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Sample records for 240pu 241pu 242pu

  1. 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

  2. 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 ).

  3. 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

  4. 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.

  5. 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.

  6. 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

  7. 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.

  8. 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.

  9. 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

  10. 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.

  11. 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

  12. 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.

  13. 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.

  14. Actinides produced by /sup 12/C + /sup 242/Pu and /sup 16/O + /sup 238/U reactions

    SciTech Connect

    Shinohara, N.; Usuda, S.; Ichikawa, S.; Suzuki, T.; Magara, M.; Okashita, H.; Yoshikawa, H.; Horiguchi, T.; Iwata, Y.; Shibata, S.; and others

    1986-09-01

    The cross sections for /sup 250/Fm, /sup 244-246/Cf, /sup 242-244/Cm, and /sup 242/Am/sup g-italic/ produced by the /sup 12/C+ /sup 242/Pu and the /sup 16/O+ /sup 238/U reactions leading to the same compound nucleus of /sup 254/Fm have been measured by using radiochemical methods. The excitation functions show that the difference between the /sup 12/C+ /sup 242/Pu and the /sup 16/O+ /sup 238/U reactions can be attributed mainly to the Coulomb barriers. Our results were compared with others reported previously for /sup 22/Ne+ /sup 232/Th, /sup 12/C+ /sup 238/U, /sup 12/C+ /sup 240,241/Pu, /sup 13/C+ /sup 241/Pu, /sup 16/O+ /sup 233/U, and /sup 16/O+ /sup 242/Pu reaction systems, and support a mechanism involving transfer of ..cap alpha..-particle clusters (C,Be,He) from projectile to target for the production of Cf and Cm isotopes.

  15. 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

  16. 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

  17. Measurement of the 242Pu neutron capture cross section

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

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

  18. 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.

  19. 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

  20. 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.

  1. Consistent Data Assimilation of Isotopes: 242Pu and 105Pd

    SciTech Connect

    G. Palmiotti; H. Hiruta; M. Salvatores

    2012-09-01

    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 are analyzed using the EMPIRE evaluated files for 242Pu and 105Pd. In particular irradiation experiments (PROFIL-1 and -2, TRAPU-1, -2 and -3) provide information about capture cross sections, and a critical configuration, COSMO, where fission spectral indexes were measured, provides information about fission cross section. The observed discrepancies between calculated and experimental results are used in conjunction with the computed sensitivity coefficients and covariance matrix for nuclear parameters in a consistent data assimilation. The results obtained by the consistent data assimilation indicate that not so large modifications on some key identified nuclear parameters allow to obtain reasonable C/E. However, for some parameters such variations are outside the range of 1 s of their initial standard deviation. This can indicate a possible conflict between differential measurements (used to calculate the initial standard deviations) and the integral measurements used in the statistical data adjustment. Moreover, an inconsistency between the C/E of two sets of irradiation experiments (PROFIL and TRAPU) is observed for 242Pu. This is the end of this project funded by the Nuclear Physics Program of the DOE Office of Science. We can indicate that a proof of principle has been demonstrated for a few isotopes for this innovative methodology. However, we are still far from having explored all the possibilities and made this methodology to be considered proved and robust. In particular many issues are worth further investigation: • Non-linear effects • Flexibility of nuclear parameters in describing cross sections • Multi-isotope consistent assimilation • Consistency between differential and integral

  2. Neutron-induced fission cross sections of 242Pu from 0.3 MeV to 3 MeV

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

    The majority of the next generation of nuclear power plants (GEN-IV) will work in the fast-neutron-energy region, as opposed to present day thermal reactors. This leads to new and more accurate nuclear-data needs for some minor actinides and structural materials. Following those upcoming demands, the Organisation for Economic Cooperation and Development Nuclear Energy Agency performed a sensitivity study. Based on the latter, an improvement in accuracy from the present 20% to 5% is required for the 242Pu(n ,f ) cross section. Within the same project both the 240Pu(n ,f ) cross section and the 242Pu(n ,f ) cross section were measured at the Van de Graaff accelerator of the Joint Research Centre at the Institute for Reference Materials and Measurements, where quasimonoenergetic neutrons were produced in an energy range from 0.3 MeV up to 3 MeV. A twin Frisch-grid ionization chamber has been used in a back-to-back configuration as fission-fragment detector. The 242Pu(n ,f ) cross section has been normalized to three different isotopes: 237Np(n ,f ) , 235U(n ,f ) , and 238U(n ,f ) . A comprehensive study of the corrections applied to the data and the uncertainties associated is given. The results obtained are in agreement with previous experimental data at the threshold region up to 0.8 MeV. The resonance-like structure at 0.8 to 1.1 MeV, visible in the evaluations and in most previous experimental values, was not reproduced with the same intensity in this experiment. For neutron energies higher than 1.1 MeV, the results of this experiment are slightly lower than the Evaluated Nuclear Data File/B-VII.1 evaluation but in agreement with the experiment of Tovesson et al. (2009) as well as Staples and Morley (1998). Finally, for energies above 1.5 MeV, the results show consistency with the present evaluations.

  3. 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.

  4. 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.

  5. Absolute measurement of the 242Pu neutron-capture cross section

    DOE PAGES

    Buckner, M. Q.; Wu, C. Y.; Henderson, R. A.; Bucher, B.; Chyzh, A.; Bredeweg, T. A.; Baramsai, B.; Couture, A.; Jandel, M.; Mosby, S.; et al

    2016-04-21

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

  6. Absolute measurement of the 242Pu neutron-capture cross section

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

  7. Determination of the 242Pu Branching Ratio via Alpha-Gamma Coincidence

    SciTech Connect

    Wang, T F

    2012-05-24

    When the burn-up is high, the {sup 242}Pu isotopic content becomes more important. The traditional correlation method will fail. The {sup 242}Pu isotopic content in the sample plays an essential role if the neutron coincidence method is used to quantify the total amount of plutonium. In one of the earlier measurements we had a chance to measure an isotopic pure (> 99.95 %) {sup 242}Pu thick sample and realized that the difference in the branching ratio (BR) value among current nuclear data3) for the two important gamma-rays at 103.5-keV and 158.8-keV. In this study, the thick sample was counted on a 15% ORTEC safeguards type HPGe to further improve BR determination of the 159-keV gamma-ray. Furthermore, we have made a thin {sup 242}Pu sample from the thick sample and performed alpha-gamma coincidence measurements. Our preliminary gamma-ray BR results are 4.37(6) E-4, 2.79(8) E-5, and 2.25(8) E-6 for 44.9-keV, 103.5-keV, and 158.9-keV, respectively.

  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. 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.

  10. New Superheavy Element Isotopes: 242Pu(48Ca,5n)285114

    SciTech Connect

    Ellison, Paul A; Gregorich, Kenneth E.; Berryman, Jill S.; Bleuel, Darren L.; Clark, Roderick M.; Dragojevic, Irena; Dvorak, Jan; Fallon, Paul; Fineman-Sotomayor, Carolina; Gates, Jacklyn M.; Gothe, Oliver R.; Lee, I-Yang; Loveland, Walter D.; McLaughlin, Joseph P.; Paschalis, Stefanos; Petri, Marina-Kalliopi; Qian, Jing; Stavsetra, Liv; Wiedeking, Mathis; Nitsche, Heino

    2010-10-22

    The new, neutron-deficient, superheavy element isotope {sup 285}114 was produced in {sup 48}Ca irradiations of {sup 242}Pu targets at a center-of-target beam energy of 256 MeV (E* = 50 MeV). The {alpha} decay of {sup 285}114 was followed by the sequential {alpha} decay of four daughter nuclides, {sup 281}Cn, {sup 277}Ds, {sup 273}Hs, and {sup 269}Sg. {sup 265}Rf was observed to decay by spontaneous fission. The measured {alpha}-decay Q values were compared with those from a macroscopic-microscopic nuclear mass model to give insight into superheavy element shell effects. The {sup 242}Pu({sup 48}Ca,5n){sup 285}114 cross section was 0.6{sub -0.5}{sup +0.9} pb.

  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.

  12. 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

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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

  18. 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.

  19. 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.

  20. 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.

  1. 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.

  2. 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

  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. New measurement of the 242Pu(n,γ) cross section at n_TOF

    NASA Astrophysics Data System (ADS)

    Lerendegui-Marco, J.; Guerrero, C.; Cortés-Giraldo, M. A.; Quesada, J. M.; Mendoza, E.; Cano-Ott, D.; Eberhardt, K.; Junghans, A.

    2016-03-01

    The use of MOX fuel (mixed-oxide fuel made of UO2 and PuO2) in nuclear reactors allows substituting a large fraction of the enriched Uranium by Plutonium reprocessed from spent fuel. With the use of such new fuel composition rich in Pu, a better knowledge of the capture and fission cross sections of the Pu isotopes becomes very important. In particular, a new series of cross section evaluations have been recently carried out jointly by the European (JEFF) and United States (ENDF) nuclear data agencies. For the case of 242Pu, the two only neutron capture time-of-flight measurements available, from 1973 and 1976, are not consistent with each other, which calls for a new time-of flight capture cross section measurement. In order to contribute to a new evaluation, we have perfomed a neutron capture cross section measurement at the n_TOF-EAR1 facility at CERN using four C6D6 detectors, using a high purity target of 95 mg. The preliminary results assessing the quality and limitations (background, statistics and γ-flash effects) of this new experimental data are presented and discussed, taking into account that the aimed accuracy of the measurement ranges between 7% and 12% depending on the neutron energy region.

  6. 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.

  7. 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

  8. 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.

  9. 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.

  10. 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.

  11. 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

  12. 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.

  13. 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.

  14. 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.

  15. 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

  16. 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).

  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. 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.

  19. 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

  20. 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

  1. 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

  2. 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.

  3. 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.

  4. 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

  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. 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}.

  7. 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

  8. 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

  9. 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.

  10. 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

  11. 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

  12. 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

  13. 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.

  14. 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

  15. 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.

  16. 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.

  17. 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).

  18. 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

  19. 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.

  20. 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.

  1. 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.

  2. 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

  3. 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.

  4. 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.

  5. 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

  6. 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.

  7. 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

  8. 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.

  9. Experimental re-evaluation of the γ-ray energy and emission probability for the 159 keV transition in 238U following the α-decay of 242Pu.

    PubMed

    Berlizov, A N; van Belle, P; Zuleger, E; Ottmar, H

    2011-02-01

    Because of the very low specific activity of (242)Pu, the non-destructive assay of this isotope by means of conventional high-resolution gamma-spectrometry (HRGS) is possible only for Pu samples highly rich in (242)Pu. For bulk samples suffering from the gamma self-attenuation and self-fluorescence effects, the only practical choice for the quantitative analysis of (242)Pu is the weak γ-line emitted in the 159 keV transition of its α-decay daughter (238)U. A recent study revealed a significant disagreement between the (242)Pu mass values in a 99.72% enriched (242)PuO(2) sample as reported by HRGS and neutron coincidence counting. This fact motivated the present study on the experimental re-evaluation of the γ-emission probability for the 159 keV transition using a combination of α-, γ- and mass-spectrometry techniques. The obtained new emission probability P(2)=(2.20±0.08)10(-6) turned out to be ≈35% smaller than the currently adopted value. The study also suggested a new value E(2)=159.018±0.016 keV for the energy of the respective γ-ray.

  10. 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.

  11. 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

  12. (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

  13. (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.

  14. [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

  15. [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.

  16. 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.

  17. 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.

  18. 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.

  19. 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.

  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. PMID:3570788

  1. 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

  2. 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

  3. 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.

  4. 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.

  5. Method for determination of neptunium in large-sized urine samples using manganese dioxide coprecipitation and 242Pu as yield tracer.

    PubMed

    Qiao, Jixin; Hou, Xiaolin; Roos, Per

    2013-02-01

    A novel method for bioassay of large volumes of human urine samples using manganese dioxide coprecipitation for preconcentration was developed for rapid determination of (237)Np. (242)Pu was utilized as a nonisotopic tracer to monitor the chemical yield of (237)Np. A sequential injection extraction chromatographic (SI-EC) system coupled with inductively coupled plasma mass spectrometry (ICPMS) was exploited to facilitate the rapid column separation and quantification. The analytical results demonstrated satisfactory performance of the MnO(2) coprecipitation as indicated by the high chemical yields close to 100% and high separation capacity of processing up to 5 L of human urine samples. The MnO(2) coprecipitation process is simple and straightforward in which a batch (8-12) of samples can be pretreated within 4 h (i.e., <0.5 h/sample). In connection with the automated column separation and ICPMS quantification, which takes less than 1.5 h in total, the overall analytical time was on average less than 2 h for each sample. The high effectiveness and sample throughput make the developed method well suited for urine bioassay of (237)Np in routine monitoring of occupationally internal radiation exposure and rapid analysis of neptunium contamination level for emergency preparedness.

  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. 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.

  9. 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.

  10. 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

  11. 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.

  12. 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.

  13. 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.

  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. 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.

  17. [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.

  18. 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

  19. 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.

  20. 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

  1. 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

  2. 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.

  3. 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.

  4. 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.

  5. 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%.

  6. 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.

  7. 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.

  8. 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

  9. 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.

  10. Plutonium isotopic determination from gamma-ray spectra

    SciTech Connect

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

    1998-12-31

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

  11. 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.

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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%.

  17. 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.

  18. 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.

  19. 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.

  20. 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

  1. 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

  2. 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.

  3. 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.

  4. Measurement of Neutron Induced and Spontaneous Fission in Pu-242 at DANCE

    NASA Astrophysics Data System (ADS)

    Chyzh, Andrii; Wu, C. Y.; Henderson, R.; Couture, A.; Lee, H. Y.; Ullmann, J.; O'Donnell, J. M.; Jandel, M.; Haight, R. C.; Bredeweg, T. A.; Dance Collaboration

    2013-10-01

    Neutron capture and fission reactions are important in nuclear engineering and physics. DANCE (Detector for Advanced Neutron Capture Measurement, LANL) combined with PPAC (avalanche technique based fission tagging detector, LLNL) were used to study neutron induced and spontaneous fission in 242Pu. 2 measurements were performed in 2013. The first experiment was done without the incident neutron beam with the fission tagging ability to study γ-rays emitted in the spontaneous fission of 242Pu. The second one - with the neutron beam to measure both the neutron capture and fission reactions. This is the first direct measurement of prompt fission γ-rays in 242Pu. The γ-ray multiplicity, γ-ray energy, and total energy of γ-rays per fission in 242Pu will be presented. These distributions of the 242Pu spontaneous fission will be compared to those in the 241Pu neutron induced fission. This work was performed under the auspices of the US Department of Energy by Los Alamos National Laboratory under Contract DE-AC52-06NA25396 and Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.

  5. 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.

  6. 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-size LMFBRs. As a benchmark, ZPR-6/7 was devoid of many 'real' reactor features, such as simulated control rods and multiple enrichment zones, in its reference form. Those kinds of features were investigated experimentally in variants of the reference ZPR-6/7 or in other critical assemblies in the Demonstration Reactor Benchmark Program.

  7. 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.

  8. /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)

  9. 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.

  10. 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

  11. 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.

  12. 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

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

    PubMed Central

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

    2012-01-01

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

  14. 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

  15. 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.

  16. 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.

  17. 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

  18. 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.

  19. 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.

  20. 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.

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

    SciTech Connect

    Beasley, T. M.

    1982-01-01

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

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

    PubMed

    Hrnecek, E; Steier, P; Wallner, A

    2005-01-01

    Environmental samples from nuclear weapons test sites at the atolls of Mururoa and Fangataufa (French Polynesia, south Pacific) have been analyzed for their content of plutonium isotopes by applying the independent techniques of decay counting (Alpha Spectrometry) and accelerator mass spectrometry (AMS). Here, we propose the combination of both techniques which results in a maximum of information on the isotopic signature of Pu in environmental samples. Plutonium was chemically separated from the bulk material by anion exchange. (242)Pu was used as an internal standard for both AMS and alpha spectrometry. The samples for alpha spectrometry were prepared by micro-precipitation with NdF(3). After alpha spectrometry, the samples were reprocessed for AMS. Pu was co-precipitated with Fe(OH)(3) and finally, solid samples were prepared. At the VERA (Vienna Environmental Research Accelerator) facility, the various Pu isotopes were separated by their isotopic masses and quantified by the AMS technique. A good agreement of the results obtained from the AMS measurements was found with those obtained from Alpha Spectrometry. Overall, the data agree on average within 10% of each other. Isotope ratios for (238)Pu, (239)Pu and (240)Pu can be extracted from our investigations. Alpha spectrometry delivers data for the (238)Pu and the combination of ((239+240))Pu concentrations in those samples. In addition, the AMS technique provides information on the individual concentrations of (240)Pu and (239)Pu. PMID:15982894

  3. Effect of precipitation, sorption and stable of isotope on maximum release rates of radionuclides from engineered barrier system (EBS) in deep repository.

    PubMed

    Malekifarsani, A; Skachek, M A

    2009-10-01

    shown that the concentrations of the following radionuclides are limited by solubility and precipitate around the waste and buffer: U, Np, Ra, Sm, Zr, Se, Tc, and Pd. The Sensitivity of maximum release rates in case precipitation shows that some nuclides such as Cs-135, Nb-94, Nb-93 m, Zr-93, Sn-126, Th-230, Pu-240, Pu-242, Pu-239, Cm-245, Am-243, Cm-245, U-233, Ac-227, Pb-210, Pa-231 and Th-229 are very little changed in case the maximum release rate from EBS corresponding to eliminate precipitation in buffer material. Some nuclides such as Se-79, Tc-99, Pd-107, Th-232, U-236, U-233, Ra-226, Np-237 U-235, U-234, and U-238 are virtually changed in the maximum release rate compared to case that taking account precipitation. In Sensitivity of maximum release rates in case to taking account stable isotopes (according to the table of inventory) there are only some nuclides with their stable isotopes in the vitrified waste. And calculation shows that Pd-107 and Se-79 are very increase in case eliminate stable isotope. The Sensitivity of maximum release rates in case retardation with sorption shows that some nuclides such as Pu-240, Pu-241, Pu-239, Cm-245, Am-241, Cm-246, and Am-243 are increased in some time in case maximum release rate from EBS corresponding to eliminate retardation in buffer material. Some nuclides such as U-235, U-233 and U-236 have a little decrease in case maximum release because their parents have short live and before decay to their daughter will released from the EBS. If the characteristic time taken for a nuclide to diffuse across the buffer exceeds its half-life, then the release rate of that nuclide from the EBS will be attenuated by radioactive decay. Thus, the retardation of the diffusion process due to sorption tends to reduce the release rates of short-lived nuclides more effectively than for the long-lived ones. For example, release rates of Pu-240, Cm-246 and Am-241, which are relatively short-lived and strongly sorbing, are very small

  4. 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.

  5. 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.

  6. 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

  7. 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).

  8. 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.

  9. 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

  10. 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.

  11. 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.

  12. 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.

  13. 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.

  14. 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

  15. 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.

  16. 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

  17. 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.

  18. 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 (

  19. 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.

  20. 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.

  1. 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.

  2. 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.

  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. 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

  5. Report on INL Activities for Uncertainty Reduction Analysis of FY11

    SciTech Connect

    G. Plamiotti; H. Hiruta; M. Salvatores

    2011-09-01

    This report presents the status of activities performed at INL under the ARC Work Package on 'Uncertainty Reduction Analyses' that has a main goal the reduction of uncertainties associated with nuclear data on neutronic integral parameters of interest for the design of advanced fast reactors under consideration by the ARC program. First, an analysis of experiments was carried out. For both JOYO (the first Japanese fast reactor) and ZPPR-9 (a large size zero power plutonium fueled experiment performed at ANL-W in Idaho) the performance of ENDF/B-VII.0 is quite satisfying except for the sodium void configurations of ZPPR-9, but for which one has to take into account the approximation of the modeling. In fact, when one uses a more detailed model (calculations performed at ANL in a companion WP) more reasonable results are obtained. A large effort was devoted to the analysis of the irradiation experiments, PROFIL-1 and -2 and TRAPU, performed at the French fast reactor PHENIX. For these experiments a pre-release of the ENDF/B-VII.1 cross section files was also used, in order to provide validation feedback to the CSWEG nuclear data evaluation community. In the PROFIL experiments improvements can be observed for the ENDF/B-VII.1 capture data in 238Pu, 241Am, 244Cm, 97Mo, 151Sm, 153Eu, and for 240Pu(n,2n). On the other hand, 240,242Pu, 95Mo, 133Cs and 145Nd capture C/E results are worse. For the major actinides 235U and especially 239Pu capture C/E's are underestimated. For fission products, 105,106Pd, 143,144Nd and 147,149Sm are significantly underestimated, while 101Ru and 151Sm are overestimated. Other C/E deviations from unity are within the combined experimental and calculated statistical uncertainty. From the TRAPU analysis, the major improvement is in the predicted 243Cm build-up, presumably due to an improved 242Cm capture evaluation. The COSMO experiment was also analyzed in order to provide useful feedback on fission cross sections. It was found out that ENDF

  6. 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

    weapons testing at that time. The age results for this component are in agreement using both {sup 242}Pu and {sup 151}Sm normalizations, although the errors for the {sup 151}Sm correction are currently larger due to the greater uncertainty of their measurements. Additional efforts to develop a concordant {sup 241}Pu-{sup 241}Am dating method for environmental collections are underway with emphasis on soil cores.

  7. The use of non-destructive passive neutron measurement methods in dismantling and radioactive waste characterization

    SciTech Connect

    Jallu, F.; Allinei, P. G.; Bernard, P.; Loridon, J.; Soyer, P.; Pouyat, D.; Torreblanca, L.; Reneleau, A.

    2011-07-01

    The cleaning up and dismantling of nuclear facilities lead to a great volume of technological radioactive wastes which need to be characterized in order to be sent to the adequate final disposal or interim storage. The control and characterization can be performed with non-destructive nuclear measurements such as gamma-ray spectrometry. Passive neutron counting is an alternative when the alpha-gamma emitters cannot be detected due to the presence of a high gamma emission resulting from fission or activation products, or when the waste matrix is too absorbing for the gamma rays of interest (too dense and/or made of high atomic number elements). It can also be a complement to gamma-ray spectrometry when two measurement results must be confronted to improve the confidence in the activity assessment. Passive neutron assays involve the detection of spontaneous fission neutrons emitted by even nuclides ({sup 238}Pu, {sup 240}Pu, {sup 242}Pu, {sup 242}Cm, {sup 244}Cm...) and neutrons resulting from ({alpha}, n) reactions with light nuclides (O, F, Be...). The latter is conditioned by the presence of high {alpha}-activity radionuclides ({sup 234}U, {sup 238}Pu, {sup 240}Pu, {sup 241}Am...) and low-Z elements, which depends on the chemical form (metallic, oxide or fluorine) of the plutonium or uranium contaminant. This paper presents the recent application of passive neutron methods to the cleaning up of a nuclear facility located at CEA Cadarache (France), which concerns the Pu mass assessment of 2714 historic, 100 litre radioactive waste drums produced between 1980 and 1997. Another application is the dismantling and decommissioning of an uranium enrichment facility for military purposes, which involves the {sup 235}U and total uranium quantifications in about a thousand, large compressors employed in the gaseous diffusion enrichment process. (authors)

  8. 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

  9. 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

  10. 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

  11. 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

  12. ANDES Measurements for Advanced Reactor Systems

    NASA Astrophysics Data System (ADS)

    Plompen, A. J. M.; Hambsch, F.-J.; Kopecky, S.; Nyman, M.; Rouki, C.; Salvador Castiñeira, P.; Schillebeeckx, P.; Belloni, F.; Berthoumieux, E.; Gunsing, F.; Lampoudis, C.; Calviani, M.; Guerrero, C.; Cano-Ott, D.; Gonzalez Romero, E.; Aïche, M.; Jurado, B.; Mathieu, L.; Derckx, X.; Farget, F.; Rodrigues Tajes, C.; Bacquias, A.; Dessagne, Ph.; Kerveno, M.; Borcea, C.; Negret, A.; Colonna, N.; Goncalves, I.; Penttilä, H.; Rinta-Antila, S.; Kolhinen, V. S.; Jokinen, A.

    2014-05-01

    A significant number of new measurements was undertaken by the ANDES “Measurements for advanced reactor systems” initiative. These new measurements include neutron inelastic scattering from 23Na, Mo, Zr, and 238U, neutron capture cross sections of 238U, 241Am, neutron induced fission cross sections of 240Pu, 242Pu, 241Am, 243Am and 245Cm, and measurements that explore the limits of the surrogate technique. The latter study the feasibility of inferring neutron capture cross sections for Cm isotopes, the neutron-induced fission cross section of 238Pu and fission yields and fission probabilities through full Z and A identification in inverse kinematics for isotopes of Pu, Am, Cm and Cf. Finally, four isotopes are studied which are important to improve predictions for delayed neutron precursors and decay heat by total absorption gamma-ray spectrometry (88Br, 94Rb, 95Rb, 137I). The measurements which are performed at state-of-the-art European facilities have the ambition to achieve the lowest possible uncertainty, and to come as close as is reasonably achievable to the target uncertainties established by sensitivity studies. An overview is presented of the activities and achievements, leaving detailed expositions to the various parties contributing to the conference.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. 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.

  19. 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.

  20. 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.

  1. 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

  2. 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.

  3. 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

  4. 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.

  5. 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

  6. LOS ALAMOS NEUTRON SCIENCE CENTER CONTRIBUTIONS TO THE DEVELOPMENT OF FUTURE POWER REACTORS

    SciTech Connect

    GAVRON, VICTOR I.; HILL, TONY S.; PITCHER, ERIC J.; TOVESSON, FREDERIK K.

    2007-01-09

    The Los Alamos Neutron Science Center (LANSCE) is a large spallation neutron complex centered around an 800 MeV high-currently proton accelerator. Existing facilities include a highly-moderated neutron facility (Lujan Center) where neutrons between thermal and keV energies are produced, and the Weapons Neutron Research Center (WNR), where a bare spallation target produces neutrons between 0.1 and several hundred MeV.The LANSCE facility offers a unique capability to provide high precision nuclear data over a large energy region, including that for fast reactor systems. In an ongoing experimental program the fission and capture cross sections are being measured for a number of minor actinides relevant for Generation-IV reactors and transmutation technology. Fission experiments makes use of both the highly moderated spallation neutron spectrum at the Lujan Center, and the unmoderated high energy spectrum at WNR. By combininb measurements at these two facilities the differential fission cross section is measured relative to the {sup 235}U(n,f) standard from subthermal energies up to about 200 MeV. An elaborate data acquisition system is designed to deal with all the different types of background present when spanning 10 energy decades. The first isotope to be measured was {sup 237}Np, and the results were used to improve the current ENDF/B-VII evaluation. Partial results have also been obtained for {sup 240}Pu and {sup 242}Pu, and the final results are expected shortly. Capture cross sections are measured at LANSCE using the Detector for Advanced Neutron Capture Experiments (DANCE). This unique instrument is highly efficient in detecting radiative capture events, and can thus handle radioactive samples of half-lives as low as 100 years. A number of capture cross sections important to fast reaction applications have been measured with DANCE. The first measurement was on {sup 237}Np(n,{gamma}), and the results have been submitted for publication. Other capture

  7. A comprehensive appraisal of 241Am in soils around Rocky Flats, Colorado.

    PubMed

    Litaor, M I; Allen, L

    1996-09-01

    Soils east of Rocky Flats Plant (RFETS) near Golden, Colorado, were contaminated with actinides because of accidental release of oils laden with plutonium isotopes. Consequently, these soils were contaminated by 241Am due to radioactive decay of 241Pu (t1/2 = 14.4 y). A spatial analysis of 241Am activity in soils east of RFETS was conducted to elucidate the magnitude and the mode of 241Am dispersion in the soil environment. 241Am activity of 178 soil samples ranged from 0.037 Bq kg-1 to 10,004 Bq kg-1 with a mean of 214 Bq kg-1, median of 7.28 Bq kg-1, standard deviation of 942 Bq kg-1, and a coefficient of variation of 4.3. Spatial analysis of 241Am in soils around RFETS was conducted using indicator kriging, which is a nonparametric technique especially suitable to model a conditional cumulative distribution function (ccdf) of highly skewed environmental data such as 241Am. The ccdf was used to generate an E-type (mean of the conditional cdf) surface. The resulted surfaces were consistent with the hypothesis that the westerly winds were the dominant mechanism of americium dispersal. The spatial distribution and dispersal mechanisms of 241Am were similar to those of 239+240Pu. The ccdf was also used to construct probability of exceedence maps of 241Am in soils. For the purpose of this report two threshold values for the probability maps were selected: (1) the mean measured background activity of 241Am (0.4 Bq kg-1), and (2) the programmatic preliminary remediation goal for residential occupancy scenario (87.7 Bq kg-1). The probability-of-exceedance maps provide estimates of spatial uncertainty associated with each threshold. The E-type maps in conjunction with the probability-of-exceedance maps provide a robust framework for future cleanup options and land use decisions. PMID:8698577

  8. 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.

