS) technique to ensure compliance with DOE standards. TIMS is used to measure atom ratios of 239Pua nd 240Puw ith respect to a tracer isotope ('Pu). These ratios are then used to calculate the amount of 239Pu and 240Pup resent. This low-level atom counting technique allows the calculation of the concentration levels of 239Pu and 240Pu in urine for at risk workers. From these concentration levels, dose assessments can be made and worker exposure levels can be monitored. Detection limits for TIMS analysis are on the order of millions of atoms, which translates to activity levels of 150 aCi 239Pua nd 500 aCi for 240Pu. pCi for Our poster presentation will discuss the ultra-sensitive, low-level analytical technique used to measure plutonium isotopes and the data verification methods used for validating isotopic measurements.

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

    NASA Astrophysics Data System (ADS)

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

    2016-08-01

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

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

    SciTech Connect

    Robert C. Roback; Don L. Koeppen

    2003-06-01

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

  13. Polonium, uranium and plutonium radionuclides in aquatic and land ecosystem of Poland.

    PubMed

    Skwarzec, Bogdan; Strumińska-Parulska, Dagmara I; Boryło, Alicja; Kabat, Krzysztof

    2012-01-01

    This article presents the results of study about distribution, inflow and accumulation of polonium, uranium and plutonium in aquatic and land environment of Poland and the southern Baltic Sea. Radionuclides of (210)Po, (234)U and (238)U as well as (239+240)Pu and (241)Pu are strongly accumulated in Baltic organisms and plants and transferred through the trophic chain. The values of bioconcentration factor (BCF) in Baltic plants and animals are higher for polonium and plutonium in comparison with uranium. The principal source of radionuclides in the southern Baltic Sea is their inflow with rivers. Total annual runoff of polonium, uranium and plutonium from the Vistula and the Odra as well as the Pomeranian rivers were calculated at 95 GBq of (210)Po, 750 GBq of (234+238)U and 160 MBq of (238+239+240)Pu. Seasonal and spatial variability of (210)Po, (238)U and (239+240)Pu levels in the Vistula and the Odra drainage basins were assessed by application of neural-network based classification, especially cluster analysis (CA), principal component analysis (PCA) and self-organizing maps (SOM). The result for the Vistula river indicated correlation between polonium and plutonium as well as polonium and uranium. In the Odra drainage basin, the biggest differences were observed in the case of (238)U. To assess if there are statistically significant differences in mean concentration values of (210)Po, (238)U and (239+240)Pu for the Vistula and the Odra rivers drainage basins were obtained by used of the non-parametric tests. Comparing to the Vistula catchment area, statistically differences concentration of (210)Po and (239+240)Pu in all year was observed for river samples collected on the Odra drainage basin.

  14. Plutonium gamma-ray measurements for mutual reciprocal inspections of dismantled nuclear weapons

    SciTech Connect

    Koenig, Z.M.; Carlson, J.B.; Clark, D.; Gosnell, T.B.

    1995-07-01

    The O`Leary-Mikhailov agreement of March 1994 stated that the U.S. and the Russian Federation would engage in mutual reciprocal inspections (MRI) of fissile materials removed from dismantled nuclear weapons. It was decided to begin with the plutonium (Pu) removed from dismantled weapons and held in storage containers. Later discussions between U.S. and Russian technical experts led to the conclusion that, to achieve the O`Leary-Mikhailov objectives, Pu MRI would need to determine that the material in the containers has properties consistent with a nuclear-weapon component. Such a property is a {sup 240}Pu/{sup 239}Pu ratio consistent with weapons-grade material. One of the candidate inspection techniques under consideration for Pu MRI is to use a narrow region (630-670 keV) of the plutonium gamma-ray spectrum, taken with a high-purity germanium detector, to determine that it is weapons-grade plutonium as well as to estimate the minimum mass necessary to produce the observed gamma-ray intensity. We developed software (the Pu600 code) for instrument control and analysis especially for this purpose. In November 1994, U.S. and Russian scientists met at the Lawrence Livermore National Laboratory for joint experiments to evaluate candidate Pu MRI inspection techniques. In one of these experiments, gamma-ray intensities were measured from three unclassified weapons-grade plutonium source standards and one reactor-grade standard (21% {sup 240}pu). Using our software, we determined the {sup 240}Pu/{sup 239}Pu ratio of these standards to accuracies within {+-}10%, which is adequate for Pu MRI. The minimum mass estimates varied, as expected, directly with the exposed surface area of the standards.

  15. CALORIMETER-BASED ADJUSTMENT OF MULTIPLICITY DETERMINED 240PU EFF KNOWN-A ANALYSIS FOR THE ASSAY OF PLUTONIUM

    SciTech Connect

    Dubose, F.

    2012-02-21

    In nuclear material processing facilities, it is often necessary to balance the competing demands of accuracy and throughput. While passive neutron multiplicity counting is the preferred method for relatively fast assays of plutonium, the presence of low-Z impurities (fluorine, beryllium, etc.) rapidly erodes the assay precision of passive neutron counting techniques, frequently resulting in unacceptably large total measurement uncertainties. Conversely, while calorimeters are immune to these impurity effects, the long count times required for high accuracy can be a hindrance to efficiency. The higher uncertainties in passive neutron measurements of impure material are driven by the resulting large (>>2) {alpha}-values, defined as the ({alpha},n):spontaneous fission neutron emission ratio. To counter impurity impacts for high-{alpha} materials, a known-{alpha} approach may be adopted. In this method, {alpha} is determined for a single item using a combination of gamma-ray and calorimetric measurements. Because calorimetry is based on heat output, rather than a statistical distribution of emitted neutrons, an {alpha}-value determined in this way is far more accurate than one determined from passive neutron counts. This fixed {alpha} value can be used in conventional multiplicity analysis for any plutonium-bearing item having the same chemical composition and isotopic distribution as the original. With the results of single calorimeter/passive neutron/gamma-ray measurement, these subsequent items can then be assayed with high precision and accuracy in a relatively short time, despite the presence of impurities. A calorimeter-based known-{alpha} multiplicity analysis technique is especially useful when requiring rapid, high accuracy, high precision measurements of multiple plutonium bearing items having a common source. The technique has therefore found numerous applications at the Savannah River Site. In each case, a plutonium (or mixed U/Pu) bearing item is divided into multiple containers. A single item from that batch is then selected for both neutron and calorimetric measurements; all remaining items undergo a neutron measurement only. Using the technique mentioned above, the 'true' {alpha} value determined from the first (calorimeter and passive neutron measured) item is used in multiplicity analysis for all other items in the batch. The justification for using this {alpha} value in subsequent calculations is the assumption that the chemical composition and isotopic distribution of all batch items are the same, giving a constant ({alpha},n):spontaneous fission ratio. This analysis method has been successfully applied to the KIS Facility, significantly improving measurement uncertainties and reducing processing times for numerous items. Comprehensive plans were later developed to extend the use of this method to other applications, including the K-Area Shuffler and the H-Area Pu-Blending Project. While only the feasibility study for the Shuffler has been completed, implementation of the method in the H-Area Pu-Blending Project is currently in progress and has been successfully applied to multiple items. This report serves to document the details of this method in order to serve as a reference for future applications. Also contained herein are specific examples of the application of known-{alpha} multiplicity analysis.

  16. Concordant plutonium-241-americium-241 dating of environmental samples: results from forest fire ash

    SciTech Connect

    Goldstein, Steven J; Oldham, Warren J; Murrell, Michael T; Katzman, Danny

    2010-12-07

    We have measured the Pu, {sup 237}Np, {sup 241}Am, and {sup 151}Sm isotopic systematics for a set of forest fire ash samples from various locations in the western U.S. including Montana, Wyoming, Idaho, and New Mexico. The goal of this study is to develop a concordant {sup 241}Pu (t{sub 1/2} = 14.4 y)-{sup 241}Am dating method for environmental collections. Environmental samples often contain mixtures of components including global fallout. There are a number of approaches for subtracting the global fallout component for such samples. One approach is to use {sup 242}/{sup 239}Pu as a normalizing isotope ratio in a three-isotope plot, where this ratio for the nonglobal fallout component can be estimated or assumed to be small. This study investigates a new, complementary method of normalization using the long-lived fission product, {sup 151}Sm (t{sub 1/2} = 90 y). We find that forest fire ash concentrates actinides and fission products with {approx}1E10 atoms {sup 239}Pu/g and {approx}1E8 atoms {sup 151}Sm/g, allowing us to measure these nuclides by mass spectrometric (MIC-TIMS) and radiometric (liquid scintillation counting) methods. The forest fire ash samples are characterized by a western U.S. regional isotopic signature representing varying mixtures of global fallout with a local component from atmospheric testing of nuclear weapons at the Nevada Test Site (NTS). Our results also show that {sup 151}Sm is well correlated with the Pu nuclides in the forest fire ash, suggesting that these nuclides have similar geochemical behavior in the environment. Results of this correlation indicate that the {sup 151}Sm/{sup 239}Pu atom ratio for global fallout is {approx}0.164, in agreement with an independent estimate of 0.165 based on {sup 137}Cs fission yields for atmospheric weapons tests at the NTS. {sup 241}Pu-{sup 241}Am dating of the non-global fallout component in the forest fire ash samples yield ages in the late 1950's-early 1960's, consistent with a peak in NTS

  17. Evidence for the Remobilization of Sellafield Waste Radionuclides in an Intertidal Salt Marsh, West Cumbria, U.K.

    NASA Astrophysics Data System (ADS)

    Morris, K.; Butterworth, J. C.; Livens, F. R.

    2000-11-01

    Intertidal sediments in north-west England contain enhanced levels of artificial radionuclides due to the authorized release of low-level liquid waste from the Sellafield reprocessing site. In this paper, the behaviour of 99Tc, 137Cs, 237Np, 238Pu, 239Pu, 240Pu, 239+240Pu and 241Am in an intertidal marsh sediment is described. The radionuclide data, together with stable element data, allow detailed interpretation of the behaviour of these artificial radionuclides in a natural environment. For 241Am and 239+240Pu, for which the Sellafield discharge history is well known, the distributions down the sediment core show a high correlation with the Sellafield discharge history. The sediment profiles for other less widely studied radionuclides, 99Tc and 237Np, have been examined in relation to both the post-1978 published discharge histories and the behaviour of other Sellafield-derived radionuclides in the core. There is strong evidence that significant post-depositional remobilization of a proportion of the most labile elements, 237Np, 137Cs and 99Tc, is occurring at the marsh.

  18. Comparison of Pu and (137)Cs as tracers of soil and sediment transport in a terrestrial environment.

    PubMed

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

    2008-02-01

    Following atmospheric nuclear weapons testing in the 1950s and 1960s significant quantities of (137)Cs and (239+240)Pu were deposited worldwide. In recent decades, (137)Cs has been commonly used as a tracer of soil erosion and sedimentation, particularly in the Northern Hemisphere where atomic deposition was three times as great as in the Southern Hemisphere. The relatively short 30-year half-life of this isotope means that its sensitivity as a tracer is rapidly decreasing. In contrast, with half-lives of 24,110 and 6561 years, the sensitivity of the two plutonium isotopes remains essentially the same as when it was deposited. Here we use the technique of Accelerator Mass Spectrometry to demonstrate the potential of anthropogenic Pu as an alternative to (137)Cs as a tracer of soil transport in Australia. We measure an average (137)Cs/(239+240)Pu activity ratio of 27.3+/-1.5 and an average (240)Pu/(239)Pu atom ratio of 0.149+/-0.003, both slightly lower than the global average.

  19. Uranium comparison by means of AMS and ICP-MS and Pu and 137Cs results around an Italian Nuclear Power Plant

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

    Italy built and commissioned 4 nuclear power plants between 1958-1978, which delivered a total of 1500 MW. All four were closed down after the Chernobyl accident following a referendum in 1987. One of the plants was Garigliano, commissioned in 1959. This plant used a 160 MW BWR1 (SEU of 2.3 %) and was operational from 1964 to 1979, when it was switched off for maintenance. It was definitively stopped in 1982, and is presently being decommissioned. We report here details on the chemistry procedure and on the measurements for soil samples, collected up to 4.5 km from the Nuclear Plant. A comparison between uranium (238U) concentration as determined by means of AMS (Accelerator Mass Spectrometry) and by ICP-MS (Inductively Coupled Plasma-Mass Spectrometry) techniques respectively at the ANU (Australian National University) and at the Ecowise company in Canberra, Australia, is reported, as well as 236U and 239;240Pu concentration results detected by AMS. 236U/238U and 240Pu/239Pu isotopic ratios by means of AMS are also provided. A contamination from Chernobyl is visible in the 137Cs/239+240Pu activity ratio measurements.

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

    PubMed

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

    2011-03-01

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

  1. A compact gas-filled avalanche counter for DANCE

    NASA Astrophysics Data System (ADS)

    Wu, C. Y.; Chyzh, A.; Kwan, E.; Henderson, R. A.; Gostic, J. M.; Carter, D.; Bredeweg, T. A.; Couture, A.; Jandel, M.; Ullmann, J. L.

    2012-12-01

    A compact gas-filled avalanche counter for the detection of fission fragments was developed for a highly segmented 4π γ-ray calorimeter, namely the Detector for Advanced Neutron Capture Experiments located at the Lujan Center of the Los Alamos Neutron Science Center. It has been used successfully for experiments with 235U, 238Pu, 239Pu, and 241Pu isotopes to provide a unique signature to differentiate the fission from the competing neutron-capture reaction channel. It was also used to study the spontaneous fission in 252Cf. The design and performance of this avalanche counter for targets with extreme α-decay rate up to ˜2.4×108/s are described.

  2. Application of Neutron-Absorbing Structural-Amorphous Metal (SAM) Coatings for Spent Nuclear Fuel (SNF) Container to Enhance Criticality Safety Controls

    SciTech Connect

    Choi, Jor-Shan; Lee, Chuck; Farmer, Joseph; Day, Dan; Wall, Mark; Saw, Cheng; Boussoufi, Moe; Liu, Ben; Egbert, Harold; Branagan, Dan; D'Amato, Andy

    2007-07-01

    Spent nuclear fuel contains fissionable materials ({sup 235}U, {sup 239}Pu, {sup 241}Pu, etc.). To prevent nuclear criticality in spent fuel storage, transportation, and during disposal, neutron-absorbing materials (or neutron poisons, such as borated stainless steel, Boral{sup TM}, Metamic{sup TM}, Ni-Gd, and others) would have to be applied. The success in demonstrating that the High-Performance Corrosion- Resistant Material (HPCRM){sup [1]} can be thermally applied as coating onto base metal to provide for corrosion resistance for many naval applications raises the interest in applying the HPCRM to USDOE/OCRWM spent fuel management program. The fact that the HPCRM relies on the high content of boron to make the material amorphous - an essential property for corrosion resistance - and that the boron has to be homogeneously distributed in the HPCRM qualify the material to be a neutron poison. (authors)

  3. Spectrum tailoring of the neutron energy spectrum in the context of delayed neutron detection

    SciTech Connect

    Koehler, William E; Tobin, Steve J; Sandoval, Nathan P; Fensin, Mike L

    2010-01-01

    For the purpose of measuring plutonium mass in spent fuel, a delayed neutron instrument is of particular interest since, if properly designed, the delayed neutron signal from {sup 235}U is significantly stronger than the signature from {sup 239}Pu or {sup 241}Pu. A key factor in properly designing a delayed neutron instrument is to minimize the fission of {sup 238}U. This minimization is achieved by keeping the interrogating neutron spectrum below {approx} 1 MeV. In the context of spent fuel measurements it is desirable to use a 14 MeV (deuterium and tritium) neutron generator for economic reasons. Spectrum tailoring is the term used to describe the inclusion of material between the 14 MeV neutrons and the interrogated object that lower the neutron energy through nuclear reactions and moderation. This report quantifies the utility of different material combination for spectrum tailoring.

  4. A compact gas-filled avalanche counter for DANCE

    DOE PAGES

    Wu, C. Y.; Chyzh, A.; Kwan, E.; Henderson, R. A.; Gostic, J. M.; Carter, D.; Bredeweg, T. A.; Couture, A.; Jandel, M.; Ullmann, J. L.

    2012-08-04

    A compact gas-filled avalanche counter for the detection of fission fragments was developed for a highly segmented 4π γ-ray calorimeter, namely the Detector for Advanced Neutron Capture Experiments located at the Lujan Center of the Los Alamos Neutron Science Center. It has been used successfully for experiments with 235U, 238Pu,239Pu, and 241Pu isotopes to provide a unique signature to differentiate the fission from the competing neutron-capture reaction channel. We also used it to study the spontaneous fission in 252Cf. The design and performance of this avalanche counter for targets with extreme α-decay rate up to ~2.4×108/s are described.

