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Sample records for 239pu 240pu isotope

  1. Determination of 240Pu/239Pu isotope ratios in Kara Sea and Novaya Zemlya sediments using accelerator mass spectrometry

    Accelerator mass spectrometry (AMS) has been used to determine Pu activity concentrations and 240Pu/239Pu isotope ratios in sediments from the Kara Sea and radioactive waste dumping sites at Novaya Zemlya. Measured 239,240Pu activities ranged from 0.06 - 9.8 Bq/kg dry weight, 240Pu/239Pu atom ratios ranged from 0.13 to 0.28, and 238Pu/239,240Pu activity ratios from 0.02 to 0.6. Perturbations from global fallout isotope ratios were evident at three sites: the Yenisey Estuary and Abrosimov Fjords where 240Pu/239Pu ratios were lower (0.13-0.14); and Stepovogo Fjord sediments where ratios were higher (up to 0.28) than fallout ratios. Based on procedural blanks, detection limits for AMS were below 1 fg Pu and the method showed good precision for isotope ratio measurements, minimal matrix, interference and memory effects. For high level samples, comparison between alpha spectrometry and AMS gave good agreement for measurement of 239,240Pu activity concentrations. (author)

  2. Isotope ratios of 240Pu/239Pu in soil samples from different areas

    Plutonium concentrations and 240Pu/239Pu atom ratios in soil samples from Japan and other areas in the world (including IAEA standard reference materials) were determined by ICP-MS. The range of 240Pu/239Pu atom ratios observed in 21 Japanese soil samples was 0.155 - 0.194 and the average was 0.180 ± 0.011, which is comparable to the global fallout value. A low ratio of about 0.05, which is derived from Pu-bomb, was found in samples from Nishiyama (Nagasaki) and Mururoa Atoll (IAEA-368), while a high ratio of about 0.31 was found in a sample from Bikini Atoll (Marshall Islands). The ratio for Irish Sea sediment (IAEA-135) was 0.21, which was higher than the global fallout value, suggesting the influence by the contamination from the Sellafield facility. The 240Pu/239Pu atom ratios in soils from the Chernobyl area were determined, and the ratio was found to be very high (about 0.4), indicating the high burn-up grade of the reactor fuel. These results show that the 240Pu/239Pu ratio can be used as a finger print to identify the source of the contamination. (author)

  3. Presence of plutonium isotopes, {sup 239}Pu and {sup 240}Pu, in soils from Chile

    Chamizo, E., E-mail: echamizo@us.es [Centro Nacional de Aceleradores, Avda. Thomas Alba Edison, 7, 41092 Sevilla (Spain); Garcia-Leon, M., E-mail: manugar@us.es [Departamento de Fisica Atomica, Molecular y Nuclear, Universidad de Sevilla, Avda. Reina Mercedes sn, 41012 Seville (Spain); Peruchena, J.I., E-mail: jiperuchena@gmail.com [Centro Nacional de Aceleradores, Avda. Thomas Alba Edison, 7, 41092 Sevilla (Spain); Cereceda, F., E-mail: francisco.cereceda@usm.cl [Laboratorio de Quimica Ambiental, Centro de Tecnologias Ambientales (CETAM), Universidad Tecnica Federico Santa Maria, Casilla 110-V, Valparaiso (Chile); Vidal, V., E-mail: victor.vidal@usm.cl [Laboratorio de Quimica Ambiental, Centro de Tecnologias Ambientales (CETAM), Universidad Tecnica Federico Santa Maria, Casilla 110-V, Valparaiso (Chile); Pinilla, E., E-mail: epinilla@unex.es [Departamento de Quimica Analitica, Facultad de Ciencias, Universidad de Extremadura, Avda. de Elvas sn, 06071 Badajoz (Spain); Miro, C., E-mail: cmiro@unex.es [Departamento de Fisica Aplicada, Universidad de Extremadura, Avda. de la Universidad sn, 10071 Caceres (Spain)

    2011-12-15

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

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

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

  5. Plutonium isotopes 238Pu, 239+240Pu, 241Pu and 240Pu/239Pu atomic ratios in the southern Baltic Sea ecosystem

    Dagmara I. Strumińska-Parulska

    2010-09-01

    Full Text Available The paper summarizes the results of plutonium findings in atmospheric fallout samples and marine samples from the southern Baltic Sea during our research in 1986-2007. The activities of 238Pu and 239+240Pu isotopes were measured with an alpha spectrometer. The activities of 241Pu were calculated indirectly by 241Am activity measurements 16-18 years after the Chernobyl accident. The 240Pu/239Pu atomic ratios were measured using accelerator mass spectrometry (AMS. The 241Pu activities indicate that the main impact of the Chernobyl accident was on the plutonium concentration in the components of the Baltic Sea ecosystem examined in this work. The highest 241Pu/239+240Pu activity ratio was found in sea water (140 ± 33. The AMS measurements of atmospheric fallout samples collected during 1986 showed a significant increase in the 240Pu/239Pu atomic ratio from 0.29 ± 0.04 in March 1986 to 0.47 ± 0.02 in April 1986.

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

    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.

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

    Xu, Yihong; Qiao, Jixin; Hou, Xiaolin;

    2014-01-01

    This paper reports an analytical method for the determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) 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 7.5×105 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...

  8. 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.

    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

  9. 240Pu/239Pu atom ratios in seawater from the western North Pacific and its marginal sea

    Full text: The atom ratio of 240Pu/239Pu is known to be a useful tracer to identify the sources of plutonium in the ocean. The objectives of this study are to measure the 239+240Pu activities and 240Pu/239Pu atom ratios in seawater from the western North Pacific and its marginal sea and to discuss the transport processes of plutonium. The 240Pu/239Pu atom ratios were measured with sector-field ICPMS. The atom ratios were significantly higher than the mean global fallout ratio. These high atom ratios proved the existence of close-in fallout plutonium originating from the Pacific proving grounds. (author)

  10. Neutron inelastic-scattering cross sections of 232Th, 233U, 235U, 238U, 239Pu and 240Pu

    Differential-neutron-emission cross sections of 232Th, 233U, 235U, 238U, 239Pu and 240Pu are measured between approx. = 1.0 and 3.5 MeV with the angle and magnitude detail needed to provide angle-integrated emission cross sections to approx. 232Th, 233U, 235U and 238U inelastic-scattering values, poor agreement is observed for 240Pu, and a serious discrepancy exists in the case of 239Pu

  11. Perturbation in the 240Pu/239Pu global fallout ratio in local sediments following the nuclear accidents at Thule (Greenland) and Palomares (Spain).

    Mitchell, P I; León Vintró, L; Dahlgaard, H; Gascó, C; Sánchez-Cabeza, J A

    1997-08-25

    It is well established that the main source of the plutonium found in marine sediments throughout the Northern Hemisphere is global stratospheric fallout, characterized by a typical 240Pu/239Pu atom ratio of approximately 0.18. Measurement of perturbations in this ratio at various sites which had been subjected to close-in fallout, mainly from surface-based testing (e.g. Bikini Atoll, Nevada test site, Mururoa Atoll), has confirmed the feasibility of using this ratio to distinguish plutonium from different fallout sources. In the present study, the 240Pu/239Pu ratio has been examined in samples of sediment (and soil) collected at Thule (Greenland) and Palomares (Spain), where accidents involving the release and dispersion of plutonium from fractured nuclear weapons occurred in 1968 and 1966, respectively. The 240Pu/239Pu ratio was measured by high-resolution alpha spectrometry and spectral deconvolution, and confirmed in the case of the most active samples by high-resolution X-ray spectrometry. Only samples which displayed plutonium heterogeneities, i.e. hot particles or concentrations well in excess (at least two orders of magnitude) of those expected from global fallout, were selected for analysis. The analytical results showed that at Thule the mean 240Pu/239Pu atom ratio was 0.033 +/- 0.004 (n = 4), while at Palomares the equivalent ratio appeared to be significantly higher at 0.056 +/- 0.003 (n = 4). Both ratios are indicative of low burn-up plutonium and are consistent with those reported for weapons-grade plutonium. It is noteworthy that the mean 238Pu/239Pu activity ratio in the Thule samples, at 0.0150 +/- 0.0017 (n = 4), was also lower than that measured in the Palomares samples, namely, 0.0275 +/- 0.0012 (n = 4). The 241Pu/239Pu ratios were similarly different. Finally, the data show, in contrast to Palomares, that not all of the samples from the Thule accident site were contaminated with plutonium of identical isotopic composition. PMID:9241884

  12. Comparison of evaluations for 235U, 239Pu, 240Pu, 241Pu and 242Pu with integral measurements

    The evaluations for 235U, 239Pu, 240Pu, 241Pu and 242Pu are considered. Intercomparison is made of the neutron cross section data from INDL/A, ENDL-84, ENDF/B-5 and ENDF/B-6 (where applicable). Integral measurements of the spectrum averaged cross sections are compared to the values derived from evaluated data libraries. (author). 40 refs, 49 figs, 11 tabs

  13. Estimation of uncertainties in resonance parameters of {sup 56}Fe, {sup 239}Pu, {sup 240}Pu and {sup 238}U

    Nakagawa, Tsuneo; Shibata, Keiichi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    1997-05-01

    Uncertainties have been estimated for the resonance parameters of {sup 56}Fe, {sup 239}Pu, {sup 240}Pu and {sup 238}U contained in JENDL-3.2. Errors of the parameters were determined from the measurements which the evaluation was based on. The estimated errors have been compiled in the MF32 of the ENDF format. The numerical results are given in tables. (author)

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

    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. PMID:25723106

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

    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 239Pu and 240Pu concentration and 240Pu/239Pu atom ratio using inductively coupled plasma sector field mass spectrometry (ICP-SFMS). Plutonium concentrations and 240Pu/239Pu atom ratios were generally consistent with previous terrestrial and marine studies in the region. The 239+240Pu 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 240Pu/239Pu atom ratios were significantly higher in marine samples compared to terrestrial and freshwater samples (t-test, p 240Pu/239Pu ratios in terrestrial samples are within the range of global fallout. • Elevated 240Pu/239Pu in marine samples was characteristic of North Pacific Ocean. • Potential sources of enriched Pu to the marine environment regionally are suggested. • Pu ratios cannot by themselves explain the enriched Pu in seawater around Amchitka

  16. Feedback on 239Pu and 240Pu nuclear data and associated covariances through the CERES integral experiments

    Benchmark measurements of irradiated and un-irradiated fuel samples were performed in the framework of the CERES collaborative program between AEA (UK Atomic Energy Agency) and CEA (French Atomic Energy Commission). These experiments provide relevant data for the validation of fuel burn-up and criticality-safety calculations for the whole fuel cycle. As part of this program, pile-oscillation measurements were carried out on a range of mixed-oxide samples with plutonium of various mass and isotopic contents, both in the MINERVE and DIMPLE reactors. Four core configurations, two over-thermalized situations and two pressurized water reactor (PWR)-type situations, were constituted with different forward and adjoint flux spectra, emphasizing fission and/or capture contributions. The experiments were analyzed using reference TRIPOLI4 calculations with the JEFF-3.1.1 library, using exact three-dimensional models of the core configurations. In a first step, calculations of each DIMPLE configuration were performed and compared with the experiment, showing very good agreements with a maximum C-E of -230 pcm. In the second step, reactivity worth experiments were analyzed, using recently developed exact-perturbation capabilities in TRIPOLI4. A consistent assimilation of calculation over experiment discrepancies was performed with the CONRAD code, using the integral data assimilation method. Covariance matrix on multigroup neutron cross sections and multiplicities were generated and significant trends were identified, especially on the 239Pu and 240Pu capture cross sections in the thermal energy range (E < 0.1 eV). Further investigations should be required to confirm these conclusions, due to the strong dependence of these trends and of posterior covariances to prior covariances. (author)

  17. Determination of the 240Pu/239Pu atom ratio in low activity environmental samples by alpha spectrometry and spectral deconvolution

    In this paper, a simple technique, based on commercially-available software developed for gamma spectra analysis (MicroSAMPO trademark), is described by which this complex multiplet can be resolved at the much lower activities typical of many environmental samples. In our approach, it is not necessary to make any alterations to the normal alpha spectrometric set-up (including energy dispersion), other than to improve collimation. The instrumental function is defined for each spectrum by fitting a modified gaussian with exponential tails to the comparatively well-resolved 242Pu ''doublet'' (used as tracer) and, if present, the 238Pu ''doublet''. The fitted peaks are used to create an energy calibration file with which, using published energy data, the positions (in channels) of the component peaks of the multiplet are predicted. These positions are not altered subsequently when MicroSAMPO's interactive multiplet analysis facility is used to quantify the relative spectral intensities of the components. Before calculating the 240Pu/239Pu ratio, it is advisable to correct for coincidence summing of alpha particles and conversion electrons. The technique has been applied to the determination of the 240Pu/239Pu ratio in a set of environmental samples, most of which were supplied by IAEA-MEL under their laboratory intercomparison programme. Subsequently, replicate samples were analysed independently using thermal ionisation mass spectrometry. The agreement between the two sets of data was most satisfactory. Further validation of this deconvolution technique was provided by the good agreement between the measured alpha-emission probabilities for the component peaks in the 239,240Pu multiplet and published values. (orig.)

  18. Perturbation in the 240Pu/239Pu global fallout ratio in local sediment following the nuclear accidents at Thule (Greenland) and Palomares (Spain)

    It is well established that the main source of the plutonium found in marine sediments throughout the Northern Hemisphere is global stratospheric fallout, characterized by a typical 240Pu/239Pu atom ratio of ∼0.18. Measurements of perturbations in this ratio at various sites which had been subjected to close-in fallout, mainly from surface-based testing, has confirmed the feasibility of using this ratio to distinguish plutonium from different fallout sources. In the present study, the 240Pu/239Pu ratio has been examined in samples of sediment collected at Thule (Greenland) and Palomares (Spain), where accidents involving the release and dispersion of plutonium from fractured nuclear weapons occurred in 1968 and 1966, respectively. The 240Pu/239Pu ratio was measured by high-resolution alpha spectrometry and spectral deconvolution. The analytical results showed that at Thule the mean 240Pu/239Pu atom ratio was 0.033±0.004, while at Palomares the equivalent ratio appeared to be significantly higher at 0.056±0.003. Both ratios are consistent with those reported for soils samples at the Nevada site and Nagasaki, and are clearly indicative of weapons-grade plutonium. 27 refs., 1 fig., 2 tabs

  19. Precision and accuracy in the determination of sup(238)Pu/(sup(239)Pu + sup(240)Pu) alpha activity ratio by alpha spectrometry

    Investigations were carried out for the evaluation of precision and accuracy in determining sup(238)Pu/(sup(239)Pu + sup(240)Pu) activity ratio by α spectrometry from the point of view of determining sup(238)Pu accurately in plutonium samples and in exploiting Isotope Dilution Alpha Spectrometry (IDAS) for determining the concentration of plutonium in the irradiated fuel dissolver solutions. Synthetic mixtures with α activity ratios ranging from 0.01 to 10 were prepared using sup(238)Pu and sup(239)Pu isotopes. Different methods which can be routinely used were tried to calculate the α activity ratio from the α spectrum taken on electrodeposited sources prepared from these mixtures. An accuracy of better than 0.5% and a precision of +- 0.2% (1 sigma) is demonstrated in the determination of α activity ratios ranging from 0.01 to 10 using electrodeposited sources and the evaluation method based on the geometric progression decrease (G.P.) for the far tail of the spectrum. (auth.)

  20. Comparison of the ENDF/B-V and SOKRATOR evaluations of 235U, 239Pu, 240Pu and 241Pu at low neutron energies

    The US and USSR's most recent evaluationsof 235U, 239Pu, 240Pu and 241Pu are compared over the thermal region and over the first few resonances. The two evaluations rest on essentially the same experimental data base and the differences reflect different approaches to the representation of the cross sections or different weightings of the experimental results. It is found that over the thermal and resolved ranges the two evaluations are very similar. Some differences in approaches are briefly discussed

  1. Speciation analysis of 129I, 137Cs, 232Th, 238U, 239Pu and 240Pu in environmental soil and sediment

    The environmental mobility and bioavailability of radionuclides are related to their physicochemical forms, namely species. We here present a speciation analysis of important radionuclides including 129I (also 127I), 137Cs, 232Th, 238U and plutonium isotopes (239Pu and 240Pu) in soil (IAEA-375) and sediment (NIST-4354) standard reference materials and two fresh sediment samples from Øvre Heimdalsvatnet Lake, Norway. A modified sequential extraction protocol was used for the speciation analysis of these samples to obtain fractionation information of target radionuclides. Analytical results reveal that the partitioning behaviour, and thus the potential mobility and bioavailability, are exclusively featured for the individual radionuclide. Iodine is relatively mobile and readily binds to organic matter, while plutonium is mainly bound to both organic matter and nitric acid leachable fractions. Thorium is predominated in nitric acid leachable fraction and caesium is primarily observed in nitric acid and aqua regia leachable fractions and residue. Our analytical results reveal that around 50% of uranium might still remain in the residue which could not be extracted with aggressive acid, namely, aqua regia.

  2. Simultaneous measurement of {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, and {sup 242}Pu by high resolution inductively coupled plasma mass spectrometer (HR ICP-MS) in marine sediments; Mesure des isotopes du plutonium des sediments marins par spectrometrie de masse a plasma couple inductivement haute resolution (HR ICP-MS)

    Bruneau, F

    1999-07-01

    Transuranics elements are of particular interest in radioecological studies because of their radiotoxicity and their potential use to decipher source fingerprints and transport processes. The simultaneous measurement of {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, and {sup 242}Pu in environmental samples requires a specific chemical procedure. This work deals with an analytical procedure which yields a very high grade of purification of Pu suitable for ultra low level detection by HR ICP-MS, from marine sediments. After the elimination of major elements (Fe, Al, Mg...) by a first chromatographic separation, a new device of purification by solvent extraction and concentration by a second chromatographic separation is used to obtain a concentrated and high purified solution of plutonium. The chemical procedure have been validated on IAEA certified sediment samples and on sediment samples collected in the roads of Cherbourg which had been previously analysed by other techniques (a spectrometry and thermo-ionisation mass spectrometer). (author)

  3. Evaluation of fission cross sections and covariances for {sup 233}U, {sup 235}U, {sup 238}U, {sup 239}Pu, {sup 240}Pu, and {sup 241}Pu

    Kawano, Toshihiko [Kyushu Univ., Fukuoka (Japan); Matsunobu, Hiroyuki [Data Engineering, Inc. (Japan); Murata, Toru [AITEL Corporation, Tokyo (JP)] [and others

    2000-02-01

    A simultaneous evaluation code SOK (Simultaneous evaluation on KALMAN) has been developed, which is a least-squares fitting program to absolute and relative measurements. The SOK code was employed to evaluate the fission cross sections of {sup 233}U, {sup 235}U, {sup 238}U, {sup 239}Pu, {sup 240}Pu, and {sup 241}Pu for the evaluated nuclear data library JENDL-3.3. Procedures of the simultaneous evaluation and the experimental database of the fission cross sections are described. The fission cross sections obtained were compared with evaluated values given in JENDL-3.2 and ENDF/B-VI. (author)

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

    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.

  5. Simultaneous measurement of 239Pu, 240Pu, 241Pu, and 242Pu by high resolution inductively coupled plasma mass spectrometer (HR ICP-MS) in marine sediments

    Transuranics elements are of particular interest in radioecological studies because of their radiotoxicity and their potential use to decipher source fingerprints and transport processes. The simultaneous measurement of 239Pu, 240Pu, 241Pu, and 242Pu in environmental samples requires a specific chemical procedure. This work deals with an analytical procedure which yields a very high grade of purification of Pu suitable for ultra low level detection by HR ICP-MS, from marine sediments. After the elimination of major elements (Fe, Al, Mg...) by a first chromatographic separation, a new device of purification by solvent extraction and concentration by a second chromatographic separation is used to obtain a concentrated and high purified solution of plutonium. The chemical procedure have been validated on IAEA certified sediment samples and on sediment samples collected in the roads of Cherbourg which had been previously analysed by other techniques (a spectrometry and thermo-ionisation mass spectrometer). (author)

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

    The variation of the 236U and 239Pu concentrations as a function of depth has been studied in a soil profile at a site in the Southern Hemisphere well removed from nuclear weapon test sites. Total inventories of 236U and 239Pu as well as the 236U/239Pu isotopic ratio were derived. For this investigation a soil core from an undisturbed forest area in the Herbert River catchment (17°30′ – 19°S) which is located in north-eastern Queensland (Australia) was chosen. The chemical separation of U and Pu was carried out with a double column which has the advantage of the extraction of both elements from a relatively large soil sample (∼20 g) within a day. The samples were measured by Accelerator Mass Spectrometry using the 14UD pelletron accelerator at the Australian National University. The highest atom concentrations of both 236U and 239Pu were found at a depth of 2–3 cm. The 236U/239Pu isotopic ratio in fallout at this site, as deduced from the ratio of the 236U and 239Pu inventories, is 0.085 ± 0.003 which is clearly lower than the Northern Hemisphere value of ∼0.2. The 236U inventory of (8.4 ± 0.3) × 1011 at/m2 was more than an order of magnitude lower than values reported for the Northern Hemisphere. The 239Pu activity concentrations are in excellent agreement with a previous study and the 239+240Pu inventory was (13.85 ± 0.29) Bq/m2. The weighted mean 240Pu/239Pu isotopic ratio of 0.142 ± 0.005 is slightly lower than the value for global fallout, but our results are consistent with the average ratio of 0.173 ± 0.027 for the southern equatorial region (0–30°S). - Highlights: • Exploration of uranium-236 (236U) and plutonium-239 (239Pu) in the Southern Hemisphere by accelerator mass spectrometry. • We report the depth profile for both isotopes from a forest site well removed from nuclear test or reactor sites. • 236U and 239Pu were deposited at the same time due to nuclear weapons tests but show a slightly different depth dependence. • The

  7. Statistical activities during 1976 and the design and initial analysis of nuclear site studies. [/sup 241/Am, /sup 137/Cs, /sup 239/Pu, /sup 240/Pu

    Gilbert, R O; Essington, E H; Brady, D N; Doctor, P G; Eberhardt, L L

    1977-05-01

    Statistical design and analysis activities for the Nevada Applied Ecology Group (NAEG) during 1976 are briefly outlined. This is followed by a description of soil data collected thus far at nuclear study sites. Radionuclide concentrations in surface soil collected along a transect from ground zero (GZ) along the main fallout pattern are given for Nuclear Site (NS) 201. Concentrations in soil collected at 315 locations on a grid system at 200 foot spacings are also given for this site. The /sup 241/Am to /sup 137/Cs ratios change over NS 201 depending on location relative to GZ. They range from less than one where /sup 241/Am is at low levels, to more than fifty where /sup 241/Am levels are high (near GZ). The estimated median /sup 239/ /sup 240/Pu to /sup 241/Am ratio is 11 and appears to be relatively constant over the area (the 95 percent lower and upper limits on the true median ratio are about 8 and 14).