  9. 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.

  10. Multipurpose Radiation Resistant Semiconductor Detectors for Alpha, Neutron & Low Energy Gamma Ray Measurements at High Temperatures in High-Intensity Gamma Ray

    SciTech Connect

    Ruddy, Frank H.

    2005-06-01

    Work scheduled under year two of DOE Grant DE-FG02-04ER63734 is on schedule and all year-two milestones have or will be met. Results to date demonstrate that unprecedented silicon carbide (SiC) energy resolution has been obtained, and that SiC detectors may achieve energy resolution that exceeds that obtainable with the best silicon alpha spectrometers. Fast-neutron energy spectrometry measurements indicate that recoil-ion energy spectrometry should be possible with SiC detectors. Furthermore, SiC detectors have been demonstrated to perform well even after gamma-ray exposures of 1.E09 Rad. This result and the previously demonstrated capability of SiC detectors to operate in elevated-temperature environments are very promising for potential DOE EMSP applications. A new class of multipurpose, radiation-resistant semiconductor detectors that can be used in elevated-temperature and high-radiation environments is being developed under this grant. These detectors, based on silicon carbide (SiC) semiconductor are designed to have larger active volumes than previously available SiC detectors, and are being tested for their response to alpha particles, X-rays and low energy gamma rays, and fast neutrons. Specifically, SiC radiation detectors with larger areas and 100-micrometer thick active regions have been designed and manufactured according to detector-design specifications. Detectors based on a Schottky diode design were specified in order to minimize the effects of the detector entrance window on alpha particle measurements. During manufacture of the Schottky diodes, the manufacturer also provided a set of large-volume SiC p-i-n diodes for testing Extensive alpha particle measurements have been carried out to test and quantify the response of the SiC Schottky diodes. Exposures to 148-Gd, 213-Po, 217-At, 221-Fr, 225-Ac, 237-Np, 238-Pu, 240-Pu, and 242-Pu sources were used to obtain detailed alpha response data in the alpha energy range from 3182.787 keV to 8375.9 ke

  11. 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

  12. 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

  13. Application of autoradiographic techniques for contaminant distribution studies in soils

    NASA Astrophysics Data System (ADS)

    Povetko, Oleg G.

    In order to determine the physical location of contaminants in soil, two solidified soil "thin" sections, which preserve the undisturbed structural characteristics of the original soil, containing weapons-grade plutonium from the Rocky Flats Environmental Test Site were prepared. Two autoradiographic methods were used in radionuclide mapping: contact autoradiography using CR-39RTMplastic alpha track detectors and neutron-induced autoradiography that produced fission fragment tracks in LexanRTM plastic detectors. The combination of the two autoradiographic methods distinguished alpha-emitting particles of natural U, from 239+240Pu and non-fissile alpha-emitters. The locations of 990 alpha "stars" caused by plutonium "hot particles" in two soil sections were recorded, particles were sized, their size-frequency and depth distributions were analyzed. Several large colloidal conglomerates of "hot particles" were found in soil profiles. One such conglomerate with a geometric size of about 500 mum contained over 94% of the total recorded contaminant alpha activity in the sample. It was found that the upper 6.5 cm of soil contained 20% of all recorded particles (mean equivalent size 0.35 mum). The deeper portion of the surface 6.5 cm soil layer contained 80% of the particles (with mean equivalent size 0.25 mum). The average specific activity (SA) for 989 hot particles (with the conglomerate of the particles excluded) with equivalent diameters over 80 nm was found to be greater than 23.9 Bq g-1 (about 90% of the overall average SA). For dissolved and defragmented (below 80 nm of equivalent diameter) actinide particles, SA was found smaller than 2.9 Bq g-1. Over 99% of the total actinide contaminant activity in the analyzed soil sample (with the conglomerate of the particles included) was found in particles with equivalent diameters over 0.08 mum. It suggests that larger particles of plutonium oxide moved down more slowly than smaller ones and no significant breakup of

  14. Corrections for Exchange and Screening Effects in Low-energy Beta Decays

    SciTech Connect

    Mougeot, X. Bé, M.-M.; Bisch, C.; Loidl, M.

    2014-06-15

    The beta spectra of {sup 241}Pu and {sup 63}Ni have been recently measured using metallic magnetic calorimeters. This powerful experimental technique allows theoretical beta spectra calculations to be tested at low energy with an accuracy never before achievable. Their comparison with classical beta calculations exhibits a significant deviation below 4 keV for {sup 241}Pu and 8 keV for {sup 63}Ni. The atomic exchange effect explains the main part of this deviation in the {sup 63}Ni beta spectrum. This effect has a significant contribution, equivalent to the magnitude of the screening, in the {sup 241}Pu beta spectrum.

  15. Improved methods of measurement and analysis of conversion electron and beta-particle spectra

    PubMed

    Dragoun; Spalek; Rysavy; Kovalik; Yakushev; Brabec; Frana; Venos

    2000-03-01

    A general statistical test of the stability of measurement conditions was demonstrated on the beta-spectra of 241Pu cumulated during four years. The alpha- and gamma-ray spectroscopy indicated stability of the 241Pu source. Monte Carlo modelling of individual collision events clarified the role of electron scattering and energy losses within a radioactive source down to energies of several hundreds of eV. The impact ionization by beta-particles of carbon and oxygen atoms in a surface contamination layer on the 241Pu and 63Ni sources was observed. PMID:10724379

  16. 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.

  17. Plutonium and americium behavior in coral atoll environments

    SciTech Connect

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

    1984-02-01

    Inventories of /sup 239 +240/Pu and /sup 241/Am greatly in excess of global fallout levels persist in the benthic environments of Bikini and Enewetak Atolls. Quantities of /sup 239 +240/Pu and lesser amounts of /sup 241/Am are continuously mobilizing from these sedimentary reservoirs. The amount of /sup 239 +240/Pu mobilized to solution at any time represents 0.08 to 0.09% of the sediment inventories to a depth of 16 cm. The mobilized /sup 239 +240/Pu has solute-like characteristics and different valence states coexist in solution - the largest fraction of the soluble plutonium is in an oxidized form (+V,VI). The adsorption of plutonium to sediments is not completely reversible because of changes that occur in the relative amounts of the mixed oxidation states in solution with time. Further, any characteristics of /sup 239 +240/Pu described at one location may not necessarily be relevant in describing its behavior elsewhere following mobilization and migration. The relative amounts of /sup 241/Am to /sup 239 +240/Pu in the sedimentary deposits at Enewetak and Bikini may be altered in future years because of mobilization and radiological decay. Mobilization of /sup 239 +240/Pu is not a process unique to these atolls, and quantities in solution derived from sedimentary deposits can be found at other global sites. These studies in the equatorial Pacific have significance in assessing the long-term behavior of the transuranics in any marine environment. 22 references, 1 figure, 13 tables.

  18. 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

  19. 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.

  20. 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

  1. SALTSTONE VAULT CLASSIFICATION SAMPLES MODULAR CAUSTIC SIDE SOLVENT EXTRACTION UNIT/ACTINIDE REMOVAL PROCESS WASTE STREAM APRIL 2011

    SciTech Connect

    Eibling, R.

    2011-09-28

    Savannah River National Laboratory (SRNL) was asked to prepare saltstone from samples of Tank 50H obtained by SRNL on April 5, 2011 (Tank 50H sampling occurred on April 4, 2011) during 2QCY11 to determine the non-hazardous nature of the grout and for additional vault classification analyses. The samples were cured and shipped to Babcock & Wilcox Technical Services Group-Radioisotope and Analytical Chemistry Laboratory (B&W TSG-RACL) to perform the Toxic Characteristic Leaching Procedure (TCLP) and subsequent extract analysis on saltstone samples for the analytes required for the quarterly analysis saltstone sample. In addition to the eight toxic metals - arsenic, barium, cadmium, chromium, mercury, lead, selenium and silver - analytes included the underlying hazardous constituents (UHC) antimony, beryllium, nickel, and thallium which could not be eliminated from analysis by process knowledge. Additional inorganic species determined by B&W TSG-RACL include aluminum, boron, chloride, cobalt, copper, fluoride, iron, lithium, manganese, molybdenum, nitrate/nitrite as Nitrogen, strontium, sulfate, uranium, and zinc and the following radionuclides: gross alpha, gross beta/gamma, 3H, 60Co, 90Sr, 99Tc, 106Ru, 106Rh, 125Sb, 137Cs, 137mBa, 154Eu, 238Pu, 239/240Pu, 241Pu, 241Am, 242Cm, and 243/244Cm. B&W TSG-RACL provided subsamples to GEL Laboratories, LLC for analysis for the VOCs benzene, toluene, and 1-butanol. GEL also determines phenol (total) and the following radionuclides: 147Pm, 226Ra and 228Ra. Preparation of the 2QCY11 saltstone samples for the quarterly analysis and for vault classification purposes and the subsequent TCLP analyses of these samples showed that: (1) The saltstone waste form disposed of in the Saltstone Disposal Facility in 2QCY11 was not characteristically hazardous for toxicity. (2) The concentrations of the eight RCRA metals and UHCs identified as possible in the saltstone waste form were present at levels below the UTS. (3) Most of the

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

    PubMed

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

    2016-03-01

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

  4. 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

  5. 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

  6. Plutonium and americium in anoxic marine sediments: Evidence against remobitization

    NASA Astrophysics Data System (ADS)

    Carpenter, R.; Beasley, T. M.

    1981-10-01

    239 + 240Pu activities of 100-450dpm/kg are found down to 15-18 cm in anoxic Saanich Inlet sediments, with a subsurface maximum in undisturbed deposits. Integrated 239 + 240Pu inventories which overlap delivery estimates are present both in two cores of anoxic sediments from Saanich Inlet and in one core of oxic sediments 65 km away in Dabob Bay, Washington. 241Am /239 + 240Pu ratios in Saanich Inlet sediments overlap ratios in unfractionated midnorthern latitude fallout, in oxic sediments from the Washington continental shelf, and in anoxic sediments from two basins off southern California and Mexico. The 239 + 240Pu /137Cs ratios in three intervals of Saanich Inlet sediments are also in agreement with ratios previously reported for oxic coastal marine sediments. The Pu inventories, the Am/Pu and Pu/Cs ratios, and the Saanich Inlet Dabob Bay comparison all argue that Pu is not rapidly remobilized in anoxic sediments. The subsurface 239 + 240Pu activity maximum is not in agreement with the historical record of peak Pu fallout in 1963-1964 unless our 210Pb-derived sedimentation rates are incorrectly high. However, they are in good agreement with previous 210Pb and varve chronologies in Saanich Inlet, and also give reasonable dates for times when 239 + 240Pu and SNAP-9A supplied 238Pu first appear in the sediments. We conclude they properly date the maximum in sedimentary 239 + 240Pu activity at 1970-1973, and seek explanations for the 7-10yr time lag after peak fallout. 239 + 240Pu inventories in one core from the eastern basin of the Cariaco Trench and in two cores from Golfo Dulce. an anoxic basin off the Pacific coast of Costa Rica, are also in reasonable agreement with fallout delivery to these latitudes when excess 210Pb inventories and fluxes are used to verify recovery of at least a major fraction of the most recently deposited sediments.

  7. 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.

  8. 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

  9. 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.

  10. 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.

  11. 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

  12. 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.

  13. 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

  14. Excess plutonium in soil near the Nevada Test Site, USA.

    PubMed

    Turner, Mary; Rudin, Mark; Cizdziel, James; Hodge, Vernon

    2003-01-01

    Two soil profiles were collected from undisturbed areas near the Nevada Test Site (NTS). The activity of 137Cs in the surface layer of the downwind Queen City Summit profile is three times higher than at the upwind site at Searchlight, NV (41.1+/-0.6 mBq/g vs. 13.0+/-0.4 mBq/g), and the 239,240Pu activity is 100 times greater (51+/-2 mBq/g vs. 0.52+/-0.03 mBq/g). An examination of the literature suggests that the 137Cs/239,240Pu and the 239,240Pu/238Pu activity ratios in soils and sediments from the northern hemisphere, due to fallout from atmospheric atomic weapons testing, have generalized values of 36+/-4 and 30+/-4, respectively (as of 1 July 1995). Deviations from these values may indicate possible contamination by sources other than fallout. Data from the surface soil of the downwind Queen City Summit profile yield a 137Cs/239,240Pu ratio of 0.81+/-0.02 and a 239,240Pu/238Pu ratio of 78+/-6. Clearly, an increase in 239,240Pu relative to 137Cs or 238Pu can account for these observations. There is compelling evidence that this "excess" 239,240Pu came from activities at the NTS during the aboveground testing of nuclear devices, more than likely from safety tests, some 40 years ago, and/or during the interim by the wind-driven resuspension of contaminated surface soil on the NTS and its transport off-site. Moreover, the two concentration profiles show that high percentages of both of these elements are retained for decades in the upper few centimeters of soil in Nevada's desert environment.

  15. 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.

  16. Feasibility of using 236U to reconstruct close-in fallout deposition from the Hiroshima atomic bomb.

    PubMed

    Sakaguchi, A; Kawai, K; Steier, P; Imanaka, T; Hoshi, M; Endo, S; Zhumadilov, K; Yamamoto, M

    2010-10-15

    The first results on the feasibility of using (236)U to reconstruct the level and spatial distribution of close-in fallout deposition from the Hiroshima A-bomb are reported, coupled with the use of global fallout (137)Cs and (239+240)Pu. The results for global fallout (236)U in soil samples (0-30cm) from Ishikawa prefecture showed that the deposition density of (236)U from the global fallout can be accurately evaluated using AMS. All deposited (236)U, (137)Cs and (239+240)Pu appeared to have been recovered using 30-cm cores. It was also noted from the depth profiles for (236)U/(239+240)Pu and (236)U/(137)Cs ratios that the downward behavior of (236)U in the soil was apparently similar to that of (239+240)Pu, while the (137)Cs was liable to be retained in upper layers compared with (236)U and (239+240)Pu. The accumulated levels were 1.78×10(13)atomsm(-2) for (236)U, 4340Bqm(-2) for (137)Cs and 141Bqm(-2) for (239+240)Pu. The ratios of (236)U/(137)Cs and (236)U/(239+240)Pu were (4.10±0.12)×10(9) and (1.26±0.04)×10(11)atomsBq(-1), respectively. Results of (236)U, (137)Cs and (239+240)Pu measurements for the seven soil cores (0-30cm) from Hiroshima were discussed on the basis of ratios of (236)U/(137)Cs and (236)U/(239+240)Pu by comparing with those from the background area in Ishikawa, indicating that the global fallout dominates the current level of (236)U accumulation in soil in the Black-rain area around Hiroshima after the Hiroshima bomb, and the contribution of the close-in fallout (236)U produced by the Hiroshima A-bomb seems difficult to observe.

  17. Feasibility of using 236U to reconstruct close-in fallout deposition from the Hiroshima atomic bomb.

    PubMed

    Sakaguchi, A; Kawai, K; Steier, P; Imanaka, T; Hoshi, M; Endo, S; Zhumadilov, K; Yamamoto, M

    2010-10-15

    The first results on the feasibility of using (236)U to reconstruct the level and spatial distribution of close-in fallout deposition from the Hiroshima A-bomb are reported, coupled with the use of global fallout (137)Cs and (239+240)Pu. The results for global fallout (236)U in soil samples (0-30cm) from Ishikawa prefecture showed that the deposition density of (236)U from the global fallout can be accurately evaluated using AMS. All deposited (236)U, (137)Cs and (239+240)Pu appeared to have been recovered using 30-cm cores. It was also noted from the depth profiles for (236)U/(239+240)Pu and (236)U/(137)Cs ratios that the downward behavior of (236)U in the soil was apparently similar to that of (239+240)Pu, while the (137)Cs was liable to be retained in upper layers compared with (236)U and (239+240)Pu. The accumulated levels were 1.78×10(13)atomsm(-2) for (236)U, 4340Bqm(-2) for (137)Cs and 141Bqm(-2) for (239+240)Pu. The ratios of (236)U/(137)Cs and (236)U/(239+240)Pu were (4.10±0.12)×10(9) and (1.26±0.04)×10(11)atomsBq(-1), respectively. Results of (236)U, (137)Cs and (239+240)Pu measurements for the seven soil cores (0-30cm) from Hiroshima were discussed on the basis of ratios of (236)U/(137)Cs and (236)U/(239+240)Pu by comparing with those from the background area in Ishikawa, indicating that the global fallout dominates the current level of (236)U accumulation in soil in the Black-rain area around Hiroshima after the Hiroshima bomb, and the contribution of the close-in fallout (236)U produced by the Hiroshima A-bomb seems difficult to observe. PMID:20797770

  18. Comparative behavior of plutonium and americium in the equatorial Pacific

    SciTech Connect

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

    1983-01-01

    Inventories of /sup 239 +240/Pu and /sup 241/Am greatly in excess of global fallout levels persist in the benthic environments of Bikini and Enewetak Atolls. The amount of /sup 239 +240/Pu mobilized to solution at the atolls can be predicted from a distribution coefficient K/sub d/ of 2.3 x 10/sup 5/ and the mean sediment concentrations. The mobilized /sup 239 +240/Pu has solute-like characteristics and different valence states coexist in solution - the largest fraction of the soluble plutonium is in an oxidized form (+V,VI). The adsorption of plutonium to sediments is not completely reversible because of changes that occur in the relative amounts of the mixed oxidation states in solution with time. Characteristics of /sup 239 +240/Pu described at one location may not necessarily describe its behavior elsewhere. The relative amounts of /sup 241/Am to /sup 239 +240/Pu may be altered in future years because of mobilization and radiological decay.

  19. 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.

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

    PubMed

    Hölgye, Z; Filgas, R

    2006-04-01

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

  1. 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.

  2. Discovery of new superheavy element isotopes

    NASA Astrophysics Data System (ADS)

    Gates, Jacklyn

    2011-04-01

    The first confirmation of element 114 production and decay was performed in 2009 with the Berkeley Gas-filled Separator at the Lawrence Berkeley National Laboratory 88-Inch Cyclotron. The 48 Ca + 242Pu reaction was used. Compound nucleus evaporation residues were separated from beam and other reaction products with the Berkeley Gas-filled separator and implanted in the focal plane detector system. Production and decay of one atom each of 287 114 (via the 242Pu(48 Ca, 3n)287 114 reaction) and 286 114(via the 242Pu(48 Ca,4n)286 114 reaction) were observed. Production cross sections, decay modes, decay energies, and half-lives and for these element 114 isotopes and their daughters were consistent with those reported by the Dubna Gas Filled Recoil Separator Group (Yuri Oganessian , J. Phys. G: Nucl. Part. Phys. 34 (2007) R165--R242). In 2010, the 48 Ca + 242Pu reaction was used again, at an increased beam energy to optimize the production of new isotope, 285 114, by the 242Pu(48 Ca,5n)285 114 reaction. The production and decay of one atom of 286 114 (via the 242Pu(48 Ca,4n)286 114 reaction) was observed, re-confirming the properties of this isotope. In addition, a single event corresponding to the production and decay of 285 114 (via the 242Pu(48 Ca,5n)285 114 reaction) was observed. The implantation of 285 114 in the detector was followed by five α-decays and a spontaneous fission event, indicating the α-decays of new isotopes, 285 114, 281Cp, 277Ds, 273Hs, 269Sg, and the spontaneous fission of new isotope, 265Rf. The decay properties of all these new isotopes match expectations based on microscopic-macroscopic mass models supplemented with extrapolations of previously reported superheavy element isotope decay properties. However, some systematic differences between observed and predicted α-decay Q-values may be used to refine models of nuclear shell effects in heavy element isotopes. Financial support was provided by the Office of High Energy and Nuclear Physics

  3. 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.

  4. 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

  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.

  6. 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

  7. 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.

  8. Plutonium, cesium and uranium series radionuclides in the Hudson River estuary and other environments. Annual technical progress report, December 1, 1979-November 30, 1980

    SciTech Connect

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

    1980-01-01

    Radionuclide activities were measured in a large number of sediment cores and suspended particle samples throughout the salinity range of the Hudson River estuary. Activities of /sup 137/Cs, /sup 134/Cs and /sup 60/Co determined by gamma spectrometry and /sup 239/ /sup 240/Pu and /sup 238/Pu determined by alpha spectrometry indicate reasonably rapid accumulation rates in the sediments of marginal cove areas, and very rapid deposition in the harbor region adjacent to New York City, resulting in /sup 239/ /sup 240/Pu accumulations there more than an order of magnitude greater than the fallout delivery rate. Measurable amounts of reactor-derived /sup 134/Cs and /sup 60/Co are found in nearly al sediment samples containing appreciable /sup 137/Cs between 15 km upstream of Indian Point and the downstream extent of our sampling about 70 km south of the reactor. Fallout /sup 239/ /sup 240/Pu reaching the Hudson appears to be almost completely retained within the systems by particle deposition, while 70 to 90% of the /sup 137/Cs derived from both reactor releases and fallout has been exported to the coastal waters in solution. Activity levels of /sup 239/ /sup 240/Pu in New York harbor sediments indicate a significant source in addition to suspended particles carried down the Hudson. The most likely cause appears to be transport into the estuary of particles from offshore waters having higher specific activities of /sup 239/ /sup 240/Pu. Measurements of fallout /sup 239/ /sup 240/Pu in a saline lake with a high carbonate ion concentration yielded water column activities about two orders of magnitude greater than has been found for fallout plutonium in other continental waters, indicating extensive mobility in some natural water environments. Experiments using lake water suggest that carbonate ion may indeed be a critical factor in regulating plutonium solubility and that low molecular weight complexes are primarily responsible for enhanced plutonium solubility.

  9. 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.

  10. 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

  11. Plutonium and radiocesium in the water column of the Hudson River estuary

    NASA Astrophysics Data System (ADS)

    Linsalata, P.; Simpson, H. J.; Olsen, C. R.; Cohen, N.; Trier, R. M.

    1985-12-01

    Isotopes of plutonium (Pu), cesium (Cs), and cobalt (Co) introduced into the Hudson River Estuary from fallout deposition, the erosion of fallout-contaminated surface soils, and nuclear reactor effluent (isotopes of Cs and Co only) have been measured in water column samples collected from 1975 to 1980 Isotopic measurements conducted independently by two research groups utilizing different sampling and analytical techniques have been summarized. The major conclusions drawn from the work are that for water samples collected by the two laboratories over similar time periods, the mean concentrations of nonfilterable239,240Pu (<0.45 μm) were identical at 0.13 fCi/l, mean concentrations of both137Cs and239,240Pu in suspended particulates were more divergent at 2,270±920 pCi/kg (±1 SD) and 1,430±430 pCi/kg for137Cs, and 19±8 pCi/kg and 12±4 pCi/kg for239,240Pu The behavior of239,240Pu and137Cs within the water column is shown to diverge within brackish waters Specifically, the magnitude of the137Cs distribution coefficient ( K d ) can be expressed as an inverse power function of the chloride ion concentrations for chlorinities between 0.1 and 4 g Cl-/l No difference in the239,240Pu K d has been observed between fresh and brackish waters Based on the expected inventories of239,240Pu and137Cs within watershed soils, the current downstream transport of these radionuclides represents fractional mobilization rates on the order of 1 4 (×10-4) per year

  12. Multipurpose Radiation Resistant Semiconductor Detectors for Alpha, Neutron & Low Energy Gamma Ray Measurements at High Temperatures in High-Intensity Gamma Ray

    SciTech Connect

    Ruddy, Frank H.

    2005-06-01

    Work scheduled under year two of DOE Grant DE-FG02-04ER63734 is on schedule and all year-two milestones have or will be met. Results to date demonstrate that unprecedented silicon carbide (SiC) energy resolution has been obtained, and that SiC detectors may achieve energy resolution that exceeds that obtainable with the best silicon alpha spectrometers. Fast-neutron energy spectrometry measurements indicate that recoil-ion energy spectrometry should be possible with SiC detectors. Furthermore, SiC detectors have been demonstrated to perform well even after gamma-ray exposures of 1.E09 Rad. This result and the previously demonstrated capability of SiC detectors to operate in elevated-temperature environments are very promising for potential DOE EMSP applications. A new class of multipurpose, radiation-resistant semiconductor detectors that can be used in elevated-temperature and high-radiation environments is being developed under this grant. These detectors, based on silicon carbide (SiC) semiconductor are designed to have larger active volumes than previously available SiC detectors, and are being tested for their response to alpha particles, X-rays and low energy gamma rays, and fast neutrons. Specifically, SiC radiation detectors with larger areas and 100-micrometer thick active regions have been designed and manufactured according to detector-design specifications. Detectors based on a Schottky diode design were specified in order to minimize the effects of the detector entrance window on alpha particle measurements. During manufacture of the Schottky diodes, the manufacturer also provided a set of large-volume SiC p-i-n diodes for testing Extensive alpha particle measurements have been carried out to test and quantify the response of the SiC Schottky diodes. Exposures to 148-Gd, 213-Po, 217-At, 221-Fr, 225-Ac, 237-Np, 238-Pu, 240-Pu, and 242-Pu sources were used to obtain detailed alpha response data in the alpha energy range from 3182.787 keV to 8375.9 ke

  13. 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.

  14. 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.

  15. 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.

  16. US Mussel Watch 1976-1978: an overview of the trace-metal, DDE, PCB, hydrocarbon, and artificial radionuclide data. [Mytilus edulis, M. californianus, Crassostrea sp

    SciTech Connect

    Farrington, J.W.; Goldberg, E.D.; Risebrough, R.W.; Martin, J.H.; Bowen, V.T.

    1983-08-01

    Data are presented for trace metals, polychlorinated biphenyls (PCBs), aromatic hydrocarbons and /sup 239/ /sup 240/Pu in Mytilus edulis, M. californianus, and Crassostrea sp. collected in the US Mussel Watch program in 1976-1978 from 62 locations on the US east and west coasts. General similarities in geographical distributions of concentrations were present in all 3 years with at least an order of magnitude elevation of concentrations of Pb, PCBs, and fossil fuel hydrocarbons in bivalves sampled near the larger urban areas. Elevated Cd and /sup 239/ /sup 240/Pu concentrations in bivalves from the central California coast are apparently related to enrichments of Cd and nuclear weapons testing fallout /sup 239/ /sup 240/Pu in intermediate depth water of the North Pacific and upwelling of this water associated with the California Current system. Data have revealed no evidence of local or regional systematic elevations of environmental concentrations of /sup 239/ /sup 240/Pu as a result of effluent releases from nuclear power reactors.

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

    PubMed

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

    2012-08-01

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

  18. 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.

  19. 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

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

    PubMed

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

    2010-02-01

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

  1. Radionuclide transport from soil to air, native vegetation, kangaroo rats and grazing cattle on the Nevada test site.

    PubMed

    Gilbert, R O; Shinn, J H; Essington, E H; Tamura, T; Romney, E M; Moor, K S; O'Farrell, T P

    1988-12-01

    Between 1970 and 1986 the Nevada Applied Ecology Group (NAEG), U.S. Department of Energy, conducted environmental radionuclide studies at weapons-testing sites on or adjacent to the Nevada Test Site. In this paper, NAEG studies conducted at two nuclear (fission) sites (NS201, NS219) and two nonnuclear (nonfission) sites (Area 13 [Project 57] and Clean Slate 2) are reviewed, synthesized and compared regarding (1) soil particle-size distribution and physical-chemical characteristics of 239 + 240Pu-bearing radioactive particles, (2) 239 + 240Pu resuspension rates and (3) transuranic and fission-product radionuclide transfers from soil to native vegetation, kangaroo rats and grazing cattle. The data indicate that transuranic radionuclides were transferred more readily on the average from soil to air, the external surfaces of native vegetation and to tissues of kangaroo rats at Area 13 than at NS201 or NS219. The 239 + 240Pu resuspension factor for undisturbed soil at Area 13 was three to four orders-of-magnitude larger than at NS201 and NS219, the geometric mean (GM) vegetation-over-soil 239 + 240Pu concentration ratio was from ten to 100 times larger than at NS201, and the GM GI-over-soil, carcass-over-soil and pelt-over-soil 239 + 240Pu ratios for kangaroo rats were about ten times larger than at NS201. These results are consistent with the finding that Area 13, compared with NS201 or NS219, has a higher percentage of radioactivity associated with smaller soil particles and a larger percentage of resuspendable and respirable soil. However, the resuspension factor increased by a factor of 27 at NS201 when the surface soil was disturbed, and by a factor of 12 at NS219 following a wildfire. The average (GM) concentration of 239 + 240Pu for the GI (and contents) of Area 13 kangaroo rats and for the rumen contents of beef cattle that grazed Area 13 were very similar (400 vs. 440 Bq kg-1 dry wt, respectively) although the variability between individuals was very large. The

  2. Sequential injection approach for simultaneous determination of ultratrace plutonium and neptunium in urine with accelerator mass spectrometry.

