Sample records for 240pu isotope activities

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

    Directory of Open Access Journals (Sweden)

    Dagmara I. Strumińska-Parulska


    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.


    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.

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

    Energy Technology Data Exchange (ETDEWEB)

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


    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.

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

    Energy Technology Data Exchange (ETDEWEB)

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


    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.

  5. Resolving Nevada Test Site and global fallout plutonium in attic dust and soils using [sup 137]Cs/[sup 239+240]Pu activity ratios

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    Cizdziel, J. (Univ. of Nevada, Reno, NV (United States)); Hodge, V. (Univ. of Nevada, Las Vegas, NV (United States). Dept. of Chemistry); Faller, S. (Environmental Protection Agency, Las Vegas, NV (United States). Radiation and Indoor Environments National Lab.)


    A simple equation using only [sup 137]Cs/[sup 239+240]Pu activity ratios was developed and evaluated as a means of resolving the plutonium in attic dust and soil from Nevada and Utah that came from Nevada Test Site fallout from that which came from global fallout. Applied to a historical data set of [sup 137]Cs and [sup 239+240]Pu activity concentrations in soils from Nevada and Utah, the activity ratio method gives results similar to the traditional [sup 240]Pu/[sup 239]Pu isotope mass ratio method. Considering the difficulty and expense of determining the [sup 240]Pu/[sup 239]Pu atom ratios, this activity ratio method is simpler, faster, and less costly, and may be useful for detecting and/or monitoring plutonium contamination in soils. Applied to samples of attic dust and soil collected from throughout southern Nevada and Utah during 1996 and 1997, it was found that all sites surveyed showed the presence of Nevada Test Site plutonium. Over 90% of the plutonium found in the samples from Beatty, Tonopah, and Queen City Summit, Nevada can be attributed to the Nevada Test Site.

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

    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.


    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. (United States)

    Xu, Yihong; Qiao, Jixin; Hou, Xiaolin; Pan, Shaoming; Roos, Per


    This paper reports an analytical method for the determination of plutonium isotopes ((238)Pu, (239)Pu, (240)Pu, (241)Pu) in environmental samples using anion exchange chromatography in combination with extraction chromatography for chemical separation of Pu. Both radiometric methods (liquid scintillation counting and alpha spectrometry) and inductively coupled plasma mass spectrometry (ICP-MS) were applied for the measurement of plutonium isotopes. The decontamination factors for uranium were significantly improved up to 7.5 × 10(5) for 20 g soil compared to the level reported in the literature, this is critical for the measurement of plutonium isotopes using mass spectrometric technique. Although the chemical yield of Pu in the entire procedure is about 55%, the analytical results of IAEA soil 6 and IAEA-367 in this work are in a good agreement with the values reported in the literature or reference values, revealing that the developed method for plutonium determination in environmental samples is reliable. The measurement results of (239+240)Pu by alpha spectrometry agreed very well with the sum of (239)Pu and (240)Pu measured by ICP-MS. ICP-MS can not only measure (239)Pu and (240)Pu separately but also (241)Pu. However, it is impossible to measure (238)Pu using ICP-MS in environmental samples even a decontamination factor as high as 10(6) for uranium was obtained by chemical separation.

  8. Time-resolved record of (236)U and (239,240)Pu isotopes from a coral growing during the nuclear testing program at Enewetak Atoll (Marshall Islands). (United States)

    Froehlich, M B; Chan, W Y; Tims, S G; Fallon, S J; Fifield, L K


    A comprehensive series of nuclear tests were carried out by the United States at Enewetak Atoll in the Marshall Islands, especially between 1952 and 1958. A Porites Lutea coral that was growing in the Enewetak lagoon within a few km of all of the high-yield tests contains a continuous record of isotopes, which are of interest (e.g. (14)C, (236)U, (239,240)Pu) through the testing period. Prior to the present work, (14)C measurements at ∼2-month resolution had shown pronounced peaks in the Δ(14)C data that coincided with the times at which tests were conducted. Here we report measurements of (236)U and (239,240)Pu on the same coral using accelerator mass spectrometry, and again find prominent peaks in the concentrations of these isotopes that closely follow those in (14)C. Consistent with the (14)C data, the magnitudes of these peaks do not, however, correlate well with the explosive yields of the corresponding tests, indicating that smaller tests probably contributed disproportionately to the debris that fell in the lagoon. Additional information about the different tests can also be obtained from the (236)U/(239)Pu and (240)Pu/(239)Pu ratios, which are found to vary dramatically over the testing period. In particular, the first thermonuclear test, Ivy-Mike, has characteristic (236)U/(239)Pu and (240)Pu/(239)Pu signatures which are diagnostic of the first arrival of nuclear test material in various archives.

  9. 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. (United States)

    Cao, Liguo; Zheng, Jian; Tsukada, Hirofumi; Pan, Shaoming; Wang, Zhongtang; Tagami, Keiko; Uchida, Shigeo


    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

  10. Extension of 239+240Pu sediment geochronology to coarse-grained marine sediments (United States)

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


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

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

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


    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

  12. Variation of the activity concentrations and fluxes of natural (210Po, 210Pb) and anthropogenic (239,240Pu, 137Cs) radionuclides in the Strait of Gibraltar (Spain). (United States)

    Gascó, C; Antón, M P; Delfanti, R; González, A M; Meral, J; Papucci, C


    The activity concentrations and fluxes of natural (210Pb, 210Po) and anthropogenic (239,240Pu, 137Cs) radionuclides have been determined in the different water masses crossing the Strait of Gibraltar. New data have been gathered during four multidisciplinary and multinational sampling campaigns, performed between 1997 and 1999 within the framework of the CANIGO-FLUGIST Project. Mean activity concentrations of 210Po (1.53+/-0.34 Bq m(-3), n = 30) and 210Pb (1.16+/-0.50 Bq m(-3), n = 31) in the Atlantic water entering the Mediterranean basin are about double those measured in the Mediterranean outflow, namely 0.84+/-0.34 Bq m(-3) (n = 22) for 210Po and 0.66+/-0.34 Bq m(-3) (n = 22) for 210Pb. The opposite trend is observed for 231,240Pu, with average concentrations of 9.9+/-3.0 mBq m(-3) (n = 29) in the incoming Atlantic flow and 22.0+/-3.0 mBq m(-3) (n = 22) in the outpouring Mediterranean water. In the case of 137Cs, the same concentrations were quantified in the waters moving inwards (2.52+/-0.28 Bq m(-3), n = 27) and outwards (2.14+/-0.52 Bq m(-3), n = 21) from the Mediterranean Sea. On this basis, the Mediterranean basin experiences a net annual input flux of 14 TBq of 210Pb and 19 TBq of 210Po, and a net annual loss of 0.34 TBq of 239,240Pu, while--at present--137Cs input and output fluxes appear to be balanced.

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

    Energy Technology Data Exchange (ETDEWEB)

    Leon Vintro, L. [University Coll., Dublin (Ireland). Dept. of Experimental Phys.; Mitchell, P.I. [University Coll., Dublin (Ireland). Dept. of Experimental Phys.; Condren, O.M. [University Coll., Dublin (Ireland). Dept. of Experimental Phys.; Moran, M. [Lawrence Livermore National Lab., Livermore, CA (United States); Vives i Batlle, J. [University Coll., Dublin (Ireland). Dept. of Experimental Phys.; Sanchez-Cabeza, J.A. [Dept. de Fisica, Universidad Autonoma de Barcelona, Bellaterra (Spain)


    In this paper, a simple technique, based on commercially-available software developed for gamma spectra analysis (MicroSAMPO {sup 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 {sup 242}Pu ``doublet`` (used as tracer) and, if present, the {sup 238}Pu ``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 {sup 240}Pu/{sup 239}Pu 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 {sup 240}Pu/{sup 239}Pu 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 {sup 239,240}Pu multiplet and published values. (orig.).

  14. A multi-radionuclide approach to evaluate the suitability of {sup 239+240}Pu as soil erosion tracer

    Energy Technology Data Exchange (ETDEWEB)

    Meusburger, Katrin, E-mail: [Environmental Geosciences, University of Basel, Bernoullistrasse 30, CH-4056 Basel (Switzerland); Mabit, Lionel, E-mail: [Soil and Water Management and Crop Nutrition Laboratory, FAO/IAEA Agriculture & Biotechnology Laboratory, IAEA Laboratories, Seibersdorf (Austria); Ketterer, Michael, E-mail: [Chemistry Department, Metropolitan State University of Denver, CO (United States); Park, Ji-Hyung, E-mail: [Department of Environmental Science & Engineering, Ewha Womans University, Seoul 120-750 (Korea, Republic of); Sandor, Tarjan [Radioanalytical Reference Laboratory, Central Agricultural Office Food and Feed Safety Directorate (Hungary); Porto, Paolo, E-mail: [Dipartimento di AGRARIA, Università degli Studi “Mediterranea” di Reggio Calabria (Italy); Alewell, Christine, E-mail: [Environmental Geosciences, University of Basel, Bernoullistrasse 30, CH-4056 Basel (Switzerland)


    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 {sup 239}Pu and {sup 240}Pu as a method to assess soil erosion magnitude by comparison to more established fallout radionuclides such as {sup 137}Cs and {sup 210}Pb{sub ex}. 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 (> 25 t ha{sup −1} yr{sup −1}). Pu isotopes further allowed determining the origin of the fallout. Both {sup 240}Pu/{sup 239}Pu atomic ratios and {sup 239+240}Pu/{sup 137}Cs activity ratios were close to the global fallout ratio. However, the depth profile of the {sup 239+240}Pu/{sup 137}Cs activity ratios in undisturbed sites showed lower ratios in the top soil increments, which might be due to higher migration rates of {sup 239+240}Pu. The activity ratios further indicated preferential transport of {sup 137}Cs from eroded sites (higher ratio compared to the global fallout) to the depositional sites (smaller ratio). As such the {sup 239+240}Pu/{sup 137}Cs activity ratio offered a new approach to parameterize a particle size correction factor that can be applied when both {sup 137}Cs and {sup 239+240}Pu have the same fallout source. Implementing this particle size correction factor in the conversion of {sup 137}Cs inventories resulted in comparable estimates of soil loss for {sup 137}Cs and {sup 239+240}Pu. The comparison among the different fallout radionuclides highlights the suitability of {sup 239+240}Pu through less preferential transport compared to {sup 137}Cs and the possibility to gain information regarding the origin of the fallout. In conclusion, {sup 239+240}Pu is a promising soil erosion tracer, however, since the behaviour i.e. vertical migration in the

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

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


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

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

    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


    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.

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

    DEFF Research Database (Denmark)

    Ezerinskis, Z.; Hou, Xiaolin; Druteikiene, R.;


    Fifty five soil samples collected in the Lithuania teritory in 2011 and 2012 were analyzed for 129I, 137Cs and Pu isotopes in order to investigate the level and distribution of artificial radioactivity in Lithuania. The activity and atomic ratio of 238Pu/239,240Pu, 129I/127I and 131I/137Cs were...... used to identify the origin of these radionuclides. The 238Pu/239þ240Pu and 240Pu/239Pu ratios in the soil samples analyzed varied in the range of 0.02e0.18 and 0.18e0.24, respectively, suggesting the global fallout as the major source of Pu in Lithuania. The values of 109 to 106 for 129I/127I atomic...... ratio revealed that the source of 129I in Lithuania is global fallout in most cases though several sampling sites shows a possible impact of reprocessing releases. Estimated 129I/131I ratio in soil samples from the southern part of Lithuania shows negligible input of the Chernobyl fallout...

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

    Energy Technology Data Exchange (ETDEWEB)

    Chamizo, Elena; López-Lora, Mercedes [Centro Nacional de Aceleradores (Universidad de Sevilla, Consejo Superior de Investigaciones Científicas, Junta de Andalucía), Thomas Alva Edison 7, 41092 Seville (Spain); Villa, María [Departamento de Física Aplicada II, Universidad de Sevilla, Av. Reina Mercedes 4A, 41012 Seville (Spain); Servicio de Radioisótopos, Centro de Investigación, Tecnología e Innovación, Universidad de Sevilla, Av. Reina Mercedes 4B, 41012 Seville (Spain); Casacuberta, Núria [Laboratory of Ion Beam Physics, ETH Zürich, Otto-Stern-Weg 5, CH-8093 Zürich (Switzerland); López-Gutiérrez, José María [Centro Nacional de Aceleradores (Universidad de Sevilla, Consejo Superior de Investigaciones Científicas, Junta de Andalucía), Thomas Alva Edison 7, 41092 Seville (Spain); Departamento de Física Aplicada I, Escuela Universitaria Politécnica, Universidad de Sevilla, Virgen de África 7, 41011 Seville (Spain); Pham, Mai Khanh [IAEA-Environment Laboratories, Monte Carlo 98000 (Monaco)


    The performance of the 1 MV AMS system at the CNA (Centro Nacional de Aceleradores, Seville, Spain) for {sup 236}U and {sup 239,240}Pu measurements has been extensively investigated. A very promising {sup 236}U/{sup 238}U abundance sensitivity of about 3 × 10{sup −11} has been recently achieved, and background figures for {sup 239}Pu of about 10{sup 6} atoms were reported in the past. These promising results lead to the use of conventional low energy AMS systems for the analysis of {sup 236}U and {sup 239}Pu and its further application in environmental studies. First {sup 236}U results obtained on our AMS system for marine samples (sediments and water) are presented here. Results of two new IAEA reference materials (IAEA-410 and IAEA-412, marine sediments from Pacific Ocean) are reported. The obtained {sup 236}U/{sup 239}Pu atom ratios, of 0.12 and 0.022, respectively, show a dependency with the contamination source (i.e. local fallout from the US tests performed at the Bikini Atoll and general fallout). The results obtained for a third IAEA reference material (IAEA-381, seawater from the Irish Sea), are also presented. In the following, the uranium and plutonium isotopic compositions obtained on a set of 5 intercomparison seawater samples from the Arctic Ocean provided by the ETH Zürich are discussed. By comparing them with the obtained results on the 600 kV AMS facility Tandy at the ETH Zürich, we demonstrate the solidity of the CNA technique for {sup 236}U/{sup 238}U determinations at, at least, 7 × 10{sup −10} level. Finally, these results are discussed in their environmental context.

  19. Plutonium, (137)Cs and uranium isotopes in Mongolian surface soils. (United States)

    Hirose, K; Kikawada, Y; Igarashi, Y; Fujiwara, H; Jugder, D; Matsumoto, Y; Oi, T; Nomura, M


    Plutonium ((238)Pu and (239,240)Pu), (137)Cs and plutonium activity ratios ((238)Pu/(239,240)Pu) as did uranium isotope ratio ((235)U/(238)U) were measured in surface soil samples collected in southeast Mongolia. The (239,240)Pu and (137)Cs concentrations in Mongolian surface soils (surface soils (0.013-0.06) coincided with that of global fallout. The (235)U/(238)U atom ratios in the surface soil show the natural one. There was a good correlation between the (239,240)Pu and (137)Cs concentrations in the surface soils. We introduce the migration depth to have better understanding of migration behaviors of anthropogenic radionuclides in surface soil. We found a difference of the migration behavior between (239,240)Pu and (137)Cs from (137)Cs/(239,240)Pu - (137)Cs plots for the Mongolian and Tsukuba surface soils; plutonium in surface soil is migrated easier than (137)Cs.

  20. Microscopic Calculations of 240Pu Fission

    Energy Technology Data Exchange (ETDEWEB)

    Younes, W; Gogny, D


    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.

  1. Determination of plutonium isotopes in seawater reference materials using isotope-dilution ICP-MS. (United States)

    Zheng, Jian; Yamada, Masatoshi


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

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

    Energy Technology Data Exchange (ETDEWEB)

    Yamada, Masatoshi; Zheng, Jian; Wang, Zhong-Liang [Nakaminato Laboratory for Marine Radioecology, National Institute of Radiological Sciences, Isozaki 3609, Hitachinaka, Ibaraki 311-1202 (Japan)


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

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

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


    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.

  4. Distribution characteristics of ¹³⁷Cs, Pu isotopes and ²⁴¹Am in soil in Korea. (United States)

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


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

  5. (137)Cs, (239+240)Pu concentrations and the (240)Pu/(239)Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary. (United States)

    Pan, S M; Tims, S G; Liu, X Y; Fifield, L K


    A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of (137)Cs and plutonium (Pu) isotopes. The (137)Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the (137)Cs and (239+240)Pu. The shape of the vertical (137)Cs distribution in the sediment core was similar to that of the Pu. The maximum (137)Cs and (239+240)Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average (240)Pu/(239)Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the (240)Pu/(239)Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The (137)Cs and (239+240)Pu inventories were estimated to be 7100 ± 1200 Bq/m(2) and 407 ± 27 Bq/m(2), respectively. Approximately 40% of the (239+240)Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure (240)Pu/(239)Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.

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

    CERN Multimedia

    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.

  7. {sup 238}Pu, {sup 239+240}Pu and {sup 241}Am levels in the terrestrial and aquatic environment of the Loire and Garonne rivers basins (France)

    Energy Technology Data Exchange (ETDEWEB)

    Rousseau, G.; Mokili, M.B.; Le Roy, C.; Pagano, V. [SUBATECH/IN2P3 (France); Gontier, G.; Boyer, C. [EDF-DPI-DIN-CIDEN (France); Chardon, P. [CNRS/IN2P3 (France); Hemidy, P.Y. [EDF-DPN-UNIE-GPRE-IEV (France)


    Plutonium and americium long-lived alpha emitter isotopes can be found in the environment because of atmospheric global fallout due to thermonuclear tests performed between 1945 and 1980, to the American SNAP 9A satellite explosion in 1964, to the Chernobyl nuclear power plant accident,... In France, the nuclear safety authority does not allow the release of artificial alpha emitters from nuclear power plants. Thus, monitoring is performed to verify the absence of these alpha emitters in liquid discharges to respect the limits set by the regulations. These thresholds ensure a very low dosimetric impact to the population compared to other radionuclides. With the objective of environmental monitoring around nuclear facilities, activity measurements of long-lived alpha emitters are carried out to detect the traces of these radionuclides. Analysis of low activity by alpha spectrometry after chemical steps were performed and used to determine the {sup 238}Pu, {sup 239+240}Pu and {sup 241}Am activities on a large set of environmental solid samples likely to be encountered in environmental monitoring as soils, sediments, terrestrial and aquatic bio-indicators. The samples collected in the terrestrial and aquatic environment of the Loire and Garonne rivers basins (France) was investigated for the 2009-2014 period. It was found that the mean activity concentration of the most frequently detected was for the radionuclide {sup 238}Pu: from <0.00031 to 0.0061 Bq/kg dry in terrestrial samples and from <0.00086 to 0.011 Bq/kg dry in aquatic samples; for the radionuclide {sup 239+240}Pu: from 0.00041 to 0.150 Bq/kg dry in terrestrial samples and from 0.0023 to 0.240 Bq/kg dry in aquatic samples and for the radionuclide {sup 241}Am: from <0.00086 to 0.087 Bq/kg dry in terrestrial samples and from 0.0022 to 0.120 Bq/kg dry in aquatic samples. {sup 238}Pu/{sup 239+240}Pu and {sup 241}Am/{sup 239+240}Pu ratios determined are in accordance with an environmental contamination due to

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

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


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

  9. Radioecologycal study of 239/240Pu in Bangka Island and Muria Peninsula: Determination of 239/240Pu in marine sediment and seawater as part of baseline data collecting for sitting of candidates of first Indonesia NPP (United States)

    Suseno, Heny; Wisnubroto, Djarot S.


    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 239/240Pu 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 239/240Pu 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 239/240Pu in Bangka Island and Muria Peninsula were range from 0.013 to 0.021 and 0.018 to 0.024 respectively. The water baseline concentration this isotope were range from 2.73 to 4.05 mBq.m-3 and 2.98 to 4.50 mBq.m-3.

  10. 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

    Energy Technology Data Exchange (ETDEWEB)

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


    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{sup −1} and 0.018 to 0.024{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}.

  11. Seasonal variations in activity concentrations of {sup 137}Cs, {sup 40}K, {sup 7}Be, {sup 228}Ac, {sup 99}Tc, {sup 90}Sr, and {sup 239/240}Pu in Fucus vesiculosus and Ascophyllum nodosum from the South-Eastern coast of Norway

    Energy Technology Data Exchange (ETDEWEB)

    Raaum, A.; Christensen, G.C. [Institute for Energy Technology, Health and Safety Dept., Kjeller (Norway)


    Brown algae have been proven to be useful indicator organisms for heavy metals and radionuclides in the marine environments due to their ability to concentrate elements from the ambient water. There is quite a lot of data available on {sup 137}Cs in brown algae, especially for Fucus Vesiculosus. Fucus Vesiculosus is also commonly used to monitor the impact of the releases of {sup 99}Tc from the reprocessing plant in Sellafield. There is however a lack of data for other long-lived anthropogenic nuclides as {sup 90}Sr and Pu, and for natural occurring radionuclides. There is also a need for more knowledge about the mechanisms for uptake and accumulation of the different elements, and about different factors influencing the uptake. In this study activity concentrations of {sup 137}Cs, {sup 40}K, {sup 7}Be, {sup 228}Ac, {sup 99}Tc, {sup 90}Sr and {sup 239/240}Pu are measured in whole plants of Fucus vesiculosus and Ascophyllum nodosum collected over a period of one year from the south-eastern coast of Norway. Significant differences between the two species have been found. For {sup 137}Cs, {sup 40}K, {sup 7}Be, {sup 228}Ra and {sup 239/240}Pu, the activity concentrations were significantly higher in Fucus vesiculosus than in Ascophyllum nodosum, whereas for {sup 99}Tc the activity concentrations were higher in Ascophyllum nodosum than in Fucus vesiculosus. There were great seasonal variations in the concentrations of the measured radionuclides. For {sup 99}Tc there was also a difference in the temporal pattern for the two species. Possible uptake mechanisms will be discussed based on the results and on the known physiological differences between the two species. (author)

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

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


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

  13. Pu-239 and Pu-240 inventories and Pu-240/ Pu-239 atom ratios in the water column off Sanriku, Japan. (United States)

    Yamada, Masatoshi; Zheng, Jian; Aono, Tatsuo


    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

  14. Angular distributions of low-spin states in {sup 240}Pu by means of the {sup 242}Pu(p,t){sup 240}Pu reaction

    Energy Technology Data Exchange (ETDEWEB)

    Spieker, Mark; Endres, Janis; Pascu, Sorin; Zilges, Andreas [Koeln Univ. (Germany). Inst. fuer Kernphysik; Bucurescu, Dorel; Zamfir, Nicolae-Victor [Horia Hulubei National Institute of Physics and Nuclear Engineering, Bucharest (Romania); Faestermann, Thomas [Physik Department, Technische Universitaet Muenchen (Germany); Hertenberger, Ralf; Wirth, Hans-Friedrich [Fakultaet fuer Physik, Ludwig-Maximilians-Universitaet Muenchen (Germany)


    Since recent experimental and theoretical studies revealed the importance of octupole correlations in the actinide region and especially in {sup 240}Pu, a {sup 242}Pu(p,t){sup 240}Pu experiment has been conducted at the Q3D magnetic spectrograph of the Maier-Leibnitz laboratory in Munich. Excited states in {sup 240}Pu were investigated up to an excitation energy of 3 MeV. Angular distributions have been measured at 9 laboratory angles between 5 {sup circle} and 40 {sup circle}. The comparison of the experimental angular distributions with DWBA calculations allowed the assignment of several low-spin states. Most of them were seen for the first time. The experimental data, especially the data on the 21 J{sup π}= 0{sup +} states, are presented and discussed in the framework of the spdf-version of the Interacting Boson Model.

  15. High-/sup 240/Pu sector experiments in ZPPR assembly 4

    Energy Technology Data Exchange (ETDEWEB)

    McFarlane, H F; Beck, C L


    The complete high-/sup 240/Pu fuel experiment in ZPPR assembly 4 is reviewed. Results of criticality, enrichment, small-sample perturbation, sodium void, /sup 238/U Doppler, control rod substitution and reaction rate measurements are presented. Comparison of these measured values with calculated results are included where possible. The relationship between the ZPPR high-/sup 240/Pu fuel experiments and the results obtained in previous critical experience is considered.

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

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


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

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

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


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

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

    CERN Multimedia

    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].

  19. Validation of new {sup 240}Pu cross section and covariance data via criticality calculation

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Do Heon; Gil, Choong-Sup; Kim, Hyeong Il; Lee, Young-Ouk, E-mail:, E-mail:, E-mail:, E-mail: [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of); Leal, Luiz C.; Dunn, Michael E., E-mail:, E-mail: [Oak Ridge National Laboratory, TN (United States)


    Recent collaboration between KAERI and ORNL has completed an evaluation for {sup 240}Pu neutron cross section with covariance data. The new {sup 240}Pu cross section data has been validated through 28 criticality safety benchmark problems taken from the ICSBEP and/or CSEWG specifications with MCNP calculations. The calculation results based on the new evaluation have been compared with those based on recent evaluations such as ENDF/B-VII.0, JEFF-3.1.1, and JENDL-4.0. In addition, the new {sup 240}Pu covariance data has been tested for some criticality benchmarks via the DANTSYS/SUSD3D-based nuclear data sensitivity and uncertainty analysis of k{sub eff}. The k{sub eff} uncertainty estimates by the new covariance data has been compared with those by JENDL-4.0, JENDL-3.3, and Low-Fidelity covariance data. (author)

  20. 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)

    Energy Technology Data Exchange (ETDEWEB)

    Bruneau, F


    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)

  1. 137Cs and (239+240)Pu levels in the Asia-Pacific regional seas. (United States)

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


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

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

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


    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.

  3. Polonium 210Po, uranium (234U, 238U and plutonium (238Pu, 239+240Pu bioaccumulation in marine birds

    Directory of Open Access Journals (Sweden)

    Strumińska-Parulska D. I.


    Full Text Available The aim of this work was the determination of 210Po, 234U, 238U, 238Pu and 239+240Pu concentration in marine birds which permanently or temporally live in the southern Baltic Sea coast. We chose 11 species of seabirds: three species permanently residing at southern Baltic Sea, four species of wintering birds and three species of migrating birds. The results show that analyzed radionuclides are non-uniformly distributed in the marine birds. The highest activities of 210Po were observed in feathers, muscles and liver. The highest uranium content was found in liver, rest of viscera and feathers, while plutonium in the digestion organs and feathers. Omnivore seabirds accumulated more polonium, plutonium than species that feed on fish, while herbivore seabirds accumulated more uranium than carnivore.

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

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


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

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

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


    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 ).

  6. Characterisation of the plutonium isotopic composition of a sediment core from Palomares, Spain, by low-energy AMS and alpha-spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Chamizo, E., E-mail: [Centro Nacional de Aceleradores (CNA), Isla de la Cartuja, 41092 Seville (Spain); Jimenez-Ramos, M.C.; Enamorado, S.M. [Centro Nacional de Aceleradores (CNA), Isla de la Cartuja, 41092 Seville (Spain); Garcia-Leon, M. [Departamento de Fisica Atomica, Molecular y Nuclear, Universidad de Sevilla, 41012 Sevilla (Spain); Garcia-Tenorio, R. [Departamento de Fisica Aplicada II, E.T.S.A, Universidad de Sevilla, 41012 Sevilla (Spain); Mas, J.L. [Departamento de Fisica Aplicada I, Universidad de Sevilla, 41012 Sevilla (Spain); Masque, P. [Institut de Ciencia i Tecnologia Ambientals, Department de Fisica, Universitat Autonoma de Barcelona, 08193 Bellaterra (Spain); Merino, J. [Amphos 21, Pg. de Rubi 29-31, E-08197 Valldoreix (Spain); Sanchez-Cabeza, J.A. [Institut de Ciencia i Tecnologia Ambientals, Department de Fisica, Universitat Autonoma de Barcelona, 08193 Bellaterra (Spain); International Atomic Energy Agency, Marine Environment Laboratories, MC-98000 (Monaco)


    The measurement of plutonium isotopes, {sup 239}Pu and {sup 240}Pu, at 670 kV on the compact accelerator mass spectrometry (AMS) system at the Centro Nacional de Aceleradores (CNA) in Seville, Spain, is now a reality. In this work, we present first Pu AMS results for environmental samples: a sediment core collected in a submarine canyon in the Mediterranean coast of the Spanish region of Palomares, affected by a nuclear accident in 1966. From the study of the {sup 240}Pu/{sup 239}Pu atomic ratio profile, showing on average levels lower than 11%, we confirm that the weapon-grade plutonium released on land during the accident, with a characteristic {sup 240}Pu/{sup 239}Pu atomic ratio of 5.8%, has found its way into the marine environment. A two-plutonium sources mixture model (Palomares and fallout) is used to elucidate the percentage of the plutonium coming from the accident. As a validation exercise of the Pu AMS measuring technique and in order to obtain the {sup 238}Pu/{sup (239+240)}Pu activity ratios, samples were also studied by alpha-spectrometry (AS). The obtained AS {sup 239+240}Pu activity concentration results fit in with the AMS ones in a wide dynamic range, thus validating the AMS technique.

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

    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


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

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

    Energy Technology Data Exchange (ETDEWEB)

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


    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

  9. Microscopic modeling of mass and charge distributions in the spontaneous fission of 240Pu (United States)

    Sadhukhan, Jhilam; Nazarewicz, Witold; Schunck, Nicolas


    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.

  10. Fission Barrier for 240Pu in the Quadrupole Constrained Relativistic Mean Field Approach

    Institute of Scientific and Technical Information of China (English)

    L(U) Hong-Feng; GENG Li-Sheng; MENG Jie


    @@ The fission barrier for 240Pu is investigated beyond the second saddle point in the potential energy surface by the constrained relativistic mean field method with the newly proposed parameter set PK1. The microscopic correction for the centre-of-mass motion is essential to provide the correct potential energy surface. The shell effects that stabilize the nuclei against the fission is also investigated by the Strutinsky method. The shapes for the ground state, fission isomer and saddle-points, etc, are studied in detail.

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

    CERN Document Server

    Sadhukhan, Jhilam; Schunck, Nicolas


    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.

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

    Energy Technology Data Exchange (ETDEWEB)

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


    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    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)


    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.

  14. Migration of plutonium from freshwater ecosystem at Hanford. [/sup 238/Pu, /sup 239/Pu, /sup 240/Pu

    Energy Technology Data Exchange (ETDEWEB)

    Emery, R. M.; Klopfer, D. C.; McShane, M. C.


    A reprocessing waste pond at Hanford has been inventoried to determine quantities of plutonium (Pu) that have been accumulated since its formation in 1944. Expressions of export were developed from these inventory data and from informed assumptions about the vectors which act to mobilize material containing Pu. This 14-acre pond provides a realistic illustration of the mobility of Pu in a lentic ecosystem. The ecological behavior of Pu in this pond is similar to that in other contaminated aquatic systems having widely differing limnological characteristics. Since its creation, this pond has received about one Ci of /sup 239/,/sup 240/Pu and /sup 238/Pu, most of which has been retained by its sediments. Submerged plants, mainly diatoms and Potamogeton, accumulate >95% of the Pu contained in biota. Emergent insects are the only direct biological route of export, mobilizing about 5 x 10/sup 3/ nCi of Pu annually, which is also the estimated maximum quantity of the Pu exported by waterfowl, birds and mammals collectively. There is no apparent significant export by wind, and it is not likely that Pu has migrated to the ground water below U-Pond via percolation. Although this pond has a rapid flushing rate, a eutrophic nutrient supply with a diverse biotic profile, and interacts with an active terrestrial environment, it appears to effectively bind Pu and prevent it from entering pathways to man and other life.

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

    Energy Technology Data Exchange (ETDEWEB)

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


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

  16. Spatial distribution of {sup 241}Am, {sup 137}Cs, {sup 238}Pu, {sup 239,240}Pu and {sup 241}Pu over 17 year periods in the Ravenglass saltmarsh, Cumbria, UK

    Energy Technology Data Exchange (ETDEWEB)

    Oh, J.-S. [GAU-Radioanalytical, School of Ocean and Earth Science, National Oceanography Centre, Southampton SO14 3ZH (United Kingdom)], E-mail:; Warwick, P.E. [GAU-Radioanalytical, School of Ocean and Earth Science, National Oceanography Centre, Southampton SO14 3ZH (United Kingdom)], E-mail:; Croudace, I.W. [GAU-Radioanalytical, School of Ocean and Earth Science, National Oceanography Centre, Southampton SO14 3ZH (United Kingdom)], E-mail:


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

  17. Pu isotopes and {sup 241}Am activities determination in the evaluation of radiochemical sequential analyzes methodology for evaporator concentrate samples using alpha spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Reis Junior, Aluisio S.; Temba, Eliane S.C.; Kastner, Geraldo F.; Monteiro, Roberto P.G., E-mail: [Centro de Desenvolvimento da Tecnologia Nuclear (SERTA/CDTN/CNEN-MG), Belo Horizonte, MG (Brazil). Servico do Reator e Tecnicas Analiticas


    Alpha spectrometry analyzes were used for activity determinations of Pu and Am isotopes in evaporator concentrate samples from nuclear power plants. In this work it was used tracers for isotopes determination and quantification. The radiometric yields ranged from 60% to 100% and the Lower Limit of Detection was estimated as being 2.05 mBqKg{sup -1}. The relative standard deviations for replicate analysis were calculated for {sup 241}Am, 15.13% (sample J) and 9.38% (sample N), and for {sup 239+240}Pu, 8.16% (sample J) and 7.95% (sample N). (author)

  18. Suitability of 239+240Pu and 137Cs as tracers for soil erosion assessment in mountain grasslands. (United States)

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


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

  19. Plutonium concentration and isotopic ratio in soil samples from central-eastern Japan collected around the 1970s (United States)

    Yang, Guosheng; Zheng, Jian; Tagami, Keiko; Uchida, Shigeo


    Obtaining Pu background data in the environment is essential for contamination source identification and assessment of environmental impact of Pu released from the Fukushima Daiichi nuclear power plant (FDNPP) accident. However, no baseline information on Pu isotopes in Fukushima Prefecture has been reported. Here we analyzed 80 surface soil samples collected from the central-eastern Japan during 1969-1977 for 239+240Pu activity concentration and 240Pu/239Pu atom ratio to establish the baseline before the FDNPP accident. We found that 239+240Pu activity concentrations ranged from 0.004 -1.46 mBq g-1, and 240Pu/239Pu atom ratios varied narrowly from 0.148 to 0.229 with a mean of 0.186 +/- 0.015. We also reconstructed the surface deposition density of 241Pu using the 241Pu/239Pu atom ratio in the Japanese fallout reference material. The obtained results indicated that, for the FDNPP-accident released 241Pu, a similar radiation impact can be estimated as was seen for the global fallout deposited 241Pu in the last decades.

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

    Energy Technology Data Exchange (ETDEWEB)

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


    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)

  1. Release of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant accident to the marine environment was negligible. (United States)

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


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

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

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


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

  3. A modelling study on {sup 137}Cs and {sup 239,240}Pu behaviour in the Alboran Sea, western Mediterranean

    Energy Technology Data Exchange (ETDEWEB)

    Perianez, R. [Departamento Fisica Aplicada I, E.U. Ingenieria Tecnica Agricola, Universidad de Sevilla, Ctra., Utrera km 1, 41013 Sevilla (Spain)], E-mail:


    A model for simulating the dispersion processes of {sup 137}Cs and {sup 239,240}Pu in the Alboran Sea is described. The model consists of two hydrodynamic models: a 2D depth-averaged model and a two-layer model which provide tidal and geostrophic currents, respectively; a sediment transport model which provides suspended particle concentrations and sedimentation rates over the domain; and the radionuclide dispersion model including interactions of dissolved radionuclides with suspended particles and bed sediments. These processes are formulated using kinetic transfer coefficients. The hydrodynamic and sediment models are run and validated in advance, and their results are then used to simulate the dispersion of {sup 137}Cs and {sup 239,240}Pu, which are introduced from atmospheric fallout. Radionuclide concentrations in the water column and distributions in bed sediments have been compared with measurements in the sea. Both set of data are, in general, in agreement. The model has also been applied to calculate radionuclide fluxes through the Strait of Gibraltar. These computed fluxes have been compared with previous estimations as well.

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

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


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

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

    Energy Technology Data Exchange (ETDEWEB)

    Noshkin, V.E.


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

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

    Energy Technology Data Exchange (ETDEWEB)

    Mitchell, P.I.; Vintro, L.L. [University Coll., Dublin (Ireland). Dept. of Physics; Dahlgaard, H. [Risoe National Lab., Roskilde (Denmark); Gasco, C.; Sanchez-Cabeza, J.A. [Barcelona Univ. (Spain). Dept. de Fisica Teorica


    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 {sup 240}Pu/{sup 239}Pu atom ratio of {approx}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 {sup 240}Pu/{sup 239}Pu 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 {sup 240}Pu/{sup 239}Pu ratio was measured by high-resolution alpha spectrometry and spectral deconvolution. The analytical results showed that at Thule the mean {sup 240}Pu/{sup 239}Pu 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.

  7. Isotope dilution gamma spectrometry for Pu using low energy photons

    Energy Technology Data Exchange (ETDEWEB)

    Paul, S.; Sarkar, A.; Alamelu, D.; Shah, R.V.; Aggarwal, S.K. [Bhabha Atomic Reseach Centre, Mumbai (India). Fuel Chemistry Div.


    Isotope dilution gamma spectrometry (IDGS) for determination of the Pu concentration, using high resolution gamma-ray spectrometry (HRGS) in the 40-150 keV energy range, is developed and described. The methodology involves purification of Pu by an anion exchange procedure, followed by the determination of Pu isotopic composition using HRGS. For isotope dilution, a pre-calibrated power reactor grade Pu ({proportional_to} 70 at. % {sup 239}Pu) solution from an Indian PHWR was used as a spike for research reactor grade Pu ({proportional_to} 95 at. % {sup 239}Pu) samples and vice versa. Changes in {sup 240}Pu/{sup 239}Pu (45.24 keV/51.62 keV) and {sup 241}Pu/{sup 239}Pu (148.57 keV/129.29 keV) activity ratios in the spiked samples were determined by gamma spectrometry. Using the atom ratios calculated from the measured activity ratios, the concentration of Pu in the sample was calculated using two different efficiency calibration methods. The isotopic composition and concentration of Pu samples both from power reactor and research reactor grade agreed well with the values obtained by isotope dilution-thermal ionization mass spectrometry. The present method also shows the superiority of using the {sup 240}Pu/{sup 239}Pu atom ratio against the {sup 241}Pu/{sup 239}Pu atom ratio in IDGS with respect to the accuracy and precision. (orig.)

  8. Sources and Spatial Distribution of Metal Pollutants in Soils near the El Paso Smelter: A Forensic Study with Pb and Pu Isotopes. (United States)

    Ketterer, Michael; Moan, Matthew; Gremillion, Paul


    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 (soils from control locations (> 10 km distant). A general trend of decreasing concentrations vs. distance from the smelter was also observed. However, the results indicate that metal concentrations vary widely even at a fixed distance from the smelter point source. This phenomenon results from a combination of natural and anthropogenic processes that disturb and re-distribute soils in the surface environment. The site conditions consist of a very arid environment with little vegetation cover that is frequently disturbed by high winds and severe episodic rainfall. To study these effects, we have investigated stratospheric fallout plutonium (239+240Pu) as a proxy measure of disturbed vs. undisturbed soil conditions. The premise is that 'undisturbed' locations will have high 239+240Pu activities, and hence contain most or all of the cumulative deposition

  9. A study on artificial radionuclides ({sup 134}Cs, {sup 137}Cs and {sup 239+240}Pu) distribution in the sediment form lake euiam

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Seung Hwan; Lee, Sang Han; Oh, Jung Suk; Choi, Jong Ki [Korea Research Institute of Standards and Science, Daejeon (Korea, Republic of); Kang, Tae Gu [National Institute of Environmental Research, Sejong (Korea, Republic of)


    The objective of this study is to identify the radionuclide distribution in public water by carrying out the analysis of artificial radionuclides(({sup 134}Cs, {sup 137}Cs, {sup 239+240}Pu), natural radionuclide({sup 210}Pb) and TOC in the lake Euiam sediment in Chuncheon, South Korea. The {sup 134}Cs concentration in all lake sediments showed below MDA values, and the {sup 137}Cs concentration in lake sediment were ranged from MDA to 8.79 Bq · kg{sup -1}-dry. The {sup 137}Cs concentrations in surface sediment were reported to be 2.4 to 4.2 Bq · kg{sup -1}-dry. The lowest concentration of {sup 137}Cs was reported at St. 4 and the highest concentration was reported at St. 3, respectively. The {sup 239+240}Pu concentration in lake sediment were ranged from 0.049 to 0.47 Bq · kg{sup -1}-dry. The lowest concentration of was reported at St. 2 and the highest concentration was reported at St. 3. The correlation(r) between the {sup 239+240}Pu concentration and {sup 137}Cs concentration in lake sediment presented higher values (0.54 to 0.97) and this suggests the behavior and origin of {sup 137}Cs is identical to the {sup 239+240}Pu in the sediment. The {sup 134}Cs concentration below MDA value and the {sup 239+240}Pu/{sup 134}Cs ratio(mean value of 0.041) indicated that the artificial radionuclides in the sediment were originated from global fallout by the atmospheric testing of nuclear weapons conducted by former USSR and U.S.A, but not from the Fukushima Daiichi NPP accident. The sedimentation rate derived from {sup 2}'1{sup 0}Pb age-dating method at St. 2 is calculated to be 0.31±0.06 cm · y{sup -1}. This value is similar to the value (0.41±0.05 cm · y{sup -1}) estimated from the {sup 137}Cs maximum peak produced from early 1960's. The content of TOC in lake Euiam sediments varied from 0.20 to 13.01%. While the highest correlation between TOC and {sup 137}Cs concentration in the sediment were found at St. 1, the others presented the low correlation.

  10. 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

    Energy Technology Data Exchange (ETDEWEB)

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


    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)

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

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


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

  12. Plutonium isotopes in the ocean off Japan after Fukushima

    Energy Technology Data Exchange (ETDEWEB)

    Buesseler, K.; Black, E.; Pike, S. [Woods Hole Oceanographic Institution (United States); Kenna, T. [Lamont-Doherty Earth Observatory (United States); Masque, P. [Universitat Autonoma de Barcelona (Spain)


    The Fukushima Dai-ichi nuclear power plants (NPPs) are known to be an unprecedented accidental source of {sup 137}Cs, {sup 134}Cs and other volatile radionuclides to the ocean. Much less is known however about the extent of input of refractory radionuclides such as plutonium to the environment. Limited available data from land soils and vegetation, suggest at least some atmospheric delivery of particulate Pu but at very low levels relative to pre-existing fallout sources. To resolve Fukushima derived Pu from weapons testing derived Pu, information regarding the Pu isotopic composition is needed. The {sup 240}Pu/{sup 239}Pu atom ratio determined by mass spectrometric techniques, and the {sup 238}Pu/{sup 239,240}Pu activity ratio as measured by alpha counting are diagnostic with respect to Pu source. We review and present new data on the Pu isotopic ratios and concentrations in the oceans, combining several data sets on dissolved (from bottle sampling), suspended particulates (from filtration), sinking particles (from sediment traps) and seafloor sediments (from cores) to look for the Fukushima Pu signal. In most samples, the {sup 240}Pu/{sup 239}Pu ratios are in the range of 0.20-0.23, characteristic of Pu ocean signal which is a combination of global fallout with a characteristic ratio of 0.18 and local fallout from the Pacific Proving Grounds with ratios higher than 0.24, and known from prior studies to influence the ocean off Japan. In 2011, in surface ocean waters, we found ratios {sup 240}Pu/{sup 239}Pu >0.3, which implies a component of Fukushima Pu had been delivered to the ocean, given NPP derived end-member ratios of 0.35-0.45. Fukushima derived Pu was not found deeper in the water column or even at all stations, consistent with its rapid removal from the ocean and the high background of pre-existing Pu in the waters and sediments, masking the new Fukushima sources. With this data a mass balance will be made between Pu from global fallout, local fallout and

  13. Accumulation of polonium 210Po, uranium (234U and 238U and plutonium (238Pu and 239+240Pu in tissues and organs of deer Carvidae from northern Poland

    Directory of Open Access Journals (Sweden)

    Strumińska-Parulska D. I.


    Full Text Available Livers, kidneys and muscles of large herbivorous animals: roe deer (Capreolus capreolus, red deer (Cervus elaphus and fallow deer (Dama dama, collected in northern Poland, were the subject of the investigation. Polonium, uranium and plutonium activities were measured using alpha spectrometry along with relevant radiochemical procedures. The average concentrations of 210Po ranged between 0.02±0.01 Bq kg−1 ww in muscles and 7.15±0.12 Bq kg−1 ww in kidneys. The concentration of 238U ranged widely between 2.49±0.18 and 69.37±5.45 mBq kg−1 ww. The average concentrations of 239+240Pu ranged between 0.18±0.04 mBq kg−1 ww in muscle and 2.77±0.60 mBq kg−1 ww in kidneys. Statistical analysis showed that the sampling location, sex, age and species did not influence on the radioisotope activities in the analyzed samples.

  14. Chronology of Pu isotopes and 236U in an Arctic ice core. (United States)

    Wendel, C C; Oughton, D H; Lind, O C; Skipperud, L; Fifield, L K; Isaksson, E; Tims, S G; Salbu, B


    In the present work, state of the art isotopic fingerprinting techniques are applied to an Arctic ice core in order to quantify deposition of U and Pu, and to identify possible tropospheric transport of debris from former Soviet Union test sites Semipalatinsk (Central Asia) and Novaya Zemlya (Arctic Ocean). An ice core chronology of (236)U, (239)Pu, and (240)Pu concentrations, and atom ratios, measured by accelerator mass spectrometry in a 28.6m deep ice core from the Austfonna glacier at Nordaustlandet, Svalbard is presented. The ice core chronology corresponds to the period 1949 to 1999. The main sources of Pu and (236)U contamination in the Arctic were the atmospheric nuclear detonations in the period 1945 to 1980, as global fallout, and tropospheric fallout from the former Soviet Union test sites Novaya Zemlya and Semipalatinsk. Activity concentrations of (239+240)Pu ranged from 0.008 to 0.254 mBq cm(-2) and (236)U from 0.0039 to 0.053 μBq cm(-2). Concentrations varied in concordance with (137)Cs concentrations in the same ice core. In contrast to previous published results, the concentrations of Pu and (236)U were found to be higher at depths corresponding to the pre-moratorium period (1949 to 1959) than to the post-moratorium period (1961 and 1962). The (240)Pu/(239)Pu ratio ranged from 0.15 to 0.19, and (236)U/(239)Pu ranged from 0.18 to 1.4. The Pu atom ratios ranged within the limits of global fallout in the most intensive period of nuclear atmospheric testing (1952 to 1962). To the best knowledge of the authors the present work is the first publication on biogeochemical cycles with respect to (236)U concentrations and (236)U/(239)Pu atom ratios in the Arctic and in ice cores.

  15. Almost twenty years' search of transuranium isotopes in effluents discharged to air from nuclear power plants with VVER reactors. (United States)

    Hölgye, Z; Filgas, R


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

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

    Directory of Open Access Journals (Sweden)

    W. T. Bu


    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.

  17. 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. (United States)

    Oikawa, Shinji; Watabe, Teruhisa; Takata, Hyoe


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

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

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


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

  19. Plutonium isotopes in the terrestrial environment at the Savannah River Site, USA: a long-term study. (United States)

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


    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.

  20. Determination of {sup 238}Pu, {sup 239+240}Pu, {sup 241}Pu and {sup 241}Am in radioactive waste from IPEN reactor

    Energy Technology Data Exchange (ETDEWEB)

    Geraldo, Bianca; Taddei, Maria Helena T.; Cheberle, Sandra M.; Ferreira, Marcelo T., E-mail:, E-mail:, E-mail:, E-mail: [Brazilian Nuclear Energy Commission (LAPOC/CNEN-MG), Pocos de Caldas, MG (Brazil). Lab. of Pocos de Caldas; Marumo, Julio T., E-mail: jtmarumo@ipen.b [Instituto de Pesquisas Energeticas e Nucleares (IPEN/CNEN-SP), Sao Paulo, SP (Brazil)


    Ion exchange resin is a common type of radioactive waste arising from treatment of coolant water of the main circuit of research and nuclear power reactors. This waste contains high concentrations of fission and activation products. The management of this waste includes its characterization in order to determine and quantify specific radionuclides including those known as difficult-to-measure radionuclides (RDM). The analysis of RDMs generally involves expensive and time-consuming complex radiochemical analysis for purification and separation of the radionuclides. The objective of this work is to show an easy methodology for quantifying plutonium and americium isotopes in spent ion exchange resin, used for purification of the cooling water of the IEA-R1 reactor located at the Nuclear and Energy Research Institute, IPEN-CNEN/SP. The resins were destroyed by acid digestion, followed by purification and separation of the Pu and Am isotopes with anionic and chromatographic resins. {sup 238}Pu, {sup 239}+{sup 24}'0Pu, and {sup 24}'1Am isotopes were analyzed in an alpha spectrometer equipped with surface barrier detectors. {sup 241}Pu isotope was analyzed by liquid scintillation counting. Chemical recovery yield ranged from 73 to 98% for Pu and 77 to 98% for Am, demonstrating that the methodology is suitable for identification and quantification of the isotopes studied in spent resins. (author)

  1. Analysis on the Isotopic Ratio of Picogram Pu by TIMS%皮克量级钚同位素丰度比的TIMS分析

    Institute of Scientific and Technical Information of China (English)

    杨天丽; 龙开明; 刘雪梅; 刘钊; 汤磊


    The isotopic abundance ratios for Pu at 6.7 pg level were measured by thermal surface ionization mass spectrometry (TIMS). During the preparation of Pu samples carbon power was used as an emitting and stabilizing reagent, which increase the collection efficiency, the ion current intense and the ion emission stability for Pu. The measurment results indicate that the relative standard deviation of 2.7% for the isotopic abundance ratios of 240Pu to 239Pu is achieved when the 240Pu ion current is 8-20 cps.

  2. Measurements of the neutron-induced fission cross sections of /sup 240/Pu and /sup 242/Pu relative to /sup 235/U. [0. 02 to 30 MeV, tables

    Energy Technology Data Exchange (ETDEWEB)

    Behrens, J. W.; Browne, J. C.; Carlson, G. W.


    A continuation is given of the fission-cross-section ratio measurements in progress at the Lawrence Livermore Laboratory. Preliminary results are provided for the /sup 240/Pu//sup 235/U and /sup 242/Pu//sup 235/U ratios from 0.02 to 30 MeV and 0.1 to 30 MeV, respectively. Using the threshold-cross-section method, the ratios were normalized to the values 1.368 +- 0.030 and 1.116 +- 0.025, respectively, from 1.75 to 4.00 MeV.

  3. Radiotoxicological analyses of {sup 239+240}Pu and {sup 241}Am in biological samples by anion-exchange and extraction chromatography: a preliminary study for internal contamination evaluations

    Energy Technology Data Exchange (ETDEWEB)

    Ridone, S.; Arginelli, D.; Bortoluzzi, S.; Canuto, G.; Montalto, M.; Nocente, M.; Vegro, M. [Italian National Agency for New Technologies, Energy and the Environment (ENEA), Research Centre of Saluggia, Radiation Protection Institute, Saluggia, VC (Italy)


    Many biological samples (urines and faeces) have been analysed by means of chromatographic extraction columns, utilising two different resins (AG 1-X2 resin chloride and T.R.U.), in order to detect the possible internal contamination of {sup 239{sup +}}{sup 240}Pu and {sup 241}Am, for some workers of a reprocessing nuclear plant in the decommissioning phase. The results obtained show on one hand the great suitability of the first resin for the determination of plutonium, and on the other the great selectivity of the second one for the determination of americium.

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

    Institute of Scientific and Technical Information of China (English)


    <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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Yamada, Masatoshi [Department of Radiation Chemistry, Institute of Radiation Emergency Medicine, Hirosaki University, Hirosaki, 036-8564, Aomori (Japan); Zheng, Jian [Research Center for Radiation Protection, National Institute of Radiological Sciences, 4-9-1 Anagawa, Inage, 263-8555, Chiba (Japan)


    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 {sup 240}Pu/{sup 239}Pu 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 {sup 240}Pu/{sup 239}Pu 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 {sup 240}Pu/{sup 239}Pu 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 {sup 239+240}Pu concentrations and {sup 240}Pu/{sup 239}Pu 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 {sup 239}Pu and {sup 240}Pu concentrations and {sup 240}Pu/{sup 239}Pu 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

  6. The plutonium isotopic composition of marine biota on Enewetak Atoll: a preliminary assessment. (United States)

    Hamilton, Terry F; Martinelli, Roger E; Kehl, Steven R; McAninch, Jeffrey E


    We have determined the level and distribution of gamma-emitting radionuclides, plutonium activity concentrations, and 240Pu/239Pu atom ratios in tissue samples of giant clam (Tridacna gigas and Hippopus hippopus), a top snail (Trochus nilaticas) and sea cucumber (Holothuria atra) collected from different locations around Enewetak Atoll. The plutonium isotopic measurements were performed using ultra-high sensitivity accelerator mass spectrometry (AMS). Elevated levels of plutonium were observed in the stomachs (includes the stomach lining) of Tridacna clam (0.62 to 2.98 Bq kg(-1), wet wt.), in the soft parts (edible portion) of top snails (0.25 to 1.7 Bq kg(-1)), wet wt.) and, to a lesser extent, in sea cucumber (0.015 to 0.22 Bq kg(-1), wet wt.) relative to muscle tissue concentrations in clam (0.006 to 0.021 Bq kg(-1), wet wt.) and in comparison with previous measurements of plutonium in fish. These data and information provide a basis for re-evaluating the relative significance of dietary intakes of plutonium from marine foods on Enewetak Atoll and, perhaps most importantly, demonstrate that discrete 240Pu239Pu isotope signatures might well provide a useful investigative tool to monitor source-term attribution and consequences on Enewetak Atoll. One potential application of immediate interest is to monitor and assess the health and ecological impacts of leakage of plutonium (as well as other radionuclides) from a low-level radioactive waste repository on Runit Island relative to background levels of fallout contamination in Enewetak Atoll lagoon.

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

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Roos, Per


    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...

  8. 232Th、233U、238Pu、240Pu、242Pu、241Am、242Cm、243Cm和244Cm的裂变释放热能研究%Thermal Energy Released in Fission of 232 Th,233 U,238 Pu, 240 Pu,242 Pu,241 Am,242 Cm,243 Cm and 244 Cm

    Institute of Scientific and Technical Information of China (English)

    赵艳飞; 马续波; 陈义学


    In the nuclear reactor design ,the precise calculation of thermal fission energy is of great significance .In the pressurized water reactor ,high energy neutron-induced fission rarely occurs ,the isotopes including 233 U ,241 Am and 243 Cm are mostly induced by thermal neutrons ,while the other isotopes such as 232Th ,238Pu ,240Pu ,242Pu ,242Cm and 244 Cm are by fast neutron . In order to carry out this work , the nuclear data extracted from the latest evaluated nuclear data file (ENDF/B-Ⅶ ) were adopted ,and the energy-conservation law for the calculation of total fission energy were used , meanw hile ,with the consideration of capture energy and the correction of βand γ ,the thermal fission energy of nine isotopes was obtained .Compared with the data excerpted from IAEA issued WIMS-D database ,the results are reasonable .The thermal fission energy and its uncertainties of the nine isotopes are :(193.939 ± 0.176) MeV for 232 Th , (200.063 ± 0.084) MeV for 233 U ,(208.786 ± 1.133 ) MeV for 238 Pu ,(211.266 ± 0.220 ) MeV for 240 Pu ,(213.862 ± 0.299 ) MeV for 242 Pu ,(215.077 ± 0.210 ) MeV for 241 Am ,(218.821 ± 0.159) MeV for 242Cm ,(218.525 ± 0.388) MeV for 243Cm ,and (220.067 ± 0.131) MeV for 244 Cm ,respectively .%在核反应堆设计中,对每次裂变释放热能进行精确计算具有重要意义。在压水堆内,高能中子诱发核裂变份额很小,233 U、241 Am、243 Cm主要由热中子诱发裂变,232 T h、238 Pu、240 Pu、242 Pu、242 Cm、244 Cm主要由快中子诱发裂变。本文采用最新的核评价数据库 ENDF/B-Ⅶ,利用质量守恒法计算裂变释放总能,同时研究了中微子带走的能量,中子俘获能及β、γ修正项,最终给出了9种核素裂变释放热能。与IAEA颁布的WIMS-D格式数据库中的裂变释放热能数据的对比表明,本文所用方法计算结果合理。9种核素每次裂变释放热能分别为:232 Th ,(193.939±0.176) MeV ;233 U ,(200.063

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

    Energy Technology Data Exchange (ETDEWEB)

    Wendel, C.C., E-mail: [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: [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: [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Skipperud, L., E-mail: [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: [Department of Nuclear Physics, Australian National University, Canberra ACT 0200 (Australia); Isaksson, E., E-mail: [Norwegian Polar Institute, Fram Centre, Hjalmar Johansens Gate 14, N9296 Tromsø (Norway); Tims, S.G., E-mail: [Department of Nuclear Physics, Australian National University, Canberra ACT 0200 (Australia); Salbu, B., E-mail: [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway)


    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

  10. Plutonium isotopes in the atmosphere of Central Europe: Isotopic composition and time evolution vs. circulation factors. (United States)

    Kierepko, Renata; Mietelski, Jerzy W; Ustrnul, Zbigniew; Anczkiewicz, Robert; Wershofen, Herbert; Holgye, Zoltan; Kapała, Jacek; Isajenko, Krzysztof


    This paper reports evidence of Pu isotopes in the lower part of the troposphere of Central Europe. The data were obtained based on atmospheric aerosol fraction samples collected from four places in three countries (participating in the informal European network known as the Ring of Five (Ro5)) forming a cell with a surface area of about 200,000km(2). We compared our original data sets from Krakow (Poland, 1990-2007) and Bialystok (Poland, 1991-2007) with the results from two other locations, Prague (Czech Republic; 1997-2004) and Braunschweig (Germany; 1990-2003) to find time evolution of the Pu isotopes. The levels of the activity concentration for (238)Pu and for ((239+240))Pu were estimated to be a few and some tens of nBqm(-3), respectively. However, we also noted some results were much higher (even about 70 times higher) than the average concentration of (238)Pu in the atmosphere. The achieved complex data sets were used to test a new approach to the problem of solving mixing isotopic traces from various sources (here up to three) in one sample. Results of our model, supported by mesoscale atmospheric circulation parameters, suggest that Pu from nuclear weapon accidents or tests and nuclear burnt-up fuel are present in the air.

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

    DEFF Research Database (Denmark)

    Xu, Yihong; Qiao, Jixin; Hou, Xiaolin


    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...

  12. Ultratrace and isotope ratios analyses of some radionuclides by ICP-MS

    Energy Technology Data Exchange (ETDEWEB)

    Helal, A.I.; Zahran, N.F.; Abd El-Lateef, A.M.; Mohsen, H.T. [Central Lab. for Elemental and Isotopic Analysis, N.R.C. Atomic Energy Authority, Cairo (Egypt); Amr, M.A. [Central Lab. for Elemental and Isotopic Analysis, N.R.C. Atomic Energy Authority, Cairo (Egypt); Nuclear Physics Dept., N.R.C., Atomic Energy Authority, Cairo (Egypt); Bashter, I.I. [Physics Dept., Faculty of Science, Zagazig Univ. (Egypt); Abbas, Y. [Physics Dept., Faculty of Science, Suez Canal Univ., Ismailia (Egypt)


    Extensive work is under way using high resolution-ICP-MS for {sup 90}Sr, {sup 234}U, {sup 235}U, {sup 238}U, {sup 239}Pu, {sup 240}Pu, and {sup 241}Am detection. Sample preparation procedures based on liquid-liquid extraction and ion exchange chromatography were developed. Sr, U, Pu, and Am were separated from their matrix and concentrated to improve the power of detection in the mass spectrometer. A microconcentric nebulizer with a desolvation introduction system (Ardius) is used. Instrumental limits of detection using Sr and U standard solutions are 0.01 ppt and 0.006 ppt for Sr and U, respectively. A study is presented on the mass interferences for the specified radionuclides. In the environmental samples investigated the {sup 90}Sr/{sup 86}Sr isotope ratio is 6.02 x 10{sup -9} and for {sup 240}Pu/{sup 239}Pu the isotope ratio is 0.17. (orig.)

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

    Energy Technology Data Exchange (ETDEWEB)

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


    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)

  14. The effect of permafrost on soil erosion using meteoric 10Be, 137Cs and 239+240Pu in the Eastern Swiss Alps (United States)

    Pichler, Barbara; Brandovà, Dagmar; Alewell, Christine; Ivy-Ochs, Susan; Kubik, Peter W.; Kneisel, Christof; Meusburger, Katrin; Ketterer, Michael; Egli, Markus


    Permafrost ecosystems are highly sensitive to climate warming. The expected changes in the thermal and hydrological soil regime might have crucial consequences on soil erosion processes. Therefore, the determination of erosional activities on the long- (since the beginning of soil formation) and mid-term (last 50-60 yr) using cosmogenic and anthropogenic radionuclides can provide important information on past and ongoing processes. Permafrost soils in the Alps and their behaviour with climate change are only rarely studied. The expected new insights will lead to a better understanding of the processes of high mountain soils and are a further step towards improving climate-related modelling of fast warming scenarios and increasing system disequilibria. Our aim is to quantify soil erosion processes in permafrost soils and nearby unfrozen soils in the Alpine (sites at 2700 m asl) and the sub-Alpine (sites 1800 m asl) range of the Swiss Alps (Upper Engadine). We hypothesise that permafrost soils differ distinctly in their long- and mid-term soil erosion rates due to different water retention capacities. Long-term soil erosion was assessed using meteoric 10Be. Meteoric 10Be in a soil profile was estimated assuming that it is has been deposited as a function of precipitation and adsorbed in the fine earth fraction (

  15. Depositional behaviors of plutonium and thorium isotopes at Tsukuba and Mt. Haruna in Japan indicate the sources of atmospheric dust. (United States)

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


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

  16. Detection of long-lived plutonium isotopes in environmental samples by Accelerator Mass Spectrometry (AMS)

    Energy Technology Data Exchange (ETDEWEB)

    Hain, Karin; Faestermann, Thomas; Fimiani, Leticia; Gomez Guzman, Jose Manuel; Korschinek, Gunther; Ludwig, Peter [Technische Universitaet Muenchen (Germany); Shinonaga, Taeko [Helmholtz Zentrum Muenchen (Germany)


    The Plutonium isotopes {sup 239}Pu (T{sub 1/2}=2.4.10{sup 4}a), {sup 240}Pu (T{sub 1/2}=6.5.10{sup 3}a) and {sup 242}Pu (T{sub 1/2}=3.7.10{sup 5}a) are anthropogenic radionuclides emitted into the environment by nuclear activities. Pu is accumulated in the human body and hence, poses a considerable hazard to human health. Due to the long half-lives, these isotopes are present in the biosphere on large time scales and a build-up can be expected. Therefore it is important to study the contamination pathway of Pu into the drinking water. At the Maier-Leibnitz-Laboratory in Munich a method to detect long-lived Pu isotopes by Accelerator Mass Spectrometry (AMS) is being developed. AMS requires only few milligrams of sample material, which is a substantial advantage over decay counting techniques. Consequently, more samples from different locations can be taken which is essential when searching for locally increased Pu concentrations as in the Pacific Ocean after the Fukushima accident in March 2011. Samples from different locations in the Pacific Ocean and from the snow-hydrosphere are planned to be investigated by AMS. The principle detection method using AMS and an overview of the status of the project is presented.

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

    DEFF Research Database (Denmark)

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


    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...

  18. AMS of the Minor Plutonium Isotopes. (United States)

    Steier, P; Hrnecek, E; Priller, A; Quinto, F; Srncik, M; Wallner, A; Wallner, G; Winkler, S


    VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure (239)Pu, (240)Pu, (241)Pu, (242)Pu and (244)Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of (244)Pu/(239)Pu = (5.7 ± 1.0) × 10(-5) based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the (242)Pu/(240)Pu ratio as an estimate of the initial (241)Pu/(239)Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method.

  19. Plutonium isotopes and 241Am in the atmosphere of Lithuania: A comparison of different source terms (United States)

    Lujanienė, G.; Valiulis, D.; Byčenkienė, S.; Šakalys, J.; Povinec, P. P.


    137Cs, 241Am and Pu isotopes collected in aerosol samples during 1994-2011 were analyzed with special emphasis on better understanding of Pu and Am behavior in the atmosphere. The results from long-term measurements of 240Pu/239Pu atom ratios showed a bimodal frequency distribution with median values of 0.195 and 0.253, indicating two main sources contributing to the Pu activities at the Vilnius sampling station. The low Pu atom ratio of 0.141 could be attributed to the weapon-grade plutonium derived from the nuclear weapon test sites. The frequency of air masses arriving from the North-West and North-East correlated with the Pu atom ratio indicating the input from the sources located in these regions (the Novaya Zemlya test site, Siberian nuclear plants), while no correlation with the Chernobyl region was observed. Measurements carried out during the Fukushima accident showed a negligible impact of this source with Pu activities by four orders of magnitude lower as compared to the Chernobyl accident. The activity concentration of actinides measured in the integrated sample collected in March-April, 2011 showed a small contribution of Pu with unusual activity and atom ratios indicating the presence of the spent fuel of different origin than that of the Chernobyl accident.