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

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

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

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

    2016-05-01

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

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

    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

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

    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

  12. Beta-decay half-lives of neutron rich Cu and Ni isotopes produced by thermal fission of 235U and 239Pu

    The half-lives of very neutron rich isotopes of Ni and Cu have been measured. The isotopes are produced in very asymmetric thermal fission of 235U and 239Pu at the I.L.L. high flux reactor. They are separated by means of the Lohengrin spectrometer. They are identified with a ΔE-E ionization chamber and implanted in one of the 8 Si planar detectors where the β- particles are also detected. The time correlations between the implantation and the detection of β- particles provide the half-life. The values obtained are compared to current theoretical predictions

  13. Determining the age and history of plutonium using isotope correlations and experimentally determined data on isotopic abundances of plutonium and 241Am

    Linear correlations using a data set of nominally cooled samples of Pu formed in Indian PHWRs using experimentally determined 241Pu/239Pu versus 240Pu/239Pu and 241Am/239Pu versus 240Pu/239Pu isotope ratios have been developed which can be used for determining the age of Pu. By correlating both Pu and Am isotopic information, an understanding of how the material was processed, when chemical separations occurred to remove 241Am as well as the true age of the Pu in sample can be obtained. Two actual samples from a PHWR with unknown origin were analyzed as a part of case study for application of this new methodology. (author)

  14. Status of 239Pu evaluations

    This paper summarises the current status of nuclear data evaluations for n+239Pu. The nuclear data we address include fission, capture, scattering cross-sections, as well as the prompt fission neutron energy spectrum, which has large sensitivities to the criticality benchmark testing. The evaluated nuclear data files currently available for 239Pu are compared, and the source of differences in the cross-sections are discussed. Some open questions on the statistical model calculations for deformed systems are also given. (authors)

  15. Isotopic signature of plutonium at Bikini atoll

    Atom ratios of the isotopes 239Pu, 240Pu, 241Pu and 244Pu were determined in sediments and soils from Bikini atoll using low energy Accelerator Mass Spectrometry. All samples had been contaminated by local fallout from nuclear weapon testing between 1946 and 1958 and show significant variations in the isotopic composition, which are ascribed to the different yields of single tests and to the mixture of material from various devices. Differences in the 244Pu/239Pu ratio (2.8-5.7x10-4) are more pronounced than in the 240Pu/239Pu ratio of the same samples and provide complementary information to distinguish the sources of contamination.

  16. Analysis Method of 241Pu Radioactivity by Isotope Dilution-Extraction Liquid Scintillation Spectrometer

    2008-01-01

    <正>241Pu is the only pure β emitter with the maximum energy of 20.81 keV in plutonium isotopes of 238Pu, 239Pu, 240Pu and 242Pu, in which 241Pu is mostly specific radioactivity because its half-life is 14.29 a.

  17. Sector field inductively coupled plasma mass spectrometry in the elemental and isotopic analysis of lanthanides and actinides

    Plutonium is one element which is indispensable in identifying the source and for estimating the hazardous effects of rad. The isotopic ratios of plutonium (240Pu/239Pu) and its total concentration in environmental samples were also precisely estimated by high resolution inductively coupled plasma mass spectrometry

  18. Ultra-sensitive Mass Spectrometric and Other Advanced Methods Applied to Biological Samples. Second interlaboratory comparison study for the analysis of 239Pu in synthetic urine at the μBq (∼100 aCi) level by mass spectrometry

    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 239Pu 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 239Pu in urine at the μBq/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 μBq of 239Pu per liter of synthetic urine. Each test sample also contained 240Pu at a 240Pu/239Pu atom ratio of ∼0.15 and natural uranium at a concentration of 50 μBq/ml. From the results of the two studies, it can be inferred that the best performance at the μBq 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. (author)

  19. Rapid Determination of Plutonium Isotopes in Environmental Samples Using Sequential Injection Extraction Chromatography and Detection by Inductively Coupled Plasma Mass Spectrometry

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

    2009-01-01

    This article presents an automated method for the rapid determination of 239Pu and 240Pu in various environmental samples. The analytical method involves the in-line separation of Pu isotopes using extraction chromatography (TEVA) implemented in a sequential injection (SI) network followed by det...

  20. Gamma-ray intensities of 239Pu

    Relative intensities of 239Pu γ-rays were precisely measured with a Ge(Li) detector which was accurately calibrated and corrections were made for self-absorption of γ-rays. Accuracies of 1-2% were obtained for strong γrays. Detector efficiences were calibrated with a standard source of 133Ba and γ-ray sources of 152Eu, 154Eu and 182Ta. Intensities per decay were determined by the measured γ-ray intensities, weight and isotopic abundance of plutonium in the source. (author)

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

    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. PMID:26476410

  2. Estimation of 240Pu Mass in a Waste Tank Using Ultra-Sensitive Detection of Radioactive Xenon Isotopes from Spontaneous Fission

    We report on a technique to detect and quantify the amount of 240Pu in a large tank used to store nuclear waste from plutonium production at the Hanford nuclear site. While the contents of this waste tank are known from previous grab sample measurements, our technique could allow for determination of the amount of 240Pu in the tank without costly sample retrieval and analysis of this highly radioactive material. This technique makes an assumption, which was confirmed, that 240Pu dominates the spontaneous fissions occurring in the tank.

  3. Transport process of Pu isotope in marginal seas of the western North Pacific Ocean

    Significant quantities of Pu isotopes have been released into the marine environment as the result of atmospheric nuclear weapons testing. Most radionuclides globally dispersed in atmospheric nuclear weapons testing were released into the environment during the 1950's and 1960's. In the western North Pacific Ocean, the principal source can be further distinguished as two distinct sources of Pu: close-in tropospheric fallout from nuclear weapons testing at the Pacific Proving Grounds (PPG) in the Marshall Islands and global stratospheric fallout. Since the 240Pu/239Pu atom ratio is characteristic for the Pu emission source, information on Pu isotopic signature is very useful to better understand the transport process in the oceans and to identify the sources of Pu. The mean atom ratio of 240Pu/239Pu from the global stratospheric fallout is 0.180 ±0.014 based on soil sample data, whereas that from close-in tropospheric fallout from the PPG is 0.33 - 0.36. The 240Pu/239Pu atom ratios in seawater samples collected in marginal seas of the western North Pacific Ocean will provide important and useful data for understanding the process controlling Pu transport and for distinguishing future Pu sources. The objectives of this study were to measure the 239+240Pu concentrations and 240Pu/239Pu atom ratios in seawater from the Sea of Okhotsk, Japan Sea, South China Sea and Sulu Sea and to discuss the transport process of Pu. Large-volume seawater samples (250 L each) were collected from the surface to the bottom in marginal seas of the western North Pacific Ocean with acoustically triggered quadruple PVC sampling bottles during the R/V Hakuho-Maru cruise. The 239Pu and 240Pu concentrations and 240Pu/239Pu 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. In the Sea of Okhotsk, the 239+240Pu concentration was 2.8 mBq m-3 in the surface water

  4. Fabrication of 12% {sup 240}Pu calorimetry standards

    Long, S.M.; Hildner, S.; Gutierrez, D.; Mills, C.; Garcia, W.; Gurule, C.

    1995-08-01

    Throughout the DOE complex, laboratories are performing calorimetric assays on items containing high burnup plutonium. These materials contain higher isotopic range and higher wattages than materials previously encountered in vault holdings. Currently, measurement control standards have been limited to utilizing 6% {sup 240}Pu standards. The lower isotopic and wattage value standards do not complement the measurement of the higher burnup material. Participants of the Calorimetry Exchange (CALEX) Program have identified the need for new calorimetric assay standards with a higher wattage and isotopic range. This paper describes the fabrication and verification measurements of the new CALEX standard containing 12% {sup 240}Pu oxide with a wattage of about 6 to 8 watts.

  5. 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

    A radioactivity measurement survey was carried out from 24 April 2008 to 3 June 2011 to determine the levels of plutonium isotopes and 240Pu/239Pu 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 241Am 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+240Pu 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+240Pu concentrations in surface waters. Higher 239+240Pu concentrations were found in bottom waters at deeper sampling locations, but the 240Pu/239Pu atom ratios were nearly constant regardless of the water depth. Higher 239+240Pu concentrations were also found in bottom sediments at deeper sampling locations, but vice versa for 240Pu/239Pu 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. - Highlights: • Pu concentration off the Japan coast before and after FDNPS accident was measured. • No regional differences were observed in 239+240Pu concentrations in surface waters. • 240Pu/239Pu atom ratios were also nearly identical in seawaters. • There were no significant

  6. Individual economical value of plutonium isotopes and analysis of the reprocessing of irradiated fuel

    An economical analysis of plutonium recycle in a PWR reactor, without any modification, is done, supposing an open market for the plutonium. The individual value of the plutonium isotopes is determined solving a system with four equations, which the unknow factors are the Pu-239, Pu-240, pu-241 and Pu-242 values. The equations are obtained equalizing the cost of plutonium fuel cycle of four different isotope mixture to the cost of the uranium fuel cycle. (E.G.)

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

    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

  8. Routine radiochemical method for the determination of 90Sr, 238Pu, 239+240Pu, 241Am and 244Cm in environmental samples

    Routine analytical procedures have been developed for the reliable simultaneous determination of 90Sr, 238Pu, 239+240Pu, 241Am and 242-244Cm, Chernobyl derived radioisotopes and fallout after nuclear weapon tests in a wide range of environmental samples: soil (100-200 g), sediments, aerosols, water and vegetation. This procedure has been applied to thousands of soil and sediment samples and hundreds of biological and water samples taken in the exclusive zone of Chernobyl NPP and different regions of Ukraine from 1989 to the present. After the sample has been properly prepared and isotopic tracers added, plutonium, americium and curium are precipitated with calcium oxalate and then lanthanum fluoride. Plutonium is separated from americium and curium by anion-exchange. Americium and curium are separated from rare earths by cation-exchange with gradient elute α-hydroxy-iso-butyric acid. During projects by AQCS IAEA 'Evaluation of Methods for 90Sr in a Mineral Matrix' and 'Proficiency Test for 239Pu, 241Pu and 241Am Measurement in a Mineral Matrix' accuracy and precision for 90Sr, 239Pu and 241Am by present procedure was evaluated. Advantages, difficulties and limitations of the method are discussed. (author)

  9. Origin and release date assessment of environmental plutonium by isotopic composition

    Varga, Zsolt [Hungarian Academy of Sciences, Radiation Safety Department, Institute of Isotopes, Budapest (Hungary)

    2007-10-15

    The origin and release date of environmental plutonium have been assessed by the measurement of plutonium and americium isotopic composition. The applicability and sensitivity of different plutonium isotope ratios, {sup 240}Pu/{sup 239}Pu and {sup 241}Pu/{sup 239}Pu measured by inductively coupled plasma sector field mass spectrometry and {sup 238}Pu/{sup 239}Pu analysed by alpha spectrometry, have been evaluated for origin determination in several types of environmental samples. With use of mixing models the contribution of different sources (e.g. global fallout or Chernobyl) can be calculated. By the measurement of the {sup 241}Am/{sup 241}Pu isotope ratio, the release date (i.e. formation of {sup 241}Pu by irradiation) can be estimated in environmental samples, which is an important parameter to distinguish recent plutonium release from previous (e.g. Chernobyl) emissions. (orig.)

  10. Origin and release date assessment of environmental plutonium by isotopic composition

    The origin and release date of environmental plutonium have been assessed by the measurement of plutonium and americium isotopic composition. The applicability and sensitivity of different plutonium isotope ratios, 240Pu/239Pu and 241Pu/239Pu measured by inductively coupled plasma sector field mass spectrometry and 238Pu/239Pu analysed by alpha spectrometry, have been evaluated for origin determination in several types of environmental samples. With use of mixing models the contribution of different sources (e.g. global fallout or Chernobyl) can be calculated. By the measurement of the 241Am/241Pu isotope ratio, the release date (i.e. formation of 241Pu by irradiation) can be estimated in environmental samples, which is an important parameter to distinguish recent plutonium release from previous (e.g. Chernobyl) emissions. (orig.)

  11. Transmutation of 239Pu with spallation neutrons

    Incineration studies of plutonium were carried out at the Synchrophasotron of the Joint Institute for Nuclear Research (JINR), Dubna, using proton beams with energies of 0.53 GeV and 1.0 GeV. Solid lead targets (8 cm in diameter and 20 cm long) were surrounded with 6 cm thick paraffin as neutron moderator and then irradiated. The transmutation of 239Pu and the associated production of fission products 91Sr, 92Sr, 97Zr, 99Mo, 103Ru, 105Ru, 129Sb, 132Te, 133I, 135I and 143Ce were studied in the present work. The plutonium samples (each 449 mg) were placed on the outer surface of moderator. For 1.0 GeV proton beam, the fission rate of 239Pu is 0.0032 atoms per proton in one gram plutonium samples, for 0.53 GeV proton this value is 0.0022. The experimental uncertainty is about 15%. The experiments are compared to two theoretical model calculations with moderate success, using the Dubna Cascade Model (CEM) and the LAHET code. The practical incineration rate of 239Pu is very high. For example: if one uses 10 mA, 1 GeV proton beams under the same (fictive) experimental conditions, the incineration rate of 239Pu via fission is 3 mg out of the 449 mg sample per day. For 0.53 GeV protons the corresponding rate is 2 mg per day. (author)

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

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

    2002-12-01

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

  13. Using 239+240Pu atmospheric deposition and a simplified mass-balance model to re-estimate the soil erosion rate. A case study of Liaodong Bay in China

    By using the mass balance model of 137Cs and introducing 239+240Pu atmospheric deposition, a simplified mass balance model of 239+240Pu was developed and the soil erosion rate was re-estimated. The results indicated that the reference inventory of 239+240Pu was estimated to be 88.4 Bq/m2 in Liaodong Bay. In addition, the atomic ratios of 240Pu/239Pu in all core samples were approximately 0.18, which indicated that the major source of Pu was the global fallout. Statistical analysis of the erosion rates derived from the model demonstrates that the 239+240Pu atmospheric deposition is a feasible way to estimate the soil erosion rate and further improve tracer technique to assess the soil erosion rate. (author)

  14. Isotope dilution alpha spectrometry for the determination of plutonium concentration in irradiated fuel dissolver solution : IDAS and R-IDAS

    The report presents a new technique, Isotope Dilution Alpha Spectrometry (IDAS) and Reverse Isotope Dilution Alpha Spectrometry (R-IDAS) for determining the concentration of plutonium in the irradiated fuel dissolver solution. The method exploits sup(238)Pu in IDAS and sup(239)Pu in R-IDAS as a spike and provides an alternative method to Isotope Dilution Mass Spectrometry (IDMS) which requires enriched sup(242)Pu as a spike. Depending upon the burn-up of the fuel, sup(238)Pu or sup(239)Pu is used as a spike to change the sup(238)Pu/(sup(239)Pu+sup(240)Pu)α activity ratio in the sample by a factor of 10. This change is determined by α-spectrometry on electrodeposited sources using a solid state silicon surface barrier detector coupled to a multichannel analyser. The validity of a simple method based on the geometric progression (G.P.) decrease for the far tail of the spectrum to correct for the tail contribution of sup(238)Pu peak (5.50 MeV) to the low energy sup(239)Pu + sup(240)Pu peak (5.17 MeV) is established. Results for the plutonium concentration on different irradiated fuel dissolver solutions with burn-uo ranging from J,000 to 100,000 MWD/TU are presented and compared with those obtained by IDMS. The values obtained by IDAS or R-IDAS and IDMS agree within 0.5%. (auth.)

  15. Evaluation of 239+240Pu, 137Cs and natural 210Pb fallout in agricultural upland fields in Rokkasho, Japan

    The background distributions of 239+240Pu and 137Cs fallout in agricultural soil were investigated in Rokkasho where Japan's first commercial nuclear fuel reprocessing plant is now being constructed. The mean inventories of 239+240Pu and 137Cs in three fields with non-yam-cultivation history were 116 Bq x m-2 and 3.4 kBq x m-2, respectively. The mean atomic ratio of 240Pu/239Pu for all studied fields was 0.18±0.04, and was similar to that of global fallout. The 239+240Pu concentrations correlated very well with 137Cs (r = 0.97) in spite of heavy disturbance of the soil, and the activity ratio of 239+240Pu/137Cs was 0.037 ± 0.007, which is a typical value for global fallout. These results showed that the nuclides had similar behavior in agricultural upland fields in Rokkasho. Since 210Pb is steadily deposited from the atmosphere to the land, this nuclide could be an index for the degree of disturbance of a field and of soil lost from the field. The ratio of excess 210Pb inventory in the soil to the equivalent inventory of atmospheric 210Pb deposition was 96%, and indicated that soil was not lost from the cultivated fields. (author)

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

    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. 105. 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

  17. Background distributions of 239+240Pu and 137Cs of upland soil in Rokkasho, Japan

    The background distributions of Pu and 137Cs in soil were investigated in Rokkasho, Aomori Prefecture, where the first commercial nuclear fuel reprocessing plant in Japan is now being constructed. Soil core samples to 1 m depth were collected at 13 upland fields in Rokkasho and control sites in Hachinohe and Hirosaki. Since fields under yam (Dioscorea babatus) cultivation, which is a common crop in Rokkasho, were dug to approximately 1 m depth at harvesting, depth profiles of fallout radionuclides are heavily disturbed for most fields in Rokkasho. The mean inventories of 239+240Pu and 137Cs in three fields with no yam cultivation history were 116 Bq m-2 and 3.4 kBq m-2, respectively and similar to values in Hachinohe. However, the inventories were approximately a half of those in Hirosaki. The mean ratio of 239Pu/240Pu for all studied fields was 0.18±0.04, and similar to that of global fallout. The Pu concentrations correlate very well with 137Cs (r=0.97) in spite of heavy disturbance of soil, and the ratio of 239+240Pu/137Cs was 0.037±0.007, which is a typical value for global fallout. (author)

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

    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

  19. Identification of the contamination source of plutonium in environmental samples with isotopic ratios determined by inductively coupled plasma mass spectrometry and alpha-spectrometry

    Concentrations of 239+249Pu in environmental samples were determined by ICP-MS and α spectrometry, showing consistent results, which suggests an applicability of ICP-MS to 239Pu and 240Pu measurement. The activity ratios of 238Pu/239+240Pu and 240Pu/239Pu were significantly different in samples from the general environment and near Sellafield reprocessing plants, indicating the usefulness of these ratios for identification of the Pu contamination source. (author)

  20. Adsorption behavior of 239Pu by Gaomiaozi bentonite

    Adsorption behavior of 239Pu by Gaomiaozi bentonite as a function of the factors of aqueous phase pH value, 239Pu initial concentration and ionic species is studied by static adsorption experiments in this paper. The following results are obtained. Adsorption equilibrium time of 239Pu by Gaomiaozi bentonite samples is about 24 h, and the adsorption distribution ratio Kd value of 239Pu increases with the pH value, but decreases with increasing initial concentration of 239Pu. And adsorption of 239Pu by bentonite samples with different ionic species show that anions affect the most on adsorption of bentonite is CO32-, followed by HCO3- and SO42-, whereas Cl- and NO3- hardly have any influence on the adsorption of bentonite. (authors)

  1. Random Probability Analysis of 48Ca +239Pu Experimental Data

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

    2014-09-01

    Element 114 (Fl), was discovered at the Flerov Laboratory of Nuclear Reactions (FLNR) using the 48Ca +244Pu reaction and the Dubna Gas-Filled Recoil Separator (DGFRS). The structural properties of the super heavy elements are still largely unknown. The extent of the region of enhanced stability near Z = 114 and N = 184 is not completely known. To examine these properties, a new experimental data set has been taken using the 48Ca +239Pu reaction at the DGFRS, in an effort to look for lighter isotopes of Fl. Progress on the production of lighter isotopes of Fl, cross-section measurements, and any nuclear decay properties will be discussed. Comparisons with reactions using heavier 242,244Pu targets and Monte Carlo random probability analysis will be highlighted. Element 114 (Fl), was discovered at the Flerov Laboratory of Nuclear Reactions (FLNR) using the 48Ca +244Pu reaction and the Dubna Gas-Filled Recoil Separator (DGFRS). The structural properties of the super heavy elements are still largely unknown. The extent of the region of enhanced stability near Z = 114 and N = 184 is not completely known. To examine these properties, a new experimental data set has been taken using the 48Ca +239Pu reaction at the DGFRS, in an effort to look for lighter isotopes of Fl. Progress on the production of lighter isotopes of Fl, cross-section measurements, and any nuclear decay properties will be discussed. Comparisons with reactions using heavier 242,244Pu targets and Monte Carlo random probability analysis will be highlighted. This work was performed under Contract DE-AC52-07NA27344 and Grant DE-NA0002135.

  2. An intercomparison experiment on isotope dilution thermal ionisation mass spectrometry using plutonium-239 spike for the determination of plutonium concentration in dissolver solution of irradiated fuel

    Determination of plutonium concentration in the dissolver solution of irradiated fuel is one of the key measurements in the nuclear fuel cycle. This report presents the results of an intercomparison experiment performed between Fuel Chemistry Division (FCD) at BARC and PREFRE, Tarapur for determining plutonium concentration in dissolver solution of irradiated fuel using 239Pu spike in isotope dilution thermal ionisation mass spectrometry (ID-TIMS). The 239Pu spike method was previously established at FCD as viable alternative to the imported enriched 242Pu or 244Pu; the spike used internationally for plutonium concentration determination by IDMS in dissolver solution of irradiated fuel. Precision and accuracy achievable for determining plutonium concentration are compared under the laboratory and the plant conditions using 239Pu spike in IDMS. For this purpose, two different dissolver solutions with 240Pu/239Pu atom ratios of about 0.3 and 0.07 corresponding, respectively, to high and low burn-up fuels, were used. The results of the intercomparison experiment demonstrate that there is no difference in the precision values obtained under the laboratory and the plant conditions; with mean precision values of better than 0.2%. Further, the plutonium concentration values determined by the two laboratories agreed within 0.3%. This exercise, therefore, demonstrates that ID-TIMS method using 239Pu spike can be used for determining plutonium concentration in dissolver solution of irradiated fuel, under the plant conditions. 7 refs., 8 tabs

  3. Fission of 239Pu with resonance neutrons

    A measurement of fission fragment energy and mass distributions in the 239Pu(n,f) resolved resonance region has been performed applying the twin Frisch-gridded ionization chamber technique. An improved pile-up rejection system has been developed to cope with the strong α background. The results for the mass and mean total kinetic energy (TKE-bar) distributions for resolved resonances do not show any strong 'pattern' of fluctuations, unlike it was the case for 235U(n,f) in the same neutron energy region. This can be explained in the frame of existing theoretical models, according to which the only possible low-energy spin states available (Jπ=0+, 1+) belong to two well separated (∼1.25 MeV) transition state bands with given fission fragment properties. An anti-correlation between TKE-bar and ν-barp was found to be not significant. The obtained small spin dependence of TKE-bar of about 70 keV is in agreement with literature values. A slight correlation was found between TKE-bar versus 1/Γf. But also this was considered not to be significant. (author)

  4. Evaluation both level and 239+240Pu spatial contamination of the Lira object and the neighbouring areas

    In the work the generalization of considerable data collection for revealing of 239+240Pu content range discriminative for Lira object and neighbouring areas is carried out. 239+240Pu mean specific activity in the soil cover surface and in the Berezovka River bottom sedimentations are determined. The correlation dependence between 239+240Pu artificial radionuclides and 137Cs is revealed. The general source of artificial radionuclide origination for examined isotopes is shown up, and it is related with global radioactive fallout

  5. Biosorption of 239Pu by immobilized sargassum fusiforme

    Sargassum fusiforme was immobilized with calcium alginates and its biosorption property to 239Pu was studied by batch and column methods. Biosorption equilibrium time of immobilized Sargassum fusiforme biosorbent to 239Pu is 120 min and biosorption efficiency is over 99.2% when the initial concentration of 239Pu is 21.5 kBq/L and pH is 2.5-5.0. After five times repetition biosorption-desorption cycles biosorption efficiency is still over 98.0% when the velocity of flow is 2 ml/min in column experiment. Immobilized Sargassum fusiforme biosorbent is better to 239Pu due to its better chemical stability, mechanical strength, lower cost, high biosorption efficiency and repeated biosorption-desorption cycles. (authors)

  6. Effects of monomeric 239Pu on the pregnant rabbit

    The effects of 239Pu treatment (0, 10 or 40 μCi/kg) on hematological measurements in pregnant rabbits were studied at 29 days of gestation. Mean clotting times were significantly increased in all plutonium-treated rabbits. There was also a significant increase in clotting time with increasing time between plutonium dosing and sample collection in rabbits injected with 10 μCi/kg. Platelet counts were significantly decreased in all rabbits exposed to 239Pu for 14 days or greater. Hematocrits were significantly depressed in rabbits exposed to 239Pu for 20 days. It is speculated that monomeric 239Pu accumulates at a hematopoietic site close to that affected in X-irradiated animals. (U.K.)