    PubMed

    Qiao, Jixin; Hou, Xiaolin; Roos, Per; Lachner, Johannes; Christl, Marcus; Xu, Yihong

    2013-09-17

    An analytical method was developed for simultaneous determination of ultratrace level plutonium (Pu) and neptunium (Np) using iron hydroxide coprecipitation in combination with automated sequential injection extraction chromatography separation and accelerator mass spectrometry (AMS) measurement. Several experimental parameters affecting the analytical performance were investigated and compared including sample preboiling operation, aging time, amount of coprecipitating reagent, reagent for pH adjustment, sedimentation time, and organic matter decomposition approach. The overall analytical results show that preboiling and aging are important for obtaining high chemical yields for both Pu and Np, which is possibly related to the aggregation and adsorption behavior of organic substances contained in urine. Although the optimal condition for Np and Pu simultaneous determination requires 5-day aging time, an immediate coprecipitation without preboiling and aging could also provide fairly satisfactory chemical yields for both Np and Pu (50-60%) with high sample throughput (4 h/sample). Within the developed method, (242)Pu was exploited as chemical yield tracer for both Pu and Np isotopes. (242)Pu was also used as a spike in the AMS measurement for quantification of (239)Pu and (237)Np concentrations. The results show that, under the optimal experimental condition, the chemical yields of (237)Np and (242)Pu are nearly identical, indicating the high feasibility of (242)Pu as a nonisotopic tracer for (237)Np determination in real urine samples. The analytical method was validated by analysis of a number of urine samples spiked with different levels of (237)Np and (239)Pu. The measured values of (237)Np and (239)Pu by AMS exhibit good agreement (R(2) ≥ 0.955) with the spiked ones confirming the reliability of the proposed method.

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

    PubMed

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

    2014-11-01

    Activity concentrations, inventories and activity ratios of (137)Cs, (238)Pu, (239 + 240)Pu and (241)Am in soil profiles were surveyed in the dry tundra and the adjoining proglacial zones of glaciers at a High Arctic site on Svalbard. Vertical profiles of radionuclide activities were determined in up to 14-cm-thick soil sequences. Additionally, soil properties (pH, organic matter, texture, mineral composition and sorption capacity) were analyzed. Results obtained in this study revealed a large range of activity concentrations and inventories of the fallout radionuclides from the undetectable to the uncommonly high levels (inventories of 30,900 ± 940, 47 ± 6, 886 ± 80 and 296 ± 19 Bq/m(2) for (137)Cs, (238)Pu, (239 + 240)Pu and (241)Am, respectively) found in two profiles from the proglacial zone. Concentration of these initially airborne radionuclides in the proglacial zone soils is related to their accumulation in cryoconites that have a large ability to concentrate trace metals. The cryoconites develop on the surface of glaciers, and the material they accumulate is deposited on land surface after the glaciers retreat. The radionuclide inventories in the tundra soils, which effectively retain radionuclides due to high organic matter contents, were comparable to the global fallout deposition for this region of the world. The (238)Pu/(239 + 240)Pu activity ratios for tundra soils suggested global fallout as the dominant source of Pu. The (238)Pu/(239 + 240)Pu and (239 + 240)Pu/(137)Cs activity ratios in the proglacial soils pointed to possible contributions of these radionuclides from other, unidentified sources. PMID:24946703

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

    PubMed

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

    2011-11-01

    The vertical profiles of (239+240)Pu and (137)Cs activities and (240)Pu/(239)Pu isotopic ratios are determined for three sediment cores of Lake Qinghai from the Qinghai-Tibetan Plateau, China, and compared with those in sediments of another three lakes (Lakes Bosten, Sugan, and Shuangta), the only existing ones closest to Lop Nor area, China's nuclear weapons test site in the northwestern part of the country. The mean inventory of 47.7 ± 18.7 MBq km(-2) for (239+240)Pu activity in Lake Qinghai is comparable to the average value of global fallout expected at the same latitude, yet the mean inventory of 1112.0 ± 78.0 MBq km(-2) for (137)Cs is slightly lower than that of global fallout. Anomalously low (240)Pu/(239)Pu isotopic ratios (0.038-0.125) were found in the 3-6.5 cm deep sediment layers, indicating the trace Pu input from early nuclear weapons research activities at Atomic City in the lake's watershed during the 1950-60s. Model calculation indicated that the Pu input accounted for approximately 5-16% of the total Pu inventory. The observation of low (240)Pu/(239)Pu ratio in the deep sediment layer provided a new time marker for recent sediment dating in the lake and around the area. The results are of great significance to the further understanding of sources, records, and environmental impacts of global and regional nuclear activities in the environment and provide important chronological information for further studies on the water eutrophication process and climatic change, and reconstruction of pollution history of organic contaminants and heavy metals in the watershed of Lake Qinghai. PMID:21950768

  5. 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

  6. 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.

  7. Radionuclide transport from soil to air, native vegetation, kangaroo rats and grazing cattle on the Nevada test site

    SciTech Connect

    Gilbert, R.O.; Shinn, J.H.; Essington, E.H.; Tamura, T.; Romney, E.M.; Moor, K.S.; O'Farrell, T.P.

    1988-12-01

    Between 1970 and 1986 the Nevada Applied Ecology Group (NAEG), U.S. Department of Energy, conducted environmental radionuclide studies at weapons-testing sites on or adjacent to the Nevada Test Site. In this paper, NAEG studies conducted at two nuclear (fission) sites (NS201, NS219) and two nonnuclear (nonfission) sites (Area 13 (Project 57) and Clean Slate 2) are reviewed, synthesized and compared regarding (1) soil particle-size distribution and physical-chemical characteristics of 239 + 240Pu-bearing radioactive particles, (2) 239 + 240Pu resuspension rates and (3) transuranic and fission-product radionuclide transfers from soil to native vegetation, kangaroo rats and grazing cattle. The data indicate that transuranic radionuclides were transferred more readily on the average from soil to air, the external surfaces of native vegetation and to tissues of kangaroo rats at Area 13 than at NS201 or NS219. The 239 + 240Pu resuspension factor for undisturbed soil at Area 13 was three to four orders-of-magnitude larger than at NS201 and NS219, the geometric mean (GM) vegetation-over-soil 239 + 240Pu concentration ratio was from ten to 100 times larger than at NS201, and the GM GI-over-soil, carcass-over-soil and pelt-over-soil 239 + 240Pu ratios for kangaroo rats were about ten times larger than at NS201. These results are consistent with the finding that Area 13, compared with NS201 or NS219, has a higher percentage of radioactivity associated with smaller soil particles and a larger percentage of resuspendable and respirable soil. However, the resuspension factor increased by a factor of 27 at NS201 when the surface soil was disturbed, and by a factor of 12 at NS219 following a wildfire.

  8. Plutonium and 137Cs in surface water of the South Pacific Ocean.

    PubMed

    Hirose, K; Aoyama, M; Fukasawa, M; Kim, C S; Komura, K; Povinec, P P; Sanchez-Cabeza, J A

    2007-08-01

    The present plutonium and 137Cs concentrations in South Pacific Ocean surface waters were determined. The water samples were collected in the South Pacific mid-latitude region (32.5 degrees S) during the BEAGLE expedition conducted in 2003-04 by JAMSTEC. 239,240Pu concentrations in surface seawater of the South Pacific were in the range of 0.5 to 4.1 mBq m(-3), whereas 137Cs concentrations ranged from 0.07 to 1.7 Bq m(-3). The observed 239,240Pu and 137Cs concentrations in the South Pacific were almost of the same level as those in the North Pacific subtropical gyre. The surface 239,240Pu in the South Pacific subtropical gyre showed larger spatial variations than 137Cs, as it may be affected by physical and biogeochemical processes. The 239,240Pu/137Cs activity ratios, which reflect biogeochemical processes in seawater, were generally smaller than that observed in global fallout, except for the most eastern station. The 239,240Pu/137Cs ratios in the South Pacific tend to be higher than that in the North Pacific. The relationships between anthropogenic radionuclides and oceanographic parameters such as salinity and nutrients were examined. The 137Cs concentrations in the western South Pacific (the Tasman Sea) and the eastern South Pacific were negatively correlated with the phosphate concentration, whereas there is no correlation between the 137Cs and nutrients concentrations in the South Pacific subtropical gyre. The mutual relationships between anthropogenic radionuclides and oceanographic parameters are important for better understanding of transport processes of anthropogenic radionuclides and their fate in the South Pacific. PMID:17459459

  9. Plutonium and 137Cs in surface water of the South Pacific Ocean.

    PubMed

    Hirose, K; Aoyama, M; Fukasawa, M; Kim, C S; Komura, K; Povinec, P P; Sanchez-Cabeza, J A

    2007-08-01

    The present plutonium and 137Cs concentrations in South Pacific Ocean surface waters were determined. The water samples were collected in the South Pacific mid-latitude region (32.5 degrees S) during the BEAGLE expedition conducted in 2003-04 by JAMSTEC. 239,240Pu concentrations in surface seawater of the South Pacific were in the range of 0.5 to 4.1 mBq m(-3), whereas 137Cs concentrations ranged from 0.07 to 1.7 Bq m(-3). The observed 239,240Pu and 137Cs concentrations in the South Pacific were almost of the same level as those in the North Pacific subtropical gyre. The surface 239,240Pu in the South Pacific subtropical gyre showed larger spatial variations than 137Cs, as it may be affected by physical and biogeochemical processes. The 239,240Pu/137Cs activity ratios, which reflect biogeochemical processes in seawater, were generally smaller than that observed in global fallout, except for the most eastern station. The 239,240Pu/137Cs ratios in the South Pacific tend to be higher than that in the North Pacific. The relationships between anthropogenic radionuclides and oceanographic parameters such as salinity and nutrients were examined. The 137Cs concentrations in the western South Pacific (the Tasman Sea) and the eastern South Pacific were negatively correlated with the phosphate concentration, whereas there is no correlation between the 137Cs and nutrients concentrations in the South Pacific subtropical gyre. The mutual relationships between anthropogenic radionuclides and oceanographic parameters are important for better understanding of transport processes of anthropogenic radionuclides and their fate in the South Pacific.

  10. Characterization of selected radionuclides in sediment and surface water in Standley Lake, Great Western Reservoir, and Mower Reservoir, Jefferson County, Colorado, 1992

    USGS Publications Warehouse

    Clow, D.W.; Johncox, D.A.

    1995-01-01

    Lake sediment and surface water from Standley Lake, Great Western Reservoir, and Mower Reservoir, near Denver, Colorado, were sampled and analyzed for selected radionuclides during August through October, 1992. Sample concentrations were summarized and compared to results from a study conducted in 1983-84. Median plutonium-239,240 (239,240Pu) concentrations in lake-sediment grab samples from Standley Lake, Great Western Reservoir, and Mower Reservoir were 0.037, 0.105, and 0.351 picocuries per gram (pCi/g). The maximum concen- tration of 239,240Pu dissolved in lake water was 0.009 picocuries per liter, substantially below limits suggested by the Colorado Department of Health and the Environment. Dissolved concentrations of gross alpha and uranium isotopes were below National Drinking Water Standards in all water samples. There was no statistically significant difference between 239,240Pu concentration in lake-sediment grab samples collected from Standley Lake in 1983-84 and in 1992; however, there was a small, but statistically significant, difference at Great Western Reservoir (p<0.05). In 1992 at Great Western Reservoir, median 239,240Pu concentrations were 0.040 pCi/g lower than in 1983-84. There was a small, but statistically significant (p<0.05) difference in 239,240Pu concentrations in lake- bottom-sediment cores collected in 1983-84 and in 1992. Measured concentrations tended to be higher in 1983-84 than in 1992. The differences were greatest at concentrations above 1.5 pCi/g; in those samples concentrations were 10 to 30% higher in 1983-84 than in 1992.

  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. Fallout radioactivity in soil and food samples in the Ukraine: Measurements of iodine, plutonium, cesium, and strontium isotopes

    SciTech Connect

    Hoshi, Masaharu; Yamamoto, Masayoshi; Kawamura, Hisao; Shinohara, Kunihiko; Shibata, Yoshisada; Kozlenko, M.T.; Takatsuji, Toshihiro; Yamashita, Shunichi; Namba, Hiroyuki; Yokoyama, Naokata

    1994-08-01

    To estimate the level and distribution of fallout attributable to the Chernobyl accident in the Ukraine, the authors sampled several kinds of substances at Korosten, Zhitomir and at Katyuzhanka, Vishgorod, Kiev in the Ukraine, and measured {sup 137}Cs, {sup 134}Cs, {sup 90}Sr, {sup 129}I, {sup 238}Pu, {sup 239,240}Pu, and the density of {sup 127}I (stable). The substances investigated were soil, dry milk, wheat, rye, drinking water, and mushrooms. Except for the mushrooms collected, which were sampled at Katyuzhanka, Vishgorod, and at Kiev, all substances were at Korosten, Zhitomir. The activity of {sup 137}Cs, {sup 134}Cs, {sup 90}Sr, {sup 238}Pu, and {sup 239,240}Pu were all higher in soil and mushrooms than in the other four substances. The activity of {sup 137}Cs was 960 and 1,210 Bq kg{sup {minus}1} in the two soil samples and 6,110 of Bq kg{sup {minus}1} in the mushrooms. The activity of {sup 134}Cs was {approximately} 15% of {sup 137}Cs in the two soil samples while <3% of {sup 137}Cs in the mushrooms. The activity concentration level of {sup 90}Sr as compared to {sup 137}Cs concentration was 15-31% in food samples other than mushrooms but only 1.9% in mushrooms and 1.4 and 1.2% in the two soil samples. The radioactivity ratios, {sup 238}Pu:{sup 239,240}Pu and {sup 239,240}Pu:{sup 137}Cs, suggested that the proportion of cesium radioisotopes and {sup 239,240}Pu in the soil attributable to the Chernobyl accident was {approximately}100% and 10-20%, respectively, while {approximately} 100% of {sup 239,240}Pu in the mushrooms was attributable to the accident. The activity of {sup 129}I was small but the ratio of {sup 129}I:{sup 127}I in the two soil samples was 4.3x10{sup {minus}8} and 1.0x10{sup {minus}7}, which is {approximately} 10 times larger than that in the global fallout. These results suggest that the areas where the soil was sampled are iodine-deficient and were contaminated slightly by the Chernobyl accident. 12 refs., 1 fig., 3 tabs.

  13. 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

  14. Interpretation of Actinide-Distribution Data Obtained from Non-Destructive and Destructive Post-Test Analyses of an Intact-Core Column of Culebra Dolomite

    SciTech Connect

    LUCERO, DANIEL A; PERKINS, W GEORGE

    1999-08-26

    The US DOE, with technical assistance from Sandia National Laboratories, has successfully received EPA certification and opened the Waste Isolation Pilot Plant (WIPP), a nuclear waste disposal facility located approximately 42 km east of Carlsbad, New Mexico. Performance assessment analyses indicate that human intrusions by inadvertent, intermittent drilling for resources provide the only credible mechanisms for releases of radionuclides from the disposal system. In modeling long-term brine releases, subsequent to a drilling event, potential migration pathways through the permeable layers of rock above the Salado formation were analyzed. Major emphasis is placed on the Culebra Member of the Rustler Formation because this is the most transmissive geologic layer overlying the WIPP site. In order to help quantify parameters for the calculated releases, radionuclide transport experiments have been earned out using intact-core columns obtained from the Culebra dolomite member of the Rustler Formation within the WIPP site. This paper deals primarily with results of analyses for {sup 241}Pu and {sup 241}Am distributions developed during transport experiments in one of these cores. Transport experiments were done using a synthetic brine that simulates Culebra brine at the core recovery location (the WIPP air-intake shaft--AIS). Hydraulic characteristics (i.e., apparent porosity and apparent dispersion coefficient) for intact-core columns were obtained via experiments using the conservative tracer {sup 22}Na. Elution experiments carried out over periods of a few days with tracers {sup 232}U and {sup 239}Np indicated that these tracers were weakly retarded as indicated by delayed elution of the species. Elution experiments with tracers {sup 241}Pu and {sup 241}Am were attempted, but no elution of either species has been observed to date, including experiments of many months' duration. In order to quantify retardation of the non-eluted species {sup 241}Pu and {sup 241}Am

  15. 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.

  16. 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

  17. 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

    Lead and copper smelting has been conducted at El Paso since the late 1800's, and as a result, environmental media near the smelter have become contaminated. A study has been conducted to investigate the sources and spatial distribution of metal pollutants (Pb, Cd, Zn, Hg, As, Cu) and concomitant tracers (Ag, In, Sb, Bi) in soils from the smelter vicinity. Sampled locations were residential and non-residential locations in El Paso (Texas, USA), Anapra (New Mexico, USA) and Ciudad Juarez (Chihuahua, Mexico). Lead isotope studies indicate that the soil Pb is derived from smelting, and is consistent with two-component mixing between lead ores from Chihuahua (northern Mexico) having 206Pb/204Pb of 18.6 - 18.8 and ores from the Hanover, New Mexico (USA) mining district with 206Pb/204Pb of ~ 17.6. The Pb isotope results also exclude other common anthropogenic Pb sources such as paint and gasoline emissions as being major contributors. Concentrations of Hg and Pb of up to 10 and 11,000 ppm were found in surface soils within 1 km of the smelter. The metal concentration results clearly indicate that soils near the smelter (< 5 km) exhibit much higher concentrations of smelter-related elements than do soils from control locations (> 10 km distant). A general trend of decreasing concentrations vs. distance from the smelter was also observed. However, the results indicate that metal concentrations vary widely even at a fixed distance from the smelter point source. This phenomenon results from a combination of natural and anthropogenic processes that disturb and re-distribute soils in the surface environment. The site conditions consist of a very arid environment with little vegetation cover that is frequently disturbed by high winds and severe episodic rainfall. To study these effects, we have investigated stratospheric fallout plutonium (239+240Pu) as a proxy measure of disturbed vs. undisturbed soil conditions. The premise is that 'undisturbed' locations will have high 239+240

  18. Accumulation of anthropogenic radionuclides in cryoconites on Alpine glaciers.

    PubMed

    Tieber, A; Lettner, H; Bossew, P; Hubmer, A; Sattler, B; Hofmann, W

    2009-07-01

    Cryoconites are airborne sediments which accumulate on the surface of glaciers. In samples of cryoconites a temperate Austrian glacier high activity concentrations of anthropogenic radionuclides were found, which stem from global and Chernobyl fallouts. Radionuclides identified were (137)Cs, (134)Cs, (238)Pu, (239+240)Pu, (90)Sr, (241)Am, (60)Co, (154)Eu, (207)Bi, and (125)Sb. Given the approximately known isotopic ratios, Cs and Pu can be separated into the contributions of either source of origin. Published (137)Cs/(134)Cs and (239+240)Pu/(238)Pu ratios were used for the discrimination of the Dachstein-glacier cryoconites according to their origin from global or Chernobyl fallout. Two different groups of cryoconites were identified, an older population dominated by nuclear weapons fallout and a younger one with predominant Chernobyl fallout. With those data a simple model was formulated to demonstrate the transition and mixing of these two populations on the glacier surface. PMID:19450909

  19. 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

  20. 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.

  1. Plutonium fractionation in southern Baltic Sea sediments.

    PubMed

    Strumińska-Parulska, Dagmara I; Skwarzec, Bogdan; Pawlukowska, Magdalena

    2012-01-01

    In this study, different chemical plutonium fractions (dissolved in water, connected to carbonates, connected to oxides, complexed with organic matter, mineral acids soluble and the rest) in sediments from the Vistula River estuary, the Gdańsk Basin and the Bornholm Deep were determined. The distribution of (239+240)Pu in analysed sediments samples was not uniform but dependent on its chemical form, depth and the sediment geomorphology. The highest amount of plutonium exists in middle parts of sediments and comes from the global atmospheric fallout from nuclear tests in 1958-1961. According to all analysed fractions, the biggest amount of (239+240)Pu was in the mobile form, connected to carbonate fractions from the Vistula River estuary, the Gulf of Gdańsk and the Bornholm Deep sediments. PMID:22612422

  2. Accumulation of anthropogenic radionuclides in cryoconites on Alpine glaciers.

    PubMed

    Tieber, A; Lettner, H; Bossew, P; Hubmer, A; Sattler, B; Hofmann, W

    2009-07-01

    Cryoconites are airborne sediments which accumulate on the surface of glaciers. In samples of cryoconites a temperate Austrian glacier high activity concentrations of anthropogenic radionuclides were found, which stem from global and Chernobyl fallouts. Radionuclides identified were (137)Cs, (134)Cs, (238)Pu, (239+240)Pu, (90)Sr, (241)Am, (60)Co, (154)Eu, (207)Bi, and (125)Sb. Given the approximately known isotopic ratios, Cs and Pu can be separated into the contributions of either source of origin. Published (137)Cs/(134)Cs and (239+240)Pu/(238)Pu ratios were used for the discrimination of the Dachstein-glacier cryoconites according to their origin from global or Chernobyl fallout. Two different groups of cryoconites were identified, an older population dominated by nuclear weapons fallout and a younger one with predominant Chernobyl fallout. With those data a simple model was formulated to demonstrate the transition and mixing of these two populations on the glacier surface.

  3. Uptake and translocation of neptunium-237, plutonium-238, plutonium-239,240, americium-241, and curium-244 by a wheat crop

    SciTech Connect

    Schulz, R.K.; Ruggieri, M.R.

    1981-07-01

    We carried out a plant uptake and translocation experiment in which a wheat crop was grown on Yolo soil contaminated with /sup 237/Np, /sup 238/Pu, /sup 239/ /sup 240/Pu, /sup 241/Am, and /sup 244/Cm. Studying pot-to-pot variability, we found the data a coefficient of variation of 21 percent. About 9 percent of this variability we ascribe to that of radioanalyses of the plant material. Both uptake and translocation of /sup 238/Pu and /sup 239/ /sup 240/Pu were found to be identical. Likewise, both uptake and translocation of /sup 241/Am and /sup 244/Cm were identical. The Pu concentration was about 10/sup 3/ lower in the grain than in the bottom one-half of the stem plus leaves.

  4. 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.

  5. Deposition of Saharan Dust in Monaco Rain 2001 2002: Radionuclides and Elemental Composition

    NASA Astrophysics Data System (ADS)

    Pham, M. K.; La Rosa, J. J.; Lee, S.-H.; Oregioni, B.; Povinec, P. P.

    2005-01-01

    Data on concentrations and activity ratios of natural and anthropogenic radio-nuclides as well as concentrations of major and trace elements in red-coloured particles (Saharan dusts) collected in Monaco rain in 2001 and 2002 (5 samples from 4 events) are presented. Different distributions of particle size as well as different activities of natural radionuclides and concentrations of trace metals have been observed for two sets of samples. The 235U/238U activity ratio is around 0.04 showing virgin natural terrestrial origin of the particles. The anthropogenic radionuclides 137Cs, 238Pu, 239+240Pu and 241Am are of global fallout origin and their annual atmospheric input to the ocean in the particulate form is estimated to be 28 37% for 137Cs, 34 45% for 239+240Pu and 36 51% for 241Am of the total annual depositional fluxes of these radionuclides to the northwest Mediterranean.

  6. Determination of plutonium content in TRR spent fuel by nondestructive neutron counting

    NASA Astrophysics Data System (ADS)

    Chen, Yen-Fu; Sheu, Rong-Jiun; Chiao, Ling-Huan; Yuan, Ming-Chen; Jiang, Shiang-Huei

    2010-07-01

    For the nuclear safeguard purpose, this work aims to nondestructively determine the plutonium content in the Taiwan Research Reactor (TRR) spent fuel rods in the storage pool before the stabilization process, which transforms the metal spent fuel rods into oxide powder. A SPent-fuel-Neutron-Counter (SPNC) system was designed and constructed to carry out underwater scan measurements of neutrons emitting from the spent fuel rod, from which the 240Pu mass in the fuel rod will be determined. The SAS2 H control module of the SCALE 5.1 code package was applied to calculate the 240Pu-to-Pu mass ratio in the TRR spent fuel rod according to the given power history. This paper presents the methodology and design of our detector system as well as the measurements of four TRR spent fuel rods in the storage pool and the comparison of the measured results with the facility declared values.

  7. The relative importance of uptake and surface adherence in determining the radionuclide contents of subterranean crops.

    PubMed

    Corey, J C; Boni, A L; Watts, J R; Adriano, D C; McLeod, K W; Pinder, J E

    1983-01-01

    The adherence of Pu-bearing particles to external surfaces of carrots, turnips, red potatoes, and sweet potatoes accounted for greater than or equal to 93% of their total Pu content. Uptake, which was measured as Pu content in peeled crops, accounted for less than or equal to 7%. Plutonium concentrations in most peeled crops were below background, and consequently, uptake could not be conclusively demonstrated. However, uptake accounted for most of the 137Cs, 40K, and 226Ra contents of subterranean crops. Concentration ratios for total radionuclide contents (i.e. surface adherence plus uptake) ranged from 3.9 X 10(1) for 40K, to 1.1 X 10(-2) for 239, 240Pu. Approximately 1.5 X 10(-3) pCi 239, 240Pu adhered per cm2 of subterranean crop surface per 1 pCi Pu/g of soil.

  8. 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.

  9. 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

  10. Biogeochemical studies of long-lived radionuclides in marine environments

    SciTech Connect

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

    1985-01-01

    Research results from several studies relevant to seabed dispoal of radioactive wastes are briefly discussed. The studies include: (1) mobilization of plutonium from Enewetak and Bikini lagoon sediments to seawater; (2) concentrations of /sup 90/Sr, /sup 137/Cs, /sup 239+240/Pu, /sup 241/Am, /sup 207/Bi and /sup 210/Pb-/sup 210/Bi-/sup 210/Po in fish from the Marshall Islands; and (3) plutonium in northeast Atlantic sediments. (ACR)

  11. Radionuclide Concentrations in Honey Bees from Area G at TA-54 during 1998

    SciTech Connect

    Haarmann, T.K.; Fresquez, P.R.

    1999-06-01

    Honey bees were collected from two colonies located at Los Alamos National Laboratory's Area G, Technical Area 54, and from one control (background) colony located near Jemez Springs, NM. Samples were analyzed for various radionuclides. Area G sample results from both colonies were higher than the upper (95%) level background concentration for {sup 239,240}Pu, {sup 3}H, and total uranium. Sample results from one colony were higher than the upper (95%) level background concentration for {sup 238}Pu.

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

    PubMed

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

    2016-10-01

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

  13. Distribution and behaviour of transuranic elements in the physical and biological compartments of the channel french shore

    NASA Astrophysics Data System (ADS)

    Germain, P.; Miramand, P.

    1984-06-01

    Biological samples (algae, suspension feeders molluscs living in contact with sediments, annelids), sediments and sea water were taken at 5 stations along the Channel shore from 1978 to 1981 in order to determine 239+240Pu, 238Pu, 241Am and 244Cm levels. In Northern Cotentin, radioactivity levels for 239+240Pu, 238Pu and 241Am were respectively about 1-10, 0.5-7 and 1-19 pCi kg -1 fresh weight in biological samples, 24-90, 11-28 and 24-31 pCi kg -1 dry weight in sediments, 1-7, 5-40 and 2-15 fCi 1 -1 in sea water. For stations far from the La Hague outlet (Seine river and Mont Saint Michel bays) levels for 239+240Pu, 238Pu and 241Am were respectively about 0.3-5, 0.1-2 and 0.2-3 pCi kg -1 fresh weight in biological samples, 30-80, 5-26 and 14-40 pCi kg -1 dry weight in sediments, and 1-, 3-4 and 3-8 fCi 1 -1 in sea water. Labelling of industrial wastes was demonstrated by the values of the 238Pu/ 239+240Pu ratios. The evolution of plutonium isotopes in sea water and in the other environmental compartments and the bio-availability of americium are discussed. Sediment-animal transfers are quantified and their processes specified. An assessment of plutonium and americium hazards from ingestion of molluscs shows that the ingested activity represents 1.1×10 -4 only of the ALI (ingestion) recommended by ICRP for members of the public.