  20. Highly enriched isotope samples of uranium and transuranium elements for scientific investigation (United States)

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


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

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

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


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

  2. Sequential determination of natural ({sup 232}Th, {sup 238}U) and anthropogenic ({sup 137}Cs, {sup 90}Sr, {sup 241}Am, {sup 239+240}Pu) radionuclides in environmental matrix

    Energy Technology Data Exchange (ETDEWEB)

    Michel, H.; Levent, D.; Barci, V.; Barci-Funel, G.; Hurel, C. [Laboratoire de Radiochimie, Sciences Analytiques et Environnement (LRSAE), Universite de Nice Sophia-Antipolis 06108 Nice Cedex (France)


    A new sequential method for the determination of both natural (U, Th) and anthropogenic (Sr, Cs, Pu, Am) radionuclides has been developed for application to soil and sediment samples. The procedure was optimised using a reference sediment (IAEA-368) and reference soils (IAEA-375 and IAEA-326). Reference materials were first digested using acids (leaching), 'total' acids on hot plate, and acids in microwave in order to compare the different digestion technique. Then, the separation and purification were made by anion exchange resin and selective extraction chromatography: Transuranic (TRU) and Strontium (SR) resins. Natural and anthropogenic alpha radionuclides were separated by Uranium and Tetravalent Actinide (UTEVA) resin, considering different acid elution medium. Finally, alpha and gamma semiconductor spectrometer and liquid scintillation spectrometer were used to measure radionuclide activities. The results obtained for strontium-90, cesium-137, thorium-232, uranium- 238, plutonium-239+240 and americium-241 isotopes by the proposed method for the reference materials provided excellent agreement with the recommended values and good chemical recoveries. (authors)

  3. Novel insights into Fukushima nuclear accident from isotopic evidence of plutonium spread along coastal rivers. (United States)

    Evrard, Olivier; Pointurier, Fabien; Onda, Yuichi; Chartin, Caroline; Hubert, Amélie; Lepage, Hugo; Pottin, Anne-Claire; Lefèvre, Irène; Bonté, Philippe; Laceby, J Patrick; Ayrault, Sophie


    The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident led to important releases of radionuclides into the environment, and trace levels of plutonium (Pu) were detected in northeastern Japan. However, measurements of Pu isotopic atom and activity ratios are required to differentiate between the contributions of global nuclear test fallout and FDNPP emissions. In this study, we used a double-focusing sector field ICP-MS to measure Pu atom and activity ratios in recently deposited sediment along rivers draining the most contaminated part of the inland radioactive plume. Results showed that plutonium isotopes (i.e., (239)Pu, (240)Pu, (241)Pu, and (242)Pu) were detected in all samples, although in extremely low concentrations. The (241)Pu/(239)Pu atom ratios measured in sediment deposits (0.0017-0.0884) were significantly higher than the corresponding values attributed to the global fallout (0.00113 ± 0.00008 on average for the Northern Hemisphere between 31°-71° N: Kelley, J. M.; Bond, L. A.; Beasley, T. M. Global distribution of Pu isotopes and (237)Np. Sci. Total. Env. 1999, 237/238, 483-500). The results indicated the presence of Pu from FDNPP, in slight excess compared to the Pu background from global fallout that represented up to ca. 60% of Pu in the analyzed samples. These results demonstrate that this radionuclide has been transported relatively long distances (∼45 km) from FDNPP and been deposited in rivers representing a potential source of Pu to the ocean. In future, the high (241)Pu/(239)Pu atom ratio of the Fukushima accident sourced-Pu should be measured to quantify the supply of continental-originating material from Fukushima Prefecture to the Pacific Ocean.

  4. Preparation of a multi-isotope plutonium AMS standard and preliminary results of a first inter-lab comparison (United States)

    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.


    The motivation of this work is to establish a new multi-isotope plutonium standard for isotopic ratio measurements with accelerator mass spectrometry (AMS), since stocks of existing solutions are declining. To this end, certified reference materials (CRMs) of each of the individual isotopes 239Pu, 240Pu, 242Pu and 244Pu were obtained from JRC IRMM (Joint Research Center Institute for Reference Materials and Measurements). These certified reference materials (IRMM-081a, IRMM-083, IRMM-043 and IRMM-042a) were diluted with nitric acid and mixed to obtain a stock standard solution with an isotopic ratio of approximately 1.0:1.0:1.0:0.1 (239Pu:240Pu:242Pu:244Pu). From this stock solution, samples were prepared for measurement of the plutonium isotopic composition by AMS. These samples have been measured in a round-robin exercise between the AMS facilities at CologneAMS, at the ANU Canberra and ETH Zurich to verify the isotopic ratio and to demonstrate the reproducibility of the measurements. The results show good agreement both between the different AMS measurements and with the gravimetrically determined nominal ratios.

  5. Conversion electron spectrometry of Pu isotopes with a silicon drift detector. (United States)

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


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

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

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


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

  7. {\\alpha}-accompanied cold ternary fission of $^{238-244}$Pu isotopes in equatorial and collinear configuration

    CERN Document Server

    Santhosh, K P; Priyanka, B


    The cold ternary fission of $^{238}$Pu, $^{240}$Pu, $^{242}$Pu and $^{244}$Pu isotopes, with $^{4}$He as light charged particle, in equatorial and collinear configuration has been studied within the Unified ternary fission model (UTFM). The fragment combination $^{100}$Zr+$^{4}$He+$^{134}$Te possessing the near doubly magic nuclei $^{134}$Te (N=82, Z=52) gives the highest yield in the alpha accompanied ternary fission of $^{238}$Pu. For the alpha accompanied ternary fission of $^{240}$Pu, $^{242}$Pu and $^{244}$Pu isotopes, the highest yield was found for the fragment combination with doubly magic nuclei $^{132}$Sn (N=82, Z=50) as the heavier fragment. The deformation and orientation of fragments have also been taken into account for the alpha accompanied ternary fission of $^{238-244}$Pu isotopes, and it has been found that in addition to closed shell effect, ground state deformation also plays an important role in determining the isotopic yield in the ternary fission process. The emission probability and ki...

  8. Isotopic composition and distribution of plutonium in northern South China Sea sediments revealed continuous release and transport of Pu from the Marshall Islands. (United States)

    Wu, Junwen; Zheng, Jian; Dai, Minhan; Huh, Chih-An; Chen, Weifang; Tagami, Keiko; Uchida, Shigeo


    The (239+240)Pu activities and (240)Pu/(239)Pu atom ratios in sediments of the northern South China Sea and its adjacent Pearl River Estuary were determined to examine the spatial and temporal variations of Pu inputs. We clarified that Pu in the study area is sourced from a combination of global fallout and close-in fallout from the Pacific Proving Grounds in the Marshall Islands where above-ground nuclear weapons testing was carried out during the period of 1952-1958. The latter source dominated the Pu input in the 1950s, as evidenced by elevated (240)Pu/(239)Pu atom ratios (>0.30) in a dated sediment core. Even after the 1950s, the Pacific Proving Grounds was still a dominant Pu source due to continuous transport of remobilized Pu from the Marshall Islands, about 4500 km away, along the North Equatorial Current followed by the transport of the Kuroshio current and its extension into the South China Sea through the Luzon Strait. Using a simple two end-member mixing model, we have quantified the contributions of Pu from the Pacific Proving Grounds to the northern South China Sea shelf and the Pearl River Estuary are 68% ± 1% and 30% ± 5%, respectively. This study also confirmed that there were no clear signals of Pu from the Fukushima Daiichi Nuclear Power Plant accident impacting the South China Sea.

  9. Plutonium and Uranium Atom Ratios and Activity Levels in Cochiti Lake Bottom Sediments Provided by Pueblo de Cochiti

    Energy Technology Data Exchange (ETDEWEB)

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


    Historical operations at the Los Alamos National Laboratory have contaminated stream sediments with plutonium and other radionuclides. A small portion of these contaminated sediments has been carried by floods into the Rio Grande drainage system, eventually to be trapped by Cochiti Lake located on Pueblo de Cochiti lands approximately 8 km downstream of the Laboratory. In this study, lake bottom sediment samples provided by the Pueblo de Cochiti were analyzed by thermal ionization mass spectrometry to determine plutonium and uranium activity levels and isotopic atom ratios. This specialized analytical method allows us to take isotopic fingerprints of radionuclides found in the sediment and to determine how much plutonium and uranium came from the Laboratory and how much was deposited by worldwide fallout or is natural. Two distinct types of samples were processed: segments of a continuous vertical core of the entire accumulated sediment sequence and other samples from across the lake bottom at the water/sediment interface. Based on measurement of the {sup 240}Pu/{sup 239}Pu atom ratio, Laboratory-derived plutonium is present in eight of nine samples at the core site. On a depth-weighted basis, approximately one-half of the {sup 239}Pu and {sup 240}Pu came from early operations at the Laboratory; the remaining plutonium came from fallout dispersed by above-ground nuclear tests. In contrast to the core site, the samples from the other locations showed little or no evidence of Laboratory-derived plutonium, with more than 90 percent of the plutonium attributable to fallout. The overall amount of plutonium in all the samples is of the same magnitude as other reservoirs in the region. The net increase in plutonium over upstream reservoirs unaffected by Laboratory activities is a maximum of 0.014 pCi/g or 3.5 times. All of the samples reflect natural uranium compositions. Laboratory-derived uranium is not identifiable, presumably because the sediment contains abundant

  10. Multi-collector Isotope Ratio Mass Spectrometer -- Operational Performance Report

    Energy Technology Data Exchange (ETDEWEB)

    Appelhans, Anthony D; Olson, John E; Watrous, Matthew G; Ward, Michael B.; Dahl, David A.


    This report describes the operational testing of a new magnetic sector mass spectrometer that utilizes seven full-sized discrete dynode electron multipliers operating simultaneously. The instrument includes a newly developed ion dispersion lens that enables the mass dispersed individual isotope beams to be separated sufficiently to allow a full-sized discrete dynode pulse counting multiplier to be used to measure each isotope beam. The performance of the instrument was measured using SRM 996 (244Pu spike) at loadings of 2.4 and 12 fg on resin beads and with SRM 4350B Columbia River Sediment samples. The measured limit of detection (3s) for 240Pu was 3.4 attograms for SRM 996. The limit of quantitation (LOQ), defined as 10 s, was 11.2 attograms. The measured concentration of 239Pu in the CRS standard was 152 ± 6 fg/g.

  11. {sup 90}Sr, {sup 238}U, {sup 234}U, {sup 137}Cs, {sup 40}K and {sup 239/240}Pu in Emmental type cheese produced in different regions of Western Europe

    Energy Technology Data Exchange (ETDEWEB)

    Froidevaux, P. E-mail:; Geering, J.-J.; Pillonel, L.; Bosset, J.-O.; Valley, J.-F


    A method is presented for the determination of {sup 90}Sr and uranium in Emmental type cheese collected in dairy plants from different European countries. Results display a significant correlation (r=0.708, Student t-test=6.02) between the {sup 90}Sr content of the cheese and the altitude of grazing. The highest {sup 90}Sr activity is 1.13 Bq kg{sup -1} of cheese and the lowest is 0.29 Bq kg{sup -1}. Uranium activity is very low with a highest {sup 238}U value of 27 mBq kg{sup -1}. In addition, {sup 234}U/{sup 238}U ratio shows a large enrichment in {sup 234}U for every location. Without any significant indication of the geographic origin of the cheese, this enrichment is believed to be due to the geological features of the pasture, soil and underground water. These results tend to prove that the contamination of milk by uranium originates principally from the water that the cows drink instead of the forage. This finding may have a great importance in models dealing with dairy food contamination by radionuclides following a nuclear accident. Also, the {sup 90}Sr content and to a lesser extent the {sup 234}U/{sup 238}U ratio could be used to trace the authenticity of the origin of the cheese. {sup 137}Cs activity is lower than the detection limit of 0.1 Bq kg{sup -1} in all the samples collected (n=20). Based on natural {sup 40}K activity in cheese (15-21 Bq kg{sup -1}), the decontamination factor for the alkaline cations from milk to cheese is about 20. Plutonium activity stays below the detection limit of 0.3 mBq kg{sup -1}.

  12. Plutonium Isotopes ((239-241)Pu) Dissolved in Pacific Ocean Waters Detected by Accelerator Mass Spectrometry: No Effects of the Fukushima Accident Observed. (United States)

    Hain, Karin; Faestermann, Thomas; Fimiani, Leticia; Golser, Robin; Gómez-Guzmán, José Manuel; Korschinek, Gunther; Kortmann, Florian; Lierse von Gostomski, Christoph; Ludwig, Peter; Steier, Peter; Tazoe, Hirofumi; Yamada, Masatoshi


    The concentration of plutonium (Pu) and the isotopic ratios of (240)Pu to (239)Pu and (241)Pu to (239)Pu were determined by accelerator mass spectrometry (AMS) in Pacific Ocean water samples (20 L each) collected in late 2012. The isotopic Pu ratios are important indicators of different contamination sources and were used to identify a possible release of Pu into the ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. In particular, (241)Pu is a well-suited indicator for a recent entry of Pu because (241)Pu from fallout of nuclear weapon testings has already significantly decayed. A total of 10 ocean water samples were prepared at the Radiochemie München of the TUM and analyzed at the Vienna Environmental Research Laboratory (VERA). Several samples showed a slightly elevated (240)Pu/(239)Pu ratio of up to 0.22 ± 0.02 compared to global fallout ((240)Pu/(239)Pu = 0.180 ± 0.007), whereas all measured (241)Pu-to-(239)Pu ratios were consistent with nuclear weapon fallout ((241)Pu/(239)Pu < 2.4 × 10(-3)), which means that no impact from the Fukushima accident was detected. From the average (241)Pu-to-(239)Pu ratio of 8-2(+3) ×10(-4) at a sampling station located at a distance of 39.6 km to FDNPP, the 1-σ upper limit for the FDNPP contribution to the (239)Pu inventory in the water column was estimated to be 0.2%. Pu, with the signature of weapon-grade Pu was found in a single sample collected around 770 km off the west coast of the United States.

  13. Natural decrease of the intensity level of artificial radioactive isotopes in the Barents Sea (United States)

    Matishov, G. G.; Matishov, D. G.; Solatie, D.; Kasatkina, N. E.; Leppanen, A.


    The results of radioecological investigations carried out within the framework of the Russian-Finnish high-latitude expedition in 2007 are presented. The characteristics of the present-day accumulation level of the significant radioecological isotopes 137Cs, 90Sr and 239,240Pu in the Barents Sea are described. The comparative analysis is performed for the radiation pollution of the environment in the 1980s and 1990s and in the first decade of the 21st century. Natural purification processes in the marine environment are the main factors of the decrease in the intensity level of artificial radioactive isotopes. These processes include repeated dilution, nuclear decay, occlusion by sediments and suspended solid material, and accumulation by aquatic inhabitants. A stable decreasing trend is observed for the intensity level of artificial radioactive isotopes in the Barents Sea.

  14. Chromium Isotope Behaviour During Aerobic Microbial Reduction Activities (United States)

    Zhang, Q.; Amor, K.; Porcelli, D.; Thompson, I.


    Microbial activity is a very important, and possibly even the dominant, reduction mechanism for many metals in natural water systems. Isotope fractionations during microbial metal reduction can reflect one major mechanism in metal cycling in the environment, and isotopic signatures can be used to identify and quantify reduction processes during biogeochemical cycling in the present environment as well as in the past. There are many Cr (VI)-reducing bacteria that have been discovered and isolated from the environment, and Cr isotopes were found to be fractionated during microbial reduction processes. In this study, Cr reduction experiments have been undertaken to determine the conditions under which Cr is reduced and the corresponding isotope signals that are generated. The experiments have been done with a facultative bacteria Pseudomonas fluorescens LB 300, and several parameters that have potential impact on reduction mechanisms have been investigated. Electron donors are important for bacteria growth and metabolism. One factor that can control the rate of Cr reduction is the nature of the electron donor. The results show that using citrate as an electron donor can stimulate bacteria reduction activity to a large extent; the reduction rate is much higher (15.10 mgˑL-1hour-1) compared with experiments using glucose (6.65 mgˑL-1ˑhour-1), acetate (4.88 mgˑL-1hour-1) or propionate (4.85 mgˑL-1hour-1) as electron donors. Groups with higher electron donor concentrations have higher reduction rates. Chromium is toxic, and when increasing Cr concentrations in the medium, the bacteria reduction rate is also higher, which reflects bacteria adapting to the toxic environment. In the natural environment, under different pH conditions, bacteria may metabolise in different ways. In our experiments with pH, bacteria performed better in reducing Cr (VI) when pH = 8, and there are no significant differences between groups with pH = 4 or pH = 6. To investigate this further, Cr

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

    Energy Technology Data Exchange (ETDEWEB)

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


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

  16. 福岛核事故向环境释放的 Pu研究进展%Plutonium Isotopes Released f rom Fukushima Daiichi Nuclear Power Plant Accident into Environment

    Institute of Scientific and Technical Information of China (English)

    倪有意; 卜文庭; 郭秋菊; 胡丹; 许宏


    福岛核事故向环境释放的放射性核素中包含了锕系元素Pu ,其中以极毒组的239 Pu、240 Pu和高毒组的241 Pu为主。本文总结并分析了针对福岛核事故向环境释放的 Pu的相关研究。据估计,福岛核事故向环境中排放的239+240 Pu总量约为109 Bq ,是切尔诺贝利核事故排放量的万分之一。此次事故排放的Pu同位素原子比(240 Pu/239 Pu和241 Pu/239 Pu)及活度比(A (238 Pu)/A (239+240 Pu))明显异于全球沉降值,可作为事故中Pu溯源的判定依据。事故所排放的Pu全部来源于核电站1~3号反应堆堆芯而非乏燃料池。现有研究报道的数据表明,在福岛核电站周围30 km范围内的陆地环境中存在来自核事故排放的Pu污染,污染相对严重的“热点”区域和该地区与核电站的相对位置没有明显关联,主要是受地形和降水的影响。而对于人们关心的海洋环境,来自福岛核事故的Pu污染非常小。核事故向海洋中排放的Pu相对于核事故前海洋环境中的Pu污染水平可忽略不计。%On March 11 , 2011 , a catastrophic tsunami induced by a magnitude 9.0 earthquake caused the terrible Fukushima Daiichi Nuclear Power Plant (FDNPP) acci‐dent ,leading to the release of a large amount of radionuclides into the environment .T he published studies on plutonium isotopes in the environment after the FDNPP accident were reviewed in this paper .The total atmospheric released amounts of Pu from the FDNPP accident were estimated to be 109 Bq ,that is only 1/10 000 of that released from the Chernobyl accident .The Pu isotopes were released from the damaged reactors ,not from the spent fuel pools in the FDNPP .The Pu isotopic ratios (240 Pu/239 Pu ,241 Pu/239 Pu) and activity ratios of A(238 Pu)/A(239+ 240 Pu) were significantly different from that of global fallout ,serving as powerful fingerprints for Pu source identification .To date , the plutonium

  17. Examining Changes in Radioxenon Isotope Activity Ratios during Subsurface Transport (United States)

    Annewandter, Robert


    The Non-Proliferation Experiment (NPE) has demonstrated and modelled the usefulness of barometric pumping induced gas transport and subsequent soil gas sampling during On-Site inspections. Generally, gas transport has been widely studied with different numerical codes. However, gas transport of radioxenons and radioiodines in the post-detonation regime and their possible fractionation is still neglected in the open peer-reviewed literature. Atmospheric concentrations of the radioxenons Xe-135, Xe-133m, Xe-133 and Xe-131m can be used to discriminate between civilian releases (nuclear power plants or medical isotope facilities), and nuclear explosion sources. It is based on the multiple isotopic activity ratio method. Yet it is not clear whether subsurface migration of the radionuclides, with eventual release into the atmosphere, can affect the activity ratios due to fractionation. Fractionation can be caused by different mass diffusivities due to mass differences between the radionuclides. Cyclical changes in atmospheric pressure can drive subsurface gas transport. This barometric pumping phenomenon causes an oscillatoric flow in upward trending fractures or highly conductive faults which, combined with diffusion into the porous matrix, leads to a net transport of gaseous components - a so-called ratcheting effect. We use a general purpose reservoir simulator (Complex System Modelling Platform, CSMP++) which is recognized by the oil industry as leading in Discrete Fracture-Matrix (DFM) simulations. It has been applied in a range of fields such as deep geothermal systems, three-phase black oil simulations, fracture propagation in fractured, porous media, and Navier-Stokes pore-scale modelling among others. It is specifically designed to account for structurally complex geologic situation of fractured, porous media. Parabolic differential equations are solved by a continuous Galerkin finite-element method, hyperbolic differential equations by a complementary finite

  18. Plutonium isotope ratio variations in North America

    Energy Technology Data Exchange (ETDEWEB)

    Steiner, Robert E [Los Alamos National Laboratory; La Mont, Stephen P [Los Alamos National Laboratory; Eisele, William F [Los Alamos National Laboratory; Fresquez, Philip R [Los Alamos National Laboratory; Mc Naughton, Michael [Los Alamos National Laboratory; Whicker, Jeffrey J [Los Alamos National Laboratory


    Historically, approximately 12,000 TBq of plutonium was distributed throughout the global biosphere by thermo nuclear weapons testing. The resultant global plutonium fallout is a complex mixture whose {sup 240}Pu/{sup 239}Pu atom ratio is a function of the design and yield of the devices tested. The average {sup 240}Pu/{sup 239}Pu atom ratio in global fallout is 0.176 + 014. However, the {sup 240}Pu/{sup 239}Pu atom ratio at any location may differ significantly from 0.176. Plutonium has also been released by discharges and accidents associated with the commercial and weapons related nuclear industries. At many locations contributions from this plutonium significantly alters the {sup 240}Pu/{sup 239}Pu atom ratios from those observed in global fallout. We have measured the {sup 240}Pu/{sup 239}Pu atom ratios in environmental samples collected from many locations in North America. This presentation will summarize the analytical results from these measurements. Special emphasis will be placed on interpretation of the significance of the {sup 240}Pu/{sup 239}Pu atom ratios measured in environmental samples collected in the Arctic and in the western portions of the United States.

  19. Non-destructive measurement of carbonic anhydrase activity and the oxygen isotope composition of soil water (United States)

    Jones, Sam; Sauze, Joana; Ogée, Jérôme; Wohl, Steven; Bosc, Alexandre; Wingate, Lisa


    Carbonic anhydrases are a group of metalloenzymes that catalyse the hydration of aqueous carbon dioxide (CO2). The expression of carbonic anhydrase by bacteria, archaea and eukarya has been linked to a variety of important biological processes including pH regulation, substrate supply and biomineralisation. As oxygen isotopes are exchanged between CO2 and water during hydration, the presence of carbonic anhydrase in plants and soil organisms also influences the oxygen isotope budget of atmospheric CO2. Leaf and soil water pools have distinct oxygen isotope compositions, owing to differences in pool sizes and evaporation rates, which are imparted on CO2during hydration. These differences in the isotopic signature of CO2 interacting with leaves and soil can be used to partition the contribution of photosynthesis and soil respiration to net terrestrial CO2 exchange. However, this relies on our knowledge of soil carbonic anhydrase activity and currently, the prevalence and function of these enzymes in soils is poorly understood. Isotopic approaches used to estimate soil carbonic anhydrase activity typically involve the inversion of models describing the oxygen isotope composition of CO2 fluxes to solve for the apparent, potentially catalysed, rate of oxygen exchange during hydration. This requires information about the composition of CO2 in isotopic equilibrium with soil water obtained from destructive, depth-resolved soil water sampling. This can represent a significant challenge in data collection given the considerable potential for spatial and temporal variability in the isotopic composition of soil water and limited a priori information with respect to the appropriate sampling resolution and depth. We investigated whether we could circumvent this requirement by constraining carbonic anhydrase activity and the composition of soil water in isotopic equilibrium with CO2 by solving simultaneously the mass balance for two soil CO2 steady states differing only in the

  20. Ultra-trace plutonium determination in small volume seawater by sector field inductively coupled plasma mass spectrometry with application to Fukushima seawater samples. (United States)

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


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

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

    Energy Technology Data Exchange (ETDEWEB)

    Martinelli, R E; Hamilton, T F; Williams, R W; Kehl, S R


    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. Reconstruction of the isotope activity content of heterogeneous nuclear waste drums. (United States)

    Krings, Thomas; Mauerhofer, Eric


    Radioactive waste must be characterized in order to verify its conformance with national regulations for intermediate storage or its disposal. Segmented gamma scanning (SGS) is a most widely applied non-destructive analytical technique for the characterization of radioactive waste drums. The isotope specific activity content is generally calculated assuming a homogeneous matrix and activity distribution for each measured drum segment. However, real radioactive waste drums exhibit non-uniform isotope and density distributions most affecting the reliability and accuracy of activities reconstruction in SGS. The presence of internal shielding structures in the waste drum contributes generally to a strong underestimation of the activity and this in particular for radioactive sources emitting low energy gamma-rays independently of their spatial distribution. In this work we present an improved method to quantify the activity of spatially concentrated gamma-emitting isotopes (point sources or hot spots) in heterogeneous waste drums with internal shielding structures. The isotope activity is reconstructed by numerical simulations and fits of the angular dependent count rate distribution recorded during the drum rotation in SGS using an analytical expression derived from a geometric model. First results of the improved method and enhancements of this method are shown and are compared to each other as well as to the conventional method which assumes a homogeneous matrix and activity distribution. It is shown that the new model improves the accuracy and the reliability of the activity reconstruction in SGS and that the presented algorithm is suitable with respect to the framework requirement of industrial application.

  3. C isotope fractionation during heterotrophic activity driven carbonate precipitation (United States)

    Balci, Nurgul; Demirel, Cansu


    Stable carbon isotopic fractionation during carbonate precipitation induced by environmentally enriched heterotrophic halophilic microorganims was experimentally investigated under various salinity (% 4.5, %8, %15) conditions at 30 °C. Halophilic heterotrophic microorganims were enriched from a hypersaline Lake Acigöl located in SW Turkey (Balci et al.,2015) and later used for the precipitation experiments (solid and liquid medium). The carbonate precipitates had relatively high δ13C values (-4.3 to -16.9 ‰) compared to the δ13C values of the organic compounds that ranged from -27.5 to -25.4 ‰. At salinity of 4.5 % δ13C values of carbonate ranged from -4.9 ‰ to -10.9 ‰ with a 13C-enrichment factor of +20 to +16 ‰ higher than the δ13C values of the associated DOC (-27.5) . At salinity 8 % δ13C values of carbonate ranged from -16.3 ‰ to -11.7 ‰ with a 13C-enrichment factor of+11.3 to+15.9 ‰ higher than the δ13C values of the associated DOC. The respected values for 15 % salinity ranged from -12.3 ‰ to -9.7 ‰ with a 13C-enrichment factor of +15.2 to+16.8 ‰ higher than the δ13C values of the associated DOC. The carbonate precipitates produced in the solid medium are more enriched in 13C relative to liquid culture experiments. These results suggest that the carbon in the solid was derived from both the bacterial oxidation of organic compounds in the medium and from the atmospheric CO2. A solid medium used in the experiments may have suppressed convective and advective mass transport favouring diffusion-controlled system. This determination suggests that the rate and equilibration of CO2 exchange with the atmosphere is the major control on C isotope composition of carbonate minerals precipitated in the experiments. Key words: Lake Acıgöl, halophilic bacteria, carbonate biomineralization, C isotopes References Nurgul Balci, Meryem Menekşe, Nevin Gül Karagüler, M. Şeref Sönmez,Patrick Meister 2015.Reproducing authigenic carbonate

  4. Carbon isotope fractionation of chlorinated ethenes during oxidation by Fe{sup 2+} activated persulfate

    Energy Technology Data Exchange (ETDEWEB)

    Marchesi, Massimo, E-mail: [Departament de Cristallografia, Mineralogia i Diposits Minerals, Universitat de Barcelona, Barcelona, Catalunya 08028 (Spain); Earth and Environmental Department, University of Waterloo, Waterloo, Ontario, Canada N2L 3G1 (Canada); Aravena, Ramon [Earth and Environmental Department, University of Waterloo, Waterloo, Ontario, Canada N2L 3G1 (Canada); Sra, Kanwartej S. [Department of Civil and Environmental Engineering, University of Waterloo, Waterloo, Ontario, Canada N2L 3G1 (Canada); Golder Associates Inc, Toronto, Ontario, Canada L5N 5Z7 (Canada); Thomson, Neil R. [Department of Civil and Environmental Engineering, University of Waterloo, Waterloo, Ontario, Canada N2L 3G1 (Canada); Otero, Neus; Soler, Albert [Departament de Cristallografia, Mineralogia i Diposits Minerals, Universitat de Barcelona, Barcelona, Catalunya 08028 (Spain); Mancini, Silvia [Golder Associates Inc, Toronto, Ontario, Canada L5N 5Z7 (Canada)


    The increased use of persulfate (S{sub 2}O{sub 8}{sup 2-}) for in situ chemical oxidation to treat groundwater and soils contaminated by chlorinated hydrocarbon compounds (CHCs) requires unbiased methods to assess treatment performance. Stable carbon isotope analysis offers a potential tool for assessing the in situ treatment performance of persulfate at sites contaminated with CHCs. This study investigated the extent of C isotope fractionation during oxidation of tetrachloroethene (PCE), trichloroethene (TCE) and cis-dichloroethene (cis-DCE) by persulfate activated by ferrous ion (Fe{sup 2+}). An average carbon isotope enrichment factor {epsilon}{sub bulk} of - 4.9 Per-Mille-Sign for PCE, - 3.6 Per-Mille-Sign for TCE and - 7.6 Per-Mille-Sign for cis-DCE were obtained in batch experiments. Variations in the initial S{sub 2}O{sub 8}{sup 2-}/Fe{sup 2+}/CHC molar ratios did not result in any significant differences in carbon isotope fractionation. The occurrence of carbon isotope fractionation during oxidation and the lack of dependence of enrichment factors upon the S{sub 2}O{sub 8}{sup 2-}/Fe{sup 2+}/CHC molar ratio demonstrate that carbon isotope analysis can potentially be used at contaminated sites as an additional technique to estimate treatment efficacy during oxidation of CHCs by Fe{sup 2+} activated persulfate. Highlights: Black-Right-Pointing-Pointer The performance of in situ chemical oxidation (ISCO) is still difficult to assess. Black-Right-Pointing-Pointer We investigated the potential of carbon isotope analysis as a new assessing tool. Black-Right-Pointing-Pointer C isotope of PCE, TCE and DCE oxidized by persulfate activated by Fe{sup 2+} was measured. Black-Right-Pointing-Pointer Enrichment factors of - 4.9 Per-Mille-Sign for PCE, - 3.6 Per-Mille-Sign for TCE and - 7.6 Per-Mille-Sign for cisDCE were obtained. Black-Right-Pointing-Pointer Carbon isotope can potentially be used to estimate the ISCO treatment efficacy.

  5. Calcium isotopic compositions as tracers of vegetation activity in boreal permafrost ecosystems (Kulingdakan watershed, Central Siberia) (United States)

    Bagard, M.; Schmitt, A.; Chabaux, F. J.; Viers, J.; Pokrovsky, O. S.; Prokushkin, A. S.; Stille, P.; Dupré, B.


    In this work, we propose to investigate the geochemical potential of calcium isotopic fractionations in a forested boreal watershed to trace the impact of vegetation activity. This is the first study carried out in a geographical area characterized by deep and continuous permafrost. For this survey, we measured Ca and Sr isotopic compositions in the different compartments (stream waters, soil solutions, precipitations, rock, soils and soil leachates, vegetation) of a 4,100 ha Siberian watershed, the Kulingdakan watershed (Putorana Plateau, Central Siberia). Our results show that the activity of the vegetation is the only process that fractionates significantly calcium isotopes within the watershed. Indeed, Ca uptake by plants and its subsequent storage in larch tree organs favours 40Ca relatively to 44Ca. Vegetation decomposition releases light δ44/40Ca that affects calcium isotopic compositions of soil solution and soil exchangeable fractions. However, this biological impact is significant only for the South-facing slope of the watershed. Indeed, soil pools from the North-facing slope present no imprint of organic matter degradation in their δ44/40Ca signatures. Furthermore, the major difference between South- and North- facing slopes lies in the importance of the vegetation and its decomposition rate. Thus, we propose that in boreal permafrost areas with limited runoff, the available stock of biomass is critical to induce or not a significant vegetation impact on the calcium isotopic compositions in the soil-water system. As a consequence, the study of preserved calcium isotopic compositions in paleosoil exchangeable phases might bring relevant information on the evolution of biological activity at the watershed scale.

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

    Energy Technology Data Exchange (ETDEWEB)

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


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

  7. Assessment of Non-Traditional Isotopic Ratios by Mass Spectrometry for Analysis of Nuclear Activities (United States)


    Assessment of Non-traditional Isotopic Ratios by Mass Spectrometry for Analysis of Nuclear Activities Distribution Statement A. Approved for pubic...12. DISTRIBUTION / AVAILABILITY STATEMENT 13. SUPPLEMENTARY NOTES 14. ABSTRACT 15. SUBJECT TERMS 16. SECURITY CLASSIFICATION OF...Fahrenheit ( o F) [T( o F) + 459.67]/1.8 kelvin (K) Radiation curie (Ci) [ activity of radionuclides] 3.7 × 10 10 per second (s –1 ) [becquerel (Bq

  8. A non-isotopic assay for histone deacetylase activity. (United States)

    Hoffmann, K; Brosch, G; Loidl, P; Jung, M


    Inhibitors of histone deacetylase (HD) bear great potential as new drugs due to their ability to modulate transcription and to induce apoptosis or differentiation in cancer cells. To study the activity of HD and the effect of potential inhibitors in vitro so far only radio-active assays have existed. For the search of new inhibitors and for the use in HD identification and purification we established a simple, non-radioactive assay that allows screening of large numbers of compounds. The assay is based on an aminocoumarin derivative of an Omega-acetylated lysine as enzyme substrate.

  9. Isotope-Dilution Mass Spectrometry for Quantification of Urinary Active Androgens Separated by Gas Chromatography


    Su Hyeon Lee; Man Ho Choi; Won-Yong Lee; Bong Chul Chung


    Cross reacting antibodies can cause an overestimation of the results of immunoassays. Therefore, alternative methodsare needed for the accurate quantification of steroids. Gas chromatography combined with isotope-dilution mass spectrometry(GC-IDMS) is developed to quantify urinary active androgens, testosterone, epitestosterone and dihydrotestosterone, which areclinically relevant androgens to both hair-loss and prostate diseases. The method devised involves enzymatic hydrolysis with β-glucur...

  10. Isotopic Evidence for Microbial Activity in Crystalline Bedrock Fractures - a Case Study from Olkiluoto, SW Finland (United States)

    Sahlstedt, E. K.; Karhu, J.; Pitkänen, P.


    Changes in the geochemical environment in crystalline bedrock fractures were investigated using the stable isotopes of C, O and S in fracture filling minerals as tracers. Of special interest were the possible changes which may occur in the subsurface at low temperatures. Especially, the influence of microbial activity was recognized as a catalyst for inducing changes in the geochemical environment. The study site is the Olkiluoto island located on the western coast of Finland, planned to host a geological repository for nuclear waste. Fracture surfaces were investigated to recognize the latest mineralizations at the site. These fillings were comprised of thin plates or small euhedral crystals of calcite and pyrite. The carbon and sulfur isotope compositions of calcite and pyrite were measured from bulk material by conventional IRMS, and in situ by secondary ion mass spectrometry. A notable feature of the late-stage fillings was high variabilities in the δ13C values of calcite and the δ34S values of pyrite, which ranged from -53.8 ‰ to +31.6 ‰ and from -50.4 ‰ to +77.7 ‰, respectively. Based on the isotopic compositions of the fillings, several features in the past hydrogeochemical environment could be recognized. The isotopic composition of the fracture fillings indicate an environment which was stratified with respect to depth. Characteristic features include bacterial sulfate reduction (BSR) occurring at depths 50 m. It appears that methanic conditions were replaced by sulfate reduction at depths >50 m likely due to infiltration of SO42--rich brackish waters. Sulfate reducing bacteria used mainly surface derived organic carbon as electron donors. Some indication of minor methanotrophic activity was recognized in anomalously low δ13C values of calcite, down to -53.8 ‰, at the depth range of 34-54 m. This methanotrophic activity may have been related to bacteria using CH4 as an electron donor in BSR.

  11. Isotopic signature of selected lanthanides for nuclear activities profiling using cloud point extraction and ICP-MS/MS. (United States)

    Labrecque, Charles; Lebed, Pablo J; Larivière, Dominic


    The presence of fission products, which include numerous isotopes of lanthanides, can impact the isotopic ratios of these elements in the environment. A cloud point extraction (CPE) method was used as a preconcentration/separation strategy prior to measurement of isotopic ratios of three lanthanides (Nd, Sm, and Eu) by inductively coupled plasma tandem mass spectrometry (ICP-MS/MS). To minimise polyatomic interference, the combination of interferents removal by CPE, reaction/collision cell conditions in He and NH3 mode and tandem quadrupole configuration was investigated and provided optimal results for the determination of isotopic ratio in environmental samples. Isotopic ratios were initially measured in San Joaquin soil (NIST-2709a), an area with little contamination of nuclear origin. Finally, samples collected from three sites with known nuclear activities (Fangataufa Lagoon in French Polynesia, Chernobyl and the Ottawa River near Chalk River Laboratory) were analysed and all exhibited altered isotopic ratios for (143/145)Nd, (147/149)Sm, and (151/153)Eu. These results demonstrate the potential of CPE and ICP-MS/MS for the detection of altered isotopic ratio in environmental samples collected in area subjected to nuclear anthropogenic contamination. The detection of variations in these isotopic ratios of fission products represents the first application of CPE in nuclear forensic investigations of environmental samples.

  12. Artificial radionuclides in a high resolution water column profile from the Catalan Sea (the Northwestern Mediterranean)

    Energy Technology Data Exchange (ETDEWEB)

    Merino, J.; Sanchez-Cabeza, J.A.; Bruach, J.M.; Masque, P.; Pujol, Ll. [Universitat Autonoma de Barcelona, Bellatera (Spain). Grup de Fisica de les Radiacions


    {sup 137}Cs, {sup 239,240}Pu and {sup 90}Sr concentration profiles (0-1200 m) were determined in filtered large volume water samples collected from the Catalan Sea (the Northwestern Mediterranean) in August 1993. Plutonium isotopes were also measured in the suspended matter. {sup 137}Cs concentrations showed a maximum surface activity of 4.45 {+-} 0.38 Bq m{sup -3} and decreased along the water column to a minimum value. The total {sup 137}Cs inventory in the water column was 3.30 {+-} 0.13 kBq m{sup -2}. {sup 90}Sr concentration profile showed a similar behaviour, but levels rose slightly near the bottom. On the other hand, soluble {sup 239,240}Pu concentrations showed a broad subsurface maximum centered at about 400 m depth, where its maximum value was found. This observation is in agreement with that found by others in open ocean waters of the Atlantic and Pacific Oceans, as well as in the Mediterranean Sea. The soluble {sup 239,240}Pu inventory was 17.4 {+-} 0.5 Bq m{sup -2}. In comparison with the inventories reported earlier, the vertical flux of plutonium was determined to be 1.97 {+-} 0.14 Bq m{sup -2} y{sup -1}, roughly 10% of the annual standing inventory. This indicated that {sup 239,240}Pu may be used to trace particulate vertical transport processes in open sea waters. (author) 21 refs.

  13. Investigation of recoil collection method for production of high specific activity nuclear medicine isotopes. (United States)

    Cheng, K Y; Kunze, J F; Ehrhardt, G J


    High specific activity radiopharmaceuticals cannot readily be produced by (n, gamma) reactions in nuclear reactors, because the great abundance of parent atoms remaining have the same chemical characteristics as the produced isotope. We have investigated the effectiveness of using recoil atom collection methods for separating the produced radioisotope. Gold-198, produced from isotopically pure (natural) gold-197, was chosen for these experiments, which were run in the high flux (approximately 10(14) n/cm2 s thermal flux) of the reflector of the University of Missouri Research Reactor. Seven separate experiments were run, with a 2 mm separation between the emitter and the collector. Collection efficiencies were only a few percent of the radioisotope atoms produced in the top atomic layer of the emitter, instead of the 30% range anticipated. Furthermore, the collected radioisotope, instead of being nearly pure, contained a large quantity of the parent. Unless the reason for the "contamination" of product with the parent can be reduced by several orders of magnitude, this "surface hot atom recoil" method appears to offer no practical application for nuclear medicine isotope production.

  14. Multisubstrate isotope labeling and metagenomic analysis of active soil bacterial communities. (United States)

    Verastegui, Y; Cheng, J; Engel, K; Kolczynski, D; Mortimer, S; Lavigne, J; Montalibet, J; Romantsov, T; Hall, M; McConkey, B J; Rose, D R; Tomashek, J J; Scott, B R; Charles, T C; Neufeld, J D


    Soil microbial diversity represents the largest global reservoir of novel microorganisms and enzymes. In this study, we coupled functional metagenomics and DNA stable-isotope probing (DNA-SIP) using multiple plant-derived carbon substrates and diverse soils to characterize active soil bacterial communities and their glycoside hydrolase genes, which have value for industrial applications. We incubated samples from three disparate Canadian soils (tundra, temperate rainforest, and agricultural) with five native carbon ((12)C) or stable-isotope-labeled ((13)C) carbohydrates (glucose, cellobiose, xylose, arabinose, and cellulose). Indicator species analysis revealed high specificity and fidelity for many uncultured and unclassified bacterial taxa in the heavy DNA for all soils and substrates. Among characterized taxa, Actinomycetales (Salinibacterium), Rhizobiales (Devosia), Rhodospirillales (Telmatospirillum), and Caulobacterales (Phenylobacterium and Asticcacaulis) were bacterial indicator species for the heavy substrates and soils tested. Both Actinomycetales and Caulobacterales (Phenylobacterium) were associated with metabolism of cellulose, and Alphaproteobacteria were associated with the metabolism of arabinose; members of the order Rhizobiales were strongly associated with the metabolism of xylose. Annotated metagenomic data suggested diverse glycoside hydrolase gene representation within the pooled heavy DNA. By screening 2,876 cloned fragments derived from the (13)C-labeled DNA isolated from soils incubated with cellulose, we demonstrate the power of combining DNA-SIP, multiple-displacement amplification (MDA), and functional metagenomics by efficiently isolating multiple clones with activity on carboxymethyl cellulose and fluorogenic proxy substrates for carbohydrate-active enzymes. Importance: The ability to identify genes based on function, instead of sequence homology, allows the discovery of genes that would not be identified through sequence alone. This

  15. Radio-ecological researches in the Sea of Japan and northwestern part of the Pacific Ocean after accident on the Japanese nuclear power plant 'Fukushima-1': the content of plutonium isotopes and strontium-90 in sea water

    Energy Technology Data Exchange (ETDEWEB)

    Fedorova, A. [Research and Production Association - RPA Typhoon (Russian Federation)


    In April-May 2011 and in August-September 2012 'Roshydromet' has conducted radio ecological researches in the Sea of Japan and on the water area of northwestern part of the Pacific Ocean (Kuril-Kamchatka area and the area of the Kuroshio current), which had purpose to make assessment of contamination hazard that can be caused to the coast of Russian Far East because of emergency releases of radioactive materials on the nuclear power plant 'Fukushima-1'. During the research works was done the sampling and processing of sea water samples not only for detection of Cs{sup 134}, Cs{sup 137}, but also for such radio-ecological significant long-living radionuclides, as {sup 90}Sr, plutonium isotopes ({sup 239,240}Pu) and tritium. Information about radionuclides was required for correct assessment of nuclear power plant 'Fukushima-1' aftermath on the Far Eastern sea water areas, but was not available in the beginning of research. In the present report the radiochemical measuring results on content of plutonium isotopes and {sup 90}Sr in the sea water from researched areas are presented. Sampling was done from the various horizons. Surface and deep water samples were filtered via the compound filter which made it possible to filter particles bigger than 1 micron. Radiochemical testing of the {sup 90}Sr and plutonium isotopes content was done separately on a suspension and in a filtrate of sea water samples. The content of {sup 90}Sr in the filtrate of the sea water that had been selected in 2011, ranges 0,7-2,4 Bq/m{sup 3}, in suspensions the interval makes 0,0013-0,021 Bq/m3. The results received in researches in 2012 are in range of 0,5-2,6 Bq/m{sup 3} of the sea water filtrate. According to results of IAEA in 2000, the average content of {sup 90}Sr in surface water of the Sea of Japan made 1,6 Bq/m{sup 3}. Hereby, the data obtained in researches in 2011-2012 agrees with results which had been presented by IAEA before the accident. The

  16. Semi-empirical Calculation for Yield of 240Pu Spontaneous Fission

    Institute of Scientific and Technical Information of China (English)

    SHU; Neng-chuan; LIU; Li-le; CHEN; Xiao-song; LIU; Ting-jin; SUN; Zheng-jun; CHEN; Yong-jing; QIAN; Jing


    <正>The spontaneous fission yield has important implication in the nuclear engineering. This work used semi-empirical model to calculate its chain yield, the result shows good agreement with the measured data. There are only 3 sets of measured data, and only too gave the chain yields and cumulative yields, covering 17 chains. It is not enough to satisfy the requirement of users. So it is needed to use theoretical model to calculate the chain yield without measured data.

  17. Artificial (Pu {sup 90}Sr, {sup 241}Am) and natural (U) isotopes in human bones from Poland

    Energy Technology Data Exchange (ETDEWEB)

    Mietelski, J.W.; Tomankiewicz, E. [Institute of Nuclear Phyics (Poland); Golec, E.; Golec, J.; Nowak, S.; Szczygiel, E. [The 5th Military Clinical Hospital and Polyclinic (Poland); Kuzma, K. [General Hospital (Poland)


    In two papers we have presented results if analyses of artificial isotopes ({sup 238,239,240}Pu, {sup 241}Am and {sup 90}Sr) content in human bones, using samples collected during hip joint replacement surgery. Since the patients were members of general population (not exposed in any particular form to artificial radionuclides) results can be treated as current background level for Poland and perhaps also whole central Europe. During this project the open question appeared - what is the level in human bones of natural alpha emitters like {sup 238}U-, {sup 234}U, for instance. Therefore about 30 human hip joint bone samples are being now analysed for the presence of uranium along with mentioned above artificial radionuclides. Samples are ashen and sequential radiochemical analyse is applied for separation of Pu, Sr and Am isotopes followed by separation of uranium using anion exchange resin. Measurements of plutonium, americium and uranium are performed using alpha spectrometry. That for {sup 90}Sr is done by LSC. Results will be presented during conference. Document available in abstract form only. (authors)

  18. Pu isotopes in soils collected downwind from Lop Nor: regional fallout vs. global fallout. (United States)

    Bu, Wenting; Ni, Youyi; Guo, Qiuju; Zheng, Jian; Uchida, Shigeo


    For the first time, soil core samples from the Jiuquan region have been analyzed for Pu isotopes for radioactive source identification and radiological assessment. The Jiuquan region is in downwind from the Lop Nor Chinese nuclear test (CNT) site. The high Pu inventories (13 to 546 Bq/m(2)) in most of the sampling locations revealed that this region was heterogeneously contaminated by the regional fallout Pu from the CNTs. The contributions of the CNTs to the total Pu in soils were estimated to be more than 40% in most cases. The (240)Pu/(239)Pu atom ratios in the soils ranged from 0.059 to 0.186 with an inventory-weighted average of 0.158, slightly lower than that of global fallout. This atom ratio could be considered as a mixed fingerprint of Pu from the CNTs. In addition, Pu in soils of Jiuquan region had a faster downward migration rate compared with other investigated places in China.

  19. LA-ICP-MS for Pu source identification at Mayak PA, the Urals, Russia. (United States)

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


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

  20. DNA-based stable isotope probing enables the identification of active bacterial endophytes in potatoes. (United States)

    Rasche, Frank; Lueders, Tillmann; Schloter, Michael; Schaefer, Sabine; Buegger, Franz; Gattinger, Andreas; Hood-Nowotny, Rebecca C; Sessitsch, Angela


    A (13)CO2 (99 atom-%, 350 ppm) incubation experiment was performed to identify active bacterial endophytes in two cultivars of Solanum tuberosum, cultivars Desirée and Merkur. We showed that after the assimilation and photosynthetic transformation of (13)CO2 into (13)C-labeled metabolites by the plant, the most directly active, cultivar specific heterotrophic endophytic bacteria that consume these labeled metabolite scan be identified by DNA stable isotope probing (DNA-SIP).Density-resolved DNA fractions obtained from SIP were subjected to 16S rRNA gene-based community analysis using terminal restriction fragment length polymorphism analysis and sequencing of generated gene libraries.Community profiling revealed community compositions that were dominated by plant chloroplast and mitochondrial 16S rRNA genes for the 'light' fractions of (13)CO2-incubated potato cultivars and of potato cultivars not incubated with (13)CO2. In the 'heavy' fractions of the (13)CO2-incubated endophyte DNA, a bacterial 492-bp terminal restriction fragment became abundant, which could be clearly identified as Acinetobacter and Acidovorax spp. in cultivars Merkur and Desirée,respectively, indicating cultivar-dependent distinctions in (13)C-label flow. These two species represent two common potato endophytes with known plant-beneficial activities.The approach demonstrated the successful detection of active bacterial endophytes in potato. DNA-SIP therefore offers new opportunities for exploring the complex nature of plant-microbe interactions and plant-dependent microbial metabolisms within the endosphere.

  1. Strontium isotope geochemistry of groundwater affected by human activities in Nandong underground river system, China

    Energy Technology Data Exchange (ETDEWEB)

    Jiang Yongjun, E-mail: [School of Geographical Sciences, Southwest University, Chongqing 400715 (China)] [Institute of Karst Environment and Rock Desertification Rehabilitation, Chongqing 400715 (China)


    Research highlights: {yields} Spatio-temporal variations of Sr concentrations and Sr isotopic composition of groundwater were investigated in a karst underground river system. {yields} Agricultural fertilizers and sewage effluents significantly modified the natural Sr isotopic signature of karst groundwater. {yields} Sr in the carbonate aquifers was relatively non-radiogenic, with low Sr concentrations, while anthropogenic Sr correlated with agricultural fertilizers and sewage effluents was relatively radiogenic, with higher Sr concentrations. {yields} {sup 87}Sr/{sup 86}Sr ratios can provide key information for natural and anthropogenic sources in karst groundwater. - Abstract: The Nandong Underground River System (NURS) is located in a typical karst area dominated by agriculture in SE Yunnan Province, China. Groundwater plays an important role in the social and economical development in the area. The effects of human activities (agriculture and sewage effluents) on the Sr isotope geochemistry were investigated in the NURS. Seventy-two representative groundwater samples, which were collected from different aquifers (calcite and dolomite), under varying land-use types, both in summer and winter, showed significant spatial differences and slight seasonal variations in Sr concentrations and {sup 87}Sr/{sup 86}Sr ratios. Agricultural fertilizers and sewage effluents significantly modified the natural {sup 87}Sr/{sup 86}Sr ratios signature of groundwater that was otherwise dominated by water-rock interaction. Three major sources of Sr could be distinguished by {sup 87}Sr/{sup 86}Sr ratios and Sr concentrations in karst groundwater. Two sources of Sr are the Triassic calcite and dolomite aquifers, where waters have low Sr concentrations (0.1-0.2 mg/L) and low {sup 87}Sr/{sup 86}Sr ratios (0.7075-0.7080 and 0.7080-0.7100, respectively); the third source is anthropogenic Sr from agricultural fertilizers and sewage effluents with waters affected having radiogenic {sup 87

  2. Activation cross-section measurement of a sort of nuclide produced with a target including two isotopes

    Institute of Scientific and Technical Information of China (English)

    ZHOU Feng-Qun; TIAN Ming-Li; SONG Yue-Li; LAN Chang-Lin; KONG Xiang-Zhong


    Based on a formula used to calculate the activation cross-section sum of two reactions producing a sort of nuclide with a target including two isotopes,the related problems in some references have been analyzed and discussed.It is pointed out that the calculation methods of the cross-section sum of two reactions producing the same radioactive nuclide for two isotopes in some references are improper and usually it is impossible to obtain the correct cross-section sum of two reactions producing the same radioactive nuclide for two isotopes in the case of using natural samples.At the same time,the related concepts are clarified and the correct processing method and representation are given.The comparison with the experimental results show that the theoretical analysis results are right.

  3. Coupled study of radionuclides and stable lead isotopes in Western Mediterranean; Etude couplee des radionucleides et des isotopes stables du plomb en Mediterranee occidentale

    Energy Technology Data Exchange (ETDEWEB)

    Miralles, J


    The aim of this work is to identified an environmental deposit able to have stored the atmospheric signal over large time-scale leaning our investigations on lead stable isotopes ({sup 206}Pb, {sup 207}Pb, {sup 208}Pb) and radionuclide ({sup 210}Pb, {sup 137}Cs, {sup 239}Pu, {sup 240}Pu) analysis. Owing to prior studies on anthropogenic lead sources, emission intensity and sedimentary accumulation, we choose to investigate the marine sediments of the Western Mediterranean. In the Gulf of Lions, the sedimentary accumulation is 110 {+-} 7 {mu}{sup -2} high in good agreement with the atmospheric inventory estimate we made from salt marshes of Camargue (99 {mu}{sup -2}). The reconstructed lead accumulation through a modelling step coupling {sup 210}Pb and stable isotopes corroborates the regional anthropogenic emissions (Ferrand, 1996). Briefly, in this context of the marine sediments are a relevant proxy to study past lead atmospheric concentration over the last hundred years. In the Alboran Sea, the study area is less constrained and more complex in terms of climatic, meteorological and hydrological conditions. The sedimentary inventory is of 153 {+-} 47 {mu}{sup -2}, 1,5 higher than in the margin sediments of the Gulf of Lions. The analysis of aerosols, sediments and settling particles evidences a continuity between the atmospheric signal and the sedimentary record. In spite of this encouraging results, the knowledge of the Alboran system is still too restricted in order to unambiguously conclude on accuracy of deep marine sediments of this area to study past atmospheric fallouts. (author)

  4. Chlorine isotopes of thermal springs in arc volcanoes for tracing shallow magmatic activity (United States)

    Li, Long; Bonifacie, Magali; Aubaud, Cyril; Crispi, Olivier; Dessert, Céline; Agrinier, Pierre


    The evaluation of the status of shallow magma body (i.e., from the final intrusion stage, to quiescence, and back to activity), one of the key parameters that trigger and sustain volcanic eruptions, has been challenging in modern volcanology. Among volatile tracers, chlorine (Cl) uniquely exsolves at shallow depths and is highly hydrophilic. Consequently, Cl enrichment in volcanic gases and thermal springs has been proposed as a sign for shallow magmatic activities. However, such enrichment could also result from numerous other processes (e.g., water evaporation, dissolution of old chloride mineral deposits, seawater contamination) that are unrelated to magmatic activity. Here, based on stable isotope compositions of chloride and dissolved inorganic carbon, as well as previous published 3He/4He data obtained in thermal springs from two recently erupted volcanoes (La Soufrière in Guadeloupe and Montagne Pelée in Martinique) in the Lesser Antilles Arc, we show that the magmatic Cl efficiently trapped in thermal springs displays negative δ37Cl values (≤ - 0.65 ‰), consistent with a slab-derived origin but distinct from the isotope compositions of chloride in surface reservoirs (e.g. seawater, local meteoric waters, rivers and cold springs) displaying common δ37Cl values of around 0‰. Using this δ37Cl difference as an index of magmatic Cl, we further examined thermal spring samples including a 30-year archive from two thermal springs in Guadeloupe covering samples from its last eruption in 1976-1977 to 2008 and an island-wide sampling event in Martinique in 2008 to trace the evolution of magmatic Cl in the volcanic hydrothermal systems over time. The results show that magmatic Cl can be rapidly flushed out of the hydrothermal systems within <30 to 80 years after the eruption, much quicker than other volatile tracers such as CO2 and noble gases, which can exsolve at greater depths and constantly migrate to the surface. Because arc volcanoes often have well

  5. Isotope microscopy visualization of the adsorption profile of 2-methylisoborneol and geosmin in powdered activated carbon. (United States)

    Matsui, Yoshihiko; Sakamoto, Asuka; Nakao, Soichi; Taniguchi, Takuma; Matsushita, Taku; Shirasaki, Nobutaka; Sakamoto, Naoya; Yurimoto, Hisayoshi


    Decreasing the particle size of powdered activated carbon may enhance its equilibrium adsorption capacity for small molecules and micropollutants, such as 2-methylisoborneol (MIB) and geosmin, as well as for macromolecules and natural organic matter. Shell adsorption, in which adsorbates do not completely penetrate the adsorbent but instead preferentially adsorb near the outer surface of the adsorbent, may explain this enhancement in equilibrium adsorption capacity. Here, we used isotope microscopy and deuterium-doped MIB and geosmin to directly visualize the solid-phase adsorbate concentration profiles of MIB and geosmin in carbon particles. The deuterium/hydrogen ratio, which we used as an index of the solid-phase concentration of MIB and geosmin, was higher in the shell region than in the inner region of carbon particles. Solid-phase concentrations of MIB and geosmin obtained from the deuterium/hydrogen ratio roughly agreed with those predicted by shell adsorption model analyses of isotherm data. The direct visualization of the localization of micropollutant adsorbates in activated carbon particles provided direct evidence of shell adsorption.

  6. Light Stable Isotopes in Aquifers Affected by Mining Activities in a Brazilian Mining Province (United States)

    Moreira, R. M.; de Carvalho, J. B.


    Iron ore is presently a main item in the Brazilian commercial agenda. Large reserves have converted this utility into an important source of export earnings and, secondarily, of raw materials for the domestic industry. Parallel to a boom in mining activities in the last years environmental impacts and a stress on natural resources have soared. A region exhibiting pronouncedly intensive mining activities lies in the central part of the State of Minas Gerais, the third economy of the federation. Mines are sited right beside the capital and neighbor towns amounting to nearly five million inhabitants and a pronounced dependence on groundwater resources. Besides, this region is a water divide enclosing the sources of main contributors to the most strategic fluvial basins in the country. Iron ore is by large the main mineral but other metals (including gold and uranium), as well as non-metals such as limestone, quartz and granite, also occur. Given the significance of this commodity in the country's trade balance and the demand of water resources with acceptable quality for human consumption, the scale of ensuing water use conflicts caused by its exploration is wide ranging and has to be coped with well grounded environmental assessment approaches. Tracer hydrology techniques might be a valuable tool in this context. The characteristics of the area being impacted have been surveyed, including climate and pluviometry, stratigraphic litology, geological structure, use of soil, mineral resources and their exploration, surface and ground water hydrology and their sundry uses. Data to be processed have been procured at local public agencies but as regard local hydrological features, particularly isotopic compositions, ad hoc surveys and methodologies were required. One instance concerns pluviometric isotopy due to the alpine character of the surveyed region altitude and temperature effects might take place. Hence different sites were monitored; cumulative pluviometer samples

  7. Specific activity and isotope abundances of strontium in purified strontium-82

    Energy Technology Data Exchange (ETDEWEB)

    Fitzsimmons, J. M.; Medvedev, D. G.; Mausner, L. F.


    A linear accelerator was used to irradiate a rubidium chloride target with protons to produce strontium-82 (Sr-82), and the Sr-82 was purified by ion exchange chromatography. The amount of strontium associated with the purified Sr-82 was determined by either: ICP-OES or method B which consisted of a summation of strontium quantified by gamma spectroscopy and ICP-MS. The summation method agreed within 10% to the ICP-OES for the total mass of strontium and the subsequent specific activities were determined to be 0.25–0.52 TBq mg-1. Method B was used to determine the isotope abundances by weight% of the purified Sr-82, and the abundances were: Sr-82 (10–20.7%), Sr-83 (0–0.05%), Sr-84 (35–48.5%), Sr-85 (16–25%), Sr-86 (12.5–23%), Sr-87 (0%), and Sr-88 (0–10%). The purified strontium contained mass amounts of Sr-82, Sr-84, Sr-85, Sr-86, and Sr-88 in abundances not associated with natural abundance, and 90% of the strontium was produced by the proton irradiation. A comparison of ICP-OES and method B for the analysis of Sr-82 indicated analysis by ICP-OES would be easier to determine total mass of strontium and comply with regulatory requirements. An ICP-OES analytical method for Sr-82 analysis was established and validated according to regulatory guidelines.

  8. An Evaluation of Activated Bismuth Isotopes in Environmental Samples From the Former Western Pacific Proving Grounds

    Energy Technology Data Exchange (ETDEWEB)

    Robison, W.L.; Brunk, J.A.; Jokela, T.A.


    {sup 207}Bi (t{sub 1/2}=32.2 y) was generated by activation of weapons material during a few ''clean'' nuclear tests at the U.S. Western Pacific Proving Grounds of Enewetak and Bikini Atolls. The radionuclides first appeared in the Enewetak environment during 1958 and in the environment of Bikini during 1956. Crater sediments from Bikini with high levels of {sup 207}Bi were analyzed by gamma spectrometry in an attempt to determine the relative concentrations of {sup 208}Bi (t{sup 1/2} = 3.68 x 10{sup 5} y). The bismuth isotopes were probably generated during the ''clean'', 9.3 Mt Poplar test held on 7/12/58. The atom ratio of {sup 208}Bi to {sup 207}Bi (R value) ranges from {approx}12 to over 200 in sections of core sediments from the largest nuclear crater at Bikini atoll. The presence of bismuth in the device is suggested to account for R values in excess of 10.

  9. Recent research activities and future subjects on stable- and radio-isotopes of chlorine in environment

    Energy Technology Data Exchange (ETDEWEB)

    Kushita, Kouhei [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment


    This report reviews the recent studies on the stable- and radio-isotopes of chlorine from a viewpoint of environmental science, partly including historic references on this element. First, general properties, occurrence, and utilization of chlorine are described. Secondly, current status and research works on chlorine-compounds, which attract special attention in recent years as environmentally hazardous materials, are reported. Thirdly, research works on stable chlorine isotopes, {sup 35}Cl and {sup 37}Cl, are described with a focus laid on the newly-developed techniques; isotopic ratio mass spectrometry (IRMS) and thermal ionization mass spectrometry (TIMS). Fourthly, recent research works on chlorine radioisotopes, {sup 36}Cl etc., are described, focusing on the development of accelerator mass spectrometry (AMS) and its application to geochemistry and others. Finally, taking account of the above-mentioned recent works on Cl isotopes, possible future research subjects are discussed. (author)

  10. Concentrations and activity ratios of uranium isotopes in groundwater from Doñana National Park, South of Spain (United States)

    Bolívar, J. P.; Olías, M.; González-García, F.; García-Tenorio, R.


    The levels and distribution of natural radionuclides in groundwaters from the unconfined Almonte-Marismas aquifer, upon which Doñana National Park is located, have been analysed. Most sampled points were multiple piezometers trying to study the vertical distribution of the hydrogeochemical characteristics in the aquifer. Temperature, pH, electrical conductivity, dissolved oxygen and redox potential were determined in the field. A large number of parameters, physico-chemical properties, major and minor ions, trace elements and natural radionuclides (U-isotopes, Th-isotopes, Ra-isotopes and 210Po), were also analysed. In the southern zone, where aeolian sands crop out, water composition is of the sodium chloride type, and the lower U-isotopes concentrations have been obtained. As water circulates through the aquifer, bicarbonate and calcium concentrations increase slightly, and higher radionuclides concentrations were measured. Finally, we have demonstrated that 234U/238U activity ratios can be used as markers of the type of groundwater and bedrock, as it has been the case for old waters with marine origin confined by a marsh in the south-east part of aquifer.

  11. Field-Scale Stable-Isotope Probing of Active Methanotrophs in a Landfill-Cover Soil (United States)

    Schroth, M. H.; Henneberger, R.; Chiri, E.


    The greenhouse gas methane (CH4) is an important contributor to global climate change. While its atmospheric concentration is increasing, a large portion of produced CH4 never reaches the atmosphere, but is consumed by aerobic methane-oxidizing bacteria (MOB). The latter are ubiquitous in soils and utilize CH4 as sole source of energy and carbon. Among other methods, MOB may be differentiated based on characteristic phospholipid fatty acids (PLFA). Stable-isotope probing (SIP) on PLFA has been widely applied to identify active members of MOB communities in laboratory incubation studies, but results are often difficult to extrapolate to the field. Thus, novel field-scale approaches are needed to link activity and identity of MOB in their natural environment. We present results of field experiments in which we combined PLFA-SIP with gas push-pull tests (GPPTs) to label active MOB at the field-scale while simultaneously quantifying CH4 oxidation activity. During a SIP-GPPT, a mixture of reactive (here 13CH4, O2) and non-reactive tracer gases (e.g., Ar, Ne, He) is injected into the soil at a location of interest. Thereafter, gas flow is reversed and the gas mixture diluted with soil air is extracted from the same location and sampled periodically. Rate constants for CH4 oxidation can be calculated by analyzing breakthrough curves of 13CH4 and a suitable non-reactive tracer gas. SIP-GPPTs were performed in a landfill-cover soil, and feasibility of this novel approach was tested at several locations along a gradient of MOB activity and soil temperature. Soil samples were collected before and after SIP-GPPTs, total PLFA were extracted, and incorporation of 13C in the polar lipid fraction was analyzed. Potential CH4 oxidation rates derived from SIP-GPPTs were similar to those derived from regular GPPTs (using unlabeled CH4) performed at the same locations prior to SIP-GPPTs, indicating that application of 13CH4 did not adversely affect bacterial CH4 oxidation rates. Rates

  12. Generation of Radixenon Isotopes

    Energy Technology Data Exchange (ETDEWEB)

    McIntyre, Justin I.; Bowyer, Ted W.; Hayes, James C.; Heimbigner, Tom R.; Morris, Scott J.; Panisko, Mark E.; Pitts, W. K.; Pratt, Sharon L.; Reeder, Paul L.; Thomas, Charles W.