  7. Comparative analysis of spent fuel isotope composition for VVER-440 compare to VVER-1000 reactors

    Calculations were made for reactor cell of fuel assemblies for VVER-440 and VVER-1000 depending on their manufactory and operation conditions. These cells were composed of the fuel assemblies with the maximum multiplying purpose (enrichment of 4.4% for both reactor types). Concentration as function of burnup of ten most usable isotopes, such as main fuel isotopes U235, U236, U238, Pu239, Pu240, Pu241, as well as some actinides, and fission products, such as Pu242, Am241, Sm149, Sm151 was analyzed

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

    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.

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

    A novel reaction pathway for production of 240Am is reported. Models of reaction cross-sections in EMPIRE II suggest 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 5.6 ± 0.2 mbarn. We discuss reasons for the discrepancy as well as production of other Am isotopes that contaminate the final product

  10. Microlocalization of 239Pu in structural elements of the interalveolar septa after inhalation of its various compounds and pentacin

    A quantitative and qualitative evaluation of 239 Pu mictodistribution in the structural elements of the interalveolar septa after inhalation of three plutonium compounds different in solubility is made. Thirty minutes after the inhalation 55.3-85.3% of plutonium (dioxide>nitrate>=citrate) was revealed in rhe cells, predominantly in the microphages. More than half of the isotope found in the noncellular elements, lies in the surface layer of the alveoli and the intercellular matter. First 239Pu is seen as ''stars'' of tracks (dioxide), mainly (nitrate) or exclusively (citrate) as individual tracks. The different extent of plutonium elimination from the interalveolar septa (dioxide239Pu from the cells is mainly determined by its escape from the macrophages (dioxide) or from all cellular elements (nitrate, citrate). Pentacin accelates elimination of plutonium from the most of the structural elements of the interalveolar septa (citrate>nitrate)

  11. Microscopic Calculations of 240Pu Fission

    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.

  12. First AID (Atom counting for Isotopic Determination).

    Roach, J. L. (Jeffrey L.); Israel, K. M. (Kimberly M.); Steiner, R. E. (Robert E.); Duffy, C. J. (Clarence J.); Roench, F. R. (Fred 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.

  13. Biological effects in intramuscular 239Pu administration during chelatotherapy

    Durable (up to 64 days) application of complexones (Ca and Zn DTPA) in the case of intramuscular administration of 239Pu large amounts in rats is studied. The results of studying the biological effect proving considerable decrease of the average lifespan of rats are given

  14. Strain differences in the embryotoxicity of 239Pu

    Comparison of the embryolethality of monomeric 239Pu injected at 9 days of gestation demonstrated that the sensitivity of Charles River CD strain was greater than that of Hilltop Wistar rats. Subsequent comparisons showed that rats derived from the Hilltop Fischer strain were more sensitive than the Wistar and, although not directly compared, more sensitive than the CD

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

    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.

  16. Performance of isotope correlations for the estimate of 242Pu

    Full text: The lack of a gamma-ray signature from 242Pu represents an Achilles heel for many plutonium isotope abundance measurements made by high-resolution gamma spectrometry (HRGS). This holds in particular for plutonium materials containing a significant fraction of this isotope. The problem is partially solved through the application of isotope correlations estimating the relative abundance of 242Pu from relations to ratios of other plutonium isotopes measurable by HRGS. In the mid of the nineties a new type of isotope correlation had been proposed for LWR plutonium based on the following relation: 242Pu/239Pu = C0·[238Pu/239Pu]c1 · [240Pu/239Pu]c2 with recommended coefficients C0, C1 and C2 for PWR and BWR fuels, respectively. We have adopted this type of correlation for the routine analysis of safeguards samples in the Euratom On-Site Laboratories and in the Institute for Transuranium Elements. In order to cover the full range of plutonium materials received for analysis, the application of the above correlation has been also extended to AGR and Magnox-type of plutonium. The differing sets of coefficients C0, C1 and C2 approximating best the correlation for the additional types of materials were determined from a set of reference isotopic data. Since in many instances the origin and the type of the plutonium are not known a priori, criteria for categorization were established helping to select the appropriate isotope correlation. Parametric plots of the ratios 238Pu/239Pu versus 240Pu/239Pu generally allow to discern unambiguously Magnox, AGR and LWR plutonium, and to some extent also BWR and PWR plutonium, as long as a mixing of the respective plutonium materials has not occurred. With this kind of categorization implemented in the routine analysis the performance of the 242Pu estimate is substantially improving in most cases. Performance data for 242Pu in particular, and for plutonium isotope abundance measurements by HRGS in general, as derived from a

  17. Subcellular binding of 239Pu in the liver of selected species of rodents

    The subcellular distribution of 239Pu in the liver of selected rodent species was investigated as well as the relation between 239Pu and the iron metabolism. The goal of the investigation was to find out why the liver discharge of 239Pu from the liver varies so much between species. (orig.)

  18. Preliminary Study on the Determination of ~(235)U and ~(239)Pu Using Delayed Neutron Counting Method

    2011-01-01

    The preliminary study on the fast measurements of 235U and 239Pu in samples containing 235U, 239Pu and 235U-239Pu mixture using delayed neutron counting method is introduced. All samples were irradiated for 30 s using the 30 kW Miniature Neutron

  19. Role of protracted exposure on the toxicology of inhaled 239PuO2

    Studies were initiated to examine in rats the effects of a protracted exposure to inhaled 239PuO2. Graphs are presented to show effect of multiple exposures to 239PuO2 on the deposition and clearance of 239Pu in the alveoli

  20. Inhaled 239PuO2 in rats with pulmonary emphysema

    The modifying effects of a pre-existing lung disease (emphysema) on the deposition, distribution, retention, and effects of inhaled 239PuO2 in the rat are being investigated. Preliminary observations indicated that the deposition and retention patterns for 239Pu particles inhaled by rats with emphysema and control rats were similar, but the distribution of inhaled 239Pu immediately after exposure was different. Respiratory function measured through one year after exposure to 239Pu was consistent with emphysema and was not altered by the 239Pu lung burden. Long-term observations are continuing. 4 references, 2 tables

  1. Metabolic pathways of 239Pu immediately after administration

    239Pu chloride was given to male rats intravenously or by the oral route. The early stages of the Pu metabolism are characterized by a fast distribution in liver and skeleton and a high concentration in the intestine and the muscle tissue. The rate of elimination from the liver and muscles was the same for both types of application. With injection into different parts of the vascular system, the binding to protein and other tissue components was identical. 239Pu is practically not absorbed from the gastrointestinal tract if given perorally. The absorbed fraction had an osteotropic character, i.e. the plutonium was bound to the organic as well as to the mineral fraction. When Pu chloride is injected intravenously, there is a slow redistribution from the characteristic hepatotropic to the osteotropic type. The function of the liver as a barrier against the plutonium is not very prominent and seems to depend on the type of compound given. (MG/AK)

  2. Distribution of Pu isotopes and 137Cs in and around the former soviet union's Semipalatinsk nuclear test site

    This paper is a report on our survey of residual radioactivity, Pu isotopes and 137Cs, within and without the territory of the Semipalatinsk nuclear test site. Soil samples within the test site were collected at approximately 30 sites along the roads connecting Kurchatov City, ground zero for the first USSR nuclear test, Balapan, Degelen Mountain and Salzhal settlement. Furthermore, outside the test site, the soil was sampled at about 20 sites, including some settlements (Mostik, Dolon, Tchagan, etc.), forest and pasture areas, along the roads from Semipalatinsk City to Kurchatov City and north Korosteli settlement. The contamination levels of long-lived radionuclides, 137Cs, 238Pu and 239,240Pu as well as 240Pu/239Pu atomic ratio in the soil were determined by non-destructive γ-spectrometric method and radiochemical separation followed by α-spectrometric and/or ICP-MS methods, respectively. The results showed that although 137Cs was within typical environmental levels except for an areas near ground zero and Balapan, 239,240Pu was elevated levels contaminated with weapons-grade plutonium in all area we visited. From the stepwise leaching of Pu from the soil, 50-80% of total 239,240Pu in most samples was found to be tightly incorporated into the soil components which might have been melted at time of detonation. (author)

  3. Further development of IDGS: Isotope dilution gamma-ray spectrometry

    The isotope dilution gamma-ray spectrometry (IDGS) technique for determining the plutonium concentration and isotopic composition of highly radioactive spent-fuel dissolver solutions has been further developed. Both the sample preparation and the analysis have been improved. The plutonium isotopic analysis is based on high-resolution, low-energy gamma-ray spectrometry. The plutonium concentration in the dissolver solutions then is calculated from the measured isotopic differences among the spike, the dissolver solution, and the spiked dissolver solution. Plutonium concentrations and isotopic compositions of dissolver solutions analyzed from this study agree well with those obtained by traditional isotope dilution mass spectrometry (IDMS) and are consistent with the first IDGS experimental result. With the current detector efficiency, sample size, and a 100-min count time, the estimated precision is ∼0.5% for 239Pu and 240Pu isotopic analyses and ∼1% for the plutonium concentration analysis. 5 refs., 2 figs., 7 tabs

  4. Latitudinal distribution and sedimentation of 90Sr, 137Cs, 241Am and 239,240Pu in bottom sediment of the Northwest Pacific Ocean

    As a part of the Worldwide Marine Radioactivity Studies (WOMARS) of the International Atomic Energy Agency's Marine Environment Laboratory (IAEA-MEL) in Monaco, bottom sediment samples were collected along with water column samples in 1997 from the Northwest Pacific Ocean, and were analysed for 90Sr, 137Cs, 239,240Pu and 241Am contents in order to identify current distribution patterns and inventories, and to elucidate sources of these radionuclides in the region where the past US nuclear weapons tests were carried out. This study complements a previous reports on bottom sediments and water column. All the reported sediment data including data from 1997 cruise revealed that sedimentary 239+240Pu and 241Am concentrations peaked both in the latitudinal bands between 10-20 deg. N and 30-40 deg. N, and 137Cs and 90Sr in the latitudinal band between 30-40 deg. N. The latitudinal bands between 10-20 deg. N and 30-40 deg. N correspond to the major areas affected by close-in fallout and global fallout, respectively. Sediment inventories of 239,240Pu and 241Am exceeded or nearly equalled their overlying water inventories near the Bikini Atoll, however, in mid latitudes, more than 70% of 239,240Pu still remains in the water column. Sediment inventories of 137Cs and 90Sr account for about ten and less than five percent of the water column inventories, respectively. 241Am inventories in sediments exceeded those of the water column. The activity ratios of 137Cs/90Sr and 241Am/239,240Pu in sediments were higher than of the global fallout ratios. 90Sr content in the bottom sediments also appears to be controlled by the carbonate contents of the sea floor. The relative contribution of global and close-in fallouts to the total 239,240Pu was estimated using a two end-member mixing model based on the atom ratios of 240Pu/239Pu. The contribution of close-in fallout in sediment appears to be about 56 % for the latitudinal belt 10-20 deg. N. It is not unexpected that close-in fallout Pu

  5. Latitudinal distribution and sedimentation of 90Sr, 137Cs, 241Am and 239,240Pu in bottom sediment of the Northwest Pacific Ocean

    As a part of the Worldwide Marine Radioactivity Studies (WOMARS) of the International Atomic Energy Agency's Marine Environment Laboratory (IAEA-MEL) in Monaco, bottom sediment samples were collected along with water column samples in 1997 from the Northwest Pacific Ocean, and were analysed for 90Sr, 137Cs, 239,240Pu and 241Am contents in order to identify current distribution patterns and inventories, and to elucidate sources of these radionuclides in the region where the past US nuclear weapons tests were carried out. This study complements a previous reports on bottom sediments and water column. All the reported sediment data including data from 1997 cruise revealed that sedimentary 239+240Pu and 241Am concentrations peaked both in the latitudinal bands between 10-20 deg. N and 30-40 deg. N, and 137Cs and 90Sr in the latitudinal band between 30-40 deg. N. The latitudinal bands between 10-20 deg N and 30-40 deg. N correspond to the major areas affected by close-in fallout and global fallout, respectively. Sediment inventories of 239+240Pu and 241Am exceeded or nearly equalled their overlying water inventories near the Bikini Atoll, however, in mid latitudes, more than 70% of 239+240Pu still remains in the water column. Sediment inventories of 137Cs and 90Sr account for about ten and less than five percent of the water column inventories, respectively. 241Am inventories in sediments exceeded those of the water column. The activity ratios of 137Cs/90Sr and 241Am/239,240Pu in sediments were higher than of the global fallout ratios. 90Sr content in the bottom sediments also appears to be controlled by the carbonate contents of the sea floor. The relative contribution of global and close-in fallouts to the total 239,240Pu was estimated using a two end-member mixing model based on the atom ratios of 240Pu/239Pu. The contribution of close-in fallout in sediment appears to be about 56 % for the latitudinal belt 10-20 deg. N. It is not unexpected that close-in fallout Pu

  6. 239PU(N, f) at Resonance Energies and its Multi-Modal Interpretation

    Hambsch, F.-J.; Bax, H.; Ruskov, I.; Demattè, L.

    2003-10-01

    A measurement of fission fragment total kinetic energy (TKE) and mass yield distributions Y (A,TKE) in the 239Pu(n,f) resolved resonance region has been performed applying the twin Frisch gridded ionization chamber technique. Special emphasis was devoted to cope with the strong α-activity of this isotope by an improved pile-up rejection system. Up to about 200 eV all fission resonances could be resolved and their two-dimensional mass yield and TKE distribution, Y(A,TKE), measured. Compared to the results on 235U(n,f), much smaller fluctuations of the fission fragment mass and TKE have been observed in the case of 239Pu. From a physical point of view such fluctuations have been expected for the fission fragment properties, because the only possible lowenergy spin states (Jπ=0+,1+) belong to well separated (about 1.25 MeV) transition state bands. Hence, it was expected to observe differences in the fission fragment mass and TKE distributions between spin 0+ and 1+ resonances. However, no spin dependence and only a slight anti-correlation of the TKE with the prompt neutron multiplicity, νp. has been found in the resolved resonance energy region above 1 eV. Within the multi-modal random neck-rupture (MM-RNR) model the Y(A,TKE) distributions have been fitted assuming three fission modes, two asymmetric and one symmetric one. The branching ratio of the two asymmetric modes shows similar fluctuations as the experimental TKE. Recently, a new theoretical approach has given a solution to the absence of pronounced fluctuations of the fission properties in the case of 239Pu. Since only one transition state is involved in the fission of 0+ and 1+ resonances with a given fission fragment distribution, no fluctuations are expected.

  7. Modeling and production of {sup 240}Am by deuteron-induced activation of a {sup 240}Pu target

    Finn, Erin C., E-mail: Erin.Finn@pnnl.gov; McNamara, Bruce, E-mail: Bruce.McNamara@pnnl.gov; Greenwood, Larry, E-mail: Larry.Greenwood@pnnl.gov; Wittman, Richard, E-mail: Richard.Wittman@pnnl.gov; Soderquist, Charles, E-mail: Chuck.Soderquist@pnnl.gov; Woods, Vincent, E-mail: Vincent.Woods@pnnl.gov; VanDevender, Brent, E-mail: Brent.Vandevender@pnnl.gov; Metz, Lori, E-mail: Lori.Metz@pnnl.gov; Friese, Judah, E-mail: Judah.Friese@pnnl.gov

    2015-04-15

    A novel reaction pathway for production of {sup 240}Am is reported. Models of reaction cross-sections in EMPIRE II suggest that deuteron-induced activation of a {sup 240}Pu target produces maximum yields of {sup 240}Am from 11.5 MeV incident deuterons. This activation had not been previously reported in the literature. A {sup 240}Pu target was activated under the modeled optimum conditions to produce {sup 240}Am. The modeled cross-section for the {sup 240}Pu(d, 2n){sup 240}Am reaction is on the order of 20–30 mbarn, but the experimentally estimated value is 5.6 ± 0.2 mbarn. We discuss reasons for the discrepancy as well as production of other Am isotopes that contaminate the final product.

  8. Distribution of Pu isotopes and {sup 137}Cs in and around the former soviet union`s Semipalatinsk nuclear test site

    Yamamoto, Masayoshi [Kanazawa Univ., Tatsunokuchi, Ishikawa (Japan). Low Level Radioactivity Laboratory; Hoshi, Masaharu; Takada, Jun; Tsukatani, Tsuneo; Sekerbaev, A.Kh.; Busev, B.I.

    1999-03-01

    This paper is a report on our survey of residual radioactivity, Pu isotopes and {sup 137}Cs, within and without the territory of the Semipalatinsk nuclear test site. Soil samples within the test site were collected at approximately 30 sites along the roads connecting Kurchatov City, ground zero for the first USSR nuclear test, Balapan, Degelen Mountain and Salzhal settlement. Furthermore, outside the test site, the soil was sampled at about 20 sites, including some settlements (Mostik, Dolon, Tchagan, etc.), forest and pasture areas, along the roads from Semipalatinsk City to Kurchatov City and north Korosteli settlement. The contamination levels of long-lived radionuclides, {sup 137}Cs, {sup 238}Pu and {sup 239,240}Pu as well as {sup 240}Pu/{sup 239}Pu atomic ratio in the soil were determined by non-destructive {gamma}-spectrometric method and radiochemical separation followed by {alpha}-spectrometric and/or ICP-MS methods, respectively. The results showed that although {sup 137}Cs was within typical environmental levels except for an areas near ground zero and Balapan, {sup 239,240}Pu was elevated levels contaminated with weapons-grade plutonium in all area we visited. From the stepwise leaching of Pu from the soil, 50-80% of total {sup 239,240}Pu in most samples was found to be tightly incorporated into the soil components which might have been melted at time of detonation. (author)

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

    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.

  10. Vertical distributions of plutonium isotopes in marine sediment cores off the Fukushima coast after the Fukushima Dai-ichi Nuclear Power Plant accident

    W. T. Bu

    2013-04-01

    Full Text Available The Fukushima Dai-ichi Nuclear Power Plant (FDNPP accident led to the release of large amounts of radionuclides into the atmosphere as well as direct discharges into the sea. In contrast to the intensive studies on the distribution of the released high volatility fission products, such as 131I, 134Cs and 137Cs, similar studies of the actinides, especially the Pu isotopes, are limited. To obtain the vertical distribution of Pu isotopes in marine sediments and to better assess the possible contamination of Pu from the FDNPP accident in the marine environment, we determined the activities of 239+240Pu and 241Pu as well as the atom ratios of 240Pu/239Pu and 241Pu/239Pu in sediment core samples collected in the western North Pacific off Fukushima from July 2011 to July 2012. We also measured surface sediment samples collected from seven Japanese estuaries before the FNDPP accident to establish the comprehensive background baseline data. The observed results of both the Pu activities and the Pu atom ratios for the sediments in the western North Pacific were comparable to the baseline data, suggesting that the FDNPP accident did not cause detectable Pu contamination to the studied regions prior to the sampling time. The Pu isotopes in the western North Pacific 30 km off the Fukushima coast originated from global fallout and Pacific Proving Ground close-in fallout.

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

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

    2015-10-01

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

  12. Neutron Resonance Parameters and Covariance Matrix of 239Pu

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

    2008-08-01

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

  13. Low level 239PuO2 life-span studies

    The purpose of this projet is to determine the dose-response curve for lung-tumor incidence in rats following inhalation of 239PuO2 at levels producing a lifespan radiation dose of 2 to 100 rad. In preliminary studies, rats were intratracheally instilled with, or inhaled 169Yb-239PuO2 or 169Yb-Yb2O3 particles. Whole-body, excreta and tissue levels of 169Yb were determined by external gamma counting; 239Pu levels were determined radiochemically by scintillation counting. It was found that 169Yb dissociated from 239PuO2 and was cleared more rapidly from the lung and the whole body. Despite this fact, however, whole-body counts performed at 7 days after exposure to 169Yb-239PuO2 gave a reproducible measure of the 239Pu lung burden

  14. Characterization of a neutron source of 239PuBe

    The spectrum equivalent dose and environmental equivalent dose f a 239PuBe source have been determined. The appropriate handling of a neutron source depends on the knowledge of its characteristics, such as its energy distribution, total rate of flowing and dosimetric magnitudes. In many facilities have not spectrometer that allows to determine the spectrum and then area monitors are used that give a dosimetric magnitude starting from measuring the flowing rate and the use of conversion factors, however this procedure has many limitations and it is preferable to measure the spectra and starting from this information the interest dosimetric magnitudes are calculated. In this work a Bonner sphere spectrometer has been used with a 6LiI(Eu) scintillator obtaining the count rates that produce, to a distance of 100 cm, a 239PuBe source of 1.85E(11) Bq. The spectrum was reconstructed starting from the count rates using BUNKIUT code and response matrix UTA4. With the spectrum information was calculated the source intensity, total flow, energy average, equivalent dose rate, environmental equivalent dose rate, equivalent dose coefficient and environmental equivalent dose coefficient. By means of two area monitors for neutrons, Eberline ASP-1 and LB 6411 of Berthold the equivalent dose and environmental equivalent dose were measured. The determinate values were compared with those reported in literature and it found that are coincident inside 17%. (Author)

  15. Decommissioning of a 239Pu contaminated incinerator facility

    In early 1978, a plutonium contaminated incinerator facility at the Los Alamos Scientific Laboratory (LASL), Los Alamos, New Mexico, was decommissioned. The project involved dismantling the facility and disposal by burial or by retrievable storage of the debri at an on-site waste disposal area. Contaminated soil from the 0.5 hectare area was buried. The facility was constructed in 1951 to incinerate plutonium contaminated wastes. It was later used as a decontamination facility. The major features included a 185 m2 control building, incinerator, cyclone dust collector, spray cooler, venturi scrubber, air filter bank, ash separator, and two 140,000 litres ash storage tanks. Preliminary soil contamination surveys were performed by a LASL developed portable phoswich detector system. Final soil contamination levels were measured with a zinc sulphide gross alpha scintillation system. Six hundred cubic metres of debris and 1200 m3 of soil contaminated with less than 10 nCi 239 Pu/g were buried at the LASL disposal area. Five cubic metres of 239 Pu contaminated ash residues were packed and stored to meet the Department of Energy's 20 year retrievable storage criteria. (author)

  16. Evaluation of neutron nuclear data for 240Pu

    Based on the experimental data evaluation and theoretical calculation, a complete set of neutron nuclear data for 240Pu has been recommended in the incident neutron energy range from 10-5 eV to 20 MeV for CENDL-2. The comparison of present evaluation with ENDF/B-6 and JENDL-3 has been carried out

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

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

    2015-02-01

    This work presents the findings of a long-term plutonium (Pu) study at Savannah River Site (SRS) conducted between 2003 and 2013. Terrestrial environmental samples were obtained at the Savannah River National Laboratory (SRNL) in the A-Area. Plutonium content and isotopic abundances were measured over this time period by α particle and thermal ionization mass spectrometry (3STIMS). We detail the complete process of the sample collection, radiochemical separation, and measurement procedure specifically targeted to trace plutonium in bulk environmental samples. Total plutonium activities were determined to be not significantly above atmospheric global fallout. However, the (238)Pu/(239+240)Pu activity ratios attributed to SRS are substantially different than fallout due to past (238)Pu production on the site. The (240)Pu/(239)Pu atom ratios are reasonably consistent from year to year and are lower than fallout indicating an admixture of weapons-grade material, while the (242)Pu/(239)Pu atom ratios are higher than fallout values, again due to actinide production activities. Overall, the plutonium signatures obtained in this study reflect a distinctive mixture of weapons-grade, heat source, and higher burn-up plutonium with fallout material. This study provides a unique opportunity for developing and demonstrating a blue print for long-term low-level monitoring of trace plutonium in the environment. PMID:25535652

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

    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.