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

    PubMed

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

    2014-12-01

    Plutonium (Pu), americium (Am), and curium (Cm) activities were measured in sediments from a former radioactive waste disposal basin located on the Savannah River Site, South Carolina, and in subsurface aquifer sediments collected downgradient from the basin. In situ Kd values (Pu concentration ratio of sediment/groundwater) derived from this field data and previously reported groundwater concentration data compared well to laboratory Kd values reported in the literature. Pu isotopic signatures confirmed multiple sources of Pu contamination. The ratio of (240)Pu/(239)Pu was appreciably lower for sediment samples compared to the associated groundwater. This isotopic ratio difference may be explained by the following: (1) (240)Pu produced by decay of (244)Cm may exist predominantly in high oxidation states (Pu(V)O2(+) and Pu(VI)O2(2+)) compared to Pu derived from the disposed waste effluents, and (2) oxidized forms of Pu sorb less to sediments than reduced forms of Pu. Isotope-specific Kd values calculated from measured Pu activities in the sediments and groundwater indicated that (240)Pu, which is derived primarily from the decay of (244)Cm, had a value of 10 ± 2 mL g(-1), whereas (239)Pu originating from the waste effluents discharged at the site had a value of 101 ± 8 mL g(-1). One possible explanation for the isotope-specific sorption behavior is that (240)Pu likely existed in the weaker sorbing oxidation states, +5 or +6, than (239)Pu, which likely existed in the +3 or +4 oxidation states. Consequently, remediation strategies for radioactively contaminated systems must consider not only the discharged contaminants but also their decay products. In this case, mitigation of Cm as well as Pu will be required to completely address Pu migration from the source term. PMID:25350948

  15. New evaluation of the alpha and gamma emission intensities in the decay of (244)Cm.

    PubMed

    Badikov, Sergey A; Chechev, Valery P

    2016-03-01

    A method for self-consistent evaluation of the absolute emission probabilities for particles and photons accompanying radionuclide decays was applied to the evaluation of the (244)Cm alpha decay data. The absolute emission probabilities evaluated by the method meet the accurate balance relationships. The self-consistency of the results was reached through an iterative scheme of calculations, using the DDEP recommended probabilities for alpha transitions to the five (240)Pu highly excited levels as an initial approximation.

  16. Analysis of core soil and water samples from the Cactus Crater Disposal Site at Enewetak atoll

    SciTech Connect

    Robison, W.L.; Noshkin, V.E.

    1981-02-18

    Core soil samples and water samples were collected from the Cactus Crater Disposal Site at Enewetak for analysis of /sup 137/Cs, /sup 90/Sr, /sup 239 +240/Pu and /sup 241/Am by both gamma spectroscopy and, through a contractor laboratory, by wet chemistry procedures. The samples processing methods, the analytical methods and the analytical quality control are all procedures developed for the continuing Marshall Island radioecology and dose assessment work.

  17. Organic nature of colloidal actinides transported in surface water environments.

    PubMed

    Santschi, Peter H; Roberts, Kimberly A; Guo, Laodong

    2002-09-01

    Elevated levels of (239,240)Pu and 241Am have been present in surficial soils of the Rocky Flats Environmental Technology Site (RFETS), CO, since the 1960s, when soils were locally contaminated in the 1960s by leaking drums stored on the 903 Pad. Further dispersion of contaminated soil particles was by wind and water. From 1998 until 2001, we examined actinide ((239,240)Pu and 241Am) concentrations and phase speciation in the surface environment at RFETS through field studies and laboratory experiments. Measurements of total (239,240)Pu and 241Am concentrations in storm runoff and pond discharge samples, collected during spring and summer times in 1998-2000, demonstrate that most of the (239,240)Pu and 241Am transported from contaminated soils to streams occurred in the particulate (> or = 0.45 microm; 40-90%) and colloidal (approximately 2 nm or 3 kDa to 0.45 microm; 10-60%) phases. Controlled laboratory investigations of soil resuspension, which simulated storm and erosion events, confirmed that most of the Pu in the 0.45 microm filter-passing phase was in the colloidal phase (> or = 80%) and that remobilization of colloid-bound Pu during soil erosion events can be greatly enhanced by humic and fulvic acids present in these soils. Most importantly, isoelectric focusing experiments of radiolabeled colloidal matter extracted from RFETS soils revealed that colloidal Pu is in the four-valent state and is mostly associated with a negatively charged organic macromolecule with a pH(IEP) of 3.1 and a molecular weight of 10-15 kDa, rather than with the more abundant inorganic (iron oxide and clay) colloids. This finding has important ramifications for possible remediation, erosion controls, and land-management strategies. PMID:12322742

  18. 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.

  19. Optimization of Heterogeneous Utilization of Thorium in PRWs to Enhance Proliferation Resistance & Reduce Waste

    SciTech Connect

    Mujid Kazimi

    2003-12-18

    Typical pressurized water reactors, although loaded with uranium fuel, produce 225 to 275 kg of plutonium per gigawatt year of operation. Although the spent fuel is highly radioactive, it nevertheless offers a potential proliferation pathway because the plutonium is relatively easy to separate, amounts to many critical masses, and aside from the alpha (n reaction on the 240 Pu isotope) does not present any significant intrinsic barrier to weapon assembly

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

    PubMed

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

    2016-10-01

    Surface of glaciers is covered by mineral and organic dust, together with microorganisms forming cryoconite granules. Despite fact that glaciers and ice sheets constitute significance part of land surface, reservoir of freshwater, and sites of high biological production, the knowledge on the cryoconite granules still remain unsatisfactory. This study presents information on radionuclide and heavy metal contents in cryoconites. Cryoconites collected from the Hans Glacier in SW Spitsbergen reveal high activity concentrations of anthropogenic ((238,239,240)Pu, (137)Cs, (90)Sr) and natural ((210)Pb) radionuclides. The (238)Pu/(239+240)Pu activity ratios in these cryoconites significantly exceed the mean global fallout ratio (0.025). The (238)Pu/(239+240)Pu ranged from 0.064 to 0.118. The (239+240)Pu/(137)Cs varied from 0.011 ± 0.003 to 0.030 ± 0.007. Such activity ratios as observed in these cryoconites were significantly higher than the values characterizing global fallout, pointing to possible contributions of these radionuclides from other sources. Heavy metals (Pb, Cd, Cu, Zn, Fe, and Mn) in cryoconites exceed both UCC concentrations and local rocks' concentrations, particularly for cadmium. The concentration ratios of stable lead isotopes ((206)Pb/(207)Pb, (208)Pb/(206)Pb) were determined to discriminate between the natural and anthropogenic sources of Pb in cryoconites and to confirm the strong anthropogenic contribution to heavy metal deposition in the Arctic. In investigated cryoconite holes, two groups of invertebrates, both extremophiles, Tardigrada and Rotifera were detected. Our study indicate that cryoconites are aggregates of mineral and organic substances on surfaces of glaciers are able to accumulate large amounts of airborne pollutants bound to extracellular polymeric substances secreted by microorganisms. PMID:27372266

  1. 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.

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

    PubMed

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

    2014-04-01

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

  3. 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.

  4. Solubility of hot fuel particles from Chernobyl--influencing parameters for individual radiation dose calculations.

    PubMed

    Garger, Evgenii K; Meisenberg, Oliver; Odintsov, Oleksiy; Shynkarenko, Viktor; Tschiersch, Jochen

    2013-10-15

    Nuclear fuel particles of Chernobyl origin are carriers of increased radioactivity (hot particles) and are still present in the atmosphere of the Chernobyl exclusion zone. Workers in the zone may inhale these particles, which makes assessment necessary. The residence time in the lungs and the transfer in the blood of the inhaled radionuclides are crucial for inhalation dose assessment. Therefore, the dissolution of several kinds of nuclear fuel particles from air filters sampled in the Chernobyl exclusion zone was studied. For this purpose filter fragments with hot particles were submersed in simulated lung fluids (SLFs). The activities of the radionuclides (137)Cs, (90)Sr, (239+240)Pu and (241)Am were measured in the SLF and in the residuum of the fragments by radiometric methods after chemical treatment. Soluble fractions as well as dissolution rates of the nuclides were determined. The influence of the genesis of the hot particles, represented by the (137)Cs/(239+240)Pu ratio, on the availability of (137)Cs was demonstrated, whereas the dissolution of (90)Sr, (239+240)Pu and (241)Am proved to be independent of genesis. No difference in the dissolution of (137)Cs and (239+240)Pu was observed for the two applied types of SLF. Increased solubility was found for smaller hot particles. A two-component exponential model was used to describe the dissolution of the nuclides as a function of time. The results were applied for determining individual inhalation dose coefficients for the workers at the Chernobyl construction site. Greater dose coefficients for the respiratory tract and smaller coefficients for the other organs were calculated (compared to ICRP default values). The effective doses were in general lower for the considered radionuclides, for (241)Am even by one order of magnitude.

  5. The Neutron Capture Cross Sections of 237NP(n,{gamma}) and 240Pu(n,{gamma}) and Its Relevance in the Transmutation of Nuclear Waste

    SciTech Connect

    Guerrero, C.; Koehler, Paul Edward; Collaboration, n_TOF

    2008-01-01

    Neutron capture cross sections of actinides are of great relevance for the Transmutation of Nuclear Waste in Accelerator Driven Systems (ADS) and Generation-IV reactors. The neutron capture cross sections of {sup 237}Np and {sup 240}Pu were measured at the n{_}TOF facility with a Total Absorption Calorimeter. The data have been analyzed with the SAMMY code. The corresponding covariance matrices have been generated. The final cross sections are presented and compared to the previously existing ones.

  6. Sediment studies at Bikini Atoll part 2. inventories of transuranium elements in surface sediments

    SciTech Connect

    Noshkin, V.E.; Eagle, R.J.; Wong, K.M.; Robison, W.L.

    1997-10-01

    This is the second of three reports on Bikini sediment studies, which discusses the concentrations and inventories of {sup 241}Am and {sup 239+240}Pu in sediments from the lagoon. Surface sediment samples were collected from 87 locations over the entire lagoon at Bikini Atoll during 1979. The collections were made to map the distribution of long-lived radionuclides associated with the bottom material and to show what modifications occurred in the composition of the sediment as a result of the testing program. Present inventories for {sup 241}Am and {sup 239+240}Pu in the surface 2 cm of sediment are estimated to be 14 and 17 TBq, respectively. These values are estimated to represent only 14% of the total inventory in the sediment column. Sediment inventories of {sup 239+240}Pu and {sup 241}Am are changing only slowly with time through chemical- physical processes that continuously mobilize small amounts of the transuranics to the water column. The lowest concentrations and inventories are associated with deposits logoonward of the eastern reef.

  7. 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

  8. 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.

  9. Source and long-term behavior of transuranic aerosols in the WIPP environment.

    PubMed

    Thakur, P; Lemons, B G

    2016-10-01

    Source and long-term behavior transuranic aerosols ((239+240)Pu, (238)Pu, and (241)Am) in the ambient air samples collected at and near the Waste Isolation Pilot Plant (WIPP) deep geologic repository site were investigated using historical data from an independent monitoring program conducted by the Carlsbad Environmental Monitoring and Research Center and an oversight monitoring program conducted by the management and operating contractor for WIPP at and near the facility. An analysis of historical data indicates frequent detections of (239+240)Pu and (241)Am, whereas (238)Pu is detected infrequently. Peaks in (239+240)Pu and (241)Am concentrations in ambient air generally occur from March to June timeframe, which is when strong and gusty winds in the area frequently give rise to blowing dust. Long-term measurements of plutonium isotopes (1985-2015) in the WIPP environment suggest that the resuspension of previously contaminated soils is likely the primary source of plutonium in the ambient air samples from WIPP and its vicinity. There is no evidence that WIPP is a source of environmental contamination that can be considered significant by any health-based standard. PMID:27394421

  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.

  11. 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.

  12. Source and long-term behavior of transuranic aerosols in the WIPP environment.

    PubMed

    Thakur, P; Lemons, B G

    2016-10-01

    Source and long-term behavior transuranic aerosols ((239+240)Pu, (238)Pu, and (241)Am) in the ambient air samples collected at and near the Waste Isolation Pilot Plant (WIPP) deep geologic repository site were investigated using historical data from an independent monitoring program conducted by the Carlsbad Environmental Monitoring and Research Center and an oversight monitoring program conducted by the management and operating contractor for WIPP at and near the facility. An analysis of historical data indicates frequent detections of (239+240)Pu and (241)Am, whereas (238)Pu is detected infrequently. Peaks in (239+240)Pu and (241)Am concentrations in ambient air generally occur from March to June timeframe, which is when strong and gusty winds in the area frequently give rise to blowing dust. Long-term measurements of plutonium isotopes (1985-2015) in the WIPP environment suggest that the resuspension of previously contaminated soils is likely the primary source of plutonium in the ambient air samples from WIPP and its vicinity. There is no evidence that WIPP is a source of environmental contamination that can be considered significant by any health-based standard.

  13. Risk-Quantified Decision-Making at Rocky Flats

    SciTech Connect

    Myers, Jeffrey C.

    2008-01-15

    Surface soils in the 903 Pad Lip Area of the Rocky Flats Environmental Technology Site (RFETS) were contaminated with {sup 239/240}Pu by site operations. To meet remediation goals, accurate definition of areas where {sup 239/240}Pu activity exceeded the threshold level of 50 pCi/g and those below 50- pCi/g needed definition. In addition, the confidence for remedial decisions needed to be quantified and displayed visually. Remedial objectives needed to achieve a 90 percent certainty that unremediated soils had less than a 10 percent chance of {sup 239/240}Pu activity exceeding 50-pCi/g. Removing areas where the chance of exceedance is greater than 10 percent creates a 90 percent confidence in the remedial effort results. To achieve the stipulated goals, the geostatistical approach of probability kriging (Myers 1997) was implemented. Lessons learnt: Geostatistical techniques provided a risk-quantified approach to remedial decision-making and provided visualizations of the excavation area. Error analysis demonstrated compliance and confirmed that more than sufficient soils were removed. Error analysis also illustrated that any soils above the threshold that were not removed would be of nominal activity. These quantitative approaches were useful from a regulatory, engineering, and stakeholder satisfaction perspective.

  14. Plutonium and 210Pb distributions in northeast Atlantic sediments: subsurface anomalies caused by non-local mixing

    NASA Astrophysics Data System (ADS)

    Smith, John Norton; Boudreau, Bernard P.; Noshkin, Victor

    1986-12-01

    The depth distributions of 210Pb and 239,240Pu measured in a suite of box cores collected from water depths of 4000-5000 m in the northeast Atlantic Ocean exhibit pronounced subsurface maxima caused by sediment reworking by benthic infauna. Small-scale spatial heterogeneity in bioturbation rates is indicated by large differences in tracer profiles from duplicate cores separated only by a few centimeters. 210Pb and 239,240Pu activity distributions from each subcore exhibit a high degree of correlation, and most tracer profiles exhibit one or more subsurface maxima. One-dimensional, "biodiffusion" analogue models do not adequately simulate the principal features of this data set. However, an inverse "conveyer belt" mixing model which simulates subsurface egestion (or a functionally equivalent process) of surficial material which is enriched both in organic debris and radioactive tracers can reproduce the subsurface tracer maxima. Single-event and continuous subsurface egestion models have been formulated and solved for different "feeding rates" and background biodiffusive fields. The single-event model provides a better fit to the data and, in particular, ensures the observed, high degree of correlation between the 210Pb and 239,240Pu activity profiles, regardless of the different tracer input functions. The most likely candidate responsible for subsurface tracer egestion is a large infaunal worm of the phylum Sipunculida which dominates the biomass below a depth of 3 cm.

  15. 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.

  16. 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.

  17. 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.

  18. 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.

  19. Deposition of artificial radionuclides from atmospheric Nuclear Weapon Tests estimated by soil inventories in French areas low-impacted by Chernobyl.

    PubMed

    Le Roux, Gaël; Duffa, Céline; Vray, Françoise; Renaud, Philippe

    2010-03-01

    Soil inventories of anthropogenic radionuclides were investigated in altitudinal transects in 2 French regions, Savoie and Montagne Noire. Rain was negligible in these 2 areas the days after the Chernobyl accident. Thus anthropogenic radionuclides are coming hypothetically only from Global Fallout following Atmospheric Nuclear Weapon Tests. This is confirmed by the isotopic signatures ((238)Pu/(239+240)Pu; (137)Cs/(239+240)Pu; and (241)Am/(239+240)Pu) close to Global Fallout value. In Savoie, a peat core age-dated by (210)Pb(ex) confirmed that the main part of deposition of anthropogenic radionuclides occurred during the late sixties and the early seventies. In agreement with previous studies, the anthropogenic radionuclide inventories are well correlated with the annual precipitations. However, this is the first time that a study investigates such a large panel of annual precipitation and therefore of anthropogenic radionuclide deposition. It seems that at high-altitude sites, deposition of artificial radionuclides was higher possibly due to orographic precipitations. PMID:19969404

  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. 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

  2. Development of Metallic Magnetic Calorimeters for Nuclear Safeguards Applications

    SciTech Connect

    Bates, Cameron Russell

    2015-03-11

    Many nuclear safeguards applications could benefit from high-resolution gamma-ray spectroscopy achievable with metallic magnetic calorimeters. This dissertation covers the development of a system for these applications based on gamma-ray detectors developed at the University of Heidelberg. It demonstrates new calorimeters of this type, which achieved an energy resolution of 45.5 eV full-width at half-maximum at 59.54 keV, roughly ten times better than current state of the art high purity germanium detectors. This is the best energy resolution achieved with a gamma-ray metallic magnetic calorimeter at this energy to date. In addition to demonstrating a new benchmark in energy resolution, an experimental system for measuring samples with metallic magnetic calorimeters was constructed at Lawrence Livermore National Laboratory. This system achieved an energy resolution of 91.3 eV full-width at half-maximum at 59.54 keV under optimal conditions. Using this system it was possible to characterize the linearity of the response, the count-rate limitations, and the energy resolution as a function of temperature of the new calorimeter. With this characterization it was determined that it would be feasible to measure 242Pu in a mixed isotope plutonium sample. A measurement of a mixed isotope plutonium sample was performed over the course of 12 days with a single two-pixel metallic magnetic calorimeter. The relative concentration of 242Pu in comparison to other plutonium isotopes was determined by direct measurement to less than half a percent accuracy. This is comparable with the accuracy of the best-case scenario using traditional indirect methods. The ability to directly measure the relative concentration of 242Pu in a sample could enable more accurate accounting and detection of indications of undeclared activities in nuclear safeguards, a better constraint on source material in forensic samples containing plutonium, and improvements in verification in a future plutonium

  3. Reproducibility and calibration of MMC-based high-resolution gamma detectors

    DOE PAGES

    Bates, C. R.; Pies, C.; Kempf, S.; Hengstler, D.; Fleischmann, A.; Gastaldo, L.; Enss, C.; Friedrich, S.

    2016-07-15

    Here, we describe a prototype γ-ray detector based on a metallic magnetic calorimeter with an energy resolution of 46 eV at 60 keV and a reproducible response function that follows a simple second-order polynomial. The simple detector calibration allows adding high-resolution spectra from different pixels and different cool-downs without loss in energy resolution to determine γ-ray centroids with high accuracy. As an example of an application in nuclear safeguards enabled by such a γ-ray detector, we discuss the non-destructive assay of 242Pu in a mixed-isotope Pu sample.

  4. Actinide neutron-induced fission cross section measurements at LANSCE

    SciTech Connect

    Tovesson, Fredrik K; Laptev, Alexander B; Hill, Tony S

    2010-01-01

    Fission cross sections of a range of actinides have been measured at the Los Alamos Neutron Science Center (LANSCE) in support of nuclear energy applications in a wide energy range from sub-thermal energies up to 200 MeV. A parallel-plate ionization chamber are used to measure fission cross sections ratios relative to the {sup 235}U standard while incident neutron energies are determined using the time-of-flight method. Recent measurements include the {sup 233,238}U, {sup 239-242}Pu and {sup 243}Am neutron-induced fission cross sections. Obtained data are presented in comparison with ex isting evaluations and previous data.

  5. Radiological Aspects of Deep-Burn Fusion-Fission Hybrid Waste in a Repository

    SciTech Connect

    Shaw, H F; Blink, J A; Farmer, J C; Karmer, K J; Latkowski, J F; Zhao, P

    2008-11-25

    The quantity, radioactivity, and isotopic characteristics of the spent fission fuel from a hybrid fusion-fission system capable of extremely high burnups are described. The waste generally has higher activity per unit mass of heavy metal, but much lower activity per unit energy generated. The very long-term radioactivity is dominated by fission products. Simple scaling calculations suggest that the dose from a repository containing such waste would be dominated by {sup 129}I, {sup 135}Cs, and {sup 242}Pu. Use of such a system for generating energy would greatly reduce the need for repository capacity.

  6. Reproducibility and calibration of MMC-based high-resolution gamma detectors

    NASA Astrophysics Data System (ADS)

    Bates, C. R.; Pies, C.; Kempf, S.; Hengstler, D.; Fleischmann, A.; Gastaldo, L.; Enss, C.; Friedrich, S.

    2016-07-01

    We describe a prototype γ-ray detector based on a metallic magnetic calorimeter with an energy resolution of 46 eV at 60 keV and a reproducible response function that follows a simple second-order polynomial. The simple detector calibration allows adding high-resolution spectra from different pixels and different cool-downs without loss in energy resolution to determine γ-ray centroids with high accuracy. As an example of an application in nuclear safeguards enabled by such a γ-ray detector, we discuss the non-destructive assay of 242Pu in a mixed-isotope Pu sample.

  7. Sources, distribution, and mobility of plutonium and radiocesium in soils, sediments and water of the Hudson River Estuary and watershed

    SciTech Connect

    Linsalata, P.

    1984-01-01

    Results of /sup 239/ /sup 240/Pu, /sup 238/Pu and /sup 137/Cs measurements are reported for soil cores sampled within the watershed, for many sediment cores and surface dredge samples taken along the length of the Hudson River Estuary and for water samples collected on a continuous basis in both fresh and estuarine reaches. Accumulations of /sup 239/ /sup 240/Pu and /sup 137/Cs measured within sediment cores taken from discrete regions of the river-estuary were summed to arrive at total sediment inventories of 1.6 +/- 0.7 Ci and 53 +/- 20 Ci, respectively. The variability observed in the sediment accumulation of radionuclides is discussed in terms of the physical and chemical characteristics of the river-estuary. Plutonium-239,240 and /sup 137/Cs were similary distributed in sediments and water sampled from fresh water reaches of the Hudson with activity ratios (i.e., /sup 239/ /sup 240/Pu//sup 1/2number/sup 7/Cs) ranging from 0.01 to 0.03. Distribution coefficients, which were determined both in vitro and in situ were similar for both nuclides (i.e., from 1 x 10/sup 5/ to 3 x 10/sup 5/ L.kg/sup -1/) in fresh water, but diverged significantly (as a result of increased /sup 137/Cs solubility) in brackish waters that exhibited chlorinities in excess of 1-2 g Cl/sup -/.L/sup -1/. The concentrations of /sup 239/ /sup 240/Pu and /sup 137/Cs observed in fresh water samples were primarily functions of the suspended load. Approximately 60-70% of the annual downstream transport of /sup 239/ /sup 240/Pu and /sup 137/Cs calculated during 1980 and 1981 (i.e., 4 +/- 0.5 mCi and 515 +/- 84 mCi, respectively) was associated with suspended particulates greater than or equal to 0.45 ..mu..m. An empirical model was developed to determine the rates of vertical migration of these nuclides in soils of the watershed.

  8. Organic matter controls on iodine and plutonium in atmospheric depositions, streams, and soils in the Fukushima Prefecture

    NASA Astrophysics Data System (ADS)

    Xu, C.; Zhang, S.; Sugiyama, Y.; Ohte, N.; Ho, Y. F.; Fujitake, N.; Kaplan, D. I.; Yeager, C. M.; Schwehr, K. A.; Santschi, P. H.

    2015-12-01

    In order to assess how environmental factors are controlling the distribution and migration of radioiodine and plutonium that were emitted from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, we quantified iodine and 239,240Pu 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. A ranking of the land uses by their stable 127I and by their 239,240Pu concentrations were quite distinct from that of 134,137Cs, indicating 137Cs might not be a good geochemical proxy for radioactive 129I or Pu in the long-term, post-FDNPP accident. Being a proxy for the long-term fate of 129I, soil 127I content was well correlated to soil organic matter (SOM) content, regardless of land use type, suggesting that SOM might be an important factor controlling iodine biogeochemistry. Other soil chemical properties, such as Eh and pH, had strong correlations to soil 127I content, but only within a given land use (e.g., within urban soils). Organic carbon (OC) and Eh were positively, and pH was negatively correlated to 127I concentrations in surface water and rain samples. It is also noticeable that 127I in the bulk deposition was concentrated along the rainwater passage likely due to plant evapotranspiration activity, with all inorganic iodine being completely converted to organo-iodine by plant organic matter. 239,240Pu activities of all soil samples were well within the global fallout range, but the Fukushima-derived 239,240Pu was detectable at a distance ~61 km away, NW of FDNPP. However, it is confined to the litter layer, even three years after the FDNPP accident-derived emissions. 239,240Pu activities were significantly correlated with soil OC and nitrogen contents, indicating Pu may be associated with nitrogen-containing SOM, similar to what has been observed at other locations in the United States, e.g., Savannah River Site (SRS) and Rocky Flats

  9. 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

  10. Isomeric ratio measurements with the ILL LOHENGRIN spectrometer

    NASA Astrophysics Data System (ADS)

    Chebboubi, A.; Kessedjian, G.; Litaize, O.; Serot, O.; Faust, H.; Bernard, D.; Blanc, A.; Köster, U.; Méplan, O.; Mutti, P.; Sage, C.

    2016-03-01

    The modelling of γ heating and neutron damage inside a nuclear reactor is essential to design the next generation of nuclear reactors. The determination of the fission fragment momentum is a key element to perform accurate calculations of the γ heating. One way to assess this information is to look at the isomeric ratio of different nuclei. According to the lifetime of the isomeric state, different experimental techniques were developed at the LOHENGRIN spectrometer. A focus on the measurement of isomeric ratios of 136I in neutron induced fission of 241Pu is presented. A discussion with the current assumptions used in the evaluation process for isomeric ratio is also shown.

  11. 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.

  12. 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.

  13. 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

  14. 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.

  15. The effect of carbonate soil on transport and dose estimates for long-lived radionuclides at a U.S. Pacific test site

    SciTech Connect

    Conrado, C L; Hamilton, T F; Robison, W L; Stoker, A C

    1999-01-01

    The US conducted a series of nuclear tests from 1946 to 1958 at Bikini, a coral atoll, in the Marshall Islands (MI). The aquatic and terrestrial environments of the atoll are still contaminated with several long-lived radionuclides that were generated during testing. The four major radionuclides found in terrestrial plants and soils are Cesium-137 ({sup 137}Cs), Strontium-90 ({sup 90}Sr), Plutonium-239+240 ({sup 239+240}Pu) and Americium-241 ({sup 241}Am). {sup 137}Cs in the coral soils is more available for uptake by plants than {sup 137}Cs associated with continental soils of North America or Europe. Soil-to-plant {sup 137}Cs median concentration ratios (CR) (kBq kg{sup {minus}1} dry weight plant/kBq kg{sup {minus}1} dry weight soil) for tropical fruits and vegetables range between 0.8 and 36, much larger than the range of 0.005 to 0.5 reported for vegetation in temperate zones. Conversely, {sup 90}Sr median CRs range from 0.006 to 1.0 at the atoll versus a range from 0.02 to 3.0 for continental silica-based soils. Thus, the relative uptake of {sup 137}Cs and {sup 90}Sr by plants in carbonate soils is reversed from that observed in silica-based soils. The CRs for {sup 239+240}Pu and {sup 241}Am are very similar to those observed in continental soils. Values range from 10{sup {minus}6} to 10{sup {minus}4} for both {sup 239+240}Pu and {sup 241}Am. No significant difference is observed between the two in coral soil.

  16. 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.

  17. 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.

  18. Historical trace element distribution in sediments from the Mississippi River delta

    USGS Publications Warehouse

    Swarzenski, P.W.; Baskaran, M.; Rosenbauer, R.J.; Orem, W.H.

    2006-01-01

    Five sediment cores were collected on the shelf of the inner Mississippi Bight in June 2003 for a suite of radionuclides to establish geochronologies and trace elements to examine patterns of contaminant deposition and accumulation. Core sites were chosen to reflect a matrix of variable water depths, proximity to the Mississippi River mouth as the primary source for terrigenous particles, and extent and duration of summertime water column hypoxia. The vertical distribution of 239,240Pu and 210Pbxs (= 210Pbtotal - 226Ra) provided reliable geochronological age constraints to develop models for mass accumulation rates and historic trace element inputs and variations. Mass accumulation rates ranged from 0.27 to 0.87 g cm-2 yr-1 and were internally consistent using either 210Pbxs or 239,240Pu. Measured inventories of 137Cs, 239,240Pu, and 210Pbxs were compared to atmospheric deposition rates to quantify potential sediment focusing or winnowing. Observed variability in calculated mass accumulation rates may be attributed foremost to site-specific proximity to the river mouth (i.e., sediment source), variability in water depth, and enhanced sediment focusing at the Mississippi River canyon site. Trace element concentrations were first normalized to Al, and then Al-normalized enrichment factors (ANEF) were calculated based on preanthropogenic and crustal trace element abundances. These ANEFs were typically > 1 for V and Ba, while for most other elements studied, either no enrichment or depletion was observed. The enrichment of Ba may be related, in part, to the seasonal occurrence of oxygen-depleted subsurface waters off the Mississippi River delta, as well as being an ubiquitous by-product of the petroleum industry. ?? 2006 Estuarine Research Federation.