  5. Analysis of spent fuel assay with a lead slowing down spectrometer

    SciTech Connect

    Gavron, Victor I; Smith, L. Eric; Ressler, Jennifer J

    2010-10-29

    Assay of fissile materials in spent fuel that are produced or depleted during the operation of a reactor, is of paramount importance to nuclear materials accounting, verification of the reactor operation history, as well as for criticality considerations for storage. In order to prevent future proliferation following the spread of nuclear energy, we must develop accurate methods to assay large quantities of nuclear fuels. We analyze the potential of using a Lead Slowing Down Spectrometer for assaying spent fuel. We conclude that it is possible to design a system that will provide around 1% statistical precision in the determination of the {sup 239}Pu, {sup 241}Pu and {sup 235}U concentrations in a PWR spent-fuel assembly, for intermediate-to-high burnup levels, using commercial neutron sources, and a system of {sup 238}U threshold fission detectors. Pending further analysis of systematic errors, it is possible that missing pins can be detected, as can asymmetry in the fuel bundle.

  6. Analysis of spent fuel assay with a lead slowing down spectrometer

    SciTech Connect

    Gavron, Victor I; Smith, L Eric; Ressler, Jennifer J

    2008-01-01

    Assay of fissile materials in spent fuel that are produced or depleted during the operation of a reactor, is of paramount importance to nuclear materials accounting, verification of the reactor operation history, as well as for criticality considerations for storage. In order to prevent future proliferation following the spread of nuclear energy, we must develop accurate methods to assay large quantities of nuclear fuels. We analyze the potential of using a Lead Slowing Down Spectrometer for assaying spent fuel. We conclude that it is possible to design a system that will provide around 1% statistical precision in the determination of the {sup 239}Pu, {sup 241}Pu and {sup 235}U concentrations in a PWR spent-fuel assembly, for intermediate-to-high burnup levels, using commercial neutron sources, and a system of {sup 238}U threshold fission detectors. Pending further analysis of systematic errors, it is possible that missing pins can be detected, as can asymmetry in the fuel bundle.

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

    PubMed

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

    2015-04-01

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

  8. Improved predictions of reactor antineutrino spectra

    SciTech Connect

    Mueller, Th. A.; Lhuillier, D.; Letourneau, A.

    2011-05-15

    Precise predictions of the antineutrino spectra emitted by nuclear reactors is a key ingredient in measurements of reactor neutrino oscillations as well as in recent applications to the surveillance of power plants in the context of nonproliferation of nuclear weapons. We report new calculations including the latest information from nuclear databases and a detailed error budget. The first part of this work is the so-called ab initio approach where the total antineutrino spectrum is built from the sum of all {beta} branches of all fission products predicted by an evolution code. Systematic effects and missing information in nuclear databases lead to final relative uncertainties in the 10-20% range. A prediction of the antineutrino spectrum associated with the fission of {sup 238}U is given based on this ab initio method. For the dominant isotopes we developed a more accurate approach combining information from nuclear databases and reference electron spectra associated with the fission of {sup 235}U, {sup 239}Pu, and {sup 241}Pu, measured at Institut Laue-Langevin (ILL) in the 1980s. We show how the anchor point of the measured total {beta} spectra can be used to suppress the uncertainty in nuclear databases while taking advantage of all the information they contain. We provide new reference antineutrino spectra for {sup 235}U, {sup 239}Pu, and {sup 241}Pu isotopes in the 2-8 MeV range. While the shapes of the spectra and their uncertainties are comparable to those of the previous analysis of the ILL data, the normalization is shifted by about +3% on average. In the perspective of the reanalysis of past experiments and direct use of these results by upcoming oscillation experiments, we discuss the various sources of errors and their correlations as well as the corrections induced by off-equilibrium effects.

  9. 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.

  10. New antineutrino energy spectra predictions from the summation of beta decay branches of the fission products.

    PubMed

    Fallot, M; Cormon, S; Estienne, M; Algora, A; Bui, V M; Cucoanes, A; Elnimr, M; Giot, L; Jordan, D; Martino, J; Onillon, A; Porta, A; Pronost, G; Remoto, A; Taín, J L; Yermia, F; Zakari-Issoufou, A-A

    2012-11-16

    In this Letter, we study the impact of the inclusion of the recently measured beta decay properties of the (102;104;105;106;107)Tc, (105)Mo, and (101)Nb nuclei in an updated calculation of the antineutrino energy spectra of the four fissible isotopes (235,238)U and (239,241)Pu. These actinides are the main contributors to the fission processes in pressurized water reactors. The beta feeding probabilities of the above-mentioned Tc, Mo, and Nb isotopes have been found to play a major role in the γ component of the decay heat of (239)Pu, solving a large part of the γ discrepancy in the 4-3000 s range. They have been measured by using the total absorption technique, insensitive to the pandemonium effect. The calculations are performed by using the information available nowadays in the nuclear databases, summing all the contributions of the beta decay branches of the fission products. Our results provide a new prediction of the antineutrino energy spectra of (235)U, (239,241)Pu, and, in particular, (238)U for which no measurement has been published yet. We conclude that new total absorption technique measurements are mandatory to improve the reliability of the predicted spectra. PMID:23215477

  11. New antineutrino energy spectra predictions from the summation of beta decay branches of the fission products.

    PubMed

    Fallot, M; Cormon, S; Estienne, M; Algora, A; Bui, V M; Cucoanes, A; Elnimr, M; Giot, L; Jordan, D; Martino, J; Onillon, A; Porta, A; Pronost, G; Remoto, A; Taín, J L; Yermia, F; Zakari-Issoufou, A-A

    2012-11-16

    In this Letter, we study the impact of the inclusion of the recently measured beta decay properties of the (102;104;105;106;107)Tc, (105)Mo, and (101)Nb nuclei in an updated calculation of the antineutrino energy spectra of the four fissible isotopes (235,238)U and (239,241)Pu. These actinides are the main contributors to the fission processes in pressurized water reactors. The beta feeding probabilities of the above-mentioned Tc, Mo, and Nb isotopes have been found to play a major role in the γ component of the decay heat of (239)Pu, solving a large part of the γ discrepancy in the 4-3000 s range. They have been measured by using the total absorption technique, insensitive to the pandemonium effect. The calculations are performed by using the information available nowadays in the nuclear databases, summing all the contributions of the beta decay branches of the fission products. Our results provide a new prediction of the antineutrino energy spectra of (235)U, (239,241)Pu, and, in particular, (238)U for which no measurement has been published yet. We conclude that new total absorption technique measurements are mandatory to improve the reliability of the predicted spectra.

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

    SciTech Connect

    Kaplan, D.; Buesseler, K.

    2010-06-29

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

  13. Even-odd effects in prompt emission of spontaneously fissioning even-even Pu isotopes

    NASA Astrophysics Data System (ADS)

    Tudora, A.; Hambsch, F.-J.; Giubega, G.; Visan, I.

    2015-01-01

    The available experimental Y (A , TKE) data for 236,238,240,242,244Pu(SF) together with the Zp model prescription with appropriate parameters allows the investigation of even-odd effects in fragment distributions. The size of the global even-odd effect in Y (Z) is decreasing from 244Pu(SF) to 236Pu(SF) confirming the general observation of a decrease of the even-odd effect with the fissility parameter. Charge polarizations (ΔZ) and root-mean squares (rms) as a function of A of 236-244Pu(SF) were obtained for the first time. In the asymmetric fission region both ΔZ (A) and rms (A) exhibit oscillations with a periodicity of about 5 mass units due to the even-odd effects. The total average charge deviations < ΔZ > (obtained by averaging ΔZ (A) over the experimental Y (A) distribution) are of about |0.5| for all studied Pu(SF) systems. The comparison of the calculated ΔZ (A) and rms (A) of 240Pu(SF) with those of 239Pu (nth , f) reported by Wahl shows an in-phase oscillation with a higher amplitude in the case of 240Pu(SF), confirming the higher even-odd effect in the case of SF. As in the previously studied cases (233,235U (nth , f), 239Pu (nth , f), 252Cf(SF)) the even-odd effects in the prompt emission of 236-244Pu(SF) are mainly due to the Z even-odd effects in fragment distributions and charge polarizations and the N even-odd effects in the average neutron separation energies from fragments < Sn >. The size of the global N even-odd effect in < Sn > is decreasing with the fissility parameter, being higher for the Pu(SF) systems compared to the previously studied systems. The prompt neutron multiplicities as a function of Z, ν (Z), exhibit sawtooth shapes with a visible staggering for asymmetric fragmentations. The size of the global Z even-odd effect in ν (Z) exhibits a decreasing trend with increasing fissility. The average prompt neutron multiplicities as a function of TKE show an increase of the even-odd effect with increasing TKE, with global effect

  14. Concepts for Alpha Coincidence Detection

    SciTech Connect

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

    2015-03-01

    The effectiveness of conventional measurement techniques for environmental monitoring is limited by background and other interferences. We are exploring a new measurement approach involving the detection of α particles in coincidence with conversion electrons as a means to simultaneously assay environmental samples for actinides without chemical separation. The initial target isotopes studied in this work are 238Pu, 239Pu, 240Pu and 241Am. We explore various aspects of the design, such as impact of the mounting of the source material, resolution requirements and impact of a background on isotopic uncertainties. We conclude that a dual gas proportional counter and a dual-sided, large-area silicon detector could provide similar performance for the measurement scenario examined.

  15. Neutron capture by fissile and fertile actinide targets

    SciTech Connect

    Maslov, Vladimir M.

    2009-01-28

    For fissile actinide targets {sup 233}U, {sup 235}U and {sup 239}Pu the capture cross sections are strongly influenced by the target spin, fission transition states spectroscopy and fission/{gamma}-emission competition of the compound nuclides. The capture cross sections were obtained via a consistent description of fission and elastic/inelastic scattering, (n,{gamma}f) reaction being included.For neutron capture reactions on even-even U, Pu and Cm nuclei the methods, proven in case of {sup 232}Th(n,{gamma}) and {sup 238}U(n,{gamma}) data analysis are used. Calculated {sup 240}Pu(n,{gamma}) and {sup 244}Cm(n,{gamma}) reaction cross sections shapes are much similar to that, observed for the {sup 238}U(n,{gamma}) and {sup 232}Th(n,{gamma}) reactions. Differences are due to fission and neutron emission competition, which depends on the (Z,N)-composition of the compound nucleus.

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

    PubMed

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

    1984-09-01

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

  17. Advanced alpha spectrum analysis based on the fitting and covariance analysis of dependent variables

    NASA Astrophysics Data System (ADS)

    Ihantola, S.; Pelikan, A.; Pöllänen, R.; Toivonen, H.

    2011-11-01

    The correct handling of statistical uncertainties is crucial especially when unfolding alpha spectra that contain a low number of counts or overlapping peaks from different nuclides. For this purpose, we have developed a new spectrum analysis software package called ADAM, which performs a full covariance calculus for alpha-particle emitting radionuclides. By analyzing a large number of simulated and measured spectra, the program was proved to give unbiased peak areas and statistically correct uncertainty limits. This applies regardless of the peak areas and the number of unknown parameters during the fitting. In addition, ADAM performs reliable deconvolution for multiplets, which opens the way for the determination of isotope ratios, such as 239Pu/240Pu.

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

    DOE PAGES

    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

  19. [Dosage of irradiation of the population in the Bryansk region with plutonium deposited in the soil after the Chernobyl AES accident].

    PubMed

    Ivanova, N P; Shvydko, N S

    1991-01-01

    Proceeding from the data on 238Pu, 239Pu, 240Pu concentrations in the soil in different areas of the Bryansk Region, exposed to radioactive contamination after the Chernobyl accident, radiation dose exposures of residents as well as agricultural workers were assessed. Criteria of the ecological and radiation-hygienic standardization were used for calculation of values of dose factors, binding the alimentary and inhalation components of an irradiation dose with characteristics of Pu deposition in the soil. Inhalation of soil particles accounted for approximately 90% of a total radiation dose of the "soil" Pu component, and the alimentary component-for approximately 10% (of this, 99% were attributed to plant products). The authors proposed prognostic assessment of an expected effective equivalent dose for a period of 70 years for people, residing in these areas (0.08-0.45 cSi for the population and 0.6-3.2 cSi for mechanics).

  20. Migration rates of radionuclides deposited after the Chernobyl accident in various North German soils.

    PubMed

    Kirchner, G; Baumgartner, D

    1992-03-01

    In three soils typical for Northern Germany including Eutric Cambisol, Orthic Podsol and Eutric Histosol (Food and Agriculture Organization nomenclature), distributions of 90Sr, 134Cs, 137Cs and 239Pu + 240Pu in the soil profiles were determined. Sampling was performed more than 3 years after deposition of Chernobyl fallout nuclides. Migration rates calculated with a compartmental model showed no significant differences between Cs originating from either atomic weapons or Chernobyl fallout. This result indicates that Chernobyl Cs may have reached sorption equilibrium with the soil matrix 3 years after the accident. Both the compartmental model and the dispersion equation reproduce distributions of most of the activities, but fail to reproduce some (minor) activity fractions that show increased mobility.

  1. Radiochemical Separations for the Pretreatment of High Level Nuclear Wastes at the Savannah River Site

    SciTech Connect

    Hobbs, D.T.

    2003-09-03

    A significant fraction of the high-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) must be pretreated to remove 137Cs, 90Sr and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. Separation processes planned at the SRS include caustic side solvent extraction for 137Cs and sorption onto monosodium titanate (MST) for 90Sr and alpha-emitters. The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes 238Pu, 239Pu and 240Pu. This paper describes the planned Sr/actinide separation process and summarizes recent tests and demonstrations with simulated and actual tank waste solutions.

  2. DEVELOPMENT OF AN IMPROVED SODIUM TITANATE FOR THE PRETREATMENT OF HIGH LEVEL NUCLEAR WASTE AT THE SAVANNAH RIVER SITE

    SciTech Connect

    Hobbs D. T.; Poirier, M. R.; Barnes, M. J.; Stallings, M. E.; Nyman, M. D.

    2005-11-22

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 137}Cs, {sup 90}Sr and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. Separation processes planned at SRS include caustic side solvent extraction, for {sup 137}Cs removal, and sorption of {sup 90}Sr and alpha-emitting radionuclides onto monosodium titanate (MST). The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes {sup 238}Pu, {sup 239}Pu and {sup 240}Pu. This paper describes recent results to produce an improved sodium titanate material that exhibits increased removal kinetics and capacity for {sup 90}Sr and alpha-emitting radionuclides compared to the baseline MST material.

  3. Multi-collector Isotope Ratio Mass Spectrometer -- Operational Performance Report

    SciTech Connect

    Appelhans, Anthony D; Olson, John E; Watrous, Matthew G; Ward, Michael B.; Dahl, David A.

    2010-12-01

    This report describes the operational testing of a new magnetic sector mass spectrometer that utilizes seven full-sized discrete dynode electron multipliers operating simultaneously. The instrument includes a newly developed ion dispersion lens that enables the mass dispersed individual isotope beams to be separated sufficiently to allow a full-sized discrete dynode pulse counting multiplier to be used to measure each isotope beam. The performance of the instrument was measured using SRM 996 (244Pu spike) at loadings of 2.4 and 12 fg on resin beads and with SRM 4350B Columbia River Sediment samples. The measured limit of detection (3s) for 240Pu was 3.4 attograms for SRM 996. The limit of quantitation (LOQ), defined as 10 s, was 11.2 attograms. The measured concentration of 239Pu in the CRS standard was 152 ± 6 fg/g.

  4. Applications of Event-by-Event Fission Modeling with FREYA

    SciTech Connect

    Vogt, R; Randrup, J

    2011-09-16

    The recently developed code FREYA (Fission Reaction Event Yield Algorithm) generates large samples of complete fission events, consisting of two receding product nuclei as well as a number of neutrons and photons, all with complete kinematic information. Thus it is possible to calculate arbitrary correlation observables whose behavior may provide unique insight into the fission process. We first discuss the present status of FREYA, which has now been extended to include spontaneous fission. Concentrating on {sup 239}Pu(n{sub th},f), {sup 240}Pu(sf) and {sup 252}Cf(sf), we discuss the neutron multiplicity correlations, the dependence of the neutron energy spectrum on the neutron multiplicity, and the relationship between the fragment kinetic energy and the number of neutrons and their energies. We also suggest novel fission observables that could be measured with modern detectors.

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

    SciTech Connect

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

    2005-05-24

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

  6. Atmospheric transport of radionuclides emitted due to wildfires near the Chernobyl Nuclear Power Plant in 2015

    NASA Astrophysics Data System (ADS)

    Evangeliou, Nikolaos; Zibtsev, Sergey; Myroniuk, Viktor; Zhurba, Marina; Hamburger, Thomas; Stohl, Andreas; Balkanski, Yves; Paugam, Ronan; Mousseau, Timothy A.; Møller, Anders P.; Kireev, Sergey I.