    Pacific Northwest National Laboratory has developed an automated system for separating Xe from air and can detect the following radioxenon isotopes, 131mXe, 133mXe, 133Xe, and 135Xe. This report details the techniques used to generate the various radioxenon isotopes that are used for the calibration of the detector as well as other isotopes that have the potential to interfere with the fission produced radioxenon isotopes. Fission production is covered first using highly enriched uranium followed by a description and results from an experiment to produce radioxenon isotopes from neutron activation of ambient xenon.

  13. Activities of \\gamma-ray emitting isotopes in rainwater from Greater Sudbury, Canada following the Fukushima incident

    CERN Document Server

    Cleveland, B T; Lawson, I T; Smith, N J T; Vazquez-Jauregui, E


    We report the activity measured in rainwater samples collected in the Greater Sudbury area of eastern Canada on 3, 16, 20, and 26 April 2011. The samples were gamma-ray counted in a germanium detector and the isotopes 131I and 137Cs, produced by the fission of 235U, and 134Cs, produced by neutron capture on 133Cs, were observed at elevated levels compared to a reference sample of ice-water. These elevated activities are ascribed to the accident at the Fukushima Dai-ichi nuclear reactor complex in Japan that followed the 11 March earthquake and tsunami. The activity levels observed at no time presented health concerns.

  14. Activable enriched stable isotope iron-58 for monitoring absorption rate of juvenile athletes for iron: a case study. (United States)

    Qian, Qinfang; Chai, Zhifang; Feng, Weiyu; Chen, Jidi; Zhang, Peiqun; Pan, Jianxiang


    Activable enriched stable isotopes can play a unique role in studies of nutritional status, metabolism, absorption rates, and bioavailability of minerals. As a practical example, eight juvenile athletes were selected to test the absorption rates of iron during training and non-training periods by enriched stable isotope of Fe-58 (enriched degree: 51.1%) via activation analysis Fe-58 (n, gamma) Fe-59 of the collected feces samples. The results indicated that the average iron absorption rates of the juvenile athletes with and without training are 9.1 +/- 2.8 and 11.9 +/- 4.7%, respectively, which implies that the long-term endurance training with high intensity makes the iron absorption rate of athletes lower. In the meantime, the comparison of the activable enriched isotope technique with atomic absorption spectrometry was performed, which showed that the former was better than the latter in reliability and sensitivity. It is because this nuclear method can distinguish the exogenous and endogenous iron in the samples, but not for non-nuclear methods.

  15. Concurrent determination of 237Np and Pu isotopes using ICP-MS: analysis of NIST environmental matrix standard reference materials 4357, 1646a, and 2702. (United States)

    Matteson, Brent S; Hanson, Susan K; Miller, Jeffrey L; Oldham, Warren J


    An optimized method was developed to analyze environmental soil and sediment samples for (237)Np, (239)Pu, and (240)Pu by ICP-MS using a (242)Pu isotope dilution standard. The high yield, short time frame required for analysis, and the commercial availability of the (242)Pu tracer are significant advantages of the method. Control experiments designed to assess method uncertainty, including variation in inter-element fractionation that occurs during the purification protocol, suggest that the overall precision for measurements of (237)Np is typically on the order of ± 5%. Measurements of the (237)Np concentration in a Peruvian Soil blank (NIST SRM 4355) spiked with a known concentration of (237)Np tracer confirmed the accuracy of the method, agreeing well with the expected value. The method has been used to determine neptunium and plutonium concentrations in several environmental matrix standard reference materials available from NIST: SRM 4357 (Radioactivity Standard), SRM 1646a (Estuarine Sediment) and SRM 2702 (Inorganics in Marine Sediment).

  16. Comparison of Pu and (137)Cs as tracers of soil and sediment transport in a terrestrial environment. (United States)

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


    Following atmospheric nuclear weapons testing in the 1950s and 1960s significant quantities of (137)Cs and (239+240)Pu were deposited worldwide. In recent decades, (137)Cs has been commonly used as a tracer of soil erosion and sedimentation, particularly in the Northern Hemisphere where atomic deposition was three times as great as in the Southern Hemisphere. The relatively short 30-year half-life of this isotope means that its sensitivity as a tracer is rapidly decreasing. In contrast, with half-lives of 24,110 and 6561 years, the sensitivity of the two plutonium isotopes remains essentially the same as when it was deposited. Here we use the technique of Accelerator Mass Spectrometry to demonstrate the potential of anthropogenic Pu as an alternative to (137)Cs as a tracer of soil transport in Australia. We measure an average (137)Cs/(239+240)Pu activity ratio of 27.3+/-1.5 and an average (240)Pu/(239)Pu atom ratio of 0.149+/-0.003, both slightly lower than the global average.

  17. Measurement of radium isotope activities in reservoir and spring water in the Cameroon Central Region

    Directory of Open Access Journals (Sweden)

    Rose Lydie Marie


    Full Text Available Purpose: To determine the activities of 226Ra and 228Ra in the reservoir and spring water samples respectively during the dry and the rainy seasons; and to calculate the annual intake Ii (Bq/y for each type of water samples. Methods: Using both well calibrated Canberra NaI(Tl and HPGe detector systems, it was possible to determine the average specific activity of those radium’s isotopes in water samples which were collected in 2010, from Reservoirs and springs in Cameroon central region including Ngoaekelle, Minboman, Etoudi and Njoungolo. Results: The average specific activity values obtained for 226Ra and 228Ra in reservoir water samples were 8.76 ± 3.50 BqL-1 and 0.64 ± 0.28 BqL-1 during the dry season and, 8.24 ±3.48 BqL-1 and 0.58 ± 0.24 BqL-1 during the rainy season respectively. For spring water, the average values were 3.50 ± 0.63 BqL-1 and below 0.0002 BqL-1 (detection limit of 228Ra in water during the dry season; 3.20 ± 0.60 BqL-1 and below 0.0002 BqL-1 (detection limit of 228Ra in water during the rainy season respectively. Assuming that the volume of drinking water for adult is 2.5 litres per day, the average annual intakes of 226Ra and 228Ra through ingestion in these water samples were 7702 Bq/y and 575 Bq/y for reservoir water; 2993 Bq/y and < 0.25 for spring water respectively. Conclusion: The results have indicated that the annual intake by the population of sampling region as a result of 226Ra in these drinking waters is 7.7 × 103Bq/y more than the maximum limit fixed by ICRP which is 7 × 103 Bq/y. There is a need for regular monitoring the radiological water quality aspect in this region.

  18. The oxygen isotope composition of phosphate released from phytic acid by the activity of wheat and Aspergillus niger phytase (United States)

    von Sperber, C.; Tamburini, F.; Brunner, B.; Bernasconi, S. M.; Frossard, E.


    Phosphorus (P) is an essential nutrient for living organisms. Under P-limiting conditions plants and microorganisms can exude extracellular phosphatases that release inorganic phosphate (Pi) from organic phosphorus compounds (Porg). Phytic acid (myo-inositol hexakisphosphate, IP6) is an important form of Porg in many soils. The enzymatic hydrolysis of IP6 by phytase yields available Pi and less phosphorylated inositol derivates as products. The hydrolysis of organic P compounds by phosphatases leaves an isotopic imprint on the oxygen isotope composition (δ18O) of released Pi, which might be used to trace P in the environment. This study aims at determining the effect of phytase on the oxygen isotope composition of released Pi. For this purpose, enzymatic assays with histidine acid phytases from wheat and Aspergillus niger were prepared using IP6, adenosine 5'-monophosphate (AMP) and glycerophosphate (GPO4) as substrates. For a comparison to the δ18O of Pi released by other extracellular enzymes, enzymatic assays with acid phosphatases from potato and wheat germ with IP6 as a substrate were prepared. During the hydrolysis of IP6 by phytase, four of the six Pi were released, and one oxygen atom from water was incorporated into each Pi. This incorporation of oxygen from water into Pi was subject to an apparent inverse isotopic fractionation (ϵ ~ 6 to 10 ‰), which was similar to that imparted by acid phosphatase from potato during the hydrolysis of IP6 (ϵ ~ 7 ‰), where less than three Pi were released. The incorporation of oxygen from water into Pi during the hydrolysis of AMP and GPO4 by phytase yielded a normal isotopic fractionation (ϵ ~ -12 ‰), similar to values reported for acid phosphatases from potato and wheat germ. We attribute this similarity in ϵ to the same amino acid sequence motif (RHGXRXP) at the active site of these enzymes, which leads to similar reaction mechanisms. We suggest that the striking

  19. The oxygen isotope composition of phosphate released from phytic acid by the activity of wheat and Aspergillus niger phytase

    Directory of Open Access Journals (Sweden)

    C. v. Sperber


    Full Text Available Phosphorus (P is an essential nutrient for living organisms. Under P-limiting conditions plants and microorganisms can exude extracellular phosphatases that release inorganic phosphate (Pi from organic phosphorus compounds (Porg. Phytic acid (IP6 is an important form of Porg in many soils. The enzymatic hydrolysis of IP6 by phytase yields plant available inorganic phosphate (Pi and less phosphorylated inositol derivates as products. The hydrolysis of organic P-compounds by phosphatases leaves an isotopic imprint on the oxygen isotope composition (δ18O of released Pi, which might be used to trace P in the environment. This study aims at determining the effect of phytase on the oxygen isotope composition of released Pi. For this purpose, enzymatic assays with histidine acid phytases from wheat and Aspergillus niger were prepared using IP6, adenosine 5'monophosphate (AMP and glycerophosphate (GPO4 as substrates. For a comparison to the δ18O of Pi released by other extracellular enzymes, enzymatic assays with acid phosphatases from potato and wheat germ with IP6 as substrate were prepared. During the hydrolysis of IP6 by phytase, four Pi are released, and one oxygen atom from water is incorporated into each Pi. This incorporation of oxygen from water into Pi is subject to an apparent inverse isotopic fractionation (ϵ ∼ 6 to 10‰, which is similar to that imparted by acid phosphatase from potato during the hydrolysis of IP6 (ϵ ∼ 7‰ where less than three Pi are released. The incorporation of oxygen from water into Pi during the hydrolysis of AMP and GPO4 by phytase yielded a normal isotopic fractionation (ϵ ∼ −12‰, again similar to values reported for acid phosphatases from potato and wheat germ. We attribute this similarity in ε to the same amino acid sequence motif (RHGXRXP at the active site of these enzymes, which leads to similar reaction mechanisms. We suggest that the striking substrate

  20. Preequilibrium and statistical model calculations for neutron activation cross sections on titanium isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Ivascu, M.; Avrigeanu, M.; Avrigeanu, V.


    Calculated data are presented on (n,p), (n,n'p) and (n,2n) reaction cross sections for stable titanium isotopes in the energy range from threshold up to 20 MeV. An improved preequilibrium approach, allowing a unitary use of preequilibrium and equilibrium emission parameters, has increased the agreement between calculated and experimental cross sections.

  1. Accumulation of atmospheric radionuclides and heavy metals in cryoconite holes on an Arctic glacier. (United States)

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


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

  2. Sr isotopes in the Orgueil CI meteorite: Chronology of early solar system hydrothermal activity

    Indian Academy of Sciences (India)

    J D Macdougall


    New Sr isotopic analyses and calculated formation ages of carbonates from the Orgueil CI meteorite are reported. Among the samples analyzed in this work, dolomites give the youngest formation ages and may have been deposited intermittently starting near the time of parent body formation and continuing for at least 30 Ma. The Sr isotope data also suggest that breunnerites (Fe-Mn-Mg carbonates) crystallized after dolomite formation. Leaching experiments on bulk meteorite samples provide evidence for a very mobile, water soluble Sr reservoir in Orgueil that is characterized by extremely radiogenic Sr (87Sr/86Sr ≈ 0.81- 0.82). This unsupported Sr reflects recent element redistribution, possibly at the time of parent body breakup recorded by the ∼10 Ma exposure age of Orgueil. The carbonate data in particular corroborate earlier indications that hydrothermal processes were among the earliest events to affect the CI parent body.

  3. Influence of orbital forcing and solar activity on water isotopes in precipitation during the mid- and late Holocene

    Directory of Open Access Journals (Sweden)

    S. Dietrich


    Full Text Available In this study we investigate the impact of mid- and late Holocene orbital forcing and solar activity on variations of the oxygen isotopic composition in precipitation. The investigation is motivated by a recently published speleothem δ18O record from the well-monitored Bunker Cave in Germany. The record reveals some high variability on multi-centennial to millennial scales that does not linearly correspond to orbital forcing. Our model study is based on a set of novel climate simulations performed with the atmosphere general circulation model ECHAM5-wiso enhanced by explicit water isotope diagnostics. From the performed model experiments, we derive the following major results: (1 the response of both orbital and solar forcing lead to changes in surface temperatures and δ18O in precipitation with similar magnitudes during the mid- and late Holocene. (2 Past δ18O anomalies correspond to changing temperatures in the orbital driven simulations. This does not hold true if an additional solar forcing is added. (3 Two orbital driven mid-Holocene experiments, simulating the mean climate state approximately 5000 and 6000 yr ago, yield very similar results. However, if an identical additional solar activity-induced forcing is added, the simulated changes of surface temperatures as well as δ18O between both periods differ. We conclude from our simulation results that non-linear effects and feedbacks of the orbital and solar activity forcing substantially alter the δ18O in precipitation pattern and its relation to temperature change.

  4. Tracing of ca 800 yr old mining activity in peat bog using Pb elemental concentrations and isotope compositions. (United States)

    Baron, S.; Carignan, J.; Ploquin, A.


    Sixty sites of slags have been documented on the Mont-Lozère in southern France. The petrographic analysis shows that slags are metallurgical wastes (800 to 850 yr BP) which certainly result from smelting activity for lead and silver extraction (Ploquin et al., 2001). The aims of this study are: 1) to trace the source of Pb ores which supplied the smelting sites, by using the Pb isotopic composition of several surrounding Pb deposits, 2) to evaluate the actual pollution caused by these slags, by using elemental and isotopic compositions of soils, water and vegetation, and 3) to document the pollution history of the region, by using elemental and isotopic compositions of peat bog cores collected in the neighbourhood of the historical smelting sites. The lead isotopic composition of galena collected in most surrounding ores is very similar to that of different slag samples. On the other hand, the high precision of the results allowed us to select the mineralised areas which were probably the ore sources. The Pb isotopic composition of slags is even more homogeneous: 208/206 Pb: 2.092±0.002; 206/207 Pb: 1.179±0.001; 208/204 Pb: 38.663±0.025; 207/204 Pb: 15.665±0.006; 206/204 Pb: 18.476±0.023, and will allow source tracing in the environment. The "Narses Mortes" peat bog, around which two smelting sites have been reported, is strongly minerotrophic and contains 8 to 60% ash. A 1.40 m core have been retrieved and divided into 58 individual samples. Minerotrophic peat bog records both atmospheric deposition, soils leaching and the grounwater influence. The measured metal concentrations are normalised to Al contents of peat bog samples and the metal/Al ratios are compared to that of the Mont-Lozère granite: relative excess in metal concentrations are found in peat bog samples. An increasing excess of most metals (Pb, Zn, Cd...) was measured for surface samples, from 55 cm depth to the top of the core (23 cm depth). This profil might be attributed to atmospheric

  5. Variability in carbon isotope fractionation of trichloroethene during degradation by persulfate activated with zero-valent iron: Effects of inorganic anions

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Yunde [State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Wuhan 430074 (China); School of Environmental Studies, China University of Geosciences, Wuhan 430074 (China); Zhou, Aiguo, E-mail: [State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Wuhan 430074 (China); School of Environmental Studies, China University of Geosciences, Wuhan 430074 (China); Gan, Yiqun; Li, Xiaoqian [State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Wuhan 430074 (China); School of Environmental Studies, China University of Geosciences, Wuhan 430074 (China)


    Stable carbon isotope analysis has the potential to be used for assessing the performance of in situ remediation of organic contaminants. Successful application of this isotope technique requires understanding the magnitude and variability in carbon isotope fractionation associated with the reactions under consideration. This study investigated the influence of inorganic anions (sulfate, bicarbonate, and chloride) on carbon isotope fractionation of trichloroethene (TCE) during its degradation by persulfate activated with zero-valent iron. The results demonstrated that the significant carbon isotope fractionation (enrichment factors ε ranging from − 3.4 ± 0.3 to − 4.3 ± 0.3 ‰) was independent on the zero-iron dosage, sulfate concentration, and bicarbonate concentration. However, the ε values (ranging from − 7.0 ± 0.4 to − 13.6 ± 1.2 ‰) were dependent on the chloride concentration, indicating that chloride could significantly affect carbon isotope fractionation during TCE degradation by persulfate activated with zero-valent iron. The dependence of ε values on chloride concentration, indicated that TCE degradation mechanisms may be different from the degradation mechanism caused by sulfate radical (SO{sub 4}·{sup −}). Ignoring the effect of chloride on ε value may cause numerous uncertainties in quantitative assessment of the performance of the in situ chemical oxidation (ISCO). - Highlights: • Significant C isotope fractionation for TCE degradation by Fe{sup 0} activated persulfate. • The enrichment factors was independent of Fe{sup 0}, SO{sub 4}{sup 2−}, or HCO{sub 3}{sup −} concentration. • Cl{sup −} significantly influenced the carbon isotope fractionation.

  6. Uranium comparison by means of AMS and ICP-MS and Pu and 137Cs results around an Italian Nuclear Power Plant

    Directory of Open Access Journals (Sweden)

    De Cesare M.


    Full Text Available Italy built and commissioned 4 nuclear power plants between 1958-1978, which delivered a total of 1500 MW. All four were closed down after the Chernobyl accident following a referendum in 1987. One of the plants was Garigliano, commissioned in 1959. This plant used a 160 MW BWR1 (SEU of 2.3 % and was operational from 1964 to 1979, when it was switched off for maintenance. It was definitively stopped in 1982, and is presently being decommissioned. We report here details on the chemistry procedure and on the measurements for soil samples, collected up to 4.5 km from the Nuclear Plant. A comparison between uranium (238U concentration as determined by means of AMS (Accelerator Mass Spectrometry and by ICP-MS (Inductively Coupled Plasma-Mass Spectrometry techniques respectively at the ANU (Australian National University and at the Ecowise company in Canberra, Australia, is reported, as well as 236U and 239;240Pu concentration results detected by AMS. 236U/238U and 240Pu/239Pu isotopic ratios by means of AMS are also provided. A contamination from Chernobyl is visible in the 137Cs/239+240Pu activity ratio measurements.

  7. Uranium comparison by means of AMS and ICP-MS and Pu and 137Cs results around an Italian Nuclear Power Plant (United States)

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


    Italy built and commissioned 4 nuclear power plants between 1958-1978, which delivered a total of 1500 MW. All four were closed down after the Chernobyl accident following a referendum in 1987. One of the plants was Garigliano, commissioned in 1959. This plant used a 160 MW BWR1 (SEU of 2.3 %) and was operational from 1964 to 1979, when it was switched off for maintenance. It was definitively stopped in 1982, and is presently being decommissioned. We report here details on the chemistry procedure and on the measurements for soil samples, collected up to 4.5 km from the Nuclear Plant. A comparison between uranium (238U) concentration as determined by means of AMS (Accelerator Mass Spectrometry) and by ICP-MS (Inductively Coupled Plasma-Mass Spectrometry) techniques respectively at the ANU (Australian National University) and at the Ecowise company in Canberra, Australia, is reported, as well as 236U and 239;240Pu concentration results detected by AMS. 236U/238U and 240Pu/239Pu isotopic ratios by means of AMS are also provided. A contamination from Chernobyl is visible in the 137Cs/239+240Pu activity ratio measurements.

  8. Variability in carbon isotope fractionation of trichloroethene during degradation by persulfate activated with zero-valent iron: Effects of inorganic anions. (United States)

    Liu, Yunde; Zhou, Aiguo; Gan, Yiqun; Li, Xiaoqian


    Stable carbon isotope analysis has the potential to be used for assessing the performance of in situ remediation of organic contaminants. Successful application of this isotope technique requires understanding the magnitude and variability in carbon isotope fractionation associated with the reactions under consideration. This study investigated the influence of inorganic anions (sulfate, bicarbonate, and chloride) on carbon isotope fractionation of trichloroethene (TCE) during its degradation by persulfate activated with zero-valent iron. The results demonstrated that the significant carbon isotope fractionation (enrichment factors ε ranging from -3.4±0.3 to -4.3±0.3‰) was independent on the zero-iron dosage, sulfate concentration, and bicarbonate concentration. However, the ε values (ranging from -7.0±0.4 to -13.6±1.2‰) were dependent on the chloride concentration, indicating that chloride could significantly affect carbon isotope fractionation during TCE degradation by persulfate activated with zero-valent iron. The dependence of ε values on chloride concentration, indicated that TCE degradation mechanisms may be different from the degradation mechanism caused by sulfate radical (SO4(-)). Ignoring the effect of chloride on ε value may cause numerous uncertainties in quantitative assessment of the performance of the in situ chemical oxidation (ISCO).

  9. Influence of orbital forcing and solar activity on water isotopes in precipitation during the mid and late Holocene

    Directory of Open Access Journals (Sweden)

    S. Dietrich


    Full Text Available In this study we investigate the impact of mid and late Holocene orbital forcing and solar activity on variations of the oxygen isotopic composition in precipitation. Our study is based on a set of novel climate simulations performed with the atmosphere general circulation model ECHAM5-wiso enhanced by explicit water isotope diagnostics. From the performed model experiments we derive the following major results: (1 the response of both orbital and solar forcing lead to changes in surface temperatures and δ18O in precipitation with similar magnitudes during the mid and late Holocene. (2 Past δ18O anomalies correspond to changing temperatures in the orbital driven simulations. This does not hold true if an additional solar forcing is added. (3 Two orbital driven mid Holocene experiments, simulating the mean climate state approximately 5000 and 6000 yr ago, yield very similar results. However, if an identical additional solar activity-induced forcing is added, the simulated changes of surface temperatures as well as δ18O between both periods differ. From our findings we conclude that the Holocene variability of δ18O in precipitation, as stored in many paleoclimate archives, is rather complex to understand since the combined effect of different external forcings on δ18O in precipitation is non-linear.

  10. A revisit to vityaz transform fault area, Central Indian Ridge: Isotopic evidence of probable hydrothermal activity.

    Digital Repository Service at National Institute of Oceanography (India)

    Shirodkar, P.V.; Banerjee, R.; Xiao, Y.K.

    into the liquid phase during water -rock interactions at high temperatures [1,2]. Boron is one of the major elements of seawater and is significantly involved in the marine biogeochemical cycles. The two stable isotopes of boron, 10B and 11B, with a relative... in the mid-oceanic ridge (MOR) area leads to rifting and crustal generation and creates severe deformities in the oceanic crust, giving rise to hydrothermalism. The basalt-seawater interaction at the ridge sites brings about further changes...

  11. Investigation of Isotopic and Geochemical Evidence for an Active Planktonic Biota in the Precambrian (United States)

    Kump, Lee R.


    The funded research was motivated by the earlier study of Burdett et al. (1990), who collected carbon and oxygen isotopic data from Paleoproterozoic rocks of the Northwest Territories from deep-and shallow-water facies of the Rocknest Platform. Their results displayed a possible decrease in (delta)C-13 with depth when arranged by increasing distance from the paleoshore. The most C-13-depleted samples were seafloor cements and fans from the underlying siliciclastic Odjick Formation, and slope carbonates of the Rocknest platform.

  12. Lead isotopes in soils and groundwaters as tracers of the impact of human activities on the surface environment: The Domizio-Flegreo Littoral (Italy) case study (United States)

    Grezzi, G.; Ayuso, R.A.; de Vivo, B.; Lima, A.; Albanese, S.


    The isotopic signature of geogenic and anthropogenic materials, in combination with concentration data for pollutants, can help trace the origin and the extent of contamination in the environment. This approach is particularly effective if naturally occurring and anthropogenically introduced metals have different isotopic ratios. Lead isotope analysis on soils from 7 profiles (1. m depth) and on groundwaters from 8 wells have been used to determine the impact of human activities on the surface environment of Domizio-Flegreo Littoral. Result obtained show that in sub-rural areas the isotopic composition of the samples collected along the soil profiles of Domizio-Flegreo Littoral is likely mostly controlled by the nature of the parent geologic material (natural) while in more urbanized areas (Giugliano) Pb isotopic composition in superficial soils is mostly influenced by anthropic sources such as motor vehicles. Lead isotopic ratios in groundwaters also show that the use of pesticides and, probably, the influence of aerosols and the presence of illegal waste disposal can influence water quality. ?? 2010 Elsevier B.V.

  13. 242Pu as tracer for simultaneous determination of 237Np and 239,240Pu in environmental samples

    DEFF Research Database (Denmark)

    Chen, Q.J.; Dahlgaard, H.; Nielsen, S.P.;


    A procedure has been developed using Pu-242 as tracer for simultaneous determination of Np-237 and Pu-239,Pu-240 in environmental samples. The validity of the method has been demonstrated by ICPMS and alpha-spectroscopy for up to 10 gram soil and sediment, seawater up to 200 litres. The paper...... describes a suitable chemical procedure for Np and Pu including a quantitative pre-concentration of neptunium and plutonium, preparation of Np4+ and Pu4+, NP(NO3)(6)(2-) and Pu(NO3)(6)(2-), The ratio of Np-237/Pu-242 (or Np-237/Pu-239) before and after the procedure has been determined using 10 g soil (free...... from Np and Pu) R-before/R-after = 1.004 +/- 3.3% (S.D n = 20) and 1 litre seawater R-before/R-after = 1.019+/-1.9% (S.D., n = 12). Results from the intercomparison samples LAEA-135, LAEA-381 and from environmental samples are presented....

  14. Procedures for determination of 239,240Pu, 241Am, 237Np, 234,238U, 2

    DEFF Research Database (Denmark)

    Chen, Q.J.; Aarkrog, Asker; Nielsen, Sven Poul;


    Since 1987, the Department of Nuclear Safety Research, Risø National Laboratory has developed procedures for analysis of low-level amounts of radioactivity in large samples of 200 liters seawater, 10 gram sediment, soil and other environmental materials.These analytical procedures provide high ch...

  15. Intracellular Cadmium Isotope Fractionation (United States)

    Horner, T. J.; Lee, R. B.; Henderson, G. M.; Rickaby, R. E.


    Recent stable isotope studies into the biological utilization of transition metals (e.g. Cu, Fe, Zn, Cd) suggest several stepwise cellular processes can fractionate isotopes in both culture and nature. However, the determination of fractionation factors is often unsatisfactory, as significant variability can exist - even between different organisms with the same cellular functions. Thus, it has not been possible to adequately understand the source and mechanisms of metal isotopic fractionation. In order to address this problem, we investigated the biological fractionation of Cd isotopes within genetically-modified bacteria (E. coli). There is currently only one known biological use or requirement of Cd, a Cd/Zn carbonic anhydrase (CdCA, from the marine diatom T. weissfloggii), which we introduce into the E. coli genome. We have also developed a cleaning procedure that allows for the treating of bacteria so as to study the isotopic composition of different cellular components. We find that whole cells always exhibit a preference for uptake of the lighter isotopes of Cd. Notably, whole cells appear to have a similar Cd isotopic composition regardless of the expression of CdCA within the E. coli. However, isotopic fractionation can occur within the genetically modified E. coli during Cd use, such that Cd bound in CdCA can display a distinct isotopic composition compared to the cell as a whole. Thus, the externally observed fractionation is independent of the internal uses of Cd, with the largest Cd isotope fractionation occurring during cross-membrane transport. A general implication of these experiments is that trace metal isotopic fractionation most likely reflects metal transport into biological cells (either actively or passively), rather than relating to expression of specific physiological function and genetic expression of different metalloenzymes.

  16. Dietary back-calculation using stable isotopes: can activities of enzymes involved in amino acid metabolism be used to improve estimates of trophic shifts in fish? (United States)

    Gaye-Siessegger, Julia; Focken, Ulfert; Abel, Hansjörg; Becker, Klaus


    The aim of this study was (1) to assess the effects of dietary protein content and feeding level on trophic shifts of C and N isotopes (Delta delta(13)C(tissue-diet) and Delta delta(15)N(tissue-diet)) and (2) to test whether the measurement of the activities of two enzymes involved in the metabolism of amino acids could improve the accuracy of estimation of the trophic shifts of C and N isotopes. For this, 36 Nile tilapia (Oreochromis niloticus) were kept under controlled conditions for 8 weeks and fed at three different levels (2, 4 and 8 g kg(-0.8) d(-1)) with three diets differing in their protein content only (20, 29 and 39 %). For each fish, food to fish body trophic shifts of C and N isotopes were measured as well as the hepatic activities of aspartate aminotransferase (ASAT) and glutamate dehydrogenase (GDH). The feeding level affected the activities of ASAT and GDH as well as the trophic shifts of C and N isotopes significantly but the dietary protein content had no significant effect except on the specific activity of ASAT. Fish fed at the lowest level had significantly higher trophic shifts of C and N isotopes than fish fed at higher levels. The trophic shifts were significantly lower in fish with a high protein utilisation. Values of the 'goodness-of-fit' for linear regressions between enzyme activities and trophic shifts were low. Thus, activities of ASAT and GDH are not suitable for predicting estimates of trophic shifts in situations where the amount of food consumed or the dietary protein content is not known. In further studies, activities of enzymes involved in the metabolism of amino acids combined with measurements of the activities of other enzymes should be used to try and improve the accuracy of estimates of trophic shifts.

  17. EROD activity and stable isotopes in seabirds to disentangle marine food web contamination after the Prestige oil spill

    Energy Technology Data Exchange (ETDEWEB)

    Velando, Alberto, E-mail: avelando@uvigo.e [Departamento de Ecoloxia e Bioloxia Animal, Facultade de Ciencias, Universidade de Vigo, Campus As Lagoas, 36310 Vigo (Spain); Munilla, Ignacio [Departamento de Botanica, Facultade de Farmacia, Universidade de Santiago de Compostela, Santiago de Compostela (Spain); Lopez-Alonso, Marta [Departamento de Patoloxia Animal, Facultade de Veterinaria, Universidade de Santiago de Compostela, Lugo (Spain); Freire, Juan [Grupo de Recursos Marinos y Pesquerias Universidade da Coruna, A Coruna (Spain); Perez, Cristobal [Departamento de Ecoloxia e Bioloxia Animal, Facultade de Ciencias, Universidade de Vigo, Campus As Lagoas, 36310 Vigo (Spain)


    In this study, we measured via surgical sampling hepatic EROD activity in yellow-legged gulls from oiled and unoiled colonies, 17 months after the Prestige oil spill. We also analyzed stable isotope composition in feathers of the biopsied gulls, in an attempt to monitor oil incorporation into marine food web. We found that yellow-legged gulls in oiled colonies were being exposed to remnant oil as shown by hepatic EROD activity levels. EROD activity was related to feeding habits of individual gulls with apparent consequences on delayed lethality. Capture-recapture analysis of biopsied gulls suggests that the surgery technique did not affect gull survival, giving support to this technique as a monitoring tool for oil exposure assessment. Our study highlights the combination of different veterinary, toxicological and ecological methodologies as a useful approach for the monitoring of exposure to remnant oil after a large oil spill. - Two years after Prestige oil spill, seabirds were exposed to remnant oil related to their feeding habits with consequences on delayed lethality.

  18. An experimental investigation of multiple sulfur isotope fractionations during heterogenous reactions between SO2 and activated carbon (United States)

    Hamasaki, H.; Watanabe, Y.; Ohmoto, H.


    Watanabe et al. (2009) reported that the reduced-S species produced from reactions between solid organic compounds and aqueous sulfate at 150-200 °C possessed anomalous isotopic fractionation (AIF) of S: Δ33S = 0.1 to 2.1 ‰. Based partly on these data, they suggested that the AIF-S signatures in some sedimentary rocks were produced during thermochemical sulfate reduction by solid organic compounds during the early stage of sediment diagenesis, rather than by atmospheric UV photolysis of volcanic SO2. Theoretical study by Lasaga et al. (2008) also suggested that variable AIF-S signatures could be generated during chemisorption of aqueous (or gaseous) S species on a solid surface (e.g., kerogen) under certain conditions. The main objective of this study was, therefore, to evaluate S isotope effects during different stages of reactions (e.g., adsorption, redox reactions) between a solid organic compound and SO2. We have conducted several series of experiments in a closed pyrex-glass system. About 1.8 gm (0.15 moles) of activated C (0.25-1.0 mm in diameter) was first evacuated at 300 °C for 5 days. Then 2.5 mmoles of pure SO2 gas was introduced in the system to react with activated carbon at 200 or 250 °C. Once the pSO2 became stabilized (typically after ~1 day), an aliquot of the SO2 gas (0.1 to 1.5 mmoles) was withdrawn into a pyrex-glass tube containing 20 % H2O2 solution to collect the SO2 as sulfate. After the pSO2 reached to a new steady value, another aliquot of SO2 was withdrawn from the system; sampling was continued until the amount of SO2 gas in the system decreased to 5 % of the initial value. The collected sulfate was converted to Ag2S for isotope analysis. After a series of experiment at 200 °C and another at 250 °C, the activated carbon was removed from the reaction system, treated sequentially by different chemical solutions to extract different forms of S compounds; the extracted S compounds were analyzed for their contents and isotopic ratios

  19. Quantification of Influenza Neuraminidase Activity by Ultra-High Performance Liquid Chromatography and Isotope Dilution Mass Spectrometry. (United States)

    Solano, Maria I; Woolfitt, Adrian R; Williams, Tracie L; Pierce, Carrie L; Gubareva, Larisa V; Mishin, Vasiliy; Barr, John R


    Mounting evidence suggests that neuraminidase's functionality extends beyond its classical role in influenza virus infection and that antineuraminidase antibodies offer protective immunity. Therefore, a renewed interest in the development of neuraminidase (NA)-specific methods to characterize the glycoprotein and evaluate potential advantages for NA standardization in influenza vaccines has emerged. NA displays sialidase activity by cleaving off the terminal N-acetylneuraminic acid on α-2,3 or α-2,6 sialic acid containing receptors of host cells. The type and distribution of these sialic acid containing receptors is considered to be an important factor in transmission efficiency of influenza viruses between and among host species. Changes in hemagglutinin (HA) binding and NA specificity in reassortant viruses may be related to the emergence of new and potentially dangerous strains of influenza. Current methods to investigate neuraminidase activity use small derivatized sugars that are poor models for natural glycoprotein receptors and do not provide information on the linkage specificity. Here, a novel approach for rapid and accurate quantification of influenza neuraminidase activity is achieved utilizing ultra-high performance liquid chromatography (UPLC) and isotope dilution mass spectrometry (IDMS). Direct LC-MS/MS quantification of NA-released sialic acid provides precise measurement of influenza neuraminidase activity over a range of substrates. The method provides exceptional sensitivity and specificity with a limit of detection of 0.38 μM for sialic acid and the capacity to obtain accurate measurements of specific enzyme activity preference toward α-2,3-sialyllactose linkages, α-2,6-sialyllactose linkages, or whole glycosylated proteins such as fetuin.

  20. Low-Enriched Uranium Fuel Conversion Activities for the High Flux Isotope Reactor, Annual Report for FY 2011

    Energy Technology Data Exchange (ETDEWEB)

    Renfro, David G [ORNL; Cook, David Howard [ORNL; Freels, James D [ORNL; Griffin, Frederick P [ORNL; Ilas, Germina [ORNL; Sease, John D [ORNL; Chandler, David [ORNL


    This report describes progress made during FY11 in ORNL activities to support converting the High Flux Isotope Reactor (HFIR) from high-enriched uranium (HEU) fuel to low-enriched uranium (LEU) fuel. Conversion from HEU to LEU will require a change in fuel form from uranium oxide to a uranium-molybdenum (UMo) alloy. With both radial and axial contouring of the fuel foil and an increase in reactor power to 100 MW, calculations indicate that the HFIR can be operated with LEU fuel with no degradation in performance to users from the current levels achieved with HEU fuel. Studies are continuing to demonstrate that the fuel thermal safety margins can be preserved following conversion. Studies are also continuing to update other aspects of the reactor steady state operation and accident response for the effects of fuel conversion. Technical input has been provided to Oregon State University in support of their hydraulic testing program. The HFIR conversion schedule was revised and provided to the GTRI program. In addition to HFIR conversion activities, technical support was provided directly to the Fuel Fabrication Capability program manager.

  1. Nitrogen isotopic patterns of vegetation as affected by breeding activity of Black-tailed Gull (Larus crassiostris): A coupled analysis of feces, inorganic soil nitrogen and flora

    Energy Technology Data Exchange (ETDEWEB)

    Mizota, C., E-mail: [Iwate University, Ueda 3-18-8, Morioka, Iwate 020-8550 (Japan)


    Two currently breeding colonies (Matsushima Bay and Rishiri island; northern Japan) of predominant Black-tailed Gull (Larus crassiostris) were studied for N isotopic patterns of flora, which is affected by increased supply of inorganic soil N derived from the microbial transformation of feces. Coupled samples of feces, topsoil and flora were collected in early to mid July (2008), when input of fecal N onto soils was at its maximum. As bird migration and breeding continued, native Japanese red-pine (Pinus densiflora), junipers (Juniperus chinensis and Juniperus rigita; Matsushima Bay colony) and Sasa senanensis (Rishiri colony) declined, while ornithocoprophilus exotic plants succeeded. Among tree species on the islands, P. densiflora with ectomycorrizal colonization appears highly susceptible to elevated concentrations of NH{sub 4}-N in the topsoil. A mechanism for best explaining the plant succession associated with the breeding activity of Black-tailed Gull was evidenced by two parameters: first, concomitant elevation of N content in the flora and second, inorganic soil N content, along with changes in N isotopic composition ({delta}{sup 15}N). Earlier isotopic data on the foliar N affected by breeding activity were compiled and reviewed. Emphasis was put on isotopic information for inorganic N in soils that controls plant succession.

  2. Impacts of Human Activities on the Occurrence of Groundwater Nitrate in an Alluvial Plain: A Multiple Isotopic Tracers Approach

    Institute of Scientific and Technical Information of China (English)

    Zhonghe Pang; Lijuan Yuan; Tianming Huang; Yanlong Kong; Jilai Liu; Yiman Li


    Nitrate pollution is a severe problem in areas with intensive agricultural activities.This study focuses on nitrate occurrence and its constraints in a selected alluvial fan using chemical data combined with environmental isotopic tracers (18O,3H,and 15N).Results show that groundwater nitrate in the study area is as high as 258.0 mg/L (hereafter NO3-) with an average of 86.8 mg/L against national drinking water limit of 45 mg/L and a regional baseline value of 14.4 mg/L.Outside of the riparian zone,nitrate occurrence is closely related to groundwater circulation and application of chemical fertilizer.High groundwater nitrate is found in the recharge area,where nitrate enters into groundwater through vertical infiltration,corresponding to high 3H and enriched 18O in the water.In the riparian zone,on the contrary,the fate of groundwater nitrate is strongly affected by groundwater level.Based on two sampling transects perpendicular to the riverbank,we found that the high level of nitrate corresponds to the deeper water table (25 m) near the urban center,where groundwater is heavily extracted.Groundwater nitrate is much lower (<12.4 mg/L) at localities with a shallow water table (5 m),which is likely caused by denitrification in the aquifer.

  3. Heterogeneous Isotopic Anomalies of Sm and Gd in the Norton County Meteorite: Evidence for Irradiation from the Active Early Sun (United States)

    Hidaka, Hiroshi; Kondo, Tomoyo; Yoneda, Shigekazu


    Large and heterogeneous isotopic variations of 150Sm/149Sm and 158Gd/157Gd due to neutron capture reactions caused by cosmic-ray irradiation were found in chemical and mineral separates from the Norton County meteorite. The light-colored separates, consisting mainly of enstatite (Mg2Si2O6), have a very large neutron fluence of 1.98 × 1017 n cm-2, which is 10 times higher than that of the whole rock. Furthermore, four chemical separates showed a large variation in neutron fluences, ranging from 1.82 × 1016 to 1.87 × 1017 n cm-2. The variable amounts of neutron fluences from a small single fragment of the Norton County meteorite cannot be simply explained by single-stage cosmic-ray irradiation in space. Rare earth element (REE) analyses revealed that the fractions with high neutron fluences have similar chemical properties to those in the early condensates in the solar system, showing depletions of Eu and Yb in their REE abundance patterns. The data provide evidence for an activity of the early Sun (T Tauri), suggesting the migration of early and intense irradiation materials into the Norton County meteorite's parent body.

  4. Fractional Absorption of Active Absorbable Algal Calcium (AAACa and Calcium Carbonate Measured by a Dual Stable-Isotope Method

    Directory of Open Access Journals (Sweden)

    Steven A. Abrams


    Full Text Available With the use of stable isotopes, this study aimed to compare the bioavailability of active absorbable algal calcium (AAACa, obtained from oyster shell powder heated to a high temperature, with an additional heated seaweed component (Heated Algal Ingredient, HAI, with that of calcium carbonate. In 10 postmenopausal women volunteers aged 59 to 77 years (mean ± S.D., 67 ± 5.3, the fractional calcium absorption of AAACa and CaCO3 was measured by a dual stable isotope method. 44Ca-enriched CaCO3 and AAACa were administered in all subjects one month apart. After a fixed-menu breakfast and pre-test urine collection (Urine 0, 42Ca-enriched CaCl2 was intravenously injected, followed by oral administration of 44Ca-enriched CaCO3 without carrier 15 minutes later, and complete urine collection for the next 24 hours (Urine 24. The fractional calcium absorption was calculated as the ratio of Augmentation of 44Ca from Urine 0 to Urine 24/ augmentation of 42Ca from Urine 0 to Urine 24. Differences and changes of 44Ca and 42Ca were corrected by comparing each with 43Ca. Fractional absorption of AAACa (mean ± S.D., 23.1 ± 6.4, was distinctly and significantly higher than that of CaCO3 (14.7 ± 6.4; p = 0.0060 by paired t-test. The mean fractional absorption was approximately 1.57-times higher for AAACa than for CaCO3. The serum 25(OH vitamin D level was low (mean ± S.D., 14.2 ± 4.95 ng/ml, as is common in this age group in Japan. Among the parameters of the bone and mineral metabolism measured, none displayed a significant correlation with the fractional absorption of CaCO3 and AAACa. Higher fractional absorption of AAACa compared with CaCO3 supports previous reports on the more beneficial effect of AAACa than CaCO3 for osteoporosis.


    Energy Technology Data Exchange (ETDEWEB)

    Diprete, D; C Diprete, C; Raymond Sigg, R


    NAA using {sup 252}Cf is used to address important areas of applied interest at SRS. Sensitivity needs for many of the applications are not severe; analyses are accomplished using a 21 mg {sup 252}Cf NAA facility. Because NAA allows analysis of bulk samples, it offers strong advantages for samples in difficult-to-digest matrices when its sensitivity is sufficient. Following radiochemical separation with stable carrier addition, chemical yields for a number methods are determined by neutron activation of the stable carrier. In some of the cases where no suitable stable carriers exist, the source has been used to generate radioactive tracers to yield separations.

  6. Carbon isotopic composition (δ(13)C and (14)C activity) of plant samples in the vicinity of the Slovene nuclear power plant. (United States)

    Sturm, Martina; Vreča, Polona; Krajcar Bronić, Ines


    δ(13)C values of various plants (apples, wheat, and maize) collected in the vicinity of the Krško Nuclear Power Plant (Slovenia) during 2008 and 2009 were determined. By measuring dried samples and their carbonized counterparts we showed that no significant isotopic fractionation occurs during the carbonization phase of the sample preparation process in the laboratory. The measured δ(13)C values of the plants were used for δ(13)C correction of their measured (14)C activities.

  7. Long-lived radionuclides in residues from operation and decommissioning of nuclear power plants

    Energy Technology Data Exchange (ETDEWEB)

    Lopez-Gutierrez, J.M., E-mail: [Centro Nacional de Aceleradores (CNA), c/Thomas Alva Edison n Degree-Sign 7, 41092 Sevilla (Spain); University of Sevilla, Departamento de Fisica Aplicada I, c/Virgen de Africa, n Degree-Sign 7, 41011 Sevilla (Spain); Gomez-Guzman, J.M.; Chamizo, E.; Peruchena, J.I. [Centro Nacional de Aceleradores (CNA), c/Thomas Alva Edison n Degree-Sign 7, 41092 Sevilla (Spain); Garcia-Leon, M. [University of Sevilla, Departamento de Fisica Atomica, Molecular y Nuclear, Apdo. 1065, 41080 Sevilla (Spain)


    Radioactive residues, in order to be classified as Low-Level Waste (LLW), need to fulfil certain conditions; the limitation of the maximum activity from long-lived radionuclides is one of these requirements. In order to verify compliance to this limitation, the abundance of these radionuclides in the residue must be determined. However, performing this determination through radiometric methods constitutes a laborious task. In this work, {sup 129}I concentrations, {sup 239+240}Pu activities, and {sup 240}Pu/{sup 239}Pu ratios are determined in low-level radioactive residues, including resins and dry sludge, from nuclear power plants in Spain. The use of Accelerator Mass Spectrometry (AMS) enables high sensitivities to be achieved, and hence these magnitudes can be re determined with good precision. Results present a high dispersion between the {sup 129}I and {sup 239+240}Pu activities found in various aliquots of the same sample, which suggests the existence of a mixture of resins with a variety of histories in the same container. As a conclusion, it is shown that activities and isotopic ratios can provide information on the processes that occur in power plants throughout the history of the residues. Furthermore, wipes from the monitoring of surface contamination of the Jose Cabrera decommissioning process have been analyzed for {sup 129}I determination. The wide range of measured activities indicates an effective dispersal of {sup 129}I throughout the various locations within a nuclear power plant. Not only could these measurements be employed in the contamination monitoring of the decommissioning process, but also in the modelling of the presence of other iodine isotopes.

  8. Enzymatic activities and stable isotope patterns of ectomycorrhizal fungi in relation to phylogeny and exploration types in an afrotropical rain forest. (United States)

    Tedersoo, Leho; Naadel, Triin; Bahram, Mohammad; Pritsch, Karin; Buegger, Franz; Leal, Miguel; Kõljalg, Urmas; Põldmaa, Kadri


    Ectomycorrhizal (ECM) fungi obtain both mineral and simple organic nutrients from soil and transport these to plant roots. Natural abundance of stable isotopes (¹⁵N and ¹³C) in fruit bodies and potential enzymatic activities of ECM root tips provide insights into mineral nutrition of these mutualistic partners. By combining rDNA sequence analysis with enzymatic and stable isotope assays of root tips, we hypothesized that phylogenetic affinities of ECM fungi are more important than ECM exploration type, soil horizon and host plant in explaining the differences in mineral nutrition of trees in an African lowland rainforest. Ectomycorrhizal fungal species belonging to extraradical mycelium-rich morphotypes generally displayed the strongest potential activities of degradation enzymes, except for laccase. The signature of ¹⁵N was determined by the ECM fungal lineage, but not by the exploration type. Potential enzymatic activities of root tips were unrelated to ¹⁵N signature of ECM root tip. The lack of correlation suggests that these methods address different aspects in plant nutrient uptake. Stable isotope analysis of root tips could provide an additional indirect assessment of fungal and plant nutrition that enables enhancement of taxonomic coverage and control for soil depth and internal nitrogen cycling in fungal tissues.

  9. Therapeutic use of radioactive isotopes

    CERN Multimedia

    Caroline Duc


    In December, researchers from ISOLDE-CERN, the Paul Scherrer Institute (PSI) and the Institut Laue-Langevin (ILL) published the results of an in vivo study which successfully proved the effectiveness of four terbium isotopes for diagnosing and treating cancerous tumours.   Four terbium isotopes suitable for clinical purposes. “ISOLDE is the only installation capable of supplying terbium isotopes of such purity and intensity in the case of three out of the four types used in this study,” explains Karl Johnson, a physicist at ISOLDE.  “Producing over a thousand different isotopes, our equipment offers the widest choice of isotopes in the world!” Initially intended for fundamental physics research, ISOLDE has diversified its activities over time to invest in various projects in the materials science, biochemistry and nuclear medicine fields. The proof-of-concept study has confirmed that the four terbium isotopes 149Tb, 152Tb, 155Tb produ...

  10. Leatherback Isotopes (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — SWFSC is currently working on a project identifying global marine isotopes using leatherback turtles (Dermochelys coriacea) as the indicator species. We currently...

  11. Isotopic Paleoclimatology (United States)

    Bowen, R.

    Paleotemperature scales were calculated by H. C. Urey and others in the 1950s to assess past temperatures, and later work using the stable isotopes of oxygen, hydrogen, and carbon employed standards such as Peedee belemnite (PDB) and Standard Mean Ocean Water (SMOW). Subsequently, subjects as diverse as ice volume and paleotemperatures, oceanic ice and sediment cores, Pleistocene/Holocene climatic changes, and isotope chronostratigraphy extending back to the Precambrian were investigated.

  12. Isotopic chirality

    Energy Technology Data Exchange (ETDEWEB)

    Floss, H.G. [Univ. of Washington, Seattle, WA (United States)


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

  13. Sequential Assessment of Cell Cycle S Phase in Flow Cytometry: A Non-Isotopic Method to Measure Lymphocyte Activation In Vitro

    Directory of Open Access Journals (Sweden)

    Ch. Kohler


    Full Text Available Lymphocyte multiplication can be induced in vitro by mitogens or specific antigens, and is usually measured using isotopic methods involving tritiated thymidine. Cellular proliferation can also be analyzed by flow cytometry techniques based on cell cycle analysis through the measurement of DNA content. We applied this method to lymphocytes from 113 individuals, to evaluate lymphocyte proliferation after stimulation in vitro by a mitogen (phytohaemagglutinin, PHA or a recall antigen (tetanus toxoid, using a kinetic approach with four points sequential measurements of the S and G2 phases over six days of culture. The proportion of cells in S phase after PHA stimulation was significantly higher than in controls overall and as early as on day three of the culture. Activation with a recall antigen significantly induced increasing S phase cell proportions up to day six. These data suggest that flow cytometric assessment of the S phase could be a useful alternative to isotopic methods measuring lymphocyte reactivity in vitro.

  14. Pre-Fukushima levels of artificial radionuclides activities in maritime samples from King George Island (South Shetlands, Antarctica)

    Energy Technology Data Exchange (ETDEWEB)

    Sobiech-Matura, K. [European Commision DG-JRC Institute for Reference Materials and Measurements, Retieseweg 111, Geel (Belgium); Institute of Botany, Zdzislaw Czeppe Department of Polar Research and Documentation, Jagiellonian University, Kopernika 27, Krakow (Poland); Mietelski, J.W. [The Henryk Niewodniczanski Institute of Nuclear Physics, Polish Academy of Sciences, W.E. Radzikowskiego 152, Krakow (Poland); Olech, M.A. [Institute of Botany, Zdzislaw Czeppe Department of Polar Research and Documentation, Jagiellonian University, Kopernika 27, Krakow (Poland); Department of Antarctic Biology, Polish Academy of Sciences, Ustrzycka 10/12, Warsaw (Poland)


    Different maritime samples were collected at King George Island during Polish scientific expeditions in years 2005/2006 and 2006/2007. They originated mainly from Admiralty Bay region. Activities of {sup 137}Cs, {sup 238,239+240}Pu, {sup 90}Sr and {sup 241}Am were measured using γ-, β- and α-spectrometry. Our measurements allow estimating the state of radioactive pollution of Antarctic environment directly before the Fukushima accident. Examined samples included different elements of Antarctic marine environment: macro-algae (e.g. Cystosphaera jacquinotii, Ascoseira mirabilis), fishes(e.g. Notothenia coriiceps, Chaenocephalus aceratus), birds (e.g. Pygoscelis adeliae, P. papua), and crustaceans (e.g. Euphausia superba, Waldeckia obesa). Activity concentrations of {sup 137}Cs vary from <0.3 to 21.8 ± 2.1 Bq/kg d.w. In comparison with results obtained for samples of animals and macro-algae previously [1,2] our results are similar or lower. Activity concentrations of {sup 239+240}Pu range from <0.2 to 455 ± 56 mBq/kg d.w. and comparing to previous results [1,2] they were similar or lower. For maritime animals from Terra Nova Bay [3] results are also similar or lower than obtained in present project. Activity concentrations of {sup 238}Pu in samples varied from <0.2 to 79 ± 22 mBq/kg d.w. In comparison to results presented in [1,2,3] our values are similar or higher. Activity concentrations obtained for {sup 90}Sr varied from <1.5 to 73 ± 24 Bq/kg d.w. and are similar or lower then values given in [2,3]. Activity concentrations of {sup 241}Am varied from <9.4 to 29.8 ± 9.3 mBq/kg d.w. and they are similar or higher than values obtained in [3] and similar to that from [1]. Obtained results show that levels of radioactive contamination were very low and in many cases lower than the detection limit. Planned further investigation will allow estimating the environmental condition after the Fukushima accident. (authors)

  15. Capture of heavy hydrogen isotopes in a metal-organic framework with active Cu(I) sites (United States)

    Weinrauch, I.; Savchenko, I.; Denysenko, D.; Souliou, S. M.; Kim, H.-H.; Le Tacon, M.; Daemen, L. L.; Cheng, Y.; Mavrandonakis, A.; Ramirez-Cuesta, A. J.; Volkmer, D.; Schütz, G.; Hirscher, M.; Heine, T.


    The production of pure deuterium and the removal of tritium from nuclear waste are the key challenges in separation of light isotopes. Presently, the technological methods are extremely energy- and cost-intensive. Here we report the capture of heavy hydrogen isotopes from hydrogen gas by selective adsorption at Cu(I) sites in a metal-organic framework. At the strongly binding Cu(I) sites (32 kJ mol-1) nuclear quantum effects result in higher adsorption enthalpies of heavier isotopes. The capture mechanism takes place most efficiently at temperatures above 80 K, when an isotope exchange allows the preferential adsorption of heavy isotopologues from the gas phase. Large difference in adsorption enthalpy of 2.5 kJ mol-1 between D2 and H2 results in D2-over-H2 selectivity of 11 at 100 K, to the best of our knowledge the largest value known to date. Combination of thermal desorption spectroscopy, Raman measurements, inelastic neutron scattering and first principles calculations for H2/D2 mixtures allows the prediction of selectivities for tritium-containing isotopologues.

  16. Standard test method for nondestructive assay of nuclear material in scrap and waste by passive-Active neutron counting using 252Cf shuffler

    CERN Document Server

    American Society for Testing and Materials. Philadelphia


    1.1 This test method covers the nondestructive assay of scrap and waste items for U, Pu, or both, using a 252Cf shuffler. Shuffler measurements have been applied to a variety of matrix materials in containers of up to several 100 L. Corrections are made for the effects of matrix material. Applications of this test method include measurements for safeguards, accountability, TRU, and U waste segregation, disposal, and process control purposes (1, 2, 3). 1.1.1 This test method uses passive neutron coincidence counting (4) to measure the 240Pu-effective mass. It has been used to assay items with total Pu contents between 0.03 g and 1000 g. It could be used to measure other spontaneously fissioning isotopes such as Cm and Cf. It specifically describes the approach used with shift register electronics; however, it can be adapted to other electronics. 1.1.2 This test method uses neutron irradiation with a moveable Cf source and counting of the delayed neutrons from the induced fissions to measure the 235U equiva...

  17. Radiosynthesis of [{sup 18}F]fluorophenyl-L-amino acids by isotopic exchange on carbonyl-activated precursors

    Energy Technology Data Exchange (ETDEWEB)

    Castillo Melean, Johnny


    Aromatic [{sup 18}F]fluoroamino acids have earlier been developed as promising probes for diagnostics using PET. However, a wider use of these radiofluorinated compounds has been limited due to radiosynthetic constraints. The work here presents an amenable three-step radiosynthesis pathway for the preparation of 2-[{sup 18}F]fluoro-L-phenylalanine (2-[{sup 18}F]Fphe), 2-[{sup 18}F]fluoro-L-tyrosine (2-[{sup 18}F]Ftyr), 6-[{sup 18}F]fuoro-L-m-tyrosine (6-[{sup 18}F]Fmtyr) and 6-[{sup 18}F]fluoro-L-DOPA (6-[{sup 18}F]FDOPA). For this, corresponding precursors were {sup 18}F-fluorinated by nucleophilic isotopic exchange, followed by either removal of an activating formyl group with Rh(PPh{sub 3}){sub 3}Cl or its conversion by Baeyer-Villiger oxidation, respectively, and subsequent hydrolysis of protecting groups in acidic medium. Two efficient synthetic approaches were developed for the preparation of highly functionalized fluoro-benzaldehydes and -ketones which were used as labeling precursors. The compounds (2S,5S)-tert-butyl 2-tert-butyl-5-(2-fluoro-5-formylbenzyl)-3-methyl-4-oxoimidazolidine-1 -carboxylate (1a), (2S,5S)-tert-butyl 5-(5-acetyl-2-fluorobenzyl)-2-tert-butyl-3-methyl-4-oxoimidazolidine-1 -carboxylate (1c), (2S,5S)-benzyl 2-tert-butyl-5-(2-fluoro-5-formylbenzyl)-3-methyl-4-oxoimidazolidine-1 -carbo-xylate (1d), 4-fluoro-3-(((2S,5R)-5-isopropyl-3,6-dimethoxy-2,5-dihydropyrazin-2-yl) me-thyl)b enzal-dehyde (1e) and 1-(4-fluoro-3-(((2S,5R)-5-isopropyl-3,6-dimethoxy-2,5-dihydropyrazin-2-yl) me-thy l)phenyl)ethanone (1f), could be prepared in six steps and overall yields of 41%, 48%, 37%, 27%, and 32%, respectively. (2S,5S)-tert-Butyl 5-(4-(benzyloxy)-2-fluoro-5-formylbenzyl)-2-tert-butyl-3-methyl-4 -oxoimidazolidi ne-1-carboxylate (1b) was prepared in ten steps with an overall yield of 19% while compounds (2S,5S)-tert-butyl 5-(5-(3,5-bis(trifluoromethyl)-benzoyl)-2-fluorobenzyl)-2-tert-butyl-3 -methyl-4-oxoimidazolidine-1-carboxylate (1g) and (2S,5S

  18. The feasibility of using Pu discharges from Sellafield to investigate the sediment dynamics of the Severn Estuary and the Welsh coast

    Energy Technology Data Exchange (ETDEWEB)

    Dunne, J.A.; Richards, D.A. [School of Geographical Sciences and Bristol Isotope Group, University of Bristol (United Kingdom)


    Decades of nuclear weapons testing and very low level radioactive waste discharges from civil nuclear sites have resulted in a global distribution of Pu isotopes. Given that the sources of these isotopes are spatially and temporally well-known, their distribution throughout the environment can provide insight into the processes that have governed their dispersal. Plutonium-239 and {sup 240}Pu have long half-lives and their atomic abundance ratio is indicative of the source, be it atmospheric fallout or releases from the nuclear industry. Plutonium is also strongly adsorbed on sediments. These characteristics make Pu an excellent tool for monitoring ocean currents, tracking sediment transport and examining the fate of the products of nuclear activities. We intend to exploit the discharges of Pu from Sellafield nuclear reprocessing plant to investigate transit times and sediment regime in inter-tidal sediments from proximal (Ravenglass Estuary, Cumbria) and distal (Portishead, North Somerset) sites. Continuing developments in analytical techniques (extraction chromatography and ion exchange) and inductively coupled plasma mass spectrometry (ICP-MS) permit isotopic analysis at low abundances (on the order of femto-grams), with reasonable efficiency and cost in comparison to traditional radiometric techniques. A major advantage of this technique is the ability to distinguish between {sup 239}Pu and {sup 240}Pu, which is not possible with alpha-spectrometry due to similar alpha energies. We present initial results using MC-ICP-MS, following methods in Lindahl et al. (2011). Document available in abstract form only. (authors)

  19. Higher peroxidase activity, leaf nutrient contents and carbon isotope composition changes in Arabidopsis thaliana are related to rutin stress. (United States)

    Hussain, M Iftikhar; Reigosa, Manuel J


    Rutin, a plant secondary metabolite that is used in cosmetics and food additive and has known medicinal properties, protects plants from UV-B radiation and diseases. Rutin has been suggested to have potential in weed management, but its mode of action at physiological level is unknown. Here, we report the biochemical, physiological and oxidative response of Arabidopsis thaliana to rutin at micromolar concentrations. It was found that fresh weight; leaf mineral contents (nitrogen, sodium, potassium, copper and aluminum) were decreased following 1 week exposure to rutin. Arabidopsis roots generate significant amounts of reactive oxygen species after rutin treatment, consequently increasing membrane lipid peroxidation, decreasing leaf Ca(2+), Mg(2+), Zn(2+), Fe(2+) contents and losing root viability. Carbon isotope composition in A. thaliana leaves was less negative after rutin application than the control. Carbon isotope discrimination values were decreased following rutin treatment, with the highest reduction compared to the control at 750μM rutin. Rutin also inhibited the ratio of CO2 from leaf to air (ci/ca) at all concentrations. Total protein contents in A. thaliana leaves were decreased following rutin treatment. It was concluded carbon isotope discrimination coincided with protein degradation, increase lipid peroxidation and a decrease in ci/ca values may be the primary action site of rutin. The present results suggest that rutin possesses allelopathic potential and could be used as a candidate to develop environment friendly natural herbicide.

  20. RNA-Based Stable Isotope Probing Suggests Allobaculum spp. as Particularly Active Glucose Assimilators in a Complex Murine Microbiota Cultured In Vitro (United States)

    Herrmann, Elena; Young, Wayne; Rosendale, Douglas; Reichert-Grimm, Verena; Conrad, Ralf


    RNA-based stable isotope probing (RNA-SIP) and metabolic profiling were used to detect actively glucose-consuming bacteria in a complex microbial community obtained from a murine model system. A faeces-derived microbiota was incubated under anaerobic conditions for 0, 2, and 4 h with 40 mM [U13C]glucose. Isopycnic density gradient ultracentrifugation and fractionation of isolated RNA into labeled and unlabeled fractions followed by 16S rRNA sequencing showed a quick adaptation of the bacterial community in response to the added sugar, which was dominated by unclassified Lachnospiraceae species. Inspection of distinct fractions of isotope-labeled RNA revealed Allobaculum spp. as particularly active glucose utilizers in the system, as the corresponding RNA showed significantly higher proportions among the labeled RNA. With time, the labeled sugar was used by a wider spectrum of faecal bacteria. Metabolic profiling indicated rapid fermentation of [U13C]glucose, with lactate, acetate, and propionate being the principal 13C-labeled fermentation products, and suggested that “cross-feeding” occurred in the system. RNA-SIP combined with metabolic profiling of 13C-labeled products allowed insights into the microbial assimilation of a general model substrate, demonstrating the appropriateness of this technology to study assimilation processes of nutritionally more relevant substrates, for example, prebiotic carbohydrates, in the gut microbiota of mice as a model system. PMID:28299315

  1. Identification of metabolically active methanogens in anaerobic digester by DNA Stable-Isotope Probing using 13C-acetate

    Directory of Open Access Journals (Sweden)

    V. Gowdaman


    Full Text Available Anaerobic digestion is gaining enormous attention due to the ability to covert organic wastes into biogas, an alternative sustainable energy. Methanogenic community plays a significant role in biogas production and also for proficient functioning of the anaerobic digester. Therefore, this study was carried out to investigate the methanogen diversity of a food waste anaerobic digester. After endogenous respiration, the digester samples were supplemented with isotopes of acetate to enrich methanogen population, and were analyzed using DNA-SIP (Stable-Isotope Probing. Following separation and fractionation of heavy (13C and light (12C DNA, PCR amplification was carried out using archaeal 16S rRNA gene followed by DGGE analysis. Sequencing of the prominent DGGE bands revealed the dominance of Methanocorpusculum labreanum species belonging to hydrogenotrophic Methanomicrobiales, which can produce methane in the presence of H2/CO2 and requires acetate for its growth. This is the first instance where Methanocorpusculum labreanum is being reported as a dominant species in an anaerobic digester operative on food waste.