  19. Artificial radioactivity and marine environment. Study of 238Pu, 239Pu+240Pu, 241Pu and 241Am in the Mediterranean sea

    This paper is in two parts. Part one is about the methods for analyzing transuranium elements particularly the development of an analytical process for plutonium and for perfecting an Americium analyzing method, capable of treating samples of 200 litres of sea water, 100 grams of sediment and 100 grams of biological matter. Part two concerns the in situ determinations carried out within the scope of the study on the distribution and behaviour of transuranium elements in the Mediterranean sea. The high sea studies concerned the effects of atmospheric fall out and the vertical distribution of Pu and Am. Studies along the coasts enabled a quantitative study to be made of the contribution of rivers to the Mediterranean and to study the distribution of Pu along the French Mediterranean coast line

  20. Chronology of Pu isotopes and {sup 236}U in an Arctic ice core

    Wendel, C.C., E-mail: cato.wendel@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Oughton, D.H., E-mail: deborah.oughton@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Lind, O.C., E-mail: ole-christian.lind@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Skipperud, L., E-mail: lindis.skipperud@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Fifield, L.K., E-mail: keith.fifield@anu.edu.au [Department of Nuclear Physics, Australian National University, Canberra ACT 0200 (Australia); Isaksson, E., E-mail: elisabeth.isaksson@npolar.no [Norwegian Polar Institute, Fram Centre, Hjalmar Johansens Gate 14, N9296 Tromsø (Norway); Tims, S.G., E-mail: steve.tims@anu.edu.au [Department of Nuclear Physics, Australian National University, Canberra ACT 0200 (Australia); Salbu, B., E-mail: brit.salbu@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway)

    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 {sup 236}U, {sup 239}Pu, and {sup 240}Pu concentrations, and atom ratios, measured by accelerator mass spectrometry in a 28.6 m 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 {sup 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 {sup 239+240}Pu ranged from 0.008 to 0.254 mBq cm{sup −2} and {sup 236}U from 0.0039 to 0.053 μBq cm{sup −2}. Concentrations varied in concordance with {sup 137}Cs concentrations in the same ice core. In contrast to previous published results, the concentrations of Pu and {sup 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 {sup 240}Pu/{sup 239}Pu ratio ranged from 0.15 to 0.19, and {sup 236}U/{sup 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 {sup 236}U concentrations and {sup 236}U/{sup 239}Pu atom ratios in the Arctic and in ice cores. - Highlights: • Concentrations and atom ratios of Pu and {sup 236}U determined in an Arctic ice core. • Concentrations of U and Pu found to be higher pre- than post-moratorium. • U and Pu concentrations

  1. The self-absorption effect of gamma rays in 239Pu

    Nuclear materials assay with gamma-ray spectrum measurement is a well-established method for safeguards. However, for a thick source, the self-absorption of characteristic low-energy gamma rays has been a handicap to accurate assay. The author has carried out Monte Carlo simulations to study this effect using the 239Pu α-decay gamma-ray spectrum as an example. The thickness of a plutonium metal source can be considered a function of gamma-ray intensity ratios. In a practical application, gamma-ray intensity ratios can be obtained from a measured spectrum. With the help of calculated curves, scientists can find the source thickness and make corrections to gamma-ray intensities, which then lead to an accurate quantitative determination of radioactive isotopes in the material

  2. Multilevel analysis of the low energy 239Pu cross sections

    It is well known that the ENDF/B-V representation of the 239Pu resonance region is not satisfactory: below 1 eV the cross sections are given by smooth files (file 3) rather than by resonance parameters. Above 1 eV the single-level formalism used in ENDF/B-V necessitates a structured file 3 contribution. The present paper presents the results of an R-matrix multilevel analysis of several recent data sets as well as of the older data. The analysis is concerned with the region up to 30 eV, an energy region that is important for thermal reactors and for which no recent multilevel analyses had previously been available

  3. R-matrix analyses of the 235U and 239Pu neutron cross sections

    The resonance parameter analysis code SAMMY was used to perform consistent resonance analyses of several 235U and 239Pu fission and capture cross section and transmission measurements up to 110 eV for 235U and up to 1 keV for 239Pu. The method of analysis, the measurement selection and the results are briefly outlined in this paper

  4. Inhaled 239PuO2 in rats with pulmonary emphysema. II

    The modifying effects of pre-existing pulmonary emphysema on deposition, distribution, retention, and effects of inhaled 239PuO2 in the rat were investigated. The presence of emphysema in the rats tested was indicated by respiratory function measurements and confirmed microscopically. Initial lung burdens of 239Pu per kg body weight were less in rats with emphysema than in control rats; however, the retention of 239Pu was similar in emphysematous and control rats. Survival and lung tumor occurrence were similar in emphysematous and control rats exposed to 239PuO2. We concluded that rats with pre-existing pulmonary emphysema were not more sensitive to the effects of inhaled 239PuO2 than control rats. (author)

  5. Assessment of 238Pu and 239+240Pu, in marine sediments of the oceans Atlantic and Pacific of Guatemala

    In this investigation samples of marine sediments were taken from 14 places representatives of the oceans coast of Guatemala. For the assesment of 238Pu and 239+240Pu in sediments a radiochemical method was used to mineralize sediments and by ionic interchange it was separated from other elements, after that an electrodeposition of plutonium was made in metallic discs. The radioactivity of plutonium was measured by alpha spectrometry system and the alpha spectrums were obtained. The levels of plutonium are not higher than other countries that shown contamination. The contamination of isotope of 239+240Pu is higher than 238Pu and the contamination by two isotopes of plutonium is higher in the Atlantic than the Pacific ocean

  6. Measurement of plutonium isotopic composition by gamma-ray spectroscopy

    The technology of the analysis of plutonium isotopic ratio is independent of the measurement geometry and applicable to samples of physical and chemical composition. Three standard plutonium samples were measured in the HPGe system. The results showed that CRM 136 and CRM 137 containing 238Pu(0.223%) and 238Pu(0.268%) were 18.4% and 14.2% error and CRM 138 of 238Pu(0.01%) was 76% error. However the analysis represented less than 1.6% and 9% error in the three standard samples of highly involved 239Pu and 240Pu. Therefore, gamma-ray spectroscopy is very effective in the plutonium isotope analysis, having greater than 10% in content

  7. The removal of inhaled 239Pu from beagle dogs by bronchopulmonary lavage and chelation therapy

    The efficacy of bronchopulmonary lavage and chelatan therapy for removing 239Pu from beagle dogs after inhalation of 239Pu aerosols having different solubilities has been investigated. The four aerosols used were nebulized from a solution of 239PuCl4 and heat treated at temperatures of 325, 600, 900 and 11500C. Groups of six beagle dogs were exposed to each of the aerosols. Subsequently, three dogs in each group were treated by lavage and intravenous injections of DTPA. The remaining three dogs in each group served as untreated controls. It was found that bronchopulmonary lavage treatment was effective in removing nearly half of the 239Pu activity from the lung regardless of the aerosol production temperature. This early removal of 239Pu activity resulted in a significant reduction in daily dose rate and therefore cumulative α dose to lung. The effectiveness of DTPA treatment depended on aerosol production temperature, and was effective in reducing accumulation of 239Pu in liver and skeleton of the dogs that inhaled aerosols produced at 3250 and 6000C by enhancing urinary excretion of 239Pu. (U.K.)

  8. Plutonium isotopic composition by gamma-ray spectroscopy

    We discuss the general approach, computerized data analysis methods, and results of measurements 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, chemical and isotopic composition that have attained 241Pu-237U equilibrium. 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 Pu mass with a precision of 0.6% for 1000-g samples of PuO2 with 12% 240Pu content. The precision of isotopic measurements depends upon many factors including sample size, sample geometry, and isotopic content. Typical ranges are found to be 238Pu, 239Pu, 0.1 to 0.5%; 240Pu, 2 to 5%; 241Pu, 0.3 to 0.7%; 242Pu (determined by isotopic correlation); and 241Am, 0.2 to 10%

  9. Numerical prediction of 239Pu migration in unsaturated porous media under infiltration scenario

    In terms of the study on site selection of a radioactive waste disposal repository in northwest China, a numerical prediction of 239Pu migration for potential groundwater pollution in the unsaturated zone was conducted with the HYDRUS-1D model. The results showed that the groundwater will not be contaminated by the migration of soluble 239Pu. And there is little possibility that 239Pu migration through groundwater path might have an unacceptable impact on exosphere. Measurements of the distribution coefficient, Kd, are critical in the determination of sorption-induced retardation of radionuclide transport. (authors)

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

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

    2005-05-01

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

  11. Calculation of 239Pu neutron inelastic cross sections

    We have calculated cross sections for neutron-induced reactions on 239Pu between 0.001 and 5 MeV, with particular emphasis on inelastic scattering. Coupled-channel and Hauser-Feshbach statistical models were used. Within the coupled-channel calculations we employed neutron optical parameters derived from simultaneous fits to total, elastic, inelastic, and resonance data. The resulting transmission coefficients were used in Hauser-Feshbach statistical calculations having a fission channel based on a double-humped barrier representation. Barrier parameters and transition state enhancements needed to reproduce well the (n,f) cross sections between 0.001 and 5 MeV were in general agreement with those from other published analyses. Calculated compound-nucleus and direct-reaction components for inelastic scattering were combined incoherently, and the resultant cross sections agreed well with the Bruyeres-le-Chatel measurements for scattering from levels occupying the ground state rotational band. Our results are in substantial disagreement with ENDF/B-V values for these levels. We are presently performing DWBA calculations to determine direct-reaction components for states occupying higher-lying vibrational bands

  12. Toxicity of 239PuO2 inhaled by aged Beagle dogs. X

    The influence of age at exposure on the metabolism, dosimetry, and biological effects of inhaled 239PuO2 particles is being studied in aged Beagle dogs (8.0-10.5 yr of age at exposure). Forty-eight dogs inhaled 239PuO2 particles with an activity median aerodynamic diameter of 1.5 mm to achieve graded levels of initial pulmonary burdens (IPB) ranging from 0.02-0.66 μCi 239Pu/kg body weight (0.75-24 kBq/kg). Twelve other dogs were exposed to the aerosol diluent only. All forty-eight exposed dogs have died, including two in the past year. The twelve control dogs have also died, including one in the past year. Radiation pneumonitis and pulmonary fibrosis have been the primary causes of death in these aged dogs exposed to 239PuO2. (author)

  13. Malignancy of transplanted hamster lung lesions induced by inhaled 239PuO2

    Selected sites from the lungs of hamsters that had inhaled 239PuO2 aerosol were serially transplanted into the cheek pouches of recipient hamsters. Up to 13 mo postexposure, no evidence of malignancy has appeared

  14. Evaluation of the thermal cross sections of 239Pu and 241Pu

    The thermal neutron cross sections of the isotopes 239Pu and 241Pu have been evaluated in the thermal neutron energy region below 1.0 eV. The method of evaluation fitted energy-dependent data constrained by a modified Adler-Adler multilevel resonance fission and capture formalism and multilevel Breit-Wigner scattering theory. The energy dependence of the number of neutrons per fission was prescribed in the theory by introducing nu as fitted resonance spin-dependent values. The data were fitted in a resonance parameter fitting code, RPFC, using the method of maximum likelihood. The code fits simultaneously the total and partial energy-dependent cross section data to the theory. The types of data explicitly fitted are total, fission, capture, total scattering, coherent scattering, and absorption cross sections plus the quantities alpha, total nu and eta. Relative energy-dependent data with precision errors are fitted along with absolute values and errors at chosen energies. RPFC also allows energy-scale adjustment and Doppler broadening of selected data sets, and fits correlated data of two isotopes simultaneously. Reference experimental data bases of original data plus condensed and modified data were assembled for the evaluation for each isotope. 19 figures, 9 tables

  15. 133Ba as a gamma-ray surrogate source for 1kg HEU and 10g 239Pu and 252Cf as a Neutron Surrogate for Pu

    Monte Carlo was performed for the purpose of relating gamma-ray signal strength from 1kg of HEU and 10g of 239Pu (as described in the ASTM standards) to the radiation emitted from an amount of 133Ba. A determination was made on the amount of 133Ba that could act as a surrogate for the specified amounts of HEU and Pu. 133Ba is not the ideal source to use as a surrogate for HEU because of its higher energies. 133Ba was chosen as the surrogate since it has a half-life of 10.54 years, rather then the more ideal surrogate of 57Co which has a half-life of 271 days. A similar Monte Carlo was performed for the purpose of relating neutron signal strength from 200g of Pu (as described in the ASTM standards) to the radiation emitted from an amount of shielded 252Cf. A determination was made on the amount of 252Cf necessary to act as a surrogate for the 200g of Pu. An ASTM standard source is a metallic sphere, cube, or right cylinder of SNM having maximum self-attenuation of its emitted radiation. For plutonium, the source should be at least 93% 239Pu, less than 6.5% 240Pu, and less than 0.5% impurities. A cadmium filter of at least 0.08cm thick should be used to reduce the impact of 241Am. For uranium, the source should contain at least 95% 235U and less than 0.25% impurities. For neutron detector testing, the neutron source shall be placed in a lead shielding container that reduces the gamma radiation from the source to 1% of its unshielded value

  16. Behaviors and transfers of anthropogenic radionuclides (137Cs, 239+240Pu and 241Am) in a protected alpine wetland (France)

    The aim of this study is to confirm and increase the knowledge on anthropogenic radionuclide (RN) behavior (137Cs, 239+240Pu, 241Am) in natural compartments (artificial pool in a protected upland area). The novelty lies on comparisons of the three main compartments (pool water, soil, sediments) of this original mountainous site. Migration processes and transfers were particularly detailed in the light of two processes: lixiviation and leaching. Regarding 238U, anthropogenic RNs, lithology, organic matter contents, sedimentation rates (210Pb) and isotopic mass balances, RNs are mainly transported by leaching processes with higher 241Am in-depth mobility compared to 137Cs (intermediate for 239+240Pu). (author)

  17. 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

    Suseno, Heny, E-mail: henis@batan.go.id [Radioactive Waste Technology Center - The Indonesian National Nuclear Energy Agency (Indonesia); Wisnubroto, Djarot S. [The Indonesian National Nuclear Energy Agency (Indonesia)

    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}.

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

    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.

  19. Calculated activities of some isotopes in the RA reactor highly enriched fuel significant for possible environmental contamination - Operational report

    This report contains calculation basis and obtained results of activities for three groups of isotopes in the RA reactor 80% enriched fuel element. The following isotopes are included: 1) 85mKr, 87Kr, 88Kr, 131J, 132J, 133J, 134J, 135J, 133Xe, 138Xe i 138Cs, 2) 89Sr, 90Sr, 91Sr, 92Sr, 95Zr, 97Zr, 103Ru, 105Ru, 106Ru, 129mTe, 134Cs, 137Cs, 140Ba, 144Ce, kao i 3) 238Pu, 239Pu i 240Pu. It was estimated that the fuel is exposed to mean neutron flux. The periodicity of reactor operation is taken into account. Calculation results are given dependent on the time of exposure. These results are to be used as source data for Ra reactor safety analyses

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

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

  1. Low-level inhaled-239PuO2 life-span studies in rats

    This study determined the dose-response curve for lung tumor incidence in rats after inhalation of high-fired 239PuO2, which gave radiation doses to the lung of from ∼5 to >1000 rads. Exposed rats were given a single, nose-only, inhalation exposure to 169Yb-239PuO2 aerosol (AMAD, 1.6 +- 0.11 μm). The effective half-time for 169Yb in the lung was 14 days, whereas ∼76% of 239Pu was cleared with a half-time of 20 days and 24%, with a half-time of 180 days. Whole-body counting for 169Yb at 14 days after exposure was an accurate method for determining 239Pu IAD in individual rats, even at IAD's as low as 0.60 nCi of 239Pu. The 239Pu lung-clearance curve and an equation describing changes in lung weight with body weight and age were used to determine lung radiation doses. The IAD's of exposure groups were 0.60 +- 0.15 nCi of 239Pu (1000 rats), 0.98 +- 0.25 (531 rats), 2.4 +- 0.69 (209 rats), 5.7 +- 1.2 (98 rats), and 7.5 +- 2.0 to 150 +- 37 nCi (300 rats); corresponding radiation doses to the lung estimated at 3 years after exposure were 8.3, 14, 33, 79, and 100 to 2100 rads, respectively. 71 refs., 5 figs., 4 tabs

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

    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

  3. Repeated inhalation exposure of rats to aerosols of 239PuO2. V

    The biological responses following protracted alpha irradiation of rat lungs are being studied. Groups of rats have been exposed once, or repeatedly, to aerosols of 239PuO2 to achieve, or to re-establish, lung burdens of 239Pu that will result in projected lifetime alpha-radiation doses to the lungs of 20, 60, 200, or 600 rad. There were dose related increases in the incidence of primary lung tumors In the rats exposed once or repeatedly to 239PuO2. Repeated inhalation exposure of rats to 239PuO2 did not increase the incidence of lung tumors, their time of occurrence nor the risk of death with a lung tumor per unit of absorbed alpha dose to the lung compared to doses received following single exposures. These findings are consistent with those in Beagle dogs repeatedly exposed to 239PuO2 in other studies, but are not consistent with previous observations In mice. The findings in mice indicated protraction of the alpha dose to the lung by repeated inhalation exposure was more carcinogenic than similar doses after a single inhalation exposure. (author)

  4. Migration of 239Pu in soluble and insoluble forms in soil

    A field experiment study was performed at the rural site of South-East Lithuania. The main tasks of the study included an evaluation of the peculiarities of partition of 239Pu in soluble (239Pu(NO3)4, 239PuCl3) and insoluble (239PuO2) forms in soddy and forest soil horizons. The results of durable experiments (418 and 326 days) have shown that from 44.1% to 92.2% of 239Pu of investigated chemical forms were accumulated in the top (0-5 cm) soil layer. Some share (5.7-39.2%) of plutonium from studied chemical forms was found in the 5-20 cm layers of studied soil samples (columns). Obtained distribution of plutonium in soil layers may be attributed to the consideration that the migration rate to the soil depth for plutonium is 0.1-1.0 cm x y-1 but for some part of plutonium 10 times higher migration rate is characteristic as well. Plutonium transfer factor (TF) to the grassland plants was calculated, the values ranged from 10-2 to 10-1. (author)

  5. Generation of an actinide isotopes cross section set for fast reactor calculations using data from ENDL and ENDF/B-IV

    A Bondarenko format 25-group cross section set of actinide isotopes was generated for the fuel cycle evaluation and the incineration study in fast reactor systems. Evaluated Nuclear Data Library of Lawrence Livermore Laboratory (U.S.) was used as the source data. The actinide isotopes treated are the following 28: Th-232, U-233, U-234, U-235, U-236, U-237, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, Pu-243, Am-241, Am-242, Am-243, Cm-242, Cm-243, Cm-245, Cm-246, Cm-247, Cm-248, Bk-249, Cf-249, Cf-250, Cf-251, Cf-252 and a pseudo-fission product. ENDF/B-IV was used for U-238. The set was then collapsed to one energy group using a large LMFBR core spectrum for the comparison with other one-group sets. (author)

  6. XAS and XRD study of annealed 238Pu- and 239Pu-substituted zircons (Zr0.92Pu0.08SiO4)

    An annealing study has been completed on two compositionally identical Pu-substituted zircons (Zr0.92Pu0.08SiO4) prepared 18 yr ago with different 238Pu/239Pu isotopic ratios. The activity and accumulated dose for each material varies greatly due to the very different half-lives of 238Pu (87.7 yr) and 239Pu (24 100 yr). The predominantly 238Pu-substituted zircon is in a highly amorphous state after accumulating a dose of 2.8x1019 α-decays/g, which is a factor of two higher than the dose previously determined necessary to amorphize this material. The 239Pu-substituted zircon has remained highly crystalline after an accumulated dose of 1.2x1017 α-decays/g. The Pu in both samples is trivalent due to sintering under reducing conditions. The short-range and long-range structures of each sample have been characterized by detailed X-ray absorption spectroscopy and X-ray diffraction (XRD) methods. The oxidation of Pu3+ to Pu4+ in the crystalline 239Pu-substituted zircon during annealing in air resulted in a decrease in lattice distortion due to the decrease in ionic radius of Pu3+ to Pu4+ on the Zr4+ site. A significant amount of PuO2 exsolved from the zircon structure after annealing at 1200 deg. C in air. Detailed characterization of the amorphous 238Pu-substituted zircon demonstrated that while devoid of long-range order it still retained a distorted zircon structure and composition over a length scale of 0.5 nm. The recrystallization of the amorphous 238Pu-substituted zircon could be achieved directly at temperatures as low as 1200 deg. C when annealed for 12 h in air; however, annealing at 1000 deg. C resulted in decomposition into constituent oxides

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

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

    1992-07-01

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

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

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

    1992-07-01

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

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

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

  10. Biochemical effects of inhaled 239PuO2 on lung lipids

    Results of experiments carried out to assess the effect of 239Pu α irradiation on lung lipid biosynthesis and to determine the lungs ability to incorporate palmitate into lavage lecithin and its turnover are reported. The experiments were carried out on rats which had inhaled 239PuO2 particles. The study of palmitate incorporation into lipids shows conclusively that for medium (23 to 42 nCi) or high (more than 100 nCi) lung depositions the incorporation by isolated mitochondria is significantly (P 239PuO2 were positive, with respect to controls in 8 of 10 instances, when measured following the label of palmitate in lung lavage lecithin. The interpretation of the significant result (P < 0.05) is that: (1) initial and/or final lecithin pool sizes were different, (2) transfer rates were affected between blood and lung, or (3) rates of degradation of lung lavage lecithin were affected. (U.K.)