    2016-04-01

    In 2015, two major fires in the Chernobyl Exclusion Zone (CEZ) have caused concerns about the secondary radioactive contamination that might have spread over Europe. The total active burned area was estimated to be about 15,000 hectares, of which 9000 hectares burned in April and 6000 hectares in August. The present paper aims to assess, for the first time, the transport and impact of these fires over Europe. For this reason, direct observations of the prevailing deposition levels of 137Cs and 90Sr, 238Pu, 239Pu, 240Pu and 241Am in the CEZ were processed together with burned area estimates. Based on literature reports, we made the conservative assumption that 20% of the deposited labile radionuclides 137Cs and 90Sr, and 10% of the more refractory 238Pu, 239Pu, 240Pu and 241Am, were resuspended by the fires. We estimate that about 10.9 TBq of 137Cs, 1.5 TBq of 90Sr, 7.8 GBq of 238Pu, 6.3 GBq of 239Pu, 9.4 GBq of 240Pu and 29.7 GBq of 241Am were released from both fire events. These releases could be classified as of "Level 3" on the relative INES (International Nuclear Events Scale) scale, which corresponds to a serious incident, in which non-lethal deterministic effects are expected from radiation. To simulate the dispersion of the resuspended radionuclides in the atmosphere and their deposition onto the terrestrial environment, we used a Lagrangian dispersion model. Spring fires redistributed radionuclides over the northern and eastern parts of Europe, while the summer fires also affected Central and Southern Europe. The more labile elements escaped more easily from the CEZ and then reached and deposited in areas far from the source, whereas the larger refractory particles were removed more efficiently from the atmosphere and thus did mainly affect the CEZ and its vicinity. For the spring 2015 fires, we estimate that about 80% of 137Cs and 90Sr and about 69% of 238Pu, 239Pu, 240Pu and 241Am were deposited over areas outside the CEZ. 93% of the labile and 97% of

  7. LITERATURE REVIEW ON MAXIMUM LOADING OF RADIONUCLIDES ON CRYSTALLINE SILICOTITANATE

    SciTech Connect

    Adu-Wusu, K.; Pennebaker, F.

    2010-10-13

    Plans are underway to use small column ion exchange (SCIX) units installed in high-level waste tanks to remove Cs-137 from highly alkaline salt solutions at Savannah River Site. The ion exchange material slated for the SCIX project is engineered or granular crystalline silicotitanate (CST). Information on the maximum loading of radionuclides on CST is needed by Savannah River Remediation for safety evaluations. A literature review has been conducted that culminated in the estimation of the maximum loading of all but one of the radionuclides of interest (Cs-137, Sr-90, Ba-137m, Pu-238, Pu-239, Pu-240, Pu-241, Am-241, and Cm-244). No data was found for Cm-244.

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

    NASA Astrophysics Data System (ADS)

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

    2005-05-01

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

  9. Recent advances in modeling fission cross sections over intermediate structures

    SciTech Connect

    Bouland, Olivier; Lynn, J. Eric; Talou, Patrick

    2009-01-01

    More accurate fission cross section calculations in presence of underlying intermediate structure are strongly desired. This paper recalls the common approximations used below the fission threshold and quantifies their impact. In particular, an exact expanded R-matrix Monte Carlo calculation of the intermediate structure, deeply mixed with the fluctuations of the class-I and II decay amplitudes, is shown. This paper also insists on the microscopic structure of the level densities as a function of the nucleus deformation and show preliminary neutron induced fission cross section calculations for {sup 239}Pu and {sup 240}Pu using newly calculated combinatorial level densities. Comparisons with recent evaluated and measured fission cross sections are made.

  10. Distribution of sup 137 Cs, sup 90 Sr, sup 238 Pu, sup 239 Pu, sup 241 Am and sup 244 Cm in Pond B, Savannah River Site

    SciTech Connect

    Whicker, F.W. ); Pinder, J.E. III; Bowling, J.W. ); Alberts, J.J. . Marine Inst.); Brisbin, I.L. Jr. )

    1989-05-01

    The gradual senescence of present-day operating nuclear facilities, and resultant contamination of aquatic and terrestrial ecosystems, emphasize the importance of understanding the behavior of radionuclides in the environment. Observations and deductions concerning mechanisms of radionuclide transport can contribute significantly to knowledge of fundamental ecological processes. This study emphasized the ecosystem-level distribution of several long-lived radionuclides in an abandoned reactor cooling impoundment after a twenty year period of chemical and biological equilibration. 90 refs., 14 figs., 5 tabs.

  11. Monte Carlo simulation of transfer reactions using extended R-matrix theory picturing surrogate-type WFCF features

    NASA Astrophysics Data System (ADS)

    Bouland, Olivier H.

    2016-03-01

    This article supplies an overview of issues related to the interpretation of surrogate measurement results for neutron-incident cross section predictions; difficulties that are somehow masked by the historical conversion route based on Weisskopf-Ewing approximation. Our proposal is to handle the various difficulties by using a more rigorous approach relying on Monte Carlo simulation of transfer reactions with extended R-matrix theory. The multiple deficiencies of the historical surrogate treatment are recalled but only one is examined in some details here; meaning the calculation of in-out-going channel Width Fluctuation Correction Factors (WFCF) which behavior witness partly the failure of Niels Bohr's compound nucleus theoretical landmark. Relevant WFCF calculations according to neutron-induced surrogate- and cross section-types as a function of neutron-induced fluctuating energy range [0 - 2.1 MeV] are presented and commented in the case of the 240Pu* and 241Pu* compound nucleus isotopes.

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

    PubMed

    Higgy, R H; Pimpl, M

    1998-12-01

    The specific radioactivities of the U-series, 232Th, 137Cs and 40K were measured in soil samples around the Inshass reactor in Cairo, using a gamma-ray spectrometer with a HpGe detector. The alpha activity of 238U, 234U and 235U was measured in the same soil samples by surface barrier detectors after radiochemical separation and the obtained results were compared with the specific activities determined by gamma-measurements. The alpha-activity of 238Pu, 239+240Pu, 241Am, 242Cm and 244Cm was measured after radiochemical separation by surface barrier detectors for both soil and plant samples. Then beta-activity of 241Pu was measured using liquid scintillation spectrometry. PMID:9776618

  13. Isotopic fingerprinting of the world's first nuclear device using post-detonation materials.

    PubMed

    Bellucci, Jeremy J; Simonetti, Antonio; Wallace, Christine; Koeman, Elizabeth C; Burns, Peter C

    2013-04-16

    In the event of a rogue nuclear attack or interception of illicit nuclear materials, timely forensic investigations are critical for accurate source attribution. Uranium (U) and plutonium (Pu) isotopic ratios of intercepted materials or postdetonation samples are, perhaps, the most valuable evidence in modern nuclear forensics. These ratios simultaneously provide information regarding the material's ''age'' (i.e., time elapsed since last purification), actinide concentrations, and relevant isotopic ratios/enrichment values. Consequently, these isotope signatures are invaluable in determining the origin, processing history, and intended purpose of any nuclear material. Here we show, for the first time, that it is feasible to determine the U and Pu isotopic compositions of historic nuclear devices from their postdetonation materials utilizing in situ U isotopic measurements. The U isotopic compositions of trinitite glass, produced subsequent to the world's first atomic explosion, indicate two sources: the device's tamper, composed of natural U that underwent fission during detonation, and natural U from the geological background. Enrichments in (234,235,236)U reflect the in situ decay of (238,239,240)Pu, the fuel used in the device. Time-integrated U isotopic modeling yields "supergrade" compositions, where (240)Pu/(239)Pu ≈ 0.01-0.03 and (238)Pu/(239)Pu ≈ 0.00011-0.00017, which are consistent with the Pu originating from the Hanford reactor. Spatially resolved U isotopic data of postdetonation debris reveal important details of the device in a relatively short time frame (hours). This capacity serves as an important deterrent to future nuclear threats and/or terrorist activities and is critical for source attribution and international security.

  14. Association of plutonium with sediments from the Ob and Yenisey Rivers and Estuaries.

    PubMed

    Skipperud, Lindis; Brown, Justin; Fifield, L Keith; Oughton, Deborah H; Salbu, Brit

    2009-04-01

    The present study applied sequential extraction techniques to investigate the binding and mobility of plutonium (Pu) in sediments from the rivers and estuaries of the Ob and Yenisey. As a study site, the Ob and Yenisey are particularly interesting as both rivers have weapons-grade Pu sources in their catchment areas, including the Russian Pu production and reprocessing plants at Mayak, Tomsk-7 and Krashnoyarsk, and the Semipalantinsk nuclear weapons testing site in Kazakhstan. Plutonium activity and (240)Pu/(239)Pu ratios were determined using accelerator mass spectrometry (AMS). Sequential extractions showed that between 47 and 80% of the Pu in Yenisey River sediments and 35-53% of the Pu in soils around the Techa River are mobilized with weak oxidising agents, which can indicate that Pu is bound to organic material. In contrast, Pu in Ob and Yenisey Estuarine sediments was more strongly bound, with 60-100% being found in the HNO(3)-extractable fraction. This change in speciation could reflect either that Pu bound to organic material in the Techa and Yenisey River sediments becomes more fixed to the sediments with time, or that organic-bound Pu is mobilized and released to the water when the sediments encounter the more saline water of the Ob and Yenisey estuaries. In general, (240)Pu/(239)Pu ratios were relatively consistent between different extraction fractions, although, in whole sediments, an increase in ratio was observed with distance from the source. This reflects the increased influence of weapon fallout from catchment runoff within the river systems, as compared to the weapons-grade sources close to the production and reprocessing plants. Knowledge of Pu speciation in the Ob and Yenisey Rivers, and the processes controlling its behaviour in estuarine systems, can improve predictions of its transfer and subsequent environmental impact to Arctic Seas. PMID:19157655

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

    PubMed

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

    2008-10-01

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

  16. Radioactive substances in tap water.

    PubMed

    Atsuumi, Ryo; Endo, Yoshihiko; Suzuki, Akihiko; Kannotou, Yasumitu; Nakada, Masahiro; Yabuuchi, Reiko

    2014-01-01

    A 9.0 magnitude (M) earthquake with an epicenter off the Sanriku coast occurred at 14: 46 on March 11, 2011. TEPCO Fukushima Daiichi Nuclear Power Plant (F-1 NPP) was struck by the earthquake and its resulting tsunami. Consequently a critical nuclear disaster developed, as a large quantity of radioactive materials was released due to a hydrogen blast. On March 16(th), 2011, radioiodine and radioactive cesium were detected at levels of 177 Bq/kg and 58 Bq/kg, respectively, in tap water in Fukushima city (about 62km northwest of TEPCO F-1 NPP). On March 20th, radioiodine was detected in tap water at a level of 965 Bq/kg, which is over the value-index of restrictions on food and drink intake (radioiodine 300 Bq/kg (infant intake 100 Bq/kg)) designated by the Nuclear Safety Commission. Therefore, intake restriction measures were taken regarding drinking water. After that, although the all intake restrictions were lifted, in order to confirm the safety of tap water, an inspection system was established to monitor all tap water in the prefecture. This system has confirmed that there has been no detection of radioiodine or radioactive cesium in tap water in the prefecture since May 5(th), 2011. Furthermore, radioactive strontium ((89) Sr, (90)Sr) and plutonium ((238)Pu, (239)Pu+(240)Pu) in tap water and the raw water supply were measured. As a result, (89) Sr, (238)Pu, (239)Pu+(240)Pu were undetectable and although (90)Sr was detected, its committed effective dose of 0.00017 mSv was much lower than the yearly 0.1 mSv of the World Health Organization guidelines for drinking water quality. In addition, the results did not show any deviations from past inspection results.

  17. 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.

  18. Actinide Targets for Neutron Cross Section Measurements

    SciTech Connect

    John D. Baker; Christopher A. McGrath

    2006-10-01

    The Advanced Fuel Cycle Initiative (AFCI) and the Generation IV Reactor Initiative have demonstrated a lack of detailed neutron cross-sections for certain "minor" actinides, those other than the most common (235U, 238U, and 239Pu). For some closed-fuel-cycle reactor designs more than 50% of reactivity will, at some point, be derived from "minor" actinides that currently have poorly known or in some cases not measured (n,?) and (n,f) cross sections. A program of measurements under AFCI has begun to correct this. One of the initial hurdles has been to produce well-characterized, highly isotopically enriched, and chemically pure actinide targets on thin backings. Using a combination of resurrected techniques and new developments, we have made a series of targets including highly enriched 239Pu, 240Pu, and 242Pu. Thus far, we have electrodeposited these actinide targets. In the future, we plan to study reductive distillation to achieve homogeneous, adherent targets on thin metal foils and polymer backings. As we move forward, separated isotopes become scarcer, and safety concerns become greater. The chemical purification and electodeposition techniques will be described.

  19. {sup 237}Np in Hemp-palm leaves of Bontenchiku for fishing gear used by the Fifth Fukuryu-Maru: 40 year after {open_quotes}Bravo{close_quotes}

    SciTech Connect

    Yamamoto, Masayoshi; Komura, Kazuhisa; Ueno, Kaoru

    1996-05-01

    The alpha radioactive components in the Hemp-palm leaves of Bontenchiku were determined with emphasis on the measurement of low-level {sup 237}Np by alpha-ray spectrometry after chemical separation. Bontenchiku is a kind of fishing gear for long-line fishing used by the Fifth Fukuryu-Maru (Lucky Dragon). This gear was exposed to fallout from the second thermonuclear test explosion (Bravo) at Bikini Atoll in March 1954. The {sup 237}Np content in the Bontenchiku sample was determined to be 11.5 {plus_minus}0.8 mBq g{sup {minus}1} with an activity ratio of {sup 237}Np: {sup 239,240}Pu and an atom ratio of {sup 237}Np: {sup 239}Pu estimated to be (2.2 {plus_minus}0.2) x 10{sup {minus}3} and 0.42 {plus_minus}0.04, respectively. The data showed the existence of a chain reaction of {sup 238}U and its ratio to be {sup 237}Np: {sup 239}Pu, as well as the presence of {sup 237}U at the time of fallout from Bravo event in March 1954. 12 refs., 5 figs., 1 tab.

  20. UPWARD MOVEMENT OF PLUTONIUM TO SURFACE SEDIMENTS DURING AN 11-YEAR FIELD STUDY

    SciTech Connect

    Kaplan, D.; Beals, D.; Cadieux, J.; Halverson, J.

    2010-01-25

    An 11-y lysimeter study was established to monitor the movement of Pu through vadose zone sediments. Sediment Pu concentrations as a function of depth indicated that some Pu moved upward from the buried source material. Subsequent numerical modeling suggested that the upward movement was largely the result of invading grasses taking up the Pu and translocating it upward. The objective of this study was to determine if the Pu of surface sediments originated from atmosphere fallout or from the buried lysimeter source material (weapons-grade Pu), providing additional evidence that plants were involved in the upward migration of Pu. The {sup 240}Pu/{sup 239}Pu and {sup 242}Pu/{sup 239}Pu atomic fraction ratios of the lysimeter surface sediments, as determined by Thermal Ionization Mass Spectroscopy (TIMS), were 0.063 and 0.00045, respectively; consistent with the signatures of the weapons-grade Pu. Our numerical simulations indicate that because plants create a large water flux, small concentrations over multiple years may result in a measurable accumulation of Pu on the ground surface. These results may have implications on the conceptual model for calculating risk associated with long-term stewardship and monitored natural attenuation management of Pu contaminated subsurface and surface sediments.

  1. Actinide Measurements by Accelerator Mass Spectrometry at Lawrence Livermore National Laboratory

    SciTech Connect

    Brown, T A; Marchetti, A A; Martinelli, R E; Cox, C C; Knezovich, J P; Hamilton, T F

    2003-09-25

    We report on the development of an accelerator mass spectrometry (AMS) system for the measurement of actinides at Lawrence Livermore National Laboratory. This AMS system is centered on a recently completed heavy isotope beam line that was designed particularly for high sensitivity, robust, high-throughput measurements of actinide concentrations and isotopic ratios. A fast isotope switching capability has been incorporated in the system, allowing flexibility in isotope selection and for the quasi-continuous normalization to a reference isotope spike. Initially, our utilization of the heavy isotope system has concentrated on the measurement of Pu isotopes. Under current operating conditions, background levels equivalent to {approx}1 x 10{sup 5} atoms are observed during routine {sup 239}Pu and {sup 240}Pu measurements. Measurements of samples containing {approx}10{sup 13} {sup 238}U atoms demonstrate that the system provides a {sup 238}U rejection factor during {sup 239}Pu measurements of {approx}10{sup 7}. Measurements of known materials, combined with results from an externally organized inter-comparison program, indicate that our {sup 239}Pu measurements are accurate and precise down to the {micro}Bq level ({approx}10{sup 6} atoms). Recently, we have investigated the performance of our heavy isotope AMS system in measurements of {sup 237}Np and {sup 236}U. Results of these investigations are discussed. The sensitivity shown by our Pu measurements, combined with the high throughput and interference rejection capabilities of our AMS system, demonstrate that AMS can provide a rapid and cost-effective measurement technique for actinides in a wide variety of studies.