  19. 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.

  20. 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.

  1. 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

  2. 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.

  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. Radionuclide concentrations in honey bees from Area G at TA-54 during 1997. Progress report

    SciTech Connect

    Haarmann, T.K.; Fresquez, P.R.

    1998-07-01

    Honey bees were collected from two colonies located at Los Alamos National Laboratory`s Area G, Technical Area 54, and from one control (background) colony located near Jamez Springs, NM. Samples were analyzed for the following: cesium ({sup 137}Cs), americium ({sup 241}Am), plutonium ({sup 238}Pu and {sup 239,240}Pu), tritium ({sup 3}H), total uranium, and gross gamma activity. Area G sample results from both colonies were higher than the upper (95%) level background concentration for {sup 238}Pu and {sup 3}H.

  5. Report of scouting study on precipitation of strontium, plutonium, and americium from Hanford complexant concentrate waste

    SciTech Connect

    Herting, D.L.

    1995-09-05

    A laboratory scouting test was conducted of precipitation methods for reducing the solubility of radionuclides in complexant concentrate (CC) waste solution. The results show that addition of strontium nitrate solution is effective in reducing the liquid phase activity of 90Sr (Strontium) in CC waste from tank 107-AN by 94% when the total strontium concentration is adjusted to 0.1 M. Addition of ferric nitrate solution effective in reducing the 241Am (Americium) activity in CC waste by 96% under the conditions described in the report. Ferric nitrate was also marginally effective in reducing the solubility of 239/240Pu (Plutonium) in CC waste

  6. Alternating-parity collective states of yrast and nonyrast bands in lanthanide and actinide nuclei

    SciTech Connect

    Nadirbekov, M. S. Yuldasheva, G. A.; Denisov, V. Yu.

    2015-03-15

    Excited collective states of even-even nuclei featuring quadrupole and octupole deformations are studied within a nonadiabatic collective model with a Gaussian potential energy. Rotational states of the yrast band and vibrational-rotational states of nonyrast bands are considered in detail. The energies of alternating-parity excited states of the yrast band in the {sup 164}Er, {sup 220}Ra, and {sup 224}Th nuclei; the yrast and first nonyrast bands in the {sup 154}Sm and {sup 160}Gd nuclei; and the yrast, first nonyrast, and second nonyrast bands in the {sup 224}Ra and {sup 240}Pu nuclei are described well on the basis of the proposed model.

  7. Effect of carbonate soil on transport and dose estimates from long-lived radionuclides at U. S. Pacific Test Site

    SciTech Connect

    Conrado, C.L.; Hamilton, T.F.; Robison, W.L.; Stoker, A.C.

    1998-09-01

    The United States conducted a series of nuclear tests from 1946 to 1958 at Bikini, a coral atoll, in the Marshall Islands (MI). The aquatic and terrestrial environments of the atoll are still contaminated with several long-lived radionuclides that were generated during testing. The four major radionuclides found in terrestrial plants and soils are Cesium-137 ({sup 137} Cs), Strontium-90 ({sup 90} Sr), Plutonium-239+ 240 ({sup 239+240}Pu) and Americium-241 ({sup 241}Am). {sup 137}Cs in the coral soils is more available for uptake by plants than {sup 137}Cs associated with continental soils of North America or Europe. Soil-to-plant {sup 137}Cs median concentration ratios (CR) (kBq kg{sup {minus}1} dry weight plant/kBq kg {sup {minus}1} dry weight soil) for tropical fruits and vegetables range between 0.8 and 36, much larger than the range of 0.005 to 0.5 reported for vegetation in temperate zones. Conversely, {sup 90}Sr median CRs range from 0.006 to 1.0 at the atoll versus a range from 0.02 to 3.0 for continental silica-based soils. Thus, the relative uptake of {sup 137}Cs and {sup 90}Sr by plants in carbonate soils is reversed from that observed in silica-based soils. The CRs for {sup 239+240}Pu and {sup 241}Am are very similar to those observed in continental soils. Values range from 10{sup {minus}6} to 10{sup {minus}4} for both {sup 239+240}Pu and {sup 241}Am. No significant difference is observed between the two in coral soil. The uptake of {sup 137}Cs by plants is enhanced because of the absence of mineral binding sites and the low concentration of potassium in the coral soil. {sup 137}Cs is bound to the organic fraction of the soil, whereas {sup 90}Sr, {sup 239+240}Pu and {sup 241}Am are primarily bound to soil particles. Assessment of plant uptake for {sup 137}Cs and {sup 90}Sr into locally grown food crops was a major contributing factor in (1) reliably predicting the radiological dose for returning residents, and (2) developing a strategy to limit the

  8. Plants as bio-monitors for Cs-137, Pu-238, Pu-239,240 and K-40 at the Savannah River Site.

    PubMed

    Caldwell, Eric Frank; Duff, Martine C; Ferguson, Caitlin E; Coughlin, Daniel P

    2011-05-01

    The Savannah River Site was constructed in South Carolina to produce plutonium (Pu) in the 1950s. Discharges associated with these now-ceased operations have contaminated large areas within the site, particularly streams associated with reactor cooling basins. Evaluating the exposure risk of contamination to an ecosystem requires methodologies that can assess the bioavailability of contaminants. Plants, as primary producers, represent an important mode of transfer of contaminants from soils and sediments into the food chain. The objective of this study was to identify local area plants for their ability to act as bio-monitors of radionuclides. The concentrations of cesium-137 ((137)Cs), potassium-40 ((40)K), (238)Pu and (239,240)Pu in plants and their associated soils were determined using γ and α spectrometry. The ratio of contamination concentration found in the plant relative to the soil was calculated to assess a concentration ratio (CR). The highest CR for (137)Cs was found in Pinus palustris needles (CR of 2.18). The correlation of soil and plant (137)Cs concentration was strong (0.76) and the R(2) (0.58) from the regression was significant (p = 0.006). This suggests the ability to predict the degree of (137)Cs contamination of a soil through analysis of the pine needles. The (238)Pu and (239,240)Pu concentrations were most elevated within the plant roots. Extremely high CR values were found in Sparganium americanum (bur-reed) roots with a value of 5.86 for (238)Pu and 5.66 for (239,240)Pu. The concentration of (40)K was measured as a known congener of (137)C. Comparing (40)K and (137)C concentrations in each plant revealed an inverse relationship for these radioisotopes. Correlating (40)K and (137)Cs was most effective in identifying plants that have a high affinity for (137)Cs uptake. The P. palustris and S. americanum proved to be particularly strong accumulators of all K congeners from the soil. Some species that were measured, warrant further

  9. Transfer of aged Pu to cattle grazing on a contaminated environment

    SciTech Connect

    Gilbert, R.O.; Engel, D.W.; Smith, D.D.; Shinn, J.H.; Anspaugh, L.R.; Eisele, G.R.

    1988-03-01

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

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

    PubMed

    Qiao, Jixin; Hou, Xiaolin

    2010-03-01

    Fractionation of plutonium isotopes ((238)Pu, (239,240)Pu) in environmental samples (i.e. soil and sediment) and bio-shielding concrete from decommissioning of nuclear reactor were carried out by dynamic sequential extraction using an on-line sequential injection (SI) system combined with a specially designed extraction column. Plutonium in the fractions from the sequential extraction was separated by ion exchange chromatography and measured using alpha spectrometry. The analytical results show a higher mobility of plutonium in bio-shielding concrete, which means attention should be paid to the treatment and disposal of nuclear waste from decommissioning. PMID:20004047

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

  12. [Migration in soil and accumulation in plants of peaceful nuclear explosion products in Perm region].

    PubMed

    Raskosha, N G; Shuktova, I I

    2015-01-01

    The data on the migration capacity in soil and accumulation of 238Pu, 239, 240Pu, 137Cs and 90Sr by plants in the area of a peaceful nuclear explosion located in the taiga zone are presented. The influence of the soil parameters on the distribution and transformation forms of the radionuclides in the podzolic soil profile was studied. The major amounts of man-made radionuclides were found in the matter of the ground lip. The accumulation parameters of pollutants by plants were the highest for the leaves, young branches and conifer of trees. PMID:25962279

  13. Accumulation of artificial radionuclides in agricultural plants in the area used for surface nuclear tests.

    PubMed

    Kozhakhanov, T E; Lukashenko, S N; Larionova, N V

    2014-11-01

    The paper reports on the study of artificial radionuclide accumulation in agricultural crops grown at the territory with high concentration of radionuclides, and first of all - with high concentration of transuranium elements. As a result of this work, peculiarities of accumulation and distribution of artificial radionuclides in the vegetative and generative organs of the studied plants have been revealed. Basic accumulation factors have been found for (137)Cs, (90)Sr, (239+240)Pu, and (241)Am in agricultural products. Accumulation factor dependence on type of planting was found for the investigated types of plants. It has been found that the vegetative organs accumulate radionuclides most of all.

  14. Plants as bio-monitors for Cs-137, Pu-238, Pu-239,240 and K-40 at the Savannah River Site.

    PubMed

    Caldwell, Eric Frank; Duff, Martine C; Ferguson, Caitlin E; Coughlin, Daniel P

    2011-05-01

    The Savannah River Site was constructed in South Carolina to produce plutonium (Pu) in the 1950s. Discharges associated with these now-ceased operations have contaminated large areas within the site, particularly streams associated with reactor cooling basins. Evaluating the exposure risk of contamination to an ecosystem requires methodologies that can assess the bioavailability of contaminants. Plants, as primary producers, represent an important mode of transfer of contaminants from soils and sediments into the food chain. The objective of this study was to identify local area plants for their ability to act as bio-monitors of radionuclides. The concentrations of cesium-137 ((137)Cs), potassium-40 ((40)K), (238)Pu and (239,240)Pu in plants and their associated soils were determined using γ and α spectrometry. The ratio of contamination concentration found in the plant relative to the soil was calculated to assess a concentration ratio (CR). The highest CR for (137)Cs was found in Pinus palustris needles (CR of 2.18). The correlation of soil and plant (137)Cs concentration was strong (0.76) and the R(2) (0.58) from the regression was significant (p = 0.006). This suggests the ability to predict the degree of (137)Cs contamination of a soil through analysis of the pine needles. The (238)Pu and (239,240)Pu concentrations were most elevated within the plant roots. Extremely high CR values were found in Sparganium americanum (bur-reed) roots with a value of 5.86 for (238)Pu and 5.66 for (239,240)Pu. The concentration of (40)K was measured as a known congener of (137)C. Comparing (40)K and (137)C concentrations in each plant revealed an inverse relationship for these radioisotopes. Correlating (40)K and (137)Cs was most effective in identifying plants that have a high affinity for (137)Cs uptake. The P. palustris and S. americanum proved to be particularly strong accumulators of all K congeners from the soil. Some species that were measured, warrant further

  15. 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.

  16. Radioactivity In Marine Organisms From Northeast Atlantic Ocean

    SciTech Connect

    Carvalho, Fernando P.; Oliveira, Joao M.

    2008-08-07

    Naturally-occurring radionuclides such as {sup 238}U, {sup 234}U, {sup 230}Th, {sup 226}Ra, {sup 210}Po, {sup 210}Pb and {sup 232}Th, and artificial radionuclides such as {sup 137}Cs, {sup 239+240}Pu and {sup 241}Am, were measured in a large number of marine species. In common fish species, typical concentrations of {sup 210}Po ranged from 10{sup 2} to 10{sup 4} mBq kg{sup -1} (wet weight), {sup 226}Ra concentrations ranged from 1x10{sup 2} to 5xl0{sup 2} mBq kg{sup -1}, {sup 238}U was at about 10 mBq kg{sup -1} and {sup 232}Th at about 0.5 mBq kg{sup -1}. Radiation doses to marine organisms originated by naturally-occurring and artificial radionuclides accumulated in tissues and by external radiation sources were computed and compared. Internal sources generally give higher contribution to the absorbed radiation dose than external sources. Amongst radionuclides accumulated in fish muscle and acting as internal radiation sources, natural {sup 210}Po and {sup 40}K give the largest contribution to the absorbed radiation dose, while artificial radionuclides such as {sup 137}Cs and {sup 239+240}Pu contribute with less than 0.5% to the absorbed radiation dose from all internal sources.

  17. Attempted validation of ICRP 30 and ICRP 66 respiratory models.

    PubMed

    Harley, N H; Fisenne, I M; Robbins, E S

    2012-11-01

    The validation of human biological models for inhaled radionuclides is nearly impossible. Requirements for validation are: (1) the measurement of the relevant human tissue data and (2) valid exposure measurements over the interval known to apply to tissue uptake. Two lung models, ICRP 30(1) and ICRP 66(2), are widely used to estimate lung doses following acute occupational or environmental exposure. Both ICRP 30 and 66 lung models are structured to estimate acute rather than chronic exposure. Two sets of human tissue measurements are available: (210)Po accumulated in tissue from inhaled cigarettes and ingested in diet and airborne global fallout (239,240)Pu accumulated in the lungs from inhalation. The human tissue measurements include pulmonary and bronchial tissue in smokers, ex-smokers and non-smokers analysed radiochemically for (210)Po, and pulmonary, bronchial and lymph nodes analysed for (239,240)Pu in lung tissue collected by the New York City Medical Examiner from 1972 to 1974. Both ICRP 30 and 66 models were included in a programme to accommodate chronic uptake. Neither lung model accurately described the estimated tissue concentrations but was within a factor of 2 from measurements. ICRP 66 was the exception and consistently overestimated the bronchial concentrations probably because of its assumption of an overly long 23-d clearance half-time in the bronchi and bronchioles. PMID:22923255

  18. 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.

  19. Radiological situation in the vicinity of Semipalatinsk nuclear test site: Dolon, Mostik, Cheremushka and Budene settlements.

    PubMed

    Sakaguchi, Aya; Yamamoto, Masayoshi; Hoshi, Masaharu; Imanaka, Tetsuji; Apsalikov, Kazbek N; Gusev, Boris I

    2006-02-01

    The present situation of radioactive contamination at the village of Dolon and nearby villages such as Mostik, Cheremushka and Budene was investigated to serve as an aid to resolve dose discrepancy between model calculations and TL measurements made for external gamma-ray dose in air in Dolon. The paper was focused on the reevaluation of the accumulated levels and distribution of long-lived radionuclides 137Cs and Pu isotopes in soil using long core samples up to a depth of 30 and 100 cm. The inventories of 137Cs and 239,240Pu found were in the wide range of 140-10,310 and 140-14,320 Bq/m2, respectively. Most of the Pu in soil was tightly incorporated into various sizes of fused particles. Both 137Cs and 239,240Pu in soil were accumulated in the smaller soil size fraction of <125 microm, and the presence of hot particles, probably due to Pu, was clearly observed by star-like patterns from alpha-tracks. The obtained data will be helpful for evaluating the current and future radiation risks to the people living around there.

  20. Contemporary radioecological state of the North-western Black Sea and the problems of environment conservation.

    PubMed

    Tereshchenko, N N; Mirzoyeva, N Yu; Gulin, S B; Milchakova, N A

    2014-04-15

    Review is devoted to the analysis of a radioecological situation in the North-western Black Sea and concerns the levels of contamination of the components of an ecosystem by the main artificial radioactive isotopes ((90)Sr, (137)Cs, (239,240)Pu). The long-term accumulation trends of these radionuclides were analyzed in components of the Black Sea ecosystem after the Chernobyl nuclear power plant accident. Zones that have an increased ability to accumulate these radioisotopes were revealed. The assessment of irradiation dose rates formed by (90)Sr, (137)Cs and (239,240)Pu in Black Sea hydrobionts was obtained. The strategy for biodiversity conservation and sustainable management of natural resources should include monitoring of the radioecological state of the marine ecosystems, and the formation of a complex of biogeochemical criteria for assessment of an ecological situation in the sea. This approach is important for marine protected areas, since it allows the formation of a basis for scientific and practical function. PMID:24461697

  1. Radionuclide Concentration in Soils and Vegetation at Low-Level Radioactive Waste Disposal Area G during 2005

    SciTech Connect

    P.R. Fresquez; M.W. McNaughton; M.J. Winch

    2005-10-01

    Soil samples were collected at 15 locations and unwashed overstory and understory vegetation samples were collected from up to nine locations within and around the perimeter of Area G, the primary disposal facility for low-level radioactive solid waste at Los Alamos National Laboratory (LANL). Soil and plant samples were also collected from the proposed expansion area west of Area G for the purpose of gaining preoperational baseline data. Soil and plant samples were analyzed for radionuclides that have shown a history of detection in past years; these included {sup 3}H, {sup 238}Pu, {sup 239,240}Pu, {sup 241}Am, {sup 234}U, {sup 235}U, and {sup 238}U for soils and {sup 3}H, {sup 238}Pu, and {sup 239,240}Pu for plants. As in previous years, the highest levels of {sup 3}H in soils and vegetation were detected at the south portion of Area G near the {sup 3}H shafts; whereas, the highest concentrations of the Pu isotopes were detected in the northern and northeastern portions near the pads for transuranic waste. All concentrations of radionuclides in soils and vegetation, however, were still very low (pCi range) and far below LANL screening levels and regulatory standards.

  2. 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

  3. 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)

  4. Radioactive Contamination of the North-western Black Sea Sediments

    NASA Astrophysics Data System (ADS)

    Gulin, S. B.; Polikarpov, G. G.; Egorov, V. N.; Martin, J. M.; Korotkov, A. A.; Stokozov, N. A.

    2002-03-01

    The paper deals with the input and deposition of the man-made radionuclides 137Cs, 238 Pu, 239+240Pu and 241Am introduced to the north-western Black Sea, over the last few decades, as the result of atmospheric nuclear weapons testing and the Chernobyl nuclear accident. One approach taken was to retrieve the deposition records of these radionuclides in the sediments. The deposition chronology was compared with monitoring data of the post-Chernobyl input of 137Cs to the NW Black Sea sediments from the Danube River. The partitioning of 137 Cs between suspended matter and water was traced along the salinity gradient in the Danube mixing zone. In sediments deposited in the vicinity of the Danube delta and the Dniepr estuary, the activity of Chernobyl 137Cs had reached its maximum 5 and 10 years after the accident, respectively. The activity ratio of 137Cs to 239+240Pu and 241 Am revealed a higher mobility of 137Cs in the Danube River basin compared to plutonium and americium. The percentage of particulate 137Cs and its distribution coefficient vs salinity have allowed the estimation of sedimentary scavenging and desorption of caesium in the Danube mixing zone. Comparison of the post-Chernobyl 137Cs input from the Danube to the 137Cs inventory in the adjacent Black Sea sediments showed that more than 70% of this radionuclide was deposited in the Danube-Black Sea mixing zone.

  5. 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.

  6. Plutonium concentrations in lichens of Rocky Flats environs

    SciTech Connect

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

    1995-03-01

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

  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. Trench ‘Bathtubbing’ and Surface Plutonium Contamination at a Legacy Radioactive Waste Site

    PubMed Central

    2013-01-01

    Radioactive waste containing a few grams of plutonium (Pu) was disposed between 1960 and 1968 in trenches at the Little Forest Burial Ground (LFBG), near Sydney, Australia. A water sampling point installed in a former trench has enabled the radionuclide content of trench water and the response of the water level to rainfall to be studied. The trench water contains readily measurable Pu activity (∼12 Bq/L of 239+240Pu in 0.45 μm-filtered water), and there is an associated contamination of Pu in surface soils. The highest 239+240Pu soil activity was 829 Bq/kg in a shallow sample (0–1 cm depth) near the trench sampling point. Away from the trenches, the elevated concentrations of Pu in surface soils extend for tens of meters down-slope. The broader contamination may be partly attributable to dispersion events in the first decade after disposal, after which a layer of soil was added above the trenched area. Since this time, further Pu contamination has occurred near the trench-sampler within this added layer. The water level in the trench-sampler responds quickly to rainfall and intermittently reaches the surface, hence the Pu dispersion is attributed to saturation and overflow of the trenches during extreme rainfall events, referred to as the ‘bathtub’ effect. PMID:24256473

  10. Transfer of natural and anthropogenic radionuclides to ants, bryophytes and lichen in a semi-natural ecosystem.

    PubMed

    Dragović, Snezana; Howard, Brenda J; Caborn, Jane A; Barnett, Catherine L; Mihailović, Nevena

    2010-07-01

    Few data are available to quantify the transfer of both natural and anthropogenic radionuclides to detritivorous invertebrates to facilitate estimation of the internal dose to such biota in models used to assess radiation exposure. To enhance the available data, activity concentrations of (137)Cs, (40)K, (90)Sr, (239 + 240)Pu, (241)Am, (235)U and (238)U were measured in ants (Formicidae) and corresponding undisturbed soil collected from the Zlatibor mountain in Serbia and ant/soil concentration ratios (CR) calculated. The (241)Am concentration ratios for ants were fourfold higher than those calculated for ants in a previous study whereas they are similar to the more numerous data previously reported for a range of detritivorous invertebrates in other studies. CR values for (137)Cs in ants were similar to the few other reported values and slightly lower than those for a range of detritivorous invertebrates. Those for (239 + 240)Pu were slightly higher than those for ants in two other studies but they were close to upper limit of a range of data reported for detritivorous invertebrates. All the CR values will be included in a future revision of the ERICA Tool database and will particularly improve the information available for uranium.

  11. Actinide measurements by AMS using fluoride matrices

    NASA Astrophysics Data System (ADS)

    Cornett, R. J.; Kazi, Z. H.; Zhao, X.-L.; Chartrand, M. G.; Charles, R. J.; Kieser, W. E.

    2015-10-01

    Actinides can be measured by alpha spectroscopy (AS), mass spectroscopy or accelerator mass spectrometry (AMS). We tested a simple method to separate Pu and Am isotopes from the sample matrix using a single extraction chromatography column. The actinides in the column eluent were then measured by AS or AMS using a fluoride target matrix. Pu and Am were coprecipitated with NdF3. The strongest AMS beams of Pu and Am were produced when there was a large excess of fluoride donor atoms in the target and the NdF3 precipitates were diluted about 6-8 fold with PbF2. The measured concentrations of 239,240Pu and 241Am agreed with the concentrations in standards of known activity and with two IAEA certified reference materials. Measurements of 239,240Pu and 241Am made at A.E. Lalonde AMS Laboratory agree, within their statistical uncertainty, with independent measurements made using the IsoTrace AMS system. This work demonstrated that fluoride targets can produce reliable beams of actinide anions and that the measurement of actinides using fluorides agree with published values in certified reference materials.

  12. Plutonium concentrations in lichens of Rocky Flats environs.

    PubMed

    Thomas, R S; Ibrahim, S A

    1995-03-01

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

  13. 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.

  14. Radionuclide bioconcentration factors and sediment partition coefficients in Arctic Seas subject to contamination from dumped nuclear wastes

    SciTech Connect

    Fisher, N.S. . Marine Sciences Research Center); Fowler, S.W.; Boisson, F.; Carroll, J. . Marine Environment Lab.); Rissanen, K. ); Salbu, B. . Lab. for Analytical Chemistry); Sazykina, T.G. ); Sjoeblom, K.L. )

    1999-06-15

    The disposal of large quantities of radioactive wastes in Arctic Seas by the former Soviet Union has prompted interest in the behavior of long-lived radionuclides in polar waters. Previous studies on the interactions of radionuclides prominent in radioactive wastes have focused on temperate waters; the extent to which the bioconcentration factors and sediment partitioning from these earlier studies could be applied to risk assessment analyses involving high latitude systems is unknown. Here the authors present concentrations in seawater and calculated in situ bioconcentration factors for [sup 90]Sr, [sup 137]Cs, and [sup 239+240]Pu (the three most important radionuclides in Arctic risk assessment models) in macroalgae, crustaceans, bivalve molluscs, sea birds, and marine mammals as well as sediment K[sub d] values for 13 radionuclides and other elements in samples taken from the Kara and Barents Seas. The data analysis shows that, typically, values for polar and temperate waters are comparable, but exceptions include 10-fold higher concentration factors for [sup 239+240]Pu in Arctic brown macroalgae, 10-fold lower K[sub d] values for [sup 90]Sr in Kara Sea sediment than in typical temperate coastal sediment, and 100-fold greater Ru K[sub d] values in Kara Sea sediment. For most elements application of temperate water bioconcentration factors and K[sub d] values to Arctic marine systems appears to be valid.

  15. Nevada Test Site Radionuclide Inventory and Distribution Program: Report No. 3, Areas 3, 7, 8, 9, and 10

    SciTech Connect

    McArthur, R D; Mead, S W

    1987-02-01

    As part of the Nevada Test Site Radionuclide Inventory and Distribution Program, 115 soil samples were collected and more than 1200 in situ measurements of gamma-emitting radionuclides were made in the northern and eastern parts of Yucca Flat. Analysis of the data led to estimated inventories of 215 Ci of /sup 239,240/Pu, 128 Ci of /sup 137/Cs, 92 Ci of /sup 90/Sr, 36 Ci each of /sup 241/Am and /sup 60/Co, 31 Ci of /sup 102m/Rh, 27 Ci of /sup 238/Pu, 25 Ci of /sup 174/Lu, 10 Ci of /sup 152/Eu, 8 Ci of /sup 155/Eu, 7 Ci of /sup 154/Eu, 5 Ci of /sup 125/Sb, 4 Ci of /sup 101/Rh, and 2 Ci of /sup 134/Cs in the surface soil of the accessible portion of Areas 8 and 10. Similar calculations with the data from Areas 3, 7, and 9 gave estimates of 145 Ci of /sup 239,240/Pu, 89 Ci of /sup 152/Eu, 62 Ci of /sup 90/Sr, 25 Ci of /sup 137/Cs, 14 Ci of /sup 154/Eu, 11 Ci of /sup 241/Am, 6 Ci each of /sup 60/Co and /sup 238/Pu, and 4 Ci of /sup 155/Eu. Additional in situ measurements at 30 locations in the southern part of Yucca Flat confirmed the low levels of radioactivity found there by an aerial survey. 1 ref., 57 figs., 10 tabs.

  16. Energy Dependent Bias in the Weighted Point Model.

    SciTech Connect

    Santi, P. A.; Geist, W. H.

    2005-01-01

    While the weighted point multiplicity model has successfully reduced the bias that is associated with variable multiplication of neutrons within a sample (which was assumed constant in the standard point multiplicity model), other potential sources of bias still exists within the weighted point model. One significant source of bias arises from the assumption that the energies of the neutrons from ({alpha},n) reactions on impurities in the sample have the same average energy as neutrons emitted from the spontaneous fission of {sup 240}Pu. An investigation into the effects that neutron energy has on the assay results (effective {sup 240}Pu mass, alpha, and multiplication) of the weighted point multiplicity model has been performed using MCNPX, Version 2.5f for impure plutonium metal samples in a number of different detector systems. The effects of energy dependence of the detection efficiency and gate fractions on the assay results, as well as the measured singles, doubles, and triples rates were also studied. Methods for mitigating the effects of neutron energy on the weighted-point multiplicity model results will be presented and discussed.

  17. Contemporary radioecological state of the North-western Black Sea and the problems of environment conservation.

    PubMed

    Tereshchenko, N N; Mirzoyeva, N Yu; Gulin, S B; Milchakova, N A

    2014-04-15

    Review is devoted to the analysis of a radioecological situation in the North-western Black Sea and concerns the levels of contamination of the components of an ecosystem by the main artificial radioactive isotopes ((90)Sr, (137)Cs, (239,240)Pu). The long-term accumulation trends of these radionuclides were analyzed in components of the Black Sea ecosystem after the Chernobyl nuclear power plant accident. Zones that have an increased ability to accumulate these radioisotopes were revealed. The assessment of irradiation dose rates formed by (90)Sr, (137)Cs and (239,240)Pu in Black Sea hydrobionts was obtained. The strategy for biodiversity conservation and sustainable management of natural resources should include monitoring of the radioecological state of the marine ecosystems, and the formation of a complex of biogeochemical criteria for assessment of an ecological situation in the sea. This approach is important for marine protected areas, since it allows the formation of a basis for scientific and practical function.