  11. Covariances for 239Pu induced cross section in the resonance range using the CONRAD code

    This paper will present the evaluation of neutron induced cross sections covariances for the 239Pu in the resonance range. The methodology used is based on marginalization and retroactive technique to allow the treatment of experimental systematic uncertainties such as normalization. In addition, as sensitivity studies performed on iso-thermal temperature moderator analysis have demonstrated the need for improving the description of the 239Pu neutron cross sections in the sub-thermal energy range and knowing the poor accuracy of the EXFOR data below the thermal energy range, integral trends have to be taken into account in this evaluation work. The focus of the presentation is to show results obtained on the 239Pu capture and fission neutron cross sections in the resonance range with an exhaustive integral validation. (authors)

  12. Medical Care for Accidental Deposition of Plutonium (239Pu) Within the Body

    With expanding uses of plutonium chances for accidental deposition within the body are increasing. Metabolism of plutonium within the body is variable, depending on chemical composition, particle size and shape, monomeric or polymeric physical state, route of entry (inhalation,or through wounds) and many other factors. A notable exception is the negligible absorption from the gastrointestinal tract. It is difficult to determine lung deposition of poorly soluble plutonium by either bioassay or in vivo counting. The intravenous administration of the chelating agent tri-sodium calcium salt of diethylenetriamine- pentaacetic acid (DTPA), soon after an accident, is quite effective in removing soluble plutonium which has been inhaled or deposited in wounds. Conditions requiring prolonged therapy are described. Effectiveness of treatment of 239Pu body depositions is greatly influenced by the solubility of the plutonium at the site of deposition. Size, frequency and duration of dose of DTPA is recommended. Mice developed fibrosarcomas following subcutaneous injections of 0.064 μCi of 239Pu, while an employee apparently developed a pre-cancerous condition after subcutaneous deposition of only 0.005 μCi. It is our policy to recommend excision of any measurable quantity of 239Pu in a superficial wound when this may be accomplished with little hazard. The maximum permissible deposition in skin or subcutaneous tissue may be much lower than that for depositions in bone liver, lung or tracheo-bronchial lymph nodes. No limiting value has been set for depositions in wounds by any official body; The surgeon must balance the benefits to be secured against the risk of the operation. A wound bearing 239Pu should be immediately washed with DTPA, normal saline, or water, in that order of preference. Methods of removal of 239Pu from the intact skin are briefly discussed. A U.S. Plutonium Registry will assist in evaluating depositions of 239Pu and effectiveness of therapy by reconciling

  13. Effects of inhalation of 239PuO2 on immune responses following lung immunization

    Results of this study indicated that the number of antibody-forming cells in lung-associated lymph nodes after intratracheal immunization was significantly lower in animals exposed to 239PuO2. Only a few antibody-forming cells were found in spleen and cervical lymph nodes. Thus, 239PuO2 exposure suppressed immune responses in lung-associated lymph nodes, although their filtering capacity was unaffected and antigen did not translocate to the spleen. Changes in immunologic responses were observed as the animals aged and the number of antibody-forming cells gradually decreased in the lung-associated lymph nodes and increased in the spleen

  14. Effects of 239Pu administered at 9 days of gestation on hematologic development of the rat

    Injection of pregnant rats with monomeric 239Pu after 9 days of gestation decreased their leukocyte and reticulocyte counts at 5 and 10 days postexposure. Most of the fetal hematologic enumerative values were unaffected by injection of monomeric 239Pu. There was, however, a major change in the maturation of the cells of the erythroid series, as indicated by a difference in the distribution between cell types. The weight of the yolk sac and fetal liver, and the cellularity of the fetal spleen were decreased

  15. Response of CR-39 plastic track detector to 239Pu and 252Cf sources

    CR-39 plastic track detectors have been irradiated with 239Pu and 252Cf sources separately at nuclear physics laboratory B.H.U., Varanasi to investigate track recording properties of detector material. All detectors etched in 6.25N NaOH solution at different temperatures for different hours. The bulk and track etch rates are calculated for both detectors (irradiated by 239Pu and 252Cf sources separately). The diameter and sensitivity along the trajectory of the track have been determined at different temperatures. (author)

  16. Pulmonary immune response of dogs after exposure to 239PuO2

    This study evaluated the cell-mediated (CMI) and humoral immune responses in four Beagle dogs five to six years after single inhalation exposures to different monodisperse 239PuO2 aerosols (0.72-1.4μm activity median aerodynamic diameter). These exposures resulted in initial lung burdens ranging from 19 to 35kBq. The immune responses induced by lung immunization of dogs that had inhaled 239PuO2 were not suppressed by large doses of chronic alpha irradiation of the lungs and tracheobronchial lymph nodes, indicating that local pulmonary immune responses are preserved despite severe radiation-induced alteration of these tissues. (author)

  17. Effect of inhaled 239PuO2 on alveolar Type II cells

    Morphological changes of rat alveolar type II (AT-II) cells were studied at 8 and 10 months following inhalation of 239PuO2 to elucidate the biological role of AT-II cells in the induction of lung tumours. TEM micrographs of random sections of lung were analysed qualitatively and quantitatively using an automatic image analyser. Eighteen morphometric parameters were obtained according to stereological principles. The results showed that, following the inhalation of 239PuO2, AT-II cells became less differentiated and the metabolism of the pulmonary surfactant in AT-II cells was disturbed. (author)

  18. Effect of inhaled 239PuO2 on alveolar type II cells

    Morphological changes of rat alveolar type II (AT-II) cells were studied at 8 and 10 months following inhalation of 239PuO2 to elucidate the biological role of At-II cells in the induction of lung tumours. TEM micrographs of random sections of lung were analysed qualitatively and quantitatively using an automatic image analyser. Eighteen morphometric parameters were obtained according to stereo logical principles. The results showed that, following the inhalation of 239PuO2, AT-II cells became less differentiated and the metabolism of the pulmonary surfactant in AT-II cells was disturbed

  19. Effects of pregnancy and lactation on the toxicity of 239Pu

    Nulliparous, pregnant, or lactating Wistar rats were injected intravenously with 0, 0.5 or 2.0 μCi of 239Pu per kilogram of body weight. Half of each group were repeatedly bred while the others were held for observation without further treatment. Treatment with either dose of 239Pu decreased the median time to appearance of mammary tumors. Repeated breeding tended to increase the mean time to appearance. Longevity was decreased in a dose-related fashion by Pu administration. Repeated breeding did not influence survival in a major way

  20. Concentrations of sup(239,240)Pu and 241Am in drinking water and organic fertilizer

    As part of an investigation of the chemistry and aquatic distribution of fallout-derived sup(239,240)Pu and 241Am in the aquatic environment a study has been made of the concentration of these nuclides in the drinking water and organic fertilizer, distributed to the populace of the Chicago area. The results clearly indicate that the concentration of sup(239,240)Pu is always lower in the water which has been treated at the Chicago Central Water Filtration Plant than in the raw water before treatment. Raw water levels are consistent with normal levels of sup(239,240)PU found in Lake Michigan waters which are approx 6 orders of magnitude below the maximum permissible concentration standard for drinking water. An additional possible source of sup(239,240)Pu and 241Am to humans can be through the distribution of the organic fertilizer, 'Nu Earth', by the Metropolitan Sanitary District, free of charge, for the use in home gardens. 'Nu Earth' consists primarily of sediment from an Imhoff Process which has been air-dried and aged in large, open-air piles. Samples of this organic fertilizer were analysed for sup(239,240)Pu and 241Am. The results indicate that there is little evidence to indicate that sup(239,240)Pu in drinking water or sup(239,240)Pu and 241Am from organic sludge will be health hazards in the Chicago area under current conditions. (U.K.)

  1. Evaluating and adjusting 239Pu, 56Fe, 28Si and 95Mo nuclear data with a Monte Carlo technique

    In this paper, Monte Carlo optimization and nuclear data evaluation are combined to produce optimal adjusted nuclear data files. The methodology is based on the so-called 'Total Monte Carlo' and the TALYS system. Not only a single nuclear data file is produced for a given isotope, but virtually an infinite number, defining probability distributions for each nuclear quantity. Then each of these random nuclear data libraries is used in a series of benchmark calculations. With a goodness-of-fit estimator, best 239Pu, 56Fe, 28Si and 95Mo evaluations for that benchmark set can be selected. A few thousands of random files are used and each of them is tested with a large number of fast, thermal and intermediate energy criticality benchmarks. From this, the best performing random file is chosen and proposed as the optimum choice among the studied random set. (authors)

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

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

    2016-10-01

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

  3. NKS-Norcmass reference material for analysis of Pu-isotopes and 237Np by mass spectrometry

    The aim of the reference material in the Norcmass-project was to produce a low-level (239Pu) sample of sufficient amount to allow individual laboratories to perform several tests without risk of using up the material. Although there are several reference materials available (eg IAEA) few have 239Pu/240Pu data and almost none have 237Np/239Pu-data. Those who have (eg IAEA-384) have very high concentrations and are not useful for testing analytical methods designed for low-level measurements where a large sample mass may be required. The reference material consist of the top 10cm of 2mm sieved soil pooled together from 12 different Danish locations collected during 2003. The Soil was blended and sieved through 0.6 and finally through a 0.4 mm sieve. A total amount of 17 kg soil was produced. Several aliquots of the material was subject to analysis by alpha spectrometry and ICP-MS. The material contain 239+240Pu at a concentration of 0.24 ± 0.01 mBq/g and a 240Pu/239Pu atom ratio of 0.19 ± 0.006. The ratio 237Np/239Pu was determined to 0.32 ± 0.01. (au)

  4. 239+240Pu and 90Sr deposition densities in undisturbed surface soil in Vietnam

    The study's goal is determination of 239+240Pu and 90Sr deposition densities from known distribution of 137Cs deposition density. The tasks done include: simultaneous determination of 239+240Pu, 90Sr and 137Cs deposition densities in undisturbed surface soil layer having depth to 20 cm and use it as basis for determining the ratios of deposition densities 239+240Pu/137Cs and 90Sr/137Cs; studying the impact of soil parameters such as soil texture, content of organic matter, Humic, Fulvic as well as of geography parameters such as latitude, longitude, annual rainfall to the variation of these ratios. (NHA)

  5. On the substantion of permissible concentrations of plutonium isotopes in the water of fresh water and sea water NPP cooling reservoirs

    Substantiation of maximum permissible concentration (PC) of plutonium isotopes (238Pu, 239Pu, 240Pu) in fresh and sea water cooling reservoirs of NPP with fast neutron reactors is given. The main criterion when calculating permissible plutonium content in water of surface reservoirs is the requirement not to exceed the established limits for radiation doses to persons resulted from water use. Data on coefficients of plutonium concentration in sea and fresh water hydrobionts are presented as well as on plutonium PC in water of fresh and sea water cooling reservoirs and bottom sediments of sea water cooling reservoirs. It is shown that doses to critical groups of population doesn't exceed potentially hazardous levels due to plutonium intake through food chains. But the calculation being carried out further should be corrected

  6. Rapid and simultaneous determination of neptunium and plutonium isotopes in environmental samples by extraction chromatography using sequential injection analysis and ICP-MS

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

    2010-01-01

    This paper reports an automated analytical method for rapid and simultaneous determination of plutonium isotopes (239Pu and 240Pu) and neptunium (237Np) in environmental samples. An extraction chromatographic column packed with TrisKem TEVA® resin was incorporated in a sequential injection (SI......) system for the isolation of plutonium and neptunium from matrix elements and interfering nuclides. Valence adjustment is a crucial step to ensure the same chemical behavior of plutonium and neptunium onto the TEVA column and consequently to accomplish their simultaneous separation and detection. Distinct...... procedures were investigated and compared for the adjustment of oxidation states of plutonium and neptunium to Pu(IV) and Np(IV), respectively. A two-step protocol using sulfite and concentrated nitric acid as redox reagents was proven to be the most effective method. The analytical results for both...

  7. Modifying effects of pre-existing fibrosis in rats exposed to aerosols of 239PuO2. II

    We have initiated a study using rats to determine the modifying effects of pre-existing pulmonary fibrosis on the retention and biological effects of inhaled 239PuO2. Pulmonary fibrosis was induced by intratracheal instillation of 8.5 IU/kg body weight of bleomycin at 45 to 49 days before inhalation exposure to an aerosol of 239PuO2. The clearance of 239Pu from the lungs of rats was decreased significantly (p 239Pu, apparently by entrapping the particles in fibrotic areas of the lung. The life span of the rats with pulmonary fibrosis was decreased by up to 25% compared with control rats having similar initial lung burdens of 239Pu. (author)

  8. Biological effects of 239PuO2 inhalation in the Rhesus monkey

    Rhesus monkeys were exposed to polydisperse, high-fired 239PuO2 aerosols and have been studied for 3 yr to determine the biological effects associated with this inhalation exposure. Initial lung burdens in 16 monkeys exposed to aerosols of 239PuO2 ranged from 7 to 1800 nCi. Two monkeys are serving as controls. The inhaled 239 PuO2 was retained with a long effective half-life in the lung with some translocation from the lung to the pulmonary lymph nodes. In animals exposed to high levels of 239PuO2, there was a depression in the number of lymphocytes in the peripheral blood. However, blood lymphocytes cultured at time periods up to 30 mo after inhalation showed no increase in chromosome aberration frequency. An animal with an estimated initial lung burden of 1000 nCi showed marked alterations in respiratory function. Only slight respiratory changes were detected in the other animals evaluated. To date, three monkeys have died, two of radiation pneumonitis and the third of gastric torsion. Comparing these data from Rhesus monkeys with those obtained from baboons and Beagle dogs indicate that Rhesus monkeys are similar to dogs in their early radiation response

  9. Pulmonary distribution of inhaled 239PuO2 in dogs

    Dogs exposed to 239PuO2 by inhalation were killed from 1 to 69 mo postexposure. The distribution of plutonium in the lungs, which was studied by analyzing autoradiographs, changed relative to time postexposure. This study investigates methods of measuring these changes

  10. R-matrix analysis of the 239Pu cross sections up to 1 keV

    The results are reported of an R-matrix resonance analysis of the 239Pu neutron cross sections up to 1 keV. After a description of the method of analysis the nearly 1600 resonance parameters obtained are listed and extensive graphical and numerical comparisons between calculated and measured cross-section and transmission date are presented. 47 refs., 47 figs., 8 tabs

  11. Yield-Energy Evaluation of 85Kr of 239Pu+n Fission

    2008-01-01

    <正>The yields of 85Kr, the important production of the 239Pu fission, were re-evaluated over the incident neutron energy 1-15 MeV, based upon all the experimental data. The yields as function of energ

  12. Effects of inhaled 239PuO2 on the primary immune response of beagle dogs

    Effects of inhaled 239PuO2 on the humoral component of the immune system were measured by intravenous immunizations of beagle dogs with keyhole limpet hemocyanin (KLH). With this T-cell-dependent antigen, a significant decrease in primary antibody response was observed in exposed versus unexposed dogs

  13. Chromosome aberration frequency in blood lymphocytes of animals with 239Pu lung burdens

    Other investigators have suggested a causal relationship between accidental 239Pu exposures in man and the presence of chromosome aberrations in blood lymphocytes. To assess this relationship experimimentally, 16 Rhesus monkeys and 171 Chinese hamsters were exposed by inhalation to 239PuO2 aerosols and an additional five hamsters were injected with 239Pu citrate and the frequency of aberrations in blood lymphocytes determined. After an initial rapid clearance phase, the 239Pu was retained in the monkey lung with a long effective half-life (greater than 500 days). At 30 days after inhalation, 99 percent of the sacrifice body burden was in the lungs of both species. The ranges of cumulative radiation dose to the hamster lungs 30 days after inhalation were calculated to be 80 to 170, 220 to 540, and 830 to 2120 rads for initial lung burden levels of 10 to 30, 30 to 70, and 180 to 260 nCi/g, respectively. By 120 days, these doses were calculated to be 40 to 350, 500 to 710, and 1440 to 2170 rads. Hamsters with the highest lung burdens had a median survival time of about 80 days. No deaths occurred in any of the other treated hamsters or monkeys by 250 days after 239Pu inhalation. Hamsters sacrificed at 30 days showed an increase in chromosome aberration frequency with increasing dose to lung. By 120 days after inhalation, the aberration frequency in the controls was 0.012. The frequency in animals with doses that produced significant life shortening (1440 to 2170 rads) had decreased to 0.018 and to 0.032 aberrations/cell in animals with lung doses of 500 to 710 rads. At 380 days after injection of 60 nCi 239Pu citrate/gm, hamster lymphocytes had an aberration frequency of 0.048 aberrations/cell. The level of chromosome damage in the 239PuO2 exposed monkeys at 30 and 90 days after inhalation was not different than observed in controls. (U.S.)

  14. ZZ AMZ, 70-Group 40 Isotope Multigroup Library for Fast Reactor Calculation

    1 - Description of program or function: format: EXPANDA; number of groups: 70-group library of multigroup constants; nuclides: H-1, Be-9, B-10, B-11, C-12, O-16, N-23, Mg, Al-27, Si, Ti, V, Cr, Mn-55, Fe, Ni, Cu, Ga, Zr, Nb-93, Mo, In-115, Sn, Pb, Th-232, Pa-233, U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, Am-241, and lumped fission products of U-233, U-235, Pu-239. origin: ENDF/B-IV and ENDF/B-V; weighting spectrum: Fission products inventories for BBR reactor at 360 and 600 days of irradiation were calculated and used as weighting function. AMZ is a 70-group library of multigroup constants for the fast reactor nuclear design code EXPANDA. Data is stored for three temperatures (300 K, 900 K, 2100 K) and for seven background cross sections. The following isotopes are available: H1, Be9, B10, B11, C12, O16, N23, Mg, Al27, Si, Ti, V, Cr, Mn55, Fe, Ni, Cu, Ga, Zr, Nb93, Mo, In115, Sn, Pb, Th232, Pa233, U233, U234, U235, U236, U238, Pu238, Pu239, Pu240, Pu241, Pu242, Am241, and lumped fission products of U233, U235, Pu239. 2 - Method of solution: Nuclear cross sections, transfer matrices, and self-shielding factors were generated from ENDF/B-IV data using the codes NJOY (PSR-0171) and RGENDF

  15. Radiation effect of 239PuO2 on human cells in vitro

    In this paper, the in vitro short and long term effects of 239PuO2 on human embryo lung fibroblast are reported. The short term effect observed is the changes in proliferation and survival of the cell line which were exposed to 239PuO2 with concentration of 0.0006 μCi/mL for a week. On 7th day, the proliferation was only 4.88 PDN (population doubling number), while the control was 10.5 PDN. On the 6th day the surviving fraction of the treated cells was 56.3% and that of the control was 96%. For the long term effect studies, the follow-up observation for 12 groups of cell culture exposed to 239PuO2 of 0.0015 and 0.003 μCi/mL was made. In the cultures exposed to 239PuO2 of 0.003 μCi/mL, the shape of the cells became shorter and their life-span shortened with a higher mortality and death appears early. In 7 cultures exposed to 239PuO2 of 0.0015 μCi/mL, the change in cell morphology was the same as above and their life span was shortened by 58.7% averagely in comparison with control. On other two cultures of them not only was no life-span shortening found, but it was longer than that in the control and their inherent characteristics of regionol arrangment disappeared. At last epithelium-like shape of transformed cells were appeared. In the electron microscope siking of the nuclear membranes into nucleus and hypertrophy of the nucleolus with netted structure can be observed. The nuclear volume increased largely and the ratio between nucleus and cytoplasm increased

  16. Worldwide data on fluxes of 239,240Pu, 238Pu to the oceans

    According to measurements (GEOSECS) the world's oceans contain approximately 16 PBq 239,240Pu, of which one-fourth is in the Atlantic and three-fourths in the Pacific Ocean. The expected inventory (from nuclear weapons testing) in the world's oceans is 12 PBq 239,240Pu including local fallout at the test sites. In the Irish Sea a local contamination of 0.3 PBq 239,240Pu from the Sellafield reprocessing plant resides in the sediments. No other sources than fallout and reprocessing add significantly to the 239,240Pu inventories in the oceans. The discrepancy between measurements and expectations are assumed to be due to an underestimate of the rainfall and dry fallout (seaspray) and thus of the Pu-deposition over the oceans, but may also to some degree be due to inadequate sampling

  17. Precision of gamma-ray measurements of the effective specific power and effective 240Pu fraction of plutonium

    This paper uses gamma-ray spectrometry data from replicate measurements on 40 plutonium-bearing samples to examine the repeatability of the effective 240Pu fraction (240Pueff) and the effective specific power (Peff) 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 (240Pueff) and calorimetry (Peff). The 40 samples had 240Pueff percentages ranging from 2 to 39% and Peff 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 Peff was smaller than that of 240Pueff. 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 240Pu correlation used in the gamma-ray spectrometry codes also supported this conclusion. 17 refs

  18. Uncertainty Budget and Efficiency Analysis for the 239Pu (n,2ny) Partial Reaction Cross-Section Measurements

    The 239Pu(n,2nγ)238Pu partial reaction cross-section, σ(n,2nγ), has been measured as a function of neutron energy for several transitions in 238Pu. Partial γ-ray cross sections for yrast, ''collector'' transitions, can provide especially valuable constraints on the magnitude and shape of the total (n,2n) reaction cross-section. In essence, nuclear reaction models will be used to infer the shape and magnitude of the total (n,2n) reaction cross-section from the measured partial γ-ray cross-sections. The reason for undertaking this somewhat indirect approach is that previous measurements of the 239Pu(n,2nγ) have been hampered by a variety of constraints. Activation measurements have several hurdles: (1) intense flux and long counting times are required to overcome the relatively long half-life of 238Pu (87 years) and (2) isotopically pure samples of 239Pu in an environment free of 238Pu contamination are difficult to come by. Neutron counting experiments are subject to significant uncertainties because (1) large background statistics from fission neutrons and (2) the experimental fission neutron multiplicity spectrum is subject to systematic errors because the flux of low-energy neutrons which induce fissions in thermally-fissile 239Pu is very difficult to characterize. In this measurement, spallation neutrons are provided by the LANSCE/WNR facility, and reaction neutron energies are determined via time-of-flight. Neutron flux is monitored in-beam with one 235U fission chamber and one 238U fission chamber. The 238U is not sensitive to background from low-energy neutrons, whereas the 235U fission chamber has better statistics. Hence, in essence the partial γ-ray cross sections are normalized to the evaluated fission cross sections of 235U and 238U. As a check of our normalization to provide additional constraints to the nuclear reaction modeling, benchmark measurements of natFe(n, n(prime)γ) and 235U(n,2nγ) have also been undertaken. The secondary γ-rays are

  19. Performance of isotope correlations for the estimate of 242Pu

    The lack of a gamma-ray signature from 242 Pu represents an Achilles heel for many plutonium isotope abundance measurements made by high-resolution gamma spectrometry (HRGS). This holds in particular for plutonium materials containing a significant fraction of this isotope. The problem is partially solved through the application of isotope correlations estimating the relative abundance of 242 Pu from relations to ratios of other plutonium isotopes measurable by HRGS. In the mid of the nineties a new type of isotope correlation had been proposed for LWR plutonium with the recommended coefficients for PWR and BWR fuels. This type of correlation was adopted for the routine analysis of safeguards samples in the Euratom On-Site Laboratories and in the Institute for Transuranium Elements. In order to cover the full range of plutonium materials received for analysis, the application of the above correlation has been also extended to AGR and Magnox-type of plutonium with different sets of coefficients approximating best the correlation for the additional types of materials were determined from a set of reference isotopic data. Since in many instances the origin and the type of the plutonium are not known a priori, criteria for categorization were established helping to select the appropriate isotope correlation. Parametric plots of the ratios 238 Pu/239 Pu versus 240 Pu/239 Pu generally allow to discern unambiguously Magnox, AGR and LWR plutonium, and to some extent also BWR and PWR plutonium, as long as a mixing of the respective plutonium materials has not occurred. With this kind of categorization implemented in the routine analysis the performance of the 242 Pu estimate is substantially improving in most cases. Performance data for 242 Pu in particular, and for plutonium isotope abundance measurements by HRGS in general, as derived from a larger set of measurement data are presented and discussed in terms of their impact on the interpretation of passive neutron

  20. Effects of combined exposure of rats to 239PuO2 and whole-body X irradiation. II

    Using F344/N rats, we are studying the biological effects of inhalation exposure to 239PuO2 aerosols combined with whole-body exposure to X rays. Data from this study will provide an improved estimate of the cancer risk from combined exposures in people. A total of 2136 (66%) of the 3232 rats to be entered into this study have been exposed. We have achieved lung burdens of 239Pu and X-ray exposures within the ranges desired. Life shortening has occurred among rats receiving whole-body exposure to X rays, but not among those exposed only to 239PuO2. (author)

  1. Characterization of a neutron source of {sup 239}PuBe; Caracterizacion de una fuente de neutrones de {sup 239}PuBe

    Hernandez V, R.; Chacon R, A.; Hernandez D, V. M.; Mercado, G. A.; Vega C, H. R. [Universidad Autonoma de Zacatecas, Unidad Academica de Estudios Nucleares, Calle Cipres No. 10, Fracc. La Penuela, 98068 Zacatecas (Mexico); Ramirez G, J. [Instituto Nacional de Estadistica Geografia e Informatica, Direccion General de Innovacion y Tecnologia de Informacion, Av. Heroes de Nacozari Sur 2301, Fracc. Jardines del Parque, 20276 Aguascalientes (Mexico)], e-mail: ruben_zac@yahoo.com

    2009-10-15

    The spectrum equivalent dose and environmental equivalent dose f a {sup 239}PuBe source have been determined. The appropriate handling of a neutron source depends on the knowledge of its characteristics, such as its energy distribution, total rate of flowing and dosimetric magnitudes. In many facilities have not spectrometer that allows to determine the spectrum and then area monitors are used that give a dosimetric magnitude starting from measuring the flowing rate and the use of conversion factors, however this procedure has many limitations and it is preferable to measure the spectra and starting from this information the interest dosimetric magnitudes are calculated. In this work a Bonner sphere spectrometer has been used with a {sup 6}LiI(Eu) scintillator obtaining the count rates that produce, to a distance of 100 cm, a {sup 239}PuBe source of 1.85E(11) Bq. The spectrum was reconstructed starting from the count rates using BUNKIUT code and response matrix UTA4. With the spectrum information was calculated the source intensity, total flow, energy average, equivalent dose rate, environmental equivalent dose rate, equivalent dose coefficient and environmental equivalent dose coefficient. By means of two area monitors for neutrons, Eberline ASP-1 and LB 6411 of Berthold the equivalent dose and environmental equivalent dose were measured. The determinate values were compared with those reported in literature and it found that are coincident inside 17%. (Author)

  2. Investigation of the resonance self-shielding effect in the α-value of 239Pu

    Gamma-spectra from 1 to 15 multiplicities were measured on 122 m flight path of the IBR-30 pulsed neutron booster using a 16-section liquid scintillation detector of a total volume of 80 l for two thin metallic radiator-samples of 239Pu in the presence of a filter-samples with four thickness: 0.3, 0.5, 1 and 2.3 mm in the neutron beam and without them. The multiplicity distribution spectra, the average multiplicities and the alpha value α = σγ/σf for 27 resonances in the energy region 7-170 eV and for the energy group in the region 4.65-2150 eV with and without filter-samples of 239Pu in the beam were obtained. The self-shielding effect in the alpha value and the average multiplicity in limits 5-40% of experimental value is observed

  3. Studies of Neutron-Induced Fission of 235U, 238U, and 239Pu

    Duke, Dana; TKE Team

    2014-09-01

    A Frisch-gridded ionization chamber and the double energy (2E) analysis method were used to study mass yield distributions and average total kinetic energy (TKE) release from neutron-induced fission of 235U, 238U, and 239Pu. Despite decades of fission research, little or no TKE data exist for high incident neutron energies. Additional average TKE information at incident neutron energies relevant to defense- and energy-related applications will provide a valuable observable for benchmarking simulations. The data can also be used as inputs in theoretical fission models. The Los Alamos Neutron Science Center-Weapons Neutron Research (LANSCE - WNR) provides a neutron beam from thermal to hundreds of MeV, well-suited for filling in the gaps in existing data and exploring fission behavior in the fast neutron region. The results of the studies on 238U, 235U, and 239Pu will be presented. LA-UR-14-24921.