  2. 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.

  3. 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.

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

    PubMed Central

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

    2013-01-01

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

  5. Burnup estimation of fuel sourcing radioactive material based on monitored Cs and Pu isotopic activity ratios in Fukushima N. P. S. accident

    SciTech Connect

    Yamamoto, T.; Suzuki, M.; Ando, Y.

    2012-07-01

    After the severe core damage of Fukushima Dai-Ichi Nuclear Power Station, radioactive material leaked from the reactor buildings. As part of monitoring of radioactivity in the site, measurements of radioactivity in soils at three fixed points have been performed for {sup 134}Cs and {sup 137}Cs with gamma-ray spectrometry and for Pu, Pu, and {sup 240}Pu with {alpha}-ray spectrometry. Correlations of radioactivity ratios of {sup 134}Cs to {sup 137}Cs, and {sup 238}Pu to the sum of {sup 239}Pu and {sup 240}Pu with fuel burnup were studied by using theoretical burnup calculations and measurements on isotopic inventories, and compared with the Cs and Pu radioactivity rations in the soils. The comparison indicated that the burnup of the fuel sourcing the radioactivity was from 18 to 38 GWd/t, which corresponded to that of the fuel in the highest power and, therefore, the highest decay heat in operating high-burnup fueled BWR cores. (authors)

  6. Main results of the 2012 joint Norwegian-Russian expedition to the dumping sites of the nuclear submarine K-27 and solid radioactive waste in Stepovogo Fjord, Novaya Zemlya.

    PubMed

    Gwynn, Justin P; Nikitin, Aleksander; Shershakov, Viacheslav; Heldal, Hilde Elise; Lind, Bjørn; Teien, Hans-Christian; Lind, Ole Christian; Sidhu, Rajdeep Singh; Bakke, Gunnar; Kazennov, Alexey; Grishin, Denis; Fedorova, Anastasia; Blinova, Oxana; Sværen, Ingrid; Lee Liebig, Penny; Salbu, Brit; Wendell, Cato Christian; Strålberg, Elisabeth; Valetova, Nailja; Petrenko, Galina; Katrich, Ivan; Logoyda, Igor; Osvath, Iolanda; Levy, Isabelle; Bartocci, Jean; Pham, Mai Khanh; Sam, Adam; Nies, Hartmut; Rudjord, Anne Liv

    2016-01-01

    This paper reports the main results of the 2012 joint Norwegian-Russian expedition to investigate the radioecological situation of the Stepovogo Fjord on the eastern coast of Novaya Zemlya, where the nuclear submarine K-27 and solid radioactive waste was dumped. Based on in situ gamma measurements and the analysis of seawater and sediment samples taken around the submarine, there was no indication of any leakage from the reactor units of K-27. With regard to the radioecological status of Stepovogo Fjord, activity concentrations of all radionuclides in seawater, sediment and biota in 2012 were in general lower than reported from the previous investigations in the 1990s. However in 2012, the activity concentrations of (137)Cs and, to a lesser extent, those of (90)Sr remained elevated in bottom water from the inner part of Stepovogo Fjord compared with surface water and the outer part of Stepovogo Fjord. Deviations from expected (238)Pu/(239,240)Pu activity ratios and (240)Pu/(239)Pu atom ratios in some sediment samples from the inner part of Stepovogo Fjord observed in this study and earlier studies may indicate the possibility of leakages from dumped waste from different nuclear sources. Although the current environmental levels of radionuclides in Stepovogo Fjord are not of immediate cause for concern, further monitoring of the situation is warranted.

  7. Vertical distribution and migration of global fallout Pu in forest soils in southwestern China.

    PubMed

    Bu, Wenting; Zheng, Jian; Guo, Qiuju; Uchida, Shigeo

    2014-10-01

    Soil samples collected in southwestern China were analyzed for Pu isotopes. The (240)Pu/(239)Pu atom ratios were around 0.18, which indicated the dominant source of global fallout. Consistent sub-surface maximums followed by exponential decline of (239+240)Pu activities in the soil cores were observed. Most of the Pu has still remained in the 0-10 cm layers since its deposition. Convection velocities and dispersion coefficients for Pu migration in the soils were estimated by the convection-dispersion equation (CDE) model. The effective convection velocities and effective dispersion coefficients ranged from 0.05 to 0.11 cm/y and from 0.06 to 0.29 cm(2)/y, respectively. Other factors that control the vertical migration of Pu in soil besides precipitation, soil particle size distribution and organic matter were suggested. Long-term migration behaviors of Pu in the soils were simulated. The results provide the Pu background baseline for further environmental monitoring and source identification of non-global fallout Pu inputs in the future.

  8. Uncertainty analysis for determination of plutonium mass by neutron multiplicity counting

    SciTech Connect

    Carrillo, L.A.; Ensslin, N.; Krick, M.S.; Langner, D.G.; Rudy, C.R.

    1998-12-31

    This paper describes an uncertainty analysis carried out in association with the use of neutron multiplicity counting to collect data, and assign a total plutonium mass. During 1997, the Los Alamos Safeguards Science and Technology Group carried out careful calorimetry and neutron multiplicity certification measurements on two {sup 239}Pu metal foils used as reference standards at the Idaho National Environmental Engineering Laboratory (INEEL). The foils were measured using a five ring neutron multiplicity counter designed for neutron measurement control activities. This multiplicity counter is well characterized, and the detector parameters were reaffirmed before the measurements were made using several well-known Los Alamos standards. Then, the {sup 240}Pu effective mass of the foils was determined directly from the multiplicity analysis without a conventional calibration curve based on representative standards. Finally, the {sup 240}Pu effective mass fraction and the total plutonium mass was calculated using gamma ray isotopics. Errors from statistical data collection, background subtraction, cosmic ray interaction, dead time corrections, calibration constants, sample geometry, and sample position were carefully estimated and propagated. The authors describe these error sources, the final calculated relative error in the foil assay, and the comparison with very accurate calorimetry measurements.

  9. Comparative skeletal distribution of americium and plutonium in man, monkey and baboon

    SciTech Connect

    Lynch, T.P.; Dagle, G.E.; Kathren, R.L.; McInroy, J.F.

    1988-10-01

    The skeletal distributions of americium and plutonium in four humans were compared with the skeletal distributions of these radioelements in baboons and monkeys. With respect to the skeletal distribution of these elements, excellent agreement was noted among the four human cases; americium data was available for all four cases and plutonium for three. The human case database was thus adequate for comparison with those of other primates. A statistically significant correlation was found between the /sup 241/Am and /sup 239/Pu + /sup 240/Pu skeletal distributions in the humans and those in non-human primates. Trabecular bone had the highest concentrations of /sup 241/Am and /sup 239 +240/Pu in man, baboon, and monkey. Scaling factors are proposed to convert the percentages of skeletal activity in animal bones to the corresponding percentages in the bones of the human skeleton. However, considerable variation was found between the humans and animals in the percentages of the skeletal activity found in the same bone. 12 refs., 7 tabs.

  10. Evaluating global atmospheric transport of plutonium with dust aerosols

    NASA Astrophysics Data System (ADS)

    Velarde, R.; Arimoto, R.; Gill, T. E.; Kang, C.; Goodell, P.

    2009-12-01

    The resuspension of soils contaminated with radionuclides from nuclear weapons tests is a mechanism by which plutonium can be re-distributed throughout the environment. To better understand the global atmospheric transport of plutonium, we measured the activity of Pu in aerosol samples from four widely separated sites that receive dust from distant sources in both Asia and Africa. High-volume aerosol samples were collected from Barbados (2005 - 2006); Gosan, South Korea (2005 - 2006); Izaña, Canary Islands (1989 - 1996); and Mauna Loa Observatory, Hawaii (2005 - 2006) to evaluate the relationship between Pu activity and mineral dust concentrations (using crustal elements such as aluminum as a dust proxy). The activity of 239,240Pu (239Pu + 240Pu) in the aerosol samples was determined by alpha spectrometry following a series of chemical separations. Concentrations of other elements were determined by a variety of techniques. Pu activity was below the detection limit in many samples. In those samples where it was detected, the Gosan site had the highest dust concentrations and highest total plutonium activity, while Mauna Loa Observatory had the lowest dust concentrations and lowest 239,240Pu activity. The Izaña samples had the second highest concentrations of dust and plutonium activity, while Barbados had the third highest levels of both crustal aerosols and plutonium activity. The dust concentrations are consistent with previous observations at these remote sites, and we propose that the plutonium (primarily from past atmospheric nuclear weapons testing, much of which took place in arid lands) was deposited on erodible soil surfaces and subsequently transported as part of the overall mineral dust load. The results of this study have implications for the global transport and fate of Pu through its association with dust, the biogeochemical and environmental impacts of other substances associated with dust, and the workings of the dust cycle itself.

  11. Short term soil erosion dynamics in alpine grasslands - Results from a Fallout Radionuclide repeated-sampling approach

    NASA Astrophysics Data System (ADS)

    Arata, Laura; Meusburger, Katrin; Zehringer, Markus; Ketterer, Michael E.; Mabit, Lionel; Alewell, Christine

    2016-04-01

    Improper land management and climate change has resulted in accelerated soil erosion rates in Alpine grasslands. To efficiently mitigate and control soil erosion and reduce its environmental impact in Alpine grasslands, reliable and validated methods for comprehensive data generation on its magnitude and spatial extent are mandatory. The use of conventional techniques (e.g. sediment traps, erosion pins or rainfall simulations) may be hindered by the extreme topographic and climatic conditions of the Alps. However, the application of the Fallout Radionuclides (FRNs) as soil tracers has already showed promising results in these specific agro-ecosystems. Once deposited on the ground, FRNs strongly bind to fine particles at the surface soil and move across the landscape primarily through physical processes. As such, they provide an effective track of soil and sediment redistribution. So far, applications of FRN in the Alps include 137Cs (half-life: 30.2 years) and 239+240Pu (239Pu [half-life = 24110 years] and 240Pu [half-life = 6561 years]). To investigate short term (4-5 years) erosion dynamics in the Swiss Alps, the authors applied a FRNs repeated sampling approach. Two study areas in the central Swiss Alps have been investigated: the Urseren Valley (Canton Uri), where significant land use changes occurred in the last centuries, and the Piora Valley (Canton Ticino), where land use change plays a minor role. Soil samples have been collected at potentially erosive sites along the valleys over a period of 4-5 years and measured for 137Cs and 239+240Pu activity. The inventory change between the sampling years indicates high erosion and deposition dynamics at both valleys. High spatial variability of 137Cs activities at all sites has been observed, reflecting the heterogeneous distribution of 137Cs fallout after the Chernobyl power plant accident in 1986. Finally, a new modelling technique to convert the inventory changes to quantitative estimates of soil erosion has

  12. Long-lived radionuclides in residues from operation and decommissioning of nuclear power plants

    NASA Astrophysics Data System (ADS)

    López-Gutiérrez, J. M.; Gómez-Guzmán, J. M.; Chamizo, E.; Peruchena, J. I.; García-León, M.

    2013-01-01

    Radioactive residues, in order to be classified as Low-Level Waste (LLW), need to fulfil certain conditions; the limitation of the maximum activity from long-lived radionuclides is one of these requirements. In order to verify compliance to this limitation, the abundance of these radionuclides in the residue must be determined. However, performing this determination through radiometric methods constitutes a laborious task. In this work, 129I concentrations, 239+240Pu activities, and 240Pu/239Pu ratios are determined in low-level radioactive residues, including resins and dry sludge, from nuclear power plants in Spain. The use of Accelerator Mass Spectrometry (AMS) enables high sensitivities to be achieved, and hence these magnitudes can be re determined with good precision. Results present a high dispersion between the 129I and 239+240Pu activities found in various aliquots of the same sample, which suggests the existence of a mixture of resins with a variety of histories in the same container. As a conclusion, it is shown that activities and isotopic ratios can provide information on the processes that occur in power plants throughout the history of the residues. Furthermore, wipes from the monitoring of surface contamination of the José Cabrera decommissioning process have been analyzed for 129I determination. The wide range of measured activities indicates an effective dispersal of 129I throughout the various locations within a nuclear power plant. Not only could these measurements be employed in the contamination monitoring of the decommissioning process, but also in the modelling of the presence of other iodine isotopes.

  13. Sources and Spatial Distribution of Metal Pollutants in Soils near the El Paso Smelter: A Forensic Study with Pb and Pu Isotopes.

    NASA Astrophysics Data System (ADS)

    Ketterer, Michael; Moan, Matthew; Gremillion, Paul

    2010-05-01

    Pu activities, and hence contain most or all of the cumulative deposition inventory of smelter pollutants, while soils with low 239+240Pu activities can be regarded as 'disturbed', and cannot contain the entire deposition inventory. 240Pu/239Pu atom ratio measurements reveal that the Pu is from stratospheric fallout, precluding other local or regional sources. Our results indicate that 239+240Pu activities are closely correlated with concentrations of smelter pollutants within a specific distance grouping; hence, the soil concentrations of contaminant metals are described by a 'distance' factor and a 'disturbance' factor, the latter being probed using 239+240Pu as an effective proxy measure. Linear correlations (r2 > 0.95) are observed for metal concentrations vs. 239+240Pu activity for a given distance grouping; lines of varying slope are observed for different distance groupings. In desert soils remote from the smelter, the metal constituents are present from other anthropogenic and geogenic sources, and their concentrations are uncorrelated with 239+240Pu activity.

  14. R-matrix analysis of the {sup 240}Pu neutron cross sections in the thermal to 5700 eV energy range

    SciTech Connect

    Derrien, H.; Bouland, O.; Larson, N.M.; Leal, L.C.

    1997-08-01

    Resonance analysis of high resolution neutron transmission data and of fission cross sections were performed in the neutron energy range from the thermal regions to 5,700 eV by using the Reich-Moore Bayesian code SAMMY. The experimental data base is described and the method of analysis is given. The experimental data were carefully examined in order to identify more resonances than those found in the current evaluated data files. The statistical properties of the resonance parameters are given. A new set of the average values of the parameters is proposed, which could be used for calculation of the average cross sections in the unresolved resonance region. The resonance parameters are available IN ENDF-6 format at the national or international data centers.

  15. The effect of permafrost on soil erosion using meteoric 10Be, 137Cs and 239+240Pu in the Eastern Swiss Alps

    NASA Astrophysics Data System (ADS)

    Pichler, Barbara; Brandovà, Dagmar; Alewell, Christine; Ivy-Ochs, Susan; Kubik, Peter W.; Kneisel, Christof; Meusburger, Katrin; Ketterer, Michael; Egli, Markus

    2013-04-01

    Permafrost ecosystems are highly sensitive to climate warming. The expected changes in the thermal and hydrological soil regime might have crucial consequences on soil erosion processes. Therefore, the determination of erosional activities on the long- (since the beginning of soil formation) and mid-term (last 50-60 yr) using cosmogenic and anthropogenic radionuclides can provide important information on past and ongoing processes. Permafrost soils in the Alps and their behaviour with climate change are only rarely studied. The expected new insights will lead to a better understanding of the processes of high mountain soils and are a further step towards improving climate-related modelling of fast warming scenarios and increasing system disequilibria. Our aim is to quantify soil erosion processes in permafrost soils and nearby unfrozen soils in the Alpine (sites at 2700 m asl) and the sub-Alpine (sites 1800 m asl) range of the Swiss Alps (Upper Engadine). We hypothesise that permafrost soils differ distinctly in their long- and mid-term soil erosion rates due to different water retention capacities. Long-term soil erosion was assessed using meteoric 10Be. Meteoric 10Be in a soil profile was estimated assuming that it is has been deposited as a function of precipitation and adsorbed in the fine earth fraction (

  16. Radioanalytical determination of 239+240Pu and 241Am in bioassay samples by anion exchange and extraction chromatography: Preliminary considerations about the two methods

    NASA Astrophysics Data System (ADS)

    Ridone, S.; Arginelli, D.; Berton, G.; Bortoluzzi, S.; Canuto, G.; Montalto, M.; Nocente, M.; Vegro, M.