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

    PubMed

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

    2015-05-01

    Spatial distribution of activity concentrations of (137)Cs, (90)Sr, and (239,240)Pu in the top layer of undisturbed meadow soils was compared between two regional transects across Lithuania: one in the SW region, more affected by the Chernobyl radioactive fallout, and the other in the NE region. Radiochemical, γ-, α-, β-, and mass spectrometric methods were used to determine the radionuclide activity. Our results validate that higher activity concentrations in the top soil layer were present in the SW region, despite the fact that sampling was performed after 22 years of the Chernobyl Nuclear Power Plant (NPP) accident. Using the activity concentration ratio (137)Cs/(239,240)Puglobal, the contribution of the Chernobyl NPP accident to the total radiocesium activity concentrations in these meadow soils was evaluated and found to be in the range of 6.5-59.1%. Meanwhile, the activity concentration ratio (238)Pu/(239,240)Pu showed that Chernobyl-derived Pu occurred at almost half of the sampling sites. The locations with maximal values of 47% of Chernobyl-derived Pu material were close to northeastern Poland, where deposition of most of non-volatile radioisotopes from the Chernobyl plume was determined. PMID:25893760

  19. Radionuclide concentrations in vegetation at a solid radioactive waste-disposal area in southeastern Idaho

    SciTech Connect

    Arthur, W.J. III

    1982-07-01

    Concentrations of /sup 238/Pu, /sup 239,240/Pu, and /sup 241/Am in crested wheatgrass (Agropyron cristatum (L.) Gaertn) and Russian thistle (Salsola kali L.) samples collected at a solid radioactive waste-disposal area in southeastern Idaho were significantly (P less than or equal to 0.05) greater than concentrations in control vegetation. No significant differences were found for /sup 90/Sr or /sup 137/Cs concentrations between the waste-disposal and control-area vegetation. Russian thistle had more radionuclide contamination than crested wheatgrass, presumably because of its greater rooting depth and spreading growth. The total radionuclide inventory of /sup 90/Sr, /sup 137/Cs, /sup 238/Pu, /sup 239,240/Pu, and /sup 241/Am in vegetation at the 36-ha waste-disposal area (77 ..mu..Ci) was not significantly (P > 0.05) greater than the 17 ..mu..Ci in control-area vegetation. Ninety percent of the radioactivity in waste-disposal area vegetation and 99% in control-area vegetation were attributed to /sup 90/Sr and /sup 137/Cs. The Pu inventory in Subsurface Disposal Area (SDA) vegetation was only 0.02% of the quantity of Pu estimated to occur in SDA surface soils in 1974. Accumulation of radionuclides by vegetation is not considered a major mode of radionuclide transport through the environment surrounding this radioactive-waste-disposal area.

  20. 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.

  1. Twenty-four years of follow-up for a Hanford plutonium wound case.

    PubMed

    Carbaugh, Eugene H; Lynch, Timothy P; Antonio, Cheryl L; Medina-Del Valle, Fernando

    2010-10-01

    A 1985 plutonium puncture wound resulted in the initial deposition of 48 kBq of transuranic alpha activity, primarily 239+240Pu and 241Am, in a worker's right index finger. Surgical excisions in the week following reduced the long-term residual wound activity to 5.4 kBq, and 164 DTPA chelation therapy administrations over 17 mo resulted in urinary excretion of about 7 kBq. The case was published in 1988, but now 24 y of follow-up data are available. Annual bioassays have included in-vivo measurements of 241Am in the wound, skeleton, liver, lung, and axillary lymph nodes, and urinalyses for plutonium and 241Am. These measurements have shown relatively stable levels of 241Am at the wound site, with gradually increasing amounts of 241Am detected in the skeleton. Liver measurements have shown erratic detection of 241Am, and the lung measurements indicate Am but as interference from activity in the axillary lymph nodes and skeleton rather than activity in the lung. Urine excretion of Pu since termination of chelation therapy has typically ranged from 10 to 20 mBq d, with Am excretion about 10% of that for 239+240Pu. Annual routine medical exams have not identified any adverse health effects associated with the intake.

  2. 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.

  3. 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.

  4. Trench 'bathtubbing' and surface plutonium contamination at a legacy radioactive waste site.

    PubMed

    Payne, Timothy E; Harrison, Jennifer J; Hughes, Catherine E; Johansen, Mathew P; Thiruvoth, Sangeeth; Wilsher, Kerry L; Cendón, Dioni I; Hankin, Stuart I; Rowling, Brett; Zawadzki, Atun

    2013-01-01

    Radioactive waste containing a few grams of plutonium (Pu) was disposed between 1960 and 1968 in trenches at the Little Forest Burial Ground (LFBG), near Sydney, Australia. A water sampling point installed in a former trench has enabled the radionuclide content of trench water and the response of the water level to rainfall to be studied. The trench water contains readily measurable Pu activity (~12 Bq/L of (239+240)Pu in 0.45 μm-filtered water), and there is an associated contamination of Pu in surface soils. The highest (239+240)Pu soil activity was 829 Bq/kg in a shallow sample (0-1 cm depth) near the trench sampling point. Away from the trenches, the elevated concentrations of Pu in surface soils extend for tens of meters down-slope. The broader contamination may be partly attributable to dispersion events in the first decade after disposal, after which a layer of soil was added above the trenched area. Since this time, further Pu contamination has occurred near the trench-sampler within this added layer. The water level in the trench-sampler responds quickly to rainfall and intermittently reaches the surface, hence the Pu dispersion is attributed to saturation and overflow of the trenches during extreme rainfall events, referred to as the 'bathtub' effect.

  5. 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.

  6. Plutonium concentrations in lichens of Rocky Flats environs.

    PubMed

    Thomas, R S; Ibrahim, S A

    1995-03-01

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

  7. Fission cross section measurements of actinides at LANSCE

    SciTech Connect

    Tovesson, Fredrik; Laptev, Alexander B; Hill, Tony S

    2010-01-01

    Fission cross sections of a range of actinides have been measured at the Los Alamos Neutron Science Center (LANSCE) in support of nuclear energy applications. By combining measurement at two LANSCE facilities, Lujan Center and the Weapons Neutron Research center (WNR), differential cross sections can be measured from sub-thermal energies up to 200 MeV. Incident neutron energies are determined using the time-of-flight method, and parallel-plate ionization chambers are used to measure fission cross sections relative to the {sup 235}U standard. Recent measurements include the {sup 233,238}U, {sup 239,242}Pu and {sup 243}Am neutron-induced fission cross sections. In this paper preliminary results for cross section data of {sup 243}Am and {sup 233}U will be presented.

  8. The Minor Actinide Transmutation-Incineration Potential Studies in High Intensity Neutron Fluxes

    SciTech Connect

    Letourneau, A.; Chabod, S.; Foucher, Y.; Marie, F.; Ridikas, D.; Veyssiere, Ch.; Blandin, Ch.

    2005-05-24

    In the framework of nuclear waste transmutation studies, the Mini-INCA project has been initiated at CEA/DSM with objectives to determine optimal conditions for transmutation and incineration of Minor Actinides (MA) in high intensity neutron fluxes. Our experimental tools based on alpha- and gamma-spectroscopy of irradiated samples and the development of fission micro-chambers could gather both microscopic information on nuclear reactions (total and partial cross sections for neutron capture and/or fission reactions) and macroscopic information on transmutation and incineration potentials. Cross sections of selected actinides (241Am, 242Am, 242Pu, 237Np, 238Np) have already been measured at ILL, showing some discrepancies when compared to evaluated data libraries but in overall good agreement with recent experimental data.

  9. Actinide targets for the synthesis of super-heavy elements

    DOE PAGES

    Roberto, J.; Alexander, Charles W.; Boll, Rose Ann; Ezold, Julie G.; Felker, Leslie Kevin; Rykaczewski, Krzysztof Piotr; Hogle, Susan L.

    2015-06-18

    Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of 48Ca beams on actinide targets. These target materials, including 242Pu, 244Pu, 243Am, 245Cm, 248Cm, 249Cf, and 249Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing themore » production of rare actinides including 249Bk, 251Cf, and 254Es are described.« less

  10. Actinide targets for the synthesis of super-heavy elements

    NASA Astrophysics Data System (ADS)

    Roberto, J. B.; Alexander, C. W.; Boll, R. A.; Burns, J. D.; Ezold, J. G.; Felker, L. K.; Hogle, S. L.; Rykaczewski, K. P.

    2015-12-01

    Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of 48Ca beams on actinide targets. These target materials, including 242Pu, 244Pu, 243Am, 245Cm, 248Cm, 249Cf, and 249Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing the production of rare actinides including 249Bk, 251Cf, and 254Es are described.

  11. Fission cross-sections, prompt fission neutron and γ-ray emission in request for nuclear applications

    NASA Astrophysics Data System (ADS)

    Hambsch, F.-J.; Salvador-Castiñeira, P.; Oberstedt, S.; Göök, A.; Billnert, R.

    2016-06-01

    In recent years JRC-IRMM has been investigating fission cross-sections of 240,242Pu in the fast-neutron energy range relevant for innovative reactor systems and requested in the High Priority Request List (HPRL) of the OECD/Nuclear Energy Agency (NEA). In addition to that, prompt neutron multiplicities are being investigated for the major isotopes 235U, 239Pu in the neutron-resonance region using a newly developed scintillation detector array (SCINTIA) and an innovative modification of the Frisch-grid ionisation chamber for fission-fragment detection. These data are highly relevant for improved neutron data evaluation and requested by the OECD/Working Party on Evaluation Cooperation (WPEC). Thirdly, also prompt fission γ-ray emission is investigated using highly efficient lanthanide-halide detectors with superior timing resolution. Again, those data are requested in the HPRL for major actinides to solve open questions on an under-prediction of decay heat in nuclear reactors. The information on prompt fission neutron and γ-ray emission is crucial for benchmarking nuclear models to study the de-excitation process of neutron-rich fission fragments. Information on γ-ray emission probabilities is also useful in decommissioning exercises on damaged nuclear power plants like Fukushima Daiichi to which JRC-IRMM is contributing. The results on the 240,242Pu fission cross section, 235U prompt neutron multiplicity in the resonance region and correlations with fission fragments and prompt γ-ray emission for several isotopes will be presented and put into perspective.

  12. Fission Fragment Yield, Cross Section and Prompt Neutron and Gamma Emission Data from Actinide Isotopes

    NASA Astrophysics Data System (ADS)

    Hambsch, F.-J.; Oberstedt, S.; Al-Adili, A.; Brys, T.; Billnert, R.; Matei, C.; Oberstedt, A.; Salvador-Castiñeira, P.; Tudora, A.; Vidali, M.

    2014-05-01

    Recent experimental investigations on major and minor actinides at the JRC-IRMM are presented. Fission-fragment distributions of isotopes with vibrational resonances in the sub-threshold fission cross section, i. e. 234,238U, have been measured. For 234U, the impact of an increased neutron multiplicity for the heavy fragments with higher incident neutron energies has been studied as observed in experiment and also recently theoretically predicted. The impact is found to be noticeable on post-neutron mass yields, which are the relevant quantities for a-priori waste assessments. The fission cross sections for 240,242Pu at threshold and in the plateau region are being investigated within the ANDES project. The results show some discrepancies to the ENDF/B-VII.1 evaluation mainly for 242Pu around 1 MeV, where the evaluation exhibits a resonance-like structure not observed so clearly in the present work. The requested target accuracy in design studies of innovative reactor concepts like Gen-IV is in the range of a few percent. In order to be able to respond to requests for measurements of prompt neutron and γ-ray emission in fission JRC-IRMM has also invested in setting up a neutron and γ-ray detector array. The neutron array is called SCINTIA and has so far been tested with 252Cf(SF). For γ-ray multiplicity and spectrum measurements of 252Cf(SF) and 235U(nth, f) lanthanum- and cerium-halide detectors were successfully used.

  13. 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.

  14. 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)

  15. 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.

  16. Prompt Fission γ-ray Spectra Characteristics - A First Summary

    NASA Astrophysics Data System (ADS)

    Oberstedt, S.; Billnert, R.; Gatera, A.; Geerts, W.; Halipré, P.; Hambsch, F.-J.; Lebois, M.; Oberstedt, A.; Marini, P.; Vidali, M.; Wilson, J. N.

    In this work we give an overview of our investigations of prompt γ-ray emission in nuclear fission. This work was conducted during the last five years in response to a high priority nuclear data request formulated by the OECD/NEA. The aim was to reveal data deficiencies responsible for a severe under-prediction of the prompt γ heating in nuclear reactor cores. We obtained new prompt fission γ-ray spectral (PFGS) data for 252Cf(SF) as well as for thermal-neutron induced fission on 235U(nth,f) and 241Pu(nth,f). In addition, first PFGS measurements with a fast-neutron beam were accomplished, too. The impact of the new data and future data needs are discussed.

  17. 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.

  18. Uptake and loss of plutonium from osteoclasts and macrophages in the mandibular condyle of the rat.

    PubMed

    Priest, N D; Giannola, S J

    1980-01-01

    Female rats were used to study the kinetics of plutonium transfer from the bone surfaces of the mandibular condyle to osteoclasts and macrophages. This study was made using autoradiographs prepared from plastic sections of the mineralized bones of animals which had been injected with 241 Pu citrate. Measurements of the concentration of plutonium in the osteoclasts and macrophages at different times after the injection of plutonium showed that plutonium was concentrated by osteoclasts from bone surfaces and was retained with a half-time of approximately 70 h. Subsequently, plutonium appeared to be transferred to macrophages. The results showed that plutonium was unlikely to be accumulated by macrophages as a result of their participation in bone resorption.

  19. 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.

  20. 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.

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

    PubMed

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

    2012-11-01

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

  2. Nuclear Data Sheets for A=241

    DOE PAGES

    Nesaraja, Caroline D.

    2015-11-27

    This paper presents available information pertaining to the nuclear structure of ground and excited states for all known nuclei with mass numbers A=24, which have been compiled and evaluated. The adopted level and decay schemes, as well as the detailed nuclear properties and configuration assignments based on experimental data are presented for these nuclides. When there are insufficient data, expected values from systematics of nuclear properties or/and theoretical calculations are quoted. Unexpected or discrepant experimental results are also noted. A summary and compilation of the discovery of various isotopes in this mass region is given in 2013Fr02 (241Np,241Pu, 241Am, 241Cm,more » 241Bk, and 241Cf), 2011Me01 (241Es), and 2013Th02 (241Fm).« less

  3. Effect of the electron decay of metallic fission products on the chemical and phase compositions of an uranium-plutonium fuel irradiated by fast neutrons

    NASA Astrophysics Data System (ADS)

    Bondarenko, G. G.; Bulatov, G. S.; Gedgovd, K. N.; Lyubimov, D. Yu.; Yakushkin, M. M.

    2011-11-01

    After fast-neutron irradiation, uranium-plutonium nitride U0.8Pu0.2N is shown to acquire a complex structure consisting of a solid solution that is based on the nitrides of uranium, plutonium, americium, neptunium, zirconium, yttrium, and lanthanides and contains condensed phases U2N3, CeRu2, BaTe, Ba3N2, CsI, Sr3N2, LaSe, metallic molybdenum, technetium, and U(Ru, Rh, Pd)3 intermetallics. The contents and compositions of these phases are calculated at a temperature of 900 K and a burn-up fraction up to 14% (U + Pu). The change in the composition of the irradiated uranium-plutonium nitride is studied during the electron decay of metallic radionuclides. The kinetics of transformation of U103Ru3, 137CsI, 140Ba3N2, and 241PuN is calculated.

  4. 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.

  5. 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.

  6. Method for Ultratrace Level (241)Am Determination in Large Soil Samples by Sector Field-Inductively Coupled Plasma Mass Spectrometry: With Emphasis on the Removal of Spectral Interferences and Matrix Effect.

    PubMed

    Wang, Zhongtang; Zheng, Jian; Cao, Liguo; Tagami, Keiko; Uchida, Shigeo

    2016-07-19

    A new method using sector field-inductively coupled plasma mass spectrometry (SF-ICPMS) was developed for the determination of (241)Am in large soil samples to provide realistic soil-plant transfer parameter data for dose assessment of nuclear waste disposal plans. We investigated four subjects: extraction behaviors of interfering elements (Bi, Tl, Hg, Pb, Hf, and Pt) on DGA resin (normal type, abbreviated as DGA-N); soil matrix element removal (Mg, Fe, Al, K, Na) using Fe(OH)3, CaF2, and CaC2O4 coprecipitations; Am and rare earth elements (REEs) separation on DGA-N and TEVA resins; and optimization of SF-ICPMS (equipped with a high efficiency nebulizer (HEN)) for Am determination. Our method utilized concentrated HNO3 to leach Am from 2 to 20 g soil samples. The CaC2O4 coprecipitation was used to remove major metals in soil and followed by Am/interfering elements separation using the proposed UTEVA + DGA-N procedure. After a further separation of REEs on TEVA resin, (241)Am was determined by HEN-SF-ICPMS. This method eliminated the matrix effect in ICPMS (241)Am measurement for large soil samples. The high decontamination factors (DFs) of interfering elements enable their thorough removal, and in particular, the DF of Pu (7 × 10(5)) was the highest ever reported in (241)Am studies; thus, this method is capable of analyzing (241)Pu-contaminated Fukushima Daiichi Nuclear Power Plant (FDNPP) sourced soil samples. A low detection limit of 0.012 mBq g(-1) for (241)Am was achieved. The chemical recovery of Am (76-82%) was stable for soil samples. This method can be employed for the low level (241)Am determination in large size soil samples that are contaminated with (241)Pu. PMID:27322003

  7. 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

    Under the auspices of the U.S. Department of Energy (USDOE), researchers from the Lawrence Livermore National Laboratory (LLNL) have recently implemented a series of initiatives to address long-term radiological surveillance needs at former nuclear test sites in the Republic of the Marshall Islands (RMI). The aim of this radiological surveillance monitoring program (RSMP) is to provide timely radiation protection for individuals in the Marshall Islands with respect to two of the most important internally deposited fallout radionuclides-cesium-137 ({sup 137}Cs) and long-lived isotopes 239 and 240 of plutonium ({sup 239+240}Pu) (Robison et al., 1997 and references therein). Therefore, whole-body counting for {sup 137}Cs and a sensitive bioassay for the presence of {sup 239+240}Pu excreted in urine were adopted as the two most applicable in vivo analytical methods to assess radiation doses for individuals in the RMI from internally deposited fallout radionuclides (see Hamilton et al., 2006a-c; Bell et al., 2002). Through 2005, the USDOE has established three permanent whole-body counting facilities in the Marshall Islands: the Enewetak Radiological Laboratory on Enewetak Atoll, the Utrok Whole-Body Counting Facility on Majuro Atoll, and the Rongelap Whole-Body Counting Facility on Rongelap Atoll. These whole-body counting facilities are operated and maintained by trained Marshallese technicians. Scientists from LLNL provide the technical support and training necessary for maintaining quality assurance for data acquisition and dose reporting. This technical basis document summarizes the methodologies used to calculate the annual total effective dose equivalent (TEDE; or dose for the calendar year of measurement) based on whole-body counting of internally deposited {sup 137}Cs and the measurement of {sup 239+240}Pu excreted in urine. Whole-body counting provides a direct measure of the total amount (or burden) of {sup 137}Cs present in the human body at the time of

  8. Americium, plutonium and uranium contamination and speciation in well waters, streams and atomic lakes in the Sarzhal region of the Semipalatinsk Nuclear Test Site, Kazakhstan.

    PubMed

    León Vintró, L; Mitchell, P I; Omarova, A; Burkitbayev, M; Jiménez Nápoles, H; Priest, N D

    2009-04-01

    New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel'kem 1 and Tel'kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that (241)Am, (239,240)Pu and (238)U concentrations in well waters within the study area are in the range 0.04-87mBq dm(-3), 0.7-99mBq dm(-3), and 74-213mBq dm(-3), respectively, and for (241)Am and (239,240)Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01mBq dm(-3), 0.08mBq dm(-3) and 0.32mBq dm(-3) for (241)Am, (239,240)Pu and (238)U, respectively. The (235)U/(238)U isotopic ratio in almost all well and stream waters is slightly elevated above the 'best estimate' value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53-85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11-42microSv (mean 21microSv). Presently, the ground water feeding these wells would not appear to be contaminated with

  9. Radionuclide concentrations in underground waters of Mururoa and Fangataufa Atolls.

    PubMed

    Mulsow, S; Coquery, M; Dovlete, C; Gastaud, J; Ikeuchi, Y; Pham, M K; Povinec, P P

    1999-09-30

    In 1997 an expedition to Mururoa and Fangataufa Atolls was carried out to sample underground waters from cavity-chimneys and carbonate monitoring wells. The aim of this study was to determine the prevailing concentration and distribution status of radionuclides. Elemental analysis of interstitial waters was carried out in the water fraction as well as in particles collected at 11 underground monitoring wells. 238Pu, 239,240Pu, 241Am, 137Cs, 90Sr, 3H, 125Sb, 155Eu and 60Co were analyzed in both fractions by alpha-, beta- and gamma-spectrometry. Measurements showed that at 60% of the sites, pH and Eh seemed to be related to tidal cycles; in contrast HTO was constant during the sampling time. Interstitial waters from carbonates and transition zones shared similar chemical composition that were not different from that of the surrounding seawater. Waters collected from basalt cavities left after nuclear tests, (Aristee and Ceto) have a different chemical signature characterized by a deficiency in Mg, K and SO4 as well as enrichment in Sr, Si, Al and Cl compared to the rest of the stations. Radionuclide concentrations present in both, water and particulate fractions, were significantly higher at Ceto and Aristee than at any other monitoring wells, except for Fuseau and Mitre monitoring wells (Fangataufa) where values similar to Ceto were found (e.g. 239,240Pu: > 20 mBq g-1). Considering that Pu isotopes showed high Kd values compared to non-sorbing radionuclides such as 3H, 90Sr and 137Cs it is very unlikely that migration from cavities to monitoring wells accounts for the concentration of Pu isotopes and Am at Fuseau 30 and Mitre 27. Perhaps the contact of lagoon waters with the well before sealing could be a possible source of the transuranics found at these sites. The 238Pu/239,240Pu ratios measured in the particles were similar to that of the lagoon (0.38), thus supporting this hypothesis. The fact that transuranics were found only in the particle fraction, in the

  10. Nuclear Data Sheets for A = 240

    SciTech Connect

    Singh, Balraj; Browne, E.

    2008-10-15

    Evaluated experimental data for radioactive decays and reactions for known nuclides (U, Np, Pu, Am, Cm, Bk, Cf) of A = 240 are presented together with adopted values for level energies, {gamma}-ray energies, relative branching ratios and other nuclear properties. This revision was primarily motivated by the need for re-evaluation of absolute gamma-ray intensities from the {epsilon} decay of {sup 240}Am to {sup 240}Pu. These quantities are essential for determining precise and accurate cross-sections for the {sup 241}Am(n,2n){sup 240}Am reaction using fast neutrons (see e.g. Americium Workshop, Santa Fe, New Mexico, September 2007, 2008To06, 2007Ta01, 2006Pe14) and {sup 241}Am({gamma},n) reaction (see e.g. 2006Ri08). For {sup 240}U, the {gamma}-ray data have now become available. The data sets for {sup 244}Pu {alpha} decay to {sup 240}U; {sup 244}Cm {alpha} decay to {sup 240}Pu and {sup 244}Cf {alpha} decay to {sup 240}Cm have been adapted from evaluations by 1998Ak04 and 2003Ak04. For {sup 244}Cm decay, evaluation by 2006BeZL under the Decay Data Evaluation Project (DDEP) is also used. The {gamma}-ray data (energies and intensities) for {sup 240}Cm decay are not considered (by the evaluators) as well established. Most detailed data are available only for {sup 240}Pu. Extensive data in the second potential well are available for this nuclide together with fission isomers and several superdeformed (SD) structures. For other nuclides spectroscopic data are rather sparse in the literature; especially for the following radioactive decays: The {epsilon} decays of {sup 240}Cf, {sup 240}Bk and {sup 240}Cm; multipolarities of {gamma}-ray transitions in {sup 240}Np from {sup 240}U {beta}{sup -} decay; {gamma}-ray transitions from {sup 244}Cf {alpha} decay and %{epsilon} branch of {sup 244}Cf decay; spins and parities of excited states in {sup 240}U and multipolarities of associated {gamma}-ray transitions in {sup 240}U. This work supersedes earlier full evaluations of A

  11. Radiation release at the nation's only operating deep geological repository--an independent monitoring perspective.

    PubMed

    Thakur, P; Ballard, S; Hardy, R

    2014-11-01

    Recent incidents at the nation's only operating deep geologic nuclear waste repository, the Waste Isolation Pilot Plant (WIPP), resulted in the release of americium and plutonium from one or more defense-related transuranic (TRU) waste containers into the environment. WIPP is a U.S. Department of Energy mined geologic repository that has been in operation since March, 1999. Over 85,000 m3 of waste in various vented payload containers have been emplaced in the repository. The primary radionuclides within the disposed waste are 239+240Pu and 241Am, which account for more than 99% of the total TRU radioactivity disposed and scheduled for disposal in the repository. For the first time in its 15 years of operation, there was an airborne radiation release from the WIPP at approximately 11:30 PM Mountain Standard Time (MST) on Friday, February 14, 2014. The radiation release was likely caused by a chemical reaction inside a TRU waste drum that contained nitrate salts and organic sorbent materials. In a recent news release, DOE announced that photos taken of the waste underground showed evidence of heat and gas pressure resulting in a deformed lid, in material expelled through that deformation, and in melted plastic and rubber and polyethylene in the vicinity of that drum. Recent entries into underground Panel 7 have confirmed that at least one waste drum containing a nitrate salt bearing waste stream from Los Alamos National Laboratory was breached underground and was the most likely source of the release. Further investigation is underway to determine if other containers contributed to the release. Air monitoring across the WIPP site intensified following the first reports of radiation detection underground to ascertain whether or not there were releases to the ground surface. Independent analytical results of air filters from sampling stations on and near the WIPP facility have been released by us at the Carlsbad Environmental Monitoring & Research Center and confirmed

  12. Nuclear Data Sheets for A = 240

    NASA Astrophysics Data System (ADS)

    Singh, Balraj; Browne, E.

    2008-10-01

    Evaluated experimental data for radioactive decays and reactions for known nuclides (U, Np, Pu, Am, Cm, Bk, Cf) of A = 240 are presented together with adopted values for level energies, γ-ray energies, relative branching ratios and other nuclear properties. This revision was primarily motivated by the need for re-evaluation of absolute gamma-ray intensities from the ɛ decay of 240Am to 240Pu. These quantities are essential for determining precise and accurate cross-sections for the 241Am(n,2n) 240Am reaction using fast neutrons (see e.g. Americium Workshop, Santa Fe, New Mexico, September 2007, 2008To06, 2007Ta01, 2006Pe14) and 241Am(γ,n) reaction (see e.g. 2006Ri08). For 240U, the γ-ray data have now become available. The data sets for 244Pu α decay to 240U; 244Cm α decay to 240Pu and 244Cf α decay to 240Cm have been adapted from evaluations by 1998Ak04 and 2003Ak04. For 244Cm decay, evaluation by 2006BeZL under the Decay Data Evaluation Project (DDEP) is also used. The γ-ray data (energies and intensities) for 240Cm decay are not considered (by the evaluators) as well established. Most detailed data are available only for 240Pu. Extensive data in the second potential well are available for this nuclide together with fission isomers and several superdeformed (SD) structures. For other nuclides spectroscopic data are rather sparse in the literature; especially for the following radioactive decays: The ɛ decays of 240Cf, 240Bk and 240Cm; multipolarities of γ-ray transitions in 240Np from 240U β decay; γ-ray transitions from 244Cf α decay and %ɛ branch of 244Cf decay; spins and parities of excited states in 240U and multipolarities of associated γ-ray transitions in 240U. This work supersedes earlier full evaluations of A = 240 published by 2004Ch64, 1984Sh34, 1977Sc13, 1970Sc39; and an evaluation published in update mode by 1990Sh04.

  13. Radiation release at the nation's only operating deep geological repository--an independent monitoring perspective.

    PubMed

    Thakur, P; Ballard, S; Hardy, R

    2014-11-01

    Recent incidents at the nation's only operating deep geologic nuclear waste repository, the Waste Isolation Pilot Plant (WIPP), resulted in the release of americium and plutonium from one or more defense-related transuranic (TRU) waste containers into the environment. WIPP is a U.S. Department of Energy mined geologic repository that has been in operation since March, 1999. Over 85,000 m3 of waste in various vented payload containers have been emplaced in the repository. The primary radionuclides within the disposed waste are 239+240Pu and 241Am, which account for more than 99% of the total TRU radioactivity disposed and scheduled for disposal in the repository. For the first time in its 15 years of operation, there was an airborne radiation release from the WIPP at approximately 11:30 PM Mountain Standard Time (MST) on Friday, February 14, 2014. The radiation release was likely caused by a chemical reaction inside a TRU waste drum that contained nitrate salts and organic sorbent materials. In a recent news release, DOE announced that photos taken of the waste underground showed evidence of heat and gas pressure resulting in a deformed lid, in material expelled through that deformation, and in melted plastic and rubber and polyethylene in the vicinity of that drum. Recent entries into underground Panel 7 have confirmed that at least one waste drum containing a nitrate salt bearing waste stream from Los Alamos National Laboratory was breached underground and was the most likely source of the release. Further investigation is underway to determine if other containers contributed to the release. Air monitoring across the WIPP site intensified following the first reports of radiation detection underground to ascertain whether or not there were releases to the ground surface. Independent analytical results of air filters from sampling stations on and near the WIPP facility have been released by us at the Carlsbad Environmental Monitoring & Research Center and confirmed

  14. USTUR WHOLE BODY CASE 0269: DEMONSTRATING EFFECTIVENESS OF I.V. CA-DTPA FOR PU

    SciTech Connect

    James, Anthony C.; Sasser , Lyle B.; Stuit, Dorothy B.; Glover, Samuel E.; Carbaugh, Eugene H.