  2. Formation of Kokumi-Enhancing γ-Glutamyl Dipeptides in Parmesan Cheese by Means of γ-Glutamyltransferase Activity and Stable Isotope Double-Labeling Studies. (United States)

    Hillmann, Hedda; Behr, Jürgen; Ehrmann, Matthias A; Vogel, Rudi F; Hofmann, Thomas


    Recently, γ-glutamyl dipeptides (γ-GPs) were found to be responsible for the attractive kokumi flavor of Parmesan cheese (PC). Quantitation of γ-GPs and their parent amino acids in 13-, 24-, and 30-month ripened PC samples by LC-MS/MS and stable isotope dilution analysis (SIDA), in-cheese (13)C-labeling studies, followed by analysis of the γ-glutamyl transferase (GGT) activity revealed γ-GPs to be generated most efficiently after 24 months of ripening by a GGT-catalyzed transfer of the γ-glutamyl moiety of L-glutamine onto various acceptor amino acids released upon casein proteolysis. Following the identification of milk as a potential GGT source in PC, the functionality of the milk's GGT to generate the target γ-GPs was validated by stable isotope double-labeling (SIDL) experiments. Therefore, raw and heat-treated milk samples were incubated with L-glutamine-[U-(13)C] and acceptor amino acids (X) and the hetero- (γ-Glu-[(13)C5]-X) and homotranspeptidation products (γ-Glu-Gln-[(13)C10]) were quantitated by LC-MS/MS-SIDA using γ-Glu-Ala-[(13)C3] as the internal standard. High GGT activity to generate the γ-GPs and preference for L-phenylalanine and L-methionine as acceptor amino acids were found in raw milk and milk samples heat-treated for 10 min up to a maximum of 65 °C. In comparison, GGT activity and SIDL studies performed with inoculated Lactobacillus strains, including Lactobacillus harbinensis and Lactobacillus casei identified in PC by means of 16S rRNA gene sequencing, did not show any significant GGT activity and unequivocally demonstrated unpasteurized cow's milk, rather than microorganisms, as a key factor in γ-glutamyl dipeptide generation in Parmesan cheese.

  3. Plutonium measurements by accelerator mass spectrometry at LLNL

    Energy Technology Data Exchange (ETDEWEB)

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


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

  4. Quantitation using a stable isotope dilution assay (SIDA) and thresholds of taste-active pyroglutamyl decapeptide ethyl esters (PGDPEs) in sake. (United States)

    Hashizume, Katsumi; Ito, Toshiko; Igarashi, Shinya


    A stable isotope dilution assay (SIDA) for two taste-active pyroglutamyl decapeptide ethyl esters (PGDPE1; (pGlu)LFGPNVNPWCOOC2H5, PGDPE2; (pGlu)LFNPSTNPWCOOC2H5) in sake was developed using deuterated isotopes and high-resolution mass spectrometry. Recognition thresholds of PGDPEs in sake were estimated as 3.8 μg/L for PGDPE1 and 8.1 μg/L for PGDPE2, evaluated using 11 student panelists aged in their twenties. Quantitated concentrations in 18 commercial sake samples ranged from 0 to 27 μg/L for PGDPE1 and from 0 to 202 μg/L for PGDPE2. The maximum levels of PGDPE1 and PGDPE2 in the sake samples were approximately 8 and 25 times higher than the estimated recognition thresholds, respectively. The results indicated that PGDPEs may play significant sensory roles in the sake. The level of PGDPEs in unpasteurized sake samples decreased during storage for 50 days at 6 °C, suggesting PGDPEs may be enzymatically decomposed.

  5. Fluid flow and water-rock interaction across the active Nankai Trough subduction zone forearc revealed by boron isotope geochemistry (United States)

    Hüpers, Andre; Kasemann, Simone A.; Kopf, Achim J.; Meixner, Anette; Toki, Tomohiro; Shinjo, Ryuichi; Wheat, C. Geoffrey; You, Chen-Feng


    Compositional changes, dehydration reactions and fluid flow in subducted sediments influence seismogenesis and arc magmatism in subduction zones. To identify fluid flow and water-rock interaction processes in the western Nankai Trough subduction zone (SW Japan) we analyzed boron concentration and boron isotope composition (δ11B) of pore fluids sampled across the subduction zone forearc from depths of up to ∼922 m below seafloor during four Integrated Ocean Drilling Program (IODP) Expeditions. The major structural regimes that were sampled by coring include: (1) sedimentary inputs, (2) the frontal thrust zone, (3) the megasplay fault zone, and (4) the forearc basin. From mass balance consideration we find that consumption of boron (B) by ash alteration and desorption of B from the solid phase, mediated by organic matter degradation, produces a net decrease in B concentrations with depth down to ∼120 μM and variable δ11B values in the range of ∼+20‰ and +49‰. Interstitial water in sediments on the incoming oceanic plate are influenced by more efficient mobilization of exchangeable B from the solid phase due to higher temperatures and alteration of the oceanic crust that acts as a sink for 10B. At the tip of the megasplay fault zone, elevated B concentration and B isotopic composition suggest that underthrust coarse-grained slope sediments provide a pathway for fluids out of the upper (balance considerations suggest a shallower fluid source depth compared to pore fluids sampled previously near the décollement zone along the central portion of the Nankai margin.

  6. Plutonium emission from the Fukushima accident

    Energy Technology Data Exchange (ETDEWEB)

    Bossew, P., E-mail: [German Federal Office for Radiation Protection, Berlin (Germany)


    A strong earthquake and subsequent tsunami on 11{sup th} March 2011 initiated a severe accident in units 1 to 4 of Fukushima Dai-ichi nuclear power plant, resulting in substantial releases of radionuclides. While much has since been published 00 environmental contamination and exposure to radio--iodine and radio-caesium, little is known about releases of plutonium and other non-volatile elements. Although the total activities of released {sup 131}I, {sup 134}Cs and {sup 137}Cs are of the same order of magnitude as of the Chernobyl accident in 1986, the contribution of little volatile elements, including Pu, is much smaller in Fukushima fallout. The reason is the different physical nature of the accident sequence which led to a release of some 10{sup -}5% of the core inventories only (to be compared with 3.5% from Chernobyl). In this contribution the available data on Pu in Fukushima fallout will be reviewed. Data sources are mainly reports and press releases by Japanese authorities and a few scientific articles. The mean ratio {sup 239+240}Pu: {sup 137}Cs in the near field around the NPP (mainly part of Fukushima prefecture and districts of adjacent prefectures) can be assumed about 3 x 10{sup -}7{sup ,} to be compared to nearly 0.01 in the vicinity of Chernobyl, down to about 3 x 10 {sup -6} in Central Europe. Isotopic ratios {sup 238}Pu: {sup 239+240} Pu are about 2.2 (0.46 and 0.035 in Chemobyl and global fallout, respectively). Activity concentrations of Fukushima- {sup 239+240} Pu in surface soil were found up to above 0.1 Bq/kg d.m. in the immediate vicinity of the Fukushima NPP and about one order of magnitude less in Fukushima city, about 60 km away. The {sup 239+240} Pu activity released into the atmosphere is roughly estimated some 10{sup 9} Bq (Chemobyl : almost 10{sup 14} Bq). (author)

  7. Identifying Low pH Active and Lactate-Utilizing Taxa within Oral Microbiome Communities from Healthy Children Using Stable Isotope Probing Techniques

    Energy Technology Data Exchange (ETDEWEB)

    McLean, Jeffrey S.; Fansler, Sarah J.; Majors, Paul D.; Mcateer, Kathleen; Allen, Lisa Z.; Shirtliff, Mark E.; Lux, Renate; Shi, Wenyuan


    Many human microbial infectious diseases including dental caries are polymicrobial in nature and how these complex multi-species communities evolve from a healthy to a diseased state is not well understood. Although many health- or disease-associated oral microbes have been characterized in vitro, their physiology in vivo in the presence of the complex oral microbiome is difficult to determine with current approaches. In addition, about half of these oral species remain uncultivated to date and little is known except their 16S rRNA sequence. Lacking culture-based physiological analyses, the functional roles of uncultivated microorganisms will remain enigmatic despite their apparent disease correlation. To start addressing these knowledge gaps, we applied a novel combination of in vivo Magnetic Resonance Spectroscopy (MRS) with RNA and DNA based Stable Isotope Probing (SIP) to oral plaque communities from healthy children for temporal monitoring of carbohydrate utilization, organic acid production and identification of metabolically active and inactive bacterial species.

  8. Stable isotope utilization methodology; Methodologie de l`emploi des isotopes stables

    Energy Technology Data Exchange (ETDEWEB)

    Roth, E. [Conservatoire National des Arts et Metiers (CNAM), 75 - Paris (France)


    The various applications of stable isotope utilization are reviewed, as a function of their specific properties: poly-isotopic abundance modification is used for tracer applications; the accurate measurement of the stable isotope abundance may be applied to isotopic dilution for ultra-trace measurement, physical constant determination, fluid volume and concentration measurement; isotopic effects, such as reaction equilibrium differences are used for separation and identification of molecule active centers (pharmacology, paleoclimatology, hydrogeological studies) while reaction rate differences (competitive and non competitive methods) are used for the study of reaction mechanisms, such as enzymatic reactions. Analysis techniques (mass spectrometry, nuclear magnetic resonance, optical methods) are reviewed. 2 figs., 18 refs.

  9. Studies on the Precise Measurement of Isotope of Trace Plutonium in Uranium by MC-ICP-MS%多接收电感耦合等离子体质谱法精确测量铀中痕量钚同位素方法研究

    Institute of Scientific and Technical Information of China (English)

    李力力; 李金英; 赵永刚; 常志远; 张继龙; 王同兴


    The infinitesimal plutonium impurity was contained in the uranium product obtained by reprocessing. The precise measurement of the isotope ratio of plutonium was beneficial to the identification of the corresponding source of uranium product. Basing on the separation of trace plutonium from uranium matrix, the operating parameters of MC-ICP-MS were studied and optimized for determining the isotope ratio of trace plutonium, such as the adjustment of resolution, selection of mode of ion extraction, elimination of background and interference, etc. The correction method of the mass discrimination was explored for MCICP-MS measuring isotope ratio. The isotope ratio of ~(239)pu/~(240)Pu in two selected uranium products obtained by reprocessing, which was measured and corrected by measuring plutonium reference material. The ratio of uranium and plutonium is more than 10~(10), and the sum of relative uncertainty for plutonium measurement is better than 5%. The measuring method of isotope ratiois establishes for ng · L~(-1) level of plutonium.%经过核燃料后处理得到的铀产品中含有极微量钚杂质,对其同位素组成进行分析有利于对应铀材料的溯源.本工作在铀钚化学分离的基础上,对影响MC-ICP-MS法精确测量痕量钚同位素丰度比值的仪器条件进行了优化,研究了仪器分辨率、离子提取模式的选择、"背景和干扰"等参数的影响,探索研究了MC-ICP-MS上质量偏倚的校正方法.对选择的两个后处理铀产品中痕量钚同位素比进行了测量,当铀钚比例达10~(10)时,测得的~(239)Pu/~(240)Pu相对不确定度优于5%.并且建立了在MC-ICP-MS上测量ng·L~(-1)量级钚同位素丰度比值的方法.

  10. Isotopic signatures associated with growth and metabolic activities of chemosynthetic nitrate-reducing microbes from deep-sea hydrothermal vents (United States)

    Perez-Rodriguez, I. M.; Foustoukos, D.; Fogel, M. L.; Sievert, S. M.


    Epsilonproteobacteria and Aquificaceae have been identified as dominant members of microbial communities at deep-sea hydrothermal vents. Cultured representatives from these two groups appear to be mostly genetically wired to perform chemosynthesis at moderate-to-high temperatures (45 - 80oC) under anaerobic and sulfidic conditions. In this study we used Caminibacter mediatlanticus and Thermovibrio ammonificans as model organisms to constrain physiological parameters associated with dissimilatory nitrate reduction to ammonium (DNRA) in deep-sea vent Epsilonproteobacteria and Aquificaceae. We postulate that nitrate-based metabolic processes are of relevance for understanding primary production as well as nitrate mobilization in deep-sea vents. By constraining growth and respiration rates during DNRA, we observed that C. mediatlanticus achieved higher cell densities than T. ammonificans while exhibiting similar growth rates. DNRA kinetic rate constants and cell-specific nitrate reduction rates (csNRR) obtained from our data showed that within similar time frames T. ammonificans used 2.5 to 3 times as much nitrate than C. mediatlanticus and it did so ~3 times faster. However, the increased consumption of nitrate in T. ammonificans did not translate into higher growth yield. This is suggestive of either differential efficiencies in energy generating pathways or differential organic matter production (cell biomass versus extracellular organic material) associated with DNRA in these microorganisms. Nitrogen isotope fractionation for nitrate was similar for both organisms, with discrimination factors of ~ -5 to -6‰ for C. mediatlanticus and ~ -7 to -8‰ for T. ammonificans. Similar experiments performed under high hydrostatic pressure conditions (50 and 200 bar) showed that changes in pressure greatly affected both growth rates and DNRA kinetic rate constants in both microorganisms, however, δ15N discrimination factors for nitrate were not affected. This study provides

  11. Long-range tropospheric transport of uranium and plutonium weapons fallout from Semipalatinsk nuclear test site to Norway. (United States)

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


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

  12. Magnetostratigraphic dating of an intensification of glacial activity in the southern Italian Alps during Marine Isotope Stage 22 (United States)

    Muttoni, Giovanni; Ravazzi, Cesare; Breda, Marzia; Pini, Roberta; Laj, Carlo; Kissel, Catherine; Mazaud, Alain; Garzanti, Eduardo


    We applied magnetostratigraphy and mammal biostratigraphy to date climate-sensitive pollen cycles and lithostratigraphic units of the Pliocene-Pleistocene Leffe sedimentary succession from the Southern Alps, Italy. The Leffe section was correlated to additional sections (Casnigo, Fornaci di Ranica, and Pianengo) to construct a stratigraphic network along a common fluviatile system (the Serio River) sourced in the Southern Alps and flowing southward into the Po River Basin. We obtained a coherent scenario of climate variability for the last ˜ 2 Myr. At Leffe, lacustrine deposition commenced during the Olduvai Normal Subchron (1.94-1.78 Ma) and lasted up to a chronologic level compatible with Marine Isotope Stage (MIS) 22 (0.87 Ma). Pollen analysis revealed that climate varied cyclically from warm-temperate to cool during this time interval, but never as cold as during glacial intervals. At around MIS 22, climate cooled globally. Gravels, attributed to high-energy braided river systems fed locally by alluvial fans, prograded from the Serio River catchment area over the Leffe Basin and toward the Po Plain in response to a generalized event of vegetation withdrawal and enhanced physical erosion. At this time, Alpine valley glaciers reached their first maximum southward expansion with glacier fronts located at only ˜ 5 km upstream from Leffe.

  13. Isotopic effects on the phonon modes in boron carbide. (United States)

    Werheit, H; Kuhlmann, U; Rotter, H W; Shalamberidze, S O


    The effect of isotopes ((10)B-(11)B; (12)C-(13)C) on the infrared- and Raman-active phonons of boron carbide has been investigated. For B isotopes, the contributions of the virtual crystal approximation, polarization vector and isotopical disorder are separated. Boron and carbon isotope effects are largely opposite to one another and indicate the share of the particular atoms in the atomic assemblies vibrating in specific phonon modes. Some infrared-active phonons behave as expected for monatomic boron crystals.

  14. Stable isotope studies

    Energy Technology Data Exchange (ETDEWEB)

    Ishida, T.


    The research has been in four general areas: (1) correlation of isotope effects with molecular forces and molecular structures, (2) correlation of zero-point energy and its isotope effects with molecular structure and molecular forces, (3) vapor pressure isotope effects, and (4) fractionation of stable isotopes. 73 refs, 38 figs, 29 tabs.

  15. Possible influence of climate factors on the reconstruction of the cosmogenic isotope 14C production rate in the earth's atmosphere and solar activity in past epochs (United States)

    Kuleshova, A. I.; Dergachev, V. A.; Kudryavtsev, I. V.; Nagovitsyn, Yu. A.; Ogurtsov, M. G.


    The paper considers the probable influence of variations of the global temperature and carbon dioxide concentration in the Earth's atmosphere on the results of reconstruction of the production rate of the cosmogenic isotope 14C in the terrestrial atmosphere for the period from the early 15th to the mid 19th century. This time interval covers the Spörer, Maunder, and Dalton minima of solar activity, as well as the Little Ice Age. It was shown that the climate changes that occurred during the Little Ice Age should be taken into account. In the Maunder and Spörer minima of solar activity, the 14C generation rate may be comparable to the values for the Dalton minimum, while exclusion of the climate effect yields extremely large values of the 14C production rate for these grand minima. In the solar activity reconstruction for past epochs, this circumstance should be taken into consideration via measurements of the 14C concentration on a long time scale.

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

    Malekifarsani, A; Skachek, M A


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

  17. The D-D Neutron Generator as an Alternative to Am(Li) Isotopic Neutron Source in the Active Well Coincidence Counter

    Energy Technology Data Exchange (ETDEWEB)

    McElroy, Robert Dennis [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Cleveland, Steven L. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)


    The 235U mass assay of bulk uranium items, such as oxide canisters, fuel pellets, and fuel assemblies, is not achievable by traditional gamma-ray assay techniques due to the limited penetration of the item by the characteristic 235U gamma rays. Instead, fast neutron interrogation methods such as active neutron coincidence counting must be used. For international safeguards applications, the most commonly used active neutron systems, the Active Well Coincidence Counter (AWCC), Uranium Neutron Collar (UNCL) and 252Cf Shuffler, rely on fast neutron interrogation using an isotopic neutron source [i.e., 252Cf or Am(Li)] to achieve better measurement accuracies than are possible using gamma-ray techniques for high-mass, high-density items. However, the Am(Li) sources required for the AWCC and UNCL systems are no longer manufactured, and newly produced systems rely on limited supplies of sources salvaged from disused instruments. The 252Cf shuffler systems rely on the use of high-output 252Cf sources, which while still available have become extremely costly for use in routine operations and require replacement every five to seven years. Lack of a suitable alternative neutron interrogation source would leave a potentially significant gap in the safeguarding of uranium processing facilities. In this work, we made use of Oak Ridge National Laboratory’s (ORNL’s) Large Volume Active Well Coincidence Counter (LV-AWCC) and a commercially available deuterium-deuterium (D-D) neutron generator to examine the potential of the D-D neutron generator as an alternative to the isotopic sources. We present the performance of the LV-AWCC with D-D generator for the assay of 235U based on the results of Monte Carlo N-Particle (MCNP) simulations and measurements of depleted uranium (DU), low enriched uranium (LEU), and highly enriched uranium (HEU) items.

  18. Nickel isotopes and methanogens (United States)

    Neubeck, A.; Ivarsson, M.


    Methanogens require Ni for their growth and as a consequence the microbial fractionation of Ni isotopes can be used as a biomarker for activity of methanogenic communities1. Anaerobic laboratory experiments was performed using methanogens to investigate methanogenic growth in a modified nutrient media2 with olivine Fo91 (5g/l) added as an additional mineral nutrient source and as the only H2 provider. One of the investigated methanogens showed an increased growth in the experiments with added olivine. There were also a close relationship between the mobilized Ni and the growth of the methanogen. Ni is an element that previously has been neglected in the study of fossilized microorganisms and their interaction with mineral substrates and, thus, there are no records or published data of Ni in association with microfossils. However, we have detected enrichments of Ni in fossilized microorganisms and ichno-fossils, respectively, from three separate locations. Ni is not present in the host rock in any of the samples. Thus, Ni is present in association with fossilized microorganisms from environments and more extensive analysis is required to understand the magnitude, uptake, preservation and fractionation of Ni in microfossils. In order to analyze Ni isotope fractionation from microbe-mineral interaction, we plan to use a high-resolution Laser-Ablation Time-of-Flight Mass Spectrometer (LMS)3. In situ profile ablation will provide detailed and localized data on fractionation patterns between microfossils and their host rock. Also, this technique will allow us to identify the change in Ni isotopic fractionation in rock samples caused by abiotic and biogenic processes in a faster and easier way and with less risk for contamination compared to the wet chemistry analyses of Ni isotopes. 1. Cameron, V., Vance, D., Archer, C. & House, C. H. A biomarker based on the stable isotopes of nickel. Proceedings of the National Academy of Sciences 106, 10944-10948 (2009). 2. Schn

  19. Measurement of O(6)-alkylguanine-DNA alkyltransferase activity in tumour cells using stable isotope dilution HPLC-ESI-MS/MS. (United States)

    Sun, Guohui; Zhao, Lijiao; Fan, Tengjiao; Ren, Ting; Zhong, Rugang


    The repair of DNA mediated by O(6)-alkylguanine-DNA alkyltransferase (AGT) provides protection against DNA damage from endogenous or exogenous alkylation of the O(6) position of guanine. However, this repair acts as a double-edged sword in cancer treatment, as it not only protects normal cells from chemotherapy-associated toxicities, but also results in cancer cell resistance to guanine O(6)-alkylating antitumour agents. Thus, AGT plays an important role in predicting the individual susceptibility to guanine O(6)-alkylating carcinogens and chemotherapies. Accordingly, it is necessary to establish a quantitative method for determining AGT activity with high accuracy, sensitivity and practicality. Here, we describe a novel nonradioactive method for measuring AGT activity using stable isotope dilution high-performance liquid chromatography electrospray ionization tandem mass spectrometry (HPLC-ESI-MS/MS). This method is based on the irreversibility of the removal of the O(6)-alkyl group from guanine by AGT and on the high affinity of O(6)-benzylguanine (O(6)-BG) as an AGT substrate. HPLC-ESI-MS/MS was used to measure the AGT activities in cell protein extracts from eight tumour lines, demonstrating that AGT activity was quite variable among different cell lines, ranging from nondetectable to 1021 fmol/mg protein. The experiments performed in intact tumour cells yielded similar results but exhibited slightly higher activities than those observed in cell protein extracts. The accuracy of this method was confirmed by an examination of AGT expression levels using western blotting analysis. To our knowledge, this method is the first mass spectrometry-based AGT activity assay, and will likely provide assistance in the screening of cancer risk or the application of chemotherapies.


    Energy Technology Data Exchange (ETDEWEB)

    Caldwell, E.; Duff, M.; Ferguson, C.


    The nuclear fuel cycle generates a considerable amount of radioactive waste, which often includes nuclear fission products, such as strontium-90 ({sup 90}Sr) and cesium-137 ({sup 137}Cs), and actinides such as uranium (U) and plutonium (Pu). When released into the environment, large quantities of these radionuclides can present considerable problems to man and biota due to their radioactive nature and, in some cases as with the actinides, their chemical toxicity. Radionuclides are expected to decay at a known rate. Yet, research has shown the rate of elimination from an ecosystem to differ from the decay rate due to physical, chemical and biological processes that remove the contaminant or reduce its biological availability. Knowledge regarding the rate by which a contaminant is eliminated from an ecosystem (ecological half-life) is important for evaluating the duration and potential severity of risk. To better understand a contaminants impact on an environment, consideration should be given to plants. As primary producers, they represent an important mode of contamination transfer from sediments and soils into the food chain. Contaminants that are chemically and/or physically sequestered in a media are less likely to be bio-available to plants and therefore an ecosystem.

  1. Medida de isótopos de Plutonio, 239Pu y 240Pu, mediante espectrometría de masas con aceleradores de baja energía


    Chamizo Calvo, Elena


    El primer bloque, sobre la descripción de la técnica y de los dos sistemas empleados, comprende los Capítulos 2, 3 y 4. En el Capítulo 2 presentaremos los fundamento s del AMS de baja energía y las características de diseño de sus instalaciones. De esta forma, veremos que un sistema compacto de AMS no es simplemente una versión a escala de uno convencional, y justificaremos las razones por las que la comunidad científica se ha visto obligada durante 20 años a usar grandes aceleradores. En el ...

  2. Chlorine isotope and Cl-Br fractionation in fluids of Poás volcano (Costa Rica): Insight into an active volcanic-hydrothermal system (United States)

    Rodríguez, Alejandro; Eggenkamp, H. G. M.; Martínez-Cruz, María; van Bergen, Manfred J.


    Halogen-rich volcanic fluids issued at the surface carry information on properties and processes operating in shallow hydrothermal systems. This paper reports a long-term record of Cl-Br concentrations and δ37Cl signatures of lake water and fumaroles from the active crater of Poás volcano (Costa Rica), where surface expressions of magmatic-hydrothermal activity have shown substantial periodic changes over the last decades. Both the hyperacid water of its crater lake (Laguna Caliente) and subaerial fumaroles show significant temporal variability in Cl-Br concentrations, Br/Cl ratios and δ37Cl, reflecting variations in the mode and magnitude of volatile transfer. The δ37Cl signatures of the lake, covering the period 1985-2012, show fluctuations between + 0.02 ± 0.06‰ and + 1.15 ± 0.09‰. Condensate samples from adjacent fumaroles on the southern shore, collected during the interval (2010-2012) with strong changes in gas temperature (107-763°C), display a much larger range from - 0.43 ± 0.09‰ to + 14.09 ± 0.08‰. Most of the variations in Cl isotope, Br/Cl and concentration signals can be attributed to interaction between magma-derived gas and liquid water in the volcanic-hydrothermal system below the crater. The δ37Cl were lowest and closest to magmatic values in (1) fumarolic gas that experienced little or no interaction with subsurface water and followed a relatively dry pathway, and (2) water that captured the bulk of magmatic halogen output so that no phase separation could induce fractionation. In contrast, elevated δ37Cl can be explained by partial scavenging and fractionation during subsurface gas-liquid interaction. Hence, strong Cl isotope fractionation leading to very high δ37Cl in Poás' fumaroles indicates that they followed a wet pathway. Highest δ37Cl values in the lake water were found mostly in periods when it received a significant input from subaqueous fumaroles or when high temperatures and low pH caused HCl evaporation. It is

  3. The use of environmental monitoring as a technique to identify isotopic enrichment activities; O uso da monitoracao ambiental como tecnica de identificacao de atividades de enriquecimento isotopico

    Energy Technology Data Exchange (ETDEWEB)

    Buchmann, Jose Henrique


    The use of environmental monitoring as a technique to identify activities related to the nuclear fuel cycle has been proposed, by international organizations, as an additional measure to the safeguards agreements in force. The elements specific for each kind of nuclear activity, or nuclear signatures, inserted in the ecosystem by several transfer paths, can be intercepted with better or worse ability by different live organisms. Depending on the kind of signature of interest, the anthropogenic material identification and quantification require the choice of adequate biologic indicators and, mainly, the use of sophisticated techniques associated with elaborate sample treatments. This work demonstrates the technical viability of using pine needles as bioindicators of nuclear signatures associated with uranium enrichment activities. Additionally, it proposes the use of a technique widely diffused nowadays in the scientific community, the High Resolution Inductively Coupled Plasma Mass Spectrometer (HR-ICP-MS), to identify the signature corresponding to that kind of activities in the ecosystem. It can be also found a description of a methodology recently being applied in analytical chemistry,based on uncertainties estimates metrological concepts, used to calculate the uncertainties associated with the obtained measurement results. Nitric acid solutions with a concentration of 0.3{sup -1}, used to wash pine needles sampled near facilities that manipulate enriched uranium and containing only 0.1 {mu}{sup -1} of uranium, exhibit a {sup 235} U: {sup 238} U isotopic abundance ratio of 0.0092{+-}0.0002, while solutions originated from samples collected at places located more than 200 km far from activities related to the nuclear fuel cycle exhibit a value of 0.0074{+-}0.0002 for this abundance ratio. Similar results were obtained for samples collected in different places permit to confirm the presence of anthropogenic uranium and demonstrate the viability of using

  4. Utilization of radioanalytical methods for the determination of isotopes of U, Pu and Am in activated charcoal from IEA-R1 reactor

    Energy Technology Data Exchange (ETDEWEB)

    Geraldo, Bianca; Marumo, Julio T., E-mail:, E-mail: [Instituto de Pesquisas Energeticas e Nucleares (IPEN/CNEN-SP), Sao Paulo, SP (Brazil); Taddei, Maria Helena T., E-mail: [Laboratorio de Pocos de Caldas (LAPOC/CNEN-MG), Pocos de Caldas, MG (Brazil)


    Activated charcoal is a radioactive waste arising from the water purification system of the nuclear research reactor. The management of this waste includes its characterization in order to identify and quantify the existing radionuclides, including those known as 'difficult-to-measure radionuclides' (RDM). The analysis of these RDM usually involves complex radiochemical costly and time consuming procedures for the purification and separation of them. The objective of this work was to define a methodology of sequential analysis of isotopes of U, Pu and Am, present in activated charcoal, evaluating chemical recovery, analysis time, quantity of radioactive waste generated and cost. Ion exchange and the chromatographic extraction methodologies were compared. Both methods showed high chemical recoveries, ranged from 74 and 100% for U, 76 and 100% for Pu and 87 and 100% for Am, demonstrating that these methods provide accurate and reliable results. However, chromatographic extraction method is more suitable for the determination of the radionuclides because it generates the smaller volume of waste and is more cost-effectively. (author)

  5. Vertical distribution and migration of global fallout Pu in forest soils in southwestern China. (United States)

    Bu, Wenting; Zheng, Jian; Guo, Qiuju; Uchida, Shigeo


    Soil samples collected in southwestern China were analyzed for Pu isotopes. The (240)Pu/(239)Pu atom ratios were around 0.18, which indicated the dominant source of global fallout. Consistent sub-surface maximums followed by exponential decline of (239+240)Pu activities in the soil cores were observed. Most of the Pu has still remained in the 0-10 cm layers since its deposition. Convection velocities and dispersion coefficients for Pu migration in the soils were estimated by the convection-dispersion equation (CDE) model. The effective convection velocities and effective dispersion coefficients ranged from 0.05 to 0.11 cm/y and from 0.06 to 0.29 cm(2)/y, respectively. Other factors that control the vertical migration of Pu in soil besides precipitation, soil particle size distribution and organic matter were suggested. Long-term migration behaviors of Pu in the soils were simulated. The results provide the Pu background baseline for further environmental monitoring and source identification of non-global fallout Pu inputs in the future.

  6. A novel methodology to investigate isotopic biosignatures (United States)

    Horner, T. J.; Lee, R. B. Y.; Henderson, G. M.; Rickaby, R. E. M.


    . coli (e.g. membranes, cytosol, etc.), including the catalytic metal atoms within CdCA. These experiments allow isotopic exchange reactions to be observed in biological systems at an unparalleled resolution, demonstrating that isotopic fractionation can occur, in vivo, on length scales as small as a few Å. We will explore future applications of this technique using the marine geochemistry of Cd as a case study. This experimental approach has great promise for studying the individual isotopic biosignatures of other biochemical reactions, in particular those which may have been active during early Earth History.

  7. Copper isotope fractionation by desert shrubs

    Energy Technology Data Exchange (ETDEWEB)

    Navarrete, Jesica U., E-mail: [University of Texas at El Paso, Department of Geological Sciences, 500 W. University Ave, El Paso, TX 79968 (United States); Viveros, Marian; Ellzey, Joanne T. [University of Texas at El Paso, Department of Biological Sciences, El Paso, TX 79968 (United States); Borrok, David M. [University of Texas at El Paso, Department of Geological Sciences, 500 W. University Ave, El Paso, TX 79968 (United States)


    Copper has two naturally occurring stable isotopes of masses 63 and 65 which can undergo mass dependent fractionation during various biotic and abiotic chemical reactions. These interactions and their resulting Cu isotope fractionations can be used to determine the mechanisms involved in the cycling of Cu in natural systems. In this study, Cu isotope changes were investigated at the organismal level in the metal-accumulating desert plant, Prosopis pubescens. Initial results suggest that the lighter Cu isotope was preferentially incorporated into the leaves of the plant, which may suggest that Cu was actively transported via intracellular proteins. The roots and stems show a smaller degree of Cu isotope fractionation and the direction and magnitude of the fractionations was dependent upon the levels of Cu exposure. Based on this and previous work with bacteria and yeast, a trend is emerging that suggests the lighter Cu isotope is preferentially incorporated into biological components, while the heavier Cu isotope tends to become enriched in aqueous solutions. In bacteria, plants and animals, intracellular Cu concentrations are strictly regulated via dozens of enzymes that can bind, transport, and store Cu. Many of these enzymes reduce Cu(II) to Cu(I). These initial results seem to fit into a broader picture of Cu isotope cycling in natural systems where oxidation/reduction reactions are fundamental in controlling the distributions of Cu isotopes.

  8. Quantification of ricin, RCA and comparison of enzymatic activity in 18 Ricinus communis cultivars by isotope dilution mass spectrometry. (United States)

    Schieltz, David M; McWilliams, Lisa G; Kuklenyik, Zsuzsanna; Prezioso, Samantha M; Carter, Andrew J; Williamson, Yulanda M; McGrath, Sara C; Morse, Stephen A; Barr, John R


    The seeds of the Ricinus communis (Castor bean) plant are the source of the economically important commodity castor oil. Castor seeds also contain the proteins ricin and R. communis agglutinin (RCA), two toxic lectins that are hazardous to human health. Radial immunodiffusion (RID) and the enzyme linked immunosorbent assay (ELISA) are two antibody-based methods commonly used to quantify ricin and RCA; however, antibodies currently used in these methods cannot distinguish between ricin and RCA due to the high sequence homology of the respective proteins. In this study, a technique combining antibody-based affinity capture with liquid chromatography and multiple reaction monitoring (MRM) mass spectrometry (MS) was used to quantify the amounts of ricin and RCA independently in extracts prepared from the seeds of eighteen representative cultivars of R. communis which were propagated under identical conditions. Additionally, liquid chromatography and MRM-MS was used to determine rRNA N-glycosidase activity for each cultivar and the overall activity in these cultivars was compared to a purified ricin standard. Of the cultivars studied, the average ricin content was 9.3 mg/g seed, the average RCA content was 9.9 mg/g seed, and the enzymatic activity agreed with the activity of a purified ricin reference within 35% relative activity.

  9. Mechanism of Flavoprotein l-6-Hydroxynicotine Oxidase: pH and Solvent Isotope Effects and Identification of Key Active Site Residues. (United States)

    Fitzpatrick, Paul F; Chadegani, Fatemeh; Zhang, Shengnan; Dougherty, Vi


    The flavoenzyme l-6-hydroxynicotine oxidase is a member of the monoamine oxidase family that catalyzes the oxidation of (S)-6-hydroxynicotine to 6-hydroxypseudooxynicotine during microbial catabolism of nicotine. While the enzyme has long been understood to catalyze oxidation of the carbon-carbon bond, it has recently been shown to catalyze oxidation of a carbon-nitrogen bond [Fitzpatrick, P. F., et al. (2016) Biochemistry 55, 697-703]. The effects of pH and mutagenesis of active site residues have now been utilized to study the mechanism and roles of active site residues. Asn166 and Tyr311 bind the substrate, while Lys287 forms a water-mediated hydrogen bond with flavin N5. The N166A and Y311F mutations result in ∼30- and ∼4-fold decreases in kcat/Km and kred for (S)-6-hydroxynicotine, respectively, with larger effects on the kcat/Km value for (S)-6-hydroxynornicotine. The K287M mutation results in ∼10-fold decreases in these parameters and a 6000-fold decrease in the kcat/Km value for oxygen. The shapes of the pH profiles are not altered by the N166A and Y311F mutations. There is no solvent isotope effect on the kcat/Km value for amines. The results are consistent with a model in which both the charged and neutral forms of the amine can bind, with the former rapidly losing a proton to a hydrogen bond network of water and amino acids in the active site prior to the transfer of hydride to the flavin.

  10. Photonuclear reactions on titanium isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Belyshev, S. S. [Moscow State University (Russian Federation); Dzhilavyan, L. Z. [Russian Academy of Sciences, Institute for Nuclear Research (Russian Federation); Ishkhanov, B. S.; Kapitonov, I. M. [Moscow State University (Russian Federation); Kuznetsov, A. A., E-mail:; Orlin, V. N.; Stopani, K. A. [Moscow State University, Skobeltsyn Institute of Nuclear Physics (Russian Federation)


    The photodisintegration of titanium isotopes in the giant-dipole-resonance energy region is studied by the photon-activation method. Bremsstrahlung photons whose spectrum has the endpoint energy of 55 MeV is used. The yields and integrated cross sections are determined for photoproton reactions on the titanium isotopes {sup 47,48,49,50}Ti. The respective experimental results are compared with their counterparts calculated on the basis of the TALYS code and a combined photonucleon-reaction model. The TALYS code disregards the isospin structure of the giant dipole resonance and is therefore unable to describe the yield of photoproton reactions on the heavy titanium isotopes {sup 49,50}Ti.

  11. Noble gas isotopic ratios from historical lavas and fumaroles at Mount Vesuvius (southern Italy): constraints for current and future volcanic activity (United States)

    Tedesco, Dario; Nagao, Keisuke; Scarsi, Paolo


    Helium, neon and argon isotope ratios have been analysed from phenocrysts of eleven lava samples belonging to the last eruptive cycle of Mount Vesuvius (1631 until 1944). The phenocrysts separates include pyroxene ( N=10) and olivine ( N=1). All phenocryst samples show similarly low gas contents (He, Ne and Ar ˜10 -10 cm 3/g). 3He/ 4He ratios, 5.3-2.11 Ra, are generally low if compared to those typical of the MORB and those of the European Subcontinental Mantle (ESCM), respectively R/ Ra 8.5±1 and 6.0-6.5. A decreasing trend is found from 1631 to 1796, while a more homogeneous set of data is obtained for more recent eruptions, as evidenced by an average R/ Ra value of 2.85. Neon ratios ( 21Ne/ 22Ne and 20Ne/ 22Ne) strongly differ from those typically found on volcanoes and suggest that a crustal component has been added in the source region to Mt. Vesuvius magmas. Argon ratios ( 40Ar/ 36Ar and 38Ar/ 36Ar) have values similar to the atmosphere and are well correlated. The low 40Ar/ 36Ar ratio (max. 302) is, however, in the range of the 40Ar/ 36Ar ratios obtained from several lava samples at other Italian volcanoes and might be considered to have a deep origin. Two hypothesis have been discussed: (1) a deep argon-like-air source, due to subduction of air-rich sediments and/or (2) a preferential loss of Ar, in comparison to lighter noble gases, from silicic melts. Helium isotopic analysis of gas samples recently collected from crater and submarine fumaroles are similar to those of lavas belonging to the final part of this eruptive cycle. This result supports the idea that no new juvenile fluids from the source region have been injected into the magmatic reservoir during the 1631-1944 eruptive cycle and, more importantly, until 1993. Both sets of data help to understand the genesis of these fluids and to constrain the current activity of the volcano.

  12. Statistical clumped isotope signatures

    NARCIS (Netherlands)

    Röckmann, T.; Popa, M. E.; Krol, M. C.; Hofmann, M. E. G.


    High precision measurements of molecules containing more than one heavy isotope may provide novel constraints on element cycles in nature. These so-called clumped isotope signatures are reported relative to the random (stochastic) distribution of heavy isotopes over all available isotopocules of a m

  13. Isotopic and enzymatic analyses of planktonic nitrogen utilisation in the vicinity of Cape Sines (Portugal) during weak upwelling activity (United States)

    Slawyk, Gerd; Coste, Bernard; Collos, Yves; Rodier, Martine


    Using measurements of 15N uptake and activities of nitrate reductase and glutamine synthetase, the utilization of nitrogenous nutrients by microplankton in the Portuguese upwelling area was investigated. During this cruise the euphotic zone of coastal waters was in most cases bisected by a nitracline forming two layers. Total inorganic nitrogen uptake rates (NH 4+ + NO 3-) in the upper mixed and nitrate-impoverished layer ranged from 0.1 to 0.8 nM h -1 and were primarily supported by regenerated (ammonium) nitrogen (62-97%), whereas they varied between 0.9 and 10.4 nM h -1 in the deep nitrate-rich layer and were mainly driven by new (nitrate) nitrogen (52-82%). Depth profiles of Chl a-specific uptake rates for ammonium and nitrate paralleled those of absolute uptake rates, i.e. values of VNH 4+Chl were highest (up to 16.1 nmol μg -1 h -1) in nitrate-poor surface waters while values of VNO 3-Chl were maximum (up to 8.4 nmol μg -1 h -1)within the nitracline. This latter vertical ordering of planktonic nitrogen nutrition was consistent with an aged upwelling situation. However, applying several indices of cell metabolism and nutritional status, such as 15N uptake/enzyme activity, surge uptake internally controlled uptake, and V maxChl/K t ratios, we were able to demonstrate that the phytoplankton assemblages inhabiting the nutrient-impoverished upper layer still bore the signature of physically mediated nitrogen (nitrate) supply generated by active upwelling that had occurred during the week before our visit to the area. This signature was the most evident in samples from the station furthest inshore and faded with distance from shore as a result of the deepening of the nitrate isopleths (weakening of upwelling activity), which showed the same offshore trend. The appearance of nitrate-rich waters at the surface, after a strong pulse of upwelling favourable winds just before the end of the cruise, led to a five-fold increase in average (over the euphotic zone

  14. Plutonium and americium in arctic waters, the North Sea and Scottish and Irish coastal zones

    DEFF Research Database (Denmark)

    Hallstadius, L.; Aarkrog, Asker; Dahlgaard, Henning;


    collected from the Irish coast in 1983. Fallout is found to dominate as a source of 239+240Pu north of latitude 65°N, while for 238Pu a substantial fraction originates from European nuclear fuel reprocessing facilities. The 238Pu/239+240Pu isotope ratio provides clear evidence of the transport of effluent...... of the Irish Sea) to Spitsbergen. 241Am found in Arctic waters probably originates from the decay of fallout 241Pu and, like Pu, tentatively has a residence time of the order of several years. Americium from Sellafield has an estimated mean residence time of 4–6 months in Scottish waters....

  15. Isotopes in heterogeneous catalysis

    CERN Document Server

    Hargreaves, Justin SJ


    The purpose of this book is to review the current, state-of-the-art application of isotopic methods to the field of heterogeneous catalysis. Isotopic studies are arguably the ultimate technique in in situ methods for heterogeneous catalysis. In this review volume, chapters have been contributed by experts in the field and the coverage includes both the application of specific isotopes - Deuterium, Tritium, Carbon-14, Sulfur-35 and Oxygen-18 - as well as isotopic techniques - determination of surface mobility, steady state transient isotope kinetic analysis, and positron emission profiling.

  16. Simultaneous analysis of oxybutynin and its active metabolite N-desethyl oxybutynin in human plasma by stable isotope dilution LC-MS/MS to support a bioequivalence study. (United States)

    Sharma, Primal; Patel, Daxesh P; Sanyal, Mallika; Berawala, Hiren; Guttikar, Swati; Shrivastav, Pranav S


    An isotope dilution high performance liquid chromatography-tandem mass spectrometry (LC-MS/MS) method has been developed for the simultaneous determination of oxybutynin and its pharmacologically active metabolite N-desethyl oxybutynin in human plasma. Extraction of oxybutynin, its metabolite and their deuterated analogs as internal standards (ISs) from 300 μL human plasma was carried out by liquid-liquid extraction with methyl tert-butyl ether-ethyl acetate solvent mixture. Chromatographic separation of analytes was performed on Cosmosil C18 (150 mm × 4.6 mm, 5 μm) column under isocratic conditions with acetonitrile-1.0mM ammonium acetate (90:10, v/v) as the mobile phase. Six endogenous plasma phospholipids (496.3/184.0, 524.3/184.0, 758.5/184.0, 786.5/184.0, 806.5/184.0 and 810.5/184.0) were monitored to determine the extraction efficiency under different extraction conditions. The precursor→product ion transition for both the analytes and ISs were monitored on a triple quadrupole mass spectrometer, operating in the multiple reaction monitoring and positive ionization mode. The method was validated over a concentration range of 0.050-10.0 ng/mL for oxybutynin and 0.500-100 ng/mL for N-desethyl oxybutynin. The mean extraction recovery for analytes (80.4%) and ISs (76.9%) was consistent across five QC levels. Bench top, wet and dry extract, freeze-thaw and long term stability was evaluated for both the analytes. The method was applied to support a bioequivalence study of 5mg tablet formulation in 74 healthy Indian subjects. Assay reproducibility was demonstrated by reanalysis of 344 incurred samples.

  17. {sup 239,} {sup 240,} {sup 241}Pu fingerprinting of plutonium in western US soils using ICPMS: solution and laser ablation measurements

    Energy Technology Data Exchange (ETDEWEB)

    Cizdziel, James V. [University of Nevada - Las Vegas, Harry Reid Center for Environmental Studies, Las Vegas, NV (United States); Ketterer, Michael E. [Northern Arizona University, Department of Chemistry and Biochemistry, Box 5698, Flagstaff, AZ (United States); Farmer, Dennis [University of Nevada - Las Vegas, Department of Health Physics, Las Vegas, NV (United States); Faller, Scott H. [US Environmental Protection Agency, Radiation and Indoor Environments National Laboratory, Box 98517, Las Vegas, NV (United States); Hodge, Vernon F. [University of Nevada - Las Vegas, Department of Chemistry, Las Vegas, NV (United States)


    .013 [{sup 240}Pu/{sup 239}Pu] - 0.0001; r {sup 2} = 0.971) with NTS and global fallout end-members. A rapid total dissolution procedure, followed by extraction chromatography and SF-ICPMS solution Pu analysis, generates excellent agreement with certified {sup 239+240}Pu activities for standard reference materials NIST 4350b, NIST 4353, NIST 4357, and IAEA 385. {sup 239+240}Pu activities and atom ratios determined by total dissolution reveal isotopic information in agreement with the LA-ICPMS dataset regarding the ubiquitous mixing of NTS and stratospheric fallout Pu sources in the regional environment. For several specific samples, the total dissolution method reveals that Pu is incompletely recovered by simpler HNO{sub 3}-HCl leaching procedures, since some of the Pu originating from the NTS is contained in refractory siliceous particles. (orig.)

  18. The estuarine geochemical reactivity of Zn isotopes and its relevance for the biomonitoring of anthropogenic Zn and Cd contaminations from metallurgical activities: Example of the Gironde fluvial-estuarine system, France (United States)

    Petit, Jérôme C. J.; Schäfer, Jörg; Coynel, Alexandra; Blanc, Gérard; Chiffoleau, Jean-François; Auger, Dominique; Bossy, Cécile; Derriennic, Hervé; Mikolaczyk, Mathilde; Dutruch, Lionel; Mattielli, Nadine


    Zinc stable isotopes measurements by MC-ICP-MS, validated by laboratory intercalibrations, were performed on wild oysters, suspended particles and filtered river/estuarine water samples to provide new constraints for the use of Zn isotopes as environmental tracers. The samples selected were representative of the long range (400 km) transport of metal (Zn, Cd, etc.) contamination from former Zn-refining activities at Decazeville (i.e. δ66Zn > 1‰) and its phasing out, recorded during 30 years in wild oysters from the Gironde Estuary mouth (RNO/ROCCH sample bank). The study also addresses additional anthropogenic sources (urban and viticulture) and focuses on geochemical reactivity of Zn in the turbidity gradient and the maximum turbidity zone (MTZ) of the fluvial Gironde Estuary. In this area, dissolved Zn showed a strong removal onto suspended particulate matter (SPM) and progressive enrichment in heavy isotopes with increasing SPM concentrations varying from δ66Zn = -0.02‰ at 2 mg/L to +0.90‰ at 1310 mg/L. These signatures were attributed to kinetically driven adsorption due to strongly increasing sorption sites in the turbidity gradient and MTZ of the estuary. Oysters from the estuary mouth, contaminated sediments from the Lot River and SPM entering the estuary showed parallel historical evolutions (1979-2010) for Zn/Cd ratios but not for δ66Zn values. Oysters had signatures varying from δ66Zn = 1.43‰ in 1983 to 1.18‰ in 2010 and were offset by δ66Zn = 0.6-0.7‰ compared to past (1988) and present SPM from the salinity gradient. Isotopic signatures in river-borne particles entering the Gironde Estuary under contrasting freshwater discharge regimes during 2003-2011 showed similar values (δ66Zn ≈ 0.35 ± 0.03‰; 1SD, n = 15), i.e. they were neither related to former metal refining activities at least for the past decade nor clearly affected by other anthropogenic sources. Therefore, the Zn isotopic signatures in Gironde oysters reflect the

  19. Historical changes in 239Pu and 240Pu sources in sedimentary records in the East China Sea: Implications for provenance and transportation

    DEFF Research Database (Denmark)

    Wang, Jinlong; Baskaran, Mark; Hou, Xiaolin


    Concentrations and isotopic compositions of plutonium (Pu) are widely used for its source identification and to determine transport processes of Pu-associated particulate matter and water. We investigated the concentrations of 239Pu and 240Pu and their ratios in a number of sediment samples from...

  20. Pb-Sr isotopic and geochemical constraints on sources and processes of lead contamination in well waters and soil from former fruit orchards, Pennsylvania, USA: A legacy of anthropogenic activities (United States)

    Ayuso, Robert A.; Foley, Nora K.


    Isotopic discrimination can be an effective tool in establishing a direct link between sources of Pb contamination and the presence of anomalously high concentrations of Pb in waters, soils, and organisms. Residential wells supplying water containing up to 1600 ppb Pb to houses built on the former Mohr orchards commercial site, near Allentown, PA, were evaluated to discern anthropogenic from geogenic sources. Pb (n = 144) and Sr (n = 40) isotopic data and REE (n = 29) data were determined for waters from residential wells, test wells (drilled for this study), and surface waters from pond and creeks. Local soils, sediments, bedrock, Zn-Pb mineralization and coal were also analyzed (n = 94), together with locally used Pb-As pesticide (n = 5). Waters from residential and test wells show overlapping values of 206Pb/207Pb, 208Pb/207Pb and 87Sr/86Sr. Larger negative Ce anomalies (Ce/Ce*) distinguish residential wells from test wells. Results show that residential and test well waters, sediments from residential water filters in water tanks, and surface waters display broad linear trends in Pb isotope plots. Pb isotope data for soils, bedrock, and pesticides have contrasting ranges and overlapping trends. Contributions of Pb from soils to residential well waters are limited and implicated primarily in wells having shallow water-bearing zones and carrying high sediment contents. Pb isotope data for residential wells, test wells, and surface waters show substantial overlap with Pb data reflecting anthropogenic actions (e.g., burning fossil fuels, industrial and urban processing activities). Limited contributions of Pb from bedrock, soils, and pesticides are evident. High Pb concentrations in the residential waters are likely related to sediment build up in residential water tanks. Redox reactions, triggered by influx of groundwater via wells into the residential water systems and leading to subtle changes in pH, are implicated in precipitation of Fe oxyhydroxides

  1. The role of extracellular carbonic anhydrase activity in inorganic carbon utilization of Phaeocystis globosa (Prymnesiophyceae) : A comparison with other marine algae using the isotopic disequilibrium technique

    NARCIS (Netherlands)

    Elzenga, JTM; Prins, HBA; Stefels, J


    The utilization of inorganic carbon species by the marine microalga Phaeocystis globasa (Prymnesiophyceae) and several other algal species from different taxa, was investigated by determining the time course of C-14 incorporation in isotopic disequilibrium experiments. From these kinetic data, concl

  2. Laser Isotope Enrichment for Medical and Industrial Applications

    Energy Technology Data Exchange (ETDEWEB)

    Leonard Bond


    Laser Isotope Enrichment for Medical and Industrial Applications by Jeff Eerkens (University of Missouri), Jay Kunze (Idaho State University), and Leonard Bond (Idaho National Laboratory) The principal isotope enrichment business in the world is the enrichment of uranium for commercial power reactor fuels. However, there are a number of other needs for separated isotopes. Some examples are: 1) Pure isotopic targets for irradiation to produce medical radioisotopes. 2) Pure isotopes for semiconductors. 3) Low neutron capture isotopes for various uses in nuclear reactors. 4) Isotopes for industrial tracer/identification applications. Examples of interest to medicine are targets to produce radio-isotopes such as S-33, Mo-98, Mo-100, W-186, Sn-112; while for MRI diagnostics, the non-radioactive Xe-129 isotope is wanted. For super-semiconductor applications some desired industrial isotopes are Si-28, Ga-69, Ge-74, Se-80, Te-128, etc. An example of a low cross section isotope for use in reactors is Zn-68 as a corrosion inhibitor material in nuclear reactor primary systems. Neutron activation of Ar isotopes is of interest in industrial tracer and diagnostic applications (e.g. oil-logging). . In the past few years there has been a sufficient supply of isotopes in common demand, because of huge Russian stockpiles produced with old electromagnetic and centrifuge separators previously used for uranium enrichment. Production of specialized isotopes in the USA has been largely accomplished using old ”calutrons” (electromagnetic separators) at Oak Ridge National Laboratory. These methods of separating isotopes are rather energy inefficient. Use of lasers for isotope separation has been considered for many decades. None of the proposed methods have attained sufficient proof of principal status to be economically attractive to pursue commercially. Some of the authors have succeeded in separating sulfur isotopes using a rather new and different method, known as condensation

  3. Zircon U-Pb geochronology, geochemistry and Sr-Nd-Pb isotopes from the metamorphic basement in the Wuhe Complex: Implications for Neoarchean active continental margin along the southeastern North China Craton and constraints on the petrogenesis of Mesozoic granitoids

    Directory of Open Access Journals (Sweden)

    Andong Wang


    Full Text Available We report zircon U-Pb geochronology, geochemistry and Sr-Nd-Pb isotope data from mafic granulites and garnet amphibolites of the Wuhe Complex in the southeastern margin of the North China Craton (NCC. In combination with previous data, our results demonstrate that these rocks represent fragments of the ancient lower crust, and have features similar to those of the granulite basement in the northern margin of the NCC. A detailed evaluation of the Pb isotope data shows that Pb isotopes cannot effectively distinguish the role of the Yangtze Craton basement from that of the NCC basement with regard to the source and generation of magmas, at least for southeastern NCC. The age data suggest that the protoliths of the granulites or amphibolites in the Wuhe Complex were most likely generated in Neoarchean and that these rocks were subjected to Paleoproterozoic (1.8–1.9 Ga high-pressure granulite facies metamorphism. This study also shows that the Precambrian metamorphic basement in the southeastern margin of the NCC might have formed in a tectonic setting characterized by a late Neoarchean active continental margin.

  4. Discovery of the Cobalt Isotopes


    Szymanski, T.; Thoennessen, M.


    Twenty-six cobalt isotopes have so far been observed; the discovery of these isotopes is discussed. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  5. Discovery of the Arsenic Isotopes

    CERN Document Server

    Shore, A; Heim, M; Schuh, A; Thoennessen, M


    Twenty-nine arsenic isotopes have so far been observed; the discovery of these isotopes is discussed. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  6. Isotope products manufacture in Russia and its prospects

    Energy Technology Data Exchange (ETDEWEB)

    Malyshev, S.V.; Okhotina, I.A.; Kalelin, E.A.; Krasnov, N.N.; Kuzin, V.V.; Malykh, J.A.; Makarovsky, S.B. [Tenex, Techsnabexport Co Ltd, Moscow (Russian Federation)


    At the present stage of the world economy development, stable and radioactive isotopes,preparations and products on their base are widely used in many fields of the national economy, medicine and scientific researches. The Russian Federation is one of the largest worldwide producers of a variety of nuclide products on the base of more than 350 isotopes, as follows: stable isotopes reactor, cyclotron, fission product radioactive isotopes, ion-radiation sources compounds, labelled with stable and radioactive isotopes, radionuclide short-lived isotope generators, radiopharmaceuticals, radionuclide light and heat sources; luminous paints on base of isotopes. The Russian Ministry for Atomic Energy coordinates activity for development and organization of manufacture and isotope products supply in Russia as well as for export. Within many years of isotope industry development, there have appeared some manufacturing centres in Russia, dealing with a variety of isotope products. The report presents the production potentialities of these centres and also an outlook on isotope production development in Russia in the next years

  7. Long-lasting Cadomian magmatic activity along an active northern Gondwana margin: U-Pb zircon and Sr-Nd isotopic evidence from the Brunovistulian Domain, eastern Bohemian Massif (United States)

    Soejono, Igor; Janoušek, Vojtěch; Žáčková, Eliška; Sláma, Jiří; Konopásek, Jiří; Machek, Matěj; Hanžl, Pavel


    Cadomian magmatic complexes of the Brunovistulian Domain crop out at the eastern termination of the Bohemian Massif. However, the age, nature and geotectonic affinity of some of pre-Variscan (meta-)igneous rock complexes from this domain are still unknown. Geochronological and geochemical study of the granitic rocks across the Brunovistulian Domain reveals new information about the timing and nature of this magmatic activity originally situated along the northern margin of Gondwana. Zircon U-Pb data (601 ± 3 Ma, Brno Massif; 634 ± 6 Ma, paraautochtonous core of the Svratka Dome; 568 ± 3 Ma, Bíteš orthogneiss) from the allochtonous Moravicum indicate the prolonged magmatic activity within the Brunovistulian Domain during the Ediacaran. The major- and trace-element and Sr-Nd isotopic signatures show heterogeneous geochemical characteristics of the granitic rocks and suggest a magmatic-arc geotectonic setting. The two-stage Depleted Mantle Nd model ages (c. 1.3-2.0 Ga) indicate derivation of the granitic rocks from a relatively primitive crustal source, as well as from an ancient and evolved continental crust of the Brunovistulian Domain. These results constrain the magmatic-arc activity to c. 635-570 Ma and provide a further evidence for a long-lived (at least c. 65 Myr) and likely episodic subduction-related magmatism at the northern margin of Gondwana. The presence of granitic intrusions derived from variously mature crustal sources at different times suggests heterogeneous crustal segments to having been involved in the magmatic-arc system during its multistage evolution.

  8. Calculation of individual isotope equilibrium constants for geochemical reactions (United States)

    Thorstenson, D.C.; Parkhurst, D.L.


    Theory is derived from the work of Urey (Urey H. C. [1947] The thermodynamic properties of isotopic substances. J. Chem. Soc. 562-581) to calculate equilibrium constants commonly used in geochemical equilibrium and reaction-transport models for reactions of individual isotopic species. Urey showed that equilibrium constants of isotope exchange reactions for molecules that contain two or more atoms of the same element in equivalent positions are related to isotope fractionation factors by ?? = (Kex)1/n, where n is the number of atoms exchanged. This relation is extended to include species containing multiple isotopes, for example 13C16O18O and 1H2H18O. The equilibrium constants of the isotope exchange reactions can be expressed as ratios of individual isotope equilibrium constants for geochemical reactions. Knowledge of the equilibrium constant for the dominant isotopic species can then be used to calculate the individual isotope equilibrium constants. Individual isotope equilibrium constants are calculated for the reaction CO2g = CO2aq for all species that can be formed from 12C, 13C, 16O, and 18O; for the reaction between 12C18 O2aq and 1H218Ol; and among the various 1H, 2H, 16O, and 18O species of H2O. This is a subset of a larger number of equilibrium constants calculated elsewhere (Thorstenson D. C. and Parkhurst D. L. [2002] Calculation of individual isotope equilibrium constants for implementation in geochemical models. Water-Resources Investigation Report 02-4172. U.S. Geological Survey). Activity coefficients, activity-concentration conventions for the isotopic variants of H2O in the solvent 1H216Ol, and salt effects on isotope fractionation have been included in the derivations. The effects of nonideality are small because of the chemical similarity of different isotopic species of the same molecule or ion. The temperature dependence of the individual isotope equilibrium constants can be calculated from the temperature dependence of the fractionation

  9. The production of stable isotopes in Spain

    Energy Technology Data Exchange (ETDEWEB)

    Urgel, M.; Iglesias, J.; Casas, J.; Saviron, J. M.; Quintanilla, M.


    The activities developed in the field of the production of stable isotopes by means of ion-exchange chromatography and thermal diffusion techniques are reported. The first method was used to study the separation of the nitrogen and boron isotopes, whereby the separation factor was determined by the break through method. Values ranging from 1,028 to 1,022 were obtained for the separation factor of nitrogen by using ammonium hydroxide solutions while the corresponding values as obtained for boron amounted to 1,035-1,027 using boric acid solutions. Using ammonium chloride or acetate and sodium borate, respectively, resulted in the obtention of values for the separation factor approaching unity. The isotopic separation has been carried out according to the method of development by displacement. The separation of the isotopes of the noble gases, oxygen, nitrogen and carbon has been accomplished resorting to the method of thermal diffusion. (Author) 16 refs.

  10. Iron isotopic fractionation during continental weathering

    Energy Technology Data Exchange (ETDEWEB)

    Fantle, Matthew S.; DePaolo, Donald J.


    The biological activity on continents and the oxygen content of the atmosphere determine the chemical pathways through which Fe is processed at the Earth's surface. Experiments have shown that the relevant chemical pathways fractionate Fe isotopes. Measurements of soils, streams, and deep-sea clay indicate that the {sup 56}Fe/{sup 54}Fe ratio ({delta}{sup 56}Fe relative to igneous rocks) varies from +1{per_thousand} for weathering residues like soils and clays, to -3{per_thousand} for dissolved Fe in streams. These measurements confirm that weathering processes produce substantial fractionation of Fe isotopes in the modern oxidizing Earth surface environment. The results imply that biologically-mediated processes, which preferentially mobilize light Fe isotopes, are critical to Fe chemistry in weathering environments, and that the {delta}{sup 56}Fe of marine dissolved Fe should be variable and negative. Diagenetic reduction of Fe in marine sediments may also be a significant component of the global Fe isotope cycle. Iron isotopes provide a tracer for the influence of biological activity and oxygen in weathering processes through Earth history. Iron isotopic fractionation during weathering may have been smaller or absent in an oxygen-poor environment such as that of the early Precambrian Earth.

  11. Chromium isotope variations

    DEFF Research Database (Denmark)

    D'Arcy, Joan Mary

    is incorporated into carbonates. Hence, ancient carbonates can potentially record the Cr isotopic composition (δ53Cr ‰) of seawater in the geological past. Reliable application and interpretation of this proxy requires a detailed knowledge about processes that fractionate Cr on the Earth’s surface...... deposited during the Early Ordovician — a time of known redox instability in ancient oceans – exhibit a significant positive Cr isotope excursion of +0.5‰. This excursion is interpreted as the reductive drawn down of dissolved Cr in seawater in response to the development of a proximal anoxic sink......, and the quantification the Cr isotope composition of major Cr fluxes into and out of ocean. This thesis adds to the current knowledge of the Cr isotope system and is divided into two studies. The focus of the first study was to determine what processes control the Cr isotopic compositionof river water and to quantify...

  12. Lasers utilizing CO2 isotopes (United States)

    Pechenin, Iu. V.; Domanov, M. S.


    The emission spectra and power characteristics of CW (C-12)(O-16)2, (C-13)(O-16)2, (C-12)(O-16)(O-18)2 and (C-12)(O-18) lasers are investigated. Laser output power is found to depend equally on the proportion of carbon and oxygen isotopes in the active medium for all isotopes except the asymmetrical (C-12)(O-16)(O-18), in which maximum output power is four to five times less due to the doubling of emission lines and limited enrichment caused by recombination into (C-12)(O-16)2 and (C-12)(O-18)2 molecules during discharge. The unsaturated gain is observed to increase linearly with enrichment, with that of nonsymmetrical molecules half that of the symmetrical molecules, while the maximum power output is independent of enrichment.

  13. Hydrothermal versus active margin sediment supply to the eastern equatorial Pacific over the past 23 million years traced by radiogenic Pb isotopes: Paleoceanographic and paleoclimatic implications (United States)

    Höfig, Tobias W.; Hoernle, Kaj; Hauff, Folkmar; Frank, Martin


    We investigated the evolution of the Pb isotopic composition of bulk sediments on the Cocos Plate in sedimentary successions of Deep Sea Drilling Project (DSDP) Site 495 and Ocean Drilling Program/Integrated Ocean Drilling Program (ODP/IODP) Site 1256 over the past 23 million years of depositional history. Our study addresses the relationship of the sediment Pb isotope record to plate tectonics, weathering inputs, and paleoceanography. It is the first effort to characterize the Pb isotopic evolution of eastern equatorial Pacific sedimentation covering the entire tectonic pathway of the Cocos Plate from its formation at the East Pacific Rise to its arrival at the Central American subduction zone. The Sites 495 and 1256 bulk sediment Pb isotope records are fully consistent over time despite distinct differences between the type of sediment deposited at both locations. A systematic and continuous trend from ∼23 to ∼6-4 Ma toward more radiogenic Pb isotopic compositions, e.g., 206Pb/204Pb ratios increase from 18.29 to 18.81, reflects a decrease in the contribution of hydrothermal particles from the East Pacific Rise and an increase in the predominantly eolian contribution of mixed weathering products from the continental arcs of the Northern and south Central Andes as well as from southern Mexico. Surprisingly, both the Pb isotopic composition of the detrital fraction and that of past seawater indicate that inputs from nearby Central America and the Galápagos Archipelago did not significantly contribute to the sediments of our core locations but were overwhelmed by other sediment sources. A systematic change to less radiogenic Pb isotope ratios in sediments younger than ∼4-3 Ma, reaching present-day 206Pb/204Pb values near 18.70, reflects a reduction of the continental input from the South Central Volcanic Zone of the Andean Arc and increased contributions from southern Mexican igneous complexes. This isotopic trend reversal took place as a consequence of

  14. Isotope abundance ratios of sr in wine provenance determinations, in a tree-root activity study, and of pb in a pollution study on tree-rings. (United States)

    Horn, P; Hölzl, S; Todt, W; Matthies, D


    Abstract In this contribution, the various and fundamentally different uses and applications of isotope signatures (of both heavy and light elements) are discussed. Examples are given for the successful use of (87)Sr/(86)Sr in uncovering fraud in wine trade. Also, in an experiment related to "Waldsterben", (87)Sr/(86)Sr analyses reveal rather unexpected responses of spruces and maple-trees to mechanical damage of their roots. In another study, from (206)Pb/(207)Pb (and (208)Pb/(207)Pb) analyses of tree growth-rings it is demonstrated that they do not accurately record lead burdens in the environment. This is contrary to current views on the subject of tree-rings as reliable banks of past heavy metal pollutions of the biosphere. Furthermore, new perspectives of applications of isotopes in biological tissues, including those of cosmogenic and nucleogenic origin will be shortly outlined.