  4. R matrix analysis of the 239Pu cross sections up to 600 eV

    The ENDF/B-V representation of the 239Pu neutron cross sections in the resonance region is unsatisfactory: the single-level formalism is used, necessitating a structured file 3 contribution. Furthermore, Salvatores et al. have stressed the need to extend the resolved resonance region above the present ENDF/B limit of 300 eV for the calculation of Doppler effect and self-shielded group cross sections. The purpose of our work is to improve the representation of the 239Pu cross sections by using a multilevel formalism (which avoids the need for the file 3 contributions) and by extending the resolved resonance range from 300 up to 600 eV. The present resonance analysis is based on the Reich-Moore multilevel formalism and was performed with the Bayesian code SAMMY. The resonance parameters published in 1974 by Derrien were used as prior information. More than 200 levels and 1000 resonance parameters are included in the analysis

  5. Toxicity of 239PuO2 in immature Beagle dogs. X

    Immature beagles have been exposed by inhalation to a monodisperse aerosol of 239PuO2 (1.5 μm AMAD) to compare the biological effects with those being observed in dogs exposed to a similar aerosol when they were young or aged adults. The study includes 96 dogs exposed to 239PuO2 and 12 controls. A total of 66 experimental and 11 control dogs are still alive. Six dogs died during the past year, all of radiation-related causes. Five dogs died from lung carcinomas and the sixth dog died of pneumonia/fibrosis, but with a lung tumor. With the large number of dogs still alive in this study, it is still premature to compare the cancer dose-response relationships for the immature and adult dogs. (author)

  6. Early effects of inhaled 239Pu(NO3)4 aerosols in beagle dogs

    Beagle dogs given a single inhalation exposure to 239Pu(NO3)4, and observed for life-span dose-effect relationship, died from radiation pneumonitis (4 of 5) at the highest dosage level, 14 to 25 mo postexposure. There were also indications in these dogs of radiation osteosis, characterized by peritrabecular fibrosis. Leukopenia, lymphopenia, neutropenia and decreased numbers of circulating monocytes and eosinophils occurred at the two highest dosage levels, as previously reported

  7. Analysis of the 239Pu neutron cross sections from 300 to 2000 eV

    A recent high-resolution measurement of the neutron fission cross section of 239Pu has allowed the extension from 1 to 2 keV of a previously reported resonance analysis of the neutron cross sections, and an improvement of the previous analysis in the range 0.3 to 1 keV. This report analyzes this region. 8 refs., 1 fig., 2 tabs

  8. 235 U consumption and 239 Pu formation on IPR-R1 reactor

    On the present world conjuncture it is necessary a rigorous storage and utilization control of nuclear materials under safeguard, specially those considered as strategic and those that could be used on the nuclear armaments fabrications as 235U and 239Pu. Brazil have signed and ratified many international pacts related to the peaceful utilization of the nuclear materials, making the compromise to attend nuclear safeguard procedures accorded with international regulatory organizations. The main goal of this work is the development of a simplified method for the estimation of the 239Pu productivity during the operation of the IPR-R1, TRIGA Mark-1 type, nuclear research reactor, that can achieve the maximum power of 100 KWt. A computational algorithm have been made to calculate the consumption of 235U on the fuel elements used on the reactor and the subsequent 239Pu formation (by the neutronic capture process), using the power generated by the reactor since the first criticality. The particular geometry of this kind of reactor allowed the calculation of the burn factors of the fuel elements discriminated by nuclear concentric rings, based on the thermal neutrons field distribution observed on experiments accomplished during a time period in similar reactors and on the IPR-R1. The simplified block diagram of the process, based on the calculation described above, is presented

  9. Neutron-induced fission cross section of 240Pu from 0.5 MeV to 3 MeV

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

    2015-07-01

    240Pu has recently been pointed out by a sensitivity study of the Organization for Economic Cooperation and Development (OECD) Nuclear Energy Agency (NEA) to be one of the isotopes whose fission cross section lacks accuracy to meet the upcoming needs for the future generation of nuclear power plants (GEN-IV). In the High Priority Request List (HPRL) of the OECD, it is suggested that the knowledge of the 240Pu(n ,f ) cross section should be improved to an accuracy within 1-3 %, compared to the present 5%. A measurement of the 240Pu cross section has been performed at the Van de Graaff accelerator of the Joint Research Center (JRC) Institute for Reference Materials and Measurements (IRMM) using quasi-monoenergetic neutrons in the energy range from 0.5 MeV to 3 MeV. A twin Frisch-grid ionization chamber (TFGIC) has been used in a back-to-back configuration as fission fragment detector. The 240Pu(n ,f ) cross section has been normalized to three different isotopes: 237Np(n ,f ) , 235U (n ,f ) , and 238U (n ,f ) . Additionally, the secondary standard reactions were benchmarked through measurements against the primary standard reaction 235U (n ,f ) in the same geometry. A comprehensive study of the corrections applied to the data and the associated uncertainties is given. The results obtained are in agreement with previous experimental data at the threshold region. For neutron energies higher than 1 MeV, the results of this experiment are slightly lower than the ENDF/B-VII.1 evaluation, but in agreement with the experiments of Laptev et al. (2004) as well as Staples and Morley (1998).

  10. Investigations of the chemical forms of 239Pu and 241Am in estuarine sediments and a salt marsh soil

    Estuarine sediments and a salt marsh soil have been fractionated by non-destructive procedures. The distribution of 239Pu and 241Am in these fractions has been determined by gel permeation chromatography and extraction with complexing agents. (author)

  11. Measurement of the fission cross-section of $^{240}$Pu and $^{242}$Pu at CERN's n_TOF Facility

    Pavlik, A F; Gonzalez romero, E M

    The n_TOF Collaboration proposes to continue the fission program, already started in 2002-2004, taking advantage of the newly constructed Work Sector Type A, with the measurement of the two isotopes : $^{240}$ Pu and $^{242}$ Pu. They are both of major importance for reactor physics applications and are included in the Nuclear Energy Agency (NEA) High Priority List [1], in the NEA WPEC Subgroup 26 Report on the accuracy of nuclear data for advanced reactor designe [2] and in the EU 6$^{th}$ Framework Programme IP-EUROTRANS/NUDATRA reports [3]. Based on those requests, the measurement of the fission cross-section of the two Pu isotopes is one of the objectives of the project ANDES of the FP7 EURATOM program [4].

  12. Group cross-sections and resonance self-shielding factors for 239Pu in the unresolved resonance region

    The authors analyse experimental data on the transmission and fission self-indication functions for 239Pu in the unresolved resonance region. Use is made of the method of generating a cross-section structure based on the multi-level R-matrix formalism (stochastic K-matrix method). Evaluations of the average resonance parameters and group constants for 239Pu are made. (author)

  13. Modification of 239Pu metabolism in the blood in various modes of iron preparation administration in the body

    A study was made of the intravenous, intraperitoneal and oral routes of iron administration. It was shown that the oral route of the entry of appropriate amounts of iron in the body made it possible to saturate the transferrin spare capacity and hence to influence 239Pu metabolism in the blood. The results obtained can be employed for improving sensitivity of indirect dosimetry methods of 239Pu in the body using chelates

  14. Cytogenetic and other biological effects of 239PuO2 inhaled by the rhesus monkey

    Sixteen immature rhesus monkeys were exposed via inhalation to an insoluble, polydisperse 239PuO2 aerosol labeled with 169Yb which had an activity median aerodynamic diameter of 1.6 μm and a sigma/sub g/ of 1.6. Four groups with three monkeys per group were exposed to achieve initial 239Pu lung burdens of 1000 to 2000, 200 to 300, 20 to 65, and 2 to 10 nCi, respectively. To determine early retention and distribution of the aerosol, four additional monkeys were exposed with initial lung burdens of 200 to 600 nCi and were sacrificed 4 hr and 30 days after inhalation exposure. Two monkeys were sham exposed and served as controls. Using data derived from external whole-body counting of the 169Yb label, it was estimated that the inhaled 239PuO2 was retained in the body with an average effective half-life of 1000 days with some translocation from the lung to the pulmonary lymph nodes. Chromosome aberrations were scored in blood lymphocytes cultured 1, 3, 7, 19, 31, and 43 months after inhalation. Only in animals with cumulative lung doses greater than 1000 rad was there a significant increase in the frequency of rings and dicentrics when compared to the controls. An animal with an estimated initial lung burden of 1000 nCi showed marked alterations in respiratory function 30 days prior to his death from pulmonary fibrosis 990 days after inhalation exposure. Only slight respiratory changes were detected in the other animals evaluated. To date, three monkeys have died, two with initial lung burdens of 1800 and 1000 nCi 239Pu which died from radiation pneumonitis and the third with an initial lung burden of 20 nCi which died of gastric torsion presumably not related to Pu exposure. Comparison of survival data from rhesus monkeys with those obtained from baboons and beagles indicates that rhesus monkeys, baboons, and dogs are similar in their early response to inhaled 239PuO2

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

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

    2016-09-01

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

  16. Determination of isobar composition and yields of 239Pu fission-products by thermal neutrons

    On the research nuclear reactor WWR-SM of INP Uz AS by means of mass-spectrometer the heavy fission-products of 239Pu nuclei induced by thermal neutrons are measured in ranges of mass Ai = 125 -157, kinetic energies Ek = 45 - 87 MeV and effective ionic charges z* = 18 - 30. 102 isobar nuclei in composition of the measured fission-products, also the partial yields of the each element giving the contribution to formation of a total yield of heavy fission-product with mass Ai are defined. (authors)

  17. On the ENDF/B unresolved resonance region formalism representation for 239Pu

    The purpose of this work is to compare the performance of several cross-section evaluation files for the calculation of average cross sections in the unresolved resonance region and to test the validity of the ENDF/B methodology for the calculation of self-shielding factors in this region. The 239Pu neutron cross sections were used for this comparison since a multilevel R-matrix analysis was available, which extended the resolved resonance region from its present ENDF/B limit of 300 eV up to 1 keV. 12 refs., 2 tabs

  18. Status of 239Pu cross-section evaluation in the resonance region at Cadarache

    Some aspects of the evaluations of 239 Pu cross-sections in the resonance region have been presented in this report. A set of resonance parameters assembling the results of a multilevel analysis in the energy range thermal to 200 eV and the result of a single analysis in the energy range 200 eV - 660eV is proposed for the calculation of the cross-sections in the energy range thermal-600eV. These parameters provide a quite good representation of the most recent measured fission cross-sections

  19. Repeated inhalation exposure of Beagle dogs to aerosols of 239PuO2. XII

    Beagle dogs were exposed once or semi-annually for 10 yr by inhalation to aerosols of 239PuO2 to study the relative doses and effects of these two types of exposures. All exposures have been completed. Dogs exposed at high levels died predominantly of radiation pneumonitis and pulmonary fibrosis. Dogs exposed at lower levels, either once or repeatedly, are dying of a variety of causes including lung cancer. Dogs have survived up to 11 yr after their first exposure. Preliminary results suggest that single and repeated exposures cause similar health effects for equal accumulated radiation doses. (author)

  20. Effects of cigarette smoke exposure on pulmonary clearance of 239PuO2 in rats

    Groups of rats were exposed or sham exposed to cigarette smoke for 7 mo, at which time they were exposed to an aerosol of 239PuO2. Rats were then subjected to whole-body counting (17-keV X-rays) periodically, beginning at day 4 after plutonium exposure, and smoke exposures or sham exposures were resumed on day 7. Clearance of plutonium from the lungs of cigarette-smoke-exposed rats was significantly slower than that from the sham-exposed rats' lungs. The difference between the two groups became significant 7 days after the resumption of cigarette-smoke exposures

  1. Direct reduction of 238PuO2 and 239PuO2 to metal

    The process for reducing 700 g 239PuO2 to metal is a standard procedure at Los Alamos National Laboratory. This process is based on research for reducing 200 g 238PuO2 to metal. This report describes in detail the experiments and development of the 200-g process. The procedure uses calcium metal as the reducing agent in a molten CaCl2 solvent system. The process to convert impure plutonia to high-purity metal by oxide reduction followed by electrorefining is also described

  2. Distribution and retention of 239Pu in the tree shrew (Tupaia belangeri) following intramuscular injection

    The retention of intramuscularly injected monomeric 239Pu has been studied in the tree shrew (Tupaia belangeri), a primitive prosimian species. Resorption from the injection site is rapid, and the main depository organs are skeleton and liver with approximately 50 and 20% of the absorbed dose, respectively. The half life of retention in skeleton is approximately 500-600 days and in liver approximately 150 days, these half lives are compared to data for the retention of transuranium elements in other animal species. Indications of liver lesions were found in 5 animals and 1 animal died at day 790 with an osteosarcoma. (author)

  3. The evaluation of the mass distribution data for 238U, 239Pu and 242Pu fission

    The mass distribution data for 238U at En=1.5, 5.5, 8.3, 11.3, 14.9, 22.0, 27.5, 50.0, 99.5, 160.0 MeV, Ep=20.0, 60.0 MeV 239Pu at En=0.17, 7.9, 14.5 MeV and 242Pu at En=15.1 MeV were evaluated and recommended based on the main available experimental data up to now. The experimental data were make necessary corrections and their errors were also made necessary adjustments. The problems concerned were discussed

  4. R-matrix analysis of the 239Pu neutron cross sections

    239Pu neutron cross-section data in the resolved resonance region were analyzed with the R-Matrix Bayesian Program SAMMY. Below 30 eV the cross sections computed with the multilevel parameters are consistent with recent fission and transmission measurements as well as with older capture and alpha measurements. Above 30 eV no suitable transmission data were available and only fission cross-section measurements were analyzed. However, since the analysis conserves the complete covariance matrix, the analysis can be updated by the Bayes method as transmission measurements become available. To date, the analysis of the fission measurements has been completed up to 300 eV. (author)

  5. Dominant lethal tests of male mice given 239Pu salt injections

    To study the possible genetic effects of 239Pu manifesting in dominant lethals, five test series (E1-E5) were performed. Males from an inbred CBA strain were given 239Pu salt injections intravenously and mated weekly to 3 CBA females each for 12 to 24 weeks. Some interruptions in the mating scheme were made. For the first two test series (E1, E2) 239Pu nitrate solution and 239Pu citrate, used in E3-E5, were prepared. The solution was millipore filtered just prior to injection. Among a total of 10255 implants sired by males given Pu-nitrate in E1 and E2 no significant excess of intra-uterine death relative to 7216 control implants occurred. Test series E3-E5 with 60 males each, used three groups of 20, with one control group. In E3, 0.5 μCi and 0.1 μCi were given per male/group, respectively; in E4 and E5, 0.25 μCi and 0.05 μCi, respectively. The males given 0.5 μCi in E3 became successively sterile from the 7th week. The results in E3-E5 point in the same direction with significant excess of intra-uterine death in E3 and E5. In E4 the females from matings from the 9th, 14th and 16th week, and in E5 females from the 9th week, were allowed to litter to give F1 offspring. Dominant lethal tests of F1 males gave concordant results in all four samples, showing significantly excessive death in offspring to F1 males whose fathers had received Pu. The excessive death was evenly distributed and did not indicate the presence of semisterile F1 males. In tests of Pu-injected males and of F1 males a remarkable excess of death in late stages of foetal development was observed. Such effects had never before been observed in this CBA strain in tests of extrinsic and intrinsic exposure to ionizing irradiation

  6. Decreased pulmonary clearance of 239PuO2 and lung toxicity induced by inhaled beryllium metal in rats

    Workers in nuclear industries may be accidentally exposed to both beryllium and plutonium. To characterized the effects of combined exposures to these agents on their pulmonary clearance, groups of F344/N rats inhaled aerosols of beryllium metal and 239PuO2 to result in initial lung burdens for beryllium metal of 0, 50, 150, and 450 μg, and for 239PuO2 of 0, 56, and 170 Bq. Rats were exposed to each possible beryllium/plutonium combination. The whole-body clearance half time of 239Pu in the absence of beryllium metal was approximately 50 days. For rats exposed to both materials, however, 239Pu clearance half-times ranged from 280 to 410 days, with no apparent dose-dependent effect of beryllium metal. Analysis of the lungs for both agents confirmed this pattern of retention. The lungs of beryllium metal-exposed rats displayed a hemorrhagic, exudative pneumonitis, with an influx of neutrophils, and later, progressive fibrosis accompanied by macrophage and epithelial cell hyperplasia. Enhanced 239PuO2 retention will increase the radiation dose to the lung and may result in an eventual synergistic neoplastic response in rats exposed to the two agents

  7. Artificial neural networks applied in the spectrometry of a 239Pu-Be source

    To explore the potential use of a neutron source and to define the procedure to handle it under safety conditions, features like neutron spectrum and the ambient dose equivalent of the source must be known. The aim of this work was to determine the spectrum, the total fluence rate and the ambient dose equivalent of a 185 GBq 239Pu-Be neutron source. Using Monte Carlo methods the spectrum, the total fluence rate, and the ambient dose equivalent of a 239Pu-Be were calculated. The spectrum was calculated at 50, 100, 200 and 300 cm from the source in air using MCNP X and MCNP 4C codes. The neutron spectrum was also obtained, at 100 cm, using a Bonner sphere spectrometer whose count rates were used to unfold the neutron spectrum, the unfolding was carried out using an Artificial Neural Network for neutron spectrometry. With the spectrum, the total neutron fluence and the ambient dose equivalent were determined. Calculated results were compared with measured values where Monte Carlo results were smaller than those measured. These differences were attributed to the presence of 241Pu during the source manufacturing. In order to match calculated and measured quantities a 0.102 w/o of 241Pu was estimated. After corrections the differences between calculated and experimental results were 1%. This result shows the advantages of using Artificial Neural Networks technology in the unfolding of neutron spectrum using as a single piece of information the count rates of a Bonner sphere spectrometer. (author)

  8. Alligator Rivers Analogue project. Geochemistry of 239Pu, 129I, 99Tc and 36Cl

    One objective of this research programme has been to evaluate the applicability of uranium orebodies as natural analogues for testing radionuclide release-rate models used in performance assessment activities. The investigated nuclides included three of the most persistent radioactive constituents of high-level wastes from nuclear fission power reactors: plutonium-239, iodine-129, and technetium-99. The feasibility of uranium minerals as analogues for the behavior of these nuclear reaction products (NRP) in spent fuel relies upon a capability to characterise NRP concentrations in the source minerals. Measured abundances of natural 239Pu, 99Tc and 129I in uranium ores are compared to calculated abundances in order to evaluate the degree to retention of these radionuclides by the ore. This modelling study also shows the extent to which various NRP are correlated, such that one provides a constraint on the production rates of others. Under most conditions, 36Cl, another long-lived neutron-capture product found in uranium ores, is shown to be an ideal in-situ monitor of the 235U fission rate, which is the dominant source term for 129I and possibly a significant one for 99Tc. Similarly, 239Pu/U ratios can be used to establish limits on the 238U neutron-induced fission rate; the ratios measured in this study suggest that 238U induced fission comprises 129I and 99Tc. 79 refs., 21 tabs., 18 figs

  9. Comparison of early mortality in baboons and dogs after inhalation of 239PuO2

    Results from experiments with baboons were compared with those from experiments with dogs to determine the relative sensitivity of the two species to early mortality from inhaled 239PuO2. To ensure a valid comparison of data developed at two laboratories, methodology differences were minimized by establishing a common pool of raw data, using the same computer programs to analyze the data, and standardizing assumptions regarding the calculation of plutonium concentration in lungs. Several comparison methods were used involving variations in estimating different parameters used in these calculations. Although nearly all comparisons suggested baboons were slightly more sensitive, none of the methods for comparing the relationship between dose and survival time showed consistently significant differences between baboons and dogs. Although the baboons were physiologically and morphologically immature when exposed to plutonium, whereas the dogs were mature, we concluded that adult baboons and dogs are similarly sensitive to the early effects of inhaled 239PuO2. Since only early mortality was considered in this comparison, the results do not apply to possible late effects caused by much lower levels of plutonium than were used in these experiments

  10. Preliminary evaluation of lung doses for dogs exposed to 239PuO2

    A group of beagle dogs exposed to inhaled 239PuO2 is being followed for life-span effects. This paper reports preliminary lung dose estimates and dose-response relationships for incidence of lung tumors and radiation pneumonitis which have been observed to date. Doses were estimated by using both conventional dose-averaging and microdosimetric techniques. Cascade impactor sampling data were used to reconstruct the original plutonium aerosol size distributions unique to each of about 120 individual dogs exposed to 239PuO2. Data providing the initial plutonium lung burden and lifetime lung retention-clearance functions of plutonium for each dog were used for calculating average dose rates, cumulative absorbed doses, and specific energy distributions. A linear dose-response relationship for lung tumor induction was estimated on the basis of cumulative lung dose. Average time to death was estimated as a function of average dose rate. Conclusions regarding the potential value of microdosimetry in the interpretation of such dose-response relationships are discussed. 8 refs., 5 figs., 1 tab

  11. Lymphocytopenia induced in beagle dogs by inhalation of 239PuO2

    To determine the life-span dose-effect relationships of inhaled plutonium, we gave 124 beagle dogs a single exposure of 239PuO2 2 to 3 years ago at six different levels, i.e., 4, 20, 80, 300, 1100, or 5800 nCi mean initial alveolar depositions. Another group (20 dogs) served as controls. All dogs were about 18 months old. At the four highest exposure levels, a chronic lymphocytopenia developed which correlated with the initial alveolar plutonium burden in regard to magnitude of depression and time of development after exposure. The nadir occurred near 10 months after exposure in dogs receiving 5800, 1100, and 300 nCi, with corresponding lymphocyte levels 40, 55, and 75 percent, respectively, of those observed in control dogs. In the 80-nCi level the nadir occurred about 2 years after exposure at approximately 80 percent of control values. At the two lowest doses, i.e., 4 and 20 nCi, no effect on lymphocyte concentrations was noted 3 years after exposure. The persistent lymphocytopenia related to plutonium inhalation may be of significance in the subsequent development of pulmonary neoplasms previously observed in beagles at this laboratory 8 to 11 years after initial lung depositions of 200 to 1000 nCi of 239Pu

  12. Comparison of acute mortality in baboons and dogs after inhalation of 239PuO2

    Results from experiments with baboons were compared with those from experiments with dogs to determine the relative sensitivity of the two species to acute mortality from inhaled 239PuO2. To assure a valid comparison of data developed at two laboratories, methodology differences were minimized by establishing a common pool of raw data, using the same computer programs to analyze the data, and standardizing assumptions regarding the calculation of radiation doses to lungs. Several comparison methods were used involving variations in estimating different parameters such as the concentration of plutonium in the lungs. Although nearly all comparisons suggested baboons were slightly more sensitive, none of the methods for comparing the relationship between dose and survival time showed consistently significant differences between baboons and dogs. Although the baboons were physiologically and morphologically immature when exposed to plutonium, whereas the dogs were mature, it was concluded that adult baboons and dogs are similarly sensitive to the acute effects of inhaled 239PuO2. Since only acute mortality was considered in this comparison, the results do not apply to possible late effects caused by much lower levels of plutonium than were used in these experiments

  13. Occurrence of bone cancer among young adult Beagles given 239Pu

    Two hundred thirty-five young adult Beagles of both sexes were each given a single intravenous injection of 239Pu-citrate at graded dose-levels averaging about 0.026 to 106 kBq/kg when they were about 1 1/2 years of age and were maintained for lifespan observation. An additional 133 young adult Beagles of both sexes were entered into the experiment as control animals. All of these animals have now died or have been removed from the colony, and the occurrence of skeletal malignancies has been determined from histological examination. There were a total of 85 radiographically apparent malignant bone tumors in 77 dogs given 239Pu, and there was one control animal that developed a skeletal malignancy. Most of these were osteosarcomas, but there were seven chondrosarcomas of bone, one liposarcoma of bone, and in addition, there was one plasma cell myeloma and one ameloblastoma (admantinoma). Only those dogs that survived to at least the minimum latent period for death with radiation-induced bone sarcoma are included in the tabulation. There appeared to be a linear relationship between the percent of dogs with bone tumor and the average skeletal dose up to a dose of about 1 Gy. All dose-levels with skeletal doses of about 2 Gy and greater exhibited close to 100% occurrence

  14. New data on the toxicity and translocation of inhaled 239PuO2 in baboons

    In 1973-1974, baboons were exposed to a polydispersed aerosol of 239PuO2, prepared at 10000C, at the Commissariat a l'Energie Atomique in France. The data published in 1978 for these baboons were used by Bair et al (1980), for comparison with those obtained in beagles exposed to 239PuO2 at the Pacific Northwest Laboratory, USA. Since our 1978 publication, 8 baboons have died or were killed by euthanasia when moribund, and 11 were still alive when the present report was drafted. Two of the eight baboons died of lung squamous cell carcinoma at 2171 and 2528 days respectively. The remaining 6 died of fibrosis, interstitial pneumonia or diseases unrelated to Pu toxicity. The relationship observed in the eight baboons between initial lung burden and survival time shows that their lifespan was longer than expected from the data curve based on the findings for the first 1000 days. However, this increased survival time was not observed if the lifespan was expressed as a function of the average lung burden. (author)

  15. Sources and Spatial Distribution of Metal Pollutants in Soils near the El Paso Smelter: A Forensic Study with Pb and Pu Isotopes.