    2008-01-28

    This whole body donation case (USTUR Registrant) involved a single acute inhalation of an acidic Pu(NO3)4 solution in the form of an aerosol ‘mist.’ Chelation treatment with i.v. Ca-EDTA was initiated on the day of the intake, and continued intermittently over 6 months. After 2½ years with no further treatment, a course of i.v. Ca-DTPA was administered. A total of 400 measurements of 239+240Pu excreted in urine were recorded; starting on the first day (both before and during the initial Ca-EDTA chelation), and continuing for 37 years. This sampling included all intervals of chelation. In addition, 91 measurements of 239+240Pu-in-feces were recorded over this whole period. The Registrant died about 38 years after the intake, at age 79 y, with extensive carcinomatosis secondary to adenocarcinoma of the prostate gland. At autopsy, all major soft tissue organs were harvested for radiochemical analyses of their 238Pu, 239+240Pu and 241Am content. Also, all types of bone (comprising about half the skeleton) were harvested for radiochemical analyses, as well as samples of skin, subcutaneous fat and muscle. This comprehensive dataset has been applied to derive ‘chelation-enhanced’ transfer rates in the ICRP Publication 67 plutonium biokinetic model, representing the behaviour of blood-borne and tissue-incorporated plutonium during intervals of therapy. The resulting model of the separate effects of i.v. Ca-EDTA and Ca-DTPA chelation shows that the therapy administered in this case succeeded in reducing substantially the long-term burden of plutonium in all body organs, except for the lungs. The calculated reductions in organ content at the time of death are approximately 40% for the liver, 60% for other soft tissues (muscle, skin, glands, etc.), 50% for the kidneys, and 50% for the skeleton. Essentially all of the substantial reduction in skeletal burden occurred in trabecular bone. This modeling exercise demonstrated that 3-y-delayed Ca-DTPA therapy was as

  15. Reconstruction of local fallout composition and gamma-ray exposure in a village contaminated by the first USSR nuclear test in the Semipalatinsk nuclear test site in Kazakhstan.

    PubMed

    Imanaka, Tetsuji; Yamamoto, Masayoshi; Kawai, Kenta; Sakaguchi, Aya; Hoshi, Masaharu; Chaizhunusova, Nailya; Apsalikov, Kazbek

    2010-11-01

    After the disintegration of the USSR in end of 1991, it became possible for foreign scientists to visit Kazakhstan, in order to investigate the radiological consequences of nuclear explosions that had been conducted at the Semipalatinsk nuclear test site (SNTS). Since the first visit in 1994, our group has been continuing expeditions for soil sampling at various areas around SNTS. The current level of local fallout at SNTS was studied through γ-spectrometry for (137)Cs as well as α-spectrometry for (239,240)Pu. Average values of soil inventory from wide areas around SNTS were 3,500 and 3,700 Bq m(-2) for (137)Cs and (239,240)Pu, respectively, as of January 1, 2000. The average level of (137)Cs is comparable to that in Japan due to global fallout, while the level of (239,240)Pu is several tens of times larger than that in Japan. Areas of strong contamination were found along the trajectories of radioactive fallout, information on which was declassified after the collapse of the USSR. Our recent efforts of soil sampling were concentrated on the area around the Dolon village heavily affected by the radioactive plume from the first USSR atomic bomb test in 1949 and located 110 km east from ground zero of the explosion. Using soil inventory data, retrospective dosimetry was attempted by reconstructing γ-ray exposure from fission product nuclides deposited on the ground. Adopting representative parameters for the initial (137)Cs deposition (13 kBq m(-2)), the refractory/volatile deposition ratio (3.8) and the plume arrival time after explosion (2.5 h), an absorbed dose in air of 600 mGy was obtained for the 1-year cumulative dose in Dolon village, due to the first bomb test in 1949. Considering possible ranges of the parameters, 350 and 910 mGy were estimated for high and low cases of γ-ray dose in air, respectively. It was encouraging that the deduced value was consistent with other estimations using thermal luminescence and archived monitoring data. The present

  16. Flux of transuranium nuclides and chlorinated hydrocarbons in the northwestern Mediterranean

    NASA Astrophysics Data System (ADS)

    Fowler, S. W.; Ballestra, S.; Villeneuve, J.-P.

    1990-09-01

    The transuranium nuclides, plutonium and americium, and selected chlorinated hydrocarbon compounds have been measured in sediment trap samples, bottom sediments and waters. These measurements have been used to quantify vertical fluxes and elucidate particulate biogeochemical cycles, of these man-made contaminants in the northwestern Mediterranean. Sediment trap experiments in the Gulf of Lions (Lacaze-Duthiers Canyon) have shown that transuranic fluxes are considerably higher in the Gulf of Lions, than those which have been reported for the northeast Pacific; principally this is due to the relatively high mass fluxes in this region of the Mediterranean. Water, surface sediment and sediment trap data indicate that 241Am is being transported downward (via particle settling) more rapidly than 239+240Pu. From direct flux measurement, residence times for 239+240Pu and 241Am in the upper 300 m were computed to be 2.5 and 0.14 years, respectively. Comparison of 239+240Pu concentrations in the water column, in 1986, with similar measurements made 5-11 years earlier suggests that fallout input to the Mediterranean has decreased by nearly a factor of 2 during the period 1975-1986. Fluxes of PCB, HCB, γ-HCH and DDT residues varied by as much as an order of magnitude, or more, both temporally and with depth. The average fluxes of most of the compounds in the Lacaze-Duthiers Canyon, during 1985-1986, were quite similar to those measured off the coast of Monaco several years earlier. Generally, the increased chlorinated hydrocarbon fluxes observed with depth were a direct result of the much higher mass fluxes which occurred at depth. Demonstrated differences in PCB concentrations in the settling particles, deposited surface sediments and overlying sediment floc indicate that simple bottom sediment resuspension is not a major contributor to the enhanced PCB flux noted at depth. The PCB concentration in sedimenting particulate material collected from deeper waters, is similar to

  17. Background radioactivity in sediments near Los Alamos, New Mexico.

    PubMed

    McLin, Stephen G

    2004-07-26

    River and reservoir sediments have been collected annually by Los Alamos National Laboratory since 1974 and 1979, respectively. These background samples are collected from five river stations and four reservoirs located throughout northern New Mexico and southern Colorado. Analyses include 3H, 90Sr, 137Cs, total U, 238Pu, 239,240Pu, 241Am, gross alpha, gross beta, and gross gamma radioactivity. Surprisingly, there are no federal or state regulatory standards in the USA that specify how to compute background radioactivity values on sediments. Hence, the sample median (or 0.50 quantile) is proposed for this background because it reflects central data tendency and is distribution-free. Estimates for the upper limit of background radioactivity on river and reservoir sediments are made for sampled analytes using the 0.95 quantile (two-tail). These analyses also show that seven of ten analytes from reservoir sediments are normally distributed, or are normally distributed after a logarithmic or square root transformation. However, only three of ten analytes from river sediments are similarly distributed. In addition, isotope ratios for 137Cs/238Pu, 137Cs/239,240Pu, and 239,240Pu/238Pu from reservoir sediments are independent of clay content, total organic carbon/specific surface area (TOC/SSA) and cation exchange capacity/specific surface area (CEC/SSA) ratios. These TOC/SSA and CEC/SSA ratios reflect sediment organic carbon and surface charge densities that are associated with radionuclide absorption, adsorption, and ion exchange reactions on clay mineral structures. These latter ratio values greatly exceed the availability of background radionuclides in the environment, and insure that measured background levels are a maximum. Since finer-grained reservoir sediments contain larger clay-sized fractions compared to coarser river sediments, they show higher background levels for most analytes. Furthermore, radioactivity values on reservoir sediments have remained

  18. Radionuclide concentrations in vegetation at the Los Alamos National Laboratory in 1998

    SciTech Connect

    G. J. Gonzales; P. R. Fresquez; M. A. Mullen; L. Naranjo, Jr.

    2000-03-01

    This report summarizes and evaluates the concentrations of {sup 3}H, {sup 137}Cs, {sup 238}Pu, {sup 239,240}Pu, {sup 241}Am, {sup 90}Sr, and total U in understory and overstory vegetation collected from Los Alamos National Laboratory (LANL), its perimeter, and regional background areas in 1998. Comparisons to conservative toxicity reference value safe limits were also made. The arithmetic mean LANL radionuclide concentrations in understory were 501 pCi L{sup {minus}1} for {sup 3}H, 0.581 pCi ash g{sup {minus}1} for {sup 137}Cs, 0.001 pCi ash g{sup {minus}1} for {sup 238}Pu, 0.008 pCi ash g{sup {minus}1} for {sup 239,240}Pu, 0.007 pCi ash g{sup {minus}1} for {sup 241}Am, 1.46 pCi ash g{sup {minus}1} for {sup 90}Sr, and 0.233 {micro}g ash g{sup {minus}1} for total uranium. The mean LANL radionuclide concentrations in overstory were 463 pCi L{sup {minus}1} for {sup 3}H, 1.51 pCi ash g{sup {minus}1} for {sup 137}Cs, 0.0004 pCi ash g{sup {minus}1} {sup 238}Pu, 0.008 pCi ash g{sup {minus}1} for {sup 239,240}Pu, 0.014 pCi ash g{sup {minus}1} for {sup 241}Am, 1.97 pCi ash g{sup {minus}1} for {sup 90}Sr, and 0.388 {micro}g ash g{sup {minus}1} for total uranium. Concentrations of radionuclides and total U in both understory and overstory vegetation at LANL generally were not statistically higher than in perimeter and regional background vegetation ({alpha} = 0.05). The exceptions were LANL {sup 3}H > perimeter {sup 3}H (understory) and LANL {sup 3}H background {sup 3}H (overstory). All maximum radionuclide concentrations were lower than toxicity reference values. With the exception of total U, the relationship between contaminant concentration in soil vs. vegetation was insignificant ({alpha} = 0.05). Generally, as the concentration of total U in soil decreased, the concentration in vegetation increased. This held true for both understory and overstory and regardless of whether data were separated by general location (LANL, perimeter, and background) or not. There was no

  19. Monopole strength function of deformed superfluid nuclei

    NASA Astrophysics Data System (ADS)

    Stoitsov, M.; Kortelainen, M.; Nakatsukasa, T.; Losa, C.; Nazarewicz, W.

    2011-10-01

    We present an efficient method for calculating strength functions using the finite-amplitude method (FAM) for deformed superfluid heavy nuclei within the framework of the nuclear density functional theory. We demonstrate that FAM reproduces strength functions obtained with the fully self-consistent quasiparticle random-phase approximation (QRPA) at a fraction of the computational cost. As a demonstration, we compute the isoscalar and isovector monopole strengths for strongly deformed configurations in 100Zr and 240Pu by considering huge quasiparticle QRPA spaces. Our approach to FAM, based on Broyden's iterative procedure, opens the possibility for large-scale calculations of strength distributions in well-deformed superfluid nuclei across the nuclear landscape.

  20. Radial Power Profile of MOX and LEU Fuel Pellet Versus Burnup

    SciTech Connect

    Chang, Gray S.; Pedersen, Robert C.

    2002-07-01

    One of challenge to burn the WG-Pu in Mixed Oxide (MOX) fuel in light water reactors (LWR) is to demonstrate that the differences between WG-MOX, RG-MOX, and LWR LEU fuel are minimal, and therefore, the commercial MOX and LEU fuel experience base is applicable. The MCWO-calculated Radial Power Profile of LEU, Weapons Grade-MOX and Reactor Grade-MOX fuel pellets at various burnups are similar toward the end of life (50 GWd/t). Therefore, the LEU fuel performance evaluation code - FRAPCON-3 with modifications, such as, the detailed fission power profiles versus burnup, can be used in the MOX fuel pellet performance analysis. MCWO also calculated the {sup 240}Pu/Pu ratio in WG-MOX versus burnup, which reaches an average of 31.25% at discharged burnup of 50 GWd/t. It meets the spent fuel standard for WG-Pu disposition in LWR. (authors)

  1. The Characterization of Biotic and Abiotic Media Upgradient and Downgradient of the Los Alamos Canyon Weir

    SciTech Connect

    P.R. Fresquez

    2006-01-15

    As per the Mitigation Action Plan for the Special Environmental Analysis of the actions taken in response to the Cerro Grande Fire, sediments, vegetation, and small mammals were collected directly up- and downgradient of the Los Alamos Canyon weir, a low-head sediment control structure located on the northeastern boundary of Los Alamos National Laboratory, to determine contaminant impacts, if any. All radionuclides ({sup 3}H, {sup 137}Cs, {sup 238}Pu, {sup 239,240}Pu, {sup 90}Sr, {sup 241}Am, {sup 234}U, {sup 235}U and {sup 238}U) and trace elements (Ag, As, Ba, Be, Cd, Cr, Cu, Hg, Ni, Pb, Sb, Se, and Tl) in these media were low and most were below regional upper level background concentrations (mean plus three sigma). The very few constituents that were above regional background concentrations were far below screening levels (set from State and Federal standards) for the protection of the human food chain and the terrestrial environment.

  2. 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).

  3. The concentration of radionuclides and metals in vegetation adjacent to and in the SRL Seepage Basins

    SciTech Connect

    Murphy, C. E. Jr.

    1992-12-14

    In 1991 the trees on the dikes surrounding the SRL Seepage Basins were sampled and analyzed to inventory the contaminants transported from the basins into the vegetation. Tree leaves and wood were collected and analyzed for {sup 90}Sr, {sup 60}Co, {sup 137}Cs, {sup 238}Pu, {sup 239,240}Pu, {sup 242,244}Cm, {sup 241}Am, Ba, Cr, Hg, Mg, Mn, Ni, and Pb. The concentrations of contaminants were influenced by sample type (leaves versus wood), species type (pines versus hardwoods), and location relative to distance from the basin. The total inventory of each contaminant in the trees was estimated. The relationships between leaf and wood, pines and hardwood, location, and mass of the material in each of these classes were used to weight the total inventory estimate. The radionuclide with the largest inventory was 0.7 mCi for {sup 90}Sr. The metallic contaminant with the largest inventory was Mn at 200 gm.

  4. The concentration of radionuclides and metals in vegetation adjacent to and in the SRL Seepage Basins

    SciTech Connect

    Murphy, C. E. Jr.

    1992-12-14

    In 1991 the trees on the dikes surrounding the SRL Seepage Basins were sampled and analyzed to inventory the contaminants transported from the basins into the vegetation. Tree leaves and wood were collected and analyzed for [sup 90]Sr, [sup 60]Co, [sup 137]Cs, [sup 238]Pu, [sup 239,240]Pu, [sup 242,244]Cm, [sup 241]Am, Ba, Cr, Hg, Mg, Mn, Ni, and Pb. The concentrations of contaminants were influenced by sample type (leaves versus wood), species type (pines versus hardwoods), and location relative to distance from the basin. The total inventory of each contaminant in the trees was estimated. The relationships between leaf and wood, pines and hardwood, location, and mass of the material in each of these classes were used to weight the total inventory estimate. The radionuclide with the largest inventory was 0.7 mCi for [sup 90]Sr. The metallic contaminant with the largest inventory was Mn at 200 gm.

  5. 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

  6. 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.

  7. Radiological dose assessments of atolls in the Northern Marshall Islands

    SciTech Connect

    Robison, W.L.

    1983-11-01

    Methods and models used to estimate the radiation doses to a returning population of the atolls in the Marshall Islands are presented. In this environment natural processes have acted on source-term radionuclides for nearly 30 years. The data bases developed for the models, and the results of the radiological dose analyses at the various atolls are described. The major radionuclides in order of their contribution to the total estimated doses were /sup 137/Cs, /sup 90/Sr, /sup 239/ /sup 240/Pu, /sup 241/Am, and /sup 60/Co. Exposure pathways in order of their contribution to the estimated doses were: terrestrial food chain, external ..gamma.., marine food chain, inhalation, and cistern water and ground water. 56 references, 13 figures, 16 tables.

  8. Concentrations of radionuclides in reef and lagoon pelagic fish from the Marshall Islands

    SciTech Connect

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

    1981-07-01

    A radiological survey was conducted from September through November of 1978 to assess the concentrations of persistent man-made radionuclides in the terrestrial and marine environments of 11 atolls and 2 islands of the Northern Marshall Islands. The atolls and islands include Rongelap, Utirik, Taka, Bikar, Rongerik, Ailinginae, Likiep, Jemo, Ailuk, Mejet, Wotho, Ujelang and Bikini. Over 4000 terrestrial and marine samples were collected for radionuclide analysis from 76 different islands. Soils, vegetation, indigenous animals, and cistern and groundwater were collected from the islands. Reef fish, pelagic species, clams, lagoon water, and sediments were obtained from the lagoons. A report is given of all available concentration data for /sup 137/Cs, /sup 90/Sr, /sup 239+240/Pu, /sup 238/Pu, /sup 241/Am as well as naturally occurring /sup 40/K and other gamma emitting radionuclides in tissues and organs of different species of fish collected from the atolls.

  9. Distribution of artificial radionuclides in lacustrine sediments in China.

    PubMed

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

    2011-07-01

    Establishing accurate historical records of the distribution, inventory and source of artificial radionuclides in the environment is important for environmental monitoring and radiological health protection due to their potential toxicity, and is also useful for identification and risk assessment of possible future environmental inputs of radionuclides from nuclear weapons tests and accidental release from the nuclear fuel reprocessing facilities or nuclear power reactors. A sector-field inductively coupled plasma mass spectrometer was used to study the recent sedimentation of Pu isotopes in 11 lakes in China. The distribution of (137)Cs was investigated using the conventional radiometric analytical methods. Based on the isotopic compositions of Pu and the activity ratio of (137)Cs/(239+240)Pu, the sources of artificial radionuclides were identified. The potential applications of Pu isotopes for sediment dating and for regional and global environmental change studies were discussed. PMID:21498412

  10. Induced fission of Pu240 within a real-time microscopic framework

    DOE PAGES

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

    2016-03-25

    Here, we describe the fissioning dynamics of 240Pu 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 nuclearmore » dynamics, where all collective degrees of freedom (CDOF) are included (unlike adiabatic treatments with a small number of CDOF).« less

  11. 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.

  12. [Dynamic study of the cytogenetic effects in blood lymphocytes from humans living in the Chernobyl Atomic Energy Station exclusion zone without permission].

    PubMed

    Bezdrobnaia, L K; Tsyganok, T V; Romanova, E P; Tarasenko, L V; Fedorchenko, V I

    2002-01-01

    The cytogenetic examination of a group of people, self-residing in ChNPP Exclusion Zone with soil contamination density 137Cs 74-477 kBq/m2, 90Sr 33-289 kBq/m2, 238, 239 + 240Pu 1.5-10.0 kBq/m2, was conducted in 1998-1999 and also 2001. It is shown, that after 12-15 years of the accident the level of chromosome damages in Zone self-residents' lymphocytes detected by a routine analysis is higher then at the residents of control Yagotin district, Kiev region and comes to a plateau. Lymphocytes with multiple chromosome damages are detected. The probability of its transuranium elements induction which are present in the Zone is discussed at present. PMID:12530160

  13. 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.

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

    PubMed

    Hirose, Katsumi; Povinec, Pavel P

    2015-01-01

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

  15. Initial performance of the advanced inventory verification sample system (AVIS)

    SciTech Connect

    Marlow, Johnna B; Swinhoe, Martyn T; Menlove, Howard O; Rael, Carlos D

    2009-01-01

    This paper describes the requirements, design and initial performance of the Advanced Inventory Verification Sample System (AVIS) a non-destructive assay (NDA) system to measure small samples of bulk mixed uranium-plutonium oxide (MOX) materials (powders and pellets). The AVIS design has evolved from previously developed conceptual physics and engineering designs for the Inventory Sample Verification System (INVS), a safeguards system for nondestructive assay of small samples. The AVIS is an integrated gamma-neutron system. Jointly designed by the Nuclear Material Control Center (NMCC) and the Los Alamos National Laboratory (LANL), AVIS is intended to meet a performance specification of a total measurement uncertainty of less than 0.5% in the neutron ({sup 240}Pu{sub effective}) measurement. This will allow the AVIS to replace destructive chemical analysis for many samples, with concomitant cost, exposure and waste generation savings for the facility. Data taken to date confirming the performance of the AVIS is presented.

  16. Prototype Neutron Portal Monitor Detector

    NASA Astrophysics Data System (ADS)

    Schier, W.

    2014-05-01

    A very large drum-shaped neutron detector which could replace the 3He neutron portal monitor detector is under development. Detection is based on the 6Li(n,3H)4He reaction. 6Li metal is evaporated onto aluminum plates then covered with 22-cm x 27-cm ZnS(Ag) scintillation sheets and sealed about the edges. The equivalent of 40 detector plates will be arrayed in the 80-cm diameter drum housing and viewed by a single 20-cm diameter hemispherical photomultiplier tube without the use of light guides. Presently 25 detector plates are installed. Light collection tests are performed with a bare 210Po alpha source on a ZnS(Ag) disk. Neutron detection studies include neutrons from a 2-curie PuBe source and from a 0.255-gram 240Pu source.

  17. A survey of radioactive fallout data in Alaska

    SciTech Connect

    DePhillips, M.P.

    1995-10-23

    Considerable attention has been directed by the scientific community to assessing the levels and fate of radionuclides in Arctic ecosystems. The following text and tables present available data and discussion of radionuclide fallout in Alaska. A literature search of 23 on-line databases (Table 1) using Alaska, Strontium (Sr), Cesium (Cs), Plutonium (Pu) and Radionuclide as constraint terms responded with 177 possible citations. After eliminating duplicate citations, 31 articles were available: 17 were relevant to the subject matter; the remainder addressed geologic issues. All of the cited literature addressed {sup 137}Cs, {sup 90}Sr and {sup 239,240}Pu as a result of radionuclide fallout from nuclear testing or accidental release.

  18. 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.

  19. The underwater coincidence counter for plutonium measurements in mixed-oxide fuel assemblies manual

    SciTech Connect

    G. W. Eccleston; H. O. Menlove; M. Abhold; M. Baker; J. Pecos

    1999-05-01

    This manual describes the Underwater Coincidence Counter (UWCC) that has been designed for the measurement of plutonium in mixed-oxide (MOX) fuel assemblies prior to irradiation. The UWCC uses high-efficiency {sup 3}He neutron detectors to measure the spontaneous-fission and induced-fission rates in the fuel assembly. Measurements can be made on MOX fuel assemblies in air or underwater. The neutron counting rate is analyzed for singles, doubles, and triples time correlations to determine the {sup 240}Pu effective mass per unit length of the fuel assembly. The system can verify the plutonium loading per unit length to a precision of less than 1% in a measurement time of 2 to 3 minutes. System design, components, performance tests, and operational characteristics are described in this manual.

  20. Dose Estimates from Ingestion of Marine and Terrestrial Animals Harvested in the Beaufort Sea and Northwestern Alaska

    SciTech Connect

    W. C. T. Inkret; M. E. Schillaci; D. W. Efurd; M. E. Ennis; M. J. Hameedi; J. M. Inkret; T. H. T. Little; G. Miller

    2000-11-01

    Between 1993 and 1995, marine and terrestrial animal samples were collected from the Beaufort Sea and northwest Alaska. These samples were analyzed at Los Alamos National Laboratory for the presence of the anthropogenic radionuclides, {sup 90}Sr, {sup 137}Cs, {sup 238}Pu, {sup 239+240}Pu, and {sup 241}Am. The measurement data were combined with food consumption rates based on survey results for populations residing in three northwest Alaskan communities and published age-dependent ingestion dose coefficients to estimate potential radiological impacts from the consumption of traditional animal foods harvested in this region. The results of this study indicate that committed equivalent doses to adults from {sup 90}Sr and {sup 137}Cs, due to consumption of traditional food sources are consistent with currently accepted estimates of average doses to adults in North America due to atmospheric nuclear weapons testing fallout.

  1. 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

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

    PubMed Central

    Hirose, Katsumi; Povinec, Pavel P.

    2015-01-01

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

  3. Concentrations of Radionuclides and Trace Elements in Soils and Vegetation Around the DARHT Facility during 2004

    SciTech Connect

    P.R. Fresquez

    2004-10-01

    Samples of soil, sediment, and unwashed overstory and understory vegetation were collected at four locations around the Dual-Axis Radiographic Hydrodynamic Test (DARHT) facility at Los Alamos National Laboratory (LANL). All samples were analyzed for concentrations of {sup 3}H, {sup 137}Cs, {sup 90}Sr, {sup 238}Pu, {sup 239,240}Pu, {sup 241}Am, {sup 234}U, {sup 235}U, {sup 238}U, Ag, As, Ba, Be, Cd, Cr, Cu, Hg, Ni, Pb, Sb, Se, and Tl. These results, which represent five years since the start of operations, were compared with baseline statistical reference level (BSRL) data established over a four-year-long preoperational period prior to DARHT operations, and to LANL and U.S. Environmental Protection Agency Screening Action Levels (SALs). Most radionuclides and trace elements in soil, sediment, and vegetation were below BSRL values and those soils/sediments that were above BSRLs were far below SALs.

  4. Application of flow analysis in determination of selected radionuclides.

    PubMed

    Kołacińska, Kamila; Trojanowicz, Marek

    2014-07-01

    The subject of this article is the review of developed applications of flow analysis methods for determination of radionuclides hard-to-detect in reactor cooling waters ((90)Sr, (239,240)Pu, and (241)Am), and also (99)Tc, which are released to the environment primarily through nuclear fuel processing. Flow analysis, which developed for decades parallel to flow methods of chemical synthesis, is widely employed in modern chemical analysis, mainly for environmental, food analysis and pharmaceutical applications. It allows the simplification of design of analytical instruments and procedures, the shortening of analysis time, improvement of precision, and often the automation of whole analytical procedure. All those factors can be also advantageous for determination of critical radionuclides for process needs and protection of environment. The review is based on 84 references, published mainly in leading analytical journals. PMID:24840425

  5. [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).

  6. 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.

  7. 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

  8. Comparisons of HELIOS Calculated Isotope Concentrations to Measured Values for Several Reactor Systems

    SciTech Connect

    Charlton, W.S.; Perry, R.T.; Fearey, B.L.; Parish, T.A.

    1998-10-21

    Heavy metal and fission product noble gas concentrations in spent fuel from two different PWR'S were calculated using HELIOS and compared to measured results from the literature. It was found that for the U-235/U-238 and Pu-240/Pu-239 isotopic ratios, the HELIOS calculation agreed to within the experimental uncertainty. For the Xe-131/Xe-134 isotopic ratios, HELIOS tended to overestimate the result by up to 4%. Conversely for the Xe-132/Xe-134 ratios, HELIOS underestimated the result by a slight amount ({approximately}1%). This suggests that either the fission product yields for Xe-131 and Xe-132 should be slightly altered or that the absorption cross-section for Xe-131 should be slightly increased. More analysis is necessary to determine which of these two alternatives is more appropriate. This work has shown that the accuracy of HELIOS (within 2% for heavy metals and within 4% for fission noble gases) is sufficient for most analyses.

  9. 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.

  10. Fiber optic calorimetry

    SciTech Connect

    Rudy, C.; Bayliss, S.; Bracken, D.; Bush, J.; Davis, P.

    1998-01-01

    A twin-bridge calorimeter using optical fiber as the sensor element was constructed and tested. This system demonstrates the principle and capability of using fiber for heat-flow measurements of special nuclear material. This calorimeter uses piezoelectric-generated phase-carrier modulation with subsequent electronic signal processing to allow phase shifts as small as 1 microradian ({mu}rad) to be measured. The sensing element consists of 21-m lengths of single-mode optical fiber wrapped around sample and reference chambers. The sensitivity of the calorimeter was determined to be 74 radians (rad) of phase shift per milliwatt of thermal power. One milliwatt of thermal power is equivalent to 400 mg of plutonium (6% {sup 240}Pu). The system noise base was about 0.2 rad, equivalent to about 1 mg of plutonium.

  11. Fiber Optic Calorimetry

    SciTech Connect

    Rudy, C.; Bayliss, S.; Bracken, D.; Bush, J.; Davis, P.

    1997-12-12

    A twin-bridge calorimeter using optical fiber as the sensor element was constructed and tested. This system demonstrates the principle and capability of using optical fibers for heat-flow measurements of special nuclear material. This calorimeter uses piezoelectric-generated phase-carrier modulation with subsequent electronic signal processes to allow phase shifts as small as 1 microradian ({micro}rad) to be measured. The sensing element consists of 21-m lengths of single-mode optical fiber wrapped around sample and reference chambers. The sensitivity of the calorimeter was determined to be 74 radians (rad) of phase shift per milliwatt of thermal power. One milliwatt of thermal power is equivalent to 400 mg of plutonium (6% {sup 240}Pu). The system noise base was about 0.2 rad, equivalent to about 1 mg of plutonium.