  15. Estimation of the activity and isotopic composition of the fuel elements of the reactor in decaying; Estimacion de la actividad y composicion isotopica de los elementos combustibles del reactor en decaimiento

    Energy Technology Data Exchange (ETDEWEB)

    Aguilar H, F. [ININ, 52045 Ocoyoacac, Estado de Mexico (Mexico)


    At the present time its are had 59 fuel elements, 3 control bars with follower and 2 instrumented irradiated fuels that its are decaying in the pool of the reactor. The burnt one that its have these fuels is not uniform, the quantity of U-235 that contain at the moment it varies between 33.5 g up to 35.2 and its have a decay of at least 12 years. The burnt of the fuels was obtained with the CREMAT code, this burnt was takes like base to estimate the current isotopic inventory and the activity of the same ones using the ORIGEN2 code. (Author)

  16. High-fidelity MCNP modeling of a D-T neutron generator for active interrogation of special nuclear material (United States)

    Katalenich, Jeff; Flaska, Marek; Pozzi, Sara A.; Hartman, Michael R.


    Fast and robust methods for interrogation of special nuclear material (SNM) are of interest to many agencies and institutions in the United States. It is well known that passive interrogation methods are typically sufficient for plutonium identification because of a relatively high neutron production rate from 240Pu [1]. On the other hand, identification of shielded uranium requires active methods using neutron or photon sources [2]. Deuterium-deuterium (2.45 MeV) and deuterium-tritium (14.1 MeV) neutron-generator sources have been previously tested and proven to be relatively reliable instruments for active interrogation of nuclear materials [3,4]. In addition, the newest generators of this type are small enough for applications requiring portable interrogation systems. Active interrogation techniques using high-energy neutrons are being investigated as a method to detect hidden SNM in shielded containers [4,5]. Due to the thickness of some containers, penetrating radiation such as high-energy neutrons can provide a potential means of probing shielded SNM. In an effort to develop the capability to assess the signal seen from various forms of shielded nuclear materials, the University of Michigan Neutron Science Laboratory's D-T neutron generator and its shielding were accurately modeled in MCNP. The generator, while operating at nominal power, produces approximately 1×10 10 neutrons/s, a source intensity which requires a large amount of shielding to minimize the dose rates around the generator. For this reason, the existing shielding completely encompasses the generator and does not include beam ports. Therefore, several MCNP simulations were performed to estimate the yield of uncollided 14.1-MeV neutrons from the generator for active interrogation experiments. Beam port diameters of 5, 10, 15, 20, and 25 cm were modeled to assess the resulting neutron fluxes. The neutron flux outside the beam ports was estimated to be approximately 2×10 4 n/cm 2 s.

  17. First measurements of anthropogenic and natural radionuclides in surface soils (10 cm) of Cote d'Ivoire

    Energy Technology Data Exchange (ETDEWEB)

    Koua, A. [Universite de Cocody, Lab. de Physique Nucleaire et Radioprotection, UFR Sciences des Structures de la Matiere et de la Technologie, Abidjan (Cote d' Ivoire); Michel, H.; Alabdullah, J.; Barci, V.; Barci-Funel, G.; Ardisson, G. [Nice Sophia-Antipolis Univ., Lab. de Radiochimie, Sciences Analytiques et Environnement, 06 (France); Aka, H.K. [Universite de Cocody, Lab. de Chimie Physique, UFR Sciences des Structures de la Matiere et de la Technologie, Abidjan (Cote d' Ivoire)


    {sup 239-240}Pu and {sup 137}Cs activities in soil samples were measured in two sites of the littoral part of Cote d'Ivoire: Abidjan and the classified forest of 'la Comoe'. Two areas were chosen: a forest and a clearing. The aim of this work is to establish a starting point for nuclear contamination data of a non-nuclear country. Measured soil cores were of 10 cm depth. {sup 137}Cs and {sup 239-240}Pu activities, mainly due to weapon nuclear tests in the 1960's, were in the range 0.37-2.3 and 0.023-0.125 Bq kg{sup -1} respectively. {sup 239-240}Pu/{sup 137}Cs values were found to be about 0.024-0.19 in agreement with the expected value for nuclear tests. (authors)

  18. Uranium isotopes fingerprint biotic reduction (United States)

    Stylo, Malgorzata; Neubert, Nadja; Wang, Yuheng; Monga, Nikhil; Romaniello, Stephen J.; Weyer, Stefan; Bernier-Latmani, Rizlan


    Knowledge of paleo-redox conditions in the Earth’s history provides a window into events that shaped the evolution of life on our planet. The role of microbial activity in paleo-redox processes remains unexplored due to the inability to discriminate biotic from abiotic redox transformations in the rock record. The ability to deconvolute these two processes would provide a means to identify environmental niches in which microbial activity was prevalent at a specific time in paleo-history and to correlate specific biogeochemical events with the corresponding microbial metabolism. Here, we demonstrate that the isotopic signature associated with microbial reduction of hexavalent uranium (U), i.e., the accumulation of the heavy isotope in the U(IV) phase, is readily distinguishable from that generated by abiotic uranium reduction in laboratory experiments. Thus, isotope signatures preserved in the geologic record through the reductive precipitation of uranium may provide the sought-after tool to probe for biotic processes. Because uranium is a common element in the Earth’s crust and a wide variety of metabolic groups of microorganisms catalyze the biological reduction of U(VI), this tool is applicable to a multiplicity of geological epochs and terrestrial environments. The findings of this study indicate that biological activity contributed to the formation of many authigenic U deposits, including sandstone U deposits of various ages, as well as modern, Cretaceous, and Archean black shales. Additionally, engineered bioremediation activities also exhibit a biotic signature, suggesting that, although multiple pathways may be involved in the reduction, direct enzymatic reduction contributes substantially to the immobilization of uranium. PMID:25902522

  19. Perchlorate isotope forensics (United States)

    Böhlke, J.K.; Sturchio, N.C.; Gu, B.; Horita, J.; Brown, G.M.; Jackson, W.A.; Batista, J.; Hatzinger, P.B.


    Perchlorate has been detected recently in a variety of soils, waters, plants, and food products at levels that may be detrimental to human health. These discoveries have generated considerable interest in perchlorate source identification. In this study, comprehensive stable isotope analyses ( 37Cl/35Cl and 18O/17O/ 16O) of perchlorate from known synthetic and natural sources reveal systematic differences in isotopic characteristics that are related to the formation mechanisms. In addition, isotopic analyses of perchlorate extracted from groundwater and surface water demonstrate the feasibility of identifying perchlorate sources in contaminated environments on the basis of this technique. Both natural and synthetic sources of perchlorate have been identified in water samples from some perchlorate occurrences in the United States by the isotopic method. ?? 2005 American Chemical Society.

  20. Isotope Production Facility (IPF) (United States)

    Federal Laboratory Consortium — The Los Alamos National Laboratory has produced radioactive isotopes for medicine and research since the mid 1970s, when targets were first irradiated using the 800...

  1. Calcium stable isotope geochemistry

    Energy Technology Data Exchange (ETDEWEB)

    Gausonne, Nikolaus [Muenster Univ. (Germany). Inst. fuer Mineralogie; Schmitt, Anne-Desiree [Strasbourg Univ. (France). LHyGeS/EOST; Heuser, Alexander [Bonn Univ. (Germany). Steinmann-Inst. fuer Geologie, Mineralogie und Palaeontologie; Wombacher, Frank [Koeln Univ. (Germany). Inst. fuer Geologie und Mineralogie; Dietzel, Martin [Technische Univ. Graz (Austria). Inst. fuer Angewandte Geowissenschaften; Tipper, Edward [Cambridge Univ. (United Kingdom). Dept. of Earth Sciences; Schiller, Martin [Copenhagen Univ. (Denmark). Natural History Museum of Denmark


    This book provides an overview of the fundamentals and reference values for Ca stable isotope research, as well as current analytical methodologies including detailed instructions for sample preparation and isotope analysis. As such, it introduces readers to the different fields of application, including low-temperature mineral precipitation and biomineralisation, Earth surface processes and global cycling, high-temperature processes and cosmochemistry, and lastly human studies and biomedical applications. The current state of the art in these major areas is discussed, and open questions and possible future directions are identified. In terms of its depth and coverage, the current work extends and complements the previous reviews of Ca stable isotope geochemistry, addressing the needs of graduate students and advanced researchers who want to familiarize themselves with Ca stable isotope research.

  2. Isotopes in Greenland Precipitation

    DEFF Research Database (Denmark)

    Faber, Anne-Katrine

    the Arctic Ocean. A comprehensive database is created based on ice core and weather station data from Greenland within the period 1890-2014. Present day annual and seasonal mean values are computed for 326 locations in Greenland. Parameterization of the spatial distribution of temperature and δ18O are used...... of model and data can be used to improve the understanding of climate changes. This is done through analysis of isotope modelling, observations and ice core measurements. This dissertation comprises three projects: (1) Modelling the isotopic response to changes in Arctic sea surface conditions, (2......) Constructing a new Greenland database of observations and present-day ice core measurements, and (3) Performance test of isotope-enabled CAM5 for Greenland. The recent decades of rapid Arctic sea ice decline are used as a basis for an observational-based model experiment using the isotope-enabled CAM model 3...

  3. Isotopically controlled semiconductors

    Energy Technology Data Exchange (ETDEWEB)

    Haller, E.E.


    A review of recent research involving isotopically controlled semiconductors is presented. Studies with isotopically enriched semiconductor structures experienced a dramatic expansion at the end of the Cold War when significant quantities of enriched isotopes of elements forming semiconductors became available for worldwide collaborations. Isotopes of an element differ in nuclear mass, may have different nuclear spins and undergo different nuclear reactions. Among the latter, the capture of thermal neutrons which can lead to neutron transmutation doping, can be considered the most important one for semiconductors. Experimental and theoretical research exploiting the differences in all the properties has been conducted and will be illustrated with selected examples. Manuel Cardona, the longtime editor-in-chief of Solid State Communications has been and continues to be one of the major contributors to this field of solid state physics and it is a great pleasure to dedicate this review to him.

  4. Isotopes through the looking glass (United States)

    Mårtensson Pendrill, Ann Marie


    Nuclear distributions affect many aspects of atomic spectra. As an example, recent experimental results for the hyperfine anomaly in Fr isotopes are considered. These depend on nuclear charge and magnetization distributions. The variations in charge radii for these isotopes were studied earlier by measuring optical isotope shifts. The hyperfine anomalies for the odd-odd isotopes involve the neutron distributions, of interest for studies of parity nonconserving effects along a chain of isotopes.

  5. Methods of isotopic geochronology (United States)

    Gorokhov, I. M.; Levchenkov, O. A.

    Papers are presented on such topics as the age of the chemical elements; the age of meteorites, the moon, and the earth; isotopic ages of the most ancient terrestrial formations; and the Archean evolution of Enderby Land in the Antarctic as evidenced by isotopic dating. Consideration is also given to a uranium-lead geochronology technique for investigating Precambrian ore deposits, a Pb-Pb technique of zircon dating, and the potentials and limitations of Sm-Nd geochronology.

  6. Oxygen Isotopes in Meteorites (United States)

    Clayton, R. N.


    Oxygen isotope abundance variations in meteorites are very useful in elucidating chemical and physical processes that occurred during the formation of the solar system (Clayton, 1993). On Earth, the mean abundances of the three stable isotopes are 16O: 99.76%, 17O: 0.039%, and 18O: 0.202%. It is conventional to express variations in abundances of the isotopes in terms of isotopic ratios, relative to an arbitrary standard, called SMOW (for standard mean ocean water), as follows:The isotopic composition of any sample can then be represented by one point on a "three-isotope plot," a graph of δ17O versus δ18O. It will be seen that such plots are invaluable in interpreting meteoritic data. Figure 1 shows schematically the effect of various processes on an initial composition at the center of the diagram. Almost all terrestrial materials lie along a "fractionation" trend; most meteoritic materials lie near a line of "16O addition" (or subtraction). (4K)Figure 1. Schematic representation of various isotopic processes shown on an oxygen three-isotope plot. Almost all terrestrial materials plot along a line of "fractionation"; most primitive meteoritic materials plot near a line of "16O addition." The three isotopes of oxygen are produced by nucleosynthesis in stars, but by different nuclear processes in different stellar environments. The principal isotope, 16O, is a primary isotope (capable of being produced from hydrogen and helium alone), formed in massive stars (>10 solar masses), and ejected by supernova explosions. The two rare isotopes are secondary nuclei (produced in stars from nuclei formed in an earlier generation of stars), with 17O coming primarily from low- and intermediate-mass stars (shielding in the UV photodissociation of CO (van Dishoeck and Black, 1988). This process results from the large differences in abundance between C16O, on the one hand, and C17O and C18O on the other. Photolysis of CO occurs by absorption of stellar UV radiation in the

  7. Concentration and depuration of some radionuclides present in a chronically exposed population of mussels (Mytilus edulis)

    Energy Technology Data Exchange (ETDEWEB)

    Clifton, R.J.; Stevens, H.E.; Hamilton, E.I.


    Factors are described which affect the concentration (p Ci g/sup -1/ dry wt) and loss of /sup 241/ Am, /sup 239 +240/Pu, /sup 238/Pu, /sup 144/Ce, /sup 137/Cs, /sup 134/Cs, /sup 106/Ru, /sup 95/Zr and /sup 95/Nb in an exposed population of mussels Mytilus edulis L. from Ravenglass on the Esk estuary, Cumbria, UK which receives radioeffluents from the British Nuclear Fuels Ltd. (BNFL) plant at Sellafield, some 10 km to the north. Tidal position and mussel body size have a negligible influence on the concentration of /sup 241/Am, /sup 137/Cs and /sup 106/Ru in the total soft tissue, but variation in soft tissue weight throughout the year has a considerable influence on the apparent concentration and depuration times of these radionuclides. Apart from the clearance (tsub(1/2) biol, 1 to 3 h) of sediment-associated activity from the digestive tract, the depuration rate profiles follow a single component clearance curve with a biological half-life in excess of 200 d for /sup 241/ Am, /sup 239 +240/Pu, /sup 238/Pu and /sup 144/Ce, and of 40 d for /sup 137/Cs. The clearance of /sup 106/Ru is more complex and consists of a 3 component depuration profile with biological half-lives of 6 h, 12 d and 260 d. The depuration profiles presented in this work are for chronically ingested isotopes under natural conditions; acute exposure will most likely result in different profiles, especially those derived from laboratory spiking experiments. Isotope ratio data support the hypothesis that the main route of entry into the mussel for the majority of the radionuclides studied is from the water.

  8. Isotope Tales: Remaining Problems, Unsolvable Questions, and Gentle Successes (United States)

    fogel, marilyn; bradley, christina; newsome, seth; filipp, fabian


    Earth's biomes function and adapt today as climate changes and ecosystems and the organisms within them adapt. Stable isotope biogeochemistry has had a major influence in understanding climate perturbations and continues to be an active area of research on many fronts. Banking on the success of compound specific stable isotope analyses of amino acids, nitrogen, carbon, and hydrogen isotopes continue to reveal subtle shifts in oceanic food webs and metabolic changes in microbes, plants, and animals. A biochemical understanding of exactly how organisms process and partition stable isotopes during metabolism remains unsolved, but is required if this field is to move beyond description to quantitation. Although the patterns of carbon and nitrogen isotopes are fairly well established in the common amino acids, we need to consider specifics: How do shifting metabolic pathways (metabolomics) influence the outcome of stable isotope partitioning? What influence does the gut microflora in animals have on isotopic labeling? What are the intramolecular isotope patterns of common amino acids and what do they tell us? What can be learned with other isotope systems, such as hydrogen? Results and ideas of how to move forward in this field will be presented starting at the molecular level and ending with ecosystems.

  9. Isotopic Evidence of Unaccounted for Fe and Cu Erythropoietic Pathways (United States)

    Albarede, F.; Telouk, P.; Lamboux, A.; Jaouen, K.; Balter, V.


    Despite its potential importance for understanding perturbations in the Fe-Cu homeostatic pathways, the natural isotopic variability of these metals in the human body remains unexplored. We measured the Fe, Cu, and Zn isotope compositions of total blood, serum, and red blood cells of ~50 young blood donors by multiple-collector ICP-MS after separation and purification by anion exchange chromatography. Zn is on average 0.2 permil heavier in erythrocytes (δ 66Zn=0.44±0.33 permil) with respect to serum but shows much less overall isotopic variability than Fe and Cu, which indicates that isotope fractionation depends more on redox conditions than on ligand coordination. On average, Fe in erythrocytes (δ 56Fe=-2.59±0.47 permil) is isotopically light by 1-2 permil with respect to serum, whereas Cu in erythrocytes (δ 65Cu=0.56±0.50 permil) is 0.8 percent heavier. Fe and Cu isotope compositions clearly separate erythrocytes of men and women. Fe and Cu from B-type men erythrocytes are visibly more fractionated than all the other blood types. Isotope compositions provide an original method for evaluating metal mass balance and homeostasis. Natural isotope variability shows that the current models of Fe and Cu erythropoiesis, which assume that erythropoiesis is restricted to bone marrow, violate mass balance requirements. It unveils unsuspected major pathways for Fe, with erythropoietic production of isotopically heavy ferritin and hemosiderin, and for Cu, with isotopically light Cu being largely channeled into blood and lymphatic circulation rather than into superoxide dismutase-laden erythrocytes. Iron isotopes provide an intrinsic measuring rod of the erythropoietic yield, while Cu isotopes seem to gauge the relative activity of erythropoiesis and lymphatics.

  10. An examination of the H/D isotope substitution effect on selectivity and activity in the cavitating ultrasound hydrogenation of aqueous 3-buten-2-ol and 1,4-pentadien-3-ol on Pd-black

    Energy Technology Data Exchange (ETDEWEB)

    Boyles, Kelly R.; Chajkowski, Sarah M.; Disselkamp, Robert S.; Peden, Charles HF


    An H/D isotope effect study of the (H2 versus D2) hydrogenation of the aqueous substrates 3-buten-2-ol (3B2OL) and 1,4-pentadien-3-ol (14PD3OL) was performed using Pd-black catalyst. Either H2O or D2O solvents were employed (for alcohol H/D isotope substitution). Two experimental processing conditions of cavitating ultrasound (CUS) and stirred/silent (SS) methods were used. Products formed include 2-butanol and 2-butanone for the former, and 3-pentanol and 3-pentanone for the latter. The observed selectivity and pseudo-first order reaction rate coefficients (e.g., activity) to these products enabled a mechanistic interpretation of the various reaction conditions to be proposed. Experiments utilized a 50 mL batch reactor maintained at 298 K, employed 5.4 atm of H2 or D2 gas, while seven aliquots were collected during the course of the reaction. We have utilized 1-propanol as an inert dopant in all experiments to enable the rapid onset of cavitation in the CUS systems as described earlier [R.S. Disselkamp et al., J. Catal., 227, 552 (2004)]. The following conclusions were noted. First, the activity of the CUS compared to SS processing were ~100-fold larger. Second, variable catalyst loading experiments for stirred/silent D2 hydrogenation processing indicated that mass transfer of hydrogen gas to the Pd-surface played a role such that higher catalyst loading reduced surface D-atom concentrations and reduced saturated alcohol formation (e.g., via reduced H-addition to surface alkyl radicals). Third, for CUS processing the ketone selectivities for experiments employing water compared to D2O indicated that 3B2OL were twice as large, whereas for 14PD3OL they were comparable. This suggests, somewhat surprisingly, that for 3B2OL enol tautomerization to ketone is a slow, and possibly rate-controlling, process. Finally, again for CUS processing, the similarity in ketone selectivities (all ~17%) for H2 compared to D2 hydrogenation for both 3B2OL and 14PD3OL suggest that both H

  11. Isotope geochemistry. Biological signatures in clumped isotopes of O₂. (United States)

    Yeung, Laurence Y; Ash, Jeanine L; Young, Edward D


    The abundances of molecules containing more than one rare isotope have been applied broadly to determine formation temperatures of natural materials. These applications of "clumped" isotopes rely on the assumption that isotope-exchange equilibrium is reached, or at least approached, during the formation of those materials. In a closed-system terrarium experiment, we demonstrate that biological oxygen (O2) cycling drives the clumped-isotope composition of O2 away from isotopic equilibrium. Our model of the system suggests that unique biological signatures are present in clumped isotopes of O2—and not formation temperatures. Photosynthetic O2 is depleted in (18)O(18)O and (17)O(18)O relative to a stochastic distribution of isotopes, unlike at equilibrium, where heavy-isotope pairs are enriched. Similar signatures may be widespread in nature, offering new tracers of biological and geochemical cycling.

  12. Stable isotopes. Applications and production; Les isotopes stables. Applications - production

    Energy Technology Data Exchange (ETDEWEB)

    Goldstein, S.; Louvet, P.; Soulie, E. [eds.


    This conference presents 46 communications concerning stable isotope production, utilization and application, grouped in 6 sessions and posters. The various themes are: biological applications (pharmacology, medical diagnosis, metabolism and protein studies, toxicity and response studies, labelled compounds), analysis procedures (NMR analysis for macromolecules, tracer studies), nuclear applications (utilization of stable isotopes in nuclear reactors), biological, physical and chemical applications (mass transfer, mobility, crystallography, isotopic exchange), stable isotope production (ion chromatography, ion cyclotron resonance, cryogenic distillation).

  13. Deformation of C isotopes

    CERN Document Server

    Kanada-Enyo, Y


    Systematic analysis of the deformations of proton and neutron densities in even-even C isotopes was done based on the method of antisymmetrized molecular dynamics. The $E2$ transition strength was discussed in relation to the deformation. We analyze the $B(E2;2^+_1\\to 0^+_1)$ in $^{16}$C, which has been recently measured to be abnormally small. The results suggest the difference of the deformations between proton and neutron densities in the neutron-rich C isotopes. It was found that stable proton structure in C isotopes plays an important role in the enhancement the neutron skin structure as well as in the systematics of $B(E2)$ in the neutron-rich C.

  14. Earth Processes: Reading the Isotopic Code (United States)

    Basu, Asish; Hart, Stan

    Publication of this monograph will coincide, to a precision of a few per mil, with the centenary of Henri Becquerel's discovery of "radiations actives" (C. R. Acad. Sci., Feb. 24, 1896). In 1896 the Earth was only 40 million years old according to Lord Kelvin. Eleven years later, Boltwood had pushed the Earth's age past 2000 million years, based on the first U/Pb chemical dating results. In exciting progression came discovery of isotopes by J. J. Thomson in 1912, invention of the mass spectrometer by Dempster (1918) and Aston (1919), the first measurement of the isotopic composition of Pb (Aston, 1927) and the final approach, using Pb-Pb isotopic dating, to the correct age of the Earth: close—2.9 Ga (Gerling, 1942), closer—3.0 Ga (Holmes, 1949) and closest—4.50 Ga (Patterson, Tilton and Inghram, 1953).

  15. Isotopes in Condensed Matter

    CERN Document Server

    G Plekhanov, Vladimir


    This book provides a concise introduction to the newly created sub-discipline of solid state physics isotopetronics. The role of isotopes in materials and their properties are describe  in this book. The problem of the enigma of the atomic mass in microphysics is briefly discussed.  The range of the applications of isotopes is wide: from biochemical process in living organisms to modern technical applications in quantum information. Isotopetronics promises to improve nanoelectronic and optoelectronic devices. With numerous illustrations this book is useful to researchers, engineers and graduate students.

  16. Even–odd effects in prompt emission of spontaneously fissioning even–even Pu isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Tudora, A., E-mail: [University of Bucharest, Faculty of Physics, Bucharest Magurele, POB MG-11, R-76900 (Romania); Hambsch, F.-J. [EC-JRC Institute for Reference Materials and Measurements (IRMM), Retieseweg 111, B-2440, Geel (Belgium); Giubega, G.; Visan, I. [University of Bucharest, Faculty of Physics, Bucharest Magurele, POB MG-11, R-76900 (Romania)


    The available experimental Y(A,TKE) data for {sup 236,238,240,242,244}Pu(SF) together with the Zp model prescription with appropriate parameters allows the investigation of even–odd effects in fragment distributions. The size of the global even–odd effect in Y(Z) is decreasing from {sup 244}Pu(SF) to {sup 236}Pu(SF) confirming the general observation of a decrease of the even–odd effect with the fissility parameter. Charge polarizations (ΔZ) and root-mean squares (rms) as a function of A of {sup 236–244}Pu(SF) were obtained for the first time. In the asymmetric fission region both ΔZ(A) and rms(A) exhibit oscillations with a periodicity of about 5 mass units due to the even–odd effects. The total average charge deviations 〈ΔZ〉 (obtained by averaging ΔZ(A) over the experimental Y(A) distribution) are of about |0.5| for all studied Pu(SF) systems. The comparison of the calculated ΔZ(A) and rms(A) of {sup 240}Pu(SF) with those of {sup 239}Pu(n{sub th},f) reported by Wahl shows an in-phase oscillation with a higher amplitude in the case of {sup 240}Pu(SF), confirming the higher even–odd effect in the case of SF. As in the previously studied cases ({sup 233,235}U(n{sub th},f), {sup 239}Pu(n{sub th},f), {sup 252}Cf(SF)) the even–odd effects in the prompt emission of {sup 236–244}Pu(SF) are mainly due to the Z even–odd effects in fragment distributions and charge polarizations and the N even–odd effects in the average neutron separation energies from fragments 〈Sn〉. The size of the global N even–odd effect in 〈Sn〉 is decreasing with the fissility parameter, being higher for the Pu(SF) systems compared to the previously studied systems. The prompt neutron multiplicities as a function of Z, ν(Z), exhibit sawtooth shapes with a visible staggering for asymmetric fragmentations. The size of the global Z even–odd effect in ν(Z) exhibits a decreasing trend with increasing fissility. The average prompt neutron multiplicities as a

  17. Estimation of Radiation Doses in the Marshall Islands Based on Whole Body Counting of Cesium-137 (137Cs) and Plutonium Urinalysis

    Energy Technology Data Exchange (ETDEWEB)

    Daniels, J; Hickman, D; Kehl, S; Hamilton, T


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

  18. Estimation of Radiation Doses in the Marshall Islands Based on Whole Body Counting of Cesium-137 (137Cs) and Plutonium Urinalysis

    Energy Technology Data Exchange (ETDEWEB)

    Daniels, J; Hickman, D; Kehl, S; Hamilton, T


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

  19. Isotope hydrology: applied discipline in earth sciences; Hydrologie isotope: une discipline des sciences de la terre

    Energy Technology Data Exchange (ETDEWEB)

    Froehlich, K.; Rozanski, K.; Araguas Araguas, L. [Isotope Hydrology Section, International Atomic Agency, Vienna (Austria)


    The discipline `isotope hydrology` is being reviewed from the perspective of the Isotope Hydrology Section of the International Atomic Energy Agency in Vienna. The Section was created in the late fifties and is activities involved int the scientific progress of the discipline. The role of the IAEA in the development of isotope hydrology has always been of a dual nature: on one hand, the Section has been and still is heavily engaged in supporting and coordinating further development of isotope methodologies, on the other hand, it serves as an interface between the methodological development in research institutes and the applied work using proven techniques in field projects on water resources assessment and management. The paper provides a brief overview of applications of isotope-based methodologies in hydrology, with emphasis on new trends and challenges related to man`s growing impact on the water cycle. This contribution is a tribute to the memory of the former Head of the Isotope Hydrology Section, Jean-Charles Fontes, to whom we owe so much. (authors) 30 refs.

  20. Sulfur isotope signatures in gypsiferous sediments of the Estancia and Tularosa Basins as indicators of sulfate sources, hydrological processes, and microbial activity (United States)

    Szynkiewicz, Anna; Moore, Craig H.; Glamoclija, Mihaela; Pratt, Lisa M.


    In order to reconstruct paleo-environmental conditions for the saline playa lakes of the Rio Grande Rift, we investigated sediment sulfate sources using sulfur isotope compositions of dissolved SO42- ions in modern surface water, groundwater, and SO42- precipitated in the form of gypsum sediments deposited during the Pleistocene and Holocene in the Tularosa and Estancia Basins. The major sulfate sources are Lower and Middle Permian marine evaporites (δ 34S of 10.9-14.4‰), but the diverse physiography of the Tularosa Basin led to a complex drainage system which contributed sulfates from various sources depending on the climate at the time of sedimentation. As inferred from sulfur isotope mass balance constraints, weathering of sulfides of magmatic/hydrothermal and sedimentary origin associated with climate oscillations during Last Glacial Maximum contributed about 35-50% of the sulfates and led to deposition of gypsum with δ 34S values of -1.2‰ to 2.2‰ which are substantially lower than Permian evaporates. In the Estancia Basin, microbial sulfate reduction appears to overprint sulfur isotopic signatures that might elucidate past groundwater flows. A Rayleigh distillation model indicates that about 3-18% of sulfates from an inorganic groundwater pool (δ 34S of 12.6-13.8‰) have been metabolized by bacteria and preserved as partially to fully reduced sulfur-bearing minerals species (elemental sulfur, monosulfides, disulfides) with distinctly negative δ 34S values (-42.3‰ to -20.3‰) compared to co-existing gypsum (-3.8‰ to 22.4‰). For the Tularosa Basin microbial sulfate reduction had negligible effect on δ 34S value of the gypsiferous sediments most likely because of higher annual temperatures (15-33 °C) and lower organic carbon content (median 0.09%) in those sediments leading to more efficient oxidation of H 2S and/or smaller rates of sulfate reduction compared to the saline playas of the Estancia Basin (5-28 °C; median 0.46% of organic carbon

  1. Discoveries of isotopes by fission

    Indian Academy of Sciences (India)

    M Thoennessen


    Of the about 3000 isotopes presently known, about 20% have been discovered in fission. The history of fission as it relates to the discovery of isotopes as well as the various reaction mechanisms leading to isotope discoveries involving fission are presented.

  2. Concentrations of plutonium and americium in plankton from the western Mediterranean Sea

    Energy Technology Data Exchange (ETDEWEB)

    Sanchez-Cabeza, Joan-Albert; Merino, Juan; Masque, Pere [Insitut de Ciencia i Tecnologia Ambiental-Departament de Fisica, Universitat Autonoma de Barcelona, 08193 Bellaterra, Barcelona (Spain); Mitchell, Peter I.; Vintro, L. Leon [Department of Experimental Physics, University College Dublin, Dublin 4 (Ireland); Schell, William R. [Graduate School of Public Health, University of Pittsburgh, Pittsburgh, PA 15261 (United States); Cross, Lluisa; Calbet, Albert [Institut de Ciencies del Mar, Pg. Maritim Barceloneta, 37-49 08003, Barcelona (Spain)


    Understanding the transfer of radionuclides through the food chain leading to man and in particular, the uptake of transuranic nuclides by plankton, is basic to assess the potential radiological risk of the consumption of marine products by man. The main sources of transuranic elements in the Mediterranean Sea in the past were global fallout and the Palomares accident, although at present smaller amounts are released from nuclear establishments in the northwestern region. Plankton from the western Mediterranean Sea was collected and analyzed for plutonium and americium in order to study their biological uptake. The microplankton fractions accounted for approximately 50% of the total plutonium contents in particulate form. At Garrucha (Palomares area), microplankton showed much higher {sup 239,240}Pu activity, indicating the contamination with plutonium from the bottom sediments. Concentration factors were within the range of the values recommended by the International Atomic Energy Agency. Continental shelf mesoplankton was observed to efficiently concentrate transuranics. In open seawaters, concentrations were much lower. We speculate that sediments might play a role in the transfer of transuranics to mesoplankton in coastal waters, although we cannot discard that the difference in species composition may also play a role. In Palomares, both {sup 239,240}Pu and {sup 241}Am showed activities five times higher than the mean values observed in continental shelf mesoplankton. As the plutonium isotopic ratios in the contaminated sample were similar to those found in material related to the accident, the contamination was attributed to bomb debris from the Palomares accident. Concentration factors in mesoplankton were also in relatively good agreement with the ranges recommended by IAEA. In the Palomares station the highest concentration factor was observed in the sample that showed predominance of the dynoflagellate Ceratium spp. Mean values of the enrichment factors

  3. Isotopic Implicit Surface Meshing

    NARCIS (Netherlands)

    Boissonnat, Jean-Daniel; Cohen-Steiner, David; Vegter, Gert


    This paper addresses the problem of piecewise linear approximation of implicit surfaces. We first give a criterion ensuring that the zero-set of a smooth function and the one of a piecewise linear approximation of it are isotopic. Then, we deduce from this criterion an implicit surface meshing algor

  4. Forensic Stable Isotope Biogeochemistry (United States)

    Cerling, Thure E.; Barnette, Janet E.; Bowen, Gabriel J.; Chesson, Lesley A.; Ehleringer, James R.; Remien, Christopher H.; Shea, Patrick; Tipple, Brett J.; West, Jason B.


    Stable isotopes are being used for forensic science studies, with applications to both natural and manufactured products. In this review we discuss how scientific evidence can be used in the legal context and where the scientific progress of hypothesis revisions can be in tension with the legal expectations of widely used methods for measurements. Although this review is written in the context of US law, many of the considerations of scientific reproducibility and acceptance of relevant scientific data span other legal systems that might apply different legal principles and therefore reach different conclusions. Stable isotopes are used in legal situations for comparing samples for authenticity or evidentiary considerations, in understanding trade patterns of illegal materials, and in understanding the origins of unknown decedents. Isotope evidence is particularly useful when considered in the broad framework of physiochemical processes and in recognizing regional to global patterns found in many materials, including foods and food products, drugs, and humans. Stable isotopes considered in the larger spatial context add an important dimension to forensic science.

  5. Isotope hydrograph separation

    Energy Technology Data Exchange (ETDEWEB)

    Fritz, P. [UFZ-Umweltforschungszentrum, Centre of Environmental Research Leipzig-Halle, Leipzig (Germany)


    Storm-runoff thus reflects the complex hydraulic behaviour of drainage basins and water-links of such systems. Water of different origin may participate in the events and in this lecture, the application of isotope techniques to separate storm hydrographs into different components will be presented.


    Institute of Scientific and Technical Information of China (English)


    <正>20072750 Huang Sijing(State Key Laboratory of Oil/Gas Reservoir Geology and Exploitation,Chengdu University of Technology,Chengdu 610059,China);Pei Changrong Age Calibration for the Boundary between Lower and Middle Triassic by Strontium Isotope Stratigraphy in Eastern Sichuan Province


    Institute of Scientific and Technical Information of China (English)


    <正>20040631 Chen Jiangfeng (School of Earth and Space Sciences, University of Science and Technology of China, Hefei, Anhui) ; Xie Zhi Relationships Between Rb-Sr, Ar - Ar Geochronometers and Oxygen Isotopic Equilibrium of Intrusions from Eastern Anhui Province, China (Geological Journal of China Universities, ISSN 1006 - 7493, CN 32 -


    Institute of Scientific and Technical Information of China (English)


    <正>20090432 Zhou Shuqing (School of Energy Resources, China University of Geosciences Beijing 100083, China); Huang Haiping Stable Isotopic Records vs. Important Events in Life Evolution and the Concurrent Environment (Geological Review, ISSN0371-5736, CN11-1952, 54(2), 2008, p.225-231, 3 illus., 1 table, 77 refs.)


    Institute of Scientific and Technical Information of China (English)


    <正>20141014Wang Hairan(State Key Laboratory of Continental Dynamics,Department of Geology,Northwest University,Xi’an710069,China);Zhao Hongge Theory and Application of Zircon U-Pb Isotope Dating Technique(Geology and Resources,ISSN1671-1947,CN21-1458/P,22(3),2013,p.229


    Institute of Scientific and Technical Information of China (English)


    <正>20070454 Bao Zengkuan (Institute of High Energy Physics, CAS, Beijing 100049, China); Yuan Wanming Apatite (U-Th)/He Dating and Its Application (Acta Petrologica et Mineralogica, ISSN1000-6524, CN11-1966/P, 24(2), 2005, p.126-132, 2 illus., 25 refs.) Key words: isotopic geochronology

  11. Isotopic constraints on biogeochemical cycling of copper in the ocean. (United States)

    Takano, Shotaro; Tanimizu, Masaharu; Hirata, Takafumi; Sohrin, Yoshiki


    Trace elements and their isotopes are being actively studied as powerful tracers in the modern ocean and as proxies for the palaeocean. Although distributions and fractionations have been reported for stable isotopes of dissolved Fe, Cu, Zn and Cd in the ocean, the data remain limited and only preliminary explanations have been given. Copper is of great interest because it is either essential or toxic to organisms and because its distribution reflects both biological recycling and scavenging. Here we present new isotopic composition data for dissolved Cu (δ(65)Cu) in seawater and rainwater. The Cu isotopic composition in surface seawater can be explained by the mixing of rain, river and deep seawater. In deep seawater, δ(65)Cu becomes heavier with oceanic circulation because of preferential scavenging of the lighter isotope ((63)Cu). In addition, we constrain the marine biogeochemical cycling of Cu using a new box model based on Cu concentrations and δ(65)Cu.

  12. Embryotoxicity of stable isotopes and use of stable isotopes in studies of teratogenetic mechanisms

    Energy Technology Data Exchange (ETDEWEB)

    Spielmann, H.; Nau, H.


    Experiments on teratogenic effects of stable isotopes from our own and other laboratories are evaluated. In the first series of investigations, the enrichment of the stable isotope /sup 13/C derived from U-/sup 13/C-glucose was studied in mouse embryos at various stages of development, including limb buds in organ culture. Preimplantation mouse embryos incubated in vitro in /sup 13/C-enriched medium for 48 hours showed normal development during subsequent differentiation in vitro and also in vivo after embryo transfer to faster mothers. These embryos were 15% to 20% enriched in /sup 13/C. Administration of U-13-C-glucose to pregnant mice during organogenesis led to an increase of the absolute /sup 13/C content of the embryo for several days after the end of isotope administration, whereas the enrichment in maternal tissue decreased. No alterations of embryonic development were detected due to stable isotope enrichment. Development of cultured mouse limb buds was unaffected by incubation with 82 mol% U-/sup 13/C-glucose as judged from morphologic and biochemical criteria. The second part of the article describes the value of deuterium-labeled drugs as probes into the mechanism of activation of teratogenic metabolites. A comparison of the pharmacokinetics as well as the teratogenicity between cyclophosphamide and some specific deuterium-labeled analogues showed that the isotope effect observed can be related to a particular metabolic pathway crucial for teratogenic activation by this drug.

  13. Characterization and Source Term Assessments of Radioactive Particles from Marshall Islands Using Non-Destructive Analytical Techniques

    Energy Technology Data Exchange (ETDEWEB)

    Jernstrom, J; Eriksson, M; Simon, R; Tamborini, G; Bildstein, O; Carlos-Marquez, R; Kehl, S R; Betti, M; Hamilton, T


    A considerable fraction of radioactivity entering the environment from different nuclear events is associated with particles. The impact of these events can only be fully assessed where there is some knowledge about the mobility of particle bound radionuclides entering the environment. The behavior of particulate radionuclides is dependent on several factors, including the physical, chemical and redox state of the environment, the characteristics of the particles (e.g., the chemical composition, crystallinity and particle size) and on the oxidative state of radionuclides contained in the particles. Six plutonium-containing particles stemming from Runit Island soil (Marshall Islands) were characterized using non-destructive analytical and microanalytical methods. By determining the activity of {sup 239,240}Pu and {sup 241}Am isotopes from their gamma peaks structural information related to Pu matrix was obtained, and the source term was revealed. Composition and elemental distribution in the particles were studied with synchrotron radiation based micro X-ray fluorescence (SR-{mu}-XRF) spectrometry. Scanning electron microscope equipped with energy dispersive X-ray detector (SEMEDX) and secondary ion mass spectrometer (SIMS) were used to examine particle surfaces. Based on the elemental composition the particles were divided into two groups; particles with plain Pu matrix, and particles where the plutonium is included in Si/O-rich matrix being more heterogeneously distributed. All of the particles were identified as fragments of initial weapons material. As containing plutonium with low {sup 240}Pu/{sup 239}Pu atomic ratio, {approx}2-6%, which corresponds to weapons grade plutonium, the source term was identified to be among the safety tests conducted in the history of Runit Island.

  14. Novel Molecular Insights into Classical and Alternative Activation States of Microglia as Revealed by Stable Isotope Labeling by Amino Acids in Cell Culture (SILAC)-based Proteomics. (United States)

    Bell-Temin, Harris; Culver-Cochran, Ashley E; Chaput, Dale; Carlson, Christina M; Kuehl, Melanie; Burkhardt, Brant R; Bickford, Paula C; Liu, Bin; Stevens, Stanley M


    Microglia, the resident immune cells of the brain, have been shown to display a complex spectrum of roles that span from neurotrophic to neurotoxic depending on their activation status. Microglia can be classified into four stages of activation, M1, which most closely matches the classical (pro-inflammatory) activation stage, and the alternative activation stages M2a, M2b, and M2c. The alternative activation stages have not yet been comprehensively analyzed through unbiased, global-scale protein expression profiling. In this study, BV2 mouse immortalized microglial cells were stimulated with agonists specific for each of the four stages and total protein expression for 4644 protein groups was quantified using SILAC-based proteomic analysis. After validating induction of the various stages through a targeted cytokine assay and Western blotting of activation states, the data revealed novel insights into the similarities and differences between the various states. The data identify several protein groups whose expression in the anti-inflammatory, pro-healing activation states are altered presumably to curtail inflammatory activation through differential protein expression, in the M2a state including CD74, LYN, SQST1, TLR2, and CD14. The differential expression of these proteins promotes healing, limits phagocytosis, and limits activation of reactive nitrogen species through toll-like receptor cascades. The M2c state appears to center around the down-regulation of a key member in the formation of actin-rich phagosomes, SLP-76. In addition, the proteomic data identified a novel activation marker, DAB2, which is involved in clathrin-mediated endocytosis and is significantly different between M2a and either M1 or M2b states. Western blot analysis of mouse primary microglia stimulated with the various agonists of the classical and alternative activation states revealed a similar trend of DAB2 expression compared with BV2 cells.

  15. Fundamental studies on kinetic isotope effect (KIE) of hydrogen isotope fractionation in natural gas systems (United States)

    Ni, Yunyan; Ma, Qisheng; Ellis, Geoffrey S.; Dai, Jinxing; Katz, Barry; Zhang, Shuichang; Tang, Yongchun


    Based on quantum chemistry calculations for normal octane homolytic cracking, a kinetic hydrogen isotope fractionation model for methane, ethane, and propane formation is proposed. The activation energy differences between D-substitute and non-substituted methane, ethane, and propane are 318.6, 281.7, and 280.2 cal/mol, respectively. In order to determine the effect of the entropy contribution for hydrogen isotopic substitution, a transition state for ethane bond rupture was determined based on density function theory (DFT) calculations. The kinetic isotope effect (KIE) associated with bond rupture in D and H substituted ethane results in a frequency factor ratio of 1.07. Based on the proposed mathematical model of hydrogen isotope fractionation, one can potentially quantify natural gas thermal maturity from measured hydrogen isotope values. Calculated gas maturity values determined by the proposed mathematical model using δD values in ethane from several basins in the world are in close agreement with similar predictions based on the δ 13C composition of ethane. However, gas maturity values calculated from field data of methane and propane using both hydrogen and carbon kinetic isotopic models do not agree as closely. It is possible that δD values in methane may be affected by microbial mixing and that propane values might be more susceptible to hydrogen exchange with water or to analytical errors. Although the model used in this study is quite preliminary, the results demonstrate that kinetic isotope fractionation effects in hydrogen may be useful in quantitative models of natural gas generation, and that δD values in ethane might be more suitable for modeling than comparable values in methane and propane.

  16. Fundamental studies on kinetic isotope effect (KIE) of hydrogen isotope fractionation in natural gas systems (United States)

    Ni, Y.; Ma, Q.; Ellis, G.S.; Dai, J.; Katz, B.; Zhang, S.; Tang, Y.


    Based on quantum chemistry calculations for normal octane homolytic cracking, a kinetic hydrogen isotope fractionation model for methane, ethane, and propane formation is proposed. The activation energy differences between D-substitute and non-substituted methane, ethane, and propane are 318.6, 281.7, and 280.2cal/mol, respectively. In order to determine the effect of the entropy contribution for hydrogen isotopic substitution, a transition state for ethane bond rupture was determined based on density function theory (DFT) calculations. The kinetic isotope effect (KIE) associated with bond rupture in D and H substituted ethane results in a frequency factor ratio of 1.07. Based on the proposed mathematical model of hydrogen isotope fractionation, one can potentially quantify natural gas thermal maturity from measured hydrogen isotope values. Calculated gas maturity values determined by the proposed mathematical model using ??D values in ethane from several basins in the world are in close agreement with similar predictions based on the ??13C composition of ethane. However, gas maturity values calculated from field data of methane and propane using both hydrogen and carbon kinetic isotopic models do not agree as closely. It is possible that ??D values in methane may be affected by microbial mixing and that propane values might be more susceptible to hydrogen exchange with water or to analytical errors. Although the model used in this study is quite preliminary, the results demonstrate that kinetic isotope fractionation effects in hydrogen may be useful in quantitative models of natural gas generation, and that ??D values in ethane might be more suitable for modeling than comparable values in methane and propane. ?? 2011 Elsevier Ltd.

  17. High-Resolution Records of the Holocene Paleoenvironmental Variation Reflected by Carbonate and Its Isotopic Compositions in Bosten Lake and Response to Glacial Activities

    Institute of Scientific and Technical Information of China (English)

    ZHANG Chengjun; ZHENG Mianping; Alexander PROKOPENKO; Steffen MISCHKE; GOU Xiaohui; YANG Qili; ZHANG Wanyi; FENG Zhaodong


    The Early Holocene paleoclimate in Bosten Lake on the northern margin of the Tarim Basin, southern Xinjiang, is reconstructed through an analysis of a 953 cm long core (BSTC2000) taken from Bosten Lake. Multiple proxies of this core, including the mineral components of carbonate, carbonate content, stable isotopic compositions of carbonate, Ca/Sr, TOC and C/N and C/S of organic matter, are used to reconstruct the climatic change since 8500 a B.P. The chronology model is made by nine AMS ~(14)C ages of leaves, seeds and organic matter contained in two parallel cores. The climate was cold and wet during 8500 to 8100 a B.P. Temperature increased from 8100 to 6400 a B.P., the climate was warm and humid, and the lake expanded. The lake level was highest during this stage. Then from 6400 to 5100 a B.P., the climate became cold and the lake level decreased slightly. During the late mid-Holocene, the climate was hot and dry from 5100 to 3100 a B.P., but there was a short cold period during 4400 to 3800 a B.P. At this temporal interval, a mass of ice and snow melting water supplied the lake at the early time and made the lake level rise. The second highest lake level stage occurred during 5200 to 3800 a B.P. The climate was cool and wet during 3100 to 2200 a B.P., when the lake expanded with decreasing evaporation. The lake had the last short-term high level during 3100 to 2800 a B.P. After this short high lake level period, the lake shrank because of the long-term lower temperature and reduced water supply. From 2200 to 1200 a B.P., the climate was hot and dry, and the lake shrank greatly. Although the temperature decreased somewhat from 1200 a B.P. to the present, the climate was warm and dry. The lake level began to rise a little again, but it did not reach the river bed altitude of the Konqi River, an outflow river of the Bosten Lake.


    Institute of Scientific and Technical Information of China (English)


    <正>20131727 Huang Xiaowen(State Key Laboratory of Ore Deposit Geochemistry,Institute of Geochemistry,Chinese Academy of Sciences,Guiyang 550002,China);Qi Liang Preliminary Study on Sample-Preparation for Re-Os Isotopic Dating of Pyrite(Geochimica,ISSN0379-1726,CN44-1398/P,41(4),2012,p.380-386,3illus.,2tables,25refs)Key words:pyrite,Re-Os dating


    Institute of Scientific and Technical Information of China (English)


    <正>20050934 Chen Zhihong (Chinese Academy of Geological Sciences, Beijing 100037, China); Lu Songnian Age of the Fushui Intermediate-Mafic Intrusive Complex in the Qinling Orogen, New Zircon U - Pb and Whole -Rock Sm and Nd Isotope Chronological Evidence (Geological Bulletin of China, ISSN 1671-2552, CN11-4648/P, 23(4), 2004, p. 322-328, 3 illus. , 3 tables, 10 refs. )


    Institute of Scientific and Technical Information of China (English)


    <正>20132601 Cui Yurong(Tianjin Institute of Geology and Mineral Resources,China Geological Survey,Tianjin 300170,China);Zhou Hongying In Situ LA-MC-ICP-MS U-Pb Isotopic Dating of Monazite(Acta Geoscientica Sinica,ISSN0375-5444,CN11-1856/P,33(6),2012,p.865-876,6illus.,4tables,41refs.)Key words:monazite,U-Pb dating


    Energy Technology Data Exchange (ETDEWEB)



    The use of isotope labels has had a fundamentally important role in the determination of mechanisms of homogeneously catalyzed reactions. Mechanistic data is valuable since it can assist in the design and rational improvement of homogeneous catalysts. There are several ways to use isotopes in mechanistic chemistry. Isotopes can be introduced into controlled experiments and followed where they go or don't go; in this way, Libby, Calvin, Taube and others used isotopes to elucidate mechanistic pathways for very different, yet important chemistries. Another important isotope method is the study of kinetic isotope effects (KIEs) and equilibrium isotope effect (EIEs). Here the mere observation of where a label winds up is no longer enough - what matters is how much slower (or faster) a labeled molecule reacts than the unlabeled material. The most careti studies essentially involve the measurement of isotope fractionation between a reference ground state and the transition state. Thus kinetic isotope effects provide unique data unavailable from other methods, since information about the transition state of a reaction is obtained. Because getting an experimental glimpse of transition states is really tantamount to understanding catalysis, kinetic isotope effects are very powerful.

  2. Stable isotopic signature of Australian monsoon controlled by regional convection (United States)

    Zwart, C.; Munksgaard, N. C.; Kurita, N.; Bird, M. I.


    The aim of this study was to identify the main meteorological drivers of rainfall isotopic variation in north Australia in order to improve the interpretation of isotopic proxy records in this region. An intense monitoring program was conducted during two monsoonal events that showed significant and systematic isotopic change over time. The results showed a close link between isotopic variation in precipitation and variability in monsoon conditions, associated with the presence of large convective envelopes propagating through the study site. The largest negative amplitudes in the isotopic signal were observed when eastward and westward moving precipitation systems within the convective envelope merged over the measurement site. This suggests that the amplitude of the isotopic signal is related to the size and activity of the convective envelope. The strong correlation between rainfall isotopic variation, regional outgoing longwave radiation and regional rainfall amount supports this conclusion. This is further strengthened by the strong relationship between isotopic variation and the integrated rainfall history of air masses prior to arriving at the measurement locations. A local amount effect was not significant and these findings support the interpretation of δ18O as proxy for regional climatic conditions rather than local rainfall amount. Meteorological parameters that characterize intra-seasonal variability of monsoon conditions were also found to be strongly linked to inter-seasonal variability of the monthly based δ18O values in the Global Network of Isotopes in Precipitation (GNIP) database. This leads to the conclusion that information about the Australian monsoon variability can likely be inferred from the isotopic proxy record in North Australia on short (intra seasonal) and long (inter seasonal or longer) timescales.

  3. Nuclear physics and stable isotopes; Physique nucleaire et isotopes stables

    Energy Technology Data Exchange (ETDEWEB)

    Goutte, D. [CEA Centre d`Etudes de Saclay, 91 - Gif-sur-Yvette (France). Dept. d`Astrophysique, de la Physique des Particules, de la Physique Nucleaire et de l`Instrumentation Associee


    The aim of this paper is to show that fundamental research in nuclear physics requires utilization of stable isotopes; stable isotopes are essential as target material since a large quantity of nucleus have to be studied in order to appreciate all the complexity of the nuclear structure, but also as a tool, such as beams, for the same purpose. Examples are given with samarium, tin and germanium isotopes. 7 figs.

  4. Influence of isotopic re-equilibration on speleothem and fluid inclusion isotope ratios after primary calcite precipitation (United States)

    Kluge, Tobias; Haderlein, Astrid; Weißbach, Therese


    quantitative estimates of oxygen isotope exchange rates and to infer the dimension of the actively participating molecular layer at the surface of the calcite mineral. References: Mavromatis, V., Bundeleva, I.A., Shirokova, L.S., Millo, C., Pokrovsky, P.S., Benezeth, P., Ader, M., Oelkers, E.H., 2015. The continuous re-equilibration of carbon isotope compositions of hydrous Mg carbonates in the presence of cyanobacteria. Chem Geol., 404, 41-51. Oelkers, E. H., Berning, U.-N., Rinder, T., Mavromatis, V., Perez-Fernandez, A., Pogge von Strandmann, P., 2015. Rapid isotopic fractionation among minerals and fluids during dissolution, precipitation, and at equilibrium. Goldschmidt abstracts, 2318.

  5. Lithium isotope separation by laser

    Energy Technology Data Exchange (ETDEWEB)

    Arisawa, T.; Maruyama, Y.; Suzuki, Y.; Shiba, K.


    A lithium isotope separation was performed using a laser isotope separation method. It was found that the lithium atoms with a natural isotopic abundance enhanced its /sup 6/Li concentration up to over 90% by tuning the laser wavelength to the /sup 2/Psub(1/2) of /sup 6/Li. Too high power, however, leads to a loss of enrichment due to the power broadening effect which was analysed by the equation of motion of density matrices.

  6. Hydrogen Isotope Exchange Properties of Porous Solids Containing Hydrogen

    Energy Technology Data Exchange (ETDEWEB)



    Porous solids such as activated alumina, silica and molecular sieves generally contain significant amounts of hydrogen atoms in the form of H2O or OH even at high temperature and low humidity environment. A significant amount of this hydrogen is available for reversible isotopic exchange. This exchange reaction is slow under normal conditions and does not render itself to practical applications. But if the exchange kinetics is improved this reaction has the potential to be used for tritium removal from gas streams or for hydrogen isotopic separation.The use of catalysts to improve the exchange kinetics between hydrogen isotope in the gas phase and that in the solid phase was investigated. Granules of alumina, silica and molecular sieve were coated with platinum or palladium as the catalyst. The granules were packed in a 2-cm diameter column for isotope exchange tests. Gas streams containing different concentrations of deuterium in nitrogen or argon were fed through the protium saturated column. Isotope concentration in column effluent was monitored to generate isotope break-through curves. The curves were analyzed to produce information on the kinetics and capacity of the material. The results showed that all materials tested provided some extent of isotope exchange but some were superior both in kinetics and capacity. This paper will present the test results.

  7. Plutonium contamination in soils in open space and residential areas near Rocky Flats, Colorado. (United States)

    Litaor, M I


    Spatial analysis of the 240Pu:239Pu isotopic ratio of 42 soil samples collected around Rocky Flats Plant near Golden, Colorado, was conducted to assess the effect of Rocky Flats Plant activity on the soil environment. Two probability maps that quantified the uncertainty of the spatial distribution of plutonium isotopic ratios were constructed using the sequential Gaussian simulation technique (sGs). Assuming a plutonium isotopic ratio range of 0.152+/-0.003 to 0.169+/-0.009 is characteristic to global fallout in Colorado, and a mean value of 0.155 is representative for the Rocky Flats Plant area, the main findings of the current work were (1) the areas northwest and southwest of Rocky Flats Plant exhibited a plutonium ratio > or = 0.155, thus were minimally impacted by the plant activity; (2) the study area east of Rocky Flats Plant (approximately 120 km2) exhibited a plutonium isotopic ratio open space and residential areas amounted to 111.2 GBq, with a standard error of estimate of 50.8 GBq.

  8. Argon isotope fractionation induced by stepwise heating (United States)

    Trieloff, Mario; Falter, Martina; Buikin, Alexei I.; Korochantseva, Ekaterina V.; Jessberger, Elmar K.; Altherr, Rainer


    Noble gas isotopes are widely used to elucidate the history of the rocks in which they have been trapped, either from distinct reservoirs or by accumulation following radioactive decay. To extract noble gases from their host rocks, stepwise heating is the most commonly used technique to deconvolve isotopically different components, e.g., atmospheric, in situ radiogenic, or excess radiogenic from mantle or crustal reservoirs. The accurate determination of the isotopic composition of these different components is of crucial importance, e.g., for ages obtained by 40Ar- 39Ar stepheating plateaus. However, diffusion theory-based model calculations predict that the stepwise thermal extraction process from mineral phases induces isotope fractionation and, hence, adulterates the original composition. Such effects are largely unconsidered, as they are small and a compelling experimental observation is lacking. We report the first unequivocal evidence for significant mass fractionation of argon isotopes during thermal extraction, observed on shungite, a carbon-rich Precambrian sedimentary rock. The degree of fractionation, as monitored by 38Ar/ 36Ar and 40Ar/ 36Ar ratios, very well agrees with theoretical predictions assuming an inverse square root dependence of diffusion coefficient and atomic mass, resulting in easier extraction of lighter isotopes. Hence, subatmospheric 40Ar/ 36Ar ratios obtained for argon extracted at low temperatures may not represent paleoatmospheric argon. Shungite argon resembles modern atmospheric composition, but constraints on the timing of trapping appear difficult to obtain, as shungites are multicomponent systems. In 40Ar- 39Ar stepwise heating, the isotope fractionation effect could cause systematic underestimations of plateau ages, between 0.15 and 0.4% depending on age, or considerably higher if samples contain appreciable atmospheric Ar. The magnitude of this effect is similar to the presently achieved uncertainties of this increasingly

  9. Cold regions isotope applications

    Energy Technology Data Exchange (ETDEWEB)

    Perrigo, L.D.; Divine, T.E.


    Pacific Northwest Laboratories (PNL) started the Cold Regions Isotope Applications Program in FY-1975 to identify special conditions in the Arctic and similar geographic areas (Cold Regions) where radioisotope power, heater, or sterilization systems would be desirable and economically viable. Significant progress was made in the first year of this program and all objectives for this initial 12-month period were achieved. The major conclusions and recommendations resulting for this effort are described below. The areas of interest covered include: radiosterilization of sewage; heating of septic tanks; and radioisotope thermoelectric generators as power sources for meteorological instruments and navigational aids. (TFD)

  10. Si Isotopes of Brownleeite (United States)

    Nakamura-Messenger, K.; Messenger, Scott R.; Ito, M.; Keller, L. P.; Clemett, S. J.; Jones, J. H.; Tatsuoka, H.; Zolensky, M. E.; Tatsuoka, H.


    Brownleeite is a manganese silicide, ideally stoichiometric MnSi, not previously observed in nature until its discovery within an interplanetary dust particle (IDP) that likely originated from a comet [1]. Three discrete brownleeite grains in the IDP L2055 I3 (4 microns in size, hereafter IDP I3) were identified with maximum dimensions of 100, 250 and 600 nm and fully analyzed using scanning-transmission electron microscopy (STEM) [1]. One of the grains (100 nm in size) was poikilitically enclosed by low-Fe, Mn-enriched (LIME) olivine. LIME olivine is epitaxial to the brownleeite with the brownleeite (200) parallel to the olivine c* [1]. LIME olivine is an enigmatic phase first reported from chondritic porous IDPs and some unequilibrated ordinary chondrites [ 2], that is commonly observed in chondritic-porous IDPs. Recently, LIME olivine has been also found in comet Wild-2 (Stardust) samples [3], indicating that LIME olivine is a common mineral component of comets. LIME olivine has been proposed to form as a high temperature condensate in the protosolar nebula [2]. Brownleeite grains also likely formed as high-temperature condensates either in the early Solar System or in the outflow of an evolved star or supernova explosion [1]. The isotopic composition of the brownleeite grains may strongly constrain their ultimate source. To test this hypothesis, we performed isotopic analyses of the brownleeite and the associated LIME olivine, using the NASA/JSC NanoSIMS 50L ion microprobe.

  11. Pu and Am determination in the environment—method development (United States)

    Afonin, M.; Simonoff, M.; Donard, O.; Michel, H.; Ardisson, G.


    A high resolution inductively coupled plasma mass spectrometric (HR-ICP-MS) method for the determination of plutonium isotopes, Am and the 240Pu/239Pu isotope ratio utilising modification of Pu-02-RC Plutonium in Soil Samples, Pu-03-RC Plutonium in Soil Residue—Total Dissolution Method, Pu-11-RC Plutonium Purification—Ion Exchange Technique, Pu-12-RC Plutonium and/or Americium in Soil or Sediments, HASL-300 was developed. Total plutonium concentrations (239+240Pu) measured in environmental samples by this HR-ICP-MS method were in good agreement with recommended data obtained from a-spectrometry. It was achieved the decreasing of the time to analyze the samples over than 33%.

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

    Energy Technology Data Exchange (ETDEWEB)

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


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

  13. Worldwide lead-isotope ratio in bivalves and sediments

    DEFF Research Database (Denmark)

    Larsen, Martin Mørk; Jacobsen, Gitte; Strand, Jakob;

    The lead-isotope ratio have been used to assess and identify impact of leaded gasoline, coal combustion and  mineral activities[ref 1] due to the difference in 206Pb (~52%), 207Pb (~24%) and 208Pb (~23%) isotope ratios. The source of these differences is the decaying of the parent isotopes of 238U...... to 206Pb, 235U to 207Pb and 232Th to 208Pb. 204Pb is the only stable Pb isotope usually contributing 1% of the total Pb. Differences in 206Pb/207Pb ratio ranges from 1.06 to 1.10 in old Pb ores (e.g. the time of the roman empire), whereas recent mining from radiogenic (high U and Th contents) ores can...

  14. Calcium isotopes in wine (United States)

    Holmden, C. E.


    The δ 44/40Ca values of bottled wine vary between -0.76% to -1.55% on the seawater scale and correlate weakly with inverse Ca concentration and Mg/Ca ratio, such that the lowest δ 44/40Ca values have the highest Ca concentrations and lowest Mg/Ca ratios. The correlation is notable in the sense that the measured wines include both whites and reds sampled from different wine growing regions of the world, and cover a wide range of quality. Trends among the data yield clues regarding the cause of the observed isotopic fractionation. White wines, and wines generally perceived to be of lower quality, have lower δ 44/40Ca values compared to red wines and wines of generally perceived higher quality. Quality was assessed qualitatively through sensory evaluation, price, and scores assigned by critics. The relationship between δ 44/40Ca and wine quality was most apparent when comparing wines of one varietal from one producer from the same growing region. In the vineyard, wine quality is related to factors such as the tonnage of the crop and the ripeness of the grapes at the time of harvesting, the thickness of the skins for reds, the age of the vines, as well as the place where the grapes were grown (terroir). Quality is also influenced by winemaking practices such as fermentation temperature, duration of skin contact, and barrel ageing. Accordingly, the relationship between δ 44/40Ca and wine quality may originate during grape ripening in the vineyard or during winemaking in the cellar. We tested the grape ripening hypothesis using Merlot grapes sampled from a vineyard in the Okanagan, British Columbia, using sugar content (degrees Brix) as an indicator of ripeness. The grapes were separated into pulp, skin, and pip fractions and were analyzed separately. Thus far, there is no clear evidence for a systematic change in δ 44/40Ca values associated with progressive ripening of grapes in the vineyard. On the day of harvesting, the δ 44/40Ca value of juice squeezed from

  15. CO/sub 2/-isotope lasers

    Energy Technology Data Exchange (ETDEWEB)

    Pechenin, Yu.V.; Domanov, M.S.


    The emission spectra and power characteristics of CW (C-12)(O-16)2, (C-13)(O-16)2, (C-12)(O-16)(O-18)2 and (C-12)(O-18) lasers are investigated. Laser output power is found to depend equally on the proportion of carbon and oxygen isotopes in the active medium for all isotopes except the asymmetrical (C-12)(O-16)(O-18), in which maximum output power is four to five times less due to the doubling of emission lines and limited enrichment caused by recombination into (C-12)(O-16)2 and (C-12)(O-18)2 molecules during discharge. The unsaturated gain is observed to increase linearly with enrichment, with that of nonsymmetrical molecules half that of the symmetrical molecules, while the maximum power output is independent of enrichment.

  16. Activation cross sections of proton and deuteron induced nuclear reactions on holmium and erbium, related to the production of $^{161}$Er and $^{160}$Er medical isotopes

    CERN Document Server

    Tárkányi, F; Takács, S; Hermanne, A; Baba, M


    Experimental excitation functions for long-lived products in proton induced reactions were measured with the activation method in the 37-65 MeV energy range on natural holmium. Stacked foil irradiation technique and high resolution gamma spectrometry were used in order to measure cross-section data for the production of $^{161}$Er, $^{160}$Er and $^{159,157}$Dy. For comparison of the production routes of medically related $^{161}$Er and $^{160}$Er radioisotopes new experimental cross section data were deduced for the $^{162}$Er(p,x)$^{161,160}$Er and $^{162}$Er(d,x)$^{161,160}$Er reactions by re-evaluating gamma-ray spectra from earlier measurements. No earlier data were found in the literature for these reactions. The experimental data are compared with results of TALYS theoretical code reported in TENDL-2015.