    2006-01-01

    During the radiation protection surveillance of exposed workers samples of urine and faeces were collected. Anion exchange chromatography was used for the separation of Pu. We investigated a technique to purify and separate Pu and Am isotopes using extraction chromatography with TRU resin. We tested different procedures to dissolve organic matter and eliminate interferences for chromatographic elution. At the end of the proces we have succeeded in electroplating the two radionuclides separately. We have also studied extraction chromatography with UTEVA resin to purify Pu isotopes and separate it from natural uranium radioisotopes, present in some biological samples. We validated a method for the determination of Pu in biological samples and a rather constant chemical yield and resolved peaks were obtained. The preliminary studies on TRU resin have indicated that it is possible to combine extraction and anion-exchange chromatography for analysing separately Pu and Am isotopes from the same sample aliquote.

  17. Evidence for Hydroxamate Siderophores and Other N-Containing Organic Compounds Controlling (239,240)Pu Immobilization and Remobilization in a Wetland Sediment.

    PubMed

    Xu, Chen; Zhang, Saijin; Kaplan, Daniel I; Ho, Yi-Fang; Schwehr, Kathleen A; Roberts, Kimberly A; Chen, Hongmei; DiDonato, Nicole; Athon, Matthew; Hatcher, Patrick G; Santschi, Peter H

    2015-10-01

    Pu concentrations in wetland surface sediments collected downstream of a former nuclear processing facility in F-Area of the Savannah River Site (SRS), USA, were ∼2.5 times greater than those measured in the associated upland aquifer sediments; similarly, the Pu concentration solid/water ratios were orders of magnitude greater in the wetland than in the low-organic matter content aquifer soils. Sediment Pu concentrations were correlated to total organic carbon and total nitrogen contents and even more strongly to hydroxamate siderophore (HS) concentrations. The HS were detected in the particulate or colloidal phases of the sediments but not in the low molecular weight fractions (<1000 Da). Macromolecules which scavenged the majority of the potentially mobile Pu were further separated from the bulk mobile organic matter fraction ("water extract") via an isoelectric focusing experiment (IEF). An electrospray ionization Fourier-transform ion cyclotron resonance ultrahigh resolution mass spectrometry (ESI FTICR-MS) spectral comparison of the IEF extract and a siderophore standard (desferrioxamine; DFO) suggested the presence of HS functionalities in the IEF extract. This study suggests that while HS are a very minor component in the sediment particulate/colloidal fractions, their concentrations greatly exceed those of ambient Pu, and HS may play an especially important role in Pu immobilization/remobilization in wetland sediments.

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

    SciTech Connect

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

    2010-12-16

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

  19. Radionuclides in Arctic sea ice: Tracers of sources, fates and ice transit time scales

    NASA Astrophysics Data System (ADS)

    Masqué, P.; Cochran, J. K.; Hirschberg, D. J.; Dethleff, D.; Hebbeln, D.; Winkler, A.; Pfirman, S.

    2007-08-01

    Arctic sea ice can incorporate sediment and associated chemical species during its formation in shallow shelf environments and can also intercept atmospherically transported material during transit. Release of this material in ice ablation areas (e.g. the Fram Strait) enhances fluxes of both sediments and associated species in such areas. We have used a suite of natural ( 7Be, 210Pb) and anthropogenic ( 137Cs, 239Pu, 240Pu) radionuclides in sea ice, sea-ice sediments (SIS), sediment trap material and bottom sediments from the Fram Strait to estimate transit times of sea ice from source to ablation areas, calculate radionuclide fluxes to the Fram Strait and investigate the role of sea-ice entrained sediments in sedimentation processes. Sea ice intercepts and transports the atmospherically supplied radionuclides 7Be and 210Pb, which are carried in the ice and are scavenged by any entrained SIS. All of the 7Be and most of the excess 210Pb measured in SIS collected in the Fram Strait are added to the ice during transit through the Arctic Ocean, and we use these radionuclides as chronometers to calculate ice transit times for individual ice floes. Transit times estimated from the 210Pb inventories in two ice cores are 1-3 years. Values estimated from the 7Be/ 210Pb excess activity ratio of SIS are about 3-5 years. Finally, equilibrium values of the activity ratio of 210Pb to its granddaughter 210Po in the ice cores indicate transit times of at least 2 years. These transit times are consistent with back-trajectory analyses of the ice floes. The latter, as well as the clay-mineral assemblage of the SIS (low smectite and high illite content), suggest that the sampled sea-ice floes originated from the eastern Siberian Arctic shelf seas such as the eastern Laptev Sea and the East Siberian Sea. This result is in agreement with the relatively low activities of 239,240Pu and 137Cs and the 240Pu/ 239Pu atom ratios (˜0.18, equivalent to that in global fallout) in SIS, indicating

  20. Cleanup levels for Am-241, Pu-239, U-234, U-235 & U-238 in soils at the Rocky Flats Environmental Technology Site

    SciTech Connect

    Roberts, R.; Colby, B.; Brooks, L.; Slaten, S.

    1997-07-03

    This presentation briefly outlines a cleanup program at a Rocky Flats site through viewgraphs and an executive summary. Exposure pathway analyses to be performed are identified, and decontamination levels are listed for open space and office worker exposure areas. The executive summary very briefly describes the technical approach, RESRAD computer code to be used for analyses, recommendations for exposure levels, and application of action levels to multiple radionuclide contamination. Determination of action levels for surface and subsurface soils, based on radiation doses, is discussed. 1 tab.

  1. Delayed neutron detection with an integrated differential die-away and delayed neutron instrument

    SciTech Connect

    Blanc, Pauline; Tobin, Stephen J; Lee, Taehoon; Hu, Jianwei S; Hendricks, John; Croft, Stephen

    2010-01-01

    The Next Generation Safeguards Initiative (NGSI) of the U.S. Department of Energy (DOE) has funded a multilab/university collaboration to quantify the plutonium (Pu) mass and detect the diversion of pins from spent nuclear fuel. The first two years of this NGSI effort was focused on quantifying the capability of a range of nondestructive assay (NDA) techniques with Monte Carlo (MCNPX) modeling and the second current phase involves measuring Spent Fuel. One of the techniques of interest in this paper involves measuring delayed neutrons. A delayed neutron instrument using 36 fission chambers and a 14 MeV neutron generator so called DT generator (Deuterium + Tritium) surrounding the fuel was previously studied as part of the NGSI effort. This paper will quantify the capability of a standalone delayed neutron instrument using 4 {sup 3}He gas filled tubes and a DT generator with significant spectrum tailoring, located far from the fuel. So that future research can assess how well a delayed neutron instrument will function as part of an integrated NDA system. A new design is going to be used to respond to the need of the techniques. This design has been modeled for a water media and is currently being optimized for borated water and air media as part of ongoing research. This new design was selected in order to minimize the fission of {sup 238}U, to use a more realistic neutron generator design in the model, to reduce cost and facilitate the integration of a delayed neutron (DN) with a differential die-away (DDA) instrument. Since this paper will focus on delayed neutron detection, the goal is to quantify the signal from {sup 235}U, {sup 239}Pu and {sup 241}Pu, which are the isotopes present in Spent Fuel that respond significantly to a neutron interrogation. This report will quantify the capability of this new delayed neutron design to measure the combined mass of {sup 235}U, {sup 239}Pu and {sup 241}Pu for 16 of the 64 assemblies of the NGSI Spent Fuel library in one

  2. Future research program on prompt γ-ray emission in nuclear fission

    NASA Astrophysics Data System (ADS)

    Oberstedt, S.; Billnert, R.; Hambsch, F.-J.; Lebois, M.; Oberstedt, A.; Wilson, J. N.

    2015-12-01

    In recent years the measurement of prompt fission γ-ray spectra (PFGS) has gained renewed interest, after about forty years since the first comprehensive studies of the reactions 235U(n th , f), 239Pu(n th ,f) and 252Cf(sf). The renaissance was initiated by requests for new values especially for γ-ray multiplicity and average total energy release per fission in neutron-induced fission of 235U and 239Pu. Both isotopes are considered the most important ones with respect to the modeling of innovative cores required for the Generation-IV reactors, the majority working with fast neutrons. During the last 5 years we have conducted a systematic study of spectral data for thermal-neutron-induced fission on 235U and 241Pu as well as for the spontaneous fission of 252Cf with unprecedented accuracy. From the new data we conclude that those reactions do not considerably contribute to the observed heat excess and suspect other reactions playing a significant role. Possible contributions may originate from fast-neutron-induced reactions on 238U, which is largely present in the fuel, or from γ-induced fission from neutron capture in the construction material. A first experiment campaign on prompt γ-ray emission from fast-neutron-induced fission on 235,238U was successfully performed in order to test our assumptions. In the following we attempt to summarize, what has been done in the field to date, and to motivate future measurement campaigns exploiting dedicated neutron and photon beams as well as upcoming highly efficient detector assemblies.

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

    SciTech Connect

    Lind, O.C.; Salbu, B.; Janssens, K.; Proost, K.; Garcia-Leon, M.; Garcia-Tenorio, R.

    2007-07-10

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

  5. Plutonium and Uranium Atom Ratios and Activity Levels in Cochiti Lake Bottom Sediments Provided by Pueblo de Cochiti

    SciTech Connect

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

    1999-05-01

    Historical operations at the Los Alamos National Laboratory have contaminated stream sediments with plutonium and other radionuclides. A small portion of these contaminated sediments has been carried by floods into the Rio Grande drainage system, eventually to be trapped by Cochiti Lake located on Pueblo de Cochiti lands approximately 8 km downstream of the Laboratory. In this study, lake bottom sediment samples provided by the Pueblo de Cochiti were analyzed by thermal ionization mass spectrometry to determine plutonium and uranium activity levels and isotopic atom ratios. This specialized analytical method allows us to take isotopic fingerprints of radionuclides found in the sediment and to determine how much plutonium and uranium came from the Laboratory and how much was deposited by worldwide fallout or is natural. Two distinct types of samples were processed: segments of a continuous vertical core of the entire accumulated sediment sequence and other samples from across the lake bottom at the water/sediment interface. Based on measurement of the {sup 240}Pu/{sup 239}Pu atom ratio, Laboratory-derived plutonium is present in eight of nine samples at the core site. On a depth-weighted basis, approximately one-half of the {sup 239}Pu and {sup 240}Pu came from early operations at the Laboratory; the remaining plutonium came from fallout dispersed by above-ground nuclear tests. In contrast to the core site, the samples from the other locations showed little or no evidence of Laboratory-derived plutonium, with more than 90 percent of the plutonium attributable to fallout. The overall amount of plutonium in all the samples is of the same magnitude as other reservoirs in the region. The net increase in plutonium over upstream reservoirs unaffected by Laboratory activities is a maximum of 0.014 pCi/g or 3.5 times. All of the samples reflect natural uranium compositions. Laboratory-derived uranium is not identifiable, presumably because the sediment contains abundant

  6. Long-term development of the radionuclide exposure of murine rodent populations in Belarus after the Chernobyl accident.

    PubMed

    Ryabokon, N I; Smolich, I I; Kudryashov, V P; Goncharova, R I

    2005-12-01

    As a determinant of the associated health risks, the behavior of radionuclides in natural ecosystems needs to be better understood. Therefore, the activity concentration of various long-lived radionuclides released due to the Chernobyl accident, and the corresponding contributions to the whole-body dose rate, was studied as a function of time in mammalian indicator species inhabiting the natural forest ecosystems of Belarus, the bank vole (Clethrionomys glareolus) and the yellow-necked mouse (Apodemus flavicollus). The activity concentrations of 137Cs, 134Cs, 90Sr, 238Pu, 239,240Pu, 241Pu and 241Am in soil and in animals were measured at five monitoring sites with different ground deposition of radionuclides at different distances from the destroyed reactor. The observed temporal pattern of the radionuclide activity concentration in the studied animal populations reflects the changes in biological availability of these isotopes for biota, mostly due to fuel particle destruction and appearance of dissolved and exchangeable forms of radionuclides. The time course of 134+137Cs activity concentrations in animal populations appeared as a sequence of increase, peak and decrease. Maximal levels of radiocesium occurred 1-2 years after deposition, followed by an exponential decrease. Concentrations of incorporated 90Sr increased up to the tenth year after deposition. The activity concentrations of transuranic elements (238Pu, 239,240Pu, 241Pu and 241Am) were much lower than those of the other radionuclides, in the studied animals. A considerable activity of 241Am in animals from areas with high levels of contamination was firstly detected 5 years after deposition, it increased up to the tenth year and is expected to increase further in the future. Maximal values of the whole-body absorbed dose rates occurred during the year of deposition, followed by a decrease in the subsequent period. Generally, this decrease was monotonic, mainly determined by the decrease of the

  7. Long-term development of the radionuclide exposure of murine rodent populations in Belarus after the Chernobyl accident.

    PubMed

    Ryabokon, N I; Smolich, I I; Kudryashov, V P; Goncharova, R I

    2005-12-01

    As a determinant of the associated health risks, the behavior of radionuclides in natural ecosystems needs to be better understood. Therefore, the activity concentration of various long-lived radionuclides released due to the Chernobyl accident, and the corresponding contributions to the whole-body dose rate, was studied as a function of time in mammalian indicator species inhabiting the natural forest ecosystems of Belarus, the bank vole (Clethrionomys glareolus) and the yellow-necked mouse (Apodemus flavicollus). The activity concentrations of 137Cs, 134Cs, 90Sr, 238Pu, 239,240Pu, 241Pu and 241Am in soil and in animals were measured at five monitoring sites with different ground deposition of radionuclides at different distances from the destroyed reactor. The observed temporal pattern of the radionuclide activity concentration in the studied animal populations reflects the changes in biological availability of these isotopes for biota, mostly due to fuel particle destruction and appearance of dissolved and exchangeable forms of radionuclides. The time course of 134+137Cs activity concentrations in animal populations appeared as a sequence of increase, peak and decrease. Maximal levels of radiocesium occurred 1-2 years after deposition, followed by an exponential decrease. Concentrations of incorporated 90Sr increased up to the tenth year after deposition. The activity concentrations of transuranic elements (238Pu, 239,240Pu, 241Pu and 241Am) were much lower than those of the other radionuclides, in the studied animals. A considerable activity of 241Am in animals from areas with high levels of contamination was firstly detected 5 years after deposition, it increased up to the tenth year and is expected to increase further in the future. Maximal values of the whole-body absorbed dose rates occurred during the year of deposition, followed by a decrease in the subsequent period. Generally, this decrease was monotonic, mainly determined by the decrease of the

  8. Characterization and Source Term Assessments of Radioactive Particles from Marshall Islands Using Non-Destructive Analytical Techniques

    SciTech Connect

    Jernstrom, J; Eriksson, M; Simon, R; Tamborini, G; Bildstein, O; Carlos-Marquez, R; Kehl, S R; Betti, M; Hamilton, T

    2005-06-11

    A considerable fraction of radioactivity entering the environment from different nuclear events is associated with particles. The impact of these events can only be fully assessed where there is some knowledge about the mobility of particle bound radionuclides entering the environment. The behavior of particulate radionuclides is dependent on several factors, including the physical, chemical and redox state of the environment, the characteristics of the particles (e.g., the chemical composition, crystallinity and particle size) and on the oxidative state of radionuclides contained in the particles. Six plutonium-containing particles stemming from Runit Island soil (Marshall Islands) were characterized using non-destructive analytical and microanalytical methods. By determining the activity of {sup 239,240}Pu and {sup 241}Am isotopes from their gamma peaks structural information related to Pu matrix was obtained, and the source term was revealed. Composition and elemental distribution in the particles were studied with synchrotron radiation based micro X-ray fluorescence (SR-{mu}-XRF) spectrometry. Scanning electron microscope equipped with energy dispersive X-ray detector (SEMEDX) and secondary ion mass spectrometer (SIMS) were used to examine particle surfaces. Based on the elemental composition the particles were divided into two groups; particles with plain Pu matrix, and particles where the plutonium is included in Si/O-rich matrix being more heterogeneously distributed. All of the particles were identified as fragments of initial weapons material. As containing plutonium with low {sup 240}Pu/{sup 239}Pu atomic ratio, {approx}2-6%, which corresponds to weapons grade plutonium, the source term was identified to be among the safety tests conducted in the history of Runit Island.

  9. Risk assessment of soil-based exposures to plutonium at experimental sites located on the Nevada Test Site and adjoining areas

    SciTech Connect

    Layton, D.W.; Anspaugh, L.R.; Bogen, K.T.; Straume, T.