    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 ( 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+240Pu activities, and hence contain most or all of the cumulative deposition inventory of smelter pollutants

  16. Study on plutonium isotopic analysis in environmental samples

    A method for determination of plutonium isotope ratio in environmental samples was investigated in our laboratory. Plutonium was separated with complex matrix and purified by using TEVA extraction chromatography resin, and determined by MC-ICP-MS. The elution of Pu from TEVA column was tested. Plutonium could be eluted from TEVA column effectively by 0.025mol·l-1 H2C2O4-0.15mol·l-1HNO3 or 10-2 mol·l-1 ascorbic acid- 0.2 mol·l-1HNO3. For one TEVA column, the decontamination factors of main environmental matrix , such as Na, K, Ca, Al, Fe, Mg, were between 104-105, and the concentration of total cation ions in the final elution was less than 10 μg·g-1, which could be determined by MC-ICP-MS directly. The decontamination of U, Th and Am was also examined, DFU/Pu=1.97x103, DFTh/Pu=7.19 x 104, DFAm/Pu=1.52x104 were obtained. The chemical recovery of plutonium during the whole process was ∼ 30%. Because of the tailing of 238U and the formation of 238UH+ while the determination of plutonium isotope by MS, it was not enough for the decontamination of uranium by using one TEVA column. A UTEVA column was needed before the solution loading in the TEVA resin. The decontamination factor of uranium could reach 1.33x106. The detection limit of Pu by MC-ICP-MS was about 2.5 fg·ml-1. The influence of U on the determination of plutonium isotope ratio was also examined. For the solution containing less than 1 ng·g-1 uranium, Aridus sample introduction system was adopted to improve the sensitivity. Meinhard PFA nebulizer was used for solutions of high uranium concentration (1- 500 ng·g-1). The results show that, the 238UH+/U+ is about 8.9x10-5 for the high content of uranium, and about 3.6x10-4 for the low content. According to the method mentioned above, two IAEA reference materials, IAEA-368 and SOIL-6 were analyzed. Purified Pu fractions were obtained by using UTEVA+TEVA extraction chromatography; 240Pu/239Pu were determined by MC-ICP-MS. The results were shown. Ocean

  17. Study on plutonium isotopic analysis in environmental samples

    A method for determination of plutonium isotope ratio in environmental samples was investigated in our laboratory. Plutonium was separated with complex matrix and purified by using TEVA extraction chromatography resin, and determined by MC-ICP-MS. The elution of Pu from TEVA column was tested. Plutonium could be eluted from TEVA column effectively by 0.025mol·l-1 H2C2O4-0.15mol·l-1HNO3 or 10-2 mol·l-1 ascorbic acid-0.2mol·l-1HNO3. For one TEVA column, the decontamination factors of main environmental matrix , such as Na, K, Ca, Al, Fe, Mg, were between 104-105, and the concentration of total cation ions in the final elution was less than 10 μg·g-1, which could be determined by MC-ICP-MS directly. The decontamination of U, Th and Am was also examined, DFU/Pu=1.97x103,DFTh/Pu=7.19x104,DFAm/Pu=1.52x104 were obtained. The chemical recovery of plutonium during the whole process was ∼30%. Because of the tailing of 238U and the formation of 238UH+ while the determination of plutonium isotope by MS, it was not enough for the decontamination of uranium by using one TEVA column. A UTEVA column was needed before the solution loading in the TEVA resin. The decontamination factor of uranium could reach 1.33x106. The detection limit of Pu by MC-ICP-MS was about 2.5 fg·ml-1. The influence of U on the determination of plutonium isotope ratio was also examined. For the solution containing less than 1 ng·g-1 uranium, Aridus sample introduction system was adopted to improve the sensitivity. Meinhard PFA nebulizer was used for solutions of high uranium concentration(1-500 ng·g-1). The results show that, the 238UH+/U+ is about 8.9x10-5 for the high content of uranium, and about 3.6x10-4 for the low content. According to the method mentioned above, two IAEA reference materials, IAEA-368 and SOIL-6 were analyzed. Purified Pu fractions were obtained by using UTEVA+TEVA extraction chromatography; 240Pu/239Pu were determined by MC-ICP-MS. The results were showed in table 1. Ocean

  18. 239Pu(n,2n) 238Pu cross section inferred from IDA calculations and GEANIE measurements

    Chen, H; Ormand, W E; Dietrich, F S

    2000-09-01

    This report presents the latest {sup 239}Pu(n,2n){sup 238}Pu cross sections inferred from calculations performed with the nuclear reaction-modeling code system, IDA, coupled with experimental measurements of partial {gamma}-ray cross sections for incident neutron energies ranging from 5.68 to 17.18 MeV. It is found that the inferred {sup 239}Pu(n,2n){sup 238}Pu cross section peaks at E{sub inc} {approx} 11.4 MeV with a peak value of approximately 326 mb. At E{sub inc} {approx} 14 MeV, the inferred {sup 239}Pu(n,2n){sup 238}Pu cross section is found to be in good agreement with previous radio-chemical measurements by Lockheed. However, the shape of the inferred {sup 239}Pu(n,2n){sup 238}Pu cross section differs significantly from previous evaluations of ENDL, ENDF/B-V and ENDF/B-VI. In our calculations, direct, preequilibrium, and compound reactions are included. Also considered in the modeling are fission and {gamma}-cascade processes in addition to particle emission. The main components of physics adopted and the parameters used in our calculations are discussed. Good agreement of the inferred {sup 239}Pu(n,2n){sup 238}Pu cross sections derived separately from IDA and GNASH calculations is shown. The two inferences provide an estimate of variations in the deduced {sup 239}Pu(n,2n){sup 238}Pu cross section originating from modeling.

  19. The isotopic signature of fallout plutonium in the North Pacific

    Plutonium analyses of a dated coral record from the French Frigate Shoals in the central North Pacific indicate that there are two major sources of Pu in this basin: close-in (tropospheric) fallout from nuclear weapons testing at the Pacific Proving Grounds in the Marshall Islands in the 1950s and global (stratospheric) fallout which peaked in 1962. Furthermore, the 240Pu/239Pu atom ratio of fallout from the Pacific Proving Grounds is characteristically higher (0.24) than that of global fallout Pu (0.18-0.19). Seawater and sediment samples from the North Pacific exhibit a wide range of 240Pu/239Pu values (0.19-0.34), with a trend towards higher ratios in the subsurface waters and sediment. Deep water 240Pu/239Pu ratios are higher in the vicinity of the Marshall Islands relative to stations further from this close-in fallout source. These preliminary data suggest that fallout Pu from the Pacific Proving Grounds is more rapidly removed from the surface waters than is global fallout Pu. Plutonium geochemistry appears to be related to the physical/chemical form of Pu-bearing particles generated by different fallout sources. (author)

  20. ZZ JFS-1, Cross-Sections Library 25-Groups ABBN and 70-Group JFS for Fast Reactor Calculation. ZZ JFS-2, 25 Group (ABBN) and 70 Group JFS Cross Sections Library for Fast Reactors. ZZ JFS-3/J2, 70 Group 30 Isotopes Cross Section Library for Fast Reactors

    1 - Description of problem or function: - JFS-V2-1: Format: ABBN energy structure; Number of groups: 25 group constants; Nuclides: Be, B-10, B-11, C, O, Na, Al, Si, Cr, Mn, Fe, Ni, Cu, Mo, Th-232, U-233, U-234, U-235, U-236, U-238, Pu-239, Pu-240, Pu-241, Pu-242, Am-241, fission products of U-235, and fission products of Pu-239. Origin: ENDF/B-IV; Weighting spectrum: The cross-section adjustment has been made by using an auxiliary equation for simultaneous evaluations for U-235, U-238, and Pu-239. - JFS-V2-2: Format: JFS energy structure; Number of groups: 70 group constants; Nuclides: Be, B-10, B-11, C, O, Na, Al, Si, Cr, Mn, Fe, Ni, Cu, Mo, Th-232, U-233, U-234, U-235, U-236, U-238, Pu-239, Pu-240, Pu-241, Pu-242, Am-241, fission products of U-235, and fission products of Pu-239. Origin: ENDF/B-IV; Weighting spectrum: The cross-section adjustment has been made by using an auxiliary equation for simultaneous evaluations for U-235, U-238, and Pu-239. - JFS-3/J2: Number of groups: 70 group constants with quarter-lethargy width; Nuclides: H-1, He-4, Be-9, B-10, B-11, C-12, N-14, O-16, Na-23, Al-27, Si, Ar, Ti, V, Cr, Mn-55, Fe, Ni, Cu, Zr, Nb-93, Mo, Eu-151, Eu-153, Gd, Gd-155, Gd-156, Gd-157, Gd-158, Gd-160, Ta-181, W, Th-228, Th-230, Th-232, Th-233, Th-234, Pa-233, U-233, U-234, U-235, U-236, U-238, Np-237, Np-239, Pu-236, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, Am-241, Am-242m, Am-242g, Am-243, Cm-242, Cm-243, Cm-244, Cm-245 and 12 LFPs for 4 mother nuclides (U-235, U-238, Pu-239 and Pu-241) and 3 burnup days (180, 1080 and 1800). Origin: JENDL-2 and ENDF/B-V; Weighting spectrum: the collision density spectrum for a typical large LMFBR core spectrum is used as the weighting function. ZZ-JFS-3/J2: To improve fast reactor group constant set JFS-3-J2 to be applicable for high burnup reactor calculation, burnup depending lumped FP group cross sections for mother fission isotopes of U-235, U-238, Pu-239 and Pu-241 have been generated by using 155 FP nuclides of JENDL-2

  1. Investigation of forming mechanism of instantaneous neutron spectrum of 235U, 239Pu, 252Cf nuclei fission

    Formation mechanism of prompt neutrons spectrum during the fission of the 235U, 239Pu nuclei by thermal and fast neutrons and spontaneous fission of 252Cf is investigated. The formation procedure for prompt neutrons spectrum during the fission of nuclei as superposition of three partial evaporation Weisskopf spectra with the mean energy of neutrons 0.4, 2.06 and 2.8 MeV is proposed. Formation mechanism of the spectrum just as during the fission of the 235U, 239Pu nuclei by thermal and fast neutrons, so spontaneous fission of the 252Cf nuclei is identical

  2. In vitro dose-response of macrophages to 239PuO2 and 241AmO2

    As part of a study designed to examine various means of solubilizing actinide particles within macrophages, we have measured the in vitro effects of 241AmO2 and 239PuO2 on these cells. Dose distribution within the cell population was estimated by autoradiography and compared to cell detachment as a function of time. The 241AmO2 and 239PuO2 were toxic in proportion to their radioactivity rather than their mass. Approximately 385 intracellular disintegrations are required from either radionuclide to cause cells to detach from the flask surface

  3. The Pöschl Teller model for total cross section of neutron scattering from 240Pu

    Neutron scattering cross-section of 240Pu have been investigated using an attractive potential. On applying the modified Pöschl-Teller model, the total cross-section of the n+240Pu in the energy range of 5-20 MeV have been calculated. It was compared with the available experimental data and evaluated data of JENDL-4.0, ENDF/B-VII.0 and CENDL-3.1 as well as with the theoretical values from TALYS-1.2 Nuclear Reaction Program, EMPIRE: 2.19 Nuclear Reaction Model Code and are found to be in reasonably good agreement. This supports the validity of the present calculation. (author)

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

    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 ).

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

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

    2010-03-31

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

  6. Pulmonary distribution of inhaled 239PuO2 in dogs

    The distribution of plutonium in the lungs was studied by analyzing autoradiographs from dogs killed up to 69 months after single, nose-only exposures to 239PuO2 aerosols. Within 5 months of exposure, the pattern of alpha-star distribution was relatively dispersed and uniform throughout the lung section, changing by 12 months to a less uniform distribution that exhibited focal concentration, subpleural concentration, and alpha-star aggregation. Increased subpleural concentrations were demonstrated infve of six dogs killed 12 or more months after exposure. The percentage of alpha stars found in localized regions of relatively high concentration and the portion found in aggregation (define here as two or more alpha stars with overlapping tracks) increased with tie postexposure. The data demonstrate that an initial relatively uniform dispersion of plutonium particles changed with time to a focally concentrated distribution with relatively small tissue volume containing most of the pulmonary plutonium burden

  7. Toxicity of inhaled 239PuO2 in immature beagle dogs

    Immature beagle dogs have been exposed by inhalation to a 1.5 μm aerodynamic diameter monodisperse aerosol of 239PuO2 to compare the biological effects with those seen in young adult and aged dogs exposed to a similar aerosol. To date, 18 dogs have been exposed to the aerosol, resulting in graded initial lung burdens ranging from 0.003 to 0.38 μCi/kg body weight. Two dogs have been exposed to the aerosol diluent and serve as controls. Two of the 18 exposed animals were sacrificed 8 days after exposure to provide information on initial deposition and distribution. All other exposed animals are alive 400 days after exposure. No dogs were exposed during the past year because of an outbreak of canine parvovirus enteritis which caused death in 8 to 10 week-old dogs

  8. Comparison of rats and dogs exposed to 239PuO2

    Rats and dogs inhaled aerosols of 239PuO2 at comparable ages relative to their lifespan. Both received a single exposure. The estimated lung doses at death in dogs were between 1100 and 11,000 rad. From two inhalation experiments, rats receiving doses in this range were chosen from the high-level exposed animals for comparison. Based on this data base, several comparisons were investigated. Metabolism of the material was compared for all animals and for animals which developed lung tumors. The differences in histopathology and tumor incidence in the lung were also reviewed. Although there were several differences between species, there were also many similarities. On-going research in dogs should produce data which will allow clarification of these relationships

  9. Quantitative scanning electron microscopic autoradiography of inhaled 239PuO2

    We have applied the scanning electron microscope (SEM) to obtain autoradiographs of particles of 239PuO2 deposited in rat lung. The technique was used to obtain quantitative information on the clearance rates of particles from the alveoli, bronchioles and trachea up to 240 d after exposure. At all times, the concentration of particles on the surface of the bronchioles was an order of magnitude greater than on the tracheal surface. The clearance of Pu from both regions followed a biphasic pattern, similar to that obtained by radiometric analysis of the whole lung. Most of the radiation dose to the bronchiolar epithelium originated from Pu particles in peribronchiolar alveoli in which they were preferentially retained, compared to other alveolar regions. The prolonged retention of particles in the peribronchiolar alveoli may be a significant factor in the induction of lung carcinomas

  10. Aerosols generated by 239PU and 233U droplets burning in air

    The inhalation hazards of radioactive aerosols produced by the explosive disruption and subsequent combustion of metallic plutonium in air are not adequately understood. Results of a study to determine whether uranium can be substituted for plutonium in such a situation in which experiments were performed under identical conditions with laser-ignited, single, freely falling droplets of 239Pu and 233U are reported. The total amounts of aerosol produced were studied quantitatively as a function of time during the combustion. Also, particle size distributions of selected aerosols were studied with aerodynamic particle separation techniques. Results showed that the ultimate quantity of aerosols, their final particle size distributions, and depositions as a function of time are not identical mainly because of the different vapor pressures of the metals, and the unlike degrees of violence of the explosions of the droplets

  11. The simultaneous determination of 235U and 239Pu using delayed neutron activation analysis

    Delayed neutron activation analysis (DNAA) remains one of the most sensitive methods of nondestructively determining fissile materials in a variety of sample matrices, provided that the samples contain only a single fissile component. This has historically been the limiting factor in many applications of DNAA, and often chemically destructive methods of analysis have needed to be utilized for many real-world samples. This work seeks to develop a method that will allow for DNAA to be utilized on samples containing multiple fissile components. Initial efforts, presented here, show that using a multivariate linear regression model to describe the delayed neutron emission profile of an irradiated sample allows for the concurrent determination of fissile nuclides in samples containing both 235U and 239Pu, without chemical separations and using only a single counting step. (author)

  12. Measurement of the ${240}$Pu(n,f) reaction cross-section

    Following proposal CERN-INTC-2010-042 / INTC-P-280 (“Measurement of the fission cross-section of $^{240}$Pu and $^{242}$Pu at CERN’s n_TOF Facility”), the parallel measurement of the $^{240}$Pu(n,f) and $^{242}$Pu(n,f) reaction cross-sections was carried out at n_TOF EAR-1. While the $^{242}$Pu measurement was successful, unexpected sample-induced damage to the detectors caused by the high α-activity of the 240Pu samples resulted in a deterioration of the detector performance over the data taking period of several months, which compromised the measurement. This obstacle can be eliminated by performing the measurement in EAR-2, where the higher neutron flux will allow collecting data in a much shorter time, thus preventing the degradation of the detectors. In addition to this obvious advantage, the measurement would also benefit from the stronger suppression of the sample-induced α-background, due to the shorter times-of-flight involved.

  13. A comparative study of the carcinogenetic effects of 241Am, 239Pu and 237Np

    In this experiment, 420 wistar rats were used to study the comparative carcinogenetic effects of 241Am, 239Pu and 237Np. These nuclides were injected to animals intravenously, subcutaneously or directly into the lung (Stansen's lung puncture method) in doses of 1.0, 5.0 and 8.5 μCi/kg, respectively. As soluble nitrate, the nuclides were rapidly transfered from the site of injection into the bone and the liver. Osteosarcomas were found in some animals 8 months to one year after intoxication. Diagnosis of osteosarcoma is based on the histopatological examination and X-ray photography. In the Am-poisoned rats the incidence of osteosarcoma is about 31-74%, varied with different doses and different routes of intoxication; in Pu-poisoned rats, the incidence of osteosarcoma is about 55-66%. while in Np-poisoned rats, it is about 36-53%. Primary lung cancers were also found in those animals poisoned by means of Stansen's lung puncture method with the above three nuclides. The incidence of primary lung cancers is about 6% in Am-and Pu-poisoned rats and 13% in Np-poisoned rats. The incidence of metastasis of osteosarcoma in lung is about 25-65% for Am-poisoned rats, 45-55% for Pu-poisoned rats and 41-80% for Np-poisoned rats. The life-span of above poisoned rats was significantly shorter than that of the normal control animals. The chemical weight for 241Am, 239Pu and 237Np in same unit of radioactivity (1.0 μCi) equals to 0.308 μg, 15.9 μg and 1418.7 μg, respectively. For this reason, we have to pay more attention to the chemical mass effect in carcinogenesis of the above three nuclides

  14. Dosimetry and response in rat pulmonary epithelium following inhalation of 239PuO2

    The distribution of inhaled 239PuO2 and pathologic changes have been studied in the lung of rats. The clearance of inhaled 237239PuO2 from the lung is a function of the amount of deposited Pu with a decrease in early alveolar clearance with increasing lung burden. With increasing time post-exposure there is a greater concentration of PuO2 and an increased aggregation of PuO2 particles in subpleural regions of the lung. Fibrotic and metaplastic lesions in the lung were usually focal, being found in subpleural regions associated with aggregates of PuO2. An average of 12 +- 6 percent of the lung volume was fibrotic at 530 days after an initial alveolar deposition of 180 nCi 239Pu. Lung tumors occupied 4 +- 6 percent and epithelial metaplasias less than 1 percent of the lung volume at this time. Cell proliferation as assayed by tritiated thymidine autoradiography was greater in fibrotic, metaplastic and neoplastic regions than in areas of normal alveolar-bronchiolar epithelium. Turnover times ranged from about 6 days for fibrotic lesions to 1 to 3 days for metaplastic and neoplastic lesions. The lung tumor doubling times were 57 to 116 days due to tumor cell necrosis and other factors that limit tumor cell survival. Cell proliferation rates for adenomatous metaplasia were similar to those for adenocarcinoma while those for squamous cell metaplasia were similar to those for squamous cell carcinoma. Squamous lesions exhibited a more rapid growth than did adenomatous lesions

  15. Comparison of metabolism and late effects in dogs and rats exposed to 239PuO2

    Lung tumors were observed proportionally earlier in relation to expected life span in dogs than in rats after inhalation of 239PuO2. Dogs appear to translocate a higher percentage of initial lung burden to liver, skeleton and thoracic lymph nodes than rats

  16. Initial deposition and early clearance of inhaled 239Pu(NO3)4 aerosols in beagle dogs

    Data from exposures of 113 beagle dogs to 239Pu(NO3)4 aerosols were analyzed for effects of aerosol properties on deposition and early clearance. The percent of inhaled aerosols deposited was not significantly dependent on particle size or aerosol concentration. The early clearance rate was significantly slower at the highest exposure levels than at medium and low levels