  17. Activation cross sections of proton and deuteron induced nuclear reactions on holmium and erbium, related to the production of (161)Er and (160)Er medical isotopes. (United States)

    Tárkányi, F; Ditrói, F; Takács, S; Hermanne, A; Baba, M


    Experimental excitation functions for long-lived products in proton induced reactions were measured with the activation method in the 37-65MeV energy range on natural holmium. Stacked foil irradiation technique and high resolution gamma spectrometry were used in order to measure cross-section data for the production of (161)Er, (160)Er and (1)(59,157)Dy. For comparison of the production routes of medically related (161)Er and (160)Er radioisotopes new experimental cross section data were deduced for the (162)Er(p,x)(161,160)Er and (162)Er(d,x)(161,160)Er reactions by re-evaluating gamma-ray spectra from earlier measurements. No earlier data were found in the literature for these reactions. The experimental data are compared with results of TALYS theoretical code reported in TENDL-2015.

  18. Radium isotopes in the lower Mississippi River (United States)

    Kraemer, T. F.; Curwick, P. B.


    Radium isotopes have been measured in Mississippi River water at several locations between St. Francisville and Venice, Louisiana. Measured activities averaged 11.1 dpm/100 L (disintegrations per minute per 100 L) for dissolved 226Ra with a 228Ra/226Ra activity ratio of 1.04 and a 224Ra/228Ra activity ratio of 1.06 for the section of river above a phosphogypsum waste-discharge input. Down river from this site, the dissolved 226Ra activity averaged 22.4 dpm/100 L with a 228Ra/226Ra activity ratio of 0.55 and a 224Ra/228Ra activity ratio of 0.87. Chemical and isotopic reequilibration of the radium in the waste with that in the river water and suspended sediments occurs very rapidly. Fluxes of 226Ra are calculated to be 2.44×1014 dpm/yr (disintegrations per minute per year) for the main stem of the Mississippi during phosphogypsum disposal compared to 0.98×1014 dpm/yr when no phosphogypsum disposal is occurring. 28Ra flux is calculated to be 1.06×1014 dpm/yr during disposal and 1.01×1014 dpm/yr in the absence of disposal. The radium flux is estimated to be 45% in the dissolved state and 55% in the adsorbed state.

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

    Energy Technology Data Exchange (ETDEWEB)

    Mujid Kazimi


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

  20. Competition from Isotopic Modelling

    Directory of Open Access Journals (Sweden)

    Virginie Fabre


    Full Text Available During later MOIS3, in Europe two populations were present, autochthonous Neanderthals and modern humans. Ecological competition between these two populations has often been evoked but never demonstrated. Our aim is to establish whether resource competition occurred. In this paper, in order to examine the possibility of ecological competition between these two populations, 599 isotopic data were subjected to rigorous statistical treatment and analysis through mixing models. The aim of this paper was to compare dietary strategies of Neanderthals and modern humans over time. Our conclusions suggest that Neanderthals and modern humans shared dietary habits in the particular environmental context of MOIS3 characterised in Europe by climatic deterioration. In this environmental context, the resource competition between Neanderthals and modern humans may have accelerated the disappearance of the Neanderthal population.

  1. Isotope Effects in ESR Spectroscopy

    Directory of Open Access Journals (Sweden)

    Werner Herrmann


    Full Text Available In order to present the relationship between ESR spectroscopy and isotope effects three levels are considered: (i ESR spectroscopy is described on a general level up to the models for interpretation of the experimental spectra, which go beyond the usually used time and mass independent spin-Hamilton operator, (ii the main characteristics of the generalized isotope effects are worked out, and finally (iii the basic, mainly quantum mechanical effects are used to describe the coupling of electron spins with the degrees of freedom, which are accessible under the selected conditions, of the respective paramagnetic object under investigation. The ESR parameters and the respective models are formalized so far, that they include the time and mass depending influences and reflect the specific isotope effects. Relations will be established between the effects in ESR spectra to spin relaxation, to spin exchange, to the magnetic isotope effect, to the Jahn-Teller effects, as well as to the influence of zero-point vibrations. Examples will be presented which demonstrate the influence of isotopes as well as the kind of accessible information. It will be differentiated with respect to isotope effects in paramagnetic centres itself and in the respective matrices up to the technique of ESR imaging. It is shown that the use of isotope effects is indispensable in ESR spectroscopy.

  2. Distribution of artificial radionuclides in deep sediments of the Mediterranean Sea

    Energy Technology Data Exchange (ETDEWEB)

    Garcia-Orellana, J. [Departament de Fisica, Universitat Autonoma de Barcelona, E-08193 Bellaterra (Spain); Institut de Ciencia i Tecnologia Ambientals (ICTA), Universitat Autonoma de Barcelona, E-08193 Bellaterra (Spain)], E-mail:; Pates, J.M. [Lancaster Environment Centre, Lancaster University, Lancaster, LA1 4YQ (United Kingdom); Masque, P. [Departament de Fisica, Universitat Autonoma de Barcelona, E-08193 Bellaterra (Spain); Institut de Ciencia i Tecnologia Ambientals (ICTA), Universitat Autonoma de Barcelona, E-08193 Bellaterra (Spain); Bruach, J.M. [Departament de Fisica, Universitat Autonoma de Barcelona, E-08193 Bellaterra (Spain); Sanchez-Cabeza, J.A. [Departament de Fisica, Universitat Autonoma de Barcelona, E-08193 Bellaterra (Spain); Institut de Ciencia i Tecnologia Ambientals (ICTA), Universitat Autonoma de Barcelona, E-08193 Bellaterra (Spain); International Atomic Energy Agency, Marine Environment Laboratories, MC-98000 (Monaco)


    Artificial radionuclides enter the Mediterranean Sea mainly through atmospheric deposition following nuclear weapons tests and the Chernobyl accident, but also through the river discharge of nuclear facility effluents. Previous studies of artificial radionuclides impact of the Mediterranean Sea have focussed on shallow, coastal sediments. However, deep sea sediments have the potential to store and accumulate pollutants, including artificial radionuclides. Deep sea marine sediment cores were collected from Mediterranean Sea abyssal plains (depth > 2000 m) and analysed for {sup 239,240}Pu and {sup 137}Cs to elucidate the concentrations, inventories and sources of these radionuclides in the deepest areas of the Mediterranean. The activity - depth profiles of {sup 210}Pb, together with {sup 14}C dating, indicate that sediment mixing redistributes the artificial radionuclides within the first 2.5 cm of the sedimentary column. The excess {sup 210}Pb inventory was used to normalize {sup 239,240}Pu and {sup 137}Cs inventories for variable sediment fluxes. The {sup 239,240}Pu/{sup 210}Pb{sub xs} ratio was uniform across the entire sea, with a mean value of 1.24 x 10{sup -3}, indicating homogeneous fallout of {sup 239,240}Pu. The {sup 137}Cs/{sup 210}Pb{sub xs} ratio showed differences between the eastern (0.049) and western basins (0.030), clearly significant impact of deep sea sediments from the Chernobyl accident. The inventory ratios of {sup 239,240}Pu/{sup 137}Cs were 0.041 and 0.025 in the western and eastern basins respectively, greater than the fallout ratio, 0.021, showing more efficient scavenging of {sup 239,240}Pu in the water column and major sedimentation of {sup 137}Cs in the eastern basin. Although areas with water depths of > 2000 m constitute around 40% of the entire Mediterranean basin, the sediments in these regions only contained 2.7% of the {sup 239,240}Pu and 0.95% of the {sup 137}Cs deposited across the Sea in 2000. These data show that the

  3. Low-Level Plutonium Bioassay Measurements at the Lawrence Livermore National Laboratory

    Energy Technology Data Exchange (ETDEWEB)

    Hamilton, T; Brown, T; Hickman, D; Marchetti, A; Williams, R; Kehl, S


    National Institute of Standards and Technology (NIST) has independently verified the accuracy and precision of the AMS detection system for low-level bioassay measurements of plutonium isotopes through participation in an intercomparison exercise whereby performance evaluation samples were prepared in a synthetic urine matrix and submitted to participating laboratories for blind analysis. The results of the analyses were then sent to the NIST to independently evaluate the performance of laboratory participants. At LLNL, the AMS measurements of {sup 239}Pu and {sup 240}Pu met ANSI 13.30 criteria for both precision and accuracy at all sample test levels. Livermore scientists continue to test the performance of the Marshall Islands Plutonium Urinalysis Program by routine blind analysis of externally prepared quality control test samples, and through the rigorous implementation of standardized methods and procedures. Although not addressed directly in the report, AMS measurements show that the urinary excretion of plutonium by selected Marshallese populations fall into a low and reproducible range. Moreover, there appears to be no evidence of small incremental intakes of plutonium associated with resettlement activities - past or present. The improved quality, reliability and detection sensitivity of AMS for low-level plutonium isotope measurements will enable DOE to develop high-quality, baseline urinary excretion data for Marshallese populations, and accurately assess and track potential uptakes of plutonium. associated with resettlement activities and/or from long-term changes in plutonium exposure conditions in the Marshall Islands.

  4. Production of stable isotopes utilizing the plasma separation process (United States)

    Bigelow, T. S.; Tarallo, F. J.; Stevenson, N. R.


    A plasma separation process (PSP) is being operated at Theragenics Corporation's®, Oak Ridge, TN, facility for the enrichment of stable isotopes. The PSP utilizes ion cyclotron mass discrimination to separate isotopes on a relatively large scale. With a few exceptions, nearly any metallic element could be processed with PSP. Output isotope enrichment factor depends on natural abundance and mass separation and can be fairly high in some cases. The Theragenics™ PSP facility is believed to be the only such process currently in operation. This system was developed and formerly operated under the US Department of Energy Advanced Isotope Separation program. Theragenics™ also has a laboratory at the PSP site capable of harvesting the isotopes from the process and a mass spectrometer system for analyzing enrichment and product purity. Since becoming operational in 2002, Theragenics™ has utilized the PSP to separate isotopes of several elements including: dysprosium, erbium, gadolinium, molybdenum and nickel. Currently, Theragenics™ is using the PSP for the separation of 102Pd, which is used as precursor for the production of 103Pd. The 103Pd radioisotope is the active ingredient in TheraSeed®, which is used in the treatment of early stage prostate cancer and being investigated for other medical applications. New industrial, medical and research applications are being investigated for isotopes that can be enriched on the PSP. Pre-enrichment of accelerator or reactor targets offers improved radioisotope production. Theragenics operates 14 cyclotrons for proton activation and has access to HFIR at ORNL for neutron activation of radioisotopes.

  5. Compelling Research Opportunities using Isotopes

    Energy Technology Data Exchange (ETDEWEB)



    Isotopes are vital to the science and technology base of the US economy. Isotopes, both stable and radioactive, are essential tools in the growing science, technology, engineering, and health enterprises of the 21st century. The scientific discoveries and associated advances made as a result of the availability of isotopes today span widely from medicine to biology, physics, chemistry, and a broad range of applications in environmental and material sciences. Isotope issues have become crucial aspects of homeland security. Isotopes are utilized in new resource development, in energy from bio-fuels, petrochemical and nuclear fuels, in drug discovery, health care therapies and diagnostics, in nutrition, in agriculture, and in many other areas. The development and production of isotope products unavailable or difficult to get commercially have been most recently the responsibility of the Department of Energy's Nuclear Energy program. The President's FY09 Budget request proposed the transfer of the Isotope Production program to the Department of Energy's Office of Science in Nuclear Physics and to rename it the National Isotope Production and Application program (NIPA). The transfer has now taken place with the signing of the 2009 appropriations bill. In preparation for this, the Nuclear Science Advisory Committee (NSAC) was requested to establish a standing subcommittee, the NSAC Isotope Subcommittee (NSACI), to advise the DOE Office of Nuclear Physics. The request came in the form of two charges: one, on setting research priorities in the short term for the most compelling opportunities from the vast array of disciplines that develop and use isotopes and two, on making a long term strategic plan for the NIPA program. This is the final report to address charge 1. NSACI membership is comprised of experts from the diverse research communities, industry, production, and homeland security. NSACI discussed research opportunities divided into three areas: (1

  6. Carbon isotope geochemistry and geobiology (United States)

    Desmarais, D.


    Carbon isotope fractionation values were used to understand the history of the biosphere. For example, plankton analyses confirmed that marine extinctions at the end of the Cretaceous period were indeed severe (see Hsu's article in Sundquist and Broeker, 1984). Variations in the isotopic compositions of carbonates and evaporitic sulfates during the Paleozoic reflect the relative abundances of euxinic (anoxic) marine environments and organic deposits from terrestrial flora. The carbon isotopic composition of Precambrian sediments suggest that the enzyme ribulose bisphosphate carboxylase has existed for perhaps 3.5 billion years.

  7. Isotope-edited infrared spectroscopy. (United States)

    Buchner, Ginka S; Kubelka, Jan


    Isotope-edited infrared (IR) spectroscopy is a powerful tool for studying structural and dynamical properties of peptides and proteins with site-specific resolution. Labeling of selected amide carbonyls with (13)C results in detectable sidebands of amide I' vibrations, which provide information about local conformation and/or solvent exposure without structural perturbation to the protein. Incorporation of isotopically labeled amino acids at specific positions is achieved by the chemical synthesis of the studied proteins. We describe the basic procedures for synthesis of (13)C isotopically edited protein samples, experimental IR spectroscopic measurements, and analysis of the site-specific structural changes from the thermal unfolding IR data.

  8. Uranium Isotope Ratios in Modern and Precambrian Soils (United States)

    DeCorte, B.; Planavsky, N.; Wang, X.; Auerbach, D. J.; Knudsen, A. C.


    Uranium isotopes (δ238U values) are an emerging paleoredox proxy that can help to better understand the redox evolution of Earth's surface environment. Recently, uranium isotopes have been used to reconstruct ocean and atmospheric redox conditions (Montoya-Pino et al., 2010; Brennecka et al., 2011; Kendall et al., 2013; Dahl et al., 2014). However, to date, there have not been studies on paleosols, despite that paleosols are, arguably better suited to directly tracking the redox conditions of the atmosphere. Sedimentary δ238U variability requires the formation of the soluble, oxidized form of U, U(VI). The formation of U(VI) is generally thought to require oxygen levels orders of magnitude higher than prebiotic levels. Without significant U mobility, it would have been impossible to develop isotopically distinct pools of uranium in ancient Earth environments. Conversely, an active U redox cycle leads to significant variability in δ238U values. Here we present a temporally and geographically expansive uranium isotope record from paleosols and modern soils to better constrain atmospheric oxygen levels during the Precambrian. Preliminary U isotope measurements of paleosols are unfractionated (relative to igneous rocks), possibly because of limited fractionation during oxidation (e.g., {Wang, 2015 #478}) or insufficient atmospheric oxygen levels to oxidize U(IV)-bearing minerals in the bedrock. Further U isotope measurements of paleosols with comparison to modern soils will resolve this issue.

  9. Heavy element stable isotope ratios: analytical approaches and applications. (United States)

    Tanimizu, Masaharu; Sohrin, Yoshiki; Hirata, Takafumi


    Continuous developments in inorganic mass spectrometry techniques, including a combination of an inductively coupled plasma ion source and a magnetic sector-based mass spectrometer equipped with a multiple-collector array, have revolutionized the precision of isotope ratio measurements, and applications of inorganic mass spectrometry for biochemistry, geochemistry, and marine chemistry are beginning to appear on the horizon. Series of pioneering studies have revealed that natural stable isotope fractionations of many elements heavier than S (e.g., Fe, Cu, Zn, Sr, Ce, Nd, Mo, Cd, W, Tl, and U) are common on Earth, and it had been widely recognized that most physicochemical reactions or biochemical processes induce mass-dependent isotope fractionation. The variations in isotope ratios of the heavy elements can provide new insights into past and present biochemical and geochemical processes. To achieve this, the analytical community is actively solving problems such as spectral interference, mass discrimination drift, chemical separation and purification, and reduction of the contamination of analytes. This article describes data calibration and standardization protocols to allow interlaboratory comparisons or to maintain traceability of data, and basic principles of isotope fractionation in nature, together with high-selectivity and high-yield chemical separation and purification techniques for stable isotope studies.

  10. Arctic Ocean sea ice drift origin derived from artificial radionuclides. (United States)

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


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


    Energy Technology Data Exchange (ETDEWEB)

    Pizzarello, Sandra, E-mail: [Department of Chemistry and Biochemistry, Arizona State University, Tempe, AZ 85018-1604 (United States)


    HCN is ubiquitous in extraterrestrial environments and is central to current theories on the origin of early solar system organic compounds such as amino acids. These compounds, observed in carbonaceous meteorites, were likely important in the origin and/or evolution of early life. As part of our attempts to understand the origin(s) of meteoritic CN{sup –}, we have analyzed the {sup 15}N/{sup 14}N isotopic composition of HCN gas released from water extracts of the Murchison meteorite and found its value to be near those of the terrestrial atmosphere. The findings, when evaluated viz-a-viz molecular abundances and isotopic data of meteoritic organic compounds, suggest that HCN formation could have occurred during the protracted water alteration processes known to have affected the mineralogy of many asteroidal bodies during their solar residence. This was an active synthetic stage, which likely involved simple gasses, organic molecules, their presolar precursors, as well as mineral catalysts and would have lead to the formation of molecules of differing isotopic composition, including some with solar values.

  12. Tracing Waste Water with Li isotopes (United States)

    Millot, R.; Desaulty, A. M.


    The contribution of human activities such as industries, agriculture and various domestic inputs, becomes more and more significant in the chemical composition of the dissolved load of rivers. Human factors act as a supplementary key process. Therefore the mass-balance for the budget of catchments and river basins include anthropogenic disturbances. In the present study, we investigate waste water tracing by the use of Li isotopes in a small river basin near Orléans in France (l'Egoutier, 15 km² and 5 km long). It is well known that Li has strategic importance for numerous industrial applications including its use in the production of batteries for both mobile devices (computers, tablets, smartphones, etc.) and electric vehicles, but also in pharmaceutical formulations. In the present work, we collected river waters samples before and after the release from a waste water treatment plant connected to an hospital. Lithium isotopic compositions are rather homogeneous in river waters with δ7Li values around -0.5‰ ± 1 along the main course of the stream (n=7). The waste water sample is very different from the natural background of the river basin with Li concentration being twice of the values without pollution and significant heavy lithium contribution (δ7Li = +4‰). These preliminary results will be discussed in relation with factors controlling the distribution of Li and its isotopes in this specific system and compared with the release of other metals such as Pb or Zn.

  13. Apparatus and process for separating hydrogen isotopes (United States)

    Heung, Leung K; Sessions, Henry T; Xiao, Xin


    The apparatus and process for separating hydrogen isotopes is provided using dual columns, each column having an opposite hydrogen isotopic effect such that when a hydrogen isotope mixture feedstock is cycled between the two respective columns, two different hydrogen isotopes are separated from the feedstock.

  14. Plutonium and uranium contamination in soils from former nuclear weapon test sites in Australia (United States)

    Child, D. P.; Hotchkis, M. A. C.


    The British government performed a number of nuclear weapon tests on Australian territory from 1952 through to 1963 with the cooperation of the Australian government. Nine fission bombs were detonated in South Australia at Emu Junction and Maralinga, and a further three fission weapons were detonated in the Monte Bello Islands off the coast of Western Australia. A number of soil samples were collected by the Australian Radiation Laboratories in 1972 and 1978 during field surveys at these nuclear weapon test sites. They were analysed by gamma spectrometry and, for a select few samples, by alpha spectrometry to measure the remaining activities of fission products, activation products and weapon materials. We have remeasured a number of these Montebello Islands and Emu Junction soil samples using the ANTARES AMS facility, ANSTO. These samples were analysed for plutonium and uranium isotopic ratios and isotopic concentrations. Very low 240Pu/239Pu ratios were measured at both sites (∼0.05 for Alpha Island and ∼0.02 for Emu Field), substantially below global fallout averages. Well correlated but widely varying 236U and plutonium concentrations were measured across both sites, but 233U did not correlate with these other isotopes and instead showed correlation with distance from ground zero, indicating in situ production in the soils.

  15. Mass-dependent and -independent signature of Fe isotopes in magnetotactic bacteria. (United States)

    Amor, Matthieu; Busigny, Vincent; Louvat, Pascale; Gélabert, Alexandre; Cartigny, Pierre; Durand-Dubief, Mickaël; Ona-Nguema, Georges; Alphandéry, Edouard; Chebbi, Imène; Guyot, François


    Magnetotactic bacteria perform biomineralization of intracellular magnetite (Fe3O4) nanoparticles. Although they may be among the earliest microorganisms capable of biomineralization on Earth, identifying their activity in ancient sedimentary rocks remains challenging because of the lack of a reliable biosignature. We determined Fe isotope fractionations by the magnetotactic bacterium Magnetospirillum magneticum AMB-1. The AMB-1 strain produced magnetite strongly depleted in heavy Fe isotopes, by 1.5 to 2.5 per mil relative to the initial growth medium. Moreover, we observed mass-independent isotope fractionations in (57)Fe during magnetite biomineralization but not in even Fe isotopes ((54)Fe, (56)Fe, and (58)Fe), highlighting a magnetic isotope effect. This Fe isotope anomaly provides a potential biosignature for the identification of magnetite produced by magnetotactic bacteria in the geological record.

  16. Quantification and isotope ratio determination of uranium in particles of environmental samples using isotope dilution thermal ionization mass spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Park, Jong-Ho [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of); Choi, Eun-Ju [Chungnam National University, Daejeon (Korea, Republic of)


    Highly accurate and precise quantitative and qualitative analysis of nuclear materials in environmental samples plays essential roles in monitoring undeclared nuclear activities of corresponding facilities. The former focuses on the quantification of uranium (U) and plutonium (Pu) contained in a whole sample, while the latter enables us to acquire the isotopic ratios, which serve as the crucial basis to trace the nuclear histories of a facility. However, the quantity of nuclear materials in a single-particle has not been acquired from the particle analysis, but has been estimated by the size of the particles. This report is to describe the method developed to determine the quantity and the isotopic ratios of uranium in a micro-particle simultaneously. Complete dissolution of particle-spike mixture by repeated addition of nitric acid on a rhenium filament was performed to ensure the homogeneity of the mixture. Thermal ionization mass spectrometry (TIMS) was utilized to measure the U isotope ratios of the mixture with high accuracy. The isotopic ratios of the uranium in the particle sample were determined by mathematical deconvolution of U isotopic ratios of the mixture. Verification using particles of a certified reference material showed that the newly developed method can be used to quantify and to determine the isotopic ratios of U in a particle simultaneously. The development of a method for simultaneous determination of the quantity and the isotope ratios of uranium contained in particles by isotope dilution thermal ionization mass spectrometry (ID-TIMS) was described. For homogeneity of the mixture of particles and spike, repeated dissolution using nitric acid for five times was performed.

  17. Alignments in the nobelium isotopes

    Institute of Scientific and Technical Information of China (English)

    ZHENG Shi-Zie; XU Fu-Rong; YUAN Cen-Xi; QI Chong


    Total-Routhian-Surface calculations have been performed to investigate the deformation and align-ment properties of the No isotopes. It is found that normal deformed and superdeformed states in these nuclei can coexist at low excitation energies. In neutron-deficient No isotopes, the superdeformed shapes can even become the ground states. Moreover, we plotted the kinematic moments of inertia of the No isotopes, which follow very nicely available experimental data. It is noted that, as the rotational frequency increases, align-ments develop at hω=0.2-0.3 MeV. Our calculations show that the occupation of the vj orbital plays an important role in the alignments of the No isotopes.

  18. Isotopic Changes During Digestion: Protein (United States)

    Tuross, N.


    Nutrient and hydrological inputs traverse a complicated route of pH, enzymatic and cellular processes in digestion in higher animals. The end products of digestion are the starting products for biosynthesis that are often used to interpret past life-ways. Using an artificial gut system, the isotopic changes (dD, d18O, d13C and d15N) of protein are documented. Three separate protein sources are subjected to the conditions, chemical and enzymatic, found in the stomach and upper small intestine with only a small shift in the oxygen isotopic composition of the proteins observed. Middle to lower small intestine parameters produced both greater isotopic effects and significantly lower molecular weight products. The role of the gastric enterocyte and the likely involvement of the internal milieu of this cell in the isotopic composition of amino acids that are transported to the liver are reported.

  19. Isotope-based quantum information

    CERN Document Server

    G Plekhanov, Vladimir


    The present book provides to the main ideas and techniques of the rapid progressing field of quantum information and quantum computation using isotope - mixed materials. It starts with an introduction to the isotope physics and then describes of the isotope - based quantum information and quantum computation. The ability to manipulate and control electron and/or nucleus spin in semiconductor devices provides a new route to expand the capabilities of inorganic semiconductor-based electronics and to design innovative devices with potential application in quantum computing. One of the major challenges towards these objectives is to develop semiconductor-based systems and architectures in which the spatial distribution of spins and their properties can be controlled. For instance, to eliminate electron spin decoherence resulting from hyperfine interaction due to nuclear spin background, isotopically controlled devices are needed (i.e., nuclear spin-depleted). In other emerging concepts, the control of the spatial...

  20. Plutonium and {sup 137}Cs in surface water of the South Pacific Ocean

    Energy Technology Data Exchange (ETDEWEB)

    Hirose, K.; Komura, K. [Meteorological Research Institute, Nagamine 1-1, Tsukuba, Ibaraki 305-0052 (Japan); Low Level Radioactivity Laboratory, Kanazawa University, Wake, Nomi, Ishikawa 923-1224 (Japan); Aoyama, M. [Meteorological Research Institute, Nagamine 1-1, Tsukuba, Ibaraki 305-0052 (Japan); Fukasawa, M. [Japan Agency for Marine-Earth Science and Technology (JAMSTEC), 2-15, Natsushima, Yokosuka 237-0061 (Japan); Kim, C.S. [Korea Institute of Nuclear Safety, Daeduk-Danji Daejeon 305-336 (Korea); Povinec, P.P. [Faculty of Mathematics, Physics and Informatics, Comenius University, Mlynska dolina F1, SK-842 48, Bratislava (Slovakia); Sanchez-Cabeza, J.A. [Marine Environment Laboratories, International Atomic Energy Agency, 4 Quai Antoine 1er, MC98000 (Monaco)


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

  1. Bioavailability of xenobiotics in unsaturated soils – implications for nucleic acid based stable isotope probing (United States)

    The use of stable isotopes to label phylogenetically informative biomolecules (phospholipid fatty acids, DNA, or RNA), typically referred to as stable isotope probing (SIP) has the potential of providing definitive evidence that a detected population is active in a specific process, if that process ...

  2. The 226Ra isotope activities in ground water samples drawn of two wells from the Meridional Pluton, Morungaba Granitoids, eastern Sao Paulo State; Atividades do 226Ra em aguas subterraneas extraidas de dois pocos localizados no pluton meridional, granitoides de Morungaba, SP

    Energy Technology Data Exchange (ETDEWEB)

    Lucas, Fabio de Oliveira; Silva Junior, Mario Goncalves da; Bertolla, Luciana; Ribeiro, Fernando Brenha [Sao Paulo Univ., SP (Brazil). Inst. de Astronomia, Geofisica e Ciencias Atmosfericas. Dept. de Geofisica]. E-mail:


    The 226Ra activities, both in solution and associated with suspended solids, were measured in ground water samples drawn from two wells drilled in a fractured granitic aquifer from the Meridional Pluton, Morungaba Granitoids, eastern Sao Paulo State. The 226Ra isotope activities were measured in a sequence of samples collected about one month apart between March, 2003 and April 2004. The 226Ra activities were measured by radon gas emanometry. The mean dissolved 226Ra activity concentration activities observed in the two wells were (44.9 {+-} 7.1) mBq/L and (51.6 {+-} 8.8) mBq/L. The 226Ra activity of the suspend solids in a liter of these waters varied between (0,6 {+-} 0,1) mBq and (13 {+-} 1) mBq, respectively. (author)

  3. Paleoproxies: Heavy Stable Isotope Perspectives (United States)

    Nagler, T. F.; Hippler, D.; Siebert, C.; Kramers, J. D.


    Recent advances in isotope ratio mass spectrometry, namely multiple collector ICP-MS and refined TIMS techniques, will significantly enhance the ability to measure heavy stable isotope fractionation, which will lead to the development of a wide array of process-identifying (bio)-geochemical tools. Thus far research in this area is not easily assessable to scientists outside the isotope field. This is due to the fact that analyzing heavy stable isotopes does not provide routine numbers which are per se true (the preciser the truer) but is still a highly experimental field. On the other hand resolving earth science problems requires specialists familiar with the environment being studied. So what is in there for paleoceanographers? In a first order approach, relating isotope variations to physical processes is straightforward. A prominent example are oxygen isotope variations with temperature. The total geological signal is of course far more complicated. At low temperatures, heavy stable isotopes variations have been reported for e.g. Ca, Cr, Fe, Cu, Zn, Mo and Tl. Fractionation mechanisms and physical parameters responsible for the observed variations are not yet resolved for most elements. Significant equilibrium isotope fractionation is expected from redox reactions of transition metals. However a difference in coordination number between two coexisting speciations of an element in the same oxidation state can also cause fractionation. Protonation of dissolved Mo is one case currently discussed. For paleoceanography studies, a principal distinction between transition metals essential for life (V to Zn plus Mo) or not will be helpful. In case of the former group, distinction between biogenic and abiogenic isotope fractionation will remain an important issue. For example, abiotic Fe redox reactions result in isotope fractionations indistinguishable in direction and magnitude from microbial effects. Only a combination of different stable isotope systems bears the

  4. NMR studies of isotopically labeled RNA

    Energy Technology Data Exchange (ETDEWEB)

    Pardi, A. [Univ. of Colorado, Boulder, CO (United States)


    In summary, the ability to generate NMR quantities of {sup 15}N and {sup 13}C-labeled RNAs has led to the development of heteronuclear multi-dimensional NMR techniques for simplifying the resonance assignment and structure determination of RNAs. These methods for synthesizing isotopically labeled RNAs are only several years old, and thus there are still relatively few applications of heteronuclear multi-dimensional NMR techniques to RNA. However, given the critical role that RNAs play in cellular function, one can expect to see an increasing number of NMR structural studies of biologically active RNAs.

  5. A Dependence of the Electronuclear System Parameters on the Component Concentration in Fuel MOX

    CERN Document Server

    Barashenkov, V S


    A dependence of the parameters of a electronuclear system with U-Pu fuel MOX on the relative share of plutonium and its isotope ^{240}Pu in fuel is investigated by means of mathematical modelling. As an example, we consider an experimental system with a heat power 10-20 kW designed in Dubna on the basis of the 660 MeV proton phasotron. The 2 % admixture of ^{240}Pu decreases the value of the neutron multiplication coefficient from 0.95 down to 0.90, neutron yield and heat power are diminished almost twice. Such a decrease can be compensated by the increase of Plutonium share in MOX from 25 up to 27 %.

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

    Energy Technology Data Exchange (ETDEWEB)

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


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

  7. IUPAC Periodic Table of Isotopes for the Educational Community

    Energy Technology Data Exchange (ETDEWEB)

    Holden N. E.; Holden,N.E.; Coplen,T.B.


    John Dalton first proposed the concept of atomic weights of the elements in the first decade of the nineteenth century. These atomic weights of the chemical elements were thought of as constants of nature, similar to the speed of light. Dmitri Mendeleev arranged the atomic weights of the elements in ascending order of value and used the systematic variation of their chemical properties to produce his Periodic Table of the Elements in 1869. Measurement of atomic weight values became an important chemical activity for a century and a half. Theodore Richards received a Noble Prize for his work in this area. In 1913, Fredrick Soddy found a species of radium, which had an atomic weight value of 228, compared to the familiar radium gas value of 226. Soddy coined the term 'isotope' (Greek for 'in the same place') to account for this second atomic weight value in the radium position of the Periodic Table. Both of these isotopes of radium are radioactive. Radioactive isotopes are energetically unstable and will decay (disintegrate) over time. The time it takes for one half of a sample of a given radioactive isotope to decay is the half-life of that isotope. In addition to having different atomic weight values, radium-226 and radium-228 also have different half-life values. Around the same time as Soddy's work, J.J. Thomson (discoverer of the electron) identified two stable (non-radioactive) isotopes of the same element, neon. Over the next 40 years, the majority of the known chemical elements were found to have two or more stable (or long-lived radioactive isotopes that contribute significantly to the determination of the atomic weights of the elements).

  8. Degradation and Isotope Source Tracking of Glyphosate and Aminomethylphosphonic Acid. (United States)

    Li, Hui; Joshi, Sunendra R; Jaisi, Deb P


    Glyphosate [N-(phosphonomethyl) glycine], an active ingredient of the herbicide Roundup, and its main metabolite, aminomethylphosphonic acid (AMPA), have been frequently reported to be present in soils and other environments and thus have heightened public concerns on their potential adverse effects. Understanding the fate of these compounds and differentiating them from other naturally occurring compounds require a toolbox of methods that can go beyond conventional methods. Here, we applied individual isotope labeling technique whereby each compound or mineral involved in the glyphosate and AMPA degradation reaction was either synthesized or chosen to have distinct (18)O/(16)O ratios so that the source of incorporated oxygen in the orthophosphate generated and corresponding isotope effect during C-P bond cleavage could be identified. Furthermore, we measured original isotope signatures of a few commercial glyphosate sources to identify their source-specific isotope signatures. Our degradation kinetics results showed that the rate of glyphosate degradation was higher than that of AMPA in all experimental conditions, and both the rate and extent of degradation were lowest under anoxic conditions. Oxygen isotope ratios (δ(18)OP) of orthophosphate generated from glyphosate and AMPA degradation suggested that one external oxygen atom from ambient water, not from dissolved oxygen or mineral, was incorporated into orthophosphate with the other three oxygen atoms inherited from the parent molecule. Interestingly, δ(18)OP values of all commercial glyphosate products studied were found to be the lightest among all orthophosphates known so far. Furthermore, isotope composition was found to be unaffected due to variable degradation kinetics, light/dark, and oxic/anoxic conditions. These results highlight the importance of phosphate oxygen isotope ratios as a nonconventional tool to potentially distinguish glyphosate sources and products from other organophosphorus compounds

  9. Isotope-committee reports 1999; Isotopkommitterapporter 1999

    Energy Technology Data Exchange (ETDEWEB)

    Alvarez, M.; McCarthy, G


    In this compilation the use of radioactive substances in therapies and in vivo examinations during 1999 is presented. For each examination the nuclide, chemical form, way of administration, number of hospitals, total number of examinations, mean activity used, interval of mean activity for the different hospitals and maximum activity is presented. Some examinations may be found at several different places. This is due to diverse routines of reporting and the confused use of old and new classifications. A certain caution is recommended when interpreting the data. Of the compilation it becomes known that during 1999 approximately 109,000 examinations and 2900 therapies were performed. The isotope committees at two hospitals have not presented their statistics.

  10. Isotopes a very short introduction

    CERN Document Server

    Ellam, Rob


    An isotope is a variant form of a chemical element, containing a different number of neutrons in its nucleus. Most elements exist as several isotopes. Many are stable while others are radioactive, and some may only exist fleetingly before decaying into other elements. In this Very Short Introduction, Rob Ellam explains how isotopes have proved enormously important across all the sciences and in archaeology. Radioactive isotopes may be familiar from their use in nuclear weapons, nuclear power, and in medicine, as well as in carbon dating. They have been central to establishing the age of the Earth and the origins of the solar system. Combining previous and new research, Ellam provides an overview of the nature of stable and radioactive isotopes, and considers their wide range of modern applications. ABOUT THE SERIES: The Very Short Introductions series from Oxford University Press contains hundreds of titles in almost every subject area. These pocket-sized books are the perfect way to get ahead in a new subjec...

  11. Exotic Structure of Carbon Isotopes

    CERN Document Server

    Suzuki, T; Hagino, K; Suzuki, Toshio; Sagawa, Hiroyuki; Hagino, Kouichi


    We studied firstly the ground state properties of C-isotopes using a deformed Hartree-Fock (HF)+ BCS model with Skyrme interactions. Shallow deformation minima are found in several neutron$-$rich C-isotopes. It is shown also that the deformation minima appear in both the oblate and the prolate sides in $^{17}$C and $^{19}$C having almost the same binding energies. Secondly, we carried out shell model calculations to study electromagnetic moments and electric dipole transitions of the C-isotopes. We point out the clear configuration dependence of the quadrupole and magnetic moments in the odd C-isotopes, which will be useful to find out the deformations and the spin-parities of the ground states of these nuclei. We studied electric dipole states of C-isotopes focusing on the interplay between low energy Pigmy strength and giant dipole resonances. Reasonable agreement is obtained with available experimental data for the photoreaction cross sections both in the low energy region below $\\hbar \\omega $=14 MeV and ...

  12. Handbook of environmental isotope geochemistry

    Energy Technology Data Exchange (ETDEWEB)

    Baskaran, Mark (ed.) [Wayne State Univ., Detroit, MI (United States). Dept. Geology


    Applications of radioactive and stable isotopes have revolutionized our understanding of the Earth and near-earth surface processes. The utility of the isotopes are ever-increasing and our sole focus is to bring out the applications of these isotopes as tracers and chronometers to a wider audience so that they can be used as powerful tools to solve environmental problems. New developments in this field remain mostly in peer-reviewed journal articles and hence our goal is to synthesize these findings for easy reference for students, faculty, regulators in governmental and non-governmental agencies, and environmental companies. While this volume maintains its rigor in terms of its depth of knowledge and quantitative information, it contains the breadth needed for wide variety problems and applications in the environmental sciences. This volume presents all of the newer and older applications of isotopes pertaining to the environmental problems in one place that is readily accessible to readers. This book not only has the depth and rigor that is needed for academia, but it has the breadth and case studies to illustrate the utility of the isotopes in a wide variety of environments (atmosphere, oceans, lakes, rivers and streams, terrestrial environments, and sub-surface environments) and serves a large audience, from students and researchers, regulators in federal, state and local governments, and environmental companies. (orig.)

  13. Rate of radiocarbon retention onto calcite by isotope exchange

    Energy Technology Data Exchange (ETDEWEB)

    Lempinen, Janne; Lehto, Jukka [Helsinki Univ. (Finland). Lab. of Radiochemistry


    Radiocarbon ({sup 14}C) is a top priority class radionuclide associated with the long-term safety of spent nuclear fuel disposal. Dissolved inorganic radiocarbon can be retained in bedrock via isotope exchange with calcite (CaCO{sub 3}) at solubility equilibrium with groundwater. In the present study, the rate of the isotope exchange process was investigated on synthetic calcite using batch experiments. Experiments were performed in solutions with a calcium concentration of 0.0002-0.1 M, including two synthetic reference groundwaters. The radiocarbon activity in the solutions decreased exponentially as a function of time, thus following first-order kinetics. The rate of isotope exchange was quantified from an exponential fit to the activity data over time. The rate of radiocarbon retention increased as a function of the calcium activity. The isotope exchange half-life was only 4.3 days at calcium ion activities over 0.01. This half-life is very much shorter than the half-life of {sup 14}C or the time scale of groundwater movements; consequently calcite can effectively retain radiocarbon from brackish and saline groundwaters.

  14. Geochemical and isotopic characteristics of groundwater from Velenje Basin, Slovenia (United States)

    Kanduč, Tjaša; Grassa, Fausto; Mori, Nataša; Verbovšek, Timotej


    The Velenje Basin in Slovenia is one of the largest actively mined coal basins in central Europe, producing around 4 million tons of lignite per year. Large amounts of groundwater are extracted from aquifers to facilitate underground mining of coal, and coal seam gas outbursts are a serious mine safety concern. This study analyses the geochemical and isotopic composition of groundwater to provide a general understanding of hydrogeological and geochemical processes in groundwater. Thirty-eight groundwater samples were taken from dewatering objects in the mine and at the surface in years 2014-2015. Groundwater in the Triassic aquifer is dominated by hydrogen carbonate, calcium, magnesium and isotopic composition of dissolved inorganic carbon in the range from -19.3 to -2.8‰ indicating degradation of soil organic matter and dissolution of carbonate minerals. In contrast, groundwater in the Pliocene aquifers is enriched in magnesium, sodium, calcium, potassium, and silicon, and has high alkalinity, with isotopic composition of dissolved inorganic carbon in the range of -14.4 to +4.6‰ . Based on isotopic composition of dissolved inorganic carbon values in all aquifers (Pliocene and Triassic), influencing processes are the dissolution of carbonate minerals and dissolution of organic matter, and additionally methanogenesis in the Pliocene aquifers. Based on the Principal Component Analysis (PCA) we can conclude that following different types of groundwater in Velenje Basin could be distinguished based on geochemical and isotopic data: Triassic aquifers with higher pH and lower conductivity and chloride, Pliocene, Pliocene 1 and Pliocene 2 aquifers with lower pH and higher conductivity and chloride contents, and Pliocene 3 and Pliocene 2, 3 aquifers with the highest pH and lowest conductivity and chloride contents. Major dissolved gas component in groundwater are carbon dioxide, nitrogen and methane. Concentrations of dissolved gases dewatering Triassic strata are low

  15. BOREAS TE-5 Tree Ring and Carbon Isotope Ratio Data (United States)

    Hall, Forrest G. (Editor); Curd, Shelaine (Editor); Ehleriinger, Jim; Brooks, J. Renee; Flanagan, Larry


    The BOREAS TE-5 team collected several data sets to investigate the vegetation-atmosphere CO2 and H2O exchange processes. These data include tree ring widths and cellulose carbon isotope data from coniferous trees collected at the BOREAS NSA and SSA in 1993 and 1994 by the BOREAS TE-5 team. Ring width data are provided for both Picea mariana and Pinus banksiana. The carbon isotope data are provided only for Pinus banksiana. The data are provided in tabular ASCII files. The data files are available on a CD-ROM (see document number 20010000884), or from the Oak Ridge National Laboratory (ORNL) Distributed Active Archive Center (DAAC).

  16. Nitrogen isotopes in Tree-Rings - An approach combining soil biogeochemistry and isotopic long series with statistical modeling (United States)

    Savard, Martine M.; Bégin, Christian; Paré, David; Marion, Joëlle; Laganière, Jérôme; Séguin, Armand; Stefani, Franck; Smirnoff, Anna


    Monitoring atmospheric emissions from industrial centers in North America generally started less than 25 years ago. To compensate for the lack of monitoring, previous investigations have interpreted tree-ring N changes using the known chronology of human activities, without facing the challenge of separating climatic effects from potential anthropogenic impacts. Here we document such an attempt conducted in the oil sands (OS) mining region of Northeastern Alberta, Canada. The reactive nitrogen (Nr)-emitting oil extraction operations began in 1967, but air quality measurements were only initiated in 1997. To investigate if the beginning and intensification of OS operations induced changes in the forest N-cycle, we sampled white spruce (Picea glauca (Moench) Voss) stands located at various distances from the main mining area, and receiving low, but different N deposition. Our approach combines soil biogeochemical and metagenomic characterization with long, well dated, tree-ring isotopic series. To objectively delineate the natural N isotopic behaviour in trees, we have characterized tree-ring N isotope (15N/14N) ratios between 1880 and 2009, used statistical analyses of the isotopic values and local climatic parameters of the pre-mining period to calibrate response functions and project the isotopic responses to climate during the extraction period. During that period, the measured series depart negatively from the projected natural trends. In addition, these long-term negative isotopic trends are better reproduced by multiple-regression models combining climatic parameters with the proxy for regional mining Nr emissions. These negative isotopic trends point towards changes in the forest soil biogeochemical N cycle. The biogeochemical data and ultimate soil mechanisms responsible for such changes will be discussed during the presentation.

  17. Hydrogen isotope separation for fusion power applications

    Energy Technology Data Exchange (ETDEWEB)

    Smith, R., E-mail: [EURATOM/CCFE Fusion Association, Culham Science Centre, Abingdon OX14 3DB (United Kingdom); JET-EFDA, Culham Science Centre, Abingdon OX14 3DB (United Kingdom); Whittaker, D.A.J.; Butler, B.; Hollingsworth, A.; Lawless, R.E.; Lefebvre, X.; Medley, S.A.; Parracho, A.I.; Wakeling, B. [EURATOM/CCFE Fusion Association, Culham Science Centre, Abingdon OX14 3DB (United Kingdom); JET-EFDA, Culham Science Centre, Abingdon OX14 3DB (United Kingdom)


    Highlights: • Summary of the tritium plant, the Active Gas Handling System (AGHS), at JET. • Review of the Water Detritiation System (WDS) under construction. • Design of the new Material Detritiation Facility (MDF). • Review of problems in fusion related to metal/hydrogen system. - Abstract: The invited talk given at MH2014 in Salford ranged over many issues associated with hydrogen isotope separation, fusion machines and the hydrogen/metal systems found in the Joint European Torus (JET) machine located near Oxford. As this sort of talk does not lend itself well to a paper below I have attempted to highlight some of the more pertinent information. After a description of the Active Gas Handling System (AGHS) a brief summary of isotope separation systems is described followed by descriptions of three major projects currently being undertaken by the Tritium Engineering and Science Group (TESG), the upgrade to the Analytical Systems (AN-GC) at the AGH, the construction of a Water Detritiation System (WDS) and a Material Detritiation Facility (MDF). Finally, a review of some of the challenges facing fusion with respect to metal/hydrogen systems is presented.

  18. Medical Isotope Production Analyses In KIPT Neutron Source Facility

    Energy Technology Data Exchange (ETDEWEB)

    Talamo, Alberto [Argonne National Lab. (ANL), Argonne, IL (United States); Gohar, Yousry [Argonne National Lab. (ANL), Argonne, IL (United States)


    Medical isotope production analyses in Kharkov Institute of Physics and Technology (KIPT) neutron source facility were performed to include the details of the irradiation cassette and the self-shielding effect. An updated detailed model of the facility was used for the analyses. The facility consists of an accelerator-driven system (ADS), which has a subcritical assembly using low-enriched uranium fuel elements with a beryllium-graphite reflector. The beryllium assemblies of the reflector have the same outer geometry as the fuel elements, which permits loading the subcritical assembly with different number of fuel elements without impacting the reflector performance. The subcritical assembly is driven by an external neutron source generated from the interaction of 100-kW electron beam with a tungsten target. The facility construction was completed at the end of 2015, and it is planned to start the operation during the year of 2016. It is the first ADS in the world, which has a coolant system for removing the generated fission power. Argonne National Laboratory has developed the design concept and performed extensive design analyses for the facility including its utilization for the production of different radioactive medical isotopes. 99Mo is the parent isotope of 99mTc, which is the most commonly used medical radioactive isotope. Detailed analyses were performed to define the optimal sample irradiation location and the generated activity, for several radioactive medical isotopes, as a function of the irradiation time.

  19. The terrestrial uranium isotope cycle. (United States)

    Andersen, Morten B; Elliott, Tim; Freymuth, Heye; Sims, Kenneth W W; Niu, Yaoling; Kelley, Katherine A


    Changing conditions on the Earth's surface can have a remarkable influence on the composition of its overwhelmingly more massive interior. The global distribution of uranium is a notable example. In early Earth history, the continental crust was enriched in uranium. Yet after the initial rise in atmospheric oxygen, about 2.4 billion years ago, the aqueous mobility of oxidized uranium resulted in its significant transport to the oceans and, ultimately, by means of subduction, back to the mantle. Here we explore the isotopic characteristics of this global uranium cycle. We show that the subducted flux of uranium is isotopically distinct, with high (238)U/(235)U ratios, as a result of alteration processes at the bottom of an oxic ocean. We also find that mid-ocean-ridge basalts (MORBs) have (238)U/(235)U ratios higher than does the bulk Earth, confirming the widespread pollution of the upper mantle with this recycled uranium. Although many ocean island basalts (OIBs) are argued to contain a recycled component, their uranium isotopic compositions do not differ from those of the bulk Earth. Because subducted uranium was probably isotopically unfractionated before full oceanic oxidation, about 600 million years ago, this observation reflects the greater antiquity of OIB sources. Elemental and isotope systematics of uranium in OIBs are strikingly consistent with previous OIB lead model ages, indicating that these mantle reservoirs formed between 2.4 and 1.8 billion years ago. In contrast, the uranium isotopic composition of MORB requires the convective stirring of recycled uranium throughout the upper mantle within the past 600 million years.

  20. Atmospheric circulation controls on the inter-annual variability in precipitation isotope ratio in Japan

    Directory of Open Access Journals (Sweden)

    N. Kurita


    Full Text Available This study explored the primary driver of variations of precipitation isotopes at multiple temporal scales (event, seasonal and inter-annual scales to provide a greater depth of interpretation for isotope proxy records in Japan. A one-year record of the isotopic composition of event-based precipitation at Nagoya in central Japan showed less seasonal variation, but there is large isotopic variability on a storm-to-storm basis. In the summer, southerly flows transport isotopically enriched moisture from subtropical marine regions with the result that the rainfall produced by the subtropical air, or warm rainfall, was relatively enriched in heavy isotopes in comparison with the other rainfall events. In the winter, storm tracks are the dominant driver of storm-to-storm isotopic variation, and relatively lower isotopic values occurred when northerly winds in association with extratropical cyclones passing off the south coast of Japan (Nangan cyclone brings cold precipitation. Using the historical 17 year record of monthly isotopes in precipitation at Tokyo station, we explored if the factors controlling event-scale isotopic variability can account for inter-annual isotopic variability. The relatively higher isotopes in summer precipitation were attributed to the higher contribution of the warm rainfall to the total summer precipitation. On the other hand, year-to-year variation of isotopic values in winter precipitation was negatively correlated with the relative ratio of the Nangan cyclone rainfall to the total winter precipitation. The 17 year precipitation history demonstrates that event-scale isotopic variability related to changes in meridional moisture transport is the primary driver of inter-annual isotopic variability in winter and summer precipitation. The meridional moisture transport to central Japan is likely linked to the activity of the western North Pacific subtropical high in summer and the intensity of the East Asian winter monsoon

  1. Non-linear Isotope Effects

    DEFF Research Database (Denmark)

    Schmidt, Johan Albrecht

    The isotopic fractionation associated with photodissociation of N2O, OCS and CO2, at different altitudes in Earth’s atmosphere, is investigated theoretically using constructed quantum mechanical models of the dissociation processes (i.e. potential energy surfaces and relevant coupling elements...... or moderate, and overall sulfur fractionation in the stratosphere is very weak which does not exclude OCS from being an acceptable background the Stratospheric Sulfate Aerosol layer. (iii) CO2 photolysis in the upper stratosphere and lower mesosphere is highly fractionating in both isotopes, enriching...

  2. Sequential Injection Method for Rapid and Simultaneous Determination of 236U, 237Np, and Pu Isotopes in Seawater

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Steier, Peter;


    An automated analytical method implemented in a novel dual-column tandem sequential injection (SI) system was developed for simultaneous determination of 236U, 237Np, 239Pu, and 240Pu in seawater samples. A combination of TEVA and UTEVA extraction chromatography was exploited to separate and purify...... target analytes, whereupon plutonium and neptunium were simultaneously isolated and purified on TEVA, while uranium was collected on UTEVA. The separation behavior of U, Np, and Pu on TEVA–UTEVA columns was investigated in detail in order to achieve high chemical yields and complete purification...... for the radionuclides of interest. 242Pu was used as a chemical yield tracer for both plutonium and neptunium. 238U was quantified in the sample before the separation for deducing the 236U concentration from the measured 236U/238U atomic ratio in the separated uranium target using accelerator mass spectrometry...

  3. Do Speleothem Stable Isotope Records Contain Hidden Tropical Cyclone Histories? Exploring C-O Isotope Correlation Patterns for Indicators of Tropical Cyclone Masking (United States)

    Frappier, A. E.; Rossington, C.


    The newly-described tropical cyclone masking effect on stable isotope paleohydrological signals in speleothem records arises from the intermittent delivery of large pulses of isotopically distinct tropical cyclone rain. Recent work shows that 18-O depleted tropical cyclone stormwater depresses the δ18O value of speleothem calcite for months to years following a tropical cyclone event, masking the background stable isotope signal of persistent climate variability. Periods of high local storm activity can lead to speleothem calcite paleohydrological signals with significant wet biases on interannual to decadal timescales. Because speleothem carbon isotope ratios are independent of tropical cyclone rainfall, tropical speleothems are known to exhibit moderate C-O isotope covariation over time, periods when C-O isotope covariation breaks down and δ18O values are low may provide a marker for times when tropical cyclone masking is important. If so, existing speleothem stable isotope records from tropical cyclone-prone regions may contain signatures of tropical cyclone masking in the temporal evolution of C-O isotope covariation patterns. We present results from an exploratory analysis of several published speleothem records that are candidates for containing tropical cyclone masking signals. For each speleothem, overall C-O isotope covariation coefficients were calculated, and transient covariation patterns were analyzed using a sliding correlation index, the Covariation of Stable Isotopes (CoSI) index, and Local Correlation (LoCo). Local tropical cyclone historical and paleotempest records are compared and a method is presented to test for the presence of tropical cyclone masking intervals. The implications for speleothem paleoclimatology and paleotempestology are discussed.

  4. The separation of stable isotopes of carbon (United States)

    Oziashvili, E. D.; Egiazarov, A. S.


    The present state of work on the separation of carbon isotopes by diffusion, fractional distillation, chemical isotopic exchange, and the selective excitation and dissociation of molecules in electrical discharges or in the field of laser radiation has been examined. The characteristics of new laboratory and industrial assemblies for separating carbon isotopes have been described. Promising directions of study aimed at developing effective technological processes for separating carbon isotopes have been noted. The bibliography contains 148 references.

  5. Brief review on the development of isotope hydrology in China

    Institute of Scientific and Technical Information of China (English)

    汪集旸; 孙占学


    The development of isotope hydrology in China is briefly reviewed. It includes oxygen and hydrogen isotopes of precipitation, application of isotope hydrological methodologies in solving water resources problems, isotope hydrological studies on brines and salt lake waters, as well as isotope hydrological investigations of thermal waters. The review focuses on isotope hydrology in China during the last two decades.

  6. Substitution of stable isotopes in Chlorella (United States)

    Flaumenhaft, E.; Katz, J. J.; Uphaus, R. A.


    Replacement of biologically important isotopes in the alga Chlorella by corresponding heavier stable isotopes produces increasingly greater deviations from the normal cell size and changes the quality and distribution of certain cellular components. The usefulness of isotopically altered organisms increases interest in the study of such permuted organisms.

  7. Dry phase reactor for generating medical isotopes (United States)

    Mackie, Thomas Rockwell; Heltemes, Thad Alexander


    An apparatus for generating medical isotopes provides for the irradiation of dry-phase, granular uranium compounds which are then dissolved in a solvent for separation of the medical isotope from the irradiated compound. Once the medical isotope is removed, the dissolved compound may be reconstituted in dry granular form for repeated irradiation.

  8. High-resolution (SIMS) versus bulk sulfur isotope patterns of pyrite in Proterozoic microbialites with diverse mat textures (United States)

    Gomes, M. L.; Fike, D. A.; Bergmann, K.; Knoll, A. H.


    Sulfur (S) isotope signatures of sedimentary pyrite preserved in marine rocks provide a rich suite of information about changes in biogeochemical cycling associated with the evolution of microbial metabolisms and oxygenation of Earth surface environments. Conventionally, these S isotope records are based on bulk rock measurements. Yet, in modern microbial mat environments, S isotope compositions of sulfide can vary by up to 40‰ over a spatial range of ~ 1 mm. Similar ranges of S isotope variability have been found in Archean pyrite grains using both Secondary Ion Mass Spectrometry and other micro-analytical techniques. These micron-scale patterns have been linked to changes in rates of microbial sulfate reduction and/or sulfide oxidation, isotopic distillation of the sulfate reservoir due to microbial sulfate reduction, and post-depositional alteration. Fine-scale mapping of S isotope compositions of pyrite can thus be used to differentiate primary environmental signals from post-depositional overprinting - improving our understanding of both. Here, we examine micron-scale S isotope patterns of pyrite in microbialites from the Mesoproterozoic-Neoproterozoic Sukhaya Tunguska Formation and Neoproterozoic Draken Formation in order to explore S isotope variability associated with different mat textures and pyrite grain morphologies. A primary goal is to link modern observations of how sulfide spatial isotope distributions reflect active microbial communities present at given depths in the mats to ancient processes driving fine-sale pyrite variability in microbialites. We find large (up to 60‰) S isotope variability within a spatial range of less than 2.5cm. The micron-scale S isotope measurements converge around the S isotope composition of pyrite extracted from bulk samples of the same microbialites. These micron-scale pyrite S isotope patterns have the potential to reveal important information about ancient biogeochemical cycling in Proterozoic mat environments

  9. Bayesian stable isotope mixing models (United States)

    In this paper we review recent advances in Stable Isotope Mixing Models (SIMMs) and place them into an over-arching Bayesian statistical framework which allows for several useful extensions. SIMMs are used to quantify the proportional contributions of various sources to a mixtur...

  10. Research Progress of Isotope Technology

    Institute of Scientific and Technical Information of China (English)

    Department; of; Isotope


    Radioactive isotope is one of the origins of nonnuclear power technology.In the 12th Five Year Plan period,CIAE made breakthrough progresses on several important fields such as research and development of preparation of radioactive nuclides,preparation of radioactive source and study of radiopharmaceuticals relied on different financial support,successfully

  11. Operation of Electromagnetic Isotope Separator

    Institute of Scientific and Technical Information of China (English)

    MI; Ya-jing


    In 2015,we mainly completed the installation of the electromagnetic isotope separator comprehensive technical transformation projects,including the work of installation,debugging,commissioning and acceptance.In June 30,2015,according to the schedule requirements,the project

  12. Isotope Harvesting Opportunities at FRIB (United States)

    Morrissey, David


    The fragmentation of fast heavy ion beams now at the National Superconducting Cyclotron Laboratory (NSCL) and in the future at the Facility for Rare Isotope Beams (FRIB) under construction produce an unprecedentedly broad spectrum of radionuclides but only a small fraction are used in the on-line rare-isotope program. Projectile fragmentation facilities provide an electromagnetically purified beam of a single projectile fragment for nuclear physics experiments ranging from low energy astrophysics, through nuclear structure studies, to probing fundamental symmetries. By augmenting the NSCL and FRIB production facilities with complimentary collection and purification of discarded ions, called isotope harvesting with chemical purification, many other nuclides will become available for off-line experiments in parallel with the primary experiment. A growing user community has established a list of key target isotopes and is working with the FRIB design team to allow inclusion of necessary equipment in the future. An overview of the possibilities and the techniques will be presented in this talk. Supported by Office of Science, US DOE and Michigan State University.

  13. The Behaviour of Chromium Isotopes during the Oxidative Weathering of Ultramafic Rocks

    DEFF Research Database (Denmark)

    Paulukat, Cora Stefanie; Døssing, Lasse Nørbye; Mondal, Sisir K.;

    Ore Group in the southern Singhbhum Craton (Orissa, India)[3]. A modern weathering profile was logged in an active open cast chromite mine (Sukinda valley). The Cr isotope data of samples from the weathering profile are fractionaed. While the least weathered horizons at the base of the profile reflect......The chromium isotope system has been proven to be a redox-sensitve proxy in ancient and modern environmental studies (e.g. [1], [2]). In this study we investigated Cr isotope fractionation during soil formation from Archean (3.1-3.3 Ga) ultramafic rocks, intruded into metamorphic rocks of the Iron...... are characterised by a Cr loss of up to 74 %. These data are consistent with the findings of Crowe et al. [2] who also studied the effects of weathering of ultramafic rocks in Indonesia on the Cr isotope system. These authors demonstrate that oxidation of Cr(III) to Cr(VI) in the soils is accompanied by isotopic...

  14. Stable isotopes of transition and post-transition metals as tracers in environmental studies (United States)

    Bullen, Tomas D.; Baskaran, Mark


    The transition and post-transition metals, which include the elements in Groups 3–12 of the Periodic Table, have a broad range of geological and biological roles as well as industrial applications and thus are widespread in the environment. Interdisciplinary research over the past decade has resulted in a broad understanding of the isotope systematics of this important group of elements and revealed largely unexpected variability in isotope composition for natural materials. Significant kinetic and equilibrium isotope fractionation has been observed for redox sensitive metals such as iron, chromium, copper, molybdenum and mercury, and for metals that are not redox sensitive in nature such as cadmium and zinc. In the environmental sciences, the isotopes are increasingly being used to understand important issues such as tracing of metal contaminant sources and fates, unraveling metal redox cycles, deciphering metal nutrient pathways and cycles, and developing isotope biosignatures that can indicate the role of biological activity in ancient and modern planetary systems.

  15. Calcium isotope analysis by mass spectrometry. (United States)

    Boulyga, Sergei F


    The variations in the isotopic composition of calcium caused by fractionation in heterogeneous systems and by nuclear reactions can provide insight into numerous biological, geological, and cosmic processes, and therefore isotopic analysis finds a wide spectrum of applications in cosmo- and geochemistry, paleoclimatic, nutritional, and biomedical studies. The measurement of calcium isotopic abundances in natural samples has challenged the analysts for more than three decades. Practically all Ca isotopes suffer from significant isobaric interferences, whereas low-abundant isotopes can be particularly affected by neighboring major isotopes. The extent of natural variations of stable isotopes appears to be relatively limited, and highly precise techniques are required to resolve isotopic effects. Isotope fractionation during sample preparation and measurements and instrumental mass bias can significantly exceed small isotope abundance variations in samples, which have to be investigated. Not surprisingly, a TIMS procedure developed by Russell et al. (Russell et al., 1978. Geochim Cosmochim Acta 42: 1075-1090) for Ca isotope measurements was considered as revolutionary for isotopic measurements in general, and that approach is used nowadays (with small modifications) for practically all isotopic systems and with different mass spectrometric techniques. Nevertheless, despite several decades of calcium research and corresponding development of mass spectrometers, the available precision and accuracy is still not always sufficient to achieve the challenging goals. The present article discusses figures of merits of presently used analytical methods and instrumentation, and attempts to critically assess their limitations. In Sections 2 and 3, mass spectrometric methods applied to precise stable isotope analysis and to the determination of (41)Ca are described. Section 4 contains a short summary of selected applications, and includes tracer experiments and the potential use

  16. A global Ge isotope budget (United States)

    Baronas, J. Jotautas; Hammond, Douglas E.; McManus, James; Wheat, C. Geoffrey; Siebert, Christopher


    We present measurements of Ge isotope composition and ancillary data for samples of river water, low- and high-temperature hydrothermal fluids, and seawater. The dissolved δ74Ge composition of analyzed rivers ranges from 2.0 to 5.6‰, which is significantly heavier than previously determined values for silicate rocks (δ74Ge = 0.4-0.7‰, Escoube et al., Geostand. Geoanal. Res., 36(2), 2012) from which dissolved Ge is primarily derived. An observed negative correlation between riverine Ge/Si and δ74Ge signatures suggests that the primary δ74Ge fractionation mechanism during rock weathering is the preferential incorporation of light isotopes into secondary weathering products. High temperature (>150 °C) hydrothermal fluids analyzed in this study have δ74Ge of 0.7-1.6‰, most likely fractionated during fluid equilibration with quartz in the reaction zone. Low temperature (25-63 °C) hydrothermal fluids are heavier (δ74Ge between 2.9‰ and 4.1‰) and most likely fractionated during Ge precipitation with hydrothermal clays. Seawater from the open ocean has a δ74Gesw value of 3.2 ± 0.4‰, and is indistinguishable among the different ocean basins at the current level of precision. This value should be regulated over time by the isotopic balance of Ge sources and sinks, and a new compilation of these fluxes is presented, along with their estimated isotopic compositions. Assuming steady-state, non-opal Ge sequestration during sediment authigenesis likely involves isotopic fractionation Δ74Gesolid-solution that is -0.6 ± 1.8‰.

  17. Modelling stable water isotopes: Status and perspectives

    Directory of Open Access Journals (Sweden)

    Werner M.


    Full Text Available Modelling of stable water isotopes H2 18O and HDO within various parts of the Earth’s hydrological cycle has clearly improved our understanding of the interplay between climatic variations and related isotope fractionation processes. In this article key principles and major research results of stable water isotope modelling studies are described. Emphasis is put on research work using explicit isotope diagnostics within general circulation models as this highly complex model setup bears many resemblances with studies using simpler isotope modelling approaches.

  18. Stable Isotope Measurements of Carbon Dioxide, Methane, and Hydrogen Sulfide Gas Using Frequency Modulation Spectroscopy (United States)

    Nowak-Lovato, K.


    Seepage from enhanced oil recovery, carbon storage, and natural gas sites can emit trace gases such as carbon dioxide, methane, and hydrogen sulfide. Trace gas emission at these locations demonstrate unique light stable isotope signatures that provide information to enable source identification of the material. Light stable isotope detection through surface monitoring, offers the ability to distinguish between trace gases emitted from sources such as, biological (fertilizers and wastes), mineral (coal or seams), or liquid organic systems (oil and gas reservoirs). To make light stable isotope measurements, we employ the ultra-sensitive technique, frequency modulation spectroscopy (FMS). FMS is an absorption technique with sensitivity enhancements approximately 100-1000x more than standard absorption spectroscopy with the advantage of providing stable isotope signature information. We have developed an integrated in situ (point source) system that measures carbon dioxide, methane and hydrogen sulfide with isotopic resolution and enhanced sensitivity. The in situ instrument involves the continuous collection of air and records the stable isotope ratio for the gas being detected. We have included in-line flask collection points to obtain gas samples for validation of isotopic concentrations using our in-house isotope ratio mass spectroscopy (IRMS). We present calibration curves for each species addressed above to demonstrate the sensitivity and accuracy of the system. We also show field deployment data demonstrating the capabilities of the system in making live dynamic measurements from an active source.