    1993-06-01

    In the late 1950s and early 1960s, a series of tests was conducted at or near the Nevada Test Site to study issues involving plutonium-bearing devices. These tests resulted in the dispersal of about 5 TBq of {sup 239,240}Pu on the surficial soils at the test locations. Access to the sites is strictly controlled; therefore, it does not constitute a threat to human health at the present time. However, because the residual {sup 239} Pu decays slowly (half-life of 24,110 y), the sites could indeed represent a long-term hazard if they are not remediated and if institutional controls are lost. To investigate the magnitude of the potential health risks for this no-remediation case, we defined three basic exposure scenarios that could bring individuals in contact with {sup 239,240}Pu at the sites: (1) a resident living in a subdivision located at a test site, (2) a resident farmer, and (3) a worker at a commercial facility. Our screening analyses indicated that doses to organs are dominated by the intemal deposition of Pu via the inhalation pathway, and thus our risk assessment focused on those factors that affect inhalation exposures and associated doses, including inhalation rates, activity patterns, tenure at a residence or occupation, indoor/outdoor air relationships, and resuspension outdoors. Cancer risks were calculated as a function of lifetime cumulative doses to the key target organs (i.e., bone surface, liver, and lungs) and risk factors for those organs. Uncertainties in the predicted cancer risks were analyzed using Monte-Carlo simulations of the probability distributions used to represent assessment parameters. The principal sources of uncertainty in the estimated risks were population mobility, the relationship between indoor and outdoor contaminant levels, and the dose and risk factors for bone, liver, and lung.

  10. Contribution of Recently Measured Nuclear Data to Reactor Antineutrino Energy Spectra Predictions

    NASA Astrophysics Data System (ADS)

    Estienne, M.; Fallot, M.; Cormon, S.; Algora, A.; Bui, V. M.; Cucoanes, A.; Elnimr, M.; Giot, L.; Jordan, D.; Martino, J.; Onillon, A.; Porta, A.; Pronost, G.; Remoto, A.; Taín, J. L.; Yermia, F.; Zakari-Issoufou, A.-A.

    2014-06-01

    The aim of this work is to study the impact of the inclusion of the recently measured β decay properties of the 102,104,105,106,107Tc, 105Mo, and 101Nb nuclei in the calculation of the antineutrino (anti-ν) energy spectra arising after the fissions of the four main fissile isotopes 235,238U, and 239,241Pu in PWRs. These β feeding probabilities, measured using the Total Absorption Technique (TAS) at the JYFL facility of Jyväskylä, have been found to play a major role in the γ component of the decay heat for 239Pu in the 4-3000 s range. Following the fission product summation method, the calculation was performed using the MCNP Utility Reactor Evolution code (MURE) coupled to the experimental spectra built from β decay properties of the fission products taken from evaluated databases. These latest TAS data are found to have a significant effect on the Pu isotope energy spectra and on the spectrum of 238U showing the importance of their measurement for a better assessment of the reactor anti-ν energy spectrum, as well as importance for fundamental neutrino physics experiments and neutrino applied physics.

  11. Determination of the Sensitivity of the Antineutrino Probe for Reactor Core Monitoring

    SciTech Connect

    Cormon, S.; Fallot, M. Bui, V.-M.; Cucoanes, A.; Estienne, M.; Lenoir, M.; Onillon, A.; Shiba, T.; Yermia, F.; Zakari-Issoufou, A.-A.

    2014-06-15

    This paper presents a feasibility study of the use of the detection of reactor-antineutrinos (ν{sup ¯}{sub e}) for non proliferation purpose. To proceed, we have started to study different reactor designs with our simulation tools. We use a package called MCNP Utility for Reactor Evolution (MURE), initially developed by CNRS/IN2P3 labs to study Generation IV reactors. The MURE package has been coupled to fission product beta decay nuclear databases for studying reactor antineutrino emission. This method is the only one able to predict the antineutrino emission from future reactor cores, which don't use the thermal fission of {sup 235}U, {sup 239}Pu and {sup 241}Pu. It is also the only way to include off-equilibrium effects, due to neutron captures and time evolution of the fission product concentrations during a reactor cycle. We will present here the first predictions of antineutrino energy spectra from innovative reactor designs (Generation IV reactors). We will then discuss a summary of our results of non-proliferation scenarios involving the latter reactor designs, taking into account reactor physics constraints.

  12. Contribution of Recently Measured Nuclear Data to Reactor Antineutrino Energy Spectra Predictions

    SciTech Connect

    Estienne, M.; Bui, V.M.; Cucoanes, A.; Elnimr, M.; Giot, L.; Martino, J.; Onillon, A.; Porta, A.; Pronost, G.; Remoto, A.; Yermia, F.; Zakari-Issoufou, A.-A.

    2014-06-15

    The aim of this work is to study the impact of the inclusion of the recently measured β decay properties of the {sup 102,104,105,106,107}Tc, {sup 105}Mo, and {sup 101}Nb nuclei in the calculation of the antineutrino (anti-ν) energy spectra arising after the fissions of the four main fissile isotopes {sup 235,238}U, and {sup 239,241}Pu in PWRs. These β feeding probabilities, measured using the Total Absorption Technique (TAS) at the JYFL facility of Jyväskylä, have been found to play a major role in the γ component of the decay heat for {sup 239}Pu in the 4-3000 s range. Following the fission product summation method, the calculation was performed using the MCNP Utility Reactor Evolution code (MURE) coupled to the experimental spectra built from β decay properties of the fission products taken from evaluated databases. These latest TAS data are found to have a significant effect on the Pu isotope energy spectra and on the spectrum of {sup 238}U showing the importance of their measurement for a better assessment of the reactor anti-ν energy spectrum, as well as importance for fundamental neutrino physics experiments and neutrino applied physics.

  13. Determination of antineutrino spectra from nuclear reactors

    SciTech Connect

    Huber, Patrick

    2011-08-15

    In this paper we study the effect of well-known higher-order corrections to the allowed {beta}-decay spectrum on the determination of antineutrino spectra resulting from the decays of fission fragments. In particular, we try to estimate the associated theory errors and find that induced currents like weak magnetism may ultimately limit our ability to improve the current accuracy and under certain circumstance could even greatly increase the theoretical errors. We also perform a critical evaluation of the errors associated with our method to extract the antineutrino spectrum using synthetic {beta} spectra. It turns out that a fit using only virtual {beta} branches with a judicious choice of the effective nuclear charge provides results with a minimal bias. We apply this method to actual data for {sup 235}U, {sup 239}Pu, and {sup 241}Pu and confirm, within errors, recent results, which indicate a net 3% upward shift in energy-averaged antineutrino fluxes. However, we also find significant shape differences which can, in principle, be tested by high-statistics antineutrino data samples.

  14. Reactor vessel fluence evaluation and dosimetry

    SciTech Connect

    Lois, L. )

    1992-01-01

    The methodology currently in use for the estimation of the fast neutron fluence to the pressure vessel (inside surface and reactor cavity) is based on discrete ordinates two-dimensional codes such as DOT or its updated version DORT. This methodology assumes a P[sub 3] scattering, an S[sub 8] quadrature approximation, and cross sections based on the ENDF/B-IV file. Associated one-dimensional codes are often used for the cross-section collapsing portion of the calculation. The neutron spectrum at the pressure vessel location of interest is estimated assuming a [sup 235]U, [sup 239]Pu, or [sup 241]Pu source spectrum or an appropriate combination thereof. The two-dimensional codes and associated methodologies were benchmarked in the early eighties using the results of the PCA and PSF Oak Ridge National Laboratory reactor experiments. The benchmarking experiments were estimated to provide an uncertainty of [approx]10%. The results of the calculations applied to a reactor were estimated to have an uncertainty of [approx]20%. This level of uncertainty was assumed in the estimation of the margin term defined in 10CFR50.61

  15. Determination of the Sensitivity of the Antineutrino Probe for Reactor Core Monitoring

    NASA Astrophysics Data System (ADS)

    Cormon, S.; Fallot, M.; Bui, V.-M.; Cucoanes, A.; Estienne, M.; Lenoir, M.; Onillon, A.; Shiba, T.; Yermia, F.; Zakari-Issoufou, A.-A.

    2014-06-01

    This paper presents a feasibility study of the use of the detection of reactor-antineutrinos (νbare) for non proliferation purpose. To proceed, we have started to study different reactor designs with our simulation tools. We use a package called MCNP Utility for Reactor Evolution (MURE), initially developed by CNRS/IN2P3 labs to study Generation IV reactors. The MURE package has been coupled to fission product beta decay nuclear databases for studying reactor antineutrino emission. This method is the only one able to predict the antineutrino emission from future reactor cores, which don't use the thermal fission of 235U, 239Pu and 241Pu. It is also the only way to include off-equilibrium effects, due to neutron captures and time evolution of the fission product concentrations during a reactor cycle. We will present here the first predictions of antineutrino energy spectra from innovative reactor designs (Generation IV reactors). We will then discuss a summary of our results of non-proliferation scenarios involving the latter reactor designs, taking into account reactor physics constraints.

  16. Application of Neutron-Absorbing Structural-Amorphous Metal (SAM) Coatings for Spent Nuclear Fuel (SNF) Container to Enhance Criticality Safety Controls

    SciTech Connect

    Choi, J; Lee, C; Day, D; Wall, M; Saw, C; MoberlyChan, W; Farmer, J; Boussoufl, M; Liu, B; Egbert, H; Branagan, D; D'Amato, A

    2006-11-13

    Spent nuclear fuel contains fissionable materials ({sup 235}U, {sup 239}Pu, {sup 241}Pu, etc.). Neutron multiplication and the potential for criticality are enhanced by the presence of a moderator during cask loading in water, water incursion in accidents conditions during spent fuel storage or transport. To prevent nuclear criticality in spent fuel storage, transportation, and during disposal, neutron-absorbing materials (or neutron poisons, such as borated stainless steel, Boral{trademark}, Metamic{trademark}, Ni-Gd, and others) would have to be applied. The success in demonstrating that the High-Performance Corrosion-Resistant material (HPCRM) can be thermally applied as coating onto base metal to provide for corrosion resistance for many naval applications raises the interest in applying the HPCRM to USDOE/OCRWM spent fuel management program. The fact that the HPCRM relies on the high content of boron to make the material amorphous--an essential property for corrosion resistance--and that the boron has to be homogeneously distributed in the HPCRM qualify the material to be a neutron poison.

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

    PubMed

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

    2010-12-15

    Information on plutonium isotope ratios in individual particles is of great importance for nuclear safeguards, nuclear forensics and so on. Although secondary ion mass spectrometry (SIMS) is successfully utilized for the analysis of individual uranium particles, the isobaric interference of americium-241 to plutonium-241 makes difficult to obtain accurate isotope ratios in individual plutonium particles. In the present work, an analytical technique by a combination of chemical separation and inductively coupled plasma mass spectrometry (ICP-MS) is developed and applied to isotope ratio analysis of individual sub-micrometer plutonium particles. The ICP-MS results for individual plutonium particles prepared from a standard reference material (NBL SRM-947) indicate that the use of a desolvation system for sample introduction improves the precision of isotope ratios. In addition, the accuracy of the (241)Pu/(239)Pu isotope ratio is much improved, owing to the chemical separation of plutonium and americium. In conclusion, the performance of the proposed ICP-MS technique is sufficient for the analysis of individual plutonium particles. PMID:21111176

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

    PubMed

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

    2010-12-15

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

  19. Biokinetics of sup 237 Pu citrate and nitrate in the rat: Implications for Pu studies in man

    SciTech Connect

    Talbot, R.J.; Knight, D.A.; Morgan, A. )

    1990-08-01

    Plutonium-237 decays mainly by electron capture with a half-life of 45 d. Alpha particles are emitted in only 5 x 10(-3)% of its disintegrations. This nuclide can now be produced with relatively small amounts of alpha-emitting contaminants so that, in principle, {sup 237}Pu can be used for studies of Pu biokinetics in man. However, because of its high specific activity, there was some doubt that its metabolism would be the same as that of the alpha- and beta-emitting isotopes of Pu normally encountered in the nuclear industry. In this study, the biokinetics of nearly pure, high specific activity {sup 237}Pu are compared with those of lower specific activity, impure {sup 237}Pu containing significant amounts of alpha-emitting Pu, following administration to rats by intravenous injection as the citrate. Both the distribution and excretion of the pure and impure {sup 237}Pu used in the two studies were similar and also in good agreement with the results of previously reported studies using {sup 239}Pu and {sup 241}Pu citrate, thus validating the use of {sup 237}Pu for studies of Pu metabolism in man. Data on the biokinetics of {sup 237}Pu nitrate are also included.

  20. Sensitivity of the Antineutrino Emission from Reactors to the Fuel Content

    SciTech Connect

    Hayes-Sterbenz, Anna C

    2012-06-25

    We investigated the antineutrino signals for several reactor core designs. In all cases we found that the antineutrino signals are distinct. The signals are distinguishable by the combination of their magnitudes and their rate of change with fuel burn-up. If the thermal power of the reactor is known, the overall uncertainty in the antineutrino flux emitted from the reactor is about 5%. The quoted uncertainty in the number of antineutrinos per fission for {sup 235}U, {sup 239}Pu, and {sup 241}Pu is less than 3% and for {sup 238}U is 8%. When folded with the uncertainty in the thermal power measurement and the uncertainty in converting the thermal power to a fission rate, the total antineutrino flux is typically quoted with an accuracy of 3-5%. This overall uncertainty in the antineutrino flux, together with the calculations presented here, suggests that the differences in fuels for the class of reactor designed considered would be detectable using antineutrino monitoring.

  1. Nondestructive NMR technique for moisture determination in radioactive materials.

    SciTech Connect

    Aumeier, S.; Gerald, R.E. II; Growney, E.; Nunez, L.; Kaminski, M.

    1998-12-04

    This progress report focuses on experimental and computational studies used to evaluate nuclear magnetic resonance (NMR) spectroscopy and magnetic resonance imaging (MRI) for detecting, quantifying, and monitoring hydrogen and other magnetically active nuclei ({sup 3}H, {sup 3}He, {sup 239}Pu, {sup 241}Pu) in Spent nuclear fuels and packaging materials. The detection of moisture by using a toroid cavity NMR imager has been demonstrated in SiO{sub 2} and UO{sub 2} systems. The total moisture was quantified by means of {sup 1}H NMR detection of H{sub 2}O with a sensitivity of 100 ppm. In addition, an MRI technique that was used to determine the moisture distribution also enabled investigators to discriminate between bulk and stationary water sorbed on the particles. This imaging feature is unavailable in any other nondestructive assay (NDA) technique. Following the initial success of this program, the NMR detector volume was scaled up from the original design by a factor of 2000. The capacity of this detector exceeds the size specified by DOE-STD-3013-96.

  2. Sequential injection method for rapid and simultaneous determination of 236U, 237Np, and Pu isotopes in seawater.

    PubMed

    Qiao, Jixin; Hou, Xiaolin; Steier, Peter; Golser, Robin

    2013-11-19

    An automated analytical method implemented in a novel dual-column tandem sequential injection (SI) system was developed for simultaneous determination of (236)U, (237)Np, (239)Pu, and (240)Pu in seawater samples. A combination of TEVA and UTEVA extraction chromatography was exploited to separate and purify target analytes, whereupon plutonium and neptunium were simultaneously isolated and purified on TEVA, while uranium was collected on UTEVA. The separation behavior of U, Np, and Pu on TEVA-UTEVA columns was investigated in detail in order to achieve high chemical yields and complete purification for the radionuclides of interest. (242)Pu was used as a chemical yield tracer for both plutonium and neptunium. (238)U was quantified in the sample before the separation for deducing the (236)U concentration from the measured (236)U/(238)U atomic ratio in the separated uranium target using accelerator mass spectrometry. Plutonium isotopes and (237)Np were measured using inductively coupled plasma mass spectrometry after separation. The analytical results indicate that the developed method is robust and efficient, providing satisfactory chemical yields (70-100%) of target analytes and relatively short analytical time (8 h/sample). PMID:24134480

  3. Resuspension and atmospheric transport of radionuclides due to wildfires near the Chernobyl Nuclear Power Plant in 2015: An impact assessment.