  17. Spatial statistical analysis of contamination level of 241Am and 239Pu, Thule, North-West Greenland

    Strodl Andersen, J. (JSA EnviroStat (Denmark))

    2011-10-15

    A spatial analysis of data on radioactive pollution on land at Thule, North-West Greenland is presented. The data comprises levels of 241Am and 239,240Pu on land. Maximum observed level of 241Am is 2.8x105 Bq m-2. Highest levels were observed near Narsaarsuk. This area was also sampled most intensively. In Groennedal the maximum observed level of 241Am is 1.9-104 Bq m-2. Prediction of the overall amount of 241Am and 239,240Pu is based on grid points within the range from the nearest measurement location. The overall amount is therefore highly dependent on the model. Under the optimal spatial model for Narsaarsuk, within the area of prediction, the predicted total amount of 241Am is 45 GBq and the predicted total amount of 239,240Pu is 270 GBq. (Author)

  18. Effect of alpha irradiation of the lungs from inhaled 239PuO2 on the immunity of mice to Listeria monocytogenes

    The pulmonary clearance of inhaled Listeria monocytogenes from the lungs of nonimmunized and immunized mice was observed 3 to 4 or 26 wks after prior exposure to 239PuO2 to achieve initial lung burdens of 2.6, 5.0 and 11.9 nanocuries (nCi). Mice from 239PuO2 and sham-exposed groups were immunized against L. monocytogenes and 1 wk later challenged via the respiratory route. Pulmonary clearance was suppressed in mice with an 11.9 nCi initial lung burden of 239Pu 26 wk after 239PuO2 inhalation but not in the mice with initial lung burdens of 2.6 and 5.0 nCi at 4 to 5 or 27 wk after 239PuO2 exposure. Mice with a mean initial lung burden of 11.9 nCi of 239Pu, which were immunized against L. monocytogenes 26 wk after 239PuO2 inhalation, had a decreased survival after respiratory challenge with L. monocytogenes when compared to immunized control animals. Body weight gain and hematological differences did not correlate with suppressed pulmonary clearance or decreased survival. Pulmonary lavage studies indicated that fewer alveolar macrophages were recoverable from mice with a mean initial lung burden of 11.9 nCi of 239Pu 26 wk after 239PuO2 inhalation. It was concluded that an initial lung burden of 11.9 nCi of 239Pu which delivered approximately 700 rads of alpha radiation to the lungs of mice resulted in decreased pulmonary clearance and decreased survival of mice which had been immunized against L. monocytogenes

  19. Association of fallout-derived 137Cs,90Sr and 239,240Pu with natural organic substances in soils

    Activity concentrations and associations of fallout-derived Cs, Sr and Pu in soils were investigated. The activity concentrations of 137Cs, 90Sr and 239,240Pu in volcanic ash soil were much higher than those in granite soil. They decreased with increasing depth in the soil. The activity ratios of 239,240Pu/137Cs and 90Sr/137Cs tended to increase slightly with increasing soil depth. Alkali extraction experiments with 0.1 M NaOH solution showed that the percentage activities of the fallout radionuclides found in the organic acid fractions were in the order 239,240Pu>90Sr>137Cs. The concentrations of 137Cs and 239,240Pu reacted with humic fractions were higher than those with fulvic fractions. In contrast to 137Cs and 239,240Pu,90Sr reacted more with fulvic fractions than with humic fractions. These results provide information about the effects of organic substances on the retention and migration of 137Cs,90Sr and 239,240Pu in soils under natural conditions

  20. The coagulation of dissolved sup(239,240)Pu in estuaries as determined from a mixing experiment

    A mixing experiment, using large volumes (100 l) of filtered (240Pu during estuarine mixing. An organic-rich freshwater with a relatively high concentration (0.8 dpm/100 l) of dissolved sup(239,) 240Pu was used as one end-member; Buzzards Bay seawater (dissolved sup(239,) 240Pu=0.04 dpm/100 l) was the other. The results demonstrate that dissolved sup(239,) 240Pu in the freshwater undergoes extensive and rapid coagulation under simulated estuarine conditions. There is a strong correlation between the amount of coagulation of dissolved sup(239,) 240Pu, humic acids (HA), and Fe. The extent of coagulation of all three constituents increases with increasing salinity and the net extent of their removal is 53%, 57%, and 100% for Pu, HA, and Fe respectively. As has been domented for Fe in freshwater, dissolved sup(239,) 240Pu appears to be stabilized by naturally occurring humic substances to form negatively charged colloids which are then coagulated by seawater cations. The extrapolation of these experimental results to real estuaries will require additonal research. (orig.)

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

    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.

  2. A study of in-line plutonium isotopic analysis for gaseous plutonium hexafluoride

    In-line plutonium isotopic analysis of gaseous plutonium hexafluoride (PuF6) is very important for process control and special nuclear material accountability in any plutonium-isotope-separation process that requires a gaseous phase. Although much effort had been devoted to analyze arbitrary plutonium samples, no isotopic analysis had been done on gaseous PuF6 samples. We have initiated a study on the use of a high-resolution, gamma-ray spectroscopy technique to analyze gaseous plutonium hexafluoride. For the first time, PuF6 gas samples with pressures varying from 0.15 to 31 torr, which were directly fed into a gas cell from a process flow loop, were measured. The isotopic results of these measurements agree very well with those of mass spectrometry measurements of solid PuF4. The precision of a 10-min measurement of a 10-torr reactor-grade PuF6 is 1.5% for 238Pu, 0.22% for 239Pu, 0.87% for 240Pu, and 17.5% for 241Pu

  3. 239Pu Prompt Fission Neutron Spectra Impact on a Set of Criticality and Experimental Reactor Benchmarks

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

    2014-04-01

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

  4. A 233U/236U/242Pu/244Pu spike for isotopic and isotope dilution analysis by mass spectrometry with internal calibration

    The Khlopin Radium Institute prepared on behalf of the IAEA a synthetic mixture of 233U, 236U, 242Pu and 244Pu isotopes. The isotopic composition and elemental concentration of uranium and plutonium were certified on the basis of analyses done by four laboratories of the IAEA Network, using mass spectrometry with internal standardization. The certified values for 233U/236U ratio and the 236U chemical concentration have a coefficient of variation of 0.05%. The latter is fixed by the uncertainty in the 235U/238U ratio of NBS500 used as internal standard. The coefficients of variation of the 244Pu/242Pu ratio and the 242Pu chemical concentration are respectively 0.10% and 0.16% and limited by the uncertainty in the 240Pu/239Pu ratio of NBS947. This four isotope mixture was used as an internal standard as well as a spike, to analyze 30 batches of LWR spent fuel solutions. The repeatability of the mass spectrometric measurements have a coefficient of variation of 0.025% for the uranium concentration, and of 0.039% for the plutonium concentration. The spiking and treatment errors had a coefficient of variation of 0.048%. (author). Refs, figs and tabs

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

    Sadhukhan, Jhilam; Schunck, Nicolas

    2016-01-01

    In this letter, we outline a methodology to calculate microscopically mass and charge distributions of spontaneous fission yields. We combine the multi-dimensional 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 characteristics.

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

    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. {sup 239+240}Pu in the Barents Sea Regions. Sources and radioecological assessment

    Iosjpe, Mikhail [Norwegian Radiation Protection Authority, P.O. Box 55, N-1332 Oesteraas (Norway)

    2014-07-01

    The radioecological assessment for {sup 239+240}Pu in the Barents sea regions was made using the compartment modelling approach. The following sources of radioactive contamination were under consideration: global fallout from atmospheric testing of nuclear weapons, transport of {sup 239+240}Pu from the Sellafield and La Hauge nuclear plants and underwater testing of nuclear weapons in Chernaya Bay, Novaya Zemlya. The box model developed at NRPA uses a modified approach for compartmental modeling, which takes into account the dispersion of radionuclides over time. The box structures for surface, mid-depth and deep water layers have been developed based on the description of polar, Atlantic and deep waters in the Arctic Ocean and the Northern Seas, as well as site-specific information for the boxes. The volume of the three water layers in each box has been calculated using detailed bathymetry together with Geographical Information Systems. The box model includes the processes of advection of radioactivity between compartments, sedimentation, diffusion of radioactivity through pore water in sediments, resuspension, mixing due to bioturbation, particle mixing and a burial process for radionuclides in deep sediment layers. Radioactive decay is calculated for all compartments. The contamination of biota is further calculated from the known radionuclide concentrations in filtered seawater in the different water regions. Doses to man are calculated on the basis of seafood consumptions, in accordance with available data for seafood catches and assumptions about human diet in the respective areas. Dose to biota are determined on the basis of calculated radionuclide concentrations in marine organisms, water and sediment, using dose conversion factors. Results of the calculations show that atmospheric deposition is the dominant source for the Barents Sea, except for the Chernaya Bay region. It is also demonstrated that the impact of the Sellafield nuclear facilities has

  8. Annular cylinders experimental programme containing plutonium solutions at different 240Pu contents

    From 1963 to 1976, 730 critical experiments dealing with annular cylinders containing plutonium nitrate solutions were conducted on Valduc critical facility, called 'Apparatus B'. They aimed at validating critical configurations encountered in the fuel cycle, especially in storage and also at validating the 240Pu cross-sections in thermal neutron spectrum. It is to be noticed that these experiments validate criticality codes either in configurations with reactor-grade plutonium coming from the reprocessing cycle or with weapon-grade plutonium coming from the decommissioning of nuclear weapons. (authors)

  9. Incidence of liver tumors in beagles with body burdens of 239Pu or 241Am

    Tetravalent 239Pu or trivalent 241Am in a citrate buffer, given via a single intravenous injection to beagles, induced very pronounced liver changes, usually at relatively long postinjection times. The lesions consisted of cell injury or cell necrosis which was followed by nodular hyperplasia and a significant incidence of primary liver tumors. The most frequent neoplasm was the bile duct adenoma, followed by the bile duct carcinoma. A lesser number of sarcomas were also induced, especially fibrosarcomas. The number of hepatic cell tumors was low. An abnormally high incidence of both hyperplastic nodules and primary liver tumors occurred at long postinjection times and at average doses extending down to ∼10 rads. The various nodular lesions and liver tumors frequently occurred as incidental findings in dogs dying from other causes, especially bone cancer. In comparison to bone neoplasia, the liver was a much less important target organ in the high-dose level groups, but in some of the low-dose groups, especially in the 241Am groups, the risk of radiation-induced liver cancer was approximately equal to or exceeded the risk of skeletal tumors. However, in any projection of the risks observed in this animal model to man, one should be mindful that the beagle skeleton is approximately 25 times more sensitive to radiation-induced bone neoplasia than is the human skeleton (Mays et al., 1976) and that the radiosensitivity difference for the beagle and human liver is unknown. 41 refs., 8 figs., 5 tabs

  10. Distribution of 239Pu and 241Am in the human skeleton

    The 241Am and 239Pu distribution in the skeletons of two former nuclear workers has been measured. The skeletons of both individuals appear to be within normal limits for Caucasian men about 50 y old. Both had lower limb bones that were heavier than the age controls and Case I had upper-body bones that were lighter than the age control group. The distribution of americium in the skeleton of Case I, 25 years post exposure, indicated that a more rapid turnover of initially deposited americium on the bone surfaces of cancellous bone, as compared to that deposited on the bone surfaces of compact bone, had occurred. This resulted in a larger proportion of americium located in the compact bone of the extremities and a lesser quantity in the more cancellous bones of the vertebral column, pelvis and rib cage. A similar shift in the distribution of plutonium occurred in Case II in the 35 y since initial deposition, but at a slower rate than that for americium. The ratio of each actinide in the liver to that in the systemic system (liver content/systemic system content) was 0.065 and 0.436, for americium and plutonium, respectively, suggesting that a much more rapid turnover of americium in the liver, compared to plutonium, provided a much larger fraction of that nuclide for circulatory feedback to the remodeling skeletal system. 8 references, 3 tables

  11. Effects of the herbicide glyphosate on the uptake of 239Pu and 241Am to vegetation

    Glyphosate (n-phosphonomethyl glycine) is a broad spectrum herbicide widely used in lowland agriculture, forestry and improved upland pastures. Although its metal chelating properties are well established, its interaction with radionuclides remains unknown. A pot experiment was conducted to determine the effect of soil applications of glyphosate on the uptake of 239Pu and 241Am to peas and carrots grown in loam, peat and sand soils. Soil-to-plant transfer factors were calculated for treated and untreated soils at harvest. The most marked effect was an increase in 241Am uptake to crops grown in loam soil. Supplementary laboratory batch experiments were conducted by shaking radiolabelled soil and its associated soil solution with glyphosate. The activity concentration of 241Am increased ten fold in the liquid phase of loam soils treated with glyphosate. It is postulated that this 241Am desorption could have been mediated by the formation of a stable Am-glyphosate complex which was subsequently more available for crop uptake than Am alone. (author)

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

    Wen, Xianfei; Yang, Haori

    2016-06-01

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

  13. Effects of combined inhalation exposure of rats to 239PuO2 and beryllium metal

    We exposed rats acutely to achieve one of two initial lung burdens (ILBs) of 239PuO2 alone or in combination with one of three ILBs of beryllium metal. Additional control groups of rats were sham exposed to air. Currently, approximately 58% of all rats planned for inclusion have been exposed. This report describes procedures used for the exposure, maintenance, and evaluation of rats in this study. Most of the animals are to be held for their life span in order to quantitate cancer incidence, with other animals assigned to serial sacrifice groups for quantitation of Pu and Be retention and determination of translocation patterns. Exposure to beryllium at any of the three doses tested retarded clearance of plutonium from the lung by a factor of approximately six. Acute inflammatory responses were studied in a separate group of rats exposed to Be. Except for rats receiving the highest ILB of beryllium metal, no differences between exposed and sham-exposed control groups have yet been noted in terms of mortality, weight changes, and clinical signs. (author)

  14. Plutonium in Soils from Northeast China and Its Potential Application for Evaluation of Soil Erosion

    Xu, Yihong; Qiao, Jixin; Hou, Xiaolin;

    2013-01-01

    Surface and soil core samples from northeast China were analyzed for Pu isotopes. The measured 240Pu/239Pu atomic ratios and 239 1 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 an...

  15. Intercalibration of selected anthropogenic radionuclides for the GEOTRACES Program

    Kenna, Timothy C.; Masqué, Pere; Mas, Jose Luis;

    2012-01-01

    As part of the GEOTRACES Program, six laboratories participated in an intercalibration exercise on several anthropogenic radionuclides of interest. The effort was successful for 239,240Pu activity, 240Pu/239Pu isotope ratio, and 137Cs activity measured in filtered seawater samples from the Bermuda...

  16. Effects of combined exposure of F344 rats to inhaled 239PuO2 and a chemical carcinogen (NNK)

    Workers in nuclear weapons facilitates have a significant potential for exposure to chemical carcinogens and to radiation from external sources or from internally deposited radionuclides such as 239Pu. Although the carcinogenic effects of inhaled 239Pu and many chemicals have been studied individually, very little information is available on their combined effects. One chemical carcinogen that workers could be exposed to, via tobacco smoke, is the tobacco-specific nitrosamine 4-(N-Methyl-N-nitrosamino)-1-(3-pyridyl)-1-butanone (NNK), a product of the curing of tobacco and pyrolysis of nicotine in tobacco. NNK causes lung tumors in rats, regardless of the route of administration and to a lesser extent tumors in the liver, nasal passages, and pancreas. The purpose of this study is to characterize the effects of combined exposure of rats to NNK and internally deposited plutonium, as well as to these agents alone

  17. Pulmonary retention and tissue distribution of 239Pu nitrate in F344 rats and syrian hamsters inhaling carbon tetrachloride

    Carbon tetrachloride (CCl4) has been used extensively in the nuclear weapons industry, so it is possible that nuclear plant workers have been exposed to CCl4 and plutonium compounds. Potential for future exposure exists during open-quotes cleanupclose quotes operations at weapon production sites such as the Hanford, Washington, and Rocky Flats, Colorado, facilities. The current Threshold Limit Value for CCl4 is 5 ppm; however, concentrations of CCl4 occurring in the nuclear weapons facilities over the past 40-50 y are unknown and may have exceeded this value. The pilot study described in this report is designed to determine whether subchronic inhalation of CCl4 by CDFregister(F-344)/CrlBR rats and Syrian golden hamsters, at concentrations expected to produce some histologic changes in liver, alters the hepatic retention and toxic effects of inhaled 239Pu nitrate 239Pu(NO3)4

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

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

    2016-04-01

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

  19. Extrapolation to man of the relation between activity and damage to organism of laboratory animals internally contaminated with 239Pu

    The relations were analyzed between the initial amount of the radionuclide deposited and mortality. The mortality curves were analyzed using the Gompaertz relation and the exponential relation was found between the rate of the mortality changes and 239Pu activity. Using comparative analysis the results of the model were approximated to man and compared with data published in the literature on human contamination. The comparison did not exclude the validity of the applied model. (author)

  20. The pore water chemistry of sup(239,240)Pu and 137Cs on sediments of Buzzards Bay, Massachusetts

    The collection of large volumes of pore water and low level radiochemical measurements of sup(239,240)Pu and 137Cs have been combined to produce the first study of these fallout artificial radionuclides in marine pore waters. Profiles from box cores taken in June and September 1982 from Buzzards Bay, Mass., are reported along with profiles of many diagenetic constituents (i.e. SO42-, alkalinity, Fe, Mn, DOC, and nutrients). The sup(239,240)Pu pore water profile is characterized by a subsurface maximum of about 0.28 dpm/100 kg lying between 3 to 11 cm. Overlying seawater, in contrast, has an activity of 0.01 +- 0.02 dpm/100 kg. Below about 11 cm, the pore water sup(239,240)Pu distribution follows that of the solid phase which decreases rapidly with depth. The pore water profiles of 137Cs are characterized by a broad and deeply penetrating maximum where activities of about 35 to 40 dpm/100 kg extend from 3 to 20 cm. Overlying seawater, in contrast, has an activity of 17 to 24 dpm/100 kg. The 137Cs and sup(239,240)Pu pore water data show that there is preferential downward transport of 137Cs and that sup(239,240)Pu does not have an active diagenetic chemistry and is not significantly mobile in these coastal sediments. (author)

  1. Alpha-particle emission probabilities in the decay of {sup 240}Pu

    Sibbens, G., E-mail: goedele.sibbens@ec.europa.e [European Commission, Joint Research Centre, Institute for Reference Materials and Measurements, Retieseweg 111, B-2440 Geel (Belgium); Pomme, S.; Altzitzoglou, T. [European Commission, Joint Research Centre, Institute for Reference Materials and Measurements, Retieseweg 111, B-2440 Geel (Belgium); Garcia-Torano, E. [Laboratorio de Metrologia de Radiaciones Ionizantes, CIEMAT, Avda. Complutense 22, 28040 Madrid (Spain); Janssen, H.; Dersch, R.; Ott, O. [Physikalisch-Technische Bundesanstalt (PTB), Bundesallee 100, 38116 Braunschweig (Germany); Martin Sanchez, A. [Departamento de Fisica, Universidad de Extremadura, Badajoz, E-06071 (Spain); Rubio Montero, M.P. [Departamento de Fisica Aplicada, Universidad de Extremadura, Merida, Badajoz, E-06800 (Spain); Loidl, M. [Laboratoire National Henri Becquerel, LNE/CEA-LIST, 91191 Gif-sur-Yvette (France); Coron, N.; Marcillac, P. de [Institut d' Astrophysique Spatiale, CNRS, 91405 Orsay Campus (France); Semkow, T.M. [Wadsworth Center, New York State Department of Health, Albany, NY 12201 (United States)

    2010-07-15

    Sources of enriched {sup 240}Pu were prepared by vacuum evaporation on quartz substrates. High-resolution alpha-particle spectrometry of {sup 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.

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

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

    2011-12-01

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

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

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

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

    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. (author)

  5. Separation and activity determination of 239+240Pu, 241Am and Curium (242and244Cm) in evaporator concentrate by Alpha Spectrometry

    Alpha spectrometry analysis was used for activity determinations of Pu, Am and Cm isotopes in evaporator concentrate samples from nuclear power plants. Using a sequential procedure the first step was Pu isolation by an anion exchange column followed by an Am and Cm separation of U and Fe by a co-precipitation with oxalic acid. The precipitate was used for americium and curium separation of strontium by using a TRU resin extraction chromatography column. Due to their chemical similarities and energy difference it was seen that the simultaneous determination of 241Am, 242Cm and 243,244Cm isotopes is possible using the 243Am as tracer, once they have peaks in different region of interest (ROI) in the alpha spectrum. In this work it was used tracers, 238Pu, 243Am, 244Cm and 232U, for determination and quantification of theirs isotopes, respectively. The standard deviations for replicate analysis were calculated and for 241Am it was (1,040 ± 160 mBqKg-1), relative standard deviation 15.38%, and for 239+240Pu it was (551 +- 44 mBqKg-1), relative standard deviation 7.98%. In addition, for the 242Cm isotope the standard deviation for determinations was(75 ± 23 mBqKg-1), with the relative standard deviation 30.67% higher than for 241Am and 239+240Pu. The radiometric yields ranged from 90% to 105% and the lower limit of detection was estimated as being 2.05 mBqKg-1. (author)

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

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

    2009-07-23

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

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

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

    2010-01-15

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

  8. Simultaneous evaluation for (n,f) cross section of 235U, 239Pu, 238U and (n,γ) cross sections of 238U

    The fission cross sections for 235U, 238U, 239Pu, the capture cross sections for 238U and the ratios for 239Pu(n,f)/235U(n,f), 238U(m,f)/235U(n,f), 238U(n,γ)/235U(n,f) were firstly evaluated respectively. The experimental data were collected, analysed, selected and corrected. The data were fitted with spline fit program

  9. Current levels of Pu isotopes and {sup 137}Cs at the former Soviet Union`s Semipalantisk nuclear test site

    Yamamoto, M. [Kanazawa Univ., Ishikawa (Japan). Low Level Radioactivity Laboratory; Tsumura, A. [National Inst. of Agro-Environmental Sciences, Ibaraki (Japan); Tsukatani, T. [Kyoto Univ. (Japan). Kyoto Institute of Economic Research

    1998-10-01

    This paper is a report on our survey of residual radioactivity in the soil of the Semipalatinsk nuclear test site in the former USSR. The soil was sampled at approximately 30 sites along the roads connecting Kurchatov City, ground zero for the first USSR nuclear test, Balapan, Degelen Mountain and Salzhal settlement. The radioactivity levels of {sup 137}Cs, {sup 238}Pu and {sup 239,240}Pu as well as the {sup 240}Pu/{sup 239}Pu atomic ratios in the soil were determined. Although {sup 137}Cs was within typical environmental levels except for an area near ground zero, {sup 239,240}Pu was at elevated levels contaminated with weapons-grade plutonium in all areas we visited. (orig.)

  10. Estimation of multi-group cross section covariances for 235,238U, 239Pu, 241Am, 56Fe, 23Na and 27Al

    This paper presents the methodology used to estimate multi-group covariances for some major isotopes used in reactor physics. The starting point of this evaluation is the modelling of the neutron induced reactions based on nuclear reaction models with parameters. These latest are the vectors of uncertainties as they are absorbing uncertainties and correlation arising from the confrontation of nuclear reaction model to microscopic experiment. These uncertainties are then propagated towards multi-group cross sections. As major breakthroughs were then asked by nuclear reactor physicists to assess proper uncertainties to be used in applications, a solution is proposed by the use of integral experiment information at two different stages in the covariance estimation. In this paper, we will explain briefly the treatment of all type of uncertainties, including experimental ones (statistical and systematic) as well as those coming from validation of nuclear data on dedicated integral experiment (nuclear data oriented). We will illustrate the use of this methodology with various isotopes such as 235,238U, 239Pu, 241Am, 56Fe, 23Na and 27Al. (authors)