  19. Heterogeneous distribution of Zn stable isotopes in mice and applications to medical sciences (United States)

    Moynier, F.; Fujii, T.; Shaw, A.; Le Borgne, M.


    Zinc is required for the function of more than 300 enzymes involved in many metabolic pathways, and is a vital micronutrient for living organisms. To investigate if Zn isotopes could be used to better understand metal homeostasis, as well as a biomarker for diseases, we assessed the distribution of natural Zn isotopes in various mouse tissues. We found that, with respect to Zn isotopes, most mouse organs are isotopically distinct and that the total range of variation within one mouse encompasses the variations observed in the Earth's crust. Therefore, biological activity must have a major impact on the distribution of Zn isotopes in inorganic materials. The most striking aspect of the data is that red blood cells and bones are enriched by ~0.5 per mil in 66Zn relative to 64Zn when compared to serum, and up to ~1 per mil when compared to the brain and liver. This fractionation is well explained by the equilibrium distribution of isotopes between different bonding environments of Zn in different organs. Differences in gender and genetic background did not appear to affect the isotopic distribution of Zn. Together, these results suggest that potential use of Zn isotopes as a tracer for dietary Zn, and for detecting disturbances in Zn metabolism due to pathological conditions.

  20. Heavy atom isotope effects on enzymatic reactions (United States)

    Paneth, Piotr


    The theory of isotope effects, which has proved to be extremely useful in providing geometrical details of transition states in a variety of chemical reactions, has recently found an application in studies of enzyme-catalyzed reactions. These reactions are multistep in nature with few steps being partially rate-limiting, thus interpretation of these isotope effects is more complex. The theoretical framework of heavy-atom isotope effects on enzymatic reactions is critically analyzed on the basis of recent results of: carbon kinetic isotope effects on carbonic anhydrase and catalytic antibodies; multiple carbon, deuterium isotope effects on reactions catalyzed by formate decarboxylase; oxygen isotope effects on binding processes in reactions catalyzed by pyruvate kinase; and equilibrium oxygen isotope effect on binding an inhibitor to lactate dehydrogenase. The advantages and disadvantages of reaction complexity in learning details of formal and molecular mechanisms are discussed in the examples of reactions catalyzed by phosphoenolpyruvate carboxylase, orotidine decarboxylase and glutamine synthetase.

  1. Zinc isotopic compositions of breast cancer tissue. (United States)

    Larner, Fiona; Woodley, Laura N; Shousha, Sami; Moyes, Ashley; Humphreys-Williams, Emma; Strekopytov, Stanislav; Halliday, Alex N; Rehkämper, Mark; Coombes, R Charles


    An early diagnostic biomarker for breast cancer is essential to improve outcome. High precision isotopic analysis, originating in Earth sciences, can detect very small shifts in metal pathways. For the first time, the natural intrinsic Zn isotopic compositions of various tissues in breast cancer patients and controls were determined. Breast cancer tumours were found to have a significantly lighter Zn isotopic composition than the blood, serum and healthy breast tissue in both groups. The Zn isotopic lightness in tumours suggests that sulphur rich metallothionein dominates the isotopic selectivity of a breast tissue cell, rather than Zn-specific proteins. This reveals a possible mechanism of Zn delivery to Zn-sequestering vesicles by metallothionein, and is supported by a similar signature observed in the copper isotopic compositions of one breast cancer patient. This change in intrinsic isotopic compositions due to cancer has the potential to provide a novel early biomarker for breast cancer.

  2. Measuring SNM Isotopic Distributions using FRAM

    Energy Technology Data Exchange (ETDEWEB)

    Geist, William H. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)


    The first group of slides provides background information on the isotopic composition of plutonium. It is shown that 240Pu is the critical isotope in neutron coincidence/multiplicity counting. Next, response function analysis to determine isotopic composition is discussed. The isotopic composition can be determined by measuring the net peak counts from each isotope and then taking the ratio of the counts for each isotope relative to the total counts for the element. Then FRAM (Fixed energy Response function Analysis with Multiple efficiencies) is explained. FRAM can control data acquisition, automatically analyze newly acquired data, analyze previously acquired data, provide information on the quality of the analysis, and facilitate analysis in unusual situations (non-standard energy calibrations, gamma rays from non-SNM isotopes, poor spectra (within limits)).

  3. Isotope hydrology of catchment basins: lithogenic and cosmogenic isotopic systems

    Energy Technology Data Exchange (ETDEWEB)

    Nimz, G. J., LLNL


    A variety of physical processes affect solute concentrations within catchment waters. The isotopic compositions of the solutes can indicate which processes have determined the observed concentrations. These processes together constitute the physical history of the water. Many solutes in natural waters are derived from the interaction between the water and the rock and/or soil within the system - these are termed `lithogenic` solutes. The isotopic compositions of these solutes provide information regarding rock-water interactions. Many other solutes have their isotopic compositions determined both within and outside of the catchment - i.e., in addition to being derived from catchment rock and soil, they are solutes that are also transported into the catchment. Important members of this group include solutes that have isotopic compositions produced by atomic particle interactions with other nuclides. The source of the atomic particles can be cosmic radiation (producing `cosmogenic` nuclides in the atmosphere and land surface), anthropogenic nuclear reactions (producing `thermonuclear` nuclides), or radioactive and fission decay of naturally-occurring elements, principally {sup 238}U (producing `in-situ` lithogenic nuclides in the deep subsurface). Current language usage often combines all of the atomic particle-produced nuclides under the heading `cosmogenic nuclides`, and for simplicity we will often follow that usage here, although always indicating which variety is being discussed. This paper addresses the processes that affect the lithogenic and cosmogenic solute concentrations in catchment waters, and how the isotopic compositions of the solutes can be used in integrative ways to identify these processes, thereby revealing the physical history of the water within a catchment system. The concept of a `system` is important in catchment hydrology. A catchment is the smallest landscape unit that can both participate in all of the aspects of the hydrologic cycle and

  4. Effective technique for numerical kinetics calculations in a system of anharmonic oscillators. Application to study of the influence of the isotopic composition of molecules on the properties of a carbon monoxide active medium

    Energy Technology Data Exchange (ETDEWEB)

    Bunkin, S.B.; Islamov, R.S.; Konev, Y.B.; Kochetov, I.V.


    A technique is described for numerical analysis of kinetic processes in a system of anharmonic oscillators, based on using implicit numerical integration and replacement of derivatives by means of backward differentiation expressions. A comparison is made with calculations by the Runge--Kutta method, and it is shown that the computer time is reduced by a factor of more than 10 when the backward differentiation method is used. The influence of the natural isotopic composition of carbon monoxide molecules on the gain and lasing properties is investigated and shown to be only slight.

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

    Energy Technology Data Exchange (ETDEWEB)

    Le Roux, Gael, E-mail: gael.leroux@ensat.f [Institut de Radioprotection et Surete Nucleaire, DEI/SESURE, Laboratoires d' Etudes Radioecologiques en milieu Continental et Marin, CEN Cadarache Bat. 153 BP 3, 13115 St Paul lez Durance (France); Duffa, Celine; Vray, Francoise; Renaud, Philippe [Institut de Radioprotection et Surete Nucleaire, DEI/SESURE, Laboratoires d' Etudes Radioecologiques en milieu Continental et Marin, CEN Cadarache Bat. 153 BP 3, 13115 St Paul lez Durance (France)


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

  6. Plutonium as a tracer for soil erosion assessment in northeast China. (United States)

    Xu, Yihong; Qiao, Jixin; Pan, Shaoming; Hou, Xiaolin; Roos, Per; Cao, Liguo


    Soil erosion is one of the most serious environmental and agricultural problems faced by human society. Assessing intensity is an important issue for controlling soil erosion and improving eco-environmental quality. The suitability of the application of plutonium (Pu) as a tracer for soil erosion assessment in northeast China was investigated by comparing with that of 137Cs. Here we build on preliminary work, in which we investigated the potential of Pu as a soil erosion tracer by sampling additional reference sites and potential erosive sites, along the Liaodong Bay region in northeast China, for Pu isotopes and 137Cs. 240Pu/239Pu atomic ratios in all samples were approximately 0.18, which indicated that the dominant source of Pu was the global fallout. Pu showed very similar distribution patterns to those of 137Cs at both uncultivated and cultivated sites. 239+240Pu concentrations in all uncultivated soil cores followed an exponential decline with soil depth, whereas at cultivated sites, Pu was homogenously distributed in plow horizons. Factors such as planted crop types, as well as methods and frequencies of irrigation and tillage were suggested to influence the distribution of radionuclides in cultivated land. The baseline inventories of 239+240Pu and 137Cs were 88.4 and 1688 Bq m(-2) respectively. Soil erosion rates estimated by 239+240Pu tracing method were consistent with those obtained by the 137Cs method, confirming that Pu is an effective tracer with a similar tracing behavior to that of 137Cs for soil erosion assessment.

  7. High-resolution quadruple sulfur isotope analyses of 3.2 Ga pyrite from the Barberton Greenstone Belt in South Africa reveal distinct environmental controls on sulfide isotopic arrays

    NARCIS (Netherlands)

    Roerdink, D.L.; Mason, P.R.D.; Whitehouse, M.J.; Reimer, T.


    Multiple sulfur isotopes in Paleoarchean pyrite record valuable information on atmospheric processes and emerging microbial activity in the early sulfur cycle. Here, we report quadruple sulfur isotope data (32S, 33S, 34S, 36S) analyzed by secondary ion mass spectrometry from pyrite in a 3.26–3.23 Ga

  8. Production of medical radioactive isotopes using KIPT electron driven subcritical facility

    Energy Technology Data Exchange (ETDEWEB)

    Talamo, Alberto [Nuclear Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (United States)], E-mail:; Gohar, Yousry [Nuclear Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (United States)


    Kharkov Institute of Physics and Technology (KIPT) of Ukraine in collaboration with Argonne National Laboratory (ANL) has a plan to construct an electron accelerator driven subcritical assembly. One of the facility objectives is the production of medical radioactive isotopes. This paper presents the ANL collaborative work performed for characterizing the facility performance for producing medical radioactive isotopes. First, a preliminary assessment was performed without including the self-shielding effect of the irradiated samples. Then, more detailed investigation was carried out including the self-shielding effect, which defined the sample size and location for producing each medical isotope. In the first part, the reaction rates were calculated as the multiplication of the cross section with the unperturbed neutron flux of the facility. Over fifty isotopes have been considered and all transmutation channels are used including (n, {gamma}), (n, 2n), (n, p), and ({gamma}, n). In the second part, the parent isotopes with high reaction rate were explicitly modeled in the calculations. Four irradiation locations were considered in the analyses to study the medical isotope production rate. The results show the self-shielding effect not only reduces the specific activity but it also changes the irradiation location that maximizes the specific activity. The axial and radial distributions of the parent capture rates have been examined to define the irradiation sample size of each parent isotope.

  9. Interstellar Isotopes: Prospects with ALMA (United States)

    Charnley Steven B.


    Cold molecular clouds are natural environments for the enrichment of interstellar molecules in the heavy isotopes of H, C, N and O. Anomalously fractionated isotopic material is found in many primitive Solar System objects, such as meteorites and comets, that may trace interstellar matter that was incorporated into the Solar Nebula without undergoing significant processing. Models of the fractionation chemistry of H, C, N and O in dense molecular clouds, particularly in cores where substantial freeze-out of molecules on to dust has occurred, make several predictions that can be tested in the near future by molecular line observations. The range of fractionation ratios expected in different interstellar molecules will be discussed and the capabilities of ALMA for testing these models (e.g. in observing doubly-substituted isotopologues) will be outlined.

  10. Natural fractionation of uranium isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Noordmann, Janine


    The topic of this thesis was the investigation of U (n({sup 238}U) / n({sup 235}U)) isotope variations in nature with a focus on samples (1) that represent the continental crust and its weathering products (i.e. granites, shales and river water) (2) that represent products of hydrothermal alteration on mid-ocean ridges (i.e. altered basalts, carbonate veins and hydrothermal water) and (3) from restricted euxinic basins (i.e. from the water column and respective sediments). The overall goal was to explore the environmental conditions and unravel the mechanisms that fractionate the two most abundant U isotopes, n({sup 238}U) and n({sup 235}U), on Earth.

  11. Variations in the chemical and stable isotope composition of carbon and sulfur species during organic-rich sediment alteration: An experimental and theoretical study of hydrothermal activity at guaymas basin, gulf of california (United States)

    Seewald, Jeffrey S.; Seyfried, William E., Jr.; Shanks, Wayne C., III


    Organic-rich diatomaceous ooze was reacted with seawater and a Na-Ca-K-Cl fluid of seawater chlorinity at 325-400°C, 400-500 bars, and fluid/sediment mass ratios of 1.56-2.35 to constrain factors regulating the abundance and stable isotope composition of C and S species during hydrothermal alteration of sediment from Guaymas Basin, Gulf of California. Alteration of inorganic and organic sedimentary components resulted in extensive exchange reactions, the release of abundant H 2S, CO 2, CH 4, and C organic, to solution, and recrystallization of the sediment to an assemblage containing albitic plagioclase, quartz, pyrrhotite, and calcite. The δ 34S cdt values of dissolved H 2S varied from -10.9 to +4.3‰ during seawater-sediment interaction at 325 and 400°C and from -16.5 to -9.0‰ during Na-Ca-K-Cl fluid-sediment interaction at 325 and 375°C. In the absence of seawater SO 4, H 2S is derived from both the transformation of pyrite to pyrrhotite and S released during the degradation of organic matter. In the presence of seawater SO 4, reduction of SO 4 contributes directly to H 2S production. Sedimentary organic matter acts as the reducing agent during pyrite and SO 4 reduction. Requisite acidity for the reduction of SO 4 is provided by Mg fixation during early-stage sediment alteration and by albite and calcite formation in Mg-free solutions. Organically derived CH 4 was characterized by δ 13C pdb values ranging between -20.8 and -23.1‰, whereas δ 13C pdb values for dissolved C organic ranged between -14.8 and -17.7%. Mass balance calculations indicate that δ13C values for organically derived CO 2 were ≥ - 14.8%. Residual solid sedimentary organic C showed small (≤ 0.7‰) depletions in 13C relative to the starting sediment. The experimental results are consistent with the isotopic and chemical composition of natural hydrothermal fluids and minerals at Guaymas Basin and permit us to better constrain sources and sinks for C and S species in subseafloor

  12. Variations in the chemical and stable isotope composition of carbon and sulfur species during organic-rich sediment alteration: An experimental and theoretical study of hydrothermal activity at guaymas basin, gulf of california (United States)

    Seewald, Jeffrey S.; Seyfried, W.E.; Shanks, Wayne C.


    Organic-rich diatomaceous ooze was reacted with seawater and a Na-Ca-K-Cl fluid of seawater chlorinity at 325-400??C, 400-500 bars, and fluid/sediment mass ratios of 1.56-2.35 to constrain factors regulating the abundance and stable isotope composition of C and S species during hydrothermal alteration of sediment from Guaymas Basin, Gulf of California. Alteration of inorganic and organic sedimentary components resulted in extensive exchange reactions, the release of abundant H2S, CO2, CH4, and Corganic, to solution, and recrystallization of the sediment to an assemblage containing albitic plagioclase, quartz, pyrrhotite, and calcite. The ??34Scdt values of dissolved H2S varied from -10.9 to +4.3??? during seawater-sediment interaction at 325 and 400??C and from -16.5 to -9.0??? during Na-Ca-K-Cl fluid-sediment interaction at 325 and 375??C. In the absence of seawater SO4, H2S is derived from both the transformation of pyrite to pyrrhotite and S released during the degradation of organic matter. In the presence of seawater SO4, reduction of SO4 contributes directly to H2S production. Sedimentary organic matter acts as the reducing agent during pyrite and SO4 reduction. Requisite acidity for the reduction of SO4 is provided by Mg fixation during early-stage sediment alteration and by albite and calcite formation in Mg-free solutions. Organically derived CH4 was characterized by ??13Cpdb values ranging between -20.8 and -23.1???, whereas ??13Cpdb values for dissolved Corganic ranged between -14.8 and -17.7%. Mass balance calculations indicate that ??13C values for organically derived CO2 were ??? - 14.8%. Residual solid sedimentary organic C showed small (??? 0.7???) depletions in 13C relative to the starting sediment. The experimental results are consistent with the isotopic and chemical composition of natural hydrothermal fluids and minerals at Guaymas Basin and permit us to better constrain sources and sinks for C and S species in subseafloor hydrothermal systems

  13. Variation of carbon isotope fractionation in hydrogenotrophic methanogenic microbial cultures and environmental samples at different energy status

    NARCIS (Netherlands)

    Penning, H.; Plugge, C.M.; Galand, P.E.; Conrad, R.


    Methane is a major product of anaerobic degradation of organic matter and an important greenhouse gas. Its stable carbon isotope composition can be used to reveal active methanogenic pathways, if associated isotope fractionation factors are known. To clarify the causes that lead to the wide variatio

  14. Quantification of in Situ Biodegradation Rate Constants Using a Novel Combined Isotope Approach (United States)

    Blum, P.; Sültenfuß, J.; Martus, P.


    Numerous studies have shown the enormous potential of the compound-specific isotope analysis (CSIA) for studying the biodegradation of organic compounds such as monoaromatic hydrocarbons (BTEX), polyaromatic hydrocarbons (PAH), chlorinated solvents and other organic contaminants and environmental transformation mechanisms in groundwater. In addition, two-dimensional isotope analysis such as carbon and hydrogen have been successfully studied indicating the potential to also investigate site-specific reaction mechanisms. The main objective of the current study however is to quantify real effective in situ biodegradation rate constants in a coal-tar contaminated aquifer by combining compound-specific isotope analysis (CSIA) and tracer-based (3H-3He) ground-water dating (TGD). Hence, groundwater samples are used to determine groundwater residence times, and carbon and hydrogen stable isotopes are analyzed for selected BTEX and PAH. The results of the hydrogen stable isotopes surprisingly indicate no isotope fractionation and therefore no biodegradation. In contrast, for stable carbon isotopes of selected BTEX such as o-xylene and toluene, isotope shifts are detected indicating active biodegradation under sulfate-reducing conditions. These and previous results of stable carbon isotopes show that only for o-xylene a clear evidence for biodegradation is possible for the studied site. Nevertheless, in combining these results with the groundwater residence times, which range between 1 year for the shallow wells (20 m below surface) and 41 years for the deeper wells (40 m below surface), it is feasible to effectively determine in situ biodegradation rate constants for o-xylene. Conversely, the outcome also evidently demonstrate the major limitations of the novel combined isotope approach for a successful implementation of monitored natural attenuation (MNA) at such field sites.

  15. Thermal Neutron Capture onto the Stable Tungsten Isotopes

    Directory of Open Access Journals (Sweden)

    Nichols A.


    Full Text Available Thermal neutron-capture measurements of the stable tungsten isotopes have been carried out using the guided thermal-neutron beam at the Budapest Reactor. Prompt singles spectra were collected and analyzed using the HYPERMET γ-ray analysis software package for the compound tungsten systems 183W, 184W, and 187W, prepared from isotopically-enriched samples of 182W, 183W, and 186W, respectively. These new data provide both confirmation and new insights into the decay schemes and structure of the tungsten isotopes reported in the Evaluated Gamma-ray Activation File based upon previous elemental analysis. The experimental data have also been compared to Monte Carlo simulations of γ-ray emission following the thermal neutron-capture process using the statistical-decay code DICEBOX. Together, the experimental cross sections and modeledfeeding contribution from the quasi continuum, have been used to determine the total radiative thermal neutron-capture cross sections for the tungsten isotopes and provide improved decay-scheme information for the structural- and neutron-data libraries.

  16. Inner radiation belt source of helium and heavy hydrogen isotopes (United States)

    Leonov, A. A.; Galper, A. M.; Koldashov, S. V.; Mikhailov, V. V.; Casolino, M.; Picozza, P.; Sparvoli, R.

    Nuclear interactions between inner zone protons and atoms in the upper atmosphere provide the main source of energetic H and He isotopes nuclei in the radiation belt. This paper reports on the specified calculations of these isotope intensities using various inner zone proton intensity models (AP-8 and SAMPEX/PET PSB97), the atmosphere drift-averaged composition and density model MSIS-90, and cross-sections of the interaction processes from the GNASH nuclear model code. To calculate drift-averaged densities and energy losses of secondaries, the particles were tracked in the geomagnetic field (modelled through IGRF-95) by integrating numerically the equation of the motion. The calculations take into account the kinematics of nuclear interactions along the whole trajectory of trapped proton. The comparison with new data obtained from the experiments on board RESURS-04 and MITA satellites and with data from SAMPEX and CRRES satellites taken during different phases of solar activity shows that the upper atmosphere is a sufficient source for inner zone helium and heavy hydrogen isotopes. The calculation results are energy spectra and angular distributions of light nuclear isotopes in the inner radiation belt that may be used to develop helium inner radiation belt model and to evaluate their contribution to SEU (single event upset) rates.

  17. Artificial radionuclides in the Northern European Marine Environment. Distribution of radiocaesium, plutonium and americium in sea water and sediments in 1995

    Energy Technology Data Exchange (ETDEWEB)

    Groettheim, Siri


    This study considers the distribution of radiocaesium, plutonium and americium in the northern marine environment. The highest radiocaesium activity in sea water was observed in Skagerrak, 26 Bq/m{sub 3}, and in surface sediments in the Norwegian Sea, 60 Bq/kg. These enhanced levels were related to Chernobyl. The highest 239,240Pu activity in surface water was measured in the western North Sea, 66 mBq/m{sub 3}. In sea water, sub-surface maxima were observed at several locations with an 239,240Pu activity up to 160 mBq/m{sub 3}, and were related to Sellafield. With the exception to the North Sea, surface sediments reflected Pu from global fallout from weapons tests only. (author)

  18. Nitrogen and Oxygen Isotopes of Low-Level Nitrate in Groundwater For Environmental Forensics (United States)

    Wang, Y.


    Sources of nitrate in water from human activities include fertilizers, animal feedlots, septic systems, wastewater treatment lagoons, animal wastes, industrial wastes and food processing wastes. Nitrogen and Oxygen isotopic analysis of nitrate in groundwater is essential to source identification and environmental forensics as nitrate from different sources carry distinctly different N and O isotopic compositions. Nitrate is extracted from groundwater samples and converted into AgNO3 using ion exchange techniques. The purified AgNO3 is then broken down into N2 and CO for N and O isotopic measurement. Since nitrate concentrations in natural ground waters are usually less than 2 mg/L, however, such method has been limited by minimum sample size it requires, in liters, which is highly nitrate concentration dependent. Here we report a TurboVap- Denitrifier method for N and O isotopic measurement of low-level dissolved nitrate, based on sample evaporation and isotopic analysis of nitrous oxide generated from nitrate by denitrifying bacteria that lack N2O- reductase activity. For most groundwater samples with mg/L-level of nitrate direct injection of water samples in mLs is applied. The volume of sample is adjusted according to its nitrate concentration to achieve a final sample size optimal for the system. For water samples with ug/L-level of nitrate, nitrate is highly concentrated using a TurboVap evaporator, followed by isotopic measurement with Denitrifier method. Benefits of TurboVap- Denitrifier method include high sensitivity and better precision in both isotopic data. This method applies to both freshwater and seawater. The analyses of isotopic reference materials in nitrate-free de-ionized water and seawater are included as method controls to correct for any blank effects. The isotopic data from groundwater and ocean profiles demonstrate the consistency of the data produced by the TurboVap-Denitrifier method.

  19. Pb isotopes during mingling and melting

    DEFF Research Database (Denmark)

    Waight, Tod Earle; Lesher, Charles E.


    Pb isotopic data are presented for hybrid rocks formed by mingling between mantle-derived tholeiitic magma of the Eocene Miki Fjord macrodike (East Greenland) and melt derived from the adjacent Precambrian basement. Bulk mixing and AFC processes between end-members readily identified in the field...... fail to model the Pb isotope systematics. Selective contamination during diffusional exchange, which can explain the complex Sr and Nd isotope compositions of the hybrid rocks (Blichert-Toft et al., 1992), cannot fully account for the variability of the Pb isotopic data using the identified crustal end......-members. The crustal anatectic end-member, although similar in Sr and Nd isotope composition, has a markedly different Pb isotopic composition than its source gneiss. The differences are consistent with preferential incorporation of radiogenic Pb from accessory phases such as metamict zircon or loosely-bound Pb from...

  20. Isotopic constraints of mantle derived carbonatitic melts from Calatrava, Spain (United States)

    Humphreys, E. R.; Bailey, K.; Hawkesworth, C. J.; Wall, F.; Avanzinelli, R.


    Carbonatite volcanism is typically associated both spatially and temporally with alkaline, ultramafic volcanism (Woolley & Church, 2005). Recent discoveries in Calatrava, Spain illustrate the activity of carbonatite in the source melts of leucitite volcanism. Melilitite pyroclastic lapilli tuffs also show a clear association with volcanic carbonate. Carbonatitic activity has been shown to initiate at depths greater than 100km (Humphreys et al., 2010) despite a maximum estimate of lithospheric thickness of 80km. The presence of aragonite and abundant mantle xenoliths in many deposits are clear indication of the rapid emplacement rates of such magmas. Carbonatitic activity in the source of the leucitite melts is indicated by carbonate inclusions within olivine xenocrysts and the presence of occasional carbonatite lenses. The composition of lead and strontium isotope ratios in the bulk rock, and spatially resolved analysis of carbonate from the groundmass and from inclusions demonstrates a genetic affinity between the inclusions and the related bulk rock composition. Lead and strontium isotopic analysis suggest that such melts do not represent the composition of convecting asthenospheric mantle. 87Sr/86Sr (0.7055-0.7068) values are higher than those of MORB and most OIB. Lead isotope ratios show a trend displaced to higher 207Pb/204Pb relative to MORB and OIB. Carbonate inclusions have less radiogenic lead values than the more radiogenic bulk rocks. Our data indicate that carbonatitic activity in the mantle is intrinsic in the generation of the leucitite lava. However, petrographic and isotopic evidence suggest a complex melt history. Olivine xenocrysts are not in equilibrium with the host leucitite, despite inclusions within olivine showing an isotopic affinity to the bulk rock. We suggest that in this example, alkaline magmatism was induced by the presence of CO2 in the mantle source. Isotopic evidence shows that the mantle producing such melts was not

  1. Research Progress of Series of Uranium Isotope Ratios Measured by AMS

    Institute of Scientific and Technical Information of China (English)

    LIN; De-yu; WANG; Chen; HUANG; Guo-rui; DONG; Ke-jun; HE; Ming; RUAN; Xiang-dong; WU; Shao-yong; ZHAO; Yong-gang; LI; Li-li; DOU; Liang; XIE; Lin-bo; WANG; Xiao-bo; YANG; Xu-ran; WANG; Xiao-ming; LAN; Xiao-xi; JIANG; Shan


    <正>The nuclear safeguards system which is used to monitor compliance with the Nuclear Non-proliferation Treaty relies to a significant degree on the analysis of environmental samples. Undeclared nuclear activities can be detected through determination of the isotopic ratios of uranium and plutonium in such samples. It is necessary to be able to measure the full suite of uranium isotopes (234U,

  2. Normalization of oxygen and hydrogen isotope data (United States)

    Coplen, T.B.


    To resolve confusion due to expression of isotopic data from different laboratories on non-corresponding scales, oxygen isotope analyses of all substances can be expressed relative to VSMOW or VPDB (Vienna Peedee belemnite) on scales normalized such that the ??18O of SLAP is -55.5% relative to VSMOW. H3+ contribution in hydrogen isotope ratio analysis can be easily determined using two gaseous reference samples that differ greatly in deuterium content. ?? 1988.

  3. Silicon isotopes: from cosmos to benthos


    Chakrabarti, Ramananda


    Silicon is the second most abundant element on the Earth and one of the more abundant elements in our Solar System. Variations in the relative abundance of the stable isotopes of Si (Si isotope fractionation) in different natural reservoirs, both terrestrial (surface and deep Earth) as well as extra-terrestrial (e.g. meteorites, lunar samples), are a powerful tracer of present and past processes involving abiotic as well as biotic systems. The versatility of the Si isotope tracer is reflected...

  4. Production of radioactive isotopes from stable isotopes, for nuclear medicine; A partir d`isotopes stables, production d`isotopes radioactifs pour la medecine nucleaire

    Energy Technology Data Exchange (ETDEWEB)

    Bourdoiseau, M. [CEA Centre d`Etudes de Saclay, 91 - Gif-sur-Yvette (France). Office des Rayonnements Ionisants


    Around 15 radioactive isotopes only are used for nuclear medicine diagnosis (kinetics or preferential fixation in the body); characteristics of these {gamma} and {beta}-minus emitters are presented: period, energy, production mode (isotopic filiation, fission product separation, cyclotron, reactor); details are given on applications, production mode, properties and consumption of various isotopes: Technetium 99m, Thallium 201, Iodine 123, Indium 111, Gallium 67, Rhenium 186, Erbium 169, Yttrium 90, Iron 59, Chromium 51, Krypton 81m. 1 tab.

  5. Quantitative microbial ecology through stable isotope probing. (United States)

    Hungate, Bruce A; Mau, Rebecca L; Schwartz, Egbert; Caporaso, J Gregory; Dijkstra, Paul; van Gestel, Natasja; Koch, Benjamin J; Liu, Cindy M; McHugh, Theresa A; Marks, Jane C; Morrissey, Ember M; Price, Lance B


    Bacteria grow and transform elements at different rates, and as yet, quantifying this variation in the environment is difficult. Determining isotope enrichment with fine taxonomic resolution after exposure to isotope tracers could help, but there are few suitable techniques. We propose a modification to stable isotope probing (SIP) that enables the isotopic composition of DNA from individual bacterial taxa after exposure to isotope tracers to be determined. In our modification, after isopycnic centrifugation, DNA is collected in multiple density fractions, and each fraction is sequenced separately. Taxon-specific density curves are produced for labeled and nonlabeled treatments, from which the shift in density for each individual taxon in response to isotope labeling is calculated. Expressing each taxon's density shift relative to that taxon's density measured without isotope enrichment accounts for the influence of nucleic acid composition on density and isolates the influence of isotope tracer assimilation. The shift in density translates quantitatively to isotopic enrichment. Because this revision to SIP allows quantitative measurements of isotope enrichment, we propose to call it quantitative stable isotope probing (qSIP). We demonstrated qSIP using soil incubations, in which soil bacteria exhibited strong taxonomic variations in (18)O and (13)C composition after exposure to [(18)O]water or [(13)C]glucose. The addition of glucose increased the assimilation of (18)O into DNA from [(18)O]water. However, the increase in (18)O assimilation was greater than expected based on utilization of glucose-derived carbon alone, because the addition of glucose indirectly stimulated bacteria to utilize other substrates for growth. This example illustrates the benefit of a quantitative approach to stable isotope probing.

  6. The trend of stable isotope separation

    Energy Technology Data Exchange (ETDEWEB)

    Yonekawa, Shigeru [Power Reactor and Nuclear Fuel Development Corp., Kamisaibara, Okayama (Japan). Ningyo Toge Works; Aoki, Eiji; Yato, Yumio


    Recently, stable isotopes are used in the field of medical science, nuclear physics, environmental science and agriculture. This report reviews the present status of stable isotope enrichment in ORNL, Urenco, Russia and PNC. Further the utilization method of the stable isotopes in the field of medical science, nuclear power and material science are described, and the application possibility of Laser separation method and Gas Centrifuge method are estimated. There are many overseas actual results of stable isotope separation with Gas Centrifuge method, therefore this method is possible enough in principle. (author).

  7. Scattering lengths of calcium and barium isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Dammalapati, U.; Willmann, L.; Knoop, S. [Kernfysisch Versneller Instituut (KVI), University of Groningen, Zernikelaan 25, 9747 AA Groningen (Netherlands); LaserLaB Vrije Universiteit, De Boelelaan 1081, 1081 HV Amsterdam (Netherlands)


    We have calculated the s-wave scattering length of all the even isotopes of calcium (Ca) and barium (Ba) in order to investigate the prospect of Bose-Einstein condensation (BEC). For Ca we have used an accurate molecular potential based on detailed spectroscopic data. Our calculations show that Ca does not provide other isotopes alternative to the recently Bose condensed {sup 40}Ca that suffers strong losses because of a very large scattering length. For Ba we show by using a model potential that the even isotopes cover a broad range of scattering lengths, opening the possibility of BEC for at least one of the isotopes.

  8. A solvent extraction technique for the isotopic measurement of dissolved copper in seawater

    Energy Technology Data Exchange (ETDEWEB)

    Thompson, Claire M., E-mail:; Ellwood, Michael J., E-mail:; Wille, Martin, E-mail:


    Graphical abstract: -- Highlights: •A new sample preparation method for seawater copper isotopic analysis (δ{sup 65}Cu). •Solvent-extraction was used to pre-concentrate metals from seawater samples. •Anion-exchange was used to purify copper from the metal-rich extract. •δ{sup 65}Cu was measured in the north Tasman Sea. •Seawater δ{sup 65}Cu may be linked to marine biological activity. -- Abstract: Stable copper (Cu) isotope geochemistry provides a new perspective for investigating and understanding Cu speciation and biogeochemical Cu cycling in seawater. In this work, sample preparation for isotopic analysis employed solvent-extraction with amino pyrollidine dithiocarbamate/diethyl dithiocarbamate (APDC/DDC), coupled with a nitric acid back-extraction, to concentrate Cu from seawater. This was followed by Cu-purification using anion-exchange. This straightforward technique is high yielding and fractionation free for Cu and allows precise measurement of the seawater Cu isotopic composition using multi-collector inductively coupled plasma mass-spectrometry. A deep-sea profile measured in the oligotrophic north Tasman Sea shows fractionation in the Cu isotopic signature in the photic zone but is relatively homogenised at depth. A minima in the Cu isotopic profile correlates with the chlorophyll a maximum at the site. These results indicate that a range of processes are likely to fractionate stable Cu isotopes in seawater.

  9. Iron isotope fractionation during Fe uptake and translocation in alpine plants. (United States)

    Kiczka, Mirjam; Wiederhold, Jan G; Kraemer, Stephan M; Bourdon, Bernard; Kretzschmar, Ruben


    The potential of stable Fe isotopes as a tracer for the biogeochemical Fe cycle depends on the understanding and quantification of the fractionation processes involved. Iron uptake and cycling by plants may influence Fe speciation in soils. Here, we determined the Fe isotopic composition of different plant parts including the complete root system of three alpine plant species (Oxyria digyna, Rumex scutatus, Agrostis gigantea) in a granitic glacier forefield, which allowed us, for the first time, to distinguish between uptake and in-plant fractionation processes. The overall range of fractionation was 4.5 per thousand in delta(56)Fe. Mass balance calculations demonstrated that fractionation toward lighter Fe isotopic composition occurred in two steps during uptake: (1) before active uptake, probably during mineral dissolution and (2) during selective uptake of Fe at the plasma membrane with an enrichment factor of -1.0 to -1.7 per thousand for all three species. Iron isotopes were further fractionated during remobilization from old into new plant tissue, which changed the isotopic composition of leaves and flowers over the season. This study demonstrates the potential of Fe isotopes as a new tool in plant nutrition studies but also reveals challenges for the future application of Fe isotope signatures in soil-plant environments.

  10. Plutonium and americium inventories in atmospheric fallout and sediment cores from Blelham Tarn, Cumbria (UK)

    Energy Technology Data Exchange (ETDEWEB)

    Michel, H. E-mail:; Barci-Funel, G.; Dalmasso, J.; Ardisson, G.; Appleby, P.G.; Haworth, E.; El-Daoushy, F


    The objective of this paper is to report on the results of a study of {sup 238}Pu, {sup 239+240}Pu and {sup 241}Am inventories onto Blelham Tarn in Cumbria (UK). The atmospheric fallout inventory was obtained by analysing soil cores and the results are in good agreement with the literature: 101 Bq m{sup -2} for {sup 239+240}Pu; 4.5 Bq m{sup -2} for {sup 238}Pu and 37 Bq m{sup -2} for {sup 241}Am. The sediment core inventory for the whole lake is compared to the atmospheric fallout inventory. The sediment activity is 60-80% higher than the estimated fallout activity, showing a catchment area contribution and in particular the stream input.

  11. Plutonium and americium inventories in atmospheric fallout and sediment cores from Blelham Tarn, Cumbria (UK). (United States)

    Michel, H; Barci-Funel, G; Dalmasso, J; Ardisson, G; Appleby, P G; Haworth, E; El-Daoushy, F


    The objective of this paper is to report on the results of a study of 238Pu, 239 + 240Pu and 241Am inventories onto Blelham Tarn in Cumbria (UK). The atmospheric fallout inventory was obtained by analysing soil cores and the results are in good agreement with the literature: 101 Bq m(-2) for 239 + 240Pu; 4.5 Bq m(-2) for 238Pu and 37 Bq m(-2) for 241Am. The sediment core inventory for the whole lake is compared to the atmospheric fallout inventory. The sediment activity is 60-80% higher than the estimated fallout activity, showing a catchment area contribution and in particular the stream input.

  12. Controlling factors of rainwater and water vapor isotopes at Bangalore, India: Constraints from observations in 2013 Indian monsoon (United States)

    Rahul, P.; Ghosh, Prosenjit; Bhattacharya, S. K.; Yoshimura, Kei


    Isotopic ratios of rainwaters are believed to decrease with the amount of rainfall. However, analyses of the isotopic composition of rainwater and water vapor samples collected from Bangalore during the monsoon period of 2013 fail to show any simple relationship with the local meteorological parameters whereas show good correlation with the regional integrated convective activity. The correlation is particularly high when the averaging is done over the preceding 8 to 15 days, showing the influence of mixing or residence time scale of atmospheric moisture. This observation emphasizes the role of regional atmospheric circulation driving the isotopic values. A comparison between observed isotope ratios in water vapor and rainwater with Isotope-enabled Global Spectral Model shows discrepancies between the two. The observed values are relatively enriched, indicating a systematic bias in the model values. The higher observed values suggest underestimation of the evaporation in the model, which we estimate to be about 28 ± 15% on average. Simultaneous analyses of rainwater and water vapor isotopic composition again show definitive presence of raindrop evaporation (31 ± 14%). We also documented a distinct pattern of isotopic variation in six samples collected at Bangalore due to mixing of vapor from a cyclonic system in close proximity that originated from the Bay of Bengal. It seems that large-scale isotopic depletion occurs during cyclones caused by Rayleigh fractionation due to massive rainout. These results demonstrate the power of rainwater and water vapor isotope monitoring to elucidate the genesis and dynamics of water recycling within synoptic-scale monsoon systems.

  13. The Application of Methane Clumped Isotope Measurements to Determine the Source of Large Methane Seeps in Alaskan Lakes (United States)

    Douglas, P. M.; Stolper, D. A.; Eiler, J. M.; Sessions, A. L.; Walter Anthony, K. M.


    Natural methane emissions from the Arctic present an important potential feedback to global warming. Arctic methane emissions may come from either active microbial sources or from deep fossil reservoirs released by the thawing of permafrost and melting of glaciers. It is often difficult to distinguish between and quantify contributions from these methane sources based on stable isotope data. Analyses of methane clumped isotopes (isotopologues with two or more rare isotopes such as 13CH3D) can complement traditional stable isotope-based classifications of methane sources. This is because clumped isotope abundances (for isotopically equilibrated systems) are a function of temperature and can be used to identify pathways of methane generation. Additionally, distinctive effects of mixing on clumped isotope abundances make this analysis valuable for determining the origins of mixed gasses. We find large variability in clumped isotope compositions of methane from seeps in several lakes, including thermokarst lakes, across Alaska. At Lake Sukok in northern Alaska we observe the emission of dominantly thermogenic methane, with a formation temperature of at least 100° C. At several other lakes we find evidence for mixing between thermogenic methane and biogenic methane that forms in low-temperature isotopic equilibrium. For example, at Eyak Lake in southeastern Alaska, analysis of three methane samples results in a distinctive isotopic mixing line between a high-temperature end-member that formed between 100-170° C, and a biogenic end-member that formed in isotopic equilibrium between 0-20° C. In this respect, biogenic methane in these lakes resembles observations from marine gas seeps, oil degradation, and sub-surface aquifers. Interestingly, at Goldstream Lake in interior Alaska, methane with strongly depleted clumped-isotope abundances, indicative of disequilibrium gas formation, is found, similar to observations from methanogen culture experiments.

  14. Modeling the carbon isotope composition of bivalve shells (Invited) (United States)

    Romanek, C.


    fractionation relations dictate that shell carbonate should be preferentially enriched in C-13 by 3 to 5 per mill (from 30° to 0°C) compared to EPF at a pH of 7.5. Anomalous positive excursions are rarely, if ever, observed in shell carbonate and they have yet to be associated with growth cessation markers in bivalves. The most likely explanation for the lack of anomalous positive values is that the percentage of metabolic carbon increases in EPF when bivalves experience stressful condition. This influx of metabolic carbon is balanced to a measureable extent by the enhanced fractionation of carbon isotopes during shell deposition from EPF at relatively low pH. These two processes may be combined in a quantitative model to extract a historical record of metabolic activity from the carbon isotope profiles of bivalve shells.

  15. CO Isotopes in Planetary Nebulae


    Balser, Dana S.; McMullin, Joseph P.; Wilson, T. L.


    Standard stellar evolution theory is inconsistent with the observed isotopic carbon ratio, 12C/13C, in evolved stars. This theory is also inconsistent with the 3He/H abundance ratios observed in Galactic HII regions, when combined with chemical evolution theory. These discrepancies have been attributed to an extra, non-standard mixing which further processes material during the RGB and should lower both the 12C/13C and 3He/H abundance ratios for stars with masses < 2 solar masses. Measurement...

  16. Silicon isotope fractionation during magmatic differentiation (United States)

    Savage, Paul S.; Georg, R. Bastian; Williams, Helen M.; Burton, Kevin W.; Halliday, Alex N.


    The Si isotopic composition of Earth's mantle is thought to be homogeneous (δ 30Si = -0.29 ± 0.08‰, 2 s.d.) and not greatly affected by partial melting and recycling. Previous analyses of evolved igneous material indicate that such rocks are isotopically heavy relative to the mantle. To understand this variation, it is necessary to investigate the degree of Si isotopic fractionation that takes place during magmatic differentiation. Here we report Si isotopic compositions of lavas from Hekla volcano, Iceland, which has formed in a region devoid of old, geochemically diverse crust. We show that Si isotopic composition varies linearly as a function of silica content, with more differentiated rocks possessing heavier isotopic compositions. Data for samples from the Afar Rift Zone, as well as various igneous USGS standards are collinear with the Hekla trend, providing evidence of a fundamental relationship between magmatic differentiation and Si isotopes. The effect of fractionation has been tested by studying cumulates from the Skaergaard Complex, which show that olivine and pyroxene are isotopically light, and plagioclase heavy, relative to the Si isotopic composition of the Earth's mantle. Therefore, Si isotopes can be utilised to model the competing effects of mafic and felsic mineral fractionation in evolving silicate liquids and cumulates. At an average SiO 2 content of ˜60 wt.%, the predicted δ 30Si value of the continental crust that should result from magmatic fractionation alone is -0.23 ± 0.05‰ (2 s.e.), barely heavier than the mantle. This is, at most, a maximum estimate, as this does not take into account weathered material whose formation drives the products toward lighter δ 30Si values. Mass balance calculations suggest that removal of continental crust of this composition from the upper mantle will not affect the Si isotopic composition of the mantle.

  17. Exploring the isotopic niche: isotopic variance, physiological incorporation, and the temporal dynamics of foraging

    Directory of Open Access Journals (Sweden)

    Justin Douglas Yeakel


    Full Text Available Consumer foraging behaviors are dynamic, changing in response to prey availability, seasonality, competition, and even the consumer's physiological state. The isotopic composition of a consumer is a product of these factors as well as the isotopic `landscape' of its prey, i.e. the isotopic mixing space. Stable isotope mixing models are used to back-calculate the most likely proportional contribution of a set of prey to a consumer's diet based on their respective isotopic distributions, however they are disconnected from ecological process. Here we build a mechanistic framework that links the ecological and physiological processes of an individual consumer to the isotopic distribution that describes its diet, and ultimately to the isotopic composition of its own tissues, defined as its `isotopic niche’. By coupling these processes, we systematically investigate under what conditions the isotopic niche of a consumer changes as a function of both the geometric properties of its mixing space and foraging strategies that may be static or dynamic over time. Results of our derivations reveal general insight into the conditions impacting isotopic niche width as a function of consumer specialization on prey, as well as the consumer's ability to transition between diets over time. We show analytically that moderate specialization on isotopically unique prey can serve to maximize a consumer's isotopic niche width, while temporally dynamic diets will tend to result in peak isotopic variance during dietary transitions. We demonstrate the relevance of our theoretical findings by examining a marine system composed of nine invertebrate species commonly consumed by sea otters. In general, our analytical framework highlights the complex interplay of mixing space geometry and consumer dietary behavior in driving expansion and contraction of the isotopic niche. Because this approach is established on ecological mechanism, it is well-suited for enhancing the

  18. Study of medical isotope production facility stack emissions and noble gas isotopic signature using automatic gamma-spectra analysis platform (United States)

    Zhang, Weihua; Hoffmann, Emmy; Ungar, Kurt; Dolinar, George; Miley, Harry; Mekarski, Pawel; Schrom, Brian; Hoffman, Ian; Lawrie, Ryan; Loosz, Tom


    The nuclear industry emissions of the four CTBT (Comprehensive Nuclear-Test-Ban Treaty) relevant radioxenon isotopes are unavoidably detected by the IMS along with possible treaty violations. Another civil source of radioxenon emissions which contributes to the global background is radiopharmaceutical production companies. To better understand the source terms of these background emissions, a joint project between HC, ANSTO, PNNL and CRL was formed to install real-time detection systems to support 135Xe, 133Xe, 131mXe and 133mXe measurements at the ANSTO and CRL 99Mo production facility stacks as well as the CANDU (CANada Deuterium Uranium) primary coolant monitoring system at CRL. At each site, high resolution gamma spectra were collected every 15 minutes using a HPGe detector to continuously monitor a bypass feed from the stack or CANDU primary coolant system as it passed through a sampling cell. HC also conducted atmospheric monitoring for radioxenon at approximately 200 km distant from CRL. A program was written to transfer each spectrum into a text file format suitable for the automatic gamma-spectra analysis platform and then email the file to a server. Once the email was received by the server, it was automatically analysed with the gamma-spectrum software UniSampo/Shaman to perform radionuclide identification and activity calculation for a large number of gamma-spectra in a short period of time (less than 10 seconds per spectrum). The results of nuclide activity together with other spectrum parameters were saved into the Linssi database. This database contains a large amount of radionuclide information which is a valuable resource for the analysis of radionuclide distribution within the noble gas fission product emissions. The results could be useful to identify the specific mechanisms of the activity release. The isotopic signatures of the various radioxenon species can be determined as a function of release time. Comparison of 133mXe and 133Xe activity


    Institute of Scientific and Technical Information of China (English)


    1 A New Therapeutic Agent for Radiation Synovectomy: Preparation of 166Ho-EDTMP-HA Bai Hongsheng Jin Xiaohai Du Jin Wang Fan Chen Daming Fan Hongqiang Cheng Zhen In order to treat the patient with inflammatory synovial disease, HA particle is labeled with 166Ho by EDTMP under the condition of pH6.0-8.0 and vibration time 15 min, its labeling efficiency is more than 98%, the size of particle is mainly in the range of 2-5 μm. The absorbed capacity is 5 mg Ho per 1g HA. Study on stability of 166Ho-EDTMP-HA in vitro shows that loss of 166Ho is less than 2% for166Ho-EDTMP-HA incubated 72 h in the 0.9% saline and 1% BSA solution at 37 ℃ .Biodistribution in vivo and extra articular leakage are investigated following injection of 166Ho-EDTMP-HA into knee of normal rabbits. The experimental results show that the extra leakage of 166Ho-EDTMP-HA is 0.32% at 48 h post-injection, most of 166Ho radioactivity leaked from the knee joint is excreted in the urine. 99% of 166Ho radioactivity is retained in the knee joint of rabbits. Thereby 166Ho-EDTMP-HA, as a new therapeutical agent of radiation synovectomy, had a value of further clinical study.

  20. Methane isotope records from Antarctic firn air (United States)

    Sowers, T. A.; Battle, M.


    The earth's climate is directly influenced by changes in the atmospheric loading of trace "greenhouse" gases. Methane is an important greenhouse gas whose atmospheric concentration has doubled over the last century as a result of various anthropogenic activities. Understanding the methane cycle in the recent past is a compelling scientific problem because increasing methane levels in the modern atmosphere will contribute to predicted future warming. The only source of air that allows us to study the long-term cycles of these gases is found in the trapped gases in ice cores and the interstitial pore spaces in firn from the central portions of Greenland and Antarctica. Firn air samples, retrieved from the South Pole in 1995 and 2001, were analyzed for δ13CH4. In December of 2005, another suite of firn air samples was recovered from the new US deep coring site located along the west Antarctic divide (WAIS D) which were analyzed for both δ13C and δ D of CH4. In general, replicate flasks were sampled from each depth from two separate drillings each year. The precision of the δ13C and δ D analyses is generally better than ± 0.2‰ and 2‰, respectively, with surface values in good agreement with NOAA (INSTAAR) biweekly flask measurements from South Pole. In all cases, δ13C and δD values decrease gradually with depth below the convective zone. However, these isotopes and CH4 mixing ratios decline sharply below the "lock-in" depth. The measured firn air profiles are primarily the result of three factors. First, tropospheric changes drive compositional changes in the near-surface convective layer that are subsequently mixed downward due to bulk air-movement within the shallow firn. Secondly, gases are mixed below the convective zone solely by molecular diffusion, leading to the gradual downward propagation of the compositional changes in the convective layer. Finally, differential gravitational settling causes the heavier atmospheric constituents (both elemental

  1. Isotope Program Report June FY2016

    Energy Technology Data Exchange (ETDEWEB)

    Lewis, Jr, Benjamin E. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Egle, Brian [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)


    Isotope Program Monthly Highlights are briefly described. These include data on isotopes shipped, updates on equipment fabrication and testing, a potential new approach for nondestructive measurement of the amount of Cf-252 deposited on a surface, and efforts to recover and purify uranium-234 obtained from old PuBe sources.

  2. Advanced Mass Spectrometers for Hydrogen Isotope Analyses

    Energy Technology Data Exchange (ETDEWEB)

    Chastagner, P.


    This report is a summary of the results of a joint Savannah River Laboratory (SRL) - Savannah River Plant (SRP) ''Hydrogen Isotope Mass Spectrometer Evaluation Program''. The program was undertaken to evaluate two prototype hydrogen isotope mass spectrometers and obtain sufficient data to permit SRP personnel to specify the mass spectrometers to replace obsolete instruments.

  3. Applications of stable isotopes in clinical pharmacology

    NARCIS (Netherlands)

    Schellekens, Reinout C A; Stellaard, Frans; Woerdenbag, Herman J; Frijlink, Henderik W; Kosterink, Jos G W


    This review aims to present an overview of the application of stable isotope technology in clinical pharmacology. Three main categories of stable isotope technology can be distinguished in clinical pharmacology. Firstly, it is applied in the assessment of drug pharmacology to determine the pharmacok

  4. Magnesium isotope geochemistry in arc volcanism (United States)

    Teng, Fang-Zhen; Hu, Yan; Chauvel, Catherine


    Incorporation of subducted slab in arc volcanism plays an important role in producing the geochemical and isotopic variations in arc lavas. The mechanism and process by which the slab materials are incorporated, however, are still uncertain. Here, we report, to our knowledge, the first set of Mg isotopic data for a suite of arc lava samples from Martinique Island in the Lesser Antilles arc, which displays one of the most extreme geochemical and isotopic ranges, although the origin of this variability is still highly debated. We find the δ26Mg of the Martinique Island lavas varies from -0.25 to -0.10, in contrast to the narrow range that characterizes the mantle (-0.25 ± 0.04, 2 SD). These high δ26Mg values suggest the incorporation of isotopically heavy Mg from the subducted slab. The large contrast in MgO content between peridotite, basalt, and sediment makes direct mixing between sediment and peridotite, or assimilation by arc crust sediment, unlikely to be the main mechanism to modify Mg isotopes. Instead, the heavy Mg isotopic signature of the Martinique arc lavas requires that the overall composition of the mantle wedge is buffered and modified by the preferential addition of heavy Mg isotopes from fluids released from the altered subducted slab during fluid-mantle interaction. This, in turn, suggests transfer of a large amount of fluid-mobile elements from the subducting slab to the mantle wedge and makes Mg isotopes an excellent tracer of deep fluid migration.

  5. Magnesium isotope geochemistry in arc volcanism. (United States)

    Teng, Fang-Zhen; Hu, Yan; Chauvel, Catherine


    Incorporation of subducted slab in arc volcanism plays an important role in producing the geochemical and isotopic variations in arc lavas. The mechanism and process by which the slab materials are incorporated, however, are still uncertain. Here, we report, to our knowledge, the first set of Mg isotopic data for a suite of arc lava samples from Martinique Island in the Lesser Antilles arc, which displays one of the most extreme geochemical and isotopic ranges, although the origin of this variability is still highly debated. We find the δ(26)Mg of the Martinique Island lavas varies from -0.25 to -0.10, in contrast to the narrow range that characterizes the mantle (-0.25 ± 0.04, 2 SD). These high δ(26)Mg values suggest the incorporation of isotopically heavy Mg from the subducted slab. The large contrast in MgO content between peridotite, basalt, and sediment makes direct mixing between sediment and peridotite, or assimilation by arc crust sediment, unlikely to be the main mechanism to modify Mg isotopes. Instead, the heavy Mg isotopic signature of the Martinique arc lavas requires that the overall composition of the mantle wedge is buffered and modified by the preferential addition of heavy Mg isotopes from fluids released from the altered subducted slab during fluid-mantle interaction. This, in turn, suggests transfer of a large amount of fluid-mobile elements from the subducting slab to the mantle wedge and makes Mg isotopes an excellent tracer of deep fluid migration.

  6. The isotopic dipole moment of HDO

    Energy Technology Data Exchange (ETDEWEB)

    Assafrao, Denise; Mohallem, Jose R [Laboratorio de Atomos e Moleculas Especiais, Departamento de Fisica, ICEx, Universidade Federal de Minas Gerais, CP 702, 30123-970, Belo Horizonte, MG (Brazil)


    An adiabatic variational approximation is used to study the monodeuterated water molecule, HDO, accounting for the isotopic effect. The isotopic dipole moment, pointing from D to H, is then calculated for the first time, yielding (1.5 {+-} 0.1) x 10{sup -3} Debye, being helpful in the interpretation of experiments. (fast track communication)

  7. Atomic lithium vapor laser isotope separation

    CERN Document Server

    Olivares, I E


    An atomic vapor laser isotope separation in lithium was performed using tunable diode lasers. The method permits also the separation of the isotopes between the sup 6 LiD sub 2 and the sup 7 LiD sub 1 lines using a self-made mass separator which includes a magnetic sector and an ion beam designed for lithium. (Author)

  8. Cadmium isotope fractionation of materials derived from various industrial processes. (United States)

    Martinková, Eva; Chrastný, Vladislav; Francová, Michaela; Šípková, Adéla; Čuřík, Jan; Myška, Oldřich; Mižič, Lukáš


    Our study represents ϵ(114/110) Cd NIST3108 values of materials resulting from anthropogenic activities such as coal burning, smelting, refining, metal coating, and the glass industry. Additionally, primary sources (ore samples, pigment, coal) processed in the industrial premises were studied. Two sphalerites, galena, coal and pigment samples exhibited ϵ(114/110) CdNIST3108 values of 1.0±0.2, 0.2±0.2, 1.3±0.1, -2.3±0.2 and -0.1±0.3, respectively. In general, all studied industrial processes were accompanied by Cd isotope fractionation. Most of the industrial materials studied were clearly distinguishable from the samples used as a primary source based on ϵ(114/110) Cd NIST3108 values. The heaviest ϵ(114/110) CdNIST3108 value of 58.6±0.9 was found for slag resulting from coal combustion, and the lightest ϵ(114/110) CdNIST3108 value of -23±2.5 was observed for waste material after Pb refinement. It is evident that ϵ(114/110) Cd NIST3108 values depend on technological processes, and in case of incomplete Cd transfer from source to final waste material, every industrial activity creates differences in Cd isotope composition. Our results show that Cd isotope analysis is a promising tool to track the origins of industrial waste products.

  9. Second international conference on isotopes. Conference proceedings

    Energy Technology Data Exchange (ETDEWEB)

    Hardy, C.J. [ed.


    The Second International Conference on Isotopes (2ICI) was hosted by the Australian Nuclear Association in Sydney, NSW, Australia. The Theme of the Second Conference: Isotopes for Industry, Health and a Better Environment recognizes that isotopes have been used in these fields successfully for many years and offer prospects for increasing use in the future. The worldwide interest in the use of research reactors and accelerators and in applications of stable and radioactive isotopes, isotopic techniques and radiation in industry, agriculture, medicine, environmental studies and research in general, was considered. Other radiation issues including radiation protection and safety were also addressed. International and national overviews and subject reviews invited from leading experts were included to introduce the program of technical sessions. The invited papers were supported by contributions accepted from participants for oral and poster presentation. A Technical Exhibition was held in association with the Conference. This volume contains the full text or extended abstracts of papers number 61- to number 114

  10. Evidence for a catalytic six-membered cyclic transition state in aminolysis of 4-nitrophenyl 3,5-dinitrobenzoate in acetonitrile: comparative brønsted-type plot, entropy of activation, and deuterium kinetic isotope effects. (United States)

    Um, Ik-Hwan; Kim, Min-Young; Bae, Ae-Ri; Dust, Julian M; Buncel, Erwin


    A kinetic study for reactions of 4-nitrophenyl 3,5-dinitrobenzoate (1a) with a series of cyclic secondary amines in acetonitrile is reported. Plots of the pseudo-first-order rate constant (kobsd) vs [amine] curve upward, while those of kobsd /[amine] vs [amine] exhibit excellent linear correlations with positive intercepts, indicating that the reaction proceeds through both uncatalyzed and catalyzed routes. Brønsted-type plots for uncatalyzed and catalyzed reactions are linear with βnuc = 1.03 and 0.69, respectively. The ΔH(⧧) and ΔS(⧧) values measured for the catalytic reaction with morpholine are -0.80 kcal/mol and -61.7 cal/(mol K), respectively. The negative ΔH(⧧) with a large negative ΔS(⧧) suggests that the reaction proceeds through a highly ordered transition state (i.e., a six-membered cyclic transition state, which includes a second amine molecule that accepts a proton from the aminium moiety of the zwitterionic tetrahedral intermediate and simultaneously donates a proton to the aryloxyl oxygen of the nucleofuge with concomitant C-OAr bond scission). This proposal is consistent with the smaller βnuc value for the catalyzed reaction as compared to the uncatalyzed reaction. An inverse deuterium kinetic isotope effect (DKIE) value of 0.93 and a contrasting normal primary DKIE value of 3.23 for the uncatalyzed and catalyzed routes, respectively, also support the proposed cyclic transition state.

  11. Using Stable Isotopes to Trace Microbial Hydrogen Production Pathways (United States)

    Moran, J.; Hill, E.; Bartholomew, R.; Yang, H.; Shi, L.; Ostrom, N. E.; Gandhi, H.; Hegg, E.; Kreuzer, H.


    Biological H2 production by hydrogenase enzymes (H2ases) plays an important role in anaerobic microbial metabolism and community structure. Despite considerable progress in elucidating H2 metabolism, the regulation of and flux through key H2 production pathways remain largely undefined. Our goal is to improve understanding of biological H2 production by using H isotope ratios to dissect proton fluxes through different H2ase enzymes and from different substrates. We hypothesized that the isotope ratio of H2 produced by various hydrogenases (H2ase) would differ, and that the H isotope ratios would allow us to define the contribution of different enzymes when more than one is present in vivo. We chose Shewanella oneidensis (S.o.) MR-1, a facultative anaerobe capable of transferring electrons to a variety of terminal acceptors, including protons, as a model system for in vivo studies. S. o. encodes one [FeFe]- and one [NiFe]-H2ase. We purified three [FeFe]-H2ases (S.o., Clostridium pasteurianum, and Chlamydomonas reinhardtii) and two [NiFe]-H2ases (S. o. and Desulfovibrio fructosovorans) to test the isotope fractionation associated with activity by each enzyme in vitro. For in vivo analysis we used wild-type S.o. as well as electron transfer-deficient and H2ase-deficient strains. We employed batch cultures using lactate as an electron donor and O2 as an initial electron acceptor (with H2 production after O2 consumption). The five H2ases we tested all had a unique isotope fractionation. Measurements of H2 produced in vivo showed distinct periods of H2 production having isotope signatures consistent with in vitro results. Isotope data as well as studies of H2 production by mutants in the genes encoding either the [NiFe]-H2ase or the [FeFe]-H2ase, respectively, show that the [NiFe]- and [FeFe]- H2ases became active at different times. The [NiFe]-H2ase both produces and consumes H2 before the [FeFe]-H2ase becomes active. RNA analysis is consistent with up regulation of

  12. Inner Radiation Belt Generation of Light Nuclei Isotope (United States)

    Galper, A. M.; Koldashov, S. V.; Leonv, A. A.; Mikhailov, V. V.


    Nuclear interactions between inner zone protons and atoms in the upper atmosphere provide the essential source of H and He isotop es nuclei in radiation belt. This paper reports the calculations of these isotop es intensities from the inner zone proton intensity model AP-8, the atmosphere drift-averaged composition and densities model MSIS-90, and cross sections for the various interaction processes. To calculate drift-averaged densities and energy losses of secondaries the particles are traced in geomagnetic field according IGRF-95 model by numerical solution of motion equation. The calculations account for nuclear interactions kinematic along the whole trapped protons trajectories. The results of calculations are compared with experimental data from SAMPEX, CRRES, RESURS-04 and MITA satellites taken during different solar activity phases. The comparison with observational data shows that the atmosphere is sufficient source for inner zone 4 He, 3 He,2 H and 3 H for L-shell less than 1.3.

  13. Isotopic signatures: An important tool in today`s world

    Energy Technology Data Exchange (ETDEWEB)

    Rokop, D.J.; Efurd, D.W.; Benjamin, T.M.; Cappis, J.H.; Chamberlin, J.W.; Poths, H.; Roensch, F.R.


    High-sensitivity/high-accuracy actinide measurement techniques developed to support weapons diagnostic capabilities at the Los Alamos National Laboratory are now being used for environmental monitoring. The measurement techniques used are Thermal Ionization Mass Spectrometry (TIMS), Alpha Spectrometry(AS), and High Resolution Gamma Spectrometry(HRGS). These techniques are used to address a wide variety of actinide inventory issues: Environmental surveillance, site characterizations, food chain member determination, sedimentary records of activities, and treaty compliance concerns. As little as 10 femtograms of plutonium can be detected in samples and isotopic signatures determined on samples containing sub-100 femtogram amounts. Uranium, present in all environmental samples, can generally yield isotopic signatures of anthropogenic origin when present at the 40 picogam/gram level. Solid samples (soils, sediments, fauna, and tissue) can range from a few particles to several kilograms in size. Water samples can range from a few milliliters to as much as 200 liters.

  14. $\\beta$-NMR of copper isotopes in ionic liquids

    CERN Multimedia

    We propose to test the feasibility of spin-polarization and $\\beta$-NMR studies on several short-lived copper isotopes, $^{58}$ Cu, $^{74}$Cu and $^{75}$Cu in crystals and liquids. The motivation is given by biological studies of Cu with $\\beta$-NMR in liquid samples, since Cu is present in a large number of enzymes involved in electron transfer and activation of oxygen. The technique is based on spin-polarization via optical pumping in the new VITO beamline. We will use the existing lasers, NMR magnet and NMR chambers and we will prepare a new optical pumping system. The studies will be devoted to tests of achieved $\\beta$-asymmetry in solid hosts, the behaviour of asymmetry when increasing vacuum, and finally NMR scans in ionic liquids. The achieved spin polarization will be also relevant for the plans to measure with high precision the magnetic moments of neutron-rich Cu isotopes.

  15. Large Sulfur Isotope Fractionation Does Not Require Disproportionation (United States)

    Sim, Min Sub; Bosak, Tanja; Ono, Shuhei


    The composition of sulfur isotopes in sedimentary sulfides and sulfates traces the sulfur cycle throughout Earth’s history. In particular, depletions of sulfur-34 (34S) in sulfide relative to sulfate exceeding 47 per mil (‰) often serve as a proxy for the disproportionation of intermediate sulfur species in addition to sulfate reduction. Here, we demonstrate that a pure, actively growing culture of a marine sulfate-reducing bacterium can deplete 34S by up to 66‰ during sulfate reduction alone and in the absence of an extracellular oxidative sulfur cycle. Therefore, similar magnitudes of sulfur isotope fractionation in sedimentary rocks do not unambiguously record the presence of other sulfur-based metabolisms or the stepwise oxygenation of Earth’s surface environment during the Proterozoic.

  16. Large sulfur isotope fractionation does not require disproportionation. (United States)

    Sim, Min Sub; Bosak, Tanja; Ono, Shuhei


    The composition of sulfur isotopes in sedimentary sulfides and sulfates traces the sulfur cycle throughout Earth's history. In particular, depletions of sulfur-34 ((34)S) in sulfide relative to sulfate exceeding 47 per mil (‰) often serve as a proxy for the disproportionation of intermediate sulfur species in addition to sulfate reduction. Here, we demonstrate that a pure, actively growing culture of a marine sulfate-reducing bacterium can deplete (34)S by up to 66‰ during sulfate reduction alone and in the absence of an extracellular oxidative sulfur cycle. Therefore, similar magnitudes of sulfur isotope fractionation in sedimentary rocks do not unambiguously record the presence of other sulfur-based metabolisms or the stepwise oxygenation of Earth's surface environment during the Proterozoic.

  17. Manus Water Isotope Investigation Field Campaign Report

    Energy Technology Data Exchange (ETDEWEB)

    Conroy, Jessica L [University of Illinois, Urbana-Champaign; Cobb, Kim M [Georgia Institute of Technology; Noone, David [University of Colorado, Boulder


    The objective of this field campaign was to investigate climatic controls on the stable isotopic composition of water vapor, precipitation, and seawater in the western tropical Pacific. Simultaneous measurements of the stable isotopic composition of vapor and precipitation from April 28 to May 8, 2013, at the Manus Tropical Western Pacific Atmospheric Radiation Measurement site, provided several key insights into the nature of the climate signal archived in precipitation and vapor isotope ratios. We observed a large shift from lower to higher isotopic values in vapor and precipitation because of the passage of a mesoscale convective system west of the site and a transition from a regional stormy period into a more quiescent period. During the quiescent period, the stable isotopic composition of vapor and precipitation indicated the predominance of oceanic evaporation in determining the isotopic composition of boundary-layer vapor and local precipitation. There was not a consistent relationship between intra-event precipitation amount at the site and the stable isotopic composition of precipitation, thus challenging simplified assumptions about the isotopic “amount effect” in the tropics on the time scale of individual storms. However, some storms did show an amount effect, and deuterium excess values in precipitation had a significant relationship with several meteorological variables, including precipitation, temperature, relative humidity, and cloud base height across all measured storms. The direction of these relationships points to condensation controls on precipitation deuterium excess values on intra-event time scales. The relationship between simultaneous measurements of vapor and precipitation isotope ratios during precipitation events indicates the ratio of precipitation-to-vapor isotope ratios can diagnose precipitation originating from a vapor source unique from boundary-layer vapor and rain re-evaporation.

  18. Radiological and multi-element analysis of sediments from the Proserpina reservoir (Spain) dating from Roman times. (United States)

    Baeza, A; Guillén, J; Ontalba Salamanca, M A; Rodríguez, A; Ager, F J


    The Proserpina dam was built in Roman times to provide drinking water to Emerita Augusta (today's Mérida in SW Spain). During maintenance work, a sediment core was extracted, offering an excellent opportunity to analyze the historical environmental impacts of the dam and its reservoir over the 2000 years since Roman times. In order to establish an accurate chronology, (14)C ages were determined by accelerator mass spectrometry (AMS). Core samples were assayed for their content in uranium and thorium series isotopes, (40)K, and the anthropogenic radionuclides (137)Cs, (90)Sr, and (239+240)Pu. Potassium-40 presented the highest activity level and was not constant with depth. The uranium and thorium series were generally in equilibrium, suggesting there had been no additional input of natural radionuclides. The presence of (137)Cs was only found in relation with the global fallout in the early 1960s. Multi-element assays were performed using the PIXE and PIGE techniques. Some variations in the multi-element concentrations were observed with depth, but the sediment core could be considered as clean, and no presumptive anthropogenic pollutants were found. Nevertheless, an unusually high Zn content was detected at depths corresponding to pre-Roman times, due to geological anomalies in the area.

  19. Prompt detection of alpha particles from 210Po: another clue to the origin of rock varnish? (United States)

    Hodge, Vernon F; Farmer, Dennis E; Diaz, Tammy; Orndorff, Richard L


    Alpha particles have been measured coming from the surfaces of rocks covered with dark red-brown rock varnish, as well as rocks that appear to have little, if any, varnish. A pronounced peak at 5.3 MeV indicates the presence of 210Po, a short-lived natural-radioactive element. Surface activities for 33 samples range from 0.008 Bq/cm2 to 0.065 Bq/cm2. It is estimated that this nuclide is concentrated 10(11) times in these paper-thin coatings above its concentration in ground-level air. Gamma rays from the decay of 137Cs, a product of testing nuclear weapons some 50 years ago, were also detected. Analysis of samples of varnish stripped from the rock revealed traces of 239,240Pu and 238Pu. The presence of all of these isotopes strongly supports the theory that varnish films derive their building blocks from the atmosphere and, with time, all rocks in arid environments will become coated.

  20. Radioactivity Distribution In Surface And Core Sediment Of The Central Part Of The Algerian Coast: An Estimation Of The Recent Sedimentation Rate

    Directory of Open Access Journals (Sweden)



    Full Text Available Sediment core samples and marine surface sediments of identical composition, mostly muddy, were collected using a Van Veen type grab and a box corer on board the M.S. Benyahia research vessel (ISMAL, along the Algerian littoral, between Algiers (36Ζ49.9 N/ 03Ζ 02.3 E and Cherchell (36Ζ 39.4 N/ 02Ζ 12.4 E, during a sampling cruise in September 1997. The samples were analysed to determine the activity concentration of natural radionuclides (uranium and thorium series and 40 K as well and artificial radionuclides ( 137 Cs and Pu isotopes, using a direct gamma spectrometry for gamma emitters and radiochemical separations and alpha spectrometry for alpha emitters. The horizontal and vertical distribution of the examined radionuclides were studied in the surface and core samples and an effort to estimate the sedimentation rate was attempted.The measured values range was: 17 - 26 Bq/Kg dry for uranium series radioisotopes, 18 – 32 Bq/Kg dry for thorium series radioisotopes, 311 - 690 Bq/Kg dry for 40 K, 0.4 - 11 Bq/Kg dry, for 137 Cs and 0.4 – 1.0 Bq/Kg dry for 239 + 240 Pu.

  1. Lead Isotopes in Highway Runoff (United States)

    Ferreira, M.; Lau, S.; Green, P. G.; Stenstrom, M. K.


    Lead (Pb) isotopes have been used extensively to study the provenance of lead pollution on air, water, and sediments. In this study, we measured Pb isotopes and Pb aqueous concentration in highway runoff in three west Los Angeles sites. Those three sites, part of a long-term study sponsored by the California Department of Transportation, represent small catchment areas, and host heavy traffic. In addition, there were no inputs of sand or salt to the highway because the sites are almost completely impervious and also due to the lack of snow to be controlled. Highway runoff from the three sites was collected for 7 storms during the 2004-2005 Winter. Grab samples were collected every 15 minutes during the first hour, and hourly afterwards. A total of 202 samples were collected and filtered into five size fractions (100μm). Aqueous concentration of Pb range from 0.08μg/L to 46.95μg/L (7.98±10.89μg/L) and it is not correlated with any of the lead isotope ratios. The 208Pb/206Pb ratio ranges from 1.983 to 2.075 (2.024±0.026) and there is no statistical difference for the mean value of the 208Pb/206Pb ratio for the four particulate size fractions (0.45-8μm, 8-20μm, 20-100μm, >100μm). However, the 208Pb/206Pb ratio of nearby soils yield 2.060±0.021 and it is statistically different from the ratios obtained for the highway runoff. This hints that the lead present in highway runoff does not come from local soils. The 207Pb/206Pb ratio ranges from 0.804 to 0.847 (0.827±0.011) and there is no statistical difference for the mean value of the 207Pb/206Pb ratio for the four particulate size fractions (0.45-8μm, 8-20μm, 20-100μm, >100μm). Surprisingly, there is also no statistical difference with the 207Pb/206Pb ratio of nearby soils (0.833±0.009).

  2. Late Holocene Human Activity Inferred from Sedimentary n-Alkanes and Their Carbon Isotope in the Huguangyan Maar Lake%湖光岩玛珥湖晚全新世人类活动的叶蜡烷烃及其碳同位素沉积记录

    Institute of Scientific and Technical Information of China (English)

    柏杨; 欧阳婷萍; 贾国东


    通过对广东省湛江市湖光岩玛珥湖晚全新世沉积物中叶蜡烷烃(n-C29,n-C31,n-C33)及其碳同位素(δ13C)进行分析,探讨该湖区约3.5 ka BP以来的植被变化历史,重点讨论了人类活动对该区域植被变化可能带来的影响。叶蜡烷烃δ13C在1.7 ka BP以前偏轻,例如长链烷烃碳同位素在1.78 ka BP为-33.27‰,表明湖区C3植物占绝对优势,表现为典型的C3型生态系统;在1.7 ka BP之后碳同位素明显快速偏重,在1.63 ka BP为-28.26‰,指示了C4植物出现和C4比例上升的过程。C4植物的出现通常指示气候的干旱化,但是烷烃Paq和ACL指数(平均链长)则显示湖区气候可能在1.7 ka BP后变湿润。通过与研究区甘蔗的同位素和ACL指数的比较分析,推测这一矛盾现象可能与湖区开始有一定规模的甘蔗种植活动有关。%In this study, late Holocene sedimentary records of leaf wax n-alkanes and theirδ13 C from Huguangyan Maar Lake (H.M.L) in Zhanjiang, Guangdong Province, were used to reconstruct the vegetation variations as well as human activities in the lake catchment over the past 3500 years. Carbon isotopic compositions (δ13C) of leaf wax n-alkanes (n-C29, n-C31 and n-C33) were predominantly lighter than-32‰before 1.7 ka BP, suggesting that a typically pure C3 ecosystem might exist before 1.7 ka BP; for example, carbon isotope average value of long-chain n-alkanes was -33.27 ‰ in 1.78 ka BP; after that δ13C values increased rapidly and significantly, carbon isotope value was-28.26‰in 1.63 ka BP, indicating the emergence and increase of C4 plants. C4 plants usually indicate an arid climate, however, the n-alkanes indices that both increased Paq and reduced ACL indicate a humid climate after 1.7 ka BP. This contradiction can be well explained by invoking anthropogenic sugarcane plantation in the catchment at 1.7 ka BP. Furthermore, when it comes to the isotope change of samples, we find

  3. 77 FR 14837 - Advisory Committee on the Medical Uses of Isotopes: Meeting Notice (United States)


    ... Medical Uses of Isotopes (ACMUI) on April 16-17, 2012. A sample of agenda items to be discussed during the...) regulations; (3) medical-related events from fiscal year 2011; (4) an update on proposed regulatory changes... perspectives; and (9) half-life activity as a function of solar activity. The agenda is subject to change....

  4. Identification of triclosan-degrading bacteria using stable isotope probing, fluorescence in situ hybridization and microautoradiography

    DEFF Research Database (Denmark)

    Lolas, Ihab Bishara Lolas; Chen, Xijuan; Bester, Kai


    -based stable isotope probing (DNA-SIP) combined with microautoradiography-fluorescence in situ hybridization (MAR-FISH) was applied to identify active triclosan degraders in an enrichment culture inoculated with activated sludge. Clone library sequences of 16S rRNA genes derived from the heavy DNA fractions...

  5. Chromium isotope uptake in carbonates

    DEFF Research Database (Denmark)

    Rodler, Alexandra

    composition of contemporaneous seawater. Marine carbonates are ubiquitous throughout Earth’s rock record rendering them a particularly interesting archive for constraining past changes in ocean chemistry. This thesis includes an investigation of the fractionation behavior of Cr isotopesduring coprecipitation......Chromium (Cr) is a redox sensitive element potentially capable of tracing fine-scale fluctuations of the oxygenation of Earth’s early surface environments and seawater. The Cr isotope composition of carbonates could perhaps be used as paleo-redox proxy to elucidate changes in the geological past...... related to the rise of oxygen and the evolution of the biosphere. However, before the Cr isotopesystem can be applied to faithfully delineate paleo-environmental changes, careful assessment of the signal robustness and a thorough understanding of the Cr cycle in Earth system processes is necessary...

  6. Measurement of isotope abundance variations in nature by gravimetric spiking isotope dilution analysis (GS-IDA). (United States)

    Chew, Gina; Walczyk, Thomas


    Subtle variations in the isotopic composition of elements carry unique information about physical and chemical processes in nature and are now exploited widely in diverse areas of research. Reliable measurement of natural isotope abundance variations is among the biggest challenges in inorganic mass spectrometry as they are highly sensitive to methodological bias. For decades, double spiking of the sample with a mix of two stable isotopes has been considered the reference technique for measuring such variations both by multicollector-inductively coupled plasma mass spectrometry (MC-ICPMS) and multicollector-thermal ionization mass spectrometry (MC-TIMS). However, this technique can only be applied to elements having at least four stable isotopes. Here we present a novel approach that requires measurement of three isotope signals only and which is more robust than the conventional double spiking technique. This became possible by gravimetric mixing of the sample with an isotopic spike in different proportions and by applying principles of isotope dilution for data analysis (GS-IDA). The potential and principle use of the technique is demonstrated for Mg in human urine using MC-TIMS for isotopic analysis. Mg is an element inaccessible to double spiking methods as it consists of three stable isotopes only and shows great potential for metabolically induced isotope effects waiting to be explored.

  7. Calculation of the inventory and near-field release rates of radioactivity from neutron-activated metal parts discharged from the high flux isotope reactor and emplaced in solid waste storage area 6 at Oak Ridge National Laboratory

    Energy Technology Data Exchange (ETDEWEB)

    Kelmers, A.D.; Hightower, J.R.


    Emplacement of contaminated reactor components involves disposal in lined and unlined auger holes in soil above the water table. The radionuclide inventory of disposed components was calculated. Information on the composition and weight of the components, as well as reasonable assumptions for the neutron flux fueling use, the time of neutron exposure, and radioactive decay after discharge, were employed in the inventory calculation. Near-field release rates of /sup 152/Eu, /sup 154/Eu, and /sup 155/Eu from control plates and cylinders were calculated for 50 years after emplacement. Release rates of the europium isotopes were uncertain. Two release-rate-limiting models were considered and a range of reasonable values were assumed for the time-to-failure of the auger-hole linear and aluminum cladding and europium solubility in SWSA-6 groundwater. The bounding europium radionuclide near-field release rates peaked at about 1.3 Ci/year total for /sup 152,154,155/Eu in 1987 for the lower bound, and at about 420 Ci/year in 1992 for the upper bound. The near-field release rates of /sup 55/Fe, /sup 59/Ni, /sup 60/Co, and /sup 63/Ni from stainless steel and cobalt alloy components, as well as of /sup 10/Be, /sup 41/Ca, and /sup 55/Fe from beryllium reflectors, were calculated for the next 100 years, assuming bulk waste corrosion was the release-rate-limiting step. Under the most conservative assumptions for the reflectors, the current (1986) total radionuclide release rate was calculated to be about 1.2 x 10/sup -4/ Ci/year, decreasing by 1992 to a steady release of about 1.5 x 10/sup -5/ Ci/year due primarily to /sup 41/Ca. 50 refs., 13 figs., 8 tabs.

  8. High sulfur isotope fractionation associated with anaerobic oxidation of methane in a low sulfate, iron rich environment

    Directory of Open Access Journals (Sweden)

    Hannah Sophia Weber


    Full Text Available Sulfur isotope signatures provide key information for the study of microbial activity in modern systems and the evolution of the Earth surface redox system. Microbial sulfate reducers shift sulfur isotope distributions by discriminating against heavier isotopes. This discrimination is strain-specific and often suppressed at sulfate concentrations in the lower micromolar range that are typical to freshwater systems and inferred for ancient oceans. Anaerobic oxidation of methane (AOM is a sulfate-reducing microbial process with a strong impact on global sulfur cycling in modern habitats and potentially in the geological past, but its impact on sulfur isotope signatures is poorly understood, especially in low sulfate environments. We investigated sulfur cycling and 34S fractionation in a low-sulfate freshwater sediment with biogeochemical conditions analogous to Early Earth environments. The zone of highest AOM activity was associated in situ with a zone of strong 34S depletions in the pool of reduced sulfur species, indicating a coupling of sulfate reduction and AOM at sulfate concentrations < 50 µmol L-1. In slurry incubations of AOM-active sediment, the addition of methane stimulated sulfate reduction and induced a bulk sulfur isotope effect of ~29 ‰. Our results imply that sulfur isotope signatures may be strongly impacted by AOM even at sulfate concentrations two orders of magnitude lower than at present oceanic levels. Therefore, we suggest that sulfur isotope fractionation during AOM must be considered when interpreting 34S signatures in modern and ancient environment.

  9. The isotope effect: Prediction, discussion, and discovery

    CERN Document Server

    Kragh, Helge


    The precise position of a spectral line emitted by an atomic system depends on the mass of the atomic nucleus and is therefore different for isotopes belonging to the same element. The possible presence of an isotope effect followed from Bohr's atomic theory of 1913, but it took several years before it was confirmed experimentally. Its early history involves the childhood not only of the quantum atom, but also of the concept of isotopy. Bohr's prediction of the isotope effect was apparently at odds with early attempts to distinguish between isotopes by means of their optical spectra. However, in 1920 the effect was discovered in HCl molecules, which gave rise to a fruitful development in molecular spectroscopy. The first detection of an atomic isotope effect was no less important, as it was by this means that the heavy hydrogen isotope deuterium was discovered in 1932. The early development of isotope spectroscopy illustrates the complex relationship between theory and experiment, and is also instructive with...

  10. Compound specific isotope analysis of organophosphorus pesticides. (United States)

    Wu, Langping; Yao, Jun; Trebse, Polonca; Zhang, Ning; Richnow, Hans H


    Compound-specific isotope analysis (CSIA) has been established as a tool to study the environmental fate of a wide range of contaminants. In this study, CSIA was developed to analyse the stable carbon isotope signatures of the widely used organophosphorus pesticides: dichlorvos, omethoate and dimethoate. The linearity of the GC-C-IRMS system was tested for target pesticides and led to an acceptable isotope composition within the uncertainty of the instrument. In order to assess the accuracy of the developed method, the effect of the evaporation procedure on measured carbon isotope composition (δ(13)C) values was studied and showed that concentration by evaporation of solvents had no significant isotope effect. The CSIA was then applied to investigate isotope fractionation of the hydrolysis and photolysis of selected pesticides. The carbon isotope fractionation of tested pesticides was quantified by the Rayleigh model, which revealed a bulk enrichment factor (ε) of -0.2±0.1‰ for hydrolysis of dichlorvos, -1.0±0.1‰ and -3.7±1.1‰ for hydrolysis and photolysis of dimethoate respectively. This study is a first step towards the application of CSIA to trace the transport and degradation of organophosphorus pesticides in the environment.

  11. Si isotope homogeneity of the solar nebula

    Energy Technology Data Exchange (ETDEWEB)

    Pringle, Emily A.; Savage, Paul S.; Moynier, Frédéric [Department of Earth and Planetary Sciences and McDonnell Center for the Space Sciences, Washington University in St. Louis, One Brookings Drive, St. Louis, MO 63130 (United States); Jackson, Matthew G. [Department of Earth Science, University of California, Santa Barbara, CA 93109 (United States); Barrat, Jean-Alix, E-mail:, E-mail:, E-mail:, E-mail:, E-mail:, E-mail: [Université Européenne de Bretagne, Université de Brest, CNRS UMR 6538 (Domaines Océaniques), I.U.E.M., Place Nicolas Copernic, F-29280 Plouzané Cedex (France)


    The presence or absence of variations in the mass-independent abundances of Si isotopes in bulk meteorites provides important clues concerning the evolution of the early solar system. No Si isotopic anomalies have been found within the level of analytical precision of 15 ppm in {sup 29}Si/{sup 28}Si across a wide range of inner solar system materials, including terrestrial basalts, chondrites, and achondrites. A possible exception is the angrites, which may exhibit small excesses of {sup 29}Si. However, the general absence of anomalies suggests that primitive meteorites and differentiated planetesimals formed in a reservoir that was isotopically homogenous with respect to Si. Furthermore, the lack of resolvable anomalies in the calcium-aluminum-rich inclusion measured here suggests that any nucleosynthetic anomalies in Si isotopes were erased through mixing in the solar nebula prior to the formation of refractory solids. The homogeneity exhibited by Si isotopes may have implications for the distribution of Mg isotopes in the solar nebula. Based on supernova nucleosynthetic yield calculations, the expected magnitude of heavy-isotope overabundance is larger for Si than for Mg, suggesting that any potential Mg heterogeneity, if present, exists below the 15 ppm level.

  12. Stable isotopic characterisation of francolite formation (United States)

    McArthur, J. M.; Benmore, R. A.; Coleman, M. L.; Soldi, C.; Yeh, H.-W.; O'Brien, G. W.


    Stable isotopic data are presented for 112 samples of francolite from 18 separate phosphate deposits. Values of δ 13C and δ 34S in most offshore deposits suggest formation within oxic or suboxic environments either by carbonate replacement or direct precipitation of francolite from water of normal marine compositions. The exceptions are concretionary francolite from Namibia, which has an isotopic composition in keeping with its formation within organic-rich sediments, and that from offshore Morocco, which has an isotopic signature of the anoxic/suboxic interface. Onshore deposits from Jordan, Mexico, South Africa and, possibly, the Permian Phosphoria Formation in the western U.S.A., are substantially depleted in 18O: they appear to be too altered for deductions to be made about their environments of formation. In other onshore deposits which are unaltered, or minimally altered, the isotopic composition suggests that some formed within sulphate-reducing sediments (Sedhura, Morocco) whilst francolite from the Georgina Basin of Australia formed at the oxic/anoxic boundary, where oxidation of biogenic H 2S decreases the δ 34S of pore water. In general, pelletal samples show non-oxic isotopic signatures, whilst non-pelletal samples show oxic isotopic signatures, but samples from Namibia, Peru (Ica Plateau) and the Californian and Moroccan margins are exceptions to this rule. Morphology may therefore be a misleading indicator of francolite genesis as no definitive relation exists between phosphorite type and isotopic signature.

  13. Stable isotope composition of land snail body water and its relation to environmental waters and shell carbonate (United States)

    Goodfriend, Glenn A.; Magaritz, Mordeckai; Gat, Joel R.


    Day-to-day and within-day (diel) variations in δD and δ18O of the body water of the land snail, Theba pisana, were studied at a site in the southern coastal plain of Israel. Three phases of variation, which relate to isotopic changes in atmospheric water vapor, were distinguished: 1) on rain days, snail water becomes isotopically depleted approximately in the direction of the rain isotope values, but always less depleted in D as is atmospheric water vapor; 2) during the 1-3 days following a rain, the snail water becomes isotopically enriched along a line with slope persists until the next rain event. The isotopic variations can be explained by isotopic equilibration with atmospheric water vapor and/or uptake of dew derived therefrom. During the winter, when the snails are active, there is only very minor enrichment in 18O relative to equilibrium with water vapor or dew, apparently as a result of metabolic activity. But this enrichment becomes pronounced after long periods of inactivity. Within-day variation in body water isotopic composition is minor on non-rain days. Shell carbonate is enriched in 18O by ca. 1-2%. relative to equilibrium with body water. In most regions, the isotopic composition of atmospheric water vapor (or dew) is a direct function of that of rain. Because the isotopic composition of snail body water is related to that of atmospheric water vapor and the isotopic composition of shell carbonate in turn is related to that of body water, land snail shell carbonate 18O should provide a reliable indication of rainfall 18O. However, local environmental conditions and the ecological properties of the snail species must be taken into account.

  14. Beneficial uses and production of isotopes

    CERN Document Server


    Isotopes, radioactive and stable, are used worldwide in various applications related to medical diagnosis or care, industry and scientific research. More than fifty countries have isotope production or separation facilities operated for domestic supply, and sometimes for international markets. This publication provides up-to-date information on the current status of, and trends in, isotope uses and production. It also presents key issues, conclusions and recommendations, which will be of interest to policy makers in governmental bodies, scientists and industrial actors in the field.

  15. The Facility for Rare Isotope Beams

    Directory of Open Access Journals (Sweden)

    Wrede C.


    Full Text Available The Facility for Rare Isotope Beams (FRIB is a United States Department of Energy user facility currently under construction on the campus of Michigan State University. Based on a 400 kW, 200 MeV/u heavy-ion driver linac, FRIB will deliver high-quality fast, thermalized, and re-accelerated beams of rare isotopes with unprecedented intensities to a variety of experimental areas and equipment. New science opportunities at the frontiers of nuclear structure, nuclear astrophysics, fundamental symmetries, and societal applications will be enabled by this future world-leading rare-isotope beam facility.

  16. The Facility for Rare Isotope Beams (United States)

    Wrede, C.


    The Facility for Rare Isotope Beams (FRIB) is a United States Department of Energy user facility currently under construction on the campus of Michigan State University. Based on a 400 kW, 200 MeV/u heavy-ion driver linac, FRIB will deliver high-quality fast, thermalized, and re-accelerated beams of rare isotopes with unprecedented intensities to a variety of experimental areas and equipment. New science opportunities at the frontiers of nuclear structure, nuclear astrophysics, fundamental symmetries, and societal applications will be enabled by this future world-leading rare-isotope beam facility.

  17. Isotopic Fractionation of Selenium Oxyanions in Wetlands (United States)

    Clark, S. K.; Johnson, T. M.


    As oxic surface waters pass through aquatic macrophytes and over anoxic sediments in wetlands and lakes, the dissolved Se load often decreases; and, Se isotope ratio measurements can provide information about the mechanisms involved. Previous work on microbially induced isotopic fractionation of Se oxyanions under nearly natural conditions using wetland sediments shows consistent Se isotopic shifts during reduction of Se(VI) and Se(IV) to insoluble Se(0). However, previous isotopic studies of total dissolved selenium in wetlands found little to no isotopic shift as dissolved selenium concentrations decreased. This suggests that plant/algal uptake, followed by deposition and degradation, is the primary route of Se transfer into sediments. However, it is possible that the effective isotopic fractionation between Se in the surface water and Se deposited into sediments is somehow much less than the fractionation induced by the reduction reaction, or that cycling of organically bound Se is involved. In this study, we report Se isotope data for Se(VI), Se(IV) and total dissolved Se, Se(T), in surface waters from three wetland/lake sites: Sweitzer Lake, CO; 33-Mile Reservoir, WY; and, a small pond adjacent to Benton Lake, MT. We isolated Se(IV) via hydride generation, and Se(VI) via ion exchange. Se(T), including any organic components, was also analyzed. Isotope analysis was performed on an Isoprobe MC-ICPMS, using a method modified from that of Rouxel et al. (2002). We used the 82Se + 74Se double spike approach, and spiked samples before species separation. Our results for all three locations indicate similar trends in concentration changes and isotopic shifts between the inflow and outflow waters. Se(T) concentrations decrease by 45-70%, and Se(VI) concentrations decrease by 60-90%, whereas Se(IV) concentrations increase by 60-150%. Concomitant 80Se/76Se shifts are +0.5-0.8‰ for Se(T); -0.1-0.5‰ for Se(VI); and +0.4-6.5‰ for Se(IV). These data provide greater

  18. Isotope fractionation during the anaerobic consumption of acetate by methanogenic and sulfate-reducing microorganisms (United States)

    Gövert, D.; Conrad, R.


    During the anaerobic degradation of organic matter in anoxic sediments and soils acetate is the most important substrate for the final step in production of CO2 and/or CH4. Sulfate-reducing bacteria (SRB) and methane-producing archaea both compete for the available acetate. Knowledge about the fractionation of 13C/12C of acetate carbon by these microbial groups is still limited. Therefore, we determined carbon isotope fractionation in different cultures of acetate-utilizing SRB (Desulfobacter postgatei, D. hydrogenophilus, Desulfobacca acetoxidans) and methanogens (Methanosarcina barkeri, M. acetivorans). Including literature values (e.g., Methanosaeta concilii), isotopic enrichment factors (epsilon) ranged between -35 and +2 permil, possibly involving equilibrium isotope effects besides kinetic isotope effects. The values of epsilon were dependent on the acetate-catabolic pathway of the particular microorganism, the methyl or carboxyl position of acetate, and the relative availability or limitation of the substrate acetate. Patterns of isotope fractionation in anoxic lake sediments and rice field soil seem to reflect the characteristics of the microorganisms actively involved in acetate catabolism. Hence, it might be possible using environmental isotopic information to determine the type of microbial metabolism converting acetate to CO2 and/or CH4.

  19. Use of the Bochum proton microprobe in isotope stratigraphy and paleoceanographic

    Energy Technology Data Exchange (ETDEWEB)

    Bruhn, F.; Bruckschen, P.; Korte, C. [Ruhr-University, Bochum (Germany). Institute fuer Geologie; Meijer, J. [Ruhr-Univ., Bochum (Germany). Inst. fuer Physik mit Ionenstrahlen; Veizer, J. [Ruhr-University Bochum (Germany). Institute fuer Geologie]|[Ottawa-Carleton Univ., Ottawa, ON (Canada)


    Over the past five years, the proton microprobe at Bochum (Germany) has been used as a trace element tool in the context of isotope stratigraphy and paleoceanographic studies. The Sr, O, and C isotopic composition of some biogenic material (e.g. calcitic brachiopod shells, phosphatic conodonts) is widely accepted to mirror, under favourable conditions, the isotopic composition of the coeval sea water. The latter, in turn, is a function of a variety of global processes, such as climatic change, volcanic activity, plate tectonics or circulation of ocean water. Thus, on the basis of the isotopic properties of fossil shell material, isotope curves can be constructed that reflect variations in the above factors over the entire Phanerozoic. However, as a consequence of the long time elapsed since deposition of the fossils, they are prone to chemical and isotopic alteration and may thus yield equivocal or even irrelevant information if no care is taken to monitor the degree of their diagenetic alteration. Trace element composition of the fossil material, combined with cathodoluminescence investigations, is one of the most frequently utilized tools to assess the diagenetic quality of the samples. Beam current was in the range of a few nA, resulting in charges of 1-10 {mu}C for a single measurement. Detection limits for point analyses were between 10 and 30 ppm for Mn, Fe, Sr, but considerably higher for rare earth elements. Accuracy around 10% for a number of elements analysed is reported. 8 refs., 2 figs.

  20. Atmospheric controls on the precipitation isotopes over the Andaman Islands, Bay of Bengal (United States)

    Chakraborty, S.; Sinha, N.; Chattopadhyay, R.; Sengupta, S.; Mohan, P. M.; Datye, A.


    Isotopic analysis of precipitation over the Andaman Island, Bay of Bengal was carried out for the year 2012 and 2013 in order to study the atmospheric controls on rainwater isotopic variations. The oxygen and hydrogen isotopic compositions are typical of the tropical marine sites but show significant variations depending on the ocean-atmosphere conditions; maximum depletion was observed during the tropical cyclones. The isotopic composition of rainwater seems to be controlled by the dynamical nature of the moisture rather than the individual rain events. Precipitation isotopes undergo systematic depletions in response to the organized convection occurring over a large area and are modulated by the integrated effect of convective activities. Precipitation isotopes appear to be linked with the monsoon intraseasonal variability in addition to synoptic scale fluctuations. During the early to mid monsoon the amount effect arose primarily due to rain re-evaporation but in the later phase it was driven by moisture convergence rather than evaporation. Amount effect had distinct characteristics in these two years, which appeared to be modulated by the intraseasonal variability of monsoon. It is shown that the variable nature of amount effect limits our ability to reconstruct the past-monsoon rainfall variability on annual to sub-annual time scale. PMID:26806683

  1. Substrate and Transition State Binding in Alkaline Phosphatase Analyzed by Computation of Oxygen Isotope Effects. (United States)

    Roston, Daniel; Cui, Qiang


    Enzymes are powerful catalysts, and a thorough understanding of the sources of their catalytic power will facilitate many medical and industrial applications. Here we have studied the catalytic mechanism of alkaline phosphatase (AP), which is one of the most catalytically proficient enzymes known. We have used quantum mechanics calculations and hybrid quantum mechanics/molecular mechanics (QM/MM) simulations to model a variety of isotope effects relevant to the reaction of AP. We have calculated equilibrium isotope effects (EIEs), binding isotope effects (BIEs), and kinetic isotope effects (KIEs) for a range of phosphate mono- and diester substrates. The results agree well with experimental values, but the model for the reaction's transition state (TS) differs from the original interpretation of those experiments. Our model indicates that isotope effects on binding make important contributions to measured KIEs on V/K, which complicated interpretation of the measured values. Our results provide a detailed interpretation of the measured isotope effects and make predictions that can test the proposed model. The model indicates that the substrate is deformed in the ground state (GS) of the reaction and partially resembles the TS. The highly preorganized active site preferentially binds conformations that resemble the TS and not the GS, which induces the substrate to adapt to the enzyme, rather than the other way around-as with classic "induced fit" models. The preferential stabilization of the TS over the GS is what lowers the barrier to the chemical step.

  2. Characterization of phenols biodegradation by compound specific stable isotope analysis (United States)

    Wei, Xi; Gilevska, Tetyana; Wenzig, Felix; Hans, Richnow; Vogt, Carsten


    Biodegradation of phenol and alkylphenols has been described under both oxic and anoxic conditions. In the absence of molecular oxygen, the degradation of phenolic compounds is initiated by microorganisms through carboxylation, fumarate addition to the methyl moiety or anoxic hydroxylation of the methyl moiety. Comparatively, under aerobic condition, the initiation mechanisms are revealed to be monoxygenation or dihydroxylation for phenol and ring hydroxylation or methyl group oxidation for cresols. While several studies biochemically characterized the enzymes and reaction mechanisms in the relevant degradation pathways, isotope fractionation patterns were rarely reported possibly due to constraints in current analytical methods. In this study, the carbon isotope fractionation patterns upon the degradation of phenol and cresols by several strains were analyzed by using isotope ratio mass spectrometry connected with liquid chromatography (LC-IRMS). The corresponding enrichment factors for carbon (ƐC) have been obtained. Cresols degradation by various strains showed generally moderate carbon isotope fractionation patterns with notable differences. For p-cresol degradation, five strains were examined. The aerobic strain Acinetobacter calcoaceticus NCIMB8250 exploits ring hydroxylation by molecular oxygen as initial reaction, and a ƐC value of -1.4±0.2‰ was obtained. Pseudomonas pseudoalcaligenes NCIMB 9867, an aerobic strain initiating cresols degradation via oxygen-dependent side chain hydroxylation, yielded a ƐC value of -2.3±0.2‰. Under nitrate-reducing conditions, Geobacter metallireducens DSM 7210 and Azoarcus buckelii DSM 14744 attacks p-cresol at the side chain by monohydroxylation using water as oxygen source; the two strains produced ƐC values of -3.6±0.4‰ and -2±0.1‰, accordingly. The sulfate-reducing Desulfosarcina cetonica DSM 7267 activating cresols by fumarate addition to the methyl moiety yielded ƐC values of -1.9±0.2‰ for p

  3. Clumped-Isotope Thermometry and Oxygen Isotope Systematics in Speleothem Calcite From a Near Cave-Entrance Environment (United States)

    Carlson, P. E.; Banner, J.; Breecker, D.; Affek, H. P.


    Speleothems that grow in well-ventilated zones of caves have not been widely used in paleoclimate studies, yet may provide paleotemperature records. These zones are characterized by low CO2 concentrations year-round and, in temperate climates, large seasonal temperature fluctuations. They are typically avoided for paleoclimate reconstruction due to concerns about kinetic isotope effects (KIE). However, speleothems in general seem to be sensitive to KIE, even in non-ventilated areas and can nonetheless provide useful paleoclimate records. At Westcave Preserve (Westcave), a shallow, well-ventilated cave in central Texas, we have found seasonal temperature differences recorded in both the oxygen isotope and clumped isotope compositions of speleothem calcite grown on glass-plate substrates harvested from active drips. Although growth rates in this cave are relatively rapid, speleothem analogs in Westcave are growing near oxygen-isotopic equilibrium with their drip waters (between the calibrations of Kim and O'Neil, 1997 and Coplen, 2007). We have tested the compatibility of the Zaarur et al. (2013) clumped isotope bulk solution thermometer calibration to glass-substrate calcite in the cave collected during various months. This technique can provide absolute temperatures, but is sensitive to kinetic isotope effects, often significantly overestimating growth temperatures of speleothems. When this thermometer was applied to calcite collected from near where the plates were impacted by drip water, it overestimated measured temperatures by 7.7 ± 4.3°C, showing moderate KIE. When applied to calcite away from the drip impact, it overestimated temperatures by 18.7 ± 4.2°C, showing KIE increasing away from the drip. Measured monthly average temperatures in the cave ranged seasonally between 8 and 28°C, and daily temperatures vary significantly. At Westcave, calcite growth rates increase with temperature, and the calcite may therefore preferentially record warmer daily or

  4. Divergence of stable isotopes in tap water across China (United States)

    Zhao, Sihan; Hu, Hongchang; Tian, Fuqiang; Tie, Qiang; Wang, Lixin; Liu, Yaling; Shi, Chunxiang


    Stable isotopes in water (e.g., δ2H and δ18O) are important indicators of hydrological and ecological patterns and processes. Tap water can reflect integrated features of regional hydrological processes and human activities. China is a large country with significant meteorological and geographical variations. This report presents the first national-scale survey of Stable Isotopes in Tap Water (SITW) across China. 780 tap water samples have been collected from 95 cities across China from December 2014 to December 2015. (1) Results yielded the Tap Water Line in China is δ2H = 7.72 δ18O + 6.57 (r2 = 0.95). (2) SITW spatial distribution presents typical “continental effect”. (3) SITW seasonal variations indicate clearly regional patterns but no trends at the national level. (4) SITW can be correlated in some parts with geographic or meteorological factors. This work presents the first SITW map in China, which sets up a benchmark for further stable isotopes research across China. This is a critical step toward monitoring and investigating water resources in climate-sensitive regions, so the human-hydrological system. These findings could be used in the future to establish water management strategies at a national or regional scale.

  5. Iron isotope geochemistry in the Antarctic cryptoendolithic microbial ecosystem (United States)

    Sun, H.


    The stable isotope composition of iron is a potentially powerful tracer of biogeochemical cycles because iron is ubiquitous, it is required by all organisms, and it is resistant to alterations during diagenesis. Here we report evidence of biological iron isotope fractionation in the weathering process of sandstone in McMurdo Dry Valleys, Antarctica, caused by the cryptoendolithic lichen-dominated microbial community that live below the rock surface. The fungi secrete oxalic acid, which under the sunlight reduces and dissolves the iron in the colonized zone. The mobilized iron diffuses to the rock surface and the rock interior below the organisms where it is re-oxidized. This leaching process is shown to prefer lighter isotopes of iron, leaving the colonized layer enriched in del 56Fe by as much 0.8 per mil. Had endolithic microorganisms occurred on Mars as commonly believed, they might have left similar iron biosignatures, well preserved in rocks because of the absence of subsequent aqueous activities.

  6. Simultaneous tracing of carbon and nitrogen isotopes in human cells. (United States)

    Nilsson, Roland; Jain, Mohit


    Stable isotope tracing is a powerful method for interrogating metabolic enzyme activities across the metabolic network of living cells. However, most studies of mammalian cells have used (13)C-labeled tracers only and focused on reactions in central carbon metabolism. Cellular metabolism, however, involves other biologically important elements, including nitrogen, hydrogen, oxygen, phosphate and sulfur. Tracing stable isotopes of such elements may help shed light on poorly understood metabolic pathways. Here, we demonstrate the use of high-resolution mass spectrometry to simultaneously trace carbon and nitrogen metabolism in human cells cultured with (13)C- and (15)N-labeled glucose and glutamine. To facilitate interpretation of the complex isotopomer data generated, we extend current methods for metabolic flux analysis to handle multivariate mass isotopomer distributions (MMIDs). We find that observed MMIDs are broadly consistent with known biochemical pathways. Whereas measured (13)C MIDs were informative for central carbon metabolism, (15)N isotopes provided evidence for nitrogen-carrying reactions in amino acid and nucleotide metabolism. This computational and experimental methodology expands the scope of metabolic flux analysis beyond carbon metabolism, and may prove important to understanding metabolic phenotypes in health and disease.

  7. On the isotopic composition of magmatic carbon in SNC meteorites (United States)

    Wright, I. P.; Grady, M. M.; Pillinger, C. T.


    SNC meteorites are thought, from many lines of evidence, to come from Mars. A line of investigation which has been pursued in our laboratory over the years involves measurement of the stable isotopic composition of carbon, in its various forms, in SNC meteorites. In order to establish a firm basis for studying the isotopic systematics of carbon in the martian surface environment, it is first necessary to try and constrain the delta C-13 of bulk Mars. Taking all of the available information, it would seem that the delta C-13 of the Earth's mantle lies somewhere in the range of -5 to -7 percent. Preliminary assessment of magnetic carbon in SNC meteorites, would tend to suggest a delta C-13 of 20 to 30 percent, which is conspicuously different from that of the terrestrial mantle. It is not obvious why there should be such a difference between the two planets, although many explanations are possible. One of these possibilities, that previous delta C-13 measurements for magnetic carbon in SNC meteorites are in error to some degree, is being actively investigated. The most recent results seem to constrain the theta C-13 of the magnetic carbon in SNC meteorites to about -20 percent, which is not at odds with previous estimates. As such, it is considered that a detailed investigation of the carbon isotopic systematics of martian surface materials does have the necessary information with which to proceed.

  8. Isotope effects of hafnium in solvent extraction using crown ethers

    Energy Technology Data Exchange (ETDEWEB)

    Fujii, Toshiyuki; Moriyama, Hirotake [Research Reactor Institute, Kyoto University, Osaka (Japan); Hirata, Takafumi [Laboratory for Planetary Sciences, Tokyo Institute of Technology, Tokyo (Japan); Nishizawa, Kazushige [Department of Nuclear Engineering, Graduate School of Engineering, Osaka University, Osaka (Japan)


    Hafnium isotopes were fractionated in a liquid-liquid extraction system by using seven types of crown ethers, tributyl phosphate, or {omicron}-diethoxybenzene. The largest isotope effect was observed in the isotope pair of {sup 177}Hf-{sup 179}Hf with dibenzo-24-crown-8; the isotope enrichment factor was observed to be 0.0129{+-}0.0032. (author)

  9. Environmental geochemistry of calcium isotopes: Applications of a new stable isotope approach

    Institute of Scientific and Technical Information of China (English)

    LIU Zhanmin; LIU Congqiang; HAN Guilin; WANG Zhongliang; XUE Zichen; SONG Zhaoliang; YANG Cheng


    This paper summarizes isotope fractionation mechanism, analytical method and applications in environmental geochemistry of calcium isotopes. Calcium isotopic composition can be used to constrain material sources and study geological and environmental processes as the isotopic composition of calcium (δ 44Ca) and fractionation processes depend on geochemical circumstances in nature. Recently, thanks to current advances in analytical technology of calcium isotopes, calcium isotopes are broadly used in biological and geochemical studies, such as the mechanism of plants imbibing nutrients through their roots, calcium transport in the environmental ecosystem, calcium cycle in oceans and paleo-oceans and paleo-climate. The elementary data show that δ44Ca values vary from -2.88‰ to 0.92‰ in natural samples.

  10. Newtonian kinetic isotope effects. Observation, prediction, and origin of heavy-atom dynamic isotope effects. (United States)

    Kelly, Kelmara K; Hirschi, Jennifer S; Singleton, Daniel A


    Intramolecular (13)C kinetic isotope effects were determined for the dimerization of cyclopentadiene. Substantial isotope effects were observed in three positions, despite the C(2) symmetry of the cycloaddition transition state and the absence of dynamical bottlenecks after this transition state. The observed isotope effects were predicted well from trajectory studies by extrapolating the outcomes of trajectories incorporating superheavy isotopes of carbon, ranging from (20)C to (140)C. Trajectory studies suggest that the isotope effects are unrelated to zero-point energy or the geometrical and momentum properties of the transition state. However, steepest-descent paths in mass-weighted coordinates correctly predict the direction of the isotope effects, supporting a novel origin in Newton's second law of motion.

  11. Isotope effects on desorption kinetics of hydrogen isotopes implanted into stainless steel by glow discharge

    Energy Technology Data Exchange (ETDEWEB)

    Matsuyama, M.; Kondo, M.; Noda, N. [Hydrogen Isotope Research Center, University of Toyama, Gofuku, Toyama (Japan); Tanaka, M.; Nishimura, K. [National Institute for Fusion Science, Toki-shi, Gifu (Japan)


    In a fusion device the control of fuel particles implies to know the desorption rate of hydrogen isotopes by the plasma-facing materials. In this paper desorption kinetics of hydrogen isotopes implanted into type 316L stainless steel by glow discharge have been studied by experiment and numerical calculation. The temperature of a maximum desorption rate depends on glow discharge time and heating rate. Desorption spectra observed under various experimental conditions have been successfully reproduced by numerical simulations that are based on a diffusion-limited process. It is suggested, therefore, that desorption rate of a hydrogen isotope implanted into the stainless steel is limited by a diffusion process of hydrogen isotope atoms in bulk. Furthermore, small isotope effects were observed for the diffusion process of hydrogen isotope atoms. (authors)

  12. Tracing contamination sources in soils with Cu and Zn isotopic ratios. (United States)

    Fekiacova, Z; Cornu, S; Pichat, S


    Copper (Cu) and zinc (Zn) are naturally present and ubiquitous in soils and are important micronutrients. Human activities contribute to the input of these metals to soils in different chemical forms, which can sometimes reach a toxic level for soil organisms and plants. Isotopic signatures could be used to trace sources of anthropogenic Cu and Zn pollution. The aim of this paper is to determine whether it is possible to identify (i) Cu and Zn contamination in soils and their sources, on the basis of their isotopic signatures, and (ii) situations that are a priori favorable or not for tracing Cu and Zn pollution using the isotopic approach. Therefore, we compiled data from the literature on Cu and Zn isotopes in soils, rocks and pollutants and added to this database the results of our own research. As only a few studies have dealt with agricultural contamination, we also studied a soil toposequence from Brittany, France, that experienced spreading of pig slurry for tens of years. In the surface horizons of the natural soils, the δ(65)Cu values vary from -0.15 to 0.44‰ and the δ(66)Zn from -0.03 to 0.43‰. Furthermore, vertical variations along soil profiles range from -0.95 to 0.44‰ for δ(65)Cu and from -0.53 to 0.64‰ for δ(66)Zn values. We concluded that pedogenetic processes can produce isotopic fractionation, yet, it is not always discernible and can be overprinted by an exogenous isotopic signature. Furthermore, some contaminants are enriched in heavy Cu or in light Zn compared to the rock or soil, but no generalization can be made. The anthropogenic inputs can be identified based on stable Cu and Zn isotope ratios if the isotope ratios of the sources are different from those of the soil, which needs to be tested for each individual case.

  13. Comparison of element and isotope diffusion of K and Ca in multicomponent silicate melts (United States)

    van der Laan, Sieger; Zhang, Youxue; Kennedy, Allen K.; Wyllie, Peter J.


    Recent experimental work has shown that the homogenization of elemental concentrations can be much slower than that of isotopic ratios when there are strong concentration gradients in SiO 2 and Al 2O 3. The ramifications of this result for magma homogenization and other petrological problems related to diffusion are significant. We report here a comparison of experimental profiles of elemental concentrations and isotopic fractions of K and Ca in rhyolite-andesite (large concentration gradients) and rhyolite-rhyolite (small concentration gradients) melt couples. When the concentration profile and the isotopic profile of the same element in a single couple are compared, the former is much shorter than the latter in the rhyolite-andesite couple, consistent with other recent studies. However, the lengths of both concentration and isotopic profiles are similar in the rhyolite-rhyolite couple. Therefore, diffusion of an element or oxide may be decoupled from or coupled with isotopic 'diffusion', depending on whether large concentration gradients of major components are present. When the two couples are compared, the intrinsic effective binary diffusivities obtained from isotopic profiles are similar for each element in the two couples, whereas the effective binary diffusivity of K obtained from the concentration profile in the rhyolite-rhyolite couple is 37 times that in the rhyolite-andesite couple. Therefore, isotopic homogenization is roughly independent of elemental homogenization and the presence of SiO 2, Al 2O 3, and other concentration gradients, whereas elemental homogenization is strongly affected by concentration gradients. Our experimental data (isotopic and concentration profiles including uphill diffusion profiles) can be modeled quantitatively to a good approximation using a modified effective binary diffusion model in which the flux of a component is assumed to be proportional to its activity gradient instead of its concentration gradient. Therefore, the

  14. Shear heating and clumped isotope reordering in carbonate faults (United States)

    Siman-Tov, Shalev; Affek, Hagit P.; Matthews, Alan; Aharonov, Einat; Reches, Ze'ev


    Natural faults are expected to heat rapidly during seismic slip and to cool quite quickly after the slip event. Here we examine clumped isotope thermometry for its ability to identify such short duration elevated temperature events along frictionally heated carbonate faults. Our approach is based on measured Δ47 values that reflect the distribution of oxygen and carbon isotopes in the calcite lattice, measuring the abundance of 13Csbnd 18O bonds, which is affected by temperature. We examine three types of calcite rock samples: (1) crushed limestone grains that were rapidly heated and then cooled in static laboratory experiments, simulating the temperature cycle experienced by fault rock during an earthquake slip; (2) limestone samples that were experimentally sheared to simulate earthquake slip events; and (3) samples from Fault Mirrors (FMs) collected from principle slip surfaces of three natural carbonate faults. Extensive FM surfaces are believed to form during earthquake slip. Our experimental results show that Δ47 values decrease rapidly (in the course of seconds) with increasing temperature and shear velocity. On the other hand, carbonate shear zones from natural faults do not show such Δ47 decrease. We suggest that the Δ47 response may be controlled by nano-size grains, the high abundance of defects, and highly stressed/strained grain boundaries within the carbonate fault zone that can reduce the activation energy for diffusion, and thus lead to an increased rate of isotopic disordering during shear experiments. In our laboratory experiments the high stress and strain on grain contacts and the presence of nanograins thus allows for rapid disordering so that a change in Δ47 occurs in a very short and relatively low intensity heating events. In natural faults it may also lead to isotopic ordering after the cessation of frictional heating thus erasing the high temperature signature of Δ47.

  15. Distribution of radionuclides in mussels, winkles and prawns: Pt. 1; Study of organisms under environmental conditions using conventional radio-analytical techniques

    Energy Technology Data Exchange (ETDEWEB)

    McDonald, P. (Scottish Research Reactor Centre, East Kilbride (United Kingdom)); Baxter, M.S.; Fowler, S.W. (International Atomic Energy Agency, Monaco (Monaco). Marine Environment Lab.)


    Mussels (Mytilus edulis) and winkles (Littorina littorea), collected from Ravenglass, Cumbria, England in the vicinity of the British Nuclear Fuels plc nuclear reprocessing plant at Sellafield, and prawns (Palaemon serratus), landed nearby at Whitehaven, have been investigated to determine the distributions of [alpha]-emitting ([sup 210]Po, [sup 238]Pu, [sup 239] [sup +] [sup 240]Pu, [sup 241]Am) and [gamma]-emitting ([sup 95]Nb, [sup 95]Zr, [sup 103]Ru, [sup 106]Ru, [sup 137]Cs, [sup 241]Am) radionuclides in their tissues and organs. Previous studies have attempted to determine the principal nuclide source to marine organisms by comparing nuclide activity ratios in their tissues, sea water and particulate material. From the environmental samples studied here, no single transport medium appears to dominate uptake. The primary radiological implantation of the observed radionuclide concentrations in Ravenglass mussels and winkles is that, from seafood ingestion, the critical group receives only a small percentage (ca. 10%) of the ICRP-recommended subsidiary dose limit. Dose contributions from [sup 210]Po are higher than those from [sup 239] + [sup 240]Pu in mussels but are less than those from [sup 239] [sup +] [sup 240]Pu in winkles. (Author).

  16. New Mexico Center for Isotopes in Medicine

    Energy Technology Data Exchange (ETDEWEB)

    Burchiel, Scott W.


    The purpose of the New Mexico Center for Isotopes in Medicine (NMCIM) is to support research, education and service missions of the UNM College of Pharmacy Radiopharmaceutical Sciences Program (COP RSP) and the Cancer Research and Treatment Center (CRTC). NMCIM developed and coordinated unique translational research in cancer radioimaging and radiotherapy agents based on novel molecules developed at UNM and elsewhere. NMCIM was the primary interface for novel radioisotopes and radiochemistries developed at the Los Alamos National Laboratory (LANL) for SPECT/PET imaging and therapy. NMCIM coordinated the use of the small animal imaging facility with the CRTC provided support services to assist investigators in their studies. NMCIM developed education and training programs that benefited professional, graduate, and postdoctoral students that utilized its unique facilities and technologies. UNM COP RSP has been active in writing research and training grants, as well as supporting contract research with industrial partners. The ultimate goal of NMCIM is to bring new radiopharmaceutical imaging and therapeutic agents into clinical trials that will benefit the health and well being of cancer and other patients in New Mexico and the U.S.

  17. [Aseptic meningitis after isotope cisternography. 2 Cases]. (United States)

    Guy, G; Comoy, J; Chevet, D; Thomas, R; le Pogamp, P


    In these two patients, as in 13 others described in the literature, a typical meningitic syndrome with excitement, confusion and a fever of 104degrees F (40degrees C) appeared 4-6 hours following the intra-thecal injection. Subsequent lumbar puncture usually reveals a cloudy C.S.F. under increased pressure. The polymorphs and proteins are increased but the glucose remains normal. There are no bacteria either on direct examination or after culture. All the patients receive antibiotics. After a course of three days, the symptoms and the fever have disappeared and the C.S.F. became normal. Bacterial contamination can be ruled out. The relative roles of iodine, radio-acitivity itself, albumine and of the radio-active element which are only used for this radiotracer are discussed. The tracer contains neither stabilizer nor pH buffer. One must presume that the syndrome is due to a direct toxic action rather than to an immunological or allergic reaction. Furthermore, it is of interest that similar reactions, without infection, are seen after spinal anaesthesia and intra-thecal injection of such differing substances such as iodine contrast media, gamma globulins, other isotopes or toxic substances (Lysol) (111In-DTPA).

  18. Short course on St-02 applications of isotope dilutions and isotopic measurements

    Energy Technology Data Exchange (ETDEWEB)

    Miller, P.


    This short course includes information on these topics and subtopics: (I) Nuclear Properties: (A) Historic roots; (B) Nomenclature; (C) Nuclear Stability and abundance; (D) Uses of isotopic techniques; (II) Instrumentation: (A) Sources; (B) Mass resolving elements; (C) Detectors; (III) Making Isotopic Measurements by ICP-MS: (A) Deadtime Correction; (B) Mass Discrimination; (C) Signal /Noise considerations; (IV) Applications and examples: (A) Isotope dilution; (B) Double Spike; (C) Biological Application; (D) Environmental Application; (E) Geological.

  19. Lead isotope studies of the Guerrero composite terrane, west-central Mexico: implications for ore genesis (United States)

    Potra, Adriana; Macfarlane, Andrew W.


    field defined by the Huetamo Sequence, suggesting that these ores may also contain metals from the sedimentary rocks. The Pb isotope ratios of ore samples from the Zimapan deposit (206Pb/204Pb = 18.771-18.848) are substantially higher than the whole-rock Pb isotope compositions of the basement rocks. The similarity of ore Pb to igneous rock Pb in the Zimapan district (206Pb/204Pb = 18.800-18.968) may indicate that the proximal source of ore metals in the hydrothermal system was the igneous activity.

  20. In Vivo Mass-independent Fractionation of Mercury Isotopes in Fish (United States)

    Das, R.; Odom, L. A.


    hyperfine coupling influence radical recombination and thus reaction kinetics. There is experimental evidence that this can occur during the inhibiting activity of methylmercury on creatine kinase. Here the enzyme provides the free radicals. Previously, reports of chemical mass- independent fractionation of isotopes in nature have involved gas phase reactions and largely explained by photolysis. It now seems that isotopic MIF can occur during metabolic processes as well.

  1. Tracing contamination sources in soils with Cu and Zn isotopic ratios

    Energy Technology Data Exchange (ETDEWEB)

    Fekiacova, Z.; Cornu, S. [INRA, UR 1119 Géochimie des Sols et des Eaux, F-13100 Aix en Provence (France); Pichat, S. [Laboratoire de Géologie de Lyon (LGL-TPE), Ecole Normale Supérieure de Lyon, CNRS, UMR 5276, 69007 Lyon (France)


    Copper (Cu) and zinc (Zn) are naturally present and ubiquitous in soils and are important micronutrients. Human activities contribute to the input of these metals to soils in different chemical forms, which can sometimes reach a toxic level for soil organisms and plants. Isotopic signatures could be used to trace sources of anthropogenic Cu and Zn pollution. The aim of this paper is to determine whether it is possible to identify (i) Cu and Zn contamination in soils and their sources, on the basis of their isotopic signatures, and (ii) situations that are a priori favorable or not for tracing Cu and Zn pollution using the isotopic approach. Therefore, we compiled data from the literature on Cu and Zn isotopes in soils, rocks and pollutants and added to this database the results of our own research. As only a few studies have dealt with agricultural contamination, we also studied a soil toposequence from Brittany, France, that experienced spreading of pig slurry for tens of years. In the surface horizons of the natural soils, the δ{sup 65}Cu values vary from − 0.15 to 0.44‰ and the δ{sup 66}Zn from − 0.03 to 0.43‰. Furthermore, vertical variations along soil profiles range from − 0.95 to 0.44‰ for δ{sup 65}Cu and from − 0.53 to 0.64‰ for δ{sup 66}Zn values. We concluded that pedogenetic processes can produce isotopic fractionation, yet, it is not always discernible and can be overprinted by an exogenous isotopic signature. Furthermore, some contaminants are enriched in heavy Cu or in light Zn compared to the rock or soil, but no generalization can be made. The anthropogenic inputs can be identified based on stable Cu and Zn isotope ratios if the isotope ratios of the sources are different from those of the soil, which needs to be tested for each individual case. - Highlights: • Pedogenetic processes produce some Cu and Zn isotope fractionation. • Pollution with distinct isotopic signatures can be traced using Cu and Zn isotopes. • Tracing

  2. Research on isotope geology: Isotopes ages of volcanic rocks from Ryeongnam Massif, Korea

    Energy Technology Data Exchange (ETDEWEB)

    Shin, Seong Cheon; Chi, Se Jung; Kim, Yoo Sook [Korea Institute of Geology Mining and Materials, Taejon (Korea, Republic of)


    Chronostratigraphy of most volcanic rocks in the Ryeongnam Massif have been undefined or mis-classified in different geological maps due to total absence of reported isotope ages. Twenty-four new isotope ages are given for age-undefined volcanic units and some related igneous bodies. Most of volcanic rocks show high [La/Yb]n ratios and LREE enrichments which are characteristics of subduction-related high-K calc-alkali volcanic rocks occurred in the active continental margin. Preliminary results on carbon and oxygen stable isotope ratios({delta}{sup 13}C=-1.7{approx}-6.2 per mil; {delta}{sup 18} O=-21.6{approx}-24.7 per mil) of druse- or phenocryst-calcite from andesitic and basaltic rocks in the southern coastal region indicate a magmatic origin. Based on new K-Ar whole-rock ages, chronological guidelines are established as follows: 1) Gayasan andesite (78{+-}4Ma) - Gurye andesitic tuff (81{+-}4Ma); 2) Gurye andesite (68{+-}4Ma) - Suncheon andesitic tuff (67{+-}3Ma) - Yeosu basaltic andesite (67{+-}3Ma) - Narodo andesite (70{+-}3Ma); 3) Taebaeg Baegbyeongsan basaltic andesite (62{+-}3Ma) - Gurye Obongsan andesite (64{+-}3Ma) - Yeosu dacite (63{+-}3Ma) - Dolsando andesite (62{+-}3Ma) - Jangheung Buyongsan andesite (65{+-}3Ma); 4) Suncheon Joryedong andesite (55{+-}2Ma) - Goheung andesite (56{+-}3Ma); 5) Taebaeg Baegbyeonsan basaltic andesite (48{+-}2Ma) - Yeosu basalt (51{+-}3Ma). Resetted age (49{+-}2Ma) of an intrusive rhyolite implies the timing of thermal alteration in the Wondong Fe-Mine of the Taebaegsan Mineralized Belt. K-Ar hornblende ages of two hornblendite stocks in the southern Jangsu suggests apparent emplacement-ages of late Triassic (210{+-}9Ma) and early Permian (274{+-}10Ma), independently. K-Ar hornblende age (1023{+-}37Ma) of the Ogbang amphibolite implies a reduction of original age due to later thermal effect probably attributed to either later intrusion or regional metamorphism. (author). 56 refs., 19 tabs., 14 figs.

  3. Isotope pattern deconvolution as rising tool for isotope tracer studies in environmental research (United States)

    Irrgeher, Johanna; Zitek, Andreas; Prohaska, Thomas


    During the last decade stable isotope tracers have emerged as versatile tool in ecological research. Besides 'intrinsic' isotope tracers caused by the natural variation of isotopes, the intentional introduction of 'extrinsic' enriched stable isotope tracers into biological systems has gained significant interest. Hereby the induced change in the natural isotopic composition of an element allows amongst others for studying the fate and fluxes of metals, trace elements and species in organisms or provides an intrinsic marker or tag of particular biological samples. Due to the shoreless potential of this methodology, the number of publications dealing with applications of isotope (double) spikes as tracers to address research questions in 'real world systems' is constantly increasing. However, some isotope systems like the natural Sr isotopic system, although potentially very powerful for this type of application, are still rarely used, mainly because their adequate measurement/determination poses major analytical challenges; as e.g. Sr is available in significant amounts in natural samples. In addition, biological systems underlie complex processes such as metabolism, adsorption/desorption or oxidation/reduction. As a consequence, classic evaluation approaches such as the isotope dilution mass spectrometry equation are often not applicable because of the unknown amount of tracer finally present in the sample. Isotope pattern deconvolution (IPD), based on multiple linear regression, serves as simplified alternative data processing strategy to double spike isotope dilution calculations. The outstanding advantage of this mathematical tool lies in the possibility of deconvolving the isotope pattern in a spiked sample without knowing the quantities of enriched isotope tracer being incorporated into the natural sample matrix as well as the degree of impurities and species-interconversion (e.g. from sample preparation). Here, the potential of IPD for environmental tracer

  4. Stable isotope production with laser techniques; Production d`isotopes stables a l`aide des techniques laser

    Energy Technology Data Exchange (ETDEWEB)

    Petit, A. [CEA Centre d`Etudes de Saclay, 91 - Gif-sur-Yvette (France). Dept. des Procedes d`Enrichissement


    Laser properties may be used for stable isotope production either by selective photoionization of an atom particular isotope, either by selective photodissociation of a molecule. Principles of both processes are reviewed and examples of calcium 43 isotope separation through photoionization and of carbon and oxygen isotope separation by photodissociation are presented. 4 figs., 1 tab., 11 refs.

  5. Beam delivery for stable isotope separation (United States)

    Forbes, Andrew; Strydom, Hendrick J.; Botha, Lourens R.; Ronander, Einar


    In the multi-photon dissociation process of Carbon isotope enrichment, IR photons are used to selectively excite a molecule with the given isotopic base element. This enrichment process is very sensitive to the beam's intensity and wavelength. Because the intensity is determined by the propagation of the field, the enrichment factors are also very dependent on the field propagation. In this paper, the influence of the wavelength and intensity of the beam, on the isotope selective dissociation of a CFC compound is investigated both experimentally and theoretically. Consideration is also given to some of the factors that influence the delivery of various beams to the reactor chamber, and their subsequent propagation through the reactor. The results show that suitable beam forming can lead to an improved isotope separation process.

  6. On the progress in stable isotope separation

    Energy Technology Data Exchange (ETDEWEB)

    Prusakov, V.N. [Kurchatov Institute, Moscow (Russian Federation)


    The principles and process of centrifuge isotope separation are reviewed; the fundamental advantage of the centrifuge over gaseous diffusion arises from the fact that the primary isotope separation effect occurs at thermodynamic equilibrium; thus, gas centrifuge enrichment uses only about 1/20 to 1/30 of the electricity per SWU (separation work unit) consumed by gaseous diffusion. The various substances that can be used in centrifuge isotope separation are listed (fluorides, oxyfluorides, {pi}-complexes, boron hydrides, metal-organic compounds, halides...). The centrifuge method productivity is much greater than with the electromagnetic separation technique; examples of centrifuge stable and radioactive isotope separation are given; the method of the residue reduction is also presented with the example of separating radioactive krypton-85 out of a nuclear reactor krypton blend. 4 figs.

  7. Stable Oxygen-18 and Deuterium Isotopes

    DEFF Research Database (Denmark)

    Müller, Sascha

    development within a given lowland headwater catchment (stream water isotopes). Based on our investigations on the precipitation isotopic composition a local meteoric water line (LMWL) was constructed and expressed as: δ2H=7.4 δ18O + 5.36‰. Moreover, we showed that under maritime temperature climate influence......, humidity is the main driver for the temporal and spatial isotopic development and temperature plays only a secondary role. Based on our investigations at a coastal lagoon aquifer we could improve quantifications of seasonal saltwater-wedge dynamics, based on isotopic tracers combined with salinity. We can...... link the observed seasonal regression/transgression pattern to the inland recharge cycle, which is expressed in hydraulic head configuration and submarine groundwater dis