    PubMed

    Evangeliou, N; Zibtsev, S; Myroniuk, V; Zhurba, M; Hamburger, T; Stohl, A; Balkanski, Y; Paugam, R; Mousseau, T A; Møller, A P; Kireev, S I

    2016-01-01

    In April and August 2015, two major fires in the Chernobyl Exclusion Zone (CEZ) caused concerns about the secondary radioactive contamination that might have spread over Europe. The present paper assessed, for the first time, the impact of these fires over Europe. About 10.9 TBq of (137)Cs, 1.5 TBq of (90)Sr, 7.8 GBq of (238)Pu, 6.3 GBq of (239)Pu, 9.4 GBq of (240)Pu and 29.7 GBq of (241)Am were released from both fire events corresponding to a serious event. The more labile elements escaped easier from the CEZ, whereas the larger refractory particles were removed more efficiently from the atmosphere mainly affecting the CEZ and its vicinity. During the spring 2015 fires, about 93% of the labile and 97% of the refractory particles ended in Eastern European countries. Similarly, during the summer 2015 fires, about 75% of the labile and 59% of the refractory radionuclides were exported from the CEZ with the majority depositing in Belarus and Russia. Effective doses were above 1 mSv y(-1) in the CEZ, but much lower in the rest of Europe contributing an additional dose to the Eastern European population, which is far below a dose from a medical X-ray. PMID:27184191

  4. AVNG system objectives and concept

    SciTech Connect

    Macarthur, Duncan W; Thron, Jonathan; Razinkov, Sergey; Livke, Alexander; Kondratov, Sergey

    2010-01-01

    Any verification measurement performed on potentially classified nuclear material must satisfy two constraints. First and foremost, no classified information can be released to the monitoring party. At the same time, the monitoring party must gain sufficient confidence from the measurement to believe that the material being measured is consistent with the host's declarations concerning that material. The attribute measurement technique addresses both concerns by measuring several attributes of the nuclear material and displaying unclassified results through green (indicating that the material does possess the specified attribute) and red (indicating that the material does not possess the specified attribute) lights. The AVNG that we describe is an attribute measurement system built by RFNC-VNIIEF in Sarov, Russia. The AVNG measures the three attributes of 'plutonium presence,' 'plutonium mass >2 kg,' and 'plutonium isotopic ratio ({sup 240}Pu to {sup 239}Pu) <0.1' and was demonstrated in Sarov for a joint US/Russian audience in June 2009. In this presentation, we will outline the goals and objectives of the AVNG measurement system. These goals are driven by the two, sometimes conflicting, requirements mentioned above. We will describe the conceptual design of the AVNG and show how this conceptual design grew out of these goals and objectives.

  5. Testing the AVNG

    SciTech Connect

    Thron, Jonathan Louis; Mac Arthur, Duncan W; Kondratov, Sergey; Livke, Alexander; Razinkov, Sergey

    2010-01-01

    An attribute measurement system (AMS) measures a number of unclassified attributes of potentially classified material. By only displaying these unclassified results as red or green lights, the AMS protects potentially classified information while still generating confidence in the measurement result. The A VNG implementation that we describe is an AMS built by RFNC - VNIIEF in Sarov, Russia. The AVNG detects neutron and gamma radiation signatures and displays the three unclassified attributes of 'plutonium presence,' 'plutonium mass > 2 kg,' and 'plutonium isotopic ratio ({sup 240}Pu to {sup 239}Pu) < 0.1.' Prior to demonstration to a joint US/Russian audience, the overall operation and thresholds of the AVNG were tested using a number of multi-kg plutonium reference material (RM) sources manufactured for this purpose. As the AVNG was designed to incorporate an open mode (where all radiation data was displayed) as well as a secure mode (where only the red/green attribute lights were visible), the AVNG was tested in both modes. We will present data from these tests using unclassified plutonium RM sources as well as detector test results obtained using smaller calibration sources.

  6. Pu isotopes in soils collected downwind from Lop Nor: regional fallout vs. global fallout

    NASA Astrophysics Data System (ADS)

    Bu, Wenting; Ni, Youyi; Guo, Qiuju; Zheng, Jian; Uchida, Shigeo

    2015-07-01

    For the first time, soil core samples from the Jiuquan region have been analyzed for Pu isotopes for radioactive source identification and radiological assessment. The Jiuquan region is in downwind from the Lop Nor Chinese nuclear test (CNT) site. The high Pu inventories (13 to 546 Bq/m2) in most of the sampling locations revealed that this region was heterogeneously contaminated by the regional fallout Pu from the CNTs. The contributions of the CNTs to the total Pu in soils were estimated to be more than 40% in most cases. The 240Pu/239Pu atom ratios in the soils ranged from 0.059 to 0.186 with an inventory-weighted average of 0.158, slightly lower than that of global fallout. This atom ratio could be considered as a mixed fingerprint of Pu from the CNTs. In addition, Pu in soils of Jiuquan region had a faster downward migration rate compared with other investigated places in China.

  7. 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

  8. 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.

  9. Results of Gamma-Ray Measurements from a Recent Demonstration for Russian Technical Experts

    SciTech Connect

    Luke, S J; Archer, D E; Gosnell, T B; Lochner, R T; Morgan, J F; White, G K; Weitz, R

    2001-06-01

    In August 2001, a group of U.S. technical experts demonstrated an Attribute Measurement System with an Information Barrier (AMSIB) for a delegation of Russian technical experts. The purpose of the demonstration was to show that attributes of a classified plutonium item of potential interest to arms control and nonproliferation transparency regimes could be ascertained without releasing any sensitive information. For this demonstration, both gamma-ray and neutron attributes were determined. We consider only the gamma-ray attributes here. The specific plutonium attributes measured were the isotopic ratio of {sup 240}Pu to {sup 239}Pu, the ''age'' of the plutonium (time elapsed since the most recent chemical purification of the plutonium), and the absence of plutonium oxide in the item's storage container. In this paper, we briefly review the technologies employed for the attribute measurements used in the gamma-ray portion of the demonstration, concentrating on the results of the test measurements of the isotopic and age attributes made on unclassified items.

  10. Actinide Targets for Neutron Cross Section Measurements (C)

    SciTech Connect

    J. D. Baker; C. A. McGrath

    2006-04-01

    The Advanced Fuel Cycle Initiative (AFCI) and the Generation IV Reactor Initiative have demonstrated a lack of detailed neutron cross-sections for certain "minor" actinides, those other than the most common (235U, 238U, and 239Pu). For some closed-fuel-cycle reactor designs more than 50% of reactivity will, at some point, be derived from “minor” actinides that currently have poorly known (n,g) and (n,f) cross sections. A program of measurements under AFCI has begun to correct this. One of the initial hurdles has been to produce well-characterized, highly isotopically enriched, and chemically pure actinide targets on thin backings. Using a combination of resurrected techniques and new developments, we have made a series of targets including highly enriched 240Pu, and 242Pu. Thus far, we have electrodeposited these actinide targets. In the future, we plan to study reductive distillation to achieve homogeneous, adherent targets on thin metal foils and polymer backings. As we move forward, separated isotopes become scarcer, and safety concerns become greater. The chemical purification and electodeposition techniques will be described.

  11. Alpha Coincidence Detection for the Assay of Actinides

    SciTech Connect

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

    2013-11-15

    Abstract – Interferences in both decay counting and mass counting techniques limit their application for some environmental monitoring applications. For example, 238U interferes with 238Pu in mass spectrometry measurements, while in conventional alpha spectroscopy measurements it is nearly impossible to separate 238Pu from 241Am and 239Pu from 240Pu. These interferences are typically resolved by using chemical separation and/or different measurement techniques for different isotopes. We are investigating radiation detector concepts to simultaneously assay these four isotopes with minimal sample preparation by exploiting radiation signatures measured in coincidence with the typical alpha decays of these isotopes. Particles in coincidence with the alpha decay include conversion electrons, gamma rays, x-rays, and Auger electrons. Each decay has a unique energy distribution enabling the separation of the isotopes. We are exploring two basic detector concepts to achieve these goals: a silicon-based design and a gas-detector design. The silicon system provides the potential for higher energy resolution at the cost of lower efficiency compared to a gas detector. In this paper, we will describe our evaluation of the different detector concepts, which will include detection efficiency, ability to resolve the isotopes, sample preparation and equipment requirements.

  12. 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.

  13. Apparatus and method for quantitative assay of generic transuranic wastes from nuclear reactors

    DOEpatents

    Caldwell, J.T.; Kunz, W.E.; Atencio, J.D.

    1982-03-31

    A combination of passive and active neutron measurements which yields quantitative information about the isotopic composition of transuranic wastes from nuclear power or weapons material manufacture reactors is described. From the measurement of prompt and delayed neutron emission and the incidence of two coincidentally emitted neutrons from induced fission of fissile material in the sample, one can quantify /sup 233/U, /sup 235/U and /sup 239/Pu isotopes in waste samples. Passive coincidence counting, including neutron multiplicity measurement and determination of the overall passive neutron flux additionally enables the separate quantitative evaluation of spontaneous fission isotopes such as /sup 240/Pu, /sup 244/Cm and /sup 252/Cf, and the spontaneous alpha particle emitter /sup 241/Am. These seven isotopes are the most important constituents of wastes from nuclear power reactors and once the mass of each isotope present is determined by the apparatus and method of the instant invention, the overall alpha particle activity can be determined to better than 1 nCi/g from known radioactivity data. Therefore, in addition to the quantitative analysis of the waste sample useful for later reclamation purposes, the alpha particle activity can be determined to decide whether permanent low-level burial is appropriate for the waste sample.

  14. Apparatus and method for quantitative assay of generic transuranic wastes from nuclear reactors

    DOEpatents

    Caldwell, John T.; Kunz, Walter E.; Atencio, James D.

    1984-01-01

    A combination of passive and active neutron measurements which yields quantitative information about the isotopic composition of transuranic wastes from nuclear power or weapons material manufacture reactors is described. From the measurement of prompt and delayed neutron emission and the incidence of two coincidentally emitted neutrons from induced fission of fissile material in the sample, one can quantify .sup.233 U, .sup.235 U and .sup.239 Pu isotopes in waste samples. Passive coincidence counting, including neutron multiplicity measurement and determination of the overall passive neutron flux additionally enables the separate quantitative evaluation of spontaneous fission isotopes such as .sup.240 Pu, .sup.244 Cm and .sup.252 Cf, and the spontaneous alpha particle emitter .sup.241 Am. These seven isotopes are the most important constituents of wastes from nuclear power reactors and once the mass of each isotope present is determined by the apparatus and method of the instant invention, the overall alpha particle activity can be determined to better than 1 nCi/g from known radioactivity data. Therefore, in addition to the quantitative analysis of the waste sample useful for later reclamation purposes, the alpha particle activity can be determined to decide whether "permanent" low-level burial is appropriate for the waste sample.

  15. Plutonium and uranium contamination in soils from former nuclear weapon test sites in Australia

    NASA Astrophysics Data System (ADS)

    Child, D. P.; Hotchkis, M. A. C.

    2013-01-01

    The British government performed a number of nuclear weapon tests on Australian territory from 1952 through to 1963 with the cooperation of the Australian government. Nine fission bombs were detonated in South Australia at Emu Junction and Maralinga, and a further three fission weapons were detonated in the Monte Bello Islands off the coast of Western Australia. A number of soil samples were collected by the Australian Radiation Laboratories in 1972 and 1978 during field surveys at these nuclear weapon test sites. They were analysed by gamma spectrometry and, for a select few samples, by alpha spectrometry to measure the remaining activities of fission products, activation products and weapon materials. We have remeasured a number of these Montebello Islands and Emu Junction soil samples using the ANTARES AMS facility, ANSTO. These samples were analysed for plutonium and uranium isotopic ratios and isotopic concentrations. Very low 240Pu/239Pu ratios were measured at both sites (∼0.05 for Alpha Island and ∼0.02 for Emu Field), substantially below global fallout averages. Well correlated but widely varying 236U and plutonium concentrations were measured across both sites, but 233U did not correlate with these other isotopes and instead showed correlation with distance from ground zero, indicating in situ production in the soils.

  16. Pu isotopes in soils collected downwind from Lop Nor: regional fallout vs. global fallout

    PubMed Central

    Bu, Wenting; Ni, Youyi; Guo, Qiuju; Zheng, Jian; Uchida, Shigeo

    2015-01-01

    For the first time, soil core samples from the Jiuquan region have been analyzed for Pu isotopes for radioactive source identification and radiological assessment. The Jiuquan region is in downwind from the Lop Nor Chinese nuclear test (CNT) site. The high Pu inventories (13 to 546 Bq/m2) in most of the sampling locations revealed that this region was heterogeneously contaminated by the regional fallout Pu from the CNTs. The contributions of the CNTs to the total Pu in soils were estimated to be more than 40% in most cases. The 240Pu/239Pu atom ratios in the soils ranged from 0.059 to 0.186 with an inventory-weighted average of 0.158, slightly lower than that of global fallout. This atom ratio could be considered as a mixed fingerprint of Pu from the CNTs. In addition, Pu in soils of Jiuquan region had a faster downward migration rate compared with other investigated places in China. PMID:26184740

  17. The Influence of Hydrothermal Plumes on the Distribution of Anthropogenic Radionuclides Between the Particulate and Dissolved Phases: Results from U.S. Geotraces Equatorial Pacific Zonal Transect GP16

    NASA Astrophysics Data System (ADS)

    Kenna, T. C.; Villa Alfageme, M.; Casacuberta Arola, N.; Masque, P.

    2014-12-01

    Here we present and discuss the results from the analysis of samples from selected stations collected on the US GEOTRACES Equatorial Pacific Zonal Transect (GP16) completed in 2013. The section, between Peru and Tahiti, encompasses a range of processes that influence the supply, removal, and internal cycling of trace metals and offers the opportunity to gain a better understanding of the drivers of the transport and fate of contaminants in the ocean. The capability to analyze water and filtered particulate samples in the quantities available, allows us to determine the partitioning of selected radionuclides among dissolved and particulate forms (Kd) and estimate Pu-particulate fluxes. The overarching objective of our work is to determine the concentrations of several anthropogenic radionuclides, including 239Pu, 240Pu, 237Np, and 137Cs with sufficient resolution to define their basin-wide distributions in the Pacific Ocean. Data collected in the East Pacific Rise hydrothermal plume allows a discussion on the partitioning behavior of plutonium and neptunium.

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

    PubMed

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

    2015-04-01

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

  19. Statistical signal processing and artificial intelligence applications in the nondestructive assay of U/Pu-bearing materials

    SciTech Connect

    Aumeier, S.E.; Forsmann, J.H.

    1998-09-01

    Over the years, a number of techniques have been developed to determine the quantity and distribution of radiative isotopes contained in given assay samples through the measurement and analysis of penetrating characteristic radiations. An active technique of particular utility when assaying samples containing very small quantities of fissionable material or when high-gamma-ray backgrounds are encountered is the delayed neutron nondestructive assay technique. The authors present the results of an analysis to evaluate the feasibility of using Kalman filters and genetic algorithms to determine multiple specific fissionable isotopic masses contained in an assay sample from a cumulative delayed neutron signal measured following neutron irradiation of the sample. Delayed neutron measurement data were generated to simulate the ideal response of the leached fuel clad monitor located at Argonne National Laboratory-West. The simulated measurement data were generated by calculating the cumulative delayed neutron count following the irradiation of a sample containing 5.9 g {sup 238}U, 9.8 g {sup 235}U, 16.9 G {sup 239}Pu, and 3.1 g {sup 240}Pu. Data were simulated for {approximately} 14-MeV neutron irradiation and irradiation with a moderated neutron beam with average neutron energy of {approximately} 200 eV, which yields a larger fissile/fertile fission ratio than the 14-MeV irradiation.

  20. Mercuric iodide room-temperature array detectors for gamma-ray imaging

    SciTech Connect

    Patt, B.

    1994-11-15

    Significant progress has been made recently in the development of mercuric iodide detector arrays for gamma-ray imaging, making real the possibility of constructing high-performance small, light-weight, portable gamma-ray imaging systems. New techniques have been applied in detector fabrication and then low noise electronics which have produced pixel arrays with high-energy resolution, high spatial resolution, high gamma stopping efficiency. Measurements of the energy resolution capability have been made on a 19-element protypical array. Pixel energy resolutions of 2.98% fwhm and 3.88% fwhm were obtained at 59 keV (241-Am) and 140-keV (99m-Tc), respectively. The pixel spectra for a 14-element section of the data is shown together with the composition of the overlapped individual pixel spectra. These techniques are now being applied to fabricate much larger arrays with thousands of pixels. Extension of these principles to imaging scenarios involving gamma-ray energies up to several hundred keV is also possible. This would enable imaging of the 208 keV and 375-414 keV 239-Pu and 240-Pu structures, as well as the 186 keV line of 235-U.

  1. Resuspension and atmospheric transport of radionuclides due to wildfires near the Chernobyl Nuclear Power Plant in 2015: An impact assessment.

    PubMed

    Evangeliou, N; Zibtsev, S; Myroniuk, V; Zhurba, M; Hamburger, T; Stohl, A; Balkanski, Y; Paugam, R; Mousseau, T A; Møller, A P; Kireev, S I

    2016-05-17

    In April and August 2015, two major fires in the Chernobyl Exclusion Zone (CEZ) caused concerns about the secondary radioactive contamination that might have spread over Europe. The present paper assessed, for the first time, the impact of these fires over Europe. About 10.9 TBq of (137)Cs, 1.5 TBq of (90)Sr, 7.8 GBq of (238)Pu, 6.3 GBq of (239)Pu, 9.4 GBq of (240)Pu and 29.7 GBq of (241)Am were released from both fire events corresponding to a serious event. The more labile elements escaped easier from the CEZ, whereas the larger refractory particles were removed more efficiently from the atmosphere mainly affecting the CEZ and its vicinity. During the spring 2015 fires, about 93% of the labile and 97% of the refractory particles ended in Eastern European countries. Similarly, during the summer 2015 fires, about 75% of the labile and 59% of the refractory radionuclides were exported from the CEZ with the majority depositing in Belarus and Russia. Effective doses were above 1 mSv y(-1) in the CEZ, but much lower in the rest of Europe contributing an additional dose to the Eastern European population, which is far below a dose from a medical X-ray.

  2. Complementary technologies for verification of excess plutonium

    SciTech Connect

    Langner, , D.G.; Nicholas, N.J.; Ensslin, N.; Fearey, B.L.; Mitchell, D.J.; Marlow, K.W.; Luke, S.J.; Gosnell, T.B.

    1998-12-31

    Three complementary measurement technologies have been identified as candidates for use in the verification of excess plutonium of weapons origin. These technologies: high-resolution gamma-ray spectroscopy, neutron multiplicity counting, and low-resolution gamma-ray spectroscopy, are mature, robust technologies. The high-resolution gamma-ray system, Pu-600, uses the 630--670 keV region of the emitted gamma-ray spectrum to determine the ratio of {sup 240}Pu to {sup 239}Pu. It is useful in verifying the presence of plutonium and the presence of weapons-grade plutonium. Neutron multiplicity counting is well suited for verifying that the plutonium is of a safeguardable quantity and is weapons-quality material, as opposed to residue or waste. In addition, multiplicity counting can independently verify the presence of plutonium by virtue of a measured neutron self-multiplication and can detect the presence of non-plutonium neutron sources. The low-resolution gamma-ray spectroscopic technique is a template method that can provide continuity of knowledge that an item that enters the a verification regime remains under the regime. In the initial verification of an item, multiple regions of the measured low-resolution spectrum form a unique, gamma-radiation-based template for the item that can be used for comparison in subsequent verifications. In this paper the authors discuss these technologies as they relate to the different attributes that could be used in a verification regime.

  3. Using anisotropies in prompt fission neutron coincidences to assess the neutron multiplication of highly multiplying subcritical plutonium assemblies

    NASA Astrophysics Data System (ADS)

    Mueller, J. M.; Mattingly, J.

    2016-07-01

    There is a significant and well-known anisotropy between the prompt neutrons emitted from a single fission event; these neutrons are most likely to be observed at angles near 0° or 180° relative to each other. However, the propagation of this anisotropy through different generations of a fission chain reaction has not been previously studied. We have measured this anisotropy in neutron-neutron coincidences from a subcritical highly-multiplying assembly of plutonium metal. The assembly was a 4.5 kg α-phase plutonium metal sphere composed of 94% 239Pu and 6% 240Pu by mass. Data were collected using two EJ-309 liquid scintillators and two EJ-299 plastic scintillators. The angular distribution of neutron-neutron coincidences was measured at 90° and 180° and found to be largely isotropic. Simulations were performed using MCNPX-PoliMi of similar plutonium metal spheres of varying sizes and a correlation between the neutron multiplication of the assembly and the anisotropy of neutron-neutron coincidences was observed. In principle, this correlation could be used to assess the neutron multiplication of an unknown assembly.

  4. Pu isotopes in soils collected downwind from Lop Nor: regional fallout vs. global fallout.

    PubMed

    Bu, Wenting; Ni, Youyi; Guo, Qiuju; Zheng, Jian; Uchida, Shigeo

    2015-07-17

    For the first time, soil core samples from the Jiuquan region have been analyzed for Pu isotopes for radioactive source identification and radiological assessment. The Jiuquan region is in downwind from the Lop Nor Chinese nuclear test (CNT) site. The high Pu inventories (13 to 546 Bq/m(2)) in most of the sampling locations revealed that this region was heterogeneously contaminated by the regional fallout Pu from the CNTs. The contributions of the CNTs to the total Pu in soils were estimated to be more than 40% in most cases. The (240)Pu/(239)Pu atom ratios in the soils ranged from 0.059 to 0.186 with an inventory-weighted average of 0.158, slightly lower than that of global fallout. This atom ratio could be considered as a mixed fingerprint of Pu from the CNTs. In addition, Pu in soils of Jiuquan region had a faster downward migration rate compared with other investigated places in China.

  5. Resuspension and atmospheric transport of radionuclides due to wildfires near the Chernobyl Nuclear Power Plant in 2015: An impact assessment

    NASA Astrophysics Data System (ADS)

    Evangeliou, N.; Zibtsev, S.; Myroniuk, V.; Zhurba, M.; Hamburger, T.; Stohl, A.; Balkanski, Y.; Paugam, R.; Mousseau, T. A.; Møller, A. P.; Kireev, S. I.

    2016-05-01

    In April and August 2015, two major fires in the Chernobyl Exclusion Zone (CEZ) caused concerns about the secondary radioactive contamination that might have spread over Europe. The present paper assessed, for the first time, the impact of these fires over Europe. About 10.9 TBq of 137Cs, 1.5 TBq of 90Sr, 7.8 GBq of 238Pu, 6.3 GBq of 239Pu, 9.4 GBq of 240Pu and 29.7 GBq of 241Am were released from both fire events corresponding to a serious event. The more labile elements escaped easier from the CEZ, whereas the larger refractory particles were removed more efficiently from the atmosphere mainly affecting the CEZ and its vicinity. During the spring 2015 fires, about 93% of the labile and 97% of the refractory particles ended in Eastern European countries. Similarly, during the summer 2015 fires, about 75% of the labile and 59% of the refractory radionuclides were exported from the CEZ with the majority depositing in Belarus and Russia. Effective doses were above 1 mSv y‑1 in the CEZ, but much lower in the rest of Europe contributing an additional dose to the Eastern European population, which is far below a dose from a medical X-ray.

  6. Resuspension and atmospheric transport of radionuclides due to wildfires near the Chernobyl Nuclear Power Plant in 2015: An impact assessment

    PubMed Central

    Evangeliou, N.; Zibtsev, S.; Myroniuk, V.; Zhurba, M.; Hamburger, T.; Stohl, A.; Balkanski, Y.; Paugam, R.; Mousseau, T. A.; Møller, A. P.; Kireev, S. I.

    2016-01-01

    In April and August 2015, two major fires in the Chernobyl Exclusion Zone (CEZ) caused concerns about the secondary radioactive contamination that might have spread over Europe. The present paper assessed, for the first time, the impact of these fires over Europe. About 10.9 TBq of 137Cs, 1.5 TBq of 90Sr, 7.8 GBq of 238Pu, 6.3 GBq of 239Pu, 9.4 GBq of 240Pu and 29.7 GBq of 241Am were released from both fire events corresponding to a serious event. The more labile elements escaped easier from the CEZ, whereas the larger refractory particles were removed more efficiently from the atmosphere mainly affecting the CEZ and its vicinity. During the spring 2015 fires, about 93% of the labile and 97% of the refractory particles ended in Eastern European countries. Similarly, during the summer 2015 fires, about 75% of the labile and 59% of the refractory radionuclides were exported from the CEZ with the majority depositing in Belarus and Russia. Effective doses were above 1 mSv y−1 in the CEZ, but much lower in the rest of Europe contributing an additional dose to the Eastern European population, which is far below a dose from a medical X-ray. PMID:27184191

  7. DEVELOPMENT OF AN IMPROVED TITANATE-BASED SORBENT FOR STRONTIUM AND ACTINIDE SEPARATIONS UNDER STRONGLY ALKALINE CONDITIONS

    SciTech Connect

    Hobbs, D.; Peters, T.; Taylor-Pashow, K.; Fink, S.

    2010-02-18

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 134,137}Cs, {sup 90}Sr, and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. Separation processes at SRS include the sorption of {sup 90}Sr and alpha-emitting radionuclides onto monosodium titanate (MST) and caustic side solvent extraction of {sup 137}Cs. The MST and separated {sup 137}Cs is encapsulated along with the sludge fraction of high-level waste (HLW) into a borosilicate glass waste form for eventual entombment at a federal repository. The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes {sup 238}Pu, {sup 239}Pu, and {sup 240}Pu; {sup 237}Np; and uranium isotopes, {sup 235}U and {sup 238}U. This paper describes recent results evaluating the performance of an improved sodium titanate material that exhibits increased removal kinetics and capacity for {sup 90}Sr and alpha-emitting radionuclides compared to the current baseline material, MST.

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

    PubMed

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

    2010-03-01

    Since the first nuclear weapons tests in the 1940s, pulsed inputs of plutonium isotopes have served as excellent tracers for understanding sources, pathways, dynamics and the fate of pollutants and particles in the marine environment. Due to the well-defined spatial and temporal inputs of Pu, the long half-lives of (240)Pu and (239)Pu and its unique chemical properties, Pu is a potential tracer for various physical and biogeochemical ocean processes, including circulation, sedimentation and biological productivity, and hence a means of assessing the impacts of global climate change. Due to the source dependency of the Pu isotopic signature, plutonium isotopes are beginning to be exploited as tools for the evaluation and improvement of regional and global ocean models that will enhance understanding of past and future changes in the oceans. This paper addresses the major sources of Pu and the physical and biogeochemical behaviour in the marine environment. Finally, the use of Pu isotopes as tracers for various oceanic processes (e.g. water mass transport, particle export, and sedimentation) is considered. PMID:19773079

  9. Estimation of Radiation Doses in the Marshall Islands Based on Whole Body Counting of Cesium-137 (137Cs) and Plutonium Urinalysis

    SciTech Connect

    Daniels, J; Hickman, D; Kehl, S; Hamilton, T

    2007-06-11

    measurement. The amount of {sup 137}Cs detected is often reported in activity units of kilo-Becquerel (kBq), where 1 kBq equals 1000 Bq and 1 Bq = 1 nuclear transformation per second (t s{sup -1}). [However, in the United States the Curie (Ci) continues to be used as the unit of radioactivity; where 1 Ci = 3.7 x 10{sup 10} Bq.] The detection of {sup 239}Pu and {sup 240}Pu in bioassay (urine) samples indicates the presence of internally deposited (systemic) plutonium in the body. Urine samples that are collected in the Marshall Islands from volunteers participating in the RSMP are transported to LLNL, where measurements for {sup 239+240}Pu are performed using a state-of-the-art technology based on Accelerator Mass Spectrometry (AMS) (Hamilton et al., 2004, 2007; Brown et al., 2004). The urinary excretion of plutonium by RSMP volunteers is usually described in activity units, expressed as micro-Becquerel ({micro}Bq) of {sup 239+240}Pu (i.e., representing the sum of the {sup 239}Pu and {sup 240}Pu activity) excreted (lost) per day (d{sup -1}), where 1 {micro}Bq d{sup -1} = 10{sup -6} Bq d{sup -1} and 1 Bq = 1 t s{sup -1}. The systemic burden of plutonium is then estimated from biokinetic relationships as described by the International Commission on Radiological Protection (e.g., see ICRP, 1990). In general, nuclear transformations are accompanied by the emission of energy and/or particles in the form of gamma rays ({gamma}), beta particles ({beta}), and/or alpha particles ({alpha}). Tissues in the human body may adsorb these emissions, where there is a potential for any deposited energy to cause biological damage. The general term used to quantify the extent of any radiation exposure is referred to as the dose. The equivalent dose is defined by the average absorbed dose in an organ or tissue weighted by the average quality factor for the type and energy of the emission causing the dose. The effective dose equivalent (EDE; as applied to the whole body), is the sum of the average

  10. INL Capabilities For Nuclear Data Measurements Using The Argonne Intense Pulsed Neutron Source Facility

    SciTech Connect

    R. Aryaeinejad; D. W. Nigg; R.V.F. Janssens; B. J. Micklich; G. Ter-Akopian; J. D. Cole

    2005-07-01

    The relevant facts concerning the Argonne National Laboratory – Intense Pulsed Neutron Source (ANL/IPNS) and the Idaho National Laboratory (INL) apparatus for use at the ANL/IPNS facility to measure differential neutron interaction cross sections of interest for advanced reactor physics applications are presented. The INL apparatus, which consists of an array of multiple types of multiple detectors operated in coincidence, signal electronics, and a data acquisition system, is presented as an application of new means and methods to measure the relevant parameters described. The immediate measurement goals involve measurement of neutron induced interaction cross sections for 240Pu and 242Pu with 241Pu, 241Am, with measurements for other nuclides of interest for advanced reactor physics applications to follow later. Specific uncertainties and error limits are presented and methods for controlling these uncertainties are described. The post experiment analysis using data sorts and data selection from a large, self-consistent data set to produce spectra that will be analyzed for direct results and used to determine cross sections is also discussed.

  11. Development of the NIST bone ash standard reference material for environmental radioactivity measurement.

    PubMed

    Lin, Z; Inn, K G; Altzitzoglou, T; Arnold, D; Cavadore, D; Ham, G J; Korun, M; Wershofen, H; Takata, Y; Young, A

    1998-01-01

    The bone ash standard reference material (SRM), a blend of 4% contaminated human bone and 96% diluent bovine bone, has been developed for radiochemical method validation and quality control for radio-bone analysis. The massic activities of 90Sr, 226Ra, 230Th, 232Th, 234U, 235U, 238U, 238Pu, (239 + 240)Pu and (243 + 244)Cm were certified using a variety of radiochemical procedures and detection methods. Measurements confirmed undetectable radionuclide heterogeneity down to a sample size of 5 g. thereby implying adequate blending of particulate materials with dilution factors of up to 17,900. The results among most of the intercomparison laboratories and their methods were consistent. Disequilibrium was observed for decay chains: 234U(0.67 mBq/g)-230Th(0.47 mBq/g)-226Ra(15.1 mBq/g)-210Pb(23 mBq/g)-210Po(13 mBq/g) and 232Th(0.99 mBq/g)-228 Ra(6.1 mBq/g)-228Th(7.1 mBq/g). The disequilibria were the results of mixing occupationally contaminated human bone with natural bovine bone and the fractionation during internal biological processes. The massic activity of 210Pb, 228Th and 241Am were not certified because of insufficient 228Ra and 241Pu data and lack of knowledge in how 222Rn and its daughters will be fractionated in the SRM bottle over time.

  12. Elemental bio-imaging of thorium, uranium, and plutonium in tissues from occupationally exposed former nuclear workers.

    PubMed

    Hare, Dominic; Tolmachev, Sergei; James, Anthony; Bishop, David; Austin, Christine; Fryer, Fred; Doble, Philip

    2010-04-15

    Internal exposure from naturally occurring radionuclides (including the inhaled long-lived actinides (232)Th and (238)U) is a component of the ubiquitous background radiation dose (National Council on Radiation Protection and Measurements. Ionizing radiation exposure of the population of the United States; NCRP Report No. 160; NCRP: Bethesda, MD, 2009). It is of interest to compare the concentration distribution of these natural alpha-emitters in the lungs and respiratory lymph nodes with those resulting from occupational exposure, including exposure to anthropogenic plutonium and depleted and enriched uranium. This study examines the application of laser ablation-inductively coupled plasma-mass spectrometry (LA-ICPMS) to quantifying and visualizing the mass distribution of uranium and thorium isotopes from both occupational and natural background exposure in human respiratory tissues and, for the first time, extends this application to the direct imaging of plutonium isotopes. Sections of lymphatic and lung tissues taken from deceased former nuclear workers with a known history of occupational exposure to specific actinide elements (uranium, plutonium, or americium) were analyzed by LA-ICPMS. Using a previously developed LA-ICPMS protocol for elemental bio-imaging of trace elements in human tissue and a new software tool, we generated images of thorium ((232)Th), uranium ((235)U and (238)U), and plutonium ((239)Pu and (240)Pu) mass distributions in sections of tissue. We used a laboratory-produced matrix-matched standard to quantify the (232)Th, (235)U, and (238)U concentrations. The plutonium isotopes (239)Pu and (240)Pu were detected by LA-ICPMS in 65 mum diameter localized regions of both a paratracheal lymph node and a sample of lung tissue from a person who was occupationally exposed to refractory plutonium (plutonium dioxide). The average (overall) (239)Pu concentration in the lymph node was 39.2 ng/g, measured by high purity germanium (HPGe) gamma

  13. Recoil Based Fuel Breeding Fuel Structure

    SciTech Connect

    Popa-Simil, Liviu

    2008-07-01

    Nuclear transmutation reactions are based on the absorption of a smaller particle as neutron, proton, deuteron, alpha, etc. The resulting compound nucleus gets out of its initial lattice mainly by taking the recoil, also with help from its sudden change in chemical properties. The recoil implantation is used in correlation with thin and ultra thin materials mainly for producing radiopharmaceuticals and ultra-thin layer radioactive tracers. In nuclear reactors, the use of nano-particulate pellets could facilitate the recoil implantation for breeding, transmutation and partitioning purposes. Using enriched {sup 238}U or {sup 232}Th leads to {sup 239}Pu and {sup 233}U production while using other actinides as {sup 240}Pu, {sup 241