  12. 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.

  13. 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.

  14. Monopole Strength Function of Deformed Superfluid Nuclei

    SciTech Connect

    Stoitsov, M. V.; Kortelainen, E. M.; Nakatsukasa, T.; Losa, C.; Nazarewicz, Witold

    2011-01-01

    We present an efficient method for calculating strength functions using the finite amplitude method (FAM) for deformed superfluid heavy nuclei within the framework of the nuclear density functional theory. We demonstrate that FAM reproduces strength functions obtained with the fully self-consistent quasi-particle random-phase approximation (QRPA) at a fraction of computational cost. As a demonstration, we compute the isoscalar and isovector monopole strength for strongly deformed configurations in ^{240}Pu by considering huge quasi-particle QRPA spaces. Our approach to FAM, based on Broyden's iterative procedure, opens the possibility for large-scale calculations of strength distributions in well-bound and weakly bound nuclei across the nuclear landscape.

  15. 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.

  16. 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.

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

    NASA Astrophysics Data System (ADS)

    Hirose, Katsumi; Povinec, Pavel P.

    2015-10-01

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

  18. 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

  19. 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.

  20. 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.

  1. 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.

  2. A Discordancy Between Short-Term Sedimentation Rate Using Pb-210, Cs-137 and Pu and Long-Term Sedimentation Rate Using C-14

    NASA Astrophysics Data System (ADS)

    Baskaran, M.; Filley, T. R.; Bianchi, T. S.; Freeman, K. H.; Hatcher, P. G.

    2005-12-01

    Short-lived radionuclides (210Pb, 137Cs, etc) have been successfully utilized to obtain sedimentation rates in freshwater and coastal marine environments over the past 3 decades. Combined use of 210Pb and Pu enable to delineate sedimentation from sediment mixing. However independent validation of short-term accumulation rates using other long-lived isotopes, such as 14C are very limited. We collected a sediment core from a sinkhole lake, Mud Lake, Florida, USA and analyzed it for 210Pb, 137Cs, 239,240Pu and 14C. The sediment inventories of 137Cs, and 239,240Pu are comparable to the regional global fallout values while 210Pb inventory is comparable to the value reported for this region. A plot of depth against 14C age yields an intercept value of 1070 yrs, indicating a reservoir correction age of 1070 yrs. Most of the data points fall either on the straight line or close to the line possibly suggesting that the relative proportion of fossil carbon had remained constant throughout the core. Due to sediment compaction, a comparison of linear sedimentation rate obtained using short-lived radionuclides with those 14C could yield considerable difference and hence we compared the mass accumulation rates obtained from these isotopes. The 210Pbxs-based sediment mass accumulation rate of 17 mg cm-2 y-1, is almost a factor of 3 higher than that obtained using 14C -derived mass accumulation rate of 6 mg cm-2 y-1. The peak fallout of Pu is well preserved in the lake core suggesting relatively minimum sediment mixing. The factors that could cause this discordancy between the long-term and short-term mass accumulation rates will be discussed.

  3. Particle count monitoring of reverse osmosis water treatment for removal of low-level radionuclides

    SciTech Connect

    Moritz, E.J.; Hoffman, C.R.; Hergert, T.R.

    1995-03-01

    Laser diode particle counting technology and analytical measurements were used to evaluate a pilot-scale reverse osmosis (RO) water treatment system for removal of particulate matter and sub-picocurie low-level radionuclides. Stormwater mixed with Waste Water Treatment Plant (WWTP) effluent from the Rocky Flats Environmental Technology Site (RFETS), formerly a Department of Energy (DOE) nuclear weapons production facility, were treated. No chemical pretreatment of the water was utilized during this study. The treatment system was staged as follows: multimedia filtration, granular activated carbon adsorption, hollow tube ultrafiltration, and reverse osmosis membrane filtration. Various recovery rates and two RO membrane models were tested. Analytical measurements included total suspended solids (TSS), total dissolved solids (TDS), gross alpha ({alpha}) and gross beta ({beta}) activity, uranium isotopes {sup 233/234}U and {sup 238}U, plutonium {sup 239/240}Pu, and americium {sup 241}Am. Particle measurement between 1--150 microns ({mu}) included differential particle counts (DPC), and total particle counts (TPC) before and after treatment at various sampling points throughout the test. Performance testing showed this treatment system produced a high quality effluent in clarity and purity. Compared to raw water levels, TSS was reduced to below detection of 5 milligrams per liter (mg/L) and TDS reduced by 98%. Gross {alpha} was essentially removed 100%, and gross {beta} was reduced an average of 94%. Uranium activity was reduced by 99%. TPC between 1-150{mu} were reduced by an average 99.8% to less than 1,000 counts per milliliter (mL), similar in purity to a good drinking water treatment plant. Raw water levels of {sup 239/240}Pu and {sup 241}Am were below reliable quantitation limits and thus no removal efficiencies could be determined for these species.

  4. 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.

  5. The Northern Marshall Islands radiological survey: Data and dose assessments

    SciTech Connect

    Robison, W.L.; Noshkin, V.E.; Conrado, C.L.

    1997-07-01

    Fallout from atmospheric nuclear tests, especially from those conducted at the Pacific Proving Grounds between 1946 and 1958, contaminated areas of the Northern Marshall Islands. A radiological survey at some Northern Marshall Islands was conducted from September through November 1978 to evaluate the extent of residual radioactive contamination. The atolls included in the Northern Marshall Islands Radiological Survey (NMIRS) were Likiep, Ailuk, Utirik, Wotho, Ujelang, Taka, Rongelap, Rongerik, Bikar, Ailinginae, and Mejit and Jemo Islands. The original test sites, Bikini and Enewetak Atolls, were also visited on the survey. An aerial survey was conducted to determine the external gamma exposure rate. Terrestrial (soil, food crops, animals, and native vegetation), cistern and well water samples, and marine (sediment, seawater, fish and clams) samples were collected to evaluate radionuclide concentrations in the atoll environment. Samples were processed and analyzed for {sup 137}Cs, {sup 90}Sr, {sup 239+240}Pu and {sup 241}Am. The dose from the ingestion pathway was calculated using the radionuclide concentration data and a diet model for local food, marine, and water consumption. The ingestion pathway contributes 70% to 90% of the estimated dose. Approximately 95% of the dose is from {sup 137}Cs accounts for about 10% to 30% of the dose. {sup 239+240}Pu and {sup 241}Am are the major contributors to dose via the inhalation pathway; however, inhalation accounts for only about 1% of the total estimated dose, based on surface soil levels and resuspension studies. All doses are computed for concentrations decay corrected to 1996. The maximum annual effective dose from manmade radionuclides at these atolls ranges from .02 mSv y{sup -1}. The background dose in the Marshall Islands is estimated to be 2.4 mSv y{sup -1} to 4.5 mSv y{sup -1}. The 50-y integral dose ranges from 0.5 to 65 mSv. 35 refs., 2 figs., 9 tabs.

  6. Systematic effects in neutron coincidence and multiplicity counting

    SciTech Connect

    Evans, Louise G; Favorite, Jeffrey A; Swinhoe, Martyn T

    2010-01-01

    Correlated neutron counting, including neutron coincidence and multiplicity counting, is an important tool in nuclear material accountancy verification. The accuracy of such measurements is of interest to the safeguards community because as the accuracy of NDA improves, the number of samples that are required to undergo destructive analysis (DA) decreases. The accuracy of a neutron mUltiplicity measurement can be affected by a number of variables. Monte Carlo neutron transport simulations with MCNPX have been performed to understand how the properties of the sample affect the count rate. These resultant count rates have been analyzed with the 'point model' in order to determine the effect on the deduced plutonium mass. The sample properties that have been investigated are density, sample position within the detector cavity, moisture content, isotopic composition, plutonium to total actinide ratio and heavy metal fraction. These parameters affect the Singles, Doubles and Triples count rates in different ways. In addition, different analysis methods use these measured quantities in different combinations, so that the final sensitivity of the {sup 240}Pu mass to each parameter also depends on the analysis method used. For example, the passive calibration curve method only used the Doubles rate to produce the {sup 240}Pu mass and so is not sensitive to changes in the Singles rate (to first order). The analysis methods considered here were passive calibration curve (non-multiplication corrected), known alpha (multiplication corrected) and multiplicity with known efficiency. The effects were studied on both a small mass MOX sample (1 g Pu) and a large MOX sample (6000 g Pu) both measured in high efficiency neutron multiplicity counters. In order to determine the final effect of each parameter it is necessary to know not only the sensitivity of the plutonium mass to that parameter, but also the range over which the parameter can realistically vary. Some estimates are

  7. 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.

  8. Radionuclide concentration ratios in Australian terrestrial wildlife and livestock: data compilation and analysis.

    PubMed

    Johansen, M P; Twining, J R

    2010-11-01

    Radionuclide concentrations in Australian terrestrial fauna, including indigenous kangaroos and lizards, as well as introduced sheep and water buffalo, are of interest when considering doses to human receptors and doses to the biota itself. Here, concentration ratio (CR) values for a variety of endemic and introduced Australian animals with a focus on wildlife and livestock inhabiting open rangeland are derived and reported. The CR values are based on U- and Th-series concentration data obtained from previous studies at mining sites and (241)Am and (239/240)Pu data from a former weapons testing site. Soil-to-muscle CR values of key natural-series radionuclides for grazing Australian kangaroo and sheep are one to two orders of magnitude higher than those of grazing cattle in North and South America, and for (210)Po, (230)Th, and (238)U are one to two orders of magnitude higher than the ERICA tool reference values. When comparing paired kangaroo and sheep CR values, results are linearly correlated (r = 0.81) for all tissue types. However, kidney and liver CR values for kangaroo are typically higher than those of sheep, particularly for (210)Pb, and (210)Po, with values in kangaroo liver more than an order of magnitude higher than those in sheep liver. Concentration ratios for organs are typically higher than those for muscle including those for (241)Am and (239/240)Pu in cooked kangaroo and rabbit samples. This study provides CR values for Australian terrestrial wildlife and livestock and suggests higher accumulation rates for select radionuclides in semi-arid Australian conditions compared with those associated with temperate conditions. PMID:20711841

  9. 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

  10. Transuranic resuspension

    SciTech Connect

    Sehmel, G.A.

    1984-04-01

    Characteristics of aged resuspension sources are more uncertain than those of new resuspension sources, which can be investigated using inert-particle controlled-tracer sources. Even though airborne concentrations are low, one aged uniform-area source which can be used for resuspension studies is the accumulated radionuclide fallout in the soil from stratospheric and tropospheric fallout debris. Airborne radionuclide concentrations from this source were investigated at convenient locations on the Hanford site. The objective is to summarize plutonium and americium resuspension research conducted by the Pacific Northwest Laboratory from 1977 to 1983. Airborne plutonium was determined at five sites in the Hanford area, and both plutonium and americium were determined at two Hanford sites. Airborne plutonium and americium were examined as a function of aerodynamic particle diameter, sampling height, wind speed increments, and wind direction increments. The following results are discussed: airborne radionuclide concentrations, ..mu..Ci/cm/sup 3/ of sampled air; radionuclide activity densities, ..mu..Ci/g of airborne solids; airborne plutonium fluxes, ..mu..Ci/(m/sup 2/ day); /sup 241/Am//sup 239 +240/Pu) activity ratios, (..mu..Ci /sup 241/Am)/(..mu..Ci/sup 239 +240/Pu); and airborne solid concentrations, ..mu..g/m/sup 3/ of sampled air. In addition, a relationship based on field data for aged plutonium sources at Bikini Atoll, the Hanford site, and Rocky Flats was developed to estimate the maximum expected plutonium activity density on airborne solids compared to activity densities for bulk surface-soil samples. As a result, it is possible to more accurately predict resuspension factor ranges as a function of the resuspension source activity densities. 31 references, 18 figures, 5 tables.

  11. 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.

  12. Territory contamination with the radionuclides representing the fuel component of Chernobyl fallout.

    PubMed

    Kashparov, V A; Lundin, S M; Zvarych, S I; Yoshchenko, V I; Levchuk, S E; Khomutinin, Y V; Maloshtan, I M; Protsak, V P

    2003-12-30

    The data obtained through a series of experiments were used to specify the correlation of activities of the fuel component radionuclides of Chernobyl fallout and to create the maps of the 30-km Chernobyl zone terrestrial density of contamination with 154Eu, 238Pu, 239+240Pu and 241Am (on 01.01.2000). In the year 2000, total inventories of the fuel component radionuclides in the upper 30-cm soil layer of the 30-km Chernobyl zone in Ukraine (outside the ChNPP industrial site, excluding the activity located in the radioactive waste storages and in the cooling pond) were estimated as: 90Sr--7.7 x 10(14) Bq; 137Cs--2.8 x 10(15) Bq; 154Eu--1.4 x 10(13) Bq; 238Pu--7.2 x 10(12) Bq; 239+240Pu--1.5 x 10(13) Bq; 241Am--1.8 x 10(13) Bq. These values correspond to 0.4-0.5% of their amounts in the ChNPP unit 4 at the moment of the accident. The current estimate is 3 times lower than the previous widely-cited estimates. Inventories of the fuel component radionuclides were also estimated in other objects within the 30-km zone and outside it. This allowed more accurate data to be obtained on the magnitude of a relative release of radionuclides in the fuel particles (FP) matrix during the Chernobyl accident outside the ChNPP industrial site. It amounts to 1.5+/-0.5% of these radionuclides in the reactor, which is 2 times lower than the previous estimates. Two-thirds of the radionuclides release in the FP was deposited on the territory of Ukraine. PMID:14630415

  13. 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.

  14. Tracing the origin of suspended sediment in a large Mediterranean river by combining continuous river monitoring and measurement of artificial and natural radionuclides.

    PubMed

    Zebracki, Mathilde; Eyrolle-Boyer, Frédérique; Evrard, Olivier; Claval, David; Mourier, Brice; Gairoard, Stéphanie; Cagnat, Xavier; Antonelli, Christelle

    2015-01-01

    Delivery of suspended sediment from large rivers to marine environments has important environmental impacts on coastal zones. In France, the Rhone River (catchment area of 98,000 km(2)) is by far the main supplier of sediment to the Mediterranean Sea and its annual solid discharge is largely controlled by flood events. This study investigates the relevance of alternative and original fingerprinting techniques based on the relative abundances of a series of radionuclides measured routinely at the Rhone River outlet to quantify the relative contribution of sediment supplied by the main tributaries during floods. Floods were classified according to the relative contribution of the main subcatchments (i.e., Oceanic, Cevenol, extensive Mediterranean and generalised). Between 2000 and 2012, 221 samples of suspended sediment were collected at the outlet and were shown to be representative of all flood types that occurred during the last decade. Three geogenic radionuclides (i.e., (238)U, (232)Th and (40)K) were used as fingerprints in a multivariate mixing model in order to estimate the relative contribution of the main subcatchment sources-characterised by different lithologies-in sediment samples collected at the outlet. Results showed that total sediment supply originating from Pre-Alpine, Upstream, and Cevenol sources amounted to 10, 7 and 2.10(6)tons, respectively. These results highlight the role of Pre-Alpine tributaries as the main sediment supplier (53%) to the Rhone River during floods. Other fingerprinting approaches based on artificial radionuclide activity ratios (i.e., (137)Cs/(239+240)Pu and (238)Pu/(239+240)Pu) were tested and provided a way to quantify sediment remobilisation or the relative contributions of the southern tributaries. In the future, fingerprinting methods based on natural radionuclides should be further applied to catchments with heterogeneous lithologies. Methods based on artificial radionuclides should be further applied to catchments

  15. Radionuclide concentrations in fish and invertebrates from Bikini Atoll

    SciTech Connect

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

    1988-01-01

    As in other global studies, /sub 137/Cs was found in the highest concentrations in edible flesh of all species of fish and in the lowest concentrations in the bone or liver. The mean concentration of /sup 137/Cs in muscle of reef fish from the southern part of the atoll is comparable to the global-fallout concentration measured in market samples of fish collected from Chicago, IL, USA, in 1982. Strontium-90 is associated generally with non-edible parts of fish, such as bone or viscera. Twenty-five to fifty percent of the total body burden of /sub 60/Co is accumulated in the muscle tissue; the remainder is distributed among the liver, skin, and viscera. The mean concentration of /sub 60/Co in fish has been decreasing at a rate faster than radiological decay alone. Most striking is the range of /sup 207/Bi concentrations among different species of fish collected at the same time and place. Highest concentrations of /sup 207/Bi were consistently detected in the muscle and other tissues of goatfish and some of the pelagic lagoon fish. In other reef fish, such as mullet, surgeonfish, and parrotfish, /sub 207/Bi was usually below detection limits by gamma spectrometry. Over 70% of the whole-body activity of /sup 207/Bi in goatfish is associated with the muscle tissue, whereas less than 5% is found in the muscle of mullet and surgeonfish. Neither /sup 239 +240/Pu nor /sup 241/Am is accumulated significantly in the muscle tissue of any species of fish. Apparently, /sup 238/Pu is in a more readily available form for accumulation by fishes than /sup 239 +240/Pu. Based on a daily ingestion rate of 200 g of fish flesh, dose rates to individuals through the fish-food ingestion pathway are well below current Federal guidelines. 24 refs., 1 fig., 27 tabs

  16. Radionuclides from the Fukushima accident in the air over Lithuania: measurement and modelling approaches.

    PubMed

    Lujanienė, G; Byčenkienė, S; Povinec, P P; Gera, M

    2012-12-01

    Analyses of (131)I, (137)Cs and (134)Cs in airborne aerosols were carried out in daily samples in Vilnius, Lithuania after the Fukushima accident during the period of March-April, 2011. The activity concentrations of (131)I and (137)Cs ranged from 12 μBq/m(3) and 1.4 μBq/m(3) to 3700 μBq/m(3) and 1040 μBq/m(3), respectively. The activity concentration of (239,240)Pu in one aerosol sample collected from 23 March to 15 April, 2011 was found to be 44.5 nBq/m(3). The two maxima found in radionuclide concentrations were related to complicated long-range air mass transport from Japan across the Pacific, the North America and the Atlantic Ocean to Central Europe as indicated by modelling. HYSPLIT backward trajectories and meteorological data were applied for interpretation of activity variations of measured radionuclides observed at the site of investigation. (7)Be and (212)Pb activity concentrations and their ratios were used as tracers of vertical transport of air masses. Fukushima data were compared with the data obtained during the Chernobyl accident and in the post Chernobyl period. The activity concentrations of (131)I and (137)Cs were found to be by 4 orders of magnitude lower as compared to the Chernobyl accident. The activity ratio of (134)Cs/(137)Cs was around 1 with small variations only. The activity ratio of (238)Pu/(239,240)Pu in the aerosol sample was 1.2, indicating a presence of the spent fuel of different origin than that of the Chernobyl accident.

  17. Isotopic Pu, Am and Cm signatures in environmental samples contaminated by the Fukushima Dai-ichi Nuclear Power Plant accident.

    PubMed

    Yamamoto, M; Sakaguchi, A; Ochiai, S; Takada, T; Hamataka, K; Murakami, T; Nagao, S

    2014-06-01

    Dust samples from the sides of roads (black substances) have been collected together with litter and soil samples at more than 100 sites contaminated heavily in the 20-km exclusion zones around Fukushima Dai-ichi Nuclear Power Plant (FDNPP) (Minamisoma City, and Namie, Futaba and Okuma Towns), in Iitate Village located from 25 to 45 km northwest of the plant and in southern areas from the plant. Isotopes of Pu, Am and Cm have been measured in the samples to evaluate their total releases into the environment from the FDNPP and to get the isotopic compositions among these nuclides. For black substances and litter samples, in addition to Pu isotopes, (241)Am, (242)Cm and (243,244)Cm were determined for most of samples examined, while for soil samples, only Pu isotopes were determined. The results provided a coherent data set on (239,240)Pu inventories and isotopic composition among these transuranic nuclides. When these activity ratios were compared with those for fuel core inventories in the FDNPP accident estimated by a group at JAEA, except (239,240)Pu/(137)Cs activity ratios, fairly good agreements were found, indicating that transuranic nuclides, probably in the forms of fine particles, were released into the environment without their large fractionations. The obtained data may lead to more accurate information about the on-site situation (e.g., burn-up, conditions of fuel during the release phase, etc.), which would be difficult to get otherwise, and more detailed information on the dispersion and deposition processes of transuranic nuclides and the behavior of these nuclides in the environment. PMID:24531259

  18. Tracer-level radioactive pilot-scale test of in situ vitrification for the stabilization of contaminated soil sites at ORNL

    SciTech Connect

    Spalding, B.P.; Jacobs, G.K.; Naney, M.T. ); Dunbar, N.W. ); Tixier, J.S.; Powell, T.D. )

    1992-11-01

    A field demonstration of in situ vitrification (ISV) was completed in May 1991, and produced approximately 12 Mg of melted earthen materials containing 12.7 mCi of radioactivity within 500 g of sludge in amodel of an old seepage trench waste disposal unit. Past waste disposal operations at Oak Ridge National Laboratory have left several contaminated seepage sites. In planning for remediation of such sites, ISV technology has been identified as a leading candidate because of the high risks associated with any retrieval option and because of the usual high quality of vitreous waste form. Major isotopes placed in the test trench were [sup 137]Cs and [sup 90]Sr, with lesser amounts of [sup 6O]Co, [sup 241]Am, and [sup 239,240]Pu. A total of 29 MWh of electrical power was delivered to the ground over a 5-day period producing a melt depth of 8.5 ft. During melting, 2.4% of the [sup 137]Cs volatilized from the melt into an off-gas containment hood and was captured quantitatively on a high efficiency particulate air filter. No volatilization of [sup 90]Sr, [sup 241]Am, or [sup 239,240]Pu was detected and > 99.993% retention of these isotopes in the melt was estimated. The use of added rare earth tracers (Ce, La, and Nd), as surrogates for transuranic isotopes, led to estimated melt retentions of >99.9995% during the test. The molten material, composed of the native soil and dolomitic limestone used for filling the test trench, reached a processing temperature of 1500[degrees]C. Standardized leaching procedures using Product Consistency Testing indicated that the ISV product has excellent characteristics relative to other vitreous nuclear waste forms.

  19. Nevada test site radionuclide inventory and distribution program: Report number 4, Areas 18 and 20

    SciTech Connect

    McArthur, R D; Mead, S W

    1988-04-01

    As part of the Radionuclide Inventory and Distribution Program on the Nevada Test Site, in situ measurements of gamma-emitting radionuclides were made at more than 600 locations in six regions near ground zeros in Areas 18 and 20. In addition, several soil samples were collected from each region and analyzed to determine inverse relaxation lengths and radionuclide ratios. Analysis of the data from Area 20 led to estimated inventories of 23 Ci of /sup 241/Am, 30 Ci of /sup 238/Pu, 41 Ci of /sup 239,240/Pu, 18 Ci of /sup 60/Co, 6.4 Ci of /sup 137/Cs, 6.0 Ci of /sup 90/Sr, 17 Ci of /sup 152/Eu, 19 Ci of /sup 154/Eu, and 6.6 Ci of /sup 155/Eu. For Area 18, the estimated inventories were 27 Ci of /sup 241/Am, 4.9 Ci of /sup 238/Pu, 150 Ci of /sup 239,240/Pu, 1.3 Ci of /sup 60/Co, 4.9 Ci of /sup 137/Cs, 13 Ci of /sup 90/Sr, 2.1 Ci of /sup 152/Eu, 1.3 Ci of /sup 154/Eu, and 1.4 Ci of /sup 155/Eu. The locations of the measurements in Area 18 were chosen by importance sampling, which permits the calculation of an estimate of the sampling error. Maps of radionuclide distributions were also generated for all regions except the area near the Palanquin and Cabriolet ground zeros. 3 refs., 65 figs., 7 tabs.

  20. 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.

  1. Pairing-induced speedup of nuclear spontaneous fission

    DOE PAGES

    Sadhukhan, Jhilam; Dobaczewski, J.; Nazarewicz, W.; Sheikh, J. A.; Baran, A.

    2014-12-22

    Collective inertia is strongly influenced at the level crossing at which the quantum system changes its microscopic configuration diabatically. Pairing correlations tend to make the large-amplitude nuclear collective motion more adiabatic by reducing the effect of these configuration changes. Competition between pairing and level crossing is thus expected to have a profound impact on spontaneous fission lifetimes. To elucidate the role of nucleonic pairing on spontaneous fission, we study the dynamic fission trajectories of 264Fm and 240Pu using the state-of-the-art self-consistent framework. We employ the superfluid nuclear density functional theory with the Skyrme energy density functional SkM* and a density-dependentmore » pairing interaction. Along with shape variables, proton and neutron pairing correlations are taken as collective coordinates. The collective inertia tensor is calculated within the nonperturbative cranking approximation. The fission paths are obtained by using the least action principle in a four-dimensional collective space of shape and pairing coordinates. Pairing correlations are enhanced along the minimum-action fission path. For the symmetric fission of 264Fm, where the effect of triaxiality on the fission barrier is large, the geometry of the fission pathway in the space of the shape degrees of freedom is weakly impacted by pairing. This is not the case for 240Pu, where pairing fluctuations restore the axial symmetry of the dynamic fission trajectory. The minimum-action fission path is strongly impacted by nucleonic pairing. In some cases, the dynamical coupling between shape and pairing degrees of freedom can lead to a dramatic departure from the static picture. As a result, in the dynamical description of nuclear fission, particle-particle correlations should be considered on the same footing as those associated with shape degrees of freedom.« less

  2. LONG-TERM DYNAMICS OF RADIONUCLIDE VERTICAL MIGRATION IN SOILS OF THE CHERNOBYL NUCLEAR POWER PLANT EXCLUSION ZONE

    SciTech Connect

    Farfan, E

    2009-11-19

    The radioactive fallout from the Chernobyl Nuclear Power Plant (ChNPP) accident consisted of fuel and condensation components. An important radioecological task associated with the late phase of the accident is to evaluate the dynamics of radionuclide mobility in soils. Identification of the variability (or invariability) in the radionuclide transfer parameters makes it possible to (1) accurately predict migration patterns and biological availability of radionuclides and (2) evaluate long-term exposure trends for the population who may reoccupy the remediated abandoned areas. In 1986-1987, a number of experimental plots were established within various tracts of the fallout plume to assist with the determination of the long-term dynamics of radionuclide vertical migration in the soils. The transfer parameters for {sup 137}Cs, {sup 90}Sr, and {sup 239,240}Pu in the soil profile, as well as their ecological half-time of the radionuclide residence (T{sub 1/2}{sup ecol}) values in the upper 5-cm thick soil layers of different grasslands were estimated at various times since the accident. Migration characteristics in the grassland soils tend to decrease as follows: {sup 90}Sr > {sup 137}Cs {ge} {sup 239,240}Pu. It was found that the {sup 137}Cs absolute T{sub 1/2}{sup ecol} values are 3-7 times higher than its radioactive decay half-life value. Therefore, changes in the exposure dose resulting from the soil deposited {sup 137}Cs now depend only on its radioactive decay. The {sup 90}Sr T{sub 1/2}{sup ecol} values for the 21st year after the fallout tend to decrease, indicating an intensification of its migration capabilities. This trend appears consistent with a pool of mobile {sup 90}Sr forms that grows over time due to destruction of the fuel particles.

  3. 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.

  4. Concentrations of radionuclides in fish collected from Bikini Atoll between 1977 and 1984

    SciTech Connect

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

    1986-07-01

    This report summarizes all available data on the concentrations of radionuclides in fish from Bikini Atoll between 1977 and 1984. As found in other global studies, /sup 137/Cs is most highly accumulated in edible flesh of all species of fish, the lowest fractions are found in the bone or liver. The mean concentration of /sup 137/Cs in muscle of reef fish from the southern part of the atoll is comparable to the global fallout concentration measured in market samples of fish collected from Chicago, Illinois, in 1982. /sup 90/Sr is generally associated with non-edible parts of fish, such as bone or viscera. Twenty-five to fifty percent of the total body burden of /sup 60/Co is accumulated in the muscle tissue; the remainder is distributed among the liver, skin, and viscera. The mean concentration of /sup 60/Co in fish has been decreasing at a rate faster than radiological decay alone. Most striking is the range of /sup 207/Bi concentrations among different species of fish collected at the same time and place. Highest concentrations of /sup 207/Bi were consistently detected in the muscle (and other tissues) of goatfish and some of the pelagic lagoon fish. In other reef fish, such as mullet, surgeonfish, and parrotfish, /sup 207/Bi was usually below detection limits by gamma spectrometry. Over 70% of the whole-body activity of /sup 207/Bi in goatfish is associated with the muscle tissue, whereas less than 5% is found in the muscle of mullet and surgeonfish. Neither /sup 239 +240/Pu nor /sup 241/Am is significantly accumulated in the muscle tissue of